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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. PMID:24293277

  2. 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.

  3. CW CO2 Laser Induced Chemical Reactions

    NASA Astrophysics Data System (ADS)

    Pola, Joseph

    1989-05-01

    CW CO2 laser driven reactions between sulfur hexafluoride and carbon oxide, carbon suboxide, carbonyl sulfide and carbon disulfide proceed at subatmospheric pressures and yield fluorinated carbon compounds and sulfur tetrafluoride. CW CO2 laser driven reactions of organic compounds in the presence of energy-conveying sulfur hexafluoride show reaction course different from that normally observed due to elimination of reactor hot surface effects. The examples concern the decomposition of polychlorohydrocarbons, 2-nitropropane, tert.-butylamine, allyl chloride, spirohexane, isobornyl acetate and the oxidation of haloolefins. CW CO2 laser induced fragmentation of 1-methyl-l-silacyclobutanes and 4-silaspiro(3.4)octane in the presence of sulfur hexafluoride is an effective way for preparation and deposition of stable organosilicon polymers.

  4. Chemical reactions occurring during direct solar reduction of CO2.

    PubMed

    Lyma, J L; Jensen, R J

    2001-09-28

    At high temperatures carbon dioxide may absorb solar radiation and react to form carbon monoxide and molecular oxygen. The CO, so produced, may be converted by well-established means to a combustible fuel, such as methanol. We intend to make a future demonstration of the solar reduction of CO2 based on these processes. This paper, however, addresses only the problem of preserving, or even enhancing, the initial photolytic CO by quenching the hot gas with colder H2O or CO2. We present model calculations with a reaction mechanism used extensively in other calculations. If a CO2 gas stream is heated and photolyzed by intense solar radiation and then allowed to cool slowly, it will react back to the initial CO2 by a series of elementary chemical reactions. The back reaction to CO2 can be terminated with the rapid addition of CO2, water, or a mixture. Calculations show that a three-fold quench with pure CO2 will stop the reactions and preserve over 90% of the initial photolytic CO. We find that water has one of two effects. It can either increase the CO level, or it can catalyze the recombination of O and CO to CO2. The gas temperature is the determining factor. If the quench gas is not sufficient to keep the temperature below approximately 1100 K, a chain-branching reaction dominates and the reaction to CO2 occurs. If the temperature stays below that level a chain terminating reaction dominates and the CO is increased. The former case occurs below approximately a fourfold quench with a water/CO2 mixture. The later case occurs when the quench is greater than fourfold. We conclude that CO2, H2O, or a mixture may quench the hot gas stream photolyzed by solar radiation and preserve the photolytic CO. PMID:11589409

  5. Interpenetrating Metal-Metalloporphyrin Framework for Selective CO2 Uptake and Chemical Transformation of CO2.

    PubMed

    Gao, Wen-Yang; Tsai, Chen-Yen; Wojtas, Lukasz; Thiounn, Timmy; Lin, Chu-Chieh; Ma, Shengqian

    2016-08-01

    Herein we report a robust primitive cubic (pcu)-topology metal-metalloporphyrin framework (MMPF), MMPF-18, which was constructed from a ubiquitous secondary building unit of a tetranuclear zinc cluster, Zn4(μ4-O)(-COO)6, and a linear organic linker of 5,15-bis(4-carboxyphenyl)porphyrin (H2bcpp). The strong π-π stacking from porphyrins and the lengthy H2bcpp ligand affords a 4-fold-interpenetrating network along with reduced void spaces and confined narrow channels. Thereby, MMPF-18 presents segmented pores and high-density metalloporphyrin centers for selective CO2 uptake over CH4 and size-selective chemical transformation of CO2 with epoxides forming cyclic carbonates under ambient conditions. PMID:27337152

  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. Utilization of CO2 fixating bacterium Actinobacillus succinogenes 130Z for simultaneous biogas upgrading and biosuccinic acid production.

    PubMed

    Gunnarsson, Ingólfur B; Alvarado-Morales, Merlin; Angelidaki, Irini

    2014-10-21

    Biogas is an attractive renewable energy carrier. However, it contains CO2 which limits its use for certain applications. Here we report a novel approach for removing CO2 from biogas and capturing it as a biochemical through a biological process. This approach entails converting CO2 into biosuccinic acid using the bacterial strain Actinobacillus succinogenes 130 Z, and simultaneously producing high-purity CH4 (> 95%). Results showed that when pressure during fermentation was increased from 101.325 to 140 kPa, higher CO2 solubility was achieved, thereby positively affecting final succinic acid yield and titer, CO2 consumption rate, and CH4 purity. When using biogas as the only CO2 source at 140 kPa, the CO2 consumption rate corresponded to 2.59 L CO2 L(-1) d(-1) with a final succinic acid titer of 14.4 g L(-1). Under this pressure condition, the highest succinic acid yield and biogas quality reached corresponded to 0.635 g g(-1) and 95.4% (v v(-1)) CH4 content, respectively, after 24 h fermentation. This work represents the first successful attempt to develop a system capable of upgrading biogas to vehicle fuel/gas grid quality and simultaneously produce biosuccinic acid, a valuable building block with large market potential in the near term. PMID:25275929

  8. CO2 mitigation via capture and chemical conversion in seawater.

    PubMed

    Rau, Greg H

    2011-02-01

    A lab-scale seawater/mineral carbonate gas scrubber was found to remove up to 97% of CO(2) in a simulated flue gas stream at ambient temperature and pressure, with a large fraction of this carbon ultimately converted to dissolved calcium bicarbonate. After full equilibration with air, up to 85% of the captured carbon was retained in solution, that is, it did not degas or precipitate. Thus, above-ground CO(2) hydration and mineral carbonate scrubbing may provide a relatively simple point-source CO(2) capture and storage scheme at coastal locations. Such low-tech CO(2) mitigation could be especially relevant for retrofitting to existing power plants and for deployment in the developing world, the primary source of future CO(2) emissions. Addition of the resulting alkaline solution to the ocean may benefit marine ecosystems that are currently threatened by acidification, while also allowing the utilization of the vast potential of the sea to safely sequester anthropogenic carbon. This approach in essence hastens Nature's own very effective but slow CO(2) mitigation process; carbonate mineral weathering is a major consumer of excess atmospheric CO(2) and ocean acidity on geologic times scales. PMID:21189009

  9. Will chemical defenses become more effective against specialist herbivores under elevated CO2?

    PubMed

    Landosky, John M; Karowe, David N

    2014-10-01

    Elevated atmospheric CO2 is known to affect plant-insect herbivore interactions. Elevated CO2 causes leaf nitrogen to decrease, the ostensible cause of herbivore compensatory feeding. CO2 may also affect herbivore consumption by altering chemical defenses via changes in plant hormones. We considered the effects of elevated CO2, in conjunction with soil fertility and damage (simulated herbivory), on glucosinolate concentrations of mustard (Brassica nigra) and collard (B. oleracea var. acephala) and the effects of leaf nitrogen and glucosinolate groups on specialist Pieris rapae consumption. Elevated CO2 affected B. oleracea but not B. nigra glucosinolates; responses to soil fertility and damage were also species-specific. Soil fertility and damage also affected B. oleracea glucosinolates differently under elevated CO2. Glucosinolates did not affect P. rapae consumption at either CO2 concentration in B. nigra, but had CO2-specific effects on consumption in B. oleracea. At ambient CO2, leaf nitrogen had strong effects on glucosinolate concentrations and P. rapae consumption but only gluconasturtiin was a feeding stimulant. At elevated CO2, direct effects of leaf nitrogen were weaker, but glucosinolates had stronger effects on consumption. Gluconasturtiin and aliphatic glucosinolates were feeding stimulants and indole glucosinolates were feeding deterrents. These results do not support the compensatory feeding hypothesis as the sole driver of changes in P. rapae consumption under elevated CO2. Support for hormone-mediated CO2 response (HMCR) was mixed; it explained few treatment effects on constitutive or induced glucosinolates, but did explain patterns in SEMs. Further, the novel feeding deterrent effect of indole glucosinolates under elevated CO2 in B. oleracae underscores the importance of defensive chemistry in CO2 response. We speculate that P. rapae indole glucosinolate detoxification mechanisms may have been overwhelmed under elevated CO2 forcing slowed

  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. PMID:23500788

  11. Chemical pathway analysis of the Martian atmosphere: CO2-formation pathways

    NASA Astrophysics Data System (ADS)

    Stock, Joachim W.; Boxe, Christopher S.; Lehmann, Ralph; Grenfell, J. Lee; Patzer, A. Beate C.; Rauer, Heike; Yung, Yuk L.

    2012-05-01

    The chemical composition of a planetary atmosphere plays an important role for atmospheric structure, stability, and evolution. Potentially complex interactions between chemical species do not often allow for an easy understanding of the underlying chemical mechanisms governing the atmospheric composition. In particular, trace species can affect the abundance of major species by acting in catalytic cycles. On Mars, such cycles even control the abundance of its main atmospheric constituent CO2. The identification of catalytic cycles (or more generally chemical pathways) by hand is quite demanding. Hence, the application of computer algorithms is beneficial in order to analyze complex chemical reaction networks. Here, we have performed the first automated quantified chemical pathways analysis of the Martian atmosphere with respect to CO2-production in a given reaction system. For this, we applied the Pathway Analysis Program (PAP) to output data from the Caltech/JPL photochemical Mars model. All dominant chemical pathways directly related to the global CO2-production have been quantified as a function of height up to 86 km. We quantitatively show that CO2-production is dominated by chemical pathways involving HOx and Ox. In addition, we find that NOx in combination with HOx and Ox exhibits a non-negligible contribution to CO2-production, especially in Mars' lower atmosphere. This study reveals that only a small number of chemical pathways contribute significantly to the atmospheric abundance of CO2 on Mars; their contributions to CO2-production vary considerably with altitude. This analysis also endorses the importance of transport processes in governing CO2-stability in the Martian atmosphere. Lastly, we identify a previously unknown chemical pathway involving HOx, Ox, and HO2-photodissociation, contributing 8% towards global CO2-production by chemical pathways using recommended up-to-date values for reaction rate coefficients.

  12. 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.

  13. 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. PMID:26995449

  14. [Study of new blended chemical absorbents to absorb CO2].

    PubMed

    Wang, Jin-Lian; Fang, Meng-Xiang; Yan, Shui-Ping; Luo, Zhong-Yang; Cen, Ke-Fa

    2007-11-01

    Three kinds of blended absorbents were investigated on bench-scale experimental bench according to absorption rate and regeneration grade to select a reasonable additive concentration. The results show that, among methyldiethanolamine (MDEA) and piperazine (PZ) mixtures, comparing MDEA : PZ = 1 : 0.4 (m : m) with MDEA : PZ = 1 : 0.2 (m : m), the absorption rate is increased by about 70% at 0.2 mol x mol(-1). When regeneration lasting for 40 min, regeneration grade of blended absorbents with PZ concentration of 0.2, 0.4, and 0.8 is decreased to 83.06%, 77.77% and 76.67% respectively while 91.04% for PZ concentration of 0. MDEA : PZ = 1 : 0.4(m : m) is a suitable ratio for MDEA/PZ mixtures as absorption and regeneration properties of the blended absorbents are all improved. The aqueous blends with 10% primary amines and 2% tertiary amines could keep high CO2 absorption rate, and lower regeneration energy consumption. Adding 2% 2-Amino-2-methyl-1-propanol (AMP) to 10% diethanolamine (DEA), the blended amine solvents have an advantage in absorption and regeneration properties over other DEA/AMP mixtures. Blended solvents, which consist of a mixture of primary amines with a small amount of tertiary amines, have the highest absorption rate among the three. And mixed absorbents of secondary amines and a small amount of sterically hindered amines have the best regeneration property. To combine absorption and regeneration properties, blends with medium activator addition to tertiary amines are competitive. PMID:18290495

  15. 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.

  16. Mechano-chemical pathways to H2O and CO2 splitting

    NASA Astrophysics Data System (ADS)

    Vedadi, Mohammad H.; Haas, Stephan

    2011-10-01

    The shock-induced collapse of CO2-filled nanobubbles is investigated using molecular dynamics simulations based on a reactive force field. The energetic nanojet and high-pressure water hammer shock formed during and after collapse of the nanobubble trigger mechano-chemical H2O-CO2 reactions, some of which lead to splitting of water and formation of O2 molecules. The dominant pathways through which splitting of water molecules occur are identified.

  17. Soil CO2 respiration: Comparison of chemical titration, CO2 IRGA analysis and the Solvita gel system

    Technology Transfer Automated Retrieval System (TEKTRAN)

    The purpose of this research is to compare the results of measured soil CO2 respiration using three methods: (1) titration method; (2) Infrared gas analysis (IRGA); and (3) the Solvita gel system for soil CO2 analysis. We acquired 36 soil samples from across the USA for comparison which ranged in pH...

  18. 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. PMID:23792821

  19. 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.

  20. Ionization controls for biomineralization-inspired CO2 chemical looping at constant room temperature.

    PubMed

    Liu, Zhaoming; Hu, Yadong; Zhao, Hongqing; Wang, Yang; Xu, Xurong; Pan, Haihua; Tang, Ruikang

    2015-04-21

    Living organisms such as corals can carry out CO2 looping efficiently via biomineralization under ambient conditions. Inspired by this natural process, we establish a solution system of calcium acetate-ethanol-water (Ca(Ac)2-C2H5OH-H2O) for CO2 chemical looping at constant room temperature. The CO2 capture is achieved by its reaction with Ca(Ac)2 to form calcium carbonate (CaCO3) mineral and HAc in the binary solvent with a high C2H5OH content. However, an increase in the H2O content in the system triggers acetic acid (HAc)-induced CaCO3 dissolution to release CO2. The system can be recovered for CO2 capture readily by the replenishment of C2H5OH. This biomimetic mineralization-based CO2 capture/release is controlled by the ionization states of the electrolytes, and is precisely regulated in the C2H5OH-H2O binary solvent. Our attempt highlights the fundamental principle of solution chemistry in reaction control and provides a bioinspired strategy for CO2 capture/release with very low cost and easy availability. PMID:25787086

  1. An upgraded carbon-based method to estimate the anthropogenic fraction of dissolved CO2 in the Atlantic Ocean

    NASA Astrophysics Data System (ADS)

    Vázquez-Rodríguez, M.; Padin, X. A.; Ríos, A. F.; Bellerby, R. G. J.; Pérez, F. F.

    2009-04-01

    An upgrade of classical methods to calculate the anthropogenic carbon (Cant) signal based on estimates of the preformed dissolved inorganic carbon (CTCO2 disequilibrium (ΔCdis) included in the formulation. The change of ΔCdis with time has shown to have non-negligible biases on Cant estimates, producing a 4 μmol kg

  2. Chemical vapor deposition on chabazite (CHA) zeolite membranes for effective post-combustion CO2 capture.

    PubMed

    Kim, Eunjoo; Lee, Taehee; Kim, Hyungmin; Jung, Won-Jin; Han, Doug-Young; Baik, Hionsuck; Choi, Nakwon; Choi, Jungkyu

    2014-12-16

    Chabazite (CHA) zeolites with a pore size of 0.37 × 0.42 nm(2) are expected to separate CO2 (0.33 nm) from larger N2 (0.364 nm) in postcombustion flue gases by recognizing their minute size differences. Furthermore, the hydrophobic siliceous constituent in CHA membranes can allow for maintaining the CO2/N2 separation performance in the presence of H2O in contrast with the CO2 affinity-based membranes. In an attempt to increase the molecular sieving ability, the pore mouth size of all silica CHA (Si-CHA) particles was reduced via the chemical vapor deposition (CVD) of a silica precursor (tetraethyl orthosilicate). Accordingly, an increase of the CVD treatment duration decreased the penetration rate of CO2 into the CVD-treated Si-CHA particles. Furthermore, the CVD process was applied to siliceous CHA membranes in order to improve their CO2/N2 separation performance. Compared to the intact CHA membranes, the CO2/N2 maximum separation factor (max SF) for CVD-treated CHA membranes was increased by ∼ 2 fold under dry conditions. More desirably, the CO2/N2 max SF was increased by ∼ 3 fold under wet conditions at ∼ 50 °C, a representative temperature of the flue gas stream. In fact, the presence of H2O in the feed disfavored the permeation of N2 more than that of CO2 through CVD-modified CHA membranes and thus, contributed to the increased CO2/N2 separation factor. PMID:25479409

  3. 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

  4. 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. PMID:26734087

  5. Sigmoid Correlations for Gas Solubility and Enthalpy Change of Chemical Absorption of CO2

    DOE PAGESBeta

    Huang, Kuan; Wu, You-Ting; Dai, Sheng

    2015-10-01

    Knowledge of the relationship between gas solubility and enthalpy change of chemical absorption of CO2 is very important for exploring energy-efficient absorbents for CO2 capture. To this end, equations that can directly correlate gas solubility with absorption enthalpy were derived through combining the van’t Hoff equation with the reaction equilibrium thermodynamic model (RETM). In this study, two typical reaction mechanisms for chemical absorption of CO2 (1:1 and 1:2) were considered for RETM. The variations of gas solubility with enthalpy change were found to be distinctively sigmoid functions, regardless of the investigated temperature and pressure or assumed reaction forms between CO2more » and the absorbent molecule. Theoretically calculated variation curves of gas solubility vs enthalpy change agreed well with experimental results reported in literature. Also, on the basis of the trade-off relationship between gas solubility and enthalpy change, criterions for evaluating energy-efficient chemical absorbents for CO2 capture were proposed.« less

  6. Global CO2-consumption by chemical weathering: What is the contribution of highly active weathering regions?

    NASA Astrophysics Data System (ADS)

    Hartmann, Jens; Jansen, Nils; Dürr, Hans H.; Kempe, Stephan; Köhler, Peter

    2010-05-01

    CO2-consumption by chemical weathering of silicates and resulting silicate/carbonate weathering ratios influences the terrestrial lateral inorganic carbon flux to the ocean and long-term climate changes. However, little is known of the spatial extension of highly active weathering regions and their proportion of global CO2-consumption. As those regions may be of significant importance for global climate change, global CO2-consumption is calculated here at high resolution, to adequately represent them. In previous studies global CO2-consumption is estimated using two different approaches: i) a reverse approach based on hydrochemical fluxes from large rivers and ii) a forward approach applying spatially explicit a function for CO2-consumption. The first approach results in an estimate without providing a spatial resolution for highly active regions and the second approach applied six lithological classes while including three sediment classes (shale, sandstone and carbonate rock) based at a 1° or 2° grid resolution. It remained uncertain, if the applied lithological classification schemes represent adequately CO2-consumption from sediments on a global scale (as well as liberation of other elements like phosphorus or silicon by chemical weatheirng). This is due to the large variability of sediment properties, their diagenetic history and the contribution from carbonates apparent in silicate dominated lithological classes. To address these issues, a CO2-consumption model, trained at high-resolution data, is applied here to a global vector based lithological map with 15 lithological classes. The calibration data were obtained from areas representing a wide range of weathering rates. Resulting global CO2-consumption by chemical weathering is similar to earlier estimates (237 Mt C a-1) but the proportion of silicate weathering is 63%, and thus larger than previous estimates (49 to 60%). The application of the enhanced lithological classification scheme reveals that it

  7. 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

  8. 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...

  9. 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

  10. 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. PMID:24599714

  11. Laboratory Investigations of the Hydro-Mechanical-Chemical Coupling Behaviour of Sandstone in CO2 Storage in Aquifers

    NASA Astrophysics Data System (ADS)

    Zhou, Hui; Hu, Dawei; Zhang, Fan; Shao, Jianfu; Feng, Xiating

    2016-02-01

    This paper is devoted to experimental investigations of the hydro-mechanical-chemical coupling behaviour of sandstone in the context of CO2 storage in aquifers. We focused on the evolution of creep strain, the transport properties and the elastic modulus of sandstone under the effect of CO2-brine or CO2 alone. A summary of previous laboratory results is first presented, including mechanical, poromechanical and hydro-mechanical-chemical coupling properties. Tests were then performed to investigate the evolution of the creep strain and permeability during the injection of CO2-brine or CO2 alone. After the injection of CO2-brine or CO2 alone, an instantaneous volumetric dilatancy was observed due to the decrease in the effective confining stress. However, CO2 alone had a significant influence on the creep strain and permeability compared to the small influence of CO2-brine. This phenomenon can be attributed to the acceleration of the CO2-brine-rock reaction by the generation of carbonic acid induced by the dissolution of CO2 into the brine. The original indentation tests on samples after the CO2-brine-rock reaction were also performed and indicated that the elastic modulus decreased with an increasing reaction time. The present laboratory results can advance our knowledge of the hydro-mechanical-chemical coupling behaviour of sandstone in CO2 storage in aquifers.

  12. 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.

  13. Impact of atmospheric CO2 rise on chemical weathering of the continental surfaces

    NASA Astrophysics Data System (ADS)

    Godderis, Y.; Roelandt, C.; Beaulieu, E.; Kaplan, J. O.; Schott, J.

    2009-04-01

    Continental weathering consumes atmospheric CO2. Recent analysis of field data has shown that this flux is rapidly reacting to ongoing climate (ref 1) and land use changes (ref 2), displaying an increase of up to 40 % over a few decades. Weathering processes are thus a potentially important component of the present day global carbon cycle. We developed numerical model describing continental weathering reactions based on laboratory kinetic laws and coupled to numerical model of the productivity of the biosphere (B-WITCH)(ref 3,4). This model is able to simulate the chemical composition of streams for both small and large continental watersheds. In this model, we emphasized the role of land plants in controlling belowground hydrological fluxes and decreasing the pH of percolating water through root respiration, both of which heavily impact weathering rates. Both climate change and increasing atmospheric CO2 concentrations affect the productivity and biogeography of the terrestrial biosphere through direct climate effects and CO2 fertilization. With our weathering model coupled to a dynamic global vegetation model, we have the capability to explore the impact of CO2 and climate change on rock weathering. With regards to CO2 fertilization, we calculate that the overall weathering rate may potentially rise by 20 % when CO2 increases up to 8 times the present day pressure for a large tropical watershed (Orinoco). This change is driven by a decrease in evapotranspiration when CO2 rises, and thus by an increase in the weathering profile drainage. We extend our sensitivity tests to the fertilization effect to 20 sites all over the world under various climatic, biospheric and lithologic conditions, and the results will be discussed. ref 1: Gislason et al., EPSL, 277, 213-222, 2008 ref 2: Raymond et al.,Nature, 451, 449-452, 2008 ref 3: Godd

  14. 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. PMID:27581929

  15. 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. PMID:24632437

  16. 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

  17. 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.

  18. A method for incorporating equilibrium chemical reactions into multiphase flow models for CO2 storage

    NASA Astrophysics Data System (ADS)

    Saaltink, Maarten W.; Vilarrasa, Victor; De Gaspari, Francesca; Silva, Orlando; Carrera, Jesús; Rötting, Tobias S.

    2013-12-01

    CO2 injection and storage in deep saline aquifers involves many coupled processes, including multiphase flow, heat and mass transport, rock deformation and mineral precipitation and dissolution. Coupling is especially critical in carbonate aquifers, where minerals will tend to dissolve in response to the dissolution of CO2 into the brine. The resulting neutralization will drive further dissolution of both CO2 and calcite. This suggests that large cavities may be formed and that proper simulation may require full coupling of reactive transport and multiphase flow. We show that solving the latter may suffice whenever two requirements are met: (1) all reactions can be assumed to occur in equilibrium and (2) the chemical system can be calculated as a function of the state variables of the multiphase flow model (i.e., liquid and gas pressure, and temperature). We redefine the components of multiphase flow codes (traditionally, water and CO2), so that they are conservative for all reactions of the chemical system. This requires modifying the traditional constitutive relationships of the multiphase flow codes, but yields the concentrations of all species and all reaction rates by simply performing speciation and mass balance calculations at the end of each time step. We applied this method to the H2O-CO2-Na-Cl-CaCO3 system, so as to model CO2 injection into a carbonate aquifer containing brine. Results were very similar to those obtained with traditional formulations, which implies that full coupling of reactive transport and multi-phase flow is not really needed for this kind of systems, but the resulting simplifications may make it advisable even for cases where the above requirements are not met. Regarding the behavior of carbonate rocks, we find that porosity development near the injection well is small because of the low solubility of calcite. Moreover, dissolution concentrates at the front of the advancing CO2 plume because the brine below the plume tends to reach

  19. Chemical pathway analysis of the lower Martian atmosphere: The CO2 stability problem

    NASA Astrophysics Data System (ADS)

    Stock, J. W.; Grenfell, J. L.; Lehmann, R.; Patzer, A. B. C.; Rauer, H.

    2012-08-01

    The chemical composition and hence the structure of terrestrial planetary atmospheres can be critically controlled by trace species which can act in catalytic cycles. Identifying such chemical pathways is in general challenging. Due to the complexity of chemical reaction networks, like those used in Martian atmospheric chemistry, automated methods become more and more useful to cope with this task. Here, we investigate the applicability of a unique analysis tool PAP (Pathway Analysis Program) to the chemistry at Mars' atmospheric surface conditions, for which we have developed a photochemical box-model. PAP is applied for the first time to the output of this model to investigate the well-known CO2 stability problem of the Martian atmosphere. We identify and rank the most dominant pathways responsible for CO2 formation and prove thereby the applicability of PAP for Mars atmospheric conditions by comparison with known chemical cycles. Furthermore, we propose here an additional new catalytic CO2 formation cycle which is also involved in the production of ozone.

  20. 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.

  1. Chemical Reactions of Portland Cement with Aqueous CO2 and Their Impacts on Cement's Mechanical Properties under Geologic CO2 Sequestration Conditions.

    PubMed

    Li, Qingyun; Lim, Yun Mook; Flores, Katharine M; Kranjc, Kelly; Jun, Young-Shin

    2015-05-19

    To provide information on wellbore cement integrity in the application of geologic CO2 sequestration (GCS), chemical and mechanical alterations were analyzed for cement paste samples reacted for 10 days under GCS conditions. The reactions were at 95 °C and had 100 bar of either N2 (control condition) or CO2 contacting the reaction brine solution with an ionic strength of 0.5 M adjusted by NaCl. Chemical analyses showed that the 3.0 cm × 1.1 cm × 0.3 cm samples were significantly attacked by aqueous CO2 and developed layer structures with a total attacked depth of 1220 μm. Microscale mechanical property analyses showed that the hardness and indentation modulus of the carbonated layer were 2-3 times greater than for the intact cement, but those in the portlandite-dissolved region decreased by ∼50%. The strength and elastic modulus of the bulk cement samples were reduced by 93% and 84%, respectively. The properties of the microscale regions, layer structure, microcracks, and swelling of the outer layers combined to affect the overall mechanical properties. These findings improve understanding of wellbore integrity from both chemical and mechanical viewpoints and can be utilized to improve the safety and efficiency of CO2 storage. PMID:25893278

  2. Graphene Coating of Silicon Nanoparticles with CO2 -Enhanced Chemical Vapor Deposition.

    PubMed

    Son, In Hyuk; Park, Jong Hwan; Kwon, Soonchul; Choi, Jang Wook; Rümmeli, Mark H

    2016-02-01

    Understanding the growth of graphene over Si species is becoming ever more important as the huge potential for the combination of these two materials becomes more apparent, not only for device fabrication but also in energy applications, particularly in Li-ion batteries. Thus, the drive for the direct fabrication of graphene over Si is crucial because indirect approaches, by their very nature, require processing steps that, in general, contaminate, damage, and are costly. In this work, the direct chemical vapor deposition growth of few-layer graphene over Si nanoparticles is systematically explored through experiment and theory with the use of a reducer, H2 or the use of a mild oxidant, CO2 combined with CH4 . Unlike the case of CH4 , with the use of CO2 as a mild oxidant in the reaction, the graphene layers form neatly over the surface and encapsulate the Si particles. SiC formation is also prevented. These structures show exceptionally good electrochemical performance as high capacity anodes for lithium-ion batteries. Density functional theory studies show the presence of CO2 not only prevents SiC formation but helps enhance the catalytic activity of the particles by maintaining an SiOx surface. In addition, CO2 can enhance graphitization. PMID:26662621

  3. 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. PMID:25603157

  4. 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.

  5. Combining microbial production with chemical upgrading.

    PubMed

    Goulas, Konstantinos A; Toste, F Dean

    2016-04-01

    This review presents developments in the chemical processing of fermentation-derived compounds, focusing on ethanol, lactic acid, 2,3-butanediol and the acetone-butanol-ethanol mixture. We examine pathways from these products to biologically-derived drop-in fuels, polymers, as well as commodity chemicals, highlighting the role of homogeneous and heterogeneous catalysts in the development of green processes for the production of fuels and high-value-added compounds from biomass. PMID:26773758

  6. 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

  7. 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.

  8. A Single-Culture Bioprocess of Methanothermobacter thermautotrophicus to Upgrade Digester Biogas by CO2-to-CH4 Conversion with H2

    PubMed Central

    Martin, Matthew R.; Fornero, Jeffrey J.; Angenent, Largus T.

    2013-01-01

    We optimized and tested a postbioprocessing step with a single-culture archaeon to upgrade biogas (i.e., increase methane content) from anaerobic digesters via conversion of CO2 into CH4 by feeding H2 gas. We optimized a culture of the thermophilic methanogen Methanothermobacter thermautotrophicus using: (1) a synthetic H2/CO2 mixture; (2) the same mixture with pressurization; (3) a synthetic biogas with different CH4 contents and H2; and (4) an industrial, untreated biogas and H2. A laboratory culture with a robust growth (dry weight of 6.4–7.4 g/L; OD600 of 13.6–15.4), a volumetric methane production rate of 21 L/L culture-day, and a H2 conversion efficiency of 89% was moved to an industrial anaerobic digester facility, where it was restarted and fed untreated biogas with a methane content of ~70% at a rate such that CO2 was in excess of the stoichiometric requirements in relation to H2. Over an 8-day operating period, the dry weight of the culture initially decreased slightly before stabilizing at an elevated level of ~8 g/L to achieve a volumetric methane production rate of 21 L/L culture-day and a H2 conversion efficiency of 62%. While some microbial contamination of the culture was observed via microscopy, it did not affect the methane production rate of the culture. PMID:24194675

  9. Biogas upgrading by chemical absorption using ammonia rich absorbents derived from wastewater.

    PubMed

    McLeod, Andrew; Jefferson, Bruce; McAdam, Ewan J

    2014-12-15

    The use of ammonia (NH3) rich wastewaters as an ecological chemical absorption solvent for the selective extraction of carbon dioxide (CO2) during biogas upgrading to 'biomethane' has been studied. Aqueous ammonia absorbents of up to 10,000 gNH3 m(-3) demonstrated CO2 absorption rates higher than recorded in the literature for packed columns using 20,000-80,000 g NH3 m(-3) which can be ascribed to the process intensification provided by the hollow fibre membrane contactor used in this study to support absorption. Centrifuge return liquors (2325 g m(-3) ionised ammonium, NH4(+)) and a regenerant (477 gNH4(+) m(-3)) produced from a cationic ion exchanger used to harvest NH4(+) from crude wastewater were also tested. Carbon dioxide fluxes measured for both wastewaters compared reasonably with analogue ammonia absorption solvents of equivalent NH3 concentration. Importantly, this demonstrates that ammonia rich wastewaters can facilitate chemically enhanced CO2 separation which eliminates the need for costly exogenic chemicals or complex chemical handling which are critical barriers to implementation of chemical absorption. When testing NH3 analogues, the potential to recover the reaction product ammonium bicarbonate (NH4HCO3) in crystalline form was also illustrated. This is significant as it suggests a new pathway for ammonia separation which avoids biological nitrification and produces ammonia stabilised into a commercially viable fertiliser (NH4HCO3). However, in real ammonia rich wastewaters, sodium bicarbonate and calcium carbonate were preferentially formed over NH4HCO3 although it is proposed that NH4HCO3 can be preferentially formed by manipulating both ion exchange and absorbent chemistry. PMID:25277752

  10. 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. PMID:17966976

  11. 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.

  12. Photocatalytic Reduction of CO2 over Heterostructure Semiconductors into Value-Added Chemicals.

    PubMed

    Guo, Ling-Ju; Wang, Yan-Jie; He, Tao

    2016-08-01

    Photoreduction of CO2 , which utilizes solar energy to convert CO2 into hydrocarbons, can be an effective means to overcome the increasing energy crisis and mitigate the rising emissions of greenhouse gas. This article covers recent advances in the CO2 photoreduction over heterostructure-based photocatalysts. The fundamentals of CO2 photoreduction and classification of the heterostructured photocatalysts are discussed first, followed by the latest work on the CO2 photoreduction over heterostructured photocatalysts in terms of the classification of the coupling semiconductors. Finally, a brief summary and a perspective on the challenges in this area are presented. PMID:27276171

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

    DOE PAGESBeta

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

    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

  14. 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. PMID:25655352

  15. 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. PMID:26051496

  16. Experimental study of the influence of chemical reactions on convective dissolution of CO2 in aqueous solutions.

    NASA Astrophysics Data System (ADS)

    Thomas, Carelle; Lemaigre, Lorena; Haudin, Florence; Zalts, Anita; D'Onofrio, Alejandro; De Wit, Anne

    2014-05-01

    Within the global context of climate change, carbon dioxide (CO2) sequestration into deep saline aquifers is one of the technologies being considered in order to tackle the accumulation of anthropogenic CO2 in the atmosphere. Upon injection of CO2 into these porous geological formations, the less dense CO2 rises above the aqueous phase, spreads laterally under the upper impermeable cap rock and starts to dissolve into the underlying brine. This leads to a buoyantly unstable stratification of denser CO2-enriched brine on top of less dense brine, which can give rise to density-driven convective fingering in the fluid. This hydrodynamic instability is a favorable process for CO2 sequestration as it accelerates the mixing of CO2 into the aqueous phase and therefore enhances the safety of the storage in the saline aquifer (by reducing the risks of leaks of CO2 to the atmosphere). The influence of chemical reactions and of the physico-chemical characteristics of the geological reservoir on the development of this instability is, however, still not completely understood. In this context, we study experimentally in a laboratory-scale reactor the influence of chemical reactions on convective fingering occurring during dissolution of CO2 in reactive aqueous solutions. Experiments are performed in Hele-Shaw cells (constructed of two vertical transparent plates separated by a thin gap) in which gaseous CO2 at atmospheric pressure flows above aqueous solutions containing chemical reactants. Dynamics occurring within the transparent fluids are visualized by Schlieren techniques, which track dynamical changes in refractive index related to density gradients in the solutions. We show that in some cases the convection can be enhanced by chemical reactions as they accelerate the development of the fingers, shorten their onset time and increase the number of fingers. In particular, we show that the presence of a color indicator (for instance bromocresol green) in the aqueous solution

  17. 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.

  18. 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.

  19. Preliminary investigation on the chemical response of cementitious grouts used for borehole sealing in geologically stored CO2

    NASA Astrophysics Data System (ADS)

    Giannoukos, Konstantinos; Hall, Matthew; Rochelle, Christopher; Milodowski, Antoni; Rigby, Sean

    2014-05-01

    The successful geological storage of CO2 in underground reservoirs aims to immobilize the injected CO2 stream in the form of secondary minerals through reaction with primary minerals or pore fluids in the host rock formations. Injection wells and other boreholes within the reservoir represent a major potential pathway for CO2 to leak back to the surface. Therefore, the stability of well seals is a critical factor for the risk assessment of existing and the design of new CO2 injection wells. Cement-based grouts emplaced within the steel borehole liner, and between the liner and the rock formation, must seal the well against leakage, both during the CO2 injection stage and for a significant time after well abandonment, to allow for the CO2 to be immobilized though rock-water interaction in the reservoir. The injected super-critical CO2 (scCO2) experiences temperatures up to 180oC and pressures at depths greater than 800m, and when dissolved in rock formation waters create chemically reactive species that could impact the stability of cement seals. In an attempt to evaluate the impact of scCO2-saturated fluids in class G oilfield grouts, batch experiments at 80bar and 60oC/ 120oC were carried for pure cement and cement-steel cylindrical samples immersed in a realistic formation porewater composition. Destructive and healing features were observed by means of backscattered scanning electron microscopy (BSE) and energy-dispersive X-ray microanalysis (EDS) elemental mapping; both phenomena were evident in Ca leaching from, and deposition on, the surface of the samples, respectively. Structural cement components like Si appear to have retained their original particle-like shape in the regions affected by the CO2 in the 60oC experiments, but their preservation at 120oC is vaguer. The liberation of Ca2+ from the hydrated cement particles (indicated by local decrease of the Ca/Si ratio), and the reactions with the incoming carbonate/bicarbonate anions seem to evolve

  20. Bimetallic catalysts for upgrading of biomass to fuels and chemicals.

    PubMed

    Alonso, David Martin; Wettstein, Stephanie G; Dumesic, James A

    2012-12-21

    Research interest in biomass conversion to fuels and chemicals has increased significantly in the last decade as the necessity for a renewable source of carbon has become more evident. Accordingly, many different reactions and processes to convert biomass into high-value products and fuels have been proposed in the literature. Special attention has been given to the conversion of lignocellulosic biomass, which does not compete with food sources and is widely available as a low cost feedstock. In this review, we start with a brief introduction on lignocellulose and the different chemical structures of its components: cellulose, hemicellulose, and lignin. These three components allow for the production of different chemicals after fractionation. After a brief overview of the main reactions involved in biomass conversion, we focus on those where bimetallic catalysts are playing an important role. Although the reactions are similar for cellulose and hemicellulose, which contain C(6) and C(5) sugars, respectively, different products are obtained, and therefore, they have been reviewed separately. The third major fraction of lignocellulose that we address is lignin, which has significant challenges to overcome, as its structure makes catalytic processing more challenging. Bimetallic catalysts offer the possibility of enabling lignocellulosic processing to become a larger part of the biofuels and renewable chemical industry. This review summarizes recent results published in the literature for biomass upgrading reactions using bimetallic catalysts. PMID:22872312

  1. Numerical Simulation of Thermal-Hydrological-Mechanical-Chemical Processes during CO2 Geo-sequestration in Saline Aquifer

    NASA Astrophysics Data System (ADS)

    zhang, R.; Winterfeld, P.; Yin, X.; Wu, Y.

    2013-12-01

    The significance of thermal-hydrologic-mechanical-chemical (THMC) processes is well recognized in the operation of CO2 geo-sequestration. Geomechanical and geochemical effects may significantly change aqueous phase composition, porosity and permeability of the formation, and in turn flow and transport. The TOUGHREACT simulator (Xu et al., 2004) has the capability to quantitatively simulate multiphase fluid flow, solute transport and geochemical reactions during CO2 sequestration in saline aquifers using a sequential coupling. Using a mean stress formulation, stresses, displacements, and rock deformations due to fluid injection have been simulated by the recently developed TOUGH2-CSM (Winterfeld and Wu, 2011) to account for the geomechanical effects in CO2 sequestration in saline aquifers. Based on these previously developed numerical simulators: TOUGH-ECO2N (Pruess, 2005), TOUGHREACT, and TOUGH2-CSM, we present general mathematical formulations of the THMC processes. Two coupled computational frameworks (sequentially coupled procedure and fully coupled procedure) are developed to simulate reactive, multiphase transport of CO2 in saline aquifer with thermal and geomechanical effects; both of them model (1) fluid and heat flow, and solute transport in the aqueous phase within a three-phase mixture, (2) stresses and displacements related to the mean stress, (3) non-isothermal effects on fluid properties and reaction processes, and (4) chemical equilibrium and kinetics of fluid-rock and gas-rock interactions. A set of partial differential equations is formulated to represent the physical, mechanical and chemical processes. The accuracy of the THMC models is demonstrated using four examples with analytical solutions: (1) 1D reactive transport under chemical equilibrium conditions, (2) 1D reactive transport with chemical kinetics, (3) 1D heat conduction, and (4) 1D consolidation. Finally, the developed reactive transport models with general chemical compositions are

  2. 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

  3. 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.

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

    PubMed

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

    2014-04-01

    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

  5. 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

  6. Using the Relationship between Vehicle Fuel Consumption and CO2 Emissions To Illustrate Chemical Principles

    NASA Astrophysics Data System (ADS)

    Oliver-Hoyo, Maria T.; Pinto, Gabriel

    2008-02-01

    This instructional resource utilizes consumer product information by which students compare theoretical stoichiometric calculations to CO 2 car emissions and fuel consumption data. Representing graphically the emission of CO 2 versus consumption of fuel provides a tangible way of connecting concepts studied in chemistry classes to everyday life. Considerable simplification of an otherwise complex chemistry problem provides comparable theoretical and actual data. Practice with unit conversion and graphing enhance this activity promoting skills used by professionals to perform emission measurements. This activity may be used to bring awareness of car emissions issues such as the environmental impact of CO 2 emissions and the differences of hybrid engines or gasoline versus diesel engines. Scientific literacy can be approached by incorporating exercises such as this one into chemistry classroom activities. Students have expressed keen interest in this type of "tangible" chemistry where a concrete example of everyday life puts textbook chemistry in context.

  7. Mechanistic studies of pyridinium electrochemistry: alternative chemical pathways in the presence of CO2.

    PubMed

    Peroff, A G; Weitz, E; Van Duyne, R P

    2016-01-21

    Protonated heterocyclic amines, such as pyridinium, have been utilized as catalysts in the electrocatalytic reduction of carbon dioxide. While these represent a new and exciting class of electrocatalysts, the details of the mechanism and faradaic processes occurring in solution are unclear. We report a series of cyclic voltammetry experiments involving Pt, Ag, Au, and Cu electrodes, under both aqueous and nonaqueous conditions, directed towards gaining an improved mechanistic understanding of pyridinium electrochemistry. Surface-enhanced Raman (SER) spectroelectrochemistry was also performed on Cu film-over-nanosphere electrodes in order to identify adsorbed species. It was found that the reduction potential of pyridinium (-0.58 V vs. SCE) and its electrochemical reversibility are unique features of platinum electrodes. In contrast, the reduction potentials on Ag, Au, and Cu electrodes are ∼400 mV more negative than Pt in both the presence and the absence of CO2. SER spectroelectrochemistry of pyridinium solutions shows no evidence for a pyridinium radical or a pyridinium ion. Increased cathodic current in the presence of CO2 is only detected at scan rates less than 10 mV s(-1) in aqueous solutions. The addition of CO2 resulted in a shift in the potential for the hydrogen evolution reaction. Pyridinium electrochemistry was observed under nonaqueous conditions; however no increase in cathodic current was observed when CO2 was added to the solution. Based on this set of results it is concluded that the reduction potential of pyridinium is surface dependent, CO2 acts as a pseudo-reserve of H(+), and pyridinium and CO2 create an alternative mechanism for hydrogen evolution. PMID:26670579

  8. 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.

  9. 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

  10. Chemical ordering and large tunnel magnetoresistance in Co2FeAl/MgAl2O4/Co2FeAl(001) junctions

    NASA Astrophysics Data System (ADS)

    Scheike, Thomas; Sukegawa, Hiroaki; Inomata, Koichiro; Ohkubo, Tadakatsu; Hono, Kazuhiro; Mitani, Seiji

    2016-05-01

    Epitaxial magnetic tunnel junctions (MTJs) with a Co2FeAl/CoFe (0.5 nm)/MgAl2O4/Co2FeAl(001) structure were fabricated by magnetron sputtering. High-temperature in situ annealing led to a high degree of B2-order in the Co2FeAl layers and cation order of the MgAl2O4 barrier. Large tunnel magnetoresistance (TMR) of up to 342% was obtained at room temperature (616% at 4 K), in contrast to the TMR ratio ( ≲ 160%) suppressed by the band-folding effect in Fe/cation-ordered MgAl2O4/Fe MTJs. The present study reveals that the high degree of B2-order and the resulting high spin polarization in the Co2FeAl electrodes enable us to bypass the band-folding problem in spinel barriers.

  11. 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).

  12. Chemical composition and antioxidant properties of candlenut oil extracted by supercritical CO2.

    PubMed

    Siddique, Bazlul Mobin; Ahmad, Anees; Alkarkhi, Abbas F M; Ibrahim, Mahamad Hakimi; K, Mohd Omar A

    2011-05-01

    Candlenut oil was extracted using supercritical CO(2) (SC-CO(2)) with an optimization of parameters, by the response surface methodology. The ground candlenut samples were treated in 2 different ways, that is, dried in either a heat oven (sample moisture content of 2.91%) or dried in a vacuum oven (sample moisture content of 1.98%), before extraction. An untreated sample (moisture content of 4.87%) was used as a control. The maximum percentage of oil was extracted from the heat-oven-dried sample (77.27%), followed by the vacuum-oven-dried sample (74.32%), and the untreated sample (70.12%). At an SC-CO(2) pressure of 48.26 Mpa and 60 min of extraction time, the optimal temperatures for extraction were found to be 76.4 °C, 73.9 °C, and 70.6 °C for the untreated, heat-oven-dried, and vacuum-oven-dried samples, respectively. The heat-oven-dried sample contains the highest percentage of linoleic acid, followed by the untreated and vacuum-oven-dried samples. The antiradical activity of candlenut oil corresponded to an IC(50) value of 30.37 mg/mL. PMID:22417332

  13. 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. PMID:26546088

  14. 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

  15. 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.

  16. The Idaho Chemical Processing Plant Special Nuclear Material vault upgrade

    SciTech Connect

    Anderson, R.C.; Holloway, E.R.

    1992-06-24

    This document discusses storage space in a Special Nuclear Material (SNM) product storage vault at the Idaho Chemical Processing Plant (ICPP) which has been recently expanded by approximately 175%. This expansion required a minimum of space and funding and resulted in a large increase in net storage capacity. Security for the additional storage is provided by standard intrusion sensors and by a real-time monitoring system, which monitors the weight of the material as it rests on weight sensors (load cells). The monitoring system also feeds weight data to a Safeguards processor which provides further confidence to Safeguards personnel. The Department of Energy requirements for bimonthly inventories for SNM stored in a particular part of this facility have been eliminated because of the guarantees provided by a real-time monitoring system. A higher efficiency has been obtained by using the expensive real estate inside a hardened product storage vault. This project has provided the ICPP with a relatively inexpensive vault upgrade and when product material is placed in this area of the vault the manpower requirements to inventory it will be reduced, resulting in a net reduction in plant worker radiation exposure.

  17. 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

  18. Morphology and chemical composition analysis on multi-pulsed CO2 laser ablation of HgCdTe crystals

    NASA Astrophysics Data System (ADS)

    Tang, Wei; Guo, Jin; Shao, Jun-feng; Wang, Ting-feng

    2013-09-01

    In order to study deeply damage mechanism of HgCdTe crystal irradiated by multi-pulsed CO2 laser and obtain the characteristics of surface morphological and chemical composition changes. Firstly, Irradiation effect experiment is conducted on the Hg0.826Cd0.174Te crystal by pulsed CO2 laser, which has a pulse width of 200ns and repetition frequency ranges from 1 Hz to 100 kHz. Then morphological and chemical composition changes of Hg0.826Cd0.174Te crystal is measured by field emission scanning electron microscope (FESEM) and damage threshold is obtained by morphology method. Finally, the impact of laser power density on morphological and chemical composition changes is analyzed. The research results show that: damage threshold of Hg0.826Cd0.174Te crystal which is irradiated by multi-pulsed CO2 laser is 950 W/cm2. The crystal surface melting phenomenon is very obvious, the obvious crack which is caused by thermal stress is not found in the surface, and a large number of bulges and pits are taken shape in the laser ablation zone. Chemical composition changes of the crystal are obvious, and a lot of O element is found in the laser ablation zone. With the increase of laser irradiation power, the content of Hg element decrease rapidly, the content of Cd, Te and O element raise by degrees, and chemical composition changes of the crystal are more and more obvious. When the irradiation power density is 1.8kW/cm2, the surface becomes smooth in the ablation zone due to the impact of laser impulse force, and the content of the chemical compositions is that Hg accounts for 0.23%, Cd accounts for 21.38%, Te accounts for 26.27%, and O accounts for 52.12%. The conclusions of the study have a reference value for the Hg0.826Cd0.174Tecrystal in the application of making infrared detector and pulsed CO2 laser in the aspect of laser processing.

  19. Magnetic and chemical order-disorder transformations in Co2Fe(Ga1-xSix) and Co2Fe(Al1-ySiy) Heusler alloys

    NASA Astrophysics Data System (ADS)

    Umetsu, Rie Y.; Okubo, Akinari; Kainuma, Ryosuke

    2012-04-01

    The concentration dependence of the order-disorder phase transformation temperature from the L21 to the B2 phase (TtL21/B2) and magnetic properties of Co2Fe(Ga1-xSix) and Co2Fe(Al1-ySiy) Heusler alloys were investigated. In the phase diagrams, a crossover of the Curie temperature (TC) and TtL21/B2 was confirmed at around y = 0.45 in Co2Fe(Al1-ySiy), whereas the TC and TtL21/B2 monotonically changed with x in Co2Fe (Ga1-xSix). The slopes of the linear concentration dependence of TtL21/B2 for Co2Fe(Al1-ySiy) drastically changed at about y = 0.45, suggesting that the chemical interchange energy between Fe and Al in Co2FeAl alloy is affected by the magnetic ordering.

  20. Towards understanding the variability in biospheric CO2 fluxes: using FTIR spectrometry and a chemical transport model to investigate the sources and sinks of carbonyl sulfide and its link to CO2

    NASA Astrophysics Data System (ADS)

    Wang, Yuting; Deutscher, Nicholas M.; Palm, Mathias; Warneke, Thorsten; Notholt, Justus; Baker, Ian; Berry, Joe; Suntharalingam, Parvadha; Jones, Nicholas; Mahieu, Emmanuel; Lejeune, Bernard; Hannigan, James; Conway, Stephanie; Mendonca, Joseph; Strong, Kimberly; Campbell, J. Elliott; Wolf, Adam; Kremser, Stefanie

    2016-02-01

    Understanding carbon dioxide (CO2) biospheric processes 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 retrievals of the atmospheric concentrations of both CO2 and OCS from measured solar absorption spectra. Here, we investigate co-located and quasi-simultaneous FTIR measurements of OCS and CO2 performed at five selected sites located in the Northern Hemisphere. These measurements are compared to simulations of OCS and CO2 using a chemical transport model (GEOS-Chem). The coupled biospheric fluxes of OCS and CO2 from the simple biosphere model (SiB) are used in the study. The CO2 simulation with SiB fluxes agrees with the measurements well, while the OCS simulation reproduced a weaker drawdown than FTIR measurements at selected sites, and a smaller latitudinal gradient in the Northern Hemisphere during growing season when comparing with HIPPO (HIAPER Pole-to-Pole Observations) data spanning both hemispheres. An offset in the timing of the seasonal cycle minimum between SiB simulation and measurements is also seen. Using OCS as a photosynthesis proxy can help to understand how the biospheric processes are reproduced in models and to further understand the carbon cycle in the real world.

  1. 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.

  2. 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. PMID:25916240

  3. 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

    2016-08-01

    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. PMID:27351778

  4. River geochemistry, chemical weathering, and atmospheric CO2 consumption rates in the Virunga Volcanic Province (East Africa)

    NASA Astrophysics Data System (ADS)

    Balagizi, Charles M.; Darchambeau, François; Bouillon, Steven; Yalire, Mathieu M.; Lambert, Thibault; Borges, Alberto V.

    2015-09-01

    We report a water chemistry data set from 13 rivers of the Virunga Volcanic Province (VVP) (Democratic Republic of Congo), sampled between December 2010 and February 2013. Most parameters showed no pronounced seasonal variation, whereas their spatial variation suggests a strong control by lithology, soil type, slope, and vegetation. High total suspended matter (289-1467 mg L-1) was recorded in rivers in the Lake Kivu catchment, indicating high soil erodibility, partly as a consequence of deforestation and farming activities. Dissolved and particulate organic carbon (DOC and POC) were lower in rivers from lava fields, and higher in nonvolcanic subcatchments. Stable carbon isotope signatures (δ13C) of POC and DOC mean δ13C of -22.5‰ and -23.5‰, respectively, are the first data to be reported for the highland of the Congo River basin and showed a much higher C4 contribution than in lowland areas. Rivers of the VVP were net sources of CH4 to the atmosphere (4-5052 nmol L-1). Most rivers show N2O concentrations close to equilibrium, but some rivers showed high N2O concentrations related to denitrification in groundwaters. δ13C signatures of dissolved inorganic carbon suggested magmatic CO2 inputs to aquifers/soil, which could have contributed to increase basalt weathering rates. This magmatic CO2-mediated basalt weathering strongly contributed to the high major cation concentrations and total alkalinity. Thus, chemical weathering (39.0-2779.9 t km-2 yr-1) and atmospheric CO2 consumption (0.4-37.0 × 106 mol km-2 yr-1) rates were higher than previously reported in the literature for basaltic terrains.

  5. Elevated CO2 alters the feeding behaviour of the pea aphid by modifying the physical and chemical resistance of Medicago truncatula.

    PubMed

    Guo, Huijuan; Sun, Yucheng; Li, Yuefei; Liu, Xianghui; Wang, Pingyan; Zhu-Salzman, Keyan; Ge, Feng

    2014-09-01

    Elevated CO(2) compromises the resistance of leguminous plants against chewing insects, but little is known about whether elevated CO(2) modifies the resistance against phloem-sucking insects or whether it has contrasting effects on the resistance of legumes that differ in biological nitrogen fixation. We tested the hypothesis that the physical and chemical resistance against aphids would be increased in Jemalong (a wild type of Medicago truncatula) but would be decreased in dnf1 (a mutant without biological nitrogen fixation) by elevated CO(2). The non-glandular and glandular trichome density of Jemalong plants increased under elevated CO(2), resulting in prolonged aphid probing. In contrast, dnf1 plants tended to decrease foliar trichome density under elevated CO(2), resulting in less surface and epidermal resistance to aphids. Elevated CO(2) enhanced the ineffective salicylic acid-dependent defence pathway but decreased the effective jasmonic acid/ethylene-dependent defence pathway in aphid-infested Jemalong plants. Therefore, aphid probing time decreased and the duration of phloem sap ingestion increased on Jemalong under elevated CO(2), which, in turn, increased aphid growth rate. Overall, our results suggest that elevated CO(2) decreases the chemical resistance of wild-type M. truncatula against aphids, and that the host's biological nitrogen fixation ability is central to this effect. PMID:24697655

  6. 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

  7. Towards understanding the variability in biospheric CO2 fluxes: using FTIR spectrometry and a chemical transport model to investigate the sources and sinks of carbonyl sulfide and its link to CO2

    NASA Astrophysics Data System (ADS)

    Wang, Y.; Deutscher, N. M.; Palm, M.; Warneke, T.; Notholt, J.; Baker, I.; Berry, J.; Suntharalingam, P.; Jones, N.; Mahieu, E.; Lejeune, B.; Campbell, J. E.; Wolf, A.; Kremser, S.

    2015-09-01

    Understanding carbon dioxide (CO2) biospheric processes is of great importance because the terrestrial exchange drives the seasonal and inter-annual 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 mean to differentiate between these processes. Solar absorption Fourier Transform InfraRed (FTIR) spectrometry allows for the retrievals of the atmospheric concentrations of both CO2 and OCS from measured solar absorption spectra. Here, we investigate co-located and quasi-simultaneous FTIR measurements of OCS and CO2 performed at three selected sites located in the Northern Hemisphere. These measurements are compared to simulations of OCS and CO2 using a chemical transport model (GEOS-Chem). The OCS simulations are driven by different land biospheric fluxes to reproduce the seasonality of the measurements. Increasing the plant uptake of Kettle et al. (2002a) by a factor of three resulted in the best comparison with FTIR measurements. However, there are still discrepancies in the latitudinal distribution when comparing with HIPPO (HIAPER Pole-to-Pole Observations) data spanning both hemispheres. The coupled biospheric fluxes of OCS and CO2 from the simple biosphere model (SiB) are used in the study and compared to measurements. The CO2 simulation with SiB fluxes agrees with the measurements well, while the OCS simulation reproduced a weaker drawdown than FTIR measurements at selected sites, and a smaller latitudinal gradient in the Northern Hemisphere during growing season. An offset in the timing of the seasonal cycle minimum between SiB simulation and measurements is also seen. Using OCS as a

  8. Flow paths and chemical reactivity of CO2 in carbonates using Mercury-Intrusion Capillary Pressure data and dimensionless numbers

    NASA Astrophysics Data System (ADS)

    Vialle, S.; Dvorkin, J. P.; Mavko, G. M.

    2012-12-01

    Experiments performed earlier by Vialle and Vanorio (2011) [1] have showed that the injection of CO2-rich water (pH=3.2) in various calcite limestones lead to heterogeneous dissolution of the pore structure, inducing secondary porosity and changing the rock stiffness. The presence of oil in the pore space affects the magnitude of these changes by lowering the reactive surface area. We present here a semi-quantitative analysis at the mesoscale to investigate how different initial pore microgeometries and heterogeneities in pore microgeometry affect the fluid-rock interactions. In particular, we aim at quantitatively explaining (1) why, in clean samples, higher-porosity micrite with rounded grains appears to be more affected by dissolution than tight micrite and spar cement and (2) why, for the same number of pore volumes of fluid injected, the magnitude of the changes in porosity (and subsequently elastic properties) differs among the studied rock samples. Rock microgeometry is studied by classical rock-physics methods, He-pycnometry and Mercury-Intrusion Capillary Pressure (MICP) tests, as well as by Scanning Electron Microscopy (SEM) imaging. Experiments were performed on subsamples (~0.5cm3) extracted from core plugs (~12cm3): two Fontainebleau sandstones, to serve as benchmarks, and two calcite carbonates from two different geological formations. In order to relate pore microgeometry to flow paths and chemical reactivity of CO2 in carbonate rocks, we chose to work at a scale that lies between the pore scale and the core scale. The method consists of physically subdividing the core plugs under examination into subsets based on the pore-throat sizes; these subsets correspond to three types of microstructure: "macropores", "microporous rounded micrite", and "spar cement"/"tight micrite". The dimensionless Péclet (Pe) and Damkhöler (Da) numbers, defined as the ratio between the advection rate and the diffusion rate, and as the ratio between the reaction rate and

  9. 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.

  10. CO2 enhanced chemical vapor deposition growth of few-layer graphene over NiO(x).

    PubMed

    Son, In Hyuk; Song, Hyun Jae; Kwon, Soonchul; Bachmatiuk, Alicja; Lee, Seung Jae; Benayad, Anass; Park, Jong Hwan; Choi, Jae-Young; Chang, Hyuk; Rümmeli, Mark H

    2014-09-23

    The use of mild oxidants in chemical vapor deposition (CVD) reactions has proven enormously useful. This was also true for the CVD growth of carbon nanotubes. As yet though, the use of mild oxidants in the CVD of graphene has remained unexplored. Here we explore the use of CO2 as a mild oxidant during the growth of graphene over Ni with CH4 as the feedstock. Both our experimental and theoretical findings provide in-depth insight into the growth mechanisms and point to the mild oxidants playing multiple roles. Mild oxidants lead to the formation of a suboxide in the Ni, which suppresses the bulk diffusion of C species suggesting a surface growth mechanism. Moreover, the formation of a suboxide leads to enhanced catalytic activity at the substrate surface, which allows reduced synthesis temperatures, even as low as 700 °C. Even at these low temperatures, the quality of the graphene is exceedingly high as indicated by a negligible D mode in the Raman spectra. These findings suggest the use of mild oxidants in the CVD fabrication as a whole could have a positive impact. PMID:25171048

  11. 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.

  12. 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.

  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. OPERATIONAL EXPERIENCE: UPGRADED MPC AND A SYSTEMS FOR THE RADIOCHEMICAL PLANT OF THE SIBERIAN CHEMICAL COMBINE

    SciTech Connect

    RODRIGUEZ,C.GOLOSKOKOV,I.FISHBONE,L.GOODEY,K.LOOMIS,M.CRAIN,B.JR.LARSEN,R.

    2003-07-18

    The success of reducing the risk of nuclear proliferation through physical protection and material control/accounting systems depends upon the development of an effective design that includes consideration of the objectives of the systems and the resources available to implement the design. Included among the objectives of the design are facility characterization, definition of threat, and identification of targets. When considering resources, the designer must consider funds available, rapid low-cost elements, technology elements, human resources, and the availability of resources to sustain operation of the end system. The Siberian Chemical Combine (SCC) is a multi-function nuclear facility located in the Tomsk region of Siberia, Russia. Beginning in 1996, SCC joined with the United States Department of Energy (US/DOE) Material Protection, Control, and Accounting (MPC&A) Program to develop and implement MPC&A upgrades for the Radiochemical, Chemical Metallurgical, Conversion, Uranium Enrichment, and Reactor Plants of the SCC. At the Radiochemical Plant the MPC&A design and implementation process has been largely completed for the Plutonium Storage Facility and related areas of the Radiochemical Plant. Design and implementation of upgrades for the Radiochemical Plant include rapid physical protection upgrades such as bricking up of doors and windows, and installation of security-hardened doors. Rapid material control and accounting upgrades include installation of modern balances and bar code equipment. Comprehensive MPC&A upgrades include the installation of access controls to sensitive areas of the Plant, alarm communication and display (AC&D) systems to detect and annunciate alarm conditions, closed circuit (CCTV) systems to assess alarm conditions, central and secondary alarm station upgrades that enable security forces to assess and respond to alarm conditions, material control and accounting upgrades that include upgraded physical inventory procedures, and

  15. 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). PMID:27428712

  16. 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. PMID:27550833

  17. A coupling alternative to reactive transport simulations for long-term prediction of chemical reactions in heterogeneous CO2 storage systems

    NASA Astrophysics Data System (ADS)

    De Lucia, M.; Kempka, T.; Kühn, M.

    2015-02-01

    Fully coupled, multi-phase reactive transport simulations of CO2 storage systems can be approximated by a simplified one-way coupling of hydrodynamics and reactive chemistry. The main characteristics of such systems, and hypotheses underlying the proposed alternative coupling, are (i) that the presence of CO2 is the only driving force for chemical reactions and (ii) that its migration in the reservoir is only marginally affected by immobilisation due to chemical reactions. In the simplified coupling, the exposure time to CO2 of each element of the hydrodynamic grid is estimated by non-reactive simulations and the reaction path of one single batch geochemical model is applied to each grid element during its exposure time. In heterogeneous settings, analytical scaling relationships provide the dependency of velocity and amount of reactions to porosity and gas saturation. The analysis of TOUGHREACT fully coupled reactive transport simulations of CO2 injection in saline aquifer, inspired to the Ketzin pilot site (Germany), both in homogeneous and heterogeneous settings, confirms that the reaction paths predicted by fully coupled simulations in every element of the grid show a high degree of self-similarity. A threshold value for the minimum concentration of dissolved CO2 considered chemically active is shown to mitigate the effects of the discrepancy between dissolved CO2 migration in non-reactive and fully coupled simulations. In real life, the optimal threshold value is unknown and has to be estimated, e.g. by means of 1-D or 2-D simulations, resulting in an uncertainty ultimately due to the process de-coupling. However, such uncertainty is more than acceptable given that the alternative coupling enables using grids of the order of millions of elements, profiting from much better description of heterogeneous reservoirs at a fraction of the calculation time of fully coupled models.

  18. A coupling alternative to reactive transport simulations for long-term prediction of chemical reactions in heterogeneous CO2 storage systems

    NASA Astrophysics Data System (ADS)

    De Lucia, M.; Kempka, T.; Kühn, M.

    2014-09-01

    Fully-coupled, multi-phase reactive transport simulations of CO2 storage systems can be approximated by a simplified one-way coupling of hydrodynamics and reactive chemistry. The main characteristics of such systems, and hypotheses underlying the proposed alternative coupling, are (i) that the presence of CO2 is the only driving force for chemical reactions and (ii) that its migration in the reservoir is only marginally affected by immobilization due to chemical reactions. In the simplified coupling, the exposure time to CO2 of each element of the hydrodynamic grid is estimated by non-reactive simulations and the reaction path of one single batch geochemical model is applied to each grid element during its exposure time. In heterogeneous settings, analytical scaling relationships provide the dependency of velocity and amount of reactions to porosity and gas saturation. The analysis of TOUGHREACT fully coupled reactive transport simulations of CO2 injection in saline aquifer, inspired to the Ketzin pilot site (Germany), both in homogeneous and heterogeneous settings, confirms that the reaction paths predicted by fully coupled simulations in every element of the grid show a high degree of self-similarity. A threshold value for the minimum concentration of dissolved CO2 considered chemically active is showed to mitigate the effects of the discrepancy between dissolved CO2 migration in non-reactive and fully coupled simulations. In real life, the optimal threshold value is unknown and has to be estimated, e.g., by means of 1-D or 2-D simulations, resulting in an uncertainty ultimately due to the process de-coupling. However, such uncertainty is more than acceptable given that the alternative coupling enables using grids in the order of million elements, profiting from much better description of heterogeneous reservoirs at a fraction of the calculation time of fully coupled models.

  19. 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

  20. 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

  1. 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.

  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. 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

  4. Chemical modification of nanometric TiO2 particles by anchoring functional silane molecules in supercritical CO2

    NASA Astrophysics Data System (ADS)

    López-Periago, Ana M.; Sandoval, Wendy; Domingo, Concepción

    2014-03-01

    Supercritical carbon dioxide (scCO2) was used as a green solvent for the grafting of complex functional organosilanes containing nitrogen moieties on titanium dioxide (TiO2) nanoparticles using two strategies. The first strategy involved the preparation of two functional silanes, 4-nitrophenyl-(3-(trimethoxysilyl)-propyl)methanimine (NPTMS) and 4-(((3-(trimethoxysilyl)propyl)imino)methyl)-benzaldehyde (FPTMS) and further deposited under anhydrous conditions and scCO2 onto the TiO2 surface. The second strategy involved the scCO2 anhydrous deposition of bifunctional commercial silanes on the TiO2 surface. Two structures were synthesized. The first consisted in grafted TiO2 nanoparticles prepared by addition of the ligand, ((1R,2R)-N-(pyridin-2-ylmethyl)-2-(((E)-pyridin-2-ylmethylene) amino)-cyclohexan-1-amine (LPy-red), and designated as Ti-Cl-LPy-red. The second structure was synthesized by the reaction of (1,2)-diaminocylohexane (Dac), through the reactive site of 3-(Trimethoxysilyl)propyl methacrylate (MPTMS) previously deposited on the TiO2 surface and designated as Ti-MP-Dac. The synthesized silanes were characterized by ATR-FT and NMR spectroscopies and mass spectrometry. ATR-FT spectroscopy confirmed the presence of the silanes on the surface of the hybrid nanoparticles. Thermogravimetic analysis was used to estimate the loading of the silane grafted through both hydrogen and covalent bonding on the TiO2 surface. Further characterization of the solid samples was done by N2 adsorption-desorption and UV-vis diffuse reflectance.

  5. 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

  6. 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

  7. 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.

  8. 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

  9. 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.

  10. Chemical Changes in Pore Water Composition due to CO2 Injection Under In-Situ P-T Condition of the Altmark Gas Reservoir, Germany

    NASA Astrophysics Data System (ADS)

    Huq, F.; Nowak, M.; Haderlein, S.; Grathwohl, P.

    2012-12-01

    CO2 storage in depleted gas reservoir combined with enhanced gas recovery may be an economically feasible option to mitigate global warming. The Altmark gas field, located in the western part of the Northeast German Basin, is being considered as a potential candidate for this purpose. Under reservoir conditions (50 bars and 125°C), the CO2 saturated water causes dissolution and subsequent precipitation of minerals of the surrounding rock matrix. Therefore, the main objective of the current study was to investigate the chemical changes in fluid composition due to dissolution/precipitation of minerals under controlled laboratory conditions. A dry sandstone plug from the Altmark reservoir was mounted in a newly designed autoclave system and flushed by a pre-equilibrated mixture of water saturated with CO2 at a constant flow rate of 0.25 cm/h for 12 days at reservoir conditions. Fluid samples were taken at regular intervals for major and trace element analysis and pH was measured simultaneously in the partially de-gassed samples. Fluid analysis showed an increased concentration of Na, K and Cl ions at the beginning indicating early leaching of halite and sylvite which initially inhibited the dissolution of alkali feldspars. Feldspar dissolution occurred later and slower indicated by lower concentrations of Na and K reflecting the lower solubility and slow dissolution kinetics of feldspar. Dissolution of anhydrite was predominantly observed from the increased concentration of Ca and SO4 at earlier time periods. However, the Ca/SO4 molar ratio (>1) indicated the concurrent dissolution of both calcite and anhydrite. The presence of carbonates buffered the pH until day 6. Moreover, the mobilization of Mn, Mg, Ba and Fe might be derived from carbonate impurities. Thermodynamic calculations of mineral saturation indices enabled an evaluation of the CO2-water-rock interactions during the experiment and highlighted the dissolution of the Ca-bearing minerals in the studied

  11. 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. PMID:24577063

  12. 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.

  13. 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.

  14. 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.

  15. 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

    2016-02-01

    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. PMID:26752014

  16. 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.

  17. 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.

  18. 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.

  19. 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.

  20. Novel bifunctional catalysts based on crystalline multi-oxide matrices containing iron ions for CO2 hydrogenation to liquid fuels and chemicals.

    PubMed

    Utsis, N; Vidruk-Nehemya, R; Landau, M V; Herskowitz, M

    2016-07-01

    Seven solid mono-, bi- and tri-metallic oxide matrices where Fe(2+,3+) ions are distributed in different chemical/spatial environments were synthesized and characterized by XRD, N2-adsorption and EDAX methods. After basification with potassium, all matrices were activated by carburization or reduction-carburization under conditions selected based on the TPC/TPR spectra, tailoring the carburization extent of iron. The performances of the activated Fe-based catalysts with respect to CO2 conversion and C5+ selectivity were measured in a fixed-bed reactor under standard conditions in transient and continuous operation modes in units containing one or three reactors in series with water separations between the reactors. The catalysts were characterized by XRD, N2-adsorption, HRTEM-EELS and XPS before and after steady-state operation in the reactors. It was found that the rate of CO2 conversion is not limited by thermodynamic equilibrium but is strongly restricted by water inhibition and it depends on the nature of the Fe-oxide precursor. The ratio between the FTS and RWGS rates, which determines the C5+ hydrocarbons productivity, is strongly affected by the nature of the Fe-oxide matrix. The catalysts derived from the Fe-Al-O spinel and Fe-Ba-hexaaluminate precursors displayed the best balance of the two functions RFTS/RRWGS = 0.77-0.78. They were followed by magnetite, CuFe-delafossite, K-ferrite, Fe-La-hexaaluminate and LaFe-perovskite with a gradual lowering of RFTS/RRWGS from 0.60 to 0.15 and a gradual decrease in the C5+ productivity. The active sites that enhance the RWGS reaction are located on the surface of the Fe-oxide phases, while the FTS and methanation reactions occur on the surface of the Fe-carbide phases. PMID:27075823

  1. 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

  2. An obsession with CO2.

    PubMed

    Jones, Norman L

    2008-08-01

    The concept that underlies this paper is that carbon dioxide (CO2) removal is at least as important as the delivery of oxygen for maximum performance during exercise. Increases in CO2 pressure and reductions in the pH of muscle influence muscle contractile properties and muscle metabolism (via effects on rate-limiting enzymes), and contribute to limiting symptoms. The approach of Barcroft exemplified the importance of integrative physiology, in describing the adaptive responses of the circulatory and respiratory systems to the demands of CO2 production during exercise. The extent to which failure in the response of one system may be countered by adaptation in another is also explained by this approach. A key factor in these linked systems is the transport of CO2 in the circulation. CO2 is mainly (90%) transported as bicarbonate ions--as such, transport of CO2 is critically related to acid-base homeostasis. Understanding in this field has been facilitated by the approach of Peter Stewart. Rooted in classical physico-chemical relationships, the approach identifies the independent variables contributing to homeostasis--the strong ion difference ([SID]), ionization of weak acids (buffers, Atot) and CO2 pressure (PCO2). The independent variables may be reliably measured or estimated in muscle, plasma, and whole blood. Equilibrium conditions are calculated to derive the dependent variables--the most important being the concentrations of bicarbonate and hydrogen ions. During heavy exercise, muscle [H+] can exceed 300 nEq.L-1 (pH 6.5), mainly due to a greatly elevated PCO2 and fall in [SID] as a result of increased lactate (La-) production. As blood flows through active muscle, [La-] increase in plasma is reduced by uptake of La- and Cl- by red blood cells, with a resultant increase in plasma [HCO3-]. Inactive muscle contributes to homeostasis through transfer of La- and Cl- into the muscle from both plasma and red blood cells; this results in a large increase in [HCO3

  3. 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

  4. 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 ...

  5. 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.

  6. 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. PMID:25044300

  7. Low-temperature superficial chemical changes and post-entrapment effects alter CO2 budget estimation in vapor bubbles of glass inclusions

    NASA Astrophysics Data System (ADS)

    Robidoux, P.; Frezzotti, M. L.; Hauri, E. H.; Aiuppa, A.

    2015-12-01

    Quantifying the CO2 budget in glass inclusions containing a shrinkage bubble has become an important topic with the development of methodology based on microthermometry and micro-Raman measurements [1]. It is possible to determine CO2 in the shrinkage bubble and to calculate the bulk inclusion+bubble CO2 content, but should the methodology be refined for natural glass inclusion samples in a volcanic arc context ? We attempt to use the method for quantifying the major gas output (CO2, H2O, S, Cl) and understanding the evolution of gas mixture from melt and vapor at San Cristóbal volcano in the Central American Volcanic Arc (CAVA) by taking into account for the first time volatile contents of < 15 - 35 μm glass inclusions by using high spatial resolution/sensitivity NanoSIMS 50L ion microprobe. The presented approach focus on 16 - 527 ppm CO2 content in uncorrected glass inclusions with the presence of a shrinkage bubble and the added CO2 content could range between 550 - 1630 ppm. H2O in the bubble (1-X μm) was quantified with a Horiba Jobin Yvon HR800 micro-Raman spectrometer instrument by developing a curve spectrum correction method to isolate and put into evidence the Raman-Water-Liquid band from the glass-water band background, and by estimating their mass and volume with 1 μm imagery precision. Inside the glass inclusions, NanoSIMS multi-elements intensity imagery allowed to visualize the region where the intersected bubble is found and it should be avoided when programming NanoSIMS spots on the inclusion surface. Carbonates peaks were also detected along the vapor bubble walls by Raman and may be associated with unstable C-phases with a variety of low-°T minerals detected by SEM [2]. The presence of such low °T mineral phases must represent important low °T superficial and hydrothermal effects and may alter the CO2 budget estimation of primary melts at San Cristóbal. [1] Moore et al., 2015, Am. Mineral. 100, 806-823. [2] Kamenetsky et al., 2001, EPSL

  8. Reactive Transport Modeling of Effects of Different (Physical, Chemical and Computational) Factors on the Convection Process during CO2 Geological Sequestration in Deep Saline Aquifers

    NASA Astrophysics Data System (ADS)

    Zhang, W.; Wang, S.

    2014-12-01

    Density-driven convective activity can significantly accelerate the transformation of the injected CO2 from supercritical or gas phase into liquid phase, thus improving the long-term storage security. It is well known that the convective instability is only caused by the heterogeneity of porous medium. However, we found that numerical perturbation resulted from the spatial and temporal discretization and the convergence criteria will affect the modeling results. Partial simulation results as follows: (1) the increase in vertical permeability (kv) has a strong effect on the convection process compared to the increasing horizontal permeability. The higher kv also can accelerate the downward migration of fingers and the CO2 dissolution; (2) increase in magnitude of medium (porosity and permeability) perturbation promotes the onset of convective activity, but does not affect the evolution of convection. However, for same magnitudes of the medium perturbation, the modification in permeability can lead to a more rapid onset of convective activity than that in porosity; and (3) the geochemical reactions and mineral compositions are important not only to the CO2 dissolution, but also to the dissolution of other species from mineral dissolution, which both can increase the water density. In additional, 3D and 2D modeling results indicated that their effect on the convection onset is similar. The CO2 dissolution rate for the higher-resolution 3D model is greatly slower than that for the higher-resolution 2D model, due to the increase in dimension for 3D model enhances the interaction of fingers. However, we found that once the bottom boundary becomes important, the decrease in CO2 dissolution rate for the 2D model is more significant than that for the 3D model. This is because the more significant interaction of fingers in the 3D model than that in the 2D model delays the downward propagation of fingers and then the impact of the bottom boundary.

  9. Capnography: monitoring CO2.

    PubMed

    Casey, Georgina

    2015-10-01

    MONITORING RESPIRATORY and metabolic function by using capnography to measure end tidal carbon dioxide is standard practice in anaesthesia. It is also becoming more common in intensive care units and during procedural sedation. End tidal carbon dioxide (EtCO2) monitoring may also be used to assess effectiveness of cardiopulmonary resuscitation. Capnography is now emerging in general medical and surgical wards to monitor respiratory depression in patients using opioid analgesics. Using EtCO2 to monitor respiratory function offers many benefits over pulse oximetry. It is important to understand the differences between these two monitoring methods, and why capnography is increasingly favoured in many situations. An understanding of the physiological processes involved in CO2 excretion allows nurses to use capnography in a safe and meaningful way, while monitoring at-risk patients in acute care. PMID:26638570

  10. 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.

  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. Direct CO2-Methanation of flue gas

    NASA Astrophysics Data System (ADS)

    Müller, Klaus; Fleige, Michael; Rachow, Fabian; Israel, Johannes; Schmeißer, Dieter

    2013-04-01

    Already discovered by Paul Sabatier in 1902 the Hydrogenation according to CO2 + 4H2 ->CH4 + 2H2O nowadays is discussed in the course of the "Power-to-Gas" approach to utilize excess energy from renewable electricity generation in times of oversupply of electricity. We investigate the behavior of this process in a simulated flue gas atmosphere of conventional base load power plants, which could be used as constant sources of the reactant CO2. In relation to an approach related to carbon capture and cycling, the conversion of CO2 directly from the flue gas of a conventional power plant is a new aspect and has several advantages: The conversion of CO2 into methane could be integrated directly into the combustion process. Even older power plants could be upgraded and used as a possible source for CO2, in the same sense as the amine cleaning of flue gas, as a post combustion process. Further, waste heat of the power plant could be used as process energy for the catalytic reaction. Therefore the influence of different flue gas compositions such as varying contents of nitrogen and residual oxygen are tested in a laboratory scale. The heterogeneous catalysis process is investigated with regard to conversion rates, yield and selectivity and long-term stability of the Ni-catalyst. Also the influence of typical contaminations like SO2 is investigated and will be presented.

  13. Greenland CO2 and δ13C of CO2 - assigning the contamination

    NASA Astrophysics Data System (ADS)

    Jenk, T.; Rubino, M.; Etheridge, D.; Bigler, M.; Blunier, T.

    2012-04-01

    Analysis of air extracted from bubbles of Greenland ice results in considerably higher CO2 concentrations compared to records from Antarctic sites. This can not be explained by the inter-hemispheric gradient expected for past climatic conditions. Instead, it is attributed to chemical reactions between impurities in the ice, contributing excess CO2 to the atmospheric signal which was initially trapped in the bubbles. This is consistent with the fact that Greenland ice contains a significantly higher amount of impurities compared to Antarctic ice. Different candidates of CO2 producing chemical reactions were suggested by previous studies: (i) the acidification of carbonates, (ii) the oxidation of hydrocarbons and (iii) the photodecarboxilation of humic like substances. However, there is no agreement on how much each of the above reactions contributes. This study aims to identify the contribution from organic and inorganic sources to the Greenland CO2 excess. Compared to previous studies we base our analysis on an increased set of parameters and data points. We discuss data of CO2 and δ13C-CO2, both in high (2.5 cm) and low resolution (55 to 110 cm) along with parallel records of chemical impurities from three different sites in Greenland. The samples for the presented high resolution CO2 and δ13C of CO2 records were measured on a new set-up at the Centre for Ice and Climate (needle cracker, GC-IRMS).

  14. The role of chemical structure on the magnetic and electronic properties of Co2FeAl0.5Si0.5/Si(111) interface

    NASA Astrophysics Data System (ADS)

    Kuerbanjiang, Balati; Nedelkoski, Zlatko; Kepaptsoglou, Demie; Ghasemi, Arsham; Glover, Stephanie E.; Yamada, Shinya; Saerbeck, Thomas; Ramasse, Quentin M.; Hasnip, Philip J.; Hase, Thomas P. A.; Bell, Gavin R.; Hamaya, Kohei; Hirohata, Atsufumi; Lazarov, Vlado K.

    2016-04-01

    We show that Co2FeAl0.5Si0.5 film deposited on Si(111) has a single crystal structure and twin related epitaxial relationship with the substrate. Sub-nanometer electron energy loss spectroscopy shows that in a narrow interface region there is a mutual inter-diffusion dominated by Si and Co. Atomic resolution aberration-corrected scanning transmission electron microscopy reveals that the film has B2 ordering. The film lattice structure is unaltered even at the interface due to the substitutional nature of the intermixing. First-principles calculations performed using structural models based on the aberration corrected electron microscopy show that the increased Si incorporation in the film leads to a gradual decrease of the magnetic moment as well as significant spin-polarization reduction. These effects can have significant detrimental role on the spin injection from the Co2FeAl0.5Si0.5 film into the Si substrate, besides the structural integrity of this junction.

  15. 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.

  16. 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

  17. CO2 laser radar

    NASA Astrophysics Data System (ADS)

    Brown, D.; Callan, R.; Constant, G.; Davies, P. H.; Foord, R.

    CO2 laser-based radars operating at 10 microns are both highly energy-efficient and eye-safe, as well as compact and rugged; they also furnish covertness-enhancing fine pointing accuracy, and are difficult to jam or otherwise confuse. Two modes of operation are generally employed: incoherent, in which the laser is simply used as a high power illumination source, and in the presently elaborated coherent or heterodyne mode. Applications encompass terrain-following and obstacle avoidance, Doppler discrimination of missile and aircraft targets, pollutant gas detection, wind measurement for weapons-aiming, and global wind field monitoring.

  18. 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.

  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. Hydrocarbonaceous material upgrading method

    SciTech Connect

    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.

  1. 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.

  2. Modeling global atmospheric CO2 with improved emission inventories and CO2 production from the oxidation of other carbon species

    NASA Astrophysics Data System (ADS)

    Nassar, R.; Jones, D. B. A.; Suntharalingam, P.; Chen, J. M.; Andres, R. J.; Wecht, K. J.; Yantosca, R. M.; Kulawik, S. S.; Bowman, K. W.; Worden, J. R.; Machida, T.; Matsueda, H.

    2010-12-01

    The use of global three-dimensional (3-D) models with satellite observations of CO2 in inverse modeling studies is an area of growing importance for understanding Earth's carbon cycle. Here we use the GEOS-Chem model (version 8-02-01) CO2 mode with multiple modifications in order to assess their impact on CO2 forward simulations. Modifications include CO2 surface emissions from shipping (~0.19 Pg C yr-1), 3-D spatially-distributed emissions from aviation (~0.16 Pg C yr-1), and 3-D chemical production of CO2 (~1.05 Pg C yr-1). Although CO2 chemical production from the oxidation of CO, CH4 and other carbon gases is recognized as an important contribution to global CO2, it is typically accounted for by conversion from its precursors at the surface rather than in the free troposphere. We base our model 3-D spatial distribution of CO2 chemical production on monthly-averaged loss rates of CO (a key precursor and intermediate in the oxidation of organic carbon) and apply an associated surface correction for inventories that have counted emissions of CO2 precursors as CO2. We also explore the benefit of assimilating satellite observations of CO into GEOS-Chem to obtain an observation-based estimate of the CO2 chemical source. The CO assimilation corrects for an underestimate of atmospheric CO abundances in the model, resulting in increases of as much as 24% in the chemical source during May-June 2006, and increasing the global annual estimate of CO2 chemical production from 1.05 to 1.18 Pg C. Comparisons of model CO2 with measurements are carried out in order to investigate the spatial and temporal distributions that result when these new sources are added. Inclusion of CO2 emissions from shipping and aviation are shown to increase the global CO2 latitudinal gradient by just over 0.10 ppm (~3%), while the inclusion of CO2 chemical production (and the surface correction) is shown to decrease the latitudinal gradient by about 0.40 ppm (~10%) with a complex spatial structure

  3. Modeling global atmospheric CO2 with improved emission inventories and CO2 production from the oxidation of other carbon species

    SciTech Connect

    Nassar, Ray; Jones, DBA; Suntharalingam, P; Chen, j.; Andres, Robert Joseph; Wecht, K. J.; Yantosca, R. M.; Kulawik, SS; Bowman, K; Worden, JR; Machida, T; Matsueda, H

    2010-01-01

    The use of global three-dimensional (3-D) models with satellite observations of CO2 in inverse modeling studies is an area of growing importance for understanding Earth s carbon cycle. Here we use the GEOS-Chem model (version 8-02-01) CO2 mode with multiple modifications in order to assess their impact on CO2 forward simulations. Modifications include CO2 surface emissions from shipping (0.19 PgC yr 1), 3-D spatially-distributed emissions from aviation (0.16 PgC yr 1), and 3-D chemical production of CO2 (1.05 PgC yr 1). Although CO2 chemical production from the oxidation of CO, CH4 and other carbon gases is recognized as an important contribution to global CO2, it is typically accounted for by conversion from its precursors at the surface rather than in the free troposphere. We base our model 3-D spatial distribution of CO2 chemical production on monthly-averaged loss rates of CO (a key precursor and intermediate in the oxidation of organic carbon) and apply an associated surface correction for inventories that have counted emissions of CO2 precursors as CO2. We also explore the benefit of assimilating satellite observations of CO into GEOS-Chem to obtain an observation-based estimate of the CO2 chemical source. The CO assimilation corrects for an underestimate of atmospheric CO abundances in the model, resulting in increases of as much as 24% in the chemical source during May June 2006, and increasing the global annual estimate of CO2 chemical production from 1.05 to 1.18 Pg C. Comparisons of model CO2 with measurements are carried out in order to investigate the spatial and temporal distributions that result when these new sources are added. Inclusion of CO2 emissions from shipping and aviation are shown to increase the global CO2 latitudinal gradient by just over 0.10 ppm (3%), while the inclusion of CO2 chemical production (and the surface correction) is shown to decrease the latitudinal gradient by about 0.40 ppm (10%) with a complex spatial structure

  4. 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

  5. [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. PMID:22697030

  6. CO2 mineralization-bridge between storage and utilization of CO2.

    PubMed

    Geerlings, Hans; Zevenhoven, Ron

    2013-01-01

    CO2 mineralization comprises a chemical reaction between suitable minerals and the greenhouse gas carbon dioxide. The CO2 is effectively sequestered as a carbonate, which is stable on geological timescales. In addition, the variety of materials that can be produced through mineralization could find applications in the marketplace, which makes implementation of the technology more attractive. In this article, we review recent developments and assess the current status of the CO2 mineralization field. In an outlook, we briefly describe a few mineralization routes, which upon further development have the potential to be implemented on a large scale. PMID:23452171

  7. Ar + CO2 and He + CO2 Plasmas in ASTRAL

    NASA Astrophysics Data System (ADS)

    Boivin, R. F.; Gardner, A.; Munoz, J.; Kamar, O.; Loch, S.

    2007-11-01

    Spectroscopy study of the ASTRAL helicon plasma source running Ar + CO2 and He + CO2 gas mixes is presented. ASTRAL produces plasmas with the following parameters: ne = 10^10 - 10^13 cm-3, Te = 2 - 10 eV and Ti = 0.03 - 0.5 eV, B-field <= 1.3 kGauss, rf power <= 2 kWatt. A 0.33 m scanning monochromator is used for this study. Using Ar + CO2 gas mixes, very different plasmas are observed as the concentration of CO2 is changed. At low CO2 concentration, the bluish plasma is essentially atomic and argon transitions dominate the spectra. Weak C I and O I lines are present in the 750 - 1000 nm range. At higher CO2 concentration, the plasma becomes essentially molecular and is characterized by intense, white plasma columns. Here, spectra are filled with molecular bands (CO2, CO2^+, CO and CO^+). Limited molecular dissociative excitation processes associated with the production of C I and O I emission are also observed. On the other hand, He + CO2 plasmas are different. Here, rf matches are only possible at low CO2 concentration. Under these conditions, the spectra are characterized by strong C I and O I transitions with little or no molecular bands. Strong dissociative processes observed in these plasmas can be link to the high Te associated with He plasmas. An analysis of the spectra with possible scientific and industrial applications will be presented.

  8. 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.

  9. Modeling global atmospheric CO2 with improved emission inventories and CO2 production from the oxidation of other carbon species

    NASA Astrophysics Data System (ADS)

    Nassar, R.; Jones, D. B. A.; Suntharalingam, P.; Chen, J. M.; Andres, R. J.; Wecht, K. J.; Yantosca, R. M.; Kulawik, S. S.; Bowman, K. W.; Worden, J. R.; Machida, T.; Matsueda, H.

    2010-07-01

    The use of global three-dimensional (3-D) models with satellite observations of CO2 in inverse modeling studies is an area of growing importance for understanding Earth's carbon cycle. Here we use the GEOS-Chem model (version 8-02-01) CO2 simulation with multiple modifications in order to assess their impact on CO2 forward simulations. Modifications include CO2 surface emissions from shipping (~0.19 Pg C/yr), 3-D spatially-distributed emissions from aviation (~0.16 Pg C/yr), and 3-D chemical production of CO2 (~1.05 Pg C/yr). Although CO2 chemical production from the oxidation of CO, CH4 and other carbon gases is recognized as an important contribution to global CO2, it is typically accounted for by conversion from its precursors at the surface rather than in the free troposphere. We base our model 3-D spatial distribution of CO2 chemical production on monthly-averaged loss rates of CO (a key precursor and intermediate in the oxidation of organic carbon) and apply an associated surface correction for inventories that have counted emissions of carbon precursor as CO2. We also explore the benefit of assimilating satellite observations of CO into GEOS-Chem to obtain an observation-based estimate of the CO2 chemical source. The CO assimilation corrects for an underestimate of atmospheric CO abundances in the model, resulting in increases of as much as 24% in the chemical source during May-June 2006, and increasing the global annual estimate of CO2 chemical production from 1.05 to 1.18 Pg C. Comparisons of model CO2 with measurements are carried out in order to investigate the spatial and temporal distributions that result when these new sources are added. Inclusion of CO2 emissions from shipping and aviation are shown to increase the global CO2 latitudinal gradient by just over 0.10 ppm (~3%), while the inclusion of CO2 chemical production (and the surface correction) is shown to decrease the latitudinal gradient by about 0.40 ppm (~10%) with a complex spatial

  10. 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.

  11. 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

  12. 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

  13. 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.

  14. 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

  15. 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...

  16. 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.

  17. 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).

  18. 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

  19. 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).

  20. 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. PMID:27376177

  1. 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.

  2. Understanding urban atmospheric CO2: Challenges and Opportunities

    NASA Astrophysics Data System (ADS)

    Pataki, D. E.; Ehleringer, J. R.; Forster, C. B.; Klewicki, J. C.; Pardyjak, E. R.; Peterson, R. E.; Steenburgh, W. J.; Tyler, B. J.

    2004-12-01

    Many studies have shown that atmospheric CO2 concentrations are elevated far above ambient levels in cities due to strong local sources. Measurements of urban atmospheric CO2 mixing ratio, its isotopic composition, and its sources and sinks provide opportunities to understand the local carbon cycle and biogeochemistry of cities, which is increasingly important in studies of regional and global change as well as urban sustainability and planning. In an ongoing project in the Salt Lake Valley, Utah, measurements of CO2 mixing ratio and the isotopic composition of CO2 have shown that vehicle exhaust significantly elevates CO2 mixing ratios above ambient, particularly in the wintertime when temperature inversions create stable conditions. Natural gas combustion also makes a large contribution to CO2 mixing ratio in the winter, but becomes negligible in the summer. However, the urban "forest" in the Salt Lake Valley plays an active role in influencing CO2 mixing ratio during the spring, summer, and fall through photosynthesis and respiration. Atmospheric CO2 measurements in the Salt Lake Valley are also useful in that they correlate with air pollutants such as aerosols, particularly in the wintertime when CO2 sources are dominated by combustion. The relationship between CO2 mixing ratio and other pollutants varies as a function of fuel source (natural gas versus gasoline) and meteorological variables that affect atmospheric chemistry of reactive compounds; therefore, these relationships provide additional information about sources and sinks for atmospheric constituents. Finally, CO2 is a stable atmospheric tracer in that it does not undergo chemical transformations in the atmosphere. Measurements in the Salt Lake Valley showed that the temporal and spatial distribution of CO2 in the wintertime may provide information about atmospheric transport during complex cold pools events if mixing ratios are monitored at multiple locations. These results suggest that studies of

  3. 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.

  4. 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

  5. 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.

  6. CO2 Sequestration Crosswell Monitoring

    NASA Astrophysics Data System (ADS)

    Morency, C.; Luo, Y.; Tromp, J.

    2010-12-01

    Geologic sequestration of CO2, a green house gas, represents an effort to reduce the large amount of CO2 generated as a by-product of fossil fuels combustion and emitted into the atmosphere. This process of sequestration involves CO2 storage deep underground into highly permeable porous media sealed by caprock. "4D seismics" is a natural non-intrusive monitoring technique which involves 3D time-lapse seismic surveys. The success of monitoring CO2 movement relies upon a proper description of the physics of the problem. We realize time-lapse migrations comparing acoustic, elastic (with or without Gassmann's formulae), and poroelastic simulations of 4D seismic imaging. This approach highlights the influence of using different physical theories on interpreting seismic data, and, more importantly, on extracting the CO2 signature from the seismic wave field. We investigate various types of inversions using (1) P-wave traveltimes, (2) P- & S-wave traveltimes and (3) P- & S-wave traveltimes and amplitudes. Simulations are performed using a spectral-element method, and finite-frequency sensitivity kernels, used in the non-linear iterative inversions, are calculated based on an adjoint method. Biot's equations are implemented in the forward and adjoint simulations to account for poroelastic effects.

  7. Multiple timescales for neutralization of fossil fuel CO2

    NASA Astrophysics Data System (ADS)

    Archer, David; Kheshgi, Haroon; Maier-Reimer, Ernst

    The long term abiological sinks for anthropogenic CO2 will be dissolution in the oceans and chemical neutralization by reaction with carbonates and basic igneous rocks. We use a detailed ocean/sediment carbon cycle model to simulate the response of the carbonate cycle in the ocean to a range of anthropogenic CO2 release scenarios. CaCO3 will play only a secondary role in buffering the CO2 concentration of the atmosphere because CaCO3 reaction uptake capacity and kinetics are limited by the dynamics of the ocean carbon cycle. Dissolution into ocean water sequesters 70-80% of the CO2 release on a time scale of several hundred years. Chemical neutralization of CO2 by reaction with CaCO3 on the sea floor accounts for another 9-15% decrease in the atmospheric concentration on a time scale of 5.5-6.8 kyr. Reaction with CaCO3 on land accounts for another 3-8%, with a time scale of 8.2 kyr. The final equilibrium with CaCO3 leaves 7.5-8% of the CO2 release remaining in the atmosphere. The carbonate chemistry of the oceans in contact with CaCO3 will act to buffer atmospheric CO2 at this higher concentration until the entire fossil fuel CO2 release is consumed by weathering of basic igneous rocks on a time scale of 200 kyr.

  8. 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

  9. 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. PMID:25802049

  10. 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.

  11. 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

  12. 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

  13. Partial pressure of CO2 and CO2 emission in a monsoon-driven hydroelectric reservoir (Danjiangkou Reservoir), China

    NASA Astrophysics Data System (ADS)

    Li, S. Y.; Zhang, Q. F.

    2013-06-01

    Hydroelectric reservoirs have been under sampled to establish them as sources or sinks of the atmospheric carbon dioxide (CO2). Such poor coverage is well known for subtropic, particularly monsoon driven reservoirs in China. Our study presented the spatiotemporal changes of the carbonate system and CO2 flux in a hydroelectric reservoir (Dangjiankou Reservoir) locating in a subtropical monsoon climate region. Our 21 filed surveys conducted during 2004-2011 revealed significantly spatial and monthly variations of surface water partial pressure of CO2 (pCO2) in the Reservoir. pCO2, showing higher concentrations in the wet and warm seasons, averaged 595 ± 545 µatm (ranging from 53-3751 µatm) in the reservoir surface, while substantially higher pCO2 (1132 ± 1220 µatm) was observed in the river downstream the dam. A clear pCO2 drawdown in the reservoir as water flows demonstrated a significantly descending order of Dan Reservoir > site close to dam > Han Reservoir. This spatial contrast can also be seen in the distributions of dissolved inorganic carbon and total alkalinity. Pronounced seasonality in pCO2 was controlled by seasonal monsoon rainfall, while photosynthetic CO2 uptake dominated spatial patterns and dry-month variability of pCO2. We further related pCO2 to water chemical properties and indicated that pCO2 had strong positive correlations with Si, TP and DOC, negative correlations with DO saturation, TN and Chl a, while weak correlations with other variables including biogenic elements. CO2 flux from the Reservoir surface showed a bottom average of 9 mmol m-2 d-2 in comparison with other hydroelectric reservoir in China. River downstream the dam had quite high flux of CO2 (119 mmol m-2 d-2), which was intermediate between temperate rivers and compared to global rivers' average. This means that water releasing from reservoir would be an important channel for atmospheric CO2 sources. The annual CO2 emission from the Danjiangkou Reservoir was estimated to be

  14. Regional scale modeling of atmospheric CO2 over East Asia and comparison with satellite observations

    NASA Astrophysics Data System (ADS)

    Shim, C.

    2012-12-01

    East Asia is now the most important regions in terms of CO2 emissions and the analyzing accurate CO2 budget is critical issue for low-carbon policy. He we show the simulated regional scale CO2 distribution. The regional scale chemical transport model (WRF-Chem) was used with 50km x 50km resolution. The lateral boundary conditions were from GEOS-Chem CO2 simulations (with 2x2.5 degree resolution) where the chemical CO2 production and 3-D emissions from aviation were included. It is clear that the seasonal changes in north-south gradient of CO2 concentration over East Asia is shown by the model. In spring, the westerly transport of CO2 from north-east China is dominant, which increases the higher CO2 concentration in northern part of East Asia in the lower troposphere (< 2km). In contrast, the strong CO2 sink of vegetation from northern part of Asia and Siberia reduces CO2 concentration significantly in northern part of East Asia. The modeling results represent that the seasonal CO2 changes in the spatial distribution are affected by both the Chinese CO2 emissions and CO2 sinks from the vegetation. The modeling results are compared with the recent GOSAT CO2 column observations and stationary data. The regional CO2 modeling study will help the global low carbon policy for responding to recent climate change.

  15. 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

  16. Efficient electrochemical CO2 conversion powered by renewable energy

    DOE PAGESBeta

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

    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

  17. 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

  18. 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. PMID:25129845

  19. 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.

  20. 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.

  1. 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

  2. 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.

  3. 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.

  4. 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

  5. On the Formation of CO2 and Other Interstellar Ices

    NASA Astrophysics Data System (ADS)

    Garrod, R. T.; Pauly, T.

    2011-07-01

    We investigate the formation and evolution of interstellar dust-grain ices under dark-cloud conditions, with a particular emphasis on CO2. We use a three-phase model (gas/surface/mantle) to simulate the coupled gas-grain chemistry, allowing the distinction of the chemically active surface from the ice layers preserved in the mantle beneath. The model includes a treatment of the competition between barrier-mediated surface reactions and thermal-hopping processes. The results show excellent agreement with the observed behavior of CO2, CO, and water ice in the interstellar medium. The reaction of the OH radical with CO is found to be efficient enough to account for CO2 ice production in dark clouds. At low visual extinctions, with dust temperatures gsim12 K, CO2 is formed by direct diffusion and reaction of CO with OH; we associate the resultant CO2-rich ice with the observational polar CO2 signature. CH4 ice is well correlated with this component. At higher extinctions, with lower dust temperatures, CO is relatively immobile and thus abundant; however, the reaction of H and O atop a CO molecule allows OH and CO to meet rapidly enough to produce a CO:CO2 ratio in the range ~2-4, which we associate with apolar signatures. We suggest that the observational apolar CO2/CO ice signatures in dark clouds result from a strongly segregated CO:H2O ice, in which CO2 resides almost exclusively within the CO component. Observed visual-extinction thresholds for CO2, CO, and H2O are well reproduced by depth-dependent models. Methanol formation is found to be strongly sensitive to dynamical timescales and dust temperatures.

  6. 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. PMID:27020396

  7. Synthesis, characterization and application of alkanolamidines and alkanolguanidines in CO(2) capture

    SciTech Connect

    Koech, Phillip K; Heldebrant, David J; Lee, Suh-Jane; Rainbolt, James E; Smurthwaite, Tricia D

    2011-03-01

    Global carbon dioxide (CO2) emission to the atmosphere is partly responsible for climate change. In order to mitigate these environmental effects CO2 capture and storage is required. Solvents currently used for this application are the energy intensive aqueous amines. Here we present the synthesis, characterization and CO2 uptake of new advanced solvents called alkanolamidines and alkanolguanidines otherwise known as CO2-binding organic Liquids (CO2BOLs). These solvents have been designed to have decreased vapor pressure and low viscosity in order to increase the CO2 uptake capacity while minimizing evaporative losses. Alkanolamidines were synthesized in 1-3 steps from commercially available materials. These compounds bind CO2 chemically via the alcohol moiety forming zwitterionic alkylcarbonates. The alkanolamidines can be regenerated thermally by heating the alkylcarbonate to 75 °C. CO2 binding capacities up to 10 wt% were achieved using these compounds. These compounds have the potential to be energy efficient CO2 capture solvents.

  8. 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.

  9. Sources of excess CO2 in Greenland ice cores

    NASA Astrophysics Data System (ADS)

    Jenk, T. M.; Rubino, M.; Etheridge, D. M.; Bigler, M.; Blunier, T.

    2012-12-01

    Analysis of air extracted from bubbles of Greenland ice show higher CO2 concentrations compared to coeval data from Antarctica with unexpected high variations of several ppm CO2 in adjacent samples. Both offset and variations are too large to be of atmospheric origin such as the inter-hemispheric gradient and can also not be explained by analytical uncertainties. Higher ice temperatures and impurity content favour post depositional processes such as reactions between the contained chemical species; this could explain enhanced variability and higher CO2 concentrations in Greenlandic compared to Antarctic ice. Various chemical reaction mechanisms leading to such CO2 in-situ production have been proposed (i.e. acidification of carbonates, oxidation of aldehydes and photodecarboxilation of humic like substances). We tested the above hypotheses combining analysis of CO2, δ13C-CO2 and chemical impurities in samples of various age and depth resolution including three Greenlandic sites (Eurocore, GRIP, NGRIP) which allowed quantification of inorganic and organic source contribution to the observed excess CO2 by using an isotopic mass balance model. The model output was investigated by comparison to the reaction-specific tracers of chemical impurities. In agreement with previous studies, our results suggest that the amount of excess CO2 in Greenland ice increases with time. We find the isotopic signature of the excess CO2 to have a more negative δ13C compared to the coeval atmospheric value. The isotopic mass balance model attributes the excess CO2 to a combination of organic and inorganic sources. The contribution from the organic source is dominant and increases with time, pointing to ongoing production in the ice for more than 1000 years. The contribution of the carbonate source is much smaller, independent of the age of the ice and tendentially enhanced in layers associated with high peaks of dust concentrations. The mechanisms and kinetics of the involved processes

  10. 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.

  11. Molecular Dynamics Simulations of CO2/Water/Quartz Interfacial Properties: Impact of CO2 Dissolution in Water.

    PubMed

    Javanbakht, Gina; Sedghi, Mohammad; Welch, William; Goual, Lamia

    2015-06-01

    The safe trapping of carbon dioxide (CO2) in deep saline aquifers is one of the major concerns of CO2 sequestration. The amount of capillary trapping is dominated by the capillary pressure of water and CO2 inside the reservoir, which in turn is controlled by the interfacial tension (IFT) and the contact angle (CA) of CO2/water/rock systems. The measurement of IFT and CA could be very challenging at reservoir conditions, especially in the presence of toxic cocontaminants. Thus, the ability to accurately predict these interfacial properties at reservoir conditions is very advantageous. Although the majority of existing molecular dynamics (MD) studies of CO2/water/mineral systems were able to capture the trends in IFT and CA variations with pressure and temperature, their predictions often deviated from experimental data, possibly due to erroneous models and/or overlooked chemical reactions. The objective of this study was to improve the MD predictions of IFT and CA of CO2/water/quartz systems at various pressure and temperature conditions by (i) considering the chemical reactions between CO2 and water and (ii) using a new molecular model for α-quartz surface. The results showed that the presence of carbonic acid at the CO2/water interface improved the predictions of IFT, especially at low temperature and high pressure where more CO2 dissolution occurs. On the other hand, the effect on CA was minor. The slight decrease in CA observed across the pressure range investigated could be attributed to an increase in the total number of H-bonds between fluid molecules and quartz surface. PMID:25965772

  12. Reaction of CO2 and Carbonate Mineral in Seawater for Mitigation of CO2 and Ocean Acidity

    NASA Astrophysics Data System (ADS)

    Rau, G. H.

    2010-12-01

    A lab-scale seawater/mineral carbonate gas scrubber was found to remove up to 97% of CO2 in a simulated flue gas stream at ambient temperature and pressure, with a large fraction of this carbon ultimately converted to dissolved calcium bicarbonate. Contrary to predictions based on classical carbonate chemistry, up to 85% of the captured carbon was retained in solution, i.e., it did not degas or precipitate, even after full equilibration with air. This is because abiotic precipitation of CaCO3 from seawater is chemically inhibited up to dissolved concentrations approaching 20X supersaturation. Thus, above-ground CO2 hydration with seawater, reaction with mineral carbonate, and conversion to dissolved Ca(HCO3)2 may provide a relatively simple point-source CO2 capture and storage scheme at coastal locations. This approach is analogous to wet limestone scrubbing of flue gas that is commonly used for SO2 removal. Such low-tech CO2 mitigation could be especially relevant for retrofitting to existing coastal power plants and for deployment in the developing world, the primary source of future CO2 emissions. An electrochemically powered version of the preceding has been demonstrated for air capture of CO2. In any case, the addition of the resulting alkaline solution to the ocean would benefit marine ecosystems that are currently challenged by acidification. This is indicated by the widespread use of miniature CO2/carbonate mineral/seawater reactors in saltwater aquaria to generate alkalinity for preserving or enhancing coral and shellfish growth. Large-scale applications would thus allow use of the planet’s largest saline reservoir, the ocean, to safely and effectively store anthropogenic carbon in a form other than molecular CO2 or carbonic acid. This approach in essence hastens Nature's own very effective but slow CO2 mitigation process; carbonate mineral weathering is a major consumer of excess atmospheric CO2 and ocean acidity on geologic times scales.

  13. 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. PMID:27300565

  14. The Nanoscale Basis of CO2 Trapping for Geologic Storage.

    PubMed

    Bourg, Ian C; Beckingham, Lauren E; DePaolo, Donald J

    2015-09-01

    Carbon capture and storage (CCS) is likely to be a critical technology to achieve large reductions in global carbon emissions over the next century. Research on the subsurface storage of CO2 is aimed at reducing uncertainties in the efficacy of CO2 storage in sedimentary rock formations. Three key parameters that have a nanoscale basis and that contribute uncertainty to predictions of CO2 trapping are the vertical permeability kv of seals, the residual CO2 saturation Sg,r in reservoir rocks, and the reactive surface area ar of silicate minerals. This review summarizes recent progress and identifies outstanding research needs in these areas. Available data suggest that the permeability of shale and mudstone seals is heavily dependent on clay fraction and can be extremely low even in the presence of fractures. Investigations of residual CO2 trapping indicate that CO2-induced alteration in the wettability of mineral surfaces may significantly influence Sg,r. Ultimately, the rate and extent of CO2 conversion to mineral phases are uncertain due to a poor understanding of the kinetics of slow reactions between minerals and fluids. Rapidly improving characterization techniques using X-rays and neutrons, and computing capability for simulating chemical interactions, provide promise for important advances. PMID:26266820

  15. 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.

  16. 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

  17. Intelligent CO 2 beam guiding

    NASA Astrophysics Data System (ADS)

    Brecher, Christian; Stimpfl, Joffrey; Emonts, Michael

    The Fraunhofer IPT has recently developed a self-diagnosing laser system technology which can monitor the process parameters of all laser system components and supports the adjustment of the beam guidance of CO2 laser production systems with large ranges of travel. The intelligent system furthermore interprets the correlated laser beam parameter responses and proposes appropriate measures for preventive maintenance. The new assisted beam guidance adjustment bases upon active reflector modules adjusting with a large angular range of average ±0.8∘ at maximum resolution and a position-sensitive detector for the position of the pilot laser.

  18. 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.

  19. Ozone Radiative Feedback in Global Warming Simulations with CO2 and non-CO2 Forcings

    NASA Astrophysics Data System (ADS)

    Ponater, M.; Rieger, V.; Dietmüller, S.

    2015-12-01

    It has been found that ozone radiative feedback acts to reduce the climate sensitivity in global warming simulations including interactive atmospheric chemistry, if the radiative forcing origins from CO2 increase. The effect can be traced to a negative feedback from stratospheric ozone changes and it is amplified by a reduced positive feedback from stratospheric water vapor.These findings cannot be simply transferred to simulations in which the warming is driven by a non-CO2 radiative forcing. Using a perturbation of surface NOx and CO emissions as an example, we demonstrate that a tropospheric ozone feedback may have significant impacts on physical feedbacks. These interactions can act to an extent that the effect of a negative ozone feedback can be reversed by changes in other feedbacks, thus increasing the climate sensitivity instead of reducing it. We also address some conceptual issues showing up as chemical feedbacks are added to set of physical feedbacks in simulation with interactive chemistry.

  20. 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.

  1. 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.

  2. 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.

  3. Passive CO2 concentration in higher plants.

    PubMed

    Sage, Rowan F; Khoshravesh, Roxana

    2016-06-01

    Photorespiratory limitations on C3 photosynthesis are substantial in warm, low CO2 conditions. To compensate, certain plants evolved mechanisms to actively concentrate CO2 around Rubisco using ATP-supported CO2 pumps such as C4 photosynthesis. Plants can also passively accumulate CO2 without additional ATP expenditure by localizing the release of photorespired and respired CO2 around Rubisco that is diffusively isolated from peripheral air spaces. Passive accumulation of photorespired CO2 occurs when glycine decarboxylase is localized to vascular sheath cells in what is termed C2 photosynthesis, and through forming sheaths of chloroplasts around the periphery of mesophyll cells. The peripheral sheaths require photorespired CO2 to re-enter chloroplasts where it can be refixed. Passive accumulation of respiratory CO2 is common in organs such as stems, fruits and flowers, due to abundant heterotrophic tissues and high diffusive resistance along the organ periphery. Chloroplasts within these organs are able to exploit this high CO2 to reduce photorespiration. CO2 concentration can also be enhanced passively by channeling respired CO2 from roots and rhizomes into photosynthetic cells of stems and leaves via lacunae, aerenchyma and the xylem stream. Through passive CO2 concentration, C3 species likely improved their carbon economy and maintained fitness during episodes of low atmospheric CO2. PMID:27058940

  4. Optical properties of heusler alloys Co2FeSi, Co2FeAl, Co2CrAl, and Co2CrGa

    NASA Astrophysics Data System (ADS)

    Shreder, E. I.; Svyazhin, A. D.; Belozerova, K. A.

    2013-11-01

    The results of an investigation of optical properties and the calculations of the electronic structure of Co2FeSi, Co2FeAl, Co2CrAl, and Co2CrGa Heusler alloys are presented. The main focus of our attention is the study of the spectral dependence of the real part (ɛ1) and imaginary part (ɛ2) of the dielectric constant in the range of wavelengths λ = 0.3-13 μm using the ellipsometric method. An anomalous behavior of the optical conductivity σ(ω) has been found in the infrared range in the Co2CrAl and Co2CrGa alloys, which differs substantially from that in the Co2FeSi and Co2FeAl alloys. The results obtained are discussed based on the calculations of the electronic structure.

  5. CO2 laser frequency multiplication

    SciTech Connect

    Not Available

    1992-03-01

    The duration of the mode-locked CO(2) laser pulses was measured to be 0.9 + or - nsec by the technique of (second harmonic) autocorrelation. Knowing the pulse duration, the spot size, and the harmonic conversion efficiency, a detailed fit of experiment to theory gave an estimate of the nonlinear coefficient of AgGaSe(2). d36 = 31 + or - V(1), in agreement with the most accurate literature values. A number of experiments were made with longer pulse trains in which the highest harmonic energy conversion reached 78%. The damage threshold was measured and it turned out to be related much more strongly to fluence than intensity. The shorter pulse trains had peak intensities of close to 300 MW 1/cm squared whereas the longer trains (3 usec) had intensities up to 40 MW 1/cm squared.

  6. New Insights into CO2 Absorption Mechanisms with Amino-Acid Ionic Liquids.

    PubMed

    Yang, Qiwei; Wang, Zhiping; Bao, Zongbi; Zhang, Zhiguo; Yang, Yiwen; Ren, Qilong; Xing, Huabin; Dai, Sheng

    2016-04-21

    The last decade saw an explosion of interest in using amine-functionalized materials for CO2 capture and conversion, and it is of great importance to elucidate the relationship between the molecular structure of amine-functionalized materials and their CO2 capacity. In this work, based on a new quantitative analysis method for the CO2 absorption mechanism of amino-acid ionic liquids (ILs) and quantum chemical calculations, we show that the small difference in the local structure of amine groups in ILs could lead to much different CO2 absorption mechanisms, which provides an opportunity for achieving higher CO2 capacity by structure design. This work revealed that the actual CO2 absorption mechanism by amino-acid ILs goes beyond the apparent CO2 /amine stoichiometry; a rigid ring structure around the amine group in ILs creates a unique electrostatic environment that inhibits the deprotonation of carbamic acid and enables actually equimolar CO2 /amine absorption. PMID:27061812

  7. 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

    NASA Astrophysics Data System (ADS)

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

    2014-06-01

    NMR spectroscopy (1H, 13C, 15N) 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 (CS32-). 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] CS2 is

  8. Sequestration of CO2 by halotolerant algae

    PubMed Central

    2014-01-01

    The potential of halotolerant algae isolated from natural resources was used to study CO2 fixation and algal lipid production. Biological fixation of CO2 in photobioreactor in presence of salinity is exploited. The CO2 concentration 1060 ppm gave the highest biomass yield (700 mg dry wt/l), the highest total lipid content (10.33%) with 80% of CO2 removal. PMID:24847439

  9. 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.

  10. Investigation of CO2 release pressures in pipeline cracks

    NASA Astrophysics Data System (ADS)

    Gorenz, Paul; Herzog, Nicoleta; Egbers, Christoph

    2013-04-01

    The CCS (Carbon Capture and Storage) technology can prevent or reduce the emissions of carbon dioxide. The main idea of this technology is the segregation and collection of CO2 from facilities with a high emission of that greenhouse gas, i.e. power plants which burn fossil fuels. To segregate CO2 from the exhaust gas the power plant must be upgraded. Up to now there are three possible procedures to segregate the carbon dioxide with different advantages and disadvantages. After segregation the carbon dioxide will be transported by pipeline to a subsurface storage location. As CO2 is at normal conditions (1013,25 Pa; 20 °C) in a gaseous phase state it must be set under high pressure to enter denser phase states to make a more efficient pipeline transport possible. Normally the carbon dioxide is set into the liquid or supercritical phase state by compressor stations which compress the gas up to 15 MPa. The pressure drop makes booster stations along the pipeline necessary which keep the CO2 in a dens phase state. Depending on the compression pressure CO2 can be transported over 300km without any booster station. The goal of this work is the investigation of release pressures in pipeline cracks. The high pressurised pipeline system consists of different parts with different failure probabilities. In most cases corrosion or obsolescence is the reason for pipeline damages. In case of a crack CO2 will escape from the pipeline and disperse into the atmosphere. Due to its nature CO2 can remain unattended for a long time. There are some studies of the CO2 dispersion process, e.g. Mazzoldi et al. (2007, 2008 and 2011) and Wang et al. (2008), but with different assumptions concerning the pipeline release pressures. To give an idea of realistic release pressures investigations with the CFD tool OpenFOAM were carried out and are presented within this work. To cover such a scenario with an accidental release of carbon dioxide a pipeline section with different diameters and

  11. Photosynthesis in a CO2 rich atmosphere

    Technology Transfer Automated Retrieval System (TEKTRAN)

    The concentration of CO2 ([CO2]) in the atmosphere is projected to reach ~550 ppm by 2050. C3 plants respond directly to growth at elevated [CO2] via stimulated photosynthesis and reduced stomatal conductance. The enhancement of photosynthesis is the result of increased velocity of carboxylation of ...

  12. CO2 mitigation via accelerated limestone weathering

    USGS Publications Warehouse

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

    2004-01-01

    The climate and environmental impacts of the current, carbon-intensive energy usage demands that effective and practical energy alternatives and CO2 mitigation strategies be found. A discussion on CO2 mitigation via accelerated limestone weathering covers limestone and seawater availability and cost; reaction rates and densities; effectiveness in CO2 sequestration; and environmental impacts and benefits.

  13. Recent Trends in Atmospheric 14CO2

    NASA Astrophysics Data System (ADS)

    Turnbull, J. C.; Rayner, P.; Bousquet, P.; Cozic, A.; Miller, J. B.; Lehman, S. J.; Peters, W.; Tans, P. P.; Ciais, P.

    2007-12-01

    The radiocarbon content of atmospheric CO2 (14CO2) varies due to a number of factors. After the near-doubling of the 14CO2 loading in the early 1960s (due to atmospheric nuclear weapons testing), many studies examined the fate of this 'bomb 14C' to understand exchange processes of CO2 with the surface reservoirs. Today, however, the atmosphere and surface reservoirs are close to equilibrium with respect to bomb 14C, and instead, changes in 14CO2 more strongly reflect the response to the addition of 14C-free fossil fuel CO2 to the atmosphere. We use an atmospheric transport model to simulate recent atmospheric 14CO2, and compare this to observations at several sites over the Northern Hemisphere continents. We show that, in the Northern Hemisphere, 14CO2 variability is dominated by the effect of fossil fuel CO2 emissions. The model simulates the time trends quite well, including both the overall secular trend and the seasonal cycle. A seasonal cycle in 14CO2 is observed at the high altitude sites of Niwot Ridge, Colorado, and Jungfraujoch, Switzerland, but the magnitude varies from year to year. Our modeling studies demonstrate that this inter-annual variability can be explained by differences in atmospheric transport. This is in contrast to CO2 concentration seasonal cycles, which are dominated by seasonal changes in CO2 source strengths.

  14. Using CO2:CO Correlations to Improve Inverse Analyses of Carbon Fluxes

    NASA Technical Reports Server (NTRS)

    Palmer, Paul I.; Suntharalingam, Parvadha; Jones, Dylan B. A.; Jacob, Daniel J.; Streets, David G.; Fu, Qingyan; Vay, Stephanie A.; Sachse, Glen W.

    2006-01-01

    Observed correlations between atmospheric concentrations of CO2 and CO represent potentially powerful information for improving CO2 surface flux estimates through coupled CO2-CO inverse analyses. We explore the value of these correlations in improving estimates of regional CO2 fluxes in east Asia by using aircraft observations of CO2 and CO from the TRACE-P campaign over the NW Pacific in March 2001. Our inverse model uses regional CO2 and CO surface fluxes as the state vector, separating biospheric and combustion contributions to CO2. CO2-CO error correlation coefficients are included in the inversion as off-diagonal entries in the a priori and observation error covariance matrices. We derive error correlations in a priori combustion source estimates of CO2 and CO by propagating error estimates of fuel consumption rates and emission factors. However, we find that these correlations are weak because CO source uncertainties are mostly determined by emission factors. Observed correlations between atmospheric CO2 and CO concentrations imply corresponding error correlations in the chemical transport model used as the forward model for the inversion. These error correlations in excess of 0.7, as derived from the TRACE-P data, enable a coupled CO2-CO inversion to achieve significant improvement over a CO2-only inversion for quantifying regional fluxes of CO2.

  15. 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. ...

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

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

  17. Solvation of Esters and Ketones in Supercritical CO2.

    PubMed

    Kajiya, Daisuke; Imanishi, Masayoshi; Saitow, Ken-ichi

    2016-02-01

    Vibrational Raman spectra for the C═O stretching modes of three esters with different functional groups (methyl, a single phenyl, and two phenyl groups) were measured in supercritical carbon dioxide (scCO2). The results were compared with Raman spectra for three ketones involving the same functional groups, measured at the same thermodynamic states in scCO2. The peak frequencies of the Raman spectra of these six solute molecules were analyzed by decomposition into the attractive and repulsive energy components, based on the perturbed hard-sphere theory. For all solute molecules, the attractive energy is greater than the repulsive energy. In particular, a significant difference in the attractive energies of the ester-CO2 and ketone-CO2 systems was observed when the methyl group is attached to the ester or ketone. This difference was significantly reduced in the solute systems with a single phenyl group and was completely absent in those with two phenyl groups. The optimized structures among the solutes and CO2 molecules based on quantum chemical calculations indicate that greater attractive energy is obtained for a system where the oxygen atom of the ester is solvated by CO2 molecules. PMID:26741296

  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. PMID:25656300

  19. Sensitivity of geochemical monitoring for CO2 sequestration in basalt

    NASA Astrophysics Data System (ADS)

    Zakharova, N. V.; Goldberg, D.; Herron, M.; Grau, J.

    2010-12-01

    Continental flood basalts is a promising target for carbon dioxide (CO2) storage due to high storage capacity, presence of seals, and potential for geochemical trapping which results in binding CO2 into stable carbonate minerals. The success of long-term CO2 storage in igneous rocks highly depends on our ability to monitor mineralization under in situ conditions. The direct chemistry measurements on cores are costly and typically do not provide continuous coverage. In this study we investigate the potential of borehole geochemical logging for monitoring of CO2 mineralization in basalt. Neutron-induced capture gamma ray spectroscopy tools allow obtaining in-situ concentration logs for up to 10 major elements which can be used to construct a quantitative mineralogical model. While this usually provides good bulk mineralogy estimates, detecting small-volume mineral alteration in volcanic rocks remains challenging, especially if borehole conditions are poor. We analyze Schlumberger Elemental Capture Spectroscopy logs and chemical core analysis from the pilot CO2 sequestration project in the Columbia River flood basalt. We use the geochemical spectroscopy logs and quantitative modeling to quantify their sensitivity to secondary mineralization in basalt. We apply statistical analysis to explain the variance in elemental concentrations (and other logs) and establish detection limits for various mineral alteration products in basalt. We use these results to evaluate monitoring capabilities and limitations of geochemical logging for CO2 mineralization after underground injection in basalt and suggest areas for future research.

  20. Continuous Measurement of CO2 concentration in Arctic Soil by Small Open-path Type CO2 Sensors

    NASA Astrophysics Data System (ADS)

    Nakamoto, K.; Oechel, W. C.; Lipson, D.

    2006-12-01

    Permafrost and seasonally thawed Arctic soils in high northern latitudes hold approximately 25 percent of the world's soil organic carbon. The predicted warming of the Arctic, coupled with regional drying, could release much of the carbon now stored in the Arctic soils. Understanding the mechanisms controlling the release of soil organic carbon as CO2 is critical to predicting sensitive Arctic soils will respond to and influence global climate change. However, there are only a few reports of soil respiration, and very few that report continuous respiration rates. The results of chamber measurements give the overall efflux from the surface and emphasize biological and chemical processes and controls. However, they do not measure soil CO2 concentrations. To our knowledge, continuous measurements of soil CO2 concentration has not been previously conducted in the Arctic, and gas diffusivity of Arctic soils that thaw and freeze are poorly known. To obtain a better understanding of the patterns and controls on carbon release from Arctic soils, long-term measurements of soil respiration and an investigation of the underlying processes were undertaken. In this study, continuous measurements of soil CO2 concentration by small open path type infrared gas analyzers in a revegetated Arctic drained lake basin at Barrow Alaska was undertaken. Measurements were conducted from the beginning of soil thaw in summer through the following winter and summer. Changes in soil CO2 concentration during freezing and thawing processes proved especially interesting. Soil CO2 concentration in the organic layer of the drained lake basin was much higher than that of Typic Psamomoturbals soil from heath vegetation cover in Greenland (Elberling and Brandt 2003) throughout the thawing season. Soil CO2 increased with increasing soil temperature and thaw depth reflecting CO2 production in the soil. Soil CO2 concentration was greater in relatively wet soil than in dry soil. Soil CO2 concentration

  1. 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

  2. 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. PMID:9734452

  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. 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.

  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. High Temperature CO2 Treatments for Inshell Walnuts

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Environmental restrictions on those fumigants currently used to disinfest inshell walnuts of field pests require that non-chemical alternatives be considered. Earlier work found that 98% CO2 at 43C for 7.3 hours should be an effective phytosanitary treatment for these insects, as it is the estimated...

  8. CO2/H(+) sensing: peripheral and central chemoreception.

    PubMed

    Lahiri, Sukhamay; Forster, Robert E

    2003-10-01

    H(+) is maintained constant in the internal environment at a given body temperature independent of external environment according to Bernard's principle of "milieu interieur". But CO2 relates to ventilation and H(+) to kidney. Hence, the title of the chapter. In order to do this, sensors for H(+) in the internal environment are needed. The sensor-receptor is CO2/H(+) sensing. The sensor-receptor is coupled to integrate and to maintain the body's chemical environment at equilibrium. This chapter dwells on this theme of constancy of H(+) of the blood and of the other internal environments. [H(+)] is regulated jointly by respiratory and renal systems. The respiratory response to [H(+)] originates from the activities of two groups of chemoreceptors in two separate body fluid compartments: (A) carotid and aortic bodies which sense arterial P(O2) and H(+); and (B) the medullary H(+) receptors on the ventrolateral medulla of the central nervous system (CNS). The arterial chemoreceptors function to maintain arterial P(O2) and H(+) constant, and medullary H(+) receptors to maintain H(+) of the brain fluid constant. Any acute change of H(+) in these compartments is taken care of almost instantly by pulmonary ventilation, and slowly by the kidney. This general theme is considered in Section 1. The general principles involving cellular CO2 reactions mediated by carbonic anhydrase (CA), transport of CO2 and H(+) are described in Section 2. Since the rest of the chapter is dependent on these key mechanisms, they are given in detail, including the role of Jacobs-Stewart Cycle and its interaction with carbonic anhydrase. Also, this section deals briefly with the mechanisms of membrane depolarization of the chemoreceptor cells because this is one mechanism on which the responses depend. The metabolic impact of endogenous CO2 appears in the section with a historical twist, in the context of acclimatization to high altitude (Section 3). Because low P(O2) at high altitude stimulates

  9. Residual CO2 trapping in Indiana limestone.

    PubMed

    El-Maghraby, Rehab M; Blunt, Martin J

    2013-01-01

    We performed core flooding experiments on Indiana limestone using the porous plate method to measure the amount of trapped CO(2) at a temperature of 50 °C and two pressures: 4.2 and 9 MPa. Brine was mixed with CO(2) for equilibration, then the mixture was circulated through a sacrificial core. Porosity and permeability tests conducted before and after 884 h of continuous core flooding confirmed negligible dissolution. A trapping curve for supercritical (sc)CO(2) in Indiana showing the relationship between the initial and residual CO(2) saturations was measured and compared with that of gaseous CO(2). The results were also compared with scCO(2) trapping in Berea sandstone at the same conditions. A scCO(2) residual trapping end point of 23.7% was observed, indicating slightly less trapping of scCO(2) in Indiana carbonates than in Berea sandstone. There is less trapping for gaseous CO(2) (end point of 18.8%). The system appears to be more water-wet under scCO(2) conditions, which is different from the trend observed in Berea; we hypothesize that this is due to the greater concentration of Ca(2+) in brine at higher pressure. Our work indicates that capillary trapping could contribute to the immobilization of CO(2) in carbonate aquifers. PMID:23167314

  10. 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

  11. Reduction of CO2 by pyridine monoimine molybdenum carbonyl complexes: Cooperative metal-ligand binding of CO2

    PubMed Central

    Sieh, Daniel; Lacy, David C.; Peters, Jonas C.

    2015-01-01

    ArPMI-Mo(CO)4 complexes (PMI = pyridine monoimine; Ar = Ph, 2,6-di-iso-propylphenyl) were synthesized and their electrochemical properties were probed with cyclic voltammetry and infrared spectroelectrochemistry (IR-SEC). The complexes exhibit a reduction at more positive potentials than the related bipyridine-Mo(CO)4 complex, which is ligand based according to IR-SEC and DFT data. To probe the reaction product in more detail, stoichiometric chemical reduction and subsequent treatment with CO2 resulted in the formation of a new product that is assigned as a ligand-bound carboxylate, [iPr2PhPMI-Mo(CO)3(CO2)]2−, by NMR spectroscopic methods. The CO2 adduct [iPr2PhPMI-Mo(CO)3(CO2)]2− could not be isolated and fully characterized. However, the assignment of the C-C coupling between the CO2 molecule and the PDI ligand was confirmed by X-ray crystallography of one of the decomposition products of [iPr2PhPMI-Mo(CO)3(CO2)]2−. PMID:25924730

  12. Reduction of CO2 by Pyridine Monoimine Molybdenum Carbonyl Complexes: Cooperative Metal-Ligand Binding of CO2.

    PubMed

    Sieh, Daniel; Lacy, David C; Peters, Jonas C; Kubiak, Clifford P

    2015-06-01

    [((Ar) PMI)Mo(CO)4 ] complexes (PMI=pyridine monoimine; Ar=Ph, 2,6-di-iso-propylphenyl) were synthesized and their electrochemical properties were probed with cyclic voltammetry and infrared spectroelectrochemistry (IR-SEC). The complexes undergo a reduction at more positive potentials than the related [(bipyridine)Mo(CO)4 ] complex, which is ligand based according to IR-SEC and DFT data. To probe the reaction product in more detail, stoichiometric chemical reduction and subsequent treatment with CO2 resulted in the formation of a new product that is assigned as a ligand-bound carboxylate, [( iPr 2PhPMI)Mo(CO)3 (CO2 )](2-) , by NMR spectroscopic methods. The CO2 adduct [( iPr 2PhPMI)Mo(CO)3 (CO2 )](2-) could not be isolated and fully characterized. However, the C-C coupling between the CO2 molecule and the PDI ligand was confirmed by X-ray crystallographic characterization of one of the decomposition products of [( iPr 2PhPMI)Mo(CO)3 (CO2 )](2-) . PMID:25924730

  13. 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.

  14. 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).

  15. Geophysical Implications of Enceladus' CO2 Frost

    NASA Astrophysics Data System (ADS)

    Matson, D.; Davies, A. G.; Johnson, T. V.; Castillo, J. C.; Lunine, J. I.

    2013-12-01

    CO2 frost has been reported on the surface of Enceladus [1]. We suggest that the frost originated from shallow gas pockets below the surface. These pockets are a natural consequence of the ocean water circulation hypothesis [2]. They are different from the plume chambers [3] and would constitute a previously unrecognized structure in the surface. The oceanic circulation uses gas bubbles to make seawater buoyant and bring up water, chemicals, and heat from a warm ocean at depth [2]. The ocean water rises through the icy crust and near the surface it spreads out laterally beneath a relatively thin ice cap, following the pattern indicated by the thermal anomalies identified in Cassini data [4,5]. Topography on the bottom of this cap ice is conducive to the formation of gas pockets. As the ocean water flows horizontally, the gas bubbles in it continue to rise vertically. Even though their vertical migration may be slow and even if the flow is relatively turbulent, some bubbles reach recesses in the bottom of the ice cap and, over time, pop and form gas pockets. The gas pockets are envisioned as being ruptured by the regular fissuring of ice in the South Polar Region. Hurford et al. [6] have modelled the tidally controlled openings of rifts in the SPR. If one of these rifts reaches a gas pocket, CO2 gas may come to the surface. The tortuosity and other properties of its route will determine if it vents as a seep or a jet. If enough gas is vented and the molecules in the transient cloud have many collisions, some of them will be scattered to the surface and freeze. It was noted by Brown, et al. [1] that the frost deposits may not be permanent and that an active replenishment processes might be necessary. Studies of CO2 frost on Iapetus suggest that migration can be significant [7]. This work was performed at the Jet Propulsion Laboratory, California Institute of Technology, under contract to NASA. al., Science 311, 1425-1428, 2006. [2] Matson D. L. et al., Icarus 221, 53

  16. 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. PMID:26596773

  17. 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.

  18. 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.

  19. Covalent Organic Frameworks for CO2 Capture.

    PubMed

    Zeng, Yongfei; Zou, Ruqiang; Zhao, Yanli

    2016-04-01

    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. PMID:26924720

  20. Radiocarbon in Tree STEM CO2 Efflux

    NASA Astrophysics Data System (ADS)

    Muhr, J.; Czimczik, C. I.; Angert, A.; Trumbore, S.

    2011-12-01

    Carbon dioxide efflux from tree stems can be a significant component of the stand-level carbon balance. Recent studies have demonstrated that tree stem CO2 efflux may reflect more than just in-situ respiration but also transport from other locations and it has been suggested that it may also include C originally respired in roots or even uptake of soil CO2. We report measurements of the radiocarbon signature of carbon emitted from a range of mature tree stems in tropical and temperate forest ecosystems. Comparison of the radiocarbon signature of respired CO2 with the observed rate of decline in atmsopheric 14C-CO2 provides a measure of the time elapsed between C fixation by the plant and its return to the atmosphere as stem CO2 efflux. In all investigated trees, we observed that stem CO2 efflux had higher radiocarbon signatures than the contemporary atmospheric 14C-CO2, and therefore was derived from C fixed one to several years earlier. In tropical forest trees, we found that the 14C signature of CO2 within the stem (~4-5 cm depth) had even higher radiocarbon signatures than the stem CO2 efflux. In one of the investigated tree species, the in-stem CO2 was derived from C sources fixed on average ~20 years previously. These results confirm observations of root-respired CO2 that also have shown contributions of C substrates older than recent photosynthetic products, and the presence of extracable C reserves in wood that reflect the presence of older C sources. Our results imply that stem CO2 efflux is not only derived from respiration of recent photosynthetic products but includes contributions from older, stored C pools. Ongoing investigations will enable us to compare CO2 efflux for trees subjected to experimental drought, and using different life strategies (deciduous versus evergreen oaks) to determine if the use of these older C stores varies with stress.

  1. 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

  2. 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. PMID:25808519

  3. Preliminary Constraints on Fossil-fuel CO2: Comparison of Tracers CO and SF6 With Measurements of 14CO2

    NASA Astrophysics Data System (ADS)

    Turnbull, J. C.; Miller, J. B.; Lehman, S. J.; Sparks, R. J.; Tans, P. P.

    2004-12-01

    CO2 derived from the combustion of fossil fuels is a significant component of the carbon balance of North America. However, on the sub-continental spatial scales and sub-annual time scales relevant to the objectives of the North American Carbon Program, estimates of combustion CO2 from traditional economic inventories are unlikely to be accurate, and may contribute to biases in the interpretation of atmospheric CO2 measurements. Indirect estimates of the combustion CO2 component can also be obtained from measured CO:CO2 ratios and SF6:CO2 ratios. The low cost and ease of measurement allow the application of these methods in intensive measurement campaigns. However, the accuracy of the combustion CO2 detection capability relies on accurately determining the emission ratio of CO:CO2 or SF6:CO2 at relevant time and space scales. In the case of CO, atmospheric chemical biases and non fossil fuel sources must also be understood. CO2 derived from fossil fuels contains no 14C, whereas other sources have a 14C content close to that of ambient air. Measurement of the 14C content in CO2 thus provides a direct tracer for fossil fuel derived CO2, without the biases associated with the indirect tracer methods. We used high-precision accelerator mass spectrometry to determine the 14C content of CO2 at several North American sites (Niwot Ridge, CO, Harvard Forest, MA and New Hampshire) during 2003 and 2004, and calculate the fossil fuel CO2 contribution in each case. We compare these results with CO:CO2 and SF6:CO2 measurements on the same samples to evaluate the indirect tracer methods at these sites. Preliminary results for wintertime measurements (when biological CO2 exchange fluxes are small) support the accuracy of the 14C method. The back-calculated emission ratios for SF6:CO2 vary significantly and consistently underestimate the global average. While the back-calculated CO:CO2 ratios are more consistent, they also underestimate the predicted values from emissions

  4. Development of optical MEMS CO2 sensors

    NASA Astrophysics Data System (ADS)

    McNeal, Mark P.; Moelders, Nicholas; Pralle, Martin U.; Puscasu, Irina; Last, Lisa; Ho, William; Greenwald, Anton C.; Daly, James T.; Johnson, Edward A.; George, Thomas

    2002-09-01

    Inexpensive optical MEMS gas and chemical sensors offer chip-level solutions to environmental monitoring, industrial health and safety, indoor air quality, and automobile exhaust emissions monitoring. Previously, Ion Optics, Inc. reported on a new design concept exploiting Si-based suspended micro-bridge structures. The devices are fabricated using conventional CMOS compatible processes. The use of photonic bandgap (PBG) crystals enables narrow band IR emission for high chemical selectivity and sensitivity. Spectral tuning was accomplished by controlling symmetry and lattice spacing of the PBG structures. IR spectroscopic studies were used to characterize transmission, absorption and emission spectra in the 2 to 20 micrometers wavelength range. Prototype designs explored suspension architectures and filament geometries. Device characterization studies measured drive and emission power, temperature uniformity, and black body detectivity. Gas detection was achieved using non-dispersive infrared (NDIR) spectroscopic techniques, whereby target gas species were determined from comparison to referenced spectra. A sensor system employing the emitter/detector sensor-chip with gas cell and reflective optics is demonstrated and CO2 gas sensitivity limits are reported.

  5. Global CO2 Emission from Volcanic Lakes

    NASA Astrophysics Data System (ADS)

    Perez, N.; Hernandez Perez, P. A.; Padilla, G.; Melian Rodriguez, G.; Padron, E.; Barrancos, J.; Calvo, D.; Kusukabe, M.; Mori, T.; Nolasco, D.

    2009-12-01

    During the last two decades, scientists have paid attention to CO2 volcanic emissions and its contribution to the global C budget. Excluding MORBs as a net source of CO2 to the atmosphere, the global CO2 discharge from subaerial volcanism has been estimated about 300 Mt y-1 and this rate accounts for both visible (plume & fumaroles) and non-visible (diffuse) volcanic gas emanations (Mörner & Etíope, 2002). However, CO2 emissions from volcanic lakes have not been considered to estimate the global CO2 discharge from subaerial volcanoes. In order to improve this global CO2 emission rate and estimate the global CO2 emission from volcanic lakes, an extensive research on CO2 emission of volcanic lakes from Phillipines, Nicaragua, Guatemala, Mexico, Indonesia, Germany, France, Cameroon, Costa Rica, El Salvador and Ecuador had been recently carried out. In-situ measurements of CO2 efflux from the surface environment of volcanic lakes were performed by means of a modified floating device of the accumulation chamber method. To quantify the total CO2 emission from each volcanic lake, CO2 efflux maps were constructed using sequential Gaussian simulations (sGs). CO2 emission rates were normalized by the lake area (km2), and volcanic lakes were grouped following classification in acid, alkaline and neutral lakes. The observed average normalized CO2 emission rate values increase from alkaline (5.5 t km-2 d-1), neutral (210.0 t km-2 d-1), to acid (676.8 t km-2 d-1) volcanic lakes. Taking into account (i) these normalized CO2 emission rates from 31 volcanic lakes, (ii) the number of volcanic lakes in the world (~ 1100), (iii) the fraction of the investigated alkaline (45%), neutral (39%), and acid (16%) volcanic lakes, and (iv) the average areas of the investigated alkaline (36,8 km2), neutral (3,7 km2), and acid (0,5 km2) volcanic lakes; the global CO2 emission from volcanic lakes is about ~ 182 Mt year-1. This estimated value is about ~ 50% of the actual estimated global CO2

  6. 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

  7. Stability of CO2 Atmospheres on Desiccated M Dwarf Exoplanets

    NASA Astrophysics Data System (ADS)

    Gao, Peter; Hu, Renyu; Robinson, Tyler D.; Li, Cheng; Yung, Yuk L.

    2015-06-01

    We investigate the chemical stability of CO2-dominated atmospheres of desiccated M dwarf terrestrial exoplanets using a one-dimensional photochemical model. Around Sun-like stars, CO2 photolysis by Far-UV (FUV) radiation is balanced by recombination reactions that depend on water abundance. Planets orbiting M dwarf stars experience more FUV radiation, and could be depleted in water due to M dwarfs’ prolonged, high-luminosity pre-main sequences. We show that, for water-depleted M dwarf terrestrial planets, a catalytic cycle relying on H2O2 photolysis can maintain a CO2 atmosphere. However, this cycle breaks down for atmospheric hydrogen mixing ratios <1 ppm, resulting in ∼40% of the atmospheric CO2 being converted to CO and O2 on a timescale of 1 Myr. The increased O2 abundance leads to high O3 concentrations, the photolysis of which forms another CO2-regenerating catalytic cycle. For atmospheres with <0.1 ppm hydrogen, CO2 is produced directly from the recombination of CO and O. These catalytic cycles place an upper limit of ∼50% on the amount of CO2 that can be destroyed via photolysis, which is enough to generate Earth-like abundances of (abiotic) O2 and O3. The conditions that lead to such high oxygen levels could be widespread on planets in the habitable zones of M dwarfs. Discrimination between biological and abiotic O2 and O3 in this case can perhaps be accomplished by noting the lack of water features in the reflectance and emission spectra of these planets, which necessitates observations at wavelengths longer than 0.95 μm.

  8. A review of mineral carbonation technologies to sequester CO2.

    PubMed

    Sanna, A; Uibu, M; Caramanna, G; Kuusik, R; Maroto-Valer, M M

    2014-12-01

    Carbon dioxide (CO2) capture and sequestration includes a portfolio of technologies that can potentially sequester billions of tonnes of CO2 per year. Mineral carbonation (MC) is emerging as a potential CCS technology solution to sequester CO2 from smaller/medium emitters, where geological sequestration is not a viable option. In MC processes, CO2 is chemically reacted with calcium- and/or magnesium-containing materials to form stable carbonates. This work investigates the current advancement in the proposed MC technologies and the role they can play in decreasing the overall cost of this CO2 sequestration route. In situ mineral carbonation is a very promising option in terms of resources available and enhanced security, but the technology is still in its infancy and transport and storage costs are still higher than geological storage in sedimentary basins ($17 instead of $8 per tCO2). Ex situ mineral carbonation has been demonstrated on pilot and demonstration scales. However, its application is currently limited by its high costs, which range from $50 to $300 per tCO2 sequestered. Energy use, the reaction rate and material handling are the key factors hindering the success of this technology. The value of the products seems central to render MC economically viable in the same way as conventional CCS seems profitable only when combined with EOR. Large scale projects such as the Skyonic process can help in reducing the knowledge gaps on MC fundamentals and provide accurate costing and data on processes integration and comparison. The literature to date indicates that in the coming decades MC can play an important role in decarbonising the power and industrial sector. PMID:24983767

  9. Optical Properties of Co2+ Doped ZnS Nanocrystals

    NASA Astrophysics Data System (ADS)

    Sarkar, R.; Kumbhakar, P.; Mitra, A. K.

    2010-10-01

    ZnS nanocrystals with Co2+ doping have been prepared through a soft chemical route. The undoped ZnS and Co2+ doped ZnS:Co nanocrystals have been analyzed using X-ray diffraction (XRD), high resolution transmission electron microscope (HRTEM), and ultraviolet-visible (UV-VIS) spectrophotometer. Undoped sample exhibits room-temperature photoluminescence (PL) emission in the blue region with a broad spectral band peaked at ˜397 nm under UV excitation. But from the 1.5% Co2+ doped samples, a strong blue emission peaked at ˜470 nm is observed and further increase in doping leads to considerable blue shift and enhancement in intensity of the PL spectrum.

  10. Production of solar fuels by CO2 plasmolysis

    NASA Astrophysics Data System (ADS)

    Goede, Adelbert P. H.; Bongers, Waldo A.; Graswinckel, Martijn F.; M. C. M van de Sanden, Richard; Leins, Martina; Kopecki, Jochen; Schulz, Andreas; Walker, Mathias

    2014-12-01

    A storage scheme for Renewable Energy (RE) based on the plasmolysis of CO2into CO and O2 has been experimentally investigated, demonstrating high energy efficiency (>50%) combined with high energy density, rapid start-stop and no use of scarce materials. The key parameter controlling energy efficiency has been identified as the reduced electric field. Basic plasma parameters including density and temperature are derived from a simple particle and energy balance model, allowing parameter specification of an upscale 100 kW reactor. With RE powered plasmolysis as the critical element, a CO2 neutral energy system becomes feasible when complemented by effective capture of CO2 at the input and separation of CO from the output gas stream followed by downstream chemical processing into hydrocarbon fuels.