Science.gov

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. 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.

  3. 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.

  4. 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

  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. PMID:26973086

  6. 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.

  7. 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

  8. 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.

  9. 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

  10. 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

  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. 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 member's 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.

  13. 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

  14. Covalent Organic Frameworks for CO2 Capture.

    PubMed

    Zeng, Yongfei; Zou, Ruqiang; Zhao, Yanli

    2016-04-01

    As an emerging class of porous crystalline materials, covalent organic frameworks (COFs) are excellent candidates for various applications. In particular, they can serve as ideal platforms for capturing CO2 to mitigate the dilemma caused by the greenhouse effect. Recent research achievements using COFs for CO2 capture are highlighted. A background overview is provided, consisting of a brief statement on the current CO2 issue, a summary of representative materials utilized for CO2 capture, and an introduction to COFs. Research progresses on: i) experimental CO2 capture using different COFs synthesized based on different covalent bond formations, and ii) computational simulation results of such porous materials on CO2 capture are summarized. Based on these experimental and theoretical studies, careful analyses and discussions in terms of the COF stability, low- and high-pressure CO2 uptake, CO2 selectivity, breakthrough performance, and CO2 capture conditions are provided. Finally, a perspective and conclusion section of COFs for CO2 capture is presented. Recent advancements in the field are highlighted and the strategies and principals involved are discussed. PMID:26924720

  15. CAPTURING CO2 WITH MGO AEROGELS

    EPA Science Inventory

    CO2 capture from flue gas requires that the adsorbent be active at relatively low CO2 concentrations (3 – 13 vol%), high temperatures (~ 250ºC), and in the presence of many other gas species. These conditions will be simulated in the student designed reactor. The...

  16. 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.

  17. Aqueous ethylenediamine for CO(2) capture.

    PubMed

    Zhou, Shan; Chen, Xi; Nguyen, Thu; Voice, Alexander K; Rochelle, Gary T

    2010-08-23

    Aqueous ethylenediamine (EDA) has been investigated as a solvent for CO(2) capture from flue gas. EDA can be used at 12 M (mol kg(-1) H(2)O) with an acceptable viscosity of 16 cP (1 cP=10(-3) Pa s) with 0.48 mol CO(2) per equivalent of EDA. Similar to monoethanolamine (MEA), EDA can be used up to 120 degrees C in a stripper without significant thermal degradation. Inhibitor A will effectively eliminate oxidative degradation. Above 120 degrees C, loaded EDA degrades with the production of its cyclic urea and other related compounds. Unlike piperazine, when exposed to oxidative degradation, EDA does not result in excessive foaming. Over much of the loading range, the CO(2) absorption rate with 12 M EDA is comparable to 7 M MEA. However, at typical rich loading, 12 M EDA absorbs CO(2) 2 times slower than 7 M MEA. The capacity of 12 M EDA is 0.72 mol CO(2)/(kg H(2)O+EDA) (for P(CO(2) )=0.5 to 5 kPa at 40 degrees C), which is about double that of MEA. The apparent heat of CO(2) desorption in EDA solution is 84 kJ mol(-1) CO(2); greater than most other amine systems. PMID:20677204

  18. 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.

  19. 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.

  20. Combustion-Assisted CO2 Capture Using MECC Membranes

    SciTech Connect

    Sherman, Steven R; Gray, Dr. Joshua R.; Brinkman, Dr. Kyle S.; Huang, Dr. Kevin

    2012-01-01

    Mixed Electron and Carbonate ion Conductor (MECC) membranes have been proposed as a means to separate CO2 from power plant flue gas. Here a modified MECC CO2 capture process is analyzed that supplements retentate pressurization and permeate evacuation as a means to create a CO2 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 CO2 in the flue gas may be captured, and a compressed CO2 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 CO2 capture system, and has the potential to meet U.S. DOE s goal that deployment of a CO2 capture system at a fossil-fueled power plant should not increase the cost of electricity from the combined facility by more than 30%.

  1. Carbon Dioxide Capture: Covalent Organic Frameworks for CO2 Capture (Adv. Mater. 15/2016).

    PubMed

    Zeng, Yongfei; Zou, Ruqiang; Zhao, Yanli

    2016-04-01

    Covalent organic frameworks (COFs) serve as ideal platforms that can selectively adsorb and separate CO2 from gas mixtures. On page 2855, R. Zou, Y. Zhao, and Y. Zeng highlight research progress in this area, compare recent achievements, and present fundamental principles. Different strategies to improve the CO2 capture capability of COFs are elaborated and the capture performance of representative COFs is analyzed. PMID:27075837

  2. 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. PMID:25594368

  3. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

  5. 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.

  6. 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.

  7. 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. PMID:22143760

  8. Porous Hexacyanometalates for CO2 capture applications

    SciTech Connect

    Motkuri, Radha K.; Thallapally, Praveen K.; McGrail, B. Peter

    2013-07-30

    Prussian blue analogues of M3[Fe(CN)6]2 x H2O (where M=Fe, Mn and Ni) were synthesized, characterized and tested for their gas sorption capabilities. The sorption studies reveal that, these Prussian blue materials preferentially sorb CO2 over N2 and CH4 at low pressure (1bar).

  9. 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

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

    PubMed

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

    2015-02-01

    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. PMID:25607244

  11. 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

  12. 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.

  13. 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

  14. 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.

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

    PubMed

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

    2016-07-27

    A series of sustainable porous carbon materials were prepared from waste polyurethane foam and investigated for capture of CO2. The effects of preparation conditions, such as precarbonization, KOH to carbon precursor weight ratio, and activation temperature, on the porous structure and CO2 adsorption properties were studied for the purpose of controlling pore sizes and nitrogen content and developing high-performance materials for capture of CO2. The sample prepared at optimum conditions shows CO2 adsorption capacities of 6.67 and 4.33 mmol·g(-1) at 0 and 25 °C under 1 bar, respectively, which are comparable to those of the best reported porous carbons prepared from waste materials. The HCl treatment experiment reveals that about 80% of CO2 adsorption capacity arises from physical adsorption, while the other 20% is due to the chemical adsorption originated from the interaction of basic N groups and CO2 molecules. The relationship between CO2 uptake and pore size at different temperatures indicates that the micropores with pore size smaller than 0.86 and 0.70 nm play a dominant role in the CO2 adsorption at 0 and 25 °C, respectively. It was found that the obtained carbon materials exhibited high recyclability and high selectivity to adsorption of CO2 from the CO2 and N2 mixture. PMID:27376177

  16. 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

  17. 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. PMID:22432609

  18. 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

  19. 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.

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

    PubMed

    Rau, Greg H

    2011-02-01

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

  1. 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.

  2. Direct Air Capture of CO2 by Physisorbent Materials.

    PubMed

    Kumar, Amrit; Madden, David G; Lusi, Matteo; Chen, Kai-Jie; Daniels, Emma A; Curtin, Teresa; Perry, John J; Zaworotko, Michael J

    2015-11-23

    Sequestration of CO2, either from gas mixtures or directly from air (direct air capture, DAC), could mitigate carbon emissions. Here five materials are investigated for their ability to adsorb CO2 directly from air and other gas mixtures. The sorbents studied are benchmark materials that encompass four types of porous material, one chemisorbent, TEPA-SBA-15 (amine-modified mesoporous silica) and four physisorbents: Zeolite 13X (inorganic); HKUST-1 and Mg-MOF-74/Mg-dobdc (metal-organic frameworks, MOFs); SIFSIX-3-Ni, (hybrid ultramicroporous material). Temperature-programmed desorption (TPD) experiments afforded information about the contents of each sorbent under equilibrium conditions and their ease of recycling. Accelerated stability tests addressed projected shelf-life of the five sorbents. The four physisorbents were found to be capable of carbon capture from CO2-rich gas mixtures, but competition and reaction with atmospheric moisture significantly reduced their DAC performance. PMID:26440308

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

    PubMed

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

    2013-06-01

    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. PMID:23678978

  4. Separation of CO2 from flue gas using electrochemical cells

    SciTech Connect

    Pennline HW, Granite EJ, Luebke DR,

    2010-06-01

    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 CO2 and O2 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 effluent 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

  5. 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.

  6. 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. PMID:25409579

  7. 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.

  8. Amine-pillared Nanosheet Adsorbents for CO2 Capture Applications

    NASA Astrophysics Data System (ADS)

    Jiang, Hui

    Amine-functionalized solid adsorbents have gained attention within the last decade for their application in carbon dioxide capture, due to their many advantages such as low energy cost for regeneration, tunable structure, elimination of corrosion problems, and additional advantages. However, one of the challenges facing this technology is to accomplish both high CO 2 capture capacity along with high CO2 diffusion rates concurrently. Current amine-based solid sorbents such as porous materials similar to SBA-15 have large pores diffusion entering molecules; however, the pores become clogged upon amine inclusion. To meet this challenge, our group's solution involves the creation of a new type of material which we are calling-amino-pillared nanosheet (APN) adsorbents which are generated from layered nanosheet precursors. These materials are being proposed because of their unique lamellar structure which exhibits ability to be modified by organic or inorganic pillars through consecutive swelling and pillaring steps to form large mesoporous interlayer spaces. After the expansion of the layer space through swelling and pillaring, the large pore space can be functionalized with amine groups. This selective functionalization is possible by the choice of amine group introduced. Our choice, large amine molecules, do not access the micropore within each layer; however, either physically or chemically immobilized onto the surface of the mesoporous interlayer space between each layer. The final goal of the research is to investigate the ability to prepare APN adsorbents from a model nanoporous layered materials including nanosheets precursor material MCM-22(P) and nanoporous layered silicate material AMH-3. MCM-22(P) contains 2-dimensional porous channels, 6 membered rings (MB) openings perpendicular to the layers and 10 MB channels in the plane of the layers. However, the transport limiting openings (6 MB) to the layers is smaller than CO2 gas molecules. In contrast, AMH-3 has

  9. 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

  10. 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. PMID:18985640

  11. A Novel Theoretical Method to Search Good Candidates of Solid Sorbents for CO2 Capture

    SciTech Connect

    Duan, Yuhua

    2008-07-01

    The increasing atmospheric CO2 concentration is the most important environmental issue of global warming that the world faces today. During past few decades, many technologies have been developing to separate and capture CO2 from coal gasifier. As high temperature CO2 absorbents, solid materials are potential candidates. Lithium silicate(Li4SiO4) and zirconate(Li2ZrO3) have been studying for CO2 capture by researchers at Toshiba and found that they absorb CO2 at 773K and release CO2 around 973K. Based on these well-known experimental exploring results on these lithium salts, we have been developing a novel theoretical methodology to search better solid materials for CO2 capture: (1) Based on the crystal structures of solids, the density functional calculations are performed to obtain their electronic structural properties and their binding energies. The energy change(ΔE) for the reaction solid_sorbent+CO2 ↔ sorbent_CO2+ solid are evaluated. (2) For a vast of data-bank of solid materials, as our first filter if |ΔE|<|ΔGLi2SiO4|, where ΔG is the free energy change for reaction of Li2SiO4+CO2↔ Li2CO3 +Li2SiO3, we select this solid as a potential good candidate for CO2 capture. (3) For these possible candidates, we further perform phonon calculations and obtain their vibration frequencies. With them, partition functions of solids(Z) can be calculated out. With Z, the thermal dynamical properties (zero point energy, entropy, enthalpy, free energy, etc.) under different conditions (temperature(T), pressure(P)) can be readily calculated. With them, the chemical potentials(Δμ)(functional of T and P) for the sorption/desorption reaction are evaluated. (4) Using Δμ as our second filter, we can reduce the number of our selected good candidates to a small number of better candidates. (5) The last step is to make the fine tune (the 3rd filter) the better candidates to a small set of the best candidates by considering the operating conditions(T, P, etc.), absorbing

  12. Synthetic Catalysts for CO2 Storage: Catalytic Improvement of Solvent Capture Systems

    SciTech Connect

    2010-08-15

    IMPACCT Project: LLNL is designing a process to pull CO2 out of the exhaust gas of coal-fired power plants so it can be transported, stored, or utilized elsewhere. Human lungs rely on an enzyme known as carbonic anhydrase to help separate CO2 from our blood and tissue as part of the normal breathing process. LLNL is designing a synthetic catalyst with the same function as this enzyme. The catalyst can be used to quickly capture CO2 from coal exhaust, just as the natural enzyme does in our lungs. LLNL is also developing a method of encapsulating chemical solvents in permeable microspheres that will greatly increase the speed of binding of CO2. The goal of the project is an industry-ready chemical vehicle that can withstand the harsh environments found in exhaust gas and enable new, simple process designs requiring less capital investment.

  13. Capture CO2 from Ambient Air Using Nanoconfined Ion Hydration.

    PubMed

    Shi, Xiaoyang; Xiao, Hang; Lackner, Klaus S; Chen, Xi

    2016-03-14

    Water confined in nanoscopic pores is essential in determining the energetics of many physical and chemical systems. Herein, we report a recently discovered unconventional, reversible chemical reaction driven by water quantities in nanopores. The reduction of the number of water molecules present in the pore space promotes the hydrolysis of CO3(2-) to HCO3(-) and OH(-). This phenomenon led to a nano-structured CO2 sorbent that binds CO2 spontaneously in ambient air when the surrounding is dry, while releasing it when exposed to moisture. The underlying mechanism is elucidated theoretically by computational modeling and verified by experiments. The free energy of CO3 (2-) hydrolysis in nanopores reduces with a decrease of water availability. This promotes the formation of OH(-), which has a high affinity to CO2 . The effect is not limited to carbonate/bicarbonate, but is extendable to a series of ions. Humidity-driven sorption opens a new approach to gas separation technology. PMID:26914978

  14. 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

  15. 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. PMID:26803257

  16. Nitrogen-rich porous adsorbents for CO2 capture and storage.

    PubMed

    Li, Pei-Zhou; Zhao, Yanli

    2013-08-01

    The construction of physical or chemical adsorbents for CO2 capture and sequestration (CCS) is a vital technology in the interim period on the way towards a sustainable low-carbon future. The search for efficient materials to satisfy the increasing demand for CCS has become extremely important. Porous materials, including porous silica, porous carbons, and newly developed metal-organic frameworks and porous organic polymers, possessing regular and well-defined porous geometry and having a high surface area and pore volume, have been widely studied for separations on laboratory scale. On account of the dipole-quadrupole interactions between the polarizable CO2 molecule and the accessible nitrogen site, the investigations have indicated that the incorporation of accessible nitrogen-donor groups into the pore walls of porous materials can improve the affinity to CO2 and increase the CO2 uptake capacity and selectivity. The CO2 -adsorption process based on solid nitrogen-rich porous adsorbents does generally not require heating of a large amount of water (60-70 wt%) for regeneration, while such a heating approach cannot be avoided in the regeneration of amine-based solution absorption processes. Thus, nitrogen-rich porous adsorbents show good regeneration properties without sacrificing high separation efficiency. As such, nitrogen-rich porous materials as highly promising CO2 adsorbents have been broadly fabricated and intensively investigated. This Focus Review highlights recent significant advances in nitrogen-rich porous materials for CCS. PMID:23744799

  17. 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. PMID:27304708

  18. 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. PMID:27469274

  19. 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%.

  20. 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

  1. 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

  2. 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

  3. 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. PMID:24060087

  4. 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

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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. PMID:21323309

  10. 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.

  11. 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. PMID:26388535

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

    SciTech Connect

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

    2011-03-01

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

  13. 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. PMID:26120972

  14. Hierarchical Mesoporous Metal-Organic Frameworks for Enhanced CO2 Capture.

    PubMed

    Mao, Yiyin; Chen, Danke; Hu, Pan; Guo, Yi; Ying, Yulong; Ying, Wen; Peng, Xinsheng

    2015-10-19

    Hierarchical porous materials are promising for catalyst, separation and sorption applications. A ligand-assisted etching process is developed for template-free synthesis of hierarchical mesoporous MOFs as single crystals and well-intergrown membranes at 40 °C. At 223 K, the hierarchical porous structures significantly improve the CO2 capture capacity of HKUST-1 by more than 44 % at pressures up to 20 kPa and 13 % at 100 kPa. Even at 323 K, the enhancement of CO2 uptake is above 25 % at pressures up to 20 kPa and 7 % at 100 kPa. The mesoporous structures not only enhance the CO2 uptake capacity but also improve the diffusion and mass transportation of CO2 . Similarly, well-intergrown mesoporous HKUST-1 membranes are synthesized, which hold the potential for film-like porous devices. Mesoporous MOF-5 crystals are also obtained by a similar ligand-assisted etching process. This may provide a facile way to prepare hierarchical porous MOF single crystals and membranes for wide-ranging applications. PMID:26471435

  15. 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. PMID:27005790

  16. 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.

  17. 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...

  18. 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...

  19. SYSTEM LEVEL IMPLICATIONS OF FLEXIBLE CO2 CAPTURE OPERATION

    EPA Science Inventory

    In ERCOT, turning flexible CO2 capture systems off during infrequent periods of peak electricity demand can avoid hundreds of millions to billions of dollars in capital costs to replace the power output lost to CO2 capture energy requirements.  When CO...

  20. 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. PMID:27253328

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

    PubMed

    Zeman, Frank

    2014-10-01

    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. PMID:25207956

  2. 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.

  3. 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.

  4. Supra-molecular networks for CO2 capture

    NASA Astrophysics Data System (ADS)

    Sadowski, Jerzy; Kestell, John

    Utilizing capabilities of low-energy electron microscopy (LEEM) for non-destructive interrogation of the real-time molecular self-assembly, we have investigated supramolecular systems based on carboxylic acid-metal complexes, such as trimesic and mellitic acid, doped with transition metals. Such 2D networks can act as host systems for transition-metal phthalocyanines (MPc; M = Fe, Ti, Sc). The electrostatic interactions of CO2 molecules with transition metal ions can be tuned by controlling the type of TM ion and the size of the pore in the host network. We further applied infrared reflection-absorption spectroscopy (IRRAS) to determine of the molecular orientation of the functional groups and the whole molecule in the 2D monolayers of carboxylic acid. The kinetics and mechanism of the CO2 adsorption/desorption on the 2D molecular network, with and without the TM ion doping, have been also investigated. This research used resources of the Center for Functional Nanomaterials, which is the U.S. DOE Office of Science User Facility, at Brookhaven National Laboratory under Contract No. DE-SC0012704.

  5. 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. PMID:27020397

  6. 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

  7. 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

    2016-05-01

    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. PMID:27081869

  8. 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

    2016-09-01

    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. PMID:27458723

  9. 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.

  10. Hybrid Solvent-Membrane CO2 Capture: A Solvent/Membrane Hybrid Post-combustion CO2 Capture Process for Existing Coal-Fired Power Plants

    SciTech Connect

    2010-07-01

    IMPACCT Project: The University of Kentucky is developing a hybrid approach to capturing CO2 from the exhaust gas of coal-fired power plants. In the first, CO2 is removed as flue gas is passed through an aqueous ammonium-based solvent. In the second, carbon-rich solution from the CO2 absorber is passed through a membrane that is designed to selectively transport the bound carbon, enhancing its concentration on the permeate side. The team’s approach would combine the best of both membrane- and solventbased carbon capture technologies. Under the ARPA-E award, the team is enabling the membrane operation to be a drop-in solution.

  11. 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.

  12. Phosphonium salt incorporated hypercrosslinked porous polymers for CO2 capture and conversion.

    PubMed

    Wang, Jinquan; Wei Yang, Jason Gan; Yi, Guangshun; Zhang, Yugen

    2015-11-01

    Various novel hypercrosslinked porous polymers with phosphonium salt incorporated into their networks were developed. These porous materials have high BET surface areas (up to 1168 m(2) g(-1)) and can be used to selectively capture CO2 and efficiently convert CO2 into cyclic carbonates. PMID:26365361

  13. Polymer blend membranes for CO2 separation from natural gas

    NASA Astrophysics Data System (ADS)

    Mukhtar, H.; Mannan, H. A.; Minh, D.; Nasir, R.; Moshshim, D. F.; Murugesan, T.

    2016-06-01

    Polymeric membranes are dominantly used in industrial gas separation membrane processes. Enhancement in membranes permeability and/or selectivity is a key challenge faced by membrane researchers. The current work represents the effect of poyetherimide blending on separation performance of polysulfone membranes. Polysulfone/poyetherimide (PSF/PEI) blend flat sheet dense membranes were synthesized and tested for permeation analysis of CO2 and CH4 gases at 6, 8 and 10 bar pressure and 25oC temperature. Morphology and thermal properties of membranes were characterized by field emission scanning electron microscope (FESEM) and thermo gravimetric analysis (TGA) respectively. Blend membranes were dense and homogeneous as deduced from FESEM analysis. Thermal stability of synthesized blend membranes was maintained by blending with PEI as characterized by TGA results. Decrease in permeability of both gases was observed by the addition of PEI due to rigidity of PEI chains. Additionally, selectivity of synthesized blend membranes was enhanced by blending PEI and blend membranes show improved selectivity over pure PSF membrane. This new material has the capability to be used as gas separation membrane material.

  14. 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. PMID:27257991

  15. 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.

  16. 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.

  17. 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.

  18. Detoxifying CO2 capture reclaimer waste by anaerobic digestion.

    PubMed

    Wang, Shuai; Hovland, Jon; Brooks, Steven; Bakke, Rune

    2014-01-01

    The decrease in toxicity of carbon capture reclaimer monoethanolamine (MEA) waste (MEAw) during anaerobic degradation of such waste together with easily degradable organics was investigated. Samples were collected from a bioreactor at steady state with 86 % organic chemical oxygen demand removal at room temperature, which had been running on MEAw for 2 years. The toxicity of the digester effluents were 126, 42 and 10 times lower than that of the MEAw to the tested freshwater trophic groups of Pseudokirchneriella subcapitata, Daphnia magna and embryos of Danio rerio, respectively. The toxicity of the tested taxonomic groups after anaerobic digestion was mainly attributed to the ammonia generated by the degradation of MEAw. PMID:24122630

  19. 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.

  20. Superstructure-based optimal design of PSA cycles for post-combustion CO2 capture

    SciTech Connect

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

    2009-07-01

    Recent developments have shown pressure/vacuum swing adsorption (PSA/VSA) to be a promising option to effectively capture CO2 from flue gas streams. In most commercial PSA cycles, the weakly adsorbed component in the mixture is the desired product, and enriching the strongly adsorbed CO2 is not a concern. Thus, it is necessary to develop PSA processes specifically targeted to obtain pure strongly adsorbed component. So far, no systematic methodology has been suggested in the literature to design PSA cycles for high purity CO2 capture. This study addresses this need and presents a systematic optimization-based formulation to synthesize PSA cycles. In particular, a novel PSA superstructure is presented to design optimal PSA cycle configurations and evaluate CO2 capture strategies. The superstructure is rich enough to predict a number of different PSA operating steps. The bed connections in the superstructure are governed by timedependent control variables, which can be varied to realize most PSA operating steps. An optimal sequence of operating steps is achieved through the formulation of an optimal control problem with the partial differential and algebraic equations of the PSA system and the cyclic steady state condition. The superstructure approach is demonstrated for case studies related to post-combustion CO2 capture. In particular, optimal PSA cycles were synthesized which maximize CO2 recovery for a given purity, and minimize overall power consumption. The results show the potential of the superstructure to predict PSA cycles with up to 98% purity and recovery of CO2. Moreover, for recovery of around 85% and purity of over 90%, these cycles can recover CO2 from atmospheric flue gas with a low power consumption of 465 kWh/tonne CO2. The approach presented is, therefore, very promising and quite useful for evaluating the suitability of different adsorbents, feedstocks and operating strategies for PSA, and assessing its usefulness for CO2 capture.

  1. A superstructure-based optimal synthesis of PSA cycles for post-combustion CO2 capture

    SciTech Connect

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

    2010-07-01

    Recent developments have shown pressure/vacuum swing adsorption (PSA/VSA) to be a promising option to effectively capture CO2 from flue gas streams. In most 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, it is necessary to concentrate CO2 to high purity to reduce CO2 sequestration costs and minimize safety and environmental risks. Thus, it is necessary to develop PSA processes specifically targeted to obtain pure strongly adsorbed component. A multitude of PSA/VSA cycles have been developed in the literature for CO2 capture from feedstocks low in CO2 concentration. However, no systematic methodology has been suggested to develop, evaluate, and optimize PSA cycles for high purity CO2 capture. This study presents a systematic optimization-based formulation to synthesize novel PSA cycles for a given application. In particular, a novel PSA superstructure is presented to design optimal PSA cycle configurations and evaluate CO2 capture strategies. The superstructure is rich enough to predict a number of different PSA operating steps. The bed connections in the superstructure are governed by time-dependent control variables, which can be varied to realize most PSA operating steps. An optimal sequence of operating steps is achieved through the formulation of an optimal control problem with the partial differential and algebraic equations of the PSA system and the cyclic steady state condition. Large-scale optimization capabilities have enabled us to adopt a complete discretization methodology to solve the optimal control problem as a largescale nonlinear program, using the nonlinear optimization solver IPOPT. The superstructure approach is demonstrated for case studies related to post-combustion CO2 capture. In particular, optimal PSA cycles were synthesized, which maximize CO2 recovery for a given purity, and minimize overall power consumption. The

  2. 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.

  3. 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.

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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.

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

    PubMed

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

    2016-06-01

    Biochar is a porous carbonaceous material with high alkalinity and rich minerals, making it possible for CO2 capture. In this study, biochars derived from pig manure, sewage sludge, and wheat straw were evaluated for their CO2 sorption behavior. All three biochars showed high sorption abilities for CO2, with the maximum capacities reaching 18.2-34.4 mg g(-1) at 25 °C. Elevating sorption temperature and moisture content promoted the transition of CO2 uptake from physical to chemical process. Mineral components such as Mg, Ca, Fe, K, etc. in biochar induced the chemical sorption of CO2 via the mineralogical reactions which occupied 17.7%-50.9% of the total sorption. FeOOH in sewage sludge biochar was transformed by sorbed CO2 into Fe(OH)2CO3, while the sorbed CO2 in pig manure biochar was precipitated as K2Ca(CO3)2 and CaMg(CO3)2, which resulted in a dominant increase of insoluble inorganic carbon in both biochars. For wheat straw biochar, sorbed CO2 induced CaCO3 transformed into soluble Ca(HCO3)2, which led to a dominant increase of soluble inorganic carbons. The results obtained from this study demonstrated that biochar as a unique carbonaceous material could distinctly be a promising sorbent for CO2 capture in which chemical sorption induced by mineralogical reactions played an important role. PMID:26995449

  11. 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

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

    PubMed

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

    2012-08-14

    CO(2) 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 CO(2) directly from the atmosphere. Air capture of CO(2) could act as insurance against CO(2) leaking from storage and furthermore may provide an option for dealing with emissions from mobile dispersed sources such as automobiles and airplanes. PMID:22843674

  13. 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.

  14. 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.

  15. 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. PMID:24578590

  16. 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

  17. Evaluation of Solid Sorbents as a Retrofit Technology for CO2 Capture

    SciTech Connect

    Sjostrom, Sharon

    2015-09-30

    ADA completed a DOE-sponsored program titled Evaluation of Solid Sorbents as a Retrofit Technology for CO2 Capture under program DE-FE0004343. During this program, sorbents were analyzed for use in a post-combustion CO2 capture process. A supported amine sorbent was selected based upon superior performance to adsorb a greater amount of CO2 than the activated carbon sorbents tested. When the most ideal sorbent at the time was selected, it was characterized and used to create a preliminary techno-economic analysis (TEA). A preliminary 550 MW coal-fired power plant using Illinois #6 bituminous coal was designed with a solid sorbent CO2 capture system using the selected supported amine sorbent to both facilitate the TEA and to create the necessary framework to scale down the design to a 1 MWe equivalent slipstream pilot facility. The preliminary techno-economic analysis showed promising results and potential for improved performance for CO2 capture compared to conventional MEA systems. As a result, a 1 MWe equivalent solid sorbent system was designed, constructed, and then installed at a coal-fired power plant in Alabama. The pilot was designed to capture 90% of the CO2 from the incoming flue gas at 1 MWe net electrical generating equivalent. Testing was not possible at the design conditions due to changes in sorbent handling characteristics at post-regenerator temperatures that were not properly incorporated into the pilot design. Thus, severe pluggage occurred at nominally 60% of the design sorbent circulation rate with heated sorbent, although no handling issues were noted when the system was operated prior to bringing the regenerator to operating temperature. Testing within the constraints of the pilot plant resulted in 90% capture of the incoming CO2 at a flow rate equivalent of 0.2 to 0.25 MWe net electrical generating equivalent. The reduction in equivalent flow rate at 90% capture was primarily the result of sorbent circulation limitations at operating

  18. 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

  19. 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

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

    DOE PAGESBeta

    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

  1. 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

  2. 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. PMID:18853819

  3. 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 . PMID:24203891

  4. 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

  5. EFFICIENT THEORETICAL SCREENING OF SOLID SORBENTS FOR CO2 CAPTURE APPLICATIONS

    SciTech Connect

    Duan, Yuhua; Sorescu, Dan C; Luebke, David

    2011-01-01

    Carbon dioxide is a major combustion product of coal, which once released into the air can contribute to global climate change. Current CO2 capture technologies for power generation processes including amine solvents and CaO-based sorbent materials require very energy intensive regeneration steps which result in significantly decreased efficiency. Hence, there is a critical need for new materials that can capture and release CO2 reversibly with acceptable energy costs if CO2 is to be captured and sequestered economically. Inorganic sorbents are one such class of materials which typically capture CO2 through the reversible formation of carbonates. 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 identifying 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 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, either from databases or from calculations, are further used for computing the thermodynamic reaction equilibrium properties of the CO2 absorption/desorption cycle based on the chemical potential and heat of reaction. Only those solid materials for which lower capture energy costs are predicted at the desired process conditions are selected as CO2 sorbent candidates and further considered for experimental validations. Solid sorbents containing

  6. 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.

  7. 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. PMID:26512792

  8. 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.

  9. Preparation and characterization of aminated graphite oxide for CO2 capture

    NASA Astrophysics Data System (ADS)

    Zhao, Yunxia; Ding, Huiling; Zhong, Qin

    2012-03-01

    Adsorption with solid sorbents is one of the most promising options for postcombustion carbon dioxide (CO2) capture. In this study, aminated graphite oxide used for CO2 adsorption was synthesized, based on the intercalation reaction of graphite oxide (GO) with amines, including ethylenediamine (EDA), diethylenetriamine (DETA) and triethylene tetramine (TETA). The structural information, surface chemistry and thermal behavior of the adsorbent samples were characterized by X-ray powder diffraction (XRD), infrared spectroscopy (IR), transmission electron microscope (TEM), elemental analysis, particle size analysis, nitrogen adsorption as well as differential thermal and thermogravimetric analysis (DSC-TGA). CO2 capture was investigated by dynamic adsorption experiments with N2sbnd CO2 mixed gases at 30 °C. The three kinds of graphite oxide samples modified by excess EDA, DETA and TETA showed similar adsorption behaviors seen from their breakthrough curves. Among them, the sample aminated by EDA exhibited the highest adsorption capacity with the longest breakthrough time of CO2. Before saturation, its adsorption capacity was up to 53.62 mg CO2/g sample. In addition, graphite oxide samples modified by different amount of EDA (EDA/GO raw ratio 10 wt%, 50 wt% and 100 wt%) were prepared in the ethanol. Their CO2 adsorption performance was investigated. The experimental results demonstrated that graphite oxide with 50 wt% EDA had the largest adsorption capacity 46.55 mg CO2/g sample.

  10. 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].

  11. 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. PMID:24022119

  12. 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

  13. Tailoring open metal sites for selective capture of CO2 in isostructural metalloporphyrin porous organic networks

    NASA Astrophysics Data System (ADS)

    Choi, Hwa Seob; Jeon, Hyung Joon; Choi, Jung Hoon; Lee, Gyu-Heon; Kang, Jeung Ku

    2015-11-01

    Porphyrin-based isostructural porous organic networks have been synthesized by varying the central metal atoms to cobalt, nickel and copper. Their selectivities for CO2 capture over N2 and Ar are found to be enhanced as the heats of adsorption for CO2 are increased in the order of Co, Ni and Cu, while the pore structures are well maintained.Porphyrin-based isostructural porous organic networks have been synthesized by varying the central metal atoms to cobalt, nickel and copper. Their selectivities for CO2 capture over N2 and Ar are found to be enhanced as the heats of adsorption for CO2 are increased in the order of Co, Ni and Cu, while the pore structures are well maintained. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr05696a

  14. Rational design and synthesis of a porous, task-specific polycarbazole for efficient CO2 capture.

    PubMed

    Jin, Tian; Xiong, Yan; Zhu, Xiang; Tian, Ziqi; Tao, Duan-Jian; Hu, Jun; Jiang, De-en; Wang, Hualin; Liu, Honglai; Dai, Sheng

    2016-03-25

    We present a rational design and synthesis of a novel porous pyridine-functionalized polycarbazole for efficient CO2 capture based on the density functional theory calculations. The task-specific polymer, generated through a one-step FeCl3-catalyzed oxidative coupling reaction, exhibits a superior CO2 uptake at 1.0 bar and 273 K (5.57 mmol g(-1)). PMID:26864392

  15. 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

  16. 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.

  17. 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.

  18. 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.

  19. 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. PMID:26660453

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

    PubMed

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

    2015-09-01

    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 . PMID:26073178

  1. 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.

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

    PubMed

    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

  3. 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

  4. 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.

  5. 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. PMID:24918477

  6. 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. PMID:24747397

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

    PubMed

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

    2014-12-16

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

  8. 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

    2015-11-01

    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. PMID:26435384

  9. Energy requirements for CO2 capture from ambient air (DAC) competitive with capture from flue-gas (PCC)

    NASA Astrophysics Data System (ADS)

    Meinrenken, Christoph

    2015-03-01

    Capture of CO2, whether from a flue gas source (PCC) or from distributed sources via ambient air (DAC), is a key enabling technology to provide carbon for sustainable synthetic energy carriers such as solar fuels. Based on thermodynamic minimum considerations, DAC is often expected to require about 3 times more energy (per ton CO2 captured) than PCC because CO2 in ambient air is more dilute. Here, we calculate the energy required for a humidity swing-based DAC installation that uses an anionic exchange resin as sorbent. The calculation uses recently measured equilibrium CO2 loadings of the sorbent as function of partial CO2 pressure, temperature, and humidity. We calculate the installation's electricity consumption to be about 45 kJ per mole of pure CO2 at 1 bar (scenario-dependent). Furthermore, we estimate the amount of heat provided by ambient air and thus provide context of the overall energy and entropy balance and thermodynamic minimum views. The electricity consumption is competitive with typical parasitic loads of PCC-equipped coal-fired power plants (40-50 kJ per mole at same pressure) and significantly lower than predicted for other DAC installations such as Na(OH) sorbent-based systems. Our analyses elucidate why DAC is not always more energy-intensive that PCC, thus alleviating often cited concerns of significant cost impediments. Financial support by ABB for research presented herein is gratefully acknowledged.

  10. Cycle development and design for CO2 capture from flue gas by vacuum swing adsorption.

    PubMed

    Zhang, Jun; Webley, Paul A

    2008-01-15

    CO2 capture and storage is an important component in the development of clean power generation processes. One CO2 capture technology is gas-phase adsorption, specifically pressure (or vacuum) swing adsorption. The complexity of these processes makes evaluation and assessment of new adsorbents difficult and time-consuming. In this study, we have developed a simple model specifically targeted at CO2 capture by pressure swing adsorption and validated our model by comparison with data from a fully instrumented pilot-scale pressure swing adsorption process. The model captures nonisothermal effects as well as nonlinear adsorption and nitrogen coadsorption. Using the model and our apparatus, we have designed and studied a large number of cycles for CO2 capture. We demonstrate that by careful management of adsorption fronts and assembly of cycles based on understanding of the roles of individual steps, we are able to quickly assess the effect of adsorbents and process parameters on capture performance and identify optimal operating regimes and cycles. We recommend this approach in contrast to exhaustive parametric studies which tend to depend on specifics of the chosen cycle and adsorbent. We show that appropriate combinations of process steps can yield excellent process performance and demonstrate how the pressure drop, and heat loss, etc. affect process performance through their effect on adsorption fronts and profiles. Finally, cyclic temperature profiles along the adsorption column can be readily used to infer concentration profiles-this has proved to be a very useful tool in cyclic function definition. Our research reveals excellent promise for the application of pressure/vacuum swing adsorption technology in the arena of CO2 capture from flue gases. PMID:18284163

  11. 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. PMID:26121208

  12. Folding of graphene slit like pore walls—a simple method of improving CO2 separation from mixtures with CH4 or N2

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

    We report for the first time a detailed procedure for creating a simulation model of energetically stable, folded graphene-like pores and simulation results of CO2/CH4 and CO2/N2 separation using these structures. We show that folding of graphene structures is a very promising method to improve the separation of CO2 from mixtures with CH4 and N2. The separation properties of the analysed materials are compared with carbon nanotubes having similar diameters or S/V ratio. The presented results have potential importance in the field of CO2 capture and sequestration.

  13. Folding of graphene slit like pore walls--a simple method of improving CO2 separation from mixtures with CH4 or N2.

    PubMed

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

    2014-12-01

    We report for the first time a detailed procedure for creating a simulation model of energetically stable, folded graphene-like pores and simulation results of CO2/CH4 and CO2/N2 separation using these structures. We show that folding of graphene structures is a very promising method to improve the separation of CO2 from mixtures with CH4 and N2. The separation properties of the analysed materials are compared with carbon nanotubes having similar diameters or S/V ratio. The presented results have potential importance in the field of CO2 capture and sequestration. PMID:25352074

  14. 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.

  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. PMID:27315143

  16. Integration of CO2 capture and mineral carbonation by using recyclable ammonium salts.

    PubMed

    Wang, Xiaolong; Maroto-Valer, M Mercedes

    2011-09-19

    A new approach to capture and store CO(2) by mineral carbonation using recyclable ammonium salts was studied. This process integrates CO(2) capture with mineral carbonation by employing NH(3), NH(4)HSO(4), and NH(4)HCO(3) in the capture, mineral dissolution, and carbonation steps, respectively. NH(4)HSO(4) and NH(3) can then be regenerated by thermal decomposition of (NH(4))(2)SO(4). The use of NH(4)HCO(3) as the source of CO(2) can avoid desorption and compression of CO(2). The mass ratio of Mg/NH(4)HCO(3)/NH(3) is the key factor controlling carbonation and the optimum ratio of 1:4:2 gives a conversion of Mg ions to hydromagnesite of 95.5%. Thermogravimetric analysis studies indicated that the regeneration efficiency of NH(4)HSO(4) and NH(3) in this process is 95%. The mass balance of the process shows that about 2.63 tonnes of serpentine, 0.12 tonnes of NH(4)HSO(4), 7.48 tonnes of NH(4)HCO(3), and 0.04 tonnes of NH(3) are required to sequester 1 tonne of CO(2) as hydromagnesite. PMID:21732542

  17. A Biomimetic Three-Dimensional Gas Exchange Unit for CO 2 Capture

    NASA Astrophysics Data System (ADS)

    Nguyen, Du Thai

    For the capture of CO2 from mixed gas streams, materials for increased gas exchange are necessary. Efficient gas exchange systems already exist in the form of vascularized lung-tissue. Herein we report a fabrication technique for the synthesis of three-dimensional microvascular gas exchange units capable of removing CO2 from flowing gas created using the recently reported Vaporization of a Sacrificial Component (VaSC) technique. We demonstrate the spatiotemporal pattern of CO2 reactivity in the microvascular gas exchange unit using colorimetric, pH sensitive dyes. Control over three-dimensional placement of channels is shown to increase capture efficiencies. A computational finite element model validates and explains the experimental observations.

  18. 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. PMID:26706226

  19. The effect of pyridine modification of Ni-DOBDC on CO2 capture under humid conditions.

    PubMed

    Bae, Youn-Sang; Liu, Jian; Wilmer, Christopher E; Sun, Hahnbi; Dickey, Allison N; Kim, Min Bum; Benin, Annabelle I; Willis, Richard R; Barpaga, Dushyant; LeVan, M Douglas; Snurr, Randall Q

    2014-03-28

    The metal-organic framework Ni-DOBDC was modified with pyridine molecules to make the normally hydrophilic internal surface more hydrophobic. Experiments and molecular simulations show that the pyridine modification reduces H2O adsorption while retaining substantial CO2 capacity under the conditions of interest for carbon capture from flue gas. PMID:24527490

  20. 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

  1. 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.

  2. Synthesis of DNL-6 with a high concentration of Si (4 Al) environments and its application in CO(2) separation.

    PubMed

    Su, Xiong; Tian, Peng; Fan, Dong; Xia, Qinghua; Yang, Yue; Xu, Shutao; Zhang, Lin; Zhang, Ying; Wang, Dehua; Liu, Zhongmin

    2013-05-01

    The synthesis of DNL-6 with a high concentration of Si (4 Al) environments [Si/(Si+Al+P)=0.182 mol, denoted as M-DNL-6] is demonstrated. This represents the highest reported concentration of such environments in silicoaluminophosphate (SAPO) molecular sieves. Adsorption studies show that the high Si (4 Al) content in M-DNL-6, with an increased number of Brønsted acid sites in the framework, greatly promotes the adsorption of CO(2). M-DNL-6 exhibits a large CO(2) uptake capacity of up to 6.18 mmol g(-1) at 273 K and 101 kPa, and demonstrates high ratios of CO(2)/CH(4) and CO(2)/N(2) separation. From breakthrough and cycling experiments, M-DNL-6 demonstrates the ability to completely separate CO(2) from CH(4) or N(2) with a dynamic capacity of approximately 8.0 wt % before breakthrough. Importantly, the adsorbed CO(2) is easily released from the adsorbent through a simple gas purging operation at room temperature to regain 95 % of the original adsorption capacity. These results suggest that M-DNL-6 can be used as a potential adsorbent for CO(2) capture in pressure swing adsorption processes. PMID:23606439

  3. 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.

  4. 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

  5. A Parametric Study for Regenerative Ammonia-Based Scrubbing for the Capture of CO2

    SciTech Connect

    Resnik, K.P.; Garber, W.; Hreda, D.C.; Yeh, J.T.; Pennline, H.W.

    2006-09-01

    A continuous gas and liquid flow, regenerative scrubbing process for CO2 capture is currently being demonstrated at the bench-scale level. An aqueous ammonia-based solution captures CO2 from simulated flue gas in an absorber and releases a nearly pure stream of CO2 in the regenerator. After the regeneration, the solution of ammonium compounds is recycled to the absorber. The design of the continuous flow unit was based on earlier exploratory results from a semi-batch reactor, where a CO2 and N2 gas mixture flowed through a well-mixed batch of ammonia-based solution. Recently, a series of tests have been conducted on the continuous unit to observe the effect of various parameters on CO2 removal efficiency and regenerator effectiveness within the flow system. The parameters that were studied include absorber temperature, regenerator temperature, initial NH3 concentration, simulated flue gas flow rate, liquid solvent inventory in the flow system, and height of the packed-bed absorber. Results from this current testing campaign conducted in the continuous scrubbing unit as well as test results from a 5-cycle semi-batch reactor will be discussed.

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

    PubMed

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

    2013-07-01

    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. PMID:23718261

  7. 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. PMID:20724072

  8. 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.

  9. 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.

  10. 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. PMID:25401996

  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. highly selective amino acid salt solutions as absorption liquid for CO(2) capture in gas-liquid membrane contactors.

    PubMed

    Simons, Katja; Nijmeijer, Kitty; Mengers, Harro; Brilman, Wim; Wessling, Matthias

    2010-08-23

    The strong anthropogenic increase in the emission of CO(2) and the related environmental impact force the developments towards sustainability and carbon capture and storage (CCS). In the present work, we combine the high product yields and selectivities of CO(2) absorption processes with the advantages of membrane technology in a membrane contactor for the separation of CO(2) from CH(4) using amino acid salt solutions as competitive absorption liquid to alkanol amine solutions. Amino acids, such as sarcosine, have the same functionality as alkanol amines (e.g., monoethanolamine=MEA), but in contrast, they exhibit a better oxidative stability and resistance to degradation. In addition, they can be made nonvolatile by adding a salt functionality, which significantly reduces the liquid loss due to evaporation at elevated temperatures in the desorber. Membrane contactor experiments using CO(2)/CH(4) feed mixtures to evaluate the overall process performance, including a full absorption/desorption cycle show that even without a temperature difference between absorber and desorber, a CO(2)/CH(4) selectivity of over 70 can be easily achieved with the sarcosine salt solution as absorption liquid. This selectivity reaches values of 120 at a temperature difference between absorber and desorber of 35 degrees C, compared to a value of only 60 for MEA under the same conditions. Although CO(2) permeance values are somewhat lower than the values obtained for MEA, the results clearly show the potential of amino acid salt solutions as competitive absorption liquids for the energy efficient removal of CO(2). In addition, due to the low absorption of CH(4) in sarcosine compared to MEA, the loss of CH(4) is reduced and significantly higher CH(4) product yields can be obtained. PMID:20623726

  13. Polyethyleneimine Incorporated Metal-Organic Frameworks Adsorbent for Highly Selective CO2 Capture

    PubMed Central

    Lin, Yichao; Yan, Qiuju; Kong, Chunlong; Chen, Liang

    2013-01-01

    A series of polyethyleneimine (PEI) incorporated MIL-101 adsorbents with different PEI loadings were reported for the first time in the present work. Although the surface area and pore volume of MIL-101 decreased significantly after loading PEI, all the resulting composites exhibited dramatically enhanced CO2 adsorption capacity at low pressures. At 100 wt% PEI loading, the CO2 adsorption capacity at 0.15 bar reached a very competitive value of 4.2 mmol g−1 at 25°C, and 3.4 mmol g−1 at 50°C. More importantly, the resulting adsorbents displayed rapid adsorption kinetics and ultrahigh selectivity for CO2 over N2 in the designed flue gas with 0.15 bar CO2 and 0.75 bar N2. The CO2 over N2 selectivity was up to 770 at 25°C, and 1200 at 50°C. We believe that the PEI based metal-organic frameworks is an attractive adsorbent for CO2 capture. PMID:23681218

  14. 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.

  15. 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.

  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. PMID:26515558

  17. Prospective life-cycle modeling of a carbon capture and storage system using metal-organic frameworks for CO2 capture

    SciTech Connect

    Sathre, R; Masanet, E

    2013-01-01

    Metal-organic frameworks (MOFs) are promising new material media for carbon dioxide (CO2) capture. Their tunable adsorption patterns may allow relatively efficient separation of gases, e.g. from power plant exhaust. Here we conduct scenario-based prospective life-cycle system modeling to estimate the potentials and implications of large-scale MOF application for post-combustion carbon capture and storage (CCS), and estimate the source and magnitude of uncertainties. The methodological approach includes parametric system modeling to quantify relations between system components; scenario projections of plausible pathways for system scale-up; proxy data on analogous materials and processes; and uncertainty analysis of parameter significance. We estimate the system-wide material and energy flows and economic costs associated with projected large-scale CCS deployment. We compare the performance of a MOF-based system to currently more mature amine-based capture technology. We discuss balancing two critical factors that determine the success of CO2 capture media: thermodynamic efficiency of the capture/regeneration cycle, and life-cycle embodied energy and cost of the material and its ancillary systems.

  18. High CO2-capture ability of a porous organic polymer bifunctionalized with carboxy and triazole groups.

    PubMed

    Xie, Lin-Hua; Suh, Myunghyun Paik

    2013-08-26

    A new porous organic polymer, SNU-C1, incorporating two different CO2 -attracting groups, namely, carboxy and triazole groups, has been synthesized. By activating SNU-C1 with two different methods, vacuum drying and supercritical-CO2 treatment, the guest-free phases, SNU-C1-va and SNU-C1-sca, respectively, were obtained. Brunauer-Emmett-Teller (BET) surface areas of SNU-C1-va and SNU-C1-sca are 595 and 830 m(2) g(-1), respectively, as estimated by the N2-adsorption isotherms at 77 K. At 298 K and 1 atm, SNU-C1-va and SNU-C1-sca show high CO2 uptakes, 2.31 mmol  g(-1) and 3.14 mmol  g(-1), respectively, the high level being due to the presence of abundant polar groups (carboxy and triazole) exposed on the pore surfaces. Five separation parameters for flue gas and landfill gas in vacuum-swing adsorption were calculated from single-component gas-sorption isotherms by using the ideal adsorbed solution theory (IAST). The data reveal excellent CO2-separation abilities of SNU-C1-va and SNU-C1-sca, namely high CO2-uptake capacity, high selectivity, and high regenerability. The gas-cycling experiments for the materials and the water-treated samples, experiments that involved treating the samples with a CO2-N2 gas mixture (15:85, v/v) followed by a pure N2 purge, further verified the high regenerability and water stability. The results suggest that these materials have great potential applications in CO2 separation. PMID:23881821

  19. Synthesis and characterization of MOF-aminated graphite oxide composites for CO2 capture

    NASA Astrophysics Data System (ADS)

    Zhao, Yunxia; Ding, Huiling; Zhong, Qin

    2013-11-01

    A kind of metal-organic frameworks (MOF-5) and aminated graphite oxide (AGO) composites were prepared for CO2 capture to mitigate global warming. MOF-5, MOF-5/GO (composite of MOF-5 and graphite oxide) and MOF-5/AGO samples were characterized by X-ray powder diffraction (XRD), infrared spectroscopy (IR), scanning electron microscope (SEM), nitrogen adsorption as well as thermogravimetric analysis to figure out their chemistry and structure information. Three types of samples with suitable specific surface area and pore diameter were chosen to test CO2 adsorption performance and stability under humidity conditions. The results indicate that high surface area and pore volume, pore similar in size to the size of gas adsorbate, and extra reactive sites modified in the composites contributes to the high CO2 capacity. Besides, the composites involved by GO or AGO show better anti-moisture performance than the parent MOF.

  20. 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.

  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. 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

  3. Hydrothermal synthesis of N-doped spherical carbon from carboxymethylcellulose for CO2 capture

    NASA Astrophysics Data System (ADS)

    Wu, Qiong; Li, Wei; Liu, Shouxin; Jin, Chunde

    2016-04-01

    Spherical carbonaceous adsorbents (CSn) with micro-porosity developed for CO2 capture were prepared by a simple hydrothermal carbonization of carboxymethylcellulose (CMC) in the presence of urea, and activated in a high temperature N2 atmosphere. The effects of specific surface area, pore structure, and N content on the CO2 adsorption capacity were systematically investigated. Urea was found to react with surface carbonyl groups and other intermediate products generated by CMC hydrothermal carbonization, which produced highly spherical morphologies that also exhibited some ordered lattice structures. The particle size of N-doped CSn was larger than that of particles prepared without urea. Nitrogen was mainly present in pyridine (N-6), pyrrolic/pyridone (N-5) and quaternary (N-Q) forms. The high CO2 capture capacity was produced by a combination of N-doping and developing micro-pore structures. At an adsorption pressure of 1 bar, the capacity was dominated by the micro-porosity. However, during initial, lower pressures the N content dominated the CO2 adsorption capacity.

  4. Characterization of carbonic anhydrase II from Chlorella vulgaris in bio-CO2 capture.

    PubMed

    Li, Li; Fu, Ming-Lai; Zhao, Yong-Hao; Zhu, Yun-Tian

    2012-11-01

    Carbonic anhydrase II (CA II) can catalyze the reversible hydration reaction of CO(2) at a maximum of 1.4 × 10(6) molecules of CO(2) per second. The crude intracellular enzyme extract containing CA II was derived from Chlorella vulgaris. A successful CO(2) capture experiment with the presence of calcium had been conducted on the premise that the temperature was conditioned at a scope of 30-40 °C, that the biocatalyst-nurtured algal growth period lasted 3 days, and that pH ranged from7.5 to 8.5. Ions of K(+), Na(+), Ca(2+), Co(2+), Cu(2+), Fe(3+), Mg(2+), Mn(2+), and Zn(2+) at 0.01, 0.1, and 0.5 M were found to exhibit no more than 30 % inhibition on the residual activity of the biocatalyst. It is reasonable to expect that calcification catalyzed by microalgae presents an alternative to geological carbon capture and sequestration through a chain of fundamental researches carried on under the guidance of sequestration technology. PMID:22821342

  5. CO2 Capture Using Electric Fields: Low-Cost Electrochromic Film on Plastic for Net-Zero Energy Building

    SciTech Connect

    2010-01-01

    Broad Funding Opportunity Announcement Project: Two faculty members at Lehigh University created a new technique called supercapacitive swing adsorption (SSA) that uses electrical charges to encourage materials to capture and release CO2. Current CO2 capture methods include expensive processes that involve changes in temperature or pressure. Lehigh University’s approach uses electric fields to improve the ability of inexpensive carbon sorbents to trap CO2. Because this process uses electric fields and not electric current, the overall energy consumption is projected to be much lower than conventional methods. Lehigh University is now optimizing the materials to maximize CO2 capture and minimize the energy needed for the process.

  6. 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

    2013-07-01

    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. PMID:23745611

  7. 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. PMID:27004536

  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. 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.

  10. 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. PMID:26840979

  11. 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. PMID:24591345

  12. 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

  13. Multiwell 14CO2-capture assay for evaluation of substrate oxidation rates of cells in culture.

    PubMed

    Collins, C L; Bode, B P; Souba, W W; Abcouwer, S F

    1998-05-01

    14CO2 capture is commonly used to evaluate the cellular oxidation rate of respiratory substrates. A modification of the established 14CO2-capture method was developed that enables the use of cells in adherent culture and easy analysis of multiple samples under different culture conditions. The use of commercially available culture and filter plates designed for use in a multiplate scintillation spectrophotometer enabled substrate oxidation rates to be evaluated for cells in a 24-well plate format without the need to dislodge the cells from the culture substrate as is required in traditional methods. Evaluation of radioactivity captured in potassium hydroxide-saturated filters was accomplished by adding scintillation fluid to the filter plate wells and counting. Alternatively, filters could be removed and placed in vials for evaluation in a conventional scintillation counter. This method was applied to the oxidation of 14C-glutamine by human breast cell lines and demonstrated concentration-dependent linear accumulation of captured counts. PMID:9591130

  14. 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.

  15. A Highly Permeable Aligned Montmorillonite Mixed-Matrix Membrane for CO2 Separation.

    PubMed

    Qiao, Zhihua; Zhao, Song; Wang, Jixiao; Wang, Shichang; Wang, Zhi; Guiver, Michael D

    2016-08-01

    Highly permeable montmorillonite layers bonded and aligned with the chain stretching orientation of polyvinylamineacid are immobilized onto a porous polysulfone substrate to fabricate aligned montmorillonite/polysulfone mixed-matrix membranes for CO2 separation. High-speed gas-transport channels are formed by the aligned interlayer gaps of the modified montmorillonite, through which CO2 transport primarily occurs. High CO2 permeance of about 800 GPU is achieved combined with a high mixed-gas selectivity for CO2 that is stable over a period of 600 h and independent of the water content in the feed. PMID:27312314

  16. Immobilization of carbonic anhydrase on carboxyl-functionalized ferroferric oxide for CO2 capture.

    PubMed

    Lv, Bihong; Yang, Zhaoren; Pan, Fujun; Zhou, Zuoming; Jing, Guohua

    2015-08-01

    New materials of Fe3O4 magnetic microspheres were functionalized with carboxyl and prepared for carbonic anhydrase (CA) immobilization to capture CO2. The optimum conditions for immobilization, such as carrier dose, enzyme dose, pH, shaking speed, temperature and contact time, were determined. The pH and thermal stability of the free and the immobilized CA were compared. The results presented that the immobilized CA had a better enzyme activity, a higher pH and thermal stability than that of the free CA. Meanwhile, CO2 capture was respectively enhanced by the free and the immobilized CA in tris(hydroxymethyl) aminomethane (Tris) buffer solution. Moreover, the immobilized CA maintained 58.5% of its initial catalytic ability even after ten recovery cycles due to the protest of the magnetic microspheres. All the results confirmed the potential use of the carboxyl-functionalized Fe3O4 magnetic microspheres immobilized CA to remove CO2 from air or flue gas. PMID:26038102

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

    PubMed

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

    2014-12-01

    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). PMID:24441866

  18. 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. PMID:20547055

  19. 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

  20. DEVELOPMENT OF MESOPOROUS MEMBRANE MATERIALS FOR CO2 SEPARATION

    SciTech Connect

    Wei-Heng Shih; Tejas Patil; Qiang Zhao

    2003-03-25

    The huge emissions of carbon dioxide from fossil fuel fired power plants and industrial plants over the last century have resulted in an increase of the atmospheric carbon dioxide concentration. Climatological modeling work has predicted severe climate disruption as a result of the trapping of heat due to CO{sub 2}. As an attempt to address this global warming effect, DOE has initiated the Vision 21 concept for future power plants. We first synthesized mesoporous aluminosilicates that have high surface area and parallel pore channels for membrane support materials. Later we synthesized microporous aluminosilicates as the potential thin membrane materials for selective CO{sub 2} adsorption. The pore size is controlled to be less that 1 nm so that the adsorption of CO{sub 2} on the pore wall will block the passage of N{sub 2}. Mesoporous and precipitated alumina were synthesized as the base material for CO{sub 2} adsorbent. The porous alumina is doped with Ba to enhance its CO{sub 2} affinity due to the basicity of Ba. It is shown by gas chromatograph (GC) that the addition of Ba enhances the separation CO{sub 2} from N{sub 2}. It was found that mesoporous alumina has larger specific surface area and better selectivity of CO{sub 2} than precipitated alumina. Ba improves the affinity of mesoporous alumina with CO{sub 2}. Phase may play an important role in selective adsorption of CO{sub 2}. It is speculated that mesoporous alumina is more reactive than precipitated alumina creating the xBaO {center_dot}Al{sub 2}O{sub 3} phase that may be more affinitive to CO{sub 2} than N{sub 2}. On the other hand, the barium aluminates phase (Ba{sub 3}Al{sub 2}O{sub 6}) in the mesoporous sample does not help the adsorption of CO{sub 2}. Microporous aluminosilicate was chosen as a suitable candidate for CO{sub 2}/N{sub 2} separation because the pore size is less than 10 {angstrom}. If a CO{sub 2} adsorbent is added to the microporous silica, the adsorption of CO{sub 2} can block the

  1. 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. PMID:27388208

  2. Combustion Characteristics of Oxy-fuel Burners for CO2 Capturing Boilers

    NASA Astrophysics Data System (ADS)

    Ahn, Joon; Kim, Hyouck Ju; Choi, Kyu Sung

    Oxy-fuel boilers have been developed to capture CO2 from the exhaust gas. A 50 kW class model burner has been developed and tested in a furnace type boiler. The burner has been scaled up to 0.5 and 3 MW class for fire-tube type boilers. The burners are commonly laid out in a coaxial type to effectively heat the combustion chamber of boilers. Burners are devised to support air and oxy-fuel combustion modes for the retrofitting scenario. FGR (flue gas recirculation) has been tried during the scale-up procedure. Oxy-fuel combustion yields stretched flame to uniformly heat the combustion chamber. It also provides the high CO2 concentration, which is over 90% in dry base. However, pure oxy-fuel combustion increases NO concentration, because of the reduced flow rate. The FGR can suppress the thermal NOx induced by the infiltration of the air.

  3. CO2 Capturing and Mineralization by (Mg)-Phyllosilicate Coated with Fabrics.

    PubMed

    Song, Dongsu; Lee, Young-Chul; Park, Seung Bin; Han, Jong-In

    2016-05-01

    To promote the practicality of magnesium (Mg)-phyllosilicate as a potent carbonation agent, two inexpensive cotton and nylon fabrics are selected and examined to assess their feasibility for use as supporting media of Mg-phyllosilicate. Mg-phyllosilicate is coated onto the fabrics via a sol-gel method, whose mechanism is explained. The characteristics of the Mg-phyllosilicate coated cotton, along with those of the carbonation products, are explored. Mg-phyllosilicate is found to mediate the carbon dioxide (CO2) mineralization process actively, even on cotton of a supporting material. Conclusively, the obtained results clearly support the potential of mineralization as a feasible option for capturing CO2, in particular with the abiotic catalyst of Mg-phyllosilicate coated onto flexible cotton. PMID:27483872

  4. DEVELOPMENT OF MESOPOROUS MEMBRANE MATERIALS FOR CO2 SEPARATION

    SciTech Connect

    Wei-Heng Shih; Qiang Zhao; Nanlin Wang

    2002-05-01

    Mesoporous and precipitated alumina were synthesized as the base material for CO{sub 2} adsorbent. The porous alumina is doped with Ba to enhance it CO{sub 2} affinity due to the basicity of Ba. it is shown by gas chromatograph (GC) that the addition of Ba enhances the separation CO{sub 2} from N{sub 2}. It was found that mesoporous alumina has larger specific surface area and better selectivity of CO{sub 2} than precipitated alumina. Ba improves the affinity of mesoporous alumina with CO{sub 2}. Phase may play an important role in selective adsorption of CO{sub 2}. It is speculated that mesoporous alumina is more reactive than precipitated alumina creating the xBaO {center_dot} Al{sub 2}O{sub 3} phase that may be more affinity to CO{sub 2} than N{sub 2}. On the other hand, the barium aluminate phase (Ba{sub 3}Al{sub 2}O{sub 6}) in the mesoporous sample does not help the adsorption of CO{sub 2}.

  5. Multiphase, multicomponent simulations and experiments of reactive flow, relevant for combining geologic CO2 sequestration with geothermal energy capture

    NASA Astrophysics Data System (ADS)

    Saar, Martin O.

    2011-11-01

    Understanding the fluid dynamics of supercritical carbon dioxide (CO2) in brine- filled porous media is important for predictions of CO2 flow and brine displacement during geologic CO2 sequestration and during geothermal energy capture using sequestered CO2 as the subsurface heat extraction fluid. We investigate multiphase fluid flow in porous media employing particle image velocimetry experiments and lattice-Boltzmann fluid flow simulations at the pore scale. In particular, we are interested in the motion of a drop (representing a CO2 bubble) through an orifice in a plate, representing a simplified porous medium. In addition, we study single-phase/multicomponent reactive transport experimentally by injecting water with dissolved CO2 into rocks/sediments typically considered for CO2 sequestration to investigate how resultant fluid-mineral reactions modify permeability fields. Finally, we investigate numerically subsurface CO2 and heat transport at the geologic formation scale.

  6. 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.

  7. 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.

  8. 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

  9. 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. PMID:27453949

  10. Carbonation of mantle peridotites: implications for permanent geological CO2 capture and storage

    NASA Astrophysics Data System (ADS)

    Paukert, A. N.; Matter, J. M.; Kelemen, P. B.; Marsala, P.; Shock, E.

    2012-12-01

    In situ carbonation of mantle peridotites serves as a natural analog to engineered mineral carbonation for geological CO2 capture and storage. For example, mantle peridotite in the Samail Ophiolite, Oman naturally captures and stores about 5x104 tons of atmospheric CO2 per year as carbonate minerals, and has been doing so for the past 50,000 years [Kelemen et al., 2011]. Our reaction path modeling of this system shows that the natural process is limited by subsurface availability of dissolved inorganic carbon, and that the rate of CO2 mineralization could be enhanced by a factor of 16,000 by injecting CO2 into the peridotite aquifer at 2 km depth and a fugacity of 100 bars. Injecting CO2 into mafic or ultramafic rock formations has been presumed difficult, as fractured crystalline rocks typically have low porosity and permeability; however these factors have yet to be comprehensively studied. To determine the actual value of these hydrogeological factors, this winter we carried out a multifaceted study of deep boreholes (up to 350m) in the mantle peridotite and the Moho transition zone of the Samail Ophiolite. A suite of physical and chemical parameters were collected, including slug tests for hydraulic conductivity, geophysical well logs for porosity and hydraulic conductivity, drill chips for extent and composition of secondary mineralization, and water and dissolved gas samples for chemical composition. All of these factors combine to provide a comprehensive look at the chemical and physical processes underlying natural mineral carbonation in mantle peridotites. Understanding the natural process is critical, as mineral carbonation in ultramafic rocks is being explored as a permanent and relatively safe option for geologic carbon sequestration. While injectivity in these ultramafic formations was believed to be low, our slug test and geophysical well log data suggest that the hydraulic conductivity of fractured peridotites can actually be fairly high - up to

  11. 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

    2013-09-01

    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. PMID:23915205

  12. 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

  13. 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

  14. 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

  15. Iron phthalocyanine modified mesoporous titania nanoparticles for photocatalytic activity and CO2 capture applications.

    PubMed

    Ramacharyulu, P V R K; Muhammad, Raeesh; Praveen Kumar, J; Prasad, G K; Mohanty, Paritosh

    2015-10-21

    An iron(II)phthalocyanine (Fepc) modified mesoporous titania (Fepc-TiO2) nanocatalyst with a specific surface area of 215 m(2) g(-1) has been synthesized by a hydrothermal method. Fepc-TiO2 degrades one of the highly toxic chemical warfare agents, sulfur mustard (SM), photocatalytically under sunlight with an exposure time of as low as 70 min. Furthermore, the mesoporous Fepc-TiO2 also captured 2.1 mmol g(-1) of CO2 at 273 K and 1 atm. PMID:26393761

  16. 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.

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

    DOE PAGESBeta

    Middleton, Richard S.; Levine, Jonathan S.; Bielicki, Jeffrey M.; Viswanathan, Hari S.; Carey, J. William; Stauffer, Philip H.

    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

  18. 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.

  19. BioCO2 - a multidisciplinary, biological approach using solar energy to capture CO2 while producing H2 and high value products.

    PubMed

    Skjånes, Kari; Lindblad, Peter; Muller, Jiri

    2007-10-01

    Many areas of algae technology have developed over the last decades, and there is an established market for products derived from algae, dominated by health food and aquaculture. In addition, the interest for active biomolecules from algae is increasing rapidly. The need for CO(2) management, in particular capture and storage is currently an important technological, economical and global political issue and will continue to be so until alternative energy sources and energy carriers diminish the need for fossil fuels. This review summarizes in an integrated manner different technologies for use of algae, demonstrating the possibility of combining different areas of algae technology to capture CO(2) and using the obtained algal biomass for various industrial applications thus bringing added value to the capturing and storage processes. Furthermore, we emphasize the use of algae in a novel biological process which produces H(2) directly from solar energy in contrast to the conventional CO(2) neutral biological methods. This biological process is a part of the proposed integrated CO(2) management scheme. PMID:17662653

  20. Tandem Mass Spectrometry Measurement of the Collision Products of Carbamate Anions Derived from CO2 Capture Sorbents: Paving the Way for Accurate Quantitation

    NASA Astrophysics Data System (ADS)

    Jackson, Phil; Fisher, Keith J.; Attalla, Moetaz Ibrahim

    2011-08-01

    The reaction between CO2 and aqueous amines to produce a charged carbamate product plays a crucial role in post-combustion capture chemistry when primary and secondary amines are used. In this paper, we report the low energy negative-ion CID results for several anionic carbamates derived from primary and secondary amines commonly used as post-combustion capture solvents. The study was performed using the modern equivalent of a triple quadrupole instrument equipped with a T-wave collision cell. Deuterium labeling of 2-aminoethanol (1,1,2,2,-d4-2-aminoethanol) and computations at the M06-2X/6-311++G(d,p) level were used to confirm the identity of the fragmentation products for 2-hydroxyethylcarbamate (derived from 2-aminoethanol), in particular the ions CN-, NCO- and facile neutral losses of CO2 and water; there is precedent for the latter in condensed phase isocyanate chemistry. The fragmentations of 2-hydroxyethylcarbamate were generalized for carbamate anions derived from other capture amines, including ethylenediamine, diethanolamine, and piperazine. We also report unequivocal evidence for the existence of carbamate anions derived from sterically hindered amines ( Tris(2-hydroxymethyl)aminomethane and 2-methyl-2-aminopropanol). For the suite of carbamates investigated, diagnostic losses include the decarboxylation product (-CO2, 44 mass units), loss of 46 mass units and the fragments NCO- ( m/z 42) and CN- ( m/z 26). We also report low energy CID results for the dicarbamate dianion (-O2CNHC2H4NHCO{2/-}) commonly encountered in CO2 capture solution utilizing ethylenediamine. Finally, we demonstrate a promising ion chromatography-MS based procedure for the separation and quantitation of aqueous anionic carbamates, which is based on the reported CID findings. The availability of accurate quantitation methods for ionic CO2 capture products could lead to dynamic operational tuning of CO2 capture-plants and, thus, cost-savings via real-time manipulation of solvent

  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. 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).

  4. 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%. PMID:26208135

  5. 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.

  6. Atomistic modeling of CO 2 capture in primary and tertiary amines - Heat of absorption and density changes

    NASA Astrophysics Data System (ADS)

    Maiti, A.; Bourcier, W. L.; Aines, R. D.

    2011-06-01

    With the aim of exploring new amine-based chemistry for CO 2 capture at large industrial scales we performed atomistic modeling of CO 2 chemisorption in aqueous solutions of primary and tertiary amines. DFT-based quantum chemical solvation calculations are shown to yield a number of important results, including the relative stability of ion species (carbamate vs. bicarbonate), heat of absorption, and density and volume changes as a function of CO 2 loading. Good agreement of simulation results with available experimental data provides confidence in the accuracy of such computational methods in predicting properties of new solvent systems and capture designs.

  7. SO2 retention by reactivated CaO-based sorbent from multiple CO2 capture cycles.

    PubMed

    Manovic, Vasilije; Anthony, Edward J

    2007-06-15

    This paper examines the reactivation of spent sorbent, produced from multiple CO2 capture cycles, for use in SO2 capture. CaO-based sorbent samples were obtained from Kelly Rock limestone using three particle size ranges, each containing different impurities levels. Using a thermogravimetric analyzer (TGA), the sulfation behavior of partially sulfated and unsulfated samples obtained after multiple calcination-carbonation cycles in a tube furnace (TF), following steam reactivation in a pressurized reactor, is examined. In addition, samples calcined/sintered under different conditions after hydration are also examined. The results show that suitably treated spent sorbent has better sulfation characteristics than that of the original sorbent. Thus for example, after 2 h sulfation, > 80% of the CaO was sulfated. In addition, the sorbent showed significant activity even after 4 h when > 95% CaO was sulfated. The results were confirmed by X-ray diffraction (XRD) analysis, which showed that, by the end of the sulfation process, samples contained CaSO4 with only traces of unreacted CaO. The superior behavior of spent reactivated sorbent appears to be due to swelling of the sorbent particles during steam hydration. This enables the development of a more suitable pore surface area and pore volume distribution for sulfation, and this has been confirmed by N2 adsorption-desorption isotherms and the Barrett-Joyner-Halenda (BJH) method. The surface area morphology of sorbent after reactivation was examined by scanning electron microscopy (SEM). Ca(OH)2 crystals were seen, which displayed their regular shape, and their elemental composition was confirmed by energy-dispersive X-ray (EDX) analysis. The improved characteristics of spent reactivated sorbent in comparison to the original and to the sorbent calcined under different conditions and hydrated indicate the beneficial effect of CO2 cycles on sorbent reactivation and subsequent sulfation. These results allow us to propose a

  8. 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.

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

    PubMed

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

    2015-07-01

    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. PMID:26023722

  10. Rapid and Accurate Machine Learning Recognition of High Performing Metal Organic Frameworks for CO2 Capture.

    PubMed

    Fernandez, Michael; Boyd, Peter G; Daff, Thomas D; Aghaji, Mohammad Zein; Woo, Tom K

    2014-09-01

    In this work, we have developed quantitative structure-property relationship (QSPR) models using advanced machine learning algorithms that can rapidly and accurately recognize high-performing metal organic framework (MOF) materials for CO2 capture. More specifically, QSPR classifiers have been developed that can, in a fraction of a section, identify candidate MOFs with enhanced CO2 adsorption capacity (>1 mmol/g at 0.15 bar and >4 mmol/g at 1 bar). The models were tested on a large set of 292 050 MOFs that were not part of the training set. The QSPR classifier could recover 945 of the top 1000 MOFs in the test set while flagging only 10% of the whole library for compute intensive screening. Thus, using the machine learning classifiers as part of a high-throughput screening protocol would result in an order of magnitude reduction in compute time and allow intractably large structure libraries and search spaces to be screened. PMID:26278259

  11. Examination of the effect of system pressure ratio and heat recuperation on the efficiency of a coal based gas turbine fuel cell hybrid power generation system with CO2 capture

    SciTech Connect

    VanOsdol, J.G.; Gemmen, R.S.; Liese, E.A

    2008-06-01

    This paper examines two coal-based hybrid configurations that employ separated anode and cathode streams for the capture and compression of CO2. One configuration uses a standard Brayton cycle, and the other adds heat recuperation ahead of the fuel cell. Results show that peak efficiencies near 55% are possible, regardless of cycle configuration, including the cost in terms of energy production of CO2 capture and compression. The power that is required to capture and compress the CO2 is shown to be approximately 15% of the total plant power.

  12. Luminescent Rhenium(I) Pyridyldiaminocarbene Complexes: Photophysics, Anion-Binding, and CO2-Capturing Properties.

    PubMed

    Ng, Chi-On; Cheng, Shun-Cheung; Chu, Wing-Kin; Tang, Kin-Man; Yiu, Shek-Man; Ko, Chi-Chiu

    2016-08-15

    A series of luminescent isocyanorhenium(I) complexes with chelating acyclic diaminocarbene ligands (N^C) has been synthesized and characterized. Two of these carbene complexes have also been structurally characterized by X-ray crystallography. These complexes show blue-to-red phosphorescence, with the emission maxima not only considerably varied with a change in the number of ancillary isocyanide ligands but also extremely sensitive to the electronic and steric nature of the substituents on the acyclic diaminocarbene ligand. A detailed study with the support of density functional theory calculations revealed that the lowest-energy absorption and phosphorescence of these complexes in a degassed CH2Cl2 solution are derived from the predominantly metal-to-ligand charge-transfer [dπ(Re) → π*(N^C)] excited state. The unprecedented anion-binding and CO2-capturing properties of the acyclic diaminocarbene have also been described. PMID:27458842

  13. 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

  14. Ex Situ CO2 capture by carbonation of steelmaking slag coupled with metalworking wastewater in a rotating packed bed.

    PubMed

    Pan, Shu-Yuan; Chiang, Pen-Chi; Chen, Yi-Hung; Tan, Chung-Sung; Chang, E-E

    2013-04-01

    Both basic oxygen furnace (BOF) slag and cold-rolling wastewater (CRW) exhibiting highly alkaline characteristics require stabilization and neutralization prior to utilization and/or final disposal. Using CO2 from flue gases as the stabilizing and neutralizing agents could also diminish CO2 emissions. In this investigation, ex situ hot stove gas containing 30 vol% CO2 in the steelmaking process was captured by accelerated carbonation of BOF slag coupled with CRW in a rotating packed bed (RPB). The developed RPB process exhibits superior results, with significant CO2 removal efficiency (η) of 96-99% in flue gas achieved within a short reaction time of 1 min at 25 °C and 1 atm. Calcite (CaCO3) was identified as the main product according to XRD and SEM-XEDS observations. In addition, the elimination of lime and Ca(OH)2 in the BOF slag during carbonation is beneficial to its further use as construction material. Consequently, the developed RPB process could capture the CO2 from the flue gas, neutralize the CRW, and demonstrate the utilization potential for BOF slag. It was also concluded that carbonation of BOF slag coupled with CRW in an RPB is a viable method for CO2 capture due to its higher mass transfer rate and CO2 removal efficiency in a short reaction time. PMID:23458276

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

    PubMed

    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

  16. 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.

  17. 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

  18. A Superacid-Catalyzed Synthesis of Porous Membranes Based on Triazine Frameworks for CO2 Separation

    SciTech Connect

    Zhu, X; Tian, CC; Mahurin, SM; Chai, SH; Wang, CM; Brown, S; Veith, GM; Luo, HM; Liu, HL; Dai, S

    2012-06-27

    A general strategy for the synthesis of porous, fluorescent, triazine-framework-based membranes with intrinsic porosity through an aromatic nitrile trimerization reaction is presented. The essence of this strategy lies in the use of a superacid to catalyze the cross-linking reaction efficiently at a low temperature, allowing porous polymer membrane architectures to be facilely derived. With fiinctionalized triazine units, the membrane exhibits an increased selectivity for membrane separation of CO2 over N-2. The good ideal CO2/N-2 selectivity of 29 +/- 2 was achieved with a CO2 permeability of 518 +/- 25 barrer. Through this general synthesis protocol, a new class of porous polymer membranes with tunable functionalities and porosities can be derived, significantly expanding the currently limited library of polymers with intrinsic microporosity for synthesizing functional membranes in separation, catalysis, and energy storage/conversion.

  19. 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

  20. The mechanism of vapor phase hydration of calcium oxide: implications for CO2 capture.

    PubMed

    Kudłacz, Krzysztof; Rodriguez-Navarro, Carlos

    2014-10-21

    Lime-based sorbents are used for fuel- and flue-gas capture, thereby representing an economic and effective way to reduce CO2 emissions. Their use involves cyclic carbonation/calcination which results in a significant conversion reduction with increasing number of cycles. To reactivate spent CaO, vapor phase hydration is typically performed. However, little is known about the ultimate mechanism of such a hydration process. Here, we show that the vapor phase hydration of CaO formed after calcination of calcite (CaCO3) single crystals is a pseudomorphic, topotactic process, which progresses via an intermediate disordered phase prior to the final formation of oriented Ca(OH)2 nanocrystals. The strong structural control during this solid-state phase transition implies that the microstructural features of the CaO parent phase predetermine the final structural and physicochemical (reactivity and attrition) features of the product hydroxide. The higher molar volume of the product can create an impervious shell around unreacted CaO, thereby limiting the efficiency of the reactivation process. However, in the case of compact, sintered CaO structures, volume expansion cannot be accommodated in the reduced pore volume, and stress generation leads to pervasive cracking. This favors complete hydration but also detrimental attrition. Implications of these results in carbon capture and storage (CCS) are discussed. PMID:25233236

  1. 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.

  2. CO2/H2 separation using a highly permeable polyurethane membrane: Molecular dynamics simulation

    NASA Astrophysics Data System (ADS)

    Azizi, Morteza; Mousavi, Seyyed Abbas

    2015-11-01

    In this study, Molecular Dynamics (MD) and Grand Canonical Monte Carlo (GCMC) simulations were conducted to investigate the diffusivity, solubility, and permeability of CO2, CO, H2, and H2O in a polyurethane membrane at three different temperatures. The characterization of the simulated structures was carried out using XRD, FFV, Tg and density calculation, and cavity size distribution. The obtained results were within the expectations reported data in the literature based on the experimental approach, indicating the authenticity of approached in this work. The results showed that the highest diffusivity and permeability coefficients were observed for H2; while the highest values of solubility coefficient were found for H2O and CO2 gases. The increase of operating temperature from 298 K to 318 K has a positive effect on the permeation of all gases and a corresponding negative effect on the selectivity of the gas pair CO2/H2. Also, the results vividly showed that CO2 and H2O gases have a profound affinity with hard phase of polyurethane, while H2 and CO were conversely adsorbed by soft one. Moreover, the enhancement of permeability and permselectivity of CO2/H2 pair confirmed using Robeson Upper-Bond graph showed its good capacity for CO2/H2 separation application.

  3. 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.

  4. 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. PMID:23654217

  5. 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.

  6. Understanding the mechanism of CO2 capture by 1,3 di-substituted imidazolium acetate based ionic liquids.

    PubMed

    Mao, James X; Steckel, Janice A; Yan, Fangyong; Dhumal, Nilesh; Kim, Hyung; Damodaran, Krishnan

    2016-01-21

    Efficient CO2 capture by ionic liquids needs a thorough understanding of underlying mechanisms of the CO2 interaction with ionic liquids, especially when it involves chemisorption. In this work we have systematically investigated the mechanism of CO2 capture by 1,3 di-substituted imidazolium acetate ionic liquids using density functional theory. Solvent effects are analyzed using QM/MM and QM/QM approaches with the help of molecular dynamics simulations and ONIOM methods. The investigation of different stepwise mechanisms shows that CO2 could be involved in the first step of the reaction mechanism, also a new two-step mechanism is proposed. The final stabilization step is analyzed and pointed out to be responsible for important experimentally-observed features of the reaction. PMID:26687108

  7. 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.

  8. Imidazolium Ionic Liquids, Imidazolylidene Heterocyclic Carbenes, and Zeolitic Imidazolate Frameworks for CO2 Capture and Photochemical Reduction.

    PubMed

    Wang, Sibo; Wang, Xinchen

    2016-02-01

    Imidazolium ionic liquids (ILs), imidazolylidene N-heterocyclic carbenes (NHCs), and zeolitic imidazolate frameworks (ZIFs) are imidazolate motifs which have been extensively investigated for CO2 adsorption and conversion applications. Summarized in this minireview is the recent progress in the capture, activation, and photochemical reduction of CO2 with these three imidazolate building blocks, from homogeneous molecular entities (ILs and NHCs) to heterogeneous crystalline scaffolds (ZIFs). The developments and existing shortcomings of the imidazolate motifs for their use in CO2 utilizations is assessed, with more of focus on CO2 photoredox catalysis. The opportunities and challenges of imidazolate scaffolds for future advancement of CO2 photochemical conversion for artificial photosynthesis are discussed. PMID:26683833

  9. 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.

  10. Carbon dioxide capture-related gas adsorption and separation in metal-organic frameworks

    SciTech Connect

    Li, JR; Ma, YG; McCarthy, MC; Sculley, J; Yu, JM; Jeong, HK; Balbuena, PB; Zhou, HC

    2011-08-01

    Reducing anthropogenic CO2 emission and lowering the concentration of greenhouse gases in the atmosphere has quickly become one of the most urgent environmental issues of our age. Carbon capture and storage (CCS) is one option for reducing these harmful CO2 emissions. While a variety of technologies and methods have been developed, the separation of CO2 from gas streams is still a critical issue. Apart from establishing new techniques, the exploration of capture materials with high separation performance and low capital cost are of paramount importance. Metal-organic frameworks (MOFs), a new class of crystalline porous materials constructed by metal-containing nodes bonded to organic bridging ligands hold great potential as adsorbents or membrane materials in gas separation. In this paper, we review the research progress (from experimental results to molecular simulations) in MOFs for CO2 adsorption, storage, and separations (adsorptive separation and membrane-based separation) that are directly related to CO2 capture. (C) 2011 Elsevier B.V. All rights reserved.

  11. Mesoporous fluorocarbon-modified silica aerogel membranes enabling long-term continuous CO2 capture with large absorption flux enhancements.

    PubMed

    Lin, Yi-Feng; Chen, Chien-Hua; Tung, Kuo-Lun; Wei, Te-Yu; Lu, Shih-Yuan; Chang, Kai-Shiun

    2013-03-01

    The use of a membrane contactor combined with a hydrophobic porous membrane and an amine absorbent has attracted considerable attention for the capture of CO2 because of its extensive use, low operational costs, and low energy consumption. The hydrophobic porous membrane interface prevents the passage of the amine absorbent but allows the penetration of CO2 molecules that are captured by the amine absorbent. Herein, highly porous SiO2 aerogels modified with hydrophobic fluorocarbon functional groups (CF3 ) were successfully coated onto a macroporous Al2 O3 membrane; their performance in a membrane contactor for CO2 absorption is discussed. The SiO2 aerogel membrane modified with CF3 functional groups exhibits the highest CO2 absorption flux and can be continuously operated for CO2 absorption for extended periods of time. This study suggests that a SiO2 aerogel membrane modified with CF3 functional groups could potentially be used in a membrane contactor for CO2 absorption. Also, the resulting hydrophobic SiO2 aerogel membrane contactor is a promising technology for large-scale CO2 absorption during the post-combustion process in power plants. PMID:23417984

  12. 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.

  13. Bimetallic nickel complexes for selective CO2 carbon capture and sequestration.

    PubMed

    Möller, F; Merz, K; Herrmann, C; Apfel, U-P

    2016-01-21

    Herein we report a dinickel azacryptand complex that enables fast, selective, and tight CO2 binding from air. Exploiting the affinity of the cavitand towards azides, CO2 release was observed. Despite the stability of the azido complex, UV irradiation under atmospheric conditions proved to be a suitable pathway for N3(-) replacement by CO2. PMID:26666316

  14. 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

  15. New directions: Potential climate and productivity benefits from CO2 capture in commercial buildings

    NASA Astrophysics Data System (ADS)

    Gall, Elliott T.; Nazaroff, William W.

    2015-02-01

    Primarily because of humanity's heavy reliance on fossil fuels, ambient CO2 levels have risen from 280 ppm in preindustrial times to 400 ppm today, and levels continue to rise by a few ppm per year (Tans and Keeling, 2014). Progress toward stabilizing atmospheric CO2 levels can be achieved not only through reducing emissions but also through the engineering of new or enhanced sinks of atmospheric CO2. Research and private sector initiatives on removing CO2 from ambient air (Boot-Handford et al., 2014) lead us to consider this challenge in the context of a well-known indoor air quality concern: elevated CO2 concentrations in occupied buildings.

  16. 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

  17. 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.

  18. 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. PMID:24730662

  19. 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

  20. Microscale phase separator for selective extraction of CO2 from methanol solution flow

    NASA Astrophysics Data System (ADS)

    Fazeli, Abdolreza; Moghaddam, Saeed

    2014-12-01

    This study is aimed at understanding the limits in reducing the size of a membrane-based CO2 separator and its pressure head needs and energy consumption, while maximizing its selectivity. The separator consists of a flow channel capped by a hydrophobic nanoporous membrane through which CO2 exits the anode flow stream of a direct methanol fuel cell (DMFC). A systematic study is conducted to determine the effect of differential pressure across the membrane, flow velocity, and flow channel dimensions on the separation process. The extraction flux was found to change linearly with pressure difference across the membrane. The effect of flow velocity on the extraction flux was negligible up to a critical velocity beyond which the separation process ceased. The separation selectivity enhanced by increasing the differential pressure across the membrane but did not change with varying the flow velocity and channel depth. Using the findings of the first part of the study, an optimal micro-separator (with a footprint of approximately 10 × 1 mm2) was designed/fabricated for a 20 W DMFC and its performance was experimentally analyzed. An unprecedented separation selectivity of close to 200 was achieved at a differential pressure of about 10 kPa and negligible energy consumption.

  1. 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.

  2. CO2 capture on micro/mesoporous composites of (zeolite A)/(MCM-41) with Ca2+ located: Computer simulation and experimental studies

    NASA Astrophysics Data System (ADS)

    Zhou, Jianhai; Zhao, Huiling; Li, Jinxia; Zhu, Yujun; Hu, Jun; Liu, Honglai; Hu, Ying

    2013-10-01

    Composing of both zeolite and mesoporous structures, micro/mesoporous composites exhibit promising CO2 capture capabilities. In this work, a full-atomic mimetic 5A-MCM-41 structure with bimodal pores has been constructed, in which the microporous structure of 5A zeolite is constructed and optimized based on zeolite A with Ca and Na cations introduced; whereas the mesoporous MCM-41 structure is produced by caving the cylindrical pores in the obtained 5A zeolite matrix. CO2 adsorption on 5A-MCM-41 has been simulated by the grand canonical Monte Carlo (GCMC). The simulation results demonstrated that CO2 is preferentially adsorbed in micropores, and the CO2 adsorption capacity and its isosteric heat on 5A-MCM-41 are much larger than those of N2. The CO2 selectivity of 5A-MCM-41 results from the electrostatic interaction of the quadrupole CO2 molecule with Ca2+ cations of the zeolite. Furthermore, the hierarchical micro/mesoporous composites are synthesized to verify the simulated predictions. By the hydrothermal reaction using 5A zeolite "seeds" as the silicon source and hexadecyl trimethylammonium bromide (CTAB) as the mesoporous template, 5A-MCM-41 composites are obtained, the characteristic results show that typical 5A microporous structure is remained and disordered mesoporous networks are produced in the composites. Moreover, the CO2 adsorption capacity of the 5A-MCM-41 composites can reach as high as 4.08 mmol/g at 100 kPa and 298 K. These observations have been strongly supported that micro/mesoporous composites with metal ions located would be promising adsorbents for CO2 separation.

  3. 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. PMID:25389800

  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. Effect of nano-silica spheres template on CO2 capture of exchange resin-based nanoporous carbons.

    PubMed

    Meng, Long-Yue; Park, Soo-Jin

    2013-01-01

    In this work, a nanoporous carbon-based adsorbent with a higher specific surface area was directly prepared from polystyrene-based cation exchange resin (PCER) by carbonization of a mixture of nano-silica spheres. The silica/PCER composites were carbonized at 1173 K with different silica/PCER ratios. The effects of nano-silica spheres content on the pore structures of nanoporous carbons were investigated by N2 full isotherms. The CO2 capture capacity was measured by CO2 isothermal adsorption at 298 K and 1 bar. From the results, it was found that the nano-silica spheres/PCER ratio had a major influence on the CO2 capture capacity and the textural properties of the prepared nanoporous carbons. The specific surface area and total pore volume, as well as the pore size of the nanoporous carbons increased with increasing silica/PCER ratio. PMID:23646745

  6. Thermodynamic analysis of the double Brayton cycle with the use of oxy combustion and capture of CO2

    NASA Astrophysics Data System (ADS)

    Ziółkowski, Paweł; Zakrzewski, Witold; Kaczmarczyk, Oktawia; Badur, Janusz

    2013-06-01

    In this paper, thermodynamic analysis of a proposed innovative double Brayton cycle with the use of oxy combustion and capture of CO2, is presented. For that purpose, the computation flow mechanics (CFM) approach has been developed. The double Brayton cycle (DBC) consists of primary Brayton and secondary inverse Brayton cycle. Inversion means that the role of the compressor and the gas turbine is changed and firstly we have expansion before compression. Additionally, the workingfluid in the DBC with the use of oxy combustion and CO2 capture contains a great amount of H2O and CO2, and the condensation process of steam (H2O) overlaps in negative pressure conditions. The analysis has been done for variants values of the compression ratio, which determines the lowest pressure in the double Brayton cycle.

  7. 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...

  8. 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. PMID:20948952

  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. 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.

  11. 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

  12. 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.

  13. 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

  14. 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.

  15. Theoretical studies on CO2 capture behavior of quaternary ammonium-based polymeric ionic liquids.

    PubMed

    Wang, Tao; Ge, Kun; Chen, Kexian; Hou, Chenglong; Fang, Mengxiang

    2016-05-14

    Quaternary ammonium-based polymeric ionic liquids (PILs) are novel CO2 sorbents as they have high capacity, high stability and high binding energy. Moreover, the binding energy of ionic pairs to CO2 is tunable by changing the hydration state so that the sorbent can be regenerated through humidity adjustment. In this study, theoretical calculations were conducted to reveal the mechanism of the humidity swing CO2 adsorption, based on model compounds of quaternary ammonium cation and carbonate anions. The electrostatic potential map demonstrates the anion, rather than the cation, is chemically preferential for CO2 adsorption. Further, the proton transfer process from water to carbonate at the sorbent interface is successfully depicted with an intermediate which has a higher energy state. By determining the CO2 adsorption energy and activation energy at different hydration states, it is discovered that water could promote CO2 adsorption by reducing the energy barrier of proton transfer. The adsorption/desorption equilibrium would shift to desorption by adding water, which constitutes the theoretical basis for humidity swing. By analyzing the hydrogen bonding and structure of the water molecules, it is interesting to find that the CO2 adsorption weakens the hydrophilicity of the sorbent and results in release of water. The requirement of latent heat for the phase change of water could significantly reduce the heat of adsorption. The special "self-cooling" effect during gas adsorption can lower the temperature of the sorbent and benefit the adsorption isotherms. PMID:27115032

  16. 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. PMID:27046045

  17. 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

  18. 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. PMID:26217886

  19. Exploration of nanoporous graphene membranes for the separation of N2 from CO2: a multi-scale computational study.

    PubMed

    Wang, Yong; Yang, Qingyuan; Li, Jinping; Yang, Jiangfeng; Zhong, Chongli

    2016-03-28

    Density functional theory (DFT) calculations and molecular dynamic (MD) simulations were performed to investigate the capability of graphene membranes with H-passivated nanopores for the separation of N2/CO2 gas mixtures. We found that the graphene membrane, H-pore-13, with its appropriate pore size of 4.06 Å, can efficiently separate N2 from CO2. Different from the previously reported preferential permeation of CO2 over N2 resulting from size sieving, H-pore-13 can exhibit high N2 selectivity over CO2 with a N2 permeance of 10(5) GPU (gas permeation unit), and no CO2 was found to pass through the pore. It was further revealed that electrostatic sieving plays a cruical role in hindering the passage of CO2 molecules through H-pore-13. PMID:26701145

  20. 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.

  1. 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

  2. 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

  3. 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. PMID:22717067

  4. Oxygen-containing functional group-facilitated CO2 capture by carbide-derived carbons

    PubMed Central

    2014-01-01

    A series of carbide-derived carbons (CDCs) with different surface oxygen contents were prepared from TiC powder by chlorination and followed by HNO3 oxidation. The CDCs were characterized systematically by a variety of means such as Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, ultimate analysis, energy dispersive spectroscopy, N2 adsorption, and transmission electron microscopy. CO2 adsorption measurements showed that the oxidation process led to an increase in CO2 adsorption capacity of the porous carbons. Structural characterizations indicated that the adsorbability of the CDCs is not directly associated with its microporosity and specific surface area. As evidenced by elemental analysis, X-ray photoelectron spectroscopy, and energy dispersive spectroscopy, the adsorbability of the CDCs has a linear correlation with their surface oxygen content. The adsorption mechanism was studied using quantum chemical calculation. It is found that the introduction of O atoms into the carbon surface facilitates the hydrogen bonding interactions between the carbon surface and CO2 molecules. This new finding demonstrated that not only the basic N-containing groups but also the acidic O-containing groups can enhance the CO2 adsorbability of porous carbon, thus providing a new approach to design porous materials with superior CO2 adsorption capacity. PMID:24872796

  5. 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. PMID:27076214

  6. A permanently porous single molecule H-bonded organic framework for selective CO2 capture.

    PubMed

    Nandi, Shyamapada; Chakraborty, Debanjan; Vaidhyanathan, Ramanathan

    2016-05-26

    Permanent porosity has been realized in a hydrogen bonded framework formed by a single tripodal tricarboxylic acid molecule. The presence of three phenyl rings linked to a flexible sp(3) nitrogen centre renders a near-propeller shape to the molecule generating an unusual 'non-planar' 3-D framework formed by highly directional planar -COOHHOOC- hydrogen bonds, propagating in all three directions. The material shows exceptional hydrolytic, acidic and thermal stability and has a surface area of 1025 m(2) g(-1). Importantly, it shows preferential adsorption of CO2 over N2 with very high selectivities (350 : 1@1 bar, 303 K). DFT modeling shows the presence of stable T-shaped CO2CO2 dimers within the channels suggesting favorable co-operativity between them. PMID:27174692

  7. 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).

  8. CaO-based pellets supported by calcium aluminate cements for high-temperature CO2 capture.

    PubMed

    Manovic, Vasilije; Anthony, Edward J

    2009-09-15

    The development of highly efficient CaO-based pellet sorbents, using inexpensive raw materials (limestones) or the spent sorbent from CO2 capture cycles, and commercially available calcium aluminate cements (CA-14, CA-25, Secar 51, and Secar 80), is described here. The pellets were prepared using untreated powdered limestones or their corresponding hydrated limes and were tested for their CO2 capture carrying capacities for 30 carbonation/calcination cycles in a thermogravimetric analyzer (TGA). Their morphology was also investigated by scanning electron microscopy (SEM) and their compositions before and after carbonation/calcination cycleswere determined by X-ray diffraction (XRD). Pellets prepared in this manner showed superior behavior during CO2 capture cycles compared to natural sorbents, with the highest conversions being > 50% after 30 cycles. This improved performance was attributed to the resulting substructure of the sorbent particles, i.e., a porous structure with nanoparticles incorporated. During carbonation/calcination cycles mayenite (Ca12Al14O33) was formed, which is believed to be responsible for the favorable performance of synthetic CaO-based sorbents doped with alumina compounds. An added advantage of the pellets produced here is their superior strength, offering the possibility of using them in fluidized bed combustion (FBC) systems with minimal sorbent loss due to attrition. PMID:19806751

  9. 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.

  10. Modulated UiO-66-Based Mixed-Matrix Membranes for CO2 Separation.

    PubMed

    Anjum, M Waqas; Vermoortele, Frederik; Khan, Asim Laeeq; Bueken, Bart; De Vos, Dirk E; Vankelecom, Ivo F J

    2015-11-18

    Mixed-matrix membranes (MMMs) composed of polyimide (PI) and metal-organic frameworks (MOFs) were synthesized using Matrimid as the polymer and zirconium terephthalate UiO-66 as the filler. The modulation approach, combined with the use of amine-functionalized linkers, was used for synthesis of the MOF fillers in order to enhance the intrinsic separation performance of the MOF and improve the particle-PI compatibility. The presence of amine groups on the MOF outer surface introduced either through the linker, through the modulator, or through both led to covalent linking between the fillers and Matrimid, which resulted in very stable membranes. In addition, the presence of amine groups inside the pores of the MOFs and the presence of linker vacancies inside the MOFs positively influenced CO2 transport. MMMs with 30 wt % loading showed excellent separation performance for CO2/CH4 mixtures. A significant increase in the mixed-gas selectivity (47.7) and permeability (19.4 barrer) compared to the unfilled Matrimid membrane (i.e., 50% more selective and 540% more permeable) was thus achieved for the MMM containing the MOF prepared from 2-aminoterephthalic acid and 4-aminobenzoic acid, respectively used as the linker and as the modulator. PMID:26458211

  11. 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.

  12. 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. PMID:24702296

  13. Preparation of a Facilitated Transport Membrane Composed of Carboxymethyl Chitosan and Polyethylenimine for CO2/N2 Separation

    PubMed Central

    Shen, Jiang-Nan; Yu, Chang-Chao; Zeng, Gan-Ning; van der Bruggen, Bart

    2013-01-01

    The miscibility of carboxymethyl chitosan/polyethylenimine (CMCS/PEI) blends was analyzed by FT-IR, TGA and SEM. Defect-free CMCS/PEI blend membranes were prepared with polysulfone (PSf) ultrafiltration membranes as support layer for the separation of CO2/N2 mixtures. The results demonstrate that the CMCS/PEI blend is miscible, due to the hydrogen bonding interaction between the two targeted polymers. For the blended membrane without water, the permeability of CO2 gas is 3.6 × 10−7 cm3 cm−2 s−1 cmHg−1 and the corresponding separation factor for CO2 and N2 gas is about 33 at the pressure of 15.2 cmHg. Meanwhile, the blended membrane with water has the better permselectivity. The blended membrane containing water with PEI content of 30 wt% has the permeance of 6.3 × 10−4 cm3 cm−2 s−1 cmHg−1 for CO2 gas and a separation factor of 325 for CO2/N2 mixtures at the same feed pressure. This indicates that the CO2 separation performance of the CMCS/PEI blend membrane is higher than that of other facilitated transport membranes reported for CO2/N2 mixture separation. PMID:23434661

  14. 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. PMID:26012371

  15. 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

  16. 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

  17. 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

  18. Cyclic stability testing of aminated-silica solid sorbent for post-combustion CO2 capture.

    PubMed

    Fisher, James C; Gray, McMahan

    2015-02-01

    The National Energy Technology Laboratory (NETL) is examining the use of solid sorbents for CO2 removal from coal-fired power plant flue gas streams. An aminated sorbent (previously reported by the NETL) is tested for stability by cyclic exposure to simulated flue gas and subsequent regeneration for 100 cycles. Each cycle was quantified using a traced gas in the simulated flue gas monitored by a mass spectrometer, which allowed for rapid determination of the capacity. PMID:25510438

  19. 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. PMID:26270956

  20. 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. PMID:22342037

  1. 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. PMID:23895233

  2. 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.

  3. 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.

  4. 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.

  5. 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.

  6. 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.

  7. Reticular Synthesis of a Series of HKUST-like MOFs with Carbon Dioxide Capture and Separation.

    PubMed

    He, Hongming; Sun, Fuxing; Ma, Shengqian; Zhu, Guangshan

    2016-09-01

    We reported a series of HKUST-like MOFs based on multiple copper-containing secondary building units (SBUs). Compound 1 is constructed by two SBUs: Cu2(CO2)4 paddle-wheel SBUs and Cu2I2 dimer SBUs. Compound 2 has Cu2(CO2)4 paddle-wheel SBUs and Cu4I4 SBUs. Furthermore, compound 3 possesses Cu2(CO2)4 paddle-wheel SBUs, Cu2I2 dimer SBUs, and Cu(CO2)4 SBUs. These compounds are promising materials for CO2 capture and separation, because they all display commendable adsorption of CO2 and high selectivity for CO2 over CH4 and N2. It is worthy to note that compound 1 exhibits the highest Brunauer-Emmett-Teller surface area (ca. 901 m(2) g(-1)) among the MOF materials based on CuxIy SBUs. In addition, compound 3 is the first case that three copper SBUs coexist in MOFs. PMID:27556744

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

    PubMed

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

    2015-06-22

    Chemical looping combustion (CLC) and chemical looping with oxygen uncoupling (CLOU) are emerging thermochemical CO2 capture cycles that allow the capture of CO2 with a small energy penalty. Here, the development of suitable oxygen carrier materials is a key aspect to transfer these promising concepts to practical installations. CuO is an attractive material for CLC and CLOU because of its high oxygen-storage capacity (20 wt %), fast reaction kinetics, and high equilibrium partial pressure of oxygen at typical operating temperatures (850-1000 °C). However, despite its promising characteristics, its low Tammann temperature requires the development of new strategies to phase-stabilize CuO-based oxygen carriers. In this work, we report a strategy based on stabilization by co-precipitated ceria (CeO2-x ), which allowed us to increase the oxygen capacity, coke resistance, and redox stability of CuO-based oxygen carriers substantially. The performance of the new oxygen carriers was evaluated in detail and compared to the current state-of-the-art materials, that is, Al2 O3 -stabilized CuO with similar CuO loadings. We also demonstrate that the higher intrinsic oxygen uptake, release, and mobility in CeO2-x -stabilized CuO leads to a three times higher carbon deposition resistance compared to that of Al2 O3 -stabilized CuO. Moreover, we report a high cyclic stability without phase intermixing for CeO2-x -supported CuO. This was accompanied by a lower reduction temperature compared to state-of-the-art Al2 O3 -supported CuO. As a result of its high resistance towards carbon deposition and fast oxygen uncoupling kinetics, CeO2-x -stabilized CuO is identified as a very promising material for CLC- and CLOU-based CO2 capture architectures. PMID:25916240

  9. Popcorn-Derived Porous Carbon for Energy Storage and CO2 Capture.

    PubMed

    Liang, Ting; Chen, Chunlin; Li, Xing; Zhang, Jian

    2016-08-16

    Porous carbon materials have drawn tremendous attention due to its applications in energy storage, gas/water purification, catalyst support, and other important fields. However, producing high-performance carbons via a facile and efficient route is still a big challenge. Here we report the synthesis of microporous carbon materials by employing a steam-explosion method with subsequent potassium activation and carbonization of the obtained popcorn. The obtained carbon features a large specific surface area, high porosity, and doped nitrogen atoms. Using as an electrode material in supercapacitor, it displays a high specific capacitance of 245 F g(-1) at 0.5 A g(-1) and a remarkable stability of 97.8% retention after 5000 cycles at 5 A g(-1). The product also exhibits a high CO2 adsorption capacity of 4.60 mmol g(-1) under 1066 mbar and 25 °C. Both areal specific capacitance and specific CO2 uptake are directly proportional to the surface nitrogen content. This approach could thus enlighten the batch production of porous nitrogen-doped carbons for a wide range of energy and environmental applications. PMID:27455183

  10. 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.

  11. Hierarchically Mesoporous o-Hydroxyazobenzene Polymers: Synthesis and Their Applications in CO2 Capture and Conversion.

    PubMed

    Ji, Guipeng; Yang, Zhenzhen; Zhang, Hongye; Zhao, Yanfei; Yu, Bo; Ma, Zhishuang; Liu, Zhimin

    2016-08-01

    The synthesis of hierarchically mesoporous polymers with multiple functionalities is challenging. Herein we reported a template-free strategy for synthesis of phenolic azo-polymers with hierarchical porous structures based on diazo-coupling reaction in aqueous solution under mild conditions. The resultant polymers have surface areas up to 593 m(2)  g(-1) with the mesopore ratio of >80 %, and a good ability to complex with metal ions, such as Cu(2+) , Zn(2+) ,Ni(2+) , achieving a metal loading up to 26.24 wt %. Moreover, the polymers complexed with Zn showed excellent performance for catalyzing the reaction of CO2 with epoxide, affording a TOF of 2570 h(-1) in the presence of tetrabutyl ammonium bromide (7.2 mol %). The polymer complexed with Cu could catalyze the oxidation of alcohol with high efficiency. PMID:27199160

  12. 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.

  13. Furfuralcohol Co-Polymerized Urea Formaldehyde Resin-derived N-Doped Microporous Carbon for CO2 Capture.

    PubMed

    Liu, Zhen; Yang, Yi; Du, Zhenyu; Xing, Wei; Komarneni, Sridhar; Zhang, Zhongdong; Gao, Xionghou; Yan, Zifeng

    2015-12-01

    Carbon-based adsorbent is considered to be one of the most promising adsorbents for CO2 capture form flue gases. In this study, a series of N-doped microporous carbon materials were synthesized from low cost and widely available urea formaldehyde resin co-polymerized with furfuralcohol. These N-doped microporous carbons showed tunable surface area in the range of 416-2273 m(2) g(-1) with narrow pore size distribution within less than 1 nm and a high density of the basic N functional groups (2.93-13.92 %). Compared with the carbon obtained from urea resin, the addition of furfuralcohol apparently changed the surface chemical composition and pore size distribution, especially ultramicropores as can be deduced from the X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FT-IR), and pore size distribution measurements and led to remarkable improvement on CO2 adsorption capacity. At 1 atm, N-doped carbons activated at 600 °C with KOH/UFFC weight ratio of 2 (UFFA-2-600) showed the highest CO2 uptake of 3.76 and 1.57 mmol g(-1) at 25 and 75 °C, respectively. PMID:26293492

  14. 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.

  15. 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

    2015-11-01

    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. PMID:26119355

  16. Co3(HCOO)6 microporous metal-organic framework membrane for separation of CO2/CH4 mixtures.

    PubMed

    Zou, Xiaoqin; Zhang, Feng; Thomas, Sebastien; Zhu, Guangshan; Valtchev, Valentin; Mintova, Svetlana

    2011-10-17

    Continuous metal-organic framework-type Co(3)(HCOO)(6) intergrown films with a one-dimensional zigzag channel system and pore aperture of 5.5 Å are prepared by secondary growth on preseeded macroporous glass-frit disks and silicon wafers. The adsorption behavior of CO(2) or CH(4) single gases on the Co(3)(HCOO)(6) membrane is investigated by in situ IR spectroscopy. It is shown that the isosteric heats of adsorption for CO(2) (17.7 kJ mol(-1)) and CH(4) (14.4 kJ mol(-1)) do not vary with increasing amount of adsorbed gases. The higher value of isosteric heat for CO(2) is an indication of the stronger interaction between the CO(2) and the Co(3)(HCOO)(6) membrane. The Co(3)(HCOO)(6) membrane is studied by binary gas permeation of CO(2) and CH(4) at different temperatures (0, 25, and 60 °C). The membrane has CO(2)/CH(4) selectivity with a separation factor higher than 10, which is due to the unique structure and molecular sieving effect. Upon increasing the temperature from 0 to 60 °C, the preferred permeance of CO(2) over CH(4) is increased from 1.70×10(-6) to 2.09×10(-6) mol m(-2) s(-1) Pa(-1), while the separation factor for CO(2)/CH(4) shows a corresponding decrease from 15.95 to 10.37. The effective pore size of the Co(3)(HCOO)(6) material combined with the pore shape do not allow the two molecules to pass simultaneously, and once the CO(2) molecules are diffused in the micropores, the CH(4) is blocked. The supported Co(3)(HCOO)(6) membrane retains high mechanical stability after a number of thermal cycles. PMID:21922579

  17. Stabilizing a high-temperature electrochemical silver-carbonate CO2 capture membrane by atomic layer deposition of a ZrO2 overcoat.

    PubMed

    Zhang, Peng; Tong, Jingjing; Jee, Youngseok; Huang, Kevin

    2016-07-28

    A high-selectivity and high-flux electrochemical silver-carbonate dual-phase membrane was coated with a nanoscaled ZrO2 layer by atomic layer deposition (ALD) for stable CO2 capture at high-temperature (≥800 °C); the latter has an important implication for direct dry methane reforming with the captured CO2 and O2 for syngas production. PMID:27417536

  18. 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.

  19. 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.

  20. 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.

  1. Accelerating progress toward operational excellence of fossil energy plants with CO2 capture

    SciTech Connect

    Zitney, S.; Liese, E.; Mahapatra, P.; Turton, R. Bhattacharyya, D.

    2012-01-01

    To address challenges in attaining operational excellence for clean energy plants, the National Energy Technology Laboratory has launched a world-class facility for Advanced Virtual Energy Simulation Training And Research (AVESTARTM). The AVESTAR Center brings together state-of-the-art, real-time, high-fidelity dynamic simulators with operator training systems and 3D virtual immersive training systems into an integrated energy plant and control room environment. This paper will highlight the AVESTAR Center simulators, facilities, and comprehensive training, education, and research programs focused on the operation and control of an integrated gasification combined cycle power plant (IGCC) with carbon dioxide capture.

  2. AVESTAR Center for operational excellence of IGCC power plants with CO2 capture

    SciTech Connect

    Provost, G,

    2012-01-01

    This slideshow presentation begins by outlining US energy challenges, particularly with respect to power generation capacity and clean energy plant operations. It goes on to describe the Advanced Virtual Energy Simulation Training And Research (AVESTAR{sup TM}). Its mission and goals are given, followed by an overview of integrated gasification combined cycle (IGCC) with CO{sub 2} capture. The Dynamic Simulator/Operator Training System (OTS) and 3D Virtual Immersive Training System (ITS) are then presented. Facilities, training, education, and R&D are covered, followed by future simulators and directions.

  3. AVESTAR Center for operational excellence of IGCC power plants with CO2 capture

    SciTech Connect

    Provost, G,

    2012-01-01

    This presentation begins with a description of U.S. Energy Challenges, particularly Power Generation Capacity and Clean Energy Plant Operations. It goes on to describe the missions and goals of the Advanced Virtual Energy Simulation Training And Research (AVESTARTM). It moves on to the subject of Integrated Gasification Combined Cycle (IGCC) with CO{sub 2} Capture, particularly a Process/Project Overview, Dynamic Simulator/Operator Training System (OTS), 3D Virtual Immersive Training System (ITS), Facilities, Training, Education, and R&D, and Future Simulators/Directions

  4. Reactive Inorganic Membranes for CO2/N2 separations: Ab-initio Density Functional Theory Calculations

    NASA Astrophysics Data System (ADS)

    Ostwal, M.; Way, J. D.; Lusk, M.

    2009-10-01

    The selectivity (CO2/N2) of mesoporous silica membranes can be enhanced by surface modification using APTS (3-aminopropyl-triethoxy silane). The hypothesized transport mechanism in such materialsis the reaction of CO2 with surface amine groups to form a carbamate species and subsequent surface ``hopping'' of CO2. DFT calculations were performed in order to elucidate the mechanism of CO2 transport in APTS modified membranes, to compute the CO2 diffusivity through the membrane, and to calculate its binding energy on an amine strand. The computed binding energy for docking one CO2 molecule to an amine was calculated to be 15.5 kcal/mol (0.67 eV). The activation/barrier energy for a CO2 molecule to hop from one amine strand (in form of carbamate) to another computed using Transition State Theory (TST) was 7.2 kcal/mol (0.31 eV) and compares well with our experimental data (˜ 8kcal/mol; 0.35 eV). In the configuration studied, CO2 hops from one strand to another in a zigzag fashion due to thermal motion of the strands; a strand with the CO2 molecule undulates and eventually moves so that the CO2 can be attracted by an adjacent strand. The CO2 diffusivity calculated using the computed activation energy ranged from 1.1 X 10-11m^2/sec (@ 25 C) to 5.7 X 10-10m^2/sec (@100 C).

  5. 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.

  6. 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.

  7. 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.

  8. 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).

  9. Carbon Dioxide Capture and Dyes Separation in a Porous Framework with Anionic Sql Net

    NASA Astrophysics Data System (ADS)

    Tan, Yanxi; Zhang, Ying; Zhang, Jian; Zheng, Yanjun

    2014-12-01

    Presented here is a water-stable MOF material [In(5-AIPA)2] ṡ Me2NH2(1; 5-AIPA = 5-Aminoisophthalic acid) built from the connecting of tetrahedral building units [In(COO)4]-. The sql net of compound 1 exhibits preferable chemical and thermal stability confirmed by thermal gravimetric analyses (TGA) and powder X-ray diffraction pattern (PXRD) measurements. The activated empty phase of 1a, as a good candidate material for CO2 capture, shows a CO2 uptake of 56.6 cm3/g and CH4/CO2 selectivity in excess of 16.4. Remarkably, based on the cation exchange mechanism, 1a has excellent MB affinity and can adsorb MB over MO from water in two hours. The results further support the idea that the ionic MOFs can find more applications in the separation of ionic dyes for the purifying of dye wastewater.

  10. Microporous Metal-Organic Framework Stabilized by Balanced Multiple Host-Couteranion Hydrogen-Bonding Interactions for High-Density CO2 Capture at Ambient Conditions.

    PubMed

    Ye, Yingxiang; Xiong, Shunshun; Wu, Xiaonan; Zhang, Liuqin; Li, Ziyin; Wang, Lihua; Ma, Xiuling; Chen, Qian-Huo; Zhang, Zhangjing; Xiang, Shengchang

    2016-01-01

    Microporous metal organic frameworks (MOFs) show promising application in several fields, but they often suffer from the weak robustness and stability after the removal of guest molecules. Here, three isostructural cationic metal-organic frameworks {[(Cu4Cl)(cpt)4(H2O)4]·3X·4DMAc·CH3OH·5H2O} (FJU-14, X = NO3, ClO4, BF4; DMAc = N,N'-dimethylacetamide) containing two types of polyhedral nanocages, one octahedron, and another tetrahedron have been synthesized from bifunctional organic ligands 4-(4H-1,2,4-triazol-4-yl) benzoic acid (Hcpt) and various copper salts. The series of MOFs FJU-14 are demonstrated as the first examples of the isostructural MOFs whose robustness, thermal stability, and CO2 capacity can be greatly improved via rational modulation of counteranions in the tetrahedral cages. The activated FJU-14-BF4-a containing BF4(-) anion can take CO2 of 95.8 cm(3) cm(-3) at ambient conditions with an adsorption enthalpy only of 18.8 kJ mol(-1). The trapped CO2 density of 0.955 g cm(-3) is the highest value among the reported MOFs. Dynamic fixed bed breakthrough experiments indicate that the separation of CO2/N2 mixture gases through a column packed with FJU-14-BF4-a solid can be efficiently achieved. The improved robustness and thermal stability for FJU-14-BF4-a can be attributed to the balanced multiple hydrogen-bonding interactions (MHBIs) between the BF4(-) counteranion and the cationic skeleton, while the high-density and low-enthalpy CO2 capture on FJU-14-BF4-a can be assigned to the multiple-point interactions between the adsorbate molecules and the framework as well as with its counteranions, as proved by single-crystal structures of the guest-free and CO2-loaded FJU-14-BF4-a samples. PMID:26653758

  11. 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

  12. 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.

  13. 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.

  14. 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

  15. ADVANCED OXYFUEL BOILERS AND PROCESS HEATERS FOR COST EFFECTIVE CO2 CAPTURE AND SEQUESTRATION

    SciTech Connect

    John Sirman; Leonard Switzer; Bart van Hassel

    2004-06-01

    This annual technical progress report summarizes the work accomplished during the second year of the program, January-December 2003, in the following task areas: Task 1--Conceptual Design, Task 2--Laboratory Scale Evaluations, Task 3--OTM Development, Task 4--Economic Evaluation and Commercialization Planning and Task 5--Program Management. The program has experienced significant delays due to several factors. The budget has also been significantly under spent. Based on recent technical successes and confirmation of process economics, significant future progress is expected. Concepts for integrating Oxygen Transport Membranes (OTMs) into boilers and process heaters to facilitate oxy-fuel combustion have been investigated. OTM reactor combustion testing was delayed to insufficient reliability of the earlier OTM materials. Substantial improvements to reliability have been identified and testing will recommence early in 2004. Promising OTM material compositions and OTM architectures have been identified that improve the reliability of the ceramic elements. Economic evaluation continued. Information was acquired that quantified the attractiveness of the advanced oxygen-fired boiler. CO{sub 2} capture and compression are still estimated to be much less than $10/ton CO{sub 2}.

  16. 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.

  17. 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. PMID:25016453

  18. Influence of Dissolved Metals on N-Nitrosamine Formation under Amine-based CO2 Capture Conditions.

    PubMed

    Wang, Zimeng; Mitch, William A

    2015-10-01

    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. PMID:26335609

  19. Characterization of the Axial Jet Separator with a CO2/Helium Mixture: Toward GC-AMS Hyphenation.

    PubMed

    Salazar, G; Agrios, K; Eichler, R; Szidat, S

    2016-02-01

    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. PMID:26652049

  20. Improved Interfacial Affinity and CO2 Separation Performance of Asymmetric Mixed Matrix Membranes by Incorporating Postmodified MIL-53(Al).

    PubMed

    Zhu, Haitao; Wang, Lina; Jie, Xingming; Liu, Dandan; Cao, Yiming

    2016-08-31

    Asymmetric mixed matrix membranes(MMMs) with MOFs hold great application potential for energy-efficient gas separations. However, the particle aggregation and nonselective interfacial microvoids restrict the gas separation performance of asymmetric MMMs. Herein, nanoporous metal-organic framework (MOF) of MIL-53(Al) was modified with aminosilane after solvothermal synthesis. The postfunctionalization by grafting alkyl chains can form hydrogen bonds with polymer chains to enhance the affinity with polymer matrix and facilitate the preferential adsorption of CO2 by dipole-quadrupole interaction with the functional group. Then the postmodified MIL-53(Al) was incorporated as filler into poly(ether imide) Ultem1000 to fabricate high-quality asymmetric MMMs with well dispersed particles in polymer matrix and good adhesion at the MOFs-polymer interface. The Ultem/S-MIL-53(Al) asymmetric MMMs exhibited remarkable combinations of gas permeance and ideal selectivity for CO2/N2 separation at 10 wt % filler loading. The CO2 permeance achieved 24.1 GPU, an increase of 165% compared with pure Ultem membrane. Meanwhile, the ideal CO2/N2 selectivity also increased from 31.0 up to 41.1. The strategy of post covalent modification for MOFs provides an effective way to improve the interfacial affinity and gas separation performance. PMID:27505152

  1. 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. PMID:27225027

  2. Integrated High Temperature Coal to Hydrogen System with CO2 Separation: Semi-Annual Progress Report 1

    SciTech Connect

    Ruud, J A; Ku, A; Ramaswamy, V; Wei, W

    2005-12-21

    This is the first semi-annual progress report for the program "Integrated High Temperature Coal to Hydrogen System with CO2 Separation." The objective of the program is to develop a detailed design for a single high-temperature syngas-cleanup module to produce a pure stream of H2 from a coal-based system and to develop the new high-temperature membrane materials at the core of that design. The novel one-box process combines a shift reactor with a high-temperature CO2-selective membrane to convert CO to CO2, remove sulfur compounds, and remove CO2 in a simple, compact, fully integrated system. In the first six months of the program, a conceptual design for the one-box system was developed in Task 1 and the performance targets for the system and the membrane were evaluated. In Task 2.1 processes were developed for creating pore architectures in ceramics that are applicable to membrane structures. In Task 2.2, candidate materials were identified that have the potential for separation of CO2 and H2S at high temperatures.

  3. Capture of atmospheric CO2 into (BiO)2CO3/graphene or graphene oxide nanocomposites with enhanced photocatalytic performance

    NASA Astrophysics Data System (ADS)

    Zhang, Wendong; Dong, Fan; Zhang, Wei

    2015-12-01

    Self-assembly of (BiO)2CO3 nanoflakes on graphene (Ge) and graphene oxide (GO) nanosheets, as an effective strategy to improve the photocatalytic performance of two-dimensional (2D) nanostructured materials, were realized by a one-pot efficient capture of atmospheric CO2 at room temperature. The as-synthesized samples were characterized by XRD, SEM, TEM, XPS, UV-vis DRS, Time-resolved ns-level PL and BET-BJH measurement. The photocatalytic activity of the obtained samples was evaluated by the removal of NO at the indoor air level under simulated solar-light irradiation. Compared with pure (BiO)2CO3, (BiO)2CO3/Ge and (BiO)2CO3/GO nanocomposites exhibited enhanced photocatalytic activity due to their large surface areas and pore volume, and efficient charge separation and transfer. The present work could provide a simple method to construct 2D nanocomposites by efficient utilization of CO2 in green synthetic strategy.

  4. 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

    2016-03-01

    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. PMID:26813048

  5. 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

  6. Extraction of Mg(OH)2 from Mg silicate minerals with NaOH assisted with H2O: implications for CO2 capture from exhaust flue gas.

    PubMed

    Madeddu, Silvia; Priestnall, Michael; Godoy, Erik; Kumar, R Vasant; Raymahasay, Sugat; Evans, Michael; Wang, Ruofan; Manenye, Seabelo; Kinoshita, Hajime

    2015-01-01

    The utilisation of Mg(OH)2 to capture exhaust CO2 has been hindered by the limited availability of brucite, the Mg(OH)2 mineral in natural deposits. Our previous study demonstrated that Mg(OH)2 can be obtained from dunite, an ultramafic rock composed of Mg silicate minerals, in highly concentrated NaOH aqueous systems. However, the large quantity of NaOH consumed was considered an obstacle for the implementation of the technology. In the present study, Mg(OH)2 was extracted from dunite reacted in solid systems with NaOH assisted with H2O. The consumption of NaOH was reduced by 97% with respect to the NaOH aqueous systems, maintaining a comparable yield of Mg(OH)2 extraction, i.e. 64.8-66%. The capture of CO2 from a CO2-N2 gas mixture was tested at ambient conditions using a Mg(OH)2 aqueous slurry. Mg(OH)2 almost fully dissolved and reacted with dissolved CO2 by forming Mg(HCO3)2 which remained in equilibrium storing the CO2 in the aqueous solution. The CO2 balance of the process was assessed from the emissions derived from the power consumption for NaOH production and Mg(OH)2 extraction together with the CO2 captured by Mg(OH)2 derived from dunite. The process resulted as carbon neutral when dunite is reacted at 250 °C for durations of 1 and 3 hours and CO2 is captured as Mg(HCO3)2. PMID:26391815

  7. 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

  8. Toward understanding amines and their degradation products from postcombustion CO2 capture processes with aerosol mass spectrometry.

    PubMed

    Ge, Xinlei; Shaw, Stephanie L; Zhang, Qi

    2014-05-01

    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

  9. A detailed study of cholinium chloride and levulinic acid deep eutectic solvent system for CO2 capture via experimental and molecular simulation approaches.

    PubMed

    Ullah, Ruh; Atilhan, Mert; Anaya, Baraa; Khraisheh, Majeda; García, Gregorio; ElKhattat, Ahmed; Tariq, Mohammad; Aparicio, Santiago

    2015-08-28

    Choline chloride + levulinic acid deep eutectic solvent is studied as a suitable material for CO2 capturing purposes. The most relevant physicochemical properties of this solvent are reported together with the CO2 solubility as a function of temperature. The corrosivity of this solvent is studied showing better performance than amine-based solvents. A theoretical study using both density functional theory and molecular dynamics approaches is carried out to analyze the properties of this fluid from the nanoscopic viewpoint, and their relationship with the macroscopic behavior of the system and its ability for CO2 capturing. The behavior of the liquid-gas interface is also studied and its role on the CO2 absorption mechanism is analyzed. The reported combined experimental and theoretical approach leads to a complete picture of the behavior of this new sorbent with regard to CO2, which together with its low cost, and the suitable environmental and toxicological properties of this solvent, lead to a promising candidate for CO2 capturing technological applications. PMID:26214080

  10. Accessing siloxane functionalized polynorbornenes via vinyl-addition polymerization for CO2 separation membranes

    DOE PAGESBeta

    Mahurin, Shannon Mark; Sokolov, Alexei P.; Saito, Tomonori; Long, Brian K.; Gmernicki, Kevin R.; Hong, Eunice; Maroon, Christopher R.

    2016-07-06

    Here, the vinyl addition polymerization of norbornylbased monomers bearing polar functional groups is often problematic, leading to low molecular weight polymers in poor yield. Herein, we provide proof-of-principle evidence that addition-type homopolymers of siloxane substituted norbornyl-based monomers may be readily synthesized using the catalyst trans-[Ni(C6F5)2(SbPh3)2]. Polymerizations using this catalyst reached moderate to high conversion in just 5 min of polymerization and produced siloxanesubstituted polymers with molecular weights exceeding 100 kg/mol. These polymers showed excellent thermal stability (Td ≥ 362 °C) and were cast into membranes that displayed high CO2 permeability and enhanced CO2/N2 selectivity as compared to related materials.

  11. TECHNOLOGY IN AN INTEGRATED ASSESSMENT MODEL: THE POTENTIAL REGIONAL DEPLOYMENT OF CARBON CAPTURE AND STORAGE IN THE CONTEXT OF GLOBAL CO2 STABILIZATION

    SciTech Connect

    Edmonds, James A.; Dooley, James J.; Kim, Son H.; Friedman, S. Julio; Wise, Marshall A.

    2007-11-19

    Technology is a critically important determinant of the cost of meeting any environmental objective. In this paper we examine the role of a particular technology, carbon dioxide capture and storage (CCS), in the stabilization of the concentration of atmospheric carbon dioxide (CO2). While CCS is not presently deployed at scale, it has the potential to deploy extensively during the course of the 21st century if concentrations of atmospheric CO2 are to be stabilized. The existing research literature has focused largely on the cost of capturing CO2, with the implicit assumption that storage options would be relatively cheap, plentiful and located in close proximity to future CO2 point sources. However, CO2 capture and storage will take place at the local and regional scale and will compete with other mitigation options that also exhibit local or regional differences. This paper provides an initial examination of the implications of regionally disaggregated demand for and supply of CO2 storage reservoirs within the context of a globally disaggregated, long-term analysis of both the geology and economics of CCS. This analysis suggests that some regions will see their ability to deploy CCS systems constrained by a lack of quality target reservoirs relative to the demand for storage placed upon these candidate geologic storage reservoirs by large stationary CO2 point sources within the region. Other regions appear to have sufficient storage capacity to easily carry them into the 22nd century. We examined the regional and global economic implications of the distribution of these sources and sinks in meeting various potential limits to atmospheric CO2 concentrations. This analysis confirms that CCS is an important potential response to climate change throughout the 21st century and a technology that can play a key role in controlling the cost of addressing climate change.

  12. Accelerated Carbonate Dissolution as a CO2 Separation and Sequestration Strategy

    SciTech Connect

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

    2004-02-18

    We have proposed a technique that could reduce CO{sub 2} emissions from near coastal fossil-fuel power plants using existing power plant cooling water flow rates (Rau and Caldeira, 1999; Caldeira and Rau, 2000). Preliminary cost estimates are as low as $68 per tonne C sequestered, as compared to > $170 per tonne C estimated for other approaches to CO{sub 2} separation with geologic or deep-ocean storage. Engineers at McDermott Technologies, Inc., have independently estimated the cost of our proposed technique, and came to the conclusion that our cost estimates were at the high end of the likely range. Interest has been expressed in pursuing this approach further both in Norway and in Japan. We have proved the viability of our concept using (1) bench-top laboratory experiments (Figures 1 and 2), (2) computer modeling of those experiments, (3) more sophisticated cost estimates, and (4) three-dimensional computer modeling of the consequences to global ocean chemistry (Figure 3 and 4). The climate and environmental impacts of our current, carbon intensive energy usage demands that effective and practical energy alternatives and CO{sub 2} mitigation strategies be found. As part of this effort, various means of capturing and storing CO{sub 2} generated from fossil-fuel-based energy production are being investigated (e.g. [3,4]). One of the proposed methods involves a geochemistry-based capture and sequestration process [5,6] that hydrates point-source, waste CO{sub 2} with water to produce a carbonic acid solution. This in turn is reacted and neutralized with limestone, thus converting the original CO{sub 2} gas to calcium bicarbonate in solution, the overall reaction being: CO{sub 2(g)} + H{sub 2}O{sub (l)} + CaCO{sub 3(s)} {yields} Ca{sub (aq)}{sup 2+} + 2HCO{sub 3(aq)}{sup -} The dissolved calcium bicarbonate produced is then released and diluted in the ocean where it would add minimally to the large, benign pool of these ions already present in seawater. Such a

  13. Development of sintering-resistant CaO-based sorbent derived from eggshells and bauxite tailings for cyclic CO2 capture.

    PubMed

    Shan, ShaoYun; Ma, AiHua; Hu, YiCheng; Jia, QingMing; Wang, YaMing; Peng, JinHui

    2016-01-01

    Carbon dioxide, one of the major greenhouse gases, are believed to be a major contributor to global warming. As a consequence, it is imperative for us to control and remove CO2 emissions. The CaO, a kind of effective CO2 sorbent at high temperature, has attracted increasing attention due to some potential advantages. The main drawback in practical application is the deterioration of CO2 capture capacity following multiples cycles. In the present study, novel low-cost porous CaO-based sorbents with excellent CO2 absorption-desorption performance were synthesized using bauxite tailings (BTs) and eggshells as raw materials via solid-phase method. Effect of different BTs content on CO2 absorption-desorption properties was investigated. Phase composition and morphologies were analyzed by XRD and SEM, and CO2 absorption properties were investigated by the simultaneous thermogravimetric analyzer. The as-prepared CaO-based sorbent doped with 10 wt% BTs showed superior CO2 absorption stability during multiple absorption-desorption cycles, with being >55% conversion after 40 cycles. This improved CO2 absorption performance was attributed to the particular morphologies of the CaO-based sorbents. Additionally, during absorption-desorption cycles the occurrence of Ca12Al14O33 phase is considered to be responsible for the excellent CO2 absorption performance of CaO-based sorbents. In the meanwhile, the use of solid waste eggshell and BTs not only decreases the release of solid waste, but also moderates the greenhouse effect resulted from CO2. PMID:26549755

  14. Efficient CO2 capture by tertiary amine-functionalized ionic liquids through Li+-stabilized zwitterionic adduct formation

    PubMed Central

    Yang, Zhen-Zhen

    2014-01-01

    Summary Highly efficient CO2 absorption was realized through formation of zwitterionic adducts, combining synthetic strategies to ionic liquids (ILs) and coordination. The essence of our strategy is to make use of multidentate cation coordination between Li+ and an organic base. Also PEG-functionalized organic bases were employed to enhance the CO2-philicity. The ILs were reacted with CO2 to form the zwitterionic adduct. Coordination effects between various lithium salts and neutral ligands, as well as the CO2 capacity of the chelated ILs obtained were investigated. For example, the CO2 capacity of PEG150MeBu2N increased steadily from 0.10 to 0.66 (mol CO2 absorbed per mol of base) through the formation of zwitterionic adducts being stabilized by Li+. PMID:25246955

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

    NASA Astrophysics Data System (ADS)

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

    2015-09-01

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

  16. Simulation of the potential effects of CO2 leakage from carbon capture and storage activities on the mobilization and speciation of metals.

    PubMed

    de Orte, Manoela Romanó; Sarmiento, Aguasanta M; DelValls, T Ángel; Riba, Inmaculada

    2014-09-15

    One of the main risks associated with carbon capture and storage (CCS) activities is the leakage of the stored CO2, which can result in several effects on the ecosystem. Laboratory-scale experiments were performed to provide data on the possible effects of CO2 leakage from CCS on the mobility of metals previously trapped in sediments. Metal-contaminated sediments were collected and submitted to acidification by means of CO2 injection using different pH treatments. The test lasted 10 days, and samples were collected at the beginning and at the end of the experiment for metal analysis. The results revealed increases in the mobility of metals such as Co, Cu, Fe, Pb and Zn due to pH decreases. Geochemical modeling demonstrated that acidification influenced the speciation of the metals, increasing the concentrations of their free forms. These data suggest the possible sediment contamination consequences of accidental CO2 leakage during CCS activities. PMID:25125286

  17. Investigation of transport and mechnical properties for hollow fibers containing ionic liquids for pre-combustion CO2 capture

    SciTech Connect

    Hopkinson, D., Wickramanayake, S., Myers, C., Sui, L., Nicola, M., Luebke, D.

    2011-01-01

    Currently available techniques for CO{sub 2} separation from flue or fuel gas cannot economically capture CO{sub 2} for sequestration. Membranes offer several advantages in CO{sub 2} separation such as simple operation, low water consumption, and in some cases higher energy efficiency. However, traditional polymer membranes are limited by the separation characteristics of the polymer and often suffer from low permeability and selectivity. Several research groups have attempted to overcome these limitations by using supported ionic liquid membranes (SILMs) in which an ionic liquid (IL) is suspended within the pores of a membrane support and serves as the active gas separation component of the membrane. For industrial applications, hollow fibers are preferred over flat membranes due to their smaller footprint, ease of high efficiency module design and low fabrication cost. In an attempt to investigate and address these issues, polymeric hollow fiber-based ionic liquid membranes were fabricated. Matrimid® and [hmim][Tf{sub 2}N] (1-hexyl-3-methylimidalzolium bis(trifluoromethyl sulfonyl) imide) were selected as the polymeric and ionic liquid materials, and the fibers were fabricated via nonsolvent-induced phase separation/extraction, employing a single layer spinneret extrusion system. The system takes advantage of the fiber morphology to enable more efficient mass transfer than traditional membranes geometries. CO{sub 2} and H{sub 2} transport properties will be reported for the Matrimid hollow fibers from 37 to 150 {degrees}C. Also, several mechanical properties such as tensile strength, modulus, and glass transition temperature have been measured for the fiber using dynamic mechanical analysis.

  18. Impact of CO2 leakage from sub-seabed carbon dioxide capture and storage (CCS) reservoirs on benthic virus-prokaryote interactions and functions.

    PubMed

    Rastelli, Eugenio; Corinaldesi, Cinzia; Dell'Anno, Antonio; Amaro, Teresa; Queirós, Ana M; Widdicombe, Stephen; Danovaro, Roberto

    2015-01-01

    Atmospheric CO2 emissions are a global concern due to their predicted impact on biodiversity, ecosystems functioning, and human life. Among the proposed mitigation strategies, CO2 capture and storage, primarily the injection of CO2 into marine deep geological formations has been suggested as a technically practical option for reducing emissions. However, concerns have been raised that possible leakage from such storage sites, and the associated elevated levels of pCO2 could locally impact the biodiversity and biogeochemical processes in the sediments above these reservoirs. Whilst a number of impact assessment studies have been conducted, no information is available on the specific responses of viruses and virus-host interactions. In the present study, we tested the impact of a simulated CO2 leakage on the benthic microbial assemblages, with specific focus on microbial activity and virus-induced prokaryotic mortality (VIPM). We found that exposure to levels of CO2 in the overlying seawater from 1,000 to 20,000 ppm for a period up to 140 days, resulted in a marked decrease in heterotrophic carbon production and organic matter degradation rates in the sediments, associated with lower rates of VIPM, and a progressive accumulation of sedimentary organic matter with increasing CO2 concentrations. These results suggest that the increase in seawater pCO2 levels that may result from CO2 leakage, can severely reduce the rates of microbial-mediated recycling of the sedimentary organic matter and viral infections, with major consequences on C cycling and nutrient regeneration, and hence on the functioning of benthic ecosystems. PMID:26441872

  19. Impact of CO2 leakage from sub-seabed carbon dioxide capture and storage (CCS) reservoirs on benthic virus–prokaryote interactions and functions

    PubMed Central

    Rastelli, Eugenio; Corinaldesi, Cinzia; Dell’Anno, Antonio; Amaro, Teresa; Queirós, Ana M.; Widdicombe, Stephen; Danovaro, Roberto

    2015-01-01

    Atmospheric CO2 emissions are a global concern due to their predicted impact on biodiversity, ecosystems functioning, and human life. Among the proposed mitigation strategies, CO2 capture and storage, primarily the injection of CO2 into marine deep geological formations has been suggested as a technically practical option for reducing emissions. However, concerns have been raised that possible leakage from such storage sites, and the associated elevated levels of pCO2 could locally impact the biodiversity and biogeochemical processes in the sediments above these reservoirs. Whilst a number of impact assessment studies have been conducted, no information is available on the specific responses of viruses and virus–host interactions. In the present study, we tested the impact of a simulated CO2 leakage on the benthic microbial assemblages, with specific focus on microbial activity and virus-induced prokaryotic mortality (VIPM). We found that exposure to levels of CO2 in the overlying seawater from 1,000 to 20,000 ppm for a period up to 140 days, resulted in a marked decrease in heterotrophic carbon production and organic matter degradation rates in the sediments, associated with lower rates of VIPM, and a progressive accumulation of sedimentary organic matter with increasing CO2 concentrations. These results suggest that the increase in seawater pCO2 levels that may result from CO2 leakage, can severely reduce the rates of microbial-mediated recycling of the sedimentary organic matter and viral infections, with major consequences on C cycling and nutrient regeneration, and hence on the functioning of benthic ecosystems. PMID:26441872

  20. CO2/light gas separation performance of cross-linked poly(vinylimidazolium) gel membranes as a function of ionic liquid loading and cross-linker content

    SciTech Connect

    Carlisle, TK; Nicodemus, GD; Gin, DL; Noble, RD

    2012-04-15

    A series of cross-linked poly(vinylimidazolium)-RTIL gel membranes was synthesized and evaluated for room-temperature, ideal CO2/N-2, CO2/CH4, and CO2/H-2 separation performance. The membranes were formed by photo-polymerization of oligo(ethylene glycol)-functionalized cross-linking (i.e., di-functional) and non-cross-linking (i.e., mono-functional) vinylimidazolium RTIL monomers with nonpolymerizable, "free RTIL." The effect of free RTIL ([emim][Tf2N]) loading on CO2 separation performance was evaluated by varying RTIL loading at three levels (45, 65, and 75 wt.%). The effect of cross-linker content on CO2 separation performance was also evaluated by varying the copolymer composition of cross-linked membranes from 5 to 100 mol% di-functional monomer. The substituent on the monofunctional RTIL monomer was also varied to investigate the effect of substituent structure and chemistry on CO2 separation performance. CO2 permeability was dramatically increased with higher loading of free RTIL. Increased RTIL loading had no effect on CO2/N-2 or CO2/CH4 permeability selectivity, but significantly improved CO2/H-2 permeability selectivity. Reducing the cross-linking monomer concentration generally improved CO2 permeability. However, anomalous permeability and selectivity behavior was observed below critical concentrations of cross-linker. The effect of the substituent on the monofunctional monomer on CO2 separation performance was minimal compared to the effects of RTIL loading and copolymer composition. (C) 2012 Elsevier B.V. All rights reserved.

  1. The cost of meeting increased cooling-water demands for CO2 capture and storage utilizing non-traditional waters from geologic saline formations

    NASA Astrophysics Data System (ADS)

    Klise, Geoffrey T.; Roach, Jesse D.; Kobos, Peter H.; Heath, Jason E.; Gutierrez, Karen A.

    2013-05-01

    Deep (> ˜800 m) saline water-bearing formations in the United States have substantial pore volume that is targeted for storage of carbon dioxide (CO2) and the associated saline water can be extracted to increase CO2 storage efficiency, manage pressure build up, and create a new water source that, once treated, can be used for power-plant cooling or other purposes. Extraction, treatment and disposal costs of saline formation water to meet added water demands from CO2 capture and storage (CCS) are discussed. This underutilized water source may be important in meeting new water demand associated with CCS. For a representative natural gas combined-cycle (NGCC) power plant, simultaneous extraction of brine from the storage formation could provide enough water to meet all CCS-related cooling demands for 177 out of the 185 (96 %) saline formations analyzed in this study. Calculated total cost of water extraction, treatment and disposal is less than 4.00 US Dollars (USD) m-3 for 93 % of the 185 formations considered. In 90 % of 185 formations, treated water costs are less than 10.00 USD tonne-1 of CO2 injected. On average, this represents approximately 6 % of the total CO2 capture and injection costs for the NGCC scenario.

  2. Ab Initio Thermodynamic Study of the CO2 Capture Properties of Potassium Carbonate Sesquihydrate, K2CO3·1.5H2O

    SciTech Connect

    Duan, Yuhua; Luebkes,David R.; Pennline, Henry W; Li, Bingyun Li; Janik, Michael J.; Halley, Woods

    2012-01-01

    By combining density functional theory and lattice phonon dynamics, the thermodynamic properties of CO2 absorption/desorption reactions with dehydrated potassium carbonates through K2CO3·1.5H2O + CO2 = 2KHCO3 + 0.5H2O(g) are analyzed. The energy change and the chemical potential of this reaction have been calculated and used to evaluate its thermodynamic properties and phase transitions. The results indicate that the K2CO3·1.5H2O can only be applied for postcombustion CO2 capture technology at temperatures lower than its phase transition temperature, which depends on the CO2 pressure and the steam pressure with the best range being PH2O ≤ 1.0 bar. Above the phase transition temperature, the sorbent will be regenerated into anhydrous K2CO3. If the steam pressure PH2O is much greater than 1.0 bar, it is possible to use the K2CO3·1.5H2O sorbent for precombustion CO2 capture technology. Compared to anhydrous K2CO3, K2CO3·1.5H2O requires less energy for regeneration.

  3. One-Step Synthesis of Microporous Carbon Monoliths Derived from Biomass with High Nitrogen Doping Content for Highly Selective CO2 Capture.

    PubMed

    Geng, Zhen; Xiao, Qiangfeng; Lv, Hong; Li, Bing; Wu, Haobin; Lu, Yunfeng; Zhang, Cunman

    2016-01-01

    The one-step synthesis method of nitrogen doped microporous carbon monoliths derived from biomass with high-efficiency is developed using a novel ammonia (NH3)-assisted activation process, where NH3 serves as both activating agent and nitrogen source. Both pore forming and nitrogen doping simultaneously proceed during the process, obviously superior to conventional chemical activation. The as-prepared nitrogen-doped active carbons exhibit rich micropores with high surface area and high nitrogen content. Synergetic effects of its high surface area, microporous structure and high nitrogen content, especially rich nitrogen-containing groups for effective CO2 capture (i.e., phenyl amine and pyridine-nitrogen) lead to superior CO2/N2 selectivity up to 82, which is the highest among known nanoporous carbons. In addition, the resulting nitrogen-doped active carbons can be easily regenerated under mild conditions. Considering the outstanding CO2 capture performance, low production cost, simple synthesis procedure and easy scalability, the resulting nitrogen-doped microporous carbon monoliths are promising candidates for selective capture of CO2 in industrial applications. PMID:27488268

  4. One-Step Synthesis of Microporous Carbon Monoliths Derived from Biomass with High Nitrogen Doping Content for Highly Selective CO2 Capture

    PubMed Central

    Geng, Zhen; Xiao, Qiangfeng; Lv, Hong; Li, Bing; Wu, Haobin; Lu, Yunfeng; Zhang, Cunman

    2016-01-01

    The one-step synthesis method of nitrogen doped microporous carbon monoliths derived from biomass with high-efficiency is developed using a novel ammonia (NH3)-assisted activation process, where NH3 serves as both activating agent and nitrogen source. Both pore forming and nitrogen doping simultaneously proceed during the process, obviously superior to conventional chemical activation. The as-prepared nitrogen-doped active carbons exhibit rich micropores with high surface area and high nitrogen content. Synergetic effects of its high surface area, microporous structure and high nitrogen content, especially rich nitrogen-containing groups for effective CO2 capture (i.e., phenyl amine and pyridine-nitrogen) lead to superior CO2/N2 selectivity up to 82, which is the highest among known nanoporous carbons. In addition, the resulting nitrogen-doped active carbons can be easily regenerated under mild conditions. Considering the outstanding CO2 capture performance, low production cost, simple synthesis procedure and easy scalability, the resulting nitrogen-doped microporous carbon monoliths are promising candidates for selective capture of CO2 in industrial applications. PMID:27488268

  5. One-Step Synthesis of Microporous Carbon Monoliths Derived from Biomass with High Nitrogen Doping Content for Highly Selective CO2 Capture

    NASA Astrophysics Data System (ADS)

    Geng, Zhen; Xiao, Qiangfeng; Lv, Hong; Li, Bing; Wu, Haobin; Lu, Yunfeng; Zhang, Cunman

    2016-08-01

    The one-step synthesis method of nitrogen doped microporous carbon monoliths derived from biomass with high-efficiency is developed using a novel ammonia (NH3)-assisted activation process, where NH3 serves as both activating agent and nitrogen source. Both pore forming and nitrogen doping simultaneously proceed during the process, obviously superior to conventional chemical activation. The as-prepared nitrogen-doped active carbons exhibit rich micropores with high surface area and high nitrogen content. Synergetic effects of its high surface area, microporous structure and high nitrogen content, especially rich nitrogen-containing groups for effective CO2 capture (i.e., phenyl amine and pyridine-nitrogen) lead to superior CO2/N2 selectivity up to 82, which is the highest among known nanoporous carbons. In addition, the resulting nitrogen-doped active carbons can be easily regenerated under mild conditions. Considering the outstanding CO2 capture performance, low production cost, simple synthesis procedure and easy scalability, the resulting nitrogen-doped microporous carbon monoliths are promising candidates for selective capture of CO2 in industrial applications.

  6. Dissolution kinetics of magnesium hydroxide for CO2 separation from coal-fired power plants.

    PubMed

    Bharadwaj, Hari Krishna; Lee, Joo-Youp; Li, Xin; Liu, Zhouyang; Keener, Tim C

    2013-04-15

    The dissolution of magnesium hydroxide in water for the release of magnesium and hydroxyl ions into the solution to maintain suitable alkalinity is a crucial step in the Mg(OH)2-based CO2 absorption process. In this study, the rate of dissolution of Mg(OH)2 was investigated under different operating conditions using a pH stat apparatus. The dissolution process was modeled using a shrinking core model and the overall Mg(OH)2 dissolution process was found to be controlled by the surface chemical reaction of Mg(OH)2 with H(+) ions. Under the chemical reaction control regime, the dissolution of Mg(OH)2 in alkaline conditions was found not to follow a first-order reaction, and the fractional order of reaction was estimated to lie between 0.20 and 0.31. This suggests that the dissolution reaction is a non-elementary reaction, consisting of a sequence of elementary reactions, via most likely forming a surface magnesium complex. The true activation energy value of 76 ± 11 kJ/gmol was found to be almost twice as much as the observed activation energy value of 42 ± 6 kJ/gmol determined at pH 8.6, and was comparable with the previously reported values. The particle sizes predicted from the intrinsic kinetics determined from the model were in good agreement with the experimentally measured particle sizes during the dissolution process. PMID:23474403

  7. Moisture-Stable Zn(II) Metal-Organic Framework as a Multifunctional Platform for Highly Efficient CO2 Capture and Nitro Pollutant Vapor Detection.

    PubMed

    Chen, Di-Ming; Tian, Jia-Yue; Chen, Min; Liu, Chun-Sen; Du, Miao

    2016-07-20

    A moisture-stable three-dimensional (3D) metal-organic framework (MOF), {(Me2NH2)[Zn2(bpydb)2(ATZ)](DMA)(NMF)2}n (1, where bpydb = 4,4'-(4,4'-bipyridine-2,6-diyl)dibenzoate, ATZ = deprotonated 5-aminotetrazole, DMA = N,N-dimethylacetamide, and NMF = N-methylformamide), with uncoordinated N-donor sites and charged framework skeleton was fabricated. This MOF exhibits interesting structural dynamic upon CO2 sorption at 195 K and high CO2/N2 (127) and CO2/CH4 (131) sorption selectivity at 298 K and 1 bar. Particularly, its CO2/CH4 selectivity is among the highest MOFs for selective CO2 separation. The results of Grand Canonical Monte Carlo (GCMC) simulation indicate that the polar framework contributes to the strong framework-CO2 binding at zero loading, and the tetrazole pillar contributes to the high CO2 uptake capacity at high loading. Furthermore, the solvent-responsive luminescent properties of 1 indicate that it could be utilized as a fluorescent sensor to detect trace amounts of nitrobenzene in both solvent and vapor systems. PMID:27340895

  8. Ultrafast vibrational spectroscopy (2D-IR) of CO2 in ionic liquids: Carbon capture from carbon dioxide's point of view.

    PubMed

    Brinzer, Thomas; Berquist, Eric J; Ren, Zhe; Dutta, Samrat; Johnson, Clinton A; Krisher, Cullen S; Lambrecht, Daniel S; Garrett-Roe, Sean

    2015-06-01

    The CO2ν3 asymmetric stretching mode is established as a vibrational chromophore for ultrafast two-dimensional infrared (2D-IR) spectroscopic studies of local structure and dynamics in ionic liquids, which are of interest for carbon capture applications. CO2 is dissolved in a series of 1-butyl-3-methylimidazolium-based ionic liquids ([C4C1im][X], where [X](-) is the anion from the series hexafluorophosphate (PF6 (-)), tetrafluoroborate (BF4 (-)), bis-(trifluoromethyl)sulfonylimide (Tf2N(-)), triflate (TfO(-)), trifluoroacetate (TFA(-)), dicyanamide (DCA(-)), and thiocyanate (SCN(-))). In the ionic liquids studied, the ν3 center frequency is sensitive to the local solvation environment and reports on the timescales for local structural relaxation. Density functional theory calculations predict charge transfer from the anion to the CO2 and from CO2 to the cation. The charge transfer drives geometrical distortion of CO2, which in turn changes the ν3 frequency. The observed structural relaxation timescales vary by up to an order of magnitude between ionic liquids. Shoulders in the 2D-IR spectra arise from anharmonic coupling of the ν2 and ν3 normal modes of CO2. Thermal fluctuations in the ν2 population stochastically modulate the ν3 frequency and generate dynamic cross-peaks. These timescales are attributed to the breakup of ion cages that create a well-defined local environment for CO2. The results suggest that the picosecond dynamics of CO2 are gated by local diffusion of anions and cations. PMID:26049445

  9. Ultrafast vibrational spectroscopy (2D-IR) of CO2 in ionic liquids: Carbon capture from carbon dioxide's point of view

    NASA Astrophysics Data System (ADS)

    Brinzer, Thomas; Berquist, Eric J.; Ren, Zhe; Dutta, Samrat; Johnson, Clinton A.; Krisher, Cullen S.; Lambrecht, Daniel S.; Garrett-Roe, Sean

    2015-06-01

    The CO2ν3 asymmetric stretching mode is established as a vibrational chromophore for ultrafast two-dimensional infrared (2D-IR) spectroscopic studies of local structure and dynamics in ionic liquids, which are of interest for carbon capture applications. CO2 is dissolved in a series of 1-butyl-3-methylimidazolium-based ionic liquids ([C4C1im][X], where [X]- is the anion from the series hexafluorophosphate (PF 6- ), tetrafluoroborate (BF 4- ), bis-(trifluoromethyl)sulfonylimide (Tf2N-), triflate (TfO-), trifluoroacetate (TFA-), dicyanamide (DCA-), and thiocyanate (SCN-)). In the ionic liquids studied, the ν3 center frequency is sensitive to the local solvation environment and reports on the timescales for local structural relaxation. Density functional theory calculations predict charge transfer from the anion to the CO2 and from CO2 to the cation. The charge transfer drives geometrical distortion of CO2, which in turn changes the ν3 frequency. The observed structural relaxation timescales vary by up to an order of magnitude between ionic liquids. Shoulders in the 2D-IR spectra arise from anharmonic coupling of the ν2 and ν3 normal modes of CO2. Thermal fluctuations in the ν2 population stochastically modulate the ν3 frequency and generate dynamic cross-peaks. These timescales are attributed to the breakup of ion cages that create a well-defined local environment for CO2. The results suggest that the picosecond dynamics of CO2 are gated by local diffusion of anions and cations.

  10. Capture and sequestration of CO2 in the interlayer space of hydrated calcium Montmorillonite clay under various geological burial depth

    NASA Astrophysics Data System (ADS)

    Yang, W.; Zaoui, A.

    2016-05-01

    We perform, at nanoscale level, the structure and dynamics of carbon dioxide molecules in hydrated Ca-montmorillonite clays. The swelling behaviour of hydrated Wyoming-type Montmorillonite including CO2 molecules and counterions is presented and analysed. In addition, the atom density profile, diffusion behaviours and radial distribution functions of CO2, interlayer water molecules and Calcium ions have been investigated at different geological burial depth of 0 km, 3 km and 6 km, which correspond to various temperature and pressure of simulation conditions. Furthermore, the influence of different hydration state on the dynamical behaviours of carbon dioxide is also explained. The calculated self-diffusion coefficient shows that the carbon dioxide species diffuse more freely with the increase of depth and water content. We also found that the presence of interlayer CO2 inhibits the diffusion of all the mobile species. These results mainly show that the hydrated clay system is an appropriate space capable of absorbing CO2 molecules.

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

    SciTech Connect

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

    2013-09-30

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

  12. SEPARATION OF CO2 FROM FLUE GASES BY CARBON-MULTIWALL CARBON NANOTUBE MEMBRANES

    SciTech Connect

    Rodney Andrews

    2001-03-01

    Multiwalled carbon nanotubes (MWNT) were found to be an effective separation media for removing CO{sub 2} from N{sub 2}. The separation mechanism favors the selective condensation of CO{sub 2} from the flowing gas stream. Significant uptakes of CO{sub 2} were measured at 30 C and 150 C over the pressure range 0.5 to 5 bar. No measurable uptake of nitrogen was found for this range of conditions. The mass uptake of CO{sub 2} by MWNT was found to increase with increasing temperature. A packed bed of MWNT completely removed CO{sub 2} from a flowing stream of CO{sub 2}/N{sub 2}, and exhibited rapid uptake kinetics for CO{sub 2}.

  13. Benzyl-Functionalized Room Temperature Ionic Liquids for CO2/N2 Separation

    SciTech Connect

    Mahurin, Shannon Mark; Dai, Thomas N; Yeary, Joshua S; Luo, Huimin; Dai, Sheng

    2011-01-01

    In this work, three classes of room temperature ionic liquids (RTILs), including imidazolium, pyridinium, and pyrrolidinium ionic liquids with a benzyl group appended to the cation, were synthesized and tested for their performance in separating CO{sub 2} and N{sub 2}. All RTILs contained the bis(trifluoromethylsulfonyl)imide anion, permitting us to distinguish the impact of the benzyl moiety attached to the cation on gas separation performance. In general, the attachment of the benzyl group increased the viscosity of the ionic liquid compared with the unfunctionalized analogs and decreased the CO{sub 2} permeability. However, all of the benzyl-modified ionic liquids exhibited enhanced CO{sub 2}/N{sub 2} selectivities compared with alkyl-based ionic liquids, with values ranging from 22.0 to 33.1. In addition, CO{sub 2} solubilities in the form of Henry's constants were also measured and compared with unfunctionalized analogs. Results of the membrane performance tests and CO{sub 2} solubility measurements demonstrate that the benzyl-functionalized RTILs have significant potential for use in the separation of carbon dioxide from combustion products.

  14. Zeolite screening for the separation of gas mixtures containing SO2, CO2 and CO.

    PubMed

    Matito-Martos, I; Martin-Calvo, A; Gutiérrez-Sevillano, J J; Haranczyk, M; Doblare, M; Parra, J B; Ania, C O; Calero, S

    2014-10-01

    We used a combination of experiments and molecular simulations to investigate at the molecular level the effects of zeolite structure on the adsorption and diffusion of sulfur dioxide, carbon dioxide and carbon monoxide as well as separation processes of their mixtures. Our study involved different zeolite topologies and revealed numerous structure-property trends depending on the temperature and pressure conditions. Sulfur dioxide, which has the strongest interactions with zeolites due to its size and polarity, showed the largest adsorption across investigated temperatures and pressures. Our results indicate that structures with channel-type pore topology and low pore volume are the most promising for selective adsorption of sulfur dioxide over carbon dioxide and carbon monoxide under room conditions, while structures with higher pore volume exhibit better storage capacity at higher pressure. Our results emphasize the need for considering both adsorption and diffusion processes in the selection of the optimal structure for a given separation process. Our findings help to identify the best materials for effective separation processes under realistic operating conditions. PMID:24691937

  15. Venting of a separate CO2-rich gas phase from submarine arc volcanoes: Examples from the Mariana and Tonga-Kermadec arcs

    NASA Astrophysics Data System (ADS)

    Lupton, John; Lilley, Marvin; Butterfield, David; Evans, Leigh; Embley, Robert; Massoth, Gary; Christenson, Bruce; Nakamura, Ko-Ichi; Schmidt, Mark

    2008-08-01

    Submersible dives on 22 active submarine volcanoes on the Mariana and Tonga-Kermadec arcs have discovered systems on six of these volcanoes that, in addition to discharging hot vent fluid, are also venting a separate CO2-rich phase either in the form of gas bubbles or liquid CO2 droplets. One of the most impressive is the Champagne vent site on NW Eifuku in the northern Mariana Arc, which is discharging cold droplets of liquid CO2 at an estimated rate of 23 mol CO2/s, about 0.1% of the global mid-ocean ridge (MOR) carbon flux. Three other Mariana Arc submarine volcanoes (NW Rota-1, Nikko, and Daikoku), and two volcanoes on the Tonga-Kermadec Arc (Giggenbach and Volcano-1) also have vent fields discharging CO2-rich gas bubbles. The vent fluids at these volcanoes have very high CO2 concentrations and elevated C/3He and δ13C (CO2) ratios compared to MOR systems, indicating a contribution to the carbon flux from subducted marine carbonates and organic material. Analysis of the CO2 concentrations shows that most of the fluids are undersaturated with CO2. This deviation from equilibrium would not be expected for pressure release degassing of an ascending fluid saturated with CO2. Mechanisms to produce a separate CO2-rich gas phase at the seafloor require direct injection of magmatic CO2-rich gas. The ascending CO2-rich gas could then partially dissolve into seawater circulating within the volcano edifice without reaching equilibrium. Alternatively, an ascending high-temperature, CO2-rich aqueous fluid could boil to produce a CO2-rich gas phase and a CO2-depleted liquid. These findings indicate that carbon fluxes from submarine arcs may be higher than previously estimated, and that experiments to estimate carbon fluxes at submarine arc volcanoes are merited. Hydrothermal sites such as these with a separate gas phase are valuable natural laboratories for studying the effects of high CO2 concentrations on marine ecosystems.

  16. ENHANCED HYDROGEN PRODUCTION INTEGRATED WITH CO2 SEPARATION IN A SINGLE-STAGE REACTOR

    SciTech Connect

    Himanshu Gupta; Mahesh Iyer; Bartev Sakadjian; Liang-Shih Fan

    2005-03-10

    Hydrogen production cannot be maximized from fossil fuels (gas/coal) via the WGS reaction at high temperatures as the WGS-equilibrium constant K{sub WGS} (= [CO{sub 2}][H{sub 2}]/[CO][H{sub 2}O]), falls with increasing temperatures. However, CO{sub 2} removal down to ppm levels by the carbonation of CaO to CaCO{sub 3} in the temperature range 650-850 C, leads to the possibility of stoichiometric H{sub 2} production at high temperature/pressure conditions and at low steam to fuel ratios. Further, CO{sub 2} is also captured in the H{sub 2} generation process, making this coal to hydrogen process compatible with CO{sub 2} sequestration goals. While microporous CaO sorbents attain <50% conversion over cyclical carbonation-calcination, the OSU-patented, mesoporous CaO sorbents are able to achieve >95% conversion. Novel calcination techniques could lead to an ever-smaller footprint, single-stage reactors that achieve maximum theoretical H{sub 2} production at high temperatures and pressures for on/off site usage. Experimental results indicate that the PCC-CaO sorbent is able to achieve complete conversion of CO for 240 seconds as compared to only a few seconds with CaO derived from natural sources.

  17. ENHANCED HYDROGEN PRODUCTION INTEGRATED WITH CO2 SEPARATION IN A SINGLE-STAGE REACTOR

    SciTech Connect

    Himanshu Gupta; Mahesh Iyer; Bartev Sakadjian; Liang-Shih Fan

    2005-04-01

    Hydrogen production by the water gas shift reaction (WGSR) is equilibrium limited due to thermodynamic constrains. However, this can be overcome by continuously removing the product CO{sub 2}, thereby driving the WGSR in the forward direction to enhance hydrogen production. This project aims at using a high reactivity, mesoporous calcium based sorbent (PCC-CaO) for removing CO{sub 2} using reactive separation scheme. Preliminary results have shown that PCC-CaO dominates in its performance over naturally occurring limestone towards enhanced hydrogen production. However, maintenance of high reactivity of the sorbent over several reaction-regeneration cycles warrants effective regeneration methods. We have identified sub-atmospheric calcination (vacuum) as vital regeneration technique that helps preserve the sorbent morphology. Sub-atmospheric calcination studies reveal the significance of vacuum level, diluent gas flow rate, thermal properties of diluent gas, and sorbent loading on the kinetics of calcination and the morphology of the resultant CaO sorbent. Steam, which can be easily separated from CO{sub 2}, has been envisioned as a potential diluent gas due to its better thermal properties resulting in effective heat transfer. A novel multi-fixed bed reactor was designed which isolates the catalyst bed from the sorbent bed during the calcination step. This should prevent any potential catalyst deactivation due to oxidation by CO{sub 2} during the regeneration phase.

  18. CO(2) capture properties of alkaline earth metal oxides and hydroxides: A combined density functional theory and lattice phonon dynamics study.

    PubMed

    Duan, Yuhua; Sorescu, Dan C

    2010-08-21

    By combining density functional theory and lattice phonon dynamics, the thermodynamic properties of CO(2) absorption/desorption reactions with alkaline earth metal oxides MO and hydroxides M(OH)(2) (where M=Be,Mg,Ca,Sr,Ba) are analyzed. The heats of reaction and the chemical potential changes of these solids upon CO(2) capture reactions have been calculated and used to evaluate the energy costs. Relative to CaO, a widely used system in practical applications, MgO and Mg(OH)(2) systems were found to be better candidates for CO(2) sorbent applications due to their lower operating temperatures (600-700 K). In the presence of H(2)O, MgCO(3) can be regenerated into Mg(OH)(2) at low temperatures or into MgO at high temperatures. This transition temperature depends not only on the CO(2) pressure but also on the H(2)O pressure. Based on our calculated results and by comparing with available experimental data, we propose a general computational search methodology which can be used as a general scheme for screening a large number of solids for use as CO(2) sorbents. PMID:20726653

  19. "Applications and future trends in polymer materials for green energy systems: from energy generation and storage, to CO2 capture and transportaion"

    SciTech Connect

    Zafiris, George

    2010-08-24

    Presentation describes United Technologies Research Center's recent work in green energy systems, including APRA-E project content to create a synthetic analogue of the carbonic anhydrase enzyme and incorporate it into a membrane for CO2 separation from the flue gas of a coal power plant.

  20. Device for separating CO2 from fossil-fueled power plant emissions

    DOEpatents

    Burchell, Timothy D [Oak Ridge, TN; Judkins, Roddie R [Knoxville, TN; Wilson, Kirk A [Knoxville, TN

    2002-04-23

    A gas separation device includes an inner conduit, and a concentric outer conduit. An electrically conductive filter media, preferably a carbon fiber composite molecular sieve, is provided in the annular space between the inner conduit and the outer conduit. Gas flows through the inner conduit and the annular space between the inner conduit and the outer conduit, so as to contact the filter media. The filter media preferentially adsorbs at least one constituent of the gas stream. The filter media is regenerated by causing an electric current to flow through the filter media. The inner conduit and outer conduit are preferably electrically conductive whereby the regeneration of the filter media can be electrically stimulated. The invention is particularly useful for the removal of CO.sub.2 from the exhaust gases of fossil-fueled power plants.

  1. Evaluation of handling and reuse approaches for the waste generated from MEA-based CO2 capture with the consideration of regulations in the UAE.

    PubMed

    Nurrokhmah, Laila; Mezher, Toufic; Abu-Zahra, Mohammad R M

    2013-01-01

    A waste slip-stream is generated from the reclaiming process of monoethanolamine (MEA) based Post-Combustion Capture (PCC). It mainly consists of MEA itself, ammonium, heat-stable salts (HSS), carbamate polymers, and water. In this study, the waste quantity and nature are characterized for Fluor's Econamine FGSM coal-fired CO2 capture base case. Waste management options, including reuse, recycling, treatment, and disposal, are investigated due to the need for a more environmentally sound handling. Regulations, economic potential, and associated costs are also evaluated. The technical, economic, and regulation assessment suggests waste reuse for NOx scrubbing. Moreover, a high thermal condition is deemed as an effective technique for waste destruction, leading to considerations of waste recycling into a coal burner or incineration. As a means of treatment, three secondary-biological processes covering Complete-Mix Activated Sludge (CMAS), oxidation ditch, and trickling filter are designed to meet the wastewater standards in the United Arab Emirates (UAE). From the economic point of view, the value of waste as a NOx scrubbing agent is 6,561,600-7,348,992 USD/year. The secondary-biological treatment cost is 0.017-0.02 USD/ton of CO2, while the cost of an on-site incinerator is 0.031 USD/ton of CO2 captured. In conclusion, secondary biological treatment is found to be the most economical option. PMID:24219116

  2. Enhanced Hydrogen Production Integrated with CO2 Separation in a Single-Stage Reactor

    SciTech Connect

    Mahesh Iyer; Himanshu Gupta; Danny Wong; Liang-Shih Fan

    2005-09-30

    Hydrogen production from coal gasification can be enhanced by driving the equilibrium limited Water Gas Shift reaction forward by incessantly removing the CO{sub 2} by-product via the carbonation of calcium oxide. This project aims at using the OSU patented high-reactivity mesoporous precipitated calcium carbonate sorbent for removing the CO{sub 2} product. Preliminary experiments demonstrate the show the superior performance of the PCC sorbent over other naturally occurring calcium sorbents. Gas composition analyses show the formation of 100% pure hydrogen. Novel calcination techniques could lead to smaller reactor footprint and single-stage reactors that can achieve maximum theoretical H{sub 2} production for multicyclic applications. Sub-atmospheric calcination studies reveal the effect of vacuum level, diluent gas flow rate, thermal properties of the diluent gas and the sorbent loading on the calcination kinetics which play an important role on the sorbent morphology. Steam, which can be easily separated from CO{sub 2}, is envisioned to be a potential diluent gas due to its enhanced thermal properties. Steam calcination studies at 700-850 C reveal improved sorbent morphology over regular nitrogen calcination. A mixture of 80% steam and 20% CO{sub 2} at ambient pressure was used to calcine the spent sorbent at 820 C thus lowering the calcination temperature. Regeneration of calcium sulfide to calcium carbonate was achieved by carbonating the calcium sulfide slurry by bubbling CO{sub 2} gas at room temperature.

  3. A Clear Insight into the Distinguishing CO2 Capture by Two Isostructural Dy(III)-Carboxylate Coordination Frameworks.

    PubMed

    Wang, Xi; Chen, Min; Du, Miao

    2016-07-01

    Two isostructural the-type Dy(III) coordination networks were successfully constructed based on a pair of analogous tribenzoate bridging ligands with phenyl and triazinyl central spacers. Notably, the active triazinyl group can obviously enhance the capability and selectivity of CO2 sorption for the porous framework. PMID:27331851

  4. Ultra-thin film composite mixed matrix membranes incorporating iron(III)-dopamine nanoparticles for CO2 separation.

    PubMed

    Kim, Jinguk; Fu, Qiang; Scofield, Joel M P; Kentish, Sandra E; Qiao, Greg G

    2016-04-21

    Iron dopamine nanoparticles (FeDA NPs) are incorporated into a nanoscale thick polyethylene glycol (PEG) matrix for the first time, to form ultra-thin film composite mixed matrix membranes (UTFC-MMMs) via a recently developed continuous assembly of polymers (CAP) nanotechnology. The FeDA NPs are prepared by in situ nano-complexation between Fe(3+) and DA and have a particle size that can be varied from 3 to 74 nanometers by adjusting the molar ratio of DA to Fe(3+) ion. The cross-linked selective layer with sub 100 nanometer thickness is prepared by atom transfer radical polymerisation of a mixture of PEG macrocross-linkers and FeDA NPs on top of a highly permeable poly(dimethyl siloxane) (PDMS) prelayer, which is spin-coated onto a porous polyacrylonitrile (PAN) substrate. The incorporation of the FeDA NPs within the PEG-based selective layer is confirmed by XPS analysis. The UTFC-MMMs (thickness: ∼45 nm) formed present excellent gas separation performance with a CO2 permeance of ∼1200 GPU (1 GPU = 10(-6) cm(3) (STP) cm(-2) s(-1) cmHg(-1)) and an enhanced CO2/N2 selectivity of over 35, which is the best performance for UTFC membranes in the reported literature. PMID:27035774

  5. Molten salt CO2 capture and electro-transformation (MSCC-ET) into capacitive carbon at medium temperature: effect of the electrolyte composition.

    PubMed

    Deng, Bowen; Chen, Zhigang; Gao, Muxing; Song, Yuqiao; Zheng, Kaiyuan; Tang, Juanjuan; Xiao, Wei; Mao, Xuhui; Wang, Dihua

    2016-08-15

    Electrochemical transformation of CO2 into functional materials or fuels (i.e., carbon, CO) in high temperature molten salts has been demonstrated as a promising way of carbon capture, utilisation and storage (CCUS) in recent years. In a view of continuous operation, the electrolysis process should match very well with the CO2 absorption kinetics. At the same time, in consideration of the energy efficiency, a molten salt electrochemical cell running at lower temperature is more beneficial to a process powered by the fluctuating renewable electricity from solar/wind farms. Ternary carbonates (Li : Na : K = 43.5 : 31.5 : 25.0) and binary chlorides (Li : K = 58.5 : 41.5), two typical kinds of eutectic melt with low melting points and a wide electrochemical potential window, could be the ideal supporting electrolyte for the molten salt CO2 capture and electro-transformation (MSCC-ET) process. In this work, the CO2 absorption behaviour in Li2O/CaO containing carbonates and chlorides were investigated on a home-made gas absorption testing system. The electrode processes as well as the morphology and properties of carbon obtained in different salts are compared to each other. It was found that the composition of molten salts significantly affects the absorption of CO2, electrode processes and performance of the product. Furthermore, the relationship between the absorption and electro-transformation kinetics are discussed based on the findings. PMID:27193751

  6. Apparatus for separating particles utilizing engineered acoustic contrast capture particles

    SciTech Connect

    Kaduchak, Gregory; Ward, Michael D

    2014-10-21

    An apparatus for separating particles from a medium includes a capillary defining a flow path therein that is in fluid communication with a medium source. The medium source includes engineered acoustic contrast capture particle having a predetermined acoustic contrast. The apparatus includes a vibration generator that is operable to produce at least one acoustic field within the flow path. The acoustic field produces a force potential minima for positive acoustic contrast particles and a force potential minima for negative acoustic contrast particles in the flow path and drives the engineered acoustic contrast capture particles to either the force potential minima for positive acoustic contrast particles or the force potential minima for negative acoustic contrast particles.

  7. Apparatus for separating particles utilizing engineered acoustic contrast capture particles

    DOEpatents

    Kaduchak, Gregory; Ward, Michael D.

    2011-12-27

    An apparatus for separating particles from a medium includes a capillary defining a flow path therein that is in fluid communication with a medium source. The medium source includes engineered acoustic contrast capture particle having a predetermined acoustic contrast. The apparatus includes a vibration generator that is operable to produce at least one acoustic field within the flow path. The acoustic field produces a force potential minima for positive acoustic contrast particles and a force potential minima for negative acoustic contrast particles in the flow path and drives the engineered acoustic contrast capture particles to either the force potential minima for positive acoustic contrast particles or the force potential minima for negative acoustic contrast particles.

  8. Apparatus for separating particles utilizing engineered acoustic contrast capture particles

    DOEpatents

    Kaduchak, Gregory; Ward, Michael D

    2016-05-17

    An apparatus for separating particles from a medium includes a capillary defining a flow path therein that is in fluid communication with a medium source. The medium source includes engineered acoustic contrast capture particle having a predetermined acoustic contrast. The apparatus includes a vibration generator that is operable to produce at least one acoustic field within the flow path. The acoustic field produces a force potential minima for positive acoustic contrast particles and a force potential minima for negative acoustic contrast particles in the flow path and drives the engineered acoustic contrast capture particles to either the force potential minima for positive acoustic contrast particles or the force potential minima for negative acoustic contrast particles.

  9. Total Synthesis of Acetate from CO2: Methyltetrahydrofolate, an Intermediate, and a Procedure for Separation of the Folates

    PubMed Central

    Parker, Donald J.; Wu, Tsai-Feng; Wood, Harland G.

    1971-01-01

    Whole-cell preparations of Clostridium thermoaceticum were exposed to a short pulse of 14CO2 under conditions in which double-labeled acetate was synthesized. Radioactive methyltetrahydrofolate monoglutamate, diglutamate, and triglutamates were isolated from extracts of the cells. The radioactivity was found to be exclusively in the five methyl position. The specific activities of the methyltetrahydrofolate derivatives were very high and were in accord with the proposal that methyltetrahydrofolates are the precursors of the methyl of acetate. A new method of separation of folates employing QAE-Sephadex chromatography and a linear gradient with triethylammonium bicarbonate is presented which completely resolves the common folate monoglutamates and, upon freeze-drying, yields salt-free preparations. PMID:5001869

  10. Effects of trace gas components in carbon capture and storage: geochemical experiments and simulation of laboratory-scale brine-rock-CO2-trace gas interaction

    NASA Astrophysics Data System (ADS)

    Stadler, Susanne; Nowak, Thomas; Heeschen, Katja; Riße, Andreas; Ostertag-Henning, Christian

    2010-05-01

    In the research activities on geological storage of carbon dioxide many studies mainly focus on the impact of pure CO2 gas on the storage formations. However, flue gas streams of power plants not only contain CO2, but also number of trace gases such as O2, N2, Ar, NOX, SOX, CO, H2, H2S, COS and CH4. These trace gases may not only interact with pipeline material, but can also trigger short-term and long-term changes within the subsurface storage lithology. The chemical reactivity of each of these compounds has to be evaluated and their interactions with each other have to be understood, especially since some of them are far more reactive than CO2. Within the project COORAL (= CO2 Purity for Capture and Storage) we concentrate on geochemical investigations to determine reaction pathways and kinetics of different mineral phases typical for potential German storage formations as influenced by the presence of trace gases within the flue gas stream. Quantitative measurements of these reactions are relatively well described for pure CO2 systems but are so far not well described for multi-component mixtures. We combine laboratory experiments (batch and flow-through) with numerical simulations applying the geochemical simulators PHREEQC and ChemApp, which will be coupled to GeoSys/RockFlow for coupled thermo-hydro-mechanical-chemical (THMC) process simulations. Calculations and experiments are performed for temperatures up to 200°C and pressures up to 50 MPa. The aim of the study is to determine optimal maximum concentration levels of trace gases in flue gas streams to be used in geological CO2 storage.

  11. A pyridyl-decorated MOF-505 analogue exhibiting hierarchical porosity, selective CO2 capture and catalytic capacity.

    PubMed

    Dang, Qin-Qin; Zhan, Yu-Fen; Duan, Li-Na; Zhang, Xian-Ming

    2015-12-14

    An expanded pyridyl-decorated MOF-505 analogue[Cu2(L)(H2O)2]·G(x) (H4L = 5,5'-(pyridine-2,5-diyl)diisophthalic acid, G = solvent molecule) has been solvothermally synthesized and reported. It exhibited rare hierarchical meso- and microporosity. With exposed unsaturated Cu(II) sites and Lewis basic pyridyl sites, the material shows both large CO2-uptake capacity (123.4 cm(3) g(-1) at 273 K, 1 bar) and high selectivity for CO2 over N2 (55.7) at 273 K. Furthermore, for the first time the compound has been exploited for its heterogeneous catalytic performance toward the cyanosilylation reaction under solvent-free conditions. The compound can be recycled up to five times with only a minor loss of activity. PMID:26527328

  12. EVALUATION OF SOLID SORBENTS AS A RETROFIT TECHNOLOGY FOR CO2 CAPTURE FROM COAL-FIRED POWER PLANTS

    SciTech Connect

    Holly Krutka; Sharon Sjostrom

    2011-07-31

    Through a U.S. Department of Energy (DOE) National Energy Technology Laboratory (NETL) funded cooperative agreement DE-NT0005649, ADA Environmental Solutions (ADA) has begun evaluating the use of solid sorbents for CO{sub 2} capture. The project objective was to address the viability and accelerate development of a solid-based CO{sub 2} capture technology. To meet this objective, initial evaluations of sorbents and the process/equipment were completed. First the sorbents were evaluated using a temperature swing adsorption process at the laboratory scale in a fixed-bed apparatus. A slipstream reactor designed to treat flue gas produced by coal-fired generation of nominally 1 kWe was designed and constructed, which was used to evaluate the most promising materials on a more meaningful scale using actual flue gas. In a concurrent effort, commercial-scale processes and equipment options were also evaluated for their applicability to sorbent-based CO{sub 2} capture. A cost analysis was completed that can be used to direct future technology development efforts. ADA completed an extensive sorbent screening program funded primarily through this project, DOE NETL cooperative agreement DE-NT0005649, with support from the Electric Power Research Institute (EPRI) and other industry participants. Laboratory screening tests were completed on simulated and actual flue gas using simulated flue gas and an automated fixed bed system. The following types and quantities of sorbents were evaluated: 87 supported amines; 31 carbon based materials; 6 zeolites; 7 supported carbonates (evaluated under separate funding); and 10 hydrotalcites. Sorbent evaluations were conducted to characterize materials and down-select promising candidates for further testing at the slipstream scale. More than half of the materials evaluated during this program were supported amines. Based on the laboratory screening four supported amine sorbents were selected for evaluation at the 1 kW scale at two different

  13. In situ growth of ZIF-8 nanocrystals on layered double hydroxide nanosheets for enhanced CO2 capture.

    PubMed

    Liu, Peng-Fei; Tao, Kai; Li, Guo-Chang; Wu, Meng-Ke; Zhu, Shuai-Ru; Yi, Fei-Yan; Zhao, Wen-Na; Han, Lei

    2016-08-01

    A hexagonal nanosheet LDH@ZIF-8 composite was fabricated by in situ growth of ZIF-8 on Zn-Al LDH without adding any zinc precursor, and exhibited a CO2 adsorption capacity of 1.0 mmol g(-1) at room temperature and 1 bar, which was significantly higher than that of pure Zn-Al LDH or ZIF-8, indicating a synergy between ZIF-8 and Zn-Al LDH. PMID:27356046

  14. Comprehensive Evaluation of a CO2-Capturing NOx-Free Repowering System with Utilization of Middle Pressure Steam in a Thermal Power Plant

    NASA Astrophysics Data System (ADS)

    Sik Pak, Pyong

    A CO2-capturing NOx-free H2O turbine power generation system is proposed in which middle pressure steam produced in a thermal power plant is utilized to increase generated power when demand for electricity is large. The proposed system can capture all the generated CO2 based on the oxygen combustion method and emits no NOx, so that it causes no urban and global environmental problems. A combined cycle power generation system with 200MW gas turbine power output is adopted as an example of a thermal power plant. It was assumed that 32 t/h of steam with 25kg/cm2 pressure produced at waste heat recovery boiler was utilized in the proposed system.It has been shown through simulation study that increase of power output by 11.8MW or 4.51% of the rated output is possible with no efficiency decrease. The amount of CO2 reduction is estimated to be 19600t/y.The unit cost of generated power is estimated to be 8.38yen/kWh, annual gross profit of the proposed system 271 million yen, depreciation year 4.87, and thus the proposed system is estimated to be economically feasible.

  15. Molecular Simulation Studies of Separation of CO2/N2, CO2/CH4, and CH4/N2 by ZIFs

    SciTech Connect

    Liu, Bei; Smit, Berend

    2010-05-13

    In this work, molecular simulations were performed to evaluate the separation performance of two typical zeolitic imidazolate frameworks (ZIFs), ZIF-68 and ZIF-69, for CO{sub 2}/N{sub 2}, CO{sub 2}/CH{sub 4}, and CH{sub 4}/N{sub 2} mixtures. To do this, we first identified a suitable force field for describing CO{sub 2}, N{sub 2}, and CH{sub 4} adsorption in ZIFs. On the basis of the validated force field, adsorption selectivities of the three mixtures in these ZIFs were simulated then. The results show that ZIF-69 is more beneficial for separating CO{sub 2} from CO{sub 2}-related mixtures than ZIF-68, mainly due to the presence of chlorine atoms in cbIM linkers in the former for the pressures we have considered. The overall separation performances of these two ZIFs for separating the chosen mixtures are comparable to typical MOFs and zeolites. In addition, this work demonstrates that the electrostatic interactions produced by the frameworks are very important for achieving high adsorption separation selectivities in ZIFs, and ideal adsorbed solution theory (IAST) may be applicable to ZIFs. Furthermore, the effect of water on the separation performance of the two ZIFs was also investigated.

  16. MoS2 Nanosheets Functionalized Composite Mixed Matrix Membrane for Enhanced CO2 Capture via Surface Drop-Coating Method.

    PubMed

    Shen, Yijia; Wang, Huixian; Zhang, Xiang; Zhang, Yatao

    2016-09-01

    Molybdenum disulfide (MoS2) is a graphene-like two-dimensional inorganic material, which has been used for the first time as an inorganic nanofiller to prepare a composite mixed matrix membrane to separate CO2 and N2. Polysulfone (PSf) was used as a support substrate and poly(dimethylsiloxane) (PDMS) was used as the gutter layer. The selective layer was prepared by mixing a CO2-philic copolymer Pebax 1657 with MoS2 nanosheets to enhance CO2 permeance. In addition, a simple drop-coating and evaporation method was developed to prepare the selective layer. Both permeability and selectivity of the MoS2-Pebax membrane have exceeded the pristine Pebax membrane. The permeability and selectivity reached to the maximum values of 64 Barrer and 93, respectively, at 0.15 wt % MoS2 nanosheets loadings. This result has been on the Robeson's upper bound line. The membrane also showed higher stability. The separation mechanism of the membrane is based on the well-known solution-diffusion mechanism. In addition, the stronger adsorption energy of MoS2 nanosheets to CO2 than N2 also provides the enhancement of gas selectivity. PMID:27541953

  17. Capture of metallic copper by high gradient magnetic separation system.

    PubMed

    Wu, Wan-I; Wu, Chung-Hsin; Hong, P K Andy; Lin, Cheng-Fang

    2011-10-01

    Valence copper was recovered from wastewater by chemical reduction and use of a high gradient magnetic separation (HGMS) system. Ammonia (NH3) and sodium dithionate (Na2S2O4) at a molar ratio of [Cu]:[NH3]:[Na2S2O4] = 1:4:3 at pH = 9.5 were used first to chemically reduce copper ion to metallic copper; the resultant metal solids were captured in an upflowing reactor space equipped with a permalloy matrix net under a high gradient magnetic field. The captured solids were predominantly 6-20 microm in diameter, with Cu2O and CuO present among the solids. Four treatment configurations with and without the use of magnetic field and metal alloy as the matrix net were tested and their effects evaluated: (1) no magnetic field or matrix, (2) no magnetic field but with matrix, (3) with magnetic field but no matrix, (4) with both magnetic field and matrix. At flow rates of 40, 60, 80 and 100 cm3/min, capture efficiencies for metallic copper in the absence of magnetic field were 87%, 86%, 63%, and 39%, respectively, and in the presence of magnetic field were 99%, 98%, 95%, and 93%, respectively. The HGMS was critical for a high capture efficiency, whereas a matrix net only marginally enhanced it. Additional tests with a larger reactor confirmed similarly high efficiencies of > 85%. The use of an alloy matrix appeared to be important when high flow rates are most likely to be employed in practical applications. PMID:22329132

  18. Ultra-thin film composite mixed matrix membranes incorporating iron(iii)-dopamine nanoparticles for CO2 separation

    NASA Astrophysics Data System (ADS)

    Kim, Jinguk; Fu, Qiang; Scofield, Joel M. P.; Kentish, Sandra E.; Qiao, Greg G.

    2016-04-01

    Iron dopamine nanoparticles (FeDA NPs) are incorporated into a nanoscale thick polyethylene glycol (PEG) matrix for the first time, to form ultra-thin film composite mixed matrix membranes (UTFC-MMMs) via a recently developed continuous assembly of polymers (CAP) nanotechnology. The FeDA NPs are prepared by in situ nano-complexation between Fe3+ and DA and have a particle size that can be varied from 3 to 74 nanometers by adjusting the molar ratio of DA to Fe3+ ion. The cross-linked selective layer with sub 100 nanometer thickness is prepared by atom transfer radical polymerisation of a mixture of PEG macrocross-linkers and FeDA NPs on top of a highly permeable poly(dimethyl siloxane) (PDMS) prelayer, which is spin-coated onto a porous polyacrylonitrile (PAN) substrate. The incorporation of the FeDA NPs within the PEG-based selective layer is confirmed by XPS analysis. The UTFC-MMMs (thickness: ~45 nm) formed present excellent gas separation performance with a CO2 permeance of ~1200 GPU (1 GPU = 10-6 cm3 (STP) cm-2 s-1 cmHg-1) and an enhanced CO2/N2 selectivity of over 35, which is the best performance for UTFC membranes in the reported literature.Iron dopamine nanoparticles (FeDA NPs) are incorporated into a nanoscale thick polyethylene glycol (PEG) matrix for the first time, to form ultra-thin film composite mixed matrix membranes (UTFC-MMMs) via a recently developed continuous assembly of polymers (CAP) nanotechnology. The FeDA NPs are prepared by in situ nano-complexation between Fe3+ and DA and have a particle size that can be varied from 3 to 74 nanometers by adjusting the molar ratio of DA to Fe3+ ion. The cross-linked selective layer with sub 100 nanometer thickness is prepared by atom transfer radical polymerisation of a mixture of PEG macrocross-linkers and FeDA NPs on top of a highly permeable poly(dimethyl siloxane) (PDMS) prelayer, which is spin-coated onto a porous polyacrylonitrile (PAN) substrate. The incorporation of the FeDA NPs within the PEG

  19. Human and environmental impact assessment of postcombustion CO2 capture focusing on emissions from amine-based scrubbing solvents to air.

    PubMed

    Veltman, Karin; Singh, Bhawna; Hertwich, Edgar G

    2010-02-15

    Carbon Capture and Storage (CCS) has become a key technology in climate change mitigation programs worldwide. CCS is well-studied in terms of greenhouse gas emission reduction potential and cost of implementation. Impacts on human health and the environment have, however, received considerably less attention. In this work, we present a first assessment of human health and environmental impacts of a postcombustion CO(2) capture facility, focusing on emissions from amine-based scrubbing solvents and their degradation products to air. We develop characterization factors for human toxicity for monoethanolamine (MEA) as these were not yet available. On the basis of the limited information available, our assessment indicates that amine-based scrubbing results in a 10-fold increase in toxic impact on freshwater ecosystems and a minor increase in toxic impacts on terrestrial ecosystems. These increases are attributed to emissions of monoethanolamine. For all other impact categories, i.e., human toxicity, marine ecotoxicity, particulate matter formation, photochemical oxidant formation, and terrestrial acidification, the CO(2) capture facility performs equally well to a conventional NGCC power plant, albeit substantial changes in flue gas composition. The oxidative degradation products of MEA, i.e., formaldehyde, acetaldehyde, and ammonia, do not contribute significantly to total environmental impacts. PMID:20095561

  20. The dynamic process of atmospheric water sorption in [EMIM][Ac] and mixtures of [EMIM][Ac] with biopolymers and CO2 capture in these systems.

    PubMed

    Chen, Yu; Sun, Xiaofu; Yan, Chuanyu; Cao, Yuanyuan; Mu, Tiancheng

    2014-10-01

    There are mainly three findings related to the dynamic process of atmospheric water sorption in the ionic liquid (IL) 1-ethyl-3-methlyl-imidazolium acetate ([EMIM][Ac]) and its mixtures with biopolymers (i.e., cellulose, chitin, and chitosan), and CO2 capture in these systems above. The analytical methods mainly include gravimetric hygroscopicity measurement and in situ infrared spectroscopy with the techniques of difference, derivative, deconvoluted attenuated total reflectance and two-dimensional correlation. These three findings are listed as below. (1) Pure [EMIM][Ac] only shows a two-regime pattern, while all the mixtures of [EMIM][Ac] with biopolymers (i.e., cellulose, chitin, and chitosan) present a three-regime tendency for the dynamic process of atmospheric water sorption. Specifically, the IL/chitosan mixture has a clear three-regime mode; the [EMIM][Ac]/chitin mixture has an unclear indiscernible regime 3; and the [EMIM][Ac]/cellulose mixture shows an indiscernible regime 2. (2) [EMIM][Ac] and its mixtures with biopolymers could physically absorb a trace amount of and chemically react with a much larger amount of CO2 from the air. The chemisorption capacity of CO2 in these pure and mixed systems is ordered as chitosan/[EMIM][Ac] mixture > chitin/[EMIM][Ac] mixture > cellulose/[EMIM][Ac] mixture > pure [EMIM][Ac] (ca. 0.09 mass ratio % g/g CO2/IL). (3) The CO2 solubility in [EMIM][Ac] decreases about 50% after being exposed to the atmospheric moist air for some specific time period. PMID:25208304

  1. Tuning the Physicochemical Properties of Diverse Phenolic Ionic Liquids for Equimolar CO2 Capture by the Substituent on the Anion

    SciTech Connect

    Dai, Sheng; Luo, Huimin; Yu, Bo; Li, Haoran; Wang, Congmin

    2012-01-01

    Phenolic ionic liquids for the efficient and reversible capture of CO{sub 2} were designed and prepared from phosphonium hydroxide and substituted phenols. The electron-withdrawing or electron-donating ability, position, and number of the substituents on the anion of these ionic liquids were correlated with the physicochemical properties of the ionic liquids. The results show that the stability, viscosity, and CO{sub 2}-capturing ability of these ionic liquids were significantly affected by the substituents. Furthermore, the relationship between the decomposition temperature, the CO{sub 2}-absorption capacity, and the basicity of these ionic liquids was quantitatively correlated and further rationalized by theoretical calculation. Indeed, these ionic liquids showed good stability, high absorption capacity, and low absorption enthalpy for CO{sub 2} capture. This method, which tunes the physicochemical properties by making use of substituent effects in the anion of the ionic liquid, is important for the design of highly efficient and reversible methods for CO{sub 2}-capture. This CO{sub 2} capture process using diverse phenolic ionic liquids is a promising potential method for CO{sub 2} absorption with both high absorption capacity and good reversibility.

  2. Na(+) doping induced changes in the reduction and charge transport characteristics of Al2O3-stabilized, CuO-based materials for CO2 capture.

    PubMed

    Imtiaz, Q; Abdala, P M; Kierzkowska, A M; van Beek, W; Schweiger, S; Rupp, J L M; Müller, C R

    2016-04-28

    Chemical looping combustion (CLC) and chemical looping with oxygen uncoupling (CLOU) are emerging CO2 capture technologies that could reduce appreciably the costs associated with the capture of CO2. In CLC and CLOU, the oxygen required to combust a hydrocarbon is provided by a solid oxygen carrier. Among the transition metal oxides typically considered for CLC and CLOU, copper oxide (CuO) stands out owing to its high oxygen carrying capacity, exothermic reduction reactions and fast reduction kinetics. However, the low Tammann (sintering) temperature of CuO is a serious drawback. In this context, it has been proposed to support CuO on high Tammann temperature and low cost alumina (Al2O3), thus, reducing the morphological changes occurring over multiple CLC or CLOU redox cycles and stabilizing, in turn, the high activity of CuO. However, in CuO-Al2O3 systems, phase stabilization and avoiding the formation of the CuAl2O4 spinel is key to obtaining a material with a high redox stability and activity. Here, we report a Na(+) doping strategy to phase stabilize Al2O3-supported CuO, yielding in turn an inexpensive material with a high redox stability and CO2 capture efficiency. We also demonstrate that doping CuO-Al2O3 with Na(+) improves the oxygen uncoupling characteristics and coke resistance of the oxygen carriers. Utilizing in situ and ex situ X-ray absorption spectroscopy (XAS), the local structure of Cu and the reduction pathways of CuO were determined as a function of the Na(+) content and cycle number. Finally, using 4-point conductivity measurements, we confirm that doping of Al2O3-supported CuO with Na(+) lowers the activation energy for charge transport explaining conclusively the improved redox characteristics of the new oxygen carriers developed. PMID:27080470

  3. Synthesis of Two-dimensional Microporous Carbonaceous Polymer Nanosheets and Their Application as High-performance CO2 Capture Sorbent.

    PubMed

    Zhang, Miao; Liu, Lin; He, Teng; Wu, Guotao; Chen, Ping

    2016-06-21

    The synthesis of two-dimensional (2D) polymer nanosheets with a well-defined microporous structure remains challenging in materials science. Here, a new kind of 2D microporous carbonaceous polymer nanosheets was synthesized through polymerization of a very low concentration of 1,4-dicyanobenzene in molten zinc chloride at 400-500 °C. This type of nanosheets has a thickness in the range of 3-20 nm, well-defined microporosity, a high surface area (∼537 m(2)  g(-1) ), and a large micropore volume (∼0.45 cm(3)  g(-1) ). The microporous carbonaceous polymer nanosheets exhibit superior CO2 sorption capability (8.14 wt % at 298 K and 1 bar) and a relatively high CO2 selectivity toward N2 (25.6). Starting from different aromatic nitrile monomers, a variety of 2D carbonaceous polymer nanosheets can be obtained showing a certain universality of the ionothermal method reported herein. PMID:27124013

  4. Regional Opportunities for Carbon Dioxide Capture and Storage in China: A Comprehensive CO2 Storage Cost Curve and Analysis of the Potential for Large Scale Carbon Dioxide Capture and Storage in the People’s Republic of China

    SciTech Connect

    Dahowski, Robert T.; Li, Xiaochun; Davidson, Casie L.; Wei, Ning; Dooley, James J.

    2009-12-01

    This study presents data and analysis on the potential for carbon dioxide capture and storage (CCS) technologies to deploy within China, including a survey of the CO2 source fleet and potential geologic storage capacity. The results presented here indicate that there is significant potential for CCS technologies to deploy in China at a level sufficient to deliver deep, sustained and cost-effective emissions reductions for China over the course of this century.

  5. Nanocomposites with graft copolymer-templated mesoporous MgTiO3 perovskite for CO2 capture applications.

    PubMed

    Roh, Dong Kyu; Kim, Sang Jin; Jeon, Harim; Kim, Jong Hak

    2013-07-24

    Mesoporous MgTiO3 perovskite with a high porosity and interfacial properties were synthesized via a solvothermal reaction at 150 °C for 10 h using a graft copolymer, i.e., poly(vinyl chloride)-g-poly(oxyethylene methacrylate) (PVC-g-POEM) with a well-ordered micellar morphology as a structure-directing agent. A PVC-g-POEM graft copolymer with a wormlike morphology was utilized as a soft matrix to prepare a mixed matrix membrane (MMM) with mesoporous MgTiO3 perovskite through a solution-casting method. The structure and morphology of PVC-g-POEM graft copolymer was carefully tuned by controlling polymer-solvent interactions, as characterized by transmission electron microscopy (TEM). The average pore diameter of the MgTiO3 perovskite was 10.4 nm, which is effective in facilitating gas transport via Knudsen diffusion through mesopores as well as improving interfacial contact with the organic polymer matrix. Because of a high porosity (0.56), the density of mesoporous MgTiO3 (1.75 g/cm(3)) was much lower than that of dense nonporous MgTiO3 (4 g/cm(3)) and not significantly higher than that of PVC-g-POEM (1.25 g/cm(3)), leading to a uniform distribution of MgTiO3 in MMM. The permeability of MMM with MgTiO3 was greater than those of MMM with only MgO or TiO2, indicating the simultaneous improvement of solubility and diffusivity in the former, as supported by CO2 temperature-programmed desorption (TPD) measurements. The MMM with MgTiO3 25 wt % exhibited a CO2 permeability improvement of 140% up to 138.7 Barrer (1 Barrer = 1 × 10(-10) cm(3)(STP) cm cm(-2) s(-1) cmHg(-1)) without a large loss of CO2/N2 selectivity. PMID:23777632

  6. Self-reactivated mesostructured Ca-Al-O composite for enhanced high-temperature CO2 capture and carbonation/calcination cycles performance.

    PubMed

    Chang, Po-Hsueh; Huang, Wei-Chen; Lee, Tai-Jung; Chang, Yen-Po; Chen, San-Yuan

    2015-03-25

    In this study, highly efficient high-temperature CO2 sorbents of calcium aluminate (Ca-Al-O) mesostructured composite were synthesized using presynthesized mesoporous alumina (MA) as a porous matrix to react with calcium nitrate through a microwave-assisted process. Upon annealing at 600 °C, a highly stable mesoporous structure composed of poorly crystalline Ca12Al14O33 phase and the CaO matrix was obtained. The Ca-Al-O mesostructured sorbents with a Ca(2+)/Al(3+) ratio of 5:1 exhibit an enhanced increasing CO2 absorption kinetics in the CO2 capture capacity from 37.2 wt % to 48.3 wt % without apparent degradation with increasing carbonation/calcination cycling up to 50 at 700 °C due to the strong self-reactivation effect of the mesoporous Ca-Al-O microstructure. Remarkable improvements in the CaO-CaCO3 conversion attained from the mesostructured Ca-Al-O composite can be explained using the concept combined with available mesoporous structure and Ca12Al14O33 phase content. However, a high Ca(2+)/Al(3+) =8:1 Ca-Al-O composite causes degradation because the pores become blocked and partial sintering induces CaO agglomeration. PMID:25730384

  7. Transformation of proton-conducting Perovskite-type into fluorite-type fast oxide ion electrolytes using a CO2 capture technique and their electrical properties.

    PubMed

    Trobec, Francesca; Thangadurai, Venkataraman

    2008-10-01

    Fast oxide ion conducting Ce 1- x M x O 2-delta (M = In, Sm; x = 0.1, 0.2) and Ce 0.8Sm 0.05Ca 0.15O 1.825 were prepared from the corresponding perovskite-like structured materials with nominal chemical composition of BaCe 1- x M x O 3-delta and BaCe 0.8Sm 0.05Ca 0.15O 2.825, respectively, by reacting with CO 2 at 800 degrees C for 12 h. Powder X-ray diffraction (PXRD) analysis showed the formation of fluorite-type CeO 2 and BaCO 3 just after reaction with CO 2. The amount of CO 2 gained per ceramic gram was found to be consistent with the Ba content. The CO 2 reacted samples were washed with dilute HCl and water, and the resultant solid product was characterized structurally and electrically employing various solid-state characterization methods, including PXRD, and alternating current (ac) impedance spectroscopy. The lattice constant of presently prepared Ce 1- x M x O 2-delta and Ce 0.8Sm 0.05Ca 0. 15O 1.825 by a CO 2 capture technique follows the expected ionic radii trend. For example, In-doped Ce 0.9In 0.1O 1.95 (In (3+) (VIII) = 0.92 A) sample showed a fluorite-type cell constant of 5.398(1) A, which is lower than the parent CeO 2 (5.411 A, Ce (4+) (VIII) = 0.97 A). Our attempt to prepare single-phase In-doped CeO 2 samples at 800, 1000, and 1500 degrees C using the ceramic method was unsuccessful. However, we were able to prepare single-phase Ce 0.9In 0.1O 1.95 and Ce 0.8In 0.2O 1.9 by the CO 2 capture method from the corresponding barium perovskites. The PXRD studies showed that the In-doped samples are thermodynamically unstable above 800 degrees C. The ac electrical conductivity studies using Pt electrodes showed the presence of bulk, grain-boundary, and electrode contributions over the investigated temperature range in the frequency range of 10 (-2)-10 (7) Hz. The bulk ionic conductivity and activation energy for the electrical conductivity of presently prepared Sm- and (Sm + Ca)-doped CeO 2 samples shows conductivities similar to those of materials

  8. Ca-rich Ca-Al-oxide, high-temperature-stable sorbents prepared from hydrotalcite precursors: synthesis, characterization, and CO2 capture capacity.

    PubMed

    Chang, Po-Hsueh; Chang, Yen-Po; Chen, San-Yuan; Yu, Ching-Tsung; Chyou, Yau-Pin

    2011-12-16

    We present the design and synthesis of Ca-rich Ca-Al-O oxides, with Ca(2+)/Al(3+) ratios of 1:1, 3:1, 5:1, and 7:1, which were prepared by hydrothermal decomposition of coprecipitated hydrotalcite-like Ca-Al-CO(3) precursors, for high-temperature CO(2) adsorption at 500-700 °C. In situ X-ray diffraction measurements indicate that the coprecipitated, Ca-rich, hydrotalcite-like powders with Ca(2+)/Al(3+) ratios of 5:1 and 7:1 contained Ca(OH)(2) and layered double hydroxide (LDH) phases. Upon annealing, LDH was first destroyed at approximately 200 °C to form an amorphous matrix, and then at 450-550 °C, the Ca(OH)(2) phase was converted into a CaO matrix with incorporated Al(3+) to form a homogeneous solid solution without a disrupted lattice structure. CaO nanocrystals were grown by thermal treatment of the weakly crystalline Ca-Al-O oxide matrix. Thermogravimetric analysis indicates that a CO(2) adsorption capacity of approximately 51 wt. % can be obtained from Ca-rich Ca-Al-O oxides prepared by calcination of 7:1 Ca-Al-CO(3) LDH phases at 600-700 °C. Furthermore, a relatively high CO(2) capture capability can be achieved, even with gas flows containing very low CO(2) concentrations (CO(2)/N(2) = 10 %). Approximately 95.6 % of the initial CO(2) adsorption capacity of the adsorbent is retained after 30 cycles of carbonation-calcination. TEM analysis indicates that carbonation-promoted CaCO(3) formation in the Ca-Al-O oxide matrix at 600 °C, but a subsequent desorption in N(2) at 700 °C, caused the formation CaO nanocrystals of approximately 10 nm. The CaO nanocrystals are widely distributed in the weakly crystalline Ca-Al-O oxide matrix and are present during the carbonation-calcination cycles. This demonstrates that Ca-Al-O sorbents that developed through the synthesis and calcination of Ca-rich Ca-Al LDH phases are suitable for long-term cyclic operation in severe temperature environments. PMID:22072595

  9. Ab Initio Screening of CO2-philic Groups.

    PubMed

    Tian, Ziqi; Saito, Tomonori; Jiang, De-En

    2015-04-23

    Ab initio calculations were used to identify CO2-philic groups. Over 55 neutral molecules were screened for CO2 affinity via binding energetics. It is found that poly(ethylene oxide)s (PEO) oligomers with more than three repeating units are good CO2-binding groups, consistent with the high-performance of PEO-based materials for CO2/N2 separation. More interestingly, two triazole groups linked with a methylene chain are also excellent for CO2 binding with a favorable interaction of more than 28 kJ/mol, indicating that polymers or covalent-organic frameworks (COFs) with triazoles may be utilized for CO2 capture. This work provides a useful guide to introduce promising organic groups into polymeric membranes and COFs for CO2/N2 separation media. PMID:25825811

  10. A methodology of the assessment of environmental and human health risks from amine emissions from post combustion CO2 capture technology

    NASA Astrophysics Data System (ADS)

    Korre, Anna; Manzoor, Saba; Simperler, Alexandra

    2015-04-01

    Post combustion CO2 capture (PCCC) technology in power plants using amines as solvent for CO2 capture, is one of the reduction technologies employed to combat escalating levels of CO2 in the atmosphere. However, amine solvents used for capturing CO2 produce negative emissions such as, nitrosamines and nitramines, which are suspected to be potent carcinogens. It is therefore essential to assess the atmospheric fate of these amine emissions in the atmosphere by studying their atmospheric chemistry, dispersion and transport pathways away from the source and deposition in the environment, so as to be able to assess accurately the risk posed to human health and the natural environment. An important knowledge gap until recently has been the consideration of the atmospheric chemistry of these amine emissions simultaneously with dispersion and deposition studies so as to perform reliable human health and environmental risk assessments. The authors have developed a methodology to assess the distribution of such emissions away from a post-combustion facility by studying the atmospheric chemistry of monoethanolamine, the most commonly used solvent for CO2 capture, and those of the resulting degradation amines, methylamine and dimethylamine. This was coupled with dispersion modeling calculations (Manzoor, et al., 2014; Manzoor et al,2015). Rate coefficients describing the entire atmospheric chemistry schemes of the amines studied were evaluated employing quantum chemical theoretical and kinetic modeling calculations. These coefficients were used to solve the advection-dispersion-chemical equation using an atmospheric dispersion model, ADMS 5. This methodology is applicable to any size of a power plant and at any geographical location. In this paper, the humman health risk assessment is integrated in the modelling study. The methodology is demonstrated on a case study on the UK's largest capture pilot plant, Ferrybridge CCPilot 100+, to estimate the dispersion, chemical

  11. A genome-scale metabolic model of Methanococcus maripaludis S2 for CO2 capture and conversion to methane.

    PubMed

    Goyal, Nishu; Widiastuti, Hanifah; Karimi, I A; Zhou, Zhi

    2014-05-01

    Methane is a major energy source for heating and electricity. Its production by methanogenic bacteria is widely known in nature. M. maripaludis S2 is a fully sequenced hydrogenotrophic methanogen and an excellent laboratory strain with robust genetic tools. However, a quantitative systems biology model to complement these tools is absent in the literature. To understand and enhance its methanogenesis from CO2, this work presents the first constraint-based genome-scale metabolic model (iMM518). It comprises 570 reactions, 556 distinct metabolites, and 518 genes along with gene-protein-reaction (GPR) associations, and covers 30% of open reading frames (ORFs). The model was validated using biomass growth data and experimental phenotypic studies from the literature. Its comparison with the in silico models of Methanosarcina barkeri, Methanosarcina acetivorans, and Sulfolobus solfataricus P2 shows M. maripaludis S2 to be a better organism for producing methane. Using the model, genes essential for growth were identified, and the efficacies of alternative carbon, hydrogen and nitrogen sources were studied. The model can predict the effects of reengineering M. maripaludis S2 to guide or expedite experimental efforts. PMID:24553424

  12. Micro-structural optimization of polybenzimidazole-based membranes for H2/CO2 separation at elevated temperatures

    SciTech Connect

    Singh, Rajinder P; Li, Xin; Dudeck, Kevin W; Benicewicz, Brian C; Berchtold, Kathryn A

    2012-06-12

    There is compelling need to develop novel separation methods to improve the energy efficiency of synthesis (syn) gas processing operations including H{sub 2} and H{sub 2}/CO production to meet power, chemicals, and fuel producer needs, as well as carbon capture and removal of other undesirable syngas impurities. To be technically and economically viable, a successful separation method must be applicable to industrially relevant gas streams at realistic process conditions and compatible with large gas volumes. H{sub 2} selective membrane technology is a promising method for syngas separations at elevated temperatures (>150 C) that could be positioned upstream or downstream of one or more of the water-gas-shift reactors (WGSRs) or integrated with a WGSR depending on application specific syngas processing. Polybenzimidazole (PBI)-based polymer chemistries are exceptional candidates for H{sub 2}/CO{sub 2} separations at elevated temperatures. In general, these materials possess excellent chemical resistance, very high glass transition temperatures (> 400 C), good mechanical properties, and an appropriate level of processability. Although commercially available PBI polymers have demonstrated commercially attractive H{sub 2}/CO{sub 2} selectivity, their H{sub 2} permeability is low. Our team s employing structural and chemical manipulations to tailor the polymer free-volume achitecture with the ultimate goal of enhancing H{sub 2} permselectivity while retaining the inherent hermochemical stability characteristics of PBI. We will discuss our synthetic approaches and their influences on the gas transport behavior of these PBI-based materials. In general, a decrease in H{sub 2}/CO{sub 2} selectivity was observed with an increase in H{sub 2} permeability. H{sub 2} permeability and H{sub 2}/CO{sub 2} selectivity at 250 C ranged from 50 to 1000 barrer and 5 to 45, respectively.

  13. Optimal control system design of an acid gas removal unit for an IGCC power plants with CO2 capture

    SciTech Connect

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

    2012-01-01

    Future IGCC plants with CO{sub 2} capture should be operated optimally in the face of disturbances without violating operational and environmental constraints. To achieve this goal, a systematic approach is taken in this work to design the control system of a selective, dual-stage Selexol-based acid gas removal (AGR) unit for a commercial-scale integrated gasification combined cycle (IGCC) power plant with pre-combustion CO{sub 2} capture. The control system design is performed in two stages with the objective of minimizing the auxiliary power while satisfying operational and environmental constraints in the presence of measured and unmeasured disturbances. In the first stage of the control system design, a top-down analysis is used to analyze degrees of freedom, define an operational objective, identify important disturbances and operational/environmental constraints, and select the control variables. With the degrees of freedom, the process is optimized with relation to the operational objective at nominal operation as well as under the disturbances identified. Operational and environmental constraints active at all operations are chosen as control variables. From the results of the optimization studies, self-optimizing control variables are identified for further examination. Several methods are explored in this work for the selection of these self-optimizing control variables. Modifications made to the existing methods will be discussed in this presentation. Due to the very large number of candidate sets available for control variables and due to the complexity of the underlying optimization problem, solution of this problem is computationally expensive. For reducing the computation time, parallel computing is performed using the Distributed Computing Server (DCS®) and the Parallel Computing® toolbox from Mathworks®. The second stage is a bottom-up design of the control layers used for the operation of the process. First, the regulatory control layer is

  14. Density functional theory study of the structural, electronic, lattice dynamical, and thermodynamic properties of Li4SiO4 and its capability for CO2 capture

    NASA Astrophysics Data System (ADS)

    Duan, Yuhua; Parlinski, K.

    2011-09-01

    The structural, electronic, lattice dynamical, optical, thermodynamic, and CO2 capture properties of monoclinic and triclinic phases of Li4SiO4 are investigated by combining density functional theory with phonon lattice dynamics calculations. We found that these two phases have some similarities in their bulk and thermodynamic properties. The calculated bulk modulus and the cohesive energies of these two phases are close to each other. Although both of them are insulators, the monoclinic phase of Li4SiO4 has a direct band gap of 5.24 eV while the triclinic Li4SiO4 phase has an indirect band gap of 4.98 eV. In both phases of Li4SiO4, the s orbital of O mainly contributes to the lower-energy second valence band (VB2) and the p orbitals contribute to the fist valence band (VB1) and the conduction bands (CBs). The s orbital of Si mainly contributes to the lower portions of the VB1 and VB2, and Si p orbitals mainly contribute to the higher portions of the VB1 and VB2. The s and p orbitals of Li contribute to both VBs and to CBs, and Li p orbitals have a higher contribution than the Li s orbital. There is possibly a phonon soft mode existing in triclinic γ-Li4SiO4; in the monoclinic Li4SiO4, there are three phonon soft modes, which correspond to the one type of Li disordered over a few sites. Their LO-TO splitting indicates that both phases of Li4SiO4 are polar anisotropic materials. The calculated infrared absorption spectra for LO and TO modes are different for these two phases of Li4SiO4. The calculated relationships of the chemical potential versus temperature and CO2 pressure for reaction of Li4SiO4 with CO2 shows that Li4SiO4 could be a good candidate for a high-temperature CO2 sorbent while used for postcombustion capture technology.

  15. A Facile and Low-Cost Route to Heteroatom Doped Porous Carbon Derived from Broussonetia Papyrifera Bark with Excellent Supercapacitance and CO2 Capture Performance.

    PubMed

    Wei, Tongye; Zhang, Qi; Wei, Xiaolin; Gao, Yong; Li, Huaming

    2016-01-01

    In this work, we present a facile and low-cost approach to synthesize heteroatom doped porous carbon via hydrothermal treatment of stem bark of broussonetia papyrifera (BP) as the biomass precursor in diluted sulfuric acid, and following thermal activation by KOH at 800 °C. The morphology, structure and textural property of the prepared porous carbon (PC) are investigated by scanning electron microscopy, transmission electron microscopy, N2 sorption isotherms, and X-ray photoelectron spectroscopy. The porous carbon possesses a high BET surface area of 1759 m(2) g(-1) and an average pore size of 3.11 nm as well as hetero-oxygen (9.09%) and nitrogen (1.7%) doping. Such porous carbon shows outstanding capacitive performances of 416 F g(-1) and 300 F g(-1) in three and two-electrode systems, respectively. As a solid-state adsorbent, the obtained porous carbon has an excellent CO2 adsorption capacity at ambient pressures of up to 6.71 and 4.45 mmol g(-1) at 0 and 25 °C, respectively. The results present one novel precursor-synthesis route for facile large-scale production of high performance porous carbon for a variety of great applications including energy storage and CO2 capture. PMID:26935397

  16. A Facile and Low-Cost Route to Heteroatom Doped Porous Carbon Derived from Broussonetia Papyrifera Bark with Excellent Supercapacitance and CO2 Capture Performance

    NASA Astrophysics Data System (ADS)

    Wei, Tongye; Zhang, Qi; Wei, Xiaolin; Gao, Yong; Li, Huaming

    2016-03-01

    In this work, we present a facile and low-cost approach to synthesize heteroatom doped porous carbon via hydrothermal treatment of stem bark of broussonetia papyrifera (BP) as the biomass precursor in diluted sulfuric acid, and following thermal activation by KOH at 800 °C. The morphology, structure and textural property of the prepared porous carbon (PC) are investigated by scanning electron microscopy, transmission electron microscopy, N2 sorption isotherms, and X-ray photoelectron spectroscopy. The porous carbon possesses a high BET surface area of 1759 m2 g-1 and an average pore size of 3.11 nm as well as hetero-oxygen (9.09%) and nitrogen (1.7%) doping. Such porous carbon shows outstanding capacitive performances of 416 F g-1 and 300 F g-1 in three and two-electrode systems, respectively. As a solid-state adsorbent, the obtained porous carbon has an excellent CO2 adsorption capacity at ambient pressures of up to 6.71 and 4.45 mmol g-1 at 0 and 25 °C, respectively. The results present one novel precursor-synthesis route for facile large-scale production of high performance porous carbon for a variety of great applications including energy storage and CO2 capture.

  17. A Facile and Low-Cost Route to Heteroatom Doped Porous Carbon Derived from Broussonetia Papyrifera Bark with Excellent Supercapacitance and CO2 Capture Performance

    PubMed Central

    Wei, Tongye; Zhang, Qi; Wei, Xiaolin; Gao, Yong; Li, Huaming

    2016-01-01

    In this work, we present a facile and low-cost approach to synthesize heteroatom doped porous carbon via hydrothermal treatment of stem bark of broussonetia papyrifera (BP) as the biomass precursor in diluted sulfuric acid, and following thermal activation by KOH at 800 °C. The morphology, structure and textural property of the prepared porous carbon (PC) are investigated by scanning electron microscopy, transmission electron microscopy, N2 sorption isotherms, and X-ray photoelectron spectroscopy. The porous carbon possesses a high BET surface area of 1759 m2 g−1 and an average pore size of 3.11 nm as well as hetero-oxygen (9.09%) and nitrogen (1.7%) doping. Such porous carbon shows outstanding capacitive performances of 416 F g−1 and 300 F g−1 in three and two-electrode systems, respectively. As a solid-state adsorbent, the obtained porous carbon has an excellent CO2 adsorption capacity at ambient pressures of up to 6.71 and 4.45 mmol g−1 at 0 and 25 °C, respectively. The results present one novel precursor-synthesis route for facile large-scale production of high performance porous carbon for a variety of great applications including energy storage and CO2 capture. PMID:26935397

  18. No More HF: Teflon-Assisted Ultrafast Removal of Silica to Generate High-Surface-Area Mesostructured Carbon for Enhanced CO2 Capture and Supercapacitor Performance.

    PubMed

    Singh, Dheeraj Kumar; Krishna, Katla Sai; Harish, Srinivasan; Sampath, Srinivasan; Eswaramoorthy, Muthusamy

    2016-02-01

    An innovative technique to obtain high-surface-area mesostructured carbon (2545 m(2)  g(-1)) with significant microporosity uses Teflon as the silica template removal agent. This method not only shortens synthesis time by combining silica removal and carbonization in a single step, but also assists in ultrafast removal of the template (in 10 min) with complete elimination of toxic HF usage. The obtained carbon material (JNC-1) displays excellent CO2 capture ability (ca. 26.2 wt % at 0 °C under 0.88 bar CO2 pressure), which is twice that of CMK-3 obtained by the HF etching method (13.0 wt %). JNC-1 demonstrated higher H2 adsorption capacity (2.8 wt %) compared to CMK-3 (1.2 wt %) at -196 °C under 1.0 bar H2 pressure. The bimodal pore architecture of JNC-1 led to superior supercapacitor performance, with a specific capacitance of 292 F g(-1) and 182 F g(-1) at a drain rate of 1 A g(-1) and 50 A g(-1) , respectively, in 1 m H2 SO4 compared to CMK-3 and activated carbon. PMID:26836336

  19. State estimation of an acid gas removal (AGR) plant as part of an integrated gasification combined cycle (IGCC) plant with CO2 capture

    SciTech Connect

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

    2012-01-01

    An accurate estimation of process state variables not only can increase the effectiveness and reliability of process measurement technology, but can also enhance plant efficiency, improve control system performance, and increase plant availability. Future integrated gasification combined cycle (IGCC) power plants with CO2 capture will have to satisfy stricter operational and environmental constraints. To operate the IGCC plant without violating stringent environmental emission standards requires accurate estimation of the relevant process state variables, outputs, and disturbances. Unfortunately, a number of these process variables cannot be measured at all, while some of them can be measured, but with low precision, low reliability, or low signal-to-noise ratio. As a result, accurate estimation of the process variables is of great importance to avoid the inherent difficulties associated with the inaccuracy of the data. Motivated by this, the current paper focuses on the state estimation of an acid gas removal (AGR) process as part of an IGCC plant with CO2 capture. This process has extensive heat and mass integration and therefore is very suitable for testing the efficiency of the designed estimators in the presence of complex interactions between process variables. The traditional Kalman filter (KF) (Kalman, 1960) algorithm has been used as a state estimator which resembles that of a predictor-corrector algorithm for solving numerical problems. In traditional KF implementation, good guesses for the process noise covariance matrix (Q) and the measurement noise covariance matrix (R) are required to obtain satisfactory filter performance. However, in the real world, these matrices are unknown and it is difficult to generate good guesses for them. In this paper, use of an adaptive KF will be presented that adapts Q and R at every time step of the algorithm. Results show that very accurate estimations of the desired process states, outputs or disturbances can be

  20. Influence of humic substances on Co 2+ sorption by a subsurface mineral separate and its mineralogic components

    NASA Astrophysics Data System (ADS)

    Zachara, J. M.; Resch, C. T.; Smith, S. C.

    1994-01-01

    The sorption of Co 2+ (10 -6 mol/L) was measured on subsurface mineral materials in the absence and presence of a sorbed leonardite humic acid (LHA) to (1) evaluate the sorptive role of mineral-bound humic substances, and (2) establish approaches to model metal ion binding in composite materials. The subsurface materials were a < 2.0 μm size fraction of an ultisol saprolite (CP) and this same material treated with dithionite-citrate-bicarbonate (DCB) to remove Fe-oxides (DCP). Comparable experiments (with and without LHA) were also performed with mineral sorbents representing dominant phases in the CP separate (gibbsite, Al-goethite, and kaolinite) to evaluate their potential contributions to Co sorption. The mineral-bound LHA ranged in concentration between 0.1-0.4 mg-C/m 2, representing approximately 0.7% of the subsurface isolate by mass. The sorption-desorption of LHA on the mineral surfaces, and its affinity for Co as a aqueous phase complexant were also determined. Batch measurements were employed (sorbents at 20-90 m 2/L; LHA-DOC at ≈11 mg-C/L) over a range in pH and ionic strength ( I) at I = 0.01 and 0.1 in NaClO 4. The LHA strongly sorbed to the subsurface mineral isolates (CP and DCP), and to all the specimen sorbents except kaolinite. Maximum sorption of LHA occurred at lower pH (≈4.5). In solid-free suspensions, the affinity of LHA for Co increased with pH and decreasing I ( Kd ranging 20-450 L/g). Mineral-bound LHA increased Co sorption on all the sorbents by factors of 10-60 %, with the greatest augmentation noted at pH values (4.5-6.5) where (1) maximum LHA sorption occurred, and (2) Co sorption to the mineral phase was weak and dominated by ion exchange. The LHA appeared simply to augment, rather than to change the intrinsic adsorption behavior of the mineral sorbents. Accordingly, predictions of the Kd for Co on the LHA-coated subsurface materials (DCP, CP) based on a linear additivity model agreed well with the experimental data, suggesting

  1. Experimental investigation of the permeability and selectivity of supported ionic liquid membranes for CO2/He separation at temperatures up to 125° C

    SciTech Connect

    Ilconich, J.B.; Myers, C.R.; Pennline, H.W.; Luebke, D.R.

    2007-07-01

    Supported liquid membranes have been prepared by impregnation of commercial porous polymer films with the ionic liquid 1-n-hexyl-3- methylimidazolium bis(trifluoromethanesulfonyl)imide. The ionic liquid has been characterized, and the membranes have been tested to determine performance in the selective separation of CO2 from He. Experiments were conducted in a constant pressure system, and pure gas permeability/selectivity data are reported. Membranes prepared with polysulfone supports have been found to be stable to 125 °C. The CO2 permeability of the membranes increases from 744 to 1200 barrer as the temperature increases from 37 to 125 °C. The CO2/He selectivity decreased from 8.7 to 3.1 over the same temperature range.

  2. Metal–organic framework based mixed matrix membranes: a solution for highly efficient CO2 capture?† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c4cs00437j Click here for additional data file.

    PubMed Central

    Seoane, Beatriz; Coronas, Joaquin; Gascon, Ignacio; Benavides, Miren Etxeberria; Karvan, Oğuz; Caro, Jürgen; Kapteijn, Freek

    2015-01-01

    The field of metal–organic framework based mixed matrix membranes (M4s) is critically reviewed, with special emphasis on their application in CO2 capture during energy generation. After introducing the most relevant parameters affecting membrane performance, we define targets in terms of selectivity and productivity based on existing literature on process design for pre- and post-combustion CO2 capture. Subsequently, the state of the art in M4s is reviewed against these targets. Because final application of these membranes will only be possible if thin separation layers can be produced, the latest advances in the manufacture of M4 hollow fibers are discussed. Finally, the recent efforts in understanding the separation performance of these complex composite materials and future research directions are outlined. PMID:25692487

  3. Modeling of mass transfer of Phospholipids in separation process with supercritical CO2 fluid by RBF artificial neural networks

    Technology Transfer Automated Retrieval System (TEKTRAN)

    An artificial Radial Basis Function (RBF) neural network model was developed for the prediction of mass transfer of the phospholipids from canola meal in supercritical CO2 fluid. The RBF kind of artificial neural networks (ANN) with orthogonal least squares (OLS) learning algorithm were used for mod...

  4. Modeling and optimization of a modified claus process as part of an integrted gasification combined cycle (IGCC) power plant with CO2 capture

    SciTech Connect

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

    2011-01-01

    The modified Claus process is one of the most common technologies for sulfur recovery from acid gas streams. Important design criteria for the Claus unit, when part of an Integrated Gasification Combined Cycle (IGCC) power plant, are the ability to destroy ammonia completely and recover sulfur thoroughly from a relatively low purity acid gas stream without sacrificing flame stability. Due to these criteria, modifications are often required to the conventional process, resulting in a modified Claus process. For the studies discussed here, these modifications include the use of a 95% pure oxygen stream as the oxidant, a split flow configuration, and the preheating of the feeds with the intermediate pressure steam generated in the waste heat boiler (WHB). In the future, for IGCC plants with CO2 capture, the Claus unit must satisfy emission standards without sacrificing the plant efficiency in the face of typical disturbances of an IGCC plant such as rapid change in the feed flowrates due to load-following and wide changes in the feed composition because of changes in the coal feed to the gasifier. The Claus unit should be adequately designed and efficiently operated to satisfy these objectives. Even though the Claus process has been commercialized for decades, most papers concerned with the modeling of the Claus process treat the key reactions as equilibrium reactions. Such models are validated by manipulating the temperature approach to equilibrium for a set of steady-state operating data, but are of limited use for dynamic studies. One of the objectives of this study is to develop a model that can be used for dynamic studies. In a Claus process, especially in the furnace and the WHB, many reactions may take place. In this work, a set of linearly independent reactions has been identified and kinetic models of the furnace flame and anoxic zones, WHB, and catalytic reactors have been developed. To facilitate the modeling of the Claus furnace, a four-stage method was

  5. ARTICLES: Isotope separation by multiphoton dissociation of molecules using high-power CO2 laser radiation. Scaling of the process for carbon isotopes

    NASA Astrophysics Data System (ADS)

    Abdushelishvili, G. I.; Avatkov, O. N.; Bagratashvili, Viktor N.; Baranov, V. Yu; Bakhtadze, A. B.; Velikhov, E. P.; Vetsko, V. M.; Gverdtsiteli, I. G.; Dolzhikov, V. S.; Esadze, G. G.; Kazakov, S. A.; Kolomiĭskiĭ, Yu R.; Letokhov, V. S.; Pigul'skiĭ, S. V.; Pis'mennyĭ, V. D.; Ryabov, Evgenii A.; Tkeshelashvili, G. I.

    1982-04-01

    Data are presented on multiphoton dissociation of halogenated methanes, CF3I and CF3Br, in a pulsed CO2 laser field in the single-pulse irradiation regime. It is shown that the high parameters of an elementary separation event (dissociation yield and selectivity, quantum efficiency) for these molecules can be used to achieve efficient laser separation of the carbon isotopes 12C and 13C. An analysis is made of problems involved in organizing the chemical cycle when the process is scaled up. A description is given of an apparatus for scaled-up laser isotope separation, including a pulse-periodic CO2 laser with a kilowatt average power, and a laser separation cell. Experiments carried out using this apparatus showed that the high parameters obtained in the single-pulse regime can also be achieved using this design and a yield rate comparable with that of traditional separation systems can be achieved for fairly low energy losses. These results make it possible to develop a commercial system for laser isotope separation using multiphoton dissociation of molecules.

  6. Buoyant dispersal of CO2 during geological storage

    NASA Astrophysics Data System (ADS)

    Hesse, M. A.; Woods, A. W.

    2010-01-01

    Carbon capture and storage is currently the only technology that may allow significant reductions in CO2 emissions from large point sources. Seismic images of geological CO2 storage show the rise of CO2 is influenced by horizontal shales. The buoyant CO2 spreads beneath impermeable barriers until a gap allows its upward migration. The large number and small scale of these barriers makes the prediction of the CO2 migration path and hence the magnitude of CO2 trapping very challenging. We show that steady buoyancy dominated flows in complex geometries can be modeled as a cascade of flux partitioning events. This approach allows the analysis of two-dimensional plume dispersal from a horizontal injection well. We show that the plume spreads laterally with height y above the source according to (y/h)1/2 L, where L is the width of the shales and h is their vertical separation. The fluid volume below successive shale layers, and therefore the magnitude of trapped CO2, increase as (y/h)5/4 above the source, so that every additional layer of barriers traps more CO2 than the one below. Upscaling small scale flow barriers by reducing the vertical permeability, common in numerical simulations of CO2 storage, does not capture the dispersion and trapping of the CO2 plume by the flow barriers.

  7. System-level modeling for geological storage of CO2

    SciTech Connect

    Zhang, Yingqi; Oldenburg, Curtis M.; Finsterle, Stefan; Bodvarsson, Gudmundur S.

    2006-04-24

    One way to reduce the effects of anthropogenic greenhousegases on climate is to inject carbon dioxide (CO2) from industrialsources into deep geological formations such as brine formations ordepleted oil or gas reservoirs. Research has and is being conducted toimprove understanding of factors affecting particular aspects ofgeological CO2 storage, such as performance, capacity, and health, safetyand environmental (HSE) issues, as well as to lower the cost of CO2capture and related processes. However, there has been less emphasis todate on system-level analyses of geological CO2 storage that considergeological, economic, and environmental issues by linking detailedrepresentations of engineering components and associated economic models.The objective of this study is to develop a system-level model forgeological CO2 storage, including CO2 capture and separation,compression, pipeline transportation to the storage site, and CO2injection. Within our system model we are incorporating detailedreservoir simulations of CO2 injection and potential leakage withassociated HSE effects. The platform of the system-level modelingisGoldSim [GoldSim, 2006]. The application of the system model is focusedon evaluating the feasibility of carbon sequestration with enhanced gasrecovery (CSEGR) in the Rio Vista region of California. The reservoirsimulations are performed using a special module of the TOUGH2 simulator,EOS7C, for multicomponent gas mixtures of methane and CO2 or methane andnitrogen. Using this approach, the economic benefits of enhanced gasrecovery can be directly weighed against the costs, risks, and benefitsof CO2 injection.

  8. Large-Scale Utilization of Biomass Energy and Carbon Dioxide Capture and Storage in the Transport and Electricity Sectors under Stringent CO2 Concentration Limit Scenarios

    SciTech Connect

    Luckow, Patrick; Wise, Marshall A.; Dooley, James J.; Kim, Son H.

    2010-08-05

    This paper examines the potential role of large scale, dedicated commercial biomass energy systems under global climate policies designed to meet atmospheric concentrations of CO2 at 400ppm and 450ppm by the end of the century. We use an integrated assessment model of energy and agriculture systems to show that, given a climate policy in which terrestrial carbon is appropriately valued equally with carbon emitted from the energy system, biomass energy has the potential to be a major component of achieving these low concentration targets. A key aspect of the research presented here is that the costs of processing and transporting biomass energy at much larger scales than current experience are explicitly incorporated into the modeling. From the scenario results, 120-160 EJ/year of biomass energy is produced globally by midcentury and 200-250 EJ/year by the end of this century. In the first half of the century, much of this biomass is from agricultural and forest residues, but after 2050 dedicated cellulosic biomass crops become the majority source, along with growing utilization of waste-to-energy. The ability to draw on a diverse set of biomass based feedstocks helps to reduce the pressure for drastic large-scale changes in land use and the attendant environmental, ecological, and economic consequences those changes would unleash. In terms of the conversion of bioenergy feedstocks into value added energy, this paper demonstrates that biomass is and will continue to be used to generate electricity as well as liquid transportation fuels. A particular focus of this paper is to show how climate policies and technology assumptions - especially the availability of carbon dioxide capture and storage (CCS) technologies - affect the decisions made about where the biomass is used in the energy system. The potential for net-negative electric sector emissions through the use of CCS with biomass feedstocks provides an attractive part of the solution for meeting stringent

  9. Coal-fuelled systems for peaking power with 100% CO2 capture through integration of solid oxide fuel cells with compressed air energy storage

    NASA Astrophysics Data System (ADS)

    Nease, Jake; Adams, Thomas A.

    2014-04-01

    In this study, a coal-fuelled integrated solid oxide fuel cell (SOFC) and compressed air energy storage (CAES) system in a load-following power production scenario is discussed. Sixteen SOFC-based plants with optional carbon capture and sequestration (CCS) and syngas shifting steps are simulated and compared to a state-of-the-art supercritical pulverised coal (SCPC) plant. Simulations are performed using a combination of MATLAB and Aspen Plus v7.3. It was found that adding CAES to a SOFC-based plant can provide load-following capabilities with relatively small effects on efficiencies (1-2% HHV depending on the system configuration) and levelized costs of electricity (∼0.35 ¢ kW-1 h-1). The load-following capabilities, as measured by least-squares metrics, show that this system may utilize coal and achieve excellent load-tracking that is not adversely affected by the inclusion of CCS. Adding CCS to the SOFC/CAES system reduces measurable direct CO2 emission to zero. A seasonal partial plant shutdown schedule is found to reduce fuel consumption by 9.5% while allowing for cleaning and maintenance windows for the SOFC stacks without significantly affecting the performance of the system (∼1% HHV reduction in efficiency). The SOFC-based systems with CCS are found to become economically attractive relative to SCPC above carbon taxes of 22 ton-1.

  10. Physically Gelled Room-Temperature Ionic Liquid-Based Composite Membranes for CO2/N-2 Separation: Effect of Composition and Thickness on Membrane Properties and Performance

    SciTech Connect

    Nguyen, PT; Voss, BA; Wiesenauer, EF; Gin, DL; Nobe, RD

    2013-07-03

    An aspartame-based, low molecular-weight organic gelator (LMOG) was used to form melt-infused and composite membranes with two different imidazolium-based room-temperature ionic liquids (RTILs) for CO2 separation from N-2. Previous work demonstrated that LMOGs can gel RTILs at low, loading levels, and this aspartame-based LMOG was selected because it has been reported to gel a large number of RTILs. The imidazolium-based RTILs were used because of their inherent good properties for CO2/light gas separations. Analysis of the resulting bulk RTIL/LMOG physical gels showed that these materials have high sol-gel transition temperatures (ca. 135 degrees C) suitable for flue gas applications. Gas permeabilities and burst pressure measurements of thick, melt infused membranes revealed a trade-off between high CO2 permeabilities and good mechanical stability as a function of the LMOG loading. Defect-free, composite membranes of the gelled RTILs were successfully fabricated by choosing an appropriate porous membrane support (hydrophobic PTFE) using a suitable coating technique (roller coating). The thicknesses of the applied composite gel layers ranged from 10.3 to 20.7 mu m, which represents an order of magnitude decrease in active layer thickness, compared to the original melt-infused gel RTIL membranes.

  11. Investigation of Ester- and Amide-Linker-Based Porous Organic Polymers for Carbon Dioxide Capture and Separation at Wide Temperatures and Pressures.

    PubMed

    Ullah, Ruh; Atilhan, Mert; Anaya, Baraa; Al-Muhtaseb, Shaheen; Aparicio, Santiago; Patel, Hasmukh; Thirion, Damien; Yavuz, Cafer T

    2016-08-17

    further exploration as efficient and cheaply available solid sorbent material for CO2 capture and separation. PMID:27458732

  12. Supported Ionic Liquid Membranes and Ion-Jelly® Membranes with [BMIM][DCA]: Comparison of Its Performance for CO2 Separation

    PubMed Central

    Couto, Ricardo; Neves, Luísa; Simões, Pedro; Coelhoso, Isabel

    2015-01-01

    In this work, a supported ionic liquid membrane (SILM) was prepared by impregnating a PVDF membrane with 1-butyl-3-methylimidazolium dicyanamide ([BMIM][DCA]) ionic liquid. This membrane was tested for its permeability to pure gases (CO2, N2 and O2) and ideal selectivities were calculated. The SILM performance was also compared to that of Ion-Jelly® membranes, a new type of gelled membranes developed recently. It was found that the PVDF membrane presents permeabilities for pure gases similar or lower to those presented by the Ion-Jelly® membranes, but with increased ideal selectivities. This membrane presents also the highest ideal selectivity (73) for the separation of CO2 from N2 when compared with SILMs using the same PVDF support but with different ionic liquids. PMID:25594165

  13. Sequestering CO2 in the Ocean: Options and Consequences

    NASA Astrophysics Data System (ADS)

    Rau, G. H.; Caldeira, K.

    2002-12-01

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

  14. Enhanced Performance of Polyurethane Hybrid Membranes for CO2 Separation by Incorporating Graphene Oxide: The Relationship between Membrane Performance and Morphology of Graphene Oxide.

    PubMed

    Wang, Ting; Zhao, Li; Shen, Jiang-nan; Wu, Li-guang; Van der Bruggen, Bart

    2015-07-01

    Polyurethane hybrid membranes containing graphene oxide (GO) with different morphologies were prepared by in situ polymerization. The separation of CO2/N2 gas mixtures was studied using these novel membranes. The results from the morphology characterization of GO samples indicated that the oxidation process in the improved Hummers method introduced oxygenated functional groups into graphite, making graphite powder exfoliate into GO nanosheets. The surface defects on the GO sheets increased when oxidation increased due to the introduction of more oxygenated functional groups. Both the increase in oxygenated functional groups on the GO surface and the decrease in the number of GO layers leads to a better distribution of GO in the polymer matrix, increasing thermal stability and gas separation performance of membranes. The addition of excess oxidant destroyed the structure of GO sheets and forms structural defects, which depressed the separation performance of membranes. The hybrid membranes containing well-distributed GO showed higher permeability and permeability selectivity for the CO2. The formation of GO aggregates in the hybrid membranes depressed the membrane performance at a high content of GO. PMID:26024066

  15. Flowsheet calculation of a combined heat and power fuel cell plant with a conceptual molten carbonate fuel cell with separate CO 2 supply

    NASA Astrophysics Data System (ADS)

    Au, S. F.; Hemmes, K.; Woudstra, N.

    A new type of MCFC with a separate CO 2 supply (improved or i-MCFC) is previously presented, which has the potential for reducing NiO cathode dissolution and system enhancement by CO 2 removal from fuel gas. This article presents the first flowsheet calculations of an i-MCFC system that utilizes the potential of reducing NiO dissolution. A submodel that simulates energy and massflows of the i-MCFC is built using standard flowsheeting components. The performance of the i-MCFC is assumed to be equal to the MCFC and differences in Nernst potentials and irreversible losses are neglected. To compare the differences in concept, a MCFC combined heat and power (CHP) system flowsheet is modified and the MCFC model substituted by the i-MCFC submodel. The overall efficiencies of both fuel cell systems are calculated using a flowsheeting program. The calculated results are compared and the differences analyzed. The overall system performance of this i-MCFC CHP system is slightly lower than the MCFC CHP reference system (about 0.1% point in average). The difference in performance is ascribed to the change in gas composition and heat capacity of the cathode gas. The change in heat capacity increases the total massflow through the i-MCFC resulting to an increase in overall auxiliary power consumption. The low CO 2 content of the cathode gas should reduce the NiO cathode dissolution to a negligible level.

  16. Mesoporous carbon originated from non-permanent porous MOFs for gas storage and CO2/CH4 separation

    PubMed Central

    Wang, Wenjing; Yuan, Daqiang

    2014-01-01

    Four nanoporous carbons prepared by direct carbonization of non-permanent highly porous MOF [Zn3(BTC)2·(H2O)3]n without any additional carbon precursors. The carbonization temperature plays an important role in the pore structures of the resultant carbons. The Brunauer-Emmett-Teller (BET) surface areas of four carbon materials vary from 464 to 1671 m2 g−1 for different carbonization temperature. All the four carbon materials showed a mesoporous structure centered at ca. 3 nm, high surface area and good physicochemical stability. Hydrogen, methane and carbon dioxide sorption measurements indicated that the C1000 has good gas uptake capabilities. The excess H2 uptake at 77 K and 17.9 bar can reach 32.9 mg g−1 and the total uptake is high to 45 mg g−1. Meanwhile, at 95 bar, the total CH4 uptake can reach as high as 208 mg g−1. Moreover the ideal adsorbed solution theory (IAST) prediction exhibited exceptionally high adsorption selectivity for CO2/CH4 in an equimolar mixture at 298 K and 1 bar (Sads = 27) which is significantly higher than that of some porous materials in the similar condition. PMID:25026895

  17. A comparison of cellulosic fuel yields and separated soil-surface CO2 fluxes in maize and prairie biofuel cropping systems

    NASA Astrophysics Data System (ADS)

    Nichols, Virginia A.

    It has been suggested that strategic incorporation of perennial vegetation into agricultural landscapes could provide ecosystem services while maintaining agricultural productivity. To evaluate potential use of prairie as a Midwestern cellulosic feedstock, we investigated theoretical cellulosic fuel yields, as well as soil-surface carbon dioxide emissions of prairie-based biofuel systems as compared to maize-based systems on fertile soils in Boone County, IA, USA. Investigated systems were: a maize-soybean rotation grown for grain only, continuous maize grown for grain and stover both with and without a winter rye cover crop, and a 31-species reconstructed prairie grown with and without spring nitrogen fertilization for fall-harvested biomass. From 2009-2013, the highest producing system was N-fertilized prairie, averaging 10.4 Mg ha -1 yr-1 above-ground biomass with average harvest removals of 7.8 Mg ha-1 yr-1. The unfertilized prairie produced 7.4 Mg ha-1 yr-1, averaging harvests of 5.3 Mg ha-1 yr-1. Lowest cellulosic biomass harvests were realized from continuous maize systems, averaging 3.5 Mg ha -1 yr-1 when grown with, and 3.7 Mg ha-1 yr-1 when grown without a winter rye cover crop, respectively. Un-fertilized prairie biomass and maize stover had equivalent dietary conversion ratios at 330 g ethanol kg-1 dry biomass, but N-fertilized prairie was lower at 315. Over four years prairie systems averaged 1287 L cellulosic ethanol ha-1 yr-1 more than maize systems, with fertilization increasing prairie ethanol production by 865 L ha-1 yr-1. Harvested biomass accounted for >90% of ethanol yield variation. A major hurdle in carbon cycling studies is the separation of the soil-surface CO2 flux into its respective components. From 2012-2013 we used a shading method to separate soil-surface CO2 resulting from oxidation of soil organic matter and CO2 derived from live-root activity in three systems: unfertilized prairie, N-fertilized prairie, and continuous maize

  18. Application of a high-throughput analyzer in evaluating solid adsorbents for post-combustion carbon capture via multicomponent adsorption of CO2, N2, and H2O.

    PubMed

    Mason, Jarad A; McDonald, Thomas M; Bae, Tae-Hyun; Bachman, Jonathan E; Sumida, Kenji; Dutton, Justin J; Kaye, Steven S; Long, Jeffrey R

    2015-04-15

    Despite the large number of metal-organic frameworks that have been studied in the context of post-combustion carbon capture, adsorption equilibria of gas mixtures including CO2, N2, and H2O, which are the three biggest components of the flue gas emanating from a coal- or natural gas-fired power plant, have never been reported. Here, we disclose the design and validation of a high-throughput multicomponent adsorption instrument that can measure equilibrium adsorption isotherms for mixtures of gases at conditions that are representative of an actual flue gas from a power plant. This instrument is used to study 15 different metal-organic frameworks, zeolites, mesoporous silicas, and activated carbons representative of the broad range of solid adsorbents that have received attention for CO2 capture. While the multicomponent results presented in this work provide many interesting fundamental insights, only adsorbents functionalized with alkylamines are shown to have any significant CO2 capacity in the presence of N2 and H2O at equilibrium partial pressures similar to those expected in a carbon capture process. Most significantly, the amine-appended metal organic framework mmen-Mg2(dobpdc) (mmen = N,N'-dimethylethylenediamine, dobpdc (4-) = 4,4'-dioxido-3,3'-biphenyldicarboxylate) exhibits a record CO2 capacity of 4.2 ± 0.2 mmol/g (16 wt %) at 0.1 bar and 40 °C in the presence of a high partial pressure of H2O. PMID:25844924

  19. Application of a High-Throughput Analyzer in Evaluating Solid Adsorbents for Post-Combustion Carbon Capture via Multicomponent Adsorption of CO2, N-2, and H2O

    SciTech Connect

    Mason, JA; McDonald, TM; Bae, TH; Bachman, JE; Sumida, K; Dutton, JJ; Kaye, SS; Long, JR

    2015-04-15

    Despite the large number of metal-organic frameworks that have been studied in the context of post-combustion carbon capture, adsorption equilibria of gas mixtures including CO2, N-2, and H2O, which are the three biggest components of the flue gas emanating from a coal- or natural gas-fired power plant, have never been reported. Here, we disclose the design and validation of a high-throughput multicomponent adsorption instrument that can measure equilibrium adsorption isotherms for mixtures of gases at conditions that are representative of an actual flue gas from a power plant. This instrument is used to study 15 different metal-organic frameworks, zeolites, mesoporous silicas, and activated carbons representative of the broad range of solid adsorbents that have received attention for CO2 capture. While the multicomponent results presented in this work provide many interesting fundamental insights, only adsorbents functionalized with alkylamines are shown to have any significant CO2 capacity in the presence of N-2 and H2O at equilibrium partial pressures similar to those expected in a carbon capture process. Most significantly, the amine-appended metal organic framework mmen-Mg-2(dobpdc) (mmen = N,N'-dimethylethylenediamine, dobpdc (4-) = 4,4'-dioxido-3,3'-biphenyldicarboxylate) exhibits a record CO2 capacity of 4.2 +/- 0.2 mmol/g (16 wt %) at 0.1 bar and 40 degrees C in the presence of a high partial pressure of H2O.

  20. Functional Arrays for Light Energy Capture and Charge Separation.

    PubMed

    Flamigni, Lucia

    2016-06-01

    This article draws, with a simplified but rigorous approach, the typical procedure for the design and optimization of functional multicomponent structures for light to chemical energy conversion for two series of multipartite structures based on prototypical chromophores: polypyridyl metal complexes and porphyrinoids. Starting from a photophysical study performed by steady-state and time-resolved spectroscopic methods, the full deactivation dynamics of the light-absorbing chromophore(s) are disclosed. The preferred deactivation step (electron transfer in this case) is then optimized. This can be done by simply operating on the solvent, but also by changing structure/components that can alter electronic and nuclear factors, via continuous feedback with the research groups in charge of the synthesis. With a presentation suitable for a wide audience, it is here discussed how the effective design of functional multicomponent structures for charge separation can be achieved. PMID:27027981

  1. Co2 geological sequestration

    SciTech Connect

    Xu, Tianfu

    2004-11-18

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

  2. Final Report for Fractionation and Separation of Polydisperse Nanoparticles into Distinct Monodisperse Fractions Using CO2 Expanded Liquids

    SciTech Connect

    Chistopher Roberts

    2007-08-31

    The overall objective of this project was to facilitate efficient fractionation and separation of polydisperse metal nanoparticle populations into distinct monodisperse fractions using the tunable solvent properties of gas expanded liquids. Specifically, the dispersibility of ligand-stabilized nanoparticles in an organic solution was controlled by altering the ligand-solvent interaction (solvation) by the addition of carbon dioxide (CO{sub 2}) gas as an antisolvent (thereby tailoring the bulk solvent strength) in a custom high pressure apparatus developed in our lab. This was accomplished by adjusting the CO{sub 2} pressure over the liquid dispersion, resulting in a simple means of tuning the nanoparticle precipitation by size. Overall, this work utilized the highly tunable solvent properties of organic/CO{sub 2} solvent mixtures to selectively size-separate dispersions of polydisperse nanoparticles (ranging from 1 to 20 nm in size) into monodisperse fractions ({+-}1nm). Specifically, three primary tasks were performed to meet the overall objective. Task 1 involved the investigation of the effects of various operating parameters (such as temperature, pressure, ligand length and ligand type) on the efficiency of separation and fractionation of Ag nanoparticles. In addition, a thermodynamic interaction energy model was developed to predict the dispersibility of different sized nanoparticles in the gas expanded liquids at various conditions. Task 2 involved the extension of the experimental procedures identified in task 1 to the separation of other metal particles used in catalysis such as Au as well as other materials such as semiconductor particles (e.g. CdSe). Task 3 involved using the optimal conditions identified in tasks 1 and 2 to scale up the process to handle sample sizes of greater than 1 g. An experimental system was designed to allow nanoparticles of increasingly smaller sizes to be precipitated sequentially in a vertical series of high pressure vessels by

  3. Enhancing the carbon capture capacities of a rigid ultra-microporous MOF through gate-opening at low CO2 pressures assisted by swiveling oxalate pillars.

    PubMed

    Banerjee, Aparna; Nandi, Shyamapada; Nasa, Parveen; Vaidhyanathan, Ramanathan

    2016-01-31

    Porosity enhancement assisted by an unusual gate opening has been realized in an exceptionally rigid ultra-microporous framework. The gate-opening has been attributed to the presence of symmetrically positioned Zn-O bonds of the Zn-oxalate units that facilitate subtle swiveling motion resulting in a drastic improvement (42%) in the CO2 capacity without compromising the CO2/N2 selectivity. PMID:26671348

  4. Fuel age impacts on gaseous fission product capture during separations

    SciTech Connect

    Jubin, Robert T.; Soelberg, Nicolas R.; Strachan, Denis M.; Ilas, G.

    2012-09-21

    relatively short half-lives, 12.3 y and 10.7 y, respectively, the dose decreases with the time from when the fuel is removed from the reactor to the time it is processed (herein “fuel age”). One possible strategy for limiting the discharges of these short halflife radionuclides is to allow the fuel to age to take advantage of radioactive decay. Therefore, the doses and required DFs are calculated as a function of fuel age. Here we calculate, given the above constraints and assumptions, the minimum ages for each fuel type that would not require additional effluent controls for the shorter half-life volatile radionuclides based on dose considerations. With respect to 129I doses, we find that the highest dose is calculated with iodine as a fine particulate. The dose scales as the fraction of the total 129I that is particulate. Therefore, we assume for all of our calculations that 100% of the 129I is particulate and allow the user of the results given here to scale our calculated doses to their needs. To summarize the data given in the body and appendices of this report, we find that the principal isotopes of concern are 3H and 129I, the latter requiring the highest DFs. The maximum DF value for 129I is 8000 for the illustrated cases. The required DF for 3H could be as high as 720, depending on the age of the fuel processed. The DF for 85Kr could be up to ~60, depending on fuel age. The DF for 14C is in many cases 1 (no treatment required) but could be as high as 30. The DFs required are within the range of DFs that are reported for the capture technologies that are available for the volatile radionuclides. Achieving the required 129I and 3H DFs is more challenging. Variations in stack design and other design factors may also significantly impact the DF requirements.

  5. Development and performance evaluation of Polydimethyl siloxane/Polysulfone (PDMS/PSF) composite membrane for CO2/CH4 separation

    NASA Astrophysics Data System (ADS)

    Suleman, M. S.; Lau, K. K.; Yeong, Y. F.

    2016-06-01

    Asymmetric polysulfone (PSF) membrane was developed by phase inversion in this study. Polysulfone (PSF) membrane was modified to develop a composite polymeric membrane. Polydimethyl siloxane (PDMS) was used to modify the PSF membrane. PDMS/PSF composite membrane was developed by dip coating of PDMS over PSF. Developed membranes were characterized in terms of membrane morphology by scanning electron microscope (SEM). Micro structure of polysulfone (PSF) membrane confirmed that developed membrane was asymmetric. Dense PDMS coating in microstructure of composite membrane was observed. Membrane swelling experiments were performed by immersing developed membranes in water for specific time period. PDMS/PSF composite membrane resisted water swelling as compared to PSF membrane. Performance of the membrane was evaluated before and after swelling within the pressure range of 2-10 bar. Reasonable decrement in permeance and selectivity was observed after membrane swelling. Thus, membrane swelling affected the separation performance of both PSF and PDMS/PSF composite membrane by decreasing the permeance and selectivity values.

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

    PubMed

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

    2016-02-01

    Capture and utilization of CO2 as alternative carbon feedstock for fuels, chemicals, and materials aims at reducing greenhouse gas emissions and fossil resource use. For capture of CO2, a large variety of CO2 sources exists. Since they emit much more CO2 than the expected demand for CO2 utilization, the environmentally most favorable CO2 sources should be selected. For this purpose, we introduce the environmental-merit-order (EMO) curve to rank CO2 sources according to their environmental impacts over the available CO2 supply. To determine the environmental impacts of CO2 capture, compression and transport, we conducted a comprehensive literature study for the energy demands of CO2 supply, and constructed a database for CO2 sources in Europe. Mapping these CO2 sources reveals that CO2 transport distances are usually small. Thus, neglecting transport in a first step, we find that environmental impacts are minimized by capturing CO2 first from chemical plants and natural gas processing, then from paper mills, power plants, and iron and steel plants. In a second step, we computed regional EMO curves considering transport and country-specific impacts for energy supply. Building upon regional EMO curves, we identify favorable locations for CO2 utilization with lowest environmental impacts of CO2 supply, so-called CO2 oases. PMID:26752014

  7. Particle capture efficiency in a multi-wire model for high gradient magnetic separation

    NASA Astrophysics Data System (ADS)

    Eisenträger, Almut; Vella, Dominic; Griffiths, Ian M.

    2014-07-01

    High gradient magnetic separation (HGMS) is an efficient way to remove magnetic and paramagnetic particles, such as heavy metals, from waste water. As the suspension flows through a magnetized filter mesh, high magnetic gradients around the wires attract and capture the particles removing them from the fluid. We model such a system by considering the motion of a paramagnetic tracer particle through a periodic array of magnetized cylinders. We show that there is a critical Mason number (ratio of viscous to magnetic forces) below which the particle is captured irrespective of its initial position in the array. Above this threshold, particle capture is only partially successful and depends on the particle's entry position. We determine the relationship between the critical Mason number and the system geometry using numerical and asymptotic calculations. If a capture efficiency below 100% is sufficient, our results demonstrate how operating the HGMS system above the critical Mason number but with multiple separation cycles may increase efficiency.

  8. Preparation of polymeric particles in CO(2) medium using non-toxic solvents: formulation and comparisons with a phase separation method.

    PubMed

    Tran, My-Kien; Swed, Amin; Boury, Frank

    2012-11-01

    The aim of this work was to elaborate formulation strategies to encapsulate a protein into biodegradable polymeric particles for sustained release purpose. In this paper, two encapsulation methods will be presented, one dealing with a phase separation phenomenon while the other involving an emulsification/extraction process in CO(2) medium. In those methods, only non-volatile injectable solvents such as glycofurol or isosorbide dimethyl ether were used to dissolve the polymer. Moreover, experimental designs were built up to help us to go further in the understanding of the processes and to better predict output responses in design space. Spherical particles were successfully generated with a satisfactory encapsulation yield. Further characterization steps such as in vitro, in vivo releases will be carried out to validate the interest of our encapsulation methods in the development of drug delivery systems. PMID:22959993

  9. CO2-neutral fuels

    NASA Astrophysics Data System (ADS)

    Goede, A. P. H.

    2015-08-01

    established by powering the conversion step by renewable energy and recapturing the CO2 emitted after combustion, ultimately from the surrounding air to cover emissions from distributed source. Carbon Capture and Utilisation (CCU) coupled to P2G thus creates a CO2-neutral energy system based on synthetic hydrocarbon fuel. It would enable a circular economy where the carbon cycle is closed by recovering the CO2 emitted after reuse of synthetic hydrocarbon fuel. The critical step, technically as well as economically, is the conversion of feedstock CO2/H2O into syngas rather than the capture of CO2 from ambient air.

  10. Optimization of a dual capture element magnetic separator for the purification of high velocity water flow

    NASA Astrophysics Data System (ADS)

    Belounis, Abdallah; Mehasni, Rabia; Ouili, Mehdi; Feliachi, Mouloud; El-Hadi Latreche, Mohamed

    2016-02-01

    In this paper a magnetic separator based on the use of a cascade arrangement of two identical capture elements has been optimized and verified. Such a separator is intended for the separation of fine particles of iron from flowing water at high velocity. The optimization has concerned the search for the excitation current and the distance between the capture elements that permit the extraction of the particles from a water flow in a circular channel at an average velocity ufav = 1.05 m/s. For such optimization we have minimized the objective function that is the distance between the capture position of a particle initially situated at a specific position and the central point of the last capture element of the arrangement. To perform the minimization, we have applied the Tabu search method. To validate the obtained results experimental verification based on the control of the evolution of the captured particle buildup and the quantifying of the separated volume of particles was achieved. Contribution to the topical issue "Numelec 2015 - Elected submissions", edited by Adel Razek

  11. Development of a Novel Gas Pressurized Process-Based Technology for CO2 Capture from Post-Combustion Flue Gases Preliminary Year 1 Techno-Economic Study Results and Methodology for Gas Pressurized Stripping Process

    SciTech Connect

    Chen, Shiaoguo

    2013-03-01

    Under the DOE’s Innovations for Existing Plants (IEP) Program, Carbon Capture Scientific, LLC (CCS) is developing a novel gas pressurized stripping (GPS) process to enable efficient post-combustion carbon capture (PCC) from coal-fired power plants. A technology and economic feasibility study is required as a deliverable in the project Statement of Project Objectives. This study analyzes a fully integrated pulverized coal power plant equipped with GPS technology for PCC, and is carried out, to the maximum extent possible, in accordance to the methodology and data provided in ATTACHMENT 3 – Basis for Technology Feasibility Study of DOE Funding Opportunity Number: DE-FOA-0000403. The DOE/NETL report on “Cost and Performance Baseline for Fossil Energy Plants, Volume 1: Bituminous Coal and Natural Gas to Electricity (Original Issue Date, May 2007), NETL Report No. DOE/NETL-2007/1281, Revision 1, August 2007” was used as the main source of reference to be followed, as per the guidelines of ATTACHMENT 3 of DE-FOA-0000403. The DOE/NETL-2007/1281 study compared the feasibility of various combinations of power plant/CO2 capture process arrangements. The report contained a comprehensive set of design basis and economic evaluation assumptions and criteria, which are used as the main reference points for the purpose of this study. Specifically, Nexant adopted the design and economic evaluation basis from Case 12 of the above-mentioned DOE/NETL report. This case corresponds to a nominal 550 MWe (net), supercritical greenfield PC plant that utilizes an advanced MEAbased absorption system for CO2 capture and compression. For this techno-economic study, CCS’ GPS process replaces the MEA-based CO2 absorption system used in the original case. The objective of this study is to assess the performance of a full-scale GPS-based PCC design that is integrated with a supercritical PC plant similar to Case 12 of the DOE/NETL report, such that it corresponds to a nominal 550 MWe

  12. High Temperature Polybenzimidazole Hollow Fiber Membranes for Hydrogen Separation and Carbon Dioxide Capture from Synthesis Gas

    DOE PAGESBeta

    Singh, Rajinder P.; Dahe, Ganpat J.; Dudeck, Kevin W.; Welch, Cynthia F.; Berchtold, Kathryn A.

    2014-12-31

    Sustainable reliance on hydrocarbon feedstocks for energy generation requires CO₂ separation technology development for energy efficient carbon capture from industrial mixed gas streams. High temperature H₂ selective glassy polymer membranes are an attractive option for energy efficient H₂/CO₂ separations in advanced power production schemes with integrated carbon capture. They enable high overall process efficiencies by providing energy efficient CO₂ separations at process relevant operating conditions and correspondingly, minimized parasitic energy losses. Polybenzimidazole (PBI)-based materials have demonstrated commercially attractive H₂/CO₂ separation characteristics and exceptional tolerance to hydrocarbon fuel derived synthesis (syngas) gas operating conditions and chemical environments. To realize a commerciallymore » attractive carbon capture technology based on these PBI materials, development of high performance, robust PBI hollow fiber membranes (HFMs) is required. In this work, we discuss outcomes of our recent efforts to demonstrate and optimize the fabrication and performance of PBI HFMs for use in pre-combustion carbon capture schemes. These efforts have resulted in PBI HFMs with commercially attractive fabrication protocols, defect minimized structures, and commercially attractive permselectivity characteristics at IGCC syngas process relevant conditions. The H₂/CO₂ separation performance of these PBI HFMs presented in this document regarding realistic process conditions is greater than that of any other polymeric system reported to-date.« less

  13. High Temperature Polybenzimidazole Hollow Fiber Membranes for Hydrogen Separation and Carbon Dioxide Capture from Synthesis Gas

    SciTech Connect

    Singh, Rajinder P.; Dahe, Ganpat J.; Dudeck, Kevin W.; Welch, Cynthia F.; Berchtold, Kathryn A.

    2014-12-31

    Sustainable reliance on hydrocarbon feedstocks for energy generation requires CO₂ separation technology development for energy efficient carbon capture from industrial mixed gas streams. High temperature H₂ selective glassy polymer membranes are an attractive option for energy efficient H₂/CO₂ separations in advanced power production schemes with integrated carbon capture. They enable high overall process efficiencies by providing energy efficient CO₂ separations at process relevant operating conditions and correspondingly, minimized parasitic energy losses. Polybenzimidazole (PBI)-based materials have demonstrated commercially attractive H₂/CO₂ separation characteristics and exceptional tolerance to hydrocarbon fuel derived synthesis (syngas) gas operating conditions and chemical environments. To realize a commercially attractive carbon capture technology based on these PBI materials, development of high performance, robust PBI hollow fiber membranes (HFMs) is required. In this work, we discuss outcomes of our recent efforts to demonstrate and optimize the fabrication and performance of PBI HFMs for use in pre-combustion carbon capture schemes. These efforts have resulted in PBI HFMs with commercially attractive fabrication protocols, defect minimized structures, and commercially attractive permselectivity characteristics at IGCC syngas process relevant conditions. The H₂/CO₂ separation performance of these PBI HFMs presented in this document regarding realistic process conditions is greater than that of any other polymeric system reported to-date.

  14. Particle-scale CO2 adsorption kinetics modeling considering three reaction mechanisms

    SciTech Connect

    Suh, Dong-Myung; Sun, Xin

    2013-09-01

    In the presence of water (H2O), dry and wet adsorptions of carbon dioxide (CO2) and physical adsorption of H2O happen concurrently in a sorbent particle. The three reactions depend on each other and have a complicated, but important, effect on CO2 capturing via a solid sorbent. In this study, transport phenomena in the sorbent were modeled, including the tree reactions, and a numerical solving procedure for the model also was explained. The reaction variable distribution in the sorbent and their average values were calculated, and simulation results were compared with experimental data to validate the proposed model. Some differences, caused by thermodynamic parameters, were observed between them. However, the developed model reasonably simulated the adsorption behaviors of a sorbent. The weight gained by each adsorbed species, CO2 and H2O, is difficult to determine experimentally. It is known that more CO2 can be captured in the presence of water. Still, it is not yet known quantitatively how much more CO2 the sorbent can capture, nor is it known how much dry and wet adsorptions separately account for CO2 capture. This study addresses those questions by modeling CO2 adsorption in a particle and simulating the adsorption process using the model. As adsorption temperature changed into several values, the adsorbed amount of each species was calculated. The captured CO2 in the sorbent particle was compared quantitatively between dry and wet conditions. As the adsorption temperature decreased, wet adsorption increased. However, dry adsorption was reduced.

  15. Rolling stones; fast weathering of olivine in shallow seas for cost-effective CO2 capture and mitigation of global warming and ocean acidification

    NASA Astrophysics Data System (ADS)

    Schuiling, R. D.; de Boer, P. L.

    2011-12-01

    Human CO2 emissions may drive the Earth into a next greenhouse state. They can be mitigated by accelerating weathering of natural rock under the uptake of CO2. We disprove the paradigm that olivine weathering in nature would be a slow process, and show that it is not needed to mill olivine to very fine, 10 μm-size grains in order to arrive at a complete dissolution within 1-