Science.gov

Sample records for co2 chemical upgrading

  1. A review on optimization production and upgrading biogas through CO2 removal using various techniques.

    PubMed

    Andriani, Dian; Wresta, Arini; Atmaja, Tinton Dwi; Saepudin, Aep

    2014-02-01

    Biogas from anaerobic digestion of organic materials is a renewable energy resource that consists mainly of CH4 and CO2. Trace components that are often present in biogas are water vapor, hydrogen sulfide, siloxanes, hydrocarbons, ammonia, oxygen, carbon monoxide, and nitrogen. Considering the biogas is a clean and renewable form of energy that could well substitute the conventional source of energy (fossil fuels), the optimization of this type of energy becomes substantial. Various optimization techniques in biogas production process had been developed, including pretreatment, biotechnological approaches, co-digestion as well as the use of serial digester. For some application, the certain purity degree of biogas is needed. The presence of CO2 and other trace components in biogas could affect engine performance adversely. Reducing CO2 content will significantly upgrade the quality of biogas and enhancing the calorific value. Upgrading is generally performed in order to meet the standards for use as vehicle fuel or for injection in the natural gas grid. Different methods for biogas upgrading are used. They differ in functioning, the necessary quality conditions of the incoming gas, and the efficiency. Biogas can be purified from CO2 using pressure swing adsorption, membrane separation, physical or chemical CO2 absorption. This paper reviews the various techniques, which could be used to optimize the biogas production as well as to upgrade the biogas quality.

  2. Bioelectrochemical removal of carbon dioxide (CO2): an innovative method for biogas upgrading.

    PubMed

    Xu, Heng; Wang, Kaijun; Holmes, Dawn E

    2014-12-01

    Innovative methods for biogas upgrading based on biological/in-situ concepts have started to arouse considerable interest. Bioelectrochemical removal of CO2 for biogas upgrading was proposed here and demonstrated in both batch and continuous experiments. The in-situ biogas upgrading system seemed to perform better than the ex-situ one, but CO2 content was kept below 10% in both systems. The in-situ system's performance was further enhanced under continuous operation. Hydrogenotrophic methanogenesis and alkali production with CO2 absorption could be major contributors to biogas upgrading. Molecular studies showed that all the biocathodes associated with biogas upgrading were dominated by sequences most similar to the same hydrogenotrophic methanogen species, Methanobacterium petrolearium (97-99% sequence identity). Conclusively, bioelectrochemical removal of CO2 showed great potential for biogas upgrading.

  3. Remote sensing of chemical warfare agent by CO2 -lidar

    NASA Astrophysics Data System (ADS)

    Geiko, Pavel P.; Smirnov, Sergey S.

    2014-11-01

    The possibilities of remote sensing of chemical warfare agent by differential absorption method were analyzed. The CO2 - laser emission lines suitable for sounding of chemical warfare agent with provision for disturbing absorptions by water vapor were choose. The detection range of chemical warfare agents was estimated for a lidar based on CO2 - laser The other factors influencing upon echolocation range were analyzed.

  4. Metal-Organic Frameworks for CO2 Chemical Transformations.

    PubMed

    He, Hongming; Perman, Jason A; Zhu, Guangshan; Ma, Shengqian

    2016-12-01

    Carbon dioxide (CO2 ), as the primary greenhouse gas in the atmosphere, triggers a series of environmental and energy related problems in the world. Therefore, there is an urgent need to develop multiple methods to capture and convert CO2 into useful chemical products, which can significantly improve the environment and promote sustainable development. Over the past several decades, metal-organic frameworks (MOFs) have shown outstanding heterogeneous catalytic activity due in part to their high internal surface area and chemical functionalities. These properties and the ability to synthesize MOF platforms allow experiments to test structure-function relationships for transforming CO2 into useful chemicals. Herein, recent developments are highlighted for MOFs participating as catalysts for the chemical fixation and photochemical reduction of CO2 . Finally, opportunities and challenges facing MOF catalysts are discussed in this ongoing research area.

  5. CO2 solvation free energy using quasi-chemical theory

    NASA Astrophysics Data System (ADS)

    Jiao, Dian; Rempe, Susan B.

    2011-06-01

    Accumulation of greenhouse gases, especially carbon dioxide, is believed to be the key factor in global climate change. To develop effective ways to remove CO2 from the atmosphere, it is helpful to understand the mechanism of CO2 solvation first. Here we investigate the thermodynamics of CO2 hydration using quasi-chemical theory. Two approaches for estimating hydration free energy are carried out. Both agree reasonably well with experimental measurements. Analysis of the free energy components reveals that the weak hydration free energy results from a balance of unfavorable molecular packing and favorable chemical association.

  6. Evaporative CO2 microchannel cooling for the LHCb VELO pixel upgrade

    NASA Astrophysics Data System (ADS)

    de Aguiar Francisco, O. A.; Buytaert, J.; Collins, P.; Dumps, R.; John, M.; Mapelli, A.; Romagnoli, G.

    2015-05-01

    The LHCb Vertex Detector (VELO) will be upgraded in 2018 to a lightweight pixel detector capable of 40 MHz readout and operation in very close proximity to the LHC beams. The thermal management of the system will be provided by evaporative CO2 circulating in microchannels embedded within thin silicon plates. This solution has been selected due to the excellent thermal efficiency, the absence of thermal expansion mismatch with silicon ASICs and sensors, the radiation hardness of CO2, and very low contribution to the material budget. Although microchannel cooling is gaining considerable attention for applications related to microelectronics, it is still a novel technology for particle physics experiments, in particular when combined with evaporative CO2 cooling. The R&D effort for LHCb is focused on the design and layout of the channels together with a fluidic connector and its attachment which must withstand pressures up to 170 bar. Even distribution of the coolant is ensured by means of the use of restrictions implemented before the entrance to a race track like layout of the main cooling channels. The coolant flow and pressure drop have been simulated as well as the thermal performance of the device. This proceeding describes the design and optimization of the cooling system for LHCb and the latest prototyping results.

  7. Effective CO2 adsorption on pristine and chemically functionalized MWCNTs

    NASA Astrophysics Data System (ADS)

    Shukrullah, Shazia; Mohamed, Norani Muti; Shaharun, Maizatul Shima; Ullah, Sami; Naz, Muhammad Yasin

    2016-11-01

    Carbon dioxide is one of the major greenhouse gases, which directly links to global warming. In this study, the laboratory produced multi-walled carbon nanotubes (MWCNTs) were amine-functionalized and tested for their potential as a CO2 adsorbent material. The CVD grown MWCNTs were treated with H2SO4/HNO3 and functionalized with 30% of 3-aminopropyltriethoxysilane (APTS). Both the pristine and functionalized MWCNTs were characterized for their surface morphology, chemical composition and functional groups by using FESEM, EDX and FTIR techniques. The acidic and APTS treatment to MWCNTs resulted in unbundling and loosening of the nanotubes from their bundled, agglomerated and entangled forms. Furthermore, oxidation and functionalization also significantly influenced the CO2 adsorption capacity of MWCNTs. The breakthrough curves (adsorption isotherms) revealed that the modified MWCNTs exhibit higher capacity for CO2 adsorption as compared to the pristine MWCNTs. Overall, CO2 uptake by the pristine and modified MWCNTs was found about 0.00025 mol/g and 0.00038 mol/g, respectively.

  8. Hydroquinone and Quinone-Grafted Porous Carbons for Highly Selective CO2 Capture from Flue Gases and Natural Gas Upgrading.

    PubMed

    Wang, Jun; Krishna, Rajamani; Yang, Jiangfeng; Deng, Shuguang

    2015-08-04

    Hydroquinone and quinone functional groups were grafted onto a hierarchical porous carbon framework via the Friedel-Crafts reaction to develop more efficient adsorbents for the selective capture and removal of carbon dioxide from flue gases and natural gas. The oxygen-doped porous carbons were characterized with scanning electron microscopy, transmission electron microscopy, X-ray powder diffraction, Fourier transform infrared spectroscopy, and Raman spectroscopy. CO2, CH4, and N2 adsorption isotherms were measured and correlated with the Langmuir model. An ideal adsorbed solution theory (IAST) selectivity for the CO2/N2 separation of 26.5 (298 K, 1 atm) was obtained on the hydroquinone-grafted carbon, which is 58.7% higher than that of the pristine porous carbon, and a CO2/CH4 selectivity value of 4.6 (298 K, 1 atm) was obtained on the quinone-grafted carbon (OAC-2), which represents a 28.4% improvement over the pristine porous carbon. The highest CO2 adsorption capacity on the oxygen-doped carbon adsorbents is 3.46 mmol g(-1) at 298 K and 1 atm. In addition, transient breakthrough simulations for CO2/CH4/N2 mixture separation were conducted to demonstrate the good separation performance of the oxygen-doped carbons in fixed bed adsorbers. Combining excellent adsorption separation properties and low heats of adsorption, the oxygen-doped carbons developed in this work appear to be very promising for flue gas treatment and natural gas upgrading.

  9. Low-temperature upgrading of low-calorific biogas for CO2 mitigation using DBD-catalyst hybrid reactor

    NASA Astrophysics Data System (ADS)

    Nozaki, Tomohiro; Tsukijihara, Hiroyuki; Fukui, Wataru; Okazaki, Ken

    2006-10-01

    Although huge amounts of biogas, which consists of 20-60% of CH4 in CO2/N2, can be obtained from landfills, coal mines, and agricultural residues, most of them are simply flared and wasted: because global warming potential of biogas is 5-15 times as potent as CO2. Poor combustibility of such biogas makes it difficult to utilize in conventional energy system. The purpose of this project is to promote the profitable recovery of methane from poor biogas via non-thermal plasma technology. We propose low-temperature steam reforming of biogas using DBD generated in catalyst beds. Methane is partially converted into hydrogen, and then fed into internal combustion engines for improved ignition stability as well as efficient operation. Low-temperature steam reforming is beneficial because exhaust gas from an engine can be used to activate catalyst beds. Space velocity (3600-15000 hr-1), reaction temperature (300-650^oC), and energy cost (30-150 kJ per mol CH4) have been investigated with simulated biogas (20-60% CH4 in mixtures of CO2/N2). The DBD enhances reaction rate of CH4 by a factor of ten at given catalyst temperatures, which is a rate-determining step of methane steam reforming, while species concentration of upgraded biogas was governed by thermodynamic equilibrium in the presence of catalyst.

  10. CO2 adsorption on chemically modified activated carbon.

    PubMed

    Caglayan, Burcu Selen; Aksoylu, A Erhan

    2013-05-15

    CO2 adsorption capacity of a commercial activated carbon was improved by using HNO3 oxidation, air oxidation, alkali impregnation and heat treatment under helium gas atmosphere. The surface functional groups produced were investigated by diffuse reflectance infrared Fourier transform spectrometer (DRIFTS). CO2 adsorption capacities of the samples were determined by gravimetric analyses for 25-200°C temperature range. DRIFTS studies revealed the formation of carboxylic acid groups on the HNO3 oxidized adsorbents. Increased aromatization and uniform distribution of the Na particles were observed on the samples prepared by Na2CO3 impregnation onto HNO3 oxidized AC support. The adsorption capacities of the nonimpregnated samples were increased by high temperature helium treatments or by increasing the adsorption temperature; both leading to decomposition of surface oxygen groups, forming sites that can easily adsorb CO2. The adsorption capacity loss due to cyclic adsorption/desorption procedures was overcome with further surface stabilization of Na2CO3 modified samples with high temperature He treatments. With Na2CO3 impregnation the mass uptakes of the adsorbents at 20 bars and 25 °C were improved by 8 and 7 folds and at 1 bar were increased 15 and 16 folds, on the average, compared to their air oxidized and nitric acid oxidized supports, respectively.

  11. Chemical transformation of CO2 during its capture by waste biomass derived biochars.

    PubMed

    Xu, Xiaoyun; Kan, Yue; Zhao, Ling; Cao, Xinde

    2016-06-01

    Biochar is a porous carbonaceous material with high alkalinity and rich minerals, making it possible for CO2 capture. In this study, biochars derived from pig manure, sewage sludge, and wheat straw were evaluated for their CO2 sorption behavior. All three biochars showed high sorption abilities for CO2, with the maximum capacities reaching 18.2-34.4 mg g(-1) at 25 °C. Elevating sorption temperature and moisture content promoted the transition of CO2 uptake from physical to chemical process. Mineral components such as Mg, Ca, Fe, K, etc. in biochar induced the chemical sorption of CO2 via the mineralogical reactions which occupied 17.7%-50.9% of the total sorption. FeOOH in sewage sludge biochar was transformed by sorbed CO2 into Fe(OH)2CO3, while the sorbed CO2 in pig manure biochar was precipitated as K2Ca(CO3)2 and CaMg(CO3)2, which resulted in a dominant increase of insoluble inorganic carbon in both biochars. For wheat straw biochar, sorbed CO2 induced CaCO3 transformed into soluble Ca(HCO3)2, which led to a dominant increase of soluble inorganic carbons. The results obtained from this study demonstrated that biochar as a unique carbonaceous material could distinctly be a promising sorbent for CO2 capture in which chemical sorption induced by mineralogical reactions played an important role.

  12. Encapsulated Ionic Liquids for CO2 Capture: Using 1-Butyl-methylimidazolium Acetate for Quick and Reversible CO2 Chemical Absorption.

    PubMed

    Moya, Cristian; Alonso-Morales, Noelia; Gilarranz, Miguel A; Rodriguez, Juan J; Palomar, Jose

    2016-12-05

    The potential advantages of applying encapsulated ionic liquid (ENIL) to CO2 capture by chemical absorption with 1-butyl-3-methylimidazolium acetate [bmim][acetate] are evaluated. The [bmim][acetate]-ENIL is a particle material with solid appearance and 70 % w/w in ionic liquid (IL). The performance of this material as CO2 sorbent was evaluated by gravimetric and fixed-bed sorption experiments at different temperatures and CO2 partial pressures. ENIL maintains the favourable thermodynamic properties of the neat IL regarding CO2 absorption. Remarkably, a drastic increase of CO2 sorption rates was achieved using ENIL, related to much higher contact area after discretization. In addition, experiments demonstrate reversibility of the chemical reaction and the efficient ENIL regeneration, mainly hindered by the unfavourable transport properties. The common drawback of ILs as CO2 chemical absorbents (low absorption rate and difficulties in solvent regeneration) are overcome by using ENIL systems.

  13. CO2 utilization: an enabling element to move to a resource- and energy-efficient chemical and fuel production.

    PubMed

    Ampelli, Claudio; Perathoner, Siglinda; Centi, Gabriele

    2015-03-13

    CO(2) conversion will be at the core of the future of low-carbon chemical and energy industry. This review gives a glimpse into the possibilities in this field by discussing (i) CO(2) circular economy and its impact on the chemical and energy value chain, (ii) the role of CO(2) in a future scenario of chemical industry, (iii) new routes for CO(2) utilization, including emerging biotechnology routes, (iv) the technology roadmap for CO(2) chemical utilization, (v) the introduction of renewable energy in the chemical production chain through CO(2) utilization, and (vi) CO(2) as a suitable C-source to move to a low-carbon chemical industry, discussing in particular syngas and light olefin production from CO(2). There are thus many stimulating possibilities offered by using CO(2) and this review shows this new perspective on CO(2) at the industrial, societal and scientific levels.

  14. Organic reactions for the electrochemical and photochemical production of chemical fuels from CO2--The reduction chemistry of carboxylic acids and derivatives as bent CO2 surrogates.

    PubMed

    Luca, Oana R; Fenwick, Aidan Q

    2015-11-01

    The present review covers organic transformations involved in the reduction of CO2 to chemical fuels. In particular, we focus on reactions of CO2 with organic molecules to yield carboxylic acid derivatives as a first step in CO2 reduction reaction sequences. These biomimetic initial steps create opportunities for tandem electrochemical/chemical reductions. We draw parallels between long-standing knowledge of CO2 reactivity from organic chemistry, organocatalysis, surface science and electrocatalysis. We point out some possible non-faradaic chemical reactions that may contribute to product distributions in the production of solar fuels from CO2. These reactions may be accelerated by thermal effects such as resistive heating and illumination.

  15. Soil CO2 dynamics, acidification, and chemical weathering in a temperate forest with experimental CO2 enrichment

    NASA Astrophysics Data System (ADS)

    Andrews, Jeffrey A.; Schlesinger, William H.

    2001-03-01

    Soils constitute a major component of the global carbon cycle that will be affected by anthropogenic additions of CO2 to the atmosphere. As part of the Duke Forest Free-Air CO2 Enrichment (FACE) experiment, we examined how forest growth at elevated (+200 ppmv) atmospheric CO2 concentration affects CO2 dynamics in the soil. Soil respiration and the concentration of CO2 in the soil pore space to a depth of 200 cm were measured over a 3-year period. Soil CO2 production was linked to soil acidification and mineral weathering by measuring changes in the composition of the soil solution, including alkalinity, Si, and major cations. The total flux of dissolved inorganic carbon to groundwater was then calculated from field measurements. The FACE fumigation gas contained a unique 13C signature that labeled newly fixed carbon, which was monitored in the soil system. As a result of CO2 enrichment, annual soil respiration increased by 27% and was accompanied by higher CO2 concentrations in the soil pore space. These changes to soil CO2 dynamics were most likely the result of increased root and rhizosphere respiration, as suggested by the changes to the δ13C of soil CO2. Increased soil CO2 under FACE accelerated the rates of soil acidification and mineral weathering. Thus an increase of 55% in atmospheric CO2 concentration over 2 years resulted in a 271% increase in soil solution cation concentration, a 162% increase in alkalinity, and a 25% increase in Si concentration at 200-cm depth. The flux of dissolved inorganic carbon to groundwater increased by 33%, indicating a negative feedback to changes in atmospheric CO2 that could regulate the global carbon cycle over geological time.

  16. Early opportunities of CO2 geological storage deployment in coal chemical industry in China

    SciTech Connect

    Wei, Ning; Li, Xiaochun; Liu, Shengnan; Dahowski, Robert T.; Davidson, Casie L.

    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 sources 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.

  17. Thermo-chemical process with sewage sludge by using CO2.

    PubMed

    Kwon, Eilhann E; Yi, Haakrho; Kwon, Hyun-Han

    2013-10-15

    This work proposed a novel methodology for energy recovery from sewage sludge via the thermo-chemical process. The impact of CO2 co-feed on the thermo-chemical process (pyrolysis and gasification) of sewage sludge was mainly investigated to enhance thermal efficiency and to modify the end products from the pyrolysis and gasification process. The CO2 injected into the pyrolysis and gasification process enhance the generation of CO. As compared to the thermo-chemical process in an inert atmosphere (i.e., N2), the generation of CO in the presence of CO2 was enhanced approximately 200% at the temperature regime from 600 to 900 °C. The introduction of CO2 into the pyrolysis and gasification process enabled the condensable hydrocarbons (tar) to be reduced considerably by expediting thermal cracking (i.e., approximately 30-40%); thus, exploiting CO2 as chemical feedstock and/or reaction medium for the pyrolysis and gasification process leads to higher thermal efficiency, which leads to environmental benefits. This work also showed that sewage sludge could be a very strong candidate for energy recovery and a raw material for chemical feedstock.

  18. Feasibility study of a novel pressure recovery system for CO2-COIL based on chemical absorption

    NASA Astrophysics Data System (ADS)

    Li, Qingwei; Jin, Yuqi; Geng, Zicai; Li, Yongzhao; Zhang, Yuelong; Sang, Fengting

    2015-02-01

    A chemical oxygen-iodine laser (COIL) is an electronic transition, low pressure, high throughput system. The use of this laser demands a suitable pressure recovery system. This paper proposed a novel pressure recovery system based on chemical absorption and the feasibility for COIL with CO2 as buffer gas (CO2-COIL) was investigated. The novel pressure recovery system works by chemisorbing the CO2-COIL effluents into two fixed-beds maintained at initial temperature of around 293-323K. Compared with the cryosorption system for N2-COIL based on physical absorption, the novel chemisorptions based pressure recovery system has a simpler logistics and a shorter run-to-run preparation time. Two kinds of solid chemo-sorbents were designed and synthesized. One was used for chemisorbing the oxidizing gases such as O2 ,Cl2 and I2, another was used for chemisorbing the acidic gas such as CO2. The capacities of the two sorbents were measured to be 3.12 mmol(O2)/g and 3.84 mmol (CO2) /g, respectively. It indicated that the synthesized sorbents could effectively chemosorb the CO2-COIL effluents. Secondly, analog test equipment was set up and used to study the feasibility of the novel pressure recovery system used for CO2-COIL. The test results showed that the novel pressure recovery system could maintain the pressure under 6 Torr for tens seconds under the continuous gas flow. It showed that the novel pressure recovery system for CO2-COIL based on chemical absorption is feasible.

  19. Biocatalysis for the application of CO2 as a chemical feedstock

    PubMed Central

    Easton, Christopher J

    2015-01-01

    Summary Biocatalysts, capable of efficiently transforming CO2 into other more reduced forms of carbon, offer sustainable alternatives to current oxidative technologies that rely on diminishing natural fossil-fuel deposits. Enzymes that catalyse CO2 fixation steps in carbon assimilation pathways are promising catalysts for the sustainable transformation of this safe and renewable feedstock into central metabolites. These may be further converted into a wide range of fuels and commodity chemicals, through the multitude of known enzymatic reactions. The required reducing equivalents for the net carbon reductions may be drawn from solar energy, electricity or chemical oxidation, and delivered in vitro or through cellular mechanisms, while enzyme catalysis lowers the activation barriers of the CO2 transformations to make them more energy efficient. The development of technologies that treat CO2-transforming enzymes and other cellular components as modules that may be assembled into synthetic reaction circuits will facilitate the use of CO2 as a renewable chemical feedstock, greatly enabling a sustainable carbon bio-economy. PMID:26734087

  20. Biocatalysis for the application of CO2 as a chemical feedstock.

    PubMed

    Alissandratos, Apostolos; Easton, Christopher J

    2015-01-01

    Biocatalysts, capable of efficiently transforming CO2 into other more reduced forms of carbon, offer sustainable alternatives to current oxidative technologies that rely on diminishing natural fossil-fuel deposits. Enzymes that catalyse CO2 fixation steps in carbon assimilation pathways are promising catalysts for the sustainable transformation of this safe and renewable feedstock into central metabolites. These may be further converted into a wide range of fuels and commodity chemicals, through the multitude of known enzymatic reactions. The required reducing equivalents for the net carbon reductions may be drawn from solar energy, electricity or chemical oxidation, and delivered in vitro or through cellular mechanisms, while enzyme catalysis lowers the activation barriers of the CO2 transformations to make them more energy efficient. The development of technologies that treat CO2-transforming enzymes and other cellular components as modules that may be assembled into synthetic reaction circuits will facilitate the use of CO2 as a renewable chemical feedstock, greatly enabling a sustainable carbon bio-economy.

  1. Global metabolic rewiring for improved CO2 fixation and chemical production in cyanobacteria

    NASA Astrophysics Data System (ADS)

    Kanno, Masahiro; Carroll, Austin L.; Atsumi, Shota

    2017-03-01

    Cyanobacteria have attracted much attention as hosts to recycle CO2 into valuable chemicals. Although cyanobacteria have been engineered to produce various compounds, production efficiencies are too low for commercialization. Here we engineer the carbon metabolism of Synechococcus elongatus PCC 7942 to improve glucose utilization, enhance CO2 fixation and increase chemical production. We introduce modifications in glycolytic pathways and the Calvin Benson cycle to increase carbon flux and redirect it towards carbon fixation. The engineered strain efficiently uses both CO2 and glucose, and produces 12.6 g l-1 of 2,3-butanediol with a rate of 1.1 g l-1 d-1 under continuous light conditions. Removal of native regulation enables carbon fixation and 2,3-butanediol production in the absence of light. This represents a significant step towards industrial viability and an excellent example of carbon metabolism plasticity.

  2. Physico-Chemical Behavior of Nanoparticles at CO2-Water-Rock Interfaces

    NASA Astrophysics Data System (ADS)

    Jun, Y.; Shao, H.; Hu, Y.; Matos, R.

    2009-12-01

    Recently, to help mitigate global climate-change and energy problems, much effort has recently been devoted to developing methods for sequestering anthropogenic CO2 from coal-fired power plants. One of the most promising methods is geological CO2 sequestration (GS). Some prior studies of geological CO2 sequestration have mainly examined the physical processes that occur during the sequestration of CO2. However, most of the relevant studies are based on hydrological transport, using simulation models rather than studying actual interfacial chemical reactions in the ground. The mechanisms, kinetics, and environmental impact of interfacial reactions among CO2-H2O-mineral surfaces at the molecular scale have not been well understood. Changes in the porosity of the mineral phases at the geological formation sites, especially the dissolution of the mineral phase or precipitation of secondary minerals in the pores, will affect the fate and transport of CO2 and the integrity of seals and the matrix within the reservoirs. So far, little is known about the kinetics of the possible geochemical reactions of supercritical CO2 in brine and pre-existing mineral interfaces, or about the ultimate fate and transport of the injected CO2. We investigated the physico-chemical property changes of reference mineral samples (clay minerals) as well as field site samples (sandstone and caprock from the Illinois Basin) by chemical reactions at CO2-H2O-mineral interfaces. We investigated whether reactions between caprock and CO2 can change the integrity of caprock. Our experimental results with caprock samples (CONSOL coal mine sites, West Virginia) indicate that after 14 days in contact with 1 atm CO2 saturated saline water at 80°C, the concentrations of dissolved metals have increased from zero to as high as 47,000 ppm. In our experiments with caprocks and sandstones from GS sites of the Midwest Geological Sequestration Consortium, we found that the most significant extent of dissolution

  3. O3, CO2 and chemical fractionation in ponderosa pine saplings

    EPA Science Inventory

    Environmental factors can affect plant tissue quality which is important for quality of organic matter inputs into soil food webs and decomposition of soil organic matter. Thus the effects of increases in CO2 and O3 and their interactions were determined for various chemical fra...

  4. CO2 recycling: a key strategy to introduce green energy in the chemical production chain.

    PubMed

    Perathoner, Siglinda; Centi, Gabriele

    2014-05-01

    The introduction of renewable energy in the chemical production chain is a key strategic factor both to realize a sustainable, resource-efficient, low-carbon economy and society and to drive innovation and competiveness in the chemical production. This Concept discusses this concept in terms of motivations, perspectives, and impact as well as technical barriers to achieve this goal. It is shown how an important element to realize this scenario is to foster the paths converting carbon dioxide (CO2) into feedstock for the chemical/process industry, which is one of the most efficient methods to rapidly introduce renewable energy into the chemical production chain. Some of the possible options to proceed in this direction are discussed, with focus on the technical barriers and enabling factors such as catalysis. The tight interconnection between CO2 management and the use of renewable energy is evidenced.

  5. Microbial, Physical and Chemical Drivers of COS and 18O-CO2 Exchange in Soils

    NASA Astrophysics Data System (ADS)

    Meredith, L. K.; Boye, K.; Whelan, M.; Pang, E.; von Sperber, C.; Brueggemann, N.; Berry, J. A.; Welander, P. V.

    2015-12-01

    Carbonyl sulfide (COS) and the oxygen isotope composition (δ18O) of CO2 are potential tools for differentiating the contributions of photosynthesis and respiration to the balance of global carbon cycling. These processes are coupled at the leaf level via the enzyme carbonic anhydrase (CA), which hydrolyzes CO2 in the first biochemical step of the photosynthetic pathway (CO2 + H2O ⇌ HCO3- + H+) and correspondingly structural analogue COS (COS + H2O → CO2 + H2S). CA also accelerates the exchange of oxygen isotopes between CO2 and H2O leading to a distinct isotopic imprint [1]. The biogeochemical cycles of these tracers include significant, yet poorly characterized soil processes that challenge their utility for probing the carbon cycle. In soils, microbial CA also hydrolyze COS and accelerate O isotope exchange between CO2 and soil water. Soils have been observed to emit COS by undetermined processes. To account for these soil processes, measurements are needed to identify the key microbial, chemical, and physical factors. In this study, we survey COS and δ18O exchange in twenty different soils spanning a variety of biomes and soil properties. By comparing COS fluxes and δ18O-CO2 values emitted from moist soils we investigate whether the same types of CA catalyze these two processes. Additionally, we seek to identify the potential chemical drivers of COS emissions by measuring COS fluxes in dry soils. These data are compared with soil physical (bulk density, volumetric water content, texture), chemical (pH, elemental analysis, sulfate, sulfur K-edge XANES), and microbial measurements (biomass and phylogeny). Furthermore, we determine the abundance and diversity of CA-encoding genes to directly link CA with measured soil function. This work will define the best predictors for COS fluxes and δ18O-CO2 values from our suite of biogeochemical measurements. The suitability of identified predictor variables can be tested in follow-up studies and applied for modeling

  6. Sorbents with high efficiency for CO2 capture based on amines-supported carbon for biogas upgrading.

    PubMed

    Pino, Lidia; Italiano, Cristina; Vita, Antonio; Fabiano, Concetto; Recupero, Vincenzo

    2016-10-01

    Sorbents for CO2 capture have been prepared by wet impregnation of a commercial active carbon (Ketjen-black, Akzo Nobel) with two CO2-philic compounds, polyethylenimine (PEI) and tetraethylenepentamine (TEPA), respectively. The effects of amine amount (from 10 to 70wt.%), CO2 concentration in the feed, sorption temperature and gas hourly space velocity on the CO2 capture performance have been investigated. The sorption capacity has been evaluated using the breakthrough method, with a fixed bed reactor equipped with on line gas chromatograph. The samples have been characterized by N2 adsorption-desorption, scanning electron microscopy and energy dispersive X-ray (SEM/EDX). A promising CO2 sorption capacity of 6.90 mmol/gsorbent has been obtained with 70wt.% of supported TEPA at 70°C under a stream containing 80vol% of CO2. Sorption tests, carried out with simulated biogas compositions (CH4/CO2 mixtures), have revealed an appreciable CO2 separation selectivity; stable performance was maintained for 20 adsorption-desorption cycles.

  7. CO2 laser scribe of chemically strengthened glass with high surface compressive stress

    NASA Astrophysics Data System (ADS)

    Li, Xinghua; Vaddi, Butchi R.

    2011-03-01

    Chemically strengthened glass is finding increasing use in handheld, IT and TV cover glass applications. Chemically strengthened glass, particularly with high (>600MPa) compressive stress (CS) and deeper depth of layer (DOL), enable to retain higher strength after damage than non-strengthened glass when its surface is abraded. Corning Gorilla® Glass has particularly proven to be advantageous over competition in this attribute. However, due to high compressive stress (CS) and Central Tension (CT) cutting ion-exchanged glass is extremely difficult and often unmanageable where ever the applications require dicing the chemically strengthened mother glass into smaller parts. We at Corning have developed a CO2 laser scribe and break method (LSB) to separate a single chemically strengthened glass sheet into plurality of devices. Furthermore, CO2 laser scribe and break method enables debris-free separation of glass with high edge strength due to its mirror-like edge finish. We have investigated laser scribe and break of chemically strengthened glass with surface compressive stress greater than 600 MPa. In this paper we present the results of CO2 scribe and break method and underlying laser scribing mechanisms. We demonstrated cross-scribe repetitively on GEN 2 size chemically strengthened glass substrates. Specimens for edge strength measurements of different thickness and CS/DOL glass were prepared using the laser scribe and break technique. The specimens were tested using the standard 4-point bend method and the results are presented.

  8. Carbamate stabilities of sterically hindered amines from quantum chemical methods: relevance for CO2 capture.

    PubMed

    Gangarapu, Satesh; Marcelis, Antonius T M; Zuilhof, Han

    2013-12-02

    The influence of electronic and steric effects on the stabilities of carbamates formed from the reaction of CO2 with a wide range of alkanolamines was investigated by quantum chemical methods. For the calculations, B3LYP, M11-L, MP2, and spin-component-scaled MP2 (SCS-MP2) methods were used, coupled with SMD and SM8 solvation models. A reduction in carbamate stability leads to an increased CO2 absorption capacity of the amine and a reduction of the energy required for solvent regeneration. Important factors for the reduction of the carbamate stability were an increase in steric hindrance around the nitrogen atom, charge on the N atom and intramolecular hydrogen bond strength. The present study indicates that secondary ethanolamines with sterically hindering groups near the N atom show significant potential as candidates for industrial CO2-capture solvents.

  9. Catalytic upgrading of butyric acid towards fine chemicals and biofuels

    PubMed Central

    Sjöblom, Magnus; Matsakas, Leonidas; Christakopoulos, Paul; Rova, Ulrika

    2016-01-01

    Fermentation-based production of butyric acid is robust and efficient. Modern catalytic technologies make it possible to convert butyric acid to important fine chemicals and biofuels. Here, current chemocatalytic and biocatalytic conversion methods are reviewed with a focus on upgrading butyric acid to 1-butanol or butyl-butyrate. Supported Ruthenium- and Platinum-based catalyst and lipase exhibit important activities which can pave the way for more sustainable process concepts for the production of green fuels and chemicals. PMID:26994015

  10. Frontiers, Opportunities, and Challenges in Biochemical and Chemical Catalysis of CO2

    SciTech Connect

    Appel, Aaron M.; Bercaw, John E.; Bocarsly, Andrew B.; Dobbek, Holger; DuBois, Daniel L.; Dupuis, Michel; Ferry, James G.; Fujita, Etsuko; Hille, Russ; Kenis, Paul; Kerfeld, Cheryl A.; Morris, Robert H.; Peden, Charles HF; Portis, Archie; Ragsdale, Steve; Rauchfuss, Thomas B.; Reek, Joost; Seefeldt, Lance C.; Thauer, Rudolf K.; Waldrop, Grover L.

    2013-08-14

    Our central premise is that catalytic scientists can learn by studying how these important metabolic processes occur in nature. Complementarily, biochemists can learn by studying how catalytic scientists view these same chemical transformations promoted by synthetic catalysts. From these studies, hypotheses can be developed and tested through manipulation of enzyme structure and by synthesizing simple molecular catalysts to incorporate different structural features of the enzymes. It is hoped that these studies will lead to new and useful concepts in catalyst design for fuel production and utilization. This paper describes the results of a workshop held to explore these concepts in regard to the development of new and more efficient catalytic processes for the conversion of CO2 to a variety of carbon-based fuels. The organization of this overview/review is as follows: 1) The first section briefly explores how interactions between the catalysis and biological communities have been fruitful in developing new catalysts for the reduction of protons to hydrogen, the simplest fuel generation reaction. 2) The second section assesses the state of the art in both biological and chemical reduction of CO2 by two electrons to form either carbon monoxide (CO) or formate (HCOO-). It also attempts to identify common principles between biological and synthetic catalysts and productive areas for future research. 3) The third section explores both biological and chemical processes that result in the reduction of CO2 beyond the level of CO and formate, again seeking to identify common principles and productive areas of future research. 4) The fourth section explores the formation of carbon-carbon bonds in biological and chemical systems in the same vein as the other sections. 5) A fifth section addresses the role of non-redox reactions of CO2 in biological systems and their role in carbon metabolism, with a parallel discussion of chemical systems. 6) In section 6, the topics of

  11. Bio-electrochemical synthesis of commodity chemicals by autotrophic acetogens utilizing CO2 for environmental remediation.

    PubMed

    Jabeen, Gugan; Farooq, Robina

    2016-09-01

    Bio-electrochemical synthesis (BES) is a technique in which electro-autotrophic bacteria such as Clostridium ljungdahlii utilize electric currents as an electron source from the cathode to reduce CO2 to extracellular, multicarbon, exquisite products through autotrophic conversion. The BES of volatile fatty acids and alcohols directly from CO2 is a sustainable alternative for non-renewable, petroleum-based polymer production. This conversion of CO2 implies reduction of greenhouse gas emissions. The synthesis of heptanoic acid, heptanol, hexanoic acid and hexanol, for the first time, by Clostridium ljungdahlii was a remarkable achievement of BES. In our study, these microorganisms were cultivated on the cathode of a bio-electrochemical cell at -400 mV by a DC power supply at 37 degree Centrigrade, pH 6.8, and was studied for both batch and continuous systems. Pre-enrichment of bio-cathode enhanced the electroactivity of cells and resulted in maximizing extracellular products in less time. The main aim of the research was to investigate the impact of low-cost substrate CO2, and the longer cathode recovery range was due to bacterial reduction of CO2 to multicarbon chemical commodities with electrons driven from the cathode. Reactor design was simplified for cost-effectiveness and to enhance energy efficiencies. The Columbic recovery of ethanoic acid, ethanol, ethyl butyrate, hexanoic acid, heptanoic acid and hexanol being in excess of 80 percent proved that BES was a remarkable technology.

  12. Microbial electrolysis desalination and chemical-production cell for CO2 sequestration.

    PubMed

    Zhu, Xiuping; Logan, Bruce E

    2014-05-01

    Mineral carbonation can be used for CO2 sequestration, but the reaction rate is slow. In order to accelerate mineral carbonation, acid generated in a microbial electrolysis desalination and chemical-production cell (MEDCC) was examined to dissolve natural minerals rich in magnesium/calcium silicates (serpentine), and the alkali generated by the same process was used to absorb CO2 and precipitate magnesium/calcium carbonates. The concentrations of Mg(2+) and Ca(2+) dissolved from serpentine increased 20 and 145 times by using the acid solution. Under optimal conditions, 24 mg of CO2 was absorbed into the alkaline solution and 13 mg of CO2 was precipitated as magnesium/calcium carbonates over a fed-batch cycle (24h). Additionally, the MEDCC removed 94% of the COD (initially 822 mg/L) and achieved 22% desalination (initially 35 g/L NaCl). These results demonstrate the viability of this process for effective CO2 sequestration using renewable organic matter and natural minerals.

  13. 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

    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.

  14. Chemical and Physical Reactions of Wellbore Cement under CO2 Storage Conditions: Effects of Cement Additives

    NASA Astrophysics Data System (ADS)

    Kutchko, B. G.; Strazisar, B. R.; Huerta, N.; Lowry, G. V.; Dzombak, D. A.; Thaulow, N.

    2008-12-01

    Sequestration of CO2 into geologic formations requires long-term storage and low leakage rates to be effective. Active and abandoned wells in candidate storage formations must be evaluated as potential leakage points. Wellbore integrity is an important part of an overall integrated assessment program being developed at NETL to assess potential risks at CO2 storage sites. Such a program is needed for ongoing policy and regulatory decisions for geologic carbon sequestration. The permeability and integrity of the cement in the well is a primary factor affecting its ability to prevent leakage. Cement must be able to maintain low permeability over lengthy exposure to reservoir conditions in a CO2 injection and storage scenario. Although it is known that cement may be altered by exposure to CO2, the results of ongoing research indicate that cement curing conditions, fluid properties, and cement additives play a significant role in the rate of alteration and reaction. The objective of this study is to improve understanding of the factors affecting wellbore cement integrity for large-scale geologic carbon sequestration projects. Due to the high frequency use of additives (pozzolan) in wellbore cement, it is also essential to understand the reaction of these cement-pozzolan systems upon exposure to CO2 under sequestration conditions (15.5 MPa and 50°C). Laboratory experiments were performed to determine the physical and chemical changes, as well as the rate of alteration of commonly used pozzolan-cement systems under simulated sequestration reservoir conditions, including both supercritical CO2 and CO2-saturated brine. The rate of alteration of the cement-pozzolan systems is considerably faster than with neat cement. However, the alteration of physical properties is much less significant with the pozzolanic blends. Permeability of a carbonated pozzolanic cement paste remains sufficiently small to block significant vertical migration of CO2 in a wellbore. All of the

  15. Development and testing of a long-range airborne CO2 DIAL chemical detection system

    NASA Astrophysics Data System (ADS)

    Higdon, N. Scott; Senft, Daniel C.; Fox, Marsha J.; Hamilton, Carla M.; Kelly, Brian T.; Dowling, James A.; Pierrottet, Diego F.; Dean, David R.; Richter, Dale A.; Bousek, Ronald R.

    1998-11-01

    The Air Force Research Laboratory has developed and tested an airborne CO2 differential absorption lidar system for the remote detection of chemicals. The Laser Airborne Remote Sensing DIAL system uses topographic backscatter to provide a long-range measurement of the column-content absorption of chemical plumes in the path of the laser beam. A high-power CO2 laser, capable of operation on multiple isotopes, and a Mersenne telescope constitute the major transceiver components. In addition to the laser, telescope, and transceiver optics, several onboard diagnostic instruments were mounted on the flight bench to monitor and optimize the system performance during airborne operation. The flight bench, electronics racks, and data acquisition and experiment control stations were designed to be integrated onto the AFRL C-135E research aircraft, and to utilize the existing pointing and tracking system on the aircraft.

  16. Chemicals loading in acetylated bamboo assisted by supercritical CO2 based on phase equilibrium data

    NASA Astrophysics Data System (ADS)

    Silviana, Petermann, M.

    2015-12-01

    Indonesia has a large tropical forest. However, the deforestation still appears annually and vastly. This reason drives a use of bamboo as wood alternative. Recently, there are many modifications of bamboo in order to prolong the shelf life. Unfortunately, the processes need more chemicals and time. Based on wood modification, esterifying of bamboo was undertaken in present of a dense gas, i.e. supercritical CO2. Calculation of chemicals loading referred to ASTM D1413-99 by using the phase equilibrium data at optimum condition by a statistical design. The results showed that the acetylation of bamboo assisted by supercritical CO2 required 14.73 kg acetic anhydride/m3 of bamboo for a treatment of one hour.

  17. Chemical and anatomical changes in Liquidambar styraciflua L. xylem after long term exposure to elevated CO2.

    PubMed

    Kim, Keonhee; Labbé, Nicole; Warren, Jeffrey M; Elder, Thomas; Rials, Timothy G

    2015-03-01

    The anatomical and chemical characteristics of sweetgum were studied after 11 years of elevated CO2 (544 ppm, ambient at 391 ppm) exposure. Anatomically, branch xylem cells were larger for elevated CO2 trees, and the cell wall thickness was thinner. Chemically, elevated CO2 exposure did not impact the structural components of the stem wood, but non-structural components were significantly affected. Principal component analysis (PCA) was employed to detect differences between the CO2 treatments by considering numerous structural and chemical variables, as well as tree size, and data from previously published sources (i.e., root biomass, production and turnover). The PCA results indicated a clear separation between trees exposed to ambient and elevated CO2 conditions. Correlation loadings plots of the PCA revealed that stem structural components, ash, Ca, Mg, total phenolics, root biomass, production and turnover were the major responses that contribute to the separation between the elevated and ambient CO2 treated trees.

  18. FMC Chemicals: Burner Management System Upgrade Improves Performance and Saves Energy at a Chemical Plant

    SciTech Connect

    Not Available

    2004-07-01

    FMC Chemicals Corporation increased the efficiency of two large coal-fired boilers at its soda ash mine in Green River, Wyoming, by upgrading the burner management system. The project yields annual energy savings of 250,000 MMBtu.

  19. Stream geochemistry, chemical weathering and CO 2 consumption potential of andesitic terrains, Dominica, Lesser Antilles

    NASA Astrophysics Data System (ADS)

    Goldsmith, Steven T.; Carey, Anne E.; Johnson, Brent M.; Welch, Susan A.; Lyons, W. Berry; McDowell, William H.; Pigott, Jeffrey S.

    2010-01-01

    Recent studies of chemical weathering of andesitic-dacitic material on high-standing islands (HSIs) have shown these terrains have some of the highest observed rates of chemical weathering and associated CO 2 consumption yet reported. However, the paucity of stream gauge data in many of these terrains has limited determination of chemical weathering product fluxes. In July 2006 and March 2008, stream water samples were collected and manual stream gauging was performed in watersheds throughout the volcanic island of Dominica in the Lesser Antilles. Distinct wet and dry season solute concentrations reveal the importance of seasonal variations on the weathering signal. A cluster analysis of the stream geochemical data shows the importance of parent material age on the overall delivery of solutes. Observed Ca:Na, HCO 3:Na and Mg:Na ratios suggest crystallinity of the parent material may also play an important role in determining weathering fluxes. From total dissolved solids concentrations and mean annual discharge calculations we calculate chemical weathering yields of (6-106 t km -2 a -1), which are similar to those previously determined for basalt terrains. Silicate fluxes (3.1-55.4 t km -2 a -1) and associated CO 2 consumption (190-1575 × 10 3 mol km -2 a -1) determined from our study are among the highest determined to date. The calculated chemical fluxes from our study confirm the weathering potential of andesitic-dacitic terrains and that additional studies of these terrains are warranted.

  20. Chemical absorption and CO2 biofixation via the cultivation of Spirulina in semicontinuous mode with nutrient recycle.

    PubMed

    da Rosa, Gabriel Martins; Moraes, Luiza; Cardias, Bruna Barcelos; de Souza, Michele da Rosa Andrade Zimmermann; Costa, Jorge Alberto Vieira

    2015-09-01

    The chemical absorption of carbon dioxide (CO2) is a technique used for the mitigation of the greenhouse effect. However, this process consumes high amounts of energy to regenerate the absorbent and to separate the CO2. CO2 removal by microalgae can be obtained via the photosynthesis process. The objective of this study was to investigate the cultivation and the macromolecules production by Spirulina sp. LEB 18 with the addition of monoethanolamine (MEA) and CO2. In the cultivation with MEA, were obtained higher results of specific growth rate, biomass productivity, CO2 biofixation, CO2 use efficiency, and lower generation time. Besides this, the carbohydrate concentration obtained at the end of this assay was approximately 96.0% higher than the control assay. Therefore, Spirulina can be produced using medium recycle and the addition of MEA, thereby promoting the reduction of CO2 emissions and showing potential for areas that require higher concentrations of carbohydrates, such as in bioethanol production.

  1. Chemical Processes with Supercritical CO2 in Engineered Geologic Systems: Significance, Previous Study, and Path Forward (Invited)

    NASA Astrophysics Data System (ADS)

    Xu, T.; Pruess, K.

    2009-12-01

    Chemical reactions with dissolved CO2 in the aqueous phase have long been considered in fundamental geosciences and practical applications. Recently, studies on geologic carbon sequestration and enhanced geothermal systems using CO2 as heat transmission fluid have brought new interests in chemical reaction processes directly with supercritical CO2 (scCO2, or gas phase). In the vicinity of a CO2 injection well, the aqueous fluid initially present in a geological formation would be quickly removed by dissolution (evaporation) into the flowing gas stream and by immiscible displacement by the scCO2, creating a gas phase dominant zone. In this zone, the water evaporation could cause formation dry-out and precipitation of salt near the injection well, reducing formation porosity, permeability, and injectivity. The scCO2 may directly attack well construction materials such as cement. Over time, the gas phase will tend to migrate upwards towards the caprock because the density of the scCO2 is lower than that of the aqueous phase. In the upper portions of the reservoir, the scCO2 will directly react with caprock minerals and alter the hydrological properties and mechanical strength. On the other hand, the scCO2 phase will maintain the dissolution into the aqueous phase, lowering pH, inducing mineral dissolution, complexing with dissolved cations, increasing CO2 solubility, increasing the density of the aqueous phase, and promoting “convective mixing”. Chemical processes are quite different in the scCO2 dominant geologic systems. The absence of an aqueous phase poses unique questions, as little is presently known about the chemistry of non-aqueous systems. Additional issues arise from the reactivity of water that is dissolved in the ScCO2 phase. In this presentation, the author will discuss the importance, state of the studies performed, and future research directions.

  2. Electrocatalytic upgrading of biomass pyrolysis oils to chemical and fuel

    NASA Astrophysics Data System (ADS)

    Lam, Chun Ho

    The present project's aim is to liquefy biomass through fast pyrolysis and then upgrade the resulting "bio-oil" to renewable fuels and chemicals by intensifying its energy content using electricity. This choice reflects three points: (a) Liquid hydrocarbons are and will long be the most practical fuels and chemical feedstocks because of their energy density (both mass and volume basis), their stability and relative ease of handling, and the well-established infrastructure for their processing, distribution and use; (b) In the U.S., the total carbon content of annually harvestable, non-food biomass is significantly less than that in a year's petroleum usage, so retention of plant-captured carbon is a priority; and (c) Modern technologies for conversion of sunlight into usable energy forms---specifically, electrical power---are already an order of magnitude more efficient than plants are at storing solar energy in chemical form. Biomass fast pyrolysis (BFP) generates flammable gases, char, and "bio-oil", a viscous, corrosive, and highly oxygenated liquid consisting of large amounts of acetic acid and water together with hundreds of other organic compounds. With essentially the same energy density as biomass and a tendency to polymerize, this material cannot practically be stored or transported long distances. It must be upgraded by dehydration, deoxygenation, and hydrogenation to make it both chemically and energetically compatible with modern vehicles and fuels. Thus, this project seeks to develop low cost, general, scalable, robust electrocatalytic methods for reduction of bio-oil into fuels and chemicals.

  3. Synthesis inversion of atmospheric CO2 using the NIRE chemical transport model

    NASA Astrophysics Data System (ADS)

    Taguchi, Shoichi

    Seasonal variations of CO2 emissions from the land biota and oceans are retrieved by use of an inverse method. Concentrations of CO2, computed by an atmospheric chemical transport model (NIRE-CTM-93), are fitted to the observed CO2 concentrations in terms of annual mean concentrations between 1984 to 1985, one-year period components, half-year components, and a global trend averaged over the years 1979 to 1996. The emissions due to fossil fuel combustion, those from land biota consisting of thirteen land areas, and those from the ocean consisting of twelve oceanic areas, are considered. The problem is solved by a least squares method, using singular value decomposition. A prior estimate of the emissions due to fossil fuel combustion is used as a tight constraint. When the annual mean emission, the net flux from the land biota during the growing season, and the net flux from the ocean are loosely constrained to zero, the solution indicates that areas consist of two groups. That is, those areas with relatively reliable estimates and those without. No reliable estimates are obtained for Africa, tropical and South America, tropical Asia, the tropical and the South Atlantic Ocean, and the western tropical Pacific. A reasonable global budget is not obtained due to unreliable estimates. The amplitude of the seasonal variations over middle-latitude North America is found to be less than that of some tropical land areas.

  4. Controlled noxious chemical stimulation: responses of rat trigeminal brainstem neurones to CO2 pulses applied to the nasal mucosa.

    PubMed

    Anton, F; Peppel, P; Euchner, I; Handwerker, H O

    1991-02-25

    The nasal mucosa of halothane-anesthetized rats was stimulated with defined CO2 pulses. Recordings were performed from single trigeminal brainstem neurons to characterize their responses to this controlled chemical irritation. All cells examined with this stimulus displayed graded discharges to increasing concentrations of CO2. Enhanced responses were obtained in a group of neurons when the duration of the interstimulus interval was increased. The application of chemical irritants, notably mustard oil or acetic acid induced vigorous ongoing discharges in all cells tested. The CO2 stimulation method described here thus provides an ideal model for the quantitative physiological and pharmacological examination of chemically induced nociception.

  5. Porous Ionic Polymers as a Robust and Efficient Platform for Capture and Chemical Fixation of Atmospheric CO2.

    PubMed

    Sun, Qi; Jin, Yingyin; Aguila, Briana; Meng, Xiangju; Ma, Shengqian; Xiao, Feng-Shou

    2017-03-22

    Direct use of atmospheric CO2 as a C1 source to synthesize high-value chemicals through environmentally benign processes is of great interest, yet challenging. Porous heterogeneous catalysts that are capable of simultaneously capturing and converting CO2 are promising candidates for such applications. Herein, a family of organic ionic polymers with nanoporous structure, large surface area, strong affinity for CO2 , and very high density of catalytic active sites (halide ions) was synthesized through the free-radical polymerization of vinylfunctionalized quaternary phosphonium salts. The resultant porous ionic polymers (PIPs) exhibit excellent activities in the cycloaddition of epoxides with atmospheric CO2 , outperforming the corresponding soluble phosphonium salt analogues and ranking among the highest of known metal-free catalytic systems. The high CO2 uptake capacity of the PIPs facilitates the enrichment of CO2 molecules around the catalytic centers, thereby benefiting its conversion. We have demonstrated for the first time that atmospheric CO2 can be directly converted to cyclic carbonates at room temperature using a heterogeneous catalytic system under metal-solvent free conditions. Moreover, the catalysts proved to be robust and fully recyclable, demonstrating promising potential for practical utilization for the chemical fixation of CO2 . Our work thereby paves a way to the advance of PIPs as a new type of platform for capture and conversion of CO2 .

  6. Chemical and magnetic interface properties of tunnel junctionswith co2mnsi/co2fesi multilayer electrode showing large tunnelingmagnetoresistance

    SciTech Connect

    Schmalhorst, J.; Ebke, D.; Sacher, M.D.; Liu, N.; Thomas, A.; Reiss, G.; Hutten, A.; Arenholz, E.

    2007-01-01

    Transport, as well as chemical and magnetic interface properties of two kinds of magnetic tunnel junctions (MTJs) with Co{sub 2}FeSi electrode, Al-O barrier, and Co-Fe counter electrode, are investigated. For junctions with Co{sub 2}FeSi single-layer electrodes, a tunnel magnetoresistance of up to 52% is found after optimal annealing for an optimal Al thickness of 1.5 nm, whereas the room temperature bulk magnetization of the Co{sub 2}FeSi film reaches only 75% of the expected value. By using a [Co{sub 2}MnSi/Co{sub 2}FeSi]{sub x10} multilayer electrode, the magnetoresistance can be increased to 114%, corresponding to a large spin polarization of 0.74, and the full bulk magnetization is reached. For Al thickness smaller than 1 nm, the TMR of both kinds of MTJs decreases rapidly to zero. On the other hand, for 2- to 3-nm-thick Al, the TMR decreases only slowly. The Al thickness dependence of the TMR is directly correlated to the element-specific magnetic moments of Fe and Co at the Co{sub 2}FeSi/Al-O interface for all Al thickness. Especially, for optimal Al thickness and annealing, the interfacial Fe moment of the single-layer electrode is about 20% smaller than for the multilayer electrode, indicating smaller atomic disorder at the barrier interface for the latter MTJ.

  7. Upgraded biogas from municipal solid waste for natural gas substitution and CO2 reduction--a case study of Austria, Italy, and Spain.

    PubMed

    Starr, Katherine; Villalba, Gara; Gabarrell, Xavier

    2015-04-01

    Biogas is rich in methane and can be further purified through biogas upgrading technologies, presenting a viable alternative to natural gas. Landfills and anaerobic digestors treating municipal solid waste are a large source of such biogas. They therefore offer an attractive opportunity to tap into this potential source of natural gas while at the same time minimizing the global warming impact resulting from methane emissions in waste management schemes (WMS) and fossil fuel consumption reduction. This study looks at the current municipal solid waste flows of Spain, Italy, and Austria over one year (2009), in order to determine how much biogas is generated. Then it examines how much natural gas could be substituted by using four different biogas upgrading technologies. Based on current waste generation rates, exploratory but realistic WMS were created for each country in order to maximize biogas production and potential for natural gas substitution. It was found that the potential substitution of natural gas by biogas resulting from the current WMS seems rather insignificant: 0.2% for Austria, 0.6% for Italy and 0.3% for Spain. However, if the WMS is redesigned to maximize biogas production, these figures can increase to 0.7% for Austria, 1% for Italy and 2% for Spain. Furthermore, the potential CO2 reduction as a consequence of capturing the biogas and replacing fossil fuel can result in up to a 93% reduction of the annual national waste greenhouse gas emissions of Spain and Italy.

  8. Colour and chemical changes of the lime wood surface due to CO2 laser thermal modification

    NASA Astrophysics Data System (ADS)

    Kubovský, Ivan; Kačík, František

    2014-12-01

    We studied colour and main wood components changes of lime wood caused by CO2 laser beam irradiation. The dry surface of lime wood (Tilia vulgaris L.) was irradiated with the CO2 laser beam (wavelength of 10.6 μm) at different exposures (expressed as the irradiation dose). Colour changes were monitored by the spectrophotometer, chemical changes were observed by the ATR-FTIR spectroscopy and carbohydrates were analysed by the HPLC method. With the growth of the irradiation dose (from 8.1 to 28.7 J cm-2) lightness (ΔL*) decrease and increase of the total colour difference (ΔE*) were observed. Higher values of the input energy lead to accelerating the mutual reaction of the functional groups resulting in the subsequent condensation of lignin. The total decrease in saccharides at the highest irradiation dose reaches 27.39% of the initial amount of saccharides in the reference sample. We have observed degradation and loss of hemicelluloses.

  9. Supercritical CO2 extract of Cinnamomum zeylanicum: chemical characterization and antityrosinase activity.

    PubMed

    Marongiu, Bruno; Piras, Alessandra; Porcedda, Silvia; Tuveri, Enrica; Sanjust, Enrico; Meli, Massimo; Sollai, Francesca; Zucca, Paolo; Rescigno, Antonio

    2007-11-28

    The volatile oil of the bark of Cinnamomum zeylanicum was extracted by means of supercritical CO2 fluid extraction in different conditions of pressure and temperature. Its chemical composition was characterized by GC-MS analysis. Nineteen compounds, which in the supercritical extract represented >95% of the oil, were identified. (E)-Cinnamaldehyde (77.1%), (E)-beta-caryophyllene (6.0%), alpha-terpineol (4.4%), and eugenol (3.0%) were found to be the major constituents. The SFE oil of cinnamon was screened for its biological activity about the formation of melanin in vitro. The extract showed antityrosinase activity and was able to reduce the formation of insoluble flakes of melanin from tyrosine. The oil also delayed the browning effect in apple homogenate. (E)-Cinnamaldehyde and eugenol were found to be mainly responsible of this inhibition effect.

  10. Solar-to-chemical and solar-to-fuel production from CO2 by metabolically engineered microorganisms.

    PubMed

    Woo, Han Min

    2017-01-11

    Recent development of carbon capture utilization (CCU) for reduction of greenhouse gas emission are reviewed. In the case of CO2 utilization, I describe development of solar-to-chemical and solar-to-fuel technology that refers to the use of solar energy to convert CO2 to desired chemicals and fuels. Photoautotrophic cyanobacterial platforms have been extensively developed on this principle, producing a diverse range of alcohols, organic acids, and isoprenoids directly from CO2. Recent breakthroughs in the metabolic engineering of cyanobacteria were reviewed. In addition, adoption of the light harvesting mechanisms from nature, photovoltaics-derived water splitting technologies have recently been integrated with microbial biotechnology to produce desired chemicals. Studies on the integration of electrode material with next-generation microbes are showcased for alternative solar-to-chemical and solar-to-fuel platforms.

  11. Chemical and anatomical changes in Liquidambar styraciflua L. xylem after long term exposure to elevated CO2

    DOE PAGES

    Kim, Keonhee; Labbé, Nicole; Warren, Jeffrey M.; ...

    2015-01-17

    The anatomical and chemical characteristics of sweetgum were studied after 11 years of elevated CO2 (544 ppm, ambient at 391 ppm) exposure. Anatomically, branch xylem cells were larger for elevated CO2 trees, and the cell wall thickness was thinner. Chemically, elevated CO2 exposure did not impact the structural components of the stem wood, but non-structural components were significantly affected. Principal component analysis (PCA) was employed to detect differences between the CO2 treatments by considering numerous structural and chemical variables, as well as tree size, and data from previously published sources (for example, root biomass, production and turnover). The PCA resultsmore » indicated a clear separation between trees exposed to ambient and elevated CO2 conditions. Lastly, correlation loadings plots of the PCA revealed that stem structural components, ash, Ca, Mg, total phenolics, root biomass, production and turnover were the major responses that contribute to the separation between the elevated and ambient CO2 treated trees.« less

  12. Analysis of anthropogenic CO2 signal in ICARTT using a regional chemical transport model and observed tracers

    NASA Astrophysics Data System (ADS)

    Campbell, J. E.; Carmichael, G. R.; Tang, Y.; Chai, T.; Vay, S. A.; Choi, Y.-H.; Sachse, G. W.; Singh, H. B.; Schnoor, J. L.; Woo, J.; Vukovich, J. M.; Streets, D. G.; Huey, L. G.; Stanier, C. O.

    2007-04-01

    Atmospheric CO2 inversion studies infer surface sources and sinks from observations and models. These studies usually require determination of the fossil fuel component of the observation, which can be estimated using anthropogenic tracers such as CO. The objective of this study is to demonstrate a new CO tracer method that accounts for overlapping forest fire and photochemical CO influences, and to quantify several aspects of the uncertainty in the CO tracer technique. Photochemistry model results and observations from the International Consortium for Atmospheric Research on Transport and Transformation experiment are used to quantify changes in the fossil fuel CO2 prediction from the CO tracer method with and without the inclusion of CO from biomass burning and photochemistry. Although the chemical sources and sinks tend to offset each other, there are regions where the chemical reactions change fossil fuel CO2 predictions by up to +/-4 ppm. Including biomass burning lowers fossil fuel CO2 by an average of 12 ppm in plumes heavily influenced by long-range transport of forest fire CO. An alternate fossil fuel CO2 calculation is done in a power plant plume using SO2 as a tracer, giving a change in 20 ppm from the CO method, indicative of uncertainty in the assumed CO:CO2 ratio.

  13. Effect of chemical environment and rock composition on fracture mechanics properties of reservoir lithologies in context of CO2 sequestration

    NASA Astrophysics Data System (ADS)

    Major, J. R.; Eichhubl, P.; Callahan, O. A.

    2015-12-01

    The coupled chemical and mechanical response of reservoir and seal rocks to injection of CO2 have major implications on the short and long term security of sequestered carbon. Many current numerical models evaluating behavior of reservoirs and seals during and after CO2 injection in the subsurface consider chemistry and mechanics separately and use only simple mechanical stability criteria while ignoring time-dependent failure parameters. CO2 injection irreversibly alters the subsurface chemical environment which can then affect geomechanical properties on a range of time scales by altering rock mineralogy and cements through dissolution, remobilization, and precipitation. It has also been documented that geomechanical parameters such as fracture toughness (KIC) and subcritical index (SCI) are sensitive to chemical environment. Double torsion fracture mechanics testing of reservoir lithologies under controlled environmental conditions relevant to CO2 sequestration show that chemical environment can measurably affect KIC and SCI. This coupled chemical-mechanical behavior is also influenced by rock composition, grains, amount and types of cement, and fabric. Fracture mechanics testing of the Aztec Sandstone, a largely silica-cemented, subarkose sandstone demonstrate it is less sensitive to chemical environment than Entrada Sandstone, a silty, clay-rich sandstone. The presence of de-ionized water lowers KIC by approximately 20% and SCI 30% in the Aztec Sandstone relative to tests performed in air, whereas the Entrada Sandstone shows reductions on the order of 70% and 90%, respectively. These results indicate that rock composition influences the chemical-mechanical response to deformation, and that the relative chemical reactivity of target reservoirs should be recognized in context of CO2 sequestration. In general, inert grains and cements such as quartz will be less sensitive to the changing subsurface environment than carbonates and clays.

  14. Metallosalen-Based Ionic Porous Polymers as Bifunctional Catalysts for the Conversion of CO2 into Valuable Chemicals.

    PubMed

    Luo, Rongchang; Chen, Yaju; He, Qian; Lin, Xiaowei; Xu, Qihang; He, Xiaohui; Zhang, Wuying; Zhou, Xiantai; Ji, Hongbing

    2016-12-31

    A series of new metallosalen-based ionic porous organic polymers (POPs) were synthesized for the first time using a simple unique strategy based on the free-radical copolymerization reaction. Various techniques were used to characterize the physicochemical properties of these catalysts. These well-designed materials endowed high surface area, hierarchical porous structures, and enhanced CO2 /N2 adsorptive selectivity. Moreover, these POPs having both metal centers (Lewis acid) and ionic units (nucleophile) could serve as bifunctional catalysts in the catalytic conversion of CO2 into high value-added chemicals without any additional co-catalyst under mild and solvent-free conditions, for example, CO2 /epoxides cycloaddition and Nformylation of amines from CO2 and hydrosilanes. The results demonstrated that the irregular porous structure was very favorable for the diffusion of substrates and products, and the microporous structural property resulted in the enrichment of CO2 near the catalytic centers in the CO2 -involved transformations. Additionally, the superhydrophobic property could not only enhance the chemoselectivity of products but also promote the stability and recyclability of catalysts.

  15. Effects of Steam and CO2 in the Fluidizing Gas when Using Bituminous Coal in Chemical-Looping Combustion

    NASA Astrophysics Data System (ADS)

    Leion, H.; Lyngfelt, A.; Mattisson, T.

    Chemical-looping combustion (CLC) is a combustion technology where an oxygen carrier is used to transfer oxygen from the combustion air to the fuel in order to avoid direct contact between air and fuel. Thus, the CO2 is inherently separated from the flue gases with a potential for considerably lower energy penalty and cost compared to other techniques for CO2 separation. The oxygen carrier is circulated between two reactors, a fuel and an air reactor, where the flue gas from the air reactor contains oxygen depleted air and the flue gas from the fuel reactor contains mainly CO2 and H2O. The water can easily be condensed and the remaining CO2 can be transported for underground storage. Most of the prior work with CLC has focused on using natural gas and syngas as fuel and oxygen carrying material normally produced from pure chemicals. However, recent work on adapting the CLC process for solid fuels with ores and natural minerals as oxygen carrier shows promising results. This paper will present results from reactivity investigations in a laboratory fluidized-bed reactor system using previously investigated natural mineral ilmenite as oxygen carrier and a bituminous Colombian coal as fuel. Experiments were conducted at a temperature of 970°C with N2, steam, and/or CO2 in the fluidizing gas. Synergy effects between steam and CO2 on fuel conversion was noted. The results show that the fuel conversion was a roughly a factor 5 faster with steam as compared to CO2 in the fluidizing gas.

  16. Calculating chemical equilibria in the heparin-Co2+ ion-glycine system

    NASA Astrophysics Data System (ADS)

    Feofanova, M. A.; Frantseva, Yu. V.; Zhuravlev, E. V.; Ryasensky, S. S.; Baranova, N. V.

    2013-08-01

    Results from investigating interactions in the heparin-Co2+ ion-glycine system are presented. The stoichiometry of cobalt complexes with heparin and glycine compositions CoOHHtpGly4- and CoHepGly3- is established.

  17. Experimental and Quantum Chemical Approaches to Develop Highly Selective Nanocatalysts for CO2 -free Power Circulation.

    PubMed

    Yamauchi, Miho; Ozawa, Nobuki; Kubo, Momoji

    2016-10-01

    Renewable electricity must be utilized to usefully suppress the atmospheric CO2 concentration and slow the progression of global warming. We have thus proposed a new concept involving CO2 -free electric power circulation systems via highly selective electrochemical reactions of alcohol/carboxylic acid redox couples. Design concepts for nanocatalysts able to catalyze highly selective electrochemical reactions are provided from both experimental and quantum mechanical perspectives.

  18. Development of a Method for Measuring Carbon Balance in Chemical Sequestration of CO2

    SciTech Connect

    Cheng, Zhongxian; Pan, Wei-Ping; Riley, John T.

    2006-09-09

    Anthropogenic CO2 released from fossil fuel combustion is a primary greenhouse gas which contributes to “global warming.” It is estimated that stationary power generation contributes over one-third of total CO2 emissions. Reducing CO2 in the atmosphere can be accomplished either by decreasing the rate at which CO2 is emitted into the atmosphere or by increasing the rate at which it is removed from it. Extensive research has been conducted on determining a fast and inexpensive method to sequester carbon dioxide. These methods can be classified into two categories, CO2 fixation by natural sink process for CO2, or direct CO2 sequestration by artificial processes. In direct sequestration, CO2 produced from sources such as coal-fired power plants, would be captured from the exhausted gases. CO2 from a combustion exhaust gas is absorbed with an aqueous ammonia solution through scrubbing. The captured CO2 is then used to synthesize ammonium bicarbonate (ABC or NH4HCO3), an economical source of nitrogen fertilizer. In this work, we studied the carbon distribution after fertilizer is synthesized from CO2. The synthesized fertilizer in laboratory is used as a “CO2 carrier” to “transport” CO2 from the atmosphere to crops. After biological assimilation and metabolism in crops treated with ABC, a considerable amount of the carbon source is absorbed by the plants with increased biomass production. The majority of the unused carbon source percolates into the soil as carbonates, such as calcium carbonate (CaCO3) and magnesium carbonate (MgCO3). These carbonates are environmentally benign. As insoluble salts, they are found in normal rocks and can be stored safely and permanently in soil. This investigation mainly focuses on the carbon distribution after the synthesized fertilizer is applied to soil. Quantitative examination of carbon distribution in an ecosystem is a challenging task since the carbon in the soil may come from various sources. Therefore synthesized 14C

  19. Chemical-mechanical coupling observed for depleted oil reservoirs subjected to long-term CO2-exposure - A case study of the Werkendam natural CO2 analogue field

    NASA Astrophysics Data System (ADS)

    Hangx, Suzanne; Bakker, Elisenda; Bertier, Pieter; Nover, Georg; Busch, Andreas

    2015-10-01

    Geological storage of CO2 is one of the most promising technologies to rapidly reduce anthropogenic emissions of carbon dioxide. In order to ensure storage integrity, it is important to understand the effect of long-term CO2/brine/rock interactions on the mechanical behaviour of a storage complex. As most of these reactions are too slow to reproduce on laboratory timescales, we studied a natural CO2 analogue reservoir (the Röt Fringe Sandstone, Werkendam field, the Netherlands; 125-135 Ma of CO2-exposure) and its unreacted counterpart. We focused on CO2-induced mineralogical and porosity-permeability changes, and their effect on mechanical behaviour of both intact rock and simulated fault gouge. Overall, CO2-exposure did not lead to drastic mineralogical changes. The CO2-exposed material shows a stronger dependence of permeability on porosity, which is attributed to differences in diagenesis (closed-system diagenesis and hydrocarbon emplacement) taking place before CO2 charging. The limited extent of reaction was in part the result of bitumen coatings protecting specific mineral phases from reaction. In local, mm-sized zones displaying significant anhydrite cement dissolution, enhanced porosity was observed. For most of the reservoir the long-term mechanical behaviour after CO2-exposure could be described by the behaviour of the unreacted sandstone, while these more 'porous' zones had a lower rock strength. In addition, CO2-exposure did not affect the fault friction behaviour, and slip is expected to result in stable sliding. Simple stress path calculations predict that reservoir failure due to depletion and injection is unlikely, even for the 'porous' zones, nor will fault reactivation occur for realistic injection scenarios.

  20. Robust C–C bonded porous networks with chemically designed functionalities for improved CO2 capture from flue gas

    PubMed Central

    Thirion, Damien; Lee, Joo S; Özdemir, Ercan

    2016-01-01

    Effective carbon dioxide (CO2) capture requires solid, porous sorbents with chemically and thermally stable frameworks. Herein, we report two new carbon–carbon bonded porous networks that were synthesized through metal-free Knoevenagel nitrile–aldol condensation, namely the covalent organic polymer, COP-156 and 157. COP-156, due to high specific surface area (650 m2/g) and easily interchangeable nitrile groups, was modified post-synthetically into free amine- or amidoxime-containing networks. The modified COP-156-amine showed fast and increased CO2 uptake under simulated moist flue gas conditions compared to the starting network and usual industrial CO2 solvents, reaching up to 7.8 wt % uptake at 40 °C. PMID:28144294

  1. Robust C-C bonded porous networks with chemically designed functionalities for improved CO2 capture from flue gas.

    PubMed

    Thirion, Damien; Lee, Joo S; Özdemir, Ercan; Yavuz, Cafer T

    2016-01-01

    Effective carbon dioxide (CO2) capture requires solid, porous sorbents with chemically and thermally stable frameworks. Herein, we report two new carbon-carbon bonded porous networks that were synthesized through metal-free Knoevenagel nitrile-aldol condensation, namely the covalent organic polymer, COP-156 and 157. COP-156, due to high specific surface area (650 m(2)/g) and easily interchangeable nitrile groups, was modified post-synthetically into free amine- or amidoxime-containing networks. The modified COP-156-amine showed fast and increased CO2 uptake under simulated moist flue gas conditions compared to the starting network and usual industrial CO2 solvents, reaching up to 7.8 wt % uptake at 40 °C.

  2. The Idaho Chemical Processing Plant Product Denitrator Upgrade

    SciTech Connect

    N /A

    1982-05-01

    The upgrade and redesign of a fluidized-bed denitrator for production of uranium trioxide from uranyl nitrate solution is discussed. The success of the project in improving process efficiency and personnel safety is also addressed based on subsequent operation.

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

    PubMed Central

    2014-01-01

    Natural mineral carbonation can be accelerated using acid and alkali solutions to enhance atmospheric CO2 sequestration, but the production of these solutions needs to be carbon-neutral. A microbial reverse-electrodialysis electrolysis and chemical-production cell (MRECC) was developed to produce these solutions and H2 gas using only renewable energy sources (organic matter and salinity gradient). Using acetate (0.82 g/L) as a fuel for microorganisms to generate electricity in the anode chamber (liquid volume of 28 mL), 0.45 mmol of acid and 1.09 mmol of alkali were produced at production efficiencies of 35% and 86%, respectively, along with 10 mL of H2 gas. Serpentine dissolution was enhanced 17–87-fold using the acid solution, with approximately 9 mL of CO2 absorbed and 4 mg of CO2 fixed as magnesium or calcium carbonates. The operational costs, based on mineral digging and grinding, and water pumping, were estimated to be only $25/metric ton of CO2 fixed as insoluble carbonates. Considering the additional economic benefits of H2 generation and possible wastewater treatment, this method may be a cost-effective and environmentally friendly method for CO2 sequestration. PMID:24741666

  4. High temperature chemical kinetic study of the H2-CO-CO2-NO reaction system

    NASA Technical Reports Server (NTRS)

    Jachimowski, C. J.

    1975-01-01

    An experimental study of the kinetics of the H2-CO-CO2-NO reaction system was made behind incident shock waves at temperatures of 2460 and 2950 K. The overall rate of the reaction was measured by monitoring radiation from the CO + O yields CO2 + h upoilon reaction. Correlation of these data with a detailed reaction mechanism showed that the high-temperature rate of the reaction N + OH yields NO + H can be described by the low-temperature (320 K) rate coefficient. Catalytic dissociation of molecular hydrogen was an important reaction under the tests conditions.

  5. A Review of Hazardous Chemical Species Associated with CO2 Capturefrom Coal-Fired Power Plants and Their Potential Fate in CO2 GeologicStorage

    SciTech Connect

    Apps, J.A.

    2006-02-23

    Conventional coal-burning power plants are major contributors of excess CO2 to the atmospheric inventory. Because such plants are stationary, they are particularly amenable to CO2 capture and disposal by deep injection into confined geologic formations. However, the energy penalty for CO2 separation and compression is steep, and could lead to a 30-40 percent reduction in useable power output. Integrated gas combined cycle (IGCC) plants are thermodynamically more efficient, i.e.,produce less CO2 for a given power output, and are more suitable for CO2 capture. Therefore, if CO2 capture and deep subsurface disposal were to be considered seriously, the preferred approach would be to build replacement IGCC plants with integrated CO2 capture, rather than retrofit existing conventional plants. Coal contains minor quantities of sulfur and nitrogen compounds, which are of concern, as their release into the atmosphere leads to the formation of urban ozone and acid rain, the destruction of stratospheric ozone, and global warming. Coal also contains many trace elements that are potentially hazardous to human health and the environment. During CO2 separation and capture, these constituents could inadvertently contaminate the separated CO2 and be co-injected. The concentrations and speciation of the co-injected contaminants would differ markedly, depending on whether CO2 is captured during the operation of a conventional or an IGCC plant, and the specific nature of the plant design and CO2 separation technology. However, regardless of plant design or separation procedures, most of the hazardous constituents effectively partition into the solid waste residue. This would lead to an approximately two order of magnitude reduction in contaminant concentration compared with that present in the coal. Potential exceptions are Hg in conventional plants, and Hg and possibly Cd, Mo and Pb in IGCC plants. CO2 capture and injection disposal could afford an opportunity to deliberately capture

  6. Dual roles of CO2*- for degrading synthetic organic chemicals in the photo/ferrioxalate system.

    PubMed

    Jeong, Joonseon; Yoon, Jeyong

    2004-09-01

    In this study, the relative importance of the dual reaction pathways of CO2*- in the photo/ferrioxalate system, where it acts both as a reductant for reducing the ferric ion and as an agent for the formation of H(2)O(2), was investigated as a function of the concentrations of ferrioxalate and oxygen. We studied the two competitive reactions of CO2*- in the photo/ferrioxalate system, which depend on the relative concentrations of ferrioxalate to oxygen, with the degradation of 2,4-dichlorophenoxyacetic acid (2,4-D), which was used as a target pollutant. At high concentrations of ferrioxalate, almost all of the CO2*- reacted with ferrioxalate to reduce Fe(III) to Fe(II), whereas at low concentrations of ferrioxalate, a majority of the CO2*- contributed to the formation of H(2)O(2), as a result of its reaction with oxygen, which allows the Fenton reaction to occur without any external supply of H(2)O(2).

  7. Fate of injected CO2 in the Wilcox Group, Louisiana, Gulf Coast Basin: Chemical and isotopic tracers of microbial-brine-rock-CO2 interactions

    USGS Publications Warehouse

    Shelton, Jenna L.; McIntosh, Jennifer C.; Warwick, Peter D.; Lee Zhi Yi, Amelia

    2016-01-01

    The “2800’ sandstone” of the Olla oil field is an oil and gas-producing reservoir in a coal-bearing interval of the Paleocene–Eocene Wilcox Group in north-central Louisiana, USA. In the 1980s, this producing unit was flooded with CO2 in an enhanced oil recovery (EOR) project, leaving ∼30% of the injected CO2 in the 2800’ sandstone post-injection. This study utilizes isotopic and geochemical tracers from co-produced natural gas, oil and brine to determine the fate of the injected CO2, including the possibility of enhanced microbial conversion of CO2 to CH4 via methanogenesis. Stable carbon isotopes of CO2, CH4 and DIC, together with mol% CO2 show that 4 out of 17 wells sampled in the 2800’ sandstone are still producing injected CO2. The dominant fate of the injected CO2appears to be dissolution in formation fluids and gas-phase trapping. There is some isotopic and geochemical evidence for enhanced microbial methanogenesis in 2 samples; however, the CO2 spread unevenly throughout the reservoir, and thus cannot explain the elevated indicators for methanogenesis observed across the entire field. Vertical migration out of the target 2800’ sandstone reservoir is also apparent in 3 samples located stratigraphically above the target sand. Reservoirs comparable to the 2800’ sandstone, located along a 90-km transect, were also sampled to investigate regional trends in gas composition, brine chemistry and microbial activity. Microbial methane, likely sourced from biodegradation of organic substrates within the formation, was found in all oil fields sampled, while indicators of methanogenesis (e.g. high alkalinity, δ13C-CO2 and δ13C-DIC values) and oxidation of propane were greatest in the Olla Field, likely due to its more ideal environmental conditions (i.e. suitable range of pH, temperature, salinity, sulfate and iron concentrations).

  8. The effect of increased atmospheric temperature and CO2 concentration during crop growth on the chemical composition and in vitro rumen fermentation characteristics of wheat straw.

    PubMed

    He, Xiangyu; Wu, Yanping; Cai, Min; Mu, Chunlong; Luo, Weihong; Cheng, Yanfen; Zhu, Weiyun

    2015-01-01

    This experiment was conducted to investigate the effects of increased atmospheric temperature and CO2 concentration during crop growth on the chemical composition and in vitro rumen fermentation characteristics of wheat straw. The field experiment was carried out from November 2012 to June 2013 at Changshu (31°32'93″N, 120°41'88″E) agro-ecological experimental station. A total of three treatments were set. The concentration of CO2 was increased to 500 μmol/mol in the first treatment (CO2 group). The temperature was increased by 2 °C in the second treatment (TEM group) and the concentration of CO2 and temperature were both increased in the third treatment (CO2 + TEM group). The mean temperature and concentration of CO2 in control group were 10.5 °C and 413 μmol/mol. At harvesting, the wheat straws were collected and analyzed for chemical composition and in vitro digestibility. Results showed that dry matter was significantly increased in all three treatments. Ether extracts and neutral detergent fiber were significantly increased in TEM and CO2 + TEM groups. Crude protein was significantly decreased in CO2 + TEM group. In vitro digestibility analysis of wheat straw revealed that gas production was significantly decreased in CO2 and CO2 + TEM groups. Methane production was significantly decreased in TEM and CO2 + TEM groups. Ammonia nitrogen and microbial crude protein were significantly decreased in all three treatments. Total volatile fatty acids were significantly decreased in CO2 and CO2 + TEM groups. In conclusion, the chemical composition of the wheat straw was affected by temperature and CO2 and the in vitro digestibility of wheat straw was reduced, especially in the combined treatment of temperature and CO2.

  9. Chemical weathering and long-term CO2 consumption in the Ayeyarwady and Mekong river basins in the Himalayas

    NASA Astrophysics Data System (ADS)

    Manaka, Takuya; Otani, Souya; Inamura, Akihiko; Suzuki, Atsushi; Aung, Thura; Roachanakanan, Raywadee; Ishiwa, Takeshige; Kawahata, Hodaka

    2015-06-01

    The role of terrestrial river systems in the global carbon cycle on a long timescale has been a subject of interest, especially in the context of past climate changes such as the global cooling in the Cenozoic. The discharges of water and carbon into the ocean from the Himalayan watersheds are among the highest in the world. However, there are few reliable geochemical data from the Ayeyarwady River. This study focused on reevaluating chemical weathering in the Himalayan watersheds based on samples taken from the Ayeyarwady, Mekong, and Chao Phraya Rivers and on chemical analysis of the composition of dissolved substances in these rivers. Comparisons of water quality showed that, unlike in previous studies, the total alkalinity budgets of the Ayeyarwady are dominated by carbonate rather than silicate weathering. Long-term CO2 consumption by silicate weathering in the Ayeyarwady is estimated to be only 63-145 × 109 mol yr-1, which is only 10% of the previous estimate. Our results also suggest that the total Himalayan watersheds account for only about 10% of the total global CO2 consumption by silicate weathering. Although we need further studies, chemical weathering and associated CO2 uptake in the Himalayas likely played a lesser role in long-term global cooling in the past than previously appreciated.

  10. A Lumped, Macroscopic Approach to Modeling Soil Moisture, CO2 Transport, and Chemical Weathering in the Critical Zone

    NASA Astrophysics Data System (ADS)

    Porporato, A. M.; Parolari, A.

    2015-12-01

    Ecohydrological processes in the root zone act as a dynamic interface between the atmosphere and the deeper soil layers, modulating the conditions that drive chemical weathering along the soil profile. Among these processes, soil moisture dynamics respond to intermittent rainfall pulses and to runoff and evapotranspiration losses. In addition, carbon dioxide (CO2) and its associated acidity are introduced into the soil moisture via root and microbial respiration. The coupling of soil moisture and CO2 dynamics in the root zone acts as an important controller of the critical zone development through the chemical weathering and water chemistry exported through runoff and percolation. Due to spatial and temporal variability and non-linearity, modeling these coupled root zone soil moisture and CO2 dynamics presents a number of challenges. In this talk, a lumped, macroscopic approach to modeling soil moisture, CO2 transport, and chemical weathering in the critical zone is introduced. The model considers a homogeneous soil column, therefore simplifying known spatial heterogeneities, and focuses on temporal variability resulting from non-linear processes and stochastic rainfall forcing. First, at short time-scales, the deterministic temporal evolution of soil moisture, dissolved inorganic carbon, pH, and alkalinity is analyzed using a dynamical system approach. Second, at longer inter-annual time-scales where rainfall stochasticity becomes an important driver of the system behavior, the system is analyzed probabilistically and its average behavior described using a novel macroscopic approach. This averaging of the nonlinear stochastic dynamics results in a closure problem that is addressed through a first-order approximation of non-linear fluxes, including the correlation between soil moisture and solutes. The model provides a method to assess how changes in external forcing or system properties propagate into and alter critical zone structure and function, and to isolate

  11. Biosynthesis of platform chemical 3-hydroxypropionic acid (3-HP) directly from CO2 in cyanobacterium Synechocystis sp. PCC 6803.

    PubMed

    Wang, Yunpeng; Sun, Tao; Gao, Xingyan; Shi, Mengliang; Wu, Lina; Chen, Lei; Zhang, Weiwen

    2016-03-01

    3-hydroxypropionic acid (3-HP) is an important platform chemical with a wide range of applications. So far large-scale production of 3-HP has been mainly through petroleum-based chemical processes, whose sustainability and environmental issues have attracted widespread attention. With the ability to fix CO2 directly, cyanobacteria have been engineered as an autotrophic microbial cell factory to produce fuels and chemicals. In this study, we constructed the biosynthetic pathway of 3-HP in cyanobacterium Synechocystis sp. PCC 6803, and then optimized the system through the following approaches: i) increasing expression of malonyl-CoA reductase (MCR) gene using different promoters and cultivation conditions; ii) enhancing supply of the precursor malonyl-CoA by overexpressing acetyl-CoA carboxylase and biotinilase; iii) improving NADPH supply by overexpressing the NAD(P) transhydrogenase gene; iv) directing more carbon flux into 3-HP by inactivating the competing pathways of PHA and acetate biosynthesis. Together, the efforts led to a production of 837.18 mg L(-1) (348.8 mg/g dry cell weight) 3-HP directly from CO2 in Synechocystis after 6 days cultivation, demonstrating the feasibility photosynthetic production of 3-HP directly from sunlight and CO2 in cyanobacteria. In addition, the results showed that overexpression of the ribulose-1, 5-bisphosphate carboxylase/oxygenase (Rubisco) gene from Anabaena sp. PCC 7120 and Synechococcus sp. PCC 7942 led to no increase of 3-HP production, suggesting CO2 fixation may not be a rate-limiting step for 3-HP biosynthesis in Synechocystis.

  12. Subcritical crack growth in a chemically reactive environment-implications for caprock integrity for CO2 storage

    NASA Astrophysics Data System (ADS)

    Fan, Z.; Eichhubl, P.; Callahan, O. A.; Major, J. R.; Chen, X.

    2015-12-01

    Seal integrity of cap-rock is a critical constraint on the long term performance of CO2 containment site. During fluid migration, the coupled geochemical reaction of minerals and geomechanical deformation of rock matrix may affect the seal integrity. The potential leakage of injected CO2 from cap-rock through preexisting fractures/faults represents a major concern associated with geological storage of CO2. To address the fundamental question of CO2 leakage through subcritical growth of fractures driven by chemically reactive fluid across caprocks, we build a Dugdale cohesive model. Ahead of the physical crack tip, a narrow band of cohesive zone is assumed to exist with the upper and lower cohesive surfaces held by the cohesive traction. In the vicinity of the crack tip, minerals dissolve due to the acidic environment and migrate from the physical crack tip into the cohesive zone causing damage of rock matrix in the form of a reduction of cohesive traction.Focusing on the dissolution of calcite and following the stress corrosion theory, we assume the degradation of cohesive traction is linearly proportional to the concentration of Ca2+whose evolution follows the reactive diffusion equation. Using a critical crack opening displacement criterion, the subcritical propagation behavior of crack due to stress corrosion is captured and the rate-limiting effects including the chemical reactions to produce the Ca2+ and the transport of minerals along the newly generated fracture cohesive zone are incorporated. Subcritical crack growth rate under different chemical environment conditions is examined and compared with the experimental fracture mechanics testing.

  13. CHEMICAL FIXATION OF CO2 IN COAL COMBUSTION PRODUCTS AND RECYCLING THROUGH BIOSYSTEMS

    SciTech Connect

    C. Henry Copeland; Paul Pier; Samantha Whitehead; Paul Enlow; Richard Strickland; David Behel

    2003-12-15

    This Annual Technical Progress Report presents the principle results in enhanced growth of algae using coal combustion products as a catalyst to increase bicarbonate levels in solution. A co-current reactor is present that increases the gas phase to bicarbonate transfer rate by a factor of five to nine. The bicarbonate concentration at a given pH is approximately double that obtained using a control column of similar construction. Algae growth experiments were performed under laboratory conditions to obtain baseline production rates and to perfect experimental methods. The final product of this initial phase in algae production is presented. Algal growth can be limited by several factors, including the level of bicarbonate available for photosynthesis, the pH of the growth solution, nutrient levels, and the size of the cell population, which determines the available space for additional growth. In order to supply additional CO2 to increase photosynthesis and algal biomass production, fly ash reactor has been demonstrated to increase the available CO2 in solution above the limits that are achievable with dissolved gas alone. The amount of dissolved CO2 can be used to control pH for optimum growth. Periodic harvesting of algae can be used to maintain algae in the exponential, rapid growth phase. An 800 liter scale up demonstrated that larger scale production is possible. The larger experiment demonstrated that indirect addition of CO2 is feasible and produces significantly less stress on the algal system. With better harvesting methods, nutrient management, and carbon dioxide management, an annual biomass harvest of about 9,000 metric tons per square kilometer (36 MT per acre) appears to be feasible. To sequester carbon, the algal biomass needs to be placed in a permanent location. If drying is undesirable, the biomass will eventually begin to aerobically decompose. It was demonstrated that algal biomass is a suitable feed to an anaerobic digester to produce methane

  14. Crystal engineering of an nbo topology metal-organic framework for chemical fixation of CO2 under ambient conditions.

    PubMed

    Gao, Wen-Yang; Chen, Yao; Niu, Youhong; Williams, Kia; Cash, Lindsay; Perez, Pastor J; Wojtas, Lukasz; Cai, Jianfeng; Chen, Yu-Sheng; Ma, Shengqian

    2014-03-03

    Crystal engineering of the nbo metal-organic framework (MOF) platform MOF-505 with a custom-designed azamacrocycle ligand (1,4,7,10-tetrazazcyclododecane-N,N',N'',N'''-tetra-p-methylbenzoic acid) leads to a high density of well-oriented Lewis active sites within the cuboctahedral cage in MMCF-2, [Cu2(Cu-tactmb)(H2O)3(NO3)2]. This MOF demonstrates high catalytic activity for the chemical fixation of CO2 into cyclic carbonates at room temperature under 1 atm pressure.

  15. Real-time measurements of chemical and isotope composition of atmospheric and volcanic CO2 at Mt. Etna (Italy)

    NASA Astrophysics Data System (ADS)

    Rizzo, Andrea L.; Jost, Hans-Jürg; Caracausi, Antonio; Paonita, Antonio; Liotta, Marcello; Martelli, Mauro

    2014-05-01

    We present unprecedented data of real-time measurements of chemical and isotope (δ13C) composition of CO2 in air and in fumarolic-plume gases collected at Mt. Etna volcano. Two campaigns of measurements were performed on 11 July and on 5-6 September 2013, by using a Delta Ray tunable diode laser. With the assumption of a two components mixing, a simple linear regression was applied to the data in order to obtain the volcanogenic δ13C. Data acquired along the route Catania-Etna, while car was moving, showed an excess of 13C-depleted CO2 when passing through inhabited centers due to atmospheric pollution produced by the cars exhaust. Fumaroles of Torre del Filosofo (2,900 m a.s.l.) displayed a δ13C between -3.2±0.03o and -3.7±0.05o comparable to IRMS measurements of discrete samples collected in the same date and in previous investigations. Diluted plume gases were collected at more than 1 km from the craters and showed δ13C=-2.2±0.2o accordingly with collected crater fumaroles. Considering the huge amount of data that may be acquired in a very short time by Delta Ray, we demonstrate that the addition to the atmospheric CO2 content of ~100 ppm of CO2 from an unknown source is enough to allow a mathematical calculation of the end-member with an uncertainty generally < 0.15‰This is feasible with the assumption of a binary mixing. We thus infer that the application performed at Mt. Etna may represent an historical step forward for the scientific community in volcanic surveillance.

  16. Highly Efficient Oxygen-Storage Material with Intrinsic Coke Resistance for Chemical Looping Combustion-Based CO2 Capture.

    PubMed

    Imtiaz, Qasim; Kurlov, Alexey; Rupp, Jennifer Lilia Marguerite; Müller, Christoph Rüdiger

    2015-06-22

    Chemical looping combustion (CLC) and chemical looping with oxygen uncoupling (CLOU) are emerging thermochemical CO2 capture cycles that allow the capture of CO2 with a small energy penalty. Here, the development of suitable oxygen carrier materials is a key aspect to transfer these promising concepts to practical installations. CuO is an attractive material for CLC and CLOU because of its high oxygen-storage capacity (20 wt %), fast reaction kinetics, and high equilibrium partial pressure of oxygen at typical operating temperatures (850-1000 °C). However, despite its promising characteristics, its low Tammann temperature requires the development of new strategies to phase-stabilize CuO-based oxygen carriers. In this work, we report a strategy based on stabilization by co-precipitated ceria (CeO2-x ), which allowed us to increase the oxygen capacity, coke resistance, and redox stability of CuO-based oxygen carriers substantially. The performance of the new oxygen carriers was evaluated in detail and compared to the current state-of-the-art materials, that is, Al2 O3 -stabilized CuO with similar CuO loadings. We also demonstrate that the higher intrinsic oxygen uptake, release, and mobility in CeO2-x -stabilized CuO leads to a three times higher carbon deposition resistance compared to that of Al2 O3 -stabilized CuO. Moreover, we report a high cyclic stability without phase intermixing for CeO2-x -supported CuO. This was accompanied by a lower reduction temperature compared to state-of-the-art Al2 O3 -supported CuO. As a result of its high resistance towards carbon deposition and fast oxygen uncoupling kinetics, CeO2-x -stabilized CuO is identified as a very promising material for CLC- and CLOU-based CO2 capture architectures.

  17. Chemical Reaction CO+OH(•) → CO2+H(•) Autocatalyzed by Carbon Dioxide: Quantum Chemical Study of the Potential Energy Surfaces.

    PubMed

    Masunov, Artëm E; Wait, Elizabeth; Vasu, Subith S

    2016-08-04

    The supercritical carbon dioxide medium, used to increase efficiency in oxy combustion fossil energy technology, may drastically alter both rates and mechanisms of chemical reactions. Here we investigate potential energy surface of the second most important combustion reaction with quantum chemistry methods. Two types of effects are reported: formation of the covalent intermediates and formation of van der Waals complexes by spectator CO2 molecule. While spectator molecule alter the activation barrier only slightly, the covalent bonding opens a new reaction pathway. The mechanism includes sequential covalent binding of CO2 to OH radical and CO molecule, hydrogen transfer from oxygen to carbon atoms, and CH bond dissociation. This reduces the activation barrier by 11 kcal/mol at the rate-determining step and is expected to accelerate the reaction rate. The finding of predicted catalytic effect is expected to play an important role not only in combustion but also in a broad array of chemical processes taking place in supercritical CO2 medium. It may open a new venue for controlling reaction rates for chemical manufacturing.

  18. Chemical reaction CO+OH • → CO2+H• autocatalyzed by carbon dioxide: Quantum chemical study of the potential energy surfaces

    DOE PAGES

    Masunov, Artem E.; Wait, Elizabeth; Vasu, Subith S.

    2016-06-28

    The supercritical carbon dioxide medium, used to increase efficiency in oxy combustion fossil energy technology, may drastically alter both rates and mechanisms of chemical reactions. Here we investigate potential energy surface of the second most important combustion reaction with quantum chemistry methods. Two types of effects are reported: formation of the covalent intermediates and formation of van der Waals complexes by spectator CO2 molecule. While spectator molecule alter the activation barrier only slightly, the covalent bonding opens a new reaction pathway. The mechanism includes sequential covalent binding of CO2 to OH radical and CO molecule, hydrogen transfer from oxygen tomore » carbon atoms, and CH bond dissociation. This reduces the activation barrier by 11 kcal/mol at the rate-determining step and is expected to accelerate the reaction rate. The finding of predicted catalytic effect is expected to play an important role not only in combustion but also in a broad array of chemical processes taking place in supercritical CO2 medium. Furthermore, tt may open a new venue for controlling reaction rates for chemical manufacturing.« less

  19. The contribution of changes in P release and CO2 consumption by chemical weathering to the historical trend in land carbon uptake

    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.

  20. The contribution of changes in P release and CO2 consumption by chemical weathering to the historical trend in land carbon uptake

    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.

  1. Long-term operation of microbial electrosynthesis cell reducing CO2 to multi-carbon chemicals with a mixed culture avoiding methanogenesis.

    PubMed

    Bajracharya, Suman; Yuliasni, Rustiana; Vanbroekhoven, Karolien; Buisman, Cees J N; Strik, David P B T B; Pant, Deepak

    2017-02-01

    In microbial electrosynthesis (MES), CO2 can be reduced preferably to multi-carbon chemicals by a biocathode-based process which uses electrochemically active bacteria as catalysts. A mixed anaerobic consortium from biological origin typically produces methane from CO2 reduction which circumvents production of multi-carbon compounds. This study aimed to develop a stable and robust CO2 reducing biocathode from a mixed culture inoculum avoiding the methane generation. An effective approach was demonstrated based on (i) an enrichment procedure involving inoculum pre-treatment and several culture transfers in H2:CO2 media, (ii) a transfer from heterotrophic to autotrophic growth and (iii) a sequential batch operation. Biomass growth and gradual acclimation to CO2 electro-reduction accomplished a maximum acetate production rate of 400mgLcatholyte(-1)d(-1) at -1V (vs. Ag/AgCl). Methane was never detected in more than 300days of operation. Accumulation of acetate up to 7-10gL(-1) was repeatedly attained by supplying (80:20) CO2:N2 mixture at -0.9 to -1V (vs. Ag/AgCl). In addition, ethanol and butyrate were also produced from CO2 reduction. Thus, a robust CO2 reducing biocathode can be developed from a mixed culture avoiding methane generation by adopting the specific culture enrichment and operation procedures without the direct addition of chemical inhibitor.

  2. Copper-manganese mixed oxides: CO2-selectivity, stable, and cyclic performance for chemical looping combustion of methane.

    PubMed

    Mungse, Pallavi; Saravanan, Govindachetty; Uchiyama, Tomoki; Nishibori, Maiko; Teraoka, Yasutake; Rayalu, Sadhana; Labhsetwar, Nitin

    2014-09-28

    Chemical looping combustion (CLC) is a key technology for oxy-fuel combustion with inherent separation of CO2 from a flue gas, in which oxygen is derived from a solid oxygen carrier. Multi-cycle CLC performance and the product selectivity towards CO2 formation were achieved using mixed oxide of Cu and Mn (CuMn2O4) (Fd3[combining macron]m, a = b = c = 0.83 nm) as an oxygen carrier. CuMn2O4 was prepared by the co-precipitation method followed by annealing at 900 °C using copper(II) nitrate trihydrate and manganese(II) nitrate tetrahydrate as metal precursors. CuMn2O4 showed oxygen-desorption as well as reducibility at elevated temperatures under CLC conditions. The lattice of CuMn2O4 was altered significantly at higher temperature, however, it was reinstated virtually upon cooling in the presence of air. CuMn2O4 was reduced to CuMnO2, Mn3O4, and Cu2O phases at the intermediate stages, which were further reduced to metallic Cu and MnO upon the removal of reactive oxygen from their lattice. CuMn2O4 showed a remarkable activity towards methane combustion reaction at 750 °C. The reduced phase of CuMn2O4 containing Cu and MnO was readily reinstated when treated with air or oxygen at 750 °C, confirming efficient regeneration of the oxygen carrier. Neither methane combustion efficiency nor oxygen carrying capacity was altered with the increase of CLC cycles at any tested time. The average oxygen carrying capacity of CuMn2O4 was estimated to be 114 mg g(-1), which was not altered significantly with the repeated CLC cycles. Pure CO2 but no CO, which is one of the possible toxic by-products, was formed solely upon methane combustion reaction of CuMn2O4. CuMn2O4 shows potential as a practical CLC material both in terms of multi-cycle performance and product selectivity towards CO2 formation.

  3. Production of chemicals from C1 gases (CO, CO2) by Clostridium carboxidivorans.

    PubMed

    Fernández-Naveira, Ánxela; Abubackar, Haris Nalakath; Veiga, María C; Kennes, Christian

    2017-03-01

    Bioprocesses in conventional second generation biorefineries are mainly based on the fermentation of sugars obtained from lignocellulosic biomass or agro-industrial wastes. An alternative to this process consists in gasifying those same feedstocks or even other carbon-containing materials to obtain syngas which can also be fermented by some anaerobic bacteria to produce chemicals or fuels. Carbon monoxide, carbon dioxide and hydrogen, which are the main components of syngas, are also found in some industrial waste gases, among others in steel industries. Clostridium carboxidivorans is able to metabolise such gases to produce ethanol and higher alcohols, i.e. butanol and hexanol, following the Wood-Ljungdahl pathway. This does simultaneously allow the removal of volatile pollutants involved in climate change. The bioconversion is a two step process in which organic acids (acetate, butyrate, hexanoate) are produced first, followed by the accumulation of alcohols; although partial overlap in time of acids and alcohols production may sometimes take place as well. Several parameters, among others pH, temperature, or gas-feed flow rates in bioreactors, affect the bioconversion process. Besides, the accumulation of high concentrations of alcohols in the fermentation broth inhibits the growth and metabolic activity of C. carboxidivorans.

  4. Direct PEM fuel cell using "organic chemical hydrides" with zero-CO2 emission and low-crossover.

    PubMed

    Kariya, Nobuko; Fukuoka, Atsushi; Ichikawa, Masaru

    2006-04-14

    A series of "organic chemical hydrides" such as cyclohexane, methylcyclohexane, cyclohexene, 2-propanol, and cyclohexanol were applied to the direct PEM fuel cell. High performances of the PEM fuel cell were achieved by using cyclohexane (OCV = 920 mV, PD(max) = 15 mW cm(-2)) and 2-propanol (OCV = 790 mV, PD(max) = 78 mW cm(-2)) as fuels without CO(2) emissions. The rates of fuel crossover for cyclohexane, 2-propanol, and methanol were estimated, and the rates of fuel permeation of cyclohexane and 2-propanol were lower than that of methanol. Water electrolysis and electro-reductive hydrogenation of acetone mediated by PEM were carried out and formation of 2-propanol in cathode side was observed. This system is the first example of a "rechargeable" direct fuel cell.

  5. Novel process and catalytic materials for converting CO2 and H2 containing mixtures to liquid fuels and chemicals.

    PubMed

    Meiri, Nora; Dinburg, Yakov; Amoyal, Meital; Koukouliev, Viatcheslav; Nehemya, Roxana Vidruk; Landau, Miron V; Herskowitz, Moti

    2015-01-01

    Carbon dioxide and water are renewable and the most abundant feedstocks for the production of chemicals and fungible fuels. However, the current technologies for production of hydrogen from water are not competitive. Therefore, reacting carbon dioxide with hydrogen is not economically viable in the near future. Other alternatives include natural gas, biogas or biomass for the production of carbon dioxide, hydrogen and carbon monoxide mixtures that react to yield chemicals and fungible fuels. The latter process requires a high performance catalyst that enhances the reverse water-gas-shift (RWGS) reaction and Fischer-Tropsch synthesis (FTS) to higher hydrocarbons combined with an optimal reactor system. Important aspects of a novel catalyst, based on a Fe spinel and three-reactor system developed for this purpose published in our recent paper and patent, were investigated in this study. Potassium was found to be a key promoter that improves the reaction rates of the RWGS and FTS and increases the selectivity of higher hydrocarbons while producing mostly olefins. It changed the texture of the catalyst, stabilized the Fe-Al-O spinel, thus preventing decomposition into Fe3O4 and Al2O3. Potassium also increased the content of Fe5C2 while shifting Fe in the oxide and carbide phases to a more reduced state. In addition, it increased the relative exposure of carbide iron on the catalysts surface, the CO2 adsorption and the adsorption strength. A detailed kinetic model of the RWGS, FTS and methanation reactions was developed for the Fe spinel catalyst based on extensive experimental data measured over a range of operating conditions. Significant oligomerization activity of the catalyst was found. Testing the pelletized catalyst with CO2, CO and H2 mixtures over a range of operating conditions demonstrated its high productivity to higher hydrocarbons. The composition of the liquid (C5+) was found to be a function of the potassium content and the composition of the feedstock.

  6. Malaria Parasite Metabolic Pathways (MPMP) Upgraded with Targeted Chemical Compounds.

    PubMed

    Ginsburg, Hagai; Abdel-Haleem, Alyaa M

    2016-01-01

    Malaria Parasite Metabolic Pathways (MPMP) is the website for the functional genomics of intraerythrocytic Plasmodium falciparum. All the published information about targeted chemical compounds has now been added. Users can find the drug target and publication details linked to a drug database for further information about the medicinal properties of each compound.

  7. The effect of nitrogen doping on mercury oxidation/chemical adsorption on the CuCo2O4(110) surface: a molecular-level description.

    PubMed

    Mei, Zhijian; Fan, Maohong; Zhang, Ruiqing; Shen, Zhemin; Wang, Wenhua

    2014-07-14

    Based on density functional theory (DFT) calculations, the detailed mercury oxidation/chemical adsorption mechanisms on the N-doped CuCo2O4(110) surface are studied. The DFT calculations show that Ow (bonded with one Cu(2+) ion and one Co(3+) ion) is far more active than Os (bonded with three Co(3+) ions) and the mercury oxidation/chemical adsorption activation energy (Ea) on the virgin CuCo2O4(110) surface involving Ow is 0.85 eV. The physically adsorbed mercury overcomes the Ea and enters the energy well that plays an important role in mercury oxidation/chemical adsorption. Nitrogen doping can greatly increase the activity of Ow and decrease the activity of Os at the same time, which greatly affect the mercury oxidation/chemical adsorption abilities on the CuCo2O4(110) surface, and the Ea variation of mercury oxidation/chemical adsorption is as follows: 0.85 eV (virgin CuCo2O4(110)) → 0.76 eV (one N-doped CuCo2O4(110)) → 0.69 eV (two N-doped CuCo2O4(110)) → 0.48 eV (three N-doped CuCo2O4(110)). In addition, N-doping can decrease the adsorption energy of mercury and mercuric oxide. The effect of N-doping on the bonding mechanism of mercury adsorption on the CuCo2O4(110) surface is analyzed by the local density of state (LDOS) and the natural bonding orbital (NBO). The calculation results correspond well to the experimental data.

  8. Mass Conservation in a Chemical Transport Model and its Effect on CO2 and SF6 Simulations

    NASA Technical Reports Server (NTRS)

    Zhu, Z.; Weaver, C.; Kawa, S. R.; Douglass, A. R.; Bhartia, P. K. (Technical Monitor)

    2002-01-01

    Chemical transport models (CTMs) must conserve mass to be useful for applications involving assessment of the effect of various pollutants on the troposphere and stratosphere. Furthermore, calculations of the evolution of constituents such as SF6 are used to evaluate overall model transport, and interpretation of such simulations is clouded if mass conservation is not assured. For realistic simulations or predictions, it is crucial that constituents are not produced or lost by transport or other processes in the CTMs. Analysis of CO2 and SF6 experiments using a CTM shows that problems with mass conservation can seriously degrade the simulations. Failure to conserve mass results from inconsistency of the surface pressure tendency and the divergence of horizontal mass flux when the model is forced by assimilated meteorological data. We have developed an effective method to eliminate the inconsistency by modifying the divergent part of the wind field. The changes in the wind fields are quite small but the impact on mass conservation is large. Parameterizations of physical processes such as convection or turbulent transport can also affect mass conservation. The lack of conservation is small but accumulates when integrations are lengthy such as required for SF6. This lack of conservation is found using winds from either a GCM or from an assimilation system. A simple adjustment removes much of the inaccuracy in the convective parameterization. A CO2 simulation using assimilated winds from the most recent version of the Goddard Earth Observing System Data Assimilation System will be used to illustrate the impact of these transport improvements.

  9. Chemical and morphological changes during olivine carbonation for CO2 storage in the presence of NaCl and NaHCO3.

    PubMed

    Gadikota, Greeshma; Matter, Juerg; Kelemen, Peter; Park, Ah-Hhyung Alissa

    2014-03-14

    The increasing concentrations of CO2 in the atmosphere are attributed to the rising consumption of fossil fuels for energy generation around the world. One of the most stable and environmentally benign methods of reducing atmospheric CO2 is by storing it as thermodynamically stable carbonate minerals. Olivine ((Mg,Fe)2SiO4) is an abundant mineral that reacts with CO2 to form Mg-carbonate. The carbonation of olivine can be enhanced by injecting solutions containing CO2 at high partial pressure into olivine-rich formations at high temperatures, or by performing ex situ mineral carbonation in a reactor system with temperature and pressure control. In this study, the effects of NaHCO3 and NaCl, whose roles in enhanced mineral carbonation have been debated, were investigated in detail along with the effects of temperature, CO2 partial pressure and reaction time for determining the extent of olivine carbonation and its associated chemical and morphological changes. At high temperature and high CO2 pressure conditions, more than 70% olivine carbonation was achieved in 3 hours in the presence of 0.64 M NaHCO3. In contrast, NaCl did not significantly affect olivine carbonation. As olivine was dissolved and carbonated, its pore volume, surface area and particle size were significantly changed and these changes influenced subsequent reactivity of olivine. Thus, for both long-term simulation of olivine carbonation in geologic formations and the ex situ reactor design, the morphological changes of olivine during its reaction with CO2 should be carefully considered in order to accurately estimate the CO2 storage capacity and understand the mechanisms for CO2 trapping by olivine.

  10. Using Carbonyl Sulfide Column Measurements and a Chemical Transport Model to Investigate Variability in Biospheric CO2 Fluxes

    NASA Astrophysics Data System (ADS)

    Wang, Y.; Palm, M.; Deutscher, N. M.; Warneke, T.; Notholt, J.; Baker, I. T.; Berry, J. A.; Suntharalingam, P.; Campbell, J. E.; Wolf, A.

    2014-12-01

    Understanding the CO2 processes on land is of great importance, because the terrestrial exchange drives the seasonal and interannual variability of CO2 in the atmosphere. Atmospheric inversions based on CO2 concentration measurements alone can only determine net biosphere fluxes, but not differentiate between photosynthesis (uptake) and respiration (production). Carbonyl sulfide (OCS) could provide an important additional constraint: it is also taken up by plants during photosynthesis but not emitted during respiration, and therefore is a potential means to differentiate between these processes. Solar absorption Fourier Transform InfraRed (FTIR) spectrometry allows for the retrieval of the atmospheric concentrations of both CO2 and OCS. Here, we investigate co-located and nearly simultaneous measurements of OCS and CO2 measured at 3 sites via FTIR spectrometers. These northern-hemispheric sites span a wide range of latitudes and all have multiple year time-series. The sites include Ny-Alesund (79°N), Bremen (53°N) and Paramaribo (6°N). We compare these measurements to simulations of OCS and CO2 using the GEOS-Chem model. The simulations are driven by different land biospheric fluxes of OCS and CO2 to match the seasonality of the measurements. The simple biosphere model (SiB-COS) are used in the study because it simultaneously calculates the biospheric fluxes of both OCS and CO2. The CO2 simulation with SiB fluxes agrees with the measurements better than a simulation using CASA. Comparison of the OCS simulations with different fluxes indicates that the latitudinal distribution of the OCS fluxes within SiB needs to be adjusted.

  11. Using Carbonyl Sulfide column measurements and a Chemical Transport Model to investigate variability in biospheric CO2 fluxes

    NASA Astrophysics Data System (ADS)

    Wang, Yuting; Petri, Christof; Palm, Mathias; Warneke, Thorsten; Baker, Ian; Berry, Joe; Suntharalingam, Parvadha; Campbell, Elliott; Wolf, Adam; Deutscher, Nick; Notholt, Justus

    2015-04-01

    Understanding the CO2 processes on land is of great importance, because the terrestrial exchange drives the seasonal and interannual variability of CO2 in the atmosphere. Atmospheric inversions based on CO2 concentration measurements alone can only determine net biosphere fluxes, but not differentiate between photosynthesis (uptake) and respiration (production). Carbonyl sulfide (OCS) could provide an important additional constraint: it is also taken up by plants during photosynthesis but not emitted during respiration, and therefore is a potential means to differentiate between these processes. Solar absorption Fourier Transform InfraRed (FTIR) spectrometry allows for the retrieval of the atmospheric concentrations of both CO2 and OCS. Here, we investigate co-located and nearly simultaneous measurements of OCS and CO2 measured at 3 sites via FTIR spectrometers. These northern-hemispheric sites span a wide range of latitudes and all have multiple year time-series. The sites include Ny-Alesund (79°N), Bremen (53°N) and Paramaribo (6°N). We compare these measurements to simulations of OCS and CO2 using the GEOS-Chem model. The simulations are driven by different land biospheric fluxes of OCS and CO2 to match the seasonality of the measurements. The simple biosphere model (SiB-COS) are used in the study because it simultaneously calculates the biospheric fluxes of both OCS and CO2. The CO2 simulation with SiB fluxes agrees with the measurements better than a simulation using CASA. Comparison of the OCS simulations with different fluxes indicates that the latitudinal distribution of the OCS fluxes within SiB needs to be adjusted.

  12. Theoretical study of the influence of chemical reactions and physical parameters on the convective dissolution of CO2 in aqueous solutions

    NASA Astrophysics Data System (ADS)

    Loodts, Vanessa; Rongy, Laurence; De Wit, Anne

    2014-05-01

    Subsurface carbon sequestration has emerged as a promising solution to the problem of increasing atmospheric carbon dioxide (CO2) levels. How does the efficiency of such a sequestration process depend on the physical and chemical characteristics of the storage site? This question is emblematic of the need to better understand the dynamics of CO2 in subsurface formations, and in particular, the properties of the convective dissolution of CO2 in the salt water of aquifers. This dissolution is known to improve the safety of the sequestration by reducing the risks of leaks of CO2 to the atmosphere. Buoyancy-driven convection makes this dissolution faster by transporting dissolved CO2 further away from the interface. Indeed, upon injection, the less dense CO2 phase rises above the aqueous layer where it starts to dissolve. The dissolved CO2 increases the density of the aqueous solution, thereby creating a layer of denser CO2-rich solution above less dense solution. This unstable density gradient in the gravity field is at the origin of convection. In this framework, we theoretically investigate the effect of CO2 pressure, salt concentration, temperature, and chemical reactions on the dissolution-driven convection of CO2 in aqueous solutions. On the basis of a linear stability analysis, we assess the stability of the time-dependent density profiles developing when CO2 dissolves in an aqueous layer below it. We predict that increasing CO2 pressure destabilizes the system with regard to buoyancy-driven convection, because it increases the density gradient at the origin of the instability. By contrast, increasing salt concentration or temperature stabilizes the system via effects on CO2 solubility, solutal expansion coefficient, diffusion coefficient and on the viscosity and density of the solution. We also show that a reaction of CO2 with chemical species dissolved in the aqueous solution can either enhance or decrease the amplitude of the convective dissolution compared

  13. Potential impacts on groundwater resources of deep CO2 storage: natural analogues for assessing potential chemical effects

    NASA Astrophysics Data System (ADS)

    Lions, J.; Gale, I.; May, F.; Nygaard, E.; Ruetters, H.; Beaubien, S.; Sohrabi, M.; Hatzignatiou, D. G.; CO2GeoNet Members involved in the present study Team

    2011-12-01

    Carbon dioxide Capture and Storage (CCS) is considered as one of the promising options for reducing atmospheric emissions of CO2 related to human activities. One of the main concerns associated with the geological storage of CO2 is that the CO2 may leak from the intended storage formation, migrate to the near-surface environment and, eventually, escape from the ground. This is a concern because such leakage may affect aquifers overlying the storage site and containing freshwater that may be used for drinking, industry and agriculture. The IEA Greenhouse Gas R&D Programme (IEAGHG) recently commissioned the CO2GeoNet Association to undertake a review of published and unpublished literature on this topic with the aim of summarizing 'state of the art' knowledge and identifying knowledge gaps and research priorities in this field. Work carried out by various CO2GeoNet members was also used in this study. This study identifies possible areas of conflict by combining available datasets to map the global and regional superposition of deep saline formations (DSF) suitable for CO2 storage and overlying fresh groundwater resources. A scenario classification is developed for the various geological settings where conflict could occur. The study proposes two approaches to address the potential impact mechanisms of CO2 storage projects on the hydrodynamics and chemistry of shallow groundwater. The first classifies and synthesizes changes of water quality observed in natural/industrial analogues and in laboratory experiments. The second reviews hydrodynamic and geochemical models, including coupled multiphase flow and reactive transport. Various models are discussed in terms of their advantages and limitations, with conclusions on possible impacts on groundwater resources. Possible mitigation options to stop or control CO2 leakage are assessed. The effect of CO2 pressure in the host DSF and the potential effects on shallow aquifers are also examined. The study provides a review of

  14. Recycling of CO2: Probing the Chemical State of the Ni(111) Surface during the Methanation Reaction with Ambient-Pressure X-Ray Photoelectron Spectroscopy.

    PubMed

    Heine, Christian; Lechner, Barbara A J; Bluhm, Hendrik; Salmeron, Miquel

    2016-10-12

    Using ambient-pressure X-ray photoelectron spectroscopy (AP-XPS), we studied the adsorption and reactions of CO2 and CO2 + H2 on the Ni(111) surface to identify the surface chemical state and the nature of the adsorbed species during the methanation reaction. In 200 mTorr CO2, we found that NiO is formed from CO2 dissociation into CO and atomic oxygen. Additionally, carbonate (CO3(2-)) is present on the surface from further reaction of CO2 with NiO. The addition of H2 into the reaction environment leads to reduction of NiO and the disappearance of CO3(2-). At temperatures >160 °C, CO adsorbed on hollow sites, and atomic carbon and OH species are present on the surface. We conclude that the methanation reaction proceeds via dissociation of CO2, followed by reduction of CO to atomic carbon and its hydrogenation to methane.

  15. A microporous Cu-MOF with optimized open metal sites and pore spaces for high gas storage and active chemical fixation of CO2.

    PubMed

    Gao, Chao-Ying; Tian, Hong-Rui; Ai, Jing; Li, Lei-Jiao; Dang, Song; Lan, Ya-Qian; Sun, Zhong-Ming

    2016-09-25

    A microporous Cu-MOF with optimized open metal sites and pore space was constructed based on a designed bent ligand; it exhibits high-capacity multiple gas storage under atmospheric pressure and efficient catalytic activity for chemical fixation of CO2 under mild conditions.

  16. Application of Chemical Doping and Architectural Design Principles To Fabricate Nanowire Co2Ni3ZnO8 Arrays for Aqueous Asymmetric Supercapacitors.

    PubMed

    Liu, Qi; Yang, Bin; Liu, Jingyuan; Yuan, Yi; Zhang, Hongsen; Liu, Lianhe; Wang, Jun; Li, Rumin

    2016-08-10

    Electrode materials derived from transition metal oxides have a serious problem of low electron transfer rate, which restricts their practical application. However, chemically doped graphene transforms the chemical bonding configuration to enhance electron transfer rate and, therefore, facilitates the successful fabrication of Co2Ni3ZnO8 nanowire arrays. In addition, the Co2Ni3ZnO8 electrode materials, considered as Ni and Zn ions doped into Co3O4, have a high electron transfer rate and electrochemical response capability, because the doping increases the degree of crystal defect and reaction of Co/Ni ions with the electrolyte. Hence, the Co2Ni3ZnO8 electrode exhibits a high rate property and excellent electrochemical cycle stability, as determined by electrochemical analysis of the relationship between specific capacitance, IR drop, Coulomb efficiency, and different current densities. From the results of a three-electrode system of electrochemical measurement, the Co2Ni3ZnO8 electrode demonstrates a specific capacitance of 1115 F g(-1) and retains 89.9% capacitance after 2000 cycles at a current density of 4 A g(-1). The energy density of the asymmetric supercapacitor (AC//Co2Ni3ZnO8) is 54.04 W h kg(-1) at the power density of 3200 W kg(-1).

  17. Chemical evolution of dissolved inorganic carbon species flowing in thin water films and its implications for (rapid) degassing of CO2 during speleothem growth

    NASA Astrophysics Data System (ADS)

    Hansen, Maximilian; Dreybrodt, Wolfgang; Scholz, Denis

    2013-04-01

    Rapid degassing of CO2 from a thin film of drip water on the surface of stalagmites is often considered to have a large effect on both speleothem growth and stable isotope values and is offered as an explanation for higher δ13C and δ18O values than expected under conditions of stable isotope equilibrium. However, the time constant for degassing of CO2 from the solution only depends on film thickness and the coefficient of molecular diffusion for CO2. Thus, for thin films, the time for degassing of CO2 is much shorter than the time for subsequent equilibration of the dissolved carbon species and precipitation of CaCO3. In this context, degassing of CO2 is always fast. Here we present three experiments that enable the determination of the time constants for degassing of CO2, τdeg, subsequent equilibration to a new pCO2, τeq, and precipitation of CaCO3, τpr, in a thin film of an H2O-CO2-CaCO3 solution flowing on a calcite surface. The experiments are performed under cave-analogue conditions. At a temperature of 20 °C and for a film thickness of δ ≈ 0.01 cm, τdeg ≈ 2 s. τeq ≈ 13 s and, thus, one order of magnitude larger. Finally, τpr ≈ 400 s for δ ≈ 0.01 cm, again one order of magnitude larger. The experimentally determined values for τdeg, τeqτpr are in good agreement with the theoretical predictions. Our results confirm that the chemical evolution of the drip water proceeds in three subsequent major steps. During the first step of degassing of CO2, pH and Ca2+ concentration remain almost constant. During equilibration to the lower pCO2 of the solution, pH increases to about 8 whereas the Ca2+ concentration still remains constant. Finally, during precipitation of calcite, pCO2 remains at its low level and pH decreases slightly. These results suggest that the drip rate may have an important influence on the stable isotope signals recorded in speleothems. Stalagmites growing beneath drip sites with stable, intermediate drip rates (i.e., in the

  18. Coal Direct Chemical Looping Retrofit to Pulverized Coal Power Plants for In-Situ CO2 Capture

    SciTech Connect

    Zeng, Liang; Li, Fanxing; Kim, Ray; Bayham, Samuel; McGiveron, Omar; Tong, Andrew; Connell, Daniel; Luo, Siwei; Sridhar, Deepak; Wang, Fei; Sun, Zhenchao; Fan, Liang-Shih

    2013-09-30

    A novel Coal Direct Chemical Looping (CDCL) system is proposed to effectively capture CO2 from existing PC power plants. The work during the past three years has led to an oxygen carrier particle with satisfactory performance. Moreover, successful laboratory, bench scale, and integrated demonstrations have been performed. The proposed project further advanced the novel CDCL technology to sub-pilot scale (25 kWth). To be more specific, the following objectives attained in the proposed project are: 1. to further improve the oxygen carrying capacity as well as the sulfur/ash tolerance of the current (working) particle; 2. to demonstrate continuous CDCL operations in an integrated mode with > 99% coal (bituminous, subbituminous, and lignite) conversion as well as the production of high temperature exhaust gas stream that is suitable for steam generation in existing PC boilers; 3. to identify, via demonstrations, the fate of sulfur and NOx; 4. to conduct thorough techno-economic analysis that validates the technical and economical attractiveness of the CDCL system. The objectives outlined above were achieved through collaborative efforts among all the participants. CONSOL Energy Inc. performed the techno-economic analysis of the CDCL process. Shell/CRI was able to perform feasibility and economic studies on the large scale particle synthesis and provide composite particles for the sub-pilot scale testing. The experience of B&W (with boilers) and Air Products (with handling gases) assisted the retrofit system design as well as the demonstration unit operations. The experience gained from the sub-pilot scale demonstration of the Syngas Chemical Looping (SCL) process at OSU was able to ensure the successful handling of the solids. Phase 1 focused on studies to improve the current particle to better suit the CDCL operations. The optimum operating conditions for the reducer reactor such as the temperature, char gasification enhancer type, and flow rate were identified. The

  19. New candidate for biofuel feedstock beyond terrestrial biomass for thermo-chemical process (pyrolysis/gasification) enhanced by carbon dioxide (CO2).

    PubMed

    Kwon, Eilhann E; Jeon, Young Jae; Yi, Haakrho

    2012-11-01

    The enhanced thermo-chemical process (i.e., pyrolysis/gasification) of various macroalgae using carbon dioxide (CO(2)) as a reaction medium was mainly investigated. The enhanced thermo-chemical process was achieved by expediting the thermal cracking of volatile chemical species derived from the thermal degradation of the macroalgae. This process enables the modification of the end products from the thermo-chemical process and significant reduction of the amount of condensable hydrocarbons (i.e., tar, ∼50%), thereby directly increasing the efficiency of the gasification process.

  20. Chemical structures of coal lithotypes before and after CO2 adsorption as investigated by advanced solid-state 13C nuclear magnetic resonance spectroscopy

    USGS Publications Warehouse

    Cao, X.; Mastalerz, Maria; Chappell, M.A.; Miller, L.F.; Li, Y.; Mao, J.

    2011-01-01

    Four lithotypes (vitrain, bright clarain, clarain, and fusain) of a high volatile bituminous Springfield Coal from the Illinois Basin were characterized using advanced solid-state 13C nuclear magnetic resonance (NMR) spectroscopy. The NMR techniques included quantitative direct polarization/magic angle spinning (DP/MAS), cross polarization/total sideband suppression (CP/TOSS), dipolar dephasing, CHn selection, and recoupled C-H long-range dipolar dephasing techniques. The lithotypes that experienced high-pressure CO2 adsorption isotherm analysis were also analyzed to determine possible changes in coal structure as a result of CO2 saturation at high pressure and subsequent evacuation. The main carbon functionalities present in original vitrain, bright clarain, clarain and fusain were aromatic carbons (65.9%-86.1%), nonpolar alkyl groups (9.0%-28.9%), and aromatic C-O carbons (4.1%-9.5%). Among these lithotypes, aromaticity increased in the order of clarain, bright clarain, vitrain, and fusain, whereas the fraction of alkyl carbons decreased in the same order. Fusain was distinct from other three lithotypes in respect to its highest aromatic composition (86.1%) and remarkably small fraction of alkyl carbons (11.0%). The aromatic cluster size in fusain was larger than that in bright clarain. The lithotypes studied responded differently to high pressure CO2 saturation. After exposure to high pressure CO2, vitrain and fusain showed a decrease in aromaticity but an increase in the fraction of alkyl carbons, whereas bright clarain and clarain displayed an increase in aromaticity but a decrease in the fraction of alkyl carbons. Aromatic fused-rings were larger for bright clarain but smaller for fusain in the post-CO2 adsorption samples compared to the original lithotypes. These observations suggested chemical CO2-coal interactions at high pressure and the selectivity of lithotypes in response to CO2 adsorption. ?? 2011 Elsevier B.V.

  1. Climate Extreme Effects on the Chemical Composition of Temperate Grassland Species under Ambient and Elevated CO2: A Comparison of Fructan and Non-Fructan Accumulators

    PubMed Central

    Zinta, Gaurav; Van den Ende, Wim; Janssens, Ivan A.; Asard, Han

    2014-01-01

    Elevated CO2 concentrations and extreme climate events, are two increasing components of the ongoing global climatic change factors, may alter plant chemical composition and thereby their economic and ecological characteristics, e.g. nutritional quality and decomposition rates. To investigate the impact of climate extremes on tissue quality, four temperate grassland species: the fructan accumulating grasses Lolium perenne, Poa pratensis, and the nitrogen (N) fixing legumes Medicago lupulina and Lotus corniculatus were subjected to water deficit at elevated temperature (+3°C), under ambient CO2 (392 ppm) and elevated CO2 (620 ppm). As a general observation, the effects of the climate extreme were larger and more ubiquitous in combination with elevated CO2. The imposed climate extreme increased non-structural carbohydrate and phenolics in all species, whereas it increased lignin in legumes and decreased tannins in grasses. However, there was no significant effect of climate extreme on structural carbohydrates, proteins, lipids and mineral contents and stoichiometric ratios. In combination with elevated CO2, climate extreme elicited larger increases in fructan and sucrose content in the grasses without affecting the total carbohydrate content, while it significantly increased total carbohydrates in legumes. The accumulation of carbohydrates in legumes was accompanied by higher activity of sucrose phosphate synthase, sucrose synthase and ADP-Glc pyrophosphorylase. In the legumes, elevated CO2 in combination with climate extreme reduced protein, phosphorus (P) and magnesium (Mg) contents and the total element:N ratio and it increased phenol, lignin, tannin, carbon (C), nitrogen (N) contents and C:N, C:P and N:P ratios. On the other hand, the tissue composition of the fructan accumulating grasses was not affected at this level, in line with recent views that fructans contribute to cellular homeostasis under stress. It is speculated that quality losses will be less

  2. An integrated system combining chemical looping hydrogen generation process and solid oxide fuel cell/gas turbine cycle for power production with CO2 capture

    NASA Astrophysics Data System (ADS)

    Chen, Shiyi; Xue, Zhipeng; Wang, Dong; Xiang, Wenguo

    2012-10-01

    In this paper, the solid oxide fuel cell/gas turbine (SOFC/GT) cycle is integrated with coal gasification and chemical looping hydrogen generation (CLHG) for electric power production with CO2 capture. The CLHG-SOFC/GT plant is configurated and the schematic process is modeled using Aspen Plus® software. Syngas, produced by coal gasification, is converted to hydrogen with CO2 separation through a three-reactors CLHG process. Hydrogen is then fueled to SOFC for power generation. The unreacted hydrogen from SOFC burns in a combustor and drives gas turbine. The heat of the gas turbine exhaust stream is recovered in HRSG for steam bottoming cycle. At a system pressure of 20 bar and a cell temperature of 900 °C, the CLHG-SOFC/GT plant has a net power efficiency of 43.53% with no CO2 emissions. The hybrid power plant performance is attractive because of high energy conversion efficiency and zero-CO2-emission. Key parameters that influence the system performance are also discussed, including system operating pressure, cell temperature, fuel utilization factor, steam reactor temperature, CO2 expander exhaust pressure and inlet gas preheating.

  3. LHCb VELO upgrade

    NASA Astrophysics Data System (ADS)

    Hennessy, Karol

    2017-02-01

    The upgrade of the LHCb experiment, scheduled for LHC Run-III, scheduled to start in 2021, will transform the experiment to a trigger-less system reading out the full detector at 40 MHz event rate. All data reduction algorithms will be executed in a high-level software farm enabling the detector to run at luminosities of 2×1033 cm-2 s-1. The Vertex Locator (VELO) is the silicon vertex detector surrounding the interaction region. The current detector will be replaced with a hybrid pixel system equipped with electronics capable of reading out at 40 MHz. The upgraded VELO will provide fast pattern recognition and track reconstruction to the software trigger. The silicon pixel sensors have 55×55 μm2 pitch, and are read out by the VeloPix ASIC, from the Timepix/Medipix family. The hottest region will have pixel hit rates of 900 Mhits/s yielding a total data rate of more than 3 Tbit/s for the upgraded VELO. The detector modules are located in a separate vacuum, separated from the beam vacuum by a thin custom made foil. The foil will be manufactured through milling and possibly thinned further by chemical etching. The material budget will be minimised by the use of evaporative CO2 coolant circulating in microchannels within 400 μm thick silicon substrates. The current status of the VELO upgrade is described and latest results from operation of irradiated sensor assemblies are presented.

  4. DIC dynamics in stream water of volcanic settings: climatic and lithology impact on the CO2 chemical weathering (Lesser Antilles, Reunion, French Massif Central and Iceland)

    NASA Astrophysics Data System (ADS)

    Rive, K.; Agrinier, P.; Gaillardet, J.

    2006-12-01

    The chemical weathering of the volcanic rocks plays a key role in the regulation of atmospheric CO2. Indeed, CO2 is one of the main proton suppliers (e.g. Louvat, 1997; Dessert et al., 2003) via the acid-base system of the dissolved inorganic carbon (DIC = H2CO3 + HCO3- + CO32-). Consequently, riverine DIC fluxes can help to constrain chemical erosion fluxes. However the behavior of DIC in rivers must be first understood because it can be affected by many geochemical processes (e.g. CO2 degassing, carbonate precipitation/dissolution, photosynthesis, organic matter decay). In order to investigate these processes, we have used the δ13C of the DIC. Four volcanic sites have been studied. They have different climates (tropical, temperate and sub-polar), different lithologies and different histories of formation: basaltic-andesitic islands (subduction arc of the Lesser Antilles: Guadeloupe, Dominica and Martinique) and basaltic islands (Reunion hot spot and Iceland hot spot-MOR system). The main differences between these sites are 1) the thickness of soils, and 2) the type and the abundance of vegetation (both are controlled by climatic factors: the mean annual temperature and the mean annual rainfall) and 3) the absence of sedimentary carbonate rocks. The common points among these sites are the high relieves and the magmatic CO2 degassing which controls the DIC of the hydrothermal springs. In such active volcanism settings, magmatic CO2 contribution is seen only in few streams, generally located close to the volcano heights and in the proximity of the hydrothermal springs. These streams show high δ13CDIC, generally around -3 ‰, and high DIC. The rivers in all sampling sites show an endmember with a δ13CDIC of about -15 ‰, characteristic of the organic matter. Therefore, like in large rivers(e.g. Aucour et al., 1999 or Telmer and Veizer, 1999), organic matters are the main sources of DIC in these streams, even on sites with few vegetation (limited to grasslands or

  5. A Bifunctional Europium-Organic Framework with Chemical Fixation of CO2 and Luminescent Detection of Al(3).

    PubMed

    Xu, Hang; Zhai, Bin; Cao, Chun-Shuai; Zhao, Bin

    2016-10-03

    A novel three-dimensional lanthanide-organic framework {[Eu(BTB)(phen)]·4.5DMF·2H2O}n (1) has been synthesized. Structural characterization suggests that framework 1 possesses one-dimensional channels with potential pore volume, and the large channels in the framework can capture CO2. Interestingly, investigations on the cycloaddition reaction of CO2 and epoxides reveal that compound 1 can be considered as an efficient catalyst for CO2 fixation with epoxides under 1 atm pressure. Importantly, 1 can be reused at least five times without any obvious loss in catalytic activity. Furthermore, the luminescent explorations of 1 reveal that 1 can act as a recyclable sensor of Al(3+), and the corresponding detection limit can reach 5 × 10(-8) M (1.35 ppb), which is obviously lower than the United States Environmental Protection Agency's recommended level of Al(3+) in drinking water (200 ppb). These results show that 1 has a level of sensitivity higher than that of other reported MOF-based sensors of Al(3+).

  6. Photoelectrocatalytic reduction of CO2 into chemicals using Pt-modified reduced graphene oxide combined with Pt-modified TiO2 nanotubes.

    PubMed

    Cheng, Jun; Zhang, Meng; Wu, Gai; Wang, Xin; Zhou, Junhu; Cen, Kefa

    2014-06-17

    The photoelectrocatalytic (PEC) reduction of CO2 into high-value chemicals is beneficial in alleviating global warming and advancing a low-carbon economy. In this work, Pt-modified reduced graphene oxide (Pt-RGO) and Pt-modified TiO2 nanotubes (Pt-TNT) were combined as cathode and photoanode catalysts, respectively, to form a PEC reactor for converting CO2 into valuable chemicals. XRD, XPS, TEM, AFM, and SEM were employed to characterize the microstructures of the Pt-RGO and Pt-TNT catalysts. Reduction products, such as C2H5OH and CH3COOH, were obtained from CO2 under band gap illumination and biased voltage. A combined liquid product generation rate (CH3OH, C2H5OH, HCOOH, and CH3COOH) of approximately 600 nmol/(h·cm(2)) was observed. Carbon atom conversion rate reached 1,130 nmol/(h·cm(2)), which were much higher than those achieved using Pt-modified carbon nanotubes and platinum carbon as cathode catalysts.

  7. CO2-neutral fuels

    NASA Astrophysics Data System (ADS)

    Goede, A. P. H.

    2015-08-01

    The need for storage of renewable energy (RE) generated by photovoltaic, concentrated solar and wind arises from the fact that supply and demand are ill-matched both geographically and temporarily. This already causes problems of overcapacity and grid congestion in countries where the fraction of RE exceeds the 20% level. A system approach is needed, which focusses not only on the energy source, but includes conversion, storage, transport, distribution, use and, last but not least, the recycling of waste. Furthermore, there is a need for more flexibility in the energy system, rather than relying on electrification, integration with other energy systems, for example the gas network, would yield a system less vulnerable to failure and better adapted to requirements. For example, long-term large-scale storage of electrical energy is limited by capacity, yet needed to cover weekly to seasonal demand. This limitation can be overcome by coupling the electricity net to the gas system, considering the fact that the Dutch gas network alone has a storage capacity of 552 TWh, sufficient to cover the entire EU energy demand for over a month. This lecture explores energy storage in chemicals bonds. The focus is on chemicals other than hydrogen, taking advantage of the higher volumetric energy density of hydrocarbons, in this case methane, which has an approximate 3.5 times higher volumetric energy density. More importantly, it allows the ready use of existing gas infrastructure for energy storage, transport and distribution. Intermittent wind electricity generated is converted into synthetic methane, the Power to Gas (P2G) scheme, by splitting feedstock CO2 and H2O into synthesis gas, a mixture of CO and H2. Syngas plays a central role in the synthesis of a range of hydrocarbon products, including methane, diesel and dimethyl ether. The splitting is accomplished by innovative means; plasmolysis and high-temperature solid oxygen electrolysis. A CO2-neutral fuel cycle is

  8. Major ion chemistry in the headwaters of the Yamuna river system:. Chemical weathering, its temperature dependence and CO 2 consumption in the Himalaya

    NASA Astrophysics Data System (ADS)

    Dalai, T. K.; Krishnaswami, S.; Sarin, M. M.

    2002-10-01

    The Yamuna river and its tributaries in the Himalaya constitute the Yamuna River System (YRS). The YRS basin has a drainage area and discharge comparable in magnitude to those of the Bhagirathi and the Alaknanda rivers, which merge to form the Ganga at the foothills of the Himalaya. A detailed geochemical study of the YRS was carried out to determine: (i) the relative significance of silicate, carbonate and evaporite weathering in contributing to its major ion composition; (ii) CO 2 consumption via silicate weathering; and (iii) the factors regulating chemical weathering of silicates in the basin. The results show that the YRS waters are mildly alkaline, with a wide range of TDS, ˜32 to ˜620 mg l-1. In these waters, the abundances of Ca, Mg and alkalinity, which account for most of TDS, are derived mainly from carbonates. Many of the tributaries in the lower reaches of the Yamuna basin are supersaturated with calcite. In addition to carbonic acid, sulphuric acid generated by oxidation of pyrites also seems to be supplying protons for chemical weathering. Silicate weathering in YRS basin contributes, on average, ˜25% (molar basis) of total cations on a basin wide scale. Silicate weathering, however, does not seem to be intense in the basin as evident from low Si/(Na*+K) in the waters, ˜1.2 and low values of chemical index of alteration (CIA) in bed sediments, ˜60. CO 2 drawdown resulting from silicate weathering in the YRS basin in the Himalaya during monsoon ranges between (4 to 7) × 10 5 moles km -2 y -1. This is higher than that estimated for the Ganga at Rishikesh for the same season. The CO 2 consumption rates in the Yamuna and the Ganga basins in the Himalaya are higher than the global average value, suggesting enhanced CO 2 drawdown in the southern slopes of the Himalaya. The impact of this enhanced drawdown on the global CO 2 budget may not be pronounced, as the drainage area of the YRS and the Ganga in the Himalaya is small. The CO 2 drawdown by

  9. Spring carbonate chemistry dynamics of surface waters in the northern East China Sea: Water mixing, biological uptake of CO2, and chemical buffering capacity

    NASA Astrophysics Data System (ADS)

    Zhai, Wei-Dong; Chen, Jian-Fang; Jin, Hai-Yan; Li, Hong-Liang; Liu, Jin-Wen; He, Xian-Qiang; Bai, Yan

    2014-09-01

    We investigated sea surface total alkalinity (TAlk), dissolved inorganic carbon (DIC), dissolved oxygen (DO), and satellite-derived chlorophyll-a in the connection between the Yellow Sea and the East China Sea (ECS) during April to early May 2007. In spring, Changjiang dilution water (CDW), ECS offshore water, and together with Yellow Sea water (YSW) occupied the northern ECS. Using 16 day composite satellite-derived chlorophyll-a images, several algal blooms were identified in the CDW and ECS offshore water. Correspondingly, biological DIC drawdown of 73 ± 20 μmol kg-1, oversaturated DO of 10-110 μmol O2 kg-1, and low fugacity of CO2 of 181-304 μatm were revealed in these two waters. YSW also showed CO2 uptake in spring, due to the very low temperature. However, its intrusion virtually counteracted CO2 uptake in the northern ECS. In the CDW and the ECS offshore water, Revelle factor was 9.3-11.7 and 8.9-10.6, respectively, while relatively high Revelle factor values of 11.4-13.0 were revealed in YSW. In the ECS offshore water, the observed relationship between DIC drawdown and oversaturated DO departed from the Redfield ratio, indicating an effect of chemical buffering capacity on the carbonate system during air-sea reequilibration. Given the fact that the chemical buffering capacity slows down the air-sea reequilibration of CO2, the early spring DIC drawdown may have durative effects on the sea surface carbonate system until early summer. Although our study is subject to limited temporal and spatial coverage of sampling, these insights are fundamental to understanding sea surface carbonate chemistry dynamics in this important ocean margin.

  10. Towards Ideal NOx and CO2 Emission Control Technology for Bio-Oils Combustion Energy System Using a Plasma-Chemical Hybrid Process

    NASA Astrophysics Data System (ADS)

    Okubo, M.; Fujishima, H.; Yamato, Y.; Kuroki, T.; Tanaka, A.; Otsuka, K.

    2013-03-01

    A pilot-scale low-emission boiler system consisting of a bio-fuel boiler and plasma-chemical hybrid NOx removal system is investigated. This system can achieve carbon neutrality because the bio-fuel boiler uses waste vegetable oil as one of the fuels. The plasma-chemical hybrid NOx removal system has two processes: NO oxidation by ozone produced from plasma ozonizers and NO2 removal using a Na2SO3 chemical scrubber. Test demonstrations of the system are carried out for mixed oils (mixture of A-heavy oil and waste vegetable oil). Stable combustion is achieved for the mixed oil (20 - 50% waste vegetable oil). Properties of flue gas—e.g., O2, CO2 and NOx—when firing mixed oils are nearly the same as those when firing heavy oil for an average flue gas flow rate of 1000 Nm3/h. NOx concentrations at the boiler outlet are 90 - 95 ppm. Furthermore, during a 300-min continuous operation when firing 20% mixed oil, NOx removal efficiency of more than 90% (less than 10 ppm NOx emission) is confirmed. In addition, the CO2 reduction when heavy oil is replaced with waste vegetable oil is estimated. The system comparison is described between the plasma-chemical hybrid NOx removal and the conventional technology.

  11. Water geochemistry of the Qiantangjiang River, East China: Chemical weathering and CO2 consumption in a basin affected by severe acid deposition

    NASA Astrophysics Data System (ADS)

    Liu, Wenjing; Shi, Chao; Xu, Zhifang; Zhao, Tong; Jiang, Hao; Liang, Chongshan; Zhang, Xuan; Zhou, Li; Yu, Chong

    2016-09-01

    The chemical composition of the Qiantangjiang River, the largest river in Zhejiang province in eastern China, was measured to understand the chemical weathering of rocks and the associated CO2 consumption and anthropogenic influences within a silicate-dominated river basin. The average total dissolved solids (TDS, 113 mg l-1) and total cation concentration (TZ+, 1357 μeq l-1) of the river waters are comparable with those of global major rivers. Ca2+ and HCO3- followed by Na2+ and SO42-, dominate the ionic composition of the river water. There are four major reservoirs (carbonates, silicates, atmospheric and anthropogenic inputs) contributing to the total dissolved load of the investigated rivers. The dissolved loads of the rivers are dominated by both carbonate and silicate weathering, which together account for about 76.3% of the total cationic load origin. The cationic chemical weathering rates of silicate and carbonate for the Qiantangjiang basin are estimated to be approximately 4.9 ton km-2 a-1 and 13.9 ton km-2 a-1, respectively. The calculated CO2 consumption rates with the assumption that all the protons involved in the weathering reaction are provided by carbonic acid are 369 × 103 mol km-2 a-1 and 273 × 103 mol km-2 a-1 by carbonate and silicate weathering, respectively. As one of the most severe impacted area by acid rain in China, H2SO4 from acid precipitation is also an important proton donor in weathering reactions. When H2SO4 is considered, the CO2 consumption rates for the river basin are estimated at 286 × 103 mol km-2 a-1 for carbonate weathering and 211 × 103 mol km-2 a-1 for silicate weathering, respectively. The results highlight that the drawdown effect of CO2 consumption by carbonate and silicate weathering can be largely overestimated if the role of sulfuric acid is ignored, especially in the area heavily impacted by acid deposition like Qiantangjiang basin. The actual CO2 consumption rates (after sulfuric acid weathering effect

  12. Final Report: Development of a Chemical Model to Predict the Interactions between Supercritical CO2, Fluid and Rock in EGS Reservoirs

    SciTech Connect

    McPherson, Brian J.; Pan, Feng

    2014-09-24

    This report summarizes development of a coupled-process reservoir model for simulating enhanced geothermal systems (EGS) that utilize supercritical carbon dioxide as a working fluid. Specifically, the project team developed an advanced chemical kinetic model for evaluating important processes in EGS reservoirs, such as mineral precipitation and dissolution at elevated temperature and pressure, and for evaluating potential impacts on EGS surface facilities by related chemical processes. We assembled a new database for better-calibrated simulation of water/brine/ rock/CO2 interactions in EGS reservoirs. This database utilizes existing kinetic and other chemical data, and we updated those data to reflect corrections for elevated temperature and pressure conditions of EGS reservoirs.

  13. Catalysis for biomass and CO2 use through solar energy: opening new scenarios for a sustainable and low-carbon chemical production.

    PubMed

    Lanzafame, Paola; Centi, Gabriele; Perathoner, Siglinda

    2014-11-21

    The use of biomass, bio-waste and CO2 derived raw materials, the latter synthesized using H2 produced using renewable energy sources, opens new scenarios to develop a sustainable and low carbon chemical production, particularly in regions such as Europe lacking in other resources. This tutorial review discusses first this new scenario with the aim to point out, between the different possible options, those more relevant to enable this new future scenario for the chemical production, commenting in particular the different drivers (economic, technological and strategic, environmental and sustainability and socio-political) which guide the selection. The case of the use of non-fossil fuel based raw materials for the sustainable production of light olefins is discussed in more detail, but the production of other olefins and polyolefins, of drop-in intermediates and other platform molecules are also analysed. The final part discusses the role of catalysis in establishing this new scenario, summarizing the development of catalysts with respect to industrial targets, for (i) the production of light olefins by catalytic dehydration of ethanol and by CO2 conversion via FTO process, (ii) the catalytic synthesis of butadiene from ethanol, butanol and butanediols, and (iii) the catalytic synthesis of HMF and its conversion to 2,5-FDCA, adipic acid, caprolactam and 1,6-hexanediol.

  14. Particulate Formation from a Copper Oxide-Based Oxygen Carrier in Chemical Looping Combustion for CO2 Capture

    EPA Science Inventory

    Attrition behavior and particle loss of a copper oxide-based oxygen carrier from a methane chemical looping combustion (CLC) process was investigated in a fluidized bed reactor. The aerodynamic diameters of most elutriated particulates, after passing through a horizontal settling...

  15. CARBON COATED (CARBONOUS) CATALYST IN EBULLATED BED REACTOR FOR PRODUCTION OF OXYGENATED CHEMICALS FROM SYNGAS/CO2

    SciTech Connect

    Peizheng Zhou

    2001-10-26

    There are a number of exothermic chemical reactions which might benefit from the temperature control and freedom from catalyst fouling provided by the ebullated bed reactor technology. A particularly promising area is production of oxygenated chemicals, such as alcohols and ethers, from synthesis gas, which can be economically produced from coal or biomass. The ebullated bed operation requires that the small-diameter ({approx}1/32 inch) catalyst particles have enough mechanical strength to avoid loss by attrition. However, all of the State Of The Art (SOTA) catalysts and advanced catalysts for the purpose are low in mechanical strength. The patented carbon-coated catalyst technology developed in our laboratory converts catalyst particles with low mechanical strength to strong catalysts suitable for ebullated bed application. This R&D program is concerned with the modification on the mechanical strength of the SOTA and advanced catalysts so that the ebullated bed technology can be utilized to produce valuable oxygenated chemicals from syngas/CO{sub 2} efficiently and economically. The objective of this R&D program is to study the technical and economic feasibility of selective production of high-value oxygenated chemicals from synthesis gas and CO{sub 2} mixed feed in an ebullated bed reactor using carbon-coated catalyst particles.

  16. CARBON COATED (CARBONOUS) CATALYST IN EBULLATED BED REACTOR FOR PRODUCTION OF OXYGENATED CHEMICALS FROM SYNGAS/CO2

    SciTech Connect

    Peizheng Zhou

    2000-11-17

    There are a number of exothermic chemical reactions which might benefit from the temperature control and freedom from catalyst fouling provided by the ebullated bed reactor technology. A particularly promising area is production of oxygenated chemicals, such as alcohols and ethers, from synthesis gas, which can be economically produced from coal or biomass. The ebullated bed operation requires that the small-diameter ({approx} 1/32 inch) catalyst particles have enough mechanical strength to avoid loss by attrition. However, all of the State Of The Art (SOTA) catalysts and advanced catalysts for the purpose are low in mechanical strength. The patented carbon-coated catalyst technology developed in our laboratory converts catalyst particles with low mechanical strength to strong catalysts suitable for ebullated bed application. This R&D program is concerned with the modification on the mechanical strength of the SOTA and advanced catalysts so that the ebullated bed technology can be utilized to produce valuable oxygenated chemicals from syngas/CO{sub 2} efficiently and economically. The objective of this R&D program is to study the technical and economic feasibility of selective production of high-value oxygenated chemicals from synthesis gas and CO{sub 2} mixed feed in an ebullated bed reactor using carbon-coated catalyst particles.

  17. Numerical investigation of biogas diffusion flames characteristics under several operation conditions in counter-flow configuration with an emphasis on thermal and chemical effects of CO2 in the fuel mixture

    NASA Astrophysics Data System (ADS)

    Mameri, A.; Tabet, F.; Hadef, A.

    2017-03-01

    This study addresses the influence of several operating conditions (composition and ambient pressure) on biogas diffusion flame structure and NO emissions with particular attention on thermal and chemical effect of CO2. The biogas flame is modeled by a counter flow diffusion flame and analyzed in mixture fraction space using flamelet approach. The GRI Mech-3.0 mechanism that involves 53 species and 325 reactions is adopted for the oxidation chemistry. It has been observed that flame properties are very sensitive to biogas composition and pressure. CO2 addition decreases flame temperature by both thermal and chemical effects. Added CO2 may participate in chemical reaction due to thermal dissociation (chemical effect). Excessively supplied CO2 plays the role of pure diluent (thermal effect). The ambient pressure rise increases temperature and reduces flame thickness, radiation losses and dissociation amount. At high pressure, recombination reactions coupled with chain carrier radicals reduction, diminishes NO mass fraction.

  18. Hydrochemical and Isotopic Constraints on the Temporal and Spatial Variability of Chemical Weathering and CO2 Fluxes: An Example From the Australian Victorian Alps

    NASA Astrophysics Data System (ADS)

    Hagedorn, B.; Cartwright, I.

    2007-12-01

    Water from a network of 11 pristine rivers draining the Australian Victorian Alps was collected at different locations during (i) high discharge (June 2006) and (ii) low discharge (February 2007) conditions and was analyzed for dissolved major ions, δ2H and δ18O, and δ34S of dissolved sulphate. River water chemistry implies that solutes are largely derived from precipitation and chemical weathering of silicate lithologies. Cl/Br ratios as low as 30 molar suggest that rivers have not dissolved halite, however, higher salinity (≥100 mmol/L) winter samples have intermediate Cl/Br ratios (600 to 2000 molar) that are attributed to minor halite dissolution at the onset of the rainy season. Subsequent mixing of river water homogenizes ratios and evaporation is the dominant process that increases downstream salinities. Oxygen and Hydrogen isotopes also indicate that mixing and evaporation have occurred. Despite the lack of carbonate outcrops in the study area and uniform negative calcite saturation indices, the dissolution of hydrothermal calcite may account for up to 67% of the total dissolved cations, generating up to 92% of all dissolved Ca and Mg. The sulphur isotope data (16 to 20°CDT) indicates that the dissolved SO4 is derived predominantly from atmospheric deposition and minor gypsum weathering and not from bacterial reduction of FeS. This militates against sulphuric acid weathering in Victorian rivers. Si/(Na* + K*) ratios suggest that silicate weathering is dominated by the transformation of plagioclase (An40) to smectite and, to a lesser extend, the production of kaolinite. In total, chemical weathering consumes 17.6 x 106 (summer) to 71.59 x 106(winter) mol/km2/yr CO2, with the highest values in rivers draining the basement outcrops rather than sedimentary rocks. This range is at the upper end of the global scale and shows that the predominance of fresh silicate lithologies exerts the main control on higher CO2 fluxes; temperature and runoff, in turn, are

  19. CARBON COATED (CARBONOUS) CATALYST IN EBULLATED BED REACTOR FOR PRODUCTION OF OXYGENATED CHEMICALS FROM SYNGAS/CO2

    SciTech Connect

    Peizheng Zhou

    2002-12-30

    This report summarizes the work completed under DOE's Support of Advanced Fuel Research program, Contract No. DE-FG26-99FT40681. The contract period was October 2000 through September 2002. This R&D program investigated the modification of the mechanical strength of catalyst extrudates using Hydrocarbon Technologies, Inc. (HTI) carbon-coated catalyst technology so that the ebullated bed technology can be utilized to produce valuable oxygenated chemicals from syngas/CO{sub 2} efficiently and economically. Exothermic chemical reactions benefit from the temperature control and freedom from catalyst fouling provided by the ebullated bed reactor technology. The carbon-coated extrudates prepared using these procedures had sufficient attrition resistance and surface area for use in ebullated bed operation. The low cost of carbon coating makes the carbon-coated catalysts highly competitive in the market of catalyst extrudates.

  20. CO2-Neutral Fuels

    NASA Astrophysics Data System (ADS)

    Goede, Adelbert; van de Sanden, Richard

    2016-06-01

    Mimicking the biogeochemical cycle of System Earth, synthetic hydrocarbon fuels are produced from recycled CO2 and H2O powered by renewable energy. Recapturing CO2 after use closes the carbon cycle, rendering the fuel cycle CO2 neutral. Non-equilibrium molecular CO2 vibrations are key to high energy efficiency.

  1. Selecting CO2 Sources for CO2 Utilization by Environmental-Merit-Order Curves.

    PubMed

    von der Assen, Niklas; Müller, Leonard J; Steingrube, Annette; Voll, Philip; Bardow, André

    2016-02-02

    Capture and utilization of CO2 as alternative carbon feedstock for fuels, chemicals, and materials aims at reducing greenhouse gas emissions and fossil resource use. For capture of CO2, a large variety of CO2 sources exists. Since they emit much more CO2 than the expected demand for CO2 utilization, the environmentally most favorable CO2 sources should be selected. For this purpose, we introduce the environmental-merit-order (EMO) curve to rank CO2 sources according to their environmental impacts over the available CO2 supply. To determine the environmental impacts of CO2 capture, compression and transport, we conducted a comprehensive literature study for the energy demands of CO2 supply, and constructed a database for CO2 sources in Europe. Mapping these CO2 sources reveals that CO2 transport distances are usually small. Thus, neglecting transport in a first step, we find that environmental impacts are minimized by capturing CO2 first from chemical plants and natural gas processing, then from paper mills, power plants, and iron and steel plants. In a second step, we computed regional EMO curves considering transport and country-specific impacts for energy supply. Building upon regional EMO curves, we identify favorable locations for CO2 utilization with lowest environmental impacts of CO2 supply, so-called CO2 oases.

  2. Chemical weathering rate, denudation rate, and atmospheric and soil CO2 consumption of Paraná flood basalts in São Paulo State, Brazil

    NASA Astrophysics Data System (ADS)

    da Conceição, Fabiano Tomazini; dos Santos, Carolina Mathias; de Souza Sardinha, Diego; Navarro, Guillermo Rafael Beltran; Godoy, Letícia Hirata

    2015-03-01

    The chemical weathering rate and atmospheric/soil CO2 consumption of Paraná flood basalts in the Preto Stream basin, São Paulo State, Brazil, were evaluated using major elements as natural tracers. Surface and rain water samples were collected in 2006, and analyses were performed to assess pH, temperature, dissolved oxygen (DO), electrical conductivity (EC) and total dissolved solids (TDS), including SO42-, NO3-, PO43 -, HCO3-, Cl-, SiO2, Ca2 +, Mg2 +, Na+ and K+. Fresh rocks and C horizon samples were also collected, taking into account their geological context, abundance and spatial distribution, to analyze major elements and mineralogy. The Preto Stream, downstream from the city of Ribeirão Preto, receives several elements/compounds as a result of anthropogenic activities, with only sulfate yielding negative flux values. The negative flux of SO42 - can be attributed to atmospheric loading that is mainly related to anthropogenic inputs. After corrections were made for atmospheric inputs, the riverine transport of dissolved material was found to be 30 t km- 2 y- 1, with the majority of the dissolved material transported during the summer (wet) months. The chemical weathering rate and atmospheric/soil CO2 consumption were 6 m/Ma and 0.4 · 106 mol km- 2 y- 1, respectively. The chemical weathering rate falls within the lower range of Paraná flood basalt denudation rates between 135 and 35 Ma previously inferred from chronological studies. This comparison suggests that rates of basalt weathering in Brazil's present-day tropical climate differ by at most one order of magnitude from those prevalent at the time of hothouse Earth. The main weathering process is the monosiallitization of anorthoclase, augite, anorthite and microcline. Magnetite is not weathered and thus remains in the soil profile.

  3. Particulate Formation from a Copper Oxide-Based Oxygen Carrier in Chemical Looping Combustion for CO2 Capture.

    PubMed

    He, Feng; Linak, William P; Deng, Shuang; Li, Fanxing

    2017-02-21

    Attrition behavior and particle loss of a copper oxide-based oxygen carrier from a methane chemical looping combustion (CLC) process was investigated in a fluidized bed reactor. The aerodynamic diameters of most elutriated particulates, after passing through a horizontal settling duct, range between 2 and 5 μm. A notable number of submicrometer particulates are also identified. Oxygen carrier attrition was observed to lead to increased CuO loss resulting from the chemical looping reactions, i.e., Cu is enriched in small particles generated primarily from fragmentation in the size range of 10-75 μm. Cyclic reduction and oxidation reactions in CLC have been determined to weaken the oxygen carrier particles, resulting in increased particulate emission rates when compared to those of oxygen carriers without redox reactions. The generation rate for particulates <10 μm was found to decrease with progressive cycles over as-prepared oxygen carrier particles and then reach a steady state. The surface of the oxygen carrier is also found to be coarsened due to a Kirkendall effect, which also explains the enrichment of Cu on particle surfaces and in small particles.

  4. Supercritical CO2 extraction, chemical characterisation and antioxidant potential of Brassica oleracea var capitata against HO·, O2(·-) and ROO·.

    PubMed

    Dal Prá, Valéria; Dolwitsch, Carolina Bolssoni; da Silveira, Géssica Domingos; Porte, Liliane; Frizzo, Clarissa; Tres, Marcus Vinicius; Mossi, Vinicius; Mazutti, Marcio Antonio; do Nascimento, Paulo Cícero; Bohrer, Denise; de Carvalho, Leandro Machado; Viana, Carine; da Rosa, Marcelo Barcellos

    2013-12-15

    In this work were extracted bioactive compounds from Brassica oleracea var capitata using supercritical CO2 and evaluated the antioxidant potential of the extracts. Five extractions were accomplished to investigate the influence of pressure (10-25 MPa) and temperature (20-60 °C) in the extraction yield, chemical composition and antioxidant potential towards peroxyl, superoxide and hydroxyl radicals. The highest extraction yield was obtained at 60 °C and 25 MPa, which was 0.47 wt% (run 2). In the characterisation of the extracts obtained was possible the identification of sulforaphane and iberin nitrile that present known biological properties. The extracts of all runs presented antioxidant activities towards the three radicals, but the highest activities for all radicals were using the extracts obtained in the run 2. The use of supercritical CO2 extraction to obtain bioactive compounds of B. oleracea var capitata showed to be a promising alternative to conventional extraction methods, since allowed the extraction of compounds with scientific and industrial interest.

  5. Assessment of the biospheric contribution to surface atmospheric CO2 concentrations over East Asia with a regional chemical transport model

    NASA Astrophysics Data System (ADS)

    Kou, Xingxia; Zhang, Meigen; Peng, Zhen; Wang, Yinghong

    2015-03-01

    A regional chemical transport model, RAMS-CMAQ, was employed to assess the impacts of biosphere-atmosphere C2 exchange on seasonal variations in atmospheric C2 concentrations over East Asia. Simulated C2 concentrations were compared with observations at 12 surface stations and the comparison showed they were generally in good agreement. Both observations and simulations suggested that surface C2 over East Asia features a summertime trough due to biospheric absorption, while in some urban areas surface C2 has a distinct summer peak, which could be attributed to the strong impact from anthropogenic emissions. Analysis of the model results indicated that biospheric fluxes and fossil-fuel emissions are comparably important in shaping spatial distributions of C2 near the surface over East Asia. Biospheric flux plays an important role in the prevailing spatial pattern of C2 enhancement and reduction on the synoptic scale due to the strong seasonality of biospheric C2 flux. The elevation of C2 levels by the biosphere during winter was found to be larger than 5 ppm in North China and Southeast China, and during summertime a significant depletion (⩾ 7 ppm) occurred in most areas, except for the Indo-China Peninsula where positive bioflux values were found.

  6. Bosch CO2 Reduction System Development

    NASA Technical Reports Server (NTRS)

    Holmes, R. F.; King, C. D.; Keller, E. E.

    1976-01-01

    Development of a Bosch process CO2 reduction unit was continued, and, by means of hardware modifications, the performance was substantially improved. Benefits of the hardware upgrading were demonstrated by extensive unit operation and data acquisition in the laboratory. This work was accomplished on a cold seal configuration of the Bosch unit.

  7. Comprehensive structural and chemical (CO2, Fe/Fe Mg, H2O) investigations of Mg-Fe cordierite with micro Raman spectroscopy

    NASA Astrophysics Data System (ADS)

    Haefeker, U.; Kaindl, R.; Tropper, P.

    2012-04-01

    The Mg-Fe silicate cordierite with the idealized formula (Fe, Mg)2Al4Si5O18 occurs as a hexagonal and an orthorhombic polymorph with disordered/ordered Al-Si distribution on the tetrahedral sites. Most of the natural cordierites are fully ordered. Six-membered rings of (Si,Al)O4 are piled in the direction of the crystallographic c-axis and form channels, laterally and vertically linked by additional (Al, Si) tetrahedrons. Mg and Fe in varying fractions occupy the octahedrally coordinated M-sites. CO2 and H2O (and other volatiles) can be incorporated into the structural channels, thus cordierite can be used for paleofluid reconstruction. The vibration energies of incorporated volatiles, their interaction with the lattice and variations of certain lattice-vibration energies caused by the Mg-Fe exchange can be determined with Raman spectroscopy, allowing chemical quantifications and structural investigations. A method for the semi-quantitative determination of CO2-contents of natural cordierites by Kaindl et al. (2006) was optimized and enhanced by Haefeker et al. (2007). CO2 contents can be measured in single crystals and thin sections with an error of ± 0.05 - 0.09 wt.-%. Based on the Mg-Fe exchange with garnet, cordierite can be used as a geothermobarometer. Recent investigations of synthetic Mg-Fe cordierites with XFe = 0 - 1 have shown a linear downshift of six selected lattice peaks between 100 and 1250 cm-1 with the Mg-Fe contents. Correlation diagrams allow an estimation of the Mg-Fe contents in synthetic and natural samples. The experimental data are in good agreement with the results of quantum-mechanical calculations of the Raman spectra of Mg- and Fe cordierite (Kaindl et al., 2011) allowing the assignment of the peaks to specific vibrations of tetrahedral and octahedral sites. Natural Mg-Fe cordierites are mainly orthorhombic with a fully ordered Al/Si distribution on the tetrahedral sites. However, the disordered hexagonal polymorph is observed in many

  8. CO2 -Responsive polymers.

    PubMed

    Lin, Shaojian; Theato, Patrick

    2013-07-25

    This Review focuses on the recent progress in the area of CO2 -responsive polymers and provides detailed descriptions of these existing examples. CO2 -responsive polymers can be categorized into three types based on their CO2 -responsive groups: amidine, amine, and carboxyl groups. Compared with traditional temperature, pH, or light stimuli-responsive polymers, CO2 -responsive polymers provide the advantage to use CO2 as a "green" trigger as well as to capture CO2 directly from air. In addition, the current challenges of CO2 -responsive polymers are discussed and the different solution methods are compared. Noteworthy, CO2 -responsive polymers are considered to have a prosperous future in various scientific areas.

  9. CO2 laser modeling

    NASA Technical Reports Server (NTRS)

    Johnson, Barry

    1992-01-01

    The topics covered include the following: (1) CO2 laser kinetics modeling; (2) gas lifetimes in pulsed CO2 lasers; (3) frequency chirp and laser pulse spectral analysis; (4) LAWS A' Design Study; and (5) discharge circuit components for LAWS. The appendices include LAWS Memos, computer modeling of pulsed CO2 lasers for lidar applications, discharge circuit considerations for pulsed CO2 lidars, and presentation made at the Code RC Review.

  10. Adsorption of carbon dioxide (CO2) at S functionalized boron nitride (BN) and aluminum nitride (AlN) nanotubes (9, 0): A quantum chemical investigation

    NASA Astrophysics Data System (ADS)

    Najafi, Meysam

    2016-10-01

    We employed density functional theory to characterize CO2 adsorption on BNNT and AlNNT surfaces. The effects of S functionalization on the adsorption of CO2 gas on BNNT and AlNNT surfaces were investigated. Results reveal that adsorptions of CO2 on studied nanotubes were exothermic and experimentally possible from the energetic viewpoint. Results show that, Ead values of CO2 on AlNNT surface were more negative than corresponding values of BNNT. Results reveal that, S functionalization of studied nanotubes causes an increase in the absolute values of Ead of CO2 on surface of studied nanotubes. These results show that, there are good linearity dependencies between Ead and orbital energy values of studied nanotubes. Therefore we can conclude the Ead and orbital energy values are highly sensitive to the adsorption process which these may be used for the selection the suitable nanotubes with enhanced CO2 adsorption potential.

  11. Effects of xenon insertion into hydrogen bromide. Comparison of the electronic structure of the HBr···CO2 and HXeBr···CO2 complexes using quantum chemical topology methods: electron localization function, atoms in molecules and symmetry adapted perturbation theory.

    PubMed

    Makarewicz, Emilia; Gordon, Agnieszka J; Mierzwicki, Krzysztof; Latajka, Zdzislaw; Berski, Slawomir

    2014-06-05

    Quantum chemistry methods have been applied to study the influence of the Xe atom inserted into the hydrogen-bromine bond (HBr → HXeBr), particularly on the nature of atomic interactions in the HBr···CO2 and HXeBr···CO2 complexes. Detailed analysis of the nature of chemical bonds has been carried out using topological analysis of the electron localization function, while topological analysis of electron density was used to gain insight into the nature of weak nonbonding interactions. Symmetry-adapted perturbation theory within the orbital approach was applied for greater understanding of the physical contributions to the total interaction energy.

  12. Advanced Technologies for Monitoring CO2 Saturation and Pore Pressure in Geologic Formations: Linking the Chemical and Physical Effects to Elastic and Transport Properties

    SciTech Connect

    Mavko, G.; Vanorio, T.; Vialle, S.; Saxena, N.

    2014-03-31

    Ultrasonic P- and S-wave velocities were measured over a range of confining pressures while injecting CO2 and brine into the samples. Pore fluid pressure was also varied and monitored together with porosity during injection. Effective medium models were developed to understand the mechanisms and impact of observed changes and to provide the means for implementation of the interpretation methodologies in the field. Ultrasonic P- and S-wave velocities in carbonate rocks show as much as 20-50% decrease after injection of the reactive CO2-brine mixture; the changes were caused by permanent changes to the rock elastic frame associated with dissolution of mineral. Velocity decreases were observed under both dry and fluid-saturated conditions, and the amount of change was correlated with the initial pore fabrics. Scanning Electron Microscope images of carbonate rock microstructures were taken before and after injection of CO2-rich water. The images reveal enlargement of the pores, dissolution of micrite (micron-scale calcite crystals), and pitting of grain surfaces caused by the fluid- solid chemical reactivity. The magnitude of the changes correlates with the rock microtexture – tight, high surface area samples showed the largest changes in permeability and smallest changes in porosity and elastic stiffness compared to those in rocks with looser texture and larger intergranular pore space. Changes to the pore space also occurred from flow of fine particles with the injected fluid. Carbonates with grain-coating materials, such as residual oil, experienced very little permanent change during injection. In the tight micrite/spar cement component, dissolution is controlled by diffusion: the mass transfer of products and reactants is thus slow and the fluid is expected to be close to thermodynamical equilibrium with the calcite, leading to very little dissolution, or even precipitation. In the microporous rounded micrite and macropores, dissolution is controlled by

  13. Structurally simple complexes of CO2.

    PubMed

    Murphy, Luke J; Robertson, Katherine N; Kemp, Richard A; Tuononen, Heikki M; Clyburne, Jason A C

    2015-03-07

    The ability to bind CO2 through the formation of low-energy, easily-broken, bonds could prove invaluable in a variety of chemical contexts. For example, weak bonds to CO2 would greatly decrease the cost of the energy-intensive sorbent-regeneration step common to most carbon capture technologies. Furthermore, exploration of this field could lead to the discovery of novel CO2 chemistry. Reduction of complexed carbon dioxide might generate chemical feedstocks for the preparation of value-added products, particularly transportation fuels or fuel precursors. Implementation on a large scale could help to drastically reduce CO2 concentrations in the atmosphere. However, literature examples of weakly bonded complexes of CO2 are relatively few and true coordination complexes to a 'naked' CO2 fragment are nearly unheard of. In this review article, a variety of complexes of CO2 featuring diverse binding modes and reactivity will be examined. Topics covered include: (A) inclusion complexes of CO2 in porous materials. (B) Zwitterionic carbamates produced from the reaction of CO2 with polyamines. (C) Carbamate salts produced from reaction of CO2 with two equivalents of an amine. (D) Insertion products of CO2 into acid-base adducts (e.g., metal complexes). (E) Lewis acid-base activated CO2, such as frustrated Lewis pair complexes. (F) Simple base-CO2 adducts, wherein the base-CO2 bond is the only interaction formed. Complexes in the last category are of particular interest, and include imidazol-2-carboxylates (N-heterocyclic carbene adducts of CO2) as well as a few other examples that lie outside NHC chemistry.

  14. Vitamin B1-catalyzed acetoin formation from acetaldehyde: a key step for upgrading bioethanol to bulk C₄ chemicals.

    PubMed

    Lu, Ting; Li, Xiukai; Gu, Liuqun; Zhang, Yugen

    2014-09-01

    The production of bulk chemicals and fuels from renewable biobased feedstocks is of significant importance for the sustainability of human society. The production of ethanol from biomass has dramatically increased and bioethanol also holds considerable potential as a versatile building block for the chemical industry. Herein, we report a highly selective process for the conversion of ethanol to C4 bulk chemicals, such as 2,3-butanediol and butene, via a vitamin B1 (thiamine)-derived N-heterocyclic carbene (NHC)-catalyzed acetoin condensation as the key step to assemble two C2 acetaldehydes into a C4 product. The environmentally benign and cheap natural catalyst vitamin B1 demonstrates high selectivity (99%), high efficiency (97% yield), and high tolerance toward ethanol and water impurities in the acetoin reaction. The results enable a novel and efficient process for ethanol upgrading.

  15. Leaf structural characteristics are less important than leaf chemical properties in determining the response of leaf mass per area and photosynthesis of Eucalyptus saligna to industrial-age changes in [CO2] and temperature.

    PubMed

    Xu, Cheng-Yuan; Salih, Anya; Ghannoum, Oula; Tissue, David T

    2012-10-01

    The rise in atmospheric [CO(2)] is associated with increasing air temperature. However, studies on plant responses to interactive effects of [CO(2)] and temperature are limited, particularly for leaf structural attributes. In this study, Eucalyptus saligna plants were grown in sun-lit glasshouses differing in [CO(2)] (290, 400, and 650 µmol mol(-1)) and temperature (26 °C and 30 °C). Leaf anatomy and chloroplast parameters were assessed with three-dimensional confocal microscopy, and the interactive effects of [CO(2)] and temperature were quantified. The relative influence of leaf structural attributes and chemical properties on the variation of leaf mass per area (LMA) and photosynthesis within these climate regimes was also determined. Leaf thickness and mesophyll size increased in higher [CO(2)] but decreased at the warmer temperature; no treatment interaction was observed. In pre-industrial [CO(2)], warming reduced chloroplast diameter without altering chloroplast number per cell, but the opposite pattern (reduced chloroplast number per cell and unchanged chloroplast diameter) was observed in both current and projected [CO(2)]. The variation of LMA was primarily explained by total non-structural carbohydrate (TNC) concentration rather than leaf thickness. Leaf photosynthetic capacity (light- and [CO(2)]-saturated rate at 28 °C) and light-saturated photosynthesis (under growth [CO(2)] and temperature) were primarily determined by leaf nitrogen contents, while secondarily affected by chloroplast gas exchange surface area and chloroplast number per cell, respectively. In conclusion, leaf structural attributes are less important than TNC and nitrogen in affecting LMA and photosynthesis responses to the studied climate regimes, indicating that leaf structural attributes have limited capacity to adjust these functional traits in a changing climate.

  16. Chemical Formation of Methanol and Hydrocarbon ("Organic") Derivatives from CO2 and H2-Carbon Sources for Subsequent Biological Cell Evolution and Life's Origin.

    PubMed

    Olah, George A; Mathew, Thomas; Prakash, G K Surya

    2017-01-18

    Formation of methanol and hydrocarbon derivatives from CO2 and H2, their simplest molecular building blocks, under biocompatible conditions is proposed. Alternate panspermia of similar extraterrestrially formed and observed hydrocarbons to earth is also discussed. The simple molecular building blocks derived from CO2 and H2 are carbon sources in the initial stage of biological evolution of cells leading to life's origin.

  17. Evidence of the chemical reaction of (18)O-labelled nitrite with CO2 in aqueous buffer of neutral pH and the formation of (18)OCO by isotope ratio mass spectrometry.

    PubMed

    Tsikas, Dimitrios; Böhmer, Anke; Gros, Gerolf; Endeward, Volker

    2016-05-01

    Inorganic nitrite (NO2(-), ON-O(-) ←→ (-)O-NO) is the autoxidation product of nitric oxide (NO). Nitrite can also be formed from inorganic nitrate (ONO2(-)), the major oxidation product of NO in erythrocytes, by the catalytic action of bacterial nitrate reductase in gut and oral microflora. Nitrite can be reduced to NO by certain cellular proteins and enzymes, as well as in the gastric juice under acidic conditions. Hemoglobin, xanthine oxidoreductase and carbonic anhydrase (CA) have been reported to convert nitrite to NO. Renal CA isoforms are involved in the reabsorption of nitrite and may, therefore, play an important role in NO homeostasis. Yet, the mechanisms underlying the action of CA on nitrite are incompletely understood. The nitrate/nitrite system is regarded as a reservoir of NO. We have recently shown that nitrite reacts chemically with carbon dioxide (CO2), the regular substrate of CA. The present communication reports a stable isotope ratio mass spectrometry (IRMS) study on the reaction of NO2(-) and CO2 performed in 50 mM HEPES buffer of pH 7.4 at 37 °C. By using (18)O-labelled nitrite ((18)ON-O(-)/(-18)O-NO) and CO2 we observed formation of (18)O-labelled CO2. This finding is an unequivocal evidence of the chemical reaction of (18)ON-O(-)/(-18)O-NO with CO2. The reaction is rapid and involves nucleophilic attack of the negatively charged nitrite via one of its oxygen atoms on the partially positively charged CO2 molecule to form the putative intermediate (18)ON-O-CO2(-)/(-)O2C-(18)O-NO. The by far largest fraction of this intermediate decomposes back to (18)ON-O(-)/(-18)O-NO and CO2. A very small fraction of the intermediate, however, rearranges and finally decomposes to form (18)OCO and nitrite. This reaction is slower in the presence of an isolated erythrocytic CA isoform II. In summary, NO2(-), CO2 and CA are ubiquitous. The chemical reaction of NO2(-) with CO2 and its modulation by CA isoforms may play important roles in the transport of

  18. CO2 laser resurfacing.

    PubMed

    Fitzpatrick, R E

    2001-07-01

    The CO2 Laser offers a variety of unique features in resurfacing facial photodamage and acne scarring. These include hemostasis, efficient removal of the epidermis in a single pass, thermally induced tissue tightening, and safe, predictable tissue interaction. Knowledge of these mechanisms will result in the capability of using the CO2 laser effectively and safely whether the goal is superficial or deep treatment.

  19. CO2 blood test

    MedlinePlus

    Bicarbonate test; HCO3-; Carbon dioxide test; TCO2; Total CO2; CO2 test - serum ... Many medicines can interfere with blood test results. Your health care provider will tell you if you need to stop taking any medicines before you have this test. DO ...

  20. Synthetic biology for CO2 fixation.

    PubMed

    Gong, Fuyu; Cai, Zhen; Li, Yin

    2016-11-01

    Recycling of carbon dioxide (CO2) into fuels and chemicals is a potential approach to reduce CO2 emission and fossil-fuel consumption. Autotrophic microbes can utilize energy from light, hydrogen, or sulfur to assimilate atmospheric CO2 into organic compounds at ambient temperature and pressure. This provides a feasible way for biological production of fuels and chemicals from CO2 under normal conditions. Recently great progress has been made in this research area, and dozens of CO2-derived fuels and chemicals have been reported to be synthesized by autotrophic microbes. This is accompanied by investigations into natural CO2-fixation pathways and the rapid development of new technologies in synthetic biology. This review first summarizes the six natural CO2-fixation pathways reported to date, followed by an overview of recent progress in the design and engineering of CO2-fixation pathways as well as energy supply patterns using the concept and tools of synthetic biology. Finally, we will discuss future prospects in biological fixation of CO2.

  1. CO2 capture in different carbon materials.

    PubMed

    Jiménez, Vicente; Ramírez-Lucas, Ana; Díaz, José Antonio; Sánchez, Paula; Romero, Amaya

    2012-07-03

    In this work, the CO(2) capture capacity of different types of carbon nanofibers (platelet, fishbone, and ribbon) and amorphous carbon have been measured at 26 °C as at different pressures. The results showed that the more graphitic carbon materials adsorbed less CO(2) than more amorphous materials. Then, the aim was to improve the CO(2) adsorption capacity of the carbon materials by increasing the porosity during the chemical activation process. After chemical activation process, the amorphous carbon and platelet CNFs increased the CO(2) adsorption capacity 1.6 times, whereas fishbone and ribbon CNFs increased their CO(2) adsorption capacity 1.1 and 8.2 times, respectively. This increase of CO(2) adsorption capacity after chemical activation was due to an increase of BET surface area and pore volume in all carbon materials. Finally, the CO(2) adsorption isotherms showed that activated amorphous carbon exhibited the best CO(2) capture capacity with 72.0 wt % of CO(2) at 26 °C and 8 bar.

  2. Toward the understanding of chemical absorption processes for post-combustion capture of carbon dioxide: electronic and steric considerations from the kinetics of reactions of CO2(aq) with sterically hindered amines.

    PubMed

    Conway, William; Wang, Xiaoguang; Fernandes, Debra; Burns, Robert; Lawrance, Geoffrey; Puxty, Graeme; Maeder, Marcel

    2013-01-15

    The present study reports (a) the determination of both the kinetic rate constants and equilibrium constants for the reaction of CO(2)(aq) with sterically hindered amines and (b) an attempt to elucidate a fundamental chemical understanding of the relationship between the amine structure and chemical properties of the amine that are relevant for postcombustion capture of CO(2) (PCC) applications. The reactions of CO(2)(aq) with a series of linear and methyl substituted primary amines and alkanolamines have been investigated using stopped-flow spectrophotometry and (1)H NMR measurements at 25.0 °C. The specific mechanism of absorption for each of the amines, that is CO(2) hydration and/or carbamate formation, is examined and, based on the mechanism, the kinetic and equilibrium constants for the formation of carbamic acid/carbamates, including protonation constants of the carbamate, are reported for amines that follow this pathway. A Brønsted correlation relating the kinetic rate constants and equilibrium constants for the formation of carbamic acid/carbamates with the protonation constant of the amine is reported. Such a relationship facilitates an understanding of the effects of steric and electronic properties of the amine toward its reactivity with CO(2). Further, such relationships can be used to guide the design of new amines with improved properties relevant to PCC applications.

  3. Chemical vs Electrochemical Formation of Li2CO3 as a Discharge Product in Li-O2/CO2 Batteries by Controlling the Superoxide Intermediate.

    PubMed

    Yin, Wei; Grimaud, Alexis; Lepoivre, Florent; Yang, Chunzhen; Tarascon, Jean Marie

    2017-01-05

    The Li-O2/CO2 battery with high capacity has recently been proposed as a new protocol to convert CO2. However, the fundamental mechanism for the reaction still remains hazy. Here, we investigated the discharge processes of Li-O2/CO2 (70%/30%) batteries in two solvents, dimethyl sulfoxide (DMSO) and 1,2-dimethoxyethane (DME). During discharge, both solvents initially show the reduction of oxygen. However, afterward, the solvent affects the reaction pathways of superoxide species by solvating Li(+) with different strength, depending on the so-called donor number. More precisely, the initial formation of CO4(•-) is favored in DMSO at the expense of lithium superoxide formation that we observed in DME. Despite the different intermediate processes, X-ray diffraction showed that Li2CO3 was the final discharge product in both solvents. Moreover, we observed that CO2 cannot be reduced within the electrochemical stability window of DMSO and DME.

  4. Effect of chemical functionalization groups on Zr6-AzoBDC to enhance H2, CH4 storage and CO2 capture: a theoretical investigation

    NASA Astrophysics Data System (ADS)

    Trang, Khung M.; Pham, Hung Q.; Pham-Tran, Nguyen-Nguyen

    2015-09-01

    Grand canonical Monte Carlo (GCMC) simulation combined with the ideal adsorbed solution theory (IAST) and a statistical method were utilized to investigate the effect of functional groups on zirconium oxide based metal-organic frameworks (MOFs) Zr6-AzoBDC (Zr6A) for the gases (H2, CH4) adsorption property and CO2/CH4 selectivity under low pressure. The results showed that phenyl groups containing nitrogen (pyridine, pyrimidine) and thiophene group enhance the gas affinity with MOFs, therefore increasing both gravimetric and volumetric uptake. In addition, this behavior can also cause significantly improved selective capture of CO2 from CO2/CH4 gas mixtures. Among functional groups studied, the sulfonic acid group can potentially improve CH4, CO2 uptake and H2 isosteric heat of adsorption. These findings would play a vital role in designing new materials toward gas adsorption properties.

  5. Outsourcing CO2 Emissions

    NASA Astrophysics Data System (ADS)

    Davis, S. J.; Caldeira, K. G.

    2009-12-01

    CO2 emissions from the burning of fossil fuels are the primary cause of global warming. Much attention has been focused on the CO2 directly emitted by each country, but relatively little attention has been paid to the amount of emissions associated with consumption of goods and services in each country. This consumption-based emissions inventory differs from the production-based inventory because of imports and exports of goods and services that, either directly or indirectly, involved CO2 emissions. Using the latest available data and reasonable assumptions regarding trans-shipment of embodied carbon through third-party countries, we developed a global consumption-based CO2 emissions inventory and have calculated associated consumption-based energy and carbon intensities. We find that, in 2004, 24% of CO2 emissions are effectively outsourced to other countries, with much of the developed world outsourcing CO2 emissions to emerging markets, principally China. Some wealthy countries, including Switzerland and Sweden, outsource over half of their consumption-based emissions, with many northern Europeans outsourcing more than three tons of emissions per person per year. The United States is both a big importer and exporter of emissions embodied in trade, outsourcing >2.6 tons of CO2 per person and at the same time as >2.0 tons of CO2 per person are outsourced to the United States. These large flows indicate that CO2 emissions embodied in trade must be taken into consideration when considering responsibility for increasing atmospheric greenhouse gas concentrations.

  6. Porous materials with optimal adsorption thermodynamics and kinetics for CO2 separation.

    PubMed

    Nugent, Patrick; Belmabkhout, Youssef; Burd, Stephen D; Cairns, Amy J; Luebke, Ryan; Forrest, Katherine; Pham, Tony; Ma, Shengqian; Space, Brian; Wojtas, Lukasz; Eddaoudi, Mohamed; Zaworotko, Michael J

    2013-03-07

    The energy costs associated with the separation and purification of industrial commodities, such as gases, fine chemicals and fresh water, currently represent around 15 per cent of global energy production, and the demand for such commodities is projected to triple by 2050 (ref. 1). The challenge of developing effective separation and purification technologies that have much smaller energy footprints is greater for carbon dioxide (CO2) than for other gases; in addition to its involvement in climate change, CO2 is an impurity in natural gas, biogas (natural gas produced from biomass), syngas (CO/H2, the main source of hydrogen in refineries) and many other gas streams. In the context of porous crystalline materials that can exploit both equilibrium and kinetic selectivity, size selectivity and targeted molecular recognition are attractive characteristics for CO2 separation and capture, as exemplified by zeolites 5A and 13X (ref. 2), as well as metal-organic materials (MOMs). Here we report that a crystal engineering or reticular chemistry strategy that controls pore functionality and size in a series of MOMs with coordinately saturated metal centres and periodically arrayed hexafluorosilicate (SiF(2-)(6)) anions enables a 'sweet spot' of kinetics and thermodynamics that offers high volumetric uptake at low CO2 partial pressure (less than 0.15 bar). Most importantly, such MOMs offer an unprecedented CO2 sorption selectivity over N2, H2 and CH4, even in the presence of moisture. These MOMs are therefore relevant to CO2 separation in the context of post-combustion (flue gas, CO2/N2), pre-combustion (shifted synthesis gas stream, CO2/H2) and natural gas upgrading (natural gas clean-up, CO2/CH4).

  7. Hydrocarbonaceous material upgrading method

    DOEpatents

    Brecher, Lee E.; Mones, Charles G.; Guffey, Frank D.

    2015-06-02

    A hydrocarbonaceous material upgrading method may involve a novel combination of heating, vaporizing and chemically reacting hydrocarbonaceous feedstock that is substantially unpumpable at pipeline conditions, and condensation of vapors yielded thereby, in order to upgrade that feedstock to a hydrocarbonaceous material condensate that meets crude oil pipeline specification.

  8. Natural Analog for Geologic Storage of CO2: CO2 accumulation in China

    NASA Astrophysics Data System (ADS)

    Liu, L.; Xu, T.; Liu, N.; Zhou, B.

    2012-12-01

    Natural accumulations of CO2 are potential analogues of CO2 geological storage that can provide useful information on the behaviour of supercritical CO2 in reservoirs. Natural CO2 accumulations are common across Northeast China, and, although they occur in a wide variety of geological settings, their distribution is principally controlled by the Mesozoic-Cenozoic rift basins and associated Quaternary volcanism. High CO2 concentrations (>60 CO2%) in natural gas reservoirs are usually related to volcanism and magmatism, and possesses mantle-genetic origin. CO2 reservoirs consist of sandstone, volcanic rocks and carbonate rocks with the buried depth from 2000-3000 m. Dawsonite is recognized in almost all of the CO2-bearing basin, which has been proved to share the same carbon source with CO2 in the reservoirs in Songliao basin, Hailaer basin and Donghai basin. Petrographic data show that dawsonite is abundant in feldspar- rich sandstone, volcanic rock fragment-rich sandstones and tuff. In some cases, high percentage of dawsonite cement constitutes a diagenetic seal, which occurs in the reservoir-mudstone caprock and prevents upward leakage of CO2. Besides dawsonite, mantle-genetic CO2 flux leads to the formation of calcite, ankerite and siderite. The statistics of porosity and permeability measured from the dawsonite-bearing sandstone and dawsonite-absent sandstone with the almost same burial depth in Songliao basin show that the mantle-genetic CO2 flux result in lower reservoir quality, suggesting that mineral trapping for CO2 is significant. Chemical analyses of formation water in Songliao basin and Hailaer basin indicate that the concentrations of TDS, HCO3-,CO32-, Mg2+,Ca2+ and Na+ + K+ in dawsonite-bearing sandstone are higher than that in dawsonite-absent sandstone. Distribution of CO2 and dawsonite is constrainted by the regional caprocks in the Songliao basin. The charging time of the mantle-genetic CO2 in China dates from 50 to 25 Ma.

  9. Integrated supply chain design for commodity chemicals production via woody biomass fast pyrolysis and upgrading.

    PubMed

    Zhang, Yanan; Hu, Guiping; Brown, Robert C

    2014-04-01

    This study investigates the optimal supply chain design for commodity chemicals (BTX, etc.) production via woody biomass fast pyrolysis and hydroprocessing pathway. The locations and capacities of distributed preprocessing hubs and integrated biorefinery facilities are optimized with a mixed integer linear programming model. In this integrated supply chain system, decisions on the biomass chipping methods (roadside chipping vs. facility chipping) are also explored. The economic objective of the supply chain model is to maximize the profit for a 20-year chemicals production system. In addition to the economic objective, the model also incorporates an environmental objective of minimizing life cycle greenhouse gas emissions, analyzing the trade-off between the economic and environmental considerations. The capital cost, operating cost, and revenues for the biorefinery facilities are based on techno-economic analysis, and the proposed approach is illustrated through a case study of Minnesota, with Minneapolis-St. Paul serving as the chemicals distribution hub.

  10. How does the critical point change during a chemical reaction in supercritical fluids? A study of the hydroformylation of propene in supercritical CO(2).

    PubMed

    Ke, J; Han, B; George, M W; Yan, H; Poliakoff, M

    2001-04-25

    An understanding of homogeneous catalysis in supercritical fluids requires a knowledge of the phase behavior and the variation in critical point as the reaction proceeds. In this paper, the critical temperatures, T(c) and pressures, P(c), have been measured for a considerable number of mixtures representing the various stages of the hydroformylation reaction of propene in supercritical CO(2) and different reactant concentrations. Critical point data have also been measured for all of the binary mixtures of the components (CO(2), H(2), CO, propene, n- and isobutyraldehyde) which are not available from the literature or can be deduced from published data. We use the stoichiometry of the reacting system to simplify greatly the phase behavior problem by defining a path through the otherwise multidimensional "phase space". Satisfactory modeling of the data (0.3% in T(c) and 3.0% in P(c)) has been achieved using the Peng-Robinson equation of state and ignoring all binary interactions which do not involve CO(2). The model is used to explore the strategies needed to avoid phase separation in continuous and batch reactions. At a given temperature, a batch reactor may need to be run under much higher pressures than a flow reactor if single-phase conditions are to be preserved throughout the course of the reaction. Most of the critical point data were measured acoustically, but a selection of points were validated using more traditional view-cell procedures.

  11. Increased chemical weathering of olivine in high-energy shelf seas can counteract human CO2 emissions and ocean acidification against a price well below that of CCS and other methods

    NASA Astrophysics Data System (ADS)

    de Boer, Poppe L.; Schuiling, Roelof D.

    2014-05-01

    In the reaction: Mg(Fe)2SiO4 (olivine) + 4 H2O 2 Mg(Fe)2+ + 4 OH- + H4SiO4, followed by 4 OH- + 4 CO2 4 HCO3-, CO2 is consumed, and Mg2+, Fe2+, H4SiO4 and HCO3- are produced. Contrary to the paradigm that olivine weathering in nature is a slow process, flume experiments show a fast reaction, consuming CO2, and raising the pH at short notice. Only under static conditions a silica coating develops that retards the reaction. In high-energy shallow marine environments such silica coatings are abraded so that the chemical reaction can continue. When kept in motion even large olivine grains and gravels, rubbing and bumping against each other and against other sediment grains, weather quickly. Experiments show that fine micron- to silt-sized olivine particles are produced, and that the chemical reaction is fast. The chemical weathering of 7 km3 olivine is needed on a yearly basis in order to compensate the human CO2 emissions. This seems much, but is of the same order of magnitude as the volume of fossil fuels (in oil equivalents ~10 km3) that are burnt annually. Olivine is readily available at the Earth' surface on all continents, and such volume of 7 km3 is exceeded by existing mines; e.g. the Bingham Canyon open pit mine in Utah has an excavated volume of 25 km3. Hydrocarbons, on the other hand, are commonly retrieved with great efforts, from great depths, and often at remote locations. Spreading of large amounts of olivine (and/or serpentinite) in high-energy shelf seas where coarse sand and gravel can be transported, will counteract human CO2 production by fossil fuel burning and ocean acidification against a price well below that of other methods; order of US 10.- per ton CO2. For example part of the continental shelf between the Shetland Isles and France, that is the Southern Bight of the North Sea, the English Channel and the Irish Sea, is covered with sand waves, and in and around the English Channel an area of well over 100,000 km2 experiences bed shear stresses

  12. The Twelve Principles of CO2 CHEMISTRY.

    PubMed

    Poliakoff, Martyn; Leitner, Walter; Streng, Emilia S

    2015-01-01

    This paper introduces a set of 12 Principles, based on the acronym CO2 CHEMISTRY, which are intended to form a set of criteria for assessing the viability of different processes or reactions for using CO2 as a feedstock for making organic chemicals. The principles aim to highlight the synergy of Carbon Dioxide Utilisation (CDU) with the components of green and sustainable chemistry as well as briefly pointing out the connection to the energy sector.

  13. [Technology upgrades and exposure to chemical agents: results of the PPTP study in the footwear industry].

    PubMed

    Gianoli, Enrica; Brusoni, Daniela; Cornaggia, Nicoletta; Saretto, Gianni

    2012-01-01

    In the present work the chemical compositions of the products used in shoes manufacturing are reported. The data were collected over the period 2004-2007 in 156 shoe factories in Vigevano area during a study aiming the evaluation of safety conditions and occupational exposure to hazardous chemicals of the employees. The study was part of a regional project for "Occupational cancer prevention in the footwear industry". In the first phase of the study an information form on production cycle, products used and their composition was filled during preliminary audit. In the second phase of the study an in depth qualitative/quantitative evaluation of professional exposure was conducted in 13 selected shoe factories. Data analysis showed the increase in use of water-based adhesives at expense of solvent-based adhesives, the reduction to less than 3.5 weight %, and up to 1 weight %, of n-hexane concentration in solvent mixtures, the increase in use of products containing less hazardous ketones, esters, cyclohexane and heptane. Only in very few cases, products containing from 4 to 12 weight% of toluene were used. These data attest a positive trend in workers risks prevention in shoes industry.

  14. Regenerable Sorbent for CO2 Removal

    NASA Technical Reports Server (NTRS)

    Alptekin, Gokhan; Jayaraman, Ambal

    2013-01-01

    A durable, high-capacity regenerable sorbent can remove CO2 from the breathing loop under a Martian atmosphere. The system design allows near-ambient temperature operation, needs only a small temperature swing, and sorbent regeneration takes place at or above 8 torr, eliminating the potential for Martian atmosphere to leak into the regeneration bed and into the breathing loop. The physical adsorbent can be used in a metabolic, heat-driven TSA system to remove CO2 from the breathing loop of the astronaut and reject it to the Martian atmosphere. Two (or more) alternating sorbent beds continuously scrub and reject CO2 from the spacesuit ventilation loop. The sorbent beds are cycled, alternately absorbing CO2 from the vent loop and rejecting the adsorbed material into the environment at a high CO2 partial pressure (above 8 torr). The system does not need to run the adsorber at cryogenic temperatures, and uses a much smaller temperature swing. The sorbent removes CO2 via a weak chemical interaction. The interaction is strong enough to enable CO2 adsorption even at 3 to 7.6 torr. However, because the interaction between the surface adsorption sites and the CO2 is relatively weak, the heat input needed to regenerate the sorbent is much lower than that for chemical absorbents. The sorbent developed in this project could potentially find use in a large commercial market in the removal of CO2 emissions from coal-fired power plants, if regulations are put in place to curb carbon emissions from power plants.

  15. Silvering substrates after CO2 snow cleaning

    NASA Astrophysics Data System (ADS)

    Zito, Richard R.

    2005-09-01

    There have been some questions in the astronomical community concerning the quality of silver coatings deposited on substrates that have been cleaned with carbon dioxide snow. These questions center around the possible existence of carbonate ions left behind on the substrate by CO2. Such carbonate ions could react with deposited silver to produce insoluble silver carbonate, thereby reducing film adhesion and reflectivity. Carbonate ions could be produced from CO2 via the following mechanism. First, during CO2 snow cleaning, a small amount of moisture can condense on a surface. This is especially true if the jet of CO2 is allowed to dwell on one spot. CO2 gas can dissolve in this moisture, producing carbonic acid, which can undergo two acid dissociations to form carbonate ions. In reality, it is highly unlikely that charged carbonate ions will remain stable on a substrate for very long. As condensed water evaporates, Le Chatelier's principle will shift the equilibrium of the chain of reactions that produced carbonate back to CO2 gas. Furthermore, the hydration of CO2 reaction of CO2 with H20) is an extremely slow process, and the total dehydrogenation of carbonic acid is not favored. Living tissues that must carry out the equilibration of carbonic acid and CO2 use the enzyme carbonic anhydrase to speed up the reaction by a factor of one million. But no such enzymatic action is present on a clean mirror substrate. In short, the worst case analysis presented below shows that the ratio of silver atoms to carbonate radicals must be at least 500 million to one. The results of chemical tests presented here support this view. Furthermore, film lift-off tests, also presented in this report, show that silver film adhesion to fused silica substrates is actually enhanced by CO2 snow cleaning.

  16. The ATLAS IBL CO2 cooling system

    NASA Astrophysics Data System (ADS)

    Verlaat, B.; Ostrega, M.; Zwalinski, L.; Bortolin, C.; Vogt, S.; Godlewski, J.; Crespo-Lopez, O.; Van Overbeek, M.; Blaszcyk, T.

    2017-02-01

    The ATLAS Pixel detector has been equipped with an extra pixel layer in the space obtained by a smaller radius beam pipe. This new pixel layer called the Insertable B-Layer (IBL) was installed in 2014 and is operational in the current ATLAS data taking. The IBL detector is cooled with evaporative CO2 and is the first of its kind in ATLAS. The ATLAS IBL CO2 cooling system is designed for lower temperature operation (< ‑35oC) than the previous developed CO2 cooling systems in High Energy Physics experiments. The cold temperatures are required to protect the pixel sensors for the expected high radiation dose received at an integrated luminosity of 550 fb1. This paper describes the design, development, construction and commissioning of the IBL CO2 cooling system. It describes the challenges overcome and the important lessons learned for the development of future systems which are now under design for the Phase-II upgrade detectors.

  17. Engineered yeast for enhanced CO2 mineralization.

    PubMed

    Barbero, Roberto; Carnelli, Lino; Simon, Anna; Kao, Albert; Monforte, Alessandra d'Arminio; Riccò, Moreno; Bianchi, Daniele; Belcher, Angela

    2013-02-01

    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.

  18. Engineered yeast for enhanced CO2 mineralization†

    PubMed Central

    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

  19. CO2 laser preionisation

    NASA Technical Reports Server (NTRS)

    Spiers, Gary D.

    1991-01-01

    The final report for work done during the reporting period of January 25, 1990 to January 24, 1991 is presented. A literature survey was conducted to identify the required parameters for effective preionization in TEA CO2 lasers and the methods and techniques for characterizing preionizers are reviewed. A numerical model of the LP-140 cavity was used to determine the cause of the transverse mode stability improvement obtained when the cavity was lengthened. The measurement of the voltage and current discharge pulses on the LP-140 were obtained and their subsequent analysis resulted in an explanation for the low efficiency of the laser. An assortment of items relating to the development of high-voltage power supplies is also provided. A program for analyzing the frequency chirp data files obtained with the HP time and frequency analyzer is included. A program to calculate the theoretical LIMP chirp is also included and a comparison between experiment and theory is made. A program for calculating the CO2 linewidth and its dependence on gas composition and pressure is presented. The program also calculates the number of axial modes under the FWHM of the line for a given resonator length. A graphical plot of the results is plotted.

  20. Measuring Nitrous Oxide Mass Transfer into Non-Aqueous CO2BOL CO2 Capture Solvents

    SciTech Connect

    Whyatt, Greg A.; Freeman, Charles J.; Zwoster, Andy; Heldebrant, David J.

    2016-03-28

    This paper investigates CO2 absorption behavior in CO2BOL solvents by decoupling the physical and chemical effects using N2O as a non-reactive mimic. Absorption measurements were performed using a wetted-wall contactor. Testing was performed using a “first generation” CO2 binding organic liquid (CO2BOL), comprised of an independent base and alcohol. Measurements were made with N2O at a lean (0.06 mol CO2/mol BOL) and rich (0.26 mol CO2/mol BOL) loading, each at three temperatures (35, 45 and 55 °C). Liquid-film mass transfer coefficients (kg') were calculated by subtracting the gas film resistance – determined from a correlation from literature – from the overall mass transfer measurement. The resulting kg' values for N2O in CO2BOLs were found to be higher than that of 5 M aqueous MEA under comparable conditions, which is supported by published measurements of Henry’s coefficients for N2O in various solvents. These results suggest that the physical solubility contribution for CO2 absorption in CO2BOLs is greater than that of aqueous amines, an effect that may pertain to other non-aqueous solvents.

  1. An X-band Co2+ EPR study of Zn1-xCoxO (x=0.005-0.1) nanoparticles prepared by chemical hydrolysis methods using diethylene glycol and denaturated alcohol at 5 K

    NASA Astrophysics Data System (ADS)

    Misra, Sushil K.; Andronenko, S. I.; Srinivasa Rao, S.; Chess, Jordan; Punnoose, A.

    2015-11-01

    EPR investigations on two types of dilute magnetic semiconductor (DMS) ZnO nanoparticles doped with 0.5-10% Co2+ ions, prepared by two chemical hydrolysis methods, using: (i) diethylene glycol ((CH2CH2OH)2O) (NC-rod-like samples), and (ii) denatured ethanol (CH3CH2OH) solutions (QC-spherical samples), were carried out at X-band (9.5 GHz) at 5 K. The analysis of EPR data for NC samples revealed the presence of several types of EPR lines: (i) two types, intense and weak, of high-spin Co2+ ions in the samples with Co concentration >0.5%; (ii) surface oxygen vacancies, and (iii) a ferromagnetic resonance (FMR) line. QC samples exhibit an intense FMR line and an EPR line due to high-spin Co2+ ions. FMR line is more intense, than the corresponding line exhibited by NC samples. These EPR spectra varied for sample with different doping concentrations. The magnetic states of these samples as revealed by EPR spectra, as well as the origin of ferromagnetism DMS samples are discussed.

  2. CO2 Laser Market

    NASA Astrophysics Data System (ADS)

    Simonsson, Samuel

    1989-03-01

    It gives me a great deal of pleasure to introduce our final speaker of this morning's session for two reasons: First of all, his company has been very much in the news not only in our own community but in the pages of Wall Street Journal and in the world economic press. And, secondly, we would like to welcome him to our shores. He is a temporary resident of the United States, for a few months, forsaking his home in Germany to come here and help with the start up of a new company which we believe, probably, ranks #1 as the world supplier of CO2 lasers now, through the combination of former Spectra Physics Industrial Laser Division and Rofin-Sinar GMBH. Samuel Simonsson is the Chairman of the Board of Rofin-Sinar, Inc., here in the U.S. and managing director of Rofin-Sinar GMBH. It is a pleasure to welcome him.

  3. Capture and Sequestration of CO2 at the Boise White Paper Mill

    SciTech Connect

    B.P. McGrail; C.J. Freeman; G.H. Beeman; E.C. Sullivan; S.K. Wurstner; C.F. Brown; R.D. Garber; D. Tobin E.J. Steffensen; S. Reddy; J.P. Gilmartin

    2010-06-16

    This report documents the efforts taken to develop a preliminary design for the first commercial-scale CO2 capture and sequestration (CCS) project associated with biomass power integrated into a pulp and paper operation. The Boise Wallula paper mill is located near the township of Wallula in Southeastern Washington State. Infrastructure at the paper mill will be upgraded such that current steam needs and a significant portion of the current mill electric power are supplied from a 100% biomass power source. A new biomass power system will be constructed with an integrated amine-based CO2 capture plant to capture approximately 550,000 tons of CO2 per year for geologic sequestration. A customized version of Fluor Corporation’s Econamine Plus™ carbon capture technology will be designed to accommodate the specific chemical composition of exhaust gases from the biomass boiler. Due to the use of biomass for fuel, employing CCS technology represents a unique opportunity to generate a net negative carbon emissions footprint, which on an equivalent emissions reduction basis is 1.8X greater than from equivalent fossil fuel sources (SPATH and MANN, 2004). Furthermore, the proposed project will offset a significant amount of current natural gas use at the mill, equating to an additional 200,000 tons of avoided CO2 emissions. Hence, the total net emissions avoided through this project equates to 1,100,000 tons of CO2 per year. Successful execution of this project will provide a clear path forward for similar kinds of emissions reduction that can be replicated at other energy-intensive industrial facilities where the geology is suitable for sequestration. This project also represents a first opportunity for commercial development of geologic storage of CO2 in deep flood basalt formations. The Boise paper mill site is host to a Phase II pilot study being carried out under DOE’s Regional Carbon Partnership Program. Lessons learned from this pilot study and other separately

  4. Volatile Organic Compounds (VOCs) and Elevated Concentrations of Carbon Dioxide (CO2) in Unsaturated-Zone Vapors Near a Chemical and Low-Level Radioactivity Waste-Disposal Facility, Amargosa Desert Research Site, Nye County, Nevada

    NASA Astrophysics Data System (ADS)

    Baker, R. J.; Andraski, B. J.; Walvoord, M. A.; Stonestrom, D. A.; Prudic, D. E.; Luo, W.

    2003-12-01

    As part of its Toxic Substances Hydrology Program, the U.S. Geological Survey is studying contaminant-transport processes in an arid environment at the Amargosa Desert Research Site (http://nevada.usgs.gov/adrs/). The site is near waste-disposal facilities 20 kilometers east of Death Valley National Park. Low-level radioactive waste was buried in unlined trenches of varying depth during 1962-92. Hazardous chemical waste was buried in unlined trenches at an adjacent facility during 1970-88. Mean annual precipitation at the site from 1981 to 2000 was 108 millimeters. The unsaturated zone is aerobic down to the water table, which is about 110 m (meters) deep. Sampling infrastructure south and west of the facility includes a grid of vapor probes 1.5 m deep, a 23.8-m-deep background borehole (JFDB), and two approximately 100-m-deep boreholes (UZB-2 and UZB-3), which are 160 m and 100 m from the nearest trench, respectively, and are instrumented for multi-level sampling. Analytes detected in unsaturated-zone-vapor samples include elevated concentrations of tritium and carbon-14; three chlorofluorocarbon (CFC) compounds, eight chlorinated solvent compounds, and toluene, all at concentrations exceeding 1,000 parts per billion (ppb) in UZB-3, and at lower concentrations in UZB-2 and in the shallow-vapor-probe grid; and CO2 in concentrations up to 2% in UZB-3, whereas maximum CO2 concentrations in JFDB are less than 0.2%. With the notable exception of toluene, VOCs that are known to be highly biodegradable are generally absent or occur at low concentrations (<100 ppb). The trends in the CO2 concentration profiles approximately parallel those of CFCs and radionuclides. The following preliminary conclusions have been drawn from the radionuclide, VOC, and CO2 data: 1. Biodegradation of organic substances is a reasonable explanation for the presence of CO2 in UZB-3 at concentrations greater those in JFDB (background), which are attributed to near-surface natural biological

  5. Acid Gas Capture Using CO2-Binding Organic Liquids

    SciTech Connect

    Heldebrant, David J.; Koech, Phillip K.; Rainbolt, James E.; Zheng, Feng

    2010-11-10

    Current chemical CO2 scrubbing technology is primarily aqueous alkanolamine based. These systems rapidly bind CO2 (forming water-soluble carbamate and bicarbonate salts) however, the process has serious disadvantages. The concentration of monoethanolamine rarely exceeds 30 wt % due to the corrosive nature of the solution, and this reduces the maximum CO2 volumetric (≤108 g/L) and gravimetric capacity (≤7 wt%) of the CO2 scrubber. The ≤30 wt % loading of ethanolamine also means that a large excess of water must be pumped and heated during CO2 capture and release, and this greatly increases the energy requirements especially considering the high specific heat of water (4 j/g-1K-1). Our approach is to switch to organic systems that chemically bind CO2 as liquid alkylcarbonate salts. Our CO2-binding organic liquids have higher CO2 solubility, lower specific heats, potential for less corrosion and lower binding energies for CO2 than aqueous systems. CO2BOLs also reversibly bind and release mixed sulfur oxides. Furthermore the CO2BOL system can be direct solvent replacements for any solvent based CO2 capture systems because they are commercially available reagents and because they are fluids they would not require extensive process re-engineering.

  6. Physical and Chemical Effects of Two-Phase Brine/Supercritical-CO2 Fluid Flow on Clastic Rocks: Real-Time Monitoring and NMR Imaging of Flow-Through Core Experiments

    NASA Astrophysics Data System (ADS)

    Shaw, C. A.; Vogt, S.; Maneval, J. E.; Brox, T.; Skidmore, M. L.; Codd, S. L.; Seymour, J. D.

    2010-12-01

    Sandstone core samples were challenged with a supercritical CO2-saturated brine mixture in a laboratory flow-through core reactor system over a range of temperatures and brine strengths. Cores of quartz arenite from the Berea formation were selected to represent ideal ‘clean’ sandstone These laboratory experiments potentially provide an analog for the acidification of pore fluids near the brine/CO2 interface during CO2 flooding of depleted clastic hydrocarbon reservoirs for carbon sequestration. Flow in the reactor was perpendicular to bedding. Initial experiments were run at 50°C and 100°C with brine concentrations of 1g/L and 10g/L (TDS) to test effects of different temperatures and brine compositions. Real-time monitoring of fluid pH and conductivity provided a measure of reaction rates. Introduction of supercritical CO2 into the brine-saturated cores initiated a reduction in pH accompanied by an increase in conductivity. NMR images of fresh cores were compared with images of challenged cores using a protocol for pixel-by-pixel comparison to determine the effects on bulk pore volume and geometry. Two types of imaging experiments were conducted: multi-slice spin echo and 3-D spin echo images. Multi-slice experiments had a slice thickness of 1.5 mm and an in-plane resolution of 0.27 mm x 0.27 mm, and 3-D experiments had a resolution of 0.47 mm x 0.55 mm x 0.55mm. Imaging results reflected the observed changes in the physical and chemical structure post-challenge. Two-dimensional relaxation correlation experiments were also conducted to probe the pore sizes, connectivity and fluid saturation of the rock cores before and after challenging. Chemical analyses and microscopic examination of the challenged cores will provide a better understanding of alteration in the cores and the changes in the volume, geometry and connectivity of pore space.

  7. Forecasting global atmospheric CO2

    NASA Astrophysics Data System (ADS)

    Agustí-Panareda, A.; Massart, S.; Chevallier, F.; Boussetta, S.; Balsamo, G.; Beljaars, A.; Ciais, P.; Deutscher, N. M.; Engelen, R.; Jones, L.; Kivi, R.; Paris, J.-D.; Peuch, V.-H.; Sherlock, V.; Vermeulen, A. T.; Wennberg, P. O.; Wunch, D.

    2014-11-01

    A new global atmospheric carbon dioxide (CO2) real-time forecast is now available as part of the pre-operational Monitoring of Atmospheric Composition and Climate - Interim Implementation (MACC-II) service using the infrastructure of the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecasting System (IFS). One of the strengths of the CO2 forecasting system is that the land surface, including vegetation CO2 fluxes, is modelled online within the IFS. Other CO2 fluxes are prescribed from inventories and from off-line statistical and physical models. The CO2 forecast also benefits from the transport modelling from a state-of-the-art numerical weather prediction (NWP) system initialized daily with a wealth of meteorological observations. This paper describes the capability of the forecast in modelling the variability of CO2 on different temporal and spatial scales compared to observations. The modulation of the amplitude of the CO2 diurnal cycle by near-surface winds and boundary layer height is generally well represented in the forecast. The CO2 forecast also has high skill in simulating day-to-day synoptic variability. In the atmospheric boundary layer, this skill is significantly enhanced by modelling the day-to-day variability of the CO2 fluxes from vegetation compared to using equivalent monthly mean fluxes with a diurnal cycle. However, biases in the modelled CO2 fluxes also lead to accumulating errors in the CO2 forecast. These biases vary with season with an underestimation of the amplitude of the seasonal cycle both for the CO2 fluxes compared to total optimized fluxes and the atmospheric CO2 compared to observations. The largest biases in the atmospheric CO2 forecast are found in spring, corresponding to the onset of the growing season in the Northern Hemisphere. In the future, the forecast will be re-initialized regularly with atmospheric CO2 analyses based on the assimilation of CO2 products retrieved from satellite measurements and

  8. Forecasting global atmospheric CO2

    NASA Astrophysics Data System (ADS)

    Agustí-Panareda, A.; Massart, S.; Chevallier, F.; Boussetta, S.; Balsamo, G.; Beljaars, A.; Ciais, P.; Deutscher, N. M.; Engelen, R.; Jones, L.; Kivi, R.; Paris, J.-D.; Peuch, V.-H.; Sherlock, V.; Vermeulen, A. T.; Wennberg, P. O.; Wunch, D.

    2014-05-01

    A new global atmospheric carbon dioxide (CO2) real-time forecast is now available as part of the pre-operational Monitoring of Atmospheric Composition and Climate - Interim Implementation (MACC-II) service using the infrastructure of the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecasting System (IFS). One of the strengths of the CO2 forecasting system is that the land surface, including vegetation CO2 fluxes, is modelled online within the IFS. Other CO2 fluxes are prescribed from inventories and from off-line statistical and physical models. The CO2 forecast also benefits from the transport modelling from a state-of-the-art numerical weather prediction (NWP) system initialized daily with a wealth of meteorological observations. This paper describes the capability of the forecast in modelling the variability of CO2 on different temporal and spatial scales compared to observations. The modulation of the amplitude of the CO2 diurnal cycle by near-surface winds and boundary layer height is generally well represented in the forecast. The CO2 forecast also has high skill in simulating day-to-day synoptic variability. In the atmospheric boundary layer, this skill is significantly enhanced by modelling the day-to-day variability of the CO2 fluxes from vegetation compared to using equivalent monthly mean fluxes with a diurnal cycle. However, biases in the modelled CO2 fluxes also lead to accumulating errors in the CO2 forecast. These biases vary with season with an underestimation of the amplitude of the seasonal cycle both for the CO2 fluxes compared to total optimized fluxes and the atmospheric CO2 compared to observations. The largest biases in the atmospheric CO2 forecast are found in spring, corresponding to the onset of the growing season in the Northern Hemisphere. In the future, the forecast will be re-initialized regularly with atmospheric CO2 analyses based on the assimilation of CO2 satellite retrievals, as they become available in

  9. CO2 laser cutting of natural granite

    NASA Astrophysics Data System (ADS)

    Riveiro, A.; Mejías, A.; Soto, R.; Quintero, F.; del Val, J.; Boutinguiza, M.; Lusquiños, F.; Pardo, J.; Pou, J.

    2016-01-01

    Commercial black granite boards (trade name: "Zimbabwe black granite") 10 mm thick, were successfully cut by a 3.5 kW CO2 laser source. Cutting quality, in terms of kerf width and roughness of the cut wall, was assessed by means of statistically planned experiments. No chemical modification of the material in the cutting walls was detected by the laser beam action. Costs associated to the process were calculated, and the main factors affecting them were identified. Results reported here demonstrate that cutting granite boards could be a new application of CO2 laser cutting machines provided a supersonic nozzle is used.

  10. Development of Novel CO2 Adsorbents for Capture of CO2 from Flue Gas

    SciTech Connect

    Fauth, D.J.; Filburn, T.P.; Gray, M.L.; Hedges, S.W.; Hoffman, J.; Pennline, H.W.; Filburn, T.

    2007-06-01

    Capturing CO2 emissions generated from fossil fuel-based power plants has received widespread attention and is considered a vital course of action for CO2 emission abatement. Efforts are underway at the Department of Energy’s National Energy Technology Laboratory to develop viable energy technologies enabling the CO2 capture from large stationary point sources. Solid, immobilized amine sorbents (IAS) formulated by impregnation of liquid amines within porous substrates are reactive towards CO2 and offer an alternative means for cyclic capture of CO2 eliminating, to some degree, inadequacies related to chemical absorption by aqueous alkanolamine solutions. This paper describes synthesis, characterization, and CO2 adsorption properties for IAS materials previously tested to bind and release CO2 and water vapor in a closed loop life support system. Tetraethylenepentamine (TEPA), acrylonitrile-modified tetraethylenepentamine (TEPAN), and a single formulation consisting of TEPAN and N, N’-bis(2-hydroxyethyl)ethylenediamine (BED) were individually supported on a poly (methyl methacrylate) (PMMA) substrate and examined. CO2 adsorption profiles leading to reversible CO2 adsorption capacities were obtained using thermogravimetry. Under 10% CO2 in nitrogen at 25°C and 1 atm, TEPA supported on PMMA over 60 minutes adsorbed ~3.2 mmol/g{sorbent} whereas, TEPAN supported on PMMA along with TEPAN and BED supported on PMMA adsorbed ~1.7 mmol/g{sorbent} and ~2.3 mmol/g{sorbent} respectively. Cyclic experiments with a 1:1 weight ratio of TEPAN and BED supported on poly (methyl methacrylate) beads utilizing a fixed-bed flow system with 9% CO2, 3.5% O2, nitrogen balance with trace gas constituents were studied. CO2 adsorption capacity was ~ 3 mmols CO2/g{sorbent} at 40°C and 1.4 atm. No beneficial effect on IAS performance was found using a moisture-laden flue gas mixture. Tests with 750 ppmv NO in a humidified gas stream revealed negligible NO sorption onto the IAS. A high SO2

  11. CO2 adsorption isotherm on clay minerals and the CO2 accessibility into the clay interlayer

    NASA Astrophysics Data System (ADS)

    Gensterblum, Yves; Bertier, Pieter; Busch, Andreas; Rother, Gernot; Krooß, Bernhard

    2013-04-01

    Large-scale CO2 storage in porous rock formations at 1-3 km depth is seen as a global warming mitigation strategy. In this process, CO2 is separated from the flue gas of coal or gas power plants, compressed, and pumped into porous subsurface reservoirs with overlying caprocks (seals). Good seals are mechanically and chemically stable caprocks with low porosity and permeability. They prevent leakage of buoyant CO2 from the reservoir. Caprocks are generally comprised of thick layers of shale, and thus mainly consist of clay minerals. These clays can be affected by CO2-induced processes, such as swelling or dissolution. The interactions of CO2 with clay minerals in shales are at present poorly understood. Sorption measurements in combination scattering techniques could provide fundamental insight into the mechanisms governing CO2-clay interaction. Volumetric sorption techniques have assessed the sorption of supercritical CO2 onto coal (Gensterblum et al., 2010; Gensterblum et al., 2009), porous silica (Rother et al., 2012a) and clays as a means of exploring the potential of large-scale storage of anthropogenic CO2 in geological reservoirs (Busch et al., 2008). On different clay minerals and shales, positive values of excess sorption were measured at gas pressures up to 6 MPa, where the interfacial fluid is assumed to be denser than the bulk fluid. However, zero and negative values were obtained at higher densities, which suggests the adsorbed fluid becomes equal to and eventually less dense than the corresponding bulk fluid, or that the clay minerals expand on CO2 charging. Using a combination of neutron diffraction and excess sorption measurements, we recently deduced the interlayer density of scCO2 in Na-montmorillonite clay in its single-layer hydration state (Rother et al., 2012b), and confirmed its low density, as well as the expansion of the basal spacings. We performed neutron diffraction experiments at the FRMII diffractometer on smectite, kaolinite and illite

  12. Hydrogen production with CO 2 capture by coupling steam reforming of methane and chemical-looping combustion: Use of an iron-based waste product as oxygen carrier burning a PSA tail gas

    NASA Astrophysics Data System (ADS)

    Ortiz, María; Gayán, Pilar; de Diego, Luis F.; García-Labiano, Francisco; Abad, Alberto; Pans, Miguel A.; Adánez, Juan

    In this work it is analyzed the performance of an iron waste material as oxygen carrier for a chemical-looping combustion (CLC) system. CLC is a novel combustion technology with the benefit of inherent CO 2 separation that can be used as a source of energy for the methane steam reforming process (SR). The tail gas from the PSA unit is used as fuel in the CLC system. The oxygen carrier behaviour with respect to gas combustion was evaluated in a continuous 500 W th CLC prototype using a simulated PSA off-gas stream as fuel. Methane or syngas as fuel were also studied for comparison purposes. The oxygen carrier showed enough high oxygen transport capacity and reactivity to fully convert syngas at 880 °C. However, lower conversion of the fuel was observed with methane containing fuels. An estimated solids inventory of 1600 kg MW th -1 would be necessary to fully convert the PSA off-gas to CO 2 and H 2O. An important positive effect of the oxygen carrier-to-fuel ratio up to 1.5 and the reactor temperature on the combustion efficiency was found. A characterization of the calcined and after-used particles was carried out showing that this iron-based material can be used as oxygen carrier in a CLC plant since particles maintain their properties (reactivity, no agglomeration, high durability, etc.) after more than 111 h of continuous operation.

  13. Is CO2 ice permanent?

    NASA Technical Reports Server (NTRS)

    Lindner, Bernhard Lee

    1992-01-01

    Carbon dioxide ice has been inferred to exist at the south pole in summertime, but Earth based measurements in 1969 of water vapor in the Martian atmosphere suggest that all CO2 ice sublined from the southern polar cap and exposed underlying water ice. This implies that the observed summertime CO2 ice is of recent origin. It appears possible to construct an energy balance model that maintains seasonal CO2 ice at the south pole year round and still reasonably simulates the polar cap regression and atmospheric pressure data. This implies that the CO2 ice observed in the summertime south polar cap could be seasonal in origin, and that minor changes in climate could cause CO2 ice to completely vanish, as would appear to have happened in 1969. However, further research remains before it is certain whether the CO2 ice observed in the summertime south polar cap is seasonal or is part of a permanent reservoir.

  14. Co2 geological sequestration

    SciTech Connect

    Xu, Tianfu

    2004-11-18

    Human activities are increasingly altering the Earth's climate. A particular concern is that atmospheric concentrations of carbon dioxide (CO{sub 2}) may be rising fast because of increased industrialization. CO{sub 2} is a so-called ''greenhouse gas'' that traps infrared radiation and may contribute to global warming. Scientists project that greenhouse gases such as CO{sub 2} will make the arctic warmer, which would melt glaciers and raise sea levels. Evidence suggests that climate change may already have begun to affect ecosystems and wildlife around the world. Some animal species are moving from one habitat to another to adapt to warmer temperatures. Future warming is likely to exceed the ability of many species to migrate or adjust. Human production of CO{sub 2} from fossil fuels (such as at coal-fired power plants) is not likely to slow down soon. It is urgent to find somewhere besides the atmosphere to put these increased levels of CO{sub 2}. Sequestration in the ocean and in soils and forests are possibilities, but another option, sequestration in geological formations, may also be an important solution. Such formations could include depleted oil and gas reservoirs, unmineable coal seams, and deep saline aquifers. In many cases, injection of CO2 into a geological formation can enhance the recovery of hydrocarbons, providing value-added byproducts that can offset the cost of CO{sub 2} capture and sequestration. Before CO{sub 2} gas can be sequestered from power plants and other point sources, it must be captured. CO{sub 2} is also routinely separated and captured as a by-product from industrial processes such as synthetic ammonia production, H{sub 2} production, and limestone calcination. Then CO{sub 2} must be compressed into liquid form and transported to the geological sequestration site. Many power plants and other large emitters of CO{sub 2} are located near geological formations that are amenable to CO{sub 2} sequestration.

  15. CO2 interaction with geomaterials.

    SciTech Connect

    Guthrie, George D.; Al-Saidi, Wissam A.; Jordan, Kenneth D.; Voora, Vamsee, K.; Romanov, Vyacheslav N.; Lopano, Christina L; Myshakin, Eugene M.; Hur, Tae Bong; Warzinski, Robert P.; Lynn, Ronald J.; Howard, Bret H.; Cygan, Randall Timothy

    2010-09-01

    This work compares the sorption and swelling processes associated with CO2-coal and CO2-clay interactions. We investigated the mechanisms of interaction related to CO2 adsortion in micropores, intercalation into sub-micropores, dissolution in solid matrix, the role of water, and the associated changes in reservoir permeability, for applications in CO2 sequestration and enhanced coal bed methane recovery. The structural changes caused by CO2 have been investigated. A high-pressure micro-dilatometer was equipped to investigate the effect of CO2 pressure on the thermoplastic properties of coal. Using an identical dilatometer, Rashid Khan (1985) performed experiments with CO2 that revealed a dramatic reduction in the softening temperature of coal when exposed to high-pressure CO2. A set of experiments was designed for -20+45-mesh samples of Argonne Premium Pocahontas No.3 coal, which is similar in proximate and ultimate analysis to the Lower Kittanning seam coal that Khan used in his experiments. No dramatic decrease in coal softening temperature has been observed in high-pressure CO2 that would corroborate the prior work of Khan. Thus, conventional polymer (or 'geopolymer') theories may not be directly applicable to CO2 interaction with coals. Clays are similar to coals in that they represent abundant geomaterials with well-developed microporous structure. We evaluated the CO2 sequestration potential of clays relative to coals and investigated the factors that affect the sorption capacity, rates, and permanence of CO2 trapping. For the geomaterials comparison studies, we used source clay samples from The Clay Minerals Society. Preliminary results showed that expandable clays have CO2 sorption capacities comparable to those of coal. We analyzed sorption isotherms, XRD, DRIFTS (infrared reflectance spectra at non-ambient conditions), and TGA-MS (thermal gravimetric analysis) data to compare the effects of various factors on CO2 trapping. In montmorillonite, CO2

  16. Reinforced photocatalytic reduction of CO2 to CO by a ternary metal oxide NiCo2O4.

    PubMed

    Wang, Zhaoyu; Jiang, Min; Qin, Jiani; Zhou, Han; Ding, Zhengxin

    2015-06-28

    The work reported herein was the facile preparation of uniform urchin-like NiCo2O4 microspheres, and their use as an efficient and stable cocatalyst for photocatalytic CO2 reduction catalysis. A combined solvothermal-calcination strategy was applied to synthesize the NiCo2O4 material that was systematically characterized by physical and chemical measurements (e.g. SEM, TEM, XRD, XPS, EDX, elemental mapping and N2 physisorption analysis). By cooperation with a visible light photosensitizer, the NiCo2O4 material effectively promoted the deoxygenative reduction of CO2 to CO by more than twenty times under mild reaction conditions. The carbon origin of CO evolution was validated by (13)CO2 isotope tracer experiments. Various reaction parameters were examined and optimized, and a possible reaction mechanism was proposed. Furthermore, the stability and reusability of NiCo2O4 cocatalysts were firmly confirmed.

  17. Elevated CO(2) and drought stress effects on the chemical composition of maize plants, their ruminal fermentation and microbial diversity in vitro.

    PubMed

    Meibaum, Birgit; Riede, Susanne; Schröder, Bernd; Manderscheid, Remy; Weigel, Hans-Joachim; Breves, Gerhard

    2012-12-01

    Climate changes are supposed to influence productivity and chemical composition of plants. In the present experiments, it was hypothesised that the incubation of plants exposed to elevated atmospheric carbon dioxide concentrations ([CO₂]) and drought stress will result in different ruminal fermentation pattern and microbial diversity compared to unaffected plants. Maize plants were grown, well-watered under ambient (380 ppm CO₂, Variant A) and elevated [CO₂] (550 ppm CO₂, Variant B). Furthermore, each CO₂ treatment was also exposed to drought stress (380 ppm and 550 ppm CO₂,Variants C and D, respectively), which received only half as much water as the well-watered plants. Plant material from these treatments was incubated in a semi-continuous in vitro fermentation experiment using the rumen simulation technique. Single strand conformation polymorphism (SSCP) analysis was conducted for Bacteria and Archaea specific profiles. The analysis of crude nutrients showed higher contents of fibre fraction in drought stress Variants C and D. Crude protein content was increased by drought stress under ambient but not under elevated [CO₂]. Fermentation of drought stress variants resulted in significantly increased pH values, decreased digestibilities of organic matter and increased ammonia-N (NH₃-N) concentrations compared with well-watered variants. Additionally, the 550 ppm CO₂ Variants B and D showed significantly lower NH₃-N concentrations than Variants A and C. The Bacteria- and Archaea-specific SSCP profiles as well as the production rates of short-chain fatty acids and their molar percentages were not affected by treatments. During the first four days of equilibration period, a decrease of molar percentage of acetate and increased molar percentages of propionate were observed for all treatments. These alterations might have been induced by adaptation of the in vitro system to the new substrate. The rumen microflora appeared to be highly adaptive and

  18. Enhancing CO2 Capture using Robust Superomniphobic Membranes.

    PubMed

    Geyer, Florian; Schönecker, Clarissa; Butt, Hans-Jürgen; Vollmer, Doris

    2017-02-01

    Superomniphobic membranes for post-combustion CO2 capture are introduced. Concentrated aqueous amine solutions stay on the topmost part of the membranes, providing a large liquid/CO2 interface. Wetting of the membrane, which reduces the capture efficiency, is prevented. The CO2 capture rates using the chemically, mechanically, and thermally stable superomniphobic membranes are enhanced by up to 40% relative to commercial membranes.

  19. Vertical transport rates and concentrations of OH and Cl radicals in the Tropical Tropopause Layer from observations of CO2 and halocarbons: implications for distributions of long- and short-lived chemical species

    NASA Astrophysics Data System (ADS)

    Park, S.; Atlas, E. L.; Jiménez, R.; Daube, B. C.; Gottlieb, E. W.; Nan, J.; Jones, D. B. A.; Pfister, L.; Conway, T. J.; Bui, T. P.; Gao, R.-S.; Wofsy, S. C.

    2010-07-01

    Rates for large-scale vertical transport of air in the Tropical Tropopause Layer (TTL) were determined using high-resolution, in situ observations of CO2 concentrations in the tropical upper troposphere and lower stratosphere during the NASA Tropical Composition, Cloud and Climate Coupling (TC4) campaign in August 2007. Upward movement of trace gases in the deep tropics was notably slower in TC4 than during the Costa Rica AURA Validation Experiment (CR-AVE), in January 2006. Transport rates in the TTL were combined with in situ measurements of chlorinated and brominated organic compounds from whole air samples to determine chemical loss rates for reactive chemical species, providing empirical vertical profiles for 24-h mean concentrations of hydroxyl radicals (OH) and chlorine atoms in the TTL. The analysis shows that important short-lived species such as CHCl3, CH2Cl2, and CH2Br2 have longer chemical lifetimes than the time for transit of the TTL, implying that these species, which are not included in most models, could readily reach the stratosphere and make significant contributions of chlorine and/or bromine to stratospheric loading.

  20. Vertical transport rates and concentrations of OH and Cl radicals in the Tropical Tropopause Layer from Observations of CO2 and halocarbons: implications for distributions of long- and short-lived chemical species

    NASA Astrophysics Data System (ADS)

    Park, S.; Atlas, E. L.; Jiménez, R.; Daube, B. C.; Gottlieb, E. W.; Nan, J.; Jones, D. B. A.; Pfister, L.; Conway, T. J.; Bui, T. P.; Gao, R.-S.; Wofsy, S. C.

    2010-03-01

    Rates for large-scale vertical transport of air in the Tropical Tropopause Layer (TTL) were determined using high-resolution, in situ observations of CO2 concentrations in the tropical upper troposphere and lower stratosphere during the NASA Tropical Composition, Cloud and Climate Coupling (TC4) campaign in August 2007. Upward movement of trace gases in the deep tropics was notably slower in TC4 than during the Costa Rica AURA Validation Experiment (CR-AVE), in January 2006. Transport rates in the TTL were combined with in situ measurements of chlorinated and brominated organic compounds from whole air samples to determine chemical loss rates for reactive chemical species, providing empirical vertical profiles for 24-h mean concentrations of hydroxyl radicals (OH) and chlorine atoms in the TTL. The analysis shows that important short-lived species such as CHCl3, CH2Cl2, and CH2Br2 have longer chemical lifetimes than the time for transit of the TTL, implying that these species, which are not included in most models, could readily reach the stratosphere and make significant contributions of chlorine and/or bromine to stratospheric loading.

  1. Leaves: Elevated CO2 levels

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Burning fossil fuels and land use changes such as deforestation and urbanization have led to a dramatic rise in the concentration of carbon dioxide (CO2) in the atmosphere since the onset of the Industrial Revolution. The highly dilute CO2 from the atmosphere enters plant leaves where it is concentr...

  2. Catalytic hydrothermal upgrading of crude bio-oils produced from different thermo-chemical conversion routes of microalgae.

    PubMed

    Duan, Peigao; Wang, Bing; Xu, Yuping

    2015-06-01

    This study presents experimental results that compare the use of hydrothermal liquefaction (HTL), alcoholysis (Al), pyrolysis (Py) and hydropyrolysis (HPy) for the production of bio-oil from a microalga (Chlorella pyrenoidosa) and the catalytic hydrothermal upgrading of crude bio-oils produced by these four conversion routes. The yields and compositions of bio-oil, solid residue, and gases were evaluated and compared. HTL resulted in a bio-oil that has a higher energy density and superior fuel properties, such as thermal and storage stabilities, compared with the other three conversion routes. The N in crude bio-oils produced from Py and HPy is more easily removed than that in the bio-oils produced from HTL and Al. The upgraded bio-oils contain reduced amounts of certain O-containing and N-containing compounds and significantly increased saturated hydrocarbon contents. All of the upgraded bio-oils have a larger fraction boiling below 350°C than their corresponding crude bio-oils.

  3. Fluid chemistry of the onshore CO2 sequestration formation at Nagaoka, Japan: 5 years passed since CO2 injection

    NASA Astrophysics Data System (ADS)

    Mito, S.; Asahara, Y.; Xue, Z.

    2011-12-01

    The CO2 injection into structural reservoirs in deep permeable geologic formations is now expected one of the most realizable methods from the point of view of the cost and the CO2 preserving capability of the geological reservoirs. The first Japanese pilot-scale CO2 sequestration project has been done in an onshore saline aquifer at Nagaoka-site, Japan. 10,400 tones of CO2 were injected into a thin aquifer at the depth of 1110 m at a rate of 20-40 tones from July 2003 to January 2005. To investigate a chemical reaction between CO2 fluids and rock forming minerals at the sequestration formation, formation water was collected before and after 1year of the injection (Mito et al., 2008). The result of chemical analyses exhibited a high concentration of HCO3-, Ca, Mg, Fe, Mn and Si in the post-CO2 injection samples compared to the original formation water. The result indicated that a chemical reaction between CO2 and formation water and rock forming minerals had occurred in the sequestration formation at the early stage of CO2 storage. A continuous resistivity monitoring from 2003 to 2011 showed an existence of stagnant free CO2 at the depth of 1110m and gradual spreading of CO2 dissolved water at a top and a bottom of the free CO2 layer (Mito and Xue 2011). This observation suggests that the CO2 trapped by formation water have gradually diffused and chemical trapping of CO2 by surrounding minerals have progressed in the formation. For long-term CO2 storage, we should clarify the reaction between CO2 and minerals occurred at the edge of the spreading CO2 fluids. We are going to collect formation water in the sequestration site at November 2011. We will show the analytical result of the sampled water and discuss about the long-term chemical reaction between the diffused CO2 fluids and rock forming minerals at the Nagaoka sequestration site. References Mito et al., 2008. International Journal of Greenhouse Gas Control, 2, 309-318. Mito and Xue 2011. Energy procedia, 4

  4. Leak Path Development in CO2 Wells

    NASA Astrophysics Data System (ADS)

    Torsater, M.; Todorovic, J.; Opedal, N.; Lavrov, A.

    2014-12-01

    Wells have in numerous scientific works been denoted the "weak link" of safe and cost-efficient CO2 Capture and Storage (CCS). Whether they are active or abandoned, all wells are man-made intrusions into the storage reservoir with sealing abilities depending on degradable materials like steel and cement. If dense CO2 is allowed to expand (e.g. due to leakage) it will cool down its surroundings and cause strong thermal and mechanical loading on the wellbore. In addition, CO2 reacts chemically with rock, cement and steel. To ensure long-term underground containment, it is therefore necessary to study how, why, where and when leakage occurs along CO2wells. If cement bonding to rock or casing is poor, leak paths can form already during drilling and completion of the well. In the present work, we have mapped the bonding quality of cement-rock and cement-steel interfaces - and measured their resistance towards CO2 flow. This involved a large experimental matrix including different rocks, steels, cement types and well fluids. The bonding qualities were measured on composite cores using micro computed tomography (µ-CT), and CO2 was flooded through the samples to determine leakage rates. These were further compared to numerical simulations of leakage through the digitalized µ-CT core data, and CO2chemical interactions with the materials were mapped using electron microscopy. We also present a new laboratory set-up for measuring how well integrity is affected by downhole temperature variations - and we showcase some initial results. Our work concludes that leak path development in CO2 wells depends critically on the drilling fluids and presflushes/spacers chosen already during drilling and completion of a well. Fluid films residing on rock and casing surfaces strongly degrade the quality of cement bonding. The operation of the well is also important, as even slight thermal cycling (between 10°C and 95°C on casing) leads to significant de-bonding of the annular cement.

  5. CO2 Sequestration short course

    SciTech Connect

    DePaolo, Donald J.; Cole, David R; Navrotsky, Alexandra; Bourg, Ian C

    2014-12-08

    Given the public’s interest and concern over the impact of atmospheric greenhouse gases (GHGs) on global warming and related climate change patterns, the course is a timely discussion of the underlying geochemical and mineralogical processes associated with gas-water-mineral-interactions encountered during geological sequestration of CO2. The geochemical and mineralogical processes encountered in the subsurface during storage of CO2 will play an important role in facilitating the isolation of anthropogenic CO2 in the subsurface for thousands of years, thus moderating rapid increases in concentrations of atmospheric CO2 and mitigating global warming. Successful implementation of a variety of geological sequestration scenarios will be dependent on our ability to accurately predict, monitor and verify the behavior of CO2 in the subsurface. The course was proposed to and accepted by the Mineralogical Society of America (MSA) and The Geochemical Society (GS).

  6. Synthesis, structure and chemical bonding of CaFe2-xRhxSi2 (x=0, 1.32, and 2) and SrCo2Si2

    NASA Astrophysics Data System (ADS)

    Hlukhyy, Viktor; Hoffmann, Andrea V.; Fässler, Thomas F.

    2013-07-01

    The finding of superconductivity in Ba0.6K0.4Fe2As2 put the attention on the investigation of compounds that crystallize with ThCr2Si2 structure type such as AT2X2 (A=alkali/alkaline earth/rare earth element; T=transition metal and X=element of the 13-15th group). In this context the silicides CaFe2Si2, CaFe0.68(6)Rh1.32(6)Si2, CaRh2Si2 and SrCo2Si2 have been synthesized by reaction of the elements under an argon atmosphere. Single crystals were obtained by special heat treatment in welded niobium/tantalum ampoules. The compounds were investigated by means of powder and single crystal X-ray diffraction. All compounds crystallize in the ThCr2Si2-type structure with space group I4/mmm (No. 139): a=3.939(1) Å, c=10.185(1) Å, R1=0.045, 85 F2 values, 8 variable parameters for CaFe2Si2; a=4.0590(2) Å, c=9.9390(8) Å, R1=0.030, 90 F2 values, 10 variable parameters for CaFe0.68(6)Rh1.32(6)Si2; a=4.0695(1) Å, c=9.9841(3) Å, R1=0.031, 114 F2 values, 9 variable parameters for CaRh2Si2; and a=3.974(1) Å, c=10.395(1) Å, R1=0.036, 95 F2 values, 8 variable parameters for SrCo2Si2. The structure of SrCo2Si2 contains isolated [Co2Si2]2- 2D-layers in the ab-plane whereas in CaFe2-xRhxSi2 the [T2Si2] layers (T=Fe and Rh) are interconnected along the c-axis via Si3Si bonds resulting in a three-dimentional (3D) [T2Si2]2- polyanions and therefore belong to the so-called collapsed form of the ThCr2Si2-type structure. The SrCo2Si2 and CaRh2Si2 are isoelectronic to the parent 122 iron-pnictide superconductors AeFe2As2 (Ae=alkaline earth elements), whereas CaFe2Si2 is a full substituted variant (As/Si) of CaFe2As2. The crystal chemistry and chemical bonding in the title compounds are discussed in terms of LMTO band structure calculations and a topological analysis using the Electron Localization Function (ELF).

  7. Effects of elevated CO2 concentrations on denitrifying and nitrifying popualtions at terrestrial CO2 leakeage analogous sites

    NASA Astrophysics Data System (ADS)

    Christine, Dictor Marie; Catherine, Joulian; Valerie, Laperche; Stephanie, Coulon; Dominique, Breeze

    2010-05-01

    CO2 capture and geological storage (CCS) is recognized to be an important option for carbon abatement in Europe. One of the risks of CCS is the leakage from storage site. A laboratory was conducted on soil samples sampled near-surface from a CO2 leakage analogous site (Latera, Italy) in order to evaluate the impact of an elevated soil CO2 concentration on terrestrial bacterial ecosystems form near surface terrestrial environments and to determine a potential bacterial indicator of CO2 leakage from storage site. Surveys were conducted along a 50m long transect across the vent centre, providing a spectrum of CO2 flux rates, soil gas concentrations and compositions (Beaubien et al., 2007). A bacterial diversity studies, performed by CE-SSCP technique, on a soil profile with increasing CO2 soil concentrations (from 0.3% to 100%) showed that a change on bacterial diversity was noted when CO2 concentration was above 50 % of CO2. From this result, 3 soil samples were taken at 70 cm depth in 3 distinct zones (background soil CO2 content, soil CO2 content of 20% and soil CO2 content of 50%). Then theses soil samples were incubated under closed jars flushed with different air atmospheres (20, 50 and 90 % of CO2) during 18 months. At initial, 3, 6, 12 and 18 months, some soil samples were collected in order to estimate the denitrifying, nitrifying activities as a function of CO2 concentration content and times. Theses enzymatic activities were chosen because one occurs under anaerobic conditions (denitrification) and the other occurs under aerobic conditions (nitrification). Both of them were involved in the nitrogen cycle and are major actors of soil function and groundwater quality preservation. Metabolic diversity using BIOLOG Ecoplates was determined on every soil samples. Physico-chemical parameters (e.g. pH, bulk chemistry, mineralogy) were analyzed to have some information about the evolution of the soil during the incubation with increasing soil CO2 concentrations

  8. The LHCb VELO upgrade

    NASA Astrophysics Data System (ADS)

    Dosil Suárez, Álvaro

    2016-07-01

    The upgrade of the LHCb experiment, planned for 2019, will transform the experiment to a trigger-less system reading out the full detector at 40 MHz event rate. All data reduction algorithms will be executed in a high-level software farm. The upgraded detector will run at luminosities of 2×1033 cm-2 s-1 and probe physics beyond the Standard Model in the heavy flavour sector with unprecedented precision. The Vertex Locator (VELO) is the silicon vertex detector surrounding the interaction region. The current detector will be replaced with a hybrid pixel system equipped with electronics capable of reading out at 40 MHz. The detector comprises silicon pixel sensors with 55×55 μm2 pitch, read out by the VeloPix ASIC, based on the TimePix/MediPix family. The hottest region will have pixel hit rates of 900 Mhits/s yielding a total data rate more than 3 Tbit/s for the upgraded VELO. The detector modules are located in a separate vacuum, separated from the beam vacuum by a thin custom made foil. The detector halves are retracted when the beams are injected and closed at stable beams, positioning the first sensitive pixel at 5.1 mm from the beams. The material budget will be minimised by the use of evaporative CO2 coolant circulating in microchannels within 400 μm thick silicon substrates.

  9. CO2 Storage related Groundwater Impacts and Protection

    NASA Astrophysics Data System (ADS)

    Fischer, Sebastian; Knopf, Stefan; May, Franz; Rebscher, Dorothee

    2016-03-01

    Injection of CO2 into the deep subsurface will affect physical and chemical conditions in the storage environment. Hence, geological CO2 storage can have potential impacts on groundwater resources. Shallow freshwater can only be affected if leakage pathways facilitate the ascent of CO2 or saline formation water. Leakage associated with CO2 storage cannot be excluded, but potential environmental impacts could be reduced by selecting suitable storage locations. In the framework of risk assessment, testing of models and scenarios against operational data has to be performed repeatedly in order to predict the long-term fate of CO2. Monitoring of a storage site should reveal any deviations from expected storage performance, so that corrective measures can be taken. Comprehensive R & D activities and experience from several storage projects will enhance the state of knowledge on geological CO2 storage, thus enabling safe storage operations at well-characterised and carefully selected storage sites while meeting the requirements of groundwater protection.

  10. Polyurethane Foam-Based Ultramicroporous Carbons for CO2 Capture.

    PubMed

    Ge, Chao; Song, Jian; Qin, Zhangfeng; Wang, Jianguo; Fan, Weibin

    2016-07-27

    A series of sustainable porous carbon materials were prepared from waste polyurethane foam and investigated for capture of CO2. The effects of preparation conditions, such as precarbonization, KOH to carbon precursor weight ratio, and activation temperature, on the porous structure and CO2 adsorption properties were studied for the purpose of controlling pore sizes and nitrogen content and developing high-performance materials for capture of CO2. The sample prepared at optimum conditions shows CO2 adsorption capacities of 6.67 and 4.33 mmol·g(-1) at 0 and 25 °C under 1 bar, respectively, which are comparable to those of the best reported porous carbons prepared from waste materials. The HCl treatment experiment reveals that about 80% of CO2 adsorption capacity arises from physical adsorption, while the other 20% is due to the chemical adsorption originated from the interaction of basic N groups and CO2 molecules. The relationship between CO2 uptake and pore size at different temperatures indicates that the micropores with pore size smaller than 0.86 and 0.70 nm play a dominant role in the CO2 adsorption at 0 and 25 °C, respectively. It was found that the obtained carbon materials exhibited high recyclability and high selectivity to adsorption of CO2 from the CO2 and N2 mixture.

  11. Co2 On Titan's Surface

    NASA Astrophysics Data System (ADS)

    McCord, Thomas B.; Combe, J.; Hayne, P.; Hansen, G. B.

    2007-10-01

    Evidence is reported for the presence of CO2 on the surface of Titan from the Cassini VIMS (an imaging visual and IR spectrometer) data (McCord et al., 2006, 2007). CO2 can be expected on Titan from basic planetary evolution models. It was also suggested as a plausible spectral component for bright material near the Huygens landing site (Rodriguez et al., 2006), based on structure in the 1.59-µm region. Hartung et al. (2006) searched for CO2 in one hemisphere, but they were able only to set an upper limit on the possible spatial coverage by pure CO2. Barnes et al., (2006) suggested CO2 as a possible candidate material for a 5-µm-bright region, named Tsegihi, based on the high 5-µm reflectance. However, these results are not inconsistent with our report. The evidence we report is three-fold: 1) A weak absorption near 4.9 µm in the 5-µm methane window for the Tui Regio region; 2) The spectral contrast between the 2.7- and 2.8-µm methane subwindows for the regions exhibiting the 4.9-µm absorption, with stronger absorption correlating with stronger contrast; and 3) the overall shape of the CO2 spectrum (for several grain-sizes) is consistent with the spectrum of one of the fundamental surface spectral components, as deduced by spectral mixture analysis modeling. The Tui Regio feature exhibits the strongest evidence in all three categories. Studies of this feature's morphology and albedo markings have suggested to some that it may be an active cryovolcanic feature (Barnes et al., 2006). If so, CO2 could be erupting and depositing as a frost. This likely happened elsewhere and at other times. Thus, CO2 could be a major constituent of the surface, but over time it may be mixed with other constituents, such as spectrally neutral organics raining from the atmosphere, thereby reducing the strength of its spectral signature.

  12. Spectroscopic study of low pressure, low temperature H2-CH4-CO2 microwave plasmas used for large area deposition of nanocrystalline diamond films. Part II: on plasma chemical processes

    NASA Astrophysics Data System (ADS)

    Nave, A. S. C.; Baudrillart, B.; Hamann, S.; Bénédic, F.; Lombardi, G.; Gicquel, A.; van Helden, J. H.; Röpcke, J.

    2016-12-01

    In a distributed antenna array (DAA) reactor, microwave H2 plasmas with admixtures of 2.5% CH4 and 1% CO2 used for the deposition of nanocrystalline diamond films have been studied by infrared laser absorption and optical emission spectroscopy (OES) techniques. The experiments were carried out in order to analyze the dependence of plasma chemical phenomena on power and pressure at relatively low pressures, up to 0.55 mbar, and power values, up to 3 kW. The evolution of the concentration of the methyl radical, CH3, of five stable molecules, CH4, CO2, CO, C2H2 and C2H6, and of vibrationally excited CO in the first and second hot band was monitored in the plasma processes by in situ infrared laser absorption spectroscopy using tunable lead salt diode lasers (TDL) and an external-cavity quantum cascade laser (EC-QCL) as radiation sources. OES was applied simultaneously to obtain complementary information about the degree of dissociation of the H2 precursor and of its gas temperature. The experimental results are presented in two separate parts. In Part I, the first paper in a two-part series, the measurement of the gas (T gas), rotational (T rot) and vibrational (T vib) temperatures of the various species in the complex plasma was the main focus of interest. Depending on the different plasma zones the gas temperature was found to range between about 360 and 1000 K inside the DAA reactor (Nave et al 2016 Plasma Sources Sci. Technol. 25 065002). In Part II, the present paper, taking into account the temperatures determined in the first paper, the concentrations of the various species, which were found to be in a range between 1011 and 1015 cm-3, are the focus of interest. The influence of the discharge parameters power and pressure on the molecular concentrations has been studied. To achieve further insight into general plasma chemical aspects the dissociation of the carbon precursor gases including their fragmentation and conversion to the reaction products has been

  13. Breadboard CO2 and humidity control system

    NASA Technical Reports Server (NTRS)

    Boehm, A. M.

    1976-01-01

    A regenerable CO2 and humidity control system is being developed for potential use on shuttle as an alternate to the baseline lithium hydroxide (LiOH)/condensing heat exchanger system. The system utilizes a sorbent material, designated HS-C, to adsorb CO2 and water vapor from the cabin atmosphere. The material is regenerated by exposing it to space vacuum. A half-size breadboard system, utilizing a flight representative HS-C canister, was designed, built, and performance tested to shuttle requirements for total CO2 and total humidity removal. The use of a new chemical matrix material allowed significant optimization of the system design by packing the HS-C chemical into the core of a heat exchanger which is manifolded to form two separate and distinct beds. Breadboard system performance was proven by parametric testing and simulated mission testing over the full range of shuttle crew sizes and metabolic loadings. Vacuum desorption testing demonstrated considerable savings in previously projected shuttle vacuum duct sizing.

  14. Enhancing the Ocean's Role in CO2 Mitigation

    NASA Astrophysics Data System (ADS)

    Rau, G. H.

    2012-12-01

    The possibility of safely increasing the ocean's significant, natural consumption and storage of excess CO2 deserves consideration since land-based efforts are thus far failing to stabilize atmospheric CO2 and associated climate and ocean chemistry impacts. Of the approximately 34 GT/yr of CO2 currently emitted to the atmosphere by human activity, the ocean consumes the equivalent of about 8 GT/yr of these emissions. These fluxes are, however, dwarfed by the annual gross amount of CO2 naturally taken up and released by the ocean, in excess of 300 GT CO2/yr. Additionally, the carbon content in the ocean is about 50 times that of the atmosphere, with the majority in a form (HCO2-) that can, through equilibrium reactions, interact with atmospheric CO2. Marine chemical, biological and physical processes that naturally affect ocean CO2 gain and loss thus intimately influence the natural carbon content of the atmosphere. Indeed, ocean chemistry in conjunction with carbonate and silicate mineral weathering is the primary mechanism that naturally moderates and consumes excess atmospheric CO2 on geologic timescales. The ocean is therefore a logical place to explore means of enhancing atmospheric and anthropogenic carbon uptake and/or sequestration in efforts to stabilize or possibly reduce atmospheric CO2 concentrations. Modification of such global processes (often only relatively slightly) forms the basis for many of the ocean-based CO2 mitigation approaches thus far proposed. These include: 1) the storage in or under the ocean of molecular CO2, or organic or inorganic derivatives that have been captured or formed on land; 2) the removal of ocean/atmosphere CO2 via biological uptake enhanced by artificially increased upwelling or nutrient addition; 3) the chemical, geochemical, or electrochemical alkalization of the ocean to increase ocean CO2 uptake with chemical transformation to bicarbonates or carbonates, and subsequent ocean storage; and 4) increased production and

  15. Synthesis, physical-chemical characterization and electrochemical performance of GdBaCo2-xNixO5+δ (x = 0-0.8) as cathode materials for IT-SOFC application

    NASA Astrophysics Data System (ADS)

    Hu, Y.; Bogicevic, C.; Bouffanais, Y.; Giot, M.; Hernandez, O.; Dezanneau, G.

    2013-11-01

    GdBaCo2-xNixO5+δ (x = 0-0.8) cathode materials have been synthesized by a citrate-gel modified chemical route, by which we have achieved a high level of substitution up to x = 0.8. Oxygen stoichiometry at room temperature has been determined by iodometry and the structural evolution as a function of Ni content has been extracted from XRD patterns analysis. All compounds are orthorhombic at room temperature and a DSC analysis reveals that the high-temperature orthorhombic-to-tetragonal phase transition is observed at lower temperature as Ni substitution increases. Three compositions, with x = 0, 0.3 and 0.6, were then chosen for further characterization: high-temperature XRD has been performed confirming the abovementioned structural evolution with temperature and allowing to determine that Ni doping diminishes slightly the thermal expansion coefficient. According to 4-probe measurements, we show that these compounds present a high electronic conductivity, suitable for cathode materials. Finally, electrochemical characterization has been performed by AC impedance spectroscopy with symmetric cells using composite electrode showing an improvement of performance at intermediate substitution levels.

  16. ACCURACY OF CO2 SENSORS

    SciTech Connect

    Fisk, William J.; Faulkner, David; Sullivan, Douglas P.

    2008-10-01

    Are the carbon dioxide (CO2) sensors in your demand controlled ventilation systems sufficiently accurate? The data from these sensors are used to automatically modulate minimum rates of outdoor air ventilation. The goal is to keep ventilation rates at or above design requirements while adjusting the ventilation rate with changes in occupancy in order to save energy. Studies of energy savings from demand controlled ventilation and of the relationship of indoor CO2 concentrations with health and work performance provide a strong rationale for use of indoor CO2 data to control minimum ventilation rates1-7. However, this strategy will only be effective if, in practice, the CO2 sensors have a reasonable accuracy. The objective of this study was; therefore, to determine if CO2 sensor performance, in practice, is generally acceptable or problematic. This article provides a summary of study methods and findings ? additional details are available in a paper in the proceedings of the ASHRAE IAQ?2007 Conference8.

  17. Sequestering CO2 in the Ocean: Options and Consequences

    NASA Astrophysics Data System (ADS)

    Rau, G. H.; Caldeira, K.

    2002-12-01

    The likelihood of negative climate and environmental impacts associated with increasing atmospheric CO2 has prompted serious consideration of various CO2 mitigation strategies. Among these are methods of capturing and storing of CO2 in the ocean. Two approaches that have received the most attention in this regard have been i) ocean fertilization to enhanced biological uptake and fixation of CO2, and ii) the chemical/mechanical capture and injection of CO2 into the deep ocean. Both methods seek to enhance or speed up natural mechanisms of CO2 uptake and storage by the ocean, namely i) the biological CO2 "pump" or ii) the passive diffusion of CO2 into the surface ocean and subsequent mixing into the deep sea. However, as will be reviewed, concerns about the capacity and effectiveness of either strategy in long-term CO2 sequestration have been raised. Both methods are not without potentially significant environmental impacts, and the costs of CO2 capture and injection (option ii) are currently prohibitive. An alternate method of ocean CO2 sequestration would be to react and hydrate CO2 rich waste gases (e.g., power plant flue gas) with seawater and to subsequently neutralize the resulting carbonic acid with limestone to produce calcium and bicarbonate ions in solution. This approach would simply speed up the CO2 uptake and sequestration that naturally (but very slowly) occurs via global carbonate weathering. This would avoid much of the increased acidity associated with direct CO2 injection while obviating the need for costly CO2 separation and capture. The addition of the resulting bicarbonate- and carbonate-rich solution to the ocean would help to counter the decrease in pH and carbonate ion concentration, and hence loss of biological calcification that is presently occurring as anthropogenic CO2 invades the ocean from the atmosphere. However, as with any approach to CO2 mitigation, the costs, impacts, risks, and benefits of this method need to be better understood

  18. Update on CO2 emissions

    SciTech Connect

    Friedingstein, P.; Houghton, R.A.; Marland, Gregg; Hackler, J.; Boden, Thomas A; Conway, T.J.; Canadell, J.G.; Raupach, Mike; Ciais, Philippe; Le Quere, Corrine

    2010-12-01

    Emissions of CO2 are the main contributor to anthropogenic climate change. Here we present updated information on their present and near-future estimates. We calculate that global CO2 emissions from fossil fuel burning decreased by 1.3% in 2009 owing to the global financial and economic crisis that started in 2008; this is half the decrease anticipated a year ago1. If economic growth proceeds as expected2, emissions are projected to increase by more than 3% in 2010, approaching the high emissions growth rates that were observed from 2000 to 20081, 3, 4. We estimate that recent CO2 emissions from deforestation and other land-use changes (LUCs) have declined compared with the 1990s, primarily because of reduced rates of deforestation in the tropics5 and a smaller contribution owing to forest regrowth elsewhere.

  19. The CO2nnect activities

    NASA Astrophysics Data System (ADS)

    Eugenia, Marcu

    2014-05-01

    Climate change is one of the biggest challenges we face today. A first step is the understanding the problem, more exactly what is the challenge and the differences people can make. Pupils need a wide competencies to meet the challenges of sustainable development - including climate change. The CO2nnect activities are designed to support learning which can provide pupils the abilities, skills, attitudes and awareness as well as knowledge and understanding of the issues. The project "Together for a clean and healthy world" is part of "The Global Educational Campaign CO2nnect- CO2 on the way to school" and it was held in our school in the period between February and October 2009. It contained a variety of curricular and extra-curricular activities, adapted to students aged from 11 to 15. These activities aimed to develop in students the necessary skills to understanding man's active role in improving the quality of the environment, putting an end to its degrading process and to reducing the effects of climate changes caused by the human intervention in nature, including transport- a source of CO2 pollution. The activity which I propose can be easily adapted to a wide range of age groups and linked to the curricula of many subjects: - Investigate CO2 emissions from travel to school -Share the findings using an international database -Compare and discuss CO2 emissions -Submit questions to a climate- and transport expert -Partner with other schools -Meet with people in your community to discuss emissions from transport Intended learning outcomes for pupils who participate in the CO2nnect campaign are: Understanding of the interconnected mobility- and climate change issue climate change, its causes and consequences greenhouse-gas emissions from transport and mobility the interlinking of social, environmental, cultural and economic aspects of the local transport system how individual choices and participation can contribute to creating a more sustainable development

  20. CO2CRC's Otway Residual Saturation and Dissolution Test: Using Reactive Ester Tracers to Determine Residual CO2 Saturation

    NASA Astrophysics Data System (ADS)

    Myers, M.; Stalker, L.; LaForce, T.; Pejcic, B.; Dyt, C.; Ho, K.; Ennis-King, J.

    2013-12-01

    Residual trapping, that is CO2 held in the rock pore space due to capillarity, is an important storage mechanism in geo-sequestration of over the short to medium term (up to 1000 years). As such residual CO2 saturation is a critical reservoir parameter for assessing the storage capacity and security of carbon capture and storage (CCS). As a component of the CO2CRC's Residual Gas Saturation and Dissolution Test at the CO2CRC Otway Project site in Victoria (Australia), we have recently tested a suite of reactive esters (triacetin, tripropionin and propylene glycol diacetate) in a single well chemical tracer test to determine residual CO2 saturation. The goal of this project was to assess and validate a suite of possible tests that could be implemented to determine residual CO2 saturation. For this test, the chemical tracers were injected with a saturated CO2/water mixture into the formation (that is already at residual CO2 saturation) where they were allowed to 'soak' for approximately 10 days allowing for the partial hydrolysis of the esters to their corresponding carboxylic acids and alcohols. Water containing the tracers was then produced from the well resulting in over 600 tracer samples over a period of 12 hours. A selection of these samples were analysed for tracer content and to establish tracer breakthrough curves. To understand the behaviour of these chemical tracers in the downhole environment containing residually trapped supercritical CO2 and formation water, it is necessary to determine the supercritical CO2/water partition coefficients. We have previously determined these in the laboratory (Myers et al., 2012) and they are used here to model the tracer behaviour and provide an estimate of the residual CO2 saturation. Two different computational simulators were used to analyse the tracer breakthrough profiles. The first is based on simple chromatographic retardation and has been used extensively in single well chemical tracer tests to determine residual

  1. Reducing cement's CO2 footprint

    USGS Publications Warehouse

    van Oss, Hendrik G.

    2011-01-01

    The manufacturing process for Portland cement causes high levels of greenhouse gas emissions. However, environmental impacts can be reduced by using more energy-efficient kilns and replacing fossil energy with alternative fuels. Although carbon capture and new cements with less CO2 emission are still in the experimental phase, all these innovations can help develop a cleaner cement industry.

  2. Efficient electrochemical CO2 conversion powered by renewable energy.

    PubMed

    Kauffman, Douglas R; Thakkar, Jay; Siva, Rajan; Matranga, Christopher; Ohodnicki, Paul R; Zeng, Chenjie; Jin, Rongchao

    2015-07-22

    The catalytic conversion of CO2 into industrially relevant chemicals is one strategy for mitigating greenhouse gas emissions. Along these lines, electrochemical CO2 conversion technologies are attractive because they can operate with high reaction rates at ambient conditions. However, electrochemical systems require electricity, and CO2 conversion processes must integrate with carbon-free, renewable-energy sources to be viable on larger scales. We utilize Au25 nanoclusters as renewably powered CO2 conversion electrocatalysts with CO2 → CO reaction rates between 400 and 800 L of CO2 per gram of catalytic metal per hour and product selectivities between 80 and 95%. These performance metrics correspond to conversion rates approaching 0.8-1.6 kg of CO2 per gram of catalytic metal per hour. We also present data showing CO2 conversion rates and product selectivity strongly depend on catalyst loading. Optimized systems demonstrate stable operation and reaction turnover numbers (TONs) approaching 6 × 10(6) molCO2 molcatalyst(-1) during a multiday (36 h total hours) CO2 electrolysis experiment containing multiple start/stop cycles. TONs between 1 × 10(6) and 4 × 10(6) molCO2 molcatalyst(-1) were obtained when our system was powered by consumer-grade renewable-energy sources. Daytime photovoltaic-powered CO2 conversion was demonstrated for 12 h and we mimicked low-light or nighttime operation for 24 h with a solar-rechargeable battery. This proof-of-principle study provides some of the initial performance data necessary for assessing the scalability and technical viability of electrochemical CO2 conversion technologies. Specifically, we show the following: (1) all electrochemical CO2 conversion systems will produce a net increase in CO2 emissions if they do not integrate with renewable-energy sources, (2) catalyst loading vs activity trends can be used to tune process rates and product distributions, and (3) state-of-the-art renewable-energy technologies are sufficient

  3. Sedimentary reservoir oxidation during geologic CO2 sequestration

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

  4. Efficient electrochemical CO2 conversion powered by renewable energy

    DOE PAGES

    Kauffman, Douglas R.; Thakkar, Jay; Siva, Rajan; ...

    2015-06-29

    Here, the catalytic conversion of CO2 into industrially relevant chemicals is one strategy for mitigating greenhouse gas emissions. Along these lines, electrochemical CO2 conversion technologies are attractive because they can operate with high reaction rates at ambient conditions. However, electrochemical systems require electricity, and CO2 conversion processes must integrate with carbon-free, renewable-energy sources to be viable on larger scales. We utilize Au25 nanoclusters as renewably powered CO2 conversion electrocatalysts with CO2 → CO reaction rates between 400 and 800 L of CO2 per gram of catalytic metal per hour and product selectivities between 80 and 95%. These performance metrics correspondmore » to conversion rates approaching 0.8–1.6 kg of CO2 per gram of catalytic metal per hour. We also present data showing CO2 conversion rates and product selectivity strongly depend on catalyst loading. Optimized systems demonstrate stable operation and reaction turnover numbers (TONs) approaching 6 × 106 mol CO2 molcatalyst–1 during a multiday (36 hours total hours) CO2electrolysis experiment containing multiple start/stop cycles. TONs between 1 × 106 and 4 × 106 molCO2 molcatalyst–1 were obtained when our system was powered by consumer-grade renewable-energy sources. Daytime photovoltaic-powered CO2 conversion was demonstrated for 12 h and we mimicked low-light or nighttime operation for 24 h with a solar-rechargeable battery. This proof-of-principle study provides some of the initial performance data necessary for assessing the scalability and technical viability of electrochemical CO2 conversion technologies. Specifically, we show the following: (1) all electrochemical CO2 conversion systems will produce a net increase in CO2 emissions if they do not integrate with renewable-energy sources, (2) catalyst loading vs activity trends can be used to tune process rates and product distributions, and (3) state-of-the-art renewable-energy technologies

  5. Is guava phenolic metabolism influenced by elevated atmospheric CO2?

    PubMed

    Mendes de Rezende, Fernanda; Pereira de Souza, Amanda; Silveira Buckeridge, Marcos; Maria Furlan, Cláudia

    2015-01-01

    Seedlings of Psidium guajava cv. Pedro Sato were distributed into four open-top chambers: two with ambient CO(2) (∼390 ppm) and two with elevated CO(2) (∼780 ppm). Monthly, five individuals of each chamber were collected, separated into root, stem and leaves and immediately frozen in liquid nitrogen. Chemical parameters were analyzed to investigate how guava invests the surplus carbon. For all classes of phenolic compounds analyzed only tannins showed significant increase in plants at elevated CO(2) after 90 days. There was no significant difference in dry biomass, but the leaves showed high accumulation of starch under elevated CO(2). Results suggest that elevated CO(2) seems to be favorable to seedlings of P. guajava, due to accumulation of starch and tannins, the latter being an important anti-herbivore substance.

  6. 5% CO2 is a potent, fast acting inhalation anticonvulsant

    PubMed Central

    Tolner, Else A.; Hochman, Daryl W.; Hassinen, Pekka; Otáhal, Jakub; Gaily, Eija; Haglund, Michael M.; Kubová, Hana; Schuchmann, Sebastian; Vanhatalo, Sampsa; Kaila, Kai

    2010-01-01

    Purpose CO2 has been long recognized for its anticonvulsant properties. We aimed to determine whether inhaling 5% CO2 can be used to suppress seizures in epilepsy patients. The effect of CO2 on cortical epileptic activity accompanying behavioral seizures was studied in rats and a non-human primate and based on these data, preliminary tests were carried out in humans. Methods In freely moving rats, cortical afterdischarges paralleled by myoclonic convulsions were evoked by sensorimotor cortex stimulation. 5% CO2 was applied for 5 minutes, 3 minutes before stimulation. In macaque monkeys, hypercarbia was induced by hypoventilation while seizure activity was electrically or chemically evoked in the sensorimotor cortex. Seven patients with drug-resistant partial epilepsy were examined with video-EEG and received 5% CO2 in medical carbogen shortly after electrographic seizure onset. Results In rats, 5% CO2 strongly suppressed cortical afterdischarges, by ca. 75%, while responses to single-pulse stimulation were reduced by about 15% only. In macaques, increasing pCO2 from 37 to 44-45 mmHg (corresponding to inhalation of 5% CO2 or less) suppressed stimulation-induced cortical afterdischarges by about 70% and single, bicuculline-induced epileptiform spikes by ca. 25%. In a pilot trial carried out in 7 patients, a rapid termination of electrographic seizures was seen despite the fact that the application of 5% CO2 was started after seizure generalization. Conclusions 5% CO2 has a fast and potent anticonvulsant action. The present data suggest that medical carbogen with 5% CO2 can be used for acute treatment to suppress seizures in epilepsy patients. PMID:20887367

  7. Crystal structures and dynamical properties of dense CO2

    PubMed Central

    Yong, Xue; Liu, Hanyu; Wu, Min; Yao, Yansun; Tse, John S.; Dias, Ranga; Yoo, Choong-Shik

    2016-01-01

    Structural polymorphism in dense carbon dioxide (CO2) has attracted significant attention in high-pressure physics and chemistry for the past two decades. Here, we have performed high-pressure experiments and first-principles theoretical calculations to investigate the stability, structure, and dynamical properties of dense CO2. We found evidence that CO2-V with the 4-coordinated extended structure can be quenched to ambient pressure below 200 K—the melting temperature of CO2-I. CO2-V is a fully coordinated structure formed from a molecular solid at high pressure and recovered at ambient pressure. Apart from confirming the metastability of CO2-V (I-42d) at ambient pressure at low temperature, results of ab initio molecular dynamics and metadynamics (MD) simulations provided insights into the transformation processes and structural relationship from the molecular to the extended phases. In addition, the simulation also predicted a phase V′(Pna21) in the stability region of CO2-V with a diffraction pattern similar to that previously assigned to the CO2-V (P212121) structure. Both CO2-V and -V′ are predicted to be recoverable and hard with a Vicker hardness of ∼20 GPa. Significantly, MD simulations found that the CO2 in phase IV exhibits large-amplitude bending motions at finite temperatures and high pressures. This finding helps to explain the discrepancy between earlier predicted static structures and experiments. MD simulations clearly indicate temperature effects are critical to understanding the high-pressure behaviors of dense CO2 structures—highlighting the significance of chemical kinetics associated with the transformations. PMID:27647887

  8. Crystal structures and dynamical properties of dense CO2.

    PubMed

    Yong, Xue; Liu, Hanyu; Wu, Min; Yao, Yansun; Tse, John S; Dias, Ranga; Yoo, Choong-Shik

    2016-10-04

    Structural polymorphism in dense carbon dioxide (CO2) has attracted significant attention in high-pressure physics and chemistry for the past two decades. Here, we have performed high-pressure experiments and first-principles theoretical calculations to investigate the stability, structure, and dynamical properties of dense CO2 We found evidence that CO2-V with the 4-coordinated extended structure can be quenched to ambient pressure below 200 K-the melting temperature of CO2-I. CO2-V is a fully coordinated structure formed from a molecular solid at high pressure and recovered at ambient pressure. Apart from confirming the metastability of CO2-V (I-42d) at ambient pressure at low temperature, results of ab initio molecular dynamics and metadynamics (MD) simulations provided insights into the transformation processes and structural relationship from the molecular to the extended phases. In addition, the simulation also predicted a phase V'(Pna21) in the stability region of CO2-V with a diffraction pattern similar to that previously assigned to the CO2-V (P212121) structure. Both CO2-V and -V' are predicted to be recoverable and hard with a Vicker hardness of ∼20 GPa. Significantly, MD simulations found that the CO2 in phase IV exhibits large-amplitude bending motions at finite temperatures and high pressures. This finding helps to explain the discrepancy between earlier predicted static structures and experiments. MD simulations clearly indicate temperature effects are critical to understanding the high-pressure behaviors of dense CO2 structures-highlighting the significance of chemical kinetics associated with the transformations.

  9. Distribution and nature of CO2 on Enceladus

    NASA Astrophysics Data System (ADS)

    Combe, J. P.; McCord, T. B.; Matson, D.; Johnson, T. V.; Scipioni, F.; Tosi, F.

    2015-12-01

    We present the first global mapping and analysis of CO2 on the surface of Enceladus, and we report the largest concentrations of free CO2 on the southern polar region using the Visual and Infrared Mapping Spectrometer (VIMS) on Cassini. Free CO2 ice and complexed CO2 were already reported near the South Pole (Brown et al., Science, 2006; Hansen, LPSC, 2010). Our work focuses on determining the amount, location and molecular state of CO2 on Enceladus, which could help identify and model geophysical processes that currently occur in the interior. One hypothesis for bringing heat and chemicals to the surface is a warm subsurface ocean containing dissolved gases, mostly CO2 (Postberg F. et al., Nature, 2009). Therefore, our observations are consistent with erupted and condensed materials onto Enceladus' surface (Matson et al., Icarus, 2012; Matson et al. AGU Fall meeting 2015). Free CO2 ice absorbs at 4.268 µm (Sandford and Allamandola, 1990) and CO2 complexed with other molecules absorbs at 4.247 μm (Chaban et al., Icarus, 2007). The Enceladus case is complicated because both free and complexed CO2 are present, and the absorption band of interest is shallow and close to the instrument detection limit. Many of the few Enceladus VIMS data sets have significant and sometimes unusual noise, which we attempted to avoid or remove. We utilized all VIMS data sets available that were collected over ten years of the Cassini mission as a way to improve the detection statistics and signal to noise. We also used wavelengths near 2.7 μm where CO2 has a narrow absorption as a filter to help identify CO2-rich areas. Finally, we selected observations that have spatial resolution better than 100 km in order to create a map that can be compared with the largest fractures, known as Tiger Stripes, in the southern polar region.

  10. Intercomparison of two cavity ring-down spectroscopy analyzers for atmospheric 13CO2 / 12CO2 measurement

    NASA Astrophysics Data System (ADS)

    Pang, Jiaping; Wen, Xuefa; Sun, Xiaomin; Huang, Kuan

    2016-08-01

    Isotope ratio infrared spectroscopy (IRIS) permits continuous in situ measurement of CO2 isotopic composition under ambient conditions. Previous studies have mainly focused on single IRIS instrument performance; few studies have considered the comparability among different IRIS instruments. In this study, we carried out laboratory and ambient measurements using two Picarro CO2δ13C analyzers (G1101-i and G2201-i (newer version)) and evaluated their performance and comparability. The best precision was 0.08-0.15 ‰ for G1101-i and 0.01-0.04 ‰ for G2201-i. The dependence of δ13C on CO2 concentration was 0.46 ‰ per 100 ppm and 0.09 ‰ per 100 ppm, the instrument drift ranged from 0.92-1.09 ‰ and 0.19-0.37 ‰, and the sensitivity of δ13C to the water vapor mixing ratio was 1.01 ‰ / % H2O and 0.09 ‰ / % H2O for G1101-i and G2201-i, respectively. The accuracy after correction by the two-point mixing ratio gain and offset calibration method ranged from -0.04-0.09 ‰ for G1101-i and -0.13-0.03 ‰ for G2201-i. The sensitivity of δ13C to the water vapor mixing ratio improved from 1.01 ‰ / % H2O before the upgrade of G1101-i (G1101-i-original) to 0.15 ‰ / % H2O after the upgrade of G1101-i (G1101-i-upgraded). Atmospheric δ13C measured by G1101-i and G2201-i captured the rapid changes in atmospheric δ13C signals on hourly to diurnal cycle scales, with a difference of 0.07 ± 0.24 ‰ between G1101-i-original and G2201-i and 0.05 ± 0.30 ‰ between G1101-i-upgraded and G2201-i. A significant linear correlation was observed between the δ13C difference of G1101-i-original and G2201-i and the water vapor concentration, but there was no significant correlation between the δ13C difference of G1101-i-upgraded and G2201-i and the water vapor concentration. The difference in the Keeling intercept values decreased from 1.24 ‰ between G1101-i-original and G2201-i to 0.36 ‰ between G1101-i-upgraded and G2201-i, which indicates the importance of consistency

  11. CO2 Acquisition Membrane (CAM)

    NASA Technical Reports Server (NTRS)

    Mason, Larry W.; Way, J. Douglas; Vlasse, Marcus

    2003-01-01

    The objective of CAM is to develop, test, and analyze thin film membrane materials for separation and purification of carbon dioxide (CO2) from mixtures of gases, such as those found in the Martian atmosphere. The membranes are targeted toward In Situ Resource Utilization (ISRU) applications that will operate in extraterrestrial environments and support future unmanned and human space missions. A primary application is the Sabatier Electrolysis process that uses Mars atmosphere CO2 as raw material for producing water, oxygen, and methane for rocket fuel and habitat support. Other applications include use as an inlet filter to collect and concentrate Mars atmospheric argon and nitrogen gases for habitat pressurization, and to remove CO2 from breathing gases in Closed Environment Life Support Systems (CELSS). CAM membrane materials include crystalline faujasite (FAU) zeolite and rubbery polymers such as silicone rubber (PDMS) that have been shown in the literature and via molecular simulation to favor adsorption and permeation of CO2 over nitrogen and argon. Pure gas permeation tests using commercial PDMS membranes have shown that both CO2 permeance and the separation factor relative to other gases increase as the temperature decreases, and low (Delta)P(Sub CO2) favors higher separation factors. The ideal CO2/N2 separation factor increases from 7.5 to 17.5 as temperature decreases from 22 C to -30 C. For gas mixtures containing CO2, N2, and Ar, plasticization decreased the separation factors from 4.5 to 6 over the same temperature range. We currently synthesize and test our own Na(+) FAU zeolite membranes using standard formulations and secondary growth methods on porous alumina. Preliminary tests with a Na(+) FAU membrane at 22 C show a He/SF6 ideal separation factor of 62, exceeding the Knudsen diffusion selectivity by an order of magnitude. This shows that the membrane is relatively free from large defects and associated non-selective (viscous flow) transport

  12. Dehydrated Prussian Blues for CO2 Storage and Separation Applications

    SciTech Connect

    Motkuri, Radha K.; Thallapally, Praveen K.; McGrail, B. Peter; Ghorishi, Behrooz S.

    2010-08-13

    Adsorption isotherms of pure gases present in flue and natural gas including CO2, N2, CH4 and water were studied using prussian blues of chemical formula M3[Co(CN)6]2 (M = Cu, Ni, Mn). These materials adsorbed 8-12 wt % of CO2 at room temperature and 1 bar of pressure with heats of adsorption ranging from 6 to 16 kcal/mol.

  13. Capture of CO2 From Recirculating Flue Gas Boilers

    SciTech Connect

    Ochs, Thomas L.

    2003-01-01

    The possible need for an economical method for the separation of CO2 from flue gas adds a new set of challenges to power plant design, construction, operation, and maintenance. Many of the new requirements of CO2 separation are similar in nature to those addressed by the mature chemical engineering processes used in petroleum refining and industrial chemical production. Chemical engineering processes are regularly used to separate heterogeneous vapors in processes such as the fractionation of hydrocarbons or the separation of the components of air. This paper addresses the application of chemical engineering processes to the mixtures of gases and vapors found in the flue gas of recirculating boilers. Adaptation of these techniques can lead to a reduction in the energy required to capture CO2.

  14. Lessons from Natural CO2 Leakage Analogue Site Studies and their Application to Secure CO2 Storage and Monitoring

    NASA Astrophysics Data System (ADS)

    Han, W.; McPherson, B. J.; Kim, K.; Chae, G.; Yum, B.

    2011-12-01

    related chemical reactions in the observation wells and tested with numerical simulation tools, which predicted thermal processes caused by solid NaCl precipitation, buoyancy-driven supercritical CO2 migration, and potential non-isothermal effects. Simulation results suggest that these processes - solid NaCl precipitation, buoyancy effects, Joule-Thomson cooling, water vaporization, and exothermic CO2 reactions - are strongly coupled and dynamic (transient). Overall, a fundamental understanding of potential thermal processes investigated through this research will be beneficial in the collection and analysis of temperature signals collectively measured from monitoring wells.

  15. Estimation of continuous anthropogenic CO2 using CO2, CO, δ13C(CO2) and Δ14C(CO2)

    NASA Astrophysics Data System (ADS)

    Vardag, S. N.; Gerbig, C.; Janssens-Maenhout, G.; Levin, I.

    2015-07-01

    We investigate different methods for estimating anthropogenic CO2 using modelled continuous atmospheric concentrations of CO2 alone, as well as CO2 in combination with the surrogate tracers CO, δ13C(CO2) and Δ14C(CO2). These methods are applied at three hypothetical stations representing rural, urban and polluted conditions. We find that independent of the tracer used, an observation-based estimate of continuous anthropogenic CO2 is not feasible at rural measurement sites due to the low signal to noise ratio of anthropogenic CO2 estimates at such settings. At urban and polluted sites, potential future continuous Δ14C(CO2) measurements with a precision of 5 ‰ or better are most promising for anthropogenic CO2 determination (precision ca. 10-20%), but the insensitivity against CO2 contributions from biofuel emissions may reduce its accuracy in the future. Other tracers, such as δ13C(CO2) and CO could provide an accurate and already available alternative if all CO2 sources in the catchment area are well characterized with respect to their isotopic signature and CO to anthropogenic CO2 ratio. We suggest a strategy for calibrating these source characteristics on an annual basis using precise Δ14C(CO2) measurements on grab samples. The precision of anthropogenic CO2 determination using δ13C(CO2) is largely determined by the measurement precision of δ13C(CO2) and CO2. The precision when using the CO-method is mainly limited by the variation of natural CO sources and CO sinks. At present, continuous anthropogenic CO2 could be determined using the tracers δ13C(CO2) and/or CO with a precision of about 30 %, a mean bias of about 10 % and without significant diurnal discrepancies. This allows significant improvement, validation and bias reduction of highly resolved emission inventories using atmospheric observation and regional modelling.

  16. The reactivity of CO2 with K atoms adsorbed on MgO powders.

    PubMed

    Preda, Gloria; Pacchioni, Gianfranco; Chiesa, Mario; Giamello, Elio

    2009-10-01

    In this combined quantum chemical and EPR study we have investigated the formation of CO(2)(-) radicals by contact of CO(2) molecules with a K precovered MgO surface. K atoms have been deposited on polycrystalline MgO samples, and then exposed to CO(2). The typical EPR signal of the isolated K atoms disappears when the reaction with CO(2) takes place and a new paramagnetic species attributed to CO(2)(-) is observed. DFT cluster model calculations show that there is a spontaneous electron transfer from the adsorbed K atom to the CO(2) molecule, with formation of K(+)CO(2)(-) surface complexes. These species have the same electronic characteristics and spin distribution of gas-phase M(+)CO(2)(-) (M = Li, Na, K) molecules, but are stabilized by the presence of the ionic surface. The most stable MgO sites where the adsorption of CO(2) occurs and the computed EPR properties are discussed.

  17. Technological advances in CO2 conversion electro-biorefinery: A step toward commercialization.

    PubMed

    ElMekawy, Ahmed; Hegab, Hanaa M; Mohanakrishna, Gunda; Elbaz, Ashraf F; Bulut, Metin; Pant, Deepak

    2016-09-01

    The global atmospheric warming due to increased emissions of carbon dioxide (CO2) has attracted great attention in the last two decades. Although different CO2 capture and storage platforms have been proposed, the utilization of captured CO2 from industrial plants is progressively prevalent strategy due to concerns about the safety of terrestrial and aquatic CO2 storage. Two utilization forms were proposed, direct utilization of CO2 and conversion of CO2 to chemicals and energy products. The latter strategy includes the bioelectrochemical techniques in which electricity can be used as an energy source for the microbial catalytic production of fuels and other organic products from CO2. This approach is a potential technique in which CO2 emissions are not only reduced, but it also produce more value-added products. This review article highlights the different methodologies for the bioelectrochemical utilization of CO2, with distinctive focus on the potential opportunities for the commercialization of these techniques.

  18. Surface Condensation of CO2 onto Kaolinite

    SciTech Connect

    Schaef, Herbert T.; Glezakou, Vassiliki Alexandra; Owen, Antionette T.; Ramprasad, Sudhir; Martin, Paul F.; McGrail, B. Peter

    2014-02-11

    The fundamental adsorption behavior of gaseous and supercritical carbon dioxide (CO2) onto poorly crystalline kaolinite (KGa-2) at conditions relevant to geologic sequestration has been investigated using a quartz crystal microbalance (QCM) and density functional theory (DFT) methods. The QCM data indicated linear adsorption of CO2 (0-0.3 mmol CO2/g KGa-2) onto the kaolinite surface up through the gaseous state (0.186 g/cm3). However in the supercritical region, CO2 adsorption increases dramatically, reaching a peak (0.9-1.0 mmol CO2/g KGa-2) near 0.43 g/cm3, before declining rapidly to surface adsorption values equivalent or below gaseous CO2. This adsorption profile was not observed with He or N2. Comparative density functional studies of CO2 interactions with kaolinite surface models rule out CO2 intercalation and confirm that surface adsorption is favored up to approximately 0.35 g/cm3 of CO2, showing distorted T-shaped CO2-CO2 clustering, typical of supercritical CO2 aggregation over the surface as the density increases. Beyond this point, the adsorption energy gain for any additional CO2 becomes less than the CO2 interaction energy (~0.2 eV) in the supercritical medium resulting in overall desorption of CO2 from the kaolinite surface.

  19. Outsourcing CO2 within China

    PubMed Central

    Feng, Kuishuang; Davis, Steven J.; Sun, Laixiang; Li, Xin; Guan, Dabo; Liu, Weidong; Liu, Zhu; Hubacek, Klaus

    2013-01-01

    Recent studies have shown that the high standard of living enjoyed by people in the richest countries often comes at the expense of CO2 emissions produced with technologies of low efficiency in less affluent, developing countries. Less apparent is that this relationship between developed and developing can exist within a single country’s borders, with rich regions consuming and exporting high-value goods and services that depend upon production of low-cost and emission-intensive goods and services from poorer regions in the same country. As the world’s largest emitter of CO2, China is a prominent and important example, struggling to balance rapid economic growth and environmental sustainability across provinces that are in very different stages of development. In this study, we track CO2 emissions embodied in products traded among Chinese provinces and internationally. We find that 57% of China’s emissions are related to goods that are consumed outside of the province where they are produced. For instance, up to 80% of the emissions related to goods consumed in the highly developed coastal provinces are imported from less developed provinces in central and western China where many low–value-added but high–carbon-intensive goods are produced. Without policy attention to this sort of interprovincial carbon leakage, the less developed provinces will struggle to meet their emissions intensity targets, whereas the more developed provinces might achieve their own targets by further outsourcing. Consumption-based accounting of emissions can thus inform effective and equitable climate policy within China. PMID:23754377

  20. Environmental potential of the use of CO2 from alcoholic fermentation processes. The CO2-AFP strategy.

    PubMed

    Alonso-Moreno, Carlos; García-Yuste, Santiago

    2016-10-15

    A novel Carbon Dioxide Utilization (CDU) approach from a relatively minor CO2 emission source, i.e., alcoholic fermentation processes (AFP), is presented. The CO2 produced as a by-product from the AFP is estimated by examining the EtOH consumed per year reported by the World Health Organization in 2014. It is proposed that the extremely pure CO2 from the AFP is captured in NaOH solutions to produce one of the Top 10 commodities in the chemical industry, Na2CO3, as a good example of an atomic economy process. The novel CDU strategy could yield over 30.6Mt of Na2CO3 in oversaturated aqueous solution on using ca. 12.7Mt of captured CO2 and this process would consume less energy than the synthetic methodology (Solvay ammonia soda process) and would not produce low-value by-products. The quantity of Na2CO3 obtained by this strategy could represent ca. 50% of the world Na2CO3 production in one year. In terms of the green economy, the viability of the strategy is discussed according to the recommendations of the CO2Chem network, and an estimation of the CO2negative emission achieved suggests a capture of around 280.0Mt of CO2 from now to 2020 or ca. 1.9Gt from now to 2050. Finally, the results obtained for this new CDU proposal are discussed by considering different scenarios; the CO2 production in a typical winemaking corporation, the CO2 released in the most relevant wine-producing countries, and the use of CO2 from AFP as an alternative for the top Na2CO3-producing countries.

  1. Isentropic transport and the seasonal cycle amplitude of CO2

    NASA Astrophysics Data System (ADS)

    Barnes, Elizabeth A.; Parazoo, Nicholas; Orbe, Clara; Denning, A. Scott

    2016-07-01

    Carbon-concentration feedbacks and carbon-climate feedbacks constitute one of the largest sources of uncertainty in future climate. Since the beginning of the modern atmospheric CO2 record, seasonal variations in CO2 have been recognized as a signal of the metabolism of land ecosystems, and quantitative attribution of changes in the seasonal cycle amplitude (SCA) of CO2 to ecosystem processes is critical for understanding and projecting carbon-climate feedbacks far into the 21st Century. Here the impact of surface carbon fluxes on the SCA of CO2 throughout the Northern Hemisphere troposphere is investigated, paying particular attention to isentropic transport across latitudes. The analysis includes both a chemical transport model GOES-Chem and an idealized tracer in a gray-radiation aquaplanet. The results of the study can be summarized by two main conclusions: (1) the SCA of CO2 roughly follows surfaces of constant potential temperature, which can explain the observed increase in SCA with latitude along pressure surfaces and (2) increasing seasonal fluxes in lower latitudes have a larger impact on the SCA of CO2 throughout most of the troposphere compared to increasing seasonal fluxes in higher latitudes. These results provide strong evidence that recently observed changes in the SCA of CO2 at high northern latitudes (poleward of 60°N) are likely driven by changes in midlatitude surface fluxes, rather than changes in Arctic fluxes.

  2. CO2 Infrared Phonon Modes in Interstellar Ice Mixtures

    NASA Astrophysics Data System (ADS)

    Cooke, Ilsa R.; Fayolle, Edith C.; Öberg, Karin I.

    2016-11-01

    CO2 ice is an important reservoir of carbon and oxygen in star- and planet-forming regions. Together with water and CO, CO2 sets the physical and chemical characteristics of interstellar icy grain mantles, including desorption and diffusion energies for other ice constituents. A detailed understanding of CO2 ice spectroscopy is a prerequisite to characterize CO2 interactions with other volatiles both in interstellar ices and in laboratory experiments of interstellar ice analogs. We report laboratory spectra of the CO2 longitudinal optical (LO) phonon mode in pure CO2 ice and in CO2 ice mixtures with H2O, CO, and O2 components. We show that the LO phonon mode position is sensitive to the mixing ratio of various ice components of astronomical interest. In the era of the James Webb Space Telescope, this characteristic could be used to constrain interstellar ice compositions and morphologies. More immediately, LO phonon mode spectroscopy provides a sensitive probe of ice mixing in the laboratory and should thus enable diffusion measurements with higher precision than has been previously possible.

  3. Integrated electromicrobial conversion of CO2 to higher alcohols.

    PubMed

    Li, Han; Opgenorth, Paul H; Wernick, David G; Rogers, Steve; Wu, Tung-Yun; Higashide, Wendy; Malati, Peter; Huo, Yi-Xin; Cho, Kwang Myung; Liao, James C

    2012-03-30

    One of the major challenges in using electrical energy is the efficiency in its storage. Current methods, such as chemical batteries, hydraulic pumping, and water splitting, suffer from low energy density or incompatibility with current transportation infrastructure. Here, we report a method to store electrical energy as chemical energy in higher alcohols, which can be used as liquid transportation fuels. We genetically engineered a lithoautotrophic microorganism, Ralstonia eutropha H16, to produce isobutanol and 3-methyl-1-butanol in an electro-bioreactor using CO(2) as the sole carbon source and electricity as the sole energy input. The process integrates electrochemical formate production and biological CO(2) fixation and higher alcohol synthesis, opening the possibility of electricity-driven bioconversion of CO(2) to commercial chemicals.

  4. Supersonic Technology for CO2 Capture: A High Efficiency Inertial CO2 Extraction System

    SciTech Connect

    2010-07-01

    IMPACCT Project: Researchers at ATK and ACENT Laboratories are developing a device that relies on aerospace wind-tunnel technologies to turn CO2 into a condensed solid for collection and capture. ATK’s design incorporates a special nozzle that converges and diverges to expand flue gas, thereby cooling it off and turning the CO2 into solid particles which are removed from the system by a cyclonic separator. This technology is mechanically simple, contains no moving parts and generates no chemical waste, making it inexpensive to construct and operate, readily scalable, and easily integrated into existing facilities. The increase in the cost to coal-fired power plants associated with introduction of this system would be 50% less than current technologies.

  5. Assessment of full-scale biological nutrient removal systems upgraded with physico-chemical processes for the removal of emerging pollutants present in wastewaters from Mexico.

    PubMed

    Estrada-Arriaga, Edson Baltazar; Cortés-Muñoz, Juana Enriqueta; González-Herrera, Arturo; Calderón-Mólgora, César Guillermo; de Lourdes Rivera-Huerta, Ma; Ramírez-Camperos, Esperanza; Montellano-Palacios, Leticia; Gelover-Santiago, Silvia Lucila; Pérez-Castrejón, Sara; Cardoso-Vigueros, Lina; Martín-Domínguez, Alejandra; García-Sánchez, Liliana

    2016-11-15

    Two full-scale biological nutrient removal systems upgraded with three physico-chemical processes (coagulation, chemical precipitation, and neutral Fenton) were evaluated in order to determine the removal of emerging pollutants (EPs) present in municipal wastewater from Mexico. Between 41 and 55 EPs were detected in the influents of two wastewater treatment plants (WWTPs), including personal care products (PPCPs), antibiotics, analgesics, antiepileptics, antilipidemics, antihypertensives, antiseptics, stimulants, and hormones. Emerging pollutants were detected at concentrations ranging from 0.69ng/L to 94,600ng/L. High concentrations of emerging pollutants were found during dry season. WWTP 1, integrated by oxidation ditches and UV light lamps, showed removal efficiencies of EPs between 20% and 22%. On the other hand, WWTP 2 consisted of anaerobic/anoxic/aerobic tanks coupled with two disinfection processes; chlorine dioxide and UV light lamps, for which the removal of EPs was significant (up to 80%). The concentrations of emerging pollutants in WWTP 1 effluent was found within a range

  6. CO2 Utilization and Storage in Shale Gas Reservoirs

    NASA Astrophysics Data System (ADS)

    Schaef, T.; Glezakou, V.; Owen, T.; Miller, Q.; Loring, J.; Davidson, C.; McGrail, P.

    2013-12-01

    supercritical CO2. Additional experiments were conducted with pressurized attenuated total reflectance infrared spectroscopy technique that tracked clay hydration, gas adsorption, and water concentrations in the fluids during exposure to CO2 and CH4. These fundamental physico-chemical data are being collected into a database for parameterization of multiphase flow and reactive transport simulations of the CO2 injection, trapping, and secondary methane in fractured shales.

  7. CO2-induced changes in mineral stoichiometry of wheat grains

    NASA Astrophysics Data System (ADS)

    Broberg, Malin; Pleijel, Håkan; Högy, Petra

    2016-04-01

    positive environmental effect and possibly as a result of reduced transpiration under eCO2, since uptake and transport of Cd is known to be related to transpiration. For elements with substantial data the response in OTC and FACE exposure systems could be compared and no large differences were observed. Our study shows that eCO2 has a significant effect on the mineral composition of wheat grain. This has strong implications for human nutrition in a world of rising CO2 concentrations. An altered chemical composition of biomass under eCO2 is also of great importance for the biogeochemical cycling of elements in general.

  8. The rise and fall of carbon dioxide: Why controlling CO2 may be necessary in greenhouses

    Technology Transfer Automated Retrieval System (TEKTRAN)

    In the winter production cycle, many of us focus on sealing up gaps in an effort to decrease air infiltration, and cut our heating bills substantially along the way. While making these changes or upgrades, we ignoring something the potential impact this has on carbon dioxide (CO2) and plant growth. ...

  9. Nutrient removal and biogas upgrading by integrating freshwater algae cultivation with piggery anaerobic digestate liquid treatment.

    PubMed

    Xu, Jie; Zhao, Yongjun; Zhao, Guohua; Zhang, Hui

    2015-08-01

    An integrated approach that combined freshwater microalgae Scenedesmus obliquus (FACHB-31) cultivation with piggery anaerobic digestate liquid treatment was investigated in this study. The characteristics of algal growth, biogas production, and nutrient removal were examined using photobioreactor bags (PBRbs) to cultivate S. obliquus (FACHB-31) in digestate with various digestate dilutions (the concentration levels of 3200, 2200, 1600, 1200, 800, and 400 mg L(-1) chemical oxygen demand (COD)) during 7-day period. The effects of the level of pollutants on nutrient removal efficiency and CO2 removal process were investigated to select the optimum system for effectively upgrade biogas and simultaneously reduce the nutrient content in digestate. The treatment performance displayed that average removal rates of COD, total nitrogen (TN), total phosphorous (TP), and CO2 were 61.58-75.29, 58.39-74.63, 70.09-88.79, and 54.26-73.81 %, respectively. All the strains grew well under any the dilution treatments. With increased initial nutrient concentration to a certain range, the CO4 content (v/v) of raw biogas increased. Differences in the biogas enrichment of S. obliquus (FACHB-31) in all treatments mainly resulted from variations in biomass productivity and CO2 uptake. Notably, the diluted digestate sample of 1600 mg L(-1) COD provided an optimal nutrient concentration for S. obliquus (FACHB-31) cultivation, where the advantageous nutrient and CO2 removals, as well as the highest productivities of biomass and biogas upgrading, were revealed. Results showed that microalgal biomass production offered real opportunities to address issues such as CO2 sequestration, wastewater treatment, and biogas production.

  10. Sources/sinks analysis with satellite sensing for exploring global atmospheric CO2 distributions

    NASA Astrophysics Data System (ADS)

    Shim, C.; Nassar, R.; Kim, J.

    2010-12-01

    There is growing interest in CO2 budget analysis since space-borne measurements of global CO2 distribution have been conducted (e.g, GOSAT project). Here we simulated the global CO2 distribution to estimate individual source/sink contributions. The chemical transport model (GEOS-Chem) was used in order to simulate the global CO2 distribution with updated global sources/sinks with 2°x2.5° horizontal resolution. In addition, 3-D emissions from aviation and chemical oxidation of CO are implemented. The model simulated CO2 amounts were compared with the GOSAT column averaged CO2 column (SWIR L2 data) from April 2009 to May 2010. The seasonal cycles of CO2 concentration were compared and the regional patterns of CO2 distribution are explained by the model with a systemic difference by 1 ~ 2% in the CO2 concentration. In other work, the GEOS-Chem CO2 concentrations show reasonable agreement with GLOBALVIEW-CO2. We further estimated the sources/sinks contributions to the global CO2 budget through 9 tagged CO2 tracers (fossil fuels, ocean exchanges, biomass burning, biofuel burning, balanced biosphere, net terrestrial exchange, ship emissions, aviation emissions, and oxidation from carbon precursors) over the years 2005-2009. Global CO2 concentration shows an increase of 2.1 ppbv/year in which the human fossil fuel and cement emissions are the main driving force (5.0 ppbv/year) for the trend. Net terrestrial and oceanic exchange of CO2 are main sinks (-2.1 ppbv/year and -0.7 ppbv/year, respectively). Our model results will help to suggest the level of reduction in global human CO2 emissions which could control the global CO2 trends in 21th century.

  11. Lasers utilizing CO2 isotopes

    NASA Astrophysics Data System (ADS)

    Pechenin, Yu V.; Domanov, M. S.

    1980-08-01

    The lasing spectra and energy characteristics were investigated for lasers operating with the isotopes 12C16O2, 13C16O2, 12C18O2, and 12C16O18O. It was found that the output power of a laser utilizing the CO2 isotopes was determined by the content of a particular isotope in the carbon dioxide gas. For equal enrichments, all the isotopes investigated, with the exception of 12C16O18O, gave comparable output powers. The unsaturated gains were identical for the most intense transitions of the symmetric molecules; the gain was a factor of two less for the asymmetric molecule. The gain rose linearly with increasing enrichment. The ultimate specific power output, given by the product of the saturation power density and the gain, was practically independent of the enrichment.

  12. Direct Capture of CO2 from Ambient Air.

    PubMed

    Sanz-Pérez, Eloy S; Murdock, Christopher R; Didas, Stephanie A; Jones, Christopher W

    2016-10-12

    The increase in the global atmospheric CO2 concentration resulting from over a century of combustion of fossil fuels has been associated with significant global climate change. With the global population increase driving continued increases in fossil fuel use, humanity's primary reliance on fossil energy for the next several decades is assured. Traditional modes of carbon capture such as precombustion and postcombustion CO2 capture from large point sources can help slow the rate of increase of the atmospheric CO2 concentration, but only the direct removal of CO2 from the air, or "direct air capture" (DAC), can actually reduce the global atmospheric CO2 concentration. The past decade has seen a steep rise in the use of chemical sorbents that are cycled through sorption and desorption cycles for CO2 removal from ultradilute gases such as air. This Review provides a historical overview of the field of DAC, along with an exhaustive description of the use of chemical sorbents targeted at this application. Solvents and solid sorbents that interact strongly with CO2 are described, including basic solvents, supported amine and ammonium materials, and metal-organic frameworks (MOFs), as the primary classes of chemical sorbents. Hypothetical processes for the deployment of such sorbents are discussed, as well as the limited array of technoeconomic analyses published on DAC. Overall, it is concluded that there are many new materials that could play a role in emerging DAC technologies. However, these materials need to be further investigated and developed with a practical sorbent-air contacting process in mind if society is to make rapid progress in deploying DAC as a means of mitigating climate change.

  13. CO2 Sequestration and Recycle by Photosynthesis

    SciTech Connect

    Steven S.C. Chuang

    2004-02-01

    Visible light-photocatalysis could provide a cost-effective route to recycle CO2 to useful chemicals or fuels. Research is planned to study the reactivity of adsorbates, their role in the photosynthesis reaction, and their relation to the nature of surface sites during photosynthesis of methanol and hydrocarbons from CO{sub 2}/H{sub 2}O. The year two research focus catalyst screening and IR studies. Key research results show Pd/TiO2 exhibits the highest activity for hydrocarbon synthesis from photocatalytic reactions. The in situ IR could successfully monitor the adsorbate hydrocarbon species on Cu/TiO2. Year III research will focus on developing a better understanding of the key factors which control the catalyst activity.

  14. A Critical Assessment of Microbiological Biogas to Biomethane Upgrading Systems.

    PubMed

    Rittmann, Simon K-M R

    2015-01-01

    Microbiological biogas upgrading could become a promising technology for production of methane (CH(4)). This is, storage of irregular generated electricity results in a need to store electricity generated at peak times for use at non-peak times, which could be achieved in an intermediate step by electrolysis of water to molecular hydrogen (H(2)). Microbiological biogas upgrading can be performed by contacting carbon dioxide (CO(2)), H(2) and hydrogenotrophic methanogenic Archaea either in situ in an anaerobic digester, or ex situ in a separate bioreactor. In situ microbiological biogas upgrading is indicated to require thorough bioprocess development, because only low volumetric CH(4) production rates and low CH(4) fermentation offgas content have been achieved. Higher volumetric production rates are shown for the ex situ microbiological biogas upgrading compared to in situ microbiological biogas upgrading. However, the ex situ microbiological biogas upgrading currently suffers from H(2) gas liquid mass transfer limitation, which results in low volumetric CH(4) productivity compared to pure H(2)/CO(2) conversion to CH(4). If waste gas utilization from biological and industrial sources can be shown without reduction in volumetric CH(4) productivity, as well as if the aim of a single stage conversion to a CH(4) fermentation offgas content exceeding 95 vol% can be demonstrated, ex situ microbiological biogas upgrading with pure or enrichment cultures of methanogens could become a promising future technology for almost CO(2)-neutral biomethane production.

  15. Circulation of waste materials, water, CO2, and O2, and production of food and animal feed within a closed and controlled system comprised of humans, goats, crops, and physical/chemical system

    NASA Astrophysics Data System (ADS)

    Tako, Yasuhiro; Tako, Yasuhiro; Tsuga, Shou-Ichi; Komatsubara, Osamu; Aibe, You-Ichi; Nozoe, Susumu; Arai, Ryuji; Tani, Takashi; Ishioka, Masanao; Masuda, Tsuyoshi; Abe, Koichi; Nakamura, Yuji

    Two humans and two goats inhabited and crops were cultivated within the Closed Ecology Experiment Facilities (CEEF). Circulation of waste in addition to circulation of water, O2 and CO2, and supply of food and animal feed from crops cultivated in the CEEF was conducted in the experiments. The two humans lived and worked in the Plant Module (PM) and the Animal and Human habitation Module (AHM) of the CEEF during 28 days at muximum continuously in 2007.

  16. Understanding chemical reactions of CO2 and its isoelectronic molecules with 1-butyl-3-methylimidazolium acetate by changing the nature of the cation: the case of CS2 in 1-butyl-1-methylpyrrolidinium acetate studied by NMR spectroscopy and density functional theory calculations.

    PubMed

    Cabaço, M Isabel; Besnard, Marcel; Chávez, Fabián Vaca; Pinaud, Noël; Sebastião, Pedro J; Coutinho, João A P; Danten, Yann

    2014-06-28

    NMR spectroscopy ((1)H, (13)C, (15)N) shows that carbon disulfide reacts spontaneously with 1-butyl-1-methylpyrrolidinium acetate ([BmPyrro][Ac]) in the liquid phase. It is found that the acetate anions play an important role in conditioning chemical reactions with CS2 leading, via coupled complex reactions, to the degradation of this molecule to form thioacetate anion (CH3COS(-)), CO2, OCS, and trithiocarbonate (CS3 (2-)). In marked contrast, the cation does not lead to the formation of any adducts allowing to conclude that, at most, its role consists in assisting indirectly these reactions. The choice of the [BmPyrro](+) cation in the present study allows disentangling the role of the anion and the cation in the reactions. As a consequence, the ensemble of results already reported on CS2-[Bmim][Ac] (1), OCS-[Bmim][Ac] (2), and CO2-[Bmim][Ac] (3) systems can be consistently rationalized. It is argued that in system (1) both anion and cation play a role. The CS2 reacts with the acetate anion leading to the formation of CH3COS(-), CO2, and OCS. After these reactions have proceeded the nascent CO2 and OCS interact with the cation to form imidazolium-carboxylate ([Bmim] CO2) and imidazolium-thiocarboxylate ([Bmim] COS). The same scenario also applies to system (2). In contrast, in the CO2-[Bmim] [Ac] system a concerted cooperative process between the cation, the anion, and the CO2 molecule takes place. A carbene issued from the cation reacts to form the [Bmim] CO2, whereas the proton released by the ring interacts with the anion to produce acetic acid. In all these systems, the formation of adduct resulting from the reaction between the solute molecule and the carbene species originating from the cation is expected. However, this species was only observed in systems (2) and (3). The absence of such an adduct in system (1) has been theoretically investigated using DFT calculations. The values of the energetic barrier of the reactions show that the formation of [Bmim

  17. 76 FR 15249 - Deferral for CO2

    Federal Register 2010, 2011, 2012, 2013, 2014

    2011-03-21

    ... area of land. Carbon can cycle fairly rapidly back to the atmosphere or it can remain stored on land... Deterioration (PSD) and Title V permitting requirements to biogenic carbon dioxide (CO 2 ) emissions from... Information CFR Code of Federal Regulations CH 4 methane CO 2 Carbon dioxide CO 2 e Carbon dioxide...

  18. Throwing new light on the reduction of CO2.

    PubMed

    Ozin, Geoffrey A

    2015-03-18

    While the chemical energy in fossil fuels has enabled the rapid rise of modern civilization, their utilization and accompanying anthropogenic CO2 emissions is occurring at a rate that is outpacing nature's carbon cycle. Its effect is now considered to be irreversible and this could lead to the demise of human society. This is a complex issue without a single solution, yet from the burgeoning global research activity and development in the field of CO2 capture and utilization, there is light at the end of the tunnel. In this article a couple of recent advances are illuminated. Attention is focused on the discovery of gas-phase, light-assisted heterogeneous catalytic materials and processes for CO2 photoreduction that operate at sufficiently high rates and conversion efficiencies, and under mild conditions, to open a new pathway for an energy transition from today's "fossil fuel economy" to a new and sustainable "CO2 economy". Whichever of the competing CO2 capture and utilization approaches proves to be the best way forward for the development of a future CO2-based solar fuels economy, hopefully this can occur in a period short enough to circumvent the predicted adverse consequences of greenhouse gas climate change.

  19. Sorbents for CO2 capture from high carbon fly ashes.

    PubMed

    Maroto-Valer, M Mercedes; Lu, Zhe; Zhang, Yinzhi; Tang, Zhong

    2008-11-01

    Fly ashes with high-unburned-carbon content, referred to as fly ash carbons, are an increasing problem for the utility industry, since they cannot be marketed as a cement extender and, therefore, have to be disposed. Previous work has explored the potential development of amine-enriched fly ash carbons for CO2 capture. However, their performance was lower than that of commercially available sorbents, probably because the samples investigated were not activated prior to impregnation and, therefore, had a very low surface area. Accordingly, the work described here focuses on the development of activated fly ash derived sorbents for CO2 capture. The samples were steam activated at 850 degrees C, resulting in a significant increase of the surface area (1075 m2/g). The activated samples were impregnated with different amine compounds, and the resultant samples were tested for CO2 capture at different temperatures. The CO2 adsorption of the parent and activated samples is typical of a physical adsorption process. The impregnation process results in a decrease of the surface areas, indicating a blocking of the porosity. The highest adsorption capacity at 30 and 70 degrees C for the amine impregnated activated carbons was probably due to a combination of physical adsorption inherent from the parent sample and chemical adsorption of the loaded amine groups. The CO2 adsorption capacities for the activated amine impregnated samples are higher than those previously published for fly ash carbons without activation (68.6 vs. 45 mg CO2/g sorbent).

  20. Public Acceptance for Geological CO2-Storage

    NASA Astrophysics Data System (ADS)

    Schilling, F.; Ossing, F.; Würdemann, H.; Co2SINK Team

    2009-04-01

    for public, press, NGOs,…). - being open for visitors (first of all for the local!) often we informed the public together with the mining authorities - being open for podium discussions and presentation etc. - organized by NGOs, Student groups, press, politics, scientific meetings… Since people usually trust scientists more than politicians and companies, scientists have an enhanced responsibility while informing the public. Once again - always tell the truth and take care of your credibility! In this case, it was most helpful that the project was embedded in the broad scientific activity of research centre which seems to have given the project a positive neutral background. As many people have an undefined fear of all operations in the underground, we tried to address all issues related to storage. Ranging from the transport, injection facility, technical installation, safety of the storage site, the wells, hydraulic system, chemical reactions etc.. When addressing all major concerns before people ask, confidence to the scientists is kept high. We never said that there is absolutely no risk (by the way, nobody would believe that!) we weighted the risk with respect to health, safety and environmental HSE issues. We explained in detail the different trapping mechanisms of the storage operation. This has to be done according to the social groups involved. For the broad public common analogues were helpful: - Trapping in the pore space - a sponge - Trapping through a tight cap rock - a bottle of mineral water with a crown cap as seal - Chemical Trapping - opening of a bottle of mineral water - Well bore integrity - problem of retightening of a bottle with a crown cap - Sucking in of fluid -instead of releasing a sandstone sample standing partly in water - Injecting of CO2 - using a soda machine - Often the concern of burning gas is addressed - showing a CO2 fire extinguisher -CO is poisonous, CO2 not: - drinking soda or even better? champaigne Beyond information of

  1. Thermal injuries as a result of CO2 laser resurfacing.

    PubMed

    Grossman, A R; Majidian, A M; Grossman, P H

    1998-09-01

    CO2 laser resurfacing of the face for fine wrinkles has gained great popularity over a short period of time. The use of the CO2 laser has proven to be effective in reducing or eliminating fine wrinkles. This tool in the surgeon's armamentarium has been added to those of dermabrasion and chemical peel. The theoretical advantage of the use of the CO2 laser for resurfacing has been better accuracy and reportedly more control of the depth of penetration. The use of the CO2 laser has been welcomed by many cosmetic surgeons. Until now, there have been few reported cases of complications with the use of the CO2 laser. To many, this would sound too good to be true; unfortunately, that is the case. The CO2 laser is a high-energy machine that can indeed cause thermal injury. This thermal injury can result in deep burns to the skin and hypertrophic scarring. We feel this is more common than is currently being reported, and we share our experience as a burn and wound care referral service. During an 18-month period, 20 consecutive patients were referred to our practice who had received injuries from the CO2 laser resurfacing laser. We present here in this review a summary of those injuries. The CO2 resurfacing laser is a very effective tool for the treatment of fine wrinkles, but it is not without the potential for serious complications. We urge caution with the use of the laser and prompt recognition and treatment of thermal injury to the skin.

  2. Reversible Acid Gas Capture Using CO2-Binding Organic Liquids

    SciTech Connect

    Heldebrant, David J.; Koech, Phillip K.; Yonker, Clement R.; Rainbolt, James E.; Zheng, Feng

    2010-08-31

    Acid gas scrubbing technology is predominantly aqueous alkanolamine based. Of the acid gases, CO2, H2S and SO2 have been shown to be reversible, however there are serious disadvantages with corrosion and high regeneration costs. The primary scrubbing system composed of monoethanolamine is limited to 30% by weight because of the highly corrosive solution. This gravimetric limitation limits the CO2 volumetric (≤108 g/L) and gravimetric capacity (≤7 wt%) of the system. Furthermore the scrubbing system has a large energy penalty from pumping and heating the excess water required to dissolve the MEA bicarbonate salt. Considering the high specific heat of water (4 j/g-1K-1), low capacities and the high corrosion we set out to design a fully organic solvent that can chemically bind all acid gases i.e. CO2 as reversible alkylcarbonate ionic liquids or analogues thereof. Having a liquid acid gas carrier improves process economics because there is no need for excess solvent to pump and to heat. We have demonstrated illustrated in Figure 1, that CO2-binding organic liquids (CO2BOLs) have a high CO2 solubility paired with a much lower specific heat (<1.5 J/g-1K-1) than aqueous systems. CO2BOLs are a subsection of a larger class of materials known as Binding Organic Liquids (BOLs). Our BOLs have been shown to reversibly bind and release COS, CS2, and SO2, which we denote COSBOLS, CS2BOLs and SO2BOLs. Our BOLs are highly tunable and can be designed for post or pre-combustion gas capture. The design and testing of the next generation zwitterionic CO2BOLs and SO2BOLs are presented.

  3. Forest succession at elevated CO2

    SciTech Connect

    Clark, James S.; Schlesinger, William H.

    2002-02-01

    We tested hypotheses concerning the response of forest succession to elevated CO2 in the FACTS-1 site at the Duke Forest. We quantified growth and survival of naturally recruited seedlings, tree saplings, vines, and shrubs under ambient and elevated CO2. We planted seeds and seedlings to augment sample sites. We augmented CO2 treatments with estimates of shade tolerance and nutrient limitation while controlling for soil and light effects to place CO2 treatments within the context of natural variability at the site. Results are now being analyzed and used to parameterize forest models of CO2 response.

  4. Isotopic CO2 Instrumentation for UAV Measurements

    NASA Astrophysics Data System (ADS)

    Gomez, A.; Silver, J.

    2013-12-01

    Carbon dioxide is the largest component of anthroprogenic green house gas emissions. Knowing atmospheric 13CO2/12CO2 ratios precisely is important for understanding biogenic and anthroprogenic sources and sinks for carbon. Instrumentation mounted on UAV aircraft would enable important spatial isotopic CO2 information. However, current isotopic CO2 instrumentation have unfavorable attributes for UAV use, such as high power requirements, high cost, high weight, and large size. Here we present the early development of a compact isotopic CO2 instrument that is designed to nullify effects of pressure, temperature and moisture, and will ultimately be suitable for UAV deployment.

  5. Aminosilicone solvents for CO(2) capture.

    PubMed

    Perry, Robert J; Grocela-Rocha, Teresa A; O'Brien, Michael J; Genovese, Sarah; Wood, Benjamin R; Lewis, Larry N; Lam, Hubert; Soloveichik, Grigorii; Rubinsztajn, Malgorzata; Kniajanski, Sergei; Draper, Sam; Enick, Robert M; Johnson, J Karl; Xie, Hong-bin; Tapriyal, Deepak

    2010-08-23

    This work describes the first report of the use of an aminosilicone solvent mix for the capture of CO(2). To maintain a liquid state, a hydroxyether co-solvent was employed which allowed enhanced physisorption of CO(2) in the solvent mixture. Regeneration of the capture solvent system was demonstrated over 6 cycles and absorption isotherms indicate a 25-50 % increase in dynamic CO(2) capacity over 30 % MEA. In addition, proof of concept for continuous CO(2) absorption was verified. Additionally, modeling to predict heats of reaction of aminosilicone solvents with CO(2) was in good agreement with experimental results.

  6. Heterogeneous catalytic conversion of CO2: a comprehensive theoretical review

    NASA Astrophysics Data System (ADS)

    Li, Yawei; Chan, Siew Hwa; Sun, Qiang

    2015-05-01

    The conversion of CO2 into fuels and useful chemicals has been intensively pursued for renewable, sustainable and green energy. However, due to the negative adiabatic electron affinity (EA) and large ionization potential (IP), the CO2 molecule is chemically inert, thus making the conversion difficult under normal conditions. Novel catalysts, which have high stability, superior efficiency and low cost, are urgently needed to facilitate the conversion. As the first step to design such catalysts, understanding the mechanisms involved in CO2 conversion is absolutely indispensable. In this review, we have summarized the recent theoretical progress in mechanistic studies based on density functional theory, kinetic Monte Carlo simulation, and microkinetics modeling. We focus on reaction channels, intermediate products, the key factors determining the conversion of CO2 in solid-gas interface thermocatalytic reduction and solid-liquid interface electrocatalytic reduction. Furthermore, we have proposed some possible strategies for improving CO2 electrocatalysis and also discussed the challenges in theory, model construction, and future research directions.

  7. CO2 Sequestration in Unmineable Coal Seams: Potential Environmental Impacts

    SciTech Connect

    Hedges, S.W.; Soong, Yee; McCarthy Jones, J.R.; Harrison, D.K.; Irdi, G.A.; Frommell, E.A.; Dilmore, R.M.; Pique, P.J.; Brown, T.D

    2005-09-01

    An initial investigation into the potential environmental impacts of CO2 sequestration in unmineable coal seams has been conducted, focusing on changes in the produced water during enhanced coalbed methane (ECBM) production using a CO2 injection process (CO2-ECBM). Two coals have been used in this study, the medium volatile bituminous Upper Freeport coal (APCS 1) of the Argonne Premium Coal Samples series, and an as-mined Pittsburgh #8 coal, which is a high volatile bituminous coal. Coal samples were reacted with either synthetic produced water or field collected produced water and gaseous carbon dioxide at 40 οC and 50 bar to evaluate the potential for mobilizing toxic metals during CO2-ECBM/sequestration. Microscopic and x-ray diffraction analysis of the post-reaction coal samples clearly show evidence of chemical reaction, and chemical analysis of the produced water shows substantial changes in composition. These results suggest that changes to the produced water chemistry and the potential for mobilizing toxic trace elements from coalbeds are important factors to be considered when evaluating deep, unmineable coal seams for CO2 sequestration.

  8. Microbial Growth under Supercritical CO2

    PubMed Central

    Peet, Kyle C.; Freedman, Adam J. E.; Hernandez, Hector H.; Britto, Vanya; Boreham, Chris; Ajo-Franklin, Jonathan B.

    2015-01-01

    Growth of microorganisms in environments containing CO2 above its critical point is unexpected due to a combination of deleterious effects, including cytoplasmic acidification and membrane destabilization. Thus, supercritical CO2 (scCO2) is generally regarded as a sterilizing agent. We report isolation of bacteria from three sites targeted for geologic carbon dioxide sequestration (GCS) that are capable of growth in pressurized bioreactors containing scCO2. Analysis of 16S rRNA genes from scCO2 enrichment cultures revealed microbial assemblages of varied complexity, including representatives of the genus Bacillus. Propagation of enrichment cultures under scCO2 headspace led to isolation of six strains corresponding to Bacillus cereus, Bacillus subterraneus, Bacillus amyloliquefaciens, Bacillus safensis, and Bacillus megaterium. Isolates are spore-forming, facultative anaerobes and capable of germination and growth under an scCO2 headspace. In addition to these isolates, several Bacillus type strains grew under scCO2, suggesting that this may be a shared feature of spore-forming Bacillus spp. Our results provide direct evidence of microbial activity at the interface between scCO2 and an aqueous phase. Since microbial activity can influence the key mechanisms for permanent storage of sequestered CO2 (i.e., structural, residual, solubility, and mineral trapping), our work suggests that during GCS microorganisms may grow and catalyze biological reactions that influence the fate and transport of CO2 in the deep subsurface. PMID:25681188

  9. Microbial growth under supercritical CO2.

    PubMed

    Peet, Kyle C; Freedman, Adam J E; Hernandez, Hector H; Britto, Vanya; Boreham, Chris; Ajo-Franklin, Jonathan B; Thompson, Janelle R

    2015-04-01

    Growth of microorganisms in environments containing CO2 above its critical point is unexpected due to a combination of deleterious effects, including cytoplasmic acidification and membrane destabilization. Thus, supercritical CO2 (scCO2) is generally regarded as a sterilizing agent. We report isolation of bacteria from three sites targeted for geologic carbon dioxide sequestration (GCS) that are capable of growth in pressurized bioreactors containing scCO2. Analysis of 16S rRNA genes from scCO2 enrichment cultures revealed microbial assemblages of varied complexity, including representatives of the genus Bacillus. Propagation of enrichment cultures under scCO2 headspace led to isolation of six strains corresponding to Bacillus cereus, Bacillus subterraneus, Bacillus amyloliquefaciens, Bacillus safensis, and Bacillus megaterium. Isolates are spore-forming, facultative anaerobes and capable of germination and growth under an scCO2 headspace. In addition to these isolates, several Bacillus type strains grew under scCO2, suggesting that this may be a shared feature of spore-forming Bacillus spp. Our results provide direct evidence of microbial activity at the interface between scCO2 and an aqueous phase. Since microbial activity can influence the key mechanisms for permanent storage of sequestered CO2 (i.e., structural, residual, solubility, and mineral trapping), our work suggests that during GCS microorganisms may grow and catalyze biological reactions that influence the fate and transport of CO2 in the deep subsurface.

  10. Amine scrubbing for CO2 capture.

    PubMed

    Rochelle, Gary T

    2009-09-25

    Amine scrubbing has been used to separate carbon dioxide (CO2) from natural gas and hydrogen since 1930. It is a robust technology and is ready to be tested and used on a larger scale for CO2 capture from coal-fired power plants. The minimum work requirement to separate CO2 from coal-fired flue gas and compress CO2 to 150 bar is 0.11 megawatt-hours per metric ton of CO2. Process and solvent improvements should reduce the energy consumption to 0.2 megawatt-hour per ton of CO2. Other advanced technologies will not provide energy-efficient or timely solutions to CO2 emission from conventional coal-fired power plants.

  11. CO2 Sparging Phase 3 Full Scale Implementation and Monitoring Report

    EPA Pesticide Factsheets

    In-situ carbon dioxide (CO2) sparging was designed and implemented to treat a subsurface causticbrine pool (CBP) formed as a result of releases from historical production of industrial chemicals at theLCP Chemicals Site, Brunswick, GA (Site).

  12. Simulation of CO 2 concentrations at Tsukuba tall tower using WRF-CO 2 tracer transport model

    NASA Astrophysics Data System (ADS)

    Ballav, Srabanti; Patra, Prabir K.; Sawa, Yousuke; Matsueda, Hidekazu; Adachi, Ahoro; Onogi, Shigeru; Takigawa, Masayuki; de, Utpal K.

    2016-02-01

    Simulation of carbon dioxide (CO2) at hourly/weekly intervals and fine vertical resolution at the continental or coastal sites is challenging because of coarse horizontal resolution of global transport models. Here the regional Weather Research and Forecasting (WRF) model coupled with atmospheric chemistry is adopted for simulating atmospheric CO2 (hereinafter WRF-CO2) in nonreactive chemical tracer mode. Model results at horizontal resolution of 27 × 27 km and 31 vertical levels are compared with hourly CO2 measurements from Tsukuba, Japan (36.05°N, 140.13 oE) at tower heights of 25 and 200 m for the entire year 2002. Using the wind rose analysis, we find that the fossil fuel emission signal from the megacity Tokyo dominates the diurnal, synoptic and seasonal variations observed at Tsukuba. Contribution of terrestrial biosphere fluxes is of secondary importance for CO2 concentration variability. The phase of synoptic scale variability in CO2 at both heights are remarkably well simulated the observed data (correlation coefficient >0.70) for the entire year. The simulations of monthly mean diurnal cycles are in better agreement with the measurements at lower height compared to that at the upper height. The modelled vertical CO2 gradients are generally greater than the observed vertical gradient. Sensitivity studies show that the simulation of observed vertical gradient can be improved by increasing the number of vertical levels from 31 in the model WRF to 37 (4 below 200 m) and using the Mellor-Yamada-Janjic planetary boundary scheme. These results have large implications for improving transport model simulation of CO2 over the continental sites.

  13. Fourier Transform Microwave Spectra of CO{2}-ETHYLENE Sulfide, CO{2}-ETHYLENE Oxide and CO{2}-PROPYLENE Oxide Complexes

    NASA Astrophysics Data System (ADS)

    Orita, Yukari; Kawashima, Yoshiyuki; Hirota, Eizi

    2010-06-01

    We have previously examined the difference in roles of O and S in structure and dynamics of the CO-ethylene oxide (EO) and CO-ethylene sulfide (ES) complexes. We have extended the investigation to CO{2}-EO and CO{2}-ES for comparison. We have also observed the CO{2}-propylene oxide (PO) complex, which is an important intermediate in the reaction of PO with CO{2} leading to polycarbonate. Both a-type and b-type transitions were observed for the CO{2}-EO and CO{2}-ES, but no c-type transitions were observed at all. We also detected the {34}S and {13}C isotopic species in natural abundance and the species containing {18}OCO and C{18}O% {2}, which were synthesized by burning paper in an {18}O{2} and{% 16}O{2} mixture. By analyzing the observed spectra we concluded the CO{2} moiety of CO{2}-EO and CO{2}-ES located in a plane % prependicular to the three-membered ring and bisecting the COC or CSC angle of EO or ES, respectively, as in the case of CO-EO and CO-ES complexes. An % ab initio MO calculation at the level of MP2/6-311G(d, p) yielded an optimized structure in good agreement with the experimental result. We have derived from the observed spectra the distance, the stretching force constant, and the binding energy of the bonds between the constituents of the CO{2}-EO and CO{2}-ES complexes and have found that the distances of the two complexes were shorter by 0.2Å than those in CO-EO and CO-ES, respectively, and that the intermolecular bonds were two times stronger in the CO{2} complexes than in the corresponding CO complexes. We have concluded from the observed spectra that the CO{2} moiety in CO{2}-PO is located on the PO three-membered ring plane opposite to the methyl group. The constituents in CO{2}-PO were more weakly bound than those in CO{2}-EO and CO{2}-ES. S. Sato, Y. Kawashima, Y. Tatamitani, and E. Hirota, 63rd International Symposium on Molecular Spectroscopy, WF05 (2008).

  14. Earth's Atmospheric CO2 Saturated IR Absorption

    NASA Astrophysics Data System (ADS)

    Wall, Ernst

    2008-10-01

    Using the on-line SpectraCalc IR absorption simulator, the amount of IR absorption by the 15 μ line of the current atmospheric CO2 was obtained and compared with that of twice the amount of CO2. The simulation required a fixed density equivalent for the atmospheric path length. This was obtained by numerically integrating the NOAA Standard Atmospheric model. While the current line is saturated, doubling the CO2 will cause a slight width increase. Using this and the blackbody radiation curve plus considering the effects of water vapor, the temperature rise of the Earth will be less than 2.5 deg. C. Integrating a NASA Martian atmospheric model, we find that the Martian atmosphere has 45 times more CO2 to penetrate than Earth, and yet, the Martian diurnal temperature swings exceed those of the Sahara desert. I.e., large amounts of CO2 alone do not necessarily cause planetary warming. As the oceans warm from any cause, more CO2 is boiled out, but if they cool, they will absorb more CO2 just as a carbonated drink does, so that temperature and CO2 density will correlate. It is to be noted that the Earth's known petroleum reserves contain only enough CO2 to increase the atmospheric CO2 by some 15%.

  15. CO2 transport over complex terrain

    USGS Publications Warehouse

    Sun, Jielun; Burns, Sean P.; Delany, A.C.; Oncley, S.P.; Turnipseed, A.A.; Stephens, B.B.; Lenschow, D.H.; LeMone, M.A.; Monson, Russell K.; Anderson, D.E.

    2007-01-01

    CO2 transport processes relevant for estimating net ecosystem exchange (NEE) at the Niwot Ridge AmeriFlux site in the front range of the Rocky Mountains, Colorado, USA, were investigated during a pilot experiment. We found that cold, moist, and CO2-rich air was transported downslope at night and upslope in the early morning at this forest site situated on a ???5% east-facing slope. We found that CO2 advection dominated the total CO2 transport in the NEE estimate at night although there are large uncertainties because of partial cancellation of horizontal and vertical advection. The horizontal CO2 advection captured not only the CO2 loss at night, but also the CO2 uptake during daytime. We found that horizontal CO2 advection was significant even during daytime especially when turbulent mixing was not significant, such as in early morning and evening transition periods and within the canopy. Similar processes can occur anywhere regardless of whether flow is generated by orography, synoptic pressure gradients, or surface heterogeneity as long as CO2 concentration is not well mixed by turbulence. The long-term net effect of all the CO2 budget terms on estimates of NEE needs to be investigated. ?? 2007 Elsevier B.V. All rights reserved.

  16. Covalent Organic Frameworks for CO2 Capture.

    PubMed

    Zeng, Yongfei; Zou, Ruqiang; Zhao, Yanli

    2016-04-20

    As an emerging class of porous crystalline materials, covalent organic frameworks (COFs) are excellent candidates for various applications. In particular, they can serve as ideal platforms for capturing CO2 to mitigate the dilemma caused by the greenhouse effect. Recent research achievements using COFs for CO2 capture are highlighted. A background overview is provided, consisting of a brief statement on the current CO2 issue, a summary of representative materials utilized for CO2 capture, and an introduction to COFs. Research progresses on: i) experimental CO2 capture using different COFs synthesized based on different covalent bond formations, and ii) computational simulation results of such porous materials on CO2 capture are summarized. Based on these experimental and theoretical studies, careful analyses and discussions in terms of the COF stability, low- and high-pressure CO2 uptake, CO2 selectivity, breakthrough performance, and CO2 capture conditions are provided. Finally, a perspective and conclusion section of COFs for CO2 capture is presented. Recent advancements in the field are highlighted and the strategies and principals involved are discussed.

  17. Energyless CO2 Absorption, Generation, and Fixation Using Atmospheric CO2.

    PubMed

    Inagaki, Fuyuhiko; Okada, Yasuhiko; Matsumoto, Chiaki; Yamada, Masayuki; Nakazawa, Kenta; Mukai, Chisato

    2016-01-01

    From an economic and ecological perspective, the efficient utilization of atmospheric CO2 as a carbon resource should be a much more important goal than reducing CO2 emissions. However, no strategy to harvest CO2 using atmospheric CO2 at room temperature currently exists, which is presumably due to the extremely low concentration of CO2 in ambient air (approximately 400 ppm=0.04 vol%). We discovered that monoethanolamine (MEA) and its derivatives efficiently absorbed atmospheric CO2 without requiring an energy source. We also found that the absorbed CO2 could be easily liberated with acid. Furthermore, a novel CO2 generator enabled us to synthesize a high value-added material (i.e., 2-oxazolidinone derivatives based on the metal catalyzed CO2-fixation at room temperature) from atmospheric CO2.

  18. Exogenously produced CO2 doubles the CO2 efflux from three north temperate lakes

    NASA Astrophysics Data System (ADS)

    Wilkinson, Grace M.; Buelo, Cal D.; Cole, Jonathan J.; Pace, Michael L.

    2016-03-01

    It is well established that lakes are typically sources of CO2 to the atmosphere. However, it remains unclear what portion of CO2 efflux is from endogenously processed organic carbon or from exogenously produced CO2 transported into lakes. We estimated high-frequency CO2 and O2 efflux from three north temperate lakes in summer to determine the proportion of the total CO2 efflux that was exogenously produced. Two of the lakes were amended with nutrients to experimentally enhance endogenous CO2 uptake. In the unfertilized lake, 50% of CO2 efflux was from exogenous sources and hydrology had a large influence on efflux. In the fertilized lakes, endogenous CO2 efflux was negative (into the lake) yet exogenous CO2 made the lakes net sources of CO2 to the atmosphere. Shifts in hydrologic regimes and nutrient loading have the potential to change whether small lakes act primarily as reactors or vents in the watershed.

  19. Lidar measurements of the column CO2 mixing ratio made by NASA Goddard's CO2 Sounder during the NASA ASCENDS 2014 Airborne campaign.

    NASA Astrophysics Data System (ADS)

    Ramanathan, A. K.; Mao, J.; Abshire, J. B.; Kawa, S. R.

    2015-12-01

    Remote sensing measurements of CO2 from space can help improve our understanding of the carbon cycle and help constrain the global carbon budget. However, such measurements need to be sufficiently accurate to detect small (1 ppm) changes in the CO2 mixing ratio (XCO2) against a large background (~ 400 ppm). Satellite measurements of XCO2 using passive spectrometers, such as those from the Japanese GOSAT (Greenhouse gas Observing Satellite) and the NASA OCO-2 (Orbiting Carbon Observatory-2) are limited to daytime sunlit portions of the Earth and are susceptible to biases from clouds and aerosols. For this reason, NASA commissioned the formulation study of ASCENDS a space-based lidar mission. NASA Goddard Space Flight Center's CO2 Sounder lidar is one candidate approach for the ASCENDS mission. The NASA GSFC CO2 Sounder measures the CO2 mixing ratio using a pulsed multi-wavelength integrated path differential absorption (IPDA) approach. The CO2 Sounder has flown in the 2011, 2013 and 2014 ASCENDS airborne campaigns over the continental US, and has produced measurements in close agreement with in situ measurements of the CO2 column. In 2014, the CO2 Sounder upgraded its laser with a precision step-locked diode laser source to improve the lidar wavelength position accuracy. It also improved its optical receiver with a low-noise, high efficiency, HgCdTe avalanche photo diode detector. The combination of these two technologies enabled lidar XCO2 measurements with unprecedented accuracy. In this presentation, we show analysis from the ASCENDS 2014 field campaign, exploring: (1) Horizontal XCO2 gradients measured by the lidar, (2) Comparisons of lidar XCO2 measurements against the Parameterized Chemistry Transport Model (PCTM), and (3) Lidar column water vapor measurements using a HDO absorption line that occurs next to the CO2 absorption line. This can reduce the uncertainty in the dry air column used in XCO2 retrievals.

  20. Chances and challenges of forest scale CO2 enrichment

    NASA Astrophysics Data System (ADS)

    Körner, Christian

    2016-04-01

    Rising CO2 is changing the biosphere's diet. As with any dietary change, both amount and quality of food matter. Atmospheric CO2 enrichment is clearly providing a rather one-sided, C-rich diet. Hence, the reaiistic experimental simulation of its effect on the single biggest C reservoir of the biosphere, that is forest, requires experimental conditions that resemble exactly that situation. In the past, trees where most commonly exposed to elevated CO2 while provided with ample other constituents of a plant's diet (soil nutrients), yielding exaggerated growth stimulation, unlikely to reflect real world responses. So, by either selecting fertile soils, disturbing the system by fire or planting activities, offering ample soil space to isolated individuals or even adding fertilizer, almost any CO2-response can be 'designed'. The 'art' of designing future Free Air CO2 Enrichment (FACE) experiments will be to avoid exactly these pitfalls. Plants can incorporate additional C only to the extent the provision of chemical elements other than C will permit, given the stoichiometry of life. Site selection (soil fertility), degree of canopy closure, recent disturbance regime or successional stage will influence CO2 effects. It is the fundamental dilemma in CO2-enrichment research that simple, homogenous, artificial test systems offer statistical power, while systems that account for 'naturalness' and species diversity do not. Any new FACE program needs to handle that tradeoff between precision and relevance. In this presentation I will advocate a pragmatic approach that will inevitably have to lean on individual tree responses, across a wide as possible range of neighborhoods, age and growth conditions, with the statistical power depending in obtaining the best possible pre-treatment traits and responses. By illustrating the results of 15 years of FACE with 30-40 m tall forest trees, I will caution against over-optimistic ecosystem scale approaches with just ONE technology

  1. Electric field effects in electrochemical CO2 reduction

    DOE PAGES

    Chen, Leanne D.; Urushihara, Makoto; Chan, Karen; ...

    2016-09-22

    Electrochemical reduction of CO2 has the potential to reduce greenhouse gas emissions while providing energy storage and producing chemical feedstocks. A mechanistic understanding of the process is crucial to the discovery of efficient catalysts, and an atomistic description of the electrochemical interface is a major challenge due to its complexity. Here, we examine the CO2 → CO electrocatalytic pathway on Ag(111) using density functional theory (DFT) calculations and an explicit model of the electrochemical interface. We show that the electric field from solvated cations in the double layer and their corresponding image charges on the metal surface significantly stabilizes keymore » intermediates—*CO2 and *COOH. At the field-stabilized sites, the formation of *CO is rate-determining. We present a microkinetic model that incorporates field effects and electrochemical barriers from ab initio calculations. As a result, the computed polarization curves show reasonable agreement with experiment without fitting any parameters.« less

  2. CO2 sequestration: Storage capacity guideline needed

    USGS Publications Warehouse

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

    2006-01-01

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

  3. R&D100: CO2 Memzyme

    SciTech Connect

    Rempe, Susan; Brinker, Jeff; Jiang, Ying-Bing; Vanegas, Juan

    2015-11-19

    By combining a water droplet loaded with CO2 enzymes in an ultrathin nanopore on a flexible substrate, researchers at Sandia National Laboratories realized the first technology that meets and exceeds DOE targets for cost-effective CO2 capture. When compared with the nearest membrane competitor, this technology delivers a three times permeation rate, twenty times higher selectivity, and ten time lower fabrication cost. The CO2 Memzyme has the potential to remove 90% of CO2 emissions and is forecasted to save the U.S. coal industry $90 billion a year compared to conventional technology.

  4. R&D100: CO2 Memzyme

    ScienceCinema

    Rempe, Susan; Brinker, Jeff; Jiang, Ying-Bing; Vanegas, Juan

    2016-07-12

    By combining a water droplet loaded with CO2 enzymes in an ultrathin nanopore on a flexible substrate, researchers at Sandia National Laboratories realized the first technology that meets and exceeds DOE targets for cost-effective CO2 capture. When compared with the nearest membrane competitor, this technology delivers a three times permeation rate, twenty times higher selectivity, and ten time lower fabrication cost. The CO2 Memzyme has the potential to remove 90% of CO2 emissions and is forecasted to save the U.S. coal industry $90 billion a year compared to conventional technology.

  5. CO2 MITIGATION VIA ACCELERATED LIMESTONE WEATHERING

    SciTech Connect

    Rau, G H; Knauss, K G; Langer, W H; Caldeira, K G

    2004-02-27

    The climate and environmental impacts of our current, carbon-intensive energy usage demands that effective and practical energy alternatives and CO2 mitigation strategies be found. As part of this effort, various means of capturing and storing CO2 generated from fossil-fuel-based energy production are being investigated. One of the proposed methods involves a geochemistry-based capture and sequestration process that hydrates point-source, waste CO2 with water to produce a carbonic acid solution. This in turn is reacted and neutralized with limestone, thus converting the original CO2 gas to calcium bicarbonate in solution, the overall reaction being:

  6. Binding energies of CO2 with some ionic liquids

    NASA Astrophysics Data System (ADS)

    Eucker, William; Bendler, John

    2007-03-01

    Room temperature ionic liquids (RTILs), a novel class of materials with negligible vapor pressures and potentiality as benign solvents, may be an ideal chemical for carbon dioxide (CO2) gas sequestration. Ab initio computational modeling was used to investigate the molecular interactions of simple RTIL anions hexafluorophosphate (PF6^-) and tetrafluoroborate (BF4^-) with CO2. Electronic potential energy surface (PES) scans of a comprehensive sampling of 1:1 anion-CO2 orientations were computed using Spartan '02 with Dunning's correlation consistent basis sets. Qualitatively, the PES scans yielded deeper, more numerous and radially closer active sites surrounding BF4^- anion as compared with the PF6^- anion. Quantitatively, the binding energies of 17.87 kJ/mol and 25.24 kJ/mol were extracted from the identified global energy minima for the PF6^- and BF4^- systems, respectively. The smaller BF4^- anion was concluded to bind more strongly to the CO2. However, literature-reported experimental Henry's law constants for CO2 dissolved in imidizolium based RTILs show greater gas solvation in the PF6^- system. The discrepancy between the energetics calculation results and the experimental solvation data will be discussed.

  7. Role of CO2 in the formation of gold deposits.

    PubMed

    Phillips, G N; Evans, K A

    2004-06-24

    Much of global gold production has come from deposits with uneconomic concentrations of base metals, such as copper, lead and zinc. These 'gold-only' deposits are thought to have formed from hot, aqueous fluids rich in carbon dioxide, but only minor significance has been attached to the role of the CO2 in the process of gold transport. This is because chemical bonding between gold ions and CO2 species is not strong, and so it is unlikely that CO2 has a direct role in gold transport. An alternative indirect role for CO2 as a weak acid that buffers pH has also appeared unlikely, because previously inferred pH values for such gold-bearing fluids are variable. Here we show that such calculated pH values are unlikely to record conditions of gold transport, and propose that CO2 may play a critical role during gold transport by buffering the fluid in a pH range where elevated gold concentration can be maintained by complexation with reduced sulphur. Our conclusions, which are supported by geochemical modelling, may provide a platform for new gold exploration methods.

  8. A novel CO 2 gas analyzer based on IR absorption

    NASA Astrophysics Data System (ADS)

    Zhang, Guangjun; Wu, Xiaoli

    2004-08-01

    Carbon dioxide (CO 2) gas analyzer can be widely used in many fields. A novel CO 2 gas analyzer based on infrared ray (IR) absorption is presented sufficiently in this paper. Applying Lambert-Beer Law, a novel space-double-beam optical structure is established successfully. The optical structure includes an IR source, a gas cell, a bandpass filter with a transmission wavelength at 4.26 μm, another bandpass filter with a transmission wavelength at 3.9 μm, and two IR detectors. Based on Redial Basic Function (RBF) artificial neural network, the measuring model of IR CO 2 analyzer is established with a high accuracy. A dynamic compensation filter is effectively designed to improve the dynamic characteristic of the IR CO 2 analyzer without gas pump. The IR CO 2 analyzer possesses the advantages of high accuracy and mechanical reliability with small volume, lightweight, and low-power consumption. Therefore, it can be used in such relevant fields as environmental protection, processing control, chemical analysis, medical diagnosis, and space environmental and control systems.

  9. Mechanism of acid reduction at low and high overpotential metal electrodes in the presence and absence of CO2: Implications for CO2 reduction by N-heterocycles

    NASA Astrophysics Data System (ADS)

    Zeitler, Elizabeth L.

    Carbon dioxide reduction is of public interest to synthesize useful materials from CO2 and for storage of renewable energy in a carbon-constrained world. Scientifically, CO2 reduction is of fundamental interest to understand the activation of small molecules and stable chemical bonds. Pyridinium catalysts have been observed to lower the overpotential for reduction of CO2 to methanol at platinum and p-GaP electrodes. In this study, the reduction of pyridinium at a variety of metal electrode surfaces was explored along with its interaction with CO2. The reduction of any weak acid analyte on platinum was found to proceed via a one-electron, proton-coupled process forming H2. The reduction potential could be predicted entirely by acid pKa. Equilibrium and kinetic isotope effects supported this assignment. A prepeak feature observed for acid reductions was examined. Reduction forming a pi-radical was observed for 4,4'-bipyridinium at platinum, gold and glassy carbon via spectroelectrochemistry. Only a small increase in radical decay was observed in the presence of CO 2. Pyridinium reduction at gold was found to occur via proton reduction. Protonated and unprotonated N-heterocycle reductions on glassy carbon can best be explained via pi-reduction. The interaction of CO2 with pyridine was examined. Current in the presence of CO2 was enhanced at slow scan rates due to the slow hydration of CO2 into carbonic acid, leading to pyridinium protonation and is not diagnostic of CO2 reduction. A variety of weak acid analytes showed current enhancement, with greater pKa values leading to greater enhancement. Solution buffering at the electrode interface by CO2 was examined. Current enhancement of pyridinium under CO2 was greater than the sum of the currents for background CO2 reduction and pyridinium reduction, indicating pyridine enhanced CO2 hydration.

  10. Performance of photoperiod and light intensity on biogas upgrade and biogas effluent nutrient reduction by the microalgae Chlorella sp.

    PubMed

    Yan, Cheng; Zheng, Zheng

    2013-07-01

    Biogas is an environment-friendly fuel but that must be upgraded before being utilized. The method about removing CO2 from biogas by microalgal culturing using biogas effluent as nutrient medium in this study could effectively upgrade biogas and simultaneously reduce the biogas effluent nutrient. Results showed that the optimum parameters for microalgal growth and biogas effluent nutrient reduction was moderate light intensity with middle photoperiod. While low light intensity with long photoperiod and moderate light intensity with middle photoperiod obtained the best biogas CO2 removal and biogas upgrade effects. Therefore, the optimal parameters were moderate light intensity 350 μmol m(-2)s(-1) with middle photoperiod 14 h light:10h dark. Under this condition, the microalgal dry weight, CH4 concentration, reduction efficiency of chemical oxygen demand, total nitrogen, and total phosphorus was 615.84 ± 33.07 mg L(-1), 92.16 ± 2.83% (v/v), 88.74 ± 3.45%, 83.94 ± 3.51%, and 80.43 ± 4.17%, respectively.

  11. CO2 Interaction with Geomaterials (Invited)

    NASA Astrophysics Data System (ADS)

    Romanov, V.; Howard, B. H.; Lynn, R. J.; Warzinski, R. P.; Hur, T.; Myshakin, E. M.; Lopano, C. L.; Voora, V. K.; Al-Saidi, W. A.; Jordan, K. D.; Cygan, R. T.; Guthrie, G. D.

    2010-12-01

    This work compares the sorption and swelling processes associated with CO2-coal and CO2-clay interactions. We investigated the mechanisms of interaction related to CO2 adsortion in micropores, intercalation into sub-micropores, dissolution in solid matrix, the role of water, and the associated changes in reservoir permeability, for applications in CO2 sequestration and enhanced coal bed methane recovery. The structural changes caused by CO2 have been investigated. A high-pressure micro-dilatometer was equipped to investigate the effect of CO2 pressure on the thermoplastic properties of coal. Using an identical dilatometer, Rashid Khan (1985) performed experiments with CO2 that revealed a dramatic reduction in the softening temperature of coal when exposed to high-pressure CO2. A set of experiments was designed for -20+45-mesh samples of Argonne Premium Pocahontas #3 coal, which is similar in proximate and ultimate analysis to the Lower Kittanning seam coal that Khan used in his experiments. No dramatic decrease in coal softening temperature has been observed in high-pressure CO2 that would corroborate the prior work of Khan. Thus, conventional polymer (or “geopolymer”) theories may not be directly applicable to CO2 interaction with coals. Clays are similar to coals in that they represent abundant geomaterials with well-developed microporous structure. We evaluated the CO2 sequestration potential of clays relative to coals and investigated the factors that affect the sorption capacity, rates, and permanence of CO2 trapping. For the geomaterials comparison studies, we used source clay samples from The Clay Minerals Society. Preliminary results showed that expandable clays have CO2 sorption capacities comparable to those of coal. We analyzed sorption isotherms, XRD, DRIFTS (infrared reflectance spectra at non-ambient conditions), and TGA-MS (thermal gravimetric analysis) data to compare the effects of various factors on CO2 trapping. In montmorillonite, CO2

  12. Detection of CO2 leaks from carbon capture and storage sites to the atmosphere with combined CO2 and O2 measurements

    NASA Astrophysics Data System (ADS)

    van Leeuwen, Charlotte; Meijer, Harro A. J.

    2015-04-01

    One of the main issues in carbon capture and storage (CCS) is the possibility of leakage of CO2 from the storage reservoir to the atmosphere, both from a public health and a climate change combat perspective. Detecting these leaks in the atmosphere is difficult due to the rapid mixing of the emitted CO2 with the surrounding air masses and the high natural variability of the atmospheric CO2 concentration. Instead of measuring only the CO2 concentration of the atmosphere, its isotopes or chemical tracers that are released together with the CO2, our method uses O2 measurements in addition to CO2 measurements to detect a leak from a CCS site. CO2 and O2 are coupled in most processes on earth. In photosynthesis, plants take up CO2 and release O2 at the same time. In respiration and fossil fuel burning, O2 is consumed while CO2 is released. In case of a leak from a CCS site, however, there is no relationship between CO2 and O2. A CO2 leak can therefore be distinguished from other sources of CO2 by looking at the atmospheric CO2-O2 ratio. A natural increase of the CO2 concentration is accompanied by a drop in the O2 concentration, while an increase in the CO2 concentration caused by a leak from a CCS site does not have any effect on the O2 concentration. To demonstrate this leak detection strategy we designed and built a transportable CO2 and O2 measurement system, that is capable of measuring the relatively minute (ppm's variations on a 21% concentration) changes in the O2 concentration. The system comprises of three cases that contain the instrumentation and gas handling equipment, the gas cylinders used as reference and calibration gases and a drying system, respectively. Air is pumped to the system from an air inlet that is placed in a small tower in the field. At the conference, we will demonstrate the success of leak detection with our system by showing measurements of several CO2 release experiments, where CO2 was released at a small distance from the air inlet of

  13. Characterization of CO2 leakage into the freshwater body

    NASA Astrophysics Data System (ADS)

    Singh, Ashok; Delfs, Jens-Olaf; Shao, Habing; Kolditz, Olaf

    2013-04-01

    Current research into Carbon dioxide Capture and Storage (CCS) is dominated by improving the CO2 storage capacity. However, potential leakage of CO2 can cause environmental problems, particularly if freshwater resources are nearby. In this regards, it is important to understand the chemistry of CO2 and the water system. CO2 leakage across the fluid interface (CO2 and water) is controlled by the difference in the partial pressure of CO2 in the storage and in the freshwater body. Once the CO2 is in solution, it equilibrates with the bicarbonate and carbonate ions. According to Millero (1994)such a system can be characterized by two parameters out of the four: total alkalinity (TA), total carbonate (TCO2), fugacity of CO2(fCO2) and pH. In the present modeling study, we are interested in the (i) CO2 leakage into a freshwater body (while injecting CO2 for storage) through an inclined fracture and (ii) characterization of the system by measuring fugacity of CO2 and pH. According to work presented by Singh et al. (2012), about 31% of injected CO2 leaks into the freshwater body. Solubility of CO2 in water follows Henry's law, while the Henry constant, K0 is calculated by an empirical relation developed by Murray and Riley (1971), which is a function of salinity and temperature. According to our results, pH and fugacity both appear to be a linear function of temperature. To simulate the discussed problem, a corresponding numerical module has been developed for multi-component fluid flow coupled with heat and mass transport processes. Governing equations and Volume Translated Peng-Robinson equations of state are implemented within the object-oriented finite element code OpenGeoSys (Kolditz et al., 2012; www.opengeosys.org). Primary variables are pressure, temperature and salinity which are obtained by solving the governing equations in a monolithic way The governing equations are discretized spatially within the context of a Galerkin approach, whereas the temporal

  14. Choosing amine-based absorbents for CO2 capture.

    PubMed

    Gomes, João; Santos, Samuel; Bordado, João

    2015-01-01

    CO2 capture from gaseous effluents is one of the great challenges faced by chemical and environmental engineers, as the increase in CO2 levels in the Earth atmosphere might be responsible for dramatic climate changes. From the existing capture technologies, the only proven and mature technology is chemical absorption using aqueous amine solutions. However, bearing in mind that this process is somewhat expensive, it is important to choose the most efficient and, at the same time, the least expensive solvents. For this purpose, a pilot test facility was assembled and includes an absorption column, as well as a stripping column, a heat exchanger between the two columns, a reboiler for the stripping column, pumping systems, surge tanks and all necessary instrumentation and control systems. Some different aquous amine solutions were tested on this facility and it was found that, from a set of six tested amines, diethanol amine is the one that turned out to be the most economical choice, as it showed a higher CO2 loading capacity (0.982 mol of CO2 per mol of amine) and the lowest price per litre (25.70 €/L), even when compared with monoethanolamine, the benchmark solvent, exhibiting a price per litre of 30.50 €/L.

  15. Rate of CO2 attack on hydrated Class H well cement under geologic sequestration conditions.

    PubMed

    Kutchko, Barbara G; Strazisar, Brian R; Lowry, Gregory V; Dzombak, David A; Thaulow, Niels

    2008-08-15

    Experiments were conducted to study the degradation of hardened cement paste due to exposure to CO2 and brine under geologic sequestration conditions (T = 50 degrees C and 30.3 MPa). The goal was to determine the rate of reaction of hydrated cement exposed to supercritical CO2 and to CO2-saturated brine to assess the potential impact of degradation in existing wells on CO2 storage integrity. Two different forms of chemical alteration were observed. The supercritical CO2 alteration of cement was similar in process to cement in contact with atmospheric CO2 (ordinary carbonation), while alteration of cement exposed to CO2-saturated brine was typical of acid attack on cement. Extrapolation of the hydrated cement alteration rate measured for 1 year indicates a penetration depth range of 1.00 +/- 0.07 mm for the CO2-saturated brine and 1.68 +/- 0.24 mm for the supercritical CO2 after 30 years. These penetration depths are consistent with observations of field samples from an enhanced oil recovery site after 30 years of exposure to CO2-saturated brine under similar temperature and pressure conditions. These results suggest that significant degradation due to matrix diffusion of CO2 in intact Class H neat hydrated cement is unlikely on time scales of decades.

  16. Capturing CO2 via reactions in nanopores.

    SciTech Connect

    Leung, Kevin; Nenoff, Tina Maria; Criscenti, Louise Jacqueline; Tang, Z; Dong, J. H.

    2008-10-01

    This one-year exploratory LDRD aims to provide fundamental understanding of the mechanism of CO2 scrubbing platforms that will reduce green house gas emission and mitigate the effect of climate change. The project builds on the team members expertise developed in previous LDRD projects to study the capture or preferential retention of CO2 in nanoporous membranes and on metal oxide surfaces. We apply Density Functional Theory and ab initio molecular dynamics techniques to model the binding of CO2 on MgO and CaO (100) surfaces and inside water-filled, amine group functionalized silica nanopores. The results elucidate the mechanisms of CO2 trapping and clarify some confusion in the literature. Our work identifies key future calculations that will have the greatest impact on CO2 capture technologies, and provides guidance to science-based design of platforms that can separate the green house gas CO2 from power plant exhaust or even from the atmosphere. Experimentally, we modify commercial MFI zeolite membranes and find that they preferentially transmit H2 over CO2 by a factor of 34. Since zeolite has potential catalytic capability to crack hydrocarbons into CO2 and H2, this finding paves the way for zeolite membranes that can convert biofuel into H2 and separate the products all in one step.

  17. CO2 Capture with Enzyme Synthetic Analogue

    SciTech Connect

    Cordatos, Harry

    2010-03-01

    Project overview provides background on carbonic anhydrase transport mechanism for CO2 in the human body and proposed approach for ARPA-E project to create a synthetic enzyme analogue and utilize it in a membrane for CO2 capture from flue gas.

  18. CO2 Capture with Enzyme Synthetic Analogue

    SciTech Connect

    Cordatos, Harry

    2010-11-08

    Overview of an ongoing, 2 year research project partially funded by APRA-E to create a novel, synthetic analogue of carbonic anhydrase and incorporate it into a membrane for removal of CO2 from flue gas in coal power plants. Mechanism background, preliminary feasibility study results, molecular modeling of analogue-CO2 interaction, and program timeline are provided.

  19. Improved Criteria for Increasing CO2 Storage Potential with CO2 Enhanced Oil Recovery

    NASA Astrophysics Data System (ADS)

    Bauman, J.; Pawar, R.

    2013-12-01

    In recent years it has been found that deployment of CO2 capture and storage technology at large scales will be difficult without significant incentives. One of the technologies that has been a focus in recent years is CO2 enhanced oil/gas recovery, where additional hydrocarbon recovery provides an economic incentive for deployment. The way CO2 EOR is currently deployed, maximization of additional oil production does not necessarily lead to maximization of stored CO2, though significant amounts of CO2 are stored regardless of the objective. To determine the potential of large-scale CO2 storage through CO2 EOR, it is necessary to determine the feasibility of deploying this technology over a wide range of oil/gas field characteristics. In addition it is also necessary to accurately estimate the ultimate CO2 storage potential and develop approaches that optimize oil recovery along with long-term CO2 storage. This study uses compositional reservoir simulations to further develop technical screening criteria that not only improve oil recovery, but maximize CO2 storage during enhanced oil recovery operations. Minimum miscibility pressure, maximum oil/ CO2 contact without the need of significant waterflooding, and CO2 breakthrough prevention are a few key parameters specific to the technical aspects of CO2 enhanced oil recovery that maximize CO2 storage. We have developed reduced order models based on simulation results to determine the ultimate oil recovery and CO2 storage potential in these formations. Our goal is to develop and demonstrate a methodology that can be used to determine feasibility and long-term CO2 storage potential of CO2 EOR technology.

  20. A model for the evolution of CO2 on Mars.

    PubMed

    Haberle, R M; Tyler, D; McKay, C P; Davis, W L

    1994-05-01

    We have constructed a model that predicts the evolution of CO2 on Mars from the end of the heavy bombardment period to the present. The model draws on published estimates of the main processes believed to affect the fate of CO2 during this period: chemical weathering, regolith uptake, polar cap formation, and atmospheric escape. Except for escape, the rate at which these processes act is controlled by surface temperatures which we calculate using a modified version of the Gierasch and Toon energy balance model (1973, J. Atmos. Sci. 30, 1502-1508). The modifications account for the change in solar luminosity with time, the greenhouse effect, and a polar and solar equatorial energy budget. Using published estimates for the main parameters, we find no evolutionary scenario in which CO2 is capable of producing a warm (global mean temperatures>250 K) and wet (surface pressures>30 mbar) early climate, and then evolves to present conditions with approximately 7 mbar in the atmosphere, <300 mbar in the regolith, and <5 mbar in the caps. Such scenarios would only exist if the early sun were brighter than standard solar models suggest, if greenhouse gases other than CO2 were present in the early atmosphere, or if the polar albedo were significantly lower than 0.75. However, these scenarios generally require the storage of large amounts of CO2 (>1 bar) in the carbonate reservoir. If the warm and wet early Mars constraint is relaxed, then we find best overall agreement with present day reservoirs for initial CO2 inventories of 0.5-1.0 bar. We also find that the polar caps can a profound effect on how the system evolves. If the initial amount of CO2 is less than some critical value, then there is not enough heating of the poles to prevent permanent caps from forming. Once formed, these caps control how the system evolves, because they set the surface pressure and, hence, the thermal environment. If the initial amount of CO2 is greater than this critical value, then caps do not

  1. Geophysical monitoring technology for CO2 sequestration

    NASA Astrophysics Data System (ADS)

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

    2016-06-01

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

  2. Zinc depolarized electrochemical CO2 concentration

    NASA Technical Reports Server (NTRS)

    Woods, R. R.; Marshall, R. D.; Schubert, F. H.

    1975-01-01

    Two zinc depolarized electrochemical carbon dioxide concentrator concepts were analytically and experimentally evaluated for portable life support system carbon dioxide (CO2) removal application. The first concept, referred to as the zinc hydrogen generator electrochemical depolarized CO2 concentrator, uses a ZHG to generate hydrogen for direct use in an EDC. The second concept, referred to as the zinc/electrochemical depolarized concentrator, uses a standard EDC cell construction modified for use with the Zn anode. The Zn anode is consumed and subsequently regenerated, thereby eliminating the need to supply H2 to the EDC for the CO2 removal process. The evaluation was based primarily on an analytical evaluation of the two ZnDCs at projected end item performance and hardware design levels. Both ZnDC concepts for PLSS CO2 removal application were found to be noncompetitive in both total equivalent launch weight and individual extravehicular activity mission volume when compared to other candidate regenerable PLSS CO2 scrubbers.

  3. The ins and outs of CO2

    PubMed Central

    Raven, John A.; Beardall, John

    2016-01-01

    It is difficult to distinguish influx and efflux of inorganic C in photosynthesizing tissues; this article examines what is known and where there are gaps in knowledge. Irreversible decarboxylases produce CO2, and CO2 is the substrate/product of enzymes that act as carboxylases and decarboxylases. Some irreversible carboxylases use CO2; others use HCO3 –. The relative role of permeation through the lipid bilayer versus movement through CO2-selective membrane proteins in the downhill, non-energized, movement of CO2 is not clear. Passive permeation explains most CO2 entry, including terrestrial and aquatic organisms with C3 physiology and biochemistry, terrestrial C4 plants and all crassulacean acid metabolism (CAM) plants, as well as being part of some mechanisms of HCO3 – use in CO2 concentrating mechanism (CCM) function, although further work is needed to test the mechanism in some cases. However, there is some evidence of active CO2 influx at the plasmalemma of algae. HCO3 – active influx at the plasmalemma underlies all cyanobacterial and some algal CCMs. HCO3 – can also enter some algal chloroplasts, probably as part of a CCM. The high intracellular CO2 and HCO3 – pools consequent upon CCMs result in leakage involving CO2, and occasionally HCO3 –. Leakage from cyanobacterial and microalgal CCMs involves up to half, but sometimes more, of the gross inorganic C entering in the CCM; leakage from terrestrial C4 plants is lower in most environments. Little is known of leakage from other organisms with CCMs, though given the leakage better-examined organisms, leakage occurs and increases the energetic cost of net carbon assimilation. PMID:26466660

  4. Stomatal proxy record of CO2 concentrations from the last termination suggests an important role for CO2 at climate change transitions

    NASA Astrophysics Data System (ADS)

    Steinthorsdottir, Margret; Wohlfarth, Barbara; Kylander, Malin E.; Blaauw, Maarten; Reimer, Paula J.

    2013-05-01

    A new stomatal proxy-based record of CO2 concentrations ([CO2]), based on Betula nana (dwarf birch) leaves from the Hässeldala Port sedimentary sequence in south-eastern Sweden, is presented. The record is of high chronological resolution and spans most of Greenland Interstadial 1 (GI-1a to 1c, Allerød pollen zone), Greenland Stadial 1 (GS-1, Younger Dryas pollen zone) and the very beginning of the Holocene (Preboreal pollen zone). The record clearly demonstrates that i) [CO2] were significantly higher than usually reported for the Last Termination and ii) the overall pattern of CO2 evolution through the studied time period is fairly dynamic, with significant abrupt fluctuations in [CO2] when the climate moved from interstadial to stadial state and vice versa. A new loss-on-ignition chemical record (used here as a proxy for temperature) lends independent support to the Hässeldala Port [CO2] record. The large-amplitude fluctuations around the climate change transitions may indicate unstable climates and that “tipping-point” situations were involved in Last Termination climate evolution. The scenario presented here is in contrast to [CO2] records reconstructed from air bubbles trapped in ice, which indicate lower concentrations and a gradual, linear increase of [CO2] through time. The prevalent explanation for the main climate forcer during the Last Termination being ocean circulation patterns needs to re-examined, and a larger role for atmospheric [CO2] considered.

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

    USGS Publications Warehouse

    Rosenbauer, R.; Koksalan, T.

    2004-01-01

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

  6. Enhanced algal CO(2) sequestration through calcite deposition by Chlorella sp. and Spirulina platensis in a mini-raceway pond.

    PubMed

    Ramanan, Rishiram; Kannan, Krishnamurthi; Deshkar, Ashok; Yadav, Raju; Chakrabarti, Tapan

    2010-04-01

    Biological CO(2) sequestration using algal reactors is one of the most promising and environmentally benign technologies to sequester CO(2). This research study was taken up to alleviate certain limitations associated with the technology such as low CO(2) sequestration efficiency and low biomass yields. The study demonstrates an increase in CO(2) sequestration efficiency by maneuvering chemically aided biological sequestration of CO(2). Chlorella sp. and Spirulina platensis showed 46% and 39% mean fixation efficiency, respectively, at input CO(2) concentration of 10%. The effect of acetazolamide, a potent carbonic anhydrase inhibitor, on CO(2) sequestration efficiency was studied to demonstrate the role of carbonic anhydrase in calcite deposition. Calcite formed by both species was characterized by scanning electron microscopy coupled electron dispersive spectroscopy and X-ray diffraction. The overall scheme of calcite deposition coupled CO(2) fixation with commercially utilizable biomass as a product seems a viable option in the efforts to sequester increasing CO(2) emissions.

  7. TES/Aura L2 Carbon Dioxide (CO2) Nadir (TL2CO2N)

    Atmospheric Science Data Center

    2017-02-27

    ... TES/Aura L2 Carbon Dioxide (CO2) Nadir (TL2CO2N) Project Title:  TES Discipline:  Tropospheric ... Earth Science Atmosphere Atmospheric Chemistry/Carbon and Hydrocarbon Compounds Order Data:  ...

  8. A usage of CO2 hydrate: convenient method to increase CO2 concentration in culturing algae.

    PubMed

    Nakano, Sho; Chang, Kwang-Hyeon; Shijima, Atsushi; Miyamoto, Hiroyuki; Sato, Yukio; Noto, Yuji; Ha, Jin-Yong; Sakamoto, Masaki

    2014-11-01

    The addition of CO2 to algal culture systems can increase algal biomass effectively. Generally, gas bubbling is used to increase CO2 levels in culture systems; however, it is difficult to quantitatively operate to control the concentration using this method. In this study, we tested the usability of CO2 hydrate for phytoplankton culture. Specifically, green algae Pseudokirchneriella subcapitata were cultured in COMBO medium that contained dissolved CO2 hydrate, after which its effects were evaluated. The experiment was conducted according to a general bioassay procedure (OECD TG201). CO2 promoted algae growth effectively (about 2-fold relative to the control), and the decrease in pH due to dissolution of the CO2 in water recovered soon because of photosynthesis. Since the CO2 hydrate method can control a CO2 concentration easily and quantitatively, it is expected to be useful in future applications.

  9. A simulation study on the abatement of CO2 emissions by de-absorption with monoethanolamine.

    PubMed

    Greer, T; Bedelbayev, A; Igreja, J M; Gomes, J F; Lie, B

    2010-01-01

    Because of the adverse effect of CO2 from fossil fuel combustion on the earth's ecosystems, the most cost-effective method for CO2 capture is an important area of research. The predominant process for CO2 capture currently employed by industry is chemical absorption in amine solutions. A dynamic model for the de-absorption process was developed with monoethanolamine (MEA) solution. Henry's law was used for modelling the vapour phase equilibrium of the CO2, and fugacity ratios calculated by the Peng-Robinson equation of state (EOS) were used for H2O, MEA, N2 and O2. Chemical reactions between CO2 and MEA were included in the model along with the enhancement factor for chemical absorption. Liquid and vapour energy balances were developed to calculate the liquid and vapour temperature, respectively.

  10. Investigation of Wyoming Bentonite Hydration in Dry to Water-Saturated Supercritical CH4 and CH4/CO2 Mixtures: Implications for CO2-Enhanced Gas Production

    NASA Astrophysics Data System (ADS)

    Loring, J.

    2015-12-01

    Injection of CO2 into low permeability shale formations leads to additional gas recovery and reduces the flux of CO2 into the atmosphere, thus combining a strong economic incentive with a permanent storage option for CO2. Reduced formation transmissivity due to clay swelling is a concern in CO2-enhanced gas production. Clay minerals partly determine the physical (i.e. permeability, brittleness) and certain chemical properties (i.e. wetting ability, gas adsorption) of shales, and montmorillonites are of particular interest because they swell by the uptake of species in their interlayer. In this study, the hydration and expansion of Na-, Cs-, and NH4+-saturated montmorillonite (Na-, Cs-, and NH4-SWy-2) in high-pressure (90 bar) and moderate temperature (50 °C) methane, carbon dioxide, and CO2/CH4 mixtures (3 and 25 mole% CO2) were investigated using in situ IR spectroscopic titrations, in situ XRD, in situ MAS-NMR, and ab initio electronic structure calculations. The overarching goal was to better understand the hydration/expansion behavior of Na-SWy-2 in CO2/CH4 fluid mixtures by comparison to Cs-, and NH4+-saturated clays. Specific aims were to (1) determine if CH4 intercalates the clays, (2) probe the effects of increasing dissolved CO2 and H2O concentrations, and (3) understand the role of cation solvation by H2O and/or CO2. In pure CH4, no evidence of CH4 intercalation was detected by IR for any of the clays. Similarly, no measurable changes to the basal spacing were observed by XRD in the presence of pure CH4. However, when dry Cs- and NH4-SWy-2 were exposed to dry fluids containing CO2, IR showed maximum CO2 penetrated the interlayer, XRD indicated the clays expanded, and NMR showed evidence for cation solvation by CO2, in line with theoretical predictions. IR titration of these clays with water showed sorbed H2O concentrations decreased with increasing dissolved CO2, suggesting competition for interlayer residency by CO2 and H2O. For Na-SWy-2, on the other

  11. Ab initio Quantum Chemical Studies of Reactions in Astrophysical Ices. Reactions Involving CH3OH, CO2, CO, HNCO in H2CO/NH3/H2O Ices

    NASA Technical Reports Server (NTRS)

    Woon, David E.

    2006-01-01

    While reactions between closed shell molecules generally involve prohibitive barriers in the gas phase, prior experimental and theoretical studies have demonstrated that some of these reactions are significantly enhanced when confined within an icy grain mantle and can occur efficiently at temperatures below 100 K with no additional energy processing. The archetypal case is the reaction of formaldehyde (H2CO) and ammonia (NH3) to yield hydroxymethylamine (NH2CH2OH). In the present work we have characterized reactions involving methanol (CH3OH), carbon dioxide (CO2), carbon monoxide (CO), and isocyanic acid (HNCO) in search of other favorable cases. Most of the emphasis is on CH3OH, which was investigated in the two-body reaction with one H2CO and the three-body reaction with two H2CO molecules. The addition of a second H2CO to the product of the reaction between CH3OH and H2CO was also considered as an alternative route to longer polyoxymethylene polymers of the -CH2O- form. The reaction between HNCO and NH3 was studied to determine if it can compete against the barrierless charge transfer process that yields OCN(-) and NH4(+). Finally, the H2CO + NH3 reaction was revisited with additional benchmark calculations that confirm that little or no barrier is present when it occurs in ice.

  12. CO2 (dry ice) cleaning system

    NASA Technical Reports Server (NTRS)

    Barnett, Donald M.

    1995-01-01

    Tomco Equipment Company has participated in the dry ice (solid carbon dioxide, CO2) cleaning industry for over ten years as a pioneer in the manufacturer of high density, dry ice cleaning pellet production equipment. For over four years Tomco high density pelletizers have been available to the dry ice cleaning industry. Approximately one year ago Tomco introduced the DI-250, a new dry ice blast unit making Tomco a single source supplier for sublimable media, particle blast, cleaning systems. This new blast unit is an all pneumatic, single discharge hose device. It meters the insertion of 1/8 inch diameter (or smaller), high density, dry ice pellets into a high pressure, propellant gas stream. The dry ice and propellant streams are controlled and mixed from the blast cabinet. From there the mixture is transported to the nozzle where the pellets are accelerated to an appropriate blasting velocity. When directed to impact upon a target area, these dry ice pellets have sufficient energy to effectively remove most surface coatings through dry, abrasive contact. The meta-stable, dry ice pellets used for CO2 cleaning, while labeled 'high density,' are less dense than alternate, abrasive, particle blast media. In addition, after contacting the target surface, they return to their equilibrium condition: a superheated gas state. Most currently used grit blasting media are silicon dioxide based, which possess a sharp tetrahedral molecular structure. Silicon dioxide crystal structures will always produce smaller sharp-edged replicas of the original crystal upon fracture. Larger, softer dry ice pellets do not share the same sharp-edged crystalline structures as their non-sublimable counterparts when broken. In fact, upon contact with the target surface, dry ice pellets will plastically deform and break apart. As such, dry ice cleaning is less harmful to sensitive substrates, workers and the environment than chemical or abrasive cleaning systems. Dry ice cleaning system

  13. CIUDENs Pilot Project for CO2 Biomonitoring Tools (PISCO2)

    NASA Astrophysics Data System (ADS)

    García, D.; Bruno, J.; Credoz, A.; Grandia, F.; Fuentes, J.; Calabuig, E.; Montoto, M.; Ciuden's Co2 Geological Storage Programme

    2011-12-01

    This paper describes CIUDENs Pilot Project for CO2 Biomonitoring Tools (PISCO2) in NW Spain; focusing on the development of biomonitoring of potential CO2 leakages through testing biogeochemical effects of CO2 injection in soils. CIUDEN is a Spanish National foundation created in 2006 dedicated to different projects related to energy and environment. One of the main activities is the construction and operation of various facilities for Research and Development in CCS. The PISCO2 installation consists of 18 cells excavated in the ground and isolated by concrete. Each cell has a 40 m3. The cells will be filled with different soils from various sites in Spain including the Hontomín site in Burgos, where CIUDENs CO2 Storage Technological Development Plant is under construction. The cells are be equipped with systems for (i) controlled CO2 injection at different depths, (ii) control of irrigation and drainage in the unsaturated soil, (iii) sampling of groundwater and gases, and (iv) monitoring of different parameters; such as water content, pH, CO2 flux, microbiological, botanical, and biogeochemical alterations and the chemical composition of water. The main objectives are: the detection of potential diffuse leakage during/after the injection operations; the use of native species as bio-indicators of early leakage; the calibration and optimization of monitoring sensors & methodologies; the optimization of existing multiphase reactive transport models and the comprehension improvement of the biogeochemical processes. The facility is planned to be fully operational in November 2011. Its configuration makes it unique and suitable for international R&D programs. CIUDEN is open for cooperative research projects with institutions all over the world. Results are expected to significantly contribute to the development of new, useful, economical and ecological biomonitoring tools for wide areas. The paper will focus on the presentation of the technical caracteristics and the

  14. CO2 Accounting and Risk Analysis for CO2 Sequestration at Enhanced Oil Recovery Sites.

    PubMed

    Dai, Zhenxue; Viswanathan, Hari; Middleton, Richard; Pan, Feng; Ampomah, William; Yang, Changbing; Jia, Wei; Xiao, Ting; Lee, Si-Yong; McPherson, Brian; Balch, Robert; Grigg, Reid; White, Mark

    2016-07-19

    Using CO2 in enhanced oil recovery (CO2-EOR) is a promising technology for emissions management because CO2-EOR can dramatically reduce sequestration costs in the absence of emissions policies that include incentives for carbon capture and storage. This study develops a multiscale statistical framework to perform CO2 accounting and risk analysis in an EOR environment at the Farnsworth Unit (FWU), Texas. A set of geostatistical-based Monte Carlo simulations of CO2-oil/gas-water flow and transport in the Morrow formation are conducted for global sensitivity and statistical analysis of the major risk metrics: CO2/water injection/production rates, cumulative net CO2 storage, cumulative oil/gas productions, and CO2 breakthrough time. The median and confidence intervals are estimated for quantifying uncertainty ranges of the risk metrics. A response-surface-based economic model has been derived to calculate the CO2-EOR profitability for the FWU site with a current oil price, which suggests that approximately 31% of the 1000 realizations can be profitable. If government carbon-tax credits are available, or the oil price goes up or CO2 capture and operating expenses reduce, more realizations would be profitable. The results from this study provide valuable insights for understanding CO2 storage potential and the corresponding environmental and economic risks of commercial-scale CO2-sequestration in depleted reservoirs.

  15. CO2 deserts: implications of existing CO2 supply limitations for carbon management.

    PubMed

    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.

  16. Effects of CO2 leakage on soil bacterial communities from simulated CO2-EOR areas.

    PubMed

    Chen, Fu; Yang, Yongjun; Ma, Yanjun; Hou, Huping; Zhang, Shaoliang; Ma, Jing

    2016-05-18

    CO2-EOR (enhanced oil recovery) has been proposed as a viable option for flooding oil and reducing anthropogenic CO2 contribution to the atmospheric pool. However, the potential risk of CO2 leakage from the process poses a threat to the ecological system. High-throughput sequencing was used to investigate the effects of CO2 emission on the composition and structure of soil bacterial communities. The diversity of bacterial communities notably decreased with increasing CO2 flux. The composition of bacterial communities varied along the CO2 flux, with increasing CO2 flux accompanied by increases in the relative abundance of Bacteroidetes and Firmicutes phyla, but decreases in the relative abundance of Acidobacteria and Chloroflexi phyla. Within the Firmicutes phylum, the genus Lactobacillus increased sharply when the CO2 flux was at its highest point. Alpha and beta diversity analysis revealed that differences in bacterial communities were best explained by CO2 flux. The redundancy analysis (RDA) revealed that differences in bacterial communities were best explained by soil pH values which related to CO2 flux. These results could be useful for evaluating the risk of potential CO2 leakages on the ecosystems associated with CO2-EOR processes.

  17. Effects of Breathing Resistance on Resting Ventilatory Sensitivity to CO2

    DTIC Science & Technology

    2014-08-12

    through the same mechanism. It is possible that hyperbaric hyperoxia further decreases chemical sensitivity to CO2. Read’s rebreathing method...retention with inhaled CO2 and breathing resistance,” Undersea and Hyperbaric Medicine, Vol. 39, No. 4, pp. 815–828, 2012. 4.Naval Sea Systems Command

  18. Elevated CO2 and Soil Nitrogen Cycling

    NASA Astrophysics Data System (ADS)

    Hofmockel, K.; Schlesinger, W.

    2002-12-01

    Although forests can be large terrestrial carbon sinks, soil fertility can limit carbon sequestration in response to increased atmospheric CO2. During five years of CO2 fertilization (ambient + 200ppm) at the Duke Free-Air CO2 Enrichment (FACE) site, net primary production increased significantly by an average of 25% in treatment plots. Total nitrogen in the foliar canopy increased by 16%, requiring an additional 1.3 g N m-2yr-1 to be taken up from soils under elevated CO2. Mechanisms supporting increased nitrogen acquisition have not been identified. Here we report on biological N-fixation rates, using the acetylene reduction assay, in litter and mineral soil during three years of the CO2 enrichment experiment. Lack of a significant CO2 treatment effect on acetylene reduction indicates that carbon is not directly limiting biological N fixation. Nutrient addition experiments using a complete block design with glucose, Fe, Mo and P indicate biological N fixation is co-limited by molybdenum and carbon. These results suggest even if elevated atmospheric CO2 enhances below-ground carbon availability via root exudation, biological nitrogen fixation may not be stimulated due to micronutrient limitations. Assessment of future carbon sequestration by forest stands must consider limitations imposed by site fertility, including micronutrients.

  19. Glacial CO2 Cycles: A Composite Scenario

    NASA Astrophysics Data System (ADS)

    Broecker, W. S.

    2015-12-01

    There are three main contributors to the glacial drawdown of atmospheric CO2 content: starvation of the supply of carbon to the ocean-atmosphere reservoir, excess CO2 storage in the deep sea, and surface-ocean cooling. In this talk, I explore a scenario in which all three play significant roles. Key to this scenario is the assumption that deep ocean storage is related to the extent of nutrient stratification of the deep Atlantic. The stronger this stratification, the larger the storage of respiration CO2. Further, it is my contention that the link between Milankovitch insolation cycles and climate is reorganizations of the ocean's thermohaline circulation leading to changes in the deep ocean's CO2 storage. If this is the case, the deep Atlantic d13C record kept in benthic foraminifera shells tells us that deep ocean CO2 storage follows Northern Hemisphere summer insolation cycles and thus lacks the downward ramp so prominent in the records of sea level, benthic 18O and CO2. Rather, the ramp is created by the damping of planetary CO2 emissions during glacial time intervals. As it is premature to present a specific scenario, I provide an example as to how these three contributors might be combined. As their magnitudes and shapes remain largely unconstrained, the intent of this exercise is to provoke creative thinking.

  20. CO2 mitigation via accelerated limestone weathering

    USGS Publications Warehouse

    Rau, Greg H.; Knauss, Kevin G.; Langer, William H.; Caldeira,

    2004-01-01

    We evaluate accelerated weathering of limestone (AWL: CO2 + CaCO3 + H2O=> Ca2+ + 2HCO3-) as a low-tech, inexpensive, high-capacity, environmentally-friendly CO2 capture and sequestration technology. With access to seawater and limestone being essential to this approach, significant limestone resources are close to most CO2-emitting power plants along the coastal US. Waste fines, representing more than 20% of current US crushed limestone production (>109 tonnes/yr), could be used as an inexpensive source of AWL carbonate. Under such circumstances CO2 mitigation cost could be as low as $3-$4/tonne. More broadly, 10-20% of US point-source CO2 emissions could be treated at $20-$30/tonne CO2. AWL end-solution disposal in the ocean would significantly reduce effects on ocean pH and carbonate chemistry relative to those caused by direct atmospheric or ocean CO2 disposal. Indeed, the increase in ocean Ca2+ and bicarbonate offered by AWL should enhance growth of corals and other calcifying marine organisms.

  1. Geological factors affecting CO2 plume distribution

    USGS Publications Warehouse

    Frailey, S.M.; Leetaru, H.

    2009-01-01

    Understanding the lateral extent of a CO2 plume has important implications with regards to buying/leasing pore volume rights, defining the area of review for an injection permit, determining the extent of an MMV plan, and managing basin-scale sequestration from multiple injection sites. The vertical and lateral distribution of CO2 has implications with regards to estimating CO2 storage volume at a specific site and the pore pressure below the caprock. Geologic and flow characteristics such as effective permeability and porosity, capillary pressure, lateral and vertical permeability anisotropy, geologic structure, and thickness all influence and affect the plume distribution to varying degrees. Depending on the variations in these parameters one may dominate the shape and size of the plume. Additionally, these parameters do not necessarily act independently. A comparison of viscous and gravity forces will determine the degree of vertical and lateral flow. However, this is dependent on formation thickness. For example in a thick zone with injection near the base, the CO2 moves radially from the well but will slow at greater radii and vertical movement will dominate. Generally the CO2 plume will not appreciably move laterally until the caprock or a relatively low permeability interval is contacted by the CO2. Conversely, in a relatively thin zone with the injection interval over nearly the entire zone, near the wellbore the CO2 will be distributed over the entire vertical component and will move laterally much further with minimal vertical movement. Assuming no geologic structure, injecting into a thin zone or into a thick zone immediately under a caprock will result in a larger plume size. With a geologic structure such as an anticline, CO2 plume size may be restricted and injection immediately below the caprock may have less lateral plume growth because the structure will induce downward vertical movement of the CO2 until the outer edge of the plume reaches a spill

  2. Estimating lake-atmosphere CO2 exchange

    USGS Publications Warehouse

    Anderson, D.E.; Striegl, R.G.; Stannard, D.I.; Michmerhuizen, C.M.; McConnaughey, T.A.; LaBaugh, J.W.

    1999-01-01

    Lake-atmosphere CO2 flux was directly measured above a small, woodland lake using the eddy covariance technique and compared with fluxes deduced from changes in measured lake-water CO2 storage and with flux predictions from boundary-layer and surface-renewal models. Over a 3-yr period, lake-atmosphere exchanges of CO2 were measured over 5 weeks in spring, summer, and fall. Observed springtime CO2 efflux was large (2.3-2.7 ??mol m-2 s-1) immediately after lake-thaw. That efflux decreased exponentially with time to less than 0.2 ??mol m-2 s-1 within 2 weeks. Substantial interannual variability was found in the magnitudes of springtime efflux, surface water CO2 concentrations, lake CO2 storage, and meteorological conditions. Summertime measurements show a weak diurnal trend with a small average downward flux (-0.17 ??mol m-2 s-1) to the lake's surface, while late fall flux was trendless and smaller (-0.0021 ??mol m-2 s-1). Large springtime efflux afforded an opportunity to make direct measurement of lake-atmosphere fluxes well above the detection limits of eddy covariance instruments, facilitating the testing of different gas flux methodologies and air-water gas-transfer models. Although there was an overall agreement in fluxes determined by eddy covariance and those calculated from lake-water storage change in CO2, agreement was inconsistent between eddy covariance flux measurements and fluxes predicted by boundary-layer and surface-renewal models. Comparison of measured and modeled transfer velocities for CO2, along with measured and modeled cumulative CO2 flux, indicates that in most instances the surface-renewal model underpredicts actual flux. Greater underestimates were found with comparisons involving homogeneous boundary-layer models. No physical mechanism responsible for the inconsistencies was identified by analyzing coincidentally measured environmental variables.

  3. Detecting small scale CO2 emission structures using OCO-2

    NASA Astrophysics Data System (ADS)

    Schwandner, Florian M.; Eldering, Annmarie; Verhulst, Kristal R.; Miller, Charles E.; Nguyen, Hai M.; Oda, Tomohiro; O'Dell, Christopher; Rao, Preeti; Kahn, Brian; Crisp, David; Gunson, Michael R.; Sanchez, Robert M.; Ashok, Manasa; Pieri, David; Linick, Justin P.; Yuen, Karen

    2016-04-01

    Localized carbon dioxide (CO2) emission structures cover spatial domains of less than 50 km diameter and include cities and transportation networks, as well as fossil fuel production, upgrading and distribution infra-structure. Anthropogenic sources increasingly upset the natural balance between natural carbon sources and sinks. Mitigation of resulting climate change impacts requires management of emissions, and emissions management requires monitoring, reporting and verification. Space-borne measurements provide a unique opportunity to detect, quantify, and analyze small scale and point source emissions on a global scale. NASA's first satellite dedicated to atmospheric CO2 observation, the July 2014 launched Orbiting Carbon Observatory (OCO-2), now leads the afternoon constellation of satellites (A-Train). Its continuous swath of 2 to 10 km in width and eight footprints across can slice through coincident emission plumes and may provide momentary cross sections. First OCO-2 results demonstrate that we can detect localized source signals in the form of urban total column averaged CO2 enhancements of ~2 ppm against suburban and rural backgrounds. OCO-2's multi-sounding swath observing geometry reveals intra-urban spatial structures reflected in XCO2 data, previously unobserved from space. The transition from single-shot GOSAT soundings detecting urban/rural differences (Kort et al., 2012) to hundreds of soundings per OCO-2 swath opens up the path to future capabilities enabling urban tomography of greenhouse gases. For singular point sources like coal fired power plants, we have developed proxy detections of plumes using bands of imaging spectrometers with sensitivity to SO2 in the thermal infrared (ASTER). This approach provides a means to automate plume detection with subsequent matching and mining of OCO-2 data for enhanced detection efficiency and validation. © California Institute of Technology

  4. Atmospheric CO2 Removal by Enhancing Weathering

    NASA Astrophysics Data System (ADS)

    Koster van Groos, A. F.; Schuiling, R. D.

    2014-12-01

    The increase of the CO2 content in the atmosphere by the release of anthropogenic CO2 may be addressed by the enhancement of weathering at the surface of the earth. The average emission of mantle-derived CO2 through volcanism is ~0.3 Gt/year (109 ton/year). Considering the ~3.000 Gt of CO2 present in the atmosphere, the residence time of CO2 in the earth's atmosphere is ~10,000 years. Because the vast proportion of carbon in biomass is recycled through the atmosphere, CO2 is continuously removed by a series of weathering reactions of silicate minerals and stored in calcium and magnesium carbonates. The addition of anthropogenic CO2 from fossil fuel and cement production, which currently exceeds 35 Gt/year and dwarfs the natural production 100-fold, cannot be compensated by current rates of weathering, and atmospheric CO2 levels are rising rapidly. To address this increase in CO2 levels, weathering rates would have to be accelerated on a commensurate scale. Olivine ((Mg,Fe)2SiO4) is the most reactive silicate mineral in the weathering process. This mineral is the major constituent in relatively common ultramafic rocks such as dunites (olivine content > 90%). To consume the current total annual anthropogenic release of CO2, using a simplified weathering reaction (Mg2SiO4 + 4CO2 + 4H2O --> 2 Mg2+ + 4HCO3- + H4SiO4) would require ~30 Gt/year or ~8-9 km3/year of dunite. This is a large volume; it is about double the total amount of ore and gravel currently mined (~ 17 Gt/year). To mine and crush these rocks to <100 μm costs ~ 8/ton. The transport and distribution over the earth's surface involves additional costs, that may reach 2-5/ton. Thus, the cost of remediation for the release of anthropogenic CO2 is 300-400 billion/year. This compares to a 2014 global GDP of ~80 trillion. Because weathering reactions require the presence of water and proceed more rapidly at higher temperatures, the preferred environments to enhance weathering are the wet tropics. From a socio

  5. The oceanic sink for anthropogenic CO2.

    PubMed

    Sabine, Christopher L; Feely, Richard A; Gruber, Nicolas; Key, Robert M; Lee, Kitack; Bullister, John L; Wanninkhof, Rik; Wong, C S; Wallace, Douglas W R; Tilbrook, Bronte; Millero, Frank J; Peng, Tsung-Hung; Kozyr, Alexander; Ono, Tsueno; Rios, Aida F

    2004-07-16

    Using inorganic carbon measurements from an international survey effort in the 1990s and a tracer-based separation technique, we estimate a global oceanic anthropogenic carbon dioxide (CO2) sink for the period from 1800 to 1994 of 118 +/- 19 petagrams of carbon. The oceanic sink accounts for approximately 48% of the total fossil-fuel and cement-manufacturing emissions, implying that the terrestrial biosphere was a net source of CO2 to the atmosphere of about 39 +/- 28 petagrams of carbon for this period. The current fraction of total anthropogenic CO2 emissions stored in the ocean appears to be about one-third of the long-term potential.

  6. 40 CFR 98.423 - Calculating CO2 supply.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... = Quarterly CO2 concentration measurement in flow for flow meter u in quarter p (wt. %CO2). Qp,u = Quarterly... (metric tons) through flow meter u. CCO2,p = Quarterly CO2 concentration measurement in flow for flow... delivered by CO2 stream u. CCO2,p,u = Quarterly CO2 concentration measurement of CO2 stream u that...

  7. 40 CFR 98.423 - Calculating CO2 supply.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... = Quarterly CO2 concentration measurement in flow for flow meter u in quarter p (wt. %CO2). Qp,u = Quarterly... (metric tons) through flow meter u. CCO2,p = Quarterly CO2 concentration measurement in flow for flow... delivered by CO2 stream u. CCO2,p,u = Quarterly CO2 concentration measurement of CO2 stream u that...

  8. CO2-Leaking Well - Analytical Modeling

    NASA Astrophysics Data System (ADS)

    Wertz, F.; Audigane, P.; Bouc, O.

    2009-04-01

    The long-term integrity of CO2 storage in geological system relies highly on local trapping mechanisms but also on the absence/control of any kind of outlets. Indeed numerous pathways (faults, wells, rock heterogeneities…) exist that can lead stored gas back to the surface. Thus, such leakage risks must be assessed and quantified if possible. In France, BRGM is inquired for evaluating safety criteria and developing a methodology for qualifying potential geological storage sites. This implies in particular to study the leakage scenario, here through a water-filled well as a worth scenario case. In order to determine the kinds of impacts leaking CO2 can have; knowing the velocity and flow rate of uprising CO2 is a necessity. That is why a better knowledge of CO2 in storage conditions and its behaviour with the environment is required. The following study aims at characterising the CO2 flowing into the well and then rising up in a water column over the vertical dimension. An analytical model was built that describes: - In a first step, the CO2 flow between the reservoir and the inside of the well, depending on quality and thickness of different seals, which determines the flow rate through the well. - In a second step, the CO2 uprising through an open and water filled well, however in steady state, which excludes a priori the characterisation of periodic or chaotic behaviours such as geyser formation. The objective is to give numerous orders of magnitude concerning CO2 thermodynamic properties while rising up: specific enthalpy, density, viscosity, velocity, flow, gas volume fraction and expansion, pressure and temperature gradient. Dissolution is partially taken into account, however without kinetic. The strength of this model is to compute analytically - easily and instantaneously - the 1-dimensional rising velocity of CO2 in a water column as a function of the CO2 density, interfacial tension and initial volume fraction. Characteristic speeds - the ones given by

  9. CO2 Driven Mineral Transformations in Fractured Reservoir

    NASA Astrophysics Data System (ADS)

    Schaef, T.

    2015-12-01

    Engineering fracture systems in low permeable formations to increase energy production, accelerate heat extraction, or to enhance injectivity for storing anthropogenic CO2, is a challenging endeavor. To complicate matters, caprocks, essential components of subsurface reservoirs, need to maintain their sealing integrity in this modified subsurface system. Supercritical CO2 (scCO2), a proposed non-aqueous based working fluid, is capable of driving mineral transformations in fracture environments. Water dissolution in scCO2 significantly impacts the reactivity of this fluid, largely due to the development of thin adsorbed H2O films on the surfaces of exposed rocks and minerals. Adsorbed H2O films are geochemically complex microenvironments that host mineral dissolution and precipitation processes that could be tailored to influence overall formation permeability. Furthermore, manipulating the composition of injected CO2 (e.g., moisture content and/or reactive gases such as O2, NOx, or SOx) could stimulate targeted mineral transformations that enhance or sustain reservoir performance. PNNL has developed specialized experimental techniques that can be used to characterize chemical reactions occurring between minerals and pressurized gases. For example, hydration of a natural shale sample (Woodford Shale) has been characterized by an in situ infrared spectroscopic technique as water partitions from the scCO2 onto the shale. Mineral dissolution and carbonate precipitation reactions were tracked by monitoring changes of Si-O and C-O stretching bands, respectively Structural changes indicated expandable clays in the shale such as montmorillonite are intercalated with scCO2, a process not observed with the non-expandable kaolinite component. Extreme scale ab initio molecular dynamics simulations were used in conjunction with model mineral systems to identify the driving force and mechanism of water films. They showed that the film nucleation and formation on minerals is

  10. Fate of H2S during the cultivation of Chlorella sp. deployed for biogas upgrading.

    PubMed

    González-Sánchez, Armando; Posten, Clemens

    2017-04-15

    The H2S may play a key role in the sulfur cycle among the biogas production by the anaerobic digestion of wastes and the biogas upgrading by a microalgae based technology. The biogas is upgraded by contacting with slightly alkaline aqueous microalgae culture, then CO2 and H2S are absorbed. The dissolved H2S could limit or inhibit the microalgae growth. This paper evaluated the role of dissolved H2S and other sulfured byproducts under prevailing biogas upgrading conditions using a microalgal technology. At initial stages of batch cultivation the growth of Chlorella sp. was presumably inhibited by dissolved H2S. After 2 days, the sulfides were oxidized mainly by oxic chemical reactions to sulfate, which was later rapidly assimilated by Chlorella sp., allowing high growing rates. The fate of H2S during the microalgae cultivation at pH > 8.5 was assessed by a mathematical model where the pentasulfide, thiosulfate and sulfite were firstly produced and converted finally to sulfate for posterior assimilation.

  11. CO2 evaporative cooling: The future for tracking detector thermal management

    NASA Astrophysics Data System (ADS)

    Tropea, P.; Daguin, J.; Petagna, P.; Postema, H.; Verlaat, B.; Zwalinski, L.

    2016-07-01

    In the last few years, CO2 evaporative cooling has been one of the favourite technologies chosen for the thermal management of tracking detectors at LHC. ATLAS Insertable B-Layer and CMS Pixel phase 1 upgrade have adopted it and their systems are now operational or under commissioning. The CERN PH-DT team is now merging the lessons learnt on these two systems in order to prepare the design and construction of the cooling systems for the new Upstream Tracker and the Velo upgrade in LHCb, due by 2018. Meanwhile, the preliminary design of the ATLAS and CMS full tracker upgrades is started, and both concepts heavily rely on CO2 evaporative cooling. This paper highlights the performances of the systems now in operation and the challenges to overcome in order to scale them up to the requirements of the future generations of trackers. In particular, it focuses on the conceptual design of a new cooling system suited for the large phase 2 upgrade programmes, which will be validated with the construction of a common prototype in the next years.

  12. Effects of diffusion impairment on O2 and CO2 time courses in pulmonary capillaries.

    NASA Technical Reports Server (NTRS)

    Wagner, P. D.; West, J. B.

    1972-01-01

    Simultaneous time courses for O2 and CO2 exchange along the capillary have been calculated for homogeneous lungs, allowing for O2-CO2 interactions, dissolved O2, and chemical reaction rates. As diffusing capacity (Dl) was reduced, the transfer of CO2 and O2 was impaired by similar amounts, in spite of the 20-fold greater diffusing capacity for CO2. The reason why CO2 is affected so much is that the slope of the content against partial pressure is so much greater in blood than tissue for this gas. Because of the shapes of their respective dissociation curves, O2 transfer was most affected at normal ventilation-perfusion ratios, whereas CO2 was most affected at high ratios. Exercise exaggerated the impairment of transfer of both gases.

  13. Reversible CO2 Capture by Conjugated Ionic Liquids through Dynamic Covalent Carbon-Oxygen Bonds.

    PubMed

    Pan, Mingguang; Cao, Ningning; Lin, Wenjun; Luo, Xiaoyan; Chen, Kaihong; Che, Siying; Li, Haoran; Wang, Congmin

    2016-09-08

    The strong chemisorption of CO2 is always accompanied by a high absorption enthalpy, and traditional methods to reduce the absorption enthalpy lead to decreased CO2 capacities. Through the introduction of a large π-conjugated structure into the anion, a dual-tuning approach for the improvement of CO2 capture by anion-functionalized ionic liquids (ILs) resulted in a high capacity of up to 0.96 molCO2  mol-1IL and excellent reversibility. The increased capacity and improved desorption were supported by quantum chemical calculations, spectroscopic investigations, and thermogravimetric analysis. The increased capacity may be a result of the strengthened dynamic covalent bonds in these π-electron-conjugated structures through anion aggregation upon the uptake of CO2 , and the improved desorption originates from the charge dispersion of interaction sites through the large π-electron delocalization. These results provide important insights into effective strategies for CO2 capture.

  14. CO2 Capture from Ambient Air by Crystallization with a Guanidine Sorbent.

    PubMed

    Seipp, Charles A; Williams, Neil J; Kidder, Michelle K; Custelcean, Radu

    2017-01-19

    Carbon capture and storage is an important strategy for stabilizing the increasing concentration of atmospheric CO2 and the global temperature. A possible approach toward reversing this trend and decreasing the atmospheric CO2 concentration is to remove the CO2 directly from air (direct air capture). Herein we report a simple aqueous guanidine sorbent that captures CO2 from ambient air and binds it as a crystalline carbonate salt by guanidinium hydrogen bonding. The resulting solid has very low aqueous solubility (Ksp =1.0(4)×10(-8) ), which facilitates its separation from solution by filtration. The bound CO2 can be released by relatively mild heating of the crystals at 80-120 °C, which regenerates the guanidine sorbent quantitatively. Thus, this crystallization-based approach to CO2 separation from air requires minimal energy and chemical input, and offers the prospect for low-cost direct air capture technologies.

  15. CO2 Sequestraion by Mineral Carbonation of Cement Material

    NASA Astrophysics Data System (ADS)

    Jo, H.; Jang, Y.

    2010-12-01

    CO2 sequestration by mineral carbonation with cement materials was investigated in this study. Ca extraction and CO2 injection tests were conducted on three different materials (lime, Portland cement, waste concrete) using different extract reagents (NH4Cl, CH3COOH, HCl, and Deionized water) under ambient temperature and pressure conditions. CO2 gas (99.9%) was injected to either supernatant without solids or suspension with solids obtained from extraction tests at 4 ml/min of flow rate. Ca concentrations were measured from filtered solutions before and after CO2 injection. The chemical and mineralogical composition of raw materials and precipitates were determined using X-ray fluorescence and X-ray diffraction, respectively. The morphology and chemical composition of precipitates were analyzed with Field Emission Scanning Electron Microscopy equipped with the Energy Dispersive X-ray analysis. For the extraction tests, Ca concentrations of the extracts were related with the CaO content and type of CaO bearing minerals of the materials, regardless of the extraction solutions. Lime had a higher Ca concentration ranging between 942.7 and 39945.0 mg/L in the extracts than waste concrete (188.4 ~ 2978.1 mg/L) in the extracts due to its higher content of CaO (CaO : 24.5% and waste concrete : 20.3%). In contrast, the Portland cement (6346.0 and 28903.5 mg/L) had lower Ca concentrations than lime (94.27 ~ 39945.0 mg/L), even though the Portland cement (56.3%) had a higher CaO content than lime (24.5%). For a given extraction solution, lime had the highest CO2 carbonation efficiency. In addition, for a given material, the CO2 carbonation efficiency was the highest when NH4Cl solution was used as an extraction solution. Results of material analyses indicate that precipitates from the CO2 injection tests consisted of mostly CaCO3, regardless of types of materials and extraction solutions.

  16. Long-term pCO2 trends in Adirondack Lakes

    NASA Astrophysics Data System (ADS)

    Seekell, David A.; Gudasz, Cristian

    2016-05-01

    Lakes are globally significant sources of CO2 to the atmosphere. However, there are few temporally resolved records of lake CO2 concentrations and long-term patterns are poorly characterized. We evaluated annual trends in the partial pressure of CO2 (pCO2) based on chemical measurements from 31 Adirondack Lakes taken monthly over an 18 year period. All lakes were supersaturated with CO2 and were sources of CO2 to the atmosphere. There were significant pCO2 trends in 29% of lakes. The median magnitude of significant positive trends was 32.1 µatm yr-1. Overall, 52% of lakes had pCO2 trends greater than those reported for the atmosphere and ocean. Significant trends in lake pCO2 were attributable to regional recovery from acid deposition and changing patterns of ice cover. These results illustrate that lake pCO2 can respond rapidly to environmental change, but the lack of significant trend in 71% of lakes indicates substantial lake-to-lake variation in magnitude of response.

  17. CO2 Sensing and CO2 Regulation of Stomatal Conductance: Advances and Open Questions.

    PubMed

    Engineer, Cawas B; Hashimoto-Sugimoto, Mimi; Negi, Juntaro; Israelsson-Nordström, Maria; Azoulay-Shemer, Tamar; Rappel, Wouter-Jan; Iba, Koh; Schroeder, Julian I

    2016-01-01

    Guard cells form epidermal stomatal gas-exchange valves in plants and regulate the aperture of stomatal pores in response to changes in the carbon dioxide (CO2) concentration ([CO2]) in leaves. Moreover, the development of stomata is repressed by elevated CO2 in diverse plant species. Evidence suggests that plants can sense [CO2] changes via guard cells and via mesophyll tissues in mediating stomatal movements. We review new discoveries and open questions on mechanisms mediating CO2-regulated stomatal movements and CO2 modulation of stomatal development, which together function in the CO2 regulation of stomatal conductance and gas exchange in plants. Research in this area is timely in light of the necessity of selecting and developing crop cultivars that perform better in a shifting climate.

  18. Fabry-Perot Interferometer for Column CO2

    NASA Technical Reports Server (NTRS)

    Heaps, William S.; Kawa, S. Randolph; Krebs, Carolyn A. (Technical Monitor)

    2002-01-01

    Global atmospheric CO2 measurements are essential to resolving significant discrepancies in our understanding of the global carbon budget and, hence, humankind's role in global climate change. The science measurement requirements for CO2 are extremely demanding (precision is less than .3%). No atmospheric chemical species has ever been measured from space with this precision. We are developing a novel application of a Fabry-Perot interferometer to detect spectral absorption of reflected sunlight by CO2 and O2 in the atmosphere. Preliminary design studies indicate that the method will be able to achieve the sensitivity and signal-to-noise detection required to measure column CO2 at the target specification. The objective of this program is to construct a prototype instrument for deployment on an aircraft to test the instrument performance and our ability to retrieve the data in the real atmosphere. To date we have assembled a laboratory bench system to begin testing the optical and electronic components. We are also undertaking some measurements of signal and noise levels for actual sunlight reflecting from the ground in order to evaluate the potential of some components to meet the exacting requirements of this measurement.

  19. Fabry-Perot Interferometer for Column CO2

    NASA Technical Reports Server (NTRS)

    Heaps, William S.; Kawa, Randolph; Bhartia, P. K. (Technical Monitor)

    2002-01-01

    Global atmospheric CO2 measurements are essential to resolving significant discrepancies in our understanding of the global carbon budget and, hence, humankind's role in global climate change. The science measurement requirements for CO2 are extremely demanding (precision approx. 0.3%). No atmospheric chemical species has ever been measured from space with this precision. We are developing a novel application of a Fabry-Perot interferometer to detect spectral absorption of reflected sunlight by CO2 and O2 in the atmosphere. Preliminary design studies indicate that the method will be able to achieve the sensitivity and signal-to-noise detection required to measure column CO2 at the target specification. The objective of this program is to construct a prototype instrument for deployment on an aircraft to test the instrument performance and our ability to retrieve the data in the real atmosphere. To date we have assembled a laboratory bench system to begin testing the optical and electronic components. We are also measuring signal and noise levels in actual sunlight to evaluate component performance.

  20. Surface modification of activated carbons for CO 2 capture

    NASA Astrophysics Data System (ADS)

    Pevida, C.; Plaza, M. G.; Arias, B.; Fermoso, J.; Rubiera, F.; Pis, J. J.

    2008-09-01

    The reduction of anthropogenic CO 2 emissions to address the consequences of climate change is a matter of concern for all developed countries. In the short term, one of the most viable options for reducing carbon emissions is to capture and store CO 2 at large stationary sources. Adsorption with solid sorbents is one of the most promising options. In this work, two series of materials were prepared from two commercial activated carbons, C and R, by heat treatment with gaseous ammonia at temperatures in the 200-800 °C range. The aim was to improve the selectivity and capacity of the sorbents to capture CO 2, by introducing basic nitrogen-functionalities into the carbons. The sorbents were characterised in terms of texture and chemical composition. Their surface chemistry was studied through temperature-programmed desorption tests and X-ray photoelectron spectroscopy. The capture performance of the carbons was evaluated by using a thermogravimetric analyser to record mass uptakes by the samples when exposed to a CO 2 atmosphere.

  1. Translucent CO2 ice on Mars ?

    NASA Astrophysics Data System (ADS)

    Schmidt, Frederic; Andrieu, Francois; Douté, Sylvain; Schmitt, Bernard

    2016-10-01

    The Martian climate is driven by the condensation/sublimation of CO2 representing 95% of the atmosphere. Many active surface features (such dark spot, dark flows), have been potentially linked to CO2 exchange. Understanding the surface/atmosphere interactions is a major issue, for both atmospheric but also surface science. This study aims at estimating the physical properties of the seasonal CO2 ice deposits. Are these deposits granular or compact? What is the thickness of the ice? How much impurities are included within the ice? These questions have been highly debated in the literature, in particular the presence of a translucent slab ice, the link with the H2O cycle. In particular the cold jet geyser model requires translucent CO2 ice. We use radiative transfer models to simulate spectroscopic data from the CRISM instrument and perform an inversion to estimate model's parameters though time. We then discuss the consistency of the results with other datasets.

  2. EPIC Computer Upgrade

    NASA Video Gallery

    Expedition 30 Commander Dan Burbank and Flight Engineer Don Pettit work on installing hardware for the Enhanced Processor and Integrated Communications (EPIC) upgrade of the International Space Sta...

  3. The D0 Upgrade

    SciTech Connect

    Abachi, S.; D0 Collaboration

    1995-07-01

    In this paper we describe the approved DO Upgrade detector, and its physics capabilities. The DO Upgrade is under construction and will run during the next Fermilab collider running period in early 1999 (Run II). The upgrade is designed to work at the higher luminosities and shorter bunch spacings expected during this run. The major elements of t he upgrade are: a new tracking system with a silicon tracker, scintillating fiber tracker, a 2T solenoid, and a central preshower detector; new calorimeter electronics; new muon trigger and tracking detectors with new muon system electronics; a forward preshower detector; new trigger electronics and DAQ improvements to handle the higher rates.

  4. Spatiotemporal variability of lake pCO2 and CO2 fluxes in a hemiboreal catchment

    NASA Astrophysics Data System (ADS)

    Natchimuthu, Sivakiruthika; Sundgren, Ingrid; Gâlfalk, Magnus; Klemedtsson, Leif; Bastviken, David

    2017-01-01

    Globally, lakes are frequently supersaturated with carbon dioxide (CO2) and are major emitters of carbon to the atmosphere. Recent studies have generated awareness of the high variability in pCO2aq (the partial pressure corresponding to the concentration in water) and CO2 fluxes to the atmosphere and the need for better accounting for this variability. However, studies simultaneously accounting for both spatial and temporal variability of pCO2aq and CO2 fluxes in lakes are rare. We measured pCO2aq (by both manual sampling and mini loggers) and CO2 fluxes, covering spatial variability in open water areas of three lakes of different character in a Swedish catchment for 2 years. Spatial pCO2aq variability within lakes was linked to distance from shore, proximity to stream inlets, and deepwater upwelling events. Temporally, pCO2aq variability was linked with variability in dissolved organic carbon, total nitrogen, and dissolved oxygen. While previous studies over short time periods (1 to 6 h) observed gas transfer velocity (k) to be more variable than pCO2aq, our work shows that over longer time (days to weeks) pCO2aq variability was greater and affected CO2 fluxes much more than k. We demonstrate that ≥8 measurement days distributed over multiple seasons in combination with sufficient spatial coverage (≥8 locations during stratification periods and 5 or less in spring and autumn) are a key for representative yearly whole lake flux estimates. This study illustrates the importance of considering spatiotemporal variability in pCO2aq and CO2 fluxes to generate representative whole lake estimates.

  5. How secure is subsurface CO2 storage? Controls on leakage in natural CO2 reservoirs

    NASA Astrophysics Data System (ADS)

    Miocic, Johannes; Gilfillan, Stuart; McDermott, Christopher; Haszeldine, Stuart

    2014-05-01

    Carbon Capture and Storage (CCS) is the only industrial scale technology available to directly reduce carbon dioxide (CO2) emissions from fossil fuelled power plants and large industrial point sources to the atmosphere. The technology includes the capture of CO2 at the source and transport to subsurface storage sites, such as depleted hydrocarbon reservoirs or saline aquifers, where it is injected and stored for long periods of time. To have an impact on the greenhouse gas emissions it is crucial that there is no or only a very low amount of leakage of CO2 from the storage sites to shallow aquifers or the surface. CO2 occurs naturally in reservoirs in the subsurface and has often been stored for millions of years without any leakage incidents. However, in some cases CO2 migrates from the reservoir to the surface. Both leaking and non-leaking natural CO2 reservoirs offer insights into the long-term behaviour of CO2 in the subsurface and on the mechanisms that lead to either leakage or retention of CO2. Here we present the results of a study on leakage mechanisms of natural CO2 reservoirs worldwide. We compiled a global dataset of 49 well described natural CO2 reservoirs of which six are leaking CO2 to the surface, 40 retain CO2 in the subsurface and for three reservoirs the evidence is inconclusive. Likelihood of leakage of CO2 from a reservoir to the surface is governed by the state of CO2 (supercritical vs. gaseous) and the pressure in the reservoir and the direct overburden. Reservoirs with gaseous CO2 is more prone to leak CO2 than reservoirs with dense supercritical CO2. If the reservoir pressure is close to or higher than the least principal stress leakage is likely to occur while reservoirs with pressures close to hydrostatic pressure and below 1200 m depth do not leak. Additionally, a positive pressure gradient from the reservoir into the caprock averts leakage of CO2 into the caprock. Leakage of CO2 occurs in all cases along a fault zone, indicating that

  6. Study on CO2 global recycling system.

    PubMed

    Takeuchi, M; Sakamoto, Y; Niwa, S

    2001-09-28

    In order to assist in finding ways to mitigate CO2 emission and to slow the depletion of fossil fuels we have established and evaluated a representative system, which consists of three technologies developed in our laboratory. These technologies were in CO2 recovery, hydrogen production and methanol synthesis and in addition we established the necessary supporting systems. Analysis of outline designs of the large scale renewable energy power generation system and this system and energy input for building plant, energy input for running plant has been conducted based on a case using this system for a 1000-MW coal fired power plant, followed by an evaluation of the material balance and energy balance. The results are as follows. Energy efficiency is 34%, the CO2 reduction rate is 41%, the balance ratio of the energy and CO2 of the system is 2.2 and 1.8, respectively, on the assumption that the primary renewable energy is solar thermal power generation, the stationary CO2 emission source is a coal-fired power plant and the generation efficiency of the methanol power plant is 60%. By adopting the system, 3.7 million tons of CO2 can be recovered, approximately 2.7 million tons of methanol can be produced, and 15.4 billion kWh of electricity can be generated per year. Compared to generating all electrical power using only coal, approximately 2.6 million tons of coal per year can be saved and approximately 2.15 million tons of CO2 emission can be reduced. Therefore, it is clearly revealed that this system would be effective to reduce CO2 emissions and to utilize renewable energy.

  7. Bifunctional Catalysts for CO2 Reduction

    DTIC Science & Technology

    2014-09-30

    AFRL-OSR-VA-TR-2014-0243 Bifunctional catalysts for CO2 reduction Theodore Betley HARVARD COLLEGE PRESIDENT & FELLOWS OF Final Report 09/30/2014...Prescribed by ANSI Std. Z39.18 PI: Theodore A. Betley Project: Bifunctional Catalysts for CO2 Reduction Project #: 130214 A. Specific Aims 1... catalyst platforms. Details for the construction of these materials, as they deviate from the salen/salan platforms will be described below. 2. Probe

  8. Influence of drying methods and agronomic variables on the chemical composition of mate tea leaves (Ilex paraguariensis A. St.-Hil) obtained from high-pressure CO2 extraction.

    PubMed

    Jacques, Rosângela Assis; Krause, Laiza Canielas; Freitas, Lisiane dos Santos; Dariva, Cláudio; Oliveira, J Vladimir; Caramão, Elina Bastos

    2007-12-12

    The main objective of this work is to assess the influence of two drying methods (microwave and vacuum oven) and some agronomic variables (plant fertilization conditions and sunlight intensity) on the characteristics of mate tea (Ilex paraguariensis) leaves extracts obtained from high-pressure carbon dioxide extractions performed in the temperature range from 20 to 40 degrees C and from 100 to 250 bar. Samples of mate were collected in an experiment conducted under agronomic control at Ervateira Barão LTDA, Brazil. Chemical distribution of the extracts was evaluated by gas chromatography coupled with a mass spectrometer detector (GC/MS). In addition to extraction variables, results showed that both sample drying methods and agronomic conditions exert a pronounced influence on the extraction yield and on the chemical distribution of the extracts.

  9. CO2 Acquisition Membrane (CAM) Project

    NASA Technical Reports Server (NTRS)

    Mason, Larry W.

    2003-01-01

    The CO2 Acquisition Membrane (CAM) project was performed to develop, test, and analyze thin film membrane materials for separation and purification of carbon dioxide (CO2) from mixtures of gases, such as those found in the Martian atmosphere. The membranes developed in this project are targeted toward In Situ Resource Utilization (ISRU) applications, such as In Situ Propellant Production (ISPP) and In Situ Consumables Production (ISCP). These membrane materials may be used in a variety of ISRU systems, for example as the atmospheric inlet filter for an ISPP process to enhance the concentration of CO2 for use as a reactant gas, to passively separate argon and nitrogen trace gases from CO2 for habitat pressurization, to provide a system for removal of CO2 from breathing gases in a closed environment, or within a process stream to selectively separate CO2 from other gaseous components. The membranes identified and developed for CAM were evaluated for use in candidate ISRU processes and other gas separation applications, and will help to lay the foundation for future unmanned sample return and human space missions. CAM is a cooperative project split among three institutions: Lockheed Martin Astronautics (LMA), the Colorado School of Mines (CSM), and Marshall Space Flight Center (MSFC).

  10. CO2 cooling in terrestrial planet thermospheres

    NASA Technical Reports Server (NTRS)

    Bougher, S. W.; Hunten, D. M.; Roble, R. G.

    1994-01-01

    We examine the recent progress in the debate on the CO2-O relaxation rate, its temperature dependence, and its corresponding impact on the thermospheric heat budgets of Venus, Earth, and Mars. This comparative approach provides the broadest range of conditions under which a common CO2-O relaxation rate should provide consistent results. New global mean calculations are presented for the heat budgets of these three planets using large CO2-O relaxation rates that have been inferred recently from Earth CO2 radiance measurements and laboratory studies. Results indicate that available Venus and Mars data constrain the CO2-O relaxation rate to be 2-4 x 10(exp -12)/cu cm/s at 300 K. For Venus, this strong cooling serves as an effective thermostat that gives rise to a small variation of thermospheric temperatures over the solar cycle, just as observed. Conversely, CO2 cooling does not appear to be dominant in the dayside heat budget of the Mars thermosphere over most of the solar cycle. For the Earth, this strong cooling implies that the lower thermosphere does not typically require significant eddy diffusion or heat conduction. However, global-scale dynamics or an additional heating mechanism may be needed to restore calculated temperatures to observed values when relaxation rates exceeding 2 x 10(exp -12)/cu cm/s are employed.

  11. CO2 Efflux from Cleared Mangrove Peat

    PubMed Central

    Lovelock, Catherine E.; Ruess, Roger W.; Feller, Ilka C.

    2011-01-01

    Background CO2 emissions from cleared mangrove areas may be substantial, increasing the costs of continued losses of these ecosystems, particularly in mangroves that have highly organic soils. Methodology/Principal Findings We measured CO2 efflux from mangrove soils that had been cleared for up to 20 years on the islands of Twin Cays, Belize. We also disturbed these cleared peat soils to assess what disturbance of soils after clearing may have on CO2 efflux. CO2 efflux from soils declines from time of clearing from ∼10 600 tonnes km−2 year−1 in the first year to 3000 tonnes km2 year−1 after 20 years since clearing. Disturbing peat leads to short term increases in CO2 efflux (27 umol m−2 s−1), but this had returned to baseline levels within 2 days. Conclusions/Significance Deforesting mangroves that grow on peat soils results in CO2 emissions that are comparable to rates estimated for peat collapse in other tropical ecosystems. Preventing deforestation presents an opportunity for countries to benefit from carbon payments for preservation of threatened carbon stocks. PMID:21738628

  12. Density of aqueous solutions of CO2

    SciTech Connect

    Garcia, Julio E.

    2001-10-10

    In this report, we present a numerical representation for the partial molar volume of CO2 in water and the calculation of the corresponding aqueous solution density. The motivation behind this work is related to the importance of having accurate representations for aqueous phase properties in the numerical simulation of carbon dioxide disposal into aquifers as well as in geothermal applications. According to reported experimental data the density of aqueous solutions of CO2 can be as much as 2-3% higher than pure water density. This density variation might produce an influence on the groundwater flow regime. For instance, in geologic sequestration of CO2, convective transport mixing might occur when, several years after injection of carbon dioxide has stopped, the CO2-rich gas phase is concentrated at the top of the formation, just below an overlaying caprock. In this particular case the heavier CO2 saturated water will flow downward and will be replaced by water with a lesser CO2 content.

  13. CO2-water-mineral reactions during CO2 leakage into glauconitic sands: geochemical and isotopic monitoring of batch experiments

    NASA Astrophysics Data System (ADS)

    Humez, P.; Lions, J.; Lagneau, V.; Negrel, Ph.

    2012-04-01

    The assessment of environmental impacts of carbon dioxide geological storage requires the investigation of the potential CO2 leakages into fresh groundwater reserves. The Albian aquifer of the Paris Basin was chosen as a case of study because i) the Paris Basin contains deep saline Jurassic and Triassic aquifers identified as targets by the French national program of CO2 geological storage and ii) the Albian aquifer is a deep freshwater resource of strategic national importance, above the Jurassic and Triassic formations. An experimental and a geochemical modelling approach were carried out in order to better understand the rock-water-CO2 interactions with two main objectives: to assess the evolution of the chemistry of the formation water and of the mineralogy of the solid phase during the interaction and to design a monitoring program for freshwater resources. The main focus is to select and develop suitable indirect indicators of the presence of CO2 in the aquifer. We present here the experimental results, which combines both major and trace elements and isotopic tools, some of them new in the CCS field. Batch reactors with a liquid/solid ratio of 10 made of appropriate materials (PTFE, stainless steel) were equipped with simultaneous controls on several parameters (pH measurement, gas phase composition, pressure, tightness…) after CO2 injection (PCO2= 2 bar; room temperature). Ten reactors were run simultaneously, over pre-determined durations of CO2-water-rock interaction (1, 7, 15 and 30 days). During the batch experiment, we observed major changes in several chemical parameters due to the CO2 injection. A sharp drop in pH from 6.6 to 4.9 was noticeable, immediately after the injection, due to CO2 dissolution in the water phase. Alkalinity varies from 1.3 mmol.L-1 in the initial water to 2.0 mmol.L-1 at the end of the 1-month experiment. Four types of ion behaviors are observed: (1) calcium, silicon and magnesium concentrations increase during the 1-month

  14. NREL's Cyanobacteria Engineering Shortens Biofuel Production Process, Captures CO2

    SciTech Connect

    2015-09-01

    This highlight describes NREL's work to systematically analyze the flow of energy in a photosynthetic microbe and show how the organism adjusts its metabolism to meet the increased energy demand for making ethylene. This work successfully demonstrates that the organism could cooperate by stimulating photosynthesis. The results encourage further genetic engineering for the conversion of CO2 to biofuels and chemicals. This highlight is being developed for the September 2015 Alliance S&T Board meeting. biofuels and chemicals. This highlight is being developed for the September 2015 Alliance S&T Board meeting.

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

    USGS Publications Warehouse

    Rosenbauer, R.J.; Koksalan, T.

    2004-01-01

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

  16. Exploratory study of some potential environmental impacts of CO2 sequestration in unmineable coal seams

    SciTech Connect

    Hedges, S.W.; Soong, Y.; Jones, R.J.; Harrison, D.K.; Irdi, G.A.; Frommell, E.A.; Dilmore, R.M.; White, C.M.

    2007-01-01

    An initial investigation into the potential environmental impacts of CO2 sequestration in unmineable coal seams has been conducted, focusing on changes in the produced water during enhanced coalbed methane (ECBM) production, using a CO2 injection process (CO2-ECBM). A high volatile bituminous coal, Pittsburgh No. 8, was reacted with synthetic produced water and gaseous carbon dioxide at 40°C and 50 bar to evaluate the potential for mobilisation of toxic metals during CO2-ECBM/sequestration. Microscopic and X-ray diffraction analysis of the post-reaction coal samples clearly show evidence of chemical reaction and chemical analysis of the synthetic produced water shows substantial changes in composition. These results suggest that changes to the produced water chemistry and the potential for mobilising toxic trace elements from coal beds are important factors to be considered when evaluating deep, unmineable coal seams for CO2 sequestration.

  17. Will atmospheric CO2 concentration continue to increase if anthropogenic CO2 emissions cease?

    NASA Astrophysics Data System (ADS)

    MacDougall, A. H.; Eby, M.; Weaver, A. J.

    2013-12-01

    If anthropogenic CO2 emissions were to suddenly cease, the evolution of the atmospheric CO2 concentration would depend on the magnitude and sign of natural carbon sources and sinks. Experiments using Earth system models indicate that overall carbon sinks would dominate. However, these models have typically neglected the permafrost carbon pool, which has the potential to introduce an additional terrestrial source of carbon to the atmosphere. Here we use the University of Victoria Earth System Climate Model, which has recently been expanded to include permafrost carbon stocks and exchanges with the atmosphere. In a scenario of zeroed CO2 and sulphate aerosol emissions, we assess whether the warming induced by specified constant concentrations of non-CO2 greenhouse gases could slow the CO2 decline following zero emissions, or even reverse this trend and cause CO2 to increase over time. We find that a radiative forcing from non-CO2 gases of approximately 0.6 W m-2 results in a near balance of CO2 emissions from the terrestrial biosphere and uptake of CO2 by the oceans, resulting in near-constant atmospheric CO2 concentrations for at least a century after emissions are eliminated. At higher values of non-CO2 radiative forcing, CO2 concentrations increase over time, regardless of when emissions cease during the 21st century. Given that the present-day radiative forcing from non-CO2 greenhouse gases is about 0.95 W m-2, our results suggest that if we were to eliminate all CO2 and aerosols emissions without also decreasing non-CO2 greenhouse gas emissions, CO2 levels would increase over time, resulting in a small increase in climate warming. The sudden and total cessation of anthropogenic CO2 emissions is an unlikely future scenario. However, such cessation experiments provide a useful method for evaluating the relative strength of the terrestrial and oceanic carbon cycle feedbacks in the presence of forcing from non-CO2 greenhouse gasses.

  18. Global CO2 simulation using GOSAT-based surface CO2 flux estimates

    NASA Astrophysics Data System (ADS)

    Takagi, H.; Oda, T.; Saito, M.; Valsala, V.; Belikov, D.; Saeki, T.; Saito, R.; Morino, I.; Uchino, O.; Yoshida, Y.; Yokota, Y.; Bril, A.; Oshchepkov, S.; Andres, R. J.; Maksyutov, S.

    2012-04-01

    Investigating the distribution and temporal variability of surface CO2 fluxes is an active research topic in the field of contemporary carbon cycle dynamics. The technique central to this effort is atmospheric inverse modeling with which surface CO2 fluxes are estimated by making corrections to a priori flux estimates such that mismatches between model-predicted and observed CO2 concentrations are minimized. Past investigations were carried out by utilizing CO2 measurements collected in global networks of surface-based monitoring sites. Now, datasets of column-averaged CO2 dry air mole fraction (XCO2) retrieved from spectral soundings collected by GOSAT are available for complementing the surface-based CO2 observations. These space-based XCO2 data are expected to enhance the spatiotemporal coverage of the existing surface observation network and thus reduce uncertainty associated with the surface flux estimates. We estimated monthly CO2 fluxes in 64 sub-continental regions from a subset of the surface-based GLOBALVIEW CO2 data and the GOSAT FTS SWIR Level 2 XCO2 retrievals. We further simulated CO2 concentrations in 3-D model space using the surface flux estimates obtained. In this presentation, we report the result of a comparison between the simulated CO2 concentrations and independent surface observations. As part of an effort in inter-comparing GOSAT-based surface CO2 flux estimates, we also look at results yielded with XCO2 data retrieved with the PPDF-DOAS algorithm and those made available by the NASA Atmospheric CO2 Observations from Space team. For this study, we used version 08.1 of the National Institute for Environmental Studies atmospheric transport model, which was driven by the Japan Meteorological Agency's JCDAS wind analysis data. The CO2 forward simulations were performed on 2.5° × 2.5° horizontal grids at 32 vertical levels between the surface and the top of the atmosphere. The a priori flux dataset used was comprised of the sum of four

  19. Commitment accounting for CO2 emissions

    NASA Astrophysics Data System (ADS)

    Davis, S. J.; Socolow, R. H.

    2013-12-01

    Long-lived energy infrastructure that burns fossil fuels represents a multi-decade 'commitment' to emit CO2. Today's global power sector, alone, represents hundreds of billions of tons of still unrealized 'committed emissions' of CO2. And every year, substantial new commitments to future emissions are made, as new power plants are built. The socioeconomic inertia of these commitments is a major barrier to climate change mitigation. Here, we quantify these annual commitments by a bottom-up analysis of all power plants commissioned between 1950 and 2011; assigning emission commitments to the year when each generator came on line. We find, assuming 40-year commitments, that the global commitment to future emissions from the world's generators in 2011 (the most recent year in our analysis) was 318 Gt CO2, of which 216 Gt CO2 were commitments from the world's coal-fired generators and 134 Gt CO2 were commitments from China's generators. Annual new global commitments exceeded 15 Gt CO2 per year in every year since 2000. Moreover, between 2005-2010 (the latest year of available emissions data), new global commitments were more than twice as large as actual emissions from all power plants. Country-specific ratios of new committed emissions to actual emissions, averaged over 1990-2010 were 4.1 for China, 2.6 for India, 0.9 for the EU, and 0.6 for the US. We urge that the reporting of annual CO2 emissions, already widely institutionalized, be augmented by 'commitment accounting' which makes these future emissions salient. Annual committed emissions and annual emissions of primary power infrastructure. New committed emissions (light green) have grown from approximately 4 Gt CO2 per year in 1960 to roughly 10 Gt CO2 per year between 1970-1995, and then to more than 15 Gt CO2 per year since 2000. Throughout this period, new committed emissions have exceeded annual emissions (blue curve, source: IEA). Although the commitments made 30-40 years ago have largely been realized (dark

  20. Precursory volcanic CO2 signals from space

    NASA Astrophysics Data System (ADS)

    Schwandner, Florian M.; Carn, Simon A.; Kataoka, Fumie; Kuze, Akihiko; Shiomi, Kei; Goto, Naoki

    2016-04-01

    Identification of earliest signals heralding volcanic unrest benefits from the unambiguous detection of precursors that reflect deviation of magmatic systems from metastable background activity. Ascent and emplacement of new basaltic magma at depth may precede eruptions by weeks to months. Transient localized carbon dioxide (CO2) emissions stemming from exsolution from depressurized magma are expected, and have been observed weeks to months ahead of magmatic surface activity. Detecting such CO2 precursors by continuous ground-based monitoring operations is unfortunately not a widely implemented method yet, save a handful of volcanoes. Detecting CO2 emissions from space offers obvious advantages - however it is technologically challenging, not the least due to the increasing atmospheric burden of CO2, against which a surface emission signal is hard to discern. In a multi-year project, we have investigated the feasibility of space-borne detection of pre-eruptive volcanic CO2 passive degassing signals using observations from the Greenhouse Gas Observing SATellite (GOSAT). Since 2010, we have observed over 40 active volcanoes from space using GOSAT's special target mode. Over 72% of targets experienced at least one eruption over that time period, demonstrating the potential utility of space-borne CO2 observations in non-imaging target-mode (point source monitoring mode). While many eruption precursors don't produce large enough CO2 signals to exceed space-borne detection thresholds of current satellite sensors, some of our observations have nevertheless already shown significant positive anomalies preceding eruptions at basaltic volcanoes. In 2014, NASA launched its first satellite dedicated to atmospheric CO2 observation, the Orbiting Carbon Observatory (OCO-2). Its observation strategy differs from the single-shot GOSAT instrument. At the expense of GOSAT's fast time series capability (3-day repeat cycle, vs. 16 for OCO-2), its 8-footprint continuous swath can slice

  1. Evaluation of CO2 Sorption Capacity of Granite for CO2 Geological Sequestration

    NASA Astrophysics Data System (ADS)

    Fujii, T.; Sato, Y.; Lin, H.; Sasaki, K.; Takahashi, T.; Inomata, H.; Hashida, T.

    2007-03-01

    Anthropogenic effects on climate can be mitigated through various measures. Among them being CO2 sequestration into geological reservoirs including deep saline aquifers, depleted oil/gas reservoirs and coal seams are interested in a powerful means for drastically reducing emissions of CO2. When CO2 would be injected into geological reservoir, it should be necessary to know the potential of CO2 storing into the reservoir. In this study, amount of CO2 sorption of granite was to evaluate experimentally at temperatures 50, 70, 100 and 200°C and pressure up to 20 MPa using a magnetic suspension balance (MSB), which allows to measure under supercritical condition. As a result, we confirmed that the granite have the potential of CO2 sorption. Sorption isotherms obtained from the MSB experiment showed that amount of CO2 sorption increased with the increasing pressure and decreased with the increasing temperature for all experimental conditions. Especially, amount of CO2 sorption at 50°C compared with that at other temperatures (70, 100 and 200°C) increased rapidly in the vicinity of the critical state. In addition, the granite showed a maximum of CO2 sorption into granite could reach up to about 1.0% by weight at 50°C and 14.4MPa. The present results may provide a fundamental knowledge for the development of CO2 geological sequestration technology.

  2. Primary, secondary, and tertiary amines for CO2 capture: designing for mesoporous CO2 adsorbents.

    PubMed

    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".

  3. Exercise carbon dioxide (CO2) retention with inhaled CO2 and breathing resistance.

    PubMed

    Shykoff, Barbara E; Warkander, Dan E

    2012-01-01

    Combined effects on respiratory minute ventilation (VE)--and thus, on end-tidal carbon dioxide partial pressure (P(ET)CO2)--of breathing resistance and elevated inspired carbon dioxide (CO2) had not been determined during heavy exercise. In this Institutional Review Board-approved, dry, sea-level study, 12 subjects in each of three phases exercised to exhaustion at 85% peak oxygen uptake while V(E) and P(ET)CO2 were measured. Participants inhaled 0%, 1%, 2% or 3% CO2 in air, or 0% or 2% CO2 in oxygen, with or without breathing resistance, mimicking the U.S. Navy's MK 16 rebreather underwater breathing apparatus (UBA). Compared to air baseline (0% inspired CO2 in air without resistance): (1) Oxygen decreased baseline V(E) (p < 0.01); (2) Inspired CO2 increased V(E) and P(ET)CO2 (p < 0.01); (3) Resistance decreased V(E) (p < 0.01); (4) Inspired CO2 with resistance elevated P(ET)CO2 (p < 0.01). In air, V(E) did not change from that with resistance alone. In oxygen, V(E) returned to oxygen baseline. End-exercise P(ET)CO2 exceeded 60 Torr (8.0 kPa) in three tests. Subjects identified hypercapnia poorly. Results support dual optimization of arterial carbon dioxide partial pressure and respiratory effort. Because elevated CO2 may not increase V(E) if breathing resistance and VE are high, rebreather UBA safety requires very low inspired CO2.

  4. 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.

  5. Thermal decomposition of dolomite under CO2-air atmosphere

    NASA Astrophysics Data System (ADS)

    Subagjo, Wulandari, Winny; Adinata, Pratitis Mega; Fajrin, Anita

    2017-01-01

    This paper reports a study on thermal decomposition of dolomite under CO2-air. Calcination was carried out non-isothermally by using thermogravimetry analysis-differential scanning calorimetry (TGA-DSC) with a heating rate of 10°C/minute in an air atmosphere as well as 10 vol% CO2 and 90 vol% air atmosphere from 25 to 950°C. In addition, a thermodynamic modeling was also carried out to simulate dolomite calcination in different level of CO2-air atmosphere by using FactSage® 7.0. The the main constituents of typical dolomite from Gresik, East Java include MgCO3 (magnesite), CaCO3 (calcite), Ca(OH)2, CaO, MgO, and less than 1% of metal impurities. Based on the kinetics analysis from TGA results, it is found that non-isothermal dolomite calcination in 10 vol% CO2 atmosphere is occurred in a two-stage reaction; the first stage is the decomposition of magnesite at 650-740 °C with activation energy of 161.23 kJ/mol, and the second stage is the decomposition of calcite at 775-820 °C with activation energy of 162.46 kJ/mol. The magnesite decomposition is found to follow nucleation reaction mechanism of Avrami Eroveyef (A3), while calcite decomposition follows second order chemical reaction equation. Thermodynamic modeling supports these kinetic analyses. The results of this research give insight to the kinetics of dolomite decomposition in CO2-air atmosphere.

  6. Continuously Regenerable Freeze-Out CO2 Control Technology

    NASA Technical Reports Server (NTRS)

    Fricker, John; Dyer, Chris; Myers, Jeff; Patten, Rich; Paul, Heather

    2007-01-01

    Carbon dioxide (CO2) removal technology development for portable life support systems (PLSS) has traditionally concentrated in the areas of solid and liquid chemical sorbents and semi-permeable membranes. Most of these systems are too heavy in gravity environments, require prohibitive amounts of consumables for operation on long term planetary missions, or are inoperable on the surface of Mars due to the presence of a CO2 atmosphere. This paper describes the effort performed to mature an innovative CO2 removal technology that meets NASA s planetary mission needs while adhering to the important guiding principles of simplicity, reliability, and operability. A breadboard cryogenic carbon dioxide scrubber (Cryo Scrubber) for a closed loop cryogenic PLSS was developed, designed, and tested, and a conceptual design suitable for a PLSS was developed based on the results of the breadboard testing. The Cryo Scrubber freezes CO2 and other trace contaminants out of expired vent loop gas using cooling available from a liquid oxygen (LOX) based PLSS. The device is continuously regenerable, with solid CO2 being removed from the cold freeze-out surfaces, sublimated, and vented overboard. Duration is limited only by the supply of LOX stored in the PLSS. Simplicity, reliability, and operability are universally important criteria for critical hardware on long duration Lunar or Mars missions. The Cryo Scrubber has no moving parts, requires no additional consumables, and uses no electrical power, contributing to its simplicity and reliability. It is easy to use; no operator action is required to prepare, use, or shut down the Cryo Scrubber, and it does not require charging or regeneration. The versatility of the concept allows for operation on earth, the moon, and Mars, and in microgravity.

  7. Photolytic production of CO2 on Iapetus

    NASA Astrophysics Data System (ADS)

    Palmer, Eric; Brown, R. H.

    2008-09-01

    Carbon Dioxide has been detected on the surface of Iapetus by Cassini's VIMS instrument at the 4.26 micron band. This CO2 is concentrated on the equatorial leading side, where we also see an abundance of dark material. The residence time of free CO2 on the surface of Iapetus is very short, thus the CO2 is unlikely to be in the form of frost; it is more likely that the CO2 is tightly bound in the form of complexed molecules. We explore the possibility of photolytically generating CO2 from a mixture of the carbon rich material and water ice that matches the expected composition of the dark material on Iapetus' surface. An ice regolith was created with flash frozen water that was crushed into sub-millimeter shards and mixed with amorphous 13C. The regolith was placed in a vacuum chamber with a surface area of 10 cm2 and a thickness of 2 cm and exposed to UV light from a deuterium lamp with peaks of flux centered around 121 and 160 nm. Temperatures were varied between 60 and 130K at a pressure of 10-8 torr. Both CO and CO2 were produced by photolytic reactions and detected by a mass spectrometer. Applying these results to Iapetus, Jeans escape calculations show that CO2 generated by photolysis will remain gravitationally bound to Iapetus for between 100 and 200 years, ballistically scattering across the surface until it is sequestered in a polar cold trap or escapes to space. The average particle will interact with the surface more than 1000 times before escaping unless interactions with surface grains causes it to become complexed, such as adsorption. We are continuing to evaluate the photochemistry for this simulated Iapetus surface using a Nicolet IR spectrometer to identify all the products generated and estimate the associated production rate.

  8. Advanced CO2 Removal Technology Development

    NASA Technical Reports Server (NTRS)

    Finn, John E.; Verma, Sunita; Forrest, Kindall; LeVan, M. Douglas

    2001-01-01

    The Advanced CO2 Removal Technical Task Agreement covers three active areas of research and development. These include a study of the economic viability of a hybrid membrane/adsorption CO2 removal system, sorbent materials development, and construction of a database of adsorption properties of important fixed gases on several adsorbent material that may be used in CO2 removal systems. The membrane/adsorption CO2 removal system was proposed as a possible way to reduce the energy consumption of the four-bed molecular sieve system now in use. Much of the energy used by the 4BMS is used to desorb water removed in the device s desiccant beds. These beds might be replaced by a desiccating membrane that moves the water from [he incoming stream directly into the outlet stream. The approach may allow the CO2 removal beds to operate at a lower temperature. A comparison between models of the 4BMS and hybrid systems is underway at Vanderbilt University. NASA Ames Research Center has been investigating a Ag-exchanged zeolites as a possible improvement over currently used Ca and Na zeolites for CO2 removal. Silver ions will complex with n:-bonds in hydrocarbons such as ethylene, giving remarkably improved selectivity for adsorption of those materials. Bonds with n: character are also present in carbon oxides. NASA Ames is also continuing to build a database for adsorption isotherms of CO2, N2, O2, CH4, and Ar on a variety of sorbents. This information is useful for analysis of existing hardware and design of new processes.

  9. Kinetics of CO2 Reduction over Nonstoichiometric Ceria

    PubMed Central

    2015-01-01

    The kinetics of CO2 reduction over nonstoichimetric ceria, CeO2−δ, a material of high potential for thermochemical conversion of sunlight to fuel, has been investigated for a wide range of nonstoichiometries (0.02 ≤ δ ≤ 0.25), temperatures (693 ≤ T ≤ 1273 K), and CO2 concentrations (0.005 ≤ pCO2 ≤ 0.4 atm). Samples were reduced thermally at 1773 K to probe low nonstoichiometries (δ < 0.05) and chemically at lower temperatures in a H2 atmosphere to prevent particle sintering and probe the effect of higher nonstoichiometries (δ < 0.25). For extents greater than δ = 0.2, oxidation rates at a given nonstoichiometry are hindered for the duration of the reaction, presumably because of near-order changes, such as lattice compression, as confirmed via Raman Spectroscopy. Importantly, this behavior is reversible and oxidation rates are not affected at lower δ. Following thermal reduction at very low δ, however, oxidation rates are an order of magnitude slower than those of chemically reduced samples, and rates monotonically increase with the initial nonstoichiometry (up to δ = 0.05). This dependence may be attributed to the formation of stable defect complexes formed between oxygen vacancies and polarons. When the same experiments are performed with 10 mol % Gd3+ doped ceria, in which defect complexes are less prevalent than in pure ceria, this dependence is not observed. PMID:26693270

  10. Carbon Dioxide Clusters: (CO_2)_6 to (CO_2)13

    NASA Astrophysics Data System (ADS)

    McKellar, A. R. W.; Oliaee, J. Norooz; Dehghany, M.; Moazzen-Ahmadi, N.

    2011-06-01

    We recenty reported assignments of specific infrared bands in the CO_2 νb{3} region (˜2350 wn) to (CO_2)_6, (CO_2)_7, (CO_2)_9, (CO_2)10, (CO_2)11, (CO_2)12, and (CO_2)13. Spectra are obtained by direct absorption using a rapid-scan tuneable diode laser spectrometer to probe a pulsed supersonic slit-jet expansion and assignments are facilitated by recent calculations of Takeuchi based on the Murthy potential. (CO_2)_6 is a symmetric top with S_6 point group symmetry which can be thought of as a stack of two planar cyclic trimers. (CO_2)13 is also an S_6 symmetric top, and consists of a single CO_2 monomer surrounded by an slightly distorted icosahedral cage. The remaining clusters are asymmetric tops without symmetry. Here we report additional CO_2 cluster results. Calculations based on the SAPT-s potential indicate that the structure of (CO_2)10 may be slightly different from that given by Takeuchi/Murthy. An additional band is observed for each of (CO_2)13 and (CO_2)10. A feature observed at 2378.2 wn is assigned as a (CO_2)_6 parallel combination band involving the sum of a fundamental and a low-lying intermolecular vibration. Most significantly, two bands are assigned to a second isomer of (CO_2)_6. This is also a symmetric top, but now with S_4 symmetry. The two symmetric hexamer isomers observed spectroscopically correspond well with the lowest energy structures given by both the SAPT-s and Murthy intermolecular potentials. [1] J. Norooz Oliaee, M. Dehgany, N. Moazzen-Ahmadi, and A.R.W. McKellar, Phys. Chem. Chem. Phys. 13, 1297 (2011). [2] H. Takeuchi, J. Phys. Chem. A 107, 5703 (2008); C.S. Murthy, S.F. O'Shea, and I.R. McDonald, Mol. Phys. 50, 531 (1983). [3] R. Bukowski, J. Sadlej, B. Jeziorski, P. Jankowski, K. Szalewicz, S.A. Kucharski, H.L. Williams, and B.M. Rice, J. Chem. Phys. 110, 3785 (1999)

  11. CO2 sensing and CO2 regulation of stomatal conductance: advances and open questions

    PubMed Central

    Engineer, Cawas; Hashimoto-Sugimoto, Mimi; Negi, Juntaro; Israelsson-Nordstrom, Maria; Azoulay-Shemer, Tamar; Rappel, Wouter-Jan; Iba, Koh; Schroeder, Julian

    2015-01-01

    Guard cells form epidermal stomatal gas exchange valves in plants and regulate the aperture of stomatal pores in response to changes in the carbon dioxide (CO2) concentration in leaves. Moreover, the development of stomata is repressed by elevated CO2 in diverse plant species. Evidence suggests that plants can sense CO2 concentration changes via guard cells and via mesophyll tissues in mediating stomatal movements. We review new discoveries and open questions on mechanisms mediating CO2-regulated stomatal movements and CO2 modulation of stomatal development, which together function in CO2-regulation of stomatal conductance and gas exchange in plants. Research in this area is timely in light of the necessity of selecting and developing crop cultivars which perform better in a shifting climate. PMID:26482956

  12. CO2 and CO Simulations and Their Source Signature Indicated by CO/CO2

    NASA Technical Reports Server (NTRS)

    Kawa, Randy; Huisheng, Bian

    2004-01-01

    Three years (2000-2002) atmospheric CO2 and CO fields are simulated by a Chemistry Transport Model driven by the assimilated meteorological fields from GEOS-4. The simulated CO2 and CO are evaluated by measurements from surface (CMDL), satellite (MOPITT/CO), and aircraft. The model-observation comparisons indicate reasonable agreement in both source and remote regions, and in the lower and upper troposphere. The simulation also captures the seasonality of CO2 and CO variations. The ratios of CO/CO2 are analyzed over different representative regions to identify the source signature, since the anthropogenic CO comes fiom the same combustion processes as CO2. This work enables us to improve satellite inversion estimates of CO2 sources and sinks by simultaneously using satellite CO measurement.

  13. The Effect of Excess Electron and hole on CO2 Adsorption and Activation on Rutile (110) surface

    PubMed Central

    Yin, Wen-Jin; Wen, Bo; Bandaru, Sateesh; Krack, Matthias; Lau, MW; Liu, Li-Min

    2016-01-01

    CO2 capture and conversion into useful chemical fuel attracts great attention from many different fields. In the reduction process, excess electron is of key importance as it participates in the reaction, thus it is essential to know whether the excess electrons or holes affect the CO2 conversion. Here, the first-principles calculations were carried out to explore the role of excess electron on adsorption and activation of CO2 on rutile (110) surface. The calculated results demonstrate that CO2 can be activated as CO2 anions or CO2 cation when the system contains excess electrons and holes. The electronic structure of the activated CO2 is greatly changed, and the lowest unoccupied molecular orbital of CO2 can be even lower than the conduction band minimum of TiO2, which greatly facilities the CO2 reduction. Meanwhile, the dissociation process of CO2 undergoes an activated CO2− anion in bend configuration rather than the linear, while the long crossing distance of proton transfer greatly hinders the photocatalytic reduction of CO2 on the rutile (110) surface. These results show the importance of the excess electrons on the CO2 reduction process. PMID:26984417

  14. The Effect of Excess Electron and hole on CO2 Adsorption and Activation on Rutile (110) surface.

    PubMed

    Yin, Wen-Jin; Wen, Bo; Bandaru, Sateesh; Krack, Matthias; Lau, M W; Liu, Li-Min

    2016-03-17

    CO2 capture and conversion into useful chemical fuel attracts great attention from many different fields. In the reduction process, excess electron is of key importance as it participates in the reaction, thus it is essential to know whether the excess electrons or holes affect the CO2 conversion. Here, the first-principles calculations were carried out to explore the role of excess electron on adsorption and activation of CO2 on rutile (110) surface. The calculated results demonstrate that CO2 can be activated as CO2 anions or CO2 cation when the system contains excess electrons and holes. The electronic structure of the activated CO2 is greatly changed, and the lowest unoccupied molecular orbital of CO2 can be even lower than the conduction band minimum of TiO2, which greatly facilities the CO2 reduction. Meanwhile, the dissociation process of CO2 undergoes an activated CO2(-) anion in bend configuration rather than the linear, while the long crossing distance of proton transfer greatly hinders the photocatalytic reduction of CO2 on the rutile (110) surface. These results show the importance of the excess electrons on the CO2 reduction process.

  15. Monitoring of near surface CO2

    NASA Astrophysics Data System (ADS)

    Faber, E.; Möller, I.; Teschner, M.; Poggenburg, J.; Spickenbom, K.; Schulz, H. J.

    2009-04-01

    Monitoring of near surface CO2 ECKHARD FABER1, INGO MÖLLER1, MANFRED TESCHNER1, JÜRGEN POGGENBURG1, KAI SPICKENBOM1, HANS-MARTIN SCHULZ1,2 1Bundesanstalt für Geowissenschaften und Rohstoffe (BGR), Stilleweg 2, D-30655 Hannover, e.faber@bgr.de 2present adress: GeoForschungsZentrum Potsdam (GFZ), Telegrafenberg, D-14473 Potsdam Underground gas storage and sequestration of carbon dioxide is one of the methods to reduce the input of antropogenic CO2 into the atmosphere and its greenhouse effect. Storage of CO2 is planned in depleted reservoirs, in aquifers and in salt caverns. Storage sites must have very small leakage rates to safely store the CO2 for centuries. Thus, a careful investigation and site selection is crucial. However, any leakage of CO2 to the surface is potentially dangerous for humans and environment. Therefore, instruments and systems for the detection of any CO2 escaping the storage sites and reaching the atmosphere have to be developed. Systems to monitor gases in deep wells, groundwater and surface sediments for leaking CO2 are developed, tested and are contnuously improved. Our group is mainly analysing CO2 in shallow (down to 3 m) soil samples using automatically operating monitoring systems. The systems are equipped with sensors to measure CO2 (and other gases) concentrations and other environmental parameters (atmospheric pressure, ambient and soil temperatures, etc.). Data are measured in short intervals (minute to subminute), are stored locally and are transferred by telemetrical systems into the BGR laboratory (Weinlich et al., 2006). In addition to soil gases monitoring systems technical equipment is available for continuous underwater gas flow measurements. Several of those monitoring systems are installed in different areas like Czech Republic, Austria, Italy and Germany. To detect any leaking gas from a sequestration site after CO2 injection, the naturally existing CO2 concentration (before injection) must be known. Thus, the natural

  16. Validation of Airborne CO2 Laser Measurements

    NASA Astrophysics Data System (ADS)

    Browell, E. V.; Dobler, J. T.; Kooi, S.; Fenn, M. A.; Choi, Y.; Vay, S. A.; Harrison, F. W.; Moore, B.; Zaccheo, T. S.

    2010-12-01

    This paper discusses the flight test validation of a unique, multi-frequency, intensity-modulated, single-beam laser absorption spectrometer (LAS) that operates near 1.57 μm for remote column CO2 measurements. This laser system is under development for a future space-based mission to determine the global distribution of regional-scale CO2 sources and sinks, which is the objective of the NASA Active Sensing of CO2 Emissions during Nights, Days, and Seasons (ASCENDS) mission. A prototype of this LAS system, called the Multi-frequency Fiber Laser Lidar (MFLL), was developed by ITT, and it has been flight tested in nine airborne campaigns since May 2005. This paper focuses on the most recent results obtained over the last two years of flight-testing where the MFLL remote CO2 column measurements were evaluated against airborne in situ CO2 profile measurements traceable to World Meteorological Organization standards. A comprehensive multiple-aircraft flight test program was conducted over Oklahoma and Virginia in July-August 2009. The MFLL obtained surface reflectance and average CO2 column variations along the 50-km flight legs over the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Central Facility (CF) in Lamont, Oklahoma; over rural Virginia and North Carolina; and over the Chesapeake Bay. For a flight altitude of 4.6 km, the average signal to noise ratio (SNR) for a 1-s CO2 column measurement was found to be 760, which is the equivalent of a CO2 mixing ratio precision of 0.60 ppmv, and for a 10-s average the SNR was found to be 2002 or 0.20 ppmv. Absolute comparisons of MFLL-derived and in situ-derived CO2 column measurements were made for all daytime flights conducted over Oklahoma and Virginia with an average agreement to within 0.32 ppmv. A major ASCENDS flight test campaign was conducted using the NASA DC-8 during 6-18 July 2010. The MFLL system and associated in situ CO2 instrumentation were operated on DC-8 flights over the Central Valley

  17. On CO2 Behavior in the Subsurface, Following Leakage from aGeologic Storage Reservoir

    SciTech Connect

    Pruess, Karsten

    2006-02-09

    and demonstrate that CO2 can be injected and stored safely ingeologic formations. This requires an understanding of the risks andhazards associated with geologic storage, and a demonstration that therisks are acceptably small or can be mitigated. Much work is currentlyunderway to develop comprehensive approaches towards risk assessment froma systems analysis perspective, which in general requires a simplifieddescription of physical and chemical processes (Maul, et al., 2004,Espie, 2004; Wildenborg, et al., 2004; Walton, et al., 2004). This typeof approach is very important, but needs to be complemented withdevelopment of an understanding of the physical and chemical processesassociated with CO2 storage and leakage (Evans, et al.,2004).

  18. Engineering cyanobacteria for direct biofuel production from CO2.

    PubMed

    Savakis, Philipp; Hellingwerf, Klaas J

    2015-06-01

    For a sustainable future of our society it is essential to close the global carbon cycle. Oxidised forms of carbon, in particular CO2, can be used to synthesise energy-rich organic molecules. Engineered cyanobacteria have attracted attention as catalysts for the direct conversion of CO2 into reduced fuel compounds. Proof of principle for this approach has been provided for a vast range of commodity chemicals, mostly energy carriers, such as short chain and medium chain alcohols. More recently, research has focused on the photosynthetic production of compounds with higher added value, most notably terpenoids. Below we review the recent developments that have improved the state-of-the-art of this approach and speculate on future developments.

  19. Direct Copolymerization of CO2 and Diols

    NASA Astrophysics Data System (ADS)

    Tamura, Masazumi; Ito, Kazuki; Honda, Masayoshi; Nakagawa, Yoshinao; Sugimoto, Hiroshi; Tomishige, Keiichi

    2016-04-01

    Direct polymerization of CO2 and diols is promising as a simple and environmental-benign method in place of conventional processes using high-cost and/or hazardous reagents such as phosgene, carbon monoxide and epoxides, however, there are no reports on the direct method due to the inertness of CO2 and severe equilibrium limitation of the reaction. Herein, we firstly substantiate the direct copolymerization of CO2 and diols using CeO2 catalyst and 2-cyanopyridine promotor, providing the alternating cooligomers in high diol-based yield (up to 99%) and selectivity (up to >99%). This catalyst system is applicable to various diols including linear C4-C10 α,ω-diols to provide high yields of the corresponding cooligomers, which cannot be obtained by well-known methods such as copolymerization of CO2 and cyclic ethers and ring-opening polymerization of cyclic carbonates. This process provides us a facile synthesis method for versatile polycarbonates from various diols and CO2 owing to simplicity of diols modification.

  20. Direct Copolymerization of CO2 and Diols

    PubMed Central

    Tamura, Masazumi; Ito, Kazuki; Honda, Masayoshi; Nakagawa, Yoshinao; Sugimoto, Hiroshi; Tomishige, Keiichi

    2016-01-01

    Direct polymerization of CO2 and diols is promising as a simple and environmental-benign method in place of conventional processes using high-cost and/or hazardous reagents such as phosgene, carbon monoxide and epoxides, however, there are no reports on the direct method due to the inertness of CO2 and severe equilibrium limitation of the reaction. Herein, we firstly substantiate the direct copolymerization of CO2 and diols using CeO2 catalyst and 2-cyanopyridine promotor, providing the alternating cooligomers in high diol-based yield (up to 99%) and selectivity (up to >99%). This catalyst system is applicable to various diols including linear C4-C10 α,ω-diols to provide high yields of the corresponding cooligomers, which cannot be obtained by well-known methods such as copolymerization of CO2 and cyclic ethers and ring-opening polymerization of cyclic carbonates. This process provides us a facile synthesis method for versatile polycarbonates from various diols and CO2 owing to simplicity of diols modification. PMID:27075987

  1. The supply chain of CO2 emissions.

    PubMed

    Davis, Steven J; Peters, Glen P; Caldeira, Ken

    2011-11-08

    CO(2) emissions from the burning of fossil fuels are conventionally attributed to the country where the emissions are produced (i.e., where the fuels are burned). However, these production-based accounts represent a single point in the value chain of fossil fuels, which may have been extracted elsewhere and may be used to provide goods or services to consumers elsewhere. We present a consistent set of carbon inventories that spans the full supply chain of global CO(2) emissions, finding that 10.2 billion tons CO(2) or 37% of global emissions are from fossil fuels traded internationally and an additional 6.4 billion tons CO(2) or 23% of global emissions are embodied in traded goods. Our results reveal vulnerabilities and benefits related to current patterns of energy use that are relevant to climate and energy policy. In particular, if a consistent and unavoidable price were imposed on CO(2) emissions somewhere along the supply chain, then all of the parties along the supply chain would seek to impose that price to generate revenue from taxes collected or permits sold. The geographical concentration of carbon-based fuels and relatively small number of parties involved in extracting and refining those fuels suggest that regulation at the wellhead, mine mouth, or refinery might minimize transaction costs as well as opportunities for leakage.

  2. CO2 DIAL measurements of water vapor

    NASA Technical Reports Server (NTRS)

    Grant, William B.; Margolis, Jack S.; Brothers, Alan M.; Tratt, David M.

    1987-01-01

    CO2 lidars have heretofore been used to measure water vapor concentrations primarily using the 10R(20) line at 10.247 microns, which has a strong overlap with a water vapor absorption line. This paper discusses the use of that line as well as other CO2 laser lines for which the absorption coefficients are weaker. The literature on measurement of water vapor absorption coefficients using CO2 lasers is reviewed, and the results from four laboratories are shown to be generally consistent with each other after they are normalized to the same partial pressure, temperature, and ethylene absorption coefficent for the 10P(14) CO2 laser line; however, the agreement with the Air Force Geophysics Laboratory's HITRAN and FASCOD 2 spectral data tapes is not good either for the water vapor absorption lines or for the water vapor continuum. Demonstration measurements of atmospheric water vapor have been conducted using the Mobile Atmospheric Pollutant Mapping System, a dual CO2 lidar system using heterodyne detection. Results are discussed for measurements using three sets of laser line pairs covering a wide range of water vapor partial pressures.

  3. The supply chain of CO2 emissions

    PubMed Central

    Davis, Steven J.; Peters, Glen P.; Caldeira, Ken

    2011-01-01

    CO2 emissions from the burning of fossil fuels are conventionally attributed to the country where the emissions are produced (i.e., where the fuels are burned). However, these production-based accounts represent a single point in the value chain of fossil fuels, which may have been extracted elsewhere and may be used to provide goods or services to consumers elsewhere. We present a consistent set of carbon inventories that spans the full supply chain of global CO2 emissions, finding that 10.2 billion tons CO2 or 37% of global emissions are from fossil fuels traded internationally and an additional 6.4 billion tons CO2 or 23% of global emissions are embodied in traded goods. Our results reveal vulnerabilities and benefits related to current patterns of energy use that are relevant to climate and energy policy. In particular, if a consistent and unavoidable price were imposed on CO2 emissions somewhere along the supply chain, then all of the parties along the supply chain would seek to impose that price to generate revenue from taxes collected or permits sold. The geographical concentration of carbon-based fuels and relatively small number of parties involved in extracting and refining those fuels suggest that regulation at the wellhead, mine mouth, or refinery might minimize transaction costs as well as opportunities for leakage. PMID:22006314

  4. Development of new measuring technique using sound velocity for CO2 concentration in Cameroonian volcanic lakes

    NASA Astrophysics Data System (ADS)

    Sanemasa, M.; Saiki, K.; Kaneko, K.; Ohba, T.; Kusakabe, M.; Tanyileke, G.; Hell, J.

    2012-12-01

    1. Introduction Limnic eruptions at Lakes Monoun and Nyos in Cameroon, which are sudden degassing of magmatic CO2 dissolved in the lake water, occurred in 1984 and 1986, respectively. The disasters killed about 1800 people around the lakes. Because of ongoing CO2 accumulation in the bottom water of the lakes, tragedy of limnic eruptions will possibly occur again. To prevent from further disasters, artificial degassing of CO2 from the lake waters has been undergoing. Additionally, CO2 monitoring of the lake waters is needed. Nevertheless, CO2 measurement is done only once or twice a year because current methods of CO2 measurement, which require chemical analysis of water samples, are not suitable for frequent measurement. In engineering field, on the other hand, a method to measure salt concentration using sound velocity has been proposed (Kleis and Sanchez, 1990). This method allows us to evaluate solute concentration fast. We applied the method to dissolved CO2 and examined the correlation between sound velocity and CO2 concentration in laboratory experiment. Furthermore, using the obtained correlation, we tried to estimate the CO2 concentration of waters in the Cameroonian lakes. 2. Laboratory experiment We examined the correlation between sound velocity and CO2 concentration. A profiler (Minos X, made by AML oceanography) and pure water were packed in cylindrical stainless vessel and high-pressure CO2 gas was injected to produce carbonated water. The profiler recorded temperature, pressure and sound velocity. Change of sound velocity was defined as difference of sound velocity between carbonated water and pure water under the same temperature and pressure conditions. CO2 concentration was calculated by Henry's law. The result indicated that the change of sound velocity [m s-1] is proportional to CO2 concentration [mmol kg-1], and the coefficient is 0.021 [m kg s-1 mmol-1]. 3. Field application Depth profiles of sound velocity, pressure, and temperature of Lakes

  5. pCO2 and CO2 Exchange During High Bora Winds in the Northern Adriatic

    DTIC Science & Technology

    2013-03-05

    coastal ocean , has not been adequately assessed. Here we show the response of surfacewater pCO2 and CO2 fluxes during high borawind in the Northern...m−2 day−1 day in thewinter cases and 29 mmol m−2 day−1 in the summer case) over themag- nitude of the mean annual value. Oceanic data measured...simultaneously to surface pCO2 measurements suggest that themost likely responsiblemechanisms for the observed pCO2 increaseswere oceanic verticalmixing and

  6. Light-duty vehicle CO2 targets consistent with 450 ppm CO2 stabilization.

    PubMed

    Winkler, Sandra L; Wallington, Timothy J; Maas, Heiko; Hass, Heinz

    2014-06-03

    We present a global analysis of CO2 emission reductions from the light-duty vehicle (LDV) fleet consistent with stabilization of atmospheric CO2 concentration at 450 ppm. The CO2 emission reductions are described by g CO2/km emission targets for average new light-duty vehicles on a tank-to-wheel basis between 2010 and 2050 that we call CO2 glide paths. The analysis accounts for growth of the vehicle fleet, changing patterns in driving distance, regional availability of biofuels, and the changing composition of fossil fuels. New light-duty vehicle fuel economy and CO2 regulations in the U.S. through 2025 and in the EU through 2020 are broadly consistent with the CO2 glide paths. The glide path is at the upper end of the discussed 2025 EU range of 68-78 g CO2/km. The proposed China regulation for 2020 is more stringent than the glide path, while the 2017 Brazil regulation is less stringent. Existing regulations through 2025 are broadly consistent with the light-duty vehicle sector contributing to stabilizing CO2 at approximately 450 ppm. The glide paths provide long-term guidance for LDV powertrain/fuel development.

  7. CO2-Binding-Organic-Liquids-Enhanced CO2 Capture using Polarity-Swing-Assisted Regeneration

    SciTech Connect

    Zhang, Jian; Kutnyakov, Igor; Koech, Phillip K.; Zwoster, Andy; Howard, Chris; Zheng, Feng; Freeman, Charles J.; Heldebrant, David J.

    2013-01-01

    A new solvent-based CO2 capture process couples the unique attributes of non-aqueous, CO2-binding organic liquids (CO2BOLs) with the newly discovered polarity-swing-assisted regeneration (PSAR) process that is unique to switchable ionic liquids. Laboratory measurements with PSAR indicate the ability to achieve a regeneration effect at 75°C comparable to that at 120°C using thermal regeneration only. Initial measurements also indicate that the kinetic behavior of CO2 release is also improved with PSAR. Abstract cleared PNWD-SA-9743

  8. Behavior of CO2/water flow in porous media for CO2 geological storage.

    PubMed

    Jiang, Lanlan; Yu, Minghao; Liu, Yu; Yang, Mingjun; Zhang, Yi; Xue, Ziqiu; Suekane, Tetsuya; Song, Yongchen

    2017-04-01

    A clear understanding of two-phase fluid flow properties in porous media is of importance to CO2 geological storage. The study visually measured the immiscible and miscible displacement of water by CO2 using MRI (magnetic resonance imaging), and investigated the factor influencing the displacement process in porous media which were filled with quartz glass beads. For immiscible displacement at slow flow rates, the MR signal intensity of images increased because of CO2 dissolution; before the dissolution phenomenon became inconspicuous at flow rate of 0.8mLmin(-1). For miscible displacement, the MR signal intensity decreased gradually independent of flow rates, because supercritical CO2 and water became miscible in the beginning of CO2 injection. CO2 channeling or fingering phenomena were more obviously observed with lower permeable porous media. Capillary force decreases with increasing particle size, which would increase permeability and allow CO2 and water to invade into small pore spaces more easily. The study also showed CO2 flow patterns were dominated by dimensionless capillary number, changing from capillary finger to stable flow. The relative permeability curve was calculated using Brooks-Corey model, while the results showed the relative permeability of CO2 slightly decreases with the increase of capillary number.

  9. Metal-CO2 Batteries on the Road: CO2 from Contamination Gas to Energy Source.

    PubMed

    Xie, Zhaojun; Zhang, Xin; Zhang, Zhang; Zhou, Zhen

    2017-04-01

    Rechargeable nonaqueous metal-air batteries attract much attention for their high theoretical energy density, especially in the last decade. However, most reported metal-air batteries are actually operated in a pure O2 atmosphere, while CO2 and moisture in ambient air can significantly impact the electrochemical performance of metal-O2 batteries. In the study of CO2 contamination on metal-O2 batteries, it has been gradually found that CO2 can be utilized as the reactant gas alone; namely, metal-CO2 batteries can work. On the other hand, investigations on CO2 fixation are in focus due to the potential threat of CO2 on global climate change, especially for its steadily increasing concentration in the atmosphere. The exploitation of CO2 in energy storage systems represents an alternative approach towards clean recycling and utilization of CO2 . Here, the aim is to provide a timely summary of recent achievements in metal-CO2 batteries, and inspire new ideas for new energy storage systems. Moreover, critical issues associated with reaction mechanisms and potential directions for future studies are discussed.

  10. The Abundance of Atmospheric CO2 in Ocean Exoplanets: a Novel CO2 Deposition Mechanism

    NASA Astrophysics Data System (ADS)

    Levi, A.; Sasselov, D.; Podolak, M.

    2017-03-01

    We consider super-Earth sized planets which have a water mass fraction large enough to form an external mantle composed of high-pressure water-ice polymorphs and also lack a substantial H/He atmosphere. We consider such planets in their habitable zone, so that their outermost condensed mantle is a global, deep, liquid ocean. For these ocean planets, we investigate potential internal reservoirs of CO2, the amount of CO2 dissolved in the ocean for the various saturation conditions encountered, and the ocean-atmosphere exchange flux of CO2. We find that, in a steady state, the abundance of CO2 in the atmosphere has two possible states. When wind-driven circulation is the dominant CO2 exchange mechanism, an atmosphere of tens of bars of CO2 results, where the exact value depends on the subtropical ocean surface temperature and the deep ocean temperature. When sea-ice formation, acting on these planets as a CO2 deposition mechanism, is the dominant exchange mechanism, an atmosphere of a few bars of CO2 is established. The exact value depends on the subpolar surface temperature. Our results suggest the possibility of a negative feedback mechanism, unique to water planets, where a reduction in the subpolar temperature drives more CO2 into the atmosphere to increase the greenhouse effect.

  11. Sensitivity analysis of a model of CO2 exchange in tundra ecosystems by the adjoint method

    SciTech Connect

    Waelbroek, C.; Louis, J.F. |

    1995-02-01

    A model of net primary production (NPP), decomposition, and nitrogen cycling in tundra ecosystems has been developed. The adjoint technique is used to study the sensitivity of the computed annual net CO2 flux to perturbation in initial conditions, climatic inputs, and model`s main parameters describing current seasonal CO2 exchange in wet sedge tundra at Barrow, Alaska. The results show that net CO2 flux is most sensitive to parameters characterizing litter chemical composition and more sensitive to decomposition parameters than to NPP parameters. This underlines the fact that in nutrient-limited ecosystems, decomposition drives net CO2 exchange by controlling mineralization of main nutrients. The results also indicate that the short-term (1 year) response of wet sedge tundra to CO2-induced warming is a significant increase in CO2 emission, creating a positive feedback to atmosphreic CO2 accumulation. However, a cloudiness increase during the same year can severely alter this response and lead to either a slight decrease or a strong increase in emitted CO2, depending on its exact timing. These results demonstrate that the adjoint method is well suited to study systems encountering regime changes, as a single run of the adjoint model provides sensitivities of the net CO2 flux to perturbations in all parameters and variables at any time of the year. Moreover, it is shown that large errors due to the presence of thresholds can be avoided by first delimiting the range of applicability of the adjoint results.

  12. Effects of elevated CO2 on fish behaviour undiminished by transgenerational acclimation

    NASA Astrophysics Data System (ADS)

    Welch, Megan J.; Watson, Sue-Ann; Welsh, Justin Q.; McCormick, Mark I.; Munday, Philip L.

    2014-12-01

    Behaviour and sensory performance of marine fishes are impaired at CO2 levels projected to occur in the ocean in the next 50-100 years, and there is limited potential for within-generation acclimation to elevated CO2 (refs , ). However, whether fish behaviour can acclimate or adapt to elevated CO2 over multiple generations remains unanswered. We tested for transgenerational acclimation of reef fish olfactory preferences and behavioural lateralization at moderate (656 μatm) and high (912 μatm) end-of-century CO2 projections. Juvenile spiny damselfish, Acanthochromis polyacanthus, from control parents (446 μatm) exhibited an innate avoidance to chemical alarm cue (CAC) when reared in control conditions. In contrast, juveniles lost their innate avoidance of CAC and even became strongly attracted to CAC when reared at elevated CO2 levels. Juveniles from parents maintained at mid-CO2 and high-CO2 levels also lost their innate avoidance of CAC when reared in elevated CO2, demonstrating no capacity for transgenerational acclimation of olfactory responses. Behavioural lateralization was also disrupted for juveniles reared under elevated CO2, regardless of parental conditioning. Our results show minimal potential for transgenerational acclimation in this fish, suggesting that genetic adaptation will be necessary to overcome the effects of ocean acidification on behaviour.

  13. Sensitivity analysis of a model of CO2 exchange in tundra ecosystems by the adjoint method

    NASA Technical Reports Server (NTRS)

    Waelbroek, C.; Louis, J.-F.

    1995-01-01

    A model of net primary production (NPP), decomposition, and nitrogen cycling in tundra ecosystems has been developed. The adjoint technique is used to study the sensitivity of the computed annual net CO2 flux to perturbation in initial conditions, climatic inputs, and model's main parameters describing current seasonal CO2 exchange in wet sedge tundra at Barrow, Alaska. The results show that net CO2 flux is most sensitive to parameters characterizing litter chemical composition and more sensitive to decomposition parameters than to NPP parameters. This underlines the fact that in nutrient-limited ecosystems, decomposition drives net CO2 exchange by controlling mineralization of main nutrients. The results also indicate that the short-term (1 year) response of wet sedge tundra to CO2-induced warming is a significant increase in CO2 emission, creating a positive feedback to atmosphreic CO2 accumulation. However, a cloudiness increase during the same year can severely alter this response and lead to either a slight decrease or a strong increase in emitted CO2, depending on its exact timing. These results demonstrate that the adjoint method is well suited to study systems encountering regime changes, as a single run of the adjoint model provides sensitivities of the net CO2 flux to perturbations in all parameters and variables at any time of the year. Moreover, it is shown that large errors due to the presence of thresholds can be avoided by first delimiting the range of applicability of the adjoint results.

  14. Quantifying the loss of methane through secondary gas mass transport (or 'slip') from a micro-porous membrane contactor applied to biogas upgrading.

    PubMed

    McLeod, Andrew; Jefferson, Bruce; McAdam, Ewan J

    2013-07-01

    Secondary gas transport during the separation of a binary gas with a micro-porous hollow fibre membrane contactor (HMFC) has been studied for biogas upgrading. In this application, the loss or 'slip' of the secondary gas (methane) during separation is a known concern, specifically since methane possesses the intrinsic calorific value. Deionised (DI) water was initially used as the physical solvent. Under these conditions, carbon dioxide (CO2) and methane (CH4) absorption were dependent upon liquid velocity (V(L)). Whilst the highest CO2 flux was recorded at high V(L), selectivity towards CO2 declined due to low residence times and a diminished gas-side partial pressure, and resulted in slip of approximately 5.2% of the inlet methane. Sodium hydroxide was subsequently used as a comparative chemical absorption solvent. Under these conditions, CO2 mass transfer increased by increasing gas velocity (VG) which is attributed to the excess of reactive hydroxide ions present in the solvent, and the fast conversion of dissolved CO2 to carbonate species reinitiating the concentration gradient at the gas-liquid interface. At high gas velocities, CH4 slip was reduced to 0.1% under chemical conditions. Methane slip is therefore dependent upon whether the process is gas phase or liquid phase controlled, since methane mass transport can be adequately described by Henry's law within both physical and chemical solvents. The addition of an electrolyte was found to further retard CH4 absorption via the salting out effect. However, their applicability to physical solvents is limited since electrolytic concentration similarly impinges upon the solvents' capacity for CO2. This study illustrates the significance of secondary gas mass transport, and furthermore demonstrates that gas-phase controlled systems are recommended where greater selectivity is required.

  15. Development of a laser remote sensing instrument to measure sub-aerial volcanic CO2 fluxes

    NASA Astrophysics Data System (ADS)

    Queisser, Manuel; Burton, Mike

    2016-04-01

    A thorough quantification of volcanic CO2 fluxes would lead to an enhanced understanding of the role of volcanoes in the geological carbon cycle. This would enable a more subtle understanding of human impact on that cycle. Furthermore, variations in volcanic CO2 emissions are a key to understanding volcanic processes such as eruption phenomenology. However, measuring fluxes of volcanic CO2 is challenging as volcanic CO2 concentrations are modest compared with the ambient CO2 concentration (~400 ppm) . Volcanic CO2 quickly dilutes with the background air. For Mt. Etna (Italy), for instance, 1000 m downwind from the crater, dispersion modelling yields a signal of ~4 ppm only. It is for this reason that many magmatic CO2 concentration measurements focus on in situ techniques, such as direct sampling Giggenbach bottles, chemical sensors, IR absorption spectrometers or mass spectrometers. However, emission rates are highly variable in time and space. Point measurements fail to account for this variability. Inferring 1-D or 2-D gas concentration profiles, necessary to estimate gas fluxes, from point measurements may thus lead to erroneous flux estimations. Moreover, in situ probing is time consuming and, since many volcanoes emit toxic gases and are dangerous as mountains, may raise safety concerns. In addition, degassing is often diffuse and spatially extended, which makes a measurement approach with spatial coverage desirable. There are techniques that allow to indirectly retrieve CO2 fluxes from correlated SO2 concentrations and fluxes. However, they still rely on point measurements of CO2 and are prone to errors of SO2 fluxes due to light dilution and depend on blue sky conditions. Here, we present a new remote sensing instrument, developed with the ERC project CO2Volc, which measures 1-D column amounts of CO2 in the atmosphere with sufficient sensitivity to reveal the contribution of magmatic CO2. Based on differential absorption LIDAR (DIAL) the instrument measures

  16. Membraneless water filtration using CO2

    NASA Astrophysics Data System (ADS)

    Shin, Sangwoo; Shardt, Orest; Warren, Patrick; Stone, Howard

    2016-11-01

    Water purification technologies such as ultrafiltration and reverse osmosis utilize porous membranes to remove suspended particles and solutes. These membranes, however, cause many drawbacks such as a high pumping cost and a need for periodic replacement due to fouling. Here we show an alternative membraneless method for separating suspended particles by exposing the colloidal suspension to CO2. Dissolution of CO2 into the suspension creates solute gradients that drive phoretic motion of particles, or so-called diffusiophoresis. Due to the large diffusion potential built up by the dissociation of carbonic acid, colloidal particles move either away from or towards the gas-liquid interface depending on their surface charge. Our findings suggest a means to separate particles without membranes or filters, thus reducing operating and maintenance costs. Using the directed motion of particles induced by exposure to CO2, we demonstrate a scalable, continuous flow, membraneless particle filtration process that exhibits very low pressure drop and is essentially free from fouling.

  17. Sequestration of CO2 by concrete carbonation.

    PubMed

    Galan, Isabel; Andrade, Carmen; Mora, Pedro; Sanjuan, Miguel A

    2010-04-15

    Carbonation of reinforced concrete is one of the causes of corrosion, but it is also a way to sequester CO2. The characteristics of the concrete cover should ensure alkaline protection for the steel bars but should also be able to combine CO2 to a certain depth. This work attempts to advance the knowledge of the carbon footprint of cement. As it is one of the most commonly used materials worldwide, it is very important to assess its impact on the environment. In order to quantify the capacity of cement based materials to combine CO2 by means of the reaction with hydrated phases to produce calcium carbonate, Thermogravimetry and the phenolphthalein indicator have been used to characterize several cement pastes and concretes exposed to different environments. The combined effect of the main variables involved in this process is discussed. The moisture content of the concrete seems to be the most influential parameter.

  18. Geochemical Monitoring for Potential Environmental Impacts of Geologic Sequestration of CO2

    NASA Astrophysics Data System (ADS)

    Thomas, B.; Kharaka, Y. K.; Cole, D. R.; Thordsen, J. J.; Conaway, C. H.; Gans, K. D.

    2013-12-01

    Geologically sequestered CO2 is buoyant, has a low viscosity and, when dissolved in brine, becomes reactive to minerals, cements and well pipes. These properties of CO2 may cause it to leak upward from the major storage reservoirs, possibly contaminating underground sources of drinking water. We have participated in several multi-laboratory field experiments to investigate the changes in chemical and isotopic parameters and added tracers that are applicable to the monitoring of the flow of injected CO2 in reservoirs and leakage into potable shallow groundwater. Geochemical results from the Frio Brine I and II pilot tests located near Dayton, Texas and from the SECARB Phase III tests at Cranfield oil field, Mississippi, proved powerful tools in: 1- Tracking the successful injection and flow of CO2 into the injection sandstones; 2- showing major changes in the chemical (pH, alkalinity, and major divalent cations) and isotopic (δ13C values of CO2, and δ18O values of CO2, and brine) compositions of formation water; 3-. showing mobilization of metals, including Fe Mn and Pb, and organic compounds , including DOC, BTEX, PAHs, and phenols following CO2 injection; and 4- showing that some of the CO2 injected into the Frio 'C' sandstone was detected in the overlying 'B' sandstone that is separated by 15 m of shale and muddy siltstone. Rapid, significant and systematic changes were also observed in the isotopic and chemical compositions of shallow groundwater at the ZERT site located in Bozeman, MT, in response to four yearly controlled injections of CO2 gas through a slotted pipe placed horizontally at a depth of ~2 m below ground level. The observed changes, included the lowering of groundwater pH from ~7.0 to values as low as 5.6, increases in the alkalinity from about 400 mg/L as HCO3 to values of up to 1330 mg/L, increases in the electrical conductance from ~600 μS/cm to up to 1800 μS/cm, as well as increases in the concentrations of cations and metals following CO2

  19. Response of ocean acidification to a gradual increase and decrease of atmospheric CO2

    NASA Astrophysics Data System (ADS)

    Cao, Long; Zhang, Han; Zheng, Meidi; Wang, Shuangjing

    2014-01-01

    We perform coupled climate-carbon cycle model simulations to examine changes in ocean acidity in response to idealized change of atmospheric CO2. Atmospheric CO2 increases at a rate of 1% per year to four times its pre-industrial level of 280 ppm and then decreases at the same rate to the pre-industrial level. Our simulations show that changes in surface ocean chemistry largely follow changes in atmospheric CO2. However, changes in deep ocean chemistry in general lag behind the change in atmospheric CO2 because of the long time scale associated with the penetration of excess CO2 into the deep ocean. In our simulations with the effect of climate change, when atmospheric CO2 reaches four times its pre-industrial level, global mean aragonite saturation horizon (ASH) shoals from the pre-industrial value of 1288 to 143 m. When atmospheric CO2 returns from the peak value of 1120 ppm to pre-industrial level, ASH is 630 m, which is approximately the value of ASH when atmospheric CO2 first increases to 719 ppm. At pre-industrial CO2 9% deep-sea cold-water corals are surrounded by seawater that is undersaturated with aragonite. When atmospheric CO2 reaches 1120 ppm, 73% cold-water coral locations are surrounded by seawater with aragonite undersaturation, and when atmospheric CO2 returns to the pre-industrial level, 18% cold-water coral locations are surrounded by seawater with aragonite undersaturation. Our analysis indicates the difficulty for some marine ecosystems to recover to their natural chemical habitats even if atmospheric CO2 content can be lowered in the future.

  20. Upgrades to NRLMOL code

    NASA Astrophysics Data System (ADS)

    Basurto, Luis

    This project consists of performing upgrades to the massively parallel NRLMOL electronic structure code in order to enhance its performance by increasing its flexibility by: a) Utilizing dynamically allocated arrays, b) Executing in a parallel environment sections of the program that were previously executed in a serial mode, c) Exploring simultaneous concurrent executions of the program through the use of an already existing MPI environment; thus enabling the simulation of larger systems than it is currently capable of performing. Also developed was a graphical user interface that will allow less experienced users to start performing electronic structure calculations by aiding them in performing the necessary configuration of input files as well as providing graphical tools for the displaying and analysis of results. Additionally, a computational toolkit that can avail of large supercomputers and make use of various levels of approximation for atomic interactions was developed to search for stable atomic clusters and predict novel stable endohedral fullerenes. As an application of the developed computational toolkit, a search was conducted for stable isomers of Sc3N C80 fullerene. In this search, about 1.2 million isomers of C80 were optimized in various charged states at the PM6 level. Subsequently, using the selected optimized isomers of C80 in various charged state, about 10,000 isomers of Sc3N C80 were constructed which were optimized using semi-empirical PM6 quantum chemical method. A few selected lowest isomers of Sc3N C80 were optimized at the DFT level. The calculation confirms the lowest 3 isomers previously reported in literature but 4 new isomers are found within the lowest 10 isomers. Using the upgraded NRLMOL code, a study was done of the electronic structure of a multichromoric molecular complex containing two of each borondipyrromethane dye, Zn-tetraphenyl-porphyrin, bisphenyl anthracene and a fullerene. A systematic examination of the effect of

  1. CO2 sequestration in basalts: laboratory measurements

    NASA Astrophysics Data System (ADS)

    Otheim, L. T.; Adam, L.; van Wijk, K.; McLing, T. L.; Podgorney, R. K.

    2010-12-01

    Geologic sequestration of CO2 is proposed as the only promising large-scale method to help reduce CO2 gas emission by its capture at large point sources and subsequent long-term storage in deep geologic formations. Reliable and cost-effective monitoring will be important aspect of ensuring geological sequestration is a safe, effective, and acceptable method for CO2 emissions mitigation. Once CO2 injection starts, seismic methods can be used to monitor the migration of the carbon dioxide plume. To calibrate changes in rock properties from field observations, we propose to first analyze changes in elastic properties on basalt cores. Carbon dioxide sequestration in basalt rocks results in fluid substitution and mixing of CO2 with water and rock mineralizations. Carbon dioxide sequestration in mafic rocks creates reactions such as Mg2SiO 4 + CaMgSi2O 6 + 4CO2 = Mg 3Ca(CO 3) 4 + 3SiO2 whereby primary silicate minerals within the basalt react with carbonic acid laden water to creating secondary carbonate minerals and silicates. Using time-lapse laboratory scale experiments, such as laser generated ultrasonic wave propagation; it is possible to observe small changes in the physical properties of a rock. We will show velocity and modulus measurements on three basalt core samples for different saturation. The ultimate goal of the project is to track seismic changes due to fluid substitution and mineralization. The porosity of our basalts ranges from 8% to 12%, and the P-wave velocity increases by 20% to 40% from dry to water saturated conditions. Petrographic analysis (CT-scans, thin sections, XRF, XRf) will aid in the characterization of the mineral structure in these basalts and its correlation to seismic properties changes resulting from fluid substitution and mineralization.

  2. CO2 Orbital Trends in Comets

    NASA Astrophysics Data System (ADS)

    Kelley, Michael; Bodewits, Dennis; Feaga, Lori; Knight, Matthew; McKay, Adam; Snodgrass, Colin; Wooden, Diane

    2016-08-01

    Carbon dioxide is a primary volatile in comet nuclei, and potentially a major contributor to comet activity (i.e., the process of mass loss). However, CO2 cannot be observed directly from the ground, and past surveys of this molecule in comets were limited to space-borne snapshot observations. This situation limits our understanding of the behavior of CO2 in comets, and its role in driving comet mass loss. To address this deficiency, we were awarded a Cy11 Spitzer program designed to quantify the production rate of CO2 on >month-long timescales for 21 comets. We request an additional 269~hr in Cy13 to complete the Spitzer portion of our survey, and to add three more comets (46P/Wirtanen and 2 Target of Opportunity Oort cloud comets). Our survey is designed to probe the orbital trends of CO2 production in the comet population. We aim to: 1) examine the role of CO2 in the persistent post-perihelion activity observed in Jupiter-family comets; 2) measure the seasonal variations of CO2/H2O as a proxy for nucleus heterogeneity, when possible; 3) search for orbital trends sensitive to cumulative insolation as a proxy for nucleus layering; and 4) examine how Oort cloud comets evolve by comparing dynamically new and old targets. The final data set will allow us to investigate the effects of heating on the evolution of comets, if nucleus structures can be inferred through activity, and set the stage for JWST investigations into comet activity and composition.

  3. Carbon Dioxide, Hydrographic, and Chemical Data Obtained During the R/V Ronald H. Brown Repeat Hydrography Cruise in the Atlantic Ocean: CLIVAR CO2 Section A16S_2005 (11 January - 24 February, 2005)

    SciTech Connect

    Kozyr, Alex

    2006-08-30

    This report presents methods, and analytical and quality control procedures for salinity, oxygen, nutrient, inorganic carbon, organic carbon, chlorofluorocarbon (CFC), and bomb 14C system parameters performed during the A16S_2005 cruise, which took place from January 11 to February 24, 2005, aboard research vessel (R/V) Ronald H. Brown under the auspices of the National Oceanic and Atmospheric Administration (NOAA). The R/V Ronald H. Brown departed Punta Arenas, Chile, on January 11, 2005, and ended its cruise in Fortaleza, Brazil, on February 24, 2005. The research conducted was one of a series of repeat hydrography sections jointly funded by NOAA and the National Science Foundation as part of the CLIVAR/CO2/repeat hydrography/tracer program. Samples were taken from 36 depths at 121 stations. The data presented in this report include the analyses of water samples for total inorganic carbon (TCO2), fugacity of CO2 (fCO2), total alkalinity (TALK), pH, dissolved organic carbon (DOC), CFC, 14C, hydrographic, and other chemical measurements. The R/V Ronald H. Brown A16S_2005 data set is available free of charge as a numeric data package (NDP) from the Carbon Dioxide Information Analysis Center (CDIAC). The NDP consists of the oceanographic data files and this printed documentation, which describes the procedures and methods used to obtain the data.

  4. CO2 Acquisition Membrane (CAM) Project

    NASA Technical Reports Server (NTRS)

    Mason, L. W.; Way, J. D.; Vlasse, M.

    2001-01-01

    The CO2 Acquisition Membrane (CAM) project will develop, test, and analyze membrane materials for separation and purification of carbon dioxide (CO2) from mixtures of gases, such as those found in the Martian atmosphere. The CAM technology will enable passive separation of these gases, allow energy efficient acquisition and purification of these important resources, and lay the foundation for future unmanned sample return and human space missions. The CAM membranes are targeted toward In Situ Resource Utilization (ISRU) applications, such as In Situ Propellant Production (ISPP) and In Situ Consumables Production (ISCP).

  5. 10 MW Supercritical CO2 Turbine Test

    SciTech Connect

    Turchi, Craig

    2014-01-29

    The Supercritical CO2 Turbine Test project was to demonstrate the inherent efficiencies of a supercritical carbon dioxide (s-CO2) power turbine and associated turbomachinery under conditions and at a scale relevant to commercial concentrating solar power (CSP) projects, thereby accelerating the commercial deployment of this new power generation technology. The project involved eight partnering organizations: NREL, Sandia National Laboratories, Echogen Power Systems, Abengoa Solar, University of Wisconsin at Madison, Electric Power Research Institute, Barber-Nichols, and the CSP Program of the U.S. Department of Energy. The multi-year project planned to design, fabricate, and validate an s-CO2 power turbine of nominally 10 MWe that is capable of operation at up to 700°C and operates in a dry-cooled test loop. The project plan consisted of three phases: (1) system design and modeling, (2) fabrication, and (3) testing. The major accomplishments of Phase 1 included: Design of a multistage, axial-flow, s-CO2 power turbine; Design modifications to an existing turbocompressor to provide s-CO2 flow for the test system; Updated equipment and installation costs for the turbomachinery and associated support infrastructure; Development of simulation tools for the test loop itself and for more efficient cycle designs that are of greater commercial interest; Simulation of s-CO2 power cycle integration into molten-nitrate-salt CSP systems indicating a cost benefit of up to 8% in levelized cost of energy; Identification of recuperator cost as a key economic parameter; Corrosion data for multiple alloys at temperatures up to 650ºC in high-pressure CO2 and recommendations for materials-of-construction; and Revised test plan and preliminary operating conditions based on the ongoing tests of related equipment. Phase 1 established that the cost of the facility needed to test the power turbine at its full power and temperature would exceed the planned funding for Phases 2 and 3. Late

  6. Crystallization of CO2 ice and the absence of amorphous CO2 ice in space

    PubMed Central

    Escribano, Rafael M.; Muñoz Caro, Guillermo M.; Cruz-Diaz, Gustavo A.; Rodríguez-Lazcano, Yamilet; Maté, Belén

    2013-01-01

    Carbon dioxide (CO2) is one of the most relevant and abundant species in astrophysical and atmospheric media. In particular, CO2 ice is present in several solar system bodies, as well as in interstellar and circumstellar ice mantles. The amount of CO2 in ice mantles and the presence of pure CO2 ice are significant indicators of the temperature history of dust in protostars. It is therefore important to know if CO2 is mixed with other molecules in the ice matrix or segregated and whether it is present in an amorphous or crystalline form. We apply a multidisciplinary approach involving IR spectroscopy in the laboratory, theoretical modeling of solid structures, and comparison with astronomical observations. We generate an unprecedented highly amorphous CO2 ice and study its crystallization both by thermal annealing and by slow accumulation of monolayers from the gas phase under an ultrahigh vacuum. Structural changes are followed by IR spectroscopy. We also devise theoretical models to reproduce different CO2 ice structures. We detect a preferential in-plane orientation of some vibrational modes of crystalline CO2. We identify the IR features of amorphous CO2 ice, and, in particular, we provide a theoretical explanation for a band at 2,328 cm−1 that dominates the spectrum of the amorphous phase and disappears when the crystallization is complete. Our results allow us to rule out the presence of pure and amorphous CO2 ice in space based on the observations available so far, supporting our current view of the evolution of CO2 ice. PMID:23858474

  7. Reducing the cost of Ca-based direct air capture of CO2.

    PubMed

    Zeman, Frank

    2014-10-07

    Direct air capture, the chemical removal of CO2 directly from the atmosphere, may play a role in mitigating future climate risk or form the basis of a sustainable transportation infrastructure. The current discussion is centered on the estimated cost of the technology and its link to "overshoot" trajectories, where atmospheric CO2 levels are actively reduced later in the century. The American Physical Society (APS) published a report, later updated, estimating the cost of a one million tonne CO2 per year air capture facility constructed today that highlights several fundamental concepts of chemical air capture. These fundamentals are viewed through the lens of a chemical process that cycles between removing CO2 from the air and releasing the absorbed CO2 in concentrated form. This work builds on the APS report to investigate the effect of modifications to the air capture system based on suggestions in the report and subsequent publications. The work shows that reduced carbon electricity and plastic packing materials (for the contactor) may have significant effects on the overall price, reducing the APS estimate from $610 to $309/tCO2 avoided. Such a reduction does not challenge postcombustion capture from point sources, estimated at $80/tCO2, but does make air capture a feasible alternative for the transportation sector and a potential negative emissions technology. Furthermore, air capture represents atmospheric reductions rather than simply avoided emissions.

  8. Carbon dioxide (CO2) biofixation by microalgae and its potential for biorefinery and biofuel production.

    PubMed

    Kassim, Mohd Asyraf; Meng, Tan Keang

    2017-04-15

    Carbon dioxide (CO2) using biological process is one of the promising approaches for CO2 capture and storage. Recently, biological sequestration using microalgae has gained many interest due to its capability to utilize CO2 as carbon source and biomass produced can be used as a feedstock for other value added product for instance biofuel and chemicals. In this study, the CO2 biofixation by two microalgae species, Chlorella sp. and Tetraselmis suecica was investigated using different elevated CO2 concentration. The effect of CO2 concentration on microalgae growth kinetic, biofixation and its chemical composition were determined using 0.04, 5, 15 and 30% CO2. The variation of initial pH value and its relationship on CO2 concentration toward cultivation medium was also investigated. The present study indicated that both microalgae displayed different tolerance toward CO2 concentration. The maximum biomass production and biofixation for Chlorella sp. of 0.64gL(-1) and 96.89mgL(-1)d(-1) was obtained when the cultivation was carried out using 5 and 15% CO2, respectively. In contrast, the maximum biomass production and CO2 biofixation for T. suecica of 0.72gL(-1) and 111.26mgL(-1)d(-1) were obtained from cultivation using 15 and 5% CO2. The pH value for the cultivation medium using CO2 was between 7.5 and 9, which is favorable for microalgal growth. The potential of biomass obtained from the cultivation as a biorefinery feedstock was also evaluated. An anaerobic fermentation of the microalgae biomass by bacteria Clostridium saccharoperbutylacenaticum N1-4 produced various type of value added product such as organic acid and solvent. Approximately 0.27 and 0.90gL(-1) of organic acid, which corresponding to acetic and butyric acid were produced from the fermentation of Chlorella sp. and T. suecica biomass. Overall, this study suggests that Chlorella sp. and T. suecica are efficient microorganism that can be used for CO2 biofixation and as a feedstock for chemical production.

  9. Efficient carbon rejection upgrades Mexico's Maya crude oil

    SciTech Connect

    Suchanek, A.J.; Moore, A.S.

    1986-08-01

    Poor-quality crude oils and resids can be effectively upgraded by a chemically efficient carbon-rejection process followed by hydrotreating. The effectiveness is demonstrated by utilizing the asphalt residual treating (ART) process to upgrade whole Maya crude oil from Mexico, in a 100,000-b/d refinery. Maya was chosen because it represents most of the world's poor-quality crude oils and resids, and because the results of processing Maya will be similar for other poor-quality feed stocks. Here is a review of the upgrade process, along with investment and operating economics of the Maya upgrade.

  10. Silicate minerals for CO2 scavenging from biogas in Autogenerative High Pressure Digestion.

    PubMed

    Lindeboom, Ralph E F; Ferrer, Ivet; Weijma, Jan; van Lier, Jules B

    2013-07-01

    Autogenerative High Pressure Digestion (AHPD) is a novel concept that integrates gas upgrading with anaerobic digestion by selective dissolution of CO2 at elevated biogas pressure. However, accumulation of CO2 and fatty acids after anaerobic digestion of glucose resulted in pH 3-5, which is incompatible with the commonly applied high-rate methanogenic processes. Therefore, we studied the use of wollastonite, olivine and anorthosite, with measured composition of CaSi1.05O3.4, Mg2Fe0.2Ni0.01Si1.2O5.3 and Na0.7Ca1K0.1Mg0.1Fe0.15Al3.1Si4O24, respectively, to scavenge CO2 during batch AHPD of glucose. Depending on the glucose to mineral ratio the pH increased to 6.0-7.5. Experiments with wollastonite showed that Ca(2+)-leaching was caused by volatile fatty acid (VFA) production during glucose digestion. At 1, 3 and 9 bar, the CH4 content reached 74%, 86% and 88%, respectively, indicating CO2 scavenging. Fixation of produced CO2 by CaCO3 precipitation in the sludge was confirmed by Fourier Transferred-InfraRed, Combined Field emission Scanning Electron Microscopy-Energy-dispersive X-ray spectroscopy and Thermogravimetric Analysis-Mass Spectroscopy.

  11. Effects of dissolved CO2 on Shallow Freshwater Microbial Communities simulating a CO2 Leakage Scenario

    NASA Astrophysics Data System (ADS)

    Gulliver, D. M.; Lowry, G. V.; Gregory, K.

    2013-12-01

    Geological carbon sequestration is likely to be part of a comprehensive strategy to minimize the atmospheric release of greenhouse gasses, establishing a concern of sequestered CO2 leakage into overlying potable aquifers. Leaking CO2 may affect existing biogeochemical processes and therefore water quality. There is a critical need to understand the evolution of CO2 exposed microbial communities that influence the biogeochemistry in these freshwater aquifers. The evolution of microbial ecology for different CO2 exposure concentrations was investigated using fluid-slurry samples obtained from a shallow freshwater aquifer (55 m depth, 0.5 MPa, 22 °C, Escatawpa, MS). The microbial community of well samples upstream and downstream of CO2 injection was characterized. In addition, batch vessel experiments were conducted with the upstream aquifer samples exposed to varying pCO2 from 0% to 100% under reservoir temperature and pressure for up to 56 days. The microbial community of the in situ experiment and the batch reactor experiment were analyzed with 16S rRNA clone libraries and qPCR. In both the in situ experiment and the batch reactor experiment, DNA concentration did not correlate with CO2 exposure. Both the in situ experiment and the batch reactors displayed a changing microbial community with increased CO2 exposure. The well water isolate, Curvibacter, appeared to be the most tolerant genus to high CO2 concentrations in the in situ experiments and to mid-CO2 concentrations in the batch reactors. In batch reactors with pCO2 concentrations higher than experienced in situ (pCO2 = 0.5 MPa), Pseudomonas appeared to be the most tolerant genus. Findings provide insight into a dynamic biogeochemical system that will alter with CO2 exposure. Adapted microbial populations will eventually give rise to the community that will impact the metal mobility and water quality. Knowledge of the surviving microbial populations will enable improved models for predicting the fate of CO2

  12. CO2 dispersion modelling over Paris region within the CO2-MEGAPARIS project

    NASA Astrophysics Data System (ADS)

    Lac, C.; Donnelly, R. P.; Masson, V.; Pal, S.; Donier, S.; Queguiner, S.; Tanguy, G.; Ammoura, L.; Xueref-Remy, I.

    2012-10-01

    Accurate simulation of the spatial and temporal variability of tracer mixing ratios over urban areas is challenging, but essential in order to utilize CO2 measurements in an atmospheric inverse framework to better estimate regional CO2 fluxes. This study investigates the ability of a high-resolution model to simulate meteorological and CO2 fields around Paris agglomeration, during the March field campaign of the CO2-MEGAPARIS project. The mesoscale atmospheric model Meso-NH, running at 2 km horizontal resolution, is coupled with the Town-Energy Balance (TEB) urban canopy scheme and with the Interactions between Soil, Biosphere and Atmosphere CO2-reactive (ISBA-A-gs) surface scheme, allowing a full interaction of CO2 between the surface and the atmosphere. Statistical scores show a good representation of the Urban Heat Island (UHI) and urban-rural contrasts. Boundary layer heights (BLH) at urban, sub-urban and rural sites are well captured, especially the onset time of the BLH increase and its growth rate in the morning, that are essential for tall tower CO2 observatories. Only nocturnal BLH at sub-urban sites are slightly underestimated a few nights, with a bias less than 50 m. At Eiffel tower, the observed spikes of CO2 maxima occur every morning exactly at the time at which the Atmospheric Boundary Layer (ABL) growth reaches the measurement height. The timing of the CO2 cycle is well captured by the model, with only small biases on CO2 concentrations, mainly linked to the misrepresentation of anthropogenic emissions, as the Eiffel site is at the heart of trafic emission sources. At sub-urban ground stations, CO2 measurements exhibit maxima at the beginning and at the end of each night, when the ABL is fully contracted, with a very strong spatio-temporal variability. The CO2 cycle at these sites is generally well reproduced by the model, even if some biases on the nocturnal maxima appear in the Paris plume parly due to small errors on the vertical transport, or in

  13. Extraction of lipids from microalgae using CO2-expanded methanol and liquid CO2.

    PubMed

    Paudel, Ashok; Jessop, Michael J; Stubbins, Spencer H; Champagne, Pascale; Jessop, Philip G

    2015-05-01

    The use of CO2-expanded methanol (cxMeOH) and liquid carbon dioxide (lCO2) is proposed to extract lipids from Botryococcus braunii. When compressed CO2 dissolves in methanol, the solvent expands in volume, decreases in polarity and so increases in its selectivity for biodiesel desirable lipids. Solid phase extraction of the algal extract showed that the cxMeOH extracted 21 mg of biodiesel desirable lipids per mL of organic solvent compared to 3mg/mL using either neat methanol or chloroform/methanol mixture. The non-polar lCO2 showed a high affinity for non-polar lipids. Using lCO2, it is possible to extract up to 10% neutral lipids relative to the mass of dry algae. Unlike extractions using conventional solvents, these new methods require little to no volatile, flammable, or chlorinated organic solvents.

  14. Flash scanning the CO2 laser: a revival of the CO2 laser in plastic surgery

    NASA Astrophysics Data System (ADS)

    Lach, Elliot

    1994-09-01

    The CO2 laser has broad clinical application yet also presents a number of practical disadvantages. These drawbacks have limited the success and utilization of this laser in plastic surgery. Flashscanner technology has recently been used for char-free CO2 laser surgery of the oropharynx, the external female genital tract, and perirectal mucosa. A commercially available optomechanical flashscanner unit `Swiftlase,' was adapted to a CO2 laser and used for treatment in numerous plastic surgical applications. Conditions and situations that were treated in this study included generalized neurofibromatosis, tuberous sclerosis, rhinophyma, viral warts, breast reconstruction, and deepithelialization prior to microsurgery or local flap transfer and/or skin graft placement. There were no significant wound healing complications. Some patients previously sustained undue scarring from conventional CO2 laser surgery. Conservative, primarily ablative CO2 laser surgery with the Swiftlase has usefulness for treatment of patients in plastic surgery including those that were previously unsuccessfully treated.

  15. Carbon Dioxide Laser Absorption Spectrometer (CO2LAS) Aircraft Measurements of CO2

    NASA Technical Reports Server (NTRS)

    Christensen, Lance E.; Spiers, Gary D.; Menzies, Robert T.; Jacob, Joseph C.; Hyon, Jason

    2011-01-01

    The Jet Propulsion Laboratory Carbon Dioxide Laser Absorption Spectrometer (CO2LAS) utilizes Integrated Path Differential Absorption (IPDA) at 2.05 microns to obtain CO2 column mixing ratios weighted heavily in the boundary layer. CO2LAS employs a coherent detection receiver and continuous-wave Th:Ho:YLF laser transmitters with output powers around 100 milliwatts. An offset frequency-locking scheme coupled to an absolute frequency reference enables the frequencies of the online and offline lasers to be held to within 200 kHz of desired values. We describe results from 2009 field campaigns when CO2LAS flew on the Twin Otter. We also describe spectroscopic studies aimed at uncovering potential biases in lidar CO2 retrievals at 2.05 microns.

  16. 76 FR 43489 - Deferral for CO2

    Federal Register 2010, 2011, 2012, 2013, 2014

    2011-07-20

    ... 2 and indicates that at present attempting to determine the net carbon cycle impact of particular... and impact biogenic sources of CO2 have in the carbon cycle. Further, methodologies are not... minimis), negative, or positive net impact on the carbon cycle. Therefore, the information EPA...

  17. Agriculture waste and rising CO2

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Currently, there are many uncertainties concerning agriculture’s role in global environmental change including the effects of rising atmospheric CO2 concentration. A viable and stable world food supply depends on productive agricultural systems, but environmental concerns within agriculture have to...

  18. CO2 laser used in cosmetology

    NASA Astrophysics Data System (ADS)

    Su, Chenglie

    1993-03-01

    Cases of various kinds of warts, nevi, papillomas, skin angiomas, ephilises, skin vegetation, scars and brandy noses were vaporized and solidified with a 2.5 - 8 W low power CO2 laser with an overall satisfaction rate up to 99.8% and the satisfaction rate for one time 92%.

  19. Transdermal CO2 application in chronic wounds.

    PubMed

    Wollina, U; Heinig, Birgit; Uhlemann, Christine

    2004-06-01

    Chronic wounds are a challenge to treatment. In this retrospective study, the effect of transdermal CO2 application on wound healing in chronic ulcers was investigated and compared to the effect of CO2 on acute surgical wounds. Eighty-six patients (52 females and 34 males) with chronic wounds of different origin except arterial occlusive disease were included. In addition, 17 patients (5 females, 12 males) with wide excision wounds after surgical therapy of acne inversa were considered. The indication for CO2 application was a wound at risk for infection. Treatment was performed with a Carboflow device once daily for 30 to 60 minutes. There was clinical evidence of improvement of granulation and reduction of discharge and malodor within 1 week of treatment in both chronic and acute wounds. Only 9 patients, all diabetics, needed an additional systemic antibiosis. The treatment was well tolerated. No adverse effects have been noted. Transdermal CO2 application is a useful method to reduce the risk of infection and improve wound healing in both chronic and certain acute wounds. Systematic prospective trials are needed.

  20. Stereotactic CO2 laser therapy for hydrocephalus

    NASA Astrophysics Data System (ADS)

    Kozodoy-Pins, Rebecca L.; Harrington, James A.; Zazanis, George A.; Nosko, Michael G.; Lehman, Richard M.

    1994-05-01

    A new fiber-optic delivery system for CO2 radiation has been used to successfully treat non-communicating hydrocephalus. This system consists of a hollow sapphire waveguide employed in the lumen of a stereotactically-guided neuroendoscope. CO2 gas flows through the bore of the hollow waveguide, creating a path for the laser beam through the cerebrospinal fluid (CSF). This delivery system has the advantages of both visualization and guided CO2 laser radiation without the same 4.3 mm diameter scope. Several patients with hydrocephalus were treated with this new system. The laser was used to create a passage in the floor of the ventricle to allow the flow of CSF from the ventricles to the sub-arachnoid space. Initial postoperative results demonstrated a relief of the clinical symptoms. Long-term results will indicate if this type of therapy will be superior to the use of implanted silicone shunts. Since CO2 laser radiation at 10.6 micrometers is strongly absorbed by the water in tissue and CSF, damage to tissue surrounding the lesion with each laser pulse is limited. The accuracy and safety of this technique may prove it to be an advantageous therapy for obstructive hydrocephalus.

  1. A validation study on CO2 chemistry

    NASA Astrophysics Data System (ADS)

    Koelman, Peter; Heijkers, Stijn; Tadayon Musavi, Samaneh; Graef, Wouter; Bogaerts, Annemie; Dijk, Van, Jan; Elementary Processes in Gas Discharges Team; Plasmant Team

    2016-09-01

    The demand for renewable energy has increased the popularity of various energy sources, such as solar and wind energy. These sources are intermittent by nature, which typically does not match the demand of energy. Therefore, storage of energy is needed. Current tools for this are, however, costly, slow, and inefficient. Storing energy by the formation of valuable fuels from CO2 is potentially an improvement. By plasma assisted CO2 dissociation CO is produced. In subsequent steps the CO is transformed in valuable fuels. An extensive CO2 microwave plasma chemistry is studied, with special attention to the vibrational modes, which provide a pathway for the dissociation. To that end we developed a global model, which is only time resolved and needs less computational time than spatially resolved models. We present the results from a verification study of the CO2 chemistry. This is done by verification of input data, and by comparison of results obtained by two independent models: ZDPlaskin and PLASIMO's Global Model. We also present results from a sensitivity study of the input data.

  2. Hydrogenation of CO2 to methanol: Importance of metal–oxide and metal–carbide interfaces in the activation of CO2

    DOE PAGES

    Rodriguez, José A.; Liu, Ping; Stacchiola, Dario J.; ...

    2015-09-30

    In this study, the high thermochemical stability of CO2 makes it very difficult to achieve the catalytic conversion of the molecule into alcohols or other hydrocarbon compounds, which can be used as fuels or the starting point for the generation of fine chemicals. Pure metals and bimetallic systems used for the CO2 → CH3OH conversion usually bind CO2 too weakly and, thus, show low catalytic activity. Here, we discuss a series of recent studies that illustrate the advantages of metal–oxide and metal–carbide interfaces when aiming at the conversion of CO2 into methanol. CeOx/Cu(111), Cu/CeOx/TiO2(110), and Au/CeOx/TiO2(110) exhibit an activity formore » the CO2 → CH3OH conversion that is 2–3 orders of magnitude higher than that of a benchmark Cu(111) catalyst. In the Cu–ceria and Au–ceria interfaces, the multifunctional combination of metal and oxide centers leads to complementary chemical properties that open active reaction pathways for methanol synthesis. Efficient catalysts are also generated after depositing Cu and Au on TiC(001). In these cases, strong metal–support interactions modify the electronic properties of the admetals and make them active for the binding of CO2 and its subsequent transformation into CH3OH at the metal–carbide interfaces.« less

  3. Toward Solar-Driven Photocatalytic CO2 Reduction Using Water as an Electron Donor.

    PubMed

    Sato, Shunsuke; Arai, Takeo; Morikawa, Takeshi

    2015-06-01

    Developing a system for the production of organic chemicals via CO2 reduction is an important area of research that has the potential to address global warming and fossil fuel consumption. In addition, CO2 reduction promotes carbon source recycling. Solar energy is the largest exploitable resource among renewable energy resources, providing more energy to Earth per hour than the total energy consumed by humans in 1 year. This report describes the advantages and disadvantages of the available CO2 reduction and H2O oxidation photocatalysts and the conjugation of photocatalytic CO2 reduction with H2O oxidation for the creation of an artificial photosynthesis system. In this system, CO2 photoreduction and H2O photooxidation proceeded simultaneously within one system under sunlight irradiation using a hybrid of semiconductors and molecular metal-complex catalysts.

  4. Graphene-Based Photocatalysts for CO2 Reduction to Solar Fuel.

    PubMed

    Low, Jingxiang; Yu, Jiaguo; Ho, Wingkei

    2015-11-05

    Recently, photocatalytic CO2 reduction for solar fuel production has attracted much attention because of its potential for simultaneously solving energy and global warming problems. Many studies have been conducted to prepare novel and efficient photocatalysts for CO2 reduction. Graphene, a two-dimensional material, has been increasingly used in photocatalytic CO2 reduction. In theory, graphene shows several remarkable properties, including excellent electronic conductivity, good optical transmittance, large specific surface area, and superior chemical stability. Attributing to these advantages, fabrication of graphene-based materials has been known as one of the most feasible strategies to improve the CO2 reduction performance of photocatalysts. This Perspective mainly focuses on the recent important advances in the fabrication and application of graphene-based photocatalysts for CO2 reduction to solar fuels. The existing challenges and difficulties of graphene-based photocatalysts are also discussed for future application.

  5. 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.

  6. Direct and reversible hydrogenation of CO2 to formate by a bacterial carbon dioxide reductase.

    PubMed

    Schuchmann, K; Müller, V

    2013-12-13

    Storage and transportation of hydrogen is a major obstacle for its use as a fuel. An increasingly considered alternative for the direct handling of hydrogen is to use carbon dioxide (CO2) as an intermediate storage material. However, CO2 is thermodynamically stable, and developed chemical catalysts often require high temperatures, pressures, and/or additives for high catalytic rates. Here, we present the discovery of a bacterial hydrogen-dependent carbon dioxide reductase from Acetobacterium woodii directly catalyzing the hydrogenation of CO2. We also demonstrate a whole-cell system able to produce formate as the sole end product from dihydrogen (H2) and CO2 as well as syngas. This discovery opens biotechnological alternatives for efficient CO2 hydrogenation either by using the isolated enzyme or by employing whole-cell catalysis.

  7. Rapid CO2 permeation across biological membranes: implications for CO2 venting from tissue.

    PubMed

    Hulikova, Alzbeta; Swietach, Pawel

    2014-07-01

    The degree to which cell membranes are barriers to CO2 transport remains controversial. Proteins, such as aquaporins and Rh complex, have been proposed to facilitate CO2 transport, implying that the nonchannel component of membranes must have greatly reduced CO2 permeability. To determine whether membrane CO2 permeation is rate limiting for gas transport, the spread of CO2 across multicellular tissue growths (spheroids) was measured using intracellular pH as a spatial readout. Colorectal HCT116 cells have basal water and NH3 permeability, indicating the functional absence of aquaporins and gas channels. However, CO2 diffusivity in HCT116 spheroids was only 24 ± 4% lower than in pure water, which can be accounted for fully by volume exclusion due to proteins. Diffusivity was unaffected by blockers of aquaporins and Rh complex (Hg(2+), p-chloromercuribenzoic acid, and 4,4'-diisothiocyano-2,2'-stilbene-disulfonic acid) but decreased under hypertonic conditions (by addition of 300 mOsm mannitol), which increases intracellular protein crowding. Similar CO2 diffusivity was measured in spheroids of T47D breast cells (basal water permeability) and NHDF-Ad fibroblasts (aquaporin-facilitated water permeability). In contrast, diffusivity of NH3, a smaller but less lipophilic gas, was considerably slower than in pure water, as expected from rate-limiting membrane permeation. In conclusion, membranes, even in the functional absence of proposed gas channels, do not restrict CO2 venting from tissue growths.-Hulikova, A., Swietach, P. Rapid CO2 permeation across biological membranes: implications for CO2 venting from tissue.

  8. Vadose Zone Remediation of CO2 Leakage from Geologic CO2 Storage Sites

    SciTech Connect

    Zhang, Yingqi; Oldenburg, Curtis M.; Benson, Sally M.

    2004-03-03

    In the unlikely event that CO2 leakage from deep geologic CO2 sequestration sites reaches the vadose zone, remediation measures for removing the CO2 gas plume may have to be undertaken. Carbon dioxide leakage plumes are similar in many ways to volatile organic compound (VOC) vapor plumes, and the same remediation approaches are applicable. We present here numerical simulation results of passive and active remediation strategies for CO2 leakage plumes in the vadose zone. The starting time for the remediation scenarios is assumed to be after a steady-state CO2 leakage plume is established in the vadose zone, and the source of this plume has been cut off. We consider first passive remediation, both with and without barometric pumping. Next, we consider active methods involving extraction wells in both vertical and horizontal configurations. To compare the effectiveness of the various remediation strategies, we define a half-life of the CO2 plume as a convenient measure of the CO2 removal rate. For CO2 removal by passive remediation approaches such as barometric pumping, thicker vadose zones generally require longer remediation times. However, for the case of a thin vadose zone where a significant fraction of the CO2 plume mass resides within the high liquid saturation region near the water table, the half-life of the CO2 plume without barometric pumping is longer than for somewhat thicker vadose zones. As for active strategies, results show that a combination of horizontal and vertical wells is the most effective among the strategies investigated, as the performance of commonly used multiple vertical wells was not investigated.

  9. The Role of the CO2 Laser and Fractional CO2 Laser in Dermatology

    PubMed Central

    Omi, Tokuya; Numano, Kayoko

    2014-01-01

    Background: Tremendous advances have been made in the medical application of the laser in the past few decades. Many diseases in the dermatological field are now indications for laser treatment that qualify for reimbursement by many national health insurance systems. Among laser types, the carbon dioxide (CO2) laser remains an important system for the dermatologist. Rationale: The lasers used in photosurgery have wavelengths that differ according to their intended use and are of various types, but the CO2 laser is one of the most widely used lasers in the dermatology field. With its wavelength in the mid-infrared at 10,600 nm, CO2 laser energy is wellabsorbed in water. As skin contains a very high water percentage, this makes the CO2 laser ideal for precise, safe ablation with good hemostasis. In addition to its efficacy in ablating benign raised lesions, the CO2 laser has been reported to be effective in the field of esthetic dermatology in the revision of acne scars as well as in photorejuvenation. With the addition of fractionation of the beam of energy into myriad microbeams, the fractional CO2 laser has offered a bridge between the frankly full ablative indications and the nonablative skin rejuvenation systems of the 2000s in the rejuvenation of photoaged skin on and off the face. Conclusions: The CO2 laser remains an efficient, precise and safe system for the dermatologist. Technological advances in CO2 laser construction have meant smaller spot sizes and greater precision for laser surgery, and more flexibility in tip sizes and protocols for fractional CO2 laser treatment. The range of dermatological applications of the CO2 laser is expected to continue to increase in the future. PMID:24771971

  10. Sustained effects of atmospheric [CO2] and nitrogen availability on forest soil CO2 efflux.

    PubMed

    Oishi, A Christopher; Palmroth, Sari; Johnsen, Kurt H; McCarthy, Heather R; Oren, Ram

    2014-04-01

    Soil CO2 efflux (Fsoil ) is the largest source of carbon from forests and reflects primary productivity as well as how carbon is allocated within forest ecosystems. Through early stages of stand development, both elevated [CO2] and availability of soil nitrogen (N; sum of mineralization, deposition, and fixation) have been shown to increase gross primary productivity, but the long-term effects of these factors on Fsoil are less clear. Expanding on previous studies at the Duke Free-Air CO2 Enrichment (FACE) site, we quantified the effects of elevated [CO2] and N fertilization on Fsoil using daily measurements from automated chambers over 10 years. Consistent with previous results, compared to ambient unfertilized plots, annual Fsoil increased under elevated [CO2] (ca. 17%) and decreased with N (ca. 21%). N fertilization under elevated [CO2] reduced Fsoil to values similar to untreated plots. Over the study period, base respiration rates increased with leaf productivity, but declined after productivity saturated. Despite treatment-induced differences in aboveground biomass, soil temperature and water content were similar among treatments. Interannually, low soil water content decreased annual Fsoil from potential values - estimated based on temperature alone assuming nonlimiting soil water content - by ca. 0.7% per 1.0% reduction in relative extractable water. This effect was only slightly ameliorated by elevated [CO2]. Variability in soil N availability among plots accounted for the spatial variability in Fsoil , showing a decrease of ca. 114 g C m(-2) yr(-1) per 1 g m(-2) increase in soil N availability, with consistently higher Fsoil in elevated [CO2] plots ca. 127 g C per 100 ppm [CO2] over the +200 ppm enrichment. Altogether, reflecting increased belowground carbon partitioning in response to greater plant nutritional needs, the effects of elevated [CO2] and N fertilization on Fsoil in this stand are sustained beyond the early stages of stand development and

  11. Isolation of microorganisms from CO2 sequestration sites through enrichments under high pCO2

    NASA Astrophysics Data System (ADS)

    Peet, K. C.; Freedman, A. J.; Boreham, C.; Thompson, J. R.

    2012-12-01

    Carbon Capture and Storage (CCS) in geologic formations has the potential to reduce greenhouse gas emissions from fossil fuel processing and combustion. However, little is known about the effects that CO2 may have on biological activity in deep earth environments. To understand microorganisms associated with these environments, we have developed a simple high-pressure enrichment methodology to cultivate organisms capable of growth under supercritical CO2 (scCO2). Growth media targeting different subsurface functional metabolic groups is added to sterilized 316 stainless steel tubing sealed with quarter turn plug valves values and pressurized to 120-136 atm using a helium-padded CO2 tank, followed by incubation at 37 °C to achieve the scCO2 state. Repeated passages of crushed subsurface rock samples and growth media under supercritical CO2 headspaces are assessed for growth via microscopic enumeration. We have utilized this method to survey sandstone cores for microbes capable of growth under scCO2 from two different geologic sites targeted for carbon sequestration activities. Reproducible growth of microbial biomass under high pCO2 has been sustained from each site. Cell morphologies consist of primarily 1-2 μm rods and oval spores, with densities from 1E5-1E7 cells per ml of culture. We have purified and characterized a bacterial strain most closely related to Bacillus subterraneus (99% 16S rRNA identity) capable of growth under scCO2. Preliminary physiological characterization of this strain indicates it is a spore-forming facultative anaerobe able to grow in 0.5 to 50 ppt salinity. Genome sequencing and analysis currently in progress will help reveal genetic mechanisms of acclimation to high pCO2 conditions associated with geologic carbon sequestration.

  12. Synthesis of sintering-resistant sorbents for CO2 capture.

    PubMed

    Liu, Wenqiang; Feng, Bo; Wu, Yueqin; Wang, Guoxiong; Barry, John; da Costa, João C Diniz

    2010-04-15

    Sorbents for high temperature CO2 capture are under intensive development owing to their potential applications in advanced zero emission power, sorption-enhanced steam methane reforming for hydrogen production and energy storage systems in chemical heat pumps. One of the challenges in the development is the prevention of sintering of the sorbent (normally a calcium oxide derivative) which causes the CO2 capture capacity of the material to deteriorate rapidly after a few cycles of utilization. Here we show that a simple wet mixing method can produce sintering-resistant sorbents from calcium and magnesium salts of d-gluconic acid. It was found that calcium oxide was well distributed in the sorbents with metal oxide nanoparticles on the surface acting as physical barriers, and the CO2 capture capacity of the sorbents was largely maintained over multiple cycles of utilization. This method was also applied to other organometallic salts of calcium and magnesium/aluminum and the produced sorbents showed similarly high reversibility.

  13. Recent advances in CO2 capture and utilization.

    PubMed

    Yu, Kai Man Kerry; Curcic, Igor; Gabriel, Joseph; Tsang, Shik Chi Edman

    2008-01-01

    Energy and the environment are two of the most important issues this century. More than 80 % of our energy comes from the combustion of fossil fuels, which will still remain the dominant energy source for years to come. It is agreed that carbon dioxide produced from the combustion process to be the most important anthropogenic greenhouse gas leading to global warming. Atmospheric CO(2) concentrations have indeed increased by almost 100 ppm since their pre-industrial level, reaching 384 ppm in 2007 with a total annual emission of over 35 Gt. Prompt global action to resolve the CO(2) crisis is therefore needed. To pursue such an action, we are urged to save energy without the unnecessary production of carbon emissions and to use energy in more efficient ways, but alternative methods to mitigate the greenhouse gas have to be considered. This Minireview highlights some recent promising research activities and their prospects in the areas of carbon capture and storage and chemical fixation of CO(2) in constructing a future low-carbon global economy with reference to energy source, thermodynamic considerations, net carbon emissions and availability of reagents.

  14. Detection of CO2 leakage by the surface-soil CO2-concentration monitoring (SCM) system in a small scale CO2 release test

    NASA Astrophysics Data System (ADS)

    Chae, Gitak; Yu, Soonyoung; Sung, Ki-Sung; Choi, Byoung-Young; Park, Jinyoung; Han, Raehee; Kim, Jeong-Chan; Park, Kwon Gyu

    2015-04-01

    Monitoring of CO2 release through the ground surface is essential to testify the safety of CO2 storage projects. We conducted a feasibility study of the multi-channel surface-soil CO2-concentration monitoring (SCM) system as a soil CO2 monitoring tool with a small scale injection. In the system, chambers are attached onto the ground surface, and NDIR sensors installed in each chamber detect CO2 in soil gas released through the soil surface. Before injection, the background CO2 concentrations were measured. They showed the distinct diurnal variation, and were positively related with relative humidity, but negatively with temperature. The negative relation of CO2 measurements with temperature and the low CO2 concentrations during the day imply that CO2 depends on respiration. The daily variation of CO2 concentrations was damped with precipitation, which can be explained by dissolution of CO2 and gas release out of pores through the ground surface with recharge. For the injection test, 4.2 kg of CO2 was injected 1 m below the ground for about 30 minutes. In result, CO2 concentrations increased in all five chambers, which were located less than 2.5 m of distance from an injection point. The Chamber 1, which is closest to the injection point, showed the largest increase of CO2 concentrations; while Chamber 2, 3, and 4 showed the peak which is 2 times higher than the average of background CO2. The CO2 concentrations increased back after decreasing from the peak around 4 hours after the injection ended in Chamber 2, 4, and 5, which indicated that CO2 concentrations seem to be recovered to the background around 4 hours after the injection ended. To determine the leakage, the data in Chamber 2 and 5, which had low increase rates in the CO2 injection test, were used for statistical analysis. The result shows that the coefficient of variation (CV) of CO2 measurements for 30 minutes is efficient to determine a leakage signal, with reflecting the abnormal change in CO2

  15. Net sea-air CO2 fluxes and modelled pCO2 in the southwestern subtropical Atlantic continental shelf during spring 2010 and summer 2011

    NASA Astrophysics Data System (ADS)

    Ito, Rosane Gonçalves; Garcia, Carlos Alberto Eiras; Tavano, Virginia Maria

    2016-05-01

    Sea-air CO2 fluxes over continental shelves vary substantially in time on both seasonal and sub-seasonal scales, driven primarily by variations in surface pCO2 due to several oceanic mechanisms. Furthermore, coastal zones have not been appropriately considered in global estimates of sea-air CO2 fluxes, despite their importance to ecology and to productivity. In this work, we aimed to improve our understanding of the role played by shelf waters in controlling sea-air CO2 fluxes by investigating the southwestern Atlantic Ocean (21-35°S) region, where physical, chemical and biological measurements were made on board the Brazilian R. V. Cruzeiro do Sul during late spring 2010 and early summer 2011. Features such as discharge from the La Plata River, intrusions of tropical waters on the outer shelf due to meandering and flow instabilities of the Brazil Current, and coastal upwelling in the Santa Marta Grande Cape and São Tomé Cape were detected by both in situ measurements and ocean colour and thermal satellite imagery. Overall, shelf waters in the study area were a source of CO2 to the atmosphere, with an average of 1.2 mmol CO2 m-2 day-1 for the late spring and 11.2 mmol CO2 m-2 day-1 for the early summer cruises. The spatial variability in ocean pCO2 was associated with surface ocean properties (temperature, salinity and chlorophyll-a concentration) in both the slope and shelf waters. Empirical algorithms for predicting temperature-normalized surface ocean pCO2 as a function of surface ocean properties were shown to perform well in both shelf and slope waters, except (a) within cyclonic eddies produced by baroclinic instability of the Brazil Current as detected by satellite SST imagery and (b) in coastal upwelling regions. In these regions, surface ocean pCO2 values were higher as a result of upwelled CO2-enriched subsurface waters. Finally, a pCO2 algorithm based on both sea surface temperature and surface chlorophyll-a was developed that enabled the spatial

  16. Investigation of Wyoming Bentonite Hydration in Dry to Water-Saturated Supercritical CH4 and CH4/CO2 Mixtures: Implications for CO2-Enhanced Gas Production

    NASA Astrophysics Data System (ADS)

    Loring, J.; Thompson, C.; Ilton, E. S.; McGrail, B. P.; Schaef, T.

    2014-12-01

    Injection of CO2 into low permeability shale formations leads to additional gas recovery and reduces the flux of CO2 into the atmosphere, thus combining a strong economic incentive with a permanent storage option for CO2. Reduced formation transmissivity due to clay swelling is a concern in CO2 -enhanced gas production. Clay minerals partly determine the physical (i.e. permeability, brittleness) and certain chemical properties (i.e. wetting ability, gas adsorption) of shales, and montmorillonites are of particular interest because they swell by the uptake of species in their interlayer. In this study, the hydration and expansion of a Na-saturated montmorillonite (Na-SWy-2) in high-pressure (90 bar) and moderate temperature (50 °C) methane and mixtures of methane and carbon dioxide were investigated usingCH4 IR spectroscopic titrations andCH4 XRD. The goals were to (1) determine if the hydration/expansion behavior of the clay in supercritical methane is different than in supercritical CO2, (2) determine if methane intercalates the clay, and (3) probe the effects of increasing CO2 concentrations. IR spectra were collected as Na-SWy-2 was titrated with water under several fluid exposures: pure methane, 25, 50, and 75 mole% CO2 in methane, and pure CO2. ComplementaryCH4 XRD experiments were conducted in the same fluids at discrete dissolved water concentrations to measure the d001 values of the clay and thus its volume change on hydration and CH4 and/or CO2 intercalation. In pure methane, no direct evidence of CH4 intercalation was detected in CH bending or stretching regions of the IR spectra. Similarly, in situ XRD indicated the montmorillonite structure was stable in the presence of CH4 and no measurable changes to the basal spacing were observed. However, under low water conditions where the montmorillonite structure was partially expanded (~sub 1W), the IR data indicated a rapid intercalation of CO2 into the interlayer, even with fluid mixtures containing the

  17. An investigation of CO2 splitting using nanosecond pulsed corona discharge: effect of argon addition on CO2 conversion and energy efficiency

    NASA Astrophysics Data System (ADS)

    Moss, M. S.; Yanallah, K.; Allen, R. W. K.; Pontiga, F.

    2017-03-01

    The plasma chemical splitting of carbon dioxide (CO2) to produce carbon monoxide (CO) in a pulsed corona discharge was investigated from both an experimental and a numerical standpoint. High voltage nanosecond pulses were applied to a stream of pure CO2 and its mixture with argon, and the gaseous products were identified using Fourier transform infrared spectroscopy. Due to the shape of pulses, the process of CO2 splitting was found to proceed in two phases. The first phase is dominated by ionization, which generates a high electron density. Then, during the second phase, direct electron impact dissociation of CO2 contributes to a large portion of CO production. Conversion and energy efficiency were calculated for the tested conditions. The conversions achieved are comparable to those obtained using other high pressure non-thermal discharges, such as dielectric barrier discharge. However, the energy efficiencies were considerably higher, which are favorable to industrial applications that require atmospheric conditions and elevated gas flow rates.

  18. Biofuels from Bacteria, Electricity, and CO2: Biofuels from CO2 Using Ammonia or Iron-Oxidizing Bacteria in Reverse Microbial Fuel Cells

    SciTech Connect

    2010-07-01

    Electrofuels Project: Electrofuels Project: Columbia University is using carbon dioxide (CO2) from ambient air, ammonia—an abundant and affordable chemical, and a bacteria called N. europaea to produce liquid fuel. The Columbia University team is feeding the ammonia and CO2 into an engineered tank where the bacteria live. The bacteria capture the energy from ammonia and then use that energy to convert CO2 into a liquid fuel. When the bacteria use up all the ammonia, renewable electricity can regenerate it and pump it back into the system—creating a continuous fuel-creation cycle. In addition, Columbia University is also working with the bacteria A. ferrooxidans to capture and use energy from ferrous iron to produce liquid fuels from CO2.

  19. Improved repetition rate mixed isotope CO2 TEA laser

    NASA Astrophysics Data System (ADS)

    Cohn, D. B.

    2014-09-01

    A compact CO2 TEA laser has been developed for remote chemical detection that operates at a repetition rate of 250 Hz. It emits 700 mJ/pulse at 10.6 μm in a multimode beam with the 12C16O2 isotope. With mixed 12C16O2 plus 13C16O2 isotopes it emits multiple lines in both isotope manifolds to improve detection of a broad range of chemicals. In particular, output pulse energies are 110 mJ/pulse at 9.77 μm, 250 mJ/pulse at 10 μm, and 550 mJ/pulse at 11.15 μm, useful for detection of the chemical agents Sarin, Tabun, and VX. Related work shows capability for long term sealed operation with a catalyst and an agile tuner at a wavelength shift rate of 200 Hz.

  20. CO2 Orbital Trends in Comets

    NASA Astrophysics Data System (ADS)

    Kelley, Michael; Feaga, Lori; Bodewits, Dennis; McKay, Adam; Snodgrass, Colin; Wooden, Diane

    2014-12-01

    Spacecraft missions to comets return a treasure trove of details of their targets, e.g., the Rosetta mission to comet 67P/Churyumov-Gerasimenko, the Deep Impact experiment at comet 9P/Tempel 1, or even the flyby of C/2013 A1 (Siding Spring) at Mars. Yet, missions are rare, the diversity of comets is large, few comets are easily accessible, and comet flybys essentially return snapshots of their target nuclei. Thus, telescopic observations are necessary to place the mission data within the context of each comet's long-term behavior, and to further connect mission results to the comet population as a whole. We propose a large Cycle 11 project to study the long-term activity of past and potential future mission targets, and select bright Oort cloud comets to infer comet nucleus properties, which would otherwise require flyby missions. In the classical comet model, cometary mass loss is driven by the sublimation of water ice. However, recent discoveries suggest that the more volatile CO and CO2 ices are the likely drivers of some comet active regions. Surprisingly, CO2 drove most of the activity of comet Hartley 2 at only 1 AU from the Sun where vigorous water ice sublimation would be expected to dominate. Currently, little is known about the role of CO2 in comet activity because telluric absorptions prohibit monitoring from the ground. In our Cycle 11 project, we will study the CO2 activity of our targets through IRAC photometry. In conjunction with prior observations of CO2 and CO, as well as future data sets (JWST) and ongoing Earth-based projects led by members of our team, we will investigate both long-term activity trends in our target comets, with a particular goal to ascertain the connections between each comet's coma and nucleus.

  1. CO2 profile retrievals from TCCON spectra

    NASA Astrophysics Data System (ADS)

    Dohe, Susanne; Hase, Frank; Sepúlveda, Eliezer; García, Omaira; Wunch, Debra; Wennberg, Paul; Gómez-Peláez, Angel; Abshire, James B.; Wofsy, Steven C.; Schneider, Matthias; Blumenstock, Thomas

    2014-05-01

    The Total Carbon Column Observing Network (TCCON) is a global network of ground-based Fourier Transform Spectrometers recording direct solar spectra in the near-infrared spectral region. With stringent requirements on the instrumentation, data processing and calibration, accurate and precise column-averaged abundances of CO2, CH4, N2O, HF, CO, H2O, and HDO are retrieved being an essential contribution for the validation of satellite data (e.g. GOSAT, OCO-2) and carbon cycle research (Olsen and Randerson, 2004). However, the determined column-averaged dry air mole fraction (DMF) contains no information about the vertical CO2 profile, due to the use of a simple scaling retrieval within the common TCCON analysis, where the fitting algorithm GFIT (e.g. Yang et al., 2005) is used. In this presentation we will apply a different procedure for calculating trace gas abundances from the measured spectra, the fitting algorithm PROFFIT (Hase et. al., 2004) which has been shown to be in very good accordance with GFIT. PROFFIT additionally offers the ability to perform profile retrievals in which the pressure broadening effect of absorption lines is used to retrieve vertical gas profiles, being of great interest especially for the CO2 modelling community. A new analyzing procedure will be shown and retrieved vertical CO2 profiles of the TCCON sites Izaña (Tenerife, Canary Islands, Spain) and Lamont (Oklahoma, USA) will be presented and compared with simultaneously performed surface in-situ measurements and CO2 profiles from different aircraft campaigns. References: - Hase, F. et al., J.Q.S.R.T. 87, 25-52, 2004. - Olsen, S.C. and Randerson, J.T., J.G.Res., 109, D023012, 2004. - Yang, Z. et al., J.Q.S.R.T., 90, 309-321, 2005.

  2. Tapping upgrade potential

    SciTech Connect

    Gill, H.S. )

    1993-01-01

    Modernizing aging hydropower stations presents plant owners with a unique opportunity for improving efficiency and plant output. But several factors should be considered before undertaking a turbine upgrade project.

  3. Training for Technology Upgrade.

    ERIC Educational Resources Information Center

    Strandberg, John

    1997-01-01

    A computer system conversion in a business was relatively painless for users and invisible to customers. The plan relied on basic training strategies that apply to a variety of technology upgrades. (Author/JOW)

  4. Selectivity for CO2 over CH4 on a functionalized periodic mesoporous phenylene-silica explained by transition state theory

    NASA Astrophysics Data System (ADS)

    Kunkel, Christian; Viñes, Francesc; Lourenço, Mirtha A. O.; Ferreira, Paula; Gomes, José R. B.; Illas, Francesc

    2017-03-01

    Efficient separation of CO2/CH4 is critical in biogas upgrading, requiring highly selective adsorbents. Based on the adsorption energies of -0.30 and -0.14 eV, previously calculated by dispersion corrected density functional theory for adsorption/desorption of CO2 and CH4 on the functionalized periodic mesoporous phenylene-silica material APTMS@Ph-PMO, respectively, transition state theory rates were derived and used to simulate the adsorption/desorption rates of these two gases on APTMS@Ph-PMO. The latter yielded an estimation of initial CO2/CH4 selectivity at various temperatures. At T = 298 K, selectivity of 32.2 agrees to an experimental value of 26.1, which validates the method used for evaluating CO2/CH4 adsorption selectivities.

  5. Optics upgrade for switchyard

    SciTech Connect

    Kobilarcik, Thomas R.; /Fermilab

    2005-08-01

    An upgrade of the Switchyard optics is proposed. This upgrade extends the P3 (old Main Ring) lattice through enclosure C. The septa for the 3-way Meson Area split is moved from enclosure F1 to enclosure M01. The functionality of the Meson Target Train is preserved. Finally, for the purpose of demonstrating that the resulting split can be transported, a straw-man lattice is proposed for enclosure M02 and beyond.

  6. Can CO2 help harvest minerals on Mars?

    PubMed

    Flinn, Edward D

    2003-11-01

    When astronauts first go to Mars, it will be difficult for them to bring everything they need to survive. Even the first tentative explorations could last as long as two years. However, spaceships can carry only limited supplies. "We might have to do what explorers have done for ages: live off the land," says chemical engineer Ken Debelak of Vanderbilt University. It is a meager atmosphere, compared to Earth's, and it is about 95% carbon dioxide. This, however, turns out to be an advantage. The CO2, says Debelak, can be used to harvest almost everything else.

  7. Cheminformatics Modeling of Amine Solutions for Assessing their CO2 Absorption Properties.

    PubMed

    Kuenemann, Melaine A; Fourches, Denis

    2017-03-07

    As stricter regulations on CO2 emissions are adopted worldwide, identifying efficient chemical processes to capture and recycle CO2 is of critical importance for industry. The most common process known as amine scrubbing suffers from the lack of available amine solutions capable of capturing CO2 efficiently. Tertiary amines characterized by low heats of reaction are considered good candidates but their absorption properties can significantly differ from one analogue to another despite high structural similarity. Herein, after collecting and curating experimental data from the literature, we have built a modeling set of 41 amine structures with their absorption properties. Then we analyzed their chemical composition using molecular descriptors and non-supervised clustering. Furthermore, we developed a series of quantitative structure-property relationships (QSPR) to assess amines' CO2 absorption properties from their structural characteristics. These models afforded reasonable prediction performances (e. g., Q(2)LOO =0.63 for CO2 absorption amount) even though they are solely based on 2D chemical descriptors and individual machine learning techniques (random forest and neural network). Overall, we believe the chemical analysis and the series of QSPR models presented in this proof-of-concept study represent new knowledge and innovative tools that could be very useful for screening and prioritizing hypothetical amines to be synthesized and tested experimentally for their CO2 absorption properties.

  8. CO2 dispersion modelling over Paris region within the CO2-MEGAPARIS project

    NASA Astrophysics Data System (ADS)

    Lac, C.; Donnelly, R. P.; Masson, V.; Pal, S.; Riette, S.; Donier, S.; Queguiner, S.; Tanguy, G.; Ammoura, L.; Xueref-Remy, I.

    2013-05-01

    Accurate simulation of the spatial and temporal variability of tracer mixing ratios over urban areas is a challenging and interesting task needed to be performed in order to utilise CO2 measurements in an atmospheric inverse framework and to better estimate regional CO2 fluxes. This study investigates the ability of a high-resolution model to simulate meteorological and CO2 fields around Paris agglomeration during the March field campaign of the CO2-MEGAPARIS project. The mesoscale atmospheric model Meso-NH, running at 2 km horizontal resolution, is coupled with the Town Energy Balance (TEB) urban canopy scheme and with the Interactions between Soil, Biosphere and Atmosphere CO2-reactive (ISBA-A-gs) surface scheme, allowing a full interaction of CO2 modelling between the sur