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Sample records for co2 separation capture

  1. Evaluation of Mars CO2 Capture and Gas Separation Technologies

    NASA Technical Reports Server (NTRS)

    Muscatello, Anthony C.; Santiago-Maldonado, Edgardo; Gibson, Tracy; Devor, Robert; Captain, James

    2011-01-01

    Recent national policy statements have established that the ultimate destination of NASA's human exploration program is Mars. In Situ Resource Utilization (ISRU) is a key technology required to ,enable such missions and it is appropriate to review progress in this area and continue to advance the systems required to produce rocket propellant, oxygen, and other consumables on Mars using the carbon dioxide atmosphere and other potential resources. The Mars Atmospheric Capture and Gas separation project is selecting, developing, and demonstrating techniques to capture and purify Martian atmospheric gases for their utilization for the production of hydrocarbons, oxygen, and water in ISRU systems. Trace gases will be required to be separated from Martian atmospheric gases to provide pure CO2 to processing elements. In addition, other Martian gases, such as nitrogen and argon, occur in concentrations high enough to be useful as buffer gas and should be captured as well. To achieve these goals, highly efficient gas separation processes will be required. These gas separation techniques are also required across various areas within the ISRU project to support various consumable production processes. The development of innovative gas separation techniques will evaluate the current state-of-the-art for the gas separation required, with the objective to demonstrate and develop light-weight, low-power methods for gas separation. Gas separation requirements include, but are not limited to the selective separation of: (1) methane and water from unreacted carbon oxides (C02-CO) and hydrogen typical of a Sabatier-type process, (2) carbon oxides and water from unreacted hydrogen from a Reverse Water-Gas Shift process, (3)/carbon oxides from oxygen from a trash/waste processing reaction, and (4) helium from hydrogen or oxygen from a propellant scavenging process. Potential technologies for the separations include' freezers, selective membranes, selective solvents, polymeric sorbents

  2. Electric field controlled CO2 capture and CO2/N2 separation on MoS2 monolayers.

    PubMed

    Sun, Qiao; Qin, Gangqiang; Ma, Yingying; Wang, Weihua; Li, Ping; Du, Aijun; Li, Zhen

    2017-01-07

    Developing new materials and technologies for efficient CO2 capture, particularly for separation of CO2 post-combustion, will significantly reduce the CO2 concentration and its impacts on the environment. A challenge for CO2 capture is to obtain high performance adsorbents with both high selectivity and easy regeneration. Here, CO2 capture/regeneration on MoS2 monolayers controlled by turning on/off external electric fields is comprehensively investigated through a density functional theory calculation. The calculated results indicate that CO2 forms a weak interaction with MoS2 monolayers in the absence of an electric field, but strongly interacts with MoS2 monolayers when an electric field of 0.004 a.u. is applied. Moreover, the adsorbed CO2 can be released from the surface of MoS2 without any energy barrier once the electric field is turned off. Compared with the adsorption of CO2, the interactions between N2 and MoS2 are not affected significantly by the external electric fields, which indicates that MoS2 monolayers can be used as a robust absorbent for controllable capture of CO2 by applying an electric field, especially to separate CO2 from the post-combustion gas mixture where CO2 and N2 are the main components.

  3. Computational investigation of thermal gas separation for CO2 capture.

    SciTech Connect

    Gallis, Michail A.; Bryan, Charles R.; Brady, Patrick Vane; Torczynski, John Robert; Brooks, Carlton, F.

    2009-09-01

    This report summarizes the work completed under the Laboratory Directed Research and Development (LDRD) project 09-1351, 'Computational Investigation of Thermal Gas Separation for CO{sub 2} Capture'. Thermal gas separation for a binary mixture of carbon dioxide and nitrogen is investigated using the Direct Simulation Monte Carlo (DSMC) method of molecular gas dynamics. Molecular models for nitrogen and carbon dioxide are developed, implemented, compared to theoretical results, and compared to several experimental thermophysical properties. The molecular models include three translational modes, two fully excited rotational modes, and vibrational modes, whose degree of excitation depends on the temperature. Nitrogen has one vibrational mode, and carbon dioxide has four vibrational modes (two of which are degenerate). These models are used to perform a parameter study for mixtures of carbon dioxide and nitrogen confined between parallel walls over realistic ranges of gas temperatures and nominal concentrations of carbon dioxide. The degree of thermal separation predicted by DSMC is slightly higher than experimental values and is sensitive to the details of the molecular models.

  4. CO2 Capture Using Electrical Energy: Electrochemically Mediated Separation for Carbon Capture and Mitigation

    SciTech Connect

    2010-07-16

    IMPACCT Project: MIT and Siemens Corporation are developing a process to separate CO2 from the exhaust of coal-fired power plants by using electrical energy to chemically activate and deactivate sorbents, or materials that absorb gases. The team found that certain sorbents bond to CO2 when they are activated by electrical energy and then transported through a specialized separator that deactivates the molecule and releases it for storage. This method directly uses the electricity from the power plant, which is a more efficient but more expensive form of energy than heat, though the ease and simplicity of integrating it into existing coal-fired power plants reduces the overall cost of the technology. This process could cost as low as $31 per ton of CO2 stored.

  5. Dynamic Entangled Porous Framework for Hydrocarbon (C2-C3) Storage, CO2 Capture, and Separation.

    PubMed

    Sikdar, Nivedita; Bonakala, Satyanarayana; Haldar, Ritesh; Balasubramanian, Sundaram; Maji, Tapas Kumar

    2016-04-18

    Storage and separation of small (C1-C3) hydrocarbons are of great significance as these are alternative energy resources and also can be used as raw materials for many industrially important materials. Selective capture of greenhouse gas, CO2 from CH4 is important to improve the quality of natural gas. Among the available porous materials, MOFs with permanent porosity are the most suitable to serve these purposes. Herein, a two-fold entangled dynamic framework {[Zn2 (bdc)2 (bpNDI)]⋅4DMF}n with pore surface carved with polar functional groups and aromatic π clouds is exploited for selective capture of CO2 , C2, and C3 hydrocarbons at ambient condition. The framework shows stepwise CO2 and C2 H2 uptake at 195 K but type I profiles are observed at 298 K. The IAST selectivity of CO2 over CH4 is the highest (598 at 298 K) among the MOFs without open metal sites reported till date. It also shows high selectivity for C2 H2 , C2 H4 , C2 H6 , and C3 H8 over CH4 at 298 K. DFT calculations reveal that aromatic π surface and the polar imide (RNC=O) functional groups are the primary adsorption sites for adsorption. Furthermore, breakthrough column experiments showed CO2 /CH4 C2 H6 /CH4 and CO2 /N2 separation capability at ambient condition.

  6. CO2 CAPTURE PROJECT - AN INTEGRATED, COLLABORATIVE TECHNOLOGY DEVELOPMENT PROJECT FOR NEXT GENERATION CO2 SEPARATION, CAPTURE AND GEOLOGIC SEQUESTRATION

    SciTech Connect

    Dr. Helen Kerr

    2003-08-01

    The CO{sub 2} Capture Project (CCP) is a joint industry project, funded by eight energy companies (BP, ChevronTexaco, EnCana, Eni, Norsk Hydro, Shell, Statoil, and Suncor) and three government agencies (1) European Union (DG Res & DG Tren), (2) Norway (Klimatek) and (3) the U.S.A. (Department of Energy). The project objective is to develop new technologies, which could reduce the cost of CO{sub 2} capture and geologic storage by 50% for retrofit to existing plants and 75% for new-build plants. Technologies are to be developed to ''proof of concept'' stage by the end of 2003. The project budget is approximately $24 million over 3 years and the work program is divided into eight major activity areas: (1) Baseline Design and Cost Estimation--defined the uncontrolled emissions from each facility and estimate the cost of abatement in $/tonne CO{sub 2}. (2) Capture Technology, Post Combustion: technologies, which can remove CO{sub 2} from exhaust gases after combustion. (3) Capture Technology, Oxyfuel: where oxygen is separated from the air and then burned with hydrocarbons to produce an exhaust with high CO{sub 2} for storage. (4) Capture Technology, Pre -Combustion: in which, natural gas and petroleum coke are converted to hydrogen and CO{sub 2} in a reformer/gasifier. (5) Common Economic Model/Technology Screening: analysis and evaluation of each technology applied to the scenarios to provide meaningful and consistent comparison. (6) New Technology Cost Estimation: on a consistent basis with the baseline above, to demonstrate cost reductions. (7) Geologic Storage, Monitoring and Verification (SMV): providing assurance that CO{sub 2} can be safely stored in geologic formations over the long term. (8) Non-Technical: project management, communication of results and a review of current policies and incentives governing CO{sub 2} capture and storage. Technology development work dominated the past six months of the project. Numerous studies are making substantial progress

  7. CO2 Capture Project: An Integrated, Collaborative Technology Development Project For CO2 Separation, Capture And Geologic Sequestration

    SciTech Connect

    Helen Kerr

    2002-01-10

    This report (which forms part of the requirements of the Statement of Work Task 0, subtask 0.4) records progress towards defining a detailed Work Plan for the CCP 30 days after contract initiation. It describes the studies planned, workscope development and technology provider bid evaluation status at that time. Business sensitive information is provided separately in Appendix 1. Contract negotiations are on hold pending award of patent waiver status to the CCP.

  8. Porous materials as high performance adsorbents for CO2 capture, gas separation and purification

    NASA Astrophysics Data System (ADS)

    Wang, Jun

    Global warming resulted from greenhouse gases emission has received a widespread attention. Among the greenhouse gases, CO2 contributes more than 60% to global warming due to its huge emission amount. The flue gas contains about 15% CO2 with N2 as the balance. If CO2 can be separated from flue gas, the benefit is not only reducing the global warming effect, but also producing pure CO2 as a very useful industry raw material. Substantial progress is urgent to be achieved in an industrial process. Moreover, energy crisis is one of the biggest challenges for all countries due to the short life of fossil fuels, such as, petroleum will run out in 50 years and coal will run out in 150 years according to today's speed. Moreover, the severe pollution to the environment caused by burning fossil fuels requires us to explore sustainable, environment-friendly, and facile energy sources. Among several alternative energy sources, natural gas is one of the most promising alternative energy sources due to its huge productivity, abundant feed stock, and ease of generation. In order to realize a substantial adsorption process in industry, synthesis of new adsorbents or modification of existing adsorbent with improved properties has become the most critical issue. This dissertation reports systemic characterization and development of five serials of novel adsorbents with advanced adsorption properties. In chapter 2, nitrogen-doped Hypercross-linking Polymers (HCPs) have been synthesized successfully with non-carcinogenic chloromethyl methyl ether (CME) as the cross-linking agent within a single step. Texture properties, surface morphology, CO2/N2 selectivity, and adsorption heat have been presented and demonstrated properly. A comprehensive discussion on factors that affect the CO2 adsorption and CO2/N 2 separation has also been presented. It was found that high micropore proportion and N-content could effectively enhance CO2 uptake and CO2/N2 separation selectivity. In chapter 3, a

  9. CO2 Capture and Separations Using MOFs: Computational and Experimental Studies.

    PubMed

    Yu, Jiamei; Xie, Lin-Hua; Li, Jian-Rong; Ma, Yuguang; Seminario, Jorge M; Balbuena, Perla B

    2017-04-10

    This Review focuses on research oriented toward elucidation of the various aspects that determine adsorption of CO2 in metal-organic frameworks and its separation from gas mixtures found in industrial processes. It includes theoretical, experimental, and combined approaches able to characterize the materials, investigate the adsorption/desorption/reaction properties of the adsorbates inside such environments, screen and design new materials, and analyze additional factors such as material regenerability, stability, effects of impurities, and cost among several factors that influence the effectiveness of the separations. CO2 adsorption, separations, and membranes are reviewed followed by an analysis of the effects of stability, impurities, and process operation conditions on practical applications.

  10. Geological Sequestration Training and Research Program in Capture and Transport: Development of the Most Economical Separation Method for CO2 Capture

    SciTech Connect

    Vahdat, Nader

    2013-09-30

    The project provided hands-on training and networking opportunities to undergraduate students in the area of carbon dioxide (CO2) capture and transport, through fundamental research study focused on advanced separation methods that can be applied to the capture of CO2 resulting from the combustion of fossil-fuels for power generation . The project team’s approach to achieve its objectives was to leverage existing Carbon Capture and Storage (CCS) course materials and teaching methods to create and implement an annual CCS short course for the Tuskegee University community; conduct a survey of CO2 separation and capture methods; utilize data to verify and develop computer models for CO2 capture and build CCS networks and hands-on training experiences. The objectives accomplished as a result of this project were: (1) A comprehensive survey of CO2 capture methods was conducted and mathematical models were developed to compare the potential economics of the different methods based on the total cost per year per unit of CO2 avoidance; and (2) Training was provided to introduce the latest CO2 capture technologies and deployment issues to the university community.

  11. CO2 CAPTURE PROJECT-AN INTEGRATED, COLLABORATIVE TECHNOLOGY DEVELOPMENT PROJECT FOR NEXT GENERATION CO2 SEPARATION, CAPTURE AND GEOLOGIC SEQUESTRATION

    SciTech Connect

    Helen Kerr

    2004-04-01

    The CO{sub 2} Capture Project (CCP) is a joint industry project, funded by eight energy companies (BP, ChevronTexaco, EnCana, Eni, Norsk Hydro, Shell, Statoil, and Suncor) and three government agencies (European Union (DG Res & DG Tren), Norway (Klimatek) and the U.S.A. (Department of Energy)). The project objective is to develop new technologies, which could reduce the cost of CO{sub 2} capture and geologic storage by 50% for retrofit to existing plants and 75% for new-build plants. Technologies are to be developed to ''proof of concept'' stage by the end of 2003. The project budget is approximately $24 million over 3 years and the work program is divided into eight major activity areas: (1) Baseline Design and Cost Estimation--defined the uncontrolled emissions from each facility and estimate the cost of abatement in $/tonne CO{sub 2}. (2) Capture Technology, Post Combustion--technologies, which can remove CO{sub 2} from exhaust gases after combustion. (3) Capture Technology, Oxyfuel--where oxygen is separated from the air and then burned with hydrocarbons to produce an exhaust with wet high concentrations of CO{sub 2} for storage. (4) Capture Technology, Pre-Combustion--in which, natural gas and petroleum coke are converted to hydrogen and CO{sub 2} in a reformer/gasifier. (5) Common Economic Model/Technology Screening--analysis and evaluation of each technology applied to the scenarios to provide meaningful and consistent comparison. (6) New Technology Cost Estimation: on a consistent basis with the baseline above, to demonstrate cost reductions. (7) Geologic Storage, Monitoring and Verification (SMV)--providing assurance that CO{sub 2} can be safely stored in geologic formations over the long term. (8) Non-Technical: project management, communication of results and a review of current policies and incentives governing CO{sub 2} capture and storage. Technology development work dominated the past six months of the project. Numerous studies have completed their

  12. CO2 Capture Project-An Integrated, Collaborative Technology Development Project for Next Generation CO2 Separation, Capture and Geologic Sequestration

    SciTech Connect

    Helen Kerr; Linda M. Curran

    2005-04-15

    The CO{sub 2} Capture Project (CCP) was a joint industry project, funded by eight energy companies (BP, ChevronTexaco, EnCana, ENI, Norsk Hydro, Shell, Statoil, and Suncor) and three government agencies (European Union [DG RES & DG TREN], the Norwegian Research Council [Klimatek Program] and the U.S. Department of Energy [NETL]). The project objective was to develop new technologies that could reduce the cost of CO{sub 2} capture and geologic storage by 50% for retrofit to existing plants and 75% for new-build plants. Technologies were to be developed to ''proof of concept'' stage by the end of 2003. Certain promising technology areas were increased in scope and the studies extended through 2004. The project budget was approximately $26.4 million over 4 years and the work program is divided into eight major activity areas: Baseline Design and Cost Estimation--defined the uncontrolled emissions from each facility and estimate the cost of abatement in $/tonne CO{sub 2}. Capture Technology, Post Combustion: technologies, which can remove CO{sub 2} from exhaust gases after combustion. Capture Technology, Oxyfuel: where oxygen is separated from the air and then burned with hydrocarbons to produce an exhaust with high CO{sub 2} for storage. Capture Technology, Pre-Combustion: in which, natural gas and petroleum cokes are converted to hydrogen and CO{sub 2} in a reformer/gasifier. Common Economic Model/Technology Screening: analysis and evaluation of each technology applied to the scenarios to provide meaningful and consistent comparison. New Technology Cost Estimation: on a consistent basis with the baseline above, to demonstrate cost reductions. Geologic Storage, Monitoring and Verification (SMV): providing assurance that CO{sub 2} can be safely stored in geologic formations over the long term. Non-Technical: project management, communication of results and a review of current policies and incentives governing CO{sub 2} capture and storage. Pre-combustion De

  13. Amine scrubbing for CO2 capture.

    PubMed

    Rochelle, Gary T

    2009-09-25

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

  14. Capturing CO2 via reactions in nanopores.

    SciTech Connect

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

    2008-10-01

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

  15. Covalent Organic Frameworks for CO2 Capture.

    PubMed

    Zeng, Yongfei; Zou, Ruqiang; Zhao, Yanli

    2016-04-20

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

  16. Aminosilicone solvents for CO(2) capture.

    PubMed

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

    2010-08-23

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

  17. Separation and capture of CO2 from large stationary sources and sequestration in geological formations--coalbeds and deep saline aquifers.

    PubMed

    White, Curt M; Strazisar, Brian R; Granite, Evan J; Hoffman, James S; Pennline, Henry W

    2003-06-01

    The topic of global warming as a result of increased atmospheric CO2 concentration is arguably the most important environmental issue that the world faces today. It is a global problem that will need to be solved on a global level. The link between anthropogenic emissions of CO2 with increased atmospheric CO2 levels and, in turn, with increased global temperatures has been well established and accepted by the world. International organizations such as the United Nations Framework Convention on Climate Change (UNFCCC) and the Intergovernmental Panel on Climate Change (IPCC) have been formed to address this issue. Three options are being explored to stabilize atmospheric levels of greenhouse gases (GHGs) and global temperatures without severely and negatively impacting standard of living: (1) increasing energy efficiency, (2) switching to less carbon-intensive sources of energy, and (3) carbon sequestration. To be successful, all three options must be used in concert. The third option is the subject of this review. Specifically, this review will cover the capture and geologic sequestration of CO2 generated from large point sources, namely fossil-fuel-fired power gasification plants. Sequestration of CO2 in geological formations is necessary to meet the President's Global Climate Change Initiative target of an 18% reduction in GHG intensity by 2012. Further, the best strategy to stabilize the atmospheric concentration of CO2 results from a multifaceted approach where sequestration of CO2 into geological formations is combined with increased efficiency in electric power generation and utilization, increased conservation, increased use of lower carbon-intensity fuels, and increased use of nuclear energy and renewables. This review covers the separation and capture of CO2 from both flue gas and fuel gas using wet scrubbing technologies, dry regenerable sorbents, membranes, cryogenics, pressure and temperature swing adsorption, and other advanced concepts. Existing

  18. CO2 Capture with Enzyme Synthetic Analogue

    SciTech Connect

    Cordatos, Harry

    2010-03-01

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

  19. CO2 capture in different carbon materials.

    PubMed

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

    2012-07-03

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

  20. Monitoring solid oxide CO2 capture sorbents in action.

    PubMed

    Keturakis, Christopher J; Ni, Fan; Spicer, Michelle; Beaver, Michael G; Caram, Hugo S; Wachs, Israel E

    2014-12-01

    The separation, capture, and storage of CO2 , the major greenhouse gas, from industrial gas streams has received considerable attention in recent years because of concerns about environmental effects of increasing CO2 concentration in the atmosphere. An emerging area of research utilizes reversible CO2 sorbents to increase conversion and rate of forward reactions for equilibrium-controlled reactions (sorption-enhanced reactions). Little fundamental information, however, is known about the nature of the sorbent surface sites, sorbent surface-CO2 complexes, and the CO2 adsorption/desorption mechanisms. The present study directly spectroscopically monitors Na2 O/Al2 O3 sorbent-CO2 surface complexes during adsorption/desorption with simultaneous analysis of desorbed CO2 gas, allowing establishment of molecular level structure-sorption relationships between individual surface carbonate complexes and the CO2 working capacity of sorbents at different temperatures.

  1. Polymer nanosieve membranes for CO2-capture applications

    NASA Astrophysics Data System (ADS)

    Du, Naiying; Park, Ho Bum; Robertson, Gilles P.; Dal-Cin, Mauro M.; Visser, Tymen; Scoles, Ludmila; Guiver, Michael D.

    2011-05-01

    Microporous organic polymers (MOPs) are of potential significance for gas storage, gas separation and low-dielectric applications. Among many approaches for obtaining such materials, solution-processable MOPs derived from rigid and contorted macromolecular structures are promising because of their excellent mass transport and mass exchange capability. Here we show a class of amorphous MOP, prepared by [2+3] cycloaddition modification of a polymer containing an aromatic nitrile group with an azide compound, showing super-permeable characteristics and outstanding CO2 separation performance, even under polymer plasticization conditions such as CO2/light gas mixtures. This unprecedented result arises from the introduction of tetrazole groups into highly microporous polymeric frameworks, leading to more favourable CO2 sorption with superior affinity in gas mixtures, and selective CO2 transport by presorbed CO2 molecules that limit access by other light gas molecules. This strategy provides a direction in the design of MOP membrane materials for economic CO2 capture processes.

  2. CO2 Capture with Liquid-to-Solid Absorbents: CO2 Capture Process Using Phase-Changing Absorbents

    SciTech Connect

    2010-10-01

    IMPACCT Project: GE and the University of Pittsburgh are developing a unique CO2 capture process in which a liquid absorbent, upon contact with CO2, changes into a solid phase. Once in solid form, the material can be separated and the CO2 can be released for storage by heating. Upon heating, the absorbent returns to its liquid form, where it can be reused to capture more CO2. The approach is more efficient than other solventbased processes because it avoids the heating of extraneous solvents such as water. This ultimately leads to a lower cost of CO2 capture and will lower the additional cost to produce electricity for coal-fired power plants that retrofit their facilities to include this technology.

  3. Capture of CO2 From Recirculating Flue Gas Boilers

    SciTech Connect

    Ochs, Thomas L.

    2003-01-01

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

  4. Synergetic effect of carbon nanopore size and surface oxidation on CO2 capture from CO2/CH4 mixtures.

    PubMed

    Furmaniak, Sylwester; Kowalczyk, Piotr; Terzyk, Artur P; Gauden, Piotr A; Harris, Peter J F

    2013-05-01

    We have studied the synergetic effect of confinement (carbon nanopore size) and surface chemistry (the number of carbonyl groups) on CO2 capture from its mixtures with CH4 at typical operating conditions for industrial adsorptive separation (298 K and compressed CO2-CH4 mixtures). Although both confinement and surface oxidation have an impact on the efficiency of CO2/CH4 adsorptive separation at thermodynamics equilibrium, we show that surface functionalization is the most important factor in designing an efficient adsorbent for CO2 capture. Systematic Monte Carlo simulations revealed that adsorption of CH4 either pure or mixed with CO2 on oxidized nanoporous carbons is only slightly increased by the presence of functional groups (surface dipoles). In contrast, adsorption of CO2 is very sensitive to the number of carbonyl groups, which can be examined by a strong electric quadrupolar moment of CO2. Interestingly, the adsorbed amount of CH4 is strongly affected by the presence of the co-adsorbed CO2. In contrast, the CO2 uptake does not depend on the molar ratio of CH4 in the bulk mixture. The optimal carbonaceous porous adsorbent used for CO2 capture near ambient conditions should consist of narrow carbon nanopores with oxidized pore walls. Furthermore, the equilibrium separation factor was the greatest for CO2/CH4 mixtures with a low CO2 concentration. The maximum equilibrium separation factor of CO2 over CH4 of ~18-20 is theoretically predicted for strongly oxidized nanoporous carbons. Our findings call for a review of the standard uncharged model of carbonaceous materials used for the modeling of the adsorption separation processes of gas mixtures containing CO2 (and other molecules with strong electric quadrupolar moment or dipole moment).

  5. CO2 capture and separation from N2/CH4 mixtures by Co@B8/Co@B8(-) and M@B9/M@B9(-) (M = Ir, Rh, Ru) clusters: a theoretical study.

    PubMed

    Wang, Weihua; Zhang, Xiaoxiao; Li, Ping; Sun, Qiao; Li, Zhen; Ren, Cong; Guo, Chao

    2015-01-29

    The discovery of advanced materials with high selectivity and efficiency is essential to realize practical carbon capture and sequestration. Here, we have investigated the interactions of the Co@B8/Co@B8(-) and M@B9/M@B9(-) (M = Ir, Rh, Ru) clusters with CO2, N2, and CH4 gas molecules theoretically. We found that neutral boron clusters have weak interaction with CO2, N2, and CH4 molecules. Similarly, the clusters with their negative charge states have also weak interaction with N2 and CH4 molecules. However, anionic clusters have a strong interaction with CO2, which can be explained by the Lewis acid-base interaction as CO2 (Lewis acid) can gain electron easily from the electron-rich anionic clusters. Moreover, the kinetic stability of the formed complexes after CO2 capture has been validated by ab initio molecular dynamics. In all, the present study demonstrates, for the first time, that the anionic boron wheel ring clusters can be used as potential advanced materials for CO2 capture and separation from flue gas and natural gas mixtures.

  6. Enzyme-based CO2 capture for advanced life support

    NASA Technical Reports Server (NTRS)

    Ge, Jijun; Cowan, Robert M.; Tu, Chingkuang; McGregor, Martin L.; Trachtenberg, Michael C.

    2002-01-01

    Elevated CO2 levels in air can lead to impaired functioning and even death to humans. Control of CO2 is critical in confined spaces that have little physical or biological buffering capacity (e.g., spacecraft, submarines, or aircraft). A novel enzyme-based contained liquid membrane bioreactor was designed for CO2 capture and certain application cases are reported in this article. The results show that the liquid layer accounts for the major transport resistance. With addition of carbonic anhydrase, the transport resistance decreased by 71%. Volatile organic compounds of the type and concentration expected to be present in either the crew cabin or a plant growth chamber did not influence carbonic anhydrase activity or reactor operation during 1-day operation. Alternative sweep method studies, examined as a means of eliminating consumables, showed that the feed gas could be used successfully in a bypass mode when combined with medium vacuum pressure (-85 kPa) to achieve CO2 separation comparable to that with an inert sweep gas. The reactor exhibited a selectivity for CO2 versus N2 of 1400:1 and CO2 versus O2 is 866:1. The CO2 permeance was 1.44 x 10(-7) mol m-2 Pa-1 s-1 (4.3 x 10(-4) cm3 cm-2 s-1 cmHg-1) at a feed concentration of 0.1% CO2. These data show that the enzyme-based contained liquid membrane is a promising candidate technology that may be suitable for NASA applications to control CO2 in the crew or plant chambers.

  7. Fingerprinting captured CO2 using natural tracers: Determining CO2 fate and proving ownership

    NASA Astrophysics Data System (ADS)

    Flude, Stephanie; Gilfillan, Stuart; Johnston, Gareth; Stuart, Finlay; Haszeldine, Stuart

    2016-04-01

    In the long term, captured CO2 will most likely be stored in large saline formations and it is highly likely that CO2 from multiple operators will be injected into a single saline formation. Understanding CO2 behavior within the reservoir is vital for making operational decisions and often uses geochemical techniques. Furthermore, in the event of a CO2 leak, being able to identify the owner of the CO2 is of vital importance in terms of liability and remediation. Addition of geochemical tracers to the CO2 stream is an effective way of tagging the CO2 from different power stations, but may become prohibitively expensive at large scale storage sites. Here we present results from a project assessing whether the natural isotopic composition (C, O and noble gas isotopes) of captured CO2 is sufficient to distinguish CO2 captured using different technologies and from different fuel sources, from likely baseline conditions. Results include analytical measurements of CO2 captured from a number of different CO2 capture plants and a comprehensive literature review of the known and hypothetical isotopic compositions of captured CO2 and baseline conditions. Key findings from the literature review suggest that the carbon isotope composition will be most strongly controlled by that of the feedstock, but significant fractionation is possible during the capture process; oxygen isotopes are likely to be controlled by the isotopic composition of any water used in either the industrial process or the capture technology; and noble gases concentrations will likely be controlled by the capture technique employed. Preliminary analytical results are in agreement with these predictions. Comparison with summaries of likely storage reservoir baseline and shallow or surface leakage reservoir baseline data suggests that C-isotopes are likely to be valuable tracers of CO2 in the storage reservoir, while noble gases may be particularly valuable as tracers of potential leakage.

  8. CO2 Capture with Enzyme Synthetic Analogue

    SciTech Connect

    Cordatos, Harry

    2010-11-08

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

  9. Enhancing CO2 Capture using Robust Superomniphobic Membranes.

    PubMed

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

    2017-02-01

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

  10. Alkylamine-tethered stable metal-organic framework for CO(2) capture from flue gas.

    PubMed

    Hu, Yingli; Verdegaal, Wolfgang M; Yu, Shu-Hong; Jiang, Hai-Long

    2014-03-01

    Different alkylamine molecules were post-synthetically tethered to the unsaturated Cr(III) centers in the metal-organic framework MIL-101. The resultant metal-organic frameworks show almost no N2 adsorption with significantly enhanced CO2 capture under ambient conditions as a result of the interaction between amine groups and CO2 molecules. Given the extraordinary stability, high CO2 uptake, ultrahigh CO2 /N2 selectivity, and mild regeneration energy, MIL-101-diethylenetriamine holds exceptional promise for post-combustion CO2 capture and CO2 /N2 separation.

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

    SciTech Connect

    2010-07-01

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

  12. Halloysite nanotubes capturing isotope selective atmospheric CO2.

    PubMed

    Jana, Subhra; Das, Sankar; Ghosh, Chiranjit; Maity, Abhijit; Pradhan, Manik

    2015-03-04

    With the aim to capture and subsequent selective trapping of CO2, a nanocomposite has been developed through selective modification of the outer surface of the halloysite nanotubes (HNTs) with an organosilane to make the nanocomposite a novel solid-phase adsorbent to adsorb CO2 from the atmosphere at standard ambient temperature and pressure. The preferential adsorption of three major abundant isotopes of CO2 ((12)C(16)O2, (13)C(16)O2, and (12)C(16)O(18)O) from the ambient air by amine functionalized HNTs has been explored using an optical cavity-enhanced integrated cavity output spectroscopy. CO2 adsorption/desorption cycling measurements demonstrate that the adsorbent can be regenerated at relatively low temperature and thus, recycled repeatedly to capture atmospheric CO2. The amine grafted halloysite shows excellent stability even in oxidative environments and has high efficacy of CO2 capture, introducing a new route to the adsorption of isotope selective atmospheric CO2.

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

    PubMed

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

    2017-01-19

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

  14. Economic and energetic analysis of capturing CO2 from ambient air.

    PubMed

    House, Kurt Zenz; Baclig, Antonio C; Ranjan, Manya; van Nierop, Ernst A; Wilcox, Jennifer; Herzog, Howard J

    2011-12-20

    Capturing carbon dioxide from the atmosphere ("air capture") in an industrial process has been proposed as an option for stabilizing global CO(2) concentrations. Published analyses suggest these air capture systems may cost a few hundred dollars per tonne of CO(2), making it cost competitive with mainstream CO(2) mitigation options like renewable energy, nuclear power, and carbon dioxide capture and storage from large CO(2) emitting point sources. We investigate the thermodynamic efficiencies of commercial separation systems as well as trace gas removal systems to better understand and constrain the energy requirements and costs of these air capture systems. Our empirical analyses of operating commercial processes suggest that the energetic and financial costs of capturing CO(2) from the air are likely to have been underestimated. Specifically, our analysis of existing gas separation systems suggests that, unless air capture significantly outperforms these systems, it is likely to require more than 400 kJ of work per mole of CO(2), requiring it to be powered by CO(2)-neutral power sources in order to be CO(2) negative. We estimate that total system costs of an air capture system will be on the order of $1,000 per tonne of CO(2), based on experience with as-built large-scale trace gas removal systems.

  15. Economic and energetic analysis of capturing CO2 from ambient air

    PubMed Central

    House, Kurt Zenz; Baclig, Antonio C.; Ranjan, Manya; van Nierop, Ernst A.; Wilcox, Jennifer; Herzog, Howard J.

    2011-01-01

    Capturing carbon dioxide from the atmosphere (“air capture”) in an industrial process has been proposed as an option for stabilizing global CO2 concentrations. Published analyses suggest these air capture systems may cost a few hundred dollars per tonne of CO2, making it cost competitive with mainstream CO2 mitigation options like renewable energy, nuclear power, and carbon dioxide capture and storage from large CO2 emitting point sources. We investigate the thermodynamic efficiencies of commercial separation systems as well as trace gas removal systems to better understand and constrain the energy requirements and costs of these air capture systems. Our empirical analyses of operating commercial processes suggest that the energetic and financial costs of capturing CO2 from the air are likely to have been underestimated. Specifically, our analysis of existing gas separation systems suggests that, unless air capture significantly outperforms these systems, it is likely to require more than 400 kJ of work per mole of CO2, requiring it to be powered by CO2-neutral power sources in order to be CO2 negative. We estimate that total system costs of an air capture system will be on the order of $1,000 per tonne of CO2, based on experience with as-built large-scale trace gas removal systems. PMID:22143760

  16. Acid Gas Capture Using CO2-Binding Organic Liquids

    SciTech Connect

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

    2010-11-10

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

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

    PubMed

    Ko, Young Gun; Shin, Seung Su; Choi, Ung Su

    2011-09-15

    CO(2) emissions, from fossil-fuel-burning power plants, the breathing, etc., influence the global worming on large scale and the man's work efficiency on small scale. The reversible capture of CO(2) is a prominent feature of CO(2) organic-inorganic hybrid adsorbent to sequester CO(2). Herein, (3-aminopropyl) trimethoxysilane (APTMS), [3-(methylamino)propyl] trimethoxysilane (MAPTMS), and [3-(diethylamino) propyl] trimethoxysilane (DEAPTMS) are immobilized on highly ordered mesoporous silicas (SBA-15) to catch CO(2) as primary, secondary, and tertiary aminosilica adsorbents. X-ray photoelectron spectroscopy was used to analyze the immobilized APTMS, MAPTMS, and DEAPTMS on the SBA-15. We report an interesting discovery that the CO(2) adsorption and desorption on the adsorbent depend on the amine type of the aminosilica adsorbent. The adsorbed CO(2) was easily desorbed from the adsorbent with the low energy consumption in the order of tertiary, secondary, and primary amino-adsorbents while the adsorption amount and the bonding-affinity increased in the reverse order. The effectiveness of amino-functionalized (1(o), 2(o), and 3(o) amines) SBA-15s as a CO(2) capturing agent was investigated in terms of adsorption capacity, adsorption-desorption kinetics, and thermodynamics. This work demonstrates apt amine types to catch CO(2) and regenerate the adsorbent, which may open new avenues to designing "CO(2) basket".

  18. Simteche Hydrate CO2 Capture Process

    SciTech Connect

    Nexant and Los Alamos National Laboratory

    2006-09-30

    As a result of an August 4, 2005 project review meeting held at Los Alamos National Laboratory (LANL) to assess the project's technical progress, Nexant/Simteche/LANL project team was asked to meet four targets related to the existing project efforts. The four targets were to be accomplished by the September 30, 2006. These four targets were: (1) The CO{sub 2} hydrate process needs to show, through engineering and sensitivity analysis, that it can achieve 90% CO{sub 2} capture from the treated syngas stream, operating at 1000 psia. The cost should indicate the potential of achieving the Sequestration Program's cost target of less than 10% increase in the cost of electricity (COE) of the non-CO{sub 2} removal IGCC plant or demonstrate a significant cost reduction from the Selexol process cost developed in the Phase II engineering analysis. (2) The ability to meet the 20% cost share requirement for research level efforts. (3) LANL identifies through equilibrium and bench scale testing a once-through 90% CO{sub 2} capture promoter that supports the potential to achieve the Sequestration Program's cost target. Nexant is to perform an engineering analysis case to verify any economic benefits, as needed; no ETM validation is required, however, for this promoter for FY06. (4) The CO{sub 2} hydrate once-through process is to be validated at 1000 psia with the ETM at a CO{sub 2} capture rate of 60% without H{sub 2}S. The performance of 68% rate of capture is based on a batch, equilibrium data with H{sub 2}S. Validation of the test results is required through multiple runs and engineering calculations. Operational issues will be solved that will specifically effect the validation of the technology. Nexant was given the primary responsibility for Target No.1, while Simteche was mainly responsible for Target No.2; with LANL having the responsibility of Targets No.3 and No.4.

  19. Amine-based CO2 capture technology development from the beginning of 2013-a review.

    PubMed

    Dutcher, Bryce; Fan, Maohong; Russell, Armistead G

    2015-02-04

    It is generally accepted by the scientific community that anthropogenic CO2 emissions are leading to global climate change, notably an increase in global temperatures commonly referred to as global warming. The primary source of anthropogenic CO2 emissions is the combustion of fossil fuels for energy. As society's demand for energy increases and more CO2 is produced, it becomes imperative to decrease the amount emitted to the atmosphere. One promising approach to do this is to capture CO2 at the effluent of the combustion site, namely, power plants, in a process called postcombustion CO2 capture. Technologies to achieve this are heavily researched due in large part to the intuitive nature of removing CO2 from the stack gas and the ease in retrofitting existing CO2 sources with these technologies. As such, several reviews have been written on postcombustion CO2 capture. However, it is a fast-developing field, and the most recent review papers already do not include the state-of-the-art research. Notable among CO2 capture technologies are amine-based technologies. Amines are well-known for their reversible reactions with CO2, which make them ideal for the separation of CO2 from many CO2-containing gases, including flue gas. For this reason, this review will cover amine-based technology developed and published in and after the year 2013.

  20. CO2-Binding-Organic-Liquids-Enhanced CO2 Capture using Polarity-Swing-Assisted Regeneration

    SciTech Connect

    Zhang, Jian; Kutnyakov, Igor; Koech, Phillip K.; Zwoster, Andy; Howard, Chris; Zheng, Feng; Freeman, Charles J.; Heldebrant, David J.

    2013-01-01

    A new solvent-based CO2 capture process couples the unique attributes of non-aqueous, CO2-binding organic liquids (CO2BOLs) with the newly discovered polarity-swing-assisted regeneration (PSAR) process that is unique to switchable ionic liquids. Laboratory measurements with PSAR indicate the ability to achieve a regeneration effect at 75°C comparable to that at 120°C using thermal regeneration only. Initial measurements also indicate that the kinetic behavior of CO2 release is also improved with PSAR. Abstract cleared PNWD-SA-9743

  1. Conductive Graphitic Carbon Nitride as an Ideal Material for Electrocatalytically Switchable CO2 Capture

    PubMed Central

    Tan, Xin; Kou, Liangzhi; Tahini, Hassan A.; Smith, Sean C.

    2015-01-01

    Good electrical conductivity and high electron mobility of the sorbent materials are prerequisite for electrocatalytically switchable CO2 capture. However, no conductive and easily synthetic sorbent materials are available until now. Here, we examined the possibility of conductive graphitic carbon nitride (g-C4N3) nanosheets as sorbent materials for electrocatalytically switchable CO2 capture. Using first-principle calculations, we found that the adsorption energy of CO2 molecules on g-C4N3 nanosheets can be dramatically enhanced by injecting extra electrons into the adsorbent. At saturation CO2 capture coverage, the negatively charged g-C4N3 nanosheets achieve CO2 capture capacities up to 73.9 × 1013 cm−2 or 42.3 wt%. In contrast to other CO2 capture approaches, the process of CO2 capture/release occurs spontaneously without any energy barriers once extra electrons are introduced or removed, and these processes can be simply controlled and reversed by switching on/off the charging voltage. In addition, these negatively charged g-C4N3 nanosheets are highly selective for separating CO2 from mixtures with CH4, H2 and/or N2. These predictions may prove to be instrumental in searching for a new class of experimentally feasible high-capacity CO2 capture materials with ideal thermodynamics and reversibility. PMID:26621618

  2. Conductive Graphitic Carbon Nitride as an Ideal Material for Electrocatalytically Switchable CO2 Capture

    NASA Astrophysics Data System (ADS)

    Tan, Xin; Kou, Liangzhi; Tahini, Hassan A.; Smith, Sean C.

    2015-12-01

    Good electrical conductivity and high electron mobility of the sorbent materials are prerequisite for electrocatalytically switchable CO2 capture. However, no conductive and easily synthetic sorbent materials are available until now. Here, we examined the possibility of conductive graphitic carbon nitride (g-C4N3) nanosheets as sorbent materials for electrocatalytically switchable CO2 capture. Using first-principle calculations, we found that the adsorption energy of CO2 molecules on g-C4N3 nanosheets can be dramatically enhanced by injecting extra electrons into the adsorbent. At saturation CO2 capture coverage, the negatively charged g-C4N3 nanosheets achieve CO2 capture capacities up to 73.9 × 1013 cm-2 or 42.3 wt%. In contrast to other CO2 capture approaches, the process of CO2 capture/release occurs spontaneously without any energy barriers once extra electrons are introduced or removed, and these processes can be simply controlled and reversed by switching on/off the charging voltage. In addition, these negatively charged g-C4N3 nanosheets are highly selective for separating CO2 from mixtures with CH4, H2 and/or N2. These predictions may prove to be instrumental in searching for a new class of experimentally feasible high-capacity CO2 capture materials with ideal thermodynamics and reversibility.

  3. Conductive Graphitic Carbon Nitride as an Ideal Material for Electrocatalytically Switchable CO2 Capture.

    PubMed

    Tan, Xin; Kou, Liangzhi; Tahini, Hassan A; Smith, Sean C

    2015-12-01

    Good electrical conductivity and high electron mobility of the sorbent materials are prerequisite for electrocatalytically switchable CO2 capture. However, no conductive and easily synthetic sorbent materials are available until now. Here, we examined the possibility of conductive graphitic carbon nitride (g-C4N3) nanosheets as sorbent materials for electrocatalytically switchable CO2 capture. Using first-principle calculations, we found that the adsorption energy of CO2 molecules on g-C4N3 nanosheets can be dramatically enhanced by injecting extra electrons into the adsorbent. At saturation CO2 capture coverage, the negatively charged g-C4N3 nanosheets achieve CO2 capture capacities up to 73.9 × 10(13) cm(-2) or 42.3 wt%. In contrast to other CO2 capture approaches, the process of CO2 capture/release occurs spontaneously without any energy barriers once extra electrons are introduced or removed, and these processes can be simply controlled and reversed by switching on/off the charging voltage. In addition, these negatively charged g-C4N3 nanosheets are highly selective for separating CO2 from mixtures with CH4, H2 and/or N2. These predictions may prove to be instrumental in searching for a new class of experimentally feasible high-capacity CO2 capture materials with ideal thermodynamics and reversibility.

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

    PubMed

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

    2016-07-27

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

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

    SciTech Connect

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

    2007-06-01

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

  6. CO(2) capture from dilute gases as a component of modern global carbon management.

    PubMed

    Jones, Christopher W

    2011-01-01

    The growing atmospheric CO(2) concentration and its impact on climate have motivated widespread research and development aimed at slowing or stemming anthropogenic carbon emissions. Technologies for carbon capture and sequestration (CCS) employing mass separating agents that extract and purify CO(2) from flue gas emanating from large point sources such as fossil fuel-fired electricity-generating power plants are under development. Recent advances in solvents, adsorbents, and membranes for postcombust- ion CO(2) capture are described here. Specifically, room-temperature ionic liquids, supported amine materials, mixed matrix and facilitated transport membranes, and metal-organic framework materials are highlighted. In addition, the concept of extracting CO(2) directly from ambient air (air capture) as a means of reducing the global atmospheric CO(2) concentration is reviewed. For both conventional CCS from large point sources and air capture, critical research needs are identified and discussed.

  7. Halloysite Nanotubes Capturing Isotope Selective Atmospheric CO2

    PubMed Central

    Jana, Subhra; Das, Sankar; Ghosh, Chiranjit; Maity, Abhijit; Pradhan, Manik

    2015-01-01

    With the aim to capture and subsequent selective trapping of CO2, a nanocomposite has been developed through selective modification of the outer surface of the halloysite nanotubes (HNTs) with an organosilane to make the nanocomposite a novel solid-phase adsorbent to adsorb CO2 from the atmosphere at standard ambient temperature and pressure. The preferential adsorption of three major abundant isotopes of CO2 (12C16O2, 13C16O2, and 12C16O18O) from the ambient air by amine functionalized HNTs has been explored using an optical cavity-enhanced integrated cavity output spectroscopy. CO2 adsorption/desorption cycling measurements demonstrate that the adsorbent can be regenerated at relatively low temperature and thus, recycled repeatedly to capture atmospheric CO2. The amine grafted halloysite shows excellent stability even in oxidative environments and has high efficacy of CO2 capture, introducing a new route to the adsorption of isotope selective atmospheric CO2. PMID:25736700

  8. CO2 Capture Using Phase-Changing Sorbents

    SciTech Connect

    Perry, RJ; Wood, BR; Genovese, S; O'Brien, MJ; Westendorf, T; Meketa, ML; Farnum, R; McDermott, J; Sultanova, I; Perry, TM; Vipperla, RK; Wichmann, LA; Enick, RM; Hong, L; Tapriyal, D

    2012-04-01

    A novel method for the postcombustion capture of CO2 from coal-fired power plants has been described utilizing an aminosilicone absorbent. 1,3-Bis(3-aminopropy1)-1,1,3,3-tetramethyldsiloxane (GAP-0) rapidly transforms from a low viscosity liquid to a friable solid upon exposure to CO2 in simulated flue gas. This material has excellent thermal stability, low vapor pressure, high CO2 loading capability, and a large dynamic CO2 capacity between rich and lean solvent loadings. Preliminary plant and process models assembled from experimental data show a decrease in parasitic energy loss from 30% to 18% when compared to the benchmark monoethanolamine (MEA) process and a concomitant lowering of the cost of electricity (COE) from 74% to 44% increase versus a plant without carbon capture.

  9. CO2 capture using zeolite 13X prepared from bentonite

    NASA Astrophysics Data System (ADS)

    Chen, Chao; Park, Dong-Wha; Ahn, Wha-Seung

    2014-02-01

    Zeolite 13X was prepared using bentonite as the raw material by alkaline fusion followed by a hydrothermal treatment without adding any extra silica or alumina sources. The prepared zeolite 13X was characterized by X-ray powder diffraction, N2-adsorption-desorption measurements, and scanning electron microscopy. The CO2 capture performance of the prepared zeolite 13X was examined under both static and flow conditions. The prepared zeolite 13X showed a high BET surface area of 688 m2/g with a high micropore volume (0.30 cm3/g), and exhibited high CO2 capture capacity (211 mg/g) and selectivity to N2 (CO2/N2 = 37) at 25 °C and 1 bar. In addition, the material showed fast adsorption kinetics, and stable CO2 adsorption-desorption recycling performance at both 25 and 200 °C.

  10. Geologic CO2 Capture via Reaction of Seawater with Peridotite

    NASA Astrophysics Data System (ADS)

    Kelemen, P. B.

    2010-12-01

    Increasing atmospheric CO2 occurring at or above predicted rates, together with slow progress on US and international support for CO2 capture and storage, renders it likely that CO2 levels in the atmosphere will reach 500 ppmv or more, which may be too high to sustain an acceptable standard of living. Thus, “negative CO2 emissions” may become necessary. Kelemen & Matter (PNAS 2008) proposed reaction of seawater with peridotite in situ as a route to negative emissions. Drilling and fracturing exposed peridotite beneath the seafloor would stimulate porous, thermal convection of seawater. Reaction would remove CO2 from the water, forming solid carbonates. Return of CO2-depleted water to the sea surface would draw down atmospheric CO2. This combines geologic CO2 capture and solid storage, and avoids the cost of industrial CO2 capture, transport and injection. Here I quantify this proposed method. Peridotite reacts with surface waters to form hydrous silicates and solid carbonate minerals such as magnesite, dolomite and calcite. Fully carbonated peridotite - in which all Mg and Ca form carbonate minerals - contains about 35 wt% CO2; 1 km3 of carbonated peridotite can contain up to ~ 1 Gt of CO2. Geologic examples demonstrate that full carbonation is possible. Plate tectonics brings mantle peridotite from beneath the crust to the surface. Most is present near slow-spreading mid-ocean ridges. These ridges have a collective length of more than 60,000 km and form ~ 8 million km3 of oceanic crust per million years given a 7 km thickness. Newly formed crust flanking slow spreading ridges is 5-15% peridotite. It is gradually buried by sediments, but is within 100 m of the seafloor for more than 10 km on either side of the ridge (~ 106 Gt of accessible peridotite within 3 km of the seafloor). Onland exposures of peridotite include thrust slices of oceanic crust and upper mantle known as ophiolites. The largest, the Oman ophiolite, contains about 16,000 km3 of peridotite

  11. Diamino protic ionic liquids for CO2 capture.

    PubMed

    Vijayraghavan, R; Pas, Steven J; Izgorodina, Ekaterina I; MacFarlane, Douglas R

    2013-12-14

    A series of multifunctional protic ionic liquids (PILs), some of which are based on a combination of primary and tertiary amines in the same moiety coupled with a carboxylic acid, have been synthesised and employed for CO2 capture, yielding absorption capacities comparable to standard absorbents. In contrast to traditional amine absorbers, CO2 was found to desorb at lower temperatures and hence could result in a significant reduction in both the energy required to strip the absorber of CO2 and the thermally activated degradation mechanisms, which in traditional absorbers result in the loss of absorber and the production of toxic compounds. The lower basicity of the amine sites resultant from PIL formation decreases the binding energy of the CO2 to the absorber. The weaker basicity is also evidenced by lower pH of the PIL CO2 absorbers, which reduces common corrosion problems associated with traditional amine absorbers.

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

    PubMed

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

    2008-11-01

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

  13. Industrial CO2 Removal: CO2 Capture from Ambient Air and Geological Sequestration

    SciTech Connect

    Dooley, James J.

    2011-06-08

    This abstract and its accompanying presentation will provide an overview of two distinct industrial processes for removing carbon dioxide (CO2) from the atmosphere as a means of addressing anthropogenic climate change. The first of these is carbon dioxide capture and storage (CCS) coupled with large scale biomass production (hereafter referred to as bioCCS). The second is CO2 capture from ambient air via industrial systems (hereafter referred to as direct air capture (DAC)). In both systems, the captured CO2 would be injected into deep geologic formations so as to isolate it from the atmosphere. The technical literature is clear that both of these technologies are technically feasible as of today (IPCC, 2005; Keith, 2009; Lackner, 2009; Luckow et al., 2010; Ranjan and Herzog, 2011). What is uncertain is the relative cost of these industrial ambient-air CO2 removal systems when compared to other emissions mitigation measures, the ultimate timing and scale of their deployment, and the resolution of potential site specific constraints that would impact their ultimate commercial deployment.

  14. Direct Capture of CO2 from Ambient Air.

    PubMed

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

    2016-10-12

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

  15. Separation of CO2 from flue gas using electrochemical cells

    SciTech Connect

    Pennline, H.W; Granite, E.J.; Luebke, D.R; Kitchin, J.R; Landon, J.; Weiland, L.M.

    2010-06-01

    ABSTRACT Past research with high temperature molten carbonate electrochemical cells has shown that carbon dioxide can be separated from flue gas streams produced by pulverized coal combustion for power generation, However, the presence of trace contaminants, i.e" sulfur dioxide and nitric oxides, will impact the electrolyte within the cell. If a lower temperature cell could be devised that would utilize the benefits of commercially-available, upstream desulfurization and denitrification in the power plant, then this CO2 separation technique can approach more viability in the carbon sequestration area, Recent work has led to the assembly and successful operation of a low temperature electrochemical cell. In the proof-of-concept testing with this cell, an anion exchange membrane was sandwiched between gas-diffusion electrodes consisting of nickel-based anode electrocatalysts on carbon paper. When a potential was applied across the cell and a mixture of oxygen and carbon dioxide was flowed over the wetted electrolyte on the cathode side, a stream of CO2 to O2 was produced on the anode side, suggesting that carbonate/ bicarbonate ions are the CO2 carrier in the membrane. Since a mixture of CO 2 and 02 is produced, the possibility exists to use this stream in oxy-firing of additional fuel. From this research, a novel concept for efficiently producing a carbon dioxide rich effiuent from combustion of a fossil fuel was proposed. Carbon dioxide and oxygen are captured from the flue gas of a fossilfuel combustor by one or more electrochemical cells or cell stacks. The separated stream is then transferred to an oxy-fired combustor which uses the gas stream for ancillary combustion, ultimately resulting in an effluent rich in carbon dioxide, A portion of the resulting flow produced by the oxy-fired combustor may be continuously recycled back into the oxy-fired combustor for temperature control and an optimal carbon dioxide rich effluent.

  16. Charge-controlled switchable CO2 capture on boron nitride nanomaterials.

    PubMed

    Sun, Qiao; Li, Zhen; Searles, Debra J; Chen, Ying; Lu, Gaoqing Max; Du, Aijun

    2013-06-05

    Increasing concerns about the atmospheric CO2 concentration and its impact on the environment are motivating researchers to discover new materials and technologies for efficient CO2 capture and conversion. Here, we report a study of the adsorption of CO2, CH4, and H2 on boron nitride (BN) nanosheets and nanotubes (NTs) with different charge states. The results show that the process of CO2 capture/release can be simply controlled by switching on/off the charges carried by BN nanomaterials. CO2 molecules form weak interactions with uncharged BN nanomaterials and are weakly adsorbed. When extra electrons are introduced to these nanomaterials (i.e., when they are negatively charged), CO2 molecules become tightly bound and strongly adsorbed. Once the electrons are removed, CO2 molecules spontaneously desorb from BN absorbents. In addition, these negatively charged BN nanosorbents show high selectivity for separating CO2 from its mixtures with CH4 and/or H2. Our study demonstrates that BN nanomaterials are excellent absorbents for controllable, highly selective, and reversible capture and release of CO2. In addition, the charge density applied in this study is of the order of 10(13) cm(-2) of BN nanomaterials and can be easily realized experimentally.

  17. Surface modification of activated carbons for CO 2 capture

    NASA Astrophysics Data System (ADS)

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

    2008-09-01

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

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

    SciTech Connect

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

    2010-08-31

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

  19. Capturing CO2 into the precipitate of a phase-changing solvent after absorption.

    PubMed

    Zheng, Shudong; Tao, Mengna; Liu, Qing; Ning, Liqi; He, Yi; Shi, Yao

    2014-01-01

    The major drawback of aqueous alkanolamine-based CO2 capture processes is the high energy penalty for regeneration. To overcome this weakness, we studied the absorption of CO2 with amines dissolved in nonaqueous solvents. It was observed that triethylenetetramine (TETA) dissolved in ethanol produces a solid precipitate after absorption, which can then be easily separated and regenerated. As a comparison, a TETA/water solution does not form any precipitate after absorbing CO2. The TETA/ethanol solution offers several advantages for CO2 capture in absorption rate, absorption capacity, and absorbent regenerability. Both the rate and capacity of CO2 absorption with the TETA/ethanol solution were significantly higher than with a TETA/water solution, because ethanol not only promotes the solubility of CO2 in the liquid phase but also facilitates the chemical reaction between TETA and CO2. This approach was able to capture 81.8% of the absorbed CO2 in the solid phase as TETA-carbamate. In addition, results show that the decomposition of TETA-carbamate can be completed at 90 °C. Moreover, the cycling absorption/regeneration runs of the TETA/ethanol solution display a relatively stable absorption performance.

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

    DOE PAGES

    Seipp, Charles A.; Univ. of Texas, Austin, TX; Williams, Neil J.; ...

    2016-12-21

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

  1. Choosing amine-based absorbents for CO2 capture.

    PubMed

    Gomes, João; Santos, Samuel; Bordado, João

    2015-01-01

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

  2. CO2 capture systems based on saccharides and organic superbases.

    PubMed

    Carrera, G V S M; Jordão, N; Branco, L C; Nunes da Ponte, M

    2015-01-01

    In this report, novel systems, based on highly abundant saccharides, D-mannose, D-glucose, β-cyclodextrin, alginic acid and mannitol, in combination with an organic superbase, tetramethylguanidine (TMG) or 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU), are studied for carbon dioxide capture. With D-mannose and D-glucose, several ratios of equivalents of alcohol groups of saccharide : superbase were tested: 1, 0.625, 0.5 and 0.25. High wt% values of CO2 uptake were obtained with TMG-based systems. However, TMG itself can react directly with CO2, and, in the presence of D-mannose, competition between carbonate and carbamate based products was established. In order to circumvent this competition and obtain exclusively the carbonate-based product, DBU was used instead as an organic superbase. In the D-mannose series the highest result was obtained with a D-mannose : DBU ratio eq. = 0.625 (13.9% CO2 uptake, 3.3/5 alcohol groups converted into carbonates). A more effective stirring system, designed to overcome the high viscosity of the products, allowed the use of a D-glucose : DBU = 1 : 1 ratio with 11.5 wt% of CO2 uptake and 2.47/5 alcohol groups converted into carbonates. Additionally a DSC thermal study was performed in order to study the stability/reversibility of the CO2 loaded systems.

  3. Synthesis of sintering-resistant sorbents for CO2 capture.

    PubMed

    Liu, Wenqiang; Feng, Bo; Wu, Yueqin; Wang, Guoxiong; Barry, John; da Costa, João C Diniz

    2010-04-15

    Sorbents for high temperature CO2 capture are under intensive development owing to their potential applications in advanced zero emission power, sorption-enhanced steam methane reforming for hydrogen production and energy storage systems in chemical heat pumps. One of the challenges in the development is the prevention of sintering of the sorbent (normally a calcium oxide derivative) which causes the CO2 capture capacity of the material to deteriorate rapidly after a few cycles of utilization. Here we show that a simple wet mixing method can produce sintering-resistant sorbents from calcium and magnesium salts of d-gluconic acid. It was found that calcium oxide was well distributed in the sorbents with metal oxide nanoparticles on the surface acting as physical barriers, and the CO2 capture capacity of the sorbents was largely maintained over multiple cycles of utilization. This method was also applied to other organometallic salts of calcium and magnesium/aluminum and the produced sorbents showed similarly high reversibility.

  4. Charged Covalent Triazine Frameworks for CO2 Capture and Conversion.

    PubMed

    Buyukcakir, Onur; Je, Sang Hyun; Talapaneni, Siddulu Naidu; Kim, Daeok; Coskun, Ali

    2017-03-01

    The quest for the development of new porous materials addressing both CO2 capture from various sources and its conversion into useful products is a very active research area and also critical in order to develop a more sustainable and environmentally-friendly society. Here, we present the first charged covalent triazine framework (cCTF) prepared by simply heating nitrile functionalized dicationic viologen derivatives under ionothermal reaction conditions using ZnCl2 as both solvent and trimerization catalyst. It has been demonstrated that the surface area, pore volume/size of cCTFs can be simply controlled by varying the synthesis temperature and the ZnCl2 content. Specifically, increasing the reaction temperature led to controlled increase in the mesopore content and facilitated the formation of hierarchical porosity, which is critical to ensure efficient mass transport within porous materials. The resulting cCTFs showed high specific surface areas up to 1247 m(2) g(-1), and high physicochemical stability. The incorporation of ionic functional moieties to porous organic polymers improved substantially their CO2 affinity (up to 133 mg g(-1), at 1 bar and 273 K) and transformed them into hierarchically porous organocatalysts for CO2 conversion. More importantly, the ionic nature of cCTFs, homogeneous charge distribution together with hierarchical porosity offered a perfect platform for the catalytic conversion of CO2 into cyclic carbonates in the presence of epoxides through an atom economy reaction in high yields and exclusive product selectivity. These results clearly demonstrate the promising aspect of incorporation of charged units into the porous organic polymers for the development of highly efficient porous organocatalysts for CO2 capture and fixation.

  5. A NOVEL CO2 SEPARATION SYSTEM

    SciTech Connect

    Robert J. Copeland; Gokhan Alptekin; Mike Cesario; Steven Gebhard; Yevgenia Gershanovich

    1999-01-01

    Because of concern over global climate change, new systems are needed that produce electricity from fossil fuels and emit less CO{sub 2}. The fundamental problem with current CO{sub 2} separation systems is the need to separate dilute CO{sub 2} and pressurize it for storage or sequestration. This is an energy intensive process that can reduce plant efficiency by 9-37% and double the cost of electricity.

  6. Mechanisms of CO2 Capture into Monoethanolamine Solution with Different CO2 Loading during the Absorption/Desorption Processes.

    PubMed

    Lv, Bihong; Guo, Bingsong; Zhou, Zuoming; Jing, Guohua

    2015-09-01

    Though the mechanism of MEA-CO2 system has been widely studied, there is few literature on the detailed mechanism of CO2 capture into MEA solution with different CO2 loading during absorption/desorption processes. To get a clear picture of the process mechanism, (13)C nuclear magnetic resonance (NMR) was used to analyze the reaction intermediates under different CO2 loadings and detailed mechanism on CO2 absorption and desorption in MEA was evaluated in this work. The results demonstrated that the CO2 absorption in MEA started with the formation of carbamate according to the zwitterion mechanism, followed by the hydration of CO2 to form HCO3(-)/CO3(2-), and accompanied by the hydrolysis of carbamate. It is interesting to find that the existence of carbamate will be influenced by CO2 loading and that it is rather unstable at high CO2 loading. At low CO2 loading, carbamate is formed fast by the reaction between CO2 and MEA. At high CO2 loading, it is formed by the reaction of CO3(-)/CO3(2-) with MEA, and the formed carbamate can be easily hydrolyzed by H(+). Moreover, CO2 desorption from the CO2-saturated MEA solution was proved to be a reverse process of absorption. Initially, some HCO3(-) were heated to release CO2 and other HCO3(-) were reacted with carbamic acid (MEAH(+)) to form carbamate, and the carbamate was then decomposed to MEA and CO2.

  7. CO2 SEPARATIONS USING ZEOLITE MEMBRANES

    SciTech Connect

    Richard D. Noble; John L. Falconer

    2001-06-30

    Zeolite and other inorganic molecular sieve membranes have shown potential for separations based on molecular size and shape because of their small pore sized, typically less than 1 nm, and their narrow pore size distribution. The high thermal and chemical stability of these inorganic crystals make them ideal materials for use in high temperature applications such as catalytic membrane reactors. Most of the progress with zeolite membranes has been with MFI zeolites prepared on porous disks and tubes. The MFI zeolite is a medium pore size structure having nearly circular pores with diameters between .53 and .56 nm. Separation experiments through MFI membranes indicate that competitive adsorption separates light gas mixtures. Light gas selectivities are typically small, however, owing to small differences in adsorption strengths and their small sizes relative to the MFI pore opening. Furthermore, competitive adsorption does not work well at high temperature where zeolite membranes are stable and have potential application. Separation by differences in size has a greater potential to work at high temperature than competitive adsorption, but pores smaller than those in MFI zeolites are required. Therefore, some studies focused on the synthesis of a small, 8-membered-pore structures such as zeolite A (0.41-nm pore diameter) and SAPO-34, a chabazite (about .4-nm pore diameter with about 1.4 nm cages) analog. The small pore size of the zeolite A and SAPO-34 structures made the separation of smaller molecules by differences in size possible. Zeolite MFI and SAPO-34 membranes were prepared on the inside surface of porous alumina tubes by hydrothermal synthesis, and single gas and binary mixture permeances were measured to characterize the membrane's performance. A mathematical diffusion model was developed to determine the relative quantities of zeolite and non-zeolite pores in different membranes by modeling the permeation date of CO{sub 2}. This model expresses the total

  8. Recent advances in CO2 capture and utilization.

    PubMed

    Yu, Kai Man Kerry; Curcic, Igor; Gabriel, Joseph; Tsang, Shik Chi Edman

    2008-01-01

    Energy and the environment are two of the most important issues this century. More than 80 % of our energy comes from the combustion of fossil fuels, which will still remain the dominant energy source for years to come. It is agreed that carbon dioxide produced from the combustion process to be the most important anthropogenic greenhouse gas leading to global warming. Atmospheric CO(2) concentrations have indeed increased by almost 100 ppm since their pre-industrial level, reaching 384 ppm in 2007 with a total annual emission of over 35 Gt. Prompt global action to resolve the CO(2) crisis is therefore needed. To pursue such an action, we are urged to save energy without the unnecessary production of carbon emissions and to use energy in more efficient ways, but alternative methods to mitigate the greenhouse gas have to be considered. This Minireview highlights some recent promising research activities and their prospects in the areas of carbon capture and storage and chemical fixation of CO(2) in constructing a future low-carbon global economy with reference to energy source, thermodynamic considerations, net carbon emissions and availability of reagents.

  9. CO2 Capture in Dry and Wet Conditions in UTSA-16 Metal-Organic Framework.

    PubMed

    Masala, Alessio; Vitillo, Jenny G; Mondino, Giorgia; Grande, Carlos A; Blom, Richard; Manzoli, Maela; Marshall, Marc; Bordiga, Silvia

    2017-01-11

    Water is the strongest competitor to CO2 in the adsorption on microporous materials, affecting their performances as CO2 scrubbers in processes such as postcombustion carbon capture. The metal-organic framework (MOF) UTSA-16 is considered a promising material for its capacity to efficiently capture CO2 in large quantities, thanks to the presence of open metal sites (OMSs). It is here shown that UTSA-16 is also able to desorb fully water already at room temperature. This property is unique from all the other materials with OMSs reported so far. UTSA-16 retains indeed the 70% of its CO2 separation capacity after admittance of water in a test flow, created to simulate the emissions from a real postcombustion carbon-capture process. This important aspect not yet observed for any other amine-free material, associated with a high material stability-tested for 160 cycles-and a small temperature swing necessary for regeneration, places UTSA-16 in the restrict number of systems with a real technological future for CO2 separation.

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

    SciTech Connect

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

    2010-06-16

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

  11. Amine modeling for CO2 capture: internals selection.

    PubMed

    Karpe, Prakash; Aichele, Clint P

    2013-04-16

    Traditionally, trays have been the mass-transfer device of choice in amine absorption units. However, the need to process large volumes of flue gas to capture CO2 and the resultant high costs of multiple trains of large trayed columns have prompted process licensors and vendors to investigate alternative mass-transfer devices. These alternatives include third-generation random packings and structured packings. Nevertheless, clear-cut guidelines for selection of packings for amine units are lacking. This paper provides well-defined guidelines and a consistent framework for the choice of mass-transfer devices for amine absorbers and regenerators. This work emphasizes the role played by the flow parameter, a measure of column liquid loading and pressure, in the type of packing selected. In addition, this paper demonstrates the significant economic advantage of packings over trays in terms of capital costs (CAPEX) and operating costs (OPEX).

  12. CO2 capture in alkanolamine-RTIL blends via carbamate crystallization: route to efficient regeneration.

    PubMed

    Hasib-ur-Rahman, Muhammad; Larachi, Faïçal

    2012-10-16

    One of the major drawbacks of aqueous alkanolamine based CO(2) capture processes is the requirement of significantly higher energy of regeneration. This weakness can be overcome by separating the CO(2)-captured product to regenerate the corresponding amine, thus avoiding the consumption of redundant energy. Replacing aqueous phase with more stable and practically nonvolatile imidazolium based room-temperature ionic liquid (RTIL) provided a viable approach for carbamate to crystallize out as supernatant solid. In the present study, regeneration capabilities of solid carbamates have been investigated. Diethanolamine (DEA) carbamate as well as 2-amino-2-methyl-1-propanol (AMP) carbamate were obtained in crystalline form by bubbling CO(2) in alkanolamine-RTIL mixtures. Hydrophobic RTIL, 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([hmim][Tf(2)N]), was used as aqueous phase substituent. Thermal behavior of the carbamates was observed by differential scanning calorimetry and thermogravimetric analysis, while the possible regeneration mechanism has been proposed through (13)C NMR and FTIR analyses. The results showed that decomposition of DEA-carbamate commenced at lower temperature (∼55 °C), compared to that of AMP-carbamate (∼75 °C); thus promising easy regeneration. The separation of carbamate as solid phase can offer two-way advantage by letting less volume to regenerate as well as by narrowing the gap between CO(2) capture and amine regeneration temperatures.

  13. CO2 capture using fly ash from coal fired power plant and applications of CO2-captured fly ash as a mineral admixture for concrete.

    PubMed

    Siriruang, Chaichan; Toochinda, Pisanu; Julnipitawong, Parnthep; Tangtermsirikul, Somnuk

    2016-04-01

    The utilization of fly ash as a solid sorbent material for CO2 capture via surface adsorption and carbonation reaction was evaluated as an economically feasible CO2 reduction technique. The results show that fly ash from a coal fired power plant can capture CO2 up to 304.7 μmol/g fly ash, consisting of 2.9 and 301.8 μmol/g fly ash via adsorption and carbonation, respectively. The CO2 adsorption conditions (temperature, pressure, and moisture) can affect CO2 capture performance of fly ash. The carbonation of CO2 with free CaO in fly ashes was evaluated and the results indicated that the reaction consumed most of free CaO in fly ash. The fly ashes after CO2 capture were further used for application as a mineral admixture for concrete. Properties such as water requirement, compressive strength, autoclave expansion, and carbonation depth of mortar and paste specimens using fly ash before and after CO2 capture were tested and compared with material standards. The results show that the expansion of mortar specimens using fly ash after CO2 capture was greatly reduced due to the reduction of free CaO content in the fly ash compared to the expansion of specimens using fresh fly ash. There were no significant differences in the water requirement and compressive strength of specimens using fly ash, before and after CO2 capture process. The results from this study can lead to an alternative CO2 capture technique with doubtless utilization of fly ash after CO2 capture as a mineral admixture for concrete.

  14. COMBUSTION-ASSISTED CO2 CAPTURE USING MECC MEMBRANES

    SciTech Connect

    Brinkman, K.; Gray, J.

    2012-03-30

    Mixed Electron and Carbonate ion Conductor (MECC) membranes have been proposed as a means to separate CO{sub 2} from power plant flue gas. Here a modified MECC CO{sub 2} capture process is analyzed that supplements retentate pressurization and permeate evacuation as a means to create a CO{sub 2} driving force with a process assisted by the catalytic combustion of syngas on the permeate side of the membrane. The combustion reactions consume transported oxygen, making it unavailable for the backwards transport reaction. With this change, the MECC capture system becomes exothermic, and steam for electricity production may be generated from the waste heat. Greater than 90% of the CO{sub 2} in the flue gas may be captured, and a compressed CO{sub 2} product stream is produced. A fossil-fueled power plant using this process would consume 14% more fuel per unit electricity produced than a power plant with no CO{sub 2} capture system, and has the potential to meet U.S. DOE's goal that deployment of a CO{sub 2} capture system at a fossil-fueled power plant should not increase the cost of electricity from the combined facility by more than 30%.

  15. CO2 capture enhancement in InOF-1 via the bottleneck effect of confined ethanol.

    PubMed

    Peralta, Ricardo A; Campos-Reales-Pineda, Alberto; Pfeiffer, Heriberto; Álvarez, J Raziel; Zárate, J Antonio; Balmaseda, Jorge; González-Zamora, Eduardo; Martínez, Ana; Martínez-Otero, Diego; Jancik, Vojtech; Ibarra, Ilich A

    2016-08-11

    CO2 capture of InOF-1 was enhanced 3.6-fold, at 1 bar and 30 °C, by confining EtOH within its pores. Direct visualisation by single crystal X-ray diffraction revealed that EtOH divides InOF-1 channels in wide sections separated by "bottlenecks" caused by EtOH molecules bonded to the μ2-OH functional groups of InOF-1.

  16. Poly(ethylenimine)-Functionalized Monolithic Alumina Honeycomb Adsorbents for CO2 Capture from Air.

    PubMed

    Sakwa-Novak, Miles A; Yoo, Chun-Jae; Tan, Shuai; Rashidi, Fereshteh; Jones, Christopher W

    2016-07-21

    The development of practical and effective gas-solid contactors is an important area in the development of CO2 capture technologies. Target CO2 capture applications, such as postcombustion carbon capture and sequestration (CCS) from power plant flue gases or CO2 extraction directly from ambient air (DAC), require high flow rates of gas to be processed at low cost. Extruded monolithic honeycomb structures, such as those employed in the catalytic converters of automobiles, have excellent potential as structured contactors for CO2 adsorption applications because of the low pressure drop imposed on fluid moving through the straight channels of such structures. Here, we report the impregnation of poly(ethylenimine) (PEI), an effective aminopolymer reported commonly for CO2 separation, into extruded monolithic alumina to form structured CO2 sorbents. These structured sorbents are first prepared on a small scale, characterized thoroughly, and compared with powder sorbents with a similar composition. Despite consistent differences observed in the filling of mesopores with PEI between the monolithic and powder sorbents, their performance in CO2 adsorption is similar across a range of PEI contents. A larger monolithic cylinder (1 inch diameter, 4 inch length) is evaluated under conditions closer to those that might be used in large-scale applications and shows a similar performance to the smaller monoliths and powders tested initially. This larger structure is evaluated over five cycles of CO2 adsorption and steam desorption and demonstrates a volumetric capacity of 350 molCO2  m-3monolith and an equilibration time of 350 min under a 0.4 m s(-1) linear flow velocity through the monolith channels using 400 ppm CO2 in N2 as the adsorption gas at 30 °C. This volumetric capacity surpasses that of a similar technology considered previously, which suggested that CO2 could be removed from air at an operating cost as low as $100 per ton.

  17. Hybrid Membrane/Absorption Process for Post-combustion CO2 Capture

    SciTech Connect

    Li, Shiguang; Shou, S.; Pyrzynski, Travis; Makkuni, Ajay; Meyer, Howard

    2013-12-31

    This report summarizes scientific/technical progress made for bench-scale membrane contactor technology for post-combustion CO2 capture from DOE Contract No. DE-FE-0004787. Budget Period 1 (BP1) membrane absorber, Budget Period 2 (BP2) membrane desorber and Budget Period 3 (BP3) integrated system and field testing studies have been completed successfully and met or exceeded the technical targets (≥ 90% CO2 removal and CO2 purity of 97% in one membrane stage). Significant breakthroughs are summarized below: BP1 research: The feasibility of utilizing the poly (ether ether ketone), PEEK, based hollow fiber contractor (HFC) in combination with chemical solvents to separate and capture at least 90% of the CO2 from simulated flue gases has been successfully established. Excellent progress has been made as we have achieved the BP1 goal: ≥ 1,000 membrane intrinsic CO2 permeance, ≥ 90% CO2 removal in one stage, ≤ 2 psi gas side pressure drop, and ≥ 1 (sec)-1 mass transfer coefficient. Initial test results also show that the CO2 capture performance, using activated Methyl Diethanol Amine (aMDEA) solvent, was not affected by flue gas contaminants O2 (~3%), NO2 (66 ppmv), and SO2 (145 ppmv). BP2 research: The feasibility of utilizing the PEEK HFC for CO2-loaded solvent regeneration has been successfully established High CO2 stripping flux, one order of magnitude higher than CO2 absorption flux, have been achieved. Refined economic evaluation based on BP1 membrane absorber and BP2 membrane desorber laboratory test data indicate that the CO2 capture costs are 36% lower than DOE’s benchmark amine absorption technology. BP3 research: A bench-scale system utilizing a membrane absorber and desorber was integrated into a continuous CO2 capture process using contactors containing 10 to 20 ft2 of membrane area. The integrated process operation was stable through a 100-hour laboratory test, utilizing a simulated flue gas stream. Greater than 90% CO2 capture combined with 97

  18. Triazine containing N-rich microporous organic polymers for CO2 capture and unprecedented CO2/N2 selectivity

    NASA Astrophysics Data System (ADS)

    Bhunia, Subhajit; Bhanja, Piyali; Das, Sabuj Kanti; Sen, Tapas; Bhaumik, Asim

    2017-03-01

    Targeted synthesis of microporous adsorbents for CO2 capture and storage is very challenging in the context of remediation from green house gases. Herein we report two novel N-rich microporous networks SB-TRZ-CRZ and SB-TRZ-TPA by extensive incorporation of triazine containing tripodal moiety in the porous polymer framework. These materials showed excellent CO2 storage capacities: SB-TRZ-CRZ displayed the CO2 uptake capacity of 25.5 wt% upto 1 bar at 273 K and SB-TRZ-TPA gave that of 16 wt% under identical conditions. The substantial dipole quadruple interaction between network (polar triazine) and CO2 boosts the selectivity for CO2/N2. SB-TRZ-CRZ has this CO2/N2 selectivity ratio of 377, whereas for SB-TRZ-TPA it was 97. Compared to other porous polymers, these materials are very cost effective, scalable and very promising material for clean energy application and environmental issues.

  19. Amine-Oxide Hybrid Materials for CO2 Capture from Ambient Air.

    PubMed

    Didas, Stephanie A; Choi, Sunho; Chaikittisilp, Watcharop; Jones, Christopher W

    2015-10-20

    Oxide supports functionalized with amine moieties have been used for decades as catalysts and chromatographic media. Owing to the recognized impact of atmospheric CO2 on global climate change, the study of the use of amine-oxide hybrid materials as CO2 sorbents has exploded in the past decade. While the majority of the work has concerned separation of CO2 from dilute mixtures such as flue gas from coal-fired power plants, it has been recognized by us and others that such supported amine materials are also perhaps uniquely suited to extract CO2 from ultradilute gas mixtures, such as ambient air. As unique, low temperature chemisorbents, they can operate under ambient conditions, spontaneously extracting CO2 from ambient air, while being regenerated under mild conditions using heat or the combination of heat and vacuum. This Account describes the evolution of our activities on the design of amine-functionalized silica materials for catalysis to the design, characterization, and utilization of these materials in CO2 separations. New materials developed in our laboratory, such as hyperbranched aminosilica materials, and previously known amine-oxide hybrid compositions, have been extensively studied for CO2 extraction from simulated ambient air (400 ppm of CO2). The role of amine type and structure (molecular, polymeric), support type and structure, the stability of the various compositions under simulated operating conditions, and the nature of the adsorbed CO2 have been investigated in detail. The requirements for an effective, practical air capture process have been outlined and the ability of amine-oxide hybrid materials to meet these needs has been discussed. Ultimately, the practicality of such a "direct air capture" process is predicated not only on the physicochemical properties of the sorbent, but also how the sorbent operates in a practical process that offers a scalable gas-solid contacting strategy. In this regard, the utility of low pressure drop monolith

  20. Dual phase high-temperature membranes for CO2 separation - performance assessment in post- and pre-combustion processes.

    PubMed

    Anantharaman, Rahul; Peters, Thijs; Xing, Wen; Fontaine, Marie-Laure; Bredesen, Rune

    2016-10-20

    Dual phase membranes are highly CO2-selective membranes with an operating temperature above 400 °C. The focus of this work is to quantify the potential of dual phase membranes in pre- and post-combustion CO2 capture processes. The process evaluations show that the dual phase membranes integrated with an NGCC power plant for CO2 capture are not competitive with the MEA process for post-combustion capture. However, dual phase membrane concepts outperform the reference Selexol technology for pre-combustion CO2 capture in an IGCC process. The two processes evaluated in this work, post-combustion NGCC and pre-combustion IGCC, represent extremes in CO2 partial pressure fed to the separation unit. Based on the evaluations it is expected that dual phase membranes could be competitive for post-combustion capture from a pulverized coal fired power plant (PCC) and pre-combustion capture from an Integrated Reforming Cycle (IRCC).

  1. A single-ligand ultra-microporous MOF for precombustion CO2 capture and hydrogen purification

    PubMed Central

    Nandi, Shyamapada; De Luna, Phil; Daff, Thomas D.; Rother, Jens; Liu, Ming; Buchanan, William; Hawari, Ayman I.; Woo, Tom K.; Vaidhyanathan, Ramanathan

    2015-01-01

    Metal organic frameworks (MOFs) built from a single small ligand typically have high stability, are rigid, and have syntheses that are often simple and easily scalable. However, they are normally ultra-microporous and do not have large surface areas amenable to gas separation applications. We report an ultra-microporous (3.5 and 4.8 Å pores) Ni-(4-pyridylcarboxylate)2 with a cubic framework that exhibits exceptionally high CO2/H2 selectivities (285 for 20:80 and 230 for 40:60 mixtures at 10 bar, 40°C) and working capacities (3.95 mmol/g), making it suitable for hydrogen purification under typical precombustion CO2 capture conditions (1- to 10-bar pressure swing). It exhibits facile CO2 adsorption-desorption cycling and has CO2 self-diffusivities of ~3 × 10−9 m2/s, which is two orders higher than that of zeolite 13X and comparable to other top-performing MOFs for this application. Simulations reveal a high density of binding sites that allow for favorable CO2-CO2 interactions and large cooperative binding energies. Ultra-micropores generated by a small ligand ensures hydrolytic, hydrostatic stabilities, shelf life, and stability toward humid gas streams. PMID:26824055

  2. A single-ligand ultra-microporous MOF for precombustion CO2 capture and hydrogen purification.

    PubMed

    Nandi, Shyamapada; De Luna, Phil; Daff, Thomas D; Rother, Jens; Liu, Ming; Buchanan, William; Hawari, Ayman I; Woo, Tom K; Vaidhyanathan, Ramanathan

    2015-12-01

    Metal organic frameworks (MOFs) built from a single small ligand typically have high stability, are rigid, and have syntheses that are often simple and easily scalable. However, they are normally ultra-microporous and do not have large surface areas amenable to gas separation applications. We report an ultra-microporous (3.5 and 4.8 Å pores) Ni-(4-pyridylcarboxylate)2 with a cubic framework that exhibits exceptionally high CO2/H2 selectivities (285 for 20:80 and 230 for 40:60 mixtures at 10 bar, 40°C) and working capacities (3.95 mmol/g), making it suitable for hydrogen purification under typical precombustion CO2 capture conditions (1- to 10-bar pressure swing). It exhibits facile CO2 adsorption-desorption cycling and has CO2 self-diffusivities of ~3 × 10(-9) m(2)/s, which is two orders higher than that of zeolite 13X and comparable to other top-performing MOFs for this application. Simulations reveal a high density of binding sites that allow for favorable CO2-CO2 interactions and large cooperative binding energies. Ultra-micropores generated by a small ligand ensures hydrolytic, hydrostatic stabilities, shelf life, and stability toward humid gas streams.

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

    SciTech Connect

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

    2016-03-28

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

  4. Measurement, standards, and data needs for CO2 capture materials: a critical review.

    PubMed

    Espinal, Laura; Poster, Dianne L; Wong-Ng, Winnie; Allen, Andrew J; Green, Martin L

    2013-01-01

    The commercial deployment of cost-effective carbon capture technology is hindered partially by the lack of a proper suite of materials-related measurements, standards, and data, which would provide critical information for the systematic design, evaluation, and performance of CO2 separation materials. Based on a literature search and conversations with the carbon capture community, we review the current status of measurements, standards, and data for the three major carbon capture materials in use today: solvents, solid sorbents, and membranes. We highlight current measurement, standards and data activities aimed to advance the development and use of carbon capture materials and major research needs that are critical to meet if innovation in carbon capture materials is to be achieved. The review reveals that although adsorbents are considered to have great potential to reduce carbon capture cost, there is no consensus on the experimental parameters to be used for evaluating sorbent properties. Another important finding is the lack of in situ experimental tools for the structural characterization of solid porous materials during CO2 adsorption, and computational methods that would enable a materials-by-design approach for their development.

  5. CO2 Capture from the Air: Technology Assessment and Implications for Climate Policy

    NASA Astrophysics Data System (ADS)

    Keith, D. W.

    2002-05-01

    It is physically possible to capture CO2 directly from the air and immobilize it in geological structures. Today, there are no large-scale technologies that achieve air capture at reasonable cost. Yet, strong arguments suggest that it will comparatively easy to develop practical air capture technologies on the timescales relevant to climate policy [1]. This paper first analyzes the cost of air capture and then assesses the implications for climate policy. We first analyze the lower bound on the cost needed for air capture, describing the thermodynamic and physical limits to the use of energy and land. We then compare the costs of air capture to the cost of capture from combustion exhaust streams. While the intrinsic minimum energy requirement is larger for air capture, we argue that air capture has important structural advantages, such as the reduction of transport costs and the larger potential for economies of scale. These advantages suggest that, in the long-run air capture be competitive with other methods of achieving deep emissions reductions. We provide a preliminary engineering-economic analysis of an air capture system based on CaO to CaCO3 chemical looping [1]. We analyze the possibility of doing the calcination in a modified pressurized fluidized bed combustor (PFBC) burning coal in a CO2 rich atmosphere with oxygen supplied by an air separation unit. The CaCO3-to-coal ratio would be ~2:1 and the system would be nearly thermally neutral. PFBC systems have been demonstrated at capacities of over 100 MW. Such systems already include CaCO3 injection for sulfur control, and operate at suitable temperatures and pressures for calcination. We assess the potential to recover heat from the dissolution of CaO in order to reduce the overall energy requirements. We analyze the possibility of adapting existing large water/air heat exchangers for use as contacting systems to capture CO2 from the air using the calcium hydroxide solution. The implications of air capture

  6. Progress Towards Commercialization of Electrochemical Membrane Technology for CO2 Capture and Power Generation

    SciTech Connect

    Ghezel-Ayagh, Hossein; Jolly, Stephen; DiNitto, M.; Hunt, Jennifer; Patel, Dilip; Steen, William A.; Richardson, C. F.; Marina, Olga A.; Pederson, Larry R.

    2014-03-01

    To address the concerns about climate change resulting from emission of CO2 by coal-fueled power plants, FuelCell Energy, Inc. has developed Combined Electric Power and Carbon-dioxide Separation (CEPACS) system concept, as a novel solution for greenhouse gas emission reduction. The CEPACS system utilizes Electrochemical Membrane (ECM) technology derived from the Company’s well established Direct FuelCell® products. The system concept works as two devices in one: it separates the CO2 from the exhaust of other plants and simultaneously, using a supplementary fuel, produces electric power at high efficiency. FCE is currently evaluating the use of ECM to cost effectively separate CO2 from the flue gas of coal fired power plants under a U.S. Department of Energy contract. The overarching objective of the project is to verify that the ECM can achieve at least 90% CO2 capture from flue gas of a PC plant with no more than 35% increase in the cost of electricity. The specific objectives and related activities presently ongoing for the project include: 1) conduct bench scale tests of ECM and 2) evaluate the effects of impurities present in the coal plant flue gas by laboratory scale performance tests of the membrane.

  7. Adsorption mechanism of graphene-like ZnO monolayer towards CO2 molecules: enhanced CO2 capture

    NASA Astrophysics Data System (ADS)

    Rao, G. S.; Hussain, T.; Islam, M. S.; Sagynbaeva, M.; Gupta, D.; Panigrahi, P.; Ahuja, R.

    2016-01-01

    This work aims to efficiently capture CO2 on two-dimensional (2D) nanostructures for effective cleaning of our atmosphere and purification of exhausts coming from fuel engines. Here, we have performed extensive first principles calculations based on density functional theory (DFT) to investigate the interaction of CO2 on a recently synthesized ZnO monolayer (ZnO-ML) in its pure, defected and functionalized form. A series of rigorous calculations yielded the most preferential binding configurations of the CO2 gas molecule on a ZnO-ML. It is observed that the substitution of one oxygen atom with boron, carbon and nitrogen on the ZnO monolayer resulted into enhanced CO2 adsorption. Our calculations show an enriched adsorption of CO2 on the ZnO-ML when substituting with foreign atoms like B, C and N. The improved adsorption energy of CO2 on ZnO suggests the ZnO-ML could be a promising candidate for future CO2 capture.

  8. Predicting the ultimate potential of natural gas SOFC power cycles with CO2 capture - Part B: Applications

    NASA Astrophysics Data System (ADS)

    Campanari, Stefano; Mastropasqua, Luca; Gazzani, Matteo; Chiesa, Paolo; Romano, Matteo C.

    2016-09-01

    An important advantage of solid oxide fuel cells (SOFC) as future systems for large scale power generation is the possibility of being efficiently integrated with processes for CO2 capture. Focusing on natural gas power generation, Part A of this work assessed the performances of advanced pressurised and atmospheric plant configurations (SOFC + GT and SOFC + ST, with fuel cell integration within a gas turbine or a steam turbine cycle) without CO2 separation. This Part B paper investigates such kind of power cycles when applied to CO2 capture, proposing two ultra-high efficiency plant configurations based on advanced intermediate-temperature SOFCs with internal reforming and low temperature CO2 separation process. The power plants are simulated at the 100 MW scale with a set of realistic assumptions about FC performances, main components and auxiliaries, and show the capability of exceeding 70% LHV efficiency with high CO2 capture (above 80%) and a low specific primary energy consumption for the CO2 avoided (1.1-2.4 MJ kg-1). Detailed results are presented in terms of energy and material balances, and a sensitivity analysis of plant performance is developed vs. FC voltage and fuel utilisation to investigate possible long-term improvements. Options for further improvement of the CO2 capture efficiency are also addressed.

  9. Process for CO2 Capture Using Ionic Liquid That Exhibits Phase Change

    SciTech Connect

    Eisinger, RS; Keller, GE

    2014-11-01

    A novel process for capturing carbon dioxide from the flue gas of a coal-fired power plant has been shown to reduce parasitic power consumption substantially. The process employs an ionic liquid created at the University of Notre Dame that has a high capacity for absorbing CO2 by chemical reaction. A distinguishing property of this ionic liquid is that it changes phase from solid to liquid upon reaction with CO2. The process uses heat generated by this phase transition to lower parasitic power consumption. The driving force for CO2 separation is a combination of temperature and pressure differences; the process could even work without the addition of heat. A realistic process was created to capture CO2 efficiently. Computer simulation of the process enabled calculation of viable process conditions and power usage. The main concepts of the process were shown to work using a lab-scale apparatus. Parasitic power consumes 23% of net power generation, 55% lower than that of the monoethanolamine (MEA) process. However, capital cost is higher. The cost of electricity (COE) is 28% lower than that of the MEA process.

  10. Equimolar CO2 capture by N-substituted amino acid salts and subsequent conversion.

    PubMed

    Liu, An-Hua; Ma, Ran; Song, Chan; Yang, Zhen-Zhen; Yu, Ao; Cai, Yu; He, Liang-Nian; Zhao, Ya-Nan; Yu, Bing; Song, Qing-Wen

    2012-11-05

    Steric bulk controls CO(2) absorption: N-substituted amino acid salts in poly(ethylene glycol) reversibly absorb CO(2) in nearly 1:1 stoichiometry. Carbamic acid is thought to be the absorbed form of CO(2); this was supported by NMR and in situ IR spectroscopy, and DFT calculations. The captured CO(2) could be converted directly into oxazolidinones and thus CO(2) desorption could be sidestepped.

  11. Amorphous Silk Fibroin Membranes for Separation of CO2

    NASA Technical Reports Server (NTRS)

    Aberg, Christopher M.; Patel, Anand K.; Gil, Eun Seok; Spontak, Richard J.; Hagg, May-Britt

    2009-01-01

    Amorphous silk fibroin has shown promise as a polymeric material derivable from natural sources for making membranes for use in removing CO2 from mixed-gas streams. For most applications of silk fibroin, for purposes other than gas separation, this material is used in its highly crystalline, nearly natural form because this form has uncommonly high tensile strength. However, the crystalline phase of silk fibroin is impermeable, making it necessary to convert the material to amorphous form to obtain the high permeability needed for gas separation. Accordingly, one aspect of the present development is a process for generating amorphous silk fibroin by treating native silk fibroin in an aqueous methanol/salt solution. The resulting material remains self-standing and can be prepared as thin film suitable for permeation testing. The permeability of this material by pure CO2 has been found to be highly improved, and its mixed-gas permeability has been found to exceed the mixed-gas permeabilities of several ultrahigh-CO2-permeable synthetic polymers. Only one of the synthetic polymers poly(trimethylsilylpropyne) [PTMSP] may be more highly permeable by CO2. PTMSP becomes unstable with time, whereas amorphous silk should not, although at the time of this reporting this has not been conclusively proven.

  12. Application of amine-tethered solid sorbents for direct CO2 capture from the ambient air.

    PubMed

    Choi, Sunho; Drese, Jeffrey H; Eisenberger, Peter M; Jones, Christopher W

    2011-03-15

    While current carbon capture and sequestration (CCS) technologies for large point sources can help address the impact of CO(2) buildup on global climate change, these technologies can at best slow the rate of increase of the atmospheric CO(2) concentration. In contrast, the direct CO(2) capture from ambient air offers the potential to be a truly carbon negative technology. We propose here that amine-based solid adsorbents have significant promise as key components of a hypothetical air capture process. Specifically, the CO(2) capture characteristics of hyperbranched aminosilica (HAS) materials are evaluated here using CO(2) mixtures that simulate ambient atmospheric concentrations (400 ppm CO(2) = "air capture") as well as more traditional conditions simulating flue gas (10% CO(2)). The air capture experiments demonstrate that the adsorption capacity of HAS adsorbents are only marginally influenced even with a significant dilution of the CO(2) concentration by a factor of 250, while capturing CO(2) reversibly without significant degradation of performance in multicyclic operation. These results suggest that solid amine-based air capture processes have the potential to be an effective approach to extracting CO(2) from the ambient air.

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

    PubMed

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

    2013-03-07

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

  14. In Situ Doping Strategy for the Preparation of Conjugated Triazine Frameworks Displaying Efficient CO2 Capture Performance.

    PubMed

    Zhu, Xiang; Tian, Chengcheng; Veith, Gabriel M; Abney, Carter W; Dehaudt, Jérémy; Dai, Sheng

    2016-09-14

    An in situ doping strategy has been developed for the generation of a novel family of hexaazatriphenylene-based conjugated triazine frameworks (CTFs) for efficient CO2 capture. The resulting task-specific materials exhibit an exceptionally high CO2 uptake capacity (up to 4.8 mmol g(-1) at 297 K and 1 bar). The synergistic effects of ultrananoporosity and rich N/O codoped CO2-philic sites bestow the framework with the highest CO2 adsorption capacity among known porous organic polymers (POPs). This innovative approach not only enables superior CO2 separation performance but also provides tunable control of surface features on POPs, thereby affording control over bulk material properties. We anticipate this novel strategy will facilitate new possibilities for the rational design and synthesis of nanoporous materials for carbon capture.

  15. Highly optimized CO2 capture by inexpensive nanoporous covalent organic polymers and their amine composites.

    PubMed

    Patel, Hasmukh A; Yavuz, Cafer T

    2015-01-01

    Carbon dioxide (CO2) storage and utilization requires effective capture strategies that limit energy penalties. Polyethylenimine (PEI)-impregnated covalent organic polymers (COPs) with a high CO2 adsorption capacity are successfully prepared in this study. A low cost COP with a high specific surface area is suitable for PEI loading to achieve high CO2 adsorption, and the optimal PEI loading is 36 wt%. Though the adsorbed amount of CO2 on amine impregnated COPs slightly decreased with increasing adsorption temperature, CO2/N2 selectivity is significantly improved at higher temperatures. The adsorption of CO2 on the sorbent is very fast, and a sorption equilibrium (10% wt) was achieved within 5 min at 313 K under the flow of simulated flue gas streams. The CO2 capture efficiency of this sorbent is not affected under repetitive adsorption-desorption cycles. The highest CO2 capture capacity of 75 mg g(-1) at 0.15 bar is achieved under dry CO2 capture however it is enhanced to 100 mg g(-1) in the mixed gas flow containing humid 15% CO2. Sorbents were found to be thermally stable up to at least 200 °C. TGA and FTIR studies confirmed the loading of PEIs on COPs. This sorbent with high and fast CO2 sorption exhibits a very promising application in direct CO2 capture from flue gas.

  16. Self-supported fibrous porous aromatic membranes for efficient CO2/N2 separations.

    PubMed

    Meng, Lingbo; Zou, Xiaoqin; Guo, Shukun; Ma, Heping; Zhao, Yongnan; Zhu, Guangshan

    2015-07-22

    In this paper, we describe a new synthesis protocol for the preparation of self-supported hollow fiber membranes composed of porous aromatic framework PAF-56P and PSF. PAF-56P was facilely prepared by the cross-coupling reaction of triangle-shaped cyanuric chloride and linear p-terophenyl monomers. The prepared PAF-56P material possesses an extended conjugated network, the structure of which is confirmed by nuclear magnetic resonance and infrared characterizations, as well as a permanent porosity with a BET surface area of 553.4 m(2) g(-1) and a pore size of 1.2 nm. PAF-56P was subsequently integrated with PSF matrix into PAF-56P/PSF asymmetric hollow fiber membranes via the dry jet-wet quench method employing PAF-56P/PSF suspensions. Scanning electron microscopy studies show that PAF-56P particles are embedded in the PSF matrix to form continuous membranes. Fabricated PAF-56P/PSF membranes were further exploited for CO2 capture, which was exemplified by gas separations of CO2/N2 mixtures. The PAF-56P/PSF membranes show a high selectivity of CO2 over N2 with a separation factor of 38.9 due to the abundant nitrogen groups in the PAF-56P framework. A preferred permeance for CO2 in the binary CO2/N2 gas mixture is obtained in the range of 93-141 GPU due to the large CO2 adsorption capacity and a large pore size of PAF-56P. Additionally, PAF-56P/PSF membranes exhibit excellent thermal and mechanical stabilities, which were examined by thermal analysis and gas separation tests with the dependencies of temperatures and pressures. The merits of high selectivity for CO2, good stability, and easy scale up make PAF-56P/PSF hollow fiber membranes of great interest for the industrial separations of CO2 from the gas exhausts.

  17. Predicting mixed-gas adsorption equilibria on activated carbon for precombustion CO2 capture.

    PubMed

    García, S; Pis, J J; Rubiera, F; Pevida, C

    2013-05-21

    We present experimentally measured adsorption isotherms of CO2, H2, and N2 on a phenol-formaldehyde resin-based activated carbon, which had been previously synthesized for the separation of CO2 in a precombustion capture process. The single component adsorption isotherms were measured in a magnetic suspension balance at three different temperatures (298, 318, and 338 K) and over a large range of pressures (from 0 to 3000-4000 kPa). These values cover the temperature and pressure conditions likely to be found in a precombustion capture scenario, where CO2 needs to be separated from a CO2/H2/N2 gas stream at high pressure (~1000-1500 kPa) and with a high CO2 concentration (~20-40 vol %). Data on the pure component isotherms were correlated using the Langmuir, Sips, and dual-site Langmuir (DSL) models, i.e., a two-, three-, and four-parameter model, respectively. By using the pure component isotherm fitting parameters, adsorption equilibrium was then predicted for multicomponent gas mixtures by the extended models. The DSL model was formulated considering the energetic site-matching concept, recently addressed in the literature. Experimental gas-mixture adsorption equilibrium data were calculated from breakthrough experiments conducted in a lab-scale fixed-bed reactor and compared with the predictions from the models. Breakthrough experiments were carried out at a temperature of 318 K and five different pressures (300, 500, 1000, 1500, and 2000 kPa) where two different CO2/H2/N2 gas mixtures were used as the feed gas in the adsorption step. The DSL model was found to be the one that most accurately predicted the CO2 adsorption equilibrium in the multicomponent mixture. The results presented in this work highlight the importance of performing experimental measurements of mixture adsorption equilibria, as they are of utmost importance to discriminate between models and to correctly select the one that most closely reflects the actual process.

  18. Monoethanolamine adsorption on TiO2 (110) for solid supported CO2 capture

    NASA Astrophysics Data System (ADS)

    Lu, Deyu; Muller, Kathrin; Senanayake, Sanjaya; Starr, David

    2012-02-01

    Solid supported CO2 capture materials are drawing substantial attention as a promising, cost-effective and environmentally friendly alternative to aqueous amine based CO2 capture. Recently CO2 capture was observed from monoethanolamine (MEA) adsorbed TiO2 powders. In order to facilitate the rational design of future solid CO2 capture materials, it is very important to understand the interaction between MEA and the TiO2 surface at the atomic level and how it affects the CO2 capture capabilities. In this work, we report a combined experimental and theoretical study of MEA adsorption on rutile TiO2 (110). We found that 1 ML of MEAs can form a stable and ordered patten on TiO2 (110). However, the amine group in MEA (the CO2 capture site) binds preferably to the TiO2 surface in the gauche mode. The binding energy of the gauche mode is about 0.8 eV larger than the trans mode, where the amine group is free, causing the present MEA/TiO2 system unable to capture CO2. We found that this large binding energy difference is originated from a combination of surface donor-acceptor bonds, H-bonds, and dipole-induced dipole interaction. Our study suggests that these effects are key factors to design future amine-based solid supported CO2 capture materials.

  19. On the potential of phase-change adsorbents for CO2 capture by temperature swing adsorption.

    PubMed

    Hefti, Max; Joss, Lisa; Bjelobrk, Zoran; Mazzotti, Marco

    2016-10-20

    We investigate the potential of a class of recently discovered metal-organic-framework materials for their use in temperature swing adsorption (TSA) processes for CO2 capture; the particularity of the considered materials is their reversible and temperature dependent step-shaped CO2 adsorption isotherm. Specifically, we present a comprehensive modeling study, where the performance of five different materials with step-shaped isotherms [McDonald et al., Nature, 2015, 519, 303] in a four step TSA cycle is assessed. The specific energy requirement of the TSA process operated with these materials is lower than for a commercial 13X zeolite, and a smaller temperature swing is required to reach similar levels of CO2 purity and recovery. The effect of a step in the adsorption isotherm is illustrated and discussed, and design criteria that lead to an optimal and robust operation of the considered TSA cycle are identified. The presented criteria could guide material scientists in designing novel materials whose step position is tailored to specific CO2 separation tasks.

  20. Feasibility study of algae-based CO2 capture

    EPA Science Inventory

    Abstract: The biomass of microalgae contains approximately 50% carbon, which is commonly obtained from the atmosphere, but can also be taken from commercial sources that produce CO2, such as coal-fired power plants. A study of operational demonstration projects is being underta...

  1. Feasibility study of algae-based CO2 capture

    EPA Science Inventory

    The biomass of microalgae contains approximately 50% carbon, which is commonly obtained from the atmosphere, but can also be taken from commercial sources that produce CO2, such as coal-fired power plants. A study of operational demonstration projects is being undertaken to eval...

  2. Atmospheric CO2 capture by algae: Negative carbon dioxide emission path.

    PubMed

    Moreira, Diana; Pires, José C M

    2016-09-01

    Carbon dioxide is one of the most important greenhouse gas, which concentration increase in the atmosphere is associated to climate change and global warming. Besides CO2 capture in large emission point sources, the capture of this pollutant from atmosphere may be required due to significant contribution of diffuse sources. The technologies that remove CO2 from atmosphere (creating a negative balance of CO2) are called negative emission technologies. Bioenergy with Carbon Capture and Storage may play an important role for CO2 mitigation. It represents the combination of bioenergy production and carbon capture and storage, keeping carbon dioxide in geological reservoirs. Algae have a high potential as the source of biomass, as they present high photosynthetic efficiencies and high biomass yields. Their biomass has a wide range of applications, which can improve the economic viability of the process. Thus, this paper aims to assess the atmospheric CO2 capture by algal cultures.

  3. Efficient electrochemical refrigeration power plant using natural gas with ∼100% CO2 capture

    NASA Astrophysics Data System (ADS)

    Al-musleh, Easa I.; Mallapragada, Dharik S.; Agrawal, Rakesh

    2015-01-01

    We propose an efficient Natural Gas (NG) based Solid Oxide Fuel Cell (SOFC) power plant equipped with ∼100% CO2 capture. The power plant uses a unique refrigeration based process to capture and liquefy CO2 from the SOFC exhaust. The capture of CO2 is carried out via condensation and purification using two rectifying columns operating at different pressures. The uncondensed gas mixture, comprising of relatively high purity unconverted fuel, is recycled to the SOFC and found to boost the power generation of the SOFC by 22%, when compared to a stand alone SOFC. If Liquefied Natural Gas (LNG) is available at the plant gate, then the refrigeration available from its evaporation is used for CO2 Capture and Liquefaction (CO2CL). If NG is utilized, then a Mixed Refrigerant (MR) vapor compression cycle is utilized for CO2CL. Alternatively, the necessary refrigeration can be supplied by evaporating the captured liquid CO2 at a lower pressure, which is then compressed to supercritical pressures for pipeline transportation. From rigorous simulations, the power generation efficiency of the proposed processes is found to be 70-76% based on lower heating value (LHV). The benefit of the proposed processes is evident when the efficiency of 73% for a conventional SOFC-Gas turbine power plant without CO2 capture is compared with an equivalent efficiency of 71.2% for the proposed process with CO2CL.

  4. Challenges and opportunities for microalgae-mediated CO2 capture and biorefinery.

    PubMed

    Seth, Jyoti R; Wangikar, Pramod P

    2015-07-01

    Aquacultures of microalgae are frontrunners for photosynthetic capture of CO2 from flue gases. Expedient implementation mandates coupling of microalgal CO2 capture with synthesis of fuels and organic products, so as to derive value from biomass. An integrated biorefinery complex houses a biomass growth and harvesting area and a refining zone for conversion to product(s) and separation to desired purity levels. As growth and downstream options require energy and incur loss of carbon, put together, the loop must be energy positive, carbon negative, or add substantial value. Feasibility studies can, thus, aid the choice from among the rapidly evolving technological options, many of which are still in the early phases of development. We summarize basic engineering calculations for the key steps of a biorefining loop where flue gases from a thermal power station are captured using microalgal biomass along with subsequent options for conversion to fuel or value added products. An assimilation of findings from recent laboratory and pilot-scale experiments and life cycle analysis (LCA) studies is presented as carbon and energy yields for growth and harvesting of microalgal biomass and downstream options. Of the biorefining options, conversion to the widely studied biofuel, ethanol, and manufacture of the platform chemical, succinic acid are presented. Both processes yield specific products and do not demand high-energy input but entail 60-70% carbon loss through fermentative respiration. Thermochemical conversions, on the other hand, have smaller carbon and energy losses but yield a mixture of products.

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

    PubMed

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

    2016-10-01

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

  6. Electrocatalytically switchable CO2 capture: first principle computational exploration of carbon nanotubes with pyridinic nitrogen.

    PubMed

    Jiao, Yan; Zheng, Yao; Smith, Sean C; Du, Aijun; Zhu, Zhonghua

    2014-02-01

    Carbon nanotubes with specific nitrogen doping are proposed for controllable, highly selective, and reversible CO2 capture. Using density functional theory incorporating long-range dispersion corrections, we investigated the adsorption behavior of CO2 on (7,7) single-walled carbon nanotubes (CNTs) with several nitrogen doping configurations and varying charge states. Pyridinic-nitrogen incorporation in CNTs is found to induce an increasing CO2 adsorption strength with electron injecting, leading to a highly selective CO2 adsorption in comparison with N2 . This functionality could induce intrinsically reversible CO2 adsorption as capture/release can be controlled by switching the charge carrying state of the system on/off. This phenomenon is verified for a number of different models and theoretical methods, with clear ramifications for the possibility of implementation with a broader class of graphene-based materials. A scheme for the implementation of this remarkable reversible electrocatalytic CO2 -capture phenomenon is considered.

  7. Surface modification of a low cost bentonite for post-combustion CO2 capture

    NASA Astrophysics Data System (ADS)

    Chen, Chao; Park, Dong-Wha; Ahn, Wha-Seung

    2013-10-01

    A low cost bentonite was modified with PEI (polyethylenimine) through a physical impregnation method. Bentonite in its natural state and after amine modification were characterized by scanning electron microscopy-energy dispersive X-ray spectroscopy, X-ray diffraction, N2 adsorption-desorption isotherms, and investigated for CO2 capture using a thermogravimetric analysis unit connected to a flow panel. The effect of adsorption temperature, PEI loading and CO2 partial pressure on the CO2 capture performance of the PEI-modified bentonite was examined. A cyclic CO2 adsorption-desorption test was also carried out to assess the stability of PEI-modified bentonite as a CO2 adsorbent. Bentonite in its natural state showed negligible CO2 uptake. After amine modification, the CO2 uptake increased significantly due to CO2 capture by amine species introduced via chemisorption. The PEI-modified bentonites showed high CO2 capture selectivity over N2, and exhibited excellent stability in cyclic CO2 adsorption-desorption runs.

  8. Effect of dolomite decomposition under CO2 on its multicycle CO2 capture behaviour under calcium looping conditions.

    PubMed

    de la Calle Martos, Antonio; Valverde, Jose Manuel; Sanchez-Jimenez, Pedro E; Perejón, Antonio; García-Garrido, Cristina; Perez-Maqueda, Luis A

    2016-06-28

    One of the major drawbacks that hinder the industrial competitiveness of the calcium looping (CaL) process for CO2 capture is the high temperature (∼930-950 °C) needed in practice to attain full calcination of limestone in a high CO2 partial pressure environment for short residence times as required. In this work, the multicycle CO2 capture performance of dolomite and limestone is analysed under realistic CaL conditions and using a reduced calcination temperature of 900 °C, which would serve to mitigate the energy penalty caused by integration of the CaL process into fossil fuel fired power plants. The results show that the fundamental mechanism of dolomite decomposition under CO2 has a major influence on its superior performance compared to limestone. The inert MgO grains resulting from dolomite decomposition help preserve a nanocrystalline CaO structure wherein carbonation in the solid-state diffusion controlled phase is promoted. The major role played by the dolomite decomposition mechanism under CO2 is clearly demonstrated by the multicycle CaO conversion behaviour observed for samples decomposed at different preheating rates. Limestone decomposition at slow heating rates yields a highly crystalline and poorly reactive CaCO3 structure that requires long periods to fully decarbonate and shows a severely reduced capture capacity in subsequent cycles. On the other hand, the nascent CaCO3 produced after dolomite half-decomposition consists of nanosized crystals with a fast decarbonation kinetics regardless of the preheating rate, thus fully decomposing from the very first cycle at a reduced calcination temperature into a CaO skeleton with enhanced reactivity as compared to limestone derived CaO.

  9. A preliminary investigation of cryogenic CO2 capture utilizing a reverse Brayton Cycle

    NASA Astrophysics Data System (ADS)

    Yuan, L. C.; Pfotenhauer, J. M.; Qiu, L. M.

    2014-01-01

    Utilizing CO2 capture and storage (CCS) technologies is a significant way to reduce carbon emissions from coal fired power plants. Cryogenic CO2 capture (CCC) is an innovative and promising CO2 capture technology, which has an apparent energy and environmental advantage compared to alternatives. A process of capturing CO2 from the flue gas of a coal-fired electrical power plant by cryogenically desublimating CO2 has been discussed and demonstrated theoretically. However, pressurizing the inlet flue gas to reduce the energy penalty for the cryogenic process will lead to a more complex system. In this paper, a modified CCC system utilizing a reverse Brayton Cycle is proposed, and the energy penalty of these two systems are compared theoretically.

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

    SciTech Connect

    2015-09-01

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

  11. Reducing the cost of Ca-based direct air capture of CO2.

    PubMed

    Zeman, Frank

    2014-10-07

    Direct air capture, the chemical removal of CO2 directly from the atmosphere, may play a role in mitigating future climate risk or form the basis of a sustainable transportation infrastructure. The current discussion is centered on the estimated cost of the technology and its link to "overshoot" trajectories, where atmospheric CO2 levels are actively reduced later in the century. The American Physical Society (APS) published a report, later updated, estimating the cost of a one million tonne CO2 per year air capture facility constructed today that highlights several fundamental concepts of chemical air capture. These fundamentals are viewed through the lens of a chemical process that cycles between removing CO2 from the air and releasing the absorbed CO2 in concentrated form. This work builds on the APS report to investigate the effect of modifications to the air capture system based on suggestions in the report and subsequent publications. The work shows that reduced carbon electricity and plastic packing materials (for the contactor) may have significant effects on the overall price, reducing the APS estimate from $610 to $309/tCO2 avoided. Such a reduction does not challenge postcombustion capture from point sources, estimated at $80/tCO2, but does make air capture a feasible alternative for the transportation sector and a potential negative emissions technology. Furthermore, air capture represents atmospheric reductions rather than simply avoided emissions.

  12. NUCLEAR POWERED CO2 CAPTURE FROM THE ATMOSPHERE

    SciTech Connect

    Sherman, S

    2008-09-22

    A process for capturing CO{sub 2} from the atmosphere was recently proposed. This process uses a closed cycle of sodium and calcium hydroxide, carbonate, and oxide transformations to capture dilute CO{sub 2} from the atmosphere and to generate a concentrated stream of CO{sub 2} that is amenable to sequestration or subsequent chemical transformations. In one of the process steps, a fossil-fueled lime kiln is needed, which reduces the net CO{sub 2} capture of the process. It is proposed to replace the fossil-fueled lime kiln with a modified kiln heated by a high-temperature nuclear reactor. This will have the effect of eliminating the use of fossil fuels for the process and increasing the net CO{sub 2} capture. Although the process is suitable to support sequestration, the use of a nuclear power source for the process provides additional capabilities, and the captured CO{sub 2} may be combined with nuclear-produced hydrogen to produce liquid fuels via Fischer-Tropsch synthesis or other technologies. Conceivably, such plants would be carbon-neutral, and could be placed virtually anywhere without being tied to fossil fuel sources or geological sequestration sites.

  13. Integrating MEA Regeneration with CO2 Compression and Peaking to Reduce CO2 Capture Costs

    SciTech Connect

    Kevin S. Fisher; Carrie Beitler; Curtis Rueter; Katherine Searcy; Dr. Gary Rochelle; Dr. Majeed Jassim

    2005-06-09

    Capturing CO{sub 2} from coal-fired power plants is a necessary component of any large-scale effort to reduce anthropogenic CO{sub 2} emissions. Conventional absorption/stripping with monoethanolamine (MEA) or similar solvents is the most likely current process for capturing CO{sub 2} from the flue gas at these facilities. However, one of the largest problems with MEA absorption/stripping is that conventional process configurations have energy requirements that result in large reductions in the net power plant output. Several alternative process configurations for reducing these parasitic energy requirements were investigated in this research with the assistance of the Platte River Power Authority, based on recovering energy from the CO{sub 2} compression train and using that energy in the MEA regeneration step. In addition, the feasibility of selective operation of the amine system at a higher CO{sub 2} removal efficiency during non-peak electricity demand periods was also evaluated. Four process configurations were evaluated: A generic base case MEA system with no compression heat recovery, CO{sub 2} vapor recompression heat recovery, and multipressure stripping with and without vapor recompression heat recovery. These configurations were simulated using a rigorous rate-based model, and the results were used to prepare capital and operating cost estimates. CO{sub 2} capture economics are presented, and the cost of CO{sub 2} capture (cost per tonne avoided) is compared among the base case and the alternative process configurations. Cost savings per tonne of CO{sub 2} avoided ranged from 4.3 to 9.8 percent. Energy savings of the improved configurations (8-10%, freeing up 13 to 17 MW of power for sale to the grid based on 500 MW unit ) clearly outweighed the modest increases in capital cost to implement them; it is therefore likely that one of these improved configurations would be used whenever MEA-based (or similar) scrubbing technologies are implemented. In fact

  14. Ambient CO2 capture and storage in bioelectrochemically mediated wastewater treatment.

    PubMed

    Huang, Zhe; Jiang, Daqian; Lu, Lu; Ren, Zhiyong Jason

    2016-09-01

    This study reports that wastewater can be used to capture and store CO2 directly from ambient air and produce energy. The proof-of-concept system consisted of an ion exchange resin column that captures and concentrates ambient CO2 using a moisture-driven cycle. The concentrated CO2 was then transferred into a microbial electrochemical carbon capture (MECC) reactor for carbon sequestration and hydrogen production. Data from an average batch cycle showed that approximately 8mmol/L CO2 was captured in the MECC cathode when 0.14g/LCOD was removed in the anode. With 90% hydrogen conversion efficiency, the energy intensity and CO2 absorption from the process could be 11.3kJ/gCOD and 0.49gCO2/gCOD respectively. If the proposed process is applied, over 68milliontons of atmospheric CO2 can be captured yearly during wastewater treatment in the US, which equates to significant economic values if CO2 taxes were to be implemented more widely.

  15. Development of low-cost amine-enriched solid sorbent for CO2 capture.

    PubMed

    Bachelor, Thuy Thi Nguyen; Toochinda, Pisanu

    2012-12-01

    CO2 capture amine-enriched solid sorbent using agricultural wastes, such as bagasse, or industrial wastes, such as mullite, as support materials could provide efficient alternative CO2 reduction due to their low cost and ability to shape into many forms. These amine-enriched solid sorbents were prepared by treatment with monoethanolamine (MEA), diethanolamine, piperazine (PZ), 2-(2-aminoethyl-amino) ethanol (AEEA) and mixtures of these amines. The performance of amine-enriched solid sorbents with various amine compositions was studied in a tubular column at 1 atm and an adsorption temperature of 303 K. The CO2 capture capacities of the amine-enriched solid sorbents were determined by gas chromatography at a desorption temperature of 393 K. Amine-enriched solid sorbents in this study exhibited high performance CO2 capture. The MEA-PZ-enriched solid sorbent does have the highest CO2 capture performance of the amine-enriched bagasse support-based sorbents, and the results indicate that PZ is the most effective promoter in this study. The CO2 capture performances of solid sorbents in this study were compared with commercial solid sorbents. This study could lead to the development of low-cost solid sorbents for CO2 capture that can be used in many industrial applications.

  16. Phase-Changing Ionic Liquids: CO2 Capture with Ionic Liquids Involving Phase Change

    SciTech Connect

    2010-07-01

    IMPACCT Project: Notre Dame is developing a new CO2 capture process that uses special ionic liquids (ILs) to remove CO2 from the gas exhaust of coal-fired power plants. ILs are salts that are normally liquid at room temperature, but Notre Dame has discovered a new class of ILs that are solid at room temperature and change to liquid when they bind to CO2. Upon heating, the CO2 is released for storage, and the ILs re-solidify and donate some of the heat generated in the process to facilitate further CO2 release. These new ILs can reduce the energy required to capture CO2 from the exhaust stream of a coal-fired power plant when compared to state-ofthe- art technology.

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

    PubMed

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

    2016-09-08

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

  18. First-principles assessment of CO2 capture mechanisms in aqueous piperazine solution.

    PubMed

    Stowe, Haley M; Paek, Eunsu; Hwang, Gyeong S

    2016-09-14

    Piperazine (PZ) and its blends have emerged as attractive solvents for CO2 capture, but the underlying reaction mechanisms still remain uncertain. Our study particularly focuses on assessing the relative roles of PZCOO(-) and PZH(+) produced from the PZ + CO2 reaction. PZCOO(-) is found to directly react with CO2 forming COO(-)PZCOO(-), whereas PZH(+) will not. However, COO(-)PZCOO(-) appears very unlikely to be produced in thermodynamic equilibrium with monocarbamates, suggesting that its existence would predominantly originate from the surface reaction that likely occurs. We also find production of H(+)PZCOO(-) to be more probable with increasing CO2 loading, due partly to the thermodynamic favorability of the PZH(+) + PZCOO(-) → H(+)PZCOO(-) + PZ reaction; the facile PZ liberation may contribute to its relatively high CO2 absorption rate. This study highlights an accurate description of surface reaction and the solvent composition effect is critical in thermodynamic and kinetic models for predicting the CO2 capture processes.

  19. Covalent Triazine-Based Frameworks with Ultramicropores and High Nitrogen Contents for Highly Selective CO2 Capture.

    PubMed

    Wang, Keke; Huang, Hongliang; Liu, Dahuan; Wang, Chang; Li, Jinping; Zhong, Chongli

    2016-05-03

    Porous organic frameworks (POFs) are a class of porous materials composed of organic precursors linked by covalent bonds. The objective of this work is to develop POFs with both ultramicropores and high nitrogen contents for CO2 capture. Specifically, two covalent triazine-based frameworks (CTFs) with ultramicropores (pores of width <7 Å) based on short (fumaronitrile, FUM) and wide monomers (1,4-dicyanonaphthalene, DCN) were synthesized. The obtained CTF-FUM and CTF-DCN possess excellent chemical and thermal stability with ultramicropores of 5.2 and 5.4 Å, respectively. In addition, they exhibit excellent ability to selectively capture CO2 due to ultramicroporous nature. Especially, CTF-FUM-350 has the highest nitrogen content (27.64%) and thus the highest CO2 adsorption capacity (57.2 cc/g at 298 K) and selectivities for CO2 over N2 and CH4 (102.4 and 20.5 at 298 K, respectively) among all CTF-FUM and CTF-DCN. More impressively, as far as we know, the CO2/CH4 selectivity is larger than that of all reported CTFs and ranks in top 10 among all reported POFs. Dynamic breakthrough curves indicate that both CTFs could indeed separate gas mixtures of CO2/N2 and CO2/CH4 completely.

  20. Polymer-silica hybrids for separation of CO2 and catalysis of organic reactions

    NASA Astrophysics Data System (ADS)

    Silva Mojica, Ernesto

    Porous materials comprising polymeric and inorganic segments have attracted interest from the scientific community due to their unique properties and functionalities. The physical and chemical characteristics of these materials can be effectively exploited for adsorption applications. This dissertation covers the experimental techniques for fabrication of poly(vinyl alcohol) (PVA) and silica (SiO2) porous supports, and their functionalization with polyamines for developing adsorbents with potential applications in separation of CO2 and catalysis of organic reactions. The supports were synthesized by processes involving (i) covalent cross-linking of PVA, (ii) hydrolysis and poly-condensation of silica precursors (i,e,. sol-gel synthesis), and formation of porous structures via (iii) direct templating and (iv) phase inversion techniques. Their physical structure was controlled by the proper combination of the preparation procedures, which resulted in micro-structured porous materials in the form of micro-particles, membranes, and pellets. Their adsorption characteristics were tailored by functionalization with polyethyleneimine (PEI), and their physicochemical properties were characterized by vibrational spectroscopy (FTIR, UV-vis), microscopy (SEM), calorimetry (TGA, DSC), and adsorption techniques (BET, step-switch adsorption). Spectroscopic investigations of the interfacial cross-linking reactions of PEI and PVA with glutaraldehyde (GA) revealed that PEI catalyzes the cross-linking reactions of PVA in absence of external acid catalysts. In-situ IR spectroscopy coupled with a focal plane array (FPA) image detector allowed the characterization of a gradient interface on a PEI/PVA composite membrane and the investigation of the cross-linking reactions as a function of time and position. The results served as a basis to postulate possible intermediates, and propose the reaction mechanisms. The formulation of amine-functionalized CO2 capture sorbents was based on the

  1. Computational Modeling of Mixed Solids for CO2 CaptureSorbents

    SciTech Connect

    Duan, Yuhua

    2015-01-01

    Since current technologies for capturing CO2 to fight global climate change are still too energy intensive, there is a critical need for development of new materials that can capture CO2 reversibly with acceptable energy costs. Accordingly, solid sorbents have been proposed to be used for CO2 capture applications through a reversible chemical transformation. By combining thermodynamic database mining with first principles density functional theory and phonon lattice dynamics calculations, a theoretical screening methodology to identify the most promising CO2 sorbent candidates from the vast array of possible solid materials has been proposed and validated. The calculated thermodynamic properties of different classes of solid materials versus temperature and pressure changes were further used to evaluate the equilibrium properties for the CO2 adsorption/desorption cycles. According to the requirements imposed by the pre- and post- combustion technologies and based on our calculated thermodynamic properties for the CO2 capture reactions by the solids of interest, we were able to screen only those solid materials for which lower capture energy costs are expected at the desired pressure and temperature conditions. Only those selected CO2 sorbent candidates were further considered for experimental validations. The ab initio thermodynamic technique has the advantage of identifying thermodynamic properties of CO2 capture reactions without any experimental input beyond crystallographic structural information of the solid phases involved. Such methodology not only can be used to search for good candidates from existing database of solid materials, but also can provide some guidelines for synthesis new materials. In this presentation, we apply our screening methodology to mixing solid systems to adjust the turnover temperature to help on developing CO2 capture Technologies.

  2. CO2 CAPTURE BY ABSORPTION WITH POTASSIUM CARBONATE

    SciTech Connect

    Gary T. Rochelle; Eric Chen; J. Tim Cullinane; Marcus Hilliard; Babatunde Oyenekan; Terraun Jones

    2003-07-28

    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. A rigorous thermodynamic model has been further developed with a standalone FORTRAN code to represent the CO{sub 2} vapor pressure and speciation of the new solvent. Gas chromatography has been used to measure the oxidative degradation of piperazine. The heat exchangers for the pilot plant have been received. The modifications are on schedule for start-up in November 2003.

  3. CO2 CAPTURE BY ABSORPTION WITH POTASSIUM CARBONATE

    SciTech Connect

    Gary T. Rochelle; Eric Chen; J. Tim Cullinane; Marcus Hillard; Babatunde Oyenekan

    2003-10-31

    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. A rigorous thermodynamic model has been further developed with a standalone FORTRAN code to represent the CO{sub 2} vapor pressure and speciation of the new solvent. The welding work has initiated and will be completed for a revised startup of the pilot plant in February 2004.

  4. CO2 CAPTURE BY ABSORPTION WITH POTASSIUM CARBONATE

    SciTech Connect

    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.

  5. CO2 CAPTURE BY ABSORPTION WITH POTASSIUM CARBONATE

    SciTech Connect

    Gary T. Rochelle; Eric Chen; J. Tim Cullinane; Marcus Hilliard; Terraun Jones

    2003-04-01

    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. A rigorous thermodynamic model has been developed with a stand-alone FORTRAN code to represent the CO{sub 2} vapor pressure and speciation of the new solvent. Parameters have been developed for use of the electrolyte NRTL model in AspenPlus. Analytical methods have been developed using gas chromatography and ion chromatography. The heat exchangers for the pilot plant have been ordered.

  6. CO2 CAPTURE BY ABSORPTION WITH POTASSIUM CARBONATE

    SciTech Connect

    Gary T. Rochelle; A. Frank Seibert

    2002-10-01

    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. A simple thermodynamic model has been developed to represent the CO{sub 2} vapor pressure and speciation of the new solvent. A rate model has been formulated to predict the CO{sub 2} flux with these solutions under absorber conditions. A process and instrumentation diagram and process flow diagram have been prepared for modifications of the existing pilot plant system.

  7. High-performance Polymer Membranes with Multi-functional Amphiphilic Micelles for CO2 Capture.

    PubMed

    Kim, Sang Jin; Jeon, Harim; Kim, Dong Jun; Kim, Jong Hak

    2015-11-01

    Herein, we report a high performance polymer membrane with simultaneously large improvements in the CO2 permeability and CO2/N2 selectivity. These improvements are obtained by incorporation of a multi-functional amphiphilic comb copolymer micelle, that is, poly(dimethylsiloxane)-g-poly(oxyethylene methacrylate) (PDMS-g-POEM), into a poly(amide-b-ethylene oxide) (Pebax) matrix. Both CO2 and N2 permeabilities continuously increased with PDMS-g-POEM content, whereas the CO2/N2 selectivity increased up to 40 wt % of PDMS-g-POEM, which enabled the maximum performance to approach the upper bound limit (2008). The membranes with PDMS-g-POEM exhibited greater CO2 permeability and CO2/N2 selectivity than those with a zeolitic imidazolate framework (ZIF-8), a well-known expensive inorganic filler, indicating the effectiveness of PDMS-g-POEM micelles for CO2 capture.

  8. Carbon-Based Adsorbents for Postcombustion CO2 Capture: A Critical Review.

    PubMed

    Creamer, Anne Elise; Gao, Bin

    2016-07-19

    The persistent increase in atmospheric CO2 from anthropogenic sources makes research directed toward carbon capture and storage imperative. Current liquid amine absorption technology has several drawbacks including hazardous byproducts and a high-energy requirement for regeneration; therefore, research is ongoing to develop more practical methods for capturing CO2 in postcombustion scenarios. The unique properties of carbon-based materials make them specifically promising for CO2 adsorption at low temperature and moderate to high partial pressure. This critical review aims to highlight the development of carbon-based solid sorbents for postcombustion CO2 capture. Specifically, it provides an overview of postcombustion CO2 capture processes with solid adsorbents and discusses a variety of carbon-based materials that could be used. This review focuses on low-cost pyrogenic carbon, activated carbon (AC), and metal-carbon composites for CO2 capture. Further, it touches upon the recent progress made to develop metal organic frameworks (MOFs) and carbon nanomaterials and their general CO2 sorption potential.

  9. Amines immobilized double-walled silica nanotubes for CO2 capture.

    PubMed

    Ko, Young Gun; Lee, Hyun Jeong; Oh, Hyun Chul; Choi, Ung Su

    2013-04-15

    Novel silica support has been required for high amine loading and good CO2 molecule diffusion into its pores to increase the performance of CO2 adsorbents. Herein, amine groups supported on double-walled silica nanotubes (DWSNTs) have been prepared via the immobilization of various aminosilanes (primary, secondary, tertiary, di-, and tri-aminosilanes) on DWSNT, and found to be a very effective adsorbent for CO2 capture. Amine groups immobilized DWSNTs captured CO2 reversibly in a temperature swing process at various adsorption temperatures (25°C, 50°C, 75°C, and 100°C). The amines on modified DWSNTs showed high CO2 capture capacity in the order of tri-, di-, primary, secondary, and tertiary amines. The CO2 capture capacity of all aminosilanes immobilized DWSNTs decreased linearly with the increase of the adsorption temperature. We expect that DWSNT would be able to inspire researchers to use it not only as a support for CO2 capture but also as a promising candidate for various applications.

  10. Spray Dried Sodium Zirconate: A Rapid Absorption Powder for CO2 Capture with Superior Cyclic Stability.

    PubMed

    Bamiduro, Faith; Ji, Guozhao; Brown, Andy P; Valerie A Dupont, Valerie A; Zhao, Ming; Milne, Steve J

    2017-04-03

    Improved powders for capturing CO2 at high temperatures are required for H2 production using sorption enhanced steam reforming. This paper examines the relationship between particle structure and carbonation rate for two types of Na2ZrO3 powder. Hollow spray-dried micro-granules with a wall thickness of 100-300 nm corresponding to the dimensions of the primary acetate derived particles gave ~75 wt % theoretical CO2 conversion after a process-relevant 5 min exposure to 15 vol % CO2. A conventional powder prepared by solid state reaction carbonated more slowly, only achieving 50 % conversion due to a greater proportion of the reaction requiring bulk diffusion through the densely agglomerated particles. The hollow granular structure of the spray dried powder was retained post-carbonation but chemical segregation resulted in islands of an amorphous Na-rich phase (Na2CO3) within a crystalline ZrO2 particle matrix. Despite this phase separation, the reverse reaction to re-form Na2ZrO3 could be achieved by heating each powder to 900 °C in N2 (no dwell time). This resulted in a very stable multicycle performance in 40 cycle tests using TGA for both powders. Kinetic analysis of TGA data showed the carbonation process fits an Avrami-Erofeyev 2-D nucleation and nuclei growth model, consistent with microstructural evidence of a surface driven transformation. Thus, we demonstrate that spray-drying is a viable processing route to enhance the carbon capture performance of Na2ZrO3 powder.

  11. Cost structure of a postcombustion CO2 capture system using CaO.

    PubMed

    Abanades, J Carlos; Grasa, G; Alonso, M; Rodriguez, N; Anthony, E J; Romeo, L M

    2007-08-01

    This paper presents the basic economics of an emerging concept for CO2 capture from flue gases in power plants. The complete system includes three key cost components: a full combustion power plant, a second power plant working as an oxy-fired fluidized bed calciner, and a fluidized bed carbonator interconnected with the calciner and capturing CO2 from the combustion power plant. The simplicity in the economic analysis is possible because the key cost data for the two major first components are well established in the open literature. It is shown that there is clear scope for a breakthrough in capture cost to around 15 $/t of CO2 avoided with this system. This is mainly because the capture system is generating additional power (from the additional coal fed to the calciner) and because the avoided CO2 comes from the capture of the CO2 generated by the coal fed to the calciner and the CO2 captured (as CaCO3) from the flue gases of the existing power plant, that is also released in the calciner.

  12. CO2 Capture by Absorption with Potassium Carbonate

    SciTech Connect

    Gary T. Rochelle; Marcus Hilliard; Eric Chen; Babatunde Oyenekan; Ross Dugas; John McLees; Andrew Sexton; Daniel Ellenberger

    2005-10-26

    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. Modeling of stripper performance suggests that vacuum stripping may be an attractive configuration for all solvents. Flexipac 1Y structured packing performs in the absorber as expected. It provides twice as much mass transfer area as IMTP No.40 dumped packing. Independent measurements of CO{sub 2} solubility give a CO{sub 2} loading that is 20% lower than that Cullinane's values with 3.6 m PZ at 100-120 C. The effective mass transfer coefficient (K{sub G}) in the absorber with 5 m K/2.5 m PZ appears to be 0 to 30% greater than that of 30 wt% MEA.

  13. CO2 Capture by Absorption with Potassium Carbonate

    SciTech Connect

    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.

  14. CO2 Capture by Absorption with Potassium Carbonate

    SciTech Connect

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

    2006-09-30

    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. Ethylenediamine was detected in a degraded solution of MEA/PZ solution, suggesting that piperazine is subject to oxidation. Stripper modeling has demonstrated that vacuum strippers will be more energy efficient if constructed short and fat rather than tall and skinny. The matrix stripper has been identified as a configuration that will significantly reduce energy use. Extensive measurements of CO{sub 2} solubility in 7 m MEA at 40 and 60 C have confirmed the work by Jou and Mather. Corrosion of carbon steel without inhibitors increases from 19 to 181 mpy in lean solutions of 6.2 m MEA/PZ as piperazine increases from 0 to 3.1 m.

  15. CO2 Capture by Absorption with Potassium Carbonate

    SciTech Connect

    Gary T. Rochelle; Marcus Hilliard; Eric Chen; Babatunde Oyenekan; Ross Dugas; John McLees; Andrew Sexton; Amorvadee Veawab

    2005-01-26

    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. In Campaign 3 of the pilot plant, the overall mass transfer coefficient for the stripper with 7 m MEA decreased from 0.06 to 0.01 mol/(m{sup 3}.s.kPa) as the rich loading increased from 0.45 to 0.6 mol CO{sub 2}/mol MEA. Anion chromatography has demonstrated that nitrate and nitrite are major degradation products of MEA and PZ with pure oxygen. In measurements with the high temperature FTIR in 7 m MEA the MEA vapor pressure varied from 2 to 20 Pa at 35 to 70 C. In 2.5 m PZ the PZ vapor pressure varied from 0.2 to 1 Pa from 37 to 70 C.

  16. CO2 CAPTURE BY ABSORPTION WITH POTASSIUM CARBONATE

    SciTech Connect

    Gary T. Rochelle; Marcus Hilliard; Eric Chen; Babatunde Oyenekan; Ross Dugas; John McLees

    2005-07-31

    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. The baseline campaign with 30% MEA has given heat duties from 40 to 70 kcal/gmol CO{sub 2} as predicted by the stripper model. The Flexipak 1Y structured packing gives significantly better performance than IMTP 40 duped packing in the absorber, but in the stripper the performance of the two packings is indistinguishable. The FTIR analyzer measured MEA volatility in the absorber represented by an activity coefficient of 0.7. In the MEA campaign the material balance closed with an average error of 3.5% and the energy balance had an average error of 5.9.

  17. CO2 Capture by Absorption with Potassium Carbonate

    SciTech Connect

    Gary T. Rochelle; Eric Chen; Babatunde Oyenekan; Andrew Sexton; Amorvadee Veawab

    2006-04-28

    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 final campaign of the pilot plant was completed in February 2006 with 5m K{sup +}/2.5m PZ and 6.4m K{sup +}/1.6m PZ using Flexipac AQ Style 20. The new cross-exchanger reduced the approach temperature to less than 9 C. Stripper modeling has demonstrated that a configuration with a ''Flashing Feed'' requires 6% less work that a simple stripper. The oxidative degradation of piperazine proceeds more slowly than that of monoethanolamine and produces ethylenediamine and other products. Uninhibited 5 m KHCO{sub 3}/2.5 m PZ corrodes 5 to 6 times faster that 30% MEA with 0.2 mol CO{sub 2}/mol MEA.

  18. CO2 CAPTURE BY ABSORPTION WITH POTASSIUM CARBONATE

    SciTech Connect

    Gary T. Rochelle; Eric Chen; Jennifer Lu; Babatunde Oyenekan; Ross Dugas

    2005-04-29

    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. Stripper modeling suggests the energy requirement with a simple stripper will be about the same for 5 m K{sup +}/2.5 m PZ and 7 m MEA. Modeling with a generic solvent shows that the optimum heat of CO{sub 2} desorption to minimize heat duty lies between 15 and 25 kcal/gmol. On-line pH and density measurements are effective indicators of loading and total alkalinity for the K+/PZ solvent. The baseline pilot plant campaign with 30% MEA has been started.

  19. CO2 CAPTURE BY ABSORPTION WITH POTASSIUM CARBONATE

    SciTech Connect

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

    2004-07-29

    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. CO{sub 2} mass transfer rates are second order in piperazine concentration and increase with ionic strength. Modeling of stripper performance suggests that 5 m K{sup +}/2.5 m PZ will require 25 to 46% less heat than 7 m MEA. The first pilot plant campaign was completed on June 24. The CO{sub 2} penetration through the absorber with 20 feet of Flexipac{trademark} 1Y varied from 0.6 to 16% as the inlet CO{sub 2} varied from 3 to 12% CO{sub 2} and the gas rate varied from 0.5 to 3 kg/m{sup 2}-s.

  20. CO2 CAPTURE BY ABSORPTION WITH POTASSIUM CARBONATE

    SciTech Connect

    Gary T. Rochelle; Eric Chen; Jennifer Lu; Babatunde Oyenekan; Ross Dugas

    2004-11-08

    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 stripper model with Aspen Custom Modeler and careful optimization of solvent rate suggests that 7 m MEA and 5 m K+/2.5 m PZ will be practically equivalent in energy requirement and optimum solution capacity. The multipressure stripper reduces energy consumption by 15% with a maximum pressure of 5 atm. The use of vanadium as a corrosion inhibitor will carry little risk of long-term environmental or health effects liability, but the disposal of solvent with vanadium will be subject to regulation, probably as a hazardous waste. Analysis of the pilot plant data from Campaign 1 has given values of the mass transfer coefficient consistent with the rate data from the wetted wall column. With a rich end pinch, 30% MEA should provide a capacity of 1.3-1.4 mole CO{sub 2}/kg solvent.

  1. CO2 Capture from Flue Gas by Phase Transitional Absorption

    SciTech Connect

    Liang Hu

    2009-06-30

    A novel absorption process called Phase Transitional Absorption was invented. What is the Phase Transitional Absorption? Phase Transitional Absorption is a two or multi phase absorption system, CO{sub 2} rich phase and CO{sub 2} lean phase. During Absorption, CO{sub 2} is accumulated in CO{sub 2} rich phase. After separating the two phases, CO{sub 2} rich phase is forward to regeneration. After regeneration, the regenerated CO{sub 2} rich phase combines CO{sub 2} lean phase to form absorbent again to complete the cycle. The advantage for Phase Transitional Absorption is obvious, significantly saving on regeneration energy. Because CO{sub 2} lean phase was separated before regeneration, only CO{sub 2} rich phase was forward to regeneration. The absorption system we developed has the features of high absorption rate, high loading and working capacity, low corrosion, low regeneration heat, no toxic to environment, etc. The process evaluation shows that our process is able to save 80% energy cost by comparing with MEA process.

  2. Progress in carbon dioxide separation and capture: a review.

    PubMed

    Yang, Hongqun; Xu, Zhenghe; Fan, Maohong; Gupta, Rajender; Slimane, Rachid B; Bland, Alan E; Wright, Ian

    2008-01-01

    This article reviews the progress made in CO2 separation and capture research and engineering. Various technologies, such as absorption, adsorption, and membrane separation, are thoroughly discussed. New concepts such as chemical-looping combustion and hydrate-based separation are also introduced briefly. Future directions are suggested. Sequestration methods, such as forestation, ocean fertilization and mineral carbonation techniques are also covered. Underground injection and direct ocean dump are not covered.

  3. CO2 Capture by Absorption with Potassium Carbonate

    SciTech Connect

    Gary T. Rochelle; Eric Chen; Babatunde Oyenekan; Andrew Sexton; Jason Davis; Marus Hiilliard; Qing Xu; David Van Wagener; Jorge M. Plaza

    2006-12-31

    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. The best solvent and process configuration, matrix with MDEA/PZ, offers 22% and 15% energy savings over the baseline and improved baseline, respectively, with stripping and compression to 10 MPa. The energy requirement for stripping and compression to 10 MPa is about 20% of the power output from a 500 MW power plant with 90% CO{sub 2} removal. The stripper rate model shows that a ''short and fat'' stripper requires 7 to 15% less equivalent work than a ''tall and skinny'' one. The stripper model was validated with data obtained from pilot plant experiments at the University of Texas with 5m K{sup +}/2.5m PZ and 6.4m K{sup +}/1.6m PZ under normal pressure and vacuum conditions using Flexipac AQ Style 20 structured packing. Experiments with oxidative degradation at low gas rates confirm the effects of Cu{sup +2} catalysis; in MEA/PZ solutions more formate and acetate is produced in the presence of Cu{sup +2}. At 150 C, the half life of 30% MEA with 0.4 moles CO{sub 2}/mole amine is about 2 weeks. At 100 C, less than 3% degradation occurred in two weeks. The solubility of potassium sulfate in MEA solution increases significantly with CO{sub 2} loading and decreases with MEA concentration. The base case corrosion rate in 5 M MEA/1,2M PZ is 22 mpy. With 1 wt% heat stable salt, the corrosion rate increases by 50% to 160% in the order: thiosulfate< oxalate

  4. Potassium-based sorbents from fly ash for high-temperature CO2 capture.

    PubMed

    Sanna, Aimaro; Maroto-Valer, M Mercedes

    2016-11-01

    Potassium-fly ash (K-FA) sorbents were investigated for high-temperature CO2 sorption. K-FAs were synthesised using coal fly ash as source of silica and aluminium. The synthesised materials were also mixed with Li2CO3 and Ca(OH)2 to evaluate their effect on CO2 capture. Temperature strongly affected the performance of the K-FA sorbents, resulting in a CO2 uptake of 1.45 mmol CO2/g sorbent for K-FA 1:1 at 700 °C. The CO2 sorption was enhanced by the presence of Li2CO3 (10 wt%), with the K-FA 1:1 capturing 2.38 mmol CO2/g sorbent at 700 °C in 5 min. This sorption was found to be similar to previously developed Li-Na-FA (2.54 mmol/g) and Li-FA (2.4 mmol/g) sorbents. The presence of 10 % Li2CO3 also accelerated sorption and desorption. The results suggest that the increased uptake of CO2 and faster reaction rates in presence of K-FA can be ascribed to the formation of K-Li eutectic phase, which favours the diffusion of potassium and CO2 in the material matrix. The cyclic experiments showed that the K-FA materials maintained stable CO2 uptake and reaction rates over 10 cycles.

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

    PubMed

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

    2016-06-01

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

  6. Biomimetic Membrane for CO2 Capture from Flue Gas

    SciTech Connect

    Michael C. Trachtenberg

    2007-05-31

    These Phase III experiments successfully addressed several issues needed to characterize a permeator system for application to a pulverized coal (PC) burning furnace/boiler assuming typical post-combustion cleanup devices in place. We completed key laboratory stage optimization and modeling efforts needed to move towards larger scale testing. The SOPO addressed six areas. Task 1--Post-Combustion Particle Cleanup--The first object was to determine if the Carbozyme permeator performance was likely to be reduced by particles (materials) in the flue gas stream that would either obstruct the mouth of the hollow fibers (HF) or stick to the HF bore wall surface. The second, based on the Acceptance Standards (see below), was to determine whether it would be preferable to clean the inlet gas stream (removing acid gases and particulates) or to develop methods to clean the Carbozyme permeator if performance declined due to HF block. We concluded that condensation of particle and particulate emissions, in the heat exchanger, could result in the formation of very sticky sulfate aerosols with a strong likelihood of obtruding the HF. These must be managed carefully and minimized to near-zero status before entering the permeator inlet stream. More extensive post-combustion cleanup is expected to be a necessary expense, independent of CO{sub 2} capture technology This finding is in agreement with views now emerging in the literature for a variety of CO{sub 2} capture methods. Task 2--Water Condensation--The key goal was to monitor and control temperature distributions within the permeator and between the permeator and its surroundings to determine whether water condensation in the pores or the HF bore would block flow, decreasing performance. A heat transfer fluid and delivery system were developed and employed. The result was near isothermal performance that avoided all instances of flow block. Direct thermocouple measurements provided the basis for developing a heat transfer

  7. The urgency of the development of CO2 capture from ambient air

    PubMed Central

    Lackner, Klaus S.; Brennan, Sarah; Matter, Jürg M.; Park, A.-H. Alissa; Wright, Allen; van der Zwaan, Bob

    2012-01-01

    CO2 capture and storage (CCS) has the potential to develop into an important tool to address climate change. Given society’s present reliance on fossil fuels, widespread adoption of CCS appears indispensable for meeting stringent climate targets. We argue that for conventional CCS to become a successful climate mitigation technology—which by necessity has to operate on a large scale—it may need to be complemented with air capture, removing CO2 directly from the atmosphere. Air capture of CO2 could act as insurance against CO2 leaking from storage and furthermore may provide an option for dealing with emissions from mobile dispersed sources such as automobiles and airplanes. PMID:22843674

  8. A low-energy chilled ammonia process exploiting controlled solid formation for post-combustion CO2 capture.

    PubMed

    Sutter, Daniel; Gazzani, Matteo; Mazzotti, Marco

    2016-10-20

    A new ammonia-based process for CO2 capture from flue gas has been developed, which utilizes the formation of solid ammonium bicarbonate to increase the CO2 concentration in the regeneration section of the process. Precipitation, separation, and dissolution of the solid phase are realized in a dedicated process section, while the packed absorption and desorption columns remain free of solids. Additionally, the CO2 wash section applies solid formation to enable a reduction of the wash water consumption. A rigorous performance assessment employing the SPECCA index (Specific Primary Energy Consumption for CO2 Avoided) has been implemented to allow for a comparison of the overall energy penalty between the new process and a standard ammonia-based capture process without solid formation. A thorough understanding of the relevant solid-solid-liquid-vapor phase equilibria and an accurate modeling of them have enabled the synthesis of the process, and have inspired the development of the optimization algorithm used to screen a wide range of operating conditions in equilibrium-based process simulations. Under the assumptions on which the analysis is based, the new process with controlled solid formation achieved a SPECCA of 2.43 MJ kgCO2(-1), corresponding to a reduction of 17% compared to the process without solid formation (with a SPECCA of 2.93 MJ kgCO2(-1)). Ways forward to confirm this significant improvement, and to increase the accuracy of the optimization are also discussed.

  9. CO2 Capture by Absorption with Potassium Carbonate

    SciTech Connect

    Gary T. Rochelle; Andrew Sexton; Jason Davis; Marcus Hilliard; Qing Xu; David Van Wagener; Jorge M. Plaza

    2007-03-31

    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. The best K{sup +}/PZ solvent, 4.5 m K{sup +}/4.5 m PZ, requires equivalent work of 31.8 kJ/mole CO{sub 2} when used with a double matrix stripper and an intercooled absorber. The oxidative degradation of piperazine or organic acids is reduced significantly by inhibitor A, but the production of ethylenediamine is unaffected. The oxidative degradation of piperazine in 7 m MEA/2 m PZ is catalyzed by Cu{sup ++}. The thermal degradation of MEA becomes significant at 120 C. The solubility of potassium sulfate in MEA/PZ solvents is increased at greater CO{sub 2} loading. The best solvent and process configuration, matrix with MDEA/PZ, offers 22% and 15% energy savings over the baseline and improved baseline, respectively, with stripping and compression to 10 MPa. The energy requirement for stripping and compression to 10 MPa is about 20% of the power output from a 500 MW power plant with 90% CO{sub 2} removal. The stripper rate model shows that a ''short and fat'' stripper requires 7 to 15% less equivalent work than a ''tall and skinny'' one. The stripper model was validated with data obtained from pilot plant experiments at the University of Texas with 5m K{sup +}/2.5m PZ and 6.4m K{sup +}/1.6m PZ under normal pressure and vacuum conditions using Flexipac AQ Style 20 structured packing. Experiments with oxidative degradation at low gas rates confirm the effects of Cu{sup +2} catalysis; in MEA/PZ solutions more formate and acetate is produced in the presence of Cu{sup +2}. At 150 C, the half life of 30% MEA with 0.4 moles CO{sub 2}/mole amine is about 2 weeks. At 100 C, less than 3% degradation occurred in two weeks. The solubility of potassium sulfate in MEA solution increases significantly with CO{sub 2} loading and decreases with MEA concentration. The base case corrosion

  10. Comparative Assessment of Gasification Based Coal Power Plants with Various CO2 Capture Technologies Producing Electricity and Hydrogen

    PubMed Central

    2014-01-01

    Seven different types of gasification-based coal conversion processes for producing mainly electricity and in some cases hydrogen (H2), with and without carbon dioxide (CO2) capture, were compared on a consistent basis through simulation studies. The flowsheet for each process was developed in a chemical process simulation tool “Aspen Plus”. The pressure swing adsorption (PSA), physical absorption (Selexol), and chemical looping combustion (CLC) technologies were separately analyzed for processes with CO2 capture. The performances of the above three capture technologies were compared with respect to energetic and exergetic efficiencies, and the level of CO2 emission. The effect of air separation unit (ASU) and gas turbine (GT) integration on the power output of all the CO2 capture cases is assessed. Sensitivity analysis was carried out for the CLC process (electricity-only case) to examine the effect of temperature and water-cooling of the air reactor on the overall efficiency of the process. The results show that, when only electricity production in considered, the case using CLC technology has an electrical efficiency 1.3% and 2.3% higher than the PSA and Selexol based cases, respectively. The CLC based process achieves an overall CO2 capture efficiency of 99.9% in contrast to 89.9% for PSA and 93.5% for Selexol based processes. The overall efficiency of the CLC case for combined electricity and H2 production is marginally higher (by 0.3%) than Selexol and lower (by 0.6%) than PSA cases. The integration between the ASU and GT units benefits all three technologies in terms of electrical efficiency. Furthermore, our results suggest that it is favorable to operate the air reactor of the CLC process at higher temperatures with excess air supply in order to achieve higher power efficiency. PMID:24578590

  11. Comparative Assessment of Gasification Based Coal Power Plants with Various CO2 Capture Technologies Producing Electricity and Hydrogen.

    PubMed

    Mukherjee, Sanjay; Kumar, Prashant; Hosseini, Ali; Yang, Aidong; Fennell, Paul

    2014-02-20

    Seven different types of gasification-based coal conversion processes for producing mainly electricity and in some cases hydrogen (H2), with and without carbon dioxide (CO2) capture, were compared on a consistent basis through simulation studies. The flowsheet for each process was developed in a chemical process simulation tool "Aspen Plus". The pressure swing adsorption (PSA), physical absorption (Selexol), and chemical looping combustion (CLC) technologies were separately analyzed for processes with CO2 capture. The performances of the above three capture technologies were compared with respect to energetic and exergetic efficiencies, and the level of CO2 emission. The effect of air separation unit (ASU) and gas turbine (GT) integration on the power output of all the CO2 capture cases is assessed. Sensitivity analysis was carried out for the CLC process (electricity-only case) to examine the effect of temperature and water-cooling of the air reactor on the overall efficiency of the process. The results show that, when only electricity production in considered, the case using CLC technology has an electrical efficiency 1.3% and 2.3% higher than the PSA and Selexol based cases, respectively. The CLC based process achieves an overall CO2 capture efficiency of 99.9% in contrast to 89.9% for PSA and 93.5% for Selexol based processes. The overall efficiency of the CLC case for combined electricity and H2 production is marginally higher (by 0.3%) than Selexol and lower (by 0.6%) than PSA cases. The integration between the ASU and GT units benefits all three technologies in terms of electrical efficiency. Furthermore, our results suggest that it is favorable to operate the air reactor of the CLC process at higher temperatures with excess air supply in order to achieve higher power efficiency.

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

    PubMed

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

    2015-08-04

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

  13. Ab initio thermodynamic approach to identify mixed solid sorbents for CO2 capture technology

    DOE PAGES

    Duan, Yuhua

    2015-10-15

    Because the current technologies for capturing CO2 are still too energy intensive, new materials must be developed that can capture CO2 reversibly with acceptable energy costs. At a given CO2 pressure, the turnover temperature (Tt) of the reaction of an individual solid that can capture CO2 is fixed. Such Tt may be outside the operating temperature range (ΔTo) for a practical capture technology. To adjust Tt to fit the practical ΔTo, in this study, three scenarios of mixing schemes are explored by combining thermodynamic database mining with first principles density functional theory and phonon lattice dynamics calculations. Our calculated resultsmore » demonstrate that by mixing different types of solids, it’s possible to shift Tt to the range of practical operating temperature conditions. According to the requirements imposed by the pre- and post- combustion technologies and based on our calculated thermodynamic properties for the CO2 capture reactions by the mixed solids of interest, we were able to identify the mixing ratios of two or more solids to form new sorbent materials for which lower capture energy costs are expected at the desired pressure and temperature conditions.« less

  14. Design, synthesis, and evaluation of nonaqueous silylamines for efficient CO2 capture.

    PubMed

    Switzer, Jackson R; Ethier, Amy L; Hart, Emily C; Flack, Kyle M; Rumple, Amber C; Donaldson, Jordan C; Bembry, Ashley T; Scott, Owen M; Biddinger, Elizabeth J; Talreja, Manish; Song, Myoung-Geun; Pollet, Pamela; Eckert, Charles A; Liotta, Charles L

    2014-01-01

    A series of silylated amines have been synthesized for use as reversible ionic liquids in the application of post-combustion carbon capture. We describe a molecular design process aimed at influencing industrially relevant carbon capture properties, such as viscosity, temperature of reversal, and enthalpy of regeneration, while maximizing the overall CO2 -capture capacity. A strong structure-property relationship among the silylamines is demonstrated in which minor structural modifications lead to significant changes in the bulk properties of the reversible ionic liquid formed from reaction with CO2 .

  15. Process for capturing CO2 arising from the calcination of the CaCO3 used in cement manufacture.

    PubMed

    Rodríguez, N; Alonso, M; Grasa, G; Abanades, J Carlos

    2008-09-15

    This paper outlines a new CaCO3 calcination method for producing a stream of CO2 (suitable for permanent geological storage after purification and compression). The process is based on the use of very hot CaO particles (T >1000 degrees C) to transfer heat from a circulating fluidized bed combustor (CFBC) to a calciner (fluidized with CO2 and/or steam). Since the fluidized bed combustor and calciner have separate atmospheres, the CO2 resulting from the decomposition of CaCO3 can be captured, while the CO2 generated in the combustion of the fuel in air is emitted to the atmosphere. We demonstrate that with this system it is possible to reduce the CO2 emissions of a cement plant by around 60%. Furthermore, since the key pieces of equipment are similar to the commercial CFBCs used in power generation plants, it is possible to establish the additional investment required for the system and to estimate the cost per ton of CO2 avoided for this process to be about 19 $/tCO2 avoided.

  16. Theoretical simulation of CO2 capture in organic cage impregnated with polyoxometalates.

    PubMed

    Gao, Jingyuan; Li, Wenliang; Zhang, Jingping

    2017-04-05

    To explore the adsorption and separation properties of CO2 in a novel material consisting of a series of polyoxometalates (POMs) impregnated within supramolecular porous catenane (shorted as SPC), grand canonical Monte Carlo (GCMC) simulations and ab initio calculations were used. GCMC simulations showed this impregnation can enhance CO2 /CH4 (or CO2 /N2 ) selectivity almost 30 times compared to the bare SPC due to the strong interaction of CO2 with the nPOMs@SPC structures. And, the loading of CO2 inhibits the adsorption of CH4 (or N2 ) as CO2 occupying the preferred adsorption sites. Furthermore, the effect of number, mass, and volume of POMs inserted in SPC on CO2 /CH4 (or CO2 /N2 ) selectivity over large pressure range was investigated in detail. Additionally, the accurate ab initio calculations further confirmed our GCMC simulations. As a result, the proposed nPOMs@SPC structures are promising candidates for CO2 /N2 and CO2 /CH4 separations. © 2017 Wiley Periodicals, Inc.

  17. Hopewell Beneficial CO2 Capture for Production of Fuels, Fertilizer and Energy

    SciTech Connect

    UOP; Honeywell Resins & Chemicals; Honeywell Process Solutions; Aquaflow Bionomics Ltd

    2010-09-30

    For Phase 1 of this project, the Hopewell team developed a detailed design for the Small Scale Pilot-Scale Algal CO2 Sequestration System. This pilot consisted of six (6) x 135 gallon cultivation tanks including systems for CO2 delivery and control, algal cultivation, and algal harvesting. A feed tank supplied Hopewell wastewater to the tanks and a receiver tank collected the effluent from the algal cultivation system. The effect of environmental parameters and nutrient loading on CO2 uptake and sequestration into biomass were determined. Additionally the cost of capturing CO2 from an industrial stack emission at both pilot and full-scale was determined. The engineering estimate evaluated Amine Guard technology for capture of pure CO2 and direct stack gas capture and compression. The study concluded that Amine Guard technology has lower lifecycle cost at commercial scale, although the cost of direct stack gas capture is lower at the pilot scale. Experiments conducted under high concentrations of dissolved CO2 did not demonstrate enhanced algae growth rate. This result suggests that the dissolved CO2 concentration at neutral pH was already above the limiting value. Even though dissolved CO2 did not show a positive effect on biomass growth, controlling its value at a constant set-point during daylight hours can be beneficial in an algae cultivation stage with high algae biomass concentration to maximize the rate of CO2 uptake. The limited enhancement of algal growth by CO2 addition to Hopewell wastewater was due at least in part to the high endogenous CO2 evolution from bacterial degradation of dissolved organic carbon present at high levels in the wastewater. It was found that the high level of bacterial activity was somewhat inhibitory to algal growth in the Hopewell wastewater. The project demonstrated that the Honeywell automation and control system, in combination with the accuracy of the online pH, dissolved O2, dissolved CO2, turbidity, Chlorophyll A and

  18. Enhanced CO2 capture on graphene via N, S dual-doping

    NASA Astrophysics Data System (ADS)

    Li, Jieyuan; Hou, Meiling; Chen, Yanqiu; Cen, Wanglai; Chu, Yinghao; Yin, Shi

    2017-03-01

    N, S doped graphene-based materials have been recently recognized as promising adsorbents for CO2 capture, but understanding of the adsorption mechanism at the atomic level is still limited. Herein, the local structures and promotion mechanism of CO2 capture by N, S doped graphene were investigated by combining density functional theory and ab initio thermodynamics. A single vacancy defected graphene involving N, S dual-doping was found to be a superior adsorbent for CO2 capture under mild conditions (<100 °C, 1 atm). The enhanced CO2 adsorption performance should be ascribed to a charge delivery channel along the S → N → CO2 path, leading to extra charge transfer from graphene to CO2. It is worth mentioning that the extra charge transfer was stimulated by the unique sp2 hybridization of pyridine N and further enhanced by S in N, S dual-doped graphene. A possible mechanism has been proposed to explain the high adsorption performance of CO2 by N, S dual-doped graphene, which offers insights for the design of new graphene-based adsorbents.

  19. Amine-modified ordered mesoporous silica: The effect of pore size on CO2 capture performance

    NASA Astrophysics Data System (ADS)

    Wang, Lin; Yao, Manli; Hu, Xin; Hu, Gengshen; Lu, Jiqing; Luo, Mengfei; Fan, Maohong

    2015-01-01

    The objective of current research is to investigate the effect of pore size of mesoporous silica supports on the CO2 capture performance of solid amine sorbents. Two ordered mesoporous silicas (OMS) with different pore sizes (5.6 nm and 7.6 nm) were synthesized as tetraethylenepentamine (TEPA) supports. A serious of techniques, such as physical adsorption, infrared spectroscopy and thermal gravimetric analysis were used to characterize the solid amine sorbents. The CO2 capture performances of the sorbents were evaluated using breakthrough method with a fixed-bed reactor equipped with an online mass spectrometer. The experimental results indicate that the pore size has significant influence on CO2 capture performance. Larger pore size could decrease the mass transfer resistance and increase the interaction between CO2 and TEPA. Therefore, OMS-7.6 is better than OMS-5.6 as amine support. The highest CO2 sorption capacities achieved with OMS-7.6 with 50 wt% TEPA loading (OMS-7.6-50) in the absence and presence of moisture are 3.45 mmol/g and 4.28 mmol/g, respectively, under the conditions of 10.0% CO2/N2 mixture at 75 °C. Cyclic CO2 adsorption-desorption experiments indicate that the solid amine sorbents are fairly stable and regenerable.

  20. CO2 capture in ionic liquid 1-alkyl-3-methylimidazolium acetate: a concerted mechanism without carbene.

    PubMed

    Yan, Fangyong; Dhumal, Nilesh R; Kim, Hyung J

    2017-01-04

    Ionic liquids (ILs) provide a promising medium for CO2 capture. Recently, the family of ILs comprising imidazolium-based cations and acetate anions, such as 1-ethyl-3-methylimidazolium acetate (EMI(+)OAc(-)), has been found to react with CO2 and form carboxylate compounds. N-Heterocyclic carbene (NHC) is widely assumed to be responsible by directly reacting with CO2 though NHC has not been detected in these ILs. Herein, a computational analysis of CO2 capture in EMI(+)OAc(-) is presented. Quantum chemistry calculations predict that NHC is unstable in a polar environment, suggesting that NHC is not formed in EMI(+)OAc(-). Ab initio molecular dynamics simulations indicate that an EMI(+) ion "activated" by the approach of a CO2 molecule can donate its acidic proton to a neighboring OAc(-) anion and form a carboxylate compound with the CO2 molecule. Analysis of this termolecular process indicates that the EMI(+)-to-OAc(-) proton transfer and the formation of 1-ethyl-3-methylimidazolium-2-carboxylate occur essentially concurrently. Based on these findings, a novel concerted mechanism that does not involve NHC is proposed for CO2 capture.

  1. Advanced Amine Solvent Formulations and Process Integration for Near-Term CO2 Capture Success

    SciTech Connect

    Fisher, Kevin S.; Searcy, Katherine; Rochelle, Gary T.; Ziaii, Sepideh; Schubert, Craig

    2007-06-28

    This Phase I SBIR project investigated the economic and technical feasibility of advanced amine scrubbing systems for post-combustion CO2 capture at coal-fired power plants. Numerous combinations of advanced solvent formulations and process configurations were screened for energy requirements, and three cases were selected for detailed analysis: a monoethanolamine (MEA) base case and two “advanced” cases: an MEA/Piperazine (PZ) case, and a methyldiethanolamine (MDEA) / PZ case. The MEA/PZ and MDEA/PZ cases employed an advanced “double matrix” stripper configuration. The basis for calculations was a model plant with a gross capacity of 500 MWe. Results indicated that CO2 capture increased the base cost of electricity from 5 cents/kWh to 10.7 c/kWh for the MEA base case, 10.1 c/kWh for the MEA / PZ double matrix, and 9.7 c/kWh for the MDEA / PZ double matrix. The corresponding cost per metric tonne CO2 avoided was 67.20 $/tonne CO2, 60.19 $/tonne CO2, and 55.05 $/tonne CO2, respectively. Derated capacities, including base plant auxiliary load of 29 MWe, were 339 MWe for the base case, 356 MWe for the MEA/PZ double matrix, and 378 MWe for the MDEA / PZ double matrix. When compared to the base case, systems employing advanced solvent formulations and process configurations were estimated to reduce reboiler steam requirements by 20 to 44%, to reduce derating due to CO2 capture by 13 to 30%, and to reduce the cost of CO2 avoided by 10 to 18%. These results demonstrate the potential for significant improvements in the overall economics of CO2 capture via advanced solvent formulations and process configurations.

  2. Finely tuning MOFs towards high-performance post-combustion CO2 capture materials.

    PubMed

    Wang, Qian; Bai, Junfeng; Lu, Zhiyong; Pan, Yi; You, Xiaozeng

    2016-01-11

    CO2 capture science and technology, particularly for the post-combustion CO2 capture, has become one of very important research fields, due to great concern of global warming. Metal-organic frameworks (MOFs) with a unique feature of structural fine-tunability, unlike the traditional porous solid materials, can provide many and powerful platforms to explore high-performance adsorbents for post-combustion CO2 capture. Until now, several strategies for finely tuning MOF structures have been developed, in which either the larger quadrupole moment and polarizability of CO2 are considered: metal ion change (I), functional groups attachment (II) and functional group insertion (III), vary the electronic nature of the pore surface; or targeting the smaller kinetic diameter of CO2 over N2 is focused on: framework interpenetration (IV), ligand shortening (V) and coordination site shifting (VI) contract the pore size of frameworks to improve their CO2 capture properties. In this review, from the viewpoint of synthetic materials scientists/chemists, we would like to introduce and summarize these strategies based upon recent work published by other groups and ourselves.

  3. Boron-Functionalized Graphene Oxide-Organic Frameworks for Highly Efficient CO2 Capture.

    PubMed

    Haque, Enamul; Islam, Md Monirul; Pourazadi, Ehsan; Sarkar, Shuranjan; Harris, Andrew T; Minett, Andrew I; Yanmaz, Ekrem; Alshehri, Saad M; Ide, Yusuke; Wu, Kevin C-W; Kaneti, Yusuf Valentino; Yamauchi, Yusuke; Hossain, Md Shahriar A

    2017-02-01

    The capture and storage of CO2 have been suggested as an effective strategy to reduce the global emissions of greenhouse gases. Hence, in recent years, many studies have been carried out to develop highly efficient materials for capturing CO2 . Until today, different types of porous materials, such as zeolites, porous carbons, N/B-doped porous carbons or metal-organic frameworks (MOFs), have been studied for CO2 capture. Herein, the CO2 capture performance of new hybrid materials, graphene-organic frameworks (GOFs) is described. The GOFs were synthesized under mild conditions through a solvothermal process using graphene oxide (GO) as a starting material and benzene 1,4-diboronic acid as an organic linker. Interestingly, the obtained GOF shows a high surface area (506 m(2)  g(-1) ) which is around 11 times higher than that of GO (46 m(2)  g(-1) ), indicating that the organic modification on the GO surface is an effective way of preparing a porous structure using GO. Our synthetic approach is quite simple, facile, and fast, compared with many other approaches reported previously. The synthesized GOF exhibits a very large CO2 capacity of 4.95 mmol g(-1) at 298 K (1 bar), which is higher those of other porous materials or carbon-based materials, along with an excellent CO2 /N2 selectivity of 48.8.

  4. Microscopic investigations of site and functional selectivity of triazole for CO2 capture and catalytic applications.

    PubMed

    Boulmène, Reda; Prakash, Muthuramalingam; Hochlaf, Majdi

    2016-11-02

    Ab initio and DFT studies on CO2 interacting with different tautomers and isomers of triazole (TZ) are carried out to understand the adsorption mechanism and their mutual preferential sites. We used post Hartree-Fock methods (MP2, CCSD(T), and CCSD(T)-F12) and various DFTs (PBE, PBE0, M05-2X, and M11) with and without considering the dispersion correction for comparison. We determined hence the equilibrium structures, vibrational frequencies and binding energies of TZ-CO2 clusters and mapped their potential energy surfaces along the intermonomer coordinates. We find that the most stable TZ-CO2 clusters, some of them are already known, are not relevant for CO2 capture in porous materials. In addition, we show that the bonding between TZ and CO2 is due to various kinds of noncovalent interactions such as π-stacking, acid-base pair electron donor-electron acceptor (EDA) interactions along with N-HO and C-HO H-bonds with CO2. Our analysis reveals the existence of site selectivity effects when CO2 binds to TZ. These effects are related to the magnitude of the interaction potentials, in the order EDA (+N-HO) > EDA (+C-HO) > C(δ+)N[double bond, length as m-dash]N > π-stacking > σ type N-HO > C-HO H-bonds. This is the first report on the importance of competition between EDA, π-stacking and σ-bonds for CO2 capture and catalytic applications. Findings from this work may be used to give insights into the site specific CO2 capture ability of porous materials such as metal organic frameworks (MOFs), zeolitic imidazolate frameworks (ZIFs) or functionalized polymers. Finally, we show that IR spectroscopy of CO2 within the pores is neither a specific nor an efficient marker in probe-molecule experiments.

  5. CO2 capture by means of an enzyme-based reactor

    NASA Technical Reports Server (NTRS)

    Cowan, R. M.; Ge, J-J; Qin, Y-J; McGregor, M. L.; Trachtenberg, M. C.

    2003-01-01

    We report a means for efficient and selective extraction of carbon dioxide (CO(2)) at low to medium concentration from mixed gas streams. CO(2) capture was accomplished by use of a novel enzyme-based, facilitated transport contained liquid membrane (EBCLM) reactor. The parametric studies we report explore both structural and operational parameters of this design. The structural parameters include carbonic anhydrase (CA) concentration, buffer concentration and pH, and liquid membrane thickness. The operational parameters are temperature, humidity of the inlet gas stream, and CO(2) concentration in the feed stream. The data show that this system effectively captures CO(2) over the range 400 ppm to at least 100,000 ppm, at or around ambient temperature and pressure. In a single pass across this homogeneous catalyst design, given a feed of 0.1% CO(2), the selectivity of CO(2) versus N(2) is 1,090 : 1 and CO(2) versus O(2) is 790 :1. CO(2) permeance is 4.71 x 10(-8) molm(-2) Pa(-1) sec(-1). The CLM design results in a system that is very stable even in the presence of dry feed and sweep gases.

  6. Towards the rational design of organic/inorganic interface for solid supported CO2 capture

    NASA Astrophysics Data System (ADS)

    He, Feng

    Monoethanolamine (MEA, HO(CH2)2NH2) aqueous solution based CO2 capture is the current technology used to mitigate power plants' green house gas emission. Solid based CO2 capture technique is regarded as a promising alternative, because it is more cost-effective and environmentally friendly than the solution based technique. Recently, solid-supported CO2 capture on MEA modified TiO 2 powders has been demonstrated [1]. It is believed that the main reaction pathway involved in solid-supported amine based CO2 capture is similar to the reaction in the amine solution, where the amine group reacts with CO2 to form carbamate (--NHCOO--). From the previous work on the MEA/TiO2 (110) system [2], it is found that MEA covered rutile TiO2 (110) did not capture CO 2. The main reaction pathway in this system was blocked because the amine group attached to the surface. In order to design a functional system, we proposed two possible mechanisms to free --NH2 from rutile TiO2 (110) surface. In this work, we investigated one of our six candidates, the 3-Amino-1-propanol (3AP, HO(CH2) 3NH2) molecule. The classical reactive force field (ReaxFF) [3] method has been employed to investigate the 3AP/TiO2 (110) system with emphasis on binding configurations and binding energies. We found that the amine group of 3AP did not attach to the rutile TiO2 (110) surface, indicating the CO2 capture capability of the 3AP/TiO 2 (110) system, which was confirmed by our experimental collaborators [4].

  7. An asymmetric tubular ceramic-carbonate dual phase membrane for high temperature CO2 separation.

    PubMed

    Dong, Xueliang; Ortiz Landeros, José; Lin, Y S

    2013-10-25

    For the first time, a tubular asymmetric ceramic-carbonate dual phase membrane was prepared by a centrifugal casting technique and used for high temperature CO2 separation. This membrane shows high CO2 permeation flux and permeance.

  8. Post-Combustion and Pre-Combustion CO2 Capture Solid Sorbents

    SciTech Connect

    Siriwardane, R.V.; Stevens, R.W.; Robinson, Clark

    2007-11-01

    Combustion of fossil fuels is one of the major sources of the greenhouse gas CO2. Pressure swing adsorption/sorption (PSA/PSS) and temperature swing adsorption/sorption (TSA/TSS) are some of the potential techniques that could be utilized for removal of CO2 from fuel gas streams. It is very important to develop sorbents to remove CO2 from fuel gas streams that are applicable for a wide range of temperatures. NETL researchers have developed novel CO2 capture sorbents for low, moderate, and high temperature applications. A novel liquid impregnated solid sorbent was developed for CO2 removal in the temperature range of ambient to 60 °C. The sorbent is regenerable at 60 – 80 °C. The sorbent formulations were prepared to be suitable for various reactor configurations (i.e., fixed and fluidized bed). Minimum fluidization gas velocities were also determined. Multi-cycle tests conducted in an atmospheric bench scale reactor with simulated flue gas indicated that the sorbent retains its CO2 sorption capacity with a CO2 removal efficiency of approximately 99% and was unaffected by presence of water vapor. The sorbent was subsequently commercially prepared by Süd Chemie to determine the viability of the sorbent for mass production. Subsequent testing showed that the commercially-synthesized sorbent possesses the same properties as the lab-synthesized equivalent. An innovative solid sorbent containing mixture of alkali earth and alkali compounds was developed for CO2 removal at 200 – 315°C from high pressure gas streams suitable for IGCC systems. The sorbent showed very high capacity for CO2 removal from a gas streams containing 28% CO2 at 200 °C and at 20 atm during a lab scale reactor test. This sorbent can be regenerated at 20 atm and at 375 °C utilizing a gas stream containing steam. High pressure enhanced the CO2 sorption process. Bench scale testing showed consistent capacities and regenerability. A unique high temperature solid sorbent was developed for CO2

  9. Dehydrated Prussian Blues for CO2 Storage and Separation Applications

    SciTech Connect

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

    2010-08-13

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

  10. Molecular simulations of nitrogen-doped hierarchical carbon adsorbents for post-combustion CO2 capture.

    PubMed

    Psarras, Peter; He, Jiajun; Wilcox, Jennifer

    2016-10-19

    A present challenge in the mitigation of anthropogenic CO2 emissions involves the design of less energy- and water-intensive capture technologies. Sorbent-based capture represents a promising solution, as these materials have negligible water requirements and do not incur the heavy energy penalties associated with solvent regeneration. However, to be considered competitive with traditional technologies (i.e., MEA capture), these sorbents must exhibit a high CO2 loading capacity and high CO2/N2 selectivity. It has been reported that ultramicroporous character and surface nitrogen functionality are of great importance to the enhancement of CO2 capacity and CO2/N2 selectivity. However, the role of pore size in combination with surface functionality in the enhancement of these properties remains unclear. To investigate these effects, grand canonical Monte Carlo (GCMC) simulations were carried out on pure and N-functionalized 3-layer graphitic slit-pore models and compared to experimental results for two high performing materials reported elsewhere. We show that the quaternary, pyridinic, and especially the oxidized pyridinic group lend to enhanced performance, with the latter providing exceptional CO2 loading (4.31 mmol g(-1)) and CO2/N2 selectivity (138.3 : 1). Increasing surface nitrogen content resulted in enhanced loading and excellent CO2/N2 selectivity (45.8 : 1-55.9 : 1), provided that the sorbent has significant ultramicroporous character. Additionally, we elucidate a threshold pore width, under which N-functionalization becomes increasingly influential on performance parameters, and show how this threshold changes with application (PC vs. NGCC capture). Finally, we propose that an alternative functionality - the nitroso group - may be responsible for the enhanced performance of some recent materials reported in the literature.

  11. Optimal synthesis of a pressure swing adsorption process for CO2 capture

    SciTech Connect

    Agarwal, A.; Biegler, L.; Zitney, S.

    2008-01-01

    The emission of carbon dioxide from cement industry and power plants that burn fossil fuels is the major cause for the accumulation of CO2 in the atmosphere, which causes long-range environmental problems. One option to mitigate the emission of CO2 is to capture it from the emission sources and store it to the ocean or depleted oil field or use it for enhanced oil recovery. CO2 recovery has been achieved by gas absorption employing solutions of carbonates and alkanolamines. However, this process is energy-intensive for the regeneration of solvent and also faces problems due to corrosion. Recently, the pressure swing adsorption (PSA) process has been considered as an alternative to the absorption process. PSA processes have been widely applied for the removal of CO2 from various feed mixtures, such as CO2 in the steam reformer off gas, landfill gas and natural gas. In all these commercial PSA cycles, the weakly adsorbed component in the mixture is the desired product and enriching the strongly adsorbed CO2 is not a concern. On the other hand, for the capture of CO2 for sequestration, it is necessary to concentrate the CO2 to a high purity to reduce the compression and transportation cost. Thus, it is necessary to develop a PSA cycle by which a high-purity product for the strongly adsorbed component with a high recovery is obtained. A multitude of PSA cycles and adsorbents have been developed for producing highly pure heavy component (CO2) from feedstock with low CO2 concentration. Kikkinides et al. suggested a 4-bed 4-step process with activated carbon as the sorbent and could recover 68% of CO2 at 99.997% purity. Chue et al. compared activated carbon and zeolite 13X on a 3-bed 7-step process and concluded that the latter is better than the former for CO2 recovery. However, the CO2 recovery was low in their process due to the lack of a countercurrent step in the chosen cycle. Choi et al. reported more than 70% CO2 recovery at more than 90% purity for a modified 3

  12. Electrochemical Capture and Release of CO2 in Aqueous Electrolytes Using an Organic Semiconductor Electrode.

    PubMed

    Apaydin, Dogukan H; Gora, Monika; Portenkirchner, Engelbert; Oppelt, Kerstin T; Neugebauer, Helmut; Jakesova, Marie; Głowacki, Eric D; Kunze-Liebhäuser, Julia; Zagorska, Malgorzata; Mieczkowski, Jozef; Sariciftci, Niyazi Serdar

    2017-04-06

    Developing efficient methods for capture and controlled release of carbon dioxide is crucial to any carbon capture and utilization technology. Herein we present an approach using an organic semiconductor electrode to electrochemically capture dissolved CO2 in aqueous electrolytes. The process relies on electrochemical reduction of a thin film of a naphthalene bisimide derivative, 2,7-bis(4-(2-(2-ethylhexyl)thiazol-4-yl)phenyl)benzo[lmn][3,8]phenanthroline-1,3,6,8(2H,7H)-tetraone (NBIT). This molecule is specifically tailored to afford one-electron reversible and one-electron quasi-reversible reduction in aqueous conditions while not dissolving or degrading. The reduced NBIT reacts with CO2 to form a stable semicarbonate salt, which can be subsequently oxidized electrochemically to release CO2. The semicarbonate structure is confirmed by in situ IR spectroelectrochemistry. This process of capturing and releasing carbon dioxide can be realized in an oxygen-free environment under ambient pressure and temperature, with uptake efficiency for CO2 capture of ∼2.3 mmol g(-1). This is on par with the best solution-phase amine chemical capture technologies available today.

  13. Evaluation of a CO2 -free commercial mosquito attractant to capture triatomines in the laboratory.

    PubMed

    Guidobaldi, F; Guerenstein, P G

    2013-12-01

    Efforts have been made to develop vertebrate odor-based attractants to lure hematophagous triatomines into traps. However, more work is needed to reach a practical, cheap, and efficient odor lure. We carried out attraction and capture tests in a dual-choice olfactometer and a pitfall trap. Here we report that a three-component, CO2 -free, synthetic blend of vertebrate odor (consisting of ammonia, L(+) lactic acid and hexanoic acid, and known as Sweetscent®) significantly induces 3(rd) -instar Rhodnius prolixus and Triatoma infestans nymphs to fall into the test capture-tube of the olfactometer. Blend constituents presented singly or in two-component blends did not evoke a response and, therefore, we propose that the insects respond specifically to the three-component blend in a synergistic way. When tested in a pitfall trap in an experimental arena, this blend induced capture in 37.5% of the lured traps, whereas 9% of the nymphs tested were captured in a single night. No insects were captured in control traps. Our work represents a proof-of-concept regarding capture of triatomines using host odor-based, CO2 -free synthetic mixtures as lures for pitfall traps. CO2 -free lures are more practical for field work than natural or CO2 -containing synthetic blends.

  14. Integrated CO2 capture-fixation chemistry via interfacial ionic liquid catalyst in laminar gas/liquid flow.

    PubMed

    Vishwakarma, Niraj K; Singh, Ajay K; Hwang, Yoon-Ho; Ko, Dong-Hyeon; Kim, Jin-Oh; Babu, A Giridhar; Kim, Dong-Pyo

    2017-03-06

    Simultaneous capture of carbon dioxide (CO2) and its utilization with subsequent work-up would significantly enhance the competitiveness of CO2-based sustainable chemistry over petroleum-based chemistry. Here we report an interfacial catalytic reaction platform for an integrated autonomous process of simultaneously capturing/fixing CO2 in gas-liquid laminar flow with subsequently providing a work-up step. The continuous-flow microreactor has built-in silicon nanowires (SiNWs) with immobilized ionic liquid catalysts on tips of cone-shaped nanowire bundles. Because of the superamphiphobic SiNWs, a stable gas-liquid interface maintains between liquid flow of organoamines in upper part and gas flow of CO2 in bottom part of channel. The intimate and direct contact of the binary reagents leads to enhanced mass transfer and facilitating reactions. The autonomous integrated platform produces and isolates 2-oxazolidinones and quinazolines-2,4(1H,3H)-diones with 81-97% yields under mild conditions. The platform would enable direct CO2 utilization to produce high-valued specialty chemicals from flue gases without pre-separation and work-up steps.

  15. Integrated CO2 capture-fixation chemistry via interfacial ionic liquid catalyst in laminar gas/liquid flow

    PubMed Central

    Vishwakarma, Niraj K.; Singh, Ajay K.; Hwang, Yoon-Ho; Ko, Dong-Hyeon; Kim, Jin-Oh; Babu, A. Giridhar; Kim, Dong-Pyo

    2017-01-01

    Simultaneous capture of carbon dioxide (CO2) and its utilization with subsequent work-up would significantly enhance the competitiveness of CO2-based sustainable chemistry over petroleum-based chemistry. Here we report an interfacial catalytic reaction platform for an integrated autonomous process of simultaneously capturing/fixing CO2 in gas–liquid laminar flow with subsequently providing a work-up step. The continuous-flow microreactor has built-in silicon nanowires (SiNWs) with immobilized ionic liquid catalysts on tips of cone-shaped nanowire bundles. Because of the superamphiphobic SiNWs, a stable gas–liquid interface maintains between liquid flow of organoamines in upper part and gas flow of CO2 in bottom part of channel. The intimate and direct contact of the binary reagents leads to enhanced mass transfer and facilitating reactions. The autonomous integrated platform produces and isolates 2-oxazolidinones and quinazolines-2,4(1H,3H)-diones with 81–97% yields under mild conditions. The platform would enable direct CO2 utilization to produce high-valued specialty chemicals from flue gases without pre-separation and work-up steps. PMID:28262667

  16. High-Throughput Screening of Metal-Organic Frameworks for CO2 Capture in the Presence of Water.

    PubMed

    Li, Song; Chung, Yongchul G; Snurr, Randall Q

    2016-10-11

    Competitive coadsorption of water is a major problem in the deployment of adsorption-based CO2 capture. Water molecules may compete for adsorption sites, reducing the capacity of the material, and dehumidification prior to separating CO2 from N2 increases process complexity and cost. The development of adsorbent materials that can selectively adsorb CO2 in the presence of water would be a major step forward in the deployment of CO2 capture materials in practice. In this study, large-scale computational screening was carried out to search for metal-organic frameworks (MOFs) with high selectivity toward CO2 over H2O. Calculating framework charges for thousands of MOFs is a significant challenge, so initial screening used a fast, but approximate, charge calculation method. On the basis of the initial screening, 15 MOFs were selected, and Monte Carlo simulations were carried out to compute the adsorption isotherms for these MOFs using more accurate framework charges calculated by density functional theory. A detailed investigation was performed on the effect of using different methods for calculating partial charges, and it was found that electrostatic interactions contribute the majority of the adsorption energy of H2O in the selected MOFs.

  17. Integrated CO2 capture-fixation chemistry via interfacial ionic liquid catalyst in laminar gas/liquid flow

    NASA Astrophysics Data System (ADS)

    Vishwakarma, Niraj K.; Singh, Ajay K.; Hwang, Yoon-Ho; Ko, Dong-Hyeon; Kim, Jin-Oh; Babu, A. Giridhar; Kim, Dong-Pyo

    2017-03-01

    Simultaneous capture of carbon dioxide (CO2) and its utilization with subsequent work-up would significantly enhance the competitiveness of CO2-based sustainable chemistry over petroleum-based chemistry. Here we report an interfacial catalytic reaction platform for an integrated autonomous process of simultaneously capturing/fixing CO2 in gas-liquid laminar flow with subsequently providing a work-up step. The continuous-flow microreactor has built-in silicon nanowires (SiNWs) with immobilized ionic liquid catalysts on tips of cone-shaped nanowire bundles. Because of the superamphiphobic SiNWs, a stable gas-liquid interface maintains between liquid flow of organoamines in upper part and gas flow of CO2 in bottom part of channel. The intimate and direct contact of the binary reagents leads to enhanced mass transfer and facilitating reactions. The autonomous integrated platform produces and isolates 2-oxazolidinones and quinazolines-2,4(1H,3H)-diones with 81-97% yields under mild conditions. The platform would enable direct CO2 utilization to produce high-valued specialty chemicals from flue gases without pre-separation and work-up steps.

  18. Plant-wide dynamic simulation of an IGCC plant with CO2 capture

    SciTech Connect

    Bhattacharyya, D.; Turton, R.; Zitney, S.

    2009-01-01

    To eliminate the harmful effects of greenhouse gases, especially that of CO2, future coalfired power plants need to consider the option for CO2 capture. The loss in efficiency for CO2 capture is less in an Integrated Gasification Combined Cycle (IGCC) plant compared to other conventional coal combustion processes. However, no IGCC plant with CO2 capture currently exists in the world. Therefore, it is important to consider the operability and controllability issues of such a plant before it is commercially built. With this objective in mind, a detailed plant-wide dynamic simulation of an IGCC plant with CO2 capture has been developed. The plant considers a General Electric Energy (GEE)-type downflow radiant-only gasifier followed by a quench section. A two-stage water gas shift (WGS) reaction is considered for conversion of about 96 mol% of CO to CO2. A two-stage acid gas removal (AGR) process based on a physical solvent is simulated for selective capture of H2S and CO2. The clean syngas is sent to a gas turbine (GT) followed by a heat recovery steam generator (HRSG). The steady state results are validated with data from a commercial gasifier. A 5 % ramp increase in the flowrate of coal is introduced to study the system dynamics. To control the conversion of CO at a desired level in the WGS reactors, the steam/CO ratio is manipulated. This strategy is found to be efficient for this operating condition. In the absence of an efficient control strategy in the AGR process, the environmental emissions exceeded the limits by a great extent.

  19. Limitations and high pressure behavior of MOF-5 for CO2 capture.

    PubMed

    Jung, Joo Young; Karadas, Ferdi; Zulfiqar, Sonia; Deniz, Erhan; Aparicio, Santiago; Atilhan, Mert; Yavuz, Cafer T; Han, Seung Min

    2013-09-14

    Porous network structures (e.g. metal-organic frameworks, MOFs) show considerable potential in dethroning monoethanol amine (MEA) from being the dominant scrubber for CO2 at the fossil-fuel-burning power generators. In contrast to their promise, structural stability and high-pressure behavior of MOFs are not well documented. We herein report moisture stability, mechanical properties and high-pressure compression on a model MOF structure, MOF-5. Our results show that MOF-5 can endure all tested pressures (0-225 bar) without losing its structural integrity, however, its moist air stability points at a 3.5 hour safety window (at 21.6 °C and 49% humidity) for an efficient CO2 capture. Isosteric heats of CO2 adsorption at high pressures show moderate interaction energy between CO2 molecules and the MOF-5 sorbent, which combined with the large sorption ability of MOF-5 in the studied pressure-temperature ranges show the viability of this sorbent for CO2 capturing purposes. The combination of the physicochemical methods we used suggests a generalized analytical standard for measuring viability in CO2 capture operations.

  20. Mechanisms of low temperature capture and regeneration of CO2 using diamino protic ionic liquids.

    PubMed

    Simons, Tristan J; Verheyen, Thomas; Izgorodina, Ekaterina I; Vijayaraghavan, R; Young, Scott; Pearson, Andrew K; Pas, Steven J; MacFarlane, Douglas R

    2016-01-14

    Carbon dioxide (CO2) chemical absorption and regeneration was investigated in two diamino carboxylate protic ionic liquids (PILs), dimethylethylenediamine formate (DMEDAH formate) and dimethylpropylenediamine acetate (DMPDAH acetate), using novel calorimetric techniques. The PILs under study have previously been shown to possess a CO2 absorption capacity similar to the industrial standard, 30% aqueous MEA, while requiring much lower temperatures to release the captured CO2. We show that this is in part due to the fact that the PILs exhibit enthalpies of CO2 desorption as low as 40 kJ mol(-1), significantly lower than the 85 kJ mol(-1) required for 30% aqueous MEA. Computational and spectroscopic analyses were used to probe the mechanism of CO2 capture, which was found to proceed via the formation of carbamate moieties on the primary amine of both DMEDAH and DMPDAH. Evidence was also found that weakly acidic counter-ions such as formate and acetate provide, unexpectedly, an additional proton acceptor site in the traditional carbamate mechanism, revealing opportunities to increase CO2 uptake capacity in the future through careful design of the anion and cation used in the PIL capture agent.

  1. Carbonic anhydrase-facilitated CO2 absorption with polyacrylamide buffering bead capture

    SciTech Connect

    Dilmore, Robert; Griffith, Craid; Liu, Zhu; Soong, Yee; Hedges, Sheila W.; Koepsel, Richard; Ataai, M

    2009-07-01

    A novel CO2 separation concept is described wherein the enzyme carbonic anhydrase (CA) is used to increase the overall rate Of CO2 absorption after which hydrated CO2 reacts with regenerable amine-bearing polyacrylamide buffering beads (PABB). Following saturation of the material's immobilized tertiary amines, CA-bearing carrier water is separated and recycled to the absorption stage while CO2-loaded material is thermally regenerated. Process application of this concept would involve operation of two or more columns in parallel with thermal regeneration with low-pressure steam taking place after the capacity of a column of amine-bearing polymeric material was exceeded. PABB CO2- bearing capacity was evaluated by thermogravimetric analysis (TGA) for beads of three acrylamido buffering monomer ingredient concentrations: 0 mol/kg bead, 0.857 mol/kg bead, and 2 mol/kg bead. TGA results demonstrate that CO2- bearing capacity increases with increasing PABB buffering concentration and that up to 78% of the theoretical CO2- bearing capacity was realized in prepared PABB samples (0.857 mol/kg recipe). The highest observed CO2-bearing capacity of PABB was 1.37 mol of CO2 per kg dry bead. TGA was also used to assess the regenerability Of CO2-loaded PABB. Preliminary results suggest that CO2 is partially driven from PABB samples at temperatures as low as 55 degrees C, with complete regeneration occurring at 100 degrees C. Other physical characteristics of PABB are discussed. In addition, the effectiveness of bovine carbonic anhydrase for the catalysis Of CO2 dissolution is evaluated. Potential benefits and drawbacks of the proposed process are discussed. Published by Elsevier Ltd.

  2. Progress in Adsorption-Based CO2 Capture by Metal-Organic Frameworks

    SciTech Connect

    Liu, Jian; Thallapally, Praveen K.; McGrail, B. Peter; Brown, Daryl R.; Liu, Jun

    2012-01-01

    Metal-organic frameworks (MOFs) have recently attracted intense research interest because of their permanent porous structures, large surface areas, and potential applications as novel adsorbents. The recent progress in adsorption-based CO2 capture by MOFs is reviewed and summarized in this paper. CO2 adsorption in MOFs has been divided into two sections, adsorption at high pressures and selective adsorption at approximate atmospheric pressures. Keys to CO2 adsorption in MOFs at high pressures and low pressures are summarized to be pore volumes of MOFs, and heats of adsorption, respectively. Many MOFs have high CO2 selectivities over N2 and CH4. Water effects on CO2 adsorption in MOFs are presented and compared with benchmark zeolites. In addition, strategies appeared in the literature to enhance CO2 adsorption capacities and/or selectivities in MOFs have been summarized into three main categories, catenation and interpenetration, chemical bonding enhancement, and electrostatic force involvement. Besides the advantages, two main challenges for using MOFs in CO2 capture, the cost of synthesis and the stability toward water vapor, have been analyzed and possible solutions and path-forward have been proposed to address the two challenges as well.

  3. Anion-activated, thermoreversible gelation system for the capture, release, and visual monitoring of CO2

    NASA Astrophysics Data System (ADS)

    Zhang, Xin; Lee, Songyi; Liu, Yifan; Lee, Minji; Yin, Jun; Sessler, Jonathan L.; Yoon, Juyoung

    2014-04-01

    Carbon dioxide (CO2) is an important green house gas. This is providing an incentive to develop new strategies to detect and capture CO2. Achieving both functions within a single molecular system represents an unmet challenge in terms of molecular design and could translate into enhanced ease of use. Here, we report an anion-activated chemosensor system, NAP-chol 1, that permits dissolved CO2 to be detected in organic media via simple color changes or through ratiometric differences in fluorescence intensity. NAP-chol 1 also acts as a super gelator for DMSO. The resulting gel is transformed into a homogeneous solution upon exposure to fluoride anions. Bubbling with CO2 regenerates the gel. Subsequent flushing with N2 or heating serves to release the CO2 and reform the sol form. This series of transformations is reversible and can be followed by easy-to-discern color changes. Thus, NAP-chol 1 allows for the capture and release of CO2 gas while acting as a three mode sensing system. In particular, it permits CO2 to be detected through reversible sol-gel transitions, simple changes in color, or ratiometric monitoring of the differences in the fluorescence features.

  4. Anion-activated, thermoreversible gelation system for the capture, release, and visual monitoring of CO2

    PubMed Central

    Zhang, Xin; Lee, Songyi; Liu, Yifan; Lee, Minji; Yin, Jun; Sessler, Jonathan L.; Yoon, Juyoung

    2014-01-01

    Carbon dioxide (CO2) is an important green house gas. This is providing an incentive to develop new strategies to detect and capture CO2. Achieving both functions within a single molecular system represents an unmet challenge in terms of molecular design and could translate into enhanced ease of use. Here, we report an anion-activated chemosensor system, NAP-chol 1, that permits dissolved CO2 to be detected in organic media via simple color changes or through ratiometric differences in fluorescence intensity. NAP-chol 1 also acts as a super gelator for DMSO. The resulting gel is transformed into a homogeneous solution upon exposure to fluoride anions. Bubbling with CO2 regenerates the gel. Subsequent flushing with N2 or heating serves to release the CO2 and reform the sol form. This series of transformations is reversible and can be followed by easy-to-discern color changes. Thus, NAP-chol 1 allows for the capture and release of CO2 gas while acting as a three mode sensing system. In particular, it permits CO2 to be detected through reversible sol-gel transitions, simple changes in color, or ratiometric monitoring of the differences in the fluorescence features. PMID:24699626

  5. Ordered mesoporous silica (OMS) as an adsorbent and membrane for separation of carbon dioxide (CO2).

    PubMed

    Chew, Thiam-Leng; Ahmad, Abdul L; Bhatia, Subhash

    2010-01-15

    Separation of carbon dioxide (CO(2)) from gaseous mixture is an important issue for the removal of CO(2) in natural gas processing and power plants. The ordered mesoporous silicas (OMS) with uniform pore structure and high density of silanol groups, have attracted the interest of researchers for separation of carbon dioxide (CO(2)) using adsorption process. These mesoporous silicas after functionalization with amino groups have been studied for the removal of CO(2). The potential of functionalized ordered mesoporous silica membrane for separation of CO(2) is also recognized. The present paper reviews the synthesis of mesoporous silicas and important issues related to the development of mesoporous silicas. Recent studies on the CO(2) separation using ordered mesoporous silicas (OMS) as adsorbent and membrane are highlighted. The future prospectives of mesoporous silica membrane for CO(2) adsorption and separation are also presented and discussed.

  6. Layered Graphene-Hexagonal BN Nanocomposites: Experimentally Feasible Approach to Charge-Induced Switchable CO2 Capture.

    PubMed

    Tan, Xin; Kou, Liangzhi; Smith, Sean C

    2015-09-07

    Recently, inducing negative charge density on hexagonal boron nitride (h-BN) has been predicted as an effective strategy for controllable, selective, and reversible CO2 capture. However, h-BN is a wide-gap semiconductor and it is not clear how to effectively induce the requisite negative charge density. In this paper, we employ first-principle calculations to propose hybrid h-BN-graphene (hybrid BN/G) nanosheets as an experimentally feasible strategy to induce charge on h-BN for charge-controlled CO2 capture. The results indicate that the charge density is effectively transferred from the graphene layer with high electronic mobility into the h-BN layer on the surface, regardless of the thickness of BN layers, such that CO2 capture/release can be simply controlled by switching on/off the charge states of hybrid BN/G system. In addition, these negatively charged hybrid BN/G are highly selective for separating CO2 from mixtures with CH4 , N2 , and/or H2 .

  7. Effects of flue gas compositions on nitrosamine and nitramine formation in postcombustion CO2 capture systems.

    PubMed

    Dai, Ning; Mitch, William A

    2014-07-01

    Amine-based technologies are emerging as the prime contender for postcombustion CO2 capture. However, concerns have arisen over the health impacts of amine-based CO2 capture associated with the release of nitrosamines and nitramines, which are byproducts from the reactions between flue gas NOx and solvent amines. In this study, flue gas compositions were systematically varied to evaluate their effects on the formation of nitrosamines and nitramines in a lab-scale CO2 capture reactor with morpholine as a model solvent amine. The accumulation of N-nitrosomorpholine in both the absorber and washwater increased linearly with both NO and NO2 for concentrations up to ∼20 ppmv. These correlations could be extrapolated to estimate N-nitrosomorpholine accumulation at extremely low NOx levels (0.3 ppmv NO2 and 1.5 ppmv NO). NO played a particularly important role in driving N-nitrosomorpholine formation in the washwater, likely following partial oxidation to NO2 by O2. The accumulation of N-nitromorpholine in both the absorber and washwater positively correlated with flue gas NO2 concentration, but not with NO concentration. Both N-nitrosomorpholine and N-nitromorpholine accumulated fastest in the absence of CO2. Flue gas humidity did not affect nitrosamine accumulation in either the absorber or the washwater unit. These results provide a basis for estimating the effects of flue gas composition on nitrosamine and nitramine accumulation in postcombustion CO2 capture systems.

  8. Human health risk assessment of nitrosamines and nitramines for potential application in CO2 capture.

    PubMed

    Ravnum, S; Rundén-Pran, E; Fjellsbø, L M; Dusinska, M

    2014-07-01

    Emission and accumulation of carbon dioxide (CO2) in the atmosphere exert an environmental and climate change challenge. An attempt to deal with this challenge is made at Mongstad by application of amines for CO2 capture and storage (CO2 capture Mongstad (CCM) project). As part of the CO2 capture process, nitrosamines and nitramines may be emitted. Toxicological testing of nitrosamines and nitramines indicate a genotoxic potential of these substances. Here we present a risk characterization and assessment for five nitrosamines (N-Nitrosodi-methylamine (NDMA) N-Nitrosodi-ethylamine (NDEA), N-Nitroso-morpholine (NNM), N-Nitroso-piperidine (NPIP), and Dinitroso-piperazine (DNP)) and two nitramines (N-Methyl-nitramine (NTMA), Dimethyl-nitramine (NDTMA)), which are potentially emitted from the CO2 capture plant (CCP). Human health risk assessment of genotoxic non-threshold substances is a heavily debated topic, and no consensus methodology exists internationally. Extrapolation modeling from high-dose animal exposures to low-dose human exposures can be crucial for the final risk calculation. In the work presented here, different extrapolation models are discussed, and suggestions on applications are given. Then, preferred methods for calculating derived minimal effect level (DMEL) are presented with the selected nitrosamines and nitramines.

  9. Alkyl amine and vegetable oil mixture-a viable candidate for CO2 capture and utilization.

    PubMed

    Uma Maheswari, A; Palanivelu, K

    2017-02-01

    In this present work, the absorption of CO2 in alkyl amines and vegetable oil mixture has been evaluated. The results showed that the absorption is higher in alkyl amines and vegetable oil mixture compared with the aqueous alkyl amines. In addition to that, by employing the greener and non-toxic vegetable oil media, the CO2 gas has been captured as well as converted into value-added products, such as carbamates of ethylenediamine, diethylenetriamine, and triethylenetetramine. The carbamates have been isolated and characterized by Fourier transform infrared and (1)H and (13)C nuclear magnetic resonance spectroscopic techniques. The formation of these products in precipitate form has not been observed in the case of aqueous medium. Among the various alkyl amine and vegetable oil combinations, triethylenetetramine in coconut oil medium showed the maximum CO2 capture capacity of 72%. The coconut oil used for the process has been recovered, recycled, and reused for 3 cycles. Thus, this novel scheme seems to be a better alternative to conquer the drawback of aqueous amine-based CO2 capture as well as for the capture and utilization of the CO2 gas to gain the value-added products.

  10. Fragmentation dynamics of CO(2)(3+) investigated by multiple electron capture in collisions with slow highly charged ions.

    PubMed

    Neumann, N; Hant, D; Schmidt, L Ph H; Titze, J; Jahnke, T; Czasch, A; Schöffler, M S; Kreidi, K; Jagutzki, O; Schmidt-Böcking, H; Dörner, R

    2010-03-12

    Fragmentation of highly charged molecular ions or clusters consisting of more than two atoms can proceed in a one step synchronous manner where all bonds break simultaneously or sequentially by emitting one ion after the other. We separated these decay channels for the fragmentation of CO(2)(3+) ions by measuring the momenta of the ionic fragments. We show that the total energy deposited in the molecular ion is a control parameter which switches between three distinct fragmentation pathways: the sequential fragmentation in which the emission of an O(+) ion leaves a rotating CO(2+) ion behind that fragments after a time delay, the Coulomb explosion and an in-between fragmentation--the asynchronous dissociation. These mechanisms are directly distinguishable in Dalitz plots and Newton diagrams of the fragment momenta. The CO(2)(3+) ions are produced by multiple electron capture in collisions with 3.2 keV/u Ar(8+) ions.

  11. Imidazole tailored deep eutectic solvents for CO2 capture enhanced by hydrogen bonds.

    PubMed

    Cao, Lingdi; Huang, Junhua; Zhang, Xiangping; Zhang, Suojiang; Gao, Jubao; Zeng, Shaojuan

    2015-11-07

    Deep eutectic solvents (DESs) have emerged as promising alternative candidates for CO2 capture in recent years. In this work, several novel DESs were firstly prepared to enhance CO2 absorption. Structural and physical properties of DESs were investigated, as well as their absorption performance of CO2. A distinct depression in the melting point up to 80 K of DESs was observed compared with that of BMIMCl. The observed red shifts of the C2H group in an imidazolium ring and its chemical shifts downfield in NMR spectra are indicative of a hydrogen bond interaction between BMIMCl and MEA. In particular, CO2 uptake in MEA : ILs (4 : 1) at room temperature and atmospheric pressure is up to 21.4 wt%, which is higher than that of 30 wt% MEA (13%). A hydrogen bond related mechanism was proposed in which ILs act as a medium to improve CO2 uptake through hydrogen bonds. Finally, the firstly reported overall heat of CO2 absorption is slightly higher than that of 30 wt% MEA, implying that the hydrogen bonds of DESs contribute to the overall heat of CO2 absorption. This study reveals that the heat of CO2 absorption can be tailored by the proper molar ratio of MEA and ILs.

  12. High-performance multilayer composite membranes with mussel-inspired polydopamine as a versatile molecular bridge for CO2 separation.

    PubMed

    Li, Panyuan; Wang, Zhi; Li, Wen; Liu, Yanni; Wang, Jixiao; Wang, Shichang

    2015-07-22

    It is desirable to develop high-performance composite membranes for efficient CO2 separation in CO2 capture process. Introduction of a highly permeable polydimethylsiloxane (PDMS) intermediate layer between a selective layer and a porous support has been considered as a simple but efficient way to enhance gas permeance while maintaining high gas selectivity, because the introduced intermediate layer could benefit the formation of an ultrathin defect-free selective layer owing to the circumvention of pore penetration phenomenon. However, the selection of selective layer materials is unfavorably restricted because of the low surface energy of PDMS. Various highly hydrophilic membrane materials such as amino group-rich polyvinylamine (PVAm), a representative facilitated transport membrane material for CO2 separation, could not be facilely coated over the surface of the hydrophobic PDMS intermediate layer uniformly. Inspired by the hydrophilic nature and strong adhesive ability of polydopamine (PDA), PDA was therefore selected as a versatile molecular bridge between hydrophobic PDMS and hydrophilic PVAm. The PDA coating endows a highly compatible interface between both components with a large surface energy difference via multiple-site cooperative interactions. The resulting multilayer composite membrane with a thin facilitated transport PVAm selective layer exhibits a notably enhanced CO2 permeance (1887 GPU) combined with a slightly improved CO2/N2 selectivity (83), as well as superior structural stability. Similarly, the multilayer composite membrane with a hydrophilic CO2-philic Pebax 1657 selective layer was also developed for enhanced CO2 separation performance.

  13. CO2 capture in amine solutions from ab initio molecular dynamics

    NASA Astrophysics Data System (ADS)

    Ma, Changru; Pietrucci, Fabio; Andreoni, Wanda

    2014-03-01

    The most mature technology for post-combustion CO2 capture exploits a cyclic process, in which CO2 is selectively and reversibly absorbed in an amine solution, typically monoethanolamine(MEA) at 30%wt concentration. Empirical efforts are ongoing worldwide to reduce the high energy penalty for amine regeneration and to increase the absorption rate. Computer simulations can help by providing new insights and the missing quantitative information. Using extensive large-scale Car-Parrinello molecular dynamics simulations, aided by accelerated sampling techniques, we have characterized the reactions leading to CO2 capture in MEA 30%wt solutions via the formation of the carbamate, and the subsequent CO2 release. Deprotonation and CO2 release turn out to be competitive for an intermediate zwitterion (free-energy barrier ~10kcal/mol), with sizable entropic contribution, whereas CO2 release from the carbamate has a much higher barrier (~50kcal/mol), mainly enthalpic and rather independent of temperature. An unprecedented characterization of structural and vibrational properties of the solution allows us to interpret recent experimental results. More results on other amines, allow us to rationalize their still unexplained better performance relative to MEA. We acknowledge PRACE for awarding us access to resource Juqueen based in Germany at Juelich.

  14. Parametric analysis of a novel cryogenic CO2 capture system based on Stirling coolers.

    PubMed

    Song, Chun Feng; Kitamura, Yutaka; Li, Shu Hong; Jiang, Wei Zhong

    2012-11-20

    CO(2) capture and storage (CCS) is an important alternative to control greenhouse gas (GHG) effects. In previous work, a novel desublimation CO(2) capture process has been exploited making use of three free piston Stirling coolers (namely, SC-1, SC-2, and SC-3, respectively). Based on the developed system, moisture and CO(2) in the flue gas can condense and desublimate in the prefreezing and main-freezing towers, respectively. Meanwhile, the storage column is chilled by SC-3 to preserve the frosted CO(2), and permanent gas (such as N(2)) passes through the system without phase change. The whole process can be implemented at atmospheric pressure and reduce the energy penalty (e.g., solvent regeneration and pressure drop) in other technologies. In this work, the influence of process parameters has been investigated in detail. The optimal conditions for the system are as follows: idle operating time is 240 min, flow rate is 5 L/min, vacuum degree of the interlayer is 2.2 × 10(3) Pa, and temperatures of SC-1, -2, and -3 are -30, -120, and -120 °C, respectively. Under these conditions, the energy consumption of the system is around 0.5 MJ(electrical)/kg CO(2) with above 90% CO(2) recovery.

  15. Amine-Impregnated Mesoporous Silica Nanotube as an Emerging Nanocomposite for CO2 Capture.

    PubMed

    Niu, Mengya; Yang, Huaming; Zhang, Xiangchao; Wang, Yutang; Tang, Aidong

    2016-07-13

    Pristine halloysite nanotubes (HNTs) were pretreated to produce mesoporous silica nanotubes (MSiNTs), which was further impregnated with polyethenimine (PEI) to prepare an emerging nanocomposite MSiNTs/PEI (MP) for CO2 capture. Thermogravimetric analysis (TGA) was employed to analyze the influences of PEI loading amount and adsorption temperature on CO2 adsorption capacity of the nanocomposite. The Brunauer-Emmett-Teller (BET) surface area (SBET) of MSiNTs was six times higher than that of HNTs, and the corresponding pore volume was more than two times higher than that of HNTs. The well dispersion of PEI within the nanotubes of MSiNTs benefits more CO2 gas adsorption, and the adsorption capacity of the nanocomposite could reach 2.75 mmol/g at 85 °C for 2 h. The CO2 adsorption on the nanocomposite was demonstrated to occur via a two-stage process: initially, a sharp linear weight increase at the beginning, and then a relatively slow adsorption step. The adsorption capacity could reach as high as 70% within 2 min. Also, the nanocomposite exhibited good stability on CO2 adsorption/desorption performance, indicating that the as-prepared emerging nanocomposite show an interesting application potential in the field of CO2 capture.

  16. Preparation and characterization of amine-functionalized sugarcane bagasse for CO2 capture.

    PubMed

    Luo, Shihe; Chen, Siyu; Chen, Shuixia; Zhuang, Linzhou; Ma, Nianfang; Xu, Teng; Li, Qihan; Hou, Xunan

    2016-03-01

    A low-cost solid amine adsorbent for CO2 capture was prepared by using sugarcane bagasse (SB), a dominant agro-industrial residue in the sugar and alcohol industry as raw materials. In this preparation process, acrylamide was grafted on SB, and the grafted fiber was then aminated with different type of amine reagents to introduce primary and secondary amine groups onto the surface of SB fibers. The graft and amination conditions were optimized. The prepared solid amine adsorbent showed remarkable CO2 adsorption capacity and the adsorption capacity of the solid amine adsorbent could reach 5.01 mmol CO2/g at room temperature. The comparison of adsorption capacities of amine fibers aminated with various amination agents demonstrated that fibers aminated with triethylenetetramine would obtain higher adsorption capacities and higher amine efficiency. These adsorbents also showed good regeneration performance, the regenerated adsorbent could maintain almost the same adsorption capacity for CO2 after 10 recycles.

  17. Efficient Theoretical Screening of Solid Sorbents for CO2 Capture Applications*

    SciTech Connect

    Duan, Yuhua; Luebke, David; Pennline, Henry

    2012-03-31

    By combining thermodynamic database mining with first principles density functional theory and phonon lattice dynamics calculations, a theoretical screening methodology to identify the most promising CO2 sorbent candidates from the vast array of possible solid materials has been proposed and validated. The ab initio thermodynamic technique has the advantage of allowing identification of thermodynamic properties of CO2 capture reactions without any experimental input beyond crystallographic structural information of the solid phases involved. For a given solid, the first step is to attempt to extract thermodynamic properties from thermodynamic databases and the available literatures. If the thermodynamic properties of the compound of interest are unknown, an ab initio thermodynamic approach is used to calculate them. These properties expressed conveniently as chemical potentials and heat of reactions, which obtained either from databases or from calculations, are further used for computing the thermodynamic reaction equilibrium properties of the CO2 absorption/desorption cycles. Only those solid materials for which lower capture energy costs are predicted at the desired process conditions are selected as CO2 sorbent candidates and are further considered for experimental validations. Solid sorbents containing alkali and alkaline earth metals have been reported in several previous studies to be good candidates for CO2 sorbent applications due to their high CO2 absorption capacity at moderate working temperatures. In addition to introducing our computational screening procedure, in this presentation we will summarize our results for solid systems composed by alkali and alkaline earth metal oxides, hydroxides, and carbon- ates/bicarbonates to validate our methodology. Additionally, applications of our computational method to mixed solid systems of Li2O with SiO2/ZrO2 with different mixing ratios, our preliminary results showed that increasing the Li2O/SiO2 ratio in

  18. Composite Membranes for CO2 Capture: High Performance Metal Organic Frameworks/Polymer Composite Membranes for Carbon Dioxide Capture

    SciTech Connect

    2010-07-01

    IMPACCT Project: A team of six faculty members at Georgia Tech are developing an enhanced membrane by fitting metal organic frameworks, compounds that show great promise for improved carbon capture, into hollow fiber membranes. This new material would be highly efficient at removing CO2 from the flue gas produced at coal-fired power plants. The team is analyzing thousands of metal organic frameworks to identify those that are most suitable for carbon capture based both on their ability to allow coal exhaust to pass easily through them and their ability to select CO2 from that exhaust for capture and storage. The most suitable frameworks would be inserted into the walls of the hollow fiber membranes, making the technology readily scalable due to their high surface area. This composite membrane would be highly stable, withstanding the harsh gas environment found in coal exhaust.

  19. High-performance Polymer Membranes with Multi-functional Amphiphilic Micelles for CO2 Capture.

    PubMed

    Kim, Sang Jin; Jeon, Harim; Kim, Dong Jun; Kim, Jong Hak

    2015-11-09

    Invited for this month's cover is the group of Jong Hak Kim at Yonsei University in South Korea. The image shows how CO2 selectively permeates through the polymer membrane containing multi-functional amphiphilic poly(dimethylsiloxane)-g-poly(oxyethylene methacrylate) (PDMS-g-POEM) comb copolymer micelles. The microphase-separated structure consists of PDMS cores and CO2 -philic POEM corona. The Full Paper itself is available at 10.1002/cssc.201501063.

  20. Effect of fossil fuels on the parameters of CO2 capture.

    PubMed

    Nagy, Tibor; Mizsey, Peter

    2013-08-06

    The carbon dioxide capture is a more and more important issue in the design and operation of boilers and/or power stations because of increasing environmental considerations. Such processes, absorber desorber should be able to cope with flue gases from the use of different fossil primary energy sources, in order to guarantee a flexible, stable, and secure energy supply operation. The changing flue gases have significant influence on the optimal operation of the capture process, that is, where the required heating of the desorber is the minimal. Therefore special considerations are devoted to the proper design and control of such boiler and/or power stations equipped with CO2 capture process.

  1. CO2 post-combustion capture in coal-fired power plants integrated with solar systems

    NASA Astrophysics Data System (ADS)

    Carapellucci, R.; Giordano, L.; Vaccarelli, M.

    2015-11-01

    The majority of the World's primary energy consumption is still based on fossil fuels, representing the largest source of global CO2 emissions. According to the Intergovernmental Panel on Climate Change (IPCC), such emissions must be significantly reduced in order to avoid the dramatic consequences of global warming. A potential way to achieve this ambitious goal is represented by the implementation of CCS (Carbon Capture and Storage) technologies. However, the significant amount of energy required by the CCS systems still represents one the major barriers for their deployment. Focusing on post-combustion capture based on amine absorption, several interesting options have been investigated to compensate the energy losses due to solvent regeneration, also using renewable energy sources. One of the most promising is based on the use of concentrating solar power (CSP), providing a part of the energy requirement of the capture island. In this study the integration of a CSP system into a coal-fired power plant with CO2 postcombustion capture is investigated. Basically, a CSP system is used to support the heat requirement for amine regeneration, by producing saturated steam at low temperature. This allows to reduce or even eliminate the conventional steam extraction from the main power plant, affecting positively net power production and efficiency. The energy analysis of the whole system is carried out using the GateCycle software to simulate the coal-fired power plant and ChemCad platform for the CO2 capture process based on amine absorption.

  2. Postcombustion Capture of CO2 with CaO in a Circulating Fluidized Bed Carbonator

    NASA Astrophysics Data System (ADS)

    Alonso, M.; Rodriguez, N.; González, B.; Grasa, G.; Murillo, R.; Abanades, J. C.

    There is an emerging postcombustion capture technology that uses CaO to capture CO2 from combustion flue gases in a circulating fluidized bed reactor. This paper summarizes recent work conducted at CSIC to understand and develop this technology. The paper includes experimental results at conditions close to those expected in the real system, carried out in continuous mode in a 30kW test facility made up of two interconnected circulating fluidized bed reactors. In one of the reactors, CO2 is captured from the gas phase by the CaO continuously circulating from a calciner. In the second reactor, the CaCO3 formed in the carbonator is regenerated to CaO and CO2 by calcination. Modeling of the system at process level, at reactor level (in particular the CFB carbonator), and at particle level (decay in capture capability of CaO) is also outlined. The work carried out so far confirms that the carbonator reactors can be designed to attain capture efficiencies between 70-90%, operating at fluid dynamic conditions close to those present in circulating fluidized bed combustors.

  3. Transient studies of an Integrated Gasification Combined Cycle (IGCC) plant with CO2 capture

    SciTech Connect

    Bhattacharyya, D.; Turton, R.; Zitney, S.

    2010-01-01

    Next-generation coal-fired power plants need to consider the option for CO2 capture as stringent governmental mandates are expected to be issued in near future. Integrated gasification combined cycle (IGCC) plants are more efficient than the conventional coal combustion processes when the option for CO2 capture is considered. However, no IGCC plant with CO2 capture currently exists in the world. Therefore, it is important to consider the operability and controllability issues of such a plant before it is commercially built. To facilitate this objective, a detailed plant-wide dynamic simulation of an IGCC plant with 90% CO2 capture has been developed in Aspen Plus Dynamics{reg_sign}. The plant considers a General Electric Energy (GEE)-type downflow radiant-only gasifier followed by a quench section. A two-stage water gas shift (WGS) reaction is considered for conversion of CO to CO2. A two-stage acid gas removal (AGR) process based on a physical solvent is simulated for selective capture of H2S and CO2. Compression of the captured CO2 for sequestration, an oxy-Claus process for removal of H2S and NH3, black water treatment, and the sour water treatment are also modeled. The tail gas from the Claus unit is recycled to the SELEXOL unit. The clean syngas from the AGR process is sent to a gas turbine followed by a heat recovery steam generator. This turbine is modeled as per published data in the literature. Diluent N2 is used from the elevated-pressure ASU for reducing the NOx formation. The heat recovery steam generator (HRSG) is modeled by considering generation of high-pressure, intermediate-pressure, and low-pressure steam. All of the vessels, reactors, heat exchangers, and the columns have been sized. The basic IGCC process control structure has been synthesized by standard guidelines and existing practices. The steady state results are validated with data from a commercial gasifier. In the future grid-connected system, the plant should satisfy the environmental

  4. CO2 capture from simulated fuel gas mixtures using semiclathrate hydrates formed by quaternary ammonium salts.

    PubMed

    Park, Sungwon; Lee, Seungmin; Lee, Youngjun; Seo, Yongwon

    2013-07-02

    In order to investigate the feasibility of semiclathrate hydrate-based precombustion CO2 capture, thermodynamic, kinetic, and spectroscopic studies were undertaken on the semiclathrate hydrates formed from a fuel gas mixture of H2 (60%) + CO2 (40%) in the presence of quaternary ammonium salts (QASs) such as tetra-n-butylammonium bromide (TBAB) and fluoride (TBAF). The inclusion of QASs demonstrated significantly stabilized hydrate dissociation conditions. This effect was greater for TBAF than TBAB. However, due to the presence of dodecahedral cages that are partially filled with water molecules, TBAF showed a relatively lower gas uptake than TBAB. From the stability condition measurements and compositional analyses, it was found that with only one step of semiclathrate hydrate formation with the fuel gas mixture from the IGCC plants, 95% CO2 can be enriched in the semiclathrate hydrate phase at room temperature. The enclathration of both CO2 and H2 in the cages of the QAS semiclathrate hydrates and the structural transition that results from the inclusion of QASs were confirmed through Raman and (1)H NMR measurements. The experimental results obtained in this study provide the physicochemical background required for understanding selective partitioning and distributions of guest gases in the QAS semiclathrate hydrates and for investigating the feasibility of a semiclathrate hydrate-based precombustion CO2 capture process.

  5. High temperature CO2 capture using calcium oxide sorbent in a fixed-bed reactor.

    PubMed

    Dou, Binlin; Song, Yongchen; Liu, Yingguang; Feng, Cong

    2010-11-15

    The gas-solid reaction and breakthrough curve of CO(2) capture using calcium oxide sorbent at high temperature in a fixed-bed reactor are of great importance, and being influenced by a number of factors makes the characterization and prediction of these a difficult problem. In this study, the operating parameters on reaction between solid sorbent and CO(2) gas at high temperature were investigated. The results of the breakthrough curves showed that calcium oxide sorbent in the fixed-bed reactor was capable of reducing the CO(2) level to near zero level with the steam of 10 vol%, and the sorbent in CaO mixed with MgO of 40 wt% had extremely low capacity for CO(2) capture at 550°C. Calcium oxide sorbent after reaction can be easily regenerated at 900°C by pure N(2) flow. The experimental data were analyzed by shrinking core model, and the results showed reaction rates of both fresh and regeneration sorbents with CO(2) were controlled by a combination of the surface chemical reaction and diffusion of product layer.

  6. Molecular template-directed synthesis of microporous polymer networks for highly selective CO2 capture.

    PubMed

    Shi, Yao-Qi; Zhu, Jing; Liu, Xiao-Qin; Geng, Jian-Cheng; Sun, Lin-Bing

    2014-11-26

    Porous polymer networks have great potential in various applications including carbon capture. However, complex monomers and/or expensive catalysts are commonly used for their synthesis, which makes the process complicated, costly, and hard to scale up. Herein, we develop a molecular template strategy to fabricate new porous polymer networks by a simple nucleophilic substitution reaction of two low-cost monomers (i.e., chloromethylbenzene and ethylene diamine). The polymerization reactions can take place under mild conditions in the absence of any catalysts. The resultant materials are interconnected with secondary amines and show well-defined micropores due to the structure-directing role of solvent molecules. These properties make our materials highly efficient for selective CO2 capture, and unusually high CO2/N2 and CO2/CH4 selectivities are obtained. Furthermore, the adsorbents can be completely regenerated under mild conditions. Our materials may provide promising candidates for selective capture of CO2 from mixtures such as flue gas and natural gas.

  7. Predicting the ultimate potential of natural gas SOFC power cycles with CO2 capture - Part A: Methodology and reference cases

    NASA Astrophysics Data System (ADS)

    Campanari, Stefano; Mastropasqua, Luca; Gazzani, Matteo; Chiesa, Paolo; Romano, Matteo C.

    2016-08-01

    Driven by the search for the highest theoretical efficiency, in the latest years several studies investigated the integration of high temperature fuel cells in natural gas fired power plants, where fuel cells are integrated with simple or modified Brayton cycles and/or with additional bottoming cycles, and CO2 can be separated via chemical or physical separation, oxy-combustion and cryogenic methods. Focusing on Solid Oxide Fuel Cells (SOFC) and following a comprehensive review and analysis of possible plant configurations, this work investigates their theoretical potential efficiency and proposes two ultra-high efficiency plant configurations based on advanced intermediate-temperature SOFCs integrated with a steam turbine or gas turbine cycle. The SOFC works at atmospheric or pressurized conditions and the resulting power plant exceeds 78% LHV efficiency without CO2 capture (as discussed in part A of the work) and 70% LHV efficiency with substantial CO2 capture (part B). The power plants are simulated at the 100 MW scale with a complete set of realistic assumptions about fuel cell (FC) performance, plant components and auxiliaries, presenting detailed energy and material balances together with a second law analysis.

  8. Hybrid heat exchange for the compression capture of CO2 from recirculated flue gas

    SciTech Connect

    Oryshchyn, Danylo B.; Ochs, Thomas L.; Summers, Cathy A.

    2004-01-01

    An approach proposed for removal of CO2 from flue gas cools and compresses a portion of a recirculated flue-gas stream, condensing its volatile materials for capture. Recirculating the flue gas concentrates SOx, H2O and CO2 while dramatically reducing N2 and NOx, enabling this approach, which uses readily available industrial components. A hybrid system of indirect and direct-contact heat exchange performs heat and mass transfer for pollutant removal and energy recovery. Computer modeling and experimentation combine to investigate the thermodynamics, heat and mass transfer, chemistry and engineering design of this integrated pollutant removal (IPR) system.

  9. Predicting Large CO2 Adsorption in Aluminosilicate Zeolites for Postcombustion Carbon Dioxide Capture

    SciTech Connect

    Kim, J; Lin, LC; Swisher, JA; Haranczyk, M; Smit, B

    2012-11-21

    Large-scale simulations of aluminosilicate zeolites were conducted to identify structures that possess large CO2 uptake for postcombustion carbon dioxide capture. In this study, we discovered that the aluminosilicate zeolite structures with the highest CO2 uptake values have an idealized silica lattice with a large free volume and a framework topology that maximizes the regions with nearest-neighbor framework atom distances from 3 to 4.5 angstrom. These predictors extend well to different Si:Al ratios and for both Na+ and Ca2+ cations, demonstrating their universal applicability in identifying the best-performing aluminosilicate zeolite structures.

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

    NASA Astrophysics Data System (ADS)

    Calvo-Muñoz, Elisa; García-Mateos, Francisco José; Rosas, Juana; Rodríguez-Mirasol, José; Cordero, Tomás

    2016-05-01

    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.

  11. Development of a carbonate absorption-based process for post-combustion CO2 capture: The role of biocatalyst to promote CO2 absorption rate

    USGS Publications Warehouse

    Lu, Y.; Ye, X.; Zhang, Z.; Khodayari, A.; Djukadi, T.

    2011-01-01

    An Integrated Vacuum Carbonate Absorption Process (IVCAP) for post-combustion carbon dioxide (CO2) capture is described. IVCAP employs potassium carbonate (PC) as a solvent, uses waste or low quality steam from the power plant for CO2 stripping, and employs a biocatalyst, carbonic anhydrase (CA) enzyme, for promoting the CO2 absorption into PC solution. A series of experiments were performed to evaluate the activity of CA enzyme mixed in PC solutions in a stirred tank reactor system under various temperatures, CA dosages, CO2 loadings, CO2 partial pressures, and the presence of major flue gas contaminants. It was demonstrated that CA enzyme is an effective biocatalyst for CO2 absorption under IVCAP conditions. ?? 2011 Published by Elsevier Ltd.

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

    PubMed

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

    2016-12-05

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

  13. CO2 adsorption and separation from natural gason phosphorene surface: Combining DFT and GCMC calculations

    NASA Astrophysics Data System (ADS)

    Zhang, Yayun; Liu, Chao; Hao, Feng; Xiao, Hang; Zhang, Shiwei; Chen, Xi

    2017-03-01

    We have examined the performance of phosphorene-based material, phosphorene slit pores (PSP), in CO2 adsorption and separation from natural gas by using Density Function Theory (DFT) calculation and Grand Canonical Monte Carlo (GCMC) simulations. First, the adsorption of CH4 and CO2molecules on phosphorene sheet were conducted by DFT study. Then, adsorption performances of natural gas components as well as their binary CO2/CH4 gas mixture were investigated at 300 K with the pressure up to 3.0 MPa. The effects of slit pore width, H, and mole ratio of CO2/CH4in the gas phase on the separation of CO2 from mixtures of CO2/CH4 were also investigated. Our DFT calculation results show that the CO2 moleculehas higher adsorption energy than that of CH4, which implies that it can be easily adsorbed to the phosphorene surface than CH4. Detailed GCMC simulations reveal that the phosphorene slit pore has a high performance in separating CO2fromnature gas and achieves the highest gas selectivity at H = 1.0 nm at pressures lower than 0.1 MPa. Moreover, the selectivity of CO2 overCO2/CH4gas mixture increases with increasing the mole ratio of CO2/CH4due to the enhanced adsorbate-adsorbent interactions for the favorable component. Therefore, it is suggested that the phosphorene is a promising candidate for natural gas purification and possessing practical potential applications in gas adsorption.

  14. Optimization of selection of chain amine scrubbers for CO2 capture.

    PubMed

    Al-Marri, Mohammed J; Khader, Mahmoud M; Giannelis, Emmanuel P; Shibl, Mohamed F

    2014-12-01

    In order to optimize the selection of a suitable amine molecule for CO2 scrubbers, a series of ab initio calculations were performed at the B3LYP/6-31+G(d,p) level of theory. Diethylenetriamine was used as a simple chain amine. Methyl and hydroxyl groups served as examples of electron donors, and electron withdrawing groups like trifluoromethyl and nitro substituents were also evaluated. Interaction distances and binding energies were employed as comparison operators. Moreover, natural bond orbital (NBO) analysis, namely the second order perturbation approach, was applied to determine whether the amine-CO2 interaction is chemical or physical. Different sizes of substituents affect the capture ability of diethylenetriamine. For instance, trifluoromethyl shields the nitrogen atom to which it attaches from the interaction with CO2. The results presented here provide a means of optimizing the choice of amine molecules for developing new amine scrubbers.

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

    PubMed

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

    2013-12-02

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

  16. Confinement of Ionic Liquids in Nanocages: Tailoring the Molecular Sieving Properties of ZIF-8 for Membrane-Based CO2 Capture.

    PubMed

    Ban, Yujie; Li, Zhengjie; Li, Yanshuo; Peng, Yuan; Jin, Hua; Jiao, Wenmei; Guo, Ang; Wang, Po; Yang, Qingyuan; Zhong, Chongli; Yang, Weishen

    2015-12-14

    Fine-tuning of effective pore size of microporous materials is necessary to achieve precise molecular sieving properties. Herein, we demonstrate that room temperature ionic liquids can be used as cavity occupants for modification of the microenvironment of MOF nanocages. Targeting CO2 capture applications, we tailored the effective cage size of ZIF-8 to be between CO2 and N2 by confining an imidazolium-based ionic liquid [bmim][Tf2 N] into ZIF-8's SOD cages by in-situ ionothermal synthesis. Mixed matrix membranes derived from ionic liquid-modified ZIF-8 exhibited remarkable combinations of permeability and selectivity that transcend the upper bound of polymer membranes for CO2 /N2 and CO2 /CH4 separation. We observed an unusual response of the membranes to varying pressure, that is, an increase in the CO2 /CH4 separation factor with pressure, which is highly desirable for practical applications in natural gas upgrading.

  17. Comparison of volatiles and mosquito capture efficacy for three carbohydrate sources in a yeast-fermentation CO2 generator

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Mosquito surveillance in remote areas with limited access to canisters of CO2 or dry ice will benefit from an effective alternative CO2 source. In this study, we document the differences in mosquito and non-mosquito capture rates from CO2 baited (dry ice or yeast fermentation of carbohydrates) CDC t...

  18. The Black Lake (Quebec, Canada) mineral carbonation experimental station: CO2 capture in mine waste

    NASA Astrophysics Data System (ADS)

    Beaudoin, G.; Constantin, M.; Duchesne, J.; Dupuis, C.; Entrazi, A.; Gras, A.; Huot, F.; Fortier, R.; Hebert, R.; Larachi, F.; Lechat, K.; Lemieux, J. M.; Molson, J. W. H.; Maldague, X.; Therrien, R.; Assima, G. P.

    2014-12-01

    Passive mineral carbonation of chrysotile mining and milling waste was discovered at the Black Lake mine, southern Québec, 10 years ago. Indurated crusts were found at the surface and within waste piles where mineral and rock fragments are cemented by hydrated magnesium carbonates. A long-term research program has yielded significant insight into the process of CO2 capture from the atmosphere, and how it can be implemented during mining operations. Laboratory experiments show that the waste mineralogy is crucial, brucite being more reactive than serpentine. Partial water saturation, circa 40%, is also critical to dissolve magnesium from minerals, and transport aqueous CO2 to precipitation sites. Grain armoring by iron oxidation induced by dissolved oxygen prevents further reaction. Two experimental cells constructed with milling waste and fitted with various monitoring probes (T, H2O content, leachate) and gas sampling ports, have been monitored for more than 3 years, along with environmental conditions. The interstitial gas in the cells remains depleted in CO2 indicating continuous capture of ambient atmospheric CO2 at rates faster than advection to reaction sites. The energy released by the exothermic mineral carbonation reactions has been observed both in laboratory experiments (up to 4 °C) and in the field. Warm air, depleted to 10 ppmv CO2, vents at the surface of the waste piles, indicating reaction with atmospheric CO2 deep inside the piles. A thermal anomaly, detected by airborne infrared and coincident with a known venting area, was selected for locating a 100 m deep borehole fitted with sensor arrays to monitor active mineral carbonation within the pile. The borehole has intersected areas where mineral carbonation has indurated the milling waste. The borehole will be monitored for the next 3 years to better understand the mineral carbonation process, and its potential to yield recoverable geothermal energy in mining environments.

  19. A novel methodology for assessing the environmental sustainability of ionic liquids used for CO2 capture.

    PubMed

    Cuéllar-Franca, Rosa M; García-Gutiérrez, Pelayo; Taylor, S F Rebecca; Hardacre, Christopher; Azapagic, Adisa

    2016-10-20

    Ionic liquids (ILs) have been proposed as suitable sorbents for CO2 capture because of their high CO2 absorption capacity, thermal stability, negligible vapour pressure and physico-chemical tunability. However, the environmental implications of ILs are currently largely unknown because of a lack of data. The issue is further complicated by their complex chemical structures and numerous precursors for which environmental data are scarce or non-existent. In an attempt to address this issue, this paper presents a new methodology for estimating life cycle environmental impacts of novel ILs, with the aim of aiding synthesis and selection of more sustainable CO2 sorbents. The methodology consists of four main steps: (1) selection of an appropriate IL and synthesis route; (2) construction of a life cycle tree; (3) life cycle assessment; and (4) recommendations for improvements. The application of the methodology is illustrated using trihexyltetradecylphosphonium 1,2,4-triazolide ([P66614][124Triz]), a promising IL for CO2 capture currently under development. Following the above steps, the paper demonstrates how the data obtained from laboratory synthesis of the IL can be scaled up to industrial production to estimate life cycle impacts and identify environmental hotspots. In this particular case, the main hotspots are the precursors used in the synthesis of the IL. Comparison of impacts with monoethanolamine (MEA), currently the most widely-used CO2 sorbent, suggests that [P66614][124Triz] has much higher impacts than MEA, including global warming potential. However, human toxicity potential is significantly higher for MEA. Therefore, the proposed methodology can be used to optimise the design of ILs and to guide selection of more sustainable CO2 sorbents. Although the focus is on ILs, the methodology is generic and can be applied to other chemicals under development.

  20. Metal-organic framework supported ionic liquid membranes for CO2 capture: anion effects.

    PubMed

    Gupta, Krishna M; Chen, Yifei; Hu, Zhongqiao; Jiang, Jianwen

    2012-04-28

    IRMOF-1 supported ionic liquid (IL) membranes are investigated for CO(2) capture by atomistic simulation. The ILs consist of identical cation 1-n-butyl-3-methylimidazolium [BMIM](+), but four different anions, namely hexafluorophosphate [PF(6)](-), tetrafluoroborate [BF(4)](-), bis(trifluoromethylsulfonyl)imide [Tf(2)N](-), and thiocyanate [SCN](-). As compared with the cation, the anion has a stronger interaction with IRMOF-1 and a more ordered structure in IRMOF-1. The small anions [PF(6)](-), [BF(4)](-), and [SCN](-) prefer to locate near to the metal-cluster, particularly the quasi-spherical [PF(6)](-) and [BF(4)](-). In contrast, the bulky and chain-like [BMIM](+) and [Tf(2)N](-) reside near the phenyl ring. Among the four anions, [Tf(2)N](-) has the weakest interaction with IRMOF-1 and thus the strongest interaction with [BMIM](+). With increasing the weight ratio of IL to IRMOF-1 (W(IL/IRMOF-1)), the selectivity of CO(2)/N(2) at infinite dilution is enhanced. At a given W(IL/IRMOF-1), the selectivity increases as [Tf(2)N](-) < [PF(6)](-) < [BF(4)](-) < [SCN](-). This hierarchy is predicted by the COSMO-RS method, and largely follows the order of binding energy between CO(2) and anion estimated by ab initio calculation. In the [BMIM][SCN]/IRMOF-1 membrane with W(IL/IRMOF-1) = 1, [SCN](-) is identified to be the most favorable site for CO(2) adsorption. [BMIM][SCN]/IRMOF-1 outperforms polymer membranes and polymer-supported ILs in CO(2) permeability, and its performance surpasses Robeson's upper bound. This simulation study reveals that the anion has strong effects on the microscopic properties of ILs and suggests that MOF-supported ILs are potentially intriguing for CO(2) capture.

  1. Analysis of CO2 Separation from Flue Gas, Pipeline Transportation, and Sequestration in Coal

    SciTech Connect

    Eric P. Robertson

    2007-09-01

    This report was written to satisfy a milestone of the Enhanced Coal Bed Methane Recovery and CO2 Sequestration task of the Big Sky Carbon Sequestration project. The report begins to assess the costs associated with separating the CO2 from flue gas and then injecting it into an unminable coal seam. The technical challenges and costs associated with CO2 separation from flue gas and transportation of the separated CO2 from the point source to an appropriate sequestration target was analyzed. The report includes the selection of a specific coal-fired power plant for the application of CO2 separation technology. An appropriate CO2 separation technology was identified from existing commercial technologies. The report also includes a process design for the chosen technology tailored to the selected power plant that used to obtain accurate costs of separating the CO2 from the flue gas. In addition, an analysis of the costs for compression and transportation of the CO2 from the point-source to an appropriate coal bed sequestration site was included in the report.

  2. Operation of a cyclonic preheater in the Ca-looping for CO2 capture.

    PubMed

    Martínez, Ana; Lara, Yolanda; Lisbona, Pilar; Romeo, Luis M

    2013-10-01

    Calcium looping is an emerging technology for CO2 capture that makes use of the calcium oxide as a sorbent. One of its main issues is the significant energy consumption in the calciner, where the regeneration of the sorbent takes place. Nevertheless, as a high temperature looping technology, the surplus heat flows may be used to reduce the energy needs in this reactor. The addition of a cyclonic preheater similar to those used in the cement industry is proposed in this work. A calcium looping system was modeled and simulated to assess the advantages and disadvantages of the inclusion of a cyclonic preheater. Despite the negative effect on the maximum average capture capacity of the sorbent, a reduction on the coal and oxygen consumptions and on the extra CO2 generated in the calciner is obtained.

  3. Electrocatalytically switchable CO2 capture: first principle computational exploration of carbon nanotubes with pyridinic nitrogen.

    PubMed

    Jiao, Yan; Zheng, Yao; Smith, Sean C; Du, Aijun; Zhu, Zhonghua

    2014-02-01

    The front cover artwork for issue 12/2013 is provided by the group of Prof. Zhonghua Zhu, in collaboration with Prof. Sean C. Smith of Oak Ridge National Laboratory, and Prof. Aijun Du from Queensland University of Technology. The image shows how carbon nanotubes and/or graphene with doped pyridinic nitrogen could be applied for controllable, highly selective, and reversible CO2 capture. The Full Paper itself is available at 10.1002/cssc.201300624.

  4. Fabrication of conjugated microporous polytriazine nanotubes and nanospheres for highly selective CO2 capture.

    PubMed

    Wang, Zhiqiang; Liu, Junling; Fu, Yu; Liu, Cheng; Pan, Chunyue; Liu, Zhiyong; Yu, Guipeng

    2017-04-06

    A one-spot template approach for fabricating porous organic nanotubes was developed and a molecular design, i.e. introducing thiophene and s-triazine functionalities to enhance host-guest interactions, lead to novel porous solids with high capacities for CO2 and exceptionally high ideal selectivities over N2 for effective gas storage and separation.

  5. Evaluation of Metal-Organic Frameworks and Porous Polymer Networks for CO2 -Capture Applications.

    PubMed

    Verdegaal, Wolfgang M; Wang, Kecheng; Sculley, Julian P; Wriedt, Mario; Zhou, Hong-Cai

    2016-03-21

    This manuscript presents experimental data for 20 adsorption materials (metal-organic frameworks, porous polymer networks, and Zeolite-5A), including CO2 and N2 isotherms and heat capacities. With input from only experimental data, working capacities per energy for each material were calculated. Furthermore, by running seven different carbon-capture scenarios in which the initial flue-gas composition and process temperature was systematically changed, we present a range of performances for each material and quantify how sensitive each is to these varying parameters. The presented calculations provide researchers with a tool to investigate promising carbon-capture materials more easily and completely.

  6. Progress with the development of a CO 2 capturing solid oxide fuel cell

    NASA Astrophysics Data System (ADS)

    Haines, M. R.; Heidug, W. K.; Li, K. J.; Moore, J. B.

    In April 2000 Siemens Westinghouse started work under a co-operation agreement with Shell International to develop and demonstrate a natural gas fired 0.25 MW solid oxide fuel cell (SOFC) modified to enable capture of carbon dioxide. The basic principles of this development and initial plans for the demonstration, which is due to start up at a Norwegian location in 2003, have been presented in environmental and fuel cell forums during 1999/2000. This paper reviews the latest technical progress with this development and discusses the large potential market for stationary power generation using SOFCs with CO 2 capturing capability.

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

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

  8. Pilot-scale production of mesoporous silica-based adsorbent for CO2 capture

    NASA Astrophysics Data System (ADS)

    Wang, Hou Chuan; Lu, Chungsying; Bai, Hsunling; Hwang, Jyh Feng; Lee, Hsiu Hsia; Chen, Wang; Kang, Yuhao; Chen, Shing-Ting; Su, Fengsheng; Kuo, Shih-Chun; Hu, Fang-Chun

    2012-07-01

    This study presents a pilot-scale spray drying system designed to manufacture spherical mesoporous silica particles (MSP) that is capable of producing up to 100 g per hour. The MSP fabricated via a nozzle pressure of 4 kg/cm2 and a drying temperature of 200 °C possess a high specific area of 1012 m2/g, a narrow pore size distribution with an average pore diameter of 2.4 nm, and large pore volume of 0.81 cm3/g. They were further modified with a tetraethylenepentamine (TEPA-MSP) to enhance CO2 adsorption selectivity from gas streams. The adsorption capacity of 15% CO2 on TEPA-MSP was significantly influenced by adsorption temperature and water vapor of air streams, and reached a maximum of 87.05 mg/g (1.98 mmol/g) at 60 °C and 129.19 mg/g (2.94 mmol/g) at a water vapor of 6.98%. The adsorption capacities and the physicochemical properties of TEPA-MSP were preserved through 20 cycles of adsorption-desorption operation. A comparative study revealed that the TEPA-MSP had better adsorption performance of 15% CO2 than the TEPA-modified granular activated carbon and zeolite. These results suggest that the TEPA-MSP can be stably employed in the prolonged cyclic CO2 adsorption and that they possess good potential for CO2 capture from flue gas.

  9. Amphiphilic Graft Copolymer Nanospheres: From Colloidal Self-Assembly to CO2 Capture Membranes.

    PubMed

    Jeon, Harim; Kim, Dong Jun; Park, Min Su; Ryu, Du Yeol; Kim, Jong Hak

    2016-04-13

    Colloidal nanosphere self-assembly effectively generates ordered nanostructures, prompting tremendous interest in many applications such as photonic crystals and templates for inverse opal fabrication. Here we report the self-assembly of low-cost, graft copolymer nanospheres for CO2 capture membranes. Specifically, poly(dimethylsiloxane)-graft-poly(4-vinylpyridine) (PDMS-g-P4VP) is synthesized via one-pot, free radical dispersion polymerization to give discrete monodisperse nanospheres. These nanospheres comprise a surface-anchored highly permeable PDMS layer and internal CO2-philic P4VP spherical core. Their diameter is controllable below the submicrometer range by varying grafting ratios. The colloidal dispersion forms a long-range, close-packed hexagonal array on a substrate by inclined deposition and convective assembly. The array shows dispersion medium-dependent packing characteristics. A thermodynamic correlation is determined using different solvents to obtain stable PDMS-g-P4VP dispersions and interpreted in terms of Flory-Huggins interaction parameter. As a proof-of-concept, the implementation of these nanospheres into membranes simultaneously enhances the CO2 permeability and CO2/N2 selectivity of PDMS-based transport matrixes. Upon physical aging of the solution, the CO2/N2 selectivity is improved up to 26, one of the highest values for highly permeable PDMS-based polymeric membranes.

  10. Co-location of air capture, subseafloor CO2 sequestration, and energy production on the Kerguelen plateau.

    PubMed

    Goldberg, David S; Lackner, Klaus S; Han, Patrick; Slagle, Angela L; Wang, Tao

    2013-07-02

    Reducing atmospheric CO2 using a combination of air capture and offshore geological storage can address technical and policy concerns with climate mitigation. Because CO2 mixes rapidly in the atmosphere, air capture could operate anywhere and in principle reduce CO2 to preindustrial levels. We investigate the Kerguelen plateau in the Indian Ocean, which offers steady wind resources, vast subseafloor storage capacities, and minimal risk of economic damages or human inconvenience and harm. The efficiency of humidity swing driven air capture under humid and windy conditions is tested in the laboratory. Powered by wind, we estimate ∼75 Mt CO2/yr could be collected using air capture and sequestered below seafloor or partially used for synfuel. Our analysis suggests that Kerguelen offers a remote and environmentally secure location for CO2 sequestration using renewable energy. Regional reservoirs could hold over 1500 Gt CO2, sequestering a large fraction of 21st century emissions.

  11. Electrochemical CO2 and O2 separation for crew and plant environments

    NASA Technical Reports Server (NTRS)

    Lee, M. G.; Grigger, David J.; Foerg, Sandra L.

    1992-01-01

    The study describes a closed ecosystem concept that includes electrochemical CO2 and O2 separators and a moisture condenser/separator for maintaining CO2, O2, and humidity levels in the crew and plant habitats at their respective optimal conditions. The key processes of this concept are aqueous electrolyte-based electrochemical CO2 and O2 separations. The principles and cell characteristics of these electrochemical gas separation processes are described. Also presented are descriptions of test hardware and the test results of the Electrochemical CO2 Separator (ECS) and the Electrochemical O2 Separator (EOS), and the combination of the ECS and the EOS. The test results proved that the ECS and EOS processes for the combined concept are viable.

  12. Towards understanding organic nitrogen species in emissions from post-combustion CO2 capture plants

    NASA Astrophysics Data System (ADS)

    Ge, X.; Zhang, Q.

    2012-12-01

    Post-combustion capture of carbon dioxide using aqueous amine solutions is the most advanced technology for reducing CO2 emissions from fossil fuel power plants. This technology, however, may lead to the emissions of amines and various nitrogen-containing degradation products with serious potential implications for human health and the environment. Understanding the chemistry of emissions from amine-based CO2-capture plants is therefore important and requires analytical methods that are capable of thoroughly characterizing the composition and concentration of organic nitrogen (ON) species in actual or simulated flue gas. In this study, we have developed a suite of methods for analyzing particulate and gaseous samples for the bulk and molecular compositions of these species. Specifically, we have optimized high-resolution aerosol mass spectrometry (HR-ToF-AMS) for real-time and offline analyses of the bulk chemistry of ON species. We have also developed methods for quantitatively analyzing up to 12 amino compounds using ion chromatography. In addition, by applying liquid chromatography-tandem mass spectrometry (LC-MS/MS), we have studied the molecular masses and empirical formulas of individual ON molecules. This suite of techniques has been applied for characterizing liquid and particulate samples generated from simulated amine-based CO2 capture process. The results from these analyses will be presented.

  13. CO2 capture and conversion with a multifunctional polyethyleneimine-tethered iminophosphine iridium catalyst/adsorbent.

    PubMed

    McNamara, Nicholas D; Hicks, Jason C

    2014-04-01

    Tunable, multifunctional materials able to capture CO2 and subsequently catalyze its conversion to formic acid were synthesized by the modification of branched polyethyleneimine (PEI) with an iminophosphine ligand coordinated to an Ir precatalyst. The molecular weight of the PEI backbone was an important component for material stability and catalytic activity, which were inversely related. The amine functionalities on PEI served three roles: 1) primary amines were used to tether the ligand and precatalyst, 2) amines were used to capture CO2 , and 3) amines served as a base for formate stabilization during catalysis. Ligand studies on imine and phosphine based ligands showed that a bidentate iminophosphine ligand resulted in the highest catalytic activity. X-ray photoelectron spectroscopy revealed that an increase in Ir 4f binding energy led to an increase in catalytic activity, which suggests that the electronics of the metal center play a significant role in catalysis. Catalyst loading studies revealed that there is a critical balance between free amines and ligand-metal sites that must be reached to optimize catalytic activity. Thus, it was found that the CO2 capture and conversion abilities of these materials could be optimized for reaction conditions by tuning the structure of the PEI-tethered materials.

  14. Bench-Scale Process for Low-Cost Carbon Dioxide (CO2) Capture Using a Phase-Changing Absorbent

    SciTech Connect

    Westendorf, Tiffany; Caraher, Joel; Chen, Wei; Farnum, Rachael; Perry, Robert; Spiry, Irina; Wilson, Paul; Wood, Benjamin

    2015-03-31

    The objective of this project is to design and build a bench-scale process for a novel phase-changing aminosilicone-based CO2-capture solvent. The project will establish scalability and technical and economic feasibility of using a phase-changing CO2-capture absorbent for post-combustion capture of CO2 from coal-fired power plants with 90% capture efficiency and 95% CO2 purity at a cost of $40/tonne of CO2 captured by 2025 and a cost of <$10/tonne of CO2 captured by 2035. In the first budget period of this project, the bench-scale phase-changing CO2 capture process was designed using data and operating experience generated under a previous project (ARPA-e project DE-AR0000084). Sizing and specification of all major unit operations was completed, including detailed process and instrumentation diagrams. The system was designed to operate over a wide range of operating conditions to allow for exploration of the effect of process variables on CO2 capture performance.

  15. Imine-Linked Polymer Based Nitrogen-Doped Porous Activated Carbon for Efficient and Selective CO2 Capture

    PubMed Central

    Alabadi, Akram; Abbood, Hayder A.; Li, Qingyin; Jing, Ni; Tan, Bien

    2016-01-01

    The preparation of nitrogen-doped activated carbon (NACs) has received significant attention because of their applications in CO2 capture and sequestration (CCS) owing to abundant nitrogen atoms on their surface and controllable pore structures by carefully controlled carbonization. We report high-surface-area porous N-doped activated carbons (NAC) by using soft-template-assisted self-assembly followed by thermal decomposition and KOH activation. The activation process was carried out under different temperature conditions (600–800 °C) using polyimine as precursor. The NAC-800 was found to have a high specific surface area (1900 m2 g−1), a desirable micropore size below 1 nm and, more importantly, a large micropore volume (0.98 cm3 g−1). NAC-800 also exhibits a significant capacity of CO2 capture i.e., over 6. 25 and 4.87 mmol g−1 at 273 K and 298 K respectively at 1.13 bar, which is one of among the highest values reported for porous carbons so far. Moreover, NAC also shows an excellent separation selectivity for CO2 over N2. PMID:27958305

  16. Imine-Linked Polymer Based Nitrogen-Doped Porous Activated Carbon for Efficient and Selective CO2 Capture

    NASA Astrophysics Data System (ADS)

    Alabadi, Akram; Abbood, Hayder A.; Li, Qingyin; Jing, Ni; Tan, Bien

    2016-12-01

    The preparation of nitrogen-doped activated carbon (NACs) has received significant attention because of their applications in CO2 capture and sequestration (CCS) owing to abundant nitrogen atoms on their surface and controllable pore structures by carefully controlled carbonization. We report high-surface-area porous N-doped activated carbons (NAC) by using soft-template-assisted self-assembly followed by thermal decomposition and KOH activation. The activation process was carried out under different temperature conditions (600–800 °C) using polyimine as precursor. The NAC-800 was found to have a high specific surface area (1900 m2 g‑1), a desirable micropore size below 1 nm and, more importantly, a large micropore volume (0.98 cm3 g‑1). NAC-800 also exhibits a significant capacity of CO2 capture i.e., over 6. 25 and 4.87 mmol g‑1 at 273 K and 298 K respectively at 1.13 bar, which is one of among the highest values reported for porous carbons so far. Moreover, NAC also shows an excellent separation selectivity for CO2 over N2.

  17. Impact of tuning CO2-philicity in polydimethylsiloxane-based membranes for carbon dioxide separation

    DOE PAGES

    Hong, Tao; Chatterjee, Sabornie; Mahurin, Shannon M.; ...

    2017-02-22

    Amidoxime-functionalized polydimethylsiloxane (AO-PDMSPNB) membranes with various amidoxime compositions were synthesized via ring-opening metathesis polymerization followed by post-polymerization modification. Compared to other previously reported PDMS-based membranes, the amidoxime-functionalized membranes show enhanced CO2 permeability and CO2/N2 selectivity. The overall gas separation performance (CO2 permeability 6800 Barrer; CO2/N2 selectivity 19) of the highest performing membrane exceeds the Robeson upper bound line, and the excellent permeability of the copolymer itself provides great potential for real world applications where huge volumes of gases are separated. This study details how tuning the CO2-philicity within rubbery polymer matrices influences gas transport properties. Key parameters for tuning gasmore » transport properties are discussed, and the experimental results show good consistency with theoretical calculations. Finally, this study provides a roadmap to enhancing gas separation performance in rubbery polymers by tuning gas solubility selectivity.« less

  18. Spectroscopic investigation into oxidative degradation of silica-supported amine sorbents for CO(2) capture.

    PubMed

    Srikanth, Chakravartula S; Chuang, Steven S C

    2012-08-01

    Oxidative degradation characteristics of silica-supported amine sorbents with varying amounts of tetraethylenepentamine (TEPA) and polyethylene glycol (PEG; P(200) or P(600) represents PEG with molecular weights of 200 or 600) have been studied by IR and NMR spectroscopy. Thermal treatment of the sorbents and liquid TEPA at 100 °C for 12 h changed their color from white to yellow. The CO(2) capture capacity of the TEPA/SiO(2) sorbents (i.e., SiO(2)-supported TEPA with a TEPA/SiO(2) ratio of 25:75) decreased by more than 60 %. IR and NMR spectroscopy studies showed that the yellow color of the degraded sorbents resulted from the formation of imide species. The imide species, consisting of NH associated with two C=O functional groups, were produced from the oxidation of methylene groups in TEPA. Imide species on the degraded sorbent are not capable of binding CO(2) due to its weak basicity. The addition of P(200) and P(600) to the supported amine sorbents improved both their CO(2) capture capacities and oxidative degradation resistance. IR spectroscopy results also showed that TEPA was immobilized on the SiO(2) surface through hydrogen bonding between amine groups and the silanol groups of SiO(2). The OH groups of PEG interact with NH(2) /NH of TEPA through hydrogen bonding. Hydrogen bonds disperse TEPA on SiO(2) and block O(2) from accessing TEPA for oxidation. Oxidative degradation resistance and CO(2) capture capacity of the supported amine sorbents can be optimized through adjusting the ratio of hydroxyl to amine groups in the TEPA/PEG mixture.

  19. Spectroscopic Investigation into Oxidative Degradation of Silica-Supported Amine Sorbents for CO2 Capture

    PubMed Central

    Srikanth, Chakravartula S; Chuang, Steven S C

    2012-01-01

    Oxidative degradation characteristics of silica-supported amine sorbents with varying amounts of tetraethylenepentamine (TEPA) and polyethylene glycol (PEG; P200 or P600 represents PEG with molecular weights of 200 or 600) have been studied by IR and NMR spectroscopy. Thermal treatment of the sorbents and liquid TEPA at 100 °C for 12 h changed their color from white to yellow. The CO2 capture capacity of the TEPA/SiO2 sorbents (i.e., SiO2-supported TEPA with a TEPA/SiO2 ratio of 25:75) decreased by more than 60 %. IR and NMR spectroscopy studies showed that the yellow color of the degraded sorbents resulted from the formation of imide species. The imide species, consisting of NH associated with two C—O functional groups, were produced from the oxidation of methylene groups in TEPA. Imide species on the degraded sorbent are not capable of binding CO2 due to its weak basicity. The addition of P200 and P600 to the supported amine sorbents improved both their CO2 capture capacities and oxidative degradation resistance. IR spectroscopy results also showed that TEPA was immobilized on the SiO2 surface through hydrogen bonding between amine groups and the silanol groups of SiO2. The OH groups of PEG interact with NH2/NH of TEPA through hydrogen bonding. Hydrogen bonds disperse TEPA on SiO2 and block O2 from accessing TEPA for oxidation. Oxidative degradation resistance and CO2 capture capacity of the supported amine sorbents can be optimized through adjusting the ratio of hydroxyl to amine groups in the TEPA/PEG mixture. PMID:22744858

  20. DUAL PHASE MEMBRANE FOR HIGH TEMPERATURE CO2 SEPARATION

    SciTech Connect

    Jerry Y.S. Lin

    2002-12-01

    This project is aimed at synthesis of a new inorganic dual-phase carbonate membrane for high temperature CO{sub 2} separation. Metal-carbonate dual-phase membranes were prepared by the direct infiltration method and the synthesis conditions were optimized. The dual-phase membranes are gas-tight with helium permeance about six orders of magnitude lower than that for the metal support. Efforts were made to test seals for permeation and separation experiments for dual-phase membrane at the intermediate temperature range (about 500 C) under oxidizing atmosphere. An effective new permeation cell with a metal seal was designed, fabricated and tested. The permeation setup provided leak-free sealing for the dual-phase membranes under the desired operation conditions. Though the reliable data showing high permeance for carbon dioxide with oxygen for the prepared metal-carbonate dual phase membrane has not been measured, the research efforts in improving membrane synthesis and setting up a new permeation cell with suitable seal have made it closer for one to demonstrate good dual-phase membranes for high temperature carbon dioxide separation. Research efforts were also directed towards preparation of a new ceramic-carbonate dual-phase membrane. Porous lanthanum cobaltite (LC) perovskite type oxide ceramic support with oxidation resistance better than the metal support and high electronic conductivity (1300-1500 S/cm in 400-600 C), was prepared and studied as an alternative support for the dual-phase carbonate membranes. The LC powder was found not reactive with the carbonate at 600 C. The porous LC disks have helium permeance and pore diameter smaller than the metal support but larger than the common {alpha}-alumina support. These results show promise to use the LC support for preparation of oxidation resistant dual-phase carbonate membranes.

  1. Direct Air Capture of CO2 - an Overview of Carbon Engineering's Technology and Pilot Plant Development

    NASA Astrophysics Data System (ADS)

    Holmes, G.; Corless, A.

    2014-12-01

    At Carbon Engineering, we are developing and commercializing technology to scrub CO2 directly from atmospheric air at industrial scale. By providing atmospheric CO2 for use in fuel production, we can enable production of transportation fuels with ultra-low carbon intensities, which command price premiums in the growing set of constrained fuels markets such as California's LCFS. We are a Calgary based startup founded in 2009 with 10 employees, and we are considered a global leader in the direct air capture (DAC) field. We will review CE's DAC technology, based on a wet-scrubbing "air contactor" which absorbs CO2 into aqueous solution, and a chemical looping "regeneration" component, which liberates pure CO2 from this aqueous solution while re-making the original absorption chemical. CE's DAC tecnology exports purified atmospheric CO2, combined with the combustion CO2 from plant energy usage, as the end product. We will also discuss CE's 2014-2015 end-to-end Pilot Demonstration Unit. This is a $7M technology demonstration plant that CE is building with the help of key industrial partners and equipment vendors. Vendor design and engineering requirements have been used to specify the pilot air contactor, pellet reactor, calciner, and slaker modules, as well as auxiliary systems. These modules will be run for several months to obtain the engineering and performance data needed for subsequent commercial plant design, as well as to test the residual integration risks associated with CE's process. By the time of the AGU conference, the pilot is expected to be in late stages of fabrication or early stages of site installation.

  2. Ultralow Parasitic Energy for Postcombustion CO2 Capture Realized in a Nickel Isonicotinate Metal-Organic Framework with Excellent Moisture Stability.

    PubMed

    Nandi, Shyamapada; Collins, Sean; Chakraborty, Debanjan; Banerjee, Debasis; Thallapally, Praveen K; Woo, Tom K; Vaidhyanathan, Ramanathan

    2017-02-08

    Metal-organic frameworks (MOFs) have attracted significant attention as solid sorbents in gas separation processes for low-energy postcombustion CO2 capture. The parasitic energy (PE) has been put forward as a holistic parameter that measures how energy efficient (and therefore cost-effective) the CO2 capture process will be using the material. In this work, we present a nickel isonicotinate based ultramicroporous MOF, 1 [Ni-(4PyC)2·DMF], that has the lowest PE for postcombustion CO2 capture reported to date. We calculate a PE of 655 kJ/kg CO2, which is lower than that of the best performing material previously reported, Mg-MOF-74. Further, 1 exhibits exceptional hydrolytic stability with the CO2 adsorption isotherm being unchanged following 7 days of steam-treatment (>85% RH) or 6 months of exposure to the atmosphere. The diffusion coefficient of CO2 in 1 is also 2 orders of magnitude higher than in zeolites currently used in industrial scrubbers. Breakthrough experiments show that 1 only loses 7% of its maximum CO2 capacity under humid conditions.

  3. Dual Phase Membrane for High Temperature CO2 Separation

    SciTech Connect

    Jerry Lin

    2007-06-30

    This project aimed at synthesis of a new inorganic dual-phase carbonate membrane for high temperature CO{sub 2} separation. Metal-carbonate dual-phase membranes were prepared by the direct infiltration method and the synthesis conditions were optimized. Permeation tests for CO{sub 2} and N{sub 2} from 450-750 C showed very low permeances of those two gases through the dual-phase membrane, which was expected due to the lack of ionization of those two particular gases. Permeance of the CO{sub 2} and O{sub 2} mixture was much higher, indicating that the gases do form an ionic species, CO{sub 3}{sup 2-}, enhancing transport through the membrane. However, at temperatures in excess of 650 C, the permeance of CO{sub 3}{sup 2-} decreased rapidly, while predictions showed that permeance should have continued to increase with temperature. XRD data obtained from used membrane indicated that lithium iron oxides formed on the support surface. This lithium iron oxide layer has a very low conductivity, which drastically reduces the flow of electrons to the CO{sub 2}/O{sub 2} gas mixture; thus limiting the formation of the ionic species required for transport through the membrane. These results indicated that the use of stainless steel supports in a high temperature oxidative environment can lead to decreased performance of the membranes. This revelation created the need for an oxidation resistant support, which could be gained by the use of a ceramic-type membrane. Work was extended to synthesize a new inorganic dual-phase carbonate membrane for high temperature CO{sub 2} separation. Helium permeance of the support before and after infiltration of molten carbonate are on the order of 10{sup -6} and 10{sup -10} moles/m{sup 2} {center_dot} Pa {center_dot} s respectively, indicating that the molten carbonate is able to sufficiently infiltrate the membrane. It was found that La{sub 0.6}Sr{sub 0.4}Co{sub 0.8}Fe{sub 0.2}O{sub 3-{delta}} (LSCF) was a suitable candidate for the support

  4. Life cycle assessment of CO2 capture and utilization: a tutorial review.

    PubMed

    von der Assen, Niklas; Voll, Philip; Peters, Martina; Bardow, André

    2014-12-07

    Capturing CO2 and using it as an alternative carbon feedstock for chemicals, fuels and materials has the potential to reduce both CO2 emissions and fossil resource depletion. To assess the actual environmental benefits of CO2 capture and utilization (CCU), life cycle assessment (LCA) is considered as suitable metric. To enhance the use of LCA of CCU, this tutorial review gives a jargon-free introduction of LCA of CCU directed at LCA novices. Nine particularly important aspects for conducting an LCA of CCU are identified and illustrated with CCU examples. These aspects, phrased as action items, can serve LCA novices as a checklist through all steps in LCA of CCU: from defining the LCA purpose and the system boundaries, over data collection and environmental impact computation, to interpretation and sensitivity analysis of the results. Finally, in the context of CCU, an outlook is given on recent developments in LCA that aim to cover all pillars of sustainability (people, planet, and profit).

  5. Density functional theory study of CO2 capture with transition metal oxides and hydroxides

    NASA Astrophysics Data System (ADS)

    Zhang, Bo; Duan, Yuhua; Johnson, Karl

    2012-02-01

    We have used density functional theory (DFT) employing several different exchange-correlation functionals (PW91, PBE, PBEsol, TPSS, and revTPSS) coupled with lattice dynamics calculations to compute the thermodynamics of CO2 absorption/desorption reactions for selected transition metal oxides, (TMO), and hydroxides, TM(OH)2, where TM = Mn, Ni, Zn, and Cd. The van't Hoff plots, which describe the reaction equilibrium as a function of the partial pressures of CO2 and H2O as well as temperature, were computed from DFT total energies, complemented by the free energy contribution of solids and gases from lattice dynamics and statistical mechanics, respectively. We find that the PBEsol functional calculations are generally in better agreement with experimental phase equilibrium data compared with the other functionals we tested. In contrast, the formation enthalpies of the compounds are better computed with the TPSS and revTPSS functionals. The PBEsol functional gives better equilibrium properties due to a partial cancellation of errors in the enthalpies of formation. We have identified all CO2 capture reactions that lie on the Gibbs free energy convex hull as a function of temperature and the partial pressures of CO2 and H2O for all TMO and TM(OH)2 systems studied here.

  6. Sequestration of CO2 discharged from anode by algal cathode in microbial carbon capture cells (MCCs).

    PubMed

    Wang, Xin; Feng, Yujie; Liu, Jia; Lee, He; Li, Chao; Li, Nan; Ren, Nanqi

    2010-08-15

    Due to increased discharge of CO(2) is incurring problems, CO(2) sequestration technologies require substantial development. By introducing anodic off gas into an algae grown cathode (Chlorella vulgaris), new microbial carbon capture cells (MCCs) were constructed and demonstrated here to be an effective technology for CO(2) emission reduction with simultaneous voltage output without aeration (610+/-50 mV, 1000 Omega). Maximum power densities increased from 4.1 to 5.6 W/m(3) when the optical density (OD) of cathodic algae suspension increased from 0.21 to 0.85 (658 nm). Compared to a stable voltage of 706+/-21 mV (1000 Omega) obtained with cathodic dissolved oxygen (DO) of 6.6+/-1.0 mg/L in MCC, voltage outputs decreased from 654 to 189 mV over 70 h in the control reactor (no algae) accompanied with a decrease in DO from 7.6 to 0.9 mg/L, indicating that cathode electron acceptor was oxygen. Gas analysis showed that all the CO(2) generated from anode was completely eliminated by catholyte, and the soluble inorganic carbon was further converted into algal biomass. These results showed the possibility of a new method for simultaneous carbon fixing, power generation and biodiesel production during wastewater treatment without aeration.

  7. Capture and conversion of CO2 at ambient conditions by a conjugated microporous polymer

    PubMed Central

    Xie, Yong; Wang, Ting-Ting; Liu, Xiao-Huan; Zou, Kun; Deng, Wei-Qiao

    2013-01-01

    Conjugated microporous polymers are a new class of porous materials with an extended π-conjugation in an amorphous organic framework. Owing to the wide-ranging flexibility in the choice and design of components and the available control of pore parameters, these polymers can be tailored for use in various applications, such as gas storage, electronics and catalysis. Here we report a class of cobalt/aluminium-coordinated conjugated microporous polymers that exhibit outstanding CO2 capture and conversion performance at atmospheric pressure and room temperature. These polymers can store CO2 with adsorption capacities comparable to metal-organic frameworks. The cobalt-coordinated conjugated microporous polymers can also simultaneously function as heterogeneous catalysts for the reaction of CO2 and propylene oxide at atmospheric pressure and room temperature, wherein the polymers demonstrate better efficiency than a homogeneous salen-cobalt catalyst. By combining the functions of gas storage and catalysts, this strategy provides a direction for cost-effective CO2 reduction processes. PMID:23727768

  8. H2CO3(s): a new candidate for CO2 capture and sequestration.

    PubMed

    Tossell, J A

    2009-04-01

    To reduce the magnitude of anthropogenic global warming it is necessary to remove CO2(g) from the effluent streams of coal-fired power plants and to sequester the CO2 either as a liquid or by reaction with other compounds. A major difficulty in achieving this goal arises from the very weak acidity of CO2(g), causing it to react only incompletely with weak bases, although this weak interaction does provide a means for "stripping" the CO2 from the acid-base complex at high temperatures. Reaction with strong bases like Na0H yields more stable complexes, but massive amounts of chemical reactants would need to be purchased and chemical products like NaHCO3 then stored. However, when gas-phase CO2 reacts with the weak base water (or when bicarbonate reacts with strong acid) the unstable product monomeric "H2CO3" can be formed. The free energy required is about 16 kcal/mol in the gas phase and about 10 kcal/mol in aqueous solution. This energy can be supplied by particle or photon excitation and is only a small fraction ofthe energy released when a mole of CH4 is converted to a mole of CO2. Although this monomeric compound is highly unstable, its oligomers are considerably more stable, due to internal H-bonding, with free energies for the larger oligomers in the gas phase which are about 4 kcal/(mol of H2CO3) lower, only about 6 kcal/mol H2CO3 higher than the gas-phase combination of CO2 and H2O at room temperature. Also, at lower temperature the entropic penalty for the oligomer is less and oligomeric H2CO3 becomes stable around the sublimation temperature of dry ice. This indicates that it may be possible to capture gas-phase CO2 directly, using only cheap and abundant H2O as a reactant, and to store the resulting (H2CO3)n as a oligomeric solid at only moderately cold temperatures. These conclusions are based on quantum computations that accurately reproduce the structures, spectra, and stabilities of H2CO3 oligomers. Methods for producing and characterizing the H2CO3

  9. Dual Phase Membrane for High Temperature CO2 Separation

    SciTech Connect

    Jerry Y.S. Lin; Matthew Anderson

    2006-09-29

    Dual-phase membranes consisting of stainless steel supports infiltrated with molten carbonate have been shown to be selective to CO{sub 2} at high temperatures (400-650 C). However, over time at high temperatures, the formation of iron oxides on the surface of the stainless steel supports render the membranes ineffective. This report details synthesis and characteristics of dual-phase carbonate membrane with an oxidation resistant perovskite type ceramic (lanthanum-strontium-cobaltite-iron; LSCF) support. Porous LSCF supports were prepared from its powder synthesized by the citrate method. Both steady state permeation and mercury porosimetry confirmed that the LSCF membrane sintered at 900 C has pores large enough to absorb molten carbonate, yet small enough to retain the molten carbonate under high pressure conditions. Results of XRD analysis have shown that LSCF and the molten carbonate mixture do not react with each other at temperatures below 700 C. Four-point method conductivity tests indicate that the support material has sufficiently high electronic conductivity for this application. Li-Na-K carbonate was coated to the porous LSCF support by a liquid infiltration method. Helium permeance of the support before and after infiltration of molten carbonate are on the order of 10{sup -6} and 10{sup -10} moles/m{sup 2} {center_dot} Pa {center_dot} s respectively, indicating that the molten carbonate is able to sufficiently infiltrate the membrane. Preliminary high temperature permeation experiments indicate that the membrane does separate CO{sub 2} in the presence of O{sub 2}, with a maximum flux of 0.623 ml/cm{sup 2} {center_dot} min obtained at 850 C.

  10. Tailoring metal-organic frameworks for CO2 capture: the amino effect.

    PubMed

    Vitillo, Jenny G; Savonnet, Marie; Ricchiardi, Gabriele; Bordiga, Silvia

    2011-09-19

    Carbon dioxide capture from processes is one of the strategies adopted to decrease anthropogenic greenhouse gas emissions. To lower the cost associated with the regeneration of amine-based scrubber systems, one of the envisaged strategies is the grafting of amines onto high-surface-area supports and, in particular, onto metal-organic frameworks (MOFs). In this study, the interaction between CO(2) and aliphatic and aromatic amines has been characterized by quantum mechanical methods (MP2), focusing attention both on species already reported in MOFs and on new amine-based linkers, to inspire the rational synthesis of new high-capacity MOFs. The calculations highlight binding-site requisites and indicate that CO(2) vibrations are independent of the adsorption energy and monitoring them in probe-molecule experiments is not a suitable marker of efficient adsorption.

  11. Efficient and Energy-Saving CO2 Capture through the Entropic Effect Induced by the Intermolecular Hydrogen Bonding in Anion-Functionalized Ionic Liquids.

    PubMed

    Luo, Xiao Y; Ding, Fang; Lin, Wen J; Qi, Yu Q; Li, Hao R; Wang, Cong M

    2014-01-16

    A strategy for improving the capture of CO2 was developed through the entropic effect by tuning the geometric construction of anion-functionalized ionic liquids. Several kinds of anion-functionalized ionic liquids with the amino group at the para or ortho position were designed and applied for the capture of CO2, which indicates that the former exhibited both higher capacity and lower enthalpy, resulting in the efficient and energy-saving CO2 capture. Viscosity measurements, spectroscopic investigations, and quantum chemical calculations showed that such a unique behavior originated from the entropic effect, which was induced by the intermolecular hydrogen bonding in these ionic liquids. The entropic control for gas separation developed by this work provides an efficient strategy to both increased capacity and reduced enthalpy.

  12. DUAL PHASE MEMBRANE FOR HIGH TEMPERATURE CO2 SEPARATION

    SciTech Connect

    Jerry Y.S. Lin; Seungjoon Chung; Matthew Anderson

    2005-12-01

    This project is intended to expand upon the previous year's research en route to the development of a sustainable dual phase membrane for CO{sub 2} separation. It was found that the pores within the supports had to be less than 9 {micro}m in order to maintain the stability of the dual phase membrane. Pores larger than 9 {micro}m would be unable to hold the molten carbonate phase in place, rendering the membrane ineffective. Calculations show that 80% of the pore volume of the 0.5 media grade metal support was filled with the molten carbonate. Information obtained from EDS and SEM confirmed that the molten carbonate completely infiltrated the pores on both the contact and non-contact size of the metal support. Permeation tests for CO{sub 2} and N{sub 2} at 450-750 C show very low permeance of those two gases through the dual phase membrane, which was expected due to the lack of ionization of those two gases. Permeance of the CO{sub 2} and O{sub 2} mixture was much higher, indicating that the gases do form an ionic species, CO{sub 3}{sup 2-}, enhancing transport through the membrane. However, at temperatures in excess of 650 C, the permeance of CO{sub 3}{sup 2-} decreased quite rapidly, while predictions showed that permeance should have continued to increase. XRD data obtained form the surface of the membrane indicated the formation of lithium iron oxides on the support. This layer has a very low conductivity, which drastically reduces the flow of electrons to the CO{sub 2}/O{sub 2} gas mixture, limiting the formation of the ionic species. These results indicate that the use of stainless steel supports in a high temperature oxidative environment can lead to decreased performance of the membranes. This revelation has created the need for an oxidation resistant support, which can be gained by the use of a ceramic-type membrane. Future research efforts will be directed towards preparation of a new ceramic-carbonate dual phase membrane. The membrane will based on an

  13. Dual Phase Membrane for High temperature CO2 Separation

    SciTech Connect

    Jerry Y.S. Lin; Matthew Anderson

    2005-12-01

    Research in the previous years in this project found that stainless steel supports are oxidized during high temperature, dual phase membrane separation of carbon dioxide (with oxygen). Consequently, a new material has been sought to alleviate the problems with oxidation. Lanthanum cobaltite oxide is a suitable candidate for the support material in the dual phase membrane due to its oxidation resistance and electronic conductivity. Porous lanthanum cobaltite membranes were prepared via the citrate method, using nitrate metal precursors as the source of La, Sr, Co and Fe. The material was prepared and ground into a powder, which was subsequently pressed into disks for sintering at 900 C. Conductivity measurements were evaluated using the four-probe DC method. Support pore size was determined by helium permeation. Conductivity of the lanthanum cobaltite material was found to be at a maximum of 0.1856 S/cm at 550 C. The helium permeance of the lanthanum cobaltite membranes for this research was on the order of 10{sup -6} moles/m{sup 2} {center_dot} Pa {center_dot} s, proving that the membranes are porous after sintering at 900 C. The average pore size based on steady state helium permeance measurements was found to be between 0.37 and 0.57 {micro}m. The lanthanum cobaltite membranes have shown to have desired porosity, pore size and electric conductivity as the support for the dual-phase membranes. Molten carbonate was infiltrated to the pores of lanthanum cobaltite membranes support. After infiltration with molten carbonate, the helium permeance of the membranes decreased by three orders of magnitude to 10{sup -9} moles/m{sup 2} {center_dot} Pa {center_dot} s. This number, however, is one order of magnitude larger than the room temperate permeance of the stainless steel supports after infiltration with molten carbonate. Optimization of the dip coating process with molten carbonate will be evaluated to determine if lower permeance values can be obtained with the

  14. A Fine-Tuned Fluorinated MOF Addresses the Needs for Trace CO2 Removal and Air Capture Using Physisorption.

    PubMed

    Bhatt, Prashant M; Belmabkhout, Youssef; Cadiau, Amandine; Adil, Karim; Shekhah, Osama; Shkurenko, Aleksander; Barbour, Leonard J; Eddaoudi, Mohamed

    2016-07-27

    The development of functional solid-state materials for carbon capture at low carbon dioxide (CO2) concentrations, namely, from confined spaces (<0.5%) and in particular from air (400 ppm), is of prime importance with respect to energy and environment sustainability. Herein, we report the deliberate construction of a hydrolytically stable fluorinated metal-organic framework (MOF), NbOFFIVE-1-Ni, with the appropriate pore system (size, shape, and functionality), ideal for the effective and energy-efficient removal of trace carbon dioxide. Markedly, the CO2-selective NbOFFIVE-1-Ni exhibits the highest CO2 gravimetric and volumetric uptake (ca. 1.3 mmol/g and 51.4 cm(3) (STP) cm(-3)) for a physical adsorbent at 400 ppm of CO2 and 298 K. Practically, NbOFFIVE-1-Ni offers the complete CO2 desorption at 328 K under vacuum with an associated moderate energy input of 54 kJ/mol, typical for the full CO2 desorption in conventional physical adsorbents but considerably lower than chemical sorbents. Noticeably, the contracted square-like channels, affording the close proximity of the fluorine centers, permitted the enhancement of the CO2-framework interactions and subsequently the attainment of an unprecedented CO2 selectivity at very low CO2 concentrations. The precise localization of the adsorbed CO2 at the vicinity of the periodically aligned fluorine centers, promoting the selective adsorption of CO2, is evidenced by the single-crystal X-ray diffraction study on NbOFFIVE-1-Ni hosting CO2 molecules. Cyclic CO2/N2 mixed-gas column breakthrough experiments under dry and humid conditions corroborate the excellent CO2 selectivity under practical carbon capture conditions. Pertinently, the notable hydrolytic stability positions NbOFFIVE-1-Ni as the new benchmark adsorbent for direct air capture and CO2 removal from confined spaces.

  15. Commerical-Scale CO2 Capture and Sequestration for the Cement Industry

    SciTech Connect

    Adolfo Garza

    2010-07-28

    On June 8, 2009, DOE issued Funding Opportunity Announcement (FOA) Number DE-FOA-000015 seeking proposals to capture and sequester carbon dioxide from industrial sources. This FOA called for what was essentially a two-tier selection process. A number of projects would receive awards to conduct front-end engineering and design (FEED) studies as Phase I. Those project sponsors selected would be required to apply for Phase II, which would be the full design, construction, and operation of their proposed technology. Over forty proposals were received, and ten were awarded Phase I Cooperative Agreements. One of those proposers was CEMEX. CEMEX proposed to capture and sequester carbon dioxide (CO2) from one of their existing cement plants and either sequester the CO2 in a geologic formation or use it for enhanced oil recovery. The project consisted of evaluating their plants to identify the plant best suited for the demonstration, identify the best available capture technology, and prepare a design basis. The project also included evaluation of the storage or sequestration options in the vicinity of the selected plant.

  16. Computational Discovery of Metal-Organic Frameworks for CO2 Capture and Energy Storage

    NASA Astrophysics Data System (ADS)

    Siegel, Donald

    2015-03-01

    Because of their high surface areas, crystallinity, and tunable properties, metal -organic frameworks (MOFs) have attracted intense interest as materials for gas capture and energy storage. An often-cited benefit of MOFs is their large number of possible structures and compositions. Nevertheless, this design flexibility also has drawbacks, as pinpointing optimal compounds from thousands of candidates can be time consuming and costly using experimental approaches. Consequently, computational approaches are garnering increasing importance as a means to accelerate the discovery of high-performing MOFs. Here we combine several computational techniques to identify promising MOFs for CO2 capture and the storage of gaseous fuels (methane and hydrogen). The techniques include: (i) high-throughput screening based on data-mining and empirical correlations; (ii) Monte Carlo simulations based on quantum-mechanically-informed forcefields; and (iii) first-principles calculations of thermodynamics and electronic structure. For CO2 capture and CH4 storage, these techniques are used to explore metal-substituted variants of M-DOBDC and M-HKUST-1. In the case of H2, we identify trends and promising adsorbents amongst 4,000 compounds mined from the Cambridge Structure Database.

  17. Low transition temperature mixtures as innovative and sustainable CO2 capture solvents.

    PubMed

    Zubeir, Lawien F; Lacroix, Mark H M; Kroon, Maaike C

    2014-12-11

    The potential of three newly discovered low transition temperature mixtures (LTTMs) is explored as sustainable substituents for the traditional carbon dioxide (CO2) absorbents. LTTMs are mixtures of two solid compounds, a hydrogen bond donor (HBD) and a hydrogen bond acceptor (HBA), which form liquids upon mixing with melting points far below those of the individual compounds. In this work the HBD is lactic acid and the HBAs are tetramethylammonium chloride, tetraethylammonium chloride, and tetrabutylammonium chloride. These compounds were found to form LTTMs for the first time at molar ratios of HBD:HBA = 2:1. First, the LTTMs were characterized by determining the thermal operating window (e.g., decomposition temperature and glass transition temperature) and the physical properties (e.g., density and viscosity). Thereafter, the phase behavior of CO2 with the LTTMs has been measured using a gravimetric magnetic suspension balance operating in the static mode at 308 and 318 K and pressures up to 2 MPa. The CO2 solubility increased with increasing chain length, increasing pressure, and decreasing temperature. The Peng-Robinson equation of state was applied to correlate the phase equilibria. From the solubility data, thermodynamic parameters were determined (e.g., Henry's law coefficient and enthalpy of absorption). The heat of absorption was found to be similar to that in conventional physical solvents (-11.21 to -14.87 kJ·mol(-1)). Furthermore, the kinetics in terms of the diffusion coefficient of CO2 in all LTTMs were determined (10(-11)-10(-10) m(2)·s(-1)). Even though the CO2 solubilities in the studied LTTMs were found to be slightly lower than those in thoroughly studied conventional physical solvents, LTTMs are a promising new class of absorbents due to their low cost, their environmentally friendly character, and their easy tunability, allowing further optimization for carbon capture.

  18. CO2 hydrate formation and dissociation in cooled porous media: a potential technology for CO2 capture and storage.

    PubMed

    Yang, Mingjun; Song, Yongchen; Jiang, Lanlan; Zhu, Ningjun; Liu, Yu; Zhao, Yuechao; Dou, Binlin; Li, Qingping

    2013-09-03

    The purpose of this study was to investigate the hydrate formation and dissociation with CO2 flowing through cooled porous media at different flow rates, pressures, temperatures, and flow directions. CO2 hydrate saturation was quantified using the mean intensity of water. The experimental results showed that the hydrate block appeared frequently, and it could be avoided by stopping CO2 flooding early. Hydrate formed rapidly as the temperature was set to 274.15 or 275.15 K, but the hydrate formation delayed when it was 276.15 K. The flow rate was an important parameter for hydrate formation; a too high or too low rate was not suitable for CO2 hydration formation. A low operating pressure was also unacceptable. The gravity made hydrate form easily in the vertically upward flow direction. The pore water of the second cycle converted to hydrate more completely than that of the first cycle, which was a proof of the hydrate "memory effect". When the pressure was equal to atmospheric pressure, hydrate did not dissociate rapidly and abundantly, and a long time or reduplicate depressurization should be used in industrial application.

  19. The O2-assisted Al/CO2 electrochemical cell: A system for CO2 capture/conversion and electric power generation

    PubMed Central

    Al Sadat, Wajdi I.; Archer, Lynden A.

    2016-01-01

    Economical and efficient carbon capture, utilization, and sequestration technologies are a requirement for successful implementation of global action plans to reduce carbon emissions and to mitigate climate change. These technologies are also essential for longer-term use of fossil fuels while reducing the associated carbon footprint. We demonstrate an O2-assisted Al/CO2 electrochemical cell as a new approach to sequester CO2 emissions and, at the same time, to generate substantial amounts of electrical energy. We report on the fundamental principles that guide operations of these cells using multiple intrusive electrochemical and physical analytical methods, including chronopotentiometry, cyclic voltammetry, direct analysis in real-time mass spectrometry, energy-dispersive x-ray spectroscopy, x-ray photoelectron spectroscopy, and coupled thermogravimetric analysis–Fourier transform infrared spectroscopy. On this basis, we demonstrate that an electrochemical cell that uses metallic aluminum as anode and a carbon dioxide/oxygen gas mixture as the active material in the cathode provides a path toward electrochemical generation of a valuable (C2) species and electrical energy. Specifically, we show that the cell first reduces O2 at the cathode to form superoxide intermediates. Chemical reaction of the superoxide with CO2 sequesters the CO2 in the form of aluminum oxalate, Al2(C2O4)3, as the dominant product. On the basis of an analysis of the overall CO2 footprint, which considers emissions associated with the production of the aluminum anode and the CO2 captured/abated by the Al/CO2-O2 electrochemical cell, we conclude that the proposed process offers an important strategy for net reduction of CO2 emissions. PMID:27453949

  20. The O2-assisted Al/CO2 electrochemical cell: A system for CO2 capture/conversion and electric power generation.

    PubMed

    Al Sadat, Wajdi I; Archer, Lynden A

    2016-07-01

    Economical and efficient carbon capture, utilization, and sequestration technologies are a requirement for successful implementation of global action plans to reduce carbon emissions and to mitigate climate change. These technologies are also essential for longer-term use of fossil fuels while reducing the associated carbon footprint. We demonstrate an O2-assisted Al/CO2 electrochemical cell as a new approach to sequester CO2 emissions and, at the same time, to generate substantial amounts of electrical energy. We report on the fundamental principles that guide operations of these cells using multiple intrusive electrochemical and physical analytical methods, including chronopotentiometry, cyclic voltammetry, direct analysis in real-time mass spectrometry, energy-dispersive x-ray spectroscopy, x-ray photoelectron spectroscopy, and coupled thermogravimetric analysis-Fourier transform infrared spectroscopy. On this basis, we demonstrate that an electrochemical cell that uses metallic aluminum as anode and a carbon dioxide/oxygen gas mixture as the active material in the cathode provides a path toward electrochemical generation of a valuable (C2) species and electrical energy. Specifically, we show that the cell first reduces O2 at the cathode to form superoxide intermediates. Chemical reaction of the superoxide with CO2 sequesters the CO2 in the form of aluminum oxalate, Al2(C2O4)3, as the dominant product. On the basis of an analysis of the overall CO2 footprint, which considers emissions associated with the production of the aluminum anode and the CO2 captured/abated by the Al/CO2-O2 electrochemical cell, we conclude that the proposed process offers an important strategy for net reduction of CO2 emissions.

  1. Isotope separation by photoselective dissociative electron capture

    DOEpatents

    Stevens, Charles G. [Pleasanton, CA

    1978-08-29

    A method of separating isotopes based on photoselective electron capture dissociation of molecules having an electron capture cross section dependence on the vibrational state of the molecule. A molecular isotope source material is irradiated to selectively excite those molecules containing a desired isotope to a predetermined vibrational state having associated therewith an electron capture energy region substantially non-overlapping with the electron capture energy ranges associated with the lowest vibration states of the molecules. The isotope source is also subjected to electrons having an energy corresponding to the non-overlapping electron capture region whereby the selectively excited molecules preferentially capture electrons and dissociate into negative ions and neutrals. The desired isotope may be in the negative ion product or in the neutral product depending upon the mechanism of dissociation of the particular isotope source used. The dissociation product enriched in the desired isotope is then separated from the reaction system by conventional means. Specifically, .sup.235 UF.sub.6 is separated from a UF.sub.6 mixture by selective excitation followed by dissociative electron capture into .sup.235 UF.sub.5 - and F.

  2. Isotope separation by photoselective dissociative electron capture

    DOEpatents

    Stevens, C.G.

    1978-08-29

    Disclosed is a method of separating isotopes based on photoselective electron capture dissociation of molecules having an electron capture cross section dependence on the vibrational state of the molecule. A molecular isotope source material is irradiated to selectively excite those molecules containing a desired isotope to a predetermined vibrational state having associated therewith an electron capture energy region substantially non-overlapping with the electron capture energy ranges associated with the lowest vibration states of the molecules. The isotope source is also subjected to electrons having an energy corresponding to the non-overlapping electron capture region whereby the selectively excited molecules preferentially capture electrons and dissociate into negative ions and neutrals. The desired isotope may be in the negative ion product or in the neutral product depending upon the mechanism of dissociation of the particular isotope source used. The dissociation product enriched in the desired isotope is then separated from the reaction system by conventional means. Specifically, [sup 235]UF[sub 6] is separated from a UF[sub 6] mixture by selective excitation followed by dissociative electron capture into [sup 235]UF[sub 5]- and F. 2 figs.

  3. Integrated Cryogenic System for CO2 Separation and Lng Production from Landfill Gas

    NASA Astrophysics Data System (ADS)

    Chang, H. M.; Chung, M. J.; Park, S. B.

    2010-04-01

    An integrated cryogenic system to separate carbon dioxide (CO2) and produce LNG from landfill gas is investigated and designed. The main objective of this design is to eliminate the requirement of a standard CO2 removal process in the liquefaction system such distillation or (temperature or pressure) swing adsorption, and to directly separate carbon dioxide as frost at the liquefying channel of methane. Two identical sets of heat exchangers are installed in parallel and switched alternatively with a time period so that one is in separation-liquefaction mode while the other is in CO2 clean-up mode. A thermal regeneration scheme is presented for the purpose of saving energy and avoiding the stoppage of LNG production followed by the flow switching. The switching period is determined from results of a combined heat and mass transfer analysis on the CO2 freeze-out process.

  4. The incorporation of graphene oxide into polysulfone mixed matrix membrane for CO2/CH4 separation

    NASA Astrophysics Data System (ADS)

    Zahri, K.; Goh, P. S.; Ismail, A. F.

    2016-06-01

    Carbon dioxide (CO2) is often found as the main impurity in natural gas, where methane (CH4) is the major component. The presence of CO2 in natural gas leads to several problems such as reducing the energy content of natural gas and cause pipeline corrosion. Thus it must be removed to meet specifications (CO2 ≤ 2 mol%) before the gas can be delivered to the pipeline. In this work, hollow fiber mixed matrix membrane (MMM) were fabricated by embedding graphene oxide (GO) into a polysulfone (PSf) polymer matrix to improve membrane properties as well as its separation performance towards CO2/CH4 gas. The membrane properties were investigated for pristine membrane and mixed matrix membrane filled with filler loading of 0.25%. The synthesized GO and properties of fabricated membranes were characterized and studied using TEM, AFM, XRD, FTIR and SEM respectively. The permeance of pure gases and ideal selectivity of CO2/CH4 gas were determined using pure gas permeation experiment. GO has affinity towards CO2 gas. The nanosheet structure creates path for small molecule gas and restricted large molecule gas to pass through the membrane. The incorporation of GO in PSf polymer enhanced the permeance of CO 2 and CO2/CH4 separation from 64.47 to 86.80 GPU and from 19 to 25 respectively.

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

    NASA Astrophysics Data System (ADS)

    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

  6. Jumpstarting commercial-scale CO2 capture and storage with ethylene production and enhanced oil recovery in the US Gulf

    DOE PAGES

    Middleton, Richard S.; Levine, Jonathan S.; Bielicki, Jeffrey M.; ...

    2015-04-27

    CO2 capture, utilization, and storage (CCUS) technology has yet to be widely deployed at a commercial scale despite multiple high-profile demonstration projects. We suggest that developing a large-scale, visible, and financially viable CCUS network could potentially overcome many barriers to deployment and jumpstart commercial-scale CCUS. To date, substantial effort has focused on technology development to reduce the costs of CO2 capture from coal-fired power plants. Here, we propose that near-term investment could focus on implementing CO2 capture on facilities that produce high-value chemicals/products. These facilities can absorb the expected impact of the marginal increase in the cost of production onmore » the price of their product, due to the addition of CO2 capture, more than coal-fired power plants. A financially viable demonstration of a large-scale CCUS network requires offsetting the costs of CO2 capture by using the CO2 as an input to the production of market-viable products. As a result, we demonstrate this alternative development path with the example of an integrated CCUS system where CO2 is captured from ethylene producers and used for enhanced oil recovery in the U.S. Gulf Coast region.« less

  7. Mars Atmospheric Capture and Gas Separation

    NASA Technical Reports Server (NTRS)

    Muscatello, Anthony; Santiago-Maldonado, Edgardo; Gibson, Tracy; Devor, Robert; Captain, James

    2011-01-01

    The Mars atmospheric capture and gas separation project is selecting, developing, and demonstrating techniques to capture and purify Martian atmospheric gases for their utilization for the production of hydrocarbons, oxygen, and water in ISRU systems. Trace gases will be required to be separated from Martian atmospheric gases to provide pure C02 to processing elements. In addition, other Martian gases, such as nitrogen and argon, occur in concentrations high enough to be useful as buffer gas and should be captured as welL To achieve these goals, highly efficient gas separation processes will be required. These gas separation techniques are also required across various areas within the ISRU project to support various consumable production processes. The development of innovative gas separation techniques will evaluate the current state-of-the-art for the gas separation required, with the objective to demonstrate and develop light-weight, low-power methods for gas separation. Gas separation requirements include, but are not limited to the selective separation of: (1) methane and water from un-reacted carbon oxides (C02- CO) and hydrogen typical of a Sabatier-type process, (2) carbon oxides and water from unreacted hydrogen from a Reverse Water-Gas Shift process, (3) carbon oxides from oxygen from a trash/waste processing reaction, and (4) helium from hydrogen or oxygen from a propellant scavenging process. Potential technologies for the separations include freezers, selective membranes, selective solvents, polymeric sorbents, zeolites, and new technologies. This paper and presentation will summarize the results of an extensive literature review and laboratory evaluations of candidate technologies for the capture and separation of C02 and other relevant gases.

  8. Molecular simulation studies of CO2 adsorption by carbon model compounds for carbon capture and sequestration applications.

    PubMed

    Liu, Yangyang; Wilcox, Jennifer

    2013-01-02

    Effects of oxygen-containing surface functionalities on the adsorption of mixtures including CO(2)/CH(4), CO(2)/N(2), and CO(2)/H(2)O have been investigated in the current work. Together with Bader charge analysis, electronic structure calculations have provided the initial framework comprising both the geometry and corresponding charge information required to carry out statistical-based molecular simulations. The adsorption isotherms and selectivity of CO(2) from CO(2)/N(2), CO(2)/CH(4), and CO(2)/H(2)O gas mixtures were determined by grand canonical Monte Carlo simulations at temperature/pressure conditions relevant to carbon capture and sequestration applications. The interactions between the surfaces with induced polarity and nonpolar/polar molecules have been investigated. It has been observed that, due to the induced polarity of the surface functionalization, the selectivity of CO(2) over CH(4) increases from approximately 2 to higher than 5, and the selectivity of CO(2) over N(2) increases from approximately 5 to 20, especially in the low-pressure regime. However, water vapor will always preferentially adsorb over CO(2) in carbon-based systems containing oxygen functionalized surfaces at conditions relevant to carbon capture application. Molecular simulation results indicate that the surface chemistry in micropores is tunable thereby influencing the selectivity for enhanced uptake of CO(2).

  9. In silico discovery of metal-organic frameworks for precombustion CO2 capture using a genetic algorithm

    PubMed Central

    Chung, Yongchul G.; Gómez-Gualdrón, Diego A.; Li, Peng; Leperi, Karson T.; Deria, Pravas; Zhang, Hongda; Vermeulen, Nicolaas A.; Stoddart, J. Fraser; You, Fengqi; Hupp, Joseph T.; Farha, Omar K.; Snurr, Randall Q.

    2016-01-01

    Discovery of new adsorbent materials with a high CO2 working capacity could help reduce CO2 emissions from newly commissioned power plants using precombustion carbon capture. High-throughput computational screening efforts can accelerate the discovery of new adsorbents but sometimes require significant computational resources to explore the large space of possible materials. We report the in silico discovery of high-performing adsorbents for precombustion CO2 capture by applying a genetic algorithm to efficiently search a large database of metal-organic frameworks (MOFs) for top candidates. High-performing MOFs identified from the in silico search were synthesized and activated and show a high CO2 working capacity and a high CO2/H2 selectivity. One of the synthesized MOFs shows a higher CO2 working capacity than any MOF reported in the literature under the operating conditions investigated here. PMID:27757420

  10. In silico discovery of metal-organic frameworks for precombustion CO2 capture using a genetic algorithm.

    PubMed

    Chung, Yongchul G; Gómez-Gualdrón, Diego A; Li, Peng; Leperi, Karson T; Deria, Pravas; Zhang, Hongda; Vermeulen, Nicolaas A; Stoddart, J Fraser; You, Fengqi; Hupp, Joseph T; Farha, Omar K; Snurr, Randall Q

    2016-10-01

    Discovery of new adsorbent materials with a high CO2 working capacity could help reduce CO2 emissions from newly commissioned power plants using precombustion carbon capture. High-throughput computational screening efforts can accelerate the discovery of new adsorbents but sometimes require significant computational resources to explore the large space of possible materials. We report the in silico discovery of high-performing adsorbents for precombustion CO2 capture by applying a genetic algorithm to efficiently search a large database of metal-organic frameworks (MOFs) for top candidates. High-performing MOFs identified from the in silico search were synthesized and activated and show a high CO2 working capacity and a high CO2/H2 selectivity. One of the synthesized MOFs shows a higher CO2 working capacity than any MOF reported in the literature under the operating conditions investigated here.

  11. Efficient CO2 Capture by Porous, Nitrogen-Doped Carbonaceous Adsorbents Derived from Task-Specific Ionic Liquids

    SciTech Connect

    Zhu, X; Hillesheim, PC; Mahurin, SM; Wang, CM; Tian, CC; Brown, S; Luo, HM; Veith, GM; Han, KS; Hagaman, EW; Liu, HL; Dai, S

    2012-08-21

    The search for a better carbon dioxide (CO2) capture material is attracting significant attention because of an increase in anthropogenic emissions. Porous materials are considered to be among the most promising candidates. A series of porous, nitrogen-doped carbons for CO2 capture have been developed by using high-yield carbonization reactions from task-specific ionic liquid (TSIL) precursors. Owing to strong interactions between the CO2 molecules and nitrogen-containing basic sites within the carbon framework, the porous nitrogen-doped compound derived from the carbonization of a TSIL at 500 degrees C, CN500, exhibits an exceptional CO2 absorption capacity of 193 mg of CO2 per g sorbent (4.39 mmol g(-1) at 0 degrees C and 1 bar), which demonstrates a significantly higher capacity than previously reported adsorbents. The application of TSILs as precursors for porous materials provides a new avenue for the development of improved materials for carbon capture.

  12. Pilot plant test of the advanced flash stripper for CO2 capture.

    PubMed

    Lin, Yu-Jeng; Chen, Eric; Rochelle, Gary T

    2016-10-20

    Alternative stripping processes have been proposed to reduce energy use for CO2 capture, but only a few have been applied to pilot-scale experiments. This paper presents the first pilot plant test results of one of the most promising stripper configurations, the advanced flash stripper with cold and warm rich solvent bypass. The campaign using aqueous piperazine was carried out at UT Austin in 2015. The advanced flash stripper improves the heat duty by over 25% compared to previous campaigns using the two-stage flash, achieving 2.1 GJ per tonne CO2 of heat duty and 32 kJ mol(-1) CO2 of total equivalent work. The bypass control strategy proposed minimized the heat duty. The test successfully demonstrated the remarkable energy performance and the operability of this advanced system. An Aspen Plus® model was validated using the pilot plant data and used to explore optimum operating and design conditions. The irreversibility analysis showed that the pilot plant performance has attained 50% thermodynamic efficiency and further energy improvement should focus on the absorber and the cross exchanger by increasing absorption rate and solvent capacity.

  13. Toward rational design of amines for CO2 capture: Substituent effect on kinetic process for the reaction of monoethanolamine with CO2.

    PubMed

    Xie, Hongbin; Wang, Pan; He, Ning; Yang, Xianhai; Chen, Jingwen

    2015-11-01

    Amines have been considered as promising candidates for post-combustion CO2 capture. A mechanistic understanding for the chemical processes involved in the capture and release of CO2 is important for the rational design of amines. In this study, the structural effects of amines on the kinetic competition among three typical products (carbamates, carbamic acids and bicarbonate) from amines+CO2 were investigated, in contrast to previous thermodynamic studies to tune the reaction of amines with CO2 based on desirable reaction enthalpy and reaction stoichiometry. We used a quantum chemical method to calculate the activation energies (Ea) for the reactions of a range of substituted monoethanolamines with CO2 covering three pathways to the three products. The results indicate that the formation of carbamates is the most favorable, among the three considered products. In addition, we found that the Ea values for all pathways linearly correlate with pKa of amines, and more importantly, the kinetic competition between carbamate and bicarbonate absorption pathways varies with pKa of the amines, i.e. stronger basicity results in less difference in Ea. These results highlight the importance of the consideration of kinetic competition among different reaction pathways in amine design.

  14. Kinetics of N-nitrosopiperazine formation from nitrite and piperazine in CO2 capture.

    PubMed

    Goldman, Mark J; Fine, Nathan A; Rochelle, Gary T

    2013-04-02

    Piperazine (PZ) is an efficient amine for carbon capture systems, but it can form N-nitrosopiperazine (MNPZ), a carcinogen, from nitrogen oxides (NO(x)) in flue gas from coal or natural gas combustion. The reaction of nitrite with PZ was studied in 0.1 to 5 mol/dm(3) PZ with 0.001 to 0.8 mol CO2/mol PZ at 50 to 135 °C. The reaction forming MNPZ is first order in nitrite, piperazine carbamate species, and hydronium ion. The activation energy is 84 ± 2 kJ/mol with a rate constant of 8.5 × 10(3) ± 1.4 × 10(3) dm(6) mol(-2) s(-1) at 100 °C. The proposed mechanism involves protonation of the carbamate species, nucleophilic attack of the carbamic acid, and formation of bicarbonate and MNPZ. These kinetics and mechanism will be useful in identifying inhibitors and other strategies to reduce nitrosamine accumulation in CO2 capture by scrubbing with PZ or other amines.

  15. Bench-Scale Testing and Process Performance Projections of CO2 Capture by CO2–Binding Organic Liquids (CO2BOLs) With and Without Polarity-Swing-Assisted Regeneration

    SciTech Connect

    Zheng, Feng; Heldebrant, David J.; Mathias, Paul M.; Koech, Phillip K.; Bhakta, Mukund; Freeman, Charles J.; Bearden, Mark D.; Zwoster, Andy

    2016-01-12

    This manuscript provides a detailed analysis of a continuous flow, bench scale study of the CO2BOL solvent platform with and without its Polarity Swing Assisted Regeneration (PSAR). This study encompassed four months of continuous flow testing of a candidate CO2BOL with a thermal regeneration and PSAR regeneration using decane antisolvent. In both regeneration schemes, steady state capture of >90 %CO2 was achieved using simulated flue gas at acceptable L/G ratios. Aspen Plus™ modeling was performed to assess process performance compared to previous equilibrium performance projections. This paper also includes net power projections, and comparisons to DOE’s Case 10 amine baseline.

  16. Development of a Dry Sorbent-based Post-Combustion CO2 Capture Technology for Retrofit in Existing Power Plants

    SciTech Connect

    Nelson, Thomas; Coleman, Luke; Anderson, Matthew; Gupta, Raghubir; Herr, Joshua; Kalluri, Ranjeeth; Pavani, Maruthi

    2009-12-31

    The objective of this research and development (R&D) project was to further the development of a solid sorbent-based CO2 capture process based on sodium carbonate (i.e. the Dry Carbonate Process) that is capable of capturing>90% of the CO2 as a nearly pure stream from coal-fired power plant flue gas with <35% increase in the cost of electrictiy (ICOE).

  17. tritium isotope separation by CO 2 laser-induced multiphoton dissociation of CTF 3

    NASA Astrophysics Data System (ADS)

    Makide, Yoshihiro; Hagiwara, Satoru; Tominaga, Takeshi; Takeuchi, Kazuo; Nakane, Ryohei

    1981-08-01

    Isotope separation of tritium at ppm concentration level was achieved by CO 2 laser-induced multiphoton dissociation of CTF 3 in CHF 3 with single-step separation factors exceeding 500. The effects of laser frequency, pulse energy, pulse duration, irradiation geometry, tritium concentration, sample pressure, and buffer gas were investigated.

  18. Technical and Energy Performance of an Advanced, Aqueous Ammonia-Based CO2 Capture Technology for a 500 MW Coal-Fired Power Station.

    PubMed

    Li, Kangkang; Yu, Hai; Feron, Paul; Tade, Moses; Wardhaugh, Leigh

    2015-08-18

    Using a rate-based model, we assessed the technical feasibility and energy performance of an advanced aqueous-ammonia-based postcombustion capture process integrated with a coal-fired power station. The capture process consists of three identical process trains in parallel, each containing a CO2 capture unit, an NH3 recycling unit, a water separation unit, and a CO2 compressor. A sensitivity study of important parameters, such as NH3 concentration, lean CO2 loading, and stripper pressure, was performed to minimize the energy consumption involved in the CO2 capture process. Process modifications of the rich-split process and the interheating process were investigated to further reduce the solvent regeneration energy. The integrated capture system was then evaluated in terms of the mass balance and the energy consumption of each unit. The results show that our advanced ammonia process is technically feasible and energy-competitive, with a low net power-plant efficiency penalty of 7.7%.

  19. A technical, economic, and environmental assessment of amine-based CO2 capture technology for power plant greenhouse gas control.

    PubMed

    Rao, Anand B; Rubin, Edward S

    2002-10-15

    Capture and sequestration of CO2 from fossil fuel power plants is gaining widespread interest as a potential method of controlling greenhouse gas emissions. Performance and cost models of an amine (MEA)-based CO2 absorption system for postcombustion flue gas applications have been developed and integrated with an existing power plant modeling framework that includes multipollutant control technologies for other regulated emissions. The integrated model has been applied to study the feasibility and cost of carbon capture and sequestration at both new and existing coal-burning power plants. The cost of carbon avoidance was shown to depend strongly on assumptions about the reference plant design, details of the CO2 capture system design, interactions with other pollution control systems, and method of CO2 storage. The CO2 avoidance cost for retrofit systems was found to be generally higher than for new plants, mainly because of the higher energy penalty resulting from less efficient heat integration as well as site-specific difficulties typically encountered in retrofit applications. For all cases, a small reduction in CO2 capture cost was afforded by the SO2 emission trading credits generated by amine-based capture systems. Efforts are underway to model a broader suite of carbon capture and sequestration technologies for more comprehensive assessments in the context of multipollutant environmental management.

  20. Aqueous Biphasic Systems for the Synthesis of Formates by Catalytic CO2 Hydrogenation: Integrated Reaction and Catalyst Separation for CO2 -Scrubbing Solutions.

    PubMed

    Scott, Martin; Blas Molinos, Beatriz; Westhues, Christian; Franciò, Giancarlo; Leitner, Walter

    2017-03-22

    Aqueous biphasic systems were investigated for the production of formate-amine adducts by metal-catalyzed CO2 hydrogenation, including typical scrubbing solutions as feedstocks. Different hydrophobic organic solvents and ionic liquids could be employed as the stationary phase for cis-[Ru(dppm)2 Cl2 ] (dppm=bis-diphenylphosphinomethane) as prototypical catalyst without any modification or tagging of the complex. The amines were found to partition between the two phases depending on their structure, whereas the formate-amine adducts were nearly quantitatively extracted into the aqueous phase, providing a favorable phase behavior for the envisaged integrated reaction/separation sequence. The solvent pair of methyl isobutyl carbinol (MIBC) and water led to the most practical and productive system and repeated use of the catalyst phase was demonstrated. The highest single batch activity with a TOFav of approximately 35 000 h(-1) and an initial TOF of approximately 180 000 h(-1) was achieved in the presence of NEt3 . Owing to higher stability, the highest productivities were obtained with methyl diethanolamine (Aminosol CST 115) and monoethanolamine (MEA), which are used in commercial scale CO2 -scrubbing processes. Saturated aqueous solutions (CO2 overpressure 5-10 bar) of MEA could be converted into the corresponding formate adducts with average turnover frequencies up to 14×10(3)  h(-1) with an overall yield of 70 % based on the amine, corresponding to a total turnover number of 150 000 over eleven recycling experiments. This opens the possibility for integrated approaches to carbon capture and utilization.

  1. Ionic liquid-based materials: a platform to design engineered CO2 separation membranes.

    PubMed

    Tomé, Liliana C; Marrucho, Isabel M

    2016-05-21

    During the past decade, significant advances in ionic liquid-based materials for the development of CO2 separation membranes have been accomplished. This review presents a perspective on different strategies that use ionic liquid-based materials as a unique tuneable platform to design task-specific advanced materials for CO2 separation membranes. Based on compilation and analysis of the data hitherto reported, we provide a judicious assessment of the CO2 separation efficiency of different membranes, and highlight breakthroughs and key challenges in this field. In particular, configurations such as supported ionic liquid membranes, polymer/ionic liquid composite membranes, gelled ionic liquid membranes and poly(ionic liquid)-based membranes are detailed, discussed and evaluated in terms of their efficiency, which is attributed to their chemical and structural features. Finally, an integrated perspective on technology, economy and sustainability is provided.

  2. In situ infrared study of the role of PEG in stabilizing silica-supported amines for CO(2) capture.

    PubMed

    Tanthana, Jak; Chuang, Steven S C

    2010-08-23

    The CO(2) capture capacity, adsorption mechanism, and degradation characteristics of two sorbents, silica-supported tetraethylenepentamine (TEPA/SiO(2)) and polyethylene-glycol-modified TEPA/SiO(2) (PEG/TEPA/SiO(2)), are studied by diffuse reflectance infrared Fourier transform spectroscopy and mass spectrometry. The CO(2) capture capacities of TEPA/SiO(2) and PEG/TEPA/SiO(2) are determined to be 2087 and 1110 micromol CO(2) g(-1) sorbent, respectively. Both sorbents adsorb CO(2) as hydrogen-bonding species, NH(2)--O, and carbamate/carboxylate species. The CO(2) adsorption half-time increases with the number of CO(2) capture cycles. Infrared results suggest that the increased adsorption half-time is a result of diffusion limitation, caused by accumulation of TEPA and PEG species on the surface of the sorbent particles. The degradation of TEPA/SiO(2) is found to correlate with the accumulation of carboxylate/carbamic species. The addition of PEG decreases the degradation rate of the sorbent and slows down the formation of carboxylate species. These carboxylate species can block CO(2) capture on amine (NH(2)/NH) sites. The stabilizing role of PEG on TEPA/SiO(2) can be attributed to hydrogen-bonding between TEPA (NH(2)/NH)and PEG (OH).

  3. CO2 capture using semi-clathrates of quaternary ammonium salt: structure change induced by CO2 and N2 enclathration.

    PubMed

    Chazallon, Bertrand; Ziskind, Michael; Carpentier, Yvain; Focsa, Cristian

    2014-11-26

    Semi-clathrates of tetrabutylammonium bromide (TBAB) are investigated for their potential application in the CO2 capture context based on hydrate technology. The three-phase lines of semi-clathrates of CO2-TBAB-H2O and N2-TBAB-H2O are established simultaneously with their structure using in situ Raman scattering performed at high pressure. The preferred crystal phase obtained at ambient pressure from solutions of 5 and 40 wt % TBAB initial concentrations is shown to change upon enclathration of CO2 or N2, or by applying a higher pressure on the system. Deep in the stability field, metastable hydrate phases are occurring at the onset of the formation and correspond to the ones expected under ambient pressure conditions. Depending on the pressure, they progressively transformed into the most stable ones when approaching equilibrium and dissociation points. Besides, it is shown that a 5 wt % TBAB original solution forms preferentially a mixed structure of both type B and type A at low gas pressure with CO2 as the guest gas. A new structure is spectroscopically characterized at pressures higher than ∼2 MPa CO2. Type A is demonstrated to be stable at 5 wt % initial TBAB concentration with N2 as the guest molecule and pressure between 8 and 12 MPa. These structural data address new insights on the relationship between the hydrophilic-anion and hydrophobic-cation intercalation with a guest gas producing hydrophobic interaction in a distorted water lattice.

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

    PubMed

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

    2017-03-22

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

  5. Coordination effect-regulated CO2 capture with an alkali metal onium salts/crown ether system

    SciTech Connect

    Yang, Zhen-Zhen; Jiang, Deen; Zhu, Xiang; Tian, Chengcheng; Brown, Suree; Do-Thanh, Chi-Linh; He, Liang-Nian; Dai, Sheng

    2014-01-01

    A coordination effect was employed to realize equimolar CO2 absorption, adopting easily synthesized amino group containing absorbents (alkali metal onium salts). The essence of our strategy was to increase the steric hindrance of cations so as to enhance a carbamic acid pathway for CO2 capture. Our easily synthesized alkali metal amino acid salts or phenolates were coordinated with crown ethers, in which highly sterically hindered cations were obtained through a strong coordination effect of crown ethers with alkali metal cations. For example, a CO2 capacity of 0.99 was attained by potassium prolinate/18-crown-6, being characterized by NMR, FT-IR, and quantum chemistry calculations to go through a carbamic acid formation pathway. The captured CO2 can be stripped under very mild conditions (50 degrees C, N-2). Thus, this protocol offers an alternative for the development of technological innovation towards efficient and low energy processes for carbon capture and sequestration.

  6. Opportunities for Decarbonizing Existing U.S. Coal-Fired Power Plants via CO2 Capture, Utilization and Storage.

    PubMed

    Zhai, Haibo; Ou, Yang; Rubin, Edward S

    2015-07-07

    This study employs a power plant modeling tool to explore the feasibility of reducing unit-level emission rates of CO2 by 30% by retrofitting carbon capture, utilization, and storage (CCUS) to existing U.S. coal-fired electric generating units (EGUs). Our goal is to identify feasible EGUs and their key attributes. The results indicate that for about 60 gigawatts of the existing coal-fired capacity, the implementation of partial CO2 capture appears feasible, though its cost is highly dependent on the unit characteristics and fuel prices. Auxiliary gas-fired boilers can be employed to power a carbon capture process without significant increases in the cost of electricity generation. A complementary CO2 emission trading program can provide additional economic incentives for the deployment of CCS with 90% CO2 capture. Selling and utilizing the captured CO2 product for enhanced oil recovery can further accelerate CCUS deployment and also help reinforce a CO2 emission trading market. These efforts would allow existing coal-fired EGUs to continue to provide a significant share of the U.S. electricity demand.

  7. Separating the influence of temperature, drought, and fire on interannual variability in atmospheric CO2.

    PubMed

    Keppel-Aleks, Gretchen; Wolf, Aaron S; Mu, Mingquan; Doney, Scott C; Morton, Douglas C; Kasibhatla, Prasad S; Miller, John B; Dlugokencky, Edward J; Randerson, James T

    2014-11-01

    The response of the carbon cycle in prognostic Earth system models (ESMs) contributes significant uncertainty to projections of global climate change. Quantifying contributions of known drivers of interannual variability in the growth rate of atmospheric carbon dioxide (CO2) is important for improving the representation of terrestrial ecosystem processes in these ESMs. Several recent studies have identified the temperature dependence of tropical net ecosystem exchange (NEE) as a primary driver of this variability by analyzing a single, globally averaged time series of CO2 anomalies. Here we examined how the temporal evolution of CO2 in different latitude bands may be used to separate contributions from temperature stress, drought stress, and fire emissions to CO2 variability. We developed atmospheric CO2 patterns from each of these mechanisms during 1997-2011 using an atmospheric transport model. NEE responses to temperature, NEE responses to drought, and fire emissions all contributed significantly to CO2 variability in each latitude band, suggesting that no single mechanism was the dominant driver. We found that the sum of drought and fire contributions to CO2 variability exceeded direct NEE responses to temperature in both the Northern and Southern Hemispheres. Additional sensitivity tests revealed that these contributions are masked by temporal and spatial smoothing of CO2 observations. Accounting for fires, the sensitivity of tropical NEE to temperature stress decreased by 25% to 2.9 ± 0.4 Pg C yr(-1) K(-1). These results underscore the need for accurate attribution of the drivers of CO2 variability prior to using contemporary observations to constrain long-term ESM responses.

  8. Separating the influence of temperature, drought, and fire on interannual variability in atmospheric CO2

    PubMed Central

    Keppel-Aleks, Gretchen; Wolf, Aaron S; Mu, Mingquan; Doney, Scott C; Morton, Douglas C; Kasibhatla, Prasad S; Miller, John B; Dlugokencky, Edward J; Randerson, James T

    2014-01-01

    The response of the carbon cycle in prognostic Earth system models (ESMs) contributes significant uncertainty to projections of global climate change. Quantifying contributions of known drivers of interannual variability in the growth rate of atmospheric carbon dioxide (CO2) is important for improving the representation of terrestrial ecosystem processes in these ESMs. Several recent studies have identified the temperature dependence of tropical net ecosystem exchange (NEE) as a primary driver of this variability by analyzing a single, globally averaged time series of CO2 anomalies. Here we examined how the temporal evolution of CO2 in different latitude bands may be used to separate contributions from temperature stress, drought stress, and fire emissions to CO2 variability. We developed atmospheric CO2 patterns from each of these mechanisms during 1997–2011 using an atmospheric transport model. NEE responses to temperature, NEE responses to drought, and fire emissions all contributed significantly to CO2 variability in each latitude band, suggesting that no single mechanism was the dominant driver. We found that the sum of drought and fire contributions to CO2 variability exceeded direct NEE responses to temperature in both the Northern and Southern Hemispheres. Additional sensitivity tests revealed that these contributions are masked by temporal and spatial smoothing of CO2 observations. Accounting for fires, the sensitivity of tropical NEE to temperature stress decreased by 25% to 2.9 ± 0.4 Pg C yr−1 K−1. These results underscore the need for accurate attribution of the drivers of CO2 variability prior to using contemporary observations to constrain long-term ESM responses. PMID:26074665

  9. Playing with ionic liquid mixtures to design engineered CO2 separation membranes.

    PubMed

    Tomé, Liliana C; Florindo, Catarina; Freire, Carmen S R; Rebelo, Luís Paulo N; Marrucho, Isabel M

    2014-08-28

    Ionic liquids have been explored as attractive alternative media for CO2 separation not only due to their low volatility but also due to their highly tuneable nature. Aiming at designing highly efficient liquid phases for flue gas separation and natural gas purification, this work focuses on the use of binary ionic liquid mixtures containing sulfate and/or cyano-functionalized anions. Several mixtures were prepared and their gas transport properties through supported ionic liquid membranes (SILMs) were investigated. The thermophysical properties of these mixtures, namely viscosity and density (data presented and discussed in ESI), were also measured so that trends between transport properties and thermophysical properties could be evaluated. The results obtained indicate that depending on the anions mixed, membranes with fine-tuned gas permeabilities, diffusivities and solubilities can be obtained. Additionally, SILMs prepared with these ionic liquid mixtures are on the upper bound of the CO2/N2 separation, or even may surpass it, indicating their potential for separating CO2 in low-pressure post-combustion processes. Overall, the use of ionic liquid mixtures combining the most selective anions with the least viscous anions is a highly promising strategy to design advanced engineered liquid phases for CO2 separation membranes.

  10. Stability of amine-functionalized cellulose during temperature-vacuum-swing cycling for CO2 capture from air.

    PubMed

    Gebald, Christoph; Wurzbacher, Jan A; Tingaut, Philippe; Steinfeld, Aldo

    2013-09-03

    The stability of amine-functionalized nanofibrilated cellulose sorbent for direct air capture of CO2 is investigated during temperature-vacuum-swing (TVS) cycling. The presence of O2 at 90 °C degrades the sorbent, reducing its CO2 adsorption capacity by 30% after 15 h of treatment in moist air with a dew point of 22 °C. In contrast, exposure to moist CO2 at 90 °C with a dew point of 22 °C does not deteriorate its CO2 adsorption capacity after 15 h. Performing 100 TVS consecutive cycles, with CO2 adsorption from ambient air containing 400-530 ppm CO2 at 30 °C and 60% relative humidity and with CO2 desorption at 90 °C and 30 mbar, resulted in a reduction of the equilibrium CO2 adsorption capacity by maximum 5%. The average CO2 adsorption capacity during TVS cyclic operation is 0.90 mmol CO2/g.

  11. Effect of SO2 and steam on CO2 capture performance of biomass-templated calcium aluminate pellets.

    PubMed

    Erans, María; Beisheim, Theodor; Manovic, Vasilije; Jeremias, Michal; Patchigolla, Kumar; Dieter, Heiko; Duan, Lunbo; Anthony, Edward J

    2016-10-20

    Four types of synthetic sorbents were developed for high-temperature post-combustion calcium looping CO2 capture using Longcal limestone. Pellets were prepared with: lime and cement (LC); lime and flour (LF); lime, cement and flour (LCF); and lime, cement and flour doped with seawater (LCFSW). Flour was used as a templating material. All samples underwent 20 cycles in a TGA under two different calcination conditions. Moreover, the prepared sorbents were tested for 10 carbonation/calcination cycles in a 68 mm-internal-diameter bubbling fluidized bed (BFB) in three environments: with no sulphur and no steam; in the presence of sulphur; and with steam. When compared to limestone, all the synthetic sorbents exhibited enhanced CO2 capture performance in the BFB experiments, with the exception of the sample doped with seawater. In the BFB tests, the addition of cement binder during the pelletisation process resulted in the increase of CO2 capture capacity from 0.08 g CO2 per g sorbent (LF) to 0.15 g CO2 per g sorbent (LCF) by the 10(th) cycle. The CO2 uptake in the presence of SO2 dramatically declined by the 10(th) cycle; for example, from 0.22 g CO2 per g sorbent to 0.05 g CO2 per g sorbent in the case of the untemplated material (LC). However, as expected all samples showed improved performance in the presence of steam, and the decay of reactivity during the cycles was less pronounced. Nevertheless, in the BFB environment, the templated pellets showed poorer CO2 capture performance. This is presumably because of material loss due to attrition under the FB conditions. By contrast, the templated materials performed better than untemplated materials under TGA conditions. This indicates that the reduction of attrition is critical when employing templated materials in realistic systems with FB reactors.

  12. Comparison of Volatiles and Mosquito Capture Efficacy For Three Carbohydrate Sources In A Yeast-Fermentation CO2 Generator.

    PubMed

    Aldridge, Robert L; Britch, Seth C; Allan, Sandra A; Tsikolia, Maia; Calix, Lesly Carolina; Bernier, Ulrich R; Linthicum, Kenneth J

    2016-12-01

    Mosquito surveillance in remote areas with limited access to canisters of CO2 or dry ice will benefit from an effective alternative CO2 source, such as the natural production of CO2 from yeast fermentation. In this study, we investigate differences in mosquito capture rates from the Centers for Disease Control and Prevention (CDC) light traps baited with dry ice compared with traps baited with yeast fermentation of several carbohydrate sources over 23 trap-nights. Results demonstrated the ability of yeast-generated CO2 to effectively attract mosquitoes to a CDC trap, regardless of carbohydrate source. Total collections of mosquitoes using dry ice were significantly higher than collections from yeast-generated CO2 sources. However, mosquito community structure, i.e., the species and relative capture rate of each species, was represented comparably across collections regardless of CO2 source. Volatiles produced by yeast fermentation were analyzed by carbohydrate source, revealing a suite of compounds, possibly synergistic, enhancing effects with CO2 on mosquito collection capability compared with the amount of CO2 used to attract mosquitoes.

  13. Membraneless laminar flow cell for electrocatalytic CO2 reduction with liquid product separation

    NASA Astrophysics Data System (ADS)

    Monroe, Morgan M.; Lobaccaro, Peter; Lum, Yanwei; Ager, Joel W.

    2017-04-01

    The production of liquid fuel products via electrochemical reduction of CO2 is a potential path to produce sustainable fuels. However, to be practical, a separation strategy is required to isolate the fuel-containing electrolyte produced at the cathode from the anode and also prevent the oxidation products (i.e. O2) from reaching the cathode. Ion-conducting membranes have been applied in CO2 reduction reactors to achieve this separation, but they represent an efficiency loss and can be permeable to some product species. An alternative membraneless approach is developed here to maintain product separation through the use of a laminar flow cell. Computational modelling shows that near-unity separation efficiencies are possible at current densities achievable now with metal cathodes via optimization of the spacing between the electrodes and the electrolyte flow rate. Laminar flow reactor prototypes were fabricated with a range of channel widths by 3D printing. CO2 reduction to formic acid on Sn electrodes was used as the liquid product forming reaction, and the separation efficiency for the dissolved product was evaluated with high performance liquid chromatography. Trends in product separation efficiency with channel width and flow rate were in qualitative agreement with the model, but the separation efficiency was lower, with a maximum value of 90% achieved.

  14. Effects of Microporosity and Surface Chemistry on Separation Performances of N-Containing Pitch-Based Activated Carbons for CO2/N2 Binary Mixture

    PubMed Central

    Lee, Min-Sang; Park, Mira; Kim, Hak Yong; Park, Soo-Jin

    2016-01-01

    In this study, N-containing pitch-based activated carbons (NPCs) were prepared using petroleum pitch with a low softening point and melamine with a high nitrogen content. The major advantage of the preparation method is that it enables variations in chemical structures and textural properties by steam activation at high temperatures. The adequate micropore structures, appropriate chemical modifications, and high adsorption enthalpies of NPCs are favorable for CO2 adsorption onto carbon surfaces. Furthermore, the structure generates a considerable gas/N-containing carbon interfacial area, and provides selective access to CO2 molecules over N2 molecules by offering an increased number of active sites on the carbon surfaces. The highest CO2/N2 selectivity, i.e., 47.5, and CO2 adsorption capacity for a CO2/N2 (0.15:0.85) binary gas mixture, i.e., 5.30 wt%, were attained at 298 K. The NPCs also gave reversible and durable CO2-capturing performances. All the results suggest that NPCs are promising CO2 sorbents, which can meet the challenges of current CO2 capture and separation techniques. PMID:26987683

  15. Effects of Microporosity and Surface Chemistry on Separation Performances of N-Containing Pitch-Based Activated Carbons for CO2/N2 Binary Mixture

    NASA Astrophysics Data System (ADS)

    Lee, Min-Sang; Park, Mira; Kim, Hak Yong; Park, Soo-Jin

    2016-03-01

    In this study, N-containing pitch-based activated carbons (NPCs) were prepared using petroleum pitch with a low softening point and melamine with a high nitrogen content. The major advantage of the preparation method is that it enables variations in chemical structures and textural properties by steam activation at high temperatures. The adequate micropore structures, appropriate chemical modifications, and high adsorption enthalpies of NPCs are favorable for CO2 adsorption onto carbon surfaces. Furthermore, the structure generates a considerable gas/N-containing carbon interfacial area, and provides selective access to CO2 molecules over N2 molecules by offering an increased number of active sites on the carbon surfaces. The highest CO2/N2 selectivity, i.e., 47.5, and CO2 adsorption capacity for a CO2/N2 (0.15:0.85) binary gas mixture, i.e., 5.30 wt%, were attained at 298 K. The NPCs also gave reversible and durable CO2-capturing performances. All the results suggest that NPCs are promising CO2 sorbents, which can meet the challenges of current CO2 capture and separation techniques.

  16. Separation of biospheric and fossil fuel fluxes of CO2 by atmospheric inversion of CO2 and 14CO2 measurements: Observation System Simulations

    NASA Astrophysics Data System (ADS)

    Basu, Sourish; Bharat Miller, John; Lehman, Scott

    2016-05-01

    National annual total CO2 emissions from combustion of fossil fuels are likely known to within 5-10 % for most developed countries. However, uncertainties are inevitably larger (by unknown amounts) for emission estimates at regional and monthly scales, or for developing countries. Given recent international efforts to establish emission reduction targets, independent determination and verification of regional and national scale fossil fuel CO2 emissions are likely to become increasingly important. Here, we take advantage of the fact that precise measurements of 14C in CO2 provide a largely unbiased tracer for recently added fossil-fuel-derived CO2 in the atmosphere and present an atmospheric inversion technique to jointly assimilate observations of CO2 and 14CO2 in order to simultaneously estimate fossil fuel emissions and biospheric exchange fluxes of CO2. Using this method in a set of Observation System Simulation Experiments (OSSEs), we show that given the coverage of 14CO2 measurements available in 2010 (969 over North America, 1063 globally), we can recover the US national total fossil fuel emission to better than 1 % for the year and to within 5 % for most months. Increasing the number of 14CO2 observations to ˜ 5000 per year over North America, as recently recommended by the National Academy of Science (NAS) (Pacala et al., 2010), we recover monthly emissions to within 5 % for all months for the US as a whole and also for smaller, highly emissive regions over which the specified data coverage is relatively dense, such as for the New England states or the NY-NJ-PA tri-state area. This result suggests that, given continued improvement in state-of-the art transport models, a measurement program similar in scale to that recommended by the NAS can provide for independent verification of bottom-up inventories of fossil fuel CO2 at the regional and national scale. In addition, we show that the dual tracer inversion framework can detect and minimize biases in

  17. Large-scale screening of zeolite structures for CO2 membrane separations.

    PubMed

    Kim, Jihan; Abouelnasr, Mahmoud; Lin, Li-Chiang; Smit, Berend

    2013-05-22

    We have conducted large-scale screening of zeolite materials for CO2/CH4 and CO2/N2 membrane separation applications using the free energy landscape of the guest molecules inside these porous materials. We show how advanced molecular simulations can be integrated with the design of a simple separation process to arrive at a metric to rank performance of over 87,000 different zeolite structures, including the known IZA zeolite structures. Our novel, efficient algorithm using graphics processing units can accurately characterize both the adsorption and diffusion properties of a given structure in just a few seconds and accordingly find a set of optimal structures for different desired purity of separated gases from a large database of porous materials in reasonable wall time. Our analysis reveals that the optimal structures for separations usually consist of channels with adsorption sites spread relatively uniformly across the entire channel such that they feature well-balanced CO2 adsorption and diffusion properties. Our screening also shows that the top structures in the predicted zeolite database outperform the best known zeolite by a factor of 4-7. Finally, we have identified a completely different optimal set of zeolite structures that are suitable for an inverse process, in which the CO2 is retained while CH4 or N2 is passed through a membrane.

  18. Large-Scale Screening of Zeolite Structures for CO2 Membrane Separations

    SciTech Connect

    Kim, JH; Abouelnasr, M; Lin, LC; Smit, B

    2013-05-22

    We have conducted large-scale screening of zeolite materials for CO2/CH4 and CO2/N-2 membrane separation applications using the free energy landscape of the guest molecules inside these porous materials. We show how advanced molecular simulations can be integrated with the design of a simple separation process to arrive at a metric to rank performance of over 87 000 different zeolite structures, including the known IZA zeolite structures. Our novel, efficient algorithm using graphics processing units can accurately characterize both the adsorption and diffusion properties of a given structure in just a few seconds and accordingly find a set of optimal structures for different desired purity of separated gases from a large database of porous materials in reasonable wall time. Our analysis reveals that the optimal structures for separations usually consist of channels with adsorption sites spread relatively uniformly across the entire channel such that they feature well-balanced CO2 adsorption and diffusion properties. Our screening also shows that the top structures in the predicted zeolite database outperform the best known zeolite by a factor of 4-7. Finally, we have identified a completely different optimal set of zeolite structures that are suitable for an inverse process, in which the CO2 is retained while CH4 or N-2 is passed through a membrane.

  19. Phase Separation Kinetics in Isopycnic Mixtures of H2O/CO2/Ethoxylated Alcohol Surfactants

    NASA Technical Reports Server (NTRS)

    Lesemann, Markus; Paulaitis, Michael E.; Kaler, Eric W.

    1999-01-01

    Ternary mixtures of H2O and CO2 with ethoxylated alcohol (C(sub i)E(sub j)) surfactants form three coexisting liquid phases at conditions where two of the phases have equal densities (isopycnic phases). Isopycnic phase behavior has been observed for mixtures containing C8E5, C10E6, and C12E6 surfactants, but not for those mixtures containing either C4E1 or C8E3 surfactants. Pressure-temperature (PT) projections for this three-phase equilibrium were determined for H2O/CO2/C8E5 and H2O/CO2/C10E6 mixtures at temperatures from approximately 25 to 33 C and pressures between 90 and 350 bar. Measurements of the microstructure in H2O/CO2/C12E6 mixtures as a function of temperature (25-31 C), pressure (63.1-90.7 bar), and CO2 composition (0-3.9 wt%) have also been carried out to show that while micellar structure remains essentially un-changed, critical concentration fluctuations increase as the phase boundary and plait point are approached. In this report, we present our first measurements of the kinetics of isopycnic phase separation for ternary mixtures of H2O/CO2/C8E5.

  20. Comparing post-combustion CO2 capture operation at retrofitted coal-fired power plants in the Texas and Great Britain electric grids

    NASA Astrophysics Data System (ADS)

    Cohen, Stuart M.; Chalmers, Hannah L.; Webber, Michael E.; King, Carey W.

    2011-04-01

    This work analyses the carbon dioxide (CO2) capture system operation within the Electric Reliability Council of Texas (ERCOT) and Great Britain (GB) electric grids using a previously developed first-order hourly electricity dispatch and pricing model. The grids are compared in their 2006 configuration with the addition of coal-based CO2 capture retrofits and emissions penalties from 0 to 100 US dollars per metric ton of CO2 (USD/tCO2). CO2 capture flexibility is investigated by comparing inflexible CO2 capture systems to flexible ones that can choose between full- and zero-load CO2 capture depending on which operating mode has lower costs or higher profits. Comparing these two grids is interesting because they have similar installed capacity and peak demand, and both are isolated electricity systems with competitive wholesale electricity markets. However, differences in capacity mix, demand patterns, and fuel markets produce diverging behaviours of CO2 capture at coal-fired power plants. Coal-fired facilities are primarily base load in ERCOT for a large range of CO2 prices but are comparably later in the dispatch order in GB and consequently often supply intermediate load. As a result, the ability to capture CO2 is more important for ensuring dispatch of coal-fired facilities in GB than in ERCOT when CO2 prices are high. In GB, higher overall coal prices mean that CO2 prices must be slightly higher than in ERCOT before the emissions savings of CO2 capture offset capture energy costs. However, once CO2 capture is economical, operating CO2 capture on half the coal fleet in each grid achieves greater emissions reductions in GB because the total coal-based capacity is 6 GW greater than in ERCOT. The market characteristics studied suggest greater opportunity for flexible CO2 capture to improve operating profits in ERCOT, but profit improvements can be offset by a flexibility cost penalty.

  1. Polyvinylidene fluoride/siloxane nanofibrous membranes for long-term continuous CO2 -capture with large absorption-flux enhancement.

    PubMed

    Lin, Yi-Feng; Wang, Chi-Sen; Ko, Chia-Chieh; Chen, Chien-Hua; Chang, Kai-Shiun; Tung, Kuo-Lun; Lee, Kueir-Rarn

    2014-02-01

    In a CO2 membrane contactor system, CO2 passes through a hydrophobic porous membrane in the gas phase to contact the amine absorbent in the liquid phase. Consequently, additional CO2 gas is absorbed by amine absorbents. This study examines highly porous polyvinylidene fluoride (PVDF)/siloxane nanofibrous layers that are modified with hydrophobic fluoroalkylsilane (FAS) functional groups and successfully coated onto a macroporous Al2 O3 membrane. The performance of these materials in a membrane contactor system for CO2 absorption is also investigated. Compared with pristine PVDF nanofibrous membranes, the PVDF/siloxane nanofibrous membranes exhibit greater solvent resistance and mechanical strength, making them more suitable for use in CO2 capture by the membrane contactor. The PVDF/siloxane nanofibrous layer in highly porous FAS-modified membranes can prevent the wetting of the membrane by the amine absorbent; this extends the periods of continuous CO2 absorption and results in a high CO2 absorption flux with a minimum of 500 % enhancement over that of the uncoated membranes. This study suggests the potential use of an FAS-modified PVDF/siloxane nanofibrous membrane in a membrane contactor system for CO2 absorption. The resulting hydrophobic membrane contactor also demonstrates the potential for large-scale CO2 absorption during post-combustion processes in power plants.

  2. Activity and stability of immobilized carbonic anhydrase for promoting CO2 absorption into a carbonate solution for post-combustion CO2 capture

    USGS Publications Warehouse

    Zhang, S.; Zhang, Z.; Lu, Y.; Rostam-Abadi, M.; Jones, A.

    2011-01-01

    An Integrated Vacuum Carbonate Absorption Process (IVCAP) currently under development could significantly reduce the energy consumed when capturing CO2 from the flue gases of coal-fired power plants. The biocatalyst carbonic anhydrase (CA) has been found to effectively promote the absorption of CO2 into the potassium carbonate solution that would be used in the IVCAP. Two CA enzymes were immobilized onto three selected support materials having different pore structures. The thermal stability of the immobilized CA enzymes was significantly greater than their free counterparts. For example, the immobilized enzymes retained at least 60% of their initial activities after 90days at 50??C compared to about 30% for their free counterparts under the same conditions. The immobilized CA also had significantly improved resistance to concentrations of sulfate (0.4M), nitrate (0.05M) and chloride (0.3M) typically found in flue gas scrubbing liquids than their free counterparts. ?? 2011 Elsevier Ltd.

  3. CaO nanocrystals grown over SiO2 microtubes for efficient CO2 capture: organogel sets the platform.

    PubMed

    Prathap, Annamalai; Shaijumon, M M; Sureshan, Kana M

    2016-01-25

    Materials that can capture and store CO2 are important. Though CaO is a cheap sorbent, it is inefficient for practical purposes due to sintering and poor diffusion of CO2 through the surface-CaCO3 layer. We have developed a high performance, sintering-resistant CaO-based sorbent by uniformly nanofabricating the CaO nanocrystals on SiO2 microtubes made by organogel templated polymerization.

  4. Continuous Flow Processing of ZIF-8 Membranes on Polymeric Porous Hollow Fiber Supports for CO2 Capture.

    PubMed

    Marti, Anne M; Wickramanayake, Wasala; Dahe, Ganpat; Sekizkardes, Ali; Bank, Tracy L; Hopkinson, David P; Venna, Surendar R

    2017-02-22

    We have utilized an environmentally friendly synthesis approach for the accelerated growth of a selective inorganic membrane on a polymeric hollow fiber support for postcombustion carbon capture. Specifically, continuous defect-free ZIF-8 thin films were grown and anchored using continuous flow synthesis on the outer surface of porous supports using water as solvent. These membranes demonstrated CO2 permeance of 22 GPU and the highest reported CO2/N2 selectivity of 52 for a continuous flow synthesized ZIF-8 membrane.

  5. Compact, Lightweight Adsorber and Sabatier Reactor for CO2 Capture and Reduction for Consumable and Propellant Production

    NASA Technical Reports Server (NTRS)

    Junaedi, Christian; Hawley, Kyle; Walsh, Dennis; Roychoudhury, Subir; Busby, Stacy A.; Abney, Morgan B.; Perry, Jay L.; Knox, James C.

    2012-01-01

    The utilization of CO2 to produce (or recycle) life support consumables, such as O2 and H2O, and to generate propellant fuels is an important aspect of NASA's concept for future, long duration planetary exploration. One potential approach is to capture and use CO2 from the Martian atmosphere to generate the consumables and propellant fuels. Precision Combustion, Inc. (PCI), with support from NASA, continues to develop its regenerable adsorber technology for capturing CO2 from gaseous atmospheres (for cabin atmosphere revitalization and in-situ resource utilization applications) and its Sabatier reactor for converting CO2 to methane and water. Both technologies are based on PCI's Microlith(R) substrates and have been demonstrated to reduce size, weight, and power consumption during CO2 capture and methanation process. For adsorber applications, the Microlith substrates offer a unique resistive heating capability that shows potential for short regeneration time and reduced power requirements compared to conventional systems. For the Sabatier applications, the combination of the Microlith substrates and durable catalyst coating permits efficient CO2 methanation that favors high reactant conversion, high selectivity, and durability. Results from performance testing at various operating conditions will be presented. An effort to optimize the Sabatier reactor and to develop a bench-top Sabatier Development Unit (SDU) will be discussed.

  6. A Life Cycle Assessment Case Study of Coal-Fired Electricity Generation with Humidity Swing Direct Air Capture of CO2 versus MEA-Based Postcombustion Capture.

    PubMed

    van der Giesen, Coen; Meinrenken, Christoph J; Kleijn, René; Sprecher, Benjamin; Lackner, Klaus S; Kramer, Gert Jan

    2017-01-17

    Most carbon capture and storage (CCS) envisions capturing CO2 from flue gas. Direct air capture (DAC) of CO2 has hitherto been deemed unviable because of the higher energy associated with capture at low atmospheric concentrations. We present a Life Cycle Assessment of coal-fired electricity generation that compares monoethanolamine (MEA)-based postcombustion capture (PCC) of CO2 with distributed, humidity-swing-based direct air capture (HS-DAC). Given suitable temperature, humidity, wind, and water availability, HS-DAC can be largely passive. Comparing energy requirements of HS-DAC and MEA-PCC, we find that the parasitic load of HS-DAC is less than twice that of MEA-PCC (60-72 kJ/mol versus 33-46 kJ/mol, respectively). We also compare other environmental impacts as a function of net greenhouse gas (GHG) mitigation: To achieve the same 73% mitigation as MEA-PCC, HS-DAC would increase nine other environmental impacts by on average 38%, whereas MEA-PCC would increase them by 31%. Powering distributed HS-DAC with photovoltaics (instead of coal) while including recapture of all background GHG, reduces this increase to 18%, hypothetically enabling coal-based electricity with net-zero life-cycle GHG. We conclude that, in suitable geographies, HS-DAC can complement MEA-PCC to enable CO2 capture independent of time and location of emissions and recapture background GHG from fossil-based electricity beyond flue stack emissions.

  7. Effects of Sulfur Doping and Humidity on CO2 Capture by Graphite Split Pore: A Theoretical Study.

    PubMed

    Li, Xiaofang; Xue, Qingzhong; Chang, Xiao; Zhu, Lei; Ling, Cuicui; Zheng, Haixia

    2017-03-08

    By use of grand canonical Monte Carlo calculations, we study the effects of sulfur doping and humidity on the performance of graphite split pore as an adsorbent for CO2 capture. It is demonstrated that S doping can greatly enhance pure CO2 uptake by graphite split pore. For example, S-graphite split pore with 33.12% sulfur shows a 39.85% rise in pure CO2 uptake (51.001 mmol/mol) compared with pristine graphite split pore at 300 K and 1 bar. More importantly, it is found that S-graphite split pore can still maintain much higher CO2 uptake than that by pristine graphite split pore in the presence of water. Especially, uptake by 33.12% sulfur-doped S-graphite split pore is 51.963 mmol of CO2/mol in the presence of water, which is 44.34% higher than that by pristine graphite split pore at 300 K and 1 bar. In addition, CO2/N2 selectivity of S-graphite split pore increases with increasing S content, resulting from stronger interactions between CO2 and S-graphite split pore. Moreover, by use of density functional theory calculations, we demonstrate that S doping can enhance adsorption energy between CO2 molecules and S-graphene surface at different humidities and furthermore enhance CO2 uptake by S-graphite split pore. Our results indicate that S-graphite split pore is a promising adsorbent material for humid CO2 capture.

  8. Adaptation to high CO2 concentration in an optimal environment: radiation capture, canopy quantum yield and carbon use efficiency

    NASA Technical Reports Server (NTRS)

    Monje, O.; Bugbee, B.

    1998-01-01

    The effect of elevated [CO2] on wheat (Triticum aestivum L. Veery 10) productivity was examined by analysing radiation capture, canopy quantum yield, canopy carbon use efficiency, harvest index and daily C gain. Canopies were grown at either 330 or 1200 micromoles mol-1 [CO2] in controlled environments, where root and shoot C fluxes were monitored continuously from emergence to harvest. A rapidly circulating hydroponic solution supplied nutrients, water and root zone oxygen. At harvest, dry mass predicted from gas exchange data was 102.8 +/- 4.7% of the observed dry mass in six trials. Neither radiation capture efficiency nor carbon use efficiency were affected by elevated [CO2], but yield increased by 13% due to a sustained increase in canopy quantum yield. CO2 enrichment increased root mass, tiller number and seed mass. Harvest index and chlorophyll concentration were unchanged, but CO2 enrichment increased average life cycle net photosynthesis (13%, P < 0.05) and root respiration (24%, P < 0.05). These data indicate that plant communities adapt to CO2 enrichment through changes in C allocation. Elevated [CO2] increases sink strength in optimal environments, resulting in sustained increases in photosynthetic capacity, canopy quantum yield and daily C gain throughout the life cycle.

  9. Efficient CO2 capture and photoreduction by amine-functionalized TiO2.

    PubMed

    Liao, Yusen; Cao, Shao-Wen; Yuan, Yupeng; Gu, Quan; Zhang, Zhenyi; Xue, Can

    2014-08-11

    Amine-functionalization of TiO2 nanoparticles, through a solvothermal approach, substantially increases the affinity of CO2 on TiO2 surfaces through chemisorption. This chemisorption allows for more effective activation of CO2 and charge transfer from excited TiO2 , and significantly enhances the photocatalytic rate of CO2 reduction into methane and CO.

  10. Impact of CO2 and climate on Last Glacial Maximum vegetation - a factor separation

    NASA Astrophysics Data System (ADS)

    Claussen, M.; Selent, K.; Brovkin, V.; Raddatz, T.; Gayler, V.

    2012-11-01

    Differences between glacial and pre-industrial potential vegetation patterns can conceptually be attributed to two factors: firstly to differences in the climate, caused by a strong increase in ice masses and the radiative effect of lower greenhouse gas concentrations, and secondly to differences in the ecophysiological effect of lower glacial atmospheric CO2 concentrations. The synergy emerging from these effects when operating simultaneously can be interpreted as sensitivity of the effect of enhancing physiologically available CO2 on shifting vegetation to climate warming. Alternatively and equally valid, it can be viewed as sensitivity of climatically induced vegetation changes to differences in physiologically available CO2. A first complete factor separation based on simulations with the MPI Earth System Model indicates that the pure climate effect mainly leads to a contraction or a shift in vegetation patterns when comparing glacial with pre-industrial simulation vegetation patterns. Globally, a reduction in fractional coverage of most plant functional types is seen - except for raingreen shrubs which strongly benefit from the colder and drier climate. The ecophysiological effect of CO2 appears to be stronger than the pure climate contribution for many plant functional types - in line with previous simulations. The ecophysiological effect of lower CO2 mainly yields a reduction in fractional coverage, a thinning of vegetation and a strong reduction in net primary production. The synergy appears to be as strong as each of the pure contributions locally. For tropical evergreen trees, the synergy appears strong also on global average. Hence this modelling study suggests that for tropical forests, an increase in CO2 has, on average, a stronger ecophysiological effect in warmer climate than in glacial climate. Alternatively, areal differences in tropical forests induced by climate warming can, on average, be expected to be larger with increasing concentration of

  11. Evaluating transformational solvent systems for post-combustion CO2 separations

    SciTech Connect

    Heldebrant, David J.; Glezakou, Vassiliki Alexandra; Koech, Phillip K.; Mathias, Paul M.; Cantu Cantu, David; Rousseau, Roger J.; Malhotra, Deepika; Bhakta, Mukund; Bearden, Mark D.; Freeman, Charles J.; Zheng, Feng

    2014-01-06

    Broad research is underway on developing transformational solvents that can capture of CO2 from flue gas with lower energy compared to aqueous amines. Water-lean, or non-aqueous, solvents are being considered as a class of transformational solvents due to the prospect of lower energy duties by not having to heat and condense water. To date, little is known about the real world performance of water-lean solvent systems compared to commercial aqueous amine technologies, and whether or not they can utilize existing or at least similar processing infrastructure. This paper provides the key results from a comprehensive three-year study of the water-lean CO2-Binding Organic Liquids (CO2BOL) solvent platform coupled with Polarity-Swing Assisted Regeneration (PSAR). We present here thermodynamic, kinetic, and bench-scale data, followed by Aspen Plus projections of full-scale process performance for three CO2BOL/PSAR cases. This paper also provides discussions on materials performance and identifies viscosity as a critical property that most greatly limits the viability of water-lean solvent platforms. We provide results from a new effort spanning molecular modeling and synthesis and experimental testing to decipher the critical material properties needed to address this challenge. We conclude with implications for development of other water-lean solvent systems

  12. Load-following control of an IGCC plant with CO2 capture

    SciTech Connect

    Bhattacharyya, D.; Turton, R.; Zitney, S.

    2011-01-01

    In this paper, a decentralized control strategy is considered for load-following control of an integrated gasification combined cycle (IGCC) plant with CO2 capture without flaring the syngas. The control strategy considered is gas turbine (GT) lead with gasifier follow. In this strategy, the GT controls the power load by manipulating its firing rate while the slurry feed flow to the gasifier is manipulated to control the syngas pressure at the GT inlet. However, the syngas pressure control is an integrating process with significant timedelay. In this work, a modified proportional-integral-derivative (PID) control is considered for syngas pressure control given that conventional PID controllers show poor control performance for integrating processes with large time delays. The conventional PID control is augmented with an internal feedback loop. The P-controller used in this internal loop converts the integrating process to an open-loop stable process. The resulting secondorder plus time delay model uses a PID controller where the tuning parameters are found by minimizing the integral time-weighted absolute error (ITAE) for disturbance rejection. A plant model with single integrator and time delay is identified by a P-control method. When a ramp change is introduced in the set-point of the load controller, the performance of both the load and pressure controllers with the modified PID control strategy is found to be superior to that using a traditional PID controller. Key

  13. CO2 capture in amine solutions: modelling and simulations with non-empirical methods

    NASA Astrophysics Data System (ADS)

    Andreoni, Wanda; Pietrucci, Fabio

    2016-12-01

    Absorption in aqueous amine solutions is the most advanced technology for the capture of CO2, although suffering from drawbacks that do not allow exploitation on large scale. The search for optimum solvents has been pursued with empirical methods and has also motivated a number of computational approaches over the last decade. However, a deeper level of understanding of the relevant chemical reactions in solution is required so as to contribute to this effort. We present here a brief critical overview of the most recent applications of computer simulations using ab initio methods. Comparison of their outcome shows a strong dependence on the structural models employed to represent the molecular systems in solution and on the strategy used to simulate the reactions. In particular, the results of very recent ab initio molecular dynamics augmented with metadynamics are summarized, showing the crucial role of water, which has been so far strongly underestimated both in the calculations and in the interpretation of experimental data. Indications are given for advances in computational approaches that are necessary if meant to contribute to the rational design of new solvents.

  14. A framework for environmental assessment of CO2 capture and storage systems

    SciTech Connect

    Sathre, R; Chester, M; Cain, J; Masanet, E

    2012-01-01

    Carbon dioxide capture and storage (CCS) is increasingly seen as a way for society to enjoy the benefits of fossil fuel energy sources while avoiding the climate disruption associated with fossil CO2 emissions. A decision to deploy CCS technology at scale should be based on robust information on its overall costs and benefits. Life-cycle assessment (LCA) is a framework for holistic assessment of the energy and environmental footprint of a system, and can provide crucial information to policy-makers, scientists, and engineers as they develop and deploy CCS systems. We identify seven key issues that should be considered to ensure that conclusions and recommendations from CCS LCA are robust: energy penalty, functional units, scale-up challenges, non-climate environmental impacts, uncertainty management, policy-making needs, and market effects. Several recent life-cycle studies have focused on detailed assessments of individual CCS technologies and applications. While such studies provide important data and information on technology performance, such case-specific data are inadequate to fully inform the decision making process. LCA should aim to describe the system-wide environmental implications of CCS deployment at scale, rather than a narrow analysis of technological performance of individual power plants. (C) 2011 Elsevier Ltd. All rights reserved.

  15. CO2 capture in amine solutions: modelling and simulations with non-empirical methods.

    PubMed

    Andreoni, Wanda; Pietrucci, Fabio

    2016-12-21

    Absorption in aqueous amine solutions is the most advanced technology for the capture of CO2, although suffering from drawbacks that do not allow exploitation on large scale. The search for optimum solvents has been pursued with empirical methods and has also motivated a number of computational approaches over the last decade. However, a deeper level of understanding of the relevant chemical reactions in solution is required so as to contribute to this effort. We present here a brief critical overview of the most recent applications of computer simulations using ab initio methods. Comparison of their outcome shows a strong dependence on the structural models employed to represent the molecular systems in solution and on the strategy used to simulate the reactions. In particular, the results of very recent ab initio molecular dynamics augmented with metadynamics are summarized, showing the crucial role of water, which has been so far strongly underestimated both in the calculations and in the interpretation of experimental data. Indications are given for advances in computational approaches that are necessary if meant to contribute to the rational design of new solvents.

  16. Biological N removal from wastes generated from amine-based CO2 capture: case monoethanolamine.

    PubMed

    Hauser, Ingrid; Colaço, Ana B; Skjæran, Julie A; Einbu, Aslak; Ostgaard, Kjetill; Svendsen, Hallvard F; Cervantes, Francisco J

    2013-02-01

    Large-scale amine-based CO(2) capture will generate waste containing large amounts of ammonia, in addition to contaminants such as the actual amine as well as degradation products thereof. Monoethanolamine (MEA) has been a dominant amine applied so far in this context. This study reveals how biological N removal can be achieved even in systems heavily contaminated by MEA in post- as well as pre-denitrification treatment systems, elucidating the rate-limiting factors of nitrification as well as aerobic and denitrifying biodegradation of MEA. The hydrolysis of MEA to ammonia readily occurred both in post- and pre-denitrification treatment systems with a hydraulic retention time of 7 h. MEA removal was ≥99 ± 1 % and total nitrogen removal 77 ± 10 % in both treatment systems. This study clearly demonstrates the advantage of pre-denitrification over post-denitrification for achieving biological nitrogen removal from MEA-contaminated effluents. Besides the removal of MEA, the removal efficiency of total nitrogen as well as organic matter was high without additional carbon source supplied.

  17. Decomposition of nitrosamines in CO2 capture by aqueous piperazine or monoethanolamine.

    PubMed

    Fine, Nathan A; Nielsen, Paul T; Rochelle, Gary T

    2014-05-20

    Amine scrubbing is an efficient method for carbon capture and sequestration, but secondary amines present in all amine solvents can form carcinogenic nitrosamines. Decomposition kinetics for n-nitrosopiperazine (MNPZ), nitrosodiethanolamine (NDELA), and nitroso-(2-hydroxyethyl) glycine (NHeGly) were measured over a range of temperature, base concentration, base strength, and CO2 loading pertinent to amine scrubbing. MNPZ and NDELA decomposition is first order in the nitrosamine, half order in base concentration, and base-catalyzed with a Brønsted slope of β = 0.5. The activation energy is 94, 106, and 112 kJ/mol for MNPZ, NDELA, and NHeGly, respectively. MNPZ readily decomposes at 150 °C in 5 M piperazine, making thermal decomposition an important mechanism for MNPZ control. However, NHeGly and NDELA are too stable at 120 °C in 7 M monoethanolamine (MEA) for thermal decomposition to be important. Base treatment during reclaiming could rapidly and selectively decompose NHeGly and NDELA to mitigate nitrosamine accumulation in MEA.

  18. CO2-Binding Organic Liquids Gas Capture with Polarity-Swing-Assisted Regeneration Full Technology Feasibility Study B1 - Solvent-based Systems

    SciTech Connect

    Heldebrant, David J

    2014-08-31

    PNNL, Fluor Corporation and Queens University (Kingston, ON) successfully completed a three year comprehensive study of the CO2BOL water-lean solvent platform with Polarity Swing Assisted Regeneration (PSAR). This study encompassed solvent synthesis, characterization, environmental toxicology, physical, thermodynamic and kinetic property measurements, Aspen Plus™ modeling and bench-scale testing of a candidate CO2BOL solvent molecule. Key Program Findings The key program findings are summarized as follows: • PSAR favorably reduced stripper duties and reboiler temperatures with little/no impact to absorption column • >90% CO2 capture was achievable at reasonable liquid-gas ratios in the absorber • High rich solvent viscosities (up to 600 cP) were successfully demonstrated in the bench-scale system. However, the projected impacts of high viscosity to capital cost and operational limits compromised the other levelized cost of electricity benefits. • Low thermal conductivity of organics significantly increased the required cross exchanger surface area, and potentially other heat exchange surfaces. • CO2BOL had low evaporative losses during bench-scale testing • There was no evidence of foaming during bench scale testing • Current CO2BOL formulation costs project to be $35/kg • Ecotoxicity (Water Daphnia) was comparable between CO2BOL and MEA (169.47 versus 103.63 mg/L) • Full dehydration of the flue gas was determined to not be economically feasible. However, modest refrigeration (13 MW for the 550 MW reference system) was determined to be potentially economically feasible, and still produce a water-lean condition for the CO2BOLs (5 wt% steady-state water loading). • CO2BOLs testing with 5 wt% water loading did not compromise anhydrous performance behavior, and showed actual enhancement of CO2 capture performance. • Mass transfer of CO2BOLs was not greatly impeded by viscosity • Facile separation of antisolvent from lean CO2BOL was

  19. Synthetic Architecture of MgO/C Nanocomposite from Hierarchical-Structured Coordination Polymer toward Enhanced CO2 Capture.

    PubMed

    Li, Ping; Liu, Wen; Dennis, John S; Zeng, Hua Chun

    2017-03-22

    Highly efficient, durable, and earth-abundant solid sorbents are of paramount importance for practical carbon capture, storage, and utilization. Here, we report a novel and facile two-step strategy to synthesize a group of hierarchically structured porous MgO/C nanocomposites using flowerlike Mg-containing coordination polymer as a precursor. The new nanocomposites exhibit superb CO2 capture performance with sorption capacity up to 30.9 wt % (at 27 °C, 1 bar CO2), fast sorption kinetics, and long cycling life. Importantly, the achieved capacity is >14 times higher than that of commercial MgO, and favorably exceeds the highest value recorded to date for MgO-based sorbents under similar operating conditions. On the basis of the morphological and textural property analysis, together with CO2 sorption mechanism study using CO2-TPD and DRIFT techniques, the outstanding performance in CO2 uptake originates from unique features of this type of sorbent materials, which include hierarchical architecture, porous building blocks of nanosheets, high specific surface area (ca. 300 m(2)/g), evenly dispersed MgO nanocrystallites (ca. 3 nm) providing abundant active sites, and the in situ generated carbon matrix that acts as a stabilizer to prevent the growth and agglomeration of MgO crystallites. The nanocomposite system developed in this work shows good potential for future low-cost CO2 abatement and utilization.

  20. An absorption mechanism and polarity-induced viscosity model for CO2 capture using hydroxypyridine-based ionic liquids.

    PubMed

    An, Xiaowei; Du, Xiao; Duan, Donghong; Shi, Lijuan; Hao, Xiaogang; Lu, Houfang; Guan, Guoqing; Peng, Changjun

    2017-01-04

    A series of new hydroxypyridine-based ionic liquids (ILs) are synthesized and applied in CO2 capture through chemical absorption, in which one IL, i.e., tetrabutylphosphonium 2-hydroxypyridine ([P4444][2-Op]), shows a viscosity as low as 193 cP with an absorption capacity as high as 1.20 mol CO2 per mol IL. Because the traditional anion-CO2 absorption mechanism cannot provide an explanation for the influences of cations and temperature on CO2 absorption capacity, herein, a novel cation-participating absorption mechanism based on the proton transfer is proposed to explain the high absorption capacity and the existence of a turning point of absorption capacity with the increase of temperature for the capture of CO2 using [P4444][n-Op] (n = 2, 3, 4) ILs. Also, the relationship between the viscosity of ILs and the linear interaction energy is proposed for the first time, which can guide how to design and synthesize ILs with low viscosity. Quantum chemistry calculations, which are based on the comprehensive analysis of dipole moment, cation-anion interaction energy and surface electrostatic potential, indicate that the different viscosities of hydroxypyridine-based ILs and the changes after CO2 absorption mainly resulted from the different distribution of negative charges in the anion.

  1. Mechanism of a reversible CO2 capture monitored by the layered perovskite Li2SrTa2O7.

    PubMed

    Galven, Cyrille; Fourquet, Jean-Louis; Suard, Emmanuelle; Crosnier-Lopez, Marie-Pierre; Le Berre, Françoise

    2010-05-07

    We demonstrate for the first time, a new CO(2) capture ability monitored by a Ruddelsden-Popper compound. Under a humid CO(2) atmosphere, Li(2)SrTa(2)O(7) is transformed into LiHSrTa(2)O(7) releasing lithium hydroxide which combined with the atmospheric CO(2) leads to Li(2)CO(3). The presence of carbonate is confirmed by IR, thermal analysis coupled with mass spectroscopy and diffraction experiments (X-ray and neutron). The structural study of LiHSrTa(2)O(7) performed with X-ray and neutron diffraction data showed that the structure differs from that of LiHSrTa(2)O(7) obtained by ionic exchange from Li(2)SrTa(2)O(7) by the Li(+)/H(+) repartition in the interlayer spacing. In the case of the LiHSrTa(2)O(7) studied in this paper, the Li(+) and H(+) ions are ordered, while in the other form, each cation is unequally distributed on 2 sites. By heating, Li(2)SrTa(2)O(7) is recovered showing that the CO(2) capture is reversible and the cyclability of the CO(2) capture has been tested during six cycles.

  2. Doping Li and K into Na2ZrO3 Sorbent to Improve Its CO2 Capture Capability

    NASA Astrophysics Data System (ADS)

    Duan, Yuhua

    Carbon dioxide is one of the major combustion products which once released into the air can contribute to global climate change. Solid sorbents have been reported in several previous studies to be promising candidates for CO2 sorbent applications due to their high CO2 absorption capacities at moderate working temperatures. However, at a given CO2 pressure, the turnover temperature (Tt) of an individual solid capture CO2 reaction is fixed and may be outside the operating temperature range (ΔTo) for a particularly capture technology. In order to shift such Tt for a solid into the range of ΔTo, its corresponding thermodynamic property must be changed by changing its structure by reacting (mixing) with other materials or doping with other elements. As an example, by combining thermodynamic database searching with ab initio thermodynamics calculations, in this work, we explored the Li- and K-doping effects on the Tt shifts of Na2ZrO3 at different doping levels. The obtained results showed that compared to pure Na2ZrO3, the Li- and K-doped mixtures Na2-αMαZrO3 (M =Li, K) have lower Tt and higher CO2 capture capacities.

  3. Impact of CO2 and climate on Last Glacial maximum vegetation - a factor separation

    NASA Astrophysics Data System (ADS)

    Claussen, M.; Selent, K.; Brovkin, V.; Raddatz, T.; Gayler, V.

    2013-06-01

    The factor separation of Stein and Alpert (1993) is applied to simulations with the MPI Earth system model to determine the factors which cause the differences between vegetation patterns in glacial and pre-industrial climate. The factors firstly include differences in the climate, caused by a strong increase in ice masses and the radiative effect of lower greenhouse gas concentrations; secondly, differences in the ecophysiological effect of lower glacial atmospheric CO2 concentrations; and thirdly, the synergy between the pure climate effect and the pure effect of changing physiologically available CO2. It is has been shown that the synergy can be interpreted as a measure of the sensitivity of ecophysiological CO2 effect to climate. The pure climate effect mainly leads to a contraction or a shift in vegetation patterns when comparing simulated glacial and pre-industrial vegetation patterns. Raingreen shrubs benefit from the colder and drier climate. The pure ecophysiological effect of CO2 appears to be stronger than the pure climate effect for many plant functional types - in line with previous simulations. The pure ecophysiological effect of lower CO2 mainly yields a reduction in fractional coverage, a thinning of vegetation and a strong reduction in net primary production. The synergy appears to be as strong as each of the pure contributions locally, but weak on global average for most plant functional types. For tropical evergreen trees, however, the synergy is strong on global average. It diminishes the difference between glacial and pre-industrial coverage of tropical evergreen trees, due to the pure climate effect and the pure ecophysiological CO2 effect, by approximately 50 per cent.

  4. Solid Sorbents for CO2 Capture from Post-Combustion and Pre-Combustion Gas Streams

    SciTech Connect

    Siriwardane, R.V.; Robinson, C.; Stevens, R.W.

    2007-08-01

    A novel liquid impregnated solid sorbent was developed for CO2 removal in the temperature range of ambient to 60 °C for both fixed bed and fluidized bed reactor applications. The sorbent is regenerable at 60-80 °C. Multi-cycle tests conducted in an atmospheric bench scale reactor with simulated flue gas demonstrated that the sorbent retains its CO2 sorption capacity with CO2 removal efficiency of about 99%. A second, novel solid sorbent containing mixture of alkali earth and alkali compounds was developed for CO2 removal at 200-315 °C from high pressure gas streams (i.e., suitable for IGCC systems). The sorbent showed very high capacity for CO2 removal from gas streams containing 28% CO2 at 200 °C and 11.2 atm during lab-scale flow reactor tests as well as regenerability at 375 °C.

  5. Efficient and reversible CO2 capture by amine functionalized-silica gel confined task-specific ionic liquid system.

    PubMed

    Aboudi, Javad; Vafaeezadeh, Majid

    2015-07-01

    Simple, efficient and practical CO2 capture method is reported using task-specific ionic liquid (IL) supported onto the amine-functionalized silica gel. The results have been shown that both the capacity and rate of the CO2 absorption notably increase in the supported IL/molecular sieve 4 Å system in comparison of homogeneous IL. Additionally, it has shown that the prepared material is capable for reversible carbon dioxide absorption for at least 10 cycles without significant loss of efficiency. The presence of the amine-based IL and the surface bonded amine groups increase the capacity of CO2 absorption even in a CO2/CH4 gas mixture through the formation of ammonium carbamate onto the surface of mesoporous material.

  6. Efficient and reversible CO2 capture by amine functionalized-silica gel confined task-specific ionic liquid system

    PubMed Central

    Aboudi, Javad; Vafaeezadeh, Majid

    2014-01-01

    Simple, efficient and practical CO2 capture method is reported using task-specific ionic liquid (IL) supported onto the amine-functionalized silica gel. The results have been shown that both the capacity and rate of the CO2 absorption notably increase in the supported IL/molecular sieve 4 Å system in comparison of homogeneous IL. Additionally, it has shown that the prepared material is capable for reversible carbon dioxide absorption for at least 10 cycles without significant loss of efficiency. The presence of the amine-based IL and the surface bonded amine groups increase the capacity of CO2 absorption even in a CO2/CH4 gas mixture through the formation of ammonium carbamate onto the surface of mesoporous material. PMID:26199747

  7. Highly Permeable Graphene Oxide/Polyelectrolytes Hybrid Thin Films for Enhanced CO2/N2 Separation Performance.

    PubMed

    Heo, Jiwoong; Choi, Moonhyun; Chang, Jungyun; Ji, Dahye; Kang, Sang Wook; Hong, Jinkee

    2017-03-28

    Separation of CO2 from other gasses offers environmental benefits since CO2 gas is the main contributor to global warming. Recently, graphene oxide (GO) based gas separation membranes are of interest due to their selective barrier properties. However, maintaining selectivity without sacrificing permeance is still challenging. Herein, we described the preparation and characterization of nanoscale GO membranes for CO2 separation with both high selectivity and permeance. The internal structure and thickness of the GO membranes were controlled by layer-by-layer (LbL) self-assembly. Polyelectrolyte layers are used as the supporting matrix and for facilitating CO2 transport. Enhanced gas separation was achieved by adjusting pH of the GO solutions and by varying the number of GO layers to provide a pathway for CO2 molecules. Separation performance strongly depends on the number of GO bilayers. The surfaces of the multilayered GO and polyelectrolyte films are characterized by atomic force microscopy and scanning electron microscopy. The (poly (diallyldimethylammonium chloride) (PDAC)/polystyrene sulfonate (PSS)) (GO/GO) multilayer membranes show a maximum CO2/N2 selectivity of 15.3 and a CO2 permeance of 1175.0 GPU. LbL-assembled GO membranes are shown to be effective candidates for CO2 separation based on their excellent CO2/N2 separation performance.

  8. Carbonic anhydrase mimics for enhanced CO2 absorption in an amine-based capture solvent.

    PubMed

    Kelsey, Rachael A; Miller, David A; Parkin, Sean R; Liu, Kun; Remias, Joe E; Yang, Yue; Lightstone, Felice C; Liu, Kunlei; Lippert, Cameron A; Odom, Susan A

    2016-01-07

    Two new small-molecule enzyme mimics of carbonic anhydrase were prepared and characterized. These complexes contain the salen-like ligand bis(hydroxyphenyl)phenanthroline. This ligand is similar to the salen-type ligands previously incorporated into carbonic anhydrase mimics but contains no hydrolyzable imine groups and therefore serves as a promising ligand scaffold for the synthesis of a more robust CO2 hydration catalyst. These homogeneous catalysts were investigated for CO2 hydration in concentrated primary amine solutions through which a dilute CO2 (14%) fluid stream was flowed and showed exceptional activity for increased CO2 absorption rates.

  9. C3 and C4 biomass allocation responses to elevated CO2 and nitrogen: contrasting resource capture strategies

    USGS Publications Warehouse

    White, K.P.; Langley, J.A.; Cahoon, D.R.; Megonigal, J.P.

    2012-01-01

    Plants alter biomass allocation to optimize resource capture. Plant strategy for resource capture may have important implications in intertidal marshes, where soil nitrogen (N) levels and atmospheric carbon dioxide (CO2) are changing. We conducted a factorial manipulation of atmospheric CO2 (ambient and ambient + 340 ppm) and soil N (ambient and ambient + 25 g m-2 year-1) in an intertidal marsh composed of common North Atlantic C3 and C4 species. Estimation of C3 stem turnover was used to adjust aboveground C3 productivity, and fine root productivity was partitioned into C3-C4 functional groups by isotopic analysis. The results suggest that the plants follow resource capture theory. The C3 species increased aboveground productivity under the added N and elevated CO2 treatment (P 2 alone. C3 fine root production decreased with added N (P 2 (P = 0.0481). The C4 species increased growth under high N availability both above- and belowground, but that stimulation was diminished under elevated CO2. The results suggest that the marsh vegetation allocates biomass according to resource capture at the individual plant level rather than for optimal ecosystem viability in regards to biomass influence over the processes that maintain soil surface elevation in equilibrium with sea level.

  10. Relationship between mosquito (Diptera: Culicidae) landing rates on a human subject and numbers captured using CO2-baited light traps

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Capture rates of female Aedes albopictus Skuse, Aedes triseriatus (Say), Anopheles quadrimaculatus Say, Culex nigripalpus Theobald, and Culex quinquefasciatus Say in CDC-type light traps supplemented with CO2 (LT) and using the human landing (HL) collection method were observed in matched-pair exper...

  11. Lime-based sorbents for high-temperature CO2 capture--a review of sorbent modification methods.

    PubMed

    Manovic, Vasilije; Anthony, Edward J

    2010-08-01

    This paper presents a review of the research on CO(2) capture by lime-based looping cycles undertaken at CanmetENERGY's (Ottawa, Canada) research laboratories. This is a new and very promising technology that may help in mitigation of global warming and climate change caused primarily by the use of fossil fuels. The intensity of the anticipated changes urgently requires solutions such as more cost-effective technologies for CO(2) capture. This new technology is based on the use of lime-based sorbents in a dual fluidized bed combustion (FBC) reactor which contains a carbonator-a unit for CO(2) capture, and a calciner-a unit for CaO regeneration. However, even though natural materials are cheap and abundant and very good candidates as solid CO(2) carriers, their performance in a practical system still shows significant limitations. These limitations include rapid loss of activity during the capture cycles, which is a result of sintering, attrition, and consequent elutriation from FBC reactors. Therefore, research on sorbent performance is critical and this paper reviews some of the promising ways to overcome these shortcomings. It is shown that reactivation by steam/water, thermal pre-treatment, and doping simultaneously with sorbent reforming and pelletization are promising potential solutions to reduce the loss of activity of these sorbents over multiple cycles of use.

  12. Energy and exergy analyses of an integrated gasification combined cycle power plant with CO2 capture using hot potassium carbonate solvent.

    PubMed

    Li, Sheng; Jin, Hongguang; Gao, Lin; Mumford, Kathryn Anne; Smith, Kathryn; Stevens, Geoff

    2014-12-16

    Energy and exergy analyses were studied for an integrated gasification combined cycle (IGCC) power plant with CO2 capture using hot potassium carbonate solvent. The study focused on the combined impact of the CO conversion ratio in the water gas shift (WGS) unit and CO2 recovery rate on component exergy destruction, plant efficiency, and energy penalty for CO2 capture. A theoretical limit for the minimal efficiency penalty for CO2 capture was also provided. It was found that total plant exergy destruction increased almost linearly with CO2 recovery rate and CO conversion ratio at low CO conversion ratios, but the exergy destruction from the WGS unit and the whole plant increased sharply when the CO conversion ratio was higher than 98.5% at the design WGS conditions, leading to a significant decrease in plant efficiency and increase in efficiency penalty for CO2 capture. When carbon capture rate was over around 70%, via a combination of around 100% CO2 recovery rate and lower CO conversion ratios, the efficiency penalty for CO2 capture was reduced. The minimal efficiency penalty for CO2 capture was estimated to be around 5.0 percentage points at design conditions in an IGCC plant with 90% carbon capture. Unlike the traditional aim of 100% CO conversion, it was recommended that extremely high CO conversion ratios should not be considered in order to decrease the energy penalty for CO2 capture and increase plant efficiency.

  13. Experimental and computational investigation of CO2 capture on amine grafted metal-organic framework NH2-MIL-101

    NASA Astrophysics Data System (ADS)

    Huang, Xiang; Lu, Jianfeng; Wang, Weilong; Wei, Xiaolan; Ding, Jing

    2016-05-01

    A standard metal-organic framework, NH2-MIL-101 based on chromium has been synthesized. For the purpose of offering more binding sites for CO2, post-synthetic modification of tetraethylenepentamine (TEPA) was conducted by using a wet impregnation method. With the aim of better understanding the thermodynamics and mechanisms of CO2 adsorption, molecular dynamics (MD) simulations have been used for structures optimization and adsorption kinetics of NH2-MIL-101/TEPA adsorbents, and the CO2 adsorption capacity with different TEPA loadings was simulated by the Monte Carlo (MC) method. Results confirmed that TEPA was successfully grafted on the coordinative unsaturated metal centers. At 1 bar and 298 K, NH2-MIL-101 combined with 50 wt% TEPA exhibited a CO2 uptake of 3.1 mmol/g-sorb. Under low loading of TEPA, the coordinative unsaturated metal centers made a relatively big contribution to CO2 adsorption. With more TEPA incorporated, the CO2 binding affinity was enhanced due to the existence of abundant amine groups. On the basis of both experimental and simulation analysis, this synthesized amine-grafted sorbent with excellent CO2 capture performance is an ideal material for greenhouse gas control.

  14. Biomimetic CO2 capture using a highly thermostable bacterial α-carbonic anhydrase immobilized on a polyurethane foam.

    PubMed

    Migliardini, Fortunato; De Luca, Viviana; Carginale, Vincenzo; Rossi, Mosè; Corbo, Pasquale; Supuran, Claudiu T; Capasso, Clemente

    2014-02-01

    The biomimetic approach represents an interesting strategy for carbon dioxide (CO2) capture, offering advantages over other methods, due to its specificity for CO2 and its eco-compatibility, as it allows concentration of CO2 from other gases, and its conversion to water soluble ions. This approach uses microorganisms capable of fixing CO2 through metabolic pathways or via the use of an enzyme, such as carbonic anhydrase (CA, EC 4.2.1.1). Recently, our group cloned and purified a novel bacterial α-CA, named SspCA, from the thermophilic bacteria, Sulfurihydrogenibium yellowstonense YO3AOP1 living in hot springs at temperatures of up to 110 °C. This enzyme showed an exceptional thermal stability, retaining its high catalytic activity for the CO2 hydration reaction even after being heated at 70 °C for several hours. In the present paper, the SspCA was immobilized within a polyurethane (PU) foam. The immobilized enzyme was found to be catalytically active and showed a long-term stability. A bioreactor containing the "PU-immobilized enzyme" (PU-SspCA) as shredded foam was used for experimental tests aimed to verify the CO2 capture capability in conditions close to those of a power plant application. In this bioreactor, a gas phase, containing CO2, was put into contact with a liquid phase under conditions, where CO2 contained in the gas phase was absorbed and efficiently converted into bicarbonate by the extremo-α-CA.

  15. Stability of a Benzyl Amine Based CO2 Capture Adsorbent in View of Regeneration Strategies

    PubMed Central

    2017-01-01

    In this work, the chemical and thermal stability of a primary amine-functionalized ion-exchange resin (Lewatit VP OC 1065) is studied in view of the potential options of regenerating this sorbent in a CO2 removal application. The adsorbent was treated continuously in the presence of air, different O2/CO2/N2 mixtures, concentrated CO2, and steam, and then the remaining CO2 adsorption capacity was measured. Elemental analysis, BET/BJH analysis, Fourier transform infrared spectroscopy, and thermogravimetric analysis were applied to characterize adsorbent properties. This material was found to be thermally and hydrothermally stable at high temperatures. However, significant oxidative degradation occurred already at moderate temperatures (above 70 °C). Temperatures above 120 °C lead to degradation in concentrated dry CO2. Adding moisture to the concentrated CO2 stream improves the CO2-induced stability. Adsorbent regeneration with nitrogen stripping is studied with various parameters, focusing on minimizing the moles of purge gas required per mole of CO2 desorbed.

  16. An overview of biological processes and their potential for CO2 capture.

    PubMed

    Goli, Amin; Shamiri, Ahmad; Talaiekhozani, Amirreza; Eshtiaghi, Nicky; Aghamohammadi, Nasrin; Aroua, Mohamed Kheireddine

    2016-12-01

    The extensive amount of available information on global warming suggests that this issue has become prevalent worldwide. Majority of countries have issued laws and policies in response to this concern by requiring their industrial sectors to reduce greenhouse gas emissions, such as CO2. Thus, introducing new and more effective treatment methods, such as biological techniques, is crucial to control the emission of greenhouse gases. Many studies have demonstrated CO2 fixation using photo-bioreactors and raceway ponds, but a comprehensive review is yet to be published on biological CO2 fixation. A comprehensive review of CO2 fixation through biological process is presented in this paper as biological processes are ideal to control both organic and inorganic pollutants. This process can also cover the classification of methods, functional mechanisms, designs, and their operational parameters, which are crucial for efficient CO2 fixation. This review also suggests the bio-trickling filter process as an appropriate approach in CO2 fixation to assist in creating a pollution-free environment. Finally, this paper introduces optimum designs, growth rate models, and CO2 fixation of microalgae, functions, and operations in biological CO2 fixation.

  17. Active CO2 Reservoir Management for Carbon Capture, Utilization, and Sequestration: Impact on Permitting, Monitoring, and Public Acceptance

    NASA Astrophysics Data System (ADS)

    Buscheck, T. A.; Chen, M.; Sun, Y.; Hao, Y.; Court, B.; Celia, M. A.; Wolery, T.; Aines, R. D.

    2011-12-01

    CO2 capture and sequestration (CCS) integrated with geothermal energy production in deep geological formations can play an important role in reducing CO2 emissions to the atmosphere and thereby mitigate global climate change. For industrial-scale CO2 injection in saline formations, pressure buildup can limit storage capacity and security. Active CO2 Reservoir Management (ACRM) combines brine production with CO2 injection to relieve pressure buildup, increase injectivity, manipulate CO2 migration, constrain brine leakage, and enable beneficial utilization of produced brine. Therefore, ACRM can be an enabler of carbon capture, utilization, and sequestration (CCUS). Useful products may include freshwater, cooling water, make-up water for pressure support in oil, gas, and geothermal reservoir operations, and geothermal energy production. Implementation barriers to industrial-scale CCS include concerns about (1) CO2 sequestration security and assurance, (2) pore-space competition with neighboring subsurface activities, (3) CO2 capture costs, and (4) water-use demands imposed by CCS operations, which is particularly important where water resources are already scarce. CCUS, enabled by ACRM, has the potential of addressing these barriers. Pressure relief from brine production can substantially reduce the driving force for potential CO2 and brine migration, as well as minimize interference with neighboring subsurface activities. Electricity generated from geothermal energy can offset a portion of the parasitic energy and financial costs of CCS. Produced brine can be used to generate freshwater by desalination technologies, such as RO, provide a source for saltwater cooling systems or be used as make-up water for oil, gas, or geothermal reservoir operations, reducing the consumption of valuable freshwater resources. We examine the impact of brine production on reducing CO2 and brine leakage. A volumetric balance between injected and produced fluids minimizes the spatial

  18. The role of zinc(II) in the absorption-desorption of CO2 by aqueous NH3, a potentially cost-effective method for CO2 capture and recycling.

    PubMed

    Mani, Fabrizio; Peruzzini, Maurizio; Barzagli, Francesco

    2008-01-01

    The absorption of CO2 by aqueous NH3 solutions has been investigated at atmospheric pressure and 0 degrees C. The CO2 absorption is fast and occurs with high efficiency (88-99%). The maximum CO2-removal efficiency increases slightly with the NH3 concentration. Addition of zinc(II) salts (as chloride, nitrate or sulfate) to the NH3 absorbent solution increases the overall CO2-absorption capacity without appreciably affecting the removal efficiency. Stripping of pure CO2 from HCO3(-) solutions is achieved by adding the calculated amount of ZnII salts, which under ambient conditions lead to rapid release of about 30-35% of the initially captured CO2. At the same time, about 65-70% of the captured CO2 is transformed into solid basic zinc carbonates. The recovery of these valuable solid products and the release of only 1/3 of free CO2 at room temperature and pressure reduces the cost of the overall process of CO2 capture, making it a potentially attractive method for CO2 capture on a larger scale.

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

    NASA Astrophysics Data System (ADS)

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

    2012-10-01

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

  20. Steady-state simulation and optimization of an integrated gasification combined cycle power plant with CO2 capture

    SciTech Connect

    Bhattacharyya, D.; Turton, R.; Zitney, S.

    2011-01-01

    Integrated gasification combined cycle (IGCC) plants are a promising technology option for power generation with carbon dioxide (CO2) capture in view of their efficiency and environmental advantages over conventional coal utilization technologies. This paper presents a three-phase, top-down, optimization-based approach for designing an IGCC plant with precombustion CO2 capture in a process simulator environment. In the first design phase, important global design decisions are made on the basis of plant-wide optimization studies with the aim of increasing IGCC thermal efficiency and thereby making better use of coal resources and reducing CO2 emissions. For the design of an IGCC plant with 90% CO2 capture, the optimal combination of the extent of carbon monoxide (CO) conversion in the water-gas shift (WGS) reactors and the extent of CO2 capture in the SELEXOL process, using dimethylether of polyethylene glycol as the solvent, is determined in the first phase. In the second design phase, the impact of local design decisions is explored considering the optimum values of the decision variables from the first phase as additional constraints. Two decisions are made focusing on the SELEXOL and Claus unit. In the third design phase, the operating conditions are optimized considering the optimum values of the decision variables from the first and second phases as additional constraints. The operational flexibility of the plant must be taken into account before taking final design decisions. Two studies on the operational flexibility of the WGS reactors and one study focusing on the operational flexibility of the sour water stripper (SWS) are presented. At the end of the first iteration, after executing all the phases once, the net plant efficiency (HHV basis) increases to 34.1% compared to 32.5% in a previously published study (DOE/NETL-2007/1281; National Energy Technology Laboratory, 2007). The study shows that the three-phase, top-down design approach presented is very

  1. Assessing the Potential of Sepiolite-Palygorskite Group Minerals as Materials for CO2 Capture and Storage Applications

    NASA Astrophysics Data System (ADS)

    Wallace, A. F.

    2015-12-01

    The carbonation of magnesium silicate minerals within ultramafic rocks is one of the most promising routes to CO2 sequestration involving chemical reaction with natural materials. However, in practice the rate of magnesium silicate carbonation is very slow at ambient temperature. Although using smaller magnesium silicate grains with greater reactive surface area can enhance reaction rates, the coherency of ultramafic rock makes crushing the material an energy-consuming task in its own right. Instead of relying on a mineral forming reaction to capture carbon, it has been hypothesized that naturally occuring nanoporous materials may be used to capture and store carbon dioxide. Sepiolite-palygorskite clays are of interest because in addition to being common minerals in marine and lacustrine sediments, they are natural weathering products of ultramafic rocks, and are already used extensively in industrial scale applications. Due to the presence of nanoscopic channel structures in sepiolite-palygorskite clays these materials exhibit extremely high surface areas. However, in the native structure the channels are filled with water. In order for these minerals to act as efficient CO2 storage materials channel water must be displaced and replaced with CO2. Herein we present preliminary findings using molecular dynamics simulations to quantify the thermodynamic driving force for displacing channel bound water with CO2 and assess the feasibility of sepiolite-palygorskite clays to act as CO2 storage materials.

  2. Putting an ultrahigh concentration of amine groups into a metal-organic framework for CO2 capture at low pressures.

    PubMed

    Liao, Pei-Qin; Chen, Xun-Wei; Liu, Si-Yang; Li, Xu-Yu; Xu, Yan-Tong; Tang, Minni; Rui, Zebao; Ji, Hongbing; Zhang, Jie-Peng; Chen, Xiao-Ming

    2016-10-19

    Tremendous efforts have been devoted to increasing the CO2 capture performance of porous materials, especially for low CO2 concentration environments. Here, we report that hydrazine can be used as a diamine short enough to functionalize the small-pore metal-organic framework [Mg2(dobdc)] (H4dobdc = 2,5-dihydroxyl-1,4-benzenedicarboxylic acid). By virtue of the ultrahigh concentration of free amine groups (6.01 mmol g(-1) or 7.08 mmol cm(-3)) capable of reversible carbamic acid formation, the new material [Mg2(dobdc)(N2H4)1.8] achieves a series of new records for CO2 capture, such as single-component isotherm uptakes of 3.89 mmol g(-1) or 4.58 mmol cm(-3) at the atmospheric CO2 concentration of 0.4 mbar at 298 K and 1.04 mmol g(-1) or 1.22 mmol cm(-3) at 328 K, as well as more than a 4.2 mmol g(-1) or 4.9 mmol cm(-3) adsorption/desorption working capacity under dynamic mixed-gas conditions with CO2 concentrations similar to those in flue gases and ambient air.

  3. Flue-gas and direct-air capture of CO2 by porous metal-organic materials

    NASA Astrophysics Data System (ADS)

    Madden, David G.; Scott, Hayley S.; Kumar, Amrit; Chen, Kai-Jie; Sanii, Rana; Bajpai, Alankriti; Lusi, Matteo; Curtin, Teresa; Perry, John J.; Zaworotko, Michael J.

    2017-01-01

    Sequestration of CO2, either from gas mixtures or directly from air (direct air capture), is a technological goal important to large-scale industrial processes such as gas purification and the mitigation of carbon emissions. Previously, we investigated five porous materials, three porous metal-organic materials (MOMs), a benchmark inorganic material, Zeolite 13X and a chemisorbent, TEPA-SBA-15, for their ability to adsorb CO2 directly from air and from simulated flue-gas. In this contribution, a further 10 physisorbent materials that exhibit strong interactions with CO2 have been evaluated by temperature-programmed desorption for their potential utility in carbon capture applications: four hybrid ultramicroporous materials, SIFSIX-3-Cu, DICRO-3-Ni-i, SIFSIX-2-Cu-i and MOOFOUR-1-Ni; five microporous MOMs, DMOF-1, ZIF-8, MIL-101, UiO-66 and UiO-66-NH2; an ultramicroporous MOM, Ni-4-PyC. The performance of these MOMs was found to be negatively impacted by moisture. Overall, we demonstrate that the incorporation of strong electrostatics from inorganic moieties combined with ultramicropores offers improved CO2 capture performance from even moist gas mixtures but not enough to compete with chemisorbents. This article is part of the themed issue 'Coordination polymers and metal-organic frameworks: materials by design'.

  4. Flue-gas and direct-air capture of CO2 by porous metal-organic materials.

    PubMed

    Madden, David G; Scott, Hayley S; Kumar, Amrit; Chen, Kai-Jie; Sanii, Rana; Bajpai, Alankriti; Lusi, Matteo; Curtin, Teresa; Perry, John J; Zaworotko, Michael J

    2017-01-13

    Sequestration of CO2, either from gas mixtures or directly from air (direct air capture), is a technological goal important to large-scale industrial processes such as gas purification and the mitigation of carbon emissions. Previously, we investigated five porous materials, three porous metal-organic materials (MOMs), a benchmark inorganic material, ZEOLITE 13X: and a chemisorbent, TEPA-SBA-15: , for their ability to adsorb CO2 directly from air and from simulated flue-gas. In this contribution, a further 10 physisorbent materials that exhibit strong interactions with CO2 have been evaluated by temperature-programmed desorption for their potential utility in carbon capture applications: four hybrid ultramicroporous materials, SIFSIX-3-CU: , DICRO-3-NI-I: , SIFSIX-2-CU-I: and MOOFOUR-1-NI: ; five microporous MOMs, DMOF-1: , ZIF-8: , MIL-101: , UIO-66: and UIO-66-NH2: ; an ultramicroporous MOM, NI-4-PYC: The performance of these MOMs was found to be negatively impacted by moisture. Overall, we demonstrate that the incorporation of strong electrostatics from inorganic moieties combined with ultramicropores offers improved CO2 capture performance from even moist gas mixtures but not enough to compete with chemisorbents.This article is part of the themed issue 'Coordination polymers and metal-organic frameworks: materials by design'.

  5. Comparison of Solvation Effects on CO2 Capture with Aqueous Amine Solutions and Amine-Functionalized Ionic Liquids.

    PubMed

    Yamada, Hidetaka

    2016-10-13

    Amines are the most widely utilized chemicals for postcombustion CO2 capture, because the reversible reactions between amines and CO2 through their moderate interaction allow effective "catch and release". Usually, CO2 is dissolved in the form of an anion such as carbamate or bicarbonate. Therefore, the reaction energy diagram is potentially governed to a large extent by the polarity of the surrounding solvent. Herein, we compared aqueous amine solutions and amine-functionalized ionic liquids by investigating their dielectric constants and performing an intrinsic reaction coordinate analysis of the CO2 absorption process. Quantum mechanical calculations at the CCSD(T)/6-311++G(d,p)//B3LYP/6-311++G(d,p) level within the continuum solvation model (SMD/IEF-PCM) revealed contrasting dependencies of C-N bond formation on the dielectric constant in those solutions. Amines react with CO2 on an energy surface that is significantly affected by the dielectric constant in conventional aqueous amine solutions, whereas amine-functionalized anions and CO2 form stable C-N bonds with a comparatively lower activation energy regardless of the dielectric constant.

  6. CO2 leakage from carbon dioxide capture and storage (CCS) systems affects organic matter cycling in surface marine sediments.

    PubMed

    Rastelli, Eugenio; Corinaldesi, Cinzia; Dell'Anno, Antonio; Amaro, Teresa; Greco, Silvestro; Lo Martire, Marco; Carugati, Laura; Queirós, Ana M; Widdicombe, Stephen; Danovaro, Roberto

    2016-12-01

    Carbon dioxide capture and storage (CCS), involving the injection of CO2 into the sub-seabed, is being promoted worldwide as a feasible option for reducing the anthropogenic CO2 emissions into the atmosphere. However, the effects on the marine ecosystems of potential CO2 leakages originating from these storage sites have only recently received scientific attention, and little information is available on the possible impacts of the resulting CO2-enriched seawater plumes on the surrounding benthic ecosystem. In the present study, we conducted a 20-weeks mesocosm experiment exposing coastal sediments to CO2-enriched seawater (at 5000 or 20,000 ppm), to test the effects on the microbial enzymatic activities responsible for the decomposition and turnover of the sedimentary organic matter in surface sediments down to 15 cm depth. Our results indicate that the exposure to high-CO2 concentrations reduced significantly the enzymatic activities in the top 5 cm of sediments, but had no effects on subsurface sediment horizons (from 5 to 15 cm depth). In the surface sediments, both 5000 and 20,000 ppm CO2 treatments determined a progressive decrease over time in the protein degradation (up to 80%). Conversely, the degradation rates of carbohydrates and organic phosphorous remained unaltered in the first 2 weeks, but decreased significantly (up to 50%) in the longer term when exposed at 20,000 ppm of CO2. Such effects were associated with a significant change in the composition of the biopolymeric carbon (due to the accumulation of proteins over time in sediments exposed to high-pCO2 treatments), and a significant decrease (∼20-50% at 5000 and 20,000 ppm respectively) in nitrogen regeneration. We conclude that in areas immediately surrounding an active and long-lasting leak of CO2 from CCS reservoirs, organic matter cycling would be significantly impacted in the surface sediment layers. The evidence of negligible impacts on the deeper sediments should be considered with

  7. Ship-in-a-bottle synthesis of amine-functionalized ionic liquids in NaY zeolite for CO2 capture

    PubMed Central

    Yu, Yinghao; Mai, Jingzhang; Wang, Lefu; Li, Xuehui; Jiang, Zheng; Wang, Furong

    2014-01-01

    CO2 capture on solid materials possesses significant advantages on the operation cost, process for large-scale CO2 capture and storage (CCS) that stimulates great interest in exploring high-performance solid CO2 adsorbents. A ship-in-a-bottle strategy was successfully developed to prepare the [APMIM]Br@NaY host–guest system in which an amine-functionalized ionic liquid (IL), 1-aminopropyl-3-methylimidazolium bromide ([APMIM]Br), was in-situ encapsulated in the NaY supercages. The genuine host-guest systems were thoroughly characterized and tested in CO2 capture from simulated flue gas. It was evidenced the encapsulated ILs are more stable than the bulk ILs. These host–guest systems exhibited superb overall CO2 capture capacity up to 4.94 mmol g−1 and the chemically adsorbed CO2 achieved 1.85 mmol g−1 depending on the [APMIM]Br loading amount. The chemisorbed CO2 can be desorbed rapidly by flushing with N2 gas at 50°C. The optimized [APMIM]Br@NaY system remains its original CO2 capture capacity in multiple cycling tests under prolonged harsh adsorption-desorption conditions. The excellent physicochemical properties and the CO2 capture performance of the host-guest systems offer them great promise for the future practice in the industrial CO2 capture. PMID:25104324

  8. Ship-in-a-bottle synthesis of amine-functionalized ionic liquids in NaY zeolite for CO2 capture.

    PubMed

    Yu, Yinghao; Mai, Jingzhang; Wang, Lefu; Li, Xuehui; Jiang, Zheng; Wang, Furong

    2014-08-08

    CO2 capture on solid materials possesses significant advantages on the operation cost, process for large-scale CO2 capture and storage (CCS) that stimulates great interest in exploring high-performance solid CO2 adsorbents. A ship-in-a-bottle strategy was successfully developed to prepare the [APMIM]Br@NaY host-guest system in which an amine-functionalized ionic liquid (IL), 1-aminopropyl-3-methylimidazolium bromide ([APMIM]Br), was in-situ encapsulated in the NaY supercages. The genuine host-guest systems were thoroughly characterized and tested in CO2 capture from simulated flue gas. It was evidenced the encapsulated ILs are more stable than the bulk ILs. These host-guest systems exhibited superb overall CO2 capture capacity up to 4.94 mmol g(-1) and the chemically adsorbed CO2 achieved 1.85 mmol g(-1) depending on the [APMIM]Br loading amount. The chemisorbed CO2 can be desorbed rapidly by flushing with N2 gas at 50 °C. The optimized [APMIM]Br@NaY system remains its original CO2 capture capacity in multiple cycling tests under prolonged harsh adsorption-desorption conditions. The excellent physicochemical properties and the CO2 capture performance of the host-guest systems offer them great promise for the future practice in the industrial CO2 capture.

  9. Co-location of air capture, sub-ocean CO2 storage and energy production on the Kerguelen plateau

    NASA Astrophysics Data System (ADS)

    Goldberg, D.; Han, P.; Lackner, K.; Wang, T.

    2011-12-01

    How can carbon capture and storage activities be sustained from an energy perspective while keeping the entire activity out of sight and away from material risk and social refrain near populated areas? In light of reducing the atmospheric CO2 level to mitigate its effect on climate change, the combination of new air-capture technologies and large offshore storage reservoirs, supplemented by carbon neutral renewable energy, could address both of these engineering and public policy concerns. Because CO2 mixes rapidly in the atmosphere, air capture scrubbers could be located anywhere in the world. Although the power requirements for this technology may reduce net efficiencies, the local availability of carbon-neutral renewable energy for this purpose would eliminate some net energy loss. Certain locations where wind speeds are high and steady, such as those observed at high latitude and across the open ocean, appeal as carbon-neutral energy sources in close proximity to immense and secure reservoirs for geological sequestration of captured CO2. In particular, sub-ocean basalt flows are vast and carry minimal risks of leakage and damages compared to on-land sites. Such implementation of a localized renewable energy source coupled with carbon capture and storage infrastructure could result in a global impact of lowered CO2 levels. We consider an extreme location on the Kerguelen plateau in the southern Indian Ocean, where high wind speeds and basalt storage reservoirs are both plentiful. Though endowed with these advantages, this mid-ocean location incurs clear material and economic challenges due to its remoteness and technological challenges for CO2 capture due to constant high humidity. We study the wind energy-air capture power balance and consider related factors in the feasibility of this location for carbon capture and storage. Other remote oceanic sites where steady winds blow and near large geological reservoirs may be viable as well, although all would require

  10. Poly(ionic liquid)/Ionic Liquid Ion-Gels with High "Free" Ionic Liquid Content: Platform Membrane Materials for CO2/Light Gas Separations.

    PubMed

    Cowan, Matthew G; Gin, Douglas L; Noble, Richard D

    2016-04-19

    -films (ca. 100-nm-thick active layer). Traditional polymeric membrane materials are limited by a trade-off between permeability and selectivity empirically described by the "Robeson upper bound"-placing the desired membrane properties beyond reach. Therefore, the investigation of advanced and composite materials that can overcome the limitations of traditional polymeric materials is the focus of significant academic and industrial research. In particular, there has been substantial work on ionic-liquid (IL)-based materials due to their gas transport properties. This review provides an overview of our collaborative work on developing poly(ionic liquid)/ionic liquid (PIL/IL) ion-gel membrane technology. We detail developmental work on the preparation of PIL/IL composites and describe how this chemical technology was adapted to allow the roll-to-roll processing and preparation of membranes with defect-free active layers ca. 100 nm thick, CO2 permeances of over 6000 GPU, and CO2/N2 selectivity of ≥20-properties with the potential to reduce the cost of CO2 removal from coal-fired power plant flue gas to ca. $15 per ton of CO2 captured. Additionally, we examine the materials developments that have produced advanced PIL/IL composite membranes. These advancements include cross-linked PIL/IL blends, step-growth PIL/IL networks with facilitated transport groups, and PIL/IL composites with microporous additives for CO2/CH4 separations.

  11. Development of nitrogen enriched nanostructured carbon adsorbents for CO2 capture.

    PubMed

    Goel, Chitrakshi; Bhunia, Haripada; Bajpai, Pramod K

    2015-10-01

    Nanostructured carbon adsorbents containing high nitrogen content were developed by templating melamine-formaldehyde resin in the pores of mesoporous silica by nanocasting technique. A series of adsorbents were prepared by altering the carbonization temperature from 400 to 700 °C and characterized in terms of their textural and morphological properties. CO2 adsorption performance was investigated at various temperatures from 30 to 100 °C by using a thermogravimetric analyzer under varying CO2 concentrations. Multiple adsorption-desorption experiments were also carried out to investigate the adsorbent regenerability. X-ray diffraction (XRD) and transmission electron microscopy (TEM) confirmed the development of nanostructured materials. Fourier transform infrared spectroscopy (FTIR) and elemental analysis indicated the development of carbon adsorbents having high nitrogen content. The surface area and pore volume of the adsorbent carbonized at 700 °C were found to be 266 m(2) g(-1) and 0.25 cm(3) g(-1) respectively. CO2 uptake profile for the developed adsorbents showed that the maximum CO2 adsorption occurred within ca. 100 s. CO2 uptake of 0.792 mmol g(-1) at 30 °C was exhibited by carbon obtained at 700 °C with complete regenerability in three adsorption-desorption cycles. Furthermore, kinetics of CO2 adsorption on the developed adsorbents was studied by fitting the experimental data of CO2 uptake to three kinetic models with best fit being obtained by fractional order kinetic model with error% within range of 5%. Adsorbent surface was found to be energetically heterogeneous as suggested by Temkin isotherm model. Also the isosteric heat of adsorption for CO2 was observed to increase from ca. 30-44 kJ mol(-1) with increase in surface coverage.

  12. CO2-laser isotope separation of tritium with pentafluoroethane-T (C2TF5)

    NASA Astrophysics Data System (ADS)

    Makide, Y.; Kato, S.; Tominaga, T.; Takeuchi, K.

    1982-08-01

    Isotope separation of tritium by CO2 laser-induced multiphoton dissociation (MPD) of C2TF5 is reported for the first time. The MPD spectrum obtained for C2TF5 comprised a broad peak at about 940 cm-1 where C2HF5 was nearly transparent. The unimolecular dissociation of C2TF5 was induced with much lower laser fluence than that for CTF3, another working molecule we proposed for laser isotope separation of tritium. The mechanisms and kinetics of the dissociation of C2TF5 and C2HF5 were investigated under various experimental conditions: laser frequency, pulse energy, pulse duration, tritium concentration, sample pressure, buffer gas pressure and irradiation geometry. Single-step separation factors exceeding 500 were achieved with the most efficient P(20) line in 00o 10o0 transition at 944.2 cm-1.

  13. Comparison of numerical predictions with CO2 pipeline release datasets of relevance to carbon capture and storage applications

    NASA Astrophysics Data System (ADS)

    Wareing, Christopher J.; Fairweather, Michael; Woolley, Robert M.; Falle, S. A. E. G.

    2015-12-01

    Predicting the correct multi-phase fluid flow behaviour during the discharge process in the near-field of sonic CO2 jets is of particular importance in assessing the risks associated with transport aspects of carbon capture and storage schemes, given the very different hazard profiles of CO2 in the gaseous and solid states. In this paper, we apply our state-of-the-art mathematical model implemented in an efficient computational method to available data. Compared to previous applications, an improved equation of state is used. We also compare to all the available data, rather than just subsets as previously, and demonstrate both the improved performance of the fluid flow model and the variation between the available datasets. The condensed phase fraction at the vent, puncture or rupture release point is revealed to be of key importance in understanding the near-field dispersion of sonic CO2.

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

    PubMed Central

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

    2016-01-01

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

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

    PubMed

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

    2016-01-01

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

  16. New Solid-Base Cu-MgO for CO2 Capture at 473 K and Removal of Nitrosamine.

    PubMed

    Li, Yan Y; Dong, Xin Y M; Sun, Xiao D; Wang, Ying; Zhu, Jian H

    2016-11-09

    To fabricate a new solid base with high efficiency in the adsorption of CO2 at 473 K and catalytic activity in the degradation of nitrosamines, magnesium oxalate and copper nitrate are mixed with the assistance of microwave irradiation followed by calcination to immobilize CuO among MgO particles. The binary solid base CuO-MgO is thus moderately reduced to form the Cu-inserted MgO composite with highly exposed strong basic sites, and it can capture 34.6 mg g(-1) of CO2 in the harsh instantaneous adsorption at 473 K and keep a high strong basicity while trapping the CO2 mixed with SO2 and NO. Besides this, the new solid base exhibits high activity in the removal of volatile nitrosamine N-nitrosopyrrolidine (NPYR), for the first time expanding the application of solid bases to environmental catalysis.

  17. Extractive separation of Cu2+-Co2+ and Ni2+-Co2+ mixtures using N-salicylideneaniline

    NASA Astrophysics Data System (ADS)

    Yamina, Boukraa

    2016-12-01

    A study on the extraction of copper(II), cobalt(II), and nickel(II) from solutions containing ions of both metals with N-salicylideneaniline(SAN) in chloroform has been realized. Distribution of the metal ions in wide range of pH has been studied. Extraction of copper(II) was always favored over that of cobalt(II). Extraction of copper(II) from binary metal solution is selective and it can be quantitatively separated from cobalt(II). The equilibrium constant of the extraction of cobalt and nickel from an aqueous solution containing both metals using SAN were evaluated. The separation factors for cobalt and nickel were expressed as a function of the distribution of nickel and cobalt. From these results, salicylideneaniline is an adequate extractant for extractive separation of such mixtures.

  18. CO2 Separation Using Thermally Optimized Membranes: A Comprehensive Project Report (2000 - 2007)

    SciTech Connect

    J.R. Klaehn; C.J. Orme; E.S. Peterson; T.A. Luther; M.G. Jones; A.K. Wertsching

    2008-03-01

    This is a complete (Fiscal Years 2000–2006) collection of the Idaho National Laboratory’s (INL) research and development contributions to the project, “CO2 Separation Using Thermally Optimized Membranes.” The INL scientific contribution to the project has varied due to the fluctuations in funding from year to year. The focus of the project was polybenzimidazole (PBI) membranes and developing PBI compounds (both substitution and blends) that provide good film formation and gas separation membranes. The underlying problem with PBI is its poor solubility in common solvents. Typically, PBI is dissolved in “aggressive” solvents, like N,N-dimethylacetamide (DMAc) and N methylpyrrolidone (NMP). The INL FY-03 research was directed toward making soluble N-substituted PBI polymers, where INL was very successful. Many different types of modified PBI polymers were synthesized; however, film formation proved to be a big problem with both unsubstituted and N-substituted PBIs. Therefore, INL researchers directed their attention to using plasticizers or additives to make the membranes more stable and workable. During the course of these studies, other high-performance polymers (like polyamides and polyimides) were found to be better materials, which could be used either by themselves or blends with PBI. These alternative high-performance polymers provided the best pathway forward for soluble high-temperature polymers with good stable film formation properties. At present, the VTEC polyimides (product of RBI, Inc.) are the best film formers that exhibit high-temperature resistance. INL’s gas testing results show VTEC polyimides have very good gas selectivities for both H2/CO2 and CO2/CH4. Overall, these high-performance polymers pointed towards new research areas where INL has gained a greater understanding of polymer film formation and gas separation. These studies are making possible a direct approach to stable polymer-based high-temperature gas separation membranes

  19. CO2 Separation Using Thermally Optimized Membranes: A Comprehensive Project Report (2000 - 2007)

    SciTech Connect

    N /A

    2008-03-04

    This is a complete (Fiscal Years 2000–2006) collection of the Idaho National Laboratory’s (INL) research and development contributions to the project, “CO2 Separation Using Thermally Optimized Membranes.” The INL scientific contribution to the project has varied due to the fluctuations in funding from year to year. The focus of the project was polybenzimidazole (PBI) membranes and developing PBI compounds (both substitution and blends) that provide good film formation and gas separation membranes. The underlying problem with PBI is its poor solubility in common solvents. Typically, PBI is dissolved in “aggressive” solvents, like N,N-dimethylacetamide (DMAc) and N methylpyrrolidone (NMP). The INL FY-03 research was directed toward making soluble N-substituted PBI polymers, where INL was very successful. Many different types of modified PBI polymers were synthesized; however, film formation proved to be a big problem with both unsubstituted and N-substituted PBIs. Therefore, INL researchers directed their attention to using plasticizers or additives to make the membranes more stable and workable. During the course of these studies, other high-performance polymers (like polyamides and polyimides) were found to be better materials, which could be used either by themselves or blends with PBI. These alternative high-performance polymers provided the best pathway forward for soluble high-temperature polymers with good stable film formation properties. At present, the VTEC polyimides (product of RBI, Inc.) are the best film formers that exhibit high-temperature resistance. INL’s gas testing results show VTEC polyimides have very good gas selectivities for both H2/CO2 and CO2/CH4. Overall, these high-performance polymers pointed towards new research areas where INL has gained a greater understanding of polymer film formation and gas separation. These studies are making possible a direct approach to stable polymer-based high-temperature gas separation membranes

  20. Azine-Linked Covalent Organic Framework (COF)-Based Mixed-Matrix Membranes for CO2 /CH4 Separation.

    PubMed

    Shan, Meixia; Seoane, Beatriz; Rozhko, Elena; Dikhtiarenko, Alla; Clet, Guillaume; Kapteijn, Freek; Gascon, Jorge

    2016-10-04

    Mixed-matrix membranes (MMMs) comprising Matrimid and a microporous azine-linked covalent organic frameworks (ACOF-1) were prepared and tested in the separation of CO2 from an equimolar CO2 /CH4 mixture. The COF-based MMMs show a more than doubling of the CO2 permeability upon 16 wt % ACOF-1 loading together with a slight increase in selectivity compared to the bare polymer. These results show the potential of COFs in the preparation of MMMs.

  1. Sustainable and hierarchical porous Enteromorpha prolifera based carbon for CO2 capture.

    PubMed

    Zhang, Zhanquan; Wang, Ke; Atkinson, John D; Yan, Xinlong; Li, Xiang; Rood, Mark J; Yan, Zifeng

    2012-08-30

    Nitrogen-containing porous carbon was synthesized from an ocean pollutant, Enteromorpha prolifera, via hydrothermal carbonization and potassium hydroxide activation. Carbons contained as much as 2.6% nitrogen in their as-prepared state. Physical and chemical properties were characterized by XRD, N(2) sorption, FTIR, SEM, TEM, and elemental analysis. The carbon exhibited a hierarchical structure with interconnected microporosity, mesoporosity and macroporosity. Inorganic minerals in the carbon matrix contributed to the development of mesoporosity and macroporosity, functioning as an in situ hard template. The carbon manifested high CO(2) capacity and facile regeneration at room temperature. The CO(2) sorption performance was investigated in the range of 0-75°C. The dynamic uptake of CO(2) is 61.4 mg/g and 105 mg/g at 25°C and 0°C, respectively, using 15% CO(2) (v/v) in N(2). Meanwhile, regeneration under Ar at 25°C recovered 89% of the carbon's initial uptake after eight cycles. A piecewise model was employed to analyze the CO(2) adsorption kinetics; the Avrami model fit well with a correlation coefficient (R(2)) of 0.98 and 0.99 at 0°C and 25°C, respectively.

  2. Carbon Dioxide Capture and Separation Techniques for Gasification-based Power Generation Point Sources

    SciTech Connect

    Pennline, H.W.; Luebke, D.R.; Jones, K.L.; Morsi, B.I.; Heintz, Y.J.; Ilconich, J.B.

    2007-06-01

    The capture/separation step for carbon dioxide (CO2) from large-point sources is a critical one with respect to the technical feasibility and cost of the overall carbon sequestration scenario. For large-point sources, such as those found in power generation, the carbon dioxide capture techniques being investigated by the in-house research area of the National Energy Technology Laboratory possess the potential for improved efficiency and reduced costs as compared to more conventional technologies. The investigated techniques can have wide applications, but the research has focused on capture/separation of carbon dioxide from flue gas (post-combustion from fossil fuel-fired combustors) and from fuel gas (precombustion, such as integrated gasification combined cycle or IGCC). With respect to fuel gas applications, novel concepts are being developed in wet scrubbing with physical absorption; chemical absorption with solid sorbents; and separation by membranes. In one concept, a wet scrubbing technique is being investigated that uses a physical solvent process to remove CO2 from fuel gas of an IGCC system at elevated temperature and pressure. The need to define an ideal solvent has led to the study of the solubility and mass transfer properties of various solvents. Pertaining to another separation technology, fabrication techniques and mechanistic studies for membranes separating CO2 from the fuel gas produced by coal gasification are also being performed. Membranes that consist of CO2-philic ionic liquids encapsulated into a polymeric substrate have been investigated for permeability and selectivity. Finally, dry, regenerable processes based on sorbents are additional techniques for CO2 capture from fuel gas. An overview of these novel techniques is presented along with a research progress status of technologies related to membranes and physical solvents.

  3. Tuning cooperativity by controlling the linker length of silica-supported amines in catalysis and CO2 capture.

    PubMed

    Brunelli, Nicholas A; Didas, Stephanie A; Venkatasubbaiah, Krishnan; Jones, Christopher W

    2012-08-29

    Cooperative interactions between aminoalkylsilanes and silanols on a silica surface can be controlled by varying the length of the alkyl linker attaching the amine to the silica surface from C1 (methyl) to C5 (pentyl). The linker length strongly affects the catalytic cooperativity of amines and silanols in aldol condensations as well as the adsorptive cooperativity for CO(2) capture. The catalytic cooperativity increases with the linker length up to propyl (C3), with longer, more flexible linkers (up to C5) providing no additional benefit or hindrance. Short linkers (C1 and C2) limit the beneficial amine-silanol cooperativity in aldol condensations, resulting in lower catalytic rates than with the C3+ linkers. For the same materials, the adsorptive cooperativity exhibits similar trends for CO(2) capture efficiency.

  4. Modified dolomite in biomass gasification with simultaneous tar reformation and CO2 capture: effect of metal loading

    NASA Astrophysics Data System (ADS)

    Di Felice, L.; Courson, C.; Foscolo, P. U.; Kiennemann, A.

    2011-03-01

    The CO2 absorption capacity of calcined dolomite [a (CaMg)O solid solution] doped with iron and nickel transition metals has been investigated in a fixed bed reactor operating at temperature conditions (650°C) at which the sorption process is thermodynamically favoured at ambient pressure. The presence of metals (catalytic sites) between CaO grains (CO2 absorption sites) may improve the potential of dolomite for the simultaneous process of catalytic tar reforming and CO2 capture in biomass gasification, with the aim of developing an effective combined catalyst and sorbent particle. It was found that iron and nickel may be optimised in the substrate reducing critical limitations on CO2 capture capacity. A Sorption Enhanced Reforming test is proposed, at 650°C, for both iron and nickel doped calcined dolomite, using toluene as model tar compound: iron has been found to be not active in such conditions, whereas the 4% Ni/(CaMg)O has been indicated as the most suitable combined catalyst and sorbent particle.

  5. Enhanced photo-H2 production of R. faecalis RLD-53 by separation of CO2 from reaction system.

    PubMed

    Liu, Bing-Feng; Ren, Nan-Qi; Ding, Jie; Xie, Guo-Jun; Cao, Guang-Li

    2009-02-01

    The effect of different gases, CO(2) concentration, and separation of CO(2) from reaction system on photo-fermentation H(2) production was investigated by batch culture in this study. Experimental results showed that different gases (Ar,N(2),CO(2), and air) as gas phase have obviously affected on photo-H(2) production and a high concentration of CO(2) can inhibit the growth and H(2) evolution of Rhodopseudomonas faecalis RLD-53. When CO(2) concentration at 5%, cell increased most rapidly the specific growth rate of 0.489 g/l/h and the specific growth rate fell to be 0.265 g/l/h when CO(2) concentration at 40%. However, the growth of RLD-53 at CO(2) concentration of 60-100% was almost completely inhibited. At CO(2) concentrations of 5% and 10%, the maximum H(2) yield was 2.54 and 2.59 mol-H(2)/mol acetate, respectively, and it was similar with the control (2.61 mol-H(2)/mol acetate). H(2) not produced when CO(2) concentration at 60-100%. In conclusion, separation of CO(2) from reaction system can stimulate H(2) production in the entire photo-H(2) production process and H(2) yield increased about 12.8-18.85% than the control.

  6. Engineering the Cyanobacterial Carbon Concentrating Mechanism for Enhanced CO2 Capture and Fixation

    SciTech Connect

    Sandh, Gustaf; Cai, Fei; Shih, Patrick; Kinney, James; Axen, Seth; Salmeen, Annette; Zarzycki, Jan; Sutter, Markus; Kerfeld, Cheryl

    2011-06-02

    In cyanobacteria CO2 fixation is localized in a special proteinaceous organelle, the carboxysome. The CO2 fixation enzymes are encapsulated by a selectively permeable protein shell. By structurally and functionally characterizing subunits of the carboxysome shell and the encapsulated proteins, we hope to understand what regulates the shape, assembly and permeability of the shell, as well as the targeting mechanism and organization of the encapsulated proteins. This knowledge will be used to enhance CO2 fixation in both cyanobacteria and plants through synthetic biology. The same strategy can also serve as a template for the production of modular synthetic bacterial organelles. Our research is conducted using a variety of techniques such as genomic sequencing and analysis, transcriptional regulation, DNA synthesis, synthetic biology, protein crystallization, Small Angle X-ray Scattering (SAXS), protein-protein interaction assays and phenotypic characterization using various types of cellular imaging, e.g. fluorescence microscopy, Transmission Electron Microscopy (TEM), and Soft X-ray Tomography (SXT).

  7. Fast and reversible direct CO2 capture from air onto all-polymer nanofibrillated cellulose-polyethylenimine foams.

    PubMed

    Sehaqui, Houssine; Gálvez, María Elena; Becatinni, Viola; cheng Ng, Yi; Steinfeld, Aldo; Zimmermann, Tanja; Tingaut, Philippe

    2015-03-03

    Fully polymeric and biobased CO2 sorbents composed of oxidized nanofibrillated cellulose (NFC) and a high molar mass polyethylenimine (PEI) have been prepared via a freeze-drying process. This resulted in NFC/PEI foams displaying a sheet structure with porosity above 97% and specific surface area in the range 2.7-8.3 m(2)·g(-1). Systematic studies on the impact of both PEI content and relative humidity on the CO2 capture capacity of the amine functionalized sorbents have been conducted under atmospheric conditions (moist air with ∼400 ppm of CO2). At 80% RH and an optimum PEI content of 44 wt %, a CO2 capacity of 2.22 mmol·g(-1), a stability over five cycles, and an exceptionally low adsorption half time of 10.6 min were achieved. In the 20-80% RH range studied, the increase in relative humidity increased CO2 capacity of NFC/PEI foams at the expense of a high H2O uptake in the range 3.8-28 mmol·g(-1).

  8. Aminosilane-Grafted Zirconia-Titiania-Silica Nanoparticles/Torlon Hollow Fiber Composites for CO2 Capture.

    PubMed

    Rownaghi, Ali A; Kant, Amit; Li, Xin; Thakkar, Harshul; Hajari, Amit; He, Yingxin; Brennan, Patrick J; Hosseini, Hooman; Koros, William J; Rezaei, Fateme

    2016-05-23

    In this work, the development of novel binary and ternary oxide/Torlon hollow fiber composites comprising zirconia, titania, and silica as amine supports was demonstrated. The resulting binary (Zr-Si/PAI-HF, Ti-Si/PAI-HF) and ternary (Zr-Ti-Si/PAI-HF) composites were then functionalized with monoamine-, diamine-, and triamine-substituted trialkoxysilanes and were evaluated in CO2 capture. Although the introduction of both Zr and Ti improved the CO2 adsorption capacity relative to that with Si/PAI-HF sorbents, zirconia was found to have a more favorable effect on the CO2 adsorption performance than titania, as previously demonstrated for amine sorbents in the powder form. The Zr-Ti-Si/PAI-HF sample with an oxide content of 20 wt % was found to exhibit a relatively high CO2 capacity, that is, 1.90 mmol g(-1) at atmospheric pressure under dry conditions, owing to more favorable synergy between the metal oxides and CO2 . The ternary fiber sorbent showed improved sorption kinetics and long-term stability in cyclic adsorption/desorption runs.

  9. Advancing adsorption and membrane separation processes for the gigaton carbon capture challenge.

    PubMed

    Wilcox, Jennifer; Haghpanah, Reza; Rupp, Erik C; He, Jiajun; Lee, Kyoungjin

    2014-01-01

    Reducing CO2 in the atmosphere and preventing its release from point-source emitters, such as coal and natural gas-fired power plants, is a global challenge measured in gigatons. Capturing CO2 at this scale will require a portfolio of gas-separation technologies to be applied over a range of applications in which the gas mixtures and operating conditions will vary. Chemical scrubbing using absorption is the current state-of-the-art technology. Considerably less attention has been given to other gas-separation technologies, including adsorption and membranes. It will take a range of creative solutions to reduce CO2 at scale, thereby slowing global warming and minimizing its potential negative environmental impacts. This review focuses on the current challenges of adsorption and membrane-separation processes. Technological advancement of these processes will lead to reduced cost, which will enable subsequent adoption for practical scaled-up application.

  10. CO2 Capture Using 2,2-Dialkylpropane-1,3-diamines

    SciTech Connect

    O'Brien, MJ; Farnum, RL; Perry, RJ

    2013-01-01

    A series of 2,2-dialkylpropane-1,3-diamines were synthesized and evaluated as potential phase-changing CO2 sorbents. In general, these compounds readily absorbed CO2 to form solid carbamate salts, which were relatively insensitive to the presence of moisture. This is one of the key performance attributes phase-changing sorbents must possess. However, these diamines were found to be less thermally stable in air than expected. The main reaction products obtained during heat aging at 150 degrees C appeared to be 1,4,5,6-tetrahydropyrimidine derivatives.

  11. Potentiel des méthodes de séparation et stockage du CO2 dans la lutte contre l'effet de serreThe role of CO2 capture and sequestration in mitigation of climate change

    NASA Astrophysics Data System (ADS)

    Jean-Baptiste, Philippe; Ducroux, René

    2003-06-01

    Increasing atmospheric level of greenhouse gases are causing global warming and putting at risk the global climate system. The main anthropogenic greenhouse gas is CO 2. Technical solutions exist to reduce CO 2 emission and stabilise atmospheric CO 2 concentration, including energy saving and energy efficiency, switch to lower carbon content fuels like natural gas and to energy sources that operate with zero CO 2 emissions such as renewable or nuclear energy, enhance the natural sinks for CO 2 (forests, soils, etc.), and last but not least, sequester CO 2 from fossil fuels combustion. The purpose of this paper is to provide an overview of the technology and cost for capture and storage of CO 2. Some of the factors that will influence application, including environmental impact, cost and efficiency, are also discussed. Capturing CO 2 and storing it in underground geological reservoirs appears as the best environmentally acceptable option. It can be done with existing technology; however, substantial R&D is needed to improve available technology and to lower the cost. Applicable to large CO 2 emitting industrial facilities such as power plants, cement factories, steel industry, etc., which amount to more than 30% of the global anthropogenic CO 2 emission, it represents a valuable tool in the battle against global warming. To cite this article: P. Jean-Baptiste, R. Ducroux, C. R. Geoscience 335 (2003).

  12. Enhanced CO2 capture in binary mixtures of 1-alkyl-3-methylimidazolium tricyanomethanide ionic liquids with water.

    PubMed

    Romanos, George E; Zubeir, Lawien F; Likodimos, Vlassis; Falaras, Polycarpos; Kroon, Maaike C; Iliev, Boyan; Adamova, Gabriela; Schubert, Thomas J S

    2013-10-10

    Absorption of carbon dioxide and water in 1-butyl-3-methylimidazoliun tricyanomethanide ([C4C1im][TCM]) and 1-octyl-3-methylimidazolium tricyanomethanide ([C8C1im][TCM]) ionic liquids (ILs) was systematically investigated for the first time as a function of the H2O content by means of a gravimetric system together with in-situ Raman spectroscopy, excess molar volume (V(E)), and viscosity deviation measurements. Although CO2 absorption was marginally affected by water at low H2O molar fractions for both ILs, an increase of the H2O content resulted in a marked enhancement of both the CO2 solubility (ca. 4-fold) and diffusivity (ca. 10-fold) in the binary [C(n)C1im][TCM]/H2O systems, in contrast to the weak and/or detrimental influence of water in most physically and chemically CO2-absorbing ILs. In-situ Raman spectroscopy on the IL/CO2 systems verified that CO2 is physically absorbed in the dry ILs with no significant effect on their structural organization. A pronounced variation of distinct tricyanomethanide Raman modes was disclosed in the [C(n)C1im][TCM]/H2O mixtures, attesting to the gradual disruption of the anion-cation coupling by the hydrogen-bonded water molecules to the [TCM](-) anions, in accordance with the positive excess molar volumes and negative viscosity deviations for the binary systems. Most importantly, CO2 absorption in the ILs/H2O mixtures at high water concentrations revealed that the [TCM](-) Raman modes tend to restore their original state for the heavily hydrated ILs, in qualitative agreement with the intriguing nonmonotonous transients of CO2 absorption kinetics unveiled by the gravimetric measurements for the hybrid solvents. A molecular exchange mechanism between CO2 in the gas phase and H2O in the liquid phase was thereby proposed to explain the enhanced CO2 absorption in the hybrid [C(n)C1im][TCM]//H2O solvents based on the subtle competition between the TCM-H2O and TCM-CO2 interactions, which renders these ILs very promising for CO2

  13. Capturing CO2 from Coal-Fired Power Plants: Challenges for a Comprehensive Strategy

    DTIC Science & Technology

    2008-08-15

    Carbon capture in an IGCC facility would happen before combustion, under pressure using a physical solvent (e.g., Selexol and Rectisol processes ...NOx), or particulate control on an existing facility. A simplified illustration of this process is provided in Figure 1. CRS-4 7 For a useful...Scottish Centre for Carbon Storage. Figure available at [http://www.geos.ed.ac.uk/ sccs/capture/postcombustion.html]. Post-combustion processes capture

  14. CO2 Capture in the Sustainable Wheat-Derived Activated Microporous Carbon Compartments

    NASA Astrophysics Data System (ADS)

    Hong, Seok-Min; Jang, Eunji; Dysart, Arthur D.; Pol, Vilas G.; Lee, Ki Bong

    2016-10-01

    Microporous carbon compartments (MCCs) were developed via controlled carbonization of wheat flour producing large cavities that allow CO2 gas molecules to access micropores and adsorb effectively. KOH activation of MCCs was conducted at 700 °C with varying mass ratios of KOH/C ranging from 1 to 5, and the effects of activation conditions on the prepared carbon materials in terms of the characteristics and behavior of CO2 adsorption were investigated. Textural properties, such as specific surface area and total pore volume, linearly increased with the KOH/C ratio, attributed to the development of pores and enlargement of pores within carbon. The highest CO2 adsorption capacities of 5.70 mol kg‑1 at 0 °C and 3.48 mol kg‑1 at 25 °C were obtained for MCC activated with a KOH/C ratio of 3 (MCC-K3). In addition, CO2 adsorption uptake was significantly dependent on the volume of narrow micropores with a pore size of less than 0.8 nm rather than the volume of larger pores or surface area. MCC-K3 also exhibited excellent cyclic stability, facile regeneration, and rapid adsorption kinetics. As compared to the pseudo-first-order model, the pseudo-second-order kinetic model described the experimental adsorption data methodically.

  15. Hyper-crosslinked cyclodextrin porous polymer: An efficient CO2 capturing material with tunable porosity

    DOE PAGES

    Meng, Bo; Li, Haiyang; East China Univ. of Science and Technology, Shanghai; ...

    2016-11-11

    We designed and synthesized the cyclodextrin (CD)-based hyper-crosslinked porous polymers (HCPPs) for selective CO2 adsorption and storage. We also explored the effect of monomer size on micropore formation, and determined a feasible way to tailor the porosity of the materials during the hyper-crosslinking process.

  16. CO2 Capture in the Sustainable Wheat-Derived Activated Microporous Carbon Compartments

    PubMed Central

    Hong, Seok-Min; Jang, Eunji; Dysart, Arthur D.; Pol, Vilas G.; Lee, Ki Bong

    2016-01-01

    Microporous carbon compartments (MCCs) were developed via controlled carbonization of wheat flour producing large cavities that allow CO2 gas molecules to access micropores and adsorb effectively. KOH activation of MCCs was conducted at 700 °C with varying mass ratios of KOH/C ranging from 1 to 5, and the effects of activation conditions on the prepared carbon materials in terms of the characteristics and behavior of CO2 adsorption were investigated. Textural properties, such as specific surface area and total pore volume, linearly increased with the KOH/C ratio, attributed to the development of pores and enlargement of pores within carbon. The highest CO2 adsorption capacities of 5.70 mol kg−1 at 0 °C and 3.48 mol kg−1 at 25 °C were obtained for MCC activated with a KOH/C ratio of 3 (MCC-K3). In addition, CO2 adsorption uptake was significantly dependent on the volume of narrow micropores with a pore size of less than 0.8 nm rather than the volume of larger pores or surface area. MCC-K3 also exhibited excellent cyclic stability, facile regeneration, and rapid adsorption kinetics. As compared to the pseudo-first-order model, the pseudo-second-order kinetic model described the experimental adsorption data methodically. PMID:27698448

  17. Biogenic polyamines capture CO2 and accelerate extracellular bacterial CaCO3 formation.

    PubMed

    Yasumoto, Ko; Yasumoto-Hirose, Mina; Yasumoto, Jun; Murata, Ryo; Sato, Shun-Ichi; Baba, Megumi; Mori-Yasumoto, Kanami; Jimbo, Mitsuru; Oshima, Yasukatsu; Kusumi, Takenori; Watabe, Shugo

    2014-08-01

    Bacteria, including cyanobacteria, as well as some fungi, are known to deposit calcium carbonate (CaCO(3)) extracellularly in calcium-containing artificial medium. Despite extensive investigation, the mechanisms involved in extracellular formation of CaCO(3) by bacteria have remained unclear. The ability of synthetic amines to remove carbon dioxide (CO(2)) from natural gas led us to examine the role of biogenic polyamines in CaCO(3) deposition by bacteria. Here, we demonstrated that biogenic polyamines such as putrescine, spermidine, and spermine were able to react with atmospheric CO(2) and the resultant carbamate anion was characterized by using nuclear magnetic resonance (NMR) analysis. Biogenic polyamines accelerated the formation of CaCO(3), and we artificially synthesized the dumbbell-shaped calcites, which had the same form as observed with bacterial CaCO3 precipitates, under nonbacterial conditions by using polyamines. The reaction rate of calcification increased with temperature with an optimum of around 40 °C. Our observation suggests a novel scheme for CO(2) dissipation that could be a potential tool in reducing atmospheric CO(2) levels and, therefore, global warming.

  18. Effects of bonding types and functional groups on CO2 capture using novel multiphase systems of liquid-like nanoparticle organic hybrid materials.

    PubMed

    Lin, Kun-Yi Andrew; Park, Ah-Hyung Alissa

    2011-08-01

    Novel liquid-like nanoparticle organic hybrid materials (NOHMs) which possess unique features including negligible vapor pressure and a high degree of tunability were synthesized and their physical and chemical properties as well as CO(2) capture capacities were investigated. NOHMs can be classified based on the synthesis methods involving different bonding types, the existence of linkers, and the addition of task-specific functional groups including amines for CO(2) capture. As a canopy of polymeric chains was grafted onto the nanoparticle cores, the thermal stability of the resulting NOHMs was improved. In order to isolate the entropy effect during CO(2) capture, NOHMs were first prepared using polymers that do not contain functional groups with strong chemical affinity toward CO(2). However, it was found that even ether groups on the polymeric canopy contributed to CO(2) capture in NOHMs via Lewis acid-base interactions, although this effect was insignificant compared to the effect of task-specific functional groups such as amine. In all cases, a higher partial pressure of CO(2) was more favorable for CO(2) capture, while a higher temperature caused an adverse effect. Multicyclic CO(2) capture tests confirmed superior recyclability of NOHMs and NOHMs also showed a higher selectivity toward CO(2) over N(2)O, O(2) and N(2).

  19. Process boundaries of irreversible scCO2 -assisted phase separation in biphasic whole-cell biocatalysis.

    PubMed

    Brandenbusch, Christoph; Glonke, Sebastian; Collins, Jonathan; Hoffrogge, Raimund; Grunwald, Klaudia; Bühler, Bruno; Schmid, Andreas; Sadowski, Gabriele

    2015-11-01

    The formation of stable emulsions in biphasic biotransformations catalyzed by microbial cells turned out to be a major hurdle for industrial implementation. Recently, a cost-effective and efficient downstream processing approach, using supercritical carbon dioxide (scCO2 ) for both irreversible emulsion destabilization (enabling complete phase separation within minutes of emulsion treatment) and product purification via extraction has been proposed by Brandenbusch et al. (2010). One of the key factors for a further development and scale-up of the approach is the understanding of the mechanism underlying scCO2 -assisted phase separation. A systematic approach was applied within this work to investigate the various factors influencing phase separation during scCO2 treatment (that is pressure, exposure of the cells to CO2 , and changes of cell surface properties). It was shown that cell toxification and cell disrupture are not responsible for emulsion destabilization. Proteins from the aqueous phase partially adsorb to cells present at the aqueous-organic interface, causing hydrophobic cell surface characteristics, and thus contribute to emulsion stabilization. By investigating the change in cell-surface hydrophobicity of these cells during CO2 treatment, it was found that a combination of catastrophic phase inversion and desorption of proteins from the cell surface is responsible for irreversible scCO2 mediated phase separation. These findings are essential for the definition of process windows for scCO2 -assisted phase separation in biphasic whole-cell biocatalysis.

  20. How much CO2 does vegetation capture in tropical cities? Case study of a residential neighborhood in Singapore

    NASA Astrophysics Data System (ADS)

    Velasco, E.; Roth, M.; Tan, S.; Quak, M.; Seth, N.; Norford, L.

    2012-12-01

    Urban vegetation might have an important role in reducing the CO2 emitted by anthropogenic activities in cities, particularly in cities with extensive and/or evergreen vegetation. In a few urban sites negative daytime CO2 fluxes during the growing season have been observed. These sites correspond to suburban neighborhoods with abundant vegetation and low population density. Usually urban surfaces are net sources of CO2 modulated in some cases by vegetation during daytime. A direct and accurate estimation of carbon uptake by urban vegetation is a difficult task due to the particular characteristics of the urban ecosystem and high variability in tree distribution and species. Here, we investigate the role of urban vegetation in the CO2 flux from a residential neighborhood in Singapore using two different approaches. CO2 fluxes measured directly by eddy covariance were compared with emissions estimated by emissions factors and activity data. The latter includes contributions from vehicular traffic, household combustion, soil respiration and human breathing. The difference between estimated emissions and measured fluxes should primarily correspond to the biogenic flux. Independently, a tree survey was conducted to estimate the annual CO2 sequestration using allometric equations and an alternative model of the theory of metabolic ecology for tropical forests. This model predicts the biomass growth rate of woody trees as a function of their size. Palm trees were also included in the survey, but their annual CO2 uptake was obtained from growth curves/rates published in the literature. Both approaches suggest that vegetation captures between 5% and 8% of the CO2 emitted in this neighborhood. Annual uptakes of 510 and 324 ton km-2 were obtained from the difference between measured fluxes and estimated emissions, and the approach based on allometric equations, respectively. The difference between both approaches can be due to uncertainties in the emissions estimates and

  1. Efficiency enhancement for natural gas liquefaction with CO2 capture and sequestration through cycles innovation and process optimization

    NASA Astrophysics Data System (ADS)

    Alabdulkarem, Abdullah

    Liquefied natural gas (LNG) plants are energy intensive. As a result, the power plants operating these LNG plants emit high amounts of CO2 . To mitigate global warming that is caused by the increase in atmospheric CO2, CO2 capture and sequestration (CCS) using amine absorption is proposed. However, the major challenge of implementing this CCS system is the associated power requirement, increasing power consumption by about 15--25%. Therefore, the main scope of this work is to tackle this challenge by minimizing CCS power consumption as well as that of the entire LNG plant though system integration and rigorous optimization. The power consumption of the LNG plant was reduced through improving the process of liquefaction itself. In this work, a genetic algorithm (GA) was used to optimize a propane pre-cooled mixed-refrigerant (C3-MR) LNG plant modeled using HYSYS software. An optimization platform coupling Matlab with HYSYS was developed. New refrigerant mixtures were found, with savings in power consumption as high as 13%. LNG plants optimization with variable natural gas feed compositions was addressed and the solution was proposed through applying robust optimization techniques, resulting in a robust refrigerant which can liquefy a range of natural gas feeds. The second approach for reducing the power consumption is through process integration and waste heat utilization in the integrated CCS system. Four waste heat sources and six potential uses were uncovered and evaluated using HYSYS software. The developed models were verified against experimental data from the literature with good agreement. Net available power enhancement in one of the proposed CCS configuration is 16% more than the conventional CCS configuration. To reduce the CO2 pressurization power into a well for enhanced oil recovery (EOR) applications, five CO2 pressurization methods were explored. New CO2 liquefaction cycles were developed and modeled using HYSYS software. One of the developed

  2. Polyethyleneimine-functionalized polyamide imide (Torlon) hollow-fiber sorbents for post-combustion CO2 capture.

    PubMed

    Li, Fuyue Stephanie; Qiu, Wulin; Lively, Ryan P; Lee, Jong Suk; Rownaghi, Ali A; Koros, William J

    2013-07-01

    Carbon dioxide emitted from existing coal-fired power plants is a major environmental concern due to possible links to global climate change. In this study, we expand upon previous work focused on aminosilane-functionalized polymeric hollow-fiber sorbents by introducing a new class of polyethyleneimine (PEI)-functionalized polymeric hollow-fiber sorbents for post-combustion carbon dioxide capture. Different molecular weight PEIs (M(n) ≈600, 1800, 10,000, and 60,000) were studied as functional groups on polyamide imide (PAI, Torlon) hollow fibers. This imide ring-opening modification introduces two amide functional groups and was confirmed by FTIR attenuated total reflectance spectroscopy. The carbon dioxide equilibrium sorption capacities of PEI-functionalized Torlon materials were characterized by using both pressure decay and gravimetric sorption methods. For equivalent PEI concentrations, PAI functionalized with lower molecular weight PEI exhibited higher carbon dioxide capacities. The effect of water in the ring-opening reaction was also studied. Up to a critical value, water in the reaction mixture enhanced the degree of functionalization of PEI to Torlon and resulted in higher carbon dioxide uptake within the functionalized material. Above the critical value, roughly 15% w/w water, the fiber morphology was lost and the fiber was soluble in the solvent. PEI-functionalized (Mn ≈600) PAI under optimal reaction conditions was observed to have the highest CO2 uptake: 4.9 g CO2 per 100 g of polymer (1.1 mmol g(-1)) at 0.1 bar and 35 °C with dry 10% CO2/90% N2 feed for thermogravimetric analysis. By using water-saturated feeds (10% CO2 /90% N2 dry basis), CO2 sorption was observed to increase to 6.0 g CO2 per 100 g of sorbent (1.4 mmol g(-1)). This material also demonstrated stability in cyclic adsorption-desorption operations, even under wet conditions at which some highly effective sorbents tend to lose performance. Thus, PEI-functionalized PAI fibers can be

  3. Formulation of Aminosilica Adsorbents into 3D-Printed Monoliths and Evaluation of Their CO2 Capture Performance.

    PubMed

    Thakkar, Harshul; Eastman, Stephen; Al-Mamoori, Ahmed; Hajari, Amit; Rownaghi, Ali A; Rezaei, Fateme

    2017-03-01

    Amine-based materials have represented themselves as a promising class of CO2 adsorbents; however, their large-scale implementation requires their formulation into suitable structures. In this study, we report formulation of aminosilica adsorbents into monolithic structures through a three-dimensional (3D) printing technique. In particular, 3D-printed monoliths were fabricated using presynthesized silica-supported tetraethylenepentamine (TEPA) and poly(ethylenimine) (PEI) adsorbents using three different approaches. In addition, a 3D-printed bare silica monolith was prepared and post-functionalized with 3-aminopropyltrimethoxysilane (APS). Characterization of the obtained monoliths indicated that aminosilica materials retained their characteristics after being extruded into 3D-printed configurations. Adsorptive performance of amine-based structured adsorbents was also investigated in CO2 capture. Our results indicated that aminosilica materials retain their structural, physical, and chemical properties in the monoliths. In addition, the aminosilica monoliths exhibited adsorptive characteristics comparable to their corresponding powders. This work highlights the importance of adsorbent materials formulations into practical contactors such as monoliths, as the scalabale technology platform, that could facilitate rapid deployment of adsorption-based CO2 capture processes on commercial scales.

  4. Energy conversion performance of black liquor gasification to hydrogen production using direct causticization with CO(2) capture.

    PubMed

    Naqvi, M; Yan, J; Dahlquist, E

    2012-04-01

    This paper estimates potential hydrogen production via dry black liquor gasification system with direct causticization integrated with a reference pulp mill. The advantage of using direct causticization is elimination of energy intensive lime kiln. Pressure swing adsorption is integrated in the carbon capture process for hydrogen upgrading. The energy conversion performance of the integrated system is compared with other bio-fuel alternatives and evaluated based on system performance indicators. The results indicated a significant hydrogen production potential (about 141MW) with an energy ratio of about 0.74 from the reference black liquor capacity (about 243.5MW) and extra biomass import (about 50MW) to compensate total energy deficit. About 867,000tonnes of CO(2) abatement per year is estimated i.e. combining CO(2) capture and CO(2) offset from hydrogen replacing motor gasoline. The hydrogen production offers a substantial motor fuel replacement especially in regions with large pulp and paper industry e.g. about 63% of domestic gasoline replacement in Sweden.

  5. CO2 Fixation, Lipid Production, and Power Generation by a Novel Air-Lift-Type Microbial Carbon Capture Cell System.

    PubMed

    Hu, Xia; Liu, Baojun; Zhou, Jiti; Jin, Ruofei; Qiao, Sen; Liu, Guangfei

    2015-09-01

    An air-lift-type microbial carbon capture cell (ALMCC) was constructed for the first time by using an air-lift-type photobioreactor as the cathode chamber. The performance of ALMCC in fixing high concentration of CO2, producing energy (power and biodiesel), and removing COD together with nutrients was investigated and compared with the traditional microbial carbon capture cell (MCC) and air-lift-type photobioreactor (ALP). The ALMCC system produced a maximum power density of 972.5 mW·m(-3) and removed 86.69% of COD, 70.52% of ammonium nitrogen, and 69.24% of phosphorus, which indicate that ALMCC performed better than MCC in terms of power generation and wastewater treatment efficiency. Besides, ALMCC demonstrated 9.98- and 1.88-fold increases over ALP and MCC in the CO2 fixation rate, respectively. Similarly, the ALMCC significantly presented a higher lipid productivity compared to those control reactors. More importantly, the preliminary analysis of energy balance suggested that the net energy of the ALMCC system was significantly superior to other systems and could theoretically produce enough energy to cover its consumption. In this work, the established ALMCC system simultaneously achieved the high level of CO2 fixation, energy recycle, and municipal wastewater treatment effectively and efficiently.

  6. CO2 capture from the atmosphere and simultaneous concentration using zeolites and amine-grafted SBA-15.

    PubMed

    Stuckert, Nicholas R; Yang, Ralph T

    2011-12-01

    CO(2) capture from the atmosphere and concentration by cyclic adsorption-desorption processes are studied for the first time. New high microporosity materials, zeolite types Li-LSX and K-LSX, are compared to zeolite NaX and amine-grafted SBA-15 with low amine content. Breakthrough performance showed low silica type X (LSX) to have the most promise for application in dry conditions and capable of high space velocities of at least 63,000 h(-1), with minimal spreading of the CO(2) breakthrough curve. Amine-grafted silica was the only adsorbent able to operate in wet conditions, but at a lower space velocity of 1500 h(-1), due to slower uptake rates. The results illustrate that the uptake rate is as important as the equilibrium adsorbed amount in determining the cyclic process performance. Li-LSX was found to have double the capacity of zeolite NaX at atmospheric conditions, also higher than all other reported zeolites. It is further demonstrated that by using a combined temperature and vacuum swing cycle, the CO(2) concentration in the desorption product is >90% for all adsorbents in pellet form. This is the first report of such high CO(2) product concentrations from a single cycle, using atmospheric air.

  7. Thermal degradation of aqueous 2-aminoethylethanolamine in CO2 capture; identification of degradation products, reaction mechanisms and computational studies.

    PubMed

    Saeed, Idris Mohamed; Lee, Vannajan Sanghiran; Mazari, Shaukat Ali; Si Ali, B; Basirun, Wan Jeffrey; Asghar, Anam; Ghalib, Lubna; Jan, Badrul Mohamed

    2017-01-01

    Amine degradation is the main significant problems in amine-based post-combustion CO2 capture, causes foaming, increase in viscosity, corrosion, fouling as well as environmental issues. Therefore it is very important to develop the most efficient solvent with high thermal and chemical stability. This study investigated thermal degradation of aqueous 30% 2-aminoethylethanolamine (AEEA) using 316 stainless steel cylinders in the presence and absence of CO2 for 4 weeks. The degradation products were identified by gas chromatography mass spectrometry (GC/MS) and liquid chromatography-time-of-flight-mass spectrometry (LC-QTOF/MS). The results showed AEEA is stable in the absence of CO2, while in the presence of CO2 AEEA showed to be very unstable and numbers of degradation products were identified. 1-(2-Hydroxyethyl)-2-imidazolidinone (HEIA) was the most abundance degradation product. A possible mechanism for the thermal degradation of AEEA has been developed to explain the formation of degradation products. In addition, the reaction energy of formation of the most abundance degradation product HEIA was calculated using quantum mechanical calculation.

  8. Amine-tethered adsorbents based on three-dimensional macroporous silica for CO(2) capture from simulated flue gas and air.

    PubMed

    Liu, Fa-Qian; Wang, Lei; Huang, Zhao-Ge; Li, Chao-Qin; Li, Wei; Li, Rong-Xun; Li, Wei-Hua

    2014-03-26

    New covalently tethered CO2 adsorbents are synthesized through the in situ polymerization of N-carboxyanhydride (NCA) of l-alanine from amine-functionalized three-dimensional (3D) interconnected macroporous silica (MPS). The interconnected macropores provide low-resistant pathways for the diffusion of CO2 molecules, while the abundant mesopores ensure the high pore volume. The adsorbents exhibit high molecular weight (of up to 13058 Da), high amine loading (more than 10.98 mmol N g(-1)), fast CO2 capture kinetics (t1/2 < 1 min), high adsorption capacity (of up to 3.86 mmol CO2 g(-1) in simulated flue gas and 2.65 mmol CO2 g(-1) in simulated ambient air under 1 atm of dry CO2), as well as good stability over 120 adsorption-desorption cycles, which allows the overall CO2 capture process to be promising and sustainable.

  9. Mesoporous carbon stabilized MgO nanoparticles synthesized by pyrolysis of MgCl2 preloaded waste biomass for highly efficient CO2 capture.

    PubMed

    Liu, Wu-Jun; Jiang, Hong; Tian, Ke; Ding, Yan-Wei; Yu, Han-Qing

    2013-08-20

    Anthropogenic CO2 emission makes significant contribution to global climate change and CO2 capture and storage is a currently a preferred technology to change the trajectory toward irreversible global warming. In this work, we reported a new strategy that the inexhaustible MgCl2 in seawater and the abundantly available biomass waste can be utilized to prepare mesoporous carbon stabilized MgO nanoparticles (mPC-MgO) for CO2 capture. The mPC-MgO showed excellent performance in the CO2 capture process with the maximum capacity of 5.45 mol kg(-1), much higher than many other MgO based CO2 trappers. The CO2 capture capacity of the mPC-MgO material kept almost unchanged in 19-run cyclic reuse, and can be regenerated at low temperature. The mechanism for the CO2 capture by the mPC-MgO was investigated by FTIR and XPS, and the results indicated that the high CO2 capture capacity and the favorable selectivity of the as-prepared materials were mainly attributed to their special structure (i.e., surface area, functional groups, and the MgO NPs). This work would open up a new pathway to slow down global warming as well as resolve the pollution of waste biomass.

  10. Ultem((R))/ZIF-8 mixed matrix hollow fiber membranes for CO2/N-2 separations

    SciTech Connect

    Dai, Y; Johnson, JR; Karvan, O; Sholl, DS; Koros, WJ

    2012-05-15

    Organic-inorganic hybrid (mixed matrix) membranes can potentially extend the separation performance of traditional polymeric materials while maintaining processing convenience. Although many dense films studies have been reported, there have been few reported cases of these materials being successfully extended to asymmetric hollow fibers. In this work we report the first successful production of mixed matrix asymmetric hollow fiber membranes containing metal-organic-framework (MOF) ZIF-8 fillers. Specifically, we have incorporated ZIF-8 into a polyetherimide (Ultem((R)) 1000) matrix and produced dual-layer asymmetric hollow fiber membranes via the dry jet-wet quench method. The outer separating layer of these composite fibers contains 13 wt% (17 vol%) of ZIF-8 filler. These membranes have been tested over a range of temperatures and pressures for a variety of gas pairs. An increase in separation performance for the CO2/N-2 gas pairs was observed for both pure gas and mixed gas feeds. (C) 2012 Elsevier B.V. All rights reserved.

  11. Equimolar CO(2) capture by imidazolium-based ionic liquids and superbase systems

    SciTech Connect

    Dai, Sheng; Wang, Chongmin; Luo, Huimin; Luo, Xiaoyan; Li, Qing; Li, Haoran

    2010-01-01

    Imidazolium-based ionic liquids continue to attract interest in many areas of chemistry because of their low melting points, relatively low viscosities, ease of synthesis, and good stabilities against oxidative and reductive conditions. However, they are not totally inert under many conditions due to the intrinsic acidity of hydrogen at the C-2 position in the imidazolium cation. In this work, this intrinsic acidity was exploited in combination with an organic superbase for the capture of CO{sub 2} under atmospheric pressure. During the absorption of CO{sub 2}, the imidazolium-based ionic liquid containing an equimolar superbase reacted with CO{sub 2} to form a liquid carboxylate salt so that the equimolar capture of CO{sub 2} with respect to the base was achieved. The effects of ionic liquid structures, types of organic superbases, absorption times, and reaction temperatures on the capture of CO{sub 2} were investigated. Our results show that this integrated ionic liquid-superbase system is capable of rapid and reversible capture of about 1 mol CO{sub 2} per mole of ionic liquid. Furthermore, the captured CO{sub 2} can be readily released by either heating or bubbling N{sub 2}, and recycled with little loss of its capture capability. This efficient and reversible catch-and-release process using the weak acidity of the C-2 proton in nonvolatile imidazolium-based ionic liquids provides a good alternative to the current CO{sub 2} capture methods that use volatile alkanols, amines, or water.

  12. Ideal CO2/Light Gas Separation Performance of Poly(vinylimidazolium) Membranes and Poly(vinylimidazolium)-Ionic Liquid Composite Films

    SciTech Connect

    Carlisle, TK; Wiesenauer, EF; Nicodemus, GD; Gin, DL; Noble, RD

    2013-01-23

    Six vinyl-based, imidazolium room-temperature ionic liquid (RTIL) monomers were synthesized and photopolymerized to form dense poly(RTIL) membranes. The effect of polymer backbone (i.e., poly(ethylene), poly(styrene), and poly(acrylate)) and functional cationic substituent (e.g., alkyl, fluoroalkyl, oligo(ethylene glycol), and disiloxane) on ideal CO2/N-2 and CO2/CH4 membrane separation performance was investigated. The vinyl-based poly(RTIL)s were found to be generally less CO2-selective compared to analogous styrene- and acrylate-based poly(RTIL)s. The CO2 permeability of n-hexyl-(69 barrers) and disiloxane- (130 barrers) substituted vinyl-based poly(RTIL)s were found to be exceptionally larger than that of previously studied styrene and acrylate poly(RTIL)s. The CO2 selectivity of oligo(ethylene glycol)-functionalized vinyl poly(RTIL)s was enhanced, and the CO2 permeability was reduced when compared to the n-hexyl-substituted vinyl-based poly(RTIL). Nominal improvement in CO2/CH4 selectivity was observed upon fluorination of the n-hexyl vinyl-based poly(RTIL), with no observed change in CO2 permeability. However, rather dramatic improvements in both CO2 permeability and selectivity were observed upon blending 20 mol % RTIL (emim Tf2N) into the n-hexyl- and disiloxane-functionalized vinyl poly(RTIL)s to form solid liquid composite films.

  13. Mechanistic insight into the CO2 capture by amidophosphoranes: interplay of the ring strain and the trans influence determines the reactivity of the frustrated Lewis pairs.

    PubMed

    Zhu, Jun; An, Ke

    2013-12-01

    CO2 capture has attracted increasing attention owing to its contribution to global warming and climate change as a greenhouse gas. As an alternative strategy to transition-metal-based chemistry and catalysis, frustrated Lewis pairs have been developed to sequester CO2 efficiently under mild conditions. However, the mechanism of CO2 sequestration with amidophosphoranes remains unclear. Herein, we present a thorough density functional theory study on a series of amidophosphoranes. Our results reveal that the interplay of the ring strain and the trans influence determines the reactivities, thus opening a new avenue to the design of frustrated Lewis pairs for CO2 capture.

  14. An Integrated Hydrogen Production-CO2 Capture Process from Fossil Fuel

    SciTech Connect

    Z. Wang; K. B. Bota

    2005-03-15

    The major project objective is to determine the feasibility of using the char from coal and/or biomass pyrolysis, ammonia and CO2 emissions at smokestacks to produce clean hydrogen and a sequestered carbon fertilizer. During this work period, literature review has been completed. The project plan, design and test schedules were made on the basis of discussion with partner in experimental issues. Installation of pilot scale units was finished and major units tests were fully performed. Modification of the pyrolyzer, reformer and gas absorption tank have been done. Integration testing is performing recently. Lab scale tests are in operation phase. The experimental installations are discussed in this paper.

  15. An Intergrated Hydrogen Production-CO2 Capture Process from Fossil Fuel

    SciTech Connect

    Z. Wang; K. B. Bota

    2006-03-15

    The major project objective is to determine the feasibility of using the char from coal and/or biomass pyrolysis, ammonia and CO2 emissions at smokestacks to produce clean hydrogen and a sequestered carbon fertilizer. During this work period, the project plan, design and test schedules were made on the basis of discussion with partner in experimental issues. Installation of pilot scale units was finished and major units tests were fully performed. Modification of the pyrolyzer, reformer and gas absorption tank have been done. Integration testing is performing recently. Lab scale tests have been performed. Field tests of char/fertilizer have been conducted.

  16. Mechanisms of CO2 capture in ionic liquids: a computational perspective.

    PubMed

    Mercy, Maxime; de Leeuw, Nora H; Bell, Robert G

    2016-10-20

    We present computational studies of CO2 sorption in two different classes of ionic liquid. The addition of carbon dioxide to four superbase ionic liquids, [P3333][Benzim], [P3333][124Triz], [P3333][123Triz] and [P3333][Bentriz], was studied using the DFT approach and considering anions alone and individual ion pairs. The addition of CO2 to the anion alone clearly resulted in the formation of a covalently-bound carbamate function with the strength of binding correlated to experimental capacity. In the ion pair however the cation significantly alters the nature of the bonding such that the overall cohesive energy is reduced. Formation of a strong carbamate function occurs at the expense of weakening the interaction between anion and cation. In [N1111][l-ALA], a representative amino acid ionic liquid, evidence was found for a low-energy monomolecular mechanism for carbamate formation, explaining the 1 : 1 molar uptake ratio observed in some amino acid ionic liquids. The mechanism involves proton transfer to the carboxylate group of the aminate anion.

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

    PubMed

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

    2015-06-22

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

  18. CO2 capture performance of bi-functional activated bleaching earth modified with basic-alcoholic solution and functionalization with monoethanolamine: isotherms, kinetics and thermodynamics.

    PubMed

    Pongstabodee, Sangobtip; Pornaroontham, Phuwadej; Pintuyothin, Nuthapol; Pootrakulchote, Nuttapol; Thouchprasitchai, Nutthavich

    2016-10-01

    CO2 capture performance of bifunctional activated bleaching earth (ABE) was investigated at atmospheric pressure. The sorbents were characterized by means of X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), Caron-Hydrogen-Nitrogen analysis (CHN), Fourier transform infrared (FT-IR) and thermal gravimetric analysis (TGA). The CO2 capacity was enhanced via basic-modification and monoethanolamine (MEA) loading of the ABE sorbent to obtain a bifunctional surface property. Here, basic-modified calcined ABE with a 30wt.% MEA loading (SAB-30) showed the highest CO2 capture capacity, but this was decreased with excess MEA loading (>30wt.%). At a 10% (V/V) initial CO2 concentration feed, the maximum capacity of SAB-30 increased from 2.71mmol/g at 30°C (without adding moisture to the feed) to 3.3mmol/g at 50°C when adding 10% (V/V) moisture to the feed. Increasing the moisture concentration further reduced the maximum CO2 capacity due to the blocking effect of the excess moisture on the sorbent surface. However, SAB-30 could completely capture CO2 even in a 100% (V/V) initial CO2 concentration feed. A maximum CO2 capacity of 5.7mmol/g for SAB-30 was achieved at 30°C. Varying the ratio of sorbent weight to total flow rate of the gas stream had no discernible effect on the equilibrium CO2 capture capacity. Avrami's equation and Toth's isotherm model provided a good fitting for the data and suggested the presence of more than one reaction pathway in the CO2 capture process and the heterogeneous adsorption surface of SAB-30. Thermodynamics studies revealed that CO2 capture on the bifunctional SAB-30 is feasible, spontaneous and exothermic in nature.

  19. The system-wide economics of a carbon dioxide capture, utilization, and storage network: Texas Gulf Coast with pure CO2-EOR flood

    NASA Astrophysics Data System (ADS)

    King, Carey W.; Gülen, Gürcan; Cohen, Stuart M.; Nuñez-Lopez, Vanessa

    2013-09-01

    This letter compares several bounding cases for understanding the economic viability of capturing large quantities of anthropogenic CO2 from coal-fired power generators within the Electric Reliability Council of Texas electric grid and using it for pure CO2 enhanced oil recovery (EOR) in the onshore coastal region of Texas along the Gulf of Mexico. All captured CO2 in excess of that needed for EOR is sequestered in saline formations at the same geographic locations as the oil reservoirs but at a different depth. We analyze the extraction of oil from the same set of ten reservoirs within 20- and five-year time frames to describe how the scale of the carbon dioxide capture, utilization, and storage (CCUS) network changes to meet the rate of CO2 demand for oil recovery. Our analysis shows that there is a negative system-wide net present value (NPV) for all modeled scenarios. The system comes close to breakeven economics when capturing CO2 from three coal-fired power plants to produce oil via CO2-EOR over 20 years and assuming no CO2 emissions penalty. The NPV drops when we consider a larger network to produce oil more quickly (21 coal-fired generators with CO2 capture to produce 80% of the oil within five years). Upon applying a CO2 emissions penalty of 602009/tCO2 to fossil fuel emissions to ensure that coal-fired power plants with CO2 capture remain in baseload operation, the system economics drop significantly. We show near profitability for the cash flow of the EOR operations only; however, this situation requires relatively cheap electricity prices during operation.

  20. Separation of CO2-CH4 mixtures on defective single walled carbon nanohorns--tip does matter.

    PubMed

    Furmaniak, Sylwester; Terzyk, Artur P; Kowalczyk, Piotr; Kaneko, Katsumi; Gauden, Piotr A

    2013-10-21

    Using realistic models of single-walled carbon nanohorns and their single-walled carbon nanotube counterparts, we study the equilibrium separation of CO2-CH4 mixtures near ambient operating conditions by using molecular simulations. We show that regardless of the studied operating conditions (i.e., total CO2-CH4 mixture pressures and mole fractions of mixture components in the bulk phase), single-walled carbon nanohorns maximize the CO2-CH4 equilibrium separation factor. Optimized samples of single-walled carbon nanohorns consisting of narrow tubular parts capped with horn-shaped tips show highly selective adsorption of CO2 over the CH4 mixture component, with the CO2-CH4 equilibrium separation factor of ~8-12. A large surface-to-volume ratio (i.e., enhanced surface forces) and unique defective morphology (i.e., packing of adsorbed molecules in quasi-one/quasi-zero dimensional nanospaces) of single-walled carbon nanohorns are their key structural properties responsible for the excellent separation performance. Our theoretical simulation results are in quantitative agreement with a recent experimental/theoretical study of the CO2-CH4 adsorption and separation on oxidized single-walled carbon nanohorns [Ohba et al., Chem. Lett., 40, 2011, 1089]. Both experiment and theory showed that the CO2-CH4 equilibrium separation factor of oxidized samples of single-walled nanohorns measured near ambient operating conditions is ~2-5. This reduction in the separation efficiency as compared to optimized samples of single-walled carbon nanohorns is theoretically justified by their lower surface-to-volume ratio (i.e., larger diameters of tubular parts and horn-shaped tips).

  1. Reversible Ionic Liquids as Double-Action Solvents for Efficient CO2 Capture

    SciTech Connect

    Eckert, Charles; Liotta, Charles

    2011-09-30

    We have developed a novel class of CO{sub 2} capture solvents, Reversible Ionic Liquids (RevILs), that offer high absorption capacity through two modes of capture: chemical reaction (chemisorption) and physical solubility (physisorption). These solvents are silicon containing alkaline compounds such as silylamines that form a liquid salt (ionic liquid) upon reaction with CO{sub 2}. Subsequently, modest elevations in temperature reverse the reaction and yield pure CO{sub 2} for sequestration. By incorporating Si in the molecules we have reduced the viscosity, thereby improving the mass transfer rates of CO{sub 2} absorption/desorption and decreasing the processing costs for pumping the solvent. In this project, we have made systematic changes to the structure of these compounds to improve several physical and thermodynamic properties important for CO{sub 2} capture. Through these structure-property paradigms, we have obtained a RevIL which requires only a third of the energy required by conventional aqueous MEA process for 90% CO{sub 2} capture.

  2. Relationship between mosquito (Diptera: Culicidae) landing rates on a human subject and numbers captured using CO2-baited light traps.

    PubMed

    Barnard, D R; Knue, G J; Dickerson, C Z; Bernier, U R; Kline, D L

    2011-06-01

    Capture rates of insectary-reared female Aedes albopictus (Skuse), Anopheles quadrimaculatus Say, Culex nigripalpus Theobald, Culex quinquefasciatus Say and Aedes triseriatus (Say) in CDC-type light traps (LT) supplemented with CO2 and using the human landing (HL) collection method were observed in matched-pair experiments in outdoor screened enclosures. Mosquito responses were compared on a catch-per-unit-effort basis using regression analysis with LT and HL as the dependent and independent variables, respectively. The average number of mosquitoes captured in 1 min by LT over a 24-h period was significantly related to the average number captured in 1 min by HL only for Cx. nigripalpus and Cx. quinquefasciatus. Patterns of diel activity indicated by a comparison of the mean response to LT and HL at eight different times in a 24-h period were not superposable for any species. The capture rate efficiency of LT when compared with HL was ≤15% for all mosquitoes except Cx. quinquefasciatus (43%). Statistical models of the relationship between mosquito responses to each collection method indicate that, except for Ae. albopictus, LT and HL capture rates are significantly related only during certain times of the diel period. Estimates of mosquito activity based on observations made between sunset and sunrise were most precise in this regard for An. quadrimaculatus and Cx. nigripalpus, as were those between sunrise and sunset for Cx. quinquefasciatus and Ae. triseriatus.

  3. An Integrated Hydrogen Producton-CO2 Capture Process from Fossil Fuel

    SciTech Connect

    Z. Wang; K.B. Bota; D. Day

    2005-12-01

    The major project objective is to determine the feasibility of using the char from coal and/or biomass pyrolysis, ammonia and CO2 emissions at smokestacks to produce clean hydrogen and a sequestered carbon fertilizer. During this work period, literature review has been completed. The project plan, design and test schedules were made on the basis of discussion with partner in experimental issues. Installation of pilot scale units was finished and major units tests were fully performed. Modification of the pyrolyzer, reformer and gas absorption tank have been done. Integration testing is performing recently. Lab scale tests have been performed. Field tests of char/fertilizer have been conducted. The experimental results are discussed in this paper.

  4. A Robust Metal-Organic Framework Combining Open Metal Sites and Polar Groups for Methane Purification and CO2 /Fluorocarbon Capture.

    PubMed

    Chen, Cheng-Xia; Zheng, Shao-Ping; Wei, Zhang-Wen; Cao, Chen-Chen; Wang, Hai-Ping; Wang, Dawei; Jiang, Ji-Jun; Fenske, Dieter; Su, Cheng-Yong

    2017-02-08

    A 3D porous perchlorinated metal-organic framework (MOF), LIFM-26, featuring dual functionality, that is, functional polar groups and open metal sites, has been synthesized using perchlorinated linear dicarboxylate to link trigonal prismatic Fe3 (μ3 -O) units. LIFM-26 exhibits good thermal and chemical stability, and possesses high porosity with a BET surface area of 1513 m(2)  g(-1) , compared with isoreticular MOF-235 and Fe3 O(F4 BDC)3 (H2 O)3 (F4 BDC=2,3,5,6-tetrafluorobenzene-1,4-dicarboxylate). Most strikingly, LIFM-26 features good gas sorption/separation performance at 298 K and 1 atm with IAST selectivity values reaching up to 36, 93, 23, 11, 46, and 202 for CO2 /CH4 , CO2 /N2 , C2 H4 /CH4 , C2 H6 /CH4 , C3 H8 /CH4 , and R22/N2 (R22=CHClF2 ), respectively, showing potential for use in biogas/natural gas purification and CO2 /R22 capture.

  5. Theoretical Predictions of the thermodynamic Properties of Solid Sorbents Capture CO2 Applications

    SciTech Connect

    Duan, Yuhua; Sorescu, Dan; Luebke David; Pennline, Henry

    2012-05-02

    We are establishing a theoretical procedure to identify most potential candidates of CO{sub 2} solid sorbents from a large solid material databank to meet the DOE programmatic goal for energy conversion; and to explore the optimal working conditions for the promising CO{sub 2} solid sorbents, especially from room to warm T ranges with optimal energy usage, used for both pre- and post-combustion capture technologies.

  6. Potential influence of CO2 release from a carbon capture storage site on release of trace metals from marine sediment.

    PubMed

    Payán, M Cruz; Verbinnen, Bram; Galan, Berta; Coz, Alberto; Vandecasteele, Carlo; Viguri, Javier R

    2012-03-01

    One of the main risks of CCS (Carbon Capture and Storage) is CO(2) leakage from a storage site. The influence of CO(2) leakage on trace metals leaching from contaminated marine sediment in a potential storage area (Northern Spain) is addressed using standardized leaching tests. The influence of the pH of the leaching solution on the leachates is evaluated using deionized water, natural seawater and acidified seawater at pH = 5, 6 and 7, obtained by CO(2) bubbling. Equilibrium leaching tests (EN 12457) were performed at different liquid-solid ratios and the results of ANC/BNC leaching test (CEN/TS 15364) were modeled using Visual Minteq. Equilibrium tests gave values of the final pH for all seawater leachates between 7 and 8 due to the high acid neutralization capacity of the sediment. Combining leaching test results and geochemical modeling provided insight in the mechanisms and prediction of trace metals leaching in acidified seawater environment.

  7. Separation of carotid body chemoreceptor responses to O2 and CO2 by oligomycin and by antimycin A.

    PubMed

    Mulligan, E; Lahiri, S

    1982-03-01

    The cat carotid chemoreceptor O2 and CO2 responses can be separated by oligomycin and by antimycin A. Both of these agents greatly diminish or abolish the chemoreceptor O2 response but not the nicotine or CO2 responses. After either oligomycin or antimycin, the responses to increases and decreases in arterial CO2 partial pressure (PaCO2) consisted of increases and decreases in activity characterized respectively by exaggerated overshoots and undershoots. These were eliminated by the carbonic anhydrase inhibitor, acetazolamide, suggesting that they resulted from changes in carotid body tissue pH. The steady-state PaCO2 response remaining after oligomycin was no longer dependent on arterial O2 partial pressure (PaO2). All effects of antimycin were readily reversible in about 20 min. The separation of the responses to O2 and CO2 indicates that there may be at least partially separate pathways of chemoreception for these two stimuli. The similarity of the oligomycin and antimycin results supports the metabolic hypothesis of chemoreception.

  8. (13)C and (15)N NMR characterization of amine reactivity and solvent effects in CO2 capture.

    PubMed

    Perinu, Cristina; Arstad, Bjørnar; Bouzga, Aud M; Jens, Klaus-J

    2014-08-28

    Factors influencing the reactivity of selected amine absorbents for carbon dioxide (CO2) capture, in terms of the tendency to form amine carbamate, have been studied. Four linear primary alkanolamines at varying chain lengths (MEA, 3A1P, 4A1B , and 5A1P ), two primary amines with different substituents in the β-position to the nitrogen (1A2P and ISOB), a secondary alkanolamine (DEA), and a sterically hindered primary amine (AMP) were investigated. The relationship between the (15)N NMR data of aqueous amines and their ability to form carbamate, as determined at equilibrium by quantitative (13)C NMR experiments, was analyzed, taking into account structural-chemical properties. For all the amines, the (15)N chemical shifts fairly reflected the observed reactivity for carbamate formation. In addition to being a useful tool for the investigation of amine reactivity, (15)N NMR data clearly provided evidence of the importance of solvent effects for the understanding of chemical dynamics in CO2 capture by aqueous amine absorbents.

  9. Scheduling the blended solution as industrial CO2 absorber in separation process by back-propagation artificial neural networks.

    PubMed

    Abdollahi, Yadollah; Sairi, Nor Asrina; Said, Suhana Binti Mohd; Abouzari-lotf, Ebrahim; Zakaria, Azmi; Sabri, Mohd Faizul Bin Mohd; Islam, Aminul; Alias, Yatimah

    2015-11-05

    It is believe that 80% industrial of carbon dioxide can be controlled by separation and storage technologies which use the blended ionic liquids absorber. Among the blended absorbers, the mixture of water, N-methyldiethanolamine (MDEA) and guanidinium trifluoromethane sulfonate (gua) has presented the superior stripping qualities. However, the blended solution has illustrated high viscosity that affects the cost of separation process. In this work, the blended fabrication was scheduled with is the process arranging, controlling and optimizing. Therefore, the blend's components and operating temperature were modeled and optimized as input effective variables to minimize its viscosity as the final output by using back-propagation artificial neural network (ANN). The modeling was carried out by four mathematical algorithms with individual experimental design to obtain the optimum topology using root mean squared error (RMSE), R-squared (R(2)) and absolute average deviation (AAD). As a result, the final model (QP-4-8-1) with minimum RMSE and AAD as well as the highest R(2) was selected to navigate the fabrication of the blended solution. Therefore, the model was applied to obtain the optimum initial level of the input variables which were included temperature 303-323 K, x[gua], 0-0.033, x[MDAE], 0.3-0.4, and x[H2O], 0.7-1.0. Moreover, the model has obtained the relative importance ordered of the variables which included x[gua]>temperature>x[MDEA]>x[H2O]. Therefore, none of the variables was negligible in the fabrication. Furthermore, the model predicted the optimum points of the variables to minimize the viscosity which was validated by further experiments. The validated results confirmed the model schedulability. Accordingly, ANN succeeds to model the initial components of the blended solutions as absorber of CO2 capture in separation technologies that is able to industries scale up.

  10. AMERICAN ELECTRIC POWER'S CONESVILLE POWER PLANT UNIT NO.5 CO2 CAPTURE RETROFIT STUDY

    SciTech Connect

    Carl R. Bozzuto; Nsakala ya Nsakala; Gregory N. Liljedahl; Mark Palkes; John L. Marion

    2001-06-30

    ALSTOM Power Inc.'s Power Plant Laboratories (ALSTOM) has teamed with American Electric Power (AEP), ABB Lummus Global Inc. (ABB), the US Department of Energy National Energy Technology Laboratory (DOE NETL), and the Ohio Coal Development Office (OCDO) to conduct a comprehensive study evaluating the technical feasibility and economics of alternate CO{sub 2} capture and sequestration technologies applied to an existing US coal-fired electric generation power plant. The motivation for this study was to provide input to potential US electric utility actions concerning GHG emissions reduction. If the US decides to reduce CO{sub 2} emissions, action would need to be taken to address existing power plants. Although fuel switching from coal to natural gas may be one scenario, it will not necessarily be a sufficient measure and some form of CO{sub 2} capture for use or disposal may also be required. The output of this CO{sub 2} capture study will enhance the public's understanding of control options and influence decisions and actions by government, regulators, and power plant owners in considering the costs of reducing greenhouse gas CO{sub 2} emissions. The total work breakdown structure is encompassed within three major reports, namely: (1) Literature Survey, (2) AEP's Conesville Unit No.5 Retrofit Study, and (3) Bench-Scale Testing and CFD Evaluation. The report on the literature survey results was issued earlier by Bozzuto, et al. (2000). Reports entitled ''AEP's Conesville Unit No.5 Retrofit Study'' and ''Bench-Scale Testing and CFD Evaluation'' are provided as companion volumes, denoted Volumes I and II, respectively, of the final report. The work performed, results obtained, and conclusions and recommendations derived therefrom are summarized.

  11. Uncertainties in assessing the environmental impact of amine emissions from a CO2 capture plant

    NASA Astrophysics Data System (ADS)

    Karl, M.; Castell, N.; Simpson, D.; Solberg, S.; Starrfelt, J.; Svendby, T.; Walker, S.-E.; Wright, R. F.

    2014-08-01

    In this study, a new model framework that couples the atmospheric chemistry transport model system Weather Research and Forecasting-European Monitoring and Evaluation Programme (WRF-EMEP) and the multimedia fugacity level III model was used to assess the environmental impact of in-air amine emissions from post-combustion carbon dioxide capture. The modelling framework was applied to a typical carbon capture plant artificially placed at Mongstad, on the west coast of Norway. The study region is characterized by high precipitation amounts, relatively few sunshine hours, predominantly westerly winds from the North Atlantic and complex topography. Mongstad can be considered as moderately polluted due to refinery activities. WRF-EMEP enables a detailed treatment of amine chemistry in addition to atmospheric transport and deposition. Deposition fluxes of WRF-EMEP simulations were used as input to the fugacity model in order to derive concentrations of nitramines and nitrosamine in lake water. Predicted concentrations of nitramines and nitrosamines in ground-level air and drinking water were found to be highly sensitive to the description of amine chemistry, especially of the night-time chemistry with the nitrate (NO3) radical. Sensitivity analysis of the fugacity model indicates that catchment characteristics and chemical degradation rates in soil and water are among the important factors controlling the fate of these compounds in lake water. The study shows that realistic emission of commonly used amines result in levels of the sum of nitrosamines and nitramines in ground-level air (0.6-10 pg m-3) and drinking water (0.04-0.25 ng L-1) below the current safety guideline for human health that is enforced by the Norwegian Environment Agency. The modelling framework developed in this study can be used to evaluate possible environmental impacts of emissions of amines from post-combustion capture in other regions of the world.

  12. Uncertainties in assessing the environmental impact of amine emissions from a CO2 capture plant

    NASA Astrophysics Data System (ADS)

    Karl, M.; Castell, N.; Simpson, D.; Solberg, S.; Starrfelt, J.; Svendby, T.; Walker, S.-E.; Wright, R. F.

    2014-03-01

    In this study, a new model framework that couples the atmospheric chemistry transport model system WRF-EMEP and the multimedia fugacity level III model was used to assess the environmental impact of amine emissions to air from post-combustion carbon dioxide capture. The modelling framework was applied to a typical carbon capture plant artificially placed at Mongstad, west coast of Norway. WRF-EMEP enables a detailed treatment of amine chemistry in addition to atmospheric transport and deposition. Deposition fluxes of WRF-EMEP simulations were used as input to the fugacity model in order to derive concentrations of nitramines and nitrosamine in lake water. Predicted concentrations of nitramines and nitrosamines in ground-level air and drinking water were found to be highly sensitive to the description of amine chemistry, especially of the night time chemistry with the nitrate (NO3) radical. Sensitivity analysis of the fugacity model indicates that catchment characteristics and chemical degradation rates in soil and water are among the important factors controlling the fate of these compounds in lake water. The study shows that realistic emission of commonly used amines result in levels of the sum of nitrosamines and nitramines in ground-level air (0.6-10 pg m-3) and drinking water (0.04-0.25 ng L-1) below the current safety guideline for human health enforced by the Norwegian Environmental Directorate. The modelling framework developed in this study can be used to evaluate possible environmental impacts of emissions of amines from post-combustion capture in other regions of the world.

  13. Illinois State Geological Survey Evaluation of CO2 Capture Options from Ethanol Plants

    SciTech Connect

    Robert Finley

    2006-09-30

    The Illinois State Geological Survey and the Midwest Geological Sequestration Consortium are conducting CO{sub 2} sequestration and enhanced oil recovery testing at six different sites in the Illinois Basin. The capital and operating costs for equipment to capture and liquefy CO{sub 2} from ethanol plants in the Illinois area were evaluated so that ethanol plants could be considered as an alternate source for CO{sub 2} in the event that successful enhanced oil recovery tests create the need for additional sources of CO{sub 2} in the area. Estimated equipment and operating costs needed to capture and liquefy 68 metric tonnes/day (75 tons/day) and 272 tonnes/day (300 tons/day) of CO{sub 2} for truck delivery from an ethanol plant are provided. Estimated costs are provided for food/beverage grade CO{sub 2} and also for less purified CO{sub 2} suitable for enhanced oil recovery or sequestration. The report includes preliminary plant and equipment designs and estimates major capital and operating costs for each of the recovery options. Availability of used equipment was assessed.

  14. Advanced Oxyfuel Boilers and Process Heaters for Cost Effective CO2 Capture and Sequestration

    SciTech Connect

    Max Christie; Rick Victor; Bart van Hassel; Nagendra Nagabushana; Juan Li; Joseph Corpus; Jamie Wilson

    2007-03-31

    The purpose of the advanced boilers and process heaters program is to assess the feasibility of integrating Oxygen Transport Membranes (OTM) into combustion processes for cost effective CO{sub 2} capture and sequestration. Introducing CO{sub 2} capture into traditional combustion processes can be expensive, and the pursuit of alternative methods, like the advanced boiler/process heater system, may yield a simple and cost effective solution. In order to assess the integration of an advanced boiler/process heater process, this program addressed the following tasks: Task 1--Conceptual Design; Task 2--Laboratory Scale Evaluation; Task 3--OTM Development; Task 4--Economic Evaluation and Commercialization Planning; and Task 5--Program Management. This Final report documents and summarizes all of the work performed for the DOE award DE-FC26-01NT41147 during the period from January 2002-March 2007. This report outlines accomplishments for the following tasks: conceptual design and economic analysis, oxygen transport membrane (OTM) development, laboratory scale evaluations, and program management.

  15. Enhanced Hydrogen Production Integrated with CO2 Separation in a Single-Stage

    SciTech Connect

    Mahesh Iyer; Shwetha Ramkumar; Liang-Shih Fan

    2006-09-30

    Enhancement in the production of high purity hydrogen from fuel gas, obtained from coal gasification, is limited by thermodynamics of the Water Gas Shift Reaction. However, this constraint can be overcome by concurrent water-gas shift (WGS) and carbonation reactions to enhance H{sub 2} production by incessantly driving the equilibrium-limited WGS reaction forward and in-situ removing the CO2 product from the gas mixture. The spent sorbent is then regenerated by calcining it to produce a pure stream of CO{sub 2} and CaO which can be reused. However while performing the cyclic carbonation and calcination it was observed that the CO{sub 2} released during the in-situ calcination causes the deactivation of the iron oxide WGS catalyst. Detailed understanding of the iron oxide phase diagram helped in developing a catalyst pretreatment procedure using a H{sub 2}/H{sub 2}O system to convert the deactivated catalyst back to its active magnetite (Fe{sub 3}O{sub 4}) form. The water gas shift reaction was studied at different temperatures, different steam to carbon monoxide ratios (S/C) 3:1, 2:1, 1:1 and different total pressures ranging from 0-300 psig. The combined water gas shift and carbonation reaction was investigated at temperatures ranging from 600-700C, S/C ratio of 3:1 to 1:1 and at different pressures of 0-300 psig and the calcium looping process was found to produce high purity hydrogen with in-situ CO{sub 2} capture.

  16. Carbon dioxide capture and separation techniques for advanced power generation point sources

    SciTech Connect

    Pennline, H.W.; Luebke, D.R.; Morsi, B.I.; Heintz, Y.J.; Jones, K.L.; Ilconich, J.B.

    2006-09-01

    The capture/separation step for carbon dioxide (CO2) from large-point sources is a critical one with respect to the technical feasibility and cost of the overall carbon sequestration scenario. For large-point sources, such as those found in power generation, the carbon dioxide capture techniques being investigated by the in-house research area of the National Energy Technology Laboratory possess the potential for improved efficiency and costs as compared to more conventional technologies. The investigated techniques can have wide applications, but the research has focused on capture/separation of carbon dioxide from flue gas (postcombustion from fossil fuel-fired combustors) and from fuel gas (precombustion, such as integrated gasification combined cycle – IGCC). With respect to fuel gas applications, novel concepts are being developed in wet scrubbing with physical absorption; chemical absorption with solid sorbents; and separation by membranes. In one concept, a wet scrubbing technique is being investigated that uses a physical solvent process to remove CO2 from fuel gas of an IGCC system at elevated temperature and pressure. The need to define an ideal solvent has led to the study of the solubility and mass transfer properties of various solvents. Fabrication techniques and mechanistic studies for hybrid membranes separating CO2 from the fuel gas produced by coal gasification are also being performed. Membranes that consist of CO2-philic silanes incorporated into an alumina support or ionic liquids encapsulated into a polymeric substrate have been investigated for permeability and selectivity. An overview of two novel techniques is presented along with a research progress status of each technology.

  17. Advanced virtual energy simulation training and research: IGCC with CO2 capture power plant

    SciTech Connect

    Zitney, S.; Liese, E.; Mahapatra, P.; Bhattacharyya, D.; Provost, G.

    2011-01-01

    In this presentation, we highlight the deployment of a real-time dynamic simulator of an integrated gasification combined cycle (IGCC) power plant with CO{sub 2} capture at the Department of Energy's (DOE) National Energy Technology Laboratory's (NETL) Advanced Virtual Energy Simulation Training and Research (AVESTARTM) Center. The Center was established as part of the DOE's accelerating initiative to advance new clean coal technology for power generation. IGCC systems are an attractive technology option, generating low-cost electricity by converting coal and/or other fuels into a clean synthesis gas mixture in a process that is efficient and environmentally superior to conventional power plants. The IGCC dynamic simulator builds on, and reaches beyond, conventional power plant simulators to merge, for the first time, a 'gasification with CO{sub 2} capture' process simulator with a 'combined-cycle' power simulator. Fueled with coal, petroleum coke, and/or biomass, the gasification island of the simulated IGCC plant consists of two oxygen-blown, downward-fired, entrained-flow, slagging gasifiers with radiant syngas coolers and two-stage sour shift reactors, followed by a dual-stage acid gas removal process for CO{sub 2} capture. The combined cycle island consists of two F-class gas turbines, steam turbine, and a heat recovery steam generator with three-pressure levels. The dynamic simulator can be used for normal base-load operation, as well as plant start-up and shut down. The real-time dynamic simulator also responds satisfactorily to process disturbances, feedstock blending and switchovers, fluctuations in ambient conditions, and power demand load shedding. In addition, the full-scope simulator handles a wide range of abnormal situations, including equipment malfunctions and failures, together with changes initiated through actions from plant field operators. By providing a comprehensive IGCC operator training system, the AVESTAR Center is poised to develop a

  18. Simultaneous CO2 and SO2 capture by using ionic liquids: a theoretical approach.

    PubMed

    García, Gregorio; Atilhan, Mert; Aparicio, Santiago

    2017-02-15

    Density functional theory (DFT) methods were used to analyze the mechanism of interaction between acidic gases and ionic liquids based on the 1-ethyl-3-methylimidazolium cation coupled with five different anions. Single ion pairs and ionic clusters containing six ion pairs were used to model the interactions of the ionic liquids with acidic gas molecules. The properties of the systems were analyzed based on geometric properties, interaction energies and Bader's theory. The cluster approach gives a more accurate representation of the behavior of ions and gases in the bulk liquid phase, and despite computational challenges, the cluster approach allows us to quantify interactions beyond short range ones used in the single ion pair-acidic gas model commonly applied in the literature. The results reported herein point out efficient simultaneous capturing of both gases especially for ionic liquids containing the acetate anion.

  19. A generic analysis of energy use and solvent selection for CO2 separation from post-combustion flue gases

    USGS Publications Warehouse

    Lu, Y.; Chen, S.; Rostam-Abadi, M.

    2008-01-01

    A thermodynamic calculation was performed to determine the theoretical minimum energy used to separate CO2 from a coal combustion flue gas in a typical adsorption-desorption system. Under ideal conditions, the minimum energy required to separate CO2 from post-combustion flue gas and produce pure CO2 at 1 atmospheric pressure was only about 1183 kJ/kg CO2. This amount could double with the addition of the driving forces of mass and heat transfer and the adverse impacts of absorption heat release on adsorption capacity. Thermodynamic analyses were also performed for the aqueous amine-based absorption process. Two CO2 reaction mechanisms, the carbamate formation reaction with primary/secondary amines and the CO2 hydration reaction with tertiary amines, were included in the absorption reaction. The reaction heat, sensible heat, and stripping heat were all important to the total heat requirement. The heat use of an ideal tertiary amine amounted to 2786 kJ/kg, compared to 3211 kJ/kg for an ideal primary amine. The heat usage of an ideal amine was about 20% lower than that of commercially available amines. Optimizing the absorption process configuration could further reduce energy use. This is an abstract of a paper presented at the 2008 AIChE Spring National Meeting (New Orleans, LA 4/6-10/2008).

  20. High-Permeance Room-Temperature Ionic-Liquid-Based Membranes for CO2/N-2 Separation

    SciTech Connect

    Zhou, JS; Mok, MM; Cowan, MG; McDanel, WM; Carlisle, TK; Gin, DL; Noble, RD

    2014-12-24

    We have developed and fabricated thin-film composite (TFC) membranes with an active layer consisting of a room-temperature ionic liquid/polymerized (room-temperature ionic liquid) [i.e., (RTIL)/poly(RTIL)] composite material. The resulting membrane has a CO2 permeance of 6100 +/- 400 GPU (where 1 GPU = 10(-6) cm(3)/(cm(2) s cmHg)) and an ideal CO2/N-2 selectivity of 22 +/- 2. This represents a new membrane with state-of-the-art CO2 permeance and good CO2/N-2 selectivity. To our knowledge, this is the first example of a TFC gas separation membrane composed of an RTIL-containing active layer.

  1. Development of Fly Ash Derived Sorbents to Capture CO2 from Flue Gas of Power Plants

    SciTech Connect

    M. Mercedes Maroto-Valer; John M. Andresen; Yinzhi Zhang; Zhe Lu

    2003-12-31

    This research program focused on the development of fly ash derived sorbents to capture CO{sub 2} from power plant flue gas emissions. The fly ash derived sorbents developed represent an affordable alternative to existing methods using specialized activated carbons and molecular sieves, that tend to be very expensive and hinder the viability of the CO{sub 2} sorption process due to economic constraints. Under Task 1 'Procurement and characterization of a suite of fly ashes', 10 fly ash samples, named FAS-1 to -10, were collected from different combustors with different feedstocks, including bituminous coal, PRB coal and biomass. These samples presented a wide range of LOI value from 0.66-84.0%, and different burn-off profiles. The samples also spanned a wide range of total specific surface area and pore volume. These variations reflect the difference in the feedstock, types of combustors, collection hopper, and the beneficiation technologies the different fly ashes underwent. Under Task 2 'Preparation of fly ash derived sorbents', the fly ash samples were activated by steam. Nitrogen adsorption isotherms were used to characterize the resultant activated samples. The cost-saving one-step activation process applied was successfully used to increase the surface area and pore volume of all the fly ash samples. The activated samples present very different surface areas and pore volumes due to the range in physical and chemical properties of their precursors. Furthermore, one activated fly ash sample, FAS-4, was loaded with amine-containing chemicals (MEA, DEA, AMP, and MDEA). The impregnation significantly decreased the surface area and pore volume of the parent activated fly ash sample. Under Task 3 'Capture of CO{sub 2} by fly ash derived sorbents', sample FAS-10 and its deashed counterpart before and after impregnation of chemical PEI were used for the CO{sub 2} adsorption at different temperatures. The sample FAS-10 exhibited a CO{sub 2} adsorption capacity of 17

  2. A CO2-Free Synthetic Host-Odor Mixture That Attracts and Captures Triatomines: Effect of Emitted Odorant Ratios.

    PubMed

    Guidobaldi, F; Guerenstein, P G

    2016-07-01

    Triatomines, vectors of Chagas Disease, are hematophagous insects. Efforts have been made to develop synthetic attractants based on vertebrate odor-to lure them into traps. However, because those lures are not practical or have low capture efficiency, they are not in use in control programs. Therefore, more work is needed to reach a practical and efficient odor lure. Recently, a three-component, CO2-free, synthetic blend of vertebrate odor (consisting of ammonia, l-(+)-lactic acid, and hexanoic acid), known as Sweetscent (Biogents AG, Regensburg, Germany), was shown to attract and capture triatomines in the laboratory. In this study, using a trap olfactometer and an odor blend with constituents similar to those of Sweetscent (delivered from low-density polyethylene sachets) we found that the odorant ratios of the mixtures have a strong effect in the capture of triatomines. The blend with the most efficient combination of odorant ratios evoked ca. 81% capture in two relevant triatomine species. In the case of the most effective odor mixtures, we measured the odor mass emission for the three components of the mixture and therefore were able to estimate the odorant ratios emitted that were responsible for such a high capture performance. Thus, in those mixtures, pentanoic acid was the main component (ca. 65 %) followed by ammonia (ca. 28%) and, l(+)-lactic acid (ca. 7 %). Our results are encouraging as efficient, practical, and cheap odor baits to trap triatomines in the field would be within reach. The odor-delivery system used should be improved to increase stability of odor emission.

  3. Radiative nucleon capture with quasi-separable potentials

    NASA Astrophysics Data System (ADS)

    Shubhchintak; Bertulani, C. A.; Mukhamedzhanov, A. M.; Kruppa, A. T.

    2016-12-01

    We study radiative capture reactions using quasi-separable potentials. This procedure allows an easier treatment of non-local effects that can be extended to three-body problems. Using this technique, we calculate the neutron and proton radiative capture cross sections on 12C. The results obtained are shown to be in good agreement with the available experimental data.

  4. JV Task 106 - Feasibility of CO2 Capture Technologies for Existing North Dakota Lignite-Fired Pulverized Coal Boilers

    SciTech Connect

    Michael L. Jones; Brandon M. Pavlish; Melanie D. Jensen

    2007-05-01

    The goal of this project is to provide a technical review and evaluation of various carbon dioxide (CO{sub 2}) capture technologies, with a focus on the applicability to lignite-fired facilities within North Dakota. The motivation for the project came from the Lignite Energy Council's (LEC's) need to identify the feasibility of CO{sub 2} capture technologies for existing North Dakota lignite-fired, pulverized coal (pc) power plants. A literature review was completed to determine the commercially available technologies as well as to identify emerging CO{sub 2} capture technologies that are currently in the research or demonstration phase. The literature review revealed few commercially available technologies for a coal-fired power plant. CO{sub 2} separation and capture using amine scrubbing have been performed for several years in industry and could be applied to an existing pc-fired power plant. Other promising technologies do exist, but many are still in the research and demonstration phases. Oxyfuel combustion, a technology that has been used in industry for several years to increase boiler efficiency, is in the process of being tailored for CO{sub 2} separation and capture. These two technologies were chosen for evaluation for CO{sub 2} separation and capture from coal-fired power plants. Although oxyfuel combustion is still in the pilot-scale demonstration phase, it was chosen to be evaluated at LEC's request because it is one of the most promising emerging technologies. As part of the evaluation of the two chosen technologies, a conceptual design, a mass and energy balance, and an economic evaluation were completed.

  5. Using one waste to tackle another: preparation of a CO2 capture material zeolite X from laterite residue and bauxite.

    PubMed

    Liu, Liying; Du, Tao; Li, Gang; Yang, Fan; Che, Shuai

    2014-08-15

    In this work, zeolite X, a benchmark adsorbent for carbon capture, has been successfully prepared from low cost waste minerals namely laterite residue and bauxite using alkali fusion process followed by hydrothermal treatment. The structure and morphology of the as-synthesized zeolite X were verified and characterized with a range of experimental techniques such as X-ray diffraction, scanning electronic microscopy and infrared spectroscopy. The surface area and (N2 and CO2) gas adsorption isotherms of this product were found comparable to that of commercial ones, demonstrating the effectiveness of synthesizing zeolite X from laterite and bauxite. Further improvement of the product purity was also accomplished by optimizing the process conditions.

  6. Towards commercial scale postcombustion capture of CO2 with monoethanolamine solvent: key considerations for solvent management and environmental impacts.

    PubMed

    Reynolds, Alicia J; Verheyen, T Vincent; Adeloju, Samuel B; Meuleman, Erik; Feron, Paul

    2012-04-03

    Chemical absorption with aqueous amine solvents is the most advanced technology for postcombustion capture (PCC) of CO(2) from coal-fired power stations and a number of pilot scale programs are evaluating novel solvents, optimizing energy efficiency, and validating engineering models. This review demonstrates that the development of commercial scale PCC also requires effective solvent management guidelines to ensure minimization of potential technical and environmental risks. Furthermore, the review reveals that while solvent degradation has been identified as a key source of solvent consumption in laboratory scale studies, it has not been validated at pilot scale. Yet this is crucial as solvent degradation products, such as organic acids, can increase corrosivity and reduce the CO(2) absorption capacity of the solvent. It also highlights the need for the development of corrosion and solvent reclamation technologies, as well as strategies to minimize emissions of solvent and degradation products, such as ammonia, aldehydes, nitrosamines and nitramines, to the atmosphere from commercial scale PCC. Inevitably, responsible management of aqueous and solid waste will require more serious consideration. This will ultimately require effective waste management practices validated at pilot scale to minimize the likelihood of adverse human and environmental impacts from commercial scale PCC.

  7. CO2 capture using limestone for cultivation of the freshwater microalga Chlorella sorokiniana PAZ and the cyanobacterium Arthrospira sp. VSJ.

    PubMed

    Zawar, Prachi; Javalkote, Vivek; Burnap, Robert; Mahulikar, Pramod; Puranik, Pravin

    2016-12-01

    The present study reports a process wherein CO2 is captured in the form of bicarbonates using calcium oxide and photosynthetically fixed into biomass. Microalgal cultures viz. Chlorella sorokiniana PAZ and Arthrospira sp. VSJ were grown in the medium containing bicarbonates. The rate of bicarbonate utilization by C. sorokiniana PAZ was higher when CO2 trapped in the presence of 2.67mM calcium oxide than in the presence of 10mM sodium hydroxide and with direct addition of 10mM sodium bicarbonate. For Arthrospira sp. VSJ the bicarbonate utilization was 92.37%, 88.34% and 59.23% for the medium containing CaO, NaOH and NaHCO3, respectively. Illumination of photosynthetically active radiation (PAR)+ultraviolet A radiation (UVA) enhanced the yield of C. sorokiniana PAZ and Arthrospira sp. VSJ by 1.3 and 1.8 folds, respectively. FTIR analysis revealed elevation in the biosynthesis of specific metabolites in response to the UVA exposure.

  8. Contactor Energy Requirements for Capturing CO2 From ambient air using NaOH determined in a pilot-scale prototype system

    NASA Astrophysics Data System (ADS)

    Stolaroff, J. K.; Keith, D.; Lowry, G.

    2005-12-01

    Systems for capturing CO2 from ambient air for sequestration have recently been proposed (e.g. Dubey et al., 2002; Zeman and Lackner, 2004; Keith et al., 2004). Capture from ambient air has a number of structural advantages over capture from point sources; in particular it makes possible future emissions scenarios with negative net CO2 emissions. The systems suggested use either a Ca(OH)2 or NaOH solution to capture CO2 and then regenerate the solution in a chemical loop. The energy requirements of such a system, however, have been hotly disputed (Herzog, 2003). The energy requirements and effectiveness of the chemical regeneration are well established as they are practiced on a large scale in the industrial kraft process used in pulp and paper production, but the energy and land use requirements of a contactor for this system are uncertain as this component of the system is not implemented industrially. In this research, we address the most controversial component of the system, the contactor, which extracts CO2 from air into solution. A prototype contactor with a spray tower design is constructed (1m by 6m), and CO2 absorption by a NaOH solution spray (5 l/min) is measured. The CO2 absorption efficiency and energy requirements per unit CO2 absorbed are calculated. The energy requirements of the contactor are found to be on the order of 10-40 kJ/mol-CO2, which is small compared to the energy of combustion of fossil fuels, and compared with the energy required for the regeneration steps. Thus, a NaOH-based spray tower design can serve as an energy-efficient contactor for capturing CO2 from ambient air. Dubey, M. K., Ziock, H., Rueff, G., Elliott, S., and Smith, W. S. (2002). ``Extraction of carbon dioxide from the atmosphere through engineered chemical sinkage''. ACS -- Division of Fuel Chemistry Reprints, 47(1):81--84. Herzog, H. (2003). Assessing the feasibility of capturing co2 from the air. Technical report, MIT Laboratory for Energy and the Environment. Keith

  9. Influence of Dissolved Metals on N-Nitrosamine Formation under Amine-based CO2 Capture Conditions.

    PubMed

    Wang, Zimeng; Mitch, William A

    2015-10-06

    As the prime contender for postcombustion CO2 capture technology, amine-based scrubbing has to address the concerns over the formation of potentially carcinogenic N-nitrosamine byproducts from reactions between flue gas NOx and amine solvents. This bench-scale study evaluated the influence of dissolved metals on the potential to form total N-nitrosamines in the solvent within the absorber unit and upon a pressure-cooker treatment that mimics desorber conditions. Among six transition metals tested for the benchmark solvent monoethanolamine (MEA), dissolved Cu promoted total N-nitrosamine formation in the absorber unit at concentrations permitted in drinking water, but not the desorber unit. The Cu effect increased with oxygen concentration. Variation of the amine structural characteristics (amine order, steric hindrance, -OH group substitution and alkyl chain length) indicated that Cu promotes N-nitrosamine formation from primary amines with hydroxyl or carboxyl groups (amino acids), but not from secondary amines, tertiary amines, sterically hindered primary amines, or amines without oxygenated groups. Ethylenediaminetetraacetate (EDTA) suppressed the Cu effect. The results suggested that the catalytic effect of Cu may be associated with the oxidative degradation of primary amines in the absorber unit, a process known to produce a wide spectrum of secondary amine products that are more readily nitrosatable than the pristine primary amines, and that can form stable N-nitrosamines. This study highlighted an intriguing linkage between amine degradation (operational cost) and N-nitrosamine formation (health hazards), all of which are challenges for commercial-scale CO2 capture technology.

  10. Influence of amine structural characteristics on N-nitrosamine formation potential relevant to postcombustion CO2 capture systems.

    PubMed

    Dai, Ning; Mitch, William A

    2013-11-19

    Concerns have arisen for the possible contamination of air or drinking water supplies downwind of amine-based CO2 capture facilities by potentially carcinogenic N-nitrosamines formed from reactions between flue gas NOx and amine solvents. This study evaluated the influence of amine structure on the potential to form total N-nitrosamines within the absorber and washwater units of a laboratory-scale CO2 capture reactor, and in the solvent after a pressure-cooker treatment as a mimic of desorber conditions. Among 16 amines representing 3 amine classes (alkanolamines, straight-chain and cyclic diamines, and amino acids), the order of the amine was the primary determinant of total N-nitrosamine formation in the absorber unit, with total N-nitrosamine formation in the order: secondary amines ≈ tertiary amines ≫ primary amines. Similar results were observed upon pressure-cooker treatment, due to reactions between nitrite and amines at high temperature. For secondary and tertiary amines, total N-nitrosamine formation under these desorber-like conditions appeared to be more important than in the absorber, but for primary amines, significant formation of total N-nitrosamines was only observed in the absorber. For diamines and amino acids, total N-nitrosamine accumulation rates in washwaters were lowest for primary amines. For alkanolamines, however, total N-nitrosamine accumulation in the washwater was similar regardless of alkanolamine order, due to the combined effects of amine reactivity toward nitrosation and amine volatility. While total N-nitrosamine accumulation rates in washwaters were generally 1-2 orders of magnitude lower than in the absorber, they were comparable to absorber rates for several primary amines. Decarboxylation of the amino acid sarcosine resulted in the accumulation of significant concentrations of N-nitrosodimethylamine and N-nitrodimethylamine in the washwater.

  11. Characterization of the Axial Jet Separator with a CO2/Helium Mixture: Toward GC-AMS Hyphenation.

    PubMed

    Salazar, G; Agrios, K; Eichler, R; Szidat, S

    2016-02-02

    Development of interfaces for sample introduction from high pressures is important for real-time online hyphenation of chromatographic and other separation devices with mass spectrometry (MS) or accelerator mass spectrometry (AMS). Momentum separators can reduce unwanted low-density gases and introduce the analyte into the vacuum. In this work, the axial jet separator, a new momentum interface, is characterized by theory and empirical optimization. The mathematical model describes the different axial penetration of the components of a jet-gas mixture and explains the empirical results for injections of CO2 in helium into MS and AMS instruments. We show that the performance of the new interface is sensitive to the nozzle size, showing good qualitative agreement with the mathematical model. Smaller nozzle sizes are more preferable due to their higher inflow capacity. The CO2 transmission efficiency of the interface into a MS instrument is ∼ 14% (CO2/helium separation factor of 2.7). The interface receives and delivers flows of ∼ 17.5 mL/min and ∼ 0.9 mL/min, respectively. For the interfaced AMS instrument, the ionization and overall efficiencies are 0.7-3% and 0.1-0.4%, respectively, for CO2 amounts of 4-0.6 μg C, which is only slightly lower compared to conventional systems using intermediate trapping. The ionization efficiency depends on to the carbon mass flow in the injected pulse and is suppressed at high CO2 flows. Relative to a conventional jet separator, the transmission efficiency of the axial jet separator is lower, but its performance is less sensitive to misalignments.

  12. Fabrication of COF-MOF Composite Membranes and Their Highly Selective Separation of H2/CO2.

    PubMed

    Fu, Jingru; Das, Saikat; Xing, Guolong; Ben, Teng; Valtchev, Valentin; Qiu, Shilun

    2016-06-22

    The search for new types of membrane materials has been of continuous interest in both academia and industry, given their importance in a plethora of applications, particularly for energy-efficient separation technology. In this contribution, we demonstrate for the first time that a metal-organic framework (MOF) can be grown on the covalent-organic framework (COF) membrane to fabricate COF-MOF composite membranes. The resultant COF-MOF composite membranes demonstrate higher separation selectivity of H2/CO2 gas mixtures than the individual COF and MOF membranes. A sound proof for the synergy between two porous materials is the fact that the COF-MOF composite membranes surpass the Robeson upper bound of polymer membranes for mixture separation of a H2/CO2 gas pair and are among the best gas separation MOF membranes reported thus far.

  13. Enhanced CO2 Resistance for Robust Oxygen Separation Through Tantalum-doped Perovskite Membranes.

    PubMed

    Zhang, Chi; Tian, Hao; Yang, Dong; Sunarso, Jaka; Liu, Jian; Liu, Shaomin

    2016-03-08

    Oxygen selective membranes with enhanced oxygen permeability and CO2 resistance are highly required in sustainable clean energy generation technologies. Here, we present novel, cobalt-free, SrFe1-x Tax O3-δ (x=0, 0.025, 0.05, 0.1, 0.2) perovskite membranes. Ta-doping induced lattice structure progression from orthorhombic (x=0) to cubic (x=0.05). SrFe0.95 Ta0.05 O3-δ (SFT0.05) showed the highest oxygen flux rates reaching 0.85 mL min(-1) cm(-2) at 950 °C on a 1.0 mm-thick membrane. Surface decoration can increase the permeation rate further. Ta inclusion within the perovskite lattice of SrFeO3-δ (SF) enhanced the CO2 resistance of the membranes significantly as evidenced by the absence of the carbonate functional groups on the FTIR spectrum when exposed to CO2 atmosphere at 850 °C. The CO2 resistance of Ta-doped SF compounds correlates with the lower basicity and the higher binding energy for the lattice oxygen. SFT0.05 demonstrated high stability during long-term permeation tests under 10% CO2 atmosphere.

  14. Temperature-/pressure-dependent selective separation of CO(2) or benzene in a chiral metal-organic framework material.

    PubMed

    Tan, Yan-Xi; He, Yan-Ping; Zhang, Jian

    2012-08-01

    Presented here is a chiral microporous metal-organic framework material with a three-fold interpenetrating diamond-type structural topology and interesting properties for selective separation. The material has a high storage capacity for CO(2) gas (4.23 mmol g(-1) at 273 K and 1 bar) and shows fantastic temperature-dependent selectivity for CO(2) over N(2). Moreover, this multifunctional material, which has a rich π system, can selectively adsorb benzene over cyclohexane at low pressure (0.05 bar) at 298 K.

  15. Hexagonal boron nitride and graphene in-plane heterostructures: An experimentally feasible approach to charge-induced switchable CO2 capture

    NASA Astrophysics Data System (ADS)

    Tan, Xin; Tahini, Hassan A.; Smith, Sean C.

    2016-10-01

    Hexagonal boron nitride (h-BN) has been proposed as a sorbent material for charge-induced switchable CO2 capture. However, h-BN is a wide-gap semiconductor, hindering injection of the requisite charge. Here, we employ first-principle calculations to support the proposal that in-plane h-BN/graphene (P-BN/G) heterostructures, consisting of alternating strips of h-BN and graphene, may provide an experimentally feasible material platform for voltage-induced charging of h-BN strips to realize switchable CO2 capture. Our results show that a significant amount of injected negative charges are distributed onto h-BN strips of P-BN/G, such that CO2 capture/release can be simply controlled by switching on/off the charge states of P-BN/G system. At saturation CO2 capture coverage, the negatively charged P-BN/G heterostructures achieve CO2 capture capacities up to 2.27 × 1014 cm-2, which is twice that which can be achieved on stacked h-BN/graphene (S-BN/G) nanosheets.

  16. Effect of Cross-Linking on the Mechanical and Thermal Properties of Poly(amidoamine) Dendrimer/Poly(vinyl alcohol) Hybrid Membranes for CO2 Separation

    PubMed Central

    Duan, Shuhong; Kai, Teruhiko; Saito, Takashi; Yamazaki, Kota; Ikeda, Kenichi

    2014-01-01

    Poly(amidoamine) (PAMAM) dendrimers were incorporated into cross-linked poly(vinyl alcohol) (PVA) matrix to improve carbon dioxide (CO2) separation performance at elevated pressures. In our previous studies, PAMAM/PVA hybrid membranes showed high CO2 separation properties from CO2/H2 mixed gases. In this study, three types of organic Ti metal compounds were selected as PVA cross-linkers that were used to prepare PAMAM/cross-linked PVA hybrid membranes. Characterization of the PAMAM/cross-linked PVA hybrid membranes was conducted using nanoindentation and thermogravimetric analyses. The effects of the cross-linker and CO2 partial pressure in the feed gas on CO2 separation performance were discussed. H2O and CO2 sorption of the PAMAM/PVA hybrid membranes were investigated to explain the obtained CO2 separation efficiencies. PMID:24957172

  17. Toward understanding amines and their degradation products from postcombustion CO2 capture processes with aerosol mass spectrometry.

    PubMed

    Ge, Xinlei; Shaw, Stephanie L; Zhang, Qi

    2014-05-06

    Amine-based postcombustion CO2 capture (PCCC) is a promising technique for reducing CO2 emissions from fossil fuel burning plants. A concern of the technique, however, is the emission of amines and their degradation byproducts. To assess the environmental risk of this technique, standardized stack sampling and analytical methods are needed. Here we report on the development of an integrated approach that centers on the application of a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) for characterizing amines and PCCC-relevant species. Molecular characterization is achieved via ion chromatography (IC) and electrospray ionization high-resolution mass spectrometry (ESI-MS). The method has been optimized, particularly, by decreasing the AMS vaporizer temperature, to gain quantitative information on the elemental composition and major nitrogen-containing species in laboratory-degraded amine solvents commonly tested for PCCC applications, including ethanolamine (MEA), methyldiethanolamine (MDEA), and piperazine (PIP). The AMS-derived nitrogen-to-carbon (N/C) ratios for the degraded solvent and product mixtures agree well with the results from a total organic carbon and total nitrogen (TOC/TN) analyzer. In addition, marker ions identified in the AMS spectra are used to estimate the mass contributions of individual species. Overall, our results indicate that this new approach is suitable for characterizing PCCC-related mixtures as well as organic nitrogen species in other sample types. As an online instrument, AMS can be used for both real-time characterization of emissions from operating PCCC plants and ambient particles in the vicinity of the facilities.

  18. Toward Understanding Amines and Their Degradation Products from Postcombustion CO2 Capture Processes with Aerosol Mass Spectrometry

    PubMed Central

    2015-01-01

    Amine-based postcombustion CO2 capture (PCCC) is a promising technique for reducing CO2 emissions from fossil fuel burning plants. A concern of the technique, however, is the emission of amines and their degradation byproducts. To assess the environmental risk of this technique, standardized stack sampling and analytical methods are needed. Here we report on the development of an integrated approach that centers on the application of a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) for characterizing amines and PCCC-relevant species. Molecular characterization is achieved via ion chromatography (IC) and electrospray ionization high-resolution mass spectrometry (ESI-MS). The method has been optimized, particularly, by decreasing the AMS vaporizer temperature, to gain quantitative information on the elemental composition and major nitrogen-containing species in laboratory-degraded amine solvents commonly tested for PCCC applications, including ethanolamine (MEA), methyldiethanolamine (MDEA), and piperazine (PIP). The AMS-derived nitrogen-to-carbon (N/C) ratios for the degraded solvent and product mixtures agree well with the results from a total organic carbon and total nitrogen (TOC/TN) analyzer. In addition, marker ions identified in the AMS spectra are used to estimate the mass contributions of individual species. Overall, our results indicate that this new approach is suitable for characterizing PCCC-related mixtures as well as organic nitrogen species in other sample types. As an online instrument, AMS can be used for both real-time characterization of emissions from operating PCCC plants and ambient particles in the vicinity of the facilities. PMID:24617831

  19. Nanometric thin film membranes manufactured on square meter scale: ultra-thin films for CO2 capture.

    PubMed

    Yave, Wilfredo; Car, Anja; Wind, Jan; Peinemann, Klaus-Viktor

    2010-10-01

    Miniaturization and manipulation of materials at nanometer scale are key challenges in nanoscience and nanotechnology. In membrane science and technology, the fabrication of ultra-thin polymer films (defect-free) on square meter scale with uniform thickness (<100 nm) is crucial. By using a tailor-made polymer and by controlling the nanofabrication conditions, we developed and manufactured defect-free ultra-thin film membranes with unmatched carbon dioxide permeances, i.e. > 5 m(3) (STP) m(-2) h(-1) bar(-1). The permeances are extremely high, because the membranes are made from a CO(2) philic polymer material and they are only a few tens of nanometers thin. Thus, these thin film membranes have potential application in the treatment of large gas streams under low pressure like, e.g., carbon dioxide separation from flue gas.

  20. Extraction of Mg(OH)2 from Mg silicate minerals with NaOH assisted with H2O: implications for CO2 capture from exhaust flue gas.