Declining Atmospheric pCO2 During the Late Miocene and Early Pliocene: New Insights from Paired Alkenone and Coccolith Stable Isotope Barometry

Science.gov (United States)

Phelps, S. R.; Polissar, P. J.; deMenocal, P. B.; Swann, J. P.; Guo, M. Y.; Stoll, H. M.

2015-12-01

The relationship between atmospheric CO2 concentrations and climate is broadly understood for the Cenozoic era: warmer periods are associated with higher atmospheric carbon dioxide. This understanding is supported by atmospheric samples of the past 800,000 years from ice cores, which suggest CO2 levels play a key role in regulating global climate on glacial interglacial timescales as well. In this context, the late Miocene poses a challenge: sea-surface temperatures indicate substantial global warmth, though existing data suggest atmospheric CO2 concentrations were lower than pre-industrial values. Recent work using the stable carbon and oxygen isotopic composition of coccolith calcite has demonstrated these organisms began actively diverting inorganic carbon away from calcification and to the site of photosynthesis during the late Miocene. This process occurs in culture experiments in response to low aqueous CO2 concentrations, and suggests decreasing atmospheric pCO2 values during the late Miocene. Here we present new data from ODP Site 806 in the western equatorial Pacific Ocean that supports declining atmospheric CO2 across the late Miocene. Carbon isotope values of coccolith calcite from Site 806 demonstrate carbon limitation and re-allocation of inorganic carbon to photosynthesis starting between ~8 and 6 Ma. The timing of this limitation at Site 806 precedes shifts at other ODP sites, reflecting the higher mixed layer temperature and resultant lower CO2 solubility at Site 806. New measurements of carbon isotope values from alkenones at Site 806 show an increase in photosynthetic carbon fractionation (ɛp) accompanied the carbon limitation evident from coccolith calcite stable isotope data. While higher ɛp is typically interpreted as higher CO2 concentrations, at Site 806, our data suggest it reflects enhancement of chloroplast CO2 from active carbon transport by the coccolithophore algae in response to lower CO2 concentrations. Our new data from ODP Site

Groundwater data improve modelling of headwater stream CO2 outgassing with a stable DIC isotope approach

Science.gov (United States)

Marx, Anne; Conrad, Marcus; Aizinger, Vadym; Prechtel, Alexander; van Geldern, Robert; Barth, Johannes A. C.

2018-05-01

A large portion of terrestrially derived carbon outgasses as carbon dioxide (CO2) from streams and rivers to the atmosphere. Particularly, the amount of CO2 outgassing from small headwater streams is highly uncertain. Conservative estimates suggest that they contribute 36 % (i.e. 0.93 petagrams (Pg) C yr-1) of total CO2 outgassing from all fluvial ecosystems on the globe. In this study, stream pCO2, dissolved inorganic carbon (DIC), and δ13CDIC data were used to determine CO2 outgassing from an acidic headwater stream in the Uhlířská catchment (Czech Republic). This stream drains a catchment with silicate bedrock. The applied stable isotope model is based on the principle that the 13C / 12C ratio of its sources and the intensity of CO2 outgassing control the isotope ratio of DIC in stream water. It avoids the use of the gas transfer velocity parameter (k), which is highly variable and mostly difficult to constrain. Model results indicate that CO2 outgassing contributed more than 80 % to the annual stream inorganic carbon loss in the Uhlířská catchment. This translated to a CO2 outgassing rate from the stream of 34.9 kg C m-2 yr-1 when normalised to the stream surface area. Large temporal variations with maximum values shortly before spring snowmelt and in summer emphasise the need for investigations at higher temporal resolution. We improved the model uncertainty by incorporating groundwater data to better constrain the isotope compositions of initial DIC. Due to the large global abundance of acidic, humic-rich headwaters, we underline the importance of this integral approach for global applications.

Eddy Covariance measurements of stable CO2 and H2O isotopologues

Science.gov (United States)

Braden-Behrens, Jelka; Knohl, Alexander

2015-04-01

The analysis of the stable isotope composition of CO2 and H2O fluxes (such as 13C, 18O and 2H in H2O and CO2) has provided valuable insights into ecosystem gas exchange. The approach builds on differences in the isotope signature of different ecosystem components that are primarily caused by the preference for or the discrimination against respective isotope species by important processes within the ecosystem (e.g. photosynthesis or leaf water diffusion). With the ongoing development of laser spectrometric methods, fast and precise measurements of isotopologue mixing ratios became possible, hence also enabling Eddy Covariance (EC) based approaches to directly measure the isotopic composition of CO2 and H2Ov net fluxes on ecosystem scale. During an eight month long measurement campaign in 2015, we plan to simultaneously measure CO2 and H2Ov isotopologue fluxes using an EC approach in a managed beech forest in Thuringia, Germany. For this purpose, we will use two different laser spectrometers for high frequency measurements of isotopic compositions: For H2Ov measurements, we will use an off axis cavity output water vapour isotope analyser (WVIA, Los Gatos Research Inc.) with 5 Hz response; and for CO2 measurements, we will use a quantum cascade laser-based system (QCLAS, Aerodyne Research Inc.) with thermoelectrically cooled detectors and up to 10 Hz measurement capability. The resulting continuous isotopologue flux measurements will be accompanied by intensive sampling campaigns on the leaf scale: Water from leaf, twig, soil and precipitation samples will be analysed in the lab using isotope ratio mass spectrometry. During data analysis we will put a focus on (i) the influence of carbon and oxygen discrimination on the isotopic signature of respective net ecosystem exchange, (ii) on the relationship between evapotranspiration and leaf water enrichment, and (iii) on the 18O exchange between carbon dioxide and water. At present, we already carried out extensive

PtRu nanoparticles embedded in nitrogen doped carbon with highly stable CO tolerance and durability

Science.gov (United States)

Ling, Ying; Yang, Zehui; Yang, Jun; Zhang, Yunfeng; Zhang, Quan; Yu, Xinxin; Cai, Weiwei

2018-02-01

As is well known, the lower durability and sluggish methanol oxidation reaction (MOR) of PtRu alloy electrocatalyst blocks the commercialization of direct methanol fuel cells (DMFCs). Here, we design a new PtRu electrocatalyst, with highly stable CO tolerance and durability, in which the PtRu nanoparticles are embedded in nitrogen doped carbon layers derived from carbonization of poly(vinyl pyrrolidone). The newly fabricated electrocatalyst exhibits no loss in electrochemical surface area (ECSA) and MOR activity after potential cycling from 0.6-1.0 V versus reversible hydrogen electrode, while commercial CB/PtRu retains only 50% of its initial ECSA. Meanwhile, due to the same protective layers, the Ru dissolution is decelerated, resulting in stable CO tolerance. Methanol oxidation reaction (MOR) testing indicates that the activity of newly fabricated electrocatalyst is two times higher than that of commercial CB/PtRu, and the fuel cell performance of the embedded PtRu electrocatalyst was comparable to that of commercial CB/PtRu. The embedded PtRu electrocatalyst is applicable in real DMFC operation. This study offers important and useful information for the design and fabrication of durable and CO tolerant electrocatalysts.

Evaluation of southern Quebec asbestos residues for CO{sub 2} sequestration by mineral carbonation : preliminary result

Energy Technology Data Exchange (ETDEWEB)

Huot, F. [Geo-conseils, Cap-Rouge, PQ (Canada); Beaudoin, G.; Hebert, R.; Constantin, M. [Laval Univ., Dept. of Geology and Geological Engineering, Quebec City, PQ (Canada); Bonin, G. [LAB Chrysotile Inc., Black Lake, PQ (Canada); Dipple, G.M. [British Columbia Univ., Vancouver, BC (Canada). Dept. of Earth and Ocean Sciences

2003-07-01

Carbon dioxide (CO{sub 2}) sequestration is one approach that can help reduce CO{sub 2} levels in the atmosphere. This paper discusses CO{sub 2} sequestration by mineral carbonation using ultramafic rock-hosted magnesian silicates (serpentine, olivine, talc). The carbonation process produces magnesite, which is a geologically stable and an environmentally safe magnesium carbonate. There are 3 potential CO{sub 2} sinks in southern Quebec that use such silicates. They are: (1) asbestos mill residues, (2) associated mine waste, and (3) ultramafic bedrock. Asbestos is extracted from serpentinized harzburgite located in the Thetford Mines and Asbestos ophiolitic massifs and also from the highly sheared Pennington Sheet. The physical and chemical properties of magnesium silicate deposits greatly determine their carbonation potential. A wide range of properties was observed in samples obtained from almost all asbestos mill residues and waste. The reaction which takes place depends on the mineral content. The kinetics of the reactions are influenced by humidity and grain size.

Continuing Studies on Direct Aqueous Mineral Carbonation of CO{sub 2} Sequestration

Energy Technology Data Exchange (ETDEWEB)

O' Connor, W.K.; Dahlin, D.C.; Nilsen, D.N.; Gerdemann, S.J.; Rush, G.E.; Penner, L.R.; Walters, R.P.; Turner, P.C.

2002-03-04

Direct aqueous mineral carbonation has been investigated as a process to convert gaseous CO{sub 2} into a geologically stable, solid final form. The process utilizes a solution of sodium bicarbonate (NaHCO{sub 3}), sodium chloride (NaCl), and water, mixed with a mineral reactant, such as olivine (Mg{sub 2}SiO{sub 4}) or serpentine [Mg{sub 3}Si{sub 2}O{sub 5}(OH){sub 4}]. Carbon dioxide is dissolved into this slurry, by diffusion through the surface and gas dispersion within the aqueous phase. The process includes dissolution of the mineral and precipitation of the magnesium carbonate mineral magnesite (MgCO{sub 3}) in a single unit operation. Activation of the silicate minerals has been achieved by thermal and mechanical means, resulting in up to 80% stoichiometric conversion of the silicate to the carbonate within 30 minutes. Heat treatment of the serpentine, or attrition grinding of the olivine and/or serpentine, appear to activate the minerals by the generation of a non-crystalline phase. Successful conversion to the carbonate has been demonstrated at ambient temperature and relatively low (10 atm) partial pressure of CO{sub 2} (P{sub CO2}). However, optimum results have been achieved using the bicarbonate-bearing solution, and high P{sub CO2}. Specific conditions include: 185 C; P{sub CO2}=150 atm; 30% solids. Studies suggest that the mineral dissolution rate is not solely surface controlled, while the carbonate precipitation rate is primarily dependent on the bicarbonate concentration of the slurry. Current and future activities include further examination of the reaction pathways and pretreatment options, the development of a continuous flow reactor, and an evaluation of the economic feasibility of the process.

Using a laser-based CO2 carbon isotope analyser to investigate gas transfer in geological media

International Nuclear Information System (INIS)

Guillon, S.; Pili, E.; Agrinier, P.

2012-01-01

CO 2 stable carbon isotopes are very attractive in environmental research to investigate both natural and anthropogenic carbon sources. Laser-based CO 2 carbon isotope analysis provides continuous measurement at high temporal resolution and is a promising alternative to isotope ratio mass spectrometry (IRMS). We performed a thorough assessment of a commercially available CO 2 Carbon Isotope Analyser (CCIA DLT-100, Los Gatos Research) that allows in situ measurement of C-13 in CO 2 . Using a set of reference gases of known CO 2 concentration and carbon isotopic composition, we evaluated the precision, long-term stability, temperature sensitivity and concentration dependence of the analyser. Despite good precision calculated from Allan variance (5.0 ppm for CO 2 concentration, and 0.05 per thousand for δC-13 at 60 s averaging), real performances are altered by two main sources of error: temperature sensitivity and dependence of C-13 on CO 2 concentration. Data processing is required to correct for these errors. Following application of these corrections, we achieve an accuracy of 8.7 ppm for CO 2 concentration and 1.3 per thousand for δC-13, which is worse compared to mass spectrometry performance, but still allowing field applications. With this portable analyser we measured CO 2 flux degassed from rock in an underground tunnel. The obtained carbon isotopic composition agrees with IRMS measurement, and can be used to identify the carbon source. (authors)

Groundwater data improve modelling of headwater stream CO2 outgassing with a stable DIC isotope approach

Directory of Open Access Journals (Sweden)

A. Marx

2018-05-01

Full Text Available A large portion of terrestrially derived carbon outgasses as carbon dioxide (CO2 from streams and rivers to the atmosphere. Particularly, the amount of CO2 outgassing from small headwater streams is highly uncertain. Conservative estimates suggest that they contribute 36 % (i.e. 0.93 petagrams (Pg C yr−1 of total CO2 outgassing from all fluvial ecosystems on the globe. In this study, stream pCO2, dissolved inorganic carbon (DIC, and δ13CDIC data were used to determine CO2 outgassing from an acidic headwater stream in the Uhlířská catchment (Czech Republic. This stream drains a catchment with silicate bedrock. The applied stable isotope model is based on the principle that the 13C ∕ 12C ratio of its sources and the intensity of CO2 outgassing control the isotope ratio of DIC in stream water. It avoids the use of the gas transfer velocity parameter (k, which is highly variable and mostly difficult to constrain. Model results indicate that CO2 outgassing contributed more than 80 % to the annual stream inorganic carbon loss in the Uhlířská catchment. This translated to a CO2 outgassing rate from the stream of 34.9 kg C m−2 yr−1 when normalised to the stream surface area. Large temporal variations with maximum values shortly before spring snowmelt and in summer emphasise the need for investigations at higher temporal resolution. We improved the model uncertainty by incorporating groundwater data to better constrain the isotope compositions of initial DIC. Due to the large global abundance of acidic, humic-rich headwaters, we underline the importance of this integral approach for global applications.

Mineral Carbonation Potential of CO2 from Natural and Industrial-based Alkalinity Sources

Science.gov (United States)

Wilcox, J.; Kirchofer, A.

2014-12-01

Mineral carbonation is a Carbon Capture and Storage (CSS) technology where gaseous CO2 is reacted with alkaline materials (such as silicate minerals and alkaline industrial wastes) and converted into stable and environmentally benign carbonate minerals (Metz et al., 2005). Here, we present a holistic, transparent life cycle assessment model of aqueous mineral carbonation built using a hybrid process model and economic input-output life cycle assessment approach. We compared the energy efficiency and the net CO2 storage potential of various mineral carbonation processes based on different feedstock material and process schemes on a consistent basis by determining the energy and material balance of each implementation (Kirchofer et al., 2011). In particular, we evaluated the net CO2 storage potential of aqueous mineral carbonation for serpentine, olivine, cement kiln dust, fly ash, and steel slag across a range of reaction conditions and process parameters. A preliminary systematic investigation of the tradeoffs inherent in mineral carbonation processes was conducted and guidelines for the optimization of the life-cycle energy efficiency are provided. The life-cycle assessment of aqueous mineral carbonation suggests that a variety of alkalinity sources and process configurations are capable of net CO2 reductions. The maximum carbonation efficiency, defined as mass percent of CO2 mitigated per CO2 input, was 83% for CKD at ambient temperature and pressure conditions. In order of decreasing efficiency, the maximum carbonation efficiencies for the other alkalinity sources investigated were: olivine, 66%; SS, 64%; FA, 36%; and serpentine, 13%. For natural alkalinity sources, availability is estimated based on U.S. production rates of a) lime (18 Mt/yr) or b) sand and gravel (760 Mt/yr) (USGS, 2011). The low estimate assumes the maximum sequestration efficiency of the alkalinity source obtained in the current work and the high estimate assumes a sequestration efficiency

CO2 Capture by Carbon Aerogel–Potassium Carbonate Nanocomposites

Directory of Open Access Journals (Sweden)

Guang Yang

2016-01-01

Full Text Available Recently, various composites for reducing CO2 emissions have been extensively studied. Because of their high sorption capacity and low cost, alkali metal carbonates are recognized as a potential candidate to capture CO2 from flue gas under moist conditions. However, undesirable effects and characteristics such as high regeneration temperatures or the formation of byproducts lead to high energy costs associated with the desorption process and impede the application of these materials. In this study, we focused on the regeneration temperature of carbon aerogel–potassium carbonate (CA–KC nanocomposites, where KC nanocrystals were formed in the mesopores of the CAs. We observed that the nanopore size of the original CA plays an important role in decreasing the regeneration temperature and in enhancing the CO2 capture capacity. In particular, 7CA–KC, which was prepared from a CA with 7 nm pores, exhibited excellent performance, reducing the desorption temperature to 380 K and exhibiting a high CO2 capture capacity of 13.0 mmol/g-K2CO3, which is higher than the theoretical value for K2CO3 under moist conditions.

Experimental evidence for carbonate precipitation and CO 2 degassing during sea ice formation

Science.gov (United States)

Papadimitriou, S.; Kennedy, H.; Kattner, G.; Dieckmann, G. S.; Thomas, D. N.

2004-04-01

Chemical and stable carbon isotopic modifications during the freezing of artificial seawater were measured in four 4 m 3 tank incubations. Three of the four incubations were inoculated with a nonaxenic Antarctic diatom culture. The 18 days of freezing resulted in 25 to 27 cm thick ice sheets overlying the residual seawater. The ice phase was characterized by a decrease in temperature from -1.9 to -2.2°C in the under-ice seawater down to -6.7°C in the upper 4 cm of the ice sheet, with a concurrent increase in the salinity of the under-ice seawater and brine inclusions of the ice sheet as a result of physical concentration of major dissolved salts by expulsion from the solid ice matrix. Measurements of pH, total dissolved inorganic carbon (C T) and its stable isotopic composition (δ 13C T) all exhibited changes, which suggest minimal effect by biological activity during the experiment. A systematic drop in pH and salinity-normalized C T by up to 0.37 pH SWS units and 376 μmol C kg -1 respectively at the lowest temperature and highest salinity part of the ice sheet were coupled with an equally systematic 13C enrichment of the C T. Calculations based on the direct pH and C T measurements indicated a steady increase in the in situ concentration of dissolved carbon dioxide (CO 2(aq)) with time and increasing salinity within the ice sheet, partly due to changes in the dissociation constants of carbonic acid in the low temperature-high salinity range within sea ice. The combined effects of temperature and salinity on the solubility of CO 2 over the range of conditions encountered during this study was a slight net decrease in the equilibrium CO 2(aq) concentration as a result of the salting-out overriding the increase in solubility with decreasing temperature. Hence, the increase in the in situ CO 2(aq) concentration lead to saturation or supersaturation of the brine inclusions in the ice sheet with respect to atmospheric pCO 2 (≈3.5 × 10 -4 atm). When all physico

Carbon sequestration in soybean crop soils: the role of hydrogen-coupled CO2 fixation

Science.gov (United States)

Graham, A.; Layzell, D. B.; Scott, N. A.; Cen, Y.; Kyser, T. K.

2011-12-01

Conversion of native vegetation to agricultural land in order to support the world's growing population is a key factor contributing to global climate change. However, the extent to which agricultural activities contribute to greenhouse gas emissions compared to carbon storage is difficult to ascertain, especially for legume crops, such as soybeans. Soybean establishment often leads to an increase in N2O emissions because N-fixation leads to increased soil available N during decomposition of the low C:N legume biomass. However, soybean establishment may also reduce net greenhouse gas emissions by increasing soil fertility, plant growth, and soil carbon storage. The mechanism behind increased carbon storage, however, remains unclear. One explanation points to hydrogen coupled CO2 fixation; the process by which nitrogen fixation releases H2 into the soil system, thereby promoting chemoautotrophic carbon fixation by soil microbes. We used 13CO2 as a tracer to track the amount and fate of carbon fixed by hydrogen coupled CO2 fixation during one-year field and laboratory incubations. The objectives of the research are to 1) quantify rates of 13CO2 fixation in soil collected from a field used for long-term soybean production 2) examine the impact of H2 gas concentration on rates of 13CO2 fixation, and 3) measure changes in δ13C signature over time in 3 soil fractions: microbial biomass, light fraction, and acid stable fraction. If this newly-fixed carbon is incorporated into the acid-stable soil C fraction, it has a good chance of contributing to long-term soil C sequestration under soybean production. Soil was collected in the field both adjacent to root nodules (nodule soil) and >3cm away (root soil) and labelled with 13CO2 (1% v/v) in the presence and absence of H2 gas. After a two week labelling period, δ13C signatures already revealed differences in the four treatments of bulk soil: -17.1 for root, -17.6 for nodule, -14.2 for root + H2, and -6.1 for nodule + H2

Vehicle emissions of greenhouse gases and related tracers from a tunnel study: : CO: CO2, N2O: CO2, CH4: CO2, O2: CO2 ratios, and the stable isotopes 13C and 18O in CO2 and CO

NARCIS (Netherlands)

Popa, Maria Elena; Vollmer, M. K.; Jordan, A.; Brand, W. A.; Pathirana, S. L.; Rothe, M.; Röckmann, T.

2014-01-01

Measurements of CO2, CO, N2O and CH4 mole fractions, O2/N2 ratios and the stable isotopes 13C and 18O in CO2 and CO have been performed in air samples from the Islisberg highway tunnel (Switzerland). The molar CO : CO2 ratios, with an average of (4.15 ± 0.34) ppb:ppm, are lower than reported in

Metabolic effects of Carbon Dioxide (CO 2 ) insufflation during ...

African Journals Online (AJOL)

Metabolic effects of Carbon Dioxide (CO 2 ) insufflation during laparoscopic surgery: changes in pH, arterial partial Pressure of Carbon Dioxide (PaCo 2 ) and End Tidal Carbon Dioxide (EtCO 2 ) ... Respiratory adjustments were done for EtCO2 levels above 60mmHg or SPO2 below 92% or adverse haemodynamic changes.

Characteristics and carbon stable isotopes of fluids in the Southern Kerala granulites and their bearing on the source of CO2

Science.gov (United States)

Santosh, M.; Jackson, D. H.; Mattey, D. P.; Harris, N. B. W.

1988-01-01

Carbon dioxide-rich inclusions commonly occur in the banded charnockites and khondalites of southern Kerala as well as in the incipient charnockites formed by desiccation of gneisses along oriented zones. The combined high density fluid inclusion isochores and the range of thermometric estimates from mineral assemblages indicate entrapment pressures in the range of 5.4 to 6.1 Kbar. The CO2 equation of state barometry closely compares with the 5 plus or minus 1 Kbar estimate from mineral phases for the region. The isochores for the high density fluid inclusions in all the three rock types pass through the P-T domain recorded by phase equilibria, implying that carbon dioxide was the dominating ambient fluid species during peak metamorphic conditions. In order to constrain the source of fluids and to evaluate the mechanism of desiccation, researchers undertook detailed investigations of the carbon stable isotope composition of entrapped fluids. Researchers report here the results of preliminary studies in some of the classic localities in southern Kerala namely, Ponmudi, Kottavattom, Manali and Kadakamon.

Determining CO2 storage potential during miscible CO2 enhanced oil recovery: Noble gas and stable isotope tracers

Science.gov (United States)

Shelton, Jenna L.; McIntosh, Jennifer C.; Hunt, Andrew; Beebe, Thomas L; Parker, Andrew D; Warwick, Peter D.; Drake, Ronald; McCray, John E.

2016-01-01

Rising atmospheric carbon dioxide (CO2) concentrations are fueling anthropogenic climate change. Geologic sequestration of anthropogenic CO2 in depleted oil reservoirs is one option for reducing CO2 emissions to the atmosphere while enhancing oil recovery. In order to evaluate the feasibility of using enhanced oil recovery (EOR) sites in the United States for permanent CO2 storage, an active multi-stage miscible CO2flooding project in the Permian Basin (North Ward Estes Field, near Wickett, Texas) was investigated. In addition, two major natural CO2 reservoirs in the southeastern Paradox Basin (McElmo Dome and Doe Canyon) were also investigated as they provide CO2 for EOR operations in the Permian Basin. Produced gas and water were collected from three different CO2 flooding phases (with different start dates) within the North Ward Estes Field to evaluate possible CO2 storage mechanisms and amounts of total CO2retention. McElmo Dome and Doe Canyon were sampled for produced gas to determine the noble gas and stable isotope signature of the original injected EOR gas and to confirm the source of this naturally-occurring CO2. As expected, the natural CO2produced from McElmo Dome and Doe Canyon is a mix of mantle and crustal sources. When comparing CO2 injection and production rates for the CO2 floods in the North Ward Estes Field, it appears that CO2 retention in the reservoir decreased over the course of the three injections, retaining 39%, 49% and 61% of the injected CO2 for the 2008, 2010, and 2013 projects, respectively, characteristic of maturing CO2 miscible flood projects. Noble gas isotopic composition of the injected and produced gas for the flood projects suggest no active fractionation, while δ13CCO2 values suggest no active CO2dissolution into formation water, or mineralization. CO2 volumes capable of dissolving in residual formation fluids were also estimated along with the potential to store pure-phase supercritical CO2. Using a combination

Hydrochemical variations in selected geothermal groundwater and carbonated springs in Korea: a baseline study for early detection of CO2 leakage.

Science.gov (United States)

Choi, Hanna; Piao, Jize; Woo, Nam C; Cho, Heuynam

2017-02-01

A baseline hydrochemistry of the above zone aquifer was examined for the potential of CO 2 early detection monitoring. Among the major ionic components and stable isotope ratios of oxygen, hydrogen, and carbon, components with a relative standard deviation (RSD) of leakage into the above zone. As an analog to the zone above CO 2 storage formation, we sampled deep groundwater, including geothermal groundwater from well depths of 400-700 m below the ground surface (bgs) and carbonated springs with a high CO 2 content in Korea. Under the natural conditions of inland geothermal groundwater, pH, electrical conductivity (EC), bicarbonate (HCO 3 ), δ 18 O, δ 2 H, and δ 13 C were relatively stable as well as sensitive to the introduction of CO 2 (g), thus showing good potential as monitoring parameters for early detection of CO 2 leakage. In carbonated springs, the parameters identified were pH, δ 18 O, and δ 2 H. Baseline hydrochemistry monitoring could provide information on parameters useful for detecting anomalies caused by CO 2 leakage as measures for early warning.

Indoor and outdoor urban atmospheric CO2: Stable carbon isotope constraints on mixing and mass balance

International Nuclear Information System (INIS)

Yanes, Yurena; Yapp, Crayton J.

2010-01-01

Research highlights: → 13 C of indoor CO 2 indicates proportion of C 4 -derived carbon in occupants' diet. → Flux balance model for ventilated rooms shows rapid approach to CO 2 steady-state. → From extant indoor CO 2 data more dietary C 4 carbon in American than European diets. → Local outdoor urban CO 2 increase of 17 ppm in ten years, no change in average 13 C. - Abstract: From July to November 2009, concentrations of CO 2 in 78 samples of ambient air collected in 18 different interior spaces on a university campus in Dallas, Texas (USA) ranged from 386 to 1980 ppm. Corresponding δ 13 C values varied from -8.9 per mille to -19.4 per mille. The CO 2 from 22 samples of outdoor air (also collected on campus) had a more limited range of concentrations from 385 to 447 ppm (avg. = 408 ppm), while δ 13 C values varied from -10.1 per mille to -8.4 per mille (avg.=-9.0 per mille). In contrast to ambient indoor and outdoor air, the concentrations of CO 2 exhaled by 38 different individuals ranged from 38,300 to 76,200 ppm (avg. = 55,100 ppm), while δ 13 C values ranged from -24.8 per mille to -17.7 per mille (avg. = -21.8 per mille). The residence times of the total air in the interior spaces of this study appear to have been on the order of 10 min with relatively rapid approaches (∼30 min) to steady-state concentrations of ambient CO 2 gas. Collectively, the δ 13 C values of the indoor CO 2 samples were linearly correlated with the reciprocal of CO 2 concentration, exhibiting an intercept of -21.8 per mille, with r 2 = 0.99 and p 2 data representing 18 interior spaces (with varying numbers of occupants), and the coincidence of the intercept (-21.8 per mille) with the average δ 13 C value for human-exhaled CO 2 demonstrates simple mixing between two inputs: (1) outdoor CO 2 introduced to the interior spaces by ventilation systems, and (2) CO 2 exhaled by human occupants of those spaces. If such simple binary mixing is a common feature of interior spaces, it

Carbon flow from volcanic CO2 into soil microbial communities of a wetland mofette.

Science.gov (United States)

Beulig, Felix; Heuer, Verena B; Akob, Denise M; Viehweger, Bernhard; Elvert, Marcus; Herrmann, Martina; Hinrichs, Kai-Uwe; Küsel, Kirsten

2015-03-01

Effects of extremely high carbon dioxide (CO2) concentrations on soil microbial communities and associated processes are largely unknown. We studied a wetland area affected by spots of subcrustal CO2 degassing (mofettes) with focus on anaerobic autotrophic methanogenesis and acetogenesis because the pore gas phase was largely hypoxic. Compared with a reference soil, the mofette was more acidic (ΔpH ∼0.8), strongly enriched in organic carbon (up to 10 times), and exhibited lower prokaryotic diversity. It was dominated by methanogens and subdivision 1 Acidobacteria, which likely thrived under stable hypoxia and acidic pH. Anoxic incubations revealed enhanced formation of acetate and methane (CH4) from hydrogen (H2) and CO2 consistent with elevated CH4 and acetate levels in the mofette soil. (13)CO2 mofette soil incubations showed high label incorporations with ∼512 ng (13)C g (dry weight (dw)) soil(-1) d(-1) into the bulk soil and up to 10.7 ng (13)C g (dw) soil(-1) d(-1) into almost all analyzed bacterial lipids. Incorporation of CO2-derived carbon into archaeal lipids was much lower and restricted to the first 10 cm of the soil. DNA-SIP analysis revealed that acidophilic methanogens affiliated with Methanoregulaceae and hitherto unknown acetogens appeared to be involved in the chemolithoautotrophic utilization of (13)CO2. Subdivision 1 Acidobacteriaceae assimilated (13)CO2 likely via anaplerotic reactions because Acidobacteriaceae are not known to harbor enzymatic pathways for autotrophic CO2 assimilation. We conclude that CO2-induced geochemical changes promoted anaerobic and acidophilic organisms and altered carbon turnover in affected soils.

A Practical Cryogen-Free CO2 Purification and Freezing Technique for Stable Isotope Analysis.

Science.gov (United States)

Sakai, Saburo; Matsuda, Shinichi

2017-04-18

Since isotopic analysis by mass spectrometry began in the early 1900s, sample gas for light-element isotopic measurements has been purified by the use of cryogens and vacuum-line systems. However, this conventional purification technique can achieve only certain temperatures that depend on the cryogens and can be sustained only as long as there is a continuous cryogen supply. Here, we demonstrate a practical cryogen-free CO 2 purification technique using an electrical operated cryocooler for stable isotope analysis. This approach is based on portable free-piston Stirling cooling technology and controls the temperature to an accuracy of 0.1 °C in a range from room temperature to -196 °C (liquid-nitrogen temperature). The lowest temperature can be achieved in as little as 10 min. We successfully purified CO 2 gas generated by carbonates and phosphoric acid reaction and found its sublimation point to be -155.6 °C at 0.1 Torr in the vacuum line. This means that the temperature required for CO 2 trapping is much higher than the liquid-nitrogen temperature. Our portable cooling system offers the ability to be free from the inconvenience of cryogen use for stable isotope analysis. It also offers a new cooling method applicable to a number of fields that use gas measurements.

Assessment of CO2 discharge in a spring using time-variant stable carbon isotope data as a natural analogue study of CO2 leakage

Science.gov (United States)

Yu, Soonyoung; Chae, Gitak; Jo, Minki; Kim, Jeong-Chan; Yun, Seong-Taek

2015-04-01

CO2-rich springs have been studied as a natural analogue of CO2 leakage through shallow subsurface environment, as they provide information on the behaviors of CO2 during the leakage from geologic CO2 storage sites. For this study, we monitored the δ13C values as well as temperature, pH, EC, DO, and alkalinity for a CO2-rich spring for 48 hours. The water samples (N=47) were collected every hour in stopper bottles without headspace to avoid the interaction with air and the CO2 degassing. The δ13C values of total dissolved inorganic carbon (TDIC) in the water samples were analyzed using a cavity ring-down spectroscopy (CRDS) system (Picarro). The values of δ13CTDIC, temperature, pH, EC, DO, and alkalinity were in the range of -9.43 ~ -8.91 o 12.3 ~ 13.2oC, 4.86 ~ 5.02, 186 ~ 189 μS/cm, 1.8 ~ 3.4 mg/L, and 0.74 ~ 0.95 meq/L, respectively. The concentrations of TDIC calculated using pH and alkalinity values were between 22.5 and 34.8 mmol/L. The δ13CTDIC data imply that dissolved carbon in the spring was derived from a deep-seated source (i.e., magmatic) that was slightly intermixed with soil CO2. Careful examination of the time-series variation of measured parameters shows the following characteristics: 1) the δ13CTDIC values are negatively correlated with pH (r = -0.59) and positively correlated with TDIC (r = 0.58), and 2) delay times of the change of pH and alkalinity following the change of δ13CTDIC values are 0 and -3 hours, respectively; the pH change occurs simultaneously with the change of δ13CTDIC, while the alkalinity change happens before 3 hours. Our results indicate that the studied CO2-rich spring is influenced by the intermittent supply of deep-seated CO2. [Acknowledgment] This work was financially supported by the fundamental research project of KIGAM and partially by the "Geo-Advanced Innovative Action (GAIA) Project (2014000530003)" from Korea Ministry of Environment (MOE).

Preferential flow pathways revealed by field based stable isotope analysis of CO2 by mid-infrared laser spectroscopy

Science.gov (United States)

van Geldern, Robert; Nowak, Martin; Zimmer, Martin; Szizybalski, Alexandra; Myrttinen, Anssi; Barth, Johannes A. C.; Jost, Hj

2016-04-01

A newly developed and commercially available isotope ratio laser spectrometer for CO2 analyses has been tested during a 10-day field monitoring campaign at the Ketzin pilot site for CO2 storage in northern Germany. The laser instrument is based on tunable laser direct absorption in the mid-infrared. The instrument recorded a continuous 10-day carbon stable isotope data set with 30 minutes resolution directly on-site in a field-based laboratory container during a tracer experiment. To test the instruments performance and accuracy the monitoring campaign was accompanied by daily CO2 sampling for laboratory analyses with isotope ratio mass spectrometry (IRMS). The carbon stable isotope ratios measured by conventional IRMS technique and by the new mid-infrared laser spectrometer agree remarkably well within 2σ analytical precision (<0.3 ‰). This proves the capability of the new mid-infrared direct absorption technique to measure high precision and accurate real-time table isotope data directly in the field. The injected CO2 tracer had a distinct δ13C value that was largely different from the reservoir background value. The laser spectroscopy data revealed a prior to this study unknown, intensive dynamic with fast changing δ13C values. The arrival pattern of the tracer suggest that the observed fluctuations were probably caused by migration along separate and distinct preferential flow paths between injection well and observation well. The new technique might contribute to a better tracing of the migration of the underground CO2 plume and help to ensure the long-term integrity of the reservoir.

Carbon flow from volcanic CO2 into soil microbial communities of a wetland mofette

Science.gov (United States)

Beulig, Felix; Heuer, Verena B.; Akob, Denise M.; Viehweger, Bernhard; Elvert, Marcus; Herrmann, Martina; Hinrichs, Kai-Uwe; Küsel, Kirsten

2015-01-01

Effects of extremely high carbon dioxide (CO2) concentrations on soil microbial communities and associated processes are largely unknown. We studied a wetland area affected by spots of subcrustal CO2 degassing (mofettes) with focus on anaerobic autotrophic methanogenesis and acetogenesis because the pore gas phase was largely hypoxic. Compared with a reference soil, the mofette was more acidic (ΔpH ~0.8), strongly enriched in organic carbon (up to 10 times), and exhibited lower prokaryotic diversity. It was dominated by methanogens and subdivision 1Acidobacteria, which likely thrived under stable hypoxia and acidic pH. Anoxic incubations revealed enhanced formation of acetate and methane (CH4) from hydrogen (H2) and CO2 consistent with elevated CH4 and acetate levels in the mofette soil. 13CO2 mofette soil incubations showed high label incorporations with ~512 ng13C g (dry weight (dw)) soil−1 d−1 into the bulk soil and up to 10.7 ng 13C g (dw) soil−1 d−1 into almost all analyzed bacterial lipids. Incorporation of CO2-derived carbon into archaeal lipids was much lower and restricted to the first 10 cm of the soil. DNA-SIP analysis revealed that acidophilic methanogens affiliated withMethanoregulaceae and hitherto unknown acetogens appeared to be involved in the chemolithoautotrophic utilization of 13CO2. Subdivision 1 Acidobacteriaceae assimilated 13CO2 likely via anaplerotic reactions because Acidobacteriaceae are not known to harbor enzymatic pathways for autotrophic CO2 assimilation. We conclude that CO2-induced geochemical changes promoted anaerobic and acidophilic organisms and altered carbon turnover in affected soils.

Experimental Investigation and Simplistic Geochemical Modeling of CO2 Mineral Carbonation Using the Mount Tawai Peridotite

Directory of Open Access Journals (Sweden)

Omeid Rahmani

2016-03-01

Full Text Available In this work, the potential of CO2 mineral carbonation of brucite (Mg(OH2 derived from the Mount Tawai peridotite (forsterite based (Mg2SiO4 to produce thermodynamically stable magnesium carbonate (MgCO3 was evaluated. The effect of three main factors (reaction temperature, particle size, and water vapor were investigated in a sequence of experiments consisting of aqueous acid leaching, evaporation to dryness of the slurry mass, and then gas-solid carbonation under pressurized CO2. The maximum amount of Mg converted to MgCO3 is ~99%, which occurred at temperatures between 150 and 175 °C. It was also found that the reduction of particle size range from >200 to <75 µm enhanced the leaching rate significantly. In addition, the results showed the essential role of water vapor in promoting effective carbonation. By increasing water vapor concentration from 5 to 10 vol %, the mineral carbonation rate increased by 30%. This work has also numerically modeled the process by which CO2 gas may be sequestered, by reaction with forsterite in the presence of moisture. In both experimental analysis and geochemical modeling, the results showed that the reaction is favored and of high yield; going almost to completion (within about one year with the bulk of the carbon partitioning into magnesite and that very little remains in solution.

Tracing the link between plant volatile organic compound emissions and CO2 fluxes and by stable isotopes

Science.gov (United States)

Werner, Christiane; Wegener, Frederik; Jardine, Kolby

2015-04-01

The vegetation exerts a large influence on the atmosphere through the emission of volatile organic compounds (VOCs) and the emission and uptake of the greenhouse gas CO2. Despite the enormous importance, processes controlling plant carbon allocation into primary and secondary metabolism, such as photosynthetic carbon uptake, respiratory CO2 emission and VOC synthesis, remains unclear. Moreover, vegetation-atmosphere CO2 exchange is associated with a large isotopic imprint due to photosynthetic carbon isotope discrimination and 13C-fractionation during respiratory CO2 release1. The latter has been proposed to be related to carbon partitioning in the metabolic branching points of the respiratory pathways and secondary metabolism, which are linked via a number of interfaces including the central metabolite pyruvate. Notably, it is a known substrate in a large array of secondary pathways leading to the biosynthesis of many volatile organic compounds (VOCs), such as volatile isoprenoids, oxygenated VOCs, aromatics, fatty acid oxidation products, which can be emitted by plants. Here we investigate the linkage between VOC emissions, CO2 fluxes and associated isotope effects based on simultaneous real-time measurements of stable carbon isotope composition of branch respired CO2 (CRDS) and VOC fluxes (PTR-MS). We utilized positionally specific 13C-labeled pyruvate branch feeding experiments in the mediterranean shrub (Halimium halimifolium) to trace the partitioning of C1, C2, and C3 carbon atoms of pyruvate into VOCs versus CO2 emissions in the light and in the dark. In the light, we found high emission rates of a large array of VOC including volatile isoprenoids, oxygenated VOCs, green leaf volatiles, aromatics, sulfides, and nitrogen containing VOCs. These observations suggest that in the light, H. halimifolium dedicates a high carbon flux through secondary biosynthetic pathways including the pyruvate dehydrogenase bypass, mevalonic acid, MEP/DOXP, shikimic acid, and

Mineral CO2 sequestration by steel slag carbonation

International Nuclear Information System (INIS)

Huijgen, W.J.J.; Comans, R.N.J.; Witkamp, G.J.

2005-12-01

Mineral CO2 sequestration, i.e., carbonation of alkaline silicate Ca/Mg minerals, analogous to natural weathering processes, is a possible technology for the reduction of carbon dioxide emissions to the atmosphere. In this paper, alkaline Ca-rich industrial residues are presented as a possible feedstock for mineral CO2 sequestration. These materials are cheap, available near large point sources of CO2, and tend to react relatively rapidly with CO2 due to their chemical instability. Ground steel slag was carbonated in aqueous suspensions to study its reaction mechanisms. Process variables, such as particle size, temperature, carbon dioxide pressure, and reaction time, were systematically varied, and their influence on the carbonation rate was investigated. The maximum carbonation degree reached was 74% of the Ca content in 30 min at 19 bar pressure, 100C, and a particle size of <38 μm. The two must important factors determining the reaction rare are particle size (<2 mm to <38 μm) and reaction temperature (25-225C). The carbonation reaction was found to occur in two steps: (1) leaching of calcium from the steel slag particles into the solution; (2) precipitation of calcite on the surface of these particles. The first step and, more in particular, the diffusion of calcium through the solid matrix toward the surface appeared to be the rate-determining reaction step, The Ca diffusion was found to be hindered by the formation of a CaCO3-coating and a Ca-depleted silicate zona during the carbonation process. Research on further enhancement of the reaction rate, which would contribute to the development of a cost-effective CO2-sequestration process, should focus particularly on this mechanism

Carbon balance of CO2-EOR for NCNO classification

Energy Technology Data Exchange (ETDEWEB)

Nunez-Lopez, Vanessa [The University of Texas at Austin; Gil-Egui, Ramon; Gonzalez-Nicolas, Ana; Hovorka, Susan D

2017-03-18

The question of whether carbon dioxide enhanced oil recovery (CO2-EOR) constitutes a valid alternative for greenhouse gas emission reduction has been frequently asked by the general public and environmental sectors. Through this technology, operational since 1972, oil production is enhanced by injecting CO2 into depleted oil reservoirs in order displace the residual oil toward production wells in a solvent/miscible process. For decades, the CO2 utilized for EOR has been most commonly sourced from natural CO2 accumulations. More recently, a few projects have emerged where anthropogenic CO2 (A-CO2) is captured at an industrial facility, transported to a depleted oil field, and utilized for EOR. If carbon geologic storage is one of the project objectives, all the CO2 injected into the oil field for EOR could technically be stored in the formation. Even though the CO2 is being prevented from entering the atmosphere, and permanently stored away in a secured geologic formation, a question arises as to whether the total CO2 volumes stored in order to produce the incremental oil through EOR are larger than the CO2 emitted throughout the entire CO2-EOR process, including the capture facility, the EOR site, and the refining and burning of the end product. We intend to answer some of these questions through a DOE-NETL funded study titled “Carbon Life Cycle Analysis of CO2-EOR for Net Carbon Negative Oil (NCNO) Classification”. NCNO is defined as oil whose carbon emissions to the atmosphere, when burned or otherwise used, are less than the amount of carbon permanently stored in the reservoir in order to produce the oil. In this paper, we focus on the EOR site in what is referred to as a gate-to-gate system, but are inclusive of the burning of the refined product, as this end member is explicitly stated in the definition of NCNO. Finally, we use Cranfield, Mississippi, as a case study and come to the conclusion that the incremental oil produced is net carbon negative.

CO/sub 2/ carbon cycle and climate interactions

Energy Technology Data Exchange (ETDEWEB)

Grassl, H; Maier-Reimer, E; Degens, E T; Kempe, S; Spitzy, A

1984-03-01

Past and expected emissions of anthropogenic CO/sub 2/ stimulate carbon cycle and climate research. Prognoses of future CO/sub 2/ levels depend on energy scenarios and on the reaction of the biosphere and hydrosphere to elevated atmospheric CO/sub 2/ concentrations. The reaction of the reservoirs vegetation, freshwater and oceans to disturbances of the carbon cycle is reviewed. For the oceans first results of a simple carbon cycle model implanted in a three-dimensional general circulation model are presented. This model allows experiments not possible with previous box models.

Closed-Cycle, Frequency-Stable CO2 Laser Technology

Science.gov (United States)

Batten, Carmen E. (Editor); Miller, Irvin M. (Editor); Wood, George M., Jr. (Editor); Willetts, David V. (Editor)

1987-01-01

These proceedings contain a collection of papers and comments presented at a workshop on technology associated with long-duration closed-cycle operation of frequency-stable, pulsed carbon dioxide lasers. This workshop was held at the NASA Langley Research Center June 10 to 12, 1986. The workshop, jointly sponsored by the National Aeronautics and Space Administration (NASA) and the Royal Signals and Radar Establishment (RSRE), was attended by 63 engineers and scientists from the United States and the United Kingdom. During the 2 1/2 days of the workshop, a number of issues relating to obtaining frequency-stable operation and to the catalytic control of laser gas chemistry were discussed, and specific recommendations concerning future activities were drafted.

Dosimetric evaluation of lithium carbonate (Li2CO3) as a dosemeter for gamma-radiation dose measurements.

Science.gov (United States)

Popoca, R; Ureña-Núñez, F

2009-06-01

This work reports the possibility of using lithium carbonate as a dosimetric material for gamma-radiation measurements. Carboxi-radical ions, CO(2)(-) and CO(3)(-), arise from the gamma irradiation of Li(2)CO(3), and these radical ions can be quantified by electron paramagnetic resonance (EPR) spectrometry. The EPR-signal response of gamma-irradiated lithium carbonate has been investigated to determine some dosimetric characteristics such as: peak-to-peak signal intensity versus gamma dose received, zero-dose response, signal fading, signal repeatability, batch homogeneity, dose rate effect and stability at different environmental conditions. Using the conventional peak-to-peak method of stable ion radicals, it is concluded that lithium carbonate could be used as a gamma dosemeter in the range of 3-100 Gy.

Mesoporous carbon composite for CO{sub 2} capture

Energy Technology Data Exchange (ETDEWEB)

Hwang, Chih-Chau; Jin, Zhong; Lu, Wei; Sun, Zhengzong; Alemany, Lawrence; Tour, James M. [Rice University, Houston, TX (United States); Lomeda, Jay R.; Flatt, Austen K. [Nalco Company, Naperville, IL (United States)

2012-07-01

Herein we report a carbon based technology that can be used to rapidly adsorb and release CO{sub 2}. CO{sub 2} uptake by the synthesized composites was determined using a gravimetric method at room temperature and atmospheric pressure. 39% polyethylenimine-mesocarbon (PEI-CMK-3) composite had {approx} 12 wt% CO{sub 2} uptake capacity and a 37% polyvinylamine meso-carbon (PVA-CMK-3) composite had {approx} 13 wt% CO{sub 2} uptake capacity. The sorbents were easily regenerated at 75 deg C and exhibit excellent stability over multiple regeneration cycles. CO{sub 2} uptake was equivalent when using 10% CO{sub 2} in 90% CH{sub 4}, C{sub 2}H{sub 6} and C{sub 3}H{sub 9} mixture, underscoring the efficacy for CO{sub 2} separation from natural gas. (author)

Faults as Windows to Monitor Gas Seepage: Application to CO2 Sequestration and CO2-EOR

Directory of Open Access Journals (Sweden)

Ronald W. Klusman

2018-03-01

Full Text Available Monitoring of potential gas seepage for CO2 sequestration and CO2-EOR (Enhanced Oil Recovery in geologic storage will involve geophysical and geochemical measurements of parameters at depth and at, or near the surface. The appropriate methods for MVA (Monitoring, Verification, Accounting are needed for both cost and technical effectiveness. This work provides an overview of some of the geochemical methods that have been demonstrated to be effective for an existing CO2-EOR (Rangely, CA, USA and a proposed project at Teapot Dome, WY, USA. Carbon dioxide and CH4 fluxes and shallow soil gas concentrations were measured, followed by nested completions of 10-m deep holes to obtain concentration gradients. The focus at Teapot Dome was the evaluation of faults as pathways for gas seepage in an under-pressured reservoir system. The measurements were supplemented by stable carbon and oxygen isotopic measurements, carbon-14, and limited use of inert gases. The work clearly demonstrates the superiority of CH4 over measurements of CO2 in early detection and quantification of gas seepage. Stable carbon isotopes, carbon-14, and inert gas measurements add to the verification of the deep source. A preliminary accounting at Rangely confirms the importance of CH4 measurements in the MVA application.

Precipitation of hydrated Mg carbonate with the aid of carbonic anhydrase for CO2 sequestration

Science.gov (United States)

Power, I. M.; Harrison, A. L.; Dipple, G. M.

2011-12-01

Strategies for sequestering CO2 directly from the atmosphere are likely required to achieve the desired reduction in CO2 concentration and avoid the most damaging effects of climate change [1]. Numerous studies have demonstrated the accelerated precipitation of calcium carbonate minerals with the aid of carbonic anhydrase (CA) as a means of sequestering CO2 in solid carbonate form; however, no study has examined precipitation of magnesium carbonate minerals using CA. Precipitation of magnesite (MgCO3) is kinetically inhibited [2]; therefore, Mg2+ must be precipitated as hydrated carbonate minerals. In laboratory experiments, the uptake of atmospheric CO2 into brine solutions (0.1 M Mg) was rate-limiting for the precipitation of dypingite [Mg5(CO3)4(OH)2-5H2O] with initial precipitation requiring 15 days [3]. It was also found that dypingite precipitation outpaced the uptake of CO2 gas into solution. CO2 uptake is limited by the hydration of CO2 to form carbonate ions [4]. Carbonic anhydrase (CA) enzymes are among the fastest known in nature and are able to catalyze the hydration of CO2, i.e., converting CO2(aq) to CO32- and HCO3- [5]. CA plays an important role in the carbon concentrating mechanism of photoautotrophic, chemoautotrophic, and heterotrophic prokaryotes and is involved in pH homeostasis, facilitated diffusion of CO2, ion transport, and the interconversion of CO2 and HCO3- [6]. Introducing CA into buffered Mg-rich solutions should allow for more rapid precipitation of hydrated magnesium carbonate minerals. Batch experiments were conducted using 125 mL flasks containing 100 mL of Millipore deionized water with 0.2 M of MgCl2-6H2O. To buffer pH, 1.0 g of pulverized brucite [Mg(OH)2] or 1.0 g of NaOH was added to the systems, which were amended with Bovine carbonic anhydrase (BCA) (Sigma-Aldrich). Solutions were stirred continuously and kept at room temperature (~22°C) with laboratory air introduced by bubbling. Temperature and pH were measured routinely

Ordered nanoporous carbon for increasing CO2 capture

International Nuclear Information System (INIS)

Yoo, Hye-Min; Lee, Seul-Yi; Park, Soo-Jin

2013-01-01

Ordered nanoporous carbons (ONCs) were prepared using a soft-templating method. The prepared ONCs materials were subjected to a controlled carbonization temperature over the temperature range, 700–1000 °C, to increase the specific surface area and total pore volume of ordered nanoporous carbon followed by carbonization of the phenolic resin. ONCs materials synthesized at various carbonization temperatures were used as adsorbents to improve the CO 2 adsorption efficiency. The surface properties of the ONCs materials were examined by X-ray photoelectron spectroscopy. The structural properties of the ONCs materials were analyzed by X-ray diffraction. The textural properties of the ONCs materials were examined using the N 2 /77 K adsorption isotherms according to the Brunauer–Emmett–Teller equation. The CO 2 adsorption capacity was measured by CO 2 isothermal adsorption at 298 K/30 bar and 298 K/1 bar. The carbonization temperature was found to have a major effect on the CO 2 adsorption capacity, resulting from the specific surface area and total pore volumes of the ONCs materials. - Graphical abstract: This schematic diagram described synthesis of ONCs. Highlights: ► ONCs materials can be prepared readily using the direct-triblock-copolymer-templating method. ► The distributions show that prominent development can be observed around the micro-pore region. ► The soft-templating method provides opportunities for controlling the pore structure of ONCs. ► From thermal power plants for CO2 capture by adsorption technology, is a new direction.

Effects of euthanasia method on stable-carbon and stable-nitrogen isotope analysis for an ectothermic vertebrate.

Science.gov (United States)

Atwood, Meredith A

2013-04-30

Stable isotope analysis is a critical tool for understanding ecological food webs; however, results can be sensitive to sample preparation methods. To limit the possibility of sample contamination, freezing is commonly used to euthanize invertebrates and preserve non-lethal samples from vertebrates. For destructive sampling of vertebrates, more humane euthanasia methods are preferred to freezing and it is essential to evaluate how these euthanasia methods affect stable isotope results. Stable isotope ratios and elemental composition of carbon and nitrogen were used to evaluate whether the euthanasia method compromised the integrity of the sample for analysis. Specifically, the stable isotope and C:N ratios were compared for larval wood frogs (Rana sylvatica  =  Lithobates sylvaticus), an ectothermic vertebrate, that had been euthanized by freezing with four different humane euthanasia methods: CO2, benzocaine, MS-222 (tricaine methanesulfonate), and 70% ethanol. The euthanasia method was not related to the δ(13)C or δ(15)N values and the comparisons revealed no differences between freezing and any of the other treatments. However, there were slight (non-significant) differences in the isotope ratios of benzocaine and CO2 when each was compared with freezing. The elemental composition was altered by the euthanasia method employed. The percentage nitrogen was higher in CO2 treatments than in freezing, and similar (non-significant) trends were seen for ethanol treatments relative to freezing. The resulting C:N ratios were higher for benzocaine treatments than for both CO2 and ethanol. Similar (non-significant) trends suggested that the C:N ratios were also higher for animals euthanized by freezing than for both CO2 and ethanol euthanasia methods. The euthanasia method had a larger effect on elemental composition than stable isotope ratios. The percentage nitrogen and the subsequent C:N ratios were most affected by the CO2 and ethanol euthanasia methods, whereas

Investigation of the potential of coal combustion fly ash for mineral sequestration of CO2 by accelerated carbonation

International Nuclear Information System (INIS)

Ukwattage, N.L.; Ranjith, P.G.; Wang, S.H.

2013-01-01

Mineral carbonation of alkaline waste materials is being studied extensively for its potential as a way of reducing the increased level of CO 2 in the atmosphere. Carbonation converts CO 2 into minerals which are stable over geological time scales. This process occurs naturally but slowly, and needs to be accelerated to offset the present rate of emissions from power plants and other emission sources. The present study attempts to identify the potential of coal fly ash as a source for carbon storage (sequestration) through ex-situ accelerated mineral carbonation. In the study, two operational parameters that could affect the reaction process were tested to investigate their effect on mineralization. Coal fly ash was mixed with water to different water-to-solid ratios and samples were carbonated in a pressure vessel at different initial CO 2 pressures. Temperature was kept constant at 40 °C. According to the results, one ton of Hazelwood fly ash could sequester 7.66 kg of CO 2 . The pressure of CO 2 inside the vessel has an effect on the rate of CO 2 uptake and the water-to-solid ratio affects the weight gain after the carbonation of fly ash. The results confirm the possibility of the manipulation of process parameters in enhancing the carbonation reaction. - Highlights: ► Mineral sequestration CO 2 by of coal fly ash is a slow process under ambient conditions. ► It can be accelerated by manipulating the process parameters inside a reactor. ► Initial CO 2 pressure and water to solid mixing ratio inside the reactor are two of those operational parameters. ► According to the test results higher CO 2 initial pressure gives higher on rates of CO 2 sequestration. ► Water to fly ash mixing ratio effect on amount of CO 2 sequestered into fly ash

Preliminary Study: Application of Off-Axis ICOS to Determine Stable Carbon Isotope in Dissolved Inorganic Carbon

Science.gov (United States)

Kim, Y. T.; Lee, J. M.; Hwang, J. H.; Piao, J.; Woo, N. C.

2015-12-01

CO2 is one of the major causes for global climate change. Because stable carbon isotope ratio is used to trace carbon source, several analytical techniques likes IRMS (Isotope Ratio Mass Spectrometry) and LAS (Laser Absorption Spectrometry) were extensively used. Off-axis ICOS, a kind of LAS, has merits on long-term stability and field application, therefore it is widely being used in CCS (Carbon Capture and Storage) field. The aim of this study is to extend the application scope of OA-ICOS to determine dissolved inorganic carbon (DIC). Because OA-ICOS showed dependence of δ13C on CO2 concentration, data processing is required. We tested CO2 Carbon Isotope Analyzer (CCIA-36-EP, Los Gatos Research) with both reference gas (δ13C= -28.28‰) and aqueous solutions prepared by dissolving sodium bicarbonate standards (δ13C= -12.26‰ and +3.96‰). The differences of δ13C between reference and measurement values are plotted by CO2 concentrations, then compared. At first, we checked the similarity between our curve pattern for reference gas and Guillon's research (δ13C= -43.99‰) by other Analyzer. To analyze aqueous samples, more errors can be caused than gas analysis. The carbon isotope fractionation occurs during dissolving standard reagents and extracting DIC as CO2 gas form. This effect is mixed with CO2 concentration dependence effect, therefore the curve patterns are different with that for reference gas. Our experiments are done for various δ13C values. It could be an important point to use OA-ICOS to analyze DIC, too.

Measurement of organic carbon stable isotope composition of different soil types by EA-IRMS system

International Nuclear Information System (INIS)

Qi Biao; Ding Lingling; Cui Jiehua; Wang Yanhong

2009-01-01

Element analyzer-isotope ratio mass spectrometers (EA-IRMS) is a rapid and precise method for measuring stable carbon isotope. Pure CO 2 reference gas was calibrated via international standard-Urea, and the δ 13 C us PDB value of pure CO 2 is (-29.523 ± 0.0181)%. Stability and linearity of the EA-IRMS system, precision of δ 13 C measurement for samples were tested through experimental comparison. Moreover, determination method of organic carbon stable isotope in soil was based on the system. The EA-IRMS system had well linearity when ion intensity ranged from 1.0 to 7.0V, and it excelled the total linearity when the ion intensity was from 1.5 to 5.0V, and the accurate result of δ 13 C for sample analysis could be obtained with precision of 0.015%. If carbon content in sample is more than 5μg, the requirement for analyzing accurate result of δ 13 C could be achieved. The organic carbon stable isotope was measured in 18 different types soil samples, the average natural abundance of 13 C was 1.082%, and the organic carbon stable isotope composition was significantly different among different type soils. (authors)

Enhancing Catalyzed Decomposition of Na2CO3 with Co2MnO x Nanowire-Decorated Carbon Fibers for Advanced Na-CO2 Batteries.

Science.gov (United States)

Fang, Cong; Luo, Jianmin; Jin, Chengbin; Yuan, Huadong; Sheng, Ouwei; Huang, Hui; Gan, Yongping; Xia, Yang; Liang, Chu; Zhang, Jun; Zhang, Wenkui; Tao, Xinyong

2018-05-23

The metal-CO 2 batteries, especially Na-CO 2 , batteries come into sight owing to their high energy density, ability for CO 2 capture, and the abundance of sodium resource. Besides the sluggish electrochemical reactions at the gas cathodes and the instability of the electrolyte at a high voltage, the final discharge product Na 2 CO 3 is a solid and poor conductor of electricity, which may cause the high overpotential and poor cycle performance for the Na-CO 2 batteries. The promotion of decomposition of Na 2 CO 3 should be an efficient strategy to enhance the electrochemical performance. Here, we design a facile Na 2 CO 3 activation experiment to screen the efficient cathode catalyst for the Na-CO 2 batteries. It is found that the Co 2 MnO x nanowire-decorated carbon fibers (CMO@CF) can promote the Na 2 CO 3 decomposition at the lowest voltage among all these metal oxide-decorated carbon fiber structures. After assembling the Na-CO 2 batteries, the electrodes based on CMO@CF show lower overpotential and better cycling performance compared with the electrodes based on pristine carbon fibers and other metal oxide-modified carbon fibers. We believe this catalyst screening method and the freestanding structure of the CMO@CF electrode may provide an important reference for the development of advanced Na-CO 2 batteries.

Automated determination of the stable carbon isotopic composition (δ13C) of total dissolved inorganic carbon (DIC) and total nonpurgeable dissolved organic carbon (DOC) in aqueous samples: RSIL lab codes 1851 and 1852

Science.gov (United States)

Révész, Kinga M.; Doctor, Daniel H.

2014-01-01

The purposes of the Reston Stable Isotope Laboratory (RSIL) lab codes 1851 and 1852 are to determine the total carbon mass and the ratio of the stable isotopes of carbon (δ13C) for total dissolved inorganic carbon (DIC, lab code 1851) and total nonpurgeable dissolved organic carbon (DOC, lab code 1852) in aqueous samples. The analysis procedure is automated according to a method that utilizes a total carbon analyzer as a peripheral sample preparation device for analysis of carbon dioxide (CO2) gas by a continuous-flow isotope ratio mass spectrometer (CF-IRMS). The carbon analyzer produces CO2 and determines the carbon mass in parts per million (ppm) of DIC and DOC in each sample separately, and the CF-IRMS determines the carbon isotope ratio of the produced CO2. This configuration provides a fully automated analysis of total carbon mass and δ13C with no operator intervention, additional sample preparation, or other manual analysis. To determine the DIC, the carbon analyzer transfers a specified sample volume to a heated (70 °C) reaction vessel with a preprogrammed volume of 10% phosphoric acid (H3PO4), which allows the carbonate and bicarbonate species in the sample to dissociate to CO2. The CO2 from the reacted sample is subsequently purged with a flow of helium gas that sweeps the CO2 through an infrared CO2 detector and quantifies the CO2. The CO2 is then carried through a high-temperature (650 °C) scrubber reactor, a series of water traps, and ultimately to the inlet of the mass spectrometer. For the analysis of total dissolved organic carbon, the carbon analyzer performs a second step on the sample in the heated reaction vessel during which a preprogrammed volume of sodium persulfate (Na2S2O8) is added, and the hydroxyl radicals oxidize the organics to CO2. Samples containing 2 ppm to 30,000 ppm of carbon are analyzed. The precision of the carbon isotope analysis is within 0.3 per mill for DIC, and within 0.5 per mill for DOC.

Carbon Balance at Landscape Level inferred fromTower CO2 Concentration Measurements

Science.gov (United States)

Chen, J. M.; Chen, B.; Higuchi, K.; Chan, D.; Shashkov, A.; Lin, H.; Liu, J.

2003-04-01

Terrestrial carbon sinks are considerable in the global carbon budget, but the accumulation of carbon in terrestrial ecosystems is very small (~0.2% per year) relative to the total carbon stocks in forests. Currently, eddy-covariance instruments mounted on towers are the only reliable means to measure carbon balance of a land surface, albeit limited to small areas and not free of caveats. In our quest of understanding the collective performance of ecosystems under the changing climate, it is highly desirable to have the ability to acquire carbon cycle information for large areas (landscape) consisting of patches of different ecosystems. For this purpose we explored methodologies of inferring carbon cycle information from tower CO2 concentration measurements affected by large areas (100-10000 km2). An ecosystem model named Boreal Ecosystem Productivity Simulator (BEPS) is coupled with a carbon-specific Vertical Diffusion Scheme (VDS) in order to decipher temporal variations in CO2 for landscape-level photosynthesis and respiration information. The coupled BEPS-VDS is applied to a unique 9-year (1990-2000 with 1997-8 missing data) 5-minute CO2 record measured on a 40-m tower over boreal forests near Fraserdale, Ontario, Canada. Over the period, the mean diurnal amplitude of the measured CO2 at 40 m increased by 5.58 ppmv, or 28% in the growing season. The increase in nighttime ecosystem respiration, causing the increase in the daily maximum CO2 concentration, was responsible for 65% of the increase in the diurnal amplitude, i.e., 3.61 ppmv, corresponding to an increase in the mean daily air temperature by about 2.77 degC and precipitation by 5% over the same period. The rest (35%) is explained by the increase in ecosystem daytime photosynthesis, causing the decrease in the daily minimum CO2 concentration. As the nighttime stable boundary layer (SBL) (270-560 m) was much shallower than the daytime convective boundary layer (CBL) (1000-1600 m), the increase in

Carbonation and CO2 uptake of concrete

International Nuclear Information System (INIS)

Yang, Keun-Hyeok; Seo, Eun-A; Tae, Sung-Ho

2014-01-01

This study developed a reliable procedure to assess the carbon dioxide (CO 2 ) uptake of concrete by carbonation during the service life of a structure and by the recycling of concrete after demolition. To generalize the amount of absorbable CO 2 per unit volume of concrete, the molar concentration of carbonatable constituents in hardened cement paste was simplified as a function of the unit content of cement, and the degree of hydration of the cement paste was formulated as a function of the water-to-cement ratio. The contribution of the relative humidity, type of finishing material for the concrete surface, and the substitution level of supplementary cementitious materials to the CO 2 diffusion coefficient in concrete was reflected using various correction factors. The following parameters varying with the recycling scenario were also considered: the carbonatable surface area of concrete crusher-runs and underground phenomena of the decreased CO 2 diffusion coefficient and increased CO 2 concentration. Based on the developed procedure, a case study was conducted for an apartment building with a principal wall system and an office building with a Rahmen system, with the aim of examining the CO 2 uptake of each structural element under different exposure environments during the service life and recycling of the building. As input data necessary for the case study, data collected from actual surveys conducted in 2012 in South Korea were used, which included data on the surrounding environments, lifecycle inventory database, life expectancy of structures, and recycling activity scenario. Ultimately, the CO 2 uptake of concrete during a 100-year lifecycle (life expectancy of 40 years and recycling span of 60 years) was estimated to be 15.5%–17% of the CO 2 emissions from concrete production, which roughly corresponds to 18%–21% of the CO 2 emissions from the production of ordinary Portland cement. - Highlights: • CO 2 uptake assessment approach owing to the

Carbon Dioxide (CO2) in Blood: MedlinePlus Lab Test Information

Science.gov (United States)

... this page: https://medlineplus.gov/labtests/carbondioxideco2inblood.html Carbon Dioxide (CO2) in Blood To use the sharing features ... this page, please enable JavaScript. What is a Carbon Dioxide (CO2) Blood Test? Carbon dioxide (CO2) is an ...

Effect of Mineral Dissolution/Precipitation and CO2 Exsolution on CO2 transport in Geological Carbon Storage.

Science.gov (United States)

Xu, Ruina; Li, Rong; Ma, Jin; He, Di; Jiang, Peixue

2017-09-19

Geological carbon sequestration (GCS) in deep saline aquifers is an effective means for storing carbon dioxide to address global climate change. As the time after injection increases, the safety of storage increases as the CO 2 transforms from a separate phase to CO 2 (aq) and HCO 3 - by dissolution and then to carbonates by mineral dissolution. However, subsequent depressurization could lead to dissolved CO 2 (aq) escaping from the formation water and creating a new separate phase which may reduce the GCS system safety. The mineral dissolution and the CO 2 exsolution and mineral precipitation during depressurization change the morphology, porosity, and permeability of the porous rock medium, which then affects the two-phase flow of the CO 2 and formation water. A better understanding of these effects on the CO 2 -water two-phase flow will improve predictions of the long-term CO 2 storage reliability, especially the impact of depressurization on the long-term stability. In this Account, we summarize our recent work on the effect of CO 2 exsolution and mineral dissolution/precipitation on CO 2 transport in GCS reservoirs. We place emphasis on understanding the behavior and transformation of the carbon components in the reservoir, including CO 2 (sc/g), CO 2 (aq), HCO 3 - , and carbonate minerals (calcite and dolomite), highlight their transport and mobility by coupled geochemical and two-phase flow processes, and consider the implications of these transport mechanisms on estimates of the long-term safety of GCS. We describe experimental and numerical pore- and core-scale methods used in our lab in conjunction with industrial and international partners to investigate these effects. Experimental results show how mineral dissolution affects permeability, capillary pressure, and relative permeability, which are important phenomena affecting the input parameters for reservoir flow modeling. The porosity and the absolute permeability increase when CO 2 dissolved water is

Carbonation of alkaline paper mill waste to reduce CO{sub 2} greenhouse gas emissions into the atmosphere

Energy Technology Data Exchange (ETDEWEB)

Perez-Lopez, R. [Laboratoire de Geophysique Interne et Tectonophysique, CNRS-OSUG-UJF, Universite Joseph Fourier Grenoble I, Maison des Geosciences, BP 53, 38041 Grenoble Cedex (France); Department of Geology, University of Huelva, Campus ' El Carmen' , 21071 Huelva (Spain)], E-mail: rafael.perez@dgeo.uhu.es; Montes-Hernandez, G. [Laboratoire de Geophysique Interne et Tectonophysique, CNRS-OSUG-UJF, Universite Joseph Fourier Grenoble I, Maison des Geosciences, BP 53, 38041 Grenoble Cedex (France); Nieto, J.M. [Department of Geology, University of Huelva, Campus ' El Carmen' , 21071 Huelva (Spain); Renard, F. [Laboratoire de Geodynamique des Chaines Alpines, CNRS-OSUG-UJF, Universite Joseph Fourier Grenoble I, Maison des Geosciences, BP 53, 38041 Grenoble Cedex (France); Physics of Geological Processes, University of Oslo (Norway); Charlet, L. [Laboratoire de Geophysique Interne et Tectonophysique, CNRS-OSUG-UJF, Universite Joseph Fourier Grenoble I, Maison des Geosciences, BP 53, 38041 Grenoble Cedex (France)

2008-08-15

The global warming of Earth's near-surface, air and oceans in recent decades is a direct consequence of anthropogenic emission of greenhouse gases into the atmosphere such as CO{sub 2}, CH{sub 4}, N{sub 2}O and CFCs. The CO{sub 2} emissions contribute approximately 60% to this climate change. This study investigates experimentally the aqueous carbonation mechanisms of an alkaline paper mill waste containing about 55 wt% portlandite (Ca(OH){sub 2}) as a possible mineralogical CO{sub 2} sequestration process. The overall carbonation reaction includes the following steps: (1) Ca release from portlandite dissolution, (2) CO{sub 2} dissolution in water and (3) CaCO{sub 3} precipitation. This CO{sub 2} sequestration mechanism was supported by geochemical modelling of final solutions using PHREEQC software, and observations by scanning electron microscope and X-ray diffraction of final reaction products. According to the experimental protocol, the system proposed would favour the total capture of approx. 218 kg of CO{sub 2} into stable calcite/ton of paper waste, independently of initial CO{sub 2} pressure. The final product from the carbonation process is a calcite (ca. 100 wt%)-water dispersion. Indeed, the total captured CO{sub 2} mineralized as calcite could be stored in degraded soils or even used for diverse industrial applications. This result demonstrates the possibility of using the alkaline liquid-solid waste for CO{sub 2} mitigation and reduction of greenhouse effect gases into the atmosphere.

Carbonation of Mg(OH){sub 2} in a pressurised fluidised bed for CO{sub 2} sequestration

Energy Technology Data Exchange (ETDEWEB)

Fagerlund, J.

2012-07-01

, but unfortunately, Mg(OH){sub 2} dehydroxylation is also affected and seemingly to a higher extent than MgCO{sub 3} formation. Although MgCO{sub 3} is thermodynamically more stable than MgO at most of the conditions investigated for this thesis, the presence of MgO in the end product has not been avoided. In other words, not all the decomposing hydroxide is able to form carbonate and the formed MgO is unreactive towards CO{sub 2} in the absence of steam. In addition, the formation of a comparatively rare crystalline carbonate form, referred to as oxymagnesite, has been detected over a range of dry or mildly dry carbonation conditions. Most of the PFB carbonation experiments have been performed (for reasons of availability) using commercially available Mg(OH){sub 2} (Dead Sea Periclase Ltd., i.e. DSP), which is much less reactive than the hydroxide produced from serpentinite (a common Mg-silicate rock) according to the first two steps of the process addressed in this thesis. At similar conditions (< 15 min, 20 bar, 500 deg C), the carbonation of serpentinite derived Mg(OH){sub 2} exceeds that of DSP-Mg(OH){sub 2} by 100%. The low reactivity of DSPMg( OH){sub 2} is not only a result of low surface area (approx 5.5 m2/g), but also of low porosity (approx 0.024 cm3/g), which apparently prevents CO{sub 2} from entering the particle, but not H{sub 2}O (which is smaller than CO{sub 2}) from exiting. The importance of water for the carbonation reaction has been demonstrated, and the reactivity of MgO in the absence of H{sub 2}O is negligible even at comparatively high CO{sub 2} pressures (20 bar). Thus it is important that excessive dehydroxylation, i.e. dehydroxylation without sequential carbonate formation, is prevented. Preliminary kinetic modelling of the carbonation step, assuming an intermediate hydrated MgO-species is produced, showed that a delicate balance between the various factors (temperature, partial pressures, fluidisation velocity and particle properties

CO2 uptake potential due to concrete carbonation: A case study

Directory of Open Access Journals (Sweden)

Edna Possan

2017-06-01

Full Text Available The cement manufacturing process accounts for about 5% CO2 (carbon dioxide released into the atmosphere. However, during its life cycle, concrete may capture CO2 through carbonation, in order to, partially, offset the impact of its production. Thus, this paper aims at studying the CO2 uptake potential of the Itaipu Dam due to concrete carbonation of such material. So, 155 cores were extracted from the concrete dam in different points to measure carbonation depth. In order to evaluate its influence on carbonation, the measurement of internal moisture distribution in concrete was also carried out. The results have shown that carbonation takes part of the whole dam area, indicating CO2 uptake potential. Up to the present moment, 13,384 tons of CO2 have been absorbed by concrete carbonation of the Itaipu Dam.

Carboxysomal carbonic anhydrases: Structure and role in microbial CO2 fixation

Energy Technology Data Exchange (ETDEWEB)

Cannon, Gordon C.; Heinhorst, Sabine; Kerfeld, Cheryl A.

2010-06-23

Cyanobacteria and some chemoautotrophic bacteria are able to grow in environments with limiting CO2 concentrations by employing a CO2-concentrating mechanism (CCM) that allows them to accumulate inorganic carbon in their cytoplasm to concentrations several orders of magnitude higher than that on the outside. The final step of this process takes place in polyhedral protein microcompartments known as carboxysomes, which contain the majority of the CO2-fixing enzyme, RubisCO. The efficiency of CO2 fixation by the sequestered RubisCO is enhanced by co-localization with a specialized carbonic anhydrase that catalyzes dehydration of the cytoplasmic bicarbonate and ensures saturation of RubisCO with its substrate, CO2. There are two genetically distinct carboxysome types that differ in their protein composition and in the carbonic anhydrase(s) they employ. Here we review the existing information concerning the genomics, structure and enzymology of these uniquely adapted carbonic anhydrases, which are of fundamental importance in the global carbon cycle.

The Density and Compressibility of BaCO3-SrCO3-CaCO3-K2CO3-Na2CO3-Li2CO3 Liquids: New Measurements and a Systematic Trend with Cation Field Strength

Science.gov (United States)

Hurt, S. M.; Lange, R. A.; Ai, Y.

2015-12-01

The volumetric properties of multi-component carbonate liquids are required to extend thermodynamic models that describe partial melting of the deep mantle (e.g. pMELTS; Ghiorso et al., 2003) to carbonate-bearing lithologies. Carbonate in the mantle is an important reservoir of carbon, which is released to the atmosphere as CO2 through volcanism, and thus contributes to the carbon cycle. Although MgCO3 is the most important carbonate component in the mantle, it is not possible to directly measure the 1-bar density and compressibility of MgCO3 liquid because, like other alkaline-earth carbonates, it decomposes at a temperature lower than its melting temperature. Despite this challenge, Liu and Lange (2003) and O'Leary et al. (2015) showed that the one bar molar volume, thermal expansion and compressibility of the CaCO3 liquid component could be obtained by measuring the density and sound speeds of stable liquids in the CaCO3-Li2CO3-Na2CO3-K2CO3 quaternary system at one bar. In this study, this same strategy is employed on SrCO3- and BaCO3-bearing alkali carbonate liquids. The density and sound speed of seven liquids in the SrCO3-Li2CO3-Na2CO3-K2CO3 quaternary and three liquids in the BaCO3-Li2CO3-Na2CO3-K2CO3 quaternary were measured from 739-1367K, with SrCO3 and BaCO3 concentrations ranging from 10-50 mol%. The density measurements were made using the double-bob Archimedean method and sound speeds were obtained with a frequency-sweep acoustic interferometer. The molar volume and sound speed measurements were used to calculate the isothermal compressibility of each liquid, and the results show the volumetric properties mix ideally with composition. The partial molar volume and compressibility of the SrCO3 and BaCO3 components are compared to those obtained for the CaCO3 component as a function of cation field strength. The results reveal a systematic trend that allows the partial molar volume and compressibility of the MgCO3 liquid component to be estimated.

Carbon Deposition in Solid Oxide Cells during Co-Electrolysis of H2O and CO2

DEFF Research Database (Denmark)

Tao, Youkun; Ebbesen, Sune Dalgaard; Mogensen, Mogens Bjerg

2014-01-01

current densities from 1.5 to 2.25 A/cm2 and reactant (H2O + CO2) conversion of up to 67%. Delamination and carbon nano-fibers were observed at the Ni-YSZ|YSZ interface for two cells with a dense microstructure operated at electrolysis current densities of 2.0 and 2.25 A/cm2 and a conversion of 59% and 67...... and the active Ni-YSZ electrode. Carbon nano-fibers were only observed close to the YSZ electrolyte, indicating a very reducing atmosphere and a large over-potential gradient in the active electrode, being highest at the interface to the bulk electrolyte and decreasing toward the Ni-YSZ support.......Carbon formation during co-electrolysis of H2O and CO2 in Ni-YSZ supported Solid Oxide Electrolysis Cells (SOECs) may occur, especially at high current density and high conversion. In order to evaluate the carbon formation limits, five galvanostatic tests were performed in this work at electrolysis...

[Differences and sources of CO2 concentration, carbon and oxygen stable isotope composition between inside and outside of a green space system and influencing factors in an urban area].

Science.gov (United States)

Sun, Shou-jia; Meng, Ping; Zhang, Jin-song; Shu, Jian-hua; Zheng, Ning

2015-10-01

The off-axis integrated cavity output spectroscopy technique was used to measure air CO2 concentration, stable carbon (δ13C) and oxygen (δ18C) isotope ratios on the Fourth Ring Road (FRR) and in the green space system of Beijing Institute of Landscape Architecture (BILA) in summer and winter seasons. The variations of CO2 concentration, δ13C value, δ18C value and the differences of them between the FRR and the BILA, which were correlated with traffic volume and meteorological factors, were analyzed at half-hour timescale. The results showed that traffic volume on the FRR was large both in summer and winter with obvious morning and evening rush hours, and more than 150 thousands vehicles were observed everyday during the observation periods. Diurnal variation of the CO2 concentration showed a two-peak curve both on the FRR and in the green space system of the BILA. In contrast, diurnal variation of δ13C value was a two-trough curve while diurnal variation of δ18O value was a single-trough curve. The differences of CO2 concentration, δ13C value and δ18O value between the FRR and the green space system of BILA in summer were greater than those in winter. The carbon isotope partitioning results showed that in summer vehicle exhaust contributed 64.9% to total atmospheric CO2 of the FRR during measurement time, while heterotrophic respiration contributed 56.3% to total atmospheric CO2 of the green space system in BILA. However, in winter atmospheric CO2 from both the FRR and green space system mostly came from vehicle exhaust. Stepwise regression analysis indicated that differences of CO2 concentration between the FRR and green space system were significantly related to vehicle volume and solar radiation at half-hour timescale, while solar radiation and relative humidity were the main meteorological factors causing δ13 and δ18O differences between the FRR and green space system. Plants in the green space system strongly assimilated CO2 from fossil fuel burning

Cost evaluation of CO2 sequestration by aqueous mineral carbonation

International Nuclear Information System (INIS)

Huijgen, Wouter J.J.; Comans, Rob N.J.; Witkamp, Geert-Jan

2007-01-01

A cost evaluation of CO 2 sequestration by aqueous mineral carbonation has been made using either wollastonite (CaSiO 3 ) or steel slag as feedstock. First, the process was simulated to determine the properties of the streams as well as the power and heat consumption of the process equipment. Second, a basic design was made for the major process equipment, and total investment costs were estimated with the help of the publicly available literature and a factorial cost estimation method. Finally, the sequestration costs were determined on the basis of the depreciation of investments and variable and fixed operating costs. Estimated costs are 102 and 77 EUR/ton CO 2 net avoided for wollastonite and steel slag, respectively. For wollastonite, the major costs are associated with the feedstock and the electricity consumption for grinding and compression (54 and 26 EUR/ton CO 2 avoided, respectively). A sensitivity analysis showed that additional influential parameters in the sequestration costs include the liquid-to-solid ratio in the carbonation reactor and the possible value of the carbonated product. The sequestration costs for steel slag are significantly lower due to the absence of costs for the feedstock. Although various options for potential cost reduction have been identified, CO 2 sequestration by current aqueous carbonation processes seems expensive relative to other CO 2 storage technologies. The permanent and inherently safe sequestration of CO 2 by mineral carbonation may justify higher costs, but further cost reductions are required, particularly in view of (current) prices of CO 2 emission rights. Niche applications of mineral carbonation with a solid residue such as steel slag as feedstock and/or a useful carbonated product hold the best prospects for an economically feasible CO 2 sequestration process. (author)

Carbon balance of China constrained by CONTRAIL aircraft CO2 measurements

Science.gov (United States)

Jiang, F.; Wang, H. M.; Chen, J. M.; Machida, T.; Zhou, L. X.; Ju, W. M.; Matsueda, H.; Sawa, Y.

2014-09-01

Terrestrial carbon dioxide (CO2) flux estimates in China using atmospheric inversion method are beset with considerable uncertainties because very few atmospheric CO2 concentration measurements are available. In order to improve these estimates, nested atmospheric CO2 inversion during 2002-2008 is performed in this study using passenger aircraft-based CO2 measurements over Eurasia from the Comprehensive Observation Network for Trace gases by Airliner (CONTRAIL) project. The inversion system includes 43 regions with a focus on China, and is based on the Bayesian synthesis approach and the TM5 transport model. The terrestrial ecosystem carbon flux modeled by the Boreal Ecosystems Productivity Simulator (BEPS) model and the ocean exchange simulated by the OPA-PISCES-T model are considered as the prior fluxes. The impacts of CONTRAIL CO2 data on inverted China terrestrial carbon fluxes are quantified, the improvement of the inverted fluxes after adding CONTRAIL CO2 data are rationed against climate factors and evaluated by comparing the simulated atmospheric CO2 concentrations with three independent surface CO2 measurements in China. Results show that with the addition of CONTRAIL CO2 data, the inverted carbon sink in China increases while those in South and Southeast Asia decrease. Meanwhile, the posterior uncertainties over these regions are all reduced (2-12%). CONTRAIL CO2 data also have a large effect on the inter-annual variation of carbon sinks in China, leading to a better correlation between the carbon sink and the annual mean climate factors. Evaluations against the CO2 measurements at three sites in China also show that the CONTRAIL CO2 measurements may have improved the inversion results.

Monitoring in situ biodegradation of hydrocarbons by using stable carbon isotopes

International Nuclear Information System (INIS)

Aggarwal, P.K.; Hinchee, R.E.

1991-01-01

Spilled or leaked nonhalogenated petroleum hydrocarbons in the soil can generally be metabolized by indigenous, aerobic bacteria. In situ biological degradation of hydrocarbons may be accelerated by supplying inorganic nutrients and/or oxygen. Approaches to monitoring and verifying enhanced in situ biodegradation have included measurements of changes over time in the (a) concentration of hydrocarbons, (b) temperature, (c) number of hydrocarbon-degrading microorganisms, (d) ratio of fast-degrading hydrocarbons (e.g., pristanes or phytanes), and (e) metabolic intermediates. Measurements of oxygen consumption over time and elevated carbon dioxide concentrations in soil gas also have been used as indicators of hydrocarbon degradation. An alternative approach that may help substantiate biodegradation is to measure stable carbon isotope ratios in soil gas CO 2 . Stable carbon isotope ratio analysis is inexpensive and commercially available at many laboratories. Carbon dioxide produced by hydrocarbon degradation may be distinguished from that produced by other processes based on the carbon isotopic compositions characteristic of the source material and/or fractionation accompanying microbial metabolism. Here the authors demonstrate the applicability of the stable isotope technique for monitoring enhanced. aerobic biodegradation of hydrocarbons using data from three locations in the United States

Utility of thermo-alkali-stable γ-CA from polyextremophilic bacterium Aeribacillus pallidus TSHB1 in biomimetic sequestration of CO2 and as a virtual peroxidase.

Science.gov (United States)

Bose, Himadri; Satyanarayana, Tulasi

2017-04-01

Aeribacillus pallidus TSHB1 polyextremophilic bacterium produces a γ-carbonic anhydrase (ApCA), which is a homotrimeric biocatalyst with a subunit molecular mass of 32 ± 2 kDa. The enzyme is stable in the pH range between 8.0 and 11.0 and thus alkali-stable and moderately thermostable with T 1/2 values of 40 ± 1, 15 ± 1, and 8 ± 0.5 min at 60, 70, and 80 °C, respectively. Activation energy for irreversible inactivation "E d " of carbonic anhydrase is 67.119 kJ mol -1 . The enzyme is stable in the presence of various flue gas contaminants such as SO 3 2- ,SO 4 2- , and NO 3 - and cations Mg 2+ , Mn 2+ , Ca 2+ , and Ba 2+ . Fluorescence studies in the presence of N-bromosuccinimide and fluorescence quenching using KI and acrylamide revealed the importance of tryptophan residues in maintaining the structural integrity of the enzyme. ApCA is more efficient than the commercially available bovine carbonic anhydrase (BCA) in CO 2 sequestration. The enzyme was successfully used in biomineralization of CO 2 from flue gas. Replacement of active site Zn 2+ with Mn 2+ enabled ApCA to function as a peroxidase which exhibited alkali-stability and moderate thermostability like ApCA.

CO{sub 2}-recycling by plants: how reliable is the carbon isotope estimation?

Energy Technology Data Exchange (ETDEWEB)

Siegwolf, R T.W.; Saurer, M [Paul Scherrer Inst. (PSI), Villigen (Switzerland); Koerner, C [Basel Univ., Basel (Switzerland)

1997-06-01

In the study of plant carbon relations, the amount of the respiratory losses from the soil was estimated, determining the gradient of the stable isotope {sup 13}C with increasing plant canopy height. According to the literature 8-26% of the CO{sub 2} released in the forests by soil and plant respiratory processes are reassimilated (recycled) by photosynthesis during the day. Our own measurements however, which we conducted in grass land showed diverging results from no indicating of carbon recycling, to a considerable {delta}{sup 13}C gradient suggesting a high carbon recycling rate. The role of other factors, such as air humidity and irradiation which influence the {delta}{sup 13}C in a canopy as well, are discussed. (author) 3 figs., 4 refs.

Mace-like hierarchical MoS2/NiCo2S4 composites supported by carbon fiber paper: An efficient electrocatalyst for the hydrogen evolution reaction

Science.gov (United States)

Sun, Lan; Wang, Tao; Zhang, Long; Sun, Yunjin; Xu, Kewei; Dai, Zhengfei; Ma, Fei

2018-02-01

The rational design and preparation of earth-abundant, stable and efficient electrocatalysts for hydrogen production is currently the subject in extensive scientific and technological researches toward the future of a clean-energy society. Herein, a mace-like MoS2/NiCo2S4 hierarchical structure is designed and synthesized on carbon fiber paper via a facile hydrothermal method, and evaluated as electrocatalyst for hydrogen evolution reaction. In the MoS2/NiCo2S4/carbon fiber paper hierarchical structures, MoS2 nanosheets are dispersively distributed on the surface of NiCo2S4 nanowires, which provides an enlarged surface area, abundant interfaces and catalytic active sites. As for hydrogen evolution reaction, such MoS2/NiCo2S4/carbon fiber paper heterostructures give rise to a hydrogen evolution reaction catalytic current density of 10 mA cm-2 with a lower overpotential of 139 mV and a smaller Tafel slope of 37 mV·dec-1 than those of MoS2/carbon fiber paper and NiCo2S4/carbon fiber paper counterparts, exhibiting a prominent electrocatalytic performance. Moreover, the electrocatalytic properties change little after 5000 CV cycles and continual electrolysis for 12 h without obvious decay, respectively, demonstrating high durability and stability. The excellent hydrogen evolution reaction performances endow the hierarchical configuration MoS2/NiCo2S4/carbon fiber paper with promising alternative in HER and other related renewable energy fields.

Stable isotope reactive transport modeling in water-rock interactions during CO2 injection

Science.gov (United States)

Hidalgo, Juan J.; Lagneau, Vincent; Agrinier, Pierre

2010-05-01

Stable isotopes can be of great usefulness in the characterization and monitoring of CO2 sequestration sites. Stable isotopes can be used to track the migration of the CO2 plume and identify leakage sources. Moreover, they provide unique information about the chemical reactions that take place on the CO2-water-rock system. However, there is a lack of appropriate tools that help modelers to incorporate stable isotope information into the flow and transport models used in CO2 sequestration problems. In this work, we present a numerical tool for modeling the transport of stable isotopes in groundwater reactive systems. The code is an extension of the groundwater single-phase flow and reactive transport code HYTEC [2]. HYTEC's transport module was modified to include element isotopes as separate species. This way, it is able to track isotope composition of the system by computing the mixing between the background water and the injected solution accounting for the dependency of diffusion on the isotope mass. The chemical module and database have been expanded to included isotopic exchange with minerals and the isotope fractionation associated with chemical reactions and mineral dissolution or precipitation. The performance of the code is illustrated through a series of column synthetic models. The code is also used to model the aqueous phase CO2 injection test carried out at the Lamont-Doherty Earth Observatory site (Palisades, New York, USA) [1]. References [1] N. Assayag, J. Matter, M. Ader, D. Goldberg, and P. Agrinier. Water-rock interactions during a CO2 injection field-test: Implications on host rock dissolution and alteration effects. Chemical Geology, 265(1-2):227-235, July 2009. [2] Jan van der Lee, Laurent De Windt, Vincent Lagneau, and Patrick Goblet. Module-oriented modeling of reactive transport with HYTEC. Computers & Geosciences, 29(3):265-275, April 2003.

A combination of CoO and Co nanoparticles supported on electrospun carbon nanofibers as highly stable air electrodes

Science.gov (United States)

Alegre, Cinthia; Busacca, Concetta; Di Blasi, Orazio; Antonucci, Vincenzo; Aricò, Antonino Salvatore; Di Blasi, Alessandra; Baglio, Vincenzo

2017-10-01

Bifunctional materials able to catalyze both the oxygen reduction (ORR) and the oxygen evolution (OER) reactions in alkaline media are still a challenge for the progress of energy conversion and storage devices such as metal-air batteries or unitized regenerative fuel cells. In this work, carbon nanofibers synthesized by electrospinning are modified with a combination of cobalt oxide and metallic cobalt (CoO-Co/CNF) and studied as a bifunctional air electrode for metal-air batteries. The performance of CoO-Co/CNF for both reactions is compared with state-of-the-art catalysts such as Pt/C and IrO2. The combination of cobalt oxide and metallic cobalt, finely distributed on the surface of graphitic carbon nanofibers, leads to a bifunctional catalyst with a half-wave potential for the ORR slightly better than Pt/C and a reversibility (ΔEOER-ORR) of 809 mV. The stability of CoO-Co/CNF is assessed by means of different stress tests: polarizations at high electrochemical potentials (2 V vs. RHE), rapid charge-discharge cycles at ±80 mA cm-2 and long durability tests by charging for 12 h at 60 mA cm-2 and discharging for 8 h at -80 mA cm-2. CoO-Co/CNF shows a remarkable stability, maintaining, at least, an 82% of its performance for the ORR after the stress tests, even when cycled for more than 100 h.

N-doped polypyrrole-based porous carbons for CO{sub 2} capture

Energy Technology Data Exchange (ETDEWEB)

Sevilla, Marta; Valle-Vigon, Patricia; Fuertes, Antonio B. [Instituto Nacional del Carbon (CSIC), P.O. Box 73, 33080 Oviedo (Spain)

2011-07-22

Highly porous N-doped carbons have been successfully prepared by using KOH as activating agent and polypyrrole (PPy) as carbon precursor. These materials were investigated as sorbents for CO{sub 2} capture. The activation process was carried out under severe (KOH/PPy = 4) or mild (KOH/PPy = 2) activation conditions at different temperatures in the 600-800 C range. Mildly activated carbons have two important characteristics: i) they contain a large number of nitrogen functional groups (up to 10.1 wt% N) identified as pyridonic-N with a small proportion of pyridinic-N groups, and ii) they exhibit, in relation to the carbons prepared with KOH/PPy = 4, narrower micropore sizes. The combination of both of these properties explains the large CO{sub 2} adsorption capacities of mildly activated carbon. In particular, a very high CO{sub 2} adsorption uptake of 6.2 mmol.g{sup -1} (0 C) was achieved for porous carbons prepared with KOH/PPy = 2 and 600 C (1700 m{sup 2}.g{sup -1}, pore size {approx} 1 nm and 10.1 wt% N. Furthermore, we observed that these porous carbons exhibit high CO{sub 2} adsorption rates, a good selectivity for CO{sub 2}-N{sub 2} separation and it can be easily regenerated. (Copyright copyright 2011 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

A method for permanent CO2 mineral carbonation

Energy Technology Data Exchange (ETDEWEB)

Dahlin, David C.; O' Connor, William K.; Nilsen, David N.; Rush, G.E.; Walters, Richard P.; Turner, Paul C.

2000-01-01

The Albany Research Center (ARC) of the U.S. Department of Energy (DOE) has been conducting research to investigate the feasibility of mineral carbonation as a method for carbon dioxide (CO2) sequestration. The research is part of a Mineral Carbonation Study Program within the Office of Fossil Energy in DOE. Other participants in this Program include DOE?s Los Alamos National Laboratory and National Energy Technology Laboratory, Arizona State University, and Science Applications International Corporation. The research has focused on ex-situ mineral carbonation in an aqueous system. The process developed at ARC reacts a slurry of magnesium silicate mineral with supercritical CO2 to produce a solid magnesium carbonate product. To date, olivine and serpentine have been used as the mineral reactant, but other magnesium silicates could be used as well. The process is designed to simulate the natural serpentinization reaction of ultramafic minerals, and consequently, these results may also be applicable to strategies for in-situ geological sequestration. Baseline tests were begun in distilled water on ground products of foundry-grade olivine. Tests conducted at 150 C and subcritical CO2 pressures (50 atm) resulted in very slow conversion to carbonate. Increasing the partial pressure of CO2 to supercritical (>73 atm) conditions, coupled with agitation of the slurry and gas dispersion within the water column, resulted in significant improvement in the extent of reaction in much shorter reaction times. A change from distilled water to a bicarbonate/salt solution further improved the rate and extent of reaction. When serpentine, a hydrated mineral, was used instead of olivine, extent of reaction was poor until heat treatment was included prior to the carbonation reaction. Removal of the chemically bound water resulted in conversion to carbonate similar to those obtained with olivine. Recent results have shown that conversions of nearly 80 pct are achievable after 30 minutes

CO2 bubble generation and migration during magma-carbonate interaction

Science.gov (United States)

Blythe, L. S.; Deegan, F. M.; Freda, C.; Jolis, E. M.; Masotta, M.; Misiti, V.; Taddeucci, J.; Troll, V. R.

2015-04-01

We conducted quantitative textural analysis of vesicles in high temperature and pressure carbonate assimilation experiments (1200 °C, 0.5 GPa) to investigate CO2 generation and subsequent bubble migration from carbonate into magma. We employed Mt. Merapi (Indonesia) and Mt. Vesuvius (Italy) compositions as magmatic starting materials and present three experimental series using (1) a dry basaltic-andesite, (2) a hydrous basaltic-andesite (2 wt% H2O), and (3) a hydrous shoshonite (2 wt% H2O). The duration of the experiments was varied from 0 to 300 s, and carbonate assimilation produced a CO2-rich fluid and CaO-enriched melts in all cases. The rate of carbonate assimilation, however, changed as a function of melt viscosity, which affected the 2D vesicle number, vesicle volume, and vesicle size distribution within each experiment. Relatively low-viscosity melts (i.e. Vesuvius experiments) facilitated efficient removal of bubbles from the reaction site. This allowed carbonate assimilation to continue unhindered and large volumes of CO2 to be liberated, a scenario thought to fuel sustained CO2-driven eruptions at the surface. Conversely, at higher viscosity (i.e. Merapi experiments), bubble migration became progressively inhibited and bubble concentration at the reaction site caused localised volatile over-pressure that can eventually trigger short-lived explosive outbursts. Melt viscosity therefore exerts a fundamental control on carbonate assimilation rates and, by consequence, the style of CO2-fuelled eruptions.

The influence of non-CO2 forcings on cumulative carbon emissions budgets

Science.gov (United States)

Tokarska, Katarzyna B.; Gillett, Nathan P.; Arora, Vivek K.; Lee, Warren G.; Zickfeld, Kirsten

2018-03-01

Carbon budgets provide a useful tool for policymakers to help meet the global climate targets, as they specify total allowable carbon emissions consistent with limiting warming to a given temperature threshold. Non-CO2 forcings have a net warming effect in the Representative Concentration Pathways (RCP) scenarios, leading to reductions in remaining carbon budgets based on CO2 forcing alone. Carbon budgets consistent with limiting warming to below 2.0 °C, with and without accounting for the effects of non-CO2 forcings, were assessed in inconsistent ways by the Intergovernmental Panel on Climate Change (IPCC), making the effects of non-CO2 forcings hard to identify. Here we use a consistent approach to compare 1.5 °C and 2.0 °C carbon budgets with and without accounting for the effects of non-CO2 forcings, using CO2-only and RCP8.5 simulations. The median allowable carbon budgets for 1.5 °C and 2.0 °C warming are reduced by 257 PgC and 418 PgC, respectively, and the uncertainty ranges on the budgets are reduced by more than a factor of two when accounting for the net warming effects of non-CO2 forcings. While our overall results are consistent with IPCC, we use a more robust methodology, and explain the narrower uncertainty ranges of carbon budgets when non-CO2 forcings are included. We demonstrate that most of the reduction in carbon budgets is a result of the direct warming effect of the non-CO2 forcings, with a secondary contribution from the influence of the non-CO2 forcings on the carbon cycle. Such carbon budgets are expected to play an increasingly important role in climate change mitigation, thus understanding the influence of non-CO2 forcings on these budgets and their uncertainties is critical.

Silvering substrates after CO2 snow cleaning

Science.gov (United States)

Zito, Richard R.

2005-09-01

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

CO2-dependent carbon isotope fractionation in the dinoflagellate Alexandrium tamarense

Science.gov (United States)

Wilkes, Elise B.; Carter, Susan J.; Pearson, Ann

2017-09-01

The carbon isotopic composition of marine sedimentary organic matter is used to resolve long-term histories of pCO2 based on studies indicating a CO2-dependence of photosynthetic carbon isotope fractionation (εP). It recently was proposed that the δ13C values of dinoflagellates, as recorded in fossil dinocysts, might be used as a proxy for pCO2. However, significant questions remain regarding carbon isotope fractionation in dinoflagellates and how such fractionation may impact sedimentary records throughout the Phanerozoic. Here we investigate εP as a function of CO2 concentration and growth rate in the dinoflagellate Alexandrium tamarense. Experiments were conducted in nitrate-limited chemostat cultures. Values of εP were measured on cells having growth rates (μ) of 0.14-0.35 d-1 and aqueous carbon dioxide concentrations of 10.2-63 μmol kg-1 and were found to correlate linearly with μ/[CO2(aq)] (r2 = 0.94) in accord with prior, analogous chemostat investigations with eukaryotic phytoplankton. A maximum fractionation (εf) value of 27‰ was characterized from the intercept of the experiments, representing the first value of εf determined for an algal species employing Form II RubisCO-a structurally and catalytically distinct form of the carbon-fixing enzyme. This value is larger than theoretical predictions for Form II RubisCO and not significantly different from the ∼25‰ εf values observed for taxa employing Form ID RubisCO. We also measured the carbon isotope contents of dinosterol, hexadecanoic acid, and phytol from each experiment, finding that each class of biomarker exhibits different isotopic behavior. The apparent CO2-dependence of εP values in our experiments strengthens the proposal to use dinocyst δ13C values as a pCO2 proxy. Moreover, the similarity between the εf value for A. tamarense and the consensus value of ∼25‰ indicates that the CO2-sensitivity of carbon isotope fractionation saturates at similar CO2 levels across all three

Capture and geologic storage of carbon dioxide (CO2)

International Nuclear Information System (INIS)

2004-11-01

This dossier about carbon sequestration presents: 1 - the world fossil fuels demand and its environmental impact; 2 - the solutions to answer the climatic change threat: limitation of fossil fuels consumption, development of nuclear and renewable energies, capture and storage of CO 2 (environmental and industrial advantage, cost); 3 - the CO 2 capture: post-combustion smokes treatment, oxi-combustion techniques, pre-combustion techniques; 4 - CO 2 storage: in hydrocarbon deposits (Weyburn site in Canada), in deep saline aquifers (Sleipner and K12B (North Sea)), in non-exploitable coal seams (Recopol European project); 5 - international and national mobilization: IEA R and D program, USA (FutureGen zero-emission coal-fired power plant, Carbon Sequestration Leadership forum), European Union (AZEP, GRACE, GESTCO, CO2STORE, NASCENT, RECOPOL, Castor, ENCAP, CO2sink etc programs), French actions (CO 2 club, network of oil and gas technologies (RTPG)), environmental stake, competitiveness, research stake. (J.S.)

[Impacts of rice straw biochar on organic carbon and CO2 release in arable soil].

Science.gov (United States)

Ke, Yue-Jin; Hu, Xue-Yu; Yi, Qing; Yu, Zhong

2014-01-01

In order to investigate the stability of biochar and the effect of biochar when added into soil on soil organic carbon, a 130-day incubation experiment was conducted with rice straw biochar produced at 500 degrees C and 700 degrees C (RBC500 and RBC700) and with addition rates of 0% (control), 3%, 6% and 100% (pure biochar), to detect the change of total organic carbon (TOC), easily oxidized carbon (EOC) and status of CO2 release, following addition of biochar in arable soil. Results showed that: the content of both TOC and EOC in soil increased with biochar addition rates comparing with the control. RBC500 had greater contributions to both TOC and EOC increasing amounts than those of RBC700 under the same biochar addition rate. TOC contents of all treatments decreased during the initial 30 days with the largest decreasing amplitude of 15.8%, and tended to be stable in late incubation stages. Same to that of TOC, EOC contents of all treatments also tended to remain stable after 30 days, but in the 30 days of early incubation, EOC in the soil decreased by 72.4% and 81.7% respectively when the added amount of RBC500 was 3% and 6% , while it was reduced by 61.3% and 69.8% respectively when the added amount of RBC700 was 3% and 6%. EOC contents of soil added with biochar produced at the same temperature were similar in the end of incubation. The reduction of soil EOC content in early incubation may be related to mineralization caused by labile fractions of biochar. During the 130-day incubation, the accumulated CO2 releases showed an order of soil and biochar mixtures soil could reduce CO2 release, the largest reduction amplitude is 41.05%. In a long time scale, biochar as a soil amendment is favorable to the deduction of greenhouse gas release and soil carbon immobilization. Biochar could be used as a soil carbon sequestration carrier.

Development of novel CO{sub 2}-stable oxygen permeable dual phase membranes for CO{sub 2} capture in an oxy-fuel process

Energy Technology Data Exchange (ETDEWEB)

Luo, Huixia

2012-07-19

The combustion of fossil fuels in power stations with pure oxygen following the oxy-fuel process allows the Sequestration of CO{sub 2}. The pure oxygen needed can be separated from air by oxygen transporting ceramics like single phase perovskites. However, most of the so far developed single phase perovskites have stability problems in a CO{sub 2} containing atmosphere. Dual phase membranes are micro-scale mixtures of an electron conducting phase and an oxygen ion conducting phase and their compositions can be tailored according to practical requirements, which are considered to be promising substitutes for the single phase perovskite materials. In my thesis the issues of phase stability for perovskite-type material with the common composition Ba{sub 0.5}Sr{sub 0.5}Co{sub 0.8}Fe{sub 3-{delta}} (BSCF) as weil as the development of a series of novel CO{sub 2}-stable dual phase membranes were studied. In Chapter 2, the phase stability and permeation behavior of a dead-end BSCF tube membrane in high-purity oxygen at temperatures below 750 C, were elucidated using powder X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDXS), high-angle annular dark-field (HAADF) and scanning transmission electron microscopy (STEM). lt was found that parts of the cubic perovskite BSCF transformed into a hexagonal perovskite Ba{sub 0.5{+-}x}Sr{sub 0.5{+-}x}CoO{sub 3-{delta}} (x {approx} 0.1) and a trigonal mixed oxide Ba{sub 1-x}Sr{sub x}CO{sub 2-y}Fe{sub y}O{sub 5{+-}{delta}} (x {approx} 0.15, y {approx} 0.25) in high-purity oxygen at 750 C. On the other hand, it was found that the partial degradation of cubic BSCF perovskite at 750 C was more pronounced under the strongly oxidizing conditions on the oxygen supply (feed) side than on the oxygen release (permeate) side of the membrane. The structural instability of BSCF is attributed to an oxidation of cobalt from Co{sup 2+} to Co{sup 3+} and Co{sup 4+}, which exhibits an ionic radius that is too small to be tolerated by

A joint global carbon inversion system using both CO2 and 13CO2 atmospheric concentration data

Science.gov (United States)

Chen, Jing M.; Mo, Gang; Deng, Feng

2017-03-01

Observations of 13CO2 at 73 sites compiled in the GLOBALVIEW database are used for an additional constraint in a global atmospheric inversion of the surface CO2 flux using CO2 observations at 210 sites (62 collocated with 13CO2 sites) for the 2002-2004 period for 39 land regions and 11 ocean regions. This constraint is implemented using prior CO2 fluxes estimated with a terrestrial ecosystem model and an ocean model. These models simulate 13CO2 discrimination rates of terrestrial photosynthesis and ocean-atmosphere diffusion processes. In both models, the 13CO2 disequilibrium between fluxes to and from the atmosphere is considered due to the historical change in atmospheric 13CO2 concentration. This joint inversion system using both13CO2 and CO2 observations is effectively a double deconvolution system with consideration of the spatial variations of isotopic discrimination and disequilibrium. Compared to the CO2-only inversion, this 13CO2 constraint on the inversion considerably reduces the total land carbon sink from 3.40 ± 0.84 to 2.53 ± 0.93 Pg C year-1 but increases the total oceanic carbon sink from 1.48 ± 0.40 to 2.36 ± 0.49 Pg C year-1. This constraint also changes the spatial distribution of the carbon sink. The largest sink increase occurs in the Amazon, while the largest source increases are in southern Africa, and Asia, where CO2 data are sparse. Through a case study, in which the spatial distribution of the annual 13CO2 discrimination rate over land is ignored by treating it as a constant at the global average of -14. 1 ‰, the spatial distribution of the inverted CO2 flux over land was found to be significantly modified (up to 15 % for some regions). The uncertainties in our disequilibrium flux estimation are 8.0 and 12.7 Pg C year-1 ‰ for land and ocean, respectively. These uncertainties induced the unpredictability of 0.47 and 0.54 Pg C year-1 in the inverted CO2 fluxes for land and ocean, respectively. Our joint inversion system is therefore

Overview on CO{sub 2} Valorization: Challenge of Molten Carbonates

Energy Technology Data Exchange (ETDEWEB)

Chery, Déborah; Lair, Virginie; Cassir, Michel, E-mail: michel.cassir@chimie-paristech.fr [Chimie ParisTech, CNRS, Institut de Recherche de Chimie Paris, PSL Research University, Paris (France)

2015-10-02

The capture and utilization of CO{sub 2} is becoming progressively one of the significant challenges in the field of energetic resources. Whatever the energetic device, it is impossible to avoid completely the production of greenhouse gas, even parting from renewable energies. Transforming CO{sub 2} into a valuable fuel, such as alcohols, CO, or even C, could constitute a conceptual revolution in the energetic bouquet offering a huge application domain. Although several routes have been tested for this purpose, on which a general panorama will be given here, molten carbonates are attracting a renewed interest aiming at dissolving and reducing carbon dioxide in such melts. Because of their unique properties, molten carbonates are already used as electrolytes in molten carbonate fuel cells; they can also provoke a breakthrough in a new economy considering CO{sub 2} as an energetic source rather than a waste. Molten carbonates’ science and technology is becoming a strategic field of research for energy and environmental issues. Our aim in this review is to put in evidence the benefits of molten carbonates to valorize CO{sub 2} and to show that it is one of the most interesting routes for such application.

Exceptionally High Efficient Co-Co2P@N, P-Codoped Carbon Hybrid Catalyst for Visible Light-Driven CO2-to-CO Conversion.

Science.gov (United States)

Fu, Wen Gan

2018-05-02

Artificial photosynthesis has attracted wide attention, particularly the development of efficient solar light-driven methods to reduce CO2 to form energy-rich carbon-based products. Because CO2 reduction is an uphill process with a large energy barrier, suitable catalysts are necessary to achieve this transformation. In addition, CO2 adsorption on a catalyst and proton transfer to CO2 are two important factors for the conversion reaction，and catalysts with high surface area and more active sites are required to improve the efficiency of CO2 reduction. Here, we report a visible light-driven system for CO2-to-CO conversion that consists of a heterogeneous hybrid catalyst of Co and Co2P nanoparticles embedded in carbon nanolayers codoped with N and P (Co-Co2P@NPC) and a homogeneous Ru(II)-based complex photosensitizer. The average generation rate of CO of the system was up to 35,000 μmol h-1 g-1 with selectivity of 79.1% in 3 h. Linear CO production at an exceptionally high rate of 63,000 μmol h-1 g-1 was observed in the first hour of reaction. Inspired by this highly active catalyst, we also synthesized Co@NC and Co2P@NPC materials and explored their structure, morphology, and catalytic properties for CO2 photoreduction. The results showed that the nanoparticle size, partially adsorbed H2O molecules on the catalyst surface, and the hybrid nature of the systems influenced their photocatalytic CO2 reduction performance. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Carbon dioxide sequestration by mineral carbonation. Feasibility of enhanced natural weathering as a CO2 emission reduction technology

International Nuclear Information System (INIS)

Huijgen, W.J.J.

2007-01-01

A possible technology that can contribute to the reduction of carbon dioxide emissions is CO2 sequestration by mineral carbonation. The basic concept behind mineral CO2 sequestration is the mimicking of natural weathering processes in which calcium or magnesium containing minerals react with gaseous CO2 and form solid calcium or magnesium carbonates. Potential advantages of mineral CO2 sequestration compared to, e.g., geological CO2 storage include (1) the permanent and inherently safe sequestration of CO2, due to the thermodynamic stability of the carbonate product formed and (2) the vast potential sequestration capacity, because of the widespread and abundant occurrence of suitable feedstock. In addition, carbonation is an exothermic process, which potentially limits the overall energy consumption and costs of CO2 emission reduction. However, weathering processes are slow, with timescales at natural conditions of thousands to millions of years. For industrial implementation, a reduction of the reaction time to the order of minutes has to be achieved by developing alternative process routes. The aim of this thesis is an investigation of the technical, energetic, and economic feasibility of CO2 sequestration by mineral carbonation. In Chapter 1 the literature published on CO2 sequestration by mineral carbonation is reviewed. Among the potentially suitable mineral feedstock for mineral CO2 sequestration, Ca-silicates, more particularly wollastonite (CaSiO3), a mineral ore, and steel slag, an industrial alkaline solid residue, are selected for further research. Alkaline Ca-rich residues seem particularly promising, since these materials are inexpensive and available near large industrial point sources of CO2. In addition, residues tend to react relatively rapidly with CO2 due to their (geo)chemical instability. Various process routes have been proposed for mineral carbonation, which often include a pre-treatment of the solid feedstock (e.g., size reduction and

Interactive Effects of CO2 Concentration and Water Regime on Stable Isotope Signatures, Nitrogen Assimilation and Growth in Sweet Pepper

Directory of Open Access Journals (Sweden)

María D. Serret

2018-01-01

Full Text Available Sweet pepper is among the most widely cultivated horticultural crops in the Mediterranean basin, being frequently grown hydroponically under cover in combination with CO2 fertilization and water conditions ranging from optimal to suboptimal. The aim of this study is to develop a simple model, based on the analysis of plant stable isotopes in their natural abundance, gas exchange traits and N concentration, to assess sweet pepper growth. Plants were grown in a growth chamber for near 6 weeks. Two [CO2] (400 and 800 μmol mol−1, three water regimes (control and mild and moderate water stress and four genotypes were assayed. For each combination of genotype, [CO2] and water regime five plants were evaluated. Water stress applied caused significant decreases in water potential, net assimilation, stomatal conductance, intercellular to atmospheric [CO2], and significant increases in water use efficiency, leaf chlorophyll content and carbon isotope composition, while the relative water content, the osmotic potential and the content of anthocyanins did change not under stress compared to control conditions support this statement. Nevertheless, water regime affects plant growth via nitrogen assimilation, which is associated with the transpiration stream, particularly at high [CO2], while the lower N concentration caused by rising [CO2] is not associated with stomatal closure. The stable isotope composition of carbon, oxygen, and nitrogen (δ13C, δ18O, and δ15N in plant matter are affected not only by water regime but also by rising [CO2]. Thus, δ18O increased probably as response to decreases in transpiration, while the increase in δ15N may reflect not only a lower stomatal conductance but a higher nitrogen demand in leaves or shifts in nitrogen metabolism associated with decreases in photorespiration. The way that δ13C explains differences in plant growth across water regimes within a given [CO2], seems to be mediated through its direct

Determination of the origin of dissolved inorganic carbon in groundwater around a reclaimed landfill in Otwock using stable carbon isotopes.

Science.gov (United States)

Porowska, Dorota

2015-05-01

Chemical and isotopic analyses of groundwater from piezometers located around a reclaimed landfill in Otwock (Poland) were performed in order to trace the origin of dissolved inorganic carbon (DIC) in the groundwater. Due to differences in the isotopic composition of carbon from different sources, an analysis of stable carbon isotopes in the groundwater, together with the Keeling plot approach and a two-component mixing model allow us to evaluate the relative contributions of carbon from these sources in the groundwater. In the natural (background) groundwater, DIC concentrations and the isotopic composition of DIC (δ(13)CDIC) comes from two sources: decomposition of organic matter and carbonate dissolution within the aquifer sediments, whereas in the leachate-contaminated groundwater, DIC concentrations and δ(13)CDIC values depend on the degradation of organic matter within the aquifer sediments and biodegradation of organic matter stored in the landfill. From the mixing model, about 4-54% of the DIC pool is derived from organic matter degradation and 96-46% from carbonate dissolution in natural conditions. In the leachate-contaminated groundwater, about 20-53% of the DIC is derived from organic matter degradation of natural origin and 80-47% from biodegradation of organic matter stored in the landfill. Partial pressure of CO2 (P CO2) was generally above the atmospheric, hence atmospheric CO2 as a source of carbon in DIC pool was negligible in the aquifer. P CO2 values in the aquifer in Otwock were always one to two orders of magnitude above the atmospheric P CO2, and thus CO2 escaped directly into the vadose zone. Copyright © 2015 Elsevier Ltd. All rights reserved.

Weeks Island gravity stable CO2 pilot: Final report

Energy Technology Data Exchange (ETDEWEB)

Johnston, J.R.; Perry, G.E.

1989-01-01

The Weeks Island ''S'' sand Reservoir B (''S'' RB) gravity-stable CO2 field test was completed during February 1988. Injection started in October 1978 and production began in January 1981 in this high-permeability, steeply-dipping sandstone reservoir. About 264,000 barrels of oil or 65 percent of the starting volume has been recovered. A 24-percent pore-volume slug of CO2 mixed with about six mole percent of natural gas (mostly methane) was injected at the start of the pilot. Since 1983, produced CO2 plus hydrocarbon gases have been recycled. CO2 usage statistics are 9.34 MCF/BO with recycle and 3.24 MCF/BO based on purchased CO2. Previous annual reports document the pilot design, implementation, and early results for the 1977 to June 1981 time period. This report is a review of early pilot history and a more detailed account of the post June 1981 results and overall interpretation. A reservoir-simulation history match of pilot performance plus core and log data from a 1983 swept-zone evaluation well are described in this report. A brief description of the production facility and an account of the corrosion control program are also included. 11 refs., 34 figs.

CO{sub 2} capture by adsorption with nitrogen enriched carbons

Energy Technology Data Exchange (ETDEWEB)

M.G. Plaza; C. Pevida; A. Arenillas; F. Rubiera; J.J. Pis [Instituto Nacional del Carbon (CSIC), Oviedo (Spain)

2007-09-15

The success of CO{sub 2} capture with solid sorbents is dependent on the development of a low cost sorbent with high CO{sub 2} selectivity and adsorption capacity. Immobilised amines are expected to offer the benefits of liquid amines in the typical absorption process, with the added advantages that solids are easy to handle and that they do not give rise to corrosion problems. In this work, different alkylamines were evaluated as a potential source of basic sites for CO{sub 2} capture, and a commercial activated carbon was used as a preliminary support in order to study the effect of the impregnation. The amine coating increased the basicity and nitrogen content of the carbon. However, it drastically reduced the microporous volume of the activated carbon, which is chiefly responsible for CO{sub 2} physisorption, thus decreasing the capacity of raw carbon at room temperature. 33 refs., 7 figs., 3 tabs.

Activation of magnesium rich minerals as carbonation feedstock materials for CO2 sequestration

International Nuclear Information System (INIS)

Maroto-Valer, M.M.; Kuchta, M.E.; Zhang, Y.; Andresen, J.M.; Fauth, D.J.

2005-01-01

Mineral carbonation, the reaction of magnesium-rich minerals such as olivine and serpentine with CO 2 to form stable mineral carbonates, is a novel and promising approach to carbon sequestration. However, the preparation of the minerals prior to carbonation can be energy intensive, where some current studies have been exploring extensive pulverization of the minerals below 37 μm, heat treatment of minerals up to 650 o C, prior separation of CO 2 from flue gases, and carbonation at high pressures, temperatures and long reaction times of up to 125 atm, 185 o C and 6 h, respectively. Thus, the objective of the mineral activation concept is to promote and accelerate carbonation reaction rates and efficiencies through surface activation to the extent that such rigorous reaction conditions were not required. The physical activations were performed with air and steam, while chemical activations were performed with a suite of acids and bases. The parent serpentine, activated serpentines, and carbonation products were characterized to determine their surface properties and assess their potential as carbonation minerals. The results indicate that the surface area of the raw serpentine, which is approximately 8 m 2 /g, can be increased through physical and chemical activation methods to over 330 m 2 /g. The chemical activations were more effective than the physical activations at increasing the surface area, with the 650 o C steam activated serpentine presenting a surface area of only 17 m 2 /g. Sulfuric acid was the most effective acid used during the chemical activations, resulting in surface areas greater than 330 m 2 /g. Several of the samples produced underwent varying degrees of carbonation. The steam activated serpentine underwent a 60% conversion to magnesite at 155 o C and 126 atm in 1 h, while the parent sample only exhibited a 7% conversion. The most promising results came from the carbonation of the extracted Mg(OH) 2 solution, where, based on the amount of

Impact of elevated CO_2 concentrations on carbonate mineral precipitation ability of sulfate-reducing bacteria and implications for CO_2 sequestration

International Nuclear Information System (INIS)

Paul, Varun G.; Wronkiewicz, David J.; Mormile, Melanie R.

2017-01-01

Interest in anthropogenic CO_2 release and associated global climatic change has prompted numerous laboratory-scale and commercial efforts focused on capturing, sequestering or utilizing CO_2 in the subsurface. Known carbonate mineral precipitating microorganisms, such as the anaerobic sulfate-reducing bacteria (SRB), could enhance the rate of conversion of CO_2 into solid minerals and thereby improve long-term storage of captured gasses. The ability of SRB to induce carbonate mineral precipitation, when exposed to atmospheric and elevated pCO_2, was investigated in laboratory scale tests with bacteria from organic-rich sediments collected from hypersaline Lake Estancia, New Mexico. The enriched SRB culture was inoculated in continuous gas flow and batch reactors under variable headspace pCO_2 (0.0059 psi to 20 psi). Solution pH, redox conditions, sulfide, calcium and magnesium concentrations were monitored in the reactors. Those reactors containing SRB that were exposed to pCO_2 of 14.7 psi or less showed Mg-calcite precipitation. Reactors exposed to 20 psi pCO_2 did not exhibit any carbonate mineralization, likely due to the inhibition of bacterial metabolism caused by the high levels of CO_2. Hydrogen, lactate and formate served as suitable electron donors for the SRB metabolism and related carbonate mineralization. Carbon isotopic studies confirmed that ∼53% of carbon in the precipitated carbonate minerals was derived from the CO_2 headspace, with the remaining carbon being derived from the organic electron donors, and the bicarbonate ions available in the liquid medium. The ability of halotolerant SRB to induce the precipitation of carbonate minerals can potentially be applied to the long-term storage of anthropogenic CO_2 in saline aquifers and other ideal subsurface rock units by converting the gas into solid immobile phases. - Highlights: • SRB under study are capable of precipitating calcite up to 14.7 psi pCO_2. • At 20 psi pCO_2, bacterial activity

State of the Carbon Cycle - Consequences of Rising Atmospheric CO2

Science.gov (United States)

Moore, D. J.; Cooley, S. R.; Alin, S. R.; Brown, M. E.; Butman, D. E.; French, N. H. F.; Johnson, Z. I.; Keppel-Aleks, G.; Lohrenz, S. E.; Ocko, I.; Shadwick, E. H.; Sutton, A. J.; Potter, C. S.; Yu, R. M. S.

2016-12-01

The rise of atmospheric CO2, largely attributable to human activity through fossil fuel emissions and land-use change, has been dampened by carbon uptake by the ocean and terrestrial biosphere. We outline the consequences of this carbon uptake as direct and indirect effects on terrestrial and oceanic systems and processes for different regions of North America and the globe. We assess the capacity of these systems to continue to act as carbon sinks. Rising CO2 has decreased seawater pH; this process of ocean acidification has impacted some marine species and altered fundamental ecosystem processes with further effects likely. In terrestrial ecosystems, increased atmospheric CO2 causes enhanced photosynthesis, net primary production, and increased water-use efficiency. Rising CO2 may change vegetation composition and carbon storage, and widespread increases in water use efficiency likely influence terrestrial hydrology and biogeochemical cycling. Consequences for human populations include changes to ecosystem services including cultural activities surrounding land use, agricultural or harvesting practices. Commercial fish stocks have been impacted and crop production yields have been changed as a result of rising CO2. Ocean and terrestrial effects are contingent on, and feedback to, global climate change. Warming and modified precipitation regimes impact a variety of ecosystem processes, and the combination of climate change and rising CO2 contributes considerable uncertainty to forecasting carbon sink capacity in the ocean and on land. Disturbance regime (fire and insects) are modified with increased temperatures. Fire frequency and intensity increase, and insect lifecycles are disrupted as temperatures move out of historical norms. Changes in disturbance patterns modulate the effects of rising CO2 depending on ecosystem type, disturbance frequency, and magnitude of events. We discuss management strategies designed to limit the rise of atmospheric CO2 and reduce

State of the Carbon Cycle - Consequences of Rising Atmospheric CO2

Science.gov (United States)

Moore, David J.; Cooley, Sarah R.; Alin, Simone R.; Brown, Molly; Butman, David E.; French, Nancy H. F.; Johnson, Zackary I.; Keppel-Aleks; Lohrenz, Steven E.; Ocko, Ilissa;

BASIN TCP Stable Isotope Composition of CO2 in Terrestrial Ecosystems

Data.gov (United States)

National Aeronautics and Space Administration — ABSTRACT: This data set reports stable isotope ratio data of CO2 (13C/12C and 18O/16O) associated with photosynthetic and respiratory exchanges across the...

Micro-CT in situ study of carbonate rock microstructural evolution for geologic CO2 storage

DEFF Research Database (Denmark)

Zheng, Yi; Yang, Yan; Rogowska, M.

2017-01-01

to achieve this is to find a suitable condition to create a stable 3D space in carbonate rock by injecting liquid to prepare space for the later CO2 injection. Micro-CT imaging is a non-destructive 3D method that can be used to study the property changes of carbonate rocks during and after CO2 injection....... The advance in lab source based micro-CT has made it capable of in situ experiments. We used a commercial bench top micro-CT (Zeiss Versa XRM410) to study the microstructure changes of chalk during liquid injection. Flexible temporal CT resolution is essential in this study because that the time scales...... of coupled physical and chemical processes can be very different. The results validated the feasibility of using a bench top CT system with a pressure cell to monitor the mesoscale multiphase interactions in chalk....

BASIN TCP Stable Isotope Composition of CO2 in Terrestrial Ecosystems

Data.gov (United States)

National Aeronautics and Space Administration — This data set reports stable isotope ratio data of CO2 (13C/12C and 18O/16O) associated with photosynthetic and respiratory exchanges across the biosphere-atmosphere...

Tailings and mineral carbonation : the potential for atmospheric CO{sub 2} sequestration

Energy Technology Data Exchange (ETDEWEB)

Rollo, H.A. [Lorax Environmental Services Ltd., Vancouver, BC (Canada); Jamieson, H.E. [Queen' s Univ., Kingston, ON (Canada). Dept. of Geological Sciences and Geological Engineering; Lee, C.A. [Dillon Consulting Ltd., Cambridge, ON (Canada)

2009-02-15

Carbon dioxide (CO{sub 2}) sequestration includes geological storage, ocean storage, organic storage, and mineral storage (mineral carbonation). This presentation discussed tailings and mineral carbonation and the potential for atmospheric CO{sub 2} sequestration. In particular, it outlined CO{sub 2} sequestration and presented a history of investigations. The Ekati Diamond Mine was discussed with particular reference to its location, geology, and processing. Other topics that were presented included mineralogy; water chemistry; modeling results; and estimates of annual CO{sub 2} sequestration. Conclusions and implications were also presented. It was concluded that ore processing at mines with ultramafic host rocks have the potential to partially offset CO{sub 2} emissions. In addition, it was found that existing tailings at ultramafic deposits may be viable source materials for CO{sub 2} sequestration by mineral carbonation. tabs., figs.

Rates of CO2 Mineralization in Geological Carbon Storage.

Science.gov (United States)

Zhang, Shuo; DePaolo, Donald J

2017-09-19

Geologic carbon storage (GCS) involves capture and purification of CO 2 at industrial emission sources, compression into a supercritical state, and subsequent injection into geologic formations. This process reverses the flow of carbon to the atmosphere with the intention of returning the carbon to long-term geologic storage. Models suggest that most of the injected CO 2 will be "trapped" in the subsurface by physical means, but the most risk-free and permanent form of carbon storage is as carbonate minerals (Ca,Mg,Fe)CO 3 . The transformation of CO 2 to carbonate minerals requires supply of the necessary divalent cations by dissolution of silicate minerals. Available data suggest that rates of transformation are highly uncertain and difficult to predict by standard approaches. Here we show that the chemical kinetic observations and experimental results, when they can be reduced to a single cation-release time scale that describes the fractional rate at which cations are released to solution by mineral dissolution, show sufficiently systematic behavior as a function of pH, fluid flow rate, and time that the rates of mineralization can be estimated with reasonable certainty. The rate of mineralization depends on both the abundance (determined by the reservoir rock mineralogy) and the rate at which cations are released from silicate minerals by dissolution into pore fluid that has been acidified with dissolved CO 2 . Laboratory-measured rates and field observations give values spanning 8 to 10 orders of magnitude, but when they are evaluated in the context of a reservoir-scale reactive transport simulation, this range becomes much smaller. The reservoir scale simulations provide limits on the applicable conditions under which silicate mineral dissolution and subsequent carbonate mineral precipitation are likely to occur (pH 4.5 to 6, fluid flow velocity less than 5 m/year, and 50-100 years or more after the start of injection). These constraints lead to estimates of

Comparison of CO(2) and bicarbonate as inorganic carbon sources for triacylglycerol and starch accumulation in Chlamydomonas reinhardtii.

Science.gov (United States)

Gardner, Robert D; Lohman, Egan; Gerlach, Robin; Cooksey, Keith E; Peyton, Brent M

2013-01-01

Microalgae are capable of accumulating high levels of lipids and starch as carbon storage compounds. Investigation into the metabolic activities involved in the synthesis of these compounds has escalated since these compounds can be used as precursors for food and fuel. Here, we detail the results of a comprehensive analysis of Chlamydomonas reinhardtii using high or low inorganic carbon concentrations and speciation between carbon dioxide and bicarbonate, and the effects these have on inducing lipid and starch accumulation during nitrogen depletion. High concentrations of CO(2) (5%; v/v) produced the highest amount of biofuel precursors, transesterified to fatty acid methyl esters, but exhibited rapid accumulation and degradation characteristics. Low CO(2) (0.04%; v/v) caused carbon limitation and minimized triacylglycerol (TAG) and starch accumulation. High bicarbonate caused a cessation of cell cycling and accumulation of both TAG and starch that was more stable than the other experimental conditions. Starch accumulated prior to TAG and then degraded as maximum TAG was reached. This suggests carbon reallocation from starch-based to TAG-based carbon storage. Copyright © 2012 Wiley Periodicals, Inc.

CuZn Alloy- Based Electrocatalyst for CO2 Reduction

KAUST Repository

Alazmi, Amira

2014-06-01

ABSTRACT CuZn Alloy- Based Electrocatalyst for CO2 Reduction Amira Alazmi Carbon dioxide (CO2) is one of the major greenhouse gases and its emission is a significant threat to global economy and sustainability. Efficient CO2 conversion leads to utilization of CO2 as a carbon feedstock, but activating the most stable carbon-based molecule, CO2, is a challenging task. Electrochemical conversion of CO2 is considered to be the beneficial approach to generate carbon-containing fuels directly from CO2, especially when the electronic energy is derived from renewable energies, such as solar, wind, geo-thermal and tidal. To achieve this goal, the development of an efficient electrocatalyst for CO2 reduction is essential. In this thesis, studies on CuZn alloys with heat treatments at different temperatures have been evaluated as electrocatalysts for CO2 reduction. It was found that the catalytic activity of these electrodes was strongly dependent on the thermal oxidation temperature before their use for electrochemical measurements. The polycrystalline CuZn electrode without thermal treatment shows the Faradaic efficiency for CO formation of only 30% at applied potential ~−1.0 V vs. RHE with current density of ~−2.55 mA cm−2. In contrast, the reduction of oxide-based CuZn alloy electrode exhibits 65% Faradaic efficiency for CO at lower applied potential about −1.0 V vs. RHE with current density of −2.55 mA cm−2. Furthermore, stable activity was achieved over several hours of the reduction reaction at the modified electrodes. Based on electrokinetic studies, this improvement could be attributed to further stabilization of the CO2•− on the oxide-based Cu-Zn alloy surface.

Barium isotope fractionation during experimental formation of the double carbonate BaMn[CO3](2) at ambient temperature.

Science.gov (United States)

Böttcher, Michael E; Geprägs, Patrizia; Neubert, Nadja; von Allmen, Katja; Pretet, Chloé; Samankassou, Elias; Nägler, Thomas F

2012-09-01

In this study, we present the first experimental results for stable barium (Ba) isotope ((137)Ba/(134)Ba) fractionation during low-temperature formation of the anhydrous double carbonate BaMn[CO(3)](2). This investigation is part of an ongoing work on Ba fractionation in the natural barium cycle. Precipitation at a temperature of 21±1°C leads to an enrichment of the lighter Ba isotope described by an enrichment factor of-0.11±0.06‰ in the double carbonate than in an aqueous barium-manganese(II) chloride/sodium bicarbonate solution, which is within the range of previous reports for synthetic pure BaCO (3) (witherite) formation.

History of CO/sub 2/

Energy Technology Data Exchange (ETDEWEB)

Degens, E T

1979-01-01

Upon arrival on earth, the reduced carbon pool split into a series of compartments: core, mantle, crust, hydrosphere, atmosphere, and biosphere. This distribution pattern is caused by the ability of carbon to adjust structurally to a wide range of pressure and temperature, and to form simple and complex molecules with oxygen, hydrogen and nitrogen. Transformation also involved oxidation of carbon to CO/sub 2/ which is mediated at depth by minerals, such as magnetite, and by water vapor above critical temperature. Guided by mineral-organic interactions, simple carbon compounds evolved in near surface environments towards physiologically interesting biochemicals. Life, as an autocatalytic system, is considered an outgrowth of such a development. This article discusses environmental parameters that control the CO/sub 2/ system, past and present. Mantle and crustal evolution is the dynamo recharging the CO/sub 2/ in sea and air; the present rate of CO/sub 2/ release from the magma is 0.05 x 10/sup 15/ g C per year. Due to the enormous buffer capacity of the chemical system ocean, such rates are too small to seriously effect the level of CO/sub 2/ in our atmosphere. In the light of geological field data and stable isotope work, it is concluded that the CO/sub 2/ content in the atmosphere has remained fairly uniform since early Precambrian time; CO/sub 2/ should thus have had little impact on paleoclimate. In contrast, the massive discharge of man-made CO/sub 2/ into our atmosphere may have serious consequences for climate, environment and society in the years to come.

In situ measurement of magnesium carbonate formation from CO2 using static high-pressure and -temperature 13C NMR.

Science.gov (United States)

Surface, J Andrew; Skemer, Philip; Hayes, Sophia E; Conradi, Mark S

2013-01-02

We explore a new in situ NMR spectroscopy method that possesses the ability to monitor the chemical evolution of supercritical CO(2) in relevant conditions for geological CO(2) sequestration. As a model, we use the fast reaction of the mineral brucite, Mg(OH)(2), with supercritical CO(2) (88 bar) in aqueous conditions at 80 °C. The in situ conversion of CO(2) into metastable and stable carbonates is observed throughout the reaction. After more than 58 h of reaction, the sample was depressurized and analyzed using in situ Raman spectroscopy, where the laser was focused on the undisturbed products through the glass reaction tube. Postreaction, ex situ analysis was performed on the extracted and dried products using Raman spectroscopy, powder X-ray diffraction, and magic-angle spinning (1)H-decoupled (13)C NMR. These separate methods of analysis confirmed a spatial dependence of products, possibly caused by a gradient of reactant availability, pH, and/or a reaction mechanism that involves first forming hydroxy-hydrated (basic, hydrated) carbonates that convert to the end-product, anhydrous magnesite. This carbonation reaction illustrates the importance of static (unmixed) reaction systems at sequestration-like conditions.

On the limits of CO2 capture capacity of carbons

OpenAIRE

Fernández Martín, Claudia; González Plaza, Marta; Pis Martínez, José Juan; Rubiera González, Fernando; Pevida García, Covadonga; Álvarez Centeno, Teresa

2010-01-01

This study shows that standard techniques used for carbons characterization, such as physical adsorption of CO2 at 273 K and N2 at 77 K, can be used to assess, with a good accuracy, the maximum capacity of carbons to capture CO2 under post- and pre-combustion conditions. The analysis of the corresponding adsorption isotherms, within the general theoretical framework of Dubinin's theory, leads to the values of the micropore volume, Wo, and the characteristic energy, Eo, of the carbons, which p...

Developments and innovation in carbon dioxide (CO{sub 2}) capture and storage technology. Volume 2: Carbon dioxide (CO{sub 2}) storage and utilisation

Energy Technology Data Exchange (ETDEWEB)

Mercedes Maroto-Valer, M. (ed.)

2010-07-01

This volume initially reviews geological sequestration of CO{sub 2}, from saline aquifer sequestration to oil and gas reservoir and coal bed storage, including coverage of reservoir sealing, and monitoring and modelling techniques used to verify geological sequestration of CO{sub 2}. Terrestrial and ocean sequestration are also reviewed, along with the environmental impact and performance assessments for these routes. The final section reviews advanced concepts for CO{sub 2} storage and utilization, such as industrial utilization, biofixation, mineral carbonation and photocatalytic reduction.

Morphology, molecular structure, and stable carbon isotopic composition of black carbon (BC) in urban topsoils.

Science.gov (United States)

Zong, Yutong; Xiao, Qing; Lu, Shenggao

2018-02-01

Urban soils contain significant amounts of black carbon (BC) from biomass and fossil fuel combustion and regard to be a pool of BC. BC in urban soils has multiple effects on environmental processes in urban system, such as global climate change, air quality, and public health. Urban topsoil samples (0-10 cm) were collected from Anshan, Liaoning Province, northeast China, which is one of the most important old steel industrial bases in China. The BC in urban topsoils was extracted using the density method. Their chemical composition, morphology, molecular structure, and stable carbon isotopic composition were examined using elemental analysis, scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM-EDS), Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), X-ray diffraction (XRD), and stable carbon isotope (δ 13 C). Elemental analysis shows that carbon content in the BC of studied soils ranged from 64.5 to 78.4%, with the average more than 70%. The O/C atomic ratio of BC is on average 0.18. The BC particle displays different morphology, including porous spherical, irregular porous fragmentary, and blocky shapes. The porous spherical BC particles has atomic molar O/C ratio determined by SEM-EDS ranging from 0.04 to 0.37. XRD indicates that BC exists in mainly combining with mineral phases hematite (Fe 2 O 3 ), kaolinite (Al 2 Si 2 O 5 (OH) 4 ), quartz (SiO 2 ), and calcite (CaCO 3 ). The FTIR spectra of BC particles show major bands at approximately 3400 cm -1 (O-H), 2920 cm -1 (C = H), 1600 cm -1 (C = C), 1230 cm -1 (C = O), and 1070 cm -1 (C = O). The stable carbon isotope (δ 13 C) of BC ranges from -24.48 to -23.18‰ with the average of -23.79 ± 0.39‰. The concentration of BC in the industrial area is significantly (p fuel combustion. Results indicated that a combination of atomic O/C ratio, porous structure, and stable carbon isotopic (δ 13 C) of BC could reflect effectively the origin of BC

Porous carbon derived via KOH activation of a hypercrosslinked porous organic polymer for efficient CO_2, CH_4, H_2 adsorptions and high CO_2/N_2 selectivity

International Nuclear Information System (INIS)

Modak, Arindam; Bhaumik, Asim

2015-01-01

Microporous carbon having Brunauer-Emmett-Teller (BET) surface area of 2186 m"2 g"−"1 and micropore volume of 0.85 cm"3 g"−"1 has been synthesized via KOH induced high temperature carbonization of a non-conjugated hypercrosslinked organic polymer. Owing to the templating and activation by KOH, we have succeeded in making a microporous carbon from this porous polymer and the resultant carbon material showed high uptake for CO_2 (7.6 mmol g"−"1) and CH_4 (2.4 mmol g"−"1) at 1 atm, 273 K together with very good selectivity for the CO_2/N_2 (30.2) separation. Furthermore, low pressure (1 atm) H_2 (2.6 wt%, 77 K) and water uptake (57.4 wt%, 298 K) ability of this polymer derived porous activated carbon is noteworthy. - Graphical abstract: Microporous carbon with BET surface area of 2186 m"2 g"−"1 has been synthesized via KOH activation of a porous organic polymer and it showed high uptake for CO_2 (7.6 mmol g"−"1), CH_4 (2.4 mmol g"−"1) and H_2 (2.6 wt%) at 1 atm together with very good selectivity for CO_2. - Highlights: • Porous carbon from hypercrosslinked organic polymer. • KOH activated carbon with BET surface area 2186 m"2 g"−"1. • High CO2 uptake (7.6 mmol g"−"1) and CO_2/N_2 selectivity (30.2). • Porous carbon also showed high H_2 (2.6 wt%) and H_2O (57.4 wt%) uptakes.

Fractional CO2 lasers contribute to the treatment of stable non-segmental vitiligo.

Science.gov (United States)

Yuan, Jinping; Chen, Hongqiang; Yan, Ru; Cui, Shaoshan; Li, Yuan-Hong; Wu, Yan; Gao, Xing-Hua; Chen, Hong-Duo

2016-12-01

Stable non-segmental vitiligo is often resistant to conventional therapies. The purpose of this study was to investigate the effect of three types of fractional lasers in the treatment of stable non-segmental vitiligo. Twenty patients were enrolled in the study. The vitiligo lesions of each patient were divided into four treatment parts, and all parts were treated with narrowband ultraviolet-B (NB-UVB). Three of the four parts were respectively treated with three types of fractional lasers (two ablative 10,600-nm CO 2 lasers and one non-ablative 1,565-nm laser), followed by topical betamethasone solution application. The treatment period lasted six months. Efficacy and satisfaction were respectively assessed by dermatologists and patients. The ablative CO 2 lasers, in combination with topical betamethasone solution and NB-UVB, achieved marked to excellent improvement on white patches assessed by dermatologists. Patients showed high satisfaction scores for the treatments. The non-ablative 1,565-nm fractional laser did not provide any further benefit in the treatment of vitiligo. No severe adverse events developed for any of the treatments. The treatment protocol with ablative CO 2 lasers, in combination with topical betamethasone solution and NB-UVB, was suitable for stable non-segmental vitiligo. For vitiligo, the ablative fractional CO 2 laser is more effective than the non-ablative fractional laser.

Energy consumption and net CO2 sequestration of aqueous mineral carbonation

International Nuclear Information System (INIS)

Huijgen, W.J.J.; Ruijg, G.J.; Comans, R.N.J.; Witkamp, G.J.

2006-12-01

Aqueous mineral carbonation is a potentially attractive sequestration technology to reduce CO2 emissions. The energy consumption of this technology, however, reduces the net amount of CO2 sequestered. Therefore, the energetic CO2 sequestration efficiency of aqueous mineral carbonation was studied in dependence of various process variables using either wollastonite (CaSiO3) or steel slag as feedstock. For wollastonite, the maximum energetic CO2 sequestration efficiency within the ranges of process conditions studied was 75% at 200C, 20 bar CO2, and a particle size of <38μm. The main energy-consuming process steps were the grinding of the feedstock and the compression of the CO2 feed. At these process conditions, a significantly lower efficiency was determined for steel slag (69%), mainly because of the lower Ca content of the feedstock. The CO2 sequestration efficiency might be improved substantially for both types of feedstock by, e.g., reducing the amount of process water applied and further grinding of the feedstock. The calculated energetic efficiencies warrant a further assessment of the (energetic) feasibility of CO2 sequestration by aqueous mineral carbonation on the basis of a pilot-scale process

Hierarchical flower-like carbon nanosheet assembly with embedded hollow NiCo{sub 2}O{sub 4} nanoparticles for high- performance lithium ion batteries

Energy Technology Data Exchange (ETDEWEB)

Fang, Ling; Qiu, Huajun; Luo, Pan; Li, Wenxiang; Zhang, Huijuan; Wang, Yu, E-mail: wangy@cqu.edu.cn

2017-05-01

Highlights: • Flower-like NiCo{sub 2}O{sub 4}@carbon nanosphere is firstly synthesized for Li-ion batteries. • The nanostructure exhibits the unique feature of hollow NiCo{sub 2}O{sub 4} nanoparticles embedded inside and graphitized carbon layers coating outside. • The sample reveals stable structure, large specific surface area and good electrical conductivity. • The composite exhibits superior rate capability, cycling capacity and excellent Coulombic efficiency. - Abstract: The fabrication of closely bounded metal oxides/carbon hybrid nano-structures is significant for its use in energy-related areas especially lithium ion batteries (LIBs). In this research, a flower-like carbon sphere with hollow NiCo{sub 2}O{sub 4} nanoparticles encapsulated inside the carbon thin nanopetal is fabricated by using a mixed basic carbonate nickel and cobalt sphere as the precursor and templates followed by the outer carbon membrane covering and two-step calcination process. When tested as anode material for LIBs, this flower-like carbon-based hybrid sphere demonstrates a significantly enhanced reversible capacity and cycling stability at various current densities.

Validation of 13CO2 breath analysis as a measurement of demethylation of stable isotope labeled aminopyrine in man

International Nuclear Information System (INIS)

Schneider, J.F.; Schoeller, D.A.; Nemchausky, B.; Bayer, J.L.; Klein, P.

1978-01-01

Interval sampling of expired breath as a simple, non-invasive assessment of the effect of liver disease upon hepatic microsomal drug metabolism, has been demonstrated with [ 14 C] dimethylaminoantipyrine (aminopyrine). In order to eliminate radiation risk the authors have validated the use of aminopyrine labeled with the stable, non-radioactive isotope 13 C. Simultaneous oral administration of both [ 14 C]- and [ 13 C] aminopyrine to five adult subjects without liver disease as well as five patients with known liver disease, resulted in the excretion of label at nearly identical rates in both individual time collections (r=0.94) as well as cumulative excretion for three hours (r=0.97). An oral dose of 2-mg/kg of [ 13 C) aminopyrine resulted in rates of production of 13 CO 2 significantly greater than baseline variations in 13 CO 2 production in the fasting, resting subject. Measurements of a single peak value at one half hour correlated closely with the determination of cumulative appearance over three hours (r=0.96). A consistent reproducible increase in the peak production of 13 CO 2 was observed when five patients received phenobarbital. Stable isotope labeled aminopyrine may be used to detect the effects of disease and treatment upon hepatic N-demethylation activity in human subjects without incurring any risk from radiation. Furthermore, the availability of another isotopic carbon label should make possible the study of direct drug-drug interaction utilizing CO 2 analysis. (Auth.)

Phenol-Formaldehyde Resin-Based Carbons for CO2 Separation at Sub-Atmospheric Pressures

Directory of Open Access Journals (Sweden)

Noelia Álvarez-Gutiérrez

2016-03-01

Full Text Available The challenge of developing effective separation and purification technologies that leave much smaller energy footprints is greater for carbon dioxide (CO2 than for other gases. In addition to its involvement in climate change, CO2 is present as an impurity in biogas and bio-hydrogen (biological production by dark fermentation, in post-combustion processes (flue gas, CO2-N2 and many other gas streams. Selected phenol-formaldehyde resin-based activated carbons prepared in our laboratory have been evaluated under static conditions (adsorption isotherms as potential adsorbents for CO2 separation at sub-atmospheric pressures, i.e., in post-combustion processes or from biogas and bio-hydrogen streams. CO2, H2, N2, and CH4 adsorption isotherms at 25 °C and up to 100 kPa were obtained using a volumetric equipment and were correlated by applying the Sips model. Adsorption equilibrium was then predicted for multicomponent gas mixtures by extending the multicomponent Sips model and the Ideal Adsorbed Solution Theory (IAST in conjunction with the Sips model. The CO2 uptakes of the resin-derived carbons from CO2-CH4, CO2-H2, and CO2-N2 at atmospheric pressure were greater than those of the reference commercial carbon (Calgon BPL. The performance of the resin-derived carbons in terms of equilibrium of adsorption seems therefore relevant to CO2 separation in post-combustion (flue gas, CO2-N2 and in hydrogen fermentation (CO2-H2, CO2-CH4.

1.5 °C carbon budget dependent on carbon cycle uncertainty and future non-CO2 forcing.

Science.gov (United States)

Mengis, Nadine; Partanen, Antti-Ilari; Jalbert, Jonathan; Matthews, H Damon

2018-04-11

Estimates of the 1.5 °C carbon budget vary widely among recent studies, emphasizing the need to better understand and quantify key sources of uncertainty. Here we quantify the impact of carbon cycle uncertainty and non-CO 2 forcing on the 1.5 °C carbon budget in the context of a prescribed 1.5 °C temperature stabilization scenario. We use Bayes theorem to weight members of a perturbed parameter ensemble with varying land and ocean carbon uptake, to derive an estimate for the fossil fuel (FF) carbon budget of 469 PgC since 1850, with a 95% likelihood range of (411,528) PgC. CO 2 emissions from land-use change (LUC) add about 230 PgC. Our best estimate of the total (FF + LUC) carbon budget for 1.5 °C is therefore 699 PgC, which corresponds to about 11 years of current emissions. Non-CO 2 greenhouse gas and aerosol emissions represent equivalent cumulative CO 2 emissions of about 510 PgC and -180 PgC for 1.5 °C, respectively. The increased LUC, high non-CO 2 emissions and decreased aerosols in our scenario, cause the long-term FF carbon budget to decrease following temperature stabilization. In this scenario, negative emissions would be required to compensate not only for the increasing non-CO 2 climate forcing, but also for the declining natural carbon sinks.

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

Energy Technology Data Exchange (ETDEWEB)

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

Efficient capture of CO2 over ordered micro-mesoporous hybrid carbon nanosphere

Science.gov (United States)

Chen, Changwei; Yu, Yanke; He, Chi; Wang, Li; Huang, Huang; Albilali, Reem; Cheng, Jie; Hao, Zhengping

2018-05-01

Four kinds of carbon-based adsorbents (micro-mesoporous hybrid carbon nanosphere and N-doped hollow carbon sphere with single-, double- or ruga-shell morphology) with different structural and textural properties were prepared and systematically studied in CO2 capture. All synthesized samples possess high specific surface area (828-910 m2 g-1), large pore volume (0.71-1.81 cm3 g-1), and different micropore contents varied from 2.1% to 46.4%. Amongst, the ordered micro-mesoporous carbon nanosphere (OM-CNS) exhibits the best adsorption performance with CO2 uptake as high as 3.01 mmol g-1 under conditions of 298 K and 1.0 bar, better than most of the reported CO2 adsorbents. The excellent CO2 adsorption capacity of OM-CNS can be reasonably attributed to the synergistic effect of ordered mesopore channels and abundant structural micropores which are beneficial for the diffusion and trapping of CO2 adsorbate. Moreover, the OM-CNS shows excellent CO2 trapping selectivity and superior stability and recyclability, which endow the OM-CNS as a promising and environmental-friendly adsorbent for CO2 capture and separation under practical conditions.

Natural CO2 Analogs for Carbon Sequestration

Energy Technology Data Exchange (ETDEWEB)

Scott H. Stevens; B. Scott Tye

2005-07-31

The report summarizes research conducted at three naturally occurring geologic CO{sub 2} fields in the US. The fields are natural analogs useful for the design of engineered long-term storage of anthropogenic CO{sub 2} in geologic formations. Geologic, engineering, and operational databases were developed for McElmo Dome in Colorado; St. Johns Dome in Arizona and New Mexico; and Jackson Dome in Mississippi. The three study sites stored a total of 2.4 billion t (46 Tcf) of CO{sub 2} equivalent to 1.5 years of power plant emissions in the US and comparable in size with the largest proposed sequestration projects. The three CO{sub 2} fields offer a scientifically useful range of contrasting geologic settings (carbonate vs. sandstone reservoir; supercritical vs. free gas state; normally pressured vs. overpressured), as well as different stages of commercial development (mostly undeveloped to mature). The current study relied mainly on existing data provided by the CO{sub 2} field operator partners, augmented with new geochemical data. Additional study at these unique natural CO{sub 2} accumulations could further help guide the development of safe and cost-effective design and operation methods for engineered CO{sub 2} storage sites.

Forecasting approach of electrochemical valorisation of CO2 in alkali molten carbonates

International Nuclear Information System (INIS)

Chery, Deborah

2015-01-01

Carbon Dioxide is a greenhouse which can be valorised by means of electrochemical valorisation into carbon monoxide. The main goals of the thesis consist in the theoretical determination of the conductive conditions leading to this electrochemical valorisation in alkali molten carbonates along with the study of the feasibility of this electrochemical reduction in binary and ternary eutectics under experimental condition. CO 2 solubility has been determined by manometric measure and increase along with the temperature. CO 2 electrochemical experimental feasibility into CO in eutectics on gold plate electrode and graphite carbon has been proved by cyclic volt-amperometry for temperatures exceeding 550 C, without gold plate electrode pretreatment and with gold plate pretreatment by an pre-electrolysis at potential slightly negative as the CO 2 reduction potential. A global approach of reactional mechanisms implied in CO 2 reduction is proposed. (author)

Carbon Dioxide (CO2 Sequestration In Bio-Concrete, An Overview

Directory of Open Access Journals (Sweden)

Faisal Alshalif A.

2017-01-01

Full Text Available The emission of CO2 into atmosphere which has increased rapidly in the last years has led to global warming. Therefore, in order to overcome the negative impacts on human and environment, the researchers focused mainly on the reduction and stabilization of CO2 which represent the main contributor in the increasing global warming. The natural capturing and conversion of CO2 from atmosphere is taken place by biological, chemical and physical processes. However, these processes need long time to cause a significant reduction in CO2. Recently, scientists shifted to use green technologies that aimed to produce concrete with high potential to adsorb CO2 in order to accelerate the reduction of CO2. In the present review the potential of bio-concrete to sequestrate CO2 based on carbonation process and as a function of carbonic anhydrase (CA is highlighted. The factors affecting CO2 sequestration in concrete and bacterial species are discussed. It is evident from the literatures, that the new trends to use bio-concrete might contribute in the reduction of CO2 and enhance the strength of non-reinforced concrete.

Polyacrylonitrile-Derived Sponge-Like Micro/Macroporous Carbon for Selective CO2 Separation.

Science.gov (United States)

Guo, Li-Ping; Hu, Qing-Tao; Zhang, Peng; Li, Wen-Cui; Lu, An-Hui

2018-03-25

CO 2 capture under a dynamical flow situation requires adsorbents possessing balanced proportion of macropores as diffusion path and micropores as adsorption reservoir. However, the construction of interconnected micro-/macropores structure coupled with abundant nitrogen species into one carbon skeleton remains a challenge. Here, we report a new approach to prepare sponge-like carbon with a well-developed micro-/macroporous structure and enriched nitrogen species through aqueous phase polymerization of acrylonitrile in the presence of graphene oxide. The tension stress caused by the uniform thermal shrinkage of polyacrylonitrile during the pyrolysis together with the favorable flexibility of graphene oxide sheets are responsible for the formation of the sponge-like morphology. The synergistic effect of micro-/macroporous framework and rich CO 2 -philic site enables such carbon to decrease resistance to mass transfer and show high CO 2 dynamic selectivity over N 2 (454) and CH 4 (11), as well as good CO 2 capacity at 298 K under low CO 2 partial pressure (0.17 bar, a typical CO 2 partial pressure in flue gas). The above attributes make this porous carbon a promising candidate for CO 2 capture from flue gas, methane sources and other relevant applications. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Observation of ferromagnetic ordering in a stable α -Co (OH) 2 phase grown on a Mo S2 surface

Science.gov (United States)

Debnath, Anup; Bhattacharya, Shatabda; Saha, Shyamal K.

2017-12-01

Because of the potential application of Co (OH) 2 in a magnetic cooling system as a result of its superior magnetocaloric effect many people have investigated magnetic properties of Co (OH) 2 . Unfortunately, most of the works have been carried out on the β -Co (OH) 2 phase due to the fact that the α -Co (OH) 2 phase is very unstable and continuously transformed into the stable β -Co (OH) 2 phase. However, in the present work, using a Mo S2 sheet as a two-dimensional template, we have been able to synthesize a stable α -Co (OH) 2 phase in addition to a β -Co (OH) 2 phase by varying the layer thickness. It is seen that for thinner samples the β phase, while for thicker samples α phase, is grown on the Mo S2 surface. Magnetic measurements are carried out for the samples over the temperature range from 2 to 300 K and it is seen that for the β phase, ferromagnetic ordering with fairly large coercivity (1271 Oe) at 2 K is obtained instead of the usual antiferromagnetism. The most interesting result is the observation of ferromagnetic ordering with a transition temperature (Curie temperature) more than 100 K in the α -Co (OH) 2 phase. Complete saturation in the hysteresis curve under application of very low field having coercivity of ˜162 Oe at 2 K and 60 Oe at 50 K is obtained. A thin stable α -Co (OH) 2 phase grown on Mo S2 surface with very soft ferromagnetic ordering will be very useful as the core material in electromagnets.

Seasonal changes in stable carbon isotope ratios within annual growth rings of Pinus radiata

International Nuclear Information System (INIS)

Walcroft, A.; Silvester, W.; Whitehead, D.; Kelliher, F.

1997-01-01

The stable isotope composition of photosynthetically assimilated carbon (δ 13 C) is determined by the ratio of the leaf internal CO 2 concentration (c i ) to that of the ambient air (c a ), and so reflects the contribution of both stomatal conductance (g s ) and the rate of photosynthesis (A). Assimilated carbon which is subsequently laid down as wood in annual growth rings may therefore represent a time integrated record of physiological responses by the whole tree to seasonal changes in the environmental variables regulating growth. We analysed the stable carbon isotope composition of Pinus radiata wood collected from two plantation forest sites in New Zealand which differ markedly in temperature, rainfall and soil characteristics. For both sites, discs were cut from the stem of several trees near ground level and whole wood samples were taken from within individual annual growth rings over a number of years. At one site, diameter bands were installed over the 1994 - 1996 growing seasons in order to date precisely the formation of wood during that time. Trees at each site consistently showed a seasonal pattern in the stable isotope composition of wood within individual growth rings. The amplitude of seasonal δ 13 C variation at the wet and dry sites were 1-2 per thousand and 4 per thousand respectively. Mean δ 13 C values from the wet site were 3 per thousand more 13 C depleted than those from the dry site implying lower water-use efficiency (carbon assimilation per unit transpiration). A process-based, model of stomatal conductance and CO 2 assimilation was combined with a soil-water balance model to estimate the average daily leaf-level intercellular CO 2 concentration (c i ). Over two growing seasons at each site there was generally good agreement between mean canopy-level c i derived from the tree-ring δ 13 C data and modelled leaf-level c i levels. Further, the ratio of annual CO 2 assimilation to transpiration estimated by the model for each site

Kinetics of carbonate dissolution in CO2-saturated aqueous system at reservoir conditions

Science.gov (United States)

Peng, Cheng; Crawshaw, John P.; Maitland, Geoffrey; Trusler, J. P. Martin

2014-05-01

In recent years, carbon capture and storage (CCS) has emerged as a key technology for limiting anthropogenic CO2 emissions while allowing the continued utilisation of fossil fuels. The most promising geological storage sites are deep saline aquifers because the capacity, integrity and injection economics are most favourable, and the environmental impact can be minimal. Many rock-fluid chemical reactions are known to occur both during and after CO2 injection in saline aquifers. The importance of rock-fluid reactions in the (CO2 + H2O) system can be understood in terms of their impact on the integrity and stability of both the formation rocks and cap rocks. The chemical interactions between CO2-acidified brines and the reservoir minerals can influence the porosity and permeability of the formations, resulting in changes in the transport processes occurring during CO2 storage. Since carbonate minerals are abundant in sedimentary rocks, one of the requirements to safely implement CO2 storage in saline aquifers is to characterise the reactivity of carbonate minerals in aqueous solutions at reservoir conditions. In this work, we reported measurements of the intrinsic rate of carbonate dissolution in CO2-saturated water under high-temperature high-pressure reservoir conditions extending up to 373 K and 14 MPa. The rate of carbonate dissolution in CO2-free HCl(aq) was also measured at ambient pressure at temperatures up to 353 K. Various pure minerals and reservoir rocks were investigated in this study, including single-crystals of calcite and magnesite, and samples of dolomite, chalks and sandstones. A specially-designed batch reactor system, implementing the rotating disc technique, was used to obtain the intrinsic reaction rate at the solid/liquid interface, free of mass transfer effects. The effective area and mineralogy of the exposed surface was determined by a combination of surface characterisation techniques including XRD, SEM, EDX and optical microscopy. The

Climatic significance of stable isotope characteristics of air-CO2 and rainfall in Delhi area water-plant-air system

International Nuclear Information System (INIS)

Datta, P.S.; Tyagi, S.K.

2002-01-01

In recent years, there is a global concern on the role of carbon dioxide in atmosphere in affecting the climate. The present models of global atmospheric circulation suggest that oceans sequester about one-third of the CO 2 released by anthropogenic activities, and biospheric productivity is the primary cause of the interannual fluctuations in the atmospheric CO 2 . However, most of the times, the excess of CO 2 in air is associated with the presence of anthropogenic pollutants from urbanised centres. Therefore, the studies on the pattern of local variations in the isotopic composition of air CO 2 and rainfall in urban areas are expected to provide important information on the atmospheric circulation processes which affect the climate on a regional scale. Internationally, aspects of climate change have been so far demonstrated using isotopic data mainly from temperate climates, and there is limited understanding of the factors controlling stable isotopic composition of air-CO 2 and rainfall in tropical regions. In this context, to assess the magnitude of the above mentioned effects, analysis of the data on the variations in the 13 C/ 12 C and 18 O/ 16 O signatures of air-CO 2 in Delhi area water-plant-air system is presented here

Mineral storage of CO2/H2S gas mixture injection in basaltic rocks

Science.gov (United States)

Clark, D. E.; Gunnarsson, I.; Aradottir, E. S.; Oelkers, E. H.; Sigfússon, B.; Snæbjörnsdottír, S. Ó.; Matter, J. M.; Stute, M.; Júlíusson, B. M.; Gíslason, S. R.

2017-12-01

Carbon capture and storage is one solution to reducing CO2 emissions in the atmosphere. The long-term geological storage of buoyant supercritical CO2 requires high integrity cap rock. Some of the risk associated with CO2 buoyancy can be overcome by dissolving CO2 into water during its injection, thus eliminating its buoyancy. This enables injection into fractured rocks, such as basaltic rocks along oceanic ridges and on continents. Basaltic rocks are rich in divalent cations, Ca2+, Mg2+ and Fe2+, which react with CO2 dissolved in water to form stable carbonate minerals. This possibility has been successfully tested as a part of the CarbFix CO2storage pilot project at the Hellisheiði geothermal power plant in Iceland, where they have shown mineralization occurs in less than two years [1, 2]. Reykjavik Energy and the CarbFix group has been injecting a mixture of CO2 and H2S at 750 m depth and 240-250°C since June 2014; by 1 January 2016, 6290 tons of CO2 and 3530 tons of H2S had been injected. Once in the geothermal reservoir, the heat exchange and sufficient dissolution of the host rock neutralizes the gas-charged water and saturates the formation water respecting carbonate and sulfur minerals. A thermally stable inert tracer was also mixed into the stream to monitor the subsurface transport and to assess the degree of subsurface carbonation and sulfide precipitation [3]. Water and gas samples have been continuously collected from three monitoring wells and geochemically analyzed. Based on the results, mineral saturation stages have been defined. These results and tracer mass balance calculations are used to evaluate the rate and magnitude of CO2 and H2S mineralization in the subsurface, with indications that mineralization of carbon and sulfur occurs within months. [1] Gunnsarsson, I., et al. (2017). Rapid and cost-effective capture and subsurface mineral storage of carbon and sulfur. Manuscript submitted for publication. [2] Matter, J., et al. (2016). Rapid

Determination of the origin of dissolved inorganic carbon in groundwater around a reclaimed landfill in Otwock using stable carbon isotopes

Energy Technology Data Exchange (ETDEWEB)

Porowska, Dorota, E-mail: dorotap@uw.edu.pl

2015-05-15

Highlights: • Research showed the origin of DIC in the groundwater around a reclaimed landfill. • Carbon isotope was used to evaluate the contributions of carbon from different sources. • The leachate-contaminated water was isotopically distinct from the natural groundwater. • DIC in the natural groundwater comes from organic matter and dissolution of carbonates. • In the contaminated water, DIC comes from organic matter in the aquifer and landfill. - Abstract: Chemical and isotopic analyses of groundwater from piezometers located around a reclaimed landfill in Otwock (Poland) were performed in order to trace the origin of dissolved inorganic carbon (DIC) in the groundwater. Due to differences in the isotopic composition of carbon from different sources, an analysis of stable carbon isotopes in the groundwater, together with the Keeling plot approach and a two-component mixing model allow us to evaluate the relative contributions of carbon from these sources in the groundwater. In the natural (background) groundwater, DIC concentrations and the isotopic composition of DIC (δ{sup 13}C{sub DIC}) comes from two sources: decomposition of organic matter and carbonate dissolution within the aquifer sediments, whereas in the leachate-contaminated groundwater, DIC concentrations and δ{sup 13}C{sub DIC} values depend on the degradation of organic matter within the aquifer sediments and biodegradation of organic matter stored in the landfill. From the mixing model, about 4–54% of the DIC pool is derived from organic matter degradation and 96–46% from carbonate dissolution in natural conditions. In the leachate-contaminated groundwater, about 20–53% of the DIC is derived from organic matter degradation of natural origin and 80–47% from biodegradation of organic matter stored in the landfill. Partial pressure of CO{sub 2} (P CO{sub 2}) was generally above the atmospheric, hence atmospheric CO{sub 2} as a source of carbon in DIC pool was negligible in the

Carbon recycling by cyanobacteria: improving CO2 fixation through chemical production.

Science.gov (United States)

Zhang, Angela; Carroll, Austin L; Atsumi, Shota

2017-09-01

Atmospheric CO2 levels have reached an alarming level due to industrialization and the burning of fossil fuels. In order to lower the level of atmospheric carbon, strategies to sequester excess carbon need to be implemented. The CO2-fixing mechanism in photosynthetic organisms enables integration of atmospheric CO2 into biomass. Additionally, through exogenous metabolic pathways in these photosynthetic organisms, fixed CO2 can be routed to produce various commodity chemicals that are currently produced from petroleum. This review will highlight studies and modifications to different components of cyanobacterial CO2-fixing systems, as well as the application of these systems toward CO2-derived chemical production. 2,3-Butanediol is given particular focus as one of the most thoroughly studied systems for conversion of CO2 to a bioproduct. © FEMS 2017. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.

Stable carbon isotope depth profiles and soil organic carbon dynamics in the lower Mississippi Basin

Science.gov (United States)

Wynn, J.G.; Harden, J.W.; Fries, T.L.

2006-01-01

Analysis of depth trends of 13C abundance in soil organic matter and of 13C abundance from soil-respired CO2 provides useful indications of the dynamics of the terrestrial carbon cycle and of paleoecological change. We measured depth trends of 13C abundance from cropland and control pairs of soils in the lower Mississippi Basin, as well as the 13C abundance of soil-respired CO2 produced during approximately 1-year soil incubation, to determine the role of several candidate processes on the 13C depth profile of soil organic matter. Depth profiles of 13C from uncultivated control soils show a strong relationship between the natural logarithm of soil organic carbon concentration and its isotopic composition, consistent with a model Rayleigh distillation of 13C in decomposing soil due to kinetic fractionation during decomposition. Laboratory incubations showed that initially respired CO 2 had a relatively constant 13C content, despite large differences in the 13C content of bulk soil organic matter. Initially respired CO2 was consistently 13C-depleted with respect to bulk soil and became increasingly 13C-depleted during 1-year, consistent with the hypothesis of accumulation of 13C in the products of microbial decomposition, but showing increasing decomposition of 13C-depleted stable organic components during decomposition without input of fresh biomass. We use the difference between 13C / 12C ratios (calculated as ??-values) between respired CO 2 and bulk soil organic carbon as an index of the degree of decomposition of soil, showing trends which are consistent with trends of 14C activity, and with results of a two-pooled kinetic decomposition rate model describing CO2 production data recorded during 1 year of incubation. We also observed inconsistencies with the Rayleigh distillation model in paired cropland soils and reasons for these inconsistencies are discussed. ?? 2005 Elsevier B.V. All rights reserved.

Integrated Energy System with Beneficial Carbon Dioxide (CO{sub 2}) Use

Energy Technology Data Exchange (ETDEWEB)

Sun, Xiaolei; Rink, Nancy

2011-04-30

To address the public concerns regarding the consequences of climate change from anthropogenic carbon dioxide (CO{sub 2}) emissions, the U.S. Department of Energy National Energy Technology Laboratory (DOE-NETL) is actively funding a CO{sub 2} management program to develop technologies capable of reducing the CO{sub 2} emissions from fossil fuel power plants and other industrial facilities. Over the past decade, this program has focused on reducing the costs of carbon capture and storage technologies. Recently, DOE-NETL launched an alternative CO{sub 2} mitigation program focusing on beneficial CO{sub 2} reuse and supporting the development of technologies that mitigate emissions by converting CO{sub 2} to solid mineral form that can be utilized for enhanced oil recovery, in the manufacturing of concrete or as a benign landfill, in the production of valuable chemicals and/or fuels. This project was selected as a CO{sub 2} reuse activity which would conduct research and development (R&D) at the pilot scale via a cost-shared Cooperative Agreement number DE-FE0001099 with DOE-NETL and would utilize funds setaside by the American Recovery and Reinvestment Act (ARRA) of 2009 for Industrial Carbon Capture and Sequestration R&D,

Wall-crossing between stable and co-stable ADHM data

Science.gov (United States)

Ohkawa, Ryo

2018-06-01

We prove formula between Nekrasov partition functions defined from stable and co-stable ADHM data for the plane following method by Nakajima and Yoshioka (Kyoto J Math 51(2):263-335, 2011) based on the theory of wall-crossing formula developed by Mochizuki (Donaldson type invariants for algebraic surfaces: transition of moduli stacks, Lecture notes in mathematics, vol 1972, Springer, Berlin, 2009). This formula is similar to conjectures by Ito et al. [J High Energy Phys 2013(5):045, 2013, (4.1), (4.2)] for A1 singularity.

Direct synthesis of dimethyl carbonate from CO2 and methanol over ...

Indian Academy of Sciences (India)

The direct synthesis of dimethyl carbonate (DMC) from carbon dioxide (CO2) and methanol is ... Zirconia and ceria-based catalysts were most effective ... construction of a validation plant for dialkyl carbonates .... (mmol of MeOH consumed/2).

CO2 Capture by Absorption with Potassium Carbonate

Energy Technology Data Exchange (ETDEWEB)

Gary T. Rochelle; Eric Chen; Babatunde Oyenekan; Andrew Sexton; Jason Davis; Marcus Hilliard; Amorvadee Veawab

2006-07-28

The objective of this work is to improve the process for CO{sub 2} capture by alkanolamine absorption/stripping by developing an alternative solvent, aqueous K{sub 2}CO{sub 3} promoted by piperazine. The pilot plant data have been reconciled using 17% inlet CO{sub 2}. A rate-based model demonstrates that the stripper is primarily controlled by liquid film mast transfer resistance, with kinetics at vacuum and diffusion of reactants and products at normal pressure. An additional major unknown ion, probably glyoxylate, has been observed in MEA degradation. Precipitation of gypsum may be a feasible approach to removing sulphate from amine solutions and providing for simultaneous removal of CO{sub 2} and SO{sub 2}. Corrosion of carbon steel in uninhibited MEA solution is increased by increased amine concentration, by addition of piperazine, and by greater CO{sub 2} loading.

Adsorbed Carbon Formation and Carbon Hydrogenation for CO_2 Methanation on the Ni(111) Surface: ASED-MO Study

International Nuclear Information System (INIS)

Choe, Sang Joon; Kang, Hae Jin; Kim, Su Jin; Park, Sung Bae; Park, Dong Ho; Huh, Do Sung

2005-01-01

Using the ASED-MO (Atom Superposition and Electron Delocalization-Molecular Orbital) theory, we investigated carbon formation and carbon hydrogenation for CO_2 methanation on the Ni (111) surface. For carbon formation mechanism, we calculated the following activation energies, 1.27 eV for CO_2 dissociation, 2.97 eV for the CO, 1.93 eV for 2CO dissociation, respectively. For carbon methanation mechanism, we also calculated the following activation energies, 0.72 eV for methylidyne, 0.52 eV for methylene and 0.50 eV for methane, respectively. We found that the calculated activation energy of CO dissociation is higher than that of 2CO dissociation on the clean surface and base on these results that the CO dissociation step are the ratedetermining of the process. The C-H bond lengths of CH_4 the intermediate complex are 1.21 A, 1.31 A for the C···H_(_1_), and 2.82 A for the height, with angles of 105 .deg. for H_(_1_)CH and 98 .deg. for H_(_1_)CH_(_1_)

CO2 (carbon dioxide) fixation by applying new chemical absorption-precipitation methods

International Nuclear Information System (INIS)

Park, Sangwon; Lee, Min-Gu; Park, Jinwon

2013-01-01

CO 2 (carbon dioxide) is the most common greenhouse gas and most of it is emitted from human activities. The methods for CO 2 emission reduction can be divided into physical, chemical, and biochemical methods. Among the physical and chemical methods, CCS (carbon capture and storage) is a well-known reducing technology. However, this method has many disadvantages including the required storage area. In general, CCS requires capture and storage processes. In this study, we propose a method for reusing the absorbed CO 2 either in nature or in industry. The emitted CO 2 was converted into CO 3 2− using a conversion solution, and then made into a carbonate by combining the conversion solution with metal ions at normal temperature and pressure. The resulting carbonate was analyzed using FT-IR (Fourier transform infrared spectroscopy) and XRD (X-ray diffraction). We verified the formation of a solid consisting of calcite and vaterite. In addition, the conversion solution that was used could be reused in the same process of CCS technology. Our study demonstrates a successful method of reducing and reusing emitted CO 2 , thereby making CO 2 a potential future resource. - Highlights: • This study focused on a new CO 2 fixation process method. • In CCS technology, the desorption process requires high thermal energy consumption. • This new method does not require a desorption process because the CO 2 is accomplished through CaCO 3 crystallization. • A new absorption method is possible instead of the conventional absorption-desorption process. • This is not only a rapid reaction for fixing CO 2 , but also economically feasible

Carbon dynamics and CO2 and CH4 outgassing in the Mekong delta

Science.gov (United States)

Borges, Alberto V.; Abril, Gwenaël; Bouillon, Steven

2018-02-01

We report a data set of biogeochemical variables related to carbon cycling obtained in the three branches (Mỹ Tho, Hàm Luông, Cố Chiên) of the Mekong delta (Bến Tre province, Vietnam) in December 2003, April 2004, and October 2004. Both the inner estuary (upstream of the mouth) and the outer estuary (river plume) were sampled, as well as side channels. The values of the partial pressure of CO2 (pCO2) ranged between 232 and 4085 ppm, O2 saturation level (%O2) between 63 and 114 %, and CH4 between 2 and 2217 nmol L-1, within the ranges of values previously reported in temperate and tropical meso- and macro-tidal estuaries. Strong seasonal variations were observed. In the upper oligohaline estuary, low pCO2 (479-753 ppm) and high %O2 (98-106 %) values were observed in April 2004 most probably related to freshwater phytoplankton growth owing to low freshwater discharge (1400 m3 s-1) and increase in water residence time; during the two other sampling periods with a higher freshwater discharge (9300-17 900 m3 s-1), higher pCO2 (1895-2664 ppm) and lower %O2 (69-84 %) values were observed in the oligohaline part of the estuary. In October 2004, important phytoplankton growth occurred in the offshore part of the river plume as attested by changes in the contribution of particulate organic carbon (POC) to total suspended matter (TSM) (%POC) and the stable isotope composition of POC (δ13C-POC), possibly related to low TSM values (improvement of light conditions for phytoplankton development), leading to low pCO2 (232 ppm) and high %O2 (114 %) values. Water in the side channels in the Mekong delta was strongly impacted by inputs from the extensive shrimp farming ponds. The values of pCO2, CH4, %O2, and the stable isotope composition of dissolved inorganic carbon (δ13C-DIC) indicated intense organic matter degradation that was partly mediated by sulfate reduction in sediments, as revealed by the slope of total alkalinity (TA) and DIC covariations. The δ13C

Mechanisms of aqueous wollastonite carbonation as a possible CO2 sequestration process

International Nuclear Information System (INIS)

Huijgen, W.J.J.; Comans, R.N.J.; Witkamp, G.J.

2006-02-01

The mechanisms of aqueous wollastonite carbonation as a possible carbon dioxide sequestration process were investigated experimentally by systematic variation of the reaction temperature, CO2 pressure, particle size, reaction time, liquid to solid ratio and agitation power. The carbonation reaction was observed to occur via the aqueous phase in two steps: (1) Ca leaching from the CaSiO3 matrix and (2) CaCO3 nucleation and growth. Leaching is hindered by a Ca-depleted silicate rim resulting from incongruent Ca-dissolution. Two temperature regimes were identified in the overall carbonation process. At temperatures below an optimum reaction temperature, the overall reaction rate is probably limited by the leaching rate of Ca. At higher temperatures, nucleation and growth of calcium carbonate is probably limiting the conversion, due to a reduced (bi)carbonate activity. The mechanisms for the aqueous carbonation of wollastonite were shown to be similar to those reported previously for an industrial residue and a Mg-silicate. The carbonation of wollastonite proceeds rapidly relative to Mg-silicates, with a maximum conversion in 15 min of 70% at 200C, 20 bar CO2 partial pressure and a particle size of <38 μm. The obtained insight in the reaction mechanisms enables the energetic and economic assessment of CO2 sequestration by wollastonite carbonation, which forms an essential next step in its further development

CO{sub 2} capture using some fly ash-derived carbon materials

Energy Technology Data Exchange (ETDEWEB)

A. Arenillas; K.M. Smith; T.C. Drage; C.E. Snape [University of Nottingham, Nottingham (United Kingdom). Nottingham Fuel and Energy Centre, School of Chemical, Environmental and Mining Engineering

2005-12-01

Adsorption is considered to be one of the more promising technologies for capturing CO{sub 2} from flue gases. For post-combustion capture, the success of such an approach is however dependent on the development of an adsorbent that can operate competitively at relatively high temperatures. In this work, low cost carbon materials derived from fly ash, are presented as effective CO{sub 2} sorbents through impregnation these with organic bases, for example, polyethylenimine aided by polyethylene glycol. The results show that for samples derived from a fly ash carbon concentrate, the CO{sub 2} adsorption capacities were relatively high (up to 4.5 wt%) especially at high temperatures (75{sup o}C), where commercial active carbons relying on physi-sorption have low capacities. The addition of PEG improves the adsorption capacity and reduces the time taken for the sample to reach the equilibrium. No CO{sub 2} seems to remain after desorption, suggesting that the process is fully reversible. 24 refs., 6 figs., 2 tabs.

Catalytic performance of activated carbon supported cobalt catalyst for CO2 reforming of CH4.

Science.gov (United States)

Zhang, Guojie; Su, Aiting; Du, Yannian; Qu, Jiangwen; Xu, Ying

2014-11-01

Syngas production by CO2 reforming of CH4 in a fixed bed reactor was investigated over a series of activated carbon (AC) supported Co catalysts as a function of Co loading (between 15 and 30wt.%) and calcination temperature (Tc=300, 400 or 500°C). The catalytic performance was assessed through CH4 and CO2 conversions and long-term stability. XRD and SEM were used to characterize the catalysts. It was found that the stability of Co/AC catalysts was strongly dependent on the Co loading and calcination temperature. For the loadings (25wt.% for Tc=300°C), stable activities have been achieved. The loading of excess Co (>wt.% 25) causes negative effects not only on the performance of the catalysts but also on the support surface properties. In addition, the experiment showed that ultrasound can enhance and promote dispersion of the active metal on the carrier, thus improving the catalytic performance of the catalyst. The catalyst activity can be long-term stably maintained, and no obvious deactivation has been observed in the first 2700min. After analyzing the characteristics, a reaction mechanism for CO2 reforming of CH4 over Co/AC catalyst was proposed. Copyright © 2014 Elsevier Inc. All rights reserved.

Modeling carbon sequestration in afforestation, agroforestry and forest management projects: the CO2FIX V.2 approach

NARCIS (Netherlands)

Masera, O.R.; Garza-Caligaris, J.F.; Kanninen, M.; Karjalainen, T.; Liski, J.; Nabuurs, G.J.; Pussinen, A.; Jong de, B.H.J.; Mohren, G.M.J.

2003-01-01

The paper describes the Version 2 of the CO2FIX (CO2FIX V.2) model, a user-friendly tool for dynamically estimating the carbon sequestration potential of forest management, agroforesty and afforestation projects. CO2FIX V.2 is a multi-cohort ecosystem-level model based on carbon accounting of forest

Geological Sequestration of CO2 by Hydrous Carbonate Formation with Reclaimed Slag

Energy Technology Data Exchange (ETDEWEB)

Von L. Richards; Kent Peaslee; Jeffrey Smith

2008-02-06

The concept of this project is to develop a process that improves the kinetics of the hydrous carbonate formation reaction enabling steelmakers to directly remove CO2 from their furnace exhaust gas. It is proposed to bring the furnace exhaust stream containing CO2 in contact with reclaimed steelmaking slag in a reactor that has an environment near the unit activity of water resulting in the production of carbonates. The CO2 emissions from the plant would be reduced by the amount sequestered in the formation of carbonates. The main raw materials for the process are furnace exhaust gases and specially prepared slag.

Aluminosilicate Dissolution and Silicate Carbonation during Geologic CO2 Sequestration

Science.gov (United States)

Min, Yujia

Geologic CO2 sequestration (GCS) is considered a promising method to reduce anthropogenic CO2 emission. Assessing the supercritical CO2 (scCO2) gas or liquid phase water (g, l)-mineral interactions is critical to evaluating the viability of GCS processes. This work contributes to our understanding of geochemical reactions at CO 2-water (g, l)-mineral interfaces, by investigating the dissolution of aluminosilicates in CO2-acidified water (l). Plagioclase and biotite were chosen as model minerals in reservoir rock and caprock, respectively. To elucidate the effects of brine chemistry, first, the influences of cations in brine including Na, Ca, and K, have been investigated. In addition to the cations, the effects of abundant anions including sulfate and oxalate were also examined. Besides the reactions in aqueous phase, we also examine the carbonation of silicates in water (g)-bearing supercritical CO2 (scCO2) under conditions relevant to GCS. For the metal carbonation, in particular, the effects of particle sizes, water, temperature, and pressure on the carbonation of wollastonite were systematically examined. For understanding the cations effects in brine, the impacts of Na concentrations up to 4 M on the dissolution of plagioclase and biotite were examined. High concentrations of Na significantly inhibited plagioclase dissolution by competing adsorption with proton and suppressing proton-promoted dissolution. Ca has a similar effect to Na, and their effects did not suppress each other when Na and Ca co-existed. For biotite, the inhibition effects of Na coupled with an enhancing effect due to ion exchange reaction between Na and interlayer K, which cracked the basal surfaces of biotite. The K in aqueous phase significantly inhibited the dissolution. If the biotite is equilibrated with NaCl solutions initially, the biotite dissolved faster than the original biotite and the dissolution was inhibited by Na and K in brine. The outcomes improve our current knowledge of

Leak detection of CO2 pipelines with simple atmospheric CO2 sensors for carbon capture and storage

NARCIS (Netherlands)

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

2013-01-01

This paper presents a field test performed with five relatively simple CO2 sensors (Vaisala Carbocap GMP343) that were placed for more than one year in a field in Ten Post, Groningen, The Netherlands. Aim was to investigate their potential use in monitoring pipelines transporting CO2 for carbon

One strategy for estimating the potential soil carbon storage due to CO2 fertilization

International Nuclear Information System (INIS)

Harrison, K.G.; Bonani, G.

1994-01-01

Soil radiocarbon measurements can be used to estimate soil carbon turnover rates and inventories. A labile component of soil carbon has the potential to respond to perturbations such as CO 2 fertilization, changing climate, and changing land use. Soil carbon has influenced past and present atmospheric CO 2 levels and will influence future levels. A model is used to calculate the amount of additional carbon stored in soil because of CO 2 fertilization

Impact of atmospheric and terrestrial CO2 feedbacks on fertilization-induced marine carbon uptake

Science.gov (United States)

Oschlies, A.

2009-08-01

The sensitivity of oceanic CO2 uptake to alterations in the marine biological carbon pump, such as brought about by natural or purposeful ocean fertilization, has repeatedly been investigated by studies employing numerical biogeochemical ocean models. It is shown here that the results of such ocean-centered studies are very sensitive to the assumption made about the response of the carbon reservoirs on the atmospheric side of the sea surface. Assumptions made include prescribed atmospheric pCO2, an interactive atmospheric CO2 pool exchanging carbon with the ocean but not with the terrestrial biosphere, and an interactive atmosphere that exchanges carbon with both oceanic and terrestrial carbon pools. The impact of these assumptions on simulated annual to millennial oceanic carbon uptake is investigated for a hypothetical increase in the C:N ratio of the biological pump and for an idealized enhancement of phytoplankton growth. Compared to simulations with interactive atmosphere, using prescribed atmospheric pCO2 overestimates the sensitivity of the oceanic CO2 uptake to changes in the biological pump, by about 2%, 25%, 100%, and >500% on annual, decadal, centennial, and millennial timescales, respectively. The smaller efficiency of the oceanic carbon uptake under an interactive atmosphere is due to the back flux of CO2 that occurs when atmospheric CO2 is reduced. Adding an interactive terrestrial carbon pool to the atmosphere-ocean model system has a small effect on annual timescales, but increases the simulated fertilization-induced oceanic carbon uptake by about 4%, 50%, and 100% on decadal, centennial, and millennial timescales, respectively, for pCO2 sensitivities of the terrestrial carbon storage in the middle range of the C4MIP models (Friedlingstein et al., 2006). For such sensitivities, a substantial fraction of oceanic carbon uptake induced by natural or purposeful ocean fertilization originates, on timescales longer than decades, not from the atmosphere

CO2 CAPTURE BY ABSORPTION WITH POTASSIUM CARBONATE

Energy Technology Data Exchange (ETDEWEB)

Gary T. Rochelle; A. Frank Seibert; J. Tim Cullinane; Terraun Jones

2003-01-01

The objective of this work is to improve the process for CO{sub 2} capture by alkanolamine absorption/stripping by developing an alternative solvent, aqueous K{sub 2}CO{sub 3} promoted by piperazine. Progress has been made in this reporting period on three subtasks. The rigorous Electrolyte Non-Random Two-Liquid (electrolyte-NRTL) model has been regressed to represent CO{sub 2} solubility in potassium carbonate/bicarbonate solutions. An analytical method for piperazine has been developed using a gas chromatograph. Funding has been obtained and equipment has been donated to provide for modifications of the existing pilot plant system with stainless steel materials.

Carbon dioxide (CO2) capture and storage : Canadian market development

International Nuclear Information System (INIS)

Hendriks, A.

2006-01-01

Carbon dioxide (CO 2 ) enhanced oil recovery (EOR) is used to extend the life of light oil reservoirs in Canada. An additional 13 per cent of original oil in place is typically recovered using CO 2 flooding processes. However, a carbon capture and storage (CCS) market is needed in order to commercialize CO 2 flooding technologies. CO 2 can be obtained from naturally-occurring accumulations in underground reservoirs, electrical and coal-fired generation plants, petrochemical facilities, and upstream oil and gas processing facilities. CO 2 is sequestered in EOR processes, in sour gas disposal processes, solvent recovery processes, and in coalbed methane (CBM) extraction. It is also disposed in depleted fields and aquifers. While CCS technologies are mature, project economics remain marginal. However, CCS in EOR is commercially feasible at current high oil prices. No transportation infrastructure is in place to transport sources of CO 2 in the high volumes needed to establish a market. While governments have created a favourable public policy environment for CCS, governments will need to address issues related to infrastructure, public perception of CCS, and stakeholder engagement with CCS projects. It was concluded that CCS and CO 2 flooding techniques have the capacity to reduce greenhouse gas (GHG) emissions while helping to sustain light oil production. tabs., figs

The global pyrogenic carbon cycle and its impact on the level of atmospheric CO2 over past and future centuries.

Science.gov (United States)

Landry, Jean-Sébastien; Matthews, H Damon

2017-08-01

The incomplete combustion of vegetation and dead organic matter by landscape fires creates recalcitrant pyrogenic carbon (PyC), which could be consequential for the global carbon budget if changes in fire regime, climate, and atmospheric CO 2 were to substantially affect gains and losses of PyC on land and in oceans. Here, we included global PyC cycling in a coupled climate-carbon model to assess the role of PyC in historical and future simulations, accounting for uncertainties through five sets of parameter estimates. We obtained year-2000 global stocks of (Central estimate, likely uncertainty range in parentheses) 86 (11-154), 47 (2-64), and 1129 (90-5892) Pg C for terrestrial residual PyC (RPyC), marine dissolved PyC, and marine particulate PyC, respectively. PyC cycling decreased atmospheric CO 2 only slightly between 1751 and 2000 (by 0.8 Pg C for the Central estimate) as PyC-related fluxes changed little over the period. For 2000 to 2300, we combined Representative Concentration Pathways (RCPs) 4.5 and 8.5 with stable or continuously increasing future fire frequencies. For the increasing future fire regime, the production of new RPyC generally outpaced the warming-induced accelerated loss of existing RPyC, so that PyC cycling decreased atmospheric CO 2 between 2000 and 2300 for most estimates (by 4-8 Pg C for Central). For the stable fire regime, however, PyC cycling usually increased atmospheric CO 2 (by 1-9 Pg C for Central), and only the most extreme choice of parameters maximizing PyC production and minimizing PyC decomposition led to atmospheric CO 2 decreases under RCPs 4.5 and 8.5 (by 5-8 Pg C). Our results suggest that PyC cycling will likely reduce the future increase in atmospheric CO 2 if landscape fires become much more frequent; however, in the absence of a substantial increase in fire frequency, PyC cycling might contribute to, rather than mitigate, the future increase in atmospheric CO 2 . © 2016 John Wiley & Sons Ltd.

Tagging CO2 to Enable Quantitative Inventories of Geological Carbon Storage

Energy Technology Data Exchange (ETDEWEB)

Lackner, Klaus; Matter, Juerg; Park, Ah-Hyung; Stute, Martin; Carson, Cantwell; Ji, Yinghuang

2014-06-30

In the wake of concerns about the long term integrity and containment of sub-surface CO2 sequestration reservoirs, many efforts have been made to improve the monitoring, verification, and accounting methods for geo-sequestered CO2. Our project aimed to demonstrate the feasibility of a system designed to tag CO2 with carbon isotope 14C immediately prior to sequestration to a level that is normal on the surface (one part per trillion). Because carbon found at depth is naturally free of 14C, this tag would easily differentiate pre-existing carbon from anthropogenic injected carbon and provide an excellent handle for monitoring its whereabouts in the subsurface. It also creates an excellent handle for adding up anthropogenic carbon inventories. Future inventories in effect count 14C atoms. Accordingly, we have developed a 14C tagging system suitable for use at the part-per-trillion level. This system consists of a gas-exchange apparatus to make disposable cartridges ready for controlled injection into a fast flowing stream of pressurized CO2. We built a high-pressure injection and tagging system, and a 14C detection system. The disposable cartridge and injection system have been successfully demonstrated in the lab with a high-pressure flow reactor, as well as in the field at the CarbFix CO2 sequestration site in Iceland. The laser-based 14C detection system originally conceived has been shown to possess inadequate sensitivity for ambient levels. Alternative methods for detecting 14C, such as saturated cavity absorption ringdown spectroscopy and scintillation counting, may still be suitable. KEYWORDS

Negative CO2 emissions via subsurface mineral carbonation in fractured peridotite

Science.gov (United States)

Kelemen, P. B.; Matter, J.

2014-12-01

Uptake of CO2 from surface water via mineral carbonation in peridotite can be engineered to achieve negative CO2 emissions. Reaction with peridotite, e.g., CO2 + olivine (A), serpentine (B) and brucite (C), forms inert, non-toxic, solid carbonates such as magnesite. Experimental studies show that A can be 80% complete in a few hours with 30 micron powders and elevated P(CO2) [1,2,3]. B is slower, but in natural systems the rate of B+C is significant [4]. Methods for capture of dilute CO2 via mineral carbonation [4,5,6,7] are not well known, though CO2 storage via mineral carbonation has been discussed for decades [8,9]. Where crushed peridotite is available, as in mine tailings, increased air or water flow could enhance CO2 uptake at a reasonable cost [4,5]. Here we focus on enhancing subsurface CO2 uptake from surface water flowing in fractured peridotite, in systems driven by thermal convection such as geothermal power plants. Return of depleted water to the surface would draw down CO2 from the air [6,7]. CO2 uptake from water, rate limited by flow in input and output wells, could exceed 1000 tons CO2/yr [7]. If well costs minus power sales were 0.1M to 1M and each system lasts 10 years this costs oil industry. Uptake of 1 Gt CO2/yr at 1000 t/well/yr requires 1M wells, comparable to the number of producing oil and gas wells in the USA. Subsurface CO2 uptake could first be applied in coastal, sub-seafloor peridotite with onshore drilling. Sub-seafloor peridotite is extensive off Oman, New Caledonia and Papua New Guinea, with smaller amounts off Spain, Morocco, USA, etc. This would be a regional contribution, used in parallel with other methods elsewhere. To achieve larger scale is conceivable. There is a giant mass of seafloor peridotite along slow-spreading mid-ocean ridges. Could robotic drills enhance CO2 uptake at a reasonable cost, while fabric chimneys transport CO2-depleted water to the sea surface? Does anyone know James Cameron's phone number? [1] O

Soil carbon dioxide (CO 2 ) efflux of two shrubs in response to plant ...

African Journals Online (AJOL)

Although plant density should affect soil carbon dioxide (CO2) efflux and carbon cycling in semi-arid regions, the effects of plant density on soil CO2 efflux are not well known. This study was performed to investigate the responses of soil CO2 efflux of two dominant shrubs (Caragana korshinkii and Salix psammophila) to ...

Accelerated Carbonation of Steel Slags Using CO{sub 2} Diluted Sources: CO{sub 2} Uptakes and Energy Requirements

Energy Technology Data Exchange (ETDEWEB)

Baciocchi, Renato, E-mail: baciocchi@ing.uniroma2.it; Costa, Giulia [Department of Civil Engineering and Computer Science Engineering, University of Rome “Tor Vergata”, Rome (Italy); Polettini, Alessandra; Pomi, Raffaella; Stramazzo, Alessio [Department of Civil and Environmental Engineering, University of Rome “La Sapienza”, Rome (Italy); Zingaretti, Daniela [Department of Civil Engineering and Computer Science Engineering, University of Rome “Tor Vergata”, Rome (Italy)

2016-01-18

This work presents the results of carbonation experiments performed on Basic Oxygen Furnace (BOF) steel slag samples employing gas mixtures containing 40 and 10% CO{sub 2} vol. simulating the gaseous effluents of gasification and combustion processes respectively, as well as 100% CO{sub 2} for comparison purposes. Two routes were tested, the slurry-phase (L/S = 5 l/kg, T = 100°C and Ptot = 10 bar) and the thin-film (L/S = 0.3–0.4 l kg, T = 50°C and Ptot = 7–10 bar) routes. For each one, the CO{sub 2} uptake achieved as a function of the reaction time was analyzed and on this basis, the energy requirements associated with each carbonation route and gas mixture composition were estimated considering to store the CO{sub 2} emissions of a medium size natural gas fired power plant (20 MW). For the slurry-phase route, maximum CO{sub 2} uptakes ranged from around 8% at 10% CO{sub 2}, to 21.1% (BOF-a) and 29.2% (BOF-b) at 40% CO{sub 2} and 32.5% (BOF-a) and 40.3% (BOF-b) at 100% CO{sub 2}. For the thin-film route, maximum uptakes of 13% (BOF-c) and 19.5% (BOF-d) at 40% CO{sub 2}, and 17.8% (BOF-c) and 20.2% (BOF-d) at 100% were attained. The energy requirements of the two analyzed process routes appeared to depend chiefly on the CO{sub 2} uptake of the slag. For both process route, the minimum overall energy requirements were found for the tests with 40% CO{sub 2} flows (i.e., 1400−1600 MJ/t{sub CO{sub 2}} for the slurry-phase and 2220 – 2550 MJ/t{sub CO{sub 2}} for the thin-film route).

Cyanobacterial carbon concentrating mechanisms facilitate sustained CO2 depletion in eutrophic lakes

Science.gov (United States)

Morales-Williams, Ana M.; Wanamaker, Alan D., Jr.; Downing, John A.

2017-06-01

Phytoplankton blooms are increasing in frequency, intensity, and duration in aquatic ecosystems worldwide. In many eutrophic lakes, these high levels of primary productivity correspond to periods of CO2 depletion in surface waters. Cyanobacteria and other groups of phytoplankton have the ability to actively transport bicarbonate (HCO3-) across their cell membrane when CO2 concentrations are limiting, possibly giving them a competitive advantage over algae not using carbon concentrating mechanisms (CCMs). To investigate whether CCMs can maintain phytoplankton bloom biomass under CO2 depletion, we measured the δ13C signatures of dissolved inorganic carbon (δ13CDIC) and phytoplankton particulate organic carbon (δ13Cphyto) in 16 mesotrophic to hypereutrophic lakes during the ice-free season of 2012. We used mass-balance relationships to determine the dominant inorganic carbon species used by phytoplankton under CO2 stress. We found a significant positive relationship between phytoplankton biomass and phytoplankton δ13C signatures as well as a significant nonlinear negative relationship between water column ρCO2 and isotopic composition of phytoplankton, indicating a shift from diffusive uptake to active uptake by phytoplankton of CO2 or HCO3- during blooms. Calculated photosynthetic fractionation factors indicated that this shift occurs specifically when surface water CO2 drops below atmospheric equilibrium. Our results indicate that active HCO3- uptake via CCMs may be an important mechanism in maintaining phytoplankton blooms when CO2 is depleted. Further increases in anthropogenic pressure, eutrophication, and cyanobacteria blooms are therefore expected to contribute to increased bicarbonate uptake to sustain primary production.

Cyanobacterial carbon concentrating mechanisms facilitate sustained CO2 depletion in eutrophic lakes

Directory of Open Access Journals (Sweden)

A. M. Morales-Williams

2017-06-01

Full Text Available Phytoplankton blooms are increasing in frequency, intensity, and duration in aquatic ecosystems worldwide. In many eutrophic lakes, these high levels of primary productivity correspond to periods of CO2 depletion in surface waters. Cyanobacteria and other groups of phytoplankton have the ability to actively transport bicarbonate (HCO3− across their cell membrane when CO2 concentrations are limiting, possibly giving them a competitive advantage over algae not using carbon concentrating mechanisms (CCMs. To investigate whether CCMs can maintain phytoplankton bloom biomass under CO2 depletion, we measured the δ13C signatures of dissolved inorganic carbon (δ13CDIC and phytoplankton particulate organic carbon (δ13Cphyto in 16 mesotrophic to hypereutrophic lakes during the ice-free season of 2012. We used mass–balance relationships to determine the dominant inorganic carbon species used by phytoplankton under CO2 stress. We found a significant positive relationship between phytoplankton biomass and phytoplankton δ13C signatures as well as a significant nonlinear negative relationship between water column ρCO2 and isotopic composition of phytoplankton, indicating a shift from diffusive uptake to active uptake by phytoplankton of CO2 or HCO3− during blooms. Calculated photosynthetic fractionation factors indicated that this shift occurs specifically when surface water CO2 drops below atmospheric equilibrium. Our results indicate that active HCO3− uptake via CCMs may be an important mechanism in maintaining phytoplankton blooms when CO2 is depleted. Further increases in anthropogenic pressure, eutrophication, and cyanobacteria blooms are therefore expected to contribute to increased bicarbonate uptake to sustain primary production.

Calcium and chemical looping technology for power generation and carbon dioxide (CO2) capture solid oxygen- and CO2-carriers

CERN Document Server

Fennell, Paul

2015-01-01

Calcium and Chemical Looping Technology for Power Generation and Carbon Dioxide (CO2) Capture reviews the fundamental principles, systems, oxygen carriers, and carbon dioxide carriers relevant to chemical looping and combustion. Chapters review the market development, economics, and deployment of these systems, also providing detailed information on the variety of materials and processes that will help to shape the future of CO2 capture ready power plants. Reviews the fundamental principles, systems, oxygen carriers, and carbon dioxide carriers relevant to calcium and chemical loopingProvi

Ventilation of subterranean CO2 and Eddy covariance incongruities over carbonate ecosystems

Directory of Open Access Journals (Sweden)

F. Domingo

2010-03-01

Full Text Available Measurements of CO2 fluxes with Eddy Covariance (EC systems are ongoing over different ecosystems around the world, through different measuring networks, in order to assess the carbon balance of these ecosystems. In carbonate ecosystems, characterized by the presence of subterranean pores and cavities, ventilation of the CO2 accumulated in these cavities and pores can act as an extra source of CO2 exchange between the ecosystem and the atmosphere. In this work we analyse the effect of the subterranean heterogeneity of a carbonate ecosystem on measurements of CO2 fluxes by comparing measurements from two EC systems with distinct footprints. Results showed that both EC systems agreed for measurements of evapotranspiration and of CO2 in periods when respiratory and photosynthetic processes were dominant (biological periods, with a regression slope of 0.99 and 0.97, respectively. However, in periods when the main source of CO2 comes from the ventilation of subterranean pores and cavities (abiotic periods agreement is not good, with a regression slope of 0.6. Ground-penetrating radar measurements of the sub-surface confirmed the existence of high sub-surface heterogeneity that, combined with different footprints, lead to differences in the measurements of the two EC systems. These results show that measurements of CO2 fluxes with Eddy covariance systems over carbonate ecosystems must be taken carefully, as they may not be representative of the ecosystem under consideration.

CO{sub 2} removal potential of carbons prepared by co-pyrolysis of sugar and nitrogen containing compounds

Energy Technology Data Exchange (ETDEWEB)

Arenillas, A.; Drage, T.C.; Smith, K.; Snape, C.E. [University of Nottingham, Fuel Science Group, School of Chemical, Environmental and Mining Engineering, University Park, Nottingham NG7 2RD (United Kingdom)

2005-08-15

The nitrogen enrichment of active carbons is reported to be effective in enhancing the specific adsorbate-adsorbent interactions for CO{sub 2}. In this work, nitrogen-enriched carbons were prepared by co-pyrolysis of sugar and a series of nitrogen compounds with different nitrogen functionalities. The results show that although the amount of nitrogen incorporated to the final adsorbent is important, the N-functionality seems to be more relevant for increasing CO{sub 2} uptake. Thus, the adsorbent obtained from urea co-pyrolysis presents the highest nitrogen content but the lowest CO{sub 2} adsorption capacity. However, the adsorbent obtained from carbazole co-pyrolysis, despite the lower amount of N incorporated, shows high CO{sub 2} uptake, up to 9wt.%, probably because the presence of more basic functionalities as determined by XPS analysis.

Reconsideration of atmospheric CO2 lifetime: potential mechanism for explaining CO2 missing sink

Science.gov (United States)

Kikuchi, R.; Gorbacheva, T.; Gerardo, R.

2009-04-01

Carbon cycle data (Intergovernmental Panel on Climate Change 1996) indicate that fossil fuel use accounts for emissions to the atmosphere of 5.5±0.5 GtC (Gigatons of carbon) annually. Other important processes in the global CO2 budget are tropical deforestation, estimated to generate about 1.6±1.0 GtC/yr; absorption by the oceans, removing about 2.0±0.8 GtC/yr; and regrowth of northern forests, taking up about 0.5±0.5 GtC/yr. However, accurate measurements of CO2 show that the atmosphere is accumulating only about 3.3±0.2 GtC/yr. The imbalance of about 1.3±1.5 GtC/yr, termed the "missing sink", represents the difference between the estimated sources and the estimated sinks of CO2; that is, we do not know where all of the anthropogenic CO2 is going. Several potential mechanisms have been proposed to explain this missing carbon, such as CO2 fertilization, climate change, nitrogen deposition, land use change, forest regrowth et al. Considering the complexity of ecosystem, most of ecosystem model cannot handle all the potential mechanisms to reproduce the real world. It has been believed that the dominant sink mechanism is the fertilizing effects of increased CO2 concentrations in the atmosphere and the addition to soils of fixed nitrogen from fossil-fuel burning and agricultural fertilizers. However, a recent analysis of long-term observations of the change in biomass and growth rates suggests that such fertilization effects are much too small to explain more than a small fraction of the observed sink. In addition, long-term experiments in which small forest patches and other land ecosystems have been exposed to elevated CO2 levels for extended periods show a rapid decrease of the fertilization effect after an initial enhancement. We will explore this question of the missing sink in atmospheric CO2 residence time. Radioactive and stable carbon isotopes (13-C/12-C) show the real CO2 lifetime is about 5 years; i.e. CO2 is quickly taken out of the atmospheric

Metal-Doped Nitrogenated Carbon as an Efficient Catalyst for Direct CO2 Electroreduction to CO and Hydrocarbons.

Science.gov (United States)

Varela, Ana Sofia; Ranjbar Sahraie, Nastaran; Steinberg, Julian; Ju, Wen; Oh, Hyung-Suk; Strasser, Peter

2015-09-07

This study explores the kinetics, mechanism, and active sites of the CO2 electroreduction reaction (CO2RR) to syngas and hydrocarbons on a class of functionalized solid carbon-based catalysts. Commercial carbon blacks were functionalized with nitrogen and Fe and/or Mn ions using pyrolysis and acid leaching. The resulting solid powder catalysts were found to be active and highly CO selective electrocatalysts in the electroreduction of CO2 to CO/H2 mixtures outperforming a low-area polycrystalline gold benchmark. Unspecific with respect to the nature of the metal, CO production is believed to occur on nitrogen functionalities in competition with hydrogen evolution. Evidence is provided that sufficiently strong interaction between CO and the metal enables the protonation of CO and the formation of hydrocarbons. Our results highlight a promising new class of low-cost, abundant electrocatalysts for synthetic fuel production from CO2 . © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

How can mountaintop CO2 observations be used to constrain regional carbon fluxes?

Science.gov (United States)

Lin, John C.; Mallia, Derek V.; Wu, Dien; Stephens, Britton B.

2017-05-01

Despite the need for researchers to understand terrestrial biospheric carbon fluxes to account for carbon cycle feedbacks and predict future CO2 concentrations, knowledge of these fluxes at the regional scale remains poor. This is particularly true in mountainous areas, where complex meteorology and lack of observations lead to large uncertainties in carbon fluxes. Yet mountainous regions are often where significant forest cover and biomass are found - i.e., areas that have the potential to serve as carbon sinks. As CO2 observations are carried out in mountainous areas, it is imperative that they are properly interpreted to yield information about carbon fluxes. In this paper, we present CO2 observations at three sites in the mountains of the western US, along with atmospheric simulations that attempt to extract information about biospheric carbon fluxes from the CO2 observations, with emphasis on the observed and simulated diurnal cycles of CO2. We show that atmospheric models can systematically simulate the wrong diurnal cycle and significantly misinterpret the CO2 observations, due to erroneous atmospheric flows as a result of terrain that is misrepresented in the model. This problem depends on the selected vertical level in the model and is exacerbated as the spatial resolution is degraded, and our results indicate that a fine grid spacing of ˜ 4 km or less may be needed to simulate a realistic diurnal cycle of CO2 for sites on top of the steep mountains examined here in the American Rockies. In the absence of higher resolution models, we recommend coarse-scale models to focus on assimilating afternoon CO2 observations on mountaintop sites over the continent to avoid misrepresentations of nocturnal transport and influence.

Granular bamboo-derived activated carbon for high CO(2) adsorption: the dominant role of narrow micropores.

Science.gov (United States)

Wei, Haoran; Deng, Shubo; Hu, Bingyin; Chen, Zhenhe; Wang, Bin; Huang, Jun; Yu, Gang

2012-12-01

Cost-effective biomass-derived activated carbons with a high CO(2) adsorption capacity are attractive for carbon capture. Bamboo was found to be a suitable precursor for activated carbon preparation through KOH activation. The bamboo size in the range of 10-200 mesh had little effect on CO(2) adsorption, whereas the KOH/C mass ratio and activation temperature had a significant impact on CO(2) adsorption. The bamboo-derived activated carbon had a high adsorption capacity and excellent selectivity for CO(2) , and also the adsorption process was highly reversible. The adsorbed amount of CO(2) on the granular activated carbon was up to 7.0 mmol g(-1) at 273 K and 1 bar, which was higher than almost all carbon materials. The pore characteristics of activated carbons responsible for high CO(2) adsorption were fully investigated. Based on the analysis of narrow micropore size distribution of several activated carbons prepared under different conditions, a more accurate micropore range contributing to CO(2) adsorption was proposed. The volume of micropores in the range of 0.33-0.82 nm had a good linear relationship with CO(2) adsorption at 273 K and 1 bar, and the narrow micropores of about 0.55 nm produced the major contribution, which could be used to evaluate CO(2) adsorption on activated carbons. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Simplified models of rates of CO2 mineralization in Geologic Carbon Storage

Science.gov (United States)

DePaolo, D. J.; Zhang, S.

2017-12-01

Geologic carbon storage (GCS) reverses the flow of carbon to the atmosphere, returning the carbon to long-term geologic storage. Models suggest that most of the injected CO2 will be "trapped" in the subsurface by physical means, but the most risk-free and permanent form of carbon storage is as carbonate minerals (Ca,Mg,Fe)CO3. The transformation of CO2 to carbonate minerals requires supply of divalent cations by dissolution of silicate minerals. Available data suggest that rates of transformation are difficult to predict. We show that the chemical kinetic observations and experimental results, when reduced to a single timescale that describes the fractional rate at which cations are released to solution by mineral dissolution, show sufficiently systematic behavior that the rates of mineralization can be estimated with reasonable certainty. Rate of mineralization depends on both the abundance (determined by the reservoir rock mineralogy) and the rate at which cations are released by dissolution into pore fluid that has been acidified with dissolved CO2. Laboratory-measured rates and field observations give values spanning 8 to 10 orders of magnitude, but when evaluated in the context of reservoir-scale reactive transport simulations, this range becomes much smaller. Reservoir scale simulations indicate that silicate mineral dissolution and subsequent carbonate mineral precipitation occur at pH 4.5 to 6, fluid flow velocity less than 5m/yr, and 50-100 years or more after the start of injection. These constraints lead to estimates of 200 to 2000 years for conversion of 60-90% of injected CO2 when the reservoir rock has a sufficient volume fraction of divalent cation-bearing silicate minerals (ca. 20%), and confirms that when reservoir rock mineralogy is not favorable the fraction of CO2 converted to carbonate minerals is minimal over 104 years. A sufficient amount of reactive minerals represents the condition by which the available cations per volume of rock plus pore

A TPD-MS study of glassy carbon surfaces oxidized by CO2 and O2

Directory of Open Access Journals (Sweden)

MILA D. LAUSEVIC

2002-11-01

Full Text Available The temperature-programmed desorption (TPD method combined with mass spectrometric (MS analysis has been applied to investigate the surface properties of carbon materials. The apparatus consisting of a temperature-programmed furnace and a quadrupole mass spectrometer was constructed in order to characterize the surface of differently treated glassy carbon samples. In this work, samples of glassy carbon exposed to air, CO2 and O2 were examined. The desorption of H2O, CO and CO2, as major products, indicated the presence of different oxide groups. The amount of these groups for all samples was calculated. It is concluded that oxidation affects the nature and the amount of the surface oxide groups and contributes to their increased stability.

Determination of free CO2 in emergent groundwaters using a commercial beverage carbonation meter

Science.gov (United States)

Vesper, Dorothy J.; Edenborn, Harry M.

2012-05-01

SummaryDissolved CO2 in groundwater is frequently supersaturated relative to its equilibrium with atmospheric partial pressure and will degas when it is conveyed to the surface. Estimates of dissolved CO2 concentrations can vary widely between different hydrochemical facies because they have different sources of error (e.g., rapid degassing, low alkalinity, non-carbonate alkalinity). We sampled 60 natural spring and mine waters using a beverage industry carbonation meter, which measures dissolved CO2 based on temperature and pressure changes as the sample volume is expanded. Using a modified field protocol, the meter was found to be highly accurate in the range 0.2-35 mM CO2. The meter provided rapid, accurate and precise measurements of dissolved CO2 in natural waters for a range of hydrochemical facies. Dissolved CO2 concentrations measured in the field with the carbonation meter were similar to CO2 determined using the pH-alkalinity approach, but provided immediate results and avoided errors from alkalinity and pH determination. The portability and ease of use of the carbonation meter in the field made it well-suited to sampling in difficult terrain. The carbonation meter has proven useful in the study of aquatic systems where CO2 degassing drives geochemical changes that result in surficial mineral precipitation and deposition, such as tufa, travertine and mine drainage deposits.

CO2 Absorption and Magnesium Carbonate Precipitation in MgCl2–NH3–NH4Cl Solutions: Implications for Carbon Capture and Storage

Directory of Open Access Journals (Sweden)

Chen Zhu

2017-09-01

Full Text Available CO2 absorption and carbonate precipitation are the two core processes controlling the reaction rate and path of CO2 mineral sequestration. Whereas previous studies have focused on testing reactive crystallization and precipitation kinetics, much less attention has been paid to absorption, the key process determining the removal efficiency of CO2. In this study, adopting a novel wetted wall column reactor, we systematically explore the rates and mechanisms of carbon transformation from CO2 gas to carbonates in MgCl2–NH3–NH4Cl solutions. We find that reactive diffusion in liquid film of the wetted wall column is the rate-limiting step of CO2 absorption when proceeding chiefly through interactions between CO2(aq and NH3(aq. We further quantified the reaction kinetic constant of the CO2–NH3 reaction. Our results indicate that higher initial concentration of NH4Cl ( ≥ 2 mol · L − 1 leads to the precipitation of roguinite [ ( NH 4 2 Mg ( CO 3 2 · 4 H 2 O ], while nesquehonite appears to be the dominant Mg-carbonate without NH4Cl addition. We also noticed dypingite formation via phase transformation in hot water. This study provides new insight into the reaction kinetics of CO2 mineral carbonation that indicates the potential of this technique for future application to industrial-scale CO2 sequestration.

Comparative study of CO2 and H2O activation in the synthesis of carbon electrode for supercapacitors

Science.gov (United States)

Taer, E.; Apriwandi, Yusriwandi, Mustika, W. S.; Zulkifli, Taslim, R.; Sugianto, Kurniasih, B.; Agustino, Dewi, P.

2018-02-01

The physical activation for the comparative study of carbon electrode synthesized for supercapacitor applications made from rubber wood sawdust has been performed successfully. Comparison of physical activation used in this research is based on the different gas activation such as CO2 and H2O. The CO2 and H2O activation are made by using an integrated carbonization and activation system. The carbonization process is performed in N2 atmosphere followed by CO2 and H2O activation process. The carbonization process at temperature of 600°C, the CO2 and H2O activation process at a temperature of 900°C and maintained at this condition for 2 h and 3 h. The electrochemical properties were analyzed using cyclic voltammetric (CV) method. The CV results show that the carbon electrode with CO2 activation has better capacitive properties than H2O, the highest specific capacitance obtained is 93.22 F/g for 3 h of activation time. In addition, the analysis of physical properties such as surface morphology and degree of crystallinity was also performed.

Carbon isotope exchange between gaseous CO2 and thin solution films: Artificial cave experiments and a complete diffusion-reaction model

Science.gov (United States)

Hansen, Maximilian; Scholz, Denis; Froeschmann, Marie-Louise; Schöne, Bernd R.; Spötl, Christoph

2017-08-01

Speleothem stable carbon isotope (δ13C) records provide important paleoclimate and paleo-environmental information. However, the interpretation of these records in terms of past climate or environmental change remains challenging because of various processes affecting the δ13C signals. A process that has only been sparsely discussed so far is carbon isotope exchange between the gaseous CO2 of the cave atmosphere and the dissolved inorganic carbon (DIC) contained in the thin solution film on the speleothem, which may be particularly important for strongly ventilated caves. Here we present a novel, complete reaction diffusion model describing carbon isotope exchange between gaseous CO2 and the DIC in thin solution films. The model considers all parameters affecting carbon isotope exchange, such as diffusion into, out of and within the film, the chemical reactions occurring within the film as well as the dependence of diffusion and the reaction rates on isotopic mass and temperature. To verify the model, we conducted laboratory experiments under completely controlled, cave-analogue conditions at three different temperatures (10, 20, 30 °C). We exposed thin (≈0.1 mm) films of a NaHCO3 solution with four different concentrations (1, 2, 5 and 10 mmol/l, respectively) to a nitrogen atmosphere containing a specific amount of CO2 (1000 and 3000 ppmV). The experimentally observed temporal evolution of the pH and δ13C values of the DIC is in good agreement with the model predictions. The carbon isotope exchange times in our experiments range from ca. 200 to ca. 16,000 s and strongly depend on temperature, film thickness, atmospheric pCO2 and the concentration of DIC. For low pCO2 (between 500 and 1000 ppmV, as for strongly ventilated caves), our time constants are substantially lower than those derived in a previous study, suggesting a potentially stronger influence of carbon isotope exchange on speleothem δ13C values. However, this process should only have an

Novel porous carbon materials with ultrahigh nitrogen contents for selective CO 2 capture

KAUST Repository

Zhao, Yunfeng; Zhao, Lan; Yao, Kexin; Yang, Yang; Zhang, Qiang; Han, Yu

2012-01-01

Nitrogen-doped carbon materials were prepared by a nanocasting route using tri-continuous mesoporous silica IBN-9 as a hard template. Rationally choosing carbon precursors and carefully controlling activation conditions result in an optimized material denoted as IBN9-NC1-A, which possesses a very high nitrogen doping concentration (∼13 wt%) and a large surface area of 890 m 2 g -1 arising from micropores (<1 nm). It exhibits an excellent performance for CO 2 adsorption over a wide range of CO 2 pressures. Specifically, its equilibrium CO 2 adsorption capacity at 25 °C reaches up to 4.50 mmol g -1 at 1 bar and 10.53 mmol g -1 at 8 bar. In particular, it shows a much higher CO 2 uptake at low pressure (e.g. 1.75 mmol g -1 at 25 °C and 0.2 bar) than any reported carbon-based materials, owing to its unprecedented nitrogen doping level. The high nitrogen contents also give rise to significantly enhanced CO 2/N 2 selectivities (up to 42), which combined with the high adsorption capacities, make these new carbon materials promising sorbents for selective CO 2 capture from power plant flue gas and other relevant applications. © 2012 The Royal Society of Chemistry.

Porous carbon from local coconut shell char by CO2 and H2O activation in the presence of K2CO3

Science.gov (United States)

Vi, Nguyen Ngoc Thuy; Truyen, Dang Hai; Trung, Bien Cong; An, Ngo Thanh; Van Dung, Nguyen; Long, Nguyen Quang

2017-09-01

Vietnamese coconut shell char was activated by steam and carbon dioxide at low temperatures with the presence of K2CO3 as a catalyst. The effects of process parameters on adsorption capability of the product including different ratio of impregnation of activation agents, activation temperature, activation time were investigated in this study. Iodine number, methylene blue adsorption capacity, specific surface area and pore size distribution were measured to assess the properties of the activated carbon. Accordingly, the porous carbon was applied for toluene removal by adsorption technology. Significant increases in specific surface area and the toluene adsorption capacity were observed when the coconut shell char was activated in CO2 flow at 720 °C for 150 minutes and the K2CO3/char weight ratio of 0.5.

Atmospheric deposition, CO2, and change in the land carbon sink

DEFF Research Database (Denmark)

Martinez-Fernandez, Cristina; Vicca, Sara; Janssens, Ivan A.

2017-01-01

Concentrations of atmospheric carbon dioxide (CO2) have continued to increase whereas atmospheric deposition of sulphur and nitrogen has declined in Europe and the USA during recent decades. Using time series of flux observations from 23 forests distributed throughout Europe and the USA, and gene...... show the need to include the effects of changing atmospheric composition, beyond CO2, to assess future dynamics of carbon-climate feedbacks not currently considered in earth system/climate modelling....

Dynamics of riverine CO2 in the Yangtze River fluvial network and their implications for carbon evasion

Science.gov (United States)

Ran, Lishan; Lu, Xi Xi; Liu, Shaoda

2017-04-01

Understanding riverine carbon dynamics is critical for not only better estimates of various carbon fluxes but also evaluating their significance in the global carbon budget. As an important pathway of global land-ocean carbon exchange, the Yangtze River has received less attention regarding its vertical carbon evasion compared with lateral transport. Using long-term water chemistry data, we calculated CO2 partial pressure (pCO2) from pH and alkalinity and examined its spatial and temporal dynamics and the impacts of environmental settings. With alkalinity ranging from 415 to > 3400 µeq L-1, the river waters were supersaturated with dissolved CO2, generally 2-20-fold the atmospheric equilibrium (i.e., 390 µatm). Changes in pCO2 were collectively controlled by carbon inputs from terrestrial ecosystems, hydrological regime, and rock weathering. High pCO2 values were observed spatially in catchments with abundant carbonate presence and seasonally in the wet season when recently fixed organic matter was exported into the river network. In-stream processing of organic matter facilitated CO2 production and sustained the high pCO2, although the alkalinity presented an apparent dilution effect with water discharge. The decreasing pCO2 from the smallest headwater streams through tributaries to the mainstem channel illustrates the significance of direct terrestrial carbon inputs in controlling riverine CO2. With a basin-wide mean pCO2 of 2662 ± 1240 µatm, substantial CO2 evasion from the Yangtze River fluvial network is expected. Future research efforts are needed to quantify the amount of CO2 evasion and assess its biogeochemical implications for watershed-scale carbon cycle. In view of the Yangtze River's relative importance in global carbon export, its CO2 evasion would be significant for global carbon budget.

CO2-laser decomposition method of carbonate for AMS 14C measurements

International Nuclear Information System (INIS)

Kitagawa, Hiroyuki

2013-01-01

A CO 2 laser decomposition method enabled the efficient preparation of carbonate samples for AMS 14 C measurement. Samples were loaded in a vacuum chamber and thermally decomposed using laser emission. CO 2 liberated from the carbonate was directly trapped in the cold finger trap of a small CO 2 reduction reactor and graphitized by a hydrogen gas reduction method using catalytic iron powder. The fraction modern values for 0.07–0.57 mg of carbon, obtained from 200 μm-diameter spots of IAEA-C1, varied with sample size in the range of 0.00072 ± 0.00003 to 0.00615 ± 0.00052. The contamination induced by the laser decomposition method and the following graphite handling was estimated to be 0.53 ± 0.21 μg of modern carbon, assuming a constant amount of extraneous carbon contamination. This method could also make it possible to avoid the time-consuming procedures of the conventional acid dissolution method that involves multiple complex steps for the preparation of carbonate samples.

Modeling CO2-Water-Mineral Wettability and Mineralization for Carbon Geosequestration.

Science.gov (United States)

Liang, Yunfeng; Tsuji, Shinya; Jia, Jihui; Tsuji, Takeshi; Matsuoka, Toshifumi

2017-07-18

Carbon dioxide (CO 2 ) capture and storage (CCS) is an important climate change mitigation option along with improved energy efficiency, renewable energy, and nuclear energy. CO 2 geosequestration, that is, to store CO 2 under the subsurface of Earth, is feasible because the world's sedimentary basins have high capacity and are often located in the same region of the world as emission sources. How CO 2 interacts with the connate water and minerals is the focus of this Account. There are four trapping mechanisms that keep CO 2 in the pores of subsurface rocks: (1) structural trapping, (2) residual trapping, (3) dissolution trapping, and (4) mineral trapping. The first two are dominated by capillary action, where wettability controls CO 2 and water two-phase flow in porous media. We review state-of-the-art studies on CO 2 /water/mineral wettability, which was found to depend on pressure and temperature conditions, salt concentration in aqueous solutions, mineral surface chemistry, and geometry. We then review some recent advances in mineral trapping. First, we show that it is possible to reproduce the CO 2 /water/mineral wettability at a wide range of pressures using molecular dynamics (MD) simulations. As the pressure increases, CO 2 gas transforms into a supercritical fluid or liquid at ∼7.4 MPa depending on the environmental temperature. This transition leads to a substantial decrease of the interfacial tension between CO 2 and reservoir brine (or pure water). However, the wettability of CO 2 /water/rock systems depends on the type of rock surface. Recently, we investigated the contact angle of CO 2 /water/silica systems with two different silica surfaces using MD simulations. We found that contact angle increased with pressure for the hydrophobic (siloxane) surface while it was almost constant for the hydrophilic (silanol) surface, in excellent agreement with experimental observations. Furthermore, we found that the CO 2 thin films at the CO 2 -hydrophilic

Carbon-14 immobilization via the CO2-Ba(OH)2 hydrate gas-solid reaction

International Nuclear Information System (INIS)

Haag, G.L.

1980-01-01

Although no restrictions have been placed on the release of carbon-14, it has been identified as a potential health hazard due to the ease in which it may be assimilated into the biosphere. The intent of the Carbon-14 Immobilization Program, funded through the Airborne Waste Program Management Office, is to develop and demonstrate a novel process for restricting off-gas releases of carbon-14 from various nuclear facilities. The process utilizes the CO 2 -Ba(OH) 2 hydrate gas-solid reaction to directly remove and immobilize carbon-14. The reaction product, BaCO 3 , possesses both the thermal and chemical stability desired for long-term waste disposal. The process is capable of providing decontamination factors in excess of 1000 and reactant utilization of greater than 99% in the treatment of high volumetric, airlike (330 ppM CO 2 ) gas streams. For the treatment of an air-based off-gas stream, the use of packed beds of Ba(OH) 2 .8H 2 O flakes to remove CO 2 has been demonstrated. However, the operating conditions must be maintained between certain upper and lower limits with respect to the partial pressure of water. If the water vapor pressure in the gas is less than the dissociation vapor pressure of Ba(OH) 2 .8H 2 O, the bed will deactivate. If the vapor pressure is considerably greater, pressure drop problems will increase with increasing humidity as the particles curl and degrade. Results have indicated that when operated in the proper regime, the bulk of the increase in pressure drop results from the conversion of Ba(OH) 2 .8H 2 O to BaCO 3 and not from the hydration of the commercial Ba(OH) 2 .8H 2 O (i.e. Ba(OH) 2 .7.50H 2 O) to Ba(OH) 2 .8H 2 O

Reducing CO2 emissions on the electric grid through a carbon disincentive policy

International Nuclear Information System (INIS)

Li, Chiao-Ting; Peng, Huei; Sun, Jing

2013-01-01

This paper studies the operation of an electric grid with renewable wind generation and plug-in electric vehicles (PEVs). In particular, PEVs will be the controllable demand that can mitigate the intermittency in wind generation and improve the capacity factors of the non-renewable generation assets on the grid. Optimization problems are formulated to minimize the costs of electricity generation, and two approaches are proposed to address the grid CO 2 emission in the optimization. The first approach directly penalizes CO 2 in the objective function, and the second approach adopts a carbon disincentive policy to alter the dispatch order of power plants, so that expensive low-CO 2 plants can replace cheap high-CO 2 plants. These two approaches result in very different outcomes: the first approach affects only the PEV charging demand on the grid and does not result in significant CO 2 reduction, whereas the second approach controls both the generation and load, and CO 2 can be reduced substantially. In addition, the carbon disincentive policy, unlike a carbon tax, does not collect any revenue; therefore, the increase in electricity cost is minimal. The effect of the proposed algorithms on the grid electricity cost and carbon emission is analyzed in details and reported. - Highlights: • We study the tradeoff between CO 2 emissions and generation cost on an electric grid. • The tradeoff was shown by Pareto fronts obtained from optimizations. • Pareto fronts shows that a carbon disincentive is effective in reducing emissions. • Controlling both supply and demand on the grid is necessary to reduce CO 2 and costs

Dependency of climate change and carbon cycle on CO2 emission pathways

International Nuclear Information System (INIS)

Nohara, Daisuke; Yoshida, Yoshikatsu; Misumi, Kazuhiro; Ohba, Masamichi

2013-01-01

Previous research has indicated that the response of globally average temperature is approximately proportional to cumulative CO 2 emissions, yet evidence of the robustness of this relationship over a range of CO 2 emission pathways is lacking. To address this, we evaluate the dependency of climate and carbon cycle change on CO 2 emission pathways using a fully coupled climate–carbon cycle model. We design five idealized pathways (including an overshoot scenario for cumulative emissions), each of which levels off to final cumulative emissions of 2000 GtC. The cumulative emissions of the overshoot scenario reach 4000 GtC temporarily, subsequently reducing to 2000 GtC as a result of continuous negative emissions. Although we find that responses of climatic variables and the carbon cycle are largely independent of emission pathways, a much weakened Atlantic meridional overturning circulation (AMOC) is projected in the overshoot scenario despite cessation of emissions. This weakened AMOC is enhanced by rapid warming in the Arctic region due to considerable temporary elevation of atmospheric CO 2 concentration and induces the decline of surface air temperature and decrease of precipitation over the northern Atlantic and Europe region. Moreover, the weakened AMOC reduces CO 2 uptake by the Atlantic and Arctic oceans. However, the weakened AMOC contributes little to the global carbon cycle. In conclusion, although climate variations have been found to be dependent on emission pathways, the global carbon cycle is relatively independent of these emission pathways, at least superficially. (letter)

First identification and thermodynamic characterization of the ternary U(VI) species, UO2(O2)(CO3)2(4-), in UO2-H2O2-K2CO3 solutions.

Science.gov (United States)

Goff, George S; Brodnax, Lia F; Cisneros, Michael R; Peper, Shane M; Field, Stephanie E; Scott, Brian L; Runde, Wolfgang H

2008-03-17

In alkaline carbonate solutions, hydrogen peroxide can selectively replace one of the carbonate ligands in UO2(CO3)3(4-) to form the ternary mixed U(VI) peroxo-carbonato species UO2(O2)(CO3)2(4-). Orange rectangular plates of K4[UO2(CO3)2(O2)].H2O were isolated and characterized by single crystal X-ray diffraction studies. Crystallographic data: monoclinic, space group P2(1)/ n, a = 6.9670(14) A, b = 9.2158(10) A, c = 18.052(4) A, Z = 4. Spectrophotometric titrations with H 2O 2 were performed in 0.5 M K 2CO 3, with UO2(O2)(CO3)2(4-) concentrations ranging from 0.1 to 0.55 mM. The molar absorptivities (M(-1) cm(-1)) for UO2(CO3)3(4-) and UO2(O2)(CO3)2(4-) were determined to be 23.3 +/- 0.3 at 448.5 nm and 1022.7 +/- 19.0 at 347.5 nm, respectively. Stoichiometric analyses coupled with spectroscopic comparisons between solution and solid state indicate that the stable solution species is UO2(O2)(CO3)2(4-), which has an apparent formation constant of log K' = 4.70 +/- 0.02 relative to the tris-carbonato complex.

Transcriptome-based analysis on carbon metabolism of Haematococcus pluvialis mutant under 15% CO2.

Science.gov (United States)

Li, Ke; Cheng, Jun; Lu, Hongxiang; Yang, Weijuan; Zhou, Junhu; Cen, Kefa

2017-06-01

To elucidate the mechanism underlying the enhanced growth rate in the Haematococcus pluvialis mutated with 60 Co-γ rays and domesticated with 15% CO 2 , transcriptome sequencing was conducted to clarify the carbon metabolic pathways of mutant cells. The CO 2 fixation rate of mutant cells increased to 2.57gL -1 d -1 under 15% CO 2 due to the enhanced photosynthesis, carbon fixation, glycolysis pathways. The upregulation of PetH, ATPF0A and PetJ related to photosynthetic electron transport, ATP synthase and NADPH generation promoted the photosynthesis. The upregulation of genes related to Calvin cycle and ppdK promoted carbon fixation in both C3 and C4 photosynthetic pathways. The reallocation of carbon was also enhanced under 15% CO 2 . The 19-, 14- and 3.5-fold upregulation of FBA, TPI and PK genes, respectively, remarkably promoted the glycolysis pathways. This accelerated the conversion of photosynthetic carbon to pyruvate, which was an essential precursor for astaxanthin and lipids biosynthesis. Copyright © 2017 Elsevier Ltd. All rights reserved.

Deep ocean ventilation, carbon isotopes, marine sedimentation and the deglacial CO2 rise

Directory of Open Access Journals (Sweden)

C. Heinze

2011-07-01

Full Text Available The link between the atmospheric CO2 level and the ventilation state of the deep ocean is an important building block of the key hypotheses put forth to explain glacial-interglacial CO2 fluctuations. In this study, we systematically examine the sensitivity of atmospheric CO2 and its carbon isotope composition to changes in deep ocean ventilation, the ocean carbon pumps, and sediment formation in a global 3-D ocean-sediment carbon cycle model. Our results provide support for the hypothesis that a break up of Southern Ocean stratification and invigorated deep ocean ventilation were the dominant drivers for the early deglacial CO2 rise of ~35 ppm between the Last Glacial Maximum and 14.6 ka BP. Another rise of 10 ppm until the end of the Holocene is attributed to carbonate compensation responding to the early deglacial change in ocean circulation. Our reasoning is based on a multi-proxy analysis which indicates that an acceleration of deep ocean ventilation during early deglaciation is not only consistent with recorded atmospheric CO2 but also with the reconstructed opal sedimentation peak in the Southern Ocean at around 16 ka BP, the record of atmospheric δ13CCO2, and the reconstructed changes in the Pacific CaCO3 saturation horizon.

Evaluation of ammonia modified and conventionally activated biomass based carbons as CO2 adsorbents in postcombustion conditions

OpenAIRE

González Plaza, Marta; García López, Susana; Rubiera González, Fernando; Pis Martínez, José Juan; Pevida García, Covadonga

2011-01-01

Low cost carbons obtained from biomass residues, olive stones and almond shells, were evaluated as CO2 adsorbents in postcombustion conditions (low CO2 partial pressure). These carbons were prepared from biomass chars by means of two different methods: physical activation with CO2 and amination. All the prepared carbons present a high CO2 adsorption capacity at 303 K, although carbons developed from almond shells show a superior CO2/N2 selectivity (lower N2 adsorption) than those obtained fro...

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

Energy Technology Data Exchange (ETDEWEB)

Verba, Circe A; O& #x27; Connor, William K.; Ideker, J.H.

2012-10-28

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

Biomass waste carbon materials as adsorbents for CO2 capture under post-combustion conditions

Directory of Open Access Journals (Sweden)

Elisa M Calvo-Muñoz

2016-05-01

Full Text Available A series of porous carbon materials obtained from biomass waste have been synthesized, with different morphologies and structural properties, and evaluated as potential adsorbents for CO2 capture in post-combustion conditions. These carbon materials present CO2 adsorption capacities, at 25 ºC and 101.3 kPa, comparable to those obtained by other complex carbon or inorganic materials. Furthermore, CO2 uptakes under these conditions can be well correlated to the narrow micropore volume, derived from the CO2 adsorption data at 0 ºC (VDRCO2. In contrast, CO2 adsorption capacities at 25 ºC and 15 kPa are more related to only pores of sizes lower than 0.7 nm. The capacity values obtained in column adsorption experiments were really promising. An activated carbon fiber obtained from Alcell lignin, FCL, presented a capacity value of 1.3 mmol/g (5.7 %wt. Moreover, the adsorption capacity of this carbon fiber was totally recovered in a very fast desorption cycle at the same operation temperature and total pressure and, therefore, without any additional energy requirement. Thus, these results suggest that the biomass waste used in this work could be successfully valorized as efficient CO2 adsorbent, under post-combustion conditions, showing excellent regeneration performance.

CO{sub 2} capture behavior of shell during calcination/carbonation cycles

Energy Technology Data Exchange (ETDEWEB)

Li, Y.J.; Zhao, C.S.; Chen, H.C.; Duan, L.B.; Chen, X.P. [School of Energy and Environment, Southeast University, Nanjing (China)

2009-08-15

The cyclic carbonation performances of shells as CO{sub 2} sorbents were investigated during multiple calcination/carbonation cycles. The carbonation kinetics of the shell and limestone are similar since they both exhibit a fast kinetically controlled reaction regime and a diffusion controlled reaction regime, but their carbonation rates differ between these two regions. Shell achieves the maximum carbonation conversion for carbonation at 680-700 C. The mactra veneriformis shell and mussel shell exhibit higher carbonation conversions than limestone after several cycles at the same reaction conditions. The carbonation conversion of scallop shell is slightly higher than that of limestone after a series of cycles. The calcined shell appears more porous than calcined limestone, and possesses more pores >230 nm, which allow large CO{sub 2} diffusion-carbonation reaction rates and higher conversion due to the increased surface area of the shell. The pores of the shell that are greater than 230 nm do not sinter significantly. The shell has more sodium ions than limestone, which probably leads to an improvement in the cyclic carbonation performance during the multiple calcination/carbonation cycles. (Abstract Copyright [2009], Wiley Periodicals, Inc.)

Stable Carbon Isotope Characterization of CO2 Loss in Acid Mine Drainage Impacted Stream Water: Observations from a Laboratory Experiment

Science.gov (United States)

Ali, H. N.; Atekwana, E. A.

2007-05-01

Water from an acid mine drainage spring, ground water from a mine tailings pile, stream water and tap water were acidified to simulate acid mine drainage (AMD) contamination. The objective was to determine how acidification of stream water by AMD affected DIC loss and carbon isotope fraction. Two 20 L HDP containers (reactors) containing samples from each source were left un-acidified and allowed to evolve under ambient conditions for several weeks in the laboratory and two others were acidified. Acidification was carried out progressively with sulfuric acid to pH <3. For acidified samples, one reactor was acidified open to the atmosphere and the other closed from contact with atmosphere and CO2(g) was collected under vacuum. The un-acidified samples did not show significant alkalinity and DIC loss, and the 13C of DIC was enriched with time. The acidified samples showed decrease in alkalinity and DIC and increase in the 13C of DIC and CO2(g) with progressive acidification. The enrichment of 13C of DIC for un-acidified samples was due to exchange with atmospheric CO2. On the other hand, the 13C enrichment in the acidified samples was due to fractionation during dehydration of HCO3- and diffusive loss of CO2(g) from the aqueous phase. The actual values measured depended on the amount of CO2 lost from the aqueous phase during acidification. Samples with greater CO2 loss (closed acidification) had greater 13C enrichment. Beyond the HCO3- titration end point, the δ13C of DIC and CO2(g) was similar and nearly constant. The result of this study suggests that AMD effects on DIC can be modeled as a first order kinetic reaction and the isotope enrichment modeled using Rayleigh distillation.

Carbon Deposition during CO2 Electrolysis in Ni-Based Solid-Oxide-Cell Electrodes

DEFF Research Database (Denmark)

Skafte, Theis Løye; Graves, Christopher R.; Blennow, P.

2015-01-01

. Electrochemical impedance spectroscopy in both H2/H2O and CO/CO2 revealed an increase in resistance of the fuel electrode after each CO2 electrolysis current-voltage curve, indicating possible carbon deposition. The difference in partial oxygen pressure between inlet and outlet was analyzed to verify carbon...... in detail. In an attempt to mitigate the degradation due to carbon deposition, the Ni-YSZ electrode was infiltrated with a gadolinium doped ceria (CGO) solution. Initial results indicate that the coking tolerance was not enhanced, but it is still unclear whether infiltrated cells degrade less. However......, infiltrated cells display a significant performance enhancement before coking, especially under electrolysis current. The investigation thus indicated carbon formation in the Ni containing fuel electrode before the thermodynamically calculated threshold for average measurements of the cell was reached...

Study on CO{sub 2} absorption enhancement by adding active carbon particles into MEA solution

Energy Technology Data Exchange (ETDEWEB)

Qian, Juan; Sun, Rui; Ma, Lian; Sun, Shaozeng [Harbin Institute of Technology, Harbin (China). School of Energy Science and Engineering

2013-07-01

The chemical absorption of CO{sub 2} is generally recognized as the most efficient post-combustion technology of CO{sub 2} separation at present. A study on CO{sub 2} absorption enhancement by adding small particles of active carbon into MEA solution is investigated within a self-designed glass stirring tank. Experiments of different particle loadings and different particle sizes have been conducted. When active carbon particle concentration is fewer, compared to the absorption rate of CO{sub 2} gas absorbed by MEA aqueous solution, the role of active carbon adsorption CO{sub 2} gas is negligible. The enhancement efficiency of CO{sub 2} absorption could be improved by 10% to the upmost in this liquid-particle system.

Atomic carbon emission from photodissociation of CO2. [planetary atmospheric chemistry

Science.gov (United States)

Wu, C. Y. R.; Phillips, E.; Lee, L. C.; Judge, D. L.

1978-01-01

Atomic carbon fluorescence, C I 1561, 1657, and 1931 A, has been observed from photodissociation of CO2, and the production cross sections have been measured. A line emission source provided the primary photons at wavelengths from threshold to 420 A. The present results suggest that the excited carbon atoms are produced by total dissociation of CO2 into three atoms. The cross sections for producing the O I 1304-A fluorescence through photodissociation of CO2 are found to be less than 0.01 Mb in the wavelength region from 420 to 835 A. The present data have implications with respect to photochemical processes in the atmospheres of Mars and Venus.

Mimic Carbonic Anhydrase Using Metal-Organic Frameworks for CO2 Capture and Conversion.

Science.gov (United States)

Jin, Chaonan; Zhang, Sainan; Zhang, Zhenjie; Chen, Yao

2018-02-19

Carbonic anhydrase (CA) is a zinc-containing metalloprotein, in which the Zn active center plays the key role to transform CO 2 into carbonate. Inspired by nature, herein we used metal-organic frameworks (MOFs) to mimic CA for CO 2 conversion, on the basis of the structural similarity between the Zn coordination in MOFs and CA active center. The biomimetic activity of MOFs was investigated by detecting the hydrolysis of para-nitrophenyl acetate, which is a model reaction used to evaluate CA activity. The biomimetic materials (e.g., CFA-1) showed good catalytic activity, and excellent reusability, and solvent and thermal stability, which is very important for practical applications. In addition, ZIF-100 and CFA-1 were used to mimic CA to convert CO 2 gas, and exhibited good efficiency on CO 2 conversion compared with those of other porous materials (e.g., MCM-41, active carbon). This biomimetic study revealed a novel CO 2 treatment method. Instead of simply using MOFs to absorb CO 2 , ZIF-100 and CFA-1 were used to mimic CA for in situ CO 2 conversion, which provides a new prospect in the biological and industrial applications of MOFs.

Whole-body CO2 production as an index of the metabolic response to sepsis

Science.gov (United States)

Whole-body carbon dioxide (CO2) production (RaCO2) is an index of substrate oxidation and energy expenditure; therefore, it may provide information about the metabolic response to sepsis. Using stable isotope techniques, we determined RaCO2 and its relationship to protein and glucose metabolism in m...

Stable isotope composition of atmospheric carbon monoxide. A modelling study

International Nuclear Information System (INIS)

Gromov, Sergey S.

2014-01-01

This study aims at an improved understanding of the stable carbon and oxygen isotope composition of the carbon monoxide (CO) in the global atmosphere by means of numerical simulations. At first, a new kinetic chemistry tagging technique for the most complete parameterisation of isotope effects has been introduced into the Modular Earth Submodel System (MESSy) framework. Incorporated into the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model, an explicit treatment of the isotope effects on the global scale is now possible. The expanded model system has been applied to simulate the chemical system containing up to five isotopologues of all carbon- and oxygen-bearing species, which ultimately determine the δ 13 C, δ 18 O and Δ 17 O isotopic signatures of atmospheric CO. As model input, a new stable isotope-inclusive emission inventory for the relevant trace gases has been compiled. The uncertainties of the emission estimates and of the resulting simulated mixing and isotope ratios have been analysed. The simulated CO mixing and stable isotope ratios have been compared to in-situ measurements from ground-based observatories and from the civil-aircraft-mounted CARIBIC-1 measurement platform. The systematically underestimated 13 CO/ 12 CO ratios of earlier, simplified modelling studies can now be partly explained. The EMAC simulations do not support the inferences of those studies, which suggest for CO a reduced input of the highly depleted in 13 C methane oxidation source. In particular, a high average yield of 0.94 CO per reacted methane (CH 4 ) molecule is simulated in the troposphere, to a large extent due to the competition between the deposition and convective transport processes affecting the CH 4 to CO reaction chain intermediates. None of the other factors, assumed or disregarded in previous studies, however hypothesised to have the potential in enriching tropospheric CO in 13 C, were found significant when explicitly simulated. The

Degradation of solid oxide cells during co-electrolysis of H2O and CO2: Carbon deposition under high current densities

DEFF Research Database (Denmark)

Tao, Youkun; Ebbesen, Sune Dalgaard; Mogensen, Mogens Bjerg

2012-01-01

conversions of the reactants were no more than 66.8 %. Ni-YSZ electrode delamination and carbon nano-fibers could be observed after test at the Ni-YSZ | YSZ electrolyte interface for two of the cells. Thermodynamic calculation shows that the reactant conversion needed for carbon formation is above 99 %, far...... above the experimental conversions. The observed carbon formation may be caused by the gas diffusion limitations at high current densities. Carbon nano-fibers were only observed close to the YSZ electrolyte indicating a large overpotential gradient at the TPBs close to the electrolyte......During co-electrolysis of H2O and CO2 using solid oxide cells (SOCs) the risk of carbon deposition in the Ni-YSZ electrode under high current densities (∼ 2.0 A/cm2) was studied in this work. Five galvanostatic tests were performed at current density between 1.5 and 2.25 A/cm2 and the average...

Southwest Pacific deep water carbonate chemistry linked to high southern latitude climate and atmospheric CO2 during the Last Glacial Termination

Science.gov (United States)

Allen, Katherine A.; Sikes, Elisabeth L.; Hönisch, Bärbel; Elmore, Aurora C.; Guilderson, Thomas P.; Rosenthal, Yair; Anderson, Robert F.

2015-08-01

A greater amount of CO2 was stored in the deep sea during glacial periods, likely via greater efficiency of the biologic pump and increased uptake by a more alkaline ocean. Reconstructing past variations in seawater carbonate ion concentration (a major component of alkalinity) enables quantification of the relative roles of different oceanic CO2 storage mechanisms and also places constraints on the timing, magnitude, and location of subsequent deep ocean ventilation. Here, we present a record of deep-water inorganic carbon chemistry since the Last Glacial Maximum (LGM; ∼19-23 ka BP), derived from sediment core RR0503-83 raised from 1627 m in New Zealand's Bay of Plenty. The core site lies within the upper limit of southern-sourced Circumpolar Deep Water (CDW), just below the lower boundary of Antarctic Intermediate Water (AAIW). We reconstruct past changes in bottom water inorganic carbon chemistry from the trace element and stable isotopic composition of calcite shells of the epibenthic foraminifer Cibicidoides wuellerstorfi. A record of ΔCO32-(ΔCO32- = [COCO32-] in situ - [CO32-] saturation) derived from the foraminiferal boron to calcium ratio (B/Ca) provides evidence for greater ice-age storage of respired CO2 and reveals abrupt deglacial shifts in [CO32-] in situ of up to 30 μmol/kg (5 times larger than the difference between average LGM and Holocene values). The rapidity of these changes suggests the influence of changing water mass structure and atmospheric circulation in addition to a decrease in CO2 content of interior waters.

Enhanced CO2 Adsorption on Activated Carbon Fibers Grafted with Nitrogen-Doped Carbon Nanotubes

Directory of Open Access Journals (Sweden)

Yu-Chun Chiang

2017-05-01

Full Text Available In this paper, multiscale composites formed by grafting N-doped carbon nanotubes (CNs on the surface of polyamide (PAN-based activated carbon fibers (ACFs were investigated and their adsorption performance for CO2 was determined. The spaghetti-like and randomly oriented CNs were homogeneously grown onto ACFs. The pre-immersion of cobalt(II ions for ACFs made the CNs grow above with a large pore size distribution, decreased the oxidation resistance, and exhibited different predominant N-functionalities after chemical vapor deposition processes. Specifically, the CNs grafted on ACFs with or without pre-immersion of cobalt(II ions were characterized by the pyridine-like structures of six-member rings or pyrrolic/amine moieties, respectively. In addition, the loss of microporosity on the specific surface area and pore volume exceeded the gain from the generation of the defects from CNs. The adsorption capacity of CO2 decreased gradually with increasing temperature, implying that CO2 adsorption was exothermic. The adsorption capacities of CO2 at 25 °C and 1 atm were between 1.53 and 1.92 mmol/g and the Freundlich equation fit the adsorption data well. The isosteric enthalpy of adsorption, implying physical adsorption, indicated that the growth of CNTs on the ACFs benefit CO2 adsorption.

Radiocarbon and stable-isotope geochemistry of organic and inorganic carbon in Lake Superior

Science.gov (United States)

Zigah, Prosper K.; Minor, Elizabeth C.; Werne, Josef P.

2012-03-01

We present a lake-wide investigation of Lake Superior carbon and organic matter biogeochemistry using radiocarbon, stable isotope, and carbon concentrations. Dissolved inorganic carbon (DIC) abundance in the lake was 121-122 Tg C, with offshore concentration andδ13C values being laterally homogenous and tightly coupled to the physical and thermal regime and biochemical processes. Offshore Δ14C of DIC (50-65‰) exhibited lateral homogeneity and was more 14C enriched than co-occurring atmospheric CO2 (˜38‰); nearshore Δ14C of DIC (36-38‰) was similar to atmospheric CO2. Dissolved organic carbon (DOC) abundance was 14.2-16.4 Tg C. DOC's concentration and δ13C were homogenous in June (mixed lake), but varied laterally during August (stratification) possibly due to spatial differences in lake productivity. Throughout sampling, DOC had modern radiocarbon values (14-58‰) indicating a semilabile nature with a turnover time of ≤60 years. Lake particulate organic carbon (POC, 0.9-1.3 Tg C) was consistently 13C depleted relative to DOC. The δ15N of epilimnetic particulate organic nitrogen shifted to more negative values during stratification possibly indicating greater use of nitrate (rather than ammonium) by phytoplankton in August. POC's radiocarbon was spatially heterogeneous (Δ14C range: 58‰ to -303‰), and generally 14C depleted relative to DOC and DIC. POC 14C depletion could not be accounted for by black carbon in the lake but, because of its spatial and temporal distribution, is attributed to sediment resuspension. The presence of old POC within the epilimnion of the open lake indicates possible benthic-pelagic coupling in the lake's organic carbon cycle; the ultimate fate of this old POC bears further investigation.

Calcium Carbonate Precipitation for CO2 Storage and Utilization: A Review of the Carbonate Crystallization and Polymorphism

Directory of Open Access Journals (Sweden)

Ribooga Chang

2017-07-01

Full Text Available The transformation of CO2 into a precipitated mineral carbonate through an ex situ mineral carbonation route is considered a promising option for carbon capture and storage (CCS since (i the captured CO2 can be stored permanently and (ii industrial wastes (i.e., coal fly ash, steel and stainless-steel slags, and cement and lime kiln dusts can be recycled and converted into value-added carbonate materials by controlling polymorphs and properties of the mineral carbonates. The final products produced by the ex situ mineral carbonation route can be divided into two categories—low-end high-volume and high-end low-volume mineral carbonates—in terms of their market needs as well as their properties (i.e., purity. Therefore, it is expected that this can partially offset the total cost of the CCS processes. Polymorphs and physicochemical properties of CaCO3 strongly rely on the synthesis variables such as temperature, pH of the solution, reaction time, ion concentration and ratio, stirring, and the concentration of additives. Various efforts to control and fabricate polymorphs of CaCO3 have been made to date. In this review, we present a summary of current knowledge and recent investigations entailing mechanistic studies on the formation of the precipitated CaCO3 and the influences of the synthesis factors on the polymorphs.

Integrated basic treatment of activated carbon for enhanced CO{sub 2} selectivity

Energy Technology Data Exchange (ETDEWEB)

Adelodun, Adedeji Adebukola; Jo, Young-Min, E-mail: ymjo@khu.ac.kr

2013-12-01

We attempted the use of three chemical agents viz nitric acid (HN), calcium nitrate (CaN) and calcium ethanoate (CaEt) to achieve enhanced CO{sub 2} selective adsorption by activated carbon (AC). In dry phase treatment, microporous coconut shell-based carbon (CS) exhibits higher CO{sub 2} capacity than coal-based. However, upon wet-phase pre-treatment, modified CS samples showed lesser CO{sub 2} adsorption efficiency. Surface characterization with X-ray photoelectron spectroscopy confirms the presence of calcium and amine species on the samples with integrated treatment (A-CaN). These samples recorded the highest low-level CO{sub 2} capture despite calcinated CaEt-doped samples (C-CaEt) showing the highest value for pure and high level CO{sub 2} adsorption capacities. The slope and linearity values of isobaric desorption were used to estimate the proportion of CO{sub 2} chemisorbed and heterogeneity of the adsorbents’ surfaces respectively. Consequently, integrated basic impregnation provides the most efficient adsorbents for selective adsorption of both indoor and outdoor CO{sub 2} levels.

De-oxygenation of CO2 by using Hydrogen, Carbon and Methane over Alumina-Supported Catalysts

Directory of Open Access Journals (Sweden)

R.Y. Raskar

2012-06-01

Full Text Available The de-oxygenation of CO2 was explored by using hydrogen, methane, carbon etc., over alumina supported catalysts. The alumina-supported ruthenium, rhodium, platinum, molybdenum, vanadium and magnesium catalysts were first reduced in hydrogen atmosphere and then used for the de-oxygenation of CO2. Furthermore, experimental variables for the de-oxygenation of CO2 were temperature (range 50 to 650 oC, H2/CO2 mole ratios (1.0 to 5, and catalyst loading (0.5 to 10 wt %. During the de-oxygenation of CO2 with H2 or CH4 or carbon, conversion of CO2, selectivity to CO and CH4 were estimated. Moreover, 25.4 % conversion of CO2 by hydrogen was observed over 1 wt% Pt/Al2O3 catalyst at 650 oC with 33.8 % selectivity to CH4. However, 8.1 to 13.9 % conversion of CO2 was observed over 1 wt% Pt/Al2O3 catalyst at 550 oC in the presence of both H2 and CH4. Moreover, 42.8 to 79.4 % CH4 was converted with 9 to 23.1 % selectivity to CO. It was observed that the de-oxygenation of CO2 by hydrogen, carbon and methane produced carbon, CO and CH4. © 2012 BCREC UNDIP. All rights reservedReceived: 6th February 2012; Revised: 23rd April 2012; Accepted: 24th April 2012[How to Cite: R. Y. Raskar, K. B. Kale, A. G. Gaikwad. (2011. De-oxygenation of CO2 by using Hydrogen, Carbon and Methane over Alumina-Supported Catalysts. Bulletin of Chemical Reaction Engineering & Catalysis, 7 (1: 59-69.  doi:10.9767/bcrec.7.1.1631.59-69][How to Link / DOI: http://dx.doi.org/10.9767/bcrec.7.1.1631.59-69 ] | View in 

Mechanistic Study of Magnesium Carbonate Semibatch Reactive Crystallization with Magnesium Hydroxide and CO2

DEFF Research Database (Denmark)

Han, B.; Qu, H. Y.; Niemi, H.

2014-01-01

This work investigates semibatch precipitation of magnesium carbonate at ambient temperature and pressure using Mg(OH)(2) and CO2 as starting materials. A thermal analysis method was developed that reflects the dissolution rate of Mg(OH)(2) and the formation of magnesium carbonate. The method...... the liquid and solid phases. A stirring rate of 650 rpm was found to be the optimum speed as the flow rate of CO2 was 1 L/min. Precipitation rate increased with gas flow rate, which indicates that mass transfer of CO2 plays a critical role in this precipitation case. Magnesium carbonate trihydrate...

Amine–mixed oxide hybrid materials for carbon dioxide adsorption from CO2/H2 mixture

Science.gov (United States)

Ravi, Navin; Aishah Anuar, Siti; Yusuf, Nur Yusra Mt; Isahak, Wan Nor Roslam Wan; Shahbudin Masdar, Mohd

2018-05-01

Bio-hydrogen mainly contains hydrogen and high level of carbon dioxide (CO2). High concentration of CO2 lead to a limitation especially in fuel cell application. In this study, the amine-mixed oxide hybrid materials for CO2 separation from bio-hydrogen model (50% CO2:50% H2) have been studied. Fourier-transform infrared spectroscopy (FTIR) and x-ray diffraction (XRD) characterizations showed that the amine–mixed oxide hybrid materials successfully adsorbed CO2 physically with no chemical adsorption evidence. The dry gas of CO2/H2 mixture adsorbed physically on amine–CuO–MgO hybrid material. No carbonates were detected after several times of adsorption, which indicated the good recyclability of adsorbents. The adsorbent system of diethanolamine (DEA)/15% CuO–75% MgO showed the highest CO2 adsorption capacity of 21.2 wt% due to the presence of polar substance on MgO surface, which can adsorb CO2 at ambient condition. The alcohol group of DEA can enhance the CO2 solubility on the adsorbent surface. In the 20% CuO–50% MgO adsorbent system, DEA as amine type showed a high CO2 adsorption of 19.4 wt%. The 10% amine loading system showed that the DEA adsorption system provided high CO2 adsorption. The BET analysis confirmed that a high amine loading contributed to the decrease in CO2 adsorption due to the low surface area of the adsorbent system.

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

Science.gov (United States)

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

2014-02-01

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

Making carbon dioxide sequestration feasible: Toward federal regulation of CO2 sequestration pipelines

International Nuclear Information System (INIS)

Mack, Joel; Endemann, Buck

2010-01-01

As the United States moves closer to a national climate change policy, it will have to focus on a variety of factors affecting the manner in which the country moves toward a future with a substantially lower carbon footprint. In addition to encouraging renewable energy, smart grid, clean fuels and other technologies, the United States will need to make substantial infrastructure investments in a variety of industries. Among the significant contributors to the current carbon footprint in the United States is the use of coal as a major fuel for the generation of electricity. One of the most important technologies that the United States can employ to reduce its carbon footprint is to sequester the carbon dioxide ('CO 2 ') from coal-fired power plants. This article focuses on the legal and policy issues surrounding a critical piece of the necessary sequestration infrastructure: CO 2 pipelines that will carry CO 2 from where it is removed from fuel or waste gas streams to where it will be sequestered. Ultimately, this article recommends developing a federally regulated CO 2 pipeline program to foster the implementation of carbon sequestration technology.

Conversion of CO₂ into Commercial Materials Using Carbon Feedstocks

Energy Technology Data Exchange (ETDEWEB)

Shen, Jian-Ping [Research Triangle Institute (RTI), Research Triangle Park, NC (United States); Peters, Jonathan [Research Triangle Institute (RTI), Research Triangle Park, NC (United States); Lail, Marty [Research Triangle Institute (RTI), Research Triangle Park, NC (United States); Mobley, Paul [Research Triangle Institute (RTI), Research Triangle Park, NC (United States); Turk, Brian [Research Triangle Institute (RTI), Research Triangle Park, NC (United States)

2014-05-31

In this project, our research focused on developing reaction chemistry that would support using carbon as a reductant for CO₂ utilization that would permit CO₂ consumption on a scale that would match or exceed anthropomorphic CO₂ generation for energy production from fossil fuels. Armed with the knowledge that reactions attempting to produce compounds with an energy content greater than CO₂ would be thermodynamically challenged and/or require significant amounts of energy, we developed a potential process that utilized a solid carbon source and recycled the carbon to effectively provide infinite time for the carbon to react. During testing of different carbon sources, we found a wide range of reaction rates. Biomass-derived samples had the most reactivity and coals and petcoke had the lowest. Because we had anticipated this challenge, we recognized that a catalyst would be necessary to improve reaction rates and conversion. From the data analysis of carbon samples, we recognized that alkali metals improved the reaction rate. Through parametric testing of catalyst formulations we were able to increase the reaction rate with petcoke by a factor of >70. Our efforts to identify the reaction mechanism to assist in improving the catalyst formulation demonstrated that the catalyst was catalyzing the extraction of oxygen from CO₂ and using this extracted oxygen to oxidize carbon. This was a significant discovery in that if we could modify the catalyst formulation to permit controlled the oxidation, we would have a very power selective oxidation process. With selective oxidation, CO₂ utilization could be effective used as one of the process steps in making many of the large volume commodity chemicals that support our modern lifestyles. The key challenges for incorporating these functionalities into the catalyst formulation were to make the oxidation selective and lower the temperature required for catalytic

Porous carbon derived via KOH activation of a hypercrosslinked porous organic polymer for efficient CO{sub 2}, CH{sub 4}, H{sub 2} adsorptions and high CO{sub 2}/N{sub 2} selectivity

Energy Technology Data Exchange (ETDEWEB)

Modak, Arindam; Bhaumik, Asim, E-mail: msab@iacs.res.in

2015-12-15

Microporous carbon having Brunauer-Emmett-Teller (BET) surface area of 2186 m{sup 2} g{sup −1} and micropore volume of 0.85 cm{sup 3} g{sup −1} has been synthesized via KOH induced high temperature carbonization of a non-conjugated hypercrosslinked organic polymer. Owing to the templating and activation by KOH, we have succeeded in making a microporous carbon from this porous polymer and the resultant carbon material showed high uptake for CO{sub 2} (7.6 mmol g{sup −1}) and CH{sub 4} (2.4 mmol g{sup −1}) at 1 atm, 273 K together with very good selectivity for the CO{sub 2}/N{sub 2} (30.2) separation. Furthermore, low pressure (1 atm) H{sub 2} (2.6 wt%, 77 K) and water uptake (57.4 wt%, 298 K) ability of this polymer derived porous activated carbon is noteworthy. - Graphical abstract: Microporous carbon with BET surface area of 2186 m{sup 2} g{sup −1} has been synthesized via KOH activation of a porous organic polymer and it showed high uptake for CO{sub 2} (7.6 mmol g{sup −1}), CH{sub 4} (2.4 mmol g{sup −1}) and H{sub 2} (2.6 wt%) at 1 atm together with very good selectivity for CO{sub 2}. - Highlights: • Porous carbon from hypercrosslinked organic polymer. • KOH activated carbon with BET surface area 2186 m{sup 2} g{sup −1}. • High CO2 uptake (7.6 mmol g{sup −1}) and CO{sub 2}/N{sub 2} selectivity (30.2). • Porous carbon also showed high H{sub 2} (2.6 wt%) and H{sub 2}O (57.4 wt%) uptakes.

The stable carbon isotope biogeochemistry of acetate and other dissolved carbon species in deep subseafloor sediments at the northern Cascadia Margin

Science.gov (United States)

Heuer, Verena B.; Pohlman, John W.; Torres, Marta E.; Elvert, Marcus; Hinrichs, Kai-Uwe

2009-01-01

Ocean drilling has revealed the existence of vast microbial populations in the deep subseafloor, but to date little is known about their metabolic activities. To better understand the biogeochemical processes in the deep biosphere, we investigate the stable carbon isotope chemistry of acetate and other carbon-bearing metabolites in sediment pore-waters. Acetate is a key metabolite in the cycling of carbon in anoxic sediments. Its stable carbon isotopic composition provides information on the metabolic processes dominating acetate turnover in situ. This study reports our findings for a methane-rich site at the northern Cascadia Margin (NE Pacific) where Expedition 311 of the Integrated Ocean Drilling Program (IODP) sampled the upper 190 m of sediment. At Site U1329, δ13C values of acetate span a wide range from −46.0‰ to −11.0‰ vs. VPDB and change systematically with sediment depth. In contrast, δ13C values of both the bulk dissolved organic carbon (DOC) (−21.6 ± 1.3‰ vs. VPDB) and the low-molecular-weight compound lactate (−20.9 ± 1.8‰ vs. VPDB) show little variability. These species are interpreted to represent the carbon isotopic composition of fermentation products. Relative to DOC, acetate is up to 23.1‰ depleted and up to 9.1‰ enriched in 13C. Broadly, 13C-depletions of acetate relative to DOC indicate flux of carbon from acetogenesis into the acetate pool while 13C-enrichments of pore-water acetate relative to DOC suggest consumption of acetate by acetoclastic methanogenesis. Isotopic relationships between acetate and lactate or DOC provide new information on the carbon flow and the presence and activity of specific functional microbial communities in distinct biogeochemical horizons of the sediment. In particular, they suggest that acetogenic CO2-reduction can coexist with methanogenic CO2-reduction, a notion contrary to the hypothesis that hydrogen levels are controlled by the thermodynamically most favorable electron

Preparation and Characterization of Impregnated Commercial Rice Husks Activated Carbon with Piperazine for Carbon Dioxide (CO2) Capture

Science.gov (United States)

Masoum Raman, S. N.; Ismail, N. A.; Jamari, S. S.

2017-06-01

Development of effective materials for carbon dioxide (CO2) capture technology is a fundamental importance to reduce CO2 emissions. This work establishes the addition of amine functional group on the surface of activated carbon to further improve the adsorption capacity of CO2. Rice husks activated carbon were modified using wet impregnation method by introducing piperazine onto the activated carbon surfaces at different concentrations and mixture ratios. These modified activated carbons were characterized by using X-Ray Diffraction (XRD), Brunauer, Emmett and Teller (BET), Fourier Transform Infrared Spectroscopy (FTIR) and Field Emission Scanning Electron Microscopy (FESEM). The results from XRD analysis show the presence of polyethylene butane at diffraction angles of 21.8° and 36.2° for modified activated carbon with increasing intensity corresponding to increase in piperazine concentration. BET results found the surface area and pore volume of non-impregnated activated carbon to be 126.69 m2/g and 0.081 cm3/g respectively, while the modified activated carbons with 4M of piperazine have lower surface area and pore volume which is 6.77 m2/g and 0.015 cm3/g respectively. At 10M concentration, the surface area and pore volume are the lowest which is 4.48 m2/g and 0.0065 cm3/g respectively. These results indicate the piperazine being filled inside the activated carbon pores thus, lowering the surface area and pore volume of the activated carbon. From the FTIR analysis, the presence of peaks at 3312 cm-1 and 1636 cm-1 proved the existence of reaction between carboxyl groups on the activated carbon surfaces with piperazine. The surface morphology of activated carbon can be clearly seen through FESEM analysis. The modified activated carbon contains fewer pores than non-modified activated carbon as the pores have been covered with piperazine.

Austria's CO2 responsibility and the carbon content of its international trade

International Nuclear Information System (INIS)

Munoz, Pablo; Steininger, Karl W.

2010-01-01

Seeking to limit global warming to 2 C puts narrow restrictions on the remaining carbon budget. While the prevalent accounting framework for carbon emissions is production based (Production-Based Principle, PBP), we here quantify the CO 2 emissions on the basis of the Consumption-Based Principle (CBP) for Austria. At a methodological level, a Multi-Regional Input-Output model with full linkages is used to account for Austria's CO 2 responsibility on a global scale. Estimates are carried out for the years 1997 and 2004. Results show that during 1997 CO 2 responsibility based on CBP were 36% larger than those based on PBP. This relation has increased through time. The CBP indicator of 2004 was 44% larger than the PBP. In terms of carbon emission location, for each Euro spent on Austrian final demand in 2004, it is estimated that two-thirds of the CO 2 emissions occur outside Austrian borders. Regarding the origin of the emissions embodied in imports, it is estimated that about one-fourth originated in non-Annex I countries in 1997. This proportion increased to one-third by 2004. Due to this divergence between CBP and PBP indicators, there is a need to re-think current accounting bases in order to properly assign CO 2 responsibilities. (author)

CO2 emission standards and investment in carbon capture

International Nuclear Information System (INIS)

Eide, Jan; Sisternes, Fernando J. de; Herzog, Howard J.; Webster, Mort D.

2014-01-01

Policy makers in a number of countries have proposed or are considering proposing CO 2 emission standards for new fossil fuel-fired power plants. The proposed standards require coal-fired power plants to have approximately the same carbon emissions as an uncontrolled natural gas-fired power plant, effectively mandating the adoption of carbon capture and sequestration (CCS) technologies for new coal plants. However, given the uncertainty in the capital and operating costs of a commercial scale coal plant with CCS, the impact of such a standard is not apparent a priori. We apply a stochastic generation expansion model to determine the impact of CO 2 emission standards on generation investment decisions, and in particular for coal plants with CCS. Moreover, we demonstrate how the incentive to invest in coal-CCS from emission standards depends on the natural gas price, the CO 2 price, and the enhanced oil recovery price, as well as on the level of the emission standard. This analysis is the first to consider the entire power system and at the same time allow the capture percentage for CCS plants to be chosen from a continuous range to meet the given standard at minimum cost. Previous system level studies have assumed that CCS plants capture 90% of the carbon, while studies of individual units have demonstrated the costs of carbon capture over a continuous range. We show that 1) currently proposed levels of emission standards are more likely to shift fossil fuel generation from coal to natural gas rather than to incentivize investment in CCS; 2) tighter standards that require some carbon reductions from natural gas-fired power plants are more likely than proposed standards to incentivize investments in CCS, especially on natural gas plants, but also on coal plants at high gas prices; and 3) imposing a less strict emission standard (emission rates higher than natural gas but lower than coal; e.g., 1500 lbs/MWh) is more likely than current proposals to incentivize

Carbonic anhydrase levels and internal lacunar CO/sub 2/ concentrations in aquatic macrophytes

Energy Technology Data Exchange (ETDEWEB)

Weaver, C.I.

1979-01-01

Carbonic anhydrase levels were examined in a variety of aquatic macrophytes from different habitats. In general, carbonic anhydrase levels increased across the habitat gradient such that activities were low in submersed aquatic macrophytes and high in emergent macrophytes with floating-leaved and free-floating plants exhibiting intermediate activities. Internal lacunar CO/sub 2/ concentrations were analyzed in relation to carbonic anhydrase activities. There was no correlation between these two parameters. Internal CO/sub 2/ concentrations ranged from low to high in submersed macrophytes, but were low in floating-leaved and emergent macrophytes. The observed internal CO/sub 2/ concentrations are discussed in relation to the individual morphologies of the plants and the environments in which they occurred.

Mechanisms of carbon dioxide acquisition and CO2 sensing in marine diatoms: a gateway to carbon metabolism.

Science.gov (United States)

Matsuda, Yusuke; Hopkinson, Brian M; Nakajima, Kensuke; Dupont, Christopher L; Tsuji, Yoshinori

2017-09-05

Diatoms are one of the most successful marine eukaryotic algal groups, responsible for up to 20% of the annual global CO 2 fixation. The evolution of a CO 2 -concentrating mechanism (CCM) allowed diatoms to overcome a number of serious constraints on photosynthesis in the marine environment, particularly low [CO 2 ] aq in seawater relative to concentrations required by the CO 2 fixing enzyme, ribulose-1,5-bisphosphate carboxylase/oxygenase (RubisCO), which is partly due to the slow diffusion rate of CO 2 in water and a limited CO 2 formation rate from [Formula: see text] in seawater. Diatoms use two alternative strategies to take up dissolved inorganic carbon (DIC) from the environment: one primarily relies on the direct uptake of [Formula: see text] through plasma-membrane type solute carrier (SLC) 4 family [Formula: see text] transporters and the other is more reliant on passive diffusion of CO 2 formed by an external carbonic anhydrase (CA). Bicarbonate taken up into the cytoplasm is most likely then actively transported into the chloroplast stroma by SLC4-type transporters on the chloroplast membrane system. Bicarbonate in the stroma is converted into CO 2 only in close proximity to RubisCO preventing unnecessary CO 2 leakage. CAs play significant roles in mobilizing DIC as it is progressively moved towards the site of fixation. However, the evolutionary types and subcellular locations of CAs are not conserved between different diatoms, strongly suggesting that this DIC mobilization strategy likely evolved multiple times with different origins. By contrast, the recent discovery of the thylakoid luminal θ-CA indicates that the strategy to supply CO 2 to RubisCO in the pyrenoid may be very similar to that of green algae, and strongly suggests convergent coevolution in CCM function of the thylakoid lumen not only among diatoms but among eukaryotic algae in general. In this review, both experimental and corresponding theoretical models of the diatom CCMs are

Carbon coated CoS_2 thermal battery electrode material with enhanced discharge performances and air stability

International Nuclear Information System (INIS)

Xie, Song; Deng, Yafeng; Mei, Jun; Yang, Zhaotang; Lau, Woon-Ming; Liu, Hao

2017-01-01

Graphical abstract: A novel carbon coated CoS_2 composite is prepared and investigated as a cathode material for thermal batteries. - Highlights: • A novel C@CoS_2 composite is successfully prepared by hydrothermal method. • The growth of CoS_2 in the glucose solution results in a smaller grain size. • The coating of carbon favors electron transfer and buffers polysulfides formation. • The in situ coated carbon layer effectively prevents the oxidation of CoS_2. • The C@CoS_2 composite shows competitive thermal stability and discharge property. - Abstract: Cobalt disulfide (CoS_2) is a promising thermal battery electrode material for its superior thermal stability and discharge performance. However, the low natural resource and poor air stability restrict its application in thermal battery fabrication. In this work, carbon coated CoS_2 composite was prepared by a facile one-pot hydrothermal method with glucose as carbon source. During the growth of CoS_2, the glucose molecules were in situ adsorbed and carbonized on the surface of the as-synthesized CoS_2, and the resultant carbon coating provided improved electrical conductivity and discharge performances to the composite. The thermal battery cell, which was fabricated with such a composite cathode and with a Li-Si anode, can output a capacity of 235.8 mAh g"−"1 and an energy density of 416.9 Wh kg"−"1 at a cut-off voltage of 1.7 V. This carbon coated CoS_2 composite also presented enhanced air stability. After being stored in dry air for 3 months, the composite can still provide a capacity of 232.4 mAh g"−"1 to 1.7 V, whereas the capacity of bare CoS_2 stored with the same condition dropped from 202.4 mAh g"−"1 to 189.7 mAh g"−"1.

A Nitrogen-Doped Carbon Catalyst for Electrochemical CO2 Conversion to CO with High Selectivity and Current Density.

Science.gov (United States)

Jhong, Huei-Ru Molly; Tornow, Claire E; Smid, Bretislav; Gewirth, Andrew A; Lyth, Stephen M; Kenis, Paul J A

2017-03-22

We report characterization of a non-precious metal-free catalyst for the electrochemical reduction of CO 2 to CO; namely, a pyrolyzed carbon nitride and multiwall carbon nanotube composite. This catalyst exhibits a high selectivity for production of CO over H 2 (approximately 98 % CO and 2 % H 2 ), as well as high activity in an electrochemical flow cell. The CO partial current density at intermediate cathode potentials (V=-1.46 V vs. Ag/AgCl) is up to 3.5× higher than state-of-the-art Ag nanoparticle-based catalysts, and the maximum current density is 90 mA cm -2 . The mass activity and energy efficiency (up to 48 %) were also higher than the Ag nanoparticle reference. Moving away from precious metal catalysts without sacrificing activity or selectivity may significantly enhance the prospects of electrochemical CO 2 reduction as an approach to reduce atmospheric CO 2 emissions or as a method for load-leveling in relation to the use of intermittent renewable energy sources. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Mechanisms of aqueous wollastonite carbonation as a possible CO2 sequestration process

NARCIS (Netherlands)

Huijgen, W.J.J.; Witkamp, G.J.; Comans, R.N.J.

2006-01-01

The mechanisms of aqueous wollastonite carbonation as a possible carbon dioxide sequestration process were investigated experimentally by systematic variation of the reaction temperature, CO2 pressure, particle size, reaction time, liquid to solid ratio and agitation power. The carbonation reaction

CO{sub 2} CAPTURE BY ABSORPTION WITH POTASSIUM CARBONATE

Energy Technology Data Exchange (ETDEWEB)

Gary T. Rochelle; J.Tim Cullinane; Marcus Hilliard; Eric Chen; Babatunde Oyenekan; Ross Dugas

2005-01-31

The objective of this work is to improve the process for CO{sub 2} capture by alkanolamine absorption/stripping by developing an alternative solvent, aqueous K{sub 2}CO{sub 3} promoted by piperazine. Thermodynamic modeling predicts that the heat of desorption of CO{sub 2} from 5m K+/2.5 PZ from 85 kJ/mole at 40 C to 30 kJ/mole at 120 C. Mass transfer modeling of this solvent suggests that carbonate and general salt concentration play a major role in catalyzing the rate of reaction of CO{sub 2} with piperazine. Stripper modeling suggests that with the multipressure stripper, the energy consumption with a generic solvent decreases by 15% as the heat of desorption is decreased from 23.8 to 18.5 kcal/gmol. A second pilot plant campaign with 5m K+/2.5 PZ was successfully completed.

Calculations from the Hadley Centre: The ocean is rising even with stable CO2

International Nuclear Information System (INIS)

Groenaas, Sigbjoern

2000-01-01

The article presents calculations and forecasts for the atmospheric CO 2 level changes in the period of 2000 to 2350. Correlations between the levels and the average global temperature and the sea level are studied for the period of 1850 to 2200. The main conclusion is that the sea level will continue to rise for several hundred years even with a stable atmospheric CO 2 concentration in the next century due to the slow response of oceans to global warming

Constraining the subsoil carbon source to cave-air CO2 and speleothem calcite in central Texas

Science.gov (United States)

Bergel, Shelly J.; Carlson, Peter E.; Larson, Toti E.; Wood, Chris T.; Johnson, Kathleen R.; Banner, Jay L.; Breecker, Daniel O.

2017-11-01

Canonical models for speleothem formation and the subsurface carbon cycle invoke soil respiration as the dominant carbon source. However, evidence from some karst regions suggests that belowground CO2 originates from a deeper, older source. We therefore investigated the carbon sources to central Texas caves. Drip-water chemistry of two caves in central Texas implies equilibration with calcite at CO2 concentrations (PCO2_sat) higher than the maximum CO2 concentrations observed in overlying soils. This observation suggests that CO2 is added to waters after they percolate through the soils, which requires a subsoil carbon source. We directly evaluate the carbon isotope composition of the subsoil carbon source using δ13C measurements on cave-air CO2, which we independently demonstrate has little to no contribution from host rock carbon. We do so using the oxidative ratio, OR, defined as the number of moles of O2 consumed per mole of CO2 produced during respiration. However, additional belowground processes that affect O2 and CO2 concentrations, such as gas-water exchange and/or diffusion, may also influence the measured oxidative ratio, yielding an apparent OR (ORapparent). Cave air in Natural Bridge South Cavern has ORapparent values (1.09 ± 0.06) indistinguishable from those expected for respiration alone (1.08 ± 0.06). Pore space gases from soils above the cave have lower values (ORapparent = 0.67 ± 0.05) consistent with respiration and gas transport by diffusion. The simplest explanation for these observations is that cave air in NB South is influenced by respiration in open-system bedrock fractures such that neither diffusion nor exchange with water influence the composition of the cave air. The radiocarbon activities of NB South cave-air CO2 suggest the subsoil carbon source is hundreds of years old. The calculated δ13C values of the subsoil carbon source are consistent with tree-sourced carbon (perhaps decomposing root matter), the δ13C values of which

Soil surface CO2 fluxes and the carbon budget of a grassland

Science.gov (United States)

Norman, J. M.; Garcia, R.; Verma, S. B.

1992-01-01

Measurements of soil surface CO2 fluxes are reported for three sites within the First International Satellite Land Surface Climatology Project (ISLSCP) Field Experiment (FIFE) area, and simple empirical equations are fit to the data to provide predictions of soil fluxes from environmental observations. A prototype soil chamber, used to make the flux measurements, is described and tested by comparing CO2 flux measurements to a 40-L chamber, a 1-m/cu chamber, and eddy correlation. Results suggest that flux measurements with the prototype chamber are consistent with measurements by other methods to within about 20 percent. A simple empirical equation based on 10-cm soil temperature, 0- to 10-cm soil volumetric water content, and leaf area index predicts the soil surface CO2 flux with a rms error of 1.2 micro-mol sq m/s for all three sites. Further evidence supports using this equation to evaluate soil surface CO2 during the 1987 FIFE experiment. The soil surface CO2 fluxes when averaged over 24 hours are comparable to daily gross canopy photosynthetic rates. For 6 days of data the net daily accumulation of carbon is about 0.6 g CO2 sq m/d; this is only a few percent of the daily gross accumulation of carbon by photosynthesis. As the soil became drier in 1989, the net accumulation of carbon by the prairie increased, suggesting that the soil flux is more sensitive to temperature and drought than the photosynthetic fluxes.

The dynamics of CO2 fixation in the Southern Ocean as indicated by carboxylase activities and organic carbon isotopic ratios

International Nuclear Information System (INIS)

Fontugne, M.

1991-01-01

Recent studies have suggested a direct relationship between the dissolved CO 2 concentration and carbon isotopic composition of phytoplankton in surface ocean. Thus, measurement of δ 13 C of planktonic organic matter in deep-sea ocean cores can potentially yield a record of the past atmospheric CO 2 variations. However, results are presented from 3 cruises in Indian and Atlantic sectors of the Southern Ocean (between 40-66degS) in which biochemical and physiological factors associated with photosynthetic processes lead to carbon isotopic fractionation by phytoplankton which cannot be directly related to variations within the mineral carbon pool. Simultaneous measurements of the carboxylase activities in the 13 C/ 12 C ratio of particulate organic carbon show that there is a large variability in phytoplankton carbon metabolism, especially on a seasonal scale, in spite of a relative uniformity of the environmental conditions. Phytoplankton carbon metabolism is clearly a main factor governing variations in the stable isotopic composition of organic matter in the euphotic layer. Interrelationships between light, Rubiso activity and δ 13 C are clearly shown by the data. Heterotrophic processes may also influence the carbon isotope mass balance, especially during the break-up of the ice pack. In addition to the influence of photosynthetic metabolism, the effect of the meridoneal temperature gradient is also verified by the data set. (author). 24 refs.; 5 figs

No influence of CO2 on stable isotope analyses of soil waters with off-axis integrated cavity output spectroscopy (OA-ICOS).

Science.gov (United States)

Sprenger, Matthias; Tetzlaff, Doerthe; Soulsby, Chris

2017-03-15

It was recently shown that the presence of CO 2 affects the stable isotope (δ 2 H and δ 18 O values) analysis of water vapor via Wavelength-Scanned Cavity Ring-Down Spectroscopy. Here, we test how much CO 2 is emitted from soil samples and if the CO 2 in the headspace influences the isotope analysis with the direct equilibration method by Off-Axis Integrated Cavity Output Spectroscopy (OA-ICOS). The headspace above different amounts of sparkling water was sampled, and its stable isotopic composition (δ 2 H and δ 18 O values) and CO 2 concentration were measured by direct equilibration and by gas chromatography, respectively. In addition, the headspace above soil samples was analyzed in the same way. Furthermore, the gravimetric water content and the loss on ignition were measured for the soil samples. The experiment with the sparkling water showed that CO 2 does not influence the stable isotope analysis by OA-ICOS. CO 2 was emitted from the soil samples and correlated with the isotopic fractionation signal, but no causal relationship between the two was determined. Instead, the fractionation signal in pore water isotopes can be explained by soil evaporation and the CO 2 can be related to soil moisture and organic matter which both enhance microbial activity. We found, despite the high CO 2 emissions from soil samples, no need for a post-correction of the pore water stable isotope analysis results, since there is no relation between CO 2 concentrations and the stable isotope results of vapor samples obtained with OA-ICOS. © 2016 The Authors. Rapid Communications in Mass Spectrometry Published by John Wiley & Sons Ltd. © 2016 The Authors. Rapid Communications in Mass Spectrometry Published by John Wiley & Sons Ltd.

Mesoporous NiCo2O4 nano-needles supported by 3D interconnected carbon network on Ni foam for electrochemical energy storage

Science.gov (United States)

Lu, Congxiang; Liu, Wen-wen; Pan, Hui; Tay, Beng Kang; Wang, Xingli; Liang, Kun; Wei, Xuezhe

2018-05-01

In this work, a three dimensional (3D) interconnected carbon network consisting of ultrathin graphite (UG) and carbon nanotubes (CNTs) on Ni foam is fabricated and employed as a novel type of substrate for mesoporous NiCo2O4 nano-needles. The successfully synthesized NiCo2O4 nano-needles/CNTs/UG on Ni foam has many advantages including facile electrolyte access and direct conducting pathways towards current collectors, which enable it to be a promising electrode material in battery-like electrochemical energy storage. Encouragingly, a high capacity of 135.1 mAh/g at the current density of 1 A/g, superior rate performance and also stable cycling for 1200 cycles at the current density of 5 A/g have been demonstrated in this novel material.

One-pot synthetic method to prepare highly N-doped nanoporous carbons for CO2 adsorption

International Nuclear Information System (INIS)

Meng, Long-Yue; Park, Soo-Jin

2014-01-01

A one-pot synthetic method was used for the preparation of nanoporous carbon containing nitrogen from polypyrrole (PPY) using NaOH as the activated agent. The activation process was carried out under set conditions (NaOH/PPY = 2 and NaOH/PPY = 4) at different temperatures in 600–900 °C for 2 h. The effect of the activation conditions on the pore structure, surface functional groups and CO 2 adsorption capacities of the prepared N-doped activated carbons was examined. The carbon was analyzed by X-ray photoelectron spectroscopy (XPS), N2/77 K full isotherms, scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The CO 2 adsorption capacity of the N-doped activated carbon was measured at 298 K and 1 bar. By dissolving the activation agents, the N-doped activated carbon exhibited high specific surface areas (755–2169 m 2 g −1 ) and high pore volumes (0.394–1.591 cm 3 g −1 ). In addition, the N-doped activated carbons contained a high N content at lower activation temperatures (7.05 wt.%). The N-doped activated carbons showed a very high CO 2 adsorption capacity of 177 mg g −1 at 298 K and 1 bar. The CO 2 adsorption capacity was found to be dependent on the microporosity and N contents. - Highlights: • A one-pot synthetic method was used for the preparation of N-doped nanoporous carbons. • Polypyrrole (PPY) were activated with NaOH under set conditions (NaOH/PPY = 2 and 4). • N-doped activated carbon exhibited high specific surface areas (2169 m 2 g −1 ). • The carbons showed a very high CO 2 adsorption capacity of 177 mg g −1 at 298 K

Measurement and Modelling of the Piperazine Potassium Carbonate Solutions for CO2 Capture

DEFF Research Database (Denmark)

Fosbøl, Philip Loldrup; Thomsen, Kaj; Waseem Arshad, Muhammad

The climate is in a critical state due to the impact of pollution by CO2 and similar greenhouse gasses. Action needs to be taken in order reduce the emission of harmful components. CO2 capture is one process to help the world population back on track in order to return to normal condition...... with the purpose of simulating the CO2 capture process. This involves equilibrium studies on physical properties in the activated carbonate solvent. Energy consumption while applying the promoted carbonate solutions using piperazine is given in overview....

Can Producing Oil Store Carbon? Greenhouse Gas Footprint of CO2EOR, Offshore North Sea.

Science.gov (United States)

Stewart, R Jamie; Haszeldine, R Stuart

2015-05-05

Carbon dioxide enhanced oil recovery (CO2EOR) is a proven and available technology used to produce incremental oil from depleted fields while permanently storing large tonnages of injected CO2. Although this technology has been used successfully onshore in North America and Europe, there are currently no CO2EOR projects in the United Kingdom. Here, we examine whether offshore CO2EOR can store more CO2 than onshore projects traditionally have and whether CO2 storage can offset additional emissions produced through offshore operations and incremental oil production. Using a high-level Life Cycle system approach, we find that the largest contribution to offshore emissions is from flaring or venting of reproduced CH4 and CO2. These can already be greatly reduced by regulation. If CO2 injection is continued after oil production has been optimized, then offshore CO2EOR has the potential to be carbon negative--even when emissions from refining, transport, and combustion of produced crude oil are included. The carbon intensity of oil produced can be just 0.056-0.062 tCO2e/bbl if flaring/venting is reduced by regulation. This compares against conventional Saudi oil 0.040 tCO2e/bbl or mined shale oil >0.300 tCO2e/bbl.

Carbon assimilation in Eucalyptus urophylla grown under high atmospheric CO2 concentrations: A proteomics perspective.

Science.gov (United States)

Santos, Bruna Marques Dos; Balbuena, Tiago Santana

2017-01-06

Photosynthetic organisms may be drastically affected by the future climate projections of a considerable increase in CO 2 concentrations. Growth under a high concentration of CO 2 could stimulate carbon assimilation-especially in C3-type plants. We used a proteomics approach to test the hypothesis of an increase in the abundance of the enzymes involved in carbon assimilation in Eucalyptus urophylla plants grown under conditions of high atmospheric CO 2 . Our strategy allowed the profiling of all Calvin-Benson cycle enzymes and associated protein species. Among the 816 isolated proteins, those involved in carbon fixation were found to be the most abundant ones. An increase in the abundance of six key enzymes out of the eleven core enzymes involved in carbon fixation was detected in plants grown at a high CO 2 concentration. Proteome changes were corroborated by the detection of a decrease in the stomatal aperture and in the vascular bundle area in Eucalyptus urophylla plantlets grown in an environment of high atmospheric CO 2 . Our proteomics approach indicates a positive metabolic response regarding carbon fixation in a CO 2 -enriched atmosphere. The slight but significant increase in the abundance of the Calvin enzymes suggests that stomatal closure did not prevent an increase in the carbon assimilation rates. The sample enrichment strategy and data analysis used here enabled the identification of all enzymes and most protein isoforms involved in the Calvin-Benson-Bessham cycle in Eucalyptus urophylla. Upon growth in CO 2 -enriched chambers, Eucalyptus urophylla plantlets responded by reducing the vascular bundle area and stomatal aperture size and by increasing the abundance of six of the eleven core enzymes involved in carbon fixation. Our proteome approach provides an estimate on how a commercially important C3-type plant would respond to an increase in CO 2 concentrations. Additionally, confirmation at the protein level of the predicted genes involved in

On the relations between the oceanic uptake of CO2 and its carbon isotopes

International Nuclear Information System (INIS)

Heimann, M.; Maier-Reimer, E.

1994-01-01

The recent proposals to estimate the oceanic uptake of CO 2 by monitoring the oceanic change in 13 C/ 12 C isotope ratio or the air-sea 13 C/ 12 C isotopic disequilibrium is reviewed. Because the history of atmospheric CO 2 and 13 CO 2 since preindustrial times is almost the same, the oceanic penetration depth of both tracers must be the same. This dynamic constraint permits the establishment of yet a third method to estimate the global ocean uptake of CO 2 from 13 C measurements. Using available observations in conjunction with canonical values for the global carbon cycle parameters the three methods yield inconsistent oceanic CO 2 uptake rates for the time period 1970-1990, ranging from 0 to over 3 GtC year -1 . However, uncertainties in the available carbon cycle data must be taken into account. Using a non-linear estimation procedure, a consistent scenario with an oceanic CO 2 uptake rate of 2.2±0.8 GtC year -1 can be established. The method also permits an investigation of the sensitivities of the different approaches. An analysis of the results of two three-dimensional simulations with the Hamburg Model of the Oceanic Carbon Cycle shows that the 13 C isotope indeed tracks the oceanic penetration of anthropogenic CO 2 . Because of its different time history, bomb produced radiocarbon, as measured at the time of GEOSECS, correlates much less well to excess carbon. (orig.)

Impacts of Low-Carbon Innovation and Its Heterogeneous Components on CO2 Emissions

Directory of Open Access Journals (Sweden)

Zheming Yan

2017-04-01

Full Text Available This paper aims to investigate the impact of low-carbon innovation on CO2 emissions. Using patent statistics, we measured low-carbon innovations for 15 major economies during the period of 1992–2012. Then, we classified low-carbon technology into clean and gray technology according to the patent classification system. Following the empirical Environmental Kuznets Curve (EKC framework, we explored the effects of low-carbon innovation and its components on CO2 emissions. We did not find any evidence of significant influence of low-carbon innovation. Through further estimations, a significantly negative effect of clean innovation was found while the effect of gray innovation is not clear. Heterogeneous impacts within low-carbon technology provide an explanation for the insignificant impact of low-carbon innovation.

Nitrogen fertilization raises CO2 efflux from inorganic carbon: A global assessment.

Science.gov (United States)

Zamanian, Kazem; Zarebanadkouki, Mohsen; Kuzyakov, Yakov

2018-03-25

Nitrogen (N) fertilization is an indispensable agricultural practice worldwide, serving the survival of half of the global population. Nitrogen transformation (e.g., nitrification) in soil as well as plant N uptake releases protons and increases soil acidification. Neutralizing this acidity in carbonate-containing soils (7.49 × 10 9  ha; ca. 54% of the global land surface area) leads to a CO 2 release corresponding to 0.21 kg C per kg of applied N. We here for the first time raise this problem of acidification of carbonate-containing soils and assess the global CO 2 release from pedogenic and geogenic carbonates in the upper 1 m soil depth. Based on a global N-fertilization map and the distribution of soils containing CaCO 3 , we calculated the CO 2 amount released annually from the acidification of such soils to be 7.48 × 10 12  g C/year. This level of continuous CO 2 release will remain constant at least until soils are fertilized by N. Moreover, we estimated that about 273 × 10 12  g CO 2 -C are released annually in the same process of CaCO 3 neutralization but involving liming of acid soils. These two CO 2 sources correspond to 3% of global CO 2 emissions by fossil fuel combustion or 30% of CO 2 by land-use changes. Importantly, the duration of CO 2 release after land-use changes usually lasts only 1-3 decades before a new C equilibrium is reached in soil. In contrast, the CO 2 released by CaCO 3 acidification cannot reach equilibrium, as long as N fertilizer is applied until it becomes completely neutralized. As the CaCO 3 amounts in soils, if present, are nearly unlimited, their complete dissolution and CO 2 release will take centuries or even millennia. This emphasizes the necessity of preventing soil acidification in N-fertilized soils as an effective strategy to inhibit millennia of CO 2 efflux to the atmosphere. Hence, N fertilization should be strictly calculated based on plant-demand, and overfertilization should be avoided not only

Calcium Carbonate Precipitation for CO{sub 2} Storage and Utilization: A Review of the Carbonate Crystallization and Polymorphism

Energy Technology Data Exchange (ETDEWEB)

Chang, Ribooga; Kim, Semin; Lee, Seungin; Choi, Soyoung; Kim, Minhee; Park, Youngjune, E-mail: young@gist.ac.kr [Carbon and Energy Systems, School of Earth Sciences and Environmental Engineering, Gwangju Institute of Science and Technology (GIST), Gwangju (Korea, Republic of)

2017-07-10

The transformation of CO{sub 2} into a precipitated mineral carbonate through an ex situ mineral carbonation route is considered a promising option for carbon capture and storage (CCS) since (i) the captured CO{sub 2} can be stored permanently and (ii) industrial wastes (i.e., coal fly ash, steel and stainless-steel slags, and cement and lime kiln dusts) can be recycled and converted into value-added carbonate materials by controlling polymorphs and properties of the mineral carbonates. The final products produced by the ex situ mineral carbonation route can be divided into two categories—low-end high-volume and high-end low-volume mineral carbonates—in terms of their market needs as well as their properties (i.e., purity). Therefore, it is expected that this can partially offset the total cost of the CCS processes. Polymorphs and physicochemical properties of CaCO{sub 3} strongly rely on the synthesis variables such as temperature, pH of the solution, reaction time, ion concentration and ratio, stirring, and the concentration of additives. Various efforts to control and fabricate polymorphs of CaCO{sub 3} have been made to date. In this review, we present a summary of current knowledge and recent investigations entailing mechanistic studies on the formation of the precipitated CaCO{sub 3} and the influences of the synthesis factors on the polymorphs.

Reactivation properties of carbide slag as a CO{sub 2} sorbent during calcination/carbonation cycles

Energy Technology Data Exchange (ETDEWEB)

Li, Yingjie; Sun, Rongyue; Liu, Hongling; Lu, Chunmei [Shandong Univ., Jinan (China). School of Energy and Power Engineering

2013-07-01

The carbide slag from polyvinyl chloride production as industry hazardous wastes was proposed as CO{sub 2} sorbent at high temperature in calcium looping cycle. The cyclic CO{sub 2} capture behavior and the microstructure characteristics of the carbide slag as one of the typical calcium-based industrial wastes during the multiple calcination/carbonation cycles. Also, the comparisons between the carbide slag and the natural limestone in cyclic CO{sub 2} capture behavior were made. XRD analysis demonstrates that the predominating constituent of the carbide slag is Ca(OH){sub 2}. The carbonation temperature ranging from 650 to 700 C is favourable to cyclic carbonation of the carbide slag. The cyclic carbonation conversions of the carbide slag is lower than that of the limestone before a certain time, but the situation is converse after that time in a thermogravimetric analyzer. The carbide slag has better cyclic CO{sub 2} capture capacity. The carbonation conversion of the carbide slag retains 0.28 after 100 calcination/carbonation cycles, while the two limestones achieve 0.08 and 0.14 respectively at the same reaction conditions in a dual fixed-bed reactor. The microstructure of the carbide slag by SEM reveals the reason why it possesses better CO{sub 2} capture capacity.

Impact of CO_2 on the Evolution of Microbial Communities Exposed to Carbon Storage Conditions, Enhanced Oil Recovery, and CO_2 Leakage

International Nuclear Information System (INIS)

Gulliver, Djuna M.; Gregory, Kelvin B.; Lowry, Gregory V.

2016-01-01

Geologic carbon storage (GCS) is a crucial part of a proposed mitigation strategy to reduce the anthropogenic carbon dioxide (CO_2) emissions to the atmosphere. During this process, CO_2 is injected as super critical carbon dioxide (SC-CO_2) in confined deep subsurface storage units, such as saline aquifers and depleted oil reservoirs. The deposition of vast amounts of CO_2 in subsurface geologic formations could unintentionally lead to CO_2 leakage into overlying freshwater aquifers. Introduction of CO_2 into these subsurface environments will greatly increase the CO_2 concentration and will create CO_2 concentration gradients that drive changes in the microbial communities present. While it is expected that altered microbial communities will impact the biogeochemistry of the subsurface, there is no information available on how CO_2 gradients will impact these communities. The overarching goal of this project is to understand how CO_2 exposure will impact subsurface microbial communities at temperatures and pressures that are relevant to GCS and CO_2 leakage scenarios. To meet this goal, unfiltered, aqueous samples from a deep saline aquifer, a depleted oil reservoir, and a fresh water aquifer were exposed to varied concentrations of CO_2 at reservoir pressure and temperature. The microbial ecology of the samples was examined using molecular, DNA-based techniques. The results from these studies were also compared across the sites to determine any existing trends. Results reveal that increasing CO_2 leads to decreased DNA concentrations regardless of the site, suggesting that microbial processes will be significantly hindered or absent nearest the CO_2 injection/leakage plume where CO_2 concentrations are highest. At CO_2 exposures expected downgradient from the CO_2 plume, selected microorganisms emerged as dominant in the CO_2 exposed conditions. Results suggest that the altered microbial community was site specific and highly dependent on pH. The site

Forgotten carbon: indirect CO2 in greenhouse gas emission inventories

International Nuclear Information System (INIS)

Gillenwater, Michael

2008-01-01

National governments that are Parties to the United Nations Framework Convention on Climate Change (UNFCCC) are required to submit greenhouse gas (GHG) inventories accounting for the emissions and removals occurring within their geographic territories. The Intergovernmental Panel on Climate Change (IPCC) provides inventory methodology guidance to the Parties of the UNFCCC. This methodology guidance, and national inventories based on it, omits carbon dioxide (CO 2 ) from the atmospheric oxidation of methane, carbon monoxide, and non-methane volatile organic compounds emissions that result from several source categories. The inclusion of this category of 'indirect' CO 2 in GHG inventories increases global anthropogenic emissions (excluding land use and forestry) between 0.5 and 0.7%. However, the effect of inclusion on aggregate UNFCCC Annex I Party GHG emissions would be to reduce the growth of total emissions, from 1990 to 2004, by 0.2% points. The effect on the GHG emissions and emission trends of individual countries varies. The paper includes a methodology for calculating these emissions and discusses uncertainties. Indirect CO 2 is equally relevant for GHG inventories at other scales, such as global, regional, organizational, and facility. Similarly, project-based methodologies, such as those used under the Clean Development Mechanism, may need revising to account for indirect CO 2

Room temperature CO and H2 sensing with carbon nanoparticles

International Nuclear Information System (INIS)

Kim, Daegyu; Pikhitsa, Peter V; Yang, Hongjoo; Choi, Mansoo

2011-01-01

We report on a shell-shaped carbon nanoparticle (SCNP)-based gas sensor that reversibly detects reducing gas molecules such as CO and H 2 at room temperature both in air and inert atmosphere. Crystalline SCNPs were synthesized by laser-assisted reactions in pure acetylene gas flow, chemically treated to obtain well-dispersed SCNPs and then patterned on a substrate by the ion-induced focusing method. Our chemically functionalized SCNP-based gas sensor works for low concentrations of CO and H 2 at room temperature even without Pd or Pt catalysts commonly used for splitting H 2 molecules into reactive H atoms, while metal oxide gas sensors and bare carbon-nanotube-based gas sensors for sensing CO and H 2 molecules can operate only at elevated temperatures. A pristine SCNP-based gas sensor was also examined to prove the role of functional groups formed on the surface of functionalized SCNPs. A pristine SCNP gas sensor showed no response to reducing gases at room temperature but a significant response at elevated temperature, indicating a different sensing mechanism from a chemically functionalized SCNP sensor.

Carbon deposition and sulfur poisoning during CO2 electrolysis in nickel-based solid oxide cell electrodes

Science.gov (United States)

Skafte, Theis Løye; Blennow, Peter; Hjelm, Johan; Graves, Christopher

2018-01-01

Reduction of CO2 to CO and O2 in the solid oxide electrolysis cell (SOEC) has the potential to play a crucial role in closing the CO2 loop. Carbon deposition in nickel-based cells is however fatal and must be considered during CO2 electrolysis. Here, the effect of operating parameters is investigated systematically using simple current-potential experiments. Due to variations of local conditions, it is shown that higher current density and lower fuel electrode porosity will cause local carbon formation at the electrochemical reaction sites despite operating with a CO outlet concentration outside the thermodynamic carbon formation region. Attempts at mitigating the issue by coating the composite nickel/yttria-stabilized zirconia electrode with carbon-inhibiting nanoparticles and by sulfur passivation proved unsuccessful. Increasing the fuel electrode porosity is shown to mitigate the problem, but only to a certain extent. This work shows that a typical SOEC stack converting CO2 to CO and O2 is limited to as little as 15-45% conversion due to risk of carbon formation. Furthermore, cells operated in CO2-electrolysis mode are poisoned by reactant gases containing ppb-levels of sulfur, in contrast to ppm-levels for operation in fuel cell mode.

Carbonic anhydrases are upstream regulators of CO2-controlled stomatal movements in guard cells

KAUST Repository

Hu, Honghong

2009-12-13

The continuing rise in atmospheric CO2 causes stomatal pores in leaves to close and thus globally affects CO2 influx into plants, water use efficiency and leaf heat stress. However, the CO2-binding proteins that control this response remain unknown. Moreover, which cell type responds to CO2, mesophyll or guard cells, and whether photosynthesis mediates this response are matters of debate. We demonstrate that Arabidopsis thaliana double-mutant plants in the beta-carbonic anhydrases betaCA1 and betaCA4 show impaired CO2-regulation of stomatal movements and increased stomatal density, but retain functional abscisic-acid and blue-light responses. betaCA-mediated CO2-triggered stomatal movements are not, in first-order, linked to whole leaf photosynthesis and can function in guard cells. Furthermore, guard cell betaca-overexpressing plants exhibit instantaneous enhanced water use efficiency. Guard cell expression of mammalian alphaCAII complements the reduced sensitivity of ca1 ca4 plants, showing that carbonic anhydrase-mediated catalysis is an important mechanism for betaCA-mediated CO2-induced stomatal closure and patch clamp analyses indicate that CO2/HCO3- transfers the signal to anion channel regulation. These findings, together with ht1-2 (ref. 9) epistasis analysis demonstrate that carbonic anhydrases function early in the CO2 signalling pathway, which controls gas-exchange between plants and the atmosphere.

Thermodynamic Data for Geochemical Modeling of Carbonate Reactions Associated with CO2 Sequestration - Literature Review

International Nuclear Information System (INIS)

Krupka, Kenneth M.; Cantrell, Kirk J.; McGrail, B. Peter

2010-01-01

Permanent storage of anthropogenic CO 2 in deep geologic formations is being considered as a means to reduce the concentration of atmospheric CO 2 and thus its contribution to global climate change. To ensure safe and effective geologic sequestration, numerous studies have been completed of the extent to which the CO 2 migrates within geologic formations and what physical and geochemical changes occur in these formations when CO 2 is injected. Sophisticated, computerized reservoir simulations are used as part of field site and laboratory CO 2 sequestration studies. These simulations use coupled multiphase flow-reactive chemical transport models and/or standalone (i.e., no coupled fluid transport) geochemical models to calculate gas solubility, aqueous complexation, reduction/oxidation (redox), and/or mineral solubility reactions related to CO 2 injection and sequestration. Thermodynamic data are critical inputs to modeling geochemical processes. The adequacy of thermodynamic data for carbonate compounds has been identified as an important data requirement for the successful application of these geochemical reaction models to CO 2 sequestration. A review of thermodynamic data for CO 2 gas and carbonate aqueous species and minerals present in published data compilations and databases used in geochemical reaction models was therefore completed. Published studies that describe mineralogical analyses from CO 2 sequestration field and natural analogue sites and laboratory studies were also reviewed to identify specific carbonate minerals that are important to CO 2 sequestration reactions and therefore require thermodynamic data. The results of the literature review indicated that an extensive thermodynamic database exists for CO 2 and CH 4 gases, carbonate aqueous species, and carbonate minerals. Values of Δ f G 298 o and/or log K r,298 o are available for essentially all of these compounds. However, log K r,T o or heat capacity values at temperatures above 298 K exist

A combined methodology using electrical resistivity tomography, ordinary kriging and porosimetry for quantifying total C trapped in carbonate formations associated with natural analogues for CO2 leakage

Science.gov (United States)

Prado-Pérez, A. J.; Aracil, E.; Pérez del Villar, L.

2014-06-01

Currently, carbon deep geological storage is one of the most accepted methods for CO2 sequestration, being the long-term behaviour assessment of these artificial systems absolutely essential to guarantee the safety of the CO2 storage. In this sense, hydrogeochemical modelling is being used for evaluating any artificial CO2 deep geological storage as a potential CO2 sinkhole and to assess the leakage processes that are usually associated with these engineered systems. Carbonate precipitation, as travertines or speleothems, is a common feature in the CO2 leakage scenarios and, therefore, is of the utmost importance to quantify the total C content trapped as a stable mineral phase in these carbonate formations. A methodology combining three classical techniques such as: electrical resistivity tomography, geostatistical analysis and mercury porosimetry is described in this work, which was developed for calculating the total amount of C trapped as CaCO3 associated with the CO2 leakages in Alicún de las Torres natural analogue (Granada, Spain). The proposed methodology has allowed estimating the amount of C trapped as calcite, as more than 1.7 Mt. This last parameter, focussed on an artificial CO2 deep geological storage, is essential for hydrogeochemical modellers when evaluating whether CO2 storages constitute or not CO2 sinkholes. This finding is extremely important when assessing the long-term behaviour and safety of any artificial CO2 deep geological storage.