Fundamental study of CO2-H2O-mineral interactions for carbon sequestration, with emphasis on the nature of the supercritical fluid-mineral interface.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bryan, Charles R.; Dewers, Thomas A.; Heath, Jason E.

2013-09-01

In the supercritical CO2-water-mineral systems relevant to subsurface CO2 sequestration, interfacial processes at the supercritical fluid-mineral interface will strongly affect core- and reservoir-scale hydrologic properties. Experimental and theoretical studies have shown that water films will form on mineral surfaces in supercritical CO2, but will be thinner than those that form in vadose zone environments at any given matric potential. The theoretical model presented here allows assessment of water saturation as a function of matric potential, a critical step for evaluating relative permeabilities the CO2 sequestration environment. The experimental water adsorption studies, using Quartz Crystal Microbalance and Fourier Transform Infrared Spectroscopymore » methods, confirm the major conclusions of the adsorption/condensation model. Additional data provided by the FTIR study is that CO2 intercalation into clays, if it occurs, does not involve carbonate or bicarbonate formation, or significant restriction of CO2 mobility. We have shown that the water film that forms in supercritical CO2 is reactive with common rock-forming minerals, including albite, orthoclase, labradorite, and muscovite. The experimental data indicate that reactivity is a function of water film thickness; at an activity of water of 0.9, the greatest extent of reaction in scCO2 occurred in areas (step edges, surface pits) where capillary condensation thickened the water films. This suggests that dissolution/precipitation reactions may occur preferentially in small pores and pore throats, where it may have a disproportionately large effect on rock hydrologic properties. Finally, a theoretical model is presented here that describes the formation and movement of CO2 ganglia in porous media, allowing assessment of the effect of pore size and structural heterogeneity on capillary trapping efficiency. The model results also suggest possible engineering approaches for optimizing trapping capacity and for monitoring ganglion formation in the subsurface.« less

A disconnect between O horizon and mineral soil carbon - Implications for soil C sequestration

NASA Astrophysics Data System (ADS)

Garten, Charles T., Jr.

2009-03-01

Changing inputs of carbon to soil is one means of potentially increasing carbon sequestration in soils for the purpose of mitigating projected increases in atmospheric CO 2 concentrations. The effect of manipulations of aboveground carbon input on soil carbon storage was tested in a temperate, deciduous forest in east Tennessee, USA. A 4.5-year experiment included exclusion of aboveground litterfall and supplemental litter additions (three times ambient) in an upland and a valley that differed in soil nitrogen availability. The estimated decomposition rate of the carbon stock in the O horizon was greater in the valley than in the upland due to higher litter quality (i.e., lower C/N ratios). Short-term litter exclusion or addition had no effect on carbon stock in the mineral soil, measured to a depth of 30 cm, or the partitioning of carbon in the mineral soil between particulate- and mineral-associated organic matter. A two-compartment model was used to interpret results from the field experiments. Field data and a sensitivity analysis of the model were consistent with little carbon transfer between the O horizon and the mineral soil. Increasing aboveground carbon input does not appear to be an effective means of promoting carbon sequestration in forest soil at the location of the present study because a disconnect exists in carbon dynamics between O horizon and mineral soil. Factors that directly increase inputs to belowground soil carbon, via roots, or reduce decomposition rates of organic matter are more likely to benefit efforts to increase carbon sequestration in forests where carbon dynamics in the O horizon are uncoupled from the mineral soil.

Reactive transport modeling of CO2 mineral sequestration in basaltic rocks

NASA Astrophysics Data System (ADS)

Aradottir, E. S.; Sonnenthal, E. L.; Bjornsson, G.; Jonsson, H.

2011-12-01

CO2 mineral sequestration in basalt may provide a long lasting, thermodynamically stable, and environmentally benign solution to reduce greenhouse gases in the atmosphere. Multi-dimensional, field scale, reactive transport models of this process have been developed with a focus on the CarbFix pilot CO2 injection in Iceland. An extensive natural analog literature review was conducted in order to identify the primary and secondary minerals associated with water-basalt interaction at low and elevated CO2 conditions. Based on these findings, an internally consistent thermodynamic database describing the mineral reactions of interest was developed and validated. Hydrological properties of field scale mass transport models were properly defined by calibration to field data using iTOUGH2. Reactive chemistry was coupled to the models and TOUGHREACT used for running predictive simulations carried out with the objective of optimizing long-term management of injection sites, to quantify the amount of CO2 that can be mineralized, and to identify secondary minerals that compete with carbonates for cations leached from the primary rock. Calibration of field data from the CarbFix reservoir resulted in a horizontal permeability for lava flows of 300 mD and a vertical permeability of 1700 mD. Active matrix porosity was estimated to be 8.5%. The CarbFix numerical models were a valuable engineering tool for designing optimal injection and production schemes aimed at increasing groundwater flow. Reactive transport simulations confirm dissolution of primary basaltic minerals as well as carbonate formation, and thus indicate in situ CO2 mineral sequestration in basalts to be a viable option. Furthermore, the simulations imply that clay minerals are most likely to compete with magnesite-siderite solid solutions for Mg and Fe leached from primary minerals, whereas zeolites compete with calcite for dissolved Ca. In the case of the CarbFix pilot injection, which involves a continuous injection of 1,100 tons CO2 in total for 6 months, the basalt hosted reservoir was estimated to have a 100% sequestering efficiency after 10 years. In the case of an upscaled 10 year long injection of 40,000 tons per year, sequestering efficiency of the same reservoir was estimated to be about 10% after 100 years. However, sequestering efficiency in the latter case has every potential of increasing substantially with time due to the vast amount of primary basaltic minerals in the reservoir.

Rapid soil formation after glacial retreat shaped by spatial patterns of organic matter accrual in microaggregates.

PubMed

Schweizer, Steffen A; Hoeschen, Carmen; Schlüter, Steffen; Kögel-Knabner, Ingrid; Mueller, Carsten W

2018-04-01

Global change contributes to the retreat of glaciers at unprecedented rates. The deglaciation facilitates biogeochemical processes on glacial deposits with initiating soil formation as an important driver of evolving ecosystems. The underlying mechanisms of soil formation and the association of soil organic matter (SOM) with mineral particles remain unclear, although further insights are critical to understand carbon sequestration in soils. We investigated the microspatial arrangement of SOM coatings at intact soil microaggregate structures during various stages of ecosystem development from 15 to >700 years after deglaciation in the proglacial environment of the Damma glacier (Switzerland). The functionally important clay-sized fraction (<2 μm) was separated into two density fractions with different amounts of organo-mineral associations: light (1.6-2.2 g/cm 3 ) and heavy (>2.2 g/cm 3 ). To quantify how SOM extends across the surface of mineral particles (coverage) and whether SOM coatings are distributed in fragmented or connected patterns (connectivity), we developed an image analysis protocol based on nanoscale secondary ion mass spectrometry (NanoSIMS). We classified SOM and mineral areas depending on the 16 O - , 12 C - , and 12 C 14 N - distributions. With increasing time after glacial retreat, the microspatial coverage and connectivity of SOM increased rapidly. The rapid soil formation led to a succession of patchy distributed to more connected SOM coatings on soil microaggregates. The maximum coverage of 55% at >700 years suggests direct evidence for SOM sequestration being decoupled from the mineral surface, as it was not completely masked by SOM and retained its functionality as an ion exchange site. The chemical composition of SOM coatings showed a rapid change toward a higher CN:C ratio already at 75 years after glacial retreat, which was associated with microbial succession patterns reflecting high N assimilation. Our results demonstrate that rapid SOM sequestration drives the microspatial succession of SOM coatings in soils, a process that can stabilize SOM for the long term. © 2017 John Wiley & Sons Ltd.

The fate of cyanide in leach wastes at gold mines: an environmental perspective

USGS Publications Warehouse

Johnson, Craig A.

2015-01-01

Cyanide-containing and cyanide-related species are subject to attenuation mechanisms that lead to dispersal to the atmosphere, chemical transformation to other carbon and nitrogen species, or sequestration as cyanometallic precipitates or adsorbed species on mineral surfaces. Dispersal to the atmosphere and chemical transformation amount to permanent elimination of cyanide, whereas sequestration amounts to storage of cyanide in locations from which it can potentially be remobilized by infiltrating waters if conditions change. From an environmental perspective, the most significant cyanide releases from gold leach operations involve catastrophic spills of process solutions or leakage of effluent to the unsaturated or saturated zones. These release pathways are unfavorable for two important cyanide attenuation mechanisms that tend to occur naturally: dispersal of free cyanide to the atmosphere and sunlight-catalyzed dissociation of strong cyanometallic complexes, which produces free cyanide that can then disperse to the atmosphere. The widest margins of environmental safety will be achieved where mineral processing operations are designed so that time for offgassing, aeration, and sunlight exposure are maximized in the event that cyanide-bearing solutions are released inadvertently.

Geochemical Modeling of Carbon Sequestration, MMV, and EOR in the Illinois Basin

USGS Publications Warehouse

Berger, P.M.; Roy, W.R.; Mehnert, E.

2009-01-01

The Illinois State Geologic Survey is conducting several ongoing CO2 sequestration projects that require geochemical models to gain an understanding of the processes occurring in the subsurface. The ISGS has collected brine and freshwater samples associated with an enhanced oil recovery project in the Loudon oil field. Geochemical modeling allows us to understand reactions with carbonate and silicate minerals in the reservoir, and the effects they have had on brine composition. For the Illinois Basin Decatur project, geochemical models should allow predictions of the reactions that will take place before CO2 injection begins. ?? 2009 Elsevier Ltd. All rights reserved.

Nanomineralogy as a new dimension in understanding elusive geochemical processes in soils: The case of low-solubility-index elements

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schindler, Michael; Hochella, Michael F.

2016-05-20

Nanomineralogy is a new dimension in understanding chemical processes in soils. These processes are revealed at the nanoscale within the structures and compositions of phases that heretofore were not even known to exist in the soils in which they are found. The discovery and understanding of soil chemistry in this way is best accessible via a combination of focused ion beam technology (for sample preparation) and high resolution, analytical transmission electron microscopy (for phase identification). We have used this scientific framework and these techniques to decipher past and present chemical processes in a soil in Sudbury, Ontario, Canada that hasmore » been impacted by both smelter contamination (acidification) and subsequent remediation within the past century. In this study, we use these methods to investigate mobilization and sequestration of the relatively immobile elements Al, Ti and Zr. In a micrometer-thick alteration layer on an albite grain, a first generation of clay minerals represents weathering of the underlying mineral prior to the acidification of the soils. Complex assemblages of Ti- and Zr-bearing nanophases occur on the surfaces of Fe-(hydr)oxide crystals and are the result of the dissolution of silicates and oxides and the mobilization of Ti- and Zr-bearing colloids under acidic conditions. These phases include anatase (TiO2), kleberite (Fe3+Ti6O11(OH)5) Ti4O7, baddelyite (ZrO2), a structural analogue to kelyshite (NaZr[Si2O6(OH)]) and authigenic zircon (ZrSiO4). Subsequent remediation of the acidic soils has resulted in the sequestration of Al and in the neoformation of the clay minerals kaolinite, smectite and illite. These complex mineral assemblages form a porous layer that controls the interaction of the underlying mineral with the environment.« less

Synthetic effect between iron oxide and sulfate mineral on the anaerobic transformation of organic substance.

PubMed

Chen, Tian-Hu; Wang, Jin; Zhou, Yue-Fei; Yue, Zheng-Bo; Xie, Qiao-Qin; Pan, Min

2014-01-01

Synthetic effect between sulfate minerals (gypsum) and iron oxide (hematite) on the anaerobic transformation of organic substance was investigated in the current study. The results showed that gypsum was completely decomposed while hematite was partially reduced. The mineral phase analysis results showed that FeS and CaCO3 was the major mineralization product. Methane generation process was inhibited and inorganic carbon contents in the precipitates were enhanced compared to the control without hematite and gypsum. The inorganic carbon content increased with the increasing of hematite dosages. Co-addition of sulfate minerals and iron oxide would have a potential application prospect in the carbon sequestration area and reduction of the greenhouse gas release. The results would also reveal the role of inorganic mineral in the global carbon cycle. Copyright © 2013 Elsevier Ltd. All rights reserved.

Predictive modeling of CO2 sequestration in deep saline sandstone reservoirs: Impacts of geochemical kinetics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Balashov, Victor N.; Guthrie, George D.; Hakala, J. Alexandra

2013-03-01

One idea for mitigating the increase in fossil-fuel generated CO{sub 2} in the atmosphere is to inject CO{sub 2} into subsurface saline sandstone reservoirs. To decide whether to try such sequestration at a globally significant scale will require the ability to predict the fate of injected CO{sub 2}. Thus, models are needed to predict the rates and extents of subsurface rock-water-gas interactions. Several reactive transport models for CO{sub 2} sequestration created in the last decade predicted sequestration in sandstone reservoirs of ~17 to ~90 kg CO{sub 2} m{sup -3|. To build confidence in such models, a baseline problem including rockmore » + water chemistry is proposed as the basis for future modeling so that both the models and the parameterizations can be compared systematically. In addition, a reactive diffusion model is used to investigate the fate of injected supercritical CO{sub 2} fluid in the proposed baseline reservoir + brine system. In the baseline problem, injected CO{sub 2} is redistributed from the supercritical (SC) free phase by dissolution into pore brine and by formation of carbonates in the sandstone. The numerical transport model incorporates a full kinetic description of mineral-water reactions under the assumption that transport is by diffusion only. Sensitivity tests were also run to understand which mineral kinetics reactions are important for CO{sub 2} trapping. The diffusion transport model shows that for the first ~20 years after CO{sub 2} diffusion initiates, CO{sub 2} is mostly consumed by dissolution into the brine to form CO{sub 2,aq} (solubility trapping). From 20-200 years, both solubility and mineral trapping are important as calcite precipitation is driven by dissolution of oligoclase. From 200 to 1000 years, mineral trapping is the most important sequestration mechanism, as smectite dissolves and calcite precipitates. Beyond 2000 years, most trapping is due to formation of aqueous HCO{sub 3}{sup -}. Ninety-seven percent of the maximum CO{sub 2} sequestration, 34.5 kg CO{sub 2} per m{sup 3} of sandstone, is attained by 4000 years even though the system does not achieve chemical equilibrium until ~25,000 years. This maximum represents about 20% CO{sub 2} dissolved as CO{sub 2},aq, 50% dissolved as HCO{sub 3}{sup -}{sub ,aq}, and 30% precipitated as calcite. The extent of sequestration as HCO{sub 3}{sup -} at equilibrium can be calculated from equilibrium thermodynamics and is roughly equivalent to the amount of Na+ in the initial sandstone in a soluble mineral (here, oligoclase). Similarly, the extent of trapping in calcite is determined by the amount of Ca2+ in the initial oligoclase and smectite. Sensitivity analyses show that the rate of CO{sub 2} sequestration is sensitive to the mineral-water reaction kinetic constants between approximately 10 and 4000 years. The sensitivity of CO{sub 2} sequestration to the rate constants decreases in magnitude respectively from oligoclase to albite to smectite.« less

Tillage and cropping sequence impacts on nitrogen cycling in dryland farming in eastern Montana, USA

USDA-ARS?s Scientific Manuscript database

Information on N cycling in dryland crops and soils as influenced by long-term tillage and cropping sequence is needed to quantify soil N sequestration, mineralization, and N balance to reduce N fertilization rate and N losses through soil processes. We evaluated the 21-yr effects of combinations of...

Erosion of soil organic carbon: implications for carbon sequestration

USGS Publications Warehouse

Van Oost, Kristof; Van Hemelryck, Hendrik; Harden, Jennifer W.; McPherson, B.J.; Sundquist, E.T.

2009-01-01

Agricultural activities have substantially increased rates of soil erosion and deposition, and these processes have a significant impact on carbon (C) mineralization and burial. Here, we present a synthesis of erosion effects on carbon dynamics and discuss the implications of soil erosion for carbon sequestration strategies. We demonstrate that for a range of data-based parameters from the literature, soil erosion results in increased C storage onto land, an effect that is heterogeneous on the landscape and is variable on various timescales. We argue that the magnitude of the erosion term and soil carbon residence time, both strongly influenced by soil management, largely control the strength of the erosion-induced sink. In order to evaluate fully the effects of soil management strategies that promote carbon sequestration, a full carbon account must be made that considers the impact of erosion-enhanced disequilibrium between carbon inputs and decomposition, including effects on net primary productivity and decomposition rates.

Nanoscale Chemical Processes Affecting Storage Capacities and Seals during Geologic CO2 Sequestration.

PubMed

Jun, Young-Shin; Zhang, Lijie; Min, Yujia; Li, Qingyun

2017-07-18

Geologic CO 2 sequestration (GCS) is a promising strategy to mitigate anthropogenic CO 2 emission to the atmosphere. Suitable geologic storage sites should have a porous reservoir rock zone where injected CO 2 can displace brine and be stored in pores, and an impermeable zone on top of reservoir rocks to hinder upward movement of buoyant CO 2 . The injection wells (steel casings encased in concrete) pass through these geologic zones and lead CO 2 to the desired zones. In subsurface environments, CO 2 is reactive as both a supercritical (sc) phase and aqueous (aq) species. Its nanoscale chemical reactions with geomedia and wellbores are closely related to the safety and efficiency of CO 2 storage. For example, the injection pressure is determined by the wettability and permeability of geomedia, which can be sensitive to nanoscale mineral-fluid interactions; the sealing safety of the injection sites is affected by the opening and closing of fractures in caprocks and the alteration of wellbore integrity caused by nanoscale chemical reactions; and the time scale for CO 2 mineralization is also largely dependent on the chemical reactivities of the reservoir rocks. Therefore, nanoscale chemical processes can influence the hydrogeological and mechanical properties of geomedia, such as their wettability, permeability, mechanical strength, and fracturing. This Account reviews our group's work on nanoscale chemical reactions and their qualitative impacts on seal integrity and storage capacity at GCS sites from four points of view. First, studies on dissolution of feldspar, an important reservoir rock constituent, and subsequent secondary mineral precipitation are discussed, focusing on the effects of feldspar crystallography, cations, and sulfate anions. Second, interfacial reactions between caprock and brine are introduced using model clay minerals, with focuses on the effects of water chemistries (salinity and organic ligands) and water content on mineral dissolution and surface morphology changes. Third, the hydrogeological responses (using wettability alteration as an example) of clay minerals to chemical reactions are discussed, which connects the nanoscale findings to the transport and capillary trapping of CO 2 in the reservoirs. Fourth, the interplay between chemical and mechanical alterations of geomedia, using wellbore cement as a model geomedium, is examined, which provides helpful insights into wellbore and caprock integrities and CO 2 mineralization. Combining these four aspects, our group has answered questions related to nanoscale chemical reactions in subsurface GCS sites regarding the types of reactions and the property alterations of reservoirs and caprocks. Ultimately, the findings can shed light on the influences of nanoscale chemical reactions on storage capacities and seals during geologic CO 2 sequestration.

Reply to 'Comments on upscaling geochemical reaction rates usingpore-scale network modeling' by Peter C. Lichtner and Qinjun Kang

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Li; Peters, Catherine A.; Celia, Michael A.

2006-05-03

Our paper "Upscaling geochemical reaction rates usingpore-scale network modeling" presents a novel application of pore-scalenetwork modeling to upscale mineral dissolution and precipitationreaction rates from the pore scale to the continuum scale, anddemonstrates the methodology by analyzing the scaling behavior ofanorthite and kaolinite reaction kinetics under conditions related to CO2sequestration. We conclude that under highly acidic conditions relevantto CO2 sequestration, the traditional continuum-based methodology may notcapture the spatial variation in concentrations from pore to pore, andscaling tools may be important in correctly modeling reactive transportprocesses in such systems. This work addresses the important butdifficult question of scaling mineral dissolution and precipitationreactionmore » kinetics, which is often ignored in fields such as geochemistry,water resources, and contaminant hydrology. Although scaling of physicalprocesses has been studied for almost three decades, very few studieshave examined the scaling issues related to chemical processes, despitetheir importance in governing the transport and fate of contaminants insubsurface systems.« less

Sequestration of Martian CO2 by mineral carbonation

PubMed Central

Tomkinson, Tim; Lee, Martin R.; Mark, Darren F.; Smith, Caroline L.

2013-01-01

Carbonation is the water-mediated replacement of silicate minerals, such as olivine, by carbonate, and is commonplace in the Earth’s crust. This reaction can remove significant quantities of CO2 from the atmosphere and store it over geological timescales. Here we present the first direct evidence for CO2 sequestration and storage on Mars by mineral carbonation. Electron beam imaging and analysis show that olivine and a plagioclase feldspar-rich mesostasis in the Lafayette meteorite have been replaced by carbonate. The susceptibility of olivine to replacement was enhanced by the presence of smectite veins along which CO2-rich fluids gained access to grain interiors. Lafayette was partially carbonated during the Amazonian, when liquid water was available intermittently and atmospheric CO2 concentrations were close to their present-day values. Earlier in Mars’ history, when the planet had a much thicker atmosphere and an active hydrosphere, carbonation is likely to have been an effective mechanism for sequestration of CO2. PMID:24149494

Clay mineral continental amplifier for marine carbon sequestration in a greenhouse ocean.

PubMed

Kennedy, Martin J; Wagner, Thomas

2011-06-14

The majority of carbon sequestration at the Earth's surface occurs in marine continental margin settings within fine-grained sediments whose mineral properties are a function of continental climatic conditions. We report very high mineral surface area (MSA) values of 300 and 570 m(2) g in Late Cretaceous black shales from Ocean Drilling Program site 959 of the Deep Ivorian Basin that vary on subcentennial time scales corresponding with abrupt increases from approximately 3 to approximately 18% total organic carbon (TOC). The observed MSA changes with TOC across multiple scales of variability and on a sample-by-sample basis (centimeter scale), provides a rigorous test of a hypothesized influence on organic carbon burial by detrital clay mineral controlled MSA. Changes in TOC also correspond with geochemical and sedimentological evidence for water column anoxia. Bioturbated intervals show a lower organic carbon loading on mineral surface area of 0.1 mg-OC m(-2) when compared to 0.4 mg-OC m(-2) for laminated and sulfidic sediments. Although either anoxia or mineral surface protection may be capable of producing TOC of < 5%, when brought together they produced the very high TOC (10-18%) apparent in these sediments. This nonlinear response in carbon burial resulted from minor precession-driven changes of continental climate influencing clay mineral properties and runoff from the African continent. This study identifies a previously unrecognized land-sea connection among continental weathering, clay mineral production, and anoxia and a nonlinear effect on marine carbon sequestration during the Coniacian-Santonian Oceanic Anoxic Event 3 in the tropical eastern Atlantic.

Serpentinite Carbonation in the Pollino Massif (southern Italy) for CO2 Sequestration

NASA Astrophysics Data System (ADS)

Carmela Dichicco, Maria; Mongelli, Giovanni; Paternoster, Michele; Rizzo, Giovanna

2015-04-01

Anthropogenic gas emissions are projected to change future climates with potentially nontrivial impacts (Keller et al., 2008 and references therein) and the impacts of the increased CO2 concentration are, among others, the greenhouse effect, the acidification of the surface of the ocean and the fertilization of ecosystems (e.g. Huijgen and Comans, 2003). Geologic Sequestration into subsurface rock formations for long-term storage is part of a process frequently referred to as "carbon capture and storage" or CCS. A major strategy for the in situ geological sequestration of CO2 involves the reaction of CO2 with Mg-silicates, especially in the form of serpentinites, which are rocks: i) relatively abundant and widely distributed in the Earth's crust, and ii) thermodynamically convenient for the formation of Mg-carbonates (e.g., Brown et al., 2011). In nature, carbonate minerals can form during serpentinization or during hydrothermal carbonation and weathering of serpentinites whereas industrial mineral carbonation processes are commonly represented by the reaction of olivine or serpentine with CO2 to form magnesite + quartz ± H2O (Power et al., 2013). Mineral carbonation occurs naturally in the subsurface as a result of fluid-rock interactions within serpentinite, which occur during serpentinization and carbonate alteration. In situ carbonation aims to promote these reactions by injecting CO2 into porous, subsurface geological formations, such as serpentinite-hosted aquifers. In the northern sector of the Pollino Massif (southern Italy) extensively occur serpentinites (Sansone et. al., 2012) and serpentinite-hosted aquifers (Margiotta et al., 2012); both serpentinites and serpentinite-hosted aquifers are the subject of a comprehensive project devoted to their possible use for in situ geological sequestration of CO2. The serpentinites derived from a lherzolitic and subordinately harzburgitic mantle, and are within tectonic slices in association with metadolerite dykes and medium to high-grade metamorphic rocks. Primary mantle minerals are olivine, clinopyroxene, orthopyroxene, and spinel whereas serpentine, magnetite, chlorite, and amphibole are pseudomorphic minerals. Olivine is replaced by serpentine forming a mesh texture and orthopyroxene is mostly altered to bastite. Water chemistry indicates serpentinites interact with meteoric water producing a Mg-HCO3 type water in a system open to CO2. Brown Jr., G.E., Calas, G., (2011) - Environmental mineralogy - understanding element behavior in ecosystems. Comptes Rendus Geoscience 343, 90-112. Huijgen W.JJ., and Comans R.N.J., (2003) - Carbon dioxide sequestrationby mineral carbonation. Report Number ECN-C-03-016, Energy research Centre of the Netherlands (ECN), Petten, the Netherlands. Keller PJ, Schmidt AD, Wittbrodt J, Stelzer EHK. (2008) - Reconstruction of zebrafish early embryonic development by scanned light sheet microscopy. Science 322: 1065-1069. Margiotta, S., Mongelli, G., Summa, V., Paternoster, M., Fiore S. (2012) - Trace element distribution and Cr(VI) speciation in Ca-HCO3 and Mg-HCO3 spring waters from the northern sector of the Pollino massif, southern Italy. Journal of Geochemical Exploration. Power I.M., Wilson S.A., Dipple G.M. (2013) - Serpentinite Carbonation for CO2 Sequestration. Elements, 9, 115-121. Sansone M.T.C., Prosser G., Rizzo G., Tartarotti P. (2012) - Spinel-peridotites of the Frido Unit ophiolites: evidence for oceanic evolution. Periodico di Mineralogia. 81, 35-59. 10.2451/2012PM0003

The Deep Carbon Cycle and CO2 Sequestration

NASA Astrophysics Data System (ADS)

Filipovitch, N. B.; Mao, W. L.; Chou, I.; Mu, K.

2009-12-01

Increased understanding of the Earth’s carbon cycle may provide insight for future carbon storage. Long term geologic sequestration of CO2 occurs in the earth via exothermic reactions between CO2 and silicate minerals to form carbonate minerals. It has been shown that while there is a large enough supply of ultra mafic igneous rock to sequester the CO2 [1], the kinetics of this natural process are too slow to effectively manage our CO2 output. Most studies have focused on studying reaction kinetics at relatively low temperatures and pressures [2,3], and have found that the reaction kinetics are either too slow or (in the case of serpentine) necessitate an uneconomical heat pretreatment [3,4]. Our experiments expand the pressures and temperatures (up to 500 bars and exceeding 200 °C) at which the CO2 + silicate reaction is studied using fused silica capillary cells and Raman and XRD analysis. By increasing our understanding of the kinetics of this process and providing a valuable input for reactive flow and transport models, these results may guide approaches for practical CO2 sequestration in carbonate minerals as a way to manage atmospheric CO2 levels. High pressure and temperature results on carbonates have implications for understanding the deep carbon cycle. Most of the previous high pressure studies on carbonates have concentrated on magnesite (MgCO3), calcite (CaCO3), or dolomite ((Ca,Mg)CO3) [5,6]. While the Mg and Ca carbonates are the most abundant, iron-rich siderite (FeCO3) may be a significant player at greater depths within the earth. We performed XRD and Raman spectroscopy experiments on siderite to lower mantle pressures (up to 40 GPa) and observed a possible phase change around 13 GPa. References 1. Lackner, Klaus S., Wendt, Christopher H., Butt, Darryl P., Joyce, Edward L., Sharp, David H., 1995, Carbon dioxide disposal in carbonate minerals, Energy, Vol.20, No. 11, pp. 1153-1170 2. Bearat, Hamdallah, McKelvy, Michael J., Chizmeshya, Andrew V.G., Gormley, Deirdre, Nunez, Ryan, Carpenter, R.W., Squires, Kyle, Wolf, George, 2006, Carbon Sequestration via Aqueous Olivine Mineral Carbonation: Role of Passivating Layer Formation, Environ. Sci. Technol., Vol. 40, pp 4802-4808 3. Wolf, George H., Chizmeshya, Andrew V. G., Diefenbacher, Jason, McKelvy, Michael J., 2004, In Situ Observation of CO2 Sequestration Reactions Using a Novel Microreaction System, Environmental Science & Technology, Vol.38, No.3, pp 932-936 4. O’Connor, W. K., Dahlin, D. C., Nilsen, D.N., Rush, G.E., Walters, R.P., and Turner, P. C., 2000, “CO2 Storage in Solid Form: A Study of Direct Mineral Carbonation,” Proc. of the 5th International Conference on Greenhouse Gas Technologies, Cairns, Australia, August 14-18, pp. 1-7 5. Isshiki, Maiko, Irifune, Tetsuo, Hirose, Kei, Ono, Shigeaki, Ohishi, Yasuo, Watanuki, Tetsu, Nishibori, Eiji, Takata, Masaki, Sakata, Makoto, 2004, Stability of magnesite and its high-pressure form in the lowermost mantle, Nature, Vol. 427, pp. 60-63 6. Kawano, Jun, Miyake, Akira, Shimobayashi, Norimasa, Kitamura, Masao, 2009, Molecular dynamics simulation of the phase transition between calcite and CaCO3-II , Journal of Physics: Condensed Matter, Vol. 21, pp. 1-11

Impact of sedimentation on wetland carbon sequestration in an agricultural watershed.

PubMed

McCarty, Gregory; Pachepsky, Yakov; Ritchie, Jerry

2009-01-01

Landscape redistribution of soil C is common within agricultural ecosystems. Little is known about the effects of upland sediment deposition on C dynamics within riparian wetlands. To assess sedimentation impact, we obtained profile samples of wetland soil and used the combination of (137)Cs, (210)Pb, and (14)C chronological markers to determine rates of C sequestration and mineral deposition over the history of a wetland within a first-order catchment under agricultural management in the coastal plains of the United States. Substantial post settlement deposition in the wetland soil was evidenced in places by a 20- to 40-cm layer of mineral soil that buried the original histosol. Soil profiles contained a minimum in C content within the top 35 cm of the profile which originated from a rapid deposition from low C upland soils. Radiocarbon and radioisotope dating showed that increases in C above this minimum were the result of C sequestered in the past approximately 50 yr. Modeling the kinetics of modern C dynamics using the (137)Cs and (210)Pb markers within these surface profiles provides strong evidence for accelerated C sequestration associated with mineral sediment deposition in the ecosystem. These findings indicate that at the landscape scale, dilution of ecosystem C by import of low C upland sediment into wetlands stimulates C sequestration by pulling soil C content below some pedogenic equilibrium value for the ecosystem. They also indicate that over the history of the wetland, rates of C accretion may be linked to mineral soil deposition.

Spatial mapping of mineralization with manganese-enhanced magnetic resonance imaging

USGS Publications Warehouse

Chesnick, I.E.; Centeno, J.A.; Todorov, T.I.; Koenig, A.E.; Potter, K.

2011-01-01

Paramagnetic manganese can be employed as a calcium surrogate to sensitize the magnetic resonance imaging (MRI) technique to the processing of calcium during the bone formation process. At low doses, after just 48h of exposure, osteoblasts take up sufficient quantities of manganese to cause marked reductions in the water proton T1 values compared with untreated cells. After just 24h of exposure, 25??M MnCl2 had no significant effect on cell viability. However, for mineralization studies 100??M MnCl2 was used to avoid issues of manganese depletion in calvarial organ cultures and a post-treatment delay of 48h was implemented to ensure that manganese ions taken up by osteoblasts is deposited as mineral. All specimens were identified by their days in vitro (DIV). Using inductively coupled plasma optical emission spectroscopy (ICP-OES), we confirmed that Mn-treated calvariae continued to deposit mineral in culture and that the mineral composition was similar to that of age-matched controls. Notably there was a significant decrease in the manganese content of DIV18 compared with DIV11 specimens, possibly relating to less manganese sequestration as a result of mineral maturation. More importantly, quantitative T1 maps of Mn-treated calvariae showed localized reductions in T1 values over the calvarial surface, indicative of local variations in the surface manganese content. This result was verified with laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). We also found that ??R1 values, calculated by subtracting the relaxation rate of Mn-treated specimens from the relaxation rate of age-matched controls, were proportional to the surface manganese content and thus mineralizing activity. From this analysis, we established that mineralization of DIV4 and DIV11 specimens occurred in all tissue zones, but was reduced for DIV18 specimens because of mineral maturation with less manganese sequestration. In DIV25 specimens, active mineralization was observed for the expanding superficial surface and ??R1 values were increased due to the mineralization of small, previously unmineralized areas. Our findings support the use of manganese-enhanced MRI (MEMRI) to study well-orchestrated mineralizing events that occur during embryonic development. In conclusion, MEMRI is more sensitive to the study of mineralization than traditional imaging approaches. ?? 2011.

Spatial mapping of mineralization with manganese-enhanced magnetic resonance imaging☆☆☆

PubMed Central

Chesnick, Ingrid E.; Centeno, Jose A.; Todorov, Todor I.; Koenig, Alan E.; Potter, Kimberlee

2011-01-01

Paramagnetic manganese can be employed as a calcium surrogate to sensitize the magnetic resonance imaging (MRI) technique to the processing of calcium during the bone formation process. At low doses, after just 48 h of exposure, osteoblasts take up sufficient quantities of manganese to cause marked reductions in the water proton T1 values compared with untreated cells. After just 24 h of exposure, 25 μM MnCl2 had no significant effect on cell viability. However, for mineralization studies 100 μM MnCl2 was used to avoid issues of manganese depletion in calvarial organ cultures and a post-treatment delay of 48 h was implemented to ensure that manganese ions taken up by osteoblasts is deposited as mineral. All specimens were identified by their days in vitro (DIV). Using inductively coupled plasma optical emission spectroscopy (ICP-OES), we confirmed that Mn-treated calvariae continued to deposit mineral in culture and that the mineral composition was similar to that of age-matched controls. Notably there was a significant decrease in the manganese content of DIV18 compared with DIV11 specimens, possibly relating to less manganese sequestration as a result of mineral maturation. More importantly, quantitative T1 maps of Mn-treated calvariae showed localized reductions in T1 values over the calvarial surface, indicative of local variations in the surface manganese content. This result was verified with laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). We also found that ΔR1 values, calculated by subtracting the relaxation rate of Mn-treated specimens from the relaxation rate of age-matched controls, were proportional to the surface manganese content and thus mineralizing activity. From this analysis, we established that mineralization of DIV4 and DIV11 specimens occurred in all tissue zones, but was reduced for DIV18 specimens because of mineral maturation with less manganese sequestration. In DIV25 specimens, active mineralization was observed for the expanding superficial surface and ΔR1 values were increased due to the mineralization of small, previously unmineralized areas. Our findings support the use of manganese-enhanced MRI (MEMRI) to study well-orchestrated mineralizing events that occur during embryonic development. In conclusion, MEMRI is more sensitive to the study of mineralization than traditional imaging approaches. PMID:21352960

Molecular modeling studies of interfacial reactions in wet supercritical CO2.

NASA Astrophysics Data System (ADS)

Glezakou, V.; McGrail, B. P.; Windisch, C. F.; Schaef, H. T.; Martin, P.

2011-12-01

In the recent years, Carbon Capture and Sequestration (CCS) technologies have gained considerable momentum in a globally organized effort to mitigate greenhouse emissions and adverse climate change. Co-sequestration refers to the capture and geologic sequestration of carbon dioxide and minor contaminants (sulfur compounds, NOx, Hg, etc.) in subsurface formations. Cosequestration offers the potential to make carbon management more economically acceptable to industry relative to sequestration of pure CO2. This may be achieved through significant savings in plant (and retrofit) capital cost, operating cost, and energy savings as well by eliminating the need for one or more individual pollutant capture systems (such as SO2 scrubbers). The latter point is important because co-sequestration may result in a net positive impact to the environment through avoided loss of power generation capacity from parasitic loads and reduced fuel needs. This paper will discuss our research on modeling, imaging and characterization of cosequestration processes and reactivity at a fundamental level. Our work examines the interactions of CO2-rich fluids with metal and mineral surfaces, and how these are affected by the presence of other gas components (e.g. SO2, H2O or NOx) commonly present in the CO2 streams. We have found that reactivity is also affected by the composition of the surface or, less obviously, by the surface exposed, for example, (104) vs (100 )of carbonate minerals. We combine experimental techniques such as XRD and Raman spectroscopy, which can detect and follow reactive processes, with ab initio modeling methods based on density functional theory, to establish a reliable correspondence between theory and experiment with predictive capability. Analysis of our molecular dynamics simulations, reveals structural information and vibrational density of states that can directly compare with XRD measurements and vibrational spectroscopy. While reactivity in CO2-containing aqueous environments has been widely studied, the reverse, i.e. reactivity in water-bearing condensed media, is not true. Our simulations show that mechanistic details in these environments can be drastically different, and they are very important in elucidating molecular transformations relevant to CCS or carbon conversion.

Sequestering CO2 in the Built Environment

NASA Astrophysics Data System (ADS)

Constantz, B. R.

2009-12-01

Calera’s Carbonate Mineralization by Aqueous Precipitation (CMAP) technology with beneficial reuse has been called, “game-changing” by Carl Pope, Director of the Sierra Club. Calera offers a solution to the scale of the carbon problem. By capturing carbon into the built environment through carbonate mineralization, Calera provides a sound and cost-effective alternative to Geologic Sequestration and Terrestrial Sequestration. The CMAP technology permanently converts carbon dioxide into a mineral form that can be stored above ground, or used as a building material. The process produces a suite of carbonate-containing minerals of various polymorphic forms. Calera product can be substituted into blends with ordinary Portland cements and used as aggregate to produce concrete with reduced carbon, carbon neutral, or carbon negative footprints. For each ton of product produced, approximately half a ton of carbon dioxide can be sequestered using the Calera process. Coal and natural gas are composed of predominately istopically light carbon, as the carbon in the fuel is plant-derived. Thus, power plant CO2 emissions have relatively low δ13C values.The carbon species throughout the CMAP process are identified through measuring the inorganic carbon content, δ13C values of the dissolved carbonate species, and the product carbonate minerals. Measuring δ13C allows for tracking the flue gas CO2 throughout the capture process. Initial analysis of the capture of propane flue gas (δ13C ˜ -25 ‰) with seawater (δ13C ˜ -10 ‰) and industrial brucite tailings from a retired magnesium oxide plant in Moss Landing, CA (δ13C ˜ -7 ‰ from residual calcite) produced carbonate mineral products with a δ13C value of ˜ -20 ‰. This isotopically light carbon, transformed from flue gas to stable carbonate minerals, can be transferred and tracked through the capture process, and finally to the built environment. CMAP provides an economical solution to global warming by producing a usable product. While the cost of this process may, in some cases, exceed the selling price of the resultant materials, the value produced combined with available carbon credits makes this CMAP technology economically and environmentally sustainable. Calera operates a pilot plant in Moss Landing, CA, which is within the Monterey Bay Marine Sanctuary. The pilot plant is complete with a coal-fired burner simulator (CFBS) and laboratory. During operation, seawater is drawn in and subsequently combined with a variety of natural and manufactured minerals. Propane or coal flue gas from the CFBS is then contacted with the slurry suspension. The precipitated minerals are separated from the seawater and are further processed to produce cement or other building materials. After the seawater flows through the Calera process, it is returned to the ocean largely unchanged, with the exception of being calcium and magnesium depleted. An overview of the process, reporting the δ13C values throughout the CMAP process, along with the risk involved in changing regulations will be presented.

CO2-rich geothermal areas in Iceland as natural analogues for geologic carbon sequestration

NASA Astrophysics Data System (ADS)

Thomas, D.; Maher, K.; Bird, D. K.; Brown, G. E.; Arnorsson, S.

2013-12-01

Geologic CO2 sequestration into mafic rocks via silicate mineral dissolution and carbonate precipitation has been suggested as a way to mitigate industrial CO2 emissions by storing CO2 in a stable form. Experimental observations of irreversible reaction of basalt with supercritical or gaseous and aqueous CO2 have resulted in carbonate precipitation, but there are no universal trends linking the extent of mineralization and type of reaction products to the bulk rock composition, glass percentage or mineralogy of the starting material. Additionally, concern exists that CO2 leakage from injection sites and migration through the subsurface may induce mineral dissolution and desorption of trace elements, potentially contaminating groundwater. This study investigates low-temperature (≤180°C) basaltic geothermal areas in Iceland with an anomalously high input of magmatic CO2 as natural analogues of the geochemical processes associated with the injection of CO2 into mafic rocks and possible leakage. Fluids that contain >4 mmol/kg total CO2 are common along the divergent Snæfellsnes Volcanic Zone in western Iceland and within the South Iceland Seismic Zone in southwest Iceland. The meteorically derived waters contain up to 80 mmol/kg dissolved inorganic carbonate (DIC). The aqueous concentration of major cations and trace elements is greater than that in Icelandic surface and groundwater and increases with DIC and decreasing pH. Concentrations of As and Ni in some samples are several times the World Health Organization (WHO) guidelines for safe drinking water. Thermodynamic modeling indicates that waters approach saturation with respect to calcite and/or aragonite, kaolinite and amorphous silica, and are undersaturated with respect to plagioclase feldspar, clinozoisite and Ca-zeolites. Petrographic study of drill cuttings from wells that intersect the CO2-rich areas indicates that the sites have undergone at least two stages of hydrothermal alteration: initial high-temperature and late stage low-temperature alteration. Imaging results from scanning electron microscopy show that calcite has replaced hydrothermally altered silicate minerals, such as albitic plagioclase. CO2-rich low-temperature fluids are not in equilibrium with correlative high-temperature hydrothermal mineral assemblages, indicating that the kinetics of mineral dissolution and secondary mineral precipitation, along with fluid residence times, are important controls on CO2 alteration and mineral formation at low temperatures. Our results have implications for predicting mineral product formation and trace element release during geologic carbon sequestration into hydrothermally altered basalts.

Clay mineral continental amplifier for marine carbon sequestration in a greenhouse ocean

PubMed Central

Kennedy, Martin J.; Wagner, Thomas

2011-01-01

The majority of carbon sequestration at the Earth’s surface occurs in marine continental margin settings within fine-grained sediments whose mineral properties are a function of continental climatic conditions. We report very high mineral surface area (MSA) values of 300 and 570 m2 g in Late Cretaceous black shales from Ocean Drilling Program site 959 of the Deep Ivorian Basin that vary on subcentennial time scales corresponding with abrupt increases from approximately 3 to approximately 18% total organic carbon (TOC). The observed MSA changes with TOC across multiple scales of variability and on a sample-by-sample basis (centimeter scale), provides a rigorous test of a hypothesized influence on organic carbon burial by detrital clay mineral controlled MSA. Changes in TOC also correspond with geochemical and sedimentological evidence for water column anoxia. Bioturbated intervals show a lower organic carbon loading on mineral surface area of 0.1 mg-OC m-2 when compared to 0.4 mg-OC m-2 for laminated and sulfidic sediments. Although either anoxia or mineral surface protection may be capable of producing TOC of < 5%, when brought together they produced the very high TOC (10–18%) apparent in these sediments. This nonlinear response in carbon burial resulted from minor precession-driven changes of continental climate influencing clay mineral properties and runoff from the African continent. This study identifies a previously unrecognized land–sea connection among continental weathering, clay mineral production, and anoxia and a nonlinear effect on marine carbon sequestration during the Coniacian-Santonian Oceanic Anoxic Event 3 in the tropical eastern Atlantic. PMID:21576498

Reaction mechanisms for enhancing carbon dioxide mineral sequestration

NASA Astrophysics Data System (ADS)

Jarvis, Karalee Ann

Increasing global temperature resulting from the increased release of carbon dioxide into the atmosphere is one of the greatest problems facing society. Nevertheless, coal plants remain the largest source of electrical energy and carbon dioxide gas. For this reason, researchers are searching for methods to reduce carbon dioxide emissions into the atmosphere from the combustion of coal. Mineral sequestration of carbon dioxide reacted in electrolyte solutions at 185°C and 2200 psi with olivine (magnesium silicate) has been shown to produce environmentally benign carbonates. However, to make this method feasible for industrial applications, the reaction rate needs to be increased. Two methods were employed to increase the rate of mineral sequestration: reactant composition and concentration were altered independently in various runs. The products were analyzed with complete combustion for total carbon content. Crystalline phases in the product were analyzed with Debye-Scherrer X-ray powder diffraction. To understand the reaction mechanism, single crystals of San Carlos Olivine were reacted in two solutions: (0.64 M NaHCO3/1 M NaCl) and (5.5 M KHCO3) and analyzed with scanning electron microscopy (SEM), transmission electron microscopy (TEM), electron energy loss spectroscopy (EELS), and fluctuation electron microscopy (FEM) to study the surface morphology, atomic crystalline structure, composition and amorphous structure. From solution chemistry studies, it was found that increasing the activity of the bicarbonate ion increased the conversion rate of carbon dioxide to magnesite. The fastest conversion, 60% conversion in one hour, occurred in a solution of 5.5 M KHCO3. The reaction product particles, magnesium carbonate, significantly increased in both number density and size on the coupon when the bicarbonate ion activity was increased. During some experiments reaction vessel corrosion also altered the mineral sequestration mechanism. Nickel ions from vessel corrosion led to nickel precipitation in the carbonate particles and the lack of an amorphous silica reaction layer on the olivine. It was concluded that nickel ions destabilized the silica passivation layer and led to faster growth of carbonate precipitates. Overall, nickel ions increased the reaction rate of mineral sequestration of carbon dioxide.

Red mud as a carbon sink: variability, affecting factors and environmental significance.

PubMed

Si, Chunhua; Ma, Yingqun; Lin, Chuxia

2013-01-15

The capacity of red mud to sequester CO(2) varied markedly due to differences in bauxite type, processing and disposal methods. Calcium carbonates were the dominant mineral phases responsible for the carbon sequestration in the investigated red mud types. The carbon sequestration capacity of red mud was not fully exploited due to shortages of soluble divalent cations for formation of stable carbonate minerals. Titanate and silicate ions were the two major oxyanions that appeared to strongly compete with carbonate ions for the available soluble Ca. Supply of additional soluble Ca and Mg could be a viable pathway for maximizing carbon sequestration in red mud and simultaneously reducing the causticity of red mud. It is roughly estimated that over 100 million tonnes of CO(2) have been unintentionally sequestered in red mud around the world to date through the natural weathering of historically produced red mud. Based on the current production rate of red mud, it is likely that some 6 million tonnes of CO(2) will be sequestered annually through atmospheric carbonation. If appropriate technologies are in place for incorporating binding cations into red mud, approximately 6 million tonnes of additional CO(2) can be captured and stored in the red mud while the hazardousness of red mud is simultaneously reduced. Copyright © 2012 Elsevier B.V. All rights reserved.

Assessing ocean alkalinity for carbon sequestration

NASA Astrophysics Data System (ADS)

Renforth, Phil; Henderson, Gideon

2017-09-01

Over the coming century humanity may need to find reservoirs to store several trillions of tons of carbon dioxide (CO2) emitted from fossil fuel combustion, which would otherwise cause dangerous climate change if it were left in the atmosphere. Carbon storage in the ocean as bicarbonate ions (by increasing ocean alkalinity) has received very little attention. Yet recent work suggests sufficient capacity to sequester copious quantities of CO2. It may be possible to sequester hundreds of billions to trillions of tons of C without surpassing postindustrial average carbonate saturation states in the surface ocean. When globally distributed, the impact of elevated alkalinity is potentially small and may help ameliorate the effects of ocean acidification. However, the local impact around addition sites may be more acute but is specific to the mineral and technology. The alkalinity of the ocean increases naturally because of rock weathering in which >1.5 mol of carbon are removed from the atmosphere for every mole of magnesium or calcium dissolved from silicate minerals (e.g., wollastonite, olivine, and anorthite) and 0.5 mol for carbonate minerals (e.g., calcite and dolomite). These processes are responsible for naturally sequestering 0.5 billion tons of CO2 per year. Alkalinity is reduced in the ocean through carbonate mineral precipitation, which is almost exclusively formed from biological activity. Most of the previous work on the biological response to changes in carbonate chemistry have focused on acidifying conditions. More research is required to understand carbonate precipitation at elevated alkalinity to constrain the longevity of carbon storage. A range of technologies have been proposed to increase ocean alkalinity (accelerated weathering of limestone, enhanced weathering, electrochemical promoted weathering, and ocean liming), the cost of which may be comparable to alternative carbon sequestration proposals (e.g., $20-100 tCO2-1). There are still many unanswered technical, environmental, social, and ethical questions, but the scale of the carbon sequestration challenge warrants research to address these.

Biogeochemical redox processes and their impact on contaminant dynamics

USGS Publications Warehouse

Borch, Thomas; Kretzschmar, Ruben; Kappler, Andreas; Van Cappellen, Philippe; Ginder-Vogel, Matthew; Campbell, Kate M.

2010-01-01

Life and element cycling on Earth is directly related to electron transfer (or redox) reactions. An understanding of biogeochemical redox processes is crucial for predicting and protecting environmental health and can provide new opportunities for engineered remediation strategies. Energy can be released and stored by means of redox reactions via the oxidation of labile organic carbon or inorganic compounds (electron donors) by microorganisms coupled to the reduction of electron acceptors including humic substances, iron-bearing minerals, transition metals, metalloids, and actinides. Environmental redox processes play key roles in the formation and dissolution of mineral phases. Redox cycling of naturally occurring trace elements and their host minerals often controls the release or sequestration of inorganic contaminants. Redox processes control the chemical speciation, bioavailability, toxicity, and mobility of many major and trace elements including Fe, Mn, C, P, N, S, Cr, Cu, Co, As, Sb, Se, Hg, Tc, and U. Redox-active humic substances and mineral surfaces can catalyze the redox transformation and degradation of organic contaminants. In this review article, we highlight recent advances in our understanding of biogeochemical redox processes and their impact on contaminant fate and transport, including future research needs.

Experimental multi-phase H2O-CO2 brine interactions at elevated temperature and pressure: Implications for CO2 sequestration in deep-saline aquifers

USGS Publications Warehouse

Rosenbauer, R.; Koksalan, T.

2004-01-01

The burning of fossil fuel and other anthropogenic activities have caused a continuous and dramatic 30% increase of atmospheric CO2 over the past 150 yr. CO2 sequestration is increasingly being viewed as a tool for managing these anthropogenic CO2 emissions to the atmosphere. CO2-saturated brine-rock experiments were carried out to evaluate the effects of multiphase H2O-CO2 fluids on mineral equilibria and the potential for CO2 sequestration in mineral phases within deep-saline aquifers. Experimental results were generally consistent with theoretical thermodynamic calculations. The solubility of CO2 was enhanced in brines in the presence of both limestone and sandstone relative to brines alone. Reactions between CO2 saturated brines and arkosic sandstones were characterized by desiccation of the brine and changes in the chemical composition of the brine suggesting fixation of CO2 in mineral phases. These reactions were occurring on a measurable but kinetically slow time scale at 120??C.

Final Report: Molecular Mechanisms of Interfacial Reactivity in Near Surface and Extreme Geochemical Environments (DE-SC0009362)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dixon, David A

2016-03-27

The prediction of the long-term stability and safety of geologic sequestration of greenhouse gases requires a detailed understanding of subsurface transport and chemical interactions between the disposed greenhouse gases and the geologic media. In this regard, mineral-fluid interactions are of prime importance since reactions that occur on or near the interface can assist in the long term sequestration of CO2 by trapping in mineral phases such as carbonates, as well as influencing the subsurface migration of the disposed fluids via creation or plugging of pores or fractures in the host rock strata. Previous research on mineral-fluid interaction for subsurface CO2more » storage has focused almost entirely on the aqueous phase, i.e., reactivity with aqueous solutions or brines containing dissolved CO2. However, interactions with neat to water-saturated non-aqueous fluids are of equal if not greater importance since supercritical CO2 (scCO2) is less dense than the aqueous phase or oil which will create a buoyant scCO2 plume that ultimately will dominate the pore volume within the caprock, and the injected scCO2 will contain water soon after injection and this water can be highly reactive. Collectively, therefore, mineral interactions with water-saturated scCO2-dominated fluids are pivotal and could result in the stable sequestration of CO2 by trapping in mineral phases such as metal carbonates within otherwise permeable zones in the caprock. The primary objective is to unravel the molecular mechanisms governing the reactivity of mineral phases important in the geologic sequestration of CO2 with variably wet supercritical carbon dioxide as a function of T, P, and mineral structure using computational chemistry. This work is in close collaboration with the PNNL Geosciences effort. The focus of the work at The University of Alabama is computational studies of the formation of magnesium and calcium carbonates and oxides and their reactivity and providing computational support of the experimental efforts at PNNL, especially for energetics, structural properties, and interpretation of spectra.« less

Experimental investigation of geochemical and mineralogical effects of CO2 sequestration on flow characteristics of reservoir rock in deep saline aquifers

PubMed Central

Rathnaweera, T. D.; Ranjith, P. G.; Perera, M. S. A.

2016-01-01

Interactions between injected CO2, brine, and rock during CO2 sequestration in deep saline aquifers alter their natural hydro-mechanical properties, affecting the safety, and efficiency of the sequestration process. This study aims to identify such interaction-induced mineralogical changes in aquifers, and in particular their impact on the reservoir rock’s flow characteristics. Sandstone samples were first exposed for 1.5 years to a mixture of brine and super-critical CO2 (scCO2), then tested to determine their altered geochemical and mineralogical properties. Changes caused uniquely by CO2 were identified by comparison with samples exposed over a similar period to either plain brine or brine saturated with N2. The results show that long-term reaction with CO2 causes a significant pH drop in the saline pore fluid, clearly due to carbonic acid (as dissolved CO2) in the brine. Free H+ ions released into the pore fluid alter the mineralogical structure of the rock formation, through the dissolution of minerals such as calcite, siderite, barite, and quartz. Long-term CO2 injection also creates a significant CO2 drying-out effect and crystals of salt (NaCl) precipitate in the system, further changing the pore structure. Such mineralogical alterations significantly affect the saline aquifer’s permeability, with important practical consequences for the sequestration process. PMID:26785912

Development of Toxicity Benchmarks and Bioaccumulation Data for N-based Organic Explosives for Terrestrial Plants and Soil Invertebrates

DTIC Science & Technology

2012-11-01

studies ................................ 205 Table 88. Distribution of the radioactivity between the soil, plant tissue, and mineralization ...the environment. The fate of these compounds is dependent upon the sum of all processes leading to their sequestration or elimination. Such...likely due to its very low concentrations in soil. 7 2.3. Effects of energetics on soil biological activity Microbes are essential components of

Geophysical Signatures to Monitor Fluids and Mineralization for CO2 Sequestration in Basalts

NASA Astrophysics Data System (ADS)

Otheim, L. T.; Adam, L.; Van Wijk, K.; Batzle, M. L.; Mcling, T. L.; Podgorney, R. K.

2011-12-01

Carbon dioxide sequestration in large reservoirs can reduce emissions of this green house gas into the atmosphere. Basalts are promising host rocks due to their volumetric extend, worldwide distribution, and recent observations that CO2-water mixtures react with basalt minerals to precipitate as carbonate minerals, trapping the CO2. The chemical reaction between carbonic acid and minerals rich in calcium, magnesium and iron precipitates carbonates in the pore space. This process would increase the elastic modulus and velocity of the rock. At the same time, the higher compressibility of CO2 over water changes the elastic properties of the rock, decreasing the saturated rock bulk modulus and the P-wave velocity. Reservoirs where the rock properties change as a result of fluid or pressure changes are commonly monitored with seismic methods. Here we present experiments to study the feasibility of monitoring CO2 migration in a reservoir and CO2-rock reactions for a sequestration scenario in basalts. Our goal is to measure the rock's elastic response to mineralization with non-contacting ultrasonic lasers, and the effect of fluid substitution at reservoir conditions at seismic and ultrasonic frequencies. For the fluid substitution experiment we observe changes in the P- and S-wave velocities when saturating the sample with super-critical (sc) CO2, CO2-water mixtures and water alone for different pore and confining pressures. The bulk modulus of the rock is significantly dependent on frequency in the 2~to 106~Hz range, for CO2-water mixtures and pure water saturations. Dry and pure CO2 (sc or gas) do not show a frequency dependence on the modulus. Moreover, the shear wave modulus is not dispersive for either fluid. The frequency dependence of the elastic parameters is related to the attenuation (1/Q) of the rock. We will show the correlation between frequency dependent moduli and attenuation data for the different elastic moduli of the rocks. Three other basalt samples were stored in a pressure chamber with a sc CO2-water solution to study the effect of mineralization on the elastic properties of the rock. The rock elastic properties are recorded with non-contacting ultrasonic lasers at room conditions. After 15 weeks the first post-mineralization scan showed differences in the rock velocities with respect to the pre-mineralization scan. The analysis is done through coda wave interferometry and direct arrivals. The samples were inserted back into the pressure vessel for continuing mineralization and subsequent scans. Finally, we will discuss the applicability of Gassmann's equation and how the combination of mineralization together with CO2-water mixture affects the velocity of waves in basalt rocks.

Enhanced convective dissolution of CO2 in reactive systems

NASA Astrophysics Data System (ADS)

de Wit, Anne; Thomas, Carelle; Loodts, Vanessa; Knaepen, Bernard; Rongy, Laurence

2017-11-01

To decrease the atmospheric concentration of CO2, sequestration techniques whereby this greenhouse gas is injected in saline aquifers present in soils are considered. Upon contact with the aquifer, the CO2 can dissolve in it and subsequently be mineralized via reactions with minerals like carbonates for instance. We investigate both experimentally and theoretically the influence of such reactions on the convective dissolution of CO2. Experiments analyze convective patterns developing when gaseous CO2 is put in contact with aqueous solutions of reactants in a confined vertical Hele-Shaw geometry. We show that the reactions can enhance convection and modify the nonlinear dynamics of density fingering. Numerical simulations further show that reactions can increase the flux of dissolving CO2, inducing a more efficient sequestration. Emphasis will be put on the control of the convective pattern properties by varying the very nature of the chemicals. Implications on the choice of optimal sequestration sites will be discussed.

The underappreciated potential of peatlands in global climate change mitigation strategies.

PubMed

Leifeld, J; Menichetti, L

2018-03-14

Soil carbon sequestration and avoidable emissions through peatland restoration are both strategies to tackle climate change. Here we compare their potential and environmental costs regarding nitrogen and land demand. In the event that no further areas are exploited, drained peatlands will cumulatively release 80.8 Gt carbon and 2.3 Gt nitrogen. This corresponds to a contemporary annual greenhouse gas emission of 1.91 (0.31-3.38) Gt CO 2 -eq. that could be saved with peatland restoration. Soil carbon sequestration on all agricultural land has comparable mitigation potential. However, additional nitrogen is needed to build up a similar carbon pool in organic matter of mineral soils, equivalent to 30-80% of the global fertilizer nitrogen application annually. Restoring peatlands is 3.4 times less nitrogen costly and involves a much smaller land area demand than mineral soil carbon sequestration, calling for a stronger consideration of peatland rehabilitation as a mitigation measure.

Brucite-driven CO2 uptake in serpentinized dunites (Ligurian Ophiolites, Montecastelli, Tuscany)

NASA Astrophysics Data System (ADS)

Boschi, Chiara; Dini, Andrea; Baneschi, Ilaria; Bedini, Federica; Perchiazzi, Natale; Cavallo, Andrea

2017-09-01

Understanding the mechanism of serpentinite weathering at low temperature - that involves carbonate formation - has become increasingly important because it represents an analog study for a cost-efficient carbon disposal strategy (i.e. carbon mineralization technology or mineral Carbon dioxide Capture and Storage, CCS). At Montecastelli (Tuscany, Italy), on-going spontaneous mineral CO2 sequestration is enhanced by brucite-rich serpentinized dunites. The dunites are embedded in brucite-free serpentinized harzburgites that belong to the ophiolitic Ligurian Units (Northern Apennine thrust-fold belt). Two main serpentinization events produced two distinct mineral assemblages in the reactive dunite bodies. The first assemblage consists of low-T pseudomorphic, mesh-textured serpentine, Fe-rich brucite (up to 20 mol.% Fe(OH)2) and minor magnetite. This was overprinted by a non-pseudomorphic, relatively high-T assemblage consisting of serpentine, Fe-poor brucite (ca. 4 mol% Fe(OH)2) and abundant magnetite. The harzburgite host rock developed a brucite-free paragenesis made of serpentine and magnetite. Present-day interaction of serpentinized dunites with slightly acidic and oxidizing meteoric water, enhances brucite dissolution and leads to precipitation of both Mg-Fe layered double hydroxides (coalingite-pyroaurite, LDHs) and hydrous Mg carbonates (hydromagnesite and nesquehonite). In contrast, the brucite-free serpentinized harzburgites are not affected by the carbonation process. In the serpentinized dunites, different carbonate minerals form depending on brucite composition (Fe-rich vs Fe-poor). Reactions in serpentinized dunites containing Fe-rich brucite produce a carbonate assemblage dominated by LDHs and minor amount of hydromagnesite. Serpentinites with a Fe-poor brucite assemblage contain large amounts of hydromagnesite and minor LDHs. Efficiency of CO2 mineral sequestration is different in the two cases owing to the distinct carbon content of LDHs (ca. 1.5 wt.%) and hydromagnesite (ca. 10 wt.%). Here, for the first time, we link the mineral composition of serpentinized ultramafic rocks to carbonate formation, concluding that Fe-poor brucite maximizes the mineral CCS efficiency.

Immobilized carbonic anhydrase on mesoporous cruciate flower-like metal organic framework for promoting CO2 sequestration.

PubMed

Ren, Sizhu; Feng, Yuxiao; Wen, Huan; Li, Conghai; Sun, Baoting; Cui, Jiandong; Jia, Shiru

2018-05-25

CO 2 capture by immobilized carbonic anhydrase (CA) has become an alternative and environmental friendly approach in CO 2 sequestration technology. However, the immobilized CA usually exhibits low CO 2 sequestration efficiency due to no gas adsorption function for the conventional CA supports. Metal organic frameworks (MOFs) are an excellent material for gas adsorption and enzyme immobilization. Herein, a combined immobilization system of CA and ZIF-8 with cruciate flower-like morphology for CO 2 adsorption was prepared for the first time by adsorbing CA onto ZIF-8. The immobilization efficiency was greater than 95%, and the maximum activity recovery reached 75%, indicating the highly efficient immobilization process. The resultant CA@ZIF-8 composites exhibited outstanding thermostability, the tolerance against denaturants, and reusability compared with free CA. Furthermore, we demonstrated for the first time that the shape of ZIF-8 could be controlled by adjusting concentrations of Zn 2+ ions at the high concentration of 2-methylimidazole (1 M). More importantly, we also demonstrated the applicability of the CA@ZIF-8 composites to the sequestration of CO 2 in carbonate minerals. The yields of the CaCO 3 obtained by using CA@ZIF-8 composites were 22-folds compared to free CA. Thus, this CA@ZIF-8 composite can be successfully used as a robust biocatalyst for sequestration of CO 2 . Copyright © 2018 Elsevier B.V. All rights reserved.

Reactivity of biogenic manganese oxide for metal sequestration and photochemistry: Computational solid state physics study (in Korean)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kwon, K.D.; Sposito, G.

2010-02-01

Many microbes, including both bacteria and fungi, produce manganese (Mn) oxides by oxidizing soluble Mn(II) to form insoluble Mn(IV) oxide minerals, a kinetically much faster process than abiotic oxidation. These biogenic Mn oxides drive the Mn cycle, coupling it with diverse biogeochemical cycles and determining the bioavailability of environmental contaminants, mainly through strong adsorption and redox reactions. This mini review introduces recent findings based on quantum mechanical density functional theory that reveal the detailed mechanisms of toxic metal adsorption at Mn oxide surfaces and the remarkable role of Mn vacancies in the photochemistry of these minerals.

Interplay between black carbon and minerals contributes to long term carbon stabilization and mineral transformation

NASA Astrophysics Data System (ADS)

Liang, B.; Weng, Y. T.; Wang, C. C.; Chiang, C. C.; Liu, C. C.; Lehmann, J.

2017-12-01

Black carbon receives increasing global wide research attention due to its role in carbon sequestration, soil fertility enhancement and remediation application. Generally considered chemically stable in bulk, the reactive surface of BC can interplays with minerals and form strong chemical bondage, which renders physical protection of BC and contributes to its long term stabilization. Using historical BC-rich Amazonian Dark Earth (ADE), we probe the in-situ organo-mineral association and transformation of BC and minerals over a millennium scale using various synchrotron-based spectroscopic (XANES, FTIR) and microscopic (TXM) methods. Higher content of SRO minerals was found in BC-rich ADE compare to adjacent tropical soils. The iron signature found in BC-rich ADE was mainly ferrihydrite/lepidocrocite, a more reactive form of Fe compared to goethite, which was dominant in adjacent soil. Abundant nano minerals particles were observed in-situ associated with BC surface, in clusters and layers. The organo-mineral interaction lowers BC bioavailability and enhances its long-term stabilization in environment, while at the same time, transforms associated minerals into more reactive forms under rapid redox/weathering environment. The results suggest that mineral physical protection for BC sequestration may be more important than previous understanding. The scale up application of BC/biochar into agricultural systems and natural environments have long lasting impact on the in-situ transformation of associated minerals.

How much will afforestation of former cropland influence soil C stocks? A synthesis of paired sampling, chronosequence sampling and repeated sampling studies

NASA Astrophysics Data System (ADS)

Vesterdal, Lars; Hansen, K.; Stupak, I.; Don, Axel; Poeplau, C.; Leifeld, Jens; van Wesemael, Bas

2010-05-01

The need for documentation of land-use change effects on soil C is high on the agenda in most signatory countries to the Kyoto Protocol. Large land areas in Europe have experienced land-use change from cropland to forest since 1990 by direct afforestation as well as abandonment and regrowth of marginally productive cropland. Soil C dynamics following land-use change remain highly uncertain due to a limited number of available studies and due to influence of interacting factors such as land use history, soil type, and climate. Common approaches for estimation of potential soil C changes following land-use change are i) paired sampling of plots with a long legacy of different land uses, ii) chronosequence studies of land-use change, and lastly iii) repeated sampling of plots subject to changed land use. This paper will synthesize the quantitative effects of cropland afforestation on soil C sequestration based on all three approaches and will report on related work within Cost 639. Paired plots of forest and cropland were used to study the general differences between soil C stocks in the two land uses. At 27 sites in Denmark distributed among different regions and soil types forest floor and mineral soil were sampled in and around soil pits. Soil C stocks were higher in forest than cropland (mean difference 22 Mg C ha-1 to 1 m depth). This difference was caused solely by the presence of a forest floor in forests; mineral soil C stocks were similar (108 vs. 109 Mg C ha-1) in the two land uses regardless of soil type and the soil layers considered. The chronosequence approach was employed in the AFFOREST project for evaluation of C sequestration in biomass and soils following afforestation of cropland. Two oak (Quercus robur) and four Norway spruce (Picea abies) afforestation chronosequences (age range 1 to 90 years) were studied in Denmark, Sweden and the Netherlands. Forest floor and mineral soil (0-25 cm) C contents were as a minimum unchanged and in most cases there was net C sequestration (range 0-1.3 Mg C ha-1 yr-1). The allocation of sequestered soil C was quite different among chronosequences; forest floors consistently sequestered C (0.1-0.7 Mg C ha-1 yr-1) but there was no general pattern in mineral soil C sequestration. While the paired sampling and the chronosequence approaches both may be confounded by site factors other than the land use, repeated sampling of plots best addresses the pure land-use change effect. Repeated sampling after 18 years was done in a systematic 7x7 km grid to address soil C changes in 15 cropland plots that were converted to forest (7-22 years since afforestation). Consistent with the other two approaches, detectable soil C changes were confined to the forest floor component; forest floor C sequestration rates were 0.24 Mg C ha-1 yr-1 while no changes were detected for mineral soils. The three approaches to estimation of soil C sequestration indeed point to a common conclusion: The potential for soil C sequestration is mainly confined to the forest floor whereas notable C sequestration is less likely to occur in the mineral soil. However, more generalizable knowledge is badly needed for reporting of land-use change effects on mineral soil C pools. WG II of Cost 639 and the FP7 project GHG Europe is currently establishing a database of LUC studies. This database will be used to establish so-called Carbon Response Functions (CRF), i.e. simple models predicting the annual rate of change in soil C pools. These CRFs may serve as tools for syntheses of land-use change effects for Europe as well as for improved reporting of soil C dynamics following land-use change.

Toxicity screening of biochar-mineral composites using germination tests.

PubMed

Mumme, Jan; Getz, Josephine; Prasad, Munoo; Lüder, Ulf; Kern, Jürgen; Mašek, Ondřej; Buss, Wolfram

2018-05-08

This study assessed the properties and toxicity (water cress germination trials) of 38 waste-derived, novel biochar-mineral composites (BMCs) produced via slow pyrolysis and hydrothermal carbonization (hydrochars). The biochars were produced from sewage sludge and compost-like output (CLO) by varying the type of mineral additive (zeolite, wood ash and lignite fly ash), the mineral-to-feedstock ratio and the carbonization process. While pure hydrochars completely inhibited germination of water cress, this effect was ameliorated by mineral additives. Seedlings grew best in pyrolysis chars and while wood ash addition decreased plant growth in many cases, 1:10 addition to CLO doubled germination rate. The factors responsible for the phytotoxicity can be attributed to pH, salinity and organic contaminants. Importantly, while pure minerals inhibited germination, conversion of minerals into BMCs reduced their inhibitory effects due to buffered release of minerals. Overall, mineral wastes (e.g., combustion ashes) and waste biomass can be used safely as sources of nutrients and stable organic carbon (for soil carbon sequestration) when converted into specific biochar-mineral composites, exploiting synergies between the constituents to deliver superior performance. Copyright © 2018 Elsevier Ltd. All rights reserved.

Photochemical mineralization of europium, titanium, and iron oxyhydroxide nanoparticles in the ferritin protein cage.

PubMed

Klem, Michael T; Mosolf, Jesse; Young, Mark; Douglas, Trevor

2008-04-07

The Fe storage protein ferritin was used as a size-constrained reaction vessel for the photoreduction and reoxidation of complexed Eu, Fe, and Ti precursors for the formation of oxyhydroxide nanoparticles. The resultant materials were characterized by dynamic light scattering, gel electrophoresis, UV-vis spectroscopy, and transmission electron microscopy. The photoreduction and reoxidation process is inspired by biological sequestration mechanisms observed in some marine siderophore systems.

Soil Organic Carbon Loss: An Overlooked Factor in the Carbon Sequestration Potential of Enhanced Mineral Weathering

NASA Astrophysics Data System (ADS)

Dietzen, Christiana; Harrison, Robert

2016-04-01

Weathering of silicate minerals regulates the global carbon cycle on geologic timescales. Several authors have proposed that applying finely ground silicate minerals to soils, where organic acids would enhance the rate of weathering, could increase carbon uptake and mitigate anthropogenic CO2 emissions. Silicate minerals such as olivine could replace lime, which is commonly used to remediate soil acidification, thereby sequestering CO2 while achieving the same increase in soil pH. However, the effect of adding this material on soil organic matter, the largest terrestrial pool of carbon, has yet to be considered. Microbial biomass and respiration have been observed to increase with decreasing acidity, but it is unclear how long the effect lasts. If the addition of silicate minerals promotes the loss of soil organic carbon through decomposition, it could significantly reduce the efficiency of this process or even create a net carbon source. However, it is possible that this initial flush of microbial activity may be compensated for by additional organic matter inputs to soil pools due to increases in plant productivity under less acidic conditions. This study aimed to examine the effects of olivine amendments on soil CO2 flux. A liming treatment representative of typical agricultural practices was also included for comparison. Samples from two highly acidic soils were split into groups amended with olivine or lime and a control group. These samples were incubated at 22°C and constant soil moisture in jars with airtight septa lids. Gas samples were extracted periodically over the course of 2 months and change in headspace CO2 concentration was determined. The effects of enhanced mineral weathering on soil organic matter have yet to be addressed by those promoting this method of carbon sequestration. This project provides the first data on the potential effects of enhanced mineral weathering in the soil environment on soil organic carbon pools.

Numerically Simulating Carbonate Mineralization of Basalt with Injection of Carbon Dioxide into Deep Saline Formations

DOE Office of Scientific and Technical Information (OSTI.GOV)

White, Mark D.; McGrail, B. Peter; Schaef, Herbert T.

2006-07-08

The principal mechanisms for the geologic sequestration of carbon dioxide in deep saline formations include geological structural trapping, hydrological entrapment of nonwetting fluids, aqueous phase dissolution and ionization, and geochemical sorption and mineralization. In sedimentary saline formations the dominant mechanisms are structural and dissolution trapping, with moderate to weak contributions from hydrological and geochemical trapping; where, hydrological trapping occurs during the imbibition of aqueous solution into pore spaces occupied by gaseous carbon dioxide, and geochemical trapping is controlled by generally slow reaction kinetics. In addition to being globally abundant and vast, deep basaltic lava formations offer mineralization kinetics that makemore » geochemical trapping a dominate mechanism for trapping carbon dioxide in these formations. For several decades the United States Department of Energy has been investigating Columbia River basalt in the Pacific Northwest as part of its environmental programs and options for natural gas storage. Recently this nonpotable and extensively characterized basalt formation is being reconsidered as a potential reservoir for geologic sequestration of carbon dioxide. The reservoir has an estimated storage capacity of 100 giga tonnes of carbon dioxide and comprises layered basalt flows with sublayering that generally alternates between low permeability massive and high permeability breccia. Chemical analysis of the formation shows 10 wt% Fe, primarily in the +2 valence. The mineralization reaction that makes basalt formations attractive for carbon dioxide sequestration is that of calcium, magnesium, and iron silicates reacting with dissolved carbon dioxide, producing carbonate minerals and amorphous quartz. Preliminary estimates of the kinetics of the silicate-to-carbonate reactions have been determined experimentally and this research is continuing to determine effects of temperature, pressure, rock composition and mineral assemblages on the reaction rates. This study numerically investigates the injection, migration and sequestration of supercritical carbon dioxide in deep Columbia River basalt formations using the multifluid subsurface flow and reactive transport simulator STOMP-CO2 with its ECKEChem module. Simulations are executed on high resolution multiple stochastic realizations of the layered basalt systems and demonstrate the migration behavior through layered basalt formations and the mineralization of dissolved carbon dioxide. Reported results include images of the migration behavior, distribution of carbonate formation, quantities of injected and sequestered carbon dioxide, and percentages of the carbon dioxide sequestered by different mechanisms over time.« less

Developing a Robust Geochemical and Reactive Transport Model to Evaluate Possible Sources of Arsenic at the CO2 Sequestration Natural Analog Site in Chimayo, New Mexico

EPA Science Inventory

Migration of carbon dioxide (CO₂) from deep storage formations into shallow drinking water aquifers is a possible system failure related to geologic CO₂ sequestration. A CO₂ leak may cause mineral precipitation/dissolution reactions, changes in a...

Investigation of the relationship between CO2 reservoir rock property change and the surface roughness change originating from the supercritical CO2-sandstone-groundwater geochemical reaction at CO2 sequestration condition

NASA Astrophysics Data System (ADS)

Lee, Minhee; Wang, Sookyun; Kim, Seyoon; Park, Jinyoung

2015-04-01

Lab scale experiments were performed to investigate the property changes of sandstone slabs and cores, resulting from the scCO2-rock-groundwater reaction for 180 days under CO2 sequestration conditions (100 bar and 50 °C). The geochemical reactions, including the surface roughness change of minerals in the slab, resulted from the dissolution and the secondary mineral precipitation for the sandstone reservoir of the Gyeongsang basin, Korea were reproduced in laboratory scale experiments and the relationship between the geochemical reaction and the physical rock property change was derived, for the consideration of successful subsurface CO2 sequestration. The use of the surface roughness value (SRrms) change rate and the physical property change rate to quantify scCO2-rock-groundwater reaction is the novel approach on the study area for CO2 sequestration in the subsurface. From the results of SPM (Scanning Probe Microscope) analyses, the SRrms for each sandstone slab was calculated at different reaction time. The average SRrms increased more than 3.5 times during early 90 days reaction and it continued to be steady after 90 days, suggesting that the surface weathering process of sandstone occurred in the early reaction time after CO2 injection into the subsurface reservoir. The average porosity of sandstone cores increased by 8.8 % and the average density decreased by 0.5 % during 90 days reaction and these values slightly changed after 90 days. The average P and S wave velocities of sandstone cores also decreased by 10 % during 90 days reaction. The trend of physical rock property change during the geochemical reaction showed in a logarithmic manner and it was also correlated to the logarithmic increase in SRrms, suggesting that the physical property change of reservoir rocks originated from scCO2 injection directly comes from the geochemical reaction process. Results suggested that the long-term estimation of the physical property change for reservoir rocks in CO2 injection site could be possible from the extrapolation process of SRrms and rocks property change rates, acquired from laboratory scale experiments. It will be aslo useful to determine the favorite CO2 injection site from the viewpoint of the safety.

Structure-dependent interactions between alkali feldspars and organic compounds: implications for reactions in geologic carbon sequestration.

PubMed

Yang, Yi; Min, Yujia; Jun, Young-Shin

2013-01-02

Organic compounds in deep saline aquifers may change supercritical CO(2) (scCO(2))-induced geochemical processes by attacking specific components in a mineral's crystal structure. Here we investigate effects of acetate and oxalate on alkali feldspar-brine interactions in a simulated geologic carbon sequestration (GCS) environment at 100 atm of CO(2) and 90 °C. We show that both organics enhance the net extent of feldspar's dissolution, with oxalate showing a more prominent effect than acetate. Further, we demonstrate that the increased reactivity of Al-O-Si linkages due to the presence of oxalate results in the promotion of both Al and Si release from feldspars. As a consequence, the degree of Al-Si order may affect the effect of oxalate on feldspar dissolution: a promotion of ~500% in terms of cumulative Si concentration was observed after 75 h of dissolution for sanidine (a highly disordered feldspar) owing to oxalate, while the corresponding increase for albite (a highly ordered feldspar) was ~90%. These results provide new insights into the dependence of feldspar dissolution kinetics on the crystallographic properties of the mineral under GCS conditions.

CO2 sequestration: Storage capacity guideline needed

USGS Publications Warehouse

Frailey, S.M.; Finley, R.J.; Hickman, T.S.

2006-01-01

Petroleum reserves are classified for the assessment of available supplies by governmental agencies, management of business processes for achieving exploration and production efficiency, and documentation of the value of reserves and resources in financial statements. Up to the present however, the storage capacity determinations made by some organizations in the initial CO2 resource assessment are incorrect technically. New publications should thus cover differences in mineral adsorption of CO2 and dissolution of CO2 in various brine waters.

Vacuolar sequestration capacity and long-distance metal transport in plants

PubMed Central

Peng, Jia-Shi; Gong, Ji-Ming

2014-01-01

The vacuole is a pivotal organelle functioning in storage of metabolites, mineral nutrients, and toxicants in higher plants. Accumulating evidence indicates that in addition to its storage role, the vacuole contributes essentially to long-distance transport of metals, through the modulation of Vacuolar sequestration capacity (VSC) which is shown to be primarily controlled by cytosolic metal chelators and tonoplast-localized transporters, or the interaction between them. Plants adapt to their environments by dynamic regulation of VSC for specific metals and hence targeting metals to specific tissues. Study of VSC provides not only a new angle to understand the long-distance root-to-shoot transport of minerals in plants, but also an efficient way to biofortify essential mineral nutrients or to phytoremediate non-essential metal pollution. The current review will focus on the most recent proceedings on the interaction mechanisms between VSC regulation and long-distance metal transport. PMID:24550927

Vacuolar sequestration capacity and long-distance metal transport in plants.

PubMed

Peng, Jia-Shi; Gong, Ji-Ming

2014-01-01

The vacuole is a pivotal organelle functioning in storage of metabolites, mineral nutrients, and toxicants in higher plants. Accumulating evidence indicates that in addition to its storage role, the vacuole contributes essentially to long-distance transport of metals, through the modulation of Vacuolar sequestration capacity (VSC) which is shown to be primarily controlled by cytosolic metal chelators and tonoplast-localized transporters, or the interaction between them. Plants adapt to their environments by dynamic regulation of VSC for specific metals and hence targeting metals to specific tissues. Study of VSC provides not only a new angle to understand the long-distance root-to-shoot transport of minerals in plants, but also an efficient way to biofortify essential mineral nutrients or to phytoremediate non-essential metal pollution. The current review will focus on the most recent proceedings on the interaction mechanisms between VSC regulation and long-distance metal transport.

Assessing the Impact of Afforestation on Soil Organic C Sequestration by Means of Sequential Density Fractionation

PubMed Central

Cong, Weiwei; Ren, Tusheng; Li, Baoguo

2015-01-01

Afforestation is a prevalent practice carried out for soil recovery and carbon sequestration. Improved understanding of the effects of afforestation on soil organic carbon (SOC) content and dynamics is necessary to identify the particular processes of soil organic matter (SOM) formation and/or decomposition that result from afforestation. To elucidate these mechanisms, we have used a sequential density fractionation technique to identify the transfer mechanisms of forest derived C to soil fractions and investigate the impact of afforestation on SOC sequestration. Surface soil samples from continuous maize crop land (C4) and forest land (C3), which had been established 5, 12 and 25 yr, respectively, on the Northeast China Plain were separated into five density fractions. SOC, nitrogen (N) concentration and δ13C data from the three forests and adjacent cropland were compared. Afforestation decreased SOC concentration in the < 2.5 g cm-3 fractions from 5 yr forest sites, but increased SOC content in the < 2.0 g cm-3 fractions from 25 yr forest sites. Afforestation did not affect soil mass distribution, SOC and N proportional weight distributions across the density fractions. The < 1.8 g cm-3 fractions from 12 and 25 yr forests showed higher C/N and lower δ13C as compared to other fractions. Incorporation of forest litter-derived C occurred from low density (< 1.8 g cm-3) fractions to aggregates of higher density (1.8-2.5 g cm-3) through aggregate recombination and C transport in the pore system of the aggregates. Some forest litter-derived C could transfer from the light fractions or directly diffuse and adsorb onto mineral particles. Results from this study indicate that microaggregate protection and association between organic material and minerals provide major contribution to the SOC sequestration in the afforested soil system. PMID:25705896

Chemical effects of carbon dioxide sequestration in the Upper Morrow Sandstone in the Farnsworth, Texas, hydrocarbon unit

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ahmmed, Bulbul; Appold, Martin S.; Fan, Tianguang

Numerical geochemical modeling was used to study the effects on pore-water composition and mineralogy from carbon dioxide (CO2) injection into the Pennsylvanian Morrow B Sandstone in the Farnsworth Unit in northern Texas to evaluate its potential for long-term CO2 sequestration. Speciation modeling showed the present Morrow B formation water to be supersaturated with respect to an assemblage of zeolite, clay, carbonate, mica, and aluminum hydroxide minerals and quartz. The principal accessory minerals in the Morrow B, feldspars and chlorite, were predicted to dissolve. A reaction-path model in which CO2 was progressively added up to its solubility limit into the Morrowmore » B formation water showed a decrease in pH from its initial value of 7 to approximately 4.1 to 4.2, accompanied by the precipitation of small amounts of quartz, diaspore, and witherite. As the resultant CO2-charged fluid reacted with more of the Morrow B mineral matrix, the model predicted a rise in pH, reaching a maximum of 5.1 to 5.2 at a water–rock ratio of 10:1. At a higher water–rock ratio of 100:1, the pH rose to only 4.6 to 4.7. Diaspore, quartz, and nontronite precipitated consistently regardless of the water–rock ratio, but the carbonate minerals siderite, witherite, dolomite, and calcite precipitated at higher pH values only. As a result, CO2 sequestration by mineral trapping was predicted to be important only at low water–rock ratios, accounting for a maximum of 2% of the added CO2 at the lowest water–rock ratio investigated of 10:1, which corresponds to a small porosity increase of approximately 0.14% to 0.15%.« less

Long-term nitrogen regulation of forest carbon sequestration

NASA Astrophysics Data System (ADS)

Yang, Y.; Luo, Y.

2009-12-01

It is well established that nitrogen (N) limits plant production but unclear how N regulates long-term terrestrial carbon (C) sequestration in response to rising atmospheric C dioxide (CO2)(Luo et al., 2004). Most experimental evidence on C-N interactions is primarily derived from short-term CO2 manipulative studies (e.g. Oren et al., 2001; Reich et al., 2006a), which abruptly increase C inputs into ecosystems and N demand from soil while atmospheric CO2 concentration in the real world is gradually increasing over time (Luo & Reynolds, 1999). It is essential to examine long-term N regulations of C sequestration in natural ecosystems. Here we present results of a synthesis of more than 100 studies on long-term C-N interactions during secondary succession. C significantly accumulates in plant, litter and forest floor in most studies, and in mineral soil in one-third studies during stand development. Substantial increases in C stock are tightly coupled with N accretion. The C: N ratio in plant increases with stand age in most cases, but remains relatively constant in litter, forest floor and mineral soil. Our results suggest that natural ecosystems could have the intrinsic capacity to maintain long-term C sequestration through external N accrual, high N use efficiency, and efficient internal N cycling.

Carbon sequestration in depleted oil shale deposits

DOEpatents

Burnham, Alan K; Carroll, Susan A

2014-12-02

A method and apparatus are described for sequestering carbon dioxide underground by mineralizing the carbon dioxide with coinjected fluids and minerals remaining from the extraction shale oil. In one embodiment, the oil shale of an illite-rich oil shale is heated to pyrolyze the shale underground, and carbon dioxide is provided to the remaining depleted oil shale while at an elevated temperature. Conditions are sufficient to mineralize the carbon dioxide.

Potential for U sequestration with select minerals and sediments via base treatment.

PubMed

Emerson, Hilary P; Di Pietro, Silvina; Katsenovich, Yelena; Szecsody, Jim

2018-06-13

Temporary base treatment is a potential remediation technique for heavy metals through adsorption, precipitation, and co-precipitation with minerals. Manipulation of pH with ammonia gas injection may be especially useful for vadose zone environments as it does not require addition of liquids that would increase the flux towards groundwater. In this research, we conducted laboratory batch experiments to evaluate the changes in uranium mobility and mineral dissolution with base treatments including sodium hydroxide, ammonium hydroxide, and ammonia gas. Our data show that partitioning of uranium to the solid phase increases by several orders of magnitude following base treatment in the presence of different minerals and natural sediments from the Hanford site. The presence of dissolved calcium and carbonate play an important role in precipitation and co-precipitation of uranium at elevated pH. In addition, significant incongruent dissolution of bulk mineral phases occurs and likely leads to precipitation of secondary mineral phases. These secondary phases may remove uranium via adsorption, precipitation, and co-precipitation processes and may coat uranium phases with low solubility minerals as the pH returns to natural conditions. Copyright © 2018 Elsevier Ltd. All rights reserved.

Engineered Escherichia coli with Periplasmic Carbonic Anhydrase as a Biocatalyst for CO2 Sequestration

PubMed Central

Jo, Byung Hoon; Kim, Im Gyu; Seo, Jeong Hyun; Kang, Dong Gyun

2013-01-01

Carbonic anhydrase is an enzyme that reversibly catalyzes the hydration of carbon dioxide (CO2). It has been suggested recently that this remarkably fast enzyme can be used for sequestration of CO2, a major greenhouse gas, making this a promising alternative for chemical CO2 mitigation. To promote the economical use of enzymes, we engineered the carbonic anhydrase from Neisseria gonorrhoeae (ngCA) in the periplasm of Escherichia coli, thereby creating a bacterial whole-cell catalyst. We then investigated the application of this system to CO2 sequestration by mineral carbonation, a process with the potential to store large quantities of CO2. ngCA was highly expressed in the periplasm of E. coli in a soluble form, and the recombinant bacterial cell displayed the distinct ability to hydrate CO2 compared with its cytoplasmic ngCA counterpart and previously reported whole-cell CA systems. The expression of ngCA in the periplasm of E. coli greatly accelerated the rate of calcium carbonate (CaCO3) formation and exerted a striking impact on the maximal amount of CaCO3 produced under conditions of relatively low pH. It was also shown that the thermal stability of the periplasmic enzyme was significantly improved. These results demonstrate that the engineered bacterial cell with periplasmic ngCA can successfully serve as an efficient biocatalyst for CO2 sequestration. PMID:23974145

Variations in soil carbon sequestration and their determinants along a precipitation gradient in seasonally dry tropical forest ecosystems.

PubMed

Campo, Julio; Merino, Agustín

2016-05-01

The effect of precipitation regime on the C cycle of tropical forests is poorly understood, despite the existence of models that suggest a drier climate may substantially alter the source-sink function of these ecosystems. Along a precipitation regime gradient containing 12 mature seasonally dry tropical forests growing under otherwise similar conditions (similar annual temperature, rainfall seasonality, and geological substrate), we analyzed the influence of variation in annual precipitation (1240 to 642 mm) and duration of seasonal drought on soil C. We investigated litterfall, decomposition in the forest floor, and C storage in the mineral soil, and analyzed the dependence of these processes and pools on precipitation. Litterfall decreased slightly - about 10% - from stands with 1240 mm yr(-1) to those with 642 mm yr(-1), while the decomposition decreased by 56%. Reduced precipitation strongly affected C storage and basal respiration in the mineral soil. Higher soil C storage at the drier sites was also related to the higher chemical recalcitrance of litter (fine roots and forest floor) and the presence of charcoal across sites, suggesting an important indirect influence of climate on C sequestration. Basal respiration was controlled by the amount of recalcitrant organic matter in the mineral soil. We conclude that in these forest ecosystems, the long-term consequences of decreased precipitation would be an increase in organic layer and mineral soil C storage, mainly due to lower decomposition and higher chemical recalcitrance of organic matter, resulting from changes in litter composition and, likely also, wildfire patterns. This could turn these seasonally dry tropical forests into significant soil C sinks under the predicted longer drought periods if primary productivity is maintained. © 2016 John Wiley & Sons Ltd.

Subarctic weathering of mineral wastes provides a sink for atmospheric CO(2).

PubMed

Wilson, Siobhan A; Dipple, Gregory M; Power, Ian M; Barker, Shaun L L; Fallon, Stewart J; Southam, Gordon

2011-09-15

The mineral waste from some mines has the capacity to trap and store CO(2) within secondary carbonate minerals via the process of silicate weathering. Nesquehonite [MgCO(3)·3H(2)O] forms by weathering of Mg-silicate minerals in kimberlitic mine tailings at the Diavik Diamond Mine, Northwest Territories, Canada. Less abundant Na- and Ca-carbonate minerals precipitate from sewage treatment effluent deposited in the tailings storage facility. Radiocarbon and stable carbon and oxygen isotopes are used to assess the ability of mine tailings to trap and store modern CO(2) within these minerals in the arid, subarctic climate at Diavik. Stable isotopic data cannot always uniquely identify the source of carbon stored within minerals in this setting; however, radiocarbon isotopic data provide a reliable quantitative estimate for sequestration of modern carbon. At least 89% of the carbon trapped within secondary carbonate minerals at Diavik is derived from a modern source, either by direct uptake of atmospheric CO(2) or indirect uptake though the biosphere. Silicate weathering at Diavik is trapping 102-114 g C/m(2)/y within nesquehonite, which corresponds to a 2 orders of magnitude increase over the background rate of CO(2) uptake predicted from arctic and subarctic river catchment data.

Barriers and Prospects of Carbon Sequestration in India.

PubMed

Gupta, Anjali; Nema, Arvind K

2014-04-01

Carbon sequestration is considered a leading technology for reducing carbon dioxide (CO2) emissions from fossil-fuel based electricity generating power plants and could permit the continued use of coal and gas whilst meeting greenhouse gas targets. India will become the world's third largest emitter of CO2 by 2015. Considering the dependence of health of the Indian global economy, there is an imperative need to develop a global approach which could address the capturing and securely storing carbon dioxide emitted from an array of energy. Therefore technology such as carbon sequestration will deliver significant CO2 reductions in a timely fashion. Considerable energy is required for the capture, compression, transport and storage steps. With the availability of potential technical storage methods for carbon sequestration like forest, mineral and geological storage options with India, it would facilitate achieving stabilization goal in the near future. This paper examines the potential carbon sequestration options available in India and evaluates them with respect to their strengths, weakness, threats and future prospects.

CO 2 Absorption and Magnesium Carbonate Precipitation in MgCl 2–NH 3–NH 4Cl Solutions: Implications for Carbon Capture and Storage

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhu, Chen; Wang, Han; Li, Gen

CO 2 absorption and carbonate precipitation are the two core processes controlling the reaction rate and path of CO 2 mineral sequestration. Whereas previous studies have focused on testing reactive crystallization and precipitation kinetics, much less attention has been paid to absorption, the key process determining the removal efficiency of CO 2. In this study, adopting a novel wetted wall column reactor, we systematically explore the rates and mechanisms of carbon transformation from CO 2 gas to carbonates in MgCl 2–NH 3–NH 4Cl solutions. We find that reactive diffusion in liquid film of the wetted wall column is the rate-limitingmore » step of CO 2 absorption when proceeding chiefly through interactions between CO 2(aq) and NH 3(aq). We further quantified the reaction kinetic constant of the CO 2–NH 3 reaction. Our results indicate that higher initial concentration of NH 4Cl ( ≥2mol∙L -1) leads to the precipitation of roguinite [(NH 4) 2Mg(CO 3) 2∙4H 2O], while nesquehonite appears to be the dominant Mg-carbonate without NH 4Cl addition. We also noticed dypingite formation via phase transformation in hot water. This study provides new insight into the reaction kinetics of CO 2 mineral carbonation that indicates the potential of this technique for future application to industrial-scale CO 2 sequestration.« less

CO 2 Absorption and Magnesium Carbonate Precipitation in MgCl 2–NH 3–NH 4Cl Solutions: Implications for Carbon Capture and Storage

DOE PAGES

Zhu, Chen; Wang, Han; Li, Gen; ...

2017-09-19

CO 2 absorption and carbonate precipitation are the two core processes controlling the reaction rate and path of CO 2 mineral sequestration. Whereas previous studies have focused on testing reactive crystallization and precipitation kinetics, much less attention has been paid to absorption, the key process determining the removal efficiency of CO 2. In this study, adopting a novel wetted wall column reactor, we systematically explore the rates and mechanisms of carbon transformation from CO 2 gas to carbonates in MgCl 2–NH 3–NH 4Cl solutions. We find that reactive diffusion in liquid film of the wetted wall column is the rate-limitingmore » step of CO 2 absorption when proceeding chiefly through interactions between CO 2(aq) and NH 3(aq). We further quantified the reaction kinetic constant of the CO 2–NH 3 reaction. Our results indicate that higher initial concentration of NH 4Cl ( ≥2mol∙L -1) leads to the precipitation of roguinite [(NH 4) 2Mg(CO 3) 2∙4H 2O], while nesquehonite appears to be the dominant Mg-carbonate without NH 4Cl addition. We also noticed dypingite formation via phase transformation in hot water. This study provides new insight into the reaction kinetics of CO 2 mineral carbonation that indicates the potential of this technique for future application to industrial-scale CO 2 sequestration.« less

Spatial Associations and Chemical Composition of Organic Carbon Sequestered in Fe, Ca, and Organic Carbon Ternary Systems.

PubMed

Sowers, Tyler D; Adhikari, Dinesh; Wang, Jian; Yang, Yu; Sparks, Donald L

2018-05-25

Organo-mineral associations of organic carbon (OC) with iron (Fe) oxides play a major role in environmental OC sequestration, a process crucial to mitigating climate change. Calcium has been found to have high coassociation with OC in soils containing high Fe content, increase OC sorption extent to poorly crystalline Fe oxides, and has long been suspected to form bridging complexes with Fe and OC. Due to the growing realization that Ca may be an important component of C cycling, we launched a scanning transmission X-ray microscopy (STXM) investigation, paired with near-edge X-ray absorption fine structure (NEXAFS) spectroscopy, in order to spatially resolve Fe, Ca, and OC relationships and probe the effect of Ca on sorbed OC speciation. We performed STXM-NEXAFS analysis on 2-line ferrihydrite reacted with leaf litter-extractable dissolved OC and citric acid in the absence and presence of Ca. Organic carbon was found to highly associate with Ca ( R 2 = 0.91). Carboxylic acid moieties were dominantly sequestered; however, Ca facilitated the additional sequestration of aromatic and phenolic moieties. Also, C NEXAFS revealed polyvalent metal ion complexation. Our results provide evidence for the presence of Fe-Ca-OC ternary complexation, which has the potential to significantly impact how organo-mineral associations are modeled.

Can a fractured caprock self-heal?

NASA Astrophysics Data System (ADS)

Elkhoury, Jean E.; Detwiler, Russell L.; Ameli, Pasha

2015-05-01

The ability of geologic seals to prevent leakage of fluids injected into the deep subsurface is critical for mitigating risks associated with greenhouse-gas sequestration and natural-gas production. Fractures caused by tectonic or injection-induced stresses create potential leakage pathways that may be further enhanced by mineral dissolution. We present results from reactive-flow experiments in fractured caprock (dolomitic anhydrite), where additional dissolution occurs in the rock matrix adjacent to the fracture surfaces. Preferential dissolution of anhydrite left a compacted layer of dolomite in the fractures. At lower flow rate, rock-fluid reactions proceeded to near equilibrium within the fracture with preferential flow paths persisting over the 6-month duration of the experiment and a negligible change in permeability. At higher flow rate, permeability decreased by a dramatic two orders of magnitude. This laboratory-scale observation of self-healing argues against the likelihood of runaway permeability growth in fractured porous caprock composed of minerals with different solubilities and reaction kinetics. However, scaling arguments suggest that at larger length scales this self-healing process may be offset by the formation of dissolution channels. Our results have relevance beyond the greenhouse-gas sequestration problem. Chemical disequilibrium at waste injection sites and in hydrothermal reservoirs will lead to reactive flows that may also significantly alter formation permeability.

Effect of aluminium on dissolved organic matter mineralization in an allophanic and kaolinitic temperate rain forest soil

NASA Astrophysics Data System (ADS)

Merino, Carolina; Matus, Francisco; Fontaine, Sebastien

2016-04-01

Aluminium (Al) and it influence on the mineralization of dissolved organic matter (DOM) and thus on carbon (C) sequestration in forest soils is poorly understood. We hypothesized that an addition of Al to the soil solution beyond a molar Al:C ratio of 0.1, induces precipitation of the organic matter which leads to an excess Al in the soil solution causing an inhibitory effect for growing microorganisms. We investigated the effect of Al concentrations for the potential of C biodegradation at different Al:C ratios from DOM and Ah mineral soil horizons from two temperate rain forest soils from southern Chile. Dissolved organic matter and surface mineral horizons were incubated with initial molar Al:C ratio from 0.08 to 1.38 found under at field conditions. Mineralization was quantified by measurement of C-CO2 evolved during 15 days. Increasing the initial Al:C ratio > 0.12, led to a considerable reduction in mineralization (up to 70%). For Al:C ratio < 0.12, the mineralization rates from DOM and mineral soils were unaffected. Consequently, there would be a considerable reduction in the biodegradation of DOM and thus an increased in the C sequestration in mineral soils with molar Al:C ratio > 0.12. The observed DOM losses in the stream water of pristine southern forests can be explained by increasing the bioavailability of organic C for Al:C ratio < 0.12. Aluminium concentration had a marked effect at the spectral ART-FTIR bands assigned to cellulose-like and aromatic compounds in Ah mineral soil, diminishing the mineralization. The present results were also confirmed by the Al fluorescence using a confocal microscopy.

Inferences from Microfractures and Geochemistry in Dynamic Shale-CO2 Packed Bed Experiments

NASA Astrophysics Data System (ADS)

Radonjic, M.; Olabode, A.

2016-12-01

Subsurface storage of large volumes of carbondioxide (CO2) is expected to have long term rock-fluid interactions impact on reservoir and seal rocks properties. Caprocks, particularly sedimentary types, are the ultimate hydraulic barrier in carbon sequestration. The mineralogical components of sedimentary rocks are geochemically active under enormous earth stresses, which generate high pressure and temperature conditions. It has been postulated that in-situ mineralization can lead to flow impedance in natural fractures in the presence of favorable geochemical and thermodynamic conditions. This experimental modelling research investigated the impact of in-situ geochemical precipitation on conductivity of fractures. Geochemical analyses were performed on four different samples of shale rocks, effluent fluids and recovered precipitates both before and after CO2-brine flooding of crushed shale rocks at moderately high temperature and pressure conditions. The results showed that most significant diagenetic changes in shale rocks after flooding with CO2-brine, reflected in the effluent fluid with predominantly calcium based minerals dissolving and precipitating under experimental conditions. Major and trace elements in the effluent (using ICP-OES analysis) indicated that multiple geochemical reactions are occurring with almost all of the constituent minerals participating. The geochemical composition of precipitates recovered after the experiments showed diagenetic carbonates and opal as the main constituents. The bulk rock showed little changes in composition except for sharper and more refined peaks on XRD analysis, suggesting that a significant portion of the amorphous content of the rocks have been removed via dissolution by the slightly acid CO2-brine fluid that was injected. Micro-indentation results captured slight reduction in the hardness of the shale rocks and this reduction appeared dependent on diagenetic quartz content. It can be inferred that convective reactive transport of dissolved minerals are involved in nanoscale precipitation-dissolution processes in shale. This reactive transport of dissolved minerals can occlude micro-fracture flow paths, thereby improving shale caprock seal integrity with respect to leakage risk under CO2 sequestration conditions.

Ferric iron-bearing sediments as a mineral trap for CO2 sequestration: Iron reduction using sulfur-bearing waste gas

USGS Publications Warehouse

Palandri, J.L.; Kharaka, Y.K.

2005-01-01

We present a novel method for geologic sequestration of anthropogenic CO2 in ferrous carbonate, using ferric iron present in widespread redbeds and other sediments. Iron can be reduced by SO2 that is commonly a component of flue gas produced by combustion of fossil fuel, or by adding SO2 or H2S derived from other industrial processes to the injected waste gas stream. Equilibrium and kinetically controlled geochemical simulations at 120 bar and 50 and 100 ??C with SO2 or H2S show that iron can be transformed almost entirely to siderite thereby trapping CO2, and simultaneously, that sulfur can be converted predominantly to dissolved sulfate. If there is an insufficient amount of sulfur-bearing gas relative to CO2 as for typical flue gas, then some of the iron is not reduced, and some of the CO2 is not sequestered. If there is an excess of sulfur-bearing gas, then complete iron reduction is ensured, and some of the iron precipitates as pyrite or other solid iron sulfide, depending on their relative precipitation kinetics. Gas mixtures with insufficient sulfur relative to CO2 can be used in sediments containing Ca, Mg, or other divalent metals capable of precipitating carbonate minerals. For quartz arenite with an initial porosity of 21% and containing 0.25 wt.% Fe2O3, approximately 0.7 g of CO2 is sequestered per kg of rock, and the porosity decrease is less than 0.03%. Sequestration of CO2 using ferric iron has the advantage of disposing of SO2 that may already be present in the combustion gas. ?? 2005 Published by Elsevier B.V.

Wettability of supercritical carbon dioxide/water/quartz systems: simultaneous measurement of contact angle and interfacial tension at reservoir conditions.

PubMed

Saraji, Soheil; Goual, Lamia; Piri, Mohammad; Plancher, Henry

2013-06-11

Injection of carbon dioxide in deep saline aquifers is considered as a method of carbon sequestration. The efficiency of this process is dependent on the fluid-fluid and rock-fluid interactions inside the porous media. For instance, the final storage capacity and total amount of capillary-trapped CO2 inside an aquifer are affected by the interfacial tension between the fluids and the contact angle between the fluids and the rock mineral surface. A thorough study of these parameters and their variations with temperature and pressure will provide a better understanding of the carbon sequestration process and thus improve predictions of the sequestration efficiency. In this study, the controversial concept of wettability alteration of quartz surfaces in the presence of supercritical carbon dioxide (sc-CO2) was investigated. A novel apparatus for measuring interfacial tension and contact angle at high temperatures and pressures based on Axisymmetric Drop Shape Analysis with no-Apex (ADSA-NA) method was developed and validated with a simple system. Densities, interfacial tensions, and dynamic contact angles of CO2/water/quartz systems were determined for a wide range of pressures and temperatures relevant to geological sequestration of CO2 in the subcritical and supercritical states. Image analysis was performed with ADSA-NA method that allows the determination of both interfacial tensions and contact angles with high accuracy. The results show that supercritical CO2 alters the wettability of quartz surface toward less water-wet conditions compared to subcritical CO2. Also we observed an increase in the water advancing contact angles with increasing temperature indicating less water-wet quartz surfaces at higher temperatures.

Carbon sequestration and fertility after centennial time scale incorporation of charcoal into soil

NASA Astrophysics Data System (ADS)

Criscuoli, Irene; Alberti, Giorgio; Baronti, Silvia; Favilli, Filippo; Martinez, Cristina; Calzolari, Costanza; Pusceddu, Emanuela; Rumpel, Cornelia; Viola, Roberto; Miglietta, Franco

2014-05-01

The addition of pyrogenic carbon (C) in the soil is considered a sustainable strategy to achieve direct C sequestration and potential reduction of non-CO2 greenhouse gas emissions. In this paper, we investigated the long term effects of charcoal addition on C sequestration and soil chemico-physical properties by studying a series of abandoned charcoal hearths in the Eastern Alps established in the XIX century. This natural setting can be seen as an analogue of a deliberate experiment with replications. Carbon sequestration was assessed indirectly by comparing the amount of C present in the hearths with the estimated amount of charcoal that was left on the soil after the carbonization. Approximately 80% of the C originally added to the soil via charcoal can still be found today, thus supporting the view that charcoal incorporation is an effective way to sequester atmospheric CO2. We also observed an improvement in the physical properties (hydrophobicity and bulk density) of charcoal hearth soils and an accumulation of nutrients compared to the adjacent soil without charcoal. Then, we focused on the morphological and physical characterization of several fragments, using scanning electron microscopy (SEM), X-ray diffraction (XRD) and X-ray fluorescence (XRF). Such study enabled the identification of peculiar morphological features of tracheids, which were tentatively associated to a differential oxidation of the structures that were created during carbonization from lignine and cellulose. In order to assess the effect of soil-aging we compared the old-biochar with a modern one obtained from the same feedstock and with similar carbonization process. XRD and XRF analysis were performed on both old and modern biochar, in order to study the multiphase crystalline structure and chemical elements found. We observed mineralization and a fossilization of old biochar samples respect to the modern ones, with accumulation of several mineral oxides and a substantial presence of quartz. A graphene structure was also found, indicating weak bonds in the carbon structures, explained by inter-molecular Van der Waals forces. Furthermore, we have detected a graphite oxide structure responsible of the bending effect in the tracheid, revealed in SEM images. We consider that those results may contribute to the ongoing debate on the best, most suitable geo-engineering strategies that can potentially enable effective and sustainable carbon sequestration in agricultural soils using biochar.

Atmospheric carbon mineralization in an industrial-scale chrysotile mining waste pile.

PubMed

Nowamooz, Ali; Dupuis, J Christian; Beaudoin, Georges; Molson, John; Lemieux, Jean-Michel; Horswill, Micha; Fortier, Richard; Larachi, Faïçal; Maldague, Xavier; Constantin, Marc; Duchesne, Josee; Therrien, René

2018-06-12

Magnesium rich minerals that are abundant in ultramafic mining waste have the potential to be used as a safe and permanent sequestration solution for carbon dioxide (CO2). Our understanding of thermo-hydro-chemical regimes that govern this reaction at an industrial scale, however, has remained an important challenge to its widespread implementation. Through a year-long monitoring experiment performed at a 110Mt chrysotile waste pile, we have documented the existence of two distinct thermo-hydro-chemical regimes that control the ingress of CO2 and the subsequent mineral carbonation of the waste. The experimental results are supported by coupled free-air/porous media numerical flow and transport model that provides insights into optimization strategies to increase the efficiency of mineral sequestration at an industrial-scale. Although functioning passively under less than optimal conditions compared to lab-scale experiments, the 110Mt Thetford Mines pile is nevertheless estimated to be sequestering up to 100 tonnes of CO2 per year, with a potential total carbon capture capacity under optimal conditions of 3 Mt. Yearly, over 100 Mt of ultramafic mine waste suitable for mineral carbonation are generated by the global mining industry. Our results show that this waste material could become a safe and permanent carbon sink for diffuse sources of CO2.

Microbially mediated mineral carbonation

NASA Astrophysics Data System (ADS)

Power, I. M.; Wilson, S. A.; Dipple, G. M.; Southam, G.

2010-12-01

Mineral carbonation involves silicate dissolution and carbonate precipitation, which are both natural processes that microorganisms are able to mediate in near surface environments (Ferris et al., 1994; Eq. 1). (Ca,Mg)SiO3 + 2H2CO3 + H2O → (Ca,Mg)CO3 + H2O + H4SiO4 + O2 (1) Cyanobacteria are photoautotrophs with cell surface characteristics and metabolic processes involving inorganic carbon that can induce carbonate precipitation. This occurs partly by concentrating cations within their net-negative cell envelope and through the alkalinization of their microenvironment (Thompson & Ferris, 1990). Regions with mafic and ultramafic bedrock, such as near Atlin, British Columbia, Canada, represent the best potential sources of feedstocks for mineral carbonation. The hydromagnesite playas near Atlin are a natural biogeochemical model for the carbonation of magnesium silicate minerals (Power et al., 2009). Field-based studies at Atlin and corroborating laboratory experiments demonstrate the ability of a microbial consortium dominated by filamentous cyanobacteria to induce the precipitation of carbonate minerals. Phototrophic microbes, such as cyanobacteria, have been proposed as a means for producing biodiesel and other value added products because of their efficiency as solar collectors and low requirement for valuable, cultivable land in comparison to crops (Dismukes et al., 2008). Carbonate precipitation and biomass production could be facilitated using specifically designed ponds to collect waters rich in dissolved cations (e.g., Mg2+ and Ca2+), which would allow for evapoconcentration and provide an appropriate environment for growth of cyanobacteria. Microbially mediated carbonate precipitation does not require large quantities of energy or chemicals needed for industrial systems that have been proposed for rapid carbon capture and storage via mineral carbonation (e.g., Lackner et al., 1995). Therefore, this biogeochemical approach may represent a readily implemented and economically efficient alternative to other technologies currently under development for mineral sequestration. Dismukes GC, Carrieri D, Bennette N, Ananyev GM, Posewitz MC (2008) Aquatic phototrophs: efficient alternatives to land-based crops for biofuels. Current Opinion in Biotechnology, 19, 235-240. Ferris FG, Wiese RG, Fyfe WS (1994) Precipitation of carbonate minerals by microorganisms: Implications of silicate weathering and the global carbon dioxide budget. Geomicrobiology Journal, 12, 1-13. Lackner KS, Wendt CH, Butt DP, Joyce EL, Jr., Sharp DH (1995) Carbon dioxide disposal in carbonate minerals. Energy, 20, 1153-1170. Power IM, Wilson SA, Thom JM, Dipple GM, Gabites JE, Southam G (2009) The hydromagnesite playas of Atlin, British Columbia, Canada: A biogeochemical model for CO2 sequestration. Chemical Geology, 206, 302-316. Thompson JB, Ferris FG (1990) Cyanobacterial precipitation of gypsum, calcite, and magnesite from natural alkaline lake water. Geology, 18, 995-998.

Final Technical Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sobecky, Patricia A; Taillefert, Martial

This final technical report describes results and findings from a research project to examine the role of microbial phosphohydrolase enzymes in naturally occurring subsurface microorganisms for the purpose of promoting the immobilization of the radionuclide uranium through the production of insoluble uranium phosphate minerals. The research project investigated the microbial mechanisms and the physical and chemical processes promoting uranium biomineralization and sequestration in oxygenated subsurface soils. Uranium biomineralization under aerobic conditions can provide a secondary biobarrier strategy to immobilize radionuclides should the metal precipitates formed by microbial dissimilatory mechanisms remobilize due to a change in redox state.

Coupled multiphase reactive flow and mineral dissolution-precipitation kinetics: Examples of long-term CO2 sequestration in Utsira Sand, Norway and Mt. Simon Formation, Midwest USA

NASA Astrophysics Data System (ADS)

Zhang, Y.; Zhang, G.; Lu, P.; Hu, B.; Zhu, C.

2017-12-01

The extent of CO2 mineralization after CO2 injection into deep saline aquifers is a result of the complex coupling of multiphase fluid flow, mass transport, and brine-mineral reactions. The effects of dissolution rate laws and groundwater flow on the long-term fate of CO2 have been seriously overlooked. To investigate these effects, we conducted multiphase (CO2 and brine) coupled reactive transport modeling of CO2 storage in two sandy formations (Utsira Sand, Norway1,2 and Mt. Simon formation, USA 3) using ToughReact and simulated a series of scenarios. The results indicated that: (1) Different dissolution rate laws for feldspars can significantly affect the amount of CO2 mineralization. Increased feldspar dissolution will promote CO2 mineral trapping through the coupling between feldspar dissolution and carbonate mineral precipitation at raised pH. The predicted amount of CO2 mineral trapping when using the principle of detailed balancing-based rate law for feldspar dissolution is about twice as much as that when using sigmoidal rate laws in the literature. (2) Mineral trapping is twice as much when regional groundwater flow is taken into consideration in long-term simulations (e.g., 10,000 years) whereas most modeling studies neglected the regional groundwater flow back and effectively simulated a batch reactor process. Under the influence of regional groundwater flow, the fresh brine from upstream continuously dissolves CO2 at the tail of CO2 plume, generating a large acidified area where large amount of CO2 mineralization takes place. The upstream replenishment of groundwater results in ˜22% mineral trapping at year 10,000, compared to ˜4% when this effect is ignored. Refs: 1Zhang, G., Lu, P., Wei, X., Zhu, C. (2016). Impacts of Mineral Reaction Kinetics and Regional Groundwater Flow on Long-Term CO2 Fate at Sleipner. Energy & Fuels, 30(5), 4159-4180. 2Zhu, C., Zhang, G., Lu, P., Meng, L., Ji, X. (2015). Benchmark modeling of the Sleipner CO2 plume: Calibration to seismic data for the uppermost layer and model sensitivity analysis. International Journal of Greenhouse Gas Control, 43, 233-246. 3Zhang, G., Lu, P., Zhang, Y., Wei, X., Zhu, C. (2015). Effects of rate law formulation on predicting CO2 sequestration in sandstone formations. International Journal of Energy Research, 39(14), 1890-1908.

The Role of Cyanobacteria in CO2 Sequestration at Mine Sites

NASA Astrophysics Data System (ADS)

Power, I. M.; Wilson, S. A.; Dipple, G. M.; Southam, G.

2009-05-01

The weathering of mine tailings occurs relatively rapidly as a result of their high surface area and the release of cations, such as Ca2+ and Mg2+, are then available to form stable carbonate minerals thereby sequestering CO2 [1]. In natural environments, silicate weathering in bedrock is biogeochemically coupled to the precipitation of carbonate minerals by microorganisms. Equation 1 describes the combined processes of bedrock weathering and carbonate precipitation by oxygenic phototrophic bacteria (e.g., cyanobacteria) [2]. (Ca,Mg)SiO3 + 2H2CO3 + H2O = (Ca,Mg)CO3 + H2O + H4SiO4 + O2 (1) Tailings from the Diavik Diamond Mine, Northwest Territories, Canada and Mount Keith Nickel Mine, Western Australia were leached using hydrochloric, sulfuric, acetic, nitric and phosphoric acids. These solutions were amended with nutrients and were inoculated with a consortium dominated by Synechococcus sp. from a hydromagnesite-wetland near Atlin, British Columbia Canada. Cyanobacteria are able to induce precipitation of carbonate minerals by the alkalinization of their microenvironment, concentrating cations on their cell membrane, which also provides regularly spaced, chemically identical sites for mineral nucleation [3-5]. Resulting biofilms and precipitates were examined using phase-contrast light microscopy and scanning electron microscopy. Results indicate that Synechococcus sp. may be able to mediate carbonate precipitation in waters produced from leaching mine tailings. Carbonate precipitation at mine sites could be facilitated using a specifically designed pond to collect drainage waters from mine tailings, which would allow for evapoconcentration and provide an appropriate environment for growth of cyanobacteria. Microbially-aided carbonate precipitation could play an important role in mineral carbonation of mine tailings as part of a CO2 sequestration strategy at mine sites. [1] Wilson et al. (2006) Am. Mineral. 91, 1331-1341. [2] Ferris et al. (1994) Geomicrobiol. J. 12, 1-13. [3] Power et al. (2007) Geochem. Trans. 8, 13. [4] Thompson and Ferris (1990) Geology 18, 995-998. [5] Schultze-Lam and Beveridge (1994) Can. J. Micro. 40, 216-223.

Microbial Reverse-Electrodialysis Electrolysis and Chemical-Production Cell for H2 Production and CO2 Sequestration.

PubMed

Zhu, Xiuping; Hatzell, Marta C; Logan, Bruce E

2014-04-08

Natural mineral carbonation can be accelerated using acid and alkali solutions to enhance atmospheric CO 2 sequestration, but the production of these solutions needs to be carbon-neutral. A microbial reverse-electrodialysis electrolysis and chemical-production cell (MRECC) was developed to produce these solutions and H 2 gas using only renewable energy sources (organic matter and salinity gradient). Using acetate (0.82 g/L) as a fuel for microorganisms to generate electricity in the anode chamber (liquid volume of 28 mL), 0.45 mmol of acid and 1.09 mmol of alkali were produced at production efficiencies of 35% and 86%, respectively, along with 10 mL of H 2 gas. Serpentine dissolution was enhanced 17-87-fold using the acid solution, with approximately 9 mL of CO 2 absorbed and 4 mg of CO 2 fixed as magnesium or calcium carbonates. The operational costs, based on mineral digging and grinding, and water pumping, were estimated to be only $25/metric ton of CO 2 fixed as insoluble carbonates. Considering the additional economic benefits of H 2 generation and possible wastewater treatment, this method may be a cost-effective and environmentally friendly method for CO 2 sequestration.

Deep horizons: Soil Carbon sequestration and storage potential in grassland soils

NASA Astrophysics Data System (ADS)

Torres-Sallan, Gemma; Schulte, Rogier; Lanigan, Gary J.; Byrne, Kenneth A.; Reidy, Brian; Creamer, Rachel

2016-04-01

Soil Organic Carbon (SOC) enhances soil fertility, holding nutrients in a plant-available form. It also improves aeration and water infiltration. Soils are considered a vital pool for C (Carbon) sequestration, as they are the largest pool of C after the oceans, and contain 3.5 more C than the atmosphere. SOC models and inventories tend to focus on the top 30 cm of soils, only analysing total SOC values. Association of C with microaggregates (53-250 μm) and silt and clay (<53 μm) is considered C sequestration as these fractions offer the greatest protection against mineralization. This study assessed the role of aggregation in C sequestration throughout the profile, down to 1 m depth, of 30 grassland sites divided in 6 soil types. One kg sample was collected for each horizon, sieved at 8 mm and dried at 40 °C. Through a wet sieving procedure, four aggregate sizes were isolated: large macroaggregates (>2000 μm); macroaggregates (250-2000 μm); microaggregates and silt & clay. Organic C associated to each aggregate fraction was analysed on a LECO combustion analyser. Sand-free C was calculated for each aggregate size. For all soil types, 84% of the SOC located in the first 30 cm was contained inside macroaggregates and large macroaggregates. Given that this fraction has a turnover time of 1 to 10 years, sampling at that depth only provides information on the labile fraction in soil, and does not consider the longer term C sequestration potential. Only when looking at the whole profile, two clear trends could be observed: 1) soils with a clay increase at depth had most of their C located in the silt and clay fractions, which indicate their enhanced C sequestration capacity, 2) free-draining soils had a bigger part of their SOC located in the macroaggregate fractions. These results indicate that current C inventories and models that focus on the top 30 cm, do not accurately measure soil C sequestration potential in soils, but rather the more labile fraction. However, at depth soil forming processes have been identified as a major factor influencing C sequestration potential in soils. This has a major impact in further quantifying and sustaining C sequestration into the future. Soils with a high sequestration potential at depth need to be managed to enhance the residence time to contribute to future off-setting of greenhouse gas emissions.

Preliminary reactive geochemical transport simulation study on CO2 geological sequestration at the Changhua Coastal Industrial Park Site, Taiwan

NASA Astrophysics Data System (ADS)

Sung, R.; Li, M.

2013-12-01

Mineral trapping by precipitated carbonate minerals is one of critical mechanisms for successful long-term geological sequestration (CGS) in deep saline aquifer. Aquifer acidification induced by the increase of carbonic acid (H2CO3) and bicarbonate ions (HCO3-) as the dissolution of injected CO2 may induce the dissolution of minerals and hinder the effectiveness of cap rock causing potential risk of CO2 leakage. Numerical assessments require capabilities to simulate complicated interactions of thermal, hydrological, geochemical multiphase processes. In this study, we utilized TOUGHREACT model to demonstrate a series of CGS simulations and assessments of (1) time evolution of aquifer responses, (2) migration distance and spatial distribution of CO2 plume, (3) effects of CO2-saline-mineral interactions, and (4) CO2 trapping components at the Changhua Costal Industrial Park (CCIP) Site, Taiwan. The CCIP Site is located at the Southern Taishi Basin with sloping and layered heterogeneous formations. At this preliminary phase, detailed information of mineralogical composition of reservoir formation and chemical composition of formation water are difficult to obtain. Mineralogical composition of sedimentary rocks and chemical compositions of formation water for CGS in deep saline aquifer from literatures (e.g. Xu et al., 2004; Marini, 2006) were adopted. CGS simulations were assumed with a constant CO2 injection rate of 1 Mt/yr at the first 50 years. Hydrogeological settings included porosities of 0.103 for shale, 0.141 for interbedding sandstone and shale, and 0.179 for sandstone; initial pore pressure distributions of 24.5 MPa to 28.7 MPa, an ambient temperature of 70°C, and 0.5 M of NaCl in aqueous solution. Mineral compositions were modified from Xu et al. (2006) to include calcite (1.9 vol. % of solid), quartz (57.9 %), kaolinite (2.0 %), illite (1.0 %), oligoclase (19.8 %), Na-smectite (3.9 %), K-feldspar (8.2 %), chlorite (4.6 %), and hematite (0.5 %) and were assumed throughout the simulation domain. Comparisons among simulated results with different mesh systems of nested meshes and non-nested meshes and considerations of multiphase reactive transport and physical transport were demonstrated in this study. Preliminary results of injection CO2 for 50 years are: (1) about 7 wt.% of injected CO2 was trapped as carbonate minerals mainly as ankerite; (2) porosities were decreased by 0.014 % and increased by 0.102 % at the injection point and beneath the cap rock, respectively, and were subsequently decreased with time due to minerals precipitation mostly as illite and ankerite; (3) differences of simulated aquifer responses between reactive transport and physical transport were insignificant; and (4) projected CO2 plumes with the nested meshes was smaller than those by the non-nested meshes after cease of CO2 injection. Keywords: CO2-Saline-Mineral Interaction, Reactive Geochemical Transport, TOUGHREACT, Mineral Trapping Assessment, Changhua Costal Industrial Park Site, Taiwan Reference: Marini, L., 2006, Geological Sequestration of Carbon Dioxide, Volume 11: Thermodynamics, Kinetics, and Reaction Path Modeling, Elsevier Science, pp.470. Xu, T., J. A. Apps and K. Pruess, 2004, Numerical simulation of CO2 disposal by mineral trapping in deep aquifers, Applied Geochemistry, Vol. 19:917-936.

Effects of Biochar Amendment on Soil Properties and Soil Carbon Sequestration

NASA Astrophysics Data System (ADS)

Zhang, R.; Zhu, S.

2015-12-01

Biochar addition to soils potentially affects various soil properties and soil carbon sequestration, and these effects are dependent on biochars derived from different feedstock materials and pyrolysis processes. The objective of this study was to investigate the effects of amendment of different biochars on soil physical and biological properties as well as soil carbon sequestration. Biochars were produced with dairy manure and woodchip at temperatures of 300, 500, and 700°C, respectively. Each biochar was mixed at 5% (w/w) with a forest soil and the mixture was incubated for 180 days, during which soil physical and biological properties, and soil respiration rates were measured. Results showed that the biochar addition significantly enhanced the formation of soil macroaggregates at the early incubation time. The biochar application significantly reduced soil bulk density, increased the amount of soil organic matter, and stimulated microbial activity and soil respiration rates at the early incubation stage. Biochar applications improved water retention capacity, with stronger effects by biochars produced at higher pyrolysis temperatures. At the same suction, the soil with woodchip biochars possessed higher water content than with the dairy manure biochars. Biochar addition significantly affected the soil physical and biological properties, which resulted in different soil carbon mineralization rates and the amount of soil carbon storage.

Carbon K-edge spectra of carbonate minerals.

PubMed

Brandes, Jay A; Wirick, Sue; Jacobsen, Chris

2010-09-01

Carbon K-edge X-ray spectroscopy has been applied to the study of a wide range of organic samples, from polymers and coals to interstellar dust particles. Identification of carbonaceous materials within these samples is accomplished by the pattern of resonances in the 280-320 eV energy region. Carbonate minerals are often encountered in the study of natural samples, and have been identified by a distinctive resonance at 290.3 eV. Here C K-edge and Ca L-edge spectra from a range of carbonate minerals are presented. Although all carbonates exhibit a sharp 290 eV resonance, both the precise position of this resonance and the positions of other resonances vary among minerals. The relative strengths of the different carbonate resonances also vary with crystal orientation to the linearly polarized X-ray beam. Intriguingly, several carbonate minerals also exhibit a strong 288.6 eV resonance, consistent with the position of a carbonyl resonance rather than carbonate. Calcite and aragonite, although indistinguishable spectrally at the C K-edge, exhibited significantly different spectra at the Ca L-edge. The distinctive spectral fingerprints of carbonates provide an identification tool, allowing for the examination of such processes as carbon sequestration in minerals, Mn substitution in marine calcium carbonates (dolomitization) and serpentinization of basalts.

Experimental multi-phase CO2-brine-rock interactions at elevated temperature and pressure: Implications for CO2 sequestration in deep-saline aquifers

USGS Publications Warehouse

Rosenbauer, R.J.; Koksalan, T.

2004-01-01

Long-term CO2 saturated brine-rock experiments were conducted to evaluate the effects of multiphase H2O-CO2 fluids on mineral equilibria and the potential for CO2 sequestration mineral phases within deep-saline aquifers. Experimental results were consistent with theoretical thermodynamic calculations when CO2-saturated brines were reacted with limestone rocks. The CO2-saturated brine-limestone reactions were characterized by compositional and mineralogical-changes in the aquifer fluid and formation rocks that were dependent on initial brine composition as were the changes in formation porosity, especially dissolved sulfate. The solubility of CO2 was enhanced in brines in the presence of both limestone and sandstone rocks relative to brines alone. Reactions between CO2 saturated brines and arkosic sandstones were characterized by desiccation of the brine and changes in the chemical composition of the brine suggesting fixation of CO2 in mineral phases. These reactions occured on a measurable but kinetically slow time scale at 120??C.

CO2–rock–brine interactions in Lower Tuscaloosa Formation at Cranfield CO2 sequestration site, Mississippi, U.S.A.

USGS Publications Warehouse

Lu, Jiemin; Kharaka, Yousif K.; Thordsen, James J.; Horita, Juske; Karamalidis, Athanasios; Griffith, Craig; Hakala, J. Alexandra; Ambats, Gil; Cole, David R.; Phelps, Tommy J.; Manning, Michael A.; Cook, Paul J.; Hovorka, Susan D.

2012-01-01

A highly integrated geochemical program was conducted at the Cranfield CO2-enhanced oil recovery (EOR) and sequestration site, Mississippi, U.S.A.. The program included extensive field geochemical monitoring, a detailed petrographic study, and an autoclave experiment under in situ reservoir conditions. Results show that mineral reactions in the Lower Tuscaloosa reservoir were minor during CO2 injection. Brine chemistry remained largely unchanged, which contrasts with significant changes observed in other field tests. Field fluid sampling and laboratory experiments show consistently slow reactions. Carbon isotopic composition and CO2 content in the gas phase reveal simple two-end-member mixing between injected and original formation gas. We conclude that the reservoir rock, which is composed mainly of minerals with low reactivity (average quartz 79.4%, chlorite 11.8%, kaolinite 3.1%, illite 1.3%, concretionary calcite and dolomite 1.5%, and feldspar 0.2%), is relatively unreactive to CO2. The significance of low reactivity is both positive, in that the reservoir is not impacted, and negative, in that mineral trapping is insignificant.

Effects of salinity and the extent of water on supercritical CO2-induced phlogopite dissolution and secondary mineral formation.

PubMed

Shao, Hongbo; Ray, Jessica R; Jun, Young-Shin

2011-02-15

To ensure the viability of geologic CO2 sequestration (GCS), we need a holistic understanding of reactions at supercritical CO2 (scCO2)-saline water-rock interfaces and the environmental factors affecting these interactions. This research investigated the effects of salinity and the extent of water on the dissolution and surface morphological changes of phlogopite [KMg2.87Si3.07Al1.23O10(F,OH)2], a model clay mineral in potential GCS sites. Salinity enhanced the dissolution of phlogopite and affected the location, shape, size, and phase of secondary minerals. In low salinity solutions, nanoscale particles of secondary minerals formed much faster, and there were more nanoparticles than in high salinity solutions. The effect of water extent was investigated by comparing scCO2-H2O(g)-phlogopite and scCO2-H2O(l)-phlogopite interactions. Experimental results suggested that the presence of a thin water film adsorbed on the phlogopite surface caused the formation of dissolution pits and a surface coating of secondary mineral phases that could change the physical properties of rocks. These results provide new information for understanding reactions at scCO2-saline water-rock interfaces in deep saline aquifers and will help design secure and environmentally sustainable CO2 sequestration projects.

An Index-Based Approach to Assessing Recalcitrance and Soil Carbon Sequestration Potential of Engineered Black Carbons (Biochars)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Harvey, Omar R.; Kuo, Li-Jung; Zimmerman, Andrew R.

2012-01-10

The ability of engineered black carbons (or biochars) to resist abiotic and, or biotic degradation (herein referred to as recalcitrance) is crucial to their successful deployment as a soil carbon sequestration strategy. A new recalcitrance index, the R{sub 50}, for assessing biochar quality for carbon sequestration is proposed. The R{sub 50} is based on the relative thermal stability of a given biochar to that of graphite and was developed and evaluated with a variety of biochars (n = 59), and soot-like black carbons. Comparison of R{sub 50}, with biochar physicochemical properties and biochar-C mineralization revealed the existence of a quantifiablemore » relationship between R{sub 50} and biochar recalcitrance. As presented here, the R{sub 50} is immediately applicable to pre-land application screening of biochars into Class A (R{sub 50} {>=} 0.70), Class B (0.50 {<=} R{sub 50} < 0.70) or Class C (R{sub 50} < 0.50) recalcitrance/carbon sequestration classes. Class A and Class C biochars would have carbon sequestration potential comparable to soot/graphite and uncharred plant biomass, respectively, while Class B biochars would have intermediate carbon sequestration potential. We believe that the coupling of the R{sub 50}, to an index-based degradation, and an economic model could provide a suitable framework in which to comprehensively assess soil carbon sequestration in biochars.« less

Dissipation of bentazone, pyrimethanil and boscalid in biochar and digestate based soil mixtures for biopurification systems.

PubMed

Mukherjee, Santanu; Tappe, Wolfgang; Weihermueller, Lutz; Hofmann, Diana; Köppchen, Stephan; Laabs, Volker; Schroeder, Tom; Vereecken, Harry; Burauel, Peter

2016-02-15

Biopurification systems, such as biofilters, are biotechnological tools to prevent point sources of pesticide pollution stemming from on-farm operations. For the purification processes pesticide sorption and mineralization and/or dissipation are essential and both largely depend on the type of filling materials and the pesticide in use. In this paper the mineralization and dissipation of three contrasting (14)C-labeled pesticides (bentazone, boscalid, and pyrimethanil) were investigated in laboratory incubation experiments using sandy soil, biochar produced from Pine woodchips, and/or digestate obtained from anaerobic digestion process using maize silage, chicken manure, beef and pig urine as feedstock. The results indicate that the addition of digestate increased pesticide mineralization, whereby the mineralization was not proportional to the digestate loads in the mixture, indicating a saturation effect in the turnover rate of pesticides. This effect was in correlation with the amount of water extractable DOC, obtained from the digestate based mixtures. Mixing biochar into the soil generally reduced total mineralization and led to larger sorption/sequestration of the pesticides, resulting in faster decrease of the extractable fraction. Also the addition of biochar to the soil/digestate mixtures reduced mineralization compared to the digestate alone mixture but mineralization rates were still higher as for the biochar/soil alone. In consequence, the addition of biochar to the soil generally decreased pesticide dissipation times and larger amounts of biochar led to high amounts of non-extractable residues of pesticide in the substrates. Among the mixtures tested, a mixture of digestate (5%) and biochar (5%) gave optimal results with respect to mineralization and simultaneous sorption for all three pesticides. Copyright © 2015 Elsevier B.V. All rights reserved.

Whole watershed quantification of net carbon fluxes by erosion and deposition within the Christina River Basin Critical Zone Observatory

NASA Astrophysics Data System (ADS)

Aufdenkampe, A. K.; Karwan, D. L.; Aalto, R. E.; Marquard, J.; Yoo, K.; Wenell, B.; Chen, C.

2012-12-01

We have proposed that the rate at which fresh, carbon-free minerals are delivered to and mix with fresh organic matter determines the rate of carbon preservation at a watershed scale (Aufdenkampe et al. 2011). Although many studies have examined the role of erosion in carbon balances, none consider that fresh carbon and fresh minerals interact. We believe that this mechanism may be a dominant sequestration process in watersheds with strong anthropogenic impacts. Our hypothesis - that the rate of mixing fresh carbon with fresh, carbon-free minerals is a primary control on watershed-scale carbon sequestration - is central to our Christina River Basin Critical Zone Observatory project (CRB-CZO, http://www.udel.edu/czo/). The Christina River Basin spans 1440 km2 from piedmont to Atlantic coastal plain physiographic provinces in the states of Pennsylvania and Delaware, and experienced intensive deforestation and land use beginning in the colonial period of the USA. Here we present a synthesis of multi-disciplinary data from the CRB-CZO on materials as they are transported from sapprolite to topsoils to colluvium to suspended solids to floodplains, wetlands and eventually to the Delaware Bay estuary. At the heart of our analysis is a spatially-integrated, flux-weighted comparison of the organic carbon to mineral surface area ratio (OC/SA) of erosion source materials versus transported and deposited materials. Because source end-members - such as forest topsoils, farmed topsoils, gullied subsoils and stream banks - represent a wide distribution of initial, pre-erosion OC/SA, we quantify source contributions using geochemical sediment fingerprinting approaches (Walling 2005). Analytes used for sediment fingerprinting include: total mineral elemental composition (including rare earth elements), fallout radioisotope activity for common erosion tracers (beryllium-7, beryllium-10, lead-210, cesium-137), particle size distribution and mineral specific surface area, in addition to organic carbon and nitrogen content with stable isotope (13C, 15N) and radiocarbon (14C) abundance to quantify OC/SA and organic carbon sources and mean age. We then use multivariate mixing model analysis to quantify the fractional contribution of each source end-member to each sample of suspended or deposited sediments. Last, we calculate a predicted OC/SA based on source end-member mixing and compare to the measured OC/SA to quantify net change in mineral complexed carbon.

Calculating carbon mass balance from unsaturated soil columns treated with CaSO₄₋minerals: test of soil carbon sequestration.

PubMed

Han, Young-Soo; Tokunaga, Tetsu K

2014-12-01

Renewed interest in managing C balance in soils is motivated by increasing atmospheric concentrations of CO2 and consequent climate change. Here, experiments were conducted in soil columns to determine C mass balances with and without addition of CaSO4-minerals (anhydrite and gypsum), which were hypothesized to promote soil organic carbon (SOC) retention and soil inorganic carbon (SIC) precipitation as calcite under slightly alkaline conditions. Changes in C contents in three phases (gas, liquid and solid) were measured in unsaturated soil columns tested for one year and comprehensive C mass balances were determined. The tested soil columns had no C inputs, and only C utilization by microbial activity and C transformations were assumed in the C chemistry. The measurements showed that changes in C inventories occurred through two processes, SOC loss and SIC gain. However, the measured SOC losses in the treated columns were lower than their corresponding control columns, indicating that the amendments promoted SOC retention. The SOC losses resulted mostly from microbial respiration and loss of CO2 to the atmosphere rather than from chemical leaching. Microbial oxidation of SOC appears to have been suppressed by increased Ca(2+) and SO4(2)(-) from dissolution of CaSO4 minerals. For the conditions tested, SIC accumulation per m(2) soil area under CaSO4-treatment ranged from 130 to 260 g C m(-1) infiltrated water (20-120 g C m(-1) infiltrated water as net C benefit). These results demonstrate the potential for increasing C sequestration in slightly alkaline soils via CaSO4-treatment. Copyright © 2014 Elsevier Ltd. All rights reserved.

Lattice Boltzmann simulation of CO2 reactive transport in network fractured media

NASA Astrophysics Data System (ADS)

Tian, Zhiwei; Wang, Junye

2017-08-01

Carbon dioxide (CO2) geological sequestration plays an important role in mitigating CO2 emissions for climate change. Understanding interactions of the injected CO2 with network fractures and hydrocarbons is key for optimizing and controlling CO2 geological sequestration and evaluating its risks to ground water. However, there is a well-known, difficult process in simulating the dynamic interaction of fracture-matrix, such as dynamic change of matrix porosity, unsaturated processes in rock matrix, and effect of rock mineral properties. In this paper, we develop an explicit model of the fracture-matrix interactions using multilayer bounce-back treatment as a first attempt to simulate CO2 reactive transport in network fractured media through coupling the Dardis's LBM porous model for a new interface treatment. Two kinds of typical fracture networks in porous media are simulated: straight cross network fractures and interleaving network fractures. The reaction rate and porosity distribution are illustrated and well-matched patterns are found. The species concentration distribution and evolution with time steps are also analyzed and compared with different transport properties. The results demonstrate the capability of this model to investigate the complex processes of CO2 geological injection and reactive transport in network fractured media, such as dynamic change of matrix porosity.

Interactions between extracellular polymeric substances and clay minerals affect soil aggregation

NASA Astrophysics Data System (ADS)

Vogel, Cordula; Rehschuh, Stephanie; Kemi Olagoke, Folasade; Redmile Gordon, Marc; Kalbiltz, Karsten

2017-04-01

Soil aggregation is crucial for carbon (C) sequestration and microbial processes have been recognised as important control of aggregate turnover (formation, stability, and destruction). However, how microorganisms contribute to these processes is still a matter of debate. An enthralling mechanism determining aggregate turnover and therefore C sequestration may be the excretion of extracellular polymeric substances (EPS) as microbial glue, but effects of EPS on aggregation is largely unknown. Moreover, interdependencies between important aggregation factors like the amount of fine-sized particles (clay content), the decomposability of organic matter and the microbial community (size and composition, as well as the excretion of EPS) are still poorly understood. Therefore, we studied the complex interactions between these factors and their role in aggregate turnover. It was hypothesized that an increase in microbial activity, induced by the input of organic substrates, will stimulate EPS production and therefore the formation and stability of aggregates. To test this hypothesis, an incubation experiment has been conducted across a gradient of clay content (montmorillonite) and substrate decomposability (starch and glucose) as main drivers of the microbial activity. A combination of aggregate separation and stability tests were applied. This results will be examined with respect to the obtained microbial parameters (amount and composition of EPS, CO2 emission, microbial biomass, phospholipid fatty acid), to disentangle the mechanisms and factors controlling aggregate turnover affected by soil microorganisms. This study is expected to provide insights on the role of EPS in the stability of aggregates. Thus, the results of this study will provide an improved understanding of the underlying processes of aggregate turnover in soils, which is necessary to implement strategies for enhanced C sequestration in agricultural soils.

Integrated Experimental and Modeling Studies of Mineral Carbonation as a Mechanism for Permanent Carbon Sequestration in Mafic/Ultramafic Rocks

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Zhengrong; Qiu, Lin; Zhang, Shuang

2014-09-30

A program of laboratory experiments, modeling and fieldwork was carried out at Yale University, University of Maryland, and University of Hawai‘i, under a DOE Award (DE-FE0004375) to study mineral carbonation as a practical method of geologic carbon sequestration. Mineral carbonation, also called carbon mineralization, is the conversion of (fluid) carbon dioxide into (solid) carbonate minerals in rocks, by way of naturally occurring chemical reactions. Mafic and ultramafic rocks, such as volcanic basalt, are natural candidates for carbonation, because the magnesium and iron silicate minerals in these rocks react with brines of dissolved carbon dioxide to form carbonate minerals. By trappingmore » carbon dioxide (CO 2) underground as a constituent of solid rock, carbonation of natural basalt formations would be a secure method of sequestering CO 2 captured at power plants in efforts to mitigate climate change. Geochemical laboratory experiments at Yale, carried out in a batch reactor at 200°C and 150 bar (15 MPa), studied carbonation of the olivine mineral forsterite (Mg 2SiO 4) reacting with CO 2 brines in the form of sodium bicarbonate (NaHCO 3) solutions. The main carbonation product in these reactions is the carbonate mineral magnesite (MgCO 3). A series of 32 runs varied the reaction time, the reactive surface area of olivine grains and powders, the concentration of the reacting fluid, and the starting ratio of fluid to olivine mass. These experiments were the first to study the rate of olivine carbonation under passive conditions approaching equilibrium. The results show that, in a simple batch reaction, olivine carbonation is fastest during the first 24 hours and then slows significantly and even reverses. A natural measure of the extent of carbonation is a quantity called the carbonation fraction, which compares the amount of carbon removed from solution, during a run, to the maximum amount that could have been removed if the olivine initially present had fully dissolved and the cations released had subsequently precipitated in carbonate minerals. The carbonation fractions observed in batch experiments with olivine grains and powders varied significantly, from less than 0.01 (1%) to more than 0.5 (50%). Over time, the carbonation fractions reached an upper limit after about 24 to 72 hours of reaction, then stayed constant or decreased. The peak Final Scientific/Technical Report DE-FE0004275 | Mineral Carbonation | 4 coincided with the appearance of secondary magnesium-bearing silicate minerals, whose formation competes for magnesium ions in solution and can even promote conditions that dissolve magnesite. The highest carbonation fractions resulted from experiments with low ratios of concentrated solution to olivine, during which amorphous silica spheres or meshes formed, instead of secondary silicate minerals. The highest carbonation fractions appear to result from competing effects. Precipitation of silica layers on olivine reduces the reactive surface area and, thus, the rate of olivine dissolution (which ultimately limits the carbonation rate), but these same silica layers can also inhibit the formation of secondary silicate minerals that consume magnesite formed in earlier stages of carbonation. Simulation of these experiments with simple geochemical models using the software program EQ3/6 reproduces the general trends observed—especially the results for the carbonation fraction in short-run experiments. Although further experimentation and better models are needed, this study nevertheless provides a framework for understanding the optimal conditions for sequestering carbon dioxide by reacting CO 2-bearing fluids with rocks containing olivine minerals. A series of experiments at the Rock Physics Laboratory at the University of Maryland studied the carbonation process during deformation of thermally cracked olivine-rich rock samples (dunite) saturated with CO 2 brines of varying compositions. A goal of these geomechanical experiments was to see if flow and deformation processes, which accompany natural carbonation reactions in underground settings, work to enhance or inhibit the reactions. The experiments involved hydrostatic compaction, followed by deformation at a constant rate of strain. Sample permeability was monitored during the reactions. Comparison of the samples’ volume changes to their axial strains (shortening) during deformation indicates that samples reacted with CO 2-saturated brines accommodate more axial compaction, before the onset of dilation (a swelling that precedes rock failure), than samples reacted with distilled water. Analyses of the reacted samples with scanning electron microscope (SEM) images indicate, first, that dissolution of olivine occurring in the initial stages of carbonation can provide pathways to fluid flow that sustain the reaction, and, second, that carbonate minerals precipitated along existing fractures in the rocks may serve as asperities, or roughness on a crack’s surface that restricts its closure. Final Scientific/Technical Report DE-FE0004275 | Mineral Carbonation | 5 In a related study undertaken by one of the principal investigators as a spin-off of the main project, a simple model of (magnesite) crystal growth in the pore space of basalts undergoing carbonation was developed. The model suggests that, under a carefully controlled program of CO 2 injection, carbonate mineral growth can harden the rock formation against earthquakes that might otherwise be induced by the injection of large fluid volumes (Yarushina and Bercovici, 2013). The overall conclusion of the research project is that mineral carbonation of underground mafic and ultramafic rock formations is a viable candidate for long-term sequestration of man-made carbon dioxide. No results obtained during the project indicate that the method is inherently intractable in its implementation; moreover, enormous volumes of basalt near Earth’s surface are candidate locations for large-scale injection programs. The geochemical experiments do indicate, however, that there will be significant engineering challenges in maintaining high rates of carbonation, by delaying the onset of chemical conditions that promote formation of secondary silicate minerals and, therefore, slow down, or even reverse, the carbonation process. It remains an open question as to whether carbonation processes can be sustained for many years in an engineered system operating on a large scale—a scale capable of accommodating millions of tons of CO 2 annually. The development of realistic theoretical models that can systematically describe the combined effects of reactive flow, precipitation and geomechanical deformation is a major barrier to further understanding of the practical viability of mineral carbonation as large-scale method of carbon sequestration.« less

Interaction of Rock Minerals with Carbon Dioxide and Brine: A Hydrothermal Investigation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sass, Bruce M.; Gupta, Neeraj; Ickes, Jennifer A.

2002-02-02

This paper presents interim results of a feasibility study on carbon dioxide (CO{sub 2}) sequestration in deep saline formations. The focus of the investigation is to examine factors that may affect chemical sequestration of CO{sub 2} in deep saline formations. Findings of the first phase of this investigation were presented in a topical report (Sass et al., 1999a). Preliminary results of the second phase, now underway, have been reported elsewhere (Sass et al., 1999b; 2001). Evaluations of the suitability of Mt. Simon formation for sequestering CO{sub 2} and economic issues are reported by Gupta et al., 1999; 2001; Smith etmore » al., 2001. This study is sponsored by the U.S. Department of Energy's (DOE) National Energy Technology Laboratory (NETL) under a Novel Concepts project grant. The overall objectives of Phase II experiments were to determine: (1) the potential for long-term sequestration of CO{sub 2} in deep, regional host rock formations; and (2) the effectiveness of overlying caprock as a barrier against upward migration of the injected CO{sub 2}. To meet these goals, experiments were conducted using rock samples from different potential host reservoirs and overlying rocks. In addition, pure mineral samples were used in some experimental runs to investigate specific mineralogical reactions. Due to space limitations, the scope of this paper will be limited to two types of equilibration experiments using pure minerals. Implications for more complex natural systems will be discussed in the report for Phase II being finalized at this time.« less

Interactions between microbial iron reduction and metal geochemistry: effect of redox cycling on transition metal speciation in iron bearing sediments.

PubMed

Cooper, D Craig; Picardal, Flynn F; Coby, Aaron J

2006-03-15

Microbial iron reduction is an important biogeochemical process that can affect metal geochemistry in sediments through direct and indirect mechanisms. With respectto Fe(III) (hydr)oxides bearing sorbed divalent metals, recent reports have indicated that (1) microbial reduction of goethite/ferrihydrite mixtures preferentially removes ferrihydrite, (2) this process can incorporate previously sorbed Zn(II) into an authigenic crystalline phase that is insoluble in 0.5 M HCl, (3) this new phase is probably goethite, and (4) the presence of nonreducible minerals can inhibit this transformation. This study demonstrates that a range of sorbed transition metals can be selectively sequestered into a 0.5 M HCl insoluble phase and that the process can be stimulated through sequential steps of microbial iron reduction and air oxidation. Microbial reduction experiments with divalent Cd, Co, Mn, Ni, Pb, and Zn indicate that all metals save Mn experienced some sequestration, with the degree of metal incorporation into the 0.5 M HCl insoluble phase correlating positively with crystalline ionic radius at coordination number = 6. Redox cycling experiments with Zn adsorbed to synthetic goethite/ferrihydrite or iron-bearing natural sediments indicate that redox cycling from iron reducing to iron oxidizing conditions sequesters more Zn within authigenic minerals than microbial iron reduction alone. In addition, the process is more effective in goethite/ferrihydrite mixtures than in iron-bearing natural sediments. Microbial reduction alone resulted in a -3x increase in 0.5 M HCl insoluble Zn and increased aqueous Zn (Zn-aq) in goethite/ferrihydrite, but did not significantly affect Zn speciation in natural sediments. Redox cycling enhanced the Zn sequestration by approximately 12% in both goethite/ferrihydrite and natural sediments and reduced Zn-aq to levels equal to the uninoculated control in goethite/ferrihydrite and less than the uninoculated control in natural sediments. These data suggest that in situ redox cycling may serve as an effective method for

Calcium silicates synthesised from industrial residues with the ability for CO2 sequestration.

PubMed

Morales-Flórez, Victor; Santos, Alberto; López, Antonio; Moriña, Isabel; Esquivias, Luis

2014-12-01

This work explored several synthesis routes to obtain calcium silicates from different calcium-rich and silica-rich industrial residues. Larnite, wollastonite and calcium silicate chloride were successfully synthesised with moderate heat treatments below standard temperatures. These procedures help to not only conserve natural resources, but also to reduce the energy requirements and CO2 emissions. In addition, these silicates have been successfully tested as carbon dioxide sequesters, to enhance the viability of CO2 mineral sequestration technologies using calcium-rich industrial by-products as sequestration agents. Two different carbon sequestration experiments were performed under ambient conditions. Static experiments revealed carbonation efficiencies close to 100% and real-time resolved experiments characterised the dynamic behaviour and ability of these samples to reduce the CO2 concentration within a mixture of gases. The CO2 concentration was reduced up to 70%, with a carbon fixation dynamic ratio of 3.2 mg CO2 per g of sequestration agent and minute. Our results confirm the suitability of the proposed synthesis routes to synthesise different calcium silicates recycling industrial residues, being therefore energetically more efficient and environmentally friendly procedures for the cement industry. © The Author(s) 2014.

Lead sequestration and species redistribution during soil organic matter decomposition

USGS Publications Warehouse

Schroth, A.W.; Bostick, B.C.; Kaste, J.M.; Friedland, A.J.

2008-01-01

The turnover of soil organic matter (SOM) maintains a dynamic chemical environment in the forest floor that can impact metal speciation on relatively short timescales. Here we measure the speciation of Pb in controlled and natural organic (O) soil horizons to quantify changes in metal partitioning during SOM decomposition in different forest litters. We provide a link between the sequestration of pollutant Pb in O-horizons, estimated by forest floor Pb inventories, and speciation using synchrotron-based X-ray fluorescence and X-ray absorption spectroscopy. When Pb was introduced to fresh forest Oi samples, it adsorbed primarily to SOM surfaces, but as decomposition progressed over two years in controlled experiments, up to 60% of the Pb was redistributed to pedogenic birnessite and ferrihydrite surfaces. In addition, a significant fraction of pollutant Pb in natural soil profiles was associated with similar mineral phases (???20-35%) and SOM (???65-80%). Conifer forests have at least 2-fold higher Pb burdens in the forest floor relative to deciduous forests due to more efficient atmospheric scavenging and slower organic matter turnover. We demonstrate that pedogenic minerals play an important role in surface soil Pb sequestration, particularly in deciduous forests, and should be considered in any assessment of pollutant Pb mobility. ?? 2008 American Chemical Society.

Nitrogen controls on ecosystem carbon sequestration: a model implementation and application to Saskatchewan, Canada

USGS Publications Warehouse

Liu, J.; Price, D.T.; Chen, J.M.

2005-01-01

A plant–soil nitrogen (N) cycling model was developed and incorporated into the Integrated BIosphere Simulator (IBIS) of Foley et al. [Foley, J.A., Prentice, I.C., Ramankutty, N., Levis, S., Pollard, D., Sitch, S., Haxeltine, A., 1996. An integrated biosphere model of land surface process, terrestrial carbon balance and vegetation dynamics. Global Biogeochem. Cycles 10, 603–628]. In the N-model, soil mineral N regulates ecosystem carbon (C) fluxes and ecosystem C:N ratios. Net primary productivity (NPP) is controlled by feedbacks from both leaf C:N and soil mineral N. Leaf C:N determines the foliar and canopy photosynthesis rates, while soil mineral N determines the N availability for plant growth and the efficiency of biomass construction. Nitrogen controls on the decomposition of soil organic matter (SOM) are implemented through N immobilization and mineralization separately. The model allows greater SOM mineralization at lower mineral N, and conversely, allows greater N immobilization at higher mineral N. The model's seasonal and inter-annual behaviours are demonstrated. A regional simulation for Saskatchewan, Canada, was performed for the period 1851–2000 at a 10 km × 10 km resolution. Simulated NPP was compared with high-resolution (1 km × 1 km) NPP estimated from remote sensing data using the boreal ecosystem productivity simulator (BEPS) [Liu, J., Chen, J.M., Cihlar, J., Park, W.M., 1997. A process-based boreal ecosystem productivity simulator using remote sensing inputs. Remote Sens. Environ. 44, 81–87]. The agreement between IBIS and BEPS, particularly in NPP spatial variation, was considerably improved when the N controls were introduced into IBIS.

Geologic Sequestration of CO2: Potential Permeability Changes in Host Formations of the San Juan Basin, New Mexico

NASA Astrophysics Data System (ADS)

Abel, A. P.; McPherson, B.; Lichtner, P.; Bond, G.; Stringer, J.; Grigg, R.

2002-12-01

Terrestrial sequestration through injection into geologic formations is one proposed method for the isolation of anthropogenic CO2 from the atmosphere. A variety of physical and chemical processes are known to occur both during and after geologic CO2 injection, including diagenetic chemical reactions and associated permeability changes. Although it is commonly assumed that CO2 sequestered in this way will ultimately become mineralized, the rates of these changes, including CO2 hydration in brines, are known to be relatively slow. Bond and others (this volume) have developed a biomimetic approach to CO2 sequestration, in which the rate of CO2 hydration is accelerated by the use of a biological catalyst. Together with the hydrated CO2, cations from produced brines may be used to form solid-state carbonate minerals at the earth's surface, or this bicarbonate solution may be reinjected for geologic sequestration. Chemical composition of produced brines will affect both the diagenetic reactions that occur within the host formation, and the precipitation reactions that will occur above ground. In a specific case study of the San Juan Basin, New Mexico, we are cataloging different brines present in that basin. We are using this information to facilitate evaluation of potential applications of the biomimetic process and geologic sequestration. In a separate collaborative study by Grigg and others (this volume), laboratory experiments have been conducted on multiphase CO2 and brine injection and flow through saturated rock cores. We are extending from that study to our specific case study of the San Juan basin, to examine and characterize potential permeability changes associated with accelerated diagenesis due to the presence of high concentrations of CO2 or bicarbonate solutions in situ. We are developing and conducting new laboratory experiments to evaluate relative permeability (to CO2 and brine) of selected strata from the Fruitland Formation and Pictured Cliffs Sandstone. In addition to relative permeability, we are conducting longer-term flow tests reflecting marked permeability changes, and documenting the changes by comparing detailed pre-test measurements of porosity and permeability to post-test measurements. We are using these experimental results to parameterize coupled-flow and reactive-chemistry models of a selected cross-section of the San Juan basin. Our flow and chemistry model is based on the Los Alamos National Laboratory reactive chemistry simulator, TRANS, coupled to the Lawrence Berkeley Laboratory flow simulator, TOUGH2. The purpose of these simulation models is to evaluate potential CO2- and bicarbonate-induced diagenetic changes in permeability and flow at the basin-scale. In addition they will provide useful information in relation to brine extraction. We are also using these calibrated basin models to examine natural diagenesis and permeability evolution associated with changing brine properties and flow conditions over geologic time.

Influence of Oxalate on Ni Fate during Fe(II)-Catalyzed Recrystallization of Hematite and Goethite.

PubMed

Flynn, Elaine D; Catalano, Jeffrey G

2018-06-05

During biogeochemical iron cycling at redox interfaces, dissolved Fe(II) induces the recrystallization of Fe(III) oxides. Oxalate and other organic acids promote dissolution of these minerals and may also induce recrystallization. These processes may redistribute trace metals among the mineral bulk, mineral surface, and aqueous solution. However, the impact of interactions among organic acids, dissolved Fe(II), and iron oxide minerals on trace metal fate in such systems is unclear. The present study thus explores the effect of oxalate on Ni release from and incorporation into hematite and goethite in the absence and presence of Fe(II). When Ni is initially structurally incorporated into the iron oxides, both oxalate and dissolved Fe(II) promote the release of Ni to aqueous solution. When both species are present, their effects on Ni release are synergistic at pH 7 but inhibitory at pH 4, indicating that cooperative and competitive interactions vary with pH. In contrast, oxalate suppresses Ni incorporation into goethite and hematite during Fe(II)-induced recrystallization, decreasing the proportion of Ni substituting in a mineral structure by up to 36%. These observations suggest that at redox interfaces oxalate largely enhances trace metal mobility. In such settings, oxalate, and likely other organic acids, may thus enhance micronutrient availability and inhibit contaminant sequestration.

Experimental design applications for modeling and assessing carbon dioxide sequestration in saline aquifers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rogers, John

2014-11-29

This project was a computer modeling effort to couple reservoir simulation and ED/RSM using Sensitivity Analysis, Uncertainty Analysis, and Optimization Methods, to assess geologic, geochemical, geomechanical, and rock-fluid effects and factors on CO 2 injectivity, capacity, and plume migration. The project objective was to develop proxy models to simplify the highly complex coupled geochemical and geomechanical models in the utilization and storage of CO 2 in the subsurface. The goals were to investigate and prove the feasibility of the ED/RSM processes and engineering development, and bridge the gaps regarding the uncertainty and unknowns of the many geochemical and geomechanical interactingmore » parameters in the development and operation of anthropogenic CO 2 sequestration and storage sites. The bottleneck in this workflow is the high computational effort of reactive transport simulation models and large number of input variables to optimize with ED/RSM techniques. The project was not to develop the reactive transport, geomechanical, or ED/RSM software, but was to use what was commercially and/or publically available as a proof of concept to generate proxy or surrogate models. A detailed geologic and petrographic mineral assemblage and geologic structure of the doubly plunging anticline was defined using the USDOE RMOTC formations of interest data (e.g., Lower Sundance, Crow Mountain, Alcova Limestone, and Red Peak). The assemblage of 23 minerals was primarily developed from literature data and petrophysical (well log) analysis. The assemblage and structure was input into a commercial reactive transport simulator to predict the effects of CO 2 injection and complex reactions with the reservoir rock. Significant impediments were encountered during the execution phase of the project. The only known commercial reactive transport simulator was incapable of simulating complex geochemistry modeled in this project. Significant effort and project funding was expended to determine the limitations of both the commercial simulator and the Lawrence Berkeley National Laboratory (LBNL) R&D simulator, TOUGHREACT available to the project. A simplified layer cake model approximating the volume of the RMOTC targeted reservoirs was defined with 1-3 minerals eventually modeled with limited success. Modeling reactive transport in porous media requires significant computational power. In this project, up to 24 processors were used to model a limited mineral set of 1-3 minerals. In addition, geomechanical aspects of injecting CO 2 into closed, semi-open, and open systems in various well completion methods was simulated. Enhanced Oil Recovery (EOR) as a storage method was not modeled. A robust and stable simulation dataset or base case was developed and used to create a master dataset with embedded instructions for input to the ED/RSM software. Little success was achieved toward the objective of the project using the commercial simulator or the LBNL simulator versions available during the time of this project. Several hundred realizations were run with the commercial simulator and ED/RSM software, most having convergence problems and terminating prematurely. A proxy model for full field CO 2 injection sequestration utilization and storage was not capable of being developed with software available for this project. Though the chemistry is reasonably known and understood, based on the amount of effort and huge computational time required, predicting CO 2 sequestration storage capacity in geologic formations to within the program goals of ±30% proved unsuccessful.« less

Mineral Influence on Microbial Survival During Carbon Sequestration

NASA Astrophysics Data System (ADS)

Santillan, E. U.; Shanahan, T. M.; Wolfe, W. W.; Bennett, P.

2012-12-01

CO2 sequestered in a deep saline aquifer will perturb subsurface biogeochemistry by acidifying the groundwater and accelerating mineral diagenesis. Subsurface microbial communities heavily influence geochemistry through their metabolic processes, such as with dissimilatory iron reducing bacteria (DIRB). However, CO2 also acts as a sterilant and will perturb these communities. We investigated the role of mineralogy and its effect on the survival of microbes at high PCO2 conditions using the model DIRB Shewanella oneidensis MR-1. Batch cultures of Shewanella were grown to stationary phase and exposed to high PCO2 using modified Parr reactors. Cell viability was then determined by plating cultures after exposure. Results indicate that at low PCO2 (2 bar), growth and iron reduction are decreased and cell death occurs within 1 hour when exposed to CO2 pressures of 10 bar or greater. Further, fatty acid analysis indicates microbial lipid degradation with C18 fatty acids being the slowest lipids to degrade. When cultures were grown in the presence of rocks or minerals representative of the deep subsurface such as carbonates and silicates and exposed to 25 bar CO2, survival lasted beyond 2 hours. The most effective protecting substratum was quartz sandstone, with cultures surviving beyond 8 hours of CO2 exposure. Scanning electron microscope images reveal biofilm formation on the mineral surfaces with copious amounts of extracellular polymeric substances (EPS) present. EPS from these biofilms acts as a reactive barrier to the CO2, slowing the penetration of CO2 into cells and resulting in increased survival. When biofilm cultures were grown with Al and As to simulate the release of toxic metals from minerals such as feldspars and clays, survival time decreased, indicating mineralogy may also enhance microbial death. Biofilms were then grown on iron-coated quartz sand to determine conversely what influence biofilms may have on mineral dissolution during CO2 perturbation. Growth media was allowed to flow through a sand-packed column at a constant flow rate with pulses of liquid CO2 injected directly into the column. Preliminary data of dissolved iron measured from the effluent indicates that biofilm columns show a slight increase in dissolved iron concentrations before and after CO2 exposure in comparison to abiotic columns. These findings imply the important relationship between microbes and minerals during CO2 sequestration. The ability minerals have to contribute to the selection of microbes has important consequences to the survival of different microbial populations in the subsurface and the consequent biogeochemical changes that may happen.

Stormwater Effects on Heavy Metal Sequestration in a Bioretention System in Culver City, California

NASA Astrophysics Data System (ADS)

Yousavich, D. J.; Ellis, A. S.; Dorsey, J.; Johnston, K.

2017-12-01

Rain Gardens, also referred to as bioretention or biofilters, are often used to capture or filter urban runoff before it drains into surface or groundwater systems. The Culver City Rain Garden (CCRG) is one such system that is designed to capture and filter runoff from approximately 11 acres of mixed-use commercial and industrial land before it enters Ballona Creek. The EPA has designated Ballona Creek as an impaired waterway and established Total Maximum Daily Loads for heavy metals. Previous research has utilized sequential extractions to establish trends in heavy metal sequestration for Cu, Pb, and Zn in bioretention media. The aim of this project is to evaluate if there is a difference in heavy metal sequestration between dry and wetted bioretention media. To characterize the stormwater at the site, influent and surface water were collected and analyzed for sulfate and heavy metals 3 times during the 2016-2017 storm season. Two soil cores from the CCRG were acquired in the summer of 2017 to analyze soil metal sequestration trends. They will be subjected to different wetting conditions, sectioned into discrete depths, and digested with an established sequential extraction technique. Surface water in the CCRG shows average Dissolved Oxygen during wet conditions of 2.92 mg/L and average pH of 6.1 indicating reducing conditions near the surface and the possible protonation of adsorption sites during wet weather conditions. Influent metal data indicate average dissolved iron levels near 1 ppm and influent Cu, Pb, and Zn levels near 0.05, 0.01, and 0.5 ppm respectively. This coupled with average surface water sulfate levels near 3 ppm indicates the potential for iron oxide and sulfide mineral formation depending on redox conditions. The sequential extraction results will elucidate whether heavy metals are adsorbed or are being sequestered in mineral formation. These results will allow for the inclusion of heavy metal sequestration trends in the design of further bioretention projects and maintenance of current sites.

Reducing soluble phosphorus in dairy effluents through application of mine drainage residuals

USGS Publications Warehouse

Sibrell, Philip L.; Penn, Chad J.; Hedin, Robert S.

2015-01-01

Three different dairy manure wastewater effluent samples were amended with mine drainage residuals (MDR) to evaluate the suitability of MDR for sequestration of phosphorus (P). Geochemical modeling of the manure wastewater compositions indicated that partially soluble P-bearing minerals including hydroxyapatite, octacalcium phosphate, and vivianite were all oversaturated in each of the manure wastewater samples. Initial MDR amendment test results indicated that these partially soluble P minerals suspended in the wastewater replenished P in the water phase as it was sorbed by the MDR samples. Further investigations revealed that the MDR samples were effective in decreasing soluble P when the amended manure was tested using the water-extractable P procedure. Under these conditions, up to 90 percent of the soluble P in the manure was converted to a sorbed, water-insoluble state. Water contamination and large-scale validation tests of the process were also conducted.

Trends, application and future prospectives of microbial carbonic anhydrase mediated carbonation process for CCUS.

PubMed

Bhagat, C; Dudhagara, P; Tank, S

2018-02-01

Growing industrialization and the desire for a better economy in countries has accelerated the emission of greenhouse gases (GHGs), by more than the buffering capacity of the earth's atmosphere. Among the various GHGs, carbon dioxide occupies the first position in the anthroposphere and has detrimental effects on the ecosystem. For decarbonization, several non-biological methods of carbon capture, utilization and storage (CCUS) have been in use for the past few decades, but they are suffering from narrow applicability. Recently, CO 2 emission and its disposal related problems have encouraged the implementation of bioprocessing to achieve a zero waste economy for a sustainable environment. Microbial carbonic anhydrase (CA) catalyses reversible CO 2 hydration and forms metal carbonates that mimic the natural phenomenon of weathering/carbonation and is gaining merit for CCUS. Thus, the diversity and specificity of CAs from different micro-organisms could be explored for CCUS. In the literature, more than 50 different microbial CAs have been explored for mineral carbonation. Further, microbial CAs can be engineered for the mineral carbonation process to develop new technology. CA driven carbonation is encouraging due to its large storage capacity and favourable chemistry, allowing site-specific sequestration and reusable product formation for other industries. Moreover, carbonation based CCUS holds five-fold more sequestration capacity over the next 100 years. Thus, it is an eco-friendly, feasible, viable option and believed to be the impending technology for CCUS. Here, we attempt to examine the distribution of various types of microbial CAs with their potential applications and future direction for carbon capture. Although there are few key challenges in bio-based technology, they need to be addressed in order to commercialize the technology. © 2017 The Society for Applied Microbiology.

Importance of charcoal in determining the age and chemistry of organic carbon in surface soils

NASA Astrophysics Data System (ADS)

Krull, Evelyn S.; Swanston, Christopher W.; Skjemstad, Jan O.; McGowan, Janine A.

2006-12-01

Understanding the chemical character and turnover time of the oldest soil organic carbon (SOC) fraction is fundamental in deciphering soil carbon sequestration processes and the fate of soil-eroded carbon in aquatic sediments. Two main processes are thought to extend the turnover time of SOC: protection by the mineral matrix and chemical recalcitrance. Various oxidation methods have been proposed to isolate the oldest and most recalcitrant SOC fraction, which is often assumed to be black carbon (BC). However, few data have been published that confirm the chemical character of the isolated fractions. Using established and newly developed methods together with 13C-NMR spectroscopy and AMS dating, we show that protection by the mineral matrix prolonged the turnover time of SOC by tens of years, but long-term (hundreds of years) stabilization was controlled by the inherent recalcitrance of SOC, determined by the type of ecosystems. In ecosystem without significant fire occurrences, the older SOC pool was comparably small and was represented by alkyl carbon. In ecosystems with high fire frequency charcoal constituted the oldest SOC pool, and constituted up to 35% of the total SOC. By applying methods with different oxidative strengths, it was possible to isolate different age groups of charcoal with different degrees of weathering. Further substantiation of this finding could provide a much greater resolution of paleo-fire events. Our results demonstrate that fire frequency plays a dominant role in determining the chemical nature and 14C abundance of SOC and that the separation of age groups of charcoal provides a means to reconstruct detailed fire histories. Our results indicate that modeling SOC turnover, transport and sequestration for frequently burnt environments requires modification of existing models, specifying an input and decay function for the charcoal pool in different environments.

IN SITU MAGIC ANGLE SPINNING NMR FOR STUDYING GEOLOGICAL CO(2) SEQUESTRATION

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hoyt, David W.; Turcu, Romulus VF; Sears, Jesse A.

2011-03-27

Geological carbon sequestration (GCS) is one of the most promising ways of mitigating atmospheric greenhouse gases (1-3). Mineral carbonation reactions are potentially important to the long-term sealing effectiveness of caprock but remain poorly predictable, particularly in low-water supercritical CO2 (scCO2)-dominated environments where the chemistry has not been adequately explored. In situ probes that provide molecular-level information is desirable for investigating mechanisms and rates of GCS mineral carbonation reactions. MAS-NMR is a powerful tool for obtaining detailed molecular structure and dynamics information of a system regardless whether the system is in a solid, a liquid, a gaseous, or a supercritical state,more » or a mixture thereof (4,5). However, MAS NMR under scCO2 conditions has never been realized due to the tremendous technical difficulties of achieving and maintaining high pressure within a fast spinning MAS rotor (6,7), where non-metal materials must be used. In this work, we report development of a unique high pressure MAS NMR capability, and its application to mineral carbonation chemistry in scCO2 under geologically relevant temperatures and pressures.« less

Are seismic velocity time-lapse changes due to fluid substitution or matrix dissolution? A CO2 sequestration study at Pohokura Field, New Zealand

NASA Astrophysics Data System (ADS)

Adam, L.; Sim, C. Y.; Macfarlane, J.; van Wijk, K.; Shragge, J. C.; Higgs, K.

2015-12-01

Time-lapse seismic signatures can be used to quantify fluid saturation and pressure changes in a reservoir undergoing CO2 sequestration. However, the injection of CO2 acidifies the water, which may dissolve and/or precipitate minerals. Understanding the impact on the rock frame from field seismic time-lapse changes remains an outstanding challenge. Here, we study the effects of carbonate-CO2-water reactions on the physical and elastic properties of rock samples with variable volumes of carbonate cementation. The effects of fluid substitution alone (brine to CO2) and those due to the combination of fluid substitution and mineral dissolution on time-lapse seismic signatures are studied by combining laboratory data, geophysical well-log data and 1-D seismic modeling. Nine rocks from Pohokura Field (New Zealand) are reacted with carbonic acid. The elastic properties are measured using a high-density laser-ultrasonic setup. We observe that P-wave velocity changes up to -19% and correlate with sandstone grain size. Coarse-grained sandstones show greater changes in elastic wave velocities due to dissolution than fine-grained sandstones. To put this in perspective, this velocity change is comparable to the effect of fluid substitution from brine to CO2. This can potentially create an ambiguity in the interpretation of the physical processes responsible for time-lapse signatures in a CO2injection scenario. The laboratory information is applied onto well-log data to model changes in elastic properties of sandstones at the well-log scale. Well-logs and core petrographic analyses are used to find an elastic model that best describes the observed elastic waves velocities in the cemented reservoir sandstones. The Constant-cement rock physics model is found to predict the elastic behaviour of the cemented sandstones. A possible late-time sequestration scenario is that both mineral dissolution and fluid substitution occur in the reservoir. 1-D synthetic seismograms show that seismic amplitudes can change up to 126% in such a scenario. Our work shows that it is important to consider that time-lapse seismic signatures in carbonate-cemented reservoirs can result not only from fluid and pressure changes but also potentially from chemical reaction between CO2-water mixtures and carbonate cemented sandstones.

Effect of CO2 Solubility on Dissolution Rates of Minerals in Porous Media Imbibed with Brine: Actual Efficiency of CO2 Sequestration

NASA Astrophysics Data System (ADS)

Alizadeh Nomeli, M.; Riaz, A.

2016-12-01

A new model is developed for geochemical reactions to access dissolution rate of minerals in saline aquifers with respect to saturated concentration of dissolved CO2 as a function of parameters that are dynamically available during computer program execution such as pressure, temperature, and salinity. A general Arrhenius-type equation, with an explicit dependence on the pH of brine, is employed to determine the rates of mineral dissolution. The amount of dissolved CO2 is determined with the help of an accurate PVTx model for the temperature range of 50-100C and pressures up to 600 bar relevant to the geologic sequestration of CO2. We show how activity coefficients for a given salinity condition alters solubility, pH, and reaction rates. We further evaluate the significance of the pre-exponential factor and the reaction order associated with the modified Arrhenius equation to determine the sensitivity of the reaction rates as a function to the pH of the system. It is found that the model can reasonably reproduce experimental data with new parameters that we obtain from sensitivity studies. Using the new rate equation, we investigate geochemically induced alterations of fracture geometry due to mineral dissolution. Finally, we use our model to evaluate the effects of temperature, pressure, and salinity on the actual efficiency of CO2 storage.

Competitive and Cooperative Effects during Nickel Adsorption to Iron Oxides in the Presence of Oxalate

DOE Office of Scientific and Technical Information (OSTI.GOV)

Flynn, Elaine D.; Catalano, Jeffrey G.

Iron oxides are ubiquitous in soils and sediments and play a critical role in the geochemical distribution of trace elements and heavy metals via adsorption and coprecipitation. The presence of organic acids may potentially alter how metals associate with iron oxide minerals through a series of cooperative or competitive processes: solution complexation, ternary surface complexation, and surface site competition. The macroscopic and molecular-scale effects of these processes were investigated for Ni adsorption to hematite and goethite at pH 7 in the presence of oxalate. The addition of this organic acid suppresses Ni uptake on both minerals. Aqueous speciation suggests thatmore » this is dominantly the result of oxalate complexing and solubilizing Ni. Comparison of the Ni surface coverage to the concentration of free (uncomplexed) Ni 2+ in solution suggests that the oxalate also alters Ni adsorption affinity. EXAFS and ATR-FTIR spectroscopies indicate that these changes in binding affinity are due to the formation of Ni–oxalate ternary surface complexes. These observations demonstrate that competition between dissolved oxalate and the mineral surface for Ni overwhelms the enhancement in adsorption associated with ternary complexation. Oxalate thus largely enhances Ni mobility, thereby increasing micronutrient bioavailability and inhibiting contaminant sequestration.« less

Density functional simulations as a tool to probe molecular interactions in wet supercritical CO2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Glezakou, Vassiliki Alexandra; McGrail, B. Peter

2013-06-03

Recent advances in mixed Gaussian and plane wave algorithms have made possible the effective use of density functional theory (DFT) in ab initio molecular dynamics (AIMD) simulations for large and chemically complex models of condensed phase materials. In this chapter, we are reviewing recent progress on the modeling and characterization of co-sequestration processes and reactivity in wet supercritical CO2 (sc-CO2). We examine the molecular transformations of mineral and metal components of a sequestration system in contact with water-bearing scCO2 media and aim to establish a reliable correspondence between experimental observations and theory models with predictive ability and transferability of resultsmore » in large scale geomechanical simulators. This work is funded by the Department of Energy, Office of Fossil Energy. A portion of the research was performed using EMSL, a national scientific user facility sponsored by the Department of Energy’s Office of Biological and Environmental Research located at Pacific Northwest National Laboratory. The Pacific Norhtwest National Laboratory (PNNL) is operated by Battelle for DOE under contract DE-AC06-76RL01830.« less

A kinetic rate model for crystalline basalt dissolution at temperature and pressure conditions relevant for geologic CO2 sequestration

NASA Astrophysics Data System (ADS)

Pollyea, R.; Rimstidt, J. D.

2016-12-01

Geologic carbon sequestration in terrestrial basalt reservoirs is predicated on permanent CO2 trapping through CO2-water-rock dissolution reactions followed by carbonate precipitation. Bench-scale experiments have shown these reaction paths to be rapid, occurring on a timescale 100 - 102 years. Moreover, recent results from the CarbFix basalt sequestration pilot project in Iceland demonstrate >95% CO2 isolation two years after a small-scale injection. In order to assess the viability of basalt sequestration worldwide (e.g., Deccan Traps, Columbia Plateau, etc.), flexible simulation tools are required that distill the dissolution reactions into a user-friendly format that is readily transmissible to existing reactive transport numerical simulators. In the present research, we combine experimental results extant in the literature for Icelandic basalt to develop kinetic rate models describing the pH-dependent dissolution of (1) basaltic glass and (2) an aggregate mineral assemblage for crystalline basalt comprising olivine, pyroxene, and plagioclase phases. In order to utilize these kinetic rate models with numerical simulation, a thermodynamic solubility model for each phase is developed for use with the reactive transport simulation code, TOUGHREACT. We use reactive transport simulation in a simple 1-D reactor to compare dissolution of the aggregate crystalline basalt phase with the traditional formulation comprising individual mineral phases for the crystalline basalt. Simulation results are in general agreement, illustrating the efficacy of this simplified approach for modeling basalt dissolution at temperature and pressure conditions typical of geologic CO2 reservoirs. Moreover, this approach may be of value to investigators seeking dissolution models for crystalline basalt in other mafic provinces.

Anisotropy of permeability of reservoir rocks over Miaoli area, NW Taiwan.

NASA Astrophysics Data System (ADS)

Bo-Siang, Xiong; Loung-Yie, Tsai

2013-04-01

The amount of the CO2 has risen since the Industrial Evolution. In order to reduce the amount of CO2 in atmosphere, CO2 sequestration is considered to be the most effective way. In recent years, research about subsurface storage of CO2 into geological formations has increased rapidly. Assessment of storage capability is needed before selecting a site for sequestration. Porosity and permeability are important assessment factors for CO2 sequestration in reservoir rocks. In order to improve the assessment, reservoir rock properties are important and need to be evaluated in advance. Porosity of sandstone is controlled by texture and degree of cementation, whereas permeability is controlled by pore-throat size, pore types and connectivity of pore throat. Sandstones of Miocene to Pleistocene in Miaoli area, NW Taiwan, were collected in this study. YOKO2 porosity/permeability detector is used to measure their permeability perpendicular and parallel to bedding planes under 3 to 60MPa confining pressure with Helium as media. Optical microscope and scanning electron microscope (SEM) were then used to observe the mineral composition, lithology, texture and pore type of sandstones, so as to explore the influence of rock properties on porosity and anisotropy of permeability, as well as the storage potential for CO2 sequestration in the future. The experimental results show that most of the horizontal permeability exceeds the vertical permeability and the anisotropy increases with increasing confining pressure. Mineral composition of sandstones studied were mainly quartz and lithic with little feldspar content. The pore types were mainly primary pores and micropores in this study. The correlation between quantity of macropores and permeability were higher than total porosity and permeability, mainly due to total porosity contains micropores which contribute little to permeability.

Effects of mineral additives on biochar formation: carbon retention, stability, and properties.

PubMed

Li, Feiyue; Cao, Xinde; Zhao, Ling; Wang, Jianfei; Ding, Zhenliang

2014-10-07

Biochar is being recognized as a promising tool for long-term carbon sequestration, and biochar with high carbon retention and strong stability is supposed to be explored for that purpose. In this study, three minerals, including kaolin, calcite (CaCO3), and calcium dihydrogen phosphate [Ca(H2PO4)2], were added to rice straw feedstock at the ratio of 20% (w/w) for biochar formation through pyrolysis treatment, aiming to improve carbon retention and stabilization in biochar. Kaolin and CaCO3 had little effect on the carbon retention, whereas Ca(H2PO4)2 increased the carbon retention by up to 29% compared to untreated biochar. Although the carbon loss from the kaolin-modified biochar with hydrogen peroxide oxidation was enhanced, CaCO3 and Ca(H2PO4)2 modification reduced the carbon loss by 18.6 and 58.5%, respectively. Moreover, all three minerals reduced carbon loss of biochar with potassium dichromate oxidation from 0.3 to 38.8%. The microbial mineralization as CO2 emission in all three modified biochars was reduced by 22.2-88.7% under aerobic incubation and 5-61% under anaerobic incubation. Enhanced carbon retention and stability of biochar with mineral treatment might be caused by the enhanced formation of aromatic C, which was evidenced by cross-polarization magic angle spinning (13)C nuclear magnetic resonance spectra and Fourier transform infrared spectroscopy analysis. Our results indicated that the three minerals, especially Ca(H2PO4)2, were effective in increasing carbon retention and strengthening biochar stabilization, which provided a novel idea that people could explore and produce the designated biochar with high carbon sequestration capacity and stability.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mouzakis, Katherine M.; Navarre-Sitchler, Alexis K.; Rother, Gernot

Carbon capture, utilization, and storage, one proposed method of reducing anthropogenic emissions of CO 2, relies on low permeability formations, such as shales, above injection formations to prevent upward migration of the injected CO 2. Porosity in caprocks evaluated for sealing capacity before injection can be altered by geochemical reactions induced by dissolution of injected CO 2 into pore fluids, impacting long-term sealing capacity. Therefore, long-term performance of CO 2 sequestration sites may be dependent on both initial distribution and connectivity of pores in caprocks, and on changes induced by geochemical reaction after injection of CO 2, which are currentlymore » poorly understood. This paper presents results from an experimental study of changes to caprock porosity and pore network geometry in two caprock formations under conditions relevant to CO 2 sequestration. Pore connectivity and total porosity increased in the Gothic Shale; while total porosity increased but pore connectivity decreased in the Marine Tuscaloosa. Gothic Shale is a carbonate mudstone that contains volumetrically more carbonate minerals than Marine Tuscaloosa. Carbonate minerals dissolved to a greater extent than silicate minerals in Gothic Shale under high CO 2 conditions, leading to increased porosity at length scales <~200 nm that contributed to increased pore connectivity. In contrast, silicate minerals dissolved to a greater extent than carbonate minerals in Marine Tuscaloosa leading to increased porosity at all length scales, and specifically an increase in the number of pores >~1 μm. Mineral reactions also contributed to a decrease in pore connectivity, possibly as a result of precipitation in pore throats or hydration of the high percentage of clays. Finally, this study highlights the role that mineralogy of the caprock can play in geochemical response to CO 2 injection and resulting changes in sealing capacity in long-term CO 2 storage projects.« less

Making carbon sequestration a paying proposition

NASA Astrophysics Data System (ADS)

Han, Fengxiang X.; Lindner, Jeff S.; Wang, Chuji

2007-03-01

Atmospheric carbon dioxide (CO2) has increased from a preindustrial concentration of about 280 ppm to about 367 ppm at present. The increase has closely followed the increase in CO2 emissions from the use of fossil fuels. Global warming caused by increasing amounts of greenhouse gases in the atmosphere is the major environmental challenge for the 21st century. Reducing worldwide emissions of CO2 requires multiple mitigation pathways, including reductions in energy consumption, more efficient use of available energy, the application of renewable energy sources, and sequestration. Sequestration is a major tool for managing carbon emissions. In a majority of cases CO2 is viewed as waste to be disposed; however, with advanced technology, carbon sequestration can become a value-added proposition. There are a number of potential opportunities that render sequestration economically viable. In this study, we review these most economically promising opportunities and pathways of carbon sequestration, including reforestation, best agricultural production, housing and furniture, enhanced oil recovery, coalbed methane (CBM), and CO2 hydrates. Many of these terrestrial and geological sequestration opportunities are expected to provide a direct economic benefit over that obtained by merely reducing the atmospheric CO2 loading. Sequestration opportunities in 11 states of the Southeast and South Central United States are discussed. Among the most promising methods for the region include reforestation and CBM. The annual forest carbon sink in this region is estimated to be 76 Tg C/year, which would amount to an expenditure of 11.1-13.9 billion/year. Best management practices could enhance carbon sequestration by 53.9 Tg C/year, accounting for 9.3% of current total annual regional greenhouse gas emission in the next 20 years. Annual carbon storage in housing, furniture, and other wood products in 1998 was estimated to be 13.9 Tg C in the region. Other sequestration options, including the direct injection of CO2 in deep saline aquifers, mineralization, and biomineralization, are not expected to lead to direct economic gain. More detailed studies are needed for assessing the ultimate changes to the environment and the associated indirect cost savings for carbon sequestration.

Making carbon sequestration a paying proposition.

PubMed

Han, Fengxiang X; Lindner, Jeff S; Wang, Chuji

2007-03-01

Atmospheric carbon dioxide (CO(2)) has increased from a preindustrial concentration of about 280 ppm to about 367 ppm at present. The increase has closely followed the increase in CO(2) emissions from the use of fossil fuels. Global warming caused by increasing amounts of greenhouse gases in the atmosphere is the major environmental challenge for the 21st century. Reducing worldwide emissions of CO(2) requires multiple mitigation pathways, including reductions in energy consumption, more efficient use of available energy, the application of renewable energy sources, and sequestration. Sequestration is a major tool for managing carbon emissions. In a majority of cases CO(2) is viewed as waste to be disposed; however, with advanced technology, carbon sequestration can become a value-added proposition. There are a number of potential opportunities that render sequestration economically viable. In this study, we review these most economically promising opportunities and pathways of carbon sequestration, including reforestation, best agricultural production, housing and furniture, enhanced oil recovery, coalbed methane (CBM), and CO(2) hydrates. Many of these terrestrial and geological sequestration opportunities are expected to provide a direct economic benefit over that obtained by merely reducing the atmospheric CO(2) loading. Sequestration opportunities in 11 states of the Southeast and South Central United States are discussed. Among the most promising methods for the region include reforestation and CBM. The annual forest carbon sink in this region is estimated to be 76 Tg C/year, which would amount to an expenditure of $11.1-13.9 billion/year. Best management practices could enhance carbon sequestration by 53.9 Tg C/year, accounting for 9.3% of current total annual regional greenhouse gas emission in the next 20 years. Annual carbon storage in housing, furniture, and other wood products in 1998 was estimated to be 13.9 Tg C in the region. Other sequestration options, including the direct injection of CO(2) in deep saline aquifers, mineralization, and biomineralization, are not expected to lead to direct economic gain. More detailed studies are needed for assessing the ultimate changes to the environment and the associated indirect cost savings for carbon sequestration.

Externally controlled pressure and temperature microreactor for in situ x-ray diffraction, visual and spectroscopic reaction investigations under supercritical and subcritical conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Diefenbacher, Jason; McKelvy, Michael; Chizmeshya, Andrew V.G.

2005-01-01

A microreactor has been developed for in situ, spectroscopic investigations of materials and reaction processes with full external pressure and temperature control from ambient conditions to 400 deg. C and 310 bar. The sample chamber is in direct contact with an external manifold, whereby gases, liquids or fluids can be injected and their activities controlled prior to and under investigation conditions. The microreactor employs high strength, single crystal moissanite windows which allow direct probe beam interaction with a sample to investigate in situ reaction processes and other materials properties. The relatively large volume of the cell, along with full opticalmore » accessibility and external temperature and pressure control, make this reaction cell well suited for experimental investigations involving any combination of gas, fluid, and solid interactions. The microreactor's capabilities are demonstrated through an in situ x-ray diffraction study of the conversion of a meta-serpentine sample to magnesite under high pressure and temperature. Serpentine is one of the mineral candidates for the implementation of mineral carbonation, an intriguing carbon sequestration candidate technology.« less

Externally controlled pressure and temperature microreactor for in situ x-ray diffraction, visual and spectroscopic reaction investigations under supercritical and subcritial conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Diefenbacher, J.; McKelvy, M.; Chizemeshya, A.V.

2010-07-13

A microreactor has been developed for in situ, spectroscopic investigations of materials and reaction processes with full external pressure and temperature control from ambient conditions to 400 C and 310 bar. The sample chamber is in direct contact with an external manifold, whereby gases, liquids or fluids can be injected and their activities controlled prior to and under investigation conditions. The microreactor employs high strength, single crystal moissanite windows which allow direct probe beam interaction with a sample to investigate in situ reaction processes and other materials properties. The relatively large volume of the cell, along with full optical accessibilitymore » and external temperature and pressure control, make this reaction cell well suited for experimental investigations involving any combination of gas, fluid, and solid interactions. The microreactor's capabilities are demonstrated through an in situ x-ray diffraction study of the conversion of a meta-serpentine sample to magnesite under high pressure and temperature. Serpentine is one of the mineral candidates for the implementation of mineral carbonation, an intriguing carbon sequestration candidate technology.« less

Response comment: Carbon sequestration on Mars

USGS Publications Warehouse

Edwards, Christopher; Ehlmann, Bethany L.

2016-01-01

Martian atmospheric pressure has important implications for the past and present habitability of the planet, including the timing and causes of environmental change. The ancient Martian surface is strewn with evidence for early water bound in minerals (e.g., Ehlmann and Edwards, 2014) and recorded in surface features such as large catastrophically created outflow channels (e.g., Carr, 1979), valley networks (Hynek et al., 2010; Irwin et al., 2005), and crater lakes (e.g., Fassett and Head, 2008). Using orbital spectral data sets coupled with geologic maps and a set of numerical spectral analysis models, Edwards and Ehlmann (2015) constrained the amount of atmospheric sequestration in early Martian rocks and found that the majority of this sequestration occurred prior to the formation of the early Hesperian/late Noachian valley networks (Fassett and Head, 2011; Hynek et al., 2010), thus implying the atmosphere was already thin by the time these surface-water-related features were formed.

Multiphase, multicomponent simulations and experiments of reactive flow, relevant for combining geologic CO2 sequestration with geothermal energy capture

NASA Astrophysics Data System (ADS)

Saar, Martin O.

2011-11-01

Understanding the fluid dynamics of supercritical carbon dioxide (CO2) in brine- filled porous media is important for predictions of CO2 flow and brine displacement during geologic CO2 sequestration and during geothermal energy capture using sequestered CO2 as the subsurface heat extraction fluid. We investigate multiphase fluid flow in porous media employing particle image velocimetry experiments and lattice-Boltzmann fluid flow simulations at the pore scale. In particular, we are interested in the motion of a drop (representing a CO2 bubble) through an orifice in a plate, representing a simplified porous medium. In addition, we study single-phase/multicomponent reactive transport experimentally by injecting water with dissolved CO2 into rocks/sediments typically considered for CO2 sequestration to investigate how resultant fluid-mineral reactions modify permeability fields. Finally, we investigate numerically subsurface CO2 and heat transport at the geologic formation scale.

Carbon Dioxide Tucked into Basalt Converts to Rock

DOE Office of Scientific and Technical Information (OSTI.GOV)

McGrail, Pete

2016-11-18

Carbon Sequestration or storing carbon dioxide underground may be one approach to reducing atmospheric levels of the greenhouse gas. Storing it in basalt formations creates a chemical reaction in which the CO2 is transformed into a mineral similar to limestone enabling permanent storage underground. A field study by researchers at the Department of Energy’s Pacific Northwest National Laboratory shows that chemical happens quickly. Within two years, CO2 injected underground in Washington state had converted to the carbonate mineral ankerite.

Carbon Dioxide Tucked into Basalt Converts to Rock

ScienceCinema

McGrail, Pete

2018-06-13

Carbon Sequestration or storing carbon dioxide underground may be one approach to reducing atmospheric levels of the greenhouse gas. Storing it in basalt formations creates a chemical reaction in which the CO2 is transformed into a mineral similar to limestone enabling permanent storage underground. A field study by researchers at the Department of Energy’s Pacific Northwest National Laboratory shows that chemical happens quickly. Within two years, CO2 injected underground in Washington state had converted to the carbonate mineral ankerite.

Nitrogen-Related Constraints of Carbon Uptake by Large-Scale Forest Expansion: Simulation Study for Climate Change and Management Scenarios

NASA Astrophysics Data System (ADS)

Kracher, Daniela

2017-11-01

Increase of forest areas has the potential to increase the terrestrial carbon (C) sink. However, the efficiency for C sequestration depends on the availability of nutrients such as nitrogen (N), which is affected by climatic conditions and management practices. In this study, I analyze how N limitation affects C sequestration of afforestation and how it is influenced by individual climate variables, increased harvest, and fertilizer application. To this end, JSBACH, the land component of the Earth system model of the Max Planck Institute for Meteorology is applied in idealized simulation experiments. In those simulations, large-scale afforestation increases the terrestrial C sink in the 21st century by around 100 Pg C compared to a business as usual land-use scenario. N limitation reduces C sequestration roughly by the same amount. The relevance of compensating effects of uptake and release of carbon dioxide by plant productivity and soil decomposition, respectively, gets obvious from the simulations. N limitation of both fluxes compensates particularly in the tropics. Increased mineralization under global warming triggers forest expansion, which otherwise is restricted by N availability. Due to compensating higher plant productivity and soil respiration, the global net effect of warming for C sequestration is however rather small. Fertilizer application and increased harvest enhance C sequestration as well as boreal expansion. The additional C sequestration achieved by fertilizer application is offset to a large part by additional emissions of nitrous oxide.

An Integrated, Low Temperature Process to Capture and Sequester Carbon Dioxide from Industrial Emissions

NASA Astrophysics Data System (ADS)

Wendlandt, R. F.; Foremski, J. J.

2013-12-01

Laboratory experiments show that it is possible to integrate (1) the chemistry of serpentine dissolution, (2) capture of CO2 gas from the combustion of natural gas and coal-fired power plants using aqueous amine-based solvents, (3) long-term CO2 sequestration via solid phase carbonate precipitation, and (4) capture solvent regeneration with acid recycling in a single, continuous process. In our process, magnesium is released from serpentine at 300°C via heat treatment with ammonium sulfate salts or at temperatures as low as 50°C via reaction with sulfuric acid. We have also demonstrated that various solid carbonate phases can be precipitated directly from aqueous amine-based (NH3, MEA, DMEA) CO2 capture solvent solutions at room temperature. Direct precipitation from the capture solvent enables regenerating CO2 capture solvent without the need for heat and without the need to compress the CO2 off gas. We propose that known low-temperature electrochemical methods can be integrated with this process to regenerate the aqueous amine capture solvent and recycle acid for dissolution of magnesium-bearing mineral feedstocks and magnesium release. Although the direct precipitation of magnesite at ambient conditions remains elusive, experimental results demonstrate that at temperatures ranging from 20°C to 60°C, either nesquehonite Mg(HCO3)(OH)●2H2O or a double salt with the formula [NH4]2Mg(CO3)2●4H2O or an amorphous magnesium carbonate precipitate directly from the capture solvent. These phases are less desirable for CO2 sequestration than magnesite because they potentially remove constituents (water, ammonia) from the reaction system, reducing the overall efficiency of the sequestration process. Accordingly, the integrated process can be accomplished with minimal energy consumption and loss of CO2 capture and acid solvents, and a net generation of 1 to 4 moles of H2O/6 moles of CO2 sequestered (depending on the solid carbonate precipitate and amount of produced H2 and O2 gas reacted to produce heat and water). Features of the integrated process include the following: 1) the four separate processes have compatible chemistry, enabling design of an integrated, continuous process scheme for CO2 capture and sequestration; 2) all 4 stages of the process can be conducted at ambient or slightly elevated temperatures; 3) precipitating carbonate directly from the capture solvent eliminates the need for costly CO2 gas compression; and 4) recycling the acid used for serpentine dissolution and the solvent used for CO2 capture reduces feed stock costs.

Chromium-removal processes during groundwater remediation by a zerovalent iron permeable reactive barrier.

PubMed

Wilkin, Richard T; Su, Chunming; Ford, Robert G; Paul, Cynthia J

2005-06-15

Solid-phase associations of chromium were examined in core materials collected from a full-scale, zerovalent iron permeable reactive barrier (PRB) at the U.S. Coast Guard Support Center located near Elizabeth City, NC. The PRB was installed in 1996 to treat groundwater contaminated with hexavalent chromium. After eight years of operation, the PRB remains effective at reducing concentrations of Cr from average values >1500 microg L(-1) in groundwater hydraulically upgradient of the PRB to values <1 microg L(-1) in groundwater within and hydraulically downgradient of the PRB. Chromium removal from groundwater occurs at the leading edge of the PRB and also within the aquifer immediately upgradient of the PRB. These regions also witness the greatest amount of secondary mineral formation due to steep geochemical gradients that result from the corrosion of zerovalent iron. X-ray absorption near-edge structure (XANES) spectroscopy indicated that chromium is predominantly in the trivalent oxidation state, confirming that reductive processes are responsible for Cr sequestration. XANES spectra and microscopy results suggest that Cr is, in part, associated with iron sulfide grains formed as a consequence of microbially mediated sulfate reduction in and around the PRB. Results of this study provide evidence that secondary iron-bearing mineral products may enhance the capacity of zerovalent iron systems to remediate Cr in groundwater, either through redox reactions at the mineral-water interface or by the release of Fe(II) to solution via mineral dissolution and/or metal corrosion.

An integrated monitoring network for hydrologic, geochemical, and sediment fluxes to characterize carbon-mineral fate in the Christina River Basin Critical Zone Observatory

NASA Astrophysics Data System (ADS)

Sawyer, A. H.; Karwan, D. L.; Lazareva, O.

2011-12-01

Organic carbon (C) -mineral complexation mechanism plays an important role in C sequestration within watersheds. The primary goal of the Christina River Basin Critical Zone Observatory in SE Pennsylvania and N Delaware, USA (one of six National Science Foundation-funded observatories) is to quantify net carbon sink or source due to mineral production and transport and its dependence on land use. This effort requires an interdisciplinary understanding of carbon and mineral fluxes across interfaces between soil, aquifer, floodplain, and river. We have established a monitoring network that targets hydrologic, geochemical, and sedimentological transport processes across channel-floodplain-aquifer interfaces within White Clay Creek Watershed. Within the channel, suspended material is sampled and analyzed for organic and mineral composition as well as geochemical fingerprints. Surface water and groundwater are analyzed for C, Fe, and Mn chemistry. Within the floodplain, in-situ sensors monitor soil moisture, pressure, temperature, conductivity, and redox potential. Integrated data analysis should yield estimates of water and solute fluxes between the vadose zone, riparian aquifer, and stream. Our preliminary data show that storm events are important for carbon and mineral fluxes-suspended material in surface water changes in source and composition throughout the storm. Meanwhile, the variation in stream stage drives surface water-groundwater exchange, facilitating changes in redox potential and providing opportunity for enhanced transport and reactions involving C, Fe, and Mn in the riparian aquifer.

Sequestering CO(2) by mineral carbonation: stability against acid rain exposure.

PubMed

Allen, Daniel J; Brent, Geoff F

2010-04-01

Mineral carbonation is a potentially attractive alternative to storage of compressed CO(2) in underground repositories, known as geosequestration. Processes for the conversion of basic ores, such as magnesium silicates, to carbonates have been proposed by various researchers, with storage of the carbonate as backfill in the original mine representing a solid carbon sink. The stability of such carbon sinks against acid rain and other sources of strong acids is examined here. It is acknowledged that in the presence of strong acid, carbonates will dissolve and release carbon dioxide. A sensitivity analysis covering annual average rainfall and pH that may be encountered in industrialized areas of the United States, China, Europe, and Australia was conducted to determine maximum CO(2) rerelease rates from mineral carbonation carbon sinks. This analysis is based on a worst-case premise that is equivalent to assuming infinitely rapid kinetics of dissolution of the carbonate. The analysis shows that under any likely conditions of pH and rainfall, leakage rates of stored CO(2) are negligible. This is illustrated in a hypothetical case study under Australian conditions. It is thus proposed that sequestration by mineral carbonation can be considered to be permanent on practical human time scales. Other possible sources of acid have also been considered.

Up-Scaling Geochemical Reaction Rates for Carbon Dioxide (CO2) in Deep Saline Aquifers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Peters, Catherine A

2013-02-28

Geochemical reactions in deep subsurface environments are complicated by the consolidated nature and mineralogical complexity of sedimentary rocks. Understanding the kinetics of these reactions is critical to our ability to make long-term predictions about subsurface processes such as pH buffering, alteration in rock structure, permeability changes, and formation of secondary precipitates. In this project, we used a combination of experiments and numerical simulation to bridge the gap between our knowledge of these reactions at the lab scale and rates that are meaningful for modeling reactive transport at core scales. The focus is on acid-driven mineral dissolution, which is specifically relevantmore » in the context of CO2-water-rock interactions in geological sequestration of carbon dioxide. The project led to major findings in three areas. First, we modeled reactive transport in pore-network systems to investigate scaling effects in geochemical reaction rates. We found significant scaling effects when CO2 concentrations are high and reaction rates are fast. These findings indicate that the increased acidity associated with geological sequestration can generate conditions for which proper scaling tools are yet to be developed. Second, we used mathematical modeling to investigate the extent to which SO2, if co-injected with CO2, would acidify formation brines. We found that there exist realistic conditions in which the impact on brine acidity will be limited due to diffusion rate-limited SO2 dissolution from the CO2 phase, and the subsequent pH shift may also be limited by the lack of availability of oxidants to produce sulfuric acid. Third, for three Viking sandstones (Alberta sedimentary basin, Canada), we employed backscattered electron microscopy and energy dispersive X-ray spectroscopy to statistically characterize mineral contact with pore space. We determined that for reactive minerals in sedimentary consolidated rocks, abundance alone is not a good predictor of mineral accessible surface area, and should not be used in reactive transport modeling. Our work showed that reaction rates would be overestimated by three to five times.« less

Earthworms facilitate carbon sequestration through unequal amplification of carbon stabilization compared with mineralization

EPA Science Inventory

A recent review concluded that earthworm presence increases CO2 emissions by 33% but does not affect soil organic carbon stocks. However, the findings are controversial and raise new questions. Here we hypothesize that neither an increase in CO2 emission nor in stabilized carbon...

Chemical-Looping Combustion and Gasification of Coals and Oxygen Carrier Development: A Brief Review

DOE PAGES

Wang, Ping; Means, Nicholas; Shekhawat, Dushyant; ...

2015-09-24

Chemical-looping technology is one of the promising CO 2 capture technologies. It generates a CO 2 enriched flue gas, which will greatly benefit CO 2 capture, utilization or sequestration. Both chemical-looping combustion (CLC) and chemical-looping gasification (CLG) have the potential to be used to generate power, chemicals, and liquid fuels. Chemical-looping is an oxygen transporting process using oxygen carriers. Recently, attention has focused on solid fuels such as coal. Coal chemical-looping reactions are more complicated than gaseous fuels due to coal properties (like mineral matter) and the complex reaction pathways involving solid fuels. The mineral matter/ash and sulfur in coalmore » may affect the activity of oxygen carriers. Oxygen carriers are the key issue in chemical-looping processes. Thermogravimetric analysis (TGA) has been widely used for the development of oxygen carriers (e.g., oxide reactivity). Two proposed processes for the CLC of solid fuels are in-situ Gasification Chemical-Looping Combustion (iG-CLC) and Chemical-Looping with Oxygen Uncoupling (CLOU). The objectives of this review are to discuss various chemical-looping processes with coal, summarize TGA applications in oxygen carrier development, and outline the major challenges associated with coal chemical-looping in iG-CLC and CLOU.« less

Humus and energy balances and greenhouse gas emissions with compost fertilization in organic farming compared with mineral fertilization

NASA Astrophysics Data System (ADS)

Erhart, Eva; Schmid, Harald; Hülsbergen, Kurt-Jürgen; Hartl, Wilfried

2015-04-01

Humus and energy balances and greenhouse gas emissions with compost fertilization in organic farming compared with mineral fertilization E. Erhart, H. Schmid, K.-J. Hülsbergen, W. Hartl The positive effects of compost fertilization on soil humus with their associated benefits for soil quality are well-established. The aim of the present study was to assess the effect of compost fertilization on humus and energy balances and greenhouse gas emissions and to compare the results of the humus balances with the changes in soil organic carbon contents measured in the soil of the experimental field. In order to assess the effects of compost use in organic farming as compared to conventional farming practice using mineral fertilizers, the field experiment with compost fertilization 'STIKO' was set up in 1992 near Vienna, Austria, on a Molli-gleyic Fluvisol. It included three treatments with compost fertilization (C1, C2 and C3 with 8, 14 and 20 t ha-1 y-1 f. m. on average of 14 years), three treatments with mineral nitrogen fertilization (N1, N2 and N3 with 29, 46 and 63 kg N ha-1 y 1 on average) and an unfertilized control (0) in six replications in a latin rectangle design. In the field trial, biowaste compost from the composting plant of the City of Vienna was used. Data from the field experiment (from 14 experimental years) were fed into the model software REPRO to calculate humus and energy balances and greenhouse gas emissions. The model software REPRO (REPROduction of soil fertility) couples the balancing of C, N and energy fluxes. For the determination of the net greenhouse effect, REPRO performs calculations of C sequestration in the soil, CO2 emissions from the use of fossil energy and N2O emissions from the soil. Humus balances showed that compost fertilization at a rate of 8 t ha-1 y-1 (C1) resulted in a positive humus balance of +115 kg C ha-1 y-1. With 14 and 20 t ha-1 y-1 compost (C2 and C3), respectively, humus accumulated at rates of 558 and 1021 kg C ha-1 y-1. With mineral fertilization at rates of 29 - 63 kg N ha-1 y-1 (N1 - N3), balances were moderately negative ( 169 to -227 kg C ha-1 y-1), while a clear humus deficit of 457 kg C ha-1 y-1 showed in the unfertilized control. Compared with measured soil organic carbon data REPRO predicted soil organic carbon contents fairly well with the exception of the treatments with high compost rates. Here REPRO clearly overestimated soil organic carbon contents for this site. Energy efficiency, as described by the output/input ratio, was highest in the control, followed by C1. Mineral fertilization treatment N3 was most energy intensive. The greenhouse gas balance indicated net carbon sequestration already with medium compost rates (C2), and net carbon sequestration of 1700 kg CO2-eq ha-1 y-1 in C3. Mineral fertilization yielded net greenhouse gas emissions of around 2000 kg CO2-eq ha-1 y 1. The highest greenhouse gas emissions had the unfertilized control due to the degradation of soil organic matter and lowest organic matter input. These findings underline that compost fertilization holds a high potential for carbon sequestration and for the reduction of greenhouse gas emissions.

A mechanistic study of the interaction of water-soluble borate glass with apatite-bound heterocyclic nitrogen-containing bisphosphonates.

PubMed

Pramanik, Chandrani; Sood, Parveen; Niu, Li-Na; Yuan, He; Ghoshal, Sushanta; Henderson, Walter; Liu, Yaodong; Jang, Seung Soon; Kumar, Satish; Pashley, David H; Tay, Franklin R

2016-02-01

Long-term oral and intravenous use of nitrogen-containing bisphosphonates (N-BPs) is associated with osteonecrosis of the jaw. Although N-BPs bind strongly to bone surfaces via non-covalent bonds, it is possible for extrinsic ions to dissociate bound N-BPs from mineralized bone by competitive desorption. Here, we investigate the effects and mechanism of using an ionic cocktail derived from borate bioactive glass for sequestration of heterocyclic N-BPs bound to apatite. By employing solid-state and solution-state analytical techniques, we confirmed that sequestration of N-BPs from bisphosphonate-bound apatite occurs in the presence of the borate-containing ionic cocktail. Simulations by density functional theory computations indicate that magnesium cation and borate anion are well within the extent of the risedronate or zoledronate anion to form precipitate complexes. The sequestration mechanism is due to the borate anion competing with bisphosphonates for similar electron-deficient sites on the apatite surface for binding. Thus, application of the borate-containing ionic cocktail represents a new topical lavage approach for removing apatite-bound heterocyclic N-BPs from exposed necrotic bone in bisphosphonate-related osteonecrosis of the jaw. Long-term oral consumption and injections of nitrogen-containing bisphosphonates (N-BPs) may result in death of the jaw bone when there is traumatic injury to the bone tissues. To date, there is no effective treatment for such a condition. This work reported the use of an ionic cocktail derived from water-soluble borate glass microfibers to displace the most potent type of N-BPs that are bound strongly to the mineral component on bone surfaces. The mechanism responsible for such an effect has been identified to be cation-mediated complexation of borate anions with negatively-charged N-BPs, allowing them to be released from the mineral surface. This borate-containing cocktail may be developed into a novel topical rinse for removing mineral-bound N-BPs from exposed dead bone. Copyright © 2015 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Compositional Determination of Shale with Simultaneous Neutron and X-ray Tomography

NASA Astrophysics Data System (ADS)

LaManna, J.; Hussey, D. S.; Baltic, E.; Jacobson, D. L.

2017-12-01

Understanding the distribution of organic material, mineral inclusions, and porosity are critical to properly model the flow of fluids through rock formations in applications ranging from hydraulic fracturing and gas extraction, CO2 sequestration, geothermal power, and aquifer management. Typically, this information is obtained on the pore scale using destructive techniques such as focused ion beam scanning electron microscopy. Neutrons and X-rays provide non-destructive, complementary probes to gain three-dimensional distributions of porosity, minerals, and organic content along with fluid interactions in fractures and pore networks on the core scale. By capturing both neutron and X-ray tomography simultaneously it is possible to capture slowly dynamic or stochastic processes with both imaging modes. To facilitate this, NIST offers a system for simultaneous neutron and X-ray tomography at the Center for Neutron Research. This instrument provides neutron and X-ray beams capable of penetrating through pressure vessels to image the specimen inside at relevant geological conditions at resolutions ranging from 15 micrometers to 100 micrometers. This talk will discuss current efforts at identifying mineral and organic content and fracture and wettability in shales relevant to gas extraction.

Experimental investigation of CO2-brine-rock interactions at simulated in-situ conditions

NASA Astrophysics Data System (ADS)

Słomski, Piotr; Lutyński, Marcin; Mastalerz, Maria; Szczepański, Jacek; Derkowski, Arkadiusz; Topór, Tomasz

2017-04-01

Geological sequestration of carbon dioxide (CO2) in deep formations (e.g. saline aquifers, oil and gas reservoirs and coalbeds) is one of the most promising options for reducing concentration of this anthropogenic greenhouse gas in the atmosphere. CO2 injected into the rock formations can be trapped by several mechanisms including structural and stratigraphic trapping, capillary CO2 trapping, dissolution trapping and mineral trapping. During dissolution trapping, CO2 dissolves in the formation brine and sinks in the reservoir as the CO2-enriched brine has an increased density. In comparison, in mineral trapping, CO2 is bound by precipitating new carbonate minerals. The latter two mechanisms depend on the temperature, pressure, and the mineralogy of the reservoir rock and the chemical composition of the brine. This study discusses laboratory scale alterations of Ordovician and Silurian shale rocks from potential CO2 sequestration site B1 in the Baltic Basin. In the reported experiment, rocks submerged in brine in specially constructed reactors were subjected to CO2 pressure of 30-35 MPa for 30-45 days at temperature of 80 oC. Shale samples were analyzed in terms of mineral composition and mesopore surface area and volume, before and after experiments, by means of X-ray diffraction and N2 low-pressure adsorption, respectively, for possible CO2 induced changes. Comparison of mineral composition before and after experiments demonstrated subtle mineral changes. The most conspicuous was a release of Fe in the form of Fe-oxyhydroxides, most probably related to the decomposition of Fe-bearing minerals like pyrite, chlorite and, less frequently, ankerite. With regard to porosity, interestingly, the most significant increase in mesopore surface area and mesopore volume was observed in samples with the largest drop of chlorite amount. The less significant mineral changes were associated with formation of kaolinite related to breakdown of feldspars and dissolution of carbonate minerals represented by calcite, dolomite, and ankerite. In the analyzed samples, no new carbonate minerals were formed during the experiments. An increase of carbonates was recorded only in three out of 13 samples. However, concentration of carbonates in these three samples is too low to conclude CO2 mineral trapping in new carbonate phases. Acknowledgments: the study was supported from grant SHALESEQ (No PL12-0109) funded by the National Centre for Research and Development.

75 FR 32171 - American Electric Power Service Corporation's Mountaineer Commercial Scale Carbon Capture and...

Federal Register 2010, 2011, 2012, 2013, 2014

2010-06-07

...) appropriated $3.4 billion to DOE for Fossil Energy Research and Development; the Department intends to use a... concentrated, high-pressure form suitable for sequestration. The concentrated CO 2 stream would be cooled and... underground resources such as ground water supplies, mineral resources, and fossil fuel resources; Fate and...

Integration of experiments across diverse environments identifies the genetic determinants of variation in Sorghum bicolor seed element composition

USDA-ARS?s Scientific Manuscript database

Increasing the bioavailable elemental nutrient content in the edible portions of the crop has the potential to increase the value of sorghum for human and animal nutrition. Seedling establishment and seed nutritional quality are in part determined by the sequestration of sufficient mineral nutrients...

Greenhouse gas fluxes of drained organic and flooded mineral agricultural soils in the United States

USDA-ARS?s Scientific Manuscript database

Drained organic soils for agriculture represent less than 1% of the area used for crops in the United States (US). However, emission of carbon dioxide (CO2) from microbial oxidation of drained organic soils offsets almost half of the contributions that carbon sequestration of other cropping systems ...

Effects of Added Organic Matter and Water on Soil Carbon Sequestration in an Arid Region

PubMed Central

Tian, Yuan; Jiang, Lianhe; Zhao, Xuechun; Zhu, Linhai; Chen, Xi; Gao, Yong; Wang, Shaoming; Zheng, Yuanrun; Rimmington, Glyn M.

2013-01-01

It is generally predicted that global warming will stimulate primary production and lead to more carbon (C) inputs to soil. However, many studies have found that soil C does not necessarily increase with increased plant litter input. Precipitation has increased in arid central Asia, and is predicted to increase more, so we tested the effects of adding fresh organic matter (FOM) and water on soil C sequestration in an arid region in northwest China. The results suggested that added FOM quickly decomposed and had minor effects on the soil organic carbon (SOC) pool to a depth of 30 cm. Both FOM and water addition had significant effects on the soil microbial biomass. The soil microbial biomass increased with added FOM, reached a maximum, and then declined as the FOM decomposed. The FOM had a more significant stimulating effect on microbial biomass with water addition. Under the soil moisture ranges used in this experiment (21.0%–29.7%), FOM input was more important than water addition in the soil C mineralization process. We concluded that short-term FOM input into the belowground soil and water addition do not affect the SOC pool in shrubland in an arid region. PMID:23875022

A Comparison of Corn (Zea mays L.) Residue and Its Biochar on Soil C and Plant Growth

PubMed Central

Calderón, Francisco J.; Benjamin, Joseph; Vigil, Merle F.

2015-01-01

In order to properly determine the value of charring crop residues, the C use efficiency and effects on crop performance of biochar needs to be compared to the un-charred crop residues. In this study we compared the addition of corn stalks to soil, with equivalent additions of charred (300 °C and 500 °C) corn residues. Two experiments were conducted: a long term laboratory mineralization, and a growth chamber trial with proso millet plants. In the laboratory, we measured soil mineral N dynamics, C use efficiency, and soil organic matter (SOM) chemical changes via infrared spectroscopy. The 300 °C biochar decreased plant biomass relative to a nothing added control. The 500°C biochar had little to no effect on plant biomass. With incubation we measured lower soil NO3 content in the corn stalk treatment than in the biochar-amended soils, suggesting that the millet growth reduction in the stalk treatment was mainly driven by N limitation, whereas other factors contributed to the biomass yield reductions in the biochar treatments. Corn stalks had a C sequestration use efficiency of up to 0.26, but charring enhanced C sequestration to values that ranged from 0.64 to 1.0. Infrared spectroscopy of the soils as they mineralized showed that absorbance at 3400, 2925-2850, 1737 cm-1, and 1656 cm-1 decreased during the incubation and can be regarded as labile SOM, corn residue, or biochar bands. Absorbances near 1600, 1500-1420, and 1345 cm-1 represented the more refractory SOM moieties. Our results show that adding crop residue biochar to soil is a sound C sequestration technology compared to letting the crop residues decompose in the field. This is because the resistance to decomposition of the chars after soil amendment offsets any C losses during charring of the crop residues. PMID:25836653

A comparison of corn (Zea mays L.) residue and its biochar on soil C and plant growth.

PubMed

Calderón, Francisco J; Benjamin, Joseph; Vigil, Merle F

2015-01-01

In order to properly determine the value of charring crop residues, the C use efficiency and effects on crop performance of biochar needs to be compared to the un-charred crop residues. In this study we compared the addition of corn stalks to soil, with equivalent additions of charred (300 °C and 500 °C) corn residues. Two experiments were conducted: a long term laboratory mineralization, and a growth chamber trial with proso millet plants. In the laboratory, we measured soil mineral N dynamics, C use efficiency, and soil organic matter (SOM) chemical changes via infrared spectroscopy. The 300 °C biochar decreased plant biomass relative to a nothing added control. The 500°C biochar had little to no effect on plant biomass. With incubation we measured lower soil NO3 content in the corn stalk treatment than in the biochar-amended soils, suggesting that the millet growth reduction in the stalk treatment was mainly driven by N limitation, whereas other factors contributed to the biomass yield reductions in the biochar treatments. Corn stalks had a C sequestration use efficiency of up to 0.26, but charring enhanced C sequestration to values that ranged from 0.64 to 1.0. Infrared spectroscopy of the soils as they mineralized showed that absorbance at 3400, 2925-2850, 1737 cm-1, and 1656 cm-1 decreased during the incubation and can be regarded as labile SOM, corn residue, or biochar bands. Absorbances near 1600, 1500-1420, and 1345 cm-1 represented the more refractory SOM moieties. Our results show that adding crop residue biochar to soil is a sound C sequestration technology compared to letting the crop residues decompose in the field. This is because the resistance to decomposition of the chars after soil amendment offsets any C losses during charring of the crop residues.

Contaminant Organic Complexes: Their Structure and Energetics in Surface Decontamination Processes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Satish C. B. Myneni

2005-12-13

Siderophores are biological macromolecules (400-2000 Da) released by bacteria in iron limiting situations to sequester Fe from iron oxyhydroxides and silicates in the natural environment. These molecules contain hydroxamate and phenolate functional groups, and exhibit very high affinity for Fe{sup 3+}. While several studies were conducted to understand the behavior of siderophores and their application to the metal sequestration and mineral dissolution, only a few of them have examined the molecular structure of siderophores and their interactions with metals and mineral surfaces in aqueous solutions. Improved understanding of the chemical state of different functional moieties in siderophores can assist inmore » the application of these biological molecules in actinide separation, sequestration and decontamination processes. The focus of our research group is to evaluate the (a) functional group chemistry of selected siderophores and their metal complexes in aqueous solutions, and (b) the nature of siderophore interactions at the mineral-water interfaces. We selected desferrioxamine B (desB), a hydroxamate siderophore, and its small structural analogue, acetohydroxamic acid (aHa), for this investigation. We examined the functional group chemistry of these molecules as a function of pH, and their complexation with aqueous and solid phase Fe(III). For solid phase Fe, we synthesized all naturally occurring Fe(III)-oxyhydroxides (goethite, lepidocrocite, akaganeite, feroxyhite) and hematite. We also synthesized Fe-oxides (goethite and hematite) of different sizes to evaluate the influence of particle size on mineral dissolution kinetics. We used a series of molecular techniques to explore the functional group chemistry of these molecules and their complexes. Infrared spectroscopy is used to specifically identify the variations in oxime group as a function of pH and Fe(III) complexation. Resonance Raman spectroscopy was used to evaluate the nature of hydroxamate binding in the case of Fe(III)-siderophore complexes and model ligands. Soft and hard X-ray spectroscopy techniques were used to examine the electronic structure of binding groups, and their local structural environment. The synchrotron X-ray studies were conducted at the Stanford Synchrotron Radiation Laboratory and at the Advanced Light Source (Lawrence Berkeley National Laboratory). These experimental vibrational and X-ray spectroscopy studies were complemented with density functional theory calculations. The highlight of this study is the evaluation of the fundamental electronic state information of the hydroxamate moiety in siderophores during deprotonation and Fe(III) complexation. The applications of soft X-ray studies are also new, and were applied, for the first time, to examine the chemistry of organic macromolecules in aqueous solutions.« less

Whole Watershed Quantification of Net Carbon Fluxes by Erosion and Deposition within the Christina River Basin Critical Zone Observatory

NASA Astrophysics Data System (ADS)

Aufdenkampe, A. K.; Karwan, D. L.; Aalto, R. E.; Marquard, J.; Yoo, K.; Wenell, B.; Chen, C.

2013-12-01

We have proposed that the rate at which fresh, carbon-free minerals are delivered to and mix with fresh organic matter determines the rate of carbon preservation at a watershed scale (Aufdenkampe et al. 2011). Although many studies have examined the role of erosion in carbon balances, none consider that fresh carbon and fresh minerals interact. We believe that this mechanism may be a dominant sequestration process in watersheds with strong anthropogenic impacts. Our hypothesis - that the rate of mixing fresh carbon with fresh, carbon-free minerals is a primary control on watershed-scale carbon sequestration - is central to our Christina River Basin Critical Zone Observatory project (CRB-CZO, http://www.udel.edu/czo/). The Christina River Basin spans 1440 km2 from piedmont to Atlantic coastal plain physiographic provinces in the states of Pennsylvania and Delaware, and experienced intensive deforestation and land use beginning in the colonial period of the USA. Here we present a synthesis of multi-disciplinary data from the CRB-CZO on materials as they are transported from sapprolite to topsoils to colluvium to suspended solids to floodplains, wetlands and eventually to the Delaware Bay estuary. At the heart of our analysis is a spatially-integrated, flux-weighted comparison of the organic carbon to mineral surface area ratio (OC/SA) of erosion source materials versus transported and deposited materials. Because source end-members - such as forest topsoils, farmed topsoils, gullied subsoils and stream banks - represent a wide distribution of initial, pre-erosion OC/SA, we quantify source contributions using geochemical sediment fingerprinting approaches (Walling 2005). Analytes used for sediment fingerprinting include: total mineral elemental composition (including rare earth elements), fallout radioisotope activity for common erosion tracers (beryllium-7, beryllium-10, lead-210, cesium-137), particle size distribution and mineral specific surface area, in addition to organic carbon and nitrogen content with stable isotope (13C, 15N) and radiocarbon (14C) abundance to quantify OC/SA and organic carbon sources and mean age. We then use multivariate mixing model analysis to quantify the fractional contribution of each source end-member to each sample of suspended or deposited sediments. Last, we calculate a predicted OC/SA based on source end-member mixing and compare to the measured OC/SA to quantify net change in mineral complexed carbon. Aufdenkampe, A.K. et al. Riverine coupling of biogeochemical cycles between land, oceans, and atmosphere. Frontiers Ecol. Environ. 9, 53-60 (2011). Walling, D. E. Tracing suspended sediment sources in catchments and river systems. Sci. Total Environ. 34, 159-184 (2005).

Testing CO2 Sequestration in an Alkaline Soil Treated with Flue Gas Desulfurization Gypsum (FGDG)

NASA Astrophysics Data System (ADS)

Han, Y.; Tokunaga, T. K.

2012-12-01

Identifying effective and economical methods for increasing carbon storage in soils is of interest for reducing soil CO2 fluxes to the atmosphere in order to partially offset anthropogenic CO2 contributions to climate change This study investigates an alternative strategy for increasing carbon retention in soils by accelerating calcite (CaCO3) precipitation and promoting soil organic carbon (SOC) complexation on mineral surfaces. The addition of calcium ion to soils with pH > 8, often found in arid and semi-arid regions, may accelerate the slow process of calcite precipitation. Increased ionic strength from addition of a soluble Ca source also suppresses microbial activity which oxidizes SOC to gaseous CO2. Through obtaining C mass balances in soil profiles, this study is quantifying the efficiency of gypsum amendments for mitigating C losses to the atmosphere. The objective of this study is to identify conditions in which inorganic and organic C sequestration is practical in semi-arid and arid soils by gypsum treatment. As an inexpensive calcium source, we proposed to use flue gas desulfurization gypsum (FGDG), a byproduct of fossil fuel burning electric power plants. To test the hypothesis, laboratory column experiments have been conducted in calcite-buffered soil with addition of gypsum and FGDG. The results of several months of column monitoring are demonstrating that gypsum-treated soil have lowered amounts of soil organic carbon loss and increased inorganic carbon (calcite) production. The excess generation of FGDG relative to industrial and agricultural needs, FGDG, is currently regarded as waste. Thus application of FGDG application in some soils may be an effective and economical means for fixing CO2 in soil organic and inorganic carbon forms.Soil carbon cycle, with proposed increased C retention by calcite precipitation and by SOC binding onto soil mineral surfaces, with both processes driven by calcium released from gypsum dissolution.

Abiotic CO2 reduction during geologic carbon sequestration facilitated by Fe(II)-bearing minerals

NASA Astrophysics Data System (ADS)

Nielsen, L. C.; Maher, K.; Bird, D. K.; Brown, G. E.; Thomas, B.; Johnson, N. C.; Rosenbauer, R. J.

2012-12-01

Redox reactions involving subsurface minerals and fluids and can lead to the abiotic generation of hydrocarbons from CO2 under certain conditions. Depleted oil reservoirs and saline aquifers targeted for geologic carbon sequestration (GCS) can contain significant quantities of minerals such as ferrous chlorite, which could facilitate the abiotic reduction of carbon dioxide to n-carboxylic acids, hydrocarbons, and amorphous carbon (C0). If such reactions occur, the injection of supercritical CO2 (scCO2) could significantly alter the oxidation state of the reservoir and cause extensive reorganization of the stable mineral assemblage via dissolution and reprecipitation reactions. Naturally occurring iron oxide minerals such as magnetite are known to catalyze CO2 reduction, resulting in the synthesis of organic compounds. Magnetite is thermodynamically stable in Fe(II) chlorite-bearing mineral assemblages typical of some reservoir formations. Thermodynamic calculations demonstrate that GCS reservoirs buffered by the chlorite-kaolinite-carbonate(siderite/magnesite)-quartz assemblage favor the reduction of CO2 to n-carboxylic acids, hydrocarbons, and C0, although the extent of abiotic CO2 reduction may be kinetically limited. To investigate the rates of abiotic CO2 reduction in the presence of magnetite, we performed batch abiotic CO2 reduction experiments using a Dickson-type rocking hydrothermal apparatus at temperatures (373 K) and pressures (100 bar) within the range of conditions relevant to GCS. Blank experiments containing CO2 and H2 were used to rule out the possibility of catalytic activity of the experimental apparatus. Reaction of brine-suspended magnetite nanoparticles with scCO2 at H2 partial pressures typical of reservoir rocks - up to 100 and 0.1 bars respectively - was used to investigate the kinetics of magnetite-catalyzed abiotic CO2 reduction. Later experiments introducing ferrous chlorite (ripidolite) were carried out to determine the potential for heterogeneous catalysis in GCS systems.

Experimental Study of Porosity Changes in Shale Caprocks Exposed to CO 2-Saturated Brines I: Evolution of Mineralogy, Pore Connectivity, Pore Size Distribution, and Surface Area

DOE PAGES

Mouzakis, Katherine M.; Navarre-Sitchler, Alexis K.; Rother, Gernot; ...

2016-07-18

Carbon capture, utilization, and storage, one proposed method of reducing anthropogenic emissions of CO 2, relies on low permeability formations, such as shales, above injection formations to prevent upward migration of the injected CO 2. Porosity in caprocks evaluated for sealing capacity before injection can be altered by geochemical reactions induced by dissolution of injected CO 2 into pore fluids, impacting long-term sealing capacity. Therefore, long-term performance of CO 2 sequestration sites may be dependent on both initial distribution and connectivity of pores in caprocks, and on changes induced by geochemical reaction after injection of CO 2, which are currentlymore » poorly understood. This paper presents results from an experimental study of changes to caprock porosity and pore network geometry in two caprock formations under conditions relevant to CO 2 sequestration. Pore connectivity and total porosity increased in the Gothic Shale; while total porosity increased but pore connectivity decreased in the Marine Tuscaloosa. Gothic Shale is a carbonate mudstone that contains volumetrically more carbonate minerals than Marine Tuscaloosa. Carbonate minerals dissolved to a greater extent than silicate minerals in Gothic Shale under high CO 2 conditions, leading to increased porosity at length scales <~200 nm that contributed to increased pore connectivity. In contrast, silicate minerals dissolved to a greater extent than carbonate minerals in Marine Tuscaloosa leading to increased porosity at all length scales, and specifically an increase in the number of pores >~1 μm. Mineral reactions also contributed to a decrease in pore connectivity, possibly as a result of precipitation in pore throats or hydration of the high percentage of clays. Finally, this study highlights the role that mineralogy of the caprock can play in geochemical response to CO 2 injection and resulting changes in sealing capacity in long-term CO 2 storage projects.« less

Microbial exudate promoted dissolution and transformation of chromium containing minerals

NASA Astrophysics Data System (ADS)

Saad, E. M.; Sun, J.; Tang, Y.

2015-12-01

Because of its utility in many industrial processes, chromium has become the second most common metal contaminant in the United States. The two most common oxidation states of chromium in nature are Cr(III), which is highly immobile, and Cr(VI), which is highly mobile and toxic. In both natural and engineered environments, the most common remediation of Cr(VI) is through reduction, which results in chromium sequestration in the low solubility mixed Cr(III)-Fe(III) (oxy)hydroxide phases. Consequently, the stability of these minerals must be examined to assess the fate of chromium in the subsurface. We examined the dissolution of mixed Cr(III)-Fe(III) (oxy)hydroxides in the presence of common microbial exudates, including the siderophore desferrioxamine B (DFOB; a common organic ligand secreted by most microbes with high affinity for ferric iron and other trivalent metal ions) and oxalate (a common organic acid produced by microbes). The solids exhibited incongruent dissolution with preferential leaching of Fe from the solid phase. Over time, this leads to a more Cr rich mineral, which is known to be more soluble than the corresponding mixed mineral phase. We are currently investigating the structure of the reacted mineral phases and soluble Cr(III) species, as well as the potential oxidation and remobilization of the soluble Cr species. Results from this study will provide insights regarding the long term transport and fate of chromium in the natural environment in the presence of microbial activities.

Constraining the effects of permeability uncertainty for geologic CO2 sequestration in a basalt reservoir

NASA Astrophysics Data System (ADS)

Jayne, R., Jr.; Pollyea, R.

2016-12-01

Carbon capture and sequestration (CCS) in geologic reservoirs is one strategy for reducing anthropogenic CO2 emissions from large-scale point-source emitters. Recent developments at the CarbFix CCS pilot in Iceland have shown that basalt reservoirs are highly effective for permanent mineral trapping on the basis of CO2-water-rock interactions, which result in the formation of carbonates minerals. In order to advance our understanding of basalt sequestration in large igneous provinces, this research uses numerical simulation to evaluate the feasibility of industrial-scale CO2 injections in the Columbia River Basalt Group (CRBG). Although bulk reservoir properties are well constrained on the basis of field and laboratory testing from the Wallula Basalt Sequestration Pilot Project, there remains significant uncertainty in the spatial distribution of permeability at the scale of individual basalt flows. Geostatistical analysis of hydrologic data from 540 wells illustrates that CRBG reservoirs are reasonably modeled as layered heterogeneous systems on the basis of basalt flow morphology; however, the regional dataset is insufficient to constrain permeability variability at the scale of an individual basalt flow. As a result, permeability distribution for this modeling study is established by centering the lognormal permeability distribution in the regional dataset over the bulk permeability measured at Wallula site, which results in a spatially random permeability distribution within the target reservoir. In order to quantify the effects of this permeability uncertainty, CO2 injections are simulated within 50 equally probable synthetic reservoir domains. Each model domain comprises three-dimensional geometry with 530,000 grid blocks, and fracture-matrix interaction is simulated as interacting continua for the two low permeability layers (flow interiors) bounding the injection zone. Results from this research illustrate that permeability uncertainty at the scale of individual basalt flows may significantly impact both injection pressure accumulation and CO2 distribution.

Sequestration of flue gas CO₂ by direct gas-solid carbonation of air pollution control system residues.

PubMed

Tian, Sicong; Jiang, Jianguo

2012-12-18

Direct gas-solid carbonation reactions of residues from an air pollution control system (APCr) were conducted using different combinations of simulated flue gas to study the impact on CO₂ sequestration. X-ray diffraction analysis of APCr determined the existence of CaClOH, whose maximum theoretical CO₂ sequestration potential of 58.13 g CO₂/kg APCr was calculated by the reference intensity ratio method. The reaction mechanism obeyed a model of a fast kinetics-controlled process followed by a slow product layer diffusion-controlled process. Temperature is the key factor in direct gas-solid carbonation and had a notable influence on both the carbonation conversion and the CO₂ sequestration rate. The optimal CO₂ sequestrating temperature of 395 °C was easily obtained for APCr using a continuous heating experiment. CO₂ content in the flue gas had a definite influence on the CO₂ sequestration rate of the kinetics-controlled process, but almost no influence on the final carbonation conversion. Typical concentrations of SO₂ in the flue gas could not only accelerate the carbonation reaction rate of the product layer diffusion-controlled process, but also could improve the final carbonation conversion. Maximum carbonation conversions of between 68.6% and 77.1% were achieved in a typical flue gas. Features of rapid CO₂ sequestration rate, strong impurities resistance, and high capture conversion for direct gas-solid carbonation were proved in this study, which presents a theoretical foundation for the applied use of this encouraging technology on carbon capture and storage.

Sequestration of U(VI) from Acidic, Alkaline, and High Ionic-Strength Aqueous Media by Functionalized Magnetic Mesoporous Silica Nanoparticles: Capacity and Binding Mechanisms

EPA Science Inventory

Uranium (VI) exhibits little adsorption onto sediment minerals in acidic, alkaline or high ionic-strength aqueous media that often occur in U mining or contaminated sites, which makes U(VI) very mobile and difficult to sequester. In this work, magnetic mesoporous silica nanoparti...

Effects of small-scale chemical reactions between supercritical CO2 and arkosic sandstone on large-scale permeability fields: An experimental study with implications for geologic carbon sequestration

NASA Astrophysics Data System (ADS)

Luhmann, A. J.; Ding, K.; Saar, M. O.; Seyfried, W. E.

2011-12-01

During geologic carbon sequestration, small, pore-scale changes in mineralogy due to dissolution and precipitation reactions can modify bulk porosity. Porosity/permeability relationships are then typically used to infer large-scale permeability field changes. However, these relationships have limited use because they do not account for changes in pore geometry. Therefore, in connection with a DOE sponsored program, involving CO2 sequestration with geothermal energy usage, we constructed a novel hydrothermal flow system that allows simultaneous determination of changes in fluid chemistry and associated changes in permeability at elevated temperatures and high CO2 pressure. Initial experiments were conducted with an arkosic sandstone core of the Eau Claire Formation from southeastern Minnesota. The core was disaggregated and then wet sieved to yield a grain size distribution of 90-120 μm that was used to fill the Teflon sleeve held within the stainless steel pressure vessel. Initial water chemistry consisted of CO2 dissolved in deionized water. Outlet pressure was set to 11 MPa, and confinement pressure was 20 MPa. Flow rates produced inlet pressures between these two extremes, allowing CO2 solubility up to 1.1 mol/kg water. Rates of fluid flow ranged from 0.04 to 1.5 mL/min at a temperature of 21°C over the course of 33 days. Based on these data, the in-situ permeability of ~1E-14 to 9E-14 m2 for the arkosic sandstone was calculated. The reaction cell temperature was then increased to 50°C, and eventually 100°C. Each temperature step was associated with a sharp decrease in permeability, such that at 100°C the permeability had decreased by approximately three orders of magnitude from the starting condition. Fluid samples indicate release of dissolved Na, Ca, Mg, K, Al, SiO2, and Cl from minerals in the core, suggesting dissolution of primary mineral components. Charge balance constraints indicate a pH of approximately 4.2 at the highest temperature run condition, considerably higher than would exist in a simple water-CO2 fluid, underscoring the effectiveness of mineral dissolution/precipitation reactions in buffering pH. Distribution of aqueous species calculations suggests possible secondary phases may include illite, muscovite, kaolinite, and quartz. We speculate that mineral precipitation occurs at the fluid-mineral interface. Thus, potentially small changes in mineralogy may produce a significant change in rock permeability.

Underestimation of soil carbon stocks by Yasso07, Q, and CENTURY models in boreal forest linked to overlooking site fertility

NASA Astrophysics Data System (ADS)

Ťupek, Boris; Ortiz, Carina; Hashimoto, Shoji; Stendahl, Johan; Dahlgren, Jonas; Karltun, Erik; Lehtonen, Aleksi

2016-04-01

The soil organic carbon stock (SOC) changes estimated by the most process based soil carbon models (e.g. Yasso07, Q and CENTURY), needed for reporting of changes in soil carbon amounts for the United Nations Framework Convention on Climate Change (UNFCCC) and for mitigation of anthropogenic CO2 emissions by soil carbon management, can be biased if in a large mosaic of environments the models are missing a key factor driving SOC sequestration. To our knowledge soil nutrient status as a missing driver of these models was not tested in previous studies. Although, it's known that models fail to reconstruct the spatial variation and that soil nutrient status drives the ecosystem carbon use efficiency and soil carbon sequestration. We evaluated SOC stock estimates of Yasso07, Q and CENTURY process based models against the field data from Swedish Forest Soil National Inventories (3230 samples) organized by recursive partitioning method (RPART) into distinct soil groups with underlying SOC stock development linked to physicochemical conditions. These models worked for most soils with approximately average SOC stocks, but could not reproduce higher measured SOC stocks in our application. The Yasso07 and Q models that used only climate and litterfall input data and ignored soil properties generally agreed with two third of measurements. However, in comparison with measurements grouped according to the gradient of soil nutrient status we found that the models underestimated for the Swedish boreal forest soils with higher site fertility. Accounting for soil texture (clay, silt, and sand content) and structure (bulk density) in CENTURY model showed no improvement on carbon stock estimates, as CENTURY deviated in similar manner. We highlighted the mechanisms why models deviate from the measurements and the ways of considering soil nutrient status in further model development. Our analysis suggested that the models indeed lack other predominat drivers of SOC stabilization presumably the different role of microbes in carbon mineralization in relation to nitrogen availability and the organo - mineral carbon associations. Our results imply that the role of soil nutrient status as a regulator of carbon mineralization has to be re-evaluated, because we should have models that have their steady state SOC stocks at right level in order to predict future SOC change.

Carbon sequestration potential of soils in southeast Germany derived from stable soil organic carbon saturation.

PubMed

Wiesmeier, Martin; Hübner, Rico; Spörlein, Peter; Geuß, Uwe; Hangen, Edzard; Reischl, Arthur; Schilling, Bernd; von Lützow, Margit; Kögel-Knabner, Ingrid

2014-02-01

Sequestration of atmospheric carbon (C) in soils through improved management of forest and agricultural land is considered to have high potential for global CO2 mitigation. However, the potential of soils to sequester soil organic carbon (SOC) in a stable form, which is limited by the stabilization of SOC against microbial mineralization, is largely unknown. In this study, we estimated the C sequestration potential of soils in southeast Germany by calculating the potential SOC saturation of silt and clay particles according to Hassink [Plant and Soil 191 (1997) 77] on the basis of 516 soil profiles. The determination of the current SOC content of silt and clay fractions for major soil units and land uses allowed an estimation of the C saturation deficit corresponding to the long-term C sequestration potential. The results showed that cropland soils have a low level of C saturation of around 50% and could store considerable amounts of additional SOC. A relatively high C sequestration potential was also determined for grassland soils. In contrast, forest soils had a low C sequestration potential as they were almost C saturated. A high proportion of sites with a high degree of apparent oversaturation revealed that in acidic, coarse-textured soils the relation to silt and clay is not suitable to estimate the stable C saturation. A strong correlation of the C saturation deficit with temperature and precipitation allowed a spatial estimation of the C sequestration potential for Bavaria. In total, about 395 Mt CO2 -equivalents could theoretically be stored in A horizons of cultivated soils - four times the annual emission of greenhouse gases in Bavaria. Although achieving the entire estimated C storage capacity is unrealistic, improved management of cultivated land could contribute significantly to CO2 mitigation. Moreover, increasing SOC stocks have additional benefits with respect to enhanced soil fertility and agricultural productivity. © 2013 John Wiley & Sons Ltd.

Permeability Changes in Reaction Induced Fracturing

NASA Astrophysics Data System (ADS)

Ulven, Ole Ivar; Malthe-Sørenssen, Anders; Kalia, Rajiv

2013-04-01

The process of fracture formation due to a volume increasing chemical reaction has been studied in a variety of different settings, e.g. weathering of dolerites by Røyne et al.[4], serpentinization and carbonation of peridotite by Rudge et al.[3] and replacement reactions in silica-poor igneous rocks by Jamtveit et al.[1]. It is generally assumed that fracture formation will increase the net permeability of the rock, and thus increase the reactant transport rate and subsequently the total reaction rate, as summarised by Kelemen et al.[2]. Røyne et al.[4] have shown that transport in fractures will have an effect on the fracture pattern formed. Understanding the feedback process between fracture formation and permeability changes is essential in assessing industrial scale CO2 sequestration in ultramafic rock, but little is seemingly known about how large the permeability change will be in reaction-induced fracturing under compression, and it remains an open question how sensitive a fracture pattern is to permeability changes. In this work, we study the permeability of fractures formed under compression, and we use a 2D discrete element model to study the fracture patterns and total reaction rates achieved with different permeabilities. We achieve an improved understanding of the feedback processes in reaction-driven fracturing, thus improving our ability to decide whether industrial scale CO2 sequestration in ultramafic rock is a viable option for long-term handling of CO2. References [1] Jamtveit, B, Putnis, C. V., and Malthe-Sørenssen, A., "Reaction induced fracturing during replacement processes," Contrib. Mineral Petrol. 157, 2009, pp. 127 - 133. [2] Kelemen, P., Matter, J., Streit, E. E., Rudge, J. F., Curry, W. B., and Blusztajn, J., "Rates and Mechanisms of Mineral Carbonation in Peridotite: Natural Processes and Recipes for Enhanced, in situ CO2 Capture and Storage," Annu. Rev. Earth Planet. Sci. 2011. 39:545-76. [3] Rudge, J. F., Kelemen, P. B., and Spiegelman, M., "A simple model of reaction induced cracking applied to serpentinization and carbonation of peridotite," Earth Planet. Sci. Lett. 291, Issues 1-4, 2010, pp. 215 - 227. [4] Røyne, A., Jamtveit, B., and Malthe-Sørenssen, A., "Controls on rock weathering rates by reaction-induced hierarchial fracturing," Earth Planet. Sci. Lett. 275, 2008, pp. 364 - 369.

Wettability shifts caused by CO2 aging on mineral surfaces

NASA Astrophysics Data System (ADS)

Liang, B.; Clarens, A. F.

2015-12-01

Interfacial forces at the CO2/brine/mineral ternary interface have a well-established impact on multiphase flow properties through porous media. In the context of geologic carbon sequestration, this wettability will impact capillary pressure, residual trapping, and a variety of other key parameters of interest. While the wettability of CO2 on pure mineral and real rock sample have been studied a great deal over the past few year, very little is known about how the wettability of these rocks could change over long time horizons as CO2 interacts with species in the brine and on the mineral surface. In this work we sought to explore the role that dilute inorganic and organic species that are likely to exist in connate brines might have on a suite of mineral species. High-pressure contact angle experiments were carried out on a suite of polished mineral surfaces. Both static captive bubble and advancing/receding contact angle measurements were carried out. The effect of ionic strength, and in particular the valence of the dominant ions in the brine are found to have an important impact on the wettability which cannot be explained solely based on the shifts in the interfacial tension between the CO2 and brine. More significantly, three organic species, formate, acetate, and oxalate, all three of which are representative species commonly encountered in the saline aquifers that are considered target repositories for carbon sequestration. All three organic species show impacts on wettability, with the organics generally increasing the CO2 wetting of the mineral surface. Not all pure minerals respond the same to the presence of organics, with micas showing a more pronounced influence than quartz. Sandstone and limestone samples aged with different kinds of hydrocarbons, a surrogate for oil-bearing rocks, are generally more CO2-wet, with larger contact angles in the CO2/brine system. Over multiple days, the contact angle decreases, which could be attributed to partitioning of oil films off of the surface and into the CO2 phase, which drives the wettability towards the original water-wet state. This effect could be particularly important for organic rich repositories like depleted oil and gas fields or fractured shale formations where organic species could be presented both on mineral surfaces and in the aqueous phase.

76 FR 24007 - Notice of Intent To Prepare an Environmental Impact Statement for the Lake Charles Carbon Capture...

Federal Register 2010, 2011, 2012, 2013, 2014

2011-04-29

... Charles Carbon Capture and Sequestration Project, Lake Charles, LA AGENCY: Department of Energy. ACTION... competitive process under the Industrial Carbon Capture and Sequestration (ICCS) Program. The Lake Charles Carbon Capture and Sequestration Project (Lake Charles CCS Project) would demonstrate: (1) advanced...

Atmospheric CO2 uptake throughout bio-enhanced brucite-water reaction at Montecastelli serpentinites (Italy)

NASA Astrophysics Data System (ADS)

Bedini, Federica; Boschi, Chiara; Ménez, Benedicte; Perchiazzi, Natale; Zanchetta, Giovanni

2014-05-01

In the last several years, interactions between microorganisms and minerals have intrigued and catched the interest of the scientific community. Montecastelli serpentinites (Tuscany, Italy) are characterized by CO2-mineral carbonation, an important process which leads to spontaneous formation of carbonate phases uptaking atmospheric CO2. In the studied areas carbonate precipitates, mainly hydrated Mg-carbonates, are present in form of crusts, coating and spherules on exposed rock surfaces, and filling rock fractures. Petrographic and mineralogical observations revealed that Tuscan brucite-rich serpentinites hosts preserve their original chemical compositions with typical mesh-textured serpentine (± brucite) after olivine, magnetite-rich mesh rims and relicts of primary spinel. Representative hydrated carbonate samples have been collected in three different areas and analyzed to investigate the role of biological activity and its influence in the serpentine-hydrated Mg-carbonates reaction. The different types of whitish precipitates have been selected under binocular microscope for XRD analyses performed at the Dipartimento di Scienze della Terra (University of Pisa, Italy): their mineralogical composition consists of mainly hydromagnesite and variable amount of other metastable carbonate phases (i.e. nesquehonite, manasseite, pyroaurite, brugnatellite and aragonite). Moreover, the crystallinity analysis of whitish crust and spherules have been carried out by detailed and quantitative XRD analyses to testify a possible biologically controlled growth, inasmuch as the crystal structure of biominerals could be affected by many lattice defects (i.e. dislocations, twinning, etc.) and this observation cause low crystallinity of the mineral. The presence of microbial cells and relicts of organic matter has already been detected by confocal laser scanning microscopy (CLSM) combined with Raman spectromicroscopy in a previous study (Bedini et al., 2013). The presence of active microbial communities in or at the serpentinites surface could promote and/or enhance the key reaction through which serpentine, reacting with the carbon dioxide, becomes hydrated Mg-carbonates. This novel study aims to provide a contribution to the identification of the biominerals that could be a valid proof between CO2-mineral sequestration and microbial activity interactions. This innovative research is designed to provide a plan in future at industrial scale to reduce and capture the greenhouse gas content by Earth's atmosphere, thanks to the precipitation of carbonate biominerals. Keywords: serpentinite, carbonation, biominerals. Bedini F., Boschi C., Ménez B., Perchiazzi N., Natali C., Zanchetta G. (2013) Interaction between Geosphere and Biosphere in CO2-mineral sequestration environment. FIST GEOITALIA 2013- XI Forum di Scienze della Terra (Pisa, Italy).

Cell surface characteristics enable encrustation-free survival of neutrophilic iron-oxidizing bacteria

NASA Astrophysics Data System (ADS)

Saini, G.; Chan, C. S.

2011-12-01

Microbial growth in mineralizing environments depends on the cells' ability to evade surface precipitation. Cell-mineral interactions may be required for metabolism, but if unmoderated, cells could become encrusted, which would limit diffusion of nutrients and waste across cell walls. A combination of cell surface charge and hydrophobicity could enable the survival of microbes in such environments by inhibiting mineral attachment. To investigate this mechanism, we characterized the surfaces of two neutrophilic iron-oxidizing bacteria (FeOB): Mariprofundus ferrooxydans, a Zetaproteobacterium from Fe(II)-rich submarine hydrothermal vents and a Betaproteobacterium Gallionellales strain R-1, recently isolated from a ferrous groundwater seep. Both bacteria produce iron oxyhydroxides, yet successfully escape surface encrustation while inhabiting milieu where iron minerals are also produced by abiotic processes. SEM-EDX and TEM-EELS analyses of cultured bacteria revealed no iron on the cell surfaces. Zeta potential measurements showed that these bacteria have very small negative surface charge (0 to -4 mV) over a pH range of 4-9, indicating near-neutrally charged surfaces. Water contact angle measurements and thermodynamic calculations demonstrate that both bacteria and abiotically-formed Fe oxhydroxides are hydrophilic. Extended-DLVO calculations showed that hydrophilic repulsion between cells and minerals dominates over electrostatic and Lifshitz-van der Waals interactions. This leads to overall repulsion between microbes and minerals, thus preventing surface encrustation. Low surface charge and hydrophilicity (determined by microbial adhesion to hydrocarbon assay) were common features for both live and azide-inhibited cells, which shows that surface characteristics do not depend on active metabolism. It is remarkable that these two phylogenetically-distant bacteria from different environments employ similar adaptations to prevent surface mineralization. Our results confirm that surface characteristics can be a mechanism for survival in mineralizing environments. We predict that biotechnological applications such as bioremediation and microbial mineral carbon sequestration will benefit from microbes that can similarly avoid encrustation.

High pressure-elevated temperature x-ray micro-computed tomography for subsurface applications.

PubMed

Iglauer, Stefan; Lebedev, Maxim

2018-06-01

Physical, chemical and mechanical pore-scale (i.e. micrometer-scale) mechanisms in rock are of key importance in many, if not all, subsurface processes. These processes are highly relevant in various applications, e.g. hydrocarbon recovery, CO 2 geo-sequestration, geophysical exploration, water production, geothermal energy production, or the prediction of the location of valuable hydrothermal deposits. Typical examples are multi-phase flow (e.g. oil and water) displacements driven by buoyancy, viscous or capillary forces, mineral-fluid interactions (e.g. mineral dissolution and/or precipitation over geological times), geo-mechanical rock behaviour (e.g. rock compaction during diagenesis) or fines migration during water production, which can dramatically reduce reservoir permeability (and thus reservoir performance). All above examples are 3D processes, and 2D experiments (as traditionally done for micro-scale investigations) will thus only provide qualitative information; for instance the percolation threshold is much lower in 3D than in 2D. However, with the advent of x-ray micro-computed tomography (μCT) - which is now routinely used - this limitation has been overcome, and such pore-scale processes can be observed in 3D at micrometer-scale. A serious complication is, however, the fact that in the subsurface high pressures and elevated temperatures (HPET) prevail, due to the hydrostatic and geothermal gradients imposed upon it. Such HPET-reservoir conditions significantly change the above mentioned physical and chemical processes, e.g. gas density is much higher at high pressure, which strongly affects buoyancy and wettability and thus gas distributions in the subsurface; or chemical reactions are significantly accelerated at increased temperature, strongly affecting fluid-rock interactions and thus diagenesis and deposition of valuable minerals. It is thus necessary to apply HPET conditions to the aforementioned μCT experiments, to be able to mimic subsurface conditions in a realistic way, and thus to obtain reliable results, which are vital input parameters required for building accurate larger-scale reservoir models which can predict the overall reservoir-scale (hectometer-scale) processes (e.g. oil production or diagenesis of a formation). We thus describe here the basic workflow of such HPET-μCT experiments, equipment requirements and apparatus design; and review the literature where such HPET-μCT experiments were used and which phenomena were investigated (these include: CO 2 geo-sequestration, oil recovery, gas hydrate formation, hydrothermal deposition/reactive flow). One aim of this paper is to give a guideline to users how to set-up a HPET-μCT experiment, and to provide a quick overview in terms of what is possible and what not, at least up to date. As a conclusion, HPET-μCT is a valuable tool when it comes to the investigation of subsurface micrometer-scaled processes, and we expect a rapidly expanding usage of HPET-μCT in subsurface engineering and the subsurface sciences. Copyright © 2018 Elsevier B.V. All rights reserved.

Dewetting of silica surfaces upon reactions with supercritical CO2 and brine: pore-scale studies in micromodels.

PubMed

Kim, Yongman; Wan, Jiamin; Kneafsey, Timothy J; Tokunaga, Tetsu K

2012-04-03

Wettability of reservoir minerals and rocks is a critical factor controlling CO(2) mobility, residual trapping, and safe-storage in geologic carbon sequestration, and currently is the factor imparting the greatest uncertainty in predicting capillary behavior in porous media. Very little information on wettability in supercritical CO(2) (scCO(2))-mineral-brine systems is available. We studied pore-scale wettability and wettability alteration in scCO(2)-silica-brine systems using engineered micromodels (transparent pore networks), at 8.5 MPa and 45 °C, over a wide range of NaCl concentrations up to 5.0 M. Dewetting of silica surfaces upon reactions with scCO(2) was observed through water film thinning, water droplet formation, and contact angle increases within single pores. The brine contact angles increased from initial values near 0° up to 80° with larger increases under higher ionic strength conditions. Given the abundance of silica surfaces in reservoirs and caprocks, these results indicate that CO(2) induced dewetting may have important consequences on CO(2) sequestration including reducing capillary entry pressure, and altering quantities of CO(2) residual trapping, relative permeability, and caprock integrity.

Numerical modeling of time-lapse monitoring of CO2 sequestration in a layered basalt reservoir

USGS Publications Warehouse

Khatiwada, M.; Van Wijk, K.; Clement, W.P.; Haney, M.

2008-01-01

As part of preparations in plans by The Big Sky Carbon Sequestration Partnership (BSCSP) to inject CO2 in layered basalt, we numerically investigate seismic methods as a noninvasive monitoring technique. Basalt seems to have geochemical advantages as a reservoir for CO2 storage (CO2 mineralizes quite rapidly while exposed to basalt), but poses a considerable challenge in term of seismic monitoring: strong scattering from the layering of the basalt complicates surface seismic imaging. We perform numerical tests using the Spectral Element Method (SEM) to identify possibilities and limitations of seismic monitoring of CO2 sequestration in a basalt reservoir. While surface seismic is unlikely to detect small physical changes in the reservoir due to the injection of CO2, the results from Vertical Seismic Profiling (VSP) simulations are encouraging. As a perturbation, we make a 5%; change in wave velocity, which produces significant changes in VSP images of pre-injection and post-injection conditions. Finally, we perform an analysis using Coda Wave Interferometry (CWI), to quantify these changes in the reservoir properties due to CO2 injection.

Advances in Geological CO{sub 2} Sequestration and Co-Sequestration with O{sub 2}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Verba, Circe A; O'Connor, William K.; Ideker, J.H.

2012-10-28

The injection of CO{sub 2} for Enhanced Oil Recovery (EOR) and sequestration in brine-bearing formations for long term storage has been in practice or under investigation in many locations globally. This study focused on the assessment of cement wellbore seal integrity in CO{sub 2}- and CO{sub 2}-O{sub 2}-saturated brine and supercritical CO{sub 2} environments. Brine chemistries (NaCl, MgCl{sub 2}, CaCl{sub 2}) at various saline concentrations were investigated at a pressure of 28.9 MPa (4200 psi) at both 50{degree}C and 85{degree}C. These parameters were selected to simulate downhole conditions at several potential CO{sub 2} injection sites in the United States. Classmore » H portland cement is not thermodynamically stable under these conditions and the formation of carbonic acid degrades the cement. Dissociation occurs and leaches cations, forming a CaCO{sub 3} buffered zone, amorphous silica, and other secondary minerals. Increased temperature affected the structure of C-S-H and the hydration of the cement leading to higher degradation rates.« less

Supercritical carbon dioxide and sulfur in the Madison Limestone: A natural analog in southwest Wyoming for geologic carbon-sulfur co-sequestration

NASA Astrophysics Data System (ADS)

Kaszuba, John P.; Navarre-Sitchler, Alexis; Thyne, Geoffrey; Chopping, Curtis; Meuzelaar, Tom

2011-09-01

The Madison Limestone on the Moxa Arch, southwest Wyoming, USA contains large volumes (65-95%) of supercritical CO 2 that it has stored naturally for 50 million years. This reservoir also contains supercritical H 2S, aqueous sulfur complexes (SO 42- and HS -), and sulfur-bearing minerals (anhydrite and pyrite). Although SO 2 is not present, these sulfur-bearing phases are known products of SO 2 disproportionation in other water-rock systems. The natural co-occurrence of SO 42-, S 2-, supercritical CO 2 and brine affords the opportunity to evaluate the fate of a carbon-sulfur co-sequestration scenario. Mineralogic data was obtained from drill core and aqueous geochemical data from wells outside and within the current supercritical CO 2-sulfur-brine-rock system. In addition to dolomite, calcite, and accessory sulfur-bearing minerals, the Madison Limestone contains accessory quartz and the aluminum-bearing minerals feldspar, illite, and analcime. Dawsonite (NaAlCO 3(OH) 2), predicted as an important carbon sink in sequestration modeling studies, is not present. After confirming equilibrium conditions for the Madison Limestone system, reaction path models were constructed with initial conditions based on data from outside the reservoir. Addition of supercritical CO 2 to the Madison Limestone was simulated and the results compared to data from inside the reservoir. The model accurately predicts the observed mineralogy and captures the fundamental changes expected in a Madison Limestone-brine system into which CO 2 is added. pH decreases from 5.7 to 4.5 at 90 °C and to 4.0 at 110 °C, as expected from dissolution of supercritical CO 2, creation of carbonic acid, and buffering by the carbonate rock. The calculated redox potential increases by 0.1 V at 90 °C and 0.15 V at 110 °C due to equilibrium among CO 2, anhydrite, and pyrite. Final calculated Eh and pH match conditions for the co-existing sulfur phases present in produced waters and core from within the reservoir. Total dissolved solids increase with reaction progress, mostly due to dissolution of calcite with an accompanying increase in dissolved bicarbonate. The Madison Limestone is a natural example of the thermodynamic end point that similar fluid-rock systems will develop following emplacement of a supercritical CO 2-sulfur mixture and is a natural analog for geologic carbon-sulfur co-sequestration.

Comparative Reactivity Study of Forsterite and Antigorite in Wet Supercritical CO2 by In Situ Infrared Spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Thompson, Christopher J.; Loring, John S.; Rosso, Kevin M.

2013-10-01

The carbonation reactions of forsterite (Mg2SiO4) and antigorite [Mg3Si2O5(OH)4], representatives of olivine and serpentine minerals, in dry and wet supercritical carbon dioxide (scCO2) at conditions relevant to geologic carbon sequestration (35 °C and 100 bar) were studied by in-situ Fourier transform infrared (FT-IR) spectroscopy. Our results confirm that water plays a critical role in the reactions between metal silicate minerals and scCO2. For neat scCO2, no reaction was observed in 24 hr for either mineral. When water was added to the scCO2, a thin water film formed on the minerals’ surfaces, and the reaction rates and extents increased as themore » water saturation level was raised from 54% to 116% (excess water). For the first time, the presence of bicarbonate, a key reaction intermediate for metal silicate reactions with scCO2, was observed in a heterogeneous system where mineral solids, an adsorbed water film, and bulk scCO2 co-exist. In excess-water experiments, approximately 4% of forsterite and less than 2% of antigorite transformed into hydrated Mg-carbonates. A precipitate similar to nesquehonite (MgCO3•3H2O) was observed for forsterite within 6 hr of reaction time, but no such precipitate was formed from antigorite until after water was removed from the scCO2 following a 24-hr reaction period. The reduced reactivity and carbonate-precipitation behavior of antigorite was attributed to slower, incongruent dissolution of the mineral and lower concentrations of Mg2+ and HCO3- in the water film. The in situ measurements employed in this work make it possible to quantify metal carbonate precipitates and key reaction intermediates such as bicarbonate for the investigation of carbonation reaction mechanisms relevant to geologic carbon sequestration.« less

Carbonation of mantle peridotites: implications for permanent geological CO2 capture and storage

NASA Astrophysics Data System (ADS)

Paukert, A. N.; Matter, J. M.; Kelemen, P. B.; Marsala, P.; Shock, E.

2012-12-01

In situ carbonation of mantle peridotites serves as a natural analog to engineered mineral carbonation for geological CO2 capture and storage. For example, mantle peridotite in the Samail Ophiolite, Oman naturally captures and stores about 5x104 tons of atmospheric CO2 per year as carbonate minerals, and has been doing so for the past 50,000 years [Kelemen et al., 2011]. Our reaction path modeling of this system shows that the natural process is limited by subsurface availability of dissolved inorganic carbon, and that the rate of CO2 mineralization could be enhanced by a factor of 16,000 by injecting CO2 into the peridotite aquifer at 2 km depth and a fugacity of 100 bars. Injecting CO2 into mafic or ultramafic rock formations has been presumed difficult, as fractured crystalline rocks typically have low porosity and permeability; however these factors have yet to be comprehensively studied. To determine the actual value of these hydrogeological factors, this winter we carried out a multifaceted study of deep boreholes (up to 350m) in the mantle peridotite and the Moho transition zone of the Samail Ophiolite. A suite of physical and chemical parameters were collected, including slug tests for hydraulic conductivity, geophysical well logs for porosity and hydraulic conductivity, drill chips for extent and composition of secondary mineralization, and water and dissolved gas samples for chemical composition. All of these factors combine to provide a comprehensive look at the chemical and physical processes underlying natural mineral carbonation in mantle peridotites. Understanding the natural process is critical, as mineral carbonation in ultramafic rocks is being explored as a permanent and relatively safe option for geologic carbon sequestration. While injectivity in these ultramafic formations was believed to be low, our slug test and geophysical well log data suggest that the hydraulic conductivity of fractured peridotites can actually be fairly high - up to meters/day, on par with fine to medium grained sandstones - so these formations may be more suitable than previously thought. Using the Samail Ophiolite as a natural analog for in situ mineral carbonation in ultramafic rocks should help predict and optimize the efficacy and security of engineered CO2 storage projects.

Development of Protective Coatings for Co-Sequestration Processes and Pipelines

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bierwagen, Gordon; Huang, Yaping

2011-11-30

The program, entitled Development of Protective Coatings for Co-Sequestration Processes and Pipelines, examined the sensitivity of existing coating systems to supercritical carbon dioxide (SCCO2) exposure and developed new coating system to protect pipelines from their corrosion under SCCO2 exposure. A literature review was also conducted regarding pipeline corrosion sensors to monitor pipes used in handling co-sequestration fluids. Research was to ensure safety and reliability for a pipeline involving transport of SCCO2 from the power plant to the sequestration site to mitigate the greenhouse gas effect. Results showed that one commercial coating and one designed formulation can both be supplied asmore » potential candidates for internal pipeline coating to transport SCCO2.« less

Microbial Carbonic Anhydrases in Biomimetic Carbon Sequestration for Mitigating Global Warming: Prospects and Perspectives

PubMed Central

Bose, Himadri; Satyanarayana, Tulasi

2017-01-01

All the leading cities in the world are slowly becoming inhospitable for human life with global warming playing havoc with the living conditions. Biomineralization of carbon dioxide using carbonic anhydrase (CA) is one of the most economical methods for mitigating global warming. The burning of fossil fuels results in the emission of large quantities of flue gas. The temperature of flue gas is quite high. Alkaline conditions are necessary for CaCO3 precipitation in the mineralization process. In order to use CAs for biomimetic carbon sequestration, thermo-alkali-stable CAs are, therefore, essential. CAs must be stable in the presence of various flue gas contaminants too. The extreme environments on earth harbor a variety of polyextremophilic microbes that are rich sources of thermo-alkali-stable CAs. CAs are the fastest among the known enzymes, which are of six basic types with no apparent sequence homology, thus represent an elegant example of convergent evolution. The current review focuses on the utility of thermo-alkali-stable CAs in biomineralization based strategies. A variety of roles that CAs play in various living organisms, the use of CA inhibitors as drug targets and strategies for overproduction of CAs to meet the demand are also briefly discussed. PMID:28890712

Microbial Carbonic Anhydrases in Biomimetic Carbon Sequestration for Mitigating Global Warming: Prospects and Perspectives.

PubMed

Bose, Himadri; Satyanarayana, Tulasi

2017-01-01

All the leading cities in the world are slowly becoming inhospitable for human life with global warming playing havoc with the living conditions. Biomineralization of carbon dioxide using carbonic anhydrase (CA) is one of the most economical methods for mitigating global warming. The burning of fossil fuels results in the emission of large quantities of flue gas. The temperature of flue gas is quite high. Alkaline conditions are necessary for CaCO 3 precipitation in the mineralization process. In order to use CAs for biomimetic carbon sequestration, thermo-alkali-stable CAs are, therefore, essential. CAs must be stable in the presence of various flue gas contaminants too. The extreme environments on earth harbor a variety of polyextremophilic microbes that are rich sources of thermo-alkali-stable CAs. CAs are the fastest among the known enzymes, which are of six basic types with no apparent sequence homology, thus represent an elegant example of convergent evolution. The current review focuses on the utility of thermo-alkali-stable CAs in biomineralization based strategies. A variety of roles that CAs play in various living organisms, the use of CA inhibitors as drug targets and strategies for overproduction of CAs to meet the demand are also briefly discussed.

Engineered Biomimetic Polymers as Tunable Agents for Controlling CaCO₃ Mineralization

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, Chun-Long; Qi, Jiahui; Zuckermann, Ronald N.

2011-01-01

In nature, living organisms use peptides and proteins to precisely control the nucleation and growth of inorganic minerals and sequester CO₂ via mineralization of CaCO₃. Here we report the exploitation of a novel class of sequence-specific non-natural polymers called peptoids as tunable agents that dramatically control CaCO₃ mineralization. We show that amphiphilic peptoids composed of hydrophobic and anionic monomers exhibit both a high degree of control over calcite growth morphology and an unprecedented 23-fold acceleration of growth at a peptoid concentration of only 50 nM, while acidic peptides of similar molecular weight exhibited enhancement factors of only ~2 or less.more » We further show that both the morphology and rate controls depend on peptoid sequence, side-chain chemistry, chain length, and concentration. These findings provide guidelines for developing sequence-specific non-natural polymers that mimic the functions of natural peptides or proteins in their ability to direct mineralization of CaCO₃, with an eye toward their application to sequestration of CO₂ through mineral trapping.« less

Mineral Dissolution and Precipitation due to Carbon Dioxide-Water-Rock Interactions: The Significance of Accessory Minerals in Carbonate Reservoirs (Invited)

NASA Astrophysics Data System (ADS)

Kaszuba, J. P.; Marcon, V.; Chopping, C.

2013-12-01

Accessory minerals in carbonate reservoirs, and in the caprocks that seal these reservoirs, can provide insight into multiphase fluid (CO2 + H2O)-rock interactions and the behavior of CO2 that resides in these water-rock systems. Our program integrates field data, hydrothermal experiments, and geochemical modeling to evaluate CO2-water-rock reactions and processes in a variety of carbonate reservoirs in the Rocky Mountain region of the US. These studies provide insights into a wide range of geologic environments, including natural CO2 reservoirs, geologic carbon sequestration, engineered geothermal systems, enhanced oil and gas recovery, and unconventional hydrocarbon resources. One suite of experiments evaluates the Madison Limestone on the Moxa Arch, Southwest Wyoming, a sulfur-rich natural CO2 reservoir. Mineral textures and geochemical features developed in the experiments suggest that carbonate minerals which constitute the natural reservoir will initially dissolve in response to emplacement of CO2. Euhedral, bladed anhydrite concomitantly precipitates in response to injected CO2. Analogous anhydrite is observed in drill core, suggesting that secondary anhydrite in the natural reservoir may be related to emplacement of CO2 into the Madison Limestone. Carbonate minerals ultimately re-precipitate, and anhydrite dissolves, as the rock buffers the acidity and reasserts geochemical control. Another suite of experiments emulates injection of CO2 for enhanced oil recovery in the Desert Creek Limestone (Paradox Formation), Paradox Basin, Southeast Utah. Euhedral iron oxyhydroxides (hematite) precipitate at pH 4.5 to 5 and low Eh (approximately -0.1 V) as a consequence of water-rock reaction. Injection of CO2 decreases pH to approximately 3.5 and increases Eh by approximately 0.1 V, yielding secondary mineralization of euhedral pyrite instead of iron oxyhydroxides. Carbonate minerals also dissolve and ultimately re-precipitate, as determined by experiments in the Madison Limestone, but pyrite will persist and iron oxyhydroxides will not recrystallize.

Quantifying carbon sequestration in forest plantations by modeling the dynamics of above and below ground carbon pools

Treesearch

Chris A. Maier; Kurt H. Johnsen

2010-01-01

Intensive pine plantation management may provide opportunities to increase carbon sequestration in the Southeastern United States. Developing management options that increase fiber production and soil carbon sequestration require an understanding of the biological and edaphic processes that control soil carbon turnover. Belowground carbon resides primarily in three...

An experimental study of the carbonation of serpentinite and partially serpentinised peridotites

NASA Astrophysics Data System (ADS)

Lacinska, Alicja M.; Styles, Michael T.; Bateman, Keith; Hall, Matthew; Brown, Paul D.

2017-06-01

In situ sequestration of CO2 in mantle peridotites has been proposed as a method to alleviate the amount of anthropogenic CO2 in the atmosphere. This study presents the results of eight-month long laboratory fluid-rock experiments on representative mantle rocks from the Oman-United Arab Emirates ophiolite to investigate this process. Small core samples (3 cm long) were reacted in wet supercritical CO2 and CO2-saturated brine at 100 bar and 70°C. The extent of carbonate formation, and hence the degree of carbon sequestration, varied greatly depending on rock type, with serpentinite (lizardite-dominated) exhibiting the highest capacity, manifested by the precipitation of magnesite MgCO3 and ferroan magnesite (Mg,Fe)CO3. The carbonate precipitation occurred predominantly on the surface of the core and subordinately within cross-cutting fractures. The extent of the CO2 reactions appeared to be principally controlled by the chemical and mineralogical composition of the rock, as well as the rock texture, with all these factors influencing the extent and rate of mineral dissolution and release of Mg and Fe for subsequent reaction with the CO2. It was calculated that ≈ 0.7 g of CO2 was captured by reacting ≈ 23 g of serpentinite, determined by the mass of magnesite formed. This equates to ≈ 30 kg CO2 per tonne of host rock, equivalent to ≈ 3% carbonation in half a year. However, recycling of carbonate present in veins within the original rock sample could mean that the overall amount is around 2%. The increased reactivity of serpentinite was associated with preferential dissolution of more reactive types of serpentine minerals and brucite, that were mainly present in the cross-cutting veins. The bulk of the serpentinite rock was little affected. This study, using relatively short term experiments, suggests that serpentinite might be a good host rock for CO2 sequestration, although long term experiments might prove that dunite and harzburgite could be an effective in an engineered system of CCSM. Wet scCO2 proved to be chemically aggressive than CO2-saturated brine and its ingress along fractures and grain boundaries resulted in greater host rock dissolution and subsequent carbonate precipitation.

Vegetation Structure Controls Carbon Sequestration Potential in a Savannah Ecosystem of Mt. Kilimanjaro Region

NASA Astrophysics Data System (ADS)

Becker, J. N.; Gutlein, A.; Sierra Cornejo, N.; Ralf, K.; Hertel, D.; Kuzyakov, Y.

2016-12-01

The savannah biome is a hotspot for biodiversity and wildlife conservation in Africa and recently got in the focus of research on carbon (C) sequestration. Savanna ecosystems are increasingly pressured by climate and land-use changes, especially around populous areas such as the Mt. Kilimanjaro region. Savanna vegetation consists of grassland with isolated trees and is therefore characterized by high spatial variation and patchiness of canopy cover and aboveground biomass. Both are major regulators for soil ecological properties and soil-atmospheric trace gas exchange (CO2, N2O, CH4), especially in water-limited environments. Our objectives were to determine spatial trends in soil properties and trace-gas fluxes during the dry season and to relate above- and belowground processes and attributes. We chose three trees from each of the two most dominant species (Acacia nilotica and Balanites aegyptiaca) in our research area. For each tree, we selected transects with nine sampling points of the same relative distances to the stem. At each sampling point (0-10 & 10-30 cm depth) we measured soil C and nitrogen (N) storage, microbial biomass C and N, Natural δ13C, soil respiration, available nutrients, pH, cation exchange capacity (CEC) as well as root biomass and -density, soil temperature and soil water content. The tree species had no effect on soil parameters and gas fluxes under the crown. CEC, C and N fractions decreased up to 50% outside the crown-covered area. Tree leaf litter had a far lower C:N ratio than leaf litter of the C4-grass species. δ13C in soil under the crowns shifted about 15% in the direction of tree leaf litter δ13C compared to soil in open area reflecting the tree litter contribution to soil organic matter. The microbial C:N ratio and CO2 efflux were about 30% higher in the open area and strongly dependent on mineral N availability. This indicates N limitation and low C-use efficiency in soil under open grassland. We conclude that the spatial structure of aboveground biomass in savanna ecosystems leads to a spatial redistribution of nutrient availability and thus in C mineralization and sequestration. Therefore, the capability of savanna ecosystems to act as C sinks is both directly and indirectly dependent on the abundance of trees regardless of their N-fixing capability.

Silicate Carbonation in Supercritical CO2 Containing Dissolved H2O: An in situ High Pressure X-Ray Diffraction Study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schaef, Herbert T.; Miller, Quin RS; Thompson, Christopher J.

2013-06-30

Technological advances have been significant in recent years for managing environmentally harmful emissions (mostly CO2) resulting from combustion of fossil fuels. Deep underground geologic formations are emerging as reasonable options for long term storage of CO2 but mechanisms controlling rock and mineral stability in contact with injected supercritical fluids containing water are relatively unknown. In this paper, we discuss mineral transformation reactions occurring between supercritical CO2 containing water and the silicate minerals forsterite (Mg2SiO4), wollastonite (CaSiO3), and enstatite (MgSiO3). This study utilizes newly developed in situ high pressure x-ray diffraction (HXRD) and in situ infra red (IR) to examine mineralmore » transformation reactions. Forsterite and enstatite were selected as they are important minerals present in igneous and mafic rocks and have been the subject of a large number of aqueous dissolution studies that can be compared with non-aqueous fluid tests in this study. Wollastonite, classified as a pyroxenoid (similar to a pyroxene), was chosen as a suitably fast reacting proxy for examining silicate carbonation processes associated with a wet scCO2 fluid as related to geologic carbon sequestration. The experiments were conducted under modest pressures (90 to 160 bar), temperatures between 35° to 70° C, and varying concentrations of dissolved water. Under these conditions scCO2 contains up to 3,500 ppm dissolved water.« less

Organic horizon and mineral soil mercury along three clear-cut forest chronosequences across the northeastern USA.

PubMed

Richardson, Justin B; Petrenko, Chelsea L; Friedland, Andrew J

2017-12-01

Mercury (Hg) is a globally distributed pollutant trace metal that has been increasing in terrestrial environments due to rising anthropogenic emissions. Vegetation plays an important role in Hg sequestration in forested environments, but increasing tree removal for biofuels and wood products may affect this process. The long-term effect of clear-cutting on forest soil Hg remains uncertain, since most studies are limited to measuring changes for < 10 years following a single harvest event. The chronosequence approach, which substitutes space for time using forest stands of different ages since clear-cutting, allows for investigation of processes occurring over decades to centuries. Here, we utilized three clear-cut forest soil chronosequences across the northeastern USA to understand Hg accumulation and retention over several decades. Total Hg concentrations and pools were quantified for five soil depth increments along three chronosequences. Our results showed Hg concentrations and pools decreased in the initial 20 years following clear-cutting. Mineral soil Hg pools decreased 21-53% (7-14 mg m -2 ) between 1-5-year-old stands and 15-25-year-old stands but mineral soil Hg pools recovered in 55-140-year-old stands to similar values as measured in 1-5-year-old stands. Our study is one of the first to demonstrate a decrease and recovery in Hg pool size. These changes in Hg did not correspond with changes in bulk density, soil C, or pH. We utilized a simple two-box model to determine how different Hg fluxes affected organic and mineral soil horizon Hg pools. Our simple model suggests that changes in litterfall and volatilization rates could have caused the observed changes in organic horizon Hg pools. However, only increases in leaching could reproduce observed decreases to mineral soil Hg pools. Further studies are needed to determine the mechanism of Hg loss from forest soils following clear-cutting.

Land use effects on soil organic carbon sequestration in calcareous leptosols in former pastureland - a case study from the Tatra Mountains (Poland)

NASA Astrophysics Data System (ADS)

Wasak, K.; Drewnik, M.

2015-05-01

The purpose of the paper is to show SOC sequestration rates in calcareous shallow soils in reforested areas in Tatra Mts. with a particular focus on the different forms of organic matter (OM) storage. Three plant communities creating a mosaic on the slopes of the valley were taken into account. After 50 years since the conversion of pastureland to grassland, dwarf pine shrub, and larch forest on soils, the development of genetic soil horizons as well as SOC sequestration in soil occur despite the steepness of slopes. SOC stock is the highest in soils under larch forest (63.5 mg ha-1, SD 16.3), while in soil under grassland and under dwarf pine shrub, this value is smaller (47.5 mg ha-1, SD 13.3 and 42.9 mg ha-1, SD 22.0 respectively). The highest amount of mineral-associated OM inside stable microaggregates (MOM FF3) is found in grassland soil (21.9-27.1% of SOC), less under dwarf pine shrub (16.3-19.3% of SOC) and larch forest (15.3-17.7% of SOC). The pool of mineral-associated OM inside transitional macroaggregates (MOM FF2) is found in soil under dwarf pine shrub (39.2-59.2% of SOC), with less under larch forest (43.8-44.7% of SOC) and the least in grassland soil (37.9-41.6% of SOC). The highest amount of the free light particulate fraction (POM LF1) is found in soil under dwarf pine shrub (6.6-10.3% of SOC), with less under larch forest (2.6-6.2% of SOC) and the least in grassland soil (1.7-4.8% of SOC).

Land use effects on soil organic carbon sequestration in calcareous Leptosols in former pastureland - a case study from the Tatra Mountains (Poland)

NASA Astrophysics Data System (ADS)

Wasak, K.; Drewnik, M.

2015-10-01

The purpose of the paper is to describe soil organic carbon (SOC) sequestration rates in calcareous shallow soils in reforested areas in the Tatra Mountains with a particular focus on different forms of organic matter (OM) storage. Three plant communities creating a mosaic on the slopes of the studied valley were taken into account. Fifty years since the conversion of pastureland to unused grassland, dwarf pine shrub and larch forest have emerged in the study area, along with the development of genetic soil horizons as well as SOC sequestration in the soil despite the steepness of slopes. SOC stock was measured to be the highest in soils under larch forest (63.5 Mg ha-1), while in soil under grassland and under dwarf pine shrub, this value was found to be smaller (47.5 and 42.9 Mg ha-1, respectively). The highest amount of mineral-associated OM inside stable microaggregates (MOM FF3) was found in grassland soil (21.9-27.1 % of SOC) and less under dwarf pine shrub (16.3-19.3 % of SOC) and larch forest (15.3-17.7 % of SOC). A pool of mineral-associated OM inside transitional macroaggregates (MOM FF2) was found in soil under dwarf pine shrub (39.2-59.2 % of SOC), with less under larch forest (43.8-44.7 % of SOC) and the least in grassland soil (37.9-41.6 % of SOC). The highest amount of the free light particulate fraction (POM LF1) was found in soil under dwarf pine shrub (6.6-10.3 % of SOC), with less under larch forest (2.6-6.2 % of SOC) and the least in grassland soil (1.7-4.8 % of SOC).

Carbon Dioxide Sequestration in Depleted Oil/Gas Fields: Evaluation of Gas Microseepage and Carbon Dioxide Fate at Rangely, Colorado USA

NASA Astrophysics Data System (ADS)

Klusman, R. W.

2002-12-01

Large-scale CO2 dioxide injection for purposes of enhanced oil recovery (EOR) has been operational at Rangely, Colorado since 1986. The Rangely field serves as an onshore prototype for CO2 sequestration in depleted fields by production of a valuable commodity which partially offsets infrastructure costs. The injection is at pressures considerably above hydrostatic pressure, enhancing the possibility for migration of buoyant gases toward the surface. Methane and CO2 were measured in shallow soil gas, deep soil gas, and as fluxes into the atmosphere in both winter and summer seasons. There were large seasonal variations in surface biological noise. The direct measurement of CH4 flux to the atmosphere gave an estimate of 400 metric tonnes per year over the 78 km2 area, and carbon dioxide flux was between 170 and 3800 metric tonnes per year. Both stable carbon isotopes and carbon-14 were used in constructing these estimates. Computer modeling of the unsaturated zone migration, and of methanotrophic oxidation rates suggests a large portion of the CH4 is oxidized in the summer, and at a much lower rate in the winter. However, deep-sourced CH4 makes a larger contribution to the atmosphere than CO2, in terms of GWP. The 23+ million tonnes of carbon dioxide that have been injected at Rangely are largely stored as dissolved CO2 and a lesser amount as bicarbonate. Scaling problems, as a result of acid gas dissolution of carbonate cement, and subsequent precipitation of CaSO4 will be an increasing problem as the system matures. Evidence for mineral sequestration was not found in the scales. Ultimate injector and field capacities will be determined by mineral precipitation in the formation as it affects porosity and permeability.

[Soil organic carbon mineralization of Black Locust forest in the deep soil layer of the hilly region of the Loess Plateau, China].

PubMed

Ma, Xin-Xin; Xu, Ming-Xiang; Yang, Kai

2012-11-01

The deep soil layer (below 100 cm) stores considerable soil organic carbon (SOC). We can reveal its stability and provide the basis for certification of the deep soil carbon sinks by studying the SOC mineralization in the deep soil layer. With the shallow soil layer (0-100 cm) as control, the SOC mineralization under the condition (temperature 15 degrees C, the soil water content 8%) of Black Locust forest in the deep soil layer (100-400 cm) of the hilly region of the Loess Plateau was studied. The results showed that: (1) There was a downward trend in the total SOC mineralization with the increase of soil depth. The total SOC mineralization in the sub-deep soil (100-200 cm) and deep soil (200-400 cm) were equivalent to approximately 88.1% and 67.8% of that in the shallow layer (0-100 cm). (2) Throughout the carbon mineralization process, the same as the shallow soil, the sub-deep and deep soil can be divided into 3 stages. In the rapid decomposition phase, the ratio of the mineralization or organic carbon to the total mineralization in the sub-deep and deep layer (0-10 d) was approximately 50% of that in the shallow layer (0-17 d). In the slow decomposition phase, the ratio of organic carbon mineralization to total mineralization in the sub-deep, deep layer (11-45 d) was 150% of that in the shallow layer (18-45 d). There was no significant difference in this ratio among these three layers (46-62 d) in the relatively stable stage. (3) There was no significant difference (P > 0.05) in the mineralization rate of SOC among the shallow, sub-deep, deep layers. The stability of SOC in the deep soil layer (100-400 cm) was similar to that in the shallow soil layer and the SOC in the deep soil layer was also involved in the global carbon cycle. The change of SOC in the deep soil layer should be taken into account when estimating the effects of soil carbon sequestration in the Hilly Region of the Loess Plateau, China.

Direct effects of temperature on forest nitrogen cycling revealed through analysis of long-term watershed records

Treesearch

E.N. Jack Brookshire; Stefan Gerber; Jackson R. Webster; James M. Vose; Wayne T. Swank

2010-01-01

The microbial conversion of organic nitrogen (N) to plant available forms is a critical determinant of plant growth and carbon sequestration in forests worldwide. In temperate zones, microbial activity is coupled to variations in temperature, yet at the ecosystem level, microbial N mineralization seems to play a minor role in determining patterns of N loss. Rather, N...

Biogeosystem Technique as a method to correct the climate

NASA Astrophysics Data System (ADS)

Kalinitchenko, Valery; Batukaev, Abdulmalik; Batukaev, Magomed; Minkina, Tatiana

2017-04-01

The climate change and uncertainties of biosphere are on agenda. Correction o the climate drivers will make the climate and biosphere more predictable and certain. Direct sequestration of fossil industrial hydrocarbons and natural methane excess for greenhouse effect reduction is a dangerous mistake. Most quantity of carbon now exists in the form of geological deposits and further reduction of carbon content in biosphere and atmosphere leads to degradation of life. We propose the biological management of the greenhouse gases changing the ratio of biological and atmospheric phases of carbon and water cycle. The biological correction of carbon cycle is the obvious measure because the biological alterations of the Earth's climate have ever been an important peculiarity of the Planet's history. At the first stage of the Earth's climate correction algorithm we use the few leading obvious principal as follows: The more greenhouse amount in atmosphere, the higher greenhouse effect; The more biological production of terrestrial ecosystem, the higher carbon dioxide biological sequestration from atmosphere; The more fresh ionized active oxygen biological production, the higher rate of methane and hydrogen sulfide oxidation in atmosphere, water and soil; The more quantity of carbon in the form of live biological matter in soil and above-ground biomass, the less quantity of carbon in atmosphere; The less sink of carbon to water system, the less emission of greenhouse gases from water system; The less rate of water consumption per unit of biological production, the less transpiration rate of water vapor as a greenhouse gas; The higher intra-soil utilization of mortal biomass, biological and mineral wastes into the plant nutrition instead of its mineralization to greenhouse gases, the less greenhouse effect; The more fossil industrial hydrocarbons are used, the higher can be Earth's biomass; The higher biomass on the Earth, the more of ecology safe food, raw material and biofuel can be produced; The less energy is consumed for climate correction, the better. The proposed algorithm was never discussed before because most of its ingredients were unenforceable. Now the possibility to execute the algorithm exists in the framework of our new scientific-technical branch - Biogeosystem Technique (BGT*). The BGT* is a transcendental (non-imitating natural processes) approach to soil processing, regulation of energy, matter, water fluxes and biological productivity of biosphere: intra-soil machining to provide the new highly productive dispersed system of soil; intra-soil pulse continuous-discrete plants watering to reduce the transpiration rate and water consumption of plants for 5-20 times; intra-soil environmentally safe return of matter during intra-soil milling processing and (or) intra-soil pulse continuous-discrete plants watering with nutrition. Are possible: waste management; reducing flow of nutrients to water systems; carbon and other organic and mineral substances transformation into the soil to plant nutrition elements; less degradation of biological matter to greenhouse gases; increasing biological sequestration of carbon dioxide in terrestrial system's photosynthesis; oxidizing methane and hydrogen sulfide by fresh photosynthesis ionized biologically active oxygen; expansion of the active terrestrial site of biosphere. The high biological product output of biosphere will be gained. BGT* robotic systems are of low cost, energy and material consumption. By BGT* methods the uncertainties of climate and biosphere will be reduced. Key words: Biogeosystem Technique, method to correct, climate

Evaluating CO2 mineralization capacity of sedimentary rock Using BCR sequential extraction procedures

NASA Astrophysics Data System (ADS)

Yang, Gang-Ting; Yu, Chi-Wen; Yang, Hsiao-Ming; Chiao, Chung-Hui; Yang, Ming-Wei

2015-04-01

To relief the high concentration of carbon dioxide in the atmosphere, carbon capture and storage (CCS) is gradually becoming an important concept to reduce greenhouse gas emissions. In IPCC Special Report on CCS, the storage mechanisms for geological formations are categorized into structural/stratigraphic, hydrodynamic and geochemical trappings. Geochemical trapping is considered as a storage mechanism, which can further increase storage capacity, effectiveness and security in terms of permanent CO2 sequestration. The injected CO2 can have geochemical interactions with pore fluid and reservoir rocks and transform into minerals. It is important to evaluate the capacity of reservoir rock for sequestrating CO2. In this study, sedimentary rock samples were collected from a 2-km-deep well in Midwestern Taiwan; and, the BCR sequential extraction experiments developed by European Union Measurement and Testing Programme were conducted. BCR was designed for extracting three major phases from soil, including exchangeable phase and carbonates (the first stage), reducible phase (the second stage) and oxidizable phase (the third stage). The chemistry of extracted solutions and rock residues were measured with ICP-MS and XRF, respectively. According to the results of XRF, considerable amounts of calcium and iron can be extracted by BCR procedures but other cations are negligible. In general, shale has a higher capacity of CO2 sequestration than sandstone. The first stage of extraction can release about 6 (sandstone) to 18.5 (shale) g of calcium from 1 kg rock, which are equivalent to 6.6 and 20.4 g CO2/kg rock, respectively. In the second stage extraction, 0.71 (sandstone) to 1.38 (shale) g/kg rock of iron can be released and can mineralized 0.56 to 1.08 g CO2/kg rock. However, there are no considerable cations extracted in the third stage of BCR as shown by the XRF analysis. In addition, the results of ICP-MS show that Mg can be released in the order of 10-3 g from 1 kg rock while cations of Zn, Co, Ni, Cd, Pb, Cu and Ba are in the order of 10-4 g.

Mechanisms of Soil Carbon Sequestration

NASA Astrophysics Data System (ADS)

Lal, Rattan

2015-04-01

Carbon (C) sequestration in soil is one of the several strategies of reducing the net emission of CO2 into the atmosphere. Of the two components, soil organic C (SOC) and soil inorganic C (SIC), SOC is an important control of edaphic properties and processes. In addition to off-setting part of the anthropogenic emissions, enhancing SOC concentration to above the threshold level (~1.5-2.0%) in the root zone has numerous ancillary benefits including food and nutritional security, biodiversity, water quality, among others. Because of its critical importance in human wellbeing and nature conservancy, scientific processes must be sufficiently understood with regards to: i) the potential attainable, and actual sink capacity of SOC and SIC, ii) permanence of the C sequestered its turnover and mean residence time, iii) the amount of biomass C needed (Mg/ha/yr) to maintain and enhance SOC pool, and to create a positive C budget, iv) factors governing the depth distribution of SOC, v) physical, chemical and biological mechanisms affecting the rate of decomposition by biotic and abiotic processes, vi) role of soil aggregation in sequestration and protection of SOC and SIC pool, vii) the importance of root system and its exudates in transfer of biomass-C into the SOC pools, viii) significance of biogenic processes in formation of secondary carbonates, ix) the role of dissolved organic C (DOC) in sequestration of SOC and SIC, and x) importance of weathering of alumino-silicates (e.g., powered olivine) in SIC sequestration. Lack of understanding of these and other basic processes leads to misunderstanding, inconsistencies in interpretation of empirical data, and futile debates. Identification of site-specific management practices is also facilitated by understanding of the basic processes of sequestration of SOC and SIC. Sustainable intensification of agroecosystems -- producing more from less by enhancing the use efficiency and reducing losses of inputs, necessitates thorough understanding of the processes, factors and causes of SOC and SIC dynamics in soils of natural and managed ecosystems.

Geophysical monitoring technology for CO2 sequestration

NASA Astrophysics Data System (ADS)

Ma, Jin-Feng; Li, Lin; Wang, Hao-Fan; Tan, Ming-You; Cui, Shi-Ling; Zhang, Yun-Yin; Qu, Zhi-Peng; Jia, Ling-Yun; Zhang, Shu-Hai

2016-06-01

Geophysical techniques play key roles in the measuring, monitoring, and verifying the safety of CO2 sequestration and in identifying the efficiency of CO2-enhanced oil recovery. Although geophysical monitoring techniques for CO2 sequestration have grown out of conventional oil and gas geophysical exploration techniques, it takes a long time to conduct geophysical monitoring, and there are many barriers and challenges. In this paper, with the initial objective of performing CO2 sequestration, we studied the geophysical tasks associated with evaluating geological storage sites and monitoring CO2 sequestration. Based on our review of the scope of geophysical monitoring techniques and our experience in domestic and international carbon capture and sequestration projects, we analyzed the inherent difficulties and our experiences in geophysical monitoring techniques, especially, with respect to 4D seismic acquisition, processing, and interpretation.

Potential for iron oxides to control metal releases in CO2 sequestration scenarios

USGS Publications Warehouse

Berger, P.M.; Roy, W.R.

2011-01-01

The potential for the release of metals into groundwater following the injection of carbon dioxide (CO2) into the subsurface during carbon sequestration projects remains an open research question. Changing the chemical composition of even the relatively deep formation brines during CO2 injection and storage may be of concern because of the recognized risks associated with the limited potential for leakage of CO2-impacted brine to the surface. Geochemical modeling allows for proactive evaluation of site geochemistry before CO2 injection takes place to predict whether the release of metals from iron oxides may occur in the reservoir. Geochemical modeling can also help evaluate potential changes in shallow aquifers were CO2 leakage to occur near the surface. In this study, we created three batch-reaction models that simulate chemical changes in groundwater resulting from the introduction of CO2 at two carbon sequestration sites operated by the Midwest Geological Sequestration Consortium (MGSC). In each of these models, we input the chemical composition of groundwater samples into React??, and equilibrated them with selected mineral phases and CO 2 at reservoir pressure and temperature. The model then simulated the kinetic reactions with other mineral phases over a period of up to 100 years. For two of the simulations, the water was also at equilibrium with iron oxide surface complexes. The first model simulated a recently completed enhanced oil recovery (EOR) project in south-central Illinois in which the MGSC injected into, and then produced CO2, from a sandstone oil reservoir. The MGSC afterwards periodically measured the brine chemistry from several wells in the reservoir for approximately two years. The sandstone contains a relatively small amount of iron oxide, and the batch simulation for the injection process showed detectable changes in several aqueous species that were attributable to changes in surface complexation sites. After using the batch reaction configuration to match measured geochemical changes due to CO2 injection, we modeled potential changes in groundwater chemistry at the Illinois Basin - Decatur Project (IBDP) site in Decatur, Illinois, USA. At the IBDP, the MGSC will inject 1 million tonnes of CO2 over the course of three years at a depth of about 2 km below the surface into the Mt. Simon Formation. Sections of the Mt. Simon Formation contain up to 10 percent iron oxide, and therefore surface complexes on iron oxides should play a major role in controlling brine chemistry. The batch simulation of this system showed a significant decrease in pH after the injection of CO2 with corresponding changes in brine chemistry resulting from both mineral precipitation/dissolution reactions and changes in the chemistry on iron oxide surfaces. To ensure the safety of shallow drinking water sources, there are several shallow monitoring wells at the IBDP that the MGSC samples regularly to determine baseline chemical concentrations. Knowing what geochemical parameters are most sensitive to CO2 disturbances allows us to focus monitoring efforts. Modeling a major influx of CO2 into the shallow groundwater allowed us to determine that were an introduction of CO2 to occur, the only immediate effect will be dolomite dissolution and calcite precipitation. ?? 2011 Published by Elsevier Ltd.

Zinc isotope and transition-element dynamics accompanying hydrozincite biomineralization in the Rio Naracauli, Sardinia, Italy

USGS Publications Warehouse

Wanty, Richard B.; Podda, F.; De Giudici, Giovanni; Cidu, R.; Lattanzi, Pierfranco

2013-01-01

The Rio Naracauli in SW Sardinia drains part of the Ingurtosu Zn–Pb mining district, and contains extreme concentrations of dissolved Zn at near-neutral pH. In the upper reaches of the stream, pH, alkalinity and Zn concentrations are such that hydrozincite [Zn5(CO3)2(OH)6] precipitates in a biologically mediated process facilitated by a microalga (Chlorella sp.) and a cyanobacterium (Scytonema sp.). Values of δ66Zn in water and solid samples ranged from − 0.35‰ to + 0.5‰ relative to the JMC 3-0749-Lyon standard, and closely follow a mass-dependent fractionation line. Two composite samples of sphalerite, the primary ore mineral in the Ingurtosu deposits, had an average δ66Zn of + 0.15‰, similar to sphalerite measured elsewhere in hydrothermal mineral deposits. Zinc isotope measurements of the stream water and the hydrozincite forming in the stream show a consistent preference for the heavy isotope, 66Zn, in the hydrozincite relative to 64Zn. Synthetic hydrozincites produced without added bacteria have δ66Zn identical to the dissolved Zn, thus suggesting a biologically mediated mineralization process in Rio Naracauli. The average fractionation, Δhdz-water, is 0.35‰, the magnitude of which is consistent with other studies, and suggests an extracellular mechanism of the biomineralization process. Zinc concentration and dissolved δ66Zn steadily decrease in the reach of the stream where the biomineralization occurs. The biomineralization process also leads to the sequestration of Pb, Cu and Ni in the hydrozincite lattice, and the coeval precipitation of an amorphous CdCO3 solid, prompting the suggestion that if optimized, the biomineralization process might represent a feasible passive remediation strategy for streams with high Zn and other metals, and with near-neutral pH.

Investigation of Mineral Transformations in Wet Supercritical CO2 by Electron Microscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arey, Bruce W.; Kovarik, Libor; Wang, Zheming

2011-10-10

The capture and storage of carbon dioxide and other greenhouse gases in deep geologic formations represents one of the most promising options for mitigating the impacts of greenhouse gases on global warming. In this regard, mineral-fluid interactions are of prime importance since such reactions can result in the long term sequestration of CO2 by trapping in mineral phases. Recently it has been recognized that interactions with neat to water-saturated non-aqueous fluids are of prime importance in understanding mineralization reactions since the introduced CO2 is likely to contain water initially or soon after injection and the supercritical CO2 (scCO2) is lessmore » dense than the aqueous phase which can result in a buoyant scCO2 plume contacting the isolating caprock. As a result, unraveling the molecular/microscopic mechanisms of mineral transformation in neat to water saturated scCO2 has taken on an added important. In this study, we are examining the interfacial reactions of the olivine mineral forsterite (Mg2SiO4) over a range of water contents up to and including complete water saturation in scCO2. The surface precipitates that form on the reacted forsterite grains are extremely fragile and difficult to experimentally characterize. In order to address this issue we have developed experimental protocols for preparing and imaging electron-transparent samples from fragile structures. These electron-transparent samples are then examined using a combination of STEM/EDX, FIB-TEM, and helium ion microscope (HIM) imaging (Figures 1-3). This combination of capabilities has provided unique insight into the geochemical processes that occur on scCO2 reacted mineral surfaces. The experimental procedures and protocols that have been developed also have useful applications for examining fragile structures on a wide variety of materials. This research was performed using EMSL, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research located at Pacific Northwest National Laboratory.« less

Climate change consequences for terrestrial ecosystem processes in NW Greeland: Results from the High Arctic Biocomplexity project

NASA Astrophysics Data System (ADS)

Welker, J. M.; Sullivan, P.; Rogers, M.; Sharp, E. D.; Sletten, R.; Burnham, J. L.; Hallet, B.; Hagedorn, B.; Czimiczk, C.

2009-12-01

Greenland is experiencing some of the fastest rates of climate warming across the Arctic including warmer summers and increases in snow fall. The effects of these new states of Greenland are however, uncertain especially for carbon, nitrogen and water biogeochemical processes, soil traits, vegetation growth patterns, mineral nutrition and plant ecophysiological processes. Since 2003 we have conducted a suite of observational and experimental measurements that have been designed to understand the fundamental nature of polar desert, polar semi-desert and fen landscapes in NW Greenland. In addition, we have established a suite of experiments to ascertain ecosystem responses to warming at multiple levels (~2030 and 2050), in conjunction with added summer rain; the consequences of added snow fall (ambient, intermediate and deep) and the effects of increases in nutrient additions (added N, P and N+P), which represent extreme warming conditions. We find that: a) the soil C pools are 6-fold larger than previously measured, b) extremely old C (up to ~30k bp) which has been buried by frost cracking and frost heaving is reaching the modern atmosphere, but in only trace amounts as measured by respired 14CO2, c) warming that simulates 2030, has only a small effect on net C sequestration but warming that simulates 2050 when combined with added summer rain, increases C sequestration by 300%, d) increases in N deposition almost immediately and completely changes the vegetation composition of polar semi-deserts shifting the NDVI values from 0.2 to 0.5 within 2 years. Our findings depict a system that is poised to contribute stronger feedbacks than previously expected as climates in NW Greenland change.

A mechanistic understanding of plagioclase dissolution based on Al occupancy and T-O bond length: from geologic carbon sequestration to ambient conditions.

PubMed

Yang, Yi; Min, Yujia; Jun, Young-Shin

2013-11-14

A quantitative description of how the bulk properties of aluminosilicates affect their dissolution kinetics is important in helping people understand the regulation of atmospheric CO2 concentration by silicate weathering and predict the fate and transport of geologically sequestered CO2 through brine-rock interactions. In this study, we employed a structure model based on the C1 space group to illustrate how differences in crystallographic properties of aluminosilicates, such as T-O (Tetrahedral site-Oxygen) bond length and Al/Si ordering, can result in quantifiable variations in mineral dissolution rates. The dissolution rates of plagioclases were measured under representative geologic carbon sequestration (GCS) conditions (90 °C, 100 atm of CO2, 1.0 M NaCl, and pH ∼ 3.1), and used to validate the model. We found that the logarithm of the characteristic time of the breakdown of Al-O-Si linkages in plagioclases follows a good linear relation with the mineral's aluminum content (nAl). The Si release rates of plagioclases can be calculated based on an assumption of dissolution congruency or on the regularity of Al/Si distribution in the constituent tetrahedra of the mineral. We further extended the application of our approach to scenarios where dissolution incongruency arises because of different linkage reactivities in the solid matrix, and compared the model predictions with published data. The application of our results enables a significant reduction of experimental work for determining the dissolution rates of structurally related aluminosilicates, given a reaction environment.

[Priming effect of biochar on the minerialization of native soil organic carbon and the mechanisms: A review.

PubMed

Chen, Ying; Liu, Yu Xue; Chen, Chong Jun; Lyu, Hao Hao; Wa, Yu Ying; He, Li Li; Yang, Sheng Mao

2018-01-01

In recent years, studies on carbon sequestration of biochar in soil has been in spotlight owing to the specific characteristics of biochar such as strong carbon stability and well developed pore structure. However, whether biochar will ultimately increase soil carbon storage or promote soil carbon emissions when applied into the soil? This question remains controversial in current academic circles. Further research is required on priming effect of biochar on mineralization of native soil organic carbon and its mechanisms. Based on the analysis of biochar characteristics, such as its carbon composition and stability, pore structure and surface morphology, research progress on the priming effect of biochar on the decomposition of native soil organic carbon was reviewed in this paper. Furthermore, possible mechanisms of both positive and negative priming effect, that is promoting and suppressing the mineralization, were put forward. Positive priming effect is mainly due to the promotion of soil microbial activity caused by biochar, the preferential mineralization of easily decomposed components in biochar, and the co-metabolism of soil microbes. While negative priming effect is mainly based on the encapsulation and adsorption protection of soil organic matter due to the internal pore structure and the external surface of biochar. Other potential reasons for negative priming effect can be the stabilization resulted from the formation of organic-inorganic complex promoted by biochar in the soil, and the inhibition of activity of soil microbes and its enzymes by biochar. Finally, future research directions were proposed in order to provide theoretical basis for the application of biochar in soil carbon sequestration.

CO2 mineral sequestration in oil-shale wastes from Estonian power production.

PubMed

Uibu, Mai; Uus, Mati; Kuusik, Rein

2009-02-01

In the Republic of Estonia, local low-grade carbonaceous fossil fuel--Estonian oil-shale--is used as a primary energy source. Combustion of oil-shale is characterized by a high specific carbon emission factor (CEF). In Estonia, the power sector is the largest CO(2) emitter and is also a source of huge amounts of waste ash. Oil-shale has been burned by pulverized firing (PF) since 1959 and in circulating fluidized-bed combustors (CFBCs) since 2004-2005. Depending on the combustion technology, the ash contains a total of up to 30% free Ca-Mg oxides. In consequence, some amount of emitted CO(2) is bound by alkaline transportation water and by the ash during hydraulic transportation and open-air deposition. The goal of this study was to investigate the possibility of improving the extent of CO(2) capture using additional chemical and technological means, in particular the treatment of aqueous ash suspensions with model flue gases containing 10-15% CO(2). The results indicated that both types of ash (PF and CFBC) could be used as sorbents for CO(2) mineral sequestration. The amount of CO(2) captured averaged 60-65% of the carbonaceous CO(2) and 10-11% of the total CO(2) emissions.

Quantification of Cation Sorption to Engineered Barrier Materials Under Extreme Conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Powell, Brian; Schlautman, Mark; Rao, Linfeng

The objective of this research is to examine mechanisms and thermodynamics of actinide sorption to engineered barrier materials (iron (oxyhydr)oxides and bentonite clay) for nuclear waste repositories under high temperature and high ionic strength conditions using a suite of macroscopic and microscopic techniques which will be coupled with interfacial reaction models. Gaining a mechanistic understanding of interfacial processes governing the sorption/sequestration of actinides at mineral-water interfaces is fundamental for the accurate prediction of actinide behavior in waste repositories. Although macroscale sorption data and various spectroscopic techniques have provided valuable information regarding speciation of actinides at solid-water interfaces, significant knowledge gapsmore » still exist with respect to sorption mechanisms and the ability to quantify sorption, particularly at high temperatures and ionic strengths. This objective is addressed through three major tasks: (1) influence of oxidation state on actinide sorption to iron oxides and clay minerals at elevated temperatures and ionic strengths; (2) calorimetric titrations of actinide-mineral suspensions; (3) evaluation of bentonite performance under repository conditions. The results of the work will include a qualitative conceptual model and a quantitative thermodynamic speciation model describing actinide partitioning to minerals and sediments, which is based upon a mechanistic understanding of specific sorption processes as determined from both micro-scale and macroscale experimental techniques. The speciation model will be a thermodynamic aqueous and surface complexation model of actinide interactions with mineral surfaces that is self-consistent with macroscopic batch sorption data, calorimetric and potentiometric titrations, X-ray absorption Spectroscopy (XAS, mainly Extended X-ray Absorption Fine Structure (EXAFS)), and electron microscopy analyses. The novelty of the proposed work lies largely in the unique system conditions which will be examined (i.e. elevated temperature and ionic strength) and the manner in which the surface complexation model will be developed in terms of specific surface species identified using XAS. These experiments will thus provide a fundamental understanding of the chemical and physical processes occurring at the solid-solution interface under expected repository conditions. Additionally, the focus on thermodynamic treatment of actinide ion interactions with minerals as proposed will provide information on the driving forces involved and contribute to the overall understanding of the high affinity many actinide ions have for oxide surfaces. The utility of this model will be demonstrated in this work through a series of advective and diffusive flow experiments.« less

Comparative Toxicities of Salts on Microbial Processes in Soil

PubMed Central

Maheshwari, Arpita; Bengtson, Per; Rousk, Johannes

2016-01-01

Soil salinization is a growing threat to global agriculture and carbon sequestration, but to date it remains unclear how microbial processes will respond. We studied the acute response to salt exposure of a range of anabolic and catabolic microbial processes, including bacterial (leucine incorporation) and fungal (acetate incorporation into ergosterol) growth rates, respiration, and gross N mineralization and nitrification rates. To distinguish effects of specific ions from those of overall ionic strength, we compared the addition of four salts frequently associated with soil salinization (NaCl, KCl, Na2SO4, and K2SO4) to a nonsaline soil. To compare the tolerance of different microbial processes to salt and to interrelate the toxicity of different salts, concentration-response relationships were established. Growth-based measurements revealed that fungi were more resistant to salt exposure than bacteria. Effects by salt on C and N mineralization were indistinguishable, and in contrast to previous studies, nitrification was not found to be more sensitive to salt exposure than other microbial processes. The ion-specific toxicity of certain salts could be observed only for respiration, which was less inhibited by salts containing SO42− than Cl− salts, in contrast to the microbial growth assessments. This suggested that the inhibition of microbial growth was explained solely by total ionic strength, while ion-specific toxicity also should be considered for effects on microbial decomposition. This difference resulted in an apparent reduction of microbial growth efficiency in response to exposure to SO42− salts but not to Cl− salts; no evidence was found to distinguish K+ and Na+ salts. PMID:26801570

Slowing the rate of loss of mineral wetlands on human dominated landscapes - Diversification of farmers markets to include carbon (Invited)

NASA Astrophysics Data System (ADS)

Creed, I. F.; Badiou, P.; Lobb, D.

2013-12-01

Canada is the fourth-largest exporter of agriculture and agri-food products in the world (exports valued at 28B), but instability of agriculture markets can make it difficult for farmers to cope with variability, and new mechanisms are needed for farmers to achieve economic stability. Capitalizing on carbon markets will help farmers achieve environmentally sustainable economic performance. In order to have a viable carbon market, governments and industries need to know what the carbon capital is and what potential there is for growth, and farmers need financial incentives that will not only allow them to conserve existing wetlands but that will also enable them to restore wetlands while making a living. In southern Ontario, farmers' needs to maximize the return on investment on marginal lands have resulted in loss of 70-90% of wetlands, making this region one of the most threatened region in terms of wetland degradation and loss in Canada. Our project establishes the role that mineral wetlands have in the net carbon balance by contributing insight into the potential benefits to carbon management provided by wetland restoration efforts in these highly degraded landscapes. The goal was to establish the magnitude of carbon offsets that could be achieved through wetland conservation (securing existing carbon stocks) and restoration (creating new carbon stocks). The experimental design was to focus on (1) small (0.2-2.0 ha) and (2) isolated (no inflow or outflow) mineral wetlands with the greatest restoration potential that included (3) a range of restoration ages (drained (0 yr), 3 yr, 6 yr, 12 yr, 20 yr, 35 yr, intact marshes) to capture potential changes in rates of carbon sequestration with restoration age of wetland. From each wetland, wetland soil carbon pools samples were collected at four positions: centre of wetland (open-water); emergent vegetation zone; wet meadow zone where flooding often occurs (i.e., high water mark); and upland where flooding rarely occurs (cores segmented into 5cm increments up to 45 cm, composited and analyzed for carbon pools using mass equivalent and carbon sequestration rates samples were taken at centre of wetland (open-water) (cores segmented into 1 cm increments up to 30 cm, composited and analyzed for Pb-210 and Cs-137 isotopes). The magnitude of wetland loss (≥10 ha) is estimated to be over 1.5 million ha in southern Ontario since the time of European settlement. About 75% of converted wetlands (1.1 million ha) are now classified as 'undifferentiated agricultural lands.' We use our measured carbon sequestration rate Mg CO2 equivalents ha/yr under different scenarios of landowner uptake (5-50%) and prices for carbon offsets (2-50/MgCO2 equivalents) to estimate carbon sequestration and the value of this sequestration in restored wetlands. The project provides empirical evidence that restoring wetlands for carbon sequence could improve the livelihood of farmers and that policies should be established to incentivize farmers to adopt wetland restoration practices on marginal areas in order to improve the economic performance and environmental sustainability of agriculture in Ontario.

Artificial Weathering as a Function of CO2 Injection in Pahang Sandstone Malaysia: Investigation of Dissolution Rate in Surficial Condition

PubMed Central

Jalilavi, Madjid; Zoveidavianpoor, Mansoor; Attarhamed, Farshid; Junin, Radzuan; Mohsin, Rahmat

2014-01-01

Formation of carbonate minerals by CO2 sequestration is a potential means to reduce atmospheric CO2 emissions. Vast amount of alkaline and alkali earth metals exist in silicate minerals that may be carbonated. Laboratory experiments carried out to study the dissolution rate in Pahang Sandstone, Malaysia, by CO2 injection at different flow rate in surficial condition. X-ray Powder Diffraction (XRD), Scanning Electron Microscope (SEM) with Energy Dispersive X-ray Spectroscopy (EDX), Atomic Absorption Spectroscopy (AAS) and weight losses measurement were performed to analyze the solid and liquid phase before and after the reaction process. The weight changes and mineral dissolution caused by CO2 injection for two hours CO2 bubbling and one week' aging were 0.28% and 18.74%, respectively. The average variation of concentrations of alkaline earth metals in solution varied from 22.62% for Ca2+ to 17.42% for Mg2+, with in between 16.18% observed for the alkali earth metal, potassium. Analysis of variance (ANOVA) test is performed to determine significant differences of the element concentration, including Ca, Mg, and K, before and after the reaction experiment. Such changes show that the deposition of alkali and alkaline earth metals and the dissolution of required elements in sandstone samples are enhanced by CO2 injection. PMID:24413195

OpenGeoSys: An Open-Source Initiative for Numerical Simulation of Thermo-Hydro-Mechanical/Chemical (THM/C) Processes in Porous Media

NASA Astrophysics Data System (ADS)

Watanabe, N.; Bilke, L.; Fischer, T.; Kalbacher, T.; Nagel, T.; Naumov, D.; Rink, K.; Shao, H.; Wang, W.; Kolditz, O.

2014-12-01

The current understanding of geochemical reactions in reservoirs for geological carbon sequestration (GCS) is largely based on aqueous chemistry (CO2 dissolves in reservoir brine and brine reacts with rocks). However, only a portion of the injected supercritical (sc) CO2 dissolves before the buoyant plume contacts caprock, where it is expected to reside for a long time. Although numerous studies have addressed scCO2-mineral reactions occurring within adsorbed aqueous films, possible reactions resulting from direct CO2-rock contact remain less understood. Does CO2 as a supercritical phase react with reservoir rocks? Do mineral react differently with scCO2 than with dissolved CO2? We selected muscovite, one of the more stable and common rock-forming silicate minerals, to react with scCO2 phase (both water-saturated and water-free) and compared with CO2-saturated-brine. The reacted basal surfaces were analyzed using atomic force microscopy and X-ray photoelectron spectroscopy for examining the changes in surface morphology and chemistry. The results show that scCO2 (regardless of its water content) altered muscovite considerably more than CO2-saturated brine; suggest CO2 diffusion into mica interlayers and localized mica dissolution into scCO2 phase. The mechanisms underlying these observations and their implications for GCS need further exploration.

Artificial weathering as a function of CO2 injection in Pahang Sandstone Malaysia: investigation of dissolution rate in surficial condition.

PubMed

Jalilavi, Madjid; Zoveidavianpoor, Mansoor; Attarhamed, Farshid; Junin, Radzuan; Mohsin, Rahmat

2014-01-13

Formation of carbonate minerals by CO2 sequestration is a potential means to reduce atmospheric CO2 emissions. Vast amount of alkaline and alkali earth metals exist in silicate minerals that may be carbonated. Laboratory experiments carried out to study the dissolution rate in Pahang Sandstone, Malaysia, by CO2 injection at different flow rate in surficial condition. X-ray Powder Diffraction (XRD), Scanning Electron Microscope (SEM) with Energy Dispersive X-ray Spectroscopy (EDX), Atomic Absorption Spectroscopy (AAS) and weight losses measurement were performed to analyze the solid and liquid phase before and after the reaction process. The weight changes and mineral dissolution caused by CO2 injection for two hours CO2 bubbling and one week' aging were 0.28% and 18.74%, respectively. The average variation of concentrations of alkaline earth metals in solution varied from 22.62% for Ca(2+) to 17.42% for Mg(2+), with in between 16.18% observed for the alkali earth metal, potassium. Analysis of variance (ANOVA) test is performed to determine significant differences of the element concentration, including Ca, Mg, and K, before and after the reaction experiment. Such changes show that the deposition of alkali and alkaline earth metals and the dissolution of required elements in sandstone samples are enhanced by CO2 injection.

Organic nitrogen storage in mineral soil: Implications for policy and management.

PubMed

Bingham, Andrew H; Cotrufo, M Francesca

2016-05-01

Nitrogen is one of the most important ecosystem nutrients and often its availability limits net primary production as well as stabilization of soil organic matter. The long-term storage of nitrogen-containing organic matter in soils was classically attributed to chemical complexity of plant and microbial residues that retarded microbial degradation. Recent advances have revised this framework, with the understanding that persistent soil organic matter consists largely of chemically labile, microbially processed organic compounds. Chemical bonding to minerals and physical protection in aggregates are more important to long-term (i.e., centuries to millennia) preservation of these organic compounds that contain the bulk of soil nitrogen rather than molecular complexity, with the exception of nitrogen in pyrogenic organic matter. This review examines for the first time the factors and mechanisms at each stage of movement into long-term storage that influence the sequestration of organic nitrogen in the mineral soil of natural temperate ecosystems. Because the factors which govern persistence are different under this newly accepted paradigm we examine the policy and management implications that are altered, such as critical load considerations, nitrogen saturation and mitigation consequences. Finally, it emphasizes how essential it is for this important but underappreciated pool to be better quantified and incorporated into policy and management decisions, especially given the lack of evidence for many soils having a finite capacity to sequester nitrogen. Published by Elsevier B.V.

Artificial Weathering as a Function of CO2 Injection in Pahang Sandstone Malaysia: Investigation of Dissolution Rate in Surficial Condition

NASA Astrophysics Data System (ADS)

Jalilavi, Madjid; Zoveidavianpoor, Mansoor; Attarhamed, Farshid; Junin, Radzuan; Mohsin, Rahmat

2014-01-01

Formation of carbonate minerals by CO2 sequestration is a potential means to reduce atmospheric CO2 emissions. Vast amount of alkaline and alkali earth metals exist in silicate minerals that may be carbonated. Laboratory experiments carried out to study the dissolution rate in Pahang Sandstone, Malaysia, by CO2 injection at different flow rate in surficial condition. X-ray Powder Diffraction (XRD), Scanning Electron Microscope (SEM) with Energy Dispersive X-ray Spectroscopy (EDX), Atomic Absorption Spectroscopy (AAS) and weight losses measurement were performed to analyze the solid and liquid phase before and after the reaction process. The weight changes and mineral dissolution caused by CO2 injection for two hours CO2 bubbling and one week' aging were 0.28% and 18.74%, respectively. The average variation of concentrations of alkaline earth metals in solution varied from 22.62% for Ca2+ to 17.42% for Mg2+, with in between 16.18% observed for the alkali earth metal, potassium. Analysis of variance (ANOVA) test is performed to determine significant differences of the element concentration, including Ca, Mg, and K, before and after the reaction experiment. Such changes show that the deposition of alkali and alkaline earth metals and the dissolution of required elements in sandstone samples are enhanced by CO2 injection.

In-situ Optical Spectroscopy Investigation of Water and Its influence on Forsterite Transformation in Supercritical CO2

NASA Astrophysics Data System (ADS)

Wang, Z.; Thompson, C. J.; Joly, A. G.; Sklarew, D. S.; Poindexter, L.; Rosso, K. M.

2009-12-01

Carbon capture and sequestration (CCS) from coal/gas-burning power plants is currently viewed as one of the most promising technologies for mitigating green house gas emissions. This strategy involves injection of supercritical CO2 (scCO2) into deep geological formations such as depleted oil and gas reservoirs and deep saline aquifers. The feasibility of this approach and the ultimate fate of the stored CO2 are determined by the interactions between scCO2, various minerals in the rock formations, and the host fluids. Currently, there is only limited knowledge about both the thermodynamic and kinetic aspects of the physical and chemical processes that occur between scCO2 and relevant minerals, such as metal silicates and metal aluminosilicates, and the role of water activity for catalyzing mineral transformation reactions. In this work, we have developed a modular in situ optical spectroscopic platform that integrates a scCO2 generation and manipulation system with an array of optical and laser spectroscopies including UV-visible, IR, Raman and laser fluorescence spectroscopy. We have used the system to study i) the dissolution and quantification of H2O/D2O in scCO2 and ii) interaction between scCO2 and a model metal silicate, forsterite (Mg2SiO4), and the effects of the presence of water under variable pressure, temperature and water content. Our results showed that H2O and D2O have unique IR spectral features over a broad spectral range from 700 cm-1 to ~ 2900 cm-1 in scCO2 and their concentrations are directly proportional to the characteristic IR bands that correspond to their stretching (D2O) and bending frequencies (both D2O and H2O). These bands offer a unique spectroscopic signature useful for qualitative and quantitative analysis of the properties and reactivity of small amounts of H2O in scCO2.

Nitrogen deposition and soil carbon sequestration: enzymes, experiments, and model estimates (Invited)

NASA Astrophysics Data System (ADS)

Goodale, C. L.; Weiss, M.; Tonitto, C.; Stone, M.

2010-12-01

Atmospheric nitrogen has long been expected to increase forest carbon sequestration, by means of enhanced productivity and litter production. More recently, N deposition has received attention for its potential for inducing soil C sequestration by suppressing microbial decomposition. Here, we present a range of measurements and model projections of the effects of N additions on soil C dynamics in forest soils of the northeastern U.S. A review of field-scale measurements of soil C stocks suggests modest enhancements of soil C storage in long-term N addition studies. Measurements of forest floor material from six long-term N addition studies showed that N additions suppressed microbial biomass and oxidative enzyme activity across sites. Additional analyses on soils from two of these sites are exploring the interactive effects of temperature and N addition on the activity of a range of extracellular enzymes used for decomposition of a range of organic matter. Incubations of forest floor material from four of these sites showed inhibition of heterotrophic respiration by an average of 28% during the first week of incubation, although this inhibition disappeared after 2 to 11 months. Nitrogen additions had no significant effect on DOC loss or on the partitioning of soil C into light or heavy (mineral-associated) organic matter. Last, we have adapted a new model of soil organic matter decomposition for the PnET-CN model to assess the long-term impact of suppressed decomposition on C sequestration in various soil C pools.

Geologic CO2 Sequestration: Predicting and Confirming Performance in Oil Reservoirs and Saline Aquifers

NASA Astrophysics Data System (ADS)

Johnson, J. W.; Nitao, J. J.; Newmark, R. L.; Kirkendall, B. A.; Nimz, G. J.; Knauss, K. G.; Ziagos, J. P.

2002-05-01

Reducing anthropogenic CO2 emissions ranks high among the grand scientific challenges of this century. In the near-term, significant reductions can only be achieved through innovative sequestration strategies that prevent atmospheric release of large-scale CO2 waste streams. Among such strategies, injection into confined geologic formations represents arguably the most promising alternative; and among potential geologic storage sites, oil reservoirs and saline aquifers represent the most attractive targets. Oil reservoirs offer a unique "win-win" approach because CO2 flooding is an effective technique of enhanced oil recovery (EOR), while saline aquifers offer immense storage capacity and widespread distribution. Although CO2-flood EOR has been widely used in the Permian Basin and elsewhere since the 1980s, the oil industry has just recently become concerned with the significant fraction of injected CO2 that eludes recycling and is therefore sequestered. This "lost" CO2 now has potential economic value in the growing emissions credit market; hence, the industry's emerging interest in recasting CO2 floods as co-optimized EOR/sequestration projects. The world's first saline aquifer storage project was also catalyzed in part by economics: Norway's newly imposed atmospheric emissions tax, which spurred development of Statoil's unique North Sea Sleipner facility in 1996. Successful implementation of geologic sequestration projects hinges on development of advanced predictive models and a diverse set of remote sensing, in situ sampling, and experimental techniques. The models are needed to design and forecast long-term sequestration performance; the monitoring techniques are required to confirm and refine model predictions and to ensure compliance with environmental regulations. We have developed a unique reactive transport modeling capability for predicting sequestration performance in saline aquifers, and used it to simulate CO2 injection at Sleipner; we are now extending this capability to address CO2-flood EOR/sequestration in oil reservoirs. We have also developed a suite of innovative geophysical and geochemical techniques for monitoring sequestration performance in both settings. These include electromagnetic induction imaging and electrical resistance tomography for tracking migration of immiscible CO2, noble gas isotopes for assessing trace CO2 leakage through the cap rock, and integrated geochemical sampling, analytical, and experimental methods for determining sequestration partitioning among solubility and mineral trapping mechanisms. We have proposed to demonstrate feasibility of the co-optimized EOR/sequestration concept and utility of our modeling and monitoring technologies to design and evaluate its implementation by conducting a demonstration project in the Livermore Oil Field. This small, mature, shallow field, located less than a mile east of Lawrence Livermore National Laboratory, is representative of many potential EOR/sequestration sites in California. In approach, this proposed demonstration is analogous to the Weyburn EOR/CO2 monitoring project, to which it will provide an important complement by virtue of its contrasting depth (immiscible versus Weyburn's miscible CO2 flood) and geologic setting (clay-capped sand versus Weyburn's anhydrite-capped carbonate reservoir).

A Novel Approach to Experimental Studies of Mineral Dissolution Kinetics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen Zhu

2006-08-31

Currently, DOE is conducting pilot CO{sub 2} injection tests to evaluate the concept of geological sequestration. One strategy that potentially enhances CO{sub 2} solubility and reduces the risk of CO{sub 2} leak back to the surface is dissolution of indigenous minerals in the geological formation and precipitation of secondary carbonate phases, which increases the brine pH and immobilizes CO{sub 2}. Clearly, the rates at which these dissolution and precipitation reactions occur directly determine the efficiency of this strategy. However, one of the fundamental problems in modern geochemistry is the persistent two to five orders of magnitude discrepancy between laboratory measuredmore » and field derived feldspar dissolution rates. To date, there is no real guidance as to how to predict silicate reaction rates for use in quantitative models. Current models for assessment of geological carbon sequestration have generally opted to use laboratory rates, in spite of the dearth of such data for compositionally complex systems, and the persistent disconnect between laboratory and field applications. Therefore, a firm scientific basis for predicting silicate reaction kinetics in CO2 injected geological formations is urgently needed to assure the reliability of the geochemical models used for the assessments of carbon sequestration strategies. The funded experimental and theoretical study attempts to resolve this outstanding scientific issue by novel experimental design and theoretical interpretation to measure silicate dissolution rates and iron carbonate precipitation rates at conditions pertinent to geological carbon sequestration. In the second year of the project, we completed CO{sub 2}-Navajo sandstone interaction batch and flow-through experiments and a Navajo sandstone dissolution experiment without the presence of CO{sub 2} at 200 C and 250-300 bars, and initiated dawsonite dissolution and solubility experiments. We also performed additional 5-day experiments at the same conditions as alkali-feldspar dissolution experiments with and without the presence of CO{sub 2} performed in the first year to check the validation of the experiments and analysis. The changes of solution chemistry as dissolution experiments progressed were monitored with on-line sampling of the aqueous phase at the constant temperature and pressure. These data allow calculating overall apparent mineral (feldspars and sandstones) dissolution rates and secondary mineral precipitation rates as a function of saturation states. State-of-the-art atomic resolution transmission electron microscopy (TEM), scanning electron microscopy (SEM), and electron microprobe was used to characterize the products and reactants. Reaction-path geochemical modeling was used to interpret the experimental results of alkali-feldspar dissolution experiments without the presence of CO{sub 2}. Two manuscripts are near completion. Also during the second year, our education goal of graduate student training has been advanced. A Ph. D. student at Indiana University is progressing well in the degree program and has taken geochemical modeling, SEM, and TEM courses, which will facilitate research in the third year. A Ph. D. student at University of Minnesota had graduated. With the success of training of graduate students and excellent experimental data in the second year, we anticipate a more fruitful year in the third year.« less

Mineral replacement reactions and element mobilization

NASA Astrophysics Data System (ADS)

Putnis, Christine V.; Ruiz-Agudo, Encarnacion; King, Helen E.; Hövelmann, Jörn; Renard, François

2016-04-01

When a mineral is out of equilibrium with an aqueous fluid, reactions will take place in an attempt to reach a new equilibrium. Commonly in the Earth dissolution at a mineral-fluid interface initiates a coupled reaction involving dissolution and precipitation (Ruiz-Agudo et al., 2014). This is a ubiquitous reaction during such processes as metamorphism, metasomatism and weathering. When rock-forming minerals such as feldspars, olivine, pyroxenes are in contact with aqueous fluids (typically NaCl-rich) resultant new phases are formed and elements present in the parent mineral are released to the fluid and therefore mobilized for transport elsewhere. This has been shown in a number of systems such as the albitisation of feldspars (Hövelmann et al., 2010) when a Ca-bearing plagioclase is replaced by albite (NaAlSi3O8). However during this reaction not only is Ca released to the fluid but most other minor elements, such as Mg, Pb, rare earth elements amongst others, are almost totally mobilized and removed in solution. This interface-coupled dissolution-precipitation reaction has many implications for the redistributon of elements in the crust of the Earth. It is also of note that albitisation occurs often in areas of high mineralization, such as in the Curnamona Province in S. Australia (Au-Cu and Ag-Pb-Zn deposits) and the Bamble District of S. Norway. Secondly atomic force microscopy (AFM) has been used to image these reactions at a nanoscale, especially at the calcite-fluid interface, such as the formation of apatite from phosphate-bearing solutions, and the sequestration of toxic elements, eg., Se and As. References Ruiz-Agudo E., Putnis C.V., Putnis A. (2014) Coupled dissolution and precipitation at mineral-fluid interfaces. Chemical Geology, 383, 132-146. Putnis C.V. and Ruiz-Agudo E. (2013) The mineral-water interface: where minerals react with the environment. Elements, 9, 177-182. Hövelmann J., Putnis A., Geisler T., Schmidt B.C., Golla-Schindler U. (2009) The replacement of plagioclase feldspars by albite: observations from hydrothermal experiments. Contrib. Min. and Pet. 159, 43-59.

Mica dust and pneumoconiosis: example of a pure occupational exposure in a muscovite milling unit.

PubMed

Hulo, Sébastien; Cherot-kornobis, Nathalie; Edme, Jean-Louis; de Broucker, Virginie; Falgayrac, Guillaume; Penel, Guillaume; Legrand-Cattan, Karinne; Remy, Jacques; Sobaszek, Annie

2013-12-01

We present pulmonary disorders of four employees who were exposed to high concentration of pure mica dust in a muscovite milling unit. All cases underwent traditional examinations with a dual-energy chest computed tomographic scan. An analysis of exhaled breath condensate by Raman microspectrometry and of mineralogical content of a lung biopsy was performed for one case. All cases showed bilateral micronodular ground glass opacities and mediastinal and hilar hyperdense lymph nodes consistent with the nodal sequestration of mineral particles. Histological analysis showed giant cell granulomas without typical silicotic nodule with high concentration of birefringent particles consistent with mica. Mica particles found in the exhaled breath condensate were identical to particles in ambient air at the company. Occupational exposure to mica dust is responsible for diffuse infiltrative lung disease by overload processes.

Novel Determination of the Orientation of Calcite on Mineral Substrates

NASA Astrophysics Data System (ADS)

Zhao, L.; Ji, X.; Teng, H.

2016-12-01

In the threat of global warming, the transformation from CO2 to stable carbonate minerals is significant to geological CO2 sequestration in the long term.Previous efforts have found that when carbonate minerals nucleate on some mineral substrates ,the time of carbon capture can be shorted .Many efforts have been focused on the dynamics when carbonate minerals nucleate on mineral substrates, but few have studied the orientation of carbonate minerals on mineral substrates. In our experiment, we mainly focused on the orientation of calcite on mineral substrates.We mixed NaHCO3 and CaCl2 to nucleate when mineral substrates were added and a multi-parameter analyzer was used to monitor in real time to determine the induction time for nucleation. On the basis of classical nucleation theory, we got a brand new formula to decide the orientation of calcite on mineral substrates. lntind=(2-cosθ+cos3θ)*16πγ3vm2(12*(kBT)3*(lnS)2)+ln(1/N0v)+ ΔEa/(kBT)where θ is the angle between the substrate and the nuclei, tind is the induction time for nucleation, γ is he average surface free energy, N0 is the total number of particles per unit volume of solution, ΔEa is the activation energy for molecular motion across the embryo-matrix interface, S is the supersaturation index ,kB is the Boltzmann constant. Using the new formula above , when biotite was used as substrate mineral ,we found that the angle between the biotite and the nuclei was 119°. Angle measured on SEM images also supported our conclusion above. Combined with SEM and Debye ring analysed by Rigaku 2D data processing software, we only found one point of (006) in Debye ring, unlike (104)(many points in one ring and it meant that the orientation of (104) is random ). That meant (001) of calcite was first formed on biotite (001). In that case we inferred that 119° was formed by (001) of botite and (012) of calcite for the intersection angle of (001) and (012) was 120°. Future research will focus on the orientation of calcite on muscovite and feldspar to find out the main influence factor of the contact relationship.

Fungal Bioweathering of Mimetite and a General Geomycological Model for Lead Apatite Mineral Biotransformations

PubMed Central

Ceci, Andrea; Kierans, Martin; Hillier, Stephen; Persiani, Anna Maria

2015-01-01

Fungi play important roles in biogeochemical processes such as organic matter decomposition, bioweathering of minerals and rocks, and metal transformations and therefore influence elemental cycles for essential and potentially toxic elements, e.g., P, S, Pb, and As. Arsenic is a potentially toxic metalloid for most organisms and naturally occurs in trace quantities in soil, rocks, water, air, and living organisms. Among more than 300 arsenic minerals occurring in nature, mimetite [Pb5(AsO4)3Cl] is the most stable lead arsenate and holds considerable promise in metal stabilization for in situ and ex situ sequestration and remediation through precipitation, as do other insoluble lead apatites, such as pyromorphite [Pb5(PO4)3Cl] and vanadinite [Pb5(VO4)3Cl]. Despite the insolubility of mimetite, the organic acid-producing soil fungus Aspergillus niger was able to solubilize mimetite with simultaneous precipitation of lead oxalate as a new mycogenic biomineral. Since fungal biotransformation of both pyromorphite and vanadinite has been previously documented, a new biogeochemical model for the biogenic transformation of lead apatites (mimetite, pyromorphite, and vanadinite) by fungi is hypothesized in this study by application of geochemical modeling together with experimental data. The models closely agreed with experimental data and provided accurate simulation of As and Pb complexation and biomineral formation dependent on, e.g., pH, cation-anion composition, and concentration. A general pattern for fungal biotransformation of lead apatite minerals is proposed, proving new understanding of ecological implications of the biogeochemical cycling of component elements as well as industrial applications in metal stabilization, bioremediation, and biorecovery. PMID:25979898

Impact of trace element additives on anaerobic digestion of sewage sludge with in-situ carbon dioxide sequestration

DOE Office of Scientific and Technical Information (OSTI.GOV)

Linville, Jessica L.; Shen, Yanwen; Schoene, Robin P.

Anaerobic digestion (AD) of sludge at wastewater treatment plants can benefit from addition of essential trace metals such as iron, nickel and cobalt to increase biogas production for utilization in combined heat and power systems, fed into natural gas pipelines or as a vehicle fuel. This study evaluated the impact and benefits of Ni/Co and olivine addition to the digester at mesophilic temperatures. These additions supplement previously reported research in which iron-rich olivine (MgSiO4) was added to sequester CO2 in-situ during batch AD of sludge. Trace element addition has been shown to stimulate and stabilize biogas production and have amore » synergistic effect on the mineral carbonation process. AD with 5% w/v olivine and 1.5 mg/L Ni/Co addition had a 17.3% increase in methane volume, a 6% increase in initial exponential methane production rate and a 56% increase in methane yield (mL CH4/g CODdegraded) compared to the control due to synergistic trace element and olivine addition while maintaining 17.7% CO2 sequestration from olivine addition. Both first-order kinetic modeling and response surface methodology modeling confirmed the combined benefit of the trace elements and olivine addition. These results were significantly higher than previously reported results with olivine addition alone [1].« less

CO 2 Mineral Sequestration in Naturally Porous Basalt

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xiong, Wei; Wells, Rachel K.; Horner, Jake A.

2018-02-27

Continental flood basalts are extensive geologic features currently being evaluated as reservoirs that are suitable for long-term storage of carbon emissions. Favorable attributes of these formations for containment of injected carbon dioxide (CO2) include high mineral trapping capacity, unique structural features, and enormous volumes. We experimentally investigated mineral carbonation in whole core samples retrieved from the Grand Ronde basalt, the same formation into which ~1000 t of CO2 was recently injected in an eastern Washington pilot-scale demonstration. The rate and extent of carbonate mineral formation at 100 °C and 100 bar were tracked via time-resolved sampling of bench-scale experiments. Basaltmore » cores were recovered from the reactor after 6, 20, and 40 weeks, and three-dimensional X-ray tomographic imaging of these cores detected carbonate mineral formation in the fracture network within 20 weeks. Under these conditions, a carbon mineral trapping rate of 1.24 ± 0.52 kg of CO2/m3 of basalt per year was estimated, which is orders of magnitude faster than rates for deep sandstone reservoirs. On the basis of these calculations and under certain assumptions, available pore space within the Grand Ronde basalt formation would completely carbonate in ~40 years, resulting in solid mineral trapping of ~47 kg of CO2/m3 of basalt.« less

Underestimation of boreal soil carbon stocks by mathematical soil carbon models linked to soil nutrient status

NASA Astrophysics Data System (ADS)

Ťupek, Boris; Ortiz, Carina A.; Hashimoto, Shoji; Stendahl, Johan; Dahlgren, Jonas; Karltun, Erik; Lehtonen, Aleksi

2016-08-01

Inaccurate estimate of the largest terrestrial carbon pool, soil organic carbon (SOC) stock, is the major source of uncertainty in simulating feedback of climate warming on ecosystem-atmosphere carbon dioxide exchange by process-based ecosystem and soil carbon models. Although the models need to simplify complex environmental processes of soil carbon sequestration, in a large mosaic of environments a missing key driver could lead to a modeling bias in predictions of SOC stock change.We aimed to evaluate SOC stock estimates of process-based models (Yasso07, Q, and CENTURY soil sub-model v4) against a massive Swedish forest soil inventory data set (3230 samples) organized by a recursive partitioning method into distinct soil groups with underlying SOC stock development linked to physicochemical conditions.For two-thirds of measurements all models predicted accurate SOC stock levels regardless of the detail of input data, e.g., whether they ignored or included soil properties. However, in fertile sites with high N deposition, high cation exchange capacity, or moderately increased soil water content, Yasso07 and Q models underestimated SOC stocks. In comparison to Yasso07 and Q, accounting for the site-specific soil characteristics (e. g. clay content and topsoil mineral N) by CENTURY improved SOC stock estimates for sites with high clay content, but not for sites with high N deposition.Our analysis suggested that the soils with poorly predicted SOC stocks, as characterized by the high nutrient status and well-sorted parent material, indeed have had other predominant drivers of SOC stabilization lacking in the models, presumably the mycorrhizal organic uptake and organo-mineral stabilization processes. Our results imply that the role of soil nutrient status as regulator of organic matter mineralization has to be re-evaluated, since correct SOC stocks are decisive for predicting future SOC change and soil CO2 efflux.

Big Sky Carbon Sequestration Partnership

DOE Office of Scientific and Technical Information (OSTI.GOV)

Susan Capalbo

2005-12-31

The Big Sky Carbon Sequestration Partnership, led by Montana State University, is comprised of research institutions, public entities and private sectors organizations, and the Confederated Salish and Kootenai Tribes and the Nez Perce Tribe. Efforts under this Partnership in Phase I are organized into four areas: (1) Evaluation of sources and carbon sequestration sinks that will be used to determine the location of pilot demonstrations in Phase II; (2) Development of GIS-based reporting framework that links with national networks; (3) Design of an integrated suite of monitoring, measuring, and verification technologies, market-based opportunities for carbon management, and an economic/risk assessmentmore » framework; (referred to below as the Advanced Concepts component of the Phase I efforts) and (4) Initiation of a comprehensive education and outreach program. As a result of the Phase I activities, the groundwork is in place to provide an assessment of storage capabilities for CO{sub 2} utilizing the resources found in the Partnership region (both geological and terrestrial sinks), that complements the ongoing DOE research agenda in Carbon Sequestration. The geology of the Big Sky Carbon Sequestration Partnership Region is favorable for the potential sequestration of enormous volume of CO{sub 2}. The United States Geological Survey (USGS 1995) identified 10 geologic provinces and 111 plays in the region. These provinces and plays include both sedimentary rock types characteristic of oil, gas, and coal productions as well as large areas of mafic volcanic rocks. Of the 10 provinces and 111 plays, 1 province and 4 plays are located within Idaho. The remaining 9 provinces and 107 plays are dominated by sedimentary rocks and located in the states of Montana and Wyoming. The potential sequestration capacity of the 9 sedimentary provinces within the region ranges from 25,000 to almost 900,000 million metric tons of CO{sub 2}. Overall every sedimentary formation investigated has significant potential to sequester large amounts of CO{sub 2}. Simulations conducted to evaluate mineral trapping potential of mafic volcanic rock formations located in the Idaho province suggest that supercritical CO{sub 2} is converted to solid carbonate mineral within a few hundred years and permanently entombs the carbon. Although MMV for this rock type may be challenging, a carefully chosen combination of geophysical and geochemical techniques should allow assessment of the fate of CO{sub 2} in deep basalt hosted aquifers. Terrestrial carbon sequestration relies on land management practices and technologies to remove atmospheric CO{sub 2} where it is stored in trees, plants, and soil. This indirect sequestration can be implemented today and is on the front line of voluntary, market-based approaches to reduce CO{sub 2} emissions. Initial estimates of terrestrial sinks indicate a vast potential for increasing and maintaining soil Carbon (C) on rangelands, and forested, agricultural, and reclaimed lands. Rangelands can store up to an additional 0.05 mt C/ha/yr, while the croplands are on average four times that amount. Estimates of technical potential for soil sequestration within the region in cropland are in the range of 2.0 M mt C/yr over 20 year time horizon. This is equivalent to approximately 7.0 M mt CO{sub 2}e/yr. The forestry sinks are well documented, and the potential in the Big Sky region ranges from 9-15 M mt CO{sub 2} equivalent per year. Value-added benefits include enhanced yields, reduced erosion, and increased wildlife habitat. Thus the terrestrial sinks provide a viable, environmentally beneficial, and relatively low cost sink that is available to sequester C in the current time frame. The Partnership recognizes the critical importance of measurement, monitoring, and verification technologies to support not only carbon trading but all policies and programs that DOE and other agencies may want to pursue in support of GHG mitigation. The efforts in developing and implementing MMV technologies for geological and terrestrial sequestration reflect this concern. Research in Phase I has identified and validated best management practices for soil C in the Partnership region, and outlined a risk/cost effectiveness framework to make comparative assessments of each viable sink, taking into account economic costs, offsetting benefits, scale of sequestration opportunities, spatial and time dimensions, environmental risks, and long-term viability. This is the basis for the integrative analysis that will be undertaken in Phase II to work with industry, state and local governments and with the pilot demonstration projects to quantify the economic costs and risks associated with all opportunities for carbon storage in the Big Sky region. Scientifically sound MMV is critical for public acceptance of these technologies.« less

Low Temperature Reaction Experiments Between Basalt, Seawater and CO2, and Implications for Carbon Dioxide Sequestration in Deep-Sea Basalts

NASA Astrophysics Data System (ADS)

Marieni, C.; Teagle, D. A. H.; Matter, J. M.

2015-12-01

Reactions between divalent cation-rich silicate minerals and CO2-bearing fluids to form (Ca, Mg, Fe) carbonate minerals could facilitate the safe and permanent storage of anthropogenic carbon dioxide. Deep-sea basalt formations provide large storage reservoir capacities and huge potential sources of Ca2+, Mg2+ and Fe2+. However, better knowledge of silicate mineral reaction rates with carbonate-bearing fluids is required to understand the overall carbon storage potential of these reservoirs. This study investigates key reactions associated with progressive seawater-rock interaction using far-from equilibrium dissolution experiments. The experiments were carried out at 40 ˚C and at constant CO2 partial pressure of 1 atm. Mid-ocean ridge basalts from the Juan de Fuca and Mid-Atlantic Ridges and a gabbro from the Troodos ophiolite were reacted with 500 mL of CO2-charged seawater using thick-walled fluorinated polypropylene bottles combined with rubber stoppers. The starting material was crushed, sieved and thoroughly cleaned to remove fine particles (< 63 μm) to ensure a particle grain size between 63 and 125 μm for all the samples. The seawater chemistry and the pH were monitored throughout the experiments by daily analysis of 1 mL of fluid. The pH increased rapidly from 4.8 to 5.0 before stabilizing at 5.1 after 10 days of reaction time. The analysis of anions (S, Cl) highlighted a substantial evaporation (up to 15 %) during the experiments, requiring a correction factor for the measured dissolved ion concentrations. Evaporation corrected silicon (Si) and calcium (Ca) concentrations in the seawater increased by 5900 % and 14 %, resulting in total dissolved Si and Ca from basalt of 0.3 % and 2.4 %, respectively. The results are comparable with literature data for fresh water experiments conducted on basaltic glass at higher temperature or pressure, illustrating the considerable potential of the mineral sequestration of CO2 in submarine basalts.

Ocean sequestration of crop residue carbon: recycling fossil fuel carbon back to deep sediments.

PubMed

Strand, Stuart E; Benford, Gregory

2009-02-15

For significant impact any method to remove CO2 from the atmosphere must process large amounts of carbon efficiently, be repeatable, sequester carbon for thousands of years, be practical, economical and be implemented soon. The only method that meets these criteria is removal of crop residues and burial in the deep ocean. We show here that this method is 92% efficient in sequestration of crop residue carbon while cellulosic ethanol production is only 32% and soil sequestration is about 14% efficient. Deep ocean sequestration can potentially capture 15% of the current global CO2 annual increase, returning that carbon backto deep sediments, confining the carbon for millennia, while using existing capital infrastructure and technology. Because of these clear advantages, we recommend enhanced research into permanent sequestration of crop residues in the deep ocean.

Water column particulate matter: A key contributor to phosphorus regeneration in a coastal eutrophic environment, the Chesapeake Bay: Particulate phosphorus in the Chesapeake Bay

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Jiying; Reardon, Patrick; McKinley, James P.

Particulate phosphorus (PP) in the water column is an essential component of phosphorus (P) cycling in aquatic ecosystems yet its composition and transformations remain largely uncharacterized. To understand the roles of suspended particulates on regeneration of inorganic P (Pi) into the water column as well as sequestration into more stable mineral precipitates, we studied seasonal variation in both organic and inorganic P speciation in suspended particles in three sites in the Chesapeake Bay using sequential P extraction, 1D (31P) and 2D (1H-31P) nuclear magnetic resonance (NMR) spectroscopies, and electron microprobe analyses (EMPA). Remineralization efficiency of particulate P average 8% andmore » 56% in shallow and deep sites respectively, suggesting the importance of PP remineralization is in resupplying water column Pi. Strong temporal and spatial variability of organic P composition, distributions, and remineralization efficiency were observed relating to water column parameters such as temperature and redox conditions: concentration of orthophosphate monoesters and diesters, and diester-to-monoester (D/M) ratios decreased with depth. Both esters and the D/M ratios were lower in the hypoxic July and September. In contrast, pyrophosphate and orthophosphate increased with depth, and polyphosphates was high in the anoxic water column. Sequential extraction and EMPA analyses of the suspended particles suggest presence of Ca-bound phosphate in the water column. We hypothesize authigenic precipitation of carbonate fluorapatite and/or its precursor mineral(s) in Pi rich water column, supported by our thermodynamic calculations. Our results, overall, reveal the important role suspended particles play in P remineralization and P sequestration in the Chesapeake Bay water column, provide important implications on P bioavailability and P sinks in similar eutrophic coastal environments.« less

Date palm waste-derived biochar composites with silica and zeolite: synthesis, characterization and implication for carbon stability and recalcitrant potential.

PubMed

Ahmad, Munir; Ahmad, Mahtab; Usman, Adel R A; Al-Faraj, Abdullah S; Abduljabbar, Adel; Ok, Yong Sik; Al-Wabel, Mohammad I

2017-03-23

Engineered organo-mineral composites were synthesized from date palm waste biochar and silica or zeolite via mechanochemical treatments. Date palm tree rachis (leaves) waste biomass was pre-treated with silica or zeolite minerals via ball milling and sonication prior to pyrolysis at 600 °C. The resultant organo-mineral composites and pristine materials were characterized using X-ray diffraction, thermogravimetric-differential thermal (TG-DTA), Fourier transform infrared, scanning electron microscope analyses and surface area and porosity analyzer to investigate the variations in physiochemical and structural characteristics. Compared to the resultant composites derived from non-milled date palm biomass, ball milling increased surface area, while decreased crystallinity index and effective particle size of the biochar composites. Silica composited biochars were located near origin in the van Krevelen diagram indicating lowest H/C and O/C molar ratios, thus suggesting higher aromaticity and lower polarity compared to other biochars. TGA thermograms indicated highest thermal stability of silica composited biochars. Ash and moisture corrected TGA thermograms were used to calculate recalcitrance index (R 50 ) of the materials, which speculated high degradability of biomass (R 50  < 0.4), minimal degradability of biochars and zeolite composited biochars (0.5 < R 50  < 0.7) and high recalcitrant nature of silica composited biochars (R 50  > 0.7). Silica composited biochars exhibited highest carbon sequestration potential (64.17-95.59%) compared to other biochars. Highest recalcitrance and carbon sequestration potential of silica composited biochars may be attributed to changes in structural arrangements in the silica-biochar complex. Encapsulations of biochar particles with amorphous silica via Si-C bonding may have prevented thermal degradation, subsequently increasing recalcitrance potential of silica composited biochars.

Climate-change effects on soils: Accelerated weathering, soil carbon and elemental cycling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Qafoku, Nikolla

2015-04-01

Climate change [i.e., high atmospheric carbon dioxide (CO2) concentrations (≥400 ppm); increasing air temperatures (2-4°C or greater); significant and/or abrupt changes in daily, seasonal, and inter-annual temperature; changes in the wet/dry cycles; intensive rainfall and/or heavy storms; extended periods of drought; extreme frost; heat waves and increased fire frequency] is and will significantly affect soil properties and fertility, water resources, food quantity and quality, and environmental quality. Biotic processes that consume atmospheric CO2, and create organic carbon (C) that is either reprocessed to CO2 or stored in soils are the subject of active current investigations, with great concern over themore » influence of climate change. In addition, abiotic C cycling and its influence on the inorganic C pool in soils is a fundamental global process in which acidic atmospheric CO2 participates in the weathering of carbonate and silicate minerals, ultimately delivering bicarbonate and Ca2+ or other cations that precipitate in the form of carbonates in soils or are transported to the rivers, lakes, and oceans. Soil responses to climate change will be complex, and there are many uncertainties and unresolved issues. The objective of the review is to initiate and further stimulate a discussion about some important and challenging aspects of climate-change effects on soils, such as accelerated weathering of soil minerals and resulting C and elemental fluxes in and out of soils, soil/geo-engineering methods used to increase C sequestration in soils, soil organic matter (SOM) protection, transformation and mineralization, and SOM temperature sensitivity. This review reports recent discoveries, identifies key research needs, and highlights opportunities offered by the climate-change effects on soils.« less

Overview of different aspects of climate change effects on soils

DOE Office of Scientific and Technical Information (OSTI.GOV)

Qafoku, Nikolla P.

2014-08-01

Climate change [i.e., high atmospheric carbon dioxide (CO 2) concentrations (≥400 ppm); increasing air temperatures (2-4°C or greater); significant and/or abrupt changes in daily, seasonal, and inter-annual temperature; changes in the wet/dry cycles; intensive rainfall and/or heavy storms; extended periods of drought; extreme frost; heat waves and increased fire frequency] is and will significantly affect soil properties and fertility, water resources, food quantity and quality, and environmental quality. Biotic processes that consume atmospheric CO 2 and create organic carbon (C) that is either reprocessed to CO 2 or stored in soils, are the subject of active current investigations with greatmore » concern over the influence of climate change. In addition, abiotic C cycling and its influence on the inorganic C pool in soils is a fundamental global process in which acidic atmospheric CO 2 participates in the weathering of carbonate and silicate minerals, ultimately delivering bicarbonate and Ca 2+ or other cations that precipitate in the form of carbonates in soils or are transported to the rivers, lakes, and oceans. Soil responses to climate change will be complex, and there are many uncertainties and unresolved issues. The objective of the review is to initiate and further stimulate a discussion about some important and challenging aspects of climate-change effects on soils, such as accelerated weathering of soil minerals and resulting C and elemental fluxes in and out of soils, soil/geo-engineering methods used to increase C sequestration in soils, soil organic matter (SOM) protection, transformation and mineralization, and SOM temperature sensitivity. This review reports recent discoveries and identifies key research needs required to understand the effects of climate change on soils.« less

Climate Change Mitigation through Enhanced Weathering in Bioenergy Crops

NASA Astrophysics Data System (ADS)

Kantola, I. B.; Masters, M. D.; Wolz, K. J.; DeLucia, E. H.

2016-12-01

Bioenergy crops are a renewable alternative to fossil fuels that reduce the net flux of CO2 to the atmosphere through carbon sequestration in plant tissues and soil. A portion of the remaining atmospheric CO2 is naturally mitigated by the chemical weathering of silica minerals, which sequester carbon as carbonates. The process of mineral weathering can be enhanced by crushing the minerals to increase surface area and applying them to agricultural soils, where warm temperatures, moisture, and plant roots and root exudates accelerate the weathering process. The carbonate byproducts of enhanced weathering are expected accumulate in soil water and reduce soil acidity, reduce nitrogen loss as N2O, and increase availability of certain soil nutrients. To determine the potential of enhanced weathering to alter the greenhouse gas balance in both annual (high disturbance, high fertilizer) and perennial (low disturbance, low fertilizer) bioenergy crops, finely ground basalt was applied to fields of maize, soybeans, and miscanthus at the University of Illinois Energy Farm. All plots showed an immediate soil temperature response at 10 cm depth, with increases of 1- 4 °C at midday. Early season CO2 and N2O fluxes mirrored soil temperature prior to canopy closure in all crops, while total N2O fluxes from miscanthus were lower than corn and soybeans in both basalt treatment and control plots. Mid-season N2O production was reduced in basalt-treated corn compared to controls. Given the increasing footprint of bioenergy crops, the ability to reduce GHG emissions in basalt-treated fields has the potential to mitigate atmospheric warming while benefitting soil fertility with the byproducts of weathering.

Nitrogen gas emissions and nitrate leaching dynamics under different tillage practices based on data synthesis and process-based modeling

NASA Astrophysics Data System (ADS)

Huang, Y.; Ren, W.; Tao, B.; Zhu, X.

2017-12-01

Nitrogen losses from the agroecosystems have been of great concern to global changes due to the effects on global warming and water pollution in the form of nitrogen gas emissions (e.g., N2O) and mineral nitrogen leaching (e.g., NO3-), respectively. Conservation tillage, particularly no-tillage (NT), may enhance soil carbon sequestration, soil aggregation and moisture; therefore it has the potential of promoting N2O emissions and reducing NO3- leaching, comparing with conventional tillage (CT). However, associated processes are significantly affected by various factors, such as soil properties, climate, and crop types. How tillage management practices affect nitrogen transformations and fluxes is still far from clear, with inconsistent even opposite results from previous studies. To fill this knowledge gap, we quantitatively investigated gaseous and leaching nitrogen losses from NT and CT agroecosystems based on data synthesis and an improved process-based agroecosystem model. Our preliminary results suggest that NT management is more efficient in reducing NO3- leaching, and meanwhile it simultaneously increases N2O emissions by approximately 10% compared with CT. The effects of NT on N2O emissions and NO3- leaching are highly influenced by the placement of nitrogen fertilizer and are more pronounced in humid climate conditions. The effect of crop types is a less dominant factor in determining N2O and NO3- losses. Both our data synthesis and process-based modeling suggest that the enhanced carbon sequestration capacity from NT could be largely compromised by relevant NT-induced increases in N2O emissions. This study provides the comprehensive quantitative assessment of NT on the nitrogen emissions and leaching in agroecosystems. It provides scientific information for identifying proper management practices for ensuring food security and minimizing the adverse environmental impacts. The results also underscore the importance of suitable nitrogen management in the NT agroecosystems for climate adaptation and mitigation.

An integrated experimental and first-principles computational study of carbon dioxide mineral carbonation reactions in olivine and serpentine

NASA Astrophysics Data System (ADS)

Gormley, Deirdre Marie

This dissertation is a unique integration of experimental and theoretical methods. The central issue that is being addressed is to find a long term and economically viable solution to the disposal of carbon dioxide gas from coal power plants. Mineral carbonation reactions have emerged as a permanent solution to the well-known "Greenhouse Gas" issue. Our group here at ASU along with groups at Los Alamos National Laboratory (LANL), National Energy Technology Laboratory (NETL), Pennsylvania State in Utah (SAIC), and the Albany Research Center (ARC) comprise the working group managed by the US Department of Energy (DOE). We have been collaborating to develop a fundamental understanding of the carbonation reactions of candidate minerals which will ultimately be used to develop a pilot plant process. Two of the candidate minerals used in mineral sequestration processes are forsterite (olivine) and lizardite (serpentine). Both candidates require pre-treatment prior to reaction with carbon dioxide. Forsterite requires attrition (grinding), while lizardite requires a pre-heat treatment (dehydroxylation) step which removes chemically bound water. In Chapter 3 of this thesis, the thermodynamic properties of seven primary oxides involved in reactions with forsterite and lizardite are compared. A novel method was developed using a theoretical molecular quantum physics approach which reproduced experimental results with great accuracy. This method can now be used for other systems where experimental thermodynamic data is unavailable. In Chapters 4 and 5, the dehydroxylation mechanism for lizardite is studied using theoretical models in conjunction with experimental results. A possible mechanism for the dehydroxylation pathway is suggested. This long-awaited result may provide new insight regarding carbonation reactions in lizardite. Chapters 6 and 7 explore the carbonation reactions in forsterite. With the help of high resolution electron microscopy images and extremely large, 10,000 atom models, we have gained new understanding of the reaction layer on the surface of the forsterite crystal. Several computer codes were tested for calculations of electron energy loss near edge spectra, as comparison with experimental electron energy loss spectra, and a reliable strategy for calculation has been suggested. The electron energy loss results have enhanced our knowledge of the forsterite reaction layer.

CO2 mitigation potential of mineral carbonation with industrial alkalinity sources in the United States.

PubMed

Kirchofer, Abby; Becker, Austin; Brandt, Adam; Wilcox, Jennifer

2013-07-02

The availability of industrial alkalinity sources is investigated to determine their potential for the simultaneous capture and sequestration of CO2 from point-source emissions in the United States. Industrial alkalinity sources investigated include fly ash, cement kiln dust, and iron and steel slag. Their feasibility for mineral carbonation is determined by their relative abundance for CO2 reactivity and their proximity to point-source CO2 emissions. In addition, the available aggregate markets are investigated as possible sinks for mineral carbonation products. We show that in the U.S., industrial alkaline byproducts have the potential to mitigate approximately 7.6 Mt CO2/yr, of which 7.0 Mt CO2/yr are CO2 captured through mineral carbonation and 0.6 Mt CO2/yr are CO2 emissions avoided through reuse as synthetic aggregate (replacing sand and gravel). The emission reductions represent a small share (i.e., 0.1%) of total U.S. CO2 emissions; however, industrial byproducts may represent comparatively low-cost methods for the advancement of mineral carbonation technologies, which may be extended to more abundant yet expensive natural alkalinity sources.

Indispensable role of biochar-inherent mineral constituents in its environmental applications: A review.

PubMed

Xu, Xiaoyun; Zhao, Yinghao; Sima, Jingke; Zhao, Ling; Mašek, Ondřej; Cao, Xinde

2017-10-01

Biochar typically consists of both carbon and mineral fractions, and the carbon fraction has been generally considered to determine its properties and applications. Recently, an increasing body of research has demonstrated that mineral components inherent in biochar, such as alkali or alkaline earth metals in the form of carbonates, phosphates, or oxides, could also influence the properties and thus the applications. The review articles published thus far have mainly focused on multiple environmental and agronomic applications of biochar, including carbon sequestration, soil improvement, environmental remediation, etc. This review aims to highlight the indispensable role of the mineral fraction of biochar in these different applications, especially in environmental applications. Specifically, it provides a critical review of current research findings related to the mineral composition of biochar and the effect of the mineral fraction on the physicochemical properties, contaminant sorption, carbon retention and stability, and nutrient bioavailability of biochar. Furthermore, the role of minerals in the emerging applications of biochar, as a precursor for fuel cells, supercapacitors, and photoactive components, is also summarized. Overall, inherent minerals should be fully considered while determining the most appropriate application for any given biochar. A thorough understanding of the role of biochar-bound minerals in different applications will also allow the design or selection of the most suitable biochar for specific applications based on the consideration of feedstock composition, production parameters, and post-treatment. Copyright © 2017 Elsevier Ltd. All rights reserved.

Experimental and simulation studies of pore scale flow and reactive transport associated with supercritical CO2 injection into brine-filled reservoir rocks (Invited)

NASA Astrophysics Data System (ADS)

DePaolo, D. J.; Steefel, C. I.; Bourg, I. C.

2013-12-01

This talk will review recent research relating to pore scale reactive transport effects done in the context of the Department of Energy-sponsored Energy Frontier Research Center led by Lawrence Berkeley National Laboratory with several other laboratory and University partners. This Center, called the Center for Nanoscale Controls on Geologic CO2 (NCGC) has focused effort on the behavior of supercritical CO2 being injected into and/or residing as capillary trapped-bubbles in sandstone and shale, with particular emphasis on the description of nanoscale to pore scale processes that could provide the basis for advanced simulations. In general, simulation of reservoir-scale behavior of CO2 sequestration assumes a number of mostly qualitative relationships that are defensible as nominal first-order descriptions of single-fluid systems, but neglect the many complications that are associated with a two-phase or three-phase reactive system. The contrasts in properties, and the mixing behavior of scCO2 and brine provide unusual conditions for water-rock interaction, and the NCGC has investigated the underlying issues by a combination of approaches including theoretical and experimental studies of mineral nucleation and growth, experimental studies of brine films, mineral wetting properties, dissolution-precipitation rates and infiltration patterns, molecular dynamic simulations and neutron scattering experiments of fluid properties for fluid confined in nanopores, and various approaches to numerical simulation of reactive transport processes. The work to date has placed new constraints on the thickness of brine films, and also on the wetting properties of CO2 versus brine, a property that varies between minerals and with salinity, and may also change with time as a result of the reactivity of CO2-saturated brine. Mineral dissolution is dependent on reactive surface area, which can be shown to vary by a large factor for various minerals, especially when correlated with interconnected pore space. High-resolution numerical simulations of reactive transport can ultimate lead to quantitative descriptions of pore scale chemistry and flow, and examples of recent developments will be presented. However, only a limited description of the processes can realistically be treated in such simulations, and only for chemically simple systems. Whether and when more complete simulations will be achievable is yet to be determined.

The specific role of fungal community structure on soil aggregation and carbon sequestration: results from long-term field study in a paddy soil

NASA Astrophysics Data System (ADS)

Murugan, Rajasekaran; Kumar, Sanjay

2015-04-01

Soil aggregate stability is a crucial soil property that affects soil biota, biogeochemical processes and C sequestration. The relationship between soil aggregate stability and soil C cycling is well known but the influence of specific fungal community structure on this relationship is largely unknown in paddy soils. The aim of the present study was to evaluate the long-term fertilisation (mineral fertiliser-MIN; farmyard manure-FYM; groundnut oil cake-GOC) effects on soil fungal community shifts associated with soil aggregates under rice-monoculture (RRR) and rice-legume-rice (RLR) systems. Fungal and bacterial communities were characterized using phospholipid fatty acids, and glucosamine and muramic acid were used as biomarkers for fungal and bacterial residues, respectively. Microbial biomass C and N, fungal biomass and residues were significantly higher in the organic fertiliser treatments than in the MIN treatment, for all aggregate sizes under both crop rotation systems. In general, fungal/bacterial biomass ratio and fungal residue C/bacterial residue C ratio were significantly higher in macroaggregate fractions (> 2000 and 250-2000 μm) than in microaggregate fractions (53-250 and <53 μm). In both crop rotation systems, the long-term application of FYM and GOC led to increased accumulation of saprotrophic fungi (SF) in aggregate fractions > 2000 μm. In contrast, we found that arbuscular mycorrhizal fungi (AMF) was surprisingly higher in aggregate fractions > 2000 μm than in aggregate fraction 250-2000 μm under MIN treatment. The RLR system showed significantly higher AMF biomass and fungal residue C/ bacterial residue C ratio in both macroaggregate fractions compared to the RRR system. The strong relationships between SF, AMF and water stable aggregates shows the specific contribution of fungi community on soil aggregate stability. Our results highlight the fact that changes within fungal community structure play an important role in shaping the soil aggregate stability and C sequestration in tropical agricultural ecosystems.

Self-limiting advection caused by the development of a dissolution/precipitation zone and implications for the fate of leaky wells in CO2 sequestration

NASA Astrophysics Data System (ADS)

Huerta, N. J.; Hesse, M. A.; Bryant, S. L.; Strazisar, B. R.

2013-12-01

Leaking wells that penetrate a geologic CO2 sequestration site provide a potential direct pathway for the escape of CO2 to an overlying aquifer or even back into the atmosphere. Leakage is a highly coupled system, involving transport of CO2-saturated brine and reaction of carbonic acid with the cement that encases wells. Carbonic acid attacks cement phases to dissolve calcium rich components and raise the fluid pH. Our experiments show that total dissolution of the cement matrix, which would lead to self-enhancing leakage, is prevented by an amorphous aluminosilicate phase that remains after dissolution to constrain fluid flux. Conversely, self-limiting behavior develops in a zone where pH is sufficiently high for carbonate minerals to become insoluble and precipitate. Extrapolation of these bench-scale observations indicates that a barrier of carbonate precipitation would develop as more CO2-saturated brine leaks along a well. The process of sealing of the pathway and the timescale of sealing are critical for any risk assessment of the sequestration operation. Using numerical models to interpret the experiments, we find a lag in self-limiting behavior which is controlled by the saturation state of carbonate phases. Sufficient residence time is crucial for the development of the precipitation zone. Precipitation need not seal uniformly across an entire fracture, only in dominant flow paths. Simply growing the width of a zone of precipitation is insufficient to capture the self-limiting behavior we observe in experiments. To seal, the precipitating material must also accumulate and grow into the open fracture space and close the aperture. Closure rate is a function of the initial leak path conductivity, pressure differential (which controls fluid flux), leak path length, and CO2-saturation in the brine. Combining these results with risk assessment tools that incorporate the well development history will give stakeholders a tool to quantitatively predict well leakage for candidate sites.

Methods to Reduce Forest Residue Volume after Timber Harvesting and Produce Black Carbon.

PubMed

Page-Dumroese, Deborah S; Busse, Matt D; Archuleta, James G; McAvoy, Darren; Roussel, Eric

2017-01-01

Forest restoration often includes thinning to reduce tree density and improve ecosystem processes and function while also reducing the risk of wildfire or insect and disease outbreaks. However, one drawback of these restoration treatments is that slash is often burned in piles that may damage the soil and require further restoration activities. Pile burning is currently used on many forest sites as the preferred method for residue disposal because piles can be burned at various times of the year and are usually more controlled than broadcast burns. In many cases, fire can be beneficial to site conditions and soil properties, but slash piles, with a large concentration of wood, needles, forest floor, and sometimes mineral soil, can cause long-term damage. We describe several alternative methods for reducing nonmerchantable forest residues that will help remove excess woody biomass, minimize detrimental soil impacts, and create charcoal for improving soil organic matter and carbon sequestration.

Field and petrological study of metasomatism and high-pressure carbonation from lawsonite eclogite-facies terrains, Alpine Corsica

NASA Astrophysics Data System (ADS)

Piccoli, Francesca; Vitale Brovarone, Alberto; Ague, Jay J.

2018-04-01

This study presents new field and petrological data on carbonated metasomatic rocks from the lawsonite-eclogite units of Alpine Corsica. These rocks form along major, slab-scale lithological boundaries of the subducted Alpine Tethys plate. Our results indicate that a large variety of rocks ranging from metamafic/ultramafic to metafelsic can react with carbon-bearing fluids, leading to carbon sequestration at high-pressure conditions. The process of carbonation includes both replacement of silicates by high-pressure carbonate, and carbonate veining. The field, microstructural and mineralogical data strongly suggest that the metasomatism was mediated by the infiltration of external fluids of mixed origin, including both mafic/ultramafic and metasedimentary sources. Our results support the following three-step evolution: (i) Release of aqueous fluids by lawsonite and/or antigorite breakdown at depth; (ii) Fluid channelization along the base of the metasedimentary pile of the subducted lithospheric plate and related reactive fluid flow leading to carbonate mineral dissolution; (iii) Further interactions of the resulting carbon-bearing fluids with slab-forming rocks at depths of ca. 70 km and carbonation of pre-existing silicate-rich lithologies. This study highlights the importance of carbonate-bearing fluids evolving along down-T, down-P paths, such as along slab-parallel lithological boundaries, for the sequestration of carbon in subduction zones, and suggests that similar processes may also operate in collisional settings. Fig. S2: Petrogenetic grid in the CaFMASH+CO2 system for the antigorite and clinopyroxene carbonation reactions, together with grossular forming reaction during decarbonation. Reactions are written with the high T assemblage to the right of the = sign.

Fungal Bioweathering of Mimetite and a General Geomycological Model for Lead Apatite Mineral Biotransformations.

PubMed

Ceci, Andrea; Kierans, Martin; Hillier, Stephen; Persiani, Anna Maria; Gadd, Geoffrey Michael

2015-08-01

Fungi play important roles in biogeochemical processes such as organic matter decomposition, bioweathering of minerals and rocks, and metal transformations and therefore influence elemental cycles for essential and potentially toxic elements, e.g., P, S, Pb, and As. Arsenic is a potentially toxic metalloid for most organisms and naturally occurs in trace quantities in soil, rocks, water, air, and living organisms. Among more than 300 arsenic minerals occurring in nature, mimetite [Pb5(AsO4)3Cl] is the most stable lead arsenate and holds considerable promise in metal stabilization for in situ and ex situ sequestration and remediation through precipitation, as do other insoluble lead apatites, such as pyromorphite [Pb5(PO4)3Cl] and vanadinite [Pb5(VO4)3Cl]. Despite the insolubility of mimetite, the organic acid-producing soil fungus Aspergillus niger was able to solubilize mimetite with simultaneous precipitation of lead oxalate as a new mycogenic biomineral. Since fungal biotransformation of both pyromorphite and vanadinite has been previously documented, a new biogeochemical model for the biogenic transformation of lead apatites (mimetite, pyromorphite, and vanadinite) by fungi is hypothesized in this study by application of geochemical modeling together with experimental data. The models closely agreed with experimental data and provided accurate simulation of As and Pb complexation and biomineral formation dependent on, e.g., pH, cation-anion composition, and concentration. A general pattern for fungal biotransformation of lead apatite minerals is proposed, proving new understanding of ecological implications of the biogeochemical cycling of component elements as well as industrial applications in metal stabilization, bioremediation, and biorecovery. Copyright © 2015, American Society for Microbiology. All Rights Reserved.

Investigation of Wyoming Bentonite Hydration in Dry to Water-Saturated Supercritical CO2: Implications for Caprock Integrity

NASA Astrophysics Data System (ADS)

Loring, J. S.; Chen, J.; Thompson, C.; Schaef, T.; Miller, Q. R.; Martin, P. F.; Ilton, E. S.; Qafoku, O.; Felmy, A. R.; Rosso, K. M.

2012-12-01

The effectiveness of geologic sequestration as an enterprise for CO2 storage depends partly on the reactivity of supercritical CO2 (scCO2) with caprock minerals. Injection of scCO2 will displace formation water, and the pore space adjacent to overlying caprocks could eventually be dominated by dry to water-saturated scCO2. Caprock formations have high concentrations of clay minerals, including expandable montmorillonites. Water-bearing scCO2 is highly reactive and capable of hydrating or dehydrating clays, possibly leading to porosity and permeability changes that directly impact caprock performance. Dehydration will cause montmorillonite clay minerals in caprocks to contract, thereby decreasing solid volume and possibly increasing caprock permeability and porosity. On the other hand, water intercalation will cause these clays to expand, thereby increasing solid volume and possibly leading to self-sealing of caprock fractures. Pacific Northwest National Laboratory's Carbon Sequestration Initiative is developing capabilities for studying wet scCO2-mineral reactions in situ. Here, we introduce novel in situ infrared (IR) spectroscopic instrumentation that enables quantitative titrations of reactant minerals with water in scCO2. Results are presented for the infrared spectroscopic titrations of Na-, Ca-, and Mg-saturated Wyoming betonites with water over concentrations ranging from zero to scCO2 saturated. These experiments were carried out at 50°C and 90 bar. Transmission IR spectroscopy was used to measure concentrations of water dissolved in the scCO2 or intercalated into the clays. The titration curves evaluated from the transmission-IR data are compared between the three types of clays to assess the effects of the cation on water partitioning. Single-reflection attenuated total reflection (ATR) IR spectroscopy was used to collect the spectrum of the clays as they hydrate at every total water concentration during the titration. Clay hydration is evidenced by increases in absorbance of the OH stretching and HOH bending modes of the intercalated waters. The ATR-IR data also indicate that CO2 is intercalated in the clay. The asymmetric stretching band of the CO2 molecules that are intercalated in the clay is narrower than that stretching band of bulk scCO2, which indicates that the spectral contribution from rotational fine structure is minimal and the intercalated CO2 is rotationally constrained. A chemometrics analysis of the complete set of ATR-IR spectra spanning the range of total water concentrations covered in the titration finds that there are at least two types of intercalated waters, two types of intercalated CO2 molecules, and the concentrations of these intercalated waters and CO2 molecules are correlated. These quantitative data, when coupled with in situ XRD results that predict interlayer spacing and clay volume, demonstrate that water and CO2 intercalation processes in expandable montmorillonite clays could lead to porosity and permeability changes that directly impact caprock performance.

In situ visualisation and characterisation of the capacity of highly reactive minerals to preserve soil organic matter (SOM) in colloids at submicron scale.

PubMed

Xiao, Jian; Wen, Yongli; Li, Huan; Hao, Jialong; Shen, Qirong; Ran, Wei; Mei, Xinlan; He, Xinhua; Yu, Guanghui

2015-11-01

Mineral-organo associations (MOAs) are a mixture of identifiable biopolymers associated with highly reactive minerals and microorganisms. However, the in situ characterization and correlation between soil organic matter (SOM) and highly reactive Al and Fe minerals are still unclear for the lack of technologies, particularly in the long-term agricultural soil colloids at submicron scale. We combined several novel techniques, including nano-scale secondary ion mass spectrometry (NanoSIMS), X-ray absorption near edge structure (XANES) and confocal laser scanning microscopy (CLSM) to characterise the capacity of highly reactive Al and Fe minerals to preserve SOM in Ferralic Cambisol in south China. Our results demonstrated that: (1) highly reactive minerals were strongly related to SOM preservation, while SOM had a more significant line correlation with the highly reactive Al minerals than the highly reactive Fe minerals, according to the regions of interest correlation analyses using NanoSIMS; (2) allophane and ferrihydrite were the potential mineral species to determine the SOM preservation capability, which was evaluated by the X-ray photoelectron spectroscopy (XPS) and Fe K-edge XANES spectroscopy techniques; and (3) soil organic biopolymers with dominant compounds, such as proteins, polysaccharides and lipids, were distributed at the rough and clustered surface of MOAs with high chemical and spatial heterogeneity according to the CLSM observation. Our results also promoted the understanding of the roles played by the highly reactive Al and Fe minerals in the spatial distribution of soil organic biopolymers and SOM sequestration. Copyright © 2015 Elsevier Ltd. All rights reserved.

The source of dissolved silicon in soil surface solutions of a temperate forest ecosystem: Ge/Si and Si isotope ratios as biogeochemical tracers

NASA Astrophysics Data System (ADS)

Cornelis, J.; Delvaux, B.; Cardinal, D.; André, L.; Ranger, J.; Opfergelt, S.

2010-12-01

Understand the biogeochemical cycle of silicon (Si) in the Earth’s critical zone and the dissolved Si transfer from the litho-pedosphere into the hydrosphere is of great interest for the global balance of biogeochemical processes, including the global C cycle. Indeed, the interaction between Si and C cycles regulates the atmospheric CO2 through the chemical weathering of silicate minerals, the C sequestration in stable organo-mineral compounds and the Si nutrition of phytoplankton CO2-consumers in oceans. H4SiO4 released by mineral dissolution contributes to the critical zone evolution through neoformation of secondary minerals, adsorption onto hydroxyl-bearing phases and recycling by vegetation and return of phytoliths on topsoil. The neoformation of secondary precipitates (clay minerals and phytoliths polymerized in plants) and adsorption of Si onto Fe and Al (hydr)oxides are processes favoring the light Si isotope incorporation, generating rivers enriched in heavy Si isotopes. On the other hand, clay minerals and phytoliths display contrasting Ge/Si ratios since clay-sized weathering products are enriched in Ge and phytoliths are depleted in Ge. Thus stable Si isotope and Ge/Si ratios constitute very interesting proxies to trace transfer of Si in the critical zone. Here we report Si isotopic and Ge/Si ratios of the different Si pools in a temperate soil-tree system (Breuil experimental forest, France) involving various tree species grown on Alumnic Cambisol derived from granitic bedrock. Relative to granitic bedrock (δ30Si = -0.07 ‰; Ge/Si = 2.5 µmol/mol), clay-sized minerals are enriched in 28Si (-1.07 ‰) and Ge (6.2 µmol/mol) while phytoliths are enriched in 28Si (-0.28 to -0.64 ‰) and depleted in Ge (0.1 to 0.3 µmol/mol). This contrast allows us to infer the relative contribution of litho/pedogenic and biogenic mineral dissolution on the release of H4SiO4 in soil surface solutions. The Si-isotope signatures and Ge/Si ratios of forest floor solutions evolve towards lighter values (-1.38 and -2.05 ‰) and higher Ge/Si ratios (2.7 µmol/mol) relative to granite bedrock. This suggests a partial dissolution of 28Si and Ge-enriched secondary clays minerals incorporated by bioturbation in organic-rich horizons, with a fractionation releasing preferentially light Si isotopes. Without considering that organic acids promote dissolution of minerals, clay minerals detected in the organic layer (vermiculite, chlorite, illite and Ca-montmorillonite) are not stable and could have been partially dissolved and transformed in the chemical environment of forest floor. Sources of H4SiO4 in forest floor solutions are influenced by tree species which control the extent of clay-sized minerals mixed in organic horizons by bioturbation and, to a lesser extent, the Si recycling by forest vegetation.

"Supergreen" Renewables: Integration of Mineral Weathering Into Renewable Energy Production for Air CO2 Removal and Storage as Ocean Alkalinity

NASA Astrophysics Data System (ADS)

Rau, G. H.; Carroll, S.; Ren, Z. J.

2015-12-01

Excess planetary CO2 and accompanying ocean acidification are naturally mitigated on geologic time scales via mineral weathering. Here, CO2 acidifies the hydrosphere, which then slowly reacts with silicate and carbonate minerals to produce dissolved bicarbonates that are ultimately delivered to the ocean. This alkalinity not only provides long-term sequestration of the excess atmospheric carbon, but it also chemically counters the effects of ocean acidification by stabilizing or raising pH and carbonate saturation state, thus helping rebalance ocean chemistry and preserving marine ecosystems. Recent research has demonstrated ways of greatly accelerating this process by its integration into energy systems. Specifically, it has been shown (1) that some 80% of the CO2 in a waste gas stream can be spontaneously converted to stable, seawater mineral bicarbonate in the presence of a common carbonate mineral - limestone. This can allow removal of CO2 from biomass combustion and bio-energy production while generating beneficial ocean alkalinity, providing a potentially cheaper and more environmentally friendly negative-CO2-emissions alternative to BECCS. It has also been demonstrated that strong acids anodically produced in a standard saline water electrolysis cell in the formation of H2 can be reacted with carbonate or silicate minerals to generate strong base solutions. These solutions are highly absorptive of air CO2, converting it to mineral bicarbonate in solution. When such electrochemical cells are powered by non-fossil energy (e.g. electricity from wind, solar, tidal, biomass, geothermal, etc. energy sources), the system generates H2 that is strongly CO2-emissions-negative, while producing beneficial marine alkalinity (2-4). The preceding systems therefore point the way toward renewable energy production that, when tightly coupled to geochemical mitigation of CO2 and formation of natural ocean "antacids", forms a high capacity, negative-CO2-emissions, "supergreen" source of fuel or electrcity. 1) http://pubs.acs.org/doi/pdf/10.1021/es102671x2) http://pubs.acs.org/doi/full/10.1021/es800366q3) http://www.pnas.org/content/110/25/10095.full.pdf4) http://pubs.acs.org/doi/abs/10.1021/acs.est.5b00875

Interactive priming of biochar and labile organic matter mineralization in a smectite-rich soil.

PubMed

Keith, Alexandra; Singh, Balwant; Singh, Bhupinder Pal

2011-11-15

Biochar is considered as an attractive tool for long-term carbon (C) storage in soil. However, there is limited knowledge about the effect of labile organic matter (LOM) on biochar-C mineralization in soil or the vice versa. An incubation experiment (20 °C) was conducted for 120 days to quantify the interactive priming effects of biochar-C and LOM-C mineralization in a smectitic clayey soil. Sugar cane residue (source of LOM) at a rate of 0, 1, 2, and 4% (w/w) in combination with two wood biochars (450 and 550 °C) at a rate of 2% (w/w) were applied to the soil. The use of biochars (~ -36‰) and LOM (-12.7‰) or soil (-14.3‰) with isotopically distinct δ(13)C values allowed the quantification of C mineralized from biochar and LOM/soil. A small fraction (0.4-1.1%) of the applied biochar-C was mineralized, and the mineralization of biochar-C increased significantly with increasing application rates of LOM, especially during the early stages of incubation. Concurrently, biochar application reduced the mineralization of LOM-C, and the magnitude of this effect increased with increasing rate of LOM addition. Over time, the interactive priming of biochar-C and LOM-C mineralization was stabilized. Biochar application possesses a considerable merit for long-term soil C-sequestration, and it has a stabilizing effect on LOM in soil.

Estimation of the reactive mineral surface area during CO2-rich fluid-rock interaction: the influence of neogenic phases

NASA Astrophysics Data System (ADS)

Scislewski, A.; Zuddas, P.

2010-12-01

Mineral dissolution and precipitation reactions actively participate to control fluid chemistry during water-rock interaction. It is however, difficult to estimate and well normalize bulk reaction rates if the mineral surface area exposed to the aqueous solution and effectively participating on the reactions is unknown. We evaluated the changing of the reactive mineral surface area during the interaction between CO2-rich fluids and Albitite/Granitoid rocks (similar mineralogy but different abundances), reacting under flow-through conditions. Our methodology, adopting an inverse modeling approach, is based on the estimation of dissolution rate and reactive surface area of the different minerals participating in the reactions by the reconstruction the chemical evolution of the interacting fluids. The irreversible mass-transfer processes is defined by a fractional degree of advancement, while calculations were carried out for Albite, Microcline, Biotite and Calcite assuming that the ion activity of dissolved silica and aluminium ions was limited by the equilibrium with quartz and kaolinite. Irrespective of the mineral abundance in granite and albitite, we found that mineral dissolution rates did not change significantly in the investigated range of time where output solution’s pH remained in the range between 6 and 8, indicating that the observed variation in fluid composition depends not on pH but rather on the variation of the parent mineral’s reactive surface area. We found that the reactive surface area of Albite varied by more than 2 orders of magnitude, while Microcline, Calcite and Biotite surface areas changed by 1-2 orders of magnitude. We propose that parent mineral chemical heterogeneity and, particularly, the stability of secondary mineral phases may explain the observed variation of the reactive surface area of the minerals. Formation of coatings at the dissolving parent mineral surfaces significantly reduced the amount of surface available to react with CO2-rich fluids, decreasing the effective reactive surface area. Predictive models of CO2 sequestration under geological conditions should take into account the inhibiting role of surface coating formation. The CO2 rich fluid-rock interactions may also have significant consequences on metal mobilization. Our results indicated that the formation of stable carbonate complexes enhances the solubility of uranium minerals of both albitite and granite, facilitating the U(IV) oxidation, and limiting the extent of uranium adsorption onto particles in oxidized waters. This clearly produces an increase of the uranium mobility with significant consequences for the environment.

Wettability effect on capillary trapping of supercritical CO2 at pore-scale: micromodel experiment and numerical modeling

NASA Astrophysics Data System (ADS)

Hu, R.; Wan, J.

2015-12-01

Wettability of reservoir minerals along pore surfaces plays a controlling role in capillary trapping of supercritical (sc) CO2 in geologic carbon sequestration. The mechanisms controlling scCO2 residual trapping are still not fully understood. We studied the effect of pore surface wettability on CO2 residual saturation at the pore-scale using engineered high pressure and high temperature micromodel (transparent pore networks) experiments and numerical modeling. Through chemical treatment of the micromodel pore surfaces, water-wet, intermediate-wet, and CO2-wet micromodels can be obtained. Both drainage and imbibition experiments were conducted at 8.5 MPa and 45 °C with controlled flow rate. Dynamic images of fluid-fluid displacement processes were recorded using a microscope with a CCD camera. Residual saturations were determined by analysis of late stage imbibition images of flow path structures. We performed direct numerical simulations of the full Navier-Stokes equations using a volume-of-fluid based finite-volume framework for the primary drainage and the followed imbibition for the micromodel experiments with different contact angles. The numerical simulations agreed well with our experimental observations. We found that more scCO2 can be trapped within the CO2-wet micromodel whereas lower residual scCO2 saturation occurred within the water-wet micromodels in both our experiments and the numerical simulations. These results provide direct and consistent evidence of the effect of wettability, and have important implications for scCO2 trapping in geologic carbon sequestration.

Effective Wettability of Heterogenous Fracture Surfaces Using the Lattice-Boltzmann Method

NASA Astrophysics Data System (ADS)

E Santos, J.; Prodanovic, M.; Landry, C. J.

2017-12-01

Fracture walls in the subsurface are often structured by minerals of different composition (potentially further altered in contact with fluids during hydrocarbon extraction or CO2 sequestration), this yields in a heterogeneous wettability of the surface in contact with the fluids. The focus of our work is to study how surfaces presenting different mineralogy and roughness affect multiphase flow in fractures. Using the Shan-Chen model of the lattice-Boltzmann method (LBM) we define fluid interaction and surface attraction parameters to simulate a system of a wetting and a non-wetting fluid. In this work, we use synthetically created fractures presenting different arrangements of wetting and non-wetting patches, and with or without roughness; representative of different mineralogy, similar workflow can be applied to fractures extracted from X-ray microtomography images of fractures porous media. The results from the LBM simulations provide an insight on how the distribution of mineralogy and surface roughness are related with the observed macroscopic contact angle. We present a comparison between the published analytical models, and our results based on surface areas, spatial distribution and local fracture aperture. The understanding of the variables that affect the contact angle is useful for the comprehension of multiphase processes in naturally fractured reservoirs like primary oil production, enhanced oil recovery and CO2 sequestration. The macroscopic contact angle analytical equations for heterogeneous surfaces with variable roughness are no longer valid in highly heterogeneous systems; we quantify the difference thus offering an alternative to analytical models.

Application of Markov chain Monte Carlo analysis to biomathematical modeling of respirable dust in US and UK coal miners

PubMed Central

Sweeney, Lisa M.; Parker, Ann; Haber, Lynne T.; Tran, C. Lang; Kuempel, Eileen D.

2015-01-01

A biomathematical model was previously developed to describe the long-term clearance and retention of particles in the lungs of coal miners. The model structure was evaluated and parameters were estimated in two data sets, one from the United States and one from the United Kingdom. The three-compartment model structure consists of deposition of inhaled particles in the alveolar region, competing processes of either clearance from the alveolar region or translocation to the lung interstitial region, and very slow, irreversible sequestration of interstitialized material in the lung-associated lymph nodes. Point estimates of model parameter values were estimated separately for the two data sets. In the current effort, Bayesian population analysis using Markov chain Monte Carlo simulation was used to recalibrate the model while improving assessments of parameter variability and uncertainty. When model parameters were calibrated simultaneously to the two data sets, agreement between the derived parameters for the two groups was very good, and the central tendency values were similar to those derived from the deterministic approach. These findings are relevant to the proposed update of the ICRP human respiratory tract model with revisions to the alveolar-interstitial region based on this long-term particle clearance and retention model. PMID:23454101

Root morphology and seed and leaf ionomic traits in a Brassica napus L. diversity panel show wide phenotypic variation and are characteristic of crop habit.

PubMed

Thomas, C L; Alcock, T D; Graham, N S; Hayden, R; Matterson, S; Wilson, L; Young, S D; Dupuy, L X; White, P J; Hammond, J P; Danku, J M C; Salt, D E; Sweeney, A; Bancroft, I; Broadley, M R

2016-10-04

Mineral nutrient uptake and utilisation by plants are controlled by many traits relating to root morphology, ion transport, sequestration and translocation. The aims of this study were to determine the phenotypic diversity in root morphology and leaf and seed mineral composition of a polyploid crop species, Brassica napus L., and how these traits relate to crop habit. Traits were quantified in a diversity panel of up to 387 genotypes: 163 winter, 127 spring, and seven semiwinter oilseed rape (OSR) habits, 35 swede, 15 winter fodder, and 40 exotic/unspecified habits. Root traits of 14 d old seedlings were measured in a 'pouch and wick' system (n = ~24 replicates per genotype). The mineral composition of 3-6 rosette-stage leaves, and mature seeds, was determined on compost-grown plants from a designed experiment (n = 5) by inductively coupled plasma-mass spectrometry (ICP-MS). Seed size explained a large proportion of the variation in root length. Winter OSR and fodder habits had longer primary and lateral roots than spring OSR habits, with generally lower mineral concentrations. A comparison of the ratios of elements in leaf and seed parts revealed differences in translocation processes between crop habits, including those likely to be associated with crop-selection for OSR seeds with lower sulphur-containing glucosinolates. Combining root, leaf and seed traits in a discriminant analysis provided the most accurate characterisation of crop habit, illustrating the interdependence of plant tissues. High-throughput morphological and composition phenotyping reveals complex interrelationships between mineral acquisition and accumulation linked to genetic control within and between crop types (habits) in B. napus. Despite its recent genetic ancestry (<10 ky), root morphology, and leaf and seed composition traits could potentially be used in crop improvement, if suitable markers can be identified and if these correspond with suitable agronomy and quality traits.

Method and apparatus for ion sequestration and a nanostructured metal phosphate

DOEpatents

Mattigod, Shas V [Richland, WA; Fryxell, Glen E [Kennewic, WA; Li, Xiaohong [Richland, WA; Parker, Kent E [Kennewick, WA; Wellman, Dawn M [West Richland, WA

2010-04-06

A nanostructured substance, a process for sequestration of ionic waste, and an ion-sequestration apparatus are disclosed in the specification. The nanostructured substance can comprise a Lewis acid transition metal bound to a phosphate, wherein the phosphate comprises a primary structural component of the substance and the Lewis acid transition metal is a reducing agent. The nanostructured substance has a Brunner-Emmet-Teller (BET) surface area greater than or equal to approximately 100 m.sup.2/g, and a distribution coefficient for an analyte, K.sub.d, greater than or equal to approximately 5000 ml/g. The process can comprise contacting a fluid and a nanostructured metal phosphate. The apparatus can comprise a vessel and a nanostructured metal phosphate. The vessel defines a volume wherein a fluid contacts the nanostructured metal phosphate.

Microbial Fuel Cell-driven caustic potash production from wastewater for carbon sequestration.

PubMed

Gajda, Iwona; Greenman, John; Melhuish, Chris; Santoro, Carlo; Ieropoulos, Ioannis

2016-09-01

This work reports on the novel formation of caustic potash (KOH) directly on the MFC cathode locking carbon dioxide into potassium bicarbonate salt (kalicinite) while producing, instead of consuming electrical power. Using potassium-rich wastewater as a fuel for microorganisms to generate electricity in the anode chamber, has resulted in the formation of caustic catholyte directly on the surface of the cathode electrode. Analysis of this liquid has shown to be highly alkaline (pH>13) and act as a CO2 sorbent. It has been later mineralised to kalicinite thus locking carbon dioxide into potassium bicarbonate salt. This work demonstrates an electricity generation method as a simple, cost-effective and environmentally friendly route towards CO2 sequestration that perhaps leads to a carbon negative economy. Moreover, it shows a potential application for both electricity production and nutrient recovery in the form of minerals from nutrient-rich wastewater streams such as urine for use as fertiliser in the future. Copyright © 2016 The Authors. Published by Elsevier Ltd.. All rights reserved.

Nitrogen Deposition to and Cycling in a Deciduous Forest

DOE PAGES

Pryor, Sara C.; Barthelmie, Rebecca J.; Carreiro, Margaret; ...

2001-01-01

The project described here seeks to answer questions regarding the role increased nitrogen (N) deposition is playing in enhanced carbon (C) sequestration in temperate mid-latitude forests, using detailed measurements from an AmeriFlux tower in southern Indiana (Morgan-Monroe State Forest, or MMSF). The measurements indicate an average atmosphere-surface N flux of approximately 6 mg-N m -2 day -1 during the 2000 growing season, with approximately 40% coming from dry deposition of ammonia (NH 3 ), nitric acid (HNO 3 ), and particle-bound N. Wet deposition and throughfall measurements indicate significant canopy uptake of N (particularly NH 4 +) at the site,more » leading to a net canopy exchange (NCE) of –6 kg-N ha -1 for the growing season. These data are used in combination with data on the aboveground C:N ratio, litterfall flux, and soil net N mineralization rates to indicate the level of potential perturbation of C sequestration at this site.« less

Carbon Sequestration in Unconventional Reservoirs: Geophysical, Geochemical and Geomechanical Considerations

NASA Astrophysics Data System (ADS)

Zakharova, Natalia V.

In the face of the environmental challenges presented by the acceleration of global warming, carbon capture and storage, also called carbon sequestration, may provide a vital option to reduce anthropogenic carbon dioxide emissions, while meeting the world's energy demands. To operate on a global scale, carbon sequestration would require thousands of geologic repositories that could accommodate billions of tons of carbon dioxide per year. In order to reach such capacity, various types of geologic reservoirs should be considered, including unconventional reservoirs such as volcanic rocks, fractured formations, and moderate-permeability aquifers. Unconventional reservoirs, however, are characterized by complex pore structure, high heterogeneity, and intricate feedbacks between physical, chemical and mechanical processes, and their capacity to securely store carbon emissions needs to be confirmed. In this dissertation, I present my contribution toward the understanding of geophysical, geochemical, hydraulic, and geomechanical properties of continental basalts and fractured sedimentary formations in the context of their carbon storage capacity. The data come from two characterization projects, in the Columbia River Flood Basalt in Washington and the Newark Rift Basin in New York, funded by the U.S. Department of Energy through Big Sky Carbon Sequestration Partnerships and TriCarb Consortium for Carbon Sequestration. My work focuses on in situ analysis using borehole geophysical measurements that allow for detailed characterization of formation properties on the reservoir scale and under nearly unaltered subsurface conditions. The immobilization of injected CO2 by mineralization in basaltic rocks offers a critical advantage over sedimentary reservoirs for long-term CO2 storage. Continental flood basalts, such as the Columbia River Basalt Group, possess a suitable structure for CO2 storage, with extensive reservoirs in the interflow zones separated by massive impermeable basalt in flow interiors. Other large igneous provinces and ocean floor basalts could accommodate centuries' worth of world's CO2 emissions. Low-volume basaltic flows and fractured intrusives may potentially serve as smaller-scale CO2 storage targets. However, as illustrated by the example of the Palisade sill in the Newark basin, even densely fractured intrusive basalts are often impermeable, and instead may serve as caprock for underlying formations. Hydraulic properties of fractured formations are very site-specific, but observations and theory suggest that the majority of fractures at depth remain closed. Hydraulic tests in the northern Newark basin indicate that fractures introduce strong anisotropy and heterogeneity to the formation properties, and very few of them augment hydraulic conductivity of these fractured formations. Overall, they are unlikely to provide enough storage capacity for safe CO 2 injection at large scales, but can be suitable for small-scale controlled experiments and pilot injection tests. The risk of inducing earthquakes by underground injection has emerged as one of the primary concerns for large-scale carbon sequestration, especially in fractured and moderately permeable formations. Analysis of in situ stress and distribution of fractures in the subsurface are important steps for evaluating the risks of induced seismicity. Preliminary results from the Newark basin suggest that local stress perturbation may potentially create favorable stress conditions for CO2 sequestration by allowing a considerable pore pressure increase without carrying large risks of fault reactivation. Additional in situ stress data are needed, however, to accurately constrain the magnitude of the minimum horizontal stress, and it is recommended that such tests be conducted at all potential CO 2 storage sites.

Soil carbon storage in plantation forests and pastures: land-use change implications

NASA Astrophysics Data System (ADS)

Scott, Neal A.; Tate, Kevin R.; Ford-Robertson, Justin; Giltrap, David J.; Tattersall Smith, C.

1999-04-01

Afforestation may lead to an accumulation of carbon (C) in vegetation, but little is known about changes in soil C storage with establishment of plantation forests. Plantation forest carbon budget models often omit mineral soil C changes from stand-level C budget calculations, while including forest floor C accumulation, or predict continuous soil C increases over several rotations. We used national soil C databases to quantify differences in soil C content between pasture and exotic pine forest plantations dominated by P. radiata (D. Don), and paired site studies to quantify changes in soil C with conversion of pasture to plantation forest in New Zealand. Overall, mineral soil C to 0.10 m was 20 40% lower under pine for all soil types (p<0.01) except soils with high clay activity (HCA), where there was no difference. Similar trends were observed in the 0.1 0.3 m layer. Moreover, mineral soil C to 0.1 m was 17 40% lower under pine than pasture in side-by-side comparisons. The only non-significant difference occurred at a site located on a HCA soil (p=0.08). When averaged across the site studies and the national databases, the difference in soil C between pasture and pine was about 16 t C ha1on non-HCA soils. This is similar to forest floor C averaged across our individual sites (about 20 t C ha1). The decrease in mineral soil C could result in about a 15% reduction in the average C sequestration potential (112 t C ha1) when pasture is converted to exotic plantation forest on non-HCA soils. The relative importance of this change in mineral soil C will likely vary depending on the productivity potential of a site and harvest impacts on the forest floor C pool. Our results emphasize that changes in soil C should be included in any calculations of C sequestration attributed to plantation forestry.

Sedimentary reservoir oxidation during geologic CO2 sequestration

NASA Astrophysics Data System (ADS)

Lammers, Laura N.; Brown, Gordon E.; Bird, Dennis K.; Thomas, Randal B.; Johnson, Natalie C.; Rosenbauer, Robert J.; Maher, Katharine

2015-04-01

Injection of carbon dioxide into subsurface geologic reservoirs during geologic carbon sequestration (GCS) introduces an oxidizing supercritical CO2 phase into a subsurface geologic environment that is typically reducing. The resulting redox disequilibrium provides the chemical potential for the reduction of CO2 to lower free energy organic species. However, redox reactions involving carbon typically require the presence of a catalyst. Iron oxide minerals, including magnetite, are known to catalyze oxidation and reduction reactions of C-bearing species. If the redox conditions in the reservoir are modified by redox transformations involving CO2, such changes could also affect mineral stability, leading to dissolution and precipitation reactions and alteration of the long-term fate of CO2 in GCS reservoirs. We present experimental evidence that reservoirs with reducing redox conditions are favorable environments for the relatively rapid abiotic reduction of CO2 to organic molecules. In these experiments, an aqueous suspension of magnetite nanoparticles was reacted with supercritical CO2 under pressure and temperature conditions relevant to GCS in sedimentary reservoirs (95-210 °C and ∼100 bars of CO2). Hydrogen production was observed in several experiments, likely caused by Fe(II) oxidation either at the surface of magnetite or in the aqueous phase. Heating of the Fe(II)-rich system resulted in elevated PH2 and conditions favorable for the reduction of CO2 to acetic acid. Implications of these results for the long-term fate of CO2 in field-scale systems were explored using reaction path modeling of CO2 injection into reservoirs containing Fe(II)-bearing primary silicate minerals, with kinetic parameters for CO2 reduction obtained experimentally. The results of these calculations suggest that the reaction of CO2 with reservoir constituents will occur in two primary stages (1) equilibration of CO2 with organic acids resulting in mineral-fluid disequilibrium, and (2) gradual dissolution of primary minerals promoting significant CO2 reduction through the release of Fe(II). The reduction of CO2 is identified as a new trapping mechanism that could significantly enhance the long-term stability of GCS reservoirs. Identification of reservoir characteristics that promote CO2 redox transformations could be used as an additional factor in screening geologic reservoirs for GCS.

Temporal Considerations of Carbon Sequestration in LCA

Treesearch

James Salazar; Richard Bergman

2013-01-01

Accounting for carbon sequestration in LCA illustrates the limitations of a single global warming characterization factor. Typical cradle-to-grave LCA models all emissions from end-of-life processes and then characterizes these flows by IPCC GWP (100-yr) factors. A novel method estimates climate change impact by characterizing annual emissions with the IPCC GHG forcing...

Soil Carbon Sequestration and the Greenhouse Effect (2nd Edition)

USDA-ARS?s Scientific Manuscript database

This volume is a second edition of the book “Soil Carbon Sequestration and The Greenhouse Effect”. The first edition was published in 2001 as SSSA Special Publ. #57. The present edition is an update of the concepts, processes, properties, practices and the supporting data. All chapters are new co...

[Review of lime carbon sink.

PubMed

Liu, Li Li; Ling, Jiang Hua; Tie, Li; Wang, Jiao Yue; Bing, Long Fei; Xi, Feng Ming

2018-01-01

Under the background of "missing carbon sink" mystery and carbon capture and storage (CCS) technology development, this paper summarized the lime material flow process carbon sink from the lime carbonation principles, impact factors, and lime utilization categories in chemical industry, metallurgy industry, construction industry, and lime kiln ash treatment. The results showed that the lime carbonation rate coefficients were mainly impacted by materials and ambient conditions; the lime carbon sink was mainly in chemical, metallurgy, and construction industries; and current researches focused on the mechanisms and impact factors for carbonation, but their carbon sequestration calculation methods had not been proposed. Therefore, future research should focus on following aspects: to establish a complete system of lime carbon sequestration accounting method in view of material flow; to calculate lime carbon sequestration in both China and the world and explain their offset proportion of CO 2 emission from lime industrial process; to analyze the contribution of lime carbon sequestration to missing carbon sink for clarifying part of missing carbon sinks; to promote the development of carbon capture and storage technology and provide some scientific bases for China's international negotiations on climate change.

Is a Clean Development Mechanism project economically justified? Case study of an International Carbon Sequestration Project in Iran.

PubMed

Katircioglu, Salih; Dalir, Sara; Olya, Hossein G

2016-01-01

The present study evaluates a carbon sequestration project for the three plant species in arid and semiarid regions of Iran. Results show that Haloxylon performed appropriately in the carbon sequestration process during the 6 years of the International Carbon Sequestration Project (ICSP). In addition to a high degree of carbon dioxide sequestration, Haloxylon shows high compatibility with severe environmental conditions and low maintenance costs. Financial and economic analysis demonstrated that the ICSP was justified from an economic perspective. The financial assessment showed that net present value (NPV) (US$1,098,022.70), internal rate of return (IRR) (21.53%), and payback period (6 years) were in an acceptable range. The results of the economic analysis suggested an NPV of US$4,407,805.15 and an IRR of 50.63%. Therefore, results of this study suggest that there are sufficient incentives for investors to participate in such kind of Clean Development Mechanism (CDM) projects.

Soil carbon sequestration is a climate stabilization wedge: comments on Sommer and Bossio (2014).

PubMed

Lassaletta, Luis; Aguilera, Eduardo

2015-04-15

Sommer and Bossio (2014) model the potential soil organic carbon (SOC) sequestration in agricultural soils (croplands and grasslands) during the next 87 years, concluding that this process cannot be considered as a climate stabilization wedge. We argue, however, that the amounts of SOC potentially sequestered in both scenarios (pessimistic and optimistic) fulfil the requirements for being considered as wedge because in both cases at least 25 GtC would be sequestered during the next 50 years. We consider that it is precisely in the near future, and meanwhile other solutions are developed, when this stabilization effort is most urgent even if after some decades the sequestration rate is significantly reduced. Indirect effects of SOC sequestration on mitigation could reinforce the potential of this solution. We conclude that the sequestration of organic carbon in agricultural soils as a climate change mitigation tool still deserves important attention for scientists, managers and policy makers. Copyright © 2015 Elsevier Ltd. All rights reserved.

Porosity developed during mineral replacement reactions: implications for fluid flux in the Earth

NASA Astrophysics Data System (ADS)

Putnis, Christine V.; Trindade Pedrosa, Elisabete; Hövelmann, Jörn; Renard, François; Ruiz-Agudo, Encarnacion

2017-04-01

Aqueous fluids, that are ubiquitous in the crust of the Earth, will move through possible pathways in rocks. Rocks characteristically have low permeability but fractures can provide fast fluid channels. Mineral grain boundaries also present easy fluid pathways. However, porosity within minerals forms when a mineral is out of equilibrium with an aqueous fluid and reactions take place in an attempt to reach a new equilibrium. Commonly, dissolution at a mineral-fluid interface initiates one or several coupled reactions involving dissolution and precipitation (Putnis C.V. and Ruiz-Agudo E., 2013; Ruiz-Agudo et al., 2014). In pseudomorphic volume-deficit reactions, a new phase forms while porosity is created, and thereby reactive fluid flow through the originally solid mineral is enhanced. These coupled dissolution-replacement reactions therefore will constrain the flux of material carried by the fluid. These reactions are common during such processes as metamorphism, metasomatism, and weathering. When rock-forming minerals such as feldspars, olivine, pyroxenes and carbonates are in contact with aqueous fluids (typically NaCl-rich) porosity is formed during the interfacial replacement reactions. Elements present in the parent mineral are released to the fluid and therefore mobilized for transport elsewhere. Porosity formation has been shown in a number of systems, such as during the albitisation of feldspars (Hövelmann et al., 2009) and the replacement of carbonates by apatite phases (Pedrosa et al., 2016). Some of these examples will be presented as well as examples from atomic force microscopy (AFM) experiments used to image these reactions at a nanoscale, especially at the calcite-fluid interface, when new phases can be directly observed forming. This mechanism has also been shown as a means of carbon and phosphorus sequestration and for the removal of toxic elements from superficial waters, such as Se and As. References Ruiz-Agudo E., Putnis C.V., Putnis A. (2014) Coupled dissolution and precipitation at mineral-fluid interfaces. Chem. Geol., 383, 132-146. Putnis C.V. and Ruiz-Agudo E. (2013) The mineral-water interface: where minerals react with the environment. Elements, 9, 177-182. Hövelmann J., Putnis A., Geisler T., Schmidt B.C., Golla-Schindler U. (2009) The replacement of plagioclase feldspars by albite: observations from hydrothermal experiments. Contrib. Min. and Pet. 159, 43-59. Pedrosa E.T., Putnis C.V., Putnis A. (2016) The pseudomorphic replacement of marble by apatite: the role of fluid composition. Chem. Geol., 425, 1-11.

Investigation of Reactions between Glauconite and Carbon Dioxide, with Implications for Carbon Sequestration

NASA Astrophysics Data System (ADS)

Nguyen, A. V.; Gabitov, R. I.; Beckingham, L. E.; Toghiani, H.; Fei, Y.; Kirkland, B. L.

2017-12-01

Mineral trapping is one potentially effective technology for long-term storage of carbon dioxide in a subsurface environment that has high temperature and pressure. Conceptually, upon injection of CO2 as a supercritical fluid into geological formations, the CO2 will react with the host rock to form a secondary carbonate mineral that is stable, thus creating a long-term carbon sink under thermodynamic condition of the reaction. Previous studies have demonstrated crystallization of magnesite by reactivity of CO2 and olivine-bearing basalt. Glauconite, a Fe/Ca/Mg bearing aluminosilicate mineral, a potential candidate for reaction with CO2 is common in sedimentary rock formations. The objectives of this study are to 1) develop a protocol for testing mineral trapping in the subsurface and 2) use that protocol to test the reactivity and effectiveness of the mineral glauconite in carbon sequestration. A sample from the Cambrian Riley Formation of Central Texas was selected for this study because it is extremely rich in glauconite. Mineral composition of the powdered sample was investigated by X-ray diffraction (XRD), which revealed that the glauconitic sandstone contains glauconite 20.4%, quartz 71%, and celadonite 8.6%. In the first experiment, 1.5 g of 0.01- 0.5 cm diameter grains reacted with a supercritical CO2 fluid in 30 g of sea water. The laboratory experiment was conducted in a stainless steel vessel in situ reservoir conditions at 120 degrees Celsius and 100 bars. After CO2 injection, pH of the brine decreased from 8.23 to 7. Scanning electron microscopy (SEM) and X-ray diffraction method showed no carbonate formed after 10 days of reaction. However, further experimental modifications facilitated formation of calcite at higher pH. In the second experiment, 0.7 g of 10-75 μm grains presumably reacted with CO2 formed by ammonium carbonate decomposition in a brine of NaCl 0.5 and CaCl2 0.25M; pH after the end of experiment was 7.74. The autoclave was set at 120 degrees Celsius and pressure of saturated water vapour for 14 days. XRD and EDS confirmed the presence of calcite in the sample after the treatment. This material is based upon work supported by the Department of Energy National Energy Technology Laboratory under the Southern States Energy Board's Cooperative Agreement Award Number DE-FE0029465.

Controlling Fluid Flow in the Subsurface through Ureolysis-Controlled Mineral Precipitation

NASA Astrophysics Data System (ADS)

Gerlach, R.; Phillips, A. J.; Cunningham, A. B.; Spangler, L.

2016-12-01

In situ urea hydrolysis has been used by us successfully to manipulate the carbonate alkalinity and control the precipitation of carbonate minerals. Urea hydrolysis can be promoted using microbial cells, enzymes or thermal energy. This technology can be used to mitigate leakage pathways, seal fractures or control fluid transport in the subsurface in hydrocarbon production, enhanced geothermal energy storage, carbon sequestration, nuclear waste disposal, etc. We have completed two field demonstrations of the urea hydrolysis-controlled in situ mineral precipitation technology. The first demonstration showed fracture sealing was possible in a sandstone formation approx. 1120' below ground surface (bgs) and that the fracture had increased resistance to re-fracturing after mineralization treatment. The second field demonstration was performed in a well with an identified channel in the cement near the wellbore at approx. 1020' bgs. The in situ mineralization treatment resulted in reduced pressure decay during shut in periods and reduced injectivity. In addition, a noticeable difference was observed in the solids percentage in the ultrasonic imaging logs before and after biomineralization treatment. The presentation will summarize and put into context the field and our recent laboratory research focusing on permeability manipulation using the in situ ureolysis-driven mineralization technology under ambient and subsurface pressure conditions. We have demonstrated permeability reductions of 3-6 orders of magnitude in 100 µm to 4mm gaps between shale, sandstone and cement/steel interfaces.

Inverse Modeling of Water-Rock-CO2 Batch Experiments: Potential Impacts on Groundwater Resources at Carbon Sequestration Sites.

PubMed

Yang, Changbing; Dai, Zhenxue; Romanak, Katherine D; Hovorka, Susan D; Treviño, Ramón H

2014-01-01

This study developed a multicomponent geochemical model to interpret responses of water chemistry to introduction of CO2 into six water-rock batches with sedimentary samples collected from representative potable aquifers in the Gulf Coast area. The model simulated CO2 dissolution in groundwater, aqueous complexation, mineral reactions (dissolution/precipitation), and surface complexation on clay mineral surfaces. An inverse method was used to estimate mineral surface area, the key parameter for describing kinetic mineral reactions. Modeling results suggested that reductions in groundwater pH were more significant in the carbonate-poor aquifers than in the carbonate-rich aquifers, resulting in potential groundwater acidification. Modeled concentrations of major ions showed overall increasing trends, depending on mineralogy of the sediments, especially carbonate content. The geochemical model confirmed that mobilization of trace metals was caused likely by mineral dissolution and surface complexation on clay mineral surfaces. Although dissolved inorganic carbon and pH may be used as indicative parameters in potable aquifers, selection of geochemical parameters for CO2 leakage detection is site-specific and a stepwise procedure may be followed. A combined study of the geochemical models with the laboratory batch experiments improves our understanding of the mechanisms that dominate responses of water chemistry to CO2 leakage and also provides a frame of reference for designing monitoring strategy in potable aquifers.

Physical and Economic Integration of Carbon Capture Methods with Sequestration Sinks

NASA Astrophysics Data System (ADS)

Murrell, G. R.; Thyne, G. D.

2007-12-01

Currently there are several different carbon capture technologies either available or in active development for coal- fired power plants. Each approach has different advantages, limitations and costs that must be integrated with the method of sequestration and the physiochemical properties of carbon dioxide to evaluate which approach is most cost effective. For large volume point sources such as coal-fired power stations, the only viable sequestration sinks are either oceanic or geological in nature. However, the carbon processes and systems under consideration produce carbon dioxide at a variety of pressure and temperature conditions that must be made compatible with the sinks. Integration of all these factors provides a basis for meaningful economic comparisons between the alternatives. The high degree of compatibility between carbon dioxide produced by integrated gasification combined cycle technology and geological sequestration conditions makes it apparent that this coupling currently holds the advantage. Using a basis that includes complete source-to-sink sequestration costs, the relative cost benefit of pre-combustion IGCC compared to other post-combustion methods is on the order of 30%. Additional economic benefits arising from enhanced oil recovery revenues and potential sequestration credits further improve this coupling.

Lignin: Characterization of a Multifaceted Crop Component

PubMed Central

2013-01-01

Lignin is a plant component with important implications for various agricultural disciplines. It confers rigidity to cell walls, and is therefore associated with tolerance to abiotic and biotic stresses and the mechanical stability of plants. In animal nutrition, lignin is considered an antinutritive component of forages as it cannot be readily fermented by rumen microbes. In terms of energy yield from biomass, the role of lignin depends on the conversion process. It contains more gross energy than other cell wall components and therefore confers enhanced heat value in thermochemical processes such as direct combustion. Conversely, it negatively affects biological energy conversion processes such as bioethanol or biogas production, as it inhibits microbial fermentation of the cell wall. Lignin from crop residues plays an important role in the soil organic carbon cycling, as it constitutes a recalcitrant carbon pool affecting nutrient mineralization and carbon sequestration. Due to the significance of lignin in several agricultural disciplines, the modification of lignin content and composition by breeding is becoming increasingly important. Both mapping of quantitative trait loci and transgenic approaches have been adopted to modify lignin in crops. However, breeding goals must be defined considering the conflicting role of lignin in different agricultural disciplines. PMID:24348159

Dynamics and climate change mitigation potential of soil organic carbon sequestration.

PubMed

Sommer, Rolf; Bossio, Deborah

2014-11-01

When assessing soil organic carbon (SOC) sequestration and its climate change (CC) mitigation potential at global scale, the dynamic nature of soil carbon storage and interventions to foster it should be taken into account. Firstly, adoption of SOC-sequestration measures will take time, and reasonably such schemes could only be implemented gradually at large-scale. Secondly, if soils are managed as carbon sinks, then SOC will increase only over a limited time, up to the point when a new SOC equilibrium is reached. This paper combines these two processes and predicts potential SOC sequestration dynamics in agricultural land at global scale and the corresponding CC mitigation potential. Assuming that global governments would agree on a worldwide effort to gradually change land use practices towards turning agricultural soils into carbon sinks starting 2014, the projected 87-year (2014-2100) global SOC sequestration potential of agricultural land ranged between 31 and 64 Gt. This is equal to 1.9-3.9% of the SRES-A2 projected 87-year anthropogenic emissions. SOC sequestration would peak 2032-33, at that time reaching 4.3-8.9% of the projected annual SRES-A2 emission. About 30 years later the sequestration rate would have reduced by half. Thus, SOC sequestration is not a C wedge that could contribute increasingly to mitigating CC. Rather, the mitigation potential is limited, contributing very little to solving the climate problem of the coming decades. However, we deliberately did not elaborate on the importance of maintaining or increasing SOC for sustaining soil health, agro-ecosystem functioning and productivity; an issue of global significance that deserves proper consideration irrespectively of any potential additional sequestration of SOC. Copyright © 2014 Elsevier Ltd. All rights reserved.

Near-term deployment of carbon capture and sequestration from biorefineries in the United States.

PubMed

Sanchez, Daniel L; Johnson, Nils; McCoy, Sean T; Turner, Peter A; Mach, Katharine J

2018-05-08

Capture and permanent geologic sequestration of biogenic CO 2 emissions may provide critical flexibility in ambitious climate change mitigation. However, most bioenergy with carbon capture and sequestration (BECCS) technologies are technically immature or commercially unavailable. Here, we evaluate low-cost, commercially ready CO 2 capture opportunities for existing ethanol biorefineries in the United States. The analysis combines process engineering, spatial optimization, and lifecycle assessment to consider the technical, economic, and institutional feasibility of near-term carbon capture and sequestration (CCS). Our modeling framework evaluates least cost source-sink relationships and aggregation opportunities for pipeline transport, which can cost-effectively transport small CO 2 volumes to suitable sequestration sites; 216 existing US biorefineries emit 45 Mt CO 2 annually from fermentation, of which 60% could be captured and compressed for pipeline transport for under $25/tCO 2 A sequestration credit, analogous to existing CCS tax credits, of $60/tCO 2 could incent 30 Mt of sequestration and 6,900 km of pipeline infrastructure across the United States. Similarly, a carbon abatement credit, analogous to existing tradeable CO 2 credits, of $90/tCO 2 can incent 38 Mt of abatement. Aggregation of CO 2 sources enables cost-effective long-distance pipeline transport to distant sequestration sites. Financial incentives under the low-carbon fuel standard in California and recent revisions to existing federal tax credits suggest a substantial near-term opportunity to permanently sequester biogenic CO 2 This financial opportunity could catalyze the growth of carbon capture, transport, and sequestration; improve the lifecycle impacts of conventional biofuels; support development of carbon-negative fuels; and help fulfill the mandates of low-carbon fuel policies across the United States. Copyright © 2018 the Author(s). Published by PNAS.

Near-term deployment of carbon capture and sequestration from biorefineries in the United States

PubMed Central

Johnson, Nils; McCoy, Sean T.; Turner, Peter A.; Mach, Katharine J.

2018-01-01

Capture and permanent geologic sequestration of biogenic CO2 emissions may provide critical flexibility in ambitious climate change mitigation. However, most bioenergy with carbon capture and sequestration (BECCS) technologies are technically immature or commercially unavailable. Here, we evaluate low-cost, commercially ready CO2 capture opportunities for existing ethanol biorefineries in the United States. The analysis combines process engineering, spatial optimization, and lifecycle assessment to consider the technical, economic, and institutional feasibility of near-term carbon capture and sequestration (CCS). Our modeling framework evaluates least cost source–sink relationships and aggregation opportunities for pipeline transport, which can cost-effectively transport small CO2 volumes to suitable sequestration sites; 216 existing US biorefineries emit 45 Mt CO2 annually from fermentation, of which 60% could be captured and compressed for pipeline transport for under $25/tCO2. A sequestration credit, analogous to existing CCS tax credits, of $60/tCO2 could incent 30 Mt of sequestration and 6,900 km of pipeline infrastructure across the United States. Similarly, a carbon abatement credit, analogous to existing tradeable CO2 credits, of $90/tCO2 can incent 38 Mt of abatement. Aggregation of CO2 sources enables cost-effective long-distance pipeline transport to distant sequestration sites. Financial incentives under the low-carbon fuel standard in California and recent revisions to existing federal tax credits suggest a substantial near-term opportunity to permanently sequester biogenic CO2. This financial opportunity could catalyze the growth of carbon capture, transport, and sequestration; improve the lifecycle impacts of conventional biofuels; support development of carbon-negative fuels; and help fulfill the mandates of low-carbon fuel policies across the United States. PMID:29686063

Integrating science, economics and law into policy: The case of carbon sequestration in climate change policy

NASA Astrophysics Data System (ADS)

Richards, Kenneth

Carbon sequestration, the extraction and storage of carbon from the atmosphere by biomass, could potentially provide a cost-effective means to reduce net greenhouse gas emissions. The claims on behalf of carbon sequestration may be inadvertently overstated, however. Several key observations emerge from this study. First, although carbon sequestration studies all report results in terms of dollars per ton, the definition of that term varies significantly, meaning that the results of various analyses can not be meaningfully compared. Second, when carbon sequestration is included in an energy-economy model of climate change policy, it appears that carbon sequestration could play a major, if not dominant role in a national carbon emission abatement program, reducing costs of emissions stabilization by as much as 80 percent, saving tens of billions of dollars per year. However, the results are very dependant upon landowners' perceived risk. Studies may also have overstated the potential for carbon sequestration because they have not considered the implementation process. This study demonstrates that three factors will reduce the cost-effectiveness of carbon sequestration. First, the implementation costs associated with measurement and governance of the government-private sector relation are higher than in the case of carbon source control. Second, legal constraints limit the range of instruments that the government can use to induce private landowners to expand their carbon sinks. The government will likely have to pay private parties to expand their sinks, or undertake direct government production. In either case, additional revenues will be required, introducing social costs associated with excess burden. Third, because of the very long time involved in developing carbon sinks (up to several decades) the government may not be able to make credible commitments against exactions of one type or another that would effectively reduce the value of private sector investments in carbon sinks. Consequently, the private sector will increase the rate of return required for participation, increasing the cost of this option. Carbon sequestration can still be a major factor in a national carbon emission abatement program. However, because of the interplay of science, economics and law, the most commonly prescribed environmental policy instruments--marketable allowance and taxes--have little or no direct role to play in the implementation process.

Carbon Sequestration: is Science Leading Policy or Will Policy Direct Science?

NASA Astrophysics Data System (ADS)

Anderson, A. K.

2007-12-01

Climate-related policy is in its infancy on capital hill, as policy makers only recently started to converge on the acceptance that climate change is a credible, scientific reality. Until recently much of the debate and policy decisions have been related to whether or not climate change, or more specifically global warming, is occurring. The climate debate has shifted from discussing the science behind climate change to addressing how we can reduce carbon dioxide emissions. In the 110th Congress, policy makers have come to realize and accept that we, as a nation, are one of the largest global emitters of carbon dioxide to the atmosphere. Geologic carbon sequestration has gained significant congressional attention and is considered to be one of the most promising carbon mitigation tools. In the present Congress, scientific experts have testified before numerous committees about the various caveats of geologic carbon sequestration. As a result, policy has been and is currently being drafted to address the challenges facing large-scale commercial demonstration of geologic sequestration facilities. Policy has been passed through both the House and Senate that is aimed at increasing funding for basic and advanced research, development, and demonstration of small- to large-scale carbon dioxide injection projects. This legislation is only the beginning of a series of legislation that is under development. In the next year, policy will be introduced that will likely address issues related to pore space and mineral rights ownership, regulatory framework for carbon dioxide transport and injection, long-term injection site monitoring protocol, personal and environmental safety, and liability issues, to name a few. Policy is not limited to the technical aspects of carbon capture, transport, and storage, but is also being developed to help stimulate a market that will be operating under climate constraints. Financial incentives have been proposed that will assist industrial carbon dioxide emitters in making the transition into a carbon-constrained economy. Science has driven the initial policy that has been proposed to date; however, the topic of carbon sequestration has been advanced through Congress at a near record-breaking pace. As such, there is an increased need to hear from scientists in academia and industry alike to continue to make good policy decisions related to carbon sequestration based on sound scientific advice.

Enhanced practical photosynthetic CO2 mitigation

DOEpatents

Bayless, David J.; Vis-Chiasson, Morgan L.; Kremer, Gregory G.

2003-12-23

This process is unique in photosynthetic carbon sequestration. An on-site biological sequestration system directly decreases the concentration of carbon-containing compounds in the emissions of fossil generation units. In this process, photosynthetic microbes are attached to a growth surface arranged in a containment chamber that is lit by solar photons. A harvesting system ensures maximum organism growth and rate of CO.sub.2 uptake. Soluble carbon and nitrogen concentrations delivered to the cyanobacteria are enhanced, further increasing growth rate and carbon utilization.

CO2 breakthrough pressure and permeability for unsaturated low-permeability sandstone of the Ordos Basin

NASA Astrophysics Data System (ADS)

Zhao, Yan; Yu, Qingchun

2017-07-01

With rising threats from greenhouse gases, capture and injection of CO2 into suitable underground formations is being considered as a method to reduce anthropogenic emissions of CO2 to the atmosphere. As the injected CO2 will remain in storage for hundreds of years, the safety of CO2 geologic sequestration is a major concern. The low-permeability sandstone of the Ordos Basin in China is regarded as both caprock and reservoir rock, so understanding the breakthrough pressure and permeability of the rock is necessary. Because part of the pore volume experiences a non-wetting phase during the CO2 injection and migration process, the rock may be in an unsaturated condition. And if accidental leakage occurs, CO2 will migrate up into the unsaturated zone. In this study, breakthrough experiments were performed at various degrees of water saturation with five core samples of low-permeability sandstone obtained from the Ordos Basin. The experiments were conducted at 40 °C and pressures of >8 MPa to simulate the geological conditions for CO2 sequestration. The results indicate that the degree of water saturation and the pore structure are the main factors affecting the rock breakthrough pressure and permeability, since the influence of calcite dissolution and clay mineral swelling during the saturation process is excluded. Increasing the average pore radius or most probable pore radius leads to a reduction in the breakthrough pressure and an increase by several orders of magnitude in scCO2 effective permeability. In addition, the breakthrough pressure rises and the scCO2 effective permeability decreases when the water saturation increases. However, when the average pore radius is greater than 0.151 μm, the degree of water saturation will has a little effect on the breakthrough pressure. On this foundation, if the most probable pore radius of the core sample reaches 1.760 μm, the breakthrough pressure will not be impacted by the increasing water saturation. We establish correlations between (1) the breakthrough pressure and average pore radius or most probable pore radius, (2) the breakthrough pressure and scCO2 effective permeability, (3) the breakthrough pressure and water saturation, and (4) the scCO2 effective permeability and water saturation. This study provides practical information for further studies of CO2 sequestration as well as the caprock evaluation.

Biotic and abiotic effects on CO2 sequestration during microbially-induced calcium carbonate precipitation.

PubMed

Okyay, Tugba Onal; Rodrigues, Debora F

2015-03-01

In this study, CO2 sequestration was investigated through the microbially-induced calcium carbonate precipitation (MICP) process with isolates obtained from a cave called 'Cave Without A Name' (Boerne, TX, USA) and the Pamukkale travertines (Denizli, Turkey). The majority of the bacterial isolates obtained from these habitats belonged to the genera Sporosarcina, Brevundimonas, Sphingobacterium and Acinetobacter. The isolates were investigated for their capability to precipitate calcium carbonate and sequester CO2. Biotic and abiotic effects of CO2 sequestration during MICP were also investigated. In the biotic effect, we observed that the rate and concentration of CO2 sequestered was dependent on the species or strains. The main abiotic factors affecting CO2 sequestration during MICP were the pH and medium components. The increase in pH led to enhanced CO2 sequestration by the growth medium. The growth medium components, on the other hand, were shown to affect both the urease activity and CO2 sequestration. Through the Plackett-Burman experimental design, the most important growth medium component involved in CO2 sequestration was determined to be urea. The optimized medium composition by the Plackett-Burman design for each isolate led to a statistically significant increase, of up to 148.9%, in CO2 uptake through calcification mechanisms. © FEMS 2015. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.

Metal Carbonation of Forsterite in Supercritical CO2 and H2O Using Solid State 29Si, 13C NMR Spectroscop

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kwak, Ja Hun; Hu, Jian Z.; Hoyt, David W.

2010-03-11

Ex situ solid state NMR was used for the first time to study fundamental mineral carbonation processes and reaction extent relevant to geologic carbon sequestration (GCS) using a model silicate mineral forsterite (Mg2SiO4)+supercriticalCO2 with and without H2O. Run conditions were 80 C and 96 atm. 29Si NMR clearly shows that in the absence of CO2, the role of H2O is to hydrolyze surface Mg-O-Si bonds to produce dissolved Mg2+, and mono- and oligomeric hydroxylated silica species. Surface hydrolysis products contain only Q0 (Si(OH)4) and Q1(Si(OH)3OSi) species. An equilibrium between Q0, Q1 and Mg2+ with a saturated concentration equivalent to lessmore » than 3.2% of the Mg2SiO4 conversion is obtained at a reaction time of up to 7 days. Using scCO2 without H2O, no reaction is observed within 7 days. Using both scCO2 and H2O, the surface reaction products for silica are mainly Q3 (SiOH(OSi)3) species accompanied by a lesser amount of Q2 (Si(OH)2(OSi)2) and Q4 (Si(OSi)4). However, no Q0 and Q1 were detected, indicating the carbonic acid formation/deprotonation and magnesite (MgCO3) precipitation reactions are faster than the forsterite hydrolysis process. Thus it can be concluded that the Mg2SiO4 hydrolysis process is the rate limiting step of the overall mineral carbonation process. 29Si NMR combined with XRD, TEM, SAED and EDX further reveal that the reaction is a surface reaction with the Mg2SiO4 crystallite in the core and with condensed Q2-Q4 species forming amorphous surface layers. 13C MAS NMR identified a possible reaction intermediate as (MgCO3)4-Mg(OH)2-5H2O. However, at long reaction times only crystallite magnesite MgCO3 products are observed.« less

Rapid Assessment of Ecosystem Services Provided by Two Mineral Extraction Sites Restored for Nature Conservation in an Agricultural Landscape in Eastern England

PubMed Central

Blaen, Phillip J.; Jia, Li; Peh, Kelvin S.-H.; Field, Rob H.; Balmford, Andrew; MacDonald, Michael A.; Bradbury, Richard B.

2015-01-01

Despite growing recognition that mineral sites restored for nature conservation can enhance local biodiversity, the wider societal benefits provided by this type of restoration relative to alternative options are not well understood. This study addresses this research gap by quantifying differences in ecosystem services provision under two common mineral site after-uses: nature conservation and agriculture. Using a combination of site-specific primary field data, benefits transfer and modelling, we show that for our sites restoration for nature conservation provides a more diverse array of ecosystem services than would be delivered under an agricultural restoration scenario. We also explore the effects of addressing different conservation targets, which we find alter the provision of ecosystem services on a service-specific basis. Highly species-focused intervention areas are associated with increased carbon storage and livestock grazing provision, whereas non-intervention areas are important for carbon sequestration, fishing, recreation and flood risk mitigation. The results of this study highlight the wider societal importance of restored mineral sites and may help conservation managers and planners to develop future restoration strategies that provide benefits for both biodiversity and human well-being. PMID:25894293

Rapid assessment of ecosystem services provided by two mineral extraction sites restored for nature conservation in an agricultural landscape in eastern England.

PubMed

Blaen, Phillip J; Jia, Li; Peh, Kelvin S-H; Field, Rob H; Balmford, Andrew; MacDonald, Michael A; Bradbury, Richard B

2015-01-01

Despite growing recognition that mineral sites restored for nature conservation can enhance local biodiversity, the wider societal benefits provided by this type of restoration relative to alternative options are not well understood. This study addresses this research gap by quantifying differences in ecosystem services provision under two common mineral site after-uses: nature conservation and agriculture. Using a combination of site-specific primary field data, benefits transfer and modelling, we show that for our sites restoration for nature conservation provides a more diverse array of ecosystem services than would be delivered under an agricultural restoration scenario. We also explore the effects of addressing different conservation targets, which we find alter the provision of ecosystem services on a service-specific basis. Highly species-focused intervention areas are associated with increased carbon storage and livestock grazing provision, whereas non-intervention areas are important for carbon sequestration, fishing, recreation and flood risk mitigation. The results of this study highlight the wider societal importance of restored mineral sites and may help conservation managers and planners to develop future restoration strategies that provide benefits for both biodiversity and human well-being.

Modeling impacts of management on carbon sequestration and trace gas emissions in forested wetland ecosystems

Treesearch

Changsheng Li; Jianbo Cui

2004-01-01

A process- based model, Wetland-DNDC, was modified to enhance its capacity to predict the impacts of management practices on carbon sequestration in and trace gas emissions from forested wetland ecosystems. The modifications included parameterization of management practices fe.g., forest harvest, chopping, burning, water management, fertilization, and tree planting),...

Encapsulation and solid state sequestration of gases by calix[6]arene-based molecular containers.

PubMed

Lavendomme, Roy; Ajami, Daniela; Moerkerke, Steven; Wouters, Johan; Rissanen, Kari; Luhmer, Michel; Jabin, Ivan

2017-06-13

Two calix[6]arene-based molecular containers were synthesized in high yields. These containers can encapsulate small guests through a unique "rotating door" complexation process. The sequestration of greenhouse gases is clearly demonstrated. They can be stored in the solid state for long periods and released via dissolution of the inclusion complex.

H2S Injection and Sequestration into Basalt - The SulFix Project

NASA Astrophysics Data System (ADS)

Gudbrandsson, S.; Moola, P.; Stefansson, A.

2014-12-01

Atmospheric H2S emissions are among major environmental concern associated with geothermal energy utilization. It is therefore of great importance for the geothermal power sector to reduce H2S emissions. Known solutions for H2S neutralization are both expensive and include production of elemental sulfur and sulfuric acid that needs to be disposed of. Icelandic energy companies that utilize geothermal power for electricity production have decided to try to find an environmentally friendly and economically feasible solution to reduce the H2S emission, in a joint venture called SulFix. The aim of SulFix project is to explore the possibilities of injecting H2S dissolved in water into basaltic formations in close proximity to the power plants for permanent fixation as sulfides. The formation of sulfides is a natural process in geothermal systems. Due to basalt being rich in iron and dissolving readily at acidic conditions, it is feasible to re-inject the H2S dissolved in water, into basaltic formations to form pyrite. To estimate the mineralization rates of H2S, in the basaltic formation, flow through experiments in columns were conducted at various H2S concentrations, temperatures (100 - 240°C) and both fresh and altered basaltic glass. The results indicate that pyrite rapidly forms during injection into fresh basalt but the precipiation in altered basalt is slower. Three different alteration stages, as a function of distance from inlet, can be observed in the column with fresh basaltic glass; (1) dissolution features along with precipitation, (2) precipitation increases, both sulfides and other secondary minerals and (3) the basalt looks to be unaltered and little if any precipitation is observed. The sulfur has precipitated in the first half of the column and thereafter the solution is possibly close to be supersaturated with respect to the rock. These results indicate that the H2S sequestration into basalt is possible under geothermal conditions. The rate limiting step is the availability of iron released from the dissolving rock. The rapid precipitation of secondary phases in the column suggests the possibility of decreased porosity in the vicinity of the injection well.

Hydrogen Cyanide in the Rhizosphere: Not Suppressing Plant Pathogens, but Rather Regulating Availability of Phosphate

PubMed Central

Rijavec, Tomaž; Lapanje, Aleš

2016-01-01

Plant growth promoting rhizobacteria produce chemical compounds with different benefits for the plant. Among them, HCN is recognized as a biocontrol agent, based on its ascribed toxicity against plant pathogens. Based on several past studies questioning the validity of this hypothesis, we have re-addressed the issue by designing a new set of in vitro experiments, to test if HCN-producing rhizobacteria could inhibit the growth of phytopathogens. The level of HCN produced by the rhizobacteria in vitro does not correlate with the observed biocontrol effects, thus disproving the biocontrol hypothesis. We developed a new concept, in which HCN does not act as a biocontrol agent, but rather is involved in geochemical processes in the substrate (e.g., chelation of metals), indirectly increasing the availability of phosphate. Since this scenario can be important for the pioneer plants living in oligotrophic alpine environments, we inoculated HCN producing bacteria into sterile mineral sand together with germinating plants and showed that the growth of the pioneer plant French sorrel was increased on granite-based substrate. No such effect could be observed for maize, where plantlets depend on the nutrients stored in the endosperm. To support our concept, we used KCN and mineral sand and showed that mineral mobilization and phosphate release could be caused by cyanide in vitro. We propose that in oligotrophic alpine environments, and possibly elsewhere, the main contribution of HCN is in the sequestration of metals and the consequential indirect increase of nutrient availability, which is beneficial for the rhizobacteria and their plant hosts. PMID:27917154

Different composition and distribution patterns of mineral-protected versus hydrolyzable lipids in shrubland soils

NASA Astrophysics Data System (ADS)

Cai, Yue; Tang, Zhiyao; Xiong, Gaoming; Xie, Zongqiang; Liu, Zongguang; Feng, Xiaojuan

2017-09-01

Mineral protection is known as an important mechanism stabilizing soil organic carbon (SOC). However, the composition, sources, and variations of mineral-protected SOC remain poorly constrained. To fill this knowledge gap, we used hydrofluoric acid to demineralize soil matrix and compared the sources and distribution of mineral-protected lipids (ML) versus hydrolyzable lipids (HL) of four typical Chinese shrubland soils. ML was found to represent a sizable fraction (9-32%) of total aliphatic lipids (including n-alkanols; n-alkanoic acids; α,ω-alkanedioic acids; hydroxyalkanoic acids; and midchain-substituted acids) in all soils. Based on carbon chain length and branch positions, microbe- and plant-derived lipids were distinguished. No significant difference was found in the ratio of microbe- to plant-derived lipids in ML versus HL, implying that plant and microbial inputs are equally important for the mineral-associated soil lipids. However, ML contained a higher proportion of nonspecific lipids, especially at depths. Furthermore, to evaluate key environmental variable(s) controlling the distribution of different lipid components, a multiple stepwise regression analysis was conducted. Notably, ML was mainly affected by SOC-to-nitrogen ratio instead of mineralogical properties, implying that the accrual of mineral-associated soil lipids relies strongly on organic matter properties. Collectively, our findings provide novel insights on sources and accumulation mechanisms of mineral-protected soil lipids. SOC decomposition and subsequent accretion of degradation products appear to be vital for the sequestration of mineral-associated soil lipids and warrant better recognition in the investigations of stable soil carbon accumulation mechanisms.

The Interfacial Behavior between Biochar and Soil Minerals and Its Effect on Biochar Stability.

PubMed

Yang, Fan; Zhao, Ling; Gao, Bin; Xu, Xiaoyun; Cao, Xinde

2016-03-01

In this study, FeCl3, AlCl3, CaCl2, and kaolinite were selected as model soil minerals and incubated with walnut shell derived biochar for 3 months and the incubated biochar was then separated for the investigation of biochar-mineral interfacial behavior using XRD and SEM-EDS. The XPS, TGA, and H2O2 oxidation were applied to evaluate effects of the interaction on the stability of biochar. Fe8O8(OH)8Cl1.35 and AlCl3·6H2O were newly formed on the biochar surface or inside of the biochar pores. At the biochar-mineral interface, organometallic complexes such as Fe-O-C were generated. All the 4 minerals enhanced the oxidation resistance of biochar surface by decreasing the relative contents of C-O, C═O, and COOH from 36.3% to 16.6-26.5%. Oxidation resistance of entire biochar particles was greatly increased with C losses in H2O2 oxidation decreasing by 13.4-79.6%, and the C recalcitrance index (R50,bicohar) in TGA analysis increasing from 44.6% to 45.9-49.6%. Enhanced oxidation resistance of biochar surface was likely due to the physical isolation from newly formed minerals, while organometallic complex formation was probably responsible for the increase in oxidation resistance of entire biochar particles. Results indicated that mineral-rich soils seemed to be a beneficial environment for biochar since soil minerals could increase biochar stability, which displays an important environmental significance of biochar for long-term carbon sequestration.

Future C loss in mid-latitude mineral soils: climate change exceeds land use mitigation potential in France

PubMed Central

Meersmans, Jeroen; Arrouays, Dominique; Van Rompaey, Anton J. J.; Pagé, Christian; De Baets, Sarah; Quine, Timothy A.

2016-01-01

Many studies have highlighted significant interactions between soil C reservoir dynamics and global climate and environmental change. However, in order to estimate the future soil organic carbon sequestration potential and related ecosystem services well, more spatially detailed predictions are needed. The present study made detailed predictions of future spatial evolution (at 250 m resolution) of topsoil SOC driven by climate change and land use change for France up to the year 2100 by taking interactions between climate, land use and soil type into account. We conclude that climate change will have a much bigger influence on future SOC losses in mid-latitude mineral soils than land use change dynamics. Hence, reducing CO2 emissions will be crucial to prevent further loss of carbon from our soils. PMID:27808169

Future C loss in mid-latitude mineral soils: climate change exceeds land use mitigation potential in France.

PubMed

Meersmans, Jeroen; Arrouays, Dominique; Van Rompaey, Anton J J; Pagé, Christian; De Baets, Sarah; Quine, Timothy A

2016-11-03

Many studies have highlighted significant interactions between soil C reservoir dynamics and global climate and environmental change. However, in order to estimate the future soil organic carbon sequestration potential and related ecosystem services well, more spatially detailed predictions are needed. The present study made detailed predictions of future spatial evolution (at 250 m resolution) of topsoil SOC driven by climate change and land use change for France up to the year 2100 by taking interactions between climate, land use and soil type into account. We conclude that climate change will have a much bigger influence on future SOC losses in mid-latitude mineral soils than land use change dynamics. Hence, reducing CO 2 emissions will be crucial to prevent further loss of carbon from our soils.

Negative Emissions Technology

NASA Astrophysics Data System (ADS)

Day, Danny

2006-04-01

Although `negative emissions' of carbon dioxide need not, in principle, involve use of biological processes to draw carbon out of the atmosphere, such `agricultural' sequestration' is the only known way to remove carbon from the atmosphere on time scales comparable to the time scale for anthropogenic increases in carbon emissions. In order to maintain the `negative emissions' the biomass must be used in such a way that the resulting carbon dioxide is separated and permanently sequestered. Two options for sequestration are in the topsoil and via geologic carbon sequestration. The former has multiple benefits, but the latter also is needed. Thus, although geologic carbon sequestration is viewed skeptically by some environmentalists as simply a way to keep using fossil fuels---it may be a key part of reversing accelerating climate forcing if rapid climate change is beginning to occur. I will first review the general approach of agricultural sequestration combined with use of resulting biofuels in a way that permits carbon separation and then geologic sequestration as a negative emissions technology. Then I discuss the process that is the focus of my company---the EPRIDA cycle. If deployed at a sufficiently large scale, it could reverse the increase in CO2 concentrations. I also estimate of benefits --carbon and other---of large scale deployment of negative emissions technologies. For example, using the EPRIDA cycle by planting and soil sequestering carbon in an area abut In 3X the size of Texas would remove the amount of carbon that is being accumulated worldwide each year. In addition to the atmospheric carbon removal, the EPRIDA approach also counters the depletion of carbon in the soil---increasing topsoil and its fertility; reduces the excess nitrogen in the water by eliminating the need for ammonium nitrate fertilizer and reduces fossil fuel reliance by providing biofuel and avoiding natural gas based fertilizer production.

A Novel Approach to Experimental Studies of Mineral Dissolution Kinetics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen Zhu; William E. Seyfried

2005-01-01

Currently, DOE is conducting pilot CO{sub 2} injection tests to evaluate the concept of geological sequestration. One strategy that potentially enhances CO{sub 2} solubility and reduces the risk of CO{sub 2} leak back to the surface is dissolution of indigenous minerals in the geological formation and precipitation of secondary carbonate phases, which increases the brine pH and immobilizes CO{sub 2}. Clearly, the rates at which these dissolution and precipitation reactions occur directly determine the efficiency of this strategy. However, one of the fundamental problems in modern geochemistry is the persistent two to five orders of magnitude discrepancy between laboratory-measured andmore » field derived feldspar dissolution rates. To date, there is no real guidance as to how to predict silicate reaction rates for use in quantitative models. Current models for assessment of geological carbon sequestration have generally opted to use laboratory rates, in spite of the dearth of such data for compositionally complex systems, and the persistent disconnect between lab and field applications. Therefore, a firm scientific basis for predicting silicate reaction kinetics in CO{sub 2} injected geological formations is urgently needed to assure the reliability of the geochemical models used for the assessments of carbon sequestration strategies. The funded experimental and theoretical study attempts to resolve this outstanding scientific issue by novel experimental design and theoretical interpretation to measure silicate dissolution rates and iron carbonate precipitation rates at conditions pertinent to geological carbon sequestration. In the first year of the project, we have successfully developed a sample preparation method and completed three batch feldspar dissolution experiments at 200 C and 300 bars. The changes of solution chemistry as dissolution experiments progressed were monitored with on-line sampling of the aqueous phase at the constant temperature and pressure. These data allow calculating overall apparent feldspar dissolution rates and secondary mineral precipitation rates as a function of saturation states. State-of-the-art atomic resolution transmission electron microscopy (TEM), scanning electron microscopy, and electron microprobe was used to characterize the reactants (feldspars before experiments). We experimented with different sample preparation methods for TEM study, and found excellent images and chemical resolution with reactants, which shows promise of the technology and establishes the baseline for comparison with products (feldspars after the experiments). Preliminary electron microscopic characterization shows that the reacted feldspars have etch pits and are covered with secondary sheet silicate phases. Reaction-path geochemical modeling is used to interpret the experimental results. We have established the software and database, and are making great progress. Also during the first year, our education goal of graduate student training has been achieved. A Ph. D. student at Indiana University is progressing well in the degree program and has taken geochemical modeling, SEM, and TEM courses, which will facilitate research in the second and third year. A Ph. D. student at University of Minnesota is progressing well in conducting the experiments, and is near graduation. With the success of training of graduate students and excellent experimental data in the first year, we anticipate a more fruitful year in the second year.« less

Sensitivity of mineral dissolution rates to physical weathering : A modeling approach

NASA Astrophysics Data System (ADS)

Opolot, Emmanuel; Finke, Peter

2015-04-01

There is continued interest on accurate estimation of natural weathering rates owing to their importance in soil formation, nutrient cycling, estimation of acidification in soils, rivers and lakes, and in understanding the role of silicate weathering in carbon sequestration. At the same time a challenge does exist to reconcile discrepancies between laboratory-determined weathering rates and natural weathering rates. Studies have consistently reported laboratory rates to be in orders of magnitude faster than the natural weathering rates (White, 2009). These discrepancies have mainly been attributed to (i) changes in fluid composition (ii) changes in primary mineral surfaces (reactive sites) and (iii) the formation of secondary phases; that could slow natural weathering rates. It is indeed difficult to measure the interactive effect of the intrinsic factors (e.g. mineral composition, surface area) and extrinsic factors (e.g. solution composition, climate, bioturbation) occurring at the natural setting, in the laboratory experiments. A modeling approach could be useful in this case. A number of geochemical models (e.g. PHREEQC, EQ3/EQ6) already exist and are capable of estimating mineral dissolution / precipitation rates as a function of time and mineral mass. However most of these approaches assume a constant surface area in a given volume of water (White, 2009). This assumption may become invalid especially at long time scales. One of the widely used weathering models is the PROFILE model (Sverdrup and Warfvinge, 1993). The PROFILE model takes into account the mineral composition, solution composition and surface area in determining dissolution / precipitation rates. However there is less coupling with other processes (e.g. physical weathering, clay migration, bioturbation) which could directly or indirectly influence dissolution / precipitation rates. We propose in this study a coupling between chemical weathering mechanism (defined as a function of reactive area, solution composition, temperature, mineral composition) and the physical weathering module in the SoilGen model which calculates the evolution of particle size (used for surface area calculation) as influenced by temperature gradients. The solution composition in the SoilGen model is also influenced by other processes such as atmospheric inputs, organic matter decomposition, cation exchange, secondary mineral formation and leaching. We then apply this coupled mechanism on a case study involving 3 loess soil profiles to analyze the sensitivity of mineral weathering rates to physical weathering. Initial results show some sensitivity but not that dramatic. The less sensitivity was attributed to dominance of resistant primary minerals (> 70% quartz). Scenarios with different sets of mineralogy will be tested and sensitivity results in terms of silicate mineral dissolution rates and CO2-consumption will be presented in the conference. References Sverdrup H and Warfvinge P., 1993. Calculating field weathering rates using a mechanistic geochemical model PROFILE. Applied Geochemistry, 8:273-283. White, A.F., 2009. Natural weathering rates of silicate minerals. In: Drever, J.I. (Ed.), Surface and Ground Water, Weathering and Soils. In: Holland, H.D., Turekian, K.K. (Eds.), Treatise on Geochemistry. vol. 5. Elsevier-Pergamon, Oxford, pp. 133-168.

Carbon Sequestration and Nitrogen Mineralization in Soil Cooperated with Organic Composts and Bio-char During Corn (Zea mays) Cultivation

NASA Astrophysics Data System (ADS)

Shin, Joung-Du; Lee, Sun-Ill; Park, Wu-Gyun; Choi, Yong-Su; Hong, Seong-Gil; Park, Sang-Won

2014-05-01

Objectives of this study were to estimate the carbon sequestration and to evaluate nitrogen mineralization and nitrification in soils cooperated with organic composts and bio-char during corn cultivation. For the experiment, the soil used in this study was clay loam types, and application rates of chemical fertilizer and bio-char were recommended amount after soil test and 2 % to soil weight, respectively. The soil samples were periodically taken at every 15 day intervals during the experimental periods. The treatments were consisted of non-application, cow manure compost, pig manure compost, swine digestate from aerobic digestion system, their bio-char cooperation. For the experimental results, residual amount of inorganic carbon was ranged from 51 to 208kg 10a-1 in soil only cooperated with different organic composts. However it was estimated to be highest at 208kg 10a-1 in the application plot of pig manure compost. In addition to bio-char application, it was ranged from 187.8 to 286kg 10a-1, but was greatest accumulated at 160.3kg 10a-1 in the application plot of cow manure compost. For nitrogen mineralization and nitrification rates, it was shown that there were generally low in the soil cooperated with bio-char compared to the only application plots of different organic composts except for 71 days after sowing. Also, they were observed to be highest in the application plot of swine digestate from aerobic digestion system. For the loss of total inorganic carbon (TIC) by run-off water, it was ranged from 0.18 to 0.36 kg 10a-1 in the different treatment plots. Also, with application of bio-char, total nitrogen was estimated to be reduced at 0.42(15.1%) and 0.38(11.8%) kg 10a-1 in application plots of the pig manure compost and aerobic digestate, respectively.

Effect of metal oxides on the stabilization of soil organic matter

NASA Astrophysics Data System (ADS)

Stelmach, Wioleta

2017-04-01

Soil organic matter (SOM) is protected from decomposition by three mechanisms: 1) biochemical stabilization through the accumulation of recalcitrant SOM compounds, 2) physical stabilization, i.e. spatial inaccessibility of SOM for microbes, and 3) chemical protection of SOM through intimate interaction with minerals and metal oxides. The latter mechanisms suggest that added organic substances (i.e. post-fermentation sludge) can be stabilized by metal oxides to increase C sequestration in soil. The aim of this study was to determine the effects of Fe2O3 - one of the dominant metal oxides in soil - on the sequestration of post-fermentation sludge C in soil by separately tracing the decomposition of sludge and of SOM to carbon dioxide (CO2). To determine changes in SOM turnover after the addition of post-fermentation sludge without/with Fe2O3, the isotopic signatures of both C sources (SOM and post-fermentation sludge) were used. Using differences in the 13C natural abundance of the soil (C3 originated, δ13C = -26) and the post-fermentation sludge (C4 originated, δ13C = -18), the CO2 fluxes arising from both C sources were tracked. Addition of post-fermentation sludge to the soil increased the CO2 production by 30% compared to soil without sludge. δ13C analysis of the total CO2 efflux revealed that post-fermentation sludge decreased SOM decomposition. Fe2O3 slightly suppressed sludge decomposition, and therefore increased C sequestration in soil. Only 30% of the post-fermentation sludge had been mineralized after one month of incubation in the soil. The collective results of my study reveal that application of post-fermentation sludge suppresses SOM decomposition, suggesting its use as a fertilizer could positively influence long-term soil quality. Finally, the success of the 13C natural abundance microcosm labeling approach in my study supports its use as an effective method of analyzing the effects of various fertilization techniques on soil nutrient retention. Such results were only possible by partitioning of the total CO2.

Final Technical Report. Reactivity of Iron-Bearing Minerals and CO 2 Sequestration and Surface Chemistry of Pyrite. An Interdisciplinary Approach

DOE Office of Scientific and Technical Information (OSTI.GOV)

Strongin, Daniel

2014-12-31

Over the course of the scientific program, two areas of research were pursued: reactions of iron oxides with supercritical CO 2 and sulfide and surface reactivity of pyrite. The latter area of interest was to understand the chemistry that results when supercritical CO 2 (scCO 2 ) with H 2 S and/or SO 2 in deep saline formations (DFS) contacts iron bearing minerals. Understanding the complexities the sulfur co-injectants introduce is a critical step in developing CO 2 sequestration as a climate-mitigating strategy. The research strategy was to understand macroscopic observations of this chemistry with anmore » atomic/molecular level view using surface analytical techniques. Research showed that the exposure of iron (oxyhdr)oxides (which included ferrihydrite, goethite, and hematite) to scCO 2 in the presence of sulfide led to reactions that formed siderite (FeCO 3). The results have important implications for the sequestration of CO 2 via carbonation reactions in the Earth’s subsurface. An earlier area of focus in the project was to understand pyrite oxidation in microscopic detail. This understanding was used to understand macroscopic observations of pyrite reactivity. Results obtained from this research led to a better understanding how pyrite reacts in a range of chemical environments. Geochemical and modern surface science techniques were used to understand the chemistry of pyrite in important environmental conditions. The program relied on a strong integration the results of these techniques to provide a fundamental understanding to the macroscopic chemistry exhibited by pyrite in the environment. Major achievements during these studies included developing an understanding of the surface sites on pyrite that controlled its reactivity under oxidizing conditions. In particular sulfur anion vacancies and/or ferric sites were sites of reactivity. Studies also showed that the adsorption of phospholipid on the surface to selectively suppress the reactivity of these sites could of potential importance for suppressing acid mine drainage in the environment (a problem common to coal-mining sites). Biotic studies showed that microbial activity that promotes the oxidation of pyrite to produce AMD could also be suppressed by the adsorption of phospholipid.« less

Modeling a CO2 mineralization experiment of fractured peridotite from the Semail ophiolite/ Oman

NASA Astrophysics Data System (ADS)

Muller, Nadja; Zhang, Guoxiang; van Noort, Reinier; Spiers, Chris; Ten Grotenhuis, Saskia; Hoedeman, Gerco

2010-05-01

Most geologic CO2 sequestration technologies focus on sedimentary rocks, where the carbon dioxide is stored in a fluid phase. A possible alternative is to trap it as a mineral in the subsurface (in-situ) in basaltic or even (ultra)mafic rocks. Carbon dioxide in aqueous solution reacts with Mg-, Ca-, and Fe-bearing silicate minerals, precipitates as (MgCa,Fe)CO3 (carbonate), and can thus be permanently sequestered. The cation donors are silicate minerals such as olivine and pyroxene which are abundant in (ultra)mafic rocks, such as peridotite. Investigations are underway to evaluate the sequestration potential of the Semail Ophiolite in Oman, utilizing the large volumes of partially serpentinized peridotite that are present. Key factors are the rate of mineralization due to dissolution of the peridotite and precipitation of carbonate, the extent of the natural and hydraulic fracture network and the accessibility of the rock to reactive fluids. To quantify the influence of dissolution rates on the overall CO2 mineralization process, small, fractured peridotite samples were exposed to supercritical CO2 and water in laboratory experiments. The samples are cored from a large rock sample in the dimension of small cylinders with 1 cm in height and diameter, with a mass of ~2g. Several experimental conditions were tested with different equipment, from large volume autoclave to small volume cold seal vessel. The 650 ml autoclave contained 400-500g of water and a sample under 10 MPa of partial CO2 pressure up to 150. The small capsules in the cold seal vessel held 1-1.5g of water and the sample under CO2 partial pressure from 15MPa to 70 MPa and temperature from 60 to 200°C. The samples remained for two weeks in the reaction vessels. In addition, bench acid bath experiments in 150 ml vials were performed open to the atmosphere at 50-80°C and pH of ~3. The main observation was that the peridotite dissolved two orders of magnitude slower in the high pressure and temperature cell of the cold seal vessel than comparative experiments in large volume autoclaves and bench acid bath vials under lower and atmospheric pressure conditions. We attributed this observation to the limited water availability in the cold seal vessel, limiting the aqueous reaction of bi-carbonate formation and magnesite precipitation. To test this hypothesis, one of the cold seal vessel experiments at 20 MPa and 100°C was simulated with a reactive transport model, using TOUGHREACT. To simulate the actual experimental conditions, the model used a grid on mm and 100's of μm scale and a fractured peridotite medium with serpentine filling the fractures. The simulation produced dissolution comparable to the experiment and showed an effective shut down of the bi-carbonation reaction within one day after the start of the experiment. If the conditions of limited water supply seen in our experiments are applicable in a field setting, we could expect dissolution may be limited by the buffering of the pH and shut down of the bi-carbonate formation. Under field conditions water and CO2 will only flow in hydraulic induced fractures and the natural fracture network that is filled with serpentine and some carbonate. The simulation result and potential implication for the field application will require further experimental investigation in the lab or field in the future.

Assessing the effect of climate change on carbon sequestration in a Mexican dry forest in the Yucatan Peninsula

Treesearch

Z. Dai; K.D. Johnson; R.A. Birdsey; J.L. Hernandez-Stefanoni; J.M. Dupuy

2015-01-01

Assessing the effect of climate change on carbon sequestration in tropical forest ecosystems is important to inform monitoring, reporting, and verification (MRV) for reducing deforestation and forest degradation (REDD), and to effectively assess forest management options under climate change. Two process-based models, Forest-DNDC and Biome-BGC, with different spatial...

A Multi-Level Approach to Outreach for Geologic Sequestration Projects

USGS Publications Warehouse

Greenberg, S.E.; Leetaru, H.E.; Krapac, I.G.; Hnottavange-Telleen, K.; Finley, R.J.

2009-01-01

Public perception of carbon capture and sequestration (CCS) projects represents a potential barrier to commercialization. Outreach to stakeholders at the local, regional, and national level is needed to create familiarity with and potential acceptance of CCS projects. This paper highlights the Midwest Geological Sequestration Consortium (MGSC) multi-level outreach approach which interacts with multiple stakeholders. The MGSC approach focuses on external and internal communication. External communication has resulted in building regional public understanding of CCS. Internal communication, through a project Risk Assessment process, has resulted in enhanced team communication and preparation of team members for outreach roles. ?? 2009 Elsevier Ltd. All rights reserved.

Potential soil carbon sequestration in overgrazed grassland ecosystems

NASA Astrophysics Data System (ADS)

Conant, Richard T.; Paustian, Keith

2002-12-01

Excessive grazing pressure is detrimental to plant productivity and may lead to declines in soil organic matter. Soil organic matter is an important source of plant nutrients and can enhance soil aggregation, limit soil erosion, and can also increase cation exchange and water holding capacities, and is, therefore, a key regulator of grassland ecosystem processes. Changes in grassland management which reverse the process of declining productivity can potentially lead to increased soil C. Thus, rehabilitation of areas degraded by overgrazing can potentially sequester atmospheric C. We compiled data from the literature to evaluate the influence of grazing intensity on soil C. Based on data contained within these studies, we ascertained a positive linear relationship between potential C sequestration and mean annual precipitation which we extrapolated to estimate global C sequestration potential with rehabilitation of overgrazed grassland. The GLASOD and IGBP DISCover data sets were integrated to generate a map of overgrazed grassland area for each of four severity classes on each continent. Our regression model predicted losses of soil C with decreased grazing intensity in drier areas (precipitation less than 333 mm yr-1), but substantial sequestration in wetter areas. Most (93%) C sequestration potential occurred in areas with MAP less than 1800 mm. Universal rehabilitation of overgrazed grasslands can sequester approximately 45 Tg C yr-1, most of which can be achieved simply by cessation of overgrazing and implementation of moderate grazing intensity. Institutional level investments by governments may be required to sequester additional C.

Preface

USGS Publications Warehouse

McPherson, Brian J.; Sundquist, Eric T.

2009-01-01

Carbon sequestration has emerged as an important option in policies to mitigate the increasing atmospheric concentrations of anthropogenic carbon dioxide (CO2). Significant quantities of anthropogenic CO2 are sequestered by natural carbon uptake in plants, soils, and the oceans. These uptake processes are objects of intense study by biogeochemists, ecologists, and other researchers who seek to understand the processes that determine the mass balance (“budget”) among global carbon fluxes. At the same time, many scientists and engineers are examining methods for deliberate carbon sequestration through storage in plants, soils, the oceans, and geological formations.

Robust CO2 Injection: Application of Bayesian-Information-Gap Decision Theory

NASA Astrophysics Data System (ADS)

Grasinger, M.; O'Malley, D.; Vesselinov, V. V.; Karra, S.

2015-12-01

Carbon capture and sequestration has the potential to reduce greenhouse gasemissions. However, care must be taken when choosing a site for CO2 seques-tration to ensure that the CO2 remains sequestered for many years, and thatthe environment is not harmed in any way. Making a rational decision be-tween potential sites for sequestration is not without its challenges because, asin the case of many environmental and subsurface problems, there is a lot ofuncertainty that exists. A method for making decisions under various typesand severities of uncertainty, Bayesian-Information-Gap Decision Theory (BIGDT), is presented. BIG DT was coupled with a numerical model for CO2 wellinjection and the resulting framework was then applied to a problem of selectingbetween two potential sites for CO2 sequestration. The results of the analysisare presented, followed by a discussion of the decision process.

Upscaling of reaction rates in reactive transport using pore-scale reactive transport model

NASA Astrophysics Data System (ADS)

Yoon, H.; Dewers, T. A.; Arnold, B. W.; Major, J. R.; Eichhubl, P.; Srinivasan, S.

2013-12-01

Dissolved CO2 during geological CO2 storage may react with minerals in fractured rocks, confined aquifers, or faults, resulting in mineral precipitation and dissolution. The overall rate of reaction can be affected by coupled processes among hydrodynamics, transport, and reactions at the (sub) pore-scale. In this research pore-scale modeling of coupled fluid flow, reactive transport, and heterogeneous reaction at the mineral surface is applied to account for permeability alterations caused by precipitation-induced pore-blocking. This work is motivated by the observed CO2 seeps from a natural analog to geologic CO2 sequestration at Crystal Geyser, Utah. A key observation is the lateral migration of CO2 seep sites at a scale of ~ 100 meters over time. A pore-scale model provides fundamental mechanistic explanations of how calcite precipitation alters flow paths by pore plugging under different geochemical compositions and pore configurations. In addition, response function of reaction rates will be constructed from pore-scale simulations which account for a range of reaction regimes characterized by the Damkohler and Peclet numbers. Newly developed response functions will be used in a continuum scale model that may account for large-scale phenomena mimicking lateral migration of surface CO2 seeps. Comparison of field observations and simulations results will provide mechanistic explanations of the lateral migration and enhance our understanding of subsurface processes associated with the CO2 injection. This work is supported as part of the Center for Frontiers of Subsurface Energy Security, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001114. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.

Electrical Resistance Tomography Field Trials to Image CO2 Sequestration

NASA Astrophysics Data System (ADS)

Newmark, R.

2003-12-01

If geologic formations are used to sequester or store carbon dioxide (CO2) for long periods of time, it will be necessary to verify the containment of injected CO2 by assessing leaks and flow paths, and by understanding the geophysical and geochemical interactions between the CO2 and the geologic minerals and fluids. Remote monitoring methods are preferred, to minimize cost and impact to the integrity of the disposal reservoir. Electrical methods are especially well suited for monitoring processes involving fluids, as electrical properties are most sensitive to the presence and nature of the fluids contained in the medium. High resolution tomographs of electrical properties have been used with success for site characterization, monitoring subsurface migration of fluids in instances of leaking underground tanks, water infiltration events, subsurface steam floods, contaminant movement, and assessing the integrity of subsurface barriers. These surveys are commonly conducted utilizing vertical arrays of point electrodes in a crosswell configuration. Alternative ways of monitoring the reservoir are desirable due to the high costs of drilling the required monitoring boreholes Recent field results obtained using steel well casings as long electrodes are also promising. We have conducted field trials to evaluate the effectiveness of long electrode ERT as a potential monitoring approach for CO2 sequestration. In these trials, CO2 is not being sequestered but rather is being used as a solvent for enhanced oil recovery. This setting offers the same conditions expected during sequestration so monitoring secondary oil recovery allows a test of the method under realistic physical conditions and operational constraints. Field experience has confirmed the challenges identified during model studies. The principal difficulty are the very small signals due to the fact that formation changes occur only over a small segment of the 5000 foot length of the electrodes. In addition, telluric noise can be comparable to the signal levels during periods of geomagnetic activity. Finally, instrumentation stability over long periods is necessary to follow trends in reservoir behavior for several years. Solutions to these and other problems will be presented along with results from the first two years of work at a producing field undergoing CO2 flood. If electrical resistance tomography (ERT) imaging can be performed using existing well casings as long electrodes, it will substantially reduce the cost to monitor CO2 sequestration. This work was performed under the auspices of the U.S. Department of Energy by University of California Lawrence Livermore National Laboratory under contract No. W-7405-Eng-48.

Carbon Capture and Storage

DOE Office of Scientific and Technical Information (OSTI.GOV)

Friedmann, S

2007-10-03

Carbon capture and sequestration (CCS) is the long-term isolation of carbon dioxide from the atmosphere through physical, chemical, biological, or engineered processes. This includes a range of approaches including soil carbon sequestration (e.g., through no-till farming), terrestrial biomass sequestration (e.g., through planting forests), direct ocean injection of CO{sub 2} either onto the deep seafloor or into the intermediate depths, injection into deep geological formations, or even direct conversion of CO{sub 2} to carbonate minerals. Some of these approaches are considered geoengineering (see the appropriate chapter herein). All are considered in the 2005 special report by the Intergovernmental Panel on Climatemore » Change (IPCC 2005). Of the range of options available, geological carbon sequestration (GCS) appears to be the most actionable and economic option for major greenhouse gas reduction in the next 10-30 years. The basis for this interest includes several factors: (1) The potential capacities are large based on initial estimates. Formal estimates for global storage potential vary substantially, but are likely to be between 800 and 3300 Gt of C (3000 and 10,000 Gt of CO{sub 2}), with significant capacity located reasonably near large point sources of the CO{sub 2}. (2) GCS can begin operations with demonstrated technology. Carbon dioxide has been separated from large point sources for nearly 100 years, and has been injected underground for over 30 years (below). (3) Testing of GCS at intermediate scale is feasible. In the US, Canada, and many industrial countries, large CO{sub 2} sources like power plants and refineries lie near prospective storage sites. These plants could be retrofit today and injection begun (while bearing in mind scientific uncertainties and unknowns). Indeed, some have, and three projects described here provide a great deal of information on the operational needs and field implementation of CCS. Part of this interest comes from several key documents written in the last three years that provide information on the status, economics, technology, and impact of CCS. These are cited throughout this text and identified as key references at the end of this manuscript. When coupled with improvements in energy efficiency, renewable energy supplies, and nuclear power, CCS help dramatically reduce current and future emissions (US CCTP 2005, MIT 2007). If CCS is not available as a carbon management option, it will be much more difficult and much more expensive to stabilize atmospheric CO{sub 2} emissions. Recent estimates put the cost of carbon abatement without CCS to be 30-80% higher that if CCS were to be available (Edmonds et al. 2004).« less

Accelerating Technology Development through Integrated Computation and Experimentation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shekhawat, Dushyant; Srivastava, Rameshwar D.; Ciferno, Jared

2013-08-15

This special section of Energy & Fuels comprises a selection of papers presented at the topical conference “Accelerating Technology Development through Integrated Computation and Experimentation”, sponsored and organized by the United States Department of Energy’s National Energy Technology Laboratory (NETL) as part of the 2012 American Institute of Chemical Engineers (AIChE) Annual Meeting held in Pittsburgh, PA, Oct 28-Nov 2, 2012. That topical conference focused on the latest research and development efforts in five main areas related to fossil energy, with each area focusing on the utilization of both experimental and computational approaches: (1) gas separations (membranes, sorbents, and solventsmore » for CO{sub 2}, H{sub 2}, and O{sub 2} production), (2) CO{sub 2} utilization (enhanced oil recovery, chemical production, mineralization, etc.), (3) carbon sequestration (flow in natural systems), (4) advanced power cycles (oxy-combustion, chemical looping, gasification, etc.), and (5) fuel processing (H{sub 2} production for fuel cells).« less

Methods to Reduce Forest Residue Volume after Timber Harvesting and Produce Black Carbon

PubMed Central

Busse, Matt D.; Archuleta, James G.; McAvoy, Darren; Roussel, Eric

2017-01-01

Forest restoration often includes thinning to reduce tree density and improve ecosystem processes and function while also reducing the risk of wildfire or insect and disease outbreaks. However, one drawback of these restoration treatments is that slash is often burned in piles that may damage the soil and require further restoration activities. Pile burning is currently used on many forest sites as the preferred method for residue disposal because piles can be burned at various times of the year and are usually more controlled than broadcast burns. In many cases, fire can be beneficial to site conditions and soil properties, but slash piles, with a large concentration of wood, needles, forest floor, and sometimes mineral soil, can cause long-term damage. We describe several alternative methods for reducing nonmerchantable forest residues that will help remove excess woody biomass, minimize detrimental soil impacts, and create charcoal for improving soil organic matter and carbon sequestration. PMID:28377830

An Impact of Mechanical Stress in Coal Briquettes on Sorption of Carbon Dioxide

NASA Astrophysics Data System (ADS)

Wierzbicki, Mirosław

2017-09-01

The presence of gases (methane or carbon dioxide) in hard coal is connected with numerous threats for miners employed in underground mining facilities. When analyzing the coal-methane system, it is necessary to determine the relationship between pressure and gas sorption. Such a relationship should be determined under conditions similar to the natural ones - when it comes to both temperature and pressure. The present paper discusses the results of research conducted with the use of coal briquettes under the state of mechanical stress. Carbon dioxide sorption isotherms were determined for different values of stress affecting the coal material. For five coal samples collected in different mines of the Upper Silesian Coal Basin, Langmuir's sorption isotherms were determined. The results point to significant impact that mechanical stress has upon the sorption process. It is about 1 percent of the value obtained for coal not subjected to stress per 1 MPa. The research results can also prove useful when analyzing hard coal seams from the perspective of their carbon dioxide sequestration abilities.

Long Time Evolution of Sequestered CO2 in Porous Media

NASA Astrophysics Data System (ADS)

Cohen, Y.; Rothman, D.

2013-12-01

CO2 sequestration is important for mitigating climate change and reducing atmospheric CO2 concentration. However, a complete physical picture able to predict both the pattern formation and the structure developing within the porous medium is lacking. We propose a theoretical model that couples transport, reaction, and the intricate geometry of the rock, in order to study the long time evolution of carbon in the brine-rock environment. As CO2 is injected into a brine-rock environment, it becomes initially trapped, and isolated bubbles are formed. Within the high CO2 phase, minerals dissolve and migrate from high concentration to low concentration regions, along with other carbonate species. The change in the concentrations at the interface moves the system out of equilibrium, drives up the saturation level, and leads to mineral precipitation. We argue that mineral precipitation in a small boundary layer may lead to lower diffusivity, slower kinetics, and eventually to a mechanical trapping of the CO2 bubbles. We investigate the reactive transport model and study the conditions that cause the mechanical separation of these two reactive fluids in porous media.

Adsorption of Dissolved Gases (CH4, CO2, H2, Noble Gases) by Water-Saturated Smectite Clay Minerals

NASA Astrophysics Data System (ADS)

Bourg, I. C.; Gadikota, G.; Dazas, B.

2016-12-01

Adsorption of dissolved gases by water-saturated clay minerals plays important roles in a range of fields. For example, gas adsorption in on clay minerals may significantly impact the formation of CH4 hydrates in fine-grained sediments, the behavior of CH4 in shale, CO2 leakage across caprocks of geologic CO2 sequestration sites, H2 leakage across engineered clay barriers of high-level radioactive waste repositories, and noble gas geochemistry reconstructions of hydrocarbon migration in the subsurface. Despite its importance, the adsorption of gases on clay minerals remains poorly understood. For example, some studies have suggested that clay surfaces promote the formation of CH4 hydrates, whereas others indicate that clay surfaces inhibit the formation of CH4 hydrates. Here, we present molecular dynamics (MD) simulations of the adsorption of a range of gases (CH4, CO2, H2, noble gases) on clay mineral surfaces. Our results indicate that the affinity of dissolved gases for clay mineral surfaces has a non-monotone dependence on the hydrated radius of the gas molecules. This non-monotone dependence arises from a combination of two effects: the polar nature of certain gas molecules (in particular, CO2) and the templating of interfacial water structure by the clay basal surface, which results in the presence of interfacial water "cages" of optimal size for intermediate-size gas molecules (such as Ne or Ar).

Improved chemometric methodologies for the assessment of soil carbon sequestration mechanisms

NASA Astrophysics Data System (ADS)

Jiménez-González, Marco A.; Almendros, Gonzalo; Álvarez, Ana M.; González-Vila, Francisco J.

2016-04-01

The factors involved soil C sequestration, which is reflected in the highly variable content of organic matter in the soils, are not yet well defined. Therefore, their identification is crucial for understanding Earth's biogeochemical cycle and global change. The main objective of this work is to contribute to a better qualitative and quantitative assessment of the mechanisms of organic C sequestration in the soil, using omic approaches not requiring the detailed knowledge of the structure of the material under study. With this purpose, we have carried out a series of chemometric approaches on a set of widely differing soils (35 representative ecosystems). In an exploratory phase, we used multivariate statistical models (e.g., multidimensional scaling, discriminant analysis with automatic backward variable selection…) to analyze arrays of more than 200 independent soil variables (physicochemical, spectroscopic, pyrolytic...) in order to select those factors (descriptors or proxies) that explain most of the total system variance (content and stability of the different C forms). These models showed that the factors determining the stabilization of organic material are greatly dependent on the soil type. In some cases, the molecular structure of organic matter seemed strongly correlated with their resilience, while in other soil types the organo-mineral interactions played a significant bearing on the accumulation of selectively preserved C forms. In any case, it was clear that the factors driving the resilience of organic matter are manifold and not exclusive. Consequently, in a second stage, prediction models of the soil C content and their biodegradability (laboratory incubation experiments) were carried out by massive data processing by partial least squares (PLS) regression of data from Py-GC-MS and Py-MS. In some models, PLS was applied to a matrix of 150 independent variables corresponding to major pyrolysis compounds (peak areas) from the 35 samples of whole soils. The variable importance in the projection (VIP) histogram obtained from this treatment (total C and total mineralization coefficients as dependent variables) illustrated the contribution of the individual compounds to the total inertia of the models (e.g., carbohydrate-derived compounds, methoxyphenols, or specific alkylbenzenes were relevant in explaining the total quality and the biodegradation rates of the organic matter). Further simplified models consisting of direct PLS analysis of the debugged ion matrix calculated by averaging all ions (45 - 250 amu) in the whole chromatographic area in the 5-60 min range (here referred to as 'rebuilt MS spectra' or 'Py-MS spectra' when obtained connecting directly the pyrolyser to the MS detector through suitable interfaces) were carried out. The above three approaches coincided in pointing out that C sequestration behave as an emergent soil property depending on the complexity of its progressive molecular levels. Most of the total variance is explained by specific assemblages of variables, strongly depending on the soil types. On the other hand, chemical biodiversity (e.g., Shannon indices or coefficients from multivariate data models) behaved as a common background in the prediction models including very different soil types. In fact, assessment of chemodiversity of the pyrolytic compound assemblages (or the Py-MS ion data) would represent a valid clue for the assessment of the extent to which the original biomass has been diagenetically reworked into chaotic structures with non-repeatable units, providing a useful proxy to forecast at least a portion of the total variance in the soil organic matter biodegradability.

By-products of the serpentinization process on the Oman ophiolite : chemical and isotopic composition of carbonate deposits in alkaline springs, and associated secondary phases

NASA Astrophysics Data System (ADS)

Sissmann, O.; Martinez, I.; Deville, E.; Beaumont, V.; Pillot, D.; Prinzhofer, A.; Vacquand, C.; Chaduteau, C.; Agrinier, P.; Guyot, F. J.

2014-12-01

The isotopic compositions (d13C, d18O) of natural carbonates produced by the alteration of basic and ultrabasic rocks on the Oman ophiolite have been measured in order to better understand their formation mechanisms. Fossil carbonates developed on altered peridotitic samples, mostly found in fractures, and contemporary carbonates were studied. The samples bear a large range of d13C. Those collected in veins are magnesian (magnesite, dolomite) and have a carbon signature reflecting mixing of processes and important fractionation (-11‰ to 8‰). Their association with talc and lizardite suggests they are by-products of a serpentinization process, that must have occurred as a carbon-rich fluid was circulating at depth. On the other hand, the carbonates are mostly calcic when formed in alkaline springs, most of which are located in the vicinity of lithological discontinuities such as the peridotite-gabbro contact (Moho). Aragonite forms a few meters below the surface of the ponds in Mg-poor water, and is systematically associated with brucite (Mg(OH)2). This suggests most of the Mg dissolved at depth has reprecipitated during the fluid's ascension through fractures or faults as carbonates and serpentine. Further up, on the surface waters of the ponds (depleted in Mg and D.I.C.), thin calcite films precipitate and reach extremely negative d13C values (-28‰), which could reflect either a biological carbon source, or kinetic fractionation from pumping atmospheric CO2. Their formation represent an efficient and natural process for carbon dioxide mineral sequestration. The d18O signature from all samples confirm the minerals crystallized from a low-temperature fluid. The hyperalkaline conditions (pH between 11 and 12) allowing for these fast precipitation kinetics are generated by the serpentinization process occurring at depth, as indicated by the measured associated H2-rich gas flows (over 50%) seeping out to the surface.

CO2 hydrate nucleation kinetics enhanced by an organo-mineral complex formed at the montmorillonite-water interface.

PubMed

Kyung, Daeseung; Lim, Hyung-Kyu; Kim, Hyungjun; Lee, Woojin

2015-01-20

In this study, we investigated experimentally and computationally the effect of organo-mineral complexes on the nucleation kinetics of CO2 hydrate. These complexes formed via adsorption of zwitter-ionic glycine (Gly-zw) onto the surface of sodium montmorillonite (Na-MMT). The electrostatic attraction between the −NH3(+) group of Gly-zw, and the negatively charged Na-MMT surface, provides the thermodynamic driving force for the organo-mineral complexation. We suggest that the complexation of Gly-zw on the Na-MMT surface accelerates CO2 hydrate nucleation kinetics by increasing the mineral–water interfacial area (thus increasing the number of effective hydrate-nucleation sites), and also by suppressing the thermal fluctuation of solvated Na(+) (a well-known hydrate formation inhibitor) in the vicinity of the mineral surface by coordinating with the −COO(–) groups of Gly-zw. We further confirmed that the local density of hydrate-forming molecules (i.e., reactants of CO2 and water) at the mineral surface (regardless of the presence of Gly-zw) becomes greater than that of bulk phase. This is expected to promote the hydrate nucleation kinetics at the surface. Our study sheds new light on CO2 hydrate nucleation kinetics in heterogeneous marine environments, and could provide knowledge fundamental to successful CO2 sequestration under seabed sediments.

Distribution of nitrogen-15 tracers applied to the canopy of a mature spruce-hemlock stand, Howland, Maine, USA

Treesearch

David Bryan Dail; David Y. Hollinger; Eric A. Davidson; Ivan Fernandez; Herman C. Sievering; Neal A. Scott; Elizabeth Gaige

2009-01-01

In N-limited ecosystems, fertilization by N deposition may enhance plant growth and thus impact C sequestration. In many N deposition-C sequestration experiments, N is added directly to the soil, bypassing canopy processes and potentially favoring N immobilization by the soil. To understand the impact of enhanced N deposition on a low fertility unmanaged forest and...

Final Scientific/Technical Report--In-Situ Generation of Iron-Chromium Precipitates for Long Term Immobilization of Chromium at the Hanford Site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Butler, Elizabeth C.; Krumholz, Lee R.; Madden, Andrew S.

Hexavalent chromium (Cr(VI)) is a toxic ground water contaminant widespread at the Hanford site and many other industrial facilities. A common remediation method for Cr(VI) is in situ reduction/immobilization, in which soluble Cr(VI) is reduced to the less soluble trivalent Cr (Cr(III)). If iron (Fe) minerals are present during the process, Cr(III) precipitates as a mixed Fe(III)-Cr(III) (Fe-Cr) solid. The objective of this exploratory research was to obtain preliminary evidence about the relationships among the method of Cr(VI) reduction (i.e., abiotic or microbial), the properties of the resulting Fe-Cr precipitates, and their tendencies to release soluble Cr(VI) in the presencemore » of the common manganese oxide birnessite. The results of this exploratory research project show that the conditions of Cr(VI) reduction—specifically the ratio of Cr to Fe, and/or whether the Cr(VI) reductant is a mineral or a microorganism—can significantly affect the tendency of the resulting Fe-Cr precipitate to release Cr(VI) to the environment in the presence of birnessite. These results suggest the chosen remediation conditions have the potential to strongly influence not only the initial success of in situ Cr(VI) reduction/immobilization, but also the potential for successful long term sequestration of Cr in the form of stable soil precipitates.« less

Cycling of oxyanion-forming trace elements in groundwaters from a freshwater deltaic marsh

NASA Astrophysics Data System (ADS)

Telfeyan, Katherine; Breaux, Alexander; Kim, Jihyuk; Kolker, Alexander S.; Cable, Jaye E.; Johannesson, Karen H.

2018-05-01

Pore waters and surface waters were collected from a freshwater system in southeastern Louisiana to investigate the geochemical cycling of oxyanion-forming trace elements (i.e., Mo, W, As, V). A small bayou (Bayou Fortier) receives input from a connecting lake (Lac des Allemands) and groundwater input at the head approximately 5 km directly south of the Mississippi River. Marsh groundwaters exchange with bayou surface water but are otherwise relatively isolated from outside hydrologic forcings, such as tides, storms, and effects from local navigation canals. Rather, redox processes in the marsh groundwaters appear to drive changes in trace element concentrations. Elevated dissolved S(-II) concentrations in marsh groundwaters suggest greater reducing conditions in the late fall and winter as compared to the spring and late summer. The data suggest that reducing conditions in marsh groundwaters initiate the dissolution of Fe(III)/Mn(IV) oxide/hydroxide minerals, which releases adsorbed and/or co-precipitated trace elements into solution. Once in solution, the fate of these elements is determined by complexation with aqueous species and precipitation with iron sulfide minerals. The trace elements remain soluble in the presence of Fe(III)- and SO42-- reducing conditions, suggesting that either kinetic limitations or complexation with aqueous ligands obfuscates the correlation between V and Mo sequestration in sediments with reducing or euxinic conditions.

Biodegradation of organic chemicals in soil/water microcosms system: Model development

USGS Publications Warehouse

Liu, L.; Tindall, J.A.; Friedel, M.J.; Zhang, W.

2007-01-01

The chemical interactions of hydrophobic organic contaminants with soils and sediments may result in strong binding and slow subsequent release rates that significantly affect remediation rates and endpoints. In order to illustrate the recalcitrance of chemical to degradation on sites, a sorption mechanism of intraparticle sequestration was postulated to operate on chemical remediation sites. Pseudo-first order sequestration kinetics is used in the study with the hypothesis that sequestration is an irreversibly surface-mediated process. A mathematical model based on mass balance equations was developed to describe the fate of chemical degradation in soil/water microcosm systems. In the model, diffusion was represented by Fick's second law, local sorption-desorption by a linear isotherm, irreversible sequestration by a pseudo-first order kinetics and biodegradation by Monod kinetics. Solutions were obtained to provide estimates of chemical concentrations. The mathematical model was applied to a benzene biodegradation batch test and simulated model responses correlated well compared to measurements of biodegradation of benzene in the batch soil/water microcosm system. A sensitivity analysis was performed to assess the effects of several parameters on model behavior. Overall chemical removal rate decreased and sequestration increased quickly with an increase in the sorption partition coefficient. When soil particle radius, a, was greater than 1 mm, an increase in radius produced a significant decrease in overall chemical removal rate as well as an increase in sequestration. However, when soil particle radius was less than 0.1 mm, an increase in radius resulted in small changes in the removal rate and sequestration. As pseudo-first order sequestration rate increased, both chemical removal rate and sequestration increased slightly. Model simulation results showed that desorption resistance played an important role in the bioavailability of organic chemicals in porous media. Complete biostabilization of chemicals on remediation sites can be achieved when the concentration of the reversibly sorbed chemical reduces to zero (i.e., undetectable), with a certain amount of irreversibly sequestrated chemical left inside the soil particle solid phase. ?? 2006 Springer Science + Business Media B.V.

Carbonate control of H2 and CH4 production in serpentinization systems at elevated P-Ts

USGS Publications Warehouse

Jones, L. Camille; Rosenbauer, Robert; Goldsmith, Jonas I.; Oze, Christopher

2010-01-01

Serpentinization of forsteritic olivine results in the inorganic synthesis of molecular hydrogen (H2) in ultramafic hydrothermal systems (e.g., mid-ocean ridge and forearc environments). Inorganic carbon in those hydrothermal systems may react with H2 to produce methane (CH4) and other hydrocarbons or react with dissolved metal ions to form carbonate minerals. Here, we report serpentinization experiments at 200°C and 300 bar demonstrating Fe2+ being incorporated into carbonates more rapidly than Fe2+ oxidation (and concomitant H2 formation) leading to diminished yields of H2 and H2-dependent CH4. In addition, carbonate formation is temporally fast in carbonate oversaturated fluids. Our results demonstrate that carbonate chemistry ultimately modulates the abiotic synthesis of both H2 and CH4 in hydrothermal ultramafic systems and that ultramafic systems present great potential for CO2-mineral sequestration.

Geochemical behavior of ultramafic waste rocks with carbon sequestration potential: a case study of the Dumont Nickel Project, Amos, Québec.

PubMed

Kandji, El Hadji Babacar; Plante, Benoit; Bussière, Bruno; Beaudoin, Georges; Dupont, Pierre-Philippe

2017-04-01

The geochemical behavior of ultramafic waste rocks and the effect of carbon sequestration by these waste rocks on the water drainage quality were investigated using laboratory-scale kinetic column tests on samples from the Dumont Nickel Project (RNC Minerals, QC, Canada). The test results demonstrated that atmospheric CO 2 dissolution induced the weathering of serpentine and brucite within the ultramafic rocks, generating high concentrations of Mg and HCO 3 - with pH values ranging between 9 and 10 in the leachates that promote the precipitation of secondary Mg carbonates. These alkaline pH values appear to have prevented the mobilization of many metals; Fe, Ni, Cu, and Zn were found at negligible concentrations in the leachates. Posttesting characterization using chemical analyses, diffuse reflectance infrared Fourier transform (DRIFT), and scanning electron microscope (SEM) observations confirmed the precipitation of secondary hydrated Mg carbonates as predicted by thermodynamic calculations. The formation of secondary Mg carbonates induced cementation of the waste particles, resulting in the development of a hardpan.

Simulation of reactive transport of injected CO2 on the Colorado Plateau, Utah, USA

USGS Publications Warehouse

White, S.P.; Allis, R.G.; Moore, J.; Chidsey, T.; Morgan, C.; Gwynn, W.; Adams, M.

2005-01-01

This paper investigates injection of CO2 into non-dome-shaped geological structures that do not provide the traps traditionally deemed necessary for the development of artificial CO2 reservoirs. We have developed a conceptual and two numerical models of the geology and groundwater along a cross-section lying approximately NW-SE and in the vicinity of the Hunter power station on the Colorado Plateau, Central Utah and identified a number of potential sequestration sites on this cross-section. Preliminary modeling identified the White Rim Sandstone as appearing to offer the properties required of a successful sequestration site. Detailed modeling of injection of CO2 into the White Rim Sandstone using the reactive chemical simulator ChemTOUGH found that 1000 years after the 30 year injection period began approximately 21% of the injected CO2 was permanently sequestered as a mineral, 52% was beneath the ground surface as a gas or dissolved in the groundwater and 17% had leaked to the surface and leakage to the surface was continuing. ?? 2005 Elsevier B.V. All rights reserved.

On a clean power generation system with the co-gasification of biomass and coal in a quadruple fluidized bed gasifier.

PubMed

Yan, Linbo; He, Boshu

2017-07-01

A clean power generation system was built based on the steam co-gasification of biomass and coal in a quadruple fluidized bed gasifier. The chemical looping with oxygen uncoupling technology was used to supply oxygen for the calciner. The solid oxide fuel cell and the steam turbine were combined to generate power. The calcium looping and mineral carbonation were used for CO 2 capture and sequestration. The aim of this work was to study the characteristics of this system. The effects of key operation parameters on the system total energy efficiency (ŋ ten ), total exergy efficiency (ŋ tex ) and carbon sequestration rate (R cs ) were detected. The energy and exergy balance calculations were implemented and the corresponding Sankey and Grassmann diagrams were drawn. It was found that the maximum energy and exergy losses occurred in the steam turbine. The system ŋ ten and ŋ tex could be ∼50% and ∼47%, and R cs could be over unit. Copyright © 2017 Elsevier Ltd. All rights reserved.

Carbon Sequestration Estimation of Street Trees Based on Point Cloud from Vehicle-Borne Laser Scanning System

NASA Astrophysics Data System (ADS)

Zhao, Y.; Hu, Q.

2017-09-01

Continuous development of urban road traffic system requests higher standards of road ecological environment. Ecological benefits of street trees are getting more attention. Carbon sequestration of street trees refers to the carbon stocks of street trees, which can be a measurement for ecological benefits of street trees. Estimating carbon sequestration in a traditional way is costly and inefficient. In order to solve above problems, a carbon sequestration estimation approach for street trees based on 3D point cloud from vehicle-borne laser scanning system is proposed in this paper. The method can measure the geometric parameters of a street tree, including tree height, crown width, diameter at breast height (DBH), by processing and analyzing point cloud data of an individual tree. Four Chinese scholartree trees and four camphor trees are selected for experiment. The root mean square error (RMSE) of tree height is 0.11m for Chinese scholartree and 0.02m for camphor. Crown widths in X direction and Y direction, as well as the average crown width are calculated. And the RMSE of average crown width is 0.22m for Chinese scholartree and 0.10m for camphor. The last calculated parameter is DBH, the RMSE of DBH is 0.5cm for both Chinese scholartree and camphor. Combining the measured geometric parameters and an appropriate carbon sequestration calculation model, the individual tree's carbon sequestration will be estimated. The proposed method can help enlarge application range of vehicle-borne laser point cloud data, improve the efficiency of estimating carbon sequestration, construct urban ecological environment and manage landscape.

Sequestration and Distribution Characteristics of Cd(II) by Microcystis aeruginosa and Its Role in Colony Formation.

PubMed

Bi, Xiangdong; Yan, Ran; Li, Fenxiang; Dai, Wei; Jiao, Kewei; Zhou, Qixing; Liu, Qi

2016-01-01

To investigate the sequestration and distribution characteristics of Cd(II) by Microcystis aeruginosa and its role in Microcystis colony formation, M. aeruginosa was exposed to six different Cd(II) concentrations for 10 days. Cd(II) exposure caused hormesis in the growth of M. aeruginosa . Low concentrations of Cd(II) significantly induced formation of small Microcystis colonies ( P < 0.05) and increased the intracellular polysaccharide (IPS) and bound extracellular polysaccharide (bEPS) contents of M. aeruginosa significantly ( P < 0.05). There was a linear relationship between the amount of Cd(II) sequestrated by algal cells and the amount added to cultures in the rapid adsorption process that occurred during the first 5 min of exposure. After 10 d, M. aeruginosa sequestrated nearly 80% of 0.2 mg L -1 added Cd(II), while >93% of Cd(II) was sequestrated in the groups with lower added concentrations of Cd(II). More than 80% of the sequestrated Cd(II) was bioadsorbed by bEPS. The Pearson correlation coefficients of exterior and interior factors related to colony formation of M. aeruginosa revealed that Cd(II) could stimulate the production of IPS and bEPS via increasing Cd(II) bioaccumulation and bioadsorption. Increased levels of cross-linking between Cd(II) and bEPS stimulated algal cell aggregation, which eventually promoted the formation of Microcystis colonies.

Sequestration and Distribution Characteristics of Cd(II) by Microcystis aeruginosa and Its Role in Colony Formation

PubMed Central

Bi, Xiangdong; Yan, Ran; Li, Fenxiang; Dai, Wei; Jiao, Kewei; Liu, Qi

2016-01-01

To investigate the sequestration and distribution characteristics of Cd(II) by Microcystis aeruginosa and its role in Microcystis colony formation, M. aeruginosa was exposed to six different Cd(II) concentrations for 10 days. Cd(II) exposure caused hormesis in the growth of M. aeruginosa. Low concentrations of Cd(II) significantly induced formation of small Microcystis colonies (P < 0.05) and increased the intracellular polysaccharide (IPS) and bound extracellular polysaccharide (bEPS) contents of M. aeruginosa significantly (P < 0.05). There was a linear relationship between the amount of Cd(II) sequestrated by algal cells and the amount added to cultures in the rapid adsorption process that occurred during the first 5 min of exposure. After 10 d, M. aeruginosa sequestrated nearly 80% of 0.2 mg L−1 added Cd(II), while >93% of Cd(II) was sequestrated in the groups with lower added concentrations of Cd(II). More than 80% of the sequestrated Cd(II) was bioadsorbed by bEPS. The Pearson correlation coefficients of exterior and interior factors related to colony formation of M. aeruginosa revealed that Cd(II) could stimulate the production of IPS and bEPS via increasing Cd(II) bioaccumulation and bioadsorption. Increased levels of cross-linking between Cd(II) and bEPS stimulated algal cell aggregation, which eventually promoted the formation of Microcystis colonies. PMID:27777956

In Vitro Assessment of Uptake and Lysosomal Sequestration of Respiratory Drugs in Alveolar Macrophage Cell Line NR8383.

PubMed

Ufuk, Ayşe; Somers, Graham; Houston, J Brian; Galetin, Aleksandra

2015-12-01

To assess accumulation and lysosomal sequestration of 9 drugs used in respiratory indications (plus imipramine as positive control) in the alveolar macrophage (AM) cell line NR8383. For all drugs, uptake at 5 μM was investigated at 37 and 4°C to delineate active uptake and passive diffusion processes. Accumulation of basic clarithromycin, formoterol and imipramine was also assessed over 0.1-100 μM concentration range. Lysosomal sequestration was investigated using ammonium chloride (NH4Cl), monensin and nigericin. Impact of lysosomal sequestration on clarithromycin accumulation kinetics was investigated. Both cell-to-medium concentration ratio (Kp) and uptake clearance (CLuptake) ranged > 400-fold for the drugs investigated. The greatest Kp was observed for imipramine (391) and clarithromycin (82), in contrast to no accumulation seen for terbutaline. A concentration-dependent accumulation was evident for the basic drugs investigated. Imipramine and clarithromycin Kp and CLuptake were reduced by 59-85% in the presence of NH4Cl and monensin/nigericin, indicating lysosomal accumulation, whereas lysosomal sequestration was not pronounced for the other 8 respiratory drugs. Clarithromycin uptake rate was altered by NH4Cl, highlighting the impact of subcellular distribution on accumulation kinetics. This study provides novel evidence of the utility of NR8383 for investigating accumulation and lysosomal sequestration of respiratory drugs in AMs.

Carbon sequestration in croplands is mainly driven by management leading to increased net primary production - evidence from long-term field experiments in Northern Europe

NASA Astrophysics Data System (ADS)

Kätterer, Thomas; Bolinder, Martin Anders; Börjesson, Gunnar; Kirchmann, Holger; Poeplau, Christopher

2014-05-01

Sustainable intensification of agriculture in regions with high production potential is a prerequisite for providing services for an increasing human population, not only food, animal feed, fiber and biofuel but also to promote biodiversity and the beauty of landscapes. We investigated the effect of different management practices on soil fertility and carbon sequestration in long-term experiments, mainly from Northern Europe. In addition, a meta-analysis on the effect of catch crops was conducted. Improved management of croplands was found to be a win-win strategy resulting in both increased soil fertility and carbon sequestration. We quantified the effect of different management practices such as N fertilization, organic amendments, catch crops and ley-arable rotations versus continuous annual cropping systems on soil carbon stocks. Increasing net primary productivity (NPP) was found to be the main driver for higher soil carbon storage. Mineral N fertilization increased soil carbon stocks by 1-2 kg C ha-1 for each kg of N applied to cropland. Ley-arable rotations, being a combination of annual and perennial crops, are expected to have C stocks intermediate between those of continuous grass- and croplands. A summary of data from 15 long-term sites showed that on average 0.5 Mg ha-1 yr-1 (range 0.3 to 1.1; median 0.4 Mg ha-1 yr-1) more carbon was retained in soils in ley-arable compared to exclusively annual systems, depending on species composition, management, soil depth and the duration of the studies. The annual C accumulation rate for catch crops determined in the meta-analysis was well within that range (0.32±0.08 Mg C ha-1 yr-1). Retention factors calculated for straw, manure, sawdust, peat, sewage sludge and composted household waste varied widely in a decadal time scale. Retention of root and rhizodeposit carbon was higher than for above-ground crop residues. We conclude that NPP is the major driver for C sequestration and emphasize that increased soil carbon stocks not always lead to net sequestration of atmospheric CO2 and that C sequestration not always leads to mitigation of greenhouse gas emissions. The consequences of different land use and management are discussed, taking into account two critical boundaries - the limited area of agricultural land on Earth and requirements to produce sufficient food, fibres and energy for a growing population.

Arsenic mobilization in shallow aquifers due to CO 2 intrusion from storage reservoirs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xiao, Ting; Dai, Zhenxue; Viswanathan, Hari S.

We developed an integrated framework of combined batch experiments and reactive transport simulations to quantify water-rock-CO 2 interactions and arsenic (As) mobilization responses to CO 2 and/or saline water leakage into USDWs. Experimental and simulation results suggest that when CO 2 is introduced, pH drops immediately that initiates release of As from clay minerals. Calcite dissolution can increase pH slightly and cause As re-adsorption. Thus, the mineralogy of the USDW is ultimately a determining factor of arsenic fate and transport. Salient results suggest that: (1) As desorption/adsorption from/onto clay minerals is the major reaction controlling its mobilization, and clay mineralsmore » could mitigate As mobilization with surface complexation reactions; (2) dissolution of available calcite plays a critical role in buffering pH; (3) high salinity in general hinders As release from minerals; and (4) the magnitude and quantitative uncertainty of As mobilization are predicated on the values of reaction rates and surface area of calcite, adsorption surface areas and equilibrium constants of clay minerals, and cation exchange capacity. Results of this study are intended to improve ability to quantify risks associated with potential leakage of reservoir fluids into shallow aquifers, in particular the possible environmental impacts of As mobilization at carbon sequestration sites.« less

Strontium and cesium release mechanisms during unsaturated flow through waste-weathered Hanford sediments.

PubMed

Chang, Hyun-Shik; Um, Wooyong; Rod, Kenton; Serne, R Jeff; Thompson, Aaron; Perdrial, Nicolas; Steefel, Carl I; Chorover, Jon

2011-10-01

Leaching behavior of Sr and Cs in the vadose zone of Hanford site (Washington) was studied with laboratory-weathered sediments mimicking realistic conditions beneath the leaking radioactive waste storage tanks. Unsaturated column leaching experiments were conducted using background Hanford pore water focused on first 200 pore volumes. The weathered sediments were prepared by 6 months reaction with a synthetic Hanford tank waste leachate containing Sr and Cs (10(-5) and 10(-3) molal representative of LO- and HI-sediment, respectively) as surrogates for (90)Sr and (137)Cs. The mineral composition of the weathered sediments showed that zeolite (chabazite-type) and feldspathoid (sodalite-type) were the major byproducts but different contents depending on the weathering conditions. Reactive transport modeling indicated that Cs leaching was controlled by ion-exchange, while Sr release was affected primarily by dissolution of the secondary minerals. The later release of K, Al, and Si from the HI-column indicated the additional dissolution of a more crystalline mineral (cancrinite-type). A two-site ion-exchange model successfully simulated the Cs release from the LO-column. However, a three-site ion-exchange model was needed for the HI-column. The study implied that the weathering conditions greatly impact the speciation of the secondary minerals and leaching behavior of sequestrated Sr and Cs.

Methanogenesis-induced pH–Eh shifts drives aqueous metal(loid) mobility in sulfide mineral systems under CO2 enriched conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Harvey, Omar R.; Qafoku, Nikolla; Cantrell, Kirk J.

2016-01-15

Accounting for microbially-mediated CO2 transformation is pivotal to assessing geochemical implications for elevated CO2 in subsurface environments. A series of batch-reactor experiments were conducted to decipher links between autotrophic methanogenesis, CO2 dynamics and aqueous Fe, As and Pb concentrations in the presence of sulfide minerals. Microbially-mediated solubility-trapping followed by pseudo-first order reduction of HCO3- to CH4 (k’ = 0.28-0.59 d-1) accounted for 95% of the CO2 loss from methanogenic experiments. Bicarbonate-to-methane reduction was pivotal in the mitigation of CO2-induced acidity (~1 pH unit) and enhancement of reducing conditions (Eh change from -0.215 to -0.332V ). Methanogenesis-associated shifts in pH-Eh valuesmore » showed no significant effect on aqueous Pb but favored, 1) increased aqueous As as a result of microbially-mediated dissolution of arsenopyrite and 2) decreased aqueous Fe due to mineral-trapping of CO2-mobilized Fe as Fe-carbonate. Its order of occurrence (and magnitude), relative to solubility- and mineral-trapping, highlighted the potential for autotrophic methanogenesis to modulate both carbon sequestration and contaminant mobility in CO2-impacted subsurface environments.« less

Arsenic mobilization in shallow aquifers due to CO 2 intrusion from storage reservoirs

DOE PAGES

Xiao, Ting; Dai, Zhenxue; Viswanathan, Hari S.; ...

2017-06-05

We developed an integrated framework of combined batch experiments and reactive transport simulations to quantify water-rock-CO 2 interactions and arsenic (As) mobilization responses to CO 2 and/or saline water leakage into USDWs. Experimental and simulation results suggest that when CO 2 is introduced, pH drops immediately that initiates release of As from clay minerals. Calcite dissolution can increase pH slightly and cause As re-adsorption. Thus, the mineralogy of the USDW is ultimately a determining factor of arsenic fate and transport. Salient results suggest that: (1) As desorption/adsorption from/onto clay minerals is the major reaction controlling its mobilization, and clay mineralsmore » could mitigate As mobilization with surface complexation reactions; (2) dissolution of available calcite plays a critical role in buffering pH; (3) high salinity in general hinders As release from minerals; and (4) the magnitude and quantitative uncertainty of As mobilization are predicated on the values of reaction rates and surface area of calcite, adsorption surface areas and equilibrium constants of clay minerals, and cation exchange capacity. Results of this study are intended to improve ability to quantify risks associated with potential leakage of reservoir fluids into shallow aquifers, in particular the possible environmental impacts of As mobilization at carbon sequestration sites.« less

Calcite and dolomite in intrusive carbonatites. II. Trace-element variations

NASA Astrophysics Data System (ADS)

Chakhmouradian, Anton R.; Reguir, Ekaterina P.; Couëslan, Christopher; Yang, Panseok

2016-04-01

The composition of calcite and dolomite from several carbonatite complexes (including a large set of petrographically diverse samples from the Aley complex in Canada) was studied by electron-microprobe analysis and laser-ablation inductively-coupled-plasma mass-spectrometry to identify the extent of substitution of rare-earth and other trace elements in these minerals and the effects of different igneous and postmagmatic processes on their composition. Analysis of the newly acquired and published data shows that the contents of rare-earth elements (REE) and certain REE ratios in magmatic calcite and dolomite are controlled by crystal fractionation of fluorapatite, monazite and, possibly, other minerals. Enrichment in REE observed in some samples (up to ~2000 ppm in calcite) cannot be accounted for by coupled substitutions involving Na, P or As. At Aley, the REE abundances and chondrite-normalized (La/Yb)cn ratios in carbonates decrease with progressive fractionation. Sequestration of heavy REE from carbonatitic magma by calcic garnet may be responsible for a steeply sloping "exponential" pattern and lowered Ce/Ce* ratios of calcite from Magnet Cove (USA) and other localities. Alternatively, the low levels of Ce and Mn in these samples could result from preferential removal of these elements by Ce4+- and Mn3+-bearing minerals (such as cerianite and spinels) at increasing f(O2) in the magma. The distribution of large-ion lithophile elements (LILE = Sr, Ba and Pb) in rock-forming carbonates also shows trends indicative of crystal fractionation effects (e.g., concomitant depletion in Ba + Pb at Aley, or Sr + Ba at Kerimasi), although the phases responsible for these variations cannot be identified unambiguously at present. Overall, element ratios sensitive to the redox state of the magma and its complexing characteristics (Eu/Eu*, Ce/Ce* and Y/Ho) are least variable and in both primary calcite and dolomite, approach the average chondritic values. In consanguineous rocks, calcite invariably has higher REE and LILE levels than dolomite. Hydrothermal reworking of carbonatites does not produce a unique geochemical fingerprint, leading instead to a variety of evolutionary trends that range from light-REE and LILE enrichment (Turiy Mys, Russia) to heavy-REE enrichment and LILE depletion (Bear Lodge, USA). These differences clearly attest to variations in the chemistry of carbonatitic fluids and, consequently, their ability to mobilize specific trace elements from earlier-crystallized minerals. An important telltale indicator of hydrothermal reworking is deviation from the primary, chondrite-like REE ratios (in particular, Y/Ho and Eu/Eu*), accompanied by a variety of other compositional changes depending on the redox state of the fluid (e.g., depletion of carbonates in Mn owing to its oxidation and sequestration by secondary oxides). The effect of supergene processes was studied on a single sample from Bear Lodge, which shows extreme depletion in Mn and Ce (both due to oxidation), coupled with enrichment in Pb and U, possibly reflecting an increased availability of Pb2+ and (UO2)2+ species in the system. On the basis of these findings, several avenues for future research can be outlined: (1) structural mechanisms of REE uptake by carbonates; (2) partitioning of REE and LILE between cogenetic calcite and dolomite; (3) the effects of fluorapatite, phlogopite and pyrochlore fractionation on the LILE budget of magmatic carbonates; (4) the cause(s) of coupled Mn-Ce depletion in some primary calcite; and (5) relations between fluid chemistry and compositional changes in hydrothermal carbonates.

Effect of heterogeneousatmospheric CO2 on simulated global carbon budget

USGS Publications Warehouse

Zhang, Zhen; Jiang, Hong; Liu, Jinxun; Ju, Weimin; Zhang, Xiuying

2013-01-01

The effects of rising atmospheric carbon dioxide (CO2) on terrestrial carbon (C) sequestration have been a key focus in global change studies. As anthropological CO2 emissions substantially increase, the spatial variability of atmospheric CO2 should be considered to reduce the potential bias on C source and sink estimations. In this study, the global spatial–temporal patterns of near surface CO2 concentrations for the period 2003-2009 were established using the SCIAMACHY satellite observations and the GLOBALVIEW-CO2 field observations. With this CO2 data and the Integrated Biosphere Simulator (IBIS), our estimation of the global mean annual NPP and NEP was 0.5% and 7% respectively which differs from the traditional C sequestration assessments. The Amazon, Southeast Asia, and Tropical Africa showed higher C sequestration than the traditional assessment, and the rest of the areas around the world showed slightly lower C sequestration than the traditional assessment. We find that the variability of NEP is less intense under heterogeneous CO2 pattern on a global scale. Further studies of the cause of CO2 variation and the interactions between natural and anthropogenic processes of C sequestration are needed.

Water-Rock Interactions in the Peridotite Aquifer of the Oman-UAE Ophiolite: Strontium Isotopic Ratio and Geochemical Evolution of Groundwater

NASA Astrophysics Data System (ADS)

Bompard, Nicolas; Matter, Juerg; Teagle, Damon

2016-04-01

The peridotite aquifer in Wadi Tayin, Sultanate of Oman, is a perfect example of natural carbonation of ultramafic rocks. In situ mineral carbonation is considered the most safest and permanent option of CO2 Capture and Sequestration (CCS). However, the process itself is yet to be characterised and a better understanding of the mechanisms involved in natural mineral carbonation is needed before geo-engineering it. We used the 87Sr/86Sr system to follow the water-rock interactions along the groundwater flowpath in the peridotite aquifer and to determine the sources of divalent cations (Mg2+, Ca2+) required for mineral carbonation. The Sr-isotope data of groundwater show that the aquifer rocks are the main source for divalent cations (Mg2+, Ca2+ and Sr2+) and secondary carbonates are their main sink. The groundwater 87Sr/86Sr ratio evolves with its pH: from 87Sr/86Sr = 0.7087 (n=3) to 0.7082 (n=8) between pH 7 and 8, and from 0.7086 (n=6) at pH 9 to 0.07075 (n=9) at pH 11. This evolution seems to support a two-step model for the water-rock interactions in the peridotite aquifer. From pH 7 to 8, secondary Ca-carbonate precipitation buffers the pH rise resulting from peridotite serpentinisation. From pH 9 to 11, peridotite serpentinisation drives the pH to alkaline condition. The change from a Mg-rich to a Ca-rich groundwater at pH 9 seems to confirm the two-step model.

Zinc speciation in mining and smelter contaminated overbank sediments by EXAFS spectroscopy

NASA Astrophysics Data System (ADS)

Van Damme, An; Degryse, Fien; Smolders, Erik; Sarret, Géraldine; Dewit, Julie; Swennen, Rudy; Manceau, Alain

2010-07-01

Overbank sediments contaminated with metalliferous minerals are a source of toxic metals that pose risks to living organisms. The overbank sediments from the Geul river in Belgium contain 4000-69,000 mg/kg Zn as a result of mining and smelting activities, principally during the 19th century. Three main Zn species were identified by powder Zn K-edge EXAFS spectroscopy: smithsonite (ZnCO 3), tetrahedrally coordinated sorbed Zn (sorbed IVZn) and Zn-containing trioctahedral phyllosilicate. Smithsonite is a primary mineral, which accounts for approximately 20-60% of the Zn in sediments affected by mining and smelting of oxidized Zn ores (mostly carbonates and silicates). This species is almost absent in sediments affected by mining and smelting of both sulphidic (ZnS, PbS) and oxidized ores, presumably because of acidic dissolution associated with the oxidation of sulphides, as suggested by the lower pH of this second type of sediment (pH(CaCl 2) <7.0 vs. pH(CaCl 2) >7.0 for the first type). Thus, sulphide minerals in sediment deposits can act as a secondary source of dissolved metals by a chemical process analogous to acid mine drainage. The sorbed IVZn component ranges up to approximately 30%, with the highest proportion occurring at pH(CaCl 2) <7.0 as a result of the readsorption of dissolved Zn 2+ on sediments constituents. Kerolite-like Zn-rich phyllosilicate is the major secondary species in all samples, and in some the only detected species, thus providing the first evidence for pervasive sequestration of Zn into this newly formed precipitate at the field scale.

PFLOTRAN: Reactive Flow & Transport Code for Use on Laptops to Leadership-Class Supercomputers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hammond, Glenn E.; Lichtner, Peter C.; Lu, Chuan

PFLOTRAN, a next-generation reactive flow and transport code for modeling subsurface processes, has been designed from the ground up to run efficiently on machines ranging from leadership-class supercomputers to laptops. Based on an object-oriented design, the code is easily extensible to incorporate additional processes. It can interface seamlessly with Fortran 9X, C and C++ codes. Domain decomposition parallelism is employed, with the PETSc parallel framework used to manage parallel solvers, data structures and communication. Features of the code include a modular input file, implementation of high-performance I/O using parallel HDF5, ability to perform multiple realization simulations with multiple processors permore » realization in a seamless manner, and multiple modes for multiphase flow and multicomponent geochemical transport. Chemical reactions currently implemented in the code include homogeneous aqueous complexing reactions and heterogeneous mineral precipitation/dissolution, ion exchange, surface complexation and a multirate kinetic sorption model. PFLOTRAN has demonstrated petascale performance using 2{sup 17} processor cores with over 2 billion degrees of freedom. Accomplishments achieved to date include applications to the Hanford 300 Area and modeling CO{sub 2} sequestration in deep geologic formations.« less

Reactive Radial Diffusion Model for the Aging/Sequestration Process

NASA Astrophysics Data System (ADS)

Ginn, T. R.; Basagaoglu, H.; McCoy, B. J.; Scow, K. M.

2001-12-01

A radial diffusion model has been formulated to simulate age-dependent bioavailability of chemical compounds to micro-organisms residing outside (and/or inside) the porous soil particles. Experimental findings in the literature indicate that the sequestration and reduction in bioavailability of contaminants are controlled presumably by the diffusion-limited sorption kinetics and the time-variant desorption process. Here we combine radial-diffusion mass transfer modeling with the exposure-time concept to generate mass-balance equations for the intra- and extra-particle concentrations. The model accomodates reversible sorption kinetics involving sorption time-dependence of the rate coefficients, distinct intra- and extra-particle biodegradation rates; and a dynamic mass interaction between the intra- and extra-particle concentrations arising from the radial diffusion concept. The model explicitly treats multiple particle classes distributed in size and chemical properties in a bulk aquifer or soil volume, which allows the simulation of the sequestration and bioavailability of contaminants in different particle size classes that have distinct diffusion, reaction, and aging properties.

Strategy And The Spreadsheet: Optimizing The Total Army To Satisfy Both

DTIC Science & Technology

2016-02-11

historically reduces military end strength at the conclusion of major conflicts. The Budget Control Act of 2011 imposed sequestration spending limits on...the military that began the process of drawing down the military through fiscal year 2021. While the 2016 defense budget delays sequestration cuts... budget by a wide margin, has started repeating a historical cycle of budget driven defense cuts. The Army’s large force represents an attractive

Pore-Scale Geochemical Reactivity Associated with CO2 Storage: New Frontiers at the Fluid-Solid Interface.

PubMed

Noiriel, Catherine; Daval, Damien

2017-04-18

The reactivity of carbonate and silicate minerals is at the heart of porosity and pore geometry changes in rocks injected with CO 2 , which ultimately control the evolution of flow and transport properties of fluids in porous and/or fractured geological reservoirs. Modeling the dynamics of CO 2 -water-rock interactions is challenging because of the resulting large geochemical disequilibrium, the reservoir heterogeneities, and the large space and time scales involved in the processes. In particular, there is a lack of information about how the macroscopic properties of a reservoir, e.g., the permeability, will evolve as a result of geochemical reactions at the molecular scale. Addressing this point requires a fundamental understanding of how the microstructures influence the macroscopic properties of rocks. The pore scale, which ranges from a few nanometers to centimeters, has stood out as an essential scale of observation of geochemical processes in rocks. Transport or surface reactivity limitations due to the pore space architecture, for instance, are best described at the pore scale itself. It can be also considered as a mesoscale for aggregating and increasing the gain of fundamental understanding of microscopic interfacial processes. Here we focus on the potential application of a combination of physicochemical measurements coupled with nanoscale and microscale imaging techniques during laboratory experiments to improve our understanding of the physicochemical mechanisms that occur at the fluid-solid interface and the dynamics of the coupling between the geochemical reactions and flow and transport modifications at the pore scale. Imaging techniques such as atomic force microscopy, vertical scanning interferometry, focused ion beam transmission electron microscopy, and X-ray microtomography, are ideal for investigating the reactivity dynamics of these complex materials. Minerals and mineral assemblages, i.e., rocks, exhibit heterogeneous and anisotropic reactivity, which challenges the continuum description of porous media and assumptions required for reactive transport modeling at larger scales. The conventional approach, which consists of developing dissolution rate laws normalized to the surface area, should be revisited to account for both the anisotropic crystallographic structure of minerals and the transport of chemical species near the interface, which are responsible for the intrinsic evolution of the mineral dissolution rate as the reaction progresses. In addition, the crystal morphology and the mineral assemblage composition, texture, and structural heterogeneities are crucial in determining whether the permeability and transport properties of the reservoir will be altered drastically or maintain the sealing properties required to ensure the safe sequestration of CO 2 for hundreds of years. Investigating the transport properties in nanometer- to micrometer-thick amorphous Si-rich surface layers (ASSLs), which develop at the fluid-mineral interface in silicates, provides future direction, as ASSLs may prevent contact between the dissolving solids and the pore fluid, potentially inhibiting the dissolution/carbonation process. Equally, at a larger scale, the growth of micrometer- to millimeter-thick alteration layers, which result from the difference in reactivity between silicates and carbonates, slows the transport in the vicinity of the fluid-solid interface in polymineralic rocks, thus limiting the global reactivity of the carbonate matrix. In contrast, in pure limestone, the global reactivity of the monomineralic rock decreases because the flow localization promotes the local reactivity within the forming channels, thus enhancing permeability changes compared with more homogeneous dissolution of the rock matrix. These results indicate that the transformation of the rock matrix should control the evolution of the transport properties in reservoirs injected with CO 2 to the same extent as the intrinsic chemical reactivity of the minerals and the reservoir hydrodynamics. This process, which is currently not captured by large-scale modeling of reactive transport, should benefit from the increasing capabilities of noninvasive and nondestructive characterization tools for pore-scale processes, ultimately constraining reactive transport modeling and improving the reliability of predictions.

Quantifying and Mapping the Supply of and Demand for Carbon Storage and Sequestration Service from Urban Trees.

PubMed

Zhao, Chang; Sander, Heather A

2015-01-01

Studies that assess the distribution of benefits provided by ecosystem services across urban areas are increasingly common. Nevertheless, current knowledge of both the supply and demand sides of ecosystem services remains limited, leaving a gap in our understanding of balance between ecosystem service supply and demand that restricts our ability to assess and manage these services. The present study seeks to fill this gap by developing and applying an integrated approach to quantifying the supply and demand of a key ecosystem service, carbon storage and sequestration, at the local level. This approach follows three basic steps: (1) quantifying and mapping service supply based upon Light Detection and Ranging (LiDAR) processing and allometric models, (2) quantifying and mapping demand for carbon sequestration using an indicator based on local anthropogenic CO2 emissions, and (3) mapping a supply-to-demand ratio. We illustrate this approach using a portion of the Twin Cities Metropolitan Area of Minnesota, USA. Our results indicate that 1735.69 million kg carbon are stored by urban trees in our study area. Annually, 33.43 million kg carbon are sequestered by trees, whereas 3087.60 million kg carbon are emitted by human sources. Thus, carbon sequestration service provided by urban trees in the study location play a minor role in combating climate change, offsetting approximately 1% of local anthropogenic carbon emissions per year, although avoided emissions via storage in trees are substantial. Our supply-to-demand ratio map provides insight into the balance between carbon sequestration supply in urban trees and demand for such sequestration at the local level, pinpointing critical locations where higher levels of supply and demand exist. Such a ratio map could help planners and policy makers to assess and manage the supply of and demand for carbon sequestration.

Process-oriented modelling to identify main drivers of erosion-induced carbon fluxes

NASA Astrophysics Data System (ADS)

Wilken, Florian; Sommer, Michael; Van Oost, Kristof; Bens, Oliver; Fiener, Peter

2017-05-01

Coupled modelling of soil erosion, carbon redistribution, and turnover has received great attention over the last decades due to large uncertainties regarding erosion-induced carbon fluxes. For a process-oriented representation of event dynamics, coupled soil-carbon erosion models have been developed. However, there are currently few models that represent tillage erosion, preferential water erosion, and transport of different carbon fractions (e.g. mineral bound carbon, carbon encapsulated by soil aggregates). We couple a process-oriented multi-class sediment transport model with a carbon turnover model (MCST-C) to identify relevant redistribution processes for carbon dynamics. The model is applied for two arable catchments (3.7 and 7.8 ha) located in the Tertiary Hills about 40 km north of Munich, Germany. Our findings indicate the following: (i) redistribution by tillage has a large effect on erosion-induced vertical carbon fluxes and has a large carbon sequestration potential; (ii) water erosion has a minor effect on vertical fluxes, but episodic soil organic carbon (SOC) delivery controls the long-term erosion-induced carbon balance; (iii) delivered sediments are highly enriched in SOC compared to the parent soil, and sediment delivery is driven by event size and catchment connectivity; and (iv) soil aggregation enhances SOC deposition due to the transformation of highly mobile carbon-rich fine primary particles into rather immobile soil aggregates.

Depositional and diagenetic variability within the Cambrian Mount Simon Sandstone: Implications for carbon dioxide sequestration

USGS Publications Warehouse

Bowen, B.B.; Ochoa, R.I.; Wilkens, N.D.; Brophy, J.; Lovell, T.R.; Fischietto, N.; Medina, C.R.; Rupp, J.A.

2011-01-01

The Cambrian Mount Simon Sandstone is the major target reservoir for ongoing geologic carbon dioxide (CO2) sequestration demonstrations throughout the midwest United States. The potential CO2 reservoir capacity, reactivity, and ultimate fate of injected CO2 depend on textural and compositional properties determined by depositional and diagenetic histories that vary vertically and laterally across the formation. Effective and efficient prediction and use of the available pore space requires detailed knowledge of the depositional and diagenetic textures and mineralogy, how these variables control the petrophysical character of the reservoir, and how they vary spatially. Here, we summarize the reservoir characteristics of the Mount Simon Sandstone based on examination of geophysical logs, cores, cuttings, and analysis of more than 150 thin sections. These samples represent different parts of the formation and depth ranges of more than 9000 ft (>2743 m) across the Illinois Basin and surrounding areas. This work demonstrates that overall reservoir quality and, specifically, porosity do not exhibit a simple relationship with depth, but vary both laterally and with depth because of changes in the primary depositional facies, framework composition (i.e., feldspar concentration), and diverse diagenetic modifications. Diagenetic processes that have been significant in modifying the reservoir include formation of iron oxide grain coatings, chemical compaction, feldspar precipitation and dissolution, multiple generations of quartz overgrowth cementation, clay mineral precipitation, and iron oxide cementation. These variables provide important inputs for calculating CO2 capacity potential, modeling reactivity, and are also an important baseline for comparisons after CO2 injection. Copyright ??2011. The American Association of Petroleum Geologists/Division of Environmental Geosciences. All rights reserved.

Carbon in Underland (A "Life at the Frontiers of Energy Research" contest entry from the 2011 Energy Frontier Research Centers (EFRCs) Summit and Forum

ScienceCinema

DePaolo, Donald J. (Director, Center for Nanoscale Control of Geologic CO2); NCGC Staff

2017-12-09

'Carbon in Underland' was submitted by the Center for Nanoscale Control of Geologic CO2 (NCGC) to the 'Life at the Frontiers of Energy Research' video contest at the 2011 Science for Our Nation's Energy Future: Energy Frontier Research Centers (EFRCs) Summit and Forum. Twenty-six EFRCs created short videos to highlight their mission and their work. This video was selected as one of five winners by a distinguished panel of judges for its 'entertaining animation and engaging explanations of carbon sequestration'. NCGC, an EFRC directed by Donald J. DePaolo at Lawrence Berkeley National Laboratory is a partnership of scientists from seven institutions: LBNL (lead) Massachusetts Institute of Technology, Lawrence Livermore National Laboratory, Oak Ridge National Laboratory, University of California, Davis, Ohio State University, and Washington University in St. Louis. The Office of Basic Energy Sciences in the U.S. Department of Energy's Office of Science established the 46 Energy Frontier Research Centers (EFRCs) in 2009. These collaboratively-organized centers conduct fundamental research focused on 'grand challenges' and use-inspired 'basic research needs' recently identified in major strategic planning efforts by the scientific community. The overall purpose is to accelerate scientific progress toward meeting the nation's critical energy challenges. The mission of the Center for Nanoscale Control of Geologic CO{sub 2} is 'to use new investigative tools, combined with experiments and computer simulations, to build a fundamental understanding of molecular-to-pore-scale processes in fluid-rock systems, and to demonstrate the ability to control critical aspects of flow, transport, and mineralization in porous rock media as applied to geologic sequestration of CO{sub 2}. Research topics are: bio-inspired, CO{sub 2} (store), greenhouse gas, and interfacial characterization.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Miller, Jeff

"Carbon in Underland" was submitted by the Center for Nanoscale Controls on Geologic CO2 (NCGC) to the "Life at the Frontiers of Energy Research" video contest at the 2011 Science for Our Nation's Energy Future: Energy Frontier Research Centers (EFRCs) Summit and Forum. Twenty-six EFRCs created short videos to highlight their mission and their work. This video was selected as one of five winners by a distinguished panel of judges for its "entertaining animation and engaging explanations of carbon sequestration". NCGC, an EFRC directed by Donald J. DePaolo at Lawrence Berkeley National Laboratory is a partnership of scientists from sevenmore » institutions: LBNL (lead) Massachusetts Institute of Technology, Lawrence Livermore National Laboratory, Oak Ridge National Laboratory, University of California, Davis, Ohio State University, and Washington University in St. Louis. The Office of Basic Energy Sciences in the U.S. Department of Energy's Office of Science established the 46 Energy Frontier Research Centers (EFRCs) in 2009. These collaboratively-organized centers conduct fundamental research focused on 'grand challenges' and use-inspired 'basic research needs' recently identified in major strategic planning efforts by the scientific community. The overall purpose is to accelerate scientific progress toward meeting the nation's critical energy challenges. The mission of the Center for Nanoscale Control of Geologic CO2 is 'to use new investigative tools, combined with experiments and computer simulations, to build a fundamental understanding of molecular-to-pore-scale processes in fluid-rock systems, and to demonstrate the ability to control critical aspects of flow, transport, and mineralization in porous rock media as applied to geologic sequestration of CO2. Research topics are: bio-inspired, CO2 (store), greenhouse gas, and interfacial characterization.« less

Measuring water adsorption on mineral surfaces in air, CO2, and supercritical CO2 with a quartz-crystal microbalance

NASA Astrophysics Data System (ADS)

Bryan, C. R.; Wells, R. K.; Burton, P. D.; Heath, J. E.; Dewers, T. A.; Wang, Y.

2011-12-01

Carbon sequestration via underground storage in geologic formations is a proposed approach for reducing industrial CO2 emissions. However, current models for carbon injection and long-term storage of supercritical CO2 (scCO2) do not consider the development and stability of adsorbed water films at the scCO2-hydrophilic mineral interface. The thickness and properties of the water films control the surface tension and wettability of the mineral surface, and on the core scale, affect rock permeability, saturation, and capillary properties. The film thickness is strongly dependent upon the activity of water in the supercritical fluid, which will change as initially anhydrous scCO2 absorbs water from formation brine. As described in a companion paper by the coauthors, the thickness of the adsorbed water layer is controlled by the disjoining pressure; structural and van der Waals components dominate at low water activity, while electrostatic forces become more important with increasing film thickness (higher water activities). As scCO2 water activity and water layer thickness increase, concomitant changes in mineral surface properties and reservoir/caprock hydrologic properties will affect the mobility of the aqueous phase and of scCO2. Moreover, the development of a water layer may be critical to mineral dissolution reactions in scCO2. Here, we describe the use of a quartz-crystal microbalance (QCM) to monitor adsorption of water by mineral surfaces. QCMs utilize a piezoelectrically-stimulated quartz wafer to measure adsorbed or deposited mass via changes in vibrational frequency. When used to measure the mass of adsorbed liquid films, the frequency response of the crystal must be corrected for the viscoelastic, rather than elastic, response of the adsorbed layer. Results are presented for adsorption to silica in N2 and CO2 at one bar, and in scCO2. Additional data are presented for water uptake by clays deposited on a QCM wafer. In this case, water uptake occurs by the combined processes of interlayer cation hydration, surface adsorption, and capillary condensation. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. This work is supported by the DOE Sandia LDRD Program.

Analysis of Geologic CO2 Sequestration at Farnham Dome, Utah, USA

NASA Astrophysics Data System (ADS)

Lee, S.; Han, W.; Morgan, C.; Lu, C.; Esser, R.; Thorne, D.; McPherson, B.

2008-12-01

The Farnham Dome in east-central Utah is an elongated, Laramide-age anticline along the northern plunge of the San Rafael uplift and the western edge of the Uinta Basin. We are helping design a proposed field demonstration of commercial-scale geologic CO2 sequestration, including injection of 2.9 million tons of CO2 over four years time. The Farnham Dome pilot site stratigraphy includes a stacked system of saline formations alternating with low-permeability units. Facilitating the potential sequestration demonstration is a natural CO2 reservoir at depth, the Jurassic-age Navajo formation, which contains an estimated 50 million tons of natural CO2. The sequestration test design includes two deep formations suitable for supercritical CO2 injection, the Jurassic-age Wingate sandstone and the Permian-age White Rim sandstone. We developed a site-specific geologic model based on available geophysical well logs and formation tops data for use with numerical simulation. The current geologic model is limited to an area of approximately 6.5x4.5 km2 and 2.5 km thick, which contains 12 stacked formations starting with the White Rim formation at the bottom (>5000 feet bgl) and extending to the Jurassic Curtis formation at the top of the model grid. With the detail of the geologic model, we are able to estimate the Farnham Dome CO2 capacity at approximately 36.5 million tones within a 5 mile radius of a single injection well. Numerical simulation of multiphase, non- isothermal CO2 injection and flow suggest that the injected CO2 plume will not intersect nearby fault zones mapped in previous geologic studies. Our simulations also examine and compare competing roles of different trapping mechanisms, including hydrostratigraphic, residual gas, solubility, and mineralization trapping. Previous studies of soil gas flux at the surface of the fault zones yield no significant evidence of CO2 leakage from the natural reservoir at Farnham Dome, and thus we use these simulations to evaluate what factors make this natural reservoir so effective for CO2 storage. Our characterization and simulation efforts are producing a CO2 sequestration framework that incorporates production and capacity estimation, area-of-review, injectivity, and trapping mechanisms. Likewise, mitigation and monitoring strategies have been formulated from the site characterization and modeling results.

Direct gas-solid carbonation of serpentinite residues in the absence and presence of water vapor: a feasibility study for carbon dioxide sequestration.

PubMed

Veetil, Sanoopkumar Puthiya; Pasquier, Louis-César; Blais, Jean-François; Cecchi, Emmanuelle; Kentish, Sandra; Mercier, Guy

2015-09-01

Mineral carbonation of serpentinite mining residue offers an environmentally secure and permanent storage of carbon dioxide. The strategy of using readily available mining residue for the direct treatment of flue gas could improve the energy demand and economics of CO2 sequestration by avoiding the mineral extraction and separate CO2 capture steps. The present is a laboratory scale study to assess the possibility of CO2 fixation in serpentinite mining residues via direct gas-solid reaction. The degree of carbonation is measured both in the absence and presence of water vapor in a batch reactor. The gas used is a simulated gas mixture reproducing an average cement flue gas CO2 composition of 18 vol.% CO2. The reaction parameters considered are temperature, total gas pressure, time, and concentration of water vapor. In the absence of water vapor, the gas-solid carbonation of serpentinite mining residues is negligible, but the residues removed CO2 from the feed gas possibly due to reversible adsorption. The presence of small amount of water vapor enhances the gas-solid carbonation, but the measured rates are too low for practical application. The maximum CO2 fixation obtained is 0.07 g CO2 when reacting 1 g of residue at 200 °C and 25 barg (pCO2 ≈ 4.7) in a gas mixture containing 18 vol.% CO2 and 10 vol.% water vapor in 1 h. The fixation is likely surface limited and restricted due to poor gas-solid interaction. It was identified that both the relative humidity and carbon dioxide-water vapor ratio have a role in CO2 fixation regardless of the percentage of water vapor.

Effects of Biochar Addition on CO2 and N2O Emissions following Fertilizer Application to a Cultivated Grassland Soil

PubMed Central

Chen, Jingjing; Kim, Hyunjin; Yoo, Gayoung

2015-01-01

Carbon (C) sequestration potential of biochar should be considered together with emission of greenhouse gases when applied to soils. In this study, we investigated CO2 and N2O emissions following the application of rice husk biochars to cultivated grassland soils and related gas emissions tos oil C and nitrogen (N) dynamics. Treatments included biochar addition (CHAR, NO CHAR) and amendment (COMPOST, UREA, NO FERT). The biochar application rate was 0.3% by weight. The temporal pattern of CO2 emissions differed according to biochar addition and amendments. CO2 emissions from the COMPOST soils were significantly higher than those from the UREA and NO FERT soils and less CO2 emission was observed when biochar and compost were applied together during the summer. Overall N2O emission was significantly influenced by the interaction between biochar and amendments. In UREA soil, biochar addition increased N2O emission by 49% compared to the control, while in the COMPOST and NO FERT soils, biochar did not have an effect on N2O emission. Two possible mechanisms were proposed to explain the higher N2O emissions upon biochar addition to UREA soil than other soils. Labile C in the biochar may have stimulated microbial N mineralization in the C-limited soil used in our study, resulting in an increase in N2O emission. Biochar may also have provided the soil with the ability to retain mineral N, leading to increased N2O emission. The overall results imply that biochar addition can increase C sequestration when applied together with compost, and might stimulate N2O emission when applied to soil amended with urea. PMID:26020941

Training Graduate and Undergraduate Students in Simulation and Risk Assessment for Carbon Sequestration

DOE Office of Scientific and Technical Information (OSTI.GOV)

McCray, John

Capturing carbon dioxide (CO2) and injecting it into deep underground formations for storage (carbon capture and underground storage, or CCUS) is one way of reducing anthropogenic CO2 emissions. Gas or aqueous-phase leakage may occur due to transport via faults and fractures, through faulty well bores, or through leaky confining materials. Contaminants of concern include aqueous salts and dissolved solids, gaseous or aqueous-phase organic contaminants, and acidic gas or aqueous-phase fluids that can liberate metals from aquifer minerals. Understanding the mechanisms and parameters that can contribute to leakage of the CO2 and the ultimate impact on shallow water aquifers that overliemore » injection formations is an important step in evaluating the efficacy and risks associated with long-term CO2 storage. Three students were supported on the grant Training Graduate and Undergraduate Students in Simulation and Risk Assessment for Carbon Sequestration. These three students each examined a different aspect of simulation and risk assessment related to carbon dioxide sequestration and the potential impacts of CO2 leakage. Two performed numerical simulation studies, one to assess leakage rates as a function of fault and deep reservoir parameters and one to develop a method for quantitative risk assessment in the event of a CO2 leak and subsequent changes in groundwater chemistry. A third student performed an experimental evaluation of the potential for metal release from sandstone aquifers under simulated leakage conditions. This study has resulted in two student first-authored published papers {Siirila, 2012 #560}{Kirsch, 2014 #770} and one currently in preparation {Menke, In prep. #809}.« less

Changes in the temperature sensitivity of SOM decomposition with grassland succession: implications for soil C sequestration.

PubMed

Nianpeng, He; Ruomeng, Wang; Yang, Gao; Jingzhong, Dai; Xuefa, Wen; Guirui, Yu

2013-12-01

Understanding the temperature sensitivity (Q 10) of soil organic matter (SOM) decomposition is important for predicting soil carbon (C) sequestration in terrestrial ecosystems under warming scenarios. Whether Q 10 varies predictably with ecosystem succession and the ways in which the stoichiometry of input SOM influences Q 10 remain largely unknown. We investigate these issues using a grassland succession series from free-grazing to 31-year grazing-exclusion grasslands in Inner Mongolia, and an incubation experiment performed at six temperatures (0, 5, 10, 15, 20, and 25°C) and with four substrates: control (CK), glucose (GLU), mixed grass leaf (GRA), and Medicago falcata leaf (MED). The results showed that basal soil respiration (20°C) and microbial biomass C (MBC) logarithmically decreased with grassland succession. Q 10 decreased logarithmically from 1.43 in free-grazing grasslands to 1.22 in 31-year grazing-exclusion grasslands. Q 10 increased significantly with the addition of substrates, and the Q 10 levels increased with increase in N:C ratios of substrate. Moreover, accumulated C mineralization was controlled by the N:C ratio of newly input SOM and by incubation temperature. Changes in Q 10 with grassland ecosystem succession are controlled by the stoichiometry of newly input SOM, MBC, and SOM quality, and the combined effects of which could partially explain the mechanisms underlying soil C sequestration in the long-term grazing-exclusion grasslands in Inner Mongolia, China. The findings highlight the effect of substrate stoichiometry on Q 10 which requires further study.

Carbon Dioxide-Water Emulsions for Enhanced Oil Recovery and Permanent Sequestration of Carbon Dioxide

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ryan, David; Golomb, Dan; Shi, Guang

2011-09-30

This project involves the use of an innovative new invention Particle Stabilized Emulsions (PSEs) of Carbon Dioxide-in-Water and Water-in-Carbon Dioxide for Enhanced Oil Recovery (EOR) and Permanent Sequestration of Carbon Dioxide. The EOR emulsion would be injected into a semi-depleted oil reservoir such as Dover 33 in Otsego County, Michigan. It is expected that the emulsion would dislocate the stranded heavy crude oil from the rock granule surfaces, reduce its viscosity, and increase its mobility. The advancing emulsion front should provide viscosity control which drives the reduced-viscosity oil toward the production wells. The make-up of the emulsion would be subsequentlymore » changed so it interacts with the surrounding rock minerals in order to enhance mineralization, thereby providing permanent sequestration of the injected CO{sub 2}. In Phase 1 of the project, the following tasks were accomplished: 1. Perform laboratory scale (mL/min) refinements on existing procedures for producing liquid carbon dioxide-in-water (C/W) and water-in-liquid carbon dioxide (W/C) emulsion stabilized by hydrophilic and hydrophobic fine particles, respectively, using a Kenics-type static mixer. 2. Design and cost evaluate scaled up (gal/min) C/W and W/C emulsification systems to be deployed in Phase 2 at the Otsego County semi-depleted oil field. 3. Design the modifications necessary to the present CO{sub 2} flooding system at Otsego County for emulsion injection. 4. Design monitoring and verification systems to be deployed in Phase 2 for measuring potential leakage of CO{sub 2} after emulsion injection. 5. Design production protocol to assess enhanced oil recovery with emulsion injection compared to present recovery with neat CO{sub 2} flooding. 6. Obtain Federal and State permits for emulsion injection. Initial research focused on creating particle stabilized emulsions with the smallest possible globule size so that the emulsion can penetrate even low-permeability crude oilcontaining formations or saline aquifers. The term globule refers to the water or liquid carbon dioxide droplets sheathed with ultrafine particles dispersed in the continuous external medium, liquid CO{sub 2} or H{sub 2}O, respectively. The key to obtaining very small globules is the shear force acting on the two intermixing fluids, and the use of ultrafine stabilizing particles or nanoparticles. We found that using Kenics-type static mixers with a shear rate in the range of 2700 to 9800 s{sup -1} and nanoparticles between 100-300 nm produced globule sizes in the 10 to 20 μm range. Particle stabilized emulsions with that kind of globule size should easily penetrate oil-bearing formations or saline aquifers where the pore and throat size can be on the order of 50 μm or larger. Subsequent research focused on creating particle stabilized emulsions that are deemed particularly suitable for Permanent Sequestration of Carbon Dioxide. Based on a survey of the literature an emulsion consisting of 70% by volume of water, 30% by volume of liquid or supercritical carbon dioxide, and 2% by weight of finely pulverized limestone (CaCO{sub 3}) was selected as the most promising agent for permanent sequestration of CO{sub 2}. In order to assure penetration of the emulsion into tight formations of sandstone or other silicate rocks and carbonate or dolomite rock, it is necessary to use an emulsion consisting of the smallest possible globule size. In previous reports we described a high shear static mixer that can create such small globules. In addition to the high shear mixer, it is also necessary that the emulsion stabilizing particles be in the submicron size, preferably in the range of 0.1 to 0.2 μm (100 to 200 nm) size. We found a commercial source of such pulverized limestone particles, in addition we purchased under this DOE Project a particle grinding apparatus that can provide particles in the desired size range. Additional work focused on attempts to generate particle stabilized emulsions with a flow through, static mixer based apparatus under a variety of conditions that are suitable for permanent sequestration of carbon dioxide. A variety of mixtures of water, CO{sub 2} and particles may also provide suitable emulsions capable of PS. In addition, it is necessary to test the robustness of PSE formation as composition changes to be certain that emulsions of appropriate size and stability form under conditions that might vary during actual large scale EOR and sequestration operations. The goal was to lay the groundwork for an apparatus and formulation that would produce homogenous microemulsions of CO{sub 2}-in-water capable of readily mixing with the waters of deep saline aquifers and allow a safer and more permanent sequestration of carbon dioxide. In addition, as a beneficial use, we hoped to produce homogenous microemulsions of water-in-CO{sub 2} capable of readily mixing with pure liquid or supercritical CO{sub 2} for use in Enhanced Oil Recovery (EOR). However, true homogeneous microemulsions have proven very difficult to produce and efforts have not yielded either a formulation or a mixing strategy that gives emulsions that do not settle out or that can be diluted with the continuous phase in varying proportions. Other mixtures of water, CO{sub 2} and particles, that are not technically homogeneous microemulsions, may also provide suitable emulsions capable of PS and EOR. For example, a homogeneous emulsion that is not a microemulsion might also provide all of the necessary characteristics desired. These characteristics would include easy formation, stability over time, appropriate size and the potential for mineralization under conditions that would be encountered under actual large scale sequestration operations. This report also describes work with surrogate systems in order to test conditions.« less

Biochar decelerates soil organic nitrogen cycling but stimulates soil nitrification in a temperate arable field trial.

PubMed

Prommer, Judith; Wanek, Wolfgang; Hofhansl, Florian; Trojan, Daniela; Offre, Pierre; Urich, Tim; Schleper, Christa; Sassmann, Stefan; Kitzler, Barbara; Soja, Gerhard; Hood-Nowotny, Rebecca Clare

2014-01-01

Biochar production and subsequent soil incorporation could provide carbon farming solutions to global climate change and escalating food demand. There is evidence that biochar amendment causes fundamental changes in soil nutrient cycles, often resulting in marked increases in crop production, particularly in acidic and in infertile soils with low soil organic matter contents, although comparable outcomes in temperate soils are variable. We offer insight into the mechanisms underlying these findings by focusing attention on the soil nitrogen (N) cycle, specifically on hitherto unmeasured processes of organic N cycling in arable soils. We here investigated the impacts of biochar addition on soil organic and inorganic N pools and on gross transformation rates of both pools in a biochar field trial on arable land (Chernozem) in Traismauer, Lower Austria. We found that biochar increased total soil organic carbon but decreased the extractable organic C pool and soil nitrate. While gross rates of organic N transformation processes were reduced by 50-80%, gross N mineralization of organic N was not affected. In contrast, biochar promoted soil ammonia-oxidizer populations (bacterial and archaeal nitrifiers) and accelerated gross nitrification rates more than two-fold. Our findings indicate a de-coupling of the soil organic and inorganic N cycles, with a build-up of organic N, and deceleration of inorganic N release from this pool. The results therefore suggest that addition of inorganic fertilizer-N in combination with biochar could compensate for the reduction in organic N mineralization, with plants and microbes drawing on fertilizer-N for growth, in turn fuelling the belowground build-up of organic N. We conclude that combined addition of biochar with fertilizer-N may increase soil organic N in turn enhancing soil carbon sequestration and thereby could play a fundamental role in future soil management strategies.

The role of advanced reactive surface area characterization in improving predictions of mineral reaction rates

NASA Astrophysics Data System (ADS)

Beckingham, L. E.; Zhang, S.; Mitnick, E.; Cole, D. R.; Yang, L.; Anovitz, L. M.; Sheets, J.; Swift, A.; Kneafsey, T. J.; Landrot, G.; Mito, S.; Xue, Z.; Steefel, C. I.; DePaolo, D. J.; Ajo Franklin, J. B.

2014-12-01

Geologic sequestration of CO2 in deep sedimentary formations is a promising means of mitigating carbon emissions from coal-fired power plants but the long-term fate of injected CO2 is challenging to predict. Reactive transport models are used to gain insight over long times but rely on laboratory determined mineral reaction rates that have been difficult to extrapolate to field systems. This, in part, is due to a lack of understanding of mineral reactive surface area. Many models use an arbitrary approximation of reactive surface area, applying orders of magnitude scaling factors to measured BET or geometric surface areas. Recently, a few more sophisticated approaches have used 2D and 3D image analyses to determine mineral-specific reactive surface areas that account for the accessibility of minerals. However, the ability of these advanced surface area estimates to improve predictions of mineral reaction rates has yet to be determined. In this study, we fuse X-ray microCT, SEM QEMSCAN, XRD, SANS, and SEM-FIB analysis to determine mineral-specific accessible reactive surface areas for a core sample from the Nagaoka pilot CO2 injection site (Japan). This sample is primarily quartz, plagioclase, smectite, K-feldspar, and pyroxene. SEM imaging shows abundant smectite cement and grain coatings that decrease the fluid accessibility of other minerals. However, analysis of FIB-SEM images reveals that smectite nano-pores are well connected such that access to underlying minerals is not occluded by smectite coatings. Mineral-specific accessible surfaces are determined, accounting for the connectivity of the pore space with and without connected smectite nano-pores. The large-scale impact of variations in accessibility and dissolution rates are then determined through continuum scale modeling using grid-cell specific information on accessible surface areas. This approach will be compared with a traditional continuum scale model using mineral abundances and common surface area estimates. Ultimately, the effectiveness of advanced surface area characterization to improve mineral dissolution rates will be evaluated by comparison of model results with dissolution rates measured from a flow-through column experiment.

Fundamental Studies of Clay and Clay-rich Mineral Reactions with H2O-CO2 Fluids: Application to Geological Carbon Dioxide Sequestration

NASA Astrophysics Data System (ADS)

Chizmeshya, A. V.

2016-12-01

Geological sequestration is currently being actively developed as a near-term, large-scale carbon sequestration technology in which supercritical carbon dioxide (scCO2) is injected below-ground into saline aquifers, depleted and existing oil and gas reservoir. Implementation strongly depends on the specific geological profile of each candidate injection site. Caprock formations that contain swellable clay minerals are of particular concern, since interaction with injected CO2 may produce complex local structural effects related to shrinkage, desiccation, and plastic response leading to CO2 escape. The current knowledge-base on rock-brine-CO2 interactions often relies on semi-empirical geochemical modeling and autoclave experiments, which necessitate quenching (de-gassing) to ambient conditions for characterization. To avoid these effects we used a moissanite-based microreaction system (Diefenbacher, J et al Rev. Mod. Inst., 76 15103 (2005)) which enables in situ synchrotron characterization of interactions under constant CO2 activity. Synchrotron studies were performed at the GSECARS sector of the Argonne National Lab APS to systematically determine the response of representative Ca- and Na-montmorillonites (STx-1, SWy-1) clays to dry/wet scCO2 (H2O-rich) fluids at T and P encountered in typical aquifers. Our main findings for hydrated STx-1 are that desiccation occurs spontaneously on the scale of minutes-hours over a wide range of conditions in dry scCO2 via release of H2O with volume changes as large as 19% in relation to the initial volume. Desiccation was not observed in wet scCO2, or in corresponding saline solutions containing 1-3 M NaCl, but quenching to ambient conditions from low-pressures leads to re-hydration in STx-1 suggesting a pressure-dependent diffusion barrier for H2O from the clay into bulk scCO2. Similar desiccation transitions with smaller volume changes of 5-9% were also observed in SWy-1 at P 140 atm and T 40 C. At high pressures ( 200 atm) minor lamellar expansion was sometimes found in STx-1 suggesting the possible intercalation of CO2. Our diffraction studies reveal an intriguing relationship between the critical dehydration temperatures and pressures, with bounds defined by critical properties of CO2.

Trace Uranium Partitioning in a Multiphase Nano-FeOOH System.

PubMed

McBriarty, Martin E; Soltis, Jennifer A; Kerisit, Sebastien; Qafoku, Odeta; Bowden, Mark E; Bylaska, Eric J; De Yoreo, James J; Ilton, Eugene S

2017-05-02

The characterization of trace elements in minerals using extended X-ray absorption fine structure (EXAFS) spectroscopy constitutes a first step toward understanding how impurities and contaminants interact with the host phase and the environment. However, limitations to EXAFS interpretation complicate the analysis of trace concentrations of impurities that are distributed across multiple phases in a heterogeneous system. Ab initio molecular dynamics (AIMD)-informed EXAFS analysis was employed to investigate the immobilization of trace uranium associated with nanophase iron (oxyhydr)oxides, a model system for the geochemical sequestration of radiotoxic actinides. The reductive transformation of ferrihydrite [Fe(OH) 3 ] to nanoparticulate iron oxyhydroxide minerals in the presence of uranyl (UO 2 ) 2+ (aq) resulted in the preferential incorporation of U into goethite (α-FeOOH) over lepidocrocite (γ-FeOOH), even though reaction conditions favored the formation of excess lepidocrocite. This unexpected result is supported by atomically resolved transmission electron microscopy. We demonstrate how AIMD-informed EXAFS analysis lifts the strict statistical limitations and uncertainty of traditional shell-by-shell EXAFS fitting, enabling the detailed characterization of the local bonding environment, charge compensation mechanisms, and oxidation states of polyvalent impurities in complex multiphase mineral systems.

Hierarchical Pore Morphology of Cretaceous Shale: A Small-Angle Neutron Scattering and Ultrasmall-Angle Neutron Scattering Study

DOE PAGES

Bahadur, J.; Melnichenko, Y. B.; Mastalerz, Maria; ...

2014-09-25

Shale reservoirs are becoming an increasingly important source of oil and natural gas supply and a potential candidate for CO 2 sequestration. Understanding the pore morphology in shale may provide clues to making gas extraction more efficient and cost-effective. The porosity of Cretaceous shale samples from Alberta, Canada, collected from different depths with varying mineralogical compositions, has been investigated by small- and ultrasmall-angle neutron scattering. Moreover these samples come from the Second White Specks and Belle Fourche formations, and their organic matter content ranges between 2 and 3%. The scattering length density of the shale specimens has been estimated usingmore » the chemical composition of the different mineral components. Scattering experiments reveal the presence of fractal and non-fractal pores. It has been shown that the porosity and specific surface area are dominated by the contribution from meso- and micropores. The fraction of closed porosity has been calculated by comparing the porosities estimated by He pycnometry and scattering techniques. There is no correlation between total porosity and mineral components, a strong correlation has been observed between closed porosity and major mineral components in the studied specimens.« less

Sequestration of non-pure carbon dioxide streams in iron oxyhydroxide-containing saline repositories

USGS Publications Warehouse

Garcia, S.; Rosenbauer, Robert J.; Palandri, James L.; Maroto-Valer, M. Mercedes

2012-01-01

Iron oxyhydroxide, goethite (α-FeOOH), was evaluated as a potential formation mineral reactant for trapping CO2 in a mineral phase such as siderite (FeCO3), when a mixture of CO2-SO 2 flue gas is injected into a saline aquifer. Two thermodynamic simulations were conducted, equilibrating a CO2-SO2 fluid mixture with a NaCl-brine and Fe-rich rocks at 150 °C and 300 bar. The modeling studies evaluated mineral and fluid composition at equilibrium and the influence of pH buffering in the system. Results show siderite precipitates both in the buffered and unbuffered system; however, the presence of an alkaline pH buffer enhances the stability of the carbonate. Based on the model, an experiment was designed to compare with thermodynamic predictions. A CO2-SO2 gas mixture was reacted in 150 ml of NaCl-NaOH brine containing 10 g of goethite at 150 °C and 300 bar for 24 days. Mineralogical and brine chemistry confirmed siderite as the predominant reaction product in the system. Seventy-six mg of CO2 are sequestered in siderite per 10 g of goethite.

Trace Uranium Partitioning in a Multiphase Nano-FeOOH System

DOE Office of Scientific and Technical Information (OSTI.GOV)

McBriarty, Martin E.; Soltis, Jennifer A.; Kerisit, Sebastien

The characterization of trace elements in minerals using extended X-ray absorption fine structure (EXAFS) spectroscopy constitutes a first step toward understanding how impurities and contaminants interact with the host phase and the environment. However, limitations to EXAFS interpretation complicate the analysis of trace concentrations of impurities that are distributed across multiple phases in a heterogeneous system. Ab initio molecular dynamics (AIMD)-informed EXAFS analysis was employed to investigate the immobilization of trace uranium associated with nanophase iron (oxyhydr)oxides, a model system for the geochemical sequestration of radiotoxic actinides. The reductive transformation of ferrihydrite [Fe(OH)3] to nanoparticulate iron oxyhydroxide minerals in themore » presence of uranyl (UO 2) 2+(aq) resulted in the preferential incorporation of U into goethite (α-FeOOH) over lepidocrocite (γ-FeOOH), even though reaction conditions favored the formation of excess lepidocrocite. This unexpected result is supported by atomically resolved transmission electron microscopy. We demonstrate how AIMD-informed EXAFS analysis lifts the strict statistical limitations and uncertainty of traditional shell-by-shell EXAFS fitting, enabling the detailed characterization of the local bonding environment, charge compensation mechanisms, and oxidation states of polyvalent impurities in complex multiphase mineral systems.« less

Greening the Mixture: An Evaluation of the Department of Defense’s Alternative Aviation Fuel Strategy

DTIC Science & Technology

2012-06-08

process begins with gasification of feedstocks such as coal, natural gas, or biomass towards the production of alternative fuels. With adequate carbon...Barrels per day CBTL Coal and Biomass to Liquid CCS Carbon Dioxide Capture and Sequestration CTL Coal to Liquid DARPA Defense Advanced Research...sequestration. Captured carbon dioxide from coal-to-liquid (CTL) or coal and biomass -to-liquid (CBTL) production could be readily injected into the

Experimental investigation of CO2-brine-rock interactions at elevated temperature and pressure: Implications for CO2 sequestration in deep-saline aquifers

USGS Publications Warehouse

Rosenbauer, R.J.; Koksalan, T.; Palandri, J.L.

2005-01-01

Deep-saline aquifers are potential repositories for excess CO2, currently being emitted to the atmosphere from anthropogenic activities, but the reactivity of supercritical CO2 with host aquifer fluids and formation minerals needs to be understood. Experiments reacting supercritical CO2 with natural and synthetic brines in the presence and absence of limestone and plagioclase-rich arkosic sandstone showed that the reaction of CO2-saturated brine with limestone results in compositional, mineralogical, and porosity changes in the aquifer fluid and rock that are dependent on initial brine composition, especially dissolved calcium and sulfate. Experiments reacting CO2-saturated, low-sulfate brine with limestone dissolved 10% of the original calcite and increased rock porosity by 2.6%. Experiments reacting high-sulfate brine with limestone, both in the presence and absence of supercritical CO2, were characterized by the precipitation of anhydrite, dolomitization of the limestone, and a final decrease in porosity of 4.5%. However, based on favorable initial porosity changes of about 15% due to the dissolution of calcite, the combination of CO2 co-injection with other mitigation strategies might help alleviate some of the well-bore scale and formation-plugging problems near the injection zone of a brine disposal well in Paradox Valley, Colorado, as well as provide a repository for CO2. Experiments showed that the solubility of CO2 is enhanced in brine in the presence of limestone by 9% at 25 ??C and 6% at 120 ??C and 200 bar relative to the brine itself. The solubility of CO2 is enhanced also in brine in the presence of arkosic sandstone by 5% at 120 ??C and 300 bar. The storage of CO 2 in limestone aquifers is limited to only ionic and hydraulic trapping. However, brine reacted with supercritical CO2 and arkose yielded fixation and sequestration of CO2 in carbonate mineral phases. Brine desiccation was observed in all experiments containing a discrete CO2 phase, promoting porosity-reducing precipitation reactions in aquifers near saturation with mineral phases. Published by Elsevier B.V.

Fluid transport in reaction induced fractures

NASA Astrophysics Data System (ADS)

Ulven, Ole Ivar; Sun, WaiChing; Malthe-Sørenssen, Anders

2015-04-01

The process of fracture formation due to a volume increasing chemical reaction has been studied in a variety of different settings, e.g. weathering of dolerites by Røyne et al. te{royne}, serpentinization and carbonation of peridotite by Rudge et al. te{rudge} and replacement reactions in silica-poor igneous rocks by Jamtveit et al. te{jamtveit}. It is generally assumed that fracture formation will increase the net permeability of the rock, and thus increase the reactant transport rate and subsequently the total rate of material conversion, as summarised by Kelemen et al. te{kelemen}. Ulven et al. te{ulven_1} have shown that for fluid-mediated processes the ratio between chemical reaction rate and fluid transport rate in bulk rock controls the fracture pattern formed, and Ulven et al. te{ulven_2} have shown that instantaneous fluid transport in fractures lead to a significant increase in the total rate of the volume expanding process. However, instantaneous fluid transport in fractures is clearly an overestimate, and achievable fluid transport rates in fractures have apparently not been studied in any detail. Fractures cutting through an entire domain might experience relatively fast advective reactant transport, whereas dead-end fractures will be limited to diffusion of reactants in the fluid, internal fluid mixing in the fracture or capillary flow into newly formed fractures. Understanding the feedback process between fracture formation and permeability changes is essential in assessing industrial scale CO2 sequestration in ultramafic rock, but little is seemingly known about how large the permeability change will be in reaction-induced fracturing. In this work, we study the feedback between fracture formation during volume expansion and fluid transport in different fracture settings. We combine a discrete element model (DEM) describing a volume expanding process and the related fracture formation with different models that describe the fluid transport in the fractures. This provides new information on how much reaction induced fracturing might accelerate a volume expanding process. Jamtveit, B, Putnis, C. V., and Malthe-Sørenssen, A., ``Reaction induced fracturing during replacement processes,'' Contrib. Mineral Petrol. 157, 2009, pp. 127 - 133. Kelemen, P., Matter, J., Streit, E. E., Rudge, J. F., Curry, W. B., and Blusztajn, J., ``Rates and Mechanisms of Mineral Carbonation in Peridotite: Natural Processes and Recipes for Enhanced, in situ CO2 Capture and Storage,'' Annu. Rev. Earth Planet. Sci. 2011. 39:545 - 76. Rudge, J. F., Kelemen, P. B., and Spiegelman, M., ``A simple model of reaction induced cracking applied to serpentinization and carbonation of peridotite,'' Earth Planet. Sc. Lett. 291, Issues 1-4, 2010, pp. 215 - 227. Røyne, A., Jamtveit, B., and Malthe-Sørenssen, A., ``Controls on rock weathering rates by reaction-induced hierarchial fracturing,'' Earth Planet. Sc. Lett. 275, 2008, pp. 364 - 369. Ulven, O. I., Storheim, H., Austrheim, H., and Malthe-Sørenssen, A. ``Fracture initiation during volume increasing reactions in rocks and applications for CO2 sequestration'', Earth Planet. Sc. Lett. 389C, 2014, pp. 132 - 142, doi:10.1016/j.epsl.2013.12.039. Ulven, O. I., Jamtveit, B., and Malthe-Sørenssen, A., ``Reaction-driven fracturing of porous rock'', J. Geophys. Res. Solid Earth 119, 2014, doi:10.1002/2014JB011102.

Mitigation of greenhouse gases emissions impact and their influence on terrestrial ecosystem.

NASA Astrophysics Data System (ADS)

Wójcik Oliveira, K.; Niedbała, G.

2018-05-01

Nowadays, one of the most important challenges faced by the humanity in the current century is the increasing temperature on Earth, caused by a growing emission of greenhouse gases into the atmosphere. Terrestrial ecosystems, as an important component of the carbon cycle, play an important role in the sequestration of carbon, which is a chance to improve the balance of greenhouse gases. Increasing CO2 absorption by terrestrial ecosystems is one way to reduce the atmospheric CO2 emissions. Sequestration of CO2 by terrestrial ecosystems is not yet fully utilized method of mitigating CO2 emission to the atmosphere. Terrestrial ecosystems, especially forests, are essential for the regulation of CO2 content in the atmosphere and more attention should be paid to seeking the natural processes of CO2 sequestration.

Strontium and cesium release mechanisms during unsaturated flow through waste-weathered Hanford sediments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chang, Hyun-Shik; Um, Wooyong; Rod, Kenton A.

2011-10-01

Leaching behavior of Sr and Cs in the vadose zone of Hanford site (WA, USA) was studied with laboratory-weathered sediments mimicking realistic conditions beneath the leaking radioactive waste storage tanks. Unsaturated column leaching experiments were conducted using background Hanford pore water focused on first 200 pore volumes. The weathered sediments were prepared by 6 months reaction with a synthetic Hanford tank waste leachate containing Sr and Cs (10-5 and 10-3 molal representative of LO- and HI-sediment, respectively) as surrogates for 90Sr and 137Cs. The mineral composition of the weathered sediments showed that zeolite (chabazite-type) and feldspathoid (sodalite-type) were the majormore » byproducts but different contents depending on the weathering conditions. Reactive transport modeling indicated that Cs leaching was controlled by ion-exchange, while Sr release was affected primarily by dissolution of the secondary minerals. The later release of K, Al, and Si from the HI-column indicated the additional dissolution of a more crystalline mineral (cancrinite-type). A two-site ion-exchange model successfully simulated the Cs release from the LO-column. However, a three-site ion-exchange model was needed for the HI-column. The study implied that the weathering conditions greatly impact the speciation of the secondary minerals and leaching behavior of sequestrated Sr and Cs.« less

Experiment and simulation study on the effects of cement minerals on the water-rock-CO2 interaction during CO2 geological storage

NASA Astrophysics Data System (ADS)

Liu, N.; Cheng, J.

2016-12-01

The CO2 geological storage is one of the most promising technology to mitigate CO2 emission. The fate of CO2 underground is dramatically affected by the CO2-water-rock interaction, which are mainly dependent on the initial aquifer mineralogy and brine components. The cement minerals are common materials in sandstone reservoir but few attention has been paid for its effects on CO2-water-rock interaction. Five batch reactions, in which 5% cement minerals were assigned to be quartz, calcite, dolomite, chlorite and Ca-montmorillonite, respectively, were conducted to understanding the cement minerals behaviors and its corresponding effects on the matrix minerals alterations during CO2 geological storage. Pure mineral powders were selected to mix and assemble the 'sandstone rock' with different cement components meanwhile keeping the matrix minerals same for each group as 70% quartz, 20% K-feldspar and 5% albite. These `rock' reacted with 750ml deionized water and CO2 under 180° and 18MPa for 15 days, during which the water chemistry evolution and minerals surface micromorphology changes has been monitored. The minerals saturation indexes calculation and phase diagram as well as the kinetic models were made by PHREEQC to uncover the minerals reaction paths. The experiment results indicated that the quartz got less eroded, on the contrary, K-feldspar and albite continuously dissolved to favor the gibbsite and kaolinite precipitations. The carbonates cement minerals quickly dissolved to reach equilibrium with the pH buffered and in turn suppressed the alkali feldspar dissolutions. No carbonates minerals precipitations occurred until the end of reactions for all groups. The simulation results were basically consistent with the experiment record but failed to simulate the non-stoichiometric reactions and the minerals kinetic rates seemed underestimated at the early stage of reactions. The cement minerals significantly dominated the reaction paths during CO2 geological storage and its effects on the CO2-water-rock interaction should be focused no matter for the benefit of injection sustainability or carbon sequestration capability. And more cement minerals such as ankerite should be included and the reservoir quality changes should also be taken consideration in the further study.

In situ measurement of magnesium carbonate formation from CO2 using static high-pressure and -temperature 13C NMR.

PubMed

Surface, J Andrew; Skemer, Philip; Hayes, Sophia E; Conradi, Mark S

2013-01-02

We explore a new in situ NMR spectroscopy method that possesses the ability to monitor the chemical evolution of supercritical CO(2) in relevant conditions for geological CO(2) sequestration. As a model, we use the fast reaction of the mineral brucite, Mg(OH)(2), with supercritical CO(2) (88 bar) in aqueous conditions at 80 °C. The in situ conversion of CO(2) into metastable and stable carbonates is observed throughout the reaction. After more than 58 h of reaction, the sample was depressurized and analyzed using in situ Raman spectroscopy, where the laser was focused on the undisturbed products through the glass reaction tube. Postreaction, ex situ analysis was performed on the extracted and dried products using Raman spectroscopy, powder X-ray diffraction, and magic-angle spinning (1)H-decoupled (13)C NMR. These separate methods of analysis confirmed a spatial dependence of products, possibly caused by a gradient of reactant availability, pH, and/or a reaction mechanism that involves first forming hydroxy-hydrated (basic, hydrated) carbonates that convert to the end-product, anhydrous magnesite. This carbonation reaction illustrates the importance of static (unmixed) reaction systems at sequestration-like conditions.

Evaluation of Advanced Reactive Surface Area Estimates for Improved Prediction of Mineral Reaction Rates in Porous Media

NASA Astrophysics Data System (ADS)

Beckingham, L. E.; Mitnick, E. H.; Zhang, S.; Voltolini, M.; Yang, L.; Steefel, C. I.; Swift, A.; Cole, D. R.; Sheets, J.; Kneafsey, T. J.; Landrot, G.; Anovitz, L. M.; Mito, S.; Xue, Z.; Ajo Franklin, J. B.; DePaolo, D.

2015-12-01

CO2 sequestration in deep sedimentary formations is a promising means of reducing atmospheric CO2 emissions but the rate and extent of mineral trapping remains difficult to predict. Reactive transport models provide predictions of mineral trapping based on laboratory mineral reaction rates, which have been shown to have large discrepancies with field rates. This, in part, may be due to poor quantification of mineral reactive surface area in natural porous media. Common estimates of mineral reactive surface area are ad hoc and typically based on grain size, adjusted several orders of magnitude to account for surface roughness and reactivity. This results in orders of magnitude discrepancies in estimated surface areas that directly translate into orders of magnitude discrepancies in model predictions. Additionally, natural systems can be highly heterogeneous and contain abundant nano- and micro-porosity, which can limit connected porosity and access to mineral surfaces. In this study, mineral-specific accessible surface areas are computed for a sample from the reservoir formation at the Nagaoka pilot CO2 injection site (Japan). Accessible mineral surface areas are determined from a multi-scale image analysis including X-ray microCT, SEM QEMSCAN, XRD, SANS, and SEM-FIB. Powder and flow-through column laboratory experiments are performed and the evolution of solutes in the aqueous phase is tracked. Continuum-scale reactive transport models are used to evaluate the impact of reactive surface area on predictions of experimental reaction rates. Evaluated reactive surface areas include geometric and specific surface areas (eg. BET) in addition to their reactive-site weighted counterparts. The most accurate predictions of observed powder mineral dissolution rates were obtained through use of grain-size specific surface areas computed from a BET-based correlation. Effectively, this surface area reflects the grain-fluid contact area, or accessible surface area, in the powder dissolution experiment. In the model of the flow-through column experiment, the accessible mineral surface area, computed from the multi-scale image analysis, is evaluated in addition to the traditional surface area estimates.

Experimental observation and numerical simulation of permeability changes in dolomite at CO2 sequestration conditions

NASA Astrophysics Data System (ADS)

Tutolo, B. M.; Luhmann, A. J.; Kong, X.; Saar, M. O.; Seyfried, W. E.

2013-12-01

Injecting surface temperature CO2 into geothermally warm reservoirs for geologic storage or energy production may result in depressed temperature near the injection well and thermal gradients and mass transfer along flow paths leading away from the well. Thermal gradients are particularly important to consider in reservoirs containing carbonate minerals, which are more soluble at lower temperatures, as well as in CO2-based geothermal energy reservoirs where lowering heat exchanger rejection temperatures increases efficiency. Additionally, equilibrating a fluid with cation-donating silicates near a low-temperature injection well and transporting the fluid to higher temperature may enhance the kinetics of mineral precipitation in such a way as to overcome the activation energy required for mineral trapping of CO2. We have investigated this process by subjecting a dolomite core to a 650-hour temperature series experiment in which the fluid was saturated with CO2 at high pressure (110-126 bars) and 21°C. This fluid was recirculated through the dolomite core, increasing permeability from 10-16 to 10-15.2 m2. Subsequently, the core temperature was raised to 50° C, and permeability decreased to 10-16.2 m2 after 289 hours, due to thermally-driven CO2 exsolution. Increasing core temperature to 100°C for the final 145 hours of the experiment caused dolomite to precipitate, which, together with further CO2 exsolution, decreased permeability to 10-16.4 m2. Post-experiment x-ray computed tomography and scanning electron microscope imagery of the dolomite core reveals abundant matrix dissolution and enlargement of flow paths at low temperatures, and subsequent filling-in of the passages at elevated temperature by dolomite. To place this experiment within the broader context of geologic CO2 sequestration, we designed and utilized a reactive transport simulator that enables dynamic calculation of CO2 equilibrium constants and fugacity and activity coefficients by incorporating mineral, fluid, and aqueous species equations of state into its structure. Phase equilibria calculations indicate that fluids traveling away from the depressed temperature zone near the injection well may exsolve and precipitate up to 200 cc CO2, 1.45 cc dolomite, and 2.3 cc calcite, per kg, but we use the reactive transport simulator to place more realistic limits on these calculations. The simulations show that thermally-induced CO2 exsolution creates velocity gradients within the modeled domain, leading to increased velocities at lower pressure due to the increasingly gas-like density of CO2. Because dolomite precipitation kinetics strongly depend on temperature, modeled dolomite precipitation effectively concentrates within high temperature regions, while calcite precipitation is predicted to occur over a broader range. Additionally, because the molar volume of dolomite is almost double that of calcite, transporting a low temperature, dolomite-saturated fluid across a thermal gradient can lead to more substantial pore space clogging. We conclude that injecting cool CO2 into geothermally warm reservoirs may substantially alter formation porosity, permeability, and injectivity, and can result in favorable conditions for permanent storage of CO2 as a solid carbonate phase.

Assessing carbon stocks, carbon sequestration, and greenhouse-gas fluxes in ecosystems of the United States under present conditions and future scenarios

USGS Publications Warehouse

Zhu, Zhi-Liang; Stackpoole, Sarah

2011-01-01

The Energy Independence and Security Act of 2007 (EISA) requires the U.S. Department of the Interior (DOI) to develop a methodology and conduct an assessment of carbon storage, carbon sequestration, and greenhouse-gas (GHG) fluxes in the Nation's ecosystems. The U.S. Geological Survey (USGS) has developed and published the methodology (U.S. Geological Survey Scientific Investigations Report 2010-5233) and has assembled an interdisciplinary team of scientists to conduct the assessment over the next three to four years, commencing in October 2010. The assessment will fulfill specific requirements of the EISA by (1) quantifying, measuring, and monitoring carbon sequestration and GHG fluxes using national datasets and science tools such as remote sensing, and biogeochemical and hydrological models, (2) evaluating a range of management and restoration activities for their effects on carbon-sequestration capacity and the reduction of GHG fluxes, and (3) assessing effects of climate change and other controlling processes (including wildland fires) on carbon uptake and GHG emissions from ecosystems.

New insights into the nation's carbon storage potential

USGS Publications Warehouse

Warwick, Peter D.; Zhu, Zhi-Liang

2012-01-01

Carbon sequestration is a method of securing carbon dioxide (CO2) to prevent its release into the atmosphere, where it contributes to global warming as a greenhouse gas. Geologic storage of CO2 in porous and permeable rocks involves injecting high-pressure CO2 into a subsurface rock unit that has available pore space. Biologic carbon sequestration refers to both natural and anthropogenic processes by which CO2 is removed from the atmosphere and stored as carbon in vegetation, soils, and sediments.

Molecular and Metabolic Mechanisms of Carbon Sequestration in Marine Thrombolites

NASA Technical Reports Server (NTRS)

Mobberley, Jennifer

2013-01-01

The overall goal of my dissertation project has been to examine the molecular processes underlying carbon sequestration in lithifying microbial ecosystems, known as thrombolitic mats, and assess their feasibility for use in bioregenerative life support systems. The results of my research and education efforts funded by the Graduate Student Researchers Program can be summarized in four peer-reviewed research publication, one educational publication, two papers in preparation, and six research presentations at local and national science meetings (see below for specific details).

Calcium, magnesium, and phosphorus metabolism in dogs given intravenous triacetin.

PubMed

Bailey, J W; Heath, H; Miles, J M

1989-02-01

Previous studies suggested that acetate in parenteral solutions may adversely affect mineral metabolism by causing sequestration of inorganic phosphate and calcium in the liver. In this study, triacetin, a short-chain triglyceride of acetate and a potential parenteral nutrient, was infused for 3 h at an isocaloric rate in mongrel dogs (n = 6) to test its effects on serum phosphorus, calcium, and magnesium metabolism. There was no change in serum P or Ca. The serum Mg concentration decreased from 0.7 +/- 0.03 to 0.57 +/- 0.03 mmol/L (p less than 0.001) by 90 min and remained at this level for the remainder of the study. The triacetin infusion did not influence fractional urinary Mg excretion; thus, the decrease in serum Mg was likely because of an increase in cellular transport of this cation. A short-chain triglyceride administered to dogs at a rate approximating resting energy expenditure has no demonstrable adverse effects on mineral metabolism.

Early Implementation of Large Scale Carbon Dioxide Removal Projects through the Cement Industry

NASA Astrophysics Data System (ADS)

Zeman, F. S.

2014-12-01

The development of large-scale carbon dioxide reduction projects requires high purity CO2and a reactive cation source. A project seeking to provide both of these requirements will likely face cost barriers with current carbon prices. The cement industry is a suitable early implementation site for such projects by virtue of the properties of its exhaust gases and those of waste concrete. Cement plants are the second largest source of industrial CO2 emissions, globally. It is also the second largest commodity after water, has no ready substitute and is literally the foundation of society. Finally, half of the CO2 emissions originate from process reactions rather than fossil fuel combustion resulting in higher flue gas CO2concentrations. These properties, with the co-benefits of oxygen combustion, create a favorable environment for spatially suitable projects. Oxygen combustion involves substituting produced oxygen for air in a combustion reaction. The absence of gaseous N2 necessitates the recirculation of exhaust gases to maintain kiln temperatures, which increase the CO2 concentrations from 28% to 80% or more. Gas exit temperatures are also elevated (>300oC) and can reach higher temperatures if the multi stage pre-heater towers, that recover heat, are re-designed in light of FGR. A ready source of cations can be found in waste concrete, a by-product of construction and demolition activities. These wastes can be processed to remove cations and then reacted with atmospheric CO2 to produce carbonate minerals. While not carbon negative, they represent a demonstration opportunity for binding atmospheric CO2while producing a saleable product (precipitated calcium carbonate). This paper will present experimental results on PCC production from waste concrete along with modeling results for oxygen combustion at cement facilities. The results will be presented with a view to mineral sequestration process design and implementation.

The United States Department of Energy's Regional Carbon Sequestration Partnerships program: a collaborative approach to carbon management.

PubMed

Litynski, John T; Klara, Scott M; McIlvried, Howard G; Srivastava, Rameshwar D

2006-01-01

This paper reviews the Regional Carbon Sequestration Partnerships (RCSP) concept, which is a first attempt to bring the U.S. Department of Energy's (DOE) carbon sequestration program activities into the "real world" by using a geographically-disposed-system type approach for the U.S. Each regional partnership is unique and covers a unique section of the U.S. and is tasked with determining how the research and development activities of DOE's carbon sequestration program can best be implemented in their region of the country. Although there is no universal agreement on the cause, it is generally understood that global warming is occurring, and many climate scientists believe that this is due, in part, to the buildup of carbon dioxide (CO(2)) in the atmosphere. This is evident from the finding presented in the National Academy of Science Report to the President on Climate Change which stated "Greenhouse gases are accumulating in Earth's atmosphere as a result of human activities, causing surface air temperatures and subsurface ocean temperatures to rise. Temperatures are, in fact, rising. The changes observed over the last several decades are likely mostly due to human activities, ...". In the United States, emissions of CO(2) originate mainly from the combustion of fossil fuels for energy production, transportation, and other industrial processes. Roughly one third of U.S. anthropogenic CO(2) emissions come from power plants. Reduction of CO(2) emissions through sequestration of carbon either in geologic formations or in terrestrial ecosystems can be part of the solution to the problem of global warming. However, a number of steps must be accomplished before sequestration can become a reality. Cost effective capture and separation technology must be developed, tested, and demonstrated; a database of potential sequestration sites must be established; and techniques must be developed to measure, monitor, and verify the sequestered CO(2). Geographical differences in fossil fuel use, the industries present, and potential sequestration sinks across the United States dictate the use of a regional approach to address the sequestration of CO(2). To accommodate these differences, the DOE has created a nationwide network of seven Regional Carbon Sequestration Partnerships (RCSP) to help determine and implement the carbon sequestration technologies, infrastructure, and regulations most appropriate to promote CO(2) sequestration in different regions of the nation. These partnerships currently represent 40 states, three Indian Nations, four Canadian Provinces, and over 200 organizations, including academic institutions, research institutions, coal companies, utilities, equipment manufacturers, forestry and agricultural representatives, state and local governments, non-governmental organizations, and national laboratories. These partnerships are dedicated to developing the necessary infrastructure and validating the carbon sequestration technologies that have emerged from DOE's core R&D and other programs to mitigate emissions of CO(2), a potent greenhouse gas. The partnerships provide a critical link to DOE's plans for FutureGen, a highly efficient and technologically sophisticated coal-fired power plant that will produce both hydrogen and electricity with near-zero emissions. Though limited to the situation in the U.S., the paper describes for the international scientific community the approach being taken by the U.S. to prepare for carbon sequestration, should that become necessary.

Vegetation turnover and nitrogen feedback drive temperate forest carbon sequestration in response to elevated CO[2]. A multi-model structural analysis

NASA Astrophysics Data System (ADS)

Walker, A. P.; Zaehle, S.; Medlyn, B. E.; De Kauwe, M. G.; Asao, S.; Hickler, T.; Lomas, M. R.; Pak, B. C.; Parton, W. J.; Quegan, S.; Ricciuto, D. M.; Wang, Y.; Warlind, D.; Norby, R. J.

2013-12-01

Predicting forest carbon (C) sequestration requires understanding the processes leading to rates of biomass C accrual (net primary productivity; NPP) and loss (turnover). In temperate forest ecosystems, experiments and models have shown that feedback via progressive nitrogen limitation (PNL) is a key driver of NPP responses to elevated CO[2]. In this analysis we show that while still important, PNL may not be as severe a constraint on NPP as indicated by some studies and that the response of turnover to elevated CO[2] could be as important, especially in the near to medium term. Seven terrestrial ecosystem and biosphere models that couple C and N cycles with varying assumptions and complexity were used to simulate responses over 300 years to a step change in CO[2] to 550 ppmv. Simulations were run for the evergreen needleleaf Duke forest and the deciduous broadleaf Oak Ridge forest FACE experiments. Whether or not a model simulated PNL under elevated CO[2] depended on model structure and the timescale of observation. Avoiding PNL depended on mechanisms that reduced ecosystem N losses. The two key assumptions that reduced N losses were whether plant N uptake was based on plant N demand and whether ecosystem N losses (volatisation and leaching) were dependent on the concentration of N in the soil solution. Assumptions on allocation and turnover resulted in very different responses of turnover to elevated CO[2], which had profound implications for C sequestration. For example, at equilibrium CABLE2.0 predicted an increase in vegetation C sequestration despite decreased NPP, while O-CN predicted much less vegetation C sequestration than would be expected from predicted NPP increases alone. Generally elevated CO[2] favoured a shift in C partitioning towards longer lived wood biomass, which increased vegetation turnover and enhanced C sequestration. Enhanced wood partitioning was overlaid by increases or decreases in self-thinning depended on whether self-thinning was simply a function of forest structure, or structure and NPP. Self-thinning assumptions altered equilibrium C sequestration and were extremely important for the immediate transient response and near-term prediction of C sequestration.

Application of a pore-scale reactive transport model to a natural analog for reaction-induced pore alterations

DOE PAGES

Yoon, Hongkyu; Major, Jonathan; Dewers, Thomas; ...

2017-01-05

Dissolved CO 2 in the subsurface resulting from geological CO 2 storage may react with minerals in fractured rocks, confined aquifers, or faults, resulting in mineral precipitation and dissolution. The overall rate of reaction can be affected by coupled processes including hydrodynamics, transport, and reactions at the (sub) pore-scale. In this work pore-scale modeling of coupled fluid flow, reactive transport, and heterogeneous reactions at the mineral surface is applied to account for permeability alterations caused by precipitation-induced pore-blocking. This paper is motivated by observations of CO 2 seeps from a natural CO 2 sequestration analog, Crystal Geyser, Utah. Observations alongmore » the surface exposure of the Little Grand Wash fault indicate the lateral migration of CO 2 seep sites (i.e., alteration zones) of 10–50 m width with spacing on the order of ~100 m over time. Sandstone permeability in alteration zones is reduced by 3–4 orders of magnitude by carbonate cementation compared to unaltered zones. One granular porous medium and one fracture network systems are used to conceptually represent permeable porous media and locations of conduits controlled by fault-segment intersections and/or topography, respectively. Simulation cases accounted for a range of reaction regimes characterized by the Damköhler (Da) and Peclet (Pe) numbers. Pore-scale simulation results demonstrate that combinations of transport (Pe), geochemical conditions (Da), solution chemistry, and pore and fracture configurations contributed to match key patterns observed in the field of how calcite precipitation alters flow paths by pore plugging. This comparison of simulation results with field observations reveals mechanistic explanations of the lateral migration and enhances our understanding of subsurface processes associated with the CO 2 injection. In addition, permeability and porosity relations are constructed from pore-scale simulations which account for a range of reaction regimes characterized by the Da and Pe numbers. Finally, the functional relationships obtained from pore-scale simulations can be used in a continuum scale model that may account for large-scale phenomena mimicking lateral migration of surface CO 2 seeps.« less

Constraining Path-Dependent Processes During Basalt-CO2 Interactions with Observations From Flow-Through and Batch Experiments

NASA Astrophysics Data System (ADS)

Thomas, D.; Garing, C.; Zahasky, C.; Harrison, A. L.; Bird, D. K.; Benson, S. M.; Oelkers, E. H.; Maher, K.

2017-12-01

Predicting the timing and magnitude of CO2 storage in basaltic rocks relies partly on quantifying the dependence of reactivity on flow path and mineral distribution. Flow-through experiments that use intact cores are advantageous because the spatial heterogeneity of pore space and reactive phases is preserved. Combining aqueous geochemical analyses and petrologic characterization with non-destructive imaging techniques (e.g. micro-computed tomography) constrains the relationship between irreversible reactions, pore connectivity and accessible surface area. Our work enhances these capabilities by dynamically imaging flow through vesicular basalts with Positron Emission Tomography (PET) scanning. PET highlights the path a fluid takes by detecting photons produced during radioactive decay of an injected radiotracer (FDG). We have performed single-phase, CO2-saturated flow-through experiments with basaltic core from Iceland at CO2 sequestration conditions (50 °C; 76-90 bar Ptot). Constant flow rate and continuous pressure measurements at the inlet and outlet of the core constrain permeability. We monitor geochemical evolution through cation and anion analysis of outlet fluid sampled periodically. Before and after reaction, we perform PET scans and characterize the core using micro-CT. The PET scans indicate a discrete, localized flow path that appears to be a micro-crack connecting vesicles, suggesting that vesicle-lining minerals are immediately accessible and important reactants. Rapid increases in aqueous cation concentration, pH and HCO3- indicate that the rock reacts nearly immediately after CO2 injection. After 24 hours the solute release decreases, which may reflect a transition to reaction with phases with slower kinetic dissolution rates (e.g. zeolites and glasses to feldspar), a decrease in available reactive surface area or precipitation. We have performed batch experiments using crushed material of the same rock to elucidate the effect of flow path geometry and mineral accessibility on geochemical evolution. Interestingly, surface area-normalized dissolution rates as evinced by SiO2 release in all experiments approach similar values ( 10-15 mol/cm2/s). Our experiments show how imaging techniques are helpful in interpreting path-dependent processes in open systems.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yoon, Hongkyu; Major, Jonathan; Dewers, Thomas

Dissolved CO 2 in the subsurface resulting from geological CO 2 storage may react with minerals in fractured rocks, confined aquifers, or faults, resulting in mineral precipitation and dissolution. The overall rate of reaction can be affected by coupled processes including hydrodynamics, transport, and reactions at the (sub) pore-scale. In this work pore-scale modeling of coupled fluid flow, reactive transport, and heterogeneous reactions at the mineral surface is applied to account for permeability alterations caused by precipitation-induced pore-blocking. This paper is motivated by observations of CO 2 seeps from a natural CO 2 sequestration analog, Crystal Geyser, Utah. Observations alongmore » the surface exposure of the Little Grand Wash fault indicate the lateral migration of CO 2 seep sites (i.e., alteration zones) of 10–50 m width with spacing on the order of ~100 m over time. Sandstone permeability in alteration zones is reduced by 3–4 orders of magnitude by carbonate cementation compared to unaltered zones. One granular porous medium and one fracture network systems are used to conceptually represent permeable porous media and locations of conduits controlled by fault-segment intersections and/or topography, respectively. Simulation cases accounted for a range of reaction regimes characterized by the Damköhler (Da) and Peclet (Pe) numbers. Pore-scale simulation results demonstrate that combinations of transport (Pe), geochemical conditions (Da), solution chemistry, and pore and fracture configurations contributed to match key patterns observed in the field of how calcite precipitation alters flow paths by pore plugging. This comparison of simulation results with field observations reveals mechanistic explanations of the lateral migration and enhances our understanding of subsurface processes associated with the CO 2 injection. In addition, permeability and porosity relations are constructed from pore-scale simulations which account for a range of reaction regimes characterized by the Da and Pe numbers. Finally, the functional relationships obtained from pore-scale simulations can be used in a continuum scale model that may account for large-scale phenomena mimicking lateral migration of surface CO 2 seeps.« less

The Importance of linking In Situ Observation to Flux Measurement in Understanding Rhizosphere Dynamics in Scaling to Global Processes

NASA Astrophysics Data System (ADS)

Allen, M. F.; Taggart, M. C.; Hernandez, R. R.; Harmon, T. C.; Rundel, P.

2017-12-01

Observation is essential for organizing outputs from sensor data to describe dynamic phenomena regulating core processes. The rhizosphere is that region of the soil layer that regulates soil carbon acquisition, turnover, and sequestration and that is most sensitive to rapid changes in soil moisture, temperature, and gases. Virtually every process regulating carbon and nutrient immobilization and mineralization occur here at the maximum rates. However, the observation of root, microbial, and animal growth, movement, and mortality are rarely undertaken at time scales of crucial events. While multiple cores or observations can be taken in space, replications in time are rarely undertaken. We coupled automated (AMR) and manual minirhizotrons (MMR) with soil and aboveground sensors for temperature (T), water content (q), CO2, and O2 to measure short-term dynamics that regulate carbon cycling. AMRs imaged rhizospheres, multiple times daily. From these images, we observed timing of root and hyphal growth and mortality in response to changes in photosynthesis, diurnal temperature fluctuations, and precipitation and drought events. Replicate manual minirhizotron tubes describe the spatial structure of those events, and replicate core samples provide measurements of standing crop at known times. We present four examples showing how observation led to understanding unusual C flux patterns in mixed-conifer forest (belowground photosynthate allocation), hot desert (CaCO3 formation and weathering), grassland (root grazing), and tropical rainforest (soil gas flux patterns).

Permafrost soils and carbon cycling

DOE PAGES

Ping, C. L.; Jastrow, J. D.; Jorgenson, M. T.; ...

2015-02-05

Knowledge of soils in the permafrost region has advanced immensely in recent decades, despite the remoteness and inaccessibility of most of the region and the sampling limitations posed by the severe environment. These efforts significantly increased estimates of the amount of organic carbon stored in permafrost-region soils and improved understanding of how pedogenic processes unique to permafrost environments built enormous organic carbon stocks during the Quaternary. This knowledge has also called attention to the importance of permafrost-affected soils to the global carbon cycle and the potential vulnerability of the region's soil organic carbon (SOC) stocks to changing climatic conditions. Inmore » this review, we briefly introduce the permafrost characteristics, ice structures, and cryopedogenic processes that shape the development of permafrost-affected soils, and discuss their effects on soil structures and on organic matter distributions within the soil profile. We then examine the quantity of organic carbon stored in permafrost-region soils, as well as the characteristics, intrinsic decomposability, and potential vulnerability of this organic carbon to permafrost thaw under a warming climate. Overall, frozen conditions and cryopedogenic processes, such as cryoturbation, have slowed decomposition and enhanced the sequestration of organic carbon in permafrost-affected soils over millennial timescales. Due to the low temperatures, the organic matter in permafrost soils is often less humified than in more temperate soils, making some portion of this stored organic carbon relatively vulnerable to mineralization upon thawing of permafrost.« less

Mobilization of Trace Metals in an Experimental Carbon Sequestration Scenario

NASA Astrophysics Data System (ADS)

Marcon, V.; Kaszuba, J. P.

2012-12-01

Mobilizing trace metals with injection of supercritical CO2 into deep saline aquifers is a concern for geologic carbon sequestration. The potential for leakage from these systems requires an understanding of how injection reservoirs interact with the overlying potable aquifers. Hydrothermal experiments were performed to evaluate metal mobilization and mechanisms of release in a carbonate storage reservoir and at the caprock-reservoir boundary. Experiments react synthetic Desert Creek limestone and/or Gothic Shale, formations in the Paradox Basin, Utah, with brine that is close to equilibrium with these rocks. A reaction temperature of 1600C accelerates the reaction kinetics without changing in-situ water-rock reactions. The experiments were allowed to reach steady state before injecting CO2. Changes in major and trace element water chemistry, dissolved carbon and sulfide, and pH were tracked throughout the experiments. CO2 injection decreases the pH by 1 to 2 units; concomitant mineral dissolution produces elevated Ba, Cu, Fe, Pb, and Zn concentrations in the brine. Concentrations subsequently decrease to approximately steady state values after 120-330 hours, likely due to mineral precipitation as seen in SEM images and predicted by geochemical modeling. In experiments that emulate the caprock-reservoir boundary, final Fe (0.7ppb), an element of secondary concern for the EPA, and Pb (0.05ppb) concentrations exceed EPA limits, whereas Ba (0.140ppb), Cu (48ppb), and Zn (433ppb) values remain below EPA limits. In experiments that simulate deeper reservoir conditions, away from the caprock boundary, final Fe (3.5ppb) and Pb (0.017ppb) values indicate less mobilization than seen at the caprock-reservoir boundary, but values still exceed EPA limits. Barium concentrations always remain below the EPA limit of 2ppb, but are more readily mobilized in experiments replicating deeper reservoir conditions. In both systems, transition elements Cd, Cr, Cu, Pb and Zn behave in a similar manner, increasing in concentration with injection but continually decreasing after about 830 hours until termination of the experiment. SEM images and geochemical models indicate initial dissolution of all rocks and minerals, re-precipitation of Ca-Mg-Fe carbonates and Fe-sulfides, and precipitation of anhydrite in both systems. Calcite dissolves more readily than dolomite in these experiments, but re-precipitates in veins on dolomite. If brines leak from a storage reservoir and mix with a potable aquifer, the experimental results suggest that Ba, Cu, and Zn will not be contaminants of concern. Pb, Fe and As (still under consideration) initially exceed the EPA threshold and may require careful attention in a sequestration scenario. However, experimentally observed trends of decreasing trace metal concentration suggest that these metals could become less of a concern during the life of a carbon repository. Finally, the caprock plays an active role in trace metal mobilization in the system. The caprock provides a source of metals, although subsequent precipitation may remove metals from solution.

Carbon Sequestration and Peat Accretion Processes in Peatland Systems: A North-South Comparison

NASA Astrophysics Data System (ADS)

Richardson, C. J.; Wang, H.; Bridgham, S. D.

2012-12-01

Millions of hectares of peatlands exist in the U.S. and Canada but few comparisons have been made on the process controlling peat accretion, carbon sequestration and GHG losses across latitudinal gradients. Historic threats to carbon sequestration for these areas have been drainage and conversion to agriculture and forestry, which promotes the decomposition of the organic matter in the soil, leading to accelerated soil subsidence, severe carbon losses, and accelerated transport of C and nutrients to adjoining ecosystems. A more recent and insidious threat to the survival of peatlands worldwide is the increased temperature and drought conditions projected for many areas of global peatlands (IPCC 2007). A comparison of carbon sequestration rates and controlling processes for southeastern shrub bogs, the Florida Everglades and selected peatlands of the northern US and Canada under current climatic conditions reveals several major differences in controlling factors and rates of sequestration and carbon flux. Numerous studies have shown that drought or drainage can unlock historically stored carbon, thus releasing more CO2 ¬ and dissolved organic carbon (Blodau et al. 2004; Furukawa et al. 2005; Von Arnold et al. 2005; Hirano et al. 2007), and such effects might last for decades (Fenner & Freeman 2011). The main driver of this process is the O2 introduced by drought or drainage, which will increase the activity of phenol oxidase, then accelerate the decomposition of phenol compounds, which is generally considered the "enzymatic latch" for carbon storage in peatlands (Freeman et al. 2001). However, our recent studies in southeastern peatlands along the coast of North Carolina have found that drought or drainage does not affect CO2 emission in some southern peatlands where the initial water level is below the ground surface (unsaturated peats), as polyphenol increases rather than decreases. Our results suggest that additional controlling factors, rather than anoxia exist in unsaturated peats, allowing them to accumulate carbon, and resist decomposition and CO2 losses. The importance of native phenolic producing plant species and substrate quality are key controlling factors. Our study offers new evidence that frequently occurring summer drought or climate-induced moderate drought will not increase the loss of stored carbon in unsaturated peatlands. These findings have important ramifications concerning carbon storage and losses in peatlands under future climate change predictions.

Quantifying and Mapping the Supply of and Demand for Carbon Storage and Sequestration Service from Urban Trees

PubMed Central

Zhao, Chang; Sander, Heather A.

2015-01-01

Studies that assess the distribution of benefits provided by ecosystem services across urban areas are increasingly common. Nevertheless, current knowledge of both the supply and demand sides of ecosystem services remains limited, leaving a gap in our understanding of balance between ecosystem service supply and demand that restricts our ability to assess and manage these services. The present study seeks to fill this gap by developing and applying an integrated approach to quantifying the supply and demand of a key ecosystem service, carbon storage and sequestration, at the local level. This approach follows three basic steps: (1) quantifying and mapping service supply based upon Light Detection and Ranging (LiDAR) processing and allometric models, (2) quantifying and mapping demand for carbon sequestration using an indicator based on local anthropogenic CO2 emissions, and (3) mapping a supply-to-demand ratio. We illustrate this approach using a portion of the Twin Cities Metropolitan Area of Minnesota, USA. Our results indicate that 1735.69 million kg carbon are stored by urban trees in our study area. Annually, 33.43 million kg carbon are sequestered by trees, whereas 3087.60 million kg carbon are emitted by human sources. Thus, carbon sequestration service provided by urban trees in the study location play a minor role in combating climate change, offsetting approximately 1% of local anthropogenic carbon emissions per year, although avoided emissions via storage in trees are substantial. Our supply-to-demand ratio map provides insight into the balance between carbon sequestration supply in urban trees and demand for such sequestration at the local level, pinpointing critical locations where higher levels of supply and demand exist. Such a ratio map could help planners and policy makers to assess and manage the supply of and demand for carbon sequestration. PMID:26317530

In situ mid-infrared spectroscopic titration of forsterite with water in supercritical CO2: Dependence of mineral carbonation on quantitative water speciation

NASA Astrophysics Data System (ADS)

Loring, J. S.; Thompson, C. J.; Wang, Z.; Schaef, H. T.; Martin, P.; Qafoku, O.; Felmy, A. R.; Rosso, K. M.

2011-12-01

Geologic sequestration of carbon dioxide holds promise for helping mitigate CO2 emissions generated from the burning of fossil fuels. Supercritical CO2 (scCO2) plumes containing variable water concentrations (wet scCO2) will displace aqueous solution and dominate the pore space adjacent to caprocks. It is important to understand possible mineral reactions with wet scCO2 to better predict long-term caprock integrity. We introduce novel in situ instrumentation that enables quantitative titrations of reactant minerals with water in scCO2 at temperatures and pressures relevant to target geologic reservoirs. The system includes both transmission and attenuated total reflection mid-infrared optics. Transmission infrared spectroscopy is used to measure concentrations of water dissolved in the scCO2, adsorbed on mineral surfaces, and incorporated into precipitated carbonates. Single-reflection attenuated total reflection infrared spectroscopy is used to monitor water adsorption, mineral dissolution, and carbonate precipitation reactions. Results are presented for the infrared spectroscopic titration of forsterite (Mg2SiO4), a model divalent metal silicate, with water in scCO2 at 100 bar and at both 50 and 75°C. The spectral data demonstrate that the quantitative speciation of water as either dissolved or adsorbed is important for understanding the types, growth rates, and amounts of carbonate precipitates formed. Relationships between dissolved/adsorbed water, water concentrations, and the role of liquid-like adsorbed water are discussed. Our results unify previous in situ studies from our laboratory based on infrared spectroscopy, nuclear magnetic resonance spectroscopy and X-ray diffraction.

The path to a successful one-million tonne demonstration of geological sequestration: Characterization, cooperation, and collaboration

USGS Publications Warehouse

Finley, R.J.; Greenberg, S.E.; Frailey, S.M.; Krapac, I.G.; Leetaru, H.E.; Marsteller, S.

2011-01-01

The development of the Illinois Basin-Decatur USA test site for a 1 million tonne injection of CO2 into the Mount Simon Sandstone saline reservoir beginning in 2011 has been a multiphase process requiring a wide array of personnel and resources that began in 2003. The process of regional characterization took two years as part of a Phase I effort focused on the entire Illinois Basin, located in Illinois, Indiana, and Kentucky, USA. Seeking the cooperation of an industrial source of CO2 and site selection within the Basin took place during Phase II while most of the concurrent research emphasis was on a set of small-scale tests of Enhanced Oil Recovery (EOR) and CO2 injection into a coal seam. Phase III began the commitment to the 1 million-tonne test site development through the collaboration of the Archer Daniels Midland Company (ADM) who is providing a site, the CO2, and developing a compression facility, of Schlumberger Carbon Services who is providing expertise for operations, drilling, geophysics, risk assessment, and reservoir modelling, and of the Illinois State Geological Survey (ISGS) whose geologists and engineers lead the Midwest Geological Sequestration Consortium (MGSC). Communications and outreach has been a collaborative effort of ADM, ISGS and Schlumberger Carbon Services. The Consortium is one of the seven Regional Carbon Sequestration Partnerships, a carbon sequestration research program supported by the National Energy Technology Laboratory of the U.S. Department of Energy. ?? 2011 Published by Elsevier Ltd.

The dynamic nature of crystal growth in pores

DOE PAGES

Godinho, Jose R. A.; Gerke, Kirill M.; Stack, Andrew G.; ...

2016-09-12

We report that the kinetics of crystal growth in porous media controls a variety of natural processes such as ore genesis and crystallization induced fracturing that can trigger earthquakes and weathering, as well as, sequestration of CO 2 and toxic metals into geological formations. Progress on understanding those processes has been limited by experimental difficulties of dynamically studying the reactive surface area and permeability during pore occlusion. Here, we show that these variables cause a time-dependency of barite growth rates in microporous silica. The rate is approximately constant and similar to that observed on free surfaces if fast flow velocitiesmore » predominate and if the time-dependent reactive surface area is accounted for. As the narrower flow paths clog, local flow velocities decrease, which causes the progressive slowing of growth rates. We conclude that mineral growth in a microporous media can be estimated based on free surface studies when a) the growth rate is normalized to the time-dependent surface area of the growing crystals, and b) the local flow velocities are above the limit at which growth is transport-limited. Lastly, accounting for the dynamic relation between microstructure, flow velocity and growth rate is shown to be crucial towards understanding and predicting precipitation in porous rocks.« less

Initial characterization of mudstone nanoporosity with small angle neutron scattering using caprocks from carbon sequestration sites.

DOE Office of Scientific and Technical Information (OSTI.GOV)

McCray, John; Navarre-Sitchler, Alexis; Mouzakis, Katherine

Geological carbon sequestration relies on the principle that CO{sub 2} injected deep into the subsurface is unable to leak to the atmosphere. Structural trapping by a relatively impermeable caprock (often mudstone such as a shale) is the main trapping mechanism that is currently relied on for the first hundreds of years. Many of the pores of the caprock are of micrometer to nanometer scale. However, the distribution, geometry and volume of porosity at these scales are poorly characterized. Differences in pore shape and size can cause variation in capillary properties and fluid transport resulting in fluid pathways with different capillarymore » entry pressures in the same sample. Prediction of pore network properties for distinct geologic environments would result in significant advancement in our ability to model subsurface fluid flow. Specifically, prediction of fluid flow through caprocks of geologic CO{sub 2} sequestration reservoirs is a critical step in evaluating the risk of leakage to overlying aquifers. The micro- and nanoporosity was analyzed in four mudstones using small angle neutron scattering (SANS). These mudstones are caprocks of formations that are currently under study or being used for carbon sequestration projects and include the Marine Tuscaloosa Group, the Lower Tuscaloosa Group, the upper and lower shale members of the Kirtland Formation, and the Pennsylvanian Gothic shale. Total organic carbon varies from <0.3% to 4% by weight. Expandable clay contents range from 10% to {approx}40% in the Gothic shale and Kirtland Formation, respectively. Neutrons effectively scatter from interfaces between materials with differing scattering length density (i.e. minerals and pores). The intensity of scattered neutrons, I(Q), where Q is the scattering vector, gives information about the volume of pores and their arrangement in the sample. The slope of the scattering data when plotted as log I(Q) vs. log Q provides information about the fractality or geometry of the pore network. Results from this study, combined with high-resolution TEM imaging, provide insight into the differences in volume and geometry of porosity between these various mudstones.« less

Activated Neutrophils Are Associated with Pediatric Cerebral Malaria Vasculopathy in Malawian Children

PubMed Central

Feintuch, Catherine Manix; Saidi, Alex; Seydel, Karl; Chen, Grace; Goldman-Yassen, Adam; Mita-Mendoza, Neida K.; Kim, Ryung S.; Frenette, Paul S.; Taylor, Terrie

2016-01-01

ABSTRACT Most patients with cerebral malaria (CM) sustain cerebral microvascular sequestration of Plasmodium falciparum-infected red blood cells (iRBCs). Although many young children are infected with P. falciparum, CM remains a rare outcome; thus, we hypothesized that specific host conditions facilitate iRBC cerebral sequestration. To identify these host factors, we compared the peripheral whole-blood transcriptomes of Malawian children with iRBC cerebral sequestration, identified as malarial-retinopathy-positive CM (Ret+CM), to the transcriptomes of children with CM and no cerebral iRBC sequestration, defined as malarial-retinopathy-negative CM (Ret-CM). Ret+CM was associated with upregulation of 103 gene set pathways, including cytokine, blood coagulation, and extracellular matrix (ECM) pathways (P < 0.01; false-discovery rate [FDR] of <0.05). Neutrophil transcripts were the most highly upregulated individual transcripts in Ret+CM patients. Activated neutrophils can modulate diverse host processes, including the ECM, inflammation, and platelet biology to potentially facilitate parasite sequestration. Therefore, we compared plasma neutrophil proteins and neutrophil chemotaxis between Ret+CM and Ret-CM patients. Plasma levels of human neutrophil elastase, myeloperoxidase, and proteinase 3, but not lactoferrin or lipocalin, were elevated in Ret+CM patients, and neutrophil chemotaxis was impaired, possibly related to increased plasma heme. Neutrophils were rarely seen in CM brain microvasculature autopsy samples, and no neutrophil extracellular traps were found, suggesting that a putative neutrophil effect on endothelial cell biology results from neutrophil soluble factors rather than direct neutrophil cellular tissue effects. Meanwhile, children with Ret-CM had lower levels of inflammation, higher levels of alpha interferon, and upregulation of Toll-like receptor pathways and other host transcriptional pathways, which may represent responses that do not favor cerebral iRBC sequestration. PMID:26884431

Research and Development of a DNDC Online Model for Farmland Carbon Sequestration and GHG Emissions Mitigation in China.

PubMed

Jiang, Zaidi; Yin, Shan; Zhang, Xianxian; Li, Changsheng; Shen, Guangrong; Zhou, Pei; Liu, Chunjiang

2017-12-01

Appropriate agricultural practices for carbon sequestration and emission mitigation have a significant influence on global climate change. However, various agricultural practices on farmland carbon sequestration usually have a major impact on greenhouse gas (GHG) emissions. It is very important to accurately quantify the effect of agricultural practices. This study developed a platform-the Denitrification Decomposition (DNDC) online model-for simulating and evaluating the agricultural carbon sequestration and emission mitigation based on the scientific process of the DNDC model, which is widely used in the simulation of soil carbon and nitrogen dynamics. After testing the adaptability of the platform on two sampling fields, it turned out that the simulated values matched the measured values well for crop yields and GHG emissions. We used the platform to estimate the effect of three carbon sequestration practices in a sampling field: nitrogen fertilization reduction, straw residue and midseason drainage. The results indicated the following: (1) moderate decrement of the nitrogen fertilization in the sampling field was able to decrease the N₂O emission while maintaining the paddy rice yield; (2) ground straw residue had almost no influence on paddy rice yield, but the CH₄ emission and the surface SOC concentration increased along with the quantity of the straw residue; (3) compared to continuous flooding, midseason drainage would not decrease the paddy rice yield and could lead to a drop in CH₄ emission. Thus, this study established the DNDC online model, which is able to serve as a reference and support for the study and evaluation of the effects of agricultural practices on agricultural carbon sequestration and GHG emissions mitigation in China.

Net carbon flux in organic and conventional olive production systems

NASA Astrophysics Data System (ADS)

Saeid Mohamad, Ramez; Verrastro, Vincenzo; Bitar, Lina Al; Roma, Rocco; Moretti, Michele; Chami, Ziad Al

2014-05-01

Agricultural systems are considered as one of the most relevant sources of atmospheric carbon. However, agriculture has the potentiality to mitigate carbon dioxide mainly through soil carbon sequestration. Some agricultural practices, particularly fertilization and soil management, can play a dual role in the agricultural systems regarding the carbon cycle contributing to the emissions and to the sequestration process in the soil. Good soil and input managements affect positively Soil Organic Carbon (SOC) changes and consequently the carbon cycle. The present study aimed at comparing the carbon footprint of organic and conventional olive systems and to link it to the efficiency of both systems on carbon sequestration by calculating the net carbon flux. Data were collected at farm level through a specific and detailed questionnaire based on one hectare as a functional unit and a system boundary limited to olive production. Using LCA databases particularly ecoinvent one, IPCC GWP 100a impact assessment method was used to calculate carbon emissions from agricultural practices of both systems. Soil organic carbon has been measured, at 0-30 cm depth, based on soil analyses done at the IAMB laboratory and based on reference value of SOC, the annual change of SOC has been calculated. Substracting sequestrated carbon in the soil from the emitted on resulted in net carbon flux calculation. Results showed higher environmental impact of the organic system on Global Warming Potential (1.07 t CO2 eq. yr-1) comparing to 0.76 t CO2 eq. yr-1 in the conventional system due to the higher GHG emissions caused by manure fertilizers compared to the use of synthetic foliar fertilizers in the conventional system. However, manure was the main reason behind the higher SOC content and sequestration in the organic system. As a resultant, the organic system showed higher net carbon flux (-1.7 t C ha-1 yr-1 than -0.52 t C ha-1 yr-1 in the conventional system reflecting higher efficiency as a sink for atmospheric CO2 (the negative value of Net C flux indicates that a system is a net sink for atmospheric CO2). In conclusion, this study illustrates the importance of including soil carbon sequestration associated with CO2 emissions in the evaluation process between alternatives of agricultural systems. Thus, organic olive system offers an opportunity to increase carbon sequestration compared to the conventional one although it causes higher C emissions from manure fertilization. Keywords: Net carbon flux, GHG, organic, olive, soil organic carbon

Quantification and characterization of colloids and organic carbon released under oscillating redox conditions

NASA Astrophysics Data System (ADS)

Jin, Yan; Afsar, Mohammad; Yan, Jing

2017-04-01

Wetlands account for 8-10% of the world's land surface but their soils contain 20-30% of globe terrestrial carbon. The carbon is intimately mixed with minerals in the soils. Thus, mineral-associated-organic carbon (MOC), which often exists as colloids, can directly affect global carbon cycling at multiple scales. When wetland soils become reduced, large quantities of MOC are released due to dissolution of metal oxides, and mobilized and discharged into adjacent streams during rainfall events. Despite the clear relevance of wetlands to global carbon reservoirs and cycling, MOC, as an important component of wetland carbon pool, is poorly understood. Further, understanding of the key factors controlling the fluxes and compositional characteristics of MOC thus the underlying reaction mechanisms that are responsible for the sequestration and stabilization of OC is also lacking. Here we present results from both field sampling and laboratory experiments on the amount, size distribution, and composition of MOC as influenced by oscillating redox conditions. Using both conventional and advanced analytical techniques, including x-ray photoelectron spectroscopy (XPS) and isotope ratio mass spectroscopy (IRMS), we identify 4 MOC size fractions: 450-1000 nm, 100-450 nm, 2.3-100 nm and < 2.3 nm. Normalized atomic% of different elements obtained from XPS analysis reveal clear variations in mineral and OC compositions in the different size fractions. In particular, the "nano sized" MOC (i.e., 2.3-100 nm fraction) has the highest Mg/Al ratio and OC/mineral ratio, the lowest percentages of Al and Si, is mostly depleted in C-C/C-H functional groups but enriched with C=0 and C-O/C-N groups in contract to other size groups. IRMS analysis shows depletion of the heavier isotope 13C from the 2.3-100 nm fraction indicating the presence of more lignin derivatives in this size fraction. The observed size-dependent heterogeneity on C attachment and release to/from MOC can lead to more accurate assessment of OC stability in redox dynamic environments such as wetlands. We propose that size-dependent MOC behavior and associated processes must be considered in future studies of OC in natural systems.

Soil organic carbon sequestration potential and gap of the sub-tropical region

NASA Astrophysics Data System (ADS)

Chiti, T.; Santini, M.; Valentini, R.

2012-04-01

A database of soil organic carbon (SOC) stocks was created for the sub-tropical belt using existing global SOC databases (WISE3; various SOTER) and new data from an ongoing project (ERC Africa-GHG) specific for the tropical forests of the African continent. The intent of this database is to evaluate the sequestration potential of a critical area of the world where most of the primary rainforests are located, and actually show undoubtedly high SOC losses associated with deforestation. About 4100 profiles, quite well distributed over the entire sub-tropical belt, were used to calculate the actual SOC stock for the 0-30 cm and 30-100 cm depths of mineral soil. First, this actual SOC stock has been related to the current Land Use Systems; successively, it has been interpolated taking into account Homogeneous Land Units (HLUs) in terms of soil type, climate zone and land use. Then, relying on consistent projections, of both climate and land use changes, for the years 2050 and 2100 under extremes IPCC-SRES emission scenarios such as the B1 and the A2, potential SOC stocks for these time frames has been calculated. Soil carbon sequestration gap is calculated by the difference of the actual SOC stock and the future projections. When subtracting potential from the actual SOC stocks, negative values represent a gap in terms of possible SOC losses and so reduced carbon sequestration. The soil carbon gap indicates locations where there will be low soil-carbon levels associated with medium-to-high actual SOC stocks, and medium soil-carbon levels associated with high actual SOC stocks, depending on soil type, climate and land use conditions. On the long term, 2076-2100, a SOC gap is observed under all scenarios in South America, just below the Amazonia basin, where are located open and fragmented forests. However, in the Amazonia basin deforestation decrease since no sensible SOC losses were observed. An important gap is observed also in the Congo basin and West Africa, but the gap is more fragmented in small spots than that observed in South America. Forests of Asia seems to be less interested from SOC losses and the projections show almost no gaps under both scenarios. The soil organic carbon sequestration potential database is intended to provide an indication at the regional level of the potential for policy makers to provide environmental services and drive specific policy to increase sustainable land management.

Developing integrated methods to address complex resource and environmental issues

USGS Publications Warehouse

Smith, Kathleen S.; Phillips, Jeffrey D.; McCafferty, Anne E.; Clark, Roger N.

2016-02-08

IntroductionThis circular provides an overview of selected activities that were conducted within the U.S. Geological Survey (USGS) Integrated Methods Development Project, an interdisciplinary project designed to develop new tools and conduct innovative research requiring integration of geologic, geophysical, geochemical, and remote-sensing expertise. The project was supported by the USGS Mineral Resources Program, and its products and acquired capabilities have broad applications to missions throughout the USGS and beyond.In addressing challenges associated with understanding the location, quantity, and quality of mineral resources, and in investigating the potential environmental consequences of resource development, a number of field and laboratory capabilities and interpretative methodologies evolved from the project that have applications to traditional resource studies as well as to studies related to ecosystem health, human health, disaster and hazard assessment, and planetary science. New or improved tools and research findings developed within the project have been applied to other projects and activities. Specifically, geophysical equipment and techniques have been applied to a variety of traditional and nontraditional mineral- and energy-resource studies, military applications, environmental investigations, and applied research activities that involve climate change, mapping techniques, and monitoring capabilities. Diverse applied geochemistry activities provide a process-level understanding of the mobility, chemical speciation, and bioavailability of elements, particularly metals and metalloids, in a variety of environmental settings. Imaging spectroscopy capabilities maintained and developed within the project have been applied to traditional resource studies as well as to studies related to ecosystem health, human health, disaster assessment, and planetary science. Brief descriptions of capabilities and laboratory facilities and summaries of some applications of project products and research findings are included in this circular. The work helped support the USGS mission to “provide reliable scientific information to describe and understand the Earth; minimize loss of life and property from natural disasters; manage water, biological, energy, and mineral resources; and enhance and protect our quality of life.” Activities within the project include the following:Spanned scales from microscopic to planetary;Demonstrated broad applications across disciplines;Included life-cycle studies of mineral resources;Incorporated specialized areas of expertise in applied geochemistry including mineralogy, hydrogeology, analytical chemistry, aqueous geochemistry, biogeochemistry, microbiology, aquatic toxicology, and public health; andIncorporated specialized areas of expertise in geophysics including magnetics, gravity, radiometrics, electromagnetics, seismic, ground-penetrating radar, borehole radar, and imaging spectroscopy.This circular consists of eight sections that contain summaries of various activities under the project. The eight sections are listed below:Laboratory Facilities and Capabilities, which includes brief descriptions of the various types of laboratories and capabilities used for the project;Method and Software Development, which includes summaries of remote-sensing, geophysical, and mineralogical methods developed or enhanced by the project;Instrument Development, which includes descriptions of geophysical instruments developed under the project;Minerals, Energy, and Climate, which includes summaries of research that applies to mineral or energy resources, environmental processes and monitoring, and carbon sequestration by earth materials;Element Cycling, Toxicity, and Health, which includes summaries of several process-oriented geochemical and biogeochemical studies and health-related research activities;Hydrogeology and Water Quality, which includes descriptions of innovative geophysical, remote-sensing, and geochemical research pertaining to hydrogeology and water-quality applications;Hazards and Disaster Assessment, which includes summaries of research and method development that were applied to natural hazards, human-caused hazards, and disaster assessments; andDatabases and Framework Studies, which includes descriptions of fundamental applications of geophysical studies and of the importance of archived data.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Catalano, Jeffrey G.; Giammar, Daniel E.; Wang, Zheming

Phosphate addition is an in situ remediation approach that may enhance the sequestration of uranium without requiring sustained reducing conditions. However, the geochemical factors that determine the dominant immobilization mechanisms upon phosphate addition are insufficiently understood to design efficient remediation strategies or accurately predict U(VI) transport. The overall objective of our project is to determine the dominant mechanisms of U(VI)-phosphate reactions in subsurface environments. Our research approach seeks to determine the U(VI)-phosphate solid that form in the presence of different groundwater cations, characterize the effects of phosphate on U(VI) adsorption and precipitation on smectite and iron oxide minerals, examples ofmore » two major reactive mineral phases in contaminated sediments, and investigate how phosphate affects U(VI) speciation and fate during water flow through sediments from contaminated sites. The research activities conducted for this project have generated a series of major findings. U(VI) phosphate solids from the autunite mineral family are the sole phases to form during precipitation, with uranyl orthophosphate not occurring despite its predicted greater stability. Calcium phosphates may take up substantial quantities of U(VI) through three different removal processes (adsorption, coprecipitation, and precipitation) but the dominance of each process varies with the pathway of reaction. Phosphate co-adsorbs with U(VI) onto smectite mineral surfaces, forming a mixed uranium-phosphate surface complex over a wide range of conditions. However, this molecular-scale association of uranium and phosphate has not effect on the overall extent of uptake. In contrast, phosphate enhanced U(VI) adsorption to iron oxide minerals at acidic pH conditions but suppresses such adsorption at neutral and alkaline pH, despite forming mixed uranium-phosphate surface complexes during adsorption. Nucleation barriers exist that inhibit U(VI) phosphate solids from precipitating in the presence of smectite and iron oxide minerals as well as sediments from contaminated sites. Phosphate addition enhances retention of U(VI) by sediments from the Rifle, CO and Hanford, WA field research sites, areas containing substantial uranium contamination of groundwater. This enhanced retention is through adsorption processes. Both fast and slow uptake and release behavior is observed, indicating that diffusion of uranium between sediment grains has a substantial effect of U(VI) fate in flowing groundwater systems. This project has revealed the complexity of U(VI)-phosphate reactions in subsurface systems. Distinct chemical processes occur in acidic and alkaline groundwater systems. For the latter, calcium phosphate formation, solution complexation, and competition between phosphate and uranium for adsorption sites may serve to either enhance or inhibit U(VI) removal from groundwater. Under the groundwater conditions present at many contaminated sites in the U.S., phosphate appears to general enhance U(VI) retention and limit transport. However, formation of low-solubility uranium phosphate solids does not occur under field-relevant conditions, despite this being the desired product of phosphate-based remediation approaches. In addition, simple equilibrium approaches fail to well-predict uranium fate in contaminated sediments amended with phosphate, with reactive transport models that include reaction rates and mass transport through occluded domains needed to properly describe the system. Phosphate addition faces challenges to being effective as a stand-alone groundwater treatment approach but would prove beneficial as an add-on to other treatment methods that will further limit uranium migration in the subsurface.« less

Reactivity of dissolved- vs. supercritical-CO2 phase toward muscovite basal surfaces

NASA Astrophysics Data System (ADS)

Wan, J.; Tokunaga, T. K.; Kim, Y.; Wang, S.; Altoe, M. V. P.; Ashby, P. D.; DePaolo, D.

2015-12-01

The current understanding of geochemical reactions in reservoirs for geological carbon sequestration (GCS) is largely based on aqueous chemistry (CO2 dissolves in reservoir brine and brine reacts with rocks). However, only a portion of the injected supercritical (sc) CO2 dissolves before the buoyant plume contacts caprock, where it is expected to reside for a long time. Although numerous studies have addressed scCO2-mineral reactions occurring within adsorbed aqueous films, possible reactions resulting from direct CO2-rock contact remain less understood. Does CO2 as a supercritical phase react with reservoir rocks? Do mineral react differently with scCO2 than with dissolved CO2? We selected muscovite, one of the more stable and common rock-forming silicate minerals, to react with scCO2 phase (both water-saturated and water-free) and compared with CO2-saturated-brine. The reacted basal surfaces were analyzed using atomic force microscopy and X-ray photoelectron spectroscopy for examining the changes in surface morphology and chemistry. The results show that scCO2 (regardless of its water content) altered muscovite considerably more than CO2-saturated brine; suggest CO2 diffusion into mica interlayers and localized mica dissolution into scCO2 phase. The mechanisms underlying these observations and their implications for GCS need further exploration.

Magnesium hydroxide extracted from a magnesium-rich mineral for CO2 sequestration in a gas-solid system.

PubMed

Lin, Pao-Chung; Huang, Cheng-Wei; Hsiao, Ching-Ta; Teng, Hsisheng

2008-04-15

Magnesium hydroxide extracted from magnesium-bearing minerals is considered a promising agent for binding CO2 as a carbonate mineral in a gas-solid reaction. An efficient extraction route consisting of hydrothermal treatment on serpentine in HCl followed by NaOH titration for Mg(OH)2 precipitation was demonstrated. The extracted Mg(OH)2 powder had a mean crystal domain size as small as 12 nm and an apparent surface area of 54 m2/g. Under one atmosphere of 10 vol% CO2/N2, carbonation of the serpentine-derived Mg(OH)2 to 26% of the stoichiometric limit was achieved at 325 degrees C in 2 h; while carbonation of a commercially available Mg(OH)2, with a mean crystal domain size of 33 nm and an apparent surface area of 3.5 m2/g, reached only 9% of the stoichiometric limit. The amount of CO2 fixation was found to be inversely proportional to the crystal domain size of the Mg(OH)2 specimens. The experimental data strongly suggested that only a monolayer of carbonates was formed on the crystal domain boundary in the gas-solid reaction, with little penetration of the carbonates into the crystal domain.

Improved grazing management may increase soil carbon sequestration in temperate steppe

NASA Astrophysics Data System (ADS)

Chen, Wenqing; Huang, Ding; Liu, Nan; Zhang, Yingjun; Badgery, Warwick B.; Wang, Xiaoya; Shen, Yue

2015-07-01

Different grazing strategies impact grassland plant production and may also regulate the soil carbon formation. For a site in semiarid temperate steppe, we studied the effect of combinations of rest, high and moderate grazing pressure over three stages of the growing season, on the process involved in soil carbon sequestration. Results show that constant moderate grazing (MMM) exhibited the highest root production and turnover accumulating the most soil carbon. While deferred grazing (RHM and RMH) sequestered less soil carbon compared to MMM, they showed higher standing root mass, maintained a more desirable pasture composition, and had better ability to retain soil N. Constant high grazing pressure (HHH) caused diminished above- and belowground plant production, more soil N losses and an unfavorable microbial environment and had reduced carbon input. Reducing grazing pressure in the last grazing stage (HHM) still had a negative impact on soil carbon. Regression analyses show that adjusting stocking rate to ~5SE/ha with ~40% vegetation utilization rate can get the most carbon accrual. Overall, the soil carbon sequestration in the temperate grassland is affected by the grazing regime that is applied, and grazing can be altered to improve soil carbon sequestration in the temperate steppe.

Improved grazing management may increase soil carbon sequestration in temperate steppe.

PubMed

Chen, Wenqing; Huang, Ding; Liu, Nan; Zhang, Yingjun; Badgery, Warwick B; Wang, Xiaoya; Shen, Yue

2015-07-03

Different grazing strategies impact grassland plant production and may also regulate the soil carbon formation. For a site in semiarid temperate steppe, we studied the effect of combinations of rest, high and moderate grazing pressure over three stages of the growing season, on the process involved in soil carbon sequestration. Results show that constant moderate grazing (MMM) exhibited the highest root production and turnover accumulating the most soil carbon. While deferred grazing (RHM and RMH) sequestered less soil carbon compared to MMM, they showed higher standing root mass, maintained a more desirable pasture composition, and had better ability to retain soil N. Constant high grazing pressure (HHH) caused diminished above- and belowground plant production, more soil N losses and an unfavorable microbial environment and had reduced carbon input. Reducing grazing pressure in the last grazing stage (HHM) still had a negative impact on soil carbon. Regression analyses show that adjusting stocking rate to ~5SE/ha with ~40% vegetation utilization rate can get the most carbon accrual. Overall, the soil carbon sequestration in the temperate grassland is affected by the grazing regime that is applied, and grazing can be altered to improve soil carbon sequestration in the temperate steppe.

Method for sequestering CO.sub.2 and SO.sub.2 utilizing a plurality of waste streams

DOEpatents

Soong, Yee [Monroeville, PA; Allen, Douglas E [Salem, MA; Zhu, Chen [Monroe County, IN

2011-04-12

A neutralization/sequestration process is provided for concomitantly addressing capture and sequestration of both CO.sub.2 and SO.sub.2 from industrial gas byproduct streams. The invented process concomitantly treats and minimizes bauxite residues from aluminum production processes and brine wastewater from oil/gas production processes. The benefits of this integrated approach to coincidental treatment of multiple industrial waste byproduct streams include neutralization of caustic byproduct such as bauxite residue, thereby decreasing the risk associated with the long-term storage and potential environmental of storing caustic materials, decreasing or obviating the need for costly treatment of byproduct brines, thereby eliminating the need to purchase CaO or similar scrubber reagents typically required for SO.sub.2 treatment of such gasses, and directly using CO.sub.2 from flue gas to neutralize bauxite residue/brine mixtures, without the need for costly separation of CO.sub.2 from the industrial byproduct gas stream by processes such as liquid amine-based scrubbers.

Ferritin: the protein nanocage and iron biomineral in health and in disease.

PubMed

Theil, Elizabeth C

2013-11-04

At the center of iron and oxidant metabolism is the ferritin superfamily: protein cages with Fe(2+) ion channels and two catalytic Fe/O redox centers that initiate the formation of caged Fe2O3·H2O. Ferritin nanominerals, initiated within the protein cage, grow inside the cage cavity (5 or 8 nm in diameter). Ferritins contribute to normal iron flow, maintenance of iron concentrates for iron cofactor syntheses, sequestration of iron from invading pathogens, oxidant protection, oxidative stress recovery, and, in diseases where iron accumulates excessively, iron chelation strategies. In eukaryotic ferritins, biomineral order/crystallinity is influenced by nucleation channels between active sites and the mineral growth cavity. Animal ferritin cages contain, uniquely, mixtures of catalytically active (H) and inactive (L) polypeptide subunits with varied rates of Fe(2+)/O2 catalysis and mineral crystallinity. The relatively low mineral order in liver ferritin, for example, coincides with a high percentage of L subunits and, thus, a low percentage of catalytic sites and nucleation channels. Low mineral order facilitates rapid iron turnover and the physiological role of liver ferritin as a general iron source for other tissues. Here, current concepts of ferritin structure/function/genetic regulation are discussed and related to possible therapeutic targets such as mini-ferritin/Dps protein active sites (selective pathogen inhibition in infection), nanocage pores (iron chelation in therapeutic hypertransfusion), mRNA noncoding, IRE riboregulator (normalizing the ferritin iron content after therapeutic hypertransfusion), and protein nanovessels to deliver medicinal or sensor cargo.

Mineral Precipitation in Fractures: Multiscale Imaging and Geochemical Modeling

NASA Astrophysics Data System (ADS)

Hajirezaie, S.; Peters, C. A.; Swift, A.; Sheets, J. M.; Cole, D. R.; Crandall, D.; Cheshire, M.; Stack, A. G.; Anovitz, L. M.

2017-12-01

For subsurface energy technologies such as geologic carbon sequestration, fractures are potential pathways for fluid migration from target formations. Highly permeable fractures may become sealed by mineral precipitation. In this study, we examined shale specimens with existing cemented fractures as natural analogues, using an array of imaging methods to characterize mineralogy and porosity at several spatial scales. In addition, we used reactive transport modeling to investigate geochemical conditions that can lead to extensive mineral precipitation and to simulate the impacts on fracture hydraulic properties. The naturally-cemented fractured rock specimens were from the Upper Wolfcamp formation in Texas, at 10,000 ft depth. The specimens were scanned using x-ray computed tomography (xCT) at resolution of 13 microns. The xCT images revealed an original fracture aperture of 1.9 mm filled with several distinct mineral phases and vuggy void regions, and the mineral phase volumes and surface areas were quantified and mapped in 3D. Specimens were thin-sectioned and examined at micron- and submicron-scales using petrographic microscopy (PM), scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDX), and small angle X-ray scattering (SAXS). Collectively these methods revealed crystals of dolomite as large as 900 microns in length overlain with a heterogeneous mixture of carbonate minerals including calcite, dolomite, and Fe-rich dolomite, interspersed at spatial scales as small as 5 microns. In addition, secondary precipitation of SiO2 was found to fill some of the void space. This multiscale imaging was used to inform the reactive transport modeling employed to examine the conditions that can cause the observed mineral precipitation in fractures at a larger scale. Two brines containing solutions that when mixed would lead to precipitation of various carbonate minerals were simulated as injectants into a fracture domain. In particular, the competing effects of transport dynamics and reaction kinetics were investigated in the context of profiles of the precipitated minerals and permeability behavior of the fracture flow path. This study contributes rich knowledge toward mastering the subsurface for energy production and storage and for the management of energy waste streams.

On Becoming Faculty Librarians: Acculturation Problems and Remedies.

ERIC Educational Resources Information Center

Mitchell, W. Bede; Morton, Bruce

1992-01-01

Discussion of the acculturation of academic librarians to faculty positions focuses on the processes of acculturation, including selection, sequestration, instruction and apprenticeship, sanctioning, certification and sponsorship, and mentoring. Difficulties with this process specific to librarians are considered, and suggestions for improving…

Lake Charles CCS Project

DOE Office of Scientific and Technical Information (OSTI.GOV)

Leib, Thomas; Cole, Dan

In late September 2014 development of the Lake Charles Clean Energy (LCCE) Plant was abandoned resulting in termination of Lake Charles Carbon Capture and Sequestration (CCS) Project which was a subset the LCCE Plant. As a result, the project was only funded through Phase 2A (Design) and did not enter Phase 2B (Construction) or Phase 2C (Operations). This report was prepared relying on information prepared and provided by engineering companies which were engaged by Leucadia Energy, LLC to prepare or review Front End Engineering and Design (FEED) for the Lake Charles Clean Energy Project, which includes the Carbon Capture andmore » Sequestration (CCS) Project in Lake Charles, Louisiana. The Lake Charles Carbon Capture and Sequestration (CCS) Project was to be a large-scale industrial CCS project intended to demonstrate advanced technologies that capture and sequester carbon dioxide (CO 2) emissions from industrial sources into underground formations. The Scope of work was divided into two discrete sections; 1) Capture and Compression prepared by the Recipient Leucadia Energy, LLC, and 2) Transport and Sequestration prepared by sub-Recipient Denbury Onshore, LLC. Capture and Compression-The Lake Charles CCS Project Final Technical Report describes the systems and equipment that would be necessary to capture CO 2 generated in a large industrial gasification process and sequester the CO 2 into underground formations. The purpose of each system is defined along with a description of its equipment and operation. Criteria for selection of major equipment are provided and ancillary utilities necessary for safe and reliable operation in compliance with environmental regulations are described. Construction considerations are described including a general arrangement of the CCS process units within the overall gasification project. A cost estimate is provided, delineated by system area with cost breakdown showing equipment, piping and materials, construction labor, engineering, and other costs. The CCS Project Final Technical Report is based on a Front End Engineering and Design (FEED) study prepared by SK E&C, completed in [June] 2014. Subsequently, Fluor Enterprises completed a FEED validation study in mid-September 2014. The design analyses indicated that the FEED package was sufficient and as expected. However, Fluor considered the construction risk based on a stick-build approach to be unacceptable, but construction risk would be substantially mitigated through utilization of modular construction where site labor and schedule uncertainty is minimized. Fluor’s estimate of the overall EPC project cost utilizing the revised construction plan was comparable to SKE&C’s value after reflecting Fluor’s assessment of project scope and risk characteristic. Development was halted upon conclusion of Phase 2A FEED and the project was not constructed.Transport and Sequestration – The overall objective of the pipeline project was to construct a pipeline to transport captured CO 2 from the Lake Charles Clean Energy project to the existing Denbury Green Line and then to the Hastings Field in Southeast Texas to demonstrate effective geologic sequestration of captured CO 2 through commercial EOR operations. The overall objective of the MVA portion of the project was to demonstrate effective geologic sequestration of captured CO 2 through commercial Enhanced Oil Recovery (EOR) operations in order to evaluate costs, operational processes and technical performance. The DOE target for the project was to capture and implement a research MVA program to demonstrate the sequestration through EOR of approximately one million tons of CO 2 per year as an integral component of commercial operations.« less

Commercial silicate phosphate sequestration and desorption leads to a gradual decline of aquatic systems.

PubMed

Svatos, Karl B W

2018-02-01

Laboratory desorption behaviour, function and elemental composition of commercially marketed silicate minerals used to sequester phosphorus pollution as well as Zeolite, Smectite, and Kaolinite were determined to see whether their use by environmental scientists and water managers in eutrophic waterways has the potential to contribute to longer-term environmental impacts. As expected, lower phosphorus concentrations were observed, following treatment. However, data relating to desorption, environmental fate and bioavailability of phospho-silicate complexes (especially those containing rare earth elements) appear to be underrepresented in product testing and trial publications. Analysis of desorption of phosphate (P) was > 5 μg[P]/L for all three non-commercial samples and 0 > μg[P]/L > 5 for all commercial silicates for a range of concentrations from 0 to 300 μg[P]/L. Based on a review of bioaccumulation data specific to the endangered Cherax tenuimanus (Hairy Marron) and other endemic species, this is significant considering anything > 20 μg[La]/L is potentially lethal to the hairy marron, other crustaceans and even other phyla. Where prokaryotic and eukaryotic effects are underreported, this represents a significant challenge. Especially where product protocols recommend continual reapplication, this is significant because both the forward and reverse reactions are equally important. The users of silicate minerals in water columns should accept the dynamic nature of the process and pay equal attention to both adsorption and desorption because desorption behaviour is an inherent trait. Even if broader desorption experimentation is difficult, expensive and time-consuming, it is a critical consideration nonetheless.

Sorption and desorption of carbamazepine from water by smectite clays.

PubMed

Zhang, Weihao; Ding, Yunjie; Boyd, Stephen A; Teppen, Brian J; Li, Hui

2010-11-01

Carbamazepine is a prescription anticonvulsant and mood stabilizing pharmaceutical administered to humans. Carbamazepine is persistent in the environment and frequently detected in water systems. In this study, sorption and desorption of carbamazepine from water was measured for smectite clays with the surface negative charges compensated with K+, Ca2+, NH4+, tetramethylammonium (TMA), trimethylphenylammonium (TMPA) and hexadecyltrimethylammonium (HDTMA) cations. The magnitude of sorption followed the order: TMPA-smectite≥HDTMA-smectite>NH4-smectite>K-smectite>Ca-smectite⩾TMA-smectite. The greatest sorption of carbamazepine by TMPA-smectite is attributed to the interaction of conjugate aromatic moiety in carbamazepine with the phenyl ring in TMPA through π-π interaction. Partitioning process is the primary mechanism for carbamazepine uptake by HDTMA-smectite. For NH4-smectite the urea moiety in carbamazepine interacts with exchanged cation NH4+ by H-bonding hence demonstrating relatively higher adsorption. Sorption by K-, Ca- and TMA-smectites from water occurs on aluminosilicate mineral surfaces. These results implicate that carbamazepine sorption by soils occurs primarily in soil organic matter, and soil mineral fractions play a secondary role. Desorption of carbamazepine from the sorbents manifested an apparent hysteresis. Increasing irreversibility of desorption vs. sorption was observed for K-, Ca-, TMA-, TMPA- and HDTMA-clays as aqueous carbamazepine concentrations increased. Desorption hysteresis of carbamazepine from K-, Ca-, NH4-smectites was greater than that from TMPA- and HDTMA-clays, suggesting that the sequestrated carbamazepine molecules in smectite interlayers are more resistant to desorption compared to those sorbed by organic phases in smectite clays. Copyright © 2010 Elsevier Ltd. All rights reserved.

Case study on combined CO₂ sequestration and low-salinity water production potential in a shallow saline aquifer in Qatar.

PubMed

Ahmed, Tausif Khizar; Nasrabadi, Hadi

2012-10-30

CO₂ is one of the byproducts of natural gas production in Qatar. The high rate of natural gas production from Qatar's North Field (world's largest non-associated gas field) has led to the production of significant amounts of CO₂. The release of CO₂ into the atmosphere may be harmful from the perspective of global warming. In this work, we study the CO₂ sequestration potential in Qatar's Aruma aquifer. The Aruma aquifer is a saline aquifer in the southwest of Qatar. It occupies an area of approximately 1985 km₂ on land (16% of Qatar's total area). We have developed a compositional model for CO₂ sequestration in the Aruma aquifer on the basis of available log and flow test data. We suggest water production at some distance from the CO₂ injection wells as a possible way to control the pore pressure. This method increases the potential for safe sequestration of CO₂ in the aquifer without losing integrity of the caprock and without any CO₂ leakage. The water produced from this aquifer is considerably less saline than seawater and could be a good water source for the desalination process, which is currently the main source of water in Qatar. The outcome of the desalination process is water with higher salinity than the seawater that is currently discharged into the sea. This discharge can have negative long-term environmental effects. The water produced from the Aruma aquifer is considerably less saline than seawater and can be a partial solution to this problem. Copyright © 2012 Elsevier Ltd. All rights reserved.

CO2 sequestration potential of Charqueadas coal field in Brazil

DOE Office of Scientific and Technical Information (OSTI.GOV)

Romanov, V; Santarosa, C; Crandall, D

2013-02-01

Although coal is not the primary source of energy in Brazil there is growing interest to evaluate the potential of coal from the south of the country for various activities. The I2B coal seamin the Charqueadas coal field has been considered a target for enhanced coal bed methane production and CO2 sequestration. A detailed experimental study of the samples from this seam was conducted at the NETL with assistance from the Pontif?cia Universidade Cat?lica Do Rio Grande Do Sul. Such properties as sorption capacity, internal structure of the samples, porosity and permeability were of primary interest in this characterization study.more » The samples used were low rank coals (high volatile bituminous and sub-bituminous) obtained from the I2B seam. It was observed that the temperature effect on adsorption capacity correlates negatively with as-received water and mineral content. Langmuir CO2 adsorption capacity of the coal samples ranged 0.61?2.09 mmol/g. The upper I2B seam appears to be overall more heterogeneous and less permeable than the lower I2B seam. The lower seam coal appears to have a large amount of micro-fractures that do not close even at 11 MPa of confining pressure.« less

Reactive Transport at the Pore Scale with Applications to the Dissolution of Carbonate Rocks for CO2 Sequestration Operations

NASA Astrophysics Data System (ADS)

Boek, E.; Gray, F.; Welch, N.; Shah, S.; Crawshaw, J.

2014-12-01

In CO2 sequestration operations, CO2 injected into a brine aquifer dissolves in the liquid to create an acidic solution. This may result in dissolution of the mineral grains in the porous medium. Experimentally, it is hard to investigate this process at the pore scale. Therefore we develop a new hybrid particle simulation algorithm to study the dissolution of solid objects in a laminar flow field, as encountered in porous media flow situations. First, we calculate the flow field using a multi-relaxation-time lattice Boltzmann (LB) algorithm implemented on GPUs, which demonstrates a very efficient use of the GPU device and a considerable performance increase over CPU calculations. Second, using a stochastic particle approach, we solve the advection-diffusion equation for a single reactive species and dissolve solid voxels according to our reaction model. To validate our simulation, we first calculate the dissolution of a solid sphere as a function of time under quiescent conditions. We compare with the analytical solution for this problem [1] and find good agreement. Then we consider the dissolution of a solid sphere in a laminar flow field and observe a significant change in the sphericity with time due to the coupled dissolution - flow process. Second, we calculate the dissolution of a cylinder in channel flow in direct comparison with corresponding dissolution experiments. We discuss the evolution of the shape and dissolution rate. Finally, we calculate the dissolution of carbonate rock samples at the pore scale in direct comparison with micro-CT experiments. This work builds on our recent research on calculation of multi-phase flow [2], [3] and hydrodynamic dispersion and molecular propagator distributions for solute transport in homogeneous and heterogeneous porous media using LB simulations [4]. It turns out that the hybrid simulation model is a suitable tool to study reactive flow processes at the pore scale. This is of great importance for CO2 storage and Enhanced Oil Recovery applications. References[1] Rice, R. G. and Do, D.D., Chem. Eng. Sci., 61, 775-778 (2006)[2] Boek, E.S. and Venturoli, M., Comp. and Maths with Appl. 59, 2305-2314 (2010)[3] Yang, J. and Boek, E.S., Comp. and Maths with Appl. 65, 882-890 (2013)[4] Yang, J. Crawshaw, J. and Boek, E.S., Water Resources Research 49, 8531-8538 (2013)

Coral bleaching under thermal stress: putative involvement of host/symbiont recognition mechanisms

PubMed Central

Vidal-Dupiol, Jeremie; Adjeroud, Mehdi; Roger, Emmanuel; Foure, Laurent; Duval, David; Mone, Yves; Ferrier-Pages, Christine; Tambutte, Eric; Tambutte, Sylvie; Zoccola, Didier; Allemand, Denis; Mitta, Guillaume

2009-01-01

Background Coral bleaching can be defined as the loss of symbiotic zooxanthellae and/or their photosynthetic pigments from their cnidarian host. This major disturbance of reef ecosystems is principally induced by increases in water temperature. Since the beginning of the 1980s and the onset of global climate change, this phenomenon has been occurring at increasing rates and scales, and with increasing severity. Several studies have been undertaken in the last few years to better understand the cellular and molecular mechanisms of coral bleaching but the jigsaw puzzle is far from being complete, especially concerning the early events leading to symbiosis breakdown. The aim of the present study was to find molecular actors involved early in the mechanism leading to symbiosis collapse. Results In our experimental procedure, one set of Pocillopora damicornis nubbins was subjected to a gradual increase of water temperature from 28°C to 32°C over 15 days. A second control set kept at constant temperature (28°C). The differentially expressed mRNA between the stressed states (sampled just before the onset of bleaching) and the non stressed states (control) were isolated by Suppression Subtractive Hybridization. Transcription rates of the most interesting genes (considering their putative function) were quantified by Q-RT-PCR, which revealed a significant decrease in transcription of two candidates six days before bleaching. RACE-PCR experiments showed that one of them (PdC-Lectin) contained a C-Type-Lectin domain specific for mannose. Immunolocalisation demonstrated that this host gene mediates molecular interactions between the host and the symbionts suggesting a putative role in zooxanthellae acquisition and/or sequestration. The second gene corresponds to a gene putatively involved in calcification processes (Pdcyst-rich). Its down-regulation could reflect a trade-off mechanism leading to the arrest of the mineralization process under stress. Conclusion Under thermal stress zooxanthellae photosynthesis leads to intense oxidative stress in the two partners. This endogenous stress can lead to the perception of the symbiont as a toxic partner for the host. Consequently, we propose that the bleaching process is due in part to a decrease in zooxanthellae acquisition and/or sequestration. In addition to a new hypothesis in coral bleaching mechanisms, this study provides promising biomarkers for monitoring coral health. PMID:19653882

Coral bleaching under thermal stress: putative involvement of host/symbiont recognition mechanisms.

PubMed

Vidal-Dupiol, Jeremie; Adjeroud, Mehdi; Roger, Emmanuel; Foure, Laurent; Duval, David; Mone, Yves; Ferrier-Pages, Christine; Tambutte, Eric; Tambutte, Sylvie; Zoccola, Didier; Allemand, Denis; Mitta, Guillaume

2009-08-04

Coral bleaching can be defined as the loss of symbiotic zooxanthellae and/or their photosynthetic pigments from their cnidarian host. This major disturbance of reef ecosystems is principally induced by increases in water temperature. Since the beginning of the 1980s and the onset of global climate change, this phenomenon has been occurring at increasing rates and scales, and with increasing severity. Several studies have been undertaken in the last few years to better understand the cellular and molecular mechanisms of coral bleaching but the jigsaw puzzle is far from being complete, especially concerning the early events leading to symbiosis breakdown. The aim of the present study was to find molecular actors involved early in the mechanism leading to symbiosis collapse. In our experimental procedure, one set of Pocillopora damicornis nubbins was subjected to a gradual increase of water temperature from 28 degrees C to 32 degrees C over 15 days. A second control set kept at constant temperature (28 degrees C). The differentially expressed mRNA between the stressed states (sampled just before the onset of bleaching) and the non stressed states (control) were isolated by Suppression Subtractive Hybridization. Transcription rates of the most interesting genes (considering their putative function) were quantified by Q-RT-PCR, which revealed a significant decrease in transcription of two candidates six days before bleaching. RACE-PCR experiments showed that one of them (PdC-Lectin) contained a C-Type-Lectin domain specific for mannose. Immunolocalisation demonstrated that this host gene mediates molecular interactions between the host and the symbionts suggesting a putative role in zooxanthellae acquisition and/or sequestration. The second gene corresponds to a gene putatively involved in calcification processes (Pdcyst-rich). Its down-regulation could reflect a trade-off mechanism leading to the arrest of the mineralization process under stress. Under thermal stress zooxanthellae photosynthesis leads to intense oxidative stress in the two partners. This endogenous stress can lead to the perception of the symbiont as a toxic partner for the host. Consequently, we propose that the bleaching process is due in part to a decrease in zooxanthellae acquisition and/or sequestration. In addition to a new hypothesis in coral bleaching mechanisms, this study provides promising biomarkers for monitoring coral health.

Carbon Dioxide Extraction from the Atmosphere Through Engineered Chemical Sinkage: Enabling Energy and Environmental Security

NASA Astrophysics Data System (ADS)

Dubey, M. K.; Ziock, H.; Rueff, G.; Smith, W. S.; Colman, J.; Elliott, S.; Lackner, K.; Johnston, N. A.

2002-05-01

We present the case for carbon dioxide (CO2) extraction from air using engineered chemical sinks as a means of sustaining fossil energy use by avoiding climate change. Existing carbon sequestration strategies such as CO2 injection into geologic formations or the deep ocean and mineral carbonation, require a pure stream of concentrated CO2 to be viable. Furthermore, current emphasis on reducing the global CO2 emissions is on large centralized power plants. However, more than half of all emissions are from the transportation sector and small, distributed sources such as home heating, etc. Most solutions for dealing with these sources explicitly or implicitly entail completely overhauling the existing infrastructure. To solve these problems, Los Alamos National Laboratory has conceived a novel approach for directly extracting CO2 from the atmosphere. Direct extraction converts the dilute CO2 (370 parts per million) in the atmosphere into a pure CO2 stream ready for permanent sequestration. It provides the following advantages: (1) Preserves our existing energy use and fuel distribution systems, which represent a large investment, (2) Indirectly captures CO2 from the myriad of small, distributed, and mobile sources that otherwise are not accessible to sequestration, (3) Allows atmospheric CO2 levels to be restored to their pre-industrial age value, (4) Provides free transport of CO2 to suitable sequestration sites by using natural atmospheric circulation, and (5) Is relatively compact and therefore inexpensive when compared to renewable concepts. Our concept harnesses atmospheric circulation to transport CO2 to sites where the CO2 is extracted by binding it to an adsorbent. The bound CO2 is then recovered as pure gas by heating together with the solid adsorbent that is recycled. As a proof of concept, we show that an aqueous Ca(OH)2 solution efficiently converts CO2 to a CaCO3 solid that can be heated to obtain pure CO2 and recover the CaO. Even with recycling costs, CO2 extraction from air blown by wind through a 1 m2 aperture could eliminate the greenhouse gas impact of a 100 kW gasoline engine, making it more favorable than renewable sources such as solar, wind, or bio-mass. We report economic and scaling arguments, atmospheric simulations and laboratory experiments on candidate adsorbents that support pursuing air-extraction as an advanced CO2 capture technology. We assess and guide synthetic advances in tailoring zeolites, amines, carbon, and ionic fluids to adsorb CO2 selectively, rapidly, and gently enough to facilitate recovery, that promise to significantly enhance the efficiency of CO2 air extraction. This method could process today's world output of CO2 at costs of about 5 cents/liter of gasoline, a manageable scale for this massive undertaking.

Regenerating temperate forest mesocosms in elevated CO2: belowground growth and nitrogen cycling.

PubMed

Berntson, G M; Bazzaz, F A

1997-12-01

The response of temperate forest ecosystems to elevated atmospheric CO 2 concentrations is important because these ecosystems represent a significant component of the global carbon cycle. Two important but not well understood processes which elevated CO 2 may substantially alter in these systems are regeneration and nitrogen cycling. If elevated CO 2 leads to changes in species composition in regenerating forest communities then the structure and function of these ecosystems may be affected. In most temperate forests, nitrogen appears to be a limiting nutrient. If elevated CO 2 leads to reductions in nitrogen cycling through increased sequestration of nitrogen in plant biomass or reductions in mineralization rates, long-term forest productivity may be constrained. To study these processes, we established mesocosms of regenerating forest communities in controlled environments maintained at either ambient (375 ppm) or elevated (700 ppm) CO 2 concentrations. Mesocosms were constructed from intact monoliths of organic forest soil. We maintained these mesocosms for 2 years without any external inputs of nitrogen and allowed the plants naturally present as seeds and rhizomes to regenerate. We used 15 N pool dilution techniques to quantify nitrogen fluxes within the mesocosms at the end of the 2 years. Elevated atmospheric CO 2 concentration significantly affected a number of plant and soil processes in the experimental regenerating forest mesocosms. These changes included increases in total plant biomass production, plant C/N ratios, ectomycorrhizal colonization of tree fine roots, changes in tree fine root architecture, and decreases in plant NH 4 + uptake rates, gross NH 4 + mineralization rates, and gross NH 4 + consumption rates. In addition, there was a shift in the relative biomass contribution of the two dominant regenerating tree species; the proportion of total biomass contributed by white birch (Betula papyrifera) decreased and the proportion of total biomass contributed by yellow birch (B. alleghaniensis) increased. However, elevated CO 2 had no significant effect on the total amount of nitrogen in plant and soil microbial biomass. In this study we observed a suite of effects due to elevated CO 2 , some of which could lead to increases in potential long term growth responses to elevated CO 2 , other to decreases. The reduced plant NH 4 + uptake rates we observed are consistent with reduced NH 4 + availability due to reduced gross mineralization rates. Reduced NH 4 + mineralization rates are consistent with the increases in C/N ratios we observed for leaf and fine root material. Together, these data suggest the positive increases in plant root architectural parameters and mycorrhizal colonization may not be as important as the potential negative effects of reduced nitrogen availability through decreased decomposition rates in a future atmosphere with elevated CO 2 .

Recovery Act: Innovative CO 2 Sequestration from Flue Gas Using Industrial Sources and Innovative Concept for Beneficial CO 2 Use

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dando, Neal; Gershenzon, Mike; Ghosh, Rajat

2012-07-31

The overall goal of this DOE Phase 2 project was to further develop and conduct pilot-scale and field testing of a biomimetic in-duct scrubbing system for the capture of gaseous CO 2 coupled with sequestration of captured carbon by carbonation of alkaline industrial wastes. The Phase 2 project, reported on here, combined efforts in enzyme development, scrubber optimization, and sequestrant evaluations to perform an economic feasibility study of technology deployment. The optimization of carbonic anhydrase (CA) enzyme reactivity and stability are critical steps in deployment of this technology. A variety of CA enzyme variants were evaluated for reactivity and stabilitymore » in both bench scale and in laboratory pilot scale testing to determine current limits in enzyme performance. Optimization of scrubber design allowed for improved process economics while maintaining desired capture efficiencies. A range of configurations, materials, and operating conditions were examined at the Alcoa Technical Center on a pilot scale scrubber. This work indicated that a cross current flow utilizing a specialized gas-liquid contactor offered the lowest system operating energy. Various industrial waste materials were evaluated as sources of alkalinity for the scrubber feed solution and as sources of calcium for precipitation of carbonate. Solids were mixed with a simulated sodium bicarbonate scrubber blowdown to comparatively examine reactivity. Supernatant solutions and post-test solids were analyzed to quantify and model the sequestration reactions. The best performing solids were found to sequester between 2.3 and 2.9 moles of CO 2 per kg of dry solid in 1-4 hours of reaction time. These best performing solids were cement kiln dust, circulating dry scrubber ash, and spray dryer absorber ash. A techno-economic analysis was performed to evaluate the commercial viability of the proposed carbon capture and sequestration process in full-scale at an aluminum smelter and a refinery location. For both cases the in-duct scrubber technology was compared to traditional amine- based capture. Incorporation of the laboratory results showed that for the application at the aluminum smelter, the in-duct scrubber system is more economical than traditional methods. However, the reverse is true for the refinery case, where the bauxite residue is not effective enough as a sequestrant, combined with challenges related to contaminants in the bauxite residue accumulating in and fouling the scrubber absorbent. Sensitivity analyses showed that the critical variables by which process economics could be improved are enzyme concentration, efficiency, and half-life. At the end of the first part of the Phase 2 project, a gate review (DOE Decision Zero Gate Point) was conducted to decide on the next stages of the project. The original plan was to follow the pre-testing phase with a detailed design for the field testing. Unfavorable process economics, however, resulted in a decision to conclude the project before moving to field testing. It is noted that CO 2 Solutions proposed an initial solution to reduce process costs through more advanced enzyme management, however, DOE program requirements restricting any technology development extending beyond 2014 as commercial deployment timeline did not allow this solution to be undertaken.« less

Effect of species composition on carbon and nitrogen stocks in forest floor and mineral soil in Norway spruce and European beech mixed forests

NASA Astrophysics Data System (ADS)

Andivia, Enrique; Rolo, Víctor; Jonard, Mathieu; Formánek, Pavel; Ponette, Quentin

2015-04-01

Management of existing forests has been identified as the main strategy to enhance carbon sequestration and to mitigate the impact of climate change on forest ecosystems. In this direction, the conversion of Norway spruce monospecific stands into mixed stands by intermingling individuals of European beech is an ongoing trend in adaptive forest management strategies, especially in Central Europe. However, studies assessing the effect of changes in tree species composition on soil organic carbon (SOC) and nitrogen stocks are still scarce and there is a lack of scientific evidence supporting tree species selection as a feasible management option to mitigate the effects of predicted future climatic scenarios. We compared C and N stocks in the forest floor (litter and humus) and the top 10 cm of mineral soil in two monospecific stands of Norway spruce and European beech and in a mixed stand of both species. The effect of tree species composition on the C and N stocks and its spatial distribution was evaluated based on litterfall, root production, elevation and canopy opening, and by using a combination of modelling and geostatistical techniques. C stock was highest in the Norway spruce and the mixed stands, while N stock was highest in the mixed stand and lowest under European beech, with intermediate values in the Norway spruce stand. Each forest type showed differences in forest floor properties, suggesting that species composition is an important factor governing forest floor characteristics, including C and N stocks. The distribution of C and N stocks between forest soil layers was different for each forest type. C and N stocks were highest in the hummus layer under Norway spruce, whereas both stocks were lowest in the European beech stand. On the other hand, the mixed stand showed the highest C and N accumulation in the uppermost mineral soil layer, while the monospecific stands showed similar values. Litterfall was the main contribution to C and N stocks of the humus layer in monospecific stands. Forest floor stocks were also influenced by microelevation and canopy opening in the European beech stand and by microelevation in the Norway spruce stand. Root turnover and Norway spruce litterfall proportion directly increased C stocks in the mineral soil of the mixed stand. Additionally, N stock in the forest floor of the mixed stand was positively correlated with the Norway spruce litterfall proportion. Spatial analyses further confirmed that species composition was the main source of spatial variability of SOC stock in mixed stands. These results suggest that the admixture of individuals of European beech and Norway spruce may lead to a translocation of SOC from the forest floor to the better protected mineral soil layer, which might be beneficial for long term SOC sequestration.

Olivine dissolution in the presence of heterotrophic bacteria (Pseudomonas reactants) extracted from Icelandic groundwater of the CO2 injection pilot site

NASA Astrophysics Data System (ADS)

Shirokova, Liudmila; Pokrovsky, Oleg; Benezeth, Pascale; Gerard, Emmanuelle; Menez, Benedicte; Alfredsson, Helgi

2010-05-01

This work is aimed at experimental modeling of the effect of heterotrophic bacteria on dissolution of important rock-forming mineral, olivine, at the conditions of CO2 storage and sequestration. Heterotrophic aerobic gram-negative bacteria were extracted from deep underground water (HK31, 1700 m deep and, t = 25-30°C) of basaltic aquifer located within the Hellisheidi CO2 injection pilot site (Iceland). Following this sampling, we separated, using culture on nutrient agar plates, four different groups of gram-negative aerobic bacteria. The enzymatic activity of studied species has been evaluated using Biolog Ecoplates and their genetic identification was performed using 18-S RNA analysis. The optimal growth conditions of bacteria on Brain Hearth Broth nutrient have been determined as 5 to 37°C and growth media pH varied from 7.0-8.2. Culturing experiments allowed determining the optimal physico-chemical conditions for bacteria experiments in the presence of basic Ca, Mg-containing silicates. Olivine (Fo92) was chosen as typical mineral of basalt, widely considered in carbon dioxide sequestration mechanisms. Dissolution experiments were performed in constant-pH (7 to 9), bicarbonate-buffered (0.001 to 0.05 M) nutrient-diluted media in batch reactors at 0-30 bars of CO2 in the presence of various biomass of Pseudomonas reactants. The release rate of magnesium, silica and iron was measured as a function of time in the presence of live, actively growing, dead (autoclaved or glutaraldehyde-treated) cells and bacteria exometabolites. Both nutrient media diluted 10 times (to 100 mg DOC/L) and inert electrolyte (NaCl, no DOC) were used. Our preliminary results indicate that the pH and dissolved organic matter are the first-order parameters that control the element release from olivine at far from equilibrium conditions. The SEM investigation of reacted surfaces reveal formation of surface roughness with much stronger mineral alteration in the presence of live bacteria compared to experiments with dead biomass. Overall, this work allows better understanding of microbially-affected silicate dissolution in basaltic aquifers and provides a firm methodological basis for constructing the mixed-flow reactors for studying the interaction of heterotrophic bacteria with rock-forming silicates at the environmental conditions of CO2-storage.

Big Sky Carbon Sequestration Partnership

DOE Office of Scientific and Technical Information (OSTI.GOV)

Susan M. Capalbo

2005-11-01

The Big Sky Carbon Sequestration Partnership, led by Montana State University, is comprised of research institutions, public entities and private sectors organizations, and the Confederated Salish and Kootenai Tribes and the Nez Perce Tribe. Efforts under this Partnership in Phase I fall into four areas: evaluation of sources and carbon sequestration sinks that will be used to determine the location of pilot demonstrations in Phase II; development of GIS-based reporting framework that links with national networks; designing an integrated suite of monitoring, measuring, and verification technologies and assessment frameworks; and initiating a comprehensive education and outreach program. The groundwork ismore » in place to provide an assessment of storage capabilities for CO2 utilizing the resources found in the Partnership region (both geological and terrestrial sinks), that would complement the ongoing DOE research agenda in Carbon Sequestration. The region has a diverse array of geological formations that could provide storage options for carbon in one or more of its three states. Likewise, initial estimates of terrestrial sinks indicate a vast potential for increasing and maintaining soil C on forested, agricultural, and reclaimed lands. Both options include the potential for offsetting economic benefits to industry and society. Steps have been taken to assure that the GIS-based framework is consistent among types of sinks within the Big Sky Partnership area and with the efforts of other DOE regional partnerships. The Partnership recognizes the critical importance of measurement, monitoring, and verification technologies to support not only carbon trading but all policies and programs that DOE and other agencies may want to pursue in support of GHG mitigation. The efforts in developing and implementing MMV technologies for geological sequestration reflect this concern. Research is also underway to identify and validate best management practices for soil C in the Partnership region, and to design a risk/cost effectiveness framework to make comparative assessments of each viable sink, taking into account economic costs, offsetting benefits, scale of sequestration opportunities, spatial and time dimensions, environmental risks, and long-term viability. Scientifically sound MMV is critical for public acceptance of these technologies. Deliverables for the 7th Quarter reporting period include (1) for the geological efforts: Reports on Technology Needs and Action Plan on the Evaluation of Geological Sinks and Pilot Project Deployment (Deliverables 2 and 3), and Report on the Feasibility of Mineralization Trapping in the Snake River Plain Basin (Deliverable 14); (2) for the terrestrial efforts: Report on the Evaluation of Terrestrial Sinks and a Report of the Best Production Practices for Soil C Sequestration (Deliverables 8 and 15). In addition, the 7th Quarter activities for the Partnership included further development of the proposed activities for the deployment and demonstration phase of the carbon sequestration pilots including geological and terrestrial pilots, expansion of the Partnership to encompass regions and institutions that are complimentary to the steps we have identified, building greater collaborations with industry and stakeholders in the region, contributed to outreach efforts that spanned all partnerships, co-authorship on the Carbon Capture and Separation report, and developed a regional basis to address future energy opportunities in the region. The deliverables and activities are discussed in the following sections and appended to this report. The education and outreach efforts have resulted in a comprehensive plan which serves as a guide for implementing the outreach activities under Phase I. The public website has been expanded and integrated with the GIS carbon atlas. We have made presentations to stakeholders and policy makers including two tribal sequestration workshops, and made connections to other federal and state agencies concerned with GHG emissions, climate change, and efficient and environmentally-friendly energy production. In addition, the Partnership has plans for integration of our outreach efforts with students, especially at the tribal colleges and at the universities involved in our Partnership. This includes collaboration with MSU and with the U.S.-Norway Summer School, extended outreach efforts at LANL and INEEL, and with the student section of the ASME. Finally, the Big Sky Partnership was involved in key meetings and symposium in the 7th quarter including the USDOE Wye Institute Conference on Carbon Sequestration and Capture (April, 2005); the DOE/NETL Fourth Annual Conference on Carbon Capture and Sequestration (May 2005); Coal Power Development Conference (Denver, June 2005) and meetings with our Phase II industry partners and Governor's staff.« less

Treatment for unstable pulmonary sequestration injury in patient with severe blunt trauma: A case report.

PubMed

Hiraki, Sakiko; Okada, Yohei; Arai, Yusuke; Ishii, Wataru; Iiduka, Ryoji

2017-08-01

Pulmonary sequestration is a congenital malformation characterized by nonfunctioning tissue not communicating with the tracheobronchial tree. As the blood pressure in the artery feeding the sequestrated lung tissue is higher than that in the normal pulmonary artery, the risk of massive hemorrhage in pulmonary sequestration is high. We herein present the first case of a severe blunt trauma patient with unstable pulmonary sequestration injury. The mechanism of pulmonary sequestration injury is vastly different than that of injury to normal lung. We suggest that proximal feeding artery embolization should be performed before surgical intervention in patients with massive hemorrhage of pulmonary sequestration due to severe chest trauma.

soil organic matter pools and quality are sensitive to global climate change in tropical forests from India

NASA Astrophysics Data System (ADS)

Mani, Shanmugam; Merino, Agustín; García-Oliva, Felipe; Riotte, Jean; Sukumar, Raman

2016-04-01

Soil organic carbon (SOC) storage and quality are some of the most important factors determining ecological process in tropical forests, which are especially sensitive to global climate change (GCC). In India, the GCC scenarios expect increasing of drought period and wildfire, which may affect the SOC, and therefore the capacity of forest for C sequestration. The aim of the study was to evaluate the amount of soil C and its quality in the mineral soil across precipitation gradient with different factors (vegetation, pH, soil texture and bedrock composition) for generate SOC predictions under GCC. Six soil samples were collected (top 10 cm depth) from 19 1-ha permanent plots in the Mudumalai Wildlife Sanctuary of southern India, which are characterised by four types of forest vegetation (i.e. dry thorn, dry deciduous, moist deciduous and semi-evergreen forest) distributed along to rainfall gradient. The driest sites are dominated by sandy soils, while the soil clay proportion increased in the wet sites. Total organic C (Leco CN analyser), and the SOM quality was assessed by Differential Scanning Calorimetry (DSC) and Solid-state 13CCP-MAS NMR analyses. Soil organic C was positively correlated with precipitation (R2 = 0.502, p<0.01) and with soil clay content (R2 =0.15, p<0.05), and negatively with soil sand content (R2=0.308, p<0.001) and with pH (R2=0.529, p<0.01); while the C/N was only found positive correlation with clay (R2= 0.350, p<0.01). The driest sites (dry thorn forest) has the lowest proportion of thermal combustion of recalcitrant organic matter (Q2,375-475 °C) than the other sites (p<0.05) and this SOC fraction correlated positively with rainfall (R2=0.27, p=0.01). The Q2 model with best fit included rainfall, pH, sand, clay, C and C/N (R2=0.52, p=0.01). Principal component analysis explains 77% of total variance. The sites on the fist component are distributed along the rainfall gradient. These results suggest that the 50% of variance was explained by precipitation and therefore vegetation type. Consequently, the drier sites has a lower C pools with a higher proportion of labile SOC fraction. As a consequence, we expect if the rainfall decreased by GCC could increase SOC mineralization, and therefore reducing the capacity of C sequestration within soil profile.

Olivine weathering in soil, and its effects on growth and nutrient uptake in Ryegrass (Lolium perenne L.): a pot experiment.

PubMed

ten Berge, Hein F M; van der Meer, Hugo G; Steenhuizen, Johan W; Goedhart, Paul W; Knops, Pol; Verhagen, Jan

2012-01-01

Mineral carbonation of basic silicate minerals regulates atmospheric CO(2) on geological time scales by locking up carbon. Mining and spreading onto the earth's surface of fast-weathering silicates, such as olivine, has been proposed to speed up this natural CO(2) sequestration ('enhanced weathering'). While agriculture may offer an existing infrastructure, weathering rate and impacts on soil and plant are largely unknown. Our objectives were to assess weathering of olivine in soil, and its effects on plant growth and nutrient uptake. In a pot experiment with perennial ryegrass (Lolium perenne L.), weathering during 32 weeks was inferred from bioavailability of magnesium (Mg) in soil and plant. Olivine doses were equivalent to 1630 (OLIV1), 8150, 40700 and 204000 (OLIV4) kg ha(-1). Alternatively, the soluble Mg salt kieserite was applied for reference. Olivine increased plant growth (+15.6%) and plant K concentration (+16.5%) in OLIV4. At all doses, olivine increased bioavailability of Mg and Ni in soil, as well as uptake of Mg, Si and Ni in plants. Olivine suppressed Ca uptake. Weathering estimated from a Mg balance was equivalent to 240 kg ha(-1) (14.8% of dose, OLIV1) to 2240 kg ha(-1) (1.1%, OLIV4). This corresponds to gross CO(2) sequestration of 290 to 2690 kg ha(-1) (29 10(3) to 269 10(3) kg km(-2).) Alternatively, weathering estimated from similarity with kieserite treatments ranged from 13% to 58% for OLIV1. The Olsen model for olivine carbonation predicted 4.0% to 9.0% weathering for our case, independent of olivine dose. Our % values observed at high doses were smaller than this, suggesting negative feedbacks in soil. Yet, weathering appears fast enough to support the 'enhanced weathering' concept. In agriculture, olivine doses must remain within limits to avoid imbalances in plant nutrition, notably at low Ca availability; and to avoid Ni accumulation in soil and crop.

Stable isotope reactive transport modeling in water-rock interactions during CO2 injection

NASA Astrophysics Data System (ADS)

Hidalgo, Juan J.; Lagneau, Vincent; Agrinier, Pierre

2010-05-01

Stable isotopes can be of great usefulness in the characterization and monitoring of CO2 sequestration sites. Stable isotopes can be used to track the migration of the CO2 plume and identify leakage sources. Moreover, they provide unique information about the chemical reactions that take place on the CO2-water-rock system. However, there is a lack of appropriate tools that help modelers to incorporate stable isotope information into the flow and transport models used in CO2 sequestration problems. In this work, we present a numerical tool for modeling the transport of stable isotopes in groundwater reactive systems. The code is an extension of the groundwater single-phase flow and reactive transport code HYTEC [2]. HYTEC's transport module was modified to include element isotopes as separate species. This way, it is able to track isotope composition of the system by computing the mixing between the background water and the injected solution accounting for the dependency of diffusion on the isotope mass. The chemical module and database have been expanded to included isotopic exchange with minerals and the isotope fractionation associated with chemical reactions and mineral dissolution or precipitation. The performance of the code is illustrated through a series of column synthetic models. The code is also used to model the aqueous phase CO2 injection test carried out at the Lamont-Doherty Earth Observatory site (Palisades, New York, USA) [1]. References [1] N. Assayag, J. Matter, M. Ader, D. Goldberg, and P. Agrinier. Water-rock interactions during a CO2 injection field-test: Implications on host rock dissolution and alteration effects. Chemical Geology, 265(1-2):227-235, July 2009. [2] Jan van der Lee, Laurent De Windt, Vincent Lagneau, and Patrick Goblet. Module-oriented modeling of reactive transport with HYTEC. Computers & Geosciences, 29(3):265-275, April 2003.

Olivine Weathering in Soil, and Its Effects on Growth and Nutrient Uptake in Ryegrass (Lolium perenne L.): A Pot Experiment

PubMed Central

ten Berge, Hein F. M.; van der Meer, Hugo G.; Steenhuizen, Johan W.; Goedhart, Paul W.; Knops, Pol; Verhagen, Jan

2012-01-01

Mineral carbonation of basic silicate minerals regulates atmospheric CO2 on geological time scales by locking up carbon. Mining and spreading onto the earth's surface of fast-weathering silicates, such as olivine, has been proposed to speed up this natural CO2 sequestration (‘enhanced weathering’). While agriculture may offer an existing infrastructure, weathering rate and impacts on soil and plant are largely unknown. Our objectives were to assess weathering of olivine in soil, and its effects on plant growth and nutrient uptake. In a pot experiment with perennial ryegrass (Lolium perenne L.), weathering during 32 weeks was inferred from bioavailability of magnesium (Mg) in soil and plant. Olivine doses were equivalent to 1630 (OLIV1), 8150, 40700 and 204000 (OLIV4) kg ha−1. Alternatively, the soluble Mg salt kieserite was applied for reference. Olivine increased plant growth (+15.6%) and plant K concentration (+16.5%) in OLIV4. At all doses, olivine increased bioavailability of Mg and Ni in soil, as well as uptake of Mg, Si and Ni in plants. Olivine suppressed Ca uptake. Weathering estimated from a Mg balance was equivalent to 240 kg ha−1 (14.8% of dose, OLIV1) to 2240 kg ha−1 (1.1%, OLIV4). This corresponds to gross CO2 sequestration of 290 to 2690 kg ha−1 (29 103 to 269 103 kg km−2.) Alternatively, weathering estimated from similarity with kieserite treatments ranged from 13% to 58% for OLIV1. The Olsen model for olivine carbonation predicted 4.0% to 9.0% weathering for our case, independent of olivine dose. Our % values observed at high doses were smaller than this, suggesting negative feedbacks in soil. Yet, weathering appears fast enough to support the ‘enhanced weathering’ concept. In agriculture, olivine doses must remain within limits to avoid imbalances in plant nutrition, notably at low Ca availability; and to avoid Ni accumulation in soil and crop. PMID:22912685

Different effects of plant-derived dissolved organic matter (DOM) and urea on the priming of soil organic carbon.

PubMed

Qiu, Qingyan; Wu, Lanfang; Ouyang, Zhu; Li, Binbin; Xu, Yanyan

2016-03-01

Soil organic carbon (SOC) mineralization is important for the regulation of the global climate and soil fertility. Decomposition of SOC may be significantly affected by the supply of plant-derived labile carbon (C). To investigate the impact of plant-derived dissolved organic matter (DOM) and urea (N) additions on the decomposition of native SOC as well as to elucidate the underlying mechanisms of priming effects (PEs), a batch of incubation experiments was conducted for 250 days by application of (13)C-labeled plant-derived DOM and urea to soils. The direction of PE induced by the addition of DOM was different from the addition of N, i.e. it switched from negative to positive in DOM-amended soils, whereas in the N-treated soil it switched from positive to negative. Adding DOM alone was favorable for soil C sequestration (59 ± 5 mg C per kg soil), whereas adding N alone or together with DOM accelerated the decomposition of native SOC, causing net C losses (-62 ± 4 and -34 ± 31 mg C per kg soil, respectively). These findings indicate that N addition and its interaction with DOM are not favorable for soil C sequestration. Adding DOM alone increased the level of dissolved organic carbon (DOC), but it did not increase the level of soil mineral N. Changes in the ratio of microbial biomass carbon (MBC) to microbial biomass nitrogen (MBN) and microbial metabolic quotient (qCO2) after the addition of DOM and N suggest that a possible shift in the microbial community composition may occur in the present study. Adding DOM with or without N increased the activities of β-glucosidase and urease. Changes in the direction and magnitude of PE were closely related to changes in soil C and N availability. Soil C and N availability might influence the PE through affecting the microbial biomass and extracellular enzyme activity as well as causing a possible shift in the microbial community composition.

Fungal endophytes and their interactions with plants in phytoremediation: A review.

PubMed

Deng, Zujun; Cao, Lixiang

2017-02-01

Endophytic microorganisms (including bacteria and fungi) are likely to interact closely with their hosts and are more protected from adverse changes in the environment. The microbiota contribute to plant growth, productivity, carbon sequestration, and phytoremediation. Elevated levels of contaminants (i.e. metals) are toxic to most plants, the plant's metabolism and growth were impaired and their potential for metal phytoextraction is highly restricted. Exploiting endophytic microorganisms to reduce metal toxicity to plants have been investigated to improve phytoremediation efficiencies. Fungi play an important role in organic and inorganic transformation, element cycling, rock and mineral transformations, bioweathering, mycogenic mineral formation, fungal-clay interactions, and metal-fungal interactions. Endophytic fungi also showed potentials to enhance phytoremediation. Compared to bacteria, most fungi exhibit a filamentous growth habit, which provides the ability to adopt both explorative or exploitative growth strategies and form linear organs of aggregated hyphae to protect fungal translocation. However, the information regarding the role of endophytic fungi in phytoremediation are incomplete, this review highlights the taxa, physiological properties, and interaction of endophytic fungi with plants in phytoremediation. Copyright © 2016 Elsevier Ltd. All rights reserved.

Impacts of Organic Ligands on Forsterite Reactivity in Supercritical CO2 Fluids

DOE Office of Scientific and Technical Information (OSTI.GOV)

Miller, Quin R.; Kaszuba, John; Schaef, Herbert T.

2015-04-07

Subsurface injection of CO2 for enhanced hydrocarbon recovery, hydraulic fracturing of unconventional reservoirs, and geologic carbon sequestration produces a complex geochemical setting in which CO2-dominated fluids containing dissolved water and organic compounds interact with rocks and minerals. The details of these reactions are relatively unknown and benefit from additional experimentally derived data. In this study, we utilized an in situ X-ray diffraction technique to examine the carbonation reactions of forsterite (Mg2SiO4) during exposure to supercritical CO2 (scCO2) that had been equilibrated with aqueous solutions of acetate, oxalate, malonate, or citrate at 50 °C and 90 bar. The organics affected themore » relative abundances of the crystalline reaction products, nesquehonite (MgCO3·3H2O) and magnesite (MgCO3), likely due to enhanced dehydration of the Mg2+ cations by the organic ligands. These results also indicate that the scCO2 solvated and transported the organic ligands to the forsterite surface. This phenomenon has profound implications for mineral transformations and mass transfer in the upper crust.« less

Treatment of Produced Water from Carbon Sequestration Sites for Water Reuse and Mineral Recovery

DOE Office of Scientific and Technical Information (OSTI.GOV)

Renew, Jay; Jenkins, Kristen; Bhagavatula, Abhijit

Southern Research along with Advanced Resources International, Inc. (ARI), Heartland Technology Partners, LLC (Heartland), New Logic Research, Inc. (New Logic), and Mr. Michael N. DiFilippo, Consultant developed a concept for an on-site strategy and design for management of produced water from CO 2 sequestration sites for maximum water reuse. When CO 2 is injected into deep saline aquifers, it may be necessary to produce water from the reservoir to reduce reservoir pressure. The New Logic Research, vibratory shear enhanced process (VSEP) membrane technology, and Heartland Technology Partners, low momentum-high turbulence (LM-HT) evaporation technology was selected for evaluation for treating thismore » produced water from a 530 MW natural gas combined cycle (NGCC) power plant by utilizing waste heat from the plant to drive the evaporation process. The technology was also evaluated for application to a coal-fired power plant in lieu of the NGCC power plant. The results from the project show that the application of the proposed technology to the 530 MW NGCC power plant scenario could be feasible. The results indicate that formation water TDS has a very large impact on the technical and economic feasibility of the process. One advantage of formations with low TDS water is that the VSEP membrane can be utilized to pre-concentrate the produced water upstream of the LM-HT. The results indicate that a significant portion of the exhaust gas from the NGCC power plant will have to be utilized to provide waste heat for the LM-HT evaporator; however, less will be required with low-TDS formation water. The CAPEX costs for LM-HT for all three formations (97.8USD to 122.7USD MM/year) and VSEP plus LM-HT (106.6USD MM/year) for the Keg River formation is high in cost but lower than all technology compared including crystallization, VSEP plus crystallization, FO plus LM-HT, VCE plus LM-HT, and VCE plus crystallization. The OPEX for the LM-HT for all three formations (6.33USD to 7.97USD MM/year) and VSEP plus LM-HT (13.29USD MM/year) for the Keg River formation is lower than crystallization, VSEP plus crystallization, FO plus LM-HT, and FO plus crystallization. Only VCE plus LM-HT and VCE plus crystallization have a comparable OPEX costs to LM-HT for all three formation and VSEP plus LM-HT for the Keg River formation. The coal-fired power plant comparison showed that it is not feasible to apply the technology to that type of fossil fuel plant. Even utilizing 20% of the flue gas, produced water could only be treated from sequestration of approximately 6% to 9% of the CO 2 produced by the coal-fired power plant. This technology operates better when applied to a NGCC power plant due to the higher temperature of the exhaust gas, approximately 1,149 oF/621 oC versus 650 oF/343 oC for flue gas at a coal fired-power plant. The high heat content of the gas turbine significantly improves system performance compared to cooler coal-fired flue gas. The results indicate that a successful S/S process could potentially be achieved with only the minimal addition of binder (4%-10% of CaO or PC). The addition of a SO 4 2- to the S/S process can enhance Ba 2+ immobilization. However, it is noted that metal or other contaminant stabilization could be more difficult based on the particular contaminant content of the produced water. Stabilization additives may be required on a case by case basis. The capital costs and operational costs for a S/S are difficult to estimate due to few large-scale installations of this process. However, the capital costs appears to be fairly small while the operational costs can be significant due to the cost of pozzolanic agents. A review of available literature on the concentrations of valuable metals in produced water from the upstream oil and gas industry indicates that Li + may be present at concentrations that would make recovery attractive. However, more research is needed on Li + concentrations in produced water from CO 2 sequestrations sites.« less

Capturing poromechanical coupling effects of the reactive fracturing process in porous rock via a DEM-network model

NASA Astrophysics Data System (ADS)

Ulven, Ole Ivar; Sun, WaiChing

2016-04-01

Fluid transport in a porous medium has important implications for understanding natural geological processes. At a sufficiently large scale, a fluid-saturated porous medium can be regarded as a two-phase continuum, with the fluid constituent flowing in the Darcian regime. Nevertheless, a fluid mediated chemical reaction can in some cases change the permeability of the rock locally: Mineral dissolution can cause increased permeability, whereas mineral precipitation can reduce the permeability. This might trigger a complicated hydro-chemo-mechanical coupling effect that causes channeling of fluids or clogging of the system. If the fluid is injected or produced at a sufficiently high rate, the pressure might increase enough to cause the onset and propagation of fractures. Fractures in return create preferential flow paths that enhance permeability, localize fluid flow and chemical reaction, prevent build-up of pore pressure and cause anisotropy of the hydro-mechanical responses of the effective medium. This leads to a complex coupled process of solid deformation, chemical reaction and fluid transport enhanced by the fracture formation. In this work, we develop a new coupled numerical model to study the complexities of feedback among fluid pressure evolution, fracture formation and permeability changes due to a chemical process in a 2D system. We combine a discrete element model (DEM) previously used to study a volume expanding process[1, 2] with a new fluid transport model based on poroelasticity[3] and a fluid-mediated chemical reaction that changes the permeability of the medium. This provides new insights into the hydro-chemo-mechanical process of a transforming porous medium. References [1] Ulven, O. I., Storheim, H., Austrheim, H., and Malthe-Sørenssen, A. "Fracture Initiation During Volume Increasing Reactions in Rocks and Applications for CO2 Sequestration", Earth Planet. Sc. Lett. 389C, 2014a, pp. 132 - 142, doi:10.1016/j.epsl.2013.12.039. [2] Ulven, O. I., Jamtveit, B., and Malthe-Sørenssen, A., "Reaction-driven fracturing of porous rock", J. Geophys. Res. Solid Earth 119, 2014b, doi:10.1002/2014JB011102. [3] Ulven, O. I., and Sun, W.C., "A locally mass-conserving dual-graph lattice model for fluid-driven fracture", in prep.

Biocatalytic CO2 sequestration based on shell regeneration

NASA Astrophysics Data System (ADS)

Lee, S.

2012-04-01

Carbon dioxide, CO2, is one of the green gases, being uniformly distributed over the earth's surface. Recently, a variety of methods exists or has been proposed for pre- or post-emission capture and sequestration of CO2. However, CCS (carbon capture & storage) do not quarntee permanent treatment of CO2 and could ingenerate environment risks. Some organisms convert CO2 into exoskeleton (e.g., mollusks) or energy sources (e.g., plants) during metabolism under atmospheric conditions. One of representative biomaterials in ocean is bivalve shell to be composed of CaCO3. Calcium carbonate is not only abundant material in the world but also thermodynamically stable mineral in the capture of CO2. Bivalve has produced CaCO3 under seawater condition, in other word, near atmospheric conditions (1 atm. and around 20-25 oC). At the inorganic point, the synthesis of CaCO3 is as followed. Ca2+ + CO32- -> CaCO3 The bivalve shell plays an important role to protect bivalve's internal organs from prodetor. What will be happened if the shell is damaged and a hole is made? Bivalve must cover the hole to prevent the oxidation of internal organs as fast as possible. From in vitro crystallization test of a notched shell, rapid CaCO3 production was identified at the damaged area. The biocatalyst related to shell regeneration was purified and named as SPSR (Soluble Protein related to Shell Regeneration) that is obtained from the oyster, Crassostrea gigas. And in vitro CaCO3 crystallization test was used to calculate the crystal growth rate of SPSR on CaCO3 crystallization. The characteristics of SPRR are discussed at the point of CO2 hydration and rapid CaCO3 synthesis. To develop the bioinspired process based on shell regeneration concept, the analysis of protein structure has been studied and the immobilization has been carried out for easy recovery of SPSR.

Dissolution Front Instabilities in Reacting Porous Media

NASA Astrophysics Data System (ADS)

Raoof, Amir; Spiers, Chris; Hassanizadeh, Majid

2013-04-01

The main objective of this research is to gain a better understanding of the relation between regime of reaction and dissolution front instability, leading to formation of channels or wormholes. Potential applications are geological sequestration of CO2 and acid-gas injection during enhanced oil recovery. The microscopic pore space is modeled using a multi-directional pore network, allowing for a distribution of pore coordination number, together with distribution of pore sizes. In order to simulate transport of multi-component chemical species, mass balance equations are solved within each element of the network (i.e., pore body and pore throat). We have considered advective and diffusive transport processes within the pore spaces together with multi-component chemical reactions, including both equilibrium and kinetic reactions. Using dimensionless scaling groups (such as Damköhler number and Péclet-Damköhler number) we characterized the dissolution front behavior, and by averaging over the network domain we calculated the evolution of porosity and permeability as well as flux-averaged concentration breakthrough curves. We obtain constitutive relations linking porosity and permeability, under conditions relevant to geological storage of CO2. Effect of distribution of reactive minerals is also evaluated and regime of reaction is shown to play a key role.

Carbon dioxide intercalation in Na-fluorohectorite clay at near-ambient conditions

NASA Astrophysics Data System (ADS)

Fossum, Jon Otto; Hemmen, Henrik; Rolseth, Erlend G.; Fonseca, Davi; Lindbo Hansen, Elisabeth; Plivelic, Tomas

2012-02-01

A molecular dynamics study by Cygan et al.[1] shows the possibility of intercalation and retention of CO2 in smectite clays at 37 ^oC and 200 bar, which suggests that clay minerals may prove suitable for carbon capture and carbon dioxide sequestration. In this work we show from x-ray diffraction measurements that gaseous CO2 intercalates into the interlayer space of the synthetic smectite clay Na-fluorohectorite. The mean interlayer distance of the clay when CO2 is intercalated is 12.5 å at -20 C and 15 bar. The magnitude of the expansion of the interlayer upon intercalation is indistinguishable from that of the dehydrated-monohydrated intercalation of H2O, but this possibility is ruled out by careful repeating the measurements exposing the clay to nitrogen gas. The dynamics of the CO2 intercalation process displays a higher intercalation rate at increased pressure, and the rate is several orders of magnitude slower than that of water or vapor at ambient pressure and temperature.[4pt] [1] Cygan, R. T.; Romanov, V. N.; Myshakin, E. M. Natural materials for carbon capture; Techincal report SAND2010-7217; Sandia National Laboratories: Albuquerque, New Mexico, November, 2010.

Carbon sequestration pilot program : estimated land available for carbon sequestration in the national highway system

DOT National Transportation Integrated Search

2010-05-01

The Federal Highway Administration (FHWA) established the Carbon Sequestration Pilot Program (CSPP) in 2008 to assess whether a roadside carbon sequestration effort through modified maintenance and management practices is appropriate and feasible for...

Analysis and Comparison of Carbon Capture & Sequestration Policies

NASA Astrophysics Data System (ADS)

Burton, E.; Ezzedine, S. M.; Reed, J.; Beyer, J. H.; Wagoner, J. L.

2010-12-01

Several states and countries have adopted or are in the process of crafting policies to enable geologic carbon sequestration projects. These efforts reflect the recognition that existing statutory and regulatory frameworks leave ambiguities or gaps that elevate project risk for private companies considering carbon sequestration projects, and/or are insufficient to address a government’s mandate to protect the public interest. We have compared the various approaches that United States’ state and federal governments have taken to provide regulatory frameworks to address carbon sequestration. A major purpose of our work is to inform the development of any future legislation in California, should it be deemed necessary to meet the goals of Assembly Bill 1925 (2006) to accelerate the adoption of cost-effective geologic sequestration strategies for the long-term management of industrial carbon dioxide in the state. Our analysis shows a diverse issues are covered by adopted and proposed carbon capture and sequestration (CCS) legislation and that many of the new laws focus on defining regulatory frameworks for underground injection of CO2, ambiguities in property issues, or assigning legal liability. While these approaches may enable the progress of early projects, future legislation requires a longer term and broader view that includes a quantified integration of CCS into a government’s overall climate change mitigation strategy while considering potentially counterproductive impacts on CCS of other climate change mitigation strategies. Furthermore, legislation should be crafted in the context of a vision for CCS as an economically viable and widespread industry. While an important function of new CCS legislation is enabling early projects, it must be kept in mind that applying the same laws or protocols in the future to a widespread CCS industry may result in business disincentives and compromise of the public interest in mitigating GHG emissions. Protection of the public interest requires that monitoring and verification track the long term fate of pipelined CO2 regardless of its end use in order to establish that climate change goals are being met.

How organic carbon derived from multiple sources contributes to carbon sequestration processes in a shallow coastal system?

PubMed Central

Watanabe, Kenta; Kuwae, Tomohiro

2015-01-01

Carbon captured by marine organisms helps sequester atmospheric CO2, especially in shallow coastal ecosystems, where rates of primary production and burial of organic carbon (OC) from multiple sources are high. However, linkages between the dynamics of OC derived from multiple sources and carbon sequestration are poorly understood. We investigated the origin (terrestrial, phytobenthos derived, and phytoplankton derived) of particulate OC (POC) and dissolved OC (DOC) in the water column and sedimentary OC using elemental, isotopic, and optical signatures in Furen Lagoon, Japan. Based on these data analysis, we explored how OC from multiple sources contributes to sequestration via storage in sediments, water column sequestration, and air–sea CO2 exchanges, and analyzed how the contributions vary with salinity in a shallow seagrass meadow as well. The relative contribution of terrestrial POC in the water column decreased with increasing salinity, whereas autochthonous POC increased in the salinity range 10–30. Phytoplankton-derived POC dominated the water column POC (65–95%) within this salinity range; however, it was minor in the sediments (3–29%). In contrast, terrestrial and phytobenthos-derived POC were relatively minor contributors in the water column but were major contributors in the sediments (49–78% and 19–36%, respectively), indicating that terrestrial and phytobenthos-derived POC were selectively stored in the sediments. Autochthonous DOC, part of which can contribute to long-term carbon sequestration in the water column, accounted for >25% of the total water column DOC pool in the salinity range 15–30. Autochthonous OC production decreased the concentration of dissolved inorganic carbon in the water column and thereby contributed to atmospheric CO2 uptake, except in the low-salinity zone. Our results indicate that shallow coastal ecosystems function not only as transition zones between land and ocean but also as carbon sequestration filters. They function at different timescales, depending on the salinity, and OC sources. PMID:25880367

Reduced carbon sequestration potential of biochar in acidic soil.

PubMed

Sheng, Yaqi; Zhan, Yu; Zhu, Lizhong

2016-12-01

Biochar application in soil has been proposed as a promising method for carbon sequestration. While factors affecting its carbon sequestration potential have been widely investigated, the number of studies on the effect of soil pH is limited. To investigate the carbon sequestration potential of biochar across a series of soil pH levels, the total carbon emission, CO 2 release from inorganic carbon, and phospholipid fatty acids (PLFAs) of six soils with various pH levels were compared after the addition of straw biochar produced at different pyrolysis temperatures. The results show that the acidic soils released more CO 2 (1.5-3.5 times higher than the control) after the application of biochar compared with neutral and alkaline soils. The degradation of both native soil organic carbon (SOC) and biochar were accelerated. More inorganic CO 2 release in acidic soil contributed to the increased degradation of biochar. Higher proportion of gram-positive bacteria in acidic soil (25%-36%) was responsible for the enhanced biochar degradation and simultaneously co-metabolism of SOC. In addition, lower substrate limitation for bacteria, indicated by higher C-O stretching after the biochar application in the acidic soil, also caused more CO 2 release. In addition to the soil pH, other factors such as clay contents and experimental duration also affected the phsico-chemical and biotic processes of SOC dynamics. Gram-negative/gram-positive bacteria ratio was found to be negatively related to priming effects, and suggested to serve as an indicator for priming effect. In general, the carbon sequestration potential of rice-straw biochar in soil reduced along with the decrease of soil pH especially in a short-term. Given wide spread of acidic soils in China, carbon sequestration potential of biochar may be overestimated without taking into account the impact of soil pH. Copyright © 2016 Elsevier B.V. All rights reserved.

Biochar Decelerates Soil Organic Nitrogen Cycling but Stimulates Soil Nitrification in a Temperate Arable Field Trial

PubMed Central

Prommer, Judith; Wanek, Wolfgang; Hofhansl, Florian; Trojan, Daniela; Offre, Pierre; Urich, Tim; Schleper, Christa; Sassmann, Stefan; Kitzler, Barbara; Soja, Gerhard; Hood-Nowotny, Rebecca Clare

2014-01-01

Biochar production and subsequent soil incorporation could provide carbon farming solutions to global climate change and escalating food demand. There is evidence that biochar amendment causes fundamental changes in soil nutrient cycles, often resulting in marked increases in crop production, particularly in acidic and in infertile soils with low soil organic matter contents, although comparable outcomes in temperate soils are variable. We offer insight into the mechanisms underlying these findings by focusing attention on the soil nitrogen (N) cycle, specifically on hitherto unmeasured processes of organic N cycling in arable soils. We here investigated the impacts of biochar addition on soil organic and inorganic N pools and on gross transformation rates of both pools in a biochar field trial on arable land (Chernozem) in Traismauer, Lower Austria. We found that biochar increased total soil organic carbon but decreased the extractable organic C pool and soil nitrate. While gross rates of organic N transformation processes were reduced by 50–80%, gross N mineralization of organic N was not affected. In contrast, biochar promoted soil ammonia-oxidizer populations (bacterial and archaeal nitrifiers) and accelerated gross nitrification rates more than two-fold. Our findings indicate a de-coupling of the soil organic and inorganic N cycles, with a build-up of organic N, and deceleration of inorganic N release from this pool. The results therefore suggest that addition of inorganic fertilizer-N in combination with biochar could compensate for the reduction in organic N mineralization, with plants and microbes drawing on fertilizer-N for growth, in turn fuelling the belowground build-up of organic N. We conclude that combined addition of biochar with fertilizer-N may increase soil organic N in turn enhancing soil carbon sequestration and thereby could play a fundamental role in future soil management strategies. PMID:24497947

Nanoscale Stress-Corrosion of Geomaterials in Aqueous Solutions

NASA Astrophysics Data System (ADS)

Criscenti, L. J.; Rimsza, J. M.; Matteo, E. N.; Jones, R. E.

2017-12-01

Predicting subcritical crack propagation in low-permeability geo-materials is an unsolved problem crucial to assessing shale caprocks at CO2 sequestration sites, and controlling fracturing for gas and oil extraction. Experiments indicate that chemical reactions at fluid-material interfaces play a major role in subcritical crack growth by weakening the material and altering crack nucleation and growth rates. However, understanding subsurface fracture has been hindered by a lack of understanding of the mechanisms relating chemical environment to mechanical outcome, and a lack of capability directly linking atomistic insight to macroscale observables. We are using both molecular simulation and experiment to develop an atomistic-level understanding of the chemical-mechanical coupling that controls subcritical crack propagation. We are investigating fracture of isotropic silica glass in different environments (air, distilled water, and Na+-rich solutions) and will extend our research to include clay minerals in shales. Molecular simulations are performed with ReaxFF, a reactive force field that allows for explicit modeling of bond breaking and formation processes during crack propagation. A coarse-graining method produces calculated fracture toughness values from the atomistic data. We are performing double cleavage drilled compression (DCDC) experiments in aqueous environmental chambers and monitoring crack propagation with either a confocal or atomic force microscope. Our results show that silica fracture toughness decreases as the environment changes from air to distilled water to Na+-rich solutions. These results suggest that our newly developed computational and experimental techniques can be used to investigate the impact of fluid composition on crack growth in geo-materials and that we will be able to use these methods to understand coupled chemo-mechanical processes and predict crack propagation in shale minerals. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology and Engineering Solutions of Sandia LLC, a wholly owned subsidiary of Honeywell International Inc. for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-NA0003525.

Assessment of CO2-Induced Geochemical Changes in Soil/Mineral-Water Systems

NASA Astrophysics Data System (ADS)

Jeong, H. Y.; Choi, H. J.

2016-12-01

Although the storage of CO2 in deep geological formations is considered the most promising sequestration path, there is still a risk that it may leak into the atmosphere. To ensure the secure operation of CO2 storage sites, thus, it is necessary to implement CO2 leakage monitoring systems. Furthermore, the leakage may alter geochemical properties of overlying geological units to have adverse environmental consequences. By elucidating geochemical changes due to CO2 leakage, it is possible to develop effective CO2 monitoring techniques and predict the influence of CO2 leakage. A series of batch experiments were conducted to simulate CO2-induced geochemical changes in soil/mineral-water systems. Soil samples, obtained from Eumseong basin in Eumseong-gun, Chungcheongbuk-do, were dried for 6 hours at 60° and then divided into two size fractions: < 106 and 106-212 mm. Minerals including mica/illite, vermiculite, and feldspar were purchased and purified if necessary. Prior to batch experiments, soils and minerals were characterized for surface area, mineralogy, elemental composition, carbon and nitrogen contents, pH buffering capacity, and metal extractability. Batch experiments were initiated by reacting 100% CO2 atmosphere with aqueous suspensions of 120 g soils or 50 g minerals in 3,000 mL of 10 mM CsClO4 at room temperature. In parallel, the batches having the same soil/mineral compositions were run under the ambient air as controls. To prevent microbial activities, all batches were sterilized with 0.03% HCHO. To track geochemical changes, pH and electrical conductivity were monitored. Also, while solutions were regularly sampled and analyzed for trace metals as well as main cations and anions, solid phases were sampled to observe changes in mineralogical compositions. Geochemical changes in both solution and solid phases during the initial 6 month reaction will be presented. Acknowledgement: The "R&D Project on Environmental Management of Geologic CO2 Storage" from the KEITI (Project Number: 2014001810003).

Soil organic carbon sequestration and tillage systems in Mediterranean environments

NASA Astrophysics Data System (ADS)

Francaviglia, Rosa; Di Bene, Claudia; Marchetti, Alessandro; Farina, Roberta

2016-04-01

Soil carbon sequestration is of special interest in Mediterranean areas, where rainfed cropping systems are prevalent, inputs of organic matter to soils are low and mostly rely on crop residues, while losses are high due to climatic and anthropic factors such as intensive and non-conservative farming practices. The adoption of reduced or no tillage systems, characterized by a lower soil disturbance in comparison with conventional tillage, has proved to be positively effective on soil organic carbon (SOC) conservation and other physical and chemical processes, parameters or functions, e.g. erosion, compaction, ion retention and exchange, buffering capacity, water retention and aggregate stability. Moreover, soil biological and biochemical processes are usually improved by the reduction of tillage intensity. The work deals with some results available in the scientific literature, and related to field experiment on arable crops performed in Italy, Greece, Morocco and Spain. Data were organized in a dataset containing the main environmental parameters (altitude, temperature, rainfall), soil tillage system information (conventional, minimum and no-tillage), soil parameters (bulk density, pH, particle size distribution and texture), crop type, rotation, management and length of the experiment in years, initial SOCi and final SOCf stocks. Sampling sites are located between 33° 00' and 43° 32' latitude N, 2-860 m a.s.l., with mean annual temperature and rainfall in the range 10.9-19.6° C and 355-900 mm. SOC data, expressed in t C ha-1, have been evaluated both in terms of Carbon Sequestration Rate, given by [(SOCf-SOCi)/length in years], and as percentage change in comparison with the initial value [(SOCf-SOCi)/SOCi*100]. Data variability due to the different environmental, soil and crop management conditions that influence SOC sequestration and losses will be examined.

Soil Carbon Sequestration and Land-Use Change: Processes and Potential

DOE Data Explorer

Post, W. M. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Kwon, K. C. [Tuskeegee University, Tuskeegee, AL (United States)

2005-01-01

When agricultural land is no longer used for cultivation and allowed to revert to natural vegetation or replanted to perennial vegetation, soil organic carbon can accumulate. This accumulation process essentially reverses some of the effects responsible for soil organic carbon losses from when the land was converted from perennial vegetation. We discuss the essential elements of what is known about soil organic matter dynamics that may result in enhanced soil carbon sequestration with changes in land-use and soil management. We review literature that reports changes in soil organic carbon after changes in land-use that favour carbon accumulation. This data summary provides a guide to approximate rates of SOC sequestration that are possible with management, and indicates the relative importance of some factors that influence the rates of organic carbon sequestration in soil. There is a large variation in the length of time for and the rate at which carbon may accumulate in soil, related to the productivity of the recovering vegetation, physical and biological conditions in the soil, and the past history of soil organic carbon inputs and physical disturbance. Maximum rates of C accumulation during the early aggrading stage of perennial vegetation growth, while substantial, are usually much less than 100g C m–2 y–1. Average rates of accumulation are similar for forest or grassland establishment: 33.8 g C m–2 y–1 and 33.2 g C m–2 y–1, respectively. These observed rates of soil organic C accumulation, when combined with the small amount of land area involved, are insufficient to account for a significant fraction of the missing C in the global carbon cycle as accumulating in the soils of formerly agricultural land.

Orientation Effects in Fault Reactivation in Geological CO2 Sequestration

NASA Astrophysics Data System (ADS)

Castelletto, N.; Ferronato, M.; Gambolati, G.; Janna, C.; Teatini, P.

2012-12-01

Geological CO2 sequestration remains one of the most promising option for reducing the greenhouse gases emission. The accurate simulation of the complex coupled physical processes occurring during the injection and the post-injection stage represents a key issue for investigating the feasibility and the safety of the sequestration. The fluid-dynamical and geochemical aspects related to sequestering CO2 underground have been widely debated in the scientific literature over more than one decade. Recently, the importance of geomechanical processes has been widely recognized. In the present modeling study, we focus on fault reactivation induced by injection, an essential aspect for the evaluation of CO2 sequestration projects that needs to be adequately investigated to avoid the generation of preferential leaking path for CO2 and the related risk of induced seismicity. We use a geomechanical model based on the structural equations of poroelasticity solved by the Finite Element (FE) - Interface Element (IE) approach. Standard FEs are used to represent a continuum, while IEs prove especially suited to assess the relative displacements of adjacent elements such as the opening and slippage of existing faults or the generation of new fractures [1]. The IEs allow for the modeling of fault mechanics using an elasto-plastic constitutive law based on the Mohr-Coulomb failure criterion. We analyze the reactivation of a single fault in a synthetic reservoir by varying the fault orientation and size, hydraulic conductivity of the faulted zone, initial vertical and horizontal stress state and Mohr-Coulomb parameters (i.e., friction angle and cohesion). References: [1] Ferronato, M., G. Gambolati, C. Janna, and P. Teatini (2008), Numerical modeling of regional faults in land subsidence prediction above gas/oil reservoirs, Int. J. Numer. Anal. Methods Geomech., 32, 633-657.

Meta-modeling soil organic carbon sequestration potential and its application at regional scale.

PubMed

Luo, Zhongkui; Wang, Enli; Bryan, Brett A; King, Darran; Zhao, Gang; Pan, Xubin; Bende-Michl, Ulrike

2013-03-01

Upscaling the results from process-based soil-plant models to assess regional soil organic carbon (SOC) change and sequestration potential is a great challenge due to the lack of detailed spatial information, particularly soil properties. Meta-modeling can be used to simplify and summarize process-based models and significantly reduce the demand for input data and thus could be easily applied on regional scales. We used the pre-validated Agricultural Production Systems sIMulator (APSIM) to simulate the impact of climate, soil, and management on SOC at 613 reference sites across Australia's cereal-growing regions under a continuous wheat system. We then developed a simple meta-model to link the APSIM-modeled SOC change to primary drivers, i.e., the amount of recalcitrant SOC, plant available water capacity of soil, soil pH, and solar radiation, temperature, and rainfall in the growing season. Based on high-resolution soil texture data and 8165 climate data points across the study area, we used the meta-model to assess SOC sequestration potential and the uncertainty associated with the variability of soil characteristics. The meta-model explained 74% of the variation of final SOC content as simulated by APSIM. Applying the meta-model to Australia's cereal-growing regions reveals regional patterns in SOC, with higher SOC stock in cool, wet regions. Overall, the potential SOC stock ranged from 21.14 to 152.71 Mg/ha with a mean of 52.18 Mg/ha. Variation of soil properties induced uncertainty ranging from 12% to 117% with higher uncertainty in warm, wet regions. In general, soils in Australia's cereal-growing regions under continuous wheat production were simulated as a sink of atmospheric carbon dioxide with a mean sequestration potential of 8.17 Mg/ha.

Microbial Diversity Analysis of the Bacterial and Archaeal Population in Present Day Stromatolites

NASA Technical Reports Server (NTRS)

Ortega, Maya C.

2011-01-01

Stromatolites are layered sedimentary structures resulting from microbial mat communities that remove carbon dioxide from their environment and biomineralize it as calcium carbonate. Although prevalent in the fossil record, stromatolites are rare in the modem world and are only found in a few locations including Highbome Cay in the Bahamas. The stromatolites found at this shallow marine site are analogs to ancient microbial mat ecosystems abundant in the Precambrian period on ancient Earth. To understand how stromatolites form and develop, it is important to identify what microorganisms are present in these mats, and how these microbes contribute to geological structure. These results will provide insight into the molecular and geochemical processes of microbial communities that prevailed on ancient Earth. Since stromatolites are formed by lithifying microbial mats that are able to mineralize calcium carbonate, understanding the biological mechanisms involved may lead to the development of carbon sequestration technologies that will be applicable in human spaceflight, as well as improve our understanding of global climate and its sustainability. The objective of my project was to analyze the archaeal and bacterial dIversity in stromatolites from Highborn Cay in the Bahamas. The first step in studying the molecular processes that the microorganisms carry out is to ascertain the microbial complexity within the mats, which includes identifying and estimating the numbers of different microbes that comprise these mats.

Project Work Plan: Sequestration of Strontium-90 Subsurface Contamination in the Hanford 100-N Area by Surface Infiltration of an Apatite Solution

DOE Office of Scientific and Technical Information (OSTI.GOV)

Szecsody, Jim E.

2006-04-30

We propose to develop an infiltration strategy that defines the precipitation rate of an apatite-forming solution and Sr-90 sequestration processes under variably saturated (low water content) conditions. We will develop this understanding through small-scale column studies, intermediate-scale two-dimensional (2-D) experiments, and numerical modeling to quantify individual and coupled processes associated with apatite formation and Sr-90 transport during and after infiltration of the Ca-citrate-PO4 solution. Development of capabilities to simulate these coupled biogeochemical processes during both injection and infiltration will be used to determine the most cost-effective means to emplace an in situ apatite barrier with a longevity of 300 yearsmore » to permanently sequester Sr-90 until it decays. Biogeochemical processes that will be investigated are citrate biodegradation and apatite precipitation rates at varying water contents as a function of water content. Coupled processes that will be investigated include the influence of apatite precipitation (which occupies pore space) on the hydraulic and transport properties of the porous media during infiltration.« less

Understanding the Transport of Patagonian Dust and Its Influence on Marine Biological Activity in the South Atlantic Ocean

NASA Technical Reports Server (NTRS)

Johnson, Matthew; Meskhidze, Nicholas; Kiliyanpilakkil, Praju; Gasso, Santiago

2010-01-01

Modeling and remote sensing techniques were applied to examine the horizontal and vertical transport pathways of Patagonian dust and quantify the effect of soluble-iron- laden mineral dust deposition on marine primary productivity in the South Atlantic Ocean (SAO) surface waters. The global chemistry transport model GEOS-Chem, implemented with an iron dissolution scheme, was applied to evaluate the atmospheric transport and deposition of mineral dust and bioavailable iron during two dust outbreaks originating in the source regions of Patagonia. In addition to this "rapidly released" iron, offline calculations were also carried out to estimate the amount of bioavailable iron leached during the residence time of dust in the ocean mixed layer. Model simulations showed that the horizontal and vertical transport pathways of Patagonian dust plumes were largely influenced by the synoptic meteorological patterns of high and low pressure systems. Model-predicted horizontal and vertical transport pathways of Patagonian dust over the SAO were in reasonable agreement with remotely-sensed data. Comparison between remotely-sensed and offline calculated ocean surface chlorophyll-a concentrations indicated that, for the two dust outbreaks examined in this study, the deposition of bioavailable iron in the SAO through atmospheric pathways was insignificant. As the two dust transport episodes examined here represent typical outflows of mineral dust from South American sources, our study suggests that the atmospheric deposition of mineral dust is unlikely to induce large scale marine primary productivity and carbon sequestration in the South Atlantic sector of the Southern Ocean.

Formation of crystalline Zn-Al layered double hydroxide precipitates on γ-alumina: the role of mineral dissolution.

PubMed

Li, Wei; Livi, Kenneth J T; Xu, Wenqian; Siebecker, Matthew G; Wang, Yujun; Phillips, Brian L; Sparks, Donald L

2012-11-06

To better understand the sequestration of toxic metals such as nickel (Ni), zinc (Zn), and cobalt (Co) as layered double hydroxide (LDH) phases in soils, we systematically examined the presence of Al and the role of mineral dissolution during Zn sorption/precipitation on γ-Al(2)O(3) (γ-alumina) at pH 7.5 using extended X-ray absorption fine structure spectroscopy (EXAFS), high-resolution transmission electron microscopy (HR-TEM), synchrotron-radiation powder X-ray diffraction (SR-XRD), and (27)Al solid-state NMR. The EXAFS analysis indicates the formation of Zn-Al LDH precipitates at Zn concentration ≥0.4 mM, and both HR-TEM and SR-XRD reveal that these precipitates are crystalline. These precipitates yield a small shoulder at δ(Al-27) = +12.5 ppm in the (27)Al solid-state NMR spectra, consistent with the mixed octahedral Al/Zn chemical environment in typical Zn-Al LDHs. The NMR analysis provides direct evidence for the existence of Al in the precipitates and the migration from the dissolution of γ-alumina substrate. To further address this issue, we compared the Zn sorption mechanism on a series of Al (hydr)oxides with similar chemical composition but differing dissolubility using EXAFS and TEM. These results suggest that, under the same experimental conditions, Zn-Al LDH precipitates formed on γ-alumina and corundum but not on less soluble minerals such as bayerite, boehmite, and gibbsite, which point outs that substrate mineral surface dissolution plays an important role in the formation of Zn-Al LDH precipitates.

Ammonoxidised lignins as slow nitrogen-releasing soil amendments and CO₂-binding matrix.

PubMed

Liebner, Falk; Pour, Georg; de la Rosa Arranz, José Maria; Hilscher, André; Rosenau, Thomas; Knicker, Heike

2011-09-05

Nitrogen (N) is a major nutrient element controlling the cycling of organic matter in the biosphere. Its availability in soils is closely related to biological productivity. In order to reduce the negative environmental impact, associated with the application of mineral N-fertilizers, the use of ammonoxidised technical lignins is suggested. They can act as potential slow N-release fertilisers which concomitantly may increase C sequestration of soils by its potential to bind CO₂. The idea of our study was to combine an improved chemical characterisation of ammonoxidised ligneous matter as well as their CO₂-binding potential, with laboratory pot experiments, performed to enable an evaluation of their behaviour and stability during the biochemical reworking occurring in active soils.

Large-scale sequestration of atmospheric carbon via plant roots in natural and agricultural ecosystems: why and how.

PubMed

Kell, Douglas B

2012-06-05

The soil holds twice as much carbon as does the atmosphere, and most soil carbon is derived from recent photosynthesis that takes carbon into root structures and further into below-ground storage via exudates therefrom. Nonetheless, many natural and most agricultural crops have roots that extend only to about 1 m below ground. What determines the lifetime of below-ground C in various forms is not well understood, and understanding these processes is therefore key to optimising them for enhanced C sequestration. Most soils (and especially subsoils) are very far from being saturated with organic carbon, and calculations show that the amounts of C that might further be sequestered (http://dbkgroup.org/carbonsequestration/rootsystem.html) are actually very great. Breeding crops with desirable below-ground C sequestration traits, and exploiting attendant agronomic practices optimised for individual species in their relevant environments, are therefore important goals. These bring additional benefits related to improvements in soil structure and in the usage of other nutrients and water.

Built-up resilience to climate change in peatlands

NASA Astrophysics Data System (ADS)

Wang, H.; Tian, J.; Ho, M.; Flanagan, N. E.; Vilgalys, R.; Richardson, C. J.

2017-12-01

Peatlands have stored about 30% of global soil carbon over millennia. Most studies suggest that climate change effects, like drought and warming, may decrease C sequestration and increase C loss in peatlands, thus resulting in a positive feedback on climate change. However, the long-term feedback between plant-microbe mediated carbon processes and climate change still remains highly uncertain. Here, we conducted a series of field and lab experiments in southern shrub and northern Sphagnum peatlands to document how previously unrecognized mechanisms regulate the buildup of anti-microbial phenolics, which protects stored carbon directly by reducing phenol oxidase activity during short-term drought, and indirectly through a shift from low-phenolics Sphagnum/herbs to high-phenolics shrubs after long-term moderate drought. We further showed a symbiosis of slow-growing decomposers concomitant with a shift of high-phenolic plants, which increased peat resistance to disturbance. Our results indicate that shrub expansion induced by climate change in boreal peatlands may be a long-term self-adaptive mechanism not only increasing carbon sequestration, but also potentially protecting soil carbon. Therefore, peatlands are highly resilient ecosystems in which the symbiotic adaption of both plants and microbes, triggered by persistent climate change, likely can acclimate to the stressors and maintain their carbon sequestration function and processes.

FULL SCALE BIOREACTOR LANDFILL FOR CARBON SEQUESTRATION AND GREENHOUSE EMISSION CONTROL

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ramin Yazdani; Jeff Kieffer; Heather Akau

2003-08-01

The Yolo County Department of Planning and Public Works is constructing a full-scale bioreactor landfill as a part of the Environmental Protection Agency's (EPA) Project XL program to develop innovative approaches for carbon sequestration and greenhouse emission control. The overall objective is to manage landfill solid waste for rapid waste decomposition and maximum landfill gas generation and capture for carbon sequestration and greenhouse emission control. Waste decomposition is accelerated by improving conditions for either the aerobic or anaerobic biological processes and involves circulating controlled quantities of liquid (leachate, groundwater, gray water, etc.), and, in the aerobic process, large volumes ofmore » air. The first phase of the project entails the construction of a 12-acre module that contains a 6-acre anaerobic cell, a 3.5-acre anaerobic cell, and a 2.5-acre aerobic cell at the Yolo County Central Landfill near Davis, California. The cells are highly instrumented to monitor bioreactor performance. Liquid addition has commenced in the 3.5-acre anaerobic cell and the 6-acre anaerobic cell. Construction of the 2.5-acre aerobic cell is nearly complete with only the biofilter remaining and is scheduled to be complete by the end of August 2003. The current project status and preliminary monitoring results are summarized in this report.« less

Structural and biophysical characterization of the α-carbonic anhydrase from the gammaproteobacterium Thiomicrospira crunogena XCL-2: insights into engineering thermostable enzymes for CO2 sequestration.

PubMed

Díaz-Torres, Natalia A; Mahon, Brian P; Boone, Christopher D; Pinard, Melissa A; Tu, Chingkuang; Ng, Robert; Agbandje-McKenna, Mavis; Silverman, David; Scott, Kathleen; McKenna, Robert

2015-08-01

Biocatalytic CO2 sequestration to reduce greenhouse-gas emissions from industrial processes is an active area of research. Carbonic anhydrases (CAs) are attractive enzymes for this process. However, the most active CAs display limited thermal and pH stability, making them less than ideal. As a result, there is an ongoing effort to engineer and/or find a thermostable CA to fulfill these needs. Here, the kinetic and thermal characterization is presented of an α-CA recently discovered in the mesophilic hydrothermal vent-isolate extremophile Thiomicrospira crunogena XCL-2 (TcruCA), which has a significantly higher thermostability compared with human CA II (melting temperature of 71.9°C versus 59.5°C, respectively) but with a tenfold decrease in the catalytic efficiency. The X-ray crystallographic structure of the dimeric TcruCA shows that it has a highly conserved yet compact structure compared with other α-CAs. In addition, TcruCA contains an intramolecular disulfide bond that stabilizes the enzyme. These features are thought to contribute significantly to the thermostability and pH stability of the enzyme and may be exploited to engineer α-CAs for applications in industrial CO2 sequestration.

Matching roots to their environment

PubMed Central

White, Philip J.; George, Timothy S.; Gregory, Peter J.; Bengough, A. Glyn; Hallett, Paul D.; McKenzie, Blair M.

2013-01-01

Background Plants form the base of the terrestrial food chain and provide medicines, fuel, fibre and industrial materials to humans. Vascular land plants rely on their roots to acquire the water and mineral elements necessary for their survival in nature or their yield and nutritional quality in agriculture. Major biogeochemical fluxes of all elements occur through plant roots, and the roots of agricultural crops have a significant role to play in soil sustainability, carbon sequestration, reducing emissions of greenhouse gasses, and in preventing the eutrophication of water bodies associated with the application of mineral fertilizers. Scope This article provides the context for a Special Issue of Annals of Botany on ‘Matching Roots to Their Environment’. It first examines how land plants and their roots evolved, describes how the ecology of roots and their rhizospheres contributes to the acquisition of soil resources, and discusses the influence of plant roots on biogeochemical cycles. It then describes the role of roots in overcoming the constraints to crop production imposed by hostile or infertile soils, illustrates root phenotypes that improve the acquisition of mineral elements and water, and discusses high-throughput methods to screen for these traits in the laboratory, glasshouse and field. Finally, it considers whether knowledge of adaptations improving the acquisition of resources in natural environments can be used to develop root systems for sustainable agriculture in the future. PMID:23821619

Contaminant desorption during long-term leaching of hydroxide-weathered Hanford sediments.

PubMed

Thompson, Aaron; Steefel, Carl I; Perdrial, Nicolas; Chorover, Ion

2010-03-15

Mineral sorption/coprecipitation is thought to be a principal sequestration mechanism for radioactive (90)Sr and (137)Cs in sediments impacted by hyperalkaline, high-level radioactive waste (HLRW) at the DOE's Hanford site. However, the long-term persistence of neo-formed, contaminant bearing phases after removal of the HLRW source is unknown. We subjected pristine Hanford sediments to hyperalkaline Na-AI-NO(3)-OH solutions containing Sr, Cs, and I at 10(-5), 10(-5), and 10(-7) molal, respectively, for 182 days with either <10 ppmv or 385 ppmv pCO(2). This resulted in the formation of feldspathoid minerals. We leached these weathered sediments with dilute, neutral-pH solutions. After 500 pore volumes (PVs), effluent Sr, Cs, NO(3), Al, Si, and pH reached a steady-state with concentrations elevated above those of feedwater. Reactive transport modeling suggests that even after 500 PV, Cs desorption can be explained by ion exchange reactions, whereas Sr desorption is best described by dissolution of Sr-substituted, neo-formed minerals. While, pCO(2) had no effect on Sr or Cs sorption, sediments weathered at <10 ppmv pCO(2) did desorb more Sr (66% vs 28%) and Cs (13% vs 8%) during leaching than those weathered at 385 ppmv pCO(2). Thus, the dissolution of neo-formed aluminosilicates may represent a long-term, low-level supply of (90)Sr at the Hanford site.

Wellbore Cement Porosity Evolution in Response to Mineral Alteration during CO 2 Flooding

DOE PAGES

Cheshire, Michael C.; Stack, Andrew G.; Carey, J. William; ...

2016-12-13

Mineral reactions during CO 2 sequestration will change the pore-size distribution and pore surface characteristics, complicating permeability and storage security predictions. In this study, we report a small/wide angle scattering study of wellbore cement that has been exposed to carbon dioxide for three decades. We have constructed detailed contour maps that describe local porosity distributions and the mineralogy of the sample and relate these quantities to the carbon dioxide reaction front on the cement. We find that the initial bimodal distribution of pores in the cement, 1–2 and 10–20 nm, is affected differently during the course of carbonation reactions. Initialmore » dissolution of cement phases occurs in the 10–20 nm pores and leads to the development of new pore spaces that are eventually sealed by CaCO 3 precipitation, leading to a loss of gel and capillary nanopores, smoother pore surfaces, and reduced porosity. This suggests that during extensive carbonation of wellbore cement, the cement becomes less permeable because of carbonate mineral precipitation within the pore space. Additionally, the loss of gel and capillary nanoporosities will reduce the reactivity of cement with CO 2 due to reactive surface area loss. Finally, this work demonstrates the importance of understanding not only changes in total porosity but also how the distribution of porosity evolves with reaction that affects permeability.« less

Straw incorporation increases crop yield and soil organic carbon sequestration but varies under different natural conditions and farming practices in China: a system analysis

NASA Astrophysics Data System (ADS)

Han, Xiao; Xu, Cong; Dungait, Jennifer A. J.; Bol, Roland; Wang, Xiaojie; Wu, Wenliang; Meng, Fanqiao

2018-04-01

Loss of soil organic carbon (SOC) from agricultural soils is a key indicator of soil degradation associated with reductions in net primary productivity in crop production systems worldwide. Technically simple and locally appropriate solutions are required for farmers to increase SOC and to improve cropland management. In the last 30 years, straw incorporation (SI) has gradually been implemented across China in the context of agricultural intensification and rural livelihood improvement. A meta-analysis of data published before the end of 2016 was undertaken to investigate the effects of SI on crop production and SOC sequestration. The results of 68 experimental studies throughout China in different edaphic conditions, climate regions and farming regimes were analyzed. Compared with straw removal (SR), SI significantly sequestered SOC (0-20 cm depth) at the rate of 0.35 (95 % CI, 0.31-0.40) Mg C ha-1 yr-1, increased crop grain yield by 13.4 % (9.3-18.4 %) and had a conversion efficiency of the incorporated straw C of 16 % ± 2 % across China. The combined SI at the rate of 3 Mg C ha-1 yr-1 with mineral fertilizer of 200-400 kg N ha-1 yr-1 was demonstrated to be the best farming practice, where crop yield increased by 32.7 % (17.9-56.4 %) and SOC sequestrated by the rate of 0.85 (0.54-1.15) Mg C ha-1 yr-1. SI achieved a higher SOC sequestration rate and crop yield increment when applied to clay soils under high cropping intensities, and in areas such as northeast China where the soil is being degraded. The SOC responses were highest in the initial starting phase of SI, then subsequently declined and finally became negligible after 28-62 years. However, crop yield responses were initially low and then increased, reaching their highest level at 11-15 years after SI. Overall, our study confirmed that SI created a positive feedback loop of SOC enhancement together with increased crop production, and this is of great practical importance to straw management as agriculture intensifies both in China and other regions with different climate conditions.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Grigg, Reid; McPherson, Brian; Lee, Rober

The Southwest Regional Partnership on Carbon Sequestration (SWP) one of seven regional partnerships sponsored by the U.S. Department of Energy (USDOE) carried out five field pilot tests in its Phase II Carbon Sequestration Demonstration effort, to validate the most promising sequestration technologies and infrastructure concepts, including three geologic pilot tests and two terrestrial pilot programs. This field testing demonstrated the efficacy of proposed sequestration technologies to reduce or offset greenhouse gas emissions in the region. Risk mitigation, optimization of monitoring, verification, and accounting (MVA) protocols, and effective outreach and communication were additional critical goals of these field validation tests. Themore » program included geologic pilot tests located in Utah, New Mexico, Texas, and a region-wide terrestrial analysis. Each geologic sequestration test site was intended to include injection of a minimum of ~75,000 tons/year CO{sub 2}, with minimum injection duration of one year. These pilots represent medium- scale validation tests in sinks that host capacity for possible larger-scale sequestration operations in the future. These validation tests also demonstrated a broad variety of carbon sink targets and multiple value-added benefits, including testing of enhanced oil recovery and sequestration, enhanced coalbed methane production and a geologic sequestration test combined with a local terrestrial sequestration pilot. A regional terrestrial sequestration demonstration was also carried out, with a focus on improved terrestrial MVA methods and reporting approaches specific for the Southwest region.« less

78 FR 10003 - Proposed Collection; Comment Request for Notice 2009-XX (NOT-151370-08)

Federal Register 2010, 2011, 2012, 2013, 2014

2013-02-12

... comments concerning Notice 2009-XX, Credit for Carbon Dioxide Sequestration under Section 45Q. [email protected] . SUPPLEMENTARY INFORMATION: Title: Credit for Carbon Dioxide Sequestration under Section... carbon dioxide sequestration (CO 2 sequestration credit) under Sec. 45Q of the Internal Revenue Code...

Method of detecting leakage from geologic formations used to sequester CO.sub.2

DOEpatents

White, Curt [Pittsburgh, PA; Wells, Arthur [Bridgeville, PA; Diehl, J Rodney [Pittsburgh, PA; Strazisar, Brian [Venetia, PA

2010-04-27

The invention provides methods for the measurement of carbon dioxide leakage from sequestration reservoirs. Tracer moieties are injected along with carbon dioxide into geological formations. Leakage is monitored by gas chromatographic analyses of absorbents. The invention also provides a process for the early leak detection of possible carbon dioxide leakage from sequestration reservoirs by measuring methane (CH.sub.4), ethane (C.sub.2H.sub.6), propane (C.sub.3H.sub.8), and/or radon (Rn) leakage rates from the reservoirs. The invention further provides a method for branding sequestered carbon dioxide using perfluorcarbon tracers (PFTs) to show ownership.

Fundamentals of carbon dioxide-enhanced oil recovery (CO2-EOR): a supporting document of the assessment methodology for hydrocarbon recovery using CO2-EOR associated with carbon sequestration

USGS Publications Warehouse

Verma, Mahendra K.

2015-01-01

The objective of this report is to provide basic technical information regarding the CO2-EOR process, which is at the core of the assessment methodology, to estimate the technically recoverable oil within the fields of the identified sedimentary basins of the United States. Emphasis is on CO2-EOR because this is currently one technology being considered as an ultimate long-term geologic storage solution for CO2 owing to its economic profitability from incremental oil production offsetting the cost of carbon sequestration.

A new model of reaction-driven cracking: fluid volume consumption and tensile failure during serpentinization

NASA Astrophysics Data System (ADS)

Eichenbaum-Pikser, J. M.; Spiegelman, M. W.; Kelemen, P. B.; Wilson, C. R.

2013-12-01

Reactive fluid flow plays an important role in a wide range of geodynamic processes, such as melt migration, formation of hydrous minerals on fault surfaces, and chemical weathering. These processes are governed by the complex coupling between fluid transport, reaction, and solid deformation. Reaction-driven cracking is a potentially critical feedback mechanism, by which volume change associated with chemical reaction drives fracture in the surrounding rock. It has been proposed to play a role in both serpentinization and carbonation of peridotite, motivating consideration of its application to mineral carbon sequestration. Previous studies of reactive cracking have focused on the increase in solid volume, and as such, have considered failure in compression. However, if the consumption of fluid is considered in the overall volume budget, the reaction can be net volume reducing, potentially leading to failure in tension. To explore these problems, we have formulated and solved a 2-D model of coupled porous flow, reaction kinetics, and elastic deformation using the finite element model assembler TerraFERMA (Wilson et al, G3 2013 submitted). The model is applied to the serpentinization of peridotite, which can be reasonably approximated as the transfer of a single reactive component (H2O) between fluid and solid phases, making it a simple test case to explore the process. The behavior of the system is controlled by the competition between the rate of volume consumption by the reaction, and the rate of volume replacement by fluid transport, as characterized by a nondimensional parameter χ, which depends on permeability, reaction rate, and the bulk modulus of the solid. Large values of χ correspond to fast fluid transport relative to reaction rate, resulting in a low stress, volume replacing regime. At smaller values of χ, fluid transport cannot keep up with the reaction, resulting in pore fluid under-pressure and tensile solid stresses. For the range of χ relevant to the serpentinization of peridotite, these stresses can reach hundreds of MPa, exceeding the tensile strength of peridotite.

Is it efficient to co-compost and co-vermicompost green waste with biochar and/or clay to reduce CO2 emissions? A short-term laboratory experiment on (vermi)composts with additives.

NASA Astrophysics Data System (ADS)

Barthod, Justine; Rumpel, Cornélia; Paradelo, Remigio; Dignac, Marie-France

2016-04-01

Intensive farming practices can lead to a depletion of soil organic matter, negatively impacting important soil properties such as structural stability, fertility and C storage. The addition of organic amendments such as compost and vermicompost, rich in carbon, helps maintaining soil organic matter levels or restoring degraded soils. Composting and vermicomposting are based on stabilization of organic matter through the mineralization of easily decomposable organic matter compounds, therefore releasing greenhouse gases, including CO2. The aim of this study was to evaluate the global potential reduction of such emissions by the use of additives (2:1 clay and/or biochar): during (vermi)composting processes and after use of the final products as soil amendments. We hypothesized that the interactions between the additives and organic matter may lead to carbon stabilization and that such interactions may be enhanced by the presence of worms (Eisenia). We added in different proportions clay (25% or 50%), biochar (10%) and a mixture of biochar (10%) with clay (25%) to pre-composted green waste. The CO2 emissions of the composting and vermicomposting processes were measured during 21 days. After that, the amendments were added to a loamy cambisol soil and the CO2 emissions were monitored during 30 days of a laboratory experiment. The most efficient treatments in terms of reducing global CO2 emissions were the co-vermicomposting process with 25% clay followed by co-composting with 50% clay and with 10% biochar plus 25% clay. In this treatment (vermicompost with 25% clay), the carbon emissions were decreased by up to 44% compared to regular compost. Addition of biochar reduced CO2 emissions only during composting. Co-composting with biochar could be a promising avenue to limit global CO2 emissions whereas in presence of worms clay additions are better suited. These findings suggest that the presence of worms increased the formation of organo-mineral associations and thus C protection up to a certain clay/organic matter ratio. This strategy could be used to enhance the stability of organic amendments and increase soil carbon sequestration.

Greenhouse gas balance of a Scots pine forest using biometric, eddy covariance and chamber measurements.

NASA Astrophysics Data System (ADS)

Gielen, Bert; De Vos, Bruno; Papale, Dario; Janssens, Ivan

2013-04-01

In recent years, the status of forests as sources or sinks of carbon has received much attention. Nonetheless, evidence-based long-term estimates of the magnitude of the carbon sequestration in forests are still scarce. In this study we present two independent estimates of net carbon sequestration in a temperate Scots pine dominated forest ecosystem over a 9 year period (2002-2010) and in addition, to determine the full greenhouse gas balance, the first results of automated chamber measurements of N2O and CH4. First, the net ecosystem carbon balance (NECB) was estimated from net ecosystem CO2 exchange as measured by the eddy covariance technique (NECBEC). To this end, the eddy covariance estimates were combined with non-CO2 carbon fluxes such as DOC leaching and VOC emissions. The second approach to determine the carbon sequestration was based on the changes in the ecosystem carbon stocks over time (NECBSC). For this NECBSC estimate, two assessments of the ecosystem carbon stocks (2002 and 2010) were compared. Results showed that the eddy covariance approach estimated a net uptake of 2.4 ± 1.25 tC ha-1 yr-1, while the stock based approach suggested a carbon sink of 1.8 ± 1.20 tC ha-1 yr-1. No significant change was observed in the mineral soil carbon, while the carbon stock of the litter layer slightly decreased. Phytomass was thus the main carbon sink (2.1 tC ha-1 yr-1) in the pine forest, predominantly in the stems (1.3 tC ha-1 yr-1). The fact that stem wood is the main carbon sink within the ecosystem implies that the future harvesting has the potential to fully offset the CO2 uptake by this Scots pine forest. Estimates of the impact of N2O and CH4 emissions from the soil on the total greenhouse gas budget will be presented.

Evaluating Impacts of CO2 and CH4 Gas Intrusion into an Unconsolidated Aquifer: Fate of As and Cd

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lawter, Amanda R.; Qafoku, Nikolla; Shao, Hongbo

2015-07-10

Abstract The sequestration of carbon dioxide (CO2) in deep underground reservoirs has been identified as an important strategy to decrease atmospheric CO2 levels and mitigate global warming, but potential risks on overlying aquifers currently lack a complete evaluation. In addition to CO2, other gases such as methane (CH4) may be present in storage reservoirs. This paper explores for the first time the combined effect of leaking CO2 and CH4 gasses on the fate of major, minor and trace elements in an aquifer overlying a potential sequestration site. Emphasis is placed on the fate of arsenic (As) and cadmium (Cd) releasedmore » from the sediments or present as soluble constituents in the leaking brine. Results from macroscopic batch and column experiments show that the presence of CH4 (at a concentration of 1 % in the mixture CO2/CH4) does not have a significant effect on solution pH or the concentrations of most major elements (such as Ca, Ba, and Mg). However, the concentrations of Mn, Mo, Si and Na are inconsistently affected by the presence of CH4 (i.e., in at least one sediment tested in this study). Cd is not released from the sediments and spiked Cd is mostly removed from the aqueous phase most likely via adsorption. The fate of sediment associated As [mainly sorbed arsenite or As(III) in minerals] and spiked As [i.e., As5+] is complex. Possible mechanisms that control the As behavior in this system are discussed in this paper. Results are significant for CO2 sequestration risk evaluation and site selection and demonstrate the importance of evaluating reservoir brine and gas stream composition during site selection to ensure the safest site is being chosen.« less

Woodland carbon code: building an evidence base for the "4 per mil" initiative in land converted to forestry.

NASA Astrophysics Data System (ADS)

Hannam, Jacqueline; Vanguelova, Elena; West, Vicky

2017-04-01

The Woodland Carbon Code is a voluntary standard for woodland creation projects in the UK. Carbon sequestration resulting from certified projects will contribute directly to the UK's national targets for reducing emissions of greenhouse gases (GHG). Whilst this is concerned primarily with above ground capture there is little empirical evidence of the longer term carbon sequestration potential of soils under this land use change in the UK. We present preliminary results from a resurvey of 20 sites originally sampled as part of the soil survey of England and Wales. It includes soil carbon stocks assessed within the soil profile (up to 1m depth) where sites have been converted to forestry in the last 40 years. The small number of sites (n=20) and high variability in soil type, forest type and original land use prevented detailed analysis between these different factors, but overall there was an increase in carbon concentration in the whole profile, driven primarily by an increase the surface organic layers. For all sites combined there was no significant difference in the C stocks between the two survey periods. The increase in carbon stock in the surface organic horizons tended to be offset by a decrease in the mineral subsoils (specifically in Brown Earth soils) primarily as a result of bulk density changes. There are presently insufficient measured data from a range of UK climate, land-use and soil type conditions to quantify with confidence soil C changes during afforestation. This is partly because of the difficulties of detecting relatively slow changes in spatially heterogeneous soils and also obtaining good examples of sites that have undergone documented land use change. Reviewing results from all ongoing afforestation projects in the UK will provide better quantification of the C sequestration potential of forest soils to be accounted for in the Woodland Carbon Code's overall GHG mitigation potential.

Variations in coal characteristics and their possible implications for CO2 sequestration: Tanquary injection site, southeastern Illinois, USA

USGS Publications Warehouse

Morse, D.G.; Mastalerz, Maria; Drobniak, A.; Rupp, J.A.; Harpalani, S.

2010-01-01

As part of the U.S. Department of Energy's Regional Sequestration Partnership program, the potential for sequestering CO2 in the largest bituminous coal reserve in United States - the Illinois Basin - is being assessed at the Tanquary site in Wabash County, southeastern Illinois. To accomplish the main project objectives, which are to determine CO2 injection rates and storage capacity, we developed a detailed coal characterization program. The targeted Springfield Coal occurs at 274m (900ft) depth, is 2.1m (7ft) thick, and is of high volatile B bituminous rank, having an average vitrinite reflectance (Ro) of 0.63%. Desorbed Springfield Coal gas content in cores from four wells ~15 to ~30m (50 to 100ft) apart varies from 4.7-6.6cm3/g (150 to 210scf/ton, dmmf) and consists, generally, of >92% CH4 with lesser amounts of N2 and then CO2. Adsorption isotherms indicate that at least three molecules of CO2 can be stored for each displaced CH4 molecule. Whole seam petrographic composition, which affects sequestration potential, averages 76.5% vitrinite, 4.2% liptinite, 11.6% inertinite, and 7.7% mineral matter. Sulfur content averages 1.59%. Well-developed coal cleats with 1 to 2cm spacing contain partial calcite and/or kaolinite fillings that may decrease coal permeability. The shallow geophysical induction log curves show much higher resistivity in the lower part of the Springfield Coal than the medium or deep curves because of invasion by freshwater drilling fluid, possibly indicating higher permeability. Gamma-ray and bulk density vary, reflecting differences in maceral, ash, and pyrite content. Because coal properties vary across the basin, it is critical to characterize injection site coals to best predict the potential for CO2 injection and storage capacity. ?? 2010 Elsevier B.V.

Aquifer disposal of carbon dioxide for greenhouse effect mitigation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gupta, N.; Naymik, T.G.; Bergman, P.

1998-07-01

Deep aquifer sequestration of carbon dioxide (CO{sup 2}), generated from power plant and other industrial emissions, is being evaluated as one of the potential options for the reduction of atmospheric greenhouse gas emissions. The major advantages of using deep aquifers are that the disposal facilities may be located close to the sources, thus reducing the CO{sub 2} transport costs. The potential capacity is much larger than the projected CO{sub 2} emissions over the next century, and it is a long-term/permanent sequestration option, because a large portion of the injected CO{sub 2} may be fixed into the aquifer by dissolution ormore » mineralization. The major limitations include the potentially high cost, the risk of upward migration, and the public perception of risk. Most of the cost is due to the need to separate CO{sub 2} from other flue gases, rather than the actual cost of disposal. Hazardous liquid waste and acid gas disposal in deep sedimentary formations is a well-established practice. There are also numerous facilities for storage of natural gases in depleted oil and gas reservoirs. The only current facility for aquifer disposal of CO{sub 2} is the offshore injection well at Sleipner Vest in the North Sea in Norway operated by Statoil. Exxon and Pertamina are planning an offshore aquifer disposal facility at Natuna gas field in Indonesia. A major evaluation of the feasibility of CO{sub 2} disposal in the European Union and Norway has been conducted under project Joule II. The data and experience obtained from the existing deep-waste disposal facilities and from the Sleipner Vest site form a strong foundation for further research and development on CO{sub 2} sequestration. Federal Energy Technology Center (FETC) is currently leading a project that uses data from an existing hazardous waste disposal facility injecting in the Mt. Simon Sandstone aquifer in Ohio to evaluate hydrogeologic, geochemical, and social issues related to CO{sub 2} disposal.« less

Aquifer disposal of carbon dioxide for greenhouse effect mitigation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gupta, N.; Naymik, T.G.; Bergman, P.

1998-04-01

Deep aquifer sequestration of carbon dioxide (CO{sub 2}) generated from power plant and other industrial emissions, is being evaluated as one of the potential options for the reduction of atmospheric greenhouse gas emissions. The major advantages of using deep aquifers are that the disposal facilities may be located close to the sources, thus reducing the CO{sub 2} transport costs. The potential capacity is much larger than the projected CO{sub 2} emissions over the next century, and it is a long-term/permanent sequestration option, because a large portion of the injected CO{sub 2} may be fixed into the aquifer by dissolution ormore » mineralization. The major limitations include the potentially high cost, the risk of upward migration, and the public perception of risk. Most of the cost is due to the need to separate CO{sub 2} from other flue gases, rather than the actual cost of disposal. Hazardous liquid waste and acid gas disposal in deep sedimentary formations is a well-established practice. There are also numerous facilities for storage of natural gases in depleted oil and gas reservoirs. The only current facility for aquifer disposal of CO{sub 2} is the offshore injection well at Sleipner Vest in the North Sea in Norway operated by Statoil. Exxon and Pertamina are planning an offshore aquifer disposal facility at Natuna gas field in Indonesia. A major evaluation of the feasibility of CO{sub 2} disposal in the European Union and Norway has been conducted under project Joule II. The data and experience obtained from the existing deep-waste disposal facilities and from the Sleipner Vest site form a strong foundation for further research and development on CO{sub 2} sequestration. Federal Energy Technology Center (FETC) is currently leading a project that uses data from an existing hazardous waste disposal facility injecting in the Mt. Simon Sandstone aquifer in Ohio to evaluate hydrogeologic, geochemical, and social issues related to CO{sub 2} disposal.« less

Predicting long-term carbon sequestration in response to CO 2 enrichment: How and why do current ecosystem models differ?

DOE PAGES

Walker, Anthony P.; Zaehle, Sönke; Medlyn, Belinda E.; ...

2015-04-27

Large uncertainty exists in model projections of the land carbon (C) sink response to increasing atmospheric CO 2. Free-Air CO 2 Enrichment (FACE) experiments lasting a decade or more have investigated ecosystem responses to a step change in atmospheric CO 2 concentration. To interpret FACE results in the context of gradual increases in atmospheric CO 2 over decades to centuries, we used a suite of seven models to simulate the Duke and Oak Ridge FACE experiments extended for 300 years of CO 2 enrichment. We also determine key modeling assumptions that drive divergent projections of terrestrial C uptake and evaluatemore » whether these assumptions can be constrained by experimental evidence. All models simulated increased terrestrial C pools resulting from CO 2 enrichment, though there was substantial variability in quasi-equilibrium C sequestration and rates of change. In two of two models that assume that plant nitrogen (N) uptake is solely a function of soil N supply, the net primary production response to elevated CO 2 became progressively N limited. In four of five models that assume that N uptake is a function of both soil N supply and plant N demand, elevated CO 2 led to reduced ecosystem N losses and thus progressively relaxed nitrogen limitation. Many allocation assumptions resulted in increased wood allocation relative to leaves and roots which reduced the vegetation turnover rate and increased C sequestration. Additionally, self-thinning assumptions had a substantial impact on C sequestration in two models. As a result, accurate representation of N process dynamics (in particular N uptake), allocation, and forest self-thinning is key to minimizing uncertainty in projections of future C sequestration in response to elevated atmospheric CO 2.« less

Vadose Zone Flow and Transport of Dissolved Organic Carbon at Multiple Scales in Humid Regimes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jardine, Philip M; Mayes, Melanie; Mulholland, Patrick J

2006-06-01

Scientists must embrace the necessity to offset global CO{sub 2} emissions regardless of politics. Efforts to enhance terrestrial organic carbon sequestration have traditionally focused on aboveground biomass and surface soils. An unexplored potential exists in thick lower horizons of widespread, mature soils such as Alfisols, Ultisols, and Oxisols. We present a case study of fate and transport of dissolved organic carbon (DOC) in a highly weathered Ultisol, involving spatial scales from the laboratory to the landscape. Our objectives were to interpret processes observed at various scales and provide an improved understanding of coupled hydrogeochemical mechanisms that control DOC mobility andmore » sequestration in deep subsoils within humid climatic regimes. Our approach is multiscale, using laboratory-scale batch and soil columns (0.2 by 1.0 m), an in situ pedon (2 by 2 by 3 m), a well-instrumented subsurface facility on a subwatershed (0.47 ha), and ephemeral and perennial stream discharge at the landscape scale (38.4 ha). Laboratory-scale experiments confirmed that lower horizons have the propensity to accumulate DOC, but that preferential fracture flow tends to limit sequestration. Intermediate-scale experiments demonstrated the beneficial effects of C diffusion into soil micropores. Field- and landscape-scale studies demonstrated coupled hydrological, geochemical, and microbiological mechanisms that limit DOC sequestration, and their sensitivity to local environmental conditions. Our results suggest a multi-scale approach is necessary to assess the propensity of deep subsoils to sequester organic C in situ. By unraveling fundamental organic C sequestration mechanisms, we improve the conceptual and quantitative understanding needed to predict and alter organic C budgets in soil systems.« less

Potential Hydrogeomechanical Impacts of Geological CO2 Sequestration

NASA Astrophysics Data System (ADS)

McPherson, B. J.; Haerer, D.; Han, W.; Heath, J.; Morse, J.

2006-12-01

Long-term sequestration of anthropogenic "greenhouse gases" such as CO2 is a proposed approach to managing climate change. Deep brine reservoirs in sedimentary basins are possible sites for sequestration, given their ubiquitous nature. We used a mathematical sedimentary basin model, including coupling of multiphase CO2-groundwater flow and rock deformation, to evaluate residence times in possible brine reservoir storage sites, migration patterns and rates away from such sites, and effects of CO2 injection on fluid pressures and rock strain. Study areas include the Uinta and Paradox basins of Utah, the San Juan basin of New Mexico, and the Permian basin of west Texas. Regional-scale hydrologic and mechanical properties, including the presence of fracture zones, were calibrated using laboratory and field data. Our initial results suggest that, in general, long-term (~100 years or more) sequestration in deep brine reservoirs is possible, if guided by robust structural and hydrologic data. However, specific processes must be addressed to characterize and minimize risks. In addition to CO2 migration from target sequestration reservoirs into other reservoirs or to the land surface, another environmental issue is displacement of brines into freshwater aquifers. We evaluated the potential for such unintended aquifer contamination by displacement of brines out of adjacent sealing layers such as marine shales. Results suggest that sustained injection of CO2 may incur significant brine displacement out of adjacent sealing layers, depending on the injection history, initial brine composition, and hydrologic properties of both reservoirs and seals. Model simulations also suggest that as injection-induced overpressures migrate, effective stresses may follow this migration under some conditions, as will associated rock strain. Such "strain migration" may lead to induced or reactivated fractures or faults, but can be controlled through reservoir engineering.

Sequestration of maize crop straw C in different soils: role of oxyhydrates in chemical binding and stabilization as recalcitrance.

PubMed

Song, Xiangyun; Li, Lianqing; Zheng, Jufeng; Pan, Genxing; Zhang, Xuhui; Zheng, Jinwei; Hussain, Qaiser; Han, Xiaojun; Yu, Xinyan

2012-05-01

While biophysical controls on the sequestration capacity of soils have been well addressed with physical protection, chemical binding and stabilization processes as well as microbial community changes, the role of chemical binding and stabilization has not yet well characterized for soil organic carbon (SOC) sequestration in rice paddies. In this study, a 6-month laboratory incubation with and without maize straw amendment (MSA) was conducted using topsoil samples from soils with different clay mineralogy and free oxy-hydrate contents collected across Southern China. The increase in SOC under MSA was found coincident with that in Fe- and Al-bound OC (Fe/Al-OC) after incubation for 30 d (R(2)=0.90, P=0.05), and with sodium dithionate-citrate-bicarbonate (DCB) extractable Fe after incubation for 180 d (R(2)=0.99, P<0.01). The increase in SOC under MSA was found higher in soils rich in DCB extractable Fe than those poor in DCB extractable Fe. The greater SOC sequestration in soils rich in DCB extractable Fe was further supported by the higher abundance of (13)C which was a natural signature of MSA. Moreover, a weak positive correlation of the increased SOC under MSA with the increased humin (R(2)=0.87, P=0.06) observed after incubation for 180 d may indicate a chemical stabilization of sequestered SOC as humin in the long run. These results improved our understanding of SOC sequestration in China's rice paddies that involves an initial chemical binding of amended C and a final stabilization as recalcitrant C of humin. Copyright © 2012 Elsevier Ltd. All rights reserved.

Plants Regulate Soil Organic Matter Decomposition in Response to Sea Level Rise

NASA Astrophysics Data System (ADS)

Megonigal, P.; Mueller, P.; Jensen, K.

2014-12-01

Tidal wetlands have a large capacity for producing and storing organic matter, making their role in the global carbon budget disproportionate to their land area. Most of the organic matter stored in these systems is in soils where it contributes 2-5 times more to surface accretion than an equal mass of minerals. Soil organic matter (SOM) sequestration is the primary process by which tidal wetlands become perched high in the tidal frame, decreasing their vulnerability to accelerated sea level rise. Plant growth responses to sea level rise are well understood and represented in century-scale forecast models of soil surface elevation change. We understand far less about the response of soil organic matter decomposition to rapid sea level rise. Here we quantified the effects of sea level on SOM decomposition rates by exposing planted and unplanted tidal marsh monoliths to experimentally manipulated flood duration. The study was performed in a field-based mesocosm facility at the Smithsonian's Global Change Research Wetland. SOM decomposition rate was quantified as CO2 efflux, with plant- and SOM-derived CO2 separated with a two end-member δ13C-CO2 model. Despite the dogma that decomposition rates are inversely related to flooding, SOM mineralization was not sensitive to flood duration over a 35 cm range in soil surface elevation. However, decomposition rates were strongly and positively related to aboveground biomass (R2≥0.59, p≤0.01). We conclude that soil carbon loss through decomposition is driven by plant responses to sea level in this intensively studied tidal marsh. If this result applies more generally to tidal wetlands, it has important implications for modeling soil organic matter and surface elevation change in response to accelerated sea level rise.

Status and potential of terrestrial carbon sequestration in West Virginia

Treesearch

Benktesh D. Sharma; Jingxin Wang

2011-01-01

Terrestrial ecosystem management offers cost-effective ways to enhance carbon (C) sequestration. This study utilized C stock and C sequestration in forest and agricultural lands, abandoned mine lands, and harvested wood products to estimate the net current annual C sequestration in West Virginia. Several management options within these components were simulated using a...

Tidal dynamics and mangrove carbon sequestration during the Oligo–Miocene in the South China Sea

PubMed Central

Collins, Daniel S.; Avdis, Alexandros; Allison, Peter A.; Johnson, Howard D.; Hill, Jon; Piggott, Matthew D.; Hassan, Meor H. Amir; Damit, Abdul Razak

2017-01-01

Modern mangroves are among the most carbon-rich biomes on Earth, but their long-term (≥106 years) impact on the global carbon cycle is unknown. The extent, productivity and preservation of mangroves are controlled by the interplay of tectonics, global sea level and sedimentation, including tide, wave and fluvial processes. The impact of these processes on mangrove-bearing successions in the Oligo–Miocene of the South China Sea (SCS) is evaluated herein. Palaeogeographic reconstructions, palaeotidal modelling and facies analysis suggest that elevated tidal range and bed shear stress optimized mangrove development along tide-influenced tropical coastlines. Preservation of mangrove organic carbon (OC) was promoted by high tectonic subsidence and fluvial sediment supply. Lithospheric storage of OC in peripheral SCS basins potentially exceeded 4,000 Gt (equivalent to 2,000 p.p.m. of atmospheric CO2). These results highlight the crucial impact of tectonic and oceanographic processes on mangrove OC sequestration within the global carbon cycle on geological timescales. PMID:28643789

Developing seeds of Arabidopsis store different minerals in two types of vacuoles and in the endoplasmic reticulum.

PubMed

Otegui, Marisa S; Capp, Roberta; Staehelin, L Andrew

2002-06-01

Mineral-accumulating compartments in developing seeds of Arabidopsis were studied using high-pressure-frozen/freeze-substituted samples. Developing seeds store minerals in three locations: in the protein storage vacuoles of the embryo, and transiently in the endoplasmic reticulum (ER) and vacuolar compartments of the chalazal endosperm. Energy dispersive x-ray spectroscopy and enzyme treatments suggest that the minerals are stored as phytic acid (myo-inositol-1,2,3,4,5,6-hexakisphosphate) salts in all three compartments, although they differ in cation composition. Whereas embryo globoids contain Mg, K, and Ca as cations, the chalazal ER deposits show high levels of Mn, and the chalazal vacuolar deposits show high levels of Zn. The appearance of the first Zn-phytate crystals coincides with the formation of network-like extensions of the chalazal vacuoles. The core of these networks consists of a branched network of tubular ER membranes, which are separated from the delineating tonoplast membranes by a layer of cytosolic material. Degradation of the networks starts with the loss of the cytosol and is followed by the retraction of the ER, generating a network of collapsed tonoplast membranes that are resorbed. Studies of fertilized fis2 seeds, which hyperaccumulate Zn-phytate crystals in the chalazal vacuolar compartments, suggest that only the intact network is active in mineral sequestration. Mineral determination analysis and structural observations showed that Zn and Mn are mobilized from the endosperm to the embryo at different developmental stages. Thus, Zn appears to be removed from the endosperm at the late globular stage, and Mn stores appear to be removed at the late bent-cotyledon stage of embryo development. The disappearance of the Mn-phytate from the endosperm coincides with the accumulation of two major Mn binding proteins in the embryo, the 33-kD protein from the oxygen-evolving complex of photosystem II and the Mn superoxide dismutase. The possible functions of transient heavy metal storage in the chalazal endosperm are discussed. A model showing how phytic acid, a potentially cytotoxic molecule, is transported from its site of synthesis, the ER, to the different mineral storage sites is presented.

Developing Seeds of Arabidopsis Store Different Minerals in Two Types of Vacuoles and in the Endoplasmic Reticulum

PubMed Central

Otegui, Marisa S.; Capp, Roberta; Staehelin, L. Andrew

2002-01-01

Mineral-accumulating compartments in developing seeds of Arabidopsis were studied using high-pressure-frozen/freeze-substituted samples. Developing seeds store minerals in three locations: in the protein storage vacuoles of the embryo, and transiently in the endoplasmic reticulum (ER) and vacuolar compartments of the chalazal endosperm. Energy dispersive x-ray spectroscopy and enzyme treatments suggest that the minerals are stored as phytic acid (myo-inositol-1,2,3,4,5,6-hexakisphosphate) salts in all three compartments, although they differ in cation composition. Whereas embryo globoids contain Mg, K, and Ca as cations, the chalazal ER deposits show high levels of Mn, and the chalazal vacuolar deposits show high levels of Zn. The appearance of the first Zn-phytate crystals coincides with the formation of network-like extensions of the chalazal vacuoles. The core of these networks consists of a branched network of tubular ER membranes, which are separated from the delineating tonoplast membranes by a layer of cytosolic material. Degradation of the networks starts with the loss of the cytosol and is followed by the retraction of the ER, generating a network of collapsed tonoplast membranes that are resorbed. Studies of fertilized fis2 seeds, which hyperaccumulate Zn-phytate crystals in the chalazal vacuolar compartments, suggest that only the intact network is active in mineral sequestration. Mineral determination analysis and structural observations showed that Zn and Mn are mobilized from the endosperm to the embryo at different developmental stages. Thus, Zn appears to be removed from the endosperm at the late globular stage, and Mn stores appear to be removed at the late bent-cotyledon stage of embryo development. The disappearance of the Mn-phytate from the endosperm coincides with the accumulation of two major Mn binding proteins in the embryo, the 33-kD protein from the oxygen-evolving complex of photosystem II and the Mn superoxide dismutase. The possible functions of transient heavy metal storage in the chalazal endosperm are discussed. A model showing how phytic acid, a potentially cytotoxic molecule, is transported from its site of synthesis, the ER, to the different mineral storage sites is presented. PMID:12084829

Fresh Water Generation from Aquifer-Pressured Carbon Storage: Interim Progress Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aines, R D; Wolery, T J; Hao, Y

2009-07-22

This project is establishing the potential for using brine pressurized by Carbon Capture and Storage (CCS) operations in saline formations as the feedstock for desalination and water treatment technologies including nanofiltration (NF) and reverse osmosis (RO). The aquifer pressure resulting from the energy required to inject the carbon dioxide provides all or part of the inlet pressure for the desalination system. Residual brine would be reinjected into the formation at net volume reduction. This process provides additional storage space (capacity) in the aquifer, reduces operational risks by relieving overpressure in the aquifer, and provides a source of low-cost fresh watermore » to offset costs or operational water needs. Computer modeling and laboratory-scale experimentation are being used to examine mineral scaling and osmotic pressure limitations for brines typical of CCS sites. Computer modeling is being used to evaluate processes in the aquifer, including the evolution of the pressure field. This progress report deals mainly with our geochemical modeling of high-salinity brines and covers the first six months of project execution (September, 2008 to March, 2009). Costs and implementation results will be presented in the annual report. The brines typical of sequestration sites can be several times more concentrated than seawater, requiring specialized modeling codes typical of those developed for nuclear waste disposal calculations. The osmotic pressure developed as the brines are concentrated is of particular concern, as are precipitates that can cause fouling of reverse osmosis membranes and other types of membranes (e.g., NF). We have now completed the development associated with tasks (1) and (2) of the work plan. We now have a contract with Perlorica, Inc., to provide support to the cost analysis and nanofiltration evaluation. We have also conducted several preliminary analyses of the pressure effect in the reservoir in order to confirm that reservoir pressure can indeed be used to drive the reverse osmosis process. Our initial conclusions from the work to date are encouraging: (1) The concept of aquifer-pressured RO to provide fresh water associated with carbon dioxide storage appears feasible. (2) Concentrated brines such as those found in Wyoming are amenable to RO treatment. We have looked at sodium chloride brines from the Nugget Formation in Sublette County. 20-25% removal with conventional methods is realistic; higher removal appears achievable with NF. The less concentrated sulfate-rich brines from the Tensleep Formation in Sublette County would support >80% removal with conventional RO. (3) Brines from other proposed sequestration sites can now be analyzed readily. An osmotic pressure curve appropriate to these brines can be used to evaluate cost and equipment specifications. (4) We have examined a range of subsurface brine compositions that is potentially pertinent to carbon sequestration and noted the principal compositional trends pertinent to evaluating the feasibility of freshwater extraction. We have proposed a general categorization for the feasibility of the process based on total dissolved solids (TDS). (5) Withdrawing pressurized brine can have a very beneficial effect on reservoir pressure and total available storage capacity. Brine must be extracted from a deeper location in the aquifer than the point of CO{sub 2} injection to prevent CO{sub 2} from migrating to the brine extraction well.« less

Different designs of kinase-phosphatase interactions and phosphatase sequestration shapes the robustness and signal flow in the MAPK cascade

PubMed Central

2012-01-01

Background The three layer mitogen activated protein kinase (MAPK) signaling cascade exhibits different designs of interactions between its kinases and phosphatases. While the sequential interactions between the three kinases of the cascade are tightly preserved, the phosphatases of the cascade, such as MKP3 and PP2A, exhibit relatively diverse interactions with their substrate kinases. Additionally, the kinases of the MAPK cascade can also sequester their phosphatases. Thus, each topologically distinct interaction design of kinases and phosphatases could exhibit unique signal processing characteristics, and the presence of phosphatase sequestration may lead to further fine tuning of the propagated signal. Results We have built four architecturally distinct types of models of the MAPK cascade, each model with identical kinase-kinase interactions but unique kinases-phosphatases interactions. Our simulations unravelled that MAPK cascade’s robustness to external perturbations is a function of nature of interaction between its kinases and phosphatases. The cascade’s output robustness was enhanced when phosphatases were sequestrated by their target kinases. We uncovered a novel implicit/hidden negative feedback loop from the phosphatase MKP3 to its upstream kinase Raf-1, in a cascade resembling the B cell MAPK cascade. Notably, strength of the feedback loop was reciprocal to the strength of phosphatases’ sequestration and stronger sequestration abolished the feedback loop completely. An experimental method to verify the presence of the feedback loop is also proposed. We further showed, when the models were activated by transient signal, memory (total time taken by the cascade output to reach its unstimulated level after removal of signal) of a cascade was determined by the specific designs of interaction among its kinases and phosphatases. Conclusions Differences in interaction designs among the kinases and phosphatases can differentially shape the robustness and signal response behaviour of the MAPK cascade and phosphatase sequestration dramatically enhances the robustness to perturbations in each of the cascade. An implicit negative feedback loop was uncovered from our analysis and we found that strength of the negative feedback loop is reciprocally related to the strength of phosphatase sequestration. Duration of output phosphorylation in response to a transient signal was also found to be determined by the individual cascade’s kinase-phosphatase interaction design. PMID:22748295

Simulating carbon sequestration using cellular automata and land use assessment for Karaj, Iran

NASA Astrophysics Data System (ADS)

Khatibi, Ali; Pourebrahim, Sharareh; Mokhtar, Mazlin Bin

2018-06-01

Carbon sequestration has been proposed as a means of slowing the atmospheric and marine accumulation of greenhouse gases. This study used observed and simulated land use/cover changes to investigate and predict carbon sequestration rates in the city of Karaj. Karaj, a metropolis of Iran, has undergone rapid population expansion and associated changes in recent years, and these changes make it suitable for use as a case study for rapidly expanding urban areas. In particular, high quality agricultural space, green space and gardens have rapidly transformed into industrial, residential and urban service areas. Five classes of land use/cover (residential, agricultural, rangeland, forest and barren areas) were considered in the study; vegetation and soil samples were taken from 20 randomly selected locations. The level of carbon sequestration was determined for the vegetation samples by calculating the amount of organic carbon present using the dry plant weight method, and for soil samples by using the method of Walkley and Black. For each area class, average values of carbon sequestration in vegetation and soil samples were calculated to give a carbon sequestration index. A cellular automata approach was used to simulate changes in the classes. Finally, the carbon sequestration indices were combined with simulation results to calculate changes in carbon sequestration for each class. It is predicted that, in the 15 year period from 2014 to 2029, much agricultural land will be transformed into residential land, resulting in a severe reduction in the level of carbon sequestration. Results from this study indicate that expansion of forest areas in urban counties would be an effective means of increasing the levels of carbon sequestration. Finally, future opportunities to include carbon sequestration into the simulation of land use/cover changes are outlined.

Going With the Flow: An Aid in Detecting and Differentiating Bronchopulmonary Sequestrations and Hybrid Lesions.

PubMed

Oliver, Edward R; DeBari, Suzanne E; Giannone, Mariann M; Pogoriler, Jennifer E; Johnson, Ann M; Horii, Steven C; Gebb, Juliana S; Howell, Lori J; Adzick, N Scott; Coleman, Beverly G

2018-02-01

To assess the ability of prenatal ultrasound (US) in identifying systemic feeding arteries in bronchopulmonary sequestrations and hybrid lesions and report the ability of US in classifying bronchopulmonary sequestrations as intralobar or extralobar. Institutional Review Board-approved radiology and clinical database searches from 2008 to 2015 were performed for prenatal lung lesions with final diagnoses of bronchopulmonary sequestrations or hybrid lesions. All patients had detailed US examinations, and most patients had ultrafast magnetic resonance imaging (MRI). Lesion location, size, and identification of systemic feeding arteries and draining veins were assessed with US. The study consisted of 102 bronchopulmonary sequestrations and 86 hybrid lesions. The median maternal age was 30 years. The median gestational age was 22 weeks 5 days. Of bronchopulmonary sequestrations, 66 had surgical pathologic confirmation, and 100 had postnatal imaging. Bronchopulmonary sequestration locations were intrathoracic (n = 77), intra-abdominal (n = 19), and transdiaphragmatic (n = 6). Of hybrid lesions, 84 had surgical pathologic confirmation, and 83 had postnatal imaging. Hybrid lesion locations were intrathoracic (n = 84) and transdiaphragmatic (n = 2). Ultrasound correctly identified systemic feeding arteries in 86 of 102 bronchopulmonary sequestrations and 79 of 86 hybrid lesions. Of patients who underwent MRI, systemic feeding arteries were reported in 62 of 92 bronchopulmonary sequestrations and 56 of 81 hybrid lesions. Ultrasound identified more systemic feeding arteries than MRI in both bronchopulmonary sequestrations and hybrid lesions (P < .01). Magnetic resonance imaging identified systemic feeding arteries that US did not in only 2 cases. In cases in which both systemic feeding arteries and draining veins were identified, US could correctly predict intrathoracic lesions as intralobar or extralobar in 44 of 49 bronchopulmonary sequestrations and 68 of 73 hybrid lesions. Ultrasound is most accurate for systemic feeding artery detection in bronchopulmonary sequestrations and hybrid lesions and can also type the lesions as intralobar or extralobar when draining veins are evaluated. © 2017 by the American Institute of Ultrasound in Medicine.

The influence of wildfire severity on soil char composition and nitrogen dynamics

NASA Astrophysics Data System (ADS)

Rhoades, Charles; Fegel, Timothy; Chow, Alex; Tsai, Kuo-Pei; Norman, John, III; Kelly, Eugene

2017-04-01

Forest fires cause lasting ecological changes and alter the biogeochemical processes that control stream water quality. Decreased plant nutrient uptake is the mechanism often held responsible for lasting post-fire shifts in nutrient supply and demand, though other upland and in-stream factors also likely contribute to elevated stream nutrient losses. Soil heating, for example, creates pyrogenic carbon (C) and char layers that influence C and nitrogen (N) cycling. Char layer composition and persistence vary across burned landscapes and are influenced first by fire behavior through the temperature and duration of combustion and then by post-fire erosion. To evaluate the link between soil char and stream C and N export we studied areas burned by the 2002 Hayman Fire, the largest wildfire in Colorado, USA history. We compared soil C and N pools and processes across ecotones that included 1) unburned forests, 2) areas with moderate and 3) high wildfire severity. We analyzed 1-2 cm thick charred organic layers that remain visible 15 years after the fire, underlying mineral soils, and soluble leachate from both layers. Unburned soils released more dissolved organic C and N (DOC and DON) from organic and mineral soil layers than burned soils. The composition of DOC leachate characterized by UV-fluorescence, emission-excitation matrices (EEMs) and Fluorescence Regional Integration (FRI) found similarity between burned and unburned soils, underscoring a common organic matter source. Humic and fulvic acid-like fractions, contained in regions V and III of the FRI model, comprised the majority of the fluorescing DOM in both unburned and char layers. Similarity between two EEMs indices (Fluorescence and Freshness), further denote that unburned soils and char layers originate from the same source and are consistent with visual evidence char layers contain significant amounts of unaltered OM. However, the EEMs humification index (HIX) and compositional analysis with pyrolysis GCMS both indicate that C contained or leached from severely-burned char layers has higher aromaticity and thus chemical stability compared to C in unburned soils. Mineral soil (0-5 cm depth) beneath char layers in high severity portions of the Hayman Fire had significantly more soil N and C and lower pH. Potential net mineralization - an index of the supply of plant-available nitrogen - differed between the severely-burned areas and both unburned and moderately-burn areas. Negative net mineralization in unburned and moderately burned soils indicates immobilization or retention of inorganic N by soil microbes. In contrast, soils burned at high severity produced inorganic N sources available to plants, leaching and gas losses. Water soluble nitrate comprised a larger proportion of inorganic N leached from the char layer of high severity burns. Mineral soil in those areas had both higher water soluble nitrate and total inorganic N in leachate. Char layers that have persisted for fifteen years influence soil N turnover within the Hayman Fire affected area and may contribute to elevated N losses in streams burned at high severity. The chemical stability of soil char layers perpetuates their importance for C sequestration and N dynamics in burned landscapes.

Speciation and weathering of selenium in upper cretaceous chalk and shale from South Dakota and Wyoming, USA

NASA Astrophysics Data System (ADS)

Kulp, Thomas R.; Pratt, Lisa M.

2004-09-01

In geologic materials, petroleum, and the environment, selenium occurs in various oxidation states (VI, IV, 0, -II), mineralized forms, and organo-Se complexes. Each of these forms is characterized by specific chemical and biochemical properties that control the element's solubility, toxicity, and environmental behavior. The organic rich chalks and shales of the Upper Cretaceous Niobrara Formation and the Pierre Shale in South Dakota and Wyoming are bentoniferous stratigraphic intervals characterized by anomalously high concentrations of naturally occurring Se. Numerous environmental problems have been associated with Se derived from these geological units, including the development of seleniferous soils and vegetation that are toxic to livestock and the contamination of drinking water supplies by Se mobilized in groundwater. This study describes a sequential extraction protocol followed by speciation treatments and quantitative analysis by Hydride Generation-Atomic Absorption Spectroscopy. This protocol was utilized to investigate the geochemical forms and the oxidation states in which Se occurs in these geologic units. Organic Se and di-selenide minerals are the predominant forms of Se present in the chalks, shales, and bentonites, but distinctive variations in these forms were observed between different sample types. Chalks contain significantly greater proportions of Se in the form of di-selenide minerals (including Se associated with pyrite) than the shales where base-soluble, humic, organo-Se complexes are more prevalent. A comparison between unweathered samples collected from lithologic drill cores and weathered samples collected from outcrop suggest that the humic, organic-Se compounds in shale are formed during oxidative weathering and that Se oxidized by weathering is more likely to be retained by shale than by chalk. Selenium enrichment in bentonites is inferred to result from secondary processes including the adsorption of Se mobilized by groundwater from surrounding organic rich sediments to clay mineral and iron hydroxide surfaces, as well as microbial reduction of Se within the bentonitic intervals. Distinct differences are inferred for the biogeochemical pathways that affected sedimentary Se sequestration during periods of chalk accumulation compared to shale deposition in the Cretaceous seaway. Mineralogy of sediment and the nature of the organic matter associated with each of these rock types have important implications for the environmental chemistry and release of Se to the environment during weathering.

Linking measurements of biodegradability, thermal stability and chemical composition to evaluate the effects of management on soil organic matter

NASA Astrophysics Data System (ADS)

Gregorich, Ed; Gillespie, Adam; Beare, Mike; Curtin, Denis; Sanei, Hamed; Yanni, Sandra

2015-04-01

The stability of soil organic matter (SOM) as it relates to resistance to microbial degradation has important implications for nutrient cycling, emission of greenhouse gases, and C sequestration. Hence, there is interest in developing new ways to accurately quantify and characterise the labile and stable forms of soil organic C. Our objectives in this study were to evaluate and describe relationships among the biodegradability, thermal stability and chemistry of SOM in soil under widely contrasting management regimes. Samples from the same soil under permanent pasture, an arable cropping rotation, and chemical fallow were fractionated (sand: 2000-50 μm; silt: 50-5 μm, and clay: < 5 μm). Biodegradability of the SOM in size fractions and whole soils was assessed in a laboratory mineralization study. The chemical composition of SOM was characterized by X-ray absorption near-edge structure (XANES) spectroscopy at the K-edge and its thermal stability was determined by analytical pyrolysis using a Rock-Eval pyrolyser. The mineralization bioassay showed that whole soils and soil fractions under fallow were less susceptible to biodegradation than other managements and that sand-associated organic matter was significantly more susceptible than that in the silt or clay fractions. Analysis by XANES showed accumulation of carboxylates and strong depletion of amides (protein) and aromatics in the fallow whole soil. Moreover, protein depletion was most significant in the sand fraction of the fallow soil. Sand fractions in fallow and cropped soils were, however, enriched in plant-derived phenols, aromatics and carboxylates compared to the sand fraction of pasture soils. In contrast, ketones, which have been identified as products of microbially-processed organic matter, were slightly enriched in the silt fraction of the pasture soil. These data suggest reduced inputs and cropping restrict the decomposition of plant residues and, without supplemental N additions, protein-N in native SOM is significantly mineralized in fallow systems to meet microbial C mineralization demands. Analytical pyrolysis showed distinct differences in the thermal stability of SOM among the size fractions and management treatments; it also showed that the loss of SOM generally involved dehydrogenation. The temperature at which half of the C was pyrolyzed showed strong correlation with mineralizable C and thus provides solid evidence for a link between the biological and thermal stability of SOM.

Revealing fate of CO2 leakage pathways in the Little Grand Wash Fault, Green River, Utah

NASA Astrophysics Data System (ADS)

Han, K.; Han, W. S.; Watson, Z. T.; Guyant, E.; Park, E.

2015-12-01

To assure long-term security of geologic carbon sequestration site, evaluation of natural CO2 leakage should be preceded before actual construction of the CO2 facility by comparing natural and artificial reservoir systems. The Little Grand Wash fault is located at the northwestern margin of the Paradox Basin and roles on a bypass of deep subsurface CO2 and brine water onto the surface, e.g., cold water geyser, CO2 spring, and surface travertine deposits. CO2 degassed out from brine at the Little Grand Wash fault zone may react with formation water and minerals while migrating through the fault conduit. Leakage observed by soil CO2 flux on the fault trace shows this ongoing transition of CO2, from supersaturated condition in deep subsurface to shallow surface equilibria. The present study aims to investigate the reactions induced by changes in hydrological and mineralogical factors inside of the fault zone. The methodology to develop site-specific geochemical model of the Little Grand Wash Fault combines calculated mechanical movements of each fluid end-member, along with chemical reactions among fluid, free CO2 gas and rock formations. Reactive transport modeling was conducted to simulate these property changes inside of the fault zone, using chemistry dataset based on 86 effluent samples of CO2 geysers, springs and in situ formation water from Entrada, Carmel, and Navajo Sandstone. Meanwhile, one- and two-dimensional models were separately developed to delineate features mentioned above. The results from the 3000-year simulation showed an appearance of self-sealing processes near the surface of the fault conduit. By tracking physicochemical changes at the depth of 15 m on the 2-dimensional model, significant changes induced by fluid mixing were indicated. Calculated rates of precipitation for calcite, illite, and pyrite showed increase in 2.6 x 10-4, 2.25 x 10-5, and 3.0 x 10-6 in mineral volume fraction at the depth of 15m, respectively. Concurrently, permeability and porosity were decreased 4.0 x 10-18 m2 and 3.0 x 10-4 due to precipitation of minerals. At the middle of the fault conduit (400 m), however, indicates consistent dissolution of minerals in formation which enhances vertical fluid migration.

Carbon dioxide sequestration in municipal solid waste incinerator (MSWI) bottom ash.

PubMed

Rendek, Eva; Ducom, Gaëlle; Germain, Patrick

2006-01-16

During bottom ash weathering, carbonation under atmospheric conditions induces physico-chemical evolutions leading to the pacification of the material. Fresh bottom ash samples were subjected to an accelerated carbonation using pure CO2. The aim of this work was to quantify the volume of CO2 that could be sequestrated with a view to reduce greenhouse gas emissions and investigate the possibility of upgrading some specific properties of the material with accelerated carbonation. Carbonation was performed by putting 4mm-sieved samples in a CO2 chamber. The CO2 pressure and the humidity of the samples were varied to optimize the reaction parameters. Unsieved material was also tested. Calcite formation resulting from accelerated carbonation was investigated by thermogravimetry and differential scanning calorimetry (TG/DSC) and metal leaching tests were performed. The volume of sequestrated CO2 was on average 12.5L/kg dry matter (DM) for unsieved material and 24 L/kg DM for 4mm-sieved samples. An ash humidity of 15% appeared to give the best results. The reaction was drastically accelerated at high pressure but it did not increase the volume of sequestrated CO2. Accelerated carbonation, like the natural phenomenon, reduces the dangerous nature of the material. It decreases the pH from 11.8 to 8.2 and causes Pb, Cr and Cd leaching to decrease. This process could reduce incinerator CO2 emissions by 0.5-1%.

Forsterite Carbonation in Wet Supercritical CO2 and Sodium Citrate

NASA Astrophysics Data System (ADS)

Qiu, L.; Schaef, T.; Wang, Z.; Miller, Q.; McGrail, P.

2013-12-01

Lin Qiu1*, Herbert T. Schaef2, Zhengrong Wang1, Quin R.S. Miller3, BP McGrail2 1. Yale University, New Haven, CT, USA 2. Pacific Northwest National Laboratory, Richland, WA, USA 3. University of Wyoming, Laramie, WY, USA Geologic reservoirs for managing carbon emissions (mostly CO2) have expanded over the last 5 years to include unconventional formations including basalts and fractured shales. Recently, ~1000 metric tons of CO2 was injected into the Columbia River Basalt (CRB) in Eastern Washington as part of the Wallula Pilot Project, Big Sky Regional Carbon Partnership. Based on reservoir conditions, the injected CO2 is present as a supercritical fluid that dissolves into the formation water over time, and reacts with basalt components to form carbonate minerals. In this paper, we discuss mineral transformation reactions occurring when the forsterite (Mg2SiO4) is exposed to wet scCO2 in equilibrium with pure water and sodium citrate solutions. Forsterite was selected as it is an important olivine group mineral present in igneous and mafic rocks. Citrate was selected as it has been shown to enhance mineral dissolution and organic ligands are possible degradation products of the microbial communities present in the formational waters of the CRB. For the supercritical phase, transformation reactions were examined by in situ high pressure x-ray diffraction (HXRD) in the presence of supercritical carbon dioxide (scCO2) in contact with water and sodium citrate solutions at conditions relevant to carbon sequestration. Experimental results show close-to-complete dissolution of forsterite in contact with scCO2 equilibrated with pure water for 90 hours (90 bar and 50°C). Under these conditions, thin films of water coated the mineral surface, providing a mechanism for silicate dissolution and transport of cations necessary for carbonate formation. The primary crystalline component initially detected with in situ HXRD was the hydrated magnesium carbonate, nesquehonite [MgCO3-3H2O], which reached a maximum concentration of 85 wt% within ~30 hours of the experiment before decreasing below detection limit. Detection of the anhydrous magnesium carbonate, magnesite [MgCO3], first occurred at 15 hours, but increased dramatically over the remaining course of the experiment to levels near 90 wt%. In contrast, the presence of sodium citrate solutions in the reactor could eliminate the formation of nesquehonite. Based on the in situ HXRD results, nesquehonite did not form during experiments having sodium citrate solutions of 0.1 M, and the forsterite carbonation proceeded directly to magnesite at a concentration 90 wt% after 80 hours. Testing with less or more concentrated sodium citrate solutions (0.01 or 0.5 M), the nesquehonite formation was not attenuated or overall carbonation rates were decreased, respectively. These results indicate the possibility of organic compounds to dissolve into wet supercritical CO2 fluids and impact the formation of hydrated crystalline carbonates (often considered as transitional phases in carbonation routes to more stable minerals). Likely processes under consideration include the formation of organic complexes with metal cations in the thin water film. These results also have implications for ex situ carbonation processes and highlight the possibility of utilizing organic additives to enhance mineral dissolution prior to carbonation.

100% Solids Polyurethane Sequestration Coating

DTIC Science & Technology

2014-04-11

Distribution Unlimited 100% Solids Polyurethane Sequestration Coating The views, opinions and/or findings contained in this report are those of the...Papers published in non peer-reviewed journals: 100% Solids Polyurethane Sequestration Coating Report Title Report developed under Topic #CBD13-101...Final Technical Report Contract #: W911NF-13-P-0010 Proposal #: 63958CHSB1 Project: 100% Solids Polyurethane Sequestration Coating

Processes regulating progressive nitrogen limitation under elevated carbon dioxide: a meta-analysis

NASA Astrophysics Data System (ADS)

Liang, Junyi; Qi, Xuan; Souza, Lara; Luo, Yiqi

2016-05-01

The nitrogen (N) cycle has the potential to regulate climate change through its influence on carbon (C) sequestration. Although extensive research has explored whether or not progressive N limitation (PNL) occurs under CO2 enrichment, a comprehensive assessment of the processes that regulate PNL is still lacking. Here, we quantitatively synthesized the responses of all major processes and pools in the terrestrial N cycle with meta-analysis of CO2 experimental data available in the literature. The results showed that CO2 enrichment significantly increased N sequestration in the plant and litter pools but not in the soil pool, partially supporting one of the basic assumptions in the PNL hypothesis that elevated CO2 results in more N sequestered in organic pools. However, CO2 enrichment significantly increased the N influx via biological N fixation and the loss via N2O emission, but decreased the N efflux via leaching. In addition, no general diminished CO2 fertilization effect on plant growth was observed over time up to the longest experiment of 13 years. Overall, our analyses suggest that the extra N supply by the increased biological N fixation and decreased leaching may potentially alleviate PNL under elevated CO2 conditions in spite of the increases in plant N sequestration and N2O emission. Moreover, our syntheses indicate that CO2 enrichment increases soil ammonium (NH4+) to nitrate (NO3-) ratio. The changed NH4+/NO3- ratio and subsequent biological processes may result in changes in soil microenvironments, above-belowground community structures and associated interactions, which could potentially affect the terrestrial biogeochemical cycles. In addition, our data synthesis suggests that more long-term studies, especially in regions other than temperate ones, are needed for comprehensive assessments of the PNL hypothesis.

Aluminosilicate Dissolution and Silicate Carbonation during Geologic CO2 Sequestration

NASA Astrophysics Data System (ADS)

Min, Yujia

Geologic CO2 sequestration (GCS) is considered a promising method to reduce anthropogenic CO2 emission. Assessing the supercritical CO2 (scCO2) gas or liquid phase water (g, l)-mineral interactions is critical to evaluating the viability of GCS processes. This work contributes to our understanding of geochemical reactions at CO 2-water (g, l)-mineral interfaces, by investigating the dissolution of aluminosilicates in CO2-acidified water (l). Plagioclase and biotite were chosen as model minerals in reservoir rock and caprock, respectively. To elucidate the effects of brine chemistry, first, the influences of cations in brine including Na, Ca, and K, have been investigated. In addition to the cations, the effects of abundant anions including sulfate and oxalate were also examined. Besides the reactions in aqueous phase, we also examine the carbonation of silicates in water (g)-bearing supercritical CO2 (scCO2) under conditions relevant to GCS. For the metal carbonation, in particular, the effects of particle sizes, water, temperature, and pressure on the carbonation of wollastonite were systematically examined. For understanding the cations effects in brine, the impacts of Na concentrations up to 4 M on the dissolution of plagioclase and biotite were examined. High concentrations of Na significantly inhibited plagioclase dissolution by competing adsorption with proton and suppressing proton-promoted dissolution. Ca has a similar effect to Na, and their effects did not suppress each other when Na and Ca co-existed. For biotite, the inhibition effects of Na coupled with an enhancing effect due to ion exchange reaction between Na and interlayer K, which cracked the basal surfaces of biotite. The K in aqueous phase significantly inhibited the dissolution. If the biotite is equilibrated with NaCl solutions initially, the biotite dissolved faster than the original biotite and the dissolution was inhibited by Na and K in brine. The outcomes improve our current knowledge of silicates dissolution to the high salinity conditions in subsurface environments. In addition to cations, the role of anions in geochemical reactions in subsurfaces are important. This study investigated the anion effects by studying sulfate and oxalate. Sulfate formed monodentate surface complexes with the Al sites on plagioclase surface and enhanced the dissolution. Oxalate was also found to enhance the plagioclase dissolution. Co-existing oxalate and sulfate suppressed the effects of sulfate on plagioclase dissolution. This information provides useful insights for understanding the roles of sulfate and organic compounds on the CO2 water-mineral interactions during scCO2 enhanced oil recovery. The results also aid in formulating a scientific guideline of the proper amount of SO2 co-injection with CO2. Water in GCS sites can exist in water-bearing scCO2 in addition to the aqueous phase in brine. Thus, it is important to understand the effects of water-bearing scCO2 on the carbonation of silicates. To address the gap between the nano- and micro-sized particles used in the laboratory to the large grains in field sites, we utilized wollastonite and investigated the effects of particle sizes on the wollastonite carbonation in water-bearing scCO2. The thickness of the reacted layer on the particle surfaces was found to be constant for different sized particles. The amorphous silica layer formed act as a diffusion barrier for water-bearing scCO2. In addition, the reaction extent was higher with more water, lower temperature, and higher pressure. Further, higher water saturation percentage and lower temperature can lead to the formation of more permeable amorphous silica layers. This thesis included the investigations of both liquid phase and vapor phase water that contacted with scCO2, and the effects of cations and anions on both formation and caprock minerals. The findings from this work improve our knowledge of the geochemical reactions at CO2-water-mineral interfaces, which will help us design a safer GCS operation and assess the impacts of GCS on the environmental safety and quality.

Assessing Impacts of 20 yr Old Miscanthus on Soil Organic Carbon Quality

NASA Astrophysics Data System (ADS)

Hu, Yaxian; Schäfer, Gerhard; Kuhn, Nikolaus

2015-04-01

The use of biomass as a renewable energy source has become increasingly popular in Upper Rhine Region to meet the demand for renewable energy. Miscanthus is one of the most favorite biofuel crops, due to its long life and large yields, as well as low energy and fertilizer inputs. However, current research on Miscanthus is mostly focused on the techniques and economics to produce biofuel or the impacts of side products such as ash and sulfur emissions to human health. Research on the potential impacts of Miscanthus onto soil quality, especially carbon quality after long-term adoption, is very limited. Some positive benefits, such as sequestrating organic carbon, have been repeatedly reported in previous research. Yet the quality of newly sequestrated organic carbon and its potential impacts onto global carbon cycling remain unclear. To fully account for the risks and benefits of Miscanthus, it is required to investigate the quality as well as the potential CO2 emissions of soil organic carbon on Miscanthus fields. As a part of the Interreg Project to assess the environmental impacts of biomass production in the Upper Rhine Region, this study aims to evaluate the carbon quality and the potential CO2 emissions after long-term Miscanthus adoption. Soils were sampled at 0-10, 10-40, 40-70, and 70-100 cm depths on three Miscanthus fields with up to 20 years of cultivation in Ammerzwiller France, Münchenstein Switzerland, and Farnsburg Switzerland. Soil texture, pH, organic carbon and nitrogen content were measured for each sampled layer. Topsoils of 0-10 cm and subsoils of 10-40 cm were also incubated for 40 days to determine the mineralization potential of the soil organic matter. Our results show that: 1) only in top soils of 0-10 cm, the 20 year old Miscanthus field has significantly higher soil organic carbon concentrations, than the control site. No significant differences were observed in deeper soil layers. Similar tendencies were also observed for organic nitrogen content as well C/N ratios. This indicates that the positive benefits of Miscanthus in sequestrating organic carbon and improving soil quality are probably only effective in top soils. 2) Soils from the 20 years old Miscanthus fields produced significantly more CO2 than the control site, suggesting the great susceptibility of organic carbon on Miscanthus fields to mineralization. Overall, our results indicate a potentially additional contribution of Miscanthus fields to atmospheric CO2 compared to reference soils, cautioning the widespread adoption of Miscanthus. Consequently, further studies aiming at a full emission balance are required to assess the overall environmental impacts of biomass production in the Upper Rhine Region.

Relating soil biochemistry to sustainable crop production

USDA-ARS?s Scientific Manuscript database

Amino acids, amino sugars, carbohydrates, phenols, and fatty acids together comprise appreciable proportions of soil organic matter (SOM). Their cycling contribute to soil processes, including nitrogen availability, carbon sequestration and aggregation. For example, soil accumulation of phenols has ...

Micro-PIV Study of Supercritical CO2-Water Interactions in Porous Micromodels

NASA Astrophysics Data System (ADS)

Kazemifar, Farzan; Blois, Gianluca; Christensen, Kenneth T.

2015-11-01

Multiphase flow of immiscible fluids in porous media is encountered in numerous natural systems and engineering applications such as enhanced oil recovery (EOR), and CO2 sequestration among others. Geological sequestration of CO2 in saline aquifers has emerged as a viable option for reducing CO2 emissions, and thus it has been the subject of numerous studies in recent years. A key objective is improving the accuracy of numerical models used for field-scale simulations by incorporation/better representation of the pore-scale flow physics. This necessitates experimental data for developing, testing and validating such models. We have studied drainage and imbibition processes in a homogeneous, two-dimensional porous micromodel with CO2 and water at reservoir-relevant conditions. Microscopic particle image velocimetry (micro-PIV) technique was applied to obtain spatially- and temporally-resolved velocity vector fields in the aqueous phase. The results provide new insight into the flow processes at the pore scale.

FULL SCALE BIOREACTOR LANDFILL FOR CARBON SEQUESTRATION AND GREENHOUSE EMISSION CONTROL

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ramin Yazdani; Jeff Kieffer; Heather Akau

2003-12-01

The Yolo County Department of Planning and Public Works is constructing a full-scale bioreactor landfill as a part of the Environmental Protection Agency's (EPA) Project XL program to develop innovative approaches for carbon sequestration and greenhouse emission control. The overall objective is to manage landfill solid waste for rapid waste decomposition and maximum landfill gas generation and capture for carbon sequestration and greenhouse emission control. Waste decomposition is accelerated by improving conditions for either the aerobic or anaerobic biological processes and involves circulating controlled quantities of liquid (leachate, groundwater, gray water, etc.), and, in the aerobic process, large volumes ofmore » air. The first phase of the project entails the construction of a 12-acre module that contains a 6-acre anaerobic cell, a 3.5-acre anaerobic cell, and a 2.5-acre aerobic cell at the Yolo County Central Landfill near Davis, California. The cells are highly instrumented to monitor bioreactor performance. Liquid addition has commenced in the 3.5-acre anaerobic cell and the 6-acre anaerobic cell. Construction of the 2.5-acre aerobic cell and biofilter has been completed. The remaining task to be completed is to test the biofilter prior to operation, which is currently anticipated to begin in January 2004. The current project status and preliminary monitoring results are summarized in this report.« less

The sequestration switch: removing industrial CO2 by direct ocean absorption.

PubMed

Ametistova, Lioudmila; Twidell, John; Briden, James

2002-04-22

This review paper considers direct injection of industrial CO2 emissions into the mid-water oceanic column below 500 m depth. Such a process is a potential candidate for switching atmospheric carbon emissions directly to long term sequestration, thereby relieving the intermediate atmospheric burden. Given sufficient research justification, the argument is that harmful impact in both the Atmosphere and the biologically rich upper marine layer could be reduced. The paper aims to estimate the role that active intervention, through direct ocean CO2 storage, could play and to outline further research and assessment for the strategy to be a viable option for climate change mitigation. The attractiveness of direct ocean injection lies in its bypassing of the Atmosphere and upper marine region, its relative permanence, its practicability using existing technologies and its quantification. The difficulties relate to the uncertainty of some fundamental scientific issues, such as plume dynamics, lowered pH of the exposed waters and associated ecological impact, the significant energy penalty associated with the necessary engineering plant and the uncertain costs. Moreover, there are considerable uncertainties regarding related international marine law. Development of the process would require acceptance of the evidence for climate change, strict requirements for large industrial consumers of fossil fuel to reduce CO2 emissions into the Atmosphere and scientific evidence for the overall beneficial impact of ocean sequestration.

Autophagy sequesters damaged lysosomes to control lysosomal biogenesis and kidney injury

PubMed Central

Maejima, Ikuko; Takahashi, Atsushi; Omori, Hiroko; Kimura, Tomonori; Takabatake, Yoshitsugu; Saitoh, Tatsuya; Yamamoto, Akitsugu; Hamasaki, Maho; Noda, Takeshi; Isaka, Yoshitaka; Yoshimori, Tamotsu

2013-01-01

Diverse causes, including pathogenic invasion or the uptake of mineral crystals such as silica and monosodium urate (MSU), threaten cells with lysosomal rupture, which can lead to oxidative stress, inflammation, and apoptosis or necrosis. Here, we demonstrate that lysosomes are selectively sequestered by autophagy, when damaged by MSU, silica, or the lysosomotropic reagent L-Leucyl-L-leucine methyl ester (LLOMe). Autophagic machinery is recruited only on damaged lysosomes, which are then engulfed by autophagosomes. In an autophagy-dependent manner, low pH and degradation capacity of damaged lysosomes are recovered. Under conditions of lysosomal damage, loss of autophagy causes inhibition of lysosomal biogenesis in vitro and deterioration of acute kidney injury in vivo. Thus, we propose that sequestration of damaged lysosomes by autophagy is indispensable for cellular and tissue homeostasis. PMID:23921551

Autophagy sequesters damaged lysosomes to control lysosomal biogenesis and kidney injury.

PubMed

Maejima, Ikuko; Takahashi, Atsushi; Omori, Hiroko; Kimura, Tomonori; Takabatake, Yoshitsugu; Saitoh, Tatsuya; Yamamoto, Akitsugu; Hamasaki, Maho; Noda, Takeshi; Isaka, Yoshitaka; Yoshimori, Tamotsu

2013-08-28

Diverse causes, including pathogenic invasion or the uptake of mineral crystals such as silica and monosodium urate (MSU), threaten cells with lysosomal rupture, which can lead to oxidative stress, inflammation, and apoptosis or necrosis. Here, we demonstrate that lysosomes are selectively sequestered by autophagy, when damaged by MSU, silica, or the lysosomotropic reagent L-Leucyl-L-leucine methyl ester (LLOMe). Autophagic machinery is recruited only on damaged lysosomes, which are then engulfed by autophagosomes. In an autophagy-dependent manner, low pH and degradation capacity of damaged lysosomes are recovered. Under conditions of lysosomal damage, loss of autophagy causes inhibition of lysosomal biogenesis in vitro and deterioration of acute kidney injury in vivo. Thus, we propose that sequestration of damaged lysosomes by autophagy is indispensable for cellular and tissue homeostasis.

On Subsurface Fracture Opening and Closure

NASA Astrophysics Data System (ADS)

Wang, Y.

2016-12-01

Mechanistic understanding of fracture opening and closure in geologic media is of significant importance to nature resource extraction and waste management, such as geothermal energy extraction, oil/gas production, radioactive waste disposal, and carbon sequestration and storage). A dynamic model for subsurface fracture opening and closure has been formulated. The model explicitly accounts for the stress concentration around individual aperture channels and the stress-activated mineral dissolution and precipitation. A preliminary model analysis has demonstrated the importance of the stress-activated dissolution mechanism in the evolution of fracture aperture in a stressed geologic medium. The model provides a reasonable explanation for some key features of fracture opening and closure observed in laboratory experiments, including a spontaneous switch from a net permeability reduction to a net permeability increase with no changes in a limestone fracture experiment.

Could Mars be dark and altered?

USGS Publications Warehouse

Calvin, Wendy M.

1998-01-01

There is a long known dichotomy in the martian albedo, with an associated, but mostly assumed, mineralogical split as well. The bright red regions are inferred to be weathered, oxidized dust and the dark grey regions unaltered volcanic material. A number of recent analyses suggest this division is unnaturally simplistic and the association of many dark regions with the former presence of water requires a re‐examination of the spectra in light of potential alteration minerals. I present an alternate interpretation of the reflectance spectral characteristics of some dark regions on Mars that includes dark layer silicates. If their presence is confirmed on Mars this will have implications for sequestration of current and past volatile inventories, clues to the extent and type of geochemical weathering, and potential zones where bacterial life forms may have emerged.

Increasing Alkalinity Export from Large Russian Arctic Rivers

NASA Astrophysics Data System (ADS)

Drake, T.; Zhulidov, A. V.; Gurtovaya, T. Y.; Spencer, R. G.

2017-12-01

Riverine carbonate alkalinity (HCO3- and CO32-) sourced from chemical weathering of minerals on land represents a significant sink for atmospheric CO2 over geologic timescales. The flux of alkalinity from rivers in the Arctic depends on precipitation, permafrost extent and thaw, groundwater flow paths, and surface vegetation, all of which are changing under a warming climate. Here we show that over the past four decades, the export of alkalinity from the Ob' and Yenisei Rivers has more than doubled. The increase is likely due to a combination of increasing precipitation and permafrost thaw in the watersheds, which lengthens hydrologic flow paths and increases residence time in soils. These trends have broad implications for the rate of carbon sequestration on land and the delivery of buffering capacity to the Arctic Ocean.

Biodegradation of PAHs and PCBs in soils and sludges

USGS Publications Warehouse

Liu, L.; Tindall, J.A.; Friedel, M.J.

2007-01-01

Results from a multi-year, pilot-scale land treatment project for PAHs and PCBs biodegradation were evaluated. A mathematical model, capable of describing sorption, sequestration, and biodegradation in soil/water systems, is applied to interpret the efficacy of a sequential active-passive biotreatment process of organic chemicals on remediation sites. To account for the recalcitrance of PAHs and PCBs in soils and sludges during long-term biotreatment, this model comprises a kinetic equation for organic chemical intraparticle sequestration process. Model responses were verified by comparison to measurements of biodegradation of PAHs and PCBs in land treatment units; a favorable match was found between them. Model simulations were performed to predict on-going biodegradation behavior of PAHs and PCBs in land treatment units. Simulation results indicate that complete biostabilization will be achieved when the concentration of reversibly sorbed chemical (S RA) reduces to undetectable levels, with a certain amount of irreversibly sequestrated residual chemical (S IA) remaining within the soil particle solid phase. The residual fraction (S IA) tends to lose its original chemical and biological activity, and hence, is much less available, toxic, and mobile than the "free" compounds. Therefore, little or no PAHs and PCBs will leach from the treatment site and constitutes no threat to human health or the environment. Biotreatment of PAHs and PCBs can be terminated accordingly. Results from the pilot-scale testing data and model calculations also suggest that a significant fraction (10-30%) of high-molecular-weight PAHs and PCBs could be sequestrated and become unavailable for biodegradation. Bioavailability (large K d , i.e., slow desorption rate) is the key factor limiting the PAHs degradation. However, both bioavailability and bioactivity (K in Monod kinetics, i.e., number of microbes, nutrients, and electron acceptor, etc.) regulate PCBs biodegradation. The sequential active-passive biotreatment can be a cost-effective approach for remediation of highly hydrophobic organic contaminants. The mathematical model proposed here would be useful in the design and operation of such organic chemical biodegradation processes on remediation sites. ?? 2007 Springer Science+Business Media B.V.

Integrity of Pre-existing Wellbores in Geological Sequestration of CO 2 – Assessment Using a Coupled Geomechanics-fluid Flow Model

DOE PAGES

Kelkar, Sharad; Carey, J. William; Dempsey, David; ...

2014-12-31

Assessment of potential CO 2 and brine leakage from wellbores is central to any consideration of the viability of geological CO 2 sequestration. Depleted oil and gas reservoirs are some of the potential candidates for consideration as sequestration sites. The sequestration sites are expected to cover laterally extensive areas to be of practical interest. Hence there is a high likelihood that such sites will contain many pre-existing abandoned wells. Most existing work on wellbore integrity has focused on field and laboratory studies of chemical reactivity. Very little work has been done on the impacts of mechanical stresses on wellbore performance.more » This study focuses on the potential enhancement of fluid flow pathways in the near-wellbore environment due to modifications in the geomechanical stress field resulting from the CO 2 injection operations. The majority of the operational scenarios for CO 2 sequestration lead to significant rise in the formation pore pressure. This is expected to lead to an expansion of the reservoir rock and build-up of shear stresses near wellbores where the existence of cement and casing are expected to constrain the expansion. If the stress buildup is large enough, this can lead to failure with attendant permeability enhancement that can potentially provide leakage pathways to shallower aquifers and the surface. In this study, we use a numerical model to simulate key features of a wellbore (casing, annulus and cement) embedded in a system that includes the upper aquifer, caprock, and storage aquifer. We present the sensitivity of damage initiation and propagation to various operational and formation parameters. We consider Mohr-Coulomb shear-failure models; tensile failure is also likely to occur but will require higher stress changes and will be preceded by shear failure. The modeling is performed using the numerical simulator FEHM developed at LANL that models coupled THM processes during multi-phase fluid flow and deformation in fractured porous media. FEHM has been developed extensively under projects on conventional/unconventional energy extraction (geothermal, oil, and gas), radionuclide and contaminant transport, watershed management, and CO 2 sequestration.« less

Site Development, Operations, and Closure Plan Topical Report 5 An Assessment of Geologic Carbon Sequestration Options in the Illinois Basin. Phase III

DOE Office of Scientific and Technical Information (OSTI.GOV)

Finley, Robert; Payne, William; Kirksey, Jim

2015-06-01

The Midwest Geological Sequestration Consortium (MGSC) has partnered with Archer Daniels Midland Company (ADM) and Schlumberger Carbon Services to conduct a large-volume, saline reservoir storage project at ADM’s agricultural products processing complex in Decatur, Illinois. The Development Phase project, named the Illinois Basin Decatur Project (IBDP) involves the injection of 1 million tonnes of carbon dioxide (CO 2) into a deep saline formation of the Illinois Basin over a three-year period. This report focuses on objectives, execution, and lessons learned/unanticipated results from the site development (relating specifically to surface equipment), operations, and the site closure plan.

Experimental Study of Porosity Changes in Shale Caprocks Exposed to Carbon Dioxide-Saturated Brine II: Insights from Aqueous Geochemistry

DOE PAGES

Miller, Quin R. S.; Wang, Xiuyu; Kaszuba, John P.; ...

2016-07-18

Laboratory experiments evaluated two shale caprock formations, the Gothic Shale and Marine Tuscaloosa Formation, at conditions relevant to carbon dioxide (CO 2) sequestration. Both rocks were exposed to CO 2-saturated brines at 160°C and 15 MPa for ~45 days. Baseline experiments for both rocks were pressurized with argon to 15 MPa for ~35 days. Varying concentrations of iron, aqueous silica, sulfate, and initial pH decreases coincide with enhanced carbonate and silicate dissolution due to reaction between CO 2-saturated brine and shale. Saturation indices were calculated and activity diagrams were constructed to gain insights into sulfate, silicate, and carbonate mineral stabilities.more » We found that upon exposure to CO 2-saturated brines, the Marine Tuscaloosa Formation appeared to be more reactive than the Gothic Shale. Evolution of aqueous geochemistry in the experiments is consistent with mineral precipitation and dissolution reactions that affect porosity. Finally, this study highlights the importance of tracking fluid chemistry to clarify downhole physicochemical responses to CO 2 injection and subsequent changes in sealing capacity in CO 2 storage and utilization projects.« less

Evaporite Caprock Integrity. An experimental study of reactive mineralogy and pore-scale heterogeneity during brine-CO 2 exposure

DOE PAGES

Smith, Megan M.; Sholokhova, Yelena; Hao, Yue; ...

2012-07-25

Characterization and geochemical data are presented from a core-flooding experiment on a sample from the Three Fingers evaporite unit forming the lower extent of caprock at the Weyburn-Midale reservoir, Canada. This low-permeability sample was characterized in detail using X-ray computed microtomography before and after exposure to CO 2-acidified brine, allowing mineral phase and voidspace distributions to be quantified in three dimensions. Solution chemistry indicated that CO 2-acidified brine preferentially dissolved dolomite until saturation was attained, while anhydrite remained unreactive. Dolomite dissolution contributed to increases in bulk permeability through the formation of a localized channel, guided by microfractures as well asmore » porosity and reactive phase distributions aligned with depositional bedding. An indirect effect of carbonate mineral reactivity with CO 2-acidified solution is voidspace generation through physical transport of anhydrite freed from the rock matrix following dissolution of dolomite. The development of high permeability fast pathways in this experiment highlights the role of carbonate content and potential fracture orientations in evaporite caprock formations considered for both geologic carbon sequestration and CO 2-enhanced oil recovery operations.« less

Mineralisation of reconstituted collagen using polyvinylphosphonic acid/polyacrylic acid templating matrix protein analogues in the presence of calcium, phosphate and hydroxyl ions

PubMed Central

Kim, Young Kyung; Gu, Li-sha; Bryan, Thomas E.; Kim, Jong Ryul; Chen, Liang; Liu, Yan; Yoon, James C.; Breschi, Lorenzo; Pashley, David H.; Tay, Franklin R.

2010-01-01

The complex morphologies of mineralised collagen fibrils are regulated through interactions between the collagen matrix and non-collagenous extracellular proteins. In the present study, polyvinylphosphonic acid, a biomimetic analogue of matrix phosphoproteins, was synthesised and confirmed with FTIR and NMR. Biomimetic mineralisation of reconstituted collagen fibrils devoid of natural non-collagenous proteins was demonstrated with TEM using a Portland cement-containing resin composite and a phosphate-containing fluid in the presence of polyacrylic acid as sequestration, and polyvinylphosphonic acid as templating matrix protein analogues. In the presence of these dual biomimetic analogues in the mineralisation medium, intrafibrillar and extrafibrillar mineralisation via bottom-up nanoparticle assembly based on the nonclassical crystallisation pathway could be identified. Conversely, only large mineral spheres with no preferred association with collagen fibrils were observed in the absence of biomimetic analogues in the medium. Mineral phases were evident within the collagen fibrils as early as 4 hours after the initially-formed amorphous calcium phosphate nanoprecursors were transformed into apatite nanocrystals. Selected area electron diffraction patterns of highly mineralised collagen fibrils were nearly identical to those of natural bone, with apatite crystallites preferentially aligned along the collagen fibril axes. PMID:20621767