Basin-Scale Hydrologic Impacts of CO2 Storage: Regulatory and Capacity Implications
DOE Office of Scientific and Technical Information (OSTI.GOV)
Birkholzer, J.T.; Zhou, Q.
Industrial-scale injection of CO{sub 2} into saline sedimentary basins will cause large-scale fluid pressurization and migration of native brines, which may affect valuable groundwater resources overlying the deep sequestration reservoirs. In this paper, we discuss how such basin-scale hydrologic impacts can (1) affect regulation of CO{sub 2} storage projects and (2) may reduce current storage capacity estimates. Our assessment arises from a hypothetical future carbon sequestration scenario in the Illinois Basin, which involves twenty individual CO{sub 2} storage projects in a core injection area suitable for long-term storage. Each project is assumed to inject five million tonnes of CO{sub 2}more » per year for 50 years. A regional-scale three-dimensional simulation model was developed for the Illinois Basin that captures both the local-scale CO{sub 2}-brine flow processes and the large-scale groundwater flow patterns in response to CO{sub 2} storage. The far-field pressure buildup predicted for this selected sequestration scenario suggests that (1) the area that needs to be characterized in a permitting process may comprise a very large region within the basin if reservoir pressurization is considered, and (2) permits cannot be granted on a single-site basis alone because the near- and far-field hydrologic response may be affected by interference between individual sites. Our results also support recent studies in that environmental concerns related to near-field and far-field pressure buildup may be a limiting factor on CO{sub 2} storage capacity. In other words, estimates of storage capacity, if solely based on the effective pore volume available for safe trapping of CO{sub 2}, may have to be revised based on assessments of pressure perturbations and their potential impact on caprock integrity and groundwater resources, respectively. We finally discuss some of the challenges in making reliable predictions of large-scale hydrologic impacts related to CO{sub 2} sequestration projects.« less
The imprint of surface fluxes and transport on variations in total column carbon dioxide
NASA Astrophysics Data System (ADS)
Keppel-Aleks, G.; Wennberg, P. O.; Washenfelder, R. A.; Wunch, D.; Schneider, T.; Toon, G. C.; Andres, R. J.; Blavier, J.-F.; Connor, B.; Davis, K. J.; Desai, A. R.; Messerschmidt, J.; Notholt, J.; Roehl, C. M.; Sherlock, V.; Stephens, B. B.; Vay, S. A.; Wofsy, S. C.
2011-07-01
New observations of the vertically integrated CO2 mixing ratio, ⟨CO2⟩, from ground-based remote sensing show that variations in ⟨CO2⟩ are primarily determined by large-scale flux patterns. They therefore provide fundamentally different information than observations made within the boundary layer, which reflect the combined influence of large scale and local fluxes. Observations of both ⟨CO2⟩ and CO2 concentrations in the free troposphere show that large-scale spatial gradients induce synoptic-scale temporal variations in ⟨CO2⟩ in the Northern Hemisphere midlatitudes through horizontal advection. Rather than obscure the signature of surface fluxes on atmospheric CO2, these synoptic-scale variations provide useful information that can be used to reveal the meridional flux distribution. We estimate the meridional gradient in ⟨CO2⟩ from covariations in ⟨CO2⟩ and potential temperature, θ, a dynamical tracer, on synoptic timescales to evaluate surface flux estimates commonly used in carbon cycle models. We find that Carnegie Ames Stanford Approach (CASA) biospheric fluxes underestimate both the ⟨CO2⟩ seasonal cycle amplitude throughout the Northern Hemisphere midlatitudes as well as the meridional gradient during the growing season. Simulations using CASA net ecosystem exchange (NEE) with increased and phase-shifted boreal fluxes better reflect the observations. Our simulations suggest that boreal growing season NEE (between 45-65° N) is underestimated by ~40 % in CASA. We describe the implications for this large seasonal exchange on inference of the net Northern Hemisphere terrestrial carbon sink.
The imprint of surface fluxes and transport on variations in total column carbon dioxide
DOE Office of Scientific and Technical Information (OSTI.GOV)
Keppel-Aleks, G; Wennberg, PO; Washenfelder, RA
2012-01-01
New observations of the vertically integrated CO{sub 2} mixing ratio,
The imprint of surface fluxes and transport on variations in total column carbon dioxide
NASA Astrophysics Data System (ADS)
Keppel-Aleks, G.; Wennberg, P. O.; Washenfelder, R. A.; Wunch, D.; Schneider, T.; Toon, G. C.; Andres, R. J.; Blavier, J.-F.; Connor, B.; Davis, K. J.; Desai, A. R.; Messerschmidt, J.; Notholt, J.; Roehl, C. M.; Sherlock, V.; Stephens, B. B.; Vay, S. A.; Wofsy, S. C.
2012-03-01
New observations of the vertically integrated CO2 mixing ratio, ⟨CO2⟩, from ground-based remote sensing show that variations in CO2⟩ are primarily determined by large-scale flux patterns. They therefore provide fundamentally different information than observations made within the boundary layer, which reflect the combined influence of large-scale and local fluxes. Observations of both ⟨CO2⟩ and CO2 concentrations in the free troposphere show that large-scale spatial gradients induce synoptic-scale temporal variations in ⟨CO2⟩ in the Northern Hemisphere midlatitudes through horizontal advection. Rather than obscure the signature of surface fluxes on atmospheric CO2, these synoptic-scale variations provide useful information that can be used to reveal the meridional flux distribution. We estimate the meridional gradient in ⟨CO2⟩ from covariations in ⟨CO2⟩ and potential temperature, θ, a dynamical tracer, on synoptic timescales to evaluate surface flux estimates commonly used in carbon cycle models. We find that simulations using Carnegie Ames Stanford Approach (CASA) biospheric fluxes underestimate both the ⟨CO2⟩ seasonal cycle amplitude throughout the Northern Hemisphere midlatitudes and the meridional gradient during the growing season. Simulations using CASA net ecosystem exchange (NEE) with increased and phase-shifted boreal fluxes better fit the observations. Our simulations suggest that climatological mean CASA fluxes underestimate boreal growing season NEE (between 45-65° N) by ~40%. We describe the implications for this large seasonal exchange on inference of the net Northern Hemisphere terrestrial carbon sink.
Using radiocarbon to investigate soil respiration impacts on atmospheric CO2
NASA Astrophysics Data System (ADS)
Phillips, C. L.; LaFranchi, B. W.; McFarlane, K. J.; Desai, A. R.
2013-12-01
While soil respiration is believed to represent the largest single source of CO2 emissions on a global scale, there are few tools available to measure soil emissions at large spatial scales. We investigated whether radiocarbon (14C) abundance in CO2 could be used to detect and characterize soil emissions in the atmosphere, taking advantage of the fact that 14C abundance in soil carbon is elevated compared to the background atmosphere, a result of thermonuclear weapons testing during the mid-20th Century (i.e. bomb-C). Working in a temperate hardwood forest in Northern Wisconsin during 2011-12, we made semi-high-frequency measurements of CO2 at nested spatial scales from the soil subsurface to 150 m above ground level. These measurements were used to investigate seasonal patterns in respired C sources, and to evaluate whether variability in soil-respired Δ14C could also be detected in atmospheric measurements. In our ground-level measurements we found large seasonal variation in soil-respired 14CO2 that correlated with soil moisture, which was likely related to root activity. Atmospheric measurements of 14CO2 in the forest canopy (2 to 30m) were used to construct Keeling plots, and these provided larger spatial-scale estimates of respired 14CO2 that largely agreed with the soil-level measurements. In collaboration with the NOAA we also examined temporal patterns of 14CO2 at the Park Falls tall-tower (150m), and found elevated 14CO2 levels during summer months that likely resulted from increased respiration from heterotrophic sources. These results demonstrate that a fingerprint from soil-respired CO2 can be detected in the seasonal patterns of atmospheric 14CO2, even at a regionally-integrating spatial scale far from the soil surface.
Subsurface Monitoring of CO2 Sequestration - A Review and Look Forward
NASA Astrophysics Data System (ADS)
Daley, T. M.
2012-12-01
The injection of CO2 into subsurface formations is at least 50 years old with large-scale utilization of CO2 for enhanced oil recovery (CO2-EOR) beginning in the 1970s. Early monitoring efforts had limited measurements in available boreholes. With growing interest in CO2 sequestration beginning in the 1990's, along with growth in geophysical reservoir monitoring, small to mid-size sequestration monitoring projects began to appear. The overall goals of a subsurface monitoring plan are to provide measurement of CO2 induced changes in subsurface properties at a range of spatial and temporal scales. The range of spatial scales allows tracking of the location and saturation of the plume with varying detail, while finer temporal sampling (up to continuous) allows better understanding of dynamic processes (e.g. multi-phase flow) and constraining of reservoir models. Early monitoring of small scale pilots associated with CO2-EOR (e.g., the McElroy field and the Lost Hills field), developed many of the methodologies including tomographic imaging and multi-physics measurements. Large (reservoir) scale sequestration monitoring began with the Sleipner and Weyburn projects. Typically, large scale monitoring, such as 4D surface seismic, has limited temporal sampling due to costs. Smaller scale pilots can allow more frequent measurements as either individual time-lapse 'snapshots' or as continuous monitoring. Pilot monitoring examples include the Frio, Nagaoka and Otway pilots using repeated well logging, crosswell imaging, vertical seismic profiles and CASSM (continuous active-source seismic monitoring). For saline reservoir sequestration projects, there is typically integration of characterization and monitoring, since the sites are not pre-characterized resource developments (oil or gas), which reinforces the need for multi-scale measurements. As we move beyond pilot sites, we need to quantify CO2 plume and reservoir properties (e.g. pressure) over large scales, while still obtaining high resolution. Typically the high-resolution (spatial and temporal) tools are deployed in permanent or semi-permanent borehole installations, where special well design may be necessary, such as non-conductive casing for electrical surveys. Effective utilization of monitoring wells requires an approach of modular borehole monitoring (MBM) were multiple measurements can be made. An example is recent work at the Citronelle pilot injection site where an MBM package with seismic, fluid sampling and distributed fiber sensing was deployed. For future large scale sequestration monitoring, an adaptive borehole-monitoring program is proposed.
Middleton, Richard S.; Levine, Jonathan S.; Bielicki, Jeffrey M.; ...
2015-04-27
CO 2 capture, utilization, and storage (CCUS) technology has yet to be widely deployed at a commercial scale despite multiple high-profile demonstration projects. We suggest that developing a large-scale, visible, and financially viable CCUS network could potentially overcome many barriers to deployment and jumpstart commercial-scale CCUS. To date, substantial effort has focused on technology development to reduce the costs of CO 2 capture from coal-fired power plants. Here, we propose that near-term investment could focus on implementing CO 2 capture on facilities that produce high-value chemicals/products. These facilities can absorb the expected impact of the marginal increase in the costmore » of production on the price of their product, due to the addition of CO 2 capture, more than coal-fired power plants. A financially viable demonstration of a large-scale CCUS network requires offsetting the costs of CO 2 capture by using the CO 2 as an input to the production of market-viable products. As a result, we demonstrate this alternative development path with the example of an integrated CCUS system where CO 2 is captured from ethylene producers and used for enhanced oil recovery in the U.S. Gulf Coast region.« less
A Commercialization Roadmap for Carbon-Negative Energy Systems
NASA Astrophysics Data System (ADS)
Sanchez, D.
2016-12-01
The Intergovernmental Panel on Climate Change (IPCC) envisages the need for large-scale deployment of net-negative CO2 emissions technologies by mid-century to meet stringent climate mitigation goals and yield a net drawdown of atmospheric carbon. Yet there are few commercial deployments of BECCS outside of niche markets, creating uncertainty about commercialization pathways and sustainability impacts at scale. This uncertainty is exacerbated by the absence of a strong policy framework, such as high carbon prices and research coordination. Here, we propose a strategy for the potential commercial deployment of BECCS. This roadmap proceeds via three steps: 1) via capture and utilization of biogenic CO2 from existing bioenergy facilities, notably ethanol fermentation, 2) via thermochemical co-conversion of biomass and fossil fuels, particularly coal, and 3) via dedicated, large-scale BECCS. Although biochemical conversion is a proven first market for BECCS, this trajectory alone is unlikely to drive commercialization of BECCS at the gigatonne scale. In contrast to biochemical conversion, thermochemical conversion of coal and biomass enables large-scale production of fuels and electricity with a wide range of carbon intensities, process efficiencies and process scales. Aside from systems integration, primarily technical barriers are involved in large-scale biomass logistics, gasification and gas cleaning. Key uncertainties around large-scale BECCS deployment are not limited to commercialization pathways; rather, they include physical constraints on biomass cultivation or CO2 storage, as well as social barriers, including public acceptance of new technologies and conceptions of renewable and fossil energy, which co-conversion systems confound. Despite sustainability risks, this commercialization strategy presents a pathway where energy suppliers, manufacturers and governments could transition from laggards to leaders in climate change mitigation efforts.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Middleton, Richard S.; Levine, Jonathan S.; Bielicki, Jeffrey M.
CO 2 capture, utilization, and storage (CCUS) technology has yet to be widely deployed at a commercial scale despite multiple high-profile demonstration projects. We suggest that developing a large-scale, visible, and financially viable CCUS network could potentially overcome many barriers to deployment and jumpstart commercial-scale CCUS. To date, substantial effort has focused on technology development to reduce the costs of CO 2 capture from coal-fired power plants. Here, we propose that near-term investment could focus on implementing CO 2 capture on facilities that produce high-value chemicals/products. These facilities can absorb the expected impact of the marginal increase in the costmore » of production on the price of their product, due to the addition of CO 2 capture, more than coal-fired power plants. A financially viable demonstration of a large-scale CCUS network requires offsetting the costs of CO 2 capture by using the CO 2 as an input to the production of market-viable products. As a result, we demonstrate this alternative development path with the example of an integrated CCUS system where CO 2 is captured from ethylene producers and used for enhanced oil recovery in the U.S. Gulf Coast region.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Frailey, Scott M.; Krapac, Ivan G.; Damico, James R.
2012-03-30
The Midwest Geological Sequestration Consortium (MGSC) carried out a small-scale carbon dioxide (CO 2) injection test in a sandstone within the Clore Formation (Mississippian System, Chesterian Series) in order to gauge the large-scale CO 2 storage that might be realized from enhanced oil recovery (EOR) of mature Illinois Basin oil fields via miscible liquid CO 2 flooding.
Diego A. Riveros-Iregui; Brian L. McGlynn; Howard E. Epstein; Daniel L. Welsch
2008-01-01
Soil CO2 efflux is a large respiratory flux from terrestrial ecosystems and a critical component of the global carbon (C) cycle. Lack of process understanding of the spatiotemporal controls on soil CO2 efflux limits our ability to extrapolate from fluxes measured at point scales to scales useful for corroboration with other ecosystem level measures of C exchange....
Pore-scale supercritical CO2 dissolution and mass transfer under imbibition conditions
DOE Office of Scientific and Technical Information (OSTI.GOV)
Chang, Chun; Zhou, Quanlin; Kneafsey, Timothy J.
2016-06-01
In modeling of geological carbon storage, dissolution of supercritical CO2 (scCO2) is often assumed to be instantaneous with equilibrium phase partitioning. In contrast, recent core-scale imbibition experiments have shown a prolonged depletion of residual scCO2 by dissolution, implying a non-equilibrium mechanism. In this study, eight pore-scale scCO2 dissolution experiments in a 2D heterogeneous, sandstone-analogue micromodel were conducted at supercritical conditions (9 MPa and 40 °C). The micromodel was first saturated with deionized (DI) water and drained by injecting scCO2 to establish a stable scCO2 saturation. DI water was then injected at constant flow rates after scCO2 drainage was completed. Highmore » resolution time-lapse images of scCO2 and water distributions were obtained during imbibition and dissolution, aided by a scCO2-soluble fluorescent dye introduced with scCO2 during drainage. These images were used to estimate scCO2 saturations and scCO2 depletion rates. Experimental results show that (1) a time-independent, varying number of water-flow channels are created during imbibition and later dominant dissolution by the random nature of water flow at the micromodel inlet, and (2) a time-dependent number of water-flow channels are created by coupled imbibition and dissolution following completion of dominant imbibition. The number of water-flow paths, constant or transient in nature, greatly affects the overall depletion rate of scCO2 by dissolution. The average mass fraction of dissolved CO2 (dsCO2) in water effluent varies from 0.38% to 2.72% of CO2 solubility, indicating non-equilibrium scCO2 dissolution in the millimeter-scale pore network. In general, the transient depletion rate decreases as trapped, discontinuous scCO2 bubbles and clusters within water-flow paths dissolve, then remains low with dissolution of large bypassed scCO2 clusters at their interfaces with longitudinal water flow, and finally increases with coupled transverse water flow and enhanced dissolution of large scCO2 clusters. The three stages of scCO2 depletion, common to experiments with time-independent water-flow paths, are revealed by zoom-in image analysis of individual scCO2 bubbles and clusters. The measured relative permeability of water, affected by scCO2 dissolution and bi-modal permeability, shows a non-monotonic dependence on saturation. The results for experiments with different injection rates imply that the non-equilibrium nature of scCO2 dissolution becomes less important when water flow is relatively low and the time scale for dissolution is large, and more pronounced when heterogeneity is strong.« less
Porosoff, Marc D.; Yan, Binhang; Chen, Jingguang G.
2015-10-22
Ocean acidification and climate change are expected to be two of the most difficult scientific challenges of the 21st century. Converting CO 2 into valuable chemicals and fuels is one of the most practical routes for reducing CO 2 emissions while fossil fuels continue to dominate the energy sector. Reducing CO 2 by H 2 using heterogeneous catalysis has been studied extensively, but there are still significant challenges in developing active, selective and stable catalysts suitable for large-scale commercialization. We study the catalytic reduction of CO 2 by H 2 can lead to the formation of three types of products:more » CO through the reverse water–gas shift (RWGS) reaction, methanol via selective hydrogenation, and hydrocarbons through combination of CO 2 reduction with Fischer–Tropsch (FT) reactions. In addition, investigations into these routes reveal that the stabilization of key reaction intermediates is critically important for controlling catalytic selectivity. Furthermore, viability of these processes is contingent on the development of a CO 2-free H 2 source on a large enough scale to significantly reduce CO 2 emissions.« less
On the Role of Multi-Scale Processes in CO2 Storage Security and Integrity
NASA Astrophysics Data System (ADS)
Pruess, K.; Kneafsey, T. J.
2008-12-01
Consideration of multiple scales in subsurface processes is usually referred to the spatial domain, where we may attempt to relate process descriptions and parameters from pore and bench (Darcy) scale to much larger field and regional scales. However, multiple scales occur also in the time domain, and processes extending over a broad range of time scales may be very relevant to CO2 storage and containment. In some cases, such as in the convective instability induced by CO2 dissolution in saline waters, space and time scales are coupled in the sense that perturbations induced by CO2 injection will grow concurrently over many orders of magnitude in both space and time. In other cases, CO2 injection may induce processes that occur on short time scales, yet may affect large regions. Possible examples include seismicity that may be triggered by CO2 injection, or hypothetical release events such as "pneumatic eruptions" that may discharge substantial amounts of CO2 over a short time period. This paper will present recent advances in our experimental and modeling studies of multi-scale processes. Specific examples that will be discussed include (1) the process of CO2 dissolution-diffusion-convection (DDC), that can greatly accelerate the rate at which free-phase CO2 is stored as aqueous solute; (2) self- enhancing and self-limiting processes during CO2 leakage through faults, fractures, or improperly abandoned wells; and (3) porosity and permeability reduction from salt precipitation near CO2 injection wells, and mitigation of corresponding injectivity loss. This work was supported by the Office of Basic Energy Sciences and by the Zero Emission Research and Technology project (ZERT) under Contract No. DE-AC02-05CH11231 with the U.S. Department of Energy.
Paul S Wills, PhD; Pfeiffer, Timothy; Baptiste, Richard; Watten, Barnaby J.
2016-01-01
Control of alkalinity, dissolved carbon dioxide (dCO2), and pH are critical in marine recirculating aquaculture systems (RAS) in order to maintain health and maximize growth. A small-scale prototype aragonite sand filled fluidized bed reactor was tested under varying conditions of alkalinity and dCO2 to develop and model the response of dCO2 across the reactor. A large-scale reactor was then incorporated into an operating marine recirculating aquaculture system to observe the reactor as the system moved toward equilibrium. The relationship between alkalinity dCO2, and pH across the reactor are described by multiple regression equations. The change in dCO2 across the small-scale reactor indicated a strong likelihood that an equilibrium alkalinity would be maintained by using a fluidized bed aragonite reactor. The large-scale reactor verified this observation and established equilibrium at an alkalinity of approximately 135 mg/L as CaCO3, dCO2 of 9 mg/L, and a pH of 7.0 within 4 days that was stable during a 14 day test period. The fluidized bed aragonite reactor has the potential to simplify alkalinity and pH control, and aid in dCO2 control in RAS design and operation. Aragonite sand, purchased in bulk, is less expensive than sodium bicarbonate and could reduce overall operating production costs.
NASA Astrophysics Data System (ADS)
Li, Y.; Kazemifar, F.; Blois, G.; Christensen, K. T.
2017-12-01
Geological sequestration of CO2 within saline aquifers is a viable technology for reducing CO2 emissions. Central to this goal is accurately predicting both the fidelity of candidate sites pre-injection of CO2 and its post-injection migration. Moreover, local fluid pressure buildup may cause activation of small pre-existing unidentified faults, leading to micro-seismic events, which could prove disastrous for societal acceptance of CCS, and possibly compromise seal integrity. Recent evidence shows that large-scale events are coupled with pore-scale phenomena, which necessitates the representation of pore-scale stress, strain, and multiphase flow processes in large-scale modeling. To this end, the pore-scale flow of water and liquid/supercritical CO2 is investigated under reservoir-relevant conditions, over a range of wettability conditions in 2D heterogeneous micromodels that reflect the complexity of a real sandstone. High-speed fluorescent microscopy, complemented by a fast differential pressure transmitter, allows for simultaneous measurement of the flow field within and the instantaneous pressure drop across the micromodels. A flexible micromodel is also designed and fabricated, to be used in conjunction with the micro-PIV technique, enabling the quantification of coupled solid-liquid interactions.
NASA Astrophysics Data System (ADS)
Heimann, M.; Prentice, I. C.; Foley, J.; Hickler, T.; Kicklighter, D. W.; McGuire, A. D.; Melillo, J. M.; Ramankutty, N.; Sitch, S.
2001-12-01
Models of biophysical and biogeochemical proceses are being used -either offline or in coupled climate-carbon cycle (C4) models-to assess climate- and CO2-induced feedbacks on atmospheric CO2. Observations of atmospheric CO2 concentration, and supplementary tracers including O2 concentrations and isotopes, offer unique opportunities to evaluate the large-scale behaviour of models. Global patterns, temporal trends, and interannual variability of the atmospheric CO2 concentration and its seasonal cycle provide crucial benchmarks for simulations of regionally-integrated net ecosystem exchange; flux measurements by eddy correlation allow a far more demanding model test at the ecosystem scale than conventional indicators, such as measurements of annual net primary production; and large-scale manipulations, such as the Duke Forest Free Air Carbon Enrichment (FACE) experiment, give a standard to evaluate modelled phenomena such as ecosystem-level CO2 fertilization. Model runs including historical changes of CO2, climate and land use allow comparison with regional-scale monthly CO2 balances as inferred from atmospheric measurements. Such comparisons are providing grounds for some confidence in current models, while pointing to processes that may still be inadequately treated. Current plans focus on (1) continued benchmarking of land process models against flux measurements across ecosystems and experimental findings on the ecosystem-level effects of enhanced CO2, reactive N inputs and temperature; (2) improved representation of land use, forest management and crop metabolism in models; and (3) a strategy for the evaluation of C4 models in a historical observational context.
CO2 deserts: implications of existing CO2 supply limitations for carbon management.
Middleton, Richard S; Clarens, Andres F; Liu, Xiaowei; Bielicki, Jeffrey M; Levine, Jonathan S
2014-10-07
Efforts to mitigate the impacts of climate change will require deep reductions in anthropogenic CO2 emissions on the scale of gigatonnes per year. CO2 capture and utilization and/or storage technologies are a class of approaches that can substantially reduce CO2 emissions. Even though examples of this approach, such as CO2-enhanced oil recovery, are already being practiced on a scale >0.05 Gt/year, little attention has been focused on the supply of CO2 for these projects. Here, facility-scale data newly collected by the U.S. Environmental Protection Agency was processed to produce the first comprehensive map of CO2 sources from industrial sectors currently supplying CO2 in the United States. Collectively these sources produce 0.16 Gt/year, but the data reveal the presence of large areas without access to CO2 at an industrially relevant scale (>25 kt/year). Even though some facilities with the capability to capture CO2 are not doing so and in some regions pipeline networks are being built to link CO2 sources and sinks, much of the country exists in "CO2 deserts". A life cycle analysis of the sources reveals that the predominant source of CO2, dedicated wells, has the largest carbon footprint further confounding prospects for rational carbon management strategies.
Pore-scale simulation of CO2-water-rock interactions
NASA Astrophysics Data System (ADS)
Deng, H.; Molins, S.; Steefel, C. I.; DePaolo, D. J.
2017-12-01
In Geologic Carbon Storage (GCS) systems, the migration of scCO2 versus CO2-acidifed brine ultimately determines the extent of mineral trapping and caprock integrity, i.e. the long-term storage efficiency and security. While continuum scale multiphase reactive transport models are valuable for large scale investigations, they typically (over-)simplify pore-scale dynamics and cannot capture local heterogeneities that may be important. Therefore, pore-scale models are needed in order to provide mechanistic understanding of how fine scale structural variations and heterogeneous processes influence the transport and geochemistry in the context of multiphase flow, and to inform parameterization of continuum scale modeling. In this study, we investigate the interplay of different processes at pore scale (e.g. diffusion, reactions, and multiphase flow) through the coupling of a well-developed multiphase flow simulator with a sophisticated reactive transport code. The objectives are to understand where brine displaced by scCO2 will reside in a rough pore/fracture, and how the CO2-water-rock interactions may affect the redistribution of different phases. In addition, the coupled code will provide a platform for model testing in pore-scale multiphase reactive transport problems.
Goodman, Angela; Sanguinito, Sean; Levine, Jonathan S.
2016-09-28
Carbon storage resource estimation in subsurface saline formations plays an important role in establishing the scale of carbon capture and storage activities for governmental policy and commercial project decision-making. Prospective CO 2 resource estimation of large regions or subregions, such as a basin, occurs at the initial screening stages of a project using only limited publicly available geophysical data, i.e. prior to project-specific site selection data generation. As the scale of investigation is narrowed and selected areas and formations are identified, prospective CO 2 resource estimation can be refined and uncertainty narrowed when site-specific geophysical data are available. Here, wemore » refine the United States Department of Energy – National Energy Technology Laboratory (US-DOE-NETL) methodology as the scale of investigation is narrowed from very large regional assessments down to selected areas and formations that may be developed for commercial storage. In addition, we present a new notation that explicitly identifies differences between data availability and data sources used for geologic parameters and efficiency factors as the scale of investigation is narrowed. This CO 2 resource estimation method is available for screening formations in a tool called CO 2-SCREEN.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Goodman, Angela; Sanguinito, Sean; Levine, Jonathan S.
Carbon storage resource estimation in subsurface saline formations plays an important role in establishing the scale of carbon capture and storage activities for governmental policy and commercial project decision-making. Prospective CO 2 resource estimation of large regions or subregions, such as a basin, occurs at the initial screening stages of a project using only limited publicly available geophysical data, i.e. prior to project-specific site selection data generation. As the scale of investigation is narrowed and selected areas and formations are identified, prospective CO 2 resource estimation can be refined and uncertainty narrowed when site-specific geophysical data are available. Here, wemore » refine the United States Department of Energy – National Energy Technology Laboratory (US-DOE-NETL) methodology as the scale of investigation is narrowed from very large regional assessments down to selected areas and formations that may be developed for commercial storage. In addition, we present a new notation that explicitly identifies differences between data availability and data sources used for geologic parameters and efficiency factors as the scale of investigation is narrowed. This CO 2 resource estimation method is available for screening formations in a tool called CO 2-SCREEN.« less
NASA Astrophysics Data System (ADS)
Hua, Wei-Bo; Guo, Xiao-Dong; Zheng, Zhuo; Wang, Yan-Jie; Zhong, Ben-He; Fang, Baizeng; Wang, Jia-Zhao; Chou, Shu-Lei; Liu, Heng
2015-02-01
Developing advanced electrode materials that deliver high energy at ultra-fast charge and discharge rates are very crucial to meet an increasing large-scale market demand for high power lithium ion batteries (LIBs). A three-dimensional (3D) nanoflower structure is successfully developed in the large-scale synthesis of LiNi1/3Co1/3Mn1/3O2 material for the first time. The fast co-precipitation is the key technique to prepare the nanoflower structure in our method. After heat treatment, the obtained LiNi1/3Co1/3Mn1/3O2 nanoflowers (NL333) pronouncedly present a pristine flower-like nano-architecture and provide fast pathways for the transport of Li-ions and electrons. As a cathode material in a LIB, the prepared NL333 electrode demonstrates an outstanding high-rate capability. Particularly, in a narrow voltage range of 2.7-4.3 V, the discharge capacity at an ultra-fast charge-discharge rate (20C) is up to 126 mAh g-1, which reaches 78% of that at 0.2C, and is much higher than that (i.e., 44.17%) of the traditional bulk LiNi1/3Co1/3Mn1/3O2.
Bioinspired Wood Nanotechnology for Functional Materials.
Berglund, Lars A; Burgert, Ingo
2018-05-01
It is a challenging task to realize the vision of hierarchically structured nanomaterials for large-scale applications. Herein, the biomaterial wood as a large-scale biotemplate for functionalization at multiple scales is discussed, to provide an increased property range to this renewable and CO 2 -storing bioresource, which is available at low cost and in large quantities. The Progress Report reviews the emerging field of functional wood materials in view of the specific features of the structural template and novel nanotechnological approaches for the development of wood-polymer composites and wood-mineral hybrids for advanced property profiles and new functions. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
NASA Astrophysics Data System (ADS)
Heeschen, Katja U.; Spangenberg, Erik; Schicks, Judith M.; Deusner, Christian; Priegnitz, Mike; Strauch, Bettina; Bigalke, Nikolaus; Luzi-Helbing, Manja; Kossel, Elke; Haeckel, Matthias; Wang, Yi
2017-04-01
Methane (CH4) hydrates are considered as a player in the field of energy supply and - if applied as such - as a possible sink for the greenhouse gas carbon dioxide (CO2). Next to the more conventional production methods depressurization and thermal stimulation, an extraction of CH4 by means of CO2 injection is investigated. The method is based on the chemical potential gradient between the CH4 hydrate phase and the injected CO2 phase. Results from small-scale laboratory experiments on the replacement method indicate recovery ratios of up to 66% CH4 but also encounter major discrepancies in conversion rates. So far it has not been demonstrated with certainty that the process rates are sufficient for an energy and cost effective production of CH4 with a concurrent sequestration of CO2. In a co-operation of GFZ and GEOMAR we used LARS (Large Scale Reservoir Simulator) to investigate the CO2-CH4-replacement method combined with thermal stimulation. LARS accommodates a sample volume of 210 l and allows for the simulation of in situ conditions typically found in gas hydrate reservoirs. Based on the sample size, diverse transport mechanisms could be simulated, which are assumed to significantly alter process yields. Temperature and pressure data complemented by a high resolution electrical resistivity tomography (ERT), gas chromatography, and flow measurements serve to interpret the experiments. In two experiments 50 kg heated CO2 was injected into sediments with CH4 hydrate saturations of 50%. While in the first experiment the CO2 was injected discontinuously in a so called "huff'n puff" manner, the second experiment saw a continuous injection. Conditions within LARS were set to 13 MPa and 8˚ C, which allow for stability of pure CO2 and CH4 hydrates as well as mixed hydrates. The CO2 was heated and entered the sediment sample with temperatures of approximately 30˚ C. In this presentation we will discuss the results from the large-scale experiments and compare them with data from small-scale experiments.
NASA Astrophysics Data System (ADS)
He, Xiangming; Li, Jianjun; Cheng, Hongwei; Jiang, Changyin; Wan, Chunrong
A novel synthesis of controlled crystallization and granulation was attempted to prepare nano-scale β-Ni(OH) 2 cathode materials for high power Ni-MH batteries. Nano-scale β-Ni(OH) 2 and Co(OH) 2 with a diameter of 20 nm were prepared by controlled crystallization, mixed by ball milling, and granulated to form about 5 μm spherical grains by spray drying granulation. Both the addition of nano-scale Co(OH) 2 and granulation significantly enhanced electrochemical performance of nano-scale Ni(OH) 2. The XRD and TEM analysis shown that there were a large amount of defects among the crystal lattice of as-prepared nano-scale Ni(OH) 2, and the DTA-TG analysis shown that it had both lower decomposition temperature and higher decomposition reaction rate, indicating less thermal stability, as compared with conventional micro-scale Ni(OH) 2, and indicating that it had higher electrochemical performance. The granulated grains of nano-scale Ni(OH) 2 mixed with nano-scale Co(OH) 2 at Co/Ni = 1/20 presented the highest specific capacity reaching its theoretical value of 289 mAh g -1 at 1 C, and also exhibited much improved electrochemical performance at high discharge capacity rate up to 10 C. The granulated grains of nano-scale β-Ni(OH) 2 mixed with nano-scale Co(OH) 2 is a promising cathode active material for high power Ni-MH batteries.
NASA Astrophysics Data System (ADS)
Oldenburg, C. M.; Peters, C. A.; Dobson, P. F.; Doughty, C.
2010-12-01
Understanding the processes involved in large-scale upward flow of CO2 related to Geologic Carbon Sequestration (GCS) is critical to evaluating trapping mechanisms and potential impacts of CO2 leakage over long distances. The Laboratory for Underground CO2 Investigations (LUCI) is being planned to be built at DUSEL to host large-scale vertical CO2 and brine flow experiments. As conceived, LUCI would consist of a 500 m-long vertical raisebore approximately 3 m in diameter which will contain three suspended long-column pressure vessels. The long-column pressure vessels are planned to be 1 m in diameter with thermal control on the outer walls with a centralized inner fiberglass well for accommodating monitoring tools for determining phase saturation, porosity, temperature, and other properties of the flow region. The outer wall of the inner fiberglass well and the inner wall of the main vessel comprise the lateral boundaries of the long vertical annular regions that will be filled with porous media in which experiments investigating flow and transport, geochemical alterations of well cement, and biological processes involving injected CO2 will be performed. The large vertical extent of the column is needed to span the full range of CO2 conditions from supercritical (scCO2, P > 7.4 MPa, T > 31 °C) to gaseous CO2 that is believed to be significant as CO2 flows upwards. Here we consider the CO2-brine flow experiments in which the annular region will be pressurized at the top and bottom and contain brine-filled porous media through which scCO2 introduced at the bottom will flow upward. We are carrying out two-phase flow simulations of the buoyancy- and pressure-driven flow of CO2 and brine upward in the annular porous media region to further design the flow columns, e.g., to determine critical length and diameter requirements, as well as to plan the experiments to be performed. The simulations are carried out using TOUGH2/ECO2N, which models two-phase non-isothermal flow and transport of water, CO2, and NaCl in porous media. To treat important issues of drainage and imbibition at the leading and trailing edges of the CO2 slug, we employ hysteretic relative permeability functions. Simulation results will be presented showing flow rate, saturation, and temperature dependence on permeability, relative permeability parameters, size of initial CO2 slug, imposed upward flow rate, and different side boundary conditions (e.g., fully insulated and temperature equal to a constant geothermal gradient).
Transforming a Liability Into An Asset-Creating a Market for CO2-based Products
NASA Astrophysics Data System (ADS)
David, B. J.
2016-12-01
This session will discuss converting CO2 from a liability into an asset. It will specifically discuss how at least 25 products can be created using CO2 as a feedstock and deployed in the market at large scale. Focus will be on products that can both achieve scale from a market standpoint as well as climate significance in use of CO2 as a feedstock. The session will describe the market drivers supporting and inhibiting commercial deployment of CO2-based products. It will list key barriers and risks in the various CO2-based product segments. These barriers/risks could occur across technology, policy, institutional, economic, and other dimensions. The means to mitigate each barrier and the likelihood for such means to be deployed will be discussed.
NASA Astrophysics Data System (ADS)
Choi, Yonghoon; Vay, Stephanie A.; Vadrevu, Krishna P.; Soja, Amber J.; Woo, Jung-Hun; Nolf, Scott R.; Sachse, Glen W.; Diskin, Glenn S.; Blake, Donald R.; Blake, Nicola J.; Singh, Hanwant B.; Avery, Melody A.; Fried, Alan; Pfister, Leonhard; Fuelberg, Henry E.
2008-04-01
High resolution in situ measurements of atmospheric CO2 were made from the NASA DC-8 aircraft during the Intercontinental Chemical Transport Experiment-North America (INTEX-NA) campaign, part of the wider International Consortium for Atmospheric Research on Transport and Transformation (ICARTT). During the summer of 2004, eighteen flights comprising 160 h of measurements were conducted within a region bounded by 27 to 53°N and 36 to 139°W over an altitude range of 0.15 to 12 km. These large-scale surveys provided the opportunity to examine the characteristics of the atmospheric CO2 signal over sparsely sampled areas of North America and adjacent ocean basins. The observations showed a high degree of variability (≤18%) due to the myriad source and sink processes influencing the air masses intercepted over the INTEX-NA sampling domain. Surface fluxes had strong effects on continental scale concentration gradients. Clear signatures of CO2 uptake were seen east of the Mississippi River, notably a persistent CO2 deficit in the lowest 2-3 km. When combining the airborne CO2 measurements with LANDSAT and MODIS data products, the lowest CO2 mixing ratios observed during the campaign (337 ppm) were tied to mid-continental agricultural fields planted in corn and soybeans. We used simultaneous measurements of CO, O3, C2Cl4, C2H6, C2H2 and other unique chemical tracers to differentiate air mass types. Coupling these distinct air mass chemical signatures with transport history permitted identification of convection, stratosphere-troposphere exchange, long-range transport from Eastern Asia, boreal wildfires, and continental outflow as competing processes at multiple scales influencing the observed concentrations. Our results suggest these are important factors contributing to the large-scale distribution in CO2 mixing ratios thus these observations offer new constraints in the computation of the North American carbon budget.
NASA Astrophysics Data System (ADS)
Blanco, K.; Aponte, H.; Vera, E.
2017-12-01
For all Industrial sector is important to extend the useful life of the materials that they use in their process, the scales of CaCO3 are common in situation where fluids are handled with high concentration of ions and besides this temperatures and CO2 concentration dissolved, that scale generates large annual losses because there is a reduction in the process efficiency or corrosion damage under deposit, among other. In order to find new alternatives to this problem, the citric acid was evaluated as scale of calcium carbonate inhibition in critical condition of temperature and concentration of CO2 dissolved. Once the results are obtained it was carried out the statistical evaluation in order to generate an equation that allow to see that behaviour, giving as result, a good efficiency of inhibition to the conditions evaluated the scales of products obtained were characterized through scanning electron microscopy.
Drought stress and tree size determine stem CO2 efflux in a tropical forest.
Rowland, Lucy; da Costa, Antonio C L; Oliveira, Alex A R; Oliveira, Rafael S; Bittencourt, Paulo L; Costa, Patricia B; Giles, Andre L; Sosa, Azul I; Coughlin, Ingrid; Godlee, John L; Vasconcelos, Steel S; Junior, João A S; Ferreira, Leandro V; Mencuccini, Maurizio; Meir, Patrick
2018-06-01
CO 2 efflux from stems (CO 2_stem ) accounts for a substantial fraction of tropical forest gross primary productivity, but the climate sensitivity of this flux remains poorly understood. We present a study of tropical forest CO 2_stem from 215 trees across wet and dry seasons, at the world's longest running tropical forest drought experiment site. We show a 27% increase in wet season CO 2_stem in the droughted forest relative to a control forest. This was driven by increasing CO 2_stem in trees 10-40 cm diameter. Furthermore, we show that drought increases the proportion of maintenance to growth respiration in trees > 20 cm diameter, including large increases in maintenance respiration in the largest droughted trees, > 40 cm diameter. However, we found no clear taxonomic influence on CO 2_stem and were unable to accurately predict how drought sensitivity altered ecosystem scale CO 2_stem , due to substantial uncertainty introduced by contrasting methods previously employed to scale CO 2_stem fluxes. Our findings indicate that under future scenarios of elevated drought, increases in CO 2_stem may augment carbon losses, weakening or potentially reversing the tropical forest carbon sink. However, due to substantial uncertainties in scaling CO 2_stem fluxes, stand-scale future estimates of changes in stem CO 2 emissions remain highly uncertain. © 2018 The Authors New Phytologist © 2018 New Phytologist Trust.
Energetic valorization of wood waste: estimation of the reduction in CO2 emissions.
Vanneste, J; Van Gerven, T; Vander Putten, E; Van der Bruggen, B; Helsen, L
2011-09-01
This paper investigates the potential CO(2) emission reductions related to a partial switch from fossil fuel-based heat and electricity generation to renewable wood waste-based systems in Flanders. The results show that valorization in large-scale CHP (combined heat and power) systems and co-firing in coal plants have the largest CO(2) reduction per TJ wood waste. However, at current co-firing rates of 10%, the CO(2) reduction per GWh of electricity that can be achieved by co-firing in coal plants is five times lower than the CO(2) reduction per GWh of large-scale CHP. Moreover, analysis of the effect of government support for co-firing of wood waste in coal-fired power plants on the marginal costs of electricity generation plants reveals that the effect of the European Emission Trading Scheme (EU ETS) is effectively counterbalanced. This is due to the fact that biomass integrated gasification combined cycles (BIGCC) are not yet commercially available. An increase of the fraction of coal-based electricity in the total electricity generation from 8 to 10% at the expense of the fraction of gas-based electricity due to the government support for co-firing wood waste, would compensate entirely for the CO(2) reduction by substitution of coal by wood waste. This clearly illustrates the possibility of a 'rebound' effect on the CO(2) reduction due to government support for co-combustion of wood waste in an electricity generation system with large installed capacity of coal- and gas-based power plants, such as the Belgian one. Copyright © 2011 Elsevier B.V. All rights reserved.
Scaling laws for perturbations in the ocean-atmosphere system following large CO2 emissions
NASA Astrophysics Data System (ADS)
Towles, N.; Olson, P.; Gnanadesikan, A.
2015-01-01
Scaling relationships are derived for the perturbations to atmosphere and ocean variables from large transient CO2 emissions. Using the carbon cycle model LOSCAR (Zeebe et al., 2009; Zeebe, 2012b) we calculate perturbations to atmosphere temperature and total carbon, ocean temperature, total ocean carbon, pH, and alkalinity, marine sediment carbon, plus carbon-13 isotope anomalies in the ocean and atmosphere resulting from idealized CO2 emission events. The peak perturbations in the atmosphere and ocean variables are then fit to power law functions of the form γDαEbeta, where D is the event duration, E is its total carbon emission, and γ is a coefficient. Good power law fits are obtained for most system variables for E up to 50 000 PgC and D up to 100 kyr. However, these power laws deviate substantially from predictions based on simplified equilibrium considerations. For example, although all of the peak perturbations increase with emission rate E/D, we find no evidence of emission rate-only scaling α + β =0, a prediction of the long-term equilibrium between CO2 input by volcanism and CO2 removal by silicate weathering. Instead, our scaling yields α + β ≃ 1 for total ocean and atmosphere carbon and 0< α + β < 1 for most of the other system variables. The deviations in these scaling laws from equilibrium predictions are mainly due to the multitude and diversity of time scales that govern the exchange of carbon between marine sediments, the ocean, and the atmosphere.
Co-governing decentralised water systems: an analytical framework.
Yu, C; Brown, R; Morison, P
2012-01-01
Current discourses in urban water management emphasise a diversity of water sources and scales of infrastructure for resilience and adaptability. During the last 2 decades, in particular, various small-scale systems emerged and developed so that the debate has largely moved from centralised versus decentralised water systems toward governing integrated and networked systems of provision and consumption where small-scale technologies are embedded in large-scale centralised infrastructures. However, while centralised systems have established boundaries of ownership and management, decentralised water systems (such as stormwater harvesting technologies for the street, allotment/house scales) do not, therefore the viability for adoption and/or continued use of decentralised water systems is challenged. This paper brings together insights from the literature on public sector governance, co-production and social practices model to develop an analytical framework for co-governing such systems. The framework provides urban water practitioners with guidance when designing co-governance arrangements for decentralised water systems so that these systems continue to exist, and become widely adopted, within the established urban water regime.
The use of forest stand age information in an atmospheric CO2 inversion applied to North America
F. Deng; J.M. Chen; Y. Pan; W. Peters; R. Birdsey; K. McCullough; J. Xiao
2013-01-01
Atmospheric inversions have become an important tool in quantifying carbon dioxide (CO2) sinks and sources at a variety of spatiotemporal scales, but associated large uncertainties restrain the inversion research community from reaching agreement on many important subjects. We enhanced an atmospheric inversion of the CO2...
Lateral transport of soil carbon and land−atmosphere CO2 flux induced by water erosion in China
Yue, Yao; Ni, Jinren; Ciais, Philippe; Piao, Shilong; Wang, Tao; Huang, Mengtian; Borthwick, Alistair G. L.; Li, Tianhong; Wang, Yichu; Chappell, Adrian; Van Oost, Kristof
2016-01-01
Soil erosion by water impacts soil organic carbon stocks and alters CO2 fluxes exchanged with the atmosphere. The role of erosion as a net sink or source of atmospheric CO2 remains highly debated, and little information is available at scales larger than small catchments or regions. This study attempts to quantify the lateral transport of soil carbon and consequent land−atmosphere CO2 fluxes at the scale of China, where severe erosion has occurred for several decades. Based on the distribution of soil erosion rates derived from detailed national surveys and soil carbon inventories, here we show that water erosion in China displaced 180 ± 80 Mt C⋅y−1 of soil organic carbon during the last two decades, and this resulted a net land sink for atmospheric CO2 of 45 ± 25 Mt C⋅y−1, equivalent to 8–37% of the terrestrial carbon sink previously assessed in China. Interestingly, the “hotspots,” largely distributed in mountainous regions in the most intensive sink areas (>40 g C⋅m−2⋅y−1), occupy only 1.5% of the total area suffering water erosion, but contribute 19.3% to the national erosion-induced CO2 sink. The erosion-induced CO2 sink underwent a remarkable reduction of about 16% from the middle 1990s to the early 2010s, due to diminishing erosion after the implementation of large-scale soil conservation programs. These findings demonstrate the necessity of including erosion-induced CO2 in the terrestrial budget, hence reducing the level of uncertainty. PMID:27247397
Lateral transport of soil carbon and land-atmosphere CO2 flux induced by water erosion in China
NASA Astrophysics Data System (ADS)
Yue, Yao; Ni, Jinren; Ciais, Philippe; Piao, Shilong; Wang, Tao; Huang, Mengtian; Borthwick, Alistair G. L.; Li, Tianhong; Wang, Yichu; Chappell, Adrian; Van Oost, Kristof
2016-06-01
Soil erosion by water impacts soil organic carbon stocks and alters CO2 fluxes exchanged with the atmosphere. The role of erosion as a net sink or source of atmospheric CO2 remains highly debated, and little information is available at scales larger than small catchments or regions. This study attempts to quantify the lateral transport of soil carbon and consequent land-atmosphere CO2 fluxes at the scale of China, where severe erosion has occurred for several decades. Based on the distribution of soil erosion rates derived from detailed national surveys and soil carbon inventories, here we show that water erosion in China displaced 180 ± 80 Mt Cṡy-1 of soil organic carbon during the last two decades, and this resulted a net land sink for atmospheric CO2 of 45 ± 25 Mt Cṡy-1, equivalent to 8-37% of the terrestrial carbon sink previously assessed in China. Interestingly, the “hotspots,” largely distributed in mountainous regions in the most intensive sink areas (>40 g Cṡm-2ṡy-1), occupy only 1.5% of the total area suffering water erosion, but contribute 19.3% to the national erosion-induced CO2 sink. The erosion-induced CO2 sink underwent a remarkable reduction of about 16% from the middle 1990s to the early 2010s, due to diminishing erosion after the implementation of large-scale soil conservation programs. These findings demonstrate the necessity of including erosion-induced CO2 in the terrestrial budget, hence reducing the level of uncertainty.
McDonald, Cory P.; Stets, Edward; Striegl, Robert G.; Butman, David
2013-01-01
Accurate quantification of CO2 flux across the air-water interface and identification of the mechanisms driving CO2 concentrations in lakes and reservoirs is critical to integrating aquatic systems into large-scale carbon budgets, and to predicting the response of these systems to changes in climate or terrestrial carbon cycling. Large-scale estimates of the role of lakes and reservoirs in the carbon cycle, however, typically must rely on aggregation of spatially and temporally inconsistent data from disparate sources. We performed a spatially comprehensive analysis of CO2 concentration and air-water fluxes in lakes and reservoirs of the contiguous United States using large, consistent data sets, and modeled the relative contribution of inorganic and organic carbon loading to vertical CO2 fluxes. Approximately 70% of lakes and reservoirs are supersaturated with respect to the atmosphere during the summer (June–September). Although there is considerable interregional and intraregional variability, lakes and reservoirs represent a net source of CO2 to the atmosphere of approximately 40 Gg C d–1 during the summer. While in-lake CO2 concentrations correlate with indicators of in-lake net ecosystem productivity, virtually no relationship exists between dissolved organic carbon and pCO2,aq. Modeling suggests that hydrologic dissolved inorganic carbon supports pCO2,aq in most supersaturated systems (to the extent that 12% of supersaturated systems simultaneously exhibit positive net ecosystem productivity), and also supports primary production in most CO2-undersaturated systems. Dissolved inorganic carbon loading appears to be an important determinant of CO2concentrations and fluxes across the air-water interface in the majority of lakes and reservoirs in the contiguous United States.
A controlled field pilot for testing near surface CO2 detection techniques and transport models
Spangler, L.H.; Dobeck, L.M.; Repasky, K.; Nehrir, A.; Humphries, S.; Keith, C.; Shaw, J.; Rouse, J.; Cunningham, A.; Benson, S.; Oldenburg, C.M.; Lewicki, J.L.; Wells, A.; Diehl, R.; Strazisar, B.; Fessenden, J.; Rahn, Thomas; Amonette, J.; Barr, J.; Pickles, W.; Jacobson, J.; Silver, E.; Male, E.; Rauch, H.; Gullickson, K.; Trautz, R.; Kharaka, Y.; Birkholzer, J.; Wielopolski, L.
2009-01-01
A field facility has been developed to allow controlled studies of near surface CO2 transport and detection technologies. The key component of the facility is a shallow, slotted horizontal well divided into six zones. The scale and fluxes were designed to address large scale CO2 storage projects and desired retention rates for those projects. A wide variety of detection techniques were deployed by collaborators from 6 national labs, 2 universities, EPRI, and the USGS. Additionally, modeling of CO2 transport and concentrations in the saturated soil and in the vadose zone was conducted. An overview of these results will be presented. ?? 2009 Elsevier Ltd. All rights reserved.
Reducing Risk in CO2 Sequestration: A Framework for Integrated Monitoring of Basin Scale Injection
NASA Astrophysics Data System (ADS)
Seto, C. J.; Haidari, A. S.; McRae, G. J.
2009-12-01
Geological sequestration of CO2 is an option for stabilization of atmospheric CO2 concentrations. Technical ability to safely store CO2 in the subsurface has been demonstrated through pilot projects and a long history of enhanced oil recovery and acid gas disposal operations. To address climate change, current injection operations must be scaled up by a factor of 100, raising issues of safety and security. Monitoring and verification is an essential component in ensuring safe operations and managing risk. Monitoring provides assurance that CO2 is securely stored in the subsurface, and the mechanisms governing transport and storage are well understood. It also provides an early warning mechanism for identification of anomalies in performance, and a means for intervention and remediation through the ability to locate the CO2. Through theoretical studies, bench scale experiments and pilot tests, a number of technologies have demonstrated their ability to monitor CO2 in the surface and subsurface. Because the focus of these studies has been to demonstrate feasibility, individual techniques have not been integrated to provide a more robust method for monitoring. Considering the large volumes required for injection, size of the potential footprint, length of time a project must be monitored and uncertainty, operational considerations of cost and risk must balance safety and security. Integration of multiple monitoring techniques will reduce uncertainty in monitoring injected CO2, thereby reducing risk. We present a framework for risk management of large scale injection through model based monitoring network design. This framework is applied to monitoring CO2 in a synthetic reservoir where there is uncertainty in the underlying permeability field controlling fluid migration. Deformation and seismic data are used to track plume migration. A modified Ensemble Kalman filter approach is used to estimate flow properties by jointly assimilating flow and geomechanical observations. Issues of risk, cost and uncertainty are considered.
Sun, Zhihong; Niinemets, Ülo; Hüve, Katja; Rasulov, Bahtijor; Noe, Steffen M
2013-05-01
Effects of elevated atmospheric [CO2] on plant isoprene emissions are controversial. Relying on leaf-scale measurements, most models simulating isoprene emissions in future higher [CO2] atmospheres suggest reduced emission fluxes. However, combined effects of elevated [CO2] on leaf area growth, net assimilation and isoprene emission rates have rarely been studied on the canopy scale, but stimulation of leaf area growth may largely compensate for possible [CO2] inhibition reported at the leaf scale. This study tests the hypothesis that stimulated leaf area growth leads to increased canopy isoprene emission rates. We studied the dynamics of canopy growth, and net assimilation and isoprene emission rates in hybrid aspen (Populus tremula × Populus tremuloides) grown under 380 and 780 μmol mol(-1) [CO2]. A theoretical framework based on the Chapman-Richards function to model canopy growth and numerically compare the growth dynamics among ambient and elevated atmospheric [CO2]-grown plants was developed. Plants grown under elevated [CO2] had higher C : N ratio, and greater total leaf area, and canopy net assimilation and isoprene emission rates. During ontogeny, these key canopy characteristics developed faster and stabilized earlier under elevated [CO2]. However, on a leaf area basis, foliage physiological traits remained in a transient state over the whole experiment. These results demonstrate that canopy-scale dynamics importantly complements the leaf-scale processes, and that isoprene emissions may actually increase under higher [CO2] as a result of enhanced leaf area production. © 2013 The Authors. New Phytologist © 2013 New Phytologist Trust.
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.
State-resolved Thermal/Hyperthermal Dynamics of Atmospheric Species
2015-06-23
gas -room temperature ionic liquid (RTIL) interfaces. 2) Large scale trajectory simulations for theoretical analysis of gas - liquid scattering studies...areas: 1) Diode laser and LIF studies of hyperthermal CO2 and NO collisions at the gas -room temperature ionic liquid (RTIL) interfaces. 2) Large...scale trajectory simulations for theoretical analysis of gas - liquid scattering studies, 3) LIF data for state-resolved scattering of hyperthermal NO at
NASA Astrophysics Data System (ADS)
Zhu, Q.; Zhuang, Q.; Henze, D.; Bowman, K.; Chen, M.; Liu, Y.; He, Y.; Matsueda, H.; Machida, T.; Sawa, Y.; Oechel, W.
2014-09-01
Regional net carbon fluxes of terrestrial ecosystems could be estimated with either biogeochemistry models by assimilating surface carbon flux measurements or atmospheric CO2 inversions by assimilating observations of atmospheric CO2 concentrations. Here we combine the ecosystem biogeochemistry modeling and atmospheric CO2 inverse modeling to investigate the magnitude and spatial distribution of the terrestrial ecosystem CO2 sources and sinks. First, we constrain a terrestrial ecosystem model (TEM) at site level by assimilating the observed net ecosystem production (NEP) for various plant functional types. We find that the uncertainties of model parameters are reduced up to 90% and model predictability is greatly improved for all the plant functional types (coefficients of determination are enhanced up to 0.73). We then extrapolate the model to a global scale at a 0.5° × 0.5° resolution to estimate the large-scale terrestrial ecosystem CO2 fluxes, which serve as prior for atmospheric CO2 inversion. Second, we constrain the large-scale terrestrial CO2 fluxes by assimilating the GLOBALVIEW-CO2 and mid-tropospheric CO2 retrievals from the Atmospheric Infrared Sounder (AIRS) into an atmospheric transport model (GEOS-Chem). The transport inversion estimates that: (1) the annual terrestrial ecosystem carbon sink in 2003 is -2.47 Pg C yr-1, which agrees reasonably well with the most recent inter-comparison studies of CO2 inversions (-2.82 Pg C yr-1); (2) North America temperate, Europe and Eurasia temperate regions act as major terrestrial carbon sinks; and (3) The posterior transport model is able to reasonably reproduce the atmospheric CO2 concentrations, which are validated against Comprehensive Observation Network for TRace gases by AIrLiner (CONTRAIL) CO2 concentration data. This study indicates that biogeochemistry modeling or atmospheric transport and inverse modeling alone might not be able to well quantify regional terrestrial carbon fluxes. However, combining the two modeling approaches and assimilating data of surface carbon flux as well as atmospheric CO2 mixing ratios might significantly improve the quantification of terrestrial carbon fluxes.
NASA Astrophysics Data System (ADS)
El Kazzi, S.; Mortelmans, W.; Nuytten, T.; Meersschaut, J.; Carolan, P.; Landeloos, L.; Conard, T.; Radu, I.; Heyns, M.; Merckling, C.
2018-04-01
We present in this paper the use of Gas Source Molecular Beam Epitaxy for the large-scale growth of transition metal dichalcogenides. Fiber-textured MoS2 co-deposited thin films (down to 1 MLs) are grown on commercially 200 mm wafer size templates where MX2 crystalline layers are achieved at temperatures ranging from RT to 550 °C. Raman Spectroscopy and photoluminescence measurements along with X-Ray Photoelectron Spectroscopy show that a low growth rate is essential for complete Mo sulfurization during MoS2 co-deposition. Finally, cross-section Transmission Electron Microscopy investigations are discussed to highlight the influence of SiO2 and Al2O3 used surfaces on MoS2 deposition.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Loring, John S.; Ilton, Eugene S.; Chen, Jeffrey
Shale formations play fundamental roles in large-scale geologic carbon sequestration (GCS) aimed primarily to mitigate climate change, and in smaller-scale GCS targeted mainly for CO2-enhanced gas recovery operations. In both technologies, CO2 is injected underground as a supercritical fluid (scCO2), where interactions with shale minerals could influence successful GCS implementation. Reactive components of shales include expandable clays, such as montmorillonites and mixed-layer illite/smectite clays. In this work, we used in situ X-ray diffraction (XRD) and in situ infrared (IR) spectroscopy to investigate the swelling/shrinkage and water/CO2 sorption of a pure montmorillonite, Na-SWy-2, when the clay is exposed to variably hydratedmore » scCO2 at 50 °C and 90 bar. Measured interlayer spacings and sorbed water concentrations at varying levels of scCO2 hydration are similar to previously reported values measured in air at ambient pressure over a range of relative humidities. IR spectra show evidence of both water and CO2 intercalation, and variations in peak shapes and positions suggest multiple sorbed types with distinct chemical environments. Based on the intensity of the asymmetric CO stretching band of the CO2 associated with the Na-SWy-2, we observed a significant increase in sorbed CO2 as the clay expands from a 0W to a 1W state, suggesting that water props open the interlayer so that CO2 can enter. However, as the clay transitions from a 1W to a 2W state, CO2 desorbs sharply. These observations were placed in the context of two conceptual models concerning hydration mechanisms for expandable clays and were also discussed in light of recent theoretical studies on CO2-H2O-clay interactions. The swelling/shrinkage of expandable clays could affect solid volume, porosity, and permeability of shales. Consequently, the results from this work could aid predictions of shale caprock integrity in large-scale GCS, as well as methane transmissivity in enhanced gas recovery operations.« less
NASA Astrophysics Data System (ADS)
Graven, H. D.; Gruber, N.
2011-12-01
The 14C-free fossil carbon added to atmospheric CO2 by combustion dilutes the atmospheric 14C/C ratio (Δ14C), potentially providing a means to verify fossil CO2 emissions calculated using economic inventories. However, sources of 14C from nuclear power generation and spent fuel reprocessing can counteract this dilution and may bias 14C/C-based estimates of fossil fuel-derived CO2 if these nuclear influences are not correctly accounted for. Previous studies have examined nuclear influences on local scales, but the potential for continental-scale influences on Δ14C has not yet been explored. We estimate annual 14C emissions from each nuclear site in the world and conduct an Eulerian transport modeling study to investigate the continental-scale, steady-state gradients of Δ14C caused by nuclear activities and fossil fuel combustion. Over large regions of Europe, North America and East Asia, nuclear enrichment may offset at least 20% of the fossil fuel dilution in Δ14C, corresponding to potential biases of more than -0.25 ppm in the CO2 attributed to fossil fuel emissions, larger than the bias from plant and soil respiration in some areas. Model grid cells including high 14C-release reactors or fuel reprocessing sites showed much larger nuclear enrichment, despite the coarse model resolution of 1.8°×1.8°. The recent growth of nuclear 14C emissions increased the potential nuclear bias over 1985-2005, suggesting that changing nuclear activities may complicate the use of Δ14C observations to identify trends in fossil fuel emissions. The magnitude of the potential nuclear bias is largely independent of the choice of reference station in the context of continental-scale Eulerian transport and inversion studies, but could potentially be reduced by an appropriate choice of reference station in the context of local-scale assessments.
Balloon-borne tropospheric CO2 observations over the equatorial eastern and western Pacific
NASA Astrophysics Data System (ADS)
Inai, Yoichi; Aoki, Shuji; Honda, Hideyuki; Furutani, Hiroshi; Matsumi, Yutaka; Ouchi, Mai; Sugawara, Satoshi; Hasebe, Fumio; Uematsu, Mitsuo; Fujiwara, Masatomo
2018-07-01
Vertical profiles of carbon dioxide (CO2) mixing ratio in the equatorial eastern and western Pacific were measured by newly developed balloon-borne CO2 sondes in February 2012 (two soundings) and February-March 2015 (four soundings), respectively. The 1-10 km vertically averaged CO2 mixing ratios lie between the background surface values in the Northern Hemisphere (NH) and those in the Southern Hemisphere (SH) monitored at ground-based sites during these periods. A backward trajectory analysis, taking account of convective mixing processes using geostationary satellite cloud-image data, is applied to the measured CO2 profiles to estimate the origin of the observed air masses. Air masses originating in the SH show low CO2 mixing ratios that are similar to the background values in the SH. This relationship is confirmed by a positive correlation (∼0.6) between the CO2 mixing ratio and the latitude of air mass origin which is found from trajectory calculations. This result suggests that the CO2 distribution in the troposphere over the equatorial Pacific is controlled by monthly time-scale, large-scale CO2 distribution and weekly time-scale atmospheric transport processes. Furthermore, this study shows that the combination of CO2 sonde measurements and trajectory analysis, taking account of convective mixing, is a useful tool in investigating CO2 transport processes.
NASA Astrophysics Data System (ADS)
Møll Nilsen, Halvor; Lie, Knut-Andreas; Andersen, Odd
2015-06-01
MRST-co2lab is a collection of open-source computational tools for modeling large-scale and long-time migration of CO2 in conductive aquifers, combining ideas from basin modeling, computational geometry, hydrology, and reservoir simulation. Herein, we employ the methods of MRST-co2lab to study long-term CO2 storage on the scale of hundreds of megatonnes. We consider public data sets of two aquifers from the Norwegian North Sea and use geometrical methods for identifying structural traps, percolation-type methods for identifying potential spill paths, and vertical-equilibrium methods for efficient simulation of structural, residual, and solubility trapping in a thousand-year perspective. In particular, we investigate how data resolution affects estimates of storage capacity and discuss workflows for identifying good injection sites and optimizing injection strategies.
Nakasaki, Kiyohiko; Marui, Taketoshi
2011-06-01
To monitor the progress of organic matter degradation in a large-scale composting facility, the percentage of organic matter degradation was determined by measuring CO(2) evolution during recomposting of compost samples withdrawn from the facility. The percentage of organic matter degradation was calculated as the ratio of the amount of CO(2) evolved from compost raw material to that evolved from each sample during recomposting in the laboratory composting apparatus. It was assumed that the difference in the cumulative emission of CO(2) between the compost raw material and a sample corresponds to the amount of CO( 2) evolved from the sample in the composting facility. Using this method, the changes in organic matter degradation during composting in practical large-scale composting facilities were estimated and it was found that the percentage of organic matter degradation increased more vigorously in the earlier stages than in the later stages of composting. The percentage of organic matter degradation finally reached 78 and 55% for the compost produced from garbage-animal manure mixture and distillery waste (shochu residue), respectively. It was thus ascertained that organic matter degradation progressed well in both composting facilities. Furthermore, by performing a plant growth assay, it was observed that the compost products of both the facilities did not inhibit seed germination and thus were useful in promoting plant growth.
Keating, Elizabeth H.; Hakala, J. Alexandra; Viswanathan, Hari; ...
2013-03-01
It is challenging to predict the degree to which shallow groundwater might be affected by leaks from a CO 2 sequestration reservoir, particularly over long time scales and large spatial scales. In this study observations at a CO 2 enriched shallow aquifer natural analog were used to develop a predictive model which is then used to simulate leakage scenarios. This natural analog provides the opportunity to make direct field observations of groundwater chemistry in the presence of elevated CO 2, to collect aquifer samples and expose them to CO 2 under controlled conditions in the laboratory, and to test themore » ability of multiphase reactive transport models to reproduce measured geochemical trends at the field-scale. The field observations suggest that brackish water entrained with the upwelling CO 2 are a more significant source of trace metals than in situ mobilization of metals due to exposure to CO 2. The study focuses on a single trace metal of concern at this site: U. Experimental results indicate that cation exchange/adsorption and dissolution/precipitation of calcite containing trace amounts of U are important reactions controlling U in groundwater at this site, and that the amount of U associated with calcite is fairly well constrained. Simulations incorporating these results into a 3-D multi-phase reactive transport model are able to reproduce the measured ranges and trends between pH, pCO 2, Ca, total C, U and Cl -at the field site. Although the true fluxes at the natural analog site are unknown, the cumulative CO 2 flux inferred from these simulations are approximately equivalent to 37.8E-3 MT, approximately corresponding to a .001% leak rate for injection at a large (750 MW) power plant. The leakage scenario simulations suggest that if the leak only persists for a short time the volume of aquifer contaminated by CO 2-induced mobilization of U will be relatively small, yet persistent over 100 a.« less
Poromechanical response of naturally fractured sorbing media
NASA Astrophysics Data System (ADS)
Kumar, Hemant
The injection of CO2 in coal seams has been utilized for enhanced gas recovery and potential CO2 sequestration in unmineable coal seams. It is advantageous because as it enhances the production and significant volumes of CO2 may be stored simultaneously. The key issues for enhanced gas recovery and geologic sequestration of CO2 include (1) Injectivity prediction: The chemical and physical processes initiated by the injection of CO2 in the coal seam leads to permeability/porosity changes (2) Up scaling: Development of full scale coupled reservoir model which may predict the enhanced production, associated permeability changes and quantity of sequestered CO2. (3) Reservoir Stimulation: The coalbeds are often fractured and proppants are placed into the fractures to prevent the permeability reduction but the permeability evolution in such cases is poorly understood. These issues are largely governed by dynamic coupling of adsorption, fluid exchange, transport, water content, stress regime, fracture geometry and physiomechanical changes in coals which are triggered by CO 2 injection. The understanding of complex interactions in coal has been investigated through laboratory experiments and full reservoir scale models are developed to answer key issues. (Abstract shortened by ProQuest.).
Assessment of brine migration risks along vertical pathways due to CO2 injection
NASA Astrophysics Data System (ADS)
Kissinger, Alexander; Class, Holger
2015-04-01
Global climate change, shortage of resources and the growing usage of renewable energy sources has lead to a growing demand for the utilization of subsurface systems. Among these competing uses are Carbon Capture and Storage (CCS), geothermal energy, nuclear waste disposal, 'renewable' methane or hydrogen storage as well as the ongoing production of fossil resources like oil, gas and coal. Additionally, these technologies may also create conflicts with essential public interests such as water supply. For example, the injection of CO2 into the subsurface causes an increase in pressure reaching far beyond the actual radius of influence of the CO2 plume, potentially leading to large amounts of displaced salt water. In this work we focus on the large scale impacts of CO2 storage on brine migration but the methodology and the obtained results may also apply to other fields like waste water disposal, where large amounts of fluid are injected into the subsurface. In contrast to modeling on the reservoir scale the spatial scale required for this work is much larger in both vertical and lateral direction, as the regional hydrogeology has to be considered. Structures such as fault zones, hydrogeological windows in the Rupelian clay or salt domes are considered as potential pathways for displaced fluids into shallow systems and their influence has to be taken into account. We put the focus of our investigations on the latter type of scenario, since there is still a poor understanding of the role that salt diapirs would play in CO2 storage projects. As there is hardly any field data available on this scale, we compare different levels of model complexity in order to identify the relevant processes for brine displacement and simplify the modeling process wherever possible, for example brine injection vs. CO2 injection, simplified geometries vs. the complex formation geometry and the role of salt induced density differences on flow. Further we investigate the impact of the displaced brine due to CO2 injection and compare it to the natural fluid exchange between shallow and deep aquifers in order to asses possible damage.
NASA Astrophysics Data System (ADS)
Goodale, C. L.; Fredriksen, G.; McCalley, C. K.; Sparks, J. P.; Thomas, S. A.
2011-12-01
The atmospheric carbon dioxide (CO2) concentration has increased to a level unprecedented in the last 2 million years, and the concentration is projected to increase further with a rate unseen in geological past. The increase in CO2 cause a rise in surface temperatures and changes in the hydrological cycle through the redistribution of rainfall patterns. All of these changes will impact the weathering of rocks, which in turn affect atmospheric CO2 concentrations via two different pathways. On the one hand, CO2 is consumed by the dissolution reaction of the exposed minerals. And on the other hand, biological CO2 fixation is affected due to changes in phosphorus release from minerals, as biological activity is constrained by phosphorus availability at large scales. The traditional view is that both effects are negligible on a centennial time scale, but recent work on catchment scale challenge this view in favor of a potential high sensitivity of weathering to ongoing climate and land use changes. To globally quantify the contribution of CO2 fixation associated with weathering on the historical trend in terrestrial CO2 uptake, we applied a model of chemical weathering and phosphorus release under climate reconstructions from four Earth System Models. The simulations indicate that changes in weathering could have contributed considerably to the trend in terrestrial CO2 uptake since the pre-industrial revolution, with warming being the main driver of change. The increase in biological CO2 fixation is of comparable magnitude as the increase in CO2 consumption by chemical weathering. Our simulations support the previous findings on catchment scale that weathering can change significantly on a centennial time scale. This finding has implications for 21st century climate projections, which ignore changes in weathering, as well as for long-term airborne fraction of CO2 emissions, whose calculation usually neglects changes in phosphorus availability.
NASA Astrophysics Data System (ADS)
Goll, D. S.; Moosdorf, N.; Brovkin, V.; Hartmann, J.
2013-12-01
The atmospheric carbon dioxide (CO2) concentration has increased to a level unprecedented in the last 2 million years, and the concentration is projected to increase further with a rate unseen in geological past. The increase in CO2 cause a rise in surface temperatures and changes in the hydrological cycle through the redistribution of rainfall patterns. All of these changes will impact the weathering of rocks, which in turn affect atmospheric CO2 concentrations via two different pathways. On the one hand, CO2 is consumed by the dissolution reaction of the exposed minerals. And on the other hand, biological CO2 fixation is affected due to changes in phosphorus release from minerals, as biological activity is constrained by phosphorus availability at large scales. The traditional view is that both effects are negligible on a centennial time scale, but recent work on catchment scale challenge this view in favor of a potential high sensitivity of weathering to ongoing climate and land use changes. To globally quantify the contribution of CO2 fixation associated with weathering on the historical trend in terrestrial CO2 uptake, we applied a model of chemical weathering and phosphorus release under climate reconstructions from four Earth System Models. The simulations indicate that changes in weathering could have contributed considerably to the trend in terrestrial CO2 uptake since the pre-industrial revolution, with warming being the main driver of change. The increase in biological CO2 fixation is of comparable magnitude as the increase in CO2 consumption by chemical weathering. Our simulations support the previous findings on catchment scale that weathering can change significantly on a centennial time scale. This finding has implications for 21st century climate projections, which ignore changes in weathering, as well as for long-term airborne fraction of CO2 emissions, whose calculation usually neglects changes in phosphorus availability.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hite, Roger
The project site is located in Livingston Parish, Louisiana, approximately 26 miles due east of Baton Rouge. This project proposed to evaluate an early Eocene-aged Wilcox oil reservoir for permanent storage of CO 2. Blackhorse Energy, LLC planned to conduct a parallel CO 2 oil recovery project in the First Wilcox Sand. The primary focus of this project was to examine and prove the suitability of South Louisiana geologic formations for large-scale geologic sequestration of CO 2 in association with enhanced oil recovery applications. This was to be accomplished through the focused demonstration of small-scale, permanent storage of CO 2more » in the First Wilcox Sand. The project was terminated at the request of Blackhorse Energy LLC on October 22, 2014.« less
Among-provence variability of gas exchange and growth in response to long-term elevated CO2 exposure
James L.J. Houpis; Paul D. Anderson; James C. Pushnik; David J. Anschel
1999-01-01
Genetic variability can have profound effects on the interpretation of results from elevated CO2 studies, and future forest management decisions. Information on which varieties are best suited to future atmospheric conditions is needed to develop future forest management practices. A large-scale screening study of the effects of elevated CO
NASA Astrophysics Data System (ADS)
Chen, Z. H.; Zhu, J.; Zeng, N.
2013-01-01
CO2 measurements have been combined with simulated CO2 distributions from a transport model in order to produce the optimal estimates of CO2 surface fluxes in inverse modeling. However one persistent problem in using model-observation comparisons for this goal relates to the issue of compatibility. Observations at a single site reflect all underlying processes of various scales that usually cannot be fully resolved by model simulations at the grid points nearest the site due to lack of spatial or temporal resolution or missing processes in models. In this article we group site observations of multiple stations according to atmospheric mixing regimes and surface characteristics. The group averaged values of CO2 concentration from model simulations and observations are used to evaluate the regional model results. Using the group averaged measurements of CO2 reduces the noise of individual stations. The difference of group averaged values between observation and modeled results reflects the uncertainties of the large scale flux in the region where the grouped stations are. We compared the group averaged values between model results with two biospheric fluxes from the model Carnegie-Ames-Stanford-Approach (CASA) and VEgetation-Global-Atmosphere-Soil (VEGAS) and observations to evaluate the regional model results. Results show that the modeling group averaged values of CO2 concentrations in all regions with fluxes from VEGAS have significant improvements for most regions. There is still large difference between two model results and observations for grouped average values in North Atlantic, Indian Ocean, and South Pacific Tropics. This implies possible large uncertainties in the fluxes there.
Verdon, James P.; Kendall, J.-Michael; Stork, Anna L.; Chadwick, R. Andy; White, Don J.; Bissell, Rob C.
2013-01-01
Geological storage of CO2 that has been captured at large, point source emitters represents a key potential method for reduction of anthropogenic greenhouse gas emissions. However, this technology will only be viable if it can be guaranteed that injected CO2 will remain trapped in the subsurface for thousands of years or more. A significant issue for storage security is the geomechanical response of the reservoir. Concerns have been raised that geomechanical deformation induced by CO2 injection will create or reactivate fracture networks in the sealing caprocks, providing a pathway for CO2 leakage. In this paper, we examine three large-scale sites where CO2 is injected at rates of ∼1 megatonne/y or more: Sleipner, Weyburn, and In Salah. We compare and contrast the observed geomechanical behavior of each site, with particular focus on the risks to storage security posed by geomechanical deformation. At Sleipner, the large, high-permeability storage aquifer has experienced little pore pressure increase over 15 y of injection, implying little possibility of geomechanical deformation. At Weyburn, 45 y of oil production has depleted pore pressures before increases associated with CO2 injection. The long history of the field has led to complicated, sometimes nonintuitive geomechanical deformation. At In Salah, injection into the water leg of a gas reservoir has increased pore pressures, leading to uplift and substantial microseismic activity. The differences in the geomechanical responses of these sites emphasize the need for systematic geomechanical appraisal before injection in any potential storage site. PMID:23836635
Verdon, James P; Kendall, J-Michael; Stork, Anna L; Chadwick, R Andy; White, Don J; Bissell, Rob C
2013-07-23
Geological storage of CO2 that has been captured at large, point source emitters represents a key potential method for reduction of anthropogenic greenhouse gas emissions. However, this technology will only be viable if it can be guaranteed that injected CO2 will remain trapped in the subsurface for thousands of years or more. A significant issue for storage security is the geomechanical response of the reservoir. Concerns have been raised that geomechanical deformation induced by CO2 injection will create or reactivate fracture networks in the sealing caprocks, providing a pathway for CO2 leakage. In this paper, we examine three large-scale sites where CO2 is injected at rates of ~1 megatonne/y or more: Sleipner, Weyburn, and In Salah. We compare and contrast the observed geomechanical behavior of each site, with particular focus on the risks to storage security posed by geomechanical deformation. At Sleipner, the large, high-permeability storage aquifer has experienced little pore pressure increase over 15 y of injection, implying little possibility of geomechanical deformation. At Weyburn, 45 y of oil production has depleted pore pressures before increases associated with CO2 injection. The long history of the field has led to complicated, sometimes nonintuitive geomechanical deformation. At In Salah, injection into the water leg of a gas reservoir has increased pore pressures, leading to uplift and substantial microseismic activity. The differences in the geomechanical responses of these sites emphasize the need for systematic geomechanical appraisal before injection in any potential storage site.
Pereira, Hugo; Páramo, Jaime; Silva, Joana; Marques, Ana; Barros, Ana; Maurício, Dinis; Santos, Tamára; Schulze, Peter; Barros, Raúl; Gouveia, Luísa; Barreira, Luísa; Varela, João
2018-03-23
Industrial production of novel microalgal isolates is key to improving the current portfolio of available strains that are able to grow in large-scale production systems for different biotechnological applications, including carbon mitigation. In this context, Tetraselmis sp. CTP4 was successfully scaled up from an agar plate to 35- and 100-m 3 industrial scale tubular photobioreactors (PBR). Growth was performed semi-continuously for 60 days in the autumn-winter season (17 th October - 14 th December). Optimisation of tubular PBR operations showed that improved productivities were obtained at a culture velocity of 0.65-1.35 m s -1 and a pH set-point for CO 2 injection of 8.0. Highest volumetric (0.08 ± 0.01 g L -1 d -1 ) and areal (20.3 ± 3.2 g m -2 d -1 ) biomass productivities were attained in the 100-m 3 PBR compared to those of the 35-m 3 PBR (0.05 ± 0.02 g L -1 d -1 and 13.5 ± 4.3 g m -2 d -1 , respectively). Lipid contents were similar in both PBRs (9-10% of ash free dry weight). CO 2 sequestration was followed in the 100-m 3 PBR, revealing a mean CO 2 mitigation efficiency of 65% and a biomass to carbon ratio of 1.80. Tetraselmis sp. CTP4 is thus a robust candidate for industrial-scale production with promising biomass productivities and photosynthetic efficiencies up to 3.5% of total solar irradiance.
Large-Scale Ocean Circulation-Cloud Interactions Reduce the Pace of Transient Climate Change
NASA Technical Reports Server (NTRS)
Trossman, D. S.; Palter, J. B.; Merlis, T. M.; Huang, Y.; Xia, Y.
2016-01-01
Changes to the large scale oceanic circulation are thought to slow the pace of transient climate change due, in part, to their influence on radiative feedbacks. Here we evaluate the interactions between CO2-forced perturbations to the large-scale ocean circulation and the radiative cloud feedback in a climate model. Both the change of the ocean circulation and the radiative cloud feedback strongly influence the magnitude and spatial pattern of surface and ocean warming. Changes in the ocean circulation reduce the amount of transient global warming caused by the radiative cloud feedback by helping to maintain low cloud coverage in the face of global warming. The radiative cloud feedback is key in affecting atmospheric meridional heat transport changes and is the dominant radiative feedback mechanism that responds to ocean circulation change. Uncertainty in the simulated ocean circulation changes due to CO2 forcing may contribute a large share of the spread in the radiative cloud feedback among climate models.
Clavel, Guylhaine; Marichy, Catherine; Willinger, Marc-Georg; Ravaine, Serge; Zitoun, David; Pinna, Nicola
2010-12-07
CoFe(2)O(4)-TiO(2) and CoFe(2)O(4)-ZnO nanoparticles/film composites were prepared from directed assembly of colloidal CoFe(2)O(4) in a Langmuir-Blodgett monolayer and atomic layer deposition (ALD) of an oxide (TiO(2) or ZnO). The combination of these two methods permits the use of well-defined nanoparticles from colloidal chemistry, their assembly on a large scale, and the control over the interface between a ferrimagnetic material (CoFe(2)O(4)) and a semiconductor (TiO(2) or ZnO). Using this approach, architectures can be assembled with a precise control from the Angstrom scale (ALD) to the micrometer scale (Langmuir-Blodgett film). The resulting heterostructures present well-calibrated thicknesses. Electron microscopy and magnetic measurement studies give evidence that the size of the nanoparticles and their intrinsic magnetic properties are not altered by the various steps involved in the synthesis process. Therefore, the approach is suitable to obtain a layered composite with a quasi-monodisperse layer of ferrimagnetic nanoparticles embedded in an ultrathin film of semiconducting material.
Sakurai, Hidehiro; Masukawa, Hajime; Kitashima, Masaharu; Inoue, Kazuhito
2010-01-01
In order to decrease CO(2) emissions from the burning of fossil fuels, the development of new renewable energy sources sufficiently large in quantity is essential. To meet this need, we propose large-scale H(2) production on the sea surface utilizing cyanobacteria. Although many of the relevant technologies are in the early stage of development, this chapter briefly examines the feasibility of such H(2) production, in order to illustrate that under certain conditions large-scale photobiological H(2) production can be viable. Assuming that solar energy is converted to H(2) at 1.2% efficiency, the future cost of H(2) can be estimated to be about 11 (pipelines) and 26.4 (compression and marine transportation) cents kWh(-1), respectively.
Wu, Haiming; Fan, Jinlin; Zhang, Jian; Ngo, Huu Hao; Guo, Wenshan
2018-02-01
Multi-stage constructed wetlands (CWs) have been proved to be a cost-effective alternative in the treatment of various wastewaters for improving the treatment performance as compared with the conventional single-stage CWs. However, few long-term full-scale multi-stage CWs have been performed and evaluated for polishing effluents from domestic wastewater treatment plants (WWTP). This study investigated the seasonal and spatial dynamics of carbon and the effects of the key factors (input loading and temperature) in the large-scale seven-stage Wu River CW polishing domestic WWTP effluents in northern China. The results indicated a significant improvement in water quality. Significant seasonal and spatial variations of organics removal were observed in the Wu River CW with a higher COD removal efficiency of 64-66% in summer and fall. Obvious seasonal and spatial variations of CH 4 and CO 2 emissions were also found with the average CH 4 and CO 2 emission rates of 3.78-35.54 mg m -2 d -1 and 610.78-8992.71 mg m -2 d -1 , respectively, while the higher CH 4 and CO 2 emission flux was obtained in spring and summer. Seasonal air temperatures and inflow COD loading rates significantly affected organics removal and CH 4 emission, but they appeared to have a weak influence on CO 2 emission. Overall, this study suggested that large-scale Wu River CW might be a potential source of GHG, but considering the sustainability of the multi-stage CW, the inflow COD loading rate of 1.8-2.0 g m -2 d -1 and temperature of 15-20 °C may be the suitable condition for achieving the higher organics removal efficiency and lower greenhouse gases (GHG) emission in polishing the domestic WWTP effluent. The obtained knowledge of the carbon dynamics in large-scale Wu River CW will be helpful for understanding the carbon cycles, but also can provide useful field experience for the design, operation and management of multi-stage CW treatments. Copyright © 2017 Elsevier Ltd. All rights reserved.
Numerical investigation for the impact of CO2 geologic sequestration on regional groundwater flow
DOE Office of Scientific and Technical Information (OSTI.GOV)
Yamamoto, H.; Zhang, K.; Karasaki, K.
Large-scale storage of carbon dioxide in saline aquifers may cause considerable pressure perturbation and brine migration in deep rock formations, which may have a significant influence on the regional groundwater system. With the help of parallel computing techniques, we conducted a comprehensive, large-scale numerical simulation of CO{sub 2} geologic storage that predicts not only CO{sub 2} migration, but also its impact on regional groundwater flow. As a case study, a hypothetical industrial-scale CO{sub 2} injection in Tokyo Bay, which is surrounded by the most heavily industrialized area in Japan, was considered, and the impact of CO{sub 2} injection on near-surfacemore » aquifers was investigated, assuming relatively high seal-layer permeability (higher than 10 microdarcy). A regional hydrogeological model with an area of about 60 km x 70 km around Tokyo Bay was discretized into about 10 million gridblocks. To solve the high-resolution model efficiently, we used a parallelized multiphase flow simulator TOUGH2-MP/ECO2N on a world-class high performance supercomputer in Japan, the Earth Simulator. In this simulation, CO{sub 2} was injected into a storage aquifer at about 1 km depth under Tokyo Bay from 10 wells, at a total rate of 10 million tons/year for 100 years. Through the model, we can examine regional groundwater pressure buildup and groundwater migration to the land surface. The results suggest that even if containment of CO{sub 2} plume is ensured, pressure buildup on the order of a few bars can occur in the shallow confined aquifers over extensive regions, including urban inlands.« less
Economics of carbon dioxide capture and utilization-a supply and demand perspective.
Naims, Henriette
2016-11-01
Lately, the technical research on carbon dioxide capture and utilization (CCU) has achieved important breakthroughs. While single CO 2 -based innovations are entering the markets, the possible economic effects of a large-scale CO 2 utilization still remain unclear to policy makers and the public. Hence, this paper reviews the literature on CCU and provides insights on the motivations and potential of making use of recovered CO 2 emissions as a commodity in the industrial production of materials and fuels. By analyzing data on current global CO 2 supply from industrial sources, best practice benchmark capture costs and the demand potential of CO 2 utilization and storage scenarios with comparative statics, conclusions can be drawn on the role of different CO 2 sources. For near-term scenarios the demand for the commodity CO 2 can be covered from industrial processes, that emit CO 2 at a high purity and low benchmark capture cost of approximately 33 €/t. In the long-term, with synthetic fuel production and large-scale CO 2 utilization, CO 2 is likely to be available from a variety of processes at benchmark costs of approx. 65 €/t. Even if fossil-fired power generation is phased out, the CO 2 emissions of current industrial processes would suffice for ambitious CCU demand scenarios. At current economic conditions, the business case for CO 2 utilization is technology specific and depends on whether efficiency gains or substitution of volatile priced raw materials can be achieved. Overall, it is argued that CCU should be advanced complementary to mitigation technologies and can unfold its potential in creating local circular economy solutions.
A Policy Option To Provide Sufficient Funding For Massive-Scale Sequestration of CO2
NASA Astrophysics Data System (ADS)
Kithil, P. W.
2007-12-01
Global emissions of CO2 now are nearly 30 billion tons per year, and are growing rapidly due to strong economic growth. Atmospheric levels of CO2 have reached 380 ppm and recent reports suggest the rate of increase has gone from 1% per year in the 1990's to 3% per year now - with potential to cross 550ppm in the 2020 decade. Without stabilization of atmospheric CO2 below 550ppm, climate models predict unacceptably higher average temperatures with significant risk of runaway global warming this century. While there is much talk about reducing CO2 emissions by switching to non-fossil energy sources, imposing energy efficiency, and a host of other changes, there are no new large-scale energy sources on the horizon. The options are to impose draconian cuts in fossil energy consumption that will keep us below 550ppm (devastating the global economy) - or to adopt massive-scale sequestration of CO2. Three approaches are feasible: biological ocean sequestration, geologic sequestration, and biological terrestrial sequestration. Biological sequestration is applicable to all CO2 sources, whereas geologic sequestration is limited to fossil-fuel power plants and some large point-source emitters such as cement plants and large industrial facilities. Sequestration provides a direct mechanism for reducing atmospheric levels of CO2, whereas offsetting technologies such as wind power or improved efficiency, reduce the need for more fossil fuels but do not physically remove CO2 from the environment. The primary geologic technique, carbon capture & sequestration (CCS), prevents CO2 from entering the atmosphere but likewise does not reduce existing levels of atmospheric CO2. Biological sequestration (ocean or terrestrial) physically removes CO2 from the atmosphere. Since we cannot shut down our global economy, urgent action is needed to counteract CO2 emissions, and avoid catastrophic climate change. Given the long lead time and/or small impact of offsetting energy sources, sequestration is the only way to achieve near and medium-term reductions in atmospheric CO2 levels. To finance massive-scale sequestration of CO2, we propose the World Trade Organization (WTO) become an active player in the sequestration market. Given the WTO's role as overseer of international trade agreements annually representing 30 trillion in imports and exports of goods and services, it is by far the largest global economic force and therefore offers the broadest economic base. Absent a real solution to CO2 emissions, the global economy - and world trade - will shrink dramatically. The WTO can jumpstart the market for CO2 sequestration by issuing long term contracts to purchase bona fide sequestration-derived CO2 credits. Under this proposal, an initial price of 100 per ton which steps-down by 5% per year could bring forth the sequestration investment needed to achieve upwards of 10 billion tons sequestered CO2 per year by 2025 (seven billion tons from biological ocean sequestration and at least three billion tons from geologic and terrestrial sequestration). Assuming a contract term of 40 years, and a parallel commodity market continues to develop for CO2 credits, at some time in the future the WTO's contractual price will be less than the commodity market price - and the WTO begins to recover its investment. Under one set of assumptions, the net WTO annual subsidy would peak at $86 billion by 2022, equal to an across-the-board WTO tariff on imports and exports of about 1.01%, then become positive a few years later as the market price climbed above WTO's contracted price. Under this proposal, the WTO effectively subsidizes CO2 sequestration in the near to medium term and then recoups its investment and reaps large profits over the long term.
Large-scale CO2 storage — Is it feasible?
NASA Astrophysics Data System (ADS)
Johansen, H.
2013-06-01
CCS is generally estimated to have to account for about 20% of the reduction of CO2 emissions to the atmosphere. This paper focuses on the technical aspects of CO2 storage, even if the CCS challenge is equally dependent upon finding viable international solutions to a wide range of economic, political and cultural issues. It has already been demonstrated that it is technically possible to store adequate amounts of CO2 in the subsurface (Sleipner, InSalah, Snøhvit). The large-scale storage challenge (several Gigatons of CO2 per year) is more an issue of minimizing cost without compromising safety, and of making international regulations.The storage challenge may be split into 4 main parts: 1) finding reservoirs with adequate storage capacity, 2) make sure that the sealing capacity above the reservoir is sufficient, 3) build the infrastructure for transport, drilling and injection, and 4) set up and perform the necessary monitoring activities. More than 150 years of worldwide experience from the production of oil and gas is an important source of competence for CO2 storage. The storage challenge is however different in three important aspects: 1) the storage activity results in pressure increase in the subsurface, 2) there is no production of fluids that give important feedback on reservoir performance, and 3) the monitoring requirement will have to extend for a much longer time into the future than what is needed during oil and gas production. An important property of CO2 is that its behaviour in the subsurface is significantly different from that of oil and gas. CO2 in contact with water is reactive and corrosive, and may impose great damage on both man-made and natural materials, if proper precautions are not executed. On the other hand, the long-term effect of most of these reactions is that a large amount of CO2 will become immobilized and permanently stored as solid carbonate minerals. The reduced opportunity for direct monitoring of fluid samples close to the reservoir, the general pressure build up, and the reactive nature of CO2, have created a need for new research and knowledge, to be used in conjunction with operating competence from the oil and gas industry. Experimental work on fluid flow, deformation and reaction, as well as simulations to predict the future performance of the injected CO2, are much more important in connection with CO2 storage, as compared with conventional oil and gas production. To conclude this overview of the CO2 storage challenge, the technical feasibility of large-scale CO2 storage has been demonstrated. The cost is however going to be significant, especially in the initial phase. The public acceptance of CCS, and the willingness to pay the bill, will depend on several important factors: a serious acceptance of the climate problem, economic and political regulations that are globally fair, and the willingness of each and one of us to accept a higher price for energy.
Zeng, Jianfei; Shen, Xiuli; Sun, Xiaoxi; Liu, Ning; Han, Lujia; Huang, Guangqun
2018-05-01
With the advantages of high treatment capacity and low operational cost, large-scale trough composting has become one of the mainstream composting patterns in composting plants in China. This study measured concentrations of O 2 , CO 2 , CH 4 and NH 3 on-site to investigate the spatial and temporal distribution of pore gas concentrations during mainstream large-scale trough composting in China. The results showed that the temperature in the center of the pile was obviously higher than that in the side of the pile. Pore O 2 concentration rapidly decreased and maintained <5% (in volume) for 38 days or more in both the center and side of the pile and effective O 2 diffusion occurred at most in every two contiguous layers. Pore CO 2 and CH 4 concentrations at each measurement point were positively correlated (0.436 ≤ r ≤ 0.570, P < 0.01) and the concentrations in the side of the pile were obviously lower than those in the center. The top layer exhibited highest pore O 2 concentration and lowest CO 2 and CH 4 concentrations, and the bottom layer was on the contrary. No significant differences in pore NH 3 concentrations between different layers or between different measurement points in the same layer were found. Therefore, mixing the center and the side of the pile when mechanical turning and adjusting the height of the pile according to the physical properties of bulking agents are suggested to optimize the oxygen distribution and promote the composting process during large-scale trough composting when the pile was naturally aerated, which will contribute to improving the current undesirable atmosphere environment in China. Copyright © 2018 Elsevier Ltd. All rights reserved.
Fuel combustion adds to anxiety over CO/sub 2/ buildup
DOE Office of Scientific and Technical Information (OSTI.GOV)
Sleeper, D.
1979-08-01
In the past 20 y, the annual rate of increase of atmosphreic carbon dioxide has grown sharply because of increased fossil fuel combustion. Most scientists agree that CO/sub 2/ buildup in the atmosphere is causing a greenhouse effect, slowly warming the earth's climate. Large-scale production of synthetic fuels that could be combusted without releasing CO/sub 2/ is examined as a possible solution. 31 references, 1 figure.
High capacity immobilized amine sorbents
Gray, McMahan L [Pittsburgh, PA; Champagne, Kenneth J [Fredericktown, PA; Soong, Yee [Monroeville, PA; Filburn, Thomas [Granby, CT
2007-10-30
A method is provided for making low-cost CO.sub.2 sorbents that can be used in large-scale gas-solid processes. The improved method entails treating an amine to increase the number of secondary amine groups and impregnating the amine in a porous solid support. The method increases the CO.sub.2 capture capacity and decreases the cost of utilizing an amine-enriched solid sorbent in CO.sub.2 capture systems.
ALMA Reveals Molecular Cloud N55 in the Large Magellanic Cloud as a Site of Massive Star Formation
NASA Astrophysics Data System (ADS)
Naslim, N.; Tokuda, K.; Onishi, T.; Kemper, F.; Wong, T.; Morata, O.; Takada, S.; Harada, R.; Kawamura, A.; Saigo, K.; Indebetouw, R.; Madden, S. C.; Hony, S.; Meixner, M.
2018-02-01
We present the molecular cloud properties of N55 in the Large Magellanic Cloud using 12CO(1–0) and 13CO(1–0) observations obtained with Atacama Large Millimeter Array. We have done a detailed study of molecular gas properties, to understand how the cloud properties of N55 differ from Galactic clouds. Most CO emission appears clumpy in N55, and molecular cores that have young stellar objects (YSOs) show larger linewidths and masses. The massive clumps are associated with high and intermediate mass YSOs. The clump masses are determined by local thermodynamic equilibrium and virial analysis of the 12CO and 13CO emissions. These mass estimates lead to the conclusion that (a) the clumps are in self-gravitational virial equilibrium, and (b) the 12CO(1–0)-to-H2 conversion factor, {X}{CO}, is 6.5 × 1020 cm‑2 (K km s‑1)‑1. This CO-to-H2 conversion factor for N55 clumps is measured at a spatial scale of ∼0.67 pc, which is about two times higher than the {X}{CO} value of the Orion cloud at a similar spatial scale. The core mass function of N55 clearly show a turnover below 200 {M}ȯ , separating the low-mass end from the high-mass end. The low-mass end of the 12CO mass spectrum is fitted with a power law of index 0.5 ± 0.1, while for 13CO it is fitted with a power law index 0.6 ± 0.2. In the high-mass end, the core mass spectrum is fitted with a power index of 2.0 ± 0.3 for 12CO, and with 2.5 ± 0.4 for 13CO. This power law behavior of the core mass function in N55 is consistent with many Galactic clouds.
NASA Astrophysics Data System (ADS)
Clargo, Nicola; Salt, Lesley; Thomas, Helmuth; de Baar, Hein
2015-04-01
Since the industrial revolution, atmospheric concentrations of carbon dioxide (CO2) have risen dramatically, largely due to the combustion of fossil fuels, changes in land-use patterns and the production of cement. The oceans have absorbed a large amount of this CO2, with resulting impacts on ocean chemistry. Coastal seas play a significant role in the mitigation of anthropogenic atmospheric CO2 as they contribute approximately 10-30% of global primary productivity despite accounting for only 7% of the surface area. The North Sea is a perfect natural laboratory in which to study the CO2 system as it consists of two biogeochemically distinct regions displaying both oceanic and relatively coastal behaviour. It has also been identified as a continental shelf pump with respect to CO2, transporting it to the deeper waters of the North Atlantic. Large scale forcing has been shown to have a significant impact on the CO2 system over varying time scales, often masking the effects of anthropogenic influence. Here, we present data from the North Sea spanning the 2001-2011 decade. In order to investigate the dynamics of the dissolved CO2 system in this region in the face of climate change, four basin-wide cruises were conducted during the summers of 2001, 2005, 2008 and 2011. The acquired Dissolved Inorganic Carbon (DIC) and alkalinity data were then used to fully resolve the carbon system in order to assess trends over the 2001-2011 decade. We find significant interannual variability, but with a consistent, notable trend in decreasing pH. We found that surface alkalinity remained relatively constant over the decade, whereas DIC increased, indicating that the pH decline is DIC-driven. We also found that the partial pressure of CO2 (pCO2) increased faster than concurrent atmospheric CO2 concentrations, and that the CO2 buffering capacity of the North Sea decreased over the decade, with implications for future CO2 uptake.
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Chuan Lu; CHI Zhang; Hai Hanag
2014-04-01
Successful geological storage and sequestration of carbon dioxide (CO2) require efficient monitoring of the migration of CO2 plume during and after large-scale injection in order to verify the containment of the injected CO2 within the target formation and to evaluate potential leakage risk. Field studies have shown that surface and cross-borehole electrical resistivity tomography (ERT) can be a useful tool in imaging and characterizing solute transport in heterogeneous subsurface. In this synthetic study, we have coupled a 3-D multiphase flow model with a parallel 3-D time-lapse ERT inversion code to explore the feasibility of using time-lapse ERT for simultaneously monitoringmore » the migration of CO2 plume in deep saline formation and potential brine intrusion into shallow fresh water aquifer. Direct comparisons of the inverted CO2 plumes resulting from ERT with multiphase flow simulation results indicate the ERT could be used to delineate the migration of CO2 plume. Detailed comparisons on the locations, sizes and shapes of CO2 plume and intruded brine plumes suggest that ERT inversion tends to underestimate the area review of the CO2 plume, but overestimate the thickness and total volume of the CO2 plume. The total volume of intruded brine plumes is overestimated as well. However, all discrepancies remain within reasonable ranges. Our study suggests that time-lapse ERT is a useful monitoring tool in characterizing the movement of injected CO2 into deep saline aquifer and detecting potential brine intrusion under large-scale field injection conditions.« less
Scaling laws for perturbations in the ocean-atmosphere system following large CO2 emissions
NASA Astrophysics Data System (ADS)
Towles, N.; Olson, P.; Gnanadesikan, A.
2015-07-01
Scaling relationships are found for perturbations to atmosphere and ocean variables from large transient CO2 emissions. Using the Long-term Ocean-atmosphere-Sediment CArbon cycle Reservoir (LOSCAR) model (Zeebe et al., 2009; Zeebe, 2012b), we calculate perturbations to atmosphere temperature, total carbon, ocean temperature, total ocean carbon, pH, alkalinity, marine-sediment carbon, and carbon-13 isotope anomalies in the ocean and atmosphere resulting from idealized CO2 emission events. The peak perturbations in the atmosphere and ocean variables are then fit to power law functions of the form of γ DαEβ, where D is the event duration, E is its total carbon emission, and γ is a coefficient. Good power law fits are obtained for most system variables for E up to 50 000 PgC and D up to 100 kyr. Although all of the peak perturbations increase with emission rate E/D, we find no evidence of emission-rate-only scaling, α + β = 0. Instead, our scaling yields α + β ≃ 1 for total ocean and atmosphere carbon and 0 < α + β < 1 for most of the other system variables.
Carbon dioxide (CO2) sequestration in deep saline aquifers and formations: Chapter 3
Rosenbauer, Robert J.; Thomas, Burt
2010-01-01
Carbon dioxide (CO2) capture and sequestration in geologic media is one among many emerging strategies to reduce atmospheric emissions of anthropogenic CO2. This chapter looks at the potential of deep saline aquifers – based on their capacity and close proximity to large point sources of CO2 – as repositories for the geologic sequestration of CO2. The petrochemical characteristics which impact on the suitability of saline aquifers for CO2 sequestration and the role of coupled geochemical transport models and numerical tools in evaluating site feasibility are also examined. The full-scale commercial CO2 sequestration project at Sleipner is described together with ongoing pilot and demonstration projects.
Global carbon management using air capture and geosequestration at remote locations
NASA Astrophysics Data System (ADS)
Lackner, K. S.; Goldberg, D.
2014-12-01
CO2 emissions need not only stop; according the IPCC, emissions need to turn negative. This requires means to remove CO2 from air and store it safely and permanently. We outline a combination of secure geosequestration and direct capture of CO2 from ambient air to create negative emissions at remote locations. Operation at remote sites avoids many difficulties associated with capture at the source, where space for added equipment is limited, good storage sites are in short supply, and proximity to private property engenders resistance. Large Igneous Provinces have been tested as secure CO2 reservoirs. CO2 and water react with reservoir rock to form stable carbonates, permanently sequestering the carbon. Outfitting reservoirs in large igneous provinces far from human habitation with ambient air capture systems creates large CO2 sequestration sites. Their remoteness offers advantages in environmental security and public acceptance and, thus, can smooth the path toward CO2 stabilization. Direct capture of CO2 from ambient air appears energetically and economically viable and could be scaled up quickly. Thermodynamic energy requirements are very small and a number of approaches have shown to be energy efficient in practice. Sorbent technologies include supported organoamines, alkaline brines, and quaternary ammonium based ion-exchange resins. To demonstrate that the stated goals of low cost and low energy consumption can be reached at scale, public research and demonstration projects are essential. We suggest co-locating air capture and geosequestration at sites where renewable energy resources can power both activities. Ready renewable energy would also allow for the co-production of synthetic fuels. Possible locations with large wind and basalt resources include Iceland and Greenland, the north-western United States, the Kerguelen plateau, Siberia and Morocco. Capture and sequestration in these reservoirs could recover all of the emissions of the 20th century and still contribute to a carbon neutral economy throughout the 21st century. Mobilizing industrial infrastructure to these areas poses a challenge. However, the urgency of the climate problem requires immediate action, with economic incentives and commitments to site evaluation and engineering development.
Takayama, Kotaro; King, Diana; Robinson, Sharon A; Osmond, Barry
2013-11-01
Long-lived shade leaves of avocado had extremely low rates of photosynthesis. Gas exchange measurements of photosynthesis were of limited use, so we resorted to Chl fluorescence imaging (CFI) and spot measurements to evaluate photosynthetic electron transport rates (ETRs) and non-photochemical quenching (NPQ). Imaging revealed a remarkable transient heterogeneity of NPQ during photosynthetic induction in these hypostomatous, heterobaric leaves, but was adequately integrated by spot measurements, despite long-lasting artifacts from repeated saturating flashes during assays. Major veins (mid-vein, first- and second-order veins) defined areas of more static large-scale heterogeneous NPQ, with more dynamic small-scale heterogeneity most strongly expressed in mesophyll cells between third- and fourth-order veins. Both responded to external CO2 concentration ([CO2]), occlusion of stomata with Vaseline™, leaf dehydration and relative humidity (RH). We interpreted these responses in terms of independent behavior of stomata in adjacent areoles that was largely expressed through CO2-limited photosynthesis. Heterogeneity was most pronounced and prolonged in the absence of net CO2 fixation in 100 p.p.m. [CO2] when respiratory and photorespiratory CO2 cycling constrained the inferred ETR to ~75% of values in 400 or 700 p.p.m. [CO2]. Likewise, sustained higher NPQ under Vaseline™, after dehydration or at low RH, also restricted ETR to ~75% of control values. Low NPQ in chloroplast-containing cells adjacent to major veins but remote from stomata suggested internal sources of high [CO2] in these tissues.
Watershed-scale drivers of air-water CO2 exchanges in two lagoonal, North Carolina (USA) estuaries
NASA Astrophysics Data System (ADS)
Van Dam, B.; Crosswell, J.; Anderson, I. C.; Paerl, H. W.
2017-12-01
Riverine loading of nutrients and organic matter act in concert to modulate CO2 fluxes in estuaries, yet quantitative relationships between these factors remain poorly defined. This study explored watershed-scale mechanisms responsible for the relatively low CO2 fluxes observed in two microtidal, lagoonal estuaries. Air-water CO2 fluxes were quantified with 74 high-resolution spatial surveys in the neighboring New River Estuary (NewRE) and Neuse River Estuary (NeuseRE), North Carolina, which experience a common climatology, but differ in marine versus riverine influence. Annually, both estuaries were relatively small sources of CO2 to the atmosphere, 12.5 and 16.3 mmol C m2 d-1 in the NeuseRE and NewRE, respectively. Variations in riverine alkalinity and inorganic carbon loading caused zones of minimum buffering capacity to occur at different locations in each estuary, enhancing the sensitivity of estuarine inorganic C chemistry to acidification. Large-scale pCO2 variations were driven by changes in freshwater age (akin to residence time), which modulate nutrient and organic carbon supply and phytoplankton flushing. Greatest pCO2 under-saturation was observed at intermediate freshwater ages, between 2-3 weeks. Biological controls on CO2 fluxes were obscured by variable inputs of river-borne CO2, which drove CO2 degassing in the river-dominated NeuseRE. Internally produced CO2 exceeded river-borne CO2 in the marine-dominated NewRE, suggesting that net ecosystem heterotrophy, rather than riverine inputs, drove CO2 fluxes in this system. Although annual CO2 fluxes were similar between systems, watershed-specific hydrologic factors led to disparate controls on internal carbonate chemistry, which can influence overall ecosystem health and response to future perturbation.
Watershed-Scale Drivers of Air-Water CO2 Exchanges in Two Lagoonal North Carolina (USA) Estuaries
NASA Astrophysics Data System (ADS)
Van Dam, Bryce R.; Crosswell, Joseph R.; Anderson, Iris C.; Paerl, Hans W.
2018-01-01
Riverine loading of nutrients and organic matter act in concert to modulate CO2 fluxes in estuaries, yet quantitative relationships between these factors remain poorly defined. This study explored watershed-scale mechanisms responsible for the relatively low CO2 fluxes observed in two microtidal, lagoonal estuaries. Air-water CO2 fluxes were quantified with 74 high-resolution spatial surveys in the neighboring New River Estuary (NewRE) and Neuse River Estuary (NeuseRE), North Carolina, which experience a common climatology but differ in marine versus riverine influence. Annually, both estuaries were relatively small sources of CO2 to the atmosphere, 12.5 and 16.3 mmol C m-2 d-1 in the NeuseRE and NewRE, respectively. Large-scale pCO2 variations were driven by changes in freshwater age, which modulates nutrient and organic carbon supply and phytoplankton flushing. Greatest pCO2 undersaturation was observed at intermediate freshwater ages, between 2 and 3 weeks. Biological controls on CO2 fluxes were obscured by variable inputs of river-borne CO2, which drove CO2 degassing in the river-dominated NeuseRE. Internally produced CO2 exceeded river-borne CO2 in the marine-dominated NewRE, suggesting that net ecosystem heterotrophy, rather than riverine inputs, drove CO2 fluxes in this system. Variations in riverine alkalinity and inorganic carbon loading caused zones of minimum buffering capacity to occur at different locations in each estuary, enhancing the sensitivity of estuarine inorganic C chemistry to acidification. Although annual CO2 fluxes were similar between systems, watershed-specific hydrologic factors led to disparate controls on internal carbonate chemistry, which can influence ecosystem biogeochemical cycling, trophic state, and response to future perturbations.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Illangasekare, Tissa; Trevisan, Luca; Agartan, Elif
2015-03-31
Carbon Capture and Storage (CCS) represents a technology aimed to reduce atmospheric loading of CO 2 from power plants and heavy industries by injecting it into deep geological formations, such as saline aquifers. A number of trapping mechanisms contribute to effective and secure storage of the injected CO 2 in supercritical fluid phase (scCO 2) in the formation over the long term. The primary trapping mechanisms are structural, residual, dissolution and mineralization. Knowledge gaps exist on how the heterogeneity of the formation manifested at all scales from the pore to the site scales affects trapping and parameterization of contributing mechanismsmore » in models. An experimental and modeling study was conducted to fill these knowledge gaps. Experimental investigation of fundamental processes and mechanisms in field settings is not possible as it is not feasible to fully characterize the geologic heterogeneity at all relevant scales and gathering data on migration, trapping and dissolution of scCO 2. Laboratory experiments using scCO 2 under ambient conditions are also not feasible as it is technically challenging and cost prohibitive to develop large, two- or three-dimensional test systems with controlled high pressures to keep the scCO 2 as a liquid. Hence, an innovative approach that used surrogate fluids in place of scCO 2 and formation brine in multi-scale, synthetic aquifers test systems ranging in scales from centimeter to meter scale developed used. New modeling algorithms were developed to capture the processes controlled by the formation heterogeneity, and they were tested using the data from the laboratory test systems. The results and findings are expected to contribute toward better conceptual models, future improvements to DOE numerical codes, more accurate assessment of storage capacities, and optimized placement strategies. This report presents the experimental and modeling methods and research results.« less
Overview of Opportunities for Co-Location of Solar Energy Technologies and Vegetation
DOE Office of Scientific and Technical Information (OSTI.GOV)
Macknick, Jordan; Beatty, Brenda; Hill, Graham
2013-12-01
Large-scale solar facilities have the potential to contribute significantly to national electricity production. Many solar installations are large-scale or utility-scale, with a capacity over 1 MW and connected directly to the electric grid. Large-scale solar facilities offer an opportunity to achieve economies of scale in solar deployment, yet there have been concerns about the amount of land required for solar projects and the impact of solar projects on local habitat. During the site preparation phase for utility-scale solar facilities, developers often grade land and remove all vegetation to minimize installation and operational costs, prevent plants from shading panels, and minimizemore » potential fire or wildlife risks. However, the common site preparation practice of removing vegetation can be avoided in certain circumstances, and there have been successful examples where solar facilities have been co-located with agricultural operations or have native vegetation growing beneath the panels. In this study we outline some of the impacts that large-scale solar facilities can have on the local environment, provide examples of installations where impacts have been minimized through co-location with vegetation, characterize the types of co-location, and give an overview of the potential benefits from co-location of solar energy projects and vegetation. The varieties of co-location can be replicated or modified for site-specific use at other solar energy installations around the world. We conclude with opportunities to improve upon our understanding of ways to reduce the environmental impacts of large-scale solar installations.« less
Integrated Mid-Continent Carbon Capture, Sequestration & Enhanced Oil Recovery Project
DOE Office of Scientific and Technical Information (OSTI.GOV)
Brian McPherson
2010-08-31
A consortium of research partners led by the Southwest Regional Partnership on Carbon Sequestration and industry partners, including CAP CO2 LLC, Blue Source LLC, Coffeyville Resources, Nitrogen Fertilizers LLC, Ash Grove Cement Company, Kansas Ethanol LLC, Headwaters Clean Carbon Services, Black & Veatch, and Schlumberger Carbon Services, conducted a feasibility study of a large-scale CCS commercialization project that included large-scale CO{sub 2} sources. The overall objective of this project, entitled the 'Integrated Mid-Continent Carbon Capture, Sequestration and Enhanced Oil Recovery Project' was to design an integrated system of US mid-continent industrial CO{sub 2} sources with CO{sub 2} capture, and geologicmore » sequestration in deep saline formations and in oil field reservoirs with concomitant EOR. Findings of this project suggest that deep saline sequestration in the mid-continent region is not feasible without major financial incentives, such as tax credits or otherwise, that do not exist at this time. However, results of the analysis suggest that enhanced oil recovery with carbon sequestration is indeed feasible and practical for specific types of geologic settings in the Midwestern U.S.« less
Cities, traffic, and CO2: A multidecadal assessment of trends, drivers, and scaling relationships
Gately, Conor K.; Hutyra, Lucy R.; Sue Wing, Ian
2015-01-01
Emissions of CO2 from road vehicles were 1.57 billion metric tons in 2012, accounting for 28% of US fossil fuel CO2 emissions, but the spatial distributions of these emissions are highly uncertain. We develop a new emissions inventory, the Database of Road Transportation Emissions (DARTE), which estimates CO2 emitted by US road transport at a resolution of 1 km annually for 1980–2012. DARTE reveals that urban areas are responsible for 80% of on-road emissions growth since 1980 and for 63% of total 2012 emissions. We observe nonlinearities between CO2 emissions and population density at broad spatial/temporal scales, with total on-road CO2 increasing nonlinearly with population density, rapidly up to 1,650 persons per square kilometer and slowly thereafter. Per capita emissions decline as density rises, but at markedly varying rates depending on existing densities. We make use of DARTE’s bottom-up construction to highlight the biases associated with the common practice of using population as a linear proxy for disaggregating national- or state-scale emissions. Comparing DARTE with existing downscaled inventories, we find biases of 100% or more in the spatial distribution of urban and rural emissions, largely driven by mismatches between inventory downscaling proxies and the actual spatial patterns of vehicle activity at urban scales. Given cities’ dual importance as sources of CO2 and an emerging nexus of climate mitigation initiatives, high-resolution estimates such as DARTE are critical both for accurately quantifying surface carbon fluxes and for verifying the effectiveness of emissions mitigation efforts at urban scales. PMID:25847992
Exploring precipitation pattern scaling methodologies and robustness among CMIP5 models
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kravitz, Ben; Lynch, Cary; Hartin, Corinne
Pattern scaling is a well-established method for approximating modeled spatial distributions of changes in temperature by assuming a time-invariant pattern that scales with changes in global mean temperature. We compare two methods of pattern scaling for annual mean precipitation (regression and epoch difference) and evaluate which method is better in particular circumstances by quantifying their robustness to interpolation/extrapolation in time, inter-model variations, and inter-scenario variations. Both the regression and epoch-difference methods (the two most commonly used methods of pattern scaling) have good absolute performance in reconstructing the climate model output, measured as an area-weighted root mean square error. We decomposemore » the precipitation response in the RCP8.5 scenario into a CO 2 portion and a non-CO 2 portion. Extrapolating RCP8.5 patterns to reconstruct precipitation change in the RCP2.6 scenario results in large errors due to violations of pattern scaling assumptions when this CO 2-/non-CO 2-forcing decomposition is applied. As a result, the methodologies discussed in this paper can help provide precipitation fields to be utilized in other models (including integrated assessment models or impacts assessment models) for a wide variety of scenarios of future climate change.« less
Exploring precipitation pattern scaling methodologies and robustness among CMIP5 models
Kravitz, Ben; Lynch, Cary; Hartin, Corinne; ...
2017-05-12
Pattern scaling is a well-established method for approximating modeled spatial distributions of changes in temperature by assuming a time-invariant pattern that scales with changes in global mean temperature. We compare two methods of pattern scaling for annual mean precipitation (regression and epoch difference) and evaluate which method is better in particular circumstances by quantifying their robustness to interpolation/extrapolation in time, inter-model variations, and inter-scenario variations. Both the regression and epoch-difference methods (the two most commonly used methods of pattern scaling) have good absolute performance in reconstructing the climate model output, measured as an area-weighted root mean square error. We decomposemore » the precipitation response in the RCP8.5 scenario into a CO 2 portion and a non-CO 2 portion. Extrapolating RCP8.5 patterns to reconstruct precipitation change in the RCP2.6 scenario results in large errors due to violations of pattern scaling assumptions when this CO 2-/non-CO 2-forcing decomposition is applied. As a result, the methodologies discussed in this paper can help provide precipitation fields to be utilized in other models (including integrated assessment models or impacts assessment models) for a wide variety of scenarios of future climate change.« less
Stochastic Modeling of CO2 Migrations and Chemical Reactions in Deep Saline Formations
NASA Astrophysics Data System (ADS)
Ni, C.; Lee, I.; Lin, C.
2013-12-01
Carbon capture and storage (CCS) has been recognized the feasible technology that can significant reduce the anthropogenic CO2 emissions from large point sources. The CO2 injection in geological formations is one of the options to permanently store the captured CO2. Based on this concept a large number of target formations have been identified and intensively investigated with different types of techniques such as the hydrogeophysical experiments or numerical simulations. The numerical simulations of CO2 migrations in saline formations recently gather much attention because a number of models are available for this purpose and there are potential sites existing in many countries. The lower part of Cholan Formation (CF) near Changhua Coastal Industrial Park (CCIP) in west central Taiwan was identified the largest potential site for CO2 sequestration. The top elevations of the KF in this area varies from 1300 to 1700m below the sea level. Laboratory experiment showed that the permeability of CF is 10-14 to 10-12 m2. Over the years the offshore seismic survey and limited onshore borehole logs have provided information for the simulation of CO2 migration in the CF although the original investigations might not focus on the purpose of CO2 sequestration. In this study we modify the TOUGHREACT model to consider the small-scale heterogeneity in target formation and the cap rock of upper CF. A Monte Carlo Simulation (MCS) approach based on the TOUGHREACT model is employed to quantify the effect of small-scale heterogeneity on the CO2 migrations and hydrochemical reactions in the CF. We assume that the small-scale variability of permeability in KF can be described with a known Gaussian distribution. Therefore, the Gaussian type random field generator such as Sequential Gaussian Simulation (SGSIM) in Geostatistical Software Library (GSLIB) can be used to provide the random permeability realizations for the MCS. A variety of statistical parameters such as the variances and correlation lengths in a Gaussian covariance model are varied in the MCS and the uncertainty of the CO2 and other chemical concentrations are evaluated based on 144 random realizations. In this study a constant injection rate of100Mt/year supercritical CO2 is applied in the bottom of CF. The continuous injection time is 20 years and the uncertainty results are evaluated at 100 years. By comparing with the case without small-scale variability simulation results show that the CO2 plume sizes in the horizontal direction increase from tens of meters to hundreds of meters when the variances of small-scale variability are varied from 1.0 to 4.0. The changes of correlation lengths (i.e., from 100m, 200m, to 400m) show small contribution on the size increases of CO2 plumes. Other uncertainties of chemical concentrations show behaviors similar to the CO2 plume patterns.
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.
NASA Astrophysics Data System (ADS)
Strefler, Jessica; Bauer, Nico; Kriegler, Elmar; Popp, Alexander; Giannousakis, Anastasis; Edenhofer, Ottmar
2018-04-01
There are major concerns about the sustainability of large-scale deployment of carbon dioxide removal (CDR) technologies. It is therefore an urgent question to what extent CDR will be needed to implement the long term ambition of the Paris Agreement. Here we show that ambitious near term mitigation significantly decreases CDR requirements to keep the Paris climate targets within reach. Following the nationally determined contributions (NDCs) until 2030 makes 2 °C unachievable without CDR. Reducing 2030 emissions by 20% below NDC levels alleviates the trade-off between high transitional challenges and high CDR deployment. Nevertheless, transitional challenges increase significantly if CDR is constrained to less than 5 Gt CO2 a‑1 in any year. At least 8 Gt CO2 a‑1 CDR are necessary in the long term to achieve 1.5 °C and more than 15 Gt CO2 a‑1 to keep transitional challenges in bounds.
Ramesh Murthy; Greg Barron-Gafford; Philip M. Dougherty; Victor c. Engels; Katie Grieve; Linda Handley; Christie Klimas; Mark J. Postosnaks; Stanley J. Zarnoch; Jianwei Zhang
2005-01-01
We examined the effects of atmospheric vapor pressure deficit (VPD) and soil moisture stress (SMS) on leaf- and stand-level CO2 exchange in model 3-year-old coppiced cottonwood (Populus deltoides Bartr.) plantations using the large-scale, controlled environments of the Biosphere 2 Laboratory. A short-term experiment was imposed...
Additive free preparative chiral SFC separations of 2,2-dimethyl-3-aryl-propanoic acids.
Wu, Dauh-Rurng; Yip, Shiuhang Henry; Li, Peng; Sun, Dawn; Kempson, James; Mathur, Arvind
2016-11-30
A series of racemic 2,2-dimethyl-3-aryl-propanoic acids were resolved by chiral supercritical fluid chromatography (SFC) without the use of an acidic additive, trifluoroacetic acid (TFA). The use of additive-free protic methanol as co-solvent in CO 2 was expanded to successfully resolve other series of carboxylic acid containing racemates. Large-scale SFC of racemic acid 4, 3-(1-(4-fluorophenyl)-1H-indazol-5-yl)-2,2-dimethyl-3-phenylpropanoic acid, in methanol without TFA as additive on both Chiralpak AD-H and Chiralcel OJ-H will be discussed, along with impact on throughput and solvent consumption. Investigation of co-solvent effect on peak sharpening of acid racemate 20, 2-(2-chloro-9-fluoro-5H-chromeno[2,3-b]pyridin-5-yl)-2-methylpropanoic acid, without TFA further indicated that methanol in CO 2 provided improved peak shape compared with isopropanol (IPA) and acetonitrile. Finally, we discuss the resolution of basic aromatic chiral amines without the addition of basic additives such as diethylamine (DEA) and application of this protocol for the large-scale SFC separation of weakly basic indazole-containing racemate 14, methyl 3-(1H-indazol-5-yl)-2,2-dimethyl-3-phenylpropanoate, in methanol without DEA. Copyright © 2016 Elsevier B.V. All rights reserved.
Large temporal scale and capacity subsurface bulk energy storage with CO2
NASA Astrophysics Data System (ADS)
Saar, M. O.; Fleming, M. R.; Adams, B. M.; Ogland-Hand, J.; Nelson, E. S.; Randolph, J.; Sioshansi, R.; Kuehn, T. H.; Buscheck, T. A.; Bielicki, J. M.
2017-12-01
Decarbonizing energy systems by increasing the penetration of variable renewable energy (VRE) technologies requires efficient and short- to long-term energy storage. Very large amounts of energy can be stored in the subsurface as heat and/or pressure energy in order to provide both short- and long-term (seasonal) storage, depending on the implementation. This energy storage approach can be quite efficient, especially where geothermal energy is naturally added to the system. Here, we present subsurface heat and/or pressure energy storage with supercritical carbon dioxide (CO2) and discuss the system's efficiency, deployment options, as well as its advantages and disadvantages, compared to several other energy storage options. CO2-based subsurface bulk energy storage has the potential to be particularly efficient and large-scale, both temporally (i.e., seasonal) and spatially. The latter refers to the amount of energy that can be stored underground, using CO2, at a geologically conducive location, potentially enabling storing excess power from a substantial portion of the power grid. The implication is that it would be possible to employ centralized energy storage for (a substantial part of) the power grid, where the geology enables CO2-based bulk subsurface energy storage, whereas the VRE technologies (solar, wind) are located on that same power grid, where (solar, wind) conditions are ideal. However, this may require reinforcing the power grid's transmission lines in certain parts of the grid to enable high-load power transmission from/to a few locations.
Ye, Siyuan; Krauss, Ken W; Brix, Hans; Wei, Mengjie; Olsson, Linda; Yu, Xueyang; Ma, Xueying; Wang, Jin; Yuan, Hongming; Zhao, Guangming; Ding, Xigui; Moss, Rebecca F
2016-01-01
Global management of wetlands to suppress greenhouse gas (GHG) emissions, facilitate carbon (C) sequestration, and reduce atmospheric CO2 concentrations while simultaneously promoting agricultural gains is paramount. However, studies that relate variability in CO2 and CH4 emissions at large spatial scales are limited. We investigated three-year emissions of soil CO2 and CH4 from the primary wetland types of the Liaohe Delta, China, by focusing on a total wetland area of 3287 km2. One percent is Suaeda salsa, 24% is Phragmites australis, and 75% is rice. While S. salsa wetlands are under somewhat natural tidal influence, P. australis and rice are managed hydrologically for paper and food, respectively. Total C emissions from CO2 and CH4 from these wetland soils were 2.9 Tg C/year, ranging from 2.5 to 3.3 Tg C/year depending on the year assessed. Primary emissions were from CO2 (~98%). Photosynthetic uptake of CO2 would mitigate most of the soil CO2 emissions, but CH4 emissions would persist. Overall, CH4 fluxes were high when soil temperatures were >18°C and pore water salinity <18 PSU. CH4 emissions from rice habitat alone in the Liaohe Delta represent 0.2% of CH4 carbon emissions globally from rice. With such a large area and interannual sensitivity in soil GHG fluxes, management practices in the Delta and similar wetlands around the world have the potential not only to influence local C budgeting, but also to influence global biogeochemical cycling.
Ye, Siyuan; Krauss, Ken W.; Brix, Hans; Wei, Mengjie; Olsson, Linda; Yu, Xueyang; Ma, Xueying; Wang, Jin; Yuan, Hongming; Zhao, Guangming; Ding, Xigui; Moss, Rebecca F.
2016-01-01
Global management of wetlands to suppress greenhouse gas (GHG) emissions, facilitate carbon (C) sequestration, and reduce atmospheric CO2 concentrations while simultaneously promoting agricultural gains is paramount. However, studies that relate variability in CO2 and CH4 emissions at large spatial scales are limited. We investigated three-year emissions of soil CO2 and CH4 from the primary wetland types of the Liaohe Delta, China, by focusing on a total wetland area of 3287 km2. One percent is Suaeda salsa, 24% is Phragmites australis, and 75% is rice. While S. salsa wetlands are under somewhat natural tidal influence, P. australis and rice are managed hydrologically for paper and food, respectively. Total C emissions from CO2 and CH4 from these wetland soils were 2.9 Tg C/year, ranging from 2.5 to 3.3 Tg C/year depending on the year assessed. Primary emissions were from CO2 (~98%). Photosynthetic uptake of CO2 would mitigate most of the soil CO2 emissions, but CH4 emissions would persist. Overall, CH4 fluxes were high when soil temperatures were >18°C and pore water salinity <18 PSU. CH4 emissions from rice habitat alone in the Liaohe Delta represent 0.2% of CH4 carbon emissions globally from rice. With such a large area and interannual sensitivity in soil GHG fluxes, management practices in the Delta and similar wetlands around the world have the potential not only to influence local C budgeting, but also to influence global biogeochemical cycling. PMID:27501148
Primary, secondary, and tertiary amines for CO2 capture: designing for mesoporous CO2 adsorbents.
Ko, Young Gun; Shin, Seung Su; Choi, Ung Su
2011-09-15
CO(2) emissions, from fossil-fuel-burning power plants, the breathing, etc., influence the global worming on large scale and the man's work efficiency on small scale. The reversible capture of CO(2) is a prominent feature of CO(2) organic-inorganic hybrid adsorbent to sequester CO(2). Herein, (3-aminopropyl) trimethoxysilane (APTMS), [3-(methylamino)propyl] trimethoxysilane (MAPTMS), and [3-(diethylamino) propyl] trimethoxysilane (DEAPTMS) are immobilized on highly ordered mesoporous silicas (SBA-15) to catch CO(2) as primary, secondary, and tertiary aminosilica adsorbents. X-ray photoelectron spectroscopy was used to analyze the immobilized APTMS, MAPTMS, and DEAPTMS on the SBA-15. We report an interesting discovery that the CO(2) adsorption and desorption on the adsorbent depend on the amine type of the aminosilica adsorbent. The adsorbed CO(2) was easily desorbed from the adsorbent with the low energy consumption in the order of tertiary, secondary, and primary amino-adsorbents while the adsorption amount and the bonding-affinity increased in the reverse order. The effectiveness of amino-functionalized (1(o), 2(o), and 3(o) amines) SBA-15s as a CO(2) capturing agent was investigated in terms of adsorption capacity, adsorption-desorption kinetics, and thermodynamics. This work demonstrates apt amine types to catch CO(2) and regenerate the adsorbent, which may open new avenues to designing "CO(2) basket". Copyright © 2011. Published by Elsevier Inc.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Keeling, Ralph F.
The major goal of this project was to improve understanding of processes that control the exchanges of CO 2 between the atmosphere and the land biosphere on decadal and longer time scales. The approach involves measuring the changes in atmospheric CO 2 concentration and the isotopes of CO 2 ( 13C/ 12C and 18O/ 16O) at background stations and uses these and other datasets to challenge and improve numerical models of the earth system. The project particularly emphasized the use of these data to improve understanding of changes occurring in boreal and arctic ecosystems over the past 50 years andmore » to seek from these data improved understanding of large-scale processes impacting carbon cycling, such as the responses to warming, CO 2 fertilization, and disturbance. The project also led to advances in the understanding of changes in water-use efficiency of land ecosystems globally based on trends in 13C/ 12C. The core element of this project was providing partial support for continuing measurements of CO 2 concentrations and isotopes from the Scripps CO 2 program, initiated by C. D. Keeling in the 1960s. The measurements included analysis of flasks collected at an array of ten stations distributed from the Arctic to the Antarctic. The project also supported modeling studies and interpretive work to help understand the origins of the large ~50% increase in the amplitude of the atmospheric CO 2 cycle detected at high northern latitudes between 1960 and present and to understand the long-term trend in carbon 13C/ 12C of CO 2. The seasonal cycle work was advanced through collaborations with colleagues at MPI Jena and Imperial College« less
Carbon dioxide recycling: emerging large-scale technologies with industrial potential.
Quadrelli, Elsje Alessandra; Centi, Gabriele; Duplan, Jean-Luc; Perathoner, Siglinda
2011-09-19
This Review introduces this special issue of ChemSusChem dedicated to CO(2) recycling. Its aim is to offer an up-to-date overview of CO(2) chemical utilization (inorganic mineralization, organic carboxylation, reduction reactions, and biochemical conversion), as a continuation and extension of earlier books and reviews on this topic, but with a specific focus on large-volume routes and projects/pilot plants that are currently emerging at (pre-)industrial level. The Review also highlights how some of these routes will offer a valuable opportunity to introduce renewable energy into the existing energy and chemical infrastructure (i.e., "drop-in" renewable energy) by synthesis of chemicals from CO(2) that are easy to transport and store. CO(2) conversion therefore has the potential to become a key pillar of the sustainable and resource-efficient production of chemicals and energy from renewables. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Influence of local capillary trapping on containment system effectiveness
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bryant, Steven
2014-03-31
Immobilization of CO 2 injected into deep subsurface storage reservoirs is a critical component of risk assessment for geologic CO 2 storage (GCS). Local capillary trapping (LCT) is a recently established mode of immobilization that arises when CO 2 migrates due to buoyancy through heterogeneous storage reservoirs. This project sought to assess the amount and extent of LCT expected in storage formations under a range of injection conditions, and to confirm the persistence of LCT if the seal overlying the reservoir were to lose its integrity. Numerical simulation using commercial reservoir simulation software was conducted to assess the influence ofmore » injection. Laboratory experiments, modeling and numerical simulation were conducted to assess the effect of compromised seal integrity. Bench-scale (0.6 m by 0.6 m by 0.03 m) experiments with surrogate fluids provided the first empirical confirmation of the key concepts underlying LCT: accumulation of buoyant nonwetting phase at above residual saturations beneath capillary barriers in a variety of structures, which remains immobile under normal capillary pressure gradients. Immobilization of above-residual saturations is a critical distinction between LCT and the more familiar “residual saturation trapping.” To estimate the possible extent of LCT in a storage reservoir an algorithm was developed to identify all potential local traps, given the spatial distribution of capillary entry pressure in the reservoir. The algorithm assumes that the driving force for CO 2 migration can be represented as a single value of “critical capillary entry pressure” P c,entry crit, such that cells with capillary entry pressure greater/less than P c,entry crit act as barriers/potential traps during CO 2 migration. At intermediate values of P c,entry crit, the barrier regions become more laterally extensive in the reservoir, approaching a percolation threshold while non-barrier regions remain numerous. The maximum possible extent of LCT thus occurs at P c,entry crit near this threshold. Testing predictions of this simple algorithm against full-physics simulations of buoyancy-driven CO 2 migration support the concept of critical capillary entry pressure. However, further research is needed to determine whether a single value of critical capillary entry pressure always applies and how that value can be determined a priori. Simulations of injection into high-resolution (cells 0.3 m on a side) 2D and 3D heterogeneous domains show two characteristic behaviors. At small gravity numbers (vertical flow velocity much less than horizontal flow velocity) the CO 2 fills local traps as well as regions that would act as local barriers if CO 2 were moving only due to buoyancy. When injection ceases, the CO 2 migrates vertically to establish large saturations within local traps and residual saturation elsewhere. At large gravity numbers, the CO 2 invades a smaller portion of the perforated interval. Within this smaller swept zone the local barriers are not invaded, but local traps are filled to large saturation during injection and remain during post-injection gravity-driven migration. The small gravity number behavior is expected in the region within 100 m of a vertical injection well at anticipated rates of injection for commercial GCS. Simulations of leakage scenarios (through-going region of large permeability imposed in overlying seal) indicate that LCT persists (i.e. CO 2 remains held in a large fraction of the local iv traps) and the persistence is independent of injection rate during storage. Simulations of leakage for the limiting case of CO 2 migrating vertically from an areally extensive emplacement in the lower portion of a reservoir showed similar strong persistence of LCT. This research has two broad implications for GCS. The first is that LCT can retain a significant fraction of the CO 2 stored in a reservoir – above and beyond the residual saturation -- if the overlying seal were to fail. Thus frameworks for risk assessment should be extended to account for LCT. The second implication is that compared to pressure driven flow in reservoirs, CO 2 migration and trapping behave in a qualitatively different manner in heterogeneous reservoirs when buoyancy is the dominant driving force for flow. Thus simulations of GCS that neglect capillary heterogeneity will fail to capture important features of the CO 2 plume. While commercial reservoir simulation software can account for fine scale capillary heterogeneity, it has not been designed to work efficiently with such domains, and no simulators can handle fine-scale resolution throughout the reservoir. A possible way to upscale the migration and trapping is to apply an “effective residual saturation” to coarse-scale grids. While the extent of overall immobilization can be correlated in this way, all coarser grids failed to capture the distance traveled by the migrating CO 2 for large gravity number. Thus it remains unclear how best to account for LCT in the routine simulation work-flow that will be needed for large-scale GCS. Alternatives meriting investigation include streamline methods, reduced-physics proxies (e.g. particle tracking), and biased invasion percolation algorithms, which are based on precisely the capillary heterogeneity essential for LCT.« less
Large CO 2 and CH 4 emissions from polygonal tundra during spring thaw in northern Alaska
Raz-Yaseef, Naama; Torn, Margaret S.; Wu, Yuxin; ...
2016-12-05
The few prethaw observations of tundra carbon fluxes suggest that there may be large spring releases, but little is known about the scale and underlying mechanisms of this phenomenon. To address these questions, we combined in this paper ecosystem eddy flux measurements from two towers near Barrow, Alaska, with mechanistic soil-core thawing experiment. During a 2 week period prior to snowmelt in 2014, large fluxes were measured, reducing net summer uptake of CO 2 by 46% and adding 6% to cumulative CH 4 emissions. Emission pulses were linked to unique rain-on-snow events enhancing soil cracking. Controlled laboratory experiment revealed thatmore » as surface ice thaws, an immediate, large pulse of trapped gases is emitted. Finally, these results suggest that the Arctic CO 2 and CH 4 spring pulse is a delayed release of biogenic gas production from the previous fall and that the pulse can be large enough to offset a significant fraction of the moderate Arctic tundra carbon sink.« less
Carbon dioxide efficiency of terrestrial enhanced weathering.
Moosdorf, Nils; Renforth, Phil; Hartmann, Jens
2014-05-06
Terrestrial enhanced weathering, the spreading of ultramafic silicate rock flour to enhance natural weathering rates, has been suggested as part of a strategy to reduce global atmospheric CO2 levels. We budget potential CO2 sequestration against associated CO2 emissions to assess the net CO2 removal of terrestrial enhanced weathering. We combine global spatial data sets of potential source rocks, transport networks, and application areas with associated CO2 emissions in optimistic and pessimistic scenarios. The results show that the choice of source rocks and material comminution technique dominate the CO2 efficiency of enhanced weathering. CO2 emissions from transport amount to on average 0.5-3% of potentially sequestered CO2. The emissions of material mining and application are negligible. After accounting for all emissions, 0.5-1.0 t CO2 can be sequestered on average per tonne of rock, translating into a unit cost from 1.6 to 9.9 GJ per tonne CO2 sequestered by enhanced weathering. However, to control or reduce atmospheric CO2 concentrations substantially with enhanced weathering would require very large amounts of rock. Before enhanced weathering could be applied on large scales, more research is needed to assess weathering rates, potential side effects, social acceptability, and mechanisms of governance.
Cities, traffic, and CO 2: A multidecadal assessment of trends, drivers, and scaling relationships
Gately, Conor K.; Hutyra, Lucy R.; Sue Wing, Ian
2015-04-06
Emissions of CO 2 from road vehicles were 1.57 billion metric tons in 2012, accounting for 28% of US fossil fuel CO 2 emissions, but the spatial distributions of these emissions are highly uncertain. We develop a new emissions inventory, the Database of Road Transportation Emissions (DARTE), which estimates CO 2 emitted by US road transport at a resolution of 1 km annually for 1980-2012. DARTE reveals that urban areas are responsible for 80% of on-road emissions growth since 1980 and for 63% of total 2012 emissions. We observe nonlinearities between CO 2 emissions and population density at broad spatial/temporalmore » scales, with total on-road CO 2 increasing nonlinearly with population density, rapidly up to 1,650 persons per square kilometer and slowly thereafter. Per capita emissions decline as density rises, but at markedly varying rates depending on existing densities. Here, we make use of DARTE's bottom-up construction to highlight the biases associated with the common practice of using population as a linear proxy for disaggregating national- or state-scale emissions. Comparing DARTE with existing downscaled inventories, we find biases of 100% or more in the spatial distribution of urban and rural emissions, largely driven by mismatches between inventory downscaling proxies and the actual spatial patterns of vehicle activity at urban scales. Here, given cities' dual importance as sources of CO 2 and an emerging nexus of climate mitigation initiatives, high-resolution estimates such as DARTE are critical both for accurately quantifying surface carbon fluxes and for verifying the effectiveness of emissions mitigation efforts at urban scales.« less
SUBTASK 2.19 – OPERATIONAL FLEXIBILITY OF CO2 TRANSPORT AND STORAGE
DOE Office of Scientific and Technical Information (OSTI.GOV)
Jensen, Melanie; Schlasner, Steven; Sorensen, James
2014-12-31
Carbon dioxide (CO2) is produced in large quantities during electricity generation and by industrial processes. These CO2 streams vary in terms of both composition and mass flow rate, sometimes substantially. The impact of a varying CO2 stream on pipeline and storage operation is not fully understood in terms of either operability or infrastructure robustness. This study was performed to summarize basic background from the literature on the topic of operational flexibility of CO2 transport and storage, but the primary focus was on compiling real-world lessons learned about flexible operation of CO2 pipelines and storage from both large-scale field demonstrations andmore » commercial operating experience. Modeling and pilot-scale results of research in this area were included to illustrate some of the questions that exist relative to operation of carbon capture and storage (CCS) projects with variable CO2 streams. It is hoped that this report’s real-world findings provide readers with useful information on the topic of transport and storage of variable CO2 streams. The real-world results were obtained from two sources. The first source consisted of five full-scale, commercial transport–storage projects: Sleipner, Snøhvit, In Salah, Weyburn, and Illinois Basin–Decatur. These scenarios were reviewed to determine the information that is available about CO2 stream variability/intermittency on these demonstration-scale projects. The five projects all experienced mass flow variability or an interruption in flow. In each case, pipeline and/or injection engineers were able to accommodate any issues that arose. Significant variability in composition has not been an issue at these five sites. The second source of real- world results was telephone interviews conducted with experts in CO2 pipeline transport, injection, and storage during which commercial anecdotal information was acquired to augment that found during the literature search of the five full-scale projects. The experts represented a range of disciplines and hailed from North America and Europe. Major findings of the study are that compression and transport of CO2 for enhanced oil recovery (EOR) purposes in the United States has shown that impurities are not likely to cause transport problems if CO2 stream composition standards are maintained and pressures are kept at 10.3 MPa or higher. Cyclic, or otherwise intermittent, CO2 supplies historically have not impacted in-field distribution pipeline networks, wellbore integrity, or reservoir conditions. The U.S. EOR industry has demonstrated that it is possible to adapt to variability and intermittency in CO2 supply through flexible operation of the pipeline and geologic storage facility. This CO2 transport and injection experience represents knowledge that can be applied in future CCS projects. A number of gaps in knowledge were identified that may benefit from future research and development, further enhancing the possibility for widespread application of CCS. This project was funded through the Energy & Environmental Research Center–U.S. Department of Energy Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FC26-08NT43291. Nonfederal funding was provided by the IEA Greenhouse Gas R&D Programme.« less
Soft X-ray Emission from Large-Scale Galactic Outflows in Seyfert Galaxies
NASA Astrophysics Data System (ADS)
Colbert, E. J. M.; Baum, S.; O'Dea, C.; Veilleux, S.
1998-01-01
Kiloparsec-scale soft X-ray nebulae extend along the galaxy minor axes in several Seyfert galaxies, including NGC 2992, NGC 4388 and NGC 5506. In these three galaxies, the extended X-ray emission observed in ROSAT HRI images has 0.2-2.4 keV X-ray luminosities of 0.4-3.5 x 10(40) erg s(-1) . The X-ray nebulae are roughly co-spatial with the large-scale radio emission, suggesting that both are produced by large-scale galactic outflows. Assuming pressure balance between the radio and X-ray plasmas, the X-ray filling factor is >~ 10(4) times as large as the radio plasma filling factor, suggesting that large-scale outflows in Seyfert galaxies are predominantly winds of thermal X-ray emitting gas. We favor an interpretation in which large-scale outflows originate as AGN-driven jets that entrain and heat gas on kpc scales as they make their way out of the galaxy. AGN- and starburst-driven winds are also possible explanations if the winds are oriented along the rotation axis of the galaxy disk. Since large-scale outflows are present in at least 50 percent of Seyfert galaxies, the soft X-ray emission from the outflowing gas may, in many cases, explain the ``soft excess" X-ray feature observed below 2 keV in X-ray spectra of many Seyfert 2 galaxies.
Wang, Yunwei; Tong, Xili; Guo, Xiaoning; Wang, Yingyong; Jin, Guoqiang; Guo, Xiangyun
2013-11-29
Highly-qualified graphene was prepared by the ultrasonic exfoliation of commercial expanded graphite (EG) under the promotion of (NH4)2CO3 decomposition. The yield of graphene from the first exfoliation is 7 wt%, and it can be increased to more than 65 wt% by repeated exfoliations. Atomic force microscopy, x-ray photoelectron spectroscopy and Raman analysis show that the as-prepared graphene only has a few defects or oxides, and more than 95% of the graphene flakes have a thickness of ~1 nm. The electrochemical performance of the as-prepared graphene is comparable to reduced graphene oxide in the determination of dopamine (DA) from the mixed solution of ascorbic acid, uric acid and DA. These results show that the decomposition of (NH4)2CO3 molecules in the EG layers under ultrasonication promotes the exfoliation of graphite and provides a low-priced route for large scale production of highly-quality graphene.
NASA Astrophysics Data System (ADS)
Wang, Yunwei; Tong, Xili; Guo, Xiaoning; Wang, Yingyong; Jin, Guoqiang; Guo, Xiangyun
2013-11-01
Highly-qualified graphene was prepared by the ultrasonic exfoliation of commercial expanded graphite (EG) under the promotion of (NH4)2CO3 decomposition. The yield of graphene from the first exfoliation is 7 wt%, and it can be increased to more than 65 wt% by repeated exfoliations. Atomic force microscopy, x-ray photoelectron spectroscopy and Raman analysis show that the as-prepared graphene only has a few defects or oxides, and more than 95% of the graphene flakes have a thickness of ˜1 nm. The electrochemical performance of the as-prepared graphene is comparable to reduced graphene oxide in the determination of dopamine (DA) from the mixed solution of ascorbic acid, uric acid and DA. These results show that the decomposition of (NH4)2CO3 molecules in the EG layers under ultrasonication promotes the exfoliation of graphite and provides a low-priced route for large scale production of highly-quality graphene.
NASA Astrophysics Data System (ADS)
Gately, Conor; Hutyra, Lucy
2016-04-01
In 2013, on-road mobile sources were responsible for over 26% of U.S. fossil fuel carbon dioxide (ffCO2) emissions, and over 34% of both CO and NOx emissions. However, accurate representations of these emissions at the scale of urban areas remains a difficult challenge. Quantifying emissions at the scale of local streets and highways is critical to provide policymakers with the information needed to develop appropriate mitigation strategies and to guide research into the underlying process that drive mobile emissions. Quantification of vehicle ffCO2 emissions at high spatial and temporal resolutions requires a detailed synthesis of data on traffic activity, roadway attributes, fleet characteristics and vehicle speeds. To accurately characterize criteria air pollutant emissions, information on local meteorology is also critical, as the temperature and relative humidity can affect emissions rates of these pollutants by as much as 400%. As the health impacts of air pollutants are more severe for residents living in close proximity (<500m) to road sources, it is critical that inventories of these emissions rely on highly resolved source data to locate potential hot-spots of exposure. In this study we utilize real-time GPS estimates of vehicle speeds to estimate ffCO2 and criteria air pollutant emissions at multiple spatial and temporal scales across a large metropolitan area. We observe large variations in emissions associated with diurnal activity patterns, congestion, sporting and civic events, and weather anomalies. We discuss the advantages and challenges of using highly-resolved source data to quantify emissions at a roadway scale, and the potential of this methodology for forecasting the air quality impacts of changes in infrastructure, urban planning policies, and regional climate.
NASA Astrophysics Data System (ADS)
Gately, C.; Hutyra, L.; Sue Wing, I.; Peterson, S.; Janetos, A.
2015-12-01
In 2013, on-road mobile sources were responsible for over 26% of U.S. fossil fuel carbon dioxide (ffCO2) emissions, and over 34% of both CO and NOx emissions. However, accurate representations of these emissions at the scale of urban areas remains a difficult challenge. Quantifying emissions at the scale of local streets and highways is critical to provide policymakers with the information needed to develop appropriate mitigation strategies and to guide research into the underlying process that drive mobile emissions. Quantification of vehicle ffCO2 emissions at high spatial and temporal resolutions requires a detailed synthesis of data on traffic activity, roadway attributes, fleet characteristics and vehicle speeds. To accurately characterize criteria air pollutant emissions, information on local meteorology is also critical, as the temperature and relative humidity can affect emissions rates of these pollutants by as much as 400%. As the health impacts of air pollutants are more severe for residents living in close proximity (<500m) to road sources, it is critical that inventories of these emissions rely on highly resolved source data to locate potential hot-spots of exposure. In this study we utilize real-time GPS estimates of vehicle speeds to estimate ffCO2 and criteria air pollutant emissions at multiple spatial and temporal scales across a large metropolitan area. We observe large variations in emissions associated with diurnal activity patterns, congestion, sporting and civic events, and weather anomalies. We discuss the advantages and challenges of using highly-resolved source data to quantify emissions at a roadway scale, and the potential of this methodology for forecasting the air quality impacts of changes in infrastructure, urban planning policies, and regional climate.
Meghrous, Jamal; Khramtsov, Nikolai; Buckland, Barry C; Cox, Manon M J; Palomares, Laura A; Srivastava, Indresh K
2015-11-01
Dissolved carbon dioxide (dCO2 ) accumulation during cell culture has been recognized as an important parameter that needs to be controlled for successful scale-up of animal cell culture because above a certain concentration there are adverse effects on cell growth performance and protein production. We investigated the effect of accumulation of dCO2 in bioreactor cultures of expresSF+(®) insect cells infected with recombinant baculoviruses expressing recombinant influenza virus hemagglutinins (rHA). Different strategies for bioreactor cultures were used to obtain various ranges of concentrations of dCO2 (<50, 50-100, 100-200, and >200 mmHg) and to determine their effects on recombinant protein production and cell metabolic activity. We show that the accumulation of dCO2 at levels > 100 mmHg resulted in reduced metabolic activity, slowed cell growth, prolonged culture viability after infection, and decreased infection kinetics. The reduced rHA yields were not caused by the decrease in the extracellular pH that resulted from dCO2 accumulation, but were most likely due to the effect of dCO2 accumulation in cells. The results obtained here at the 2 L scale have been used for the design of large-scale processes to manufacture the rHA based recombinant vaccine Flublok™ at the 2500 L scale Biotechnol. Bioeng. 2015;112: 2267-2275. © 2015 Wiley Periodicals, Inc. © 2015 Wiley Periodicals, Inc.
High-flux solar-driven thermochemical dissociation of CO2 and H2O using nonstoichiometric ceria.
Chueh, William C; Falter, Christoph; Abbott, Mandy; Scipio, Danien; Furler, Philipp; Haile, Sossina M; Steinfeld, Aldo
2010-12-24
Because solar energy is available in large excess relative to current rates of energy consumption, effective conversion of this renewable yet intermittent resource into a transportable and dispatchable chemical fuel may ensure the goal of a sustainable energy future. However, low conversion efficiencies, particularly with CO(2) reduction, as well as utilization of precious materials have limited the practical generation of solar fuels. By using a solar cavity-receiver reactor, we combined the oxygen uptake and release capacity of cerium oxide and facile catalysis at elevated temperatures to thermochemically dissociate CO(2) and H(2)O, yielding CO and H(2), respectively. Stable and rapid generation of fuel was demonstrated over 500 cycles. Solar-to-fuel efficiencies of 0.7 to 0.8% were achieved and shown to be largely limited by the system scale and design rather than by chemistry.
PLSS Scale Demonstration of MTSA Temperature Swing Adsorption Bed Concept for CO2 Removal/Rejection
NASA Technical Reports Server (NTRS)
Iacomini, Christine S.; Powers, Aaron; Paul, Heather L.
2009-01-01
Metabolic heat regenerated temperature swing adsorption (MTSA) incorporated into a portable life support system (PLSS) is being explored as a viable means of removing and rejecting carbon dioxide (CO2) from an astronaut s ventilation loop. Sorbent pellets used in previous work are inherently difficult to quickly heat and cool. Further, their use in packed beds create large undesirable pressure drop. Thus work has been done to assess the application and performance of aluminum foam wash coated with a layer of sorbent. A to-scale sorbent bed, as envisioned studying use by a Martian PLSS, was designed, built, and tested. Performance of the assembly in regards to CO2 adsorption and pressure drop were assessed and the results are presented.
Amine enriched solid sorbents for carbon dioxide capture
Gray, McMahan L.; Soong, Yee; Champagne, Kenneth J.
2003-04-15
A new method for making low-cost CO.sub.2 sorbents that can be used in large-scale gas-solid processes. The new method entails treating a solid substrate with acid or base and simultaneous or subsequent treatment with a substituted amine salt. The method eliminates the need for organic solvents and polymeric materials for the preparation of CO.sub.2 capture systems.
Laser-absorption sensing of gas composition of products from coal gasification
NASA Astrophysics Data System (ADS)
Jeffries, Jay B.; Sur, Ritobrata; Sun, Kai; Hanson, Ronald K.
2014-06-01
A prototype in-situ laser-absorption sensor for the real-time composition measurement (CO, CH4, H2O and CO2) of synthesis gas products of coal gasification (called here syngas) was designed, tested in the laboratory, and demonstrated during field-measurement campaigns in a pilot-scale entrained flow gasifier at the University of Utah and in an engineering-scale, fluidized-bed transport gasifier at the National Carbon Capture Center (NCCC). The prototype design and operation were improved by the lessons learned from each field test. Laser-absorption measurements are problematic in syngas flows because efficient gasifiers operate at elevated pressures (10-50 atm) where absorption transitions are collision broadened and absorption transitions that are isolated at 1 atm become blended into complex features, and because syngas product streams can contain significant particulate, producing significant non-absorption scattering losses of the transmission of laser light. Thus, the prototype sensor used a new wavelength-scanned, wavelength-modulation spectroscopy strategy with 2f-detection and 1f-normalization (WMS-2f/1f) that can provide sensitive absorption measurements of species with spectra blended by collision broadening even in the presence of large non-absorption laser transmission losses (e.g., particulate scattering, beam steering, etc.). The design of the sensor for detection of CO, CH4, H2O and CO2 was optimized for the specific application of syngas monitoring at the output of large-scale gasifiers. Sensor strategies, results and lessons learned from these field measurement campaigns are discussed.
Basin scale controls on CO2 and CH4 emissions from the Upper Mississippi River
Crawford, John T.; Loken, Luke C.; Stanley, Emily H.; Stets, Edward G.; Dornblaser, Mark M.; Striegl, Robert G.
2016-01-01
The Upper Mississippi River, engineered for river navigation in the 1930s, includes a series of low-head dams and navigation pools receiving elevated sediment and nutrient loads from the mostly agricultural basin. Using high-resolution, spatially resolved water quality sensor measurements along 1385 river kilometers, we show that primary productivity and organic matter accumulation affect river carbon dioxide and methane emissions to the atmosphere. Phytoplankton drive CO2to near or below atmospheric equilibrium during the growing season, while anaerobic carbon oxidation supports a large proportion of the CO2 and CH4 production. Reductions of suspended sediment load, absent of dramatic reductions in nutrients, will likely further reduce net CO2emissions from the river. Large river pools, like Lake Pepin, which removes the majority of upstream sediments, and large agricultural tributaries downstream that deliver significant quantities of sediments and nutrients, are likely to persist as major geographical drivers of greenhouse gas emissions.
Southern Ocean carbon-wind stress feedback
NASA Astrophysics Data System (ADS)
Bronselaer, Ben; Zanna, Laure; Munday, David R.; Lowe, Jason
2018-02-01
The Southern Ocean is the largest sink of anthropogenic carbon in the present-day climate. Here, Southern Ocean pCO2 and its dependence on wind forcing are investigated using an equilibrium mixed layer carbon budget. This budget is used to derive an expression for Southern Ocean pCO2 sensitivity to wind stress. Southern Ocean pCO2 is found to vary as the square root of area-mean wind stress, arising from the dominance of vertical mixing over other processes such as lateral Ekman transport. The expression for pCO2 is validated using idealised coarse-resolution ocean numerical experiments. Additionally, we show that increased (decreased) stratification through surface warming reduces (increases) the sensitivity of the Southern Ocean pCO2 to wind stress. The scaling is then used to estimate the wind-stress induced changes of atmospheric pCO_2 in CMIP5 models using only a handful of parameters. The scaling is further used to model the anthropogenic carbon sink, showing a long-term reversal of the Southern Ocean sink for large wind stress strength.
NASA Astrophysics Data System (ADS)
LaFranchi, B. W.; Campbell, J. E.; Cameron-Smith, P. J.; Bambha, R.; Michelsen, H. A.
2013-12-01
Urbanized regions are responsible for a disproportionately large percentage (30-40%) of global anthropogenic greenhouse gas (GHG) emissions, despite covering only 2% of the Earth's surface area [Satterthwaite, 2008]. As a result, policies enacted at the local level in these urban areas can, in aggregate, have a large global impact, both positive and negative. In order to address the scientific questions that are required to drive these policy decisions, methods are needed that resolve gross CO2 flux components from the net flux. Recent work suggests that the critical knowledge gaps in CO2 surface fluxes could be addressed through the combined analysis of atmospheric carbonyl sulfide (COS) and radiocarbon in atmospheric CO2 (14CO2) [e.g. Campbell et al., 2008; Graven et al., 2009]. The 14CO2 approach relies on mass balance assumptions about atmospheric CO2 and the large differences in 14CO2 abundance between fossil and natural sources of CO2 [Levin et al., 2003]. COS, meanwhile, is a potentially transformative tracer of photosynthesis because its variability in the atmosphere has been found to be influenced primarily by vegetative uptake, scaling linearly will gross primary production (GPP) [Kettle et al., 20027]. Taken together, these two observations provide constraints on two of the three main components of the CO2 budget at the urban scale: photosynthesis and fossil fuel emissions. The third component, respiration, can then be determined by difference if the net flux is known. Here we present a general overview of our synthesized model-observation approach for improving surface flux estimates of CO2 for the upwind fetch of a ~30m tower located in Livermore, CA, USA, a suburb (pop. ~80,000) at the eastern edge of the San Francisco Bay Area. Additionally, we will present initial results from a one week observational intensive, which includes continuous CO2, CH4, CO, SO2, NOx, and O3 observations in addition to measurements of 14CO2 and COS from air samples collected every ~1-3 hours during this time period. References Campbell, J. E., et. al., Science, 322, 1085-1088, 2008. Graven, H. D., et al., Tellus B, 61, 536-546, 2009. Kettle, A. J., et al., J. Geophys. Res.-Atmos., 107, 2002. Levin, I., et al., Geophys. Res. Lett., 30, 2003. Satterthwaite, D., Environment and Urbanization, 20, 539-549, 2008.
Structural Variation Shapes the Landscape of Recombination in Mouse
Morgan, Andrew P.; Gatti, Daniel M.; Najarian, Maya L.; Keane, Thomas M.; Galante, Raymond J.; Pack, Allan I.; Mott, Richard; Churchill, Gary A.; de Villena, Fernando Pardo-Manuel
2017-01-01
Meiotic recombination is an essential feature of sexual reproduction that ensures faithful segregation of chromosomes and redistributes genetic variants in populations. Multiparent populations such as the Diversity Outbred (DO) mouse stock accumulate large numbers of crossover (CO) events between founder haplotypes, and thus present a unique opportunity to study the role of genetic variation in shaping the recombination landscape. We obtained high-density genotype data from 6886 DO mice, and localized 2.2 million CO events to intervals with a median size of 28 kb. The resulting sex-averaged genetic map of the DO population is highly concordant with large-scale (order 10 Mb) features of previously reported genetic maps for mouse. To examine fine-scale (order 10 kb) patterns of recombination in the DO, we overlaid putative recombination hotspots onto our CO intervals. We found that CO intervals are enriched in hotspots compared to the genomic background. However, as many as 26% of CO intervals do not overlap any putative hotspots, suggesting that our understanding of hotspots is incomplete. We also identified coldspots encompassing 329 Mb, or 12% of observable genome, in which there is little or no recombination. In contrast to hotspots, which are a few kilobases in size, and widely scattered throughout the genome, coldspots have a median size of 2.1 Mb and are spatially clustered. Coldspots are strongly associated with copy-number variant (CNV) regions, especially multi-allelic clusters, identified from whole-genome sequencing of 228 DO mice. Genes in these regions have reduced expression, and epigenetic features of closed chromatin in male germ cells, which suggests that CNVs may repress recombination by altering chromatin structure in meiosis. Our findings demonstrate how multiparent populations, by bridging the gap between large-scale and fine-scale genetic mapping, can reveal new features of the recombination landscape. PMID:28592499
Structural Variation Shapes the Landscape of Recombination in Mouse.
Morgan, Andrew P; Gatti, Daniel M; Najarian, Maya L; Keane, Thomas M; Galante, Raymond J; Pack, Allan I; Mott, Richard; Churchill, Gary A; de Villena, Fernando Pardo-Manuel
2017-06-01
Meiotic recombination is an essential feature of sexual reproduction that ensures faithful segregation of chromosomes and redistributes genetic variants in populations. Multiparent populations such as the Diversity Outbred (DO) mouse stock accumulate large numbers of crossover (CO) events between founder haplotypes, and thus present a unique opportunity to study the role of genetic variation in shaping the recombination landscape. We obtained high-density genotype data from [Formula: see text] DO mice, and localized 2.2 million CO events to intervals with a median size of 28 kb. The resulting sex-averaged genetic map of the DO population is highly concordant with large-scale (order 10 Mb) features of previously reported genetic maps for mouse. To examine fine-scale (order 10 kb) patterns of recombination in the DO, we overlaid putative recombination hotspots onto our CO intervals. We found that CO intervals are enriched in hotspots compared to the genomic background. However, as many as [Formula: see text] of CO intervals do not overlap any putative hotspots, suggesting that our understanding of hotspots is incomplete. We also identified coldspots encompassing 329 Mb, or [Formula: see text] of observable genome, in which there is little or no recombination. In contrast to hotspots, which are a few kilobases in size, and widely scattered throughout the genome, coldspots have a median size of 2.1 Mb and are spatially clustered. Coldspots are strongly associated with copy-number variant (CNV) regions, especially multi-allelic clusters, identified from whole-genome sequencing of 228 DO mice. Genes in these regions have reduced expression, and epigenetic features of closed chromatin in male germ cells, which suggests that CNVs may repress recombination by altering chromatin structure in meiosis. Our findings demonstrate how multiparent populations, by bridging the gap between large-scale and fine-scale genetic mapping, can reveal new features of the recombination landscape. Copyright © 2017 by the Genetics Society of America.
Economic and energetic analysis of capturing CO2 from ambient air
House, Kurt Zenz; Baclig, Antonio C.; Ranjan, Manya; van Nierop, Ernst A.; Wilcox, Jennifer; Herzog, Howard J.
2011-01-01
Capturing carbon dioxide from the atmosphere (“air capture”) in an industrial process has been proposed as an option for stabilizing global CO2 concentrations. Published analyses suggest these air capture systems may cost a few hundred dollars per tonne of CO2, making it cost competitive with mainstream CO2 mitigation options like renewable energy, nuclear power, and carbon dioxide capture and storage from large CO2 emitting point sources. We investigate the thermodynamic efficiencies of commercial separation systems as well as trace gas removal systems to better understand and constrain the energy requirements and costs of these air capture systems. Our empirical analyses of operating commercial processes suggest that the energetic and financial costs of capturing CO2 from the air are likely to have been underestimated. Specifically, our analysis of existing gas separation systems suggests that, unless air capture significantly outperforms these systems, it is likely to require more than 400 kJ of work per mole of CO2, requiring it to be powered by CO2-neutral power sources in order to be CO2 negative. We estimate that total system costs of an air capture system will be on the order of $1,000 per tonne of CO2, based on experience with as-built large-scale trace gas removal systems. PMID:22143760
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hancu, Dan
GE Global Research has developed, over the last 8 years, a platform of cost effective CO2 capture technologies based on a non-aqueous aminosilicone solvent (GAP-1m). As demonstrated in previous funded DOE projects (DE-FE0007502 and DEFE0013755), the GAP-1m solvent has increased CO2 working capacity, lower volatility and corrosivity than the benchmark aqueous amine technology. Performance of the GAP-1m solvent was recently demonstrated in a 0.5 MWe pilot at National Carbon Capture Center, AL with real flue gas for over 500 hours of operation using a Steam Stripper Column (SSC). The pilot-scale PSTU engineering data were used to (i) update the techno-economicmore » analysis, and EH&S assessment, (ii) perform technology gap analysis, and (iii) conduct the solvent manufacturability and scale-up study.« less
The cost of getting CCS wrong: Uncertainty, infrastructure design, and stranded CO 2
Middleton, Richard Stephen; Yaw, Sean Patrick
2018-01-11
Carbon capture, and storage (CCS) infrastructure will require industry—such as fossil-fuel power, ethanol production, and oil and gas extraction—to make massive investment in infrastructure. The cost of getting these investments wrong will be substantial and will impact the success of CCS technology. Multiple factors can and will impact the success of commercial-scale CCS, including significant uncertainties regarding capture, transport, and injection-storage decisions. Uncertainties throughout the CCS supply chain include policy, technology, engineering performance, economics, and market forces. In particular, large uncertainties exist for the injection and storage of CO 2. Even taking into account upfront investment in site characterization, themore » final performance of the storage phase is largely unknown until commercial-scale injection has started. We explore and quantify the impact of getting CCS infrastructure decisions wrong based on uncertain injection rates and uncertain CO 2 storage capacities using a case study managing CO 2 emissions from the Canadian oil sands industry in Alberta. We use SimCCS, a widely used CCS infrastructure design framework, to develop multiple CCS infrastructure scenarios. Each scenario consists of a CCS infrastructure network that connects CO 2 sources (oil sands extraction and processing) with CO 2 storage reservoirs (acid gas storage reservoirs) using a dedicated CO 2 pipeline network. Each scenario is analyzed under a range of uncertain storage estimates and infrastructure performance is assessed and quantified in terms of cost to build additional infrastructure to store all CO 2. We also include the role of stranded CO 2, CO 2 that a source was expecting to but cannot capture due substandard performance in the transport and storage infrastructure. Results show that the cost of getting the original infrastructure design wrong are significant and that comprehensive planning will be required to ensure that CCS becomes a successful climate mitigation technology. Here, we show that the concept of stranded CO 2 can transform a seemingly high-performing infrastructure design into the worst case scenario.« less
The cost of getting CCS wrong: Uncertainty, infrastructure design, and stranded CO 2
DOE Office of Scientific and Technical Information (OSTI.GOV)
Middleton, Richard Stephen; Yaw, Sean Patrick
Carbon capture, and storage (CCS) infrastructure will require industry—such as fossil-fuel power, ethanol production, and oil and gas extraction—to make massive investment in infrastructure. The cost of getting these investments wrong will be substantial and will impact the success of CCS technology. Multiple factors can and will impact the success of commercial-scale CCS, including significant uncertainties regarding capture, transport, and injection-storage decisions. Uncertainties throughout the CCS supply chain include policy, technology, engineering performance, economics, and market forces. In particular, large uncertainties exist for the injection and storage of CO 2. Even taking into account upfront investment in site characterization, themore » final performance of the storage phase is largely unknown until commercial-scale injection has started. We explore and quantify the impact of getting CCS infrastructure decisions wrong based on uncertain injection rates and uncertain CO 2 storage capacities using a case study managing CO 2 emissions from the Canadian oil sands industry in Alberta. We use SimCCS, a widely used CCS infrastructure design framework, to develop multiple CCS infrastructure scenarios. Each scenario consists of a CCS infrastructure network that connects CO 2 sources (oil sands extraction and processing) with CO 2 storage reservoirs (acid gas storage reservoirs) using a dedicated CO 2 pipeline network. Each scenario is analyzed under a range of uncertain storage estimates and infrastructure performance is assessed and quantified in terms of cost to build additional infrastructure to store all CO 2. We also include the role of stranded CO 2, CO 2 that a source was expecting to but cannot capture due substandard performance in the transport and storage infrastructure. Results show that the cost of getting the original infrastructure design wrong are significant and that comprehensive planning will be required to ensure that CCS becomes a successful climate mitigation technology. Here, we show that the concept of stranded CO 2 can transform a seemingly high-performing infrastructure design into the worst case scenario.« less
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.
Greenhouse gas exchange over grazed systems
NASA Astrophysics Data System (ADS)
Felber, R.; Ammann, C.; Neftel, A.
2012-04-01
Grasslands act as sinks and sources of greenhouse gases (GHG) and are, in conjunction with livestock production systems, responsible for a large share of GHG emissions. Whereas ecosystem scale flux measurements (eddy covariance) are commonly used to investigate CO2 exchange (and is becoming state-of-the-art for other GHGs, too), GHG emissions from agricultural animals are usually investigated on the scale of individual animals. Therefore eddy covariance technique has to be tested for combined systems (i.e. grazed systems). Our project investigates the ability of field scale flux measurements to reliably quantify the contribution of grazing dairy cows to the net exchange of CO2 and CH4. To quantify the contribution of the animals to the net flux the position, movement, and grazing/rumination activity of each cow are recorded. In combination with a detailed footprint analysis of the eddy covariance fluxes, the animal related CO2 and CH4 emissions are derived and compared to standard emission values derived from respiration chambers. The aim of the project is to test the assumption whether field scale CO2 flux measurements adequately include the respiration of grazing cows and to identify potential errors in ecosystem Greenhouse gas budgets.
NASA Astrophysics Data System (ADS)
Zulueta, Rommel Callejo
Natural ecosystems are rarely structurally or functionally homogeneous. This is true for the complex coastal regions of Magdalena Bay, Baja California Sur, Mexico, and the Barrow Peninsula on the Arctic Coastal Plain of Alaska. The coastal region of Magdalena Bay is comprised of the Pacific coastal ocean, eutrophic lagoon, mangroves, and desert ecosystems all adjacent and within a few kilometers, while the Barrow Peninsula is a mosaic of small ponds, thaw lakes, different aged vegetated thaw-lake basins ( VDTLBs ) and interstitial tundra which have been dynamically formed by both short- and long-term processes. We used a combination of tower- and small environmental research aircraft (SERA)-based eddy covariance measurements to characterize the spatial and temporal patterns of CO2, latent, and sensible heat fluxes along with MODIS NDVI, and land surface information, to scale the SERA-based CO2 fluxes up to the regional scale. In the first part of this research, the spatial variability in ecosystem fluxes from the Pacific coastal ocean, eutrophic lagoon, mangroves, and desert areas of northern Magdalena Bay were studied. SERA-derived average midday CO2 fluxes from the desert showed a slight uptake of -1.32 mumol CO2 m-2 s-1, the coastal ocean also showed uptake of -3.48 mumol CO2 m-2 s -1, and the lagoon mangroves showed the highest uptake of -8.11 mumol CO2 m-2 s-1. Additional simultaneous measurements of NDVI allowed simple linear modeling of CO2 flux as a function of NDVI for the mangroves of the Magdalena Bay region. In the second part of this research, the spatial variability of ecosystem fluxes across the 1802 km2 Barrow Peninsula region was studied. During typical 2006 summer conditions, the midday hourly CO2 flux over the region was -2.04 x 105 kgCO2 hr-1. The CO2 fluxes among the interstitial tundra, Ancient and Old VDTLBs, as well as between the Medium and Young VDTLBs were not significantly different. Combined, the interstitial tundra and Old and Ancient VDTLBs, represent ˜67% of the Barrow Peninsula surface area, accounting for ˜59% of the regional flux signal. Though the Medium and Young VDTLBs represent ˜11% of the surface area, they account for a large portion, ˜35%, of the total regional flux. The remaining ˜22% of the surface area are lakes and contributed the remaining ˜6% of the total regional flux. Previous studies treated vegetated areas of the region as a single surface type with measurements from a few study sites; doing so could underestimate the regional flux by ˜22%. The San Diego State University Sky Arrow 650TCN Environmental Research Aircraft proved to be an effective tool in characterizing land-atmosphere fluxes of energy, CO2 and water across heterogeneous landscapes at the scale of 1 km, and was capable of discriminating fluxes from the various ecosystem and land surface types a few kilometers distant. Here, we demonstrate that SERA-based approaches have the ability to cover large spatial scales while measuring the turbulent fluxes across a number of surfaces and combined with ground- and satellite-based measurements provide a valuable tool for both scaling and validation of regional-scale fluxes.
Lin, Yi-Feng; Chen, Chien-Hua; Tung, Kuo-Lun; Wei, Te-Yu; Lu, Shih-Yuan; Chang, Kai-Shiun
2013-03-01
The use of a membrane contactor combined with a hydrophobic porous membrane and an amine absorbent has attracted considerable attention for the capture of CO2 because of its extensive use, low operational costs, and low energy consumption. The hydrophobic porous membrane interface prevents the passage of the amine absorbent but allows the penetration of CO2 molecules that are captured by the amine absorbent. Herein, highly porous SiO2 aerogels modified with hydrophobic fluorocarbon functional groups (CF3 ) were successfully coated onto a macroporous Al2 O3 membrane; their performance in a membrane contactor for CO2 absorption is discussed. The SiO2 aerogel membrane modified with CF3 functional groups exhibits the highest CO2 absorption flux and can be continuously operated for CO2 absorption for extended periods of time. This study suggests that a SiO2 aerogel membrane modified with CF3 functional groups could potentially be used in a membrane contactor for CO2 absorption. Also, the resulting hydrophobic SiO2 aerogel membrane contactor is a promising technology for large-scale CO2 absorption during the post-combustion process in power plants. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Hirota, Mitsuru; Zhang, Pengcheng; Gu, Song; Shen, Haihua; Kuriyama, Takeo; Li, Yingnian; Tang, Yanhong
2010-07-01
Characterizing the spatial variation in the CO2 flux at both large and small scales is essential for precise estimation of an ecosystem's CO2 sink strength. However, little is known about small-scale CO2 flux variations in an ecosystem. We explored these variations in a Kobresia meadow ecosystem on the Qinghai-Tibetan plateau in relation to spatial variability in species composition and biomass. We established 14 points and measured net ecosystem production (NEP), gross primary production (GPP), and ecosystem respiration (Re) in relation to vegetation biomass, species richness, and environmental variables at each point, using an automated chamber system during the 2005 growing season. Mean light-saturated NEP and GPP were 30.3 and 40.5 micromol CO2 m(-2) s(-1) [coefficient of variation (CV), 42.7 and 29.4], respectively. Mean Re at 20 degrees C soil temperature, Re(20), was -10.9 micromol CO2 m(-2) s(-1) (CV, 27.3). Re(20) was positively correlated with vegetation biomass. GPP(max) was positively correlated with species richness, but 2 of the 14 points were outliers. Vegetation biomass was the main determinant of spatial variation of Re, whereas species richness mainly affected that of GPP, probably reflecting the complexity of canopy structure and light partitioning in this small grassland patch.
López-Padilla, Alexis; Ruiz-Rodriguez, Alejandro; Restrepo Flórez, Claudia Estela; Rivero Barrios, Diana Marsela; Reglero, Guillermo; Fornari, Tiziana
2016-01-01
Vaccinium meridionale Swartz (Mortiño or Colombian blueberry) is one of the Vaccinium species abundantly found across the Colombian mountains, which are characterized by high contents of polyphenolic compounds (anthocyanins and flavonoids). The supercritical fluid extraction (SFE) of Vaccinium species has mainly focused on the study of V. myrtillus L. (blueberry). In this work, the SFE of Mortiño fruit from Colombia was studied in a small-scale extraction cell (273 cm3) and different extraction pressures (20 and 30 MPa) and temperatures (313 and 343 K) were investigated. Then, process scaling-up to a larger extraction cell (1350 cm3) was analyzed using well-known semi-empirical engineering approaches. The Broken and Intact Cell (BIC) model was adjusted to represent the kinetic behavior of the low-scale extraction and to simulate the large-scale conditions. Extraction yields obtained were in the range 0.1%–3.2%. Most of the Mortiño solutes are readily accessible and, thus, 92% of the extractable material was recovered in around 30 min. The constant CO2 residence time criterion produced excellent results regarding the small-scale kinetic curve according to the BIC model, and this conclusion was experimentally validated in large-scale kinetic experiments. PMID:28773640
NASA Astrophysics Data System (ADS)
Vogel, F. R.; Chan, E.; Huang, L.; Levin, I.; Worthy, D.
2013-12-01
Urban areas are said to be responsible for approximately 75% of anthropogenic Greenhouse Gases (GHGs) emissions while comprising only two percent of the land area [1]. This limited spatial expansion should facilitate a monitoring of anthropogenic GHGs from atmospheric observations. As major sources of emissions, cities also have a huge potential to drive emissions reductions. To effectively manage emissions, cities must however, first measure and report these publicly [2]. Modelling studies and measurements of CO2 from fossil fuel burning (FFCO2) in densely populated areas does, however, pose several challenges: Besides continuous in-situ observations, i.e. finding an adequate atmospheric transport model, a sufficiently fine-grained FFCO2 emission model and the proper background reference observations to distinguish the large-scale from the local/urban contributions to the observed FFCO2 concentration offsets ( ΔFFCO2) are required. Pilot studies which include the data from two 'sister sites*' in the vicinity of Toronto, Canada helped to derive flux estimates for Non-CO2 GHGs [3] and improve our understanding of urban FFCO2 emissions. Our 13CO2 observations reveal that the contribution of natural gas burning (mostly due to domestic heating) account for 80%×7% of FFCO2 emissions in the Greater Toronto Area (GTA) during winter. Our 14CO2 observations in the GTA, furthermore, show that the local offset of CO2 (ΔCO2) between our two sister sites can be largely attributed to urban FFCO2 emissions. The seasonal cycle of the observed ΔFFCO2 in Toronto, combined with high-resolution atmospheric modeling, helps to independently assess the contribution from different emission sectors (transportation, primary energy and industry, domestic heating) as predicted by a dedicated city-scale emission inventory, which deviates from a UNFCCC-based inventory. [1] D. Dodman. 2009. Blaming cities for climate change? An analysis of urban greenhouse gas emissions inventories. Environment and Urbanization, 21,185. [2] Arikan Y., Desaim R., Bhatia P. and W. K. Fong, 2012 Global Protocol for Community-Scale Greenhouse Gas Emissions (GPC), C40 Cities Climate Leadership group, available at: http://www.c40.org [3] Vogel, F. R., Ishizawa, M., Chan, E., Chan, D., Hammer, S., Levin, I., & Worthy, D. E. J. (2012). Regional non-CO2 greenhouse gas fluxes inferred from atmospheric measurements in Ontario, Canada. Journal of Integrative Environmental Sciences, 9(1), 41-55. *The term 'sister sites' refers to sites that share a common background signal (i.e. common large scale influence), while significantly differing sensitivities to urban GHG emissions. In our case: Egbert, Ontario and Downsview, Toronto, Ontario.
NASA Astrophysics Data System (ADS)
Saltiel, S.; Bonner, B. P.; Ajo Franklin, J. B.
2014-12-01
Time-lapse seismic monitoring (4D) is currently the primary technique available for tracking sequestered CO2 in a geologic storage reservoir away from monitoring wells. The main seismic responses to injection are those due to direct fluid substitution, changes in differential pressure, and chemical interactions with reservoir rocks; the importance of each depends on reservoir/injection properties and temporal/spatial scales of interest. As part of the Big Sky Carbon Sequestration Partnership, we are monitoring the upcoming large scale (1 million ton+) CO2 injection in Kevin Dome, north central Montana. As part of this research, we predict the relative significance of these three effects, as an aid in design of field surveys. Analysis is undertaken using existing open-hole well log data and cores from wells drilled at producer and injector pads as well as core experiments. For this demonstration site, CO2 will be produced from a natural reservoir and re-injected down dip, where the formation is saturated with brine. Effective medium models based on borehole seismic velocity measurements predict relatively small effects (less than 40 m/s change in V¬p) due to the injection of more compressible supercritical CO2. This is due to the stiff dolomite reservoir rock, with high seismic velocities (Vp~6000 m/s, Vs~3000 m/s) and fairly low porosity (<10%). Assuming pure dolomite mineralogy, these models predict a slight increase in Vp during CO2 injection. This velocity increase is due to the lower density of CO2 relative to brine; which outweighs the small change in modulus compared to the stiff reservoir rock. We present both room pressure and in-situ P/T ultrasonic experiments using core samples obtained from the reservoir; such measurements are undertaken to access the expected seismic velocities under pressurized injection. The reservoir appears to have fairly low permeability. Large-volume injection is expected to produce large local pore pressure increases, which may have the largest immediate effect on seismic velocities. Increasing pore pressure lowers the differential pressure due to confining stress, which decreases seismic velocities by opening cracks. The magnitude of this effect depends both on rock microstructure and fracture at the field scale; core scale measurements will help separate these effects.
Ye, Siyuan; Krauss, Ken W.; Brix, Hans; Wei, Mengjie; Olsson, Linda; Yu, Xueyang; Ma, Yueying; Wang, Jin; Yuan, Hongming; Zhao, Guangming; Ding, Xigui; Moss, Rebecca
2016-01-01
Global management of wetlands to suppress greenhouse gas (GHG) emissions, facilitate carbon (C) sequestration, and reduce atmospheric CO2 concentrations while simultaneously promoting agricultural gains is paramount. However, studies that relate variability in CO2 and CH4 emissions at large spatial scales are limited. We investigated three-year emissions of soil CO2 and CH4 from the primary wetland types of the Liaohe Delta, China, by focusing on a total wetland area of 3287 km2. One percent is Suaeda salsa, 24% is Phragmites australis, and 75% is rice. While S. salsa wetlands are under somewhat natural tidal influence, P. australis and rice are managed hydrologically for paper and food, respectively. Total C emissions from CO2 and CH4 from these wetland soils were 2.9 Tg C/year, ranging from 2.5 to 3.3 Tg C/year depending on the year assessed. Primary emissions were from CO2 (~98%). Photosynthetic uptake of CO2 would mitigate most of the soil CO2 emissions, but CH4 emissions would persist. Overall, CH4 fluxes were high when soil temperatures were >18°C and pore water salinity <18 PSU. CH4 emissions from rice habitat alone in the Liaohe Delta represent 0.2% of CH4 carbon emissions globally from rice. With such a large area and interannual sensitivity in soil GHG fluxes, management practices in the Delta and similar wetlands around the world have the potential not only to influence local C budgeting, but also to influence global biogeochemical cycling.
NASA Astrophysics Data System (ADS)
Zhao, Suping; Yu, Ye; Qin, Dahe; Yin, Daiying; He, Jianjun
2017-12-01
To solve traffic congestion and to improve urban air quality, long-lasting and large-scale even-odd license plate controlled plan was implemented by local government during 20 November to 26 December 2016 in urban Lanzhou, a semi-arid valley city of northwest China. The traffic control measures provided an invaluable opportunity to evaluate its effects on urban air quality in less developed cities of northwest China. Based on measured simultaneously air pollutants and meteorological parameters, the abatement of traffic-related pollutants induced by the implemented control measures such as CO, PM2.5 and PM10 (the particulate matter with diameter less than 2.5 μm and 10 μm) concentrations were firstly quantified by comparing the air quality data in urban areas with those in rural areas (uncontrolled zones). The concentrations of CO, NO2 from motor vehicles and fine particulate matter (PM2.5) were shown to have significant decreases of 15%-23% during traffic control period from those measured before control period with hourly maximum CO, PM2.5, and NO2/SO2 reduction of 43%, 35% and 141.4%, respectively. The influence of the control measures on AQI (air quality index) and ozone was less as compared to its effect on other air pollutants. Therefore, to alleviate serious winter haze pollution in China and to protect human health, the stringent long-term and large-scale even-odd license plate controlled plan should be implemented aperiodically in urban areas, especially for the periods with poor diffusion conditions.
FutureGen 2.0 Oxy-combustion Large Scale Test – Final Report
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kenison, LaVesta; Flanigan, Thomas; Hagerty, Gregg
The primary objectives of the FutureGen 2.0 CO 2 Oxy-Combustion Large Scale Test Project were to site, permit, design, construct, and commission, an oxy-combustion boiler, gas quality control system, air separation unit, and CO 2 compression and purification unit, together with the necessary supporting and interconnection utilities. The project was to demonstrate at commercial scale (168MWe gross) the capability to cleanly produce electricity through coal combustion at a retrofitted, existing coal-fired power plant; thereby, resulting in near-zeroemissions of all commonly regulated air emissions, as well as 90% CO 2 capture in steady-state operations. The project was to be fully integratedmore » in terms of project management, capacity, capabilities, technical scope, cost, and schedule with the companion FutureGen 2.0 CO 2 Pipeline and Storage Project, a separate but complementary project whose objective was to safely transport, permanently store and monitor the CO 2 captured by the Oxy-combustion Power Plant Project. The FutureGen 2.0 Oxy-Combustion Large Scale Test Project successfully achieved all technical objectives inclusive of front-end-engineering and design, and advanced design required to accurately estimate and contract for the construction, commissioning, and start-up of a commercial-scale "ready to build" power plant using oxy-combustion technology, including full integration with the companion CO 2 Pipeline and Storage project. Ultimately the project did not proceed to construction due to insufficient time to complete necessary EPC contract negotiations and commercial financing prior to expiration of federal co-funding, which triggered a DOE decision to closeout its participation in the project. Through the work that was completed, valuable technical, commercial, and programmatic lessons were learned. This project has significantly advanced the development of near-zero emission technology and will be helpful to plotting the course of, and successfully executing future large demonstration projects. This Final Scientific and Technical Report describes the technology and engineering basis of the project, inclusive of process systems, performance, effluents and emissions, and controls. Further, the project cost estimate, schedule, and permitting requirements are presented, along with a project risk and opportunity assessment. Lessons-learned related to these elements are summarized in this report. Companion reports Oxy-combustion further document the accomplishments and learnings of the project, including: A.01 Project Management Report which describes what was done to coordinate the various participants, and to track their performance with regard to schedule and budget B.02 Lessons Learned - Technology Integration, Value Improvements, and Program Management, which describes the innovations and conclusions that we arrived upon during the development of the project, and makes recommendations for improvement of future projects of a similar nature . B.03 Project Economics, which details the capital and operation costs and their basis, and also illustrates the cost of power produced by the plant with certain sensitivities. B.04 Power Plant, Pipeline, and Injection Site Interfaces, which details the interfaces between the two FutureGen projects B.05 Contractual Mechanisms for Design, Construction, and Operation, which describes the major EPC, and Operations Contracts required to execute the project.« less
Carbon Dioxide Emissions Effects of Grid-Scale Electricity Storage in a Decarbonizing Power System
Craig, Michael T.; Jaramillo, Paulina; Hodge, Bri-Mathias
2018-01-03
While grid-scale electricity storage (hereafter 'storage') could be crucial for deeply decarbonizing the electric power system, it would increase carbon dioxide (CO 2) emissions in current systems across the United States. To better understand how storage transitions from increasing to decreasing system CO 2 emissions, we quantify the effect of storage on operational CO 2 emissions as a power system decarbonizes under a moderate and strong CO 2 emission reduction target through 2045. Under each target, we compare the effect of storage on CO 2 emissions when storage participates in only energy, only reserve, and energy and reserve markets. Wemore » conduct our study in the Electricity Reliability Council of Texas (ERCOT) system and use a capacity expansion model to forecast generator fleet changes and a unit commitment and economic dispatch model to quantify system CO 2 emissions with and without storage. We find that storage would increase CO 2 emissions in the current ERCOT system, but would decrease CO 2 emissions in 2025 through 2045 under both decarbonization targets. Storage reduces CO 2 emissions primarily by enabling gas-fired generation to displace coal-fired generation, but also by reducing wind and solar curtailment. We further find that the market in which storage participates drives large differences in the magnitude, but not the direction, of the effect of storage on CO 2 emissions.« less
Carbon Dioxide Emissions Effects of Grid-Scale Electricity Storage in a Decarbonizing Power System
DOE Office of Scientific and Technical Information (OSTI.GOV)
Craig, Michael T.; Jaramillo, Paulina; Hodge, Bri-Mathias
While grid-scale electricity storage (hereafter 'storage') could be crucial for deeply decarbonizing the electric power system, it would increase carbon dioxide (CO 2) emissions in current systems across the United States. To better understand how storage transitions from increasing to decreasing system CO 2 emissions, we quantify the effect of storage on operational CO 2 emissions as a power system decarbonizes under a moderate and strong CO 2 emission reduction target through 2045. Under each target, we compare the effect of storage on CO 2 emissions when storage participates in only energy, only reserve, and energy and reserve markets. Wemore » conduct our study in the Electricity Reliability Council of Texas (ERCOT) system and use a capacity expansion model to forecast generator fleet changes and a unit commitment and economic dispatch model to quantify system CO 2 emissions with and without storage. We find that storage would increase CO 2 emissions in the current ERCOT system, but would decrease CO 2 emissions in 2025 through 2045 under both decarbonization targets. Storage reduces CO 2 emissions primarily by enabling gas-fired generation to displace coal-fired generation, but also by reducing wind and solar curtailment. We further find that the market in which storage participates drives large differences in the magnitude, but not the direction, of the effect of storage on CO 2 emissions.« less
Carbon dioxide emissions effects of grid-scale electricity storage in a decarbonizing power system
NASA Astrophysics Data System (ADS)
Craig, Michael T.; Jaramillo, Paulina; Hodge, Bri-Mathias
2018-01-01
While grid-scale electricity storage (hereafter ‘storage’) could be crucial for deeply decarbonizing the electric power system, it would increase carbon dioxide (CO2) emissions in current systems across the United States. To better understand how storage transitions from increasing to decreasing system CO2 emissions, we quantify the effect of storage on operational CO2 emissions as a power system decarbonizes under a moderate and strong CO2 emission reduction target through 2045. Under each target, we compare the effect of storage on CO2 emissions when storage participates in only energy, only reserve, and energy and reserve markets. We conduct our study in the Electricity Reliability Council of Texas (ERCOT) system and use a capacity expansion model to forecast generator fleet changes and a unit commitment and economic dispatch model to quantify system CO2 emissions with and without storage. We find that storage would increase CO2 emissions in the current ERCOT system, but would decrease CO2 emissions in 2025 through 2045 under both decarbonization targets. Storage reduces CO2 emissions primarily by enabling gas-fired generation to displace coal-fired generation, but also by reducing wind and solar curtailment. We further find that the market in which storage participates drives large differences in the magnitude, but not the direction, of the effect of storage on CO2 emissions.
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
NASA Technical Reports Server (NTRS)
Pagano, Thomas S.; Olsen, Edward T.
2012-01-01
The Atmospheric Infrared Sounder (AIRS) is a hyperspectral infrared instrument on the EOS Aqua Spacecraft, launched on May 4, 2002. AIRS has 2378 infrared channels ranging from 3.7 microns to 15.4 microns and a 13.5 km footprint. AIRS, in conjunction with the Advanced Microwave Sounding Unit (AMSU), produces temperature profiles with 1K/km accuracy, water vapor profiles (20%/2km), infrared cloud height and fraction, and trace gas amounts for CO2, CO, SO2, O3 and CH4 in the mid to upper troposphere. AIRS wide swath(cedilla) +/-49.5 deg , enables daily global daily coverage for over 95% of the Earth's surface. AIRS data are used for weather forecasting, validating climate model distribution and processes, and observing long-range transport of greenhouse gases. In this study, we examine the large scale and regional horizontal variability in the AIRS Mid-tropospheric Carbon Dioxide product as a function of season and associate the observed variability with known atmospheric transport processes, and sources and sinks of CO2.
Leetaru, H.E.; Frailey, S.M.; Damico, J.; Mehnert, E.; Birkholzer, J.; Zhou, Q.; Jordan, P.D.
2009-01-01
Large scale geologic sequestration tests are in the planning stages around the world. The liability and safety issues of the migration of CO2 away from the primary injection site and/or reservoir are of significant concerns for these sequestration tests. Reservoir models for simulating single or multi-phase fluid flow are used to understand the migration of CO2 in the subsurface. These models can also help evaluate concerns related to brine migration and basin-scale pressure increases that occur due to the injection of additional fluid volumes into the subsurface. The current paper presents different modeling examples addressing these issues, ranging from simple geometric models to more complex reservoir fluid models with single-site and basin-scale applications. Simple geometric models assuming a homogeneous geologic reservoir and piston-like displacement have been used for understanding pressure changes and fluid migration around each CO2 storage site. These geometric models are useful only as broad approximations because they do not account for the variation in porosity, permeability, asymmetry of the reservoir, and dip of the beds. In addition, these simple models are not capable of predicting the interference between different injection sites within the same reservoir. A more realistic model of CO2 plume behavior can be produced using reservoir fluid models. Reservoir simulation of natural gas storage reservoirs in the Illinois Basin Cambrian-age Mt. Simon Sandstone suggest that reservoir heterogeneity will be an important factor for evaluating storage capacity. The Mt. Simon Sandstone is a thick sandstone that underlies many significant coal fired power plants (emitting at least 1 million tonnes per year) in the midwestern United States including the states of Illinois, Indiana, Kentucky, Michigan, and Ohio. The initial commercial sequestration sites are expected to inject 1 to 2 million tonnes of CO2 per year. Depending on the geologic structure and permeability anisotropy, the CO2 injected into the Mt. Simon are expected to migrate less than 3 km. After 30 years of continuous injection followed by 100 years of shut-in, the plume from a 1 million tonnes a year injection rate is expected to migrate 1.6 km for a 0 degree dip reservoir and over 3 km for a 5 degree dip reservoir. The region where reservoir pressure increases in response to CO2 injection is typically much larger than the CO2 plume. It can thus be anticipated that there will be basin wide interactions between different CO2 injection sources if multiple, large volume sites are developed. This interaction will result in asymmetric plume migration that may be contrary to reservoir dip. A basin- scale simulation model is being developed to predict CO2 plume migration, brine displacement, and pressure buildup for a possible future sequestration scenario featuring multiple CO2 storage sites within the Illinois Basin Mt. Simon Sandstone. Interactions between different sites will be evaluated with respect to impacts on pressure and CO2 plume migration patterns. ?? 2009 Elsevier Ltd. All rights reserved.
NASA Astrophysics Data System (ADS)
Sullivan, A. B.; Mulholland, P. J.; Jones, J. B.
2001-05-01
Headwater streams are almost always supersaturated with CO2 compared to concentrations expected in equilibrium with atmospheric CO2. Direct measurements of CO2 in two streams in eastern Tennessee with different bedrock lithologies (Walker Branch, Upper Gum Hollow Branch) over a year revealed levels of supersaturation of two to five times atmospheric CO2. Highest levels were generally found during the summer months. Springs discharging into the stream had dissolved CO2 concentration up to an order of magnitude higher than that in streamwater. These levels of supersaturation are a reflection of the high concentrations of CO2 in soil produced by root respiration and organic matter decomposition. The hydrologic connection between soil CO2 and streamwater CO2 forms the basis of our method to determine soil CO2 concentrations and efflux from the soil to the atmosphere. The method starts with streamwater measurements of CO2. Then corrections are made for evasion from the stream surface using injections of a conservative solute tracer and volatile gas, and for instream metabolism using a dissolved oxygen change technique. The approach then works backward along the hydrologic flowpath and evaluates the contribution of bedrock weathering, which consumes CO2, by examining the changes in major ion chemistry between precipitation and the stream. This produces estimates of CO2 concentration in soil water and soil atmosphere, which when coupled with soil porosity, allows estimation of CO2 efflux from soil. The hydrologic integration of CO2 signals from whole watersheds into streamwater allows calculation of soil CO2 efflux at large scales. These estimates are at scales larger than current chamber or tower methods, and can provide broad estimates of soil CO2 efflux with easily collected stream chemistry data.
Lifetime of carbon capture and storage as a climate-change mitigation technology
Szulczewski, Michael L.; MacMinn, Christopher W.; Herzog, Howard J.; Juanes, Ruben
2012-01-01
In carbon capture and storage (CCS), CO2 is captured at power plants and then injected underground into reservoirs like deep saline aquifers for long-term storage. While CCS may be critical for the continued use of fossil fuels in a carbon-constrained world, the deployment of CCS has been hindered by uncertainty in geologic storage capacities and sustainable injection rates, which has contributed to the absence of concerted government policy. Here, we clarify the potential of CCS to mitigate emissions in the United States by developing a storage-capacity supply curve that, unlike current large-scale capacity estimates, is derived from the fluid mechanics of CO2 injection and trapping and incorporates injection-rate constraints. We show that storage supply is a dynamic quantity that grows with the duration of CCS, and we interpret the lifetime of CCS as the time for which the storage supply curve exceeds the storage demand curve from CO2 production. We show that in the United States, if CO2 production from power generation continues to rise at recent rates, then CCS can store enough CO2 to stabilize emissions at current levels for at least 100 y. This result suggests that the large-scale implementation of CCS is a geologically viable climate-change mitigation option in the United States over the next century. PMID:22431639
Quantification of fossil fuel CO2 emissions on the building/street scale for a large U.S. city.
Gurney, Kevin R; Razlivanov, Igor; Song, Yang; Zhou, Yuyu; Benes, Bedrich; Abdul-Massih, Michel
2012-11-06
In order to advance the scientific understanding of carbon exchange with the land surface, build an effective carbon monitoring system, and contribute to quantitatively based U.S. climate change policy interests, fine spatial and temporal quantification of fossil fuel CO(2) emissions, the primary greenhouse gas, is essential. Called the "Hestia Project", this research effort is the first to use bottom-up methods to quantify all fossil fuel CO(2) emissions down to the scale of individual buildings, road segments, and industrial/electricity production facilities on an hourly basis for an entire urban landscape. Here, we describe the methods used to quantify the on-site fossil fuel CO(2) emissions across the city of Indianapolis, IN. This effort combines a series of data sets and simulation tools such as a building energy simulation model, traffic data, power production reporting, and local air pollution reporting. The system is general enough to be applied to any large U.S. city and holds tremendous potential as a key component of a carbon-monitoring system in addition to enabling efficient greenhouse gas mitigation and planning. We compare the natural gas component of our fossil fuel CO(2) emissions estimate to consumption data provided by the local gas utility. At the zip code level, we achieve a bias-adjusted Pearson r correlation value of 0.92 (p < 0.001).
Detection of Chemicals Inhibiting Photorespiratory Senescence in a Large Scale Survival Chamber
Manning, David T.; Campbell, Andrew J.; Chen, Tsong Meng; Tolbert, N. E.; Smith, E. Wayne
1984-01-01
A large scale survival chamber was developed as a screen for detecting chemical treatments that extend the survival time of illuminated soybean seedlings at CO2 concentrations below the compensation point. In theory, extended survival should indicate potential for improved crop performance via decreased photorespiration and increased photosynthetic efficiency. An automated control system regulated CO2 concentrations, temperature and plant watering during a continuous CO2-removal photoperiod of 72 hours. An endogenously controlled circadian rhythm of net photosynthesis occurred throughout the continuous light treatment. Spray applications of 3.49 millimolar 2-(4-chlorophenoxy)-2-methylpropanoic acid (CPMP) significantly decreased leaf chlorophyll loss, compared with the control, after 72 hours of subcompensation-point stress. Treatment with CPMP also consistently increased leaf chlorophyll per unit area under nonstress greenhouse conditions. These effects may be due to increases in specific leaf weight produced by CPMP although the compound did not consistently act as a height retardant. The compound, 3-butyl-2-hydroxy-4H-pyrido[1,2-a]pyrimidin-4-one (BHPP), inhibited senescence under low CO2 conditions but did not decrease leaf light transmission at ambient CO2 levels. The cytokinin N6-benzyladenine (BA) retarded low CO2 stress senescence although greening effects were not observed. Neither 2-hydroxy-3-butynoic acid (HBA) nor its butyl ester, inhibitors of glycolate oxidase, influenced low CO2 survival. Cyclohexanecarboxylic acid (CHCA) and sodium naphthenate had no effect upon subcompensation-point senescence. Antisenescence effects of CPMP, BHPP, and BA do not appear to be directly attributable to effects upon the competing carbon paths of photosynthesis and photorespiration. Protection against low CO2 stress and increased chlorophyll synthesis under nonstress conditions may represent separate effects upon plastids by some of the compounds. This screen will identify compounds which inhibit photorespiratory senescence without decreasing the CO2 compensation point. Images Fig. 1 PMID:16663949
NASA Astrophysics Data System (ADS)
Park, Yongchan; Choi, Byoungyoung; Shinn, Youngjae
2015-04-01
Captured CO2 streams contain various levels of impurities which vary depending on the combustion technology and CO2 sources such as a power plant and iron and steel production processes. Common impurities or contaminants are non-condensable gases like nitrogen, oxygen and hydrogen, and are also air pollutants like sulphur and nitrogen oxides. Specifically for geological storage, the non-condensable gases in CO2 streams are not favourable because they can decrease density of the injected CO2 stream and can affect buoyancy of the plume. However, separation of these impurities to obtain the CO2 purity higher than 99% would greatly increase the cost of capture. In 2010, the Korean Government announced a national framework to develop CCS, with the aim of developing two large scale integrated CCS projects by 2020. In order to achieve this goal, a small scale injection project into Pohang basin near shoreline has begun which is seeking the connection with a capture project, especially at a steel company. Any onshore sites that are suitable for the geological storage are not identified by this time so we turned to the shallow offshore Pohang basin where is close to a large-scale CO2 source. Currently, detailed site surveys are being undertaken and the collected data were used to establish a geological model of the basin. In this study, we performed preliminary modelling study on the effect of impurities on the geological storage using the geological model. Using a potential compositions of impurities in CO2 streams from the steel company, we firstly calculated density and viscosity of CO2 streams as a function of various pressure and temperature conditions with CMG-WINPROP and then investigated the effect of the non-condensable gases on storage capacity, injectivity and plume migrations with CMG-GEM. Further simulations to evaluate the areal and vertical sweep efficiencies by impurities were perform in a 2D vertical cross section as well as in a 3D simulation grid. Also, pressure increases caused by the impurities and the partitioning between CO2 and other non-condensable gases were explored. In addition, the possibility of using these contaminants as a tracer were examined.
NASA Astrophysics Data System (ADS)
Kort, E. A.; Gvakharia, A.; Smith, M. L.; Conley, S.; Frauhammer, K.
2017-12-01
Nitrous Oxide (N2O) is a crucial atmospheric trace gas that drives 21st century stratospheric ozone depletion and substantively impacts climate. Anthropogenic emissions drive the global imbalance and annual growth of N2O, and the dominant anthropogenic source is fertilizer production and application, both of which have large uncertainties. In this presentation we will discuss the FEAST campaign, a study designed to demonstrate new approaches to quantify N2O emissions from fertilizer production and usage with aircraft measurements. In the FEAST campaign we deployed new instrumentation along with experienced flight sensors onboard the Scientific Aviation Mooney aircraft to make 40 hours of continuous 1Hz measurements of N2O, CO2, CO, H2O, CH4, O3, T, and winds. The Mississippi River Valley provided an optimal target as this location includes significant fertilizer production facilities as well as large cropland areas (dominated by corn, soy, rice, and cotton) with substantive fertilizer application. By leveraging our payload and unique airborne capabilities we directly observe and quantify N2O emissions from individual fertilizer production facilities (as well as CO2 and CH4 emissions from these same facilities). We are also able to quantify N2O fluxes from large cropland areas ( 100's km) employing a mass balance approach, a first for N2O, and will show results highlighting differences between crop types and amounts of applied fertilizer. The ability to quantify fluxes of croplands at 100km scale enables new understanding of processes controlling emissions at spatial scales that has eluded prior studies that either rely on extrapolation of small (flux chamber, towers), or work on 1,000+ km spatial scales (regional-global inversions from atmospheric measurements).
Improved simulation of regional CO2 surface concentrations using GEOS-Chem and fluxes from VEGAS
NASA Astrophysics Data System (ADS)
Chen, Z. H.; Zhu, J.; Zeng, N.
2013-08-01
CO2 measurements have been combined with simulated CO2 distributions from a transport model in order to produce the optimal estimates of CO2 surface fluxes in inverse modeling. However, one persistent problem in using model-observation comparisons for this goal relates to the issue of compatibility. Observations at a single station reflect all underlying processes of various scales. These processes usually cannot be fully resolved by model simulations at the grid points nearest the station due to lack of spatial or temporal resolution or missing processes in the model. In this study the stations in one region were grouped based on the amplitude and phase of the seasonal cycle at each station. The regionally averaged CO2 at all stations in one region represents the regional CO2 concentration of this region. The regional CO2 concentrations from model simulations and observations were used to evaluate the regional model results. The difference of the regional CO2 concentration between observation and modeled results reflects the uncertainty of the large-scale flux in the region where the grouped stations are. We compared the regional CO2 concentrations between model results with biospheric fluxes from the Carnegie-Ames-Stanford Approach (CASA) and VEgetation-Global-Atmosphere-Soil (VEGAS) models, and used observations from GLOBALVIEW-CO2 to evaluate the regional model results. The results show the largest difference of the regionally averaged values between simulations with fluxes from VEGAS and observations is less than 5 ppm for North American boreal, North American temperate, Eurasian boreal, Eurasian temperate and Europe, which is smaller than the largest difference between CASA simulations and observations (more than 5 ppm). There is still a large difference between two model results and observations for the regional CO2 concentration in the North Atlantic, Indian Ocean, and South Pacific tropics. The regionally averaged CO2 concentrations will be helpful for comparing CO2 concentrations from modeled results and observations and evaluating regional surface fluxes from different methods.
NASA Astrophysics Data System (ADS)
Campbell, J. E.; Hilton, T. W.; Laine, M.; Wang, Y.; Berry, J. A.; Hannigan, J. W.
2017-12-01
The seasonal amplitude in atmospheric CO2 has grown over the last 50 years, pointing to a fundamental shift in the regional carbon cycle. Theoretical drivers from the amplitude growth include changes in terrestrial photosynthesis and heterotrophic respiration. However, large-scale, measurement-based evidence for these mechanisms is unclear. Here we analyze historical measurements of carbonyl sulfide which also show long-term growth in seasonal amplitude. We use this new trend to interpret the underlying mechanisms of CO2 amplitude growth and to validate global ecosystem models.
Gibon, Thomas; Wood, Richard; Arvesen, Anders; Bergesen, Joseph D; Suh, Sangwon; Hertwich, Edgar G
2015-09-15
Climate change mitigation demands large-scale technological change on a global level and, if successfully implemented, will significantly affect how products and services are produced and consumed. In order to anticipate the life cycle environmental impacts of products under climate mitigation scenarios, we present the modeling framework of an integrated hybrid life cycle assessment model covering nine world regions. Life cycle assessment databases and multiregional input-output tables are adapted using forecasted changes in technology and resources up to 2050 under a 2 °C scenario. We call the result of this modeling "technology hybridized environmental-economic model with integrated scenarios" (THEMIS). As a case study, we apply THEMIS in an integrated environmental assessment of concentrating solar power. Life-cycle greenhouse gas emissions for this plant range from 33 to 95 g CO2 eq./kWh across different world regions in 2010, falling to 30-87 g CO2 eq./kWh in 2050. Using regional life cycle data yields insightful results. More generally, these results also highlight the need for systematic life cycle frameworks that capture the actual consequences and feedback effects of large-scale policies in the long term.
Zheng, Yun; Wang, Jianchen; Yu, Bo; Zhang, Wenqiang; Chen, Jing; Qiao, Jinli; Zhang, Jiujun
2017-03-06
High-temperature solid oxide electrolysis cells (SOECs) are advanced electrochemical energy storage and conversion devices with high conversion/energy efficiencies. They offer attractive high-temperature co-electrolysis routes that reduce extra CO 2 emissions, enable large-scale energy storage/conversion and facilitate the integration of renewable energies into the electric grid. Exciting new research has focused on CO 2 electrochemical activation/conversion through a co-electrolysis process based on the assumption that difficult C[double bond, length as m-dash]O double bonds can be activated effectively through this electrochemical method. Based on existing investigations, this paper puts forth a comprehensive overview of recent and past developments in co-electrolysis with SOECs for CO 2 conversion and utilization. Here, we discuss in detail the approaches of CO 2 conversion, the developmental history, the basic principles, the economic feasibility of CO 2 /H 2 O co-electrolysis, and the diverse range of fuel electrodes as well as oxygen electrode materials. SOEC performance measurements, characterization and simulations are classified and presented in this paper. SOEC cell and stack designs, fabrications and scale-ups are also summarized and described. In particular, insights into CO 2 electrochemical conversions, solid oxide cell material behaviors and degradation mechanisms are highlighted to obtain a better understanding of the high temperature electrolysis process in SOECs. Proposed research directions are also outlined to provide guidelines for future research.
NASA Astrophysics Data System (ADS)
Zhang, Jingyong; Wu, Lingyun; Huang, Gang; Notaro, Michael
2011-02-01
In this study, we focus on a deciduous forest in central Massachusetts and investigate the relationships between global climate indices and CO2 exchange using eddy-covariance flux measurements from 1992 to 2007. Results suggest that large-scale circulation patterns influence the annual CO2 exchange in the forest through their effects on the local surface climate. Annual gross ecosystem exchange (GEE) in the forest is closely associated with spring El Niño-Southern Oscillation (ENSO) and Pacific Decadal Oscillation (PDO), previous fall Atlantic Multidecadal Oscillation (AMO), and previous winter East Pacific-North Pacific (EP-NP) pattern. Annual net ecosystem exchange (NEE) responds to previous fall AMO and PDO, while annual respiration (R) is impacted by previous fall ENSO and Pacific/North American Oscillation (PNA). Regressions based on these relationships are developed to simulate the annual GEE, NEE, and R. To avoid problems of multicollinearity, we compute a "Composite Index for GEE (CIGEE)" based on a linear combination of spring ENSO and PDO, fall AMO, and winter EP-NP and a "Composite Index for R (CIR)" based on a linear combination of fall ENSO and PNA. CIGEE, CIR, and fall AMO and PDO can explain 41, 27, and 40% of the variance of the annual GEE, R, and NEE, respectively. We further apply the methodology to two other northern midlatitude forests and find that interannual variabilities in NEE of the two forests are largely controlled by large-scale circulation patterns. This study suggests that global climate indices provide the potential for predicting CO2 exchange variability in the northern midlatitude forests.
Impacts of large-scale climatic disturbances on the terrestrial carbon cycle.
Erbrecht, Tim; Lucht, Wolfgang
2006-07-27
The amount of carbon dioxide in the atmosphere steadily increases as a consequence of anthropogenic emissions but with large interannual variability caused by the terrestrial biosphere. These variations in the CO2 growth rate are caused by large-scale climate anomalies but the relative contributions of vegetation growth and soil decomposition is uncertain. We use a biogeochemical model of the terrestrial biosphere to differentiate the effects of temperature and precipitation on net primary production (NPP) and heterotrophic respiration (Rh) during the two largest anomalies in atmospheric CO2 increase during the last 25 years. One of these, the smallest atmospheric year-to-year increase (largest land carbon uptake) in that period, was caused by global cooling in 1992/93 after the Pinatubo volcanic eruption. The other, the largest atmospheric increase on record (largest land carbon release), was caused by the strong El Niño event of 1997/98. We find that the LPJ model correctly simulates the magnitude of terrestrial modulation of atmospheric carbon anomalies for these two extreme disturbances. The response of soil respiration to changes in temperature and precipitation explains most of the modelled anomalous CO2 flux. Observed and modelled NEE anomalies are in good agreement, therefore we suggest that the temporal variability of heterotrophic respiration produced by our model is reasonably realistic. We therefore conclude that during the last 25 years the two largest disturbances of the global carbon cycle were strongly controlled by soil processes rather then the response of vegetation to these large-scale climatic events.
Impacts of large-scale climatic disturbances on the terrestrial carbon cycle
Erbrecht, Tim; Lucht, Wolfgang
2006-01-01
Background The amount of carbon dioxide in the atmosphere steadily increases as a consequence of anthropogenic emissions but with large interannual variability caused by the terrestrial biosphere. These variations in the CO2 growth rate are caused by large-scale climate anomalies but the relative contributions of vegetation growth and soil decomposition is uncertain. We use a biogeochemical model of the terrestrial biosphere to differentiate the effects of temperature and precipitation on net primary production (NPP) and heterotrophic respiration (Rh) during the two largest anomalies in atmospheric CO2 increase during the last 25 years. One of these, the smallest atmospheric year-to-year increase (largest land carbon uptake) in that period, was caused by global cooling in 1992/93 after the Pinatubo volcanic eruption. The other, the largest atmospheric increase on record (largest land carbon release), was caused by the strong El Niño event of 1997/98. Results We find that the LPJ model correctly simulates the magnitude of terrestrial modulation of atmospheric carbon anomalies for these two extreme disturbances. The response of soil respiration to changes in temperature and precipitation explains most of the modelled anomalous CO2 flux. Conclusion Observed and modelled NEE anomalies are in good agreement, therefore we suggest that the temporal variability of heterotrophic respiration produced by our model is reasonably realistic. We therefore conclude that during the last 25 years the two largest disturbances of the global carbon cycle were strongly controlled by soil processes rather then the response of vegetation to these large-scale climatic events. PMID:16930463
Gately, Conor K; Hutyra, Lucy R; Peterson, Scott; Sue Wing, Ian
2017-10-01
On-road emissions vary widely on time scales as short as minutes and length scales as short as tens of meters. Detailed data on emissions at these scales are a prerequisite to accurately quantifying ambient pollution concentrations and identifying hotspots of human exposure within urban areas. We construct a highly resolved inventory of hourly fluxes of CO, NO 2 , NO x , PM 2.5 and CO 2 from road vehicles on 280,000 road segments in eastern Massachusetts for the year 2012. Our inventory integrates a large database of hourly vehicle speeds derived from mobile phone and vehicle GPS data with multiple regional datasets of vehicle flows, fleet characteristics, and local meteorology. We quantify the 'excess' emissions from traffic congestion, finding modest congestion enhancement (3-6%) at regional scales, but hundreds of local hotspots with highly elevated annual emissions (up to 75% for individual roadways in key corridors). Congestion-driven reductions in vehicle fuel economy necessitated 'excess' consumption of 113 million gallons of motor fuel, worth ∼ $415M, but this accounted for only 3.5% of the total fuel consumed in Massachusetts, as over 80% of vehicle travel occurs in uncongested conditions. Across our study domain, emissions are highly spatially concentrated, with 70% of pollution originating from only 10% of the roads. The 2011 EPA National Emissions Inventory (NEI) understates our aggregate emissions of NO x , PM 2.5 , and CO 2 by 46%, 38%, and 18%, respectively. However, CO emissions agree within 5% for the two inventories, suggesting that the large biases in NO x and PM 2.5 emissions arise from differences in estimates of diesel vehicle activity. By providing fine-scale information on local emission hotspots and regional emissions patterns, our inventory framework supports targeted traffic interventions, transparent benchmarking, and improvements in overall urban air quality. Copyright © 2017 Elsevier Ltd. All rights reserved.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Schaap, Marcel G.
Carbon capture and storage (CCS) of carbon dioxide emissions generated by production or combustion of fossil fuels is a technologically viable means to reduce the build-up of CO2 in the atmosphere and oceans. Using advantages of scale and location, CCS is particularly suitable for large point sources near ubiquitous deep saline aquifers, depleted gas reservoirs, or at production reservoirs for enhanced oil recovery (EOR). In the BES-funded research project, Oregon State University (OSU) carried out capillary trapping experiments with proxy fluids that mimic the properties of the scCO2/brine system under ambient temperatures and pressures, and successfully developed a unique andmore » novel x-ray compatible, high-pressure, elevated temperature setup to study the scCO2/brine system under challenging reservoir conditions. Both methodologies were applied to a variety of porous media, including synthetic (glass bead) and geologic (Bentheimer sandstone) materials. The University of Arizona (UA) developed pore-scale lattice Boltzmann (LB) models which are able to handle the experimental conditions for proxy fluids, as well as the scCO2/brine system, that are capable of simulating permeability in volumes of tens of millions of fluid elements. We reached the following summary findings (main institute indicated): 1. (OSU/UA) To understand capillary trapping in a multiphase fluid-porous medium system, the system must be analyzed from a pore-scale force balance perspective; trapping can be enhanced by manipulating wetting and nonwetting phase fluid properties. 2. (OSU) Pore-scale fluid connectivity and topology has a clear and direct effect on nonwetting phase capillary trapping efficiency. 3. (OSU) Rock type and flow regime also have a pronounced effects on capillary trapping. 4. (OSU/UA) There is a predictable relationship between NWP connectivity and NWP saturation, which allows for development of injection strategies that optimize trapping. The commonly used Land model (Land, 1968) does not predict amount of trapped NWP accurately. 5. (UA) There are ambiguities regarding the segmentation of large-volume gray-scale CT data into pore-volumes suitable for pore-scale modeling. Simulated permeabilities vary by three orders of magnitude and do not resemble observed values very well. Small-volume synchrotron-based CT data (such as produced by OSU) does not suffer significantly from segmentation ambiguities. 6. (UA) A standard properly parameterized Shan-Chen model LB model is useful for simulating porous media with proxy fluids as well as the scCO2/brine system and produces results that are consistent with tomographic observations. 7. (UA) A LB model with fluid-interactions defined by a (modified) Peng-Robinson Equation of State is able to handle the scCO2/brine system with variable solid phase wettability. This model is numerically stable at temperatures between 0 and 250 °C and pressures between 3 and 50 MPa, and produces appropriate densities above the critical point of CO2 and exhibits three-phase separation below. Based on above findings OSU and UA have proposed continued experimentation and pore-scale modeling of the scCO2/brine system. The reported research has extensively covered capillary trapping using proxy fluids, but due to limited beam-time availability we were unable to apply our high-pressure CO2 setup to sufficient variation in fluid properties, and initial scCO2 connectivity. New data will also allow us to test, calibrate and apply our LB models to reservoir conditions beyond those that are currently feasible experimentally. Such experiments and simulations will also allow us to provide information how suitable proxy fluids are for the scCO2/brine system. We believe it would be worthwhile to pursue the following new research questions: 1. What are the fundamental differences in the physics underlying capillary trapping at ambient vs. supercritical conditions? 2. Do newly developed pore-scale trapping interactions and relationships translate to continuum scales? A motivation for these questions was elaborated in “Capillary Trapping of Super-Critical CO2: Linking Pore and Continuum Scales to Verify new Relationships” that was submitted to DOE-BES in 2015.« less
Amazon River carbon dioxide outgassing fuelled by wetlands.
Abril, Gwenaël; Martinez, Jean-Michel; Artigas, L Felipe; Moreira-Turcq, Patricia; Benedetti, Marc F; Vidal, Luciana; Meziane, Tarik; Kim, Jung-Hyun; Bernardes, Marcelo C; Savoye, Nicolas; Deborde, Jonathan; Souza, Edivaldo Lima; Albéric, Patrick; Landim de Souza, Marcelo F; Roland, Fabio
2014-01-16
River systems connect the terrestrial biosphere, the atmosphere and the ocean in the global carbon cycle. A recent estimate suggests that up to 3 petagrams of carbon per year could be emitted as carbon dioxide (CO2) from global inland waters, offsetting the carbon uptake by terrestrial ecosystems. It is generally assumed that inland waters emit carbon that has been previously fixed upstream by land plant photosynthesis, then transferred to soils, and subsequently transported downstream in run-off. But at the scale of entire drainage basins, the lateral carbon fluxes carried by small rivers upstream do not account for all of the CO2 emitted from inundated areas downstream. Three-quarters of the world's flooded land consists of temporary wetlands, but the contribution of these productive ecosystems to the inland water carbon budget has been largely overlooked. Here we show that wetlands pump large amounts of atmospheric CO2 into river waters in the floodplains of the central Amazon. Flooded forests and floating vegetation export large amounts of carbon to river waters and the dissolved CO2 can be transported dozens to hundreds of kilometres downstream before being emitted. We estimate that Amazonian wetlands export half of their gross primary production to river waters as dissolved CO2 and organic carbon, compared with only a few per cent of gross primary production exported in upland (not flooded) ecosystems. Moreover, we suggest that wetland carbon export is potentially large enough to account for at least the 0.21 petagrams of carbon emitted per year as CO2 from the central Amazon River and its floodplains. Global carbon budgets should explicitly address temporary or vegetated flooded areas, because these ecosystems combine high aerial primary production with large, fast carbon export, potentially supporting a substantial fraction of CO2 evasion from inland waters.
CoCoNUT: an efficient system for the comparison and analysis of genomes
2008-01-01
Background Comparative genomics is the analysis and comparison of genomes from different species. This area of research is driven by the large number of sequenced genomes and heavily relies on efficient algorithms and software to perform pairwise and multiple genome comparisons. Results Most of the software tools available are tailored for one specific task. In contrast, we have developed a novel system CoCoNUT (Computational Comparative geNomics Utility Toolkit) that allows solving several different tasks in a unified framework: (1) finding regions of high similarity among multiple genomic sequences and aligning them, (2) comparing two draft or multi-chromosomal genomes, (3) locating large segmental duplications in large genomic sequences, and (4) mapping cDNA/EST to genomic sequences. Conclusion CoCoNUT is competitive with other software tools w.r.t. the quality of the results. The use of state of the art algorithms and data structures allows CoCoNUT to solve comparative genomics tasks more efficiently than previous tools. With the improved user interface (including an interactive visualization component), CoCoNUT provides a unified, versatile, and easy-to-use software tool for large scale studies in comparative genomics. PMID:19014477
Liu, Heping; Zhang, Qianyu; Katul, Gabriel G.; ...
2016-05-24
CO 2 emissions from inland waters are commonly determined by indirect methods that are based on the product of a gas transfer coefficient and the concentration gradient at the air water interface (e.g., wind-based gas transfer models). The measurements of concentration gradient are typically collected during the day in fair weather throughout the course of a year. Direct measurements of eddy covariance CO 2 fluxes from a large inland water body (Ross Barnett reservoir, Mississippi, USA) show that CO 2 effluxes at night are approximately 70% greater than those during the day. At longer time scales, frequent synoptic weather eventsmore » associated with extratropical cyclones induce CO 2 flux pulses, resulting in further increase in annual CO 2 effluxes by 16%. Therefore, CO 2 emission rates from this reservoir, if these diel and synoptic processes are under-sampled, are likely to be underestimated by approximately 40%. Our results also indicate that the CO 2 emission rates from global inland waters reported in the literature, when based on indirect methods, are likely underestimated. Field samplings and indirect modeling frameworks that estimate CO 2 emissions should account for both daytime-nighttime efflux difference and enhanced emissions during synoptic weather events. Furthermore, the analysis here can guide carbon emission sampling to improve regional carbon estimates.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Liu, Heping; Zhang, Qianyu; Katul, Gabriel G.
CO 2 emissions from inland waters are commonly determined by indirect methods that are based on the product of a gas transfer coefficient and the concentration gradient at the air water interface (e.g., wind-based gas transfer models). The measurements of concentration gradient are typically collected during the day in fair weather throughout the course of a year. Direct measurements of eddy covariance CO 2 fluxes from a large inland water body (Ross Barnett reservoir, Mississippi, USA) show that CO 2 effluxes at night are approximately 70% greater than those during the day. At longer time scales, frequent synoptic weather eventsmore » associated with extratropical cyclones induce CO 2 flux pulses, resulting in further increase in annual CO 2 effluxes by 16%. Therefore, CO 2 emission rates from this reservoir, if these diel and synoptic processes are under-sampled, are likely to be underestimated by approximately 40%. Our results also indicate that the CO 2 emission rates from global inland waters reported in the literature, when based on indirect methods, are likely underestimated. Field samplings and indirect modeling frameworks that estimate CO 2 emissions should account for both daytime-nighttime efflux difference and enhanced emissions during synoptic weather events. Furthermore, the analysis here can guide carbon emission sampling to improve regional carbon estimates.« less
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
NASA Astrophysics Data System (ADS)
Basu, Sourish; Bharat Miller, John; Lehman, Scott
2016-05-01
National annual total CO2 emissions from combustion of fossil fuels are likely known to within 5-10 % for most developed countries. However, uncertainties are inevitably larger (by unknown amounts) for emission estimates at regional and monthly scales, or for developing countries. Given recent international efforts to establish emission reduction targets, independent determination and verification of regional and national scale fossil fuel CO2 emissions are likely to become increasingly important. Here, we take advantage of the fact that precise measurements of 14C in CO2 provide a largely unbiased tracer for recently added fossil-fuel-derived CO2 in the atmosphere and present an atmospheric inversion technique to jointly assimilate observations of CO2 and 14CO2 in order to simultaneously estimate fossil fuel emissions and biospheric exchange fluxes of CO2. Using this method in a set of Observation System Simulation Experiments (OSSEs), we show that given the coverage of 14CO2 measurements available in 2010 (969 over North America, 1063 globally), we can recover the US national total fossil fuel emission to better than 1 % for the year and to within 5 % for most months. Increasing the number of 14CO2 observations to ˜ 5000 per year over North America, as recently recommended by the National Academy of Science (NAS) (Pacala et al., 2010), we recover monthly emissions to within 5 % for all months for the US as a whole and also for smaller, highly emissive regions over which the specified data coverage is relatively dense, such as for the New England states or the NY-NJ-PA tri-state area. This result suggests that, given continued improvement in state-of-the art transport models, a measurement program similar in scale to that recommended by the NAS can provide for independent verification of bottom-up inventories of fossil fuel CO2 at the regional and national scale. In addition, we show that the dual tracer inversion framework can detect and minimize biases in estimates of the biospheric flux that would otherwise arise in a traditional CO2-only inversion when prescribing fixed but inaccurate fossil fuel fluxes.
Critical Dynamics of Gravito-Convective Mixing in Geological Carbon Sequestration
Soltanian, Mohamad Reza; Amooie, Mohammad Amin; Dai, Zhenxue; Cole, David; Moortgat, Joachim
2016-01-01
When CO2 is injected in saline aquifers, dissolution causes a local increase in brine density that can cause Rayleigh-Taylor-type gravitational instabilities. Depending on the Rayleigh number, density-driven flow may mix dissolved CO2 throughout the aquifer at fast advective time-scales through convective mixing. Heterogeneity can impact density-driven flow to different degrees. Zones with low effective vertical permeability may suppress fingering and reduce vertical spreading, while potentially increasing transverse mixing. In more complex heterogeneity, arising from the spatial organization of sedimentary facies, finger propagation is reduced in low permeability facies, but may be enhanced through more permeable facies. The connectivity of facies is critical in determining the large-scale transport of CO2-rich brine. We perform high-resolution finite element simulations of advection-diffusion transport of CO2 with a focus on facies-based bimodal heterogeneity. Permeability fields are generated by a Markov Chain approach, which represent facies architecture by commonly observed characteristics such as volume fractions. CO2 dissolution and phase behavior are modeled with the cubic-plus-association equation-of-state. Our results show that the organization of high-permeability facies and their connectivity control the dynamics of gravitationally unstable flow. We discover new flow regimes in both homogeneous and heterogeneous media and present quantitative scaling relations for their temporal evolution. PMID:27808178
Emissions of nitrous oxide from biomass burning
NASA Technical Reports Server (NTRS)
Winstead, Edward L.; Cofer, Wesley R., III; Levine, Joel S.
1991-01-01
A study has been conducted which compared N2O results obtained over large prescribed fires or wildfires, in which 'grab-sampling' with storage had been used with N2O measurements made in near-real time. CO2-normalized emission ratios obtained initially from the laboratory fires are substantially lower than those obtained over large-scale biomass fires. Combustion may not be the only source of N2O in large fire smoke plumes; physical, chemical, and biochemical processes in the soil may be altered by large biomass fires, leading to large N2O releases.
Star formation associated with a large-scale infrared bubble
NASA Astrophysics Data System (ADS)
Xu, Jin-Long; Ju, Bing-Gang
2014-09-01
Aims: To investigate how a large-scale infrared bubble centered at l = 53.9° and b = 0.2° forms, and to study if star formation is taking place at the periphery of the bubble, we performed a multiwavelength study. Methods: Using the data from the Galactic Ring Survey (GRS) and Galactic Legacy Infrared Mid-Plane Survey Extraordinaire (GLIMPSE), we performed a study of a large-scale infrared bubble with a size of about 16 pc at a distance of 2.0 kpc. We present the 12CO J = 1-0, 13CO J = 1-0, and C18O J = 1-0 observations of HII region G53.54-0.01 (Sh2-82) obtained at the Purple Mountain Observation (PMO) 13.7 m radio telescope to investigate the detailed distribution of associated molecular material. In addition, we also used radiorecombination line and VLA data. To select young stellar objects (YSOs) consistent with this region, we used the GLIMPSE I catalog. Results: The large-scale infrared bubble shows a half-shell morphology at 8 μm. The H II regions of G53.54-0.01, G53.64+0.24, and G54.09-0.06 are situated on the bubble. Comparing the radio recombination line velocities and associated 13CO J = 1-0 components of the three H II regions, we found that the 8 μm emission associated with H II region G53.54-0.01 should belong to the foreground emission, and only overlap with the large-scale infrared bubble in the line of sight. Three extended green objects (EGOs, the candidate massive young stellar objects), as well as three H II regions and two small-scale bubbles are found located in the G54.09-0.06 complex, indicating an active massive star-forming region. Emission from C18O at J = 1-0 presents four cloud clumps on the northeastern border of H II region G53.54-0.01. By comparing the spectral profiles of 12CO J = 1-0, 13CO J = 1-0, and C18O J = 1-0 at the peak position of each clump, we found the collected gas in the three clumps, except for the clump coinciding with a massive YSO (IRAS 19282+1814). Using the evolutive model of the H II region, we derived that the age of H II region G53.54-0.01 is 1.5 × 106 yr. The significant enhancement of several Class I and Class II YSOs around G53.54-0.01 indicates the presence of some recently formed stars, which may be triggered by this H II region through the collect-and-collapse process. Final CO cubes (12, 13, 18, FITS format) are only available at the CDS via anonymous ftp to http://cdsarc.u-strasbg.fr (ftp://130.79.128.5) or via http://cdsarc.u-strasbg.fr/viz-bin/qcat?J/A+A/569/A36
The economics and environmental impacts of large-scale wind power in a carbon constrained world
NASA Astrophysics Data System (ADS)
Decarolis, Joseph Frank
Serious climate change mitigation aimed at stabilizing atmospheric concentrations of CO2 will require a radical shift to a decarbonized energy supply. The electric power sector will be a primary target for deep reductions in CO2 emissions because electric power plants are among the largest and most manageable point sources of emissions. With respect to new capacity, wind power is currently one of the most inexpensive ways to produce electricity without CO2 emissions and it may have a significant role to play in a carbon constrained world. Yet most research in the wind industry remains focused on near term issues, while energy system models that focus on century-long time horizons undervalue wind by imposing exogenous limits on growth. This thesis fills a critical gap in the literature by taking a closer look at the cost and environmental impacts of large-scale wind. Estimates of the average cost of wind generation---now roughly 4¢/kWh---do not address the cons arising from the spatial distribution and intermittency of wind. This thesis develops a theoretical framework for assessing the intermittency cost of wind. In addition, an economic characterization of a wind system is provided in which long-distance electricity transmission, storage, and gas turbines are used to supplement variable wind power output to meet a time-varying load. With somewhat optimistic assumptions about the cost of wind turbines, the use of wind to serve 50% of demand adds ˜1--2¢/kWh to the cost of electricity, a cost comparable to that of other large-scale low carbon technologies. This thesis also explores the environmental impacts posed by large-scale wind. Though avian mortality and noise caused controversy in the early years of wind development, improved technology and exhaustive siting assessments have minimized their impact. The aesthetic valuation of wind farms can be improved significantly with better design, siting, construction, and maintenance procedures, but opposition may increase as wind is developed on a large scale. Finally, this thesis summarizes collaborative work utilizing general circulation models to determine whether wind turbines have an impact of climate. The results suggest that the climatic impact is non-negligible at continental scales, but further research is warranted.
NASA Astrophysics Data System (ADS)
Chang, Binbin; Zhang, Shouren; Yin, Hang; Yang, Baocheng
2017-08-01
Herein, considering the great potential of nitrogen-doped hierarchical porous carbons in energy storage and CO2 capture, we designed a convenient and easily large-scale production strategy for preparing nitrogen-doped hierarchical porous carbon sphere (NHPCS) materials. In this synthesis route, spherical resorcinol-formaldehyde (RF) resins were selected as carbon precursor, and then the ZnCl2-impregnated RF resin spheres were carbonized in a NH3 atmosphere at a temperature range of 600-800 °C. During the one-step heat-treatment process, nitrogen atom could be efficiently incorporated into the carbon skeleton, and the interconnected and hierarchical pore structure with different micro/mesopore proportion could be generated and tuned by adjusting the activating agent ZnCl2 dosage and carbonization temperature. The resultant nitrogen-doped hierarchical porous carbon sphere materials exhibited a satisfactory charge storage capacity, and the optimal sample of NHPCS-2-8 with a high mesopore proportion obtained at 800 °C with a ZnCl2/RF mass ratio of 2:1 presented a specific capacitance of 273.8 F g-1 at a current density of 0.5 A g-1. More importantly, the assembled NHPCS-2-8-based symmetric capacitor displayed a high energy density of 17.2 Wh kg-1 at a power density of 178.9 W kg-1 within a voltage window of 0 ∼ 1.8 V in 0.5 M Na2SO4 aqueous electrolyte. In addition, the CO2 capture application of these NHPCS materials was also explored, and the optimal sample of NHPCS-0-8 with a large micropore proportion prepared at 800 °C exhibited an exceptional CO2 uptake capacity at ambient pressures of up to 4.23 mmol g-1 at 0 °C.
Walker, Berkley J; Orr, Douglas J; Carmo-Silva, Elizabete; Parry, Martin A J; Bernacchi, Carl J; Ort, Donald R
2017-06-01
Rates of carbon dioxide assimilation through photosynthesis are readily modeled using the Farquhar, von Caemmerer, and Berry (FvCB) model based on the biochemistry of the initial Rubisco-catalyzed reaction of net C 3 photosynthesis. As models of CO 2 assimilation rate are used more broadly for simulating photosynthesis among species and across scales, it is increasingly important that their temperature dependencies are accurately parameterized. A vital component of the FvCB model, the photorespiratory CO 2 compensation point (Γ * ), combines the biochemistry of Rubisco with the stoichiometry of photorespiratory release of CO 2 . This report details a comparison of the temperature response of Γ * measured using different techniques in three important model and crop species (Nicotiana tabacum, Triticum aestivum, and Glycine max). We determined that the different Γ * determination methods produce different temperature responses in the same species that are large enough to impact higher-scale leaf models of CO 2 assimilation rate. These differences are largest in N. tabacum and could be the result of temperature-dependent increases in the amount of CO 2 lost from photorespiration per Rubisco oxygenation reaction.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Oldenburg, Curt; Pruess, Karsten; Birkholzer, Jens
The paper examines the pressure increase resulting from injection of CO2 into a 1D radial system with closed boundaries. The finding is that unacceptably high pressures are obtained when only 1% or less of the pore volume is occupied by injected CO2. These results are used to make the general conclusion that large-scale CCS is not feasible.
Dussadee, Natthawud; Reansuwan, Kamoldara; Ramaraj, Rameshprabu
2014-03-01
This research project evaluated biogas production using anaerobic co-digestion of pig manure and elephant grass silage in large scale to delivered transportation directly for cars. Anaerobic co-digestion was estimated in three full-scale continuously stirred tank reactors (CSTRs) at 40°C. In the form of compressed bio-methane gas (CBG) production was 14,400m(3)/day (CH4 60-70%) amount of CBG was 9600m(3)/day. The procedure was enhanced by using molecular sieve, activated carbon for removal of moisture and CO2 membrane H2S and CO2 respectively. The results were demonstrated the amount of CO2, H2S gas was reduced along with CH4 was improved up to 90% by volume and compressed to 250bar tank pressure gauge to the fuel for cars. The CBG production, methane gas improvement and performance were evaluated before entering the delivered systems according to the energy standards. The production of CBG is advantageous to strengthen the Thailand biogas market. Copyright © 2014 Elsevier Ltd. All rights reserved.
Global Warming in Geologic Time
Archer, David
2018-01-01
The notion is pervasive in the climate science community and in the public at large that the climate impacts of fossil fuel CO2 release will only persist for a few centuries. This conclusion has no basis in theory or models of the atmosphere / ocean carbon cycle, which we review here. The largest fraction of the CO2 recovery will take place on time scales of centuries, as CO2 invades the ocean, but a significant fraction of the fossil fuel CO2, ranging in published models in the literature from 20-60%, remains airborne for a thousand years or longer. Ultimate recovery takes place on time scales of hundreds of thousands of years, a geologic longevity typically associated in public perceptions with nuclear waste. The glacial / interglacial climate cycles demonstrate that ice sheets and sea level respond dramatically to millennial-timescale changes in climate forcing. There are also potential positive feedbacks in the carbon cycle, including methane hydrates in the ocean, and peat frozen in permafrost, that are most sensitive to the long tail of the fossil fuel CO2 in the atmosphere.
Recent progress and perspectives in the photocatalytic CO2 reduction of Ti-oxide-based nanomaterials
NASA Astrophysics Data System (ADS)
Sohn, Youngku; Huang, Weixin; Taghipour, Fariborz
2017-02-01
The conversion of CO2 with H2O to valuable chemicals and fuels is a new solution to current environmental and energy problems, and the high energy barrier of these reactions can be overcome by the input of solar and electrical energy. However, the reduction efficiencies and selectivities of these reactions are insufficient for practical use, and significant effort and strategy are required to overcome the many obstacles preventing the large-scale application of photocatalytic CO2 reduction. This article reviews recent progress in CO2 reduction using titanium oxide-based materials and various strategic factors for increasing photocatalytic efficiency. This article also highlights non-titanium-oxide catalysts, the photoelectrocatalytic reduction of CO2, and other recent review articles concerning the recycling of CO2 to value-added carbon compounds.
Assessment of brine migration along vertical pathways due to CO2 injection
NASA Astrophysics Data System (ADS)
Kissinger, Alexander; Class, Holger
2016-04-01
Global climate change, shortage of resources and the growing usage of renewable energy sources has lead to a growing demand for the utilization of subsurface systems which may create conflicts with essential public interests such as water supply from aquifers. For example, brine migration into potential drinking water aquifers due to the injection of CO2 into deep saline aquifers is perceived as a potential threat resulting from the Carbon Capture and Storage Technology (CCS). In this work, we focus on the large scale impacts of CO2 storage on brine migration but the methodology and the obtained results may also apply to other fields like waste water disposal, where large amounts of fluid are injected into the subsurface. We consider a realistic (but not real) on-shore site in the North German Basin with characteristic geological features. In contrast to modeling on the reservoir scale, the spatial scale in this work is much larger in both vertical and lateral direction, since the regional hydrogeology is considered as well. Structures such as fault zones, hydrogeological windows in the Rupelian clay or salt wall flanks are considered as potential pathways for displaced fluids into shallow systems and their influence needs to be taken into account. Simulations on this scale always require a compromise between the accuracy of the description of the relevant physical processes, data availability and computational resources. Therefore, we test different model simplifications and discuss them with respect to the relevant physical processes and the expected data availability. The simplifications in the models are concerned with the role of salt-induced density differences on the flow, with injection of brine (into brine) instead of CO2 into brine, and with simplifying the geometry of the site.
NASA Astrophysics Data System (ADS)
Sauer, U.; Schuetze, C.; Dietrich, P.
2013-12-01
The MONACO project (Monitoring approach for geological CO2 storage sites using a hierarchic observation concept) aims to find reliable monitoring tools that work on different spatial and temporal scales at geological CO2 storage sites. This integrative hierarchical monitoring approach based on different levels of coverage and resolutions is proposed as a means of reliably detecting CO2 degassing areas at ground surface level and for identifying CO2 leakages from storage formations into the shallow subsurface, as well as CO2 releases into the atmosphere. As part of this integrative hierarchical monitoring concept, several methods and technologies from ground-based remote sensing (Open-path Fourier-transform infrared (OP-FTIR) spectroscopy), regional measurements (near-surface geophysics, chamber-based soil CO2 flux measurement) and local in-situ measurements (using shallow boreholes) will either be combined or used complementary to one another. The proposed combination is a suitable concept for investigating CO2 release sites. This also presents the possibility of adopting a modular monitoring concept whereby our monitoring approach can be expanded to incorporate other methods in various coverage scales at any temporal resolution. The link between information obtained from large-scale surveys and local in-situ monitoring can be realized by sufficient geophysical techniques for meso-scale monitoring, such as geoelectrical and self-potential (SP) surveys. These methods are useful for characterizing fluid flow and transport processes in permeable near-surface sedimentary layers and can yield important information concerning CO2-affected subsurface structures. Results of measurements carried out a natural analogue site in the Czech Republic indicate that the hierarchical monitoring approach represents a successful multidisciplinary modular concept that can be used to monitor both physical and chemical processes taking place during CO2 migration and seepage. The application of FTIR spectroscopy in combination with soil gas surveys and geophysical investigations results in a comprehensive site characterization, including atmospheric and near-surface CO2 distribution, as well as subsurface structural features. We observed a correlation of higher CO2 concentration and flux rates at the meso-scale that coincides with distinct geophysical anomalies. Here, we found prominent SP anomalies and zones of lower resistivity in the geoelectrical images compared to undisturbed regions nearby. This presentation will discuss the results we obtained and illustrate the influence of CO2 on electrical parameters measured under field conditions in relation to environmental parameters.
Urban cross-sector actions for carbon mitigation with local health co-benefits in China
NASA Astrophysics Data System (ADS)
Ramaswami, Anu; Tong, Kangkang; Fang, Andrew; Lal, Raj M.; Nagpure, Ajay Singh; Li, Yang; Yu, Huajun; Jiang, Daqian; Russell, Armistead G.; Shi, Lei; Chertow, Marian; Wang, Yangjun; Wang, Shuxiao
2017-10-01
Cities offer unique strategies to reduce fossil fuel use through the exchange of energy and materials across homes, businesses, infrastructure and industries co-located in urban areas. However, the large-scale impact of such strategies has not been quantified. Using new models and data sets representing 637 Chinese cities, we find that such cross-sectoral strategies--enabled by compact urban design and circular economy policies--contribute an additional 15%-36% to national CO2 mitigation, compared to conventional single-sector strategies. As a co-benefit, ~25,500 to ~57,500 deaths annually are avoided from air pollution reduction. The benefits are highly variable across cities, ranging from <1%-37% for CO2 emission reduction and <1%-47% for avoided premature deaths. These results, using multi-scale, multi-sector physical systems modelling, identify cities with high carbon and health co-benefit potential and show that urban-industrial symbiosis is a significant carbon mitigation strategy, achievable with a combination of existing and advanced technologies in diverse city types.
CO2 Emissions in an Oil Palm Plantation on Tropical Peat in Malaysia
NASA Astrophysics Data System (ADS)
Leclerc, M.; Zhang, G.; Jantan, N. M.; Harun, M. H.; Kamarudin, N.; Choo, Y. M.
2016-12-01
Tropical peats are large contributors to greenhouse gas emissions and differ markedly from their counterparts at temperate latitudes. The rapid deforestation and subsequent land conversion of tropical virgin forests in Southeast Asia have been decried by environmental groups worldwide even though there is currently little robust scientific evidence to ascertain the net amount of greenhouse gas released to the atmosphere. The conversion to oil palm plantation at a large scale further exacerbates the situation. This paper shows preliminary data on CO2 emissions in a converted oil palm plantation grown on tropical peat in northeast Malaysia.
Energy: the microfluidic frontier.
Sinton, David
2014-09-07
Global energy is largely a fluids problem. It is also large-scale, in stark contrast to microchannels. Microfluidic energy technologies must offer either massive scalability or direct relevance to energy processes already operating at scale. We have to pick our fights. Highlighted here are the exceptional opportunities I see, including some recent successes and areas where much more attention is needed. The most promising directions are those that leverage high surface-to-volume ratios, rapid diffusive transport, capacity for high temperature and high pressure experiments, and length scales characteristic of microbes and fluids (hydrocarbons, CO2) underground. The most immediate areas of application are where information is the product; either fluid sample analysis (e.g. oil analysis); or informing operations (e.g. CO2 transport in microporous media). I'll close with aspects that differentiate energy from traditional microfluidics applications, the uniquely important role of engineering in energy, and some thoughts for the research community forming at the nexus of lab-on-a-chip and energy--a microfluidic frontier.
Low-Power, Chip-Scale, Carbon Dioxide Gas Sensors for Spacesuit Monitoring
NASA Technical Reports Server (NTRS)
Rani, Asha; Shi, Chen; Thomson, Brian; Debnath, Ratan; Wen, Boamei; Motayed, Abhishek; Chullen, Cinda
2018-01-01
N5 Sensors, Inc. through a Small Business Technology Transfer (STTR) contract award has been developing ultra-small, low-power carbon dioxide (CO2) gas sensors, suited for monitoring CO2 levels inside NASA spacesuits. Due to the unique environmental conditions within the spacesuits, such as high humidity, large temperature swings, and operating pressure swings, measurement of key gases relevant to astronaut's safety and health such as(CO2), is quite challenging. Conventional non-dispersive infrared absorption based CO2 sensors present challenges inside the spacesuits due to size, weight, and power constraints, along with the ability to sense CO2 in a high humidity environment. Unique chip-scale, nanoengineered chemiresistive gas-sensing architecture has been developed for this application, which can be operated in a typical space-suite environmental conditions. Unique design combining the selective adsorption properties of the nanophotocatalytic clusters of metal-oxides and metals, provides selective detection of CO2 in high relative humidity conditions. All electronic design provides a compact and low-power solution, which can be implemented for multipoint detection of CO2 inside the spacesuits. This paper will describe the sensor architecture, development of new photocatalytic material for better sensor response, and advanced structure for better sensitivity and shorter response times.
NASA Astrophysics Data System (ADS)
Campanari, Stefano; Mastropasqua, Luca; Gazzani, Matteo; Chiesa, Paolo; Romano, Matteo C.
2016-09-01
An important advantage of solid oxide fuel cells (SOFC) as future systems for large scale power generation is the possibility of being efficiently integrated with processes for CO2 capture. Focusing on natural gas power generation, Part A of this work assessed the performances of advanced pressurised and atmospheric plant configurations (SOFC + GT and SOFC + ST, with fuel cell integration within a gas turbine or a steam turbine cycle) without CO2 separation. This Part B paper investigates such kind of power cycles when applied to CO2 capture, proposing two ultra-high efficiency plant configurations based on advanced intermediate-temperature SOFCs with internal reforming and low temperature CO2 separation process. The power plants are simulated at the 100 MW scale with a set of realistic assumptions about FC performances, main components and auxiliaries, and show the capability of exceeding 70% LHV efficiency with high CO2 capture (above 80%) and a low specific primary energy consumption for the CO2 avoided (1.1-2.4 MJ kg-1). Detailed results are presented in terms of energy and material balances, and a sensitivity analysis of plant performance is developed vs. FC voltage and fuel utilisation to investigate possible long-term improvements. Options for further improvement of the CO2 capture efficiency are also addressed.
The role of optimality in characterizing CO2 seepage from geological carbon sequestration sites
DOE Office of Scientific and Technical Information (OSTI.GOV)
Cortis, Andrea; Oldenburg, Curtis M.; Benson, Sally M.
Storage of large amounts of carbon dioxide (CO{sub 2}) in deep geological formations for greenhouse gas mitigation is gaining momentum and moving from its conceptual and testing stages towards widespread application. In this work we explore various optimization strategies for characterizing surface leakage (seepage) using near-surface measurement approaches such as accumulation chambers and eddy covariance towers. Seepage characterization objectives and limitations need to be defined carefully from the outset especially in light of large natural background variations that can mask seepage. The cost and sensitivity of seepage detection are related to four critical length scales pertaining to the size ofmore » the: (1) region that needs to be monitored; (2) footprint of the measurement approach, and (3) main seepage zone; and (4) region in which concentrations or fluxes are influenced by seepage. Seepage characterization objectives may include one or all of the tasks of detecting, locating, and quantifying seepage. Each of these tasks has its own optimal strategy. Detecting and locating seepage in a region in which there is no expected or preferred location for seepage nor existing evidence for seepage requires monitoring on a fixed grid, e.g., using eddy covariance towers. The fixed-grid approaches needed to detect seepage are expected to require large numbers of eddy covariance towers for large-scale geologic CO{sub 2} storage. Once seepage has been detected and roughly located, seepage zones and features can be optimally pinpointed through a dynamic search strategy, e.g., employing accumulation chambers and/or soil-gas sampling. Quantification of seepage rates can be done through measurements on a localized fixed grid once the seepage is pinpointed. Background measurements are essential for seepage detection in natural ecosystems. Artificial neural networks are considered as regression models useful for distinguishing natural system behavior from anomalous behavior suggestive of CO{sub 2} seepage without need for detailed understanding of natural system processes. Because of the local extrema in CO{sub 2} fluxes and concentrations in natural systems, simple steepest-descent algorithms are not effective and evolutionary computation algorithms are proposed as a paradigm for dynamic monitoring networks to pinpoint CO{sub 2} seepage areas.« less
NASA Astrophysics Data System (ADS)
Parker, Robert J.; Boesch, Hartmut; Wooster, Martin J.; Moore, David P.; Webb, Alex J.; Gaveau, David; Murdiyarso, Daniel
2016-08-01
The 2015-2016 strong El Niño event has had a dramatic impact on the amount of Indonesian biomass burning, with the El Niño-driven drought further desiccating the already-drier-than-normal landscapes that are the result of decades of peatland draining, widespread deforestation, anthropogenically driven forest degradation and previous large fire events. It is expected that the 2015-2016 Indonesian fires will have emitted globally significant quantities of greenhouse gases (GHGs) to the atmosphere, as did previous El Niño-driven fires in the region. The form which the carbon released from the combustion of the vegetation and peat soils takes has a strong bearing on its atmospheric chemistry and climatological impacts. Typically, burning in tropical forests and especially in peatlands is expected to involve a much higher proportion of smouldering combustion than the more flaming-characterised fires that occur in fine-fuel-dominated environments such as grasslands, consequently producing significantly more CH4 (and CO) per unit of fuel burned. However, currently there have been no aircraft campaigns sampling Indonesian fire plumes, and very few ground-based field campaigns (none during El Niño), so our understanding of the large-scale chemical composition of these extremely significant fire plumes is surprisingly poor compared to, for example, those of southern Africa or the Amazon.Here, for the first time, we use satellite observations of CH4 and CO2 from the Greenhouse gases Observing SATellite (GOSAT) made in large-scale plumes from the 2015 El Niño-driven Indonesian fires to probe aspects of their chemical composition. We demonstrate significant modifications in the concentration of these species in the regional atmosphere around Indonesia, due to the fire emissions.Using CO and fire radiative power (FRP) data from the Copernicus Atmosphere Service, we identify fire-affected GOSAT soundings and show that peaks in fire activity are followed by subsequent large increases in regional greenhouse gas concentrations. CH4 is particularly enhanced, due to the dominance of smouldering combustion in peatland fires, with CH4 total column values typically exceeding 35 ppb above those of background "clean air" soundings. By examining the CH4 and CO2 excess concentrations in the fire-affected GOSAT observations, we determine the CH4 to CO2 (CH4 / CO2) fire emission ratio for the entire 2-month period of the most extreme burning (September-October 2015), and also for individual shorter periods where the fire activity temporarily peaks. We demonstrate that the overall CH4 to CO2 emission ratio (ER) for fires occurring in Indonesia over this time is 6.2 ppb ppm-1. This is higher than that found over both the Amazon (5.1 ppb ppm-1) and southern Africa (4.4 ppb ppm-1), consistent with the Indonesian fires being characterised by an increased amount of smouldering combustion due to the large amount of organic soil (peat) burning involved. We find the range of our satellite-derived Indonesian ERs (6.18-13.6 ppb ppm-1) to be relatively closely matched to that of a series of close-to-source, ground-based sampling measurements made on Kalimantan at the height of the fire event (7.53-19.67 ppb ppm-1), although typically the satellite-derived quantities are slightly lower on average. This seems likely because our field sampling mostly intersected smaller-scale peat-burning plumes, whereas the large-scale plumes intersected by the GOSAT Thermal And Near infrared Sensor for carbon Observation - Fourier Transform Spectrometer (TANSO-FTS) footprints would very likely come from burning that was occurring in a mixture of fuels that included peat, tropical forest and already-cleared areas of forest characterised by more fire-prone vegetation types than the natural rainforest biome (e.g. post-fire areas of ferns and scrubland, along with agricultural vegetation).The ability to determine large-scale ERs from satellite data allows the combustion behaviour of very large regions of burning to be characterised and understood in a way not possible with ground-based studies, and which can be logistically difficult and very costly to consider using aircraft observations. We therefore believe the method demonstrated here provides a further important tool for characterising biomass burning emissions, and that the GHG ERs derived for the first time for these large-scale Indonesian fire plumes during an El Niño event point to more routinely assessing spatiotemporal variations in biomass burning ERs using future satellite missions. These will have more complete spatial sampling than GOSAT and will enable the contributions of these fires to the regional atmospheric chemistry and climate to be better understood.
Quantifying CO2 Emissions from Individual Power Plants using OCO-2 Observations
NASA Astrophysics Data System (ADS)
Nassar, R.; Hill, T. G.; McLinden, C. A.; Wunch, D.; Jones, D. B. A.; Crisp, D.
2017-12-01
In order to better manage anthropogenic CO2 emissions, improved methods of quantifying emissions are needed at all spatial scales from the national level down to the facility level. Although the Orbiting Carbon Observatory 2 (OCO-2) satellite was not designed for monitoring power plant emissions, we show that in select cases, CO2 observations from OCO-2 can be used to quantify daily CO2 emissions from individual mid- to large-sized coal power plants by fitting the data to plume model simulations. Emission estimates for US power plants are within 1-13% of reported daily emission values enabling application of the approach to international sites that lack detailed emission information. These results affirm that a constellation of future CO2 imaging satellites, optimized for point sources, could be used for the Monitoring, Reporting and Verification (MRV) of CO2 emissions from individual power plants to support the implementation of climate policies.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Doug Cathro
The Lake Charles CCS Project is a large-scale industrial carbon capture and sequestration (CCS) project which will demonstrate advanced technologies that capture and sequester carbon dioxide (CO{sub 2}) emissions from industrial sources into underground formations. Specifically the Lake Charles CCS Project will accelerate commercialization of large-scale CO{sub 2} storage from industrial sources by leveraging synergy between a proposed petroleum coke to chemicals plant (the LCC Gasification Project) and the largest integrated anthropogenic CO{sub 2} capture, transport, and monitored sequestration program in the U.S. Gulf Coast Region. The Lake Charles CCS Project will promote the expansion of EOR in Texas andmore » Louisiana and supply greater energy security by expanding domestic energy supplies. The capture, compression, pipeline, injection, and monitoring infrastructure will continue to sequester CO{sub 2} for many years after the completion of the term of the DOE agreement. The objectives of this project are expected to be fulfilled by working through two distinct phases. The overall objective of Phase 1 was to develop a fully definitive project basis for a competitive Renewal Application process to proceed into Phase 2 - Design, Construction and Operations. Phase 1 includes the studies attached hereto that will establish: the engineering design basis for the capture, compression and transportation of CO{sub 2} from the LCC Gasification Project, and the criteria and specifications for a monitoring, verification and accounting (MVA) plan at the Hastings oil field in Texas. The overall objective of Phase 2, provided a successful competitive down-selection, is to execute design, construction and operations of three capital projects: (1) the CO{sub 2} capture and compression equipment, (2) a Connector Pipeline from the LLC Gasification Project to the Green Pipeline owned by Denbury and an affiliate of Denbury, and (3) a comprehensive MVA system at the Hastings oil field.« less
The Chemical Route to a Carbon Dioxide Neutral World.
Martens, Johan A; Bogaerts, Annemie; De Kimpe, Norbert; Jacobs, Pierre A; Marin, Guy B; Rabaey, Korneel; Saeys, Mark; Verhelst, Sebastian
2017-03-22
Excessive CO 2 emissions in the atmosphere from anthropogenic activity can be divided into point sources and diffuse sources. The capture of CO 2 from flue gases of large industrial installations and its conversion into fuels and chemicals with fast catalytic processes seems technically possible. Some emerging technologies are already being demonstrated on an industrial scale. Others are still being tested on a laboratory or pilot scale. These emerging chemical technologies can be implemented in a time window ranging from 5 to 20 years. The massive amounts of energy needed for capturing processes and the conversion of CO 2 should come from low-carbon energy sources, such as tidal, geothermal, and nuclear energy, but also, mainly, from the sun. Synthetic methane gas that can be formed from CO 2 and hydrogen gas is an attractive renewable energy carrier with an existing distribution system. Methanol offers advantages as a liquid fuel and is also a building block for the chemical industry. CO 2 emissions from diffuse sources is a difficult problem to solve, particularly for CO 2 emissions from road, water, and air transport, but steady progress in the development of technology for capturing CO 2 from air is being made. It is impossible to ban carbon from the entire energy supply of mankind with the current technological knowledge, but a transition to a mixed carbon-hydrogen economy can reduce net CO 2 emissions and ultimately lead to a CO 2 -neutral world. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
NASA Astrophysics Data System (ADS)
Lischka, Silke; Bach, Lennart T.; Schulz, Kai-Georg; Riebesell, Ulf
2017-01-01
Community approaches to investigating ocean acidification (OA) effects suggest a high tolerance of micro- and mesozooplankton to carbonate chemistry changes expected to occur within this century. Plankton communities in the coastal areas of the Baltic Sea frequently experience pH variations partly exceeding projections for the near future both on a diurnal and seasonal basis. We conducted a large-scale mesocosm CO2 enrichment experiment ( ˜ 55 m3) enclosing the natural plankton community in Tvärminne-Storfjärden for 8 weeks during June-August 2012 and studied community and species-taxon response of ciliates and mesozooplankton to CO2 elevations expected for this century. In addition to the response to fCO2, we also considered temperature and chlorophyll a variations in our analyses. Shannon diversity of ciliates significantly decreased with fCO2 and temperature with a greater dominance of smaller species. The mixotrophic Myrionecta rubra seemed to indirectly and directly benefit from higher CO2 concentrations in the post-bloom phase through increased occurrence of picoeukaryotes (most likely Cryptophytes) and Dinophyta at higher CO2 levels. With respect to mesozooplankton, we did not detect significant effects for either total abundance or for Shannon diversity. The cladocera Bosmina sp. occurred at distinctly higher abundance for a short time period during the second half of the experiment in three of the CO2-enriched mesocosms except for the highest CO2 level. The ratio of Bosmina sp. with empty to embryo- or resting-egg-bearing brood chambers, however, was significantly affected by CO2, temperature, and chlorophyll a. An indirect CO2 effect via increased food availability (Cyanobacteria) stimulating Bosmina sp. reproduction cannot be ruled out. Although increased regenerated primary production diminishes trophic transfer in general, the presence of organisms able to graze on bacteria such as cladocerans may positively impact organic matter transfer to higher trophic levels. Thus, under increasing OA in cladoceran-dominated mesozooplankton communities, the importance of the microbial loop in the pelagic zone may be temporarily enhanced and carbon transfer to higher trophic levels may be stimulated.
Fabrication and performance of a double layered Mn-Co-Ni-O/Mn-Co-Ni-Cu-O thin film detector
NASA Astrophysics Data System (ADS)
Zhou, Wei; Yin, Yiming; Yao, Niangjuan; Jiang, Lin; Qu, Yue; Wu, Jing; Gao, Y. Q.; Huang, Jingguo; Huang, Zhiming
2018-01-01
A thermal sensitive infrared and THz detector was fabricated by a double layered Mn-Co-Ni-O/Mn-Co-Ni-Cu-O films. The Mn-Co-Ni-O material, as one type of transition metal oxides, has long been used as a candidate for thermal sensors or infrared detectors. The resistivity of a most important Mn-Co-Ni-O thin film, Mn1. 96Co0.96Ni0.48O4(MCN) , is about 200 Ω·cm at room temperature, which ranges about 2 orders larger than that of VOx detectors. Therefore, the thickness of a typical squared Mn-Co-Ni-O IR detector should be about 10 μm, which is too large for focal plane arrays applications. To reduce the resistivity of Mn-Co-Ni-O thin film, 1/6 of Co element was replaced by Cu. Meanwhile, a cover layer of MCN film was deposited onto the Mn-Co-Ni-Cu-O film to improve the long term stability. The detector fabricated by the double layered Mn-Co-Ni-O/Mn-Co-Ni-Cu-O films showed large response to blackbody and 170 GHz radiation. The NEP of the detector was estimated to be the order of 10-8 W/Hz0. 5. By applying thermal isolation structure and additional absorption materials, the detection performance can be largely improved by 1-2 orders according to numerical estimation. The double layered Mn-Co-Ni-O film detector shows great potentials in applications in large scale IR detection arrays, and broad-band imaging.
Koulikov, Serguei; Assonov, Sergey; Fajgelj, Ales; Tans, Pieter
2018-07-01
The manuscript explores some advantages and limitations of laser based optical spectroscopy, aimed at achieving robust, high-reproducibility 13 C 16 O 2 and 12 C 16 O 2 ratio determinations on the VPDB-CO 2 δ 13 C scale by measuring the absorbance of line pairs of 13 C 16 O 2 and 12 C 16 O 2 . In particular, the sensitivities of spectroscopic lines to both pressure (P) and temperature (T) are discussed. Based on the considerations and estimations presented, a level of reproducibility of the 13 C 16 O 2 / 12 C 16 O 2 ratio determinations may be achieved of about 10 -6 . Thus one may establish an optical spectroscopic measurement technique for robust, high-precision 13 C 16 O 2 and 12 C 16 O 2 ratio measurements aimed at very low uncertainty. (Notably, creating such an optical instrument and developing technical solutions is beyond the scope of this paper.) The total combined uncertainty will also include the uncertainty component(s) related to the accuracy of calibration on the VPDB-CO 2 δ 13 C scale. Addressing high-accuracy calibrations is presently not straightforward - absolute numerical values of 13 C/ 12 C for the VPDB-CO 2 scale are not well known. Traditional stable isotope mass-spectrometry uses calibrations vs CO 2 evolved from the primary carbonate reference materials; which can hardly be used for calibrating commercial optical stable isotope analysers. In contrast to mass-spectrometry, the major advantage of the laser-based spectrometric technique detailed in this paper is its high robustness. Therefore one can introduce a new spectrometric δ 13 C characterisation method which, being once well-calibrated on the VPDB-CO 2 scale, may not require any further (re-)calibrations. This can be used for characterisation of δ 13 C in CO 2 -in-air mixtures with high precision and also with high accuracy. If this technique can be realised with the estimated long-term reproducibility (order of 10 -6 ), it could potentially serve as a more convenient Optical Transfer Standard (OTS), characterising large amounts of CO 2 gas mixtures on the VPDB-CO 2 δ 13 C scale without having to compare to carbonate-evolved CO 2 . Furthermore, if the OTS method proves to be successful, it might be considered for re-defining the VPDB-CO 2 δ 13 C-scale as the ratio of selected CO 2 spectroscopic absorbance lines measured at pre-defined T & P conditions. The approach can also be expanded to δ 18 O characterisation (using 16 O 12 C 18 O and 16 O 12 C 16 O absorbance lines) of CO 2 gas mixtures and potentially to other isotope ratios of other gases. Copyright © 2018 Elsevier B.V. All rights reserved.
Interpretation of hydraulic tests performed at a carbonate rock site for CO2 storage
NASA Astrophysics Data System (ADS)
María Gómez Castro, Berta; Fernández López, Sheila; Carrera, Jesús; de Simone, Silvia; Martínez, Lurdes; Roetting, Tobias; Soler, Joaquim; Ortiz, Gema; de Dios, Carlos; Huber, Christophe
2014-05-01
Interpretation of hydraulic tests performed at a carbonate rock site for CO2 storage Berta Gómez, Sheila Fernández, Tobias Roetting, Lurdes Martínez, Silvia de Simone, Joaquim Soler, Jesus Carrera, Gema Ortiz, Christophe Huber, Carlos de Dios Proper design of CO2 geological storage facilities requires knowledge of the reservoir hydraulic parameters. Specifically, permeability controls the flux of CO2, the rate at which it dissolves, local and regional pressure buildup and the likelihood of induced seismicity. Permeability is obtained from hydraulic tests, which may yield local permeability, which controls injectivity, and large scale permeability, which controls pressure buildup at the large scale. If pressure response measurements are obtained at different elevations, hydraulic tests may also yield vertical permeability, which controls the rate at which CO2 dissolves. The objective of this work is to discuss the interpretation of hydraulic tests at deep reservoirs and the conditions under which these permeabilities can be obtained. To achieve this objective, we have built a radially symmetric model, including a skin and radial as well as vertical heterogeneity. We use this model to simulate hydraulic tests with increasing degrees of complexity about the medium response. We start by assuming Darcy flow, then add coupled mechanical effects (fractures opening) and, finally, we add thermal effects. We discuss how these affect the conventional interpretation of the tests and how to identify their presence. We apply these findings to the interpretation of hydraulic tests at Hontomin.
NASA Astrophysics Data System (ADS)
ul-Haq, Zia; Rana, Asim Daud; Ali, Muhammad; Mahmood, Khalid; Tariq, Salman; Qayyum, Zarmina
2015-08-01
This study presents major anthropogenic sources of carbon monoxide (CO) in Pakistan and discusses the spatio-temporal variability of tropospheric CO over Pakistan and neighboring regions of Afghanistan, India and Iran for a period from 2003 to 2012 using satellite-sensed (AIRS/AMSU) data. The results show a large spatio-temporal variability of CO over the study region mostly associated with anthropogenic activities such as crop residue burning, vehicular transport, and electricity and energy generation, and local meteorology. The annual mean value of tropospheric CO is observed to be 115 ± 2 ppbv that remains almost steady during the study period with decadal increase of only 2%. Due to more anthropogenic emissions of CO and its transport, the eastern zone shows a higher average value of 122 ± 2 ppbv with 2.7% decadal increase than the western zone (111 ± 3 ppbv with 1.4% decadal increase). Elevated concentrations of CO have been observed over the Indo-Gangetic Basin, Lahore, Karachi, and Delhi. During the study period large fluctuations in CO mean monthly values are found ranging from 99 ppbv to 131 ppbv. The fact that, in spite of a large increase in the CO emissions from 2003 to 2012, its average concentration remains almost stable indicates that a large scale regional transport contributes substantially to the tropospheric CO. Carbon monoxide concentrations exhibit a strong seasonal pattern with maximum amplitude in spring and minimum in autumn. July is found to have the highest decadal increasing trend of 13% followed by August at 8%, whereas May has the highest decreasing trend of -8% followed by November at -4.4%.
Carbon dioxide supersaturation in the surface waters of lakes
DOE Office of Scientific and Technical Information (OSTI.GOV)
Cole, J.J.; Caraco, N.F.; Kling, G.W.
1994-09-09
Data on the partial pressure of carbon dioxide (CO{sub 2}) in the surface waters from a large number of lakes (1835) with a worldwide distribution show that only a small proportion of the 4665 samples analyzed (less than 10 percent) were within {+-}20 percent of equilibrium with the atmosphere and that most samples (87 percent) were supersaturated. The mean partial pressure of CO{sub 2} averaged 1036 microatmospheres, about three times the value in the overlying atmosphere, indicating that lakes are sources rather than sinks of atmospheric CO{sub 2}. On a global scale, the potential efflux of CO{sub 2} from lakesmore » (about 0.14 x 10{sup 15} grams of carbon per year) is about half as large as riverine transport of organic plus inorganic carbon to the ocean. Lakes are a small but potentially important conduit for carbon for terrestrial sources to the atmospheric sink. 18 refs., 2 figs., 1 tab.« less
NASA Astrophysics Data System (ADS)
Niezgodzki, Igor; Knorr, Gregor; Lohmann, Gerrit; Tyszka, Jarosław; Markwick, Paul J.
2017-09-01
We investigate the impact of different CO2 levels and different subarctic gateway configurations on the surface temperatures during the latest Cretaceous using the Earth System Model COSMOS. The simulated temperatures are compared with the surface temperature reconstructions based on a recent compilation of the latest Cretaceous proxies. In our numerical experiments, the CO2 level ranges from 1 to 6 times the preindustrial (PI) CO2 level of 280 ppm. On a global scale, the most reasonable match between modeling and proxy data is obtained for the experiments with 3 to 5 × PI CO2 concentrations. However, the simulated low- (high-) latitude temperatures are too high (low) as compared to the proxy data. The moderate CO2 levels scenarios might be more realistic, if we take into account proxy data and the dead zone effect criterion. Furthermore, we test if the model-data discrepancies can be caused by too simplistic proxy-data interpretations. This is distinctly seen at high latitudes, where most proxies are biased toward summer temperatures. Additional sensitivity experiments with different ocean gateway configurations and constant CO2 level indicate only minor surface temperatures changes (< 1°C) on a global scale, with higher values (up to 8°C) on a regional scale. These findings imply that modeled and reconstructed temperature gradients are to a large degree only qualitatively comparable, providing challenges for the interpretation of proxy data and/or model sensitivity. With respect to the latter, our results suggest that an assessment of greenhouse worlds is best constrained by temperatures in the midlatitudes.
Watershed-Scale Heterogeneity of the Biophysical Controls on Soil Respiration
NASA Astrophysics Data System (ADS)
Riveros, D. A.; Pacific, V. J.; McGlynn, B. L.; Welsch, D. L.; Epstein, H. E.; Muth, D. J.; Marshall, L.; Wraith, J.
2006-12-01
Large gaps exist in our understanding of the variability of soil respiration response to changing hydrologic conditions across spatial and temporal scales. Determining the linkages between the hydrologic cycle and the biophysical controls of soil respiration from the local point, to the plot, to the watershed scale is critical to understanding the dynamics of net ecosystem CO2 exchange (NEE). To study the biophysical controls of soil respiration, we measured soil CO2 concentration, soil CO2 flux, dissolved CO2 in stream water, soil moisture, soil temperature, groundwater dynamics, and precipitation at 20-minute intervals throughout the growing season at 4 sites and at weekly intervals at 62 sites covering the range of topographic position, slope, aspect, land cover, and upslope accumulated area conditions in a 555-ha subalpine watershed in central Montana. Our goal was to quantify watershed-scale heterogeneity in soil CO2 concentrations and surface efflux and gain understanding of the biophysical controls on soil respiration. We seek to improve our ability to evaluate and predict soil respiration responses to a dynamic hydrologic cycle across multiple temporal and spatial scales. We found that time lags between biophysical controls and soil respiration can occur from hourly to daily scales. The sensitivity of soil respiration to changes in environmental conditions is controlled by the antecedent soil moisture and by topographic position. At the watershed scale, significant differences in soil respiration exist between upland (dry) and lowland (wet) sites. However, differences in the magnitude and timing of soil respiration also exist within upland settings due to heterogeneity in soil temperature, soil moisture, and soil organic matter. Finally, we used a process-based model to simulate respiration at different times of the year across spatial locations. Our simulations highlight the importance of autotrophic and heterotrophic respiration (production) over diffusivity and soil physical properties (transport). Our work begins to address the disconnect between point, footprint, watershed scale estimates of ecosystem respiration and the role of a dynamic hydrologic cycle.
The influence of large-scale wind power on global climate.
Keith, David W; Decarolis, Joseph F; Denkenberger, David C; Lenschow, Donald H; Malyshev, Sergey L; Pacala, Stephen; Rasch, Philip J
2004-11-16
Large-scale use of wind power can alter local and global climate by extracting kinetic energy and altering turbulent transport in the atmospheric boundary layer. We report climate-model simulations that address the possible climatic impacts of wind power at regional to global scales by using two general circulation models and several parameterizations of the interaction of wind turbines with the boundary layer. We find that very large amounts of wind power can produce nonnegligible climatic change at continental scales. Although large-scale effects are observed, wind power has a negligible effect on global-mean surface temperature, and it would deliver enormous global benefits by reducing emissions of CO(2) and air pollutants. Our results may enable a comparison between the climate impacts due to wind power and the reduction in climatic impacts achieved by the substitution of wind for fossil fuels.
Projected land photosynthesis constrained by changes in the seasonal cycle of atmospheric CO2.
Wenzel, Sabrina; Cox, Peter M; Eyring, Veronika; Friedlingstein, Pierre
2016-10-27
Uncertainties in the response of vegetation to rising atmospheric CO 2 concentrations contribute to the large spread in projections of future climate change. Climate-carbon cycle models generally agree that elevated atmospheric CO 2 concentrations will enhance terrestrial gross primary productivity (GPP). However, the magnitude of this CO 2 fertilization effect varies from a 20 per cent to a 60 per cent increase in GPP for a doubling of atmospheric CO 2 concentrations in model studies. Here we demonstrate emergent constraints on large-scale CO 2 fertilization using observed changes in the amplitude of the atmospheric CO 2 seasonal cycle that are thought to be the result of increasing terrestrial GPP. Our comparison of atmospheric CO 2 measurements from Point Barrow in Alaska and Cape Kumukahi in Hawaii with historical simulations of the latest climate-carbon cycle models demonstrates that the increase in the amplitude of the CO 2 seasonal cycle at both measurement sites is consistent with increasing annual mean GPP, driven in part by climate warming, but with differences in CO 2 fertilization controlling the spread among the model trends. As a result, the relationship between the amplitude of the CO 2 seasonal cycle and the magnitude of CO 2 fertilization of GPP is almost linear across the entire ensemble of models. When combined with the observed trends in the seasonal CO 2 amplitude, these relationships lead to consistent emergent constraints on the CO 2 fertilization of GPP. Overall, we estimate a GPP increase of 37 ± 9 per cent for high-latitude ecosystems and 32 ± 9 per cent for extratropical ecosystems under a doubling of atmospheric CO 2 concentrations on the basis of the Point Barrow and Cape Kumukahi records, respectively.
Lidar Measurements of Atmospheric CO2 From Regional to Global Scales
NASA Technical Reports Server (NTRS)
Lin, Bing; Harrison, F. Wallace; Nehrir, Amin; Browell, Edward; Dobler, Jeremy; Campbell, Joel; Meadows, Byron; Obland, Michael; Ismail, Syed; Kooi, Susan;
2015-01-01
Atmospheric CO2 is a critical forcing for the Earth's climate and the knowledge on its distributions and variations influences predictions of the Earth's future climate. Large uncertainties in the predictions persist due to limited observations. This study uses the airborne Intensity-Modulated Continuous-Wave (IMCW) lidar developed at NASA Langley Research Center to measure regional atmospheric CO2 spatio-temporal variations. Further lidar development and demonstration will provide the capability of global atmospheric CO2 estimations from space, which will significantly advances our knowledge on atmospheric CO2 and reduce the uncertainties in the predictions of future climate. In this presentation, atmospheric CO2 column measurements from airborne flight campaigns and lidar system simulations for space missions will be discussed. A measurement precision of approx.0.3 ppmv for a 10-s average over desert and vegetated surfaces has been achieved. Data analysis also shows that airborne lidar CO2 column measurements over these surfaces agree well with in-situ measurements. Even when thin cirrus clouds present, consistent CO2 column measurements between clear and thin cirrus cloudy skies are obtained. Airborne flight campaigns have demonstrated that precise atmospheric column CO2 values can be measured from current IM-CW lidar systems, which will lead to use this airborne technique in monitoring CO2 sinks and sources in regional and continental scales as proposed by the NASA Atmospheric Carbon and Transport â€" America project. Furthermore, analyses of space CO2 measurements shows that applying the current IM-CW lidar technology and approach to space, the CO2 science goals of space missions will be achieved, and uncertainties in CO2 distributions and variations will be reduced.
McEwen, Sara; Polatajko, Helene; Baum, Carolyn; Rios, Jorge; Cirone, Dianne; Doherty, Meghan; Wolf, Timothy
2014-01-01
Purpose The purpose of this study was to estimate the effect of the Cognitive Orientation to daily Occupational Performance (CO-OP) approach compared to usual outpatient rehabilitation on activity and participation in people less than 3 months post stroke. Methods An exploratory, single blind, randomized controlled trial with a usual care control arm was conducted. Participants referred to 2 stroke rehabilitation outpatient programs were randomized to receive either Usual Care or CO-OP. The primary outcome was actual performance of trained and untrained self-selected activities, measured using the Performance Quality Rating Scale (PQRS). Additional outcomes included the Canadian Occupational Performance Measure (COPM), the Stroke Impact Scale Participation Domain, the Community Participation Index, and the Self Efficacy Gauge. Results Thirty-five (35) eligible participants were randomized; 26 completed the intervention. Post-intervention, PQRS change scores demonstrated CO-OP had a medium effect over Usual Care on trained self-selected activities (d=0.5) and a large effect on untrained (d=1.2). At a 3 month follow-up, PQRS change scores indicated a large effect of CO-OP on both trained (d=1.6) and untrained activities (d=1.1). CO-OP had a small effect on COPM and a medium effect on the Community Participation Index perceived control and the Self-Efficacy Gauge. Conclusion CO-OP was associated with a large treatment effect on follow up performances of self-selected activities, and demonstrated transfer to untrained activities. A larger trial is warranted. PMID:25416738
McEwen, Sara; Polatajko, Helene; Baum, Carolyn; Rios, Jorge; Cirone, Dianne; Doherty, Meghan; Wolf, Timothy
2015-07-01
The purpose of this study was to estimate the effect of the Cognitive Orientation to daily Occupational Performance (CO-OP) approach compared with usual outpatient rehabilitation on activity and participation in people <3 months poststroke. An exploratory, single-blind, randomized controlled trial, with a usual-care control arm, was conducted. Participants referred to 2 stroke rehabilitation outpatient programs were randomized to receive either usual care or CO-OP. The primary outcome was actual performance of trained and untrained self-selected activities, measured using the Performance Quality Rating Scale (PQRS). Additional outcomes included the Canadian Occupational Performance Measure (COPM), the Stroke Impact Scale Participation Domain, the Community Participation Index, and the Self-Efficacy Gauge. A total of 35 eligible participants were randomized; 26 completed the intervention. Post intervention, PQRS change scores demonstrated that CO-OP had a medium effect over usual care on trained self-selected activities (d = 0.5) and a large effect on untrained activities (d = 1.2). At a 3-month follow-up, PQRS change scores indicated a large effect of CO-OP on both trained (d = 1.6) and untrained activities (d = 1.1). CO-OP had a small effect on COPM and a medium effect on the Community Participation Index perceived control and on the Self-Efficacy Gauge. CO-OP was associated with a large treatment effect on follow-up performances of self-selected activities and demonstrated transfer to untrained activities. A larger trial is warranted. © The Author(s) 2014.
NASA Astrophysics Data System (ADS)
Goodman, H.
2017-12-01
This investigation seeks to develop sealant technology that can restore containment to completed wells that suffer CO2 gas leakages currently untreatable using conventional technologies. Experimentation is performed at the Mont Terri Underground Research Laboratory (MT-URL) located in NW Switzerland. The laboratory affords investigators an intermediate-scale test site that bridges the gap between the laboratory bench and full field-scale conditions. Project focus is the development of CO2 leakage remediation capability using sealant technology. The experimental concept includes design and installation of a field scale completion package designed to mimic well systems heating-cooling conditions that may result in the development of micro-annuli detachments between the casing-cement-formation boundaries (Figure 1). Of particular interest is to test novel sealants that can be injected in to relatively narrow micro-annuli flow-paths of less than 120 microns aperture. Per a special report on CO2 storage submitted to the IPCC[1], active injection wells, along with inactive wells that have been abandoned, are identified as one of the most probable sources of leakage pathways for CO2 escape to the surface. Origins of pressure leakage common to injection well and completions architecture often occur due to tensile cracking from temperature cycles, micro-annulus by casing contraction (differential casing to cement sheath movement) and cement sheath channel development. This discussion summarizes the experiment capability and sealant testing results. The experiment concludes with overcoring of the entire mock-completion test site to assess sealant performance in 2018. [1] IPCC Special Report on Carbon Dioxide Capture and Storage (September 2005), section 5.7.2 Processes and pathways for release of CO2 from geological storage sites, page 244
NASA Astrophysics Data System (ADS)
Will, R. A.; Balch, R. S.
2015-12-01
The Southwest Partnership on Carbon Sequestration is performing seismic based characterization and monitoring activities at an active CO2 EOR project at Farnsworth Field, Texas. CO2 is anthropogenically sourced from a fertilizer and an ethanol plant. The field has 13 CO2 injectors and has sequestered 302,982 metric tonnes of CO2 since October 2013. The field site provides an excellent laboratory for testing a range of monitoring technologies in an operating CO2 flood since planned development is sequential and allows for multiple opportunities to record zero CO2 baseline data, mid-flood data, and fully flooded data. The project is comparing and contrasting several scales of seismic technologies in order to determine best practices for large scale commercial sequestration projects. Characterization efforts include an 85 km2 3D surface seismic survey, baseline and repeat 3D VSP surveys centered on injection wells, cross-well tomography baseline and repeat surveys between injector/producer pairs, and a borehole passive seismic array to monitor induced seismicity. All surveys have contributed to detailed geologic models which were then used for fluid flow and risk assessment simulations. 3D VSP and cross-well data with repeat surveys have allowed for direct comparisons of the reservoir prior to CO2 injection and at eight months into injection, with a goal of imaging the CO2 plume as it moves away from injection wells. Additional repeat surveys at regular intervals will continue to refine the plume. The goal of this work is to demonstrate seismic based technologies to monitor CO2 sequestration projects, and to contribute to best practices manuals for commercial scale CO2 sequestration projects. In this talk the seismic plan will be outlined, progress towards goals enumerated, and preliminary results from baseline and repeat seismic data will be discussed. Funding for this project is provided by the U.S. Department of Energy under Award No. DE-FC26-05NT42591.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bowers, Geoffrey M.; Schaef, H. Todd; Loring, John S.
This paper explores the molecular-scale interactions between CO 2 and the representative smectite mineral hectorite under supercritical conditions (90 bar, 50°C) using novel in situ X-ray diffraction (XRD), infrared (IR) spectroscopy, and magic angle spinning (MAS) nuclear magnetic resonance (NMR) techniques. Particular emphasis is placed on understanding the roles of the smectite charge balancing cation (CBC) and H O in these interactions. The data show that supercritical CO 2 (scCO 2) can be adsorbed on external surfaces and in the confined interlayer spaces of hectorite at 50°C and 90 bar, with the uptake of CO 2 into the interlayer favoredmore » at low H 2O content and when the basal spacing is similar to a monolayer hydrate of hectorite (1WL, ~12.5 Å). These results are in agreement with published spectroscopic and molecular modeling data for the related smectite Na-montmorillonite.Charge balancing cations with small radii, large hydration energies, and low polarizabilities tend to scavenge H 2O from humid scCO 2 or retain the H 2O they held before scCO 2 exposure, swelling spontaneously to a bilayer hydrate (2WL) dominated state that largely prevents CO 2-ion interactions and influences the extent of CO 2 intercalation into the interlayer. In contrast, ions with large radii, low hydration energies, and large polarizabilities more readily form close associations with CO 2 with the energetics enabling coexistence of CO 2 and H2O in the interlayer over a wide range of scCO 2 humidities. Integrating our results with those from molecular dynamics simulations of wet CO 2-bearing montmorillonites suggest that adsorbed CO 2 in 1WL-type interlayers is oriented with its long axis parallel to the clay sheets and experiences dynamics dominated by anisotropic rotation about the axis perpendicular to the CO 2 long axis at rates of at least ~105 Hz. If appreciable CO 2 is adsorbed in 2WL-type interlayers, it must experience a mean orientation and dynamic averaging affects that mimic the 1WL-type adsorption environment. External surface adsorbed CO 2 is dynamically similar to the 1WL case, but the CO 2 long axis samples a larger range of orientations with respect to the smectite surface and adopts a different mean angle between the long axis and the smectite surface. Our data also suggest that equilibrating hectorite with a largevolume of scCO 2 at 50°C and 90 bar leads to interlayer dehydration, with the extent of dehydration correlating with the hydrophilicity of the CBC.« less
USDA-ARS?s Scientific Manuscript database
In nearly all large-scale models, CO2 efflux from soil (i.e., soil respiration) is represented as a function of soil temperature. However, the relationship between soil respiration and soil temperature is highly variable at the local scale, and there is often a pronounced hysteresis in the soil resp...
Interferometric Mapping of Perseus Outflows with MASSES
NASA Astrophysics Data System (ADS)
Stephens, Ian; Dunham, Michael; Myers, Philip C.; MASSES Team
2017-01-01
The MASSES (Mass Assembly of Stellar Systems and their Evolution with the SMA) survey, a Submillimeter Array (SMA) large-scale program, is mapping molecular lines and continuum emission about the 75 known Class 0/I sources in the Perseus Molecular Cloud. In this talk, I present some of the key results of this project, with a focus on the CO(2-1) maps of the molecular outflows. In particular, I investigate how protostars inherit their rotation axes from large-scale magnetic fields and filamentary structure.
Cao, Jing; Fu, Wuyou; Yang, Haibin; Yu, Qingjiang; Zhang, Yanyan; Liu, Shikai; Sun, Peng; Zhou, Xiaoming; Leng, Yan; Wang, Shuangming; Liu, Bingbing; Zou, Guangtian
2009-04-09
Actinomorphic tubular ZnO/CoFe(2)O(4) nanocomposites were fabricated in large scale via a simple solution method at low temperature. The phase structures, morphologies, particle size, shell thickness, chemical compositions of the composites have been characterized by X-ray diffraction (XRD), field emission scanning electron microscope (FESEM), energy dispersive X-ray spectroscopy (EDS), and transmission electron microscopy (TEM). The as-synthesized nanocomposites were uniformly dispersed into the phenolic resin then the mixture was pasted on metal plate with the area of 200 mm x 200 mm as the microwave absorption test plate. The test of microwave absorption was carried out by the radar-absorbing materials (RAM) reflectivity far field radar cross-section (RCS) method. The range of microwave absorption is from 2 to 18 Hz and the best microwave absorption reach to 28.2 dB at 8.5 Hz. The results indicate that the composites are of excellence with respect to microwave absorption.
NASA Astrophysics Data System (ADS)
Dieudonné, E.; Gibert, F.; Xueref-remy, I. C.; Lopez, M.; Schmidt, M.; Ravetta, F.
2012-12-01
The development of anthropogenic activities since the pre-industrial era has greatly increased CO2 concentrations in the atmosphere, very likely causing the observed rise in global temperature. Therefore, accurate estimations of CO2 emission fluxes are very important for climate predictions. At the continental scale, CO2 fluxes can be estimated rather precisely using inverse modeling while tower turbulent flux measurements (eddy-covariance or EC) can provide an estimation of local-scale fluxes. However, this method cannot be applied to monitor urban CO2 emissions due to their large horizontal variability, so that a regional scale approach seems more suited. Unfortunately, at this scale, anthropogenic and biospheric fluxes are mixed, diluted and advected in the atmospheric boundary-layer (ABL) and the balance between these processes is not well known. Yet, independent estimations of CO2 fluxes would be needed to verify existing high resolution emission inventories and assess the efficiency of future mitigation policies. Several experiments dedicated to quantifying CO2 emissions from megacities are ongoing, like the CO2-MEGAPARIS research project [a,b]. In this framework, a network of lidars and in-situ sensors has been set up in Paris region. An original ABL mass budget method is used to infer the properties of advected anthropogenic CO2 and CO emissions from Paris urban area [c]. The method is applied in the center of Paris, at neighboring suburban sites located 20 km away, and at a rural station (100 km downwind). The budget uses ABL depths from elastic lidars, CO2 and CO concentrations from both the ICOS [d] and CO2-MEGAPARIS networks to quantify vertical advection and storage terms in the ABL mass budget. EC measurements are used to monitor biospheric surface fluxes. The budget in Paris provides a direct estimation of the average CO2 and CO fluxes from the city, while the budget at the suburban and rural stations provides an estimation of the advected fluxes. These anthropogenic fluxes are compared to the CITEPA and IER emission inventories using the air mass footprint from a Lagrangian Particle Dispersion Model in backward mode. Results from a case study in March 2012 are presented to assess the propagation of Paris CO2 and CO plume, the precision of the method and its ability to provide an independent verification of urban emission inventories. References: [a] Xueref-Remy et al., Abstract n°A13F-0277, AGU Fall Meeting 2010, San Francisco, USA [b] http://co2-megaparis.lsce.ipsl.fr/ [c] Gibert et al., J. Geophys. Research, 112, D10301 (2007) [d] http://www.icos-infrastructure.eu/
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.
An imperative need for global change research in tropical forests.
Zhou, Xuhui; Fu, Yuling; Zhou, Lingyan; Li, Bo; Luo, Yiqi
2013-09-01
Tropical forests play a crucial role in regulating regional and global climate dynamics, and model projections suggest that rapid climate change may result in forest dieback or savannization. However, these predictions are largely based on results from leaf-level studies. How tropical forests respond and feedback to climate change is largely unknown at the ecosystem level. Several complementary approaches have been used to evaluate the effects of climate change on tropical forests, but the results are conflicting, largely due to confounding effects of multiple factors. Although altered precipitation and nitrogen deposition experiments have been conducted in tropical forests, large-scale warming and elevated carbon dioxide (CO2) manipulations are completely lacking, leaving many hypotheses and model predictions untested. Ecosystem-scale experiments to manipulate temperature and CO2 concentration individually or in combination are thus urgently needed to examine their main and interactive effects on tropical forests. Such experiments will provide indispensable data and help gain essential knowledge on biogeochemical, hydrological and biophysical responses and feedbacks of tropical forests to climate change. These datasets can also inform regional and global models for predicting future states of tropical forests and climate systems. The success of such large-scale experiments in natural tropical forests will require an international framework to coordinate collaboration so as to meet the challenges in cost, technological infrastructure and scientific endeavor.
Deployment, Design, and Commercialization of Carbon-Negative Energy Systems
NASA Astrophysics Data System (ADS)
Sanchez, Daniel Lucio
Climate change mitigation requires gigaton-scale carbon dioxide removal technologies, yet few examples exist beyond niche markets. This dissertation informs large-scale implementation of bioenergy with carbon capture and sequestration (BECCS), a carbon-negative energy technology. It builds on existing literature with a novel focus on deployment, design, commercialization, and communication of BECCS. BECCS, combined with aggressive renewable deployment and fossil emission reductions, can enable a carbon-negative power system in Western North America by 2050, with up to 145% emissions reduction from 1990 levels. BECCS complements other sources of renewable energy, and can be deployed in a manner consistent with regional policies and design considerations. The amount of biomass resource available limits the level of fossil CO2 emissions that can still satisfy carbon emissions caps. Offsets produced by BECCS are more valuable to the power system than the electricity it provides. Implied costs of carbon for BECCS are relatively low ( 75/ton CO2 at scale) for a capital-intensive technology. Optimal scales for BECCS are an order of magnitude larger than proposed scales found in existing literature. Deviations from optimal scaled size have little effect on overall systems costs - suggesting that other factors, including regulatory, political, or logistical considerations, may ultimately have a greater influence on plant size than the techno-economic factors considered. The flexibility of thermochemical conversion enables a viable transition pathway for firms, utilities and governments to achieve net-negative CO 2 emissions in production of electricity and fuels given increasingly stringent climate policy. Primary research, development (R&D), and deployment needs are in large-scale biomass logistics, gasification, gas cleaning, and geological CO2 storage. R&D programs, subsidies, and policy that recognize co-conversion processes can support this pathway to commercialization. Here, firms can embrace a gradual transition pathway to deep decarbonization, limiting economic dislocation and increasing transfer of knowledge between the fossil and renewable sectors. Global cumulative capital investment needs for BECCS through 2050 are over 1.9 trillion (2015$, 4% real interest rate) for scenarios likely to limit global warming to 2 °C. This scenario envisions deployment of as much as 24 GW/yr of BECCS by 2040 in the electricity sector. To achieve theses rates of deployment within 15-20 years, governments and firms must commit to research, development, and deployment on an unprecedented scale. Three primary issues complicate emissions accounting for BECCS: cross-sector CO2 accounting, regrowth, and timing. Switchgrass integration decreases lifecycle greenhouse gas impacts of co-conversion systems with CCS, across a wide range of land-use change scenarios. Risks at commercial scale include adverse effects on food security, land conservation, social equity, and biodiversity, as well as competition for water resources. This dissertation argues for an iterative risk management approach to BECCS sustainability, with standards being updated as more knowledge is gained through deployment. Sustainability impacts and public opposition to BECCS may be reduced with transparent measurement and communication. Commercial-scale deployment is dependent on the coordination of a wide range of actors, many with different incentives and worldviews. Despite this problem, this dissertation challenges governments, industry incumbents, and emerging players to research, support, and deploy BECCS.
Resolving the Nuclear Obscuring Disk in the Compton-thick Seyfert Galaxy NGC 5643 with ALMA
NASA Astrophysics Data System (ADS)
Alonso-Herrero, A.; Pereira-Santaella, M.; García-Burillo, S.; Davies, R. I.; Combes, F.; Asmus, D.; Bunker, A.; Díaz-Santos, T.; Gandhi, P.; González-Martín, O.; Hernán-Caballero, A.; Hicks, E.; Hönig, S.; Labiano, A.; Levenson, N. A.; Packham, C.; Ramos Almeida, C.; Ricci, C.; Rigopoulou, D.; Rosario, D.; Sani, E.; Ward, M. J.
2018-06-01
We present ALMA Band 6 12CO(2–1) line and rest-frame 232 GHz continuum observations of the nearby Compton-thick Seyfert galaxy NGC 5643 with angular resolutions 0.″11–0.″26 (9–21 pc). The CO(2–1) integrated line map reveals emission from the nuclear and circumnuclear region with a two-arm nuclear spiral extending ∼10″ on each side. The circumnuclear CO(2–1) kinematics can be fitted with a rotating disk, although there are regions with large residual velocities and/or velocity dispersions. The CO(2–1) line profiles of these regions show two different velocity components. One is ascribed to the circular component and the other to the interaction of the AGN outflow, as traced by the [O III]λ5007 Å emission, with molecular gas in the disk a few hundred parsecs from the AGN. On nuclear scales, we detected an inclined CO(2–1) disk (diameter 26 pc, FWHM) oriented almost in a north–south direction. The CO(2–1) nuclear kinematics can be fitted with a rotating disk that appears to be tilted with respect to the large-scale disk. There are strong non-circular motions in the central 0.″2–0.″3 with velocities of up to 110 km s‑1. In the absence of a nuclear bar, these motions could be explained as radial outflows in the nuclear disk. We estimate a total molecular gas mass for the nuclear disk of M(H2) = 1.1 × 107 M ⊙ and an H2 column density toward the location of the AGN of N(H2) ∼ 5 × 1023 cm‑2, for a standard CO-to-H2 conversion factor. We interpret this nuclear molecular gas disk as the obscuring torus of NGC 5643 as well as the collimating structure of the ionization cone.
Influence of the biosphere and circulation on atmospheric CO2
NASA Astrophysics Data System (ADS)
Corbett, A.; Jiang, X.; La, J.; Olsen, E. T.; Licata, S. J.; Yung, Y. L.
2017-12-01
Using multiple satellite CO2 retrievals (e.g., AIRS, GOSAT, and OCO-2), we have investigated seasonal changes of CO2 as a function of latitudes and altitudes. The annual cycle of atmospheric CO2 is closely related to the exchange of CO2 between the biosphere and the atmosphere, so we also examine solar-induced fluorescence (SIF). High SIF value means more CO2 uptake by photosynthesis, which will lead to lower atmospheric CO2 concentrations. The satellite data demonstrate a negative correlation between atmospheric CO2 and SIF. SIF can be influenced by precipitation and evaporation. We have found a positive correlation between SIF and the difference of precipitation and evaporation, suggesting there is more CO2 uptake by vegetation when more water is available. In addition to the annual cycle, large-scale circulation, such as South Atlantic Walker Circulation, can also modulate atmospheric CO2 concentrations. As seen from AIRS, GOSAT, and OCO-2 CO2 retrievals, there is less CO2 over the South Atlantic Ocean than over South America from December to March. Results in this study will help us better understand interactions between the biosphere, circulation, and atmospheric CO2.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Zhao, Xianhui; Walker, Devin; Maiti, Debtanu
Cylindrical NiMg/Ce 0.6Zr 0.4O 2 pellet catalysts with two different sizes (large: radius = 1.59 mm; and small: radius = 0.75 mm) were produced by extrusion of powder catalysts. The small catalyst pellets had a higher specific surface area, pore volume, average pore size, radial crush strength, and resistance to breakage than the large ones. Tri-reforming tests with surrogate biogas were conducted at 3 bar and 882 °C, with the feed molar ratios of CH 4: CO 2: air fixed at 1.0: 0.7: 0.95 and the H 2O/CH 4 molar feed ratio (0.35 – 1.16) varied. The small catalyst pelletsmore » exhibited lower internal mass transfer resistance and higher coking resistance, compared to the large ones. CO 2 conversion decreased and H 2/CO molar ratio increased with the increase of H 2O/CH 4 molar feed ratio, which are consistent with the trends predicted by thermodynamic equilibrium calculations. Finally, the results indicate that the NiMg/Ce 0.6Zr 0.4O 2 catalyst pellets are promising for commercial scale applications.« less
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.
International law poses problems for negative emissions research
NASA Astrophysics Data System (ADS)
Brent, Kerryn; McGee, Jeffrey; McDonald, Jan; Rohling, Eelco J.
2018-06-01
New international governance arrangements that manage environmental risk and potential conflicts of interests are needed to facilitate negative emissions research that is essential to achieving the large-scale CO2 removal implied by the Paris Agreement targets.
Efficient parallel simulation of CO2 geologic sequestration insaline aquifers
DOE Office of Scientific and Technical Information (OSTI.GOV)
Zhang, Keni; Doughty, Christine; Wu, Yu-Shu
2007-01-01
An efficient parallel simulator for large-scale, long-termCO2 geologic sequestration in saline aquifers has been developed. Theparallel simulator is a three-dimensional, fully implicit model thatsolves large, sparse linear systems arising from discretization of thepartial differential equations for mass and energy balance in porous andfractured media. The simulator is based on the ECO2N module of the TOUGH2code and inherits all the process capabilities of the single-CPU TOUGH2code, including a comprehensive description of the thermodynamics andthermophysical properties of H2O-NaCl- CO2 mixtures, modeling singleand/or two-phase isothermal or non-isothermal flow processes, two-phasemixtures, fluid phases appearing or disappearing, as well as saltprecipitation or dissolution. The newmore » parallel simulator uses MPI forparallel implementation, the METIS software package for simulation domainpartitioning, and the iterative parallel linear solver package Aztec forsolving linear equations by multiple processors. In addition, theparallel simulator has been implemented with an efficient communicationscheme. Test examples show that a linear or super-linear speedup can beobtained on Linux clusters as well as on supercomputers. Because of thesignificant improvement in both simulation time and memory requirement,the new simulator provides a powerful tool for tackling larger scale andmore complex problems than can be solved by single-CPU codes. Ahigh-resolution simulation example is presented that models buoyantconvection, induced by a small increase in brine density caused bydissolution of CO2.« less
NASA Astrophysics Data System (ADS)
Possinger, A. R.; Zachman, M.; Lehmann, J.
2016-12-01
An important, yet largely overlooked case of soil organic carbon (SOC) stabilization through mineral-organic associations is the co-precipitation of dissolved organic matter (DOM) into mineral precipitates as they form. The contribution of co-precipitated DOM to the mineral-stabilized SOC pool is expected to be greatest in soil environments with frequent mineral dissolution and precipitation processes. Compared to surface adsorption, properties of mineral-organic co-precipitates are expected to differ at both the particle scale (e.g., total carbon (C) content and composition) and the molecular scale (e.g., impurities in mineral structure), with potential implications for stability and C turnover; additionally, these properties vary across C sources, amounts, and forms. Consequently, high-resolution visualization and characterization combined with bulk chemical measurements is needed to provide a more complete understanding of co-precipitate formation processes and properties, especially as a function of C co-precipitant characteristics. In this study, we evaluate the effect of model C compound and DOM chemical properties (e.g., iron-binding affinity) on the formation, structure, and chemical properties of ferrihydrite (Fh) (Fe3+3O2 •0.5H2O) co-precipitates. Salicylic acid (SA), sucrose and water-extractable DOM from coniferous or deciduous-dominated organic soils were either adsorbed to pre-formed Fh or co-precipitated with Fh. At a C/Fe ratio 10, the amount of co-precipitated C differed among all organic compounds, and for DOM, was more than 2X greater for co-precipitation than adsorption, suggesting a greater capacity for C retention. To probe the molecular-scale C spatial distribution of Fh-SA particles, we obtained Scanning Transmission Electron Microscopy with Electron Energy Loss Spectroscopy (STEM-EELS) maps at a nanometer-scale spatial pixel resolution. Additionally, we will present chemical characteristics of organic-Fh co-precipitates and adsorption complexes investigated in bulk using C Near-Edge X-ray Absorption Fine Structure (NEXAFS) and Fourier Transform Infrared (FT-IR) spectroscopy. Ultimately, these observations of model co-precipitation systems will be used to better interpret observations of putative co-precipitated OM in natural soils.
Critical dynamics of gravito-convective mixing in geological carbon sequestration
Soltanian, Mohamad Reza; Amooie, Mohammad Amin; Dai, Zhenxue; ...
2016-11-03
When CO 2 is injected in saline aquifers, dissolution causes a local increase in brine density that can cause Rayleigh-Taylor-type gravitational instabilities. Depending on the Rayleigh number, density-driven flow may mix dissolved CO 2 throughout the aquifer at fast advective time-scales through convective mixing. Heterogeneity can impact density-driven flow to different degrees. Zones with low effective vertical permeability may suppress fingering and reduce vertical spreading, while potentially increasing transverse mixing. In more complex heterogeneity, arising from the spatial organization of sedimentary facies, finger propagation is reduced in low permeability facies, but may be enhanced through more permeable facies. The connectivitymore » of facies is critical in determining the large-scale transport of CO 2-rich brine. We perform high-resolution finite element simulations of advection-diffusion transport of CO 2 with a focus on facies-based bimodal heterogeneity. Permeability fields are generated by a Markov Chain approach, which represent facies architecture by commonly observed characteristics such as volume fractions. CO 2 dissolution and phase behavior are modeled with the cubic-plus-association equation-of-state. Our results show that the organization of high-permeability facies and their connectivity control the dynamics of gravitationally unstable flow. Lastly, we discover new flow regimes in both homogeneous and heterogeneous media and present quantitative scaling relations for their temporal evolution.« less
Cernusak, Lucas A; Farquhar, Graham D; Wong, S Chin; Stuart-Williams, Hilary
2004-10-01
We measured the oxygen isotope composition (delta(18)O) of CO(2) respired by Ricinus communis leaves in the dark. Experiments were conducted at low CO(2) partial pressure and at normal atmospheric CO(2) partial pressure. Across both experiments, the delta(18)O of dark-respired CO(2) (delta(R)) ranged from 44 per thousand to 324 per thousand (Vienna Standard Mean Ocean Water scale). This seemingly implausible range of values reflects the large flux of CO(2) that diffuses into leaves, equilibrates with leaf water via the catalytic activity of carbonic anhydrase, then diffuses out of the leaf, leaving the net CO(2) efflux rate unaltered. The impact of this process on delta(R) is modulated by the delta(18)O difference between CO(2) inside the leaf and in the air, and by variation in the CO(2) partial pressure inside the leaf relative to that in the air. We developed theoretical equations to calculate delta(18)O of CO(2) in leaf chloroplasts (delta(c)), the assumed location of carbonic anhydrase activity, during dark respiration. Their application led to sensible estimates of delta(c), suggesting that the theory adequately accounted for the labeling of CO(2) by leaf water in excess of that expected from the net CO(2) efflux. The delta(c) values were strongly correlated with delta(18)O of water at the evaporative sites within leaves. We estimated that approximately 80% of CO(2) in chloroplasts had completely exchanged oxygen atoms with chloroplast water during dark respiration, whereas approximately 100% had exchanged during photosynthesis. Incorporation of the delta(18)O of leaf dark respiration into ecosystem and global scale models of C(18)OO dynamics could affect model outputs and their interpretation.
A composite large-scale CO survey at high Galactic latitudes in the second quadrant
NASA Technical Reports Server (NTRS)
Heithausen, A.; Stacy, J. G.; Thaddeus, P.
1990-01-01
Surveys of the second quadrant of the Galaxy undertaken with the CfA 1.2-m telescope have been combined to produce a map of approximately 620 sq deg in the 2.6-mm CO (J = 1-0) line at high Galactic latitudes. CO was detected over about 13 percent of the region surveyed, an order of magnitude more gas by area than previously estimated. In contrast, only 26 percent of the area predicted by Desert et al. (1988) to contain molecular gas actually reveals CO, and about two-thirds of the clouds detected are not listed in their catalog of IR excess clouds.
Carbonyl Sulfide: is it AN Isotope of CO2 on Steroids?
NASA Astrophysics Data System (ADS)
Berry, J. A.; Campbell, J. E.; Baker, I. T.; Whelan, M.; Hilton, T. W.
2015-12-01
The behavior of OCS in the atmosphere is very similar to that of CO2 and reminiscent of an isotopologue. It is stable, has a turnover time of a couple of years (similar to that of 18O in CO2). It can be measured with adequate accuracy - despite the fact that its abundance is one millionth that of CO2, but there is one dramatic difference. The seasonal variation in the concentration of OCS relative to its background concentration can be 6-10 fold larger than the corresponding variation in CO2 concentration. Furthermore there are large spatial gradients in atmospheric OCS, with the concentrations being generally lower over the continents than the ocean, and lower in the atmospheric boundary layer over vegetated surfaces than in the free troposphere. These gradients have been clearly resolved by flask sampling from aircraft and recently by satellite measurements. The dynamics of OCS are larger than any other conserved atmospheric gas and certainly dwarf isotopic gradients. There are strong differences in the kinetics of CO2 and OCS exchange with leaves (similar to an isotopic fractionation), but these are not responsible for the large atmospheric signals. The major driver of these gradients is a large spatial separation between the major sources of OCS (the tropical ocean) and the major sink (the terrestrial biosphere). This talk will review the biogeochemical cycle of OCS; the kinetics of its exchange with leaves and soils; the distribution of sources and sinks, and the local and large scale gradients of OCS concentration in the atmosphere.
High throughput screening of CO2-tolerating microalgae using GasPak bags
2013-01-01
Background Microalgae are diverse in terms of their speciation and function. More than 35,000 algal strains have been described, and thousands of algal cultures are maintained in different culture collection centers. The ability of CO2 uptake by microalgae varies dramatically among algal species. It becomes challenging to select suitable algal candidates that can proliferate under high CO2 concentration from a large collection of algal cultures. Results Here, we described a high throughput screening method to rapidly identify high CO2 affinity microalgae. The system integrates a CO2 mixer, GasPak bags and microplates. Microalgae on the microplates will be cultivated in GasPak bags charged with different CO2 concentrations. Using this method, we identified 17 algal strains whose growth rates were not influenced when the concentration of CO2 was increased from 2 to 20% (v/v). Most CO2 tolerant strains identified in this study were closely related to the species Scenedesmus and Chlorococcum. One of Scenedesmus strains (E7A) has been successfully tested in in the scale up photo bioreactors (500 L) bubbled with flue gas which contains 10-12% CO2. Conclusion Our high throughput CO2 testing system provides a rapid and reliable way for identifying microalgal candidate strains that can grow under high CO2 condition from a large pool of culture collection species. This high throughput system can also be modified for selecting algal strains that can tolerate other gases, such as NOx, SOx, or flue gas. PMID:24341988
Early opportunities of CO2 geological storage deployment in coal chemical industry in China
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wei, Ning; Li, Xiaochun; Liu, Shengnan
2014-11-12
Abstract: Carbon dioxide capture and geological storage (CCS) is regarded as a promising option for climate change mitigation; however, the high capture cost is the major barrier to large-scale deployment of CCS technologies. High-purity CO2 emission sources can reduce or even avoid the capture requirements and costs. Among these high-purity CO2 sources, certain coal chemical industry processes are very important, especially in China. In this paper, the basic characteristics of coal chemical industries in China is investigated and analyzed. As of 2013 there were more than 100 coal chemical plants in operation or in late planning stages. These emission sourcesmore » together emit 430 million tons CO2 per year, of which about 30% are emit high-purity and pure CO2 (CO2 concentration >80% and >99% respectively).Four typical source-sink pairs are studied by a techno-economic evaluation, including site screening and selection, source-sink matching, concept design, and experienced economic evaluation. The technical-economic evaluation shows that the levelized cost of a CO2 capture and aquifer storage project in the coal chemistry industry ranges from 14 USD/t to 17 USD/t CO2. When a 15USD/t CO2 tax and 15USD/t for CO2 sold to EOR are considered, the levelized cost of CCS project are negative, which suggests a net economic benefit from some of these CCS projects. This might provide China early opportunities to deploy and scale-up CCS projects in the near future.« 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
Shi, Yusheng; Matsunaga, Tsuneo
2017-07-01
Biomass burning is a large important source of greenhouse gases and atmospheric aerosols, and can contribute greatly to the temporal variations of CO 2 emissions at regional and global scales. In this study, we compared four globally gridded CO 2 emission inventories from biomass burning during the period of 2002-2011, highlighting the similarities and differences in seasonality and interannual variability of the CO 2 emissions both at regional and global scales. The four datasets included Global Fire Emissions Database 4s with small fires (GFED4s), Global Fire Assimilation System 1.0 (GFAS1.0), Fire INventory from NCAR 1.0 (FINN1.0), and Global Inventory for Chemistry-Climate studies-GFED4s (G-G). The results showed that in general, the four inventories presented consistent temporal trend but with large differences as well. Globally, CO 2 emissions of GFED4s, GFAS1.0, and G-G all peaked in August with the exception in FINN1.0, which recorded another peak in annual March. The interannual trend of all datasets displayed an overall decrease in CO 2 emissions during 2002-2011, except for the inconsistent FINN1.0, which showed a tendency to increase during the considered period. Meanwhile, GFED4s and GFAS1.0 noted consistent agreement from 2002 to 2011 at both global (R 2 > 0.8) and continental levels (R 2 > 0.7). FINN1.0 was found to have the poorest temporal correlations with the other three inventories globally (R 2 < 0.6). The lower estimation in savanna CO 2 emissions and higher calculation in cropland CO 2 emissions by FINN1.0 from 2002 to 2011 was the primary reason for the temporal differences of the four inventories. Besides, the contributions of the three land covers (forest, savanna, and cropland) on CO 2 emissions in each region varied greatly within the year (>80%) but showed small variations through the years (<40%).
Rashev, Svetoslav; Moule, David C; Rashev, Vladimir
2012-11-01
We perform converged high precision variational calculations to determine the frequencies of a large number of vibrational levels in S(0) D(2)CO, extending from low to very high excess vibrational energies. For the calculations we use our specific vibrational method (recently employed for studies on H(2)CO), consisting of a combination of a search/selection algorithm and a Lanczos iteration procedure. Using the same method we perform large scale converged calculations on the vibrational level spectral structure and fragmentation at selected highly excited overtone states, up to excess vibrational energies of ∼17,000 cm(-1), in order to study the characteristics of intramolecular vibrational redistribution (IVR), vibrational level density and mode selectivity. Copyright © 2012 Elsevier B.V. All rights reserved.
Ellett, Kevin M.; Middleton, Richard S.; Stauffer, Philip H.; ...
2017-08-18
The application of integrated system models for evaluating carbon capture and storage technology has expanded steadily over the past few years. To date, such models have focused largely on hypothetical scenarios of complex source-sink matching involving numerous large-scale CO 2 emitters, and high-volume, continuous reservoirs such as deep saline formations to function as geologic sinks for carbon storage. Though these models have provided unique insight on the potential costs and feasibility of deploying complex networks of integrated infrastructure, there remains a pressing need to translate such insight to the business community if this technology is to ever achieve a trulymore » meaningful impact in greenhouse gas mitigation. Here, we present a new integrated system modelling tool termed SimCCUS aimed at providing crucial decision support for businesses by extending the functionality of a previously developed model called SimCCS. The primary innovation of the SimCCUS tool development is the incorporation of stacked geological reservoir systems with explicit consideration of processes and costs associated with the operation of multiple CO 2 utilization and storage targets from a single geographic location. In such locations provide significant efficiencies through economies of scale, effectively minimizing CO 2 storage costs while simultaneously maximizing revenue streams via the utilization of CO 2 as a commodity for enhanced hydrocarbon recovery.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Berné, O.; Cernicharo, J.; Marcelino, N., E-mail: olivier.berne@irap.omp.eu
2014-11-01
Using the IRAM 30 m telescope, we have surveyed a 1 × 0.°8 part of the Orion molecular cloud in the {sup 12}CO and {sup 13}CO (2-1) lines with a maximal spatial resolution of ∼11'' and spectral resolution of ∼0.4 km s{sup –1}. The cloud appears filamentary, clumpy, and with a complex kinematical structure. We derive an estimated mass of the cloud of 7700 M {sub ☉} (half of which is found in regions with visual extinctions A{sub V} below ∼10) and a dynamical age for the nebula of the order of 0.2 Myr. The energy balance suggests that magneticmore » fields play an important role in supporting the cloud, at large and small scales. According to our analysis, the turbulent kinetic energy in the molecular gas due to outflows is comparable to turbulent kinetic energy resulting from the interaction of the cloud with the H II region. This latter feedback appears negative, i.e., the triggering of star formation by the H II region is inefficient in Orion. The reduced data as well as additional products such as the column density map are made available online (http://userpages.irap.omp.eu/∼oberne/Olivier{sub B}erne/Data).« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ellett, Kevin M.; Middleton, Richard S.; Stauffer, Philip H.
The application of integrated system models for evaluating carbon capture and storage technology has expanded steadily over the past few years. To date, such models have focused largely on hypothetical scenarios of complex source-sink matching involving numerous large-scale CO 2 emitters, and high-volume, continuous reservoirs such as deep saline formations to function as geologic sinks for carbon storage. Though these models have provided unique insight on the potential costs and feasibility of deploying complex networks of integrated infrastructure, there remains a pressing need to translate such insight to the business community if this technology is to ever achieve a trulymore » meaningful impact in greenhouse gas mitigation. Here, we present a new integrated system modelling tool termed SimCCUS aimed at providing crucial decision support for businesses by extending the functionality of a previously developed model called SimCCS. The primary innovation of the SimCCUS tool development is the incorporation of stacked geological reservoir systems with explicit consideration of processes and costs associated with the operation of multiple CO 2 utilization and storage targets from a single geographic location. In such locations provide significant efficiencies through economies of scale, effectively minimizing CO 2 storage costs while simultaneously maximizing revenue streams via the utilization of CO 2 as a commodity for enhanced hydrocarbon recovery.« less
Simulated changes in aridity from the last glacial maximum to 4xCO2
NASA Astrophysics Data System (ADS)
Greve, Peter; Roderick, Michael L.; Seneviratne, Sonia I.
2017-11-01
Aridity is generally defined as the ‘degree to which a climate lacks moisture to sustain life in terrestrial ecosystems’. Several recent studies using the ‘aridity index’ (the ratio of potential evaporation to precipitation), have concluded that aridity will increase with CO2 because of increasing temperature. However, the ‘aridity index’ is—counterintuitively—not a direct measure of aridity per se (when defined as above) and there is widespread evidence that contradicts the ‘warmer is more arid’ interpretation. We provide here an assessment of multi-model changes in a broad set of aridity metrics over a large range of atmospheric CO2 concentrations ranging from conditions at the last glacial maximum to 4xCO2, using an ensemble of simulations from state-of-the-art Earth system models. Most measures of aridity do not show increasing aridity on global scales under conditions of increasing atmospheric CO2 concentrations and related global warming, although we note some varying responses depending on the considered variables. The response is, furthermore, more nuanced at regional scales, but in the majority of regions aridity does not increase with CO2 in the majority of metrics. Our results emphasize that it is not the climate models that project overwhelming increases of aridity with increasing CO2, but rather a secondary, offline, impact model—the ‘aridity index’—that uses climate model output as input.
NASA Astrophysics Data System (ADS)
Cihan, A.; Illangasekare, T. H.; Zhou, Q.; Birkholzer, J. T.; Rodriguez, D.
2010-12-01
The capillary and dissolution trapping processes are believed to be major trapping mechanisms during CO2 injection and post-injection in heterogeneous subsurface environments. These processes are important at relatively shorter time periods compared to mineralization and have a strong impact on storage capacity and leakage risks, and they are suitable to investigate at reasonable times in the laboratory. The objectives of the research presented is to investigate the effect of the texture transitions and variability in heterogeneous field formations on the effective capillary and dissolution trapping at the field scale through multistage analysis comprising of experimental and modeling studies. A series of controlled experiments in intermediate-scale test tanks are proposed to investigate the key processes involving (1) viscous fingering of free-phase CO2 along high-permeability (or high-K) fast flow pathways, (2) dynamic intrusion of CO2 from high-K zones into low-K zones by capillarity (as well as buoyancy), (3) diffusive transport of dissolved CO2 into low-K zones across large interface areas, and (4) density-driven convective mass transfer into CO2-free regions. The test tanks contain liquid sampling ports to measure spatial and temporal changes in concentration of dissolved fluid as the injected fluid migrates. In addition to visualization and capturing images through digital photography, X-ray and gamma attenuation methods are used to measure phase saturations. Heterogeneous packing configurations are created with tightly packed sands ranging from very fine to medium fine to mimic sedimentary rocks at potential storage formations. Effect of formation type, injection pressure and injection rate on trapped fluid fraction are quantified. Macroscopic variables such as saturation, pressure and concentration that are measured will be used for testing the existing macroscopic models. The applicability of multiphase flow theories will be evaluated by comparing with the experimental data. Existing upscaling methodologies will be tested using experimental data for accurately estimating parameters of the large-scale heterogeneous porous media. This paper presents preliminary results from the initial-stage experiments and the modeling analysis. In the future, we will design and conduct a comprehensive set of experiments for improving the fundamental understanding of the processes, and refine and calibrate the models simulating the effective capillary and dissolution trapping with an ultimate goal to design efficient and safe storage schemes.
Carbon dioxide capture from atmospheric air using sodium hydroxide spray.
Stolaroff, Joshuah K; Keith, David W; Lowry, Gregory V
2008-04-15
In contrast to conventional carbon capture systems for power plants and other large point sources, the system described in this paper captures CO2 directly from ambient air. This has the advantages that emissions from diffuse sources and past emissions may be captured. The objective of this research is to determine the feasibility of a NaOH spray-based contactor for use in an air capture system by estimating the cost and energy requirements per unit CO2 captured. A prototype system is constructed and tested to measure CO2 absorption, energy use, and evaporative water loss and compared with theoretical predictions. A numerical model of drop collision and coalescence is used to estimate operating parameters for a full-scale system, and the cost of operating the system per unit CO2 captured is estimated. The analysis indicates that CO2 capture from air for climate change mitigation is technically feasible using off-the-shelf technology. Drop coalescence significantly decreases the CO2 absorption efficiency; however, fan and pump energy requirements are manageable. Water loss is significant (20 mol H2O/mol CO2 at 15 degrees C and 65% RH) but can be lowered by appropriately designing and operating the system. The cost of CO2 capture using NaOH spray (excluding solution recovery and CO2 sequestration, which may be comparable) in the full-scale system is 96 $/ton-CO2 in the base case, and ranges from 53 to 127 $/ton-CO2 under alternate operating parameters and assumptions regarding capital costs and mass transfer rate. The low end of the cost range is reached by a spray with 50 microm mean drop diameter, which is achievable with commercially available spray nozzles.
NASA Astrophysics Data System (ADS)
Fakhari, Abbas; Li, Yaofa; Bolster, Diogo; Christensen, Kenneth T.
2018-04-01
We implement a phase-field based lattice-Boltzmann (LB) method for numerical simulation of multiphase flows in heterogeneous porous media at pore scales with wettability effects. The present method can handle large density and viscosity ratios, pertinent to many practical problems. As a practical application, we study multiphase flow in a micromodel representative of CO2 invading a water-saturated porous medium at reservoir conditions, both numerically and experimentally. We focus on two flow cases with (i) a crossover from capillary fingering to viscous fingering at a relatively small capillary number, and (ii) viscous fingering at a relatively moderate capillary number. Qualitative and quantitative comparisons are made between numerical results and experimental data for temporal and spatial CO2 saturation profiles, and good agreement is found. In particular, a correlation analysis shows that any differences between simulations and results are comparable to intra-experimental differences from replicate experiments. A key conclusion of this work is that system behavior is highly sensitive to boundary conditions, particularly inlet and outlet ones. We finish with a discussion on small-scale flow features, such as the emergence of strong recirculation zones as well as flow in which the residual phase is trapped, including a close look at the detailed formation of a water cone. Overall, the proposed model yields useful information, such as the spatiotemporal evolution of the CO2 front and instantaneous velocity fields, which are valuable for understanding the mechanisms of CO2 infiltration at the pore scale.
Quantifying CO2 Emissions From Individual Power Plants From Space
NASA Astrophysics Data System (ADS)
Nassar, Ray; Hill, Timothy G.; McLinden, Chris A.; Wunch, Debra; Jones, Dylan B. A.; Crisp, David
2017-10-01
In order to better manage anthropogenic CO2 emissions, improved methods of quantifying emissions are needed at all spatial scales from the national level down to the facility level. Although the Orbiting Carbon Observatory 2 (OCO-2) satellite was not designed for monitoring power plant emissions, we show that in some cases, CO2 observations from OCO-2 can be used to quantify daily CO2 emissions from individual middle- to large-sized coal power plants by fitting the data to plume model simulations. Emission estimates for U.S. power plants are within 1-17% of reported daily emission values, enabling application of the approach to international sites that lack detailed emission information. This affirms that a constellation of future CO2 imaging satellites, optimized for point sources, could monitor emissions from individual power plants to support the implementation of climate policies.
Eichner, Meri J; Klawonn, Isabell; Wilson, Samuel T; Littmann, Sten; Whitehouse, Martin J; Church, Matthew J; Kuypers, Marcel MM; Karl, David M; Ploug, Helle
2017-01-01
Gradients of oxygen (O2) and pH, as well as small-scale fluxes of carbon (C), nitrogen (N) and O2 were investigated under different partial pressures of carbon dioxide (pCO2) in field-collected colonies of the marine dinitrogen (N2)-fixing cyanobacterium Trichodesmium. Microsensor measurements indicated that cells within colonies experienced large fluctuations in O2, pH and CO2 concentrations over a day–night cycle. O2 concentrations varied with light intensity and time of day, yet colonies exposed to light were supersaturated with O2 (up to ~200%) throughout the light period and anoxia was not detected. Alternating between light and dark conditions caused a variation in pH levels by on average 0.5 units (equivalent to 15 nmol l−1 proton concentration). Single-cell analyses of C and N assimilation using secondary ion mass spectrometry (SIMS; large geometry SIMS and nanoscale SIMS) revealed high variability in metabolic activity of single cells and trichomes of Trichodesmium, and indicated transfer of C and N to colony-associated non-photosynthetic bacteria. Neither O2 fluxes nor C fixation by Trichodesmium were significantly influenced by short-term incubations under different pCO2 levels, whereas N2 fixation increased with increasing pCO2. The large range of metabolic rates observed at the single-cell level may reflect a response by colony-forming microbial populations to highly variable microenvironments. PMID:28398346
NASA Astrophysics Data System (ADS)
Balzarolo, M.; Vescovo, L.; Hammerle, A.; Gianelle, D.; Papale, D.; Tomelleri, E.; Wohlfahrt, G.
2015-05-01
In this paper we explore the skill of hyperspectral reflectance measurements and vegetation indices (VIs) derived from these in estimating carbon dioxide (CO2) fluxes of grasslands. Hyperspectral reflectance data, CO2 fluxes and biophysical parameters were measured at three grassland sites located in European mountain regions using standardized protocols. The relationships between CO2 fluxes, ecophysiological variables, traditional VIs and VIs derived using all two-band combinations of wavelengths available from the whole hyperspectral data space were analysed. We found that VIs derived from hyperspectral data generally explained a large fraction of the variability in the investigated dependent variables but differed in their ability to estimate midday and daily average CO2 fluxes and various derived ecophysiological parameters. Relationships between VIs and CO2 fluxes and ecophysiological parameters were site-specific, likely due to differences in soils, vegetation parameters and environmental conditions. Chlorophyll and water-content-related VIs explained the largest fraction of variability in most of the dependent variables. Band selection based on a combination of a genetic algorithm with random forests (GA-rF) confirmed that it is difficult to select a universal band region suitable across the investigated ecosystems. Our findings have major implications for upscaling terrestrial CO2 fluxes to larger regions and for remote- and proximal-sensing sampling and analysis strategies and call for more cross-site synthesis studies linking ground-based spectral reflectance with ecosystem-scale CO2 fluxes.
Multi-scale modeling of CO2 dispersion leaked from seafloor off the Japanese coast.
Kano, Yuki; Sato, Toru; Kita, Jun; Hirabayashi, Shinichiro; Tabeta, Shigeru
2010-02-01
A numerical simulation was conducted to predict the change of pCO(2) in the ocean caused by CO(2) leaked from an underground aquifer, in which CO(2) is purposefully stored. The target space of the present model was the ocean above the seafloor. The behavior of CO(2) bubbles, their dissolution, and the advection-diffusion of dissolved CO(2) were numerically simulated. Here, two cases for the leakage rate were studied: an extreme case, 94,600 t/y, which assumed that a large fault accidentally connects the CO(2) reservoir and the seafloor; and a reasonable case, 3800 t/y, based on the seepage rate of an existing EOR site. In the extreme case, the calculated increase in DeltapCO(2) experienced by floating organisms was less than 300 ppm, while that for immobile organisms directly over the fault surface periodically exceeded 1000 ppm, if momentarily. In the reasonable case, the calculated DeltapCO(2) and pH were within the range of natural fluctuation. Copyright 2009 Elsevier Ltd. All rights reserved.
NASA Astrophysics Data System (ADS)
Aman, M.; Sun, Y.; Ilgen, A.; Espinoza, N.
2015-12-01
Injection of large volumes of CO2 into geologic formations can help reduce the atmospheric CO2 concentration and lower the impact of burning fossil fuels. However, the injection of CO2 into the subsurface shifts the chemical equilibrium between the mineral assemblage and the pore fluid. This shift will situationally facilitate dissolution and reprecipitation of mineral phases, in particular intergranular cements, and can potentially affect the long term mechanical stability of the host formation. The study of these coupled chemical-mechanical reservoir rock responses can help identify and control unexpected emergent behavior associated with geological CO2 storage.Experiments show that micro-mechanical methods are useful in capturing a variety of mechanical parameters, including Young's modulus, hardness and fracture toughness. In particular, micro-mechanical measurements are well-suited for examining thin altered layers on the surfaces of rock specimens, as well as capturing variability on the scale of lithofacies. We performed indentation and scratching tests on sandstone and siltstone rocks altered in natural CO2-brine environments, as well as on analogous samples altered under high pressure, temperature, and dissolved CO2 conditions in a controlled laboratory experiment. We performed geochemical modeling to support the experimental observations, in particular to gain the insight into mineral dissolution/precipitation as a result of the rock-water-CO2reactions. The comparison of scratch measurements performed on specimens both unaltered and altered by CO2 over geologic time scales results in statistically different values for fracture toughness and scratch hardness, indicating that long term exposure to CO2 caused mechanical degradation of the reservoir rock. Geochemical modeling indicates that major geochemical change caused by CO2 invasion of Entrada sandstone is dissolution of hematite cement, and its replacement with siderite and dolomite during the alteration process.
Empirically constrained estimates of Alaskan regional Net Ecosystem Exchange of CO2, 2012-2014
NASA Astrophysics Data System (ADS)
Commane, R.; Lindaas, J.; Benmergui, J. S.; Luus, K. A.; Chang, R. Y. W.; Miller, S. M.; Henderson, J.; Karion, A.; Miller, J. B.; Sweeney, C.; Miller, C. E.; Lin, J. C.; Oechel, W. C.; Zona, D.; Euskirchen, E. S.; Iwata, H.; Ueyama, M.; Harazono, Y.; Veraverbeke, S.; Randerson, J. T.; Daube, B. C.; Pittman, J. V.; Wofsy, S. C.
2015-12-01
We present data-driven estimates of the regional net ecosystem exchange of CO2 across Alaska for three years (2012-2014) derived from CARVE (Carbon in the Arctic Reservoirs Vulnerability Experiment) aircraft measurements. Integrating optimized estimates of annual NEE, we find that the Alaskan region was a small sink of CO2 during 2012 and 2014, but a significant source of CO2 in 2013, even before including emissions from the large forest fire season during 2013. We investigate the drivers of this interannual variability, and the larger spring and fall emissions of CO2 in 2013. To determine the optimized fluxes, we couple the Polar Weather Research and Forecasting (PWRF) model with the Stochastic Time-Inverted Lagrangian Transport (STILT) model, to produce footprints of surface influence that we convolve with a remote-sensing driven model of NEE across Alaska, the Polar Vegetation Photosynthesis and Respiration Model (Polar-VPRM). For each month we calculate a spatially explicit additive flux (ΔF) by minimizing the difference between the measured profiles of the aircraft CO2 data and the modeled profiles, using a framework that combines a uniform correction at regional scales and a Bayesian inversion of residuals at smaller scales. A rigorous estimate of total uncertainty (including atmospheric transport, measurement error, etc.) was made with a combination of maximum likelihood estimation and Monte Carlo error propagation. Our optimized fluxes are consistent with other measurements on multiple spatial scales, including CO2 mixing ratios from the CARVE Tower near Fairbanks and eddy covariance flux towers in both boreal and tundra ecosystems across Alaska. For times outside the aircraft observations (Dec-April) we use the un-optimized polar-VPRM, which has shown good agreement with both tall towers and eddy flux data outside the growing season. This approach allows us to robustly estimate the annual CO2 budget for Alaska and investigate the drivers of both the seasonal cycle and the interannual variability of CO2 for the region.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bieging, John H.; Revelle, Melissa; Peters, William L.
2014-09-01
We mapped the NGC 1333 section of the Perseus Molecular Cloud in the J = 2-1 emission lines of {sup 12}CO and {sup 13}CO over a 50' × 60' region (3.4 × 4.1 pc at the cloud distance of 235 pc), using the Arizona Radio Observatory Heinrich Hertz Submillimeter Telescope. The angular resolution is 38'' (0.04 pc) and velocity resolution is 0.3 km s{sup –1}. We compare our velocity moment maps with known positions of young stellar objects (YSOs) and (sub)millimeter dust continuum emission. The CO emission is brightest at the center of the cluster of YSOs, but is detectedmore » over the full extent of the mapped region at ≥10 × rms. The morphology of the CO channel maps shows a kinematically complex structure, with many elongated features extending from the YSO cluster outward by ∼1 pc. One notable feature appears as a narrow serpentine structure that curves and doubles back, with a total length of ∼3 pc. The {sup 13}CO velocity channel maps show evidence for many low-density cavities surrounded by partial shell-like structures, consistent with previous studies. Maps of the velocity moments show localized effects of bipolar outflows from embedded YSOs, as well as a large-scale velocity gradient around the central core of YSOs, suggestive of large-scale turbulent cloud motions determining the location of current star formation. The CO/{sup 13}CO intensity ratios show the distribution of the CO opacity, which exhibits a complex kinematic structure. Identified YSOs are located mainly at the positions of greatest CO opacity. The maps are available for download as FITS files.« less
Carr, T.R.; Merriam, D.F.; Bartley, J.D.
2005-01-01
Large-scale relational databases and geographic information system tools are used to integrate temperature, pressure, and water geo-chemistry data from numerous wells to better understand regional-scale geothermal and hydrogeological regimes of the lower Paleozoic aquifer systems in the mid-continent and to evaluate their potential for geologic CO2 sequestration. The lower Paleozoic (Cambrian to Mississippian) aquifer systems in Kansas, Missouri, and Oklahoma comprise one of the largest regional-scale saline aquifer systems in North America. Understanding hydrologic conditions and processes of these regional-scale aquifer systems provides insight to the evolution of the various sedimentary basins, migration of hydrocarbons out of the Anadarko and Arkoma basins, and the distribution of Arbuckle petroleum reservoirs across Kansas and provides a basis to evaluate CO2 sequestration potential. The Cambrian and Ordovician stratigraphic units form a saline aquifer that is in hydrologic continuity with the freshwater recharge from the Ozark plateau and along the Nemaha anticline. The hydrologic continuity with areas of freshwater recharge provides an explanation for the apparent underpressure in the Arbuckle Group. Copyright ?? 2005. The American Association of Petroleum Geologists. All rights reserved.
Blombach, Bastian; Takors, Ralf
2015-01-01
Carbon dioxide formation mirrors the final carbon oxidation steps of aerobic metabolism in microbial and mammalian cells. As a consequence, CO2/HCO3− dissociation equilibria arise in fermenters by the growing culture. Anaplerotic reactions make use of the abundant CO2/HCO3− levels for refueling citric acid cycle demands and for enabling oxaloacetate-derived products. At the same time, CO2 is released manifold in metabolic reactions via decarboxylation activity. The levels of extracellular CO2/HCO3− depend on cellular activities and physical constraints such as hydrostatic pressures, aeration, and the efficiency of mixing in large-scale bioreactors. Besides, local CO2/HCO3− levels might also act as metabolic inhibitors or transcriptional effectors triggering regulatory events inside the cells. This review gives an overview about fundamental physicochemical properties of CO2/HCO3− in microbial and mammalian cultures effecting cellular physiology, production processes, metabolic activity, and transcriptional regulation. PMID:26284242
Carbon and water vapor fluxes of different ecosystems in Oklahoma
USDA-ARS?s Scientific Manuscript database
Information on exchange of energy, carbon dioxide (CO2), and water vapor (H2O) for major terrestrial ecosystems is vital to quantify carbon and water balances on a large-scale. It is also necessary to develop, test, and improve crop models and satellite-based production efficiency and evapotranspira...
NRG CO 2NCEPT - Confirmation Of Novel Cost-effective Emerging Post-combustion Technology
DOE Office of Scientific and Technical Information (OSTI.GOV)
Stevenson, Matthew; Armpriester, Anthony
Under DOE's solicitation DE-FOA-0001190, NRG and Inventys conceptualized a Large-Scale pilot (>10MWe) post-combustion CO 2 capture project using Inventys' VeloxoThermTM carbon capture technology. The technology is comprised of an intensified thermal swing adsorption (TSA) process that uses a patented architecture of structured adsorbent and a novel process design and embodiment to capture CO 2 from industrial flue gas streams. The result of this work concluded that the retrofit of this technology is economically and technically viable, but that the sorbent material selected for the program would need improving to meet the techno-economic performance requirements of the solicitation.
Monitoring CO2 sources and sinks from space : the Orbiting Carbon Observatory (OCO) Mission
NASA Technical Reports Server (NTRS)
Crisp, David
2006-01-01
NASA's Orbiting Carbon Observatory (OCO) will make the first space-based measurements of atmospheric carbon dioxide (CO2) with the precision, resolution, and coverage needed to characterize the geographic distribution of CO2 sources and sinks and quantify their variability over the seasonal cycle. OCO is currently scheduled for launch in 2008. The observatory will carry a single instrument that incorporates three high-resolution grating spectrometers designed to measure the near-infrared absorption by CO2 and molecular oxygen (O2) in reflected sunlight. OCO will fly 12 minutes ahead of the EOS Aqua platform in the Earth Observing System (EOS) Afternoon Constellation (A-Train). The in-strument will collect 12 to 24 soundings per second as the Observatory moves along its orbit track on the day side of the Earth. A small sampling footprint (<3 km2 at nadir) was adopted to reduce biases in each sounding associated with clouds and aerosols and spatial variations in surface topography. A comprehensive ground-based validation program will be used to assess random errors and biases in the XCO2 product on regional to continental scales. Measurements collected by OCO will be assimilated with other environmental measurements to retrieve surface sources and sinks of CO2. This information could play an important role in monitoring the integrity of large scale CO2 sequestration projects.
Hierarchical Engine for Large-scale Infrastructure Co-Simulation
DOE Office of Scientific and Technical Information (OSTI.GOV)
2017-04-24
HELICS is designed to support very-large-scale (100,000+ federates) cosimulations with off-the-shelf power-system, communication, market, and end-use tools. Other key features include cross platform operating system support, the integration of both event driven (e.g., packetized communication) and time-series (e.g., power flow) simulations, and the ability to co-iterate among federates to ensure physical model convergence at each time step.
NASA Astrophysics Data System (ADS)
Hacar, A.; Alves, J.; Burkert, A.; Goldsmith, P.
2016-06-01
Context. Since their first detection in the interestellar medium, (sub-)millimeter line observations of different CO isotopic variants have routinely been employed to characterize the kinematic properties of the gas in molecular clouds. Many of these lines exhibit broad linewidths that greatly exceed the thermal broadening expected for the low temperatures found within these objects. These observed suprathermal CO linewidths are assumed to originate from unresolved supersonic motions inside clouds. Aims: The lowest rotational J transitions of some of the most abundant CO isotopologues, 12CO and 13CO, are found to present large optical depths. In addition to well-known line saturation effects, these large opacities present a non-negligible contribution to their observed linewidths. Typically overlooked in the literature, in this paper we aim to quantify the impact of these opacity broadening effects on the current interpretation of the CO suprathermal line profiles. Methods: Combining large-scale observations and LTE modeling of the ground J = 1-0 transitions of the main 12CO, 13CO, C18O isotopologues, we have investigated the correlation of the observed linewidths as a function of the line opacity in different regions of the Taurus molecular cloud. Results: Without any additional contributions to the gas velocity field, a large fraction of the apparently supersonic (ℳ ~ 2-3) linewidths measured in both 12CO and 13CO (J = 1-0) lines can be explained by the saturation of their corresponding sonic-like, optically thin C18O counterparts assuming standard isotopic fractionation. Combined with the presence of multiple components detected in some of our C18O spectra, these opacity effects also seem to be responsible for most of the highly supersonic linewidths (ℳ > 8-10) detected in some of the broadest 12CO and 13CO spectra in Taurus. Conclusions: Our results demonstrate that most of the suprathermal 12CO and 13CO linewidths reported in nearby clouds like Taurus could be primarily created by a combination of opacity broadening effects and multiple gas velocity components blended in these saturated emission lines. Once corrected by their corresponding optical depth, each of these gas components present transonic intrinsic linewidths consistently traced by the three isotopologues, 12CO, 13CO, and C18O, with differences within a factor of 2. Highly correlated and velocity-coherent at large scales, the largest and highly supersonic velocity differences inside clouds are generated by the relative motions between individual gas components. In contrast to the classical interpretation within the framework of microscopic turbulence, this highly discretized structure of the molecular gas traced in CO suggest that the gas dynamics inside molecular clouds could be better described by the properties of a fully resolved macroscopic turbulence.
Ren, Dong; Shen, Yun; Yang, Yao; Shen, Luxi; Levin, Barnaby D A; Yu, Yingchao; Muller, David A; Abruña, Héctor D
2017-10-18
Ni-rich LiNi x Mn y Co 1-x-y O 2 (x > 0.5) (NMC) materials have attracted a great deal of interest as promising cathode candidates for Li-ion batteries due to their low cost and high energy density. However, several issues, including sensitivity to moisture, difficulty in reproducibly preparing well-controlled morphology particles and, poor cyclability, have hindered their large scale deployment; especially for electric vehicle (EV) applications. In this work, we have developed a uniform, highly stable, high-energy density, Ni-rich LiNi 0.6 Mn 0.2 Co 0.2 O 2 cathode material by systematically optimizing synthesis parameters, including pH, stirring rate, and calcination temperature. The particles exhibit a spherical morphology and uniform size distribution, with a well-defined structure and homogeneous transition-metal distribution, owing to the well-controlled synthesis parameters. The material exhibited superior electrochemical properties, when compared to a commercial sample, with an initial discharge capacity of 205 mAh/g at 0.1 C. It also exhibited a remarkable rate capability with discharge capacities of 157 mAh/g and 137 mAh/g at 10 and 20 C, respectively, as well as high tolerance to air and moisture. In order to demonstrate incorporation into a commercial scale EV, a large-scale 4.7 Ah LiNi 0.6 Mn 0.2 Co 0.2 O 2 Al-full pouch cell with a high cathode loading of 21.6 mg/cm 2 , paired with a graphite anode, was fabricated. It exhibited exceptional cyclability with a capacity retention of 96% after 500 cycles at room temperature. This material, which was obtained by a fully optimized scalable synthesis, delivered combined performance metrics that are among the best for NMC materials reported to date.
Aggregation of carbon dioxide sequestration storage assessment units
Blondes, Madalyn S.; Schuenemeyer, John H.; Olea, Ricardo A.; Drew, Lawrence J.
2013-01-01
The U.S. Geological Survey is currently conducting a national assessment of carbon dioxide (CO2) storage resources, mandated by the Energy Independence and Security Act of 2007. Pre-emission capture and storage of CO2 in subsurface saline formations is one potential method to reduce greenhouse gas emissions and the negative impact of global climate change. Like many large-scale resource assessments, the area under investigation is split into smaller, more manageable storage assessment units (SAUs), which must be aggregated with correctly propagated uncertainty to the basin, regional, and national scales. The aggregation methodology requires two types of data: marginal probability distributions of storage resource for each SAU, and a correlation matrix obtained by expert elicitation describing interdependencies between pairs of SAUs. Dependencies arise because geologic analogs, assessment methods, and assessors often overlap. The correlation matrix is used to induce rank correlation, using a Cholesky decomposition, among the empirical marginal distributions representing individually assessed SAUs. This manuscript presents a probabilistic aggregation method tailored to the correlations and dependencies inherent to a CO2 storage assessment. Aggregation results must be presented at the basin, regional, and national scales. A single stage approach, in which one large correlation matrix is defined and subsets are used for different scales, is compared to a multiple stage approach, in which new correlation matrices are created to aggregate intermediate results. Although the single-stage approach requires determination of significantly more correlation coefficients, it captures geologic dependencies among similar units in different basins and it is less sensitive to fluctuations in low correlation coefficients than the multiple stage approach. Thus, subsets of one single-stage correlation matrix are used to aggregate to basin, regional, and national scales.
Jie, Xiangyu; Gonzalez-Cortes, Sergio; Xiao, Tiancun; Wang, Jiale; Yao, Benzhen; Slocombe, Daniel R; Al-Megren, Hamid A; Dilworth, Jonathan R; Thomas, John M; Edwards, Peter P
2017-08-14
Hydrogen as an energy carrier promises a sustainable energy revolution. However, one of the greatest challenges for any future hydrogen economy is the necessity for large scale hydrogen production not involving concurrent CO 2 production. The high intrinsic hydrogen content of liquid-range alkane hydrocarbons (including diesel) offers a potential route to CO 2 -free hydrogen production through their catalytic deep dehydrogenation. We report here a means of rapidly liberating high-purity hydrogen by microwave-promoted catalytic dehydrogenation of liquid alkanes using Fe and Ni particles supported on silicon carbide. A H 2 production selectivity from all evolved gases of some 98 %, is achieved with less than a fraction of a percent of adventitious CO and CO 2 . The major co-product is solid, elemental carbon. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Microgravity Investigation of Cement Solidification
NASA Technical Reports Server (NTRS)
Neves, Juliana; Radlinska, Aleksandra; Scheetz, Barry
2017-01-01
Concrete is the most widely used man-made material in the world, second only to water. The large-scale production of cements contributes to approximately 5% anthropogenic CO2 emission. Microgravity research can lead to more durable and hence more cost-effective material.
Short run effects of a price on carbon dioxide emissions from U.S. electric generators.
Newcomer, Adam; Blumsack, Seth A; Apt, Jay; Lave, Lester B; Morgan, M Granger
2008-05-01
The price of delivered electricity will rise if generators have to pay for carbon dioxide emissions through an implicit or explicit mechanism. There are two main effects that a substantial price on CO2 emissions would have in the short run (before the generation fleet changes significantly). First, consumers would react to increased price by buying less, described by their price elasticity of demand. Second, a price on CO2 emissions would change the order in which existing generators are economically dispatched, depending on their carbon dioxide emissions and marginal fuel prices. Both the price increase and dispatch changes depend on the mix of generation technologies and fuels in the region available for dispatch, although the consumer response to higher prices is the dominant effect. We estimate that the instantaneous imposition of a price of $35 per metric ton on CO2 emissions would lead to a 10% reduction in CO2 emissions in PJM and MISO at a price elasticity of -0.1. Reductions in ERCOT would be about one-third as large. Thus, a price on CO2 emissions that has been shown in earlier workto stimulate investment in new generation technology also provides significant CO2 reductions before new technology is deployed at large scale.
Song, Ah Young; Choi, Ha Young; Lee, Eun Song; Han, Jaejoon; Min, Sea C
2018-04-01
Films containing microencapsulated cinnamon oil (CO) were developed using a large-scale production system to protect against the Indian meal moth (Plodia interpunctella). CO at concentrations of 0%, 0.8%, or 1.7% (w/w ink mixture) was microencapsulated with polyvinyl alcohol. The microencapsulated CO emulsion was mixed with ink (47% or 59%, w/w) and thinner (20% or 25%, w/w) and coated on polypropylene (PP) films. The PP film was then laminated with a low-density polyethylene (LDPE) film on the coated side. The film with microencapsulated CO at 1.7% repelled P. interpunctella most effectively. Microencapsulation did not negatively affect insect repelling activity. The release rate of cinnamaldehyde, an active repellent, was lower when CO was microencapsulated than that in the absence of microencapsulation. Thermogravimetric analysis exhibited that microencapsulation prevented the volatilization of CO. The tensile strength, percentage elongation at break, elastic modulus, and water vapor permeability of the films indicated that microencapsulation did not affect the tensile and moisture barrier properties (P > 0.05). The results of this study suggest that effective films for the prevention of Indian meal moth invasion can be produced by the microencapsulation of CO using a large-scale film production system. Low-density polyethylene-laminated polypropylene films printed with ink incorporating microencapsulated cinnamon oil using a large-scale film production system effectively repelled Indian meal moth larvae. Without altering the tensile and moisture barrier properties of the film, microencapsulation resulted in the release of an active repellent for extended periods with a high thermal stability of cinnamon oil, enabling commercial film production at high temperatures. This anti-insect film system may have applications to other food-packaging films that use the same ink-printing platform. © 2018 Institute of Food Technologists®.
CNTs grown on nanoporous carbon from zeolitic imidazolate frameworks for supercapacitors.
Kim, Jeonghun; Young, Christine; Lee, Jaewoo; Park, Min-Sik; Shahabuddin, Mohammed; Yamauchi, Yusuke; Kim, Jung Ho
2016-10-27
Carbon nanotubes (CNT) grown on nanoporous carbon (NPC), which yields coexisting amorphous and graphitic nanoarchitectures, have been prepared on a large scale from zeolitic imidazolate framework (ZIF) by introducing bimetallic ions (Co 2+ and Zn 2+ ). Interestingly, the hybrid Co/Zn-ZIF-derived NPC showed rich graphitic CNTs on the surface. This NPC was utilized for a coin-type supercapacitor cell with an aqueous electrolyte, which showed enhanced retention at high current density and good stability over 10 000 cycles.
Edmunds, Peter J; Burgess, Scott C
2016-12-15
Body size has large effects on organism physiology, but these effects remain poorly understood in modular animals with complex morphologies. Using two trials of a ∼24 day experiment conducted in 2014 and 2015, we tested the hypothesis that colony size of the coral Pocillopora verrucosa affects the response of calcification, aerobic respiration and gross photosynthesis to temperature (∼26.5 and ∼29.7°C) and P CO 2 (∼40 and ∼1000 µatm). Large corals calcified more than small corals, but at a slower size-specific rate; area-normalized calcification declined with size. Whole-colony and area-normalized calcification were unaffected by temperature, P CO 2 , or the interaction between the two. Whole-colony respiration increased with colony size, but the slopes of these relationships differed between treatments. Area-normalized gross photosynthesis declined with colony size, but whole-colony photosynthesis was unaffected by P CO 2 , and showed a weak response to temperature. When scaled up to predict the response of large corals, area-normalized metrics of physiological performance measured using small corals provide inaccurate estimates of the physiological performance of large colonies. Together, these results demonstrate the importance of colony size in modulating the response of branching corals to elevated temperature and high P CO 2 . © 2016. Published by The Company of Biologists Ltd.
Winnick, Matthew J.; Maher, Kate
2018-01-27
Recent studies have suggested that thermodynamic limitations on chemical weathering rates exert a first-order control on riverine solute fluxes and by extension, global chemical weathering rates. As such, these limitations may play a prominent role in the regulation of carbon dioxide levels (pCO 2) over geologic timescales by constraining the maximum global weathering flux. In this study, we develop a theoretical scaling relationship between equilibrium solute concentrations and pCO 2 based on equilibrium constants and reaction stoichiometry relating primary mineral dissolution and secondary mineral precipitation. Here, we test this theoretical scaling relationship against reactive transport simulations of chemical weathering profilesmore » under open-and closed-system conditions, representing partially and fully water-saturated regolith, respectively. Under open-system conditions, equilibrium bicarbonate concentrations vary as a power-law function of pCO 2(y =kx n)where nis dependent on reaction stoichiometry and kis dependent on both reaction stoichiometry and the equilibrium constant. Under closed-system conditions, bicarbonate concentrations vary linearly with pCO 2 at low values and approach open-system scaling at high pCO 2. To describe the potential role of thermodynamic limitations in the global silicate weathering feedback, we develop a new mathematical framework to assess weathering feedback strength in terms of both (1) steady-state atmospheric pCO 2 concentrations, and (2) susceptibility to secular changes in degassing rates and transient carbon cycle perturbations, which we term 1st and 2nd order feedback strength, respectively. Finally, we discuss the implications of these results for the effects of vascular land plant evolution on feedback strength, the potential role of vegetation in controlling modern solute fluxes, and the application of these frameworks to a more complete functional description of the silicate weathering feedback. Most notably, the dependence of equilibrium solute concentrations on pCO 2 may represent a direct weathering feedback largely independent of climate and modulated by belowground organic carbon respiration.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Winnick, Matthew J.; Maher, Kate
Recent studies have suggested that thermodynamic limitations on chemical weathering rates exert a first-order control on riverine solute fluxes and by extension, global chemical weathering rates. As such, these limitations may play a prominent role in the regulation of carbon dioxide levels (pCO 2) over geologic timescales by constraining the maximum global weathering flux. In this study, we develop a theoretical scaling relationship between equilibrium solute concentrations and pCO 2 based on equilibrium constants and reaction stoichiometry relating primary mineral dissolution and secondary mineral precipitation. Here, we test this theoretical scaling relationship against reactive transport simulations of chemical weathering profilesmore » under open-and closed-system conditions, representing partially and fully water-saturated regolith, respectively. Under open-system conditions, equilibrium bicarbonate concentrations vary as a power-law function of pCO 2(y =kx n)where nis dependent on reaction stoichiometry and kis dependent on both reaction stoichiometry and the equilibrium constant. Under closed-system conditions, bicarbonate concentrations vary linearly with pCO 2 at low values and approach open-system scaling at high pCO 2. To describe the potential role of thermodynamic limitations in the global silicate weathering feedback, we develop a new mathematical framework to assess weathering feedback strength in terms of both (1) steady-state atmospheric pCO 2 concentrations, and (2) susceptibility to secular changes in degassing rates and transient carbon cycle perturbations, which we term 1st and 2nd order feedback strength, respectively. Finally, we discuss the implications of these results for the effects of vascular land plant evolution on feedback strength, the potential role of vegetation in controlling modern solute fluxes, and the application of these frameworks to a more complete functional description of the silicate weathering feedback. Most notably, the dependence of equilibrium solute concentrations on pCO 2 may represent a direct weathering feedback largely independent of climate and modulated by belowground organic carbon respiration.« less
NASA Astrophysics Data System (ADS)
Winnick, Matthew J.; Maher, Kate
2018-03-01
Recent studies have suggested that thermodynamic limitations on chemical weathering rates exert a first-order control on riverine solute fluxes and by extension, global chemical weathering rates. As such, these limitations may play a prominent role in the regulation of carbon dioxide levels (pCO2) over geologic timescales by constraining the maximum global weathering flux. In this study, we develop a theoretical scaling relationship between equilibrium solute concentrations and pCO2 based on equilibrium constants and reaction stoichiometry relating primary mineral dissolution and secondary mineral precipitation. We test this theoretical scaling relationship against reactive transport simulations of chemical weathering profiles under open- and closed-system conditions, representing partially and fully water-saturated regolith, respectively. Under open-system conditions, equilibrium bicarbonate concentrations vary as a power-law function of pCO2 (y = kxn) where n is dependent on reaction stoichiometry and k is dependent on both reaction stoichiometry and the equilibrium constant. Under closed-system conditions, bicarbonate concentrations vary linearly with pCO2 at low values and approach open-system scaling at high pCO2. To describe the potential role of thermodynamic limitations in the global silicate weathering feedback, we develop a new mathematical framework to assess weathering feedback strength in terms of both (1) steady-state atmospheric pCO2 concentrations, and (2) susceptibility to secular changes in degassing rates and transient carbon cycle perturbations, which we term 1st and 2nd order feedback strength, respectively. Finally, we discuss the implications of these results for the effects of vascular land plant evolution on feedback strength, the potential role of vegetation in controlling modern solute fluxes, and the application of these frameworks to a more complete functional description of the silicate weathering feedback. Most notably, the dependence of equilibrium solute concentrations on pCO2 may represent a direct weathering feedback largely independent of climate and modulated by belowground organic carbon respiration.
NASA Astrophysics Data System (ADS)
Jansson, Anna; Lischka, Silke; Boxhammer, Tim; Schulz, Kai G.; Norkko, Joanna
2016-06-01
Anthropogenic carbon dioxide (CO2) emissions are causing severe changes in the global inorganic carbon balance of the oceans. Associated ocean acidification is expected to pose a major threat to marine ecosystems worldwide, and it is also expected to be amplified in the Baltic Sea where the system is already exposed to relatively large natural seasonal and diel pH fluctuations. We studied the responses of larvae of the benthic key species Macoma balthica to a range of future CO2 scenarios using six ˜ 55 m3 mesocosms encompassing the entire pelagic community. The mesocosms were deployed in the northern Baltic Sea in June 2012. We focused on the survival, growth and subsequent settlement process of Macoma balthica when exposed to different levels of future CO2. The size and time to settlement of M. balthica increased along the CO2 gradient, suggesting a developmental delay. With ongoing climate change, both the frequency and extent of regularly occurring high CO2 conditions are likely to increase, and a permanent pH decrease will likely occur. The strong impact of increasing CO2 levels on early-stage bivalves is alarming as these stages are crucial for sustaining viable populations, and a failure in their recruitment would ultimately lead to negative effects on the population.
Modeling and optimal design of CO2 Direct Air Capture systems in large arrays
NASA Astrophysics Data System (ADS)
Sadri Irani, Samaneh; Luzzatto-Fegiz, Paolo
2017-11-01
As noted by the 2014 IPCC report, while the rise in atmospheric CO2 would be slowed by emissions reductions, removing atmospheric CO2 is an important part of possible paths to climate stabilization. Direct Air Capture of CO2 with chemicals (DAC) is one of several proposed carbon capture technologies. There is an ongoing debate on whether DAC is an economically viable approach to alleviate climate change. In addition, like all air capture strategies, DAC is strongly constrained by the net-carbon problem, namely the need to control CO2 emissions associated with the capture process (for example, if DAC not powered by renewables). Research to date has focused on the chemistry and economics of individual DAC devices. However, the fluid mechanics of their large-scale deployment has not been examined in the literature, to the best of our knowledge. In this presentation, we develop a model for flow through an array of DAC devices, varying their lateral extent and their separation. We build on a recent theory of canopy flows, introducing terms for CO2 entrainment into the array boundary layer, and transport into the farm. In addition, we examine the possibility of driving flow passively by wind, thereby reducing energy consumption. The optimal operational design is established considering the total cost, drag force, energy consumption and total CO2 capture.
The Role of Optimality in Characterizing CO2 Seepage from Geological Carbon Sequestration Sites
NASA Astrophysics Data System (ADS)
Cortis, A.; Oldenburg, C. M.; Benson, S. M.
2007-12-01
Storage of large amounts of carbon dioxide (CO2) in deep geological formations for greenhouse-gas mitigation is gaining momentum and moving from its conceptual and testing stages towards widespread application. In this talk we explore various optimization strategies for characterizing surface leakage (seepage) using near-surface measurement approaches such as accumulation chambers and eddy covariance towers. Seepage characterization objectives and limitations need to be defined carefully from the outset especially in light of large natural background variations that can mask seepage. The cost and sensitivity of seepage detection are related to four critical length scales pertaining to the size of the: (1) region that needs to be monitored; (2) footprint of the measurement approach; (3) main seepage zone; and (4) region in which concentrations or fluxes are influenced by seepage. Seepage characterization objectives may include one or all of the tasks of detecting, locating, and quantifying seepage. Each of these tasks has its own optimal strategy. Detecting and locating seepage in a region in which there is no expected or preferred location for seepage nor existing evidence for seepage requires monitoring on a fixed grid, e.g., using eddy covariance towers. The fixed-grid approaches needed to detect seepage are expected to require large numbers of eddy covariance towers for large-scale geologic CO2 storage. Once seepage has been detected and roughly located, seepage zones and features can be optimally pinpointed through a dynamic search strategy, e.g., employing accumulation chambers and/or soil-gas sampling. Quantification of seepage rates can be done through measurements on a localized fixed grid once the seepage is pinpointed. Background measurements are essential for seepage detection in natural ecosystems. Artificial neural networks are considered as regression models useful for distinguishing natural system behavior from anomalous behavior suggestive of CO2 seepage without need for detailed understanding of natural system processes. Because of the local extrema in CO2 fluxes and concentrations in natural systems, simple steepest-descent algorithms are not effective and evolutionary computation algorithms are proposed as a paradigm for dynamic monitoring networks to pinpoint CO2 seepage areas. This work was carried out within the ZERT project, funded by the Assistant Secretary for Fossil Energy, Office of Sequestration, Hydrogen, and Clean Coal Fuels, National Energy Technology Laboratory, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.
Geng, Yan; Wang, Yonghui; Yang, Kuo; Wang, Shaopeng; Zeng, Hui; Baumann, Frank; Kuehn, Peter; Scholten, Thomas; He, Jin-Sheng
2012-01-01
The Tibetan Plateau is an essential area to study the potential feedback effects of soils to climate change due to the rapid rise in its air temperature in the past several decades and the large amounts of soil organic carbon (SOC) stocks, particularly in the permafrost. Yet it is one of the most under-investigated regions in soil respiration (Rs) studies. Here, Rs rates were measured at 42 sites in alpine grasslands (including alpine steppes and meadows) along a transect across the Tibetan Plateau during the peak growing season of 2006 and 2007 in order to test whether: (1) belowground biomass (BGB) is most closely related to spatial variation in Rs due to high root biomass density, and (2) soil temperature significantly influences spatial pattern of Rs owing to metabolic limitation from the low temperature in cold, high-altitude ecosystems. The average daily mean Rs of the alpine grasslands at peak growing season was 3.92 µmol CO2 m−2 s−1, ranging from 0.39 to 12.88 µmol CO2 m−2 s−1, with average daily mean Rs of 2.01 and 5.49 µmol CO2 m−2 s−1 for steppes and meadows, respectively. By regression tree analysis, BGB, aboveground biomass (AGB), SOC, soil moisture (SM), and vegetation type were selected out of 15 variables examined, as the factors influencing large-scale variation in Rs. With a structural equation modelling approach, we found only BGB and SM had direct effects on Rs, while other factors indirectly affecting Rs through BGB or SM. Most (80%) of the variation in Rs could be attributed to the difference in BGB among sites. BGB and SM together accounted for the majority (82%) of spatial patterns of Rs. Our results only support the first hypothesis, suggesting that models incorporating BGB and SM can improve Rs estimation at regional scale. PMID:22509373
DOE Office of Scientific and Technical Information (OSTI.GOV)
Raz-Yaseef, Naama; Torn, Margaret S.; Wu, Yuxin
The few prethaw observations of tundra carbon fluxes suggest that there may be large spring releases, but little Is lmown about the scale and underlying mechanisms of this phenomenon. To address these questions, we combined ecosystem eddy flux measurements from two towers near Barrow, Alaska, with mechanistic soil-core thawing experiment During a 2week period prior to snowmelt In 2014, large fluxes were measured, reducing net summer uptake of CO2 by 46% and adding 6% to cumulative CH4 emissions. Emission pulses were linked to unique rain-on-snow events enhancing soli cracking. Controlled laboratory experiment revealed that as surface Ice thaws, an immediate,more » large pulse of trapped gases Is emitted. These results suggest that the Arctic C02 and CH4 spring pulse is a delayed release of biogenic gas production from the previous fall and that the pulse can be large enough to offset a significant fraction of the moderate Arctic tundra carbon sink.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Krishnamurthy, Krish R.
Post-combustion CO 2 capture (PCC) technology offers flexibility to treat the flue gas from both existing and new coal-fired power plants and can be applied to treat all or a portion of the flue gas. Solvent-based technologies are today the leading option for PCC from commercial coal-fired power plants as they have been applied in large-scale in other applications. Linde and BASF have been working together to develop and further improve a PCC process incorporating BASF’s novel aqueous amine-based solvent technology. This technology offers significant benefits compared to other solvent-based processes as it aims to reduce the regeneration energy requirementsmore » using novel solvents that are very stable under the coal-fired power plant feed gas conditions. BASF has developed the desired solvent based on the evaluation of a large number of candidates. In addition, long-term small pilot-scale testing of the BASF solvent has been performed on a lignite-fired flue gas. In coordination with BASF, Linde has evaluated a number of options for capital cost reduction in large engineered systems for solvent-based PCC technology. This report provides a summary of the work performed and results from a project supported by the US DOE (DE-FE0007453) for the pilot-scale demonstration of a Linde-BASF PCC technology using coal-fired power plant flue gas at a 1-1.5 MWe scale in Wilsonville, AL at the National Carbon Capture Center (NCCC). Following a project kick-off meeting in November 2011 and the conclusion of pilot plant design and engineering in February 2013, mechanical completion of the pilot plant was achieved in July 2014, and final commissioning activities were completed to enable start-up of operations in January 2015. Parametric tests were performed from January to December 2015 to determine optimal test conditions and evaluate process performance over a variety of operation parameters. A long-duration 1500-hour continuous test campaign was performed from May to August 2016 at a selected process condition to evaluate process performance and solvent stability over a longer period similar to how the process would operate as a continuously running large-scale PCC plant. The pilot plant integrated a number of unique features of the Linde-BASF technology aimed at lowering overall energy consumption and capital costs. During the overall test period including startup, parametric testing and long-duration testing, the pilot plant was operated for a total of 6,764 hours out of which testing with flue gas was performed for 4,109 hours. The pilot plant testing demonstrated all of the performance targets including CO 2 capture rate exceeding 90%, CO 2 purity exceeding 99.9 mol% (dry), flue gas processing capacity up to 15,500 lbs/hr (equivalent to 1.5 MWe capacity slipstream), regeneration energy as low as 2.7 GJ/tonne CO 2, and regenerator operating pressure up to 3.4 bara. Excellent solvent stability performance data was measured and verified by Linde and BASF during both test campaigns. In addition to process data, significant operational learnings were gained from pilot tests that will contribute greatly to the commercial success of PCC. Based on a thorough techno-economic assessment (TEA) of the Linde-BASF PCC process integrated with a 550 MWe supercritical coal-fired power plant, the net efficiency of the integrated power plant with CO 2 capture is increased from 28.4% with the DOE/NETL Case 12 reference to 30.9% with the Linde-BASF PCC plant previously presented utilizing the BASF OASE® blue solvent [Ref. 4], and is further increased to 31.4% using a Linde-BASF PCC plant with BASF OASE® blue solvent and an advanced stripper interstage heater (SIH) configuration. The Linde-BASF PCC plant incorporating the BASF OASE® blue solvent also results in significantly lower overall capital costs, thereby reducing the cost of electricity (COE) and cost of CO 2 captured from $147.25/MWh and $56.49/MT CO 2, respectively, for the reference DOE/NETL Case 12 plant, to $128.49/MWh and $41.85/MT CO2 for process case LB1, respectively, and $126.65/MWh and $40.66/MT CO 2 for process case SIH, respectively. With additional innovative Linde-BASF PCC process configuration improvements, the COE and cost of CO 2 captured can be further reduced to $125.51/MWh and $39.90/MT CO 2 for a further optimized PCC process defined as LB1-CREB. Most notably, the Linde-BASF process options assessed have already demonstrated the potential to lower the cost of CO 2 captured below the DOE target of $40/MT CO 2 at the 550 MWe scale for second generation PCC technologies. Project organization, structure, goals, tasks, accomplishments, process criteria and milestones will be presented in this report along with highlights and key results from parametric and long-duration testing of the Linde-BASF PCC pilot. The parametric and long-duration testing campaigns were aimed at validating the performance of the PCC technology against targets determined from a preliminary techno-economic assessment. The stability of the solvent with extended operation in a realistic power plant setting was measured with performance verified. Additionally, general solvent classification information, process operating conditions, normalized solvent performance data, solvent stability test results, flue gas conditions data, CO 2 purity data in the gaseous product stream, steam requirements and process flow diagrams, and updated process economic data for a scaled-up 550 MWe supercritical power plant with CO 2 capture are presented and discussed in this report.« less
Pure dipolar-interacted CoFe{sub 2}O{sub 4} nanoparticles and their magnetic properties
DOE Office of Scientific and Technical Information (OSTI.GOV)
Xu, Shi-tao; School of Physics and Electronic Information, Huaibei Normal University, Huaibei 235000; Ma, Yong-qing, E-mail: yqma@ahu.edu.cn
2015-02-15
Graphical abstract: The mono-dispersed CoFe{sub 2}O{sub 4} nanoparticles with the uniform size of 10.5 ± 2 nm were first synthesized and then they were embedded in amorphous SiO{sub 2} matrix with different CoFe{sub 2}O{sub 4} nanoparticles’ concentrations. The large coercivity (3056 Oe) and the remanence ratio (0.63) were obtained by suitably diluting CoFe{sub 2}O{sub 4} nanoparticles into the SiO{sub 2} matrix. The reciprocal of the absolute maximum of δm and the M{sub r}/M{sub s} ratio behave in the same trend (as shown in (e)), indicating that the M{sub r}/M{sub s} ratio was dominated by the interparticle dipolar interaction. The presentmore » work is meaningful for revealing the underlying mechanism in nano-scaled magnetic system and improving the magnetic performance. - Highlights: • The mono-dispersed CoFe{sub 2}O{sub 4} nanoparticles with the uniform size of 10.5 ± 2 nm were synthesized by the thermal decomposition of metals acetylacetonates in solvents with high boiling point. • The large coercivity (3056 Oe) and the remanence ratio (0.63) were obtained by diluting CoFe{sub 2}O{sub 4} nanoparticles into the SiO{sub 2} matrix with a suitable concentration. • The surface anisotropy and interparticle dipolar interaction affect the magnetic performance and magnetic ordering state. • It was observed that the M{sub r}/M{sub s} ratio was dominated by the interparticle dipolar interaction. - Abstract: The mono-dispersed and uniform CoFe{sub 2}O{sub 4} nanoparticles were synthesized by the thermal decomposition of Fe(acac){sub 3} and Co(acac){sub 2}. Then the CoFe{sub 2}O{sub 4} nanoparticles were diluted in amorphous SiO{sub 2} matrix with different CoFe{sub 2}O{sub 4} nanoparticles’ concentrations. All samples show the positive or negative exchange bias behavior, indicating the presence of canted spin layer at the CoFe{sub 2}O{sub 4} nanoparticles’ surface. The large effective anisotropy constant (3.38 × 10{sup 6} erg/cm{sup 3}) was observed, which can be attributed to the induced surface anisotropy by the canted surface spins. The reduced magnetization (M{sub r}/M{sub s}) was dominated by the interparticle dipolar interaction while the coercivity (H{sub c}) was determined by the synergistic effects of the surface anisotropy, interparticle dipolar interaction and interface effect. By suitably diluting CoFe{sub 2}O{sub 4} in the SiO{sub 2} matrix, the high H{sub c} (3056 Oe) and the M{sub r}/M{sub s} (0.63) can be obtained, which is larger than most of those reported before. The present work is meaningful for revealing the underlying mechanism in nano-scaled magnetic system and improving the magnetic performance.« less
Large CO2 and CH4 release from a flooded formerly drained fen
NASA Astrophysics Data System (ADS)
Sachs, T.; Franz, D.; Koebsch, F.; Larmanou, E.; Augustin, J.
2016-12-01
Drained peatlands are usually strong carbon dioxide (CO2) sources. In Germany, up to 4.5 % of the national CO2 emissions are estimated to be released from agriculturally used peatlands and for some peatland-rich northern states, such as Mecklenburg-Western Pomerania, this share increases to about 20%. Reducing this CO2 source and restoring the peatlands' natural carbon sink is one objective of large-scale nature protection and restoration measures, in which 37.000 ha of drained and degraded peatlands in Mecklenburg-Western Pomerania are slated for rewetting. It is well known, however, that in the initial phase of rewetting, a reduction of the CO2 source strength is usually accompanied by an increase in CH4 emissions. Thus, whether and when the intended effects of rewetting with regard to greenhouse gases are achieved, depends on the balance of CO2 and CH4 fluxes and on the duration of the initial CH4 emission phase. In 2013, a new Fluxnet site went online at a flooded formerly drained river valley fen site near Zarnekow, NE Germany (DE-Zrk), to investigate the combined CO2 and CH4 dynamics at such a heavily degraded and rewetted peatland. The site is dominated by open water with submerged and floating vegetation and surrounding Typha latifolia.Nine year after rewetting, we found large CH4 emissions of 53 g CH4 m-2 a-1 from the open water area, which are 4-fold higher than from the surrounding vegetation zone (13 g CH4 m-2 a-1). Surprisingly, both the open water and the vegetated area were net CO2 sources of 158 and 750 g CO2 m-2 a-1, respectively. Unusual meteorological conditions with a warm and dry summer and a mild winter might have facilitated high respiration rates, particularly from temporally non-inundated organic mud in the vegetation zone.
NASA Astrophysics Data System (ADS)
Plampin, Michael R.; Porter, Mark L.; Pawar, Rajesh J.; Illangasekare, Tissa H.
2017-12-01
To assess the risks of Geologic Carbon Sequestration (GCS), it is crucial to understand the fundamental physicochemical processes that may occur if and when stored CO2 leaks upward from a deep storage reservoir into the shallow subsurface. Intermediate-scale experiments allow for improved understanding of the multiphase evolution processes that control CO2 migration behavior in the subsurface, because the boundary conditions, initial conditions, and porous media parameters can be better controlled and monitored in the laboratory than in field settings. For this study, a large experimental test bed was designed to mimic a cross section of a shallow aquifer with layered geologic heterogeneity. As water with aqueous CO2 was injected into the system to mimic a CO2-charged water leakage scenario, the spatiotemporal evolution of the multiphase CO2 plume was monitored. Similar experiments were performed with two different sand combinations to assess the relative effects of different types of geologic facies transitions on the CO2 evolution processes. Significant CO2 attenuation was observed in both scenarios, but by fundamentally different mechanisms. When the porous media layers had very different permeabilities, attenuation was caused by local accumulation (structural trapping) and slow redissolution of gas phase CO2. When the permeability difference between the layers was relatively small, on the other hand, gas phase continually evolved over widespread areas near the leading edge of the aqueous plume, which also attenuated CO2 migration. This improved process understanding will aid in the development of models that could be used for effective risk assessment and monitoring programs for GCS projects.
Plampin, Michael R.; Porter, Mark L.; Pawar, Rajesh J.; ...
2017-11-15
In order to assess the risks of Geologic Carbon Sequestration (GCS), it is crucial to understand the fundamental physicochemical processes that may occur if and when stored CO 2 leaks upward from a deep storage reservoir into the shallow subsurface. Intermediate-scale experiments allow for improved understanding of the multiphase evolution processes that control CO 2 migration behaviour in the subsurface, because the boundary conditions, initial conditions, and porous media parameters can be better controlled and monitored in the laboratory than in field settings. For this study, a large experimental test bed was designed to mimic a cross-section of a shallowmore » aquifer with layered geologic heterogeneity. As water with aqueous CO 2 was injected into the system to mimic a CO 2-charged water leakage scenario, the spatiotemporal evolution of the multiphase CO 2 plume was monitored. Similar experiments were performed with two different sand combinations to assess the relative effects of different types of geologic facies transitions on the CO 2 evolution processes. Significant CO 2 attenuation was observed in both scenarios, but by fundamentally different mechanisms. When the porous media layers had very different permeabilities, attenuation was caused by local accumulation (structural trapping) and slow re-dissolution of gas phase CO 2. When the permeability difference between the layers was relatively small, on the other hand, gas phase continually evolved over widespread areas near the leading edge of the aqueous plume, which also attenuated CO 2 migration. In conclusion, this improved process understanding will aid in the development of models that could be used for effective risk assessment and monitoring programs for GCS projects.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Plampin, Michael R.; Porter, Mark L.; Pawar, Rajesh J.
In order to assess the risks of Geologic Carbon Sequestration (GCS), it is crucial to understand the fundamental physicochemical processes that may occur if and when stored CO 2 leaks upward from a deep storage reservoir into the shallow subsurface. Intermediate-scale experiments allow for improved understanding of the multiphase evolution processes that control CO 2 migration behaviour in the subsurface, because the boundary conditions, initial conditions, and porous media parameters can be better controlled and monitored in the laboratory than in field settings. For this study, a large experimental test bed was designed to mimic a cross-section of a shallowmore » aquifer with layered geologic heterogeneity. As water with aqueous CO 2 was injected into the system to mimic a CO 2-charged water leakage scenario, the spatiotemporal evolution of the multiphase CO 2 plume was monitored. Similar experiments were performed with two different sand combinations to assess the relative effects of different types of geologic facies transitions on the CO 2 evolution processes. Significant CO 2 attenuation was observed in both scenarios, but by fundamentally different mechanisms. When the porous media layers had very different permeabilities, attenuation was caused by local accumulation (structural trapping) and slow re-dissolution of gas phase CO 2. When the permeability difference between the layers was relatively small, on the other hand, gas phase continually evolved over widespread areas near the leading edge of the aqueous plume, which also attenuated CO 2 migration. In conclusion, this improved process understanding will aid in the development of models that could be used for effective risk assessment and monitoring programs for GCS projects.« less
NASA Astrophysics Data System (ADS)
Burger, Magdalena; Berger, Sina; Spangenberg, Ines; Blodau, Christian
2016-06-01
Ponds smaller than 10 000 m2 likely account for about one-third of the global lake perimeter. The release of methane (CH4) and carbon dioxide (CO2) from these ponds is often high and significant on the landscape scale. We measured CO2 and CH4 fluxes in a temperate peatland in southern Ontario, Canada, in summer 2014 along a transect from the open water of a small pond (847 m2) towards the surrounding floating mat (5993 m2) and in a peatland reference area. We used a high-frequency closed chamber technique and distinguished between diffusive and ebullitive CH4 fluxes. CH4 fluxes and CH4 bubble frequency increased from a median of 0.14 (0.00 to 0.43) mmol m-2 h-1 and 4 events m-2 h-1 on the open water to a median of 0.80 (0.20 to 14.97) mmol m-2 h-1 and 168 events m-2 h-1 on the floating mat. The mat was a summer hot spot of CH4 emissions. Fluxes were 1 order of magnitude higher than at an adjacent peatland site. During daytime the pond was a net source of CO2 equivalents to the atmosphere amounting to 0.13 (-0.02 to 1.06) g CO2 equivalents m-2 h-1, whereas the adjacent peatland site acted as a sink of -0.78 (-1.54 to 0.29) g CO2 equivalents m-2 h-1. The photosynthetic CO2 uptake on the floating mat did not counterbalance the high CH4 emissions, which turned the floating mat into a strong net source of 0.21 (-0.11 to 2.12) g CO2 equivalents m-2 h-1. This study highlights the large small-scale variability of CH4 fluxes and CH4 bubble frequency at the peatland-pond interface and the importance of the often large ecotone areas surrounding small ponds as a source of greenhouse gases to the atmosphere.
NASA Astrophysics Data System (ADS)
Blodau, Christian; Burger, Magdalena; Berger, Sina; Spangenberg, Ines
2016-04-01
Ponds smaller than 10000 m2 likely account for about one third of the global lake perimeter. The release of methane (CH4) and carbon dioxide (CO2) from these ponds is often high and significant on the landscape scale. We measured CO2 and CH4 fluxes in a temperate peatland in southern Ontario, Canada, in summer 2014 along a transect from the open water of a small pond (847 m2) towards the surrounding floating mat (5993 m2) and in a peatland reference area. We used a high-frequency closed chamber technique and distinguished between diffusive and ebullitive CH4 fluxes. CH4 fluxes and CH4 bubble frequency increased from a median of 0.14 (0.00 to 0.43) mmol m-2 h-1 and 4 events m-2 h-1 on the open water to a median of 0.80 (0.20 to 14.97) mmol m-2 h-1 and 168 events m-2 h-1 on the floating mat. The mat was a summer hot spot of CH4 emissions. Fluxes were one order of magnitude higher than at an adjacent peatland site. During daytime the pond was a net source of CO2 equivalents to the atmosphere amounting to 0.13 (-0.02 to 1.06) g CO2 equivalents m-2 h-1, whereas the adjacent peatland site acted as a sink of -0.78 (-1.54 to 0.29) g CO2 equivalents m-2 h-1. The photosynthetic CO2 uptake on the floating mat did not counterbalance the high CH4 emissions, which turned the floating mat into a strong net source of 0.21 (-0.11 to 2.12) g CO2 equivalents m-2 h-1. This study highlights the large small-scale variability of CH4 fluxes and CH4 bubble frequency at the peatland-pond interface and the importance of the often large ecotone areas surrounding small ponds as a source of greenhouse gases to the atmosphere.
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.
ALMA IMAGING OF THE CO (6-5) LINE EMISSION IN NGC 7130
DOE Office of Scientific and Technical Information (OSTI.GOV)
Zhao, Yinghe; Lu, Nanyao; Xu, C. Kevin
2016-04-01
In this paper, we report our high-resolution (0.″20 × 0.″14 or ∼70 × 49 pc) observations of the CO(6-5) line emission, which probes warm and dense molecular gas, and the 434 μm dust continuum in the nuclear region of NGC 7130, obtained with the Atacama Large Millimeter Array (ALMA). The CO line and dust continuum fluxes detected in our ALMA observations are 1230 ± 74 Jy km s{sup −1} and 814 ± 52 mJy, respectively, which account for 100% and 51% of their total fluxes. We find that the CO(6-5) and dust emissions are generally spatially correlated, but their brightest peaks show an offset of ∼70 pc, suggestingmore » that the gas and dust emissions may start decoupling at this physical scale. The brightest peak of the CO(6-5) emission does not spatially correspond to the radio continuum peak, which is likely dominated by an active galactic nucleus (AGN). This, together with our additional quantitative analysis, suggests that the heating contribution of the AGN to the CO(6-5) emission in NGC 7130 is negligible. The CO(6-5) and the extinction-corrected Pa-α maps display striking differences, suggestive of either a breakdown of the correlation between warm dense gas and star formation at linear scales of <100 pc or a large uncertainty in our extinction correction to the observed Pa-α image. Over a larger scale of ∼2.1 kpc, the double-lobed structure found in the CO(6-5) emission agrees well with the dust lanes in the optical/near-infrared images.« less
Rupert Seidl; Thomas A. Spies; Werner Rammer; E. Ashley Steel; Robert J. Pabst; Keith. Olsen
2012-01-01
Forest ecosystems are the most important terrestrial carbon (C) storage globally, and presently mitigate anthropogenic climate change by acting as a large and persistent sink for atmospheric CO2. Yet, forest C density varies greatly in space, both globally and at stand and landscape levels. Understanding the multi-scale drivers of this variation...
Natalie A. Griffiths; Paul J. Hanson; Daniel M. Ricciuto; Colleen M. Iversen; Anna M. Jensen; Avni Malhotra; Karis J. McFarlane; Richard J. Norby; Khachik Sargsyan; Stephen D. Sebestyen; Xiaoying Shi; Anthony P. Walker; Eric J. Ward; Jeffrey M. Warren; David J. Weston
2017-01-01
We are conducting a large-scale, long-term climate change response experiment in an ombrotrophic peat bog in Minnesota to evaluate the effects of warming and elevated CO2 on ecosystem processes using empirical and modeling approaches. To better frame future assessments of peatland responses to climate change, we characterized and compared spatial...
NASA Astrophysics Data System (ADS)
LaForce, T.; Ennis-King, J.; Paterson, L.
2013-12-01
Residual CO2 saturation is a critically important parameter in CO2 storage as it can have a large impact on the available secure storage volume and post-injection CO2 migration. A suite of single-well tests to measure residual trapping was conducted at the Otway test site in Victoria, Australia during 2011. One or more of these tests could be conducted at a prospective CO2 storage site before large-scale injection. The test involved injection of 150 tonnes of pure carbon dioxide followed by 454 tonnes of CO2-saturated formation water to drive the carbon dioxide to residual saturation. This work presents a brief overview of the full test sequence, followed by the analysis and interpretation of the tests using noble gas tracers. Prior to CO2 injection krypton (Kr) and xenon (Xe) tracers were injected and back-produced to characterise the aquifer under single-phase conditions. After CO2 had been driven to residual the two tracers were injected and produced again. The noble gases act as non-partitioning aqueous-phase tracers in the undisturbed aquifer and as partitioning tracers in the presence of residual CO2. To estimate residual saturation from the tracer test data a one-dimensional radial model of the near-well region is used. In the model there are only two independent parameters: the apparent dispersivity of each tracer and the residual CO2 saturation. Independent analysis of the Kr and Xe tracer production curves gives the same estimate of residual saturation to within the accuracy of the method. Furthermore the residual from the noble gas tracer tests is consistent with other measurements in the sequence of tests.
Lindenmaier, Rodica; Dubey, Manvendra K.; Henderson, Bradley G.; Butterfield, Zachary T.; Herman, Jay R.; Rahn, Thom; Lee, Sang-Hyun
2014-01-01
There is a pressing need to verify air pollutant and greenhouse gas emissions from anthropogenic fossil energy sources to enforce current and future regulations. We demonstrate the feasibility of using simultaneous remote sensing observations of column abundances of CO2, CO, and NO2 to inform and verify emission inventories. We report, to our knowledge, the first ever simultaneous column enhancements in CO2 (3–10 ppm) and NO2 (1–3 Dobson Units), and evidence of δ13CO2 depletion in an urban region with two large coal-fired power plants with distinct scrubbing technologies that have resulted in ∆NOx/∆CO2 emission ratios that differ by a factor of two. Ground-based total atmospheric column trace gas abundances change synchronously and correlate well with simultaneous in situ point measurements during plume interceptions. Emission ratios of ∆NOx/∆CO2 and ∆SO2/∆CO2 derived from in situ atmospheric observations agree with those reported by in-stack monitors. Forward simulations using in-stack emissions agree with remote column CO2 and NO2 plume observations after fine scale adjustments. Both observed and simulated column ∆NO2/∆CO2 ratios indicate that a large fraction (70–75%) of the region is polluted. We demonstrate that the column emission ratios of ∆NO2/∆CO2 can resolve changes from day-to-day variation in sources with distinct emission factors (clean and dirty power plants, urban, and fires). We apportion these sources by using NO2, SO2, and CO as signatures. Our high-frequency remote sensing observations of CO2 and coemitted pollutants offer promise for the verification of power plant emission factors and abatement technologies from ground and space. PMID:24843169
NASA Astrophysics Data System (ADS)
Lu, Hai-Sheng; Zhang, Haimin; Liu, Rongrong; Zhang, Xian; Zhao, Huijun; Wang, Guozhong
2017-01-01
Metal-organic frameworks (MOFs) materials have aroused great research interest in different areas owing to their unique properties, such as high surface area, various composition, well-organized framework and controllable porous structure. Controllable fabrication of MOFs materials at macro-scale may be more promising for their large-scale practical applications. Here we report the synthesis of macro-scale Co-MOFs crystals using 1,3,5-benzenetricarboxylic acid (H3BTC) linker in the presence of Co2+, triethylamine (TEA) and nonanoic acid by a facile solvothermal reaction. Further, the as-fabricated Co-MOFs as precursor was pyrolytically treated at different temperatures in N2 atmosphere to obtain metallic Co nanoparticles embedded in N-doped porous carbon layers (denoted as Co@NPC). The results demonstrate that the Co-MOFs derived sample obtained at 900 °C (Co@NPC-900) shows a porous structure (including micropore and mesopore) with a surface area of 110.8 m2 g-1 and an N doping level of 1.62 at.% resulted from TEA in the pyrolysis process. As electrocatalyst, the Co@NPC-900 exhibits bifunctional electrocatalytic activities toward the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in alkaline media which are key reactions in some renewable energy technologies such as fuel cells and rechargeable metal-air batteries. The results indicate that the Co@NPC-900 can afford an onset potential of 1.50 V (vs. RHE) and a potential value of 1.61 V (vs. RHE) at a current density of 10 mA cm-2 for ORR and OER with high applicable stability, respectively. The efficient catalytic activity of Co@NPC-900 as bifunctional oxygen electrocatalyst can be ascribed to N doping and embedded metallic Co nanoparticles in carbon structure providing catalytic active sites and porous structure favourable for electrocatalysis-related mass transport.
Large Scale Cross Drive Correlation Of Digital Media
2016-03-01
NAVAL POSTGRADUATE SCHOOL MONTEREY, CALIFORNIA THESIS LARGE SCALE CROSS-DRIVE CORRELATION OF DIGITAL MEDIA by Joseph Van Bruaene March 2016 Thesis Co...CROSS-DRIVE CORRELATION OF DIGITAL MEDIA 5. FUNDING NUMBERS 6. AUTHOR(S) Joseph Van Bruaene 7. PERFORMING ORGANIZATION NAME(S) AND ADDRESS(ES) Naval...the ability to make large scale cross-drive correlations among a large corpus of digital media becomes increasingly important. We propose a
Year-round CH4 and CO2 flux dynamics in two contrasting freshwater ecosystems of the subarctic
NASA Astrophysics Data System (ADS)
Jammet, Mathilde; Dengel, Sigrid; Kettner, Ernesto; Parmentier, Frans-Jan W.; Wik, Martin; Crill, Patrick; Friborg, Thomas
2017-11-01
Lakes and wetlands, common ecosystems of the high northern latitudes, exchange large amounts of the climate-forcing gases methane (CH4) and carbon dioxide (CO2) with the atmosphere. The magnitudes of these fluxes and the processes driving them are still uncertain, particularly for subarctic and Arctic lakes where direct measurements of CH4 and CO2 emissions are often of low temporal resolution and are rarely sustained throughout the entire year. Using the eddy covariance method, we measured surface-atmosphere exchange of CH4 and CO2 during 2.5 years in a thawed fen and a shallow lake of a subarctic peatland complex. Gas exchange at the fen exhibited the expected seasonality of a subarctic wetland with maximum CH4 emissions and CO2 uptake in summer, as well as low but continuous emissions of CH4 and CO2 throughout the snow-covered winter. The seasonality of lake fluxes differed, with maximum CO2 and CH4 flux rates recorded at spring thaw. During the ice-free seasons, we could identify surface CH4 emissions as mostly ebullition events with a seasonal trend in the magnitude of the release, while a net CO2 flux indicated photosynthetic activity. We found correlations between surface CH4 emissions and surface sediment temperature, as well as between diel CO2 uptake and diel solar input. During spring, the breakdown of thermal stratification following ice thaw triggered the degassing of both CH4 and CO2. This spring burst was observed in 2 consecutive years for both gases, with a large inter-annual variability in the magnitude of the CH4 degassing. On the annual scale, spring emissions converted the lake from a small CO2 sink to a CO2 source: 80 % of total annual carbon emissions from the lake were emitted as CO2. The annual total carbon exchange per unit area was highest at the fen, which was an annual sink of carbon with respect to the atmosphere. Continuous respiration during the winter partly counteracted the fen summer sink by accounting for, as both CH4 and CO2, 33 % of annual carbon exchange. Our study shows (1) the importance of overturn periods (spring or fall) for the annual CH4 and CO2 emissions of northern lakes, (2) the significance of lakes as atmospheric carbon sources in subarctic landscapes while fens can be a strong carbon sink, and (3) the potential for ecosystem-scale eddy covariance measurements to improve the understanding of short-term processes driving lake-atmosphere exchange of CH4 and CO2.
Using carbon dioxide in fisheries and aquatic invasive species management
Treanor, Hilary B.; Ray, Andrew M.; Layhee, Megan J.; Watten, Barnaby J.; Gross, Jason A.; Gresswell, Robert E.; Webb, Molly A. H.
2017-01-01
To restore native fish populations, fisheries programs often depend on active removal of aquatic invasive species. Chemical removal can be an effective method of eliminating aquatic invasive species, but chemicals can induce mortality in nontarget organisms and persist in the environment. Carbon dioxide (CO2) is an emerging alternative to traditional chemical control agents because it has been demonstrated to be toxic to fish, but is naturally occurring and readily neutralized. In addition, CO2 is a commercially available gas, is highly soluble, and has high absorption efficiency. When these characteristics are paired with advances in modern, large-scale gas delivery technologies, opportunities to use CO2 in natural or artificial (e.g., canals) waters to manage fish become increasingly feasible. Our objective is to describe the history of CO2 use in fisheries and outline potential future applications of CO2 to suppress and manipulate aquatic species in field and aquaculture settings.
NASA Astrophysics Data System (ADS)
Schicks, Judith; Heeschen, Katja; Spangenberg, Erik; Luzi-Helbing, Manja; Beeskow-Strauch, Bettina; Priegnitz, Mike; Giese, Ronny; Abendroth, Sven; Thaler, Jan
2017-04-01
Natural gas hydrates occur at all active and passive continental margins, in permafrost regions, and deep lakes. Since they are supposed to contain enormous amounts of methane, gas hydrates are discussed as an energy resource. For the production of gas from hydrate bearing sediments, three different production methods were tested during the last decade: depressurization, thermal and chemical stimulation as well as combinations of these methods. In the framework of the SUGAR project we developed a Large Scale Reservoir Simulator (LARS) with a total volume of 425L to test these three methods in a pilot plant scale. For this purpose we formed hydrate from methane saturated brine in sediments under conditions close to natural gas hydrate deposits. The obtained hydrate saturations varied between 40-90%. Hydrate saturation and distribution were determined using electrical resistivity tomography (ERT). The volumes of the produced gas and water were determined and the gas phase was analyzed via gas chromatography. Multi-step depressurization, thermal stimulation applying in-situ combustion as well as chemical stimulation via the injection of CO2 and a CO2-N2-mixture were tested. Depressurization and thermal stimulation appear to be less complicated compared to the chemical stimulation. For the understanding of the macroscopically observed processes on a molecular level, we also performed experiments on a smaller scale using microscopic observation, Raman spectroscopy and X-ray diffraction. The results of these experiments are of particular importance for the understanding of the processes occurring during the CO2-CH4 swapping. Under the chosen experimental conditions the observations indicate a (partial) decomposition and reformation of the hydrate structure rather than a diffusion-controlled exchange of the molecules.
Fingerprinting captured CO2 using natural tracers: Determining CO2 fate and proving ownership
NASA Astrophysics Data System (ADS)
Flude, Stephanie; Gilfillan, Stuart; Johnston, Gareth; Stuart, Finlay; Haszeldine, Stuart
2016-04-01
In the long term, captured CO2 will most likely be stored in large saline formations and it is highly likely that CO2 from multiple operators will be injected into a single saline formation. Understanding CO2 behavior within the reservoir is vital for making operational decisions and often uses geochemical techniques. Furthermore, in the event of a CO2 leak, being able to identify the owner of the CO2 is of vital importance in terms of liability and remediation. Addition of geochemical tracers to the CO2 stream is an effective way of tagging the CO2 from different power stations, but may become prohibitively expensive at large scale storage sites. Here we present results from a project assessing whether the natural isotopic composition (C, O and noble gas isotopes) of captured CO2 is sufficient to distinguish CO2 captured using different technologies and from different fuel sources, from likely baseline conditions. Results include analytical measurements of CO2 captured from a number of different CO2 capture plants and a comprehensive literature review of the known and hypothetical isotopic compositions of captured CO2 and baseline conditions. Key findings from the literature review suggest that the carbon isotope composition will be most strongly controlled by that of the feedstock, but significant fractionation is possible during the capture process; oxygen isotopes are likely to be controlled by the isotopic composition of any water used in either the industrial process or the capture technology; and noble gases concentrations will likely be controlled by the capture technique employed. Preliminary analytical results are in agreement with these predictions. Comparison with summaries of likely storage reservoir baseline and shallow or surface leakage reservoir baseline data suggests that C-isotopes are likely to be valuable tracers of CO2 in the storage reservoir, while noble gases may be particularly valuable as tracers of potential leakage.
, multi-scale observing systems under challenging field conditions to document unexpectedly large soil CO2 pleased to recognize the Building Technology and Urban Systems Division's Retro-commissioning Sensor synthetic biology while providing novel approaches for crop engineering to support Berkeley Lab and DOE's
DOE Office of Scientific and Technical Information (OSTI.GOV)
Cordiner, M. A.; Milam, S. N.; Mumma, M. J.
2014-09-01
Results are presented from the first cometary observations using the Atacama Large Millimeter/Submillimeter Array (ALMA), including measurements of the spatially resolved distributions of HCN, HNC, H{sub 2}CO, and dust within the comae of two comets: C/2012 F6 (Lemmon) and C/2012 S1 (ISON), observed at heliocentric distances of 1.5 AU and 0.54 AU, respectively. These observations (with angular resolution ≈0.''5), reveal an unprecedented level of detail in the distributions of these fundamental cometary molecules, and demonstrate the power of ALMA for quantitative measurements of the distributions of molecules and dust in the inner comae of typical bright comets. In both comets, HCN ismore » found to originate from (or within a few hundred kilometers of) the nucleus, with a spatial distribution largely consistent with spherically symmetric, uniform outflow. By contrast, the HNC distributions are clumpy and asymmetrical, with peaks at cometocentric radii ∼500-1000 km, consistent with release of HNC in collimated outflow(s). Compared to HCN, the H{sub 2}CO distribution in comet Lemmon is very extended. The interferometric visibility amplitudes are consistent with coma production of H{sub 2}CO and HNC from unidentified precursor material(s) in both comets. Adopting a Haser model, the H{sub 2}CO parent scale length is found to be a few thousand kilometers in Lemmon and only a few hundred kilometers in ISON, consistent with the destruction of the precursor by photolysis or thermal degradation at a rate that scales in proportion to the solar radiation flux.« less
NiMg/Ceria-Zirconia Cylindrical Pellet Catalysts for Tri-reforming of Surrogate Biogas
Zhao, Xianhui; Walker, Devin; Maiti, Debtanu; ...
2017-12-22
Cylindrical NiMg/Ce 0.6Zr 0.4O 2 pellet catalysts with two different sizes (large: radius = 1.59 mm; and small: radius = 0.75 mm) were produced by extrusion of powder catalysts. The small catalyst pellets had a higher specific surface area, pore volume, average pore size, radial crush strength, and resistance to breakage than the large ones. Tri-reforming tests with surrogate biogas were conducted at 3 bar and 882 °C, with the feed molar ratios of CH 4: CO 2: air fixed at 1.0: 0.7: 0.95 and the H 2O/CH 4 molar feed ratio (0.35 – 1.16) varied. The small catalyst pelletsmore » exhibited lower internal mass transfer resistance and higher coking resistance, compared to the large ones. CO 2 conversion decreased and H 2/CO molar ratio increased with the increase of H 2O/CH 4 molar feed ratio, which are consistent with the trends predicted by thermodynamic equilibrium calculations. Finally, the results indicate that the NiMg/Ce 0.6Zr 0.4O 2 catalyst pellets are promising for commercial scale applications.« less
Component-specific dynamics of riverine mangrove CO2 efflux in the Florida coastal Everglades
Troxler, Tiffany G.; Barr, Jordan G.; Fuentes, Jose D.; Engel, Victor C.; Anderson, Gordon H.; Sanchez, Christopher; Lagomosino, David; Price, Rene; Davis, Stephen E.
2015-01-01
Carbon cycling in mangrove forests represents a significant portion of the coastal wetland carbon (C) budget across the latitudes of the tropics and subtropics. Previous research suggests fluctuations in tidal inundation, temperature and salinity can influence forest metabolism and C cycling. Carbon dioxide (CO2) from respiration that occurs from below the canopy is contributed from different components. In this study, we investigated variation in CO2 flux among different below-canopy components (soil, leaf litter, course woody debris, soil including pneumatophores, prop roots, and surface water) in a riverine mangrove forest of Shark River Slough estuary, Everglades National Park (Florida, USA). The range in CO2 flux from different components exceeded that measured among sites along the oligohaline-saline gradient. Black mangrove (Avicennia germinans) pneumatophores contributed the largest average CO2 flux. Over a narrow range of estuarine salinity (25–35 practical salinity units (PSU)), increased salinity resulted in lower CO2 flux to the atmosphere. Tidal inundation reduced soil CO2 flux overall but increased the partial pressure of CO2 (pCO2) observed in the overlying surface water upon flooding. Higher pCO2 in surface water is then subject to tidally driven export, largely as HCO3. Integration and scaling of CO2 flux rates to forest scale allowed for improved understanding of the relative contribution of different below-canopy components to mangrove forest ecosystem respiration (ER). Summing component CO2fluxes suggests a more significant contribution of below-canopy respiration to ER than previously considered. An understanding of below-canopy CO2 component fluxes and their contributions to ER can help to elucidate how C cycling will change with discrete disturbance events (e.g., hurricanes) and long-term change, including sea-level rise, and potential impact mangrove forests. As such, key controls on below-canopy ER must be taken into consideration when developing and modeling mangrove forest C budgets.
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.
Biogeologic Carbon Sequestration - a Cost-Effective Proposal
NASA Astrophysics Data System (ADS)
Shaw, G. H.; Kuhns, R.
2009-05-01
Carbon sequestration has been proposed as a strategy for reducing the impact of carbon dioxide emissions from burning of fossil fuels. There are two main routes: 1) capture CO2 emissions from power plants or other large point sources followed by some form of "burial/sequestration", and 2) extraction of CO2 from the ambient atmosphere (involving substantial concentration relative to atmospheric levels) also followed by burial/sequestration. In either case the goal is to achieve significant long-term isolation of CO2 at an economically sustainable price, perhaps measured by some "market price" for CO2, such as the European carbon futures market, where the price is now (2/3/09) about 14-15/tonne of CO2. The second approach, removal of CO2 from the atmosphere, has the potential benefit of reversing the previous buildup of atmospheric CO2, and perhaps even providing a means to "adjust" terrestrial climate by regulating atmospheric CO2 concentrations. For the present, ideas of planetary "geo-engineering" are not as popular as reducing the impact of continued CO2 emissions. In fact, the energy and capital costs of extraction from a dilute atmosphere appear to make this approach uneconomical. Proposals to fertilize the open ocean suffer from concerns about long term ecosystem effects, to say nothing of a lack of verifiability. There is, however, an approach using biological systems that can not only extract significant amounts of CO2, but can do so cost-effectively. Lakes are known in which primary productivity approaches or exceeds 1gm C/cm2-yr. This equates to removal of 35,000 tonnes of CO2 per km2 per year, with a "market value" of about 500,000/yr. Such productivity only occurs under highly eutrophic conditions, and presumably requires significant nutrient additions. As such it would be unthinkable to pursue this technique on a large scale in extant lakes. If, however, it is possible to produce one or more large artificial lakes under acceptable conditions it is conceivable that this approach to carbon sequestration could prove invaluable in both the near and long term.
New Approaches to Quantifying Transport Model Error in Atmospheric CO2 Simulations
NASA Technical Reports Server (NTRS)
Ott, L.; Pawson, S.; Zhu, Z.; Nielsen, J. E.; Collatz, G. J.; Gregg, W. W.
2012-01-01
In recent years, much progress has been made in observing CO2 distributions from space. However, the use of these observations to infer source/sink distributions in inversion studies continues to be complicated by difficulty in quantifying atmospheric transport model errors. We will present results from several different experiments designed to quantify different aspects of transport error using the Goddard Earth Observing System, Version 5 (GEOS-5) Atmospheric General Circulation Model (AGCM). In the first set of experiments, an ensemble of simulations is constructed using perturbations to parameters in the model s moist physics and turbulence parameterizations that control sub-grid scale transport of trace gases. Analysis of the ensemble spread and scales of temporal and spatial variability among the simulations allows insight into how parameterized, small-scale transport processes influence simulated CO2 distributions. In the second set of experiments, atmospheric tracers representing model error are constructed using observation minus analysis statistics from NASA's Modern-Era Retrospective Analysis for Research and Applications (MERRA). The goal of these simulations is to understand how errors in large scale dynamics are distributed, and how they propagate in space and time, affecting trace gas distributions. These simulations will also be compared to results from NASA's Carbon Monitoring System Flux Pilot Project that quantified the impact of uncertainty in satellite constrained CO2 flux estimates on atmospheric mixing ratios to assess the major factors governing uncertainty in global and regional trace gas distributions.
Carbon dioxide and methane emissions from the scale model of open dairy lots.
Ding, Luyu; Cao, Wei; Shi, Zhengxiang; Li, Baoming; Wang, Chaoyuan; Zhang, Guoqiang; Kristensen, Simon
2016-07-01
To investigate the impacts of major factors on carbon loss via gaseous emissions, carbon dioxide (CO2) and methane (CH4) emissions from the ground of open dairy lots were tested by a scale model experiment at various air temperatures (15, 25, and 35 °C), surface velocities (0.4, 0.7, 1.0, and 1.2 m sec(-1)), and floor types (unpaved soil floor and brick-paved floor) in controlled laboratory conditions using the wind tunnel method. Generally, CO2 and CH4 emissions were significantly enhanced with the increase of air temperature and velocity (P < 0.05). Floor type had different effects on the CO2 and CH4 emissions, which were also affected by air temperature and soil characteristics of the floor. Although different patterns were observed on CH4 emission from the soil and brick floors at different air temperature-velocity combinations, statistical analysis showed no significant difference in CH4 emissions from different floors (P > 0.05). For CO2, similar emissions were found from the soil and brick floors at 15 and 25 °C, whereas higher rates were detected from the brick floor at 35 °C (P < 0.05). Results showed that CH4 emission from the scale model was exponentially related to CO2 flux, which might be helpful in CH4 emission estimation from manure management. Gaseous emissions from the open lots are largely dependent on outdoor climate, floor systems, and management practices, which are quite different from those indoors. This study assessed the effects of floor types and air velocities on CO2 and CH4 emissions from the open dairy lots at various temperatures by a wind tunnel. It provided some valuable information for decision-making and further studies on gaseous emissions from open lots.
NASA Astrophysics Data System (ADS)
Liu, Xia; Guo, Yuedong; Hu, Haiqing; Sun, Chengkun; Zhao, Xikuan; Wei, Changlei
2015-12-01
To quantify the fluxes and examine the controls on greenhouse gas emissions from the permafrost marshes where the fate of the large quantity of soil organic carbon remains poorly understood, we measured carbon dioxide (CO2) and methane (CH4) emissions in the northern region of the Great Xing'an Mountains, northeast China, in the thawing seasons of 2011 and 2012. The mean CO2 and CH4 fluxes from the marshes were estimated at 403.47 and 0.14 mg m-2 h-1 on average during the two years. Soil temperature was determined as the primary control on the seasonal greenhouse gas emissions during the growing period. The Q10 values, calculated from the exponential regression between soil temperature and CO2 emissions, suggest that the sensitivity of CO2 flux to climate warming has a high spatially variability in the study area. Absorption of atmospheric CH4 was seasonally detected at the sites with lower water table, which confirms the potential of the natural marshes as CH4 sink when water table goes down due to climate change. When viewed from the ecosystem scale, the mean annual water table level and aboveground primary production were deemed as the dominant influencing factors for the mean annual fluxes, which suggests that there were different controls on the gas emissions at different spatial scales. Therefore, the primary controls of the CO2 and CH4 emissions at different spatial scales need to be surveyed in more detail when focusing on the future alteration of greenhouse gas emissions from permafrost marshes due to climate warming.
THE CO-TO-H{sub 2} CONVERSION FACTOR AND DUST-TO-GAS RATIO ON KILOPARSEC SCALES IN NEARBY GALAXIES
DOE Office of Scientific and Technical Information (OSTI.GOV)
Sandstrom, K. M.; Walter, F.; Leroy, A. K.
2013-11-01
We present ∼kiloparsec spatial resolution maps of the CO-to-H{sub 2} conversion factor (α{sub CO}) and dust-to-gas ratio (DGR) in 26 nearby, star-forming galaxies. We have simultaneously solved for α{sub CO} and the DGR by assuming that the DGR is approximately constant on kiloparsec scales. With this assumption, we can combine maps of dust mass surface density, CO-integrated intensity, and H I column density to solve for both α{sub CO} and the DGR with no assumptions about their value or dependence on metallicity or other parameters. Such a study has just become possible with the availability of high-resolution far-IR maps frommore » the Herschel key program KINGFISH, {sup 12}CO J = (2-1) maps from the IRAM 30 m large program HERACLES, and H I 21 cm line maps from THINGS. We use a fixed ratio between the (2-1) and (1-0) lines to present our α{sub CO} results on the more typically used {sup 12}CO J = (1-0) scale and show using literature measurements that variations in the line ratio do not affect our results. In total, we derive 782 individual solutions for α{sub CO} and the DGR. On average, α{sub CO} = 3.1 M{sub ☉} pc{sup –2} (K km s{sup –1}){sup –1} for our sample with a standard deviation of 0.3 dex. Within galaxies, we observe a generally flat profile of α{sub CO} as a function of galactocentric radius. However, most galaxies exhibit a lower α{sub CO} value in the central kiloparsec—a factor of ∼2 below the galaxy mean, on average. In some cases, the central α{sub CO} value can be factors of 5-10 below the standard Milky Way (MW) value of α{sub CO,{sub MW}} = 4.4 M{sub ☉} pc{sup –2} (K km s{sup –1}){sup –1}. While for α{sub CO} we find only weak correlations with metallicity, the DGR is well-correlated with metallicity, with an approximately linear slope. Finally, we present several recommendations for choosing an appropriate α{sub CO} for studies of nearby galaxies.« less
Boreal forests and atmosphere - Biosphere exchange of carbon dioxide
NASA Technical Reports Server (NTRS)
D'Arrigo, Rosanne; Jacoby, Gordon C.; Fung, Inez Y.
1987-01-01
Two approaches to investigating the role of boreal forests in the global carbon cycle are presented. First, a tracer support model which incorporates the normalized-difference vegetation index obtained from advanced, very high resolution radiometer radiances was used to simulate the annual cycle of CO2 in the atmosphere. Results indicate that the seasonal growth of the combined boreal forests of North America and Eurasia accounts for about 50 percent of the mean seasonal CO2 amplitude recorded at Pt. Barrow, Alaska and about 30 percent of the more globally representative CO2 signal at Mauna Loa, Hawaii. Second, tree-ring width data from four boreal treeline sites in northern Canada were positively correlated with Pt. Barrow CO2 drawdown for the period 1971-1982. These results suggest that large-scale changes in the growth of boreal forests may be contributing to the observed increasing trend in CO2 amplitude. They further suggest that tree-ring data may be applicable as indices for CO2 uptake and remote sensing estimates of photosynthetic activity.
Interaction of SO2 and CO with the Ti2O3(101¯2) surface
NASA Astrophysics Data System (ADS)
Smith, Kevin E.; Henrich, Victor E.
1985-10-01
The interaction of sulfur dioxide with the nearly perfect (101¯2) surface of the corundum transition-metal oxide Ti2O3 has been studied using ultraviolet and x-ray photoemission spectroscopies and low-energy electron diffraction. The reaction of SO2 with Ti2O3 is found to be extremely vigorous, with SO2 adsorbing dissociatively and catalyzing the complete oxidation of the surface to TiO2 and TiS2. This result is significant since exposure to large amounts of O2 does not result in the production of large amounts of TiO2 at the Ti2O3 surface. Dissociative adsorption of SO2 continues for exposures up to at least 104 L (1 L=10-6Torr sec). The reaction is accompanied by large scale surface disorder and by an increase in the work function of 1.32 eV. In contrast, CO adsorbs molecularly for exposures >=105 L, with an extramolecular relaxation-polarization shift of 3.0 eV. For CO exposures <=104 L, the chemisorption mechanism is tentatively identified as dissociative adsorption at defect sites. Inclusive of this study, the interaction of four oxygen-containing molecules (SO2, CO, H2O, and O2) with Ti2O3(101¯2) surfaces has been studied, and their behavior is compared and trends isolated with a view to understanding the oxidation of Ti2O3.
Sandrini, Giovanni; Cunsolo, Serena; Schuurmans, J. Merijn; Matthijs, Hans C. P.; Huisman, Jef
2015-01-01
Rising CO2 concentrations may have large effects on aquatic microorganisms. In this study, we investigated how elevated pCO2 affects the harmful freshwater cyanobacterium Microcystis aeruginosa. This species is capable of producing dense blooms and hepatotoxins called microcystins. Strain PCC 7806 was cultured in chemostats that were shifted from low to high pCO2 conditions. This resulted in a transition from a C-limited to a light-limited steady state, with a ~2.7-fold increase of the cyanobacterial biomass and ~2.5-fold more microcystin per cell. Cells increased their chlorophyll a and phycocyanin content, and raised their PSI/PSII ratio at high pCO2. Surprisingly, cells had a lower dry weight and contained less carbohydrates, which might be an adaptation to improve the buoyancy of Microcystis when light becomes more limiting at high pCO2. Only 234 of the 4691 genes responded to elevated pCO2. For instance, expression of the carboxysome, RuBisCO, photosystem and C metabolism genes did not change significantly, and only a few N assimilation genes were expressed differently. The lack of large-scale changes in the transcriptome could suit a buoyant species that lives in eutrophic lakes with strong CO2 fluctuations very well. However, we found major responses in inorganic carbon uptake. At low pCO2, cells were mainly dependent on bicarbonate uptake, whereas at high pCO2 gene expression of the bicarbonate uptake systems was down-regulated and cells shifted to CO2 and low-affinity bicarbonate uptake. These results show that the need for high-affinity bicarbonate uptake systems ceases at elevated CO2. Moreover, the combination of an increased cyanobacterial abundance, improved buoyancy, and higher toxin content per cell indicates that rising atmospheric CO2 levels may increase the problems associated with the harmful cyanobacterium Microcystis in eutrophic lakes. PMID:25999931
NASA Astrophysics Data System (ADS)
Lydersen, Ida; Sopher, Daniel; Juhlin, Christopher
2015-04-01
Geological storage of CO2 is one of the available options to reduce CO2-emissions from large point sources. Previous work in the Baltic Sea Basin has inferred a large storage potential in several stratigraphic units. The most promising of these is the Faludden sandstone, exhibiting favorable reservoir properties and forming a regional stratigraphic trap. A potential location for a pilot CO2 injection site, to explore the suitability of the Faludden reservoir is onshore Gotland, Sweden. In this study onshore and offshore data have been digitized and interpreted, along with well data, to provide a detailed characterization of the Faludden reservoir below parts of Gotland. Maps and regional seismic profiles describing the extent and top structure of the Faludden sandstone are presented. The study area covers large parts of the island of Gotland, and extends about 50-70km offshore. The seismic data presented is part of a larger dataset acquired by Oljeprospektering AB (OPAB) between 1970 and 1990. The dataset is to this date largely unpublished, therefore re-processing and interpretation of these data provide improved insight into the subsurface of the study area. Two longer seismic profiles crossing Gotland ENE-WSW have been interpreted to give a large scale, regional control of the Faludden sandstone. A relatively tight grid of land seismic following the extent of the Faludden sandstone along the eastern coast to the southernmost point has been interpreted to better understand the actual distribution and geometry of the Faludden sandstone beneath Gotland. The maps from this study help to identify the most suitable area for a potential test injection site for CO2-storage, and to further the geological understanding of the area in general.
Buscheck, Thomas A.; Bielicki, Jeffrey M.; Edmunds, Thomas A.; ...
2016-05-05
We present an approach that uses the huge fluid and thermal storage capacity of the subsurface, together with geologic carbon dioxide (CO 2) storage, to harvest, store, and dispatch energy from subsurface (geothermal) and surface (solar, nuclear, fossil) thermal resources, as well as excess energy on electric grids. Captured CO 2 is injected into saline aquifers to store pressure, generate artesian flow of brine, and provide a supplemental working fluid for efficient heat extraction and power conversion. Concentric rings of injection and production wells create a hydraulic mound to store pressure, CO 2, and thermal energy. This energy storage canmore » take excess power from the grid and excess/waste thermal energy, and dispatch that energy when it is demanded and thus enable higher penetration of variable renewable energy technologies (e.g., wind, solar). CO 2 stored in the subsurface functions as a cushion gas to provide enormous pressure-storage capacity and displace large quantities of brine, some of which can be treated for a variety of beneficial uses. Geothermal power and energy-storage applications may generate enough revenues to compensate for CO 2 capture costs. While our approach can use nitrogen (N 2), in addition to CO 2, as a supplemental fluid, and store thermal energy, this study focuses using CO 2 for geothermal energy production and grid-scale energy storage. We conduct a techno-economic assessment to determine the levelized cost of electricity of using this approach to generate geothermal power. We present a reservoir pressure-management strategy that diverts a small portion of the produced brine for beneficial consumptive use to reduce the pumping cost of fluid recirculation, while reducing the risk of seismicity, caprock fracture, and CO 2 leakage.« less
NASA Astrophysics Data System (ADS)
Kohanpur, A. H.; Chen, Y.; Valocchi, A. J.; Tudek, J.; Crandall, D.
2016-12-01
CO2-brine flow in deep natural rocks is the focus of attention in geological storage of CO2. Understanding rock/flow properties at pore-scale is a vital component in field-scale modeling and prediction of fate of injected CO2. There are many challenges in working at the pore scale, such as size and selection of representative elementary volume (REV), particularly for material with complex geometry and heterogeneity, and the high computational costs. These issues factor into trade-offs that need to be made in choosing and applying pore-scale models. On one hand, pore-network modeling (PNM) simplifies the geometry and flow equations but can provide characteristic curves on fairly large samples. On the other hand, the lattice Boltzmann method (LBM) solves Navier-Stokes equations on the real geometry but is limited to small samples due to its high computational costs. Thus, both methods have some advantages but also face some challenges, which warrants a more detailed comparison and evaluation. In this study, we used industrial and micro-CT scans of actual reservoir rock samples to characterize pore structure at different resolutions. We ran LBM models directly on the characterized geometry and PNM on the equivalent 3D extracted network to determine single/two-phase flow properties during drainage and imbibition processes. Specifically, connectivity, absolute permeability, relative permeability curve, capillary pressure curve, and interface location are compared between models. We also did simulations on several subsamples from different locations including different domain sizes and orientations to encompass analysis of heterogeneity and isotropy. This work is primarily supported as part of the Center for Geologic Storage of CO2, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science and partially supported by the International Institute for Carbon-Neutral Energy Research (WPI-I2CNER) based at Kyushu University, Japan.
Campeau, Audrey; Del Giorgio, Paul A
2014-04-01
It is now widely accepted that boreal rivers and streams are regionally significant sources of carbon dioxide (CO2), yet their role as methane (CH4) emitters, as well as the sensitivity of these greenhouse gas (GHG) emissions to climate change, are still largely undefined. In this study, we explore the large-scale patterns of fluvial CO2 and CH4 partial pressure (pCO2 , pCH4) and gas exchange (k) relative to a set of key, climate-sensitive river variables across 46 streams and rivers in two distinct boreal landscapes of Northern Québec. We use the resulting models to determine the direction and magnitude of C-gas emissions from these boreal fluvial networks under scenarios of climate change. River pCO2 and pCH4 were positively correlated, although the latter was two orders of magnitude more variable. We provide evidence that in-stream metabolism strongly influences the dynamics of surface water pCO2 and pCH4 , but whereas pCO2 is not influenced by temperature in the surveyed streams and rivers, pCH4 appears to be strongly temperature-dependent. The major predictors of ambient gas concentrations and exchange were water temperature, velocity, and DOC, and the resulting models indicate that total GHG emissions (C-CO2 equivalent) from the entire network may increase between by 13 to 68% under plausible scenarios of climate change over the next 50 years. These predicted increases in fluvial GHG emissions are mostly driven by a steep increase in the contribution of CH4 (from 36 to over 50% of total CO2 -equivalents). The current role of boreal fluvial networks as major landscape sources of C is thus likely to expand, mainly driven by large increases in fluvial CH4 emissions. © 2013 John Wiley & Sons Ltd.
Leakey, Andrew D. B.; Lau, Jennifer A.
2012-01-01
Variation in atmospheric [CO2] is a prominent feature of the environmental history over which vascular plants have evolved. Periods of falling and low [CO2] in the palaeo-record appear to have created selective pressure for important adaptations in modern plants. Today, rising [CO2] is a key component of anthropogenic global environmental change that will impact plants and the ecosystem goods and services they deliver. Currently, there is limited evidence that natural plant populations have evolved in response to contemporary increases in [CO2] in ways that increase plant productivity or fitness, and no evidence for incidental breeding of crop varieties to achieve greater yield enhancement from rising [CO2]. Evolutionary responses to elevated [CO2] have been studied by applying selection in controlled environments, quantitative genetics and trait-based approaches. Findings to date suggest that adaptive changes in plant traits in response to future [CO2] will not be consistently observed across species or environments and will not be large in magnitude compared with physiological and ecological responses to future [CO2]. This lack of evidence for strong evolutionary effects of elevated [CO2] is surprising, given the large effects of elevated [CO2] on plant phenotypes. New studies under more stressful, complex environmental conditions associated with climate change may revise this view. Efforts are underway to engineer plants to: (i) overcome the limitations to photosynthesis from today's [CO2] and (ii) benefit maximally from future, greater [CO2]. Targets range in scale from manipulating the function of a single enzyme (e.g. Rubisco) to adding metabolic pathways from bacteria as well as engineering the structural and functional components necessary for C4 photosynthesis into C3 leaves. Successfully improving plant performance will depend on combining the knowledge of the evolutionary context, cellular basis and physiological integration of plant responses to varying [CO2]. PMID:22232771
Leakey, Andrew D B; Lau, Jennifer A
2012-02-19
Variation in atmospheric [CO(2)] is a prominent feature of the environmental history over which vascular plants have evolved. Periods of falling and low [CO(2)] in the palaeo-record appear to have created selective pressure for important adaptations in modern plants. Today, rising [CO(2)] is a key component of anthropogenic global environmental change that will impact plants and the ecosystem goods and services they deliver. Currently, there is limited evidence that natural plant populations have evolved in response to contemporary increases in [CO(2)] in ways that increase plant productivity or fitness, and no evidence for incidental breeding of crop varieties to achieve greater yield enhancement from rising [CO(2)]. Evolutionary responses to elevated [CO(2)] have been studied by applying selection in controlled environments, quantitative genetics and trait-based approaches. Findings to date suggest that adaptive changes in plant traits in response to future [CO(2)] will not be consistently observed across species or environments and will not be large in magnitude compared with physiological and ecological responses to future [CO(2)]. This lack of evidence for strong evolutionary effects of elevated [CO(2)] is surprising, given the large effects of elevated [CO(2)] on plant phenotypes. New studies under more stressful, complex environmental conditions associated with climate change may revise this view. Efforts are underway to engineer plants to: (i) overcome the limitations to photosynthesis from today's [CO(2)] and (ii) benefit maximally from future, greater [CO(2)]. Targets range in scale from manipulating the function of a single enzyme (e.g. Rubisco) to adding metabolic pathways from bacteria as well as engineering the structural and functional components necessary for C(4) photosynthesis into C(3) leaves. Successfully improving plant performance will depend on combining the knowledge of the evolutionary context, cellular basis and physiological integration of plant responses to varying [CO(2)].
Large- and Very-Large-Scale Motions in Katabatic Flows Over Steep Slopes
NASA Astrophysics Data System (ADS)
Giometto, M. G.; Fang, J.; Salesky, S.; Parlange, M. B.
2016-12-01
Evidence of large- and very-large-scale motions populating the boundary layer in katabatic flows over steep slopes is presented via direct numerical simulations (DNSs). DNSs are performed at a modified Reynolds number (Rem = 967), considering four sloping angles (α = 60°, 70°, 80° and 90°). Large coherent structures prove to be strongly dependent on the inclination of the underlying surface. Spectra and co-spectra consistently show signatures of large-scale motions (LSMs), with streamwise extension on the order of the boundary layer thickness. A second low-wavenumber mode characterizes pre-multiplied spectra and co-spectra when the slope angle is below 70°, indicative of very-large-scale motions (VLSMs). In addition, conditional sampling and averaging shows how LSMs and VLSMs are induced by counter-rotating roll modes, in agreement with findings from canonical wall-bounded flows. VLSMs contribute to the stream-wise velocity variance and shear stress in the above-jet regions up to 30% and 45% respectively, whereas both LSMs and VLSMs are inactive in the near-wall regions.
NASA Astrophysics Data System (ADS)
Lischka, S.; Bach, L. T.; Schulz, K.-G.; Riebesell, U.
2015-12-01
Community approaches investigating ocean acidification (OA) effects suggest a high tolerance of micro- and mesozooplankton to carbonate chemistry changes expected to occur within this century. Plankton communities in the coastal areas of the Baltic Sea frequently experience pH variations partly exceeding projections for the near future both on a diurnal and seasonal basis, thus some level of tolerance/adaptation may be expected. We conducted a large-scale mesocosm CO2 enrichment experiment (~ 55 m3) enclosing the natural plankton community in Tvärminne/Storfjärden for eight weeks during June-August 2012 and studied community and species/taxon response of microzooplankton (ciliates) and mesozooplankton to CO2 elevations expected for this century. Besides the response to fCO2 and associate changes in carbonate chemistry speciation, we also considered temperature and chlorophyll a variations in our analyses. Shannon diversity of microzooplankton significantly decreased with fCO2 and temperature with a greater dominance of smaller species. Small sized ciliates (Myrionecta rubra, Balanion comatum, Strombidium cf. epidemum, Strobilidium sp.) showed significant relations with one or more of the factors. The phototrophic Myrionecta rubra seemed to directly benefit from higher CO2 concentrations and showed increased abundance in the pre-bloom phase. With respect to meszooplankton, we neither detected significant effects for total abundance nor for Shannon diversity. The cladocera Bosmina occurred at distinctly higher abundance (more than twice as high compared to the control mesocosms) for a short time period during the second half of the experiment in three of the CO2-enriched mesocosms except for the highest CO2 level. The ratio of Bosmina with empty to embryo/resting egg bearing brood chambers, however, was significantly affected by all three factors. An indirect CO2 effect via increased food availability stimulating Bosmina reproduction is suggested, but too low sampling frequency of this highly flexible organism probably entailed proving a significant relation with fCO2. Filter-feeding cladocerans effectively transfer microbial loop carbon to higher trophic levels. Thus, under increasing OA in cladoceran dominated mesozooplankton communities the importance of the microbial loop in the pelagic zone may be enhanced and carbon transfer to higher trophic levels stimulated.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Dubey, Manvendra Krishna
Forests soak up 25% of the carbon dioxide (CO 2) emitted by anthropogenic fossil energy use (10 Gt C y -1) moderating its atmospheric accumulation. How this terrestrial CO 2 uptake will evolve with climate change in the 21st century is largely unknown. Rainforests are the most active ecosystems with the Amazon basin storing 120 Gt C as biomass and exchanging 18 Gt C y -1 of CO 2 via photosynthesis and respiration and fixing carbon at 2-3 kg C m -2 y -1. Furthermore, the intense hydrologic and carbon cycles are tightly coupled in the Amazon where about halfmore » of the water is recycled by evapotranspiration and the other half imported from the ocean by Northeasterly trade winds. Climate models predict a drying in the Amazon with reduced carbon uptake while observationally guided assessments indicate sustained uptake. We will resolve this huge discrepancy in the size and sign of the future Amazon carbon cycle by performing the first simultaneous regional scale high frequency measurements of atmospheric CO 2, H 2O, HOD, CH 4, N 2O and CO at the T3 site in Manacupuru, Brazil as part of DOE's GoAmazon project. Our data will be used to inform and develop DOE's CLM on the tropical carbon-water couplings at the appropriate grid scale (10-50km). Our measurements will also validate the CO 2 data from Japan's GOSAT and NASA's imminent OCO-2 satellite (launch date July 2014).« less
Diffusion of CO2 in Large Crystals of Cu-BTC MOF.
Tovar, Trenton M; Zhao, Junjie; Nunn, William T; Barton, Heather F; Peterson, Gregory W; Parsons, Gregory N; LeVan, M Douglas
2016-09-14
Carbon dioxide adsorption in metal-organic frameworks has been widely studied for applications in carbon capture and sequestration. A critical component that has been largely overlooked is the measurement of diffusion rates. This paper describes a new reproducible procedure to synthesize millimeter-scale Cu-BTC single crystals using concentrated reactants and an acetic acid modulator. Microscopic images, X-ray diffraction patterns, Brunauer-Emmett-Teller surface areas, and thermogravimetric analysis results all confirm the high quality of these Cu-BTC single crystals. The large crystal size aids in the accurate measurement of micropore diffusion coefficients. Concentration-swing frequency response performed at varying gas-phase concentrations gives diffusion coefficients that show very little dependence on the loading up to pressures of 0.1 bar. The measured micropore diffusion coefficient for CO2 in Cu-BTC is 1.7 × 10(-9) m(2)/s.
How can mountaintop CO 2 observations be used to constrain regional carbon fluxes?
Lin, John C.; Mallia, Derek V.; Wu, Dien; ...
2017-05-03
Despite the need for researchers to understand terrestrial biospheric carbon fluxes to account for carbon cycle feedbacks and predict future CO 2 concentrations, knowledge of these fluxes at the regional scale remains poor. This is particularly true in mountainous areas, where complex meteorology and lack of observations lead to large uncertainties in carbon fluxes. Yet mountainous regions are often where significant forest cover and biomass are found – i.e., areas that have the potential to serve as carbon sinks. As CO 2 observations are carried out in mountainous areas, it is imperative that they are properly interpreted to yield informationmore » about carbon fluxes. In this paper, we present CO 2 observations at three sites in the mountains of the western US, along with atmospheric simulations that attempt to extract information about biospheric carbon fluxes from the CO 2 observations, with emphasis on the observed and simulated diurnal cycles of CO 2. We show that atmospheric models can systematically simulate the wrong diurnal cycle and significantly misinterpret the CO 2 observations, due to erroneous atmospheric flows as a result of terrain that is misrepresented in the model. This problem depends on the selected vertical level in the model and is exacerbated as the spatial resolution is degraded, and our results indicate that a fine grid spacing of ~4 km or less may be needed to simulate a realistic diurnal cycle of CO 2 for sites on top of the steep mountains examined here in the American Rockies. In conclusion, in the absence of higher resolution models, we recommend coarse-scale models to focus on assimilating afternoon CO 2 observations on mountaintop sites over the continent to avoid misrepresentations of nocturnal transport and influence.« less
How can mountaintop CO2 observations be used to constrain regional carbon fluxes?
NASA Astrophysics Data System (ADS)
Lin, John C.; Mallia, Derek V.; Wu, Dien; Stephens, Britton B.
2017-05-01
Despite the need for researchers to understand terrestrial biospheric carbon fluxes to account for carbon cycle feedbacks and predict future CO2 concentrations, knowledge of these fluxes at the regional scale remains poor. This is particularly true in mountainous areas, where complex meteorology and lack of observations lead to large uncertainties in carbon fluxes. Yet mountainous regions are often where significant forest cover and biomass are found - i.e., areas that have the potential to serve as carbon sinks. As CO2 observations are carried out in mountainous areas, it is imperative that they are properly interpreted to yield information about carbon fluxes. In this paper, we present CO2 observations at three sites in the mountains of the western US, along with atmospheric simulations that attempt to extract information about biospheric carbon fluxes from the CO2 observations, with emphasis on the observed and simulated diurnal cycles of CO2. We show that atmospheric models can systematically simulate the wrong diurnal cycle and significantly misinterpret the CO2 observations, due to erroneous atmospheric flows as a result of terrain that is misrepresented in the model. This problem depends on the selected vertical level in the model and is exacerbated as the spatial resolution is degraded, and our results indicate that a fine grid spacing of ˜ 4 km or less may be needed to simulate a realistic diurnal cycle of CO2 for sites on top of the steep mountains examined here in the American Rockies. In the absence of higher resolution models, we recommend coarse-scale models to focus on assimilating afternoon CO2 observations on mountaintop sites over the continent to avoid misrepresentations of nocturnal transport and influence.
Massa, Charly
2017-01-01
CO2 emissions from preindustrial land-use change (LUC) are subject to large uncertainties. Although atmospheric CO2 records suggest only a small land carbon (C) source since 5,000 y before present (5 kyBP), the concurrent C sink by peat buildup could mask large early LUC emissions. Here, we combine updated continuous peat C reconstructions with the land C balance inferred from double deconvolution analyses of atmospheric CO2 and δ13C at different temporal scales to investigate the terrestrial C budget of the Holocene and the last millennium and constrain LUC emissions. LUC emissions are estimated with transient model simulations for diverging published scenarios of LU area change and shifting cultivation. Our results reveal a large terrestrial nonpeatland C source after the Mid-Holocene (66 ± 25 PgC at 7–5 kyBP and 115 ± 27 PgC at 5–3 kyBP). Despite high simulated per-capita CO2 emissions from LUC in early phases of agricultural development, humans emerge as a driver with dominant global C cycle impacts only in the most recent three millennia. Sole anthropogenic causes for particular variations in the CO2 record (∼20 ppm rise after 7 kyBP and ∼10 ppm fall between 1500 CE and 1600 CE) are not supported. This analysis puts a strong constraint on preindustrial vs. industrial-era LUC emissions and suggests that upper-end scenarios for the extent of agricultural expansion before 1850 CE are not compatible with the C budget thereafter. PMID:28137849
Matos, C; Pereira, S; Amorim, E V; Bentes, I; Briga-Sá, A
2014-09-15
Wastewater and greywater have different scales of end-uses in irrigation in Portugal. Wastewater is treated in a central wastewater treatment plant and reused in public/private large areas of irrigation, like agriculture, public gardens and golf courses. On the contrary, greywater reuse is generally applied in in situ small scales, treated and used in the same place, generally in the production site. The main aim of this paper is to compare the two types of systems: a wastewater centralized reuse system (WWCRS) and a greywater decentralized reuse system (GWDRS) in terms of water quality, energy consumption and CO2 emissions. In this paper, the main characteristics of both streams are presented and the degree of treatment required in each stream is analyzed. The advantages and disadvantages of its reuse in different scales, in terms of water quality, energy consumption and CO2 emissions are discussed. A methodology to calculate the energy consumptions and CO2 emissions related to wastewater treatment that may be applied in different cases is presented. A hypothetical example of the two systems: one referring to a WWCRS and the other to a GWDRS is presented. The energy consumption and the CO2 emissions are analyzed and compared. The WWCRS needs a higher degree of treatment and so it spends more energy and leads to more CO2 emissions to the environment than the GWDRS that consumed between 11.8 and 37.5% of the energy consumed in the WWCRS considering the same number of inhabitants served. Copyright © 2014 Elsevier B.V. All rights reserved.
Patterns of CO2 and radiocarbon across high northern latitudes during International Polar Year 2008
NASA Astrophysics Data System (ADS)
Vay, S. A.; Choi, Y.; Vadrevu, K. P.; Blake, D. R.; Tyler, S. C.; Wisthaler, A.; Hecobian, A.; Kondo, Y.; Diskin, G. S.; Sachse, G. W.; Woo, J.-H.; Weinheimer, A. J.; Burkhart, J. F.; Stohl, A.; Wennberg, P. O.
2011-07-01
High-resolution in situ CO2 measurements were conducted aboard the NASA DC-8 aircraft during the ARCTAS/POLARCAT field campaign, a component of the wider 2007-2008 International Polar Year activities. Data were recorded during large-scale surveys spanning the North American sub-Arctic to the North Pole from 0.04 to 12 km altitude in spring and summer of 2008. Influences on the observed CO2 concentrations were investigated using coincident CO, black carbon, CH3CN, HCN, O3, C2Cl4, and Δ14CO2 data, and the FLEXPART model. In spring, the CO2 spatial distribution from 55°N to 90°N was largely determined by the long-range transport of air masses laden with Asian anthropogenic pollution intermingled with Eurasian fire emissions evidenced by the greater variability in the mid-to-upper troposphere. At the receptor site, the enhancement ratios of CO2 to CO in pollution plumes ranged from 27 to 80 ppmv ppmv-1 with the highest anthropogenic content registered in plumes sampled poleward of 80°N. In summer, the CO2 signal largely reflected emissions from lightning-ignited wildfires within the boreal forests of northern Saskatchewan juxtaposed with uptake by the terrestrial biosphere. Measurements within fresh fire plumes yielded CO2 to CO emission ratios of 4 to 16 ppmv ppmv-1 and a mean CO2 emission factor of 1698 ± 280 g kg-1 dry matter. From the 14C in CO2 content of 48 whole air samples, mean spring (46.6 ± 4.4‰) and summer (51.5 ± 5‰) Δ14CO2 values indicate a 5‰ seasonal difference. Although the northern midlatitudes were identified as the emissions source regions for the majority of the spring samples, depleted Δ14CO2 values were observed in <1% of the data set. Rather, ARCTAS Δ14CO2 observations (54%) revealed predominately a pattern of positive disequilibrium (1-7‰) with respect to background regardless of season owing to both heterotrophic respiration and fire-induced combustion of biomass. Anomalously enriched Δ14CO2 values (101-262‰) measured in emissions from Lake Athabasca and Eurasian fires speak to biomass burning as an increasingly important contributor to the mass excess in Δ14CO2 observations in a warming Arctic, representing an additional source of uncertainty in the quantification of fossil fuel CO2.
Cryogenic Calcite: A Morphologic and Isotopic Analog to the ALH84001 Carbonates
NASA Technical Reports Server (NTRS)
Niles, P. B.; Leshin, L. A.; Socki, R. A.; Guan, Y.; Ming, D. W.; Gibson, E. K.
2004-01-01
Martian meteorite ALH84001 carbonates preserve large and variable microscale isotopic compositions, which in some way reflect their formation environment. These measurements show large variations (>20%) in the carbon and oxygen isotopic compositions of the carbonates on a 10-20 micron scale that are correlated with chemical composition. However, the utilization of these data sets for interpreting the formation conditions of the carbonates is complex due to lack of suitable terrestrial analogs and the difficulty of modeling under non-equilibrium conditions. Thus, the mechanisms and processes are largely unknown that create and preserve large microscale isotopic variations in carbonate minerals. Experimental tests of the possible environments and mechanisms that lead to large microscale isotopic variations can help address these concerns. One possible mechanism for creating large carbon isotopic variations in carbonates involves the freezing of water. Carbonates precipitate during extensive CO2 degassing that occurs during the freezing process as the fluid s decreasing volume drives CO2 out. This rapid CO2 degassing results in a kinetic isotopic fractionation where the CO2 gas has a much lighter isotopic composition causing an enrichment of 13C in the remaining dissolved bicarbonate. This study seeks to determine the suitability of cryogenically formed carbonates as analogs to ALH84001 carbonates. Specifically, our objective is to determine how accurately models using equilibrium fractionation factors approximate the isotopic compositions of cryogenically precipitated carbonates. This includes determining the accuracy of applying equilibrium fractionation factors during a kinetic process, and determining how isotopic variations in the fluid are preserved in microscale variations in the precipitated carbonates.
Volumetric Properties and Fluid Phase Equilibria of CO2 + H2O
DOE Office of Scientific and Technical Information (OSTI.GOV)
Capobianco, Ryan; Gruszkiewicz, Miroslaw; Wesolowski, David J
2013-01-01
The need for accurate modeling of fluid-mineral processes over wide ranges of temperature, pressure and composition highlighted considerable uncertainties of available property data and equations of state, even for the CO2 + H2O binary system. In particular, the solubility, activity, and ionic dissociation equilibrium data for the CO2-rich phase, which are essential for understanding dissolution/precipitation, fluid-matrix reactions, and solute transport, are uncertain or missing. In this paper we report the results of a new experimental study of volumetric and phase equilibrium properties of CO2 + H2O, to be followed by measurements for bulk and confined multicomponent fluid mixtures. Mixture densitiesmore » were measured by vibrating tube densimetry (VTD) over the entire composition range at T = 200 and 250 C and P = 20, 40, 60, and 80 MPa. Initial analysis of the mutual solubilities, determined from volumetric data, shows good agreement with earlier results for the aqueous phase, but finds that the data of Takenouchi and Kennedy (1964) significantly overestimated the solubility of water in supercritical CO2 (by a factor of more than two at 200 C). Resolving this well-known discrepancy will have a direct impact on the accuracy of predictive modeling of CO2 injection in geothermal reservoirs and geological carbon sequestration through improved equations of state, needed for calibration of predictive molecular-scale models and large-scale reactive transport simulations.« less
Natural analogues for CO2 storage sites - analysis of a global dataset
NASA Astrophysics Data System (ADS)
Miocic, Johannes; Gilfillan, Stuart; McDermott, Christopher; Haszeldine, R. Stuart
2013-04-01
Carbon Capture and Storage is the only industrial scale technology currently available to reduce CO2 emissions from fossil-fuelled power plants and large industrial source to the atmosphere and thus mitigate climate change. CO2 is captured at the source and transported to subsurface storage sites, such as depleted oil and gas fields or saline aquifers. In order to have an effect on emissions and to be considered safe it is crucial that the amount of CO2 leaking from storage sites to shallow aquifers or the surface remains very low (<1% over 1000 years). Some process that influence the safety of a reservoir, such as CO2-rock-brine interactions, can be studied using experiments on both laboratory and field-scale. However, long-term processes such as the development of leakage pathways can only be understood by either predictive modelling or by studying natural CO2 reservoirs as analogues for long term CO2 storage sites. Natural CO2 reservoirs have similar geological trapping mechanisms as anticipated for CO2 storage sites and often have held CO2 for a geological period of time (millions of years) without any indication for leakage. Yet, migration of CO2 from reservoirs to the surface is also common and evidenced by gas seeps such as springs and soil degassing. We have compiled and analysed a dataset comprising of more than 50 natural CO2 reservoirs from different settings all around the globe to provide an overview of the factors that are important for the retention of CO2 in the subsurface and what processes lead to leakage of CO2 from the reservoir. Initial results indicate that if the reservoir is found to be leaking, CO2 migration is along faults and not through caprock layers. This indicates that faults act as fluid pathways and play an important role when characterizing a storage site. Additionally, it appears that overpressure of the overburden and the state of CO2 in the reservoir influence the likelihood of migration and hence the safety of a reservoir.
Thermal oxidation of nuclear graphite: A large scale waste treatment option.
Theodosiou, Alex; Jones, Abbie N; Marsden, Barry J
2017-01-01
This study has investigated the laboratory scale thermal oxidation of nuclear graphite, as a proof-of-concept for the treatment and decommissioning of reactor cores on a larger industrial scale. If showed to be effective, this technology could have promising international significance with a considerable impact on the nuclear waste management problem currently facing many countries worldwide. The use of thermal treatment of such graphite waste is seen as advantageous since it will decouple the need for an operational Geological Disposal Facility (GDF). Particulate samples of Magnox Reactor Pile Grade-A (PGA) graphite, were oxidised in both air and 60% O2, over the temperature range 400-1200°C. Oxidation rates were found to increase with temperature, with a particular rise between 700-800°C, suggesting a change in oxidation mechanism. A second increase in oxidation rate was observed between 1000-1200°C and was found to correspond to a large increase in the CO/CO2 ratio, as confirmed through gas analysis. Increasing the oxidant flow rate gave a linear increase in oxidation rate, up to a certain point, and maximum rates of 23.3 and 69.6 mg / min for air and 60% O2 respectively were achieved at a flow of 250 ml / min and temperature of 1000°C. These promising results show that large-scale thermal treatment could be a potential option for the decommissioning of graphite cores, although the design of the plant would need careful consideration in order to achieve optimum efficiency and throughput.
Thermal oxidation of nuclear graphite: A large scale waste treatment option
Jones, Abbie N.; Marsden, Barry J.
2017-01-01
This study has investigated the laboratory scale thermal oxidation of nuclear graphite, as a proof-of-concept for the treatment and decommissioning of reactor cores on a larger industrial scale. If showed to be effective, this technology could have promising international significance with a considerable impact on the nuclear waste management problem currently facing many countries worldwide. The use of thermal treatment of such graphite waste is seen as advantageous since it will decouple the need for an operational Geological Disposal Facility (GDF). Particulate samples of Magnox Reactor Pile Grade-A (PGA) graphite, were oxidised in both air and 60% O2, over the temperature range 400–1200°C. Oxidation rates were found to increase with temperature, with a particular rise between 700–800°C, suggesting a change in oxidation mechanism. A second increase in oxidation rate was observed between 1000–1200°C and was found to correspond to a large increase in the CO/CO2 ratio, as confirmed through gas analysis. Increasing the oxidant flow rate gave a linear increase in oxidation rate, up to a certain point, and maximum rates of 23.3 and 69.6 mg / min for air and 60% O2 respectively were achieved at a flow of 250 ml / min and temperature of 1000°C. These promising results show that large-scale thermal treatment could be a potential option for the decommissioning of graphite cores, although the design of the plant would need careful consideration in order to achieve optimum efficiency and throughput. PMID:28793326
DOE Office of Scientific and Technical Information (OSTI.GOV)
Malhotra, Vivak
The USA is embarking upon tackling the serious environmental challenges posed to the world by greenhouse gases, especially carbon dioxide (CO2). The dimension of the problem is daunting. In fact, according to the Energy Information Agency, nearly 6 billion metric tons of CO2 were produced in the USA in 2007 with coal-burning power plants contributing about 2 billion metric tons. To mitigate the concerns associated with CO2 emission, geological sequestration holds promise. Among the potential geological storage sites, unmineable coal seams and shale formations in particular show promise because of the probability of methane recovery while sequestering the CO2. However.more » the success of large-scale sequestration of CO2 in coal and shale would hinge on a thorough understanding of CO2's interactions with host reservoirs. An important parameter for successful storage of CO2 reservoirs would be whether the pressurized CO2 would remain invariant in coal and shale formations under reasonable internal and/or external perturbations. Recent research has brought to the fore the potential of induced seismicity, which may result in caprock compromise. Therefore, to evaluate the potential risks involved in sequestering CO2 in Illinois bituminous coal seams and shale, we studied: (i) the mechanical behavior of Murphysboro (Illinois) and Houchin Creek (Illinois) coals, (ii) thermodynamic behavior of Illinois bituminous coal at - 100oC ≤ T ≤ 300oC, (iii) how high pressure CO2 (up to 20.7 MPa) modifies the viscosity of the host, (iv) the rate of emission of CO2 from Illinois bituminous coal and shale cores if the cores, which were pressurized with high pressure (≤ 20.7 MPa) CO2, were exposed to an atmospheric pressure, simulating the development of leakage pathways, (v) whether there are any fractions of CO2 stored in these hosts which are resistance to emission by simply exposing the cores to atmospheric pressure, and (vi) how compressive shockwaves applied to the coal and shale cores, which were pressurized with high pressure CO2, determine the fate of sequestered CO2 in these cores. Our results suggested that Illinois bituminous coal in its unperturbed state, i.e., when not pressurized with CO2, showed large variations in the mechanical properties. Modulus varied from 0.7 GPa to 3.4 GPa even though samples were extracted from a single large chunk of coal. We did not observe any glass transition for Illinois bituminous coal at - 100oC ≤ T ≤ 300oC, however, when the coal was pressurized with CO2 at ambient ≤ P ≤ 20.7 MPa, the viscosity of the coal decreased and inversely scaled with the CO2 pressure. The decrease in viscosity as a function of pressure could pose CO2 injection problems for coal as lower viscosity would allow the solid coal to flow to plug the fractures, fissures, and cleats. Our experiments also showed a very small fraction of CO2 was absorbed in coal; and when CO2 pressurized coals were exposed to atmospheric conditions, the loss of CO2 from coals was massive. Half of the sequestered gas from the coal cores was lost in less than 20 minutes. Our shockwave experiments on Illinois bituminous coal, New Albany shale (Illinois), Devonian shale (Ohio), and Utica shale (Ohio) presented clear evidence that the significant emission of the sequestered CO2 from these formations cannot be discounted during seismic activity, especially if caprock is compromised. It is argued that additional shockwave studies, both compressive and transverse, would be required for successfully mapping the risks associated with sequestering high pressure CO2 in coal and shale formations.« less
Liquid Hydrocarbon Production from CO2 : Recent Development in Metal-Based Electrocatalysis.
Daiyan, Rahman; Lu, Xunyu; Ng, Yun Hau; Amal, Rose
2017-11-23
Rising levels of CO 2 accumulation in the atmosphere have attracted considerable interest in technologies capable of CO 2 capture, storage and conversion. The electrochemical reduction of CO 2 into high-value liquid organic products could be of vital importance to mitigate this issue. The conversion of CO 2 into liquid fuels by using photovoltaic cells, which can readily be integrated in the current infrastructure, will help realize the creation of a sustainable cycle of carbon-based fuel that will promote zero net CO 2 emissions. Despite promising findings, significant challenges still persist that must be circumvented to make the technology profitable for large-scale utilization. With such possibilities, this Minireview presents the current high-performing catalysts for the electrochemical reduction of CO 2 to liquid hydrocarbons, address the limitations and unify the current understanding of the different reaction mechanisms. The Minireview also explores current research directions to improve process efficiencies and production rate and discusses the scope of using photo-assisted electrochemical reduction systems to find stable, highly efficient catalysts that can harvest solar energy directly to convert CO 2 into liquid hydrocarbons. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Divergent biophysical controls of aquatic CO2 and CH4 in the World's two largest rivers.
Borges, Alberto V; Abril, Gwenaël; Darchambeau, François; Teodoru, Cristian R; Deborde, Jonathan; Vidal, Luciana O; Lambert, Thibault; Bouillon, Steven
2015-10-23
Carbon emissions to the atmosphere from inland waters are globally significant and mainly occur at tropical latitudes. However, processes controlling the intensity of CO2 and CH4 emissions from tropical inland waters remain poorly understood. Here, we report a data-set of concurrent measurements of the partial pressure of CO2 (pCO2) and dissolved CH4 concentrations in the Amazon (n = 136) and the Congo (n = 280) Rivers. The pCO2 values in the Amazon mainstem were significantly higher than in the Congo, contrasting with CH4 concentrations that were higher in the Congo than in the Amazon. Large-scale patterns in pCO2 across different lowland tropical basins can be apprehended with a relatively simple statistical model related to the extent of wetlands within the basin, showing that, in addition to non-flooded vegetation, wetlands also contribute to CO2 in river channels. On the other hand, dynamics of dissolved CH4 in river channels are less straightforward to predict, and are related to the way hydrology modulates the connectivity between wetlands and river channels.
Imaging diffuse clouds: bright and dark gas mapped in CO
NASA Astrophysics Data System (ADS)
Liszt, H. S.; Pety, J.
2012-05-01
Aims: We wish to relate the degree scale structure of galactic diffuse clouds to sub-arcsecond atomic and molecular absorption spectra obtained against extragalactic continuum background sources. Methods: We used the ARO 12 m telescope to map J = 1-0 CO emission at 1' resolution over 30' fields around the positions of 11 background sources occulted by 20 molecular absorption line components, of which 11 had CO emission counterparts. We compared maps of CO emission to sub-arcsec atomic and molecular absorption spectra and to the large-scale distribution of interstellar reddening. Results: 1) The same clouds, identified by their velocity, were seen in absorption and emission and atomic and molecular phases, not necessarily in the same direction. Sub-arcsecond absorption spectra are a preview of what is seen in CO emission away from the continuum. 2) The CO emission structure was amorphous in 9 cases, quasi-periodic or wave-like around B0528+134 and tangled and filamentary around BL Lac. 3) Strong emission, typically 4-5 K at EB - V ≤ 0.15 mag and up to 10-12 K at EB - V ≲ 0.3 mag was found, much brighter than toward the background targets. Typical covering factors of individual features at the 1 K km s-1 level were 20%. 4) CO-H2 conversion factors as much as 4-5 times below the mean value N(H2)/WCO = 2 × 1020 H2 cm-2 (K km s-1)-1 are required to explain the luminosity of CO emission at/above the level of 1 K km s-1. Small conversion factors and sharp variability of the conversion factor on arcminute scales are due primarily to CO chemistry and need not represent unresolved variations in reddening or total column density. Conclusions: Like Fermi and Planck we see some gas that is dark in CO and other gas in which CO is overluminous per H2. A standard CO-H2 conversion factor applies overall owing to balance between the luminosities per H2 and surface covering factors of bright and dark CO, but with wide variations between sightlines and across the faces of individual clouds. Based on observations obtained with the ARO Kitt Peak 12 m telescope.Appendices are available in electronic form at http://www.aanda.org
NASA Technical Reports Server (NTRS)
Boering, Kristie A.; Connell, Peter; Rotman, Douglas
2005-01-01
Until recently, the stable isotopic composition of chemically and datively important stratospheric species, such as ozone (O3), carbon dioxide (CO2), nitrous oxide (N2O), and methane (CH4), was largely unexplored, despite indications from the few measurements available and theoretical studies that global-scale isotopic variations will provide a unique tool for quantifying rates of global-scale mass transport into, within, and out of the stratosphere and for understanding the mechanisms of chemical reactions involved in ozone production. The number and geographical extent of observations are beginning to increase rapidly, however, as access to the stratosphere, both directly and by remote-sensing, has increased over the last 10 years and as new analytical techniques have been developed that make global-scale isotope measurements by whole-air sampling more feasible. The objective of this study, begun in April 1999, is to incorporate into the Livermore 2D model the likely photochemical fractionation processes that determine the isotopic compositions of stratospheric CO2, N2O, CH4, and O3, and to use the model results and new observations from NASA field campaigns in 1996 and 1997 to investigate stratospheric chemistry and mass transport. Additionally, since isotopic signatures from the stratosphere are transferred to the troposphere by downward transport at middle and high latitudes, the isotopic compositions may also serve as sensitive tracers of stratosphere-totroposphere transport. Comparisons of model results with stratospheric and upper tropospheric observations from these campaigns, as well as with ground-based observations from new NOAA and NSF-sponsored studies, will help determine whether the magnitudes of the stratospheric fractionation processes are large enough to use as global-scale tracers of transport into the troposphere and, if so, will be used to help constrain the degree of coupling between the troposphere and the stratosphere.
Ooi, Jillian L. S.; Van Niel, Kimberly P.; Kendrick, Gary A.; Holmes, Karen W.
2014-01-01
Background Seagrass species in the tropics occur in multispecies meadows. How these meadows are maintained through species co-existence and what their ecological drivers may be has been an overarching question in seagrass biogeography. In this study, we quantify the spatial structure of four co-existing species and infer potential ecological processes from these structures. Methods and Results Species presence/absence data were collected using underwater towed and dropped video cameras in Pulau Tinggi, Malaysia. The geostatistical method, utilizing semivariograms, was used to describe the spatial structure of Halophila spp, Halodule uninervis, Syringodium isoetifolium and Cymodocea serrulata. Species had spatial patterns that were oriented in the along-shore and across-shore directions, nested with larger species in meadow interiors, and consisted of multiple structures that indicate the influence of 2–3 underlying processes. The Linear Model of Coregionalization (LMC) was used to estimate the amount of variance contributing to the presence of a species at specific spatial scales. These distances were <2.5 m (micro-scale), 2.5–50 m (fine-scale) and >50 m (broad-scale) in the along-shore; and <2.5 m (micro-scale), 2.5–140 m (fine-scale) and >140 m (broad-scale) in the across-shore. The LMC suggests that smaller species (Halophila spp and H. uninervis) were most influenced by broad-scale processes such as hydrodynamics and water depth whereas large, localised species (S. isoetifolium and C. serrulata) were more influenced by finer-scale processes such as sediment burial, seagrass colonization and growth, and physical disturbance. Conclusion In this study, we provide evidence that spatial structure is distinct even when species occur in well-mixed multispecies meadows, and we suggest that size-dependent plant traits have a strong influence on the distribution and maintenance of tropical marine plant communities. This study offers a contrast from previous spatial models of seagrasses which have largely focused on monospecific temperate meadows. PMID:24497978
Ooi, Jillian L S; Van Niel, Kimberly P; Kendrick, Gary A; Holmes, Karen W
2014-01-01
Seagrass species in the tropics occur in multispecies meadows. How these meadows are maintained through species co-existence and what their ecological drivers may be has been an overarching question in seagrass biogeography. In this study, we quantify the spatial structure of four co-existing species and infer potential ecological processes from these structures. Species presence/absence data were collected using underwater towed and dropped video cameras in Pulau Tinggi, Malaysia. The geostatistical method, utilizing semivariograms, was used to describe the spatial structure of Halophila spp, Halodule uninervis, Syringodium isoetifolium and Cymodocea serrulata. Species had spatial patterns that were oriented in the along-shore and across-shore directions, nested with larger species in meadow interiors, and consisted of multiple structures that indicate the influence of 2-3 underlying processes. The Linear Model of Coregionalization (LMC) was used to estimate the amount of variance contributing to the presence of a species at specific spatial scales. These distances were <2.5 m (micro-scale), 2.5-50 m (fine-scale) and >50 m (broad-scale) in the along-shore; and <2.5 m (micro-scale), 2.5-140 m (fine-scale) and >140 m (broad-scale) in the across-shore. The LMC suggests that smaller species (Halophila spp and H. uninervis) were most influenced by broad-scale processes such as hydrodynamics and water depth whereas large, localised species (S. isoetifolium and C. serrulata) were more influenced by finer-scale processes such as sediment burial, seagrass colonization and growth, and physical disturbance. In this study, we provide evidence that spatial structure is distinct even when species occur in well-mixed multispecies meadows, and we suggest that size-dependent plant traits have a strong influence on the distribution and maintenance of tropical marine plant communities. This study offers a contrast from previous spatial models of seagrasses which have largely focused on monospecific temperate meadows.
Luan, Chuhao; Shao, Yang; Lu, Qi; Gao, Shenghan; Huang, Kai; Wu, Hui; Yao, Kefu
2018-05-30
An efficient and selective catalyst is in urgent need for carbon dioxide electroreduction and silver is one of the promising candidates with affordable costs. Here we fabricated large-scale vertically standing Ag nanowire arrays with high crystallinity and electrical conductivity as carbon dioxide electroreduction catalysts by a simple nanomolding method that was usually considered not feasible for metallic crystalline materials. A great enhancement of current densities and selectivity for CO at moderate potentials was achieved. The current density for CO ( j co ) of Ag nanowire array with 200 nm in diameter was more than 2500 times larger than that of Ag foil at an overpotential of 0.49 V with an efficiency over 90%. The origin of enhanced performances are attributed to greatly increased electrochemically active surface area (ECSA) and higher intrinsic activity compared to those of polycrystalline Ag foil. More low-coordinated sites on the nanowires which can stabilize the CO 2 intermediate better are responsible for the high intrinsic activity. In addition, the impact of surface morphology that induces limited mass transportation on reaction selectivity and efficiency of nanowire arrays with different diameters was also discussed.
Subtask – CO 2 storage and enhanced bakken recovery research program
DOE Office of Scientific and Technical Information (OSTI.GOV)
Sorensen, James; Hawthorne, Steven; Smith, Steven
Small improvements in productivity could increase technically recoverable oil in the Bakken Petroleum System by billions of barrels. The use of CO 2 for enhanced oil recovery (EOR) in tight oil reservoirs is a relatively new concept. The large-scale injection of CO 2 into the Bakken would also result in the geological storage of significant amounts of CO 2. The Energy & Environmental Research Center (EERC) has conducted laboratory and modeling activities to examine the potential for CO 2 storage and EOR in the Bakken. Specific activities included the characterization and subsequent modeling of North Dakota study areas as wellmore » as dynamic predictive simulations of possible CO 2 injection schemes to predict the potential CO 2 storage and EOR in those areas. Laboratory studies to evaluate the ability of CO 2 to remove hydrocarbons from Bakken rocks and determine minimum miscibility pressures for Bakken oil samples were conducted. Data from a CO 2 injection test conducted in the Elm Coulee area of Montana in 2009 were evaluated with an eye toward the possible application of knowledge gained to future injection tests in other areas. A first-order estimation of potential CO 2 storage capacity in the Bakken Formation in North Dakota was also conducted. Key findings of the program are as follows. The results of the research activities suggest that CO 2 may be effective in enhancing the productivity of oil from the Bakken and that the Bakken may hold the ability to geologically store between 120 Mt and 3.2 Gt of CO 2. However, there are no clear-cut answers regarding the most effective approach for using CO 2 to improve oil productivity or the storage capacity of the Bakken. The results underscore the notion that an unconventional resource will likely require unconventional methods of both assessment and implementation when it comes to the injection of CO 2. In particular, a better understanding of the fundamental mechanisms controlling the interactions between CO 2, oil, and other reservoir fluids in these unique formations is necessary to develop accurate assessments of potential CO 2 storage and EOR in the Bakken. In addition, existing modeling and simulation software packages do not adequately address or incorporate the unique properties of these tight, unconventional reservoirs in terms of their impact on CO 2 behavior. These knowledge gaps can be filled by conducting scaled-up laboratory activities integrated with improved modeling and simulation techniques, the results of which will provide a robust foundation for pilot-scale field injection tests. Finally, field-based data on injection, fluid production, and long-term monitoring from pilot-scale CO 2 injection tests in the Bakken are necessary to verify and validate the findings of the laboratory- and modeling-based research efforts. This subtask was funded through the EERC–U.S. Department of Energy (DOE) Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FC26-08NT43291. Nonfederal funding was provided by the North Dakota Industrial Commission, Marathon Oil Corporation, Continental Resources Inc., and TAQA North, Ltd.« less
Yoshida, Nozomu; Levine, Jonathan S.; Stauffer, Philip H.
2016-03-22
Numerical reservoir models of CO 2 injection in saline formations rely on parameterization of laboratory-measured pore-scale processes. Here, we have performed a parameter sensitivity study and Monte Carlo simulations to determine the normalized change in total CO 2 injected using the finite element heat and mass-transfer code (FEHM) numerical reservoir simulator. Experimentally measured relative permeability parameter values were used to generate distribution functions for parameter sampling. The parameter sensitivity study analyzed five different levels for each of the relative permeability model parameters. All but one of the parameters changed the CO 2 injectivity by <10%, less than the geostatistical uncertainty that applies to all large subsurface systems due to natural geophysical variability and inherently small sample sizes. The exception was the end-point CO 2 relative permeability, kmore » $$0\\atop{r}$$ CO2, the maximum attainable effective CO 2 permeability during CO 2 invasion, which changed CO2 injectivity by as much as 80%. Similarly, Monte Carlo simulation using 1000 realizations of relative permeability parameters showed no relationship between CO 2 injectivity and any of the parameters but k$$0\\atop{r}$$ CO2, which had a very strong (R 2 = 0.9685) power law relationship with total CO 2 injected. Model sensitivity to k$$0\\atop{r}$$ CO2 points to the importance of accurate core flood and wettability measurements.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Yoshida, Nozomu; Levine, Jonathan S.; Stauffer, Philip H.
Numerical reservoir models of CO 2 injection in saline formations rely on parameterization of laboratory-measured pore-scale processes. Here, we have performed a parameter sensitivity study and Monte Carlo simulations to determine the normalized change in total CO 2 injected using the finite element heat and mass-transfer code (FEHM) numerical reservoir simulator. Experimentally measured relative permeability parameter values were used to generate distribution functions for parameter sampling. The parameter sensitivity study analyzed five different levels for each of the relative permeability model parameters. All but one of the parameters changed the CO 2 injectivity by <10%, less than the geostatistical uncertainty that applies to all large subsurface systems due to natural geophysical variability and inherently small sample sizes. The exception was the end-point CO 2 relative permeability, kmore » $$0\\atop{r}$$ CO2, the maximum attainable effective CO 2 permeability during CO 2 invasion, which changed CO2 injectivity by as much as 80%. Similarly, Monte Carlo simulation using 1000 realizations of relative permeability parameters showed no relationship between CO 2 injectivity and any of the parameters but k$$0\\atop{r}$$ CO2, which had a very strong (R 2 = 0.9685) power law relationship with total CO 2 injected. Model sensitivity to k$$0\\atop{r}$$ CO2 points to the importance of accurate core flood and wettability measurements.« less
Changes and Attribution of Extreme Precipitation in Climate Models: Subdaily and Daily Scales
NASA Astrophysics Data System (ADS)
Zhang, W.; Villarini, G.; Scoccimarro, E.; Vecchi, G. A.
2017-12-01
Extreme precipitation events are responsible for numerous hazards, including flooding, soil erosion, and landslides. Because of their significant socio-economic impacts, the attribution and projection of these events is of crucial importance to improve our response, mitigation and adaptation strategies. Here we present results from our ongoing work.In terms of attribution, we use idealized experiments [pre-industrial control experiment (PI) and 1% per year increase (1%CO2) in atmospheric CO2] from ten general circulation models produced under the Coupled Model Intercomparison Project Phase 5 (CMIP5) and the fraction of attributable risk to examine the CO2 effects on extreme precipitation at the sub-daily and daily scales. We find that the increased CO2 concentration substantially increases the odds of the occurrence of sub-daily precipitation extremes compared to the daily scale in most areas of the world, with the exception of some regions in the sub-tropics, likely in relation to the subsidence of the Hadley Cell. These results point to the large role that atmospheric CO2 plays in extreme precipitation under an idealized framework. Furthermore, we investigate the changes in extreme precipitation events with the Community Earth System Model (CESM) climate experiments using the scenarios consistent with the 1.5°C and 2°C temperature targets. We find that the frequency of annual extreme precipitation at a global scale increases in both 1.5°C and 2°C scenarios until around 2070, after which the magnitudes of the trend become much weaker or even negative. Overall, the frequency of global annual extreme precipitation is similar between 1.5°C and 2°C for the period 2006-2035, and the changes in extreme precipitation in individual seasons are consistent with those for the entire year. The frequency of extreme precipitation in the 2°C experiments is higher than for the 1.5°C experiment after the late 2030s, particularly for the period 2071-2100.
Wang, Min; Jang, Sung Kyu; Jang, Won-Jun; Kim, Minwoo; Park, Seong-Yong; Kim, Sang-Woo; Kahng, Se-Jong; Choi, Jae-Young; Ruoff, Rodney S; Song, Young Jae; Lee, Sungjoo
2013-05-21
Direct chemical vapor deposition (CVD) growth of single-layer graphene on CVD-grown hexagonal boron nitride (h-BN) film can suggest a large-scale and high-quality graphene/h-BN film hybrid structure with a defect-free interface. This sequentially grown graphene/h-BN film shows better electronic properties than that of graphene/SiO2 or graphene transferred on h-BN film, and suggests a new promising template for graphene device fabrication. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Soil carbon change in reconstructed tallgrass prairies
USDA-ARS?s Scientific Manuscript database
Reconstructing former cropland to tallgrass prairie can increase soil carbon (C) and enhance C sequestration to mitigate increases in atmospheric CO2. This large-scale study was conducted at Neal Smith National Wildlife Refuge (NSNWR) in Jasper County, south-central IA. Tracts of cropped land at NSN...
NASA Astrophysics Data System (ADS)
Chen, F.; Wiese, B.; Zhou, Q.; Birkholzer, J. T.; Kowalsky, M. B.
2013-12-01
The Stuttgart formation used for ongoing CO2 injection at the Ketzin pilot test site in Germany is highly heterogeneous in nature. The site characterization data, including 3D seismic amplitude images, the regional geology data, and the core measurements and geophysical logs of the wells show the formation is composed of permeable sandstone channels of varying thickness and length embedded in less permeable mudstones. Most of the sandstone channels are located in the upper 10-15 m of the formation, with only a few sparsely distributed sandstone channels in the bottom 70-m layer. Three-dimensional seismic data help to identify the large-scale facies distribution patterns in the Stuttgart formation, but are unable to resolve internal structures at a smaller scale (e.g. ~100 m). Heterogeneity has a large effect on the pressure propagation measured during a suite of pumping tests conducted in 2007-2008 and also impacts strongly the CO2 arrival times observed during the ongoing CO2 injection experiment. The arrival time of the CO2 plume at the observation well Ktzi 202was 12.5 times greater than at the other observation well Ktzi 200, even though the distance to the injection well is only 2.2 times farther than that of Ktzi 200. To characterize subsurface properties and help predict the behavior of injected CO2 in subsequent experiments, we develop a TOUGH2/EOS9 model for modeling the hydraulic pumping tests and use the inverse modeling tool iTOUGH2 for automatic model calibration. The model domain is parameterized using multiple zones, with each zone assumed to have uniform rock properties. The calibrated model produces system responses that are in good agreement with the measured pressure drawdown data, indicating that it captures the essential flow processes occurring during the pumping tests. The estimated permeability distribution shows that the heterogeneity is significant and that the study site is situated a semi-closed system with one or two sides open to permeable regions and the others effectively blocked by low-permeability regions. A low-permeability zone appears at the northern boundary of the model. Of the three wells that are analyzed, permeable channels are found to connect Ktzi 202 with Ktzi 200/Ktzi 201, while a low-permeability zone is observed between Ktzi 201 and Ktzi 200. The calibrated results are consistent with the crosshole ERT data and can help explain the position of a CO2 plume, inferred from 3D seismic surveys in a subsequent CO2 injection experiment. Because the CO2 transport that occurs during a CO2 injection and the pressure propagation that occurs during pumping tests are sensitive to different scales of subsurface heterogeneity, direct application of a model calibrated from pumping test data is inappropriate for predicting CO2 arrival. However, by including a thin layer of highly permeable sandstone, we present a proof-of-concept model that produces CO2 arrival times comparable to those observed at the site.
Study of CO2 sorbents for extravehicular activity
NASA Technical Reports Server (NTRS)
Colombo, G. V.
1973-01-01
Portable life support equipment was studied for meeting the requirements of extravehicular activities. Previous studies indicate that the most promising method for performing the CO2 removal function removal function were metallic oxides and/or metallic hydroxides. Mgo, Ag2, and Zno metallic oxides and Mg(OH)2 and Zn(OH)2 metallic hydroxides were studied, by measuring sorption and regeneration properties of each material. The hydroxides of Mg and Zn were not regenerable and the zinc oxide compounds showed no stable form. A silver oxide formulation was developed which rapidly absorbs approximately 95% of its 0.19 Kg CO2 Kg oxide and has shown no sorption or structural degeneration through 22 regenerations. It is recommended that the basic formula be further developed and tested in large-scale beds under simulated conditions.
The ALMA-PILS Survey: Formaldehyde deuteration in warm gas on small scales toward IRAS 16293-2422 B
NASA Astrophysics Data System (ADS)
Persson, M. V.; Jørgensen, J. K.; Müller, H. S. P.; Coutens, A.; van Dishoeck, E. F.; Taquet, V.; Calcutt, H.; van der Wiel, M. H. D.; Bourke, T. L.; Wampfler, S. F.
2018-02-01
Context. The enhanced degrees of deuterium fractionation observed in envelopes around protostars demonstrate the importance of chemistry at low temperatures, relevant in pre- and protostellar cores. Formaldehyde is an important species in the formation of methanol and more complex molecules. Aims: Here, we aim to present the first study of formaldehyde deuteration on small scales around the prototypical low-mass protostar IRAS 16293-2422 using high spatial and spectral resolution Atacama Large Millimeter/submillimeter Array (ALMA) observations. We determine the excitation temperature, abundances and fractionation level of several formaldehyde isotopologues, including its deuterated forms. Methods: Excitation temperature and column densities of formaldehyde in the gas close to one of the components of the binary were constrained through modeling of optically thin lines assuming local thermodynamical equilibrium. The abundance ratios were compared to results from previous single dish observations, astrochemical models and local ISM values. Results: Numerous isotopologues of formaldehyde are detected, among them H2C17O, and D213CO for the first time in the ISM. The large range of upper energy levels covered by the HDCO lines help constrain the excitation temperature to 106 ± 13 K. Using the derived column densities, formaldehyde shows a deuterium fractionation of HDCO/H2CO = 6.5 ± 1%, D2CO/HDCO = 12.8-4.1+3.3%, and D2CO/H2CO = 0.6(4) ± 0.1%. The isotopic ratios derived are 16O/18O = 805-79+43, 18O/17O = 3.2-0.3+0.2, and 12C/13C = 56-11+8. Conclusions: The HDCO/H2CO ratio is lower than that found in previous studies, highlighting the uncertainties involved in interpreting single dish observations of the inner warm regions. The D2CO/HDCO ratio is only slightly larger than the HDCO/H2CO ratio. This is consistent with formaldehyde forming in the ice as soon as CO has frozen onto the grains, with most of the deuteration happening toward the end of the prestellar core phase. A comparison with available time-dependent chemical models indicates that the source is in the early Class 0 stage.
Sources and Fate of DIC in Swedish Streams
NASA Astrophysics Data System (ADS)
Campeau, A.; Wallin, M.; Bishop, K. H.; Giesler, R.; Mörth, C. M.; Venkiteswaran, J. J.
2015-12-01
DIC export by streams and rivers is a major component of the global C cycle. However, many questions remain about the source and fate of aquatic DIC and CO2. Stable carbon isotope δ13C can provide information about the source and evolution of DIC and CO2 along hydrological networks. But the interpretation of δ13C values must be made with caution, since several biogeochemical processes affect the isotopic signal. In this study, we developed a systematic approach resolving these influences when interpreting large-scale patterns in δ13C-DIC and δ13C-CO2 values with regard to the source and fate of C in low order streams. We analyzed δ13C-DIC values in streams from four different regions of Sweden. Taken together they span large gradients in climate, geomorphology and lithology. The source of the DIC pool was predominantly biogenic in three of the regions (δ13C-DICsource = -17.4‰), but not the northernmost, where a clear geogenic input could be identified (δ13C-DICsource =-8.2 ‰). Our results suggest that soil respired CO2 is the main source of stream CO2 (δ13C-CO2source=-22.9‰) in all four regions, yet aquatic processes can also be a contributing component of the DIC pool in streams, with corresponding influence on the δ13C values. Once CO2 was in the stream, degassing was the primary control on its fate. However, there were indications that aquatic biological processes added CO2, (by DOC degradation) in the southernmost region, and that CO2 was removed (by photosynthesis) in the most central region. Correctly interpreted, the carbon stable isotope data can serve as a powerful tool for identifying the source and fate of stream DIC.
Characterization of iron carbonate scales developed under carbon dioxide corrosion conditions
NASA Astrophysics Data System (ADS)
de Moraes, Flavio Dias
1999-11-01
Carbon steel CO2 corrosion is a common and very serious problem in the oil industry. It often results in severe damage to pipes and equipment. Besides controlling direct costs associated with loss of production and replacement or repair to the equipment damaged by corrosion, life and environmental safety must be protected with the thorough study of this type of corrosion. For a given type of steel, the CO2 corrosion rates are strongly influenced by many mechanical and environmental factors, such as flow velocity, temperature, gas-liquid ratio, oil-water ratio, CO2 partial pressure, and the chemical composition of the produced water. Under specific conditions, a corrosion product, the iron carbonate (FeCO3), can deposit over the corroding metal as a scale and dramatically reduce the CO2 corrosion rates on carbon steels. The ability to reliably predict the protective characteristics of such scales so that this knowledge may be used to mitigate the CO2 corrosion problem is the main objective of this research. CO2 corrosion tests performed under various CO2 corrosion flowing conditions in a flow loop were used to generate and study FeCO3 scales. In situ Electrochemical Impedance Spectroscopy (EIS) techniques were successfully used to monitor the development of the scales throughout the duration of the tests. The EIS monitoring enabled the identification of the type of scales being formed and the quantification of the protection they give. A procedure using EIS, SEM and X-ray diffraction was developed to electrochemically and morphologically characterize the scales formed. In this work, morphology of the scales was proved to be the most important characteristic related to CO2 corrosion protection, and temperature was found to be the main environmental parameter controlling the morphology of the scales. For the environmental conditions tested, a correlation was developed to predict the type of iron carbonate scales that would be formed and the amount of CO2 corrosion protection these scales would provide to carbon steels.
Molecular clouds and the large-scale structure of the galaxy
NASA Technical Reports Server (NTRS)
Thaddeus, Patrick; Stacy, J. Gregory
1990-01-01
The application of molecular radio astronomy to the study of the large-scale structure of the Galaxy is reviewed and the distribution and characteristic properties of the Galactic population of Giant Molecular Clouds (GMCs), derived primarily from analysis of the Columbia CO survey, and their relation to tracers of Population 1 and major spiral features are described. The properties of the local molecular interstellar gas are summarized. The CO observing programs currently underway with the Center for Astrophysics 1.2 m radio telescope are described, with an emphasis on projects relevant to future comparison with high-energy gamma-ray observations. Several areas are discussed in which high-energy gamma-ray observations by the EGRET (Energetic Gamma-Ray Experiment Telescope) experiment aboard the Gamma Ray Observatory will directly complement radio studies of the Milky Way, with the prospect of significant progress on fundamental issues related to the structure and content of the Galaxy.
NASA Astrophysics Data System (ADS)
Dou, S.; Commer, M.; Ajo Franklin, J. B.; Freifeld, B. M.; Robertson, M.; Wood, T.; McDonald, S.
2017-12-01
Archer Daniels Midland Company's (ADM) world-scale agricultural processing and biofuels production complex located in Decatur, Illinois, is host to two industrial-scale carbon capture and storage projects. The first operation within the Illinois Basin-Decatur Project (IBDP) is a large-scale pilot that injected 1,000,000 metric tons of CO2 over a three year period (2011-2014) in order to validate the Illinois Basin's capacity to permanently store CO2. Injection for the second operation, the Illinois Industrial Carbon Capture and Storage Project (ICCS), started in April 2017, with the purpose of demonstrating the integration of carbon capture and storage (CCS) technology at an ethanol plant. The capacity to store over 1,000,000 metric tons of CO2 per year is anticipated. The latter project is accompanied by the development of an intelligent monitoring system (IMS) that will, among other tasks, perform hydrogeophysical joint analysis of pressure, temperature and seismic reflection data. Using a preliminary radial model assumption, we carry out synthetic joint inversion studies of these data combinations. We validate the history-matching process to be applied to field data once CO2-breakthrough at observation wells occurs. This process will aid the estimation of permeability and porosity for a reservoir model that best matches monitoring observations. The reservoir model will further be used for forecasting studies in order to evaluate different leakage scenarios and develop appropriate early-warning mechanisms. Both the inversion and forecasting studies aim at building an IMS that will use the seismic and pressure-temperature data feeds for providing continuous model calibration and reservoir status updates.
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.
NASA Astrophysics Data System (ADS)
Xueref-Remy, I.
2010-12-01
Atmospheric CO2 concentration has been increasing of more than 30% since the pre-industrial era due to human activities, and is very likely involved in the recent global temperature increase [IPCC, 2007]. Although we have good estimates of the CO2 fluxes on a global basis, and have a relatively well-established system to detect the large-scale trends, regional information (10-500km) is needed if society is ever to manage or verify carbon emissions. We must improve our understanding of regional variations in the sources and sinks of CO2 because they help identify possible sequestration or emission management options. New programs are needed to improve our understanding of meso-scale carbon fluxes, and to discriminate between the anthropogenic and biospheric sources which are very strongly overlapped in European countries. In this context we need to monitor the emissions originating from the megalopolis such as Paris and its agglomeration, and the way they are spreading in the background atmosphere. Nowadays, inventories (CITEPA, AIRPARIF) based on statistical information provide CO2 emissions from Ile de France and all others regions of France, but no independent verification based on CO2 measurements has been done yet. Atmospheric measurements coupled to a meso-scale model can be used to provide such verification, especially to detect the interannual and decadal trends which could result from regional management strategy. The CO2-MEGAPARIS project (2009-2012) objective is to develop four independent methods to verify the emission inventories, and to monitor the daily to monthly CO2 emissions from Ile de France as well as their spreading to neighbouring regions with a scale up to 2x2 km2. The first method consists in developing a synergy between a mesoscale model (CHIMERE/MM5), inventories and observations using a top-down approach based on an inversion technique to retrieve surface fluxes (3 new observing stations are developed among which the top of the Eiffel tower). The second method is to assess the anthropogenic emissions from Ile de France using the Radon method based on correlations between the concentrations of Radon 222 (continental tracer) and atmospheric CO2. The third method is to study the propagation of the anthropogenic plume towards the region Centre by applying an atmospheric boundary layer budget at LSCE’s observation site in Orléans forest. The fourth method is to conduct intensive measurements of in-situ CO2 and tracers (CO, potassium, dC13, dC14, ....) in Paris agglomeration to better assess the role and the variability of CO2 sources in Ile-de-France. Especially, a joined campaign with the MEGAPOLI EU-project has been conducted in winter 2010. First results of the CO2-MEGAPARIS project will be presented.
Management effects on greenhouse gas dynamics in fen ditches.
Peacock, Mike; Ridley, Luke M; Evans, Chris D; Gauci, Vincent
2017-02-01
Globally, large areas of peatland have been drained through the digging of ditches, generally to increase agricultural production. By lowering the water table it is often assumed that drainage reduces landscape-scale emissions of methane (CH 4 ) into the atmosphere to negligible levels. However, drainage ditches themselves are known to be sources of CH 4 and other greenhouse gases (GHGs), but emissions data are scarce, particularly for carbon dioxide (CO 2 ) and nitrous oxide (N 2 O), and show high spatial and temporal variability. Here, we report dissolved GHGs and diffusive fluxes of CH 4 and CO 2 from ditches at three UK lowland fens under different management; semi-natural fen, cropland, and cropland restored to low-intensity grassland. Ditches at all three fens emitted GHGs to the atmosphere, but both fluxes and dissolved GHGs showed extensive variation both seasonally and within-site. CH 4 fluxes were particularly large, with medians peaking at all three sites in August at 120-230mgm -2 d -1 . Significant between site differences were detected between the cropland and the other two sites for CO 2 flux and all three dissolved GHGs, suggesting that intensive agriculture has major effects on ditch biogeochemistry. Multiple regression models using environmental and water chemistry data were able to explain 29-59% of observed variation in dissolved GHGs. Annual CH 4 fluxes from the ditches were 37.8, 18.3 and 27.2gCH 4 m -2 yr -1 for the semi-natural, grassland and cropland, and annual CO 2 fluxes were similar (1100 to 1440gCO 2 m -2 yr -1 ) among sites. We suggest that fen ditches are important contributors to landscape-scale GHG emissions, particularly for CH 4 . Ditch emissions should be included in GHG budgets of human modified fens, particularly where drainage has removed the original terrestrial CH 4 source, e.g. agricultural peatlands. Copyright © 2016 Elsevier B.V. All rights reserved.
Lei, Huang; Zhishan, Zhang
2015-01-01
The below-ground CO2 concentration in some crusted soils or flooded fields is usually ten or hundred times larger than the normal levels. Recently, a large number of studies have focused on elevated CO2 in the atmosphere; however, only few have examined the influence of elevated root zone CO2 on plant growth and vegetation succession. In the present study, a closed-air CO2 enrichment (CACE) system was designed to simulate elevated CO2 concentrations in the root zones. The physio-ecological characteristics of two typical xerophytic shrubs C. korshinskii and A. ordosica in re-vegetated desert areas were investigated at different soil CO2 concentrations from March 2011 to October 2013. Results showed that plant growth, phenophase, photosynthetic rate, stomatal conductance, transpiration rate, and water use efficiency for the two xerophytic shrubs were all increased at first and then decreased with increasing soil CO2 concentrations, and the optimal soil CO2 concentration thresholds for C. korshinskii and A. ordosica were 0.554 and 0.317%, respectively. And A. ordosica was more tolerate to root zone CO2 variation when compared with C. korshinskii, possible reasons and vegetation succession were also discussed.
Frerichs, Janin; Rakoczy, Jana; Ostertag-Henning, Christian; Krüger, Martin
2014-01-21
Carbon Capture and Storage (CCS) is currently under debate as large-scale solution to globally reduce emissions of the greenhouse gas CO2. Depleted gas or oil reservoirs and saline aquifers are considered as suitable reservoirs providing sufficient storage capacity. We investigated the influence of high CO2 concentrations on the indigenous bacterial population in the saline formation fluids of a natural gas field. Bacterial community changes were closely examined at elevated CO2 concentrations under near in situ pressures and temperatures. Conditions in the high pressure reactor systems simulated reservoir fluids i) close to the CO2 injection point, i.e. saturated with CO2, and ii) at the outer boundaries of the CO2 dissolution gradient. During the incubations with CO2, total cell numbers remained relatively stable, but no microbial sulfate reduction activity was detected. After CO2 release and subsequent transfer of the fluids, an actively sulfate-respiring community was re-established. The predominance of spore-forming Clostridiales provided evidence for the resilience of this taxon against the bactericidal effects of supercritical (sc)CO2. To ensure the long-term safety and injectivity, the viability of fermentative and sulfate-reducing bacteria has to be considered in the selection, design, and operation of CCS sites.
Heath, Jason E; McKenna, Sean A; Dewers, Thomas A; Roach, Jesse D; Kobos, Peter H
2014-01-21
CO2 storage efficiency is a metric that expresses the portion of the pore space of a subsurface geologic formation that is available to store CO2. Estimates of storage efficiency for large-scale geologic CO2 storage depend on a variety of factors including geologic properties and operational design. These factors govern estimates on CO2 storage resources, the longevity of storage sites, and potential pressure buildup in storage reservoirs. This study employs numerical modeling to quantify CO2 injection well numbers, well spacing, and storage efficiency as a function of geologic formation properties, open-versus-closed boundary conditions, and injection with or without brine extraction. The set of modeling runs is important as it allows the comparison of controlling factors on CO2 storage efficiency. Brine extraction in closed domains can result in storage efficiencies that are similar to those of injection in open-boundary domains. Geomechanical constraints on downhole pressure at both injection and extraction wells lower CO2 storage efficiency as compared to the idealized scenario in which the same volumes of CO2 and brine are injected and extracted, respectively. Geomechanical constraints should be taken into account to avoid potential damage to the storage site.
NASA Astrophysics Data System (ADS)
Zuo, X. Z.; Yang, J.; Yuan, B.; Song, D. P.; Tang, X. W.; Zhang, K. J.; Zhu, X. B.; Song, W. H.; Dai, J. M.; Sun, Y. P.
2015-03-01
We investigate the structural, magnetic, dielectric properties, and scaling behaviors of Aurivillius compounds Bi6-x/3Fe2Ti3-2x(WCo)xO18 (0 ≤ x ≤ 0.15). The room-temperature weak ferromagnetism is observed for the W/Co co-doped samples. The results of the dielectric constant ɛr, complex impedance Z ″ , the dc conductivity σdc, and hopping frequency fH manifest that the dielectric relaxation of the x = 0 sample and the doped samples in the dielectric anomaly region (450-750 K) can be ascribed to the trap-controlled ac conduction around the doubly ionized oxygen vacancies and the localized hopping process of oxygen vacancies, respectively. The scaling behaviors reveal that the dynamic process of both electrons in the x = 0 sample and oxygen vacancies in the doped samples is temperature independent. The ferroelectric Curie-temperature Tc decreases slightly from 973 K to 947 K with increasing the doping level of W/Co. In addition, the dielectric loss exhibits a dielectric relaxation above 800 K with the rather large activation energies (1.95 eV ≤ Ea ≤ 2.72 eV).
NASA Astrophysics Data System (ADS)
Bastos, Ana; Peregon, Anna; Gani, Érico A.; Khudyaev, Sergey; Yue, Chao; Li, Wei; Gouveia, Célia M.; Ciais, Philippe
2018-06-01
While the global carbon budget (GCB) is relatively well constrained over the last decades of the 20th century [1], observations and reconstructions of atmospheric CO2 growth rate present large discrepancies during the earlier periods [2]. The large uncertainty in GCB has been attributed to the land biosphere, although it is not clear whether the gaps between observations and reconstructions are mainly because land-surface models (LSMs) underestimate inter-annual to decadal variability in natural ecosystems, or due to inaccuracies in land-use change reconstructions. As Eurasia encompasses about 15% of the terrestrial surface, 20% of the global soil organic carbon pool and constitutes a large CO2 sink, we evaluate the potential contribution of natural and human-driven processes to induce large anomalies in the biospheric CO2 fluxes in the early 20th century. We use an LSM specifically developed for high-latitudes, that correctly simulates Eurasian C-stocks and fluxes from observational records [3], in order to evaluate the sensitivity of the Eurasian sink to the strong high-latitude warming occurring between 1930 and 1950. We show that the LSM with improved high-latitude phenology, hydrology and soil processes, contrary to the group of LSMs in [2], is able to represent enhanced vegetation growth linked to boreal spring warming, consistent with tree-ring time-series [4]. By compiling a dataset of annual agricultural area in the Former Soviet Union that better reflects changes in cropland area linked with socio-economic fluctuations during the early 20th century, we show that land-abadonment during periods of crisis and war may result in reduced CO2 emissions from land-use change (44%–78% lower) detectable at decadal time-scales. Our study points to key processes that may need to be improved in LSMs and LUC datasets in order to better represent decadal variability in the land CO2 sink, and to better constrain the GCB during the pre-observational record.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Dodds, K.; Daley, T.; Freifeld, B.
2009-05-01
The Australian Cooperative Research Centre for Greenhouse Gas Technologies (CO2CRC) is currently injecting 100,000 tons of CO{sub 2} in a large-scale test of storage technology in a pilot project in southeastern Australia called the CO2CRC Otway Project. The Otway Basin, with its natural CO{sub 2} accumulations and many depleted gas fields, offers an appropriate site for such a pilot project. An 80% CO{sub 2} stream is produced from a well (Buttress) near the depleted gas reservoir (Naylor) used for storage (Figure 1). The goal of this project is to demonstrate that CO{sub 2} can be safely transported, stored underground, andmore » its behavior tracked and monitored. The monitoring and verification framework has been developed to monitor for the presence and behavior of CO{sub 2} in the subsurface reservoir, near surface, and atmosphere. This monitoring framework addresses areas, identified by a rigorous risk assessment, to verify conformance to clearly identifiable performance criteria. These criteria have been agreed with the regulatory authorities to manage the project through all phases addressing responsibilities, liabilities, and to assure the public of safe storage.« less
FEASIBILITY OF LARGE-SCALE OCEAN CO2 SEQUESTRATION
DOE Office of Scientific and Technical Information (OSTI.GOV)
Dr. Peter Brewer; Dr. James Barry
2002-09-30
We have continued to carry out creative small-scale experiments in the deep ocean to investigate the science underlying questions of possible future large-scale deep-ocean CO{sub 2} sequestration as a means of ameliorating greenhouse gas growth rates in the atmosphere. This project is closely linked to additional research funded by the DoE Office of Science, and to support from the Monterey Bay Aquarium Research Institute. The listing of project achievements here over the past year reflects these combined resources. Within the last project year we have: (1) Published a significant workshop report (58 pages) entitled ''Direct Ocean Sequestration Expert's Workshop'', basedmore » upon a meeting held at MBARI in 2001. The report is available both in hard copy, and on the NETL web site. (2) Carried out three major, deep ocean, (3600m) cruises to examine the physical chemistry, and biological consequences, of several liter quantities released on the ocean floor. (3) Carried out two successful short cruises in collaboration with Dr. Izuo Aya and colleagues (NMRI, Osaka, Japan) to examine the fate of cold (-55 C) CO{sub 2} released at relatively shallow ocean depth. (4) Carried out two short cruises in collaboration with Dr. Costas Tsouris, ORNL, to field test an injection nozzle designed to transform liquid CO{sub 2} into a hydrate slurry at {approx}1000m depth. (5) In collaboration with Prof. Jill Pasteris (Washington University) we have successfully accomplished the first field test of a deep ocean laser Raman spectrometer for probing in situ the physical chemistry of the CO{sub 2} system. (6) Submitted the first major paper on biological impacts as determined from our field studies. (7) Submitted a paper on our measurements of the fate of a rising stream of liquid CO{sub 2} droplets to Environmental Science & Technology. (8) Have had accepted for publication in Eos the first brief account of the laser Raman spectrometer success. (9) Have had two papers submitted for the Greenhouse Gas Technology--6 Conference (Kyoto) accepted. (10) Been nominated by the U.S. Dept. of State to attend the Nov. 2002 IPCC Workshop on Carbon Capture and Storage. (11) Given presentations at national meetings, including the AGU Ocean Sciences Meeting, the American Chemical Society, the Minerals, Materials, and Metals Society, the National Academy of Engineering, and given numerous invited lectures.« less
Carbon degassing from the lithosphere
NASA Astrophysics Data System (ADS)
Mörner, Nils-Axel; Etiope, Giuseppe
2002-06-01
So far, the role of present-day Earth degassing in global C budget and climate effects has been focused to volcanic emissions. The non-volcanic escape of CO 2-CH 4 from the upper mantle, from carbonate bearing rocks in the crust, from hydrocarbon accumulations and from surface deposits and processes is here discussed in detail. An inventory of recent available data is presented. For the first time, a so large quantity of data is considered altogether showing clearly that the geological flux of carbon was previously significantly underestimated. Several lines of evidence show that non-volcanic C fluxes in «colder» environments are much greater than generally assumed. Local and regional data suggest that metamorphic decarbonation, hydrocarbon leakage and mud volcanoes could be significant CO 2-CH 4 sources at global scale. Moreover, extensive surface gas-geochemical observations, including soil-atmosphere flux investigations, open the possibility that ecosystems controlled by biogenic activity (soil, permafrost, seawater) can host important components of endogenous C gas (geogas), even in the absence of surface gas manifestations. This would imply the existence of a geological diffuse, background emission over large areas of our planet. New theories concerning the occurrence of pervasive geogas and lithospheric processes of C-gas production («lithospheric loss in rigidity») can be taken as novel reference and rationale for re-evaluating geological sources of CO 2 and CH 4, and an important endeavour and work prospect for the years to come. Our survey shows that it is still very hard to arrive at a meaningful estimate of the lithospheric non-volcanic degassing into the atmosphere. Orders of 10 2-10 3 Mt CO 2/year can be provisionally considered. Assuming as lower limit for a global subaerial volcanic degassing 300 Mt/year, the lithosphere may emit directly into the atmosphere at least 600 Mt CO 2/year (about 10% of the C source due to deforestation and land-use exchange), an estimate we still consider conservative. It is likely that temporal variations of lithosphere degassing, at Quaternary and secular scale, may influence the atmospheric C budget. The present-day lithosphere degassing would seem higher than the value considered to balance at Ma time-scale the CO 2 uptake due to silicate weathering.
NASA Astrophysics Data System (ADS)
Heath, J. E.; Dewers, T. A.; McPherson, B. J.; Wilson, T. H.; Flach, T.
2009-12-01
Understanding and characterizing transport properties of fine-grained rocks is critical in development of shale gas plays or assessing retention of CO2 at geologic storage sites. Difficulties arise in that both small scale (i.e., ~ nm) properties of the rock matrix and much larger scale fractures, faults, and sedimentological architecture govern migration of multiphase fluids. We present a multi-scale investigation of sealing and transport properties of the Kirtland Formation, which is a regional aquitard and reservoir seal in the San Juan Basin, USA. Sub-micron dual FIB/SEM imaging and reconstruction of 3D pore networks in core samples reveal a variety of pore types, including slit-shaped pores that are co-located with sedimentary structures and variations in mineralogy. Micron-scale chemical analysis and XRD reveal a mixture of mixed-layer smectite/illite, chlorite, quartz, and feldspar with little organic matter. Analysis of sub-micron digital reconstructions, mercury capillary injection pressure, and gas breakthrough measurements indicate a high quality sealing matrix. Natural full and partially mineralized fractures observed in core and in FMI logs include those formed from early soil-forming processes, differential compaction, and tectonic events. The potential impact of both fracture and matrix properties on large-scale transport is investigated through an analysis of natural helium from core samples, 3D seismic data and poro-elastic modeling. While seismic interpretations suggest considerable fracturing of the Kirtland, large continuous fracture zones and faults extending through the seal to the surface cannot be inferred from the data. Observed Kirtland Formation multi-scale transport properties are included as part of a risk assessment methodology for CO2 storage. Acknowledgements: The authors gratefully acknowledge the U.S. Department of Energy’s (DOE) National Energy Technology Laboratory for sponsoring this project. The DOE’s Basic Energy Science Office funded the dual FIB/SEM analysis. The Kirtland Formation overlies the coal seams of the Fruitland into which CO2 has been injected as a Phase II demonstration of the Southwest Regional Partnership on Carbon Sequestration. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the U.S. Department of Energy under contract DE-ACOC4-94AL85000.
Rasilo, Terhi; Prairie, Yves T; Del Giorgio, Paul A
2015-03-01
Lakes are a major component of boreal landscapes, and whereas lake CO2 emissions are recognized as a major component of regional C budgets, there is still much uncertainty associated to lake CH4 fluxes. Here, we present a large-scale study of the magnitude and regulation of boreal lake summer diffusive CH4 fluxes, and their contribution to total lake carbon (C) emissions, based on in situ measurements of concentration and fluxes of CH4 and CO2 in 224 lakes across a wide range of lake type and environmental gradients in Québec. The diffusive CH4 flux was highly variable (mean 11.6 ± 26.4 SD mg m(-2) d(-1) ), and it was positively correlated with temperature and lake nutrient status, and negatively correlated with lake area and colored dissolved organic matter (CDOM). The relationship between CH4 and CO2 concentrations fluxes was weak, suggesting major differences in their respective sources and/or regulation. For example, increasing water temperature leads to higher CH4 flux but does not significantly affect CO2 flux, whereas increasing CDOM concentration leads to higher CO2 flux but lower CH4 flux. CH4 contributed to 8 ± 23% to the total lake C emissions (CH4 + CO2 ), but 18 ± 25% to the total flux in terms of atmospheric warming potential, expressed as CO2 -equivalents. The incorporation of ebullition and plant-mediated CH4 fluxes would further increase the importance of lake CH4 . The average Q10 of CH4 flux was 3.7, once other covarying factors were accounted for, but this apparent Q10 varied with lake morphometry and was higher for shallow lakes. We conclude that global climate change and the resulting shifts in temperature will strongly influence lake CH4 fluxes across the boreal biome, but these climate effects may be altered by regional patterns in lake morphometry, nutrient status, and browning. © 2014 John Wiley & Sons Ltd.
The Geomechanics of CO 2 Storage in Deep Sedimentary Formations
DOE Office of Scientific and Technical Information (OSTI.GOV)
Rutqvist, Jonny
2012-01-12
This study provides a review of the geomechanics and modeling of geomechanics associated with geologic carbon storage (GCS), focusing on storage in deep sedimentary formations, in particular saline aquifers. The paper first introduces the concept of storage in deep sedimentary formations, the geomechanical processes and issues related with such an operation, and the relevant geomechanical modeling tools. This is followed by a more detailed review of geomechanical aspects, including reservoir stress-strain and microseismicity, well integrity, caprock sealing performance, and the potential for fault reactivation and notable (felt) seismic events. Geomechanical observations at current GCS field deployments, mainly at the Inmore » Salah CO 2 storage project in Algeria, are also integrated into the review. The In Salah project, with its injection into a relatively thin, low-permeability sandstone is an excellent analogue to the saline aquifers that might be used for large scale GCS in parts of Northwest Europe, the U.S. Midwest, and China. Some of the lessons learned at In Salah related to geomechanics are discussed, including how monitoring of geomechanical responses is used for detecting subsurface geomechanical changes and tracking fluid movements, and how such monitoring and geomechanical analyses have led to preventative changes in the injection parameters. Recently, the importance of geomechanics has become more widely recognized among GCS stakeholders, especially with respect to the potential for triggering notable (felt) seismic events and how such events could impact the long-term integrity of a CO 2 repository (as well as how it could impact the public perception of GCS). As described in the paper, to date, no notable seismic event has been reported from any of the current CO 2 storage projects, although some unfelt microseismic activities have been detected by geophones. However, potential future commercial GCS operations from large power plants will require injection at a much larger scale. In conclusion, for such large-scale injections, a staged, learn-as-you-go approach is recommended, involving a gradual increase of injection rates combined with continuous monitoring of geomechanical changes, as well as siting beneath a multiple layered overburden for multiple flow barrier protection, should an unexpected deep fault reactivation occur.« less
NASA Technical Reports Server (NTRS)
Huang, Jingfeng; Hsu, N. Christina; Tsay, Si-Chee; Zhang, Chidong; Jeong, Myeong Jae; Gautam, Ritesh; Bettenhausen, Corey; Sayer, Andrew M.; Hansell, Richard A.; Liu, Xiaohong;
2012-01-01
One of the seven scientific areas of interests of the 7-SEAS field campaign is to evaluate the impact of aerosol on cloud and precipitation (http://7-seas.gsfc.nasa.gov). However, large-scale covariability between aerosol, cloud and precipitation is complicated not only by ambient environment and a variety of aerosol effects, but also by effects from rain washout and climate factors. This study characterizes large-scale aerosol-cloud-precipitation covariability through synergy of long-term multi ]sensor satellite observations with model simulations over the 7-SEAS region [10S-30N, 95E-130E]. Results show that climate factors such as ENSO significantly modulate aerosol and precipitation over the region simultaneously. After removal of climate factor effects, aerosol and precipitation are significantly anti-correlated over the southern part of the region, where high aerosols loading is associated with overall reduced total precipitation with intensified rain rates and decreased rain frequency, decreased tropospheric latent heating, suppressed cloud top height and increased outgoing longwave radiation, enhanced clear-sky shortwave TOA flux but reduced all-sky shortwave TOA flux in deep convective regimes; but such covariability becomes less notable over the northern counterpart of the region where low ]level stratus are found. Using CO as a proxy of biomass burning aerosols to minimize the washout effect, large-scale covariability between CO and precipitation was also investigated and similar large-scale covariability observed. Model simulations with NCAR CAM5 were found to show similar effects to observations in the spatio-temporal patterns. Results from both observations and simulations are valuable for improving our understanding of this region's meteorological system and the roles of aerosol within it. Key words: aerosol; precipitation; large-scale covariability; aerosol effects; washout; climate factors; 7- SEAS; CO; CAM5
NASA Astrophysics Data System (ADS)
Dekker, Iris N.; Houweling, Sander; Aben, Ilse; Röckmann, Thomas; Krol, Maarten; Martínez-Alonso, Sara; Deeter, Merritt N.; Worden, Helen M.
2017-12-01
The growth of mega-cities leads to air quality problems directly affecting the citizens. Satellite measurements are becoming of higher quality and quantity, which leads to more accurate satellite retrievals of enhanced air pollutant concentrations over large cities. In this paper, we compare and discuss both an existing and a new method for estimating urban-scale trends in CO emissions using multi-year retrievals from the MOPITT satellite instrument. The first method is mainly based on satellite data, and has the advantage of fewer assumptions, but also comes with uncertainties and limitations as shown in this paper. To improve the reliability of urban-to-regional scale emission trend estimation, we simulate MOPITT retrievals using the Weather Research and Forecast model with chemistry core (WRF-Chem). The difference between model and retrieval is used to optimize CO emissions in WRF-Chem, focusing on the city of Madrid, Spain. This method has the advantage over the existing method in that it allows both a trend analysis of CO concentrations and a quantification of CO emissions. Our analysis confirms that MOPITT is capable of detecting CO enhancements over Madrid, although significant differences remain between the yearly averaged model output and satellite measurements (R2 = 0.75) over the city. After optimization, we find Madrid CO emissions to be lower by 48 % for 2002 and by 17 % for 2006 compared with the EdgarV4.2 emission inventory. The MOPITT-derived emission adjustments lead to better agreement with the European emission inventory TNO-MAC-III for both years. This suggests that the downward trend in CO emissions over Madrid is overestimated in EdgarV4.2 and more realistically represented in TNO-MACC-III. However, our satellite and model based emission estimates have large uncertainties, around 20 % for 2002 and 50 % for 2006.
Utilization of Integrated Assessment Modeling for determining geologic CO2 storage security
NASA Astrophysics Data System (ADS)
Pawar, R.
2017-12-01
Geologic storage of carbon dioxide (CO2) has been extensively studied as a potential technology to mitigate atmospheric concentration of CO2. Multiple international research & development efforts, large-scale demonstration and commercial projects are helping advance the technology. One of the critical areas of active investigation is prediction of long-term CO2 storage security and risks. A quantitative methodology for predicting a storage site's long-term performance is critical for making key decisions necessary for successful deployment of commercial scale projects where projects will require quantitative assessments of potential long-term liabilities. These predictions are challenging given that they require simulating CO2 and in-situ fluid movements as well as interactions through the primary storage reservoir, potential leakage pathways (such as wellbores, faults, etc.) and shallow resources such as groundwater aquifers. They need to take into account the inherent variability and uncertainties at geologic sites. This talk will provide an overview of an approach based on integrated assessment modeling (IAM) to predict long-term performance of a geologic storage site including, storage reservoir, potential leakage pathways and shallow groundwater aquifers. The approach utilizes reduced order models (ROMs) to capture the complex physical/chemical interactions resulting due to CO2 movement and interactions but are computationally extremely efficient. Applicability of the approach will be demonstrated through examples that are focused on key storage security questions such as what is the probability of leakage of CO2 from a storage reservoir? how does storage security vary for different geologic environments and operational conditions? how site parameter variability and uncertainties affect storage security, etc.
NASA Astrophysics Data System (ADS)
Raheja, G.; Shusterman, A.; Martin, S.; Shahar, E.; Laughner, J.; Turner, A. J.; Miller, M. K.; Cohen, R. C.
2016-12-01
The Berkeley Atmospheric CO2 Observation Network (BEACO2N) is a high-density network of 28 carbon dioxide sensors distributed around the San Francisco Bay Area that serve to enhance understanding of intra-city variations in CO2 concentrations that are not necessarily captured by sparser networks maintained by local and national air quality management agencies. We partner with designers at the San Francisco Exploratorium to create a suite of interactive exhibits and hands-on activities that creatively visualize data from BEACO2N for general audiences. Museum goers can manipulate a light-up "bar graph" of live CO2 concentrations by exhaling on an in-room sensor, query the current readings of rooftop sensors using a scale model of the Wired Pier observation system, scroll through the data from other BEACO2N sites projected on a 3-D "topographic table" of the Bay Area, and view interpolated CO2 fields driven by research-grade weather models on a nine-screen LCD display. We present lessons learned from these initial installations, from layperson audience feedback to details of the Stochastic Time-Inverted Lagrangian Transport (STILT) model coupled to Weather Research and Forecasting (WRF) weather fields used to generate intuitive concentration maps. We propose that compelling visual demonstrations of elevated CO2 concentrations due to routine small-scale high-emission anthropogenic activities (e.g. rush hour) and/or special events (such as fireworks or factory fires) generate deeper engagement in local environmental issues and interest in undertaking personal actions that can become part of the broader climate solution. While global means and other large-scale aggregate climate metrics can lead to feelings of disconnect and subsequent ambivalence, via such exhibitions, distributed network instruments like BEACO2N can provide the local sensitivity needed to "personalize" greenhouse gas concentrations to a given individual or community and incite the drive toward understanding, education, and action.
Strengthening seasonal marine CO2 variations due to increasing atmospheric CO2
NASA Astrophysics Data System (ADS)
Landschützer, Peter; Gruber, Nicolas; Bakker, Dorothee C. E.; Stemmler, Irene; Six, Katharina D.
2018-01-01
The increase of atmospheric CO2 (ref. 1) has been predicted to impact the seasonal cycle of inorganic carbon in the global ocean2,3, yet the observational evidence to verify this prediction has been missing. Here, using an observation-based product of the oceanic partial pressure of CO2 (pCO2) covering the past 34 years, we find that the winter-to-summer difference of the pCO2 has increased on average by 2.2 ± 0.4 μatm per decade from 1982 to 2015 poleward of 10° latitude. This is largely in agreement with the trend expected from thermodynamic considerations. Most of the increase stems from the seasonality of the drivers acting on an increasing oceanic pCO2 caused by the uptake of anthropogenic CO2 from the atmosphere. In the high latitudes, the concurrent ocean-acidification-induced changes in the buffer capacity of the ocean enhance this effect. This strengthening of the seasonal winter-to-summer difference pushes the global ocean towards critical thresholds earlier, inducing stress to ocean ecosystems and fisheries4. Our study provides observational evidence for this strengthening seasonal difference in the oceanic carbon cycle on a global scale, illustrating the inevitable consequences of anthropogenic CO2 emissions.
Impacts devalue the potential of large-scale terrestrial CO2 removal through biomass plantations
NASA Astrophysics Data System (ADS)
Boysen, L. R.; Lucht, W.; Gerten, D.; Heck, V.
2016-09-01
Large-scale biomass plantations (BPs) are often considered a feasible and safe climate engineering proposal for extracting carbon from the atmosphere and, thereby, reducing global mean temperatures. However, the capacity of such terrestrial carbon dioxide removal (tCDR) strategies and their larger Earth system impacts remain to be comprehensively studied—even more so under higher carbon emissions and progressing climate change. Here, we use a spatially explicit process-based biosphere model to systematically quantify the potentials and trade-offs of a range of BP scenarios dedicated to tCDR, representing different assumptions about which areas are convertible. Based on a moderate CO2 concentration pathway resulting in a global mean warming of 2.5 °C above preindustrial level by the end of this century—similar to the Representative Concentration Pathway (RCP) 4.5—we assume tCDR to be implemented when a warming of 1.5 °C is reached in year 2038. Our results show that BPs can slow down the progression of increasing cumulative carbon in the atmosphere only sufficiently if emissions are reduced simultaneously like in the underlying RCP4.5 trajectory. The potential of tCDR to balance additional, unabated emissions leading towards a business-as-usual pathway alike RCP8.5 is therefore very limited. Furthermore, in the required large-scale applications, these plantations would induce significant trade-offs with food production and biodiversity and exert impacts on forest extent, biogeochemical cycles and biogeophysical properties.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lin, John C.; Mallia, Derek V.; Wu, Dien
Despite the need for researchers to understand terrestrial biospheric carbon fluxes to account for carbon cycle feedbacks and predict future CO 2 concentrations, knowledge of these fluxes at the regional scale remains poor. This is particularly true in mountainous areas, where complex meteorology and lack of observations lead to large uncertainties in carbon fluxes. Yet mountainous regions are often where significant forest cover and biomass are found – i.e., areas that have the potential to serve as carbon sinks. As CO 2 observations are carried out in mountainous areas, it is imperative that they are properly interpreted to yield informationmore » about carbon fluxes. In this paper, we present CO 2 observations at three sites in the mountains of the western US, along with atmospheric simulations that attempt to extract information about biospheric carbon fluxes from the CO 2 observations, with emphasis on the observed and simulated diurnal cycles of CO 2. We show that atmospheric models can systematically simulate the wrong diurnal cycle and significantly misinterpret the CO 2 observations, due to erroneous atmospheric flows as a result of terrain that is misrepresented in the model. This problem depends on the selected vertical level in the model and is exacerbated as the spatial resolution is degraded, and our results indicate that a fine grid spacing of ~4 km or less may be needed to simulate a realistic diurnal cycle of CO 2 for sites on top of the steep mountains examined here in the American Rockies. In conclusion, in the absence of higher resolution models, we recommend coarse-scale models to focus on assimilating afternoon CO 2 observations on mountaintop sites over the continent to avoid misrepresentations of nocturnal transport and influence.« less
A review of mineral carbonation technologies to sequester CO2.
Sanna, A; Uibu, M; Caramanna, G; Kuusik, R; Maroto-Valer, M M
2014-12-07
Carbon dioxide (CO2) capture and sequestration includes a portfolio of technologies that can potentially sequester billions of tonnes of CO2 per year. Mineral carbonation (MC) is emerging as a potential CCS technology solution to sequester CO2 from smaller/medium emitters, where geological sequestration is not a viable option. In MC processes, CO2 is chemically reacted with calcium- and/or magnesium-containing materials to form stable carbonates. This work investigates the current advancement in the proposed MC technologies and the role they can play in decreasing the overall cost of this CO2 sequestration route. In situ mineral carbonation is a very promising option in terms of resources available and enhanced security, but the technology is still in its infancy and transport and storage costs are still higher than geological storage in sedimentary basins ($17 instead of $8 per tCO2). Ex situ mineral carbonation has been demonstrated on pilot and demonstration scales. However, its application is currently limited by its high costs, which range from $50 to $300 per tCO2 sequestered. Energy use, the reaction rate and material handling are the key factors hindering the success of this technology. The value of the products seems central to render MC economically viable in the same way as conventional CCS seems profitable only when combined with EOR. Large scale projects such as the Skyonic process can help in reducing the knowledge gaps on MC fundamentals and provide accurate costing and data on processes integration and comparison. The literature to date indicates that in the coming decades MC can play an important role in decarbonising the power and industrial sector.
The co-evolution of social institutions, demography, and large-scale human cooperation.
Powers, Simon T; Lehmann, Laurent
2013-11-01
Human cooperation is typically coordinated by institutions, which determine the outcome structure of the social interactions individuals engage in. Explaining the Neolithic transition from small- to large-scale societies involves understanding how these institutions co-evolve with demography. We study this using a demographically explicit model of institution formation in a patch-structured population. Each patch supports both social and asocial niches. Social individuals create an institution, at a cost to themselves, by negotiating how much of the costly public good provided by cooperators is invested into sanctioning defectors. The remainder of their public good is invested in technology that increases carrying capacity, such as irrigation systems. We show that social individuals can invade a population of asocials, and form institutions that support high levels of cooperation. We then demonstrate conditions where the co-evolution of cooperation, institutions, and demographic carrying capacity creates a transition from small- to large-scale social groups. © 2013 John Wiley & Sons Ltd/CNRS.
A life cycle greenhouse gas inventory of a tree production system
Alissa Kendall; E. Gregory McPherson
2012-01-01
PurposeThis study provides a detailed, process-based life cycle greenhouse gas (GHG) inventory of an ornamental tree production system for urban forestry. The success of large-scale tree planting initiatives for climate protection depends on projects being net sinks for CO2 over their entire life cycle....
Quantifying soil respiration at landscape scales. Chapter 11
John B. Bradford; Michael G. Ryan
2008-01-01
Soil CO2, efflux, or soil respiration, represents a substantial component of carbon cycling in terrestrial ecosystems. Consequently, quantifying soil respiration over large areas and long time periods is an increasingly important goal. However, soil respiration rates vary dramatically in space and time in response to both environmental conditions...
Lee, Won-June; Park, Won-Tae; Park, Sungjun; Sung, Sujin; Noh, Yong-Young; Yoon, Myung-Han
2015-09-09
Ultrathin and dense metal oxide gate di-electric layers are reported by a simple printing of AlOx and HfOx sol-gel precursors. Large-area printed indium gallium zinc oxide (IGZO) thin-film transistor arrays, which exhibit mobilities >5 cm(2) V(-1) s(-1) and gate leakage current of 10(-9) A cm(-2) at a very low operation voltage of 2 V, are demonstrated by continuous simple bar-coated processes. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Molecular Mechanisms in the shock induced decomposition of FOX-7
NASA Astrophysics Data System (ADS)
Mishra, Ankit; Tiwari, Subodh C.; Nakano, Aiichiro; Vashishta, Priya; Kalia, Rajiv; CACS Team
Experimental and first principle computational studies on FOX 7 have either involved a very small system consisting of a few atoms or they did not take into account the decomposition mechanisms under extreme conditions of temperature and pressure. We have performed a large-scale reactive MD simulation using ReaxFF-lg force field to study the shock decomposition of FOX 7. The chemical composition of the principal decomposition products correlates well with experimental observations. Furthermore, we observed that the production of N2 and H2O was inter molecular in nature and was through different chemical pathways. Moreover, the production of CO and CO2 was delayed due to production of large stable C,O atoms cluster. These critical insights into the initial processes involved in the shock induced decomposition of FOX-7 will greatly help in understanding the factors playing an important role in the insensitiveness of this high energy material. This research is supported by AFOSR Award No. FA9550-16-1-0042.
DOE Office of Scientific and Technical Information (OSTI.GOV)
James P. Barry; Peter G. Brewer
OAK-B135 This report summarizes activities and results of investigations of the potential environmental consequences of direct injection of carbon dioxide into the deep-sea as a carbon sequestration method. Results of field experiments using small scale in situ releases of liquid CO2 are described in detail. The major conclusions of these experiments are that mortality rates of deep sea biota will vary depending on the concentrations of CO2 in deep ocean waters that result from a carbon sequestration project. Large changes in seawater acidity and carbon dioxide content near CO2 release sites will likely cause significant harm to deep-sea marine life.more » Smaller changes in seawater chemistry at greater distances from release sites will be less harmful, but may result in significant ecosystem changes.« less
NASA Astrophysics Data System (ADS)
Nakamura, Fumitaka; Dobashi, Kazuhito; Shimoikura, Tomomi; Tanaka, Tomohiro; Onishi, Toshikazu
2017-03-01
We present the results of wide-field 12CO (J=2{--}1) and 13CO (J=2{--}1) observations toward the Aquila Rift and Serpens molecular cloud complexes (25^\\circ < l< 33^\\circ and 1^\\circ < b< 6^\\circ ) at an angular resolution of 3.‧4 (≈ 0.25 pc) and at a velocity resolution of 0.079 km s-1 with velocity coverage of -5 {km} {{{s}}}-1< {V}{LSR}< 35 {km} {{{s}}}-1. We found that the 13CO emission better traces the structures seen in the extinction map, and derived the {X}{13{CO}}-factor of this region. Applying SCIMES to the 13CO data cube, we identified 61 clouds and derived their mass, radii, and line widths. The line width-radius relation of the identified clouds basically follows those of nearby molecular clouds. The majority of the identified clouds are close to virial equilibrium, although the dispersion is large. By inspecting the 12CO channel maps by eye, we found several arcs that are spatially extended to 0.°2-3° in length. In the longitude-velocity diagrams of 12CO, we also found two spatially extended components that appear to converge toward Serpens South and the W40 region. The existence of two components with different velocities and arcs suggests that large-scale expanding bubbles and/or flows play a role in the formation and evolution of the Serpens South and W40 cloud.
NASA Astrophysics Data System (ADS)
Ye, X.; Lauvaux, T.; Kort, E. A.; Lin, J. C.; Oda, T.; Yang, E.; Wu, D.
2016-12-01
Rapid economic development has given rise to a steady increase of global carbon emissions, which have accumulated in the atmosphere for the past 200 years. Urbanization has concentrated about 70% of the global fossil-fuel CO2 emissions in large metropolitan areas distributed around the world, which represents the most significant anthropogenic contribution to climate change. However, highly uncertain quantifications of urban CO2 emissions are commonplace for numerous cities because of poorly-documented inventories of energy consumption. Therefore, accurate estimates of carbon emissions from global observing systems are a necessity if mitigation strategies are meant to be implemented at global scales. Space-based observations of total column averaged CO2 concentration (XCO2) provide a very promising and powerful tool to quantify urban CO2 fluxes. For the first time, measurements from the Orbiting Carbon Observatory 2 (OCO-2) mission are assimilated in a high resolution inverse modeling system to quantify fossil-fuel CO2 emissions of multiple cities around the globe. The Open-source Data Inventory for Anthropogenic CO2 (ODIAC) emission inventory is employed as a first guess, while the atmospheric transport is simulated using the WRF-Chem model at 1-km resolution. Emission detection and quantification is performed with an Ensemble Kalman Filter method. We demonstrate here the potential of the inverse approach for assimilating thousands of OCO-2 retrievals along tracks near metropolitan areas. We present the detection potential of the system with real-case applications near power plants and present inverse emissions using actual OCO-2 measurements on various urban landscapes. Finally, we will discuss the potential of OCO-2-like satellite instruments for monitoring temporal variations of fossil-fuel CO2 emissions over multiple years, which can provide valuable insights for future satellite observation strategies.
Modeling of sonochemistry in water in the presence of dissolved carbon dioxide.
Authier, Olivier; Ouhabaz, Hind; Bedogni, Stefano
2018-07-01
CO 2 capture and utilization (CCU) is a process that captures CO 2 emissions from sources such as fossil fuel power plants and reuses them so that they will not enter the atmosphere. Among the various ways of recycling CO 2 , reduction reactions are extensively studied at lab-scale. However, CO 2 reduction by standard methods is difficult. Sonochemistry may be used in CO 2 gas mixtures bubbled through water subjected to ultrasound waves. Indeed, the sonochemical reduction of CO 2 in water has been already investigated by some authors, showing that fuel species (CO and H 2 ) are obtained in the final products. The aim of this work is to model, for a single bubble, the close coupling of the mechanisms of bubble dynamics with the kinetics of gas phase reactions in the bubble that can lead to CO 2 reduction. An estimation of time-scales is used to define the controlling steps and consequently to solve a reduced model. The calculation of the concentration of free radicals and gases formed in the bubble is undertaken over many cycles to look at the effects of ultrasound frequency, pressure amplitude, initial bubble radius and bubble composition in CO 2 . The strong effect of bubble composition on the CO 2 reduction rate is confirmed in accordance with experimental data from the literature. When the initial fraction of CO 2 in the bubble is low, bubble growth and collapse are slightly modified with respect to simulation without CO 2 , and chemical reactions leading to CO 2 reduction are promoted. However, the peak collapse temperature depends on the thermal properties of the CO 2 and greatly decreases as the CO 2 increases in the bubble. The model shows that initial bubble radius, ultrasound frequency and pressure amplitude play a critical role in CO 2 reduction. Hence, in the case of a bubble with an initial radius of around 5 μm, CO 2 reduction appears to be more favorable at a frequency around 300 kHz than at a low frequency of around 20 kHz. Finally, the industrial application of ultrasound to CO 2 reduction in water would be largely dependent on sonochemical efficiency. Under the conditions tested, this process does not seem to be sufficiently efficient. Copyright © 2018 Elsevier B.V. All rights reserved.
Chen, Huilong; Lu, Shuang; Gong, Feilong; Liu, Huanzhen; Li, Feng
2017-01-01
Three-dimensional hierarchical Co3O4 nanobooks have been synthesized successfully on a large scale by calcining orthorhombic Co(CO3)0.5(OH)·0.11H2O precursors with identical morphologies. Based on the influence of reaction time and urea concentration on the nanostructures of the precursors, a stepwise splitting growth mechanism can be proposed to understand the formation of the 3D nanobooks. The 3D Co3O4 nanobooks exhibit excellent pseudocapacitive performances with specific capacitances of 590, 539, 476, 453, and 421 F/g at current densities of 0.5, 1, 2, 4, and 8 A/g, respectively. The devices can retain ca. 97.4% of the original specific capacitances after undergoing charge–discharge cycle tests 1000 times continuously at 4 A/g. PMID:28394297
NASA Astrophysics Data System (ADS)
Kato, E.; Yamagata, Y.
2014-12-01
Bioenergy with Carbon Capture and Storage (BECCS) is a key component of mitigation strategies in future socio-economic scenarios that aim to keep mean global temperature rise below 2°C above pre-industrial, which would require net negative carbon emissions in the end of the 21st century. Because of the additional need for land, developing sustainable low-carbon scenarios requires careful consideration of the land-use implications of deploying large-scale BECCS. We evaluated the feasibility of the large-scale BECCS in RCP2.6, which is a scenario with net negative emissions aiming to keep the 2°C temperature target, with a top-down analysis of required yields and a bottom-up evaluation of BECCS potential using a process-based global crop model. Land-use change carbon emissions related to the land expansion were examined using a global terrestrial biogeochemical cycle model. Our analysis reveals that first-generation bioenergy crops would not meet the required BECCS of the RCP2.6 scenario even with a high fertilizer and irrigation application. Using second-generation bioenergy crops can marginally fulfill the required BECCS only if a technology of full post-process combustion CO2 capture is deployed with a high fertilizer application in the crop production. If such an assumed technological improvement does not occur in the future, more than doubling the area for bioenergy production for BECCS around 2050 assumed in RCP2.6 would be required, however, such scenarios implicitly induce large-scale land-use changes that would cancel half of the assumed CO2 sequestration by BECCS. Otherwise a conflict of land-use with food production is inevitable.
NASA Astrophysics Data System (ADS)
Kato, Etsushi; Yamagata, Yoshiki
2014-09-01
Bioenergy with Carbon Capture and Storage (BECCS) is a key component of mitigation strategies in future socioeconomic scenarios that aim to keep mean global temperature rise below 2°C above preindustrial, which would require net negative carbon emissions in the end of the 21st century. Because of the additional need for land, developing sustainable low-carbon scenarios requires careful consideration of the land-use implications of deploying large scale BECCS. We evaluated the feasibility of the large-scale BECCS in RCP2.6, which is a scenario with net negative emissions aiming to keep the 2°C temperature target, with a top-down analysis of required yields and a bottom-up evaluation of BECCS potential using a process-based global crop model. Land-use change carbon emissions related to the land expansion were examined using a global terrestrial biogeochemical cycle model. Our analysis reveals that first-generation bioenergy crops would not meet the required BECCS of the RCP2.6 scenario even with a high-fertilizer and irrigation application. Using second-generation bioenergy crops can marginally fulfill the required BECCS only if a technology of full postprocess combustion CO2 capture is deployed with a high-fertilizer application in the crop production. If such an assumed technological improvement does not occur in the future, more than doubling the area for bioenergy production for BECCS around 2050 assumed in RCP2.6 would be required; however, such scenarios implicitly induce large-scale land-use changes that would cancel half of the assumed CO2 sequestration by BECCS. Otherwise, a conflict of land use with food production is inevitable.
Large-scale bioenergy production: how to resolve sustainability trade-offs?
NASA Astrophysics Data System (ADS)
Humpenöder, Florian; Popp, Alexander; Bodirsky, Benjamin Leon; Weindl, Isabelle; Biewald, Anne; Lotze-Campen, Hermann; Dietrich, Jan Philipp; Klein, David; Kreidenweis, Ulrich; Müller, Christoph; Rolinski, Susanne; Stevanovic, Miodrag
2018-02-01
Large-scale 2nd generation bioenergy deployment is a key element of 1.5 °C and 2 °C transformation pathways. However, large-scale bioenergy production might have negative sustainability implications and thus may conflict with the Sustainable Development Goal (SDG) agenda. Here, we carry out a multi-criteria sustainability assessment of large-scale bioenergy crop production throughout the 21st century (300 EJ in 2100) using a global land-use model. Our analysis indicates that large-scale bioenergy production without complementary measures results in negative effects on the following sustainability indicators: deforestation, CO2 emissions from land-use change, nitrogen losses, unsustainable water withdrawals and food prices. One of our main findings is that single-sector environmental protection measures next to large-scale bioenergy production are prone to involve trade-offs among these sustainability indicators—at least in the absence of more efficient land or water resource use. For instance, if bioenergy production is accompanied by forest protection, deforestation and associated emissions (SDGs 13 and 15) decline substantially whereas food prices (SDG 2) increase. However, our study also shows that this trade-off strongly depends on the development of future food demand. In contrast to environmental protection measures, we find that agricultural intensification lowers some side-effects of bioenergy production substantially (SDGs 13 and 15) without generating new trade-offs—at least among the sustainability indicators considered here. Moreover, our results indicate that a combination of forest and water protection schemes, improved fertilization efficiency, and agricultural intensification would reduce the side-effects of bioenergy production most comprehensively. However, although our study includes more sustainability indicators than previous studies on bioenergy side-effects, our study represents only a small subset of all indicators relevant for the SDG agenda. Based on this, we argue that the development of policies for regulating externalities of large-scale bioenergy production should rely on broad sustainability assessments to discover potential trade-offs with the SDG agenda before implementation.
Acceleration of modern acidification in the South China Sea driven by anthropogenic CO2
Liu, Yi; Peng, Zicheng; Zhou, Renjun; Song, Shaohua; Liu, Weiguo; You, Chen-Feng; Lin, Yen-Po; Yu, Kefu; Wu, Chung-Che; Wei, Gangjian; Xie, Luhua; Burr, George S.; Shen, Chuan-Chou
2014-01-01
Modern acidification by the uptake of anthropogenic CO2 can profoundly affect the physiology of marine organisms and the structure of ocean ecosystems. Centennial-scale global and regional influences of anthropogenic CO2 remain largely unknown due to limited instrumental pH records. Here we present coral boron isotope-inferred pH records for two periods from the South China Sea: AD 1048–1079 and AD 1838–2001. There are no significant pH differences between the first period at the Medieval Warm Period and AD 1830–1870. However, we find anomalous and unprecedented acidification during the 20th century, pacing the observed increase in atmospheric CO2. Moreover, pH value also varies in phase with inter-decadal changes in Asian Winter Monsoon intensity. As the level of atmospheric CO2 keeps rising, the coupling global warming via weakening the winter monsoon intensity could exacerbate acidification of the South China Sea and threaten this expansive shallow water marine ecosystem. PMID:24888785
Acceleration of modern acidification in the South China Sea driven by anthropogenic CO2
NASA Astrophysics Data System (ADS)
Liu, Yi; Peng, Zicheng; Zhou, Renjun; Song, Shaohua; Liu, Weiguo; You, Chen-Feng; Lin, Yen-Po; Yu, Kefu; Wu, Chung-Che; Wei, Gangjian; Xie, Luhua; Burr, George S.; Shen, Chuan-Chou
2014-06-01
Modern acidification by the uptake of anthropogenic CO2 can profoundly affect the physiology of marine organisms and the structure of ocean ecosystems. Centennial-scale global and regional influences of anthropogenic CO2 remain largely unknown due to limited instrumental pH records. Here we present coral boron isotope-inferred pH records for two periods from the South China Sea: AD 1048-1079 and AD 1838-2001. There are no significant pH differences between the first period at the Medieval Warm Period and AD 1830-1870. However, we find anomalous and unprecedented acidification during the 20th century, pacing the observed increase in atmospheric CO2. Moreover, pH value also varies in phase with inter-decadal changes in Asian Winter Monsoon intensity. As the level of atmospheric CO2 keeps rising, the coupling global warming via weakening the winter monsoon intensity could exacerbate acidification of the South China Sea and threaten this expansive shallow water marine ecosystem.
Shim, Hyun-Woo; Lim, Ah-Hyeon; Kim, Jae-Chan; Jang, Eunjin; Seo, Seung-Deok; Lee, Gwang-Hee; Kim, T. Doohun; Kim, Dong-Wan
2013-01-01
Template-driven strategy has been widely used to synthesize inorganic nano/micro materials. Here, we used a bottom-up controlled synthesis route to develop a powerful solution-based method of fabricating three-dimensional (3D), hierarchical, porous-Co3O4 superstructures that exhibit the morphology of flower-like microspheres (hereafter, RT-Co3O4). The gram-scale RT-Co3O4 was facilely prepared using one-pot synthesis with bacterial templating at room temperature. Large-surface-area RT-Co3O4 also has a noticeable pseudocapacitive performance because of its high mass loading per area (~10 mg cm−2), indicating a high capacitance of 214 F g−1 (2.04 F cm−2) at 2 A g−1 (19.02 mA cm−2), a Coulombic efficiency averaging over 95%, and an excellent cycling stability that shows a capacitance retention of about 95% after 4,000 cycles. PMID:23900049
DOE Office of Scientific and Technical Information (OSTI.GOV)
Liu, Shaoqing; Zhuang, Qianlai; Chen, Min
Current terrestrial ecosystem models are usually driven with global average annual atmospheric carbon dioxide (CO 2) concentration data at the global scale. However, high-precision CO 2 measurement from eddy flux towers showed that seasonal, spatial surface atmospheric CO 2 concentration differences were as large as 35 ppmv and the site-level tests indicated that the CO 2 variation exhibited different effects on plant photosynthesis. Here we used a process-based ecosystem model driven with two spatially and temporally explicit CO 2 data sets to analyze the atmospheric CO 2 fertilization effects on the global carbon dynamics of terrestrial ecosystems from 2003 tomore » 2010. Our results demonstrated that CO 2 seasonal variation had a negative effect on plant carbon assimilation, while CO2 spatial variation exhibited a positive impact. When both CO 2 seasonal and spatial effects were considered, global gross primary production and net ecosystem production were 1.7 Pg C•yr –1 and 0.08 Pg C•yr –1 higher than the simulation using uniformly distributed CO 2 data set and the difference was significant in tropical and temperate evergreen broadleaf forest regions. Moreover, this study suggests that the CO 2 observation network should be expanded so that the realistic CO 2 variation can be incorporated into the land surface models to adequately account for CO 2 fertilization effects on global terrestrial ecosystem carbon dynamics.« less
Liu, Shaoqing; Zhuang, Qianlai; Chen, Min; ...
2016-07-25
Current terrestrial ecosystem models are usually driven with global average annual atmospheric carbon dioxide (CO 2) concentration data at the global scale. However, high-precision CO 2 measurement from eddy flux towers showed that seasonal, spatial surface atmospheric CO 2 concentration differences were as large as 35 ppmv and the site-level tests indicated that the CO 2 variation exhibited different effects on plant photosynthesis. Here we used a process-based ecosystem model driven with two spatially and temporally explicit CO 2 data sets to analyze the atmospheric CO 2 fertilization effects on the global carbon dynamics of terrestrial ecosystems from 2003 tomore » 2010. Our results demonstrated that CO 2 seasonal variation had a negative effect on plant carbon assimilation, while CO2 spatial variation exhibited a positive impact. When both CO 2 seasonal and spatial effects were considered, global gross primary production and net ecosystem production were 1.7 Pg C•yr –1 and 0.08 Pg C•yr –1 higher than the simulation using uniformly distributed CO 2 data set and the difference was significant in tropical and temperate evergreen broadleaf forest regions. Moreover, this study suggests that the CO 2 observation network should be expanded so that the realistic CO 2 variation can be incorporated into the land surface models to adequately account for CO 2 fertilization effects on global terrestrial ecosystem carbon dynamics.« less
Driving terrestrial ecosystem models from space
NASA Technical Reports Server (NTRS)
Waring, R. H.
1993-01-01
Regional air pollution, land-use conversion, and projected climate change all affect ecosystem processes at large scales. Changes in vegetation cover and growth dynamics can impact the functioning of ecosystems, carbon fluxes, and climate. As a result, there is a need to assess and monitor vegetation structure and function comprehensively at regional to global scales. To provide a test of our present understanding of how ecosystems operate at large scales we can compare model predictions of CO2, O2, and methane exchange with the atmosphere against regional measurements of interannual variation in the atmospheric concentration of these gases. Recent advances in remote sensing of the Earth's surface are beginning to provide methods for estimating important ecosystem variables at large scales. Ecologists attempting to generalize across landscapes have made extensive use of models and remote sensing technology. The success of such ventures is dependent on merging insights and expertise from two distinct fields. Ecologists must provide the understanding of how well models emulate important biological variables and their interactions; experts in remote sensing must provide the biophysical interpretation of complex optical reflectance and radar backscatter data.
Stocker, Benjamin David; Yu, Zicheng; Massa, Charly; Joos, Fortunat
2017-02-14
CO 2 emissions from preindustrial land-use change (LUC) are subject to large uncertainties. Although atmospheric CO 2 records suggest only a small land carbon (C) source since 5,000 y before present (5 kyBP), the concurrent C sink by peat buildup could mask large early LUC emissions. Here, we combine updated continuous peat C reconstructions with the land C balance inferred from double deconvolution analyses of atmospheric CO 2 and [Formula: see text]C at different temporal scales to investigate the terrestrial C budget of the Holocene and the last millennium and constrain LUC emissions. LUC emissions are estimated with transient model simulations for diverging published scenarios of LU area change and shifting cultivation. Our results reveal a large terrestrial nonpeatland C source after the Mid-Holocene (66 [Formula: see text] 25 PgC at 7-5 kyBP and 115 [Formula: see text] 27 PgC at 5-3 kyBP). Despite high simulated per-capita CO 2 emissions from LUC in early phases of agricultural development, humans emerge as a driver with dominant global C cycle impacts only in the most recent three millennia. Sole anthropogenic causes for particular variations in the CO 2 record ([Formula: see text]20 ppm rise after 7 kyBP and [Formula: see text]10 ppm fall between 1500 CE and 1600 CE) are not supported. This analysis puts a strong constraint on preindustrial vs. industrial-era LUC emissions and suggests that upper-end scenarios for the extent of agricultural expansion before 1850 CE are not compatible with the C budget thereafter.
Ship-in-a-bottle synthesis of amine-functionalized ionic liquids in NaY zeolite for CO2 capture
Yu, Yinghao; Mai, Jingzhang; Wang, Lefu; Li, Xuehui; Jiang, Zheng; Wang, Furong
2014-01-01
CO2 capture on solid materials possesses significant advantages on the operation cost, process for large-scale CO2 capture and storage (CCS) that stimulates great interest in exploring high-performance solid CO2 adsorbents. A ship-in-a-bottle strategy was successfully developed to prepare the [APMIM]Br@NaY host–guest system in which an amine-functionalized ionic liquid (IL), 1-aminopropyl-3-methylimidazolium bromide ([APMIM]Br), was in-situ encapsulated in the NaY supercages. The genuine host-guest systems were thoroughly characterized and tested in CO2 capture from simulated flue gas. It was evidenced the encapsulated ILs are more stable than the bulk ILs. These host–guest systems exhibited superb overall CO2 capture capacity up to 4.94 mmol g−1 and the chemically adsorbed CO2 achieved 1.85 mmol g−1 depending on the [APMIM]Br loading amount. The chemisorbed CO2 can be desorbed rapidly by flushing with N2 gas at 50°C. The optimized [APMIM]Br@NaY system remains its original CO2 capture capacity in multiple cycling tests under prolonged harsh adsorption-desorption conditions. The excellent physicochemical properties and the CO2 capture performance of the host-guest systems offer them great promise for the future practice in the industrial CO2 capture. PMID:25104324
NASA Astrophysics Data System (ADS)
Stuart, Jessica F.
The primary focus of this work has been to develop high-energy capacity batteries capable of undergoing multiple electron charge transfer redox reactions to address the growing demand for improved electrical energy storage systems that can be applied to a range of applications. As the levels of carbon dioxide (CO2) increase in the Earth's atmosphere, the effects on climate change become increasingly apparent. According to the Energy Information Administration (EIA), the U.S. electric power sector is responsible for the release of 2,039 million metric tons of CO2 annually, equating to 39% of total U.S. energy-related CO2 emissions. Both nationally and abroad, there are numerous issues associated with the generation and use of electricity aside from the overwhelming dependence on fossil fuels and the subsequent carbon emissions, including reliability of the grid and the utilization of renewable energies. Renewable energy makes up a relatively small portion of total energy contributions worldwide, accounting for only 13% of the 3,955 billion kilowatt-hours of electricity produced each year, as reported by the EIA. As the demand to reduce our dependence on fossils fuels and transition to renewable energy sources increases, cost effective large-scale electrical energy storage must be established for renewable energy to become a sustainable option for the future. A high capacity energy storage system capable of leveling the intermittent nature of energy sources such as solar, wind, and water into the electric grid and provide electricity at times of high demand will facilitate this transition. In 2008, the Licht Group presented the highest volumetric energy capacity battery, the vanadium diboride (VB2) air battery, exceedingly proficient in transferring eleven electrons per molecule. This body of work focuses on new developments to this early battery such as fundamentally understanding the net discharge mechanism of the system, evaluation of the properties and performance of nanoscopic anodic materials in addition to the previously developed macroscopic system, as well as the exploration of a high-energy capacity TiB 2/VB2 composite anode. However, the greatest challenge to this room temperature VB2 primary battery is to develop a means to electrochemically recharge the anodic material (how to reinsert the eleven electrons per molecule that are removed during the battery's discharge). Rechargeable batteries, such as the new molten air battery presented in this thesis, offer a high intrinsic capacity mode for energy storage and overcome problems such as the need for higher energy capacity, cost-effective batteries for a range of electronic, transportation, and large-scale power storage devices. Molten air batteries presented and discussed in this work are viable systems that provide a means to electrochemically recharge the VB2-air battery and deliver large-scale energy storage due to their scalability, location flexibility, construction from readily available resources, and offer increased energy storage capacity for the electric grid. One example is the VB2 molten air battery, which discharges according to: VB 2 + 11/4 O2 → 1/ 2 V2O5 + B2O3 (1). Previously, our group has shown that carbon dioxide can be captured from atmospheric air concentrations at solar efficiencies as high as 50%, and that carbon dioxide emissions associated with the production of several commodities can be electrochemically avoided in by the Solar Thermal Electrochemical Process (STEP). Utilizing this process, the carbon molten air battery relies on carbon dioxide directly from the air: Charging: CO2 (g) → C (solid) + O2 (g) (2) Discharging: C (solid) + O2 (g) → CO2 (g) (3). More specifically, in a molten carbonate electrolyte containing added oxide, such as lithium carbonate with lithium oxide, the four-electron charging reaction, Equation 2, approaches 100% faradic efficiency and can be described as the following two equations: O2- (dissolved) + CO2 (g) → CO 32- (molten) (2a) CO32- (molten) ?→ C (solid) + O2 (g) + O2- (dissolved) (2b). Thus, powered by the oxidation of carbon formed directly from the CO 2 in our earth's atmosphere, the carbon molten air battery is a viable system to provide large-scale energy storage. These batteries are rechargeable and have amongst the highest intrinsic battery storage capacities available. The electron charge transfer chemistry is demonstrated through three examples. These examples utilize iron, carbon, and vanadium diboride as reactive materials, each containing intrinsic volumetric energy capacities of 10,000 Wh/L for Fe to Fe (III), 19,000 Wh/L for C to CO2, and 27,000 Wh/L for VB2 to B2O3 and V2O 5, compared to 6,200 Wh/L for the lithium air battery.
NASA Astrophysics Data System (ADS)
Cyronak, T.; Santos, I. R.; Erler, D.; Maher, D. T.; Eyre, B.
2013-12-01
The carbon chemistry of coral reef lagoons can be highly variable over short time scales. While much of the diel variability in seawater carbon chemistry is explained by biological processes, external sources such as river and groundwater seepage may deliver large amounts of organic and inorganic carbon to coral reefs and represent a poorly understood feedback to ocean acidification. Here, we assess the impact of submarine groundwater discharge (SGD) on pCO2 variability in two coral reef lagoons with distinct SGD driving mechanisms. Diel variability of pCO2 in the two ecosystems was explained by a combination of biological drivers and SGD inputs. In Rarotonga, a South Pacific volcanic island, SGD was driven primarily by a steep terrestrial hydraulic gradient, and the lagoon was influenced by the high pCO2 (5,501 μatm) of the fresh groundwater. In Heron Island, a Great Barrier Reef coral cay, SGD was dominated by seawater recirculation through sediments (i.e. tidal pumping) and pCO2 was mainly impacted through the stimulation of biological processes. The Rarotonga water column had a relatively higher average pCO2 (549 μatm) than Heron Island (471 μatm). However, pCO2 exhibited a greater diel range in Heron Island (778 μatm) than in Rarotonga (507 μatm). The Rarotonga lagoon received 31.2 mmol CO2 m-2 d-1 from SGD, while the Heron Island lagoon received 12.3 mmol CO2 m-2 d-1. Over the course of this study both systems were sources of CO2 to the atmosphere (3.00 to 9.67 mmol CO2 m-2 d-1), with SGD-derived CO2 contributing a large portion to the air-sea CO2 flux. The relationship between both water column pH and aragonite saturation state (ΩAr) and radon (222Rn) concentrations indicate that SGD may enhance the local acidification of some coral reef lagoons. Studies measuring the carbon chemistry of coral reefs (e.g. community metabolism, calcification rates) may need to consider SGD-derived CO2.
A Global Perspective of Atmospheric CO2 Concentrations
NASA Technical Reports Server (NTRS)
Putman, William M.; Ott, Lesley; Darmenov, Anton; daSilva, Arlindo
2016-01-01
Carbon dioxide (CO2) is the most important greenhouse gas affected by human activity. About half of the CO2 emitted from fossil fuel combustion remains in the atmosphere, contributing to rising temperatures, while the other half is absorbed by natural land and ocean carbon reservoirs. Despite the importance of CO2, many questions remain regarding the processes that control these fluxes and how they may change in response to a changing climate. The Orbiting Carbon Observatory-2 (OCO-2), launched on July 2, 2014, is NASA's first satellite mission designed to provide the global view of atmospheric CO2 needed to better understand both human emissions and natural fluxes. This visualization shows how column CO2 mixing ratio, the quantity observed by OCO-2, varies throughout the year. By observing spatial and temporal gradients in CO2 like those shown, OCO-2 data will improve our understanding of carbon flux estimates. But, CO2 observations can't do that alone. This visualization also shows that column CO2 mixing ratios are strongly affected by large-scale weather systems. In order to fully understand carbon flux processes, OCO-2 observations and atmospheric models will work closely together to determine when and where observed CO2 came from. Together, the combination of high-resolution data and models will guide climate models towards more reliable predictions of future conditions.
SPECTRAL LINE DE-CONFUSION IN AN INTENSITY MAPPING SURVEY
DOE Office of Scientific and Technical Information (OSTI.GOV)
Cheng, Yun-Ting; Bock, James; Bradford, C. Matt
2016-12-01
Spectral line intensity mapping (LIM) has been proposed as a promising tool to efficiently probe the cosmic reionization and the large-scale structure. Without detecting individual sources, LIM makes use of all available photons and measures the integrated light in the source confusion limit to efficiently map the three-dimensional matter distribution on large scales as traced by a given emission line. One particular challenge is the separation of desired signals from astrophysical continuum foregrounds and line interlopers. Here we present a technique to extract large-scale structure information traced by emission lines from different redshifts, embedded in a three-dimensional intensity mapping data cube.more » The line redshifts are distinguished by the anisotropic shape of the power spectra when projected onto a common coordinate frame. We consider the case where high-redshift [C ii] lines are confused with multiple low-redshift CO rotational lines. We present a semi-analytic model for [C ii] and CO line estimates based on the cosmic infrared background measurements, and show that with a modest instrumental noise level and survey geometry, the large-scale [C ii] and CO power spectrum amplitudes can be successfully extracted from a confusion-limited data set, without external information. We discuss the implications and limits of this technique for possible LIM experiments.« less
NASA Astrophysics Data System (ADS)
Andrews, A. E.; Hu, L.; Thoning, K. W.; Nehrkorn, T.; Mountain, M. E.; Jacobson, A. R.; Michalak, A.; Dlugokencky, E. J.; Sweeney, C.; Worthy, D. E. J.; Miller, J. B.; Fischer, M. L.; Biraud, S.; van der Velde, I. R.; Basu, S.; Tans, P. P.
2017-12-01
CarbonTracker-Lagrange (CT-L) is a new high-resolution regional inverse modeling system for improved estimation of North American CO2 fluxes. CT-L uses footprints from the Stochastic Time-Inverted Lagrangian Transport (STILT) model driven by high-resolution (10 to 30 km) meteorological fields from the Weather Research and Forecasting (WRF) model. We performed a suite of synthetic-data experiments to evaluate a variety of inversion configurations, including (1) solving for scaling factors to an a priori flux versus additive corrections, (2) solving for fluxes at 3-hrly resolution versus at coarser temporal resolution, (3) solving for fluxes at 1o × 1o resolution versus at large eco-regional scales. Our framework explicitly and objectively solves for the optimal solution with a full error covariance matrix with maximum likelihood estimation, thereby enabling rigorous uncertainty estimates for the derived fluxes. In the synthetic-data inversions, we find that solving for weekly scaling factors of a priori Net Ecosystem Exchange (NEE) at 1o × 1o resolution with optimization of diurnal cycles of CO2 fluxes yields faithful retrieval of the specified "true" fluxes as those solved at 3-hrly resolution. In contrast, a scheme that does not allow for optimization of diurnal cycles of CO2 fluxes suffered from larger aggregation errors. We then applied the optimal inversion setup to estimate North American fluxes for 2007-2015 using real atmospheric CO2 observations, multiple prior estimates of NEE, and multiple boundary values estimated from the NOAA's global Eulerian CarbonTracker (CarbonTracker) and from an empirical approach. Our derived North American land CO2 fluxes show larger seasonal amplitude than those estimated from the CarbonTracker, removing seasonal biases in the CarbonTracker's simulated CO2 mole fractions. Independent evaluations using in-situ CO2 eddy covariance flux measurements and independent aircraft profiles also suggest an improved estimation on North American CO2 fluxes from CT-L. Furthermore, our derived CO2 flux anomalies over North America corresponding to the 2012 North American drought and the 2015 El Niño are larger than derived by the CarbonTracker. They also indicate different responses of ecosystems to those anomalous climatic events.
Large-scale phase separation with nano-twin domains in manganite spinel (Co,Fe,Mn){sub 3}O{sub 4}
DOE Office of Scientific and Technical Information (OSTI.GOV)
Horibe, Y., E-mail: horibe@post.matsc.kyutech.ac.jp; Takeyama, S.; Mori, S.
The effect of Mn concentration on the formation of nano-domain structures in the spinel oxide (Co,Fe,Mn){sub 3}O{sub 4} was investigated by electron diffraction, bright-, and dark-field imaging technique with transmission electron microscopy. Large scale phase separation with nano-twin domains was observed in Co{sub 0.6}Fe{sub 1.0}Mn{sub 1.4}O{sub 4}, in contrast to the highly aligned checkerboard nano-domains in Co{sub 0.6}Fe{sub 0.9}Mn{sub 1.5}O{sub 4}. Diffusion of the Mn{sup 3+} ions with the Jahn-Teller distortions is suggested to play an important role in the formation of checkerboard nano-domain structure.
Ito, Akihiko; Inatomi, Motoko; Huntzinger, Deborah N.; ...
2016-05-12
The seasonal-cycle amplitude (SCA) of the atmosphere–ecosystem carbon dioxide (CO 2) exchange rate is a useful metric of the responsiveness of the terrestrial biosphere to environmental variations. It is unclear, however, what underlying mechanisms are responsible for the observed increasing trend of SCA in atmospheric CO 2 concentration. Using output data from the Multi-scale Terrestrial Model Intercomparison Project (MsTMIP), we investigated how well the SCA of atmosphere–ecosystem CO 2 exchange was simulated with 15 contemporary terrestrial ecosystem models during the period 1901–2010. Also, we made attempt to evaluate the contributions of potential mechanisms such as atmospheric CO 2, climate, land-use,more » and nitrogen deposition, through factorial experiments using different combinations of forcing data. Under contemporary conditions, the simulated global-scale SCA of the cumulative net ecosystem carbon flux of most models was comparable in magnitude with the SCA of atmospheric CO 2 concentrations. Results from factorial simulation experiments showed that elevated atmospheric CO 2 exerted a strong influence on the seasonality amplification. When the model considered not only climate change but also land-use and atmospheric CO 2 changes, the majority of the models showed amplification trends of the SCAs of photosynthesis, respiration, and net ecosystem production (+0.19 % to +0.50 % yr –1). In the case of land-use change, it was difficult to separate the contribution of agricultural management to SCA because of inadequacies in both the data and models. The simulated amplification of SCA was approximately consistent with the observational evidence of the SCA in atmospheric CO 2 concentrations. Large inter-model differences remained, however, in the simulated global tendencies and spatial patterns of CO 2 exchanges. Further studies are required to identify a consistent explanation for the simulated and observed amplification trends, including their underlying mechanisms. Furthermore, this study implied that monitoring of ecosystem seasonality would provide useful insights concerning ecosystem dynamics.« less
NASA Astrophysics Data System (ADS)
Zhao, Y.; Qiu, L. P.; Xu, R. Y.; Xie, F. J.; Zhang, Q.; Yu, Y. Y.; Nielsen, C. P.; Qin, H. X.; Wang, H. K.; Wu, X. C.; Li, W. Q.; Zhang, J.
2015-11-01
With most eastern Chinese cities facing major air quality challenges, there is a strong need for city-scale emission inventories for use in both chemical transport modeling and the development of pollution control policies. In this paper, a high-resolution emission inventory (with a horizontal resolution of 3 × 3 km) of air pollutants and CO2 for Nanjing, a typical large city in the Yangtze River Delta, is developed, incorporating the best available information on local sources. Emission factors and activity data at the unit or facility level are collected and compiled using a thorough on-site survey of major sources. Over 900 individual plants, which account for 97 % of the city's total coal consumption, are identified as point sources, and all of the emission-related parameters including combustion technology, fuel quality, and removal efficiency of air pollution control devices (APCD) are analyzed. New data-collection approaches including continuous emission monitoring systems and real-time monitoring of traffic flows are employed to improve spatiotemporal distribution of emissions. Despite fast growth of energy consumption between 2010 and 2012, relatively small interannual changes in emissions are found for most air pollutants during this period, attributed mainly to benefits of growing APCD deployment and the comparatively strong and improving regulatory oversight of the large point sources that dominate the levels and spatial distributions of Nanjing emissions overall. The improvement of this city-level emission inventory is indicated by comparisons with observations and other inventories at larger spatial scale. Relatively good spatial correlations are found for SO2, NOx, and CO between the city-scale emission estimates and concentrations at nine state-operated monitoring sites (R = 0.58, 0.46, and 0.61, respectively). The emission ratios of specific pollutants including BC to CO, OC to EC, and CO2 to CO compare well to top-down constraints from ground observations. The interannual variability and spatial distribution of NOx emissions are consistent with NO2 vertical column density measured by the Ozone Monitoring Instrument (OMI). In particular, the Nanjing city-scale emission inventory correlates better with satellite observations than the downscaled Multi-resolution Emission Inventory for China (MEIC) does when emissions from power plants are excluded. This indicates improvement in emission estimation for sectors other than power generation, notably industry and transportation. A high-resolution emission inventory may also provide a basis to consider the quality of instrumental observations. To further improve emission estimation and evaluation, more measurements of both emission factors and ambient levels of given pollutants are suggested; the uncertainties of emission inventories at city scale should also be fully quantified and compared with those at national scale.
NASA Astrophysics Data System (ADS)
Zhao, Y.; Qiu, L.; Xu, R.; Xie, F.; Zhang, Q.; Yu, Y.; Nielsen, C. P.; Qin, H.; Wang, H.; Wu, X.; Li, W.; Zhang, J.
2015-07-01
With most eastern Chinese cities facing major air quality challenges, there is a strong need for city-scale emission inventories for use in both chemical transport modeling and the development of pollution control policies. In this paper, a high-resolution emission inventory of air pollutants and CO2 for Nanjing, a typical large city in the Yangtze River Delta, is developed incorporating the best available information on local sources. Emission factors and activity data at the unit or facility level are collected and compiled using a thorough onsite survey of major sources. Over 900 individual plants, which account for 97 % of the city's total coal consumption, are identified as point sources, and all of the emission-related parameters including combustion technology, fuel quality, and removal efficiency of air pollution control devices (APCD) are analyzed. New data-collection approaches including continuous emission monitoring systems and real-time monitoring of traffic flows are employed to improve spatiotemporal distribution of emissions. Despite fast growth of energy consumption between 2010 and 2012, relatively small inter-annual changes in emissions are found for most air pollutants during this period, attributed mainly to benefits of growing APCD deployment and the comparatively strong and improving regulatory oversight of the large point sources that dominate the levels and spatial distributions of Nanjing emissions overall. The improvement of this city-level emission inventory is indicated by comparisons with observations and other inventories at larger spatial scale. Relatively good spatial correlations are found for SO2, NOx, and CO between the city-scale emission estimates and concentrations at 9 state-opertated monitoring sites (R = 0.58, 0.46, and 0.61, respectively). The emission ratios of specific pollutants including BC to CO, OC to EC, and CO2 to CO compare well to top-down constraints from ground observations. The inter-annual variability and spatial distribution of NOx emissions are consistent with NO2 vertical column density measured by the Ozone Monitoring Instrument (OMI). In particular, the Nanjing city-scale emission inventory correlates better with satellite observations than the downscaled Multi-resolution Emission Inventory for China (MEIC) does when emissions from power plants are excluded. This indicates improvement in emission estimation for sectors other than power generation, notably industry and transportation. High-resolution emission inventory may also provide a basis to consider the quality of instrumental observations. To further improve emission estimation and evaluation, more measurements of both emission factors and ambient levels of given pollutants are suggested; the uncertainties of emission inventories at city scale should also be fully quantified and compared with those at national scale.
CO2 Dissociation using the Versatile Atmospheric Dielectric Barrier Discharge Experiment (VADER)
NASA Astrophysics Data System (ADS)
Lindon, Michael Allen
As of 2013, the Carbon Dioxide Information Analysis Center (CDIAC) estimates that the world emits approximately 36 trillion metric tons of Carbon Dioxide (CO2) into the atmosphere every year. These large emissions have been correlated to global warming trends that have many consequences across the globe, including glacial retraction, ocean acidification and increased severity of weather events. With green technologies still in the infancy stage, it can be expected that CO2 emissions will stay this way for along time to come. Approximately 41% of the emissions are due to electricity production, which pump out condensed forms of CO2. This danger to our world is why research towards new and innovative ways of controlling CO2 emissions from these large sources is necessary. As of now, research is focused on two primary methods of CO2 reduction from condensed CO2 emission sources (like fossil fuel power plants): Carbon Capture and Sequestration (CCS) and Carbon Capture and Utilization (CCU). CCS is the process of collecting CO2 using absorbers or chemicals, extracting the gas from those absorbers and finally pumping the gas into reservoirs. CCU on the other hand, is the process of reacting CO2 to form value added chemicals, which can then be recycled or stored chemically. A Dielectric Barrier discharge (DBD) is a pulsed, low temperature, non-thermal, atmospheric pressure plasma which creates high energy electrons suitable for dissociating CO2 into its components (CO and O) as one step in the CCU process. Here I discuss the viability of using a DBD for CO2 dissociation on an industrial scale as well as the fundamental physics and chemistry of a DBD for CO2 dissociation. This work involved modeling the DBD discharge and chemistry, which showed that there are specific chemical pathways and plasma parameters that can be adjusted to improve the CO2 reaction efficiencies and rates. Experimental studies using the Versatile Atmospheric dielectric barrier Discharge ExpeRiment (VADER) demonstrated how different factors, like voltage, frequency and the addition of a photocatalyst, change the efficiency of CO2 dissociation in VADER and the plasma chemistry involved.
Pacific-wide contrast highlights resistance of reef calcifiers to ocean acidification.
Comeau, S; Carpenter, R C; Nojiri, Y; Putnam, H M; Sakai, K; Edmunds, P J
2014-09-07
Ocean acidification (OA) and its associated decline in calcium carbonate saturation states is one of the major threats that tropical coral reefs face this century. Previous studies of the effect of OA on coral reef calcifiers have described a wide variety of outcomes for studies using comparable partial pressure of CO2 (pCO2) ranges, suggesting that key questions remain unresolved. One unresolved hypothesis posits that heterogeneity in the response of reef calcifiers to high pCO2 is a result of regional-scale variation in the responses to OA. To test this hypothesis, we incubated two coral taxa (Pocillopora damicornis and massive Porites) and two calcified algae (Porolithon onkodes and Halimeda macroloba) under 400, 700 and 1000 μatm pCO2 levels in experiments in Moorea (French Polynesia), Hawaii (USA) and Okinawa (Japan), where environmental conditions differ. Both corals and H. macroloba were insensitive to OA at all three locations, while the effects of OA on P. onkodes were location-specific. In Moorea and Hawaii, calcification of P. onkodes was depressed by high pCO2, but for specimens in Okinawa, there was no effect of OA. Using a study of large geographical scale, we show that resistance to OA of some reef species is a constitutive character expressed across the Pacific. © 2014 The Author(s) Published by the Royal Society. All rights reserved.
Engineered yeast for enhanced CO2 mineralization†
Barbero, Roberto; Carnelli, Lino; Simon, Anna; Kao, Albert; Monforte, Alessandra d’Arminio; Riccò, Moreno; Bianchi, Daniele; Belcher, Angela
2014-01-01
In this work, a biologically catalyzed CO2 mineralization process for the capture of CO2 from point sources was designed, constructed at a laboratory scale, and, using standard chemical process scale-up protocols, was modeled and evaluated at an industrial scale. A yeast display system in Saccharomyces cerevisae was used to screen several carbonic anhydrase isoforms and mineralization peptides for their impact on CO2 hydration, CaCO3 mineralization, and particle settling rate. Enhanced rates for each of these steps in the CaCO3 mineralization process were confirmed using quantitative techniques in lab-scale measurements. The effect of these enhanced rates on the CO2 capture cost in an industrial scale CO2 mineralization process using coal fly ash as the CaO source was evaluated. The model predicts a process using bCA2- yeast and fly ash is ~10% more cost effective per ton of CO2 captured than a process with no biological molecules, a savings not realized by wild-type yeast and high-temperature stable recombinant CA2 alone or in combination. The levelized cost of electricity for a power plant using this process was calculated and scenarios in which this process compares favorably to CO2 capture by MEA absorption process are presented. PMID:25289021
Poly(ethylenimine)-Functionalized Monolithic Alumina Honeycomb Adsorbents for CO2 Capture from Air.
Sakwa-Novak, Miles A; Yoo, Chun-Jae; Tan, Shuai; Rashidi, Fereshteh; Jones, Christopher W
2016-07-21
The development of practical and effective gas-solid contactors is an important area in the development of CO2 capture technologies. Target CO2 capture applications, such as postcombustion carbon capture and sequestration (CCS) from power plant flue gases or CO2 extraction directly from ambient air (DAC), require high flow rates of gas to be processed at low cost. Extruded monolithic honeycomb structures, such as those employed in the catalytic converters of automobiles, have excellent potential as structured contactors for CO2 adsorption applications because of the low pressure drop imposed on fluid moving through the straight channels of such structures. Here, we report the impregnation of poly(ethylenimine) (PEI), an effective aminopolymer reported commonly for CO2 separation, into extruded monolithic alumina to form structured CO2 sorbents. These structured sorbents are first prepared on a small scale, characterized thoroughly, and compared with powder sorbents with a similar composition. Despite consistent differences observed in the filling of mesopores with PEI between the monolithic and powder sorbents, their performance in CO2 adsorption is similar across a range of PEI contents. A larger monolithic cylinder (1 inch diameter, 4 inch length) is evaluated under conditions closer to those that might be used in large-scale applications and shows a similar performance to the smaller monoliths and powders tested initially. This larger structure is evaluated over five cycles of CO2 adsorption and steam desorption and demonstrates a volumetric capacity of 350 molCO2 m-3monolith and an equilibration time of 350 min under a 0.4 m s(-1) linear flow velocity through the monolith channels using 400 ppm CO2 in N2 as the adsorption gas at 30 °C. This volumetric capacity surpasses that of a similar technology considered previously, which suggested that CO2 could be removed from air at an operating cost as low as $100 per ton. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Liu, Qi; Zhou, Yong; Tu, Wenguang; Yan, Shicheng; Zou, Zhigang
2014-01-06
A facile solution-chemical route was developed for the generalized preparation of a family of highly uniform metal germanate nanowires on a large scale. This route is based on the use of hydrazine monohydrate/H2O as a mixed solvent under solvothermal conditions. Hydrazine has multiple effects on the generation of the nanowires: as an alkali solvent, a coordination agent, and crystal anisotropic growth director. Different-percentage cobalt-doped Cd2Ge2O6 nanowires were also successfully obtained through the addition of Co(OAc)2·4H2O to the initial reaction mixture for future investigation of the magnetic properties of these nanowires. The considerably negative conduction band level of the Cd2Ge2O6 nanowire offers a high driving force for photogenerated electron transfer to CO2 under UV-vis illumination, which facilitates CO2 photocatalytic reduction to a renewable hydrocarbon fuel in the presence of water vapor at room temperature.
NASA Astrophysics Data System (ADS)
van der Velde, Ivar R.; Miller, John B.; van der Molen, Michiel K.; Tans, Pieter P.; Vaughn, Bruce H.; White, James W. C.; Schaefer, Kevin; Peters, Wouter
2018-01-01
To improve our understanding of the global carbon balance and its representation in terrestrial biosphere models, we present here a first dual-species application of the CarbonTracker Data Assimilation System (CTDAS). The system's modular design allows for assimilating multiple atmospheric trace gases simultaneously to infer exchange fluxes at the Earth surface. In the prototype discussed here, we interpret signals recorded in observed carbon dioxide (CO2) along with observed ratios of its stable isotopologues 13CO2/12CO2 (δ13C). The latter is in particular a valuable tracer to untangle CO2 exchange from land and oceans. Potentially, it can also be used as a proxy for continent-wide drought stress in plants, largely because the ratio of 13CO2 and 12CO2 molecules removed from the atmosphere by plants is dependent on moisture conditions.The dual-species CTDAS system varies the net exchange fluxes of both 13CO2 and CO2 in ocean and terrestrial biosphere models to create an ensemble of 13CO2 and CO2 fluxes that propagates through an atmospheric transport model. Based on differences between observed and simulated 13CO2 and CO2 mole fractions (and thus δ13C) our Bayesian minimization approach solves for weekly adjustments to both net fluxes and isotopic terrestrial discrimination that minimizes the difference between observed and estimated mole fractions.With this system, we are able to estimate changes in terrestrial δ13C exchange on seasonal and continental scales in the Northern Hemisphere where the observational network is most dense. Our results indicate a decrease in stomatal conductance on a continent-wide scale during a severe drought. These changes could only be detected after applying combined atmospheric CO2 and δ13C constraints as done in this work. The additional constraints on surface CO2 exchange from δ13C observations neither affected the estimated carbon fluxes nor compromised our ability to match observed CO2 variations. The prototype presented here can be of great benefit not only to study the global carbon balance but also to potentially function as a data-driven diagnostic to assess multiple leaf-level exchange parameterizations in carbon-climate models that influence the CO2, water, isotope, and energy balance.
CO2 fluxes from diffuse degassing in Italy
NASA Astrophysics Data System (ADS)
Cardellini, C.; Chiodini, G.; Frondini, F.; Caliro, S.
2016-12-01
Central and southern Italy are affected by an intense process of CO2 Earth degassing from both active volcanoes, and tectonically active areas. Regional scale studies, based on C mass balance of groundwater of regional aquifers in not volcanically active areas, highlighted the presence of two large CO2 degassing structures that, for magnitude and the geochemical-isotopic features, were related to a regional process of mantle degassing. Quantitative estimates provided a CO2 flux of 9 Mt/y for the region (62000 km2). Besides the magnitude of the process, a strong link between the deep CO2 degassing and the seismicity of the region and a strict correlation between migration of deep CO2-rich fluids and the heat flux have been highlighted. In addition, the region is also characterised by the presence of many cold gas emissions where deeply derived CO2 is released by vents and soil diffuse degassing areas. Both direct CO2 expulsion at the surface and C-rich groundwater are different manifestations of the same process, in fact, the deeply produced gas can be dissolved by groundwater or emitted directly to the atmosphere depending on the gas flux rate, and the geological-structural and hydrogeological settings. Quantitative estimations of the CO2 fluxes are available only for a limited number ( 30) of the about 270 catalogued gas manifestations allowing an estimations of a CO2 flux of 1.4 Mt/y. Summing the two estimates the non-volcanic CO2 flux from the region results globally relevant, being from 2 to 10% of the estimated present-day global CO2 discharge from subaerial volcanoes. Large amounts of CO2 is also discharged by soil diffuse degassing in volcanic-hydrothermal systems. Specific surveys at Solfatara of Pozzuoli (Campi Flegrei Caldera) pointed out the relevance of this process. CO2 diffuse degassing at Solfatara, measured since 1998 shows a persistent CO2 flux of 1300 t/d (± 390 t/d), a flux comparable to an erupting volcano. The quantification of diffuse CO2 degassing in Italy points out the relevance of non-volcanic CO2 degassing and of soil degassing from volcanoes, suggesting that the actual underestimation of the global CO2 degassing, may arise also from the lack of specific and systematic studies of the numerous "degassing areas" of the world, that would contribute to better constrain the global CO2 budget.
Large-Scale CO Maps of the Lupus Molecular Cloud Complex
NASA Astrophysics Data System (ADS)
Tothill, N. F. H.; Löhr, A.; Parshley, S. C.; Stark, A. A.; Lane, A. P.; Harnett, J. I.; Wright, G. A.; Walker, C. K.; Bourke, T. L.; Myers, P. C.
2009-11-01
Fully sampled degree-scale maps of the 13CO 2-1 and CO 4-3 transitions toward three members of the Lupus Molecular Cloud Complex—Lupus I, III, and IV—trace the column density and temperature of the molecular gas. Comparison with IR extinction maps from the c2d project requires most of the gas to have a temperature of 8-10 K. Estimates of the cloud mass from 13CO emission are roughly consistent with most previous estimates, while the line widths are higher, around 2 km s-1. CO 4-3 emission is found throughout Lupus I, indicating widespread dense gas, and toward Lupus III and IV. Enhanced line widths at the NW end and along the edge of the B 228 ridge in Lupus I, and a coherent velocity gradient across the ridge, are consistent with interaction between the molecular cloud and an expanding H I shell from the Upper-Scorpius subgroup of the Sco-Cen OB Association. Lupus III is dominated by the effects of two HAe/Be stars, and shows no sign of external influence. Slightly warmer gas around the core of Lupus IV and a low line width suggest heating by the Upper-Centaurus-Lupus subgroup of Sco-Cen, without the effects of an H I shell.
The Effect of CO2 Pressure on Chromia Scale Microstructure at 750°C
NASA Astrophysics Data System (ADS)
Pint, B. A.; Unocic, K. A.
2018-06-01
To understand and model performance in supercritical CO2 (sCO2) for high-efficiency, concentrating solar power (CSP) and fossil energy power cycles, reaction rates are compared at 750°C in 0.1 MPa CO2 and 30 MPa sCO2 as well as laboratory air as a baseline on structural materials such as Ni-based alloy 625. Due to the thin reaction products formed even after 5000 h, scanning transmission electron microscopy was used to study the Cr-rich surface oxide scale. The scales formed in CO2 and sCO2 had a much finer grain size with more voids observed in CO2. However, the observations on alloy 625 were complicated by Mo and Nb-rich precipitates in the adjacent substrate and Al internal oxidation. To simplify the system, a binary Ni-22Cr alloy was exposed for 1000 h in similar environments. After exposure in sCO2, there was an indication of carbon segregation detected on the Cr2O3 grain boundaries. After exposure in air, metallic Ni precipitates were observed in the scale that were not observed in the scale formed on alloy 625. The scale formed in air on a second Ni-22Cr model alloy with Mn and Si additions did not contain Ni precipitates, suggesting caution when drawing conclusions from model alloys.
Carbon uptake in granular basalt is mitigated by added organic carbon.
NASA Astrophysics Data System (ADS)
Howard, E. L.; Van Haren, J. L. M.; Dontsova, K.
2017-12-01
Soils represent a large, and potentially long-term, storage component of the global carbon budget. Accurate projections of the response of soil respiration -the release of CO2 from soils generated either through root respiration or microbial respiration- to rainfall events remains one of the largest uncertainties in global carbon cycling models. Similarly poorly represented in models is the uptake of CO2 by basalt soils. In an attempt to address these unknowns, we have investigated how the addition of carbon influences the negative CO2 flux observed after wetting basalt. At Biosphere 2 we have constructed a large scale environmentally controlled experiment known as the Landscape Evolution Observatory (LEO). The objective of LEO is to observe the interactions between water, microbes, and climate in the formation of soil and landscapes utilizing granular basalt as a young soil. Previous studies show that water addition to the LEO soil leads to considerable CO2 uptake and that the addition of plants does not alter this response. In this study, we conducted soil incubations to investigate the effect of varying soil carbon content on CO2 fluxes. During incubations we measured CO2 emissions from two types of soil (granular basalt and sand soil) mixed with seven (0, 5, 10, 25, 50, 75, 100%) different proportions of Kalso prairie. The carbon content varied from nearly zero in the basalt to 6.5% in the Kalso Prarie soil. Other parameters that influence soil CO2 fluxes such as pH were taken into account. In conclusion, our experiments confirm that unweathered basalt will consume CO2 when wetted, whereas added carbon will cause a strong pulse of CO2 following water addition. This supports our hypotheses that the carbon content is a large contributor and that maturation of basalt flows will lead to a shift in the carbon dynamics from inorganic to organic dominated. Likewise, these transitions would be expected to be present during soil formation after primary succession and even after anthropogenic alteration to landscape function.
Waszczuk, M A; Zavos, H M S; Gregory, A M; Eley, T C
2016-01-01
Depression and anxiety persist within and across diagnostic boundaries. The manner in which common v. disorder-specific genetic and environmental influences operate across development to maintain internalizing disorders and their co-morbidity is unclear. This paper investigates the stability and change of etiological influences on depression, panic, generalized, separation and social anxiety symptoms, and their co-occurrence, across adolescence and young adulthood. A total of 2619 twins/siblings prospectively reported symptoms of depression and anxiety at mean ages 15, 17 and 20 years. Each symptom scale showed a similar pattern of moderate continuity across development, largely underpinned by genetic stability. New genetic influences contributing to change in the developmental course of the symptoms emerged at each time point. All symptom scales correlated moderately with one another over time. Genetic influences, both stable and time-specific, overlapped considerably between the scales. Non-shared environmental influences were largely time- and symptom-specific, but some contributed moderately to the stability of depression and anxiety symptom scales. These stable, longitudinal environmental influences were highly correlated between the symptoms. The results highlight both stable and dynamic etiology of depression and anxiety symptom scales. They provide preliminary evidence that stable as well as newly emerging genes contribute to the co-morbidity between depression and anxiety across adolescence and young adulthood. Conversely, environmental influences are largely time-specific and contribute to change in symptoms over time. The results inform molecular genetics research and transdiagnostic treatment and prevention approaches.
NASA Astrophysics Data System (ADS)
Rosolem, R.; Zeng, X.; Shuttleworth, W. J.; Saleska, S. R.; Huxman, T. E.
2009-12-01
Biosphere 2 (B2) is a large-scale Earth science facility near Tucson (Arizona) that encompasses about 3.15 acres of land and houses five natural biomes. Sealed off to the outside world, B2 allows scientists to exert precise climate and mass balance control at large scales. The tropical rainforest (TRF) mesocosm area is about 1900 sq. meters and contains plant species from different tropical regions. B2 provides a unique controlled laboratory for carrying out experiments to investigate rainforest biome behavior in response to imposed environmental stresses at plot-scales (e.g., temperature, rainfall, humidity, and CO2 levels), providing the missing link between the laboratory scale and the real world. However, lack of repetitions (the facility contains only a single mesocosm for each biome) poses limitations to the analysis of the results. A well-established land surface parameterization scheme (LSP) may overcome this lack of repetitions by providing a reliable assessment of the biome under a variety of conditions. Modeling approaches can also facilitate and improve future experimental designs in B2. Here we challenge a LSP, the Simple Biosphere 3 (SiB3) model, to simulate the main aspects of the biosphere-atmosphere exchanges inside B2-TRF biome. Model simulations include B2-TRF under normal (i.e., operational) conditions, and during short-term perturbations, such as drought conditions and different treatments of CO2 concentration. A hypothetical simulation which combines both drought and high CO2 levels is performed with SiB3 and analyzed on the basis of future predictions of tropical rainforest under climate change. The main objectives of this study is to determine whether or not SiB3 is capable of representing B2-TRF at a wide range of conditions, and if we can use the combination of past field experiments and modeling to improve our understanding on how tropical rainforests may respond to these changes. Results show that our modified version of SiB3 is capable of reproducing the characteristics of B2-TRF remarkably well. Net photosynthesis is reduced quite substantially during drought periods, followed by a recovery period when the biome is re-watered. Increase in CO2 levels tends to enhance net photosynthesis, but soil respiration remains fairly unchanged, similarly to what past B2-TRF studies suggested. When CO2 levels are increased in combination with drought periods (hypothetical experiment), the vegetation response in SiB3 is quite different depending on the available Photosynthetically Active Radiation (PAR). At relatively lower PAR levels, vegetation response to drought conditions is minimal. However, at relatively high PAR, drought effects offset any response to CO2 fertilization. We recognize that the combination of modeling and field experiments is beneficial in both ways, so that advancing of research inside B2 may be expanded to improve in situ experiments as well as future parameterizations in land surface models.
NASA Astrophysics Data System (ADS)
Streibel, Martin
2015-04-01
In 2012 the German Parliament passed the transposition of the EC Directive 2009/31/EC the "Carbon Dioxide Storage Law" (KSpG). The law focuses on the demonstration of the CO2 storage technology and mainly regulates the storage part of the Carbon Capture and Storage (CCS) chain. As the law has a conceptual character, appendix 1 provides a description of criteria for the characterisation and assessment of a potential CO2 storage site starting with field data ending with requirements for dynamic modelling of the storage complex. Appendix 2 describes the expected monitoring system during all relevant phases of a life cycle of a CO2 storage site. The criteria given in the appendices are of general nature, which reflects on one hand that the CO2 storage technology is still being developed and on the other hand that site specific aspects needs to be considered. In 2004 the Federal Ministry of Education and Research of Germany launched the programme GEOTECHNOLOGIEN with one key aspect being the development of technologies for a sustainable storage of carbon dioxide in geological formations. Within this research field more than 30 projects in three phases have been funded until the end of 2014. In order to benefit from the gathered knowledge and use the experiences for the policy/law making process the umbrella project AUGE has been launched in October 2012 with a life time of three years. The aim of the project is to review and compile all results of projects funded during the three phases to underpin the appendices of the KSpG. In the first part of the paper the most important findings of the project with regard to the overall risk of a geological CO2 storage and the procedure of compiling the guidance document will be discussed. Milestones of this project were • the compilation of the results of national, European and international projects; • interviews with stakeholders; • a workshops to define state of the art for certain involved technologies and existing gaps; • a workshop to understand the limitations of existing simulation tools for large scale CO2 storage. In a second part of the paper it is discussed what kind of guidance documents are actually still required for regulation of large scale CO2 storage sites.
Device Scale Modeling of Solvent Absorption using MFIX-TFM
DOE Office of Scientific and Technical Information (OSTI.GOV)
Carney, Janine E.; Finn, Justin R.
Recent climate change is largely attributed to greenhouse gases (e.g., carbon dioxide, methane) and fossil fuels account for a large majority of global CO 2 emissions. That said, fossil fuels will continue to play a significant role in the generation of power for the foreseeable future. The extent to which CO 2 is emitted needs to be reduced, however, carbon capture and sequestration are also necessary actions to tackle climate change. Different approaches exist for CO 2 capture including both post-combustion and pre-combustion technologies, oxy-fuel combustion and/or chemical looping combustion. The focus of this effort is on post-combustion solvent-absorption technology.more » To apply CO 2 technologies at commercial scale, the availability and maturity and the potential for scalability of that technology need to be considered. Solvent absorption is a proven technology but not at the scale needed by typical power plant. The scale up and down and design of laboratory and commercial packed bed reactors depends heavily on the specific knowledge of two-phase pressure drop, liquid holdup, the wetting efficiency and mass transfer efficiency as a function of operating conditions. Simple scaling rules often fail to provide proper design. Conventional reactor design modeling approaches will generally characterize complex non-ideal flow and mixing patterns using simplified and/or mechanistic flow assumptions. While there are varying levels of complexity used within these approaches, none of these models resolve the local velocity fields. Consequently, they are unable to account for important design factors such as flow maldistribution and channeling from a fundamental perspective. Ideally design would be aided by development of predictive models based on truer representation of the physical and chemical processes that occur at different scales. Computational fluid dynamic (CFD) models are based on multidimensional flow equations with first principle foundations. CFD models can include a more accurate physical description of flow processes and be modified to include more complex behavior. Wetting performance and spatial liquid distribution inside the absorber are recognized as weak areas of knowledge requiring further investigation. CFD tools offer a possible method to investigating such topics and gaining a better understanding of their influence on reactor performance. This report focuses first on describing a hydrodynamic model for countercurrent gas-liquid flow through a packed column and then on the chemistry, heat and mass transfer specific to CO 2 absorption using monoethanolamine (MEA). The indicated model is implemented in MFIX, a CFD open source software package. The user defined functions needed to build this model are described in detail along with the keywords for the corresponding input file. A test case is outlined along with a few results. The example serves to briefly illustrate the developed CFD tool and its potential capability to investigate solvent absorption.« less
NASA Astrophysics Data System (ADS)
Christen, A.; Crawford, B.; Ketler, R.; Lee, J. K.; McKendry, I. G.; Nesic, Z.; Caitlin, S.
2015-12-01
Measurements of long-lived greenhouse gases in the urban atmosphere are potentially useful to constrain and validate urban emission inventories, or space-borne remote-sensing products. We summarize and compare three different approaches, operating at different scales, that directly or indirectly identify, attribute and quantify emissions (and uptake) of carbon dioxide (CO2) in urban environments. All three approaches are illustrated using in-situ measurements in the atmosphere in and over Vancouver, Canada. Mobile sensing may be a promising way to quantify and map CO2 mixing ratios at fine scales across heterogenous and complex urban environments. We developed a system for monitoring CO2 mixing ratios at street level using a network of mobile CO2 sensors deployable on vehicles and bikes. A total of 5 prototype sensors were built and simultaneously used in a measurement campaign across a range of urban land use types and densities within a short time frame (3 hours). The dataset is used to aid in fine scale emission mapping in combination with simultaneous tower-based flux measurements. Overall, calculated CO2 emissions are realistic when compared against a spatially disaggregated scale emission inventory. The second approach is based on mass flux measurements of CO2 using a tower-based eddy covariance (EC) system. We present a continuous 7-year long dataset of CO2 fluxes measured by EC at the 28m tall flux tower 'Vancouver-Sunset'. We show how this dataset can be combined with turbulent source area models to quantify and partition different emission processes at the neighborhood-scale. The long-term EC measurements are within 10% of a spatially disaggregated scale emission inventory. Thirdly, at the urban scale, we present a dataset of CO2 mixing ratios measured using a tethered balloon system in the urban boundary layer above Vancouver. Using a simple box model, net city-scale CO2 emissions can be determined using measured rate of change of CO2 mixing ratios, estimated CO2 advection and entrainment fluxes. Daily city-scale emissions totals predicted by the model are within 32% of a spatially scaled municipal greenhouse gas inventory. In summary, combining information from different approaches and scales is a promising approach to establish long-term emission monitoring networks in cities.
NASA Astrophysics Data System (ADS)
Wuerth, S. M.; Fung, I. Y.; Anderson, J. L.; Raeder, K.
2016-12-01
A long-standing challenge in carbon cycle science is the inference of surface fluxes from atmospheric CO2 observations. Here we present initial results from our carbon-weather data assimilation system coupled to a mass-balance inversion . Our system combines the Community Atmosphere Model (CAM 5FV) with state-of-the-art ensemble data assimilation techniques from the Data Assimilation Research Testbed (DART), and assimilates OCO-2 XCO2 observations together with raw meteorological observations. The system uses a mass balance of the optimized atmospheric state to calculate CO2 sources and sinks throughout the globe. We present results from observing system simulation experiments (OSSE) aimed at comparing two different mass-balance approaches' abilities to detect under-reporting of national-scale CO2 emissions. In both experiments, we define a true state as the atmospheric state resulting from running CAM with a prognostic carbon cycle and CO2 emissions from CarbonTracker CT2015. Meteorological and OCO-2-like observations are harvested from this true state for assimilation. We create a hypothetical scenario in which fossil fuel CO2 emissions of a large emitter are scaled to half of their true values. Surface fluxes are then estimated using one of two approaches. The first approach computes, at every 6-hourly assimilation window, surface fluxes as the residual in the mass balance equation after divergence has been accounted for. The updated surface fluxes are then used as forcing in the ensuing CAM forecast. The second approach uses the initial false emissions for two weeks of model integration, then computes improved emissions by adding the time-averaged analysis increment in near-surface CO2 mixing ratio to the initial false emissions. The two weeks are re-run with these updated fluxes, and the process is then repeated for further refinement of fluxes. The advantages and disadvantages of the two approaches are discussed, and the system's ability to recover the true fluxes is assessed.
Formation of TiC core-graphitic mantle grains from CO gas
NASA Astrophysics Data System (ADS)
Kimura, Yuki; Nuth, Joseph A.; Ferguson, Frank T.
2006-05-01
We demonstrate a new formation route for TiC core-graphitic mantle spherules that does not require carbon-atom addition and the very long time scales associated with such growth (Bernatowicz et al. 1996). Carbonaceous materials can be formed from C2H2 and its derivatives, as well as from CO gas. In this paper, we will demonstrate that large-cage-structure carbon particles can be produced from CO gas by the Boudouard reaction. Since the sublimation temperature for such fullerenes is low, the large cages can be deposited onto previously nucleated TiC and produce TiC core-graphitic mantle spherules. New constraints for the formation conditions and the time scale for the formation of TiC core-graphitic mantle spherules are suggested by the results of this study. In particular, TiC core-graphitic mantle grains that are found in primitive meteorites that have never experienced hydration could be mantled by fullerenes or carbon nanotubes rather than by graphite. In situ observations of these grains in primitive anhydrous meteoritic matrix could confirm or refute this prediction and would demonstrate that the graphitic mantle on such grains is a metamorphic feature due to interaction of the presolar fullerenes with water within the meteorite matrix.
NASA Astrophysics Data System (ADS)
Oldenburg, C. M.; Zhou, Q.; Birkholzer, J. T.
2017-12-01
The injection of supercritical CO2 (scCO2) in fractured reservoirs has been conducted at several storage sites. However, no site-specific dual-continuum modeling for fractured reservoirs has been reported and modeling studies have generally underestimated the fracture-matrix interactions. We developed a conceptual model for enhanced CO2 storage to take into account global scCO2 migration in the fracture continuum, local storage of scCO2 and dissolved CO2 (dsCO2) in the matrix continuum, and driving forces for scCO2 invasion and dsCO2 diffusion from fractures. High-resolution discrete fracture-matrix models were developed for a column of idealized matrix blocks bounded by vertical and horizontal fractures and for a km-scale fractured reservoir. The column-scale simulation results show that equilibrium storage efficiency strongly depends on matrix entry capillary pressure and matrix-matrix connectivity while the time scale to reach equilibrium is sensitive to fracture spacing and matrix flow properties. The reservoir-scale modeling results shows that the preferential migration of scCO2 through fractures is coupled with bulk storage in the rock matrix that in turn retards the fracture scCO2 plume. We also developed unified-form diffusive flux equations to account for dsCO2 storage in brine-filled matrix blocks and found solubility trapping is significant in fractured reservoirs with low-permeability matrix.
NASA Astrophysics Data System (ADS)
Campbell, Elliott
Measurements of atmospheric carbon dioxide (CO2) have led to an understanding of the past and present CO2 trends at global scales. However, many of the processes that underlie the CO 2 fluxes are highly uncertain, especially at smaller spatial scales in the terrestrial biosphere. Our abilities to forecast climate change and manage the carbon cycle are reliant on an understanding of these underlying processes. In this dissertation, new steps were taken to understand the biogenic and anthropogenic processes based on analysis with an atmospheric transport model and simultaneous measurements of CO2 and other trace gases. The biogenic processes were addressed by developing an approach for quantifying photosynthesis and respiration surface fluxes using observations of CO 2 and carbonyl sulfide (COS). There is currently no reliable method for separating the influence of these gross biosphere fluxes on atmospheric CO2 concentrations. First, the plant sink for COS was quantified as a function of the CO2 photosynthesis uptake using the STEM transport model and measurements of COS and CO2 from the INTEX-NA campaign. Next, the STEM inversion model was modified for the simultaneous optimization of fluxes using COS and CO2 measurements and using only CO 2 measurements. The CO2-only inversion was found to be process blind, while the simultaneous COS/CO2 inversion was found to provide a unique estimate of the respiration and photosynthesis component fluxes. Further validation should be pursued with independent observations. The approach presented here is the first application of COS measurements for inferring information about the carbon cycle. Anthropogenic emissions were addressed by improving the estimate of the fossil fuel component of observed CO2 by using observed carbon monoxide (CO). Recent applications of the CO approach were based on simple approximations of non-fossil fuel influences on the measured CO such as sources from oxidation of volatile organic carbon species, sinks from oxidation of CO, and sources from forest fires. A revised CO method was developed using STEM simulations of atmospheric reactions and tracers of different combustion sources. Applications of the revised method to the NASA INTEX-NA measurements showed large differences with conventional methods. Application to the INTEX-B measurements resulted in partitioning of continental and offshore oil rig sources around Mexico.
Controlling Cooperative CO2 Adsorption in Diamine-Appended Mg2(dobpdc) Metal-Organic Frameworks.
Siegelman, Rebecca L; McDonald, Thomas M; Gonzalez, Miguel I; Martell, Jeffrey D; Milner, Phillip J; Mason, Jarad A; Berger, Adam H; Bhown, Abhoyjit S; Long, Jeffrey R
2017-08-02
In the transition to a clean-energy future, CO 2 separations will play a critical role in mitigating current greenhouse gas emissions and facilitating conversion to cleaner-burning and renewable fuels. New materials with high selectivities for CO 2 adsorption, large CO 2 removal capacities, and low regeneration energies are needed to achieve these separations efficiently at scale. Here, we present a detailed investigation of nine diamine-appended variants of the metal-organic framework Mg 2 (dobpdc) (dobpdc 4- = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) that feature step-shaped CO 2 adsorption isotherms resulting from cooperative and reversible insertion of CO 2 into metal-amine bonds to form ammonium carbamate chains. Small modifications to the diamine structure are found to shift the threshold pressure for cooperative CO 2 adsorption by over 4 orders of magnitude at a given temperature, and the observed trends are rationalized on the basis of crystal structures of the isostructural zinc frameworks obtained from in situ single-crystal X-ray diffraction experiments. The structure-activity relationships derived from these results can be leveraged to tailor adsorbents to the conditions of a given CO 2 separation process. The unparalleled versatility of these materials, coupled with their high CO 2 capacities and low projected energy costs, highlights their potential as next-generation adsorbents for a wide array of CO 2 separations.
NASA Astrophysics Data System (ADS)
Jansson, A.; Lischka, S.; Boxhammer, T.; Schulz, K. G.; Norkko, J.
2015-12-01
Anthropogenic carbon dioxide (CO2) emissions are causing severe changes in the global inorganic carbon balance of the oceans. Associated ocean acidification is expected to impose a major threat to marine ecosystems worldwide, and it is also expected to be amplified in the Baltic Sea where the system is already at present exposed to relatively large natural seasonal and diel pH fluctuations. The response of organisms to future ocean acidification has primarily been studied in single-species experiments, whereas the knowledge of community-wide responses is still limited. To study responses of the Baltic Sea pelagic community to a range of future CO2-scenarios, six ∼ 55 m3 pelagic mesocosms were deployed in the northern Baltic Sea in June 2012. In this specific study we focused on the tolerance, development and subsequent settlement process of the larvae of the benthic key-species Macoma balthica when exposed to different levels of future CO2. We found that the settling of M. balthica was delayed along the increasing CO2 gradient of the mesocosms. Also, when exposed to increasing CO2 levels larvae settled at a larger size, indicating a developmental delay. With on-going climate change, both the frequency and extent of regularly occurring high CO2 conditions is likely to increase, and a permanent pH decrease will likely occur. The strong impact of increasing CO2 levels on early-stage bivalves is alarming as these stages are crucial for sustaining viable populations, and a failure in their recruitment would ultimately lead to negative effects on the population.
Liquid membrane purification of biogas
DOE Office of Scientific and Technical Information (OSTI.GOV)
Majumdar, S.; Guha, A.K.; Lee, Y.T.
1991-03-01
Conventional gas purification technologies are highly energy intensive. They are not suitable for economic removal of CO{sub 2} from methane obtained in biogas due to the small scale of gas production. Membrane separation techniques on the other hand are ideally suited for low gas production rate applications due to their modular nature. Although liquid membranes possess a high species permeability and selectivity, they have not been used for industrial applications due to the problems of membrane stability, membrane flooding and poor operational flexibility, etc. A new hollow-fiber-contained liquid membrane (HFCLM) technique has been developed recently. This technique overcomes the shortcomingsmore » of the traditional immobilized liquid membrane technology. A new technique uses two sets of hydrophobic, microporous hollow fine fibers, packed tightly in a permeator shell. The inter-fiber space is filled with an aqueous liquid acting as the membrane. The feed gas mixture is separated by selective permeation of a species through the liquid from one fiber set to the other. The second fiber set carries a sweep stream, gas or liquid, or simply the permeated gas stream. The objectives (which were met) of the present investigation were as follows. To study the selective removal of CO{sub 2} from a model biogas mixture containing 40% CO{sub 2} (the rest being N{sub 2} or CH{sub 4}) using a HFCLM permeator under various operating modes that include sweep gas, sweep liquid, vacuum and conventional permeation; to develop a mathematical model for each mode of operation; to build a large-scale purification loop and large-scale permeators for model biogas separation and to show stable performance over a period of one month.« less
Divergent biophysical controls of aquatic CO2 and CH4 in the World’s two largest rivers
Borges, Alberto V.; Abril, Gwenaël; Darchambeau, François; Teodoru, Cristian R.; Deborde, Jonathan; Vidal, Luciana O.; Lambert, Thibault; Bouillon, Steven
2015-01-01
Carbon emissions to the atmosphere from inland waters are globally significant and mainly occur at tropical latitudes. However, processes controlling the intensity of CO2 and CH4 emissions from tropical inland waters remain poorly understood. Here, we report a data-set of concurrent measurements of the partial pressure of CO2 (pCO2) and dissolved CH4 concentrations in the Amazon (n = 136) and the Congo (n = 280) Rivers. The pCO2 values in the Amazon mainstem were significantly higher than in the Congo, contrasting with CH4 concentrations that were higher in the Congo than in the Amazon. Large-scale patterns in pCO2 across different lowland tropical basins can be apprehended with a relatively simple statistical model related to the extent of wetlands within the basin, showing that, in addition to non-flooded vegetation, wetlands also contribute to CO2 in river channels. On the other hand, dynamics of dissolved CH4 in river channels are less straightforward to predict, and are related to the way hydrology modulates the connectivity between wetlands and river channels. PMID:26494107
Menon, Binuraj R K; Menon, Navya; Fisher, Karl; Rigby, Stephen E J; Leys, David; Scrutton, Nigel S
2015-01-01
How cobalamin-dependent enzymes promote C–Co homolysis to initiate radical catalysis has been debated extensively. For the pyridoxal 5′-phosphate and cobalamin-dependent enzymes lysine 5,6-aminomutase and ornithine 4,5-aminomutase (OAM), large-scale re-orientation of the cobalamin-binding domain linked to C–Co bond breakage has been proposed. In these models, substrate binding triggers dynamic sampling of the B12-binding Rossmann domain to achieve a catalytically competent ‘closed’ conformational state. In ‘closed’ conformations of OAM, Glu338 is thought to facilitate C–Co bond breakage by close association with the cobalamin adenosyl group. We investigated this using stopped-flow continuous-wave photolysis, viscosity dependence kinetic measurements, and electron paramagnetic resonance spectroscopy of a series of Glu338 variants. We found that substrate-induced C–Co bond homolysis is compromised in Glu388 variant forms of OAM, although photolysis of the C–Co bond is not affected by the identity of residue 338. Electrostatic interactions of Glu338 with the 5′-deoxyadenosyl group of B12 potentiate C–Co bond homolysis in ‘closed’ conformations only; these conformations are unlocked by substrate binding. Our studies extend earlier models that identified a requirement for large-scale motion of the cobalamin domain. Our findings indicate that large-scale motion is required to pre-organize the active site by enabling transient formation of ‘closed’ conformations of OAM. In ‘closed’ conformations, Glu338 interacts with the 5′-deoxyadenosyl group of cobalamin. This interaction is required to potentiate C–Co homolysis, and is a crucial component of the approximately 1012 rate enhancement achieved by cobalamin-dependent enzymes for C–Co bond homolysis. PMID:25627283
The influence of clouds and diffuse radiation on ecosystem-atmosphere CO2 and CO18O exhanges
DOE Office of Scientific and Technical Information (OSTI.GOV)
Still, C.J.; Riley, W.J.; Biraud, S.C.
2009-05-01
This study evaluates the potential impact of clouds on ecosystem CO{sub 2} and CO{sub 2} isotope fluxes ('isofluxes') in two contrasting ecosystems (a broadleaf deciduous forest and a C{sub 4} grassland), in a region for which cloud cover, meteorological, and isotope data are available for driving the isotope-enabled land surface model, ISOLSM. Our model results indicate a large impact of clouds on ecosystem CO{sub 2} fluxes and isofluxes. Despite lower irradiance on partly cloudy and cloudy days, predicted forest canopy photosynthesis was substantially higher than on clear, sunny days, and the highest carbon uptake was achieved on the cloudiest day.more » This effect was driven by a large increase in light-limited shade leaf photosynthesis following an increase in the diffuse fraction of irradiance. Photosynthetic isofluxes, by contrast, were largest on partly cloudy days, as leaf water isotopic composition was only slightly depleted and photosynthesis was enhanced, as compared to adjacent clear sky days. On the cloudiest day, the forest exhibited intermediate isofluxes: although photosynthesis was highest on this day, leaf-to-atmosphere isofluxes were reduced from a feedback of transpiration on canopy relative humidity and leaf water. Photosynthesis and isofluxes were both reduced in the C{sub 4} grass canopy with increasing cloud cover and diffuse fraction as a result of near-constant light limitation of photosynthesis. These results suggest that some of the unexplained variation in global mean {delta}{sup 18}O of CO{sub 2} may be driven by large-scale changes in clouds and aerosols and their impacts on diffuse radiation, photosynthesis, and relative humidity.« less
Stripe Antiferromagnetic Spin Fluctuations in SrCo 2As 2
DOE Office of Scientific and Technical Information (OSTI.GOV)
Jayasekara, Wageesha; Lee, Young-Jin; Pandey, Abhishek
Inelastic neutron scattering measurements of paramagnetic SrCo 2As 2 at T = 5 K reveal antiferromagnetic (AFM) spin fluctuations that are peaked at a wave vector of Q AFM = (1/2, 1/2, 1) and possess a large energy scale. These stripe spin fluctuations are similar to those found in AFe 2As 2 compounds, where spin-density wave AFM is driven by Fermi surface nesting between electron and hole pockets separated by Q AFM. SrCo 2As 2 has a more complex Fermi surface and band-structure calculations indicate a potential instability toward either a ferromagnetic or stripe AFM ground state. The results suggestmore » that stripe AFM magnetism is a general feature of both iron and cobalt-based arsenides and the search for spin fluctuation-induced unconventional superconductivity should be expanded to include cobalt-based compounds.« less
Uncertainty in gridded CO 2 emissions estimates
Hogue, Susannah; Marland, Eric; Andres, Robert J.; ...
2016-05-19
We are interested in the spatial distribution of fossil-fuel-related emissions of CO 2 for both geochemical and geopolitical reasons, but it is important to understand the uncertainty that exists in spatially explicit emissions estimates. Working from one of the widely used gridded data sets of CO 2 emissions, we examine the elements of uncertainty, focusing on gridded data for the United States at the scale of 1° latitude by 1° longitude. Uncertainty is introduced in the magnitude of total United States emissions, the magnitude and location of large point sources, the magnitude and distribution of non-point sources, and from themore » use of proxy data to characterize emissions. For the United States, we develop estimates of the contribution of each component of uncertainty. At 1° resolution, in most grid cells, the largest contribution to uncertainty comes from how well the distribution of the proxy (in this case population density) represents the distribution of emissions. In other grid cells, the magnitude and location of large point sources make the major contribution to uncertainty. Uncertainty in population density can be important where a large gradient in population density occurs near a grid cell boundary. Uncertainty is strongly scale-dependent with uncertainty increasing as grid size decreases. In conclusion, uncertainty for our data set with 1° grid cells for the United States is typically on the order of ±150%, but this is perhaps not excessive in a data set where emissions per grid cell vary over 8 orders of magnitude.« less
Deep ALMA imaging of the merger NGC 1614. Is CO tracing a massive inflow of non-starforming gas?
NASA Astrophysics Data System (ADS)
König, S.; Aalto, S.; Muller, S.; Gallagher, J. S.; Beswick, R. J.; Xu, C. K.; Evans, A.
2016-10-01
Aims: Observations of the molecular gas over scales of ~0.5 to several kpc provide crucial information on how molecular gas moves through galaxies, especially in mergers and interacting systems, where it ultimately reaches the galaxy center, accumulates, and feeds nuclear activity. Studying the processes involved in the gas transport is one of the important steps forward to understand galaxy evolution. Methods: 12CO, 13CO, and C18O 1-0 high-sensitivity ALMA observations (~4'' × 2'') were used to assess the properties of the large-scale molecular gas reservoir and its connection to the circumnuclear molecular ring in the merger NGC 1614. Specifically, the role of excitation and abundances were studied in this context. We also observed the molecular gas high-density tracers CN and CS. Results: The spatial distributions of the detected 12CO 1-0 and 13CO 1-0 emission show significant differences. 12CO traces the large-scale molecular gas reservoir, which is associated with a dust lane that harbors infalling gas, and extends into the southern tidal tails. 13CO emission is for the first time detected in the large-scale dust lane. In contrast to 12CO, its line emission peaks between the dust lane and the circumnuclear molecular ring. A 12CO-to-13CO 1-0 intensity ratio map shows high values in the ring region (~30) that are typical for the centers of luminous galaxy mergers and even more extreme values in the dust lane (>45). Surprisingly, we do not detect C18O emission in NGC 1614, but we do observe gas emitting the high-density tracers CN and CS. Conclusions: We find that the 12CO-to-13CO 1-0 line ratio in NGC 1614 changes from >45 in the 2 kpc dust lane to ~30 in the starburst nucleus. This drop in ratio with decreasing radius is consistent with the molecular gas in the dust lane being kept in a diffuse, unbound state while it is being funneled toward the nucleus. This also explains why there are no (or very faint) signs of star formation in the dust lane, despite its high 12CO luminosity. In the inner 1.5 kpc, the gas is compressed into denser and most likely self-gravitating clouds (traced by CN and CS emission), allowing it to power the intense central starburst. We find a high 16O-to-18O abundance ratio in the starburst region (≥900), typical of quiescent disk gas. This is surprising because by now, the starburst is expected to have enriched the nuclear interstellar medium in 18O relative to 16O. We suggest that the massive inflow of gas may be partially responsible for the low 18O/16O abundance since it will dilute the starburst enrichment with unprocessed gas from greater radial distances. The 12CO-to-13CO abundance of >90 we infer from the line ratio is consistent with this scenario. It suggests that the nucleus of NGC 1614 is in a transient phase of its evolution where the starburst and the nuclear growth is still being fuelled by returning gas from the minor merger event.
NASA Astrophysics Data System (ADS)
Dednam, W.; Botha, A. E.
2015-01-01
Solvation of bio-molecules in water is severely affected by the presence of co-solvent within the hydration shell of the solute structure. Furthermore, since solute molecules can range from small molecules, such as methane, to very large protein structures, it is imperative to understand the detailed structure-function relationship on the microscopic level. For example, it is useful know the conformational transitions that occur in protein structures. Although such an understanding can be obtained through large-scale molecular dynamic simulations, it is often the case that such simulations would require excessively large simulation times. In this context, Kirkwood-Buff theory, which connects the microscopic pair-wise molecular distributions to global thermodynamic properties, together with the recently developed technique, called finite size scaling, may provide a better method to reduce system sizes, and hence also the computational times. In this paper, we present molecular dynamics trial simulations of biologically relevant low-concentration solvents, solvated by aqueous co-solvent solutions. In particular we compare two different methods of calculating the relevant Kirkwood-Buff integrals. The first (traditional) method computes running integrals over the radial distribution functions, which must be obtained from large system-size NVT or NpT simulations. The second, newer method, employs finite size scaling to obtain the Kirkwood-Buff integrals directly by counting the particle number fluctuations in small, open sub-volumes embedded within a larger reservoir that can be well approximated by a much smaller simulation cell. In agreement with previous studies, which made a similar comparison for aqueous co-solvent solutions, without the additional solvent, we conclude that the finite size scaling method is also applicable to the present case, since it can produce computationally more efficient results which are equivalent to the more costly radial distribution function method.
Instrumentation for analytical scale supercritical fluid chromatography.
Berger, Terry A
2015-11-20
Analytical scale supercritical fluid chromatography (SFC) is largely a sub-discipline of high performance liquid chromatography (HPLC), in that most of the hardware and software can be used for either technique. The aspects that separate the 2 techniques stem from the use of carbon dioxide (CO2) as the main component of the mobile phase in SFC. The high compressibility and low viscosity of CO2 mean that pumps, and autosamplers designed for HPLC either need to be modified or an alternate means of dealing with compressibility needs to be found. The inclusion of a back pressure regulator and a high pressure flow cell for any UV-Vis detector are also necessary. Details of the various approaches, problems and solutions are described. Characteristics, such as adiabatic vs. isothermal compressibility, thermal gradients, and refractive index issues are dealt with in detail. Copyright © 2015 Elsevier B.V. All rights reserved.
Turner, P V; Kloeze, H; Dam, A; Ward, D; Leung, N; Brown, E E L; Whiteman, A; Chiappetta, M E; Hunter, D B
2012-07-01
Appropriate emergency disaster preparedness is a key priority for agricultural agencies to allow effective response to serious avian disease outbreaks. There is a need to develop rapid, humane, and safe depopulation techniques for poultry that are widely applicable across a range of farm settings. Whole barn depopulation with carbon dioxide (CO(2)) has been investigated as a humane and efficient means of killing large numbers of birds in the event of a reportable disease outbreak. It has also been considered as a method for depopulating barns containing end-of-lay hens, particularly when there is limited local slaughter and rendering capacity. Determining the best method of humanely killing large flocks of birds remains problematic and is being investigated by a coordinated international effort. While whole barn depopulation using CO(2) inhalation has been explored, physiologic responses of chickens have not been characterized in field settings and assessment of animal welfare is hampered without this information. In this study, 12 cull laying hens were surgically instrumented with telemetry transmitters to record electroencephalographs, electrocardiographs, body temperature, and activity during 2 large-scale field CO(2) euthanasia trials of end-of-lay hens. The day following surgery, instrumented hens were placed in barns with other birds, barns were sealed, and animals were killed by CO(2) inhalation delivered via a specially designed liquid CO(2) manifold. Instrumented birds were monitored by infrared thermography, and ambient temperature, CO(2), and O(2) concentrations were recorded. Results from these studies indicate that instrumented hens lost consciousness within 2 min of CO(2) levels reaching 18 to 20%. Mild to moderate head shaking, gasping, and 1 to 2 clonic muscle contractions were noted in hens before unconsciousness; however, brain death followed rapidly (<5 min). Evaluation of welfare costs and benefits suggest clear advantages over catching and transporting cull hens for slaughter. The financial costs with this method are greater, however, than those estimated for traditional slaughter techniques. Results of these studies are being used to develop national protocols for whole barn depopulation of hens by CO(2) inhalation.
NASA Astrophysics Data System (ADS)
Kuang, Min; Wen, Zhong Quan; Guo, Xiao Long; Zhang, Sheng Mao; Zhang, Yu Xin
2014-12-01
An effective and rational strategy is developed for large-scale growth of firecracker-like Ni-substituted Co3O4 (NiCo2O4) nanosheets on β-MnO2 nanowires (NWs) with robust adhesion as high-performance electrode for electrochemical capacitors. The NiCo2O4-MnO2 nanostructures display much higher specific capacitance (343 F g-1 at current density of 0.5 A g-1), better rate capability (75.3% capacitance retention from 0.5 A g-1 to 8 A g-1) and excellent cycle stability (5% capacitance loss after 3000 cycles) than Co3O4-MnO2 nanostructures. Moreover, an asymmetric supercapacitor based on NiCo2O4-MnO2 NWs as the positive electrode and activated graphenes (AG) as the negative electrode achieves an energy density of 9.4 Wh kg-1 and a maximum power density of 2.5 kW kg-1. These attractive findings suggest this novel core-shell nanostructure promising for electrochemical applications as an efficient supercapacitive electrode.
Convective Instability and Mass Transport of the Diffusion Layer in CO2 Sequestration
NASA Astrophysics Data System (ADS)
Backhaus, S.
2011-12-01
The long-term fate of supercritical (sc) CO2 in saline aquifers is critical to the security of carbon sequestration, an important option for eliminating or reducing the emissions of this most prevalent greenhouse gas. scCO2 is less dense than brine and floats to the top of the aquifer where it is trapped in a metastable state by a geologic feature such as a low permeability cap rock. Dissolution into the underlying brine creates a CO2-brine mixture that is denser than brine, eliminating buoyancy and removing the threat of CO2 escaping back to the atmosphere. If molecular diffusion were the only dissolution mechanism, the CO2 waste stream from a typical large coal-fired electrical power plant may take upward of 10,000 years to no longer pose a threat, however, a convective instability of the dense diffusion boundary layer between the scCO2 and the brine can dramatically increase the dissolution rates, shortening the lifetime of the scCO2 waste pool. We present results of 2D and 3D similitude-correct, laboratory-scale experiments using an analog fluid system. The experiments and flow visualization reveal the onset of the convective instability, the dynamics of the fluid flows during the convective processes, and the long-term mass transfer rates.
Pore-scale supercritical CO 2 dissolution and mass transfer under drainage conditions
Chang, Chun; Zhou, Quanlin; Oostrom, Mart; ...
2016-12-05
Recently, both core- and pore-scale imbibition experiments have shown non-equilibrium dissolution of supercritical CO 2 (scCO 2) and a prolonged depletion of residual scCO 2. In this paper, pore-scale scCO 2 dissolution and mass transfer under drainage conditions were investigated using a two-dimensional heterogeneous micromodel and a novel fluorescent water dye with a sensitive pH range between 3.7 and 6.5. Drainage experiments were conducted at 9 MPa and 40 °C by injecting scCO 2 into the sandstone-analogue pore network initially saturated by water without dissolved CO 2 (dsCO 2). During the experiments, time-lapse images of dye intensity, reflecting water pH,more » were obtained. These images show non-uniform pH in individual pores and pore clusters, with average pH levels gradually decreasing with time. Further analysis on selected pores and pore clusters shows that (1) rate-limited mass transfer prevails with slowly decreasing pH over time when the scCO 2-water interface area is low with respect to the volume of water-filled pores and pore clusters, (2) fast scCO 2 dissolution and phase equilibrium occurs when scCO 2 bubbles invade into water-filled pores, significantly enhancing the area-to-volume ratio, and (3) a transition from rate-limited to diffusion-limited mass transfer occurs in a single pore when a medium area-to-volume ratio is prevalent. The analysis also shows that two fundamental processes – scCO 2 dissolution at phase interfaces and diffusion of dsCO 2 at the pore scale (10–100 µm) observed after scCO 2 bubble invasion into water-filled pores without pore throat constraints – are relatively fast. The overall slow dissolution of scCO 2 in the millimeter-scale micromodel can be attributed to the small area-to-volume ratios that represent pore-throat configurations and characteristics of phase interfaces. Finally, this finding is applicable for the behavior of dissolution at pore, core, and field scales when water-filled pores and pore clusters of varying size are surrounded by scCO 2 at narrow pore throats.« less
Pore-scale supercritical CO 2 dissolution and mass transfer under drainage conditions
DOE Office of Scientific and Technical Information (OSTI.GOV)
Chang, Chun; Zhou, Quanlin; Oostrom, Mart
Recently, both core- and pore-scale imbibition experiments have shown non-equilibrium dissolution of supercritical CO 2 (scCO 2) and a prolonged depletion of residual scCO 2. In this paper, pore-scale scCO 2 dissolution and mass transfer under drainage conditions were investigated using a two-dimensional heterogeneous micromodel and a novel fluorescent water dye with a sensitive pH range between 3.7 and 6.5. Drainage experiments were conducted at 9 MPa and 40 °C by injecting scCO 2 into the sandstone-analogue pore network initially saturated by water without dissolved CO 2 (dsCO 2). During the experiments, time-lapse images of dye intensity, reflecting water pH,more » were obtained. These images show non-uniform pH in individual pores and pore clusters, with average pH levels gradually decreasing with time. Further analysis on selected pores and pore clusters shows that (1) rate-limited mass transfer prevails with slowly decreasing pH over time when the scCO 2-water interface area is low with respect to the volume of water-filled pores and pore clusters, (2) fast scCO 2 dissolution and phase equilibrium occurs when scCO 2 bubbles invade into water-filled pores, significantly enhancing the area-to-volume ratio, and (3) a transition from rate-limited to diffusion-limited mass transfer occurs in a single pore when a medium area-to-volume ratio is prevalent. The analysis also shows that two fundamental processes – scCO 2 dissolution at phase interfaces and diffusion of dsCO 2 at the pore scale (10–100 µm) observed after scCO 2 bubble invasion into water-filled pores without pore throat constraints – are relatively fast. The overall slow dissolution of scCO 2 in the millimeter-scale micromodel can be attributed to the small area-to-volume ratios that represent pore-throat configurations and characteristics of phase interfaces. Finally, this finding is applicable for the behavior of dissolution at pore, core, and field scales when water-filled pores and pore clusters of varying size are surrounded by scCO 2 at narrow pore throats.« less
Pore-scale supercritical CO 2 dissolution and mass transfer under drainage conditions
DOE Office of Scientific and Technical Information (OSTI.GOV)
Chang, Chun; Zhou, Quanlin; Oostrom, Mart
Abstract: Recently, both core- and pore-scale imbibition experiments have shown non-equilibrium dissolution of supercritical CO 2 (scCO 2) and a prolonged depletion of residual scCO 2. In this study, pore-scale scCO 2 dissolution and mass transfer under drainage conditions were investigated using a two-dimensional heterogeneous micromodel and a novel fluorescent water dye with a sensitive pH range between 3.7 and 6.5. Drainage experiments were conducted at 9 MPa and 40 °C by injecting scCO 2 into the sandstone-analogue pore network initially saturated by water without dissolved CO 2 (dsCO 2). During the experiments, time-lapse images of dye intensity, reflecting watermore » pH, were obtained. These images show non-uniform pH in individual pores and pore clusters, with average pH levels gradually decreasing with time. Further analysis on selected pores and pore clusters shows that (1) rate-limited mass transfer prevails with slowly decreasing pH over time when the scCO 2-water interface area is low with respect to the volume of water-filled pores and pore clusters, (2) fast scCO 2 dissolution and phase equilibrium occurs when scCO 2 bubbles invade into water-filled pores, significantly enhancing the area-to-volume ratio, and (3) a transition from rate-limited to diffusion-limited mass transfer occurs in a single pore when a medium area-to-volume ratio is prevalent. The analysis also shows that two fundamental processes – scCO 2 dissolution at phase interfaces and diffusion of dsCO 2 at the pore scale (10-100 µm) observed after scCO 2 bubble invasion into water-filled pores without pore throat constraints – are relatively fast. The overall slow dissolution of scCO 2 in the millimeter-scale micromodel can be attributed to the small area-to-volume ratios that represent pore-throat configurations and characteristics of phase interfaces. This finding is applicable for the behavior of dissolution at pore, core, and field scales when water-filled pores and pore clusters of varying size are surrounded by scCO 2 at narrow pore throats.« less
NASA Astrophysics Data System (ADS)
Stewart, H. A.; Barrio, M.; Akhurst, M.; Aagaard, P.; Alcalde, J.; Bauer, A.; Bradwell, T.; Cavanagh, A.; Faleide, J. I.; Furre, A. K.; Haszeldine, S.; Hjelstuen, B. O.; Holloway, S.; Johansen, H.; Johnson, G.; Kuerschner, W.; Mondol, N. H.; Querendez, E.; Ringrose, P. S.; Sejrup, H. P.; Stewart, M.; Stoddart, D.; Wilkinson, M.; Zalmstra, H.
2014-12-01
The sedimentary strata of the North Sea Basin (NSB) record the glacial and interglacial history of environmental change in the Northern Hemisphere, and are a proposed location for the engineered storage of carbon dioxide (CO2) captured from power plant and industrial sources to reduce greenhouse gas emissions. These aspects interact in the geomechanical and fluid flow domain, as ice sheet dynamics change the properties of potential seal and reservoir rocks that are the prospective geological storage strata for much of Europe's captured CO2. The intensification of the global glacial-interglacial cycle at the onset of the Pleistocene (2.5-2.7 Ma) was a critical tipping-point in Earth's recent climate history. The increased severity of glaciations at the Plio-Pleistocene boundary triggered the first development of large-scale continental ice sheets in the Northern Hemisphere. The central part of the NSB preserves a unique history of the depositional record spanning at least the last 3 Ma, which also forms the overburden and seal to the underlying CO2 reservoirs. There is good evidence that these ice sheets created strong feedback loops that subsequently affected the evolution of the Quaternary climate system through complex ocean-atmosphere-cryosphere linkages. Understanding NSB dynamics, including the role of fluids in controlling compaction, cementation, and diagenetic processes in shale-dominated basins, is essential for CO2 storage site characterisation to increase understanding and confidence in secure storage. An increased understanding of the overlying sequence will inform quantitative predictions of the performance of prospective CO2 storage sites in glaciated areas in Europe and worldwide; to include improved resolution of glacial cycles (depositional and chronological framework), characterise pore fluids, flow properties of glacial landforms within the sequence (e.g. tunnel valleys) and the geomechanical effects (quantify compaction, rock stiffness, strength and stress profiles) of advancing and retreating ice on the underlying strata to verify and constrain models of glaciation. This presentation describes current work and introduces a proposal submitted to the Integrated Ocean Discovery Program (852-Pre) by the authors.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kitanidis, Peter
As large-scale, commercial storage projects become operational, the problem of utilizing information from diverse sources becomes more critically important. In this project, we developed, tested, and applied an advanced joint data inversion system for CO 2 storage modeling with large data sets for use in site characterization and real-time monitoring. Emphasis was on the development of advanced and efficient computational algorithms for joint inversion of hydro-geophysical data, coupled with state-of-the-art forward process simulations. The developed system consists of (1) inversion tools using characterization data, such as 3D seismic survey (amplitude images), borehole log and core data, as well as hydraulic,more » tracer and thermal tests before CO 2 injection, (2) joint inversion tools for updating the geologic model with the distribution of rock properties, thus reducing uncertainty, using hydro-geophysical monitoring data, and (3) highly efficient algorithms for directly solving the dense or sparse linear algebra systems derived from the joint inversion. The system combines methods from stochastic analysis, fast linear algebra, and high performance computing. The developed joint inversion tools have been tested through synthetic CO 2 storage examples.« less
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.
Scaling Relations between Gas and Star Formation in Nearby Galaxies
NASA Astrophysics Data System (ADS)
Bigiel, Frank; Leroy, Adam; Walter, Fabian
2011-04-01
High resolution, multi-wavelength maps of a sizeable set of nearby galaxies have made it possible to study how the surface densities of H i, H2 and star formation rate (ΣHI, ΣH2, ΣSFR) relate on scales of a few hundred parsecs. At these scales, individual galaxy disks are comfortably resolved, making it possible to assess gas-SFR relations with respect to environment within galaxies. ΣH2, traced by CO intensity, shows a strong correlation with ΣSFR and the ratio between these two quantities, the molecular gas depletion time, appears to be constant at about 2 Gyr in large spiral galaxies. Within the star-forming disks of galaxies, ΣSFR shows almost no correlation with ΣHI. In the outer parts of galaxies, however, ΣSFR does scale with ΣHI, though with large scatter. Combining data from these different environments yields a distribution with multiple regimes in Σgas - ΣSFR space. If the underlying assumptions to convert observables to physical quantities are matched, even combined datasets based on different SFR tracers, methodologies and spatial scales occupy a well define locus in Σgas - ΣSFR space.
NASA Astrophysics Data System (ADS)
Galfond, B.; Riemer, D. D.; Swart, P. K.
2014-12-01
In order for Carbon Capture Utilization and Storage (CCUS) to gain wide acceptance as a method for mitigating atmospheric CO2 concentrations, schemes must be devised to ensure that potential leakage is detected. New regulations from the US Environmental Protection Agency require monitoring and accounting for Class VI injection wells, which will remain a barrier to wide scale CCUS deployment until effective and efficient monitoring techniques have been developed and proven. Monitoring near-surface CO2 at injection sites to ensure safety and operational success requires high temporal resolution CO2 concentration and carbon isotopic (δ13C) measurements. The only technologies currently capable of this rapid measurement of δ13C are optical techniques such as Cavity Ringdown Spectroscopy (CRDS). We have developed a comprehensive remote monitoring approach using CRDS and a custom manifold system to obtain accurate rapid measurements from a large sample area over an extended study period. Our modified Picarro G1101-i CRDS allows for automated rapid and continuous field measurement of δ13CO2 and concentrations of relevant gas species. At our field site, where preparations have been underway for Enhanced Oil Recovery (EOR) operations, we have been able to measure biogenic effects on a diurnal scale, as well as variation due to precipitation and seasonality. Taking these background trends into account, our statistical treatment of real data has been used to improve signal-to-noise ratios by an order of magnitude over published models. Our system has proven field readiness for the monitoring of sites with even modest CO2 fluxes.
The U. S. DOE Carbon Storage Program: Status and Future Directions
NASA Astrophysics Data System (ADS)
Damiani, D.
2016-12-01
The U.S. Department of Energy (DOE) is taking steps to reduce carbon dioxide (CO2) emissions through clean energy innovation, including carbon capture and storage (CCS) research. The Office of Fossil Energy Carbon Storage Program is focused on ensuring the safe and permanent storage and/or utilization of CO2 captured from stationary sources. The Program is developing and advancing geologic storage technologies both onshore and offshore that will significantly improve the effectiveness of CCS, reduce the cost of implementation, and be ready for widespread commercial deployment in the 2025-2035 timeframe. The technology development and field testing conducted through this Program will be used to benefit the existing and future fleet of fossil fuel power generating and industrial facilities by creating tools to increase our understanding of geologic reservoirs appropriate for CO2 storage and the behavior of CO2 in the subsurface. The Program is evaluating the potential for storage in depleted oil and gas reservoirs, saline formations, unmineable coal, organic-rich shale formations, and basalt formations. Since 1997, DOE's Carbon Storage Program has significantly advanced the CCS knowledge base through a diverse portfolio of applied research projects. The Core Storage R&D research component focuses on analytic studies, laboratory, and pilot- scale research to develop technologies that can improve wellbore integrity, increase reservoir storage efficiency, improve management of reservoir pressure, ensure storage permanence, quantitatively assess risks, and identify and mitigate potential release of CO2 in all types of storage formations. The Storage Field Management component focuses on scale-up of CCS and involves field validation of technology options, including large-volume injection field projects at pre-commercial scale to confirm system performance and economics. Future research involves commercial-scale characterization for regionally significant storage locations capable of storing from 50 to 100 million metric tons of CO2 in a saline formation. These projects will lay the foundation for fully integrated carbon capture and storage demonstrations of future first of a kind (FOAK) coal power projects. Future research will also bring added focus on offshore CCS.
NASA Astrophysics Data System (ADS)
Kountouris, Panagiotis; Gerbig, Christoph; Rödenbeck, Christian; Karstens, Ute; Koch, Thomas F.; Heimann, Martin
2018-03-01
Optimized biogenic carbon fluxes for Europe were estimated from high-resolution regional-scale inversions, utilizing atmospheric CO2 measurements at 16 stations for the year 2007. Additional sensitivity tests with different data-driven error structures were performed. As the atmospheric network is rather sparse and consequently contains large spatial gaps, we use a priori biospheric fluxes to further constrain the inversions. The biospheric fluxes were simulated by the Vegetation Photosynthesis and Respiration Model (VPRM) at a resolution of 0.1° and optimized against eddy covariance data. Overall we estimate an a priori uncertainty of 0.54 GtC yr-1 related to the poor spatial representation between the biospheric model and the ecosystem sites. The sink estimated from the atmospheric inversions for the area of Europe (as represented in the model domain) ranges between 0.23 and 0.38 GtC yr-1 (0.39 and 0.71 GtC yr-1 up-scaled to geographical Europe). This is within the range of posterior flux uncertainty estimates of previous studies using ground-based observations.
Tian, Liangliang; He, Gege; Cai, Yanhua; Wu, Shenping; Su, Yongyao; Yan, Hengqing; Yang, Cong; Chen, Yanling; Li, Lu
2018-02-16
Inspired by kinetics, the design of hollow hierarchical electrocatalysts through large-scale integration of building blocks is recognized as an effective approach to the achievement of superior electrocatalytic performance. In this work, a hollow, hierarchical Co 3 O 4 architecture (Co 3 O 4 HHA) was constructed using a coordinated etching and precipitation (CEP) method followed by calcination. The resulting Co 3 O 4 HHA electrode exhibited excellent electrocatalytic activity in terms of high sensitivity (839.3 μA mM -1 cm -2 ) and reliable stability in glucose detection. The high sensitivity could be attributed to the large specific surface area (SSA), ample unimpeded penetration diffusion paths and high electron transfer rate originating from the unique two-dimensional (2D) sheet-like character and hollow porous architecture. The hollow hierarchical structure also affords sufficient interspace for accommodation of volume change and structural strain, resulting in enhanced stability. The results indicate that Co 3 O 4 HHA could have potential for application in the design of non-enzymatic glucose sensors, and that the construction of hollow hierarchical architecture provides an efficient way to design highly active, stable electrocatalysts.
NASA Astrophysics Data System (ADS)
Tian, Liangliang; He, Gege; Cai, Yanhua; Wu, Shenping; Su, Yongyao; Yan, Hengqing; Yang, Cong; Chen, Yanling; Li, Lu
2018-02-01
Inspired by kinetics, the design of hollow hierarchical electrocatalysts through large-scale integration of building blocks is recognized as an effective approach to the achievement of superior electrocatalytic performance. In this work, a hollow, hierarchical Co3O4 architecture (Co3O4 HHA) was constructed using a coordinated etching and precipitation (CEP) method followed by calcination. The resulting Co3O4 HHA electrode exhibited excellent electrocatalytic activity in terms of high sensitivity (839.3 μA mM-1 cm-2) and reliable stability in glucose detection. The high sensitivity could be attributed to the large specific surface area (SSA), ample unimpeded penetration diffusion paths and high electron transfer rate originating from the unique two-dimensional (2D) sheet-like character and hollow porous architecture. The hollow hierarchical structure also affords sufficient interspace for accommodation of volume change and structural strain, resulting in enhanced stability. The results indicate that Co3O4 HHA could have potential for application in the design of non-enzymatic glucose sensors, and that the construction of hollow hierarchical architecture provides an efficient way to design highly active, stable electrocatalysts.
On the calculation of air-sea fluxes of CO2 in the presence of temperature and salinity gradients
NASA Astrophysics Data System (ADS)
Woolf, D. K.; Land, P. E.; Shutler, J. D.; Goddijn-Murphy, L. M.; Donlon, C. J.
2016-02-01
The presence of vertical temperature and salinity gradients in the upper ocean and the occurrence of variations in temperature and salinity on time scales from hours to many years complicate the calculation of the flux of carbon dioxide (CO2) across the sea surface. Temperature and salinity affect the interfacial concentration of aqueous CO2 primarily through their effect on solubility with lesser effects related to saturated vapor pressure and the relationship between fugacity and partial pressure. The effects of temperature and salinity profiles in the water column and changes in the aqueous concentration act primarily through the partitioning of the carbonate system. Climatological calculations of flux require attention to variability in the upper ocean and to the limited validity of assuming "constant chemistry" in transforming measurements to climatological values. Contrary to some recent analysis, it is shown that the effect on CO2 fluxes of a cool skin on the sea surface is large and ubiquitous. An opposing effect on calculated fluxes is related to the occurrence of warm layers near the surface; this effect can be locally large but will usually coincide with periods of low exchange. A salty skin and salinity anomalies in the upper ocean also affect CO2 flux calculations, though these haline effects are generally weaker than the thermal effects.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ito, Akihiko; Inatomi, Motoko; Huntzinger, Deborah N.
The seasonal-cycle amplitude (SCA) of the atmosphere–ecosystem carbon dioxide (CO 2) exchange rate is a useful metric of the responsiveness of the terrestrial biosphere to environmental variations. It is unclear, however, what underlying mechanisms are responsible for the observed increasing trend of SCA in atmospheric CO 2 concentration. Using output data from the Multi-scale Terrestrial Model Intercomparison Project (MsTMIP), we investigated how well the SCA of atmosphere–ecosystem CO 2 exchange was simulated with 15 contemporary terrestrial ecosystem models during the period 1901–2010. Also, we made attempt to evaluate the contributions of potential mechanisms such as atmospheric CO 2, climate, land-use,more » and nitrogen deposition, through factorial experiments using different combinations of forcing data. Under contemporary conditions, the simulated global-scale SCA of the cumulative net ecosystem carbon flux of most models was comparable in magnitude with the SCA of atmospheric CO 2 concentrations. Results from factorial simulation experiments showed that elevated atmospheric CO 2 exerted a strong influence on the seasonality amplification. When the model considered not only climate change but also land-use and atmospheric CO 2 changes, the majority of the models showed amplification trends of the SCAs of photosynthesis, respiration, and net ecosystem production (+0.19 % to +0.50 % yr -1). In the case of land-use change, it was difficult to separate the contribution of agricultural management to SCA because of inadequacies in both the data and models. The simulated amplification of SCA was approximately consistent with the observational evidence of the SCA in atmospheric CO 2 concentrations. Large inter-model differences remained, however, in the simulated global tendencies and spatial patterns of CO 2 exchanges. Further studies are required to identify a consistent explanation for the simulated and observed amplification trends, including their underlying mechanisms. Nevertheless, this study implied that monitoring of ecosystem seasonality would provide useful insights concerning ecosystem dynamics.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ito, Akihiko; Inatomi, Motoko; Huntzinger, Deborah N.
The seasonal-cycle amplitude (SCA) of the atmosphere–ecosystem carbon dioxide (CO 2) exchange rate is a useful metric of the responsiveness of the terrestrial biosphere to environmental variations. It is unclear, however, what underlying mechanisms are responsible for the observed increasing trend of SCA in atmospheric CO 2 concentration. Using output data from the Multi-scale Terrestrial Model Intercomparison Project (MsTMIP), we investigated how well the SCA of atmosphere–ecosystem CO 2 exchange was simulated with 15 contemporary terrestrial ecosystem models during the period 1901–2010. Also, we made attempt to evaluate the contributions of potential mechanisms such as atmospheric CO 2, climate, land-use,more » and nitrogen deposition, through factorial experiments using different combinations of forcing data. Under contemporary conditions, the simulated global-scale SCA of the cumulative net ecosystem carbon flux of most models was comparable in magnitude with the SCA of atmospheric CO 2 concentrations. Results from factorial simulation experiments showed that elevated atmospheric CO 2 exerted a strong influence on the seasonality amplification. When the model considered not only climate change but also land-use and atmospheric CO 2 changes, the majority of the models showed amplification trends of the SCAs of photosynthesis, respiration, and net ecosystem production (+0.19 % to +0.50 % yr –1). In the case of land-use change, it was difficult to separate the contribution of agricultural management to SCA because of inadequacies in both the data and models. The simulated amplification of SCA was approximately consistent with the observational evidence of the SCA in atmospheric CO 2 concentrations. Large inter-model differences remained, however, in the simulated global tendencies and spatial patterns of CO 2 exchanges. Further studies are required to identify a consistent explanation for the simulated and observed amplification trends, including their underlying mechanisms. Furthermore, this study implied that monitoring of ecosystem seasonality would provide useful insights concerning ecosystem dynamics.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Dubey, Manvendra; Parket, Harrison; Myers, Katherine
Forests soak up 25% of the carbon dioxide (CO2) emitted by anthropogenic fossil energy use (10 Gt C y-1), moderating its atmospheric accumulation. How this terrestrial CO2 uptake will evolve with climate change in the 21st Century is largely unknown. Rainforests are the most active ecosystems, with the Amazon basin storing 120 Gt C as biomass and exchanging 18 Gt C y-1 of CO2 via photosynthesis and respiration and fixing carbon at 2-3 kg C m-2 y-1. Furthermore, the intense hydrologic and carbon cycles are tightly coupled in the Amazon where about half of the water is recycled by evapotranspirationmore » and the other half imported from the ocean by Northeasterly trade winds. Climate models predict a drying in the Amazon with reduced carbon uptake while observationally guided assessments indicate sustained uptake. We set out to resolve this huge discrepancy in the size and sign of the future Amazon carbon cycle by performing the first simultaneous regional-scale high-frequency measurements of atmospheric CO2, H2O, HOD, CH4, N2O, and CO at the T3 site in Manacupuru, Brazil, as part of DOE's GoAmazon 2014/15 project. Our data will be used to inform and develop DOE's Community Land Model (CLM) on the tropical carbon-water couplings at the appropriate grid scale (10-50 km). Our measurements will also validate the CO2 data from Japan's Greenhouse gases Observing Satellite (GOSAT) and NASA's Orbiting Carbon Observatory (OCO)-2 satellite (launched in July, 2014). Our data addresses these science questions: 1. How does ecosystem heterogeneity and climate variability influence the rainforest carbon cycle? 2. How well do current tropical ecosystem models simulate the observed regional carbon cycle? 3. Does nitrogen deposition (from the Manaus, Brazil, plume) enhance rainforest carbon uptake?« less
Cheng, Lei; Wu, Cheng Hao; Jarry, Angelique; Chen, Wei; Ye, Yifan; Zhu, Junfa; Kostecki, Robert; Persson, Kristin; Guo, Jinghua; Salmeron, Miquel; Chen, Guoying; Doeff, Marca
2015-08-19
The interfacial resistances of symmetrical lithium cells containing Al-substituted Li7La3Zr2O12 (LLZO) solid electrolytes are sensitive to their microstructures and histories of exposure to air. Air exposure of LLZO samples with large grain sizes (∼150 μm) results in dramatically increased interfacial impedances in cells containing them, compared to those with pristine large-grained samples. In contrast, a much smaller difference is seen between cells with small-grained (∼20 μm) pristine and air-exposed LLZO samples. A combination of soft X-ray absorption (sXAS) and Raman spectroscopy, with probing depths ranging from nanometer to micrometer scales, revealed that the small-grained LLZO pellets are more air-stable than large-grained ones, forming far less surface Li2CO3 under both short- and long-term exposure conditions. Surface sensitive X-ray photoelectron spectroscopy (XPS) indicates that the better chemical stability of the small-grained LLZO is related to differences in the distribution of Al and Li at sample surfaces. Density functional theory calculations show that LLZO can react via two different pathways to form Li2CO3. The first, more rapid, pathway involves a reaction with moisture in air to form LiOH, which subsequently absorbs CO2 to form Li2CO3. The second, slower, pathway involves direct reaction with CO2 and is favored when surface lithium contents are lower, as with the small-grained samples. These observations have important implications for the operation of solid-state lithium batteries containing LLZO because the results suggest that the interfacial impedances of these devices is critically dependent upon specific characteristics of the solid electrolyte and how it is prepared.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Losey, London M; Andres, Robert Joseph; Marland, Gregg
2006-12-01
Detailed understanding of global carbon cycling requires estimates of CO2 emissions on temporal and spatial scales finer than annual and country. This is the first attempt to derive such estimates for a large, developing, Southern Hemisphere country. Though data on energy use are not complete in terms of time and geography, there are enough data available on the sale or consumption of fuels in Brazil to reasonably approximate the temporal and spatial patterns of fuel use and CO2 emissions. Given the available data, a strong annual cycle in emissions from Brazil is not apparent. CO2 emissions are unevenly distributed withinmore » Brazil as the population density and level of development both vary widely.« less
NASA Astrophysics Data System (ADS)
Pochanart, Pakpong; Kato, Shungo; Katsuno, Takao; Akimoto, Hajime
The roles of Eurasian/Siberian continental air masses transport and the impact of large-scale East Asian anthropogenic emissions on tropospheric ozone and carbon monoxide levels in northeast Asia were investigated. Seasonal behaviors of O 3 and CO mixing ratios in background continental (BC) air masses and regionally polluted continental (RPC) air masses were identified using trajectory analyses of Eurasian continental air masses and multi-year O 3 and CO data observed at Happo, a mountain site in Japan. RPC air masses show significantly higher O 3 and CO mixing ratios (annual average of 53.9±6.0 and 200±41 ppb, respectively) than BC air masses (44.4±3.6 and 167±17 ppb, respectively). Large scale anthropogenic emissions in East Asia are suggested to contribute about 10 ppb of photochemical O 3 and 32 ppb of CO at Happo. A comparative study of O 3 and CO observed at other sites, i.e., Oki Islands and Mondy in northeast Asia, showed similarities suggesting that O 3 mixing ratios in BC air masses at Happo could be representative for remote northeast Asia. However, CO mixing ratios in BC air masses at Happo are higher than the background level in Siberia. The overestimate is probably related to an increase in the CO baseline gradient between Siberia and the East Asia Pacific rim, and perturbations by sub-grid scale pollution transport and regional-scale boreal forest fires in Siberia when the background continental air masses are transported to Japan.
NASA Technical Reports Server (NTRS)
Harri, A.-M.; Polkko, J.; Siili, T.; Crisp, D.
1998-01-01
Pressure observations are crucial for the success of the Mars Volatiles and Climate Surveyor (MVACS) Meteorology (MET) package onboard the Mars Polar Lander (MPL), due for launch early next year. The spacecraft is expected to land in December 1999 (L(sub s) = 256 degrees) at a high southern latitude (74 degrees - 78 degrees S). The nominal period of operation is 90 sols but may last up to 210 sols. The MVACS/MET experiment will provide the first in situ observations of atmospheric pressure, temperature, wind, and humidity in the southern hemisphere of Mars and in the polar regions. The martian atmosphere goes through a large-scale atmospheric pressure cycle due to the annual condensation/sublimation of the atmospheric CO2. Pressure also exhibits short period variations associated with dust storms, tides, and other atmospheric events. A series of pressure measurements can hence provide us with information on the large-scale state and dynamics of the atmosphere, including the CO2 and dust cycles as well as local weather phenomena. The measurements can also shed light on the shorter time scale phenomena (e.g., passage of dust devils) and hence be important in contributing to our understanding of mixing and transport of heat, dust, and water vapor.
Devaraju, N; Bala, G; Nemani, R
2015-09-01
Land-use changes since the start of the industrial era account for nearly one-third of the cumulative anthropogenic CO2 emissions. In addition to the greenhouse effect of CO2 emissions, changes in land use also affect climate via changes in surface physical properties such as albedo, evapotranspiration and roughness length. Recent modelling studies suggest that these biophysical components may be comparable with biochemical effects. In regard to climate change, the effects of these two distinct processes may counterbalance one another both regionally and, possibly, globally. In this article, through hypothetical large-scale deforestation simulations using a global climate model, we contrast the implications of afforestation on ameliorating or enhancing anthropogenic contributions from previously converted (agricultural) land surfaces. Based on our review of past studies on this subject, we conclude that the sum of both biophysical and biochemical effects should be assessed when large-scale afforestation is used for countering global warming, and the net effect on global mean temperature change depends on the location of deforestation/afforestation. Further, although biochemical effects trigger global climate change, biophysical effects often cause strong local and regional climate change. The implication of the biophysical effects for adaptation and mitigation of climate change in agriculture and agroforestry sectors is discussed. © 2014 John Wiley & Sons Ltd.
The fate of carbonates along a subducting slab
NASA Astrophysics Data System (ADS)
Bouilhol, P.; Debret, B.; Inglis, E.
2017-12-01
Carbon long-term cycling is a subject of recent controversy as new mass balance calculations suggest that most carbon is transferred from the slab to the mantle wedge by fluids during subduction, limiting the efficiency of carbon recycling to the deep mantle. Here, we examine the mobility of carbon at large scale during subduction through field, petrographic and geochemical studies on exhumed portion of the alpine slab that have recorded different metamorphic conditions during subduction. We studied serpentinite samples, metasomatic horizon between serpentinites and sediments, as well as veins hosted in serpentinites. Samples are from the Western Alps (Queyras and Zermatt) and have recorded a prograde metamorphic history from low temperature blueshist to eclogite facies P-T conditions. We show that during subduction there are several stages of carbonate precipitation and dissolution at metasomatic interfaces between metasedimentary and ultramafic rocks in the slab, as well as within the serpentinites. The early stage of subduction sees carbonate precipitation from the sediment derived fluids into the serpentnites. At higher temperature, when the dehydration shift from sediment to serpentinite dominated, the carbonates are dissolved, inducing the release of CO2 rich fluids. This occurs before the eclogite facies is attained, providing strong evidence for the mobility of carbon in fluids during the early stages of subduction. These fluids are a potential metasomatic agent for the fore-arc mantle wedge, corroborating the observation of carbonate bearing veins in sub-arc mantle ultramafic rocks. In eclogite facies conditions, olivine and carbonate veins within the serpentinites witness the mobility of CO2 during serpentinite dehydration, and may provide clues about the large scale recycling of CO2 within the deep mantle, as well as secondary precipitation associated with exhumation. Trace elements, Fe and Zn isotopic composition of the different samples provides evidence for a large scale transfer of both sulfate and carbonate bearing fluids during the early stages of subduction, and could imply an overlooked role of the fore-arc in melt genesis.
NASA Astrophysics Data System (ADS)
Garapati, N.; Randolph, J.; Saar, M. O.
2013-12-01
CO2-Plume Geothermal (CPG) involves injection of CO2 as a working fluid to extract heat from naturally high permeable sedimentary basins. The injected CO2 forms a large subsurface CO2 plume that absorbs heat from the geothermal reservoir and eventually buoyantly rises to the surface. The heat density of sedimentary basins is typically relatively low.However, this drawback is likely counteracted by the large accessible volume of natural reservoirs compared to artificial, hydrofractured, and thus small-scale, reservoirs. Furthermore, supercritical CO2has a large mobility (inverse kinematic viscosity) and expansibility compared to water resulting in the formation of a strong thermosiphon which eliminates the need for parasitic pumping power requirements and significantly increasing electricity production efficiency. Simultaneously, the life span of the geothermal power plant can be increased by operating the CPG system such that it depletes the geothermal reservoir heat slowly. Because the produced CO2 is reinjected into the ground with the main CO2 sequestration stream coming from a CO2 emitter, all of the CO2 is ultimately geologically sequestered resulting in a CO2 sequestering geothermal power plant with a negative carbon footprint. Conventional geothermal process requires pumping of huge amount of water for the propagation of the fractures in the reservoir, but CPG process eliminates this requirement and conserves water resources. Here, we present results for performance of a CPG system as a function of various geologic properties of multilayered systemsincludingpermeability anisotropy, rock thermal conductivity, geothermal gradient, reservoir depth and initial native brine salinity as well as spacing between the injection and production wells. The model consists of a 50 m thick, radially symmetric grid with a semi-analytic heat exchange and no fluid flow at the top and bottom boundaries and no fluid and heat flow at the lateral boundaries. We design Plackett-Burman experiments resulting in 16 simulations for the seven parameters investigated. The reservoir is divided into 3-, 4-, or 5- layer systems with log-normal permeability distributions. We consider 10 sets of values for each case resulting in a total of 16x3x10 =480 simulations.We analyze the performance of the system to maximize the amount of heat energy extracted, minimize reservoir temperature depletion and maximize the CO2concentration in the produced fluid. Achieving the latter objective reduces power system problems as Welch and Boyle (GRC Trans. 2009) found that CO2 concentration should be >94% in the systems they investigated.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Chang, J.I.; Tsai, J.J.; Wu, K.H.
2005-07-01
The impacts of the aeration and the agitation on the composting process of synthetic food wastes made of dog food were studied in a laboratory-scale reactor. Two major peaks of CO{sub 2} evolution rate were observed. Each peak represented an independent stage of composting associated with the activities of thermophilic bacteria. CO{sub 2} evolutions known to correlate well with microbial activities and reactor temperatures were fitted successfully to a modified Gompertz equation, which incorporated three biokinetic parameters, namely, CO{sub 2} evolution potential, specific CO{sub 2} evolution rate, and lag phase time. No parameters that describe the impact of operating variablesmore » are involved. The model is only valid for the specified experimental conditions and may look different with others. The effects of operating parameters such as aeration and agitation were studied statistically with multivariate regression technique. Contour plots were constructed using regression equations for the examination of the dependence of CO{sub 2} evolution potentials on aeration and agitation. In the first stage, a maximum CO{sub 2} evolution potential was found when the aeration rate and the agitation parameter were set at 1.75 l/kg solids-min and 0.35, respectively. In the second stage, a maximum existed when the aeration rate and the agitation parameter were set at 1.8 l/kg solids-min and 0.5, respectively. The methods presented here can also be applied for the optimization of large-scale composting facilities that are operated differently and take longer time.« less
Ruocco, Miriam; Musacchia, Francesco; Olivé, Irene; Costa, Monya M; Barrote, Isabel; Santos, Rui; Sanges, Remo; Procaccini, Gabriele; Silva, João
2017-08-01
Here, we report the first use of massive-scale RNA-sequencing to explore seagrass response to CO 2 -driven ocean acidification (OA). Large-scale gene expression changes in the seagrass Cymodocea nodosa occurred at CO 2 levels projected by the end of the century. C. nodosa transcriptome was obtained using Illumina RNA-Seq technology and de novo assembly, and differential gene expression was explored in plants exposed to short-term high CO 2 /low pH conditions. At high pCO 2 , there was a significant increased expression of transcripts associated with photosynthesis, including light reaction functions and CO 2 fixation, and also to respiratory pathways, specifically for enzymes involved in glycolysis, in the tricarboxylic acid cycle and in the energy metabolism of the mitochondrial electron transport. The upregulation of respiratory metabolism is probably supported by the increased availability of photosynthates and increased energy demand for biosynthesis and stress-related processes under elevated CO 2 and low pH. The upregulation of several chaperones resembling heat stress-induced changes in gene expression highlighted the positive role these proteins play in tolerance to intracellular acid stress in seagrasses. OA further modifies C. nodosa secondary metabolism inducing the transcription of enzymes related to biosynthesis of carbon-based secondary compounds, in particular the synthesis of polyphenols and isoprenoid compounds that have a variety of biological functions including plant defence. By demonstrating which physiological processes are most sensitive to OA, this research provides a major advance in the understanding of seagrass metabolism in the context of altered seawater chemistry from global climate change. © 2017 John Wiley & Sons Ltd.
Multiphase modeling of geologic carbon sequestration in saline aquifers.
Bandilla, Karl W; Celia, Michael A; Birkholzer, Jens T; Cihan, Abdullah; Leister, Evan C
2015-01-01
Geologic carbon sequestration (GCS) is being considered as a climate change mitigation option in many future energy scenarios. Mathematical modeling is routinely used to predict subsurface CO2 and resident brine migration for the design of injection operations, to demonstrate the permanence of CO2 storage, and to show that other subsurface resources will not be degraded. Many processes impact the migration of CO2 and brine, including multiphase flow dynamics, geochemistry, and geomechanics, along with the spatial distribution of parameters such as porosity and permeability. In this article, we review a set of multiphase modeling approaches with different levels of conceptual complexity that have been used to model GCS. Model complexity ranges from coupled multiprocess models to simplified vertical equilibrium (VE) models and macroscopic invasion percolation models. The goal of this article is to give a framework of conceptual model complexity, and to show the types of modeling approaches that have been used to address specific GCS questions. Application of the modeling approaches is shown using five ongoing or proposed CO2 injection sites. For the selected sites, the majority of GCS models follow a simplified multiphase approach, especially for questions related to injection and local-scale heterogeneity. Coupled multiprocess models are only applied in one case where geomechanics have a strong impact on the flow. Owing to their computational efficiency, VE models tend to be applied at large scales. A macroscopic invasion percolation approach was used to predict the CO2 migration at one site to examine details of CO2 migration under the caprock. © 2015, National Ground Water Association.
On the development of a methodology for extensive in-situ and continuous atmospheric CO2 monitoring
NASA Astrophysics Data System (ADS)
Wang, K.; Chang, S.; Jhang, T.
2010-12-01
Carbon dioxide is recognized as the dominating greenhouse gas contributing to anthropogenic global warming. Stringent controls on carbon dioxide emissions are viewed as necessary steps in controlling atmospheric carbon dioxide concentrations. From the view point of policy making, regulation of carbon dioxide emissions and its monitoring are keys to the success of stringent controls on carbon dioxide emissions. Especially, extensive atmospheric CO2 monitoring is a crucial step to ensure that CO2 emission control strategies are closely followed. In this work we develop a methodology that enables reliable and accurate in-situ and continuous atmospheric CO2 monitoring for policy making. The methodology comprises the use of gas filter correlation (GFC) instrument for in-situ CO2 monitoring, the use of CO2 working standards accompanying the continuous measurements, and the use of NOAA WMO CO2 standard gases for calibrating the working standards. The use of GFC instruments enables 1-second data sampling frequency with the interference of water vapor removed from added dryer. The CO2 measurements are conducted in the following timed and cycled manner: zero CO2 measurement, two standard CO2 gases measurements, and ambient air measurements. The standard CO2 gases are calibrated again NOAA WMO CO2 standards. The methodology is used in indoor CO2 measurements in a commercial office (about 120 people working inside), ambient CO2 measurements, and installed in a fleet of in-service commercial cargo ships for monitoring CO2 over global marine boundary layer. These measurements demonstrate our method is reliable, accurate, and traceable to NOAA WMO CO2 standards. The portability of the instrument and the working standards make the method readily applied for large-scale and extensive CO2 measurements.
Natural variability of pCO2 and pH in the Atlantic and Pacific coastal margins of the U.S
NASA Astrophysics Data System (ADS)
Sutton, A. J.; Sabine, C. L.; Feely, R. A.; Newton, J.; Salisbury, J.; Vandemark, D. C.; Musielewicz, S. B.; Maenner-Jones, S.; Bott, R.; Lawrence-Slavas, N.
2011-12-01
The discovery that seawater chemistry is changing as a result of carbon dioxide (CO2) emissions, referred to as "ocean acidification", has prompted a large effort to understand how this changing chemistry will impact marine life. Changes in carbon chemistry have been documented in the open ocean; however, in dynamic coastal systems where many marine species live, ocean acidification and the natural biogeochemical variability that organisms are currently exposed to are poorly quantified. In 2010 we began equipping coastal moorings currently measuring pCO2 with pH and other biogeochemical sensors to measure ocean acidification parameters at 3 hour intervals in the surface water. Here we present the magnitude and diurnal to seasonal variability of pCO2 and pH during the first year of observations at 2 sites in the Atlantic and Pacific coastal margins of the U.S.: the Gulf of Maine and outer coast of Washington state. Both the magnitude and range of pCO2 and pH values were much greater at the coastal moorings compared to the open ocean mooring at Ocean Station Papa in the North Pacific and also varied between the two coastal mooring sites. We observed maximum pCO2 values in coastal waters exceeding predicted values for the open ocean at 2x pre-industrial CO2 levels. The range of pCO2 and pH values during this time series was approximately 4 times the range observed at open ocean mooring Papa (2007-2011 time series). In many cases, large variance was observed at short time scales, with values fluctuating more than 200 μatm pCO2 and 0.2 pH between 3-hour cycles. These types of observations are critical for understanding how ocean acidification will manifest in naturally dynamic coastal systems and for informing the experimental design of species response studies that aim to mimic carbon chemistry experienced by coastal marine organisms.
Field Measurements of Respiratory Del13CO2 and Photodegradation
NASA Astrophysics Data System (ADS)
van Asperen, H.; Sabbatini, S.; Nicolini, G.; Warneke, T.; Papale, D.; Notholt, J.
2014-12-01
Carbon decomposition dynamics have been studied in a variety of ecosystems and its variation can mostly be explained in terms of environmental variables (e.g. temperature and precipitation). However, carbon dynamics in arid, water limited regions have shown to be very different and are still largely unknown. Several studies have indicated the importance of photodegradation, the direct breakdown of organic matter by sunlight, in these arid regions. A FTIR (Fourier Transform Infrared Spectrometer) was set up to continuously measure concentrations of CO2, CH4, N2O, CO as well as del13C in CO2. The FTIR was connected to 2 different flux measurement systems: a Flux Gradient system and 2 flux chambers, providing a continuous data set of gas concentrations and biosphere-atmosphere gas fluxes at different heights and scales. Field measurements showed photodegradation induced carbon fluxes. Also, respiratory del13CO2 was determined by use of Keeling plots, and was determined to vary between -25‰ and -21‰. A clear diurnal pattern in respiratory del13CO2 was found, suggesting either different (dominant) respiratory processes between day and night or the effect of diffusive fractionation.
Diego A. Riveros-Iregui; Brian L. McGlynn
2009-01-01
We investigated the spatial and temporal variability of soil CO2 efflux across 62 sites of a 393-ha complex watershed of the northern Rocky Mountains. Growing season (83 day) cumulative soil CO2 efflux varied from ~300 to ~2000 g CO2 m-2, depending upon landscape position, with a median of 879.8 g CO2 m-2. Our findings revealed that highest soil CO2 efflux rates were...
Injection of Super-Critical CO2 in Brine Saturated Sandstone:
NASA Astrophysics Data System (ADS)
Ott, Holger; de Kloe, Kees; Taberner, Conxita; Marcelis, Fons; Makurat, Axel
2010-05-01
Presently, large-scale geological sequestration of CO2, originating from sources like fossil-fueled power plants and contaminated gas production, is seen as an option to reduce anthropogenic emission of greenhouse gases to the atmosphere. Deep saline aquifers and depleted oil and gas fields are potential subsurface deposits for CO2. Injected CO2, however, interacts physically and chemically with the formation leading to uncertainties for CCS projects. One of these uncertainties is related to a dry-out zone that is likely to form around the well bore owing to the injection of dry CO2. Precipitation of salt (mainly halite) that is associated with that drying out of a saline formation has the potential to impair injectivity, and could even lead to the loss of a well. If dry (or under-saturated), super-critical (SC) CO2 is injected into water-bearing geological formations like saline aquifers, water is removed by either advection of the aqueous phase or by evaporation of water and subsequent advection in the injected CO2-rich phase. Both mechanisms act in parallel, however while advection of the aqueous phase decreases with increasing CO2 saturation (diminished mobility), evaporation becomes increasingly important as the aqueous phase becomes immobile. Below residual water saturation, only evaporation takes place and the formation dries out if no additional source of water is available. If water evaporates, the salts originally present in the water are left behind. In case of highly saline formations, the amount of salt that potentially precipitates per unit volume can be quite substantial. It depends on salinity, the solubility limit of water in the CO2 rich phase, and on the ratio of advection and evaporation rates. Since saturations and flow rates cover a large range as functions of space and time close to the well bore, there is no easy answer to the questions whether, where and how salt precipitation impacts injectivity. The present paper presents results of core-flood experiments that were performed to investigate the spatial and temporal precipitation of salt due to the injection of dry CO2 and to understand the underlying mechanisms; super-critical CO2 was injected into brine-saturated sandstone (Berea) samples under realistic pressure and temperature conditions and at high injection rate. To match flow rates that are realistic for the near well-bore area, the experiments were performed on small-scale samples with a cross section of less than 1 cm2. Density profiles were measured by mCT (micro computer tomography) scanning during injection. Reference scans and brine doping with a contrast agent allow the distinction between the CO2-rich phase, the aqueous phase and precipitated solid salt even on pore scale. By means of mCT scanning, spatial and time evolution of halite precipitation in rock samples have been observed under sequestration conditions. Pattern formation of solid salt along the main flow direction as well as a cross-sectional pattern formation has been found. However, while there are areas of high local solid salt accumulation, permeability remained unaffected, which might be a result of the precipitation pattern. The results were complemented by (ex-situ) eSEM/EDAX measurements to study where and how salt precipitates on the microscopic scale. The SEM results cannot be directly translated to in-situ conditions, as salt migrates post-experiment at ambient conditions, but give valuable insight into microscopic processes controlling deposition. Numerical simulations have been performed for a qualitative understanding of principle mechanisms and show a dependency of the observed profile on injection rate and capillary pressure.
Zhao, Xiulan; Yang, Feng; Chen, Junhan; Ding, Li; Liu, Xiyan; Yao, Fengrui; Li, Meihui; Zhang, Daqi; Zhang, Zeyao; Liu, Xu; Yang, Juan; Liu, Kaihui; Li, Yan
2018-04-19
Bimetallic catalysts play important roles in the selective growth of single-walled carbon nanotubes (SWNTs). Using the simple salts (NH4)6W7O24·6H2O and Co(CH3COO)2·4H2O as precursors, tungsten-cobalt catalysts were prepared. The catalysts were composed of W6Co7 intermetallic compounds and tungsten-dispersed cobalt. With the increase of the W/Co ratio in the precursors, the content of W6Co7 was increased. Because the W6Co7 intermetallic compound can enable the chirality specified growth of SWNTs, the selectivity of the resulting SWNTs is improved at a higher W/Co ratio. At a W/Co ratio of 6 : 4 and under optimized chemical vapor deposition conditions, we realized the direct growth of semiconducting SWNTs with the purity of ∼96%, in which ∼62% are (14, 4) tubes. Using salts as precursors to prepare tungsten-cobalt bimetallic catalysts is flexible and convenient. This offers an efficient pathway for the large-scale preparation of chirality enriched semiconducting SWNTs.
Geomechanical effects on CO 2 leakage through fault zones during large-scale underground injection
DOE Office of Scientific and Technical Information (OSTI.GOV)
Rinaldi, Antonio P.; Rutqvist, Jonny; Cappa, Frédéric
2013-12-01
The importance of geomechanics—including the potential for faults to reactivate during large-scale geologic carbon sequestration operations—has recently become more widely recognized. However, notwithstanding the potential for triggering notable (felt) seismic events, the potential for buoyancy-driven CO 2 to reach potable groundwater and the ground surface is actually more important from public safety and storage-efficiency perspectives. In this context, this paper extends the previous studies on the geomechanical modeling of fault responses during underground carbon dioxide injection, focusing on the short-term integrity of the sealing caprock, and hence on the potential for leakage of either brine or CO 2 to reachmore » the shallow groundwater aquifers during active injection. We consider stress/strain-dependent permeability and study the leakage through the fault zone as its permeability changes during a reactivation, also causing seismicity. We analyze several scenarios related to the volume of CO 2 injected (and hence as a function of the overpressure), involving both minor and major faults, and analyze the profile risks of leakage for different stress/strain-permeability coupling functions. We conclude that whereas it is very difficult to predict how much fault permeability could change upon reactivation, this process can have a significant impact on the leakage rate. Moreover, our analysis shows that induced seismicity associated with fault reactivation may not necessarily open up a new flow path for leakage. Results show a poor correlation between magnitude and amount of fluid leakage, meaning that a single event is generally not enough to substantially change the permeability along the entire fault length. Finally, and consequently, even if some changes in permeability occur, this does not mean that the CO 2 will migrate up along the entire fault, breaking through the caprock to enter the overlying aquifer.« less
Synthesis and characterization of α-cobalt hydroxide nanobelts
NASA Astrophysics Data System (ADS)
Tian, L.; Zhu, J. L.; Chen, L.; An, B.; Liu, Q. Q.; Huang, K. L.
2011-08-01
α-Cobalt hydroxide was synthesized by a facile hydrothermal process from Co(Ac)2 and NH3·H2O in the presence of 1,3-propanediol. The large-scale-prepared cobalt hydroxide has a uniform nanobelt morphology with a considerably high aspect-ratio more than 20 which may be advantageous for exploration of their physicochemical properties. This synthetic method is convenient, economical, and controllable. The samples were characterized by powder X-ray diffraction, energy dispersive spectrum, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, CHN element analysis, thermogravimetric and differential-thermogravimetric analysis, which revealed the compound is lamellar structural cobalt organic-inorganic hybrid with the chemical formula of Co(OH)1.49(NH3)0.01(CO3 2-)0.22(Ac-)0.07(H2O)0.11 and single-crystalline.
Design of electrolyzer for carbon dioxide conversion to fuels and chemicals
NASA Astrophysics Data System (ADS)
Rosen, Jonathan S.
The stabilization of global atmospheric CO2 levels requires a transition towards a renewable energy based economy as well as methods for handling current CO2 output from fossil fuels. Challenges with renewable energy intermittency have thus far limited the use of these alternative energy sources to only a fraction of the current energy portfolio. To enable more widespread use of renewable energy systems, methods of large scale energy storage must be developed to store excess renewable energy when demand is low and allow for combined use of energy storage and renewable systems when demand is high. To date, no one technique has demonstrated energy storage methods on the gigawatt scale needed for integration with renewable sources; therefore the development of suitable energy storage technologies, such as CO2 electrolysis to fuels is needed. In this work, research efforts have focused on two major thrusts related to electrochemical methods of CO 2 conversion to fuels. The first thrust focuses on the synthesis and design of highly efficient anode and cathode catalysts with emphasis on understanding structure-property relationships. A second thrust focuses on the design of novel electrochemical devices for CO2 conversion and integration of synthesized materials into flow cell systems. On the anode side, the synthesis of highly active catalysts using abundant transition metals is crucial to reducing capital costs and enabling widespread use of electrochemical CO2 conversion devices. Highly active mesoporous Co3O4 and metal-substituted Co3O4 water oxidation catalysts were designed to investigate the role of the spinel structure on water oxidation activity. Further analysis of metal substituted samples reveal the importance of the octahedral sites in the spinel structure, which was later used to design an Mg-Co3O4 sample with improved water oxidation activity. The design of efficient cathode materials which can selectivity reduce CO2 to fuels and chemicals is critical to the widespread use of CO2 electrolysis. A nanoporous Ag material was synthesized through a dealloying technique able to operate with less than 0.5 V overpotential and high selectivity towards CO. CO is a valuable intermediate chemical which can used in Fischer-Tropsch or Gas-to-liquids technologies to produce liquids fuels. A detailed investigation of nanostructured Ag catalysts found stepped sites to be responsible for enhanced CO2 reduction activity due to improved stabilization of the COOH intermediate on the catalyst surface. In addition, an low-cost Zn dendrite electrocatalyst was developed using an electroplating technique. Low coordinated sites formed through electrodeposition demonstrated the suppression of hydrogen evolution while maintaining CO activity. The Zn dendrite electrocatalyst was further examined using a newly developed in situ X-ray absorption technique able to probe catalyst stability and crystalline structure under CO2 reduction operating conditions. A final hurdle in the realization of CO2 electrolysis technologies is the integration of catalysts into working flow cell devices. To address this issue and enable testing in a practical system, a highly efficient and robust CO2 electrolysis flow cell was designed including the scale up of the previous nanoporous Ag synthesis procedure. Using the modified porous Ag catalyst, currents in the Amp regime were demonstrated approaching rates needed for energy storage applications. Stability on the order of days was successfully demonstrated due to use of robust system components and conditions suitable for process scale up.
NASA Technical Reports Server (NTRS)
1985-01-01
The goal of defining a CO2 laser transmitter approach suited to Shuttle Coherent Atmospheric Lidar Experiment (SCALE) requirements is discussed. The adaptation of the existing WINDVAN system to the shuttle environment is addressed. The size, weight, reliability, and efficiency of the existing WINDVAN system are largely compatible with SCALE requirements. Repacking is needed for compatibility with vacuum and thermal environments. Changes are required to ensure survival through launch and landing, mechanical, vibration, and acoustic loads. Existing WINDVAN thermal management approaches depending on convection need to be upgraded zero gravity operations.
Role of Atmospheric CO2 in the Ice Ages (Invited)
NASA Astrophysics Data System (ADS)
Toggweiler, J. R.
2010-12-01
Ice cores from Antarctica provide our most highly resolved records of glacial-interglacial climate change. They feature big transitions every 100,000 years or so in which Antarctica warms by up to 10 deg. C while the level of atmospheric CO2 rises by up to 100 ppm. We have no other records like these from any other location, so the assumption is often made that the Earth's mean temperature varies like the temperatures in Antarctica. The striking co-variation between the two records is taken to mean 1) that there is a causal relationship between the global temperature and atmospheric CO2 and 2) that atmospheric CO2 is a powerful agent of climate change during the ice ages. The problem is that the mechanism most often invoked to explain the CO2 variations operates right next to Antarctica and, as such, provides a fairly direct way to explain the temperature variations in Antarctica as well. If so, Antarctic temperatures go up and down for the same reason that atmospheric CO2 goes up and down, in which case no causation can be inferred. Climate models suggest that the 100-ppm CO2 increases during the big transitions did not increase surface temperatures by more than 2 deg. C. This is not nearly enough to explain the observed variability. A better reason for thinking that atmospheric CO2 is important is that its temporal variations are concentrated in the 100,000-yr band. In my presentation I will argue that atmospheric CO2 is important because it has the longest time scale in the system. We observe empirically that atmospheric CO2 remains low for 50,000 years during the second half of each 100,000-yr cycle. The northern ice sheets become especially large toward the ends of these intervals, and it is large ice sheets that make the Earth especially cold. This leads me to conclude that atmospheric CO2 is important because of its slow and persistent influence on the northern ice sheets over the second half of each 100,000-yr cycle.
Monitoring Atmospheric CO2 From Space: Challenge & Approach
NASA Technical Reports Server (NTRS)
Lin, Bing; Harrison, F. Wallace; Nehrir, Amin; Browell, Edward; Dobler, Jeremy; Campbell, Joel; Meadows, Byron; Obland, Michael; Kooi, Susan; Fan, Tai-Fang;
2015-01-01
Atmospheric CO2 is the key radiative forcing for the Earth's climate and may contribute a major part of the Earth's warming during the past 150 years. Advanced knowledge on the CO2 distributions and changes can lead considerable model improvements in predictions of the Earth's future climate. Large uncertainties in the predictions have been found for decades owing to limited CO2 observations. To obtain precise measurements of atmospheric CO2, certain challenges have to be overcome. For an example, global annual means of the CO2 are rather stable, but, have a very small increasing trend that is significant for multi-decadal long-term climate. At short time scales (a second to a few hours), regional and subcontinental gradients in the CO2 concentration are very small and only in an order of a few parts per million (ppm) compared to the mean atmospheric CO2 concentration of about 400 ppm, which requires atmospheric CO2 space monitoring systems with extremely high accuracy and precision (about 0.5 ppm or 0.125%) in spatiotemporal scales around 75 km and 10-s. It also requires a decadal-scale system stability. Furthermore, rapid changes in high latitude environments such as melting ice, snow and frozen soil, persistent thin cirrus clouds in Amazon and other tropical areas, and harsh weather conditions over Southern Ocean all increase difficulties in satellite atmospheric CO2 observations. Space lidar approaches using Integrated Path Differential Absorption (IPDA) technique are considered to be capable of obtaining precise CO2 measurements and, thus, have been proposed by various studies including the 2007 Decadal Survey (DS) of the U.S. National Research Council. This study considers to use the Intensity-Modulated Continuous-Wave (IM-CW) lidar to monitor global atmospheric CO2 distribution and variability from space. Development and demonstration of space lidar for atmospheric CO2 measurements have been made through joint adventure of NASA Langley Research Center and Exelis, Inc. As prototype space IPDA lidars, airborne laser absorption lidar systems operating in 1.57 CO2 absorption band have been developed and tested through lab, ground-based range, and flight campaigns. Very encouraging results have been obtained. The signal-to-noise ratio (SNR) for clear sky IPDA measurements of CO2 differential absorption optical depth (DAOD) for a 10-s integration over vegetated areas with about 10 km range was found to be as high as 1300, resulting in an error 0.077% or equivalent CO2 mixing ratio (XCO2) column precision of 0.3 ppm. Precise range measurements using the IM-CW lidar approach were also achieved, and the uncertainties have been shown to be at sub meter level. Based on the airborne lidar development, space lidar and atmospheric CO2 observations are simulated. It shows that with the IM-CW approach, accurate atmospheric CO2 measurements can be achieved from space, and a space mission such as that proposed by the DS will meet science goals of atmospheric CO2 monitoring.
``Large''- vs Small-scale friction control in turbulent channel flow
NASA Astrophysics Data System (ADS)
Canton, Jacopo; Örlü, Ramis; Chin, Cheng; Schlatter, Philipp
2017-11-01
We reconsider the ``large-scale'' control scheme proposed by Hussain and co-workers (Phys. Fluids 10, 1049-1051 1998 and Phys. Rev. Fluids, 2, 62601 2017), using new direct numerical simulations (DNS). The DNS are performed in a turbulent channel at friction Reynolds number Reτ of up to 550 in order to eliminate low-Reynolds-number effects. The purpose of the present contribution is to re-assess this control method in the light of more modern developments in the field, in particular also related to the discovery of (very) large-scale motions. The goals of the paper are as follows: First, we want to better characterise the physics of the control, and assess what external contribution (vortices, forcing, wall motion) are actually needed. Then, we investigate the optimal parameters and, finally, determine which aspects of this control technique actually scale in outer units and can therefore be of use in practical applications. In addition to discussing the mentioned drag-reduction effects, the present contribution will also address the potential effect of the naturally occurring large-scale motions on frictional drag, and give indications on the physical processes for potential drag reduction possible at all Reynolds numbers.
ASTE Surveys of Galactic Star-Forming Regions
NASA Astrophysics Data System (ADS)
Kohno, Kotaro
2008-05-01
We report some recent highlights on the observational studies of Galactic star formation based on surveys using the Atacama Submillimeter Telescope Experiment (ASTE), a new 10 m telescope in the Atacama desert in northern Chile (Kohno et al., 2008, ApSS, 313, 279). The highlights will include (1) a large scale CO(3-2) imaging survey of the Galactic Center, unveiling the presence of numerous compact high velocity clouds with high CO(3-2)/CO(1-0) ratios as a "fossil” of the recent burst of star formation in the Galactic Center region (Oka et al., 2007, PASJ, 59, 15; Nagai et al., 2007, PASJ, 59, 25; Tanaka et al., 2007, PASJ, 59, 323), (2) a large scale CO(3-2) imaging survey of the Sgr arm and inter-am regions, revealing the distinct difference on the morphology and physical property of molecular gas between the arm and inter-arm regions for the first time (Sawada, Koda, et al., in prep.), and (3) a wide area 1.1 mm imaging survey of Southern low mass star-forming regions such as Chamaeleon and Lupus molecular clouds using the bolometer camera AzTEC (Wilson et al., 2008, MNRAS, in press) mounted on ASTE, yielding detections of starless cores with a very low mass detection limist down to 0.1 solar masses (Hiramatsu, Tsukagoshi, Kawabe et al., in prep.). Related topics on the massive star-forming regions in very nearby galaxies such as LMC (Minamidani et al., 2008, ApJS, in press) and M 33 (Tosaki et al., 2007, ApJ, 664, L27; Onodera et al., in prep.; Komugi et al., in prep.) will also be reviewed.
NASA Astrophysics Data System (ADS)
Siqueira, M. B.; Katul, G. G.
2009-12-01
A one-dimensional analytical model that predicts foliage CO2 uptake rates, turbulent fluxes, and mean concentration throughout the roughness sub-layer (RSL), a layer that extends from the ground surface up to 5 times the canopy height (h), is proposed. The model combines the mean continuity equation for CO2 with first-order closure principles for turbulent fluxes and simplified physiological and radiative transfer schemes for foliage uptake. This combination results in a second-order ordinary differential equation in which it is imposed soil respiration (RE) as lower and CO2 concentration well above the RSL as upper boundary conditions. An inverse version of the model was tested against data sets from two contrasting ecosystems: a tropical forest (TF, h=40 m) and a managed irrigated rice canopy (RC, h=0.7 m) - with good agreement noted between modeled and measured mean CO2 concentration profiles within the entire RSL (see figure). Sensitivity analysis on the model parameters revealed a plausible scaling regime between them and a dimensionless parameter defined by the ratio between external (RE) and internal (stomatal conductance) characteristics controlling the CO2 exchange process. The model can be used to infer the thickness of the RSL for CO2 exchange, the inequality in zero-plane displacement between CO2 and momentum, and its consequences on modeled CO2 fluxes. A simplified version of the solution is well suited for being incorporated into large-scale climate models. Furthermore, the model framework here can be used to a priori estimate relative contributions from the soil surface and the atmosphere to canopy-air CO2 concentration thereby making it synergetic to stable isotopes studies. Panels a) and c): Profiles of normalized measured leaf area density distribution (a) for TF and RC, respectively. Continuous lines are the constant a used in the model and dashed lines represent data-derived profiles. Panels b) and d) are modeled and ensemble-averaged measured CO2 profiles reference to the uppermost measured point for TF and RC, respectively.
Jacques-Joseph Ébelmen, the founder of earth system science
NASA Astrophysics Data System (ADS)
Berner, Robert A.
2012-11-01
The fundamental principles of the factors affecting the global carbon cycle, the global sulfur cycle and the levels of atmospheric CO2 and O2 over long-term (multimillion year) time scales were first elucidated by Jacques-Joseph Ébelmen in 1845. He covered all major processes in such a correct manner that no appreciable changes in them have been elucidated since then. Unfortunately, his ideas were forgotten and were independently deduced by others only 100 to 150 years later. In this article, his reasoning is shown in detail, via a number of original quotations, and the results of a mathematical model by the author for CO2 and O2 over the Phanerozoic Eon (past 542 million years) are presented. In agreement with Ébelmen's predictions, there apparently have been large changes in the levels of atmospheric CO2 and O2 over geologic time.
NASA Astrophysics Data System (ADS)
Rani, Sanju; Bao, Ningzhong; Roy, Somnath C.
2014-01-01
A viable option for recycling carbon dioxide is through the sunlight-powered photocatalytic conversion of CO2 and water vapor into hydrocarbon fuels over highly active nanocatalysts. With photocatalytic CO2 reduction sunlight, a renewable energy source as durable as the sun, is used to drive the catalytic reaction with the resultant fuel products compatible with the current hydrocarbon-based energy infrastructure. The use of co-catalyst (Cu, Pt)-sensitized TiO2 nanoparticle wafers in the photocatalytic conversion of CO2 and water vapor to hydrocarbon fuels, with optimal humidity levels and exposure times established. We also attempted to increase product formation by sputtering both co-catalysts on the nanoparticle wafer's surface, with the resulting product rates significantly higher than that of either the Cu or Pt coated samples. When the TiO2 nanoparticle wafers are used in a flow-through membrane implementation we find a significant increase in product rates of formation, including methane, hydrogen, and carbon monoxide. We believe that nanocatalyst-based flow-through membranes are a viable route for achieving large-scale and low cost photocatalytic solar fuel production.
NASA Astrophysics Data System (ADS)
Dubey, M. K.; Parker, H. A.; Wennberg, P. O.; Wunch, D.; Jacobson, A. R.; Kawa, S. R.; Keppel-Aleks, G.; Basu, S.; O'Dell, C.; Frankenberg, C.; Michalak, A. M.; Baker, D. F.; Christofferson, B.; Restrepo-Coupe, N.; Saleska, S. R.; De Araujo, A. C.; Miller, J. B.
2016-12-01
The Amazon basin stores 150-200 PgC, exchanges 18 PgC with the atmosphere every year and has taken up 0.42-0.65 PgC/y over the past two decades. Despite its global significance, the response of the tropical carbon cycle to climate variability and change is ill constrained as evidenced by the large negative and positive feedbacks in future climate simulations. The complex interplay of radiation, water and ecosystem phenology remains unresolved in current tropical ecosystem models. We use high frequency regional scale TCCON observations of column CO2, CO and CH4 near Manaus, Brazil that began in October 2014 to understand the aforementioned interplay of processes in regulating biosphere-atmosphere exchange. We observe a robust daily column CO2 uptake of about 2 ppm (4 ppm to 0.5 ppm) over 8 hours and evaluate how it changes as we transition to the dry season. Back-trajectory calculations show that the daily CO2 uptake footprint is terrestrial and influenced by the heterogeneity of the Amazon rain forests. The column CO falls from above 120 ppb to below 80 ppb as we transition from the biomass burning to wet seasons. The daily mean column CO2 rises by 3 ppm from October through June. Removal of biomass burning, secular CO2 increase and variations from transport (by Carbon tracker simulations) implies an increase of 2.3 ppm results from tropical biospheric processes (respiration and photosynthesis). This is consistent with ground-based remote sensing and eddy flux observations that indicate that leaf development and demography drives the tropical carbon cycle in regions that are not water limited and is not considered in current models. We compare our observations with output from 7 CO2 inversion transport models with assimilated meteorology and find that while 5 models reproduce the CO2 seasonal cycle all of them under predict the daily drawdown of CO2 by a factor of 3. This indicates that the CO2 flux partitioning between photosynthesis and respiration is incorrect in current models and needs refinement. Finally, we use OCO-2 column CO2 and Solar Induced Fluorescence observations over the Amazon to elucidate the tropical carbon cycle mechanisms at larger scales.
Development of WRF-CO2 4DVAR Data Assimilation System
NASA Astrophysics Data System (ADS)
Zheng, T.; French, N. H. F.
2016-12-01
Four dimensional variational (4DVar) assimilation systems have been widely used for CO2 inverse modeling at global scale. At regional scale, however, 4DVar assimilation systems have been lacking. At present, most regional CO2 inverse models use Lagrangian particle backward trajectory tools to compute influence function in an analytical/synthesis framework. To provide a 4DVar based alternative, we developed WRF-CO2 4DVAR based on Weather Research and Forecasting (WRF), its chemistry extension (WRF-Chem), and its data assimilation system (WRFDA/WRFPLUS). Different from WRFDA, WRF-CO2 4DVAR does not optimize meteorology initial condition, instead it solves for the optimized CO2 surface fluxes (sources/sink) constrained by atmospheric CO2 observations. Based on WRFPLUS, we developed tangent linear and adjoint code for CO2 emission, advection, vertical mixing in boundary layer, and convective transport. Furthermore, we implemented an incremental algorithm to solve for optimized CO2 emission scaling factors by iteratively minimizing the cost function in a Bayes framework. The model sensitivity (of atmospheric CO2 with respect to emission scaling factor) calculated by tangent linear and adjoint model agrees well with that calculated by finite difference, indicating the validity of the newly developed code. The effectiveness of WRF-CO2 4DVar for inverse modeling is tested using forward-model generated pseudo-observation data in two experiments: first-guess CO2 fluxes has a 50% overestimation in the first case and 50% underestimation in the second. In both cases, WRF-CO2 4DVar reduces cost function to less than 10-4 of its initial values in less than 20 iterations and successfully recovers the true values of emission scaling factors. We expect future applications of WRF-CO2 4DVar with satellite observations will provide insights for CO2 regional inverse modeling, including the impacts of model transport error in vertical mixing.
NASA Astrophysics Data System (ADS)
Yıldız, U. A.; Kristensen, L. E.; van Dishoeck, E. F.; Hogerheijde, M. R.; Karska, A.; Belloche, A.; Endo, A.; Frieswijk, W.; Güsten, R.; van Kempen, T. A.; Leurini, S.; Nagy, Z.; Pérez-Beaupuits, J. P.; Risacher, C.; van der Marel, N.; van Weeren, R. J.; Wyrowski, F.
2015-04-01
Context. During the embedded stage of star formation, bipolar molecular outflows and UV radiation from the protostar are important feedback processes. Both processes reflect the accretion onto the forming star and affect subsequent collapse or fragmentation of the cloud. Aims: Our aim is to quantify the feedback, mechanical and radiative, for a large sample of low-mass sources in a consistent manner. The outflow activity is compared to radiative feedback in the form of UV heating by the accreting protostar to search for correlations and evolutionary trends. Methods: Large-scale maps of 26 young stellar objects, which are part of the Herschel WISH key program are obtained using the CHAMP+ instrument on the Atacama Pathfinder EXperiment (12CO and 13CO 6-5; Eup ~ 100 K), and the HARP-B instrument on the James Clerk Maxwell Telescope (12CO and 13CO 3-2; Eup ~ 30 K). The maps have high spatial resolution, particularly the CO 6-5 maps taken with a 9″ beam, resolving the morphology of the outflows. The maps are used to determine outflow parameters and the results are compared with higher-J CO lines obtained with Herschel. Envelope models are used to quantify the amount of UV-heated gas and its temperature from 13CO 6-5 observations. Results: All sources in our sample show outflow activity, with the spatial extent decreasing from the Class 0 to the Class I stage. Consistent with previous studies, the outflow force, FCO, is larger for Class 0 sources than for Class I sources, even if their luminosities are comparable. The outflowing gas typically extends to much greater distances than the power-law envelope and therefore influences the surrounding cloud material directly. Comparison of the CO 6-5 results with HIFI H2O and PACS high-J CO lines, both tracing currently shocked gas, shows that the two components are linked, even though the transitions do not probe the same gas. The link does not extend down to CO 3-2. The conclusion is that CO 6-5 depends on the shock characteristics (density and velocity), whereas CO 3-2 is more sensitive to conditions in the surrounding environment (density). The radiative feedback is responsible for increasing the gas temperature by a factor of two, up to 30-50 K, on scales of a few thousand AU, particularly along the direction of the outflow. The mass of the UV heated gas exceeds the mass contained in the entrained outflow in the inner ~3000 AU and is therefore at least as important on small scales. Appendix A is available in electronic form at http://www.aanda.orgThe CHAMP+ maps (data cubes) are only available at the CDS via anonymous ftp to http://cdsarc.u-strasbg.fr (ftp://130.79.128.5) or via http://cdsarc.u-strasbg.fr/viz-bin/qcat?J/A+A/576/A109
Seo, Yongwon; Jo, Sung-Ho; Ryu, Chong Kul; Yi, Chang-Keun
2007-10-01
CO(2) capture from flue gas using a sodium-based solid sorbent was investigated in a bubbling fluidized-bed reactor. Carbonation and regeneration temperature on CO(2) removal was determined. The extent of the chemical reactivity after carbonation or regeneration was characterized via (13)C NMR. In addition, the physical properties of the sorbent such as pore size, pore volume, and surface area after carbonation or regeneration were measured by gas adsorption method (BET). With water vapor pretreatment, near complete CO(2) removal was initially achieved and maintained for about 1-2min at 50 degrees C with 2s gas residence time, while without proper water vapor pretreatment CO(2) removal abruptly decreased from the beginning. Carbonation was effective at the lower temperature over the 50-70 degrees C temperature range, while regeneration more effective at the higher temperature over the 135-300 degrees C temperature range. To maintain the initial 90% CO(2) removal, it would be necessary to keep the regeneration temperature higher than about 135 degrees C. The results obtained in this study can be used as basic data for designing and operating a large scale CO(2) capture process with two fluidized-bed reactors.
Observability of planet-disc interactions in CO kinematics
NASA Astrophysics Data System (ADS)
Pérez, Sebastián; Casassus, S.; Benítez-Llambay, P.
2018-06-01
Empirical evidence of planets in gas-rich circumstellar discs is required to constrain giant planet formation theories. Here we study the kinematic patterns which arise from planet-disc interactions and their observability in CO rotational emission lines. We perform three-dimensional hydrodynamical simulations of single giant planets, and predict the emergent intensity field with radiative transfer. Pressure gradients at planet-carved gaps, spiral wakes and vortices bear strong kinematic counterparts. The iso-velocity contours in the CO(2-1) line centroids vo reveal large-scale perturbations, corresponding to abrupt transitions from below sub-Keplerian to super-Keplerian rotation along with radial and vertical flows. The increase in line optical depth at the edge of the gap also modulates vo, but this is a mild effect compared to the dynamical imprint of the planet-disc interaction. The large-scale deviations from the Keplerian rotation thus allow the planets to be indirectly detected via the first moment maps of molecular gas tracers, at ALMA angular resolutions. The strength of these deviations depends on the mass of the perturber. This initial study paves the way to eventually determine the mass of the planet by comparison with more detailed models.
Design of high-activity single-atom catalysts via n-p codoping
NASA Astrophysics Data System (ADS)
Wang, Xiaonan; Zhou, Haiyan; Zhang, Xiaoyang; Jia, Jianfeng; Wu, Haishun
2018-03-01
The large-scale synthesis of stable single-atom catalysts (SACs) in experiments remains a significant challenge due to high surface free energy of metal atom. Here, we propose a concise n-p codoping approach, and find it can not only disperse the relatively inexpensive metal, copper (Cu), onto boron (B)-doped graphene, but also result in high-activity SACs. We use CO oxidation on B/Cu codoped graphene as a prototype example, and demonstrate that: (1) a stable SAC can be formed by stronger electrostatic attraction between the metal atom (n-type Cu) and support (p-type B-doped graphene). (2) the energy barrier of the prototype CO oxidation on B/Cu codoped graphene is 0.536 eV by the Eley-Rideal mechanism. Further analysis shows that the spin selection rule can provide well theoretical insight into high activity of our suggested SAC. The concept of n-p codoping may lead to new strategy in large-scale synthesis of stable single-atom catalysts.
NASA Astrophysics Data System (ADS)
Paris, Jean-Daniel; Belan, Boris D.; Ancellet, Gérard; Nédélec, Philippe; Arshinov, Mikhail Yu.; Pruvost, Arnaud; Berchet, Antoine; Arzoumanian, Emmanuel; Pison, Isabelle; Ciais, Philippe; Law, Kathy
2014-05-01
Despite the unique scientific value of better knowing atmospheric composition over Siberia, regional observations of the tropospheric composition over this region are still lacking. Large local anthropogenic emissions, strong ecosystem gas exchange across the vast forest expanse, and processes feeding back to global climate such as wetlands CH4 emissions, seabed hydrates destabilization and degrading permafrost make this region particularly crucial to investigate. We aim at addressing this need in the YAK-AEROSIB program by collecting high-precision in-situ measurements of the vertical distribution of CO2, CH4, CO, O3, black carbon and ultrafine particles distribution in the Siberian troposphere, as well as other parameters including aerosol lidar profiles, on a pan-Siberian aircraft transect. Campaigns are performed almost annually since 2006 until now on this regular route, while special campaigns are occasionnally arranged to sample the troposphere elsewere (e.g. Russian Arctic coast). We show the background tropospheric composition obtained from these surveys, the variability and the impact of large-scale transport of anthropogenic emissions from Europe and Asia, as well as the impact of biomass burning plumes both from local wildfires (2012) and from remote sources elsewhere in Asia. Long range transport of anthropogenic emissions is shown to have a discernible impact on O3 distribution, although its lower-tropospheric variability is largely driven by surface deposition. Regional sources and sinks drive the lower troposphere CO2 and CH4 concentrations. Recent efforts aim at better understanding the respective role of CH4 emission processes (including methanogenesis in wetlands and emissions by wildfires) in driving its large scale atmospheric variability over the region. Generally, the YAK AEROSIB provide unique observations over Siberia, documenting both direct impact of regional sources and aged air masses experiencing long range transport toward the high Arctic.
Three-dimensional Distribution of Greenhouse Gas Concentrations over Megacities Observed by GOSAT
NASA Astrophysics Data System (ADS)
Kikuchi, N.; Kuze, A.; Kataoka, F.; Shiomi, K.; Hashimoto, M.; Suto, H.; Knuteson, R. O.; Iraci, L. T.; Yates, E. L.; Gore, W.; Tanaka, T.
2017-12-01
Since the launch in January 2009, TANSO-FTS onboard GOSAT continues to observe the global distribution of carbon dioxide (CO2) and methane (CH4) concentrations. The regular grid observation is the standard observation mode, because a reduction of the uncertainty in the surface fluxes of CO2 and CH4in a subcontinental scale is one of the prime objectives of GOSAT. To meet an increasing demand for monitoring the anthropogenic emission of the greenhouses gases from large cities, GOSAT has carried out extensive target mode observations over several megacities since 2016. Although the footprint of TANSO-FTS is relatively large, the flexible pointing mechanism enables us to cover a city and the surrounding area at the same time. Another advantage of GOSAT TANSO-FTS is that it measures both SWIR and TIR spectra at the same footprint. By adding TIR windows to the existing SWIR retrieval algorithm, we can get the degrees of freedom larger than 2 for CO2 concentrations. This means that we can retrieve not only the column averaged concentration of CO2 (XCO2), but also the two-layer structure of CO2 concentrations, independent of the a priori constraint. In this study, we present three-dimensional distributions of CO2 and CH4 retrieved from GOSAT observations over several megacities including New York City. Fig. 1 shows the seasonal variation of XCO2 over New York City in 2016 covered by 16 footprints of GOSAT observations. A three-dimensional representation of CO2 concentrations is shown in Fig. 2 observed on September 15, 2016. In this example, CO2 concentrations were lower in the lower atmosphere in most of GOSAT footprints, indicating that CO2 was depleted in the lower atmosphere as expected for the summer season. In the winter season, the CO2 concentrations were enhanced in the lower atmosphere as shown in Fig. 3. This example indicates that GOSAT can detect variations in both the column and the vertical structure of CO2 over megacities. Similar analyses are underway for other megacities and will be shown in the presentation.
Geoengineering, marine microalgae, and climate stabilization in the 21st century
NASA Astrophysics Data System (ADS)
Greene, Charles H.; Huntley, Mark E.; Archibald, Ian; Gerber, Léda N.; Sills, Deborah L.; Granados, Joe; Beal, Colin M.; Walsh, Michael J.
2017-03-01
Society has set ambitious targets for stabilizing mean global temperature. To attain these targets, it will have to reduce CO2 emissions to near zero by mid-century and subsequently remove CO2 from the atmosphere during the latter half of the century. There is a recognized need to develop technologies for CO2 removal; however, attempts to develop direct air-capture systems have faced both energetic and financial constraints. Recently, BioEnergy with Carbon Capture and Storage (BECCS) has emerged as a leading candidate for removing CO2 from the atmosphere. However, BECCS can have negative consequences on land, nutrient, and water use as well as biodiversity and food production. Here, we describe an alternative approach based on the large-scale industrial production of marine microalgae. When cultivated with proper attention to power, carbon, and nutrient sources, microalgae can be processed to produce a variety of biopetroleum products, including carbon-neutral biofuels for the transportation sector and long-lived, potentially carbon-negative construction materials for the built environment. In addition to these direct roles in mitigating and potentially reversing the effects of fossil CO2 emissions, microalgae can also play an important indirect role. As microalgae exhibit much higher primary production rates than terrestrial plants, they require much less land area to produce an equivalent amount of bioenergy and/or food. On a global scale, the avoided emissions resulting from displacement of conventional agriculture may exceed the benefits of microalgae biofuels in achieving the climate stabilization goals.
Chen, Zhenwei; Zhang, Lei; Zhang, Guo
2016-01-01
Co-registration is one of the most important steps in interferometric synthetic aperture radar (InSAR) data processing. The standard offset-measurement method based on cross-correlating uniformly distributed patches takes no account of specific geometric transformation between images or characteristics of ground scatterers. Hence, it is inefficient and difficult to obtain satisfying co-registration results for image pairs with relatively big distortion or large incoherent areas. Given this, an improved co-registration strategy is proposed in this paper which takes both the geometric features and image content into consideration. Firstly, some geometric transformations including scale, flip, rotation, and shear between images were eliminated based on the geometrical information, and the initial co-registration polynomial was obtained. Then the registration points were automatically detected by integrating the signal-to-clutter-ratio (SCR) thresholds and the amplitude information, and a further co-registration process was performed to refine the polynomial. Several comparison experiments were carried out using 2 TerraSAR-X data from the Hong Kong airport and 21 PALSAR data from the Donghai Bridge. Experiment results demonstrate that the proposed method brings accuracy and efficiency improvements for co-registration and processing abilities in the cases of big distortion between images or large incoherent areas in the images. For most co-registrations, the proposed method can enhance the reliability and applicability of co-registration and thus promote the automation to a higher level. PMID:27649207
Chen, Zhenwei; Zhang, Lei; Zhang, Guo
2016-09-17
Co-registration is one of the most important steps in interferometric synthetic aperture radar (InSAR) data processing. The standard offset-measurement method based on cross-correlating uniformly distributed patches takes no account of specific geometric transformation between images or characteristics of ground scatterers. Hence, it is inefficient and difficult to obtain satisfying co-registration results for image pairs with relatively big distortion or large incoherent areas. Given this, an improved co-registration strategy is proposed in this paper which takes both the geometric features and image content into consideration. Firstly, some geometric transformations including scale, flip, rotation, and shear between images were eliminated based on the geometrical information, and the initial co-registration polynomial was obtained. Then the registration points were automatically detected by integrating the signal-to-clutter-ratio (SCR) thresholds and the amplitude information, and a further co-registration process was performed to refine the polynomial. Several comparison experiments were carried out using 2 TerraSAR-X data from the Hong Kong airport and 21 PALSAR data from the Donghai Bridge. Experiment results demonstrate that the proposed method brings accuracy and efficiency improvements for co-registration and processing abilities in the cases of big distortion between images or large incoherent areas in the images. For most co-registrations, the proposed method can enhance the reliability and applicability of co-registration and thus promote the automation to a higher level.
[Japanese epidemiologic investigation for non-steroidal anti-inflammatory drugs-induced ulcers].
Miyake, Kazumasa; Sakamoto, Choitsu
2011-06-01
This review summaried epidemiologic investigation for non-steroidal anti-inflammatory drugs (NSAIDs)-induced ulcers to focus on the Japanese evidence. In Japan, national health insurance does not cover procedures that prevent or lower the risk for NSAIDs-induced ulcer. In NSAIDs treatment to patients with risk factors, it is desirable to administer antiulcer agents. However, in Japan, there are no large-scale studies on the efficacy of co-medication such as proton pump inhibitors, prostaglandin analogs (misoprostol) or histamine-H2 receptor antagonists or on the effectiveness of H. pylori eradication or selective COX-2 antagonists. In the future, large-scale clinical studies should be conducted to accumulate high quality evidence including cost-effectiveness and overall safety including cardiovascular events, because Japanese differ from Westerners in several genetical or acquired factors.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Raduha, S.; Butler, D.; Mozley, P. S.
Here, we examined the potential impact on CO 2 transport of zones of deformation bands in reservoir rock that transition to opening-mode fractures within overlying caprock. Sedimentological and petrophysical measurements were collected along an approximately 5 m × 5 m outcrop of the Slick Rock and Earthy Members of the Entrada Sandstone on the eastern flank of the San Rafael Swell, Utah, USA. Measured deformation band permeability (2 mD) within the reservoir facies is about three orders of magnitude lower than the host sandstone. Average permeability of the caprock facies (0.0005 mD) is about seven orders of magnitude lower thanmore » the host sandstone. Aperture-based permeability estimates of the opening-mode caprock fractures are high (3.3 × 10 7 mD). High-resolution CO 2–H 2O transport models incorporate these permeability data at the millimeter scale. We then varied fault properties at the reservoir/caprock interface between open fractures and deformation bands as part of a sensitivity study. Numerical modeling results suggest that zones of deformation bands within the reservoir strongly compartmentalize reservoir pressures largely blocking lateral, cross-fault flow of supercritical CO 2. Significant vertical CO 2 transport into the caprock occurred in some scenarios along opening-mode fractures. The magnitude of this vertical CO 2 transport depends on the small-scale geometry of the contact between the opening-mode fracture and the zone of deformation bands, as well as the degree to which fractures penetrate caprock. Finally, the presence of relatively permeable units within the caprock allows storage of significant volumes of CO 2, particularly when the fracture network does not extend all the way through the caprock.« less
Raduha, S.; Butler, D.; Mozley, P. S.; ...
2016-06-18
Here, we examined the potential impact on CO 2 transport of zones of deformation bands in reservoir rock that transition to opening-mode fractures within overlying caprock. Sedimentological and petrophysical measurements were collected along an approximately 5 m × 5 m outcrop of the Slick Rock and Earthy Members of the Entrada Sandstone on the eastern flank of the San Rafael Swell, Utah, USA. Measured deformation band permeability (2 mD) within the reservoir facies is about three orders of magnitude lower than the host sandstone. Average permeability of the caprock facies (0.0005 mD) is about seven orders of magnitude lower thanmore » the host sandstone. Aperture-based permeability estimates of the opening-mode caprock fractures are high (3.3 × 10 7 mD). High-resolution CO 2–H 2O transport models incorporate these permeability data at the millimeter scale. We then varied fault properties at the reservoir/caprock interface between open fractures and deformation bands as part of a sensitivity study. Numerical modeling results suggest that zones of deformation bands within the reservoir strongly compartmentalize reservoir pressures largely blocking lateral, cross-fault flow of supercritical CO 2. Significant vertical CO 2 transport into the caprock occurred in some scenarios along opening-mode fractures. The magnitude of this vertical CO 2 transport depends on the small-scale geometry of the contact between the opening-mode fracture and the zone of deformation bands, as well as the degree to which fractures penetrate caprock. Finally, the presence of relatively permeable units within the caprock allows storage of significant volumes of CO 2, particularly when the fracture network does not extend all the way through the caprock.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Voltolini, Marco; Kwon, Tae-Hyuk; Ajo-Franklin, Jonathan
Pore-scale distribution of supercritical CO 2 (scCO 2) exerts significant control on a variety of key hydrologic as well as geochemical processes, including residual trapping and dissolution. Despite such importance, only a small number of experiments have directly characterized the three-dimensional distribution of scCO 2 in geologic materials during the invasion (drainage) process. Here, we present a study which couples dynamic high-resolution synchrotron X-ray micro-computed tomography imaging of a scCO 2/brine system at in situ pressure/temperature conditions with quantitative pore-scale modeling to allow direct validation of a pore-scale description of scCO2 distribution. The experiment combines high-speed synchrotron radiography with tomographymore » to characterize the brine saturated sample, the scCO 2 breakthrough process, and the partially saturated state of a sandstone sample from the Domengine Formation, a regionally extensive unit within the Sacramento Basin (California, USA). The availability of a 3D dataset allowed us to examine correlations between grains and pores morphometric parameters and the actual distribution of scCO 2 in the sample, including the examination of the role of small-scale sedimentary structure on CO2 distribution. The segmented scCO 2/brine volume was also used to validate a simple computational model based on the local thickness concept, able to accurately simulate the distribution of scCO 2 after drainage. The same method was also used to simulate Hg capillary pressure curves with satisfactory results when compared to the measured ones. Finally, this predictive approach, requiring only a tomographic scan of the dry sample, proved to be an effective route for studying processes related to CO 2 invasion structure in geological samples at the pore scale.« less
Voltolini, Marco; Kwon, Tae-Hyuk; Ajo-Franklin, Jonathan
2017-10-21
Pore-scale distribution of supercritical CO 2 (scCO 2) exerts significant control on a variety of key hydrologic as well as geochemical processes, including residual trapping and dissolution. Despite such importance, only a small number of experiments have directly characterized the three-dimensional distribution of scCO 2 in geologic materials during the invasion (drainage) process. Here, we present a study which couples dynamic high-resolution synchrotron X-ray micro-computed tomography imaging of a scCO 2/brine system at in situ pressure/temperature conditions with quantitative pore-scale modeling to allow direct validation of a pore-scale description of scCO2 distribution. The experiment combines high-speed synchrotron radiography with tomographymore » to characterize the brine saturated sample, the scCO 2 breakthrough process, and the partially saturated state of a sandstone sample from the Domengine Formation, a regionally extensive unit within the Sacramento Basin (California, USA). The availability of a 3D dataset allowed us to examine correlations between grains and pores morphometric parameters and the actual distribution of scCO 2 in the sample, including the examination of the role of small-scale sedimentary structure on CO2 distribution. The segmented scCO 2/brine volume was also used to validate a simple computational model based on the local thickness concept, able to accurately simulate the distribution of scCO 2 after drainage. The same method was also used to simulate Hg capillary pressure curves with satisfactory results when compared to the measured ones. Finally, this predictive approach, requiring only a tomographic scan of the dry sample, proved to be an effective route for studying processes related to CO 2 invasion structure in geological samples at the pore scale.« less
Pore scale study of multiphase multicomponent reactive transport during CO 2 dissolution trapping
DOE Office of Scientific and Technical Information (OSTI.GOV)
Chen, Li; Wang, Mengyi; Kang, Qinjun
Solubility trapping is crucial for permanent CO 2 sequestration in deep saline aquifers. For the first time, a pore-scale numerical method is developed to investigate coupled scCO 2-water two-phase flow, multicomponent (CO 2(aq), H +, HCO 3 –, CO 3 2 – and OH –) mass transport, heterogeneous interfacial dissolution reaction, and homogeneous dissociation reactions. Pore-scale details of evolutions of multiphase distributions and concentration fields are presented and discussed. Time evolutions of several variables including averaged CO 2(aq) concentration, scCO 2 saturation, and pH value are analyzed. Specific interfacial length, an important variable which cannot be determined but is requiredmore » by continuum models, is investigated in detail. Mass transport coefficient or efficient dissolution rate is also evaluated. The pore-scale results show strong non-equilibrium characteristics during solubility trapping due to non-uniform distributions of multiphase as well as slow mass transport process. Complicated coupling mechanisms between multiphase flow, mass transport and chemical reactions are also revealed. Lastly, effects of wettability are also studied. The pore-scale studies provide deep understanding of non-linear non-equilibrium multiple physicochemical processes during CO 2 solubility trapping processes, and also allow to quantitatively predict some important empirical relationships, such as saturation-interfacial surface area, for continuum models.« less
Pore scale study of multiphase multicomponent reactive transport during CO 2 dissolution trapping
Chen, Li; Wang, Mengyi; Kang, Qinjun; ...
2018-04-26
Solubility trapping is crucial for permanent CO 2 sequestration in deep saline aquifers. For the first time, a pore-scale numerical method is developed to investigate coupled scCO 2-water two-phase flow, multicomponent (CO 2(aq), H +, HCO 3 –, CO 3 2 – and OH –) mass transport, heterogeneous interfacial dissolution reaction, and homogeneous dissociation reactions. Pore-scale details of evolutions of multiphase distributions and concentration fields are presented and discussed. Time evolutions of several variables including averaged CO 2(aq) concentration, scCO 2 saturation, and pH value are analyzed. Specific interfacial length, an important variable which cannot be determined but is requiredmore » by continuum models, is investigated in detail. Mass transport coefficient or efficient dissolution rate is also evaluated. The pore-scale results show strong non-equilibrium characteristics during solubility trapping due to non-uniform distributions of multiphase as well as slow mass transport process. Complicated coupling mechanisms between multiphase flow, mass transport and chemical reactions are also revealed. Lastly, effects of wettability are also studied. The pore-scale studies provide deep understanding of non-linear non-equilibrium multiple physicochemical processes during CO 2 solubility trapping processes, and also allow to quantitatively predict some important empirical relationships, such as saturation-interfacial surface area, for continuum models.« less
Geospatial analysis of near-term potential for carbon-negative bioenergy in the United States
Baik, Ejeong; Turner, Peter A.; Mach, Katharine J.; Field, Christopher B.; Benson, Sally M.
2018-01-01
Bioenergy with carbon capture and storage (BECCS) is a negative-emissions technology that may play a crucial role in climate change mitigation. BECCS relies on the capture and sequestration of carbon dioxide (CO2) following bioenergy production to remove and reliably sequester atmospheric CO2. Previous BECCS deployment assessments have largely overlooked the potential lack of spatial colocation of suitable storage basins and biomass availability, in the absence of long-distance biomass and CO2 transport. These conditions could constrain the near-term technical deployment potential of BECCS due to social and economic barriers that exist for biomass and CO2 transport. This study leverages biomass production data and site-specific injection and storage capacity estimates at high spatial resolution to assess the near-term deployment opportunities for BECCS in the United States. If the total biomass resource available in the United States was mobilized for BECCS, an estimated 370 Mt CO2⋅y−1 of negative emissions could be supplied in 2020. However, the absence of long-distance biomass and CO2 transport, as well as limitations imposed by unsuitable regional storage and injection capacities, collectively decrease the technical potential of negative emissions to 100 Mt CO2⋅y−1. Meeting this technical potential may require large-scale deployment of BECCS technology in more than 1,000 counties, as well as widespread deployment of dedicated energy crops. Specifically, the Illinois basin, Gulf region, and western North Dakota have the greatest potential for near-term BECCS deployment. High-resolution spatial assessment as conducted in this study can inform near-term opportunities that minimize social and economic barriers to BECCS deployment. PMID:29531081
Implications of 'Peak Oil' for Atmospheric CO2 and Climate
NASA Astrophysics Data System (ADS)
Kharecha, P. A.; Hansen, J. E.
2008-12-01
Unconstrained CO2 emission from fossil fuel burning has been the dominant cause of observed anthropogenic global warming. The amounts of "proven" and potential fossil fuel reserves are uncertain and debated. Regardless of the true values, society has flexibility in the degree to which it chooses to exploit these reserves, especially unconventional fossil fuels and those located in extreme or pristine environments. If conventional oil production peaks within the next few decades, it may have a large effect on future atmospheric CO2 and climate change, depending upon subsequent energy choices. Assuming that proven oil and gas reserves do not greatly exceed estimates of the Energy Information Administration -- and recent trends are toward lower estimates -- we show that it is feasible to keep atmospheric CO2 from exceeding about 450 ppm by 2100, provided that emissions from coal, unconventional fossil fuels, and land use are constrained. Coal-fired facilities without sequestration must be phased out before midcentury to achieve this CO2 limit. It is also important to "stretch" conventional oil reserves via energy conservation and efficiency, thus averting strong pressures to extract liquid fuels from coal or unconventional fossil fuels while clean technologies are being developed for the era "beyond fossil fuels". We argue that a rising price on carbon emissions is needed to discourage conversion of the vast fossil resources into usable reserves, and to keep CO2 below 450 ppm. It is also plausible that CO2 can be returned below 350 ppm by 2100 or sooner, if more aggressive mitigation measures are enacted, most notably a phase-out of global coal emissions by circa 2030 and large- scale reforestation, primarily in the tropics but also in temperate regions.
NASA Astrophysics Data System (ADS)
Gurney, K. R.; Chandrasekaran, V.; Mendoza, D. L.; Geethakumar, S.
2010-12-01
The Vulcan Project has estimated United States fossil fuel CO2 emissions at the hourly time scale and at spatial scales below the county level for the year 2002. Vulcan is built from a wide variety of observational data streams including regulated air pollutant emissions reporting, traffic monitoring, energy statistics, and US census data. In addition to these data sets, Vulcan relies on a series of modeling assumptions and constructs to interpolate in space, time and transform non-CO2 reporting into an estimate of CO2 combustion emissions. The recent version 2.0 of the Vulcan inventory has produced advances in a number of categories with particular emphasis on improved temporal structure. Onroad transportation emissions now avail of roughly 5000 automated traffic count monitors allowing for much improved diurnal and weekly time structure in our onroad transportation emissions. Though the inventory shows excellent agreement with independent national-level CO2 emissions estimates, uncertainty quantification has been a challenging task given the large number of data sources and numerous modeling assumptions. However, we have now accomplished a complete uncertainty estimate across all the Vulcan economic sectors and will present uncertainty estimates as a function of space, time, sector and fuel. We find that, like the underlying distribution of CO2 emissions themselves, the uncertainty is also strongly lognormal with high uncertainty associated with a relatively small number of locations. These locations typically are locations reliant upon coal combustion as the dominant CO2 source. We will also compare and contrast Vulcan fossil fuel CO2 emissions estimates against estimates built from DOE fuel-based surveys at the state level. We conclude that much of the difference between the Vulcan inventory and DOE statistics are not due to biased estimation but mechanistic differences in supply versus demand and combustion in space/time.
Downscaling the NOAA CarbonTracker Inversion for North America
NASA Astrophysics Data System (ADS)
Petron, G.; Andrews, A. E.; Chen, H.; Trudeau, M. E.; Eluszkiewicz, J.; Nehrkorn, T.; Henderson, J.; Sweeney, C.; Karion, A.; Masarie, K.; Bruhwiler, L.; Miller, J. B.; Miller, B. R.; Peters, W.; Gourdji, S. M.; Mueller, K. L.; Michalak, A. M.; Tans, P. P.
2011-12-01
We are developing a regional extension of the NOAA CarbonTracker CO2 data-assimilation system for a limited domain covering North America. The regional assimilation will use pre-computed and species-independent atmospheric sampling footprints from a Lagrangian Particle Dispersion Model. Each footprint relates an observed trace gas concentration to upwind fluxes. Once a footprint library has been computed, it can be used repeatedly to quickly test different inversion strategies and, importantly, for inversions using multiple species data (e.g., anthropogenic tracers such as radiocarbon and carbon monoxide and biological tracers such as carbonyl sulfide and stable isotopes of CO2). The current global CarbonTracker (CT) assimilation framework has some important limitations. For example, the assimilation adjusts scaling factors for different vegetation classes within large regions. This means, for example, that all crops within temperate North America are scaled together. There is currently no distinction between crops such as corn and sorghum, which utilize the C4 photosynthesis pathway and C3 crops like soybeans, wheat, cotton, etc. The optimization scales only the net CO2 flux, rather than adjusting photosynthesis and respiration fluxes separately, which limits the flexibility of the inversion and sometimes results in unrealistic diurnal cycles of CO2 flux. The time-series of residuals (CT - observed) for continental sites in North America reveals a persistent excess of CO2 during summer. This summertime positive bias is also apparent in the comparison of CT posterior CO2 with aircraft data and with data from Pacific marine boundary layer sites, suggesting that some of the problem may originate outside of North America. For the regional inversion, we will use footprints from the Stochastic Time-Inverted Lagrangian Transport Model driven by meteorological fields from a customized high-resolution simulation with the Weather Research Forecast (WRF) model. We will use empirically corrected boundary conditions in order to minimize sensitivity to inaccurate fluxes or transport outside of our domain. We plan to test a variety of inversion strategies that effectively exploit CO2 and isotopic data from the relatively dense North American sampling network for 2007-2010.
Prevented mortality and greenhouse gas emissions from historical and projected nuclear power.
Kharecha, Pushker A; Hansen, James E
2013-05-07
In the aftermath of the March 2011 accident at Japan's Fukushima Daiichi nuclear power plant, the future contribution of nuclear power to the global energy supply has become somewhat uncertain. Because nuclear power is an abundant, low-carbon source of base-load power, it could make a large contribution to mitigation of global climate change and air pollution. Using historical production data, we calculate that global nuclear power has prevented an average of 1.84 million air pollution-related deaths and 64 gigatonnes of CO2-equivalent (GtCO2-eq) greenhouse gas (GHG) emissions that would have resulted from fossil fuel burning. On the basis of global projection data that take into account the effects of the Fukushima accident, we find that nuclear power could additionally prevent an average of 420,000-7.04 million deaths and 80-240 GtCO2-eq emissions due to fossil fuels by midcentury, depending on which fuel it replaces. By contrast, we assess that large-scale expansion of unconstrained natural gas use would not mitigate the climate problem and would cause far more deaths than expansion of nuclear power.
Prevented Mortality and Greenhouse Gas Emissions From Historical and Projected Nuclear Power
NASA Technical Reports Server (NTRS)
Kharecha, Pushker A.; Hansen, James E.
2013-01-01
In the aftermath of the March 2011 accident at Japan's Fukushima Daiichi nuclear power plant, the future contribution of nuclear power to the global energy supply has become somewhat uncertain. Because nuclear power is an abundant, low-carbon source of base-load power, it could make a large contribution to mitigation of global climate change and air pollution. Using historical production data, we calculate that global nuclear power has prevented an average of 1.84 million air pollution-related deaths and 64 gigatonnes of CO2-equivalent (GtCO2-eq) greenhouse gas (GHG) emissions that would have resulted from fossil fuel burning. On the basis of global projection data that take into account the effects of the Fukushima accident, we find that nuclear power could additionally prevent an average of 420 000-7.04 million deaths and 80-240 GtCO2-eq emissions due to fossil fuels by midcentury, depending on which fuel it replaces. By contrast, we assess that large-scale expansion of unconstrained natural gas use would not mitigate the climate problem and would cause far more deaths than expansion of nuclear power.
Higher fungal diversity is correlated with lower CO2 emissions from dead wood in a natural forest.
Yang, Chunyan; Schaefer, Douglas A; Liu, Weijie; Popescu, Viorel D; Yang, Chenxue; Wang, Xiaoyang; Wu, Chunying; Yu, Douglas W
2016-08-24
Wood decomposition releases almost as much CO2 to the atmosphere as does fossil-fuel combustion, so the factors regulating wood decomposition can affect global carbon cycling. We used metabarcoding to estimate the fungal species diversities of naturally colonized decomposing wood in subtropical China and, for the first time, compared them to concurrent measures of CO2 emissions. Wood hosting more diverse fungal communities emitted less CO2, with Shannon diversity explaining 26 to 44% of emissions variation. Community analysis supports a 'pure diversity' effect of fungi on decomposition rates and thus suggests that interference competition is an underlying mechanism. Our findings extend the results of published experiments using low-diversity, laboratory-inoculated wood to a high-diversity, natural system. We hypothesize that high levels of saprotrophic fungal biodiversity could be providing globally important ecosystem services by maintaining dead-wood habitats and by slowing the atmospheric contribution of CO2 from the world's stock of decomposing wood. However, large-scale surveys and controlled experimental tests in natural settings will be needed to test this hypothesis.
Higher fungal diversity is correlated with lower CO2 emissions from dead wood in a natural forest
Yang, Chunyan; Schaefer, Douglas A.; Liu, Weijie; Popescu, Viorel D.; Yang, Chenxue; Wang, Xiaoyang; Wu, Chunying; Yu, Douglas W.
2016-01-01
Wood decomposition releases almost as much CO2 to the atmosphere as does fossil-fuel combustion, so the factors regulating wood decomposition can affect global carbon cycling. We used metabarcoding to estimate the fungal species diversities of naturally colonized decomposing wood in subtropical China and, for the first time, compared them to concurrent measures of CO2 emissions. Wood hosting more diverse fungal communities emitted less CO2, with Shannon diversity explaining 26 to 44% of emissions variation. Community analysis supports a ‘pure diversity’ effect of fungi on decomposition rates and thus suggests that interference competition is an underlying mechanism. Our findings extend the results of published experiments using low-diversity, laboratory-inoculated wood to a high-diversity, natural system. We hypothesize that high levels of saprotrophic fungal biodiversity could be providing globally important ecosystem services by maintaining dead-wood habitats and by slowing the atmospheric contribution of CO2 from the world’s stock of decomposing wood. However, large-scale surveys and controlled experimental tests in natural settings will be needed to test this hypothesis. PMID:27553882
NASA Astrophysics Data System (ADS)
Xiao, Yuanhua; Zhang, Aiqin; Liu, Shaojun; Zhao, Jihong; Fang, Shaoming; Jia, Dianzeng; Li, Feng
2012-12-01
Free-standing and porous hierarchical nanoarchitectures constructed with cobalt cobaltite (Co3O4) nanowalls have been successfully synthesized in large scale by calcining three dimensional (3D) hierarchical nanostructures consisting of single crystalline cobalt carbonate hydroxide hydrate - Co(CO3)0.5(OH)·0.11H2O nanowalls prepared with a solvothermal method. The step-by-step decomposition of the precursor can generate porous Co3O4 nanowalls with BET surface area of 88.34 m2 g-1. The as-prepared Co3O4 nanoarchitectures show superior specific capacitance to the most Co3O4 supercapacitor electrode materials to date. After continuously cycled for 1000 times of charge-discharge at 4 A g-1, the supercapacitors can retain ca 92.3% of their original specific capacitances. The excellent performances of the devices can be attributed to the porous and hierarchical 3D nanostructure of the materials.
Small-scale structure of the CO emission in S255 from lunar occultation observations
NASA Technical Reports Server (NTRS)
Schloerb, F. P.; Scoville, N. Z.
1980-01-01
Two lunar occultations of the S255 H II region/molecular cloud complex were observed in the 2.6 mm CO line during 1978 and 1979. The resolution obtained (between 4 arcsec and 7 arcsec) enables us to resolve bright sources that are much smaller than the 44 arcsec telescope beam. In addition to the large-scale structure (approximately 10 arcmin in size) seen in previous CO maps, the observations reveal two high-temperature emission regions in the cloud core associated with two compact infrared sources about 20 arcsec apart. The first CO hot spot is larger in size with a Gaussian width of 41 arcsec + or - 7 arcsec and a peak temperature of 65 K. Its center falls between the two small infrared sources S255 IRS1 and IRS2. The linear size and peak temperature of this source are remarkably similar to those in the Orion Kleinmann-Low nebula. The second source is revealed from a discontinuous change in the CO line flux as the lunar limb crossed S255 IRS1. The size of this component is less than 7 arcsec; its temperature must exceed 200 K. No evidence is found for exceptionally high temperatures at the boundary of the two H II regions crossed during the occultations.
LARGE-SCALE CO MAPS OF THE LUPUS MOLECULAR CLOUD COMPLEX
DOE Office of Scientific and Technical Information (OSTI.GOV)
Tothill, N. F. H.; Loehr, A.; Stark, A. A.
2009-11-01
Fully sampled degree-scale maps of the {sup 13}CO 2-1 and CO 4-3 transitions toward three members of the Lupus Molecular Cloud Complex-Lupus I, III, and IV-trace the column density and temperature of the molecular gas. Comparison with IR extinction maps from the c2d project requires most of the gas to have a temperature of 8-10 K. Estimates of the cloud mass from {sup 13}CO emission are roughly consistent with most previous estimates, while the line widths are higher, around 2 km s{sup -1}. CO 4-3 emission is found throughout Lupus I, indicating widespread dense gas, and toward Lupus III andmore » IV. Enhanced line widths at the NW end and along the edge of the B 228 ridge in Lupus I, and a coherent velocity gradient across the ridge, are consistent with interaction between the molecular cloud and an expanding H I shell from the Upper-Scorpius subgroup of the Sco-Cen OB Association. Lupus III is dominated by the effects of two HAe/Be stars, and shows no sign of external influence. Slightly warmer gas around the core of Lupus IV and a low line width suggest heating by the Upper-Centaurus-Lupus subgroup of Sco-Cen, without the effects of an H I shell.« less
Sharbatian, Atena; Abedini, Ali; Qi, ZhenBang; Sinton, David
2018-02-20
Carbon capture, storage, and utilization technologies target a reduction in net CO 2 emissions to mitigate greenhouse gas effects. The largest such projects worldwide involve storing CO 2 through enhanced oil recovery-a technologically and economically feasible approach that combines both storage and oil recovery. Successful implementation relies on detailed measurements of CO 2 -oil properties at relevant reservoir conditions (P = 2.0-13.0 MPa and T = 23 and 50 °C). In this paper, we demonstrate a microfluidic method to quantify the comprehensive suite of mutual properties of a CO 2 and crude oil mixture including solubility, diffusivity, extraction pressure, minimum miscibility pressure (MMP), and contact angle. The time-lapse oil swelling/extraction in response to CO 2 exposure under stepwise increasing pressure was quantified via fluorescence microscopy, using the inherent fluorescence property of the oil. The CO 2 solubilities and diffusion coefficients were determined from the swelling process with measurements in strong agreement with previous results. The CO 2 -oil MMP was determined from the subsequent oil extraction process with measurements within 5% of previous values. In addition, the oil-CO 2 -silicon contact angle was measured throughout the process, with contact angle increasing with pressure. In contrast with conventional methods, which require days and ∼500 mL of fluid sample, the approach here provides a comprehensive suite of measurements, 100-fold faster with less than 1 μL of sample, and an opportunity to better inform large-scale CO 2 projects.
NASA Astrophysics Data System (ADS)
Katul, Gabriel G.; Oren, Ram; Manzoni, Stefano; Higgins, Chad; Parlange, Marc B.
2012-09-01
The role of evapotranspiration (ET) in the global, continental, regional, and local water cycles is reviewed. Elevated atmospheric CO2, air temperature, vapor pressure deficit (D), turbulent transport, radiative transfer, and reduced soil moisture all impact biotic and abiotic processes controlling ET that must be extrapolated to large scales. Suggesting a blueprint to achieve this link is the main compass of this review. Leaf-scale transpiration (fe) as governed by the plant biochemical demand for CO2 is first considered. When this biochemical demand is combined with mass transfer formulations, the problem remains mathematically intractable, requiring additional assumptions. A mathematical "closure" that assumes stomatal aperture is autonomously regulated so as to maximize the leaf carbon gain while minimizing water loss is proposed, which leads to analytical expressions for leaf-scale transpiration. This formulation predicts well the effects of elevated atmospheric CO2 and increases in D on fe. The case of soil moisture stress is then considered using extensive gas exchange measurements collected in drought studies. Upscaling the fe to the canopy is then discussed at multiple time scales. The impact of limited soil water availability within the rooting zone on the upscaled ET as well as some plant strategies to cope with prolonged soil moisture stress are briefly presented. Moving further up in direction and scale, the soil-plant system is then embedded within the atmospheric boundary layer, where the influence of soil moisture on rainfall is outlined. The review concludes by discussing outstanding challenges and how to tackle them by means of novel theoretical, numerical, and experimental approaches.
NASA Astrophysics Data System (ADS)
Du, Q.; Liu, H.; Liu, Y.; Wang, L.; Xu, L.
2017-12-01
Erhai lake is located in the southeastern margin of Tibetan Plateau. Based on the 4 years measurement over Erhai lake with eddy covariance technique (EC) from 2012 to 2015, the diurnal and seasonal variations of latent and sensible heat and CO2 fluxes, and their controlling factors over different time scales were analyzed. The diurnal average LE ranged from 31 to 171 Wm-2, while Hs ranged from -31 to 21 Wm-2. Bowen ratio was larger during January and May and smaller during June and October. The lake continued storing heat during January and June, and releasing heat since July. The diurnal average CO2 fluxes during nighttime were higher than the daytime, and carbon uptake was almost observed during the midday time of the day for the whole study period. The annual carbon budget fluctuated from 117.5 to 161.7 g C m-2 a-1, while annual total evaporation (ET) from 1120.8 to 1228.5 mm for the four-years period. The Erhai Lake behaved as a net carbon source over the whole period but carbon uptake was observed during the middle time of each year. The difference between water surface and air temperature (DeltaT) and the product of DeltaT and wind speed were the main controlling factors for Hs from halfhourly to monthly scale. There was significant relationship between wind speed, the product of wind speed and vapor pressure deficit (VPD) and LE on halfhourly and daily scales. The total cloud amount and net radiation (Rn) had a large effect on monthly variation of LE. Photosynthetic active radiation (PAR) and wind speed was mainly responsible for the variation of halfhourly and daily CO2 fluxes, respectively. The total cloud amount was the most important factors controlling for annual total ET. The annual rainfall, water surface temperature was observed to be negatively related with annual CO2 fluxes.
Novel Inorganic/Polymer Composite Membranes for CO 2 Capture
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ho, W.S. Winston; Dutta, Prabir K.; Schmit, Steve J.
The objective of this project is to develop a cost-effective design and manufacturing process for new membrane modules that capture CO 2 from flue gas in coal-fired power plants. The membrane consisted of a thin selective layer including inorganic (zeolite) embedded in a polymer structure so that it can be made in a continuous manufacturing process. The membrane was incorporated in spiral-wound modules for the field test with actual flue gas at the National Carbon Capture Center (NCCC) in Wilsonville, AL and bench scale tests with simulated flue gas at the Ohio State University (OSU). Using the modules for post-combustionmore » CO 2 capture is expected to achieve the DOE target of $40/tonne CO 2 captured (in 2007 dollar) for 2025. Membranes with the amine-containing polymer cover layer on zeolite-Y (ZY) nanoparticles deposited on the polyethersulfone (PES) substrate were successfully synthesized. The membranes showed a high CO 2 permeance of about 1100 GPU (gas permeation unit, 1 GPU = 10 -6 cm 3 (STP)/(cm 2 • s • cm Hg), 3000 GPU = 10-6 mol/(m 2 • s • Pa)) with a high CO 2/N 2 selectivity of > 200 at the typical flue gas conditions at 57°C (about 17% water vapor in feed gas) and > 1400 GPU CO 2 permeance with > 500 CO 2/N 2 selectivity at 102°C (~ 80% water vapor). The synthesis of ZY nanoparticles was successfully scaled up, and the pilot-scale membranes were also successfully fabricated using the continuous membrane machine at OSU. The transport performance of the pilot-scale membranes agreed reasonably well with the lab-scale membranes. The results from both the lab-scale and scale-up membranes were used for the techno-economic analysis. The scale-up membranes were fabricated into prototype spiral-wound membrane modules for continuous testing with simulated or real flue gas. For real flue gas testing, we worked with NCCC, in consultation with TriSep Corporation, Gradient Technology and American Electric Power (AEP). The membrane module demonstrated > 800 GPU of CO 2 permeance and > 150 CO 2/N 2 selectivity when tested with real flue gas at NCCC. The results obtained were used to update the techno-economic analysis. In addition, the EH&S assessment of the membranes for post-combustion CO 2 capture was conducted.« less
Rodosta, T.; Litynski, J.; Plasynski, S.; Spangler, L.; Finley, R.; Steadman, E.; Ball, D.; Gerald, H.; McPherson, B.; Burton, E.; Vikara, D.
2011-01-01
The U.S. Department of Energy (DOE) is the lead federal agency for the development and deployment of carbon sequestration technologies. The Regional Carbon Sequestration Partnerships (RCSPs) are the mechanism DOE utilizes to prove the technology and to develop human capital, stakeholder networks, information for regulatory policy, best practices documents and training to work toward the commercialization of carbon capture and storage (CCS). The RCSPs are tasked with determining the most suitable technologies, regulations, and infrastructure for carbon capture, transport, and storage in their respective geographic areas of responsibility. The seven partnerships include more than 400 state agencies, universities, national laboratories, private companies, and environmental organizations, spanning 43 states and four Canadian provinces. The Regional Partnerships Initiative is being implemented in three phases: Characterization, Validation, and Development. The initial Characterization Phase began in 2003 and was completed in 2005 and focused on characterization of CO2 storage potential within each region. It was followed by the Validation Phase, which began in 2005 and is nearing completion in 2011. The focus of the Validation Phase has been on small-scale field tests throughout the seven partnerships in various formation types such as saline, oil-bearing, and coal seams. The Validation Phase has characterized suitable CO2 storage reservoirs and identified the need for comprehensive legal and regulatory frameworks to enable commercial-scale CCS deployment. Finally, the Development Phase will consist of a series of large-scale, one-million-ton, injection tests throughout the United States and Canada. The objective of these large-scale tests is to identify the regulatory path or challenges in permitting CCS projects, to demonstrate the technology can inject CO2 safely, and to verify its permanence in geologic formations in preparation for the commercialization of geologic sequestration. ?? 2010 Elsevier Ltd. All rights reserved. ?? 2011 Published by Elsevier Ltd.
Unraveling the dynamics of magmatic CO2 degassing at Mammoth Mountain, California
NASA Astrophysics Data System (ADS)
Peiffer, Loïc; Wanner, Christoph; Lewicki, Jennifer L.
2018-02-01
The accumulation of magmatic CO2 beneath low-permeability barriers may lead to the formation of CO2-rich gas reservoirs within volcanic systems. Such accumulation is often evidenced by high surface CO2 emissions that fluctuate over time. The temporal variability in surface degassing is believed in part to reflect a complex interplay between deep magmatic degassing and the permeability of degassing pathways. A better understanding of the dynamics of CO2 degassing is required to improve monitoring and hazards mitigation in these systems. Owing to the availability of long-term records of CO2 emissions rates and seismicity, Mammoth Mountain in California constitutes an ideal site towards such predictive understanding. Mammoth Mountain is characterized by intense soil CO2 degassing (up to ∼1000 t d-1) and tree kill areas that resulted from leakage of CO2 from a CO2-rich gas reservoir located in the upper ∼4 km. The release of CO2-rich fluids from deeper basaltic intrusions towards the reservoir induces seismicity and potentially reactivates faults connecting the reservoir to the surface. While this conceptual model is well-accepted, there is still a debate whether temporally variable surface CO2 fluxes directly reflect degassing of intrusions or variations in fault permeability. Here, we report the first large-scale numerical model of fluid and heat transport for Mammoth Mountain. We discuss processes (i) leading to the initial formation of the CO2-rich gas reservoir prior to the occurrence of high surface CO2 degassing rates and (ii) controlling current CO2 degassing at the surface. Although the modeling settings are site-specific, the key mechanisms discussed in this study are likely at play at other volcanic systems hosting CO2-rich gas reservoirs. In particular, our model results illustrate the role of convection in stripping a CO2-rich gas phase from a rising hydrothermal fluid and leading to an accumulation of a large mass of CO2 (∼107-108 t) in a shallow gas reservoir. Moreover, we show that both, short-lived (months to years) and long-lived (hundreds of years) events of magmatic fluid injection can lead to critical pressures within the reservoir and potentially trigger fault reactivation. Our sensitivity analysis suggests that observed temporal fluctuations in surface degassing are only indirectly controlled by variations in magmatic degassing and are mainly the result of temporally variable fault permeability. Finally, we suggest that long-term CO2 emission monitoring, seismic tomography and coupled thermal-hydraulic-mechanical modeling are important for CO2-related hazard mitigation.
NASA Astrophysics Data System (ADS)
Winkler, A. J.; Brovkin, V.; Myneni, R.; Alexandrov, G.
2017-12-01
Plant growth in the northern high latitudes benefits from increasing temperature (radiative effect) and CO2 fertilization as a consequence of rising atmospheric CO2 concentration. This enhanced gross primary production (GPP) is evident in large scale increase in summer time greening over the 36-year record of satellite observations. In this time period also various global ecosystem models simulate a greening trend in terms of increasing leaf area index (LAI). We also found a persistent greening trend analyzing historical simulations of Earth system models (ESM) participating in Phase 5 of the Coupled Model Intercomparison Project (CMIP5). However, these models span a large range in strength of the LAI trend, expressed as sensitivity to both key environmental factors, temperature and CO2 concentration. There is also a wide spread in magnitude of the associated increase of terrestrial GPP among the ESMs, which contributes to pronounced uncertainties in projections of future climate change. Here we demonstrate that there is a linear relationship across the CMIP5 model ensemble between projected GPP changes and historical LAI sensitivity, which allows using the observed LAI sensitivity as an "emerging constraint" on GPP estimation at future CO2 concentration. This constrained estimate of future GPP is substantially higher than the traditional multi-model mean suggesting that the majority of current ESMs may be significantly underestimating carbon fixation by vegetation in NHL. We provide three independent lines of evidence in analyzing observed and simulated CO2 amplitude as well as atmospheric CO2 inversion products to arrive at the same conclusion.
NASA Astrophysics Data System (ADS)
Hatala, Jaclyn Anne
The Sacramento-San Joaquin Delta in California was drained for agriculture and human settlement over a century ago, resulting in extreme rates of soil subsidence and release of CO2 to the atmosphere from peat oxidation. Because of this century-long ecosystem carbon imbalance where heterotrophic respiration exceeded net primary productivity, most of the land surface in the Delta is now up to 8 meters below sea level. To potentially reverse this trend of chronic carbon loss from Delta ecosystems, land managers have begun converting drained lands back to flooded ecosystems, but at the cost of increased production of CH4, a much more potent greenhouse gas than CO2. To evaluate the impacts of inundation on the biosphere-atmophere exchange of CO2 and CH4 in the Delta, I first measured and analyzed net fluxes of CO2 and CH4 for two continuous years with the eddy covariance technique in a drained peatland pasture and a recently re-flooded rice paddy. This analysis demonstrated that the drained pasture was a consistent large source of CO2 and small source of CH 4, whereas the rice paddy was a mild sink for CO2 and a mild source of CH4. However more importantly, this first analysis revealed nuanced complexities for measuring and interpreting patterns in CO2 and CH4 fluxes through time and space. CO2 and CH4 fluxes are inextricably linked in flooded ecosystems, as plant carbon serves as the primary substrate for the production of CH4 and wetland plants also provide the primary transport pathway of CH4 flux to the atmosphere. At the spatially homogeneous rice paddy during the summer growing season, I investigated rapid temporal coupling between CO2 and CH4 fluxes. Through wavelet Granger-causality analysis, I demonstrated that daily fluctuations in growing season gross ecosystem productivity (photosynthesis) exert a stronger control than temperature on the diurnal pattern in CH4 flux from rice. At a spatially heterogeneous restored wetland site, I analyzed the spatial coupling between net CO2 and CH4 fluxes by characterizing two-dimensional patterns of emergent vegetation within eddy covariance flux footprints. I combined net CO2 and CH4 fluxes from three eddy flux towers with high-resolution remote sensing imagery classified for emergent vegetation and an analytical 2-D flux footprint model to assess the impact of vegetation fractal pattern and abundance on the measured flux. Both emergent vegetation abundance and fractal complexity are important metrics for constraining variability within CO2 and CH4 flux in this complex landscape. Scaling between carbon flux measurements at individual sites and regional scales depends on the connection to remote sensing metrics that can be broadly applied. In the final chapter of this dissertation, I analyzed a long term dataset of hyperspectral ground reflectance measurements collected within the flux tower footprints of three structurally similar yet functionally diverse ecosystems: an annual grassland, a degraded pepperweed pasture, and a rice paddy. The normalized difference vegetation index (NDVI) was highly correlated with landscape-scale photosynthesis across all sites, however this work also revealed new potential spectral indices with high correlation to both net and partitioned CO2 fluxes. This analysis within this dissertation serves as a framework for considering the impacts of temporal and spatial heterogeneity on measured landscape-scale fluxes of CO2 and CH4. Scaling measurements through time and space is especially critical for interpreting fluxes of trace gases with a high degree of temporal heterogeneity, like CH4 and N 2O, from landscapes that have a high degree of spatial heterogeneity, like wetlands. This work articulates a strong mechanistic connection between CO2 and CH4 fluxes in wetland ecosystems, and provides important management considerations for implementing and monitoring inundated land-use conversion as an effective carbon management strategy in the California Delta.
Continental-scale variation in controls of summer CO2 in United States lakes
NASA Astrophysics Data System (ADS)
Lapierre, Jean-Francois; Seekell, David A.; Filstrup, Christopher T.; Collins, Sarah M.; Emi Fergus, C.; Soranno, Patricia A.; Cheruvelil, Kendra S.
2017-04-01
Understanding the broad-scale response of lake CO2 dynamics to global change is challenging because the relative importance of different controls of surface water CO2 is not known across broad geographic extents. Using geostatistical analyses of 1080 lakes in the conterminous United States, we found that lake partial pressure of CO2 (pCO2) was controlled by different chemical and biological factors related to inputs and losses of CO2 along climate, topography, geomorphology, and land use gradients. Despite weak spatial patterns in pCO2 across the study extent, there were strong regional patterns in the pCO2 driver-response relationships, i.e., in pCO2 "regulation." Because relationships between lake CO2 and its predictors varied spatially, global models performed poorly in explaining the variability in CO2 for U.S. lakes. The geographically varying driver-response relationships of lake pCO2 reflected major landscape gradients across the study extent and pointed to the importance of regional-scale variation in pCO2 regulation. These results indicate a higher level of organization for these physically disconnected systems than previously thought and suggest that changes in climate and land use could induce shifts in the main pathways that determine the role of lakes as sources and sinks of atmospheric CO2.
Diurnal sampling reveals significant variation in CO2 emission from a tropical productive lake.
Reis, P C J; Barbosa, F A R
2014-08-01
It is well accepted in the literature that lakes are generally net heterotrophic and supersaturated with CO2 because they receive allochthonous carbon inputs. However, autotrophy and CO2 undersaturation may happen for at least part of the time, especially in productive lakes. Since diurnal scale is particularly important to tropical lakes dynamics, we evaluated diurnal changes in pCO2 and CO2 flux across the air-water interface in a tropical productive lake in southeastern Brazil (Lake Carioca) over two consecutive days. Both pCO2 and CO2 flux were significantly different between day (9:00 to 17:00) and night (21:00 to 5:00) confirming the importance of this scale for CO2 dynamics in tropical lakes. Net heterotrophy and CO2 outgassing from the lake were registered only at night, while significant CO2 emission did not happen during the day. Dissolved oxygen concentration and temperature trends over the diurnal cycle indicated the dependence of CO2 dynamics on lake metabolism (respiration and photosynthesis). This study indicates the importance of considering the diurnal scale when examining CO2 emissions from tropical lakes.
Carbon dioxide and the uneasy interactions of trees and savannah grasses
Bond, William J.; Midgley, Guy F.
2012-01-01
Savannahs are a mixture of trees and grasses often occurring as alternate states to closed forests. Savannah fires are frequent where grass productivity is high in the wet season. Fires help maintain grassy vegetation where the climate is suitable for woodlands or forests. Saplings in savannahs are particularly vulnerable to topkill of above-ground biomass. Larger trees are more fire-resistant and suffer little damage when burnt. Recruitment to large mature tree size classes depends on sapling growth rates to fire-resistant sizes and the time between fires. Carbon dioxide (CO2) can influence the growth rate of juvenile plants, thereby affecting tree recruitment and the conversion of open savannahs to woodlands. Trees have increased in many savannahs throughout the world, whereas some humid savannahs are being invaded by forests. CO2 has been implicated in this woody increase but attribution to global drivers has been controversial where changes in grazing and fire have also occurred. We report on diverse tests of the magnitude of CO2 effects on both ancient and modern ecosystems with a particular focus on African savannahs. Large increases in trees of mesic savannahs in the region cannot easily be explained by land use change but are consistent with experimental and simulation studies of CO2 effects. Changes in arid savannahs seem less obviously linked to CO2 effects and may be driven more by overgrazing. Large-scale shifts in the tree–grass balance in the past and the future need to be better understood. They not only have major impacts on the ecology of grassy ecosystems but also on Earth–atmosphere linkages and the global carbon cycle in ways that are still being discovered. PMID:22232770