WorldWideScience

Sample records for co2 mineral carbonation

  1. 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

  2. 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

  3. 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

  4. 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

  5. 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.

  6. 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

  7. How much CO2 is trapped in carbonate minerals of a natural CO2 occurrence?

    Science.gov (United States)

    Király, Csilla; Szabó, Zsuzsanna; Szamosfalvi, Ágnes; Cseresznyés, Dóra; Király, Edit; Szabó, Csaba; Falus, György

    2017-04-01

    Carbon Capture and Storage (CCS) is a transitional technology to decrease CO2 emissions from human fossil fuel usage and, therefore, to mitigate climate change. The most important criteria of a CO2 geological storage reservoir is that it must hold the injected CO2 for geological time scales without its significant seepage. The injected CO2 undergoes physical and chemical reactions in the reservoir rocks such as structural-stratigraphic, residual, dissolution or mineral trapping mechanisms. Among these, the safest is the mineral trapping, when carbonate minerals such as calcite, ankerite, siderite, dolomite and dawsonite build the CO2 into their crystal structures. The study of natural CO2 occurrences may help to understand the processes in CO2 reservoirs on geological time scales. This is the reason why the selected, the Mihályi-Répcelak natural CO2 occurrence as our research area, which is able to provide particular and highly significant information for the future of CO2 storage. The area is one of the best known CO2 fields in Central Europe. The main aim of this study is to estimate the amount of CO2 trapped in the mineral phase at Mihályi-Répcelak CO2 reservoirs. For gaining the suitable data, we apply petrographic, major and trace element (microprobe and LA-ICP-MS) and stable isotope analysis (mass spectrometry) and thermodynamic and kinetic geochemical models coded in PHREEQC. Rock and pore water compositions of the same formation, representing the pre-CO2 flooding stages of the Mihályi-Répcelak natural CO2 reservoirs are used in the models. Kinetic rate parameters are derived from the USGS report of Palandri and Kharaka (2004). The results of petrographic analysis show that a significant amount of dawsonite (NaAlCO3(OH)2, max. 16 m/m%) precipitated in the rock due to its reactions with CO2 which flooded the reservoir. This carbonate mineral alone traps about 10-30 kg/m3 of the reservoir rock from the CO2 at Mihályi-Répcelak area, which is an

  8. 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

  9. 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)

  10. 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

  11. 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

  12. 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

  13. 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.

  14. 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

  15. ATOMIC-LEVEL IMAGING OF CO2 DISPOSAL AS A CARBONATE MINERAL: OPTIMIZING REACTION PROCESS DESIGN; A

    International Nuclear Information System (INIS)

    M.J. McKelvy; R. Sharma; A.V.G. Chizmeshya; H. Bearat; R.W. Carpenter

    2001-01-01

    Fossil fuels, especially coal, can support the energy demands of the world for centuries to come, if the environmental problems associated with CO(sub 2) emissions can be overcome. Permanent and safe methods for CO(sub 2) capture and disposal/storage need to be developed. Mineralization of stationary-source CO(sub 2) emissions as carbonates can provide such safe capture and long-term sequestration. Mg-rich lamellar-hydroxide based minerals (e.g., brucite and serpentine) offer a class of widely available, low-cost materials, with intriguing mineral carbonation potential. Carbonation of such materials inherently involves dehydroxylation, which can disrupt the material down to the atomic level. As such, controlled dehydroxylation, before and/or during carbonation, may provide an important parameter for enhancing carbonation reaction processes. Mg(OH)(sub 2) was chosen as the model material for investigating lamellar hydroxide mineral dehydroxylation/carbonation mechanisms due to (i) its structural and chemical simplicity, (ii) interest in Mg(OH)(sub 2) gas-solid carbonation as a potentially cost-effective CO(sub 2) mineral sequestration process component, and (iii) its structural and chemical similarity to other lamellar-hydroxide-based minerals (e.g., serpentine-based minerals) whose carbonation reaction processes are being explored due to their low-cost CO(sub 2) sequestration potential. Fundamental understanding of the mechanisms that govern dehydroxylation/carbonation processes is essential for minimizing the cost of any lamellar-hydroxide-based mineral carbonation sequestration process. This report covers the third year progress of this grant, as well as providing an integrated overview of the progress in years 1-3, as we have been granted a one-year no-cost extension to wrap up a few studies and publications to optimize project impact

  16. Kinetics of carbonate mineral dissolution in CO2-acidified brines at storage reservoir conditions.

    Science.gov (United States)

    Peng, Cheng; Anabaraonye, Benaiah U; Crawshaw, John P; Maitland, Geoffrey C; Trusler, J P Martin

    2016-10-20

    We report experimental measurements of the dissolution rate of several carbonate minerals in CO 2 -saturated water or brine at temperatures between 323 K and 373 K and at pressures up to 15 MPa. The dissolution kinetics of pure calcite were studied in CO 2 -saturated NaCl brines with molalities of up to 5 mol kg -1 . The results of these experiments were found to depend only weakly on the brine molality and to conform reasonably well with a kinetic model involving two parallel first-order reactions: one involving reactions with protons and the other involving reaction with carbonic acid. The dissolution rates of dolomite and magnesite were studied in both aqueous HCl solution and in CO 2 -saturated water. For these minerals, the dissolution rates could be explained by a simpler kinetic model involving only direct reaction between protons and the mineral surface. Finally, the rates of dissolution of two carbonate-reservoir analogue minerals (Ketton limestone and North-Sea chalk) in CO 2 -saturated water were found to follow the same kinetics as found for pure calcite. Vertical scanning interferometry was used to study the surface morphology of unreacted and reacted samples. The results of the present study may find application in reactive-flow simulations of CO 2 -injection into carbonate-mineral saline aquifers.

  17. Evaluation of Southern Quebec asbestos residues for CO2 sequestration by mineral carbonation

    Energy Technology Data Exchange (ETDEWEB)

    Beaudoin, G.; Hebert, R.; Constantin, M. [Laval Univ., Quebec City, PQ (Canada); Bonin, G. [LAB Chrysotile Inc., Black Lake, PQ (Canada); Dipple, G. [British Columbia Univ., Vancouver, BC (Canada)

    2003-08-01

    One alternative to help reduce carbon dioxide (CO{sub 2}) levels in the atmosphere is to sequester CO{sub 2} 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. Three CO{sub 2} sinks exist in southern Quebec use such silicates. They are: (1) asbestos mill residues, (2) associated mine waste, and (3) ultramafic bedrock. Extraction of asbestos in the region has been accomplished 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.

  18. 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

  19. 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

  20. 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

  1. Cost Evaluation of CO2 Sequestration by Aqueous Mineral Carbonation

    NARCIS (Netherlands)

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

    2007-01-01

    A cost evaluation of CO2 sequestration by aqueous mineral carbonation has been made using either wollastonite (CaSiO3) 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

  2. Mineral CO2 sequestration in alkaline solid residues

    International Nuclear Information System (INIS)

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

    2004-12-01

    Mineral carbonation is a promising sequestration route for the permanent and safe storage of carbon dioxide. In addition to calcium- or magnesium-containing primary minerals, suitable alkaline solid residues can be used as feedstock. The use of alkaline residues has several advantages, such as their availability close to CO2 sources and their higher reactivity for carbonation than primary minerals. In addition, the environmental quality of residues can potentially be improved by carbonation. In this study, key factors of the mineral CO2 sequestration process are identified, their influence on the carbonation process is examined, and environmental properties of the reaction products with regard to their possible beneficial utilization are investigated. The use of alkaline solid residues forms a potentially attractive alternative for the first mineral sequestration plants

  3. 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.

  4. CO2 emissions: mineral carbonation and Finnish pulp and paper industry (CO2 Nordic Plus) and use of serpentinites in energy and metal industry (ECOSERP)

    International Nuclear Information System (INIS)

    Fogelholm, C.-J.; Raiski, T.; Teir, S.

    2007-01-01

    Abstract Mineral carbonation has been investigated at Helsinki University of Technology (TKK), laboratory of energy engineering and environmental protection since year 2000. The Finnish Technology Agency Tekes and the Finnish Recovery Boiler Committee are funding through the ClimBus technology programme, in conjunction with the Nordic Energy Research Programme, the research regarding the application of ex situ mineral carbonation processes. One aspect is to verify the possible use of mineral carbonation for the separation, utilisation and long-term storage of carbon dioxide (CO 2 ) in the pulp and paper industry. The Geological Survey of Finland (GTK) has been screening since 2004 the location, quality and suitability of the Finnish processed serpentine and stoped serpentinite storage of mines and in situ serpentinite bodies of ultramafic rock formations for mineral carbonation of CO 2 . Tekes and the GTK are funding development work through the ClimBus technology programme on the utilisation of serpentine and serpentinite for CO 2 sequestration purposes, based on economical and environmental evaluation of mineral and mining processing operations. Also the options for other use of serpentine and serpentinite are evaluated. The most promising magnesium- and calcium-based sources for carbonation are by-products of mining processes of ultramafic rocks (such as serpentinites and serpentine) and steelmaking slags. Carbonated minerals could possibly be used as paper coating materials (PCC), fillers or construction materials. For magnesium carbonate new markets and applications must be developed. (orig.)

  5. Carbon Mineralization by Aqueous Precipitation for Beneficial Use of CO2 from Flue Gas

    Energy Technology Data Exchange (ETDEWEB)

    Devenney, Martin; Gilliam, Ryan; Seeker, Randy

    2014-06-01

    The objective of this project is to demonstrate an innovative process to mineralize CO2 from flue gas directly to reactive carbonates and maximize the value and versatility of its beneficial use products. The program scope includes the design, construction, and testing of a CO2 Conversion to Material Products (CCMP) Pilot Demonstration Plant utilizing CO2 from the flue gas of a power production facility in Moss Landing, CA as well as flue gas from coal combustion. This topical report covers Phase 2b, which is the construction phase of pilot demonstration subsystems that make up the integrated plant. The subsystems included are the mineralization subsystem, the Alkalinity Based on Low Energy (ABLE) subsystem, the waste calcium oxide processing subsystem, and the fiber cement board production subsystem. The fully integrated plant is now capable of capturing CO2 from various sources (gas and coal) and mineralizing into a reactive calcium carbonate binder and subsequently producing commercial size (4ftx8ft) fiber cement boards. The topical report provides a description of the “as built” design of these subsystems and the results of the commissioning activities that have taken place to confirm operability. At the end of Phase 2b, the CCMP pilot demonstration is fully ready for testing.

  6. Carbonate mineral solubility at low temperatures in the Na-K-Mg-Ca-H-Cl-SO 4-OH-HCO 3-CO 3-CO 2-H 2O system

    Science.gov (United States)

    Marion, Giles M.

    2001-06-01

    Carbonate minerals have played an important role in the geochemical evolution of Earth, and may have also played an important role in the geochemical evolution of Mars and Europa. Several models have been published in recent years that describe chloride and sulfate mineral solubilities in concentrated brines using the Pitzer equations. Few of these models are parameterized for subzero temperatures, and those that are do not include carbonate chemistry. The objectives of this work are to estimate Pitzer-equation bicarbonate-carbonate parameters and carbonate mineral solubility products and to incorporate them into the FREZCHEM model to predict carbonate mineral solubilities in the Na-K-Mg-Ca-H-Cl-SO 4-OH-HCO 3-CO 3-CO 2-H 2O system at low temperatures (≤25°C) with a special focus on subzero temperatures. Most of the Pitzer-equation parameters and equilibrium constants are taken from the literature and extrapolated into the subzero temperature range. Solubility products for 14 sodium, potassium, magnesium, and calcium bicarbonate and carbonate minerals are included in the model. Most of the experimental data are at temperatures ≥ -8°C; only for the NaHCO 3-NaCl-H 2O and Na 2CO 3-NaCl-H 2O systems are there bicarbonate and carbonate data to temperatures as low as -21.6°C. In general, the fit of the model to the experimental data is good. For example, calculated eutectic temperatures and compositions for NaHCO 3, Na 2CO 3, and their mixtures with NaCl and Na 2SO 4 salts are in good agreement with experimental data to temperatures as low as -21.6°C. Application of the model to eight saline, alkaline carbonate waters give predicted pHs ranging from 9.2 to 10.2, in comparison with measured pHs that range from 8.7 to 10.2. The model suggests that the CaCO 3 mineral that precipitates during seawater freezing is probably calcite and not ikaite. The model demonstrates that a proposed salt assemblage for the icy surface of Europa consisting of highly hydrated MgSO 4

  7. 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.

  8. Dissolved organic carbon and nitrogen mineralization strongly affect co2 emissions following lime application to acidic soil

    International Nuclear Information System (INIS)

    Shaaban, M.; Peng, Q.; Lin, S.; Wu, Y.

    2014-01-01

    Emission of greenhouse gases from agricultural soils has main contribution to the climatic change and global warming. Dynamics of dissolved organic carbon (DOC) and nitrogen mineralization can affect CO/sub 2/ emission from soils. Influence of DOC and nitrogen mineralization on CO/sub 2/ emissions following lime application to acidic soil was investigated in current study. Laboratory experiment was conducted under aerobic conditions with 25% moisture contents (66% water-filled pore space) at 25 degree C in the dark conditions. Different treatments of lime were applied to acidic soil as follows: CK (control), L (low rate of lime: 0.2g lime / 100 g soil) and H (high rate of lime: 0.5g lime /100g soil). CO/sub 2/ emissions were measured by gas chromatography and dissolved organic carbon, NH4 +-N, NO/sub 3/ --N and soil pH were measured during incubation study. Addition of lime to acidic soil significantly increased the concentration of DOC and N mineralization rate. Higher concentrations of DOC and N mineralization, consequently, increased the CO/sub 2/ emissions from lime treated soils. Cumulative CO/sub 2/ emission was 75% and 71% higher from L and H treatments as compared to CK. The results of current study suggest that DOC and N mineralization are critical in controlling gaseous emissions of CO/sub 2/ from acidic soils following lime application. (author)

  9. 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

  10. Mineralization of Carbon Dioxide: Literature Review

    Energy Technology Data Exchange (ETDEWEB)

    Romanov, V; Soong, Y; Carney, C; Rush, G; Nielsen, B; O' Connor, W

    2015-01-01

    CCS research has been focused on CO2 storage in geologic formations, with many potential risks. An alternative to conventional geologic storage is carbon mineralization, where CO2 is reacted with metal cations to form carbonate minerals. Mineralization methods can be broadly divided into two categories: in situ and ex situ. In situ mineralization, or mineral trapping, is a component of underground geologic sequestration, in which a portion of the injected CO2 reacts with alkaline rock present in the target formation to form solid carbonate species. In ex situ mineralization, the carbonation reaction occurs above ground, within a separate reactor or industrial process. This literature review is meant to provide an update on the current status of research on CO2 mineralization. 2

  11. Carbon Mineralization by Aqueous Precipitation for Beneficial Use of CO2 from Flue Gas

    Energy Technology Data Exchange (ETDEWEB)

    Devenney, Martin [Calera Corporation, Moss Landing, CA (United States); Gilliam, Ryan [Calera Corporation, Moss Landing, CA (United States); Seeker, Randy [Calera Corporation, Moss Landing, CA (United States)

    2015-06-30

    The objective of this project was to demonstrate an innovative process to mineralize CO2 from flue gas directly to reactive carbonates and maximize the value and versatility of its beneficial use products. The program scope includes the design, construction, and testing of a CO2 Conversion to Material Products (CCMP) Pilot Demonstration Plant utilizing CO2 from the flue gas of a power production facility in Moss Landing, CA as well as flue gas from coal combustion. This final report details all development, analysis, design and testing of the project. Also included in the final report are an updated Techno-Economic Analysis and CO2 Lifecycle Analysis. The subsystems included in the pilot demonstration plant are the mineralization subsystem, the Alkalinity Based on Low Energy (ABLE) subsystem, the waste calcium oxide processing subsystem, and the fiber cement board production subsystem. The fully integrated plant was proven to be capable of capturing CO2 from various sources (gas and coal) and mineralizing it into a reactive calcium carbonate binder and subsequently producing commercial size (4ftx8ft) fiber cement boards. The final report provides a description of the “as built” design of these subsystems and the results of the commissioning activities that have taken place to confirm operability. The report also discusses the results of the fully integrated operation of the facility. Fiber cement boards have been produced in this facility exclusively using reactive calcium carbonate from captured CO2 from flue gas. These boards meet all US and China appropriate acceptance standards. Use demonstrations for these boards are now underway.

  12. CO{sub 2} Energy Reactor – Integrated Mineral Carbonation: Perspectives on Lab-Scale Investigation and Products Valorization

    Energy Technology Data Exchange (ETDEWEB)

    Santos, Rafael M., E-mail: rafael.santos@alumni.utoronto.ca [Chemical and Environmental Laboratories (CEL), School of Applied Chemical and Environmental Sciences, Sheridan Institute of Technology, Brampton, ON (Canada); Knops, Pol C. M.; Rijnsburger, Keesjan L. [Innovation Concepts B.V., Twello (Netherlands); Chiang, Yi Wai [School of Engineering, University of Guelph, Guelph, ON (Canada)

    2016-02-15

    To overcome the challenges of mineral CO{sub 2} sequestration, Innovation Concepts B.V. is developing a unique proprietary gravity pressure vessel (GPV) reactor technology and has focussed on generating reaction products of high economic value. The GPV provides intense process conditions through hydrostatic pressurization and heat exchange integration that harvests exothermic reaction energy, thereby reducing energy demand of conventional reactor designs, in addition to offering other benefits. In this paper, a perspective on the status of this technology and outlook for the future is provided. To date, laboratory-scale tests of the envisioned process have been performed in a tubular “rocking autoclave” reactor. The mineral of choice has been olivine [~Mg{sub 1.6}Fe{sup 2+}{sub 0.4}(SiO{sub 4}) + ppm Ni/Cr], although asbestos, steel slags, and oil shale residues are also under investigation. The effect of several process parameters on reaction extent and product properties has been tested: CO{sub 2} pressure, temperature, residence time, additives (buffers, lixiviants, chelators, oxidizers), solids loading, and mixing rate. The products (carbonates, amorphous silica, and chromite) have been physically separated (based on size, density, and magnetic properties), characterized (for chemistry, mineralogy, and morphology), and tested in intended applications (as pozzolanic carbon-negative building material). Economically, it is found that product value is the main driver for mineral carbonation, rather than, or in addition to, the sequestered CO{sub 2}. The approach of using a GPV and focusing on valuable reaction products could thus make CO{sub 2} mineralization a feasible and sustainable industrial process.

  13. Experimental Studies on the Interaction of scCO2 and scCO2-SO2 With Rock Forming Minerals at Conditions of Geologic Carbon Storages - First Results

    Science.gov (United States)

    Erzinger, J.; Wilke, F.; Wiersberg, T.; Vasquez Parra, M.

    2010-12-01

    Co-injection of SO2 (plus possibly NOx and O2) during CO2 storage in deep saline aquifers may cause stronger brine acidification than CO2 alone. Because of that, we investigate chemical corrosion of rocks and rock-forming minerals with impure supercritical CO2 (scCO2) at possible storage conditions of >73.7 bar and >31°C. Contaminates were chosen with respect to the composition of CO2 captured industrially from coal-fired power plants using the oxyfuel technology. The resulting data should build a base for the long-term prediction of the behavior of CO2 in geologic storage reservoirs. Experiments of up to 1000 hrs duration have been performed with 10 natural mineral concentrates (calcite, dolomite, siderite, anhydrite, hematite, albite, microcline, kaolinite, muscovite, biotite) in 3n NaCl solution and pure scCO2 or scCO2+SO2 (99.5+0.5 vol%). The NaCl reaction fluid resembles the average salinity of deep formation waters of the North German Basin and is not free of oxygen. To increase reaction rates all minerals were ground and the reagents agitated either by stirring or shaking in autoclaves of about one liter in volume. The autoclaves consist of Hastelloy™ or ferromagnetic stainless steel fully coated with PTFE. We used in average 15 g of solids, 700 ml liquid, and the vessels were pressurized up to 100 bars with CO2 or CO2-SO2 mixture. Experiments were run at temperatures up to 90°C. Before, during and after the experiments small amounts fluids were sampled and analyzed for dissolved constituents and pH. Solid phases were characterized by XRF, XRD, and EMPA before and after the experiments. Pure scCO2 corrodes all carbonates, reacts only slightly with anhydrite, albite, and microcline at a minimum pH of 4, and does not recognizably interact with the others. After the experiment, albite has gained in a, not yet fully identified, carbonate phase which might be dawsonite. Reaction fluids of the experiments with scCO2+SO2 have mostly lower pH than using scCO2

  14. Carbon dioxide sequestration by direct mineral carbonation with carbonic acid

    Energy Technology Data Exchange (ETDEWEB)

    O' Connor, W.K.; Dahlin, D.C.; Nilsen, D.N.; Walters, R.P.; Turner, P.C.

    2000-07-01

    The Albany Research Center (ARC) of the US Department of Energy (DOE) has been conducting a series of mineral carbonation tests at its Albany, Oregon, facility over the past 2 years as part of a Mineral Carbonation Study Program within the DOE. The ARC tests have focused on ex-situ mineral carbonation in an aqueous system. The process developed at ARC utilizes a slurry of water mixed with a magnesium silicate mineral, olivine [forsterite and member (mg{sub 2}SiO{sub 4})], or serpentine [Mg{sub 3}Si{sub 2}O{sub 5}(OH){sub 4}]. This slurry is reacted with supercritical carbon dioxide (CO{sub 2}) to produce magnesite (MgCO{sub 3}). The CO{sub 2} is dissolved in water to form carbonic acid (H{sub 2}CO{sub 3}), which dissociates to H{sup +} and HCO{sub 3}{sup {minus}}. The H{sup +} reacts with the mineral, liberating Mg{sup 2+} cations which react with the bicarbonate to form the solid carbonate. The process is designed to simulate the natural serpentinization reaction of ultramafic minerals, and for this reason, these results may also be applicable to in-situ geological sequestration regimes. Results of the baseline tests, conducted on ground products of the natural minerals, have been encouraging. Tests conducted at ambient temperature (22 C) and subcritical CO{sub 2} pressures (below 73 atm) resulted in very slow conversion to the carbonate. However, when elevated temperatures and pressures are utilized, coupled with continuous stirring of the slurry and gas dispersion within the water column, significant reaction occurs within much shorter reaction times. Extent of reaction, as measured by the stoichiometric conversion of the silicate mineral (olivine) to the carbonate, is roughly 90% within 24 hours, using distilled water, and a reaction temperature of 185 C and a partial pressure of CO{sub 2} (P{sub CO{sub 2}}) of 115 atm. Recent tests using a bicarbonate solution, under identical reaction conditions, have achieved roughly 83% conversion of heat treated serpentine

  15. Carbon dioxide sequestration by mineral carbonation

    NARCIS (Netherlands)

    Huijgen, W.J.J.

    2007-01-01

    The increasing atmospheric carbon dioxide (CO2) concentration, mainly caused by fossil fuel combustion, has lead to concerns about global warming. A possible technology that can contribute to the reduction of carbon dioxide emissions is CO2 sequestration by mineral carbonation. The basic concept

  16. Microbe-driven turnover offsets mineral-mediated storage of soil carbon under elevated CO2

    Science.gov (United States)

    Sulman, Benjamin N.; Phillips, Richard P.; Oishi, A. Christopher; Shevliakova, Elena; Pacala, Stephen W.

    2014-12-01

    The sensitivity of soil organic carbon (SOC) to changing environmental conditions represents a critical uncertainty in coupled carbon cycle-climate models. Much of this uncertainty arises from our limited understanding of the extent to which root-microbe interactions induce SOC losses (through accelerated decomposition or `priming') or indirectly promote SOC gains (via `protection' through interactions with mineral particles). We developed a new SOC model to examine priming and protection responses to rising atmospheric CO2. The model captured disparate SOC responses at two temperate free-air CO2 enrichment (FACE) experiments. We show that stabilization of `new' carbon in protected SOC pools may equal or exceed microbial priming of `old' SOC in ecosystems with readily decomposable litter and high clay content (for example, Oak Ridge). In contrast, carbon losses induced through priming dominate the net SOC response in ecosystems with more resistant litters and lower clay content (for example, Duke). The SOC model was fully integrated into a global terrestrial carbon cycle model to run global simulations of elevated CO2 effects. Although protected carbon provides an important constraint on priming effects, priming nonetheless reduced SOC storage in the majority of terrestrial areas, partially counterbalancing SOC gains from enhanced ecosystem productivity.

  17. Carbon dioxide sequestration by direct mineral carbonation with carbonic acid

    Energy Technology Data Exchange (ETDEWEB)

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

    2000-01-01

    The Albany Research Center (ARC) of the U.S. Dept. of Energy (DOE) has been conducting a series of mineral carbonation tests at its Albany, Oregon, facility over the past 2 years as part of a Mineral Carbonation Study Program within the DOE. Other participants in this Program include the Los Alamos National Laboratory, Arizona State University, Science Applications International Corporation, and the DOE National Energy Technology Laboratory. The ARC tests have focused on ex-situ mineral carbonation in an aqueous system. The process developed at ARC utilizes a slurry of water mixed with a magnesium silicate mineral, olivine [forsterite end member (Mg2SiO4)], or serpentine [Mg3Si2O5(OH)4]. This slurry is reacted with supercritical carbon dioxide (CO2) to produce magnesite (MgCO3). The CO2 is dissolved in water to form carbonic acid (H2CO3), which dissociates to H+ and HCO3 -. The H+ reacts with the mineral, liberating Mg2+ cations which react with the bicarbonate to form the solid carbonate. The process is designed to simulate the natural serpentinization reaction of ultramafic minerals, and for this reason, these results may also be applicable to in-situ geological sequestration regimes. Results of the baseline tests, conducted on ground products of the natural minerals, have been encouraging. Tests conducted at ambient temperature (22 C) and subcritical CO2 pressures (below 73 atm) resulted in very slow conversion to the carbonate. However, when elevated temperatures and pressures are utilized, coupled with continuous stirring of the slurry and gas dispersion within the water column, significant reaction occurs within much shorter reaction times. Extent of reaction, as measured by the stoichiometric conversion of the silicate mineral (olivine) to the carbonate, is roughly 90% within 24 hours, using distilled water, and a reaction temperature of 185?C and a partial pressure of CO2 (PCO2) of 115 atm. Recent tests using a bicarbonate solution, under identical reaction

  18. In situ mid-infrared spectroscopic titration of forsterite with water in supercritical CO2: Dependence of mineral carbonation on quantitative water speciation

    Science.gov (United States)

    Loring, J. S.; Thompson, C. J.; Wang, Z.; Schaef, H. T.; Martin, P.; Qafoku, O.; Felmy, A. R.; Rosso, K. M.

    2011-12-01

    Geologic sequestration of carbon dioxide holds promise for helping mitigate CO2 emissions generated from the burning of fossil fuels. Supercritical CO2 (scCO2) plumes containing variable water concentrations (wet scCO2) will displace aqueous solution and dominate the pore space adjacent to caprocks. It is important to understand possible mineral reactions with wet scCO2 to better predict long-term caprock integrity. We introduce novel in situ instrumentation that enables quantitative titrations of reactant minerals with water in scCO2 at temperatures and pressures relevant to target geologic reservoirs. The system includes both transmission and attenuated total reflection mid-infrared optics. Transmission infrared spectroscopy is used to measure concentrations of water dissolved in the scCO2, adsorbed on mineral surfaces, and incorporated into precipitated carbonates. Single-reflection attenuated total reflection infrared spectroscopy is used to monitor water adsorption, mineral dissolution, and carbonate precipitation reactions. Results are presented for the infrared spectroscopic titration of forsterite (Mg2SiO4), a model divalent metal silicate, with water in scCO2 at 100 bar and at both 50 and 75°C. The spectral data demonstrate that the quantitative speciation of water as either dissolved or adsorbed is important for understanding the types, growth rates, and amounts of carbonate precipitates formed. Relationships between dissolved/adsorbed water, water concentrations, and the role of liquid-like adsorbed water are discussed. Our results unify previous in situ studies from our laboratory based on infrared spectroscopy, nuclear magnetic resonance spectroscopy and X-ray diffraction.

  19. Numerical simulation of CO2 disposal by mineral trapping in deep aquifers

    International Nuclear Information System (INIS)

    Xu Tianfu; Apps, John A.; Pruess, Karsten

    2004-01-01

    Carbon dioxide disposal into deep aquifers is a potential means whereby atmospheric emissions of greenhouse gases may be reduced. However, our knowledge of the geohydrology, geochemistry, geophysics, and geomechanics of CO 2 disposal must be refined if this technology is to be implemented safely, efficiently, and predictably. As a prelude to a fully coupled treatment of physical and chemical effects of CO 2 injection, the authors have analyzed the impact of CO 2 immobilization through carbonate mineral precipitation. Batch reaction modeling of the geochemical evolution of 3 different aquifer mineral compositions in the presence of CO 2 at high pressure were performed. The modeling considered the following important factors affecting CO 2 sequestration: (1) the kinetics of chemical interactions between the host rock minerals and the aqueous phase, (2) CO 2 solubility dependence on pressure, temperature and salinity of the system, and (3) redox processes that could be important in deep subsurface environments. The geochemical evolution under CO 2 injection conditions was evaluated. In addition, changes in porosity were monitored during the simulations. Results indicate that CO 2 sequestration by matrix minerals varies considerably with rock type. Under favorable conditions the amount of CO 2 that may be sequestered by precipitation of secondary carbonates is comparable with and can be larger than the effect of CO 2 dissolution in pore waters. The precipitation of ankerite and siderite is sensitive to the rate of reduction of Fe(III) mineral precursors such as goethite or glauconite. The accumulation of carbonates in the rock matrix leads to a considerable decrease in porosity. This in turn adversely affects permeability and fluid flow in the aquifer. The numerical experiments described here provide useful insight into sequestration mechanisms, and their controlling geochemical conditions and parameters

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

    Energy Technology Data Exchange (ETDEWEB)

    Bryan, Charles R.; Dewers, Thomas A.; Heath, Jason E.; Wang, Yifeng; Matteo, Edward N.; Meserole, Stephen P.; Tallant, David Robert

    2013-09-01

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

  1. CO2 emissions: mineral carbonation and Finnish pulp and paper industry (CONordicPlus) and use of serpentinites in energy and metal industry (ECOSERP)

    International Nuclear Information System (INIS)

    Fogelholm, C.J.; Raiski, T.; Teir, S.

    2006-01-01

    Mineral carbonation has been investigated at Helsinki University of Technology (TKK), laboratory of energy engineering and environmental protection since year 2000. The Finnish Technology Agency Tekes and the Finnish Recovery Boiler Committee are funding through the ClimBus technology programme, in conjunction with the Nordic Energy Research Programme, the research regarding the application of ex situ mineral carbonation processes. One aspect is to verify the possible use of mineral carbonation for the separation, utilisation and long-term storage of carbon dioxide (CO2) in the pulp and paper industry. The Geological Survey of Finland (GTK) has been screening since 2004 the location, quality and suitability of the Finnish processed serpentine and stopped serpentinite storage of mines and in situ serpentinite bodies of ultramafic rock formations for mineral carbonation of CO2. Tekes and the GTK are funding development work through the ClimBus technology programme on the utilisation of serpentine and serpentinite for CO2 sequestration purposes, based on economical and environmental evaluation of mineral and mining processing operations. Also the options for other use of serpentine and serpentinite are evaluated. The most promising magnesium and calcium-based sources for carbonation are by products of mining processes of ultramafic rocks (such as serpentinites and serpentine) and steelmaking slags. Carbonated minerals could possibly be used as paper coating materials (PCC), fillers or construction materials. For magnesium carbonate new markets and applications must be developed. (orig.)

  2. Analysis of mineral trapping for CO{sub 2} disposal in deep aquifers

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Tianfu; Apps, John A.; Pruess, Karsten

    2001-07-20

    CO{sub 2} disposal into deep aquifers has been suggested as a potential means whereby atmospheric emissions of greenhouse gases may be reduced. However, our knowledge of the geohydrology, geochemistry, geophysics, and geomechanics of CO{sub 2} disposal must be refined if this technology is to be implemented safely, efficiently, and predictably. As a prelude to a fully coupled treatment of physical and chemical effects of CO{sub 2} injection, we have analyzed the impact of CO{sub 2} immobilization through carbonate precipitation. A survey of all major classes of rock-forming minerals, whose alteration would lead to carbonate precipitation, indicated that very few minerals are present in sufficient quantities in aquifer host rocks to permit significant sequestration of CO{sub 2}. We performed batch reaction modeling of the geochemical evolution of three different aquifer mineralogies in the presence of CO{sub 2} at high pressure. Our modeling considered (1) redox processes that could be important in deep subsurface environments, (2) the presence of organic matter, (3) the kinetics of chemical interactions between the host rock minerals and the aqueous phase, and (4) CO{sub 2} solubility dependence on pressure, temperature and salinity of the system. The geochemical evolution under both natural background and CO{sub 2} injection conditions was evaluated. In addition, changes in porosity were monitored during the simulations. Results indicate that CO{sub 2} sequestration by matrix minerals varies considerably with rock type. Under favorable conditions the amount of CO{sub 2} that may be sequestered by precipitation of secondary carbonates is comparable with and can be larger than the effect of CO{sub 2} dissolution in pore waters. The precipitation of ankerite and siderite is sensitive to the rate of reduction of ferric mineral precursors such as glauconite, which in turn is dependent on the reactivity of associated organic material. The accumulation of carbonates in

  3. 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

  4. Review of CO2 Reduction Technologies using Mineral Carbonation of Iron and Steel Making Slag in Malaysia

    Science.gov (United States)

    Norhana Selamat, Siti; Nor, Nik Hisyamudin Muhd; Rashid, Muhammad Hanif Abdul; Fauzi Ahmad, Mohd; Mohamad, Fariza; Ismail, Al Emran; Fahrul Hassan, Mohd; Turan, Faiz Mohd; Zain, Mohd Zamzuri Mohd; Abu Bakar, Elmi; Seiji, Yokoyama

    2017-10-01

    Climate change, greenhouse gas effect, and global warming is envisioning to turn more awful and more terrible by year. Since the leading cause of global warming is uncontrolled CO2 in atmosphere. The amount of unused steel slag is expected to increment later on, steel industries is one of the mechanical industries that contribute the CO2 emission. That because this businesses deliver carbon in light of powers reductant and substantial volume of steel. The changes of atmosphere these day is truly developing concern and that make steel creator are confronted with test of discovering methods for bringing down CO2 emission. Malaysia is working decidedly in the diminishment of CO2 gas. There are a few techniques in decreasing the amount of CO2 in the air as underlined by the Intergovernmental Panel of Climate Change (IPCC), an organization under the United Country however CCS is an extremely encouraging innovation to moderate CO2 emission in air. Mineral carbonation is another technique to store carbon dioxide permanently, long term stability and vast capacity.

  5. Experimental and simulation studies on mineral trapping of CO2 with brine

    International Nuclear Information System (INIS)

    Soong, Y.; Goodman, A.L.; McCarthy-Jones, J.R.; Baltrus, J.P.

    2004-01-01

    The reaction of carbon dioxide (CO 2 ) with brine samples collected from the Oriskany Formation in Indiana County, PA, was investigated in an autoclave reactor under various conditions. A geochemical code, PHREEQC, was used as to simulate the reaction in the autoclave reactor. The combined experimental and modeling data suggests that pH (pH > 9) plays a key role in the formation of carbonate minerals. The effects of temperature and CO 2 pressure have a lesser impact on the formation of carbonate minerals

  6. Experiment and simulation study on the effects of cement minerals on the water-rock-CO2 interaction during CO2 geological storage

    Science.gov (United States)

    Liu, N.; Cheng, J.

    2016-12-01

    The CO2 geological storage is one of the most promising technology to mitigate CO2 emission. The fate of CO2 underground is dramatically affected by the CO2-water-rock interaction, which are mainly dependent on the initial aquifer mineralogy and brine components. The cement minerals are common materials in sandstone reservoir but few attention has been paid for its effects on CO2-water-rock interaction. Five batch reactions, in which 5% cement minerals were assigned to be quartz, calcite, dolomite, chlorite and Ca-montmorillonite, respectively, were conducted to understanding the cement minerals behaviors and its corresponding effects on the matrix minerals alterations during CO2 geological storage. Pure mineral powders were selected to mix and assemble the 'sandstone rock' with different cement components meanwhile keeping the matrix minerals same for each group as 70% quartz, 20% K-feldspar and 5% albite. These `rock' reacted with 750ml deionized water and CO2 under 180° and 18MPa for 15 days, during which the water chemistry evolution and minerals surface micromorphology changes has been monitored. The minerals saturation indexes calculation and phase diagram as well as the kinetic models were made by PHREEQC to uncover the minerals reaction paths. The experiment results indicated that the quartz got less eroded, on the contrary, K-feldspar and albite continuously dissolved to favor the gibbsite and kaolinite precipitations. The carbonates cement minerals quickly dissolved to reach equilibrium with the pH buffered and in turn suppressed the alkali feldspar dissolutions. No carbonates minerals precipitations occurred until the end of reactions for all groups. The simulation results were basically consistent with the experiment record but failed to simulate the non-stoichiometric reactions and the minerals kinetic rates seemed underestimated at the early stage of reactions. The cement minerals significantly dominated the reaction paths during CO2 geological

  7. Analysis of mineral trapping for CO(sub 2) disposal in deep aquifers; TOPICAL

    International Nuclear Information System (INIS)

    Xu, Tianfu; Apps, John A.; Pruess, Karsten

    2001-01-01

    CO(sub 2) disposal into deep aquifers has been suggested as a potential means whereby atmospheric emissions of greenhouse gases may be reduced. However, our knowledge of the geohydrology, geochemistry, geophysics, and geomechanics of CO(sub 2) disposal must be refined if this technology is to be implemented safely, efficiently, and predictably. As a prelude to a fully coupled treatment of physical and chemical effects of CO(sub 2) injection, we have analyzed the impact of CO(sub 2) immobilization through carbonate precipitation. A survey of all major classes of rock-forming minerals, whose alteration would lead to carbonate precipitation, indicated that very few minerals are present in sufficient quantities in aquifer host rocks to permit significant sequestration of CO(sub 2). We performed batch reaction modeling of the geochemical evolution of three different aquifer mineralogies in the presence of CO(sub 2) at high pressure. Our modeling considered (1) redox processes that could be important in deep subsurface environments, (2) the presence of organic matter, (3) the kinetics of chemical interactions between the host rock minerals and the aqueous phase, and (4) CO(sub 2) solubility dependence on pressure, temperature and salinity of the system. The geochemical evolution under both natural background and CO(sub 2) injection conditions was evaluated. In addition, changes in porosity were monitored during the simulations. Results indicate that CO(sub 2) sequestration by matrix minerals varies considerably with rock type. Under favorable conditions the amount of CO(sub 2) that may be sequestered by precipitation of secondary carbonates is comparable with and can be larger than the effect of CO(sub 2) dissolution in pore waters. The precipitation of ankerite and siderite is sensitive to the rate of reduction of ferric mineral precursors such as glauconite, which in turn is dependent on the reactivity of associated organic material. The accumulation of carbonates in

  8. Microbially mediated mineral carbonation

    Science.gov (United States)

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

    2010-12-01

    Mineral carbonation involves silicate dissolution and carbonate precipitation, which are both natural processes that microorganisms are able to mediate in near surface environments (Ferris et al., 1994; Eq. 1). (Ca,Mg)SiO3 + 2H2CO3 + H2O → (Ca,Mg)CO3 + H2O + H4SiO4 + O2 (1) Cyanobacteria are photoautotrophs with cell surface characteristics and metabolic processes involving inorganic carbon that can induce carbonate precipitation. This occurs partly by concentrating cations within their net-negative cell envelope and through the alkalinization of their microenvironment (Thompson & Ferris, 1990). Regions with mafic and ultramafic bedrock, such as near Atlin, British Columbia, Canada, represent the best potential sources of feedstocks for mineral carbonation. The hydromagnesite playas near Atlin are a natural biogeochemical model for the carbonation of magnesium silicate minerals (Power et al., 2009). Field-based studies at Atlin and corroborating laboratory experiments demonstrate the ability of a microbial consortium dominated by filamentous cyanobacteria to induce the precipitation of carbonate minerals. Phototrophic microbes, such as cyanobacteria, have been proposed as a means for producing biodiesel and other value added products because of their efficiency as solar collectors and low requirement for valuable, cultivable land in comparison to crops (Dismukes et al., 2008). Carbonate precipitation and biomass production could be facilitated using specifically designed ponds to collect waters rich in dissolved cations (e.g., Mg2+ and Ca2+), which would allow for evapoconcentration and provide an appropriate environment for growth of cyanobacteria. Microbially mediated carbonate precipitation does not require large quantities of energy or chemicals needed for industrial systems that have been proposed for rapid carbon capture and storage via mineral carbonation (e.g., Lackner et al., 1995). Therefore, this biogeochemical approach may represent a readily

  9. Spatial variation of sediment mineralization supports differential CO2 emissions from a tropical hydroelectric reservoir

    Directory of Open Access Journals (Sweden)

    Simone Jaqueline Cardoso

    2013-04-01

    Full Text Available Substantial amounts of organic matter (OM from terrestrial ecosystems are buried as sediments in inland waters. It is still unclear to what extent this OM constitutes a sink of carbon, and how much of it is returned to the atmosphere upon mineralization to carbon dioxide (CO2. The construction of reservoirs affects the carbon cycle by increasing OM sedimentation at the regional scale. In this study we determine the OM mineralization in the sediment of three zones (river, transition and dam of a tropical hydroelectric reservoir in Brazil as well as identify the composition of the carbon pool available for mineralization. We measured sediment OC mineralization rates and related them to the composition of the OM, bacterial abundance and pCO2 of the surface water of the reservoir. Terrestrial OM was an important substrate for the mineralization. In the river and transition zones most of the OM was allochthonous (56 % and 48 %, respectively while the dam zone had the lowest allochthonous contribution (7 %. The highest mineralization rates were found in the transition zone (154.80 ± 33.50 mg C m-2 d-1 and the lowest in the dam (51.60 ± 26.80 mg C m-2 d-1. Moreover, mineralization rates were significantly related to bacterial abundance (r2 = 0.50, p < 0.001 and pCO2 in the surface water of the reservoir (r2 = 0.73, p < 0.001. The results indicate that allochthonous OM has different contributions to sediment mineralization in the three zones of the reservoir. Further, the sediment mineralization, mediated by heterotrophic bacteria metabolism, significantly contributes to CO2 supersaturation in the water column, resulting in higher pCO2 in the river and transition zones in comparison with the dam zone, affecting greenhouse gas emission estimations from hydroelectric reservoirs.

  10. Rapid solubility and mineral storage of CO2 in basalt

    DEFF Research Database (Denmark)

    Gislason, Sigurdur R.; Broecker, W.S.; Gunnlaugsson, E.

    2014-01-01

    The long-term security of geologic carbon storage is critical to its success and public acceptance. Much of the security risk associated with geological carbon storage stems from its buoyancy. Gaseous and supercritical CO2 are less dense than formation waters, providing a driving force for it to ......The long-term security of geologic carbon storage is critical to its success and public acceptance. Much of the security risk associated with geological carbon storage stems from its buoyancy. Gaseous and supercritical CO2 are less dense than formation waters, providing a driving force...... for it to escape back to the surface. This buoyancy can be eliminated by the dissolution of CO2 into water prior to, or during its injection into the subsurface. The dissolution makes it possible to inject into fractured rocks and further enhance mineral storage of CO2 especially if injected into silicate rocks...... rich in divalent metal cations such as basalts and ultra-mafic rocks. We have demonstrated the dissolution of CO2 into water during its injection into basalt leading to its geologic solubility storage in less than five minutes and potential geologic mineral storage within few years after injection [1...

  11. 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

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

    Science.gov (United States)

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

    2013-12-01

    Accessory minerals in carbonate reservoirs, and in the caprocks that seal these reservoirs, can provide insight into multiphase fluid (CO2 + H2O)-rock interactions and the behavior of CO2 that resides in these water-rock systems. Our program integrates field data, hydrothermal experiments, and geochemical modeling to evaluate CO2-water-rock reactions and processes in a variety of carbonate reservoirs in the Rocky Mountain region of the US. These studies provide insights into a wide range of geologic environments, including natural CO2 reservoirs, geologic carbon sequestration, engineered geothermal systems, enhanced oil and gas recovery, and unconventional hydrocarbon resources. One suite of experiments evaluates the Madison Limestone on the Moxa Arch, Southwest Wyoming, a sulfur-rich natural CO2 reservoir. Mineral textures and geochemical features developed in the experiments suggest that carbonate minerals which constitute the natural reservoir will initially dissolve in response to emplacement of CO2. Euhedral, bladed anhydrite concomitantly precipitates in response to injected CO2. Analogous anhydrite is observed in drill core, suggesting that secondary anhydrite in the natural reservoir may be related to emplacement of CO2 into the Madison Limestone. Carbonate minerals ultimately re-precipitate, and anhydrite dissolves, as the rock buffers the acidity and reasserts geochemical control. Another suite of experiments emulates injection of CO2 for enhanced oil recovery in the Desert Creek Limestone (Paradox Formation), Paradox Basin, Southeast Utah. Euhedral iron oxyhydroxides (hematite) precipitate at pH 4.5 to 5 and low Eh (approximately -0.1 V) as a consequence of water-rock reaction. Injection of CO2 decreases pH to approximately 3.5 and increases Eh by approximately 0.1 V, yielding secondary mineralization of euhedral pyrite instead of iron oxyhydroxides. Carbonate minerals also dissolve and ultimately re-precipitate, as determined by experiments in the

  13. Carbon Mineralization by Aqueous Precipitation for Beneficial Use of CO2 from Flue Gas

    Energy Technology Data Exchange (ETDEWEB)

    Devenney, Martin; Gilliam, Ryan; Seeker, Randy

    2013-08-01

    The objective of this project is to demonstrate an innovative process to mineralize CO2 from flue gas directly to reactive carbonates and maximize the value and versatility of its beneficial use products. The program scope includes the design, construction, and testing of a CO2 Conversion to Material Products (CCMP) Pilot Demonstration Plant utilizing CO2 from the flue gas of a power production facility in Moss Landing, CA. This topical report covers Subphase 2a which is the design phase of pilot demonstration subsystems. Materials of construction have been selected and proven in both lab scale and prototype testing to be acceptable for the reagent conditions of interest. The target application for the reactive carbonate material has been selected based upon small-scale feasibility studies and the design of a continuous fiber board production line has been completed. The electrochemical cell architecture and components have been selected based upon both lab scale and prototype testing. The appropriate quality control and diagnostic techniques have been developed and tested along with the required instrumentation and controls. Finally the demonstrate site infrastructure, NEPA categorical exclusion, and permitting is all ready for the construction and installation of the new units and upgrades.

  14. CO{sub 2} emissions: mineral carbonation and Finnish pulp and paper industry (CO{sub Nordic Plus}) and use of serpentinites in energy and metal industry (ECOSERP); Hiilidioksidipaeaestoet: Mineraalikarbonointi ja Suomen massaja paperiteollisuus (CO{sub 2} Nordic plus) ja serpentiinin hyoetykaeyttoe energia- ja metalliteollisuudessa (ECOSERP)

    Energy Technology Data Exchange (ETDEWEB)

    Fogelholm, C.J.; Raiski, T.; Teir, S. [Helsinki Univ. of Technology, Espoo (Finland). Lab of Energy Engineering and Environmental Protection

    2006-12-19

    Mineral carbonation has been investigated at Helsinki University of Technology (TKK), laboratory of energy engineering and environmental protection since year 2000. The Finnish Technology Agency Tekes and the Finnish Recovery Boiler Committee are funding through the ClimBus technology programme, in conjunction with the Nordic Energy Research Programme, the research regarding the application of ex situ mineral carbonation processes. One aspect is to verify the possible use of mineral carbonation for the separation, utilisation and long-term storage of carbon dioxide (CO2) in the pulp and paper industry. The Geological Survey of Finland (GTK) has been screening since 2004 the location, quality and suitability of the Finnish processed serpentine and stopped serpentinite storage of mines and in situ serpentinite bodies of ultramafic rock formations for mineral carbonation of CO2. Tekes and the GTK are funding development work through the ClimBus technology programme on the utilisation of serpentine and serpentinite for CO2 sequestration purposes, based on economical and environmental evaluation of mineral and mining processing operations. Also the options for other use of serpentine and serpentinite are evaluated. The most promising magnesium and calcium-based sources for carbonation are by products of mining processes of ultramafic rocks (such as serpentinites and serpentine) and steelmaking slags. Carbonated minerals could possibly be used as paper coating materials (PCC), fillers or construction materials. For magnesium carbonate new markets and applications must be developed. (orig.)

  15. 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.

  16. Carbon dioxide sequestration by aqueous mineral carbonation of magnesium silicate minerals

    Energy Technology Data Exchange (ETDEWEB)

    Gerdemann, Stephen J.; Dahlin, David C.; O' Connor, William K.; Penner, Larry R.

    2003-01-01

    The dramatic increase in atmospheric carbon dioxide since the Industrial Revolution has caused concerns about global warming. Fossil-fuel-fired power plants contribute approximately one third of the total human-caused emissions of carbon dioxide. Increased efficiency of these power plants will have a large impact on carbon dioxide emissions, but additional measures will be needed to slow or stop the projected increase in the concentration of atmospheric carbon dioxide. By accelerating the naturally occurring carbonation of magnesium silicate minerals it is possible to sequester carbon dioxide in the geologically stable mineral magnesite (MgCO3). The carbonation of two classes of magnesium silicate minerals, olivine (Mg2SiO4) and serpentine (Mg3Si2O5(OH)4), was investigated in an aqueous process. The slow natural geologic process that converts both of these minerals to magnesite can be accelerated by increasing the surface area, increasing the activity of carbon dioxide in the solution, introducing imperfections into the crystal lattice by high-energy attrition grinding, and in the case of serpentine, by thermally activating the mineral by removing the chemically bound water. The effect of temperature is complex because it affects both the solubility of carbon dioxide and the rate of mineral dissolution in opposing fashions. Thus an optimum temperature for carbonation of olivine is approximately 185 degrees C and 155 degrees C for serpentine. This paper will elucidate the interaction of these variables and use kinetic studies to propose a process for the sequestration of the carbon dioxide.

  17. An experimental study on mineral sequestration of CO2 in basics and ultra basics rocks

    International Nuclear Information System (INIS)

    Dufaud, F.

    2006-11-01

    The first part of the thesis is dedicated to dissolution data of siderite FeCO 3 and magnetite Fe 3 O 4 which have been monitored in situ on the FAME beamline of the european synchrotron radiation facility in Grenoble. Iron in solution close to siderite single crystals is shown to be divalent hydrated. The small size of the experimentally investigated volume of solution (200 *400 micrometer and 3 mm height) allowed to work with single crystals in well defined geometries. No specific interaction was observed between iron (II) and dissolved inorganic carbon, suggesting that modelling siderite evolution under high CO 2 pressures by using CO 2 -less very acidic (pH 1-2) solutions is adequate. Using initial reaction rates, we get an activation energy for siderite dissolution of 62 kJ.mol -1 , consistent with existing literature data. Such a value is suggestive of a mineral/solution interface mechanism.. Data from this study and from literature are consistent over a temperature range 25 C - 125 C and a pH range pH 1-7 with an empirical law: pk = pH + E a /(ln(10)*RT(K)) - log(S/V) - 10,5 where E a = 62 kJ.mol -1 and S/V is the ratio between solid surface S and fluid volume V. A value of activation energy of 73.5 kJ.mol -1 is obtained in the case of magnetite, also consistent with mineral/solution processes. The second and major part of the thesis work is the realization of analogical experiments for simulating carbonation of basic and ultra basic minerals. Experiments were carried out on consolidated rock cores at 90 C and 280 bar of CO 2 (low temperature experiments) and on powders contained in metallic capsules at 400-500 C and 1000-1700 bars of CO 2 (high temperature experiments). The rate of mineral storage of CO 2 was defined as the molar ratio of solid carbonate formed over total CO 2 injected. It is of about 1% in three months in low temperature experiments whereas it reaches several tens of percents per hour in high temperature experiments. In all cases

  18. Mineral Carbonation Employing Ultramafic Mine Waste

    Science.gov (United States)

    Southam, G.; McCutcheon, J.; Power, I. M.; Harrison, A. L.; Wilson, S. A.; Dipple, G. M.

    2014-12-01

    Carbonate minerals are an important, stable carbon sink being investigated as a strategy to sequester CO2 produced by human activity. A natural playa (Atlin, BC, CAN) that has demonstrated the ability to microbially-accelerate hydromagnesite formation was used as an experimental model. Growth of microbial mats from Atlin, in a 10 m long flow-through bioreactor catalysed hydromagnesite precipitation under 'natural' conditions. To enhance mineral carbonation, chrysotile from the Clinton Creek Asbestos Mine (YT, CAN) was used as a target substrate for sulphuric acid leaching, releasing as much as 94% of the magnesium into solution via chemical weathering. This magnesium-rich 'feedstock' was used to examine the ability of the microbialites to enhance carbonate mineral precipitation using only atmospheric CO2 as the carbon source. The phototrophic consortium catalysed the precipitation of platy hydromagnesite [Mg5(CO3)4(OH)2·4H2O] accompanied by magnesite [MgCO3], aragonite [CaCO3], and minor dypingite [Mg5(CO3)4(OH)2·5H2O]. Scanning Electron Microscopy-Energy Dispersive Spectroscopy indicated that cell exteriors and extracellular polymeric substances (EPS) served as nucleation sites for carbonate precipitation. In many cases, entire cyanobacteria filaments were entombed in magnesium carbonate coatings, which appeared to contain a framework of EPS. Cell coatings were composed of small crystals, which intuitively resulted from rapid crystal nucleation. Excess nutrient addition generated eutrophic conditions in the bioreactor, resulting in the growth of a pellicle that sealed the bioreactor contents from the atmosphere. The resulting anaerobic conditions induced fermentation and subsequent acid generation, which in turn caused a drop in pH to circumneutral values and a reduction in carbonate precipitation. Monitoring of the water chemistry conditions indicated that a high pH (> 9.4), and relatively high concentrations of magnesium (> 3000 ppm), compared with the natural

  19. 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.

  20. Spatial variation of sediment mineralization supports differential CO2 emissions from a tropical hydroelectric reservoir.

    Science.gov (United States)

    Cardoso, Simone J; Vidal, Luciana O; Mendonça, Raquel F; Tranvik, Lars J; Sobek, Sebastian; Fábio, Roland

    2013-01-01

    Substantial amounts of organic matter (OM) from terrestrial ecosystems are buried as sediments in inland waters. It is still unclear to what extent this OM constitutes a sink of carbon, and how much of it is returned to the atmosphere upon mineralization to carbon dioxide (CO2). The construction of reservoirs affects the carbon cycle by increasing OM sedimentation at the regional scale. In this study we determine the OM mineralization in the sediment of three zones (river, transition, and dam) of a tropical hydroelectric reservoir in Brazil as well as identify the composition of the carbon pool available for mineralization. We measured sediment organic carbon mineralization rates and related them to the composition of the OM, bacterial abundance and pCO2 of the surface water of the reservoir. Terrestrial OM was an important substrate for the mineralization. In the river and transition zones most of the OM was allochthonous (56 and 48%, respectively) while the dam zone had the lowest allochthonous contribution (7%). The highest mineralization rates were found in the transition zone (154.80 ± 33.50 mg C m(-) (2) d(-) (1)) and the lowest in the dam (51.60 ± 26.80 mg C m(-) (2) d(-) (1)). Moreover, mineralization rates were significantly related to bacterial abundance (r (2) = 0.50, p hydroelectric reservoirs.

  1. Mechanisms for chemostatic behavior in catchments: implications for CO2 consumption by mineral weathering

    Science.gov (United States)

    Clow, David W.; Mast, M. Alisa

    2010-01-01

    Concentrations of weathering products in streams often show relatively little variation compared to changes in discharge, both at event and annual scales. In this study, several hypothesized mechanisms for this “chemostatic behavior” were evaluated, and the potential for those mechanisms to influence relations between climate, weathering fluxes, and CO2 consumption via mineral weathering was assessed. Data from Loch Vale, an alpine catchment in the Colorado Rocky Mountains, indicates that cation exchange and seasonal precipitation and dissolution of amorphous or poorly crystalline aluminosilicates are important processes that help regulate solute concentrations in the stream; however, those processes have no direct effect on CO2 consumption in catchments. Hydrograph separation analyses indicate that old water stored in the subsurface over the winter accounts for about one-quarter of annual streamflow, and almost one-half of annual fluxes of Na and SiO2 in the stream; thus, flushing of old water by new water (snowmelt) is an important component of chemostatic behavior. Hydrologic flushing of subsurface materials further induces chemostatic behavior by reducing mineral saturation indices and increasing reactive mineral surface area, which stimulate mineral weathering rates. CO2 consumption by carbonic acid mediated mineral weathering was quantified using mass-balance calculations; results indicated that silicate mineral weathering was responsible for approximately two-thirds of annual CO2 consumption, and carbonate weathering was responsible for the remaining one-third. CO2 consumption was strongly dependent on annual precipitation and temperature; these relations were captured in a simple statistical model that accounted for 71% of the annual variation in CO2 consumption via mineral weathering in Loch Vale.

  2. Impacts of Nickel Nanoparticles on Mineral Carbonation

    Directory of Open Access Journals (Sweden)

    Marius Bodor

    2014-01-01

    Full Text Available This work presents experimental results regarding the use of pure nickel nanoparticles (NiNP as a mineral carbonation additive. The aim was to confirm if the catalytic effect of NiNP, which has been reported to increase the dissolution of CO2 and the dissociation of carbonic acid in water, is capable of accelerating mineral carbonation processes. The impacts of NiNP on the CO2 mineralization by four alkaline materials (pure CaO and MgO, and AOD and CC steelmaking slags, on the product mineralogy, on the particle size distribution, and on the morphology of resulting materials were investigated. NiNP-containing solution was found to reach more acidic pH values upon CO2 bubbling, confirming a higher quantity of bicarbonate ions. This effect resulted in acceleration of mineral carbonation in the first fifteen minutes of reaction time when NiNP was present. After this initial stage, however, no benefit of NiNP addition was seen, resulting in very similar carbonation extents after one hour of reaction time. It was also found that increasing solids content decreased the benefit of NiNP, even in the early stages. These results suggest that NiNP has little contribution to mineral carbonation processes when the dissolution of alkaline earth metals is rate limiting.

  3. Ex-situ and in-situ mineral carbonation as a means to sequester carbon dioxide

    Energy Technology Data Exchange (ETDEWEB)

    Gerdemann, Stephen J.; Dahlin, David C.; O' Connor, William K.; Penner, Larry R.; Rush, G.E.

    2004-01-01

    The U. S. Department of Energy's Albany Research Center is investigating mineral carbonation as a method of sequestering CO2 from coal-fired-power plants. Magnesium-silicate minerals such as serpentine [Mg3Si2O5(OH)4] and olivine (Mg2SiO4) react with CO2 to produce magnesite (MgCO3), and the calcium-silicate mineral, wollastonite (CaSiO3), reacts to form calcite (CaCO3). It is possible to carry out these reactions either ex situ (above ground in a traditional chemical processing plant) or in situ (storage underground and subsequent reaction with the host rock to trap CO2 as carbonate minerals). For ex situ mineral carbonation to be economically attractive, the reaction must proceed quickly to near completion. The reaction rate is accelerated by raising the activity of CO2 in solution, heat (but not too much), reducing the particle size, high-intensity grinding to disrupt the crystal structure, and, in the case of serpentine, heat-treatment to remove the chemically bound water. All of these carry energy/economic penalties. An economic study illustrates the impact of mineral availability and process parameters on the cost of ex situ carbon sequestration. In situ carbonation offers economic advantages over ex situ processes, because no chemical plant is required. Knowledge gained from the ex situ work was applied to long-term experiments designed to simulate in situ CO2 storage conditions. The Columbia River Basalt Group (CRBG), a multi-layered basaltic lava formation, has potentially favorable mineralogy (up to 25% combined concentration of Ca, Fe2+, and Mg cations) for storage of CO2. However, more information about the interaction of CO2 with aquifers and the host rock is needed. Core samples from the CRBG, as well as samples of olivine, serpentine, and sandstone, were reacted in an autoclave for up to 2000 hours at elevated temperatures and pressures. Changes in core porosity, secondary mineralizations, and both solution and solid chemistry were measured.

  4. Hydrothermal Valorization of Steel Slags—Part I: Coupled H2 Production and CO2 Mineral Sequestration

    Directory of Open Access Journals (Sweden)

    Camille Crouzet

    2017-10-01

    Full Text Available A new process route for the valorization of BOF steel slags combining H2 production and CO2 mineral sequestration is investigated at 300°C (HT under hydrothermal conditions. A BOF steel slag stored several weeks outdoor on the production site was used as starting material. To serve as a reference, room temperature (RT carbonation of the same BOF steel slag has been monitored with in situ Raman spectroscopy and by measuring pH and PCO2 on a time-resolved basis. CO2 uptake under RT and HT are, respectively, 243 and 327 kg CO2/t of fresh steel slag, which add up with the 63 kg of atmospheric CO2 per ton already uptaken by the starting steel slag on the storage site. The CO2 gained by the sample at HT is bounded to the carbonation of brownmillerite. H2 yield decreased by about 30% in comparison to the same experiment performed without added CO2, due to sequestration of ferrous iron in a Mg-rich siderite phase. Ferric iron, initially present in brownmillerite, is partitioned between an Fe-rich clay mineral of saponite type and metastable hematite. Saponite is likely stabilized by the presence of Al, whereas hematite may represent a metastable product of brownmillerite carbonation. Mg-rich wüstite is involved in at least two competing reactions, i.e., oxidation into magnetite and carbonation into siderite. Results of both water-slag and water-CO2-slag experiments after 72 h are consistent with a kinetics enhancement of the former reaction when a CO2 partial pressure imposes a pH between 5 and 6. Three possible valorization routes, (1 RT carbonation prior to hydrothermal oxidation, (2 RT carbonation after hydrothermal treatment, and (3 combined HT carbonation and oxidation are discussed in light of the present results and literature data.

  5. 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.

  6. 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

  7. CO2 fixation using magnesium silicate minerals part 1: Process description and performance

    International Nuclear Information System (INIS)

    Fagerlund, Johan; Nduagu, Experience; Romão, Inês; Zevenhoven, Ron

    2012-01-01

    This paper describes a staged carbonation process for magnesium silicate mineral carbonation. This carbon dioxide capture and storage (CCS) alternative involves the production of magnesium hydroxide, followed by its carbonation in a pressurised fluidised bed (PFB) reactor. The goal is to utilise the heat of the carbonation reaction to drive the Mg(OH) 2 production step. The results show that Mg(OH) 2 can be produced successfully (up to 78% Mg extraction extent achieved so far) and efficiently from different serpentinite minerals from locations worldwide (Finland, Lithuania, Australia, Portugal…). From the extraction step, ammonium sulphate is recovered while iron oxides (from the mineral) are obtained as by-products. The carbonation step, while still being developed, resulted in >50%-wt conversion in 10 min (500 °C, 20 bar) for > 300 μm serpentinite-derived Mg(OH) 2 particles. Thus the reaction rate achieved so far is much faster than what is currently being considered fast in the field of mineral carbonation. -- Highlights: ► Magnesium silicate-based rock can sequester CO 2 as stable magnesium carbonate. ► Abundance of rock material offers a larger capacity than other CCS methods. ► Mg(OH) 2 production is followed by its carbonation in a pressurised fluidised bed. ► Carbonation reaches >50% in around 10 min for >0.3 mm particles. ► Mg(OH) 2 produced from different rock material show the same performance.

  8. 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

  9. SIMULTANEOUS MECHANICAL AND HEAT ACTIVATION: A NEW ROUTE TO ENHANCE SERPENTINE CARBONATION REACTIVITY AND LOWER CO2 MINERAL SEQUESTRATION PROCESS COST

    Energy Technology Data Exchange (ETDEWEB)

    M.J. McKelvy; J. Diefenbacher; R. Nunez; R.W. Carpenter; A.V.G. Chizmeshya

    2005-01-01

    Coal can support a large fraction of global energy demands for centuries to come, if the environmental problems associated with CO{sub 2} emissions can be overcome. Unlike other candidate technologies, which propose long-term storage (e.g., ocean and geological sequestration), mineral sequestration permanently disposes of CO{sub 2} as geologically stable mineral carbonates. Only benign, naturally occurring materials are formed, eliminating long-term storage and liability issues. Serpentine carbonation is a leading mineral sequestration process candidate, which offers large scale, permanent sequestration. Deposits exceed those needed to carbonate all the CO{sub 2} that could be generated from global coal reserves, and mining and milling costs are reasonable ({approx}$4 to $5/ton). Carbonation is exothermic, providing exciting low-cost process potential. The remaining goal is to develop an economically viable process. An essential step in this development is increasing the carbonation reaction rate and degree of completion, without substantially impacting other process costs. Recently, the Albany Research Center (ARC) has accelerated serpentine carbonation, which occurs naturally over geological time, to near completion in less than an hour. While reaction rates for natural serpentine have been found to be too slow for practical application, both heat and mechanical (attrition grinding) pretreatment were found to substantially enhance carbonation reactivity. Unfortunately, these processes are too energy intensive to be cost-effective in their present form. In this project we explored the potential that utilizing power plant waste heat (e.g., available up to {approx}200-250 C) during mechanical activation (i.e., thermomechanical activation) offers to enhance serpentine mineral carbonation, while reducing pretreatment energy consumption and process cost. This project was carried out in collaboration with the Albany Research Center (ARC) to maximize the insight into the

  10. A Novel Approach to Mineral Carbonation: Enhancing Carbonation While Avoiding Mineral Pretreatment Process Cost

    Energy Technology Data Exchange (ETDEWEB)

    Andrew V. G. Chizmeshya; Michael J. McKelvy; Kyle Squires; Ray W. Carpenter; Hamdallah Bearat

    2007-06-21

    Known fossil fuel reserves, especially coal, can support global energy demands for centuries to come, if the environmental problems associated with CO{sub 2} emissions can be overcome. Unlike other CO{sub 2} sequestration candidate technologies that propose long-term storage, mineral sequestration provides permanent disposal by forming geologically stable mineral carbonates. Carbonation of the widely occurring mineral olivine (e.g., forsterite, Mg{sub 2}SiO{sub 4}) is a large-scale sequestration process candidate for regional implementation, which converts CO{sub 2} into the environmentally benign mineral magnesite (MgCO{sub 3}). The primary goal is cost-competitive process development. As the process is exothermic, it inherently offers low-cost potential. Enhancing carbonation reactivity is key to economic viability. Recent studies at the U.S. DOE Albany Research Center have established that aqueous-solution carbonation using supercritical CO{sub 2} is a promising process; even without olivine activation, 30-50% carbonation has been achieved in an hour. Mechanical activation (e.g., attrition) has accelerated the carbonation process to an industrial timescale (i.e., near completion in less than an hour), at reduced pressure and temperature. However, the activation cost is too high to be economical and lower cost pretreatment options are needed. We have discovered that robust silica-rich passivating layers form on the olivine surface during carbonation. As carbonation proceeds, these passivating layers thicken, fracture and eventually exfoliate, exposing fresh olivine surfaces during rapidly-stirred/circulating carbonation. We are exploring the mechanisms that govern carbonation reactivity and the impact that (1) modeling/controlling the slurry fluid-flow conditions, (2) varying the aqueous ion species/size and concentration (e.g., Li+, Na+, K+, Rb+, Cl-, HCO{sub 3}{sup -}), and (3) incorporating select sonication offer to enhance exfoliation and carbonation. Thus

  11. A Novel Approach To Mineral Carbonation: Enhancing Carbonation While Avoiding Mineral Pretreatment Process Cost

    Energy Technology Data Exchange (ETDEWEB)

    Michael J. McKelvy; Andrew V. G. Chizmeshya; Kyle Squires; Ray W. Carpenter; Hamdallah Bearat

    2006-06-21

    Known fossil fuel reserves, especially coal, can support global energy demands for centuries to come, if the environmental problems associated with CO{sub 2} emissions can be overcome. Unlike other CO{sub 2} sequestration candidate technologies that propose long-term storage, mineral sequestration provides permanent disposal by forming geologically stable mineral carbonates. Carbonation of the widely occurring mineral olivine (e.g., forsterite, Mg{sub 2}SiO{sub 4}) is a large-scale sequestration process candidate for regional implementation, which converts CO{sub 2} into the environmentally benign mineral magnesite (MgCO{sub 3}). The primary goal is cost-competitive process development. As the process is exothermic, it inherently offers low-cost potential. Enhancing carbonation reactivity is key to economic viability. Recent studies at the U.S. DOE Albany Research Center have established that aqueous-solution carbonation using supercritical CO{sub 2} is a promising process; even without olivine activation, 30-50% carbonation has been achieved in an hour. Mechanical activation (e.g., attrition) has accelerated the carbonation process to an industrial timescale (i.e., near completion in less than an hour), at reduced pressure and temperature. However, the activation cost is too high to be economical and lower cost pretreatment options are needed. Herein, we report our second year progress in exploring a novel approach that offers the potential to substantially enhance carbonation reactivity while bypassing pretreatment activation. As our second year progress is intimately related to our earlier work, the report is presented in that context to provide better overall understanding of the progress made. We have discovered that robust silica-rich passivating layers form on the olivine surface during carbonation. As carbonation proceeds, these passivating layers thicken, fracture and eventually exfoliate, exposing fresh olivine surfaces during rapidly

  12. Hydrothermal Valorization of Steel Slags—Part I: Coupled H{sub 2} Production and CO{sub 2} Mineral Sequestration

    Energy Technology Data Exchange (ETDEWEB)

    Crouzet, Camille [University Grenoble Alpes, University Savoie Mont Blanc, CNRS, IRD, IFSTTAR, ISTerre, Grenoble (France); LRCS and RS2E, CNRS-UMR7314, University Picardie Jules Verne, Amiens (France); Aix Marseille University, CNRS, Centrale Marseille, M2P2, Marseille (France); Brunet, Fabrice, E-mail: fabrice.brunet@univ-grenoble-alpes.fr; Montes-Hernandez, German [University Grenoble Alpes, University Savoie Mont Blanc, CNRS, IRD, IFSTTAR, ISTerre, Grenoble (France); Recham, Nadir [LRCS and RS2E, CNRS-UMR7314, University Picardie Jules Verne, Amiens (France); Findling, Nathaniel [University Grenoble Alpes, University Savoie Mont Blanc, CNRS, IRD, IFSTTAR, ISTerre, Grenoble (France); Ferrasse, Jean-Henry [Aix Marseille University, CNRS, Centrale Marseille, M2P2, Marseille (France); Goffé, Bruno [Aix-Marseille University, CNRS, IRD, Coll. de France, CEREGE, Aix-en-Provence (France)

    2017-10-30

    A new process route for the valorization of BOF steel slags combining H{sub 2} production and CO{sub 2} mineral sequestration is investigated at 300°C (HT) under hydrothermal conditions. A BOF steel slag stored several weeks outdoor on the production site was used as starting material. To serve as a reference, room temperature (RT) carbonation of the same BOF steel slag has been monitored with in situ Raman spectroscopy and by measuring pH and P{sub CO2} on a time-resolved basis. CO{sub 2} uptake under RT and HT are, respectively, 243 and 327 kg CO{sub 2}/t of fresh steel slag, which add up with the 63 kg of atmospheric CO{sub 2} per ton already uptaken by the starting steel slag on the storage site. The CO{sub 2} gained by the sample at HT is bounded to the carbonation of brownmillerite. H{sub 2} yield decreased by about 30% in comparison to the same experiment performed without added CO{sub 2}, due to sequestration of ferrous iron in a Mg-rich siderite phase. Ferric iron, initially present in brownmillerite, is partitioned between an Fe-rich clay mineral of saponite type and metastable hematite. Saponite is likely stabilized by the presence of Al, whereas hematite may represent a metastable product of brownmillerite carbonation. Mg-rich wüstite is involved in at least two competing reactions, i.e., oxidation into magnetite and carbonation into siderite. Results of both water-slag and water-CO{sub 2}-slag experiments after 72 h are consistent with a kinetics enhancement of the former reaction when a CO{sub 2} partial pressure imposes a pH between 5 and 6. Three possible valorization routes, (1) RT carbonation prior to hydrothermal oxidation, (2) RT carbonation after hydrothermal treatment, and (3) combined HT carbonation and oxidation are discussed in light of the present results and literature data.

  13. Estimation of the efficiency of hydrocarbon mineralization in soil by measuring CO2-emission and variations in the isotope composition of carbon dioxide

    Science.gov (United States)

    Dubrovskaya, Ekaterina; Turkovskaya, Olga

    2010-05-01

    Estimation of the efficiency of hydrocarbon mineralization in soil by measuring CO2-emission and variations in the isotope composition of carbon dioxide E. Dubrovskaya1, O. Turkovskaya1, A. Tiunov2, N. Pozdnyakova1, A. Muratova1 1 - Institute of Biochemistry and Physiology of Plants and Microorganisms, RAS, Saratov, 2 - A.N. Severtsov Institute of Ecology and Evolution, RAS, Moscow, Russian Federation Hydrocarbon mineralization in soil undergoing phytoremediation was investigated in a laboratory experiment by estimating the variation in the 13С/12С ratio in the respired СО2. Hexadecane (HD) was used as a model hydrocarbon pollutant. The polluted soil was planted with winter rye (Secale cereale) inoculated with Azospirillum brasilense strain SR80, which combines the abilities to promote plant growth and to degrade oil hydrocarbon. Each vegetated treatment was accompanied with a corresponding nonvegetated one, and uncontaminated treatments were used as controls. Emission of carbon dioxide, its isotopic composition, and the residual concentration of HD in the soil were examined after two and four weeks. At the beginning of the experiment, the CO2-emission level was higher in the uncontaminated than in the contaminated soil. After two weeks, the quantity of emitted carbon dioxide decreased by about three times and did not change significantly in all uncontaminated treatments. The presence of HD in the soil initially increased CO2 emission, but later the respiration was reduced. During the first two weeks, nonvegetated soil had the highest CO2-emission level. Subsequently, the maximum increase in respiration was recorded in the vegetated contaminated treatments. The isotope composition of plant material determines the isotope composition of soil. The soil used in our experiment had an isotopic signature typical of soils formed by C3 plants (δ13C,-22.4‰). Generally, there was no significant fractionation of the carbon isotopes of the substrates metabolized by the

  14. Thermodynamic Data for Geochemical Modeling of Carbonate Reactions Associated with CO2 Sequestration – Literature Review

    Energy Technology Data Exchange (ETDEWEB)

    Krupka, Kenneth M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Cantrell, Kirk J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); McGrail, B. Peter [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2010-09-01

    Permanent storage of anthropogenic CO2 in deep geologic formations is being considered as a means to reduce the concentration of atmospheric CO2 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 CO2 migrates within geologic formations and what physical and geochemical changes occur in these formations when CO2 is injected. Sophisticated, computerized reservoir simulations are used as part of field site and laboratory CO2 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 CO2 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 CO2 sequestration. A review of thermodynamic data for CO2 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 CO2 sequestration field and natural analogue sites and laboratory studies were also reviewed to identify specific carbonate minerals that are important to CO2 sequestration reactions and therefore require thermodynamic data. The results of the literature review indicated that an extensive thermodynamic database exists for CO2 and CH4 gases, carbonate aqueous species, and carbonate minerals. Values of ΔfG298° and/or log Kr,298° are available for essentially all of these compounds. However, log Kr,T° or heat capacity values at temperatures above 298 K exist for less than

  15. Commentary: Ex Situ Aqueous Mineral Carbonation

    Energy Technology Data Exchange (ETDEWEB)

    Gadikota, Greeshma, E-mail: gadikota@princeton.edu [Department of Civil and Environmental Engineering, Princeton University, Princeton, NJ (United States)

    2016-05-26

    CO{sub 2} conversion to calcium and magnesium carbonates has garnered considerable attention since it is a thermodynamically downhill pathway to safely and permanently sequester large quantities of CO{sub 2}. This seminal work performed at The National Energy Technology Laboratory in Albany (NETL-Albany) reports the conversion of calcium- and magnesium-bearing silicate minerals, such as olivine [(Mg, Fe){sub 2}SiO{sub 4}], wollastonite (CaSiO{sub 3}), and serpentine [Mg{sub 3}Si{sub 2}O{sub 5}(OH){sub 4}], as they are reacted with CO{sub 2} in an aqueous environment to form magnesium or calcium carbonates. This paper discusses various pretreatment methods of the starting materials, such as grinding or heat treatment of hydroxylated Mg silicates, to enhance the reaction kinetics. The effects of various chemical additives (e.g., NaCl and NaHCO{sub 3}), and reaction parameters, such as temperature, pressure, and reaction time, on the conversion are investigated. Feasibility assessments and energy and economic analyses of the direct carbonation of calcium- and magnesium-bearing minerals are presented.

  16. Numerical modeling of injection and mineral trapping of CO2 withH2S and SO2 in a Sandstone Formation

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Tianfu; Apps, John A.; Pruess, Karsten; Yamamoto, Hajime

    2004-09-07

    Carbon dioxide (CO{sub 2}) injection into deep geologic formations could decrease the atmospheric accumulation of this gas from anthropogenic sources. Furthermore, by co-injecting H{sub 2}S or SO{sub 2}, the products respectively of coal gasification or combustion, with captured CO{sub 2}, problems associated with surface disposal would be mitigated. We developed models that simulate the co-injection of H{sub 2}S or SO{sub 2} with CO{sub 2} into an arkose formation at a depth of about 2 km and 75 C. The hydrogeology and mineralogy of the injected formation are typical of those encountered in Gulf Coast aquifers of the United States. Six numerical simulations of a simplified 1-D radial region surrounding the injection well were performed. The injection of CO{sub 2} alone or co-injection with SO{sub 2} or H{sub 2}S results in a concentrically zoned distribution of secondary minerals surrounding a leached and acidified region adjacent to the injection well. Co-injection of SO{sub 2} with CO{sub 2} results in a larger and more strongly acidified zone, and alteration differs substantially from that caused by the co-injection of H{sub 2}S or injection of CO{sub 2} alone. Precipitation of carbonates occurs within a higher pH (pH > 5) peripheral zone. Significant quantities of CO{sub 2} are sequestered by ankerite, dawsonite, and lesser siderite. The CO{sub 2} mineral-trapping capacity of the formation can attain 40-50 kg/m{sup 3} medium for the selected arkose. In contrast, secondary sulfates precipitate at lower pH (pH < 5) within the acidified zone. Most of the injected SO{sub 2} is transformed and immobilized through alunite precipitation with lesser amounts of anhydrite and minor quantities of pyrite. The dissolved CO{sub 2} increases with time (enhanced solubility trapping). The mineral alteration induced by injection of CO{sub 2} with either SO{sub 2} or H{sub 2}S leads to corresponding changes in porosity. Significant increases in porosity occur in the acidified

  17. Mineral carbonation of gaseous carbon dioxide using a clay-hosted cation exchange reaction.

    Science.gov (United States)

    Kang, Il-Mo; Roh, Ki-Min

    2013-01-01

    The mineral carbonation method is still a challenge in practical application owing to: (1) slow reaction kinetics, (2) high reaction temperature, and (3) continuous mineral consumption. These constraints stem from the mode of supplying alkaline earth metals through mineral acidification and dissolution. Here, we attempt to mineralize gaseous carbon dioxide into calcium carbonate, using a cation exchange reaction of vermiculite (a species of expandable clay minerals). The mineralization is operated by draining NaCI solution through vermiculite powders and continuously dropping into the pool of NaOH solution with CO2 gas injected. The mineralization temperature is regulated here at 293 and 333 K for 15 min. As a result of characterization, using an X-ray powder diffractometer and a scanning electron microscopy, two types of pure CaCO3 polymorphs (vaterite and calcite) are identified as main reaction products. Their abundance and morphology are heavily dependent on the mineralization temperature. Noticeably, spindle-shaped vaterite, which is quite different from a typical vaterite morphology (polycrystalline spherulite), forms predominantly at 333 K (approximately 98 wt%).

  18. Effect of oxygen co-injected with carbon dioxide on Gothic shale caprock–CO2–brine interaction during geologic carbon sequestration

    Energy Technology Data Exchange (ETDEWEB)

    Jung, Hun Bok; Um, Wooyong; Cantrell, Kirk J.

    2013-09-01

    Co-injection of oxygen, a significant component in CO2 streams produced by the oxyfuel combustion process, can cause a significant alteration of the redox state in deep geologic formations during geologic carbon sequestration. The potential impact of co-injected oxygen on the interaction between synthetic CO2–brine (0.1 M NaCl) and shale caprock (Gothic shale from the Aneth Unit in Utah) and mobilization of trace metals was investigated at ~ 10 MPa and ~ 75 °C. A range of relative volume percentages of O2 to CO2 (0, 1, 4 and 8%) were used in these experiments to address the effect of oxygen on shale–CO2–brine interaction under various conditions. Major mineral phases in Gothic shale are quartz, calcite, dolomite, montmorillonite, and pyrite. During Gothic shale–CO2–brine interaction in the presence of oxygen, pyrite oxidation occurred extensively and caused enhanced dissolution of calcite and dolomite. Pyrite oxidation and calcite dissolution subsequently resulted in the precipitation of Fe(III) oxides and gypsum (CaSO4·2H2O). In the presence of oxygen, dissolved Mn and Ni were elevated because of oxidative dissolution of pyrite. The mobility of dissolved Ba was controlled by barite (BaSO4) precipitation in the presence of oxygen. Dissolved U in the experimental brines increased to ~ 8–14 μg/L, with concentrations being slightly higher in the absence of oxygen than in the presence of oxygen. Experimental and modeling results indicate the interaction between shale caprock and oxygen co-injected with CO2 during geologic carbon sequestration can exert significant impacts on brine pH, solubility of carbonate minerals, stability of sulfide minerals, and mobility of trace metals. The major impact of oxygen is most likely to occur in the zone near CO2 injection wells where impurity gases can accumulate. Finally, oxygen in CO2

  19. Reuse of Cement Kiln Dust for backfilling and CO2 carbonation

    Directory of Open Access Journals (Sweden)

    Lutyński Marcin

    2017-01-01

    Full Text Available The study aims to investigate possible alternative paths of reusing Cement Kiln Dust in mining technologies or as mineral sorbent for CO2 capture. Properties of CKD and bottom slag slurry were assessed and these were ia.: chemical composition, compressive strength and excess water content. Results show that CKD/bottom slag slurry mixed in the proportion of 25%/75% can be used as a backfill material if concentration of contaminants in the leaching tests is at the acceptable level. Second part of the study was devoted to the assessment of CKD as a sorbent in Calcium looping technologies or for mineral carbonation. TGA and DSC study shows that the rate of CO2 capture (carbonation is determined by the free CaO content. The highest carbonation rate was within the temperature range of 600-800°C.

  20. 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.

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

    Science.gov (United States)

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

    2014-10-07

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

  2. SkyMine Carbon Mineralization Pilot Project

    Energy Technology Data Exchange (ETDEWEB)

    Christenson, Norm; Walters, Jerel

    2014-12-31

    This Topical Report addresses accomplishments achieved during Phase 2b of the SkyMine® Carbon Mineralization Pilot Project. The primary objectives of this project are to design, construct, and operate a system to capture CO2 from a slipstream of flue gas from a commercial coal-fired cement kiln, convert that CO2 to products having commercial value (i.e., beneficial use), show the economic viability of the CO2 capture and conversion process, and thereby advance the technology to the point of readiness for commercial scale demonstration and deployment. The overall process is carbon negative, resulting in mineralization of CO2 that would otherwise be released into the atmosphere. The project will also substantiate market opportunities for the technology by sales of chemicals into existing markets, and identify opportunities to improve technology performance and reduce costs at the commercial scale. The project is being conducted in two phases. The primary objectives of Phase 1 were to evaluate proven SkyMine® process chemistry for commercial pilot-scale operation and complete the preliminary design for the pilot plant to be built and operated in Phase 2, complete a NEPA evaluation, and develop a comprehensive carbon life cycle analysis. The objective of Phase 2b was to build the pilot plant to be operated and tested in Phase 2c.

  3. Procedure to use phosphogypsum industrial waste for mineral CO2 sequestration

    International Nuclear Information System (INIS)

    Cárdenas-Escudero, C.; Morales-Flórez, V.; Pérez-López, R.; Santos, A.; Esquivias, L.

    2011-01-01

    Highlights: ► Phosphogypsum wastes are proposed to reduce CO 2 greenhouse gas emissions. ► Phosphogypsum dissolution with NaOH results in Ca(OH) 2 precipitation and Na 2 SO 4 . ► Aqueous carbonation of Ca(OH) 2 with CO 2 results in the CaCO 3 precipitation. ► Metals contained in the phosphogypsum are transferred to the final calcite. ► Applications of CaCO 3 and Na 2 SiO 4 by-products are proposed to improve viability. - Abstract: Industrial wet phosphoric acid production in Huelva (SW Spain) has led to the controversial stockpiling of waste phosphogypsum by-products, resulting in the release of significant quantities of toxic impurities in salt marshes in the Tinto river estuary. In the framework of the fight against global climate change and the effort to reduce carbon dioxide emissions, a simple and efficient procedure for CO 2 mineral sequestration is presented in this work, using phosphogypsum waste as a calcium source. Our results demonstrate the high efficiency of portlandite precipitation by phosphogypsum dissolution using an alkaline soda solution. Carbonation experiments performed at ambient pressure and temperature resulted in total conversion of the portlandite into carbonate. The fate of trace elements present in the phosphogypsum waste was also investigated, and trace impurities were found to be completely transferred to the final calcite. We believe that the procedure proposed here should be considered not only as a solution for reducing old stockpiles of phosphogypsum wastes, but also for future phosphoric acid and other gypsum-producing industrial processes, resulting in more sustainable production.

  4. An experimental study on mineral sequestration of CO{sub 2} in basics and ultra basics rocks; Etude experimentale des reactions de carbonatation minerale du CO{sub 2} dans les roches basiques et ultrabasiques

    Energy Technology Data Exchange (ETDEWEB)

    Dufaud, F

    2006-11-15

    The first part of the thesis is dedicated to dissolution data of siderite FeCO{sub 3} and magnetite Fe{sub 3}O{sub 4} which have been monitored in situ on the FAME beamline of the european synchrotron radiation facility in Grenoble. Iron in solution close to siderite single crystals is shown to be divalent hydrated. The small size of the experimentally investigated volume of solution (200 *400 micrometer and 3 mm height) allowed to work with single crystals in well defined geometries. No specific interaction was observed between iron (II) and dissolved inorganic carbon, suggesting that modelling siderite evolution under high CO{sub 2} pressures by using CO{sub 2}-less very acidic (pH 1-2) solutions is adequate. Using initial reaction rates, we get an activation energy for siderite dissolution of 62 kJ.mol{sup -1}, consistent with existing literature data. Such a value is suggestive of a mineral/solution interface mechanism.. Data from this study and from literature are consistent over a temperature range 25 C - 125 C and a pH range pH 1-7 with an empirical law: pk = pH + E{sub a}/(ln(10)*RT(K)) - log(S/V) - 10,5 where E{sub a} = 62 kJ.mol{sup -1} and S/V is the ratio between solid surface S and fluid volume V. A value of activation energy of 73.5 kJ.mol{sup -1} is obtained in the case of magnetite, also consistent with mineral/solution processes. The second and major part of the thesis work is the realization of analogical experiments for simulating carbonation of basic and ultra basic minerals. Experiments were carried out on consolidated rock cores at 90 C and 280 bar of CO{sub 2} (low temperature experiments) and on powders contained in metallic capsules at 400-500 C and 1000-1700 bars of CO{sub 2} (high temperature experiments). The rate of mineral storage of CO{sub 2} was defined as the molar ratio of solid carbonate formed over total CO{sub 2} injected. It is of about 1% in three months in low temperature experiments whereas it reaches several tens of

  5. Assessment of CO2 Mineralization and Dynamic Rock Properties at the Kemper Pilot CO2 Injection Site

    Science.gov (United States)

    Qin, F.; Kirkland, B. L.; Beckingham, L. E.

    2017-12-01

    CO2-brine-mineral reactions following CO2 injection may impact rock properties including porosity, permeability, and pore connectivity. The rate and extent of alteration largely depends on the nature and evolution of reactive mineral interfaces. In this work, the potential for geochemical reactions and the nature of the reactive mineral interface and corresponding hydrologic properties are evaluated for samples from the Lower Tuscaloosa, Washita-Fredericksburg, and Paluxy formations. These formations have been identified as future regionally extensive and attractive CO2 storage reservoirs at the CO2 Storage Complex in Kemper County, Mississippi, USA (Project ECO2S). Samples from these formations were obtained from the Geological Survey of Alabama and evaluated using a suite of complementary analyses. The mineral composition of these samples will be determined using petrography and powder X-ray Diffraction (XRD). Using these compositions, continuum-scale reactive transport simulations will be developed and the potential CO2-brine-mineral interactions will be examined. Simulations will focus on identifying potential reactive minerals as well as the corresponding rate and extent of reactions. The spatial distribution and accessibility of minerals to reactive fluids is critical to understanding mineral reaction rates and corresponding changes in the pore structure, including pore connectivity, porosity and permeability. The nature of the pore-mineral interface, and distribution of reactive minerals, will be determined through imaging analysis. Multiple 2D scanning electron microscopy (SEM) backscattered electron (BSE) images and energy dispersive x-ray spectroscopy (EDS) images will be used to create spatial maps of mineral distributions. These maps will be processed to evaluate the accessibility of reactive minerals and the potential for flow-path modifications following CO2 injection. The "Establishing an Early CO2 Storage Complex in Kemper, MS" project is funded by

  6. Carbonated miscanthus mineralized aggregates for reducing environmental impact of lightweight concrete blocks

    Directory of Open Access Journals (Sweden)

    Courard Luc

    2017-01-01

    Full Text Available At a time when the cement industry is largely responsible for the production of CO2 in the construction sector, it is useful to make this production a reverse phenomenon: that is CO2 capture. The CO2 absorption process called carbonation, improves specific properties of the concrete during the conversion of carbon dioxide CO2 into calcium carbonate CaCO3. Current environmental concerns motivate the study of carbonation in order to maximize the absorption of carbon dioxide. Moreover, lightweight concrete with bio-based products knows an interesting development in the construction field, especially as thermal insulation panels for walls in buildings. Before identifying and quantifying the basic physical characteristics of concrete made from miscanthus, it is necessary to optimize the composition of the product. The long-term stability as well as the reinforcement may be obtained by means of a mineralization process of the natural product: a preparation with a lime and/or cement-based material is necessary to reinforce the cohesion of the bio-based product. Mineralization process is described as well as the way of producing blocks for CO2 capture by means of accelerated carbonation. Finally, concrete blocks produced with miscanthus mineralized aggregates offer interesting mechanical properties and minimal environmental impact.

  7. On the potential for CO2 mineral storage in continental flood basalts – PHREEQC batch- and 1D diffusion–reaction simulations

    Directory of Open Access Journals (Sweden)

    Van Pham Thi

    2012-06-01

    Full Text Available Abstract Continental flood basalts (CFB are considered as potential CO2 storage sites because of their high reactivity and abundant divalent metal ions that can potentially trap carbon for geological timescales. Moreover, laterally extensive CFB are found in many place in the world within reasonable distances from major CO2 point emission sources. Based on the mineral and glass composition of the Columbia River Basalt (CRB we estimated the potential of CFB to store CO2 in secondary carbonates. We simulated the system using kinetic dependent dissolution of primary basalt-minerals (pyroxene, feldspar and glass and the local equilibrium assumption for secondary phases (weathering products. The simulations were divided into closed-system batch simulations at a constant CO2 pressure of 100 bar with sensitivity studies of temperature and reactive surface area, an evaluation of the reactivity of H2O in scCO2, and finally 1D reactive diffusion simulations giving reactivity at CO2 pressures varying from 0 to 100 bar. Although the uncertainty in reactive surface area and corresponding reaction rates are large, we have estimated the potential for CO2 mineral storage and identified factors that control the maximum extent of carbonation. The simulations showed that formation of carbonates from basalt at 40 C may be limited to the formation of siderite and possibly FeMg carbonates. Calcium was largely consumed by zeolite and oxide instead of forming carbonates. At higher temperatures (60 – 100 C, magnesite is suggested to form together with siderite and ankerite. The maximum potential of CO2 stored as solid carbonates, if CO2 is supplied to the reactions unlimited, is shown to depend on the availability of pore space as the hydration and carbonation reactions increase the solid volume and clog the pore space. For systems such as in the scCO2 phase with limited amount of water, the total carbonation potential is limited by the amount of water present

  8. CO2 Mineralization and Utilization using Steel Slag for Establishing a Waste-to-Resource Supply Chain.

    Science.gov (United States)

    Pan, Shu-Yuan; Chung, Tai-Chun; Ho, Chang-Ching; Hou, Chin-Jen; Chen, Yi-Hung; Chiang, Pen-Chi

    2017-12-08

    Both steelmaking via an electric arc furnace and manufacturing of portland cement are energy-intensive and resource-exploiting processes, with great amounts of carbon dioxide (CO 2 ) emission and alkaline solid waste generation. In fact, most CO 2 capture and storage technologies are currently too expensive to be widely applied in industries. Moreover, proper stabilization prior to utilization of electric arc furnace slag are still challenging due to its high alkalinity, heavy metal leaching potentials and volume instability. Here we deploy an integrated approach to mineralizing flue gas CO 2 using electric arc furnace slag while utilizing the reacted product as supplementary cementitious materials to establish a waste-to-resource supply chain toward a circular economy. We found that the flue gas CO 2 was rapidly mineralized into calcite precipitates using electric arc furnace slag. The carbonated slag can be successfully utilized as green construction materials in blended cement mortar. By this modulus, the global CO 2 reduction potential using iron and steel slags was estimated to be ~138 million tons per year.

  9. Magnesium hydroxide extracted from a magnesium-rich mineral for CO2 sequestration in a gas-solid system.

    Science.gov (United States)

    Lin, Pao-Chung; Huang, Cheng-Wei; Hsiao, Ching-Ta; Teng, Hsisheng

    2008-04-15

    Magnesium hydroxide extracted from magnesium-bearing minerals is considered a promising agent for binding CO2 as a carbonate mineral in a gas-solid reaction. An efficient extraction route consisting of hydrothermal treatment on serpentine in HCl followed by NaOH titration for Mg(OH)2 precipitation was demonstrated. The extracted Mg(OH)2 powder had a mean crystal domain size as small as 12 nm and an apparent surface area of 54 m2/g. Under one atmosphere of 10 vol% CO2/N2, carbonation of the serpentine-derived Mg(OH)2 to 26% of the stoichiometric limit was achieved at 325 degrees C in 2 h; while carbonation of a commercially available Mg(OH)2, with a mean crystal domain size of 33 nm and an apparent surface area of 3.5 m2/g, reached only 9% of the stoichiometric limit. The amount of CO2 fixation was found to be inversely proportional to the crystal domain size of the Mg(OH)2 specimens. The experimental data strongly suggested that only a monolayer of carbonates was formed on the crystal domain boundary in the gas-solid reaction, with little penetration of the carbonates into the crystal domain.

  10. 78 FR 23524 - Approval and Promulgation of Implementation Plans; North Carolina: Deferral of Carbon Dioxide (CO2

    Science.gov (United States)

    2013-04-19

    ... Promulgation of Implementation Plans; North Carolina: Deferral of Carbon Dioxide (CO 2 ) Emissions From... (IBR) the federal deferral of, until July 21, 2014, PSD applicability to biogenic carbon dioxide (CO 2... decomposition of biologically-based materials other than fossil fuels and mineral sources of carbon. Examples of...

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

    Science.gov (United States)

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

    2014-01-01

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

  12. Wollastonite Carbonation in Water-Bearing Supercritical CO2: Effects of Particle Size.

    Science.gov (United States)

    Min, Yujia; Li, Qingyun; Voltolini, Marco; Kneafsey, Timothy; Jun, Young-Shin

    2017-11-07

    The performance of geologic CO 2 sequestration (GCS) can be affected by CO 2 mineralization and changes in the permeability of geologic formations resulting from interactions between water-bearing supercritical CO 2 (scCO 2 ) and silicates in reservoir rocks. However, without an understanding of the size effects, the findings in previous studies using nanometer- or micrometer-size particles cannot be applied to the bulk rock in field sites. In this study, we report the effects of particle sizes on the carbonation of wollastonite (CaSiO 3 ) at 60 °C and 100 bar in water-bearing scCO 2 . After normalization by the surface area, the thickness of the reacted wollastonite layer on the surfaces was independent of particle sizes. After 20 h, the reaction was not controlled by the kinetics of surface reactions but by the diffusion of water-bearing scCO 2 across the product layer on wollastonite surfaces. Among the products of reaction, amorphous silica, rather than calcite, covered the wollastonite surface and acted as a diffusion barrier to water-bearing scCO 2 . The product layer was not highly porous, with a specific surface area 10 times smaller than that of the altered amorphous silica formed at the wollastonite surface in aqueous solution. These findings can help us evaluate the impacts of mineral carbonation in water-bearing scCO 2 .

  13. Long-term C-CO2 emissions and carbon crop residue mineralization in an oxisol under different tillage and crop rotation systems

    Directory of Open Access Journals (Sweden)

    Ben-Hur Costa de Campos

    2011-06-01

    Full Text Available Soil C-CO2 emissions are sensitive indicators of management system impacts on soil organic matter (SOM. The main soil C-CO2 sources at the soil-plant interface are the decomposition of crop residues, SOM turnover, and respiration of roots and soil biota. The objectives of this study were to evaluate the impacts of tillage and cropping systems on long-term soil C-CO2 emissions and their relationship with carbon (C mineralization of crop residues. A long-term experiment was conducted in a Red Oxisol in Cruz Alta, RS, Brazil, with subtropical climate Cfa (Köppen classification, mean annual precipitation of 1,774 mm and mean annual temperature of 19.2 ºC. Treatments consisted of two tillage systems: (a conventional tillage (CT and (b no tillage (NT in combination with three cropping systems: (a R0- monoculture system (soybean/wheat, (b R1- winter crop rotation (soybean/wheat/soybean/black oat, and (c R2- intensive crop rotation (soybean/ black oat/soybean/black oat + common vetch/maize/oilseed radish/wheat. The soil C-CO2 efflux was measured every 14 days for two years (48 measurements, by trapping the CO2 in an alkaline solution. The soil gravimetric moisture in the 0-0.05 m layer was determined concomitantly with the C-CO2 efflux measurements. The crop residue C mineralization was evaluated with the mesh-bag method, with sampling 14, 28, 56, 84, 112, and 140 days after the beginning of the evaluation period for C measurements. Four C conservation indexes were used to assess the relation between C-CO2 efflux and soil C stock and its compartments. The crop residue C mineralization fit an exponential model in time. For black oat, wheat and maize residues, C mineralization was higher in CT than NT, while for soybean it was similar. Soil moisture was higher in NT than CT, mainly in the second year of evaluation. There was no difference in tillage systems for annual average C-CO2 emissions, but in some individual evaluations, differences between

  14. Hidden shift of the ionome of plants exposed to elevated CO2 depletes minerals at the base of human nutrition

    Science.gov (United States)

    Loladze, Irakli

    2014-01-01

    Mineral malnutrition stemming from undiversified plant-based diets is a top global challenge. In C3 plants (e.g., rice, wheat), elevated concentrations of atmospheric carbon dioxide (eCO2) reduce protein and nitrogen concentrations, and can increase the total non-structural carbohydrates (TNC; mainly starch, sugars). However, contradictory findings have obscured the effect of eCO2 on the ionome—the mineral and trace-element composition—of plants. Consequently, CO2-induced shifts in plant quality have been ignored in the estimation of the impact of global change on humans. This study shows that eCO2 reduces the overall mineral concentrations (−8%, 95% confidence interval: −9.1 to −6.9, p carbon:minerals in C3 plants. The meta-analysis of 7761 observations, including 2264 observations at state of the art FACE centers, covers 130 species/cultivars. The attained statistical power reveals that the shift is systemic and global. Its potential to exacerbate the prevalence of ‘hidden hunger’ and obesity is discussed. DOI: http://dx.doi.org/10.7554/eLife.02245.001 PMID:24867639

  15. 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

    To date, a number of methods to accelerate natural weathering or in other words increase the CO{sub 2} uptake rate of various minerals have been suggested; commonly this is known as mineral carbonation or CO{sub 2} mineralisation. A brief literature review of recently published articles in this field is presented, showing that the interest in mineral carbonation is increasing. However, it should be noted that mineral carbonation is only one option in a larger portfolio of various carbon dioxide capture and storage (CCS) alternatives. Unlike many other options, the CO{sub 2} mineralisation option considered in this thesis is largely founded on the possibility to utilise the exothermic nature of magnesium carbonation and based on this notion, it has been divided into three steps. The first two steps are energy demanding, while the third step is energy 'negative', and in theory, the source of the energy required in the first two steps. Unfortunately, however, the energy demanded by the first two steps, Mg extraction and Mg(OH){sub 2} production, is (currently) much higher than what could be generated by the subsequent Mg(OH){sub 2} carbonation step. Nevertheless, opportunities to reduce the energy intensity of the process in question are still being investigated, and while an energy-neutral carbonation process might be difficult to achieve, energy requirements can still be rendered industrially acceptable (and comparable to or even better than for other CCS methods). The main focus of this thesis lies with the third step, Mg(OH){sub 2} carbonation, which is performed using a pressurised fluidised bed (PFB). The elevated CO{sub 2} pressure conditions (typically approx 20 bar) allow for the carbonation reaction to take place at higher temperatures (typically approx 500 deg C) than otherwise due to thermodynamic constraints on carbonate stability. The increase in reaction rate as a function of temperature follows the Arrhenius equation of exponential increase

  16. On the interaction of pure and impure supercritical CO2 with rock forming minerals in saline aquifers: An experimental geochemical approach

    International Nuclear Information System (INIS)

    Wilke, Franziska D.H.; Vásquez, Mónica; Wiersberg, Thomas; Naumann, Rudolf; Erzinger, Jörg

    2012-01-01

    The aim of this experimental study was to evaluate and compare the geochemical impact of pure and impure CO 2 on rock forming minerals of possible CO 2 storage reservoirs. This geochemical approach takes into account the incomplete purification of industrial captured CO 2 and the related effects during injection, and provides relevant data for long-term storage simulations of this specific greenhouse gas. Batch experiments were conducted to investigate the interactions of supercritical CO 2 , brine and rock-forming mineral concentrates (albite, microcline, kaolinite, biotite, muscovite, calcite, dolomite and anhydrite) using a newly developed experimental setup. After up to 42 day (1000 h) experiments using pure and impure supercritical CO 2 the dissolution and solution characteristics were examined by XRD, XRF, SEM and EDS for the solid, and ICP–MS and IC for the fluid reactants, respectively. Experiments with mixtures of supercritical CO 2 (99.5 vol.%) and SO 2 or NO 2 impurities (0.5 vol.%) suggest the formation of H 2 SO 4 and HNO 3 , reflected in pH values between 1 and 4 for experiments with silicates and anhydrite and between 5 and 6 for experiments with carbonates. These acids should be responsible for the general larger amount of cations dissolved from the mineral phases compared to experiments using pure CO 2 . For pure CO 2 a pH of around 4 was obtained using silicates and anhydrite, and 7–8 for carbonates. Dissolution of carbonates was observed after both pure and impure CO 2 experiments. Anhydrite was corroded by approximately 50 wt.% and gypsum precipitated during experiments with supercritical CO 2 + NO 2 . Silicates do not exhibit visible alterations during all experiments but released an increasing amount of cations in the reaction fluid during experiments with impure CO 2 . Nonetheless, precipitated secondary carbonates could not be identified.

  17. Chemical and Biological Catalytic Enhancement of Weathering of Silicate Minerals and industrial wastes as a Novel Carbon Capture and Storage Technology

    Science.gov (United States)

    Park, A. H. A.

    2014-12-01

    Increasing concentration of CO2 in the atmosphere is attributed to rising consumption of fossil fuels around the world. The development of solutions to reduce CO2 emissions to the atmosphere is one of the most urgent needs of today's society. One of the most stable and long-term solutions for storing CO2 is via carbon mineralization, where minerals containing metal oxides of Ca or Mg are reacted with CO2 to produce thermodynamically stable Ca- and Mg-carbonates that are insoluble in water. Carbon mineralization can be carried out in-situ or ex-situ. In the case of in-situ mineralization, the degree of carbonation is thought to be limited by both mineral dissolution and carbonate precipitation reaction kinetics, and must be well understood to predict the ultimate fate of CO2 within geological reservoirs. While the kinetics of in-situ mineral trapping via carbonation is naturally slow, it can be enhanced at high temperature and high partial pressure of CO2. The addition of weak organic acids produced from food waste has also been shown to enhance mineral weathering kinetics. In the case of the ex-situ carbon mineralization, the role of these ligand-bearing organic acids can be further amplified for silicate mineral dissolution. Unfortunately, high mineral dissolution rates often lead to the formation of a silica-rich passivation layer on the surface of silicate minerals. Thus, the use of novel solvent mixture that allows chemically catalyzed removal of this passivation layer during enhanced Mg-leaching surface reaction has been proposed and demonstrated. Furthermore, an engineered biological catalyst, carbonic anhydrase, has been developed and evaluated to accelerate the hydration of CO2, which is another potentially rate-limiting step of the carbonation reaction. The development of these novel catalytic reaction schemes has significantly improved the overall efficiency and sustainability of in-situ and ex-situ mineral carbonation technologies and allowed direct

  18. 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,

  19. Enzymatic, urease-mediated mineralization of gellan gum hydrogel with calcium carbonate, magnesium-enriched calcium carbonate and magnesium carbonate for bone regeneration applications.

    Science.gov (United States)

    Douglas, Timothy E L; Łapa, Agata; Samal, Sangram Keshari; Declercq, Heidi A; Schaubroeck, David; Mendes, Ana C; der Voort, Pascal Van; Dokupil, Agnieszka; Plis, Agnieszka; De Schamphelaere, Karel; Chronakis, Ioannis S; Pamuła, Elżbieta; Skirtach, Andre G

    2017-12-01

    Mineralization of hydrogel biomaterials is considered desirable to improve their suitability as materials for bone regeneration. Calcium carbonate (CaCO 3 ) has been successfully applied as a bone regeneration material, but hydrogel-CaCO 3 composites have received less attention. Magnesium (Mg) has been used as a component of calcium phosphate biomaterials to stimulate bone-forming cell adhesion and proliferation and bone regeneration in vivo, but its effect as a component of carbonate-based biomaterials remains uninvestigated. In the present study, gellan gum (GG) hydrogels were mineralized enzymatically with CaCO 3 , Mg-enriched CaCO 3 and magnesium carbonate to generate composite biomaterials for bone regeneration. Hydrogels loaded with the enzyme urease were mineralized by incubation in mineralization media containing urea and different ratios of calcium and magnesium ions. Increasing the magnesium concentration decreased mineral crystallinity. At low magnesium concentrations calcite was formed, while at higher concentrations magnesian calcite was formed. Hydromagnesite (Mg 5 (CO 3 ) 4 (OH) 2 .4H 2 O) formed at high magnesium concentration in the absence of calcium. The amount of mineral formed and compressive strength decreased with increasing magnesium concentration in the mineralization medium. The calcium:magnesium elemental ratio in the mineral formed was higher than in the respective mineralization media. Mineralization of hydrogels with calcite or magnesian calcite promoted adhesion and growth of osteoblast-like cells. Hydrogels mineralized with hydromagnesite displayed higher cytotoxicity. In conclusion, enzymatic mineralization of GG hydrogels with CaCO 3 in the form of calcite successfully reinforced hydrogels and promoted osteoblast-like cell adhesion and growth, but magnesium enrichment had no definitive positive effect. Copyright © 2017 John Wiley & Sons, Ltd. Copyright © 2017 John Wiley & Sons, Ltd.

  20. Calculation of Site-specific Carbon-isotope Fractionation in Pedogenic Oxide Minerals

    Energy Technology Data Exchange (ETDEWEB)

    Rustad, James R.; Zarzycki, Piotr

    2008-07-29

    Ab initio molecular dynamics and quantum chemistry techniques are used to calculate the structure, vibrational frequencies, and carbon-isotope fractionation factors of the carbon dioxide component [CO2(m)] of soil (oxy)hydroxide minerals goethite, diaspore, and gibbsite. We have identified two possible pathways of incorporation of CO2(m) into (oxy)hydroxide crystal structures: one in which the C4+ substitutes for four H+ [CO2(m)A] and another in which C4+ substitutes for (Al3+,Fe3+) + H+ [CO2(m)B]. Calculations of isotope fractionation factors give large differences between the two structures, with the CO2(m)A being isotopically lighter than CO2(m)B by ≈10 per mil in the case of gibbsite and nearly 20 per mil in the case of goethite. The reduced partition function ratio of CO2(m)B structure in goethite differs from CO2(g) by <1 per mil. The predicted fractionation for gibbsite is >10 per mil higher, close to those measured for calcite and aragonite. The surprisingly large difference in the carbon-isotope fractionation factor between the CO2(m)A and CO2(m)B structures within a given mineral suggests that the isotopic signatures of soil (oxy)hydroxide could be heterogeneous.

  1. Microbial and Chemical Enhancement of In-Situ Carbon Mineralization in Geological Formation

    Energy Technology Data Exchange (ETDEWEB)

    Matter, J.; Chandran, K.

    2013-05-31

    Predictions of global energy usage suggest a continued increase in carbon emissions and rising concentrations of CO{sub 2} in the atmosphere unless major changes are made to the way energy is produced and used. Various carbon capture and storage (CCS) technologies are currently being developed, but unfortunately little is known regarding the fundamental characteristics of CO{sub 2}-mineral reactions to allow a viable in-situ carbon mineralization that would provide the most permanent and safe storage of geologically-injected CO{sub 2}. The ultimate goal of this research project was to develop a microbial and chemical enhancement scheme for in-situ carbon mineralization in geologic formations in order to achieve long-term stability of injected CO{sub 2}. Thermodynamic and kinetic studies of CO{sub 2}-mineral-brine systems were systematically performed to develop the in-situ mineral carbonation process that utilizes organic acids produced by a microbial reactor. The major participants in the project are three faculty members and their graduate and undergraduate students at the School of Engineering and Applied Science and at the Lamont-Doherty Earth Observatory at Columbia University: Alissa Park in Earth and Environmental Engineering & Chemical Engineering (PI), Juerg Matter in Earth and Environmental Science (Co-PI), and Kartik Chandran in Earth and Environmental Engineering (Co-PI). Two graduate students, Huangjing Zhao and Edris Taher, were trained as a part of this project as well as a number of graduate students and undergraduate students who participated part-time. Edris Taher received his MS degree in 2012 and Huangjing Zhao will defend his PhD on Jan. 15th, 2014. The interdisciplinary training provided by this project was valuable to those students who are entering into the workforce in the United States. Furthermore, the findings from this study were and will be published in referred journals to disseminate the results. The list of the papers is given at

  2. Nitrogen and Carbon Cycling in a Grassland Community Ecosystem as Affected by Elevated Atmospheric CO2

    Directory of Open Access Journals (Sweden)

    H. A. Torbert

    2012-01-01

    Full Text Available Increasing global atmospheric carbon dioxide (CO2 concentration has led to concerns regarding its potential effects on terrestrial ecosystems and the long-term storage of carbon (C and nitrogen (N in soil. This study examined responses to elevated CO2 in a grass ecosystem invaded with a leguminous shrub Acacia farnesiana (L. Willd (Huisache. Seedlings of Acacia along with grass species were grown for 13 months at CO2 concentrations of 385 (ambient, 690, and 980 μmol mol−1. Elevated CO2 increased both C and N inputs from plant growth which would result in higher soil C from litter fall, root turnover, and excretions. Results from the incubation indicated an initial (20 days decrease in N mineralization which resulted in no change in C mineralization. However, after 40 and 60 days, an increase in both C and N mineralization was observed. These increases would indicate that increases in soil C storage may not occur in grass ecosystems that are invaded with Acacia over the long term.

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

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Zhengrong [Yale Univ., New Haven, CT (United States); Qiu, Lin [Yale Univ., New Haven, CT (United States); Zhang, Shuang [Yale Univ., New Haven, CT (United States); Bolton, Edward [Yale Univ., New Haven, CT (United States); Bercovici, David [Yale Univ., New Haven, CT (United States); Ague, Jay [Yale Univ., New Haven, CT (United States); Karato, Shun-Ichiro [Yale Univ., New Haven, CT (United States); Oristaglio, Michael [Yale Univ., New Haven, CT (United States); Zhu, Wen-Iu [Univ. of Maryland, College Park, MD (United States); Lisabeth, Harry [Univ. of Maryland, College Park, MD (United States); Johnson, Kevin [Univ. of Hawaii, Honolulu, HI (United States)

    2014-09-30

    A program of laboratory experiments, modeling and fieldwork was carried out at Yale University, University of Maryland, and University of Hawai‘i, under a DOE Award (DE-FE0004375) to study mineral carbonation as a practical method of geologic carbon sequestration. Mineral carbonation, also called carbon mineralization, is the conversion of (fluid) carbon dioxide into (solid) carbonate minerals in rocks, by way of naturally occurring chemical reactions. Mafic and ultramafic rocks, such as volcanic basalt, are natural candidates for carbonation, because the magnesium and iron silicate minerals in these rocks react with brines of dissolved carbon dioxide to form carbonate minerals. By trapping carbon dioxide (CO2) underground as a constituent of solid rock, carbonation of natural basalt formations would be a secure method of sequestering CO2 captured at power plants in efforts to mitigate climate change. Geochemical laboratory experiments at Yale, carried out in a batch reactor at 200°C and 150 bar (15 MPa), studied carbonation of the olivine mineral forsterite (Mg2SiO4) reacting with CO2 brines in the form of sodium bicarbonate (NaHCO3) solutions. The main carbonation product in these reactions is the carbonate mineral magnesite (MgCO3). A series of 32 runs varied the reaction time, the reactive surface area of olivine grains and powders, the concentration of the reacting fluid, and the starting ratio of fluid to olivine mass. These experiments were the first to study the rate of olivine carbonation under passive conditions approaching equilibrium. The results show that, in a simple batch reaction, olivine carbonation is fastest during the first 24 hours and then slows significantly and even reverses. A natural measure of the extent of carbonation is a quantity called the carbonation fraction, which compares the amount of carbon removed from solution, during a run, to the maximum amount

  4. Procedure to use phosphogypsum industrial waste for mineral CO{sub 2} sequestration

    Energy Technology Data Exchange (ETDEWEB)

    Cardenas-Escudero, C. [Departamento de Fisica de la Materia Condensada, Facultad de Fisica, Universidad de Sevilla, Av. Reina Mercedes s/n, 41012 Seville (Spain); Instituto de Ciencia de Materiales de Sevilla (CSIC-US), Av. Americo Vespucio, 49, 41092 Seville (Spain); Morales-Florez, V., E-mail: victor.morales@icmse.csic.es [Instituto de Ciencia de Materiales de Sevilla (CSIC-US), Av. Americo Vespucio, 49, 41092 Seville (Spain); Perez-Lopez, R. [Departamento de Geologia, Facultad de Ciencias Experimentales, Universidad de Huelva, Campus Universitario Campus del Carmen, Avenida de las Fuerzas Armadas, 21071 Huelva (Spain); Instituto de Diagnostico Ambiental y Estudios del Agua (IDAeA-CSIC), Jordi Girona 18, 08034 Barcelona (Spain); Santos, A. [Departamento de Ciencias de la Tierra, Universidad de Cadiz, Campus del Rio San Pedro, Av. Republica Saharaui s/n, 11510 Puerto Real (Spain); Esquivias, L. [Departamento de Fisica de la Materia Condensada, Facultad de Fisica, Universidad de Sevilla, Av. Reina Mercedes s/n, 41012 Seville (Spain); Instituto de Ciencia de Materiales de Sevilla (CSIC-US), Av. Americo Vespucio, 49, 41092 Seville (Spain)

    2011-11-30

    Highlights: Black-Right-Pointing-Pointer Phosphogypsum wastes are proposed to reduce CO{sub 2} greenhouse gas emissions. Black-Right-Pointing-Pointer Phosphogypsum dissolution with NaOH results in Ca(OH){sub 2} precipitation and Na{sub 2}SO{sub 4}. Black-Right-Pointing-Pointer Aqueous carbonation of Ca(OH){sub 2} with CO{sub 2} results in the CaCO{sub 3} precipitation. Black-Right-Pointing-Pointer Metals contained in the phosphogypsum are transferred to the final calcite. Black-Right-Pointing-Pointer Applications of CaCO{sub 3} and Na{sub 2}SiO{sub 4} by-products are proposed to improve viability. - Abstract: Industrial wet phosphoric acid production in Huelva (SW Spain) has led to the controversial stockpiling of waste phosphogypsum by-products, resulting in the release of significant quantities of toxic impurities in salt marshes in the Tinto river estuary. In the framework of the fight against global climate change and the effort to reduce carbon dioxide emissions, a simple and efficient procedure for CO{sub 2} mineral sequestration is presented in this work, using phosphogypsum waste as a calcium source. Our results demonstrate the high efficiency of portlandite precipitation by phosphogypsum dissolution using an alkaline soda solution. Carbonation experiments performed at ambient pressure and temperature resulted in total conversion of the portlandite into carbonate. The fate of trace elements present in the phosphogypsum waste was also investigated, and trace impurities were found to be completely transferred to the final calcite. We believe that the procedure proposed here should be considered not only as a solution for reducing old stockpiles of phosphogypsum wastes, but also for future phosphoric acid and other gypsum-producing industrial processes, resulting in more sustainable production.

  5. Geochemical modelling of CO2-water-rock interactions for carbon storage : data requirements and outputs

    International Nuclear Information System (INIS)

    Kirste, D.

    2008-01-01

    A geochemical model was used to predict the short-term and long-term behaviour of carbon dioxide (CO 2 ), formation water, and reservoir mineralogy at a carbon sequestration site. Data requirements for the geochemical model included detailed mineral petrography; formation water chemistry; thermodynamic and kinetic data for mineral phases; and rock and reservoir physical characteristics. The model was used to determine the types of outputs expected for potential CO 2 storage sites and natural analogues. Reaction path modelling was conducted to determine the total reactivity or CO 2 storage capability of the rock by applying static equilibrium and kinetic simulations. Potential product phases were identified using the modelling technique, which also enabled the identification of the chemical evolution of the system. Results of the modelling study demonstrated that changes in porosity and permeability over time should be considered during the site selection process.

  6. Carbon Mineralization by Aqueous Precipitation for Beneficial Use of CO2 from Flue Gas

    Energy Technology Data Exchange (ETDEWEB)

    Brent Constantz; Randy Seeker; Martin Devenney

    2010-06-30

    Calera's innovative Mineralization via Aqueous Precipitation (MAP) technology for the capture and conversion of CO{sub 2} to useful materials for use in the built environment was further developed and proven in the Phase 1 Department of Energy Grant. The process was scaled to 300 gallon batch reactors and subsequently to Pilot Plant scale for the continuous production of product with the production of reactive calcium carbonate material that was evaluated as a supplementary cementitious material (SCM). The Calera SCM{trademark} was evaluated as a 20% replacement for ordinary portland cement and demonstrated to meet the industry specification ASTM 1157 which is a standard performance specification for hydraulic cement. The performance of the 20% replacement material was comparable to the 100% ordinary portland cement control in terms of compressive strength and workability as measured by a variety of ASTM standard tests. In addition to the performance metrics, detailed characterization of the Calera SCM was performed using advanced analytical techniques to better understand the material interaction with the phases of ordinary portland cement. X-ray synchrotron diffraction studies at the Advanced Photon Source in Argonne National Lab confirmed the presence of an amorphous phase(s) in addition to the crystalline calcium carbonate phases in the reactive carbonate material. The presence of carboaluminate phases as a result of the interaction of the reactive carbonate materials with ordinary portland cement was also confirmed. A Life Cycle Assessment was completed for several cases based on different Calera process configurations and compared against the life cycle of ordinary portland cement. In addition to the materials development efforts, the Calera technology for the production of product using an innovative building materials demonstration plant was developed beyond conceptual engineering to a detailed design with a construction schedule and cost estimate.

  7. Modeling of fate and transport of co-injection of H2S with CO2 in deep saline formations

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, W.; Xu, T.; Li, Y.

    2010-12-15

    The geological storage of CO{sub 2} in deep saline formations is increasing seen as a viable strategy to reduce the release of greenhouse gases into the atmosphere. However, costs of capture and compression of CO{sub 2} from industrial waste streams containing small quantities of sulfur and nitrogen compounds such as SO{sub 2}, H{sub 2}S and N{sub 2} are very expensive. Therefore, studies on the co-injection of CO{sub 2} containing other acid gases from industrial emissions are very important. In this paper, numerical simulations were performed to study the co-injection of H{sub 2}S with CO{sub 2} in sandstone and carbonate formations. Results indicate that the preferential dissolution of H{sub 2}S gas (compared with CO{sub 2} gas) into formation water results in the delayed breakthrough of H{sub 2}S gas. Co-injection of H{sub 2}S results in the precipitation of pyrite through interactions between the dissolved H{sub 2}S and Fe{sup 2+} from the dissolution of Fe-bearing minerals. Additional injection of H{sub 2}S reduces the capabilities for solubility and mineral trappings of CO{sub 2} compared to the CO{sub 2} only case. In comparison to the sandstone (siliciclastic) formation, the carbonate formation is less favorable to the mineral sequestration of CO{sub 2}. Different from CO{sub 2} mineral trapping, the presence of Fe-bearing siliciclastic and/or carbonate is more favorable to the H{sub 2}S mineral trapping.

  8. Scientific and Engineering Progress in CO2 Mineralization Using Industrial Waste and Natural Minerals

    Directory of Open Access Journals (Sweden)

    Heping Xie

    2015-03-01

    Full Text Available The issues of reducing CO2 levels in the atmosphere, sustainably utilizing natural mineral resources, and dealing with industrial waste offer challenging opportunities for sustainable development in energy and the environment. The latest advances in CO2 mineralization technology involving natural minerals and industrial waste are summarized in this paper, with great emphasis on the advancement of fundamental science, economic evaluation, and engineering applications. We discuss several leading large-scale CO2 mineralization methodologies from a technical and engineering-science perspective. For each technology option, we give an overview of the technical parameters, reaction pathway, reactivity, procedural scheme, and laboratorial and pilot devices. Furthermore, we present a discussion of each technology based on experimental results and the literature. Finally, current gaps in knowledge are identified in the conclusion, and an overview of the challenges and opportunities for future research in this field is provided.

  9. 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.

  10. Depth-Dependent Mineral Soil CO2 Production Processes: Sensitivity to Harvesting-Induced Changes in Soil Climate.

    Science.gov (United States)

    Kellman, Lisa; Myette, Amy; Beltrami, Hugo

    2015-01-01

    Forest harvesting induces a step change in the climatic variables (temperature and moisture), that control carbon dioxide (CO2) production arising from soil organic matter decomposition within soils. Efforts to examine these vertically complex relationships in situ within soil profiles are lacking. In this study we examined how the climatic controls on CO2 production change within vertically distinct layers of the soil profile in intact and clearcut forest soils of a humid temperate forest system of Atlantic Canada. We measured mineral soil temperature (0, 5, 10, 20, 50 and 100 cm depth) and moisture (0-15 cm and 30-60 cm depth), along with CO2 surface efflux and subsurface concentrations (0, 2.5, 5, 10, 20, 35, 50, 75 and 100 cm depth) in 1 m deep soil pits at 4 sites represented by two forest-clearcut pairs over a complete annual cycle. We examined relationships between surface efflux at each site, and soil heat, moisture, and mineral soil CO2 production. Following clearcut harvesting we observed increases in temperature through depth (1-2°C annually; often in excess of 4°C in summer and spring), alongside increases in soil moisture (30%). We observed a systematic breakdown in the expected exponential relationship between CO2 production and heat with mineral soil depth, consistent with an increase in the role moisture plays in constraining CO2 production. These findings should be considered in efforts to model and characterize mineral soil organic matter decomposition in harvested forest soils.

  11. The Carbonation of Wollastonite: A Model Reaction to Test Natural and Biomimetic Catalysts for Enhanced CO2 Sequestration

    Directory of Open Access Journals (Sweden)

    Fulvio Di Lorenzo

    2018-05-01

    Full Text Available One of the most promising strategies for the safe and permanent disposal of anthropogenic CO2 is its conversion into carbonate minerals via the carbonation of calcium and magnesium silicates. However, the mechanism of such a reaction is not well constrained, and its slow kinetics is a handicap for the implementation of silicate mineral carbonation as an effective method for CO2 capture and storage (CCS. Here, we studied the different steps of wollastonite (CaSiO3 carbonation (silicate dissolution → carbonate precipitation as a model CCS system for the screening of natural and biomimetic catalysts for this reaction. Tested catalysts included carbonic anhydrase (CA, a natural enzyme that catalyzes the reversible hydration of CO2(aq, and biomimetic metal-organic frameworks (MOFs. Our results show that dissolution is the rate-limiting step for wollastonite carbonation. The overall reaction progresses anisotropically along different [hkl] directions via a pseudomorphic interface-coupled dissolution–precipitation mechanism, leading to partial passivation via secondary surface precipitation of amorphous silica and calcite, which in both cases is anisotropic (i.e., (hkl-specific. CA accelerates the final carbonate precipitation step but hinders the overall carbonation of wollastonite. Remarkably, one of the tested Zr-based MOFs accelerates the dissolution of the silicate. The use of MOFs for enhanced silicate dissolution alone or in combination with other natural or biomimetic catalysts for accelerated carbonation could represent a potentially effective strategy for enhanced mineral CCS.

  12. Integrating Steel Production with Mineral Carbon Sequestration

    Energy Technology Data Exchange (ETDEWEB)

    Klaus Lackner; Paul Doby; Tuncel Yegulalp; Samuel Krevor; Christopher Graves

    2008-05-01

    The objectives of the project were (i) to develop a combination iron oxide production and carbon sequestration plant that will use serpentine ores as the source of iron and the extraction tailings as the storage element for CO2 disposal, (ii) the identification of locations within the US where this process may be implemented and (iii) to create a standardized process to characterize the serpentine deposits in terms of carbon disposal capacity and iron and steel production capacity. The first objective was not accomplished. The research failed to identify a technique to accelerate direct aqueous mineral carbonation, the limiting step in the integration of steel production and carbon sequestration. Objective (ii) was accomplished. It was found that the sequestration potential of the ultramafic resource surfaces in the US and Puerto Rico is approximately 4,647 Gt of CO2 or over 500 years of current US production of CO2. Lastly, a computer model was developed to investigate the impact of various system parameters (recoveries and efficiencies and capacities of different system components) and serpentinite quality as well as incorporation of CO2 from sources outside the steel industry.

  13. Mineral CO2 sequestration in basalts and ultra-basic rocks: impact of secondary silicated phases on the carbonation process

    International Nuclear Information System (INIS)

    Sissmann, Olivier

    2013-01-01

    The formation of carbonates constitutes a stable option for carbon dioxide (CO 2 ) geological sequestration, and is prone to play a significant role in reducing emissions of anthropic origin. However, our comprehension of the carbonation mechanism, as well as of the kinetics limitations encountered during this chemical reaction, remains poorly developed. Though there is a large number of studies focusing on the dissolution kinetics of basic silicates and on the precipitation of carbonates, few have inquired about the impact that the formation of non-carbonated secondary phases can have on these reaction's kinetics. It is the approach chosen here, as only solid knowledge of the global carbonation mechanism can make this process predictive and efficient. Experimental data on dissolution and carbonation have therefore been determined in batch reactors, on relevant minerals and rocks. Firstly, we studied the carbonation of olivine (a major phase within peridotites and minor within basalts) at 90 deg. C and under pCO 2 of 280 bars. The dissolution of San Carlos olivine (Mg 1.76 Fe 0.24 SiO 4 ) is slowed down by the formation of a surface silica gel, when the fluid reaches equilibrium with amorphous silica. The transport of species to the reactive medium becomes the limiting step of the process, slowing down the dissolution process of San Carlos olivine by 5 orders of magnitude. However, this passivation doesn't occur during the alteration of Ca-olivine (Ca 2 SiO 4 ), though a surface silica layer does form. This comparison suggests that it isn't the structure of the silicate but its chemical composition, which controls the transport properties through the interfacial layer. The second part explores the effects of organic ligands and of temperature variations on the formation of those phases. The addition of citrate at 90 deg. C increases the kinetics of San Carlos olivine by one order of magnitude, and allows the release of enough Mg in the aqueous medium to form

  14. Morphological changes during enhanced carbonation of asbestos containing material and its comparison to magnesium silicate minerals

    International Nuclear Information System (INIS)

    Gadikota, Greeshma; Natali, Claudio; Boschi, Chiara; Park, Ah-Hyung Alissa

    2014-01-01

    The disintegration of asbestos containing materials (ACM) over time can result in the mobilization of toxic chrysotile ((Mg, Fe) 3 Si 2 O 5 (OH) 4 )) fibers. Therefore, carbonation of these materials can be used to alter the fibrous morphology of asbestos and help mitigate anthropogenic CO 2 emissions, depending on the amount of available alkaline metal in the materials. A series of high pressure carbonation experiments were performed in a batch reactor at P CO2 of 139 atm using solvents containing different ligands (i.e., oxalate and acetate). The results of ACM carbonation were compared to those of magnesium silicate minerals which have been proposed to permanently store CO 2 via mineral carbonation. The study revealed that oxalate even at a low concentration of 0.1 M was effective in enhancing the extent of ACM carbonation and higher reaction temperatures also resulted in increased ACM carbonation. Formation of phases such as dolomite ((Ca, Mg)(CO 3 ) 2 ), whewellite (CaC 2 O 4 ·H 2 O) and glushinskite (MgC 2 O 4 ·2H 2 O) and a reduction in the chrysotile content was noted. Significant changes in the particle size and surface morphologies of ACM and magnesium silicate minerals toward non-fibrous structures were observed after their carbonation

  15. Dissolution and secondary mineral precipitation in basalts due to reactions with carbonic acid

    Science.gov (United States)

    Kanakiya, Shreya; Adam, Ludmila; Esteban, Lionel; Rowe, Michael C.; Shane, Phil

    2017-06-01

    One of the leading hydrothermal alteration processes in volcanic environments is when rock-forming minerals with high concentrations of iron, magnesium, and calcium react with CO2 and water to form carbonate minerals. This is used to the advantage of geologic sequestration of anthropogenic CO2. Here we experimentally investigate how mineral carbonation processes alter the rock microstructure due to CO2-water-rock interactions. In order to characterize these changes, CO2-water-rock alteration in Auckland Volcanic Field young basalts (less than 0.3 Ma) is studied before and after a 140 day reaction period. We investigate how whole core basalts with similar geochemistry but different porosity, permeability, pore geometry, and volcanic glass content alter due to CO2-water-rock reactions. Ankerite and aluminosilicate minerals precipitate as secondary phases in the pore space. However, rock dissolution mechanisms are found to dominate this secondary mineral precipitation resulting in an increase in porosity and decrease in rigidity of all samples. The basalt with the highest initial porosity and volcanic glass volume shows the most secondary mineral precipitation. At the same time, this sample exhibits the greatest increase in porosity and permeability, and a decrease in rock rigidity post reaction. For the measured samples, we observe a correlation between volcanic glass volume and rock porosity increase due to rock-fluid reactions. We believe this study can help understand the dynamic rock-fluid interactions when monitoring field scale CO2 sequestration projects in basalts.

  16. Interactions between CO2, saline water and minerals during geological storage of CO2

    International Nuclear Information System (INIS)

    Hellevang, Helge

    2006-06-01

    The topic of this thesis is to gain a better understanding of interactions between injected CO 2 , aqueous solutions and formation mineralogies. The main focus is concerned with the potential role mineral reactions play in safe long term storage of CO 2 . The work is divided into an experimental part concentrated on the potential of dawsonite (NaAl(OH) 2 CO 3 ) as a permanent storage host of CO 2 , and the development of a new geochemical code ACCRETE that is coupled with the ATHENA multiphase flow simulator. The thesis is composed of two parts: (I) the first part introducing CO 2 storage, geochemical interactions and related work; and (II) the second part that consists of the papers. Part I is composed as follows: Chapter 2 gives a short introduction to geochemical reactions considered important during CO 2 storage, including a thermodynamic framework. Chapter 3 presents objectives of numerical work related to CO 2 -water-rock interactions including a discussion of factors that influence the outcome of numerical simulations. Chapter 4 presents the main results from paper A to E. Chapter 5 give some details about further research that we propose based on the present work and related work in the project. Several new activities have emerged from research on CO 2 -water-rock interaction during the project. Several of the proposed activities are already initiated. Papers A to F are then listed in Part II of the thesis after the citation list. The thesis presents the first data on the reaction kinetics of dawsonite at different pH (Paper A), and comprehensive numerical simulations, both batch- and large scale 3D reactive transport, that illustrate the role different carbonates have for safe storage of CO 2 in geological formations (Papers C to F). The role of dawsonite in CO 2 storage settings is treated throughout the study (Papers A to E) After the main part of the thesis (Part I and II), two appendices are included: Appendix A lists reactions that are included in the

  17. Simulation of CO2–water–rock interactions on geologic CO2 sequestration under geological conditions of China

    International Nuclear Information System (INIS)

    Wang, Tianye; Wang, Huaiyuan; Zhang, Fengjun; Xu, Tianfu

    2013-01-01

    Highlights: • We determined the feasibilities of geologic CO 2 sequestration in China. • We determined the formation of gibbsite suggested CO 2 can be captured by rocks. • We suggested the mechanisms of CO 2 –water–rock interactions. • We found the corrosion and dissolution of the rock increased as temperature rose. -- Abstract: The main purpose of this study focused on the feasibility of geologic CO 2 sequestration within the actual geological conditions of the first Carbon Capture and Storage (CCS) project in China. This study investigated CO 2 –water–rock interactions under simulated hydrothermal conditions via physicochemical analyses and scanning electron microscopy (SEM). Mass loss measurement and SEM showed that corrosion of feldspars, silica, and clay minerals increased with increasing temperature. Corrosion of sandstone samples in the CO 2 -containing fluid showed a positive correlation with temperature. During reaction at 70 °C, 85 °C, and 100 °C, gibbsite (an intermediate mineral product) formed on the sample surface. This demonstrated mineral capture of CO 2 and supported the feasibility of geologic CO 2 sequestration. Chemical analyses suggested a dissolution–reprecipitation mechanism underlying the CO 2 –water–rock interactions. The results of this study suggested that mineral dissolution, new mineral precipitation, and carbonic acid formation-dissociation are closely interrelated in CO 2 –water–rock interactions

  18. The Ladbroke Grove-Katnook carbon dioxide natural laboratory: a recent CO{sub 2} accumulation in a lithic sandstone reservoir

    Energy Technology Data Exchange (ETDEWEB)

    Watson, M.N. [Adelaide Univ., SA (Australia). Australian School of Petroleum; Zwingmann, N. [CSIRO Petroleum, Bentley, WA (Australia); Lemon, N.M. [Santos Ltd., Adelaide, SA (Australia)

    2004-08-01

    The Ladbroke Grove and Katnook Gas Fields, within the western Otway Basin, southeastern South Australia, provide a natural laboratory to study the effects of CO{sub 2} on siliciclastic reservoirs. CO{sub 2} degassing from nearby volcanics has migrated into the methane accumulation of the Ladbroke Grove Field within the Pretty Hill Formation. CO{sub 2} levels in the Ladbroke Grove Field range from 26 to 57 mol% while Katnook has less than 1 mol%. In Ladbroke Grove, the CO{sub 2} has altered or dissolved most of the reactive minerals, somewhat constrained by the Pleistocene to Recent age of the CO{sub 2} influx. The developed late-stage kaolinite, quartz and less soluble carbonate are products of the reactions involving CO{sub 2} and reactive minerals. The major formation water types were identified using the geochemical code EQ3NR. Ladbroke Grove waters above the gas-water contact (GWC) have bicarbonate levels an order of magnitude higher than the other waters analysed. Below the GWC, Ladbroke Grove and Katnook formation waters have similar ionic compositions, however, pH levels in Ladbroke Grove are low relative to Katnook. The Ladbroke Grove Field has efficiently stored CO{sub 2} in a gaseous and aqueous phase since the influx began in the Pleistocene. In addition, due to the high amount of reactive minerals within the reservoir, mineralisation of ferroan carbonates has also occurred as a more permanent form of mineral storage of some of the CO{sub 2}. (author)

  19. Morphological changes during enhanced carbonation of asbestos containing material and its comparison to magnesium silicate minerals

    Energy Technology Data Exchange (ETDEWEB)

    Gadikota, Greeshma [Department of Chemical Engineering, Columbia University, 500 West 120th Street, New York, NY 10027 (United States); Natali, Claudio; Boschi, Chiara [Institute of Geosciences and Earth Resources – National Research Council, Pisa (Italy); Park, Ah-Hyung Alissa, E-mail: ap2622@columbia.edu [Department of Earth and Environmental Engineering, Columbia University, 500 West 120th Street, New York, NY 10027 (United States); Department of Chemical Engineering, Columbia University, 500 West 120th Street, New York, NY 10027 (United States); Lenfest Center for Sustainable Energy, Columbia University, 500 West 120th Street, New York, NY 10027 (United States)

    2014-01-15

    The disintegration of asbestos containing materials (ACM) over time can result in the mobilization of toxic chrysotile ((Mg, Fe){sub 3}Si{sub 2}O{sub 5}(OH){sub 4})) fibers. Therefore, carbonation of these materials can be used to alter the fibrous morphology of asbestos and help mitigate anthropogenic CO{sub 2} emissions, depending on the amount of available alkaline metal in the materials. A series of high pressure carbonation experiments were performed in a batch reactor at P{sub CO2} of 139 atm using solvents containing different ligands (i.e., oxalate and acetate). The results of ACM carbonation were compared to those of magnesium silicate minerals which have been proposed to permanently store CO{sub 2} via mineral carbonation. The study revealed that oxalate even at a low concentration of 0.1 M was effective in enhancing the extent of ACM carbonation and higher reaction temperatures also resulted in increased ACM carbonation. Formation of phases such as dolomite ((Ca, Mg)(CO{sub 3}){sub 2}), whewellite (CaC{sub 2}O{sub 4}·H{sub 2}O) and glushinskite (MgC{sub 2}O{sub 4}·2H{sub 2}O) and a reduction in the chrysotile content was noted. Significant changes in the particle size and surface morphologies of ACM and magnesium silicate minerals toward non-fibrous structures were observed after their carbonation.

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

    KAUST Repository

    Zhu, Xiuping

    2014-05-01

    Mineral carbonation can be used for CO2 sequestration, but the reaction rate is slow. In order to accelerate mineral carbonation, acid generated in a microbial electrolysis desalination and chemical-production cell (MEDCC) was examined to dissolve natural minerals rich in magnesium/calcium silicates (serpentine), and the alkali generated by the same process was used to absorb CO2 and precipitate magnesium/calcium carbonates. The concentrations of Mg2+ and Ca2+ dissolved from serpentine increased 20 and 145 times by using the acid solution. Under optimal conditions, 24mg of CO2 was absorbed into the alkaline solution and 13mg of CO2 was precipitated as magnesium/calcium carbonates over a fed-batch cycle (24h). Additionally, the MEDCC removed 94% of the COD (initially 822mg/L) and achieved 22% desalination (initially 35g/L NaCl). These results demonstrate the viability of this process for effective CO2 sequestration using renewable organic matter and natural minerals. © 2014 Elsevier Ltd.

  1. Magnesium sulphate’s influence on calcium carbonate minerals

    DEFF Research Database (Denmark)

    Nielsen, Mia Rohde

    The purpose of this PhD thesis was to explore the influence of magnesium sulphate (MgSO4 (aq)) on calcium carbonate (CaCO3) minerals and what role the MgSO40 ion pair had. CaCO3 minerals are abundant and widespread on Earth, particularly in marine environments, and have been so throughout Earth...

  2. Reactivity of micas and cap-rock in wet supercritical CO_2 with SO_2 and O_2 at CO_2 storage conditions

    International Nuclear Information System (INIS)

    Pearce, Julie K.; Dawson, Grant K.W.; Law, Alison C.K.; Biddle, Dean; Golding, Suzanne D.

    2016-01-01

    Seal or cap-rock integrity is a safety issue during geological carbon dioxide capture and storage (CCS). Industrial impurities such as SO_2, O_2, and NOx, may be present in CO_2 streams from coal combustion sources. SO_2 and O_2 have been shown recently to influence rock reactivity when dissolved in formation water. Buoyant water-saturated supercritical CO_2 fluid may also come into contact with the base of cap-rock after CO_2 injection. Supercritical fluid-rock reactions have the potential to result in corrosion of reactive minerals in rock, with impurity gases additionally present there is the potential for enhanced reactivity but also favourable mineral precipitation. The first observation of mineral dissolution and precipitation on phyllosilicates and CO_2 storage cap-rock (siliciclastic reservoir) core during water-saturated supercritical CO_2 reactions with industrial impurities SO_2 and O_2 at simulated reservoir conditions is presented. Phyllosilicates (biotite, phlogopite and muscovite) were reacted in contact with a water-saturated supercritical CO_2 containing SO_2, or SO_2 and O_2, and were also immersed in the gas-saturated bulk water. Secondary precipitated sulfate minerals were formed on mineral surfaces concentrated at sheet edges. SO_2 dissolution and oxidation resulted in solution pH decreasing to 0.74 through sulfuric acid formation. Phyllosilicate dissolution released elements to solution with ∼50% Fe mobilized. Geochemical modelling was in good agreement with experimental water chemistry. New minerals nontronite (smectite), hematite, jarosite and goethite were saturated in models. A cap-rock core siltstone sample from the Surat Basin, Australia, was also reacted in water-saturated supercritical CO_2 containing SO_2 or in pure supercritical CO_2. In the presence of SO_2, siderite and ankerite were corroded, and Fe-chlorite altered by the leaching of mainly Fe and Al. Corrosion of micas in the cap-rock was however not observed as the pH was

  3. 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 processes are considered, we expect CO 2 degassing and carbonate mineral precipitation from the brine inclusions of the ice sheet, which were saturated or highly supersaturated with respect to both the anhydrous (calcite, aragonite, vaterite) and hydrated (ikaite) carbonate minerals.

  4. Experimental reactivity with CO2 of clayey cap-rock and carbonate reservoir of the Paris basin

    International Nuclear Information System (INIS)

    Hubert, G.

    2009-01-01

    The constant increase in the quantity of carbon dioxide in the atmosphere is regarded as being the principal cause of the current global warming. The geological sequestration of CO 2 seems to be an ideal solution to reduce the increase of greenhouse gases (of which CO 2 ) in the atmosphere but only if the reservoir's cap-rock keep its integrity for several hundreds or thousands of years. Batch experimental simulations were conducted to observe the reactivity of a cap-rock made of clay and a carbonate reservoir with CO 2 at 80 C and 150 C for a pressure of 150 bar with an equilibrated water. The analytical protocol established allowed to compare the rocks before and after experimentations finding a very low reactivity, focusing on aluminium in phyllosilicates. Textural analysis shows that CO 2 does not affect the properties of adsorption and the specific surface. The study of carbonate reservoir by confocal microscopy has revealed phenomena of dissolution-precipitation which have no significant impact on chemistry and structure of the reservoir. The numerical simulations carried out on mineral reference as calcium montmorillonite or clinochlore show a significant reaction in the presence of CO 2 not achieved experimentally, probably due to lacunas in the thermodynamic databases or the kinetics of reactions. The simulations on Bure show no reaction on the major minerals confirming the results with batch experiments. (author)

  5. Experimental Precipitation of Carbonate Minerals: Effect of pH, Supersaturation and Substrate

    OpenAIRE

    Tetteh, Abednego

    2012-01-01

    Understanding the controlling factors and elucidating the requirements and conditions necessary for carbon dioxide (CO2) storage by mineral trapping (or carbonation) is of paramount interest for any technical application as a means for carbon dioxide capture and storage (CCS). The effect of pH, supersaturation and substrate has been studied using non-stirred batch reactors at initial constant temperature of 150 oC. These conditions are relevant for mineral trapping. A set of experiments was c...

  6. Carbon mineralization in surface and subsurface soils in a subtropical mixed forest in central China

    Science.gov (United States)

    Liu, F.; Tian, Q.

    2014-12-01

    About a half of soil carbon is stored in subsurface soil horizons, their dynamics have the potential to significantly affect carbon balancing in terrestrial ecosystems. However, the main factors regulating subsurface soil carbon mineralization are poorly understood. As affected by mountain humid monsoon, the subtropical mountains in central China has an annual precipitation of about 2000 mm, which causes strong leaching of ions and nutrition. The objectives of this study were to monitor subsurface soil carbon mineralization and to determine if it is affected by nutrient limitation. We collected soil samples (up to 1 m deep) at three locations in a small watershed with three soil layers (0-10 cm, 10-30 cm, below 30 cm). For the three layers, soil organic carbon (SOC) ranged from 35.8 to 94.4 mg g-1, total nitrogen ranged from 3.51 to 8.03 mg g-1, microbial biomass carbon (MBC) ranged from 170.6 to 718.4 μg g-1 soil. We measured carbon mineralization with the addition of N (100 μg N/g soil), P (50 μg P/g soil), and liable carbon (glucose labeled by 5 atom% 13C, at five levels: control, 10% MBC, 50% MBC, 100% MBC, 200% MBC). The addition of N and P had negligible effects on CO2 production in surface soil layers; in the deepest soil layer, the addition of N and P decreased CO2 production from 4.32 to 3.20 μg C g-1 soil carbon h-1. Glucose addition stimulated both surface and subsurface microbial mineralization of SOC, causing priming effects. With the increase of glucose addition rate from 10% to 200% MBC, the primed mineralization rate increased from 0.19 to 3.20 μg C g-1 soil carbon h-1 (fifth day of glucose addition). The magnitude of priming effect increased from 28% to 120% as soil layers go deep compare to the basal CO2 production (fifth day of 200% MBC glucose addition, basal CO2 production rate for the surface and the deepest soil was 11.17 and 2.88 μg C g-1 soil carbon h-1). These results suggested that the mineralization of subsurface carbon is more

  7. Sustained effects of atmospheric [CO2] and nitrogen availability on forest soil CO2 efflux

    Science.gov (United States)

    A. Christopher Oishi; Sari Palmroth; Kurt H. Johnsen; Heather R. McCarthy; Ram. Oren

    2014-01-01

    Soil CO2 efflux (Fsoil) is the largest source of carbon from forests and reflects primary productivity as well as how carbon is allocated within forest ecosystems. Through early stages of stand development, both elevated [CO2] and availability of soil nitrogen (N; sum of mineralization, deposition, and fixation) have been shown to increase gross primary productivity,...

  8. Comparison of the Wymark CO2 Reservoir with the Midale Beds at the Weyburn CO2 Injection Project

    International Nuclear Information System (INIS)

    Ryerson, F.; Johnson, J.

    2010-01-01

    The Devonian carbonates of the Duperow Formation on the western flank of the Williston Basin in southwest Saskatchewan contain natural accumulations of CO 2 , and may have done so for as long as 50 m.y. in the views of some investigations. These carbonate sediments are characterized by a succession of carbonate cycles capped by anhydrite-rich evaporites that are thought to act as seals to fluid migration. The Weyburn CO 2 injection site lies 400 km to the east in a series of Mississippian carbonates that were deposited in a similar depositional environment. That natural CO 2 can be stored long-term within carbonate strata has motivated the investigation of the Duperow rocks as a potential natural analogue to storage of anthropogenic CO 2 that may ultimately provide additional confidence for CO 2 sequestration in carbonate lithologies. For the Duperow strata to represent a legitimate analog for Midale injection and storage, the similarity in lithofacies, whole rock compositions, mineral compositions and porosity with the Midale Beds must be established. Previous workers have demonstrated the similarity of the lithofacies at both sites. Here we compare the whole rock compositions, mineralogy and mineral compositions. The major mineral phases at both locales are calcite, dolomite and anhydrite. In addition, accessory pyrite, fluorite and celestine are also observed. The distribution of porosity in the Midale Vuggy units is virtually identical to that of the Duperow Formation, but the Marly units of the Midale have significantly higher porosity. The Duperow Formation is topped by the Dinesmore evaporite that is particularly rich in anhydrite, and often contains authigenic K-feldspar. The chemistry of dolomite and calcite from the two localities also overlaps. Silicate minerals are in low abundance within the analyzed Duperow samples, < 3 wt% on a normative basis, with quartz the only phase identifiable in x-ray diffraction patterns. The Midale Beds contain

  9. 2,4,6-Trinitrotoluene mineralization and bacterial production rates of natural microbial assemblages from coastal sediments

    International Nuclear Information System (INIS)

    Montgomery, Michael T.; Coffin, Richard B.; Boyd, Thomas J.; Smith, Joseph P.; Walker, Shelby E.; Osburn, Christopher L.

    2011-01-01

    The nitrogenous energetic constituent, 2,4,6-Trinitrotoluene (TNT), is widely reported to be resistant to bacterial mineralization (conversion to CO 2 ); however, these studies primarily involve bacterial isolates from freshwater where bacterial production is typically limited by phosphorus. This study involved six surveys of coastal waters adjacent to three biome types: temperate broadleaf, northern coniferous, and tropical. Capacity to catabolize and mineralize TNT ring carbon to CO 2 was a common feature of natural sediment assemblages from these coastal environments (ranging to 270+/-38 μg C kg -1 d -1 ). More importantly, these mineralization rates comprised a significant proportion of total heterotrophic production. The finding that most natural assemblages surveyed from these ecosystems can mineralize TNT ring carbon to CO 2 is consistent with recent reports that assemblage components can incorporate TNT ring carbon into bacterial biomass. These data counter the widely held contention that TNT is recalcitrant to bacterial catabolism of the ring carbon in natural environments. - Highlights: → TNT mineralization is a common feature of natural bacterial assemblages in coastal sediments. → TNT mineralization rates comprised a significant proportion of total heterotrophic production. → These data counter the widely held contention that TNT is recalcitrant to bacterial catabolism of the ring carbon in natural environments. - The capacity to mineralize TNT ring carbon to CO 2 is a common feature of natural bacterial assemblages in coastal sediment.

  10. Process-based modeling of silicate mineral weathering responses to increasing atmospheric CO2 and climate change

    Science.gov (United States)

    Banwart, Steven A.; Berg, Astrid; Beerling, David J.

    2009-12-01

    A mathematical model describes silicate mineral weathering processes in modern soils located in the boreal coniferous region of northern Europe. The process model results demonstrate a stabilizing biological feedback mechanism between atmospheric CO2 levels and silicate weathering rates as is generally postulated for atmospheric evolution. The process model feedback response agrees within a factor of 2 of that calculated by a weathering feedback function of the type generally employed in global geochemical carbon cycle models of the Earth's Phanerozoic CO2 history. Sensitivity analysis of parameter values in the process model provides insight into the key mechanisms that influence the strength of the biological feedback to weathering. First, the process model accounts for the alkalinity released by weathering, whereby its acceleration stabilizes pH at values that are higher than expected. Although the process model yields faster weathering with increasing temperature, because of activation energy effects on mineral dissolution kinetics at warmer temperature, the mineral dissolution rate laws utilized in the process model also result in lower dissolution rates at higher pH values. Hence, as dissolution rates increase under warmer conditions, more alkalinity is released by the weathering reaction, helping maintain higher pH values thus stabilizing the weathering rate. Second, the process model yields a relatively low sensitivity of soil pH to increasing plant productivity. This is due to more rapid decomposition of dissolved organic carbon (DOC) under warmer conditions. Because DOC fluxes strongly influence the soil water proton balance and pH, this increased decomposition rate dampens the feedback between productivity and weathering. The process model is most sensitive to parameters reflecting soil structure; depth, porosity, and water content. This suggests that the role of biota to influence these characteristics of the weathering profile is as important, if not

  11. Threshold of carbonate saturation state determined by CO2 control experiment

    Directory of Open Access Journals (Sweden)

    A. Negishi

    2012-04-01

    Full Text Available Acidification of the oceans by increasing anthropogenic CO2 emissions will cause a decrease in biogenic calcification and an increase in carbonate dissolution. Previous studies have suggested that carbonate dissolution will occur in polar regions and in the deep sea where saturation state with respect to carbonate minerals (Ω will be a (aragonite saturation state value of >1. This is probably related to the dissolution of reef carbonate (Mg-calcite, which is more soluble than aragonite. However, the threshold of Ω for the dissolution of natural sediments has not been clearly determined. We designed an experimental dissolution system with conditions mimicking those of a natural coral reef, and measured the dissolution rates of aragonite in corals, and of Mg-calcite excreted by other marine organisms, under conditions of Ωa > 1, with controlled seawater pCO2. The experimental data show that dissolution of bulk carbonate sediments sampled from a coral reef occurs at Ωa values of 3.7 to 3.8. Mg-calcite derived from foraminifera and coralline algae dissolves at Ωa values between 3.0 and 3.2, and coralline aragonite starts to dissolve when Ωa = 1.0. We show that nocturnal carbonate dissolution of coral reefs occurs mainly by the dissolution of foraminiferans and coralline algae in reef sediments.

  12. Soil organic carbon redistribution by water erosion--the role of CO2 emissions for the carbon budget.

    Science.gov (United States)

    Wang, Xiang; Cammeraat, Erik L H; Romeijn, Paul; Kalbitz, Karsten

    2014-01-01

    A better process understanding of how water erosion influences the redistribution of soil organic carbon (SOC) is sorely needed to unravel the role of soil erosion for the carbon (C) budget from local to global scales. The main objective of this study was to determine SOC redistribution and the complete C budget of a loess soil affected by water erosion. We measured fluxes of SOC, dissolved organic C (DOC) and CO2 in a pseudo-replicated rainfall-simulation experiment. We characterized different C fractions in soils and redistributed sediments using density fractionation and determined C enrichment ratios (CER) in the transported sediments. Erosion, transport and subsequent deposition resulted in significantly higher CER of the sediments exported ranging between 1.3 and 4.0. In the exported sediments, C contents (mg per g soil) of particulate organic C (POC, C not bound to soil minerals) and mineral-associated organic C (MOC) were both significantly higher than those of non-eroded soils indicating that water erosion resulted in losses of C-enriched material both in forms of POC and MOC. The averaged SOC fluxes as particles (4.7 g C m(-2) yr(-1)) were 18 times larger than DOC fluxes. Cumulative emission of soil CO2 slightly decreased at the erosion zone while increased by 56% and 27% at the transport and depositional zone, respectively, in comparison to non-eroded soil. Overall, CO2 emission is the predominant form of C loss contributing to about 90.5% of total erosion-induced C losses in our 4-month experiment, which were equal to 18 g C m(-2). Nevertheless, only 1.5% of the total redistributed C was mineralized to CO2 indicating a large stabilization after deposition. Our study also underlines the importance of C losses by particles and as DOC for understanding the effects of water erosion on the C balance at the interface of terrestrial and aquatic ecosystems.

  13. 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.

  14. 2,4,6-Trinitrotoluene mineralization and bacterial production rates of natural microbial assemblages from coastal sediments

    Energy Technology Data Exchange (ETDEWEB)

    Montgomery, Michael T., E-mail: michael.montgomery@nrl.navy.mil [Naval Research Laboratory, Marine Biogeochemistry Section, Code 6114, 4555 Overlook Avenue, Washington, DC 20375 (United States); Coffin, Richard B., E-mail: richard.coffin@nrl.navy.mil [Naval Research Laboratory, Marine Biogeochemistry Section, Code 6114, 4555 Overlook Avenue, Washington, DC 20375 (United States); Boyd, Thomas J., E-mail: thomas.boyd@nrl.navy.mil [Naval Research Laboratory, Marine Biogeochemistry Section, Code 6114, 4555 Overlook Avenue, Washington, DC 20375 (United States); Smith, Joseph P., E-mail: joseph.smith@nrl.navy.mil [Naval Research Laboratory, Marine Biogeochemistry Section, Code 6114, 4555 Overlook Avenue, Washington, DC 20375 (United States); Walker, Shelby E., E-mail: Shelby.Walker@noaa.gov [Naval Research Laboratory, Marine Biogeochemistry Section, Code 6114, 4555 Overlook Avenue, Washington, DC 20375 (United States); Osburn, Christopher L., E-mail: chris_osburn@ncsu.edu [Marine, Earth and Atmospheric Sciences, North Carolina State University, Raleigh, NC 27695 (United States)

    2011-12-15

    The nitrogenous energetic constituent, 2,4,6-Trinitrotoluene (TNT), is widely reported to be resistant to bacterial mineralization (conversion to CO{sub 2}); however, these studies primarily involve bacterial isolates from freshwater where bacterial production is typically limited by phosphorus. This study involved six surveys of coastal waters adjacent to three biome types: temperate broadleaf, northern coniferous, and tropical. Capacity to catabolize and mineralize TNT ring carbon to CO{sub 2} was a common feature of natural sediment assemblages from these coastal environments (ranging to 270+/-38 {mu}g C kg{sup -1} d{sup -1}). More importantly, these mineralization rates comprised a significant proportion of total heterotrophic production. The finding that most natural assemblages surveyed from these ecosystems can mineralize TNT ring carbon to CO{sub 2} is consistent with recent reports that assemblage components can incorporate TNT ring carbon into bacterial biomass. These data counter the widely held contention that TNT is recalcitrant to bacterial catabolism of the ring carbon in natural environments. - Highlights: > TNT mineralization is a common feature of natural bacterial assemblages in coastal sediments. > TNT mineralization rates comprised a significant proportion of total heterotrophic production. > These data counter the widely held contention that TNT is recalcitrant to bacterial catabolism of the ring carbon in natural environments. - The capacity to mineralize TNT ring carbon to CO{sub 2} is a common feature of natural bacterial assemblages in coastal sediment.

  15. 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.

  16. DEVELOPMENT OF A CO2 SEQUESTRATION MODULE BY INTEGRATING MINERAL ACTIVATION AND AQUEOUS CARBONATION. ANNUAL TECHNICAL PROGRESS REPORT

    International Nuclear Information System (INIS)

    George Alexander; M. Mercedes Maroto-Valer; Parvana Aksoy; Harold Schobert

    2006-01-01

    Mineral carbonation provides a potential option for the long-term storage of carbon dioxide. Serpentine has been chosen as the feedstock mineral, due to its abundance and availability. However, the relatively low reactivity of serpentine has warranted research into physical and chemical treatments that have been shown to greatly increase its reactivity. The use of sulfuric acid as an accelerating medium for the removal of magnesium from serpentine has recently been investigated. In addition to the challenges presented by the dissolution of serpentine, another challenge is the subsequent carbonation of the magnesium ions. A stable hydration sphere for the magnesium ion reduces the carbonation kinetics by obstructing the formation of the carbonation products. Accordingly, this research has evaluated the solubility of carbon dioxide in aqueous solution, the interaction between the dissociation products of carbon dioxide, and the carbonation potential of the magnesium ion

  17. Geochemical modeling of the influence of silicate mineral alteration on alkalinity production and carbonate precipitation

    Science.gov (United States)

    Herda, Gerhard; Kraemer, Stephan M.; Gier, Susanne; Meister, Patrick

    2016-04-01

    High CO2 partial pressure (pCO2) in deep rock reservoirs causes acidification of the porefluid. Such conditions occur during injection and subsurface storage of CO2 (to prevent the release of greenhouse gas) but also naturally in zones of strong methanogenic microbial activity in organic matter-rich ocean margin sediments. The acidic fluids are corrosive to carbonates and bear the risk of leakage of CO2 gas to the surface. Porefluid acidification may be moderated by processes that increase the alkalinity, i.e. that produce weak acid anions capable of buffering the acidification imposed by the CO2. Often, alkalinity increases as a result of anaerobic microbial activity, such as anaerobic oxidation of methane. However, on a long term the alteration of silicates, in particular, clay minerals, may be a more efficient mechanism of alkalinity production. Under altered temperature, pressure and porefluid composition at depth, clay minerals may change to thermodynamically more stable states, thereby increasing the alkalinity of the porefluid by partial leaching of Mg-(OH)2 and Ca-(OH)2 (e.g. Wallmann et al., 2008; Mavromatis et al., 2014). This alteration may even be enhanced by a high pCO2. Thus, silicate alteration can be essential for a long-term stabilization of volatile CO2 in the form of bicarbonate or may even induce precipitation of carbonate minerals, but these processes are not fully understood yet. The goal of this study is to simulate the alkalinity effect of silicate alteration under diagenetic conditions and high pCO2 by geochemical modeling. We are using the program PHREEQC (Parkhurst and Appelo, 2013) to generate high rock/fluid ratio characteristics for deep subsurface rock reservoirs. Since we are interested in the long-term evolution of diagenetic processes, over millions of years, we do not consider kinetics but calculate the theoretically possible equilibrium conditions. In a first step we are calculating the saturation state of different clay minerals

  18. 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.

  19. CO2 Energy Reactor - Integrated Mineral Carbonation: Perspectives on Lab-Scale Investigation and Products Valorization

    OpenAIRE

    Rafael M Santos; Pol CM Knops; Keesjan L Rijnsburger; Yi Wai eChiang

    2016-01-01

    To overcome the challenges of mineral CO2 sequestration, Innovation Concepts B.V. is developing a unique proprietary gravity pressure vessel (GPV) reactor technology and has focussed on generating reaction products of high economic value. The GPV provides intense process conditions through hydrostatic pressurization and heat exchange integration that harvests exothermic reaction energy, thereby reducing energy demand of conventional reactor designs, in addition to offering other benefits. In ...

  20. Precipitation kinetics of Mg-carbonates, influence of organic ligands and consequences for CO2 mineral sequestration

    International Nuclear Information System (INIS)

    Gautier, Q.

    2012-01-01

    Forming magnesium carbonate minerals through carbonation of magnesium silicates has been proposed as a safe and durable way to store carbon dioxide, with a possibly high potential to offset anthropogenic CO 2 emissions. To date however, chemical reactions involved in this process are facing strong kinetic limitations, which originate in the low reactivity of both Mg-silicates and Mg-carbonates. Numerous studies have focused on the dissolution of Mg-silicates, under the questionable hypothesis that this step limits the whole process. This thesis work focuses instead on the mechanisms and rates of formation of magnesium carbonates, which are the final products of carbonation reactions. The first part of the work is dedicated to studying the influence on magnesite precipitation kinetics of three organic ligands known to accelerate Mg-silicates dissolution rates: oxalate, citrate and EDTA. With help of mixed-flow reactor experiments performed between 100 and 150 C, we show that these ligands significantly reduce magnesite growth rates, through two combined mechanisms: (1) complexation of Mg 2+ cations in aqueous solution, which was rigorously estimated from a thermodynamic database established through a critical review of the literature, and (2) adsorption of ligands to a limited number of surface sites, leading to a decrease of the precipitation rate constant. The observed growth inhibition is maximal with citrate. We then used hydrothermal atomic force microscopy to probe the origin of the documented growth inhibition. Our observations show that citrate and oxalate interact with the crystal growth process on magnesite surface, modifying the shape of growth hillocks as well as the step generation frequency through spiral growth. We also show that the ligands adsorb preferentially on different kink-sites, which is probably related to their different structures and chemical properties. We propose that the stronger magnesite growth inhibition caused by citrate is related

  1. Limited carbon storage in soil and litter of experimental forest plots under increased atmospheric CO2

    International Nuclear Information System (INIS)

    Schlesinger, W.H.; Lichter, J.

    2001-01-01

    The current rise in atmospheric CO 2 concentration is thought to be mitigated in part by carbon sequestration within forest ecosystems, where carbon can be stored in vegetation or soils. The storage of carbon in soils is determined by the fraction that is sequestered in persistent organic materials, such as humus. In experimental forest plots of loblolly pine (Pinus taeda) exposed to high CO 2 concentrations, nearly half of the carbon uptake is allocated to short-lived tissues, largely foliage. These tissues fall to the ground and decompose, normally contributing only a small portion of their carbon content to refractory soil humic materials. Such findings call into question the role of soils as long-term carbon sinks, and show the need for a better understanding of carbon cycling in forest soils. Here we report a significant accumulation of carbon in the litter layer of experimental forest plots after three years of growth at increased CO 2 concentrations (565 μ l 1 ). But fast turnover times of organic carbon in the litter layer (of about three years) appear to constrain the potential size of this carbon sink. Given the observation that carbon accumulation in the deeper mineral soil layers was absent, we suggest that significant, long-term net carbon sequestration in forest soils is unlikely. (author)

  2. A review of accelerated carbonation technology in the treatment of cement-based materials and sequestration of CO2

    International Nuclear Information System (INIS)

    Fernandez Bertos, M.; Simons, S.J.R.; Hills, C.D.; Carey, P.J.

    2004-01-01

    Moist calcium silicate minerals are known to readily react with carbon dioxide (CO 2 ). The reaction products can cause rapid hardening and result in the production of monolithic materials. Today, accelerated carbonation is a developing technology, which may have potential for the treatment of wastes and contaminated soils and for the sequestration of CO 2 , an important greenhouse gas. This paper reviews recent developments in this emerging technology and provides information on the parameters that control the process. The effects of the accelerated carbonation reaction on the solid phase are discussed and future potential applications of this technology are also considered

  3. Soil Organic Carbon Redistribution by Water Erosion – The Role of CO2 Emissions for the Carbon Budget

    Science.gov (United States)

    Wang, Xiang; Cammeraat, Erik L. H.; Romeijn, Paul; Kalbitz, Karsten

    2014-01-01

    A better process understanding of how water erosion influences the redistribution of soil organic carbon (SOC) is sorely needed to unravel the role of soil erosion for the carbon (C) budget from local to global scales. The main objective of this study was to determine SOC redistribution and the complete C budget of a loess soil affected by water erosion. We measured fluxes of SOC, dissolved organic C (DOC) and CO2 in a pseudo-replicated rainfall-simulation experiment. We characterized different C fractions in soils and redistributed sediments using density fractionation and determined C enrichment ratios (CER) in the transported sediments. Erosion, transport and subsequent deposition resulted in significantly higher CER of the sediments exported ranging between 1.3 and 4.0. In the exported sediments, C contents (mg per g soil) of particulate organic C (POC, C not bound to soil minerals) and mineral-associated organic C (MOC) were both significantly higher than those of non-eroded soils indicating that water erosion resulted in losses of C-enriched material both in forms of POC and MOC. The averaged SOC fluxes as particles (4.7 g C m−2 yr−1) were 18 times larger than DOC fluxes. Cumulative emission of soil CO2 slightly decreased at the erosion zone while increased by 56% and 27% at the transport and depositional zone, respectively, in comparison to non-eroded soil. Overall, CO2 emission is the predominant form of C loss contributing to about 90.5% of total erosion-induced C losses in our 4-month experiment, which were equal to 18 g C m−2. Nevertheless, only 1.5% of the total redistributed C was mineralized to CO2 indicating a large stabilization after deposition. Our study also underlines the importance of C losses by particles and as DOC for understanding the effects of water erosion on the C balance at the interface of terrestrial and aquatic ecosystems. PMID:24802350

  4. The CarbFix Pilot Project in Iceland - CO2 capture and mineral storage in basaltic rocks

    Science.gov (United States)

    Sigurdardottir, H.; Sigfusson, B.; Aradottir, E. S.; Gunnlaugsson, E.; Gislason, S. R.; Alfredsson, H. A.; Broecker, W. S.; Matter, J. M.; Stute, M.; Oelkers, E.

    2010-12-01

    The overall objective of the CarbFix project is to develop and optimize a practical and cost-effective technology for capturing CO2 and storing it via in situ mineral carbonation in basaltic rocks, as well as to train young scientist to carry the corresponding knowledge into the future. The project consists of a field injection of CO2 charged water at the Hellisheidi geothermal power plant in SW Iceland, laboratory experiments, numerical reactive transport modeling, tracer tests, natural analogue and cost analysis. The CO2 injection site is situated about 3 km south of the Hellisheidi geothermal power plant. Reykjavik Energy operates the power plant, which currently produces 60,000 tons/year CO2 of magmatic origin. The produced geothermal gas mainly consists of CO2 and H2S. The two gases will be separated in a pilot gas treatment plant, and CO2 will be transported in a pipeline to the injection site. There, CO2 will be fully dissolved in 20 - 25°C water during injection at 25 - 30 bar pressure, resulting in a single fluid phase entering the storage formation, which consists of relatively fresh basaltic lavas. The CO2 charged water is reactive and will dissolve divalent cations from the rock, which will combine with the dissolved carbon to form solid thermodynamically stable carbonate minerals. The injection test is designed to inject 2200 tons of CO2 per year. In the past three years the CarbFix project has been addressing background fluid chemistries at the injection site and characterizing the target reservoir for the planned CO2 injection. Numerous groundwater samples have been collected and analysed. A monitoring and accounting plan has been developed, which integrates surface, subsurface and atmospheric monitoring. A weather station is operating at the injection site for continuous monitoring of atmospheric CO2 and to track all key parameters for the injection. Environmental authorities have granted licenses for the CO2 injection and the use of tracers, based

  5. Implications for carbon processing beneath the Greenland Ice Sheet from dissolved CO2 and CH4 concentrations of subglacial discharge

    Science.gov (United States)

    Pain, A.; Martin, J.; Martin, E. E.

    2017-12-01

    Subglacial carbon processes are of increasing interest as warming induces ice melting and increases fluxes of glacial meltwater into proglacial rivers and the coastal ocean. Meltwater may serve as an atmospheric source or sink of carbon dioxide (CO2) or methane (CH4), depending on the magnitudes of subglacial organic carbon (OC) remineralization, which produces CO2 and CH4, and mineral weathering reactions, which consume CO2 but not CH4. We report wide variability in dissolved CO2 and CH4 concentrations at the beginning of the melt season (May-June 2017) between three sites draining land-terminating glaciers of the Greenland Ice Sheet. Two sites, located along the Watson River in western Greenland, drain the Isunnguata and Russell Glaciers and contained 1060 and 400 ppm CO2, respectively. In-situ CO2 flux measurements indicated that the Isunnguata was a source of atmospheric CO2, while the Russell was a sink. Both sites had elevated CH4 concentrations, at 325 and 25 ppm CH4, respectively, suggesting active anaerobic OC remineralization beneath the ice sheet. Dissolved CO2 and CH4 reached atmospheric equilibrium within 2.6 and 8.6 km downstream of Isunnguata and Russell discharge sites, respectively. These changes reflect rapid gas exchange with the atmosphere and/or CO2 consumption via instream mineral weathering. The third site, draining the Kiagtut Sermiat in southern Greenland, had about half atmospheric CO2 concentrations (250 ppm), but approximately atmospheric CH4 concentrations (2.1 ppm). Downstream CO2 flux measurements indicated ingassing of CO2 over the entire 10-km length of the proglacial river. CO2 undersaturation may be due to more readily weathered lithologies underlying the Kiagtut Sermiat compared to Watson River sites, but low CH4 concentrations also suggest limited contributions of CO2 and CH4 from OC remineralization. These results suggest that carbon processing beneath the Greenland Ice Sheet may be more variable than previously recognized

  6. Mineral dissolution and precipitation in carbonate dominated terranes assessed using Mg isotopes

    Science.gov (United States)

    Tipper, E.; Calmels, D.; Gaillardet, J.; Galy, A.

    2013-12-01

    Carbonate weathering by carbonic acid consumes atmospheric CO2 during mineral dissolution, fixing it as aqueous bicarbonate over millennial time-scales. Ocean acidification has increased the solubility of CO2 in seawater by changing the balance of pH to alkalinity (the oceanic reservoir of carbon). This has lengthened the time-scale for CO2 sequestration by carbonate weathering to tens of thousands of years. At a global scale, the net consumption of CO2 is at least equal to that from silicate weathering, but there is far less work on carbonate weathering compared to silicate weathering because it has generally been assumed to be CO2 neutral on geological time-scales. Carbonate rocks are more readily dissolved than silicate rocks, meaning that their dissolution will likely respond much more rapidly to global environmental change when compared with the dissolution of silicate minerals. Although far less concentrated than Ca in many carbonates, Mg substitutes for Ca and is more concentrated than any other metal ion. Tracing the behavior of Mg in river waters, using Mg stable isotopes (26Mg/24Mg ratio expressed as delta26Mg in per mil units) is therefore a novel way to understand the complex series of dissolution/precipitation reactions that govern solute concentrations of Ca and Mg, and hence CO2 transfer by carbonate weathering. We present new Mg isotope data on a series of river and spring waters from the Jura mountains in North-East France. The stratigraphic column is relatively uniform throughout the Jura mountains and is dominated by limestones. As the limestone of the Jura Mountains were deposited in high-energy shallow water environments (shore line, lagoon and coral reefs), they are usually clay and organic poor. The delta26Mg of the local rocks is very constant at circa -4permil. The delta26Mg of the river waters is also fairly constant, but offset from the rock at -2.5permil. This is an intriguing observation because the dissolution of limestones is expected

  7. Carbon and nitrogen mineralization in vineyard acid soils amended with a bentonitic winery waste

    Science.gov (United States)

    Fernández-Calviño, David; Rodríguez-Salgado, Isabel; Pérez-Rodríguez, Paula; Díaz-Raviña, Montserrat; Nóvoa-Muñoz, Juan Carlos; Arias-Estévez, Manuel

    2015-04-01

    Carbon mineralization and nitrogen ammonification processes were determined in different vineyard soils. The measurements were performed in samples non-amended and amended with different bentonitic winery waste concentrations. Carbon mineralization was measured as CO2 released by the soil under laboratory conditions, whereas NH4+ was determined after its extraction with KCl 2M. The time evolution of both, carbon mineralization and nitrogen ammonification, was followed during 42 days. The released CO2 was low in the analyzed vineyard soils, and hence the metabolic activity in these soils was low. The addition of the bentonitic winery waste to the studied soils increased highly the carbon mineralization (2-5 fold), showing that the organic matter added together the bentonitic waste to the soil have low stability. In both cases, amended and non-amended samples, the maximum carbon mineralization was measured during the first days (2-4 days), decreasing as the incubation time increased. The NH4+ results showed an important effect of bentonitic winery waste on the ammonification behavior in the studied soils. In the non-amended samples the ammonification was no detected in none of the soils, whereas in the amended soils important NH4+ concentrations were detected. In these cases, the ammonification was fast, reaching the maximum values of NH4 between 7 and 14 days after the bentonitic waste additions. Also, the percentages of ammonification respect to the total nitrogen in the soil were high, showing that the nitrogen provided by the bentonitic waste to the soil is non-stable. The fast carbon mineralization found in the soils amended with bentonitic winery wastes shows low possibilities of the use of this waste for the increasing the organic carbon pools in the soil.On the other hand, the use of this waste as N-fertilizer can be possible. However, due its fast ammonification, the waste should be added to the soils during active plant growth periods.

  8. The influence of included minerals on the intrinsic reactivity of chars prepared under N{sub 2} and CO{sub 2} environment

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Hong; Li, Huan; Chen, Jiabao; Zhao, Bo; Hu, Guangzhou [China Univ. of Mining and Technology, Jiangsu (China). School of Chemical Engineering

    2013-07-01

    Oxy-fuel technology could be successfully used to retrofit existing coal-fired power plants or alternatively be used to design and build new coal-fired power plants with almost zero emissions. Char reactivity under oxy-fuel conditions will have a significant impact on the coal burnout. In this paper, two fractions, representing organic-rich particles and organic particles with included minerals, were separated from each of three Chinese coals of different rank. They were then devolatilized at 1,450 C in a drop tube furnace (DTF) under N{sub 2} and CO{sub 2} environment, respectively. The chars were subjected to nitrogen adsorption study, thermogravimetric analysis and XRD analysis. It was found that char reactivity of all three pairs of chars were increased under CO{sub 2} environment as compared with that under N{sub 2} environment, but with differing trend. For the organic-rich samples the reactivity difference is increased with decreasing rank. On the contrary, for the samples of organic particles with included minerals, the reactivity difference is decreased with decreasing rank. Mechanism analysis showed that they are resulted not from gasification, but from a combination of changes in surface area and in the orderness of carbon structure in the chars, both of which, in turn, are resulted from the higher heat capacity of CO{sub 2} and the interaction between metastable liquid phase and the included minerals.

  9. Enzymatic, urease-mediated mineralization of gellan gum hydrogel with calcium carbonate, magnesium-enriched calcium carbonate and magnesium carbonate for bone regeneration applications

    DEFF Research Database (Denmark)

    Douglas, Timothy E L; Łapa, Agata; Samal, Sangram Keshari

    2017-01-01

    enzymatically with CaCO3 , Mg-enriched CaCO3 and magnesium carbonate to generate composite biomaterials for bone regeneration. Hydrogels loaded with the enzyme urease were mineralized by incubation in mineralization media containing urea and different ratios of calcium and magnesium ions. Increasing...

  10. 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.

  11. 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.

  12. Benthic Carbon Mineralization and Nutrient Turnover in a Scottish Sea Loch

    DEFF Research Database (Denmark)

    Glud, Ronnie N.; Berg, Peter; Stahl, Henrik

    2016-01-01

    Based on in situ microprofiles, chamber incubations and eddy covariance measurements, we investigated the benthic carbon mineralization and nutrient regeneration in a ~65-m-deep sedimentation basin of Loch Etive, UK. The sediment hosted a considerable amount of infauna that was dominated by the b......Based on in situ microprofiles, chamber incubations and eddy covariance measurements, we investigated the benthic carbon mineralization and nutrient regeneration in a ~65-m-deep sedimentation basin of Loch Etive, UK. The sediment hosted a considerable amount of infauna that was dominated....... The average benthic O2 exchange as derived by chamber incubations and the eddy covariance approach were similar (14.9 ± 2.5 and 13.1 ± 9.0 mmol m−2 day−1) providing confidence in the two measuring approaches. Moreover, the non-invasive eddy approach revealed a flow-dependent benthic O2 flux that was partly...... ascribed to enhanced ventilation of infauna burrows during periods of elevated flow rates. The ratio in exchange rates of ΣCO2 and O2 was close to unity, confirming that the O2 uptake was a good proxy for the benthic carbon mineralization in this setting. The infauna activity resulted in highly dynamic...

  13. The effect of alkaline cations on the Intercalation of Carbon Dioxide in Sepiolite Minerals: a Molecular Dynamics Investigation.

    Science.gov (United States)

    Tavanti, Francesco; Muniz-Miranda, Francesco; Pedone, Alfonso

    2018-03-01

    The ability of the sepiolite mineral to intercalate CO2 molecules inside its channels in the presence of different alkaline cations (K+, Na+ and Li+) has been studied by classical Molecular Dynamics simulations. Starting from an alkaline-free sepiolite crystalline model we built three models with stoichiometry Mg320Si440Al40O1200(OH)160X+40•480H2O. On these models, we gradually replaced the water molecules present in the channels with carbon dioxide and determined the energy of this exchange reaction as well as the structural organization and dynamics of carbon dioxide in the channels. The adsorption energy shows that the Li-containing sepiolite mineral retains more carbon dioxide with respect to those with sodium and potassium cations in the channels. Moreover, the ordered patterns of CO2 molecules observed in the alkaline-free sepiolite mineral are in part destabilized by the presence of cations decreasing the adsorption capacity of this clay mineral.

  14. SkyMine Carbon Mineralization Pilot Project

    Energy Technology Data Exchange (ETDEWEB)

    Joe Jones; Clive Barton; Mark Clayton; Al Yablonsky; David Legere

    2010-09-30

    This Topical Report addresses accomplishments achieved during Phase 1 of the SkyMine{reg_sign} Carbon Mineralization Pilot Project. The primary objectives of this project are to design, construct, and operate a system to capture CO{sub 2} from a slipstream of flue gas from a commercial coal-fired cement kiln, convert that CO{sub 2} to products having commercial value (i.e., beneficial use), show the economic viability of the CO{sub 2} capture and conversion process, and thereby advance the technology to a point of readiness for commercial scale demonstration and proliferation. The project will also substantiate market opportunities for the technology by sales of chemicals into existing markets, and identify opportunities to improve technology performance and reduce costs at commercial scale. The primary objectives of Phase 1 of the project were to elaborate proven SkyMine{reg_sign} process chemistry to commercial pilot-scale operation and complete the preliminary design ('Reference Plant Design') for the pilot plant to be built and operated in Phase 2. Additionally, during Phase 1, information necessary to inform a DOE determination regarding NEPA requirements for the project was developed, and a comprehensive carbon lifecycle analysis was completed. These items were included in the formal application for funding under Phase 2. All Phase 1 objectives were successfully met on schedule and within budget.

  15. Capture, transport and storage of CO2

    International Nuclear Information System (INIS)

    De Boer, B.

    2008-01-01

    The emission of greenhouse gas CO2 in industrial processes and electricity production can be reduced on a large scale. Available techniques include post-combustion, pre-combustion, the oxy-fuel process, CO2 fixation in industrial processes and CO2 mineralization. In the Netherlands, plans for CO2 capture are not developing rapidly (CCS - carbon capture and storage). [mk] [nl

  16. Radiocarbon as a Reactive Tracer for Tracking Permanent CO2 Storage in Basaltic Rocks

    Energy Technology Data Exchange (ETDEWEB)

    Matter, Juerg [Columbia Univ., New York, NY (United States); Stute, Martin [Columbia Univ., New York, NY (United States); Schlosser, Peter [Columbia Univ., New York, NY (United States); Broecker, Wallace [Columbia Univ., New York, NY (United States)

    2015-09-30

    In view of concerns about the long-term integrity and containment of CO2 storage in geologic reservoirs, many efforts have been made to improve the monitoring, verification and accounting methods for geologically stored CO2. Our project aimed to demonstrate that carbon-14 (14C) could be used as a reactive tracer to monitor geochemical reactions and evaluate the extent of mineral trapping of CO2 in basaltic rocks. The capacity of a storage reservoir for mineral trapping of CO2 is largely a function of host rock composition. Mineral carbonation involves combining CO2 with divalent cations including Ca2+, Mg2+ and Fe2+. The most abundant geological sources for these cations are basaltic rocks. Based on initial storage capacity estimates, we know that basalts have the necessary capacity to store million to billion tons of CO2 via in situ mineral carbonation. However, little is known about CO2-fluid-rock reactions occurring in a basaltic storage reservoir during and post-CO2 injection. None of the common monitoring and verification techniques have been able to provide a surveying tool for mineral trapping. The most direct method for quantitative monitoring and accounting involves the tagging of the injected CO2 with 14C because 14C is not present in deep geologic reservoirs prior to injection. Accordingly, we conducted two CO2 injection tests at the CarbFix pilot injection site in Iceland to study the feasibility of 14C as a reactive tracer for monitoring CO2-fluid-rock reactions and CO2 mineralization. Our newly developed monitoring techniques, using 14C as a reactive tracer, have been successfully demonstrated. For the first time, permanent and safe disposal of CO2 as environmentally benign carbonate minerals in basaltic rocks could be shown. Over 95% of the injected CO2 at the Carb

  17. Mineral Carbonation of Phosphogypsum Waste for Production of Useful Carbonate and Sulfate Salts

    Energy Technology Data Exchange (ETDEWEB)

    Mattila, Hannu-Petteri, E-mail: hmattila@abo.fi; Zevenhoven, Ron [Thermal and Flow Engineering Laboratory, Åbo Akademi University, Turku (Finland)

    2015-11-16

    Phosphogypsum (CaSO{sub 4}·2H{sub 2}O, PG) waste is produced in large amounts during phosphoric acid (H{sub 3}PO{sub 4}) production. Minor quantities are utilized in construction or agriculture, while most of the material is stockpiled, creating an environmental challenge to prevent pollution of natural waters. In principle, the gypsum waste could be used to capture several hundred megatonnes of carbon dioxide (CO{sub 2}). For example, when gypsum is converted to ammonium sulfate [(NH{sub 4}){sub 2}SO{sub 4}] with ammonia (NH{sub 3}) and CO{sub 2}, also solid calcium carbonate (CaCO{sub 3}) is generated. The ammonium sulfate can be utilized as a fertilizer or in other mineral carbonation processes that use magnesium silicate-based rock as feedstock, while calcium carbonate has various uses as, e.g., filler material. The reaction extent of the described process was studied by thermodynamic modeling and experimentally as a function of reactant concentrations and temperature. Other essential properties such as purity and quality of the solid products are also followed. Conversion efficiencies of >95% calcium from PG to calcium carbonate are obtained. Scalenohedral, rhombohedral, and prismatic calcite particles can be produced, although the precipitates contain certain contaminants such as rare earth metals and sulfur from the gypsum. A reverse osmosis membrane cartridge is also tested as an alternative and energy-efficient method of concentrating the ammonium sulfate salt solution instead of the traditional evaporation of the process solution.

  18. Metabolism of carbon-14 labelled l-tryptophan, l-kynerenine and hydroxy-l-kynerenine in miners with scleroderma

    International Nuclear Information System (INIS)

    Hankes, L.V.; De Bruin, E.; Jansen, C.R.; Voster, L.; Schmaeler, M.

    1977-01-01

    Six South African white miners were studied with the 2-g l-tryptophan load test and tracer doses of L-tryptophan-7a-carbon-14, L-kynurenine-keto-carbon-14 and hydroxy-L-kynerenine-keto-carbon-14. The breath 14 CO 2 and 14 urinary metabolites were measured. When they were compared with a previous study of American women with scleroderma, similar 14 CO 2 and tryptophan metabolite excretion patterns were observed in the data from the miners. The labelled quinolinic acid excretion was more significantly elevated in the South African miners' urine than in the urine of the American women. The data from both studies suggest that some patients with scleroderma have an altered step in the tryptophan metabolic pathway after hydroxy-anthranilic acid. What relationship exists between the induction of pulmonary silicosis and the subsequent development of scleroderma, requires additional human studies

  19. 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.

  20. Carbon K-edge spectra of carbonate minerals.

    Science.gov (United States)

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

    2010-09-01

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

  1. Carbon K-edge Spectra of Carbonate Minerals

    Energy Technology Data Exchange (ETDEWEB)

    Brandes, J.; Wirick, S; Jacobsen, C

    2010-01-01

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

  2. 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)

  3. 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

    nighttime respiration was actually smaller than the increase in daytime photosynthesis according simulations using BEPS-VDS. This is because the same amount of change in ppmv at 40 m required a larger change in the surface flux in CBL than in SBL, i.e. CBL was able to dilute the surface effects in a higher air column than was SBL. As a consequence, we found that the boreal landscape in the vicinity of the tower up to 100 km, consisting of mostly black spruce forests with small fractions of aspen and wetland, acted as a carbon sink in the 1990-2000 period. The absolute magnitude of the sink requires modeling for 50-100 years, but we infer from the short CO2 record that the sink magnitude increased by 0.44 gC/(m2.y) on average, i.e., the accumulated effect over the 11 years was 4.8 gC/m2. Our model simulations indicate that improved nutrient mineralization in soil at higher temperatures was the main cause for enhanced photosynthesis. Although uncertainties exist in these estimates, the results suggest the usefulness of air CO2 records at high frequencies (at least hourly) for long periods.

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

    KAUST Repository

    Zhu, Xiuping; Logan, Bruce E.

    2014-01-01

    Mineral carbonation can be used for CO2 sequestration, but the reaction rate is slow. In order to accelerate mineral carbonation, acid generated in a microbial electrolysis desalination and chemical-production cell (MEDCC) was examined to dissolve

  5. Mineral carbonation of phosphogypsum waste for production of useful carbonate and sulfate salts

    Directory of Open Access Journals (Sweden)

    Hannu-Petteri eMattila

    2015-11-01

    Full Text Available Phosphogypsum (CaSO4·2H2O waste is produced in large amounts during phosphoric acid (H3PO4 production. Minor quantities are utilized in construction or agriculture, while most of the material is stockpiled, creating an environmental challenge to prevent pollution of natural waters. In principle, the gypsum waste could be used to capture several hundred Mt of carbon dioxide (CO2. For example, when gypsum is converted to ammonium sulfate ((NH42SO4 with ammonia (NH3 and CO2, also solid calcium carbonate (CaCO3 is generated. The ammonium sulfate can be utilized as a fertilizer or in other mineral carbonation processes that use magnesium silicate-based rock as feedstock, while calcium carbonate has various uses as e.g. filler material. The reaction extent of the described process was studied by thermodynamic modeling and experimentally as a function of reactant concentrations and temperature. Other essential properties such as purity and quality of the solid products are also followed. Conversion efficiencies of >95% calcium from phosphogypsum to calcium carbonate are obtained. Scalenohedral, rhombohedral and prismatic calcite particles can be produced, though the precipitates contain certain contaminants such as rare earth metals and sulfur from the gypsum. A reverse osmosis membrane cartridge is also tested as an alternative and energy-efficient method of concentrating the ammonium sulfate salt solution instead of the traditional evaporation of the process solution.

  6. Crystal structure of cobalt hydroxide carbonate Co2CO3(OH)2: density functional theory and X-ray diffraction investigation.

    Science.gov (United States)

    González-López, Jorge; Cockcroft, Jeremy K; Fernández-González, Ángeles; Jimenez, Amalia; Grau-Crespo, Ricardo

    2017-10-01

    The cobalt carbonate hydroxide Co 2 CO 3 (OH) 2 is a technologically important solid which is used as a precursor for the synthesis of cobalt oxides in a wide range of applications. It also has relevance as a potential immobilizer of the toxic element cobalt in the natural environment, but its detailed crystal structure is so far unknown. The structure of Co 2 CO 3 (OH) 2 has now been investigated using density functional theory (DFT) simulations and powder X-ray diffraction (PXRD) measurements on samples synthesized via deposition from aqueous solution. Two possible monoclinic phases are considered, with closely related but symmetrically different crystal structures, based on those of the minerals malachite [Cu 2 CO 3 (OH) 2 ] and rosasite [Cu 1.5 Zn 0.5 CO 3 (OH) 2 ], as well as an orthorhombic phase that can be seen as a common parent structure for the two monoclinic phases, and a triclinic phase with the structure of the mineral kolwezite [Cu 1.34 Co 0.66 CO 3 (OH) 2 ]. The DFT simulations predict that the rosasite-like and malachite-like phases are two different local minima of the potential energy landscape for Co 2 CO 3 (OH) 2 and are practically degenerate in energy, while the orthorhombic and triclinic structures are unstable and experience barrierless transformations to the malachite phase upon relaxation. The best fit to the PXRD data is obtained using a rosasite model [monoclinic with space group P112 1 /n and cell parameters a = 3.1408 (4) Å, b = 12.2914 (17) Å, c = 9.3311 (16) Å and γ = 82.299 (16)°]. However, some features of the PXRD pattern are still not well accounted for by this refinement and the residual parameters are relatively poor. The relationship between the rosasite and malachite phases of Co 2 CO 3 (OH) 2 is discussed and it is shown that they can be seen as polytypes. Based on the similar calculated stabilities of these two polytypes, it is speculated that some level of stacking disorder could account for the poor

  7. Carbon dioxide sequestration induced mineral precipitation healing of fractured reservoir seals

    Science.gov (United States)

    Welch, N.; Crawshaw, J.

    2017-12-01

    Initial experiments and the thermodynaic basis for carbon dioxide sequestration induced mineral precipitation healing of fractures through reservoir seals will be presented. The basis of this work is the potential exists for the dissolution of reservoir host rock formation carbonate minerals in the acidified injection front of CO2 during sequestration or EOR. This enriched brine and the bulk CO2 phase will then flow through the reservoir until contact with the reservoir seal. At this point any fractures present in the reservoir seal will be the preferential flow path for the bulk CO2 phase as well as the acidified brine front. These fractures would currently be filled with non-acidified brine saturated in seal formation brine. When the acidifeid brine from the host formation and the cap rock brine mix there is the potential for minerals to fall out of solution, and for these precipitated minerals to decrease or entirely cut off the fluid flow through the fractures present in a reservoir seal. Initial equilibrium simulations performed using the PHREEQC1 database drived from the PHREEQE2 database are used to show the favorable conditions under which this mineral precipitation can occurs. Bench scale fluid mixing experiments were then performed to determine the kinetics of the mineral precipitation process, and determine the progress of future experiemnts involving fluid flow within fractured anhydrite reservoir seal samples. 1Parkhurst, D.L., and Appelo, C.A.J., 2013, Description of input and examples for PHREEQC version 3—A computer program for speciation, batch-reaction, one-dimensional transport, and inverse geochemical calculations: U.S. Geological Survey Techniques and Methods, book 6, chap. A43, 497 p., available only at https://pubs.usgs.gov/tm/06/a43/. 2Parkhurst, David L., Donald C. Thorstenson, and L. Niel Plummer. PHREEQE: a computer program for geochemical calculations. No. 80-96. US Geological Survey, Water Resources Division,, 1980.

  8. 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.

  9. Electrochemical reduction of CO2 to CO over Zn in propylene carbonate/tetrabutylammonium perchlorate

    Science.gov (United States)

    Shen, Feng-xia; Shi, Jin; Chen, Tian-you; Shi, Feng; Li, Qing-yuan; Zhen, Jian-zheng; Li, Yun-fei; Dai, Yong-nian; Yang, Bin; Qu, Tao

    2018-02-01

    Developing low cost and high efficient electrode for carbon dioxide (CO2) reduction in organic media is essential for practical application. Zn is a cheap metal and has high catalytic effects on CO2 reduction to carbon monoxide (CO) in aqueous solution. However, little attention has been given to investigate the performance of Zn in organic media for CO2 reduction. In present work, we have conducted CO2 reduction in propylene carbonate/tetrabutylammonium perchlorate on Zn due to that propylene carbonate is a widely used industrial absorber, and tetrabutylammonium perchlorate is a commonly used organic supporting electrolyte. In addition, because electrochemical reduction of CO2 to CO naturally produces H2O, we have discussed water effects on CO2 reduction in propylene carbonate/tetrabutylammonium perchlorate+6.8 wt % H2O. Our experiment results reveal that the faradaic efficiency for CO formation reaches to 83%, and the current density remains stable at 6.72 mA/cm2 at voltage -2.3 V for 4 h. Interestingly, Zn presents higher catalytic activity than Ag, and slightly lower than Au. X-ray photoelectron spectroscopy results confirm that no poisonous species is formed and absorbed on the cathode, which is an important advantage in practical application.

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

    Science.gov (United States)

    Scislewski, A.; Zuddas, P.

    2010-12-01

    with CO2-rich fluids, decreasing the effective reactive surface area. Predictive models of CO2 sequestration under geological conditions should take into account the inhibiting role of surface coating formation. The CO2 rich fluid-rock interactions may also have significant consequences on metal mobilization. Our results indicated that the formation of stable carbonate complexes enhances the solubility of uranium minerals of both albitite and granite, facilitating the U(IV) oxidation, and limiting the extent of uranium adsorption onto particles in oxidized waters. This clearly produces an increase of the uranium mobility with significant consequences for the environment.

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

    Science.gov (United States)

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

    2017-12-01

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

  12. CO_2 valorization - Part. 2: chemical transformation ways

    International Nuclear Information System (INIS)

    Dumergues, Laurent

    2016-01-01

    Carbon dioxide (CO_2) can be used in many ways as a raw material or chemical reagent. The chemical conversion of CO_2 used as a feedstock is achievable by different techniques: mineralization, organic synthesis, hydrogenation, dry reforming, electrolysis, thermolysis, etc. The products obtained have applications as energy products, chemicals, building materials, etc. Choosing an appropriate CO_2 reuse technology will depend on technical and economic requirements (such as the CO_2 purity needed, technological maturity, cost-effectiveness, etc.) and also environmental and social criteria

  13. Microorganisms implication in the CO2 geologic storage processes

    International Nuclear Information System (INIS)

    Dupraz, S.

    2008-01-01

    A first result of this thesis is the building and validation of a circulation reactor named BCC (Bio-mineralization Control Cell). The reactor has the functionality of a biological reactor and allows a monitoring of physico-chemical characteristics such as Eh, pH, electrical conductivity, spectro-photochemical parameters. It also has a capability of percolation through rock cores. It is a first step toward an analogical modeling of interactions between injected CO 2 and deep bio-spheric components. Moreover, a new spectro-photochemical method for monitoring reduced sulfur species has been developed which allows efficient monitoring of sulfate-reducing metabolisms. In the thesis, we have tested four metabolisms relevant to bio-mineralisation or biological assimilation of CO 2 : a reference ureolytic aerobic strain, Bacillus pasteurii, a sulfate-reducing bacterium, Desulfovibrio longus, a sulfate-reducing consortium (DVcons) and an homoacetogenic bacterium, Acetobacterium carbinolicum. In the case of Bacillus pasteurii, which is considered as a model for non photosynthetic prokaryotic carbonate bio-mineralization, we have demonstrated that the biological basification and carbonate bio-mineralization processes can be modelled accurately both analogically and numerically under conditions relevant to deep CO 2 storage, using a synthetic saline groundwater. We have shown that salinity has a positive effect on CO 2 mineral trapping by this bacterium; we have measured the limits of the system in terms of CO 2 pressure and we have shown that the carbonates that nucleate on intracellular calcium phosphates have specific carbon isotope signatures. The studied deep-subsurface strains (Desulfovibrio longus and Acetobacterium carbinolicum) as well as the sulfate-reducing consortium also have capabilities of converting CO 2 into solid carbonates, much less efficient though than in the case of Bacillus pasteurii. However, once inoculated in synthetic saline groundwater and

  14. Carbon isotope composition of CO2-rich inclusions in cumulate-forming mantle minerals from Stromboli volcano (Italy)

    Science.gov (United States)

    Gennaro, Mimma Emanuela; Grassa, Fausto; Martelli, Mauro; Renzulli, Alberto; Rizzo, Andrea Luca

    2017-10-01

    We report on measurements of concentration and carbon isotope composition (δ13CCO2) of CO2 trapped in fluid inclusions of olivine and clinopyroxene crystals separated from San Bartolo ultramafic cumulate Xenoliths (SBX) formed at mantle depth (i.e., beneath a shallow Moho supposed to be at 14.8 km). These cumulates, erupted about 2 ka ago at Stromboli volcano (Italy), have been already investigated by Martelli et al. (2014) mainly for Sr-Nd isotopes and for their noble gases geochemistry. The concentration of CO2 varies of one order of magnitude from 3.8·10- 8 mol g- 1 to 4.8·10- 7 mol g- 1, with δ13C values between - 2.8‰ and - 1.5‰ vs V-PDB. These values overlap the range of measurements performed in the crater gases emitted at Stromboli (- 2.5‰ residence within the volcano plumbing system. Such δ13C values are higher than those commonly reported for MORB-like upper mantle (- 8 ÷ - 4‰) and likely reflect the source contamination of the local mantle wedge by CO2 coming from the decarbonation of the sediments carried by the subducting Ionian slab with a contribution of organic carbon up to 7%.

  15. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Peters, Catherine A

    2013-02-28

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

  17. Carbonate Mineral Formation on Mars: Clues from Stable Isotope Variation Seen in Cryogenic Laboratory Studies of Carbonate Salts

    Science.gov (United States)

    Socki, Richard; Niles, Paul B.; Sun, Tao; Fu, Qi; Romanek, Christopher S.; Gibson, Everett K.

    2013-01-01

    The geologic history of water on the planet Mars is intimately connected to the formation of carbonate minerals through atmospheric CO2 and its control of the climate history of Mars. Carbonate mineral formation under modern martian atmospheric conditions could be a critical factor in controlling the martian climate in a means similar to the rock weathering cycle on Earth. The combination of evidence for liquid water on the martian surface and cold surface conditions suggest fluid freezing could be very common on the surface of Mars. Cryogenic calcite forms readily when a rise in pH occurs as a result of carbon dioxide degassing quickly from freezing Ca-bicarbonate-rich water solutions. This is a process that has been observed in some terrestrial settings such as arctic permafrost cave deposits, lakebeds of the Dry Valleys of Antarctica, and in aufeis (river icings) from rivers of N.E. Alaska. We report here the results of a series of laboratory experiments that were conducted to simulate potential cryogenic carbonate formation on the planet Mars. These results indicate that carbonates grown under martian conditions (controlled atmospheric pressure and temperature) show enrichments from starting bicarbonate fluids in both carbon and oxygen isotopes beyond equilibrium values with average delta13C(DIC-CARB) values of 20.5%0 which exceed the expected equilibrium fractionation factor of [10(sup 3) ln alpha = 13%0] at 0 degC. Oxygen isotopes showed a smaller enrichment with delta18O(H2O-CARB) values of 35.5%0, slightly exceeding the equilibrium fractionation factor of [10(sup 3) ln alpha = 34%0 ] at 0degC. Large kinetic carbon isotope effects during carbonate precipitation could substantially affect the carbon isotope evolution of CO2 on Mars allowing for more efficient removal of 13C from the Noachian atmosphere enriched by atmospheric loss. This mechanism would be consistent with the observations of large carbon isotope variations in martian materials despite the

  18. 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

  19. Varying response of the concentration and content of soybean seed mineral elements, carbohydrates, organic acids, amino acids, protein, and oil to phosphorus starvation and CO2 enrichment

    Science.gov (United States)

    A detailed investigation of the concentration (g-1 seed weight) and content (g plant-1) of seed mineral elements and metabolic profile under phosphorus (P) starvation at ambient (aCO2) and elevated carbon dioxide (eCO2) in soybean is limited. Soybean plants were grown in a controlled environment at ...

  20. 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 ...

  1. Interface Induced Carbonate Mineralization: A Fundamental Geochemical Process Relevant to Carbon Sequestration

    Energy Technology Data Exchange (ETDEWEB)

    Teng, H. Henry [PI, The George Washington University; Xu, Huifang [Co-PI, University of Wisconsin-Madison

    2013-07-17

    We have approached the long-standing geochemical question why anhydrous high-Mg carbonate minerals (i.e., magnesite and dolomite) cannot be formed at ambient conditions from a new perspective by exploring the formation of MgCO{sub 3} and Mg{sub x}Ca{sub (1-x)}CO{sub 3} in non-aqueous solutions. Data collected from our experiments in this funding period suggest that a fundamental barrier, other than cation hydration, exists that prevents Mg{sup 2+} and CO{sub 3}{sup 2-} ions from forming long-range ordered structures. We propose that this barrier mainly stems from the lattice limitation on the spatial configuration of CO{sub 3} groups in magnesite crystals. On the other hand, the measured higher distribution coefficients of Mg between magnesian calcites formed in the absence and presence of water give us a first direct proof to support and quantify the cation hydration effect.

  2. [Effects of different types of litters on soil organic carbon mineralization].

    Science.gov (United States)

    Shi, Xue-Jun; Pan, Jian-Jun; Chen, Jin-Ying; Yang, Zhi-Qiang; Zhang, Li-Ming; Sun, Bo; Li, Zhong-Pei

    2009-06-15

    Using litter incubation experiment in laboratory, decomposition discrepancies of four typical litters from Zijin Mountain were analyzed. The results show that organic carbon mineralization rates of soil with litters all involve fast and slow decomposition stages, and the differences are that the former has shorter duration,more daily decomposition quantity while the latter is opposite. Organic carbon mineralization rates of soil with litters rapidly reached maximum in the early days of incubation, and the order is soil with Cynodon dactylon litter (CK + BMD) (23.88 +/- 0.62) mg x d(-1), soil with Pinus massoniana litter (CK+ PML) (17.93 +/- 0.99) mg x d(-1), soil with Quercus acutissima litter (CK+ QAC) (15.39 +/- 0.16) mg x d(-1) and soil with Cyclobalanopsis glauca litter (CK + CGO) (7.26 +/- 0.34) mg x d(-1), and with significant difference between each other (p litter initial chemical elements. The amount of organic carbon mineralized accumulation within three months incubation is (CK + BMD) (338.21 +/- 6.99) mg, (CK + QAC) (323.48 +/- 13.68) mg, (CK + PML) (278.34 +/- 13.91) mg and (CK + CGO) (245.21 +/- 4.58) mg. 198.17-297.18 mg CO2-C are released during litter incubation, which occupies 20.29%-31.70% of the total litter organic carbon amounts. Power curve model can describe the trends of organic carbon mineralization rate and mineralized accumulation amount,which has a good correlation with their change.

  3. Solution chemistry of carbonate minerals and its effects on the flotation of hematite with sodium oleate

    Science.gov (United States)

    Li, Dong; Yin, Wan-zhong; Xue, Ji-wei; Yao, Jin; Fu, Ya-feng; Liu, Qi

    2017-07-01

    The effects of carbonate minerals (dolomite and siderite) on the flotation of hematite using sodium oleate as a collector were investigated through flotation tests, supplemented by dissolution measurements, solution chemistry calculations, zeta-potential measurements, Fourier transform infrared (FTIR) spectroscopic studies, and X-ray photoelectron spectroscopy (XPS) analyses. The results of flotation tests show that the presence of siderite or dolomite reduced the recovery of hematite and that the inhibiting effects of dolomite were stronger. Dissolution measurements, solution chemistry calculations, and flotation tests confirmed that both the cations (Ca2+ and Mg2+) and CO3 2- ions dissolved from dolomite depressed hematite flotation, whereas only the CO3 2- ions dissolved from siderite were responsible for hematite depression. The zeta-potential, FTIR spectroscopic, and XPS analyses indicated that Ca2+, Mg2+, and CO3 2- (HCO3 -) could adsorb onto the hematite surface, thereby hindering the adsorption of sodium oleate, which was the main reason for the inhibiting effects of carbonate minerals on hematite flotation.

  4. 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.

  5. Carbon Mineralization by Aqueous Precipitation for Beneficial Use of CO2 from Flue Gas. Phase I. Final Topical Report

    International Nuclear Information System (INIS)

    Constantz, Brent; Seeker, Randy; Devenney, Martin

    2010-01-01

    Calera's innovative Mineralization via Aqueous Precipitation (MAP) technology for the capture and conversion of CO 2 to useful materials for use in the built environment was further developed and proven in the Phase 1 Department of Energy Grant. The process was scaled to 300 gallon batch reactors and subsequently to Pilot Plant scale for the continuous production of product with the production of reactive calcium carbonate material that was evaluated as a supplementary cementitious material (SCM). The Calera SCM(trademark) was evaluated as a 20% replacement for ordinary portland cement and demonstrated to meet the industry specification ASTM 1157 which is a standard performance specification for hydraulic cement. The performance of the 20% replacement material was comparable to the 100% ordinary portland cement control in terms of compressive strength and workability as measured by a variety of ASTM standard tests. In addition to the performance metrics, detailed characterization of the Calera SCM was performed using advanced analytical techniques to better understand the material interaction with the phases of ordinary portland cement. X-ray synchrotron diffraction studies at the Advanced Photon Source in Argonne National Lab confirmed the presence of an amorphous phase(s) in addition to the crystalline calcium carbonate phases in the reactive carbonate material. The presence of carboaluminate phases as a result of the interaction of the reactive carbonate materials with ordinary portland cement was also confirmed. A Life Cycle Assessment was completed for several cases based on different Calera process configurations and compared against the life cycle of ordinary portland cement. In addition to the materials development efforts, the Calera technology for the production of product using an innovative building materials demonstration plant was developed beyond conceptual engineering to a detailed design with a construction schedule and cost estimate.

  6. 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.

  7. A new nonlinear optical silicate carbonate K2Ca[Si2O5](CO3) with a hybrid structure of kalsilite and soda-like layered fragments

    Science.gov (United States)

    Belokoneva, Elena L.; Stefanovich, Sergey Yu.; Volkov, Anatoly S.; Dimitrova, Olga V.

    2016-10-01

    Single crystals of a new silicate carbonate, K2Ca[Si2O5](CO3), have been synthesized in a multi-components hydrothermal solution with a pH value close to neutral and a high concentration of a carbonate mineralizer. The new compound has an axial structure (s.g. P6322) with unit cell parameters a = 5.04789 (15), c = 17.8668 (6) Å. Pseudosymmetry of the structure corresponds to s.g. P63/mmc which is broken only by one oxygen position. The structure consists of two layered fragments: one of the type of the mineral kalsilite (KAlSiO4) and the other of the high-temperature soda-like α-Na2CO3, Ca substituting for Na. The electro-neutral layer K2[Si2O5] (denoted K) as well as the layer Ca(CO3) (denoted S) may separately correspond to individual structures. In K2Ca[Si2O5](CO3) the S-K layers are connected together via Ca-O interactions between Ca atoms from the carbonate layer and apical O atoms from the silicate one, and also via K-O interlayer interactions. A hypothetical acentric structure, sp.gr. P-62c, is predicted on the basis of the order-disorder theory. It presents another symmetrical option for the arrangement of K-layers relative to S-layers. The K,Ca-silicate-carbonate powder produces a moderate SHG signal that is two times larger that of the α-quartz powder standard and close to other silicates with acentric structures and low electronic polarizability.

  8. Quantitative percutaneous CO2 measurement following CO2 mineral water baths by means of the isotope ratio

    International Nuclear Information System (INIS)

    Mass, I.; Huebner, G.; Birkenfeld, H.; Zelaitis, L.; Ploetner, G.

    1983-01-01

    A method for the quantitative determination of the carbon dioxide penetration through the human skin during a medical carbon dioxide mineral water bath is described. The natural isotope variation of carbon in the carbon dioxide of bath water, blood, and exspiratory gas are used for the calculation of the penetrated carbon dioxide amount. The method permits to optimize the effectiveness of medical carbon dioxide baths. (author)

  9. Soil organic carbon and nitrogen pools drive soil C-CO2 emissions from selected soils in Maritime Antarctica.

    Science.gov (United States)

    Pires, C V; Schaefer, C E R G; Hashigushi, A K; Thomazini, A; Filho, E I F; Mendonça, E S

    2017-10-15

    The ongoing trend of increasing air temperatures will potentially affect soil organic matter (SOM) turnover and soil C-CO 2 emissions in terrestrial ecosystems of Maritime Antarctica. The effects of SOM quality on this process remain little explored. We evaluated (i) the quantity and quality of soil organic matter and (ii) the potential of C release through CO 2 emissions in lab conditions in different soil types from Maritime Antarctica. Soil samples (0-10 and 10-20cm) were collected in Keller Peninsula and the vicinity of Arctowski station, to determine the quantity and quality of organic matter and the potential to emit CO 2 under different temperature scenarios (2, 5, 8 and 11°C) in lab. Soil organic matter mineralization is low, especially in soils with low organic C and N contents. Recalcitrant C form is predominant, especially in the passive pool, which is correlated with humic substances. Ornithogenic soils had greater C and N contents (reaching to 43.15gkg -1 and 5.22gkg -1 for total organic carbon and nitrogen, respectively). C and N were more present in the humic acid fraction. Lowest C mineralization was recorded from shallow soils on basaltic/andesites. C mineralization rates at 2°C were significant lower than at higher temperatures. Ornithogenic soils presented the lowest values of C-CO 2 mineralized by g of C. On the other hand, shallow soils on basaltic/andesites were the most sensitive sites to emit C-CO 2 by g of C. With permafrost degradation, soils on basaltic/andesites and sulfates are expected to release more C-CO 2 than ornithogenic soils. With greater clay contents, more protection was afforded to soil organic matter, with lower microbial activity and mineralization. The trend of soil temperature increases will favor C-CO 2 emissions, especially in the reduced pool of C stored and protected on permafrost, or in occasional Histosols. Copyright © 2016 Elsevier B.V. All rights reserved.

  10. Factors for Microbial Carbon Sources in Organic and Mineral Soils from Eastern United States Deciduous Forests

    Energy Technology Data Exchange (ETDEWEB)

    Stitt, Caroline R. [Mills College, Oakland, CA (United States)

    2013-09-16

    Forest soils represent a large portion of global terrestrial carbon; however, which soil carbon sources are used by soil microbes and respired as carbon dioxide (CO2) is not well known. This study will focus on characterizing microbial carbon sources from organic and mineral soils from four eastern United States deciduous forests using a unique radiocarbon (14C) tracer. Results from the dark incubation of organic and mineral soils are heavily influenced by site characteristics when incubated at optimal microbial activity temperature. Sites with considerable differences in temperature, texture, and location differ in carbon source attribution, indicating that site characteristics play a role in soil respiration.

  11. 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...

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

    Science.gov (United States)

    Garten, Charles T., Jr.

    2009-03-01

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

  13. Stochastic Approach to Determine CO2 Hydrate Induction Time in Clay Mineral Suspensions

    Science.gov (United States)

    Lee, K.; Lee, S.; Lee, W.

    2008-12-01

    A large number of induction time data for carbon dioxide hydrate formation were obtained from a batch reactor consisting of four independent reaction cells. Using resistance temperature detector(RTD)s and a digital microscope, we successfully monitored the whole process of hydrate formation (i.e., nucleation and crystal growth) and detected the induction time. The experiments were carried out in kaolinite and montmorillonite suspensions at temperatures between 274 and 277 K and pressures ranging from 3.0 to 4.0 MPa. Each set of data was analyzed beforehand whether to be treated by stochastic manner or not. Geochemical factors potentially influencing the hydrate induction time under different experimental conditions were investigated by stochastic analyses. We observed that clay mineral type, pressure, and temperature significantly affect the stochastic behavior of the induction times for CO2 hydrate formation in this study. The hydrate formation kinetics along with stochastic analyses can provide basic understanding for CO2 hydrate storage in deep-sea sediment and geologic formation, securing its stability under the environments.

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

    Science.gov (United States)

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

    2016-12-01

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

  15. Mineral nutrition and plant responses to elevated levels of atmospheric CO{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Ahluwalia, A.

    1996-08-01

    The atmospheric concentration of CO{sub 2}, a radiatively-active ({open_quotes}green-house{close_quotes}) gas, is increasing. This increase is considered a post-industrial phenomenon attributable to increasing rates of fossil fuel combustion and changing land use practices, particularly deforestation. Climate changes resulting from such elevated atmospheric CO{sub 2} levels, in addition to the direct effects of increased CO{sub 2}, are expected to modify the productivity of forests and alter species distributions. Elevated levels of CO{sub 2} have been shown, in some cases, to lead to enhanced growth rates in plants, particularly those with C{sub 3} metabolism - indicating that plant growth is CO{sub 2}-limited in these situations. Since the major process underlying growth is CO{sub 2} assimilation via photosynthesis in leaves, plant growth represents a potential for sequestering atmospheric carbon into biomass, but this potential could be hampered by plant carbon sink size. Carbon sinks are utilization sites for assimilated carbon, enabling carbon assimilation to proceed without potential inhibition from the accumulation of assimilate (photosynthate). Plant growth provides new sinks for assimilated carbon which permits greater uptake of atmospheric carbon dioxide. However, sinks are, on the whole, reduced in size by stress events due to the adverse effects of stress on photosynthetic rates and therefore growth. This document reviews some of the literature on plant responses to increasing levels of atmospheric carbon dioxide and to inadequate nutrient supply rates, and with this background, the potential for nutrient-limited plants to respond to increasing carbon dioxide is addressed. Conclusions from the literature review are then tested experimentally by means of a case study exploring carbon-nitrogen interactions in seedlings of loblolly pine.

  16. Seasonal dynamics of permafrost carbon emissions: A passive, quasi-continuous 14CO2 sampler

    Science.gov (United States)

    Pedron, S.; Xu, X.; Walker, J. C.; Welker, J. M.; Klein, E. S.; Euskirchen, E. S.; Czimczik, C. I.

    2017-12-01

    Millennia of carbon (C) fixation by tundra vegetation, coupled with low rates of C mineralization by soil microorganisms and preservation in permafrost, have allowed Arctic soils to accumulate vast quantities of organic C (1672 Pg C total). Today, the Arctic is rapidly warming (0.48oC decade-1) and widespread degradation of permafrost may subject permafrost C to microbial mineralization and fluxes to the atmosphere, accelerating climate change. Loss of permafrost C can be quantified in situ by measuring the radiocarbon (14C) content of soil and ecosystem respiration, because permafrost C is older (depleted in 14C) than current plant products and soil C cycling operates on timescales of years to centuries. Here, we use 14C analysis of CO2 respired from graminoid tundra in Arctic Alaska to 1) apportion how plant and microbial respiration contribute to ecosystem respiration in spring, summer, and fall, and 2) elucidate the C sources of microbial respiration throughout the year. We used a novel, passive sampling system, capable of trapping diffusive CO2 throughout the active layer of tussock sedge tundra (n=4, from mineral soil to air) over periods of 2 days to 3 weeks in June 2017. CO2 was collected into various sizes of canisters, ranging from 0.5-32 L, and analyzed for its 14C content at UC Irvine's KCCAMS laboratory. To evaluate the system's efficiency, and quantify the temporal and spatial variability of ecosystem respiration sources, we co-deployed 3 Vaisala Carbocap [CO2] and temperature probes, and traditional chambers (n=6) and gas wells (n=10) for sampling of ecosystem- and soil-respired 14CO2 over 15 min-24 hours. A comparison of traditional methods with our new sampler indicates that the system accurately sampled the expected [CO2] depth gradient. The CO2 sampling rate was positively correlated to soil [CO2] (R2=0.963), equivalent to 1.4*10-3±1.6*10-3 mg C/L/month/ppm (n=8). Gas well and probe concentrations were of the same order of magnitude on the same

  17. Normalization of stable isotope data for carbonate minerals: implementation of IUPAC guideline

    Science.gov (United States)

    Kim, Sang-Tae; Coplen, Tyler B.; Horita, Juske

    2015-01-01

    Carbonate minerals provide a rich source of geochemical information because their δ13C and δ18O values provide information about surface and subsurface Earth processes. However, a significant problem is that the same δ18O value is not reported for the identical carbonate sample when analyzed in different isotope laboratories in spite of the fact that the International Union of Pure and Applied Chemistry (IUPAC) has provided reporting guidelines for two decades. This issue arises because (1) the δ18O measurements are performed on CO2 evolved by reaction of carbonates with phosphoric acid, (2) the acid-liberated CO2 is isotopically fractionated (enriched in 18O) because it contains only two-thirds of the oxygen from the solid carbonate, (3) this oxygen isotopic fractionation factor is a function of mineralogy, temperature, concentration of the phosphoric acid, and δ18O value of water in the phosphoric acid, (4) researchers may use any one of an assortment of oxygen isotopic fractionation factors that have been published for various minerals at various reaction temperatures, and (5) it sometimes is not clear how one should calculate δ18OVPDB values on a scale normalized such that the δ18O value of SLAP reference water is −55.5 ‰ relative to VSMOW reference water.

  18. Validating predictions of evolving porosity and permeability in carbonate reservoir rocks exposed to CO2-brine

    Science.gov (United States)

    Smith, M. M.; Hao, Y.; Carroll, S.

    2017-12-01

    Improving our ability to better forecast the extent and impact of changes in porosity and permeability due to CO2-brine-carbonate reservoir interactions should lower uncertainty in long-term geologic CO2 storage capacity estimates. We have developed a continuum-scale reactive transport model that simulates spatial and temporal changes to porosity, permeability, mineralogy, and fluid composition within carbonate rocks exposed to CO2 and brine at storage reservoir conditions. The model relies on two primary parameters to simulate brine-CO2-carbonate mineral reaction: kinetic rate constant(s), kmineral, for carbonate dissolution; and an exponential parameter, n, relating porosity change to resulting permeability. Experimental data collected from fifteen core-flooding experiments conducted on samples from the Weyburn (Saskatchewan, Canada) and Arbuckle (Kansas, USA) carbonate reservoirs were used to calibrate the reactive-transport model and constrain the useful range of k and n values. Here we present the results of our current efforts to validate this model and the use of these parameter values, by comparing predictions of extent and location of dissolution and the evolution of fluid permeability against our results from new core-flood experiments conducted on samples from the Duperow Formation (Montana, USA). Agreement between model predictions and experimental data increase our confidence that these parameter ranges need not be considered site-specific but may be applied (within reason) at various locations and reservoirs. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.

  19. Biomimetic mineralization of calcium carbonate/carboxymethylcellulose microspheres for lysozyme immobilization

    International Nuclear Information System (INIS)

    Lu Zheng; Zhang Juan; Ma Yunzi; Song Siyue; Gu Wei

    2012-01-01

    Porous calcium carbonate/carboxymethylcellulose (CaCO 3 /CMC) microspheres were prepared by the biomimetic mineralization method for lysozyme immobilization via adsorption. The size and morphology of CaCO 3 /CMC microspheres were characterized by transmitted electron microscopy (TEM) and zeta potential measurement. The lysozyme immobilization was verified by Fourier transform infrared (FTIR) spectroscopy. The effects of pHs and temperatures on lysozyme adsorption were investigated as well. It was revealed that CaCO 3 /CMC microspheres could immobilize lysozyme efficiently via electrostatic interactions and a maximum adsorption capacity of 450 mg/g was achieved at pH 9.2 and 25 °C. Moreover, it was found that the adsorption process fitted well with the Langmuir isothermal model. In addition, UV, fluorescence, and circular dichroism (CD) spectroscopic studies showed that lysozyme maintained its original secondary structure during the adsorption/desorption process. Our study therefore demonstrated that CaCO 3 /CMC microsphere can be used as a cost-effective and efficient support for lysozyme immobilization. - Graphical abstract: CaCO 3 /CMC microsphere was prepared by a facile biomimetic mineralization method and can be used as an efficient and cost-effective support for lysozyme immobilization. Highlights: ► CaCO 3 /CMC microspheres were prepared by the biomimetic mineralization method. ► Lysozyme was efficiently immobilized to CaCO 3 /CMC microspheres via adsorption. ► A maximum adsorption capacity of 450 mg/g was obtained at pH 9.2 and 25 °C. ► The original secondary structure of lysozyme was maintained upon immobilization.

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

    KAUST Repository

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

    2014-01-01

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

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

    KAUST Repository

    Zhu, Xiuping

    2014-03-24

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

  2. Mineral carbonation - possibilities in and ex-situ, evaluation and experiments in laboratory. Final report

    International Nuclear Information System (INIS)

    Bodenan, F.; Bailly, L.; Piantone, P.; Seron, A.; Touze, S.

    2006-01-01

    This report proposes a state of the art of the knowledge and a synthesis of the studies realized at the BRGM since many years, especially in the following domains: the possibilities of the natural minerals and alkaline wastes for the CO 2 sequestration under mineral form, a accounting analysis of the ex-situ processes called direct and indirect, the design of experimental bench scale to study the mineral carbonation at ambient conditions and at high pressure and temperature. (A.L.B.)

  3. 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.

  4. Simulating trends in crop yield and soil carbon in a long-term experiment - effects of rising CO2, N deposition and improved cultivation

    DEFF Research Database (Denmark)

    Berntsen, Jørgen; Petersen, Bjørn Molt; Olesen, Jørgen E.

    2006-01-01

    Measurements of crop yield and soil carbon in the Bad Lauchstädt long-term fertiliser experiment were analysed with the FASSET model. The model satisfactorily predicted yield and soil carbon development in four treatments: no fertiliser, mineral fertiliser, farmyard manure and farmyard manure plus...... was the use of new crop varieties and/or pesticides, while the increase in atmospheris CO2 and changes in local N deposition were of lesser importance. The rise in CO2 thus only explained 9-37% of the yield increase. The observed and simulated developments in soil carbon were quite different in the four...

  5. Highly CO2-supersaturated melts in the Pannonian lithospheric mantle - A transient carbon reservoir?

    Science.gov (United States)

    Créon, Laura; Rouchon, Virgile; Youssef, Souhail; Rosenberg, Elisabeth; Delpech, Guillaume; Szabó, Csaba; Remusat, Laurent; Mostefaoui, Smail; Asimow, Paul D.; Antoshechkina, Paula M.; Ghiorso, Mark S.; Boller, Elodie; Guyot, François

    2017-08-01

    determined by Raman spectroscopy and microthermometry (0.1-1.1 GPa). The CO2/silicate melt mass ratios in the metasomatic agent that percolated through the lithospheric mantle below the Pannonian Basin are estimated to be between 9.0 and 25.4 wt.%, values consistent with metasomatism either by (1) silicate melts already supersaturated in CO2 before reaching lithospheric depths or (2) carbonatite melts that interacted with mantle peridotite to generate carbonated silicic melts. Taking the geodynamical context of the Pannonian Basin and our calculations of the CO2/silicate melt mass ratios in the metasomatic agent into account, we suggest that slab-derived melts initially containing up to 25 wt.% of CO2 migrated into the lithospheric mantle and exsolved CO2-rich fluid that became trapped in secondary fluid inclusions upon fracturing of the peridotite mineral matrix. We propose a first-order estimate of 2000 ppm as the minimal bulk CO2 concentration in the lithospheric mantle below the Pannonian Basin. This transient carbon reservoir is believed to be degassed through the Pannonian Basin due to volcanism and tectonic events, mostly focused along the lithospheric-scale regional Mid-Hungarian shear Zone.

  6. Shale-brine-CO2 interactions and the long-term stability of carbonate-rich shale caprock

    Science.gov (United States)

    Ilgen, A.; Aman, M.; Espinoza, D. N.; Rodriguez, M. A.; Griego, J.; Dewers, T. A.; Feldman, J.; Stewart, T.; Choens, R. C., II

    2017-12-01

    Geological carbon storage (GCS) requires an impermeable caprock (e.g., shale) that prevents the upward migration and escape of carbon dioxide (CO2) from the subsurface. Geochemical alteration can occur at the caprock-reservoir rock interface, which could lead to the altering of the rock's mechanical properties, compromising the seal. We performed laboratory experiments on Mancos shale to quantify the coupled chemical-mechanical response of carbonate-rich shale in CO2-brine mixtures at conditions typical to GCS. We constructed geochemical models, calibrated them using laboratory results, and extended to time scales required for GCS. We observed the dissolution of calcite and kaolinite and the precipitation of gypsum and amorphous aluminum (hydr)oxide following the introduction of CO2. To address whether this mineral alteration causes changes in micro-mechanical properties, we examined altered Mancos shale using micro-mechanical (scratch) testing, measuring the scratch toughness of mm-scale shale lithofacies. The quartz-rich regions of the Mancos shale did not show significant changes in scratch toughness following 1-week alteration in a CO2-brine mixture. However, the scratch toughness of the calcite-rich, originally softer regions decreased by about 50%. These observations illustrate a coupled and localized chemical-mechanical response of carbonate-rich shale to the injection of CO2. This suggests a localized weakening of the caprock may occur, potentially leading to the development of preferential flow paths. The identification of vulnerable lithofacies within caprock and a characterization of mineralogical heterogeneity is imperative at prospective GCS sites. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC., a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy's National Nuclear Security Administration under contract DE

  7. A greenhouse-scale photosynthetic microbial bioreactor for carbon sequestration in magnesium carbonate minerals.

    Science.gov (United States)

    McCutcheon, Jenine; Power, Ian M; Harrison, Anna L; Dipple, Gregory M; Southam, Gordon

    2014-08-19

    A cyanobacteria dominated consortium collected from an alkaline wetland located near Atlin, British Columbia, Canada accelerated the precipitation of platy hydromagnesite [Mg5(CO3)4(OH)2·4H2O] in a linear flow-through experimental model wetland. The concentration of magnesium decreased rapidly within 2 m of the inflow point of the 10-m-long (∼1.5 m(2)) bioreactor. The change in water chemistry was monitored over two months along the length of the channel. Carbonate mineralization was associated with extra-cellular polymeric substances in the nutrient-rich upstream portion of the bioreactor, while the lower part of the system, which lacked essential nutrients, did not exhibit any hydromagnesite precipitation. A mass balance calculation using the water chemistry data produced a carbon sequestration rate of 33.34 t of C/ha per year. Amendment of the nutrient deficiency would intuitively allow for increased carbonation activity. Optimization of this process will have application as a sustainable mining practice by mediating magnesium carbonate precipitation in ultramafic mine tailings storage facilities.

  8. 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)

  9. Vibrational spectra of the hydrated carbonate minerals ikaite, monohydrocalcite, lansfordite and nesquehonite

    Science.gov (United States)

    Coleyshaw, Esther E.; Crump, Gregory; Griffith, William P.

    2003-08-01

    The Raman (200-4000 cm -1) and infrared (600-4000 cm -1) spectra of four rare carbonate hydrate minerals are reported. These are naturally occurring and synthetic ikaite CaCO 3 · 6H 2O, and nesquehonite MgCO 3 · 3H 2O; natural monohydrocalcite CaCO 3 · H 2O, and synthetic lansfordite MgCO 3 · 5H 2O. The spectra of synthetic ikaite partially substituted with 2H 2O and also with 13C were measured, as were those of synthetic deuteriated nesquehonite. Spectra of ikaite and lansfordite, both of which decompose at room temperatures, were measured below 0 °C. Assignments of fundamental modes are proposed.

  10. The Arctic Ocean marine carbon cycle: evaluation of air-sea CO2 exchanges, ocean acidification impacts and potential feedbacks

    Directory of Open Access Journals (Sweden)

    N. R. Bates

    2009-11-01

    Full Text Available At present, although seasonal sea-ice cover mitigates atmosphere-ocean gas exchange, the Arctic Ocean takes up carbon dioxide (CO2 on the order of −66 to −199 Tg C year−1 (1012 g C, contributing 5–14% to the global balance of CO2 sinks and sources. Because of this, the Arctic Ocean has an important influence on the global carbon cycle, with the marine carbon cycle and atmosphere-ocean CO2 exchanges sensitive to Arctic Ocean and global climate change feedbacks. In the near-term, further sea-ice loss and increases in phytoplankton growth rates are expected to increase the uptake of CO2 by Arctic Ocean surface waters, although mitigated somewhat by surface warming in the Arctic. Thus, the capacity of the Arctic Ocean to uptake CO2 is expected to alter in response to environmental changes driven largely by climate. These changes are likely to continue to modify the physics, biogeochemistry, and ecology of the Arctic Ocean in ways that are not yet fully understood. In surface waters, sea-ice melt, river runoff, cooling and uptake of CO2 through air-sea gas exchange combine to decrease the calcium carbonate (CaCO3 mineral saturation states (Ω of seawater while seasonal phytoplankton primary production (PP mitigates this effect. Biological amplification of ocean acidification effects in subsurface waters, due to the remineralization of organic matter, is likely to reduce the ability of many species to produce CaCO3 shells or tests with profound implications for Arctic marine ecosystems

  11. 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.

  12. 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.

  13. Mid-infrared and near-infrared spectroscopic study of selected magnesium carbonate minerals containing ferric iron-Implications for the geosequestration of greenhouse gases.

    Science.gov (United States)

    Frost, Ray L; Reddy, B Jagannadha; Bahfenne, Silmarilly; Graham, Jessica

    2009-04-01

    The proposal to remove greenhouse gases by pumping liquefied CO(2) several kilometres below the ground implies that many carbonate containing minerals will be formed. Among these minerals brugnatellite and coalingite are probable. Two ferric ion bearing minerals brugnatellite and coalingite with a hydrotalcite-like structure have been characterised by a combination of infrared and near-infrared (NIR) spectroscopy. The infrared spectra of the OH stretching region are characterised by OH and water stretching vibrations. Both the first and second fundamental overtones of these bands are observed in the NIR spectra in the 7030-7235 cm(-1) and 10,490-10,570 cm(-1) regions. Intense (CO(3))(2-) symmetric and antisymmetric stretching vibrations support the concept that the carbonate ion is distorted. The position of the water bending vibration indicates the water is strongly hydrogen bonded in the mineral structure. Split NIR bands at around 8675 and 11,100 cm(-1) indicate that some replacement of magnesium ions by ferrous ions in the mineral structure has occurred. Near-infrared spectroscopy is ideal for the assessment of the formation of carbonate minerals.

  14. 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.

  15. Reactions between olivine and CO2-rich seawater at 300 °C: Implications for H2 generation and CO2 sequestration on the early Earth

    Directory of Open Access Journals (Sweden)

    Hisahiro Ueda

    2017-03-01

    Full Text Available To understand the influence of fluid CO2 on ultramafic rock-hosted seafloor hydrothermal systems on the early Earth, we monitored the reaction between San Carlos olivine and a CO2-rich NaCl fluid at 300 °C and 500 bars. During the experiments, the total carbonic acid concentration (ΣCO2 in the fluid decreased from approximately 65 to 9 mmol/kg. Carbonate minerals, magnesite, and subordinate amount of dolomite were formed via the water-rock interaction. The H2 concentration in the fluid reached approximately 39 mmol/kg within 2736 h, which is relatively lower than the concentration generated by the reaction between olivine and a CO2-free NaCl solution at the same temperature. As seen in previous hydrothermal experiments using komatiite, ferrous iron incorporation into Mg-bearing carbonate minerals likely limited iron oxidation in the fluids and the resulting H2 generation during the olivine alteration. Considering carbonate mineralogy over the temperature range of natural hydrothermal fields, H2 generation is likely suppressed at temperatures below approximately 300 °C due to the formation of the Mg-bearing carbonates. Nevertheless, H2 concentration in fluid at 300 °C could be still high due to the temperature dependency of magnetite stability in ultramafic systems. Moreover, the Mg-bearing carbonates may play a key role in the ocean-atmosphere system on the early Earth. Recent studies suggest that the subduction of carbonated ultramafic rocks may transport surface CO2 species into the deep mantle. This process may have reduced the huge initial amount of CO2 on the surface of the early Earth. Our approximate calculations demonstrate that the subduction of the Mg-bearing carbonates formed in komatiite likely played a crucial role as one of the CO2 carriers from the surface to the deep mantle, even in hot subduction zones.

  16. 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

  17. Sequestering CO2 in the Built Environment

    Science.gov (United States)

    Constantz, B. R.

    2009-12-01

    Calera’s Carbonate Mineralization by Aqueous Precipitation (CMAP) technology with beneficial reuse has been called, “game-changing” by Carl Pope, Director of the Sierra Club. Calera offers a solution to the scale of the carbon problem. By capturing carbon into the built environment through carbonate mineralization, Calera provides a sound and cost-effective alternative to Geologic Sequestration and Terrestrial Sequestration. The CMAP technology permanently converts carbon dioxide into a mineral form that can be stored above ground, or used as a building material. The process produces a suite of carbonate-containing minerals of various polymorphic forms. Calera product can be substituted into blends with ordinary Portland cements and used as aggregate to produce concrete with reduced carbon, carbon neutral, or carbon negative footprints. For each ton of product produced, approximately half a ton of carbon dioxide can be sequestered using the Calera process. Coal and natural gas are composed of predominately istopically light carbon, as the carbon in the fuel is plant-derived. Thus, power plant CO2 emissions have relatively low δ13C values.The carbon species throughout the CMAP process are identified through measuring the inorganic carbon content, δ13C values of the dissolved carbonate species, and the product carbonate minerals. Measuring δ13C allows for tracking the flue gas CO2 throughout the capture process. Initial analysis of the capture of propane flue gas (δ13C ˜ -25 ‰) with seawater (δ13C ˜ -10 ‰) and industrial brucite tailings from a retired magnesium oxide plant in Moss Landing, CA (δ13C ˜ -7 ‰ from residual calcite) produced carbonate mineral products with a δ13C value of ˜ -20 ‰. This isotopically light carbon, transformed from flue gas to stable carbonate minerals, can be transferred and tracked through the capture process, and finally to the built environment. CMAP provides an economical solution to global warming by producing

  18. Variations in the patterns of soil organic carbon mineralization and microbial communities in response to exogenous application of rice straw and calcium carbonate

    International Nuclear Information System (INIS)

    Feng, Shuzhen; Huang, Yuan; Ge, Yunhui; Su, Yirong; Xu, Xinwen; Wang, Yongdong; He, Xunyang

    2016-01-01

    The addition of exogenous inorganic carbon (CaCO 3 ) and organic carbon has an important influence on soil organic carbon (SOC) mineralization in karst soil, but the microbial mechanisms underlying the SOC priming effect are poorly understood. We conducted a 100-day incubation experiment involving four treatments of the calcareous soil in southwestern China's karst region: control, 14 C-labeled rice straw addition, 14 C-labeled CaCO 3 addition, and a combination of 14 C-labeled rice straw and CaCO 3 . Changes in soil microbial communities were characterized using denaturing gradient gel electrophoresis with polymerase chain reaction (PCR-DGGE) and real-time quantitative PCR (q-PCR). Both 14 C-rice straw and Ca 14 CO 3 addition stimulated SOC mineralization, suggesting that organic and inorganic C affected SOC stability. Addition of straw alone had no significant effect on bacterial diversity; however, when the straw was added in combination with calcium carbonate, it had an inhibitory effect on bacterial and fungal diversity. At the beginning of the experimental period, exogenous additives increased bacterial abundance, although at the end of the 100-day incubation bacterial community abundance had gradually declined. Incubation time, exogenous input, and their interaction significantly affected SOC mineralization (in terms of priming and the cumulative amount of mineralization), microbial biomass carbon (MBC), and microbial community abundance and diversity. Moreover, the key factors influencing SOC mineralization were MBC, bacterial diversity, and soil pH. Overall, these findings support the view that inorganic C is involved in soil C turnover with the participation of soil microbial communities, promoting soil C cycling in the karst region. - Highlights: • Different patterns of 14 C-rice straw and Ca 14 CO 3 addition on positive priming effects of SOC mineralization. • Inorganic C is involved in soil C cycling with the participation of soil microbial

  19. Investigating Natural Analogues for Co{sub 2} Sequestration in Ultra Mafic Rocks: A Reactive Transport Modelling Approach

    Energy Technology Data Exchange (ETDEWEB)

    Gherardi, F. [Istituto di Geoscienze e Georisorse, Consiglio Nazionale delle Ricerche, Pisa (Italy)

    2013-07-15

    Serpentinites of Ligurian ophiolites are studied as natural analogues for CO{sub 2} mineral sequestration in Italy. Mineralogical and geochemical observations indicate that silicification and carbonation are typical alteration processes induced by the interaction of CO{sub 2} charged fluids with pristine ultramafic rocks. Multicomponent reactive transport models have been applied to reproduce natural patterns and investigate carbon sequestration efficiency under high P{sub CO2} conditions. Temporal changes in porosity and permeability are predicted to affect the spatial and temporal occurrence of secondary minerals. The feedback between mineralogical transformations and transport properties of the geological media emerges as a key factor controlling the mineral carbonation potential of the investigated ultramafic rocks. (author)

  20. 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.)

  1. 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

  2. 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.

  3. Effect of iron cation on geochemical trapping of CO2 in brine

    Science.gov (United States)

    Liu, Qi; Maroto-Valer, Mercedes

    2014-05-01

    Carbon dioxide sequestration using brines has emerged as a promising technology to mitigate the adverse impacts of climate change due to its large storage capacity and favorable chemistries. However, the permanent storage (mineral trapping) of CO2 in brines takes significantly long periods of time as the formation and precipitation of carbonates is very slow .[1]. The main parameters reported to effect on mineral trapping of CO2 sequestration in brines are brine composition, brine pH, system temperature and pressure.[2, 3]. It is suggested that the precipitation of mineral carbonates is mostly dependent on brine pH. Previous studies by the authors concluded that iron in natural brines causes pH instability, but it was not ascertained whether ferric iron or ferrous iron caused pH instability .[4]. Accordingly, the aim of this project is to study synthetic brines mimicking the major ions found in natural brines and including different concentrations of ferric and ferrous iron. Three brines were prepared, as follows: Brine 1 was prepared with ferric Fe3+ iron, Brine 2 prepared with ferrous Fe2+ iron and Brine 3 prepared with no iron. A series of pH stability studies and carbonation reactions were conducted using the above three brines. It is concluded that the ferrous iron causes pH instability, while ferric iron might promote carbonate precipitation. .1. Garcia, S., et al., Sequestration of non-pure carbon dioxide streams in iron oxyhydroxide-containing saline repositories. International Journal of Greenhouse Gas Control, 2012. 7: p. 89-97. 2. Liu, Q. and M.M. Maroto-Valer, Investigation of the pH effect of a typical host rock and buffer solution on CO 2 sequestration in synthetic brines. Fuel Processing Technology, 2010. 91(10): p. 1321-1329. 3. Liu, Q. and M.M. MarotoValer, Parameters affecting mineral trapping of CO2 sequestration in brines. Greenhouse Gases: Science and Technology, 2011. 1(3): p. 211-222. 4. Druckenmiller, M.L. and M.M. Maroto-Valer, Carbon

  4. 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.

  5. Subsurface Water as Natural CO{sub 2} Sink

    Energy Technology Data Exchange (ETDEWEB)

    Gillon, M. [Centre National de la Recherche Scientifique (UMR CNRS 8148-IDES), Interaction et Dynamique des Environnements de Surface, Universite Paris 11 and Centre National de la Recherche Scientifique (UMR UAPV-INRA EMMAH), Environnement Mediterraneen et Modelisation des Agro-Hydrosystemes, Universite d' Avignon et des Pays de Vaucluse, Avignon, (France); Barbecot, F.; Gibert, E.; Massault, M. [Centre National de La Recherche Scientifique (UMR CNRS 8148-IDES), Interaction et Dynamique des Environnements de Surface, Universite Paris 11 (France)

    2013-07-15

    In aquifer recharge areas, groundwater mineralization acts as an important sink for CO{sub 2} (assessed at 100 Mt{sub co2}/a on a European scale). An isotopic study of C fluxes in the unsaturated zone of a sand carbonate aquifer shows that the physical and geochemical processes controlling CO{sub 2} abstraction induce changes in the isotopic composition of both dissolved and matrix carbonates. An integrated record of these fluxes toward the aquifers is evidenced through isotopic investigation of the recharge areas. It is evidenced that the unsaturated zone represents an archive of pristine conditions, and would help to quantify downward C fluxes and environmental changes related to this CO{sub 2} abstraction process. (author)

  6. Exploratory Research on Simulation of CO2-Brine-Mineral Interactions

    Energy Technology Data Exchange (ETDEWEB)

    Chen Zhu; Shiao hung Chiang

    2005-11-01

    Application of many carbon sequestration strategies requires knowledge of thermodynamic properties for the extremely complex chemical system of CO{sub 2}-SO{sub 2}-H{sub 2}O-NaCl-CaCl{sub 2}-MgCl{sub 2}. This University Coal Research Phase I program has been successful and highly productive in exploring an approach to develop an equation of state (EOS) to describe thermodynamic properties in the above chemical system. We have compiled available laboratory experimental data and thermodynamic models, and evaluated their appropriateness for the carbon sequestration process. Based on this literature review, we provided an improved CO{sub 2} solubility model for the CO{sub 2}-H{sub 2}O-NaCl system, which incorporates newly available experimental measurements funded by DOE, and is valid in temperature range from 273 to 533 K, pressure from 0 to 2000 bar, and salinity from 0 to 4.5 molality of NaCl equivalent. The improved model also greatly improves the computational efficiency of CO{sub 2} solubility calculations and thus is better suited to be incorporated into large computer simulation models (e.g., reservoir simulation models). The literature review and model development provided insights of the data needs and directions for future work. Synergetic collaboration with DOE scientists has resulted in simulations of injected CO{sub 2} fate in sandstone aquifer with a one-dimensional numerical coupled reactive transport model. We evaluated over 100 references on CO{sub 2} solubility and submitted two manuscripts to peer-reviewed journals. One paper has been accepted for publication in ''Environmental Geosciences''.

  7. CO2 Emission Factors for Coals

    Directory of Open Access Journals (Sweden)

    P. Orlović-Leko

    2015-03-01

    Full Text Available Emission factors are used in greenhouse gas inventories to estimate emissions from coal combustion. In the absence of direct measures, emissions factors are frequently used as a quick, low cost way to estimate emissions values. Coal combustion has been a major contributor to the CO2 flux into the atmosphere. Nearly all of the fuel carbon (99 % in coal is converted to CO2 during the combustion process. The carbon content is the most important coal parameter which is the measure of the degree of coalification (coal rank. Coalification is the alteration of vegetation to form peat, succeeded by the transformation of peat through lignite, sub-bituminous, bituminous to anthracite coal. During the geochemical or metamorphic stage, the progressive changes that occur within the coal are an increase in the carbon content and a decrease in the hydrogen and oxygen content resulting in a loss of volatiles. Heterogeneous composition of coal causes variation in CO2 emission from different coals. The IPCC (Intergovernmental Panel on Climate Change has produced guidelines on how to produce emission inventories which includes emission factors. Although 2006 IPCC Guidelines provided the default values specified according to the rank of the coal, the application of country-specific emission factors was recommended when estimating the national greenhouse gas emissions. This paper discusses the differences between country-specific emission factors and default IPCC CO2 emission factors, EF(CO2, for coals. Also, this study estimated EF(CO2 for two different types of coals and peat from B&H, on the basis fuel analyses. Carbon emission factors for coal mainly depend on the carbon content of the fuel and vary with both rank and geographic origin, which supports the idea of provincial variation of carbon emission factors. Also, various other factors, such as content of sulphur, minerals and macerals play an important role and influence EF(CO2 from coal. Carbonate minerals

  8. Microbiological and Geochemical Survey of CO2-Dominated Mofette and Mineral Waters of the Cheb Basin, Czech Republic

    Directory of Open Access Journals (Sweden)

    Patryk Krauze

    2017-12-01

    Full Text Available The Cheb Basin (NW Bohemia, Czech Republic is a shallow, neogene intracontinental basin. It is a non-volcanic region which features frequent earthquake swarms and large-scale diffuse degassing of mantle-derived CO2 at the surface that occurs in the form of CO2-rich mineral springs and wet and dry mofettes. So far, the influence of CO2 degassing onto the microbial communities has been studied for soil environments, but not for aquatic systems. We hypothesized, that deep-trenching CO2 conduits interconnect the subsurface with the surface. This admixture of deep thermal fluids should be reflected in geochemical parameters and in the microbial community compositions. In the present study four mineral water springs and two wet mofettes were investigated through an interdisciplinary survey. The waters were acidic and differed in terms of organic carbon and anion/cation concentrations. Element geochemical and isotope analyses of fluid components were used to verify the origin of the fluids. Prokaryotic communities were characterized through quantitative PCR and Illumina 16S rRNA gene sequencing. Putative chemolithotrophic, anaerobic and microaerophilic organisms connected to sulfur (e.g., Sulfuricurvum, Sulfurimonas and iron (e.g., Gallionella, Sideroxydans cycling shaped the core community. Additionally, CO2-influenced waters form an ecosystem containing many taxa that are usually found in marine or terrestrial subsurface ecosystems. Multivariate statistics highlighted the influence of environmental parameters such as pH, Fe2+ concentration and conductivity on species distribution. The hydrochemical and microbiological survey introduces a new perspective on mofettes. Our results support that mofettes are either analogs or rather windows into the deep biosphere and furthermore enable access to deeply buried paleo-sediments.

  9. Investigating Interactions between the Silica and Carbon Cycles during Precipitation and Early Diagenesis of Authigenic Clay/Carbonate-Mineral Associations in the Carbonate Rock Record

    Science.gov (United States)

    McKenzie, J. A.; Francisca Martinez Ruiz, F.; Sanchez-Roman, M.; Anjos, S.; Bontognali, T. R. R.; Nascimento, G. S.; Vasconcelos, C.

    2017-12-01

    The study of authigenic clay/carbonate-mineral associations within carbonate sequences has important implications for the interpretation of scientific problems related with rock reservoir properties, such as alteration of potential porosity and permeability. More specifically, when clay minerals are randomly distributed within the carbonate matrix, it becomes difficult to predict reservoir characteristics. In order to understand this mineral association in the geological record, we have undertaken a comparative study of specially designed laboratory experiments with modern environments, where clay minerals have been shown to precipitate together with a range of carbonate minerals, including calcite, Mg-calcite and dolomite. Two modern dolomite-forming environments, the Coorong lakes, South Australia and Brejo do Espinho Rio de Janeiro, Brazil, were selected for this investigation. For comparative evaluation, enrichment microbial culture experiments, using natural pore water from Brejo do Espinho as the growth medium to promote mineral precipitation, were performed under both aerobic and anaerobic conditions. To establish the environmental parameters and biological processes facilitating the dual mineral association, the experimental samples have been compared with the natural minerals using HRTEM measurements. The results demonstrate that the clay and carbonate minerals apparently do not co-precipitate, but the precipitation of the different minerals in the same sample has probably occurred under different environmental conditions with variable chemistries, e.g., hypersalinity versus normal salinity resulting from the changing ratio of evaporation versus precipitation. Thus, the investigated mineral association is not a product of diagenetic processes but of sequential in situ precipitation processes related to changes in the silica and carbon availability. Implications for ancient carbonate formations will be presented and discussed in the context of a specific

  10. Mineral carbonation: energy costs of pretreatment options and insights gained from flow loop reaction studies

    Energy Technology Data Exchange (ETDEWEB)

    Penner, Larry R.; O' Connor, William K.; Dahlin, David C.; Gerdemann, Stephen J.; Rush, Gilbert E.

    2004-01-01

    Sequestration of carbon as a stable mineral carbonate has been proposed to mitigate environmental concerns that carbon dioxide may with time escape from its sequestered matrix using alternative sequestration technologies. A method has been developed to prepare stable carbonate products by reacting CO2 with magnesium silicate minerals in aqueous bicarbonate/chloride media at high temperature and pressure. Because this approach is inherently expensive due to slow reaction rates and high capital costs, studies were conducted to improve the reaction rates through mineral pretreatment steps and to cut expenses through improved reactor technology. An overview is given for the estimated cost of the process including sensitivity to grinding and heating as pretreatment options for several mineral feedstocks. The energy costs are evaluated for each pretreatment in terms of net carbon avoided. New studies with a high-temperature, high-pressure flow-loop reactor have yielded information on overcoming kinetic barriers experienced with processing in stirred autoclave reactors. Repeated tests with the flow-loop reactor have yielded insights on wear and failure of system components, on challenges to maintain and measure flow, and for better understanding of the reaction mechanism.

  11. Mineral carbonation: energy costs of pretreatment options and insights gained from flow loop reaction studies

    International Nuclear Information System (INIS)

    Penner, Larry R.; O'Connor, William K.; Dahlin, David C.; Gerdemann, Stephen J.; Rush, Gilbert E.

    2004-01-01

    Sequestration of carbon as a stable mineral carbonate has been proposed to mitigate environmental concerns that carbon dioxide may with time escape from its sequestered matrix using alternative sequestration technologies. A method has been developed to prepare stable carbonate products by reacting CO2 with magnesium silicate minerals in aqueous bicarbonate/chloride media at high temperature and pressure. Because this approach is inherently expensive due to slow reaction rates and high capital costs, studies were conducted to improve the reaction rates through mineral pretreatment steps and to cut expenses through improved reactor technology. An overview is given for the estimated cost of the process including sensitivity to grinding and heating as pretreatment options for several mineral feedstocks. The energy costs are evaluated for each pretreatment in terms of net carbon avoided. New studies with a high-temperature, high-pressure flow-loop reactor have yielded information on overcoming kinetic barriers experienced with processing in stirred autoclave reactors. Repeated tests with the flow-loop reactor have yielded insights on wear and failure of system components, on challenges to maintain and measure flow, and for better understanding of the reaction mechanism

  12. Probing Metal Carbonation Reactions of CO2 in a Model System Containing Forsterite and H2O Using Si-29, C-13 Magic Angle Sample Spinning NMR Spectroscopy

    Science.gov (United States)

    Hu, J.; Kwak, J.; Hoyt, D. W.; Sears, J. A.; Rosso, K. M.; Felmy, A. R.

    2009-12-01

    Ex situ solid state NMR have been used for the first time to study fundamental mineral carbonation processes and reaction extent relevant to geologic carbon sequestration using a model silicate mineral forsterite (Mg2SiO4)+scCO2 with and without H2O. Run conditions were 80C and 96 bar. Si-29 NMR clearly shows that in the absence of CO2, the role of H2O is to hydrolyze surface Mg-O-Si bonds to produce Mg2+, and mono- and oligomeric hydroxylated silica species. The surface hydrolysis products contain only Q0 (Si(OH)4) and Q1 (Si(OH)3OSi) species. An equilibrium between Q0, Q1 and Mg2+ with a saturated concentration equivalent to less than 3.2% of the Mg2SiO4 conversion is obtained at a reaction time of up to 7 days. Using scCO2 without H2O, no reaction is observed within 7 days. Using both scCO2 and H2O, the surface reaction products for silica are mainly Q3 (SiOH(OSi)3) species accompanied by a lesser amount of Q2 (Si(OH)2(OSi)2) and Q4 (Si(OSi)4). However, no Q0 and Q1 were detected, indicating the carbonic acid formation/deprotonation and magnesite (MgCO3) precipitation reactions are faster than the forsterite hydrolysis process. Thus it can be concluded that the Mg2SiO4 hydrolysis process is the rate limiting step of the overall mineral carbonation process. Si-29 NMR combined with XRD, TEM, SAED and EDX further reveal that the reaction is a surface reaction with the Mg2SiO4 crystallite in the core and with condensed Q2-Q4 species forming amorphous surface layers. C-13 MAS NMR identified a possible reaction intermediates as (MgCO3)4*Mg(OH)2*5H2O. However, at long reaction times only crystallite magnesite MgCO3 products are observed. This research is part of a broader effort at PNNL to develop experimental tools and fundamental insights into chemical transformations affecting subsurface CO2 reactive transport. Si-29 (left) and C-13 (right) MAS NMR spectra of Mg2SiO4 under various reaction conditions. Si-29 NMR reveals that in scCO2 without H2O, no reaction is

  13. 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.

  14. 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

  15. 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; hide

    2016-01-01

    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

  16. The impact of CO2 on shallow groundwater chemistry: observations at a natural analog site and implications for carbon sequestration

    Energy Technology Data Exchange (ETDEWEB)

    Keating, Elizabeth [Los Alamos National Laboratory; Fessenden, Julianna [Los Alamos National Laboratory; Kanjorski, Nancy [NON LANL; Koning, Dan [NM BUREAU OF GEOLOGY AND MINERAL RESOURCES; Pawar, Rajesh [Los Alamos National Laboratory

    2008-01-01

    In a natural analog study of risks associated with carbon sequestration, impacts of CO{sub 2} on shallow groundwater quality have been measured in a sandstone aquifer in New Mexico, USA. Despite relatively high levels of dissolved CO{sub 2}, originating from depth and producing geysering at one well, pH depression and consequent trace element mobility are relatively minor effects due to the buffering capacity of the aquifer. However, local contamination due to influx of saline waters in a subset of wells is significant. Geochemical modeling of major ion concentrations suggests that high alkalinity and carbonate mineral dissolution buffers pH changes due to CO{sub 2} influx. Analysis oftrends in dissolved trace elements, chloride, and CO2 reveal no evidence of in-situ trace element mobilization. There is clear evidence, however, that As, U, and Pb are locally co-transported into the aquifer with CO{sub 2}-rich saline water. This study illustrates the role that local geochemical conditions will play in determining the effectiveness of monitoring strategies for CO{sub 2} leakage. For example, if buffering is significant, pH monitoring may not effectively detect CO2 leakage. This study also highlights potential complications that CO{sub 2}carrier fluids, such as saline waters, pose in monitoring impacts ofgeologic sequestration.

  17. Carbon Footprint of Biofuel Sugarcane Produced in Mineral and Organic Soils in Florida

    Energy Technology Data Exchange (ETDEWEB)

    Izursa, Jose-Luis; Hanlon, Edward; Amponsah, Nana; Capece, John

    2013-02-06

    Ethanol produced from sugarcane is an existing and accessible form of renewable energy. In this study, we applied the Life Cycle Assessment (LCA) approach to estimate the Carbon Footprint (CFP) of biofuel sugarcane produced on mineral (sandy) and organic (muck) soils in Florida. CFP was estimated from greenhouse gas (GHG) emissions (CO2, CH4, and N2O) during the biofuel sugarcane cultivation. The data for the energy (fossil fuels and electricity), equipment, and chemical fertilizers were taken from enterprise budgets prepared by the University of Florida based on surveys and interviews obtained from local growers during the cropping years 2007/2008 and 2009/2010 for mineral soils and 2008/2009 for organic soils. Emissions from biomass burning and organic land use were calculated based on the IPCC guidelines. The results show that the CFP for biofuel sugarcane production is 0.04 kg CO2e kg-1y-1 when produced in mineral soils and 0.46 kg CO2e kg-1y-1 when produced in organic soils. Most of the GHG emissions from production of biofuel sugarcane in mineral soils come from equipment (33%), fertilizers (28%), and biomass burning (27%); whereas GHG emissions from production in organic soils come predominantly from the soil (93%). This difference should be considered to adopt new practices for a more sustainable farming system if biofuel feedstocks are to be considered.

  18. Variations in the patterns of soil organic carbon mineralization and microbial communities in response to exogenous application of rice straw and calcium carbonate

    Energy Technology Data Exchange (ETDEWEB)

    Feng, Shuzhen [Key Laboratory of Agro-ecological Processes in Subtropical Region, Institute of Subtropical Agriculture, Chinese Academy of Sciences, Changsha 410125 (China); University of Chinese Academy of Sciences, Beijing 100039 (China); Huanjiang Observation and Research Station for Karst Ecosystems, Chinese Academy of Sciences, Huangjiang 547100 (China); Huang, Yuan [Key Laboratory of Agro-ecological Processes in Subtropical Region, Institute of Subtropical Agriculture, Chinese Academy of Sciences, Changsha 410125 (China); University of Chinese Academy of Sciences, Beijing 100039 (China); Xinjiang Institute of Ecology and Geography, Chinese Academy of Sciences, Urumqi 830011 (China); Ge, Yunhui [Key Laboratory of Agro-ecological Processes in Subtropical Region, Institute of Subtropical Agriculture, Chinese Academy of Sciences, Changsha 410125 (China); College of Bioscience and Biotechnology, Hunan Agricultural University, Changsha 410128 (China); Su, Yirong [Key Laboratory of Agro-ecological Processes in Subtropical Region, Institute of Subtropical Agriculture, Chinese Academy of Sciences, Changsha 410125 (China); Huanjiang Observation and Research Station for Karst Ecosystems, Chinese Academy of Sciences, Huangjiang 547100 (China); Xu, Xinwen; Wang, Yongdong [Xinjiang Institute of Ecology and Geography, Chinese Academy of Sciences, Urumqi 830011 (China); He, Xunyang, E-mail: hbhpjhn@isa.ac.cn [Key Laboratory of Agro-ecological Processes in Subtropical Region, Institute of Subtropical Agriculture, Chinese Academy of Sciences, Changsha 410125 (China); Huanjiang Observation and Research Station for Karst Ecosystems, Chinese Academy of Sciences, Huangjiang 547100 (China)

    2016-11-15

    The addition of exogenous inorganic carbon (CaCO{sub 3}) and organic carbon has an important influence on soil organic carbon (SOC) mineralization in karst soil, but the microbial mechanisms underlying the SOC priming effect are poorly understood. We conducted a 100-day incubation experiment involving four treatments of the calcareous soil in southwestern China's karst region: control, {sup 14}C-labeled rice straw addition, {sup 14}C-labeled CaCO{sub 3} addition, and a combination of {sup 14}C-labeled rice straw and CaCO{sub 3}. Changes in soil microbial communities were characterized using denaturing gradient gel electrophoresis with polymerase chain reaction (PCR-DGGE) and real-time quantitative PCR (q-PCR). Both {sup 14}C-rice straw and Ca{sup 14}CO{sub 3} addition stimulated SOC mineralization, suggesting that organic and inorganic C affected SOC stability. Addition of straw alone had no significant effect on bacterial diversity; however, when the straw was added in combination with calcium carbonate, it had an inhibitory effect on bacterial and fungal diversity. At the beginning of the experimental period, exogenous additives increased bacterial abundance, although at the end of the 100-day incubation bacterial community abundance had gradually declined. Incubation time, exogenous input, and their interaction significantly affected SOC mineralization (in terms of priming and the cumulative amount of mineralization), microbial biomass carbon (MBC), and microbial community abundance and diversity. Moreover, the key factors influencing SOC mineralization were MBC, bacterial diversity, and soil pH. Overall, these findings support the view that inorganic C is involved in soil C turnover with the participation of soil microbial communities, promoting soil C cycling in the karst region. - Highlights: • Different patterns of {sup 14}C-rice straw and Ca{sup 14}CO{sub 3} addition on positive priming effects of SOC mineralization. • Inorganic C is involved in

  19. An Experimental Study of Surfactant Alternating CO2 Injection for Enhanced Oil Recovery of Carbonated Reservoir

    Directory of Open Access Journals (Sweden)

    Asghar Gandomkar

    2016-10-01

    Full Text Available Core flooding experiments were conducted with the objective of evaluating near miscible surfactant alternating CO2 injection and the effect of surfactant concentrations on gas-oil and water displacements in porous media. The core samples were provided from a low permeability mixed wet oil reservoir at 156 °F and 1900 psia. In addition, very few studies of surfactant adsorption on carbonate minerals have been conducted. Hence, the surfactant adsorption on carbonate rock was determined by core flooding and crushed tests. It was found that for the crushed rock, the required equilibrium time is approximately five hours, while it is more than four days for the flow-through tests. Hysteresis effects demonstrated that the irreducible water saturations were 5 to 10% higher than the initial connate water saturation after drainage cycles during 5000 ppm surfactant solution. Furthermore, near-miscible surfactant alternating CO2 injection process led to a 4-17% increase in the recovery factor in comparison to water alternating gas process.

  20. [Organic carbon and carbon mineralization characteristics in nature forestry soil].

    Science.gov (United States)

    Yang, Tian; Dai, Wei; An, Xiao-Juan; Pang, Huan; Zou, Jian-Mei; Zhang, Rui

    2014-03-01

    Through field investigation and indoor analysis, the organic carbon content and organic carbon mineralization characteristics of six kinds of natural forest soil were studied, including the pine forests, evergreen broad-leaved forest, deciduous broad-leaved forest, mixed needle leaf and Korean pine and Chinese pine forest. The results showed that the organic carbon content in the forest soil showed trends of gradual decrease with the increase of soil depth; Double exponential equation fitted well with the organic carbon mineralization process in natural forest soil, accurately reflecting the mineralization reaction characteristics of the natural forest soil. Natural forest soil in each layer had the same mineralization reaction trend, but different intensity. Among them, the reaction intensity in the 0-10 cm soil of the Korean pine forest was the highest, and the intensities of mineralization reaction in its lower layers were also significantly higher than those in the same layers of other natural forest soil; comparison of soil mineralization characteristics of the deciduous broad-leaved forest and coniferous and broad-leaved mixed forest found that the differences of litter species had a relatively strong impact on the active organic carbon content in soil, leading to different characteristics of mineralization reaction.

  1. 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...

  2. 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.

  3. Bioethanol: the new source for growing CO{sub 2} demand?; Bioetanol: a nova fonte para a demanda crescente por CO{sub 2}?

    Energy Technology Data Exchange (ETDEWEB)

    Martynowicz, Emile T.M.J. [Norit Haffmans, Venlo (Netherlands); Mekss, Varidots Dainis Thorvalds [Norit do Brasil Ltda., Sao Paulo, SP (Brazil)

    2009-11-01

    In recent years, while customers demand a more sustainable greener CO{sub 2} source, the worldwide demand for food-grade CO{sub 2} is steadily increasing. In Brazil, a large bio-ethanol producer, the CO{sub 2} from the bio-ethanol production is an alternative. The research focused on the activated carbon filter in a CO{sub 2} recovery plant in respect to its removal efficiency for sulfurous compounds, such as H{sub 2}S and COS. Five different types of activated carbons were investigated both in pilot scale tests as well as in full scale tests. The different adsorption behavior in respect to COS for the activated carbon was attributed to the variance in mineral trace element composition of the activated carbon. Finally, an activated carbon was selected, that could remove H{sub 2}S, DMS and COS concentrations in the low ppm range to levels of less than 20 ppbw, in even more than 50 thermal adsorption/desorption cycles. This activated carbon was tested in a full scale plant and proved to be very suitable for the process conditions encountered in a bioethanol plant. (author)

  4. Experiments and geochemical modelling of CO{sub 2} sequestration by olivine: Potential, quantification

    Energy Technology Data Exchange (ETDEWEB)

    Garcia, B., E-mail: Bruno.Garcia@ifp.fr [Institut Francais du Petrole, 1 et 4 Avenue du Bois Preau, 92852 Rueil Malmaison (France); Beaumont, V.; Perfetti, E.; Rouchon, V.; Blanchet, D. [Institut Francais du Petrole, 1 et 4 Avenue du Bois Preau, 92852 Rueil Malmaison (France); Oger, P.; Dromart, G. [Universite de Lyon, CNRS, UMR 5570, ENS de Lyon, Site Monod, 15 Parvis Rene Descartes BP 7000, Lyon F-69342 (France); Huc, A.-Y.; Haeseler, F. [Institut Francais du Petrole, 1 et 4 Avenue du Bois Preau, 92852 Rueil Malmaison (France)

    2010-09-15

    Aqueous solutions equilibrated with supercritical CO{sub 2} (150 deg. C and total pressure of 150 bar) were investigated in order to characterize their respective conditions of carbonation. Dissolution of olivine and subsequent precipitation of magnesite with a net consumption of CO{sub 2} were expected. A quantified pure mineral phase (powders with different olivine grain diameter [20-80 {mu}m], [80-125 {mu}m], [125-200 {mu}m] and [>200 {mu}m]), and CO{sub 2} (as dried ice) were placed in closed-batch reactors (soft Au tubes) in the presence of solutions. Different salinities (from 0 to 3400 mM) and different ratios of solution/solid (mineral phase) (from 0.1 to 10) were investigated. Experiments were performed over periods from 2 to 8 weeks. Final solid products were quantified by the Rock-Eval 6 technique, and identified using X-ray diffraction, Raman spectroscopy, electron microprobe and scanning electron microscopy. Gaseous compounds were quantified by a vacuum line equipped with a Toepler pump and identified and measured by gas chromatography (GC). Carbon mass balances were calculated. Olivine reacted completely with CO{sub 2}, trapping up to 57 {+-} 2% (eqC of initial CO{sub 2}) as magnesite; some amorphous silica also formed. Olivine grain diameter and solution/mineral ratios appeared to be the primary controls on the reaction, salinity acting as a second order parameter. During the experiments, fluid analyses may not be performed with approach adopted but, geochemical modelling was attempted to give information about the solution composition. This showed an interesting mineral matrix evolution. Under the experimental conditions, olivine appeared to be a good candidate for CO{sub 2} trapping into a geologically stable carbonate, magnesite. The possible use of mafic and ultramafic rocks for CO{sub 2} sequestration is discussed.

  5. 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.

  6. 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.

  7. 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

  8. 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.

  9. 大気CO_2濃度上昇が植物−土壌系に及ぼす影響評価のための島根県の天然CO_2泉の利用可能性

    OpenAIRE

    足立, 文彦; 増永, 二之; 上堂園, 明

    2008-01-01

    Sites in Ganryuji with mineral springs and Torijigoku with pure carbon dioxide(CO_2)springs were examined for their potential as experimental areas to study the effects of elevated atmospheric CO_2 concentration on soil-plant system. Soils in Ganryuji mineral spring was highly contaminated with mineral spring water. Torijigoku CO_2 spring emits very high concentration of CO_2(>30%)at a vent soil surface. Average CO_2 concentration in the middle part of the grassland was 500-1000ppm in the aft...

  10. Larnite powders and larnite/silica aerogel composites as effective agents for CO{sub 2} sequestration by carbonation

    Energy Technology Data Exchange (ETDEWEB)

    Santos, A., E-mail: alberto.santos@uca.es [Departamento de Ciencias de la Tierra, Universidad de Cadiz, Puerto Real, 11510 Cadiz (Spain); Ajbary, M.; Morales-Florez, V. [Departamento de Fisica de la Materia Condensada, Universidad de Cadiz, Puerto Real, 11510 Cadiz (Spain); Kherbeche, A. [Universite Sidi Mohamed Ben Abdellah, Ecole Superieure de Technologie, Fes (Morocco); Pinero, M. [Departamento de Fisica Aplicada, Universidad de Cadiz, Puerto Real, 11510 Cadiz (Spain); Esquivias, L. [Departamento de Fisica de la Materia Condensada, Facultad de Fisica, Instituto de Ciencias de Materiales de Sevilla (CSIC), Universidad de Sevilla, 41012 Sevilla (Spain)

    2009-09-15

    This paper presents the results of the carbonation reaction of two sample types: larnite (Ca{sub 2}SiO{sub 4}) powders and larnite/silica aerogel composites, the larnite acting as an active phase in a process of direct mineral carbonation. First, larnite powders were synthesized by the reaction of colloidal silica and calcium nitrate in the presence of ethylene glycol. Then, to synthesize the composites, the surface of the larnite powders was chemically modified with 3-aminopropyltriethoxysilane (APTES), and later this mixture was added to a silica sol previously prepared from tetraethylorthosilicate (TEOS). The resulting humid gel was dried in an autoclave under supercritical conditions for the ethanol. The textures and chemical compositions of the powders and composites were characterized.The carbonation reaction of both types of samples was evaluated by means of X-ray diffraction and thermogravimetric analysis. Both techniques confirm the high efficiency of the reaction at room temperature and atmospheric pressure. A complete transformation of the silicate into carbonate resulted after submitting the samples to a flow of pure CO{sub 2} for 15 min. This indicates that for this reaction time, 1 t of larnite could eliminate about 550 kg of CO{sub 2}. The grain size, porosity, and specific surface area are the factors controlling the reaction.

  11. 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.

  12. 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)

  13. 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.

  14. Pore space quantification of carbonate rocks before-after supercritical CO2 interaction by optical image analysis

    Science.gov (United States)

    Berrezueta, Edgar; José Domínguez-Cuesta, María

    2017-04-01

    The aim of this research is to show an experimental application of an automated quantification process of optical porosity in thin sections. Petrographic studies using scanning electronic microscopy, optical microscopy (OpM) and optical image analysis (OIA) could provide a reproducible pore characterization of carbonate rocks in applications related to the geological storage of CO2. This research is focused on i) the quantification of optical pores in a carbonate rock before and after supercritical CO2-rich brine (P ≈ 7.5 MPa and T ≈ 35 °C) and ii) the description of the process followed to guarantee the reproducibility of the OIA method on images acquired with high-resolution scanner. Mineral images were acquired from thin sections using a high-resolution scanner (HRS). Digital images were geo-referenced by using geographic information system to ensure correct spatial correlation and superposition. The optical measures of porosity by image analysis on the carbonates thin sections showed an effective pore segmentation considering different cross-polarized light conditions (90°/0°; 120°/30°) and plane-polarized light conditions (90°/-) of the same petrographic scene. The pore characterization by OpM and OIA-HRS has allowed a preliminary approximation of pore evolution in carbonate rocks under the supercritical CO2-rich brine. This study shows a fast, effective and reproducible methodology that allowed a preliminary characterization (changes in the pore network) of the samples studied. The procedure carried out could be applied to similar experimental injection tests.

  15. Sequestering CO2 by mineralization into useful nesquehonite-based products

    Directory of Open Access Journals (Sweden)

    Fredrik Paul Glasser

    2016-02-01

    Full Text Available The precipitation of magnesium hydroxy-carbonate hydrates has been suggested as a route to sequester CO2 into solids. We report the development of self-cementing compositions based on nesquehonite, MgCO3·3H2O, that are made from CO2-containing gas streams, the CO2 being separated from other gases by its high solubility in alkaline water, while magnesium is typically provided by waste desalination brines. Precipitation conditions are adjusted to optimize the formation of nesquehonite and the crystalline solid can readily be washed free of chloride. Products can be prepared to achieve self-cementation following two routes: (i thermal activation of the nesquehonite then rehydration of the precursor or (ii direct curing of a slurry of nesquehonite. The products thus obtained contain ~ 30 wt% CO2 and could form the basis for a new generation of lightweight, thermally insulating boards, blocks and panels, with sufficient strength for general construction.

  16. 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.

  17. Alteration of bentonite when contacted with supercritical CO2

    Science.gov (United States)

    Jinseok, K.; Jo, H. Y.; Yun, S. T.

    2014-12-01

    Deep saline formations overlaid by impermeable caprocks with a high sealing capacity are attractive CO2 storage reservoirs. Shales, which consist of mainly clay minerals, are potential caprocks for the CO2 storage reservoirs. The properties of clay minerals in shales may affect the sealing capacity of shales. In this study, changes in clay minerals' properties when contacted with supercritical (SC) CO2 at various conditions were investigated. Bentonite, whichis composed of primarily montmorillonite, was used as the clay material in this study. Batch reactor tests on wet bentonite samples in the presence of SC CO2 with or without aqueous phases were conducted at high pressure (12 MPa) and moderate temperature (50 oC) conditions for a week. Results show that the bentonite samples obtained from the tests with SC CO2 had less change in porosity than those obtained from the tests without SC CO2 (vacuum-drying) at a given reaction time, indicating that the bentonite samples dried in the presence of SC CO2 maintained their structure. These results suggest that CO2 molecules can diffuse into interlayer of montmorillonite, which is a primary mineral of bentonite, and form a single CO2 molecule layer or double CO2 molecule layers. The CO2 molecules can displace water molecules in the interlayer, resulting in maintaining the interlayer spacing when dehydration occurs. Noticeable changes in reacted bentonite samples obtained from the tests with an aqueous phase (NaCl, CaCl2, or sea water) are decreases in the fraction of plagioclase and pyrite and formation of carbonate minerals (i.e., calcite and dolomite) and halite. In addition, no significant exchanges of Na or Ca on the exchangeable complex of the montmorillonite in the presence of SC CO2 occurred, resulting in no significant changes in the swelling capacity of bentonite samples after reacting with SC CO2 in the presence of aqueous phases. These results might be attributed by the CO2 molecule layer, which prevents

  18. Evaluation of the CO2 sequestration capacity for coal fly ash using a flow-through column reactor under ambient conditions

    International Nuclear Information System (INIS)

    Jo, Ho Young; Ahn, Joon-Hoon; Jo, Hwanju

    2012-01-01

    Highlights: ► A conceptual in-situ mineral carbonation method using a coal ash pond is proposed. ► CO 2 uptake occurred by carbonation reaction of CO 2 with Ca 2+ ions from coal fly ash. ► The CO 2 sequestration capacity was affected by the solid dosage. ► Seawater can be used as a solvent for mineral carbonation of coal fly ash. - Abstract: An in-situ CO 2 sequestration method using coal ash ponds located in coastal regions is proposed. The CO 2 sequestration capacity of coal fly ash (CFA) by mineral carbonation was evaluated in a flow-through column reactor under various conditions (solid dosage: 100–330 g/L, CO 2 flow rate: 20–80 mL/min, solvent type: deionized (DI) water, 1 M NH 4 Cl solution, and seawater). The CO 2 sequestration tests were conducted on CFA slurries using flow-through column reactors to simulate more realistic flow-through conditions. The CO 2 sequestration capacity increased when the solid dosage was increased, whereas it was affected insignificantly by the CO 2 flow rate. A 1 M NH 4 Cl solution was the most effective solvent, but it was not significantly different from DI water or seawater. The CO 2 sequestration capacity of CFA under the flow-through conditions was approximately 0.019 g CO 2 /g CFA under the test conditions (solid dosage: 333 g/L, CO 2 flow rate: 40 mL/min, and solvent: seawater).

  19. Effects of Climate Change and Organic Matter Amendments on the Fate of Soil Carbon and the Global Warming Potential of CO2, CH4, and N2O Emissions in an Upland Soil

    Science.gov (United States)

    Simmonds, M.; Muehe, E. M.; Fendorf, S. E.

    2017-12-01

    Our current understanding of the mechanisms driving carbon stabilization in soil organic matter (SOM) and its release to the atmosphere is insufficient for predicting the response of soil carbon dynamics to future climatic conditions. The persistence of SOM has been studied primarily within the context of biochemical, physical, and geochemical protection from decomposition. More recently, bioenergetic constraints on SOM decomposition due to oxygen limitations have been demonstrated in submerged soils. However, the relevance of anaerobic domains in upland soils is uncertain. To better understand how upland soils will respond to climate change, we conducted a 52-day incubation of an upland soil at constant soil moisture (field capacity) under varying air temperatures (32°C and 37°C), CO2 concentrations (398 and 850 ppmv), and soil organic carbon contents (1.3%, 2.4%). Overall, we observed a stimulatory effect of future climate (elevated temperature and CO2) and higher carbon inputs on net SOM mineralization rates (higher CO2, CH4 and N2O emissions). Importantly, CH4 emissions were observed in the soils with added plant residue, indicating anaerobic microsites are relevant in upland soils, and significantly impact microbial respiration pathways, rates of SOM mineralization, and the global warming potential of trace gas emissions. These findings have important implications for positive soil carbon-climate feedbacks, and warrant further investigation into representing anaerobic soil domains of upland soils in biogeochemical models.

  20. Free atmospheric CO2 enrichment increased above ground biomass but did not affec symbiotic N2-fixation and soil carbon dynamics in a mixed deciduous stand in Wales

    NARCIS (Netherlands)

    Hoosbeek, M.R.; Lukac, M.; Velthorst, E.J.; Smith, A.R.; Godbold, D.

    2011-01-01

    Through increases in net primary production (NPP), elevated CO2 is hypothesized to increase the amount of plant litter entering the soil. The fate of this extra carbon on the forest floor or in mineral soil is currently not clear. Moreover, increased rates of NPP can be maintained only if forests

  1. 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.

  2. Efficient Electrocatalytic Reduction of CO2 by Nitrogen-Doped Nanoporous Carbon/Carbon Nanotube Membranes - A Step Towards the Electrochemical CO2 Refinery

    KAUST Repository

    Wang, Hong; Jia, Jia; Song, Pengfei; Wang, Qiang; Li, Debao; Min, Shixiong; Qian, Chenxi; Wang, Lu; Li, Young Feng; Ma, Chun; Wu, Tao; Yuan, Jiayin; Antonietti, Markus; Ozin, Geoffrey A.

    2017-01-01

    The search for earth abundant, efficient and stable electrocatalysts that can enable the chemical reduction of CO2 to value-added chemicals and fuels at an industrially relevant scale, is a high priority for the development of a global network of renewable energy conversion and storage systems that can meaningfully impact greenhouse gas induced climate change. Here we introduce a straightforward, low cost, scalable and technologically relevant method to manufacture an all-carbon, electroactive, nitrogen-doped nanoporous carbon-carbon nanotube composite membrane. The membrane is demonstrated to function as a binder-free, high-performance electrode for the electrocatalytic reduction of CO2 to formate. The Faradaic efficiency for the production of formate is 81%. Furthermore, the robust structural and electrochemical properties of the membrane endow it with excellent long-term stability.

  3. Efficient Electrocatalytic Reduction of CO2 by Nitrogen-Doped Nanoporous Carbon/Carbon Nanotube Membranes - A Step Towards the Electrochemical CO2 Refinery

    KAUST Repository

    Wang, Hong

    2017-05-12

    The search for earth abundant, efficient and stable electrocatalysts that can enable the chemical reduction of CO2 to value-added chemicals and fuels at an industrially relevant scale, is a high priority for the development of a global network of renewable energy conversion and storage systems that can meaningfully impact greenhouse gas induced climate change. Here we introduce a straightforward, low cost, scalable and technologically relevant method to manufacture an all-carbon, electroactive, nitrogen-doped nanoporous carbon-carbon nanotube composite membrane. The membrane is demonstrated to function as a binder-free, high-performance electrode for the electrocatalytic reduction of CO2 to formate. The Faradaic efficiency for the production of formate is 81%. Furthermore, the robust structural and electrochemical properties of the membrane endow it with excellent long-term stability.

  4. Leakage and Seepage of CO2 from Geologic Carbon Sequestration Sites: CO2 Migration into Surface Water

    International Nuclear Information System (INIS)

    Oldenburg, Curt M.; Lewicki, Jennifer L.

    2005-01-01

    Geologic carbon sequestration is the capture of anthropogenic carbon dioxide (CO 2 ) and its storage in deep geologic formations. One of the concerns of geologic carbon sequestration is that injected CO 2 may leak out of the intended storage formation, migrate to the near-surface environment, and seep out of the ground or into surface water. In this research, we investigate the process of CO 2 leakage and seepage into saturated sediments and overlying surface water bodies such as rivers, lakes, wetlands, and continental shelf marine environments. Natural CO 2 and CH 4 fluxes are well studied and provide insight into the expected transport mechanisms and fate of seepage fluxes of similar magnitude. Also, natural CO 2 and CH 4 fluxes are pervasive in surface water environments at levels that may mask low-level carbon sequestration leakage and seepage. Extreme examples are the well known volcanic lakes in Cameroon where lake water supersaturated with respect to CO 2 overturned and degassed with lethal effects. Standard bubble formation and hydrostatics are applicable to CO 2 bubbles in surface water. Bubble-rise velocity in surface water is a function of bubble size and reaches a maximum of approximately 30 cm s -1 at a bubble radius of 0.7 mm. Bubble rise in saturated porous media below surface water is affected by surface tension and buoyancy forces, along with the solid matrix pore structure. For medium and fine grain sizes, surface tension forces dominate and gas transport tends to occur as channel flow rather than bubble flow. For coarse porous media such as gravels and coarse sand, buoyancy dominates and the maximum bubble rise velocity is predicted to be approximately 18 cm s -1 . Liquid CO 2 bubbles rise slower in water than gaseous CO 2 bubbles due to the smaller density contrast. A comparison of ebullition (i.e., bubble formation) and resulting bubble flow versus dispersive gas transport for CO 2 and CH 4 at three different seepage rates reveals that

  5. Investigating CO2 Reservoirs at Gale Crater and Evidence for a Dense Early Atmosphere

    Science.gov (United States)

    Niles, P. B.; Archer, P. D.; Heil, E.; Eigenbrode, J.; McAdam, A.; Sutter, B.; Franz, H.; Navarro-Gonzalez, R.; Ming, D.; Mahaffy, P. R.; hide

    2015-01-01

    One of the most compelling features of the Gale landing site is its age. Based on crater counts, the formation of Gale crater is dated to be near the beginning of the Hesperian near the pivotal Hesperian/Noachian transition. This is a time period on Mars that is linked to increased fluvial activity through valley network formation and also marks a transition from higher erosion rates/clay mineral formation to lower erosion rates with mineralogies dominated by sulfate minerals. Results from the Curiosity mission have shown extensive evidence for fluvial activity within the crater suggesting that sediments on the floor of the crater and even sediments making up Mt. Sharp itself were the result of longstanding activity of liquid water. Warm/wet conditions on early Mars are likely due to a thicker atmosphere and increased abundance of greenhouse gases including the main component of the atmosphere, CO2. Carbon dioxide is minor component of the Earth's atmosphere yet plays a major role in surface water chemistry, weathering, and formation of secondary minerals. An ancient martian atmosphere was likely dominated by CO2 and any waters in equilibrium with this atmosphere would have different chemical characteristics. Studies have noted that high partial pressures of CO2 would result in increased carbonic acid formation and lowering of the pH so that carbonate minerals are not stable. However, if there were a dense CO2 atmosphere present at the Hesperian/Noachian transition, it would have to be stored in a carbon reservoir on the surface or lost to space. The Mt. Sharp sediments are potentially one of the best places on Mars to investigate these CO2 reservoirs as they are proposed to have formed in the early Hesperian, from an alkaline lake, and record the transition to an aeolian dominated regime near the top of the sequence. The total amount of CO2 in the Gale crater soils and sediments is significant but lower than expected if a thick atmosphere was present at the

  6. 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).

  7. 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.

  8. From Carbonatite to Ikaite: How high-T carbonates are transformed into low-T carbonate minerals in SW Greenland

    Science.gov (United States)

    Stockmann, G. J.; Tollefsen, E.; Ranta, E.; Skelton, A.; Sturkell, E.; Lundqvist, L.

    2015-12-01

    The 1300 Ma Grønnedal-Íka igneous complex in southwest Greenland comprises nepheline syenites and carbonatites. It belongs to a suite of intrusions formed 1300-1100 Ma ago referred to as the Gardar period. In modern time (the last ca. 8000 years), fluid-rock interactions involving the nepheline syenites and carbonatites gives rise to about one thousand submarine columns made of the rare low-T mineral ikaite (CaCO3x6H2O). The columns are found in a shallow, narrow fjord named Ikka Fjord and their distribution clearly follows the outcrop of the Grønnedal-Íka complex. When meteoric water percolates through the highly fractured complex, a sodium carbonate solution of pH 10 is formed through hitherto unknown fluid-rock reactions. This basic solution seeps up through fractures at the bottom of Ikka Fjord and when mixed with seawater, the mineral ikaite is formed. As the seepage water has a lower density than seawater, there is an upwards flow that creates columns. What is peculiar about ikaite is its limited stability making it unstable above +6 °C. Isotopic studies of ikaite reveal a seawater origin for the Ca2+ ions, and the carbonatite being the most likely source for the CO32- ions. The carbonatite is mainly of søvite composition (CaCO3) with high contents of siderite and ankerite in certain areas. The nepheline syenites contain Na,K-rich minerals like nepheline, alkali-feldspar, aegirine-augite, katophorite and biotite. Nepheline is mainly replaced by muscovite, and aegirine-augite partly by chlorite, which could release sodium into solution. A dolerite dyke of unknown age prompted extensive mineralization of magnetite by activating hydrothermal fluid convection. The fluid interacted with the carbonatite, replacing siderite and ankerite by magnetite and later hematite. In a newly launched project at Stockholm University, we are trying to unravel the chemical reactions taking place inside the Grønnedal-Íka igneous complex leading to the formation of the

  9. Mineral composition of durum wheat grain and pasta under increasing atmospheric CO2 concentrations.

    Science.gov (United States)

    Beleggia, Romina; Fragasso, Mariagiovanna; Miglietta, Franco; Cattivelli, Luigi; Menga, Valeria; Nigro, Franca; Pecchioni, Nicola; Fares, Clara

    2018-03-01

    The concentrations of 10 minerals were investigated in the grain of 12 durum wheat genotypes grown under free air CO 2 enrichment conditions, and in four of their derived pasta samples, using inductively coupled plasma mass spectrometry. Compared to ambient CO 2 (400ppm; AMB), under elevated CO 2 (570ppm; ELE), the micro-element and macro-element contents showed strong and significant decreases in the grain: Mn, -28.3%; Fe, -26.7%; Zn, -21.9%; Mg, -22.7%; Mo, -40.4%; K, -22.4%; and Ca, -19.5%. These variations defined the 12 genotypes as sensitive or non-sensitive to ELE. The pasta samples under AMB and ELE showed decreased mineral contents compared to the grain. Nevertheless, the contributions of the pasta to the recommended daily allowances remained relevant, also for the micro-elements under ELE conditions (range, from 18% of the recommended daily allowance for Zn, to 70% for Mn and Mo). Copyright © 2017 Elsevier Ltd. All rights reserved.

  10. 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_)

  11. Carbon Isotope Systematics in Mineral-Catalyzed Hydrothermal Organic Synthesis Processes at High Temperature and Pressures

    Science.gov (United States)

    Fu, Qi; Socki, R. A.; Niles, Paul B.

    2011-01-01

    Observation of methane in the Martian atmosphere has been reported by different detection techniques. Reduction of CO2 and/or CO during serpentization by mineral surface catalyzed Fischer-Tropsch Type (FTT) synthesis may be one possible process responsible for methane generation on Mars. With the evidence a recent study has discovered for serpentinization in deeply buried carbon rich sediments, and more showing extensive water-rock interaction in Martian history, it seems likely that abiotic methane generation via serpentinization reactions may have been common on Mars. Experiments involving mineral-catalyzed hydrothermal organic synthesis processes were conducted at 750 C and 5.5 Kbars. Alkanes, alcohols and carboxylic acids were identified as organic compounds. No "isotopic reversal" of delta C-13 values was observed for alkanes or carboxylic acids, suggesting a different reaction pathway than polymerization. Alcohols were proposed as intermediaries formed on mineral surfaces at experimental conditions. Carbon isotope data were used in this study to unravel the reaction pathways of abiotic formation of organic compounds in hydrothermal systems at high temperatures and pressures. They are instrumental in constraining the origin and evolution history of organic compounds on Mars and other planets.

  12. 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

  13. Explorative economic analysis of a novel biogas upgrading technology using carbon mineralization. A case study for Spain

    NARCIS (Netherlands)

    Starr, Katherine; Ramirez, Andrea; Meerman, Hans; Villalba, Gara; Gabarrell, Xavier

    2015-01-01

    This paper studies the potential application of a novel biogas upgrading technology called alkaline with regeneration (AwR). This technology uses an alkaline solution, along with carbon mineralization, to remove and store CO2 from biogas in order to create biomethane, a substitute of natural gas.

  14. 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

  15. 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.

  16. Dolomite decomposition under CO2

    International Nuclear Information System (INIS)

    Guerfa, F.; Bensouici, F.; Barama, S.E.; Harabi, A.; Achour, S.

    2004-01-01

    Full text.Dolomite (MgCa (CO 3 ) 2 is one of the most abundant mineral species on the surface of the planet, it occurs in sedimentary rocks. MgO, CaO and Doloma (Phase mixture of MgO and CaO, obtained from the mineral dolomite) based materials are attractive steel-making refractories because of their potential cost effectiveness and world wide abundance more recently, MgO is also used as protective layers in plasma screen manufacture ceel. The crystal structure of dolomite was determined as rhombohedral carbonates, they are layers of Mg +2 and layers of Ca +2 ions. It dissociates depending on the temperature variations according to the following reactions: MgCa (CO 3 ) 2 → MgO + CaO + 2CO 2 .....MgCa (CO 3 ) 2 → MgO + Ca + CaCO 3 + CO 2 .....This latter reaction may be considered as a first step for MgO production. Differential thermal analysis (DTA) are used to control dolomite decomposition and the X-Ray Diffraction (XRD) was used to elucidate thermal decomposition of dolomite according to the reaction. That required samples were heated to specific temperature and holding times. The average particle size of used dolomite powders is 0.3 mm, as where, the heating temperature was 700 degree celsius, using various holding times (90 and 120 minutes). Under CO 2 dolomite decomposed directly to CaCO 3 accompanied by the formation of MgO, no evidence was offered for the MgO formation of either CaO or MgCO 3 , under air, simultaneous formation of CaCO 3 , CaO and accompanied dolomite decomposition

  17. Ecological imperatives for aquatic CO2-concentrating mechanisms.

    Science.gov (United States)

    Maberly, Stephen C; Gontero, Brigitte

    2017-06-01

    In aquatic environments, the concentration of inorganic carbon is spatially and temporally variable and CO2 can be substantially oversaturated or depleted. Depletion of CO2 plus low rates of diffusion cause inorganic carbon to be more limiting in aquatic than terrestrial environments, and the frequency of species with a CO2-concentrating mechanism (CCM), and their contribution to productivity, is correspondingly greater. Aquatic photoautotrophs may have biochemical or biophysical CCMs and exploit CO2 from the sediment or the atmosphere. Though partly constrained by phylogeny, CCM activity is related to environmental conditions. CCMs are absent or down-regulated when their increased energy costs, lower CO2 affinity, or altered mineral requirements outweigh their benefits. Aquatic CCMs are most widespread in environments with low CO2, high HCO3-, high pH, and high light. Freshwater species are generally less effective at inorganic carbon removal than marine species, but have a greater range of ability to remove carbon, matching the environmental variability in carbon availability. The diversity of CCMs in seagrasses and marine phytoplankton, and detailed mechanistic studies on larger aquatic photoautotrophs are understudied. Strengthening the links between ecology and CCMs will increase our understanding of the mechanisms underlying ecological success and will place mechanistic studies in a clearer ecological context. © The Author 2017. Published by Oxford University Press on behalf of the Society for Experimental Biology. All rights reserved. For permissions, please email: journals.permissions@oup.com.

  18. Analysis of ex situ processes of CO2 sequestration. Final report

    International Nuclear Information System (INIS)

    Touze, S.; Bourgeois, F.; Baranger, P.; Durst, P.

    2004-01-01

    The aim of this study is to bring quantitative elements to evaluate the validation of the CO 2 mineral sequestration to limit the greenhouse effect gases. This analysis aims to calculate the CO 2 accounting of the system (internal energy production balance the energy expend) sequestrated CO 2 and produced CO 2 . The first part detailed the possible experimental solutions. Then two carbonation processes, direct and indirect, have been chosen of the analysis. (A.L.B.)

  19. 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.

  20. 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

  1. 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.

  2. 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

  3. Temperature response of permafrost soil carbon is attenuated by mineral protection.

    Science.gov (United States)

    Gentsch, Norman; Wild, Birgit; Mikutta, Robert; Čapek, Petr; Diáková, Katka; Schrumpf, Marion; Turner, Stephanie; Minnich, Cynthia; Schaarschmidt, Frank; Shibistova, Olga; Schnecker, Jörg; Urich, Tim; Gittel, Antje; Šantrůčková, Hana; Bárta, Jiři; Lashchinskiy, Nikolay; Fuß, Roland; Richter, Andreas; Guggenberger, Georg

    2018-05-18

    Climate change in Arctic ecosystems fosters permafrost thaw and makes massive amounts of ancient soil organic carbon (OC) available to microbial breakdown. However, fractions of the organic matter (OM) may be protected from rapid decomposition by their association with minerals. Little is known about the effects of mineral-organic associations (MOA) on the microbial accessibility of OM in permafrost soils and it is not clear which factors control its temperature sensitivity. In order to investigate if and how permafrost soil OC turnover is affected by mineral controls, the heavy fraction (HF) representing mostly MOA was obtained by density fractionation from 27 permafrost soil profiles of the Siberian Arctic. In parallel laboratory incubations, the unfractionated soils (bulk) and their HF were comparatively incubated for 175 days at 5 and 15°C. The HF was equivalent to 70 ± 9% of the bulk CO 2 respiration as compared to a share of 63 ± 1% of bulk OC that was stored in the HF. Significant reduction of OC mineralization was found in all treatments with increasing OC content of the HF (HF-OC), clay-size minerals and Fe or Al oxyhydroxides. Temperature sensitivity (Q10) decreased with increasing soil depth from 2.4 to 1.4 in the bulk soil and from 2.9 to 1.5 in the HF. A concurrent increase in the metal-to-HF-OC ratios with soil depth suggests a stronger bonding of OM to minerals in the subsoil. There, the younger 14 C signature in CO 2 than that of the OC indicates a preferential decomposition of the more recent OM and the existence of a MOA fraction with limited access of OM to decomposers. These results indicate strong mineral controls on the decomposability of OM after permafrost thaw and on its temperature sensitivity. Thus, we here provide evidence that OM temperature sensitivity can be attenuated by MOA in permafrost soils. © 2018 John Wiley & Sons Ltd.

  4. 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

  5. Element mobilization and immobilization from carbonate rocks between CO 2 storage reservoirs and the overlying aquifers during a potential CO 2 leakage

    Energy Technology Data Exchange (ETDEWEB)

    Lawter, Amanda R.; Qafoku, Nikolla P.; Asmussen, R. Matthew; Kukkadapu, Ravi K.; Qafoku, Odeta; Bacon, Diana H.; Brown, Christopher F.

    2018-04-01

    Despite the numerous studies on changes within the reservoir following CO2 injection and the effects of CO2 release into overlying aquifers, little or no literature is available on the effect of CO2 release on rock between the storage reservoirs and subsurface. To address this knowledge gap, relevant rock materials, temperatures and pressures were used to study mineralogical and elemental changes in this intermediate zone. After rocks reacted with CO2, liquid analysis showed an increase of major elements (e.g., Ca, and Mg) and variable concentrations of potential contaminants (e.g., Sr and Ba); lower concentrations were observed in N2 controls. In experiments with As/Cd and/or organic spikes, representing potential contaminants in the CO2 plume originating in the storage reservoir, most or all of these contaminants were removed from the aqueous phase. SEM and Mössbauer spectroscopy results showed the formation of new minerals and Fe oxides in some CO2-reacted samples, indicating potential for contaminant removal through mineral incorporation or adsorption onto Fe oxides. These experiments show the interactions between the CO2-laden plume and the rock between storage reservoirs and overlying aquifers have the potential to affect the level of risk to overlying groundwater, and should be considered during site selection and risk evaluation.

  6. Beyond temperature: Clumped isotope signatures in dissolved inorganic carbon species and the influence of solution chemistry on carbonate mineral composition

    Science.gov (United States)

    Tripati, Aradhna K.; Hill, Pamela S.; Eagle, Robert A.; Mosenfelder, Jed L.; Tang, Jianwu; Schauble, Edwin A.; Eiler, John M.; Zeebe, Richard E.; Uchikawa, Joji; Coplen, Tyler B.; Ries, Justin B.; Henry, Drew

    2015-10-01

    ;Clumped-isotope; thermometry is an emerging tool to probe the temperature history of surface and subsurface environments based on measurements of the proportion of 13C and 18O isotopes bound to each other within carbonate minerals in 13C18O16O22- groups (heavy isotope ;clumps;). Although most clumped isotope geothermometry implicitly presumes carbonate crystals have attained lattice equilibrium (i.e., thermodynamic equilibrium for a mineral, which is independent of solution chemistry), several factors other than temperature, including dissolved inorganic carbon (DIC) speciation may influence mineral isotopic signatures. Therefore we used a combination of approaches to understand the potential influence of different variables on the clumped isotope (and oxygen isotope) composition of minerals. We conducted witherite precipitation experiments at a single temperature and at varied pH to empirically determine 13C-18O bond ordering (Δ47) and δ18O of CO32- and HCO3- molecules at a 25 °C equilibrium. Ab initio cluster models based on density functional theory were used to predict equilibrium 13C-18O bond abundances and δ18O of different DIC species and minerals as a function of temperature. Experiments and theory indicate Δ47 and δ18O compositions of CO32- and HCO3- ions are significantly different from each other. Experiments constrain the Δ47-δ18O slope for a pH effect (0.011 ± 0.001; 12 ⩾ pH ⩾ 7). Rapidly-growing temperate corals exhibit disequilibrium mineral isotopic signatures with a Δ47-δ18O slope of 0.011 ± 0.003, consistent with a pH effect. Our theoretical calculations for carbonate minerals indicate equilibrium lattice calcite values for Δ47 and δ18O are intermediate between HCO3- and CO32-. We analyzed synthetic calcites grown at temperatures ranging from 0.5 to 50 °C with and without the enzyme carbonic anhydrase present. This enzyme catalyzes oxygen isotopic exchange between DIC species and is present in many natural systems. The two

  7. 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

  8. 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.

  9. 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

  10. Study of the reactivity of pure minerals in presence of CO2 at the supercritical state. Measurement of the portlandite carbonation kinetics

    International Nuclear Information System (INIS)

    Regnault, O.

    2008-04-01

    The efficiency on the long term of CO 2 geological storage will rely on trapping mechanisms and good sealing properties of the cap rock and the eventual access wells. A series of experiments has been devised to observe and quantify the reactivity of portlandite with supercritical CO 2 . The portlandite has been chosen as a key component of calcium-rich cement for its interest in borehole cement degradation. Initial carbonation rates have been measured under different conditions: pressure 160 bar, temperatures 80, 120, and 200 C and with various amount of water. SEM observations show that the reacting fluid state (absence or presence of liquid phase) controls strongly the carbonation behaviour and the reaction path. A specific geochemical model has been developed in order to account for the particular conditions of our experiments. These results (portlandite carbonation rate and water-poor geochemical system modelling techniques) should be useful to simulate well-bore cement degradation. (author)

  11. [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.

  12. 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

  13. Why is Dawsonite Absent in CO2 Charged Reservoirs? Pourquoi la dawsonite est-elle absente des réservoirs chargés en CO2 ?

    OpenAIRE

    Hellevang H.; Declercq J.; Aagaard P.

    2011-01-01

    Growth of the sodiumaluminium-hydroxy carbonate dawsonite (NaAl(OH)2CO3) after charging saline aquifers with CO2 has been assumed in a plethora of numerical simulations at different mineralogies, aqueous solutions, pressures and temperatures. It appears however that dawsonite is less abundant than expected in natural CO2 storage analogues if we take into account the thermodynamic stability alone. We have mapped the thermodynamic stability of dawsonite relative to mineral phases like al...

  14. Elevated moisture stimulates carbon loss from mineral soils by releasing protected organic matter.

    Science.gov (United States)

    Huang, Wenjuan; Hall, Steven J

    2017-11-24

    Moisture response functions for soil microbial carbon (C) mineralization remain a critical uncertainty for predicting ecosystem-climate feedbacks. Theory and models posit that C mineralization declines under elevated moisture and associated anaerobic conditions, leading to soil C accumulation. Yet, iron (Fe) reduction potentially releases protected C, providing an under-appreciated mechanism for C destabilization under elevated moisture. Here we incubate Mollisols from ecosystems under C 3 /C 4 plant rotations at moisture levels at and above field capacity over 5 months. Increased moisture and anaerobiosis initially suppress soil C mineralization, consistent with theory. However, after 25 days, elevated moisture stimulates cumulative gaseous C-loss as CO 2 and CH 4 to >150% of the control. Stable C isotopes show that mineralization of older C 3 -derived C released following Fe reduction dominates C losses. Counter to theory, elevated moisture may significantly accelerate C losses from mineral soils over weeks to months-a critical mechanistic deficiency of current Earth system models.

  15. Hydrogeochemical and stable isotopic investigations on CO2-rich mineral waters from Harghita Mts. (Eastern Carpathians, Romania)

    Science.gov (United States)

    Kis, Boglárka-Mercedesz; Baciu, Călin; Kármán, Krisztina; Kékedy-Nagy, Ladislau; Francesco, Italiano

    2013-04-01

    There is a worldwide interest on geothermal, mineral and groundwater as a resource for energy, drinking water supply and therapeutic needs. The increasing trend in replacing tap water with commercial bottled mineral water for drinking purposes has become an economic, hydrogeologic and medical concern in the last decades. Several investigations have been carried out worldwide on different topics related to geothermal and mineral waters, dealing with mineral water quality assessment, origin of geothermal and mineral waters, geochemical processes that influence water chemistry and water-rock interaction In Romania, the Călimani-Gurghiu-Harghita Neogene to Quaternary volcanic chain (Eastern Carpathians) is one of the most important areas from the point of view of CO2-rich mineral waters. These mineral water springs occur within other post-volcanic phenomena like dry CO2 emissions, moffettes, bubbling pools, H2S gas emissions etc. Mineral waters from this area are used for bottling, local spas and drinking purposes for local people. The number of springs, around 2000 according to literature data, shows that there is still a significant unexploited potential for good quality drinking water in this area. Within the youngest segment of the volcanic chain, the Harghita Mts., its volcaniclastic aprons and its boundary with the Transylvanian Basin, we have carried out an investigation on 23 CO2-rich mineral water springs from a hydrogeochemical and stable isotopic point of view. The mineral waters are Ca-Mg-HCO3 to Na-Cl type. Sometimes mixing between the two types can be observed. We have detected a great influence of water-rock interaction on the stable isotopic composition of the mineral waters, shown by isotopic shifts to the heavier oxygen isotope, mixing processes between shallow and deeper aquifers and local thermal anomalies. Acknowledgements: The present work was financially supported by the Romanian National Research Council, Project PN-II-ID-PCE-2011-3-0537 and by

  16. 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 ...

  17. 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).

  18. Numerical Study on CO2-Brine-Rock Interaction of Enhanced Geothermal Systems with CO2 as Heat Transmission Fluid

    Directory of Open Access Journals (Sweden)

    Wan Yuyu

    2016-01-01

    Full Text Available Enhanced Geothermal Systems (EGS with CO2 instead of water as heat transmission fluid is an attractive concept for both geothermal resources development and CO2 geological sequestration. Previous studies show that CO2 has lots of favorable properties as heat transmission fluid and also can offer geologic storage of CO2 as an ancillary benefit. However, after CO2 injection into geological formations, chemical reaction between brine and rock can change chemical characteristics of saline and properties of rock such as porosity and permeability. Is this advantage or disadvantage for EGS operating? To answer this question, we have performed chemically reactive transport modeling to investigate fluid-rock interactions and CO2 mineral carbonation of Enhanced Geothermal Systems (EGS site at Desert Peak (Nevada operated with CO2. The simulation results show that (1 injection CO2 can create a core zone fulfilled with CO2 as main working domain for EGS, and (2 CO2 storage can induced self-enhancing alteration of EGS.

  19. 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.

  20. 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.

  1. 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

  2. Reactor design considerations in mineral sequestration of carbon dioxide

    International Nuclear Information System (INIS)

    Ityokumbul, M.T.; Chander, S.; O'Connor, William K.; Dahlin, David C.; Gerdemann, Stephen J.

    2001-01-01

    One of the promising approaches to lowering the anthropogenic carbon dioxide levels in the atmosphere is mineral sequestration. In this approach, the carbon dioxide reacts with alkaline earth containing silicate minerals forming magnesium and/or calcium carbonates. Mineral carbonation is a multiphase reaction process involving gas, liquid and solid phases. The effective design and scale-up of the slurry reactor for mineral carbonation will require careful delineation of the rate determining step and how it changes with the scale of the reactor. The shrinking core model was used to describe the mineral carbonation reaction. Analysis of laboratory data indicates that the transformations of olivine and serpentine are controlled by chemical reaction and diffusion through an ash layer respectively. Rate parameters for olivine and serpentine carbonation are estimated from the laboratory data

  3. Crystal-field-driven redox reactions: How common minerals split H2O and CO2 into reduced H2 and C plus oxygen

    Science.gov (United States)

    Freund, F.; Batllo, F.; Leroy, R. C.; Lersky, S.; Masuda, M. M.; Chang, S.

    1991-01-01

    It is difficult to prove the presence of molecular H2 and reduced C in minerals containing dissolved H2 and CO2. A technique was developed which unambiguously shows that minerals grown in viciously reducing environments contain peroxy in their crystal structures. The peroxy represent interstitial oxygen atoms left behind when the solute H2O and/or CO2 split off H2 and C as a result of internal redox reactions, driven by the crystal field. The observation of peroxy affirms the presence of H2 and reduced C. It shows that the solid state is indeed an unusual reaction medium.

  4. Sequestering CO{sub 2} by Mineralization into Useful Nesquehonite-Based Products

    Energy Technology Data Exchange (ETDEWEB)

    Glasser, Fredrik Paul, E-mail: f.p.glasser@abdn.ac.uk; Jauffret, Guillaume; Morrison, Jennie [Department of Chemistry, University of Aberdeen, Aberdeen (United Kingdom); Galvez-Martos, Jose-Luis; Patterson, Naomi; Imbabi, Mohammed Salah-Eldin [School of Engineering, University of Aberdeen, Aberdeen (United Kingdom)

    2016-02-11

    The precipitation of magnesium hydroxy-carbonate hydrates has been suggested as a route to sequester CO{sub 2} into solids. We report the development of self-cementing compositions based on nesquehonite, MgCO{sub 3}⋅3H{sub 2}O, that are made from CO{sub 2}-containing gas streams, the CO{sub 2} being separated from other gases by its high solubility in alkaline water, while magnesium is typically provided by waste desalination brines. Precipitation conditions are adjusted to optimize the formation of nesquehonite and the crystalline solid can readily be washed free of chloride. Products can be prepared to achieve self-cementation following two routes: (i) thermal activation of the nesquehonite then rehydration of the precursor or (ii) direct curing of a slurry of nesquehonite. The products thus obtained contain ~30 wt% CO{sub 2} and could form the basis for a new generation of lightweight, thermally insulating boards, blocks, and panels, with sufficient strength for general construction.

  5. 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.

  6. Response of Microbial Soil Carbon Mineralization Rates to Oxygen Limitations

    Science.gov (United States)

    Keiluweit, M.; Denney, A.; Nico, P. S.; Fendorf, S. E.

    2014-12-01

    The rate of soil organic matter (SOM) mineralization is known to be controlled by climatic factors as well as molecular structure, mineral-organic associations, and physical protection. What remains elusive is to what extent oxygen (O2) limitations impact overall rates of microbial SOM mineralization (oxidation) in soils. Even within upland soils that are aerobic in bulk, factors limiting O2 diffusion such as texture and soil moisture can result in an abundance of anaerobic microsites in the interior of soil aggregates. Variation in ensuing anaerobic respiration pathways can further impact SOM mineralization rates. Using a combination of (first) aggregate model systems and (second) manipulations of intact field samples, we show how limitations on diffusion and carbon bioavailability interact to impose anaerobic conditions and associated respiration constraints on SOM mineralization rates. In model aggregates, we examined how particle size (soil texture) and amount of dissolved organic carbon (bioavailable carbon) affect O2 availability and distribution. Monitoring electron acceptor profiles (O2, NO3-, Mn and Fe) and SOM transformations (dissolved, particulate, mineral-associated pools) across the resulting redox gradients, we then determined the distribution of operative microbial metabolisms and their cumulative impact on SOM mineralization rates. Our results show that anaerobic conditions decrease SOM mineralization rates overall, but those are partially offset by the concurrent increases in SOM bioavailability due to transformations of protective mineral phases. In intact soil aggregates collected from soils varying in texture and SOM content, we mapped the spatial distribution of anaerobic microsites. Optode imaging, microsensor profiling and 3D tomography revealed that soil texture regulates overall O2 availability in aggregate interiors, while particulate SOM in biopores appears to control the fine-scale distribution of anaerobic microsites. Collectively, our

  7. Sustained effects of atmospheric [CO2] and nitrogen availability on forest soil CO2 efflux.

    Science.gov (United States)

    Oishi, A Christopher; Palmroth, Sari; Johnsen, Kurt H; McCarthy, Heather R; Oren, Ram

    2014-04-01

    Soil CO2 efflux (Fsoil ) is the largest source of carbon from forests and reflects primary productivity as well as how carbon is allocated within forest ecosystems. Through early stages of stand development, both elevated [CO2] and availability of soil nitrogen (N; sum of mineralization, deposition, and fixation) have been shown to increase gross primary productivity, but the long-term effects of these factors on Fsoil are less clear. Expanding on previous studies at the Duke Free-Air CO2 Enrichment (FACE) site, we quantified the effects of elevated [CO2] and N fertilization on Fsoil using daily measurements from automated chambers over 10 years. Consistent with previous results, compared to ambient unfertilized plots, annual Fsoil increased under elevated [CO2] (ca. 17%) and decreased with N (ca. 21%). N fertilization under elevated [CO2] reduced Fsoil to values similar to untreated plots. Over the study period, base respiration rates increased with leaf productivity, but declined after productivity saturated. Despite treatment-induced differences in aboveground biomass, soil temperature and water content were similar among treatments. Interannually, low soil water content decreased annual Fsoil from potential values - estimated based on temperature alone assuming nonlimiting soil water content - by ca. 0.7% per 1.0% reduction in relative extractable water. This effect was only slightly ameliorated by elevated [CO2]. Variability in soil N availability among plots accounted for the spatial variability in Fsoil , showing a decrease of ca. 114 g C m(-2) yr(-1) per 1 g m(-2) increase in soil N availability, with consistently higher Fsoil in elevated [CO2] plots ca. 127 g C per 100 ppm [CO2] over the +200 ppm enrichment. Altogether, reflecting increased belowground carbon partitioning in response to greater plant nutritional needs, the effects of elevated [CO2] and N fertilization on Fsoil in this stand are sustained beyond the early stages of stand development and

  8. Beyond temperature: Clumped isotope signatures in dissolved inorganic carbon species and the influence of solution chemistry on carbonate mineral composition

    Science.gov (United States)

    Tripati, Aradhna K.; Hill, Pamela S.; Eagle, Robert A.; Mosenfelder, Jed L.; Tang, Jianwu; Schauble, Edwin A.; Eiler, John M.; Zeebe, Richard E.; Uchikawa, Joji; Coplen, Tyler B.; Ries, Justin B.; Henry, Drew

    2015-01-01

    “Clumped-isotope” thermometry is an emerging tool to probe the temperature history of surface and subsurface environments based on measurements of the proportion of 13C and 18O isotopes bound to each other within carbonate minerals in 13C18O16O22- groups (heavy isotope “clumps”). Although most clumped isotope geothermometry implicitly presumes carbonate crystals have attained lattice equilibrium (i.e., thermodynamic equilibrium for a mineral, which is independent of solution chemistry), several factors other than temperature, including dissolved inorganic carbon (DIC) speciation may influence mineral isotopic signatures. Therefore we used a combination of approaches to understand the potential influence of different variables on the clumped isotope (and oxygen isotope) composition of minerals.We conducted witherite precipitation experiments at a single temperature and at varied pH to empirically determine 13C-18O bond ordering (Δ47) and δ18O of CO32- and HCO3- molecules at a 25 °C equilibrium. Ab initio cluster models based on density functional theory were used to predict equilibrium 13C-18O bond abundances and δ18O of different DIC species and minerals as a function of temperature. Experiments and theory indicate Δ47 and δ18O compositions of CO32- and HCO3- ions are significantly different from each other. Experiments constrain the Δ47-δ18O slope for a pH effect (0.011 ± 0.001; 12 ⩾ pH ⩾ 7). Rapidly-growing temperate corals exhibit disequilibrium mineral isotopic signatures with a Δ47-δ18O slope of 0.011 ± 0.003, consistent with a pH effect.Our theoretical calculations for carbonate minerals indicate equilibrium lattice calcite values for Δ47 and δ18O are intermediate between HCO3− and CO32−. We analyzed synthetic calcites grown at temperatures ranging from 0.5 to 50 °C with and without the enzyme carbonic anhydrase present. This enzyme catalyzes oxygen isotopic exchange between DIC species and is present in many

  9. 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.

  10. Mass-balance modeling of mineral weathering rates and CO2 consumption in the forested, metabasaltic Hauver Branch watershed, Catoctin Mountain, Maryland, USA

    Science.gov (United States)

    Rice, Karen; Price, Jason R.; Szymanski, David W.

    2013-01-01

    Mineral weathering rates and a forest macronutrient uptake stoichiometry were determined for the forested, metabasaltic Hauver Branch watershed in north-central Maryland, USA. Previous studies of Hauver Branch have had an insufficient number of analytes to permit determination of rates of all the minerals involved in chemical weathering, including biomass. More equations in the mass-balance matrix were added using existing mineralogic information. The stoichiometry of a deciduous biomass term was determined using multi-year weekly to biweekly stream-water chemistry for a nearby watershed, which drains relatively unreactive quartzite bedrock.At Hauver Branch, calcite hosts ~38 mol% of the calcium ion (Ca2+) contained in weathering minerals, but its weathering provides ~90% of the stream water Ca2+. This occurs in a landscape with a regolith residence time of more than several Ka (kiloannum). Previous studies indicate that such old regolith does not typically contain dissolving calcite that affects stream Ca2+/Na+ ratios. The relatively high calcite dissolution rate likely reflects dissolution of calcite in fractures of the deep critical zone.Of the carbon dioxide (CO2) consumed by mineral weathering, calcite is responsible for approximately 27%, with the silicate weathering consumption rate far exceeding that of the global average. The chemical weathering of mafic terrains in decaying orogens thus may be capable of influencing global geochemical cycles, and therefore, climate, on geological timescales. Based on carbon-balance calculations, atmospheric-derived sulfuric acid is responsible for approximately 22% of the mineral weathering occurring in the watershed. Our results suggest that rising air temperatures, driven by global warming and resulting in higher precipitation, will cause the rate of chemical weathering in the Hauver Branch watershed to increase until a threshold temperature is reached. Beyond the threshold temperature, increased recharge would

  11. 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.

  12. 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.

  13. 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.

  14. [Temperature sensitivity of CO2 fluxes from rhizosphere soil mineralization and root decomposition in Pinus massoniana and Castanopsis sclerophylla forests].

    Science.gov (United States)

    Liu, Yu; Hu, Xiao-Fei; Chen, Fu-Sheng; Yuan, Ping-Cheng

    2013-06-01

    Rhizospheric and non-rhizospheric soils and the absorption, transition, and storage roots were sampled from the mid-subtropical Pinus massoniana and Castanopsis sclerophylla forests to study the CO2 fluxes from soil mineralization and root decomposition in the forests. The samples were incubated in closed jars at 15 degrees C, 25 degrees C, 35 degrees C, and 45 degrees C, respectively, and alkali absorption method was applied to measure the CO2 fluxes during 53 days incubation. For the two forests, the rhizospheric effect (ratio of rhizospheric to non-rhizospheric soil) on the CO2 flux from soil mineralization across all incubation temperature ranged from 1.12 to 3.09, with a decreasing trend along incubation days. There was no significant difference in the CO2 flux from soil mineralization between the two forests at 15 degrees C, but the CO2 flux was significantly higher in P. massoniana forest than in C. sclerophylla forest at 25 degrees C and 35 degrees C, and in an opposite pattern at 45 degrees C. At all incubation temperature, the CO2 release from the absorption root decomposition was higher than that from the transition and storage roots decomposition, and was smaller in P. massoniana than in C. sclerophylla forest for all the root functional types. The Q10 values of the CO2 fluxes from the two forests were higher for soils (1.21-1.83) than for roots (0.96-1.36). No significant differences were observed in the Q10 values of the CO2 flux from soil mineralization between the two forests, but the Q10 value of the CO2 flux from root decomposition was significantly higher in P. massoniana than in C. sclerophylla forest. It was suggested that the increment of CO2 flux from soil mineralization under global warming was far higher than that from root decomposition, and for P. massoniana than for C. sclerophylla forest. In subtropics of China, the adaptability of zonal climax community to global warming would be stronger than that of pioneer community.

  15. 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.

  16. REDUCING UNCERTAINTIES IN MODEL PREDICTIONS VIA HISTORY MATCHING OF CO2 MIGRATION AND REACTIVE TRANSPORT MODELING OF CO2 FATE AT THE SLEIPNER PROJECT

    Energy Technology Data Exchange (ETDEWEB)

    Zhu, Chen

    2015-03-31

    An important question for the Carbon Capture, Storage, and Utility program is “can we adequately predict the CO2 plume migration?” For tracking CO2 plume development, the Sleipner project in the Norwegian North Sea provides more time-lapse seismic monitoring data than any other sites, but significant uncertainties still exist for some of the reservoir parameters. In Part I, we assessed model uncertainties by applying two multi-phase compositional simulators to the Sleipner Benchmark model for the uppermost layer (Layer 9) of the Utsira Sand and calibrated our model against the time-lapsed seismic monitoring data for the site from 1999 to 2010. Approximate match with the observed plume was achieved by introducing lateral permeability anisotropy, adding CH4 into the CO2 stream, and adjusting the reservoir temperatures. Model-predicted gas saturation, CO2 accumulation thickness, and CO2 solubility in brine—none were used as calibration metrics—were all comparable with the interpretations of the seismic data in the literature. In Part II & III, we evaluated the uncertainties of predicted long-term CO2 fate up to 10,000 years, due to uncertain reaction kinetics. Under four scenarios of the kinetic rate laws, the temporal and spatial evolution of CO2 partitioning into the four trapping mechanisms (hydrodynamic/structural, solubility, residual/capillary, and mineral) was simulated with ToughReact, taking into account the CO2-brine-rock reactions and the multi-phase reactive flow and mass transport. Modeling results show that different rate laws for mineral dissolution and precipitation reactions resulted in different predicted amounts of trapped CO2 by carbonate minerals, with scenarios of the conventional linear rate law for feldspar dissolution having twice as much mineral trapping (21% of the injected CO2) as scenarios with a Burch-type or Alekseyev et al.–type rate law for feldspar dissolution (11%). So far, most reactive transport modeling (RTM) studies for

  17. Metal release from sandstones under experimentally and numerically simulated CO2 leakage conditions.

    Science.gov (United States)

    Kirsch, Katie; Navarre-Sitchler, Alexis K; Wunsch, Assaf; McCray, John E

    2014-01-01

    Leakage of CO2 from a deep storage formation into an overlying potable aquifer may adversely impact water quality and human health. Understanding CO2-water-rock interactions is therefore an important step toward the safe implementation of geologic carbon sequestration. This study targeted the geochemical response of siliclastic rock, specifically three sandstones of the Mesaverde Group in northwestern Colorado. To test the hypothesis that carbonate minerals, even when present in very low levels, would be the primary source of metals released into a CO2-impacted aquifer, two batch experiments were conducted. Samples were reacted for 27 days with water and CO2 at partial pressures of 0.01 and 1 bar, representing natural background levels and levels expected in an aquifer impacted by a small leakage, respectively. Concentrations of major (e.g., Ca, Mg) and trace (e.g., As, Ba, Cd, Fe, Mn, Pb, Sr, U) elements increased rapidly after CO2 was introduced into the system, but did not exceed primary Maximum Contaminant Levels set by the U.S. Environmental Protection Agency. Results of sequential extraction suggest that carbonate minerals, although volumetrically insignificant in the sandstone samples, are the dominant source of mobile metals. This interpretation is supported by a simple geochemical model, which could simulate observed changes in fluid composition through CO2-induced calcite and dolomite dissolution.

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

    Science.gov (United States)

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

    2017-12-01

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

  19. Reactivity of dissolved- vs. supercritical-CO2 phase toward muscovite basal surfaces

    Science.gov (United States)

    Wan, J.; Tokunaga, T. K.; Kim, Y.; Wang, S.; Altoe, M. V. P.; Ashby, P. D.; DePaolo, D.

    2015-12-01

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

  20. 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.

  1. 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.

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

    Science.gov (United States)

    Sung, R.; Li, M.

    2013-12-01

    Mineral trapping by precipitated carbonate minerals is one of critical mechanisms for successful long-term geological sequestration (CGS) in deep saline aquifer. Aquifer acidification induced by the increase of carbonic acid (H2CO3) and bicarbonate ions (HCO3-) as the dissolution of injected CO2 may induce the dissolution of minerals and hinder the effectiveness of cap rock causing potential risk of CO2 leakage. Numerical assessments require capabilities to simulate complicated interactions of thermal, hydrological, geochemical multiphase processes. In this study, we utilized TOUGHREACT model to demonstrate a series of CGS simulations and assessments of (1) time evolution of aquifer responses, (2) migration distance and spatial distribution of CO2 plume, (3) effects of CO2-saline-mineral interactions, and (4) CO2 trapping components at the Changhua Costal Industrial Park (CCIP) Site, Taiwan. The CCIP Site is located at the Southern Taishi Basin with sloping and layered heterogeneous formations. At this preliminary phase, detailed information of mineralogical composition of reservoir formation and chemical composition of formation water are difficult to obtain. Mineralogical composition of sedimentary rocks and chemical compositions of formation water for CGS in deep saline aquifer from literatures (e.g. Xu et al., 2004; Marini, 2006) were adopted. CGS simulations were assumed with a constant CO2 injection rate of 1 Mt/yr at the first 50 years. Hydrogeological settings included porosities of 0.103 for shale, 0.141 for interbedding sandstone and shale, and 0.179 for sandstone; initial pore pressure distributions of 24.5 MPa to 28.7 MPa, an ambient temperature of 70°C, and 0.5 M of NaCl in aqueous solution. Mineral compositions were modified from Xu et al. (2006) to include calcite (1.9 vol. % of solid), quartz (57.9 %), kaolinite (2.0 %), illite (1.0 %), oligoclase (19.8 %), Na-smectite (3.9 %), K-feldspar (8.2 %), chlorite (4.6 %), and hematite (0.5 %) and were

  3. 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.

  4. 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....

  5. Laser-induced breakdown spectroscopy analysis of minerals: Carbonates and silicates

    International Nuclear Information System (INIS)

    McMillan, Nancy J.; Harmon, Russell S.; De Lucia, Frank C.; Miziolek, Andrzej M.

    2007-01-01

    Laser-induced breakdown spectroscopy (LIBS) provides an alternative chemical analytical technique that obviates the issues of sample preparation and sample destruction common to most laboratory-based analytical methods. This contribution explores the capability of LIBS analysis to identify carbonate and silicate minerals rapidly and accurately. Fifty-two mineral samples (18 carbonates, 9 pyroxenes and pyroxenoids, 6 amphiboles, 8 phyllosilicates, and 11 feldspars) were analyzed by LIBS. Two composite broadband spectra (averages of 10 shots each) were calculated for each sample to produce two databases each containing the composite LIBS spectra for the same 52 mineral samples. By using correlation coefficients resulting from the regression of the intensities of pairs of LIBS spectra, all 52 minerals were correctly identified in the database. If the LIBS spectra of each sample were compared to a database containing the other 51 minerals, 65% were identified as a mineral of similar composition from the same mineral family. The remaining minerals were misidentified for two reasons: 1) the mineral had high concentrations of an element not present in the database; and 2) the mineral was identified as a mineral with similar elemental composition from a different family. For instance, the Ca-Mg carbonate dolomite was misidentified as the Ca-Mg silicate diopside. This pilot study suggests that LIBS has promise in mineral identification and in situ analysis of minerals that record geological processes

  6. 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.

  7. 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.

  8. 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

  9. 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

  10. 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)

  11. Oxalate secretion by ectomycorrhizal Paxillus involutus is mineral-specific and controls calcium weathering from minerals

    Science.gov (United States)

    Schmalenberger, A.; Duran, A. L.; Bray, A. W.; Bridge, J.; Bonneville, S.; Benning, L. G.; Romero-Gonzalez, M. E.; Leake, J. R.; Banwart, S. A.

    2015-01-01

    Trees and their associated rhizosphere organisms play a major role in mineral weathering driving calcium fluxes from the continents to the oceans that ultimately control long-term atmospheric CO2 and climate through the geochemical carbon cycle. Photosynthate allocation to tree roots and their mycorrhizal fungi is hypothesized to fuel the active secretion of protons and organic chelators that enhance calcium dissolution at fungal-mineral interfaces. This was tested using 14CO2 supplied to shoots of Pinus sylvestris ectomycorrhizal with the widespread fungus Paxillus involutus in monoxenic microcosms, revealing preferential allocation by the fungus of plant photoassimilate to weather grains of limestone and silicates each with a combined calcium and magnesium content of over 10 wt.%. Hyphae had acidic surfaces and linear accumulation of weathered calcium with secreted oxalate, increasing significantly in sequence: quartz, granite mineral-specific oxalate exudation in ectomycorrhizal weathering to dissolve calcium bearing minerals, thus contributing to the geochemical carbon cycle. PMID:26197714

  12. 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

  13. Carbonate mineral dissolution kinetics in high pressure experiments

    Science.gov (United States)

    Dethlefsen, F.; Dörr, C.; Schäfer, D.; Ebert, M.

    2012-04-01

    The potential CO2 reservoirs in the North German Basin are overlain by a series of Mesozoic barrier rocks and aquifers and finally mostly by Tertiary and Quaternary close-to-surface aquifers. The unexpected rise of stored CO2 from its reservoir into close-to-surface aquifer systems, perhaps through a broken well casing, may pose a threat to groundwater quality because of the acidifying effect of CO2 dissolution in water. The consequences may be further worsening of the groundwater quality due to the mobilization of heavy metals. Buffer mechanisms counteracting the acidification are for instance the dissolution of carbonates. Carbonate dissolution kinetics is comparably fast and carbonates can be abundant in close-to-surface aquifers. The disadvantages of batch experiments compared to column experiments in order to determine rate constants are well known and have for instance been described by v. GRINSVEN and RIEMSDIJK (1992). Therefore, we have designed, developed, tested, and used a high-pressure laboratory column system to simulate aquifer conditions in a flow through setup within the CO2-MoPa project. The calcite dissolution kinetics was determined for CO2-pressures of 6, 10, and 50 bars. The results were evaluated by using the PHREEQC code with a 1-D reactive transport model, applying a LASAGA (1984) -type kinetic dissolution equation (PALANDRI and KHARAKA, 2004; eq. 7). While PALANDRI and KHARAKA (2004) gave calcite dissolution rate constants originating from batch experiments of log kacid = -0.3 and log kneutral = -5.81, the data of the column experiment were best fitted using log kacid = -2.3 and log kneutral = -7.81, so that the rate constants fitted using the lab experiment applying 50 bars pCO2 were approximately 100 times lower than according to the literature data. Rate constants of experiments performed at less CO2 pressure (pCO2 = 6 bars: log kacid = -1.78; log kneutral = -7.29) were only 30 times lower than literature data. These discrepancies in the

  14. Zinc oxide nanoparticles affect carbon and nitrogen mineralization of Phoenix dactylifera leaf litter in a sandy soil.

    Science.gov (United States)

    Rashid, Muhammad Imtiaz; Shahzad, Tanvir; Shahid, Muhammad; Ismail, Iqbal M I; Shah, Ghulam Mustafa; Almeelbi, Talal

    2017-02-15

    We investigated the impact of zinc oxide nanoparticles (ZnO NPs; 1000mgkg -1 soil) on soil microbes and their associated soil functions such as date palm (Phoenix dactylifera) leaf litter (5gkg -1 soil) carbon and nitrogen mineralization in mesocosms containing sandy soil. Nanoparticles application in litter-amended soil significantly decreased the cultivable heterotrophic bacterial and fungal colony forming units (cfu) compared to only litter-amended soil. The decrease in cfu could be related to lower microbial biomass carbon in nanoparticles-litter amended soil. Likewise, ZnO NPs also reduced CO 2 emission by 10% in aforementioned treatment but this was higher than control (soil only). Labile Zn was only detected in the microbial biomass of nanoparticles-litter applied soil indicating that microorganisms consumed this element from freely available nutrients in the soil. In this treatment, dissolved organic carbon and mineral nitrogen were 25 and 34% lower respectively compared to litter-amended soil. Such toxic effects of nanoparticles on litter decomposition resulted in 130 and 122% lower carbon and nitrogen mineralization efficiency respectively. Hence, our results entail that ZnO NPs are toxic to soil microbes and affect their function i.e., carbon and nitrogen mineralization of applied litter thus confirming their toxicity to microbial associated soil functions. Copyright © 2016 Elsevier B.V. All rights reserved.

  15. Evaluation of the CO{sub 2} sequestration capacity for coal fly ash using a flow-through column reactor under ambient conditions

    Energy Technology Data Exchange (ETDEWEB)

    Jo, Ho Young, E-mail: hyjo@korea.ac.kr [Department of Earth and Environmental Sciences, Korea University, Anam-dong, Seongbuk-gu, Seoul 136-713 (Korea, Republic of); Ahn, Joon-Hoon; Jo, Hwanju [Department of Earth and Environmental Sciences, Korea University, Anam-dong, Seongbuk-gu, Seoul 136-713 (Korea, Republic of)

    2012-11-30

    Highlights: Black-Right-Pointing-Pointer A conceptual in-situ mineral carbonation method using a coal ash pond is proposed. Black-Right-Pointing-Pointer CO{sub 2} uptake occurred by carbonation reaction of CO{sub 2} with Ca{sup 2+} ions from coal fly ash. Black-Right-Pointing-Pointer The CO{sub 2} sequestration capacity was affected by the solid dosage. Black-Right-Pointing-Pointer Seawater can be used as a solvent for mineral carbonation of coal fly ash. - Abstract: An in-situ CO{sub 2} sequestration method using coal ash ponds located in coastal regions is proposed. The CO{sub 2} sequestration capacity of coal fly ash (CFA) by mineral carbonation was evaluated in a flow-through column reactor under various conditions (solid dosage: 100-330 g/L, CO{sub 2} flow rate: 20-80 mL/min, solvent type: deionized (DI) water, 1 M NH{sub 4}Cl solution, and seawater). The CO{sub 2} sequestration tests were conducted on CFA slurries using flow-through column reactors to simulate more realistic flow-through conditions. The CO{sub 2} sequestration capacity increased when the solid dosage was increased, whereas it was affected insignificantly by the CO{sub 2} flow rate. A 1 M NH{sub 4}Cl solution was the most effective solvent, but it was not significantly different from DI water or seawater. The CO{sub 2} sequestration capacity of CFA under the flow-through conditions was approximately 0.019 g CO{sub 2}/g CFA under the test conditions (solid dosage: 333 g/L, CO{sub 2} flow rate: 40 mL/min, and solvent: seawater).

  16. 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.

  17. Variations in pCO2 during summer in the surface water of an unproductive lake in northern Sweden

    International Nuclear Information System (INIS)

    Jonsson, A.; Aaberg, J.; Jansson, M.

    2007-01-01

    Unproductive lakes are generally supersaturated with carbon dioxide (CO 2 ) and emit CO 2 to the atmosphere continuously during ice-free periods. However, temporal variation of the partial pressure of CO 2 (pCO 2 ) and thus of CO 2 evasion to atmosphere is poorly documented. We therefore carried out temporally high-resolution (every 6 h) measurements of the pCO 2 using an automated logger system in the surface water of a subarctic, unproductive, lake in the birch forest belt. The study period was June-September 2004. We found that the pCO 2 showed large seasonal variation, but low daily variation. The seasonal variation was likely mainly caused by variations in input and mineralization of allochthonous organic matter. Stratification depth probably also influenced pCO 2 of the surface water by controlling the volume in which mineralization of dissolved organic carbon (DOC) occurred. In lakes, with large variations in pCO 2 , as in our study lake a high (weekly) sampling intensity is recommended for obtaining accurate estimates of the evasion of CO 2

  18. 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.

  19. Protein-assisted synthesis of double-shelled CaCO3 microcapsules and their mineralization with heavy metal ions.

    Science.gov (United States)

    Li, Xuan Qi; Feng, Zhiwei; Xia, Yinyan; Zeng, Hua Chun

    2012-02-13

    Calcium carbonate (CaCO(3)) is one of the most abundant and important biominerals in nature. Due to its biocompatibility, biodegradability and nontoxicity, CaCO(3) has been investigated extensively in recent years for various fundamental properties and technological applications. Inspired by basic wall structures of cells, we report a protein-assisted approach to synthesize CaCO(3) into a double-shelled structural configuration. Due to varying reactivities of outer and inner shells, the CaCO(3) microcapsules exhibit different sorption capacities and various resultant structures toward different kinds of heavy metal ions, analogical to biologically controlled mineralization (BCM) processes. Surprisingly, three mineralization modes resembling those found in BCM were found with these bacterium-like "CaCO(3) cells". Our investigation of the cytotoxicity (MTT assay protocol) also indicates that the CaCO(3) microcapsules have almost no cytotoxicity against HepG2 cells, and they might be useful for future application of detoxifying heavy metal ions after further study. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  20. 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...

  1. 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.

  2. 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.)

  3. 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...

  4. 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.

  5. 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.

  6. 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.

  7. 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...

  8. 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.

  9. Monitoring CO2 emissions to gain a dynamic view of carbon allocation to arbuscular mycorrhizal fungi.

    Science.gov (United States)

    Slavíková, Renata; Püschel, David; Janoušková, Martina; Hujslová, Martina; Konvalinková, Tereza; Gryndlerová, Hana; Gryndler, Milan; Weiser, Martin; Jansa, Jan

    2017-01-01

    Quantification of carbon (C) fluxes in mycorrhizal plants is one of the important yet little explored tasks of mycorrhizal physiology and ecology. 13 CO 2 pulse-chase labelling experiments are increasingly being used to track the fate of C in these plant-microbial symbioses. Nevertheless, continuous monitoring of both the below- and aboveground CO 2 emissions remains a challenge, although it is necessary to establish the full C budget of mycorrhizal plants. Here, a novel CO 2 collection system is presented which allows assessment of gaseous CO 2 emissions (including isotopic composition of their C) from both belowground and shoot compartments. This system then is used to quantify the allocation of recently fixed C in mycorrhizal versus nonmycorrhizal Medicago truncatula plants with comparable biomass and mineral nutrition. Using this system, we confirmed substantially greater belowground C drain in mycorrhizal versus nonmycorrhizal plants, with the belowground CO 2 emissions showing large variation because of fluctuating environmental conditions in the glasshouse. Based on the assembled 13 C budget, the C allocation to the mycorrhizal fungus was between 2.3% (increased 13 C allocation to mycorrhizal substrate) and 2.9% (reduction of 13 C allocation to mycorrhizal shoots) of the plant gross photosynthetic production. Although the C allocation to shoot respiration (measured during one night only) did not differ between the mycorrhizal and nonmycorrhizal plants under our experimental conditions, it presented a substantial part (∼10%) of the plant C budget, comparable to the amount of CO 2 released belowground. These results advocate quantification of both above- and belowground CO 2 emissions in future studies.

  10. 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.

  11. Mineralogical controls on porosity and water chemistry during O_2-SO_2-CO_2 reaction of CO_2 storage reservoir and cap-rock core

    International Nuclear Information System (INIS)

    Pearce, Julie K.; Golab, Alexandra; Dawson, Grant K.W.; Knuefing, Lydia; Goodwin, Carley; Golding, Suzanne D.

    2016-01-01

    Reservoir and cap-rock core samples with variable lithology's representative of siliciclastic reservoirs used for CO_2 storage have been characterized and reacted at reservoir conditions with an impure CO_2 stream and low salinity brine. Cores from a target CO_2 storage site in Queensland, Australia were tested. Mineralogical controls on the resulting changes to porosity and water chemistry have been identified. The tested siliciclastic reservoir core samples can be grouped generally into three responses to impure CO_2-brine reaction, dependent on mineralogy. The mineralogically clean quartzose reservoir cores had high porosities, with negligible change after reaction, in resolvable porosity or mineralogy, calculated using X-ray micro computed tomography and QEMSCAN. However, strong brine acidification and a high concentration of dissolved sulphate were generated in experiments owing to minimal mineral buffering. Also, the movement of kaolin has the potential to block pore throats and reduce permeability. The reaction of the impure CO_2-brine with calcite-cemented cap-rock core samples caused the largest porosity changes after reaction through calcite dissolution; to the extent that one sample developed a connection of open pores that extended into the core sub-plug. This has the potential to both favor injectivity but also affect CO_2 migration. The dissolution of calcite caused the buffering of acidity resulting in no significant observable silicate dissolution. Clay-rich cap-rock core samples with minor amounts of carbonate minerals had only small changes after reaction. Created porosity appeared mainly disconnected. Changes were instead associated with decreases in density from Fe-leaching of chlorite or dissolution of minor amounts of carbonates and plagioclase. The interbedded sandstone and shale core also developed increased porosity parallel to bedding through dissolution of carbonates and reactive silicates in the sandy layers. Tight interbedded cap

  12. Preparation of granular activated carbons from yellow mombin fruit stones for CO2 adsorption.

    Science.gov (United States)

    Fiuza, Raildo Alves; Medeiros de Jesus Neto, Raimundo; Correia, Laise Bacelar; Carvalho Andrade, Heloysa Martins

    2015-09-15

    Stones of yellow mombin, a native fruit of the tropical America and West Indies, were used as starting materials to produce activated carbons, subsequently used as adsorbent for CO2 capture. The carbonaceous materials were either chemically activated with HNO3, H3PO4 and KOH or physically activated with CO2. The carbon samples were characterized by SEM, EDX, TG/DTA, Raman spectroscopy, physical adsorption for textural analysis and by acid-base titrations. The CO2 adsorption capacity and adsorption cycles were investigated by TG. The results indicate that the capacity of CO2 adsorption may be maximized on highly basic surfaces of micropores smaller than 1 nm. The KOH activated carbon showed high and stable capacity of CO2 adsorption after 10 cycles. Copyright © 2015 Elsevier Ltd. All rights reserved.

  13. 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)

  14. 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.

  15. 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 

  16. 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...

  17. Geological and Geotechnical Site Investigation for the Design of a CO2 Rich Flue Gas Direct Injection and Storage Facility

    Energy Technology Data Exchange (ETDEWEB)

    Metz, Paul; Bolz, Patricia

    2013-03-25

    With international efforts to limit anthropogenic carbon in the atmosphere, various CO{sub 2} sequestration methods have been studied by various facilities worldwide. Basalt rock in general has been referred to as potential host material for mineral carbonation by various authors, without much regard for compositional variations due to depositional environment, subsequent metamorphism, or hydrothermal alteration. Since mineral carbonation relies on the presence of certain magnesium, calcium, or iron silicates, it is necessary to study the texture, mineralogy, petrology, and geochemistry of specific basalts before implying potential for mineral carbonation. The development of a methodology for the characterization of basalts with respect to their susceptibility for mineral carbonation is proposed to be developed as part of this research. The methodology will be developed based on whole rock data, petrography and microprobe analyses for samples from the Caledonia Mine in Michigan, which is the site for a proposed small-scale demonstration project on mineral carbonation in basalt. Samples from the Keweenaw Peninsula will be used to determine general compositional trends using whole rock data and petrography. Basalts in the Keweenaw Peninsula have been subjected to zeolite and prehnite-pumpellyite facies metamorphism with concurrent native copper deposition. Alteration was likely due to the circulation of CO{sub 2}-rich fluids at slightly elevated temperatures and pressures, which is the process that is attempted to be duplicated by mineral carbonation.

  18. 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.

  19. 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.

  20. Experimental investigation of CO2-brine-rock interactions at elevated temperature and pressure: Implications for CO2 sequestration in deep-saline aquifers

    Science.gov (United States)

    Rosenbauer, R.J.; Koksalan, T.; Palandri, J.L.

    2005-01-01

    Deep-saline aquifers are potential repositories for excess CO2, currently being emitted to the atmosphere from anthropogenic activities, but the reactivity of supercritical CO2 with host aquifer fluids and formation minerals needs to be understood. Experiments reacting supercritical CO2 with natural and synthetic brines in the presence and absence of limestone and plagioclase-rich arkosic sandstone showed that the reaction of CO2-saturated brine with limestone results in compositional, mineralogical, and porosity changes in the aquifer fluid and rock that are dependent on initial brine composition, especially dissolved calcium and sulfate. Experiments reacting CO2-saturated, low-sulfate brine with limestone dissolved 10% of the original calcite and increased rock porosity by 2.6%. Experiments reacting high-sulfate brine with limestone, both in the presence and absence of supercritical CO2, were characterized by the precipitation of anhydrite, dolomitization of the limestone, and a final decrease in porosity of 4.5%. However, based on favorable initial porosity changes of about 15% due to the dissolution of calcite, the combination of CO2 co-injection with other mitigation strategies might help alleviate some of the well-bore scale and formation-plugging problems near the injection zone of a brine disposal well in Paradox Valley, Colorado, as well as provide a repository for CO2. Experiments showed that the solubility of CO2 is enhanced in brine in the presence of limestone by 9% at 25 ??C and 6% at 120 ??C and 200 bar relative to the brine itself. The solubility of CO2 is enhanced also in brine in the presence of arkosic sandstone by 5% at 120 ??C and 300 bar. The storage of CO 2 in limestone aquifers is limited to only ionic and hydraulic trapping. However, brine reacted with supercritical CO2 and arkose yielded fixation and sequestration of CO2 in carbonate mineral phases. Brine desiccation was observed in all experiments containing a discrete CO2 phase

  1. 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

  2. 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.

  3. Simplified models of transport and reactions in conditions of CO2 storage in saline aquifers

    Science.gov (United States)

    Suchodolska, Katarzyna; Labus, Krzysztof

    2016-04-01

    Simple hydrogeochemical models may serve as tools of preliminary assessment of CO2 injection and sequestraton impact on the aquifer and cap-rocks. In order to create models of reaction and transport in conditions of CO2 injection and storage, the TOUGHREACT simulator, and the Geochemist's Workbench software were applied. The chemical composition of waters for kinetic transport models based on the water - rock equilibrium calculations. Analyses of reaction and transport of substances during CO2 injection and storage period were carried out in three scenarios: one-dimensional radial model, and two-dimensional model of CO2 injection and sequestration, and one-dimensional model of aquifer - cap-rock interface. Modeling was performed in two stages. The first one simulated the immediate changes in the aquifer and insulating rocks impacted by CO2 injection (100 days in case of reaction model and 30 years in transport and reaction model), the second - enabled assessment of long-term effects of sequestration (20000 years). Reactions' quality and progress were monitored and their effects on formation porosity and sequestration capacity in form of mineral, residual and free phase of CO2 were calculated. Calibration of numerical models (including precipitation of secondary minerals, and correction of kinetics parameters) describing the initial stage of injection, was based on the experimental results. Modeling allowed to evaluate the pore space saturation with gas, changes in the composition and pH of pore waters, relationships between porosity and permeability changes and crystallization or dissolution minerals. We assessed the temporal and spatial extent of crystallization processes, and the amount of carbonates trapping. CO2 in mineral form. The calculated sequestration capacity of analyzed formations reached n·100 kg/m3 for the: dissolved phase - CO(aq), gas phase - CO2(g) and mineral phase, but as much as 101 kg/m3 for the supercritical phase - SCCO2. Processes of gas

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

    DEFF Research Database (Denmark)

    Beulig, Felix

    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 ......2-induced geochemical changes promoted anaerobic and acidophilic organisms and altered carbon turnover in affected soils.......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...

  5. 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.

  6. 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.

  7. 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)

  8. 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

  9. 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.

  10. 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

  11. Electron Transfer Strategies Regulate Carbonate Mineral and Micropore Formation

    Science.gov (United States)

    Zeng, Zhirui; Tice, Michael M.

    2018-01-01

    Some microbial carbonates are robust biosignatures due to their distinct morphologies and compositions. However, whether carbonates induced by microbial iron reduction have such features is unknown. Iron-reducing bacteria use various strategies to transfer electrons to iron oxide minerals (e.g., membrane-bound enzymes, soluble electron shuttles, nanowires, as well as different mechanisms for moving over or attaching to mineral surfaces). This diversity has the potential to create mineral biosignatures through manipulating the microenvironments in which carbonate precipitation occurs. We used Shewanella oneidensis MR-1, Geothrix fermentans, and Geobacter metallireducens GS-15, representing three different strategies, to reduce solid ferric hydroxide in order to evaluate their influence on carbonate and micropore formation (micro-size porosity in mineral rocks). Our results indicate that electron transfer strategies determined the morphology (rhombohedral, spherical, or long-chained) of precipitated calcium-rich siderite by controlling the level of carbonate saturation and the location of carbonate formation. Remarkably, electron transfer strategies also produced distinctive cell-shaped micropores in both carbonate and hydroxide minerals, thus producing suites of features that could potentially serve as biosignatures recording information about the sizes, shapes, and physiologies of iron-reducing organisms.

  12. An investigation of reaction parameters on geochemical storage of non-pure CO2 streams in iron oxides-bearing formations

    Energy Technology Data Exchange (ETDEWEB)

    Garcia, Susana; Liu, Q.; Bacon, Diana H.; Maroto-Valer, M. M.

    2014-08-26

    Hematite deposit that is the main FeIII-bearing mineral in sedimentary red beds was proposed as a potential host repository for converting CO2 into carbonate minerals such as siderite (FeCO3), when CO2–SO2 gas mixtures are co-injected. This work investigated CO2 mineral trapping using hematite and sensitivity of the reactive systems to different parameters, including particle size, gas composition, temperature, pressure, and solid-to-liquid ratio. Experimental and modelling studies of hydrothermal experiments were conducted, which emulated a CO2 sequestration scenario by injecting CO2-SO2 gas streams into a NaCl-NaOH brine hosted in iron oxide-containing aquifer. This study provides novel information on the mineralogical changes and fluid chemistry derived from the co-injection of CO2-SO2 gas mixtures in hematite deposit. It can be concluded that the amount of siderite precipitate depends primarily on the SO2 content of the gas stream. Increasing SO2 content in the system could promote the reduction of Fe3+ from the hematite sample to Fe2+, which will be further available for its precipitation as siderite. Moreover, siderite precipitation is enhanced at low temperatures and high pressures. The influence of the solid to liquid ratio on the overall carbonation reaction suggests that the conversion increases if the system becomes more diluted.

  13. [Effects of Chinese prickly ash orchard on soil organic carbon mineralization and labile organic carbon in karst rocky desertification region of Guizhou province].

    Science.gov (United States)

    Zhang, Wen-Juan; Liao, Hong-Kai; Long, Jian; Li, Juan; Liu, Ling-Fei

    2015-03-01

    Taking 5-year-old Chinese prickly ash orchard (PO-5), 17-year-old Chinese prickly ash orchard (PO- 17), 30-year-old Chinese prickly ash orchard (PO-30) and the forest land (FL, about 60 years) in typical demonstration area of desertification control test in southwestern Guizhou as our research objects, the aim of this study using a batch incubation experiment was to research the mineralization characteristics of soil organic carbon and changes of the labile soil organic carbon contents at different depths (0-15 cm, 15-30 cm, and 30-50 cm). The results showed that: the cumulative mineralization amounts of soil organic carbon were in the order of 30-year-old Chinese prickly ash orchard, the forest land, 5-year-old Chinese prickly ash orchard and 17-year-old Chinese prickly ash orchard at corresponding depth. Distribution ratios of CO2-C cumulative mineralization amount to SOC contents were higher in Chinese prickly ash orchards than in forest land at each depth. Cultivation of Chinese prickly ash in long-term enhanced the mineralization of soil organic carbon, and decreased the stability of soil organic carbon. Readily oxidized carbon and particulate organic carbon in forest land soils were significantly more than those in Chinese prickly ash orchards at each depth (P < 0.05). With the increasing times of cultivation of Chinese prickly ash, the contents of readily oxidized carbon and particulate organic carbon first increased and then declined at 0-15 cm and 15-30 cm depth, respectively, but an opposite trend was found at 30-50 cm depth. At 0-15 cm and 15-30 cm, cultivation of Chinese prickly ash could be good for improving the contents of labile soil organic carbon in short term, but it was not conducive in long-term. In this study, we found that cultivation of Chinese prickly ash was beneficial for the accumulation of labile organic carbon at the 30-50 cm depth.

  14. 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.

  15. 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.

  16. 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

  17. Electron Transfer Strategies Regulate Carbonate Mineral and Micropore Formation.

    Science.gov (United States)

    Zeng, Zhirui; Tice, Michael M

    2018-01-01

    Some microbial carbonates are robust biosignatures due to their distinct morphologies and compositions. However, whether carbonates induced by microbial iron reduction have such features is unknown. Iron-reducing bacteria use various strategies to transfer electrons to iron oxide minerals (e.g., membrane-bound enzymes, soluble electron shuttles, nanowires, as well as different mechanisms for moving over or attaching to mineral surfaces). This diversity has the potential to create mineral biosignatures through manipulating the microenvironments in which carbonate precipitation occurs. We used Shewanella oneidensis MR-1, Geothrix fermentans, and Geobacter metallireducens GS-15, representing three different strategies, to reduce solid ferric hydroxide in order to evaluate their influence on carbonate and micropore formation (micro-size porosity in mineral rocks). Our results indicate that electron transfer strategies determined the morphology (rhombohedral, spherical, or long-chained) of precipitated calcium-rich siderite by controlling the level of carbonate saturation and the location of carbonate formation. Remarkably, electron transfer strategies also produced distinctive cell-shaped micropores in both carbonate and hydroxide minerals, thus producing suites of features that could potentially serve as biosignatures recording information about the sizes, shapes, and physiologies of iron-reducing organisms. Key Words: Microbial iron reduction-Micropore-Electron transfer strategies-Microbial carbonate. Astrobiology 18, 28-36.

  18. Reactivity of dolomite in water-saturated supercritical carbon dioxide: Significance for carbon capture and storage and for enhanced oil and gas recovery

    International Nuclear Information System (INIS)

    Wang Xiuyu; Alvarado, Vladimir; Swoboda-Colberg, Norbert; Kaszuba, John P.

    2013-01-01

    Highlights: ► Dolomite reactivity with wet and dry supercritical CO 2 were evaluated. ► Dolomite does not react with dry CO 2 . ► H 2 O-saturated supercritical CO 2 dissolves dolomite and precipitates carbonate mineral. ► Temperature/reaction time control morphology and extent of carbonate mineralization. ► Reaction with wet CO 2 may impact trapping, caprock integrity, and CCS/EOR injectivity. - Abstract: Carbon dioxide injection in porous reservoirs is the basis for carbon capture and storage, enhanced oil and gas recovery. Injected carbon dioxide is stored at multiple scales in porous media, from the pore-level as a residual phase to large scales as macroscopic accumulations by the injection site, under the caprock and at reservoir internal capillary pressure barriers. These carbon dioxide saturation zones create regions across which the full spectrum of mutual CO 2 –H 2 O solubility may occur. Most studies assume that geochemical reaction is restricted to rocks and carbon dioxide-saturated formation waters, but this paradigm ignores injection of anhydrous carbon dioxide against brine and water-alternating-gas flooding for enhanced oil recovery. A series of laboratory experiments was performed to evaluate the reactivity of the common reservoir mineral dolomite with water-saturated supercritical carbon dioxide. Experiments were conducted at reservoir conditions (55 and 110 °C, 25 MPa) and elevated temperature (220 °C, 25 MPa) for approximately 96 and 164 h (4 and 7 days). Dolomite dissolves and new carbonate mineral precipitates by reaction with water-saturated supercritical carbon dioxide. Dolomite does not react with anhydrous supercritical carbon dioxide. Temperature and reaction time control the composition, morphology, and extent of formation of new carbonate minerals. Mineral dissolution and re-precipitation due to reaction with water-saturated carbon dioxide may affect the contact line between phases, the carbon dioxide contact angle, and the

  19. 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.

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

    Science.gov (United States)

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

  1. 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

  2. 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.

  3. Interfacially controlled phenomena in the system K2CO3-KAlO2

    International Nuclear Information System (INIS)

    Cook, L.P.

    1981-01-01

    Potassium carbonate has become of special interest to a number of ceramists because of its use as ionizing seed material which is added to combustion gases to produce a conductive plasma in magnetohydrodynamic electrical power generators. In this high temperature environment, chemical interaction occurs not only with ceramic components of the system such as electrodes and insulators, but also with the mineral ash of the coal used to fuel the generator. As a result, potassium aluminate is an important component of the slags accummulating in such generators. The system K 2 CO 3 -KAlO 2 is under investigation as part of a more general study of potassium carbonate - slag interaction. This note is a summary of some preliminary observations on the phase equilibria of K 2 CO 3 -KAlO 2 with focus on the unusual melting behavior of Kat''CO 3 /KAlO 2 mixtures which appears to have its origin in interfacial interaction

  4. 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

  5. Geochemical Interaction of Middle Bakken Reservoir Rock and CO2 during CO2-Based Fracturing

    Science.gov (United States)

    Nicot, J. P.; Lu, J.; Mickler, P. J.; Ribeiro, L. H.; Darvari, R.

    2015-12-01

    This study was conducted to investigate the effects of geochemical interactions when CO2 is used to create the fractures necessary to produce hydrocarbons from low-permeability Middle Bakken sandstone. The primary objectives are to: (1) identify and understand the geochemical reactions related to CO2-based fracturing, and (2) assess potential changes of reservoir property. Three autoclave experiments were conducted at reservoir conditions exposing middle Bakken core fragments to supercritical CO2 (sc-CO2) only and to CO2-saturated synthetic brine. Ion-milled core samples were examined before and after the reaction experiments using scanning electron microscope, which enabled us to image the reaction surface in extreme details and unambiguously identify mineral dissolution and precipitation. The most significant changes in the reacted rock samples exposed to the CO2-saturated brine is dissolution of the carbonate minerals, particularly calcite which displays severely corrosion. Dolomite grains were corroded to a lesser degree. Quartz and feldspars remained intact and some pyrite framboids underwent slight dissolution. Additionally, small amount of calcite precipitation took place as indicated by numerous small calcite crystals formed at the reaction surface and in the pores. The aqueous solution composition changes confirm these petrographic observations with increase in Ca and Mg and associated minor elements and very slight increase in Fe and sulfate. When exposed to sc-CO2 only, changes observed include etching of calcite grain surface and precipitation of salt crystals (halite and anhydrite) due to evaporation of residual pore water into the sc-CO2 phase. Dolomite and feldspars remained intact and pyrite grains were slightly altered. Mercury intrusion capillary pressure tests on reacted and unreacted samples shows an increase in porosity when an aqueous phase is present but no overall porosity change caused by sc-CO2. It also suggests an increase in permeability

  6. 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....

  7. 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.

  8. Heavy metal immobilization via microbially induced carbonate precipitation and co-precipitation

    Science.gov (United States)

    Lauchnor, E. G.; Stoick, E.

    2017-12-01

    Microbially induced CaCO3 precipitation (MICP) has been successfully used in applications such as porous media consolidation and sealing of leakage pathways in the subsurface, and it has the potential to be used for remediation of metal and radionuclide contaminants in surface and groundwater. In this work, MICP is investigated for removal of dissolved heavy metals from contaminated mine discharge water via co-precipitation in CaCO3 or formation of other metal carbonates. The bacterially catalyzed hydrolysis of urea produces inorganic carbon and ammonium and increases pH and the saturation index of carbonate minerals to promote precipitation of CaCO3. Other heavy metal cations can be co-precipitated in CaCO3 as impurities or by replacing Ca2+ in the crystal lattice. We performed laboratory batch experiments of MICP in alkaline mine drainage sampled from an abandoned mine site in Montana and containing a mixture of heavy metals at near neutral pH. Both a model bacterium, Sporosarcina pasteurii, and a ureolytic bacterium isolated from sediments on the mine site were used to promote MICP. Removal of dissolved metals from the aqueous phase was determined via inductively coupled plasma mass spectrometry and resulting precipitates were analyzed via electron microscopy and energy dispersive x-ray spectroscopy (EDX). Both S. pasteurii and the native ureolytic isolate demonstrated ureolysis, increased the pH and promoted precipitation of CaCO3 in batch tests. MICP by the native bacterium reduced concentrations of the heavy metals zinc, copper, cadmium, nickel and manganese in the water. S. pasteurii was also able to promote MICP, but with less removal of dissolved metals. Analysis of precipitates revealed calcium carbonate and phosphate minerals were likely present. The native isolate is undergoing identification via 16S DNA sequencing. Ongoing work will evaluate biofilm formation and MICP by the isolate in continuous flow, gravel-filled laboratory columns. This research

  9. Liming induces carbon dioxide (CO2) emission in PSB inoculated alkaline soil supplemented with different phosphorus sources.

    Science.gov (United States)

    Adnan, Muhammad; Shah, Zahir; Sharif, Muhammad; Rahman, Hidayatur

    2018-04-01

    Agricultural land is a major sink of global organic carbon (C). Its suitable management is crucial for improving C sequestration and reducing soil CO 2 emission. Incubation experiments were performed to assess the impact of phosphate solubilizing bacterial (PSB) inoculation (inoculated and uninoculated) and soil calcification (4.78, 10, 15, and 20% crushed CaCO 3 ) with phosphorus (P) sources [single superphosphate (SSP), rock phosphate (RP), farm yard manure (FYM), and poultry manure (PM)] in experiment 1 and with various rates of PM (4, 8, and 12 kg ha -1 ) in experiment 2 on cumulative soil respiration. These experiments were arranged in three factorial, complete randomize design (CRD) with three replications. Interactively, lime with P sources (at day 1 and 3) and lime with PSB (at day 1) significantly expedited soil respiration. Mainly, PSB inoculation, liming, PM fertilization, and its various rates significantly enhanced soil respiration with time over control/minimum in alkaline soil at all incubation periods. Higher CO 2 emission was detected in soil supplemented with organic P sources (PM and FYM) than mineral sources (SSP and RP). CO 2 emission was noted to increase with increasing PM content. Since liming intensified CO 2 discharge from soil, therefore addition of lime to an alkaline soil should be avoided; instead, integrated approaches must be adopted for P management in alkaline calcareous soils for climate-smart agriculture.

  10. Contrasting Impact of Future CO2 Emission Scenarios on the Extent of CaCO3 Mineral Undersaturation in the Humboldt Current System

    Science.gov (United States)

    Franco, A. C.; Gruber, N.; Frölicher, T. L.; Kropuenske Artman, L.

    2018-03-01

    The eastern boundary upwelling systems are among those regions that are most vulnerable to an ocean acidification-induced transition toward undersaturated conditions with respect to mineral CaCO3, but no assessment exists yet for the Humboldt Current System. Here we use a high-resolution (˜7.5 km) regional ocean model to investigate past and future changes in ocean pH and CaCO3 saturation state in this system. We find that within the next few decades, the nearshore waters off Peru are projected to become corrosive year round with regard to aragonite, the more soluble form of CaCO3. The volume of aragonite undersaturated water off Peru will continue to increase in the future irrespective of the amount of CO2 emitted to the atmosphere. In contrast, the development of the saturation state with regard to calcite, a less soluble form of carbonate, depends strongly on the scenario followed. By 2050, calcite undersaturation appears in the nearshore waters off Peru occasionally, but by 2090 in a high-emission scenario (RCP8.5), ˜60% of the water in the euphotic zone will become permanently calcite undersaturated. Most of this calcite undersaturation off Peru can likely be avoided if a low emission scenario (RCP2.6) consistent with the Paris Agreement is followed. The progression of ocean acidification off Chile follows a similar pattern, except that the saturation states are overall higher. But also here, calcite undersaturated waters will become common in the subsurface waters under the RCP8.5 scenario by the end of this century, while this can be avoided under the RCP2.6 scenario.

  11. 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

  12. 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.)

  13. 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.

  14. LIBS Sensor for Sub-surface CO2 Leak Detection in Carbon Sequestration

    Directory of Open Access Journals (Sweden)

    Jinesh JAIN

    2017-07-01

    Full Text Available Monitoring carbon sequestration poses numerous challenges to the sensor community. For example, the subsurface environment is notoriously harsh, with large potential mechanical, thermal, and chemical stresses, making long-term stability and survival a challenge to any potential in situ monitoring method. Laser induced breakdown spectroscopy (LIBS has been demonstrated as a promising technology for chemical monitoring of harsh environments and hard to reach places. LIBS has a real- time monitoring capability and can be used for the elemental and isotopic analysis of solid, liquid, and gas samples. The flexibility of the probe design and the use of fiber- optics has made LIBS particularly suited for remote measurements. The paper focuses on developing a LIBS instrument for downhole high-pressure, high-temperature brine experiments, where CO2 leakage could result in changes in the trace mineral composition of an aquifer. The progress in fabricating a compact, robust, and simple LIBS sensor for widespread subsurface leak detection is presented.

  15. 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

  16. Experimental Study of Cement - Sandstone/Shale - Brine - CO2 Interactions.

    Science.gov (United States)

    Carroll, Susan A; McNab, Walt W; Torres, Sharon C

    2011-11-11

    Reactive-transport simulation is a tool that is being used to estimate long-term trapping of CO2, and wellbore and cap rock integrity for geologic CO2 storage. We reacted end member components of a heterolithic sandstone and shale unit that forms the upper section of the In Salah Gas Project carbon storage reservoir in Krechba, Algeria with supercritical CO2, brine, and with/without cement at reservoir conditions to develop experimentally constrained geochemical models for use in reactive transport simulations. We observe marked changes in solution composition when CO2 reacted with cement, sandstone, and shale components at reservoir conditions. The geochemical model for the reaction of sandstone and shale with CO2 and brine is a simple one in which albite, chlorite, illite and carbonate minerals partially dissolve and boehmite, smectite, and amorphous silica precipitate. The geochemical model for the wellbore environment is also fairly simple, in which alkaline cements and rock react with CO2-rich brines to form an Fe containing calcite, amorphous silica, smectite and boehmite or amorphous Al(OH)3. Our research shows that relatively simple geochemical models can describe the dominant reactions that are likely to occur when CO2 is stored in deep saline aquifers sealed with overlying shale cap rocks, as well as the dominant reactions for cement carbonation at the wellbore interface.

  17. 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.

  18. A literature review of actinide-carbonate mineral interactions

    International Nuclear Information System (INIS)

    Stout, D.L.

    1993-10-01

    Chemical retardation of actinides in groundwater systems is a potentially important mechanism for assessing the performance of the Waste Isolation Pilot Plant (WIPP), a facility intended to demonstrate safe disposal of transuranic waste. Rigorous estimation of chemical retardation during transport through the Culebra Dolomite, a water-bearing unit overlying the WIPP, requires a mechanistic understanding of chemical reactions between dissolved elements and mineral surfaces. This report represents a first step toward this goal by examining the literature for pertinent experimental studies of actinide-carbonate interactions. A summary of existing models is given, along with the types of experiments on which these models are based. Articles pertaining to research into actinide interactions with carbonate minerals are summarized. Select articles involving trace element-carbonate mineral interactions are also reviewed and may serve as templates for future research. A bibliography of related articles is included. Americium(III), and its nonradioactive analog neodymium(III), partition strongly from aqueous solutions into carbonate minerals. Recent thermodynamic, kinetic, and surface studies show that Nd is preferentially removed from solution, forming a Nd-Ca carbonate solid solution. Neptunium(V) is rapidly removed from solution by carbonates. Plutonium incorporation into carbonates is complicated by multiple oxidation states. Little research has been done on the radium(H) and thorium(IV) carbonate systems. Removal of uranyl ion from solution by calcite is limited to monolayer surface coverage

  19. 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

  20. Carbonizing bituminous minerals

    Energy Technology Data Exchange (ETDEWEB)

    1921-05-01

    A process for carbonizing bituminous minerals, like oil-shale, in a furnace with addition of air in the presence of heat-receiving material is characterized by the fact that to the feed such solid or liquid material (with the exception of oil) is added, which, through vaporization or heat-binding decomposition or conversion, hinders the establishment of excessive temperatures.

  1. 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

  2. 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.

  3. 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.

  4. 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.

  5. 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.

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

    Science.gov (United States)

    Han, Young-Soo; Tokunaga, Tetsu K

    2014-12-01

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

  7. CO 2 breakthrough—Caprock sealing efficiency and integrity for carbon geological storage

    KAUST Repository

    Espinoza, D. Nicolas; Santamarina, Carlos

    2017-01-01

    Small pores in high specific surface clay-rich caprocks give rise to high capillary entry pressures and high viscous drag that hinder the migration of buoyant carbon dioxide CO2. We measured the breakthrough pressure and ensuing CO2 permeability

  8. CO2 adsorption-assisted CH4 desorption on carbon models of coal surface: A DFT study

    Science.gov (United States)

    Xu, He; Chu, Wei; Huang, Xia; Sun, Wenjing; Jiang, Chengfa; Liu, Zhongqing

    2016-07-01

    Injection of CO2 into coal is known to improve the yields of coal-bed methane gas. However, the technology of CO2 injection-enhanced coal-bed methane (CO2-ECBM) recovery is still in its infancy with an unclear mechanism. Density functional theory (DFT) calculations were performed to elucidate the mechanism of CO2 adsorption-assisted CH4 desorption (AAD). To simulate coal surfaces, different six-ring aromatic clusters (2 × 2, 3 × 3, 4 × 4, 5 × 5, 6 × 6, and 7 × 7) were used as simplified graphene (Gr) carbon models. The adsorption and desorption of CH4 and/or CO2 on these carbon models were assessed. The results showed that a six-ring aromatic cluster model (4 × 4) can simulate the coal surface with limited approximation. The adsorption of CO2 onto these carbon models was more stable than that in the case of CH4. Further, the adsorption energies of single CH4 and CO2 in the more stable site were -15.58 and -18.16 kJ/mol, respectively. When two molecules (CO2 and CH4) interact with the surface, CO2 compels CH4 to adsorb onto the less stable site, with a resulting significant decrease in the adsorption energy of CH4 onto the surface of the carbon model with pre-adsorbed CO2. The Mulliken charges and electrostatic potentials of CH4 and CO2 adsorbed onto the surface of the carbon model were compared to determine their respective adsorption activities and changes. At the molecular level, our results showed that the adsorption of the injected CO2 promoted the desorption of CH4, the underlying mechanism of CO2-ECBM.

  9. Effects of high CO2 levels on dynamic photosynthesis: carbon gain, mechanisms, and environmental interactions.

    Science.gov (United States)

    Tomimatsu, Hajime; Tang, Yanhong

    2016-05-01

    Understanding the photosynthetic responses of terrestrial plants to environments with high levels of CO2 is essential to address the ecological effects of elevated atmospheric CO2. Most photosynthetic models used for global carbon issues are based on steady-state photosynthesis, whereby photosynthesis is measured under constant environmental conditions; however, terrestrial plant photosynthesis under natural conditions is highly dynamic, and photosynthetic rates change in response to rapid changes in environmental factors. To predict future contributions of photosynthesis to the global carbon cycle, it is necessary to understand the dynamic nature of photosynthesis in relation to high CO2 levels. In this review, we summarize the current body of knowledge on the photosynthetic response to changes in light intensity under experimentally elevated CO2 conditions. We found that short-term exposure to high CO2 enhances photosynthetic rate, reduces photosynthetic induction time, and reduces post-illumination CO2 burst, resulting in increased leaf carbon gain during dynamic photosynthesis. However, long-term exposure to high CO2 during plant growth has varying effects on dynamic photosynthesis. High levels of CO2 increase the carbon gain in photosynthetic induction in some species, but have no significant effects in other species. Some studies have shown that high CO2 levels reduce the biochemical limitation on RuBP regeneration and Rubisco activation during photosynthetic induction, whereas the effects of high levels of CO2 on stomatal conductance differ among species. Few studies have examined the influence of environmental factors on effects of high levels of CO2 on dynamic photosynthesis. We identified several knowledge gaps that should be addressed to aid future predictions of photosynthesis in high-CO2 environments.

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

    Science.gov (United States)

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

    2010-01-01

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

  11. Characterisation, quantification and modelling of CO2 transport and interactions in a carbonate vadose zone: application to a CO2 diffusive leakage in a geological sequestration context

    International Nuclear Information System (INIS)

    Cohen, Gregory

    2013-01-01

    Global warming is related to atmospheric greenhouse gas concentration increase and especially anthropogenic CO 2 emissions. Geologic sequestration has the potential capacity and the longevity to significantly diminish anthropogenic CO 2 emissions. This sequestration in deep geological formation induces leakage risks from the geological reservoir. Several leakage scenarios have been imagined. Since it could continue for a long period, inducing environmental issues and risks for human, the scenario of a diffusive leakage is the most worrying. Thus, monitoring tools and protocols are needed to set up a near-surface monitoring plan. The present thesis deals with this problematic. The aims are the characterisation, the quantification and the modelling of transport and interactions of CO 2 in a carbonate unsaturated zone. This was achieved following an experimental approach on a natural pilot site in Saint-Emilion (Gironde, France), where diffusive gas leakage experiments were set up in a carbonate unsaturated zone. Different aspects were investigated during the study: natural pilot site description and instrumentation; the physical and chemical characterisation of carbonate reservoir heterogeneity; the natural functioning of the carbonate unsaturated zone and especially the set-up of a CO 2 concentrations baseline; the characterisation of gas plume extension following induced diffusive leakage in the carbonate unsaturated zone and the study of gas-water-rock interactions during a CO 2 diffusive leakage in a carbonate unsaturated zone through numerical simulations. The results show the importance of the carbonate reservoir heterogeneity characterisation as well as the sampling and analysing methods for the different phases. The baseline set-up is of main interest since it allows discrimination between the induced and the natural CO 2 concentrations variations. The transfer of CO 2 in a carbonate unsaturated zone is varying in function of physical and chemical properties

  12. Effect of carbonic anhydrase on silicate weathering and carbonate formation at present day CO2 concentrations compared to primordial values

    Science.gov (United States)

    Xiao, Leilei; Lian, Bin; Hao, Jianchao; Liu, Congqiang; Wang, Shijie

    2015-01-01

    It is widely recognized that carbonic anhydrase (CA) participates in silicate weathering and carbonate formation. Nevertheless, it is still not known if the magnitude of the effect produced by CA on surface rock evolution changes or not. In this work, CA gene expression from Bacillus mucilaginosus and the effects of recombination protein on wollastonite dissolution and carbonate formation under different conditions are explored. Real-time fluorescent quantitative PCR was used to explore the correlation between CA gene expression and sufficiency or deficiency in calcium and CO2 concentration. The results show that the expression of CA genes is negatively correlated with both CO2 concentration and ease of obtaining soluble calcium. A pure form of the protein of interest (CA) is obtained by cloning, heterologous expression, and purification. The results from tests of the recombination protein on wollastonite dissolution and carbonate formation at different levels of CO2 concentration show that the magnitudes of the effects of CA and CO2 concentration are negatively correlated. These results suggest that the effects of microbial CA in relation to silicate weathering and carbonate formation may have increased importance at the modern atmospheric CO2 concentration compared to 3 billion years ago. PMID:25583135

  13. Variations in pCO{sub 2} during summer in the surface water of an unproductive lake in northern Sweden

    Energy Technology Data Exchange (ETDEWEB)

    Jonsson, A.; Aaberg, J.; Jansson, M. [Dept. of Ecology and Environmental Sci ence, Umeaa Univ., 901 87 Umeaa (Sweden)]. e-mail: anders.jonsson@emg.umu.se

    2007-11-15

    Unproductive lakes are generally supersaturated with carbon dioxide (CO{sub 2}) and emit CO{sub 2} to the atmosphere continuously during ice-free periods. However, temporal variation of the partial pressure of CO{sub 2} (pCO{sub 2}) and thus of CO{sub 2} evasion to atmosphere is poorly documented. We therefore carried out temporally high-resolution (every 6 h) measurements of the pCO{sub 2} using an automated logger system in the surface water of a subarctic, unproductive, lake in the birch forest belt. The study period was June-September 2004. We found that the pCO{sub 2} showed large seasonal variation, but low daily variation. The seasonal variation was likely mainly caused by variations in input and mineralization of allochthonous organic matter. Stratification depth probably also influenced pCO{sub 2} of the surface water by controlling the volume in which mineralization of dissolved organic carbon (DOC) occurred. In lakes, with large variations in pCO{sub 2}, as in our study lake a high (weekly) sampling intensity is recommended for obtaining accurate estimates of the evasion of CO{sub 2}.

  14. Characterizing biospheric carbon balance using CO2 observations from the OCO-2 satellite

    Directory of Open Access Journals (Sweden)

    S. M. Miller

    2018-05-01

    Full Text Available NASA's Orbiting Carbon Observatory 2 (OCO-2 satellite launched in summer of 2014. Its observations could allow scientists to constrain CO2 fluxes across regions or continents that were previously difficult to monitor. This study explores an initial step toward that goal; we evaluate the extent to which current OCO-2 observations can detect patterns in biospheric CO2 fluxes and constrain monthly CO2 budgets. Our goal is to guide top-down, inverse modeling studies and identify areas for future improvement. We find that uncertainties and biases in the individual OCO-2 observations are comparable to the atmospheric signal from biospheric fluxes, particularly during Northern Hemisphere winter when biospheric fluxes are small. A series of top-down experiments indicate how these errors affect our ability to constrain monthly biospheric CO2 budgets. We are able to constrain budgets for between two and four global regions using OCO-2 observations, depending on the month, and we can constrain CO2 budgets at the regional level (i.e., smaller than seven global biomes in only a handful of cases (16 % of all regions and months. The potential of the OCO-2 observations, however, is greater than these results might imply. A set of synthetic data experiments suggests that retrieval errors have a salient effect. Advances in retrieval algorithms and to a lesser extent atmospheric transport modeling will improve the results. In the interim, top-down studies that use current satellite observations are best-equipped to constrain the biospheric carbon balance across only continental or hemispheric regions.

  15. A simple approach to estimate soil organic carbon and soil co/sub 2/ emission

    International Nuclear Information System (INIS)

    Abbas, F.

    2013-01-01

    SOC (Soil Organic Carbon) and soil CO/sub 2/ (Carbon Dioxide) emission are among the indicator of carbon sequestration and hence global climate change. Researchers in developed countries benefit from advance technologies to estimate C (Carbon) sequestration. However, access to the latest technologies has always been challenging in developing countries to conduct such estimates. This paper presents a simple and comprehensive approach for estimating SOC and soil CO/sub 2/ emission from arable- and forest soils. The approach includes various protocols that can be followed in laboratories of the research organizations or academic institutions equipped with basic research instruments and technology. The protocols involve soil sampling, sample analysis for selected properties, and the use of a worldwide tested Rothamsted carbon turnover model. With this approach, it is possible to quantify SOC and soil CO/sub 2/ emission over short- and long-term basis for global climate change assessment studies. (author)

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

    DEFF Research Database (Denmark)

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

    2017-01-01

    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......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...

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

    Science.gov (United States)

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

    2014-12-01

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

  18. Evidence for CO2 reactive adsorption on nanoporous S- and N-doped carbon at ambient conditions

    Energy Technology Data Exchange (ETDEWEB)

    Bandosz, Teresa J. [City College of New York, NY (United States). Dept. of Chemistry; Seredych, Mykola [City College of New York, NY (United States). Dept. of Chemistry; Rodríguez-Castellón, Enrique [Univ. of Malaga (Spain). Dept. of Inorganic Chemistry; Cheng, Yongqiang [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division; Daemen, Luke L. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division; Ramírez-Cuesta, Anibal J. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division

    2015-10-08

    CO2 interactions with nanoporous S- and N-doped polymer-derived carbon and commercial wood-based carbon were investigated in a broad range of conditions. The results showed that during CO2 adsorption nitrogen and sulfur species as well as water were released from the carbon surface as a result of chemical reactions of the surface groups with CO2. Inelastic neutron scattering experiments provided the unprecedented ability to characterize very small amounts of CO2 and H2O and revealed for the first time their physical/chemical status in the confined space of nanoporous carbons. The results obtained suggest that the reactivity of the carbon surface should be considered when CO2 storage media are chosen and when CO2 is used as a probe to determine the microporosity of carbon materials.

  19. Preparation and characterization of pitch-based nanoporous carbons for improving CO{sub 2} capture

    Energy Technology Data Exchange (ETDEWEB)

    Lee, Seul-Yi; Yoo, Hye-Min [Department of Chemistry, Inha University, 100 Inharo, Nam-gu, Incheon (Korea, Republic of); Park, Sang Wook; Hee Park, Sang; Oh, Young Se [GS Caltex Corporation, Munji-dong, Yuseong-gu, Daejeon (Korea, Republic of); Rhee, Kyong Yop [Industrial Liaison Research Institute, Department of Mechanical Engineering, College of Engineering, Kyung Hee University, Yongin (Korea, Republic of); Park, Soo-Jin, E-mail: sjpark@inha.ac.kr [Department of Chemistry, Inha University, 100 Inharo, Nam-gu, Incheon (Korea, Republic of)

    2014-07-01

    Pitch is considered a promising low-cost carbon precursor. However, when pitch is pyrolyzed, it forms polycrystalline graphite, which is non-porous, and therefore, not useful for CO{sub 2} adsorption. In this work, pitch was chemically activated to obtain a large specific surface area and micropore volume. Varying weight ratios of KOH (i.e., 0, 1, 2, and 3) were used as the activating agent. The characteristics of the samples were investigated using scanning electron microscopy (SEM), N{sub 2}/77 K adsorption isotherms, and X-ray diffraction (XRD). The CO{sub 2} adsorption performance was studied by isothermal adsorption/desorption measurements. The results showed that an increase in specific surface areas and total pore volumes of pitch-based nanoporous carbons, resulted in an enhancement of CO{sub 2} adsorption capacity. - Graphical abstract: This is the surface morphologies of pitch precursor and pitch-derived activated carbon (AC-2). - Highlights: • Pitch is considered a promising low-cost carbon precursor. • Specific surface area: 1442 m{sup 2}/g and micropore volume: 0.504 cm{sup 3}/g. • CO{sub 2} adsorption capacity showed 203 mg/g (@ RT/1 bar)

  20. High Pressure Adsorption Isotherm of CO2 on Activated Carbon using Volumetric Method

    Directory of Open Access Journals (Sweden)

    Awaludin Martin

    2011-05-01

    Full Text Available Adsorption system is ones of the most effective methods for CO2 separating with other substances that produced from the burning of fossil fuels. In the design for that application, beside of characteristics of porous material (adsorbent data, CO2 adsorption data on the adsorbent (kinetic and thermodynamic are also needed. The aim of this research is resulting isothermal adsorption data at pressures up to 3.5 MPa by indirect methods (volumetric method at isothermal temperature of 300, 308, 318 and 338 K. Adsorbent that used in this research is activated carbon made from East of Kalimantan coals by physical activation method (CO2 which is the surface area of activated carbon is 668 m2/g and pore volume is 0.47 mL/g. Carbon dioxide (CO2 that used in this research is high purity carbon dioxide with a purity of 99.9%. Data from the experiment results then correlated using the Langmuir and Toth equations model. The results showed that the maximum adsorption capacity is 0.314 kg/kg at 300 K and 3384.69 kPa. The results of regression of experiment data using Langmuir and Toth models were 3.4% and 1.7%.

  1. CO{sub 2}MPARE. CO2 Model for Operational Programme Assessment in EU Regions. Improved carbon management with EU Regional Policy. Final Report

    Energy Technology Data Exchange (ETDEWEB)

    Hekkenberg, M. [ECN Policy Studies, Amsterdam (Netherlands); Schram, J. [Energies Demain, Montreuil Sous Bois (France); Amerighi, O. [Italian National Agency for New Technologies, Energy and Sustainable Economic Development ENEA, Rome (Italy); Keppo, I. [University College London UCL, London (United Kingdom); Papagianni, S. [Centre for Renewable Energy Sources and Saving CRES, Pikermi Attiki (Greece); Ten Donkelaar, M. [ENVIROS, Prague (Czech Republic)

    2013-03-15

    The CO2MPARE model supports national and regional authorities in making balanced decisions for their investment portfolio under their regional development programmes, in particular under their Operational Programmes of EU Regional Policy. The EU's climate objectives require that investments across the EU are channeled towards low-carbon development. The carbon impacts of investments should therefore be seriously considered in the decision making process of regional development programmes. The CO2MPARE model informs national and regional authorities on the impacts that the investments under various Operational Programmes can have in terms of CO2 emissions. Knowing which investments lead either to additional emissions or rather to emission reductions, and what the overall impact of a programme is, represents the first step towards investment decisions that have decarbonisation co-benefits. CO2MPARE estimates the combined carbon impact of all activities that take place under a programme, and provides insights into the relative contributions of the different themes. Through its high aggregation level, it allows comparison of investment scenarios rather than individual projects. As such, it aims to support informed decisions on investment strategies rather than project investment decisions. In doing so, it also helps to build and develop a 'carbon culture' within the authorities directly or indirectly in charge of managing Regional Policy Operational Programmes. The model is primarily aimed at Operational Programmes co-financed by the European Regional Development Fund (ERDF)

  2. 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.

  3. RISING ATMOSPHERIC CO2 AND CARBON SEQUESTRATION IN FORESTS

    Science.gov (United States)

    Rising CO2 concentrations in the Earth's atmosphere could alter Earth's climate system, but it is thought that higher concentrations may improve plant growth by way of the fertilization effect. Forests, an important part of the Earth's carbon cycle, are postulated to sequester a...

  4. CO2-Induced Changes in Wheat Grain Composition: Meta-Analysis and Response Functions

    Directory of Open Access Journals (Sweden)

    Malin C. Broberg

    2017-04-01

    Full Text Available Elevated carbon dioxide (eCO2 stimulates wheat grain yield, but simultaneously reduces protein/nitrogen (N concentration. Also, other essential nutrients are subject to change. This study is a synthesis of wheat experiments with eCO2, estimating the effects on N, minerals (B, Ca, Cd, Fe, K, Mg, Mn, Na, P, S, Zn, and starch. The analysis was performed by (i deriving response functions to assess the gradual change in element concentration with increasing CO2 concentration, (ii meta-analysis to test the average magnitude and significance of observed effects, and (iii relating CO2 effects on minerals to effects on N and grain yield. Responses ranged from zero to strong negative effects of eCO2 on mineral concentration, with the largest reductions for the nutritionally important elements of N, Fe, S, Zn, and Mg. Together with the positive but small and non-significant effect on starch concentration, the large variation in effects suggests that CO2-induced responses cannot be explained only by a simple dilution model. To explain the observed pattern, uptake and transport mechanisms may have to be considered, along with the link of different elements to N uptake. Our study shows that eCO2 has a significant effect on wheat grain stoichiometry, with implications for human nutrition in a world of rising CO2.

  5. Isotopic and Geochemical Signatures of Melgaco CO{sub 2} Rich Cold Mineralwaters, NW Portugal

    Energy Technology Data Exchange (ETDEWEB)

    Carreira, P. M.; Nunes, D. [Instituto Tecnologico e Nuclear, Unidade de Ciencias Quimicas e Radiofarmaceuticas, Sacavem (Portugal); Marques, J. M. [Instituto Superior Tecnico, Universidade Tecnica de Lisboa, Lisbon (Portugal); Carvalho, M. R. [Universidade de Lisboa, Faculdade de Ciencias, Departamento de Geologia, Lisbon (Portugal); Antunes da Silva, M. [UNICER Bebidas, S.A, S. Mamede de Infesta (Portugal)

    2013-07-15

    The isotopic and chemical compositions of CO{sub 2} rich mineral waters found in the NW of Portugal were investigated. These mineral waters are mainly related to granitic and granodioritic rocks. Based on their chemical composition, two water types are distinguished (Ca-HCO{sub 3} and Ca-Na-HCO{sub 3}), indicating different underground flow paths. Through comparison with local shallow groundwaters, water chemistry indicates that the Melgaco mineral waters evolved through water-rock interaction with the hosted rocks. Stable isotope data indicates the meteoric origin of these CO{sub 2} rich mineral waters, being recharged from about 480 up to 730 m a.s.l. Considering the {delta}{sup 18}O, {delta}{sup 2}H and the hydrochemical data, no indication of mixing seems to occur between the shallow and deep groundwater systems. The {delta}{sup 13}C determinations carried out on TDIC of the CO{sub 2} rich mineral waters point to the hypothesis of methanogenesis (upper mantle CH{sub 4} source) within the system, leading to {sup 13}C enrichment. The negligible {sup 14}C content ({approx} 2 pMC) also indicates a mantle derived carbon source for the groundwater system. (author)

  6. Exploring biotic vs. abiotic controls on syngenetic carbonate and clay mineral precipitation

    Science.gov (United States)

    Nascimento, Gabriela S.; McKenzie, Judith A.; Martinez Ruiz, Francisca; Bontognali, Tomaso R. R.; Vasconcelos, Crisogono

    2016-04-01

    A possible syngenetic relationship between carbonate and clay mineral precipitation has been reported for sedimentary rocks deposited in both lacustrine and marine sedimentary environments throughout the geological record. In particular, the mineral dolomite is often found associated with Mg-rich clays, such as stevensite. It is notable that this carbonate/clay association has been recorded in numerous samples taken from modern dolomite precipitating environments; for example, the Coorong lakes, South Australia, coastal sabkhas, Abu Dhabi, UAE and coastal hypersaline lagoons (Lagoa Vermelha and Brejo do Espinho) east of Rio de Janeiro, Brazil. An HRTEM study of samples from these three locations indicates a possible physical/chemical association between the Ca-dolomite and Mg-rich clays, demonstrating a probable co-precipitation. To test this hypothesis, we have conducted a series of biotic and abiotic laboratory experiments. If this syngenesis actually occurs in nature, what, if any, are the biogeochemical processes controlling these precipitation reactions? Our experiments were designed to determine the extent of the biotic versus abiotic component influencing the mineral precipitation and, in the case of a biotic influence, to understand the mechanism through which microorganisms might mediate the formation of clay minerals. The experiments were carried out in the Geomicrobiology Laboratory of ETH Zürich using cultures of living microbes and artificial organic compounds that simulate functional groups present in natural biofilms formed under both aerobic and anaerobic conditions. In addition, pure inorganic experiments were designed to understand possible physico-chemical conditions for diagenetic processes that could induce dissolution of Mg-carbonates and precipitation of Mg-rich clays. Our results show a remarkable biotic influence during the formation of clay minerals. Specifically, extracellular polymeric substances (EPS), released by microbes in their

  7. Is it efficient to co-compost and co-vermicompost green waste with biochar and/or clay to reduce CO2 emissions? A short-term laboratory experiment on (vermi)composts with additives.

    Science.gov (United States)

    Barthod, Justine; Rumpel, Cornélia; Paradelo, Remigio; Dignac, Marie-France

    2016-04-01

    Intensive farming practices can lead to a depletion of soil organic matter, negatively impacting important soil properties such as structural stability, fertility and C storage. The addition of organic amendments such as compost and vermicompost, rich in carbon, helps maintaining soil organic matter levels or restoring degraded soils. Composting and vermicomposting are based on stabilization of organic matter through the mineralization of easily decomposable organic matter compounds, therefore releasing greenhouse gases, including CO2. The aim of this study was to evaluate the global potential reduction of such emissions by the use of additives (2:1 clay and/or biochar): during (vermi)composting processes and after use of the final products as soil amendments. We hypothesized that the interactions between the additives and organic matter may lead to carbon stabilization and that such interactions may be enhanced by the presence of worms (Eisenia). We added in different proportions clay (25% or 50%), biochar (10%) and a mixture of biochar (10%) with clay (25%) to pre-composted green waste. The CO2 emissions of the composting and vermicomposting processes were measured during 21 days. After that, the amendments were added to a loamy cambisol soil and the CO2 emissions were monitored during 30 days of a laboratory experiment. The most efficient treatments in terms of reducing global CO2 emissions were the co-vermicomposting process with 25% clay followed by co-composting with 50% clay and with 10% biochar plus 25% clay. In this treatment (vermicompost with 25% clay), the carbon emissions were decreased by up to 44% compared to regular compost. Addition of biochar reduced CO2 emissions only during composting. Co-composting with biochar could be a promising avenue to limit global CO2 emissions whereas in presence of worms clay additions are better suited. These findings suggest that the presence of worms increased the formation of organo-mineral associations and thus C

  8. Characterization of Qatar's surface carbonates for CO2 capture and thermochemical energy storage

    Science.gov (United States)

    Kakosimos, Konstantinos E.; Al-Haddad, Ghadeer; Sakellariou, Kyriaki G.; Pagkoura, Chrysa; Konstandopoulos, Athanasios G.

    2017-06-01

    Samples of surface carbonates were collected from three different areas of the Qatar peninsula. We employed material characterization techniques to examine the morphology and composition of the samples, while their CO2 capture capacity was assessed via multiple successive calcination-carbonation cycles. Our samples were mainly calcite and dolomite based. Calcite samples showed higher initial capacity of around 11 mmol CO2 g-1 which decayed rapidly to less than 2 mmol CO2 g-1. On the other hand, dolomite samples showed an excellent stability (˜15 cycles) with a capacity of 6 mmol CO2 g-1. The performance of the dolomite samples is better compared to other similar natural samples, from literature. A promising result for future studies towards improving their performance by physical and chemical modification.

  9. 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

  10. Assessment of the role of micropore size and N-doping in CO2 capture by porous carbons.

    Science.gov (United States)

    Sevilla, Marta; Parra, Jose B; Fuertes, Antonio B

    2013-07-10

    The role of micropore size and N-doping in CO2 capture by microporous carbons has been investigated by analyzing the CO2 adsorption properties of two types of activated carbons with analogous textural properties: (a) N-free carbon microspheres and (b) N-doped carbon microspheres. Both materials exhibit a porosity made up exclusively of micropores ranging in size between micropores with a size below 0.8 nm. It was also observed that the CO2 capture capacities of undoped and N-doped carbons are analogous which shows that the nitrogen functionalities present in these N-doped samples do not influence CO2 adsorption. Taking into account the temperature invariance of the characteristic curve postulated by the Dubinin theory, we show that CO2 uptakes can be accurately predicted by using the adsorption data measured at just one temperature.

  11. Superior capture of CO2 achieved by introducing extra-framework cations into N-doped microporous carbon

    KAUST Repository

    Zhao, Yunfeng

    2012-12-21

    We designed and prepared a novel microporous carbon material (KNC-A-K) for selective CO2 capture. The combination of a high N-doping concentration (>10 wt %) and extra-framework cations, which were introduced into carbonaceous sorbents for the first time, endowed KNC-A-K with exceptional CO2 adsorption capabilities, especially at low pressures. Specifically, KNC-A-K exhibited CO2 uptake of 1.62 mmol g -1 at 25 C and 0.1 bar, far exceeding the CO2 adsorption capability of most reported carbon material to date. Single component adsorption isotherms indicated that its CO2/N2 selectivity was 48, which also significantly surpasses the selectivity of conventional carbon materials. Furthermore, breakthrough experiments were conducted to evaluate the CO2 separation capability of KNC-A-K on CO2/N2 (10:90 v/v) mixtures under kinetic flow conditions, and the obtained CO 2/N2 selectivity was as high as 44, comparable to that predicted from equilibrium adsorption data. Upon facile regeneration, KNC-A-K showed constant CO2 adsorption capacity and selectivity during multiple mixed-gas separation cycles. Its outstanding low-pressure CO 2 adsorption ability makes KNC-A-K a promising candidate for selective CO2 capture from flue gas. Theoretical calculations indicated that K+ ions play a key role in promoting CO2 adsorption via electrostatic interactions. In addition, we found that HCl molecules anchored in N-doped carbon have a similar promotion effect on CO 2 adsorption, which contradicts the conventional wisdom that the neutralization of basic sites by acids diminishes the adsorption of acidic CO2 gas. © 2012 American Chemical Society.

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

    Science.gov (United States)

    Han, Y.; Tokunaga, T. K.

    2012-12-01

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

  13. Microbe-driven turnover offsets mineral-mediated storage of soil carbon under elevated CO2

    Science.gov (United States)

    Benjamin N. Sulman; Richard P. Phillips; A. Christopher Oishi; Elena Shevliakova; Stephen W. Pacala

    2014-01-01

    The sensitivity of soil organic carbon (SOC) to changing environmental conditions represents a critical uncertainty in coupled carbon cycle–climate models1.Much of this uncertainty arises from our limited understanding of the extent to which root–microbe interactions induce SOC losses (through accelerated decomposition or ‘priming’2) or indirectly promote SOC gains (...

  14. Evidence that an internal carbonic anhydrase is present in 5% CO2-grown and air-grown Chlamydomonas

    International Nuclear Information System (INIS)

    Moroney, J.V.; Togasaki, R.K.; Husic, H.D.; Tolbert, N.E.

    1987-01-01

    Inorganic carbon (C/sub i/) uptake was measured in wild-type cells of Chlamydomonas reinhardtii, and in cia-3, a mutant strain of C. reinhardtii that cannot grow with air levels of CO 2 . Both air-grown cells, that have a CO 2 concentrating system, and 5% CO 2 -grown cells that do not have this system, were used. When the external pH was 5.1 or 7.3, air-grown, wild-type cells accumulated inorganic carbon (C/sub i/) and this accumulation was enhanced when the permeant carbonic anhydrase inhibitor, ethoxyzolamide, was added. When the external pH was 5.1, 5% CO 2 -grown cells also accumulated some C/sub i/, although not as much as air-grown cells and this accumulation was stimulated by the addition of ethoxyzolamide. At the same time, ethoxyzolamide inhibited CO 2 fixation by high CO 2 -grown, wild-type cells at both pH 5.1 and 7.3. These observations imply that 5% CO 2 -grown, wild-type cells, have a physiologically important internal carbonic anhydrase, although the major carbonic anhydrase located in the periplasmic space is only present in air-grown cells. Inorganic carbon uptake by cia-3 cells supported this conclusion. This mutant strain, which is thought to lack an internal carbonic anhydrase, was unaffected by ethoxyzolamide at pH 5.1. Other physiological characteristics of cia-3 resemble those of wild-type cells that have been treated with ethoxyzolamide. It is concluded that an internal carbonic anhydrase is under different regulatory control than the periplasmic carbonic anhydrase

  15. Carbon dioxide (CO 2 ) utilizing strain database | Saini | African ...

    African Journals Online (AJOL)

    Culling of excess carbon dioxide from our environment is one of the major challenges to scientific communities. Many physical, chemical and biological methods have been practiced to overcome this problem. The biological means of CO2 fixation using various microorganisms is gaining importance because database of ...

  16. Accelerated Carbonation of Steel Slag Compacts: Development of High-Strength Construction Materials

    Energy Technology Data Exchange (ETDEWEB)

    Quaghebeur, Mieke; Nielsen, Peter, E-mail: peter.nielsen@vito.be; Horckmans, Liesbeth [Sustainable Materials Management, VITO, Mol (Belgium); Van Mechelen, Dirk [RECMIX bvba, Genk (Belgium)

    2015-12-17

    Mineral carbonation involves the capture and storage of carbon dioxide in carbonate minerals. Mineral carbonation presents opportunities for the recycling of steel slags and other alkaline residues that are currently landfilled. The Carbstone process was initially developed to transform non-hydraulic steel slags [stainless steel (SS) slag and basic oxygen furnace (BOF) slags] in high-quality construction materials. The process makes use of accelerated mineral carbonation by treating different types of steel slags with CO{sub 2} at elevated pressure (up to 2 MPa) and temperatures (20–140°C). For SS slags, raising the temperature from 20 to 140°C had a positive effect on the CO{sub 2} uptake, strength development, and the environmental properties (i.e., leaching of Cr and Mo) of the carbonated slag compacts. For BOF slags, raising the temperature was not beneficial for the carbonation process. Elevated CO{sub 2} pressure and CO{sub 2} concentration of the feed gas had a positive effect on the CO{sub 2} uptake and strength development for both types of steel slags. In addition, the compaction force had a positive effect on the strength development. The carbonates that are produced in situ during the carbonation reaction act as a binder, cementing the slag particles together. The carbonated compacts (Carbstones) have technical properties that are equivalent to conventional concrete products. An additional advantage is that the carbonated materials sequester 100–150 g CO{sub 2}/kg slag. The technology was developed on lab scale by the optimization of process parameters with regard to compressive strength development, CO{sub 2} uptake, and environmental properties of the carbonated construction materials. The Carbstone technology was validated using (semi-)industrial equipment and process conditions.

  17. Studying biosphere-atmosphere exchange of CO2 through Carbon-13 stable isotopes

    NARCIS (Netherlands)

    Velde, van der I.R.

    2015-01-01

    Summary Thesis ‘Studying biosphere-atmosphere exchange of CO2 through

    carbon-13 stable isotopes’

    Ivar van der Velde

    Making predictions of future climate is difficult, mainly due to large uncertainties in the carbon cycle. The rate at which carbon is stored in the oceans and

  18. Carbonic acid as a reserve of carbon dioxide on icy moons: The formation of carbon dioxide (CO2) in a polar environment

    International Nuclear Information System (INIS)

    Jones, Brant M.; Kaiser, Ralf I.; Strazzulla, Giovanni

    2014-01-01

    Carbon dioxide (CO 2 ) has been detected on the surface of several icy moons of Jupiter and Saturn via observation of the ν 3 band with the Near-Infrared Mapping Spectrometer on board the Galileo spacecraft and the Visible-Infrared Mapping Spectrometer on board the Cassini spacecraft. Interestingly, the CO 2 band for several of these moons exhibits a blueshift along with a broader profile than that seen in laboratory studies and other astrophysical environments. As such, numerous attempts have been made in order to clarify this abnormal behavior; however, it currently lacks an acceptable physical or chemical explanation. We present a rather surprising result pertaining to the synthesis of carbon dioxide in a polar environment. Here, carbonic acid was synthesized in a water (H 2 O)-carbon dioxide (CO 2 ) (1:5) ice mixture exposed to ionizing radiation in the form of 5 keV electrons. The irradiated ice mixture was then annealed, producing pure carbonic acid which was then subsequently irradiated, recycling water and carbon dioxide. However, the observed carbon dioxide ν 3 band matches almost exactly with that observed on Callisto; subsequent temperature program desorption studies reveal that carbon dioxide synthesized under these conditions remains in solid form until 160 K, i.e., the sublimation temperature of water. Consequently, our results suggest that carbon dioxide on Callisto as well as other icy moons is indeed complexed with water rationalizing the shift in peak frequency, broad profile, and the solid state existence on these relatively warm moons.

  19. CO2/N2 Gas Separation Using Nanocomposite Membranes Comprised of Ethylene-Propylene-Diene Monomer/Multi-Walled Carbon Nanotube (EPDM/MWCNT

    Directory of Open Access Journals (Sweden)

    Zeinab Rajabi

    2015-07-01

    Full Text Available Nanocomposite membranes of ethylene-propylene-diene monomer/multiwalled carbon nanotubes (EPDM/MWCNT were prepared by solution casting, solvent evaporation and cross-link technique to be applied in CO2/N2 gas separation. Both simple and functionalized MWCNTs have been used. The effect of incorporated different amounts multiwalled carbon nanotubes (0-4 wt%, of both simple and functionalized types, on the performance of nanocomposite membranes was studied. Fourier transform infrared (FTIR spectroscopy and field emission scanning electron microscopy (FESEM were used to evaluate the structural/morphological observations of nanocomposite membranes. Comparing the FTIR results of pure and functionalized nanotubes confirmed the presence of carboxylic groups on the functional carbon nanotubes. The FESEM images indicated that at low concentrations, carbon nanotube particles were dispersed well in the EPDM matrix, but they formed agglomerates at concentrations beyond 1 wt%. By incorporation of MWCNTs, the mechanicalproperties of nanocomposite membranes including tensile strength, Young's modulus and elongation-at-break considerably were improved. By increasing carbon nanotube loading up to 0.75 wt%, the permeability of both CO2 and N2 and the CO2/N2 selectivity increased. Further loading led to higher permeability of CO2/N2, while the selectivity ofthe system decreased that could be attributed to further agglomeration of carbon nanotube particles. Furthermore, functionalization of carbon nanotubes improved their dispersion and the mechanical properties and gas separation performance of nanocomposite membranes. Through functionalizing of MWCNTs, both the CO2 permeability and CO2/N2 selectivity of the optimum membrane (0.75 wt% MWCNTs increased from 37.95 and 18.03 Barrer to 57.57 and 23.43 Barrer, respectively. At ambient temperature, by the increase in feed pressure a slight increase in the permeability of both CO2 and N2 gases was observed, while the CO2

  20. Carbon mineralization and carbonate preservation in modern cold-water coral reef sediments on the Norwegian shelf

    Directory of Open Access Journals (Sweden)

    L. M. Wehrmann

    2009-04-01

    Full Text Available Cold-water coral ecosystems are considered hot-spots of biodiversity and biomass production and may be a regionally important contributor to carbonate production. The impact of these ecosystems on biogeochemical processes and carbonate preservation in associated sediments were studied at Røst Reef and Traenadjupet Reef, two modern (post-glacial cold-water coral reefs on the Mid-Norwegian shelf. Sulfate and iron reduction as well as carbonate dissolution and precipitation were investigated by combining pore-water geochemical profiles, steady state modeling, as well as solid phase analyses and sulfate reduction rate measurements on gravity cores of up to 3.25 m length. Low extents of sulfate depletion and dissolved inorganic carbon (DIC production, combined with sulfate reduction rates not exceeding 3 nmol S cm−3 d−1, suggested that overall anaerobic carbon mineralization in the sediments was low. These data showed that the coral fragment-bearing siliciclastic sediments were effectively decoupled from the productive pelagic ecosystem by the complex reef surface framework. Organic matter being mineralized by sulfate reduction was calculated to consist of 57% carbon bound in CH2O groups and 43% carbon in -CH2- groups. Methane concentrations were below 1 μM, and failed to support the hypothesis of a linkage between the distribution of cold-water coral reefs and the presence of hydrocarbon seepage. Reductive iron oxide dissolution linked to microbial sulfate reduction buffered the pore-water carbonate system and inhibited acid-driven coral skeleton dissolution. A large pool of reactive iron was available leading to the formation of iron sulfide minerals. Constant pore-water Ca2+, Mg2+ and Sr2+ concentrations in most cores and decreasing Ca2+ and Sr2+ concentrations with depth in core 23–18 GC indicated diagenetic carbonate precipitation. This was

  1. Quantitative spectrographic determination of zirconium minerals

    International Nuclear Information System (INIS)

    Rocal Adell, M.; Alvarez Gonzalez, F.; Fernandez Cellini, R.

    1958-01-01

    The method described in the following report permits the quantitative determination of zirconium in minerals and rocks in a 0,02-100% of ZrO 2 concentration rate. The excitation is carried out by a 10 ampere continuous current arc among carbon electrodes, and placing the sample in a crater of 2 mm depth. For low concentrations a dilution of the sample with the same weight as its own in carbon powder and with 1/25 of its weight of Co 3 O 4 (internal patron) is carried out. Line Zr 2571,4, Co 2585,3 and Co 2587,2 are used. (Author) 6 refs

  2. Ammonia-treated porous carbon derived from ZIF-8 for enhanced CO{sub 2} adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Ma, Xiancheng [School of Energy Science and Engineering, Central South University, Changsha 410083, Hunan (China); Li, Liqing, E-mail: liqingli@hotmail.com [School of Energy Science and Engineering, Central South University, Changsha 410083, Hunan (China); Wang, Shaobin [Department of Chemical Engineering, Curtin University, GPO Box U1987, Perth 6845, WA (Australia); Lu, Mingming [Department of Civil and Environmental Engineering, University of Cincinnati, Cincinnati, OH 45221 (United States); Li, Hailong; Ma, Weiwu [School of Energy Science and Engineering, Central South University, Changsha 410083, Hunan (China); Keener, Tim C. [Department of Civil and Environmental Engineering, University of Cincinnati, Cincinnati, OH 45221 (United States)

    2016-04-30

    Graphical abstract: The role of nitrogen species in increasing CO{sub 2} adsorption capacity has been explained with the mechanisms of base–acid interaction, as well as hydrogen bonds interaction. - Highlights: • A porous carbon (ZC) was prepared at 900 °C using ZIF-8 as a solid template for CO{sub 2} adsorption. • The ZC was further treated by ammonia functionalization to improve CO{sub 2} uptake. • The detailed interaction mechanism between N-containing groups and CO{sub 2} molecules is elucidated. - Abstract: A porous carbon (ZC) was prepared at 900 °C using zeolitic imidazolate framework-8 (ZIF-8) as a solid template for CO{sub 2} adsorption. The ZC was further treated by ammonia functionalization to improve CO{sub 2} uptake. The textural and surface characteristics of ZC samples were determined by X-ray diffraction (XRD), N{sub 2} adsorption, Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). It was revealed that ammonia treatment at 600 °C considerably enhanced the specific surface area and N-content of ZC. However, the pyrrolic-N group was decreased, yet the pyridinic-N group was increased with an increased temperature. The pyrrolic-N significantly enhanced CO{sub 2} adsorption. The ammonia treatment, on the one hand, increases the alkalinity of ZC sample and the base–acid interaction between N-containing functional groups with CO{sub 2}. On the other hand, the ammonia treatment increased pyrrolic-N group (NH) into carbon surface facilitating the hydrogen-bonding interactions between proton of pyrrolic-N and CO{sub 2} molecules.

  3. Is carbon / CO2 taxes implementation timely for electricity and heat generation in Romania ?

    International Nuclear Information System (INIS)

    Tutuianu, O.; Fulger, E.D.; Vieru, A.; Feher, M.

    1996-01-01

    Lately, carbon / CO 2 taxes are very much discussed in Europe and in many countries of the world as economic and financial instruments for reducing the CO 2 emissions. Some countries have already introduced such taxes while in other countries or international organisations they are under study, especially concerning the moment, the way of implementation and the amount of taxes. CO 2 emissions in Romania, in absolute and specific values (per capita, per kWh equivalent) are lower than in other countries. This can be justified by the low level of electricity and heat output owing to the recent economic restructuring and by the energy sector characteristics: natural gas major contribution, hydroelectric power, cogeneration and nuclear power implementation. We can also mention, as a positive factor, the CO 2 absorption potential of the Romanian forests. Carbon / CO 2 taxes introduction has severe economic and social impact, such as: domestic coal extraction blockage, increase in the electricity and heat prices, decrease of Romanian export products competitiveness and reduction of population standard of living. Therefore, the authors are considering that carbon / CO 2 taxes introduction is not timely by the year 2000 for the Romanian electricity and heat generation. (author). 3 figs. 2 tabs. 10 refs

  4. Determination of the equation parameters of carbon flow curves and estimated carbon flow and CO2 emissions from broiler production.

    Science.gov (United States)

    Henn, J D; Bockor, L; Borille, R; Coldebella, A; Ribeiro, A M L; Kessler, A M

    2015-09-01

    The objective of this study was to determine the equation parameters of carbon (i.e., C) flow curves and to estimate C flow and carbon dioxide (i.e., CO2) emissions from the production of 1- to 49-day-old broilers from different genetic strains. In total, 384 1-day-old chicks were used, distributed into 4 groups: high-performance males (Cobb-M) and females (Cobb-F), and intermediate-performance males (C44-M) and females (C44-F), with 6 replicates/treatment according to a completely randomized study design. Carbon intake and retention were calculated based on diet and body C composition, and expired C was stoichiometrically estimated as digestible C intake-C retention-C in the urine. Litter C emission was estimated as initial litter C+C in the excreta-final litter C. Carbon flow curves were determined fitting data by nonlinear regression using the Gompertz function. Expired CO2 was calculated based on expired C. The applied nonlinear model presented goodness-of-fit for all responses (R2>0.99). Carbon dioxide production was highly correlated with growth rate. At 42 d age, CO2 expiration (g/bird) was 3,384.4 for Cobb-M, 2,947.9 for Cobb-F, 2,512.5 for C44-M, and 2185.1 for C44-F. Age also significantly affected CO2 production: to achieve 2.0 kg BW, CO2 expiration (g/bird) was 1,794.3 for Cobb-M, 2,016.5 for Cobb-F, 2617.7 for C44-M, and 3,092.3 for C44-F. The obtained equations present high predictability to estimate individual CO2 emissions in strains of Cobb and C44 broilers of any weight, or age, reared between 1 and 49 d age. © 2015 Poultry Science Association Inc.

  5. Assessing the use of composts from multiple sources based on the characteristics of carbon mineralization in soil.

    Science.gov (United States)

    Zhang, Xu; Zhao, Yue; Zhu, Longji; Cui, Hongyang; Jia, Liming; Xie, Xinyu; Li, Jiming; Wei, Zimin

    2017-12-01

    In order to improve soil quality, reduce wastes and mitigate climate change, it is necessary to understand the balance between soil organic carbon (SOC) accumulation and depletion under different organic waste compost amended soils. The effects of proportion (5%, 15%, 30%), compost type (sewage sludge (SS), tomato stem waste (TSW), municipal solid waste (MSW), kitchen waste (KW), cabbage waste (CW), peat (P), chicken manure (CM), dairy cattle manure (DCM)) and the black soil (CK). Their initial biochemical composition (carbon, nitrogen, C:N ratio) on carbon (C) mineralization in soil amended compost have been investigated. The CO 2 -C production of different treatments were measured to indicate the levels of carbon (C) mineralization during 50d of laboratory incubation. And the one order E model (M1E) was used to quantify C mineralization kinetics. The results demonstrated that the respiration and C mineralization of soil were promoted by amending composts. The C mineralization ability increased when the percentage of compost added to the soil also increased and affected by compost type in the order CM>KW, CW>SS, DCM, TSW>MSW, P>CK at the same amended level. Based on the values of C 0 and k 1 from M1E model, a management method in agronomic application of compost products to the precise fertilization was proposed. The SS, DCM and TSW composts were more suitable in supplying fertilizer to the plant. Otherwise, The P and MSW composts can serve the purpose of long-term nutrient retention, whereas the CW and KW composts could be used as soil remediation agent. Copyright © 2017 Elsevier Ltd. All rights reserved.

  6. The review of recent carbonate minerals processing technology

    Science.gov (United States)

    Solihin

    2018-02-01

    Carbonate is one of the groups of minerals that can be found in relatively large amount in the earth crust. The common carbonate minerals are calcium carbonate (calcite, aragonite, depending on its crystal structure), magnesium carbonate (magnesite), calcium-magnesium carbonate (dolomite), and barium carbonate (barite). A large amount of calcite can be found in many places in Indonesia such as Padalarang, Sukabumi, and Tasikmalaya (West Java Provence). Dolomite can be found in a large amount in Gresik, Lamongan, and Tuban (East Java Provence). Magnesite is quite rare in Indonesia, and up to the recent years it can only be found in Padamarang Island (South East Sulawesi Provence). The carbonate has been being exploited through open pit mining activity. Traditionally, calcite can be ground to produce material for brick production, be carved to produce craft product, or be roasted to produce lime for many applications such as raw materials for cement, flux for metal smelting, etc. Meanwhile, dolomite has traditionally been used as a raw material to make brick for local buildings and to make fertilizer for coconut oil plant. Carbonate minerals actually consist of important elements needed by modern application. Calcium is one of the elements needed in artificial bone formation, slow release fertilizer synthesis, dielectric material production, etc. Magnesium is an important material in automotive industry to produce the alloy for vehicle main parts. It is also used as alloying element in the production of special steel for special purpose. Magnesium oxide can be used to produce slow release fertilizer, catalyst and any other modern applications. The aim of this review article is to present in brief the recent technology in processing carbonate minerals. This review covers both the technology that has been industrially proven and the technology that is still in research and development stage. One of the industrially proven technologies to process carbonate mineral is

  7. Effect of carbonation temperature on CO_2 adsorption capacity of CaO derived from micro/nanostructured aragonite CaCO_3

    International Nuclear Information System (INIS)

    Hlaing, Nwe Ni; Sreekantan, Srimala; Hinode, Hirofumi; Kurniawan, Winarto; Thant, Aye Aye; Othman, Radzali; Mohamed, Abdul Rahman; Salime, Chris

    2016-01-01

    Recent years, CaO-based synthetic materials have been attracted attention as potential adsorbents for CO_2 capture mainly due to their high CO_2 adsorption capacity. In this study, micro/nanostructured aragonite CaCO_3 was synthesized by a simple hydrothermal method with using polyacrylamide (PAM). The structural, morphological and thermal properties of the synthesized sample were investigated by X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM) and thermogravimetry analysis (TG-DTA). The XRD and FESEM results showed that the obtained sample was aragonite CaCO_3 with aggregated nanorods and microspheres composed of nanorods. A TG-DTA apparatus with Thermoplus 2 software was used to investigate the effect of carbonation temperature on the CO_2 adsorption capacity of CaO derived from aragonite CaCO_3 sample. At 300 °C, the sample reached the CO_2 adsorption capacity of 0.098 g-CO_2/g-adsorbent, whereas the sample achieved the highest capacity of 0.682 g-CO_2/g-adsorbent at 700 °C. The results showed that the carbonation temperature significantly influenced on the CO_2 adsorption capacity of the CaO derived from aragonite CaCO_3.

  8. Second Generation CO2 FEP Analysis: CASSIF - Carbon Storage Scenario Identification Framework

    NARCIS (Netherlands)

    Yavuz, F.; Tilburg, T. van; David, P.; Spruijt, M.; Wildenborg, T.

    2009-01-01

    Carbon dioxide Capture and Storage (CCS) is a promising contribution to reduce further increase of atmospheric CO2 emissions from fossil fuels. The CCS concept anticipates that large amounts of CO2 are going to be stored in the subsurface for the long term. Since CCS is a rather new technology,

  9. Hierarchical saturation of soil carbon pools near a natural CO2 spring

    NARCIS (Netherlands)

    Kool, D.M.; Chung, H.; Tate, K.R.; Ross, D.J.; Newton, P.C.D.; Six, J.

    2007-01-01

    Soil has been identified as a possible carbon (C) sink to mitigate increasing atmospheric CO2 concentration. However, several recent studies have suggested that the potential of soil to sequester C is limited and that soil may become saturated with C under increasing CO2 levels. To test this concept

  10. CAPTURING EXHAUST CO2 GAS USING MOLTEN CARBONATE FUEL CELLS

    Directory of Open Access Journals (Sweden)

    Prateek Dhawan

    2016-03-01

    Full Text Available Carbon dioxide is considered as one of the major contenders when the question of greenhouse effect arises. So for any industry or power plant it is of utmost importance to follow certain increasingly stringent environment protection rules and laws. So it is significant to keep eye on any possible methods to reduce carbon dioxide emissions in an efficient way. This paper reviews the available literature so as to try to provide an insight of the possibility of using Molten Carbonate Fuel Cells (MCFCs as the carbon capturing and segregating devices and the various factors that affect the performance of MCFCs during the process of CO2 capture.

  11. The effect of carbon tax on per capita CO2 emissions

    International Nuclear Information System (INIS)

    Lin Boqiang; Li Xuehui

    2011-01-01

    As the most efficient market-based mitigation instrument, carbon tax is highly recommended by economists and international organizations. Countries like Denmark, Finland, Sweden, Netherlands and Norway were the first adopters of carbon tax and as such, research on the impacts and problems of carbon tax implementation in these countries will provide great practical significance as well as caution for countries that are to levy the tax. Different from the existing studies that adopt the model simulation approaches, in this article, we comprehensively estimate the real mitigation effects of the five north European countries by employing the method of difference-in-difference (DID). The results indicate that carbon tax in Finland imposes a significant and negative impact on the growth of its per capita CO 2 emissions. Meanwhile, the effects of carbon tax in Denmark, Sweden and Netherlands are negative but not significant. The mitigation effects of carbon tax are weakened due to the tax exemption policies on certain energy intensive industries in these countries. Notwithstanding, in Norway, as the rapid growth of energy products drives a substantial increase of CO 2 emissions in oil drilling and natural gas exploitation sectors, carbon tax actually has not realized its mitigation effects. - Highlights: → DID method is employed to test the real mitigation effect of carbon tax. → Carbon tax in Finland imposes a significant and negative impact. → The effects of carbon tax in other four countries are limited. → Tax exemption or tax relief is the main reason of limited effects. → High tax rates and recycling the revenue contribute to emission reduction.

  12. Synthesis and photocatalytic CO2 reduction performance of Cu2O/Coal-based carbon nanoparticle composites

    Science.gov (United States)

    Dedong, Zhang; Maimaiti, Halidan; Awati, Abuduheiremu; Yisilamu, Gunisakezi; Fengchang, Sun; Ming, Wei

    2018-05-01

    The photocatalytic reduction of CO2 into hydrocarbons provides a promising approach to overcome the challenges of environmental crisis and energy shortage. Here we fabricated a cuprous oxide (Cu2O) based composite photocatalyst consisting of Cu2O/carbon nanoparticles (CNPs). To prepare the CNPs, coal samples from Wucaiwan, Xinjiang, China, were first treated with HNO3, followed by hydrogen peroxide (H2O2) oxidation to strip nanocrystalline carbon from coal. After linking with oxygen-containing group such as hydroxyl, coal-based CNPs with sp2 carbon structure and multilayer graphene lattice structure were synthesized. Subsequently, the CNPs were loaded onto the surface of Cu2O nanoparticles prepared by in-situ reduction of copper chloride (CuCl2·2H2O). The physical properties and chemical structure of the Cu2O/CNPs as well as photocatalytic activity of CO2/H2O reduction into CH3OH were measured. The results demonstrate that the Cu2O/CNPs are composed of spherical particles with diameter of 50 nm and mesoporous structure, which are suitable for CO2 adsorption. Under illumination of visible light, electron-hole pairs are generated in Cu2O. Thanks to the CNPs, the fast recombination of electron-hole pairs is suppressed. The energy gradient formed on the surface of Cu2O/CNPs facilitates the efficient separation of electron-hole pairs for CO2 reduction and H2O oxidation, leading to enhanced photocatalytic activity.

  13. Carbon Dioxide Utilization (CO2U) ICEF Roadmap 2.0. Draft October 2017

    Energy Technology Data Exchange (ETDEWEB)

    Sandalow, D; Aines, R; Friedmann, J; McCormick, C; McCoy, S

    2017-10-02

    Last year, experts from CO2 Sciences, Columbia University and Valence Strategic came together to develop a roadmap. That document, Carbon Dioxide Utilization ICEF Roadmap 1.0, released at the UNFCCC Marrakesh Climate Change Conference in 2016, surveyed the commercial and technical landscape of CO2 conversion and use. The document provided extensive background and analysis and has helped to provide a foundation for additional studies, including this one.This roadmap is meant to complement and expand upon the work of its predecessor. Based in part on a workshop at Columbia University’s Center on Global Energy Policy in July 2017, it explores three distinct categories of CO2-based products, the technologies that can be harnessed to convert CO2 to these products, and the associated research and development needs. It also explores the complicated topic of life cycle analysis—critically important when considering the climate impacts of CO2 conversion and use—as well as policy tools that could be used to promote CO2-based products.

  14. 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

    settings such as the carbonate reservoirs in the North Sea. The final aim of our project is to find out how to control the evolution of petrophysical parameters during CO2 injection using an optimal combination of flow rate, injection pressure and chemical composition of the influent. The first step...... 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...

  15. CO{sub 2} capture using fly ash-derived activated carbons impregnated with low molecular mass amines

    Energy Technology Data Exchange (ETDEWEB)

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

    2005-07-01

    Two different approaches to develop high capacity CO{sub 2} sorbents are presented. Firstly, the modification of the surface chemistry of low cost carbons by impregnation with a basic nitrogen-containing polymer (i.e.polyethylenimine) is described. Relatively low molecular mass (MM) amines, namely diethanolamine (DEA, MM 105) and tetraethylenepentaamineacrylonitrile (TEPAN, MM 311) are used to produce high capacity CO{sub 2} sorbents from activated carbons derived from unburned carbon in fly ash, which have low mesoporosities. The CO{sub 2} adsorption capacity and thermal stability of the prepared sorbents was measured as a function of temperature in a thermogravimetric analyser. The results indicate that TEPAN is more effective than DEA; at a temperature of 75{sup o}C, fly ash-derived activated carbons loaded with TEPAN achieved CO{sub 2} adsorption capacities in excess of 5 wt%, which compares fabvourably with the CO{sub 2} absorption capacity of 6.5 wt% achieved with a mesoporous silica loaded with TEPAN, and outperforms fly ash-derived activated carbons loaded with PEI. TEPAN has also been shown to have a higher thermal stability than DEA. The second approach involves the development of high nitrogen content carbon matrix adsorbents by carbonisation and subsequent thermal or chemical activation of a range of materials (polyacrylonitrile, glucose-amine mixtures, melamine and urea/melamine-formaldehyde resins). 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. However, the adsorbent obtained from carbazole-sugar co-pyrolysis, despite the lower amount of N incorporated, shows high CO{sub 2} uptake, up to 9 wt%, probably because the presence of more basic functionalities as determined by XPS analysis. 9 refs., 2 figs.

  16. Susceptibility of Granite Rock to scCO2/Water at 200 degrees C and 250 degrees C

    Energy Technology Data Exchange (ETDEWEB)

    Sugama, T.; Gill, S., Ecker, L., Butcher, T., Warren, J.

    2011-01-01

    Granite rock comprising anorthoclase-type albite and quartz as its major phases and biotite mica as the minor one was exposed to supercritical carbon dioxide (scCO{sub 2})/water at 250 C and 13.78 MPa pressure for 104 hours. For comparison purpose, four other rocks, albite, hornblende, diorite, and quartz, also were exposed. During the exposure of granite, ionic carbonic acid, known as the wet carbonation reactant, preferentially reacted with anorthoclase-type albite and biotite, rather than with quartz. The susceptibility of biotite to wet carbonation was higher than that of anorthoclase-type albite. All the carbonation by-products of anorthoclase-type albite were amorphous phases including Na- and K-carbonates, a kaolinite clay-like compound, and silicon dioxide, while wet carbonation converted biotite into potassium aluminum silicate, siderite, and magnesite in crystalline phases and hydrogen fluoride (HF). Three of these reaction by-products, Na- and K-carbonates and HF, were highly soluble in water. Correspondingly, the carbonated top surface layer, about 1.27 mm thick as carbonation depth, developed porous microstructure with numerous large voids, some of which have a size of {>=} 10 {mu}m, reflecting the erosion of granite by the leaching of these water-soluble reaction by-products. Comparing with this carbonation depth, its depth of other minerals was considerable lower, particularly, for hornblende and diorite with 0.07 and 0.02 mm, while no carbonate compound was detected in quartz. The major factor governing these low carbonation depths in these rocks was the formation of water-insensitive scale-like carbonate by-products such as calcite (CaCO{sub 3}), siderite (FeCO{sub 3}), and magnesite (MgCO{sub 3}). Their formation within the superficial layer of these minerals served as protective barrier layer that inhibits and retards further carbonation of fresh underlying minerals, even if the exposure time was extended. Thus, the coverage by this barrier layer

  17. In situ evidence of mineral physical protection and carbon stabilization revealed by nanoscale 3-D tomography

    Science.gov (United States)

    Weng, Yi-Tse; Wang, Chun-Chieh; Chiang, Cheng-Cheng; Tsai, Heng; Song, Yen-Fang; Huang, Shiuh-Tsuen; Liang, Biqing

    2018-05-01

    An approach for nanoscale 3-D tomography of organic carbon (OC) and associated mineral nanoparticles was developed to illustrate their spatial distribution and boundary interplay, using synchrotron-based transmission X-ray microscopy (TXM). The proposed 3-D tomography technique was first applied to in situ observation of a laboratory-made consortium of black carbon (BC) and nanomineral (TiO2, 15 nm), and its performance was evaluated using dual-scan (absorption contrast and phase contrast) modes. This novel tool was then successfully applied to a natural OC-mineral consortium from mountain soil at a spatial resolution of 60 nm, showing the fine structure and boundary of OC, the distribution of abundant nano-sized minerals, and the 3-D organo-mineral association in situ. The stabilization of 3500-year-old natural OC was mainly attributed to the physical protection of nano-sized iron (Fe)-containing minerals (Fe oxyhydroxides including ferrihydrite, goethite, and lepidocrocite), and the strong organo-mineral complexation. In situ evidence revealed an abundance of mineral nanoparticles, in dense thin layers or nano-aggregates/clusters, instead of crystalline clay-sized minerals on or near OC surfaces. The key working minerals for C stabilization were reactive short-range-order (SRO) mineral nanoparticles and poorly crystalline submicron-sized clay minerals. Spectroscopic analyses demonstrated that the studied OC was not merely in crisscross co-localization with reactive SRO minerals; there could be a significant degree of binding between OC and the minerals. The ubiquity and abundance of mineral nanoparticles on the OC surface, and their heterogeneity in the natural environment may have been severely underestimated by traditional research approaches. Our in situ description of organo-mineral interplay at the nanoscale provides direct evidence to substantiate the importance of mineral physical protection for the long-term stabilization of OC. This high-resolution 3-D

  18. The sensitivity of terrestrial carbon storage to historical climate variability and atmospheric CO2 in the United States

    Science.gov (United States)

    Tian, H.; Melillo, J. M.; Kicklighter, D. W.; McGuire, A. D.; Helfrich, J.

    1999-04-01

    We use the Terrestrial Ecosystem Model (TEM, Version 4.1) and the land cover data set of the international geosphere biosphere program to investigate how increasing atmospheric CO2 concentration and climate variability during 1900 1994 affect the carbon storage of terrestrial ecosystems in the conterminous USA, and how carbon storage has been affected by land-use change. The estimates of TEM indicate that over the past 95years a combination of increasing atmospheric CO2 with historical temperature and precipitation variability causes a 4.2% (4.3Pg C) decrease in total carbon storage of potential vegetation in the conterminous US, with vegetation carbon decreasing by 7.2% (3.2Pg C) and soil organic carbon decreasing by 1.9% (1.1Pg C). Several dry periods including the 1930s and 1950s are responsible for the loss of carbon storage. Our factorial experiments indicate that precipitation variability alone decreases total carbon storage by 9.5%. Temperature variability alone does not significantly affect carbon storage. The effect of CO2 fertilization alone increases total carbon storage by 4.4%. The effects of increasing atmospheric CO2 and climate variability are not additive. Interactions among CO2, temperature and precipitation increase total carbon storage by 1.1%. Our study also shows substantial year-to-year variations in net carbon exchange between the atmosphere and terrestrial ecosystems due to climate variability. Since the 1960s, we estimate these terrestrial ecosystems have acted primarily as a sink of atmospheric CO2 as a result of wetter weather and higher atmospheric CO2 concentrations. For the 1980s, we estimate the natural terrestrial ecosystems, excluding cropland and urban areas, of the conterminous US have accumulated 78.2 Tg C yr1 because of the combined effect of increasing atmospheric CO2 and climate variability. For the conterminous US, we estimate that the conversion of natural ecosystems to cropland and urban areas has caused a 18.2% (17.7Pg C

  19. Carbon Disulfide (CS2) Mechanisms in Formation of Atmospheric Carbon Dioxide (CO2) Formation from Unconventional Shale Gas Extraction and Processing Operations and Global Climate Change.

    Science.gov (United States)

    Rich, Alisa L; Patel, Jay T

    2015-01-01

    Carbon disulfide (CS2) has been historically associated with the production of rayon, cellophane, and carbon tetrachloride. This study identifies multiple mechanisms by which CS2 contributes to the formation of CO2 in the atmosphere. CS2 and other associated sulfide compounds were found by this study to be present in emissions from unconventional shale gas extraction and processing (E&P) operations. The breakdown products of CS2; carbonyl sulfide (COS), carbon monoxide (CO), and sulfur dioxide (SO2) are indirect greenhouse gases (GHGs) that contribute to CO2 levels in the atmosphere. The heat-trapping nature of CO2 has been found to increase the surface temperature, resulting in regional and global climate change. The purpose of this study is to identify five mechanisms by which CS2 and the breakdown products of CS2 contribute to atmospheric concentrations of CO2. The five mechanisms of CO2 formation are as follows: Chemical Interaction of CS2 and hydrogen sulfide (H2S) present in natural gas at high temperatures, resulting in CO2 formation;Combustion of CS2 in the presence of oxygen producing SO2 and CO2;Photolysis of CS2 leading to the formation of COS, CO, and SO2, which are indirect contributors to CO2 formation;One-step hydrolysis of CS2, producing reactive intermediates and ultimately forming H2S and CO2;Two-step hydrolysis of CS2 forming the reactive COS intermediate that reacts with an additional water molecule, ultimately forming H2S and CO2. CS2 and COS additionally are implicated in the formation of SO2 in the stratosphere and/or troposphere. SO2 is an indirect contributor to CO2 formation and is implicated in global climate change.

  20. Post-combustion CO2 capture with activated carbons using fixed bed adsorption

    Science.gov (United States)

    Al Mesfer, Mohammed K.; Danish, Mohd; Fahmy, Yasser M.; Rashid, Md. Mamoon

    2018-03-01

    In the current work, the capturing of carbon dioxide from flue gases of post combustion emission using fixed bed adsorption has been carried out. Two grades of commercial activated carbon (sorbent-1 and sorbent-2) were used as adsorbent. Feed consisting of CO2 and N2 mixture was used for carrying out the adsorption. The influence of bed temperature, feed rate, equilibrium partial pressure and initial % CO2 in feed were considered for analyzing adsorption-desorption process. It was found that the total adsorption-desorption cycle time decreases with increased column temperature and feed rates. The time required to achieve the condition of bed saturation decreases with increased bed temperature and feed rates. The amount of CO2 adsorbed/Kg of the adsorbent declines with increased bed temperature with in studied range for sorbent-1 and sorbent-2. It was suggested that the adsorption capacity of the both the sorbents increases with increased partial pressure of the gas.

  1. Pre injection characterisation and evaluation of CO{sub 2} sequestration potential in the Haizume formation, Niigata basin, Japan; Caracterisation avant injection et evaluation du potentiel de sequestration de CO{sub 2} dans la formation de Haizume, bassin de Niigata, Japon. Modelisation geochimique des interactions eau-mineraux-CO{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Zwingmann, N. [CSIRO Petroleum, ARRC, Bentley, WA (Australia); Mito, S.; Sorai, M.; Ohsumi, T. [RITE, Kyoto (Japan); Zwingmann, N. [Western, Univ. (Australia); Sorai, M. [Mitsubishi Research Institute, Inc. (Japan)

    2005-03-15

    The Research Institute of Innovative Technology for the Earth (RITE) is carrying out a small-scale CO{sub 2} injection field experiment to investigate the feasibility of geological sequestration of CO{sub 2} greenhouse gas in the south-west of Nagaoka City, Niigata Prefecture, Japan. Prior to the injection geochemical reactions caused by CO{sub 2} injections were investigated using the geochemical modelling code (EQ3/6). The injection formation is the sedimentary marine Haizume Formation (Pleistocene) in the Uonuma Group, which is covered by a mud-stone seal. The formation is mainly composed of quartz, plagioclase, feldspar, pyroxene, and clays (smectite, chlorite). The sandstone shows minor consolidation and grain size is medium to coarse sand. The total dissolved solid (TDS) of the formation water is approximately 6100 mg/l and the water contains a high Ca{sup 2+} ({>=} 20% of Na{sup +} concentration). The geochemical model was used for an initial adjustment of the formation water chemistry to the formation conditions and a modelling of the formation water-mineral-CO{sub 2} reactions. The modelling results showed a high reactivity of the minerals in the CO{sub 2} rich environment and high mineral conversion rate within the formation. At the final state, approximately 23 mol of CO{sub 2} were taken into 1 kg of formation water and more than 90% of this was stored within carbonate minerals. In this simulation, some uncertainty is associated with the time scale and a more detailed investigation is planned and will address accurate evaluation. (authors)

  2. Carbon mineralization in mine tailing ponds amended with pig slurries and marble wastes

    Directory of Open Access Journals (Sweden)

    Raul Zornoza

    2012-07-01

    Full Text Available Effective application of organic residues to reclaim soils requires the optimization of the waste management to minimize CO2 emissions and optimize soil C sequestration efficiency. In this study, the short-term effects of pig slurry amendment alone and together with marble waste on organic matter mineralization in two tailing ponds from Cartagena-La Unión Mining District (SE Spain were investigated in a field remediation experiment. The treatments were: marble waste (MW, pig slurry (PS, marble waste + pig slurry (MW+PS, and control. Soil carbon mineralization was determined using a static chamber method with alkali absorption during 70 days. Soil respiration rates in all plots were higher the first days of the experiment owing to higher soil moisture and higher mean air temperature. MW plots followed the same pattern than control plots, with similar respiration rates. The addition of pig slurry caused a significant increase in the respiration rates, although in MW+PS plots, respiration rates were lower than in PS plots. The cumulative quantities of C-CO2 evolved from the pig slurry mineralization were fitted to a first-order kinetic model explaining 90% of the data. This model implies the presence of only one mineralisable pool (C0. The values of the index C0*constant rate/added C were similar for PS plots in both tailing ponds, but lower in the MW+PS treatment, suggesting that the application of marble reduces the degradability of the organic compounds present in the pig slurry. Thus, the application of marble wastes contributes to slow down the loss of organic matter by mineralization.

  3. Effects of functional groups and soluble matrices in fish otolith on calcium carbonate mineralization

    Energy Technology Data Exchange (ETDEWEB)

    Ren Dongni; Li Zhuo; Gao Yonghua; Feng Qingling, E-mail: biomater@mail.tsinghua.edu.c [State Key Laboratory of New Ceramics and Fine Processing, Department of Materials Science and Engineering, Tsinghua University, Beijing 100084 (China)

    2010-10-01

    Calcium carbonate mineralization is significantly influenced by organic matrices in vivo. The effect mainly relies on functional groups in proteins. In order to study the influence of functional groups on calcium carbonate mineralization, -OH, -NH{sub 2} and -COOH groups were grafted onto single crystal silicon chips, and such modified chips were used as substrates in in vitro mineralization experiments. An x-ray photoelectron spectroscopy (XPS) test was conducted to examine the grafting efficiency, and the three groups were successfully grafted. Calcium carbonate mineralization on a modified silicon substrate was examined by a scanning electron microscope (SEM) and x-ray diffraction (XRD), and the results showed that the effects of -OH, -NH{sub 2} and -COOH groups were quite different. Furthermore, a water-soluble protein matrix (WSM) and an acid-soluble protein matrix (ASM) extracted from fish otolith were adsorbed onto the -COOH-modified silicon substrate, and the effects of the protein matrices on calcium carbonate mineralization were studied. The results showed that both WSM and ASM of lapillus could mediate aragonite crystallization, but the size and morphology of the formed crystals were different. The WSM and ASM of asteriscus adsorbed on the silicon substrate had little effect on calcium carbonate mineralization; almost all the crystals were calcite, while both asteriscus WSM and ASM in solution could mediate vaterite crystals, and the morphologies of vaterite crystal aggregates were different.

  4. Effects of functional groups and soluble matrices in fish otolith on calcium carbonate mineralization

    International Nuclear Information System (INIS)

    Ren Dongni; Li Zhuo; Gao Yonghua; Feng Qingling

    2010-01-01

    Calcium carbonate mineralization is significantly influenced by organic matrices in vivo. The effect mainly relies on functional groups in proteins. In order to study the influence of functional groups on calcium carbonate mineralization, -OH, -NH 2 and -COOH groups were grafted onto single crystal silicon chips, and such modified chips were used as substrates in in vitro mineralization experiments. An x-ray photoelectron spectroscopy (XPS) test was conducted to examine the grafting efficiency, and the three groups were successfully grafted. Calcium carbonate mineralization on a modified silicon substrate was examined by a scanning electron microscope (SEM) and x-ray diffraction (XRD), and the results showed that the effects of -OH, -NH 2 and -COOH groups were quite different. Furthermore, a water-soluble protein matrix (WSM) and an acid-soluble protein matrix (ASM) extracted from fish otolith were adsorbed onto the -COOH-modified silicon substrate, and the effects of the protein matrices on calcium carbonate mineralization were studied. The results showed that both WSM and ASM of lapillus could mediate aragonite crystallization, but the size and morphology of the formed crystals were different. The WSM and ASM of asteriscus adsorbed on the silicon substrate had little effect on calcium carbonate mineralization; almost all the crystals were calcite, while both asteriscus WSM and ASM in solution could mediate vaterite crystals, and the morphologies of vaterite crystal aggregates were different.

  5. Effects of functional groups and soluble matrices in fish otolith on calcium carbonate mineralization.

    Science.gov (United States)

    Ren, Dongni; Li, Zhuo; Gao, Yonghua; Feng, Qingling

    2010-10-01

    Calcium carbonate mineralization is significantly influenced by organic matrices in vivo. The effect mainly relies on functional groups in proteins. In order to study the influence of functional groups on calcium carbonate mineralization, -OH, -NH2 and -COOH groups were grafted onto single crystal silicon chips, and such modified chips were used as substrates in in vitro mineralization experiments. An x-ray photoelectron spectroscopy (XPS) test was conducted to examine the grafting efficiency, and the three groups were successfully grafted. Calcium carbonate mineralization on a modified silicon substrate was examined by a scanning electron microscope (SEM) and x-ray diffraction (XRD), and the results showed that the effects of -OH, -NH2 and -COOH groups were quite different. Furthermore, a water-soluble protein matrix (WSM) and an acid-soluble protein matrix (ASM) extracted from fish otolith were adsorbed onto the -COOH-modified silicon substrate, and the effects of the protein matrices on calcium carbonate mineralization were studied. The results showed that both WSM and ASM of lapillus could mediate aragonite crystallization, but the size and morphology of the formed crystals were different. The WSM and ASM of asteriscus adsorbed on the silicon substrate had little effect on calcium carbonate mineralization; almost all the crystals were calcite, while both asteriscus WSM and ASM in solution could mediate vaterite crystals, and the morphologies of vaterite crystal aggregates were different.

  6. The effects of atmospheric [CO2] on carbon isotope fractionation and magnesium incorporation into biogenic marine calcite

    Science.gov (United States)

    Vieira, Veronica

    1997-01-01

    The influences of atmospheric carbon dioxide on the fractionation of carbon isotopes and the magnesium incorporation into biogenic marine calcite were investigated using samples of the calcareous alga Amphiroa and benthic foraminifer Sorites grown in the Biosphere 2 Ocean system under variable atmospheric CO2 concentrations (approximately 500 to 1200 ppm). Carbon isotope fractionation was studied in both the organic matter and the skeletal carbonate. Magnesium analysis was to be performed on the carbonate removed during decalcification. These data have not been collected due to technical problems. Carbon isotope data from Amphiroa yields a linear relation between [CO2] and Delta(sup 13)C(sub Corg)values suggesting that the fractionation of carbon isotopes during photosynthesis is positively correlated with atmospheric [CO2]. [CO2] and Delta(sup 13)C(sub Corg) values for Sorites produce a relation that is best described by a hyperbolic function where Delta(sup 13)C(sub Corg) values increase between 300 and 700 ppm and decrease from 700 to 1200 ppm. Further investigation of this relation and Sorites physiology is needed.

  7. A 13C labelling study on carbon fluxes in Arctic plankton communities under elevated CO2 levels

    Directory of Open Access Journals (Sweden)

    A. de Kluijver

    2013-03-01

    Full Text Available The effect of CO2 on carbon fluxes (production, consumption, and export in Arctic plankton communities was investigated during the 2010 EPOCA (European project on Ocean Acidification mesocosm study off Ny Ålesund, Svalbard. 13C labelled bicarbonate was added to nine mesocosms with a range in pCO2 (185 to 1420 μatm to follow the transfer of carbon from dissolved inorganic carbon (DIC into phytoplankton, bacterial and zooplankton consumers, and export. A nutrient–phytoplankton–zooplankton–detritus model amended with 13C dynamics was constructed and fitted to the data to quantify uptake rates and carbon fluxes in the plankton community. The plankton community structure was characteristic for a post-bloom situation and retention food web and showed high bacterial production (∼31% of primary production, high abundance of mixotrophic phytoplankton, low mesozooplankton grazing (∼6% of primary production and low export (∼7% of primary production. Zooplankton grazing and export of detritus were sensitive to CO2: grazing decreased and export increased with increasing pCO2. Nutrient addition halfway through the experiment increased the export, but not the production rates. Although mixotrophs showed initially higher production rates with increasing CO2, the overall production of POC (particulate organic carbon after nutrient addition decreased with increasing CO2. Interestingly, and contrary to the low nutrient situation, much more material settled down in the sediment traps at low CO2. The observed CO2 related effects potentially alter future organic carbon flows and export, with possible consequences for the efficiency of the biological pump.

  8. Numerical Investigation into the Impact of CO2-Water-Rock Interactions on CO2 Injectivity at the Shenhua CCS Demonstration Project, China

    Directory of Open Access Journals (Sweden)

    Guodong Yang

    2017-01-01

    Full Text Available A 100,000 t/year demonstration project for carbon dioxide (CO2 capture and storage in the deep saline formations of the Ordos Basin, China, has been successfully completed. Field observations suggested that the injectivity increased nearly tenfold after CO2 injection commenced without substantial pressure build-up. In order to evaluate whether this unique phenomenon could be attributed to geochemical changes, reactive transport modeling was conducted to investigate CO2-water-rock interactions and changes in porosity and permeability induced by CO2 injection. The results indicated that using porosity-permeability relationships that include tortuosity, grain size, and percolation porosity, other than typical Kozeny-Carman porosity-permeability relationship, it is possible to explain the considerable injectivity increase as a consequence of mineral dissolution. These models might be justified in terms of selective dissolution along flow paths and by dissolution or migration of plugging fines. In terms of geochemical changes, dolomite dissolution is the largest source of porosity increase. Formation physical properties such as temperature, pressure, and brine salinity were found to have modest effects on mineral dissolution and precipitation. Results from this study could have practical implications for a successful CO2 injection and enhanced oil/gas/geothermal production in low-permeability formations, potentially providing a new basis for screening of storage sites and reservoirs.

  9. 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.

  10. A study of CO2 precipitation method considering an ionic CO2 and Ca(OH)2 slurry

    International Nuclear Information System (INIS)

    Park, Sangwon; Jo, Hoyong; Kang, Dongwoo; Park, Jinwon

    2014-01-01

    CCS (carbon capture and storage) is the most popular technology used for the reduction of CO 2 in the post-combustion stage. However, the CCS process has some disadvantages including uncertainty about the stability of the land that is used to store the separated CO 2 . Consequently, CCU (carbon capture and utilization) technologies have recently received increased attention as a possible replacement for CCS. In this study, we utilized CO 2 fixation methods by using the metal carbonate mechanism. We selected 5 and 30 wt% MEA (mono-ethanolamine) solutions to rapidly make a carbonate and Ca(OH) 2 slurry. In all of the experiments, normal temperature and pressure conditions were maintained (except during desorption to check for residual CO 2 in the MEA solution). Consequently, most of the CO 2 was converted to carbonate. The MEA converted CO 2 to ionic CO 2 and rapidly created calcium carbonate. Also the formed solids that were observed were determined to be CaCO 3 and Ca(OH) 2 by X-ray diffractometry. Also, the MEA solution could be reused to absorb CO 2 . Therefore, we have confirmed the development of our suggested CCS process. This process has the ability not only to reuse emitted CO 2 , but it can also be employed to reuse construction wastes that include heavy metals. - Highlights: • We propose novel CO 2 conversion technology by utilizing an amine solution. • In this study, alkaline solutions were used to produce CO 2 precipitate. • The MEA (mono-ethanolamine) solution has a sufficient potential to fix CO 2 with metal sources under moderate condition. • Also, the Ca(OH) 2 slurry yielded enough Ca 2+ ions to make carbonate

  11. Fundamentals of carbon dioxide-enhanced oil recovery (CO2-EOR): a supporting document of the assessment methodology for hydrocarbon recovery using CO2-EOR associated with carbon sequestration

    Science.gov (United States)

    Verma, Mahendra K.

    2015-01-01

    The objective of this report is to provide basic technical information regarding the CO2-EOR process, which is at the core of the assessment methodology, to estimate the technically recoverable oil within the fields of the identified sedimentary basins of the United States. Emphasis is on CO2-EOR because this is currently one technology being considered as an ultimate long-term geologic storage solution for CO2 owing to its economic profitability from incremental oil production offsetting the cost of carbon sequestration.

  12. Preparation of a carbon molecular sieve and application to separation of N2, O2 and CO2 in a fixed bed

    Directory of Open Access Journals (Sweden)

    Soares J.L.

    2003-01-01

    Full Text Available The emission of CO2 from power plants that burn fossil fuels is the major cause of the accumulation of CO2 in the atmosphere. The separation of CO2 from CO2/air mixtures can play a key role in alleviating this problem. This separation can be carried out by using suitable adsorbents, such as carbon molecular sieves. In this work, a CMS was prepared by deposition of polyfurfuryl alcohol polymer on activated carbon. After deposition of the polymer, the material was carbonized at 800masculineC for 2 hours. This material was used to separate O2/N2 mixtures and CO2 in a fixed bed at room temperature. Experimental breakthrough curves obtained were fitted to theoretical models in order to establish the main mechanisms of mass transfer. The breakthrough curves showed that it is possible to separate O2, N2 and CO2. The shape of the breakthrough curves was not influenced by the total flow, indicating that the gas contact for the gas mixture was good. The experimental data were fitted to theoretical models and it was established that the main mechanism of mass transfer was intraparticle diffusion.

  13. Mesocosm-Scale Experimental Quantification of Plant-Fungi Associations on Carbon Fluxes and Mineral Weathering

    Science.gov (United States)

    Andrews, M. Y.; Palmer, B.; Leake, J. R.; Banwart, S. A.; Beerling, D. J.

    2009-12-01

    The rise of land plants in the Paleozoic is classically implicated as driving lower atmospheric CO2 levels through enhanced weathering of Ca and Mg bearing silicate minerals. However, this view overlooks the fact that plants coevolved with associated mycorrhizal fungi over this time, with many of the weathering processes usually ascribed to plants actually being driven by the combined activities of roots and mycorrhizal fungi. Here we present initial results from a novel mesocosm-scale laboratory experiment designed to allow investigation of plant-driven carbon flux and mineral weathering at different soil depths under ambient (400 ppm) and elevated (1500 ppm) atmospheric CO2. Four species of plants were chosen to address evolutionary trends in symbiotic mycorrhizal association and rooting depth on biologically driven silicate weathering under the different CO2 regimes. Gymnosperms were used to investigate potential differences in weathering capabilities of two fungal symbioses: Sequoia sempervirens and Metasequoia glyptostroboides (arbuscular mycorrhizal, AM) and Pinus sylvestris (ectomycorrhizal, EM), and the shallow rooted ancient fern, Osmunda regalis, used to provide a contrast to the three more deeply rooted trees. Plants were grown in a cylindrical mesocosm with four horizontal inserts at each depth. These inserts are a mesh-covered dual-core unit whereby an inner core containing silicate minerals can be rotated within an outer core. The mesh excludes roots from the cylinders allowing fungal-rock pairings to be examined at each depth. Each core contains either basalt or granite, each with severed (rotated cores) or intact (static cores) mycorrhizae. This system provides a unique opportunity to examine the ability of a plant to weather minerals with and without its symbiotic fungi. Preliminary results indicate marked differences in nutritional and water requirements, and response to elevated CO2 between the species. The bulk solution chemistries (p

  14. Compiled records of carbon isotopes in atmospheric CO2 for historical simulations in CMIP6

    Directory of Open Access Journals (Sweden)

    H. Graven

    2017-12-01

    Full Text Available The isotopic composition of carbon (Δ14C and δ13C in atmospheric CO2 and in oceanic and terrestrial carbon reservoirs is influenced by anthropogenic emissions and by natural carbon exchanges, which can respond to and drive changes in climate. Simulations of 14C and 13C in the ocean and terrestrial components of Earth system models (ESMs present opportunities for model evaluation and for investigation of carbon cycling, including anthropogenic CO2 emissions and uptake. The use of carbon isotopes in novel evaluation of the ESMs' component ocean and terrestrial biosphere models and in new analyses of historical changes may improve predictions of future changes in the carbon cycle and climate system. We compile existing data to produce records of Δ14C and δ13C in atmospheric CO2 for the historical period 1850–2015. The primary motivation for this compilation is to provide the atmospheric boundary condition for historical simulations in the Coupled Model Intercomparison Project 6 (CMIP6 for models simulating carbon isotopes in the ocean or terrestrial biosphere. The data may also be useful for other carbon cycle modelling activities.

  15. Compiled records of carbon isotopes in atmospheric CO2 for historical simulations in CMIP6

    Science.gov (United States)

    Graven, Heather; Allison, Colin E.; Etheridge, David M.; Hammer, Samuel; Keeling, Ralph F.; Levin, Ingeborg; Meijer, Harro A. J.; Rubino, Mauro; Tans, Pieter P.; Trudinger, Cathy M.; Vaughn, Bruce H.; White, James W. C.

    2017-12-01

    The isotopic composition of carbon (Δ14C and δ13C) in atmospheric CO2 and in oceanic and terrestrial carbon reservoirs is influenced by anthropogenic emissions and by natural carbon exchanges, which can respond to and drive changes in climate. Simulations of 14C and 13C in the ocean and terrestrial components of Earth system models (ESMs) present opportunities for model evaluation and for investigation of carbon cycling, including anthropogenic CO2 emissions and uptake. The use of carbon isotopes in novel evaluation of the ESMs' component ocean and terrestrial biosphere models and in new analyses of historical changes may improve predictions of future changes in the carbon cycle and climate system. We compile existing data to produce records of Δ14C and δ13C in atmospheric CO2 for the historical period 1850-2015. The primary motivation for this compilation is to provide the atmospheric boundary condition for historical simulations in the Coupled Model Intercomparison Project 6 (CMIP6) for models simulating carbon isotopes in the ocean or terrestrial biosphere. The data may also be useful for other carbon cycle modelling activities.

  16. IUPAC-NIST Solubility Data Series. 95. Alkaline Earth Carbonates in Aqueous Systems. Part 2. Ca

    Science.gov (United States)

    Vanderdeelen, Jan

    2012-06-01

    The alkaline earth carbonates are an important class of minerals. This article is part of a volume in the IUPAC-NIST Solubility Data Series that compiles and critically evaluates solubility data of the alkaline earth carbonates in water and in simple aqueous electrolyte solutions. Part 1 outlined the procedure adopted in this volume, and presented the beryllium and magnesium carbonates. Part 2, the current paper, compiles and critically evaluates the solubility data of calcium carbonate. The chemical forms included are the anhydrous CaCO3 types calcite, aragonite, and vaterite, the monohydrate monohydrocalcite (CaCO3. H2O), the hexahydrate ikaite (CaCO3.6H2O), and an amorphous form. The data were analyzed with two model variants, and thermodynamic data of each form consistent with each of the models and with the CODATA key values for thermodynamics are presented.

  17. Effects of porous carbon additives on the CO{sub 2} absorption performance of lithium orthosilicate

    Energy Technology Data Exchange (ETDEWEB)

    Jeoung, Sungeun; Lee, Jae Hwa [Department of Chemistry, School of Natural Science, Ulsan National Institute of Science and Technology (UNIST), UNIST-gil 50, Ulsan 44919 (Korea, Republic of); Kim, Ho Young [Department of Chemical Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), UNIST-gil 50, Ulsan 44919 (Korea, Republic of); Moon, Hoi Ri, E-mail: hoirimoon@unist.ac.kr [Department of Chemistry, School of Natural Science, Ulsan National Institute of Science and Technology (UNIST), UNIST-gil 50, Ulsan 44919 (Korea, Republic of)

    2016-08-10

    Highlights: • Composites of Li{sub 4}SiO{sub 4} and porous carbon materials were prepared for CO{sub 2} absorbents. • The kinetic parameters of the composites were examined. • The pores of CMK-3 in Li{sub 4}SiO{sub 4} aid the diffusion of CO{sub 2}. - Abstract: Lithium orthosilicate (Li{sub 4}SiO{sub 4}) is an attractive high-temperature CO{sub 2} sorbent (>650 °C) because of its large theoretical absorption capacity of up to 36.7 wt%. However, slow kinetics and partial reactions with CO{sub 2} hinder its proper operation as a sorbent under practical conditions. To allow the use of this sorbent at lower operation temperatures, the present studies explored the way to improve the CO{sub 2} absorption kinetics and increase the degree of reaction of Li{sub 4}SiO{sub 4}. Porous carbon materials such as CMK-3 were introduced into the sorbent to provide an internal gas pathway. Upon calcination conditions, the carbon amount was controlled in the composites (Li{sub 4}SiO{sub 4}@CMK-X%, where X represents the amounts of CMK-3). In Li{sub 4}SiO{sub 4}@CMK-1.8%, CMK-3 is distributed over the whole solid; in contrast, the additive in Li{sub 4}SiO{sub 4}@CMK-0.5% is mainly observed near the surface of the solid. CO{sub 2} gas sorption study of the composites showed that pores of CMK-3 in Li{sub 4}SiO{sub 4} aid the diffusion of CO{sub 2}. In addition, we found that the incorporation of porous carbon provides more active sites for interactions with CO{sub 2} through the formation of cavities between Li{sub 4}SiO{sub 4} and CMK-3. Li{sub 4}SiO{sub 4}@CMK-1.8% had an increased CO{sub 2} absorption capacity (35.4 wt%) and rate (15.2 wt% for the first 5 min) at 600 °C, compared to the CO{sub 2} absorption capacity (16.3 wt%) and rate (5.1 wt% for the first 5 min) of pristine Li{sub 4}SiO{sub 4} (p-Li{sub 4}SiO{sub 4}). To confirm the influence of porous carbon on the CO{sub 2} absorption properties, multi-walled carbon nanotube (MWCNT) was also examined as an additive

  18. The Formation of Carbonate Minerals and the Mobility of Heavy Metals during Water-CO2-Mafic Rock Interactions

    DEFF Research Database (Denmark)

    Olsson, Jonas

    to the carbonate precipitation in CarbFix project. In the third study, water and solid samples from two alkaline springs in Oman were examined. The elements detected in the spring waters in order of abundance were Na, Cl, Ca, Mg, SO4, K, Br, Si, F, B, Sr, Al, Fe, Mo, Zn, Ni, Cu, Mn, V, Ba, Cr, Co, Ti, Hg and Pb...

  19. Earth 2075 (CO2) - can Ocean-Amplified Carbon Capture (oacc) Impart Atmospheric CO2-SINKING Ability to CCS Fossil Energy?

    Science.gov (United States)

    Fry, R.; Routh, M.; Chaudhuri, S.; Fry, S.; Ison, M.; Hughes, S.; Komor, C.; Klabunde, K.; Sethi, V.; Collins, D.; Polkinghorn, W.; Wroobel, B.; Hughes, J.; Gower, G.; Shkolnik, J.

    2017-12-01

    Previous attempts to capture atmospheric CO2 by algal blooming were stalled by ocean viruses, zooplankton feeding, and/or bacterial decomposition of surface blooms, re-releasing captured CO2 instead of exporting it to seafloor. CCS fossil energy coupling could bypass algal bloom limits—enabling capture of 10 GtC/yr atmospheric CO2 by selective emiliania huxleyi (EHUX) blooming in mid-latitude open oceans, far from coastal waters and polar seas. This could enable a 500 GtC drawdown, 350 ppm restoration by 2050, 280 ppm CO2 by 2075, and ocean pH 8.2. White EHUX blooms could also reflect sunlight back into outer space and seed extra ocean cloud cover, via DMS release, to raise albedo 1.8%—restoring preindustrial temperature (ΔT = 0°C) by 2030. Open oceans would avoid post-bloom anoxia, exclusively a coastal water phenomenon. The EHUX calcification reaction initially sources CO2, but net sinking prevails in follow-up equilibration reactions. Heavier-than-water EHUX sink captured CO2 to the sea floor before surface decomposition occurs. Seeding EHUX high on their nonlinear growth curve could accelerate short-cycle secondary open-ocean blooming—overwhelming mid-latitude viruses, zooplankton, and competition from other algae. Mid-latitude "ocean deserts" exhibit low viral, zooplankton, and bacterial counts. Thermocline prevents nutrient upwelling that would otherwise promote competing algae. Adding nitrogen nutrient would foster exclusive EHUX blooming. Elevated EHUX seed levels could arise from sealed, pH-buffered, floating, seed-production bioreactors infused with 10% CO2 from carbon feedstock supplied by inland CCS fossil power plants capturing 90% of emissions as liquid CO2. Deep-water SPAR platforms extract natural gas from beneath the sea floor. On-platform Haber and pH processing could convert extracted CH4 to buffered NH4+ nutrient, enabling ≥0.7 GtC/yr of bioreactor seed production and 10 GtC/yr of amplified secondary open-ocean CO2 capture—making CCS

  20. Activated carbons prepared from hazelnut shells, walnut shells and peanut shells for high CO2 adsorption

    Directory of Open Access Journals (Sweden)

    Lewicka Katarzyna

    2017-06-01

    Full Text Available Research treats about producing activated carbons for CO2 capture from hazelnut shells (HN, walnut shells (WN and peanut shells (PN. Saturated solution of KOH was used as an activating agent in ratio 1:1. Samples were carbonized in the furnace in the range of temperatures 600°C–900°C. Properties of carbons were tested by N2 adsorption method, using BET equation, DFT method and volumetric CO2 adsorption method. With the increase of carbonization temperature specific surface area of studied samples increased. The largest surface area was calculated for samples carbonized at 900°C and the highest values of CO2 adsorption had samples: PN900 at 0°C (5.5 mmol/g and WN900 at 25°C (4.34 mmol/g. All of the samples had a well-developed microporous structure.

  1. A decade of free‐air CO2 enrichment increased the carbon throughput in a grass‐clover ecosystem but did not drastically change carbon allocation patterns

    DEFF Research Database (Denmark)

    Staddon, Philip Louis; Reinsch, Sabine; Olsson, Pål A.

    2014-01-01

    labelling to determine whether elevated CO2 (+230 μL L−1) concentration changes the fate of recently assimilated carbon in the soil microbial community. Elevated CO2 (eCO2) concentration had an overall positive effect on microbial abundance (P negative bacteria showing significantly...... increased quantities. Gram‐negative bacteria and saprotrophic fungi tended to utilize a higher amount of recently assimilated carbon under eCO2. Arbuscular mycorrhizal fungi (AMF) utilized plant‐assimilated carbon within 1 day after the 13CO2 pulse and 13C uptake patterns in AMF suggest that carbon transfer...

  2. Carbon mineralization and pyrite oxidation in groundwater: Importance for silicate weathering in boreal forest soils and stream base-flow chemistry

    International Nuclear Information System (INIS)

    Klaminder, J.; Grip, H.; Moerth, C.-M.; Laudon, H.

    2011-01-01

    Research highlights: → Organic compounds is mineralized during later transport in deep groundwater aquifers. → Carbonic acid generated by this process stimulates dissolution of silicate minerals. → Protons derived from pyrite oxidation also affects weathering in deep groundwater. → The identified weathering mechanisms affect base-flow chemistry in boreal streams. - Abstract: What role does mineralized organic C and sulfide oxidation play in weathering of silicate minerals in deep groundwater aquifers? In this study, how H 2 CO 3 , produced as a result of mineralization of organic matter during groundwater transport, affects silicate weathering in the saturated zone of the mineral soil along a 70 m-long boreal hillslope is demonstrated. Stream water measurements of base cations and δ 18 O are included to determine the importance of the deep groundwater system for downstream surface water. The results suggest that H 2 CO 3 generated from organic compounds being mineralized during the lateral transport stimulates weathering at depths between 0.5 and 3 m in the soil. This finding is indicated by progressively increasing concentrations of base cations-, silica- and inorganic C (IC) in the groundwater along the hillslope that co-occur with decreasing organic C (OC) concentrations. Protons derived from sulfide oxidation appear to be an additional driver of the weathering process as indicated by a build-up of SO 4 2- in the groundwater during lateral transport and a δ 34 S per mille value of +0.26-3.76 per mille in the deep groundwater indicating S inputs from pyrite. The two identified active acids in the deep groundwater are likely to control the base-flow chemistry of streams draining larger catchments (>1 km 2 ) as evident by δ 18 O signatures and base cation concentrations that overlap with that of the groundwater.

  3. Carbon mineralization and pyrite oxidation in groundwater: Importance for silicate weathering in boreal forest soils and stream base-flow chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Klaminder, J., E-mail: jonatan.klaminder@emg.umu.se [Department of Forest Ecology and Management, SLU, SE-901 83 Umea (Sweden)] [Department of Ecology and Environmental Science, Umea University, SE-901 87 (Sweden); Grip, H. [Department of Forest Ecology and Management, SLU, SE-901 83 Umea (Sweden); Moerth, C.-M. [Department of Geological Sciences, Stockholm University, 106 91 Stockholm (Sweden); Laudon, H. [Department of Forest Ecology and Management, SLU, SE-901 83 Umea (Sweden)

    2011-03-15

    Research highlights: {yields} Organic compounds is mineralized during later transport in deep groundwater aquifers. {yields} Carbonic acid generated by this process stimulates dissolution of silicate minerals. {yields} Protons derived from pyrite oxidation also affects weathering in deep groundwater. {yields} The identified weathering mechanisms affect base-flow chemistry in boreal streams. - Abstract: What role does mineralized organic C and sulfide oxidation play in weathering of silicate minerals in deep groundwater aquifers? In this study, how H{sub 2}CO{sub 3}, produced as a result of mineralization of organic matter during groundwater transport, affects silicate weathering in the saturated zone of the mineral soil along a 70 m-long boreal hillslope is demonstrated. Stream water measurements of base cations and {delta}{sup 18}O are included to determine the importance of the deep groundwater system for downstream surface water. The results suggest that H{sub 2}CO{sub 3} generated from organic compounds being mineralized during the lateral transport stimulates weathering at depths between 0.5 and 3 m in the soil. This finding is indicated by progressively increasing concentrations of base cations-, silica- and inorganic C (IC) in the groundwater along the hillslope that co-occur with decreasing organic C (OC) concentrations. Protons derived from sulfide oxidation appear to be an additional driver of the weathering process as indicated by a build-up of SO{sub 4}{sup 2-} in the groundwater during lateral transport and a {delta}{sup 34}S per mille value of +0.26-3.76 per mille in the deep groundwater indicating S inputs from pyrite. The two identified active acids in the deep groundwater are likely to control the base-flow chemistry of streams draining larger catchments (>1 km{sup 2}) as evident by {delta}{sup 18}O signatures and base cation concentrations that overlap with that of the groundwater.

  4. Quantification of CO2 generation in sedimentary basins through carbonate/clays reactions with uncertain thermodynamic parameters

    Science.gov (United States)

    Ceriotti, G.; Porta, G. M.; Geloni, C.; Dalla Rosa, M.; Guadagnini, A.

    2017-09-01

    We develop a methodological framework and mathematical formulation which yields estimates of the uncertainty associated with the amounts of CO2 generated by Carbonate-Clays Reactions (CCR) in large-scale subsurface systems to assist characterization of the main features of this geochemical process. Our approach couples a one-dimensional compaction model, providing the dynamics of the evolution of porosity, temperature and pressure along the vertical direction, with a chemical model able to quantify the partial pressure of CO2 resulting from minerals and pore water interaction. The modeling framework we propose allows (i) estimating the depth at which the source of gases is located and (ii) quantifying the amount of CO2 generated, based on the mineralogy of the sediments involved in the basin formation process. A distinctive objective of the study is the quantification of the way the uncertainty affecting chemical equilibrium constants propagates to model outputs, i.e., the flux of CO2. These parameters are considered as key sources of uncertainty in our modeling approach because temperature and pressure distributions associated with deep burial depths typically fall outside the range of validity of commonly employed geochemical databases and typically used geochemical software. We also analyze the impact of the relative abundancy of primary phases in the sediments on the activation of CCR processes. As a test bed, we consider a computational study where pressure and temperature conditions are representative of those observed in real sedimentary formation. Our results are conducive to the probabilistic assessment of (i) the characteristic pressure and temperature at which CCR leads to generation of CO2 in sedimentary systems, (ii) the order of magnitude of the CO2 generation rate that can be associated with CCR processes.

  5. Single-, double-, and triple-photoionization cross sections of carbon monoxide (CO) and ionic fragmentation of CO+, CO2+, and CO3+

    International Nuclear Information System (INIS)

    Masuoka, T.; Nakamura, E.

    1993-01-01

    Single-, double-, and triple-photoionization processes of carbon monoxide (CO) have been studied in the photon-energy region of 37--100 eV by use of time-of-flight mass spectrometry and a photoion-photoion-coincidence method together with synchrotron radiation. The single-, double-, and triple-photoionization cross sections of CO are determined. Ion branching ratios and the partial cross sections for the individual ions respectively produced from the precursors CO + and CO 2+ are determined separately at excitation energies where the molecular and dissociative single- and double-photoionization processes compete. The threshold for the molecular double photoionization was found to be 41.3±0.2 eV. Furthermore, in single photoionization, the production of CO + is dominant whereas with double photoionization dissociation becomes dominant

  6. Transport and transformation of soil-derived CO2, CH4 and DOC sustain CO2 supersaturation in small boreal streams.

    Science.gov (United States)

    Rasilo, Terhi; Hutchins, Ryan H S; Ruiz-González, Clara; Del Giorgio, Paul A

    2017-02-01

    Streams are typically supersaturated in carbon dioxide (CO 2 ) and methane (CH 4 ), and are recognized as important components of regional carbon (C) emissions in northern landscapes. Whereas there is consensus that in most of the systems the CO 2 emitted by streams represents C fixed in the terrestrial ecosystem, the pathways delivering this C to streams are still not well understood. We assessed the contribution of direct soil CO 2 injection versus the oxidation of soil-derived dissolved organic C (DOC) and CH 4 in supporting CO 2 supersaturation in boreal streams in Québec. We measured the concentrations of CO 2 , CH 4 and DOC in 43 streams and adjacent soil waters during summer base-flow period. A mass balance approach revealed that all three pathways are significant, and that the mineralization of soil-derived DOC and CH 4 accounted for most of the estimated stream CO 2 emissions (average 75% and 10%, respectively), and that these estimated contributions did not change significantly between the studied low order (≤3) streams. Whereas some of these transformations take place in the channel proper, our results suggest that they mainly occur in the hyporheic zones of the streams. Our results further show that stream CH 4 emissions can be fully explained by soil CH 4 inputs. This study confirms that these boreal streams, and in particular their hyporheic zones, are extremely active processors of soil derived DOC and CH 4 , not just vents for soil produced CO 2 . Copyright © 2016 Elsevier B.V. All rights reserved.

  7. Modeling long-term carbon residue in the ocean-atmosphere system following large CO2 emissions

    Science.gov (United States)

    Towles, N. J.; Olson, P.; Gnanadesikan, A.

    2013-12-01

    We use the LOSCAR carbon cycle model (Zeebe et al., 2009; Zeebe, 2012) to calculate the residual carbon in the ocean and atmosphere following large CO2 emissions. We consider the system response to CO2 emissions ranging from 100 to 20000 PgC, and emission durations from 100 yr to 100 kyr, subject to a wide range of system parameters such as the strengths of silicate weathering and the oceanic biological carbon pump. We define the carbon gain factor as the ratio of residual carbon in the ocean-atmosphere to the total emitted carbon. For moderate sized emissions shorter than about 50 kyr, we find that the carbon gain factor grows during the emission and peaks at about 1.7, primarily due to the erosion of carbonate marine sediments. In contrast, for longer emissions, the carbon gain factor peaks at a smaller value, and for very large emissions (more than 5000 PgC), the gain factor decreases with emission size due to carbonate sediment exhaustion. This gain factor is sensitive to model parameters such as low latitude efficiency of the biological pump. The timescale for removal of the residual carbon (reducing the carbon gain factor to zero) depends strongly on the assumed sensitivity of silicate weathering to atmospheric pCO2, and ranges from less than one million years to several million years.

  8. Co@Carbon and Co 3 O4@Carbon nanocomposites derived from a single MOF for supercapacitors.

    Science.gov (United States)

    Dai, Engao; Xu, Jiao; Qiu, Junjie; Liu, Shucheng; Chen, Ping; Liu, Yi

    2017-10-03

    Developing a composite electrode containing both carbon and transition metal/metal oxide as the supercapacitor electrode can combine the merits and mitigate the shortcomings of both the components. Herein, we report a simple strategy to prepare the hybrid nanostructure of Co@Carbon and Co 3 O 4 @Carbon by pyrolysis a single MOFs precursor. Co-based MOFs (Co-BDC) nanosheets with morphology of regular parallelogram slice have been prepared by a bottom-up synthesis strategy. One-step pyrolysis of Co-BDC, produces a porous carbon layer incorporating well-dispersed Co and Co 3 O 4 nanoparticles. The as-prepared cobalt-carbon composites exhibit the thin layer morphology and large specific surface area with hierarchical porosity. These features significantly improve the ion-accessible surface area for charge storage and shorten the ion transport length in thin dimension, thus contributing to a high specific capacitance. Improved capacitance performance was successfully realized for the asymmetric supercapacitors (ASCs) (Co@Carbon//Co 3 O 4 @Carbon), better than those of the symmetric supercapacitors (SSCs) based on Co@Carbon and Co 3 O 4 @Carbon materials (i.e., Co@Carbon//Co@Carbon and Co 3 O 4 @Carbon//Co 3 O 4 @Carbon). The working voltage of the ASCs can be extended to 1.5 V and show a remarkable high power capability in aqueous electrolyte. This work provides a controllable strategy for nanostructured carbon-metal and carbon-metal oxide composite electrodes from a single precursor.

  9. Corrosion of a hot potassium carbonate CO/sub 2/ removal plant

    International Nuclear Information System (INIS)

    Johnson, J.J.

    1987-01-01

    After ten years of successful operation, a hot potassium carbonate CO/sub 2/ removal plant experienced severe corrosion to the 2'' (50 mm) thick carbon steel absorber process vessel over a fourteen month period. This corrosive attack resulted in complete penetration on three separate occasions. Although the cause of this corrosion is still uncertain, it appears to be the result of decreasing strength of the vanadium pentoxide inhibitor, due to increasing concentrations of hydrogen sulfide in the feed gas. After extensive research, Chevron believes that stainless steel metallurgy or replacement of the hot potassium carbonate process are the only reliable long-term solutions

  10. CO2 consumption and bicarbonate fluxes by chemical weathering in North America.

    Science.gov (United States)

    Jansen, Nils; Hartmann, Jens; Lauerwald, Ronny

    2010-05-01

    Cations released by chemical weathering are mainly counterbalanced by atmospheric/soil CO2 dissolved in water. Existing approaches to quantify CO2 consumption by chemical weathering are mostly based on the parameters runoff and lithology. Land cover is not implemented as predictor in existing regional or global scale models for atmospheric/soil CO2 consumption. Here, bicarbonate fluxes in North American rivers are quantified by an empirical forward model using the predictors runoff, lithology and land cover. The model was calibrated on chemical data from 338 river monitoring stations throughout North America. It was extrapolated to the entire North American continent by applying the model equation spatially explicitly to the geodata used for model calibration. Because silicate mineral weathering derived bicarbonate in rivers originates entirely from atmospheric/soil CO2, but carbonate mineral weathering additionally releases lithogenic bicarbonate, those source minerals are distinguished to quantify the CO2 consumption by chemical weathering. Extrapolation of the model results in a total bicarbonate flux of 51 Mt C a-1 in North America; 70% of which originate from atmospheric/soil CO2. On average, chemical weathering consumes 2.64 t atmospheric/soil C km-2 a-1 (~ 30%-40% above published world average values). For a given runoff and land cover, carbonate-rich sedimentary rocks export the most bicarbonate. However, half of this is assumed to be of lithogenic origin. Thus, the most atmospheric/soil CO2 per runoff is modeled to be consumed by basic plutonics. The least bicarbonate is exported and the least CO2 is consumed per runoff by weathering of metamorphic rocks. Of the distinguished different land cover classes of which urban areas export the most bicarbonate for a given lithology and runoff, followed by shrubs, grasslands and managed lands. For a given runoff and lithology, the least bicarbonate is exported from areas with forested land cover. The model shows 1

  11. Hot and cold CO{sub 2}-rich mineral waters in Chaves geothermal area (northern Portugal)

    Energy Technology Data Exchange (ETDEWEB)

    Aires-Barros, Luis; Marques, Jose Manuel; Graca, Rui Cores; Matias, Maria Jose [Universidade Tecnica de Lisboa, Lab. de Mineralogia e Petrologia (LAMPIST), Lisboa (Portugal); Weijden, Cornelis H. van der; Kreulen, Rob [Utrecht Univ., Dept. of Geochemistry, Utrecht (Netherlands); Eggenkamp, Hermanus Gerardus M. [Utrecht Univ., Dept. of Geochemistry, Utrecht (Netherlands); Reading Univ., Postgraduate Research Inst. for Sedimentology, Reading (United Kingdom)

    1998-02-01

    In order to update the geohydrologic characterisation of Chaves geothermal area, coupled isotopic and chemical studies have been carried out on hot and cold CO{sub 2}-rich mineral waters discharging, in northern Portugal, along one of the major regional NNE-trending faults (the so-called Verin-Chaves-Penacova Depression). Based upon their location, and chemical and isotopic composition, the analysed waters can be divided into two groups. The northern group belongs to the HCO{sub 3}/Na/CO{sub 2}-rich type, and consists of the hot spring waters of Chaves and the cold spring waters of Vilarelho da Raia. The {delta}D and {delta}{sup 18}O values show that these waters are of meteoric origin. The lack of an {sup 18}O shift indicates that there is no evidence of water/rock interaction at high temperatures. The southern group includes the cold spring waters of Campilho/Vidago and Sabroso/Pedras Salgadas. Their chemistry is similar to that of the northern group but their heavier {delta}D and {delta}{sup 18}O values could be attributed to different recharge altitudes. Mixing between deep mineralised waters and dilute superficial waters of meteoric origin might explain the higher {sup 3}H activity found in the Vidago and Pedras Salgadas mineral waters. Alternatively, they could be mainly related to shallow underground flowpaths. The {delta}{sup 13}C values support a deep-seated origin for the CO{sub 2}. The {delta}{sup 37}Cl is comparable in all the mineral waters of the study areas, indicating a common origin of Cl. The {sup 87}Sr/{sup 86}Sr ratios in waters seem to be dominated by the dissolution of plagioclases or granitic rocks. (Author)

  12. Carbon dioxide (CO2) sequestration in deep saline aquifers and formations: Chapter 3

    Science.gov (United States)

    Rosenbauer, Robert J.; Thomas, Burt

    2010-01-01

    Carbon dioxide (CO2) capture and sequestration in geologic media is one among many emerging strategies to reduce atmospheric emissions of anthropogenic CO2. This chapter looks at the potential of deep saline aquifers – based on their capacity and close proximity to large point sources of CO2 – as repositories for the geologic sequestration of CO2. The petrochemical characteristics which impact on the suitability of saline aquifers for CO2 sequestration and the role of coupled geochemical transport models and numerical tools in evaluating site feasibility are also examined. The full-scale commercial CO2 sequestration project at Sleipner is described together with ongoing pilot and demonstration projects.

  13. Mechanisms of scale formation and carbon dioxide partial pressure influence. Part II. Application in the study of mineral waters of reference.

    Science.gov (United States)

    Gal, Jean-Yves; Fovet, Yannick; Gache, Nathalie

    2002-02-01

    In the first part, we have designed a new model of evolution for the calco-carbonic system which includes the hydrated forms of CaCO3: CaCO3 amorphous, CaCO3 x 6H2O (ikaite) and CaCO3 x H2O (monohydrate) (J. Eur. Hydr. 30 (1999) 47). According to this model, it is the precipitation of one or other of these hydrated forms which could be responsible for the breakdown of the metastable state. After this first step, the precipitates evolve to dehydrated solid forms. Through the elaboration of computer programs in which the CaCO3(0) (aq) ion pair formation was considered, this model was compared to experimental data obtained by the critical pH method applied to synthetic solutions. In the present article, the same method was applied for four French mineral waters, at 25 degrees C under study. Three samples formed a precipitation during the sodium hydroxide addition. For these three cases, this precipitation began for the CaCO3 H2O saturation. The added volume of sodium hydroxide was more than what was required for neutralizing free CO2 initially in solution. These results indicate that during a spontaneous scaling phenomenon, the pH rises at the same time by loss of the initial free CO2 and of the one produced by the hydrogen carbonate ions decomposition. Then we calculated, at various temperatures for the three studied scaling waters: CO2 partial pressures and loss of total carbon corresponding to the solubility products of CaCO3 hydrated forms. The results show that the partial pressure monitoring of the carbon dioxide is important in managing the behavior of scaling waters.

  14. Change in cap rock porosity triggered by pressure and temperature dependent CO2–water–rock interactions in CO2 storage systems

    Directory of Open Access Journals (Sweden)

    Christina Hemme

    2017-03-01

    Full Text Available Carbon capture and storage in deep geological formations is a method to reduce greenhouse gas emissions. Supercritical CO2 is injected into a reservoir and dissolves in the brine. Under the impact of pressure and temperature (P–T the aqueous species of the CO2-acidified brine diffuse through the cap rock where they trigger CO2–water–rock interactions. These geochemical reactions result in mineral dissolution and precipitation along the CO2 migration path and are responsible for a change in porosity and therefore for the sealing capacity of the cap rock. This study focuses on the diffusive mass transport of CO2 along a gradient of decreasing P–T conditions. The process is retraced with a one-dimensional hydrogeochemical reactive mass transport model. The semi-generic hydrogeochemical model is based on chemical equilibrium thermodynamics. Based on a broad variety of scenarios, including different initial mineralogical, chemical and physical parameters, the hydrogeochemical parameters that are most sensitive for safe long-term CO2 storage are identified. The results demonstrate that P–T conditions have the strongest effect on the change in porosity and the effect of both is stronger at high P–T conditions because the solubility of the mineral phases involved depends on P–T conditions. Furthermore, modeling results indicate that the change in porosity depends strongly on the initial mineralogical composition of the reservoir and cap rock as well as on the brine compositions. Nevertheless, a wide range of conditions for safe CO2 storage is identified.

  15. 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

    the onset of carbon deposition. The outlet gas composition at each current step was estimated based on the inlet gas composition and the reactant conversion using Faraday's law. The increase in voltage was observed at lower outlet pCO/pCO2 ratios than that corresponding to the expected thermodynamic......The carbon formation threshold in an operating cell was investigated during electrolysis of an idealized reactant atmosphere of CO and CO2. The electrolysis current was gradually increased in steps until the cell voltage spontaneously increased, thereby indicating cell degradation and possibly...

  16. Environmental Benign Synthesis of Lithium Silicates and Mg-Al Layered Double Hydroxide from Vermiculite Mineral for CO2 Capture

    Directory of Open Access Journals (Sweden)

    Yu Zhang

    2017-04-01

    Full Text Available This research introduces a completely new environmental benign synthesis route for obtaining two kinds of inter-mediate and high temperature CO2 sorbents, Mg-Al layered double hydroxide (LDH and Li4SiO4, from vermiculite. The mineral vermiculite was leached with acid, from which the obtained SiO2 was used for the synthesis of Li4SiO4 and the leaching waste water was used for the synthesis of Mg-Al LDH. Therefore, no waste was produced during the whole process. Both Li4SiO4 and Mg-Al LDH sorbents were carefully characterized using XRD, SEM, and BET analyses. The CO2 capturing performance of these two sorbents was comprehensively evaluated. The influence of the Li/Si ratio, calcination temperature, calcination time, and sorption temperature on the CO2 sorption capacity of Li4SiO4, and the sorption temperature on the CO2 sorption capacity of LDH, were investigated. The optimal leaching acid concentration for vermiculite and the CO2 sorption/desorption cycling performance of both the Li4SiO4 and Mg-Al LDH sorbents were determined. In sum, this demonstrated a unique and environment-friendly scheme for obtaining two CO2 sorbents from cheap raw materials, and this idea is applicable to the efficient utilization of other minerals.

  17. Nanophase Carbonates on Mars: Implications for Carbonate Formation and Habitability

    Science.gov (United States)

    Archer, P. Douglas, Jr.; Lauer, H. Vern; Ming, Douglas W.; Niles, Paul B.; Morris, Richard V.; Rampe, Elizabeth B.; Sutter, Brad

    2014-01-01

    Despite having an atmosphere composed primarily of CO2 and evidence for abundant water in the past, carbonate minerals have only been discovered in small amounts in martian dust [1], in outcrops of very limited extent [2, 3], in soils in the Northern Plains (the landing site of the 2007 Phoenix Mars Scout Mission) [4] and may have recently been detected in aeolian material and drilled and powdered sedimentary rock in Gale Crater (the Mars Science Laboratory [MSL] landing site) [5]. Thermal analysis of martian soils by instruments on Phoenix and MSL has demonstrated a release of CO2 at temperatures as low as 250-300 degC, much lower than the traditional decomposition temperatures of calcium or magnesium carbonates. Thermal decomposition temperature can depend on a number of factors such as instrument pressure and ramp rate, and sample particle size [6]. However, if the CO2 released at low temperatures is from carbonates, small particle size is the only effect that could have such a large impact on decomposition temperature, implying the presence of extremely fine-grained (i.e., "nanophase" or clay-sized) carbonates. We hypothesize that this lower temperature release is the signature of small particle-sized (clay-sized) carbonates formed by the weathering of primary minerals in dust or soils through interactions with atmospheric water and carbon dioxide and that this process may persist under current martian conditions. Preliminary work has shown that clay-sized carbonate grains can decompose at much lower temperatures than previously thought. The first work took carbonate, decomposed it to CaO, then flowed CO2 over these samples held at temperatures >100 degC to reform carbonates. Thermal analysis confirmed that carbonates were indeed formed and transmission electron microsopy was used to determine crystal sized were on the order of 10 nm. The next step used minerals such as diopside and wollastonite that were sealed in a glass tube with a CO2 and H2O source. After

  18. Carbonated water flooding : Process overview in the frame of co2 flooding

    NARCIS (Netherlands)

    Peksa, A.E.

    2017-01-01

    The main scope of the work related to the physical and dynamical processes associated with the injection of carbonated water in porous media. Carbonated water flooding is an alternative for traditional CO2 flooding. Both methods have the potential to recover any oil left behind after primary and

  19. New Technologies for Dealing with CO2 Emission and Carbonate Discharge Control Issues Associated with Energy Production

    Science.gov (United States)

    Tuwati, Abdulwahab

    Carbonates and bicarbonates as two water contaminants and CO2 as an air pollutant are the byproducts of a number of fossil fuel based energy production processes. It is well known that the eco-environmental impacts of the carbon based compounds are rather negative. Discharge of co-produced waters containing carbonates and bicarbonates can lead to the significant increase of alkalinity and sodicity and eventual degradation of the quality of soils. In addition, many studies have indicated that huge CO2 emission into the atmosphere can result in disastrous climate changes in the future. Therefore, people are increasingly interested in controlling these carbon compounds. A number of technologies such as ion exchange and electrodialysis have been developed for removal of carbonates and bicarbonates from co-produced waters. However, they are too expensive to be widely used by energy producers, farmers and ranchers. Although many approaches including membrane filtration have been explored for CO2 emission control, their costs are not acceptable to fossil fuel generating companies at all. Therefore, searching cost-effective methods for control of the carbon compounds have attracted many researchers' attentions. New technologies have been developed in this research to overcome the abovementioned challenges. For example, a regenerable solid sorbent (KTi) synthesized with K2CO3 and nanoporous TiO(OH)2 can be used to capture CO2. The CO2 sorption capacity of KTi is about 36 times higher than that of conventional K2CO3. The highest CO2 sorption capacity achieved with KTi is 1.69 mmol-CO2/g-KTi. It should be noted that the theoretical sorption capacity of the KTi can be as high as 3.32 mmol-CO 2/g-KTi. Therefore, the potential and improvement in CO2 sorption capacity with the use of nanoporous TiO(OH)2 is significant. Moreover, nanostructured KTi based CO2 separation (from flue gas) does not need additional high specific-heat capacity and high vaporization-enthalpy H2O. This

  20. An integrated study of fluid–rock interaction in a CO2-based enhanced geothermal system: A case study of Songliao Basin, China

    International Nuclear Information System (INIS)

    Na, Jin; Xu, Tianfu; Yuan, Yilong; Feng, Bo; Tian, Hailong; Bao, Xinhua

    2015-01-01

    Highlights: • We evaluated the interactions between rock, brine, and CO 2 in CO 2 -EGS using laboratory experiments. • We examined changes of the dissolved ionic composition of the solution. • Minerals dissolve (feldspar and calcite) or precipitate (secondly carbonates). • We used numerical simulations to reproduce chemical processes of CO 2 -EGS. • Numerical simulations were generally consistent with experimental results. - Abstract: The reactive behavior of a mixture of supercritical CO 2 and brine under physical–chemical conditions relevant to the CO 2 -based Enhanced Geothermal System (CO 2 -EGS) is largely unknown. Thus, laboratory experiments and numerical simulations were employed in this study to investigate the fluid–rock interaction occurring in the CO 2 -EGS. Rock samples and thermal–physical conditions specific to the Yingcheng Formation of Songliao Basin, China, an EGS research site, were used. Experiments were conducted by using of reactors at high temperature and pressure. Six batch reaction experiments injected with supercritical CO 2 were designed at temperatures of 150–170 °C and a pressure of 35 MPa. Moreover, a separate experiment at the same experimental conditions without injection of CO 2 was also conducted for comparison. Analyses of scanning electron microscopy (SEM) and X-ray diffraction (XRD) of the resulting solids were conducted to characterize changes in mineral phases. Numerical simulations were also performed under the same conditions as those used in the experiments. Significant mineral alterations were detected at the CO 2 -EGS reservoir, which may change the properties of fluid flow. The presence of supercritical CO 2 led to an dissolution of primary minerals such as calcite and K-feldspar and precipitations of secondary carbonate such as calcite and ankerite. The numerical simulations were generally consistent with laboratory experiments, which provide a tool for scaling the time up for long period of reservoir