Multishelled CaO Microspheres Stabilized by Atomic Layer Deposition of Al2 O3 for Enhanced CO2 Capture Performance.

PubMed

Armutlulu, Andac; Naeem, Muhammad Awais; Liu, Hsueh-Ju; Kim, Sung Min; Kierzkowska, Agnieszka; Fedorov, Alexey; Müller, Christoph R

2017-11-01

CO 2 capture and storage is a promising concept to reduce anthropogenic CO 2 emissions. The most established technology for capturing CO 2 relies on amine scrubbing that is, however, associated with high costs. Technoeconomic studies show that using CaO as a high-temperature CO 2 sorbent can significantly reduce the costs of CO 2 capture. A serious disadvantage of CaO derived from earth-abundant precursors, e.g., limestone, is the rapid, sintering-induced decay of its cyclic CO 2 uptake. Here, a template-assisted hydrothermal approach to develop CaO-based sorbents exhibiting a very high and cyclically stable CO 2 uptake is exploited. The morphological characteristics of these sorbents, i.e., a porous shell comprised of CaO nanoparticles coated by a thin layer of Al 2 O 3 (<3 nm) containing a central void, ensure (i) minimal diffusion limitations, (ii) space to accompany the substantial volumetric changes during CO 2 capture and release, and (iii) a minimal quantity of Al 2 O 3 for structural stabilization, thus maximizing the fraction of CO 2 -capture-active CaO. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ionic-Liquid-Based CO2 Capture Systems: Structure, Interaction and Process.

PubMed

Zeng, Shaojuan; Zhang, Xiangping; Bai, Lu; Zhang, Xiaochun; Wang, Hui; Wang, Jianji; Bao, Di; Li, Mengdie; Liu, Xinyan; Zhang, Suojiang

2017-07-26

The inherent structure tunability, good affinity with CO 2 , and nonvolatility of ionic liquids (ILs) drive their exploration and exploitation in CO 2 separation field, and has attracted remarkable interest from both industries and academia. The aim of this Review is to give a detailed overview on the recent advances on IL-based materials, including pure ILs, IL-based solvents, and IL-based membranes for CO 2 capture and separation from the viewpoint of molecule to engineering. The effects of anions, cations and functional groups on CO 2 solubility and selectivity of ILs, as well as the studies on degradability of ILs are reviewed, and the recent developments on functionalized ILs, IL-based solvents, and IL-based membranes are also discussed. CO 2 separation mechanism with IL-based solvents and IL-based membranes are explained by combining molecular simulation and experimental characterization. Taking into consideration of the applications and industrialization, the recent achievements and developments on the transport properties of IL fluids and the process design of IL-based processes are highlighted. Finally, the future research challenges and perspectives of the commercialization of CO 2 capture and separation with IL-based materials are posed.

CO 2 capture from IGCC gas streams using the AC-ABC process

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nagar, Anoop; McLaughlin, Elisabeth; Hornbostel, Marc

The objective of this project was to develop a novel, low-cost CO 2 capture process from pre-combustion gas streams. The bench-scale work was conducted at the SRI International. A 0.15-MWe integrated pilot plant was constructed and operated for over 700 hours at the National Carbon Capture Center, Wilsonville, AL. The AC-ABC (ammonium carbonate-ammonium bicarbonate) process for capture of CO 2 and H 2S from the pre-combustion gas stream offers many advantages over Selexol-based technology. The process relies on the simple chemistry of the NH 3-CO 2-H 2O-H 2S system and on the ability of the aqueous ammoniated solution to absorbmore » CO 2 at near ambient temperatures and to release it as a high-purity, high-pressure gas at a moderately elevated regeneration temperature. It is estimated the increase in cost of electricity (COE) with the AC-ABC process will be ~ 30%, and the cost of CO 2 captured is projected to be less than $27/metric ton of CO 2 while meeting 90% CO 2 capture goal. The Bechtel Pressure Swing Claus (BPSC) is a complementary technology offered by Bechtel Hydrocarbon Technology Solutions, Inc. BPSC is a high-pressure, sub-dew-point Claus process that allows for nearly complete removal of H 2S from a gas stream. It operates at gasifier pressures and moderate temperatures and does not affect CO 2 content. When coupled with AC-ABC, the combined technologies allow a nearly pure CO 2 stream to be captured at high pressure, something which Selexol and other solvent-based technologies cannot achieve.« less

Active chemisorption sites in functionalized ionic liquids for carbon capture.

PubMed

Cui, Guokai; Wang, Jianji; Zhang, Suojiang

2016-07-25

Development of novel technologies for the efficient and reversible capture of CO2 is highly desired. In the last decade, CO2 capture using ionic liquids has attracted intensive attention from both academia and industry, and has been recognized as a very promising technology. Recently, a new approach has been developed for highly efficient capture of CO2 by site-containing ionic liquids through chemical interaction. This perspective review focuses on the recent advances in the chemical absorption of CO2 using site-containing ionic liquids, such as amino-based ionic liquids, azolate ionic liquids, phenolate ionic liquids, dual-functionalized ionic liquids, pyridine-containing ionic liquids and so on. Other site-containing liquid absorbents such as amine-based solutions, switchable solvents, and functionalized ionic liquid-amine blends are also investigated. Strategies have been discussed for how to activate the existent reactive sites and develop novel reactive sites by physical and chemical methods to enhance CO2 absorption capacity and reduce absorption enthalpy. The carbon capture mechanisms of these site-containing liquid absorbents are also presented. Particular attention has been paid to the latest progress in CO2 capture in multiple-site interactions by amino-free anion-functionalized ionic liquids. In the last section, future directions and prospects for carbon capture by site-containing ionic liquids are outlined.

Updated (BP3) Technical and Economic Feasibility Study - Electrochemical Membrane for Carbon Dioxide Capture and Power Generation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ghezel-Ayagh, Hossein

This topical report summarizes the results of an updated Technical & Economic Feasibility Study (T&EFS) which was conducted in Budget Period 3 of the project to evaluate the performance and cost of the Electrochemical Membrane (ECM)-based CO 2 capture system. The ECM technology is derived from commercially available inorganic membranes; the same used in FuelCell Energy’s commercial fuel cell power plants and sold under the trade name Direct FuelCell® (DFC®). The ECM stacks are utilized in the Combined Electric Power (generation) And Carbon dioxide Separation (CEPACS) systems which can be deployed as add-ons to conventional power plants (Pulverized Coal, Combinedmore » Cycle, etc.) or industrial facilities to simultaneously produce power while capturing >90% of the CO 2 from the flue gas. In this study, an ECM-based CEPACS plant was designed to capture and compress >90% of the CO 2 (for sequestration or beneficial use) from the flue gas of a reference 550 MW (nominal, net AC) Pulverized Coal (PC) Rankine Cycle (Subcritical steam) power plant. ECM performance was updated based on bench scale ECM stack test results. The system process simulations were performed to generate the CEPACS plant performance estimates. The performance assessment included estimation of the parasitic power consumption for CO 2 capture and compression, and the efficiency impact on the PC plant. While the ECM-based CEPACS system for the 550 MW PC plant captures 90% of CO 2 from the flue gas, it generates additional (net AC) power after compensating for the auxiliary power requirements of CO 2 capture and compression. An equipment list, ECM stacks packaging design, and CEPACS plant layout were developed to facilitate the economic analysis. Vendor quotes were also solicited. The economic feasibility study included estimation of CEPACS plant capital cost, cost of electricity (COE) analyses and estimation of cost per ton of CO 2 captured. The incremental COE for the ECM-based CO 2 capture is expected to meet U.S. DOE’s target of 35%. This study has indicated that CEPACS systems offer significant benefits with respect to cost, performance, water consumption and emissions to environment. The realization of these benefits will provide a single solution to carbon dioxide capture in addition to meeting the increasing demand for electricity.« less

Updated (BP3) Technical and Economic Feasibility Study - Electrochemical Membrane for Carbon Dioxide Capture and Power Generation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ghezel-Ayagh, Hossein

This topical report summarizes the results of an updated Technical & Economic Feasibility Study (T&EFS) which was conducted in Budget Period 3 of the project to evaluate the performance and cost of the Electrochemical Membrane (ECM)-based CO2 capture system. The ECM technology is derived from commercially available inorganic membranes; the same used in FuelCell Energy’s commercial fuel cell power plants and sold under the trade name Direct FuelCell® (DFC®). The ECM stacks are utilized in the Combined Electric Power (generation) And Carbon dioxide Separation (CEPACS) systems which can be deployed as add-ons to conventional power plants (Pulverized Coal, Combined Cycle,more » etc.) or industrial facilities to simultaneously produce power while capturing >90% of the CO2 from the flue gas. In this study, an ECM-based CEPACS plant was designed to capture and compress >90% of the CO2 (for sequestration or beneficial use) from the flue gas of a reference 550 MW (nominal, net AC) Pulverized Coal (PC) Rankine Cycle (Subcritical steam) power plant. ECM performance was updated based on bench scale ECM stack test results. The system process simulations were performed to generate the CEPACS plant performance estimates. The performance assessment included estimation of the parasitic power consumption for CO2 capture and compression, and the efficiency impact on the PC plant. While the ECM-based CEPACS system for the 550 MW PC plant captures 90% of CO2 from the flue gas, it generates additional (net AC) power after compensating for the auxiliary power requirements of CO2 capture and compression. An equipment list, ECM stacks packaging design, and CEPACS plant layout were developed to facilitate the economic analysis. Vendor quotes were also solicited. The economic feasibility study included estimation of CEPACS plant capital cost, cost of electricity (COE) analyses and estimation of cost per ton of CO2 captured. The incremental COE for the ECM-based CO2 capture is expected to meet U.S. DOE’s target of 35%. This study has indicated that CEPACS systems offer significant benefits with respect to cost, performance, water consumption and emissions to environment. The realization of these benefits will provide a single solution to carbon dioxide capture in addition to meeting the increasing demand for electricity.« less

Nitrosamines and Nitramines in Amine-Based Carbon Dioxide Capture Systems: Fundamentals, Engineering Implications, and Knowledge Gaps.

PubMed

Yu, Kun; Mitch, William A; Dai, Ning

2017-10-17

Amine-based absorption is the primary contender for postcombustion CO 2 capture from fossil fuel-fired power plants. However, significant concerns have arisen regarding the formation and emission of toxic nitrosamine and nitramine byproducts from amine-based systems. This paper reviews the current knowledge regarding these byproducts in CO 2 capture systems. In the absorber, flue gas NO x drives nitrosamine and nitramine formation after its dissolution into the amine solvent. The reaction mechanisms are reviewed based on CO 2 capture literature as well as biological and atmospheric chemistry studies. In the desorber, nitrosamines are formed under high temperatures by amines reacting with nitrite (a hydrolysis product of NO x ), but they can also thermally decompose following pseudo-first order kinetics. The effects of amine structure, primarily amine order, on nitrosamine formation and the corresponding mechanisms are discussed. Washwater units, although intended to control emissions from the absorber, can contribute to additional nitrosamine formation when accumulated amines react with residual NO x . Nitramines are much less studied than nitrosamines in CO 2 capture systems. Mitigation strategies based on the reaction mechanisms in each unit of the CO 2 capture systems are reviewed. Lastly, we highlight research needs in clarifying reaction mechanisms, developing analytical methods for both liquid and gas phases, and integrating different units to quantitatively predict the accumulation and emission of nitrosamines and nitramines.

Design of Aminopolymer Structure to Enhance Performance and Stability of CO2 Sorbents: Poly(propylenimine) vs Poly(ethylenimine).

PubMed

Pang, Simon H; Lee, Li-Chen; Sakwa-Novak, Miles A; Lively, Ryan P; Jones, Christopher W

2017-03-15

Studies on aminopolymer/oxide composite materials for direct CO 2 capture from air have often focused on the prototypical poly(ethylenimine) (PEI) as the aminopolymer. However, it is known that PEI will oxidatively degrade at elevated temperatures. This degradation has been ascribed to the presence of secondary amines, which, when oxidized, lose their CO 2 capture capacity. Here, we demonstrate the use of small molecule poly(propylenimine) (PPI) in linear and dendritic architectures supported in silica as adsorbent materials for direct CO 2 capture from air. Regardless of amine loading or aminopolymer architecture, the PPI-based sorbents are found to be more efficient for CO 2 capture than PEI-based sorbents. Moreover, PPI is found to be more resistant to oxidative degradation than PEI, even while containing secondary amines, as supported by FTIR, NMR, and ESI-MS studies. These results suggest that PPI-based CO 2 sorbents may allow for longer sorbent working lifetimes due to an increased tolerance to sorbent regeneration conditions and suggest that the presence of secondary amines may not mean that all aminopolymers will oxidatively degrade.

Assessment of Solid Sorbent Systems for Post-Combustion Carbon Dioxide Capture at Coal-Fired Power Plants

NASA Astrophysics Data System (ADS)

Glier, Justin C.

In an effort to lower future CO2 emissions, a wide range of technologies are being developed to scrub CO2 from the flue gases of fossil fuel-based electric power and industrial plants. This thesis models one of several early-stage post-combustion CO2 capture technologies, solid sorbent-based CO2 capture process, and presents performance and cost estimates of this system on pulverized coal power plants. The spreadsheet-based software package Microsoft Excel was used in conjunction with AspenPlus modelling results and the Integrated Environmental Control Model to develop performance and cost estimates for the solid sorbent-based CO2 capture technology. A reduced order model also was created to facilitate comparisons among multiple design scenarios. Assumptions about plant financing and utilization, as well as uncertainties in heat transfer and material design that affect heat exchanger and reactor design were found to produce a wide range of cost estimates for solid sorbent-based systems. With uncertainties included, costs for a supercritical power plant with solid sorbent-based CO2 capture ranged from 167 to 533 per megawatt hour for a first-of-a-kind installation (with all costs in constant 2011 US dollars) based on a 90% confidence interval. The median cost was 209/MWh. Post-combustion solid sorbent-based CO2 capture technology is then evaluated in terms of the potential cost for a mature system based on historic experience as technologies are improved with sequential iterations of the currently available system. The range costs for a supercritical power plant with solid sorbent-based CO2 capture was found to be 118 to 189 per megawatt hour with a nominal value of 163 per megawatt hour given the expected range of technological improvement in the capital and operating costs and efficiency of the power plant after 100 GW of cumulative worldwide experience. These results suggest that the solid sorbent-based system will not be competitive with currently available liquid amine-systems in the absence of significant new improvements in solid sorbent properties and process system design to reduce the heat exchange surface area in the regenerator and cross-flow heat exchanger. Finally, the importance of these estimates for policy makers is discussed.

Membrane Process to Capture CO{sub 2} from Coal-Fired Power Plant Flue Gas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Merkel, Tim; Wei, Xiaotong; Firat, Bilgen

2012-03-31

This final report describes work conducted for the U.S. Department of Energy National Energy Technology Laboratory (DOE NETL) on development of an efficient membrane process to capture carbon dioxide (CO{sub 2}) from power plant flue gas (award number DE-NT0005312). The primary goal of this research program was to demonstrate, in a field test, the ability of a membrane process to capture up to 90% of CO{sub 2} in coal-fired flue gas, and to evaluate the potential of a full-scale version of the process to perform this separation with less than a 35% increase in the levelized cost of electricity (LCOE).more » Membrane Technology and Research (MTR) conducted this project in collaboration with Arizona Public Services (APS), who hosted a membrane field test at their Cholla coal-fired power plant, and the Electric Power Research Institute (EPRI) and WorleyParsons (WP), who performed a comparative cost analysis of the proposed membrane CO{sub 2} capture process. The work conducted for this project included membrane and module development, slipstream testing of commercial-sized modules with natural gas and coal-fired flue gas, process design optimization, and a detailed systems and cost analysis of a membrane retrofit to a commercial power plant. The Polaris? membrane developed over a number of years by MTR represents a step-change improvement in CO{sub 2} permeance compared to previous commercial CO{sub 2}-selective membranes. During this project, membrane optimization work resulted in a further doubling of the CO{sub 2} permeance of Polaris membrane while maintaining the CO{sub 2}/N{sub 2} selectivity. This is an important accomplishment because increased CO{sub 2} permeance directly impacts the membrane skid cost and footprint: a doubling of CO{sub 2} permeance halves the skid cost and footprint. In addition to providing high CO{sub 2} permeance, flue gas CO{sub 2} capture membranes must be stable in the presence of contaminants including SO{sub 2}. Laboratory tests showed no degradation in Polaris membrane performance during two months of continuous operation in a simulated flue gas environment containing up to 1,000 ppm SO{sub 2}. A successful slipstream field test at the APS Cholla power plant was conducted with commercialsize Polaris modules during this project. This field test is the first demonstration of stable performance by commercial-sized membrane modules treating actual coal-fired power plant flue gas. Process design studies show that selective recycle of CO{sub 2} using a countercurrent membrane module with air as a sweep stream can double the concentration of CO{sub 2} in coal flue gas with little energy input. This pre-concentration of CO{sub 2} by the sweep membrane reduces the minimum energy of CO{sub 2} separation in the capture unit by up to 40% for coal flue gas. Variations of this design may be even more promising for CO{sub 2} capture from NGCC flue gas, in which the CO{sub 2} concentration can be increased from 4% to 20% by selective sweep recycle. EPRI and WP conducted a systems and cost analysis of a base case MTR membrane CO{sub 2} capture system retrofitted to the AEP Conesville Unit 5 boiler. Some of the key findings from this study and a sensitivity analysis performed by MTR include: The MTR membrane process can capture 90% of the CO{sub 2} in coal flue gas and produce high-purity CO{sub 2} (>99%) ready for sequestration. CO{sub 2} recycle to the boiler appears feasible with minimal impact on boiler performance; however, further study by a boiler OEM is recommended. For a membrane process built today using a combination of slight feed compression, permeate vacuum, and current compression equipment costs, the membrane capture process can be competitive with the base case MEA process at 90% CO{sub 2} capture from a coal-fired power plant. The incremental LCOE for the base case membrane process is about equal to that of a base case MEA process, within the uncertainty in the analysis. With advanced membranes (5,000 gpu for CO{sub 2} and 50 for CO{sub 2}/N{sub 2}), operating with no feed compression and low-cost CO{sub 2} compression equipment, an incremental LCOE of $33/MWh at 90% capture can be achieved (40% lower than the advanced MEA case). Even with lower cost compression, it appears unlikely that a membrane process using high feed compression (>5 bar) can be competitive with amine absorption, due to the capital cost and energy consumption of this equipment. Similarly, low vacuum pressure (<0.2 bar) cannot be used due to poor efficiency and high cost of this equipment. High membrane permeance is important to reduce the capital cost and footprint of the membrane unit. CO{sub 2}/N{sub 2} selectivity is less important because it is too costly to generate a pressure ratio where high selectivity can be useful. A potential cost ?sweet spot? exists for use of membrane-based technology, if 50-70% CO{sub 2} capture is acceptable. There is a minimum in the cost of CO{sub 2} avoided/ton that membranes can deliver at 60% CO{sub 2} capture, which is 20% lower than the cost at 90% capture. Membranes operating with no feed compression are best suited for lower capture rates. Currently, it appears that the biggest hurdle to use of membranes for post-combustion CO{sub 2} capture is compression equipment cost. An alternative approach is to use sweep membranes in parallel with another CO{sub 2} capture technology that does not require feed compression or vacuum equipment. Hybrid designs that utilize sweep membranes for selective CO{sub 2} recycle show potential to significantly reduce the minimum energy of CO{sub 2} separation.« less

Room-temperature ionic liquids and composite materials: platform technologies for CO(2) capture.

PubMed

Bara, Jason E; Camper, Dean E; Gin, Douglas L; Noble, Richard D

2010-01-19

Clean energy production has become one of the most prominent global issues of the early 21st century, prompting social, economic, and scientific debates regarding energy usage, energy sources, and sustainable energy strategies. The reduction of greenhouse gas emissions, specifically carbon dioxide (CO(2)), figures prominently in the discussions on the future of global energy policy. Billions of tons of annual CO(2) emissions are the direct result of fossil fuel combustion to generate electricity. Producing clean energy from abundant sources such as coal will require a massive infrastructure and highly efficient capture technologies to curb CO(2) emissions. Current technologies for CO(2) removal from other gases, such as those used in natural gas sweetening, are also capable of capturing CO(2) from power plant emissions. Aqueous amine processes are found in the vast majority of natural gas sweetening operations in the United States. However, conventional aqueous amine processes are highly energy intensive; their implementation for postcombustion CO(2) capture from power plant emissions would drastically cut plant output and efficiency. Membranes, another technology used in natural gas sweetening, have been proposed as an alternative mechanism for CO(2) capture from flue gas. Although membranes offer a potentially less energy-intensive approach, their development and industrial implementation lags far behind that of amine processes. Thus, to minimize the impact of postcombustion CO(2) capture on the economics of energy production, advances are needed in both of these areas. In this Account, we review our recent research devoted to absorptive processes and membranes. Specifically, we have explored the use of room-temperature ionic liquids (RTILs) in absorptive and membrane technologies for CO(2) capture. RTILs present a highly versatile and tunable platform for the development of new processes and materials aimed at the capture of CO(2) from power plant flue gas and in natural gas sweetening. The desirable properties of RTIL solvents, such as negligible vapor pressures, thermal stability, and a large liquid range, make them interesting candidates as new materials in well-known CO(2) capture processes. Here, we focus on the use of RTILs (1) as absorbents, including in combination with amines, and (2) in the design of polymer membranes. RTIL amine solvents have many potential advantages over aqueous amines, and the versatile chemistry of imidazolium-based RTILs also allows for the generation of new types of CO(2)-selective polymer membranes. RTIL and RTIL-based composites can compete with, or improve upon, current technologies. Moreover, owing to our experience in this area, we are developing new imidazolium-based polymer architectures and thermotropic and lyotropic liquid crystals as highly tailorable materials based on and capable of interacting with RTILs.

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

PubMed

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

2016-10-20

Dual phase membranes are highly CO 2 -selective membranes with an operating temperature above 400 °C. The focus of this work is to quantify the potential of dual phase membranes in pre- and post-combustion CO 2 capture processes. The process evaluations show that the dual phase membranes integrated with an NGCC power plant for CO 2 capture are not competitive with the MEA process for post-combustion capture. However, dual phase membrane concepts outperform the reference Selexol technology for pre-combustion CO 2 capture in an IGCC process. The two processes evaluated in this work, post-combustion NGCC and pre-combustion IGCC, represent extremes in CO 2 partial pressure fed to the separation unit. Based on the evaluations it is expected that dual phase membranes could be competitive for post-combustion capture from a pulverized coal fired power plant (PCC) and pre-combustion capture from an Integrated Reforming Cycle (IRCC).

Pilot-Scale Silicone Process for Low-Cost Carbon Dioxide Capture Preliminary Techno-Economic Analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Singh, Surinder; Spiry, Irina; Wood, Benjamin

This report presents system and economic analysis for a carbon-capture unit which uses an aminosilicone-based solvent for CO{sub 2} capture in a pulverized coal (PC) boiler. The aminosilicone solvent is a 60/40 wt/wt mixture of 3-aminopropyl end-capped polydimethylsiloxane (GAP-1m) with tri-ethylene glycol (TEG) as a co-solvent. For comparison purposes, the report also shows results for a carbon-capture unit based on a conventional approach using mono-ethanol amine (MEA). The first year removal cost of CO{sub 2} for the aminosilicone-based carbon-capture process ismore » $46.04/ton of CO2 as compared to $$60.25/ton of CO{sub 2} when MEA is used. The aminosilicone-based process has <77% of the CAPEX of a system using MEA solvent. The lower CAPEX is due to several factors, including the higher working capacity of the aminosilicone solvent compared the MEA, which reduces the solvent flow rate required, reducing equipment sizes. If it is determined that carbon steel can be used in the rich-lean heat exchanger in the carbon capture unit, the first year removal cost of CO{sub 2} decreases to $$44.12/ton. The aminosilicone-based solvent has a higher thermal stability than MEA, allowing desorption to be conducted at higher temperatures and pressures, decreasing the number of compressor stages needed. The aminosilicone-based solvent also has a lower vapor pressure, allowing the desorption to be conducted in a continuous-stirred tank reactor versus a more expensive packed column. The aminosilicone-based solvent has a lower heat capacity, which decreases the heat load on the desorber. In summary, the amino-silicone solvent has significant advantages over conventional systems using MEA.« less

Metal-Organic Frameworks as Potential Platforms for Carbon Dioxide Capture and Chemical Transformation

NASA Astrophysics Data System (ADS)

Gao, Wenyang

The anthropogenic carbon dioxide (CO2) emission into the atmosphere, mainly through the combustion of fossil fuels, has resulted in a balance disturbance of the carbon cycle. Overwhelming scientific evidence proves that the escalating level of atmospheric CO2 is deemed as the main culprit for global warming and climate change. It is thus imperative to develop viable CO2 capture and sequestration (CCS) technologies to reduce CO2 emissions, which is also essential to avoid the potential devastating effects in future. The drawbacks of energy-cost, corrosion and inefficiency for amine-based wet-scrubbing systems which are currently used in industry, have prompted the exploration of alternative approaches for CCS. Extensive efforts have been dedicated to the development of functional porous materials, such as activated carbons, zeolites, porous organic polymers, and metal-organic frameworks (MOFs) to capture CO2. However, these adsorbents are limited by either poor selectivity for CO2 separation from gas mixtures or low CO2 adsorption capacity. Therefore, it is still highly demanding to design next-generation adsorbent materials fulfilling the requirements of high CO2 selectivity and enough CO2 capacity, as well as high water/moisture stability under practical conditions. Metal-organic frameworks (MOFs) have been positioned at the forefront of this area as a promising type of candidate amongst various porous materials. This is triggered by the modularity and functionality of pore size, pore walls and inner surface of MOFs by use of crystal engineering approaches. In this work, several effective strategies, such as incorporating 1,2,3-triazole groups as moderate Lewis base centers into MOFs and employing flexible azamacrocycle-based ligands to build MOFs, demonstrate to be promising ways to enhance CO 2 uptake capacity and CO2 separation ability of porous MOFs. It is revealed through in-depth studies on counter-intuitive experimental observations that the local electric field favours more than the richness of exposed nitrogen atoms for the interactions between MOFs and CO2 molecules, which provides a new perspective for future design of new MOFs and other types of porous materials for CO2 capture. Meanwhile, to address the water/moisture stability issue of MOFs, remote stabilization of copper paddlewheel clusters is achieved by strengthening the bonding between organic ligands and triangular inorganic copper trimers, which in turn enhances the stability of the whole MOF network and provides a better understanding of the mechanism promoting prospective suitable MOFs with enhanced water stability. In contrast with CO2 capture by sorbent materials, the chemical transformation of the captured CO2 into value-added products represents an alternative which is attractive and sustainable, and has been of escalating interest. The nanospace within MOFs not only provides the inner porosity for CO2 capture, but also engenders accessible room for substrate molecules for catalytic purpose. It is demonstrated that high catalytic efficiency for chemical fixation of CO2 into cyclic carbonates under ambient conditions is achieved on MOF-based nanoreactors featuring a high-density of well-oriented Lewis active sites. Furthermore, described for the first time is that CO 2 can be successfully inserted into aryl C-H bonds of a MOF to generate carboxylate groups. This proof-of-concept study contributes a different perspective to the current landscape of CO2 capture and transformation. In closing, the overarching goal of this work is not only to seek efficient MOF adsorbents for CO2 capture, but also to present a new yet attractive scenario of CO2 utilization on MOF platforms.

CO 2 Capture from Ambient Air by Crystallization with a Guanidine Sorbent

DOE PAGES

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

2016-12-21

Carbon capture and storage is an important strategy for stabilizing the increasing concentration of atmospheric CO 2 and the global temperature. A possible approach toward reversing this trend and decreasing the atmospheric CO 2 concentration is to remove the CO 2 directly from air (direct air capture). In this paper, we report a simple aqueous guanidine sorbent that captures CO 2 from ambient air and binds it as a crystalline carbonate salt by guanidinium hydrogen bonding. The resulting solid has very low aqueous solubility (K sp=1.0(4)×10 -8), which facilitates its separation from solution by filtration. The bound CO 2 canmore » be released by relatively mild heating of the crystals at 80–120 °C, which regenerates the guanidine sorbent quantitatively. Finally and thus, this crystallization-based approach to CO 2 separation from air requires minimal energy and chemical input, and offers the prospect for low-cost direct air capture technologies.« less

Sequential capture of CO2 and SO2 in a pressurized TGA simulating FBC conditions.

PubMed

Sun, Ping; Grace, John R; Lim, C Jim; Anthony, Edward J

2007-04-15

Four FBC-based processes were investigated as possible means of sequentially capturing SO2 and CO2. Sorbent performance is the key to their technical feasibility. Two sorbents (a limestone and a dolomite) were tested in a pressurized thermogravimetric analyzer (PTGA). The sorbent behaviors were explained based on complex interaction between carbonation, sulfation, and direct sulfation. The best option involved using limestone or dolomite as a SO2-sorbent in a FBC combustor following cyclic CO2 capture. Highly sintered limestone is a good sorbent for SO2 because of the generation of macropores during calcination/carbonation cycling.

High-Surface-Area CO2 Sponge: High Performance CO2 Scrubbing Based on Hollow Fiber-Supported Designer Ionic Liquid Sponges

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

IMPACCT Project: The team from ORNL and Georgia Tech is developing a new technology that will act like a sponge, integrating a new, alcohol-based ionic liquid into hollow fibers (magnified image, right) to capture CO2 from the exhaust produced by coal-fired power plants. Ionic liquids, or salts that exist in liquid form, are promising materials for carbon capture and storage, but their tendency to thicken when combined with CO2 limits their efficiency and poses a challenge for their development as a cost-effective alternative to current-generation solutions. Adding alcohol to the mix limits this tendency to thicken in the presence ofmore » CO2 but can also make the liquid more likely to evaporate, which would add significantly to the cost of CO2 capture. To solve this problem, ORNL is developing new classes of ionic liquids with high capacity for absorbing CO2. ORNL’s sponge would reduce the cost associated with the energy that would need to be diverted from power plants to capture CO2 and release it for storage.« less

Bench Scale Process for Low Cost CO 2 Capture Using a PhaseChanging Absorbent: Techno-Economic Analysis Topical Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Miebach, Barbara; McDuffie, Dwayne; Spiry, Irina

The objective of this project is to design and build a bench-scale process for a novel phase-changing CO 2 capture solvent. The project will establish scalability and technical and economic feasibility of using a phase-changing CO 2 capture absorbent for post-combustion capture of CO 2 from coal-fired power plants with 90% capture efficiency and 95% CO 2 purity at a cost of $40/tonne of CO 2 captured by 2025 and a cost of <$10/tonne of CO 2 captured by 2035. This report presents system and economic analysis for a process that uses a phase changing aminosilicone solvent to remove COmore » 2 from pulverized coal (PC) power plant flue gas. The aminosilicone solvent is a pure 1,3-bis(3-aminopropyl)-1,1,3,3-tetramethyldisiloxane (GAP-0). Performance of the phase-changing aminosilicone technology is compared to that of a conventional carbon capture system using aqueous monoethanolamine (MEA). This analysis demonstrates that the aminosilicone process has significant advantages relative to an MEA-based system. The first-year CO 2 removal cost for the phase-changing CO 2 capture process is $52.1/tonne, compared to $66.4/tonne for the aqueous amine process. The phase-changing CO 2 capture process is less costly than MEA because of advantageous solvent properties that include higher working capacity, lower corrosivity, lower vapor pressure, and lower heat capacity. The phase-changing aminosilicone process has approximately 32% lower equipment capital cost compared to that of the aqueous amine process. However, this solvent is susceptible to thermal degradation at CSTR desorber operating temperatures, which could add as much as $88/tonne to the CO 2 capture cost associated with solvent makeup. Future work is focused on mitigating this critical risk by developing an advanced low-temperature desorber that can deliver comparable desorption performance and significantly reduced thermal degradation rate.« less

Hybrid Membrane/Absorption Process for Post-combustion CO2 Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Shiguang; Shou, S.; Pyrzynski, Travis

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 leastmore » 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% CO2 product purity was achieved throughout the test. Membrane contactor modules have been scaled from bench scale 2-inch diameter by 12-inch long (20 ft2 membrane surface area) modules to 4-inch diameter by 60-inch long pilot scale modules (165 ft2 membrane surface area). Pilot scale modules were tested in an integrated absorption/regeneration system for CO2 capture field tests at a coal-fired power plant (Midwest Generation’s Will County Station located in Romeoville, IL). Absorption and regeneration contactors were constructed utilizing high performance super-hydrophobic, nano-porous PEEK membranes with CO2 gas permeance of 2,000 GPU and a 1,000 GPU, respectively. Field tests using aMDEA solvent achieved greater than 90% CO2 removal in a single stage. The absorption mass transfer coefficient was 1.2 (sec)-1, exceeding the initial target of 1.0 (sec)-1. This mass transfer coefficient is over one order of magnitude greater than that of conventional gas/liquid contacting equipment. The economic evaluation based on field tests data indicates that the CO2 capture cost associated with membrane contactor technology is $54.69 (Yr 2011$)/tonne of CO2 captured when using aMDEA as a solvent. It is projected that the DOE’s 2025 cost goal of $40 (Yr 2011$)/tonne of CO2 captured can be met by decreasing membrane module cost and by utilizing advanced CO2 capture solvents. In the second stage of the field test, an advanced solvent, Hitachi’s H3-1 was utilized. The use of H3-1 solvent increased mass transfer coefficient by 17% as compared to aMDEA solvent. The high mass transfer coefficient of H3-1 solvent combined with much more favorable solvent regeneration requirements, indicate that the projected savings achievable with membrane contactor process can be further improved. H3-1 solvent will be used in the next pilot-scale development phase. The integrated absorption/regeneration process design and high performance membrane contactors developed in the current bench-scale program will be used as the base technology for future pilot-scale development.« less

An Integrated, Low Temperature Process to Capture and Sequester Carbon Dioxide from Industrial Emissions

NASA Astrophysics Data System (ADS)

Wendlandt, R. F.; Foremski, J. J.

2013-12-01

Laboratory experiments show that it is possible to integrate (1) the chemistry of serpentine dissolution, (2) capture of CO2 gas from the combustion of natural gas and coal-fired power plants using aqueous amine-based solvents, (3) long-term CO2 sequestration via solid phase carbonate precipitation, and (4) capture solvent regeneration with acid recycling in a single, continuous process. In our process, magnesium is released from serpentine at 300°C via heat treatment with ammonium sulfate salts or at temperatures as low as 50°C via reaction with sulfuric acid. We have also demonstrated that various solid carbonate phases can be precipitated directly from aqueous amine-based (NH3, MEA, DMEA) CO2 capture solvent solutions at room temperature. Direct precipitation from the capture solvent enables regenerating CO2 capture solvent without the need for heat and without the need to compress the CO2 off gas. We propose that known low-temperature electrochemical methods can be integrated with this process to regenerate the aqueous amine capture solvent and recycle acid for dissolution of magnesium-bearing mineral feedstocks and magnesium release. Although the direct precipitation of magnesite at ambient conditions remains elusive, experimental results demonstrate that at temperatures ranging from 20°C to 60°C, either nesquehonite Mg(HCO3)(OH)●2H2O or a double salt with the formula [NH4]2Mg(CO3)2●4H2O or an amorphous magnesium carbonate precipitate directly from the capture solvent. These phases are less desirable for CO2 sequestration than magnesite because they potentially remove constituents (water, ammonia) from the reaction system, reducing the overall efficiency of the sequestration process. Accordingly, the integrated process can be accomplished with minimal energy consumption and loss of CO2 capture and acid solvents, and a net generation of 1 to 4 moles of H2O/6 moles of CO2 sequestered (depending on the solid carbonate precipitate and amount of produced H2 and O2 gas reacted to produce heat and water). Features of the integrated process include the following: 1) the four separate processes have compatible chemistry, enabling design of an integrated, continuous process scheme for CO2 capture and sequestration; 2) all 4 stages of the process can be conducted at ambient or slightly elevated temperatures; 3) precipitating carbonate directly from the capture solvent eliminates the need for costly CO2 gas compression; and 4) recycling the acid used for serpentine dissolution and the solvent used for CO2 capture reduces feed stock costs.

Enabling CCS via Low-temperature Geothermal Energy Integration for Fossil-fired Power Generation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Davidson, Casie L.; Heldebrant, D. J.; Bearden, M. D.

Here, among the key barriers to commercial scale deployment is the cost associated with CO 2 capture. This is particularly true for existing large, fossil-fired assets that account for a large fraction of the electricity generation fleet in developed nations, including the U.S. Fitting conventional combustion technologies with CO 2 capture systems can carry an energy penalty of thirty percent or more, resulting in an increased price of power to the grid, as well as an overall decrease in net plant output. Taken together with the positive growth in demand for electricity, this implies a need for accelerated capital build-outmore » in the power generation markets to accommodate both demand growth and decreased output at retrofitted plants. In this paper, the authors present the results of a study to assess the potential to use geothermal energy to provide boiler feedwater preheating, capturing efficiency improvements designed to offset the losses associated with CO 2 capture. Based on NETL benchmark cases and subsequent analysis of the application using site-specific data from the North Valmy power plant, several cases for CO 2 capture were evaluated. These included geothermally assisted MEA capture, CO2BOLs capture, and stand-alone hybrid power generation, compared with a baseline, no-geothermal case. Based on Case 10, and assuming 2.7 MMlb/h of geothermally sourced 150 ºC water, the parasitic power load associated with MEA capture could be offset by roughly seven percent, resulting in a small (~1 percent) overall loss to net power generation, but at levelized costs of electricity similar to the no-geothermal CCS case. For the CO 2BOLs case, the availability of 150°C geothermal fluid could allow the facility to not only offset the net power decrease associated with CO 2BOLs capture alone, but could increase nameplate capacity by two percent. The geothermally coupled CO 2BOLs case also decreases LCOE by 0.75 ¢/kWh relative to the non-hybrid CO 2BOLs case, with the improved performance over the MEA case driven by the lower regeneration temperature and associated duty for CO 2BOLs relative to MEA.« less

Enabling CCS via Low-temperature Geothermal Energy Integration for Fossil-fired Power Generation

DOE PAGES

Davidson, Casie L.; Heldebrant, D. J.; Bearden, M. D.; ...

2017-08-18

Here, among the key barriers to commercial scale deployment is the cost associated with CO 2 capture. This is particularly true for existing large, fossil-fired assets that account for a large fraction of the electricity generation fleet in developed nations, including the U.S. Fitting conventional combustion technologies with CO 2 capture systems can carry an energy penalty of thirty percent or more, resulting in an increased price of power to the grid, as well as an overall decrease in net plant output. Taken together with the positive growth in demand for electricity, this implies a need for accelerated capital build-outmore » in the power generation markets to accommodate both demand growth and decreased output at retrofitted plants. In this paper, the authors present the results of a study to assess the potential to use geothermal energy to provide boiler feedwater preheating, capturing efficiency improvements designed to offset the losses associated with CO 2 capture. Based on NETL benchmark cases and subsequent analysis of the application using site-specific data from the North Valmy power plant, several cases for CO 2 capture were evaluated. These included geothermally assisted MEA capture, CO2BOLs capture, and stand-alone hybrid power generation, compared with a baseline, no-geothermal case. Based on Case 10, and assuming 2.7 MMlb/h of geothermally sourced 150 ºC water, the parasitic power load associated with MEA capture could be offset by roughly seven percent, resulting in a small (~1 percent) overall loss to net power generation, but at levelized costs of electricity similar to the no-geothermal CCS case. For the CO 2BOLs case, the availability of 150°C geothermal fluid could allow the facility to not only offset the net power decrease associated with CO 2BOLs capture alone, but could increase nameplate capacity by two percent. The geothermally coupled CO 2BOLs case also decreases LCOE by 0.75 ¢/kWh relative to the non-hybrid CO 2BOLs case, with the improved performance over the MEA case driven by the lower regeneration temperature and associated duty for CO 2BOLs relative to MEA.« less

Development of Novel Carbon Sorbents for CO{sub 2} Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krishnan, Gopala; Hornbostel, Marc; Bao, Jianer

2013-11-30

An innovative, low-cost, and low-energy-consuming carbon dioxide (CO{sub 2}) capture technology was developed, based on CO{sub 2}adsorption on a high-capacity and durable carbon sorbent. This report describes the (1) performance of the concept on a bench-scale system; (2) results of parametric tests to determine the optimum operating conditions; (3) results of the testing with a flue gas from coal-fired boilers; and (4) evaluation of the technical and economic viability of the technology. The process uses a falling bed of carbon sorbent microbeads to separate the flue gas into two streams: a CO{sub 2} -lean flue gas stream from which >more » 90% of the CP{sub 2} is removed and a pure stream of CO{sub 2} that is ready for compression and sequestration. The carbo sorbent microbeads have several unique properties such as high CO{sub 2} capacity, low heat of adsorption and desorption (25 to 28 kJ/mole), mechanically robust, and rapid adsorption and desorption rates. The capture of CO{sub 2} from the flue gas is performed at near ambient temperatures in whic the sorbent microbeads flow down by gravity counter-current with the up-flow of the flue gas. The adsorbed CO{sub 2} is stripped by heating the CO{sub 2}-loaded sorbent to - 100°C, in contact with low-pressure (- 5 psig) steam in a section at the bottom of the adsorber. The regenerated sorben is dehydrated of adsorbed moisture, cooled, and lifted back to the adsorber. The CO{sub 2} from the desorber is essentially pure and can be dehydrated, compressed, and transported to a sequestration site. Bench-scale tests using a simulated flue gas showed that the integrated system can be operated to provide > 90% CO{sub 2} capture from a 15% CO{sub 2} stream in the adsorber and produce > 98% CO{sub 2} at the outlet of the stripper. Long-term tests ( 1,000 cycles) showed that the system can be operated reliably without sorbent agglomeration or attrition. The bench-scale reactor was also operated using a flue gas stream from a coal-fired boil at the University of Toledo campus for about 135 h, comprising 7,000 cycles of adsorption and desorption using the desulfurized flue gas that contained only 4.5% v/v CO{sub 2}. A capture efficiency of 85 to 95% CO{sub 2} was achieved under steady-state conditi ons. The CO{sub 2} adsorption capacity did not change significantly during the field test, as determined from the CO{sub 2} adsorptio isotherms of fresh and used sorbents. The process is also being tested using the flue gas from a PC-fired power plant at the National Carbon Capture Center (NCCC), Wilsonville, AL. The cost of electricity was calculated for CO{sub 2} capture using the carbon sorbent and compared with the no-CO{sub 2} capture and CO{sub 2} capture with an amine-based system. The increase i the levelized cost of electricity (L-COE) is about 37% for CO{sub 2} capture using the carbon sorbent in comparison to 80% for an amine-based system, demonstrating the economic advantage of C capture using the carbon sorbent. The 37% increase in the L-COE corresponds to a cost of capture of $30/ton of CO{sub 2}, including compression costs, capital cost for the capture system, and increased plant operating and capital costs to make up for reduced plant efficiency. Preliminary sensitivity analyses showed capital costs, pressure drops in the adsorber, and steam requirement for the regenerator are the major variables in determining the cost of CO{sub 2} capture. The results indicate that further long-term testing with a flue gas from a pulverized coal­ fired boiler should be performed to obtain additional data relating to the effects of flue gas contaminants, the ability to reduce pressure drop by using alternate structural packing , and the use of low-cost construction materials.« less

Graphene-based porous silica sheets impregnated with polyethyleneimine for superior CO2 capture.

PubMed

Yang, Shubin; Zhan, Liang; Xu, Xiaoyue; Wang, Yanli; Ling, Licheng; Feng, Xinliang

2013-04-18

It is demonstrated that graphene-based porous silica sheets can serve as an efficient carrier support for PEI via a simple nanocasting technology. The resulting materials possess thin nature, high PEI loading content and high thermal-conductivity. Such features are favorable for the efficient diffusion and adsorption of CO2 as well as the rapid thermal transfer during the CO2 capture process. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Low Cost, High Capacity Regenerable Sorbent for Carbon Dioxide Capture from Existing Coal-fired Power Plants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Alptekin, Gokhan; Jayaraman, Ambalavanan; Dietz, Steven

In this project TDA Research, Inc (TDA) has developed a new post combustion carbon capture technology based on a vacuum swing adsorption system that uses a steam purge and demonstrated its technical feasibility and economic viability in laboratory-scale tests and tests in actual coal derived flue gas. TDA uses an advanced physical adsorbent to selectively remove CO 2 from the flue gas. The sorbent exhibits a much higher affinity for CO 2 than N 2, H 2O or O 2, enabling effective CO 2 separation from the flue gas. We also carried out a detailed process design and analysis ofmore » the new system as part of both sub-critical and super-critical pulverized coal fired power plants. The new technology uses a low cost, high capacity adsorbent that selectively removes CO 2 in the presence of moisture at the flue gas temperature without a need for significant cooling of the flue gas or moisture removal. The sorbent is based on a TDA proprietary mesoporous carbon that consists of surface functionalized groups that remove CO 2 via physical adsorption. The high surface area and favorable porosity of the sorbent also provides a unique platform to introduce additional functionality, such as active groups to remove trace metals (e.g., Hg, As). In collaboration with the Advanced Power and Energy Program of the University of California, Irvine (UCI), TDA developed system simulation models using Aspen PlusTM simulation software to assess the economic viability of TDA’s VSA-based post-combustion carbon capture technology. The levelized cost of electricity including the TS&M costs for CO 2 is calculated as $116.71/MWh and $113.76/MWh for TDA system integrated with sub-critical and super-critical pulverized coal fired power plants; much lower than the $153.03/MWhand $147.44/MWh calculated for the corresponding amine based systems. The cost of CO 2 captured for TDA’s VSA based system is $38.90 and $39.71 per tonne compared to $65.46 and $66.56 per tonne for amine based system on 2011 $ basis, providing 40% lower cost of CO 2 captured. In this analysis we have used a sorbent life of 4 years. If a longer sorbent life can be maintained (which is not unreasonable for fixed bed commercial PSA systems), this would lower the cost of CO 2 captured by $0.05 per tonne (e.g., to $38.85 and $39.66 per tonne at 5 years sorbent replacement). These system analysis results suggest that TDA’s VSA-based post-combustion capture technology can substantially improve the power plant’s thermal performance while achieving near zero emissions, including greater than 90% carbon capture. The higher net plant efficiency and lower capital and operating costs results in a substantial reduction in the cost of carbon capture and cost of electricity for the power plant equipped with TDA’s technology.« less

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

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 (H 2 ), with and without carbon dioxide (CO 2 ) 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 CO 2 capture. The performances of the above three capture technologies were compared with respect to energetic and exergetic efficiencies, and the level of CO 2 emission. The effect of air separation unit (ASU) and gas turbine (GT) integration on the power output of all the CO 2 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 CO 2 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 H 2 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.

Computational designing and screening of solid materials for CO2capture

NASA Astrophysics Data System (ADS)

Duan, Yuhua

In this presentation, we will update our progress on computational designing and screening of solid materials for CO2 capture. 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 have been proposed and validated at NETL. The advantage of this method is that it identifies the thermodynamic properties of the CO2 capture reaction as a function of temperature and pressure without any experimental input beyond crystallographic structural information of the solid phases involved. 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 identify only those solid materials for which lower capture energy costs are expected at the desired working conditions. In addition, we present a simulation scheme to increase and decrease the turnover temperature (Tt) of solid capturing CO2 reaction by mixing other solids. Our results also show that some solid sorbents can serve as bi-functional materials: CO2 sorbent and CO oxidation catalyst. Such dual functionality could be used for removing both CO and CO2 after water-gas-shift to obtain pure H2.

Ultrafast and Stable CO2 Capture Using Alkali Metal Salt-Promoted MgO-CaCO3 Sorbents.

PubMed

Cui, Hongjie; Zhang, Qiming; Hu, Yuanwu; Peng, Chong; Fang, Xiangchen; Cheng, Zhenmin; Galvita, Vladimir V; Zhou, Zhiming

2018-06-20

As a potential candidate for precombustion CO 2 capture at intermediate temperatures (200-400 °C), MgO-based sorbents usually suffer from low kinetics and poor cyclic stability. Herein, a general and facile approach is proposed for the fabrication of high-performance MgO-based sorbents via incorporation of CaCO 3 into MgO followed by deposition of a mixed alkali metal salt (AMS). The AMS-promoted MgO-CaCO 3 sorbents are capable of adsorbing CO 2 at an ultrafast rate, high capacity, and good stability. The CO 2 uptake of sorbent can reach as high as above 0.5 g CO 2 g sorbent -1 after only 5 min of sorption at 350 °C, accounting for vast majority of the total uptake. In addition, the sorbents are very stable even under severe but more realistic conditions (desorption in CO 2 at 500 °C), where the CO 2 uptake of the best sorbent is stabilized at 0.58 g CO 2 g sorbent -1 in 20 consecutive cycles. The excellent CO 2 capture performance of the sorbent is mainly due to the promoting effect of molten AMS, the rapid formation of CaMg(CO 3 ) 2 , and the plate-like structure of sorbent. The exceptional ultrafast rate and the good stability of the AMS-promoted MgO-CaCO 3 sorbents promise high potential for practical applications, such as precombustion CO 2 capture from integrated gasification combined cycle plants and sorption-enhanced water gas shift process.

Computational Modeling of Mixed Solids for CO2 CaptureSorbents

DOE Office of Scientific and Technical Information (OSTI.GOV)

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 differentmore » 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.« less

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Jian; Kutnyakov, Igor; Koech, Phillip K.

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

Tandem mass spectrometry measurement of the collision products of carbamate anions derived from CO2 capture sorbents: paving the way for accurate quantitation.

PubMed

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

2011-08-01

The reaction between CO(2) 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,-d(4)-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 CO(2) 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 (-CO(2), 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 ((-)O(2)CNHC(2)H(4)NHCO(2)(-)) commonly encountered in CO(2) 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 CO(2) capture products could lead to dynamic operational tuning of CO(2) capture-plants and, thus, cost-savings via real-time manipulation of solvent regeneration energies.

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.

Oxidatively-Stable Linear Poly(propylenimine)-Containing Adsorbents for CO2 Capture from Ultra-Dilute Streams.

PubMed

Pang, Simon H; Lively, Ryan P; Jones, Christopher W

2018-05-29

Aminopolymer-based solid sorbents have been widely investigated for CO2 capture from dilute streams such as flue gas or ambient air. However, the oxidative stability of the most well-studied aminopolymer, poly(ethylenimine) (PEI), is limited, causing it to lose its CO2 capture capacity after exposure to oxygen at elevated temperatures. Here we demonstrate the use of linear poly(propylenimine) (PPI), synthesized via a simple cationic ring-opening polymerization, as a more oxidatively-stable alternative to PEI with high CO2 capacity and amine efficiency. The performance of linear PPI/SBA-15 composites is investigated over a range of CO2 capture conditions (CO2 partial pressure, adsorption temperature) to examine the trade-off between adsorption capacity and sorption site accessibility, which may be expected to be more limited in linear polymers relative to the prototypical hyperbranched PEI. Linear PPI/SBA-15 composites are more efficient at CO2 capture and retain 65-83% of their CO2 capacity after exposure to a harsh oxidative treatment, compared to 20-40% retention for linear PEI. Additionally, we demonstrate long-term stability of linear PPI sorbents over 50 adsorption/desorption cycles with no loss in performance. Combined with other strategies for improving oxidative stability and adsorption kinetics, linear PPI may play a role as a component of stable, solid adsorbents in commercial applications for CO2 capture. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Life cycle assessment of carbon capture and utilization from ammonia process in Mexico.

PubMed

Morales Mora, M A; Vergara, C Pretelín; Leiva, M A; Martínez Delgadillo, S A; Rosa-Domínguez, E R

2016-12-01

Post-combustion CO 2 capture (PCC) of flue gas from an ammonia plant (AP) and the environmental performance of the carbon capture utilization (CCU) technology for greenhouse gas (GHG) emissions to an enhanced oil recovery (EOR) system in Mexico was performed as case study. The process simulations (PS) and life cycle assessment (LCA) were used as supporting tools to quantify the CO 2 capture and their environmental impacts, respectively. Two scenarios were considered: 1) the AP with its shift and CO 2 removal unit and 2) Scenario 1 plus PCC of the flue gas from the AP primary reformer (AP-2CO 2 ) and the global warming (GW) impact. Also, the GW of the whole of a CO 2 -EOR project, from these two streams of captured CO 2 , was evaluated. Results show that 372,426 tCO 2 /year can be PCC from the flue gas of the primary reformer and 480,000 tons/y of capacity from the AP. The energy requirement for solvent regeneration is estimated to be 2.8 MJ/kgCO 2 or a GW impact of 0.22 kgCO 2e /kgCO 2 captured. GW performances are 297.6 kgCO 2e emitted/barrel (bbl) for scenario one, and 106.5 kgCO 2e emitted/bbl for the second. The net emissions, in scenario one, were 0.52 tCO 2e /bbl and 0.33 tCO 2e /bbl in scenario two. Based on PS, this study could be used to evaluate the potential of CO 2 capture of 4080 t/d of 4 ammonia plants. The integration of PS-LCA to a PCC study allows the applicability as methodological framework for the development of a cluster of projects in which of CO 2 could be recycled back to fuel, chemical, petrochemical products or for enhanced oil recovery (EOR). With AP-2CO 2, "CO 2 emission free" ammonia production could be achieved. Copyright © 2016 Elsevier Ltd. All rights reserved.

Ab initio thermodynamic approach to identify mixed solid sorbents for CO 2 capture technology

DOE PAGES

Duan, Yuhua

2015-10-15

Because the current technologies for capturing CO 2 are still too energy intensive, new materials must be developed that can capture CO 2 reversibly with acceptable energy costs. At a given CO 2 pressure, the turnover temperature (T t) of the reaction of an individual solid that can capture CO 2 is fixed. Such T t may be outside the operating temperature range (ΔT o) for a practical capture technology. To adjust T t to fit the practical ΔT o, in this study, three scenarios of mixing schemes are explored by combining thermodynamic database mining with first principles density functionalmore » theory and phonon lattice dynamics calculations. Our calculated results demonstrate that by mixing different types of solids, it’s possible to shift T t 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 CO 2 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

High CO2 absorption capacity by chemisorption at cations and anions in choline-based ionic liquids.

PubMed

Bhattacharyya, Shubhankar; Filippov, Andrei; Shah, Faiz Ullah

2017-11-29

The effect of CO 2 absorption on the aromaticity and hydrogen bonding in ionic liquids is investigated. Five different ionic liquids with choline based cations and aprotic N-heterocyclic anions were synthesized. Purity and structures of the synthesized ionic liquids were characterized by 1 H and 13 C NMR spectroscopy. CO 2 capture performance was studied at 20 °C and 40 °C under three different pressures (1, 3, 6 bar). The IL [N 1,1,6,2OH ][4-Triz] showed the highest CO 2 capture capacity (28.6 wt%, 1.57 mol of CO 2 per mol of the IL, 6.48 mol of CO 2 per kg of the ionic liquid) at 20 °C and 1 bar. The high CO 2 capture capacity of the [N 1,1,6,2OH ][4-Triz] IL is due to the formation of carbonic acid (-OCO 2 H) together with carbamate by participation of the -OH group of the [N 1,1,6,2OH ] + cation in the CO 2 capture process. The structure of the adduct formed by CO 2 reaction with the IL [N 1,1,6,2OH ][4-Triz] was probed by using IR, 13 C NMR and 1 H- 13 C HMBC NMR experiments utilizing 13 C labeled CO 2 gas. 1 H and 13 C PFG NMR studies were performed before and after CO 2 absorption to explore the effect of cation-anion structures on the microscopic ion dynamics in ILs. The ionic mobility was significantly increased after CO 2 reaction due to lowering of aromaticity in the case of ILs with aromatic N-heterocyclic anions.

Synthesis of highly efficient CaO-based, self-stabilizing CO2 sorbents via structure-reforming of steel slag.

PubMed

Tian, Sicong; Jiang, Jianguo; Yan, Feng; Li, Kaimin; Chen, Xuejing

2015-06-16

Capturing anthropogenic CO2 in a cost-effective and highly efficient manner is one of the most challenging issues faced by scientists today. Herein, we report a novel structure-reforming approach to convert steel slag, a cheap, abundant, and nontoxic calcium-rich industrial waste, as the only feedstock into superior CaO-based, self-stabilizing CO2 sorbents. The CO2 capture capacity of all the steel slag-derived sorbents was improved more than 10-fold compared to the raw slag, with the maximum uptake of CO2 achieving at 0.50 gCO2 gsorbent(-1). Additionally, the initial steel slag-derived sorbent could retain 0.25 gCO2 gsorbent(-1), that is, a decay rate of only 12% over 30 carbonation-calcination cycles, the excellent self-stabilizing property allowed it to significantly outperform conventional CaO, and match with most of the existing synthetic CaO-based sorbents. A synergistic effect that facilitated CO2 capture by CaO-based sorbents was clearly recognized when Mg and Al, the most common elements in steel slag, coexisted with CaO in the forms of MgO and Al2O3, respectively. During the calcium looping process, MgO served as a well spacer to increase the porosity of sorbents together with Al2O3 serving as a durable stabilizer to coresist the sintering of CaCO3 grains at high temperatures.

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.

Reinventing Design Principles for Developing Low-Viscosity Carbon Dioxide-Binding Organic Liquids for Flue Gas Clean Up

DOE Office of Scientific and Technical Information (OSTI.GOV)

None, None

2017-01-11

Anthropogenic carbon dioxide (CO 2) emission from point sources, such as coal fired-power plants, account for the majority of the green houses gasses in the atmosphere. Capture, storage and utilization are required to mitigate adverse environmental effects. Aqueous amine-based CO 2 capture solvents are currently considered the industry standard, but deployment to market is limited by their high regeneration energy demand. In that context, energy efficient and less-viscous water-lean transformational solvent systems known as CO 2 Binding Organic Liquids (CO 2BOLs) are being developed in our group to advance this technology to commercialization. Herein, we present a logical design approachmore » based on fundamental concepts of organic chemistry and computer simulations aimed at lowering solvent viscosity. Conceptually, viscosity reduction would be achieved by systemmatic methods such as introduction of steric hindrance on the anion to minimize the intermolecular cation-anion interactions, fine tuning the electronics, hydrogen bonding orientation and strength, and charge solvation. Conventional standard trial-and-error approaches while effective, are time consuming and economically expensive. Herein, we rethink the metrics and design principles of low-viscosity CO 2 capture solvents using a combined synthesis and computational modeling approach. We critically study the impacts of modyfying factors such as as orientation of hydrogen bonding, introduction of higher degrees of freedom and cation or anion charge solvation and assess if or how each factor impacts viscosity of CO 2BOL CO 2 capture solvents. Ultimately, we found that hydrogen bond orientation and strength is predominantly influencing the viscosity in CO 2BOL solvents. With this knowledge, a new 1-MEIPADM-2-BOL CO 2BOL variant was synthesized and tested, resulting in a solvent that is approximately 60% less viscous at 25 mol% CO 2 loading with respect to our base compound 1-IPADM-2-BOL. The insights gained from the current study redefines the fundamental concepts and understanding of what influences viscosity in concentrated organic CO 2 capture solvents.« less

Balsam-Pear-Skin-Like Porous Polyacrylonitrile Nanofibrous Membranes Grafted with Polyethyleneimine for Postcombustion CO2 Capture.

PubMed

Zhang, Yufei; Guan, Jiming; Wang, Xianfeng; Yu, Jianyong; Ding, Bin

2017-11-22

Amine-containing sorbents have been extensively studied for postcombustion carbon dioxide (CO 2 ) capture because of their ability to chemisorb CO 2 from the flue gas. However, most sorbents are in the form of powders currently, which is not the ideal configuration for the flue gas separation because of the fragile nature and poor mechanical properties, resulting in blocking of the flow pipes and difficult recycling. Herein, we present a novel approach for the facile fabrication of flexible, robust, and polyethyleneimine-grafted (PEI-grafted) hydrolyzed porous PAN nanofibrous membranes (HPPAN-PEI NFMs) through the combination of electrospinning, pore-forming process, hydrolysis reaction, and the subsequent grafting technique. Excitingly, we find that all the resultant porous PAN (PPAN) fibers exhibit a balsam-pear-skin-like porous structure due to the selective removal of poly(vinylpyrrolidone) (PVP) from PAN/PVP fibers by water extraction. Significantly, the HPPAN-PEI NFMs retain their mesoporosity, as well as exhibit good thermal stability and prominent tensile strength (11.1 MPa) after grafting, guaranteeing their application in CO 2 trapping from the flue gas. When exposed to CO 2 at 40 °C, the HPPAN-PEI NFMs show an enhanced CO 2 adsorption capacity of 1.23 mmol g -1 (based on the overall quantity of the sample) or 6.15 mmol g -1 (based on the quantity of grafted PEI). Moreover, the developed HPPAN-PEI NFMs display significantly selective capture for CO 2 over N 2 and excellent recyclability. The CO 2 capacity retains 92% of the initial value after 20 adsorption-desorption cycle tests, indicating that the resultant HPPAN-PEI NFMs have good long-term stability. This work paves the way for fabricating NFM-based solid adsorption materials endowed with a porous structure applied to efficient postcombustion CO 2 capture.

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

NASA Astrophysics Data System (ADS)

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

2017-03-01

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

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

PubMed

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

2017-03-06

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

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

PubMed Central

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

2017-01-01

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

Theoretical calculating the thermodynamic properties of solid sorbents for CO{sub 2} capture applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Duan, Yuhua

2012-11-02

Since current technologies for capturing CO{sub 2} to fight global climate change are still too energy intensive, there is a critical need for development of new materials that can capture CO{sub 2} reversibly with acceptable energy costs. Accordingly, solid sorbents have been proposed to be used for CO{sub 2} 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 CO{sub 2} sorbent candidates from the vast array of possible solid materials has been proposed and validated. The calculatedmore » thermodynamic properties of different classes of solid materials versus temperature and pressure changes were further used to evaluate the equilibrium properties for the CO{sub 2} adsorption/desorption cycles. According to the requirements imposed by the pre- and post- combustion technologies and based on our calculated thermodynamic properties for the CO{sub 2} 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 CO{sub 2} sorbent candidates were further considered for experimental validations. The ab initio thermodynamic technique has the advantage of identifying thermodynamic properties of CO{sub 2} 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 first introduce our screening methodology and the results on a testing set of solids with known thermodynamic properties to validate our methodology. Then, by applying our computational method to several different kinds of solid systems, we demonstrate that our methodology can predict the useful information to help developing CO{sub 2} capture Technologies.« less

CaO-based CO2 sorbents: from fundamentals to the development of new, highly effective materials.

PubMed

Kierzkowska, Agnieszka M; Pacciani, Roberta; Müller, Christoph R

2013-07-01

The enormous anthropogenic emission of the greenhouse gas CO2 is most likely the main reason for climate change. Considering the continuing and indeed growing utilisation of fossil fuels for electricity generation and transportation purposes, development and implementation of processes that avoid the associated emissions of CO2 are urgently needed. CO2 capture and storage, commonly termed CCS, would be a possible mid-term solution to reduce the emissions of CO2 into the atmosphere. However, the costs associated with the currently available CO2 capture technology, that is, amine scrubbing, are prohibitively high, thus making the development of new CO2 sorbents a highly important research challenge. Indeed, CaO, readily obtained through the calcination of naturally occurring limestone, has been proposed as an alternative CO2 sorbent that could substantially reduce the costs of CO2 capture. However, one of the major drawbacks of using CaO derived from natural sources is its rapidly decreasing CO2 uptake capacity with repeated carbonation-calcination reactions. Here, we review the current understanding of fundamental aspects of the cyclic carbonation-calcination reactions of CaO such as its reversibility and kinetics. Subsequently, recent attempts to develop synthetic, CaO-based sorbents that possess high and cyclically stable CO2 uptakes are presented. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ultralow Parasitic Energy for Postcombustion CO 2 Capture Realized in a Nickel Isonicotinate Metal–Organic Framework with Excellent Moisture Stability

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nandi, Shyamapada; Collins, Sean; Chakraborty, Debanjan

2017-01-25

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

Lime-Based Sorbents for High-Temperature CO2 Capture—A Review of Sorbent Modification Methods

PubMed Central

Manovic, Vasilije; Anthony, Edward J.

2010-01-01

This paper presents a review of the research on CO2 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 CO2 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 CO2 capture, and a calciner—a unit for CaO regeneration. However, even though natural materials are cheap and abundant and very good candidates as solid CO2 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

Bench-Scale Silicone Process for Low-Cost CO{sub 2} Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vipperla, Ravikumar; Yee, Michael; Steele, Ray

This report presents system and economic analysis for a carbon capture unit which uses an amino-silicone solvent for CO{sub 2} capture and sequestration (CCS) in a pulverized coal (PC) boiler. The amino-silicone solvent is based on GAP-1 with Tri-Ethylene Glycol (TEG) as a co-solvent. The report also shows results for a CCS unit based on a conventional approach using mono-ethanol amine (MEA). Models were developed for both processes and used to calculate mass and energy balances. Capital costs and energy penalty were calculated for both systems, as well as the increase in cost of electricity. The amino-silicone solvent based systemmore » demonstrates significant advantages compared to the MEA system.« less

Heat recovery from sorbent-based CO.sub.2 capture

DOEpatents

Jamal, Aqil; Gupta, Raghubir P

2015-03-10

The present invention provides a method of increasing the efficiency of exothermic CO.sub.2 capture processes. The method relates to withdrawing heat generated during the exothermic capture of CO.sub.2 with various sorbents via heat exchange with a working fluid. The working fluid is provided at a temperature and pressure such that it is in the liquid state, and has a vaporization temperature in a range such that the heat arising from the reaction of the CO.sub.2 and the sorbent causes a phase change from liquid to vapor state in whole or in part and transfers heat from to the working fluid. The resulting heated working fluid may subsequently be used to generate power.

Capturing molecular multimode relaxation processes in excitable gases based on decomposition of acoustic relaxation spectra

NASA Astrophysics Data System (ADS)

Zhu, Ming; Liu, Tingting; Wang, Shu; Zhang, Kesheng

2017-08-01

Existing two-frequency reconstructive methods can only capture primary (single) molecular relaxation processes in excitable gases. In this paper, we present a reconstructive method based on the novel decomposition of frequency-dependent acoustic relaxation spectra to capture the entire molecular multimode relaxation process. This decomposition of acoustic relaxation spectra is developed from the frequency-dependent effective specific heat, indicating that a multi-relaxation process is the sum of the interior single-relaxation processes. Based on this decomposition, we can reconstruct the entire multi-relaxation process by capturing the relaxation times and relaxation strengths of N interior single-relaxation processes, using the measurements of acoustic absorption and sound speed at 2N frequencies. Experimental data for the gas mixtures CO2-N2 and CO2-O2 validate our decomposition and reconstruction approach.

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

PubMed

Uma Maheswari, A; Palanivelu, K

2017-02-01

In this present work, the absorption of CO 2 in alkyl amines and vegetable oil mixture has been evaluated. The results showed that the absorption is higher in alkyl amines and vegetable oil mixture compared with the aqueous alkyl amines. In addition to that, by employing the greener and non-toxic vegetable oil media, the CO 2 gas has been captured as well as converted into value-added products, such as carbamates of ethylenediamine, diethylenetriamine, and triethylenetetramine. The carbamates have been isolated and characterized by Fourier transform infrared and 1 H and 13 C nuclear magnetic resonance spectroscopic techniques. The formation of these products in precipitate form has not been observed in the case of aqueous medium. Among the various alkyl amine and vegetable oil combinations, triethylenetetramine in coconut oil medium showed the maximum CO 2 capture capacity of 72%. The coconut oil used for the process has been recovered, recycled, and reused for 3 cycles. Thus, this novel scheme seems to be a better alternative to conquer the drawback of aqueous amine-based CO 2 capture as well as for the capture and utilization of the CO 2 gas to gain the value-added products.

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.

CO2 Capture by Injection of Flue Gas or CO2-N2 Mixtures into Hydrate Reservoirs: Dependence of CO2 Capture Efficiency on Gas Hydrate Reservoir Conditions.

PubMed

Hassanpouryouzband, Aliakbar; Yang, Jinhai; Tohidi, Bahman; Chuvilin, Evgeny; Istomin, Vladimir; Bukhanov, Boris; Cheremisin, Alexey

2018-04-03

Injection of flue gas or CO 2 -N 2 mixtures into gas hydrate reservoirs has been considered as a promising option for geological storage of CO 2 . However, the thermodynamic process in which the CO 2 present in flue gas or a CO 2 -N 2 mixture is captured as hydrate has not been well understood. In this work, a series of experiments were conducted to investigate the dependence of CO 2 capture efficiency on reservoir conditions. The CO 2 capture efficiency was investigated at different injection pressures from 2.6 to 23.8 MPa and hydrate reservoir temperatures from 273.2 to 283.2 K in the presence of two different saturations of methane hydrate. The results showed that more than 60% of the CO 2 in the flue gas was captured and stored as CO 2 hydrate or CO 2 -mixed hydrates, while methane-rich gas was produced. The efficiency of CO 2 capture depends on the reservoir conditions including temperature, pressure, and hydrate saturation. For a certain reservoir temperature, there is an optimum reservoir pressure at which the maximum amount of CO 2 can be captured from the injected flue gas or CO 2 -N 2 mixtures. This finding suggests that it is essential to control the injection pressure to enhance CO 2 capture efficiency by flue gas or CO 2 -N 2 mixtures injection.

Ca-Embedded C2N: an efficient adsorbent for CO2 capture.

PubMed

Liu, Yuzhen; Meng, Zhaoshun; Guo, Xiaojian; Xu, Genjian; Rao, Dewei; Wang, Yuhui; Deng, Kaiming; Lu, Ruifeng

2017-10-25

Carbon dioxide as a greenhouse gas causes severe impacts on the environment, whereas it is also a necessary chemical feedstock that can be converted into carbon-based fuels via electrochemical reduction. To efficiently and reversibly capture CO 2 , it is important to find novel materials for a good balance between adsorption and desorption. In this study, we performed first-principles calculations and grand canonical Monte Carlo (GCMC) simulations, to systematically study metal-embedded carbon nitride (C 2 N) nanosheets for CO 2 capture. Our first-principles results indicated that Ca atoms can be uniformly trapped in the cavity center of C 2 N structure, while the transition metals (Sc, Ti, V, Cr, Mn, Fe, Co) are favorably embedded in the sites off the center of the cavity. The determined maximum number of CO 2 molecules with strong physisorption showed that Ca-embedded C 2 N monolayer is the most promising CO 2 adsorbent among all considered metal-embedded materials. Moreover, GCMC simulations revealed that at room temperature the gravimetric density for CO 2 adsorbed on Ca-embedded C 2 N reached 50 wt% at 30 bar and 23 wt% at 1 bar, higher than other layered materials, thus providing a satisfactory system for the CO 2 capture and utilization.

CO 2 Capture by Cold Membrane Operation with Actual Power Plant Flue Gas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chaubey, Trapti; Kulkarni, Sudhir; Hasse, David

The main objective of the project was to develop a post-combustion CO 2 capture process based on the hybrid cold temperature membrane operation. The CO 2 in the flue gas from coal fired power plant is pre-concentrated to >60% CO 2 in the first stage membrane operation followed by further liquefaction of permeate stream to achieve >99% CO 2 purity. The aim of the project was based on DOE program goal of 90% CO 2 capture with >95% CO 2 purity from Pulverized Coal (PC) fired power plants with $40/tonne of carbon capture cost by 2025. The project moves themore » technology from TRL 4 to TRL 5. The project involved optimization of Air Liquide commercial 12” PI-1 bundle to improve the bundle productivity by >30% compared to the previous baseline (DE-FE0004278) using computational fluid dynamics (CFD) modeling and bundle testing with synthetic flue gas at 0.1 MWe bench scale skid located at Delaware Research and Technology Center (DRTC). In parallel, the next generation polyimide based novel PI-2 membrane was developed with 10 times CO 2 permeance compared to the commercial PI-1 membrane. The novel PI-2 membrane was scaled from mini-permeator to 1” permeator and 1” bundle for testing. Bundle development was conducted with a Development Spin Unit (DSU) installed at MEDAL. Air Liquide’s cold membrane technology was demonstrated with real coal fired flue gas at the National Carbon Capture Center (NCCC) with a 0.3 MWe field-test unit (FTU). The FTU was designed to incorporate testing of two PI-1 commercial membrane bundles (12” or 6” diameter) in parallel or series. A slip stream was sent to the next generation PI-2 membrane for testing with real flue gas. The system exceeded performance targets with stable PI-1 membrane operation for over 500 hours of single bundle, steady state testing. The 12” PI-1 bundle exceeded the productivity target by achieving ~600 Nm3/hr, where the target was set at ~455 Nm3/hr at 90% capture rate. The cost of 90% CO 2 capture from a 550 MWe net coal power plant was estimated between 40 and $45/tonne. A 6” PI-1 bundle exhibited superior bundle performance compared to the 12” PI-1 bundle. However, the carbon capture cost was not lower with the 6” PI-1 bundle due to the higher bundle installed cost. A 1” PI-1 bundle was tested to compare bundles with different length / diameter ratios. This bundle exhibited the lowest performance due to the different fiber winding pattern and increased bundle non-ideality. Several long-term and parametric tests were conducted with 3,200 hours of total run-time at NCCC. Finally, the new PI-2 membrane fiber was tested at a small scale (1” modules) in real flue gas and exhibited up to 10 times the CO 2 permeance and slightly lower CO 2/N 2 selectivity as the commercial PI-1 fiber. This corresponded to a projected 4 - 5 times increase in the productivity per bundle and a potential cost reduction of $3/tonne for CO2 capture, as compared with PI-1. An analytical campaign was conducted to trace different impurities such as NOx, mercury, Arsenic, Selenium in gas and liquid samples through the carbon capture system. An Environmental, Health and Safety (EH&S) analysis was completed to estimate emissions from a 550 MWe net power plant with carbon capture using cold membrane. A preliminary design and cost analysis was completed for 550 tpd (~25 MWe) plant to assess the capital investment and carbon capture cost for PI-1 and PI-2 membrane solutions from coal fired flue gas. A comparison was made with an amine based solution with significant cost advantage for the membrane at this scale. Additional preliminary design and cost analysis was completed between coal, natural gas and SMR flue gas for carbon capture at 550 tpd (~25 MWe) plant.« less

Borophene as a Promising Material for Charge-Modulated Switchable CO2 Capture.

PubMed

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

2017-06-14

Ideal carbon dioxide (CO 2 ) capture materials for practical applications should bind CO 2 molecules neither too weakly to limit good loading kinetics nor too strongly to limit facile release. Although charge-modulated switchable CO 2 capture has been proposed to be a controllable, highly selective, and reversible CO 2 capture strategy, the development of a practical gas-adsorbent material remains a great challenge. In this study, by means of density functional theory (DFT) calculations, we have examined the possibility of conductive borophene nanosheets as promising sorbent materials for charge-modulated switchable CO 2 capture. Our results reveal that the binding strength of CO 2 molecules on negatively charged borophene can be significantly enhanced by injecting extra electrons into the adsorbent. At saturation CO 2 capture coverage, the negatively charged borophene achieves CO 2 capture capacities up to 6.73 × 10 14 cm -2 . In contrast to the other CO 2 capture methods, the CO 2 capture/release processes on negatively charged borophene are reversible with fast kinetics and can be easily controlled via switching on/off the charges carried by borophene nanosheets. Moreover, these negatively charged borophene nanosheets are highly selective for separating CO 2 from mixtures with CH 4 , H 2 , and/or N 2 . This theoretical exploration will provide helpful guidance for identifying experimentally feasible, controllable, highly selective, and high-capacity CO 2 capture materials with ideal thermodynamics and reversibility.

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

PubMed

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

2016-10-01

Sorbents for CO 2 capture have been prepared by wet impregnation of a commercial active carbon (Ketjen-black, Akzo Nobel) with two CO 2 -philic compounds, polyethylenimine (PEI) and tetraethylenepentamine (TEPA), respectively. The effects of amine amount (from 10 to 70wt.%), CO 2 concentration in the feed, sorption temperature and gas hourly space velocity on the CO 2 capture performance have been investigated. The sorption capacity has been evaluated using the breakthrough method, with a fixed bed reactor equipped with on line gas chromatograph. The samples have been characterized by N 2 adsorption-desorption, scanning electron microscopy and energy dispersive X-ray (SEM/EDX). A promising CO 2 sorption capacity of 6.90 mmol/g sorbent has been obtained with 70wt.% of supported TEPA at 70°C under a stream containing 80vol% of CO 2 . Sorption tests, carried out with simulated biogas compositions (CH 4 /CO 2 mixtures), have revealed an appreciable CO 2 separation selectivity; stable performance was maintained for 20 adsorption-desorption cycles. Copyright © 2016. Published by Elsevier B.V.

Hierarchical calibration and validation for modeling bench-scale solvent-based carbon capture. Part 1: Non-reactive physical mass transfer across the wetted wall column: Original Research Article: Hierarchical calibration and validation for modeling bench-scale solvent-based carbon capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Chao; Xu, Zhijie; Lai, Canhai

A hierarchical model calibration and validation is proposed for quantifying the confidence level of mass transfer prediction using a computational fluid dynamics (CFD) model, where the solvent-based carbon dioxide (CO2) capture is simulated and simulation results are compared to the parallel bench-scale experimental data. Two unit problems with increasing level of complexity are proposed to breakdown the complex physical/chemical processes of solvent-based CO2 capture into relatively simpler problems to separate the effects of physical transport and chemical reaction. This paper focuses on the calibration and validation of the first unit problem, i.e. the CO2 mass transfer across a falling ethanolaminemore » (MEA) film in absence of chemical reaction. This problem is investigated both experimentally and numerically using nitrous oxide (N2O) as a surrogate for CO2. To capture the motion of gas-liquid interface, a volume of fluid method is employed together with a one-fluid formulation to compute the mass transfer between the two phases. Bench-scale parallel experiments are designed and conducted to validate and calibrate the CFD models using a general Bayesian calibration. Two important transport parameters, e.g. Henry’s constant and gas diffusivity, are calibrated to produce the posterior distributions, which will be used as the input for the second unit problem to address the chemical adsorption of CO2 across the MEA falling film, where both mass transfer and chemical reaction are involved.« less

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

PubMed

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

2012-11-20

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tande, Brian; Seames, Wayne; Benson, Steve

The objective of this project was to evaluate the use of composite polymer membranes and porous membrane contactors to regenerate physical and chemical solvents for capture of carbon dioxide (CO 2) from synthesis gas or flue gas, with the goal of improving the energy efficiency of carbon capture. Both a chemical solvent (typical for a post-combustion capture of CO 2 from flue gas) and a physical solvent (typical for pre- combustion capture of CO 2 from syngas) were evaluated using two bench-scale test systems constructed for this project. For chemical solvents, polytetrafluoroethylene and polypropylene membranes were found to be ablemore » to strip CO 2 from a monoethanolamine (MEA) solution with high selectivity without significant degradation of the material. As expected, the regeneration temperature was the most significant parameter affecting the CO 2 flux through the membrane. Pore size was also found to be important, as pores larger than 5 microns lead to excessive pore wetting. For physical solvents, polydimethyl-siloxane (PDMS)-based membranes were found to have a higher CO 2 permeability than polyvinylalcohol (PVOH) based membranes, while also minimizing solvent loss. Overall, however, the recovery of CO 2 in these systems is low – less than 2% for both chemical and physical solvents – primarily due to the small surface area of the membrane test apparatus. To obtain the higher regeneration rates needed for this application, a much larger surface area would be needed. Further experiments using, for example, a hollow fiber membrane module could determine if this process could be commercially viable.« less

Computational materials chemistry for carbon capture using porous materials

NASA Astrophysics Data System (ADS)

Sharma, Abhishek; Huang, Runhong; Malani, Ateeque; Babarao, Ravichandar

2017-11-01

Control over carbon dioxide (CO2) release is extremely important to decrease its hazardous effects on the environment such as global warming, ocean acidification, etc. For CO2 capture and storage at industrial point sources, nanoporous materials offer an energetically viable and economically feasible approach compared to chemisorption in amines. There is a growing need to design and synthesize new nanoporous materials with enhanced capability for carbon capture. Computational materials chemistry offers tools to screen and design cost-effective materials for CO2 separation and storage, and it is less time consuming compared to trial and error experimental synthesis. It also provides a guide to synthesize new materials with better properties for real world applications. In this review, we briefly highlight the various carbon capture technologies and the need of computational materials design for carbon capture. This review discusses the commonly used computational chemistry-based simulation methods for structural characterization and prediction of thermodynamic properties of adsorbed gases in porous materials. Finally, simulation studies reported on various potential porous materials, such as zeolites, porous carbon, metal organic frameworks (MOFs) and covalent organic frameworks (COFs), for CO2 capture are discussed.

Assessing Atmospheric CO2 Entrapped in Clay Nanotubes using Residual Gas Analyzer.

PubMed

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

2016-02-16

A residual gas analyzer (RGA) coupled with a high-vacuum chamber has been explored to measure atmospheric CO2 entrapped in aminosilane-modified clay nanotubes. Ambient CO2 uptake efficacy together with stability of these novel adsorbents composed of both primary and/or secondary amine sites has been demonstrated at standard ambient temperature and pressure. The unprecedented sensitivity and accuracy of the RGA-based mass spectrometry technique toward atmospheric CO2 measurement has been substantiated with a laser-based optical cavity-enhanced integrated cavity output spectroscopy. The adsorption kinetics of atmospheric CO2 on amine-functionalized clay nanotubes followed the fractional-order kinetic model compared to that of the pseudo-first-order or pseudo-second-order rate equations. The efficiency along with stability of these novel adsorbents has also been demonstrated by their repetitive use for CO2 capture in the oxidative environment. Our findings thus point to a fundamental study on the atmospheric CO2 adsorption by amine-loaded adsorbents using an easy handling and low-cost benchtop RGA-based mass spectrometer, opening a new strategy for CO2 capture and sequestering study.

Effective Elastic and Neutron Capture Cross Section Calculations Corresponding to Simulated Fluid Properties from CO2 Push-Pull Simulations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chugunov, Nikita; Altundas, Bilgin

The submission contains a .xls files consisting of 10 excel sheets, which contain combined list of pressure, saturation, salinity, temperature profiles from the simulation of CO2 push-pull using Brady reservoir model and the corresponding effective compressional and shear velocity, bulk density, and fluid and time-lapse neutron capture cross section profiles of rock at times 0 day (baseline) through 14 days. First 9 sheets (each named after the corresponding CO2 push-pull simulation time) contains simulated pressure, saturation, temperature, salinity profiles and the corresponding effective elastic and neutron capture cross section profiles of rock matrix at the time of CO2 injection. Eachmore » sheet contains two sets of effective compressional velocity profiles of the rock, one based on Gassmann and the other based on Patchy saturation model. Effective neutron capture cross section calculations are done using a proprietary neutron cross-section simulator (SNUPAR) whereas for the thermodynamic properties of CO2 and bulk density of rock matrix filled with fluid, a standalone fluid substitution tool by Schlumberger is used. Last sheet in the file contains the bulk modulus of solid rock, which is inverted from the rock properties (porosity, sound speed etc) based on Gassmann model. Bulk modulus of solid rock in turn is used in the fluid substitution.« less

Mechanochemically Activated, Calcium Oxide-Based, Magnesium Oxide-Stabilized Carbon Dioxide Sorbents.

PubMed

Kurlov, Alexey; Broda, Marcin; Hosseini, Davood; Mitchell, Sharon J; Pérez-Ramírez, Javier; Müller, Christoph R

2016-09-08

Carbon dioxide capture and storage (CCS) is a promising approach to reduce anthropogenic CO2 emissions and mitigate climate change. However, the costs associated with the capture of CO2 using the currently available technology, that is, amine scrubbing, are considered prohibitive. In this context, the so-called calcium looping process, which relies on the reversible carbonation of CaO, is an attractive alternative. The main disadvantage of naturally occurring CaO-based CO2 sorbents, such as limestone, is their rapid deactivation caused by thermal sintering. Here, we report a scalable route based on wet mechanochemical activation to prepare MgO-stabilized, CaO-based CO2 sorbents. We optimized the synthesis conditions through a fundamental understanding of the underlying stabilization mechanism, and the quantity of MgO required to stabilize CaO could be reduced to as little as 15 wt %. This allowed the preparation of CO2 sorbents that exceed the CO2 uptake of the reference limestone by 200 %. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Rational construction of a stable Zn4O-based MOF for highly efficient CO2 capture and conversion.

PubMed

Zhou, Hui-Fang; Liu, Bo; Hou, Lei; Zhang, Wen-Yan; Wang, Yao-Yu

2018-01-11

By employing a carboxylate ligand derived from benzene-1,4-dicarboxylate, a chemically stable Zn 4 O-based self-penetrating metal-organic framework has been rationally synthesized, which exhibits high CO 2 adsorption and efficient catalytic conversion for CO 2 cycloaddition.

Effects of water vapor pretreatment time and reaction temperature on CO(2) capture characteristics of a sodium-based solid sorbent in a bubbling fluidized-bed reactor.

PubMed

Seo, Yongwon; Jo, Sung-Ho; Ryu, Chong Kul; Yi, Chang-Keun

2007-10-01

CO(2) capture from flue gas using a sodium-based solid sorbent was investigated in a bubbling fluidized-bed reactor. Carbonation and regeneration temperature on CO(2) removal was determined. The extent of the chemical reactivity after carbonation or regeneration was characterized via (13)C NMR. In addition, the physical properties of the sorbent such as pore size, pore volume, and surface area after carbonation or regeneration were measured by gas adsorption method (BET). With water vapor pretreatment, near complete CO(2) removal was initially achieved and maintained for about 1-2min at 50 degrees C with 2s gas residence time, while without proper water vapor pretreatment CO(2) removal abruptly decreased from the beginning. Carbonation was effective at the lower temperature over the 50-70 degrees C temperature range, while regeneration more effective at the higher temperature over the 135-300 degrees C temperature range. To maintain the initial 90% CO(2) removal, it would be necessary to keep the regeneration temperature higher than about 135 degrees C. The results obtained in this study can be used as basic data for designing and operating a large scale CO(2) capture process with two fluidized-bed reactors.

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

Biochemical Capture and Removal of Carbon Dioxide

NASA Technical Reports Server (NTRS)

Trachtenberg, Michael C.

1998-01-01

We devised an enzyme-based facilitated transport membrane bioreactor system to selectively remove carbon dioxide (CO2) from the space station environment. We developed and expressed site-directed enzyme mutants for CO2 capture. Enzyme kinetics showed the mutants to be almost identical to the wild type save at higher pH. Both native enzyme and mutant enzymes were immobilized to different supports including nylons, glasses, sepharose, methacrylate, titanium and nickel. Mutant enzyme could be attached and removed from metal ligand supports and the supports reused at least five times. Membrane systems were constructed to test CO2 selectivity. These included proteic membranes, thin liquid films and enzyme-immobilized teflon membranes. Selectivity ratios of more than 200:1 were obtained for CO2 versus oxygen with CO2 at 0.1%. The data indicate that a membrane based bioreactor can be constructed which could bring CO2 levels close to Earth.

Creating markets for captured carbon: Retrofit of Abbott Power Plant and Future Utilization of Captured CO 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

O'Brien, Kevin C.; Lu, Yongqi; Patel, Vinod

The successful implementation of CCUS requires the confluence of technology, regulatory, and financial factors. One of the factors that impact this confluence is the ability to utilize and monetize captured CO 2. The generally accepted utilization approach has been CO 2-based Enhanced Oil Recovery (EOR), yet this is not always feasible and/or a preferable approach. There is a need to be able to explore a multitude of utilization approaches in order to identify a portfolio of potential utilization mechanisms. This portfolio must be adapted based on the economy of the region. In response to this need, the University of Illinoismore » has formed a Carbon Dioxide Utilization and Reduction (COOULR) Center. The open nature of the university, coupled with a university policy to reduce CO 2 emissions, provides a model for the issues communities will face when attempting to reduce emissions while still maintaining reliable and affordable power. This Center is one of the key steps in the formation of a market for captured CO 2. Furthermore, the goal of the Center is to not only evaluate technologies, but also demonstrate at a large pilot scale how communities may be able to adjust to the need to reduce GHG emissions.« less

Creating markets for captured carbon: Retrofit of Abbott Power Plant and Future Utilization of Captured CO 2

DOE PAGES

O'Brien, Kevin C.; Lu, Yongqi; Patel, Vinod; ...

2017-01-01

The successful implementation of CCUS requires the confluence of technology, regulatory, and financial factors. One of the factors that impact this confluence is the ability to utilize and monetize captured CO 2. The generally accepted utilization approach has been CO 2-based Enhanced Oil Recovery (EOR), yet this is not always feasible and/or a preferable approach. There is a need to be able to explore a multitude of utilization approaches in order to identify a portfolio of potential utilization mechanisms. This portfolio must be adapted based on the economy of the region. In response to this need, the University of Illinoismore » has formed a Carbon Dioxide Utilization and Reduction (COOULR) Center. The open nature of the university, coupled with a university policy to reduce CO 2 emissions, provides a model for the issues communities will face when attempting to reduce emissions while still maintaining reliable and affordable power. This Center is one of the key steps in the formation of a market for captured CO 2. Furthermore, the goal of the Center is to not only evaluate technologies, but also demonstrate at a large pilot scale how communities may be able to adjust to the need to reduce GHG emissions.« less

Electricity from fossil fuels without CO2 emissions: assessing the costs of carbon dioxide capture and sequestration in U.S. electricity markets.

PubMed

Johnson, T L; Keith, D W

2001-10-01

The decoupling of fossil-fueled electricity production from atmospheric CO2 emissions via CO2 capture and sequestration (CCS) is increasingly regarded as an important means of mitigating climate change at a reasonable cost. Engineering analyses of CO2 mitigation typically compare the cost of electricity for a base generation technology to that for a similar plant with CO2 capture and then compute the carbon emissions mitigated per unit of cost. It can be hard to interpret mitigation cost estimates from this plant-level approach when a consistent base technology cannot be identified. In addition, neither engineering analyses nor general equilibrium models can capture the economics of plant dispatch. A realistic assessment of the costs of carbon sequestration as an emissions abatement strategy in the electric sector therefore requires a systems-level analysis. We discuss various frameworks for computing mitigation costs and introduce a simplified model of electric sector planning. Results from a "bottom-up" engineering-economic analysis for a representative U.S. North American Electric Reliability Council (NERC) region illustrate how the penetration of CCS technologies and the dispatch of generating units vary with the price of carbon emissions and thereby determine the relationship between mitigation cost and emissions reduction.

Electricity from Fossil Fuels without CO2 Emissions: Assessing the Costs of Carbon Dioxide Capture and Sequestration in U.S. Electricity Markets.

PubMed

Johnson, Timothy L; Keith, David W

2001-10-01

The decoupling of fossil-fueled electricity production from atmospheric CO 2 emissions via CO 2 capture and sequestration (CCS) is increasingly regarded as an important means of mitigating climate change at a reasonable cost. Engineering analyses of CO 2 mitigation typically compare the cost of electricity for a base generation technology to that for a similar plant with CO 2 capture and then compute the carbon emissions mitigated per unit of cost. It can be hard to interpret mitigation cost estimates from this plant-level approach when a consistent base technology cannot be identified. In addition, neither engineering analyses nor general equilibrium models can capture the economics of plant dispatch. A realistic assessment of the costs of carbon sequestration as an emissions abatement strategy in the electric sector therefore requires a systems-level analysis. We discuss various frameworks for computing mitigation costs and introduce a simplified model of electric sector planning. Results from a "bottom-up" engineering-economic analysis for a representative U.S. North American Electric Reliability Council (NERC) region illustrate how the penetration of CCS technologies and the dispatch of generating units vary with the price of carbon emissions and thereby determine the relationship between mitigation cost and emissions reduction.

High-throughput screening of metal-porphyrin-like graphenes for selective capture of carbon dioxide

PubMed Central

Bae, Hyeonhu; Park, Minwoo; Jang, Byungryul; Kang, Yura; Park, Jinwoo; Lee, Hosik; Chung, Haegeun; Chung, ChiHye; Hong, Suklyun; Kwon, Yongkyung; Yakobson, Boris I.; Lee, Hoonkyung

2016-01-01

Nanostructured materials, such as zeolites and metal-organic frameworks, have been considered to capture CO2. However, their application has been limited largely because they exhibit poor selectivity for flue gases and low capture capacity under low pressures. We perform a high-throughput screening for selective CO2 capture from flue gases by using first principles thermodynamics. We find that elements with empty d orbitals selectively attract CO2 from gaseous mixtures under low CO2 pressures (~10−3 bar) at 300 K and release it at ~450 K. CO2 binding to elements involves hybridization of the metal d orbitals with the CO2 π orbitals and CO2-transition metal complexes were observed in experiments. This result allows us to perform high-throughput screening to discover novel promising CO2 capture materials with empty d orbitals (e.g., Sc– or V–porphyrin-like graphene) and predict their capture performance under various conditions. Moreover, these findings provide physical insights into selective CO2 capture and open a new path to explore CO2 capture materials. PMID:26902156

High-throughput screening of metal-porphyrin-like graphenes for selective capture of carbon dioxide.

PubMed

Bae, Hyeonhu; Park, Minwoo; Jang, Byungryul; Kang, Yura; Park, Jinwoo; Lee, Hosik; Chung, Haegeun; Chung, ChiHye; Hong, Suklyun; Kwon, Yongkyung; Yakobson, Boris I; Lee, Hoonkyung

2016-02-23

Nanostructured materials, such as zeolites and metal-organic frameworks, have been considered to capture CO2. However, their application has been limited largely because they exhibit poor selectivity for flue gases and low capture capacity under low pressures. We perform a high-throughput screening for selective CO2 capture from flue gases by using first principles thermodynamics. We find that elements with empty d orbitals selectively attract CO2 from gaseous mixtures under low CO2 pressures (~10(-3) bar) at 300 K and release it at ~450 K. CO2 binding to elements involves hybridization of the metal d orbitals with the CO2 π orbitals and CO2-transition metal complexes were observed in experiments. This result allows us to perform high-throughput screening to discover novel promising CO2 capture materials with empty d orbitals (e.g., Sc- or V-porphyrin-like graphene) and predict their capture performance under various conditions. Moreover, these findings provide physical insights into selective CO2 capture and open a new path to explore CO2 capture materials.

High-throughput screening of metal-porphyrin-like graphenes for selective capture of carbon dioxide

NASA Astrophysics Data System (ADS)

Bae, Hyeonhu; Park, Minwoo; Jang, Byungryul; Kang, Yura; Park, Jinwoo; Lee, Hosik; Chung, Haegeun; Chung, Chihye; Hong, Suklyun; Kwon, Yongkyung; Yakobson, Boris I.; Lee, Hoonkyung

2016-02-01

Nanostructured materials, such as zeolites and metal-organic frameworks, have been considered to capture CO2. However, their application has been limited largely because they exhibit poor selectivity for flue gases and low capture capacity under low pressures. We perform a high-throughput screening for selective CO2 capture from flue gases by using first principles thermodynamics. We find that elements with empty d orbitals selectively attract CO2 from gaseous mixtures under low CO2 pressures (~10-3 bar) at 300 K and release it at ~450 K. CO2 binding to elements involves hybridization of the metal d orbitals with the CO2 π orbitals and CO2-transition metal complexes were observed in experiments. This result allows us to perform high-throughput screening to discover novel promising CO2 capture materials with empty d orbitals (e.g., Sc- or V-porphyrin-like graphene) and predict their capture performance under various conditions. Moreover, these findings provide physical insights into selective CO2 capture and open a new path to explore CO2 capture materials.

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. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Cycle development and design for CO{sub 2} capture from flue gas by vacuum swing adsorption

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jun Zhang; Paul A. Webley

CO{sub 2} capture and storage is an important component in the development of clean power generation processes. One CO{sub 2} 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 CO{sub 2} 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 non-isothermal effects as well as nonlinear adsorption and nitrogen coadsorption. Using the model and ourmore » apparatus, we have designed and studied a large number of cycles for CO{sub 2} 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 CO{sub 2} capture from flue gases. 20 refs., 6 figs., 2 tabs.« less

Design of protonation constant measurement apparatus for carbon dioxide capturing solvents

NASA Astrophysics Data System (ADS)

Ma'mun, S.; Amelia, E.; Rahmat, V.; Alwani, D. R.; Kurniawan, D.

2016-11-01

Global warming phenomenon has led to world climate change caused by high concentrations of greenhouse gases (GHG), e.g. carbon dioxide (CO2), in the atmosphere. Carbon dioxide is produced in large amount from coal-fired power plants, iron and steel production, cement production, chemical and petrochemical manufacturing, natural gas purification, and transportation. Carbon dioxide emissions seem to rise from year to year; some efforts to reduce the emissions are, therefore, required. Amine-based absorption could be deployed for post-combustion capture. Some parameters, e.g. mass transfer coefficients and chemical equilibrium constants, are required for a vapor-liquid equilibrium modeling. Protonation constant (pKa), as one of those parameters, could then be measured experimentally. Therefore, an experimental setup to measure pKa of CO2 capturing solvents was designed and validated by measuring the pKa of acetic acid at 30 to 70 °C by a potentiometric titration method. The set up was also used to measure the pKa of MEA at 27 °C. Based on the validation results and due to low vapor pressure of CO2 capturing solvents in general, e.g. alkanolamines, the setup could therefore be used for measuring pKa of the CO2 capturing solvents at temperatures up to 70 °C.

Thermodynamic Properties of CO{sub 2} Capture Reaction by Solid Sorbents: Theoretical Predictions and Experimental Validations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Duan, Yuhua; Luebke, David; Pennline, Henry

2012-01-01

It is generally accepted that current technologies for capturing CO{sub 2} are still too energy intensive. Hence, there is a critical need for development of new materials that can capture CO{sub 2} reversibly with acceptable energy costs. Accordingly, solid sorbents have been proposed to be used for CO{sub 2} 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 CO{sub 2} sorbent candidates from the vast array of possible solid materials has been proposed and validated. The calculatedmore » thermodynamic properties of different classes of solid materials versus temperature and pressure changes were further used to evaluate the equilibrium properties for the CO{sub 2} adsorption/desorption cycles. According to the requirements imposed by the pre- and post- combustion technologies and based on our calculated thermodynamic properties for the CO{sub 2} 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. These CO{sub 2} sorbent candidates were further considered for experimental validations. In this presentation, we first introduce our screening methodology with validating by solid dataset of alkali and alkaline metal oxides, hydroxides and bicarbonates which thermodynamic properties are available. Then, by studying a series of lithium silicates, we found that by increasing the Li{sub 2}O/SiO{sub 2} ratio in the lithium silicates their corresponding turnover temperatures for CO{sub 2} capture reactions can be increased. Compared to anhydrous K{sub 2}CO{sub 3}, the dehydrated K{sub 2}CO{sub 3}1.5H{sub 2}O can only be applied for post-combustion CO{sub 2} capture technology at temperatures lower than its phase transition (to anhydrous phase) temperature, which depends on the CO{sub 2} pressure and the steam pressure with the best range being PH{sub 2}O≤1.0 bar. Above the phase-transition temperature, the sorbent will be regenerated into anhydrous K{sub 2}CO{sub 3}. Our theoretical investigations on Na-promoted MgO sorbents revealed that the sorption process takes place through formation of the Na{sub 2}Mg(CO{sub 3}){sub 2} double carbonate with better reaction kinetics over porous MgO, that of pure MgO sorbent. The experimental sorption tests also indicated that the Na-promoted MgO sorbent has high reactivity and capacity towards CO{sub 2} sorption and can be easily regenerated either through pressure or temperature swing processes.« less

Measuring the Absorption Rate of CO 2 in Nonaqueous CO 2 -Binding Organic Liquid Solvents with a Wetted-Wall Apparatus

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mathias, Paul M.; Zheng, Feng; Heldebrant, David J.

2015-09-17

The kinetics of the absorption of CO 2 into two nonaqueous CO 2-binding organic liquid (CO 2BOL) solvents were measured at T=35, 45, and 55 °C with a wetted-wall column. Selected CO 2 loadings were run with a so-called “first-generation” CO 2BOL, comprising an independent base and alcohol, and a “second-generation” CO 2BOL, in which the base and alcohol were conjoined. Liquid-film mass-transfer coefficient (k'g) values for both solvents were measured to be comparable to values for monoethanolamine and piperazine aqueous solvents under a comparable driving force, in spite of far higher solution viscosities. An inverse temperature dependence of themore » k'g value was also observed, which suggests that the physical solubility of CO 2 in organic liquids may be making CO 2 mass transfer faster than expected. Aspen Plus software was used to model the kinetic data and compare the CO 2 absorption behavior of nonaqueous solvents with that of aqueous solvent platforms. This work continues our development of the CO2BOL solvents. Previous work established the thermodynamic properties related to CO 2 capture. The present paper quantitatively studies the kinetics of CO 2 capture and develops a rate-based model.« less

PNNL Report on the Development of Bench-scale CFD Simulations for Gas Absorption across a Wetted Wall Column

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Chao; Xu, Zhijie; Lai, Canhai

This report is prepared for the demonstration of hierarchical prediction of carbon capture efficiency of a solvent-based absorption column. A computational fluid dynamics (CFD) model is first developed to simulate the core phenomena of solvent-based carbon capture, i.e., the CO2 physical absorption and chemical reaction, on a simplified geometry of wetted wall column (WWC) at bench scale. Aqueous solutions of ethanolamine (MEA) are commonly selected as a CO2 stream scrubbing liquid. CO2 is captured by both physical and chemical absorption using highly CO2 soluble and reactive solvent, MEA, during the scrubbing process. In order to provide confidence bound on themore » computational predictions of this complex engineering system, a hierarchical calibration and validation framework is proposed. The overall goal of this effort is to provide a mechanism-based predictive framework with confidence bound for overall mass transfer coefficient of the wetted wall column (WWC) with statistical analyses of the corresponding WWC experiments with increasing physical complexity.« less

Microporous metal organic framework [M2(hfipbb)2(ted)] (M=Zn, Co; H2hfipbb=4,4-(hexafluoroisopropylidene)-bis(benzoic acid); ted=triethylenediamine): Synthesis, structure analysis, pore characterization, small gas adsorption and CO2/N2 separation properties

NASA Astrophysics Data System (ADS)

Xu, William W.; Pramanik, Sanhita; Zhang, Zhijuan; Emge, Thomas J.; Li, Jing

2013-04-01

Carbon dioxide is a greenhouse gas that is a major contributor to global warming. Developing methods that can effectively capture CO2 is the key to reduce its emission to the atmosphere. Recent research shows that microporous metal organic frameworks (MOFs) are emerging as a promising family of adsorbents that may be promising for use in adsorption based capture and separation of CO2 from power plant waste gases. In this work we report the synthesis, crystal structure analysis and pore characterization of two microporous MOF structures, [M2(hfipbb)2(ted)] (M=Zn (1), Co (2); H2hfipbb=4,4-(hexafluoroisopropylidene)-bis(benzoic acid); ted=triethylenediamine). The CO2 and N2 adsorption experiments and IAST calculations are carried out on [Zn2(hfipbb)2(ted)] under conditions that mimic post-combustion flue gas mixtures emitted from power plants. The results show that the framework interacts with CO2 strongly, giving rise to relatively high isosteric heats of adsorption (up to 28 kJ/mol), and high adsorption selectivity for CO2 over N2, making it promising for capturing and separating CO2 from CO2/N2 mixtures.

Pre-Combustion Carbon Capture by a Nanoporous, Superhydrophobic Membrane Contactor Process

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meyer, Howard; Zhou, S James; Ding, Yong

2012-03-31

This report summarizes progress made during Phase I and Phase II of the project: "Pre-Combustion Carbon Capture by a Nanoporous, Superhydrophobic Membrane Contactor Process," under contract DE-FE-0000646. The objective of this project is to develop a practical and cost effective technology for CO{sub 2} separation and capture for pre-combustion coal-based gasification plants using a membrane contactor/solvent absorption process. The goals of this technology development project are to separate and capture at least 90% of the CO{sub 2} from Integrated Gasification Combined Cycle (IGCC) power plants with less than 10% increase in the cost of energy services. Unlike conventional gas separationmore » membranes, the membrane contactor is a novel gas separation process based on the gas/liquid membrane concept. The membrane contactor is an advanced mass transfer device that operates with liquid on one side of the membrane and gas on the other. The membrane contactor can operate with pressures that are almost the same on both sides of the membrane, whereas the gas separation membranes use the differential pressure across the membrane as driving force for separation. The driving force for separation for the membrane contactor process is the chemical potential difference of CO{sub 2} in the gas phase and in the absorption liquid. This process is thus easily tailored to suit the needs for pre-combustion separation and capture of CO{sub 2}. Gas Technology Institute (GTI) and PoroGen Corporation (PGC) have developed a novel hollow fiber membrane technology that is based on chemically and thermally resistant commercial engineered polymer poly(ether ether ketone) or PEEK. The PEEK membrane material used in the membrane contactor during this technology development program is a high temperature engineered plastic that is virtually non-destructible under the operating conditions encountered in typical gas absorption applications. It can withstand contact with most of the common treating solvents. GTI and PGC have developed a nanoporous and superhydrophobic PEEK-based hollow fiber membrane contactor tailored for the membrane contactor/solvent absorption application for syngas cleanup. The membrane contactor modules were scaled up to 8-inch diameter commercial size modules. We have performing extensive laboratory and bench testing using pure gases, simulated water-gas-shifted (WGS) syngas stream, and a slipstream from a gasification derived syngas from GTI's Flex-Fuel Test Facility (FFTF) gasification plant under commercially relevant conditions. The team have also carried out an engineering and economic analysis of the membrane contactor process to evaluate the economics of this technology and its commercial potential. Our test results have shown that 90% CO{sub 2} capture can be achieved with several physical solvents such as water and chilled methanol. The rate of CO{sub 2} removal by the membrane contactor is in the range of 1.5 to 2.0 kg/m{sup 2}/hr depending on the operating pressures and temperatures and depending on the solvents used. The final economic analysis has shown that the membrane contactor process will cause the cost of electricity to increase by 21% from the base plant without CO{sub 2} capture. The goal of 10% increase in levelized cost of electricity (LCOE) from base DOE Case 1(base plant without capture) is not achieved by using the membrane contactor. However, the 21% increase in LCOE is a substantial improvement as compared with the 31.6% increase in LCOE as in DOE Case 2(state of art capture technology using 2-stages of Selexol{TM}).« less

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.

Effect of CuO on the efficiency of sulfur capture of Ca-based compounds during coal combustion.

PubMed

Zheng, Li-Qing; Lu, Wen-Ying; Liu, Guo-Guang

2003-05-01

The efficiency of sulfur capture of CaO, Ca(OH)2 and CaCO3 as well as the effect of CuO on them were studied. Results showed that the efficiency of sulfur capture of Ca(OH)2 is the highest among these three compounds. When CuO was used with each of CaO, Ca(OH)2 and CaCO3 at the same time, the efficiency of all of them would rise, and that of Ca(OH)2 raise most. The efficiency of sulfur capture of Ca(OH)2 with CuO is 14.4% higher than that without CuO.

Electrochemical capture and release of carbon dioxide

DOE PAGES

Rheinhardt, Joseph H.; Singh, Poonam; Tarakeshwar, Pilarisetty; ...

2017-01-18

Understanding the chemistry of carbon dioxide is key to affecting changes in atmospheric concentrations. One area of intense interest is CO 2 capture in chemically reversible cycles relevant to carbon capture technologies. Most CO 2 capture methods involve thermal cycles in which a nucleophilic agent captures CO 2 from impure gas streams (e.g., flue gas), followed by a thermal process in which pure CO 2 is released. Several reviews have detailed progress in these approaches. A less explored strategy uses electrochemical cycles to capture CO 2 and release it in pure form. These cycles typically rely on electrochemical generation ofmore » nucleophiles that attack CO 2 at the electrophilic carbon atom, forming a CO 2 adduct. Then, CO 2 is released in pure form via a subsequent electrochemical step. In this Perspective, we describe electrochemical cycles for CO 2 capture and release, emphasizing electrogenerated nucleophiles. As a result, we also discuss some advantages and disadvantages inherent in this general approach.« less

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.

The steps of activating a prospective CO 2 hydrogenation catalyst with combined CO 2 capture and reduction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lao, D. B.; Galan, B. R.; Linehan, J. C.

2016-08-10

Combining carbon capture and reduction is an efficient strategy to alleviate the high energy requirements for seperation, compression, and storage of CO2 prior to reduction. Recent studies have shown that catalytic hydrogenations of CO2 can be performed without added pressure of CO2 using switchable ionic liquids. It’s ambiguous whether the alkylcarbonate (captured CO2) is reduced as it is in dynamic equilibrium with neutral CO2 in solution. New studies are presented to elucidate the reactivity of CO2 and CO2 captured in solution.

Process and Material Design for Micro-Encapsulated Ionic Liquids in Post-Combustion CO 2 Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hong, Bo; Brennecke, Joan F; McCready, Mark

Aprotic Heterocyclic Anion (AHA) Ionic Liquids (ILs) have been identified as promising new solvents for post-combustion carbon capture due to their high CO 2 uptake and the high tenability 1,2 of their binding energy with CO 2. Some of these compounds change phase (solid to liquid) on absorption of CO 2; these Phase Change ILs (PCILs)3 offer the additional advantage that part of the heat needed to desorb the CO2 from the absorbent is provided by the heat of fusion as the PCIL solidifies upon release of CO 2. However, the relatively high viscosity of AHA ILs and the occurrencemore » of a phase change in PCILs present challenges for conventional absorption equipment. To overcome these challenges we are pursuing the use of new technology to micro-encapsulate the AHA ILs and PCILs. Our partners at Lawrence Livermore National Laboratory have successfully demonstrated this technology in the application of post-combustion carbon capture with sodium and potassium carbonate solutions,4 and have recently shown the feasibility of micro-encapsulation of an AHA IL for carbon capture.5 The large effective surface area and high CO 2 permeability of the micro-capsules is expected to offset the drawback of the high IL viscosity and to provide for a more efficient and cost-effective mass transfer operation involving AHA ILs and PCILs. These opportunities, however, present us with both process and materials design questions. For example, what is the target CO 2 absorption strength (enthalpy of chemical absorption) for the tunable AHA IL? What is the target for micro-capsule diameter in order to obtain a high mass transfer rate and good fluidization performance? What are the appropriate temperatures and pressures for the absorber and stripper? In order to address these and other questions, we have developed a rate-based model of a post-combustion CO 2 capture process using micro-encapsulated ILs. As a performance baseline, we have also developed a rate-based model of a standard packed bed absorber using an un-encapsulated AHA IL absorbent. Using such models we can determine optimal CO 2 capture performance and investigate the sensitivity of the optimum with respect to the key thermo-physical and transport properties of the IL (e.g., CO 2 binding energy, viscosity, etc.) and the micro-capsules (e.g. diameter, CO 2 permeability, etc.). Results of these process and material design studies will be presented, and the performance of this novel micro-encapsulation technology will be assessed.« less

Amine enriched solid sorbents for carbon dioxide capture

DOEpatents

Gray, McMahan L.; Soong, Yee; Champagne, Kenneth J.

2003-04-15

A new method for making low-cost CO.sub.2 sorbents that can be used in large-scale gas-solid processes. The new method entails treating a solid substrate with acid or base and simultaneous or subsequent treatment with a substituted amine salt. The method eliminates the need for organic solvents and polymeric materials for the preparation of CO.sub.2 capture systems.

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

PubMed

Sanna, Aimaro; Maroto-Valer, M Mercedes

2016-11-01

Potassium-fly ash (K-FA) sorbents were investigated for high-temperature CO 2 sorption. K-FAs were synthesised using coal fly ash as source of silica and aluminium. The synthesised materials were also mixed with Li 2 CO 3 and Ca(OH) 2 to evaluate their effect on CO 2 capture. Temperature strongly affected the performance of the K-FA sorbents, resulting in a CO 2 uptake of 1.45 mmol CO 2 /g sorbent for K-FA 1:1 at 700 °C. The CO 2 sorption was enhanced by the presence of Li 2 CO 3 (10 wt%), with the K-FA 1:1 capturing 2.38 mmol CO 2 /g sorbent at 700 °C in 5 min. This sorption was found to be similar to previously developed Li-Na-FA (2.54 mmol/g) and Li-FA (2.4 mmol/g) sorbents. The presence of 10 % Li 2 CO 3 also accelerated sorption and desorption. The results suggest that the increased uptake of CO 2 and faster reaction rates in presence of K-FA can be ascribed to the formation of K-Li eutectic phase, which favours the diffusion of potassium and CO 2 in the material matrix. The cyclic experiments showed that the K-FA materials maintained stable CO 2 uptake and reaction rates over 10 cycles.

Incorporation of Alkylamine into Metal-Organic Frameworks through a Brønsted Acid-Base Reaction for CO2 Capture.

PubMed

Li, Hao; Wang, Kecheng; Feng, Dawei; Chen, Ying-Pin; Verdegaal, Wolfgang; Zhou, Hong-Cai

2016-10-06

The escalating atmospheric CO 2 concentration is one of the most urgent environmental concerns of our age. To effectively capture CO 2 , various materials have been studied. Among them, alkylamine-modified metal-organic frameworks (MOFs) are considered to be promising candidates. In most cases, alkylamine molecules are integrated into MOFs through the coordination bonds formed between open metal sites (OMSs) and amine groups. Thus, the alkylamine density, as well as the corresponding CO 2 uptake in MOFs, are severely restricted by the density of OMSs. To overcome this limit, other approaches to incorporating alkylamine into MOFs are highly desired. We have developed a new method based on Brønsted acid-base reaction to tether alkylamines into Cr-MIL-101-SO 3 H for CO 2 capture. A systematic optimization of the amine tethering process was also conducted to maximize the CO 2 uptake of the modified MOF. Under the optimal amine tethering condition, the obtained tris(2-aminoethyl)amine-functionalized Cr-MIL-101-SO 3 H (Cr-MIL-101-SO 3 H-TAEA) has a cyclic CO 2 uptake of 2.28 mmol g -1 at 150 mbar and 40 °C, and 1.12 mmol g -1 at 0.4 mbar and 20 °C. The low-cost starting materials and simple synthetic procedure for the preparation of Cr-MIL-101-SO 3 H-TAEA suggest that it has the potential for large-scale production and practical applications. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Advanced wastewater treatment using microalgae: effect of temperature on removal of nutrients and organic carbon

NASA Astrophysics Data System (ADS)

Mohamad, Shurair; Fares, Almomani; Judd, Simon; Bhosale, Rahul; Kumar, Anand; Gosh, Ujjal; Khreisheh, Majeda

2017-05-01

This study evaluated the use of mixed indigenous microalgae (MIMA) as a treatment process for wastewaters and CO2 capturing technology at different temperatures. The study follows the growth rate of MIMA, CO2 Capturing from flue gas, removals of organic matter and nutrients from three types of wastewater (primary effluent, secondary effluent and septic effluent). A noticeable difference between the growth patterns of MIMA was observed at different CO2 and different operational temperatures. MIMA showed the highest growth grate when injected with CO2 dosage of 10% compared to the growth for the systems injected with 5% and 15 % of CO2. Ammonia and phosphorus removals for Spirulina were 69%, 75%, and 83%, and 20%, 45% and 75 % for the media injected with 0, 5 and 10% CO2. The results of this study show that simple and cost-effective microalgae-based wastewater treatment systems can be successfully employed at different temperatures as a successful CO2 capturing technology even with the small probability of inhibition at high temperatures.

Reinventing Design Principles for Developing Low-Viscosity Carbon Dioxide-Binding Organic Liquids for Flue Gas Clean Up.

PubMed

Malhotra, Deepika; Koech, Phillip K; Heldebrant, David J; Cantu, David C; Zheng, Feng; Glezakou, Vassiliki-Alexandra; Rousseau, Roger

2017-02-08

Anthropogenic CO 2 emissions from point sources (e.g., coal fired-power plants) account for the majority of the greenhouse gases in the atmosphere. Water-lean solvent systems such as CO 2 -binding organic liquids (CO 2 BOLs) are being developed to reduce the energy requirement for CO 2 capture. Many water-lean solvents such as CO 2 BOLs are currently limited by the high viscosities of concentrated electrolyte solvents, thus many of these solvents have yet to move toward commercialization. Conventional standard trial-and-error approaches for viscosity reduction, while effective, are time consuming and economically expensive. We rethink the metrics and design principles of low-viscosity CO 2 -capture solvents using a combined synthesis and computational modeling approach. We critically study the effects of viscosity reducing factors such as orientation of hydrogen bonding, introduction of higher degrees of freedom, and cation or anion charge solvation, and assess whether or how each factor affects viscosity of CO 2 BOL CO 2 capture solvents. Ultimately, we found that hydrogen bond orientation and strength is the predominant factor influencing the viscosity in CO 2 BOL solvents. With this knowledge, a new CO 2 BOL variant, 1-MEIPADM-2-BOL, was synthesized and tested, resulting in a solvent that is approximately 60 % less viscous at 25 mol % CO 2 loading than our base compound 1-IPADM-2-BOL. The insights gained from the current study redefine the fundamental concepts and understanding of what influences viscosity in concentrated organic CO 2 -capture solvents. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

NASA Astrophysics Data System (ADS)

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

2018-05-01

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

Bench Scale Process for Low Cost CO 2 Capture Using a Phase-Changing Absorbent: Final Scientific/Technical Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Westendorf, Tiffany; Buddle, Stanlee; Caraher, Joel

The objective of this project is to design and build a bench-scale process for a novel phase-changing aminosilicone-based CO 2-capture solvent. The project will establish scalability and technical and economic feasibility of using a phase-changing CO 2-capture absorbent for post-combustion capture of CO 2 from coal-fired power plants. The U.S. Department of Energy’s goal for Transformational Carbon Capture Technologies is the development of technologies available for demonstration by 2025 that can capture 90% of emitted CO 2 with at least 95% CO 2 purity for less than $40/tonne of CO 2 captured. In the first budget period of the project,more » 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 CO 2 capture performance. In the second budget period of the project, individual bench-scale unit operations were tested to determine the performance of each of each unit. Solids production was demonstrated in dry simulated flue gas across a wide range of absorber operating conditions, with single stage CO 2 conversion rates up to 75mol%. Desorber operation was demonstrated in batch mode, resulting in desorption performance consistent with the equilibrium isotherms for GAP-0/CO 2 reaction. Important risks associated with gas humidity impact on solids consistency and desorber temperature impact on thermal degradation were explored, and adjustments to the bench-scale process were made to address those effects. Corrosion experiments were conducted to support selection of suitable materials of construction for the major unit operations in the process. The bench scale unit operations were assembled into a continuous system to support steady state system testing. In the third budget period of the project, continuous system testing was conducted, including closed-loop operation of the absorber and desober systems. Slurries of GAP-0/GAP-0 carbamate/water mixtures produced in the absorber were pumped successfully to the desorber unit, and regenerated solvent was returned to the absorber. A techno-economic analysis, EH&S risk assessment, and solvent manufacturability study were completed.« less

Optimization of the structural characteristics of CaO and its effective stabilization yield high-capacity CO2 sorbents.

PubMed

Naeem, Muhammad Awais; Armutlulu, Andac; Imtiaz, Qasim; Donat, Felix; Schäublin, Robin; Kierzkowska, Agnieszka; Müller, Christoph R

2018-06-19

Calcium looping, a CO 2 capture technique, may offer a mid-term if not near-term solution to mitigate climate change, triggered by the yet increasing anthropogenic CO 2 emissions. A key requirement for the economic operation of calcium looping is the availability of highly effective CaO-based CO 2 sorbents. Here we report a facile synthesis route that yields hollow, MgO-stabilized, CaO microspheres featuring highly porous multishelled morphologies. As a thermal stabilizer, MgO minimized the sintering-induced decay of the sorbents' CO 2 capacity and ensured a stable CO 2 uptake over multiple operation cycles. Detailed electron microscopy-based analyses confirm a compositional homogeneity which is identified, together with the characteristics of its porous structure, as an essential feature to yield a high-performance sorbent. After 30 cycles of repeated CO 2 capture and sorbent regeneration, the best performing material requires as little as 11 wt.% MgO for structural stabilization and exceeds the CO 2 uptake of the limestone-derived reference material by ~500%.

Dynamic acid/base equilibrium in single component switchable ionic liquids and consequences on viscosity

DOE PAGES

Cantu, David C.; Lee, Juntaek; Lee, Mal -Soon; ...

2016-03-28

The deployment of transformational non-aqueous CO 2-capture solvent systems is encumbered by high viscosity even at intermediate uptakes. Using single-molecule CO 2 binding organic liquids as a prototypical example, we identify the key molecular features controlling bulk liquid viscosity and CO 2 uptake kinetics. Fast uptake kinetics arise from close proximity of the alcohol and amine sites that are involved in CO 2 binding. This process results in the concerted formation of a Zwitterion containing both an alkylcarbonate and a protonated amine. The hydrogen bonding between the two functional groups ultimately determines the solution viscosity. Based on molecular simulation, thismore » work reveals options to significantly reduce viscosity with molecular modifications that shift the proton transfer equilibrium towards a neutral acid/amine species as opposed to the ubiquitously accepted Zwitterionic state. Lastly, the molecular design concepts proposed here, for the alkyl-carbonate systems, are readily extensible to other CO 2 capture technologies, such as the carbamate- or imidazole-based solvent chemistries.« less

Two-dimensional nitrides as highly efficient potential candidates for CO2 capture and activation.

PubMed

Morales-Salvador, Raul; Morales-García, Ángel; Viñes, Francesc; Illas, Francesc

2018-06-13

The performance of novel two-dimensional nitrides in carbon capture and storage (CCS) is analyzed for a broad range of pressures and temperatures. Employing an integrated theoretical framework where CO2 adsorption/desorption rates on the M2N (M = Ti, Zr, Hf, V, Nb, Ta, Cr, Mo, and W) surfaces are derived from transition state theory and density functional theory based calculations, the present theoretical simulations consistently predict that, depending on the particular composition, CO2 can be strongly adsorbed and even activated at temperatures above 1000 K. For practical purposes, Ti2N, Zr2N, Hf2N, V2N, Nb2N, and Ta2N are predicted as the best suited materials for CO2 activation. Moreover, the estimated CO2 uptake of 2.32-7.96 mol CO2 kg-1 reinforces the potential of these materials for CO2 abatement.

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.

Global carbon management using air capture and geosequestration at remote locations

NASA Astrophysics Data System (ADS)

Lackner, K. S.; Goldberg, D.

2014-12-01

CO2 emissions need not only stop; according the IPCC, emissions need to turn negative. This requires means to remove CO2 from air and store it safely and permanently. We outline a combination of secure geosequestration and direct capture of CO2 from ambient air to create negative emissions at remote locations. Operation at remote sites avoids many difficulties associated with capture at the source, where space for added equipment is limited, good storage sites are in short supply, and proximity to private property engenders resistance. Large Igneous Provinces have been tested as secure CO2 reservoirs. CO2 and water react with reservoir rock to form stable carbonates, permanently sequestering the carbon. Outfitting reservoirs in large igneous provinces far from human habitation with ambient air capture systems creates large CO2 sequestration sites. Their remoteness offers advantages in environmental security and public acceptance and, thus, can smooth the path toward CO2 stabilization. Direct capture of CO2 from ambient air appears energetically and economically viable and could be scaled up quickly. Thermodynamic energy requirements are very small and a number of approaches have shown to be energy efficient in practice. Sorbent technologies include supported organoamines, alkaline brines, and quaternary ammonium based ion-exchange resins. To demonstrate that the stated goals of low cost and low energy consumption can be reached at scale, public research and demonstration projects are essential. We suggest co-locating air capture and geosequestration at sites where renewable energy resources can power both activities. Ready renewable energy would also allow for the co-production of synthetic fuels. Possible locations with large wind and basalt resources include Iceland and Greenland, the north-western United States, the Kerguelen plateau, Siberia and Morocco. Capture and sequestration in these reservoirs could recover all of the emissions of the 20th century and still contribute to a carbon neutral economy throughout the 21st century. Mobilizing industrial infrastructure to these areas poses a challenge. However, the urgency of the climate problem requires immediate action, with economic incentives and commitments to site evaluation and engineering development.

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.

Ship-in-a-bottle synthesis of amine-functionalized ionic liquids in NaY zeolite for CO2 capture

PubMed Central

Yu, Yinghao; Mai, Jingzhang; Wang, Lefu; Li, Xuehui; Jiang, Zheng; Wang, Furong

2014-01-01

CO2 capture on solid materials possesses significant advantages on the operation cost, process for large-scale CO2 capture and storage (CCS) that stimulates great interest in exploring high-performance solid CO2 adsorbents. A ship-in-a-bottle strategy was successfully developed to prepare the [APMIM]Br@NaY host–guest system in which an amine-functionalized ionic liquid (IL), 1-aminopropyl-3-methylimidazolium bromide ([APMIM]Br), was in-situ encapsulated in the NaY supercages. The genuine host-guest systems were thoroughly characterized and tested in CO2 capture from simulated flue gas. It was evidenced the encapsulated ILs are more stable than the bulk ILs. These host–guest systems exhibited superb overall CO2 capture capacity up to 4.94 mmol g−1 and the chemically adsorbed CO2 achieved 1.85 mmol g−1 depending on the [APMIM]Br loading amount. The chemisorbed CO2 can be desorbed rapidly by flushing with N2 gas at 50°C. The optimized [APMIM]Br@NaY system remains its original CO2 capture capacity in multiple cycling tests under prolonged harsh adsorption-desorption conditions. The excellent physicochemical properties and the CO2 capture performance of the host-guest systems offer them great promise for the future practice in the industrial CO2 capture. PMID:25104324

Easily regenerable solid adsorbents based on polyamines for carbon dioxide capture from the air.

PubMed

Goeppert, Alain; Zhang, Hang; Czaun, Miklos; May, Robert B; Prakash, G K Surya; Olah, George A; Narayanan, S R

2014-05-01

Adsorbents prepared easily by impregnation of fumed silica with polyethylenimine (PEI) are promising candidates for the capture of CO2 directly from the air. These inexpensive adsorbents have high CO2 adsorption capacity at ambient temperature and can be regenerated in repeated cycles under mild conditions. Despite the very low CO2 concentration, they are able to scrub efficiently all CO2 out of the air in the initial hours of the experiments. The influence of parameters such as PEI loading, adsorption and desorption temperature, particle size, and PEI molecular weight on the adsorption behavior were investigated. The mild regeneration temperatures required could allow the use of waste heat available in many industrial processes as well as solar heat. CO2 adsorption from the air has a number of applications. Removal of CO2 from a closed environment, such as a submarine or space vehicles, is essential for life support. The supply of CO2-free air is also critical for alkaline fuel cells and batteries. Direct air capture of CO2 could also help mitigate the rising concerns about atmospheric CO2 concentration and associated climatic changes, while, at the same time, provide the first step for an anthropogenic carbon cycle. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Technoeconomic Assessment of an Advanced Aqueous Ammonia-Based Postcombustion Capture Process Integrated with a 650-MW Coal-Fired Power Station.

PubMed

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

2016-10-04

Using a rigorous, rate-based model and a validated economic model, we investigated the technoeconomic performance of an aqueous NH 3 -based CO 2 capture process integrated with a 650-MW coal-fired power station. First, the baseline NH 3 process was explored with the process design of simultaneous capture of CO 2 and SO 2 to replace the conventional FGD unit. This reduced capital investment of the power station by US$425/kW (a 13.1% reduction). Integration of this NH 3 baseline process with the power station takes the CO 2 -avoided cost advantage over the MEA process (US$67.3/tonne vs US$86.4/tonne). We then investigated process modifications of a two-stage absorption, rich-split configuration and interheating stripping to further advance the NH 3 process. The modified process reduced energy consumption by 31.7 MW/h (20.2% reduction) and capital costs by US$55.4 million (6.7% reduction). As a result, the CO 2 -avoided cost fell to $53.2/tonne: a savings of $14.1 and $21.9/tonne CO 2 compared with the NH 3 baseline and advanced MEA process, respectively. The analysis of energy breakdown and cost distribution indicates that the technoeconomic performance of the NH 3 process still has great potential to be improved.

Energy and economic analysis of the carbon dioxide capture installation with the use of monoethanolamine and ammonia

NASA Astrophysics Data System (ADS)

Bochon, Krzysztof; Chmielniak, Tadeusz

2015-03-01

In the study an accurate energy and economic analysis of the carbon capture installation was carried out. Chemical absorption with the use of monoethanolamine (MEA) and ammonia was adopted as the technology of carbon dioxide (CO2) capture from flue gases. The energy analysis was performed using a commercial software package to analyze the chemical processes. In the case of MEA, the demand for regeneration heat was about 3.5 MJ/kg of CO2, whereas for ammonia it totalled 2 MJ/kg CO2. The economic analysis was based on the net present value (NPV) method. The limit price for CO2 emissions allowances at which the investment project becomes profitable (NPV = 0) was more than 160 PLN/Mg for MEA and less than 150 PLN/Mg for ammonia. A sensitivity analysis was also carried out to determine the limit price of CO2 emissions allowances depending on electricity generation costs at different values of investment expenditures.

Evaluation of Solid Sorbents as a Retrofit Technology for CO 2 Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sjostrom, Sharon

2016-06-02

ADA completed a DOE-sponsored program titled Evaluation of Solid Sorbents as a Retrofit Technology for CO 2 Capture under program DE-FE0004343. During this program, sorbents were analyzed for use in a post-combustion CO 2 capture process. A supported amine sorbent was selected based upon superior performance to adsorb a greater amount of CO 2 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 sorbentmore » CO 2 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 CO 2 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 CO 2 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 CO 2 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 temperatures combined with pre-loading of the sorbent with CO 2 prior to entering the adsorber. Specifically, CO 2-rich gas was utilized to convey sorbent from the regenerator to the adsorber. This gas was nominally 45°C below the regenerator temperature during testing. ADA’s post-combustion capture system with modifications to overcome pilot constraints, in conjunction with incorporating a sorbent with CO 2 working capacity of 15 g CO 2/100 g sorbent and a contact time of 10 to 15 minutes or less with flue gas could provide significant cost and performance benefits when compared to an MEA system.« less

Novel shortcut estimation method for regeneration energy of amine solvents in an absorption-based carbon capture process.

PubMed

Kim, Huiyong; Hwang, Sung June; Lee, Kwang Soon

2015-02-03

Among various CO2 capture processes, the aqueous amine-based absorption process is considered the most promising for near-term deployment. However, the performance evaluation of newly developed solvents still requires complex and time-consuming procedures, such as pilot plant tests or the development of a rigorous simulator. Absence of accurate and simple calculation methods for the energy performance at an early stage of process development has lengthened and increased expense of the development of economically feasible CO2 capture processes. In this paper, a novel but simple method to reliably calculate the regeneration energy in a standard amine-based carbon capture process is proposed. Careful examination of stripper behaviors and exploitation of energy balance equations around the stripper allowed for calculation of the regeneration energy using only vapor-liquid equilibrium and caloric data. Reliability of the proposed method was confirmed by comparing to rigorous simulations for two well-known solvents, monoethanolamine (MEA) and piperazine (PZ). The proposed method can predict the regeneration energy at various operating conditions with greater simplicity, greater speed, and higher accuracy than those proposed in previous studies. This enables faster and more precise screening of various solvents and faster optimization of process variables and can eventually accelerate the development of economically deployable CO2 capture processes.

Economics of carbon dioxide capture and utilization-a supply and demand perspective.

PubMed

Naims, Henriette

2016-11-01

Lately, the technical research on carbon dioxide capture and utilization (CCU) has achieved important breakthroughs. While single CO 2 -based innovations are entering the markets, the possible economic effects of a large-scale CO 2 utilization still remain unclear to policy makers and the public. Hence, this paper reviews the literature on CCU and provides insights on the motivations and potential of making use of recovered CO 2 emissions as a commodity in the industrial production of materials and fuels. By analyzing data on current global CO 2 supply from industrial sources, best practice benchmark capture costs and the demand potential of CO 2 utilization and storage scenarios with comparative statics, conclusions can be drawn on the role of different CO 2 sources. For near-term scenarios the demand for the commodity CO 2 can be covered from industrial processes, that emit CO 2 at a high purity and low benchmark capture cost of approximately 33 €/t. In the long-term, with synthetic fuel production and large-scale CO 2 utilization, CO 2 is likely to be available from a variety of processes at benchmark costs of approx. 65 €/t. Even if fossil-fired power generation is phased out, the CO 2 emissions of current industrial processes would suffice for ambitious CCU demand scenarios. At current economic conditions, the business case for CO 2 utilization is technology specific and depends on whether efficiency gains or substitution of volatile priced raw materials can be achieved. Overall, it is argued that CCU should be advanced complementary to mitigation technologies and can unfold its potential in creating local circular economy solutions.

The Concept and Analytical Investigation of CO2 and Steam Co-Electrolysis for Resource Utilization in Space Exploration

NASA Technical Reports Server (NTRS)

McKellar, Michael G.; Stoots, Carl M.; Sohal, Manohar S.; Mulloth, Lila M.; Luna, Bernadette; Abney, Morgan B.

2010-01-01

CO2 acquisition and utilization technologies will have a vital role in designing sustainable and affordable life support and in situ fuel production architectures for human and robotic exploration of Moon and Mars. For long-term human exploration to be practical, reliable technologies have to be implemented to capture the metabolic CO2 from the cabin air and chemically reduce it to recover oxygen. Technologies that enable the in situ capture and conversion of atmospheric CO2 to fuel are essential for a viable human mission to Mars. This paper describes the concept and mathematical analysis of a closed-loop life support system based on combined electrolysis of CO2 and steam (co-electrolysis). Products of the coelectrolysis process include oxygen and syngas (CO and H2) that are suitable for life support and synthetic fuel production, respectively. The model was developed based on the performance of a co-electrolysis system developed at Idaho National Laboratory (INL). Individual and combined process models of the co-electrolysis and Sabatier, Bosch, Boudouard, and hydrogenation reactions are discussed and their performance analyses in terms of oxygen production and CO2 utilization are presented.

The Ca-looping process for CO2 capture and energy storage: role of nanoparticle technology

NASA Astrophysics Data System (ADS)

Valverde, Jose Manuel

2018-02-01

The calcium looping (CaL) process, based on the cyclic carbonation/calcination of CaO, has come into scene in the last years with a high potential to be used in large-scale technologies aimed at mitigating global warming. In the CaL process for CO2 capture, the CO2-loaded flue gas is used to fluidize a bed of CaO particles at temperatures around 650 °C. The carbonated particles are then circulated into a calciner reactor wherein the CaO solids are regenerated at temperatures near 950 °C under high CO2 concentration. Calcination at such harsh conditions causes a marked sintering and loss of reactivity of the regenerated CaO. This main drawback could be however compensated from the very low cost of natural CaO precursors such as limestone or dolomite. Another emerging application of the CaL process is thermochemical energy storage (TCES) in concentrated solar power (CSP) plants. Importantly, carbonation/calcination conditions to maximize the global CaL-CSP plant efficiency could differ radically from those used for CO2 capture. Thus, carbonation could be carried out at high temperatures under high CO2 partial pressure for maximum efficiency, whereas the solids could be calcined at relatively low temperatures in the absence of CO2 to promote calcination. Our work highlights the critical role of carbonation/calcination conditions on the performance of CaO derived from natural precursors. While conditions in the CaL process for CO2 capture lead to a severe CaO deactivation with the number of cycles, the same material may exhibit a high and stable conversion at optimum CaL-CSP conditions. Moreover, the type of CaL conditions influences critically the reaction kinetics, which plays a main role on the optimization of relevant operation parameters such as the residence time in the reactors. This paper is devoted to a brief review on the latest research activity in our group concerning these issues as well as the possible role of nanoparticle technology to enhance the activity of Ca-based materials at CaL conditions for CO2 capture and energy storage.

Electrochemical Membrane for Carbon Dioxide Capture and Power Generation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ghezel-Ayagh, Hossein

FuelCell Energy, Inc. (FCE), in collaboration with AECOM Corporation (formerly URS Corporation) and Pacific Northwest National Laboratory, has been developing a novel Combined Electric Power and Carbon-dioxide Separation (CEPACS) system. The CEPACS system is based on electrochemical membrane (ECM) technology derived from FCE’s carbonate fuel cell products featuring internal (methane steam) reforming and carrying the trade name of Direct FuelCell®. The unique chemistry of carbonate fuel cells offers an innovative approach for separation of CO 2 from existing fossil-fuel power plant exhaust streams (flue gases). The ECM-based CEPACS system has the potential to become a transformational CO 2-separation technology bymore » working as two devices in one: it separates the CO 2 from the exhaust of other plants such as an existing coal-fired plant and simultaneously produces clean electric power at high efficiency using a supplementary fuel. The development effort was carried out under the U.S. Department of Energy (DOE) cooperative agreement DE-FE0007634. The overall objective of this project was to successfully demonstrate the ability of FCE’s ECM-based CEPACS system technology to separate ≥90% of the CO 2 from a simulated Pulverized Coal (PC) power plant flue gas stream and to compress the captured CO2 to a state that can be easily transported for sequestration or beneficial use. In addition, a key objective was to show, through the technical and economic feasibility study and bench scale testing, that the ECM-based CEPACS system is an economical alternative for CO 2 capture in PC power plants, and that it meets DOE’s objective related to the incremental cost of electricity (COE) for post-combustion CO 2 capture (no more than 35% increase in COE). The project was performed in three budget periods (BP). The specific objective for BP1 was to complete the Preliminary Technical and Economic Feasibility Study. The T&EF study was based on the carbon capture system size suitable for a reference 550 MW PC power plant. The specific objectives for BP2 were to perform (flue gas) contaminant effect evaluation tests, small area membrane tests using clean simulated flue gas, design a flue gas pretreatment system for processing of the gas feed to ECM, update the Technical & Economic Feasibility Study (T&EFS) incorporating results of contaminant effect tests and small area membrane tests, and to prepare a test facility for bench scale testing. The specific objectives for BP3 were to perform bench scale testing (parametric and long-duration testing) of a 11.7 m 2 ECM-based CO 2 capture, purification and compression system, and update (as final) the Technical and Economic Feasibility Study. In addition, an Environmental Health and Safety evaluation (assessment) of the ECM technology was included. This final technical report presents the progress made under the project.« less

Techno-Economic Analysis of a Secondary Air Stripper Process

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heberle, J.R.; Nikolic, Heather; Thompson, Jesse

We present results of an initial techno-economic assessment on a post-combustion CO2 capture process developed by the Center for Applied Energy Research (CAER) at the University of Kentucky using Mitsubishi Hitachi Power Systems’ H3-1 aqueous amine solvent. The analysis is based on data collected at a 0.7 MWe pilot unit combined with laboratory data and process simulations. The process adds a secondary air stripper to a conventional solvent process, which increases the cyclic loading of the solvent in two ways. First, air strips additional CO2 from the solvent downstream of the conventional steam-heated thermal stripper. This extra stripping of CO2more » reduces the lean loading entering the absorber. Second, the CO2-enriched air is then sent to the boiler for use as secondary air. This recycling of CO2 results in a higher concentration of CO2 in the flue gas sent to the absorber, and hence a higher rich loading of the solvent exiting the absorber. A process model was incorporated into a full-scale supercritical pulverized coal power plant model to determine the plant performance and heat and mass balances. The performance and heat and mass balance data were used to size equipment and develop cost estimates for capital and operating costs. Lifecycle costs were considered through a levelized cost of electricity (LCOE) assessment based on the capital cost estimate and modeled performance. The results of the simulations show that the CAER process yields a regeneration energy of 3.12 GJ/t CO2, a $53.05/t CO2 capture cost, and LCOE of $174.59/MWh. This compares to the U.S. Department of Energy’s projected costs (Case 10) of regeneration energy of 3.58 GJ/t CO2 , a $61.31/t CO2 capture cost, and LCOE of $189.59/MWh. For H3-1, the CAER process results in a regeneration energy of 2.62 GJ/tCO2 with a stripper pressure of 5.2 bar, a capture cost of $46.93/t CO2, and an LCOE of $164.33/MWh.« less

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

Innovative nano-layered solid sorbents for CO2 capture.

PubMed

Li, Bingyun; Jiang, Bingbing; Fauth, Daniel J; Gray, McMahan L; Pennline, Henry W; Richards, George A

2011-02-14

Nano-layered sorbents for CO(2) capture, for the first time, were developed using layer-by-layer nanoassembly. A CO(2)-adsorbing polymer and a strong polyelectrolyte were alternately immobilized within porous particles. The developed sorbents had fast CO(2) adsorption and desorption properties and their CO(2) capture capacity increased with increasing nano-layers of the CO(2)-adsorbing polymer.

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

NASA Astrophysics Data System (ADS)

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

2013-10-01

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

Electricity without carbon dioxide: Assessing the role of carbon capture and sequestration in United States electric markets

NASA Astrophysics Data System (ADS)

Johnson, Timothy Lawrence

2002-09-01

Stabilization of atmospheric greenhouse gas concentrations will likely require significant cuts in electric sector carbon dioxide (CO2) emissions. The ability to capture and sequester CO2 in a manner compatible with today's fossil-fuel based power generating infrastructure offers a potentially low-cost contribution to a larger climate change mitigation strategy. This thesis fills a niche between economy-wide studies of CO 2 abatement and plant-level control technology assessments by examining the contribution that carbon capture and sequestration (CCS) might make toward reducing US electric sector CO2 emissions. The assessment's thirty year perspective ensures that costs sunk in current infrastructure remain relevant and allows time for technological diffusion, but remains free of assumptions about the emergence of unidentified radical innovations. The extent to which CCS might lower CO2 mitigation costs will vary directly with the dispatch of carbon capture plants in actual power-generating systems, and will depend on both the retirement of vintage capacity and competition from abatement alternatives such as coal-to-gas fuel switching and renewable energy sources. This thesis therefore adopts a capacity planning and dispatch model to examine how the current distribution of generating units, natural gas prices, and other industry trends affect the cost of CO2 control via CCS in an actual US electric market. The analysis finds that plants with CO2 capture consistently provide significant reductions in base-load emissions at carbon prices near 100 $/tC, but do not offer an economical means of meeting peak demand unless CO2 reductions in excess of 80 percent are required. Various scenarios estimate the amount by which turn-over of the existing generating infrastructure and the severity of criteria pollutant constraints reduce mitigation costs. A look at CO2 sequestration in the seabed beneath the US Outer Continental Shelf (OCS) complements this model-driven assessment by considering issues of risk, geological storage capacity, and regulation. Extensive experience with offshore oil and gas operations suggests that the technical uncertainties associated with OCS sequestration are not large. The legality of seabed CO 2 disposal under US law and international environmental agreements, however, is ambiguous, and the OCS may be the first region where these regulatory regimes clash over CO2 sequestration.

Bench-Scale Development of a Hot Carbonate Absorption Process with Crystallization-Enabled High-Pressure Stripping for Post-Combustion CO{sub 2} Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lu, Yongqi; DeVries, Nicholas; Ruhter, David

A novel Hot Carbonate Absorption Process with Crystallization-Enabled High-Pressure Stripping (Hot-CAP) has been developed by the University of Illinois at Urbana-Champaign and Carbon Capture Scientific, LLC in this three-year, bench-scale project. The Hot-CAP features a concentrated carbonate solution (e.g., K{sub 2}CO{sub 3}) for CO{sub 2} absorption and a bicarbonate slurry (e.g., KHCO{sub 3}) for high-pressure CO{sub 2} stripping to overcome the energy use and other disadvantages associated with the benchmark monoethanolamine (MEA) process. The project was aimed at performing laboratory- and bench-scale experiments to prove its technical feasibility and generate process engineering and scale-up data, and conducting a techno-economic analysismore » (TEA) to demonstrate its energy use and cost competitiveness over MEA. To meet project goals and objectives, a combination of experimental, modeling, process simulation, and economic analysis studies were applied. Carefully designed and intensive experiments were conducted to measure thermodynamic and reaction engineering data relevant to four major unit operations in the Hot-CAP (i.e., CO{sub 2} absorption, CO{sub 2} stripping, bicarbonate crystallization, and sulfate reclamation). The rate promoters that could accelerate the CO{sub 2} absorption rate into the potassium carbonate/bicarbonate (PCB) solution to a level greater than that into the 5 M MEA solution were identified, and the superior performance of CO{sub 2} absorption into PCB was demonstrated in a bench-scale packed-bed column. Kinetic data on bicarbonate crystallization were developed and applied for crystallizer design and sizing. Parametric testing of high-pressure CO{sub 2} stripping with concentrated bicarbonate-dominant slurries at high temperatures ({>=}140{degrees}C) in a bench-scale stripping column demonstrated lower heat use than with MEA. The feasibility of a modified process for combining SO{sub 2} removal with CO{sub 2} capture was preliminarily demonstrated. In addition to the experimental studies, the technical challenges pertinent to fouling of slurry-handling equipment and the design of the crystallizer and stripper were addressed through consultation with vendors and engineering analyses. A process flow diagram of the Hot-CAP was then developed and a TEA was performed to compare the energy use and cost performance of a nominal 550-MWe subcritical pulverized coal (PC)-fired power plant without CO{sub 2} capture (DOE/NETL Case 9) with the benchmark MEA-based post-combustion CO{sub 2} capture (PCC; DOE/NETL Case 10) and the Hot-CAP-based PCC. The results revealed that the net power produced in the PC + Hot-CAP is 609 MWe, greater than the PC + MEA (550 MWe). The 20-year levelized cost of electricity (LCOE) for the PC + Hot-CAP, including CO{sub 2} transportation and storage, is 120.3 mills/kWh, a 60% increase over the base PC plant without CO{sub 2} capture. The LCOE increase for the Hot-CAP is 29% lower than that for MEA. TEA results demonstrated that the Hot-CAP is energy-efficient and cost-effective compared with the benchmark MEA process.« less

Bench-Scale Silicone Process for Low-Cost CO{sub 2} Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vipperla, Ravikumar; Yee, Michael; Steele, Ray

This report presents system and economic analysis for a carbon capture unit which uses an amino-silicone solvent for CO{sub 2} capture and sequestration (CCS) in a pulverized coal (PC) boiler. The amino-silicone solvent is based on GAP-1 with tri-ethylene glycol (TEG) as a co-solvent. For comparison purposes, the report also shows results for a CCS unit based on a conventional approach using mono-ethanol amine (MEA). At a steam temperature of 395 °C (743 °F), the CCS energy penalty for amino-silicone solvent is only 30.4% which compares to a 35.9% energy penalty for MEA. The increase in COE for the amino-siliconemore » solvent relative to the non-capture case is between 98% and 103% (depending on the solvent cost) which compares to an ~109% COE cost increase for MEA. In summary, the amino-silicone solvent has significant advantages over conventional systems using MEA.« less

Holey graphene frameworks for highly selective post-combustion carbon capture

PubMed Central

Chowdhury, Shamik; Balasubramanian, Rajasekhar

2016-01-01

Atmospheric CO2 concentrations continue to rise rapidly in response to increased combustion of fossil fuels, contributing to global climate change. In order to mitigate the effects of global warming, development of new materials for cost-effective and energy-efficient CO2 capture is critically important. Graphene-based porous materials are an emerging class of solid adsorbents for selectively removing CO2 from flue gases. Herein, we report a simple and scalable approach to produce three-dimensional holey graphene frameworks with tunable porosity and pore geometry, and demonstrate their application as high-performance CO2 adsorbents. These holey graphene macrostructures exhibit a significantly improved specific surface area and pore volume compared to their pristine counterparts, and can be effectively used in post-combustion CO2 adsorption systems because of their intrinsic hydrophobicity together with good gravimetric storage capacities, rapid removal capabilities, superior cycling stabilities, and moderate initial isosteric heats. In addition, an exceptionally high CO2 over N2 selectivity can be achieved under conditions relevant to capture from the dry exhaust gas stream of a coal burning power plant, suggesting the possibility of recovering highly pure CO2 for long-term sequestration and/or utilization for downstream applications. PMID:26879393

Holey graphene frameworks for highly selective post-combustion carbon capture.

PubMed

Chowdhury, Shamik; Balasubramanian, Rajasekhar

2016-02-16

Atmospheric CO2 concentrations continue to rise rapidly in response to increased combustion of fossil fuels, contributing to global climate change. In order to mitigate the effects of global warming, development of new materials for cost-effective and energy-efficient CO2 capture is critically important. Graphene-based porous materials are an emerging class of solid adsorbents for selectively removing CO2 from flue gases. Herein, we report a simple and scalable approach to produce three-dimensional holey graphene frameworks with tunable porosity and pore geometry, and demonstrate their application as high-performance CO2 adsorbents. These holey graphene macrostructures exhibit a significantly improved specific surface area and pore volume compared to their pristine counterparts, and can be effectively used in post-combustion CO2 adsorption systems because of their intrinsic hydrophobicity together with good gravimetric storage capacities, rapid removal capabilities, superior cycling stabilities, and moderate initial isosteric heats. In addition, an exceptionally high CO2 over N2 selectivity can be achieved under conditions relevant to capture from the dry exhaust gas stream of a coal burning power plant, suggesting the possibility of recovering highly pure CO2 for long-term sequestration and/or utilization for downstream applications.

Holey graphene frameworks for highly selective post-combustion carbon capture

NASA Astrophysics Data System (ADS)

Chowdhury, Shamik; Balasubramanian, Rajasekhar

2016-02-01

Atmospheric CO2 concentrations continue to rise rapidly in response to increased combustion of fossil fuels, contributing to global climate change. In order to mitigate the effects of global warming, development of new materials for cost-effective and energy-efficient CO2 capture is critically important. Graphene-based porous materials are an emerging class of solid adsorbents for selectively removing CO2 from flue gases. Herein, we report a simple and scalable approach to produce three-dimensional holey graphene frameworks with tunable porosity and pore geometry, and demonstrate their application as high-performance CO2 adsorbents. These holey graphene macrostructures exhibit a significantly improved specific surface area and pore volume compared to their pristine counterparts, and can be effectively used in post-combustion CO2 adsorption systems because of their intrinsic hydrophobicity together with good gravimetric storage capacities, rapid removal capabilities, superior cycling stabilities, and moderate initial isosteric heats. In addition, an exceptionally high CO2 over N2 selectivity can be achieved under conditions relevant to capture from the dry exhaust gas stream of a coal burning power plant, suggesting the possibility of recovering highly pure CO2 for long-term sequestration and/or utilization for downstream applications.

Energy and material balance of CO2 capture from ambient air.

PubMed

Zeman, Frank

2007-11-01

Current Carbon Capture and Storage (CCS) technologies focus on large, stationary sources that produce approximately 50% of global CO2 emissions. We propose an industrial technology that captures CO2 directly from ambient air to target the remaining emissions. First, a wet scrubbing technique absorbs CO2 into a sodium hydroxide solution. The resultant carbonate is transferred from sodium ions to calcium ions via causticization. The captured CO2 is released from the calcium carbonate through thermal calcination in a modified kiln. The energy consumption is calculated as 350 kJ/mol of CO2 captured. It is dominated by the thermal energy demand of the kiln and the mechanical power required for air movement. The low concentration of CO2 in air requires a throughput of 3 million cubic meters of air per ton of CO2 removed, which could result in significant water losses. Electricity consumption in the process results in CO2 emissions and the use of coal power would significantly reduce to net amount captured. The thermodynamic efficiency of this process is low but comparable to other "end of pipe" capture technologies. As another carbon mitigation technology, air capture could allow for the continued use of liquid hydrocarbon fuels in the transportation sector.

Carbon dioxide capture using covalent organic frameworks (COFs) type material-a theoretical investigation.

PubMed

Dash, Bibek

2018-04-26

The present work deals with a density functional theory (DFT) study of porous organic framework materials containing - groups for CO 2 capture. In this study, first principle calculations were performed for CO 2 adsorption using N-containing covalent organic framework (COFs) models. Ab initio and DFT-based methods were used to characterize the N-containing porous model system based on their interaction energies upon complexing with CO 2 and nitrogen gas. Binding energies (BEs) of CO 2 and N 2 molecules with the polymer framework were calculated with DFT methods. Hybrid B3LYP and second order MP2 methods combined with of Pople 6-31G(d,p) and correlation consistent basis sets cc-pVDZ, cc-pVTZ and aug-ccVDZ were used to calculate BEs. The effect of linker groups in the designed covalent organic framework model system on the CO 2 and N 2 interactions was studied using quantum calculations.

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 for global climate policy are examined using DIAM [2], a stylized integrated assessment model. We find that air capture can fundamentally alter the temporal dynamics of global warming mitigation. The reason for this is that air capture differs from conventional mitigation in three key aspects. First, it removes emissions from any part of the economy with equal ease or difficulty, so its cost provides an absolute cap on the cost of mitigation. Second, it permits reduction in concentrations faster than the natural carbon cycle: the effects of irreversibility are thus partly alleviated. Third, because it is less coupled with the energy system, air capture may offer stronger economies of scale and smaller adjustment costs than the more conventional mitigation technologies. Air capture limits the total cost of a worst-case climate scenario. In an optimal sequential decision framework with uncertainty, existence of air capture decreases the need for near-term precautionary abatement. Like geoengineering, air capture thus poses a moral hazard. 1. S. Elliott, et al. Compensation of atmospheric CO2 buildup through engineered chemical sinkage. Geophys. Res. Let., 28:1235-1238, 2001. 2. Minh Ha-Duong, Michael J. Grubb, and Jean-Charles Hourcade. Influence of socioeconomic inertia and uncertainty on optimal CO2-emission abatement. Nature, 390: 270-274, 1997.

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

PubMed

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

2013-07-02

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

Novel Application of Carbonate Fuel Cell for Capturing Carbon Dioxide from Flue Gas Streams

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jolly, Stephen; Ghezel-Ayagh, Hossein; Willman, Carl

To address concerns about climate change resulting from emission of CO2 by coal-fueled power plants, FuelCell Energy, Inc. has developed the Combined Electric Power and Carbon-dioxide Separation (CEPACS) system concept. The CEPACS system utilizes Electrochemical Membrane (ECM) technology derived from the Company’s Direct FuelCell® products. The system separates the CO2 from the flue gas of other plants and produces electric power using a supplementary fuel. FCE is currently evaluating the use of ECM to cost effectively separate CO2 from the flue gas of Pulverized Coal (PC) power plants under a U.S. Department of Energy contract. The overarching objective of themore » project is to verify that the ECM can achieve at least 90% CO2 capture from the flue gas with no more than 35% increase in the cost of electricity. The project activities include: 1) laboratory scale operational and performance tests of a membrane assembly, 2) performance tests of the membrane to evaluate the effects of impurities present in the coal plant flue gas, in collaboration with Pacific Northwest National Laboratory, 3) techno-economic analysis for an ECM-based CO2 capture system applied to a 550 MW existing PC plant, in partnership with URS Corporation, and 4) bench scale (11.7 m2 area) testing of an ECM-based CO2 separation and purification system.« less

CO2 Accounting and Risk Analysis for CO2 Sequestration at Enhanced Oil Recovery Sites.

PubMed

Dai, Zhenxue; Viswanathan, Hari; Middleton, Richard; Pan, Feng; Ampomah, William; Yang, Changbing; Jia, Wei; Xiao, Ting; Lee, Si-Yong; McPherson, Brian; Balch, Robert; Grigg, Reid; White, Mark

2016-07-19

Using CO2 in enhanced oil recovery (CO2-EOR) is a promising technology for emissions management because CO2-EOR can dramatically reduce sequestration costs in the absence of emissions policies that include incentives for carbon capture and storage. This study develops a multiscale statistical framework to perform CO2 accounting and risk analysis in an EOR environment at the Farnsworth Unit (FWU), Texas. A set of geostatistical-based Monte Carlo simulations of CO2-oil/gas-water flow and transport in the Morrow formation are conducted for global sensitivity and statistical analysis of the major risk metrics: CO2/water injection/production rates, cumulative net CO2 storage, cumulative oil/gas productions, and CO2 breakthrough time. The median and confidence intervals are estimated for quantifying uncertainty ranges of the risk metrics. A response-surface-based economic model has been derived to calculate the CO2-EOR profitability for the FWU site with a current oil price, which suggests that approximately 31% of the 1000 realizations can be profitable. If government carbon-tax credits are available, or the oil price goes up or CO2 capture and operating expenses reduce, more realizations would be profitable. The results from this study provide valuable insights for understanding CO2 storage potential and the corresponding environmental and economic risks of commercial-scale CO2-sequestration in depleted reservoirs.

Synergistic Carbon Dioxide Capture and Conversion in Porous Materials.

PubMed

Zhang, Yugen; Lim, Diane S W

2015-08-24

Global climate change and excessive CO2 emissions have caused widespread public concern in recent years. Tremendous efforts have been made towards CO2 capture and conversion. This has led to the development of numerous porous materials as CO2 capture sorbents. Concurrently, the conversion of CO2 into value-added products by chemical methods has also been well-documented recently. However, realizing the attractive prospect of direct, in situ chemical conversion of captured CO2 into other chemicals remains a challenge. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

NASA Astrophysics Data System (ADS)

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

2017-06-01

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

Conceptual Design of Optimized Fossil Energy Systems with Capture and Sequestration of Carbon Dioxide

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nils Johnson; Joan Ogden

2010-12-31

In this final report, we describe research results from Phase 2 of a technical/economic study of fossil hydrogen energy systems with carbon dioxide (CO{sub 2}) capture and storage (CCS). CO{sub 2} capture and storage, or alternatively, CO{sub 2} capture and sequestration, involves capturing CO{sub 2} from large point sources and then injecting it into deep underground reservoirs for long-term storage. By preventing CO{sub 2} emissions into the atmosphere, this technology has significant potential to reduce greenhouse gas (GHG) emissions from fossil-based facilities in the power and industrial sectors. Furthermore, the application of CCS to power plants and hydrogen production facilitiesmore » can reduce CO{sub 2} emissions associated with electric vehicles (EVs) and hydrogen fuel cell vehicles (HFCVs) and, thus, can also improve GHG emissions in the transportation sector. This research specifically examines strategies for transitioning to large-scale coal-derived energy systems with CCS for both hydrogen fuel production and electricity generation. A particular emphasis is on the development of spatially-explicit modeling tools for examining how these energy systems might develop in real geographic regions. We employ an integrated modeling approach that addresses all infrastructure components involved in the transition to these energy systems. The overall objective is to better understand the system design issues and economics associated with the widespread deployment of hydrogen and CCS infrastructure in real regions. Specific objectives of this research are to: Develop improved techno-economic models for all components required for the deployment of both hydrogen and CCS infrastructure, Develop novel modeling methods that combine detailed spatial data with optimization tools to explore spatially-explicit transition strategies, Conduct regional case studies to explore how these energy systems might develop in different regions of the United States, and Examine how the design and cost of coal-based H{sub 2} and CCS infrastructure depend on geography and location.« less

Solvent-free nanofluid with three structure models based on the composition of a MWCNT/SiO2 core and its adsorption capacity of CO2

NASA Astrophysics Data System (ADS)

Yang, R. L.; Zheng, Y. P.; Wang, T. Y.; Li, P. P.; Wang, Y. D.; Yao, D. D.; Chen, L. X.

2018-01-01

A series of core/shell nanoparticle organic/inorganic hybrid materials (NOHMs) with different weight ratios of two components, consisting of multi-walled carbon nanotubes (MWCNTs) and silicon dioxide (SiO2) as the core were synthesized. The NOHMs display a liquid-like state in the absence of solvent at room temperature. Five NOHMs were categorized into three kinds of structure states based on different weight ratio of two components in the core, named the power strip model, the critical model and the collapse model. The capture capacities of these NOHMs for CO2 were investigated at 298 K and CO2 pressures ranging from 0 to 5 MPa. Compared with NOHMs having a neat MWCNT core, it was revealed that NOHMs with the power strip model show better adsorption capacity toward CO2 due to its lower viscosity and more reactive groups that can react with CO2. In addition, the capture capacities of NOHMs with the critical model were relatively worse than the neat MWCNT-based NOHM. The result is attributed to the aggregation of SiO2 in these samples, which may cause the consumption and hindrance of reactive groups. However, the capture capacity of NOHMs with the collapse model was the worst of all the NOHMs, owing to its lowest content of reactive groups and hollow structure in MWCNTs. In addition, they presented non-interference of MWCNTs and SiO2 without aggregation state.

Water Vapor Adsorption on Biomass Based Carbons under Post-Combustion CO2 Capture Conditions: Effect of Post-Treatment

PubMed Central

Querejeta, Nausika; Plaza, Marta G.; Rubiera, Fernando; Pevida, Covadonga

2016-01-01

The effect of post-treatment upon the H2O adsorption performance of biomass-based carbons was studied under post-combustion CO2 capture conditions. Oxygen surface functionalities were partially replaced through heat treatment, acid washing, and wet impregnation with amines. The surface chemistry of the final carbon is strongly affected by the type of post-treatment: acid treatment introduces a greater amount of oxygen whereas it is substantially reduced after thermal treatment. The porous texture of the carbons is also influenced by post-treatment: the wider pore volume is somewhat reduced, while narrow microporosity remains unaltered only after acid treatment. Despite heat treatment leading to a reduction in the number of oxygen surface groups, water vapor adsorption was enhanced in the higher pressure range. On the other hand acid treatment and wet impregnation with amines reduce the total water vapor uptake thus being more suitable for post-combustion CO2 capture applications. PMID:28773488

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

NASA Astrophysics Data System (ADS)

Silva Mojica, Ernesto

Porous materials comprising polymeric and inorganic segments have attracted interest from the scientific community due to their unique properties and functionalities. The physical and chemical characteristics of these materials can be effectively exploited for adsorption applications. This dissertation covers the experimental techniques for fabrication of poly(vinyl alcohol) (PVA) and silica (SiO2) porous supports, and their functionalization with polyamines for developing adsorbents with potential applications in separation of CO2 and catalysis of organic reactions. The supports were synthesized by processes involving (i) covalent cross-linking of PVA, (ii) hydrolysis and poly-condensation of silica precursors (i,e,. sol-gel synthesis), and formation of porous structures via (iii) direct templating and (iv) phase inversion techniques. Their physical structure was controlled by the proper combination of the preparation procedures, which resulted in micro-structured porous materials in the form of micro-particles, membranes, and pellets. Their adsorption characteristics were tailored by functionalization with polyethyleneimine (PEI), and their physicochemical properties were characterized by vibrational spectroscopy (FTIR, UV-vis), microscopy (SEM), calorimetry (TGA, DSC), and adsorption techniques (BET, step-switch adsorption). Spectroscopic investigations of the interfacial cross-linking reactions of PEI and PVA with glutaraldehyde (GA) revealed that PEI catalyzes the cross-linking reactions of PVA in absence of external acid catalysts. In-situ IR spectroscopy coupled with a focal plane array (FPA) image detector allowed the characterization of a gradient interface on a PEI/PVA composite membrane and the investigation of the cross-linking reactions as a function of time and position. The results served as a basis to postulate possible intermediates, and propose the reaction mechanisms. The formulation of amine-functionalized CO2 capture sorbents was based on the spectroscopic investigation of the interactions of CO 2 with amine molecules under simulated CO2 capture conditions. Industrial CO2 capture processes involve fluidization and require degradation-resistant sorbents in the form of pellets. Agglomeration of silica-based CO2 capture sorbents involved the formulation of a polymer binder solution and the design of a scalable pelletization process. The characterization of these pellets revealed the formation of a CO 2-permeable polymer-silica network, which is resistant to attrition, and exhibits similar CO2 capture and degradation performance as the non-pelletized sorbents. The performance of these sorbents and pellets was tested in lab-scale and bench-scale adsorption units, using in-house fabricated fixed-bed and fluidized-bed reactors. A compartmental modeling technique was used to simulate the CO2 adsorption process and to elucidate the kinetic and thermodynamic parameters that impact the commercial viability of emerging CO2 capture technologies. The fundamental concepts and experimental techniques developed for the preparation of CO2 capture sorbents served as a basis for fabricating amine-functionalized polymer-silica hybrids for applications in catalysis of organic reactions. (i) Basic catalysts for carbon-carbon addition reactions were prepared by immobilization of amine molecules on silica supports. The activity of these catalysts and the mechanisms of base-catalyzed organic condensation reactions were investigated by an in-situ FTIR micro-scale reactor. (ii) Particle-loaded PVA composite membranes were selected for immobilization of glucose oxidase (GOx). GOx was immobilized by adsorption at pH values between 3.5 and 7.1. The results showed that adsorption was primarily achieved via hydrophobic interactions, and that PVA membranes loaded with amine-functionalized particles could help retain the activity of immobilized GOx by providing a proper hydrophilic/hydrophobic balance to the immobilized enzymes micro-environment.

Computational evaluation of metal-organic frameworks for carbon dioxide capture

NASA Astrophysics Data System (ADS)

Yu, Jiamei

Metal-organic frameworks (MOFs), a new class of porous solids comprised of metal-containing nodes linked by organic ligands, have become promising materials for gas separations. In particular, their flexible chemistry makes them attractive for CO2 capture from flue gas streams in post-combustion plants. Although numerous efforts have been exerted on the investigation of MOFs for CO2 capture, the exploration of the effects from coexisting components present in very dilute proportions in flue gases is limited because of the experimental difficulty to determine the coadsorption of CO2 with trace components. In this regard, molecular simulations show superiority. In this study, molecular simulations are used to estimate the influence of impurities: water, O2, and SO2 on post-combustion CO2 capture in MOFs. Firstly, two MOFs with coordinatively unsaturated metal sites (CUMs), HKUST-1 and Mg-MOF-74 are explored. Increase of CO 2 adsorption is observed for hydrated HKUST-1; on the contrary, the opposite water adsorption behavior is observed in hydrated Mg-MOF-74, leading to decrease of CO2 adsorption. Further, water effects on CO 2 capture in M-HKUST1 (M = Mg, Zn, Co, Ni) are evaluated to test whether comparing the binding energy could be a general method to evaluate water effects in MOFs with CUMs. It is found that the method works well for Zn-, Co-, and Ni-HKUST1 but partially for Mg-HKUST1. In addition, the effects of O2 and SO2 on CO2 capture in MOFs are also investigated for the first time, showing that the effects of O2 may be negligible but SO2 has negative effects in the CO 2 capture process in HKUST-1 systems. Secondly, the influences of water on CO2 capture in three UiO-66 MOFs with functional groups, --NH2, --OH and --Br are explored, respectively. For UiO-66-NH2 and -OH, the presence of water lowers CO2 adsorption significantly; in contrast, water shows much smaller effects in UiO-66-Br. Moreover, the presence of SO 2 decreases water adsorption but enhances CO2 uptakes slightly in both UiO-66-NH2 and -Br. Finally, the effects of impurities on CO2 capture in a MOF with suitable pore size (PCN-200) are analyzed. The adsorption of both CO 2 and N2 decrease substantially even with 1% water present in the mixture. In addition, the presence of low SO2 does not show obvious effect in PCN-200. However, a lower CO2 adsorption is observed for a mixture with a high SO2 content. In collaboration with experimental groups, the performances of three new MOFs in CO2 capture are evaluated using molecular simulations. The computational results demonstrate the feasibility of precisely designing single-molecule traps (SMT) for CO2 capture. Also, a multi-functional MOF with micro-porosity, open Cu2+ sites and amine groups has also proved computationally the selective adsorption of CO2 over CH4 and N2. Last, we demonstrate that charge separation is an effective strategy for improving CO2 capture in MOFs.

Dynamic modeling and control of a solid-sorbent CO{sub 2} capture process with two-stage bubbling fluidized bed adsorber reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Modekurti, S.; Bhattacharyya, D.; Zitney, S.

2012-01-01

Solid-sorbent-based CO{sub 2} capture processes have strong potential for reducing the overall energy penalty for post-combustion capture from the flue gas of a conventional pulverized coal power plant. However, the commercial success of this technology is contingent upon it operating over a wide range of capture rates, transient events, malfunctions, and disturbances, as well as under uncertainties. To study these operational aspects, a dynamic model of a solid-sorbent-based CO{sub 2} capture process has been developed. In this work, a one-dimensional (1D), non-isothermal, dynamic model of a two-stage bubbling fluidized bed (BFB) adsorber-reactor system with overflow-type weir configuration has been developedmore » in Aspen Custom Modeler (ACM). The physical and chemical properties of the sorbent used in this study are based on a sorbent (32D) developed at National Energy Technology Laboratory (NETL). Each BFB is divided into bubble, emulsion, and cloud-wake regions with the assumptions that the bubble region is free of solids while both gas and solid phases coexist in the emulsion and cloud-wake regions. The BFB dynamic model includes 1D partial differential equations (PDEs) for mass and energy balances, along with comprehensive reaction kinetics. In addition to the two BFB models, the adsorber-reactor system includes 1D PDE-based dynamic models of the downcomer and outlet hopper, as well as models of distributors, control valves, and other pressure-drop devices. Consistent boundary and initial conditions are considered for simulating the dynamic model. Equipment items are sized and appropriate heat transfer options, wherever needed, are provided. Finally, a valid pressure-flow network is developed and a lower-level control system is designed. Using ACM, the transient responses of various process variables such as flue gas and sorbent temperatures, overall CO{sub 2} capture, level of solids in the downcomer and hopper have been studied by simulating typical disturbances such as change in the temperature, flowrate, and composition of the flue gas. To maintain the overall CO{sub 2} capture at a desired level in face of the typical disturbances, two control strategies were considered–a proportional-integral-derivative (PID)-based feedback control strategy and a feedforward-augmented feedback control strategy. Dynamic simulation results show that both the strategies result in unacceptable overshoot/undershoot and a long settling time. To improve the control system performance, a linear model predictive controller (LMPC) is designed. In summary, the overall results illustrate how optimizing the operation and control of carbon capture systems can have a significant impact on the extent and the rate at which commercial-scale capture processes will be scaled-up, deployed, and used in the years to come.« less

Subtask 2.18 - Advancing CO 2 Capture Technology: Partnership for CO 2 Capture (PCO 2C) Phase III

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kay, John; Azenkeng, Alexander; Fiala, Nathan

2016-03-31

Industries and utilities continue to investigate ways to decrease their carbon footprint. Carbon capture and storage (CCS) can enable existing power generation facilities to meet the current national CO 2 reduction goals. The Partnership for CO2 Capture Phase III focused on several important research areas in an effort to find ways to decrease the cost of capture across both precombustion and postcombustion platforms. Two flue gas pretreatment technologies for postcombustion capture, an SO 2 reduction scrubbing technology from Cansolv Technologies Inc. and the Tri-Mer filtration technology that combines particulate, NOx, and SO 2 control, were evaluated on the Energy &more » Environmental Research Center’s (EERC’s) pilot-scale test system. Pretreating the flue gas should enable more efficient, and therefore less expensive, CO 2 capture. Both technologies were found to be effective in pretreating flue gas prior to CO 2 capture. Two new postcombustion capture solvents were tested, one from the Korea Carbon Capture and Sequestration R&D Center (KCRC) and one from CO 2 Solutions Incorporated. Both of these solvents showed the ability to capture CO 2 while requiring less regeneration energy, which would reduce the cost of capture. Hydrogen separation membranes from Commonwealth Scientific and Industrial Research Organisation were evaluated through precombustion testing. They are composed of vanadium alloy, which is less expensive than the palladium alloys that are typically used. Their performance was comparable to that of other membranes that have been tested at the EERC. Aspen Plus® software was used to model the KCRC and CO 2 Solutions solvents and found that they would result in significantly improved overall plant performance. The modeling effort also showed that the parasitic steam load at partial capture of 45% is less than half that of 90% overall capture, indicating savings that could be accrued if 90% capture is not required. Modeling of three regional power plants using the Carnegie Mellon Integrated Environmental Control Model showed that, among other things, the use of a bypass during partial capture may minimize the size of the capture tower(s) and result in a slight reduction in the revenue required to operate the capture facility. The results reinforced that a one-size-fits-all approach cannot be taken to adding capture to a power plant. Laboratory testing indicated that Fourier transform infrared spectroscopy could be used to continuously sample stack emissions at CO 2 capture facilities to detect and quantify any residual amine or its degradation products, particularly nitrosamines. The information gathered during Phase III is important for utility stakeholders as they determine how to reduce their CO 2 emissions in a carbon-constrained world. This subtask was funded through the EERC–U.S. Department of Energy (DOE) Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FC26-08NT43291. Nonfederal funding was provided by the North Dakota Industrial Commission, PPL Montana, Nebraska Public Power District, Tri-Mer Corporation, Montana–Dakota Utilities Co., Basin Electric Power Cooperative, KCRC/Korean Institute of Energy Research, Cansolv Technologies, and CO 2 Solutions, Inc.« less

Large Pilot Scale Testing of Linde/BASF Post-Combustion CO 2 Capture Technology at the Abbott Coal-Fired Power Plant

DOE Office of Scientific and Technical Information (OSTI.GOV)

O'Brien, Kevin C.

The work summarized in this report is the first step towards a project that will re-train and create jobs for personnel in the coal industry and continue regional economic development to benefit regions impacted by previous downturns. The larger project is aimed at capturing ~300 tons/day (272 metric tonnes/day) CO 2 at a 90% capture rate from existing coal- fired boilers at the Abbott Power Plant on the campus of University of Illinois (UI). It will employ the Linde-BASF novel amine-based advanced CO 2 capture technology, which has already shown the potential to be cost-effective, energy efficient and compact atmore » the 0.5-1.5 MWe pilot scales. The overall objective of the project is to design and install a scaled-up system of nominal 15 MWe size, integrate it with the Abbott Power Plant flue gas, steam and other utility systems, and demonstrate the viability of continuous operation under realistic conditions with high efficiency and capacity. The project will also begin to build a workforce that understands how to operate and maintain the capture plants by including students from regional community colleges and universities in the operation and evaluation of the capture system. This project will also lay the groundwork for follow-on projects that pilot utilization of the captured CO 2 from coal-fired power plants. The net impact will be to demonstrate a replicable means to (1) use a standardized procedure to evaluate power plants for their ability to be retrofitted with a pilot capture unit; (2) design and construct reliable capture systems based on the Linde-BASF technology; (3) operate and maintain these systems; (4) implement training programs with local community colleges and universities to establish a workforce to operate and maintain the systems; and (5) prepare to evaluate at the large pilot scale level various methods to utilize the resulting captured CO 2. Towards the larger project goal, the UI-led team, together with Linde, has completed a preliminary design for the carbon capture pilot plant with basic engineering and cost estimates, established permitting needs, identified approaches to address Environmental, Health, and Safety concerns related to pilot plant installation and operation, developed approaches for long-term use of the captured carbon, and established strategies for workforce development and job creation that will re-train coal operators to operate carbon capture plants. This report describes Phase I accomplishments and demonstrates that the project team is well-prepared for full implementation of Phase 2, to design, build, and operate the carbon capture pilot plant.« less

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

NASA Astrophysics Data System (ADS)

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

2014-01-01

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

Integrating Waste Heat from CO 2 Removal and Coal-Fired Flue Gas to Increase Plant Efficiency

DOE Office of Scientific and Technical Information (OSTI.GOV)

Irvin, Nick; Kowalczyk, Joseph

In project DE-FE0007525, Southern Company Services demonstrated heat integration methods for the capture and sequestration of carbon dioxide produced from pulverized coal combustion. A waste heat recovery technology (termed High Efficiency System) from Mitsubishi Heavy Industries America was integrated into an existing 25-MW amine-based CO 2 capture process (Kansai Mitsubishi Carbon Dioxide Recovery Process®1) at Southern Company’s Plant Barry to evaluate improvements in the energy performance of the pulverized coal plant and CO 2 capture process. The heat integration system consists of two primary pieces of equipment: (1) the CO 2 Cooler which uses product CO 2 gas from themore » capture process to heat boiler condensate, and (2) the Flue Gas Cooler which uses air heater outlet flue gas to further heat boiler condensate. Both pieces of equipment were included in the pilot system. The pilot CO 2 Cooler used waste heat from the 25-MW CO 2 capture plant (but not always from product CO 2 gas, as intended). The pilot Flue Gas Cooler used heat from a slipstream of flue gas taken from downstream of Plant Barry’s air heater. The pilot also included a 0.25-MW electrostatic precipitator. The 25-MW High Efficiency System operated for approximately six weeks over a four month time period in conjunction with the 25-MW CO 2 capture facility at Plant Barry. Results from the program were used to evaluate the technical and economic feasibility of full-scale implementation of this technology. The test program quantified energy efficiency improvements to a host power plant that could be realized due to the High Efficiency System. Through the execution of this project, the team verified the integrated operation of the High Efficiency System and Kansai Mitsubishi Carbon Dioxide Recovery Process®. The ancillary benefits of the High Efficiency System were also quantified, including reduced water consumption, a decrease in toxic air emissions, and better overall air quality control systems performance.« less

Co-firing coal and biomass blends and their influence on the post-combustion CO2 capture installation

NASA Astrophysics Data System (ADS)

Więckol-Ryk, Angelika; Smoliński, Adam

2017-10-01

Co-firing of biomass with coal for energy production is a well-known technology and plays an important role in the electricity sector. The post-combustion capture integrated with biomass-fired power plants (Bio-CCS) seems to be a new alternative for reducing greenhouse gas emissions. This study refers to the best known and advanced technology for post-combustion CO2 capture (PCC) based on a chemical absorption in monoethanolamine (MEA). The co-firing of hard coal with four types of biomass was investigated using a laboratory fixed bed reactor system. The comparison of gaseous products emitted from the combustion of coal and different biomass blends were determined using gas chromatography. Research proved that co-firing of biomass in fossil fuel power plants is beneficial for PCC process. It may also reduce the corrosion of CO2 capture installation. The oxygen concentration in the flue gases from hard coal combustion was comparable with the respective value for a fuel blend of biomass content of 20% w/w. It was also noted that an increase in biomass content in a sample from 20 to 40 % w/w increased the concentration of oxygen in the flue gas streams. However, this concentration should not have a significant impact on the rate of amine oxidative degradation.

The influence of the precursor and synthesis method on the CO2 capture capacity of carpet waste-based sorbents.

PubMed

Olivares-Marín, M; García, S; Pevida, C; Wong, M S; Maroto-Valer, M

2011-10-01

Adsorption is one of the most promising technologies for reducing CO(2) emissions and at present several different types of sorbents are being investigated. The use of sorbents obtained from low-cost and abundant precursors (i.e. solid wastes) appears an attractive strategy to adopt because it will contribute to a reduction not only in operational costs but also in the amount of waste that is dumped and burned in landfills every year. Following on from previous studies by the authors, in this work several carbon-based adsorbents were developed from different carpet wastes (pre-consumer and post-consumer wastes) by chemical activation with KOH at various activation temperatures (600-900 °C) and KOH:char impregnation ratios (0.5:1 to 4:1). The prepared materials were characterised by chemical analysis and gas adsorption (N(2), -196 °C; CO(2), 0 °C), and tested for CO(2) adsorption at temperatures of 25 and 100 °C. It was found that both the type of precursor and the conditions of activation (i.e. impregnation ratios, and activation temperatures), had a huge influence on the microporosity of the resultant samples and their CO(2) capture capacities. The carbon-based adsorbent that presented the maximum CO(2) capture capacities at 25 and 100 °C (13.8 wt.% and 3.1 wt.%, respectively), was prepared from a pre-consumer carpet waste and was activated at 700 °C using a KOH:char impregnation ratio of 1:1. This sample showed the highest narrow microporosity volume (0.47 cm(3) g(-1)), thus confirming that only pores of less than 1 nm are effective for CO(2) adsorption at atmospheric pressure. Copyright © 2011 Elsevier Ltd. All rights reserved.

Pilot plant studies of the CO{sub 2} capture performance of aqueous MEA and mixed MEA/MDEA solvents at the University of Regina CO{sub 2} capture technology development plant and the Boundary Dam CO{sub 2} capture demonstration

DOE Office of Scientific and Technical Information (OSTI.GOV)

Idem, R.; Wilson, M.; Tontiwachwuthikul, P.

2006-04-12

Evaluations of the benefits of using a mixed MEA/MDEA solvent for CO{sub 2} capture in terms of the heat requirement for solvent regeneration, lean and rich loadings, CO{sub 2} production, and solvent stability were performed by comparing the performance of aqueous 5 kmol/m{sup 3} MEA with that of an aqueous 4:1 molar ratio MEA/MDEA blend of 5 kmol/ml total amine concentration as a function of the operating time. The tests were performed using two pilot CO{sub 2} capture plants of the International Test Centre for CO{sub 2} Capture (ITC), which provided two different sources and compositions of flue gas. Themore » University of Regina CO{sub 2} plant (UR unit) processes flue gas from the combustion of natural gas while the Boundary Dam CO{sub 2} plant (BD unit) processes flue gas from a coal-fired electric power station. The results show that a huge heat-duty reduction can be achieved by using a mixed MEA/MDEA solution instead of a single MEA solution in an industrial environment of a CO{sub 2} capture plant. However, this benefit is dependent on whether the chemical stability of the solvent can be maintained.« less

Biocatalytic CO2 sequestration based on shell regeneration

NASA Astrophysics Data System (ADS)

Lee, S.

2012-04-01

Carbon dioxide, CO2, is one of the green gases, being uniformly distributed over the earth's surface. Recently, a variety of methods exists or has been proposed for pre- or post-emission capture and sequestration of CO2. However, CCS (carbon capture & storage) do not quarntee permanent treatment of CO2 and could ingenerate environment risks. Some organisms convert CO2 into exoskeleton (e.g., mollusks) or energy sources (e.g., plants) during metabolism under atmospheric conditions. One of representative biomaterials in ocean is bivalve shell to be composed of CaCO3. Calcium carbonate is not only abundant material in the world but also thermodynamically stable mineral in the capture of CO2. Bivalve has produced CaCO3 under seawater condition, in other word, near atmospheric conditions (1 atm. and around 20-25 oC). At the inorganic point, the synthesis of CaCO3 is as followed. Ca2+ + CO32- -> CaCO3 The bivalve shell plays an important role to protect bivalve's internal organs from prodetor. What will be happened if the shell is damaged and a hole is made? Bivalve must cover the hole to prevent the oxidation of internal organs as fast as possible. From in vitro crystallization test of a notched shell, rapid CaCO3 production was identified at the damaged area. The biocatalyst related to shell regeneration was purified and named as SPSR (Soluble Protein related to Shell Regeneration) that is obtained from the oyster, Crassostrea gigas. And in vitro CaCO3 crystallization test was used to calculate the crystal growth rate of SPSR on CaCO3 crystallization. The characteristics of SPRR are discussed at the point of CO2 hydration and rapid CaCO3 synthesis. To develop the bioinspired process based on shell regeneration concept, the analysis of protein structure has been studied and the immobilization has been carried out for easy recovery of SPSR.

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.

Feasibility study of algae-based Carbon Dioxide capture ...

EPA Pesticide Factsheets

SUMMARY: 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 evaluate the benefits of using algae to reduce CO2 emissions from industrial and small-scale utility power boilers. The operations are being studied for the use of CO2 from flue gas for algae growth along with the production of biofuels and other useful products to prepare a comprehensive characterization of the economic feasibility of using algae to capture CO2. Information is being generated for analyses of the potential for these technologies to advance in the market and assist in meeting environmental goals, as well as to examine their associated environmental implications. Three electric power generation plants (coal and fuel oil fired) equipped to send flue-gas emissions to algae culture at demonstration facilities are being studied. Data and process information are being collected and developed to facilitate feasibility and modeling evaluations of the CO2 to algae technology. An understanding of process requirements to apply this technology to existing industries would go far in advancing carbon capture opportunities. Documenting the successful use of this technology could help bring “low-tech”, low-cost, CO2 to algae, carbon capture to multiple size industries and

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

Class and Home Problems: Carbon Dioxide Capture from Coal-Fired Power Plants Using Calcium Looping

ERIC Educational Resources Information Center

Deshpande, Niranjani; Phalak, Nihar; Fan, Liang-Shih; Sundaresan, Sankaran

2015-01-01

Calcium looping is based on the simple premise of the reversible reaction between CO[subscript 2] and CaO. This reaction can be used for separation of CO2 from a mixture of gases; most notably the technology finds applications in CO[subscript 2] removal from gas streams in fossil fuel-based energy systems. This article gives a brief overview of…

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...

A Comparative Study of the CO2 Absorption in Some Solvent-Free Alkanolamines and in Aqueous Monoethanolamine (MEA).

PubMed

Barzagli, Francesco; Mani, Fabrizio; Peruzzini, Maurizio

2016-07-05

The neat secondary amines 2-(methylamino)ethanol, 2-(ethylamino)ethanol, 2-(isopropylamino)ethanol, 2-(benzylamino)ethanol and 2-(butylamino)ethanol react with CO2 at 50-60 °C and room pressure yielding liquid carbonated species without their dilution with any additional solvent. These single-component absorbents have the theoretical CO2 capture capacity of 0.50 (mol CO2/mol amine) due to the formation of the corresponding amine carbamates and protonated amines that were identified by the (13)C NMR analysis. These single-component absorbents were used for CO2 capture (15% and 40% v/v in air) in two series of different procedures: (1) batch experiments aimed at investigating the efficiency and the rate of CO2 capture; (2) continuous cycles of absorption-desorption carried out in packed columns with absorption temperatures brought at 50-60 °C and desorption temperatures at 100-120 °C at room pressure. A number of different amines and experimental setups gave CO2 capture efficiency greater than 90%. For comparison purposes, 30 wt % aqueous MEA was used for CO2 capture under the same operational conditions described for the solvent-free amines. The potential advantages of solvent-free alkanolamines over aqueous MEA in the CO2 capture process were discussed.

Multiphase flow simulations of a moving fluidized bed regenerator in a carbon capture unit

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sarkar, Avik; Pan, Wenxiao; Suh, Dong-Myung

2014-10-01

To accelerate the commercialization and deployment of carbon capture technologies, computational fluid dynamics (CFD)-based tools may be used to model and analyze the performance of carbon capture devices. This work presents multiphase CFD-based flow simulations for the regeneration device responsible for extracting CO 2 from CO 2-loaded sorbent particles before the particles are recycled. The use of solid particle sorbents in this design is a departure from previously reported systems, where aqueous sorbents are employed. Another new feature is the inclusion of a series of perforated plates along the regenerator height. The influence of these plates on sorbent distribution ismore » examined for varying sorbent holdup, fluidizing gas velocity, and particle size. The residence time distribution of sorbents is also measured to classify the low regime as plug flow or well-mixed flow. The purpose of this work is to better understand the sorbent flow characteristics before reaction kinetics of CO 2 desorption can be implemented.« less

Highly Surface-Active Ca(OH)2 Monolayer as a CO2 Capture Material.

PubMed

Özçelik, V Ongun; Gong, Kai; White, Claire E

2018-03-14

Greenhouse gas emissions originating from fossil fuel combustion contribute significantly to global warming, and therefore the design of novel materials that efficiently capture CO 2 can play a crucial role in solving this challenge. Here, we show that reducing the dimensionality of bulk crystalline portlandite results in a stable monolayer material, named portlandene, that is highly effective at capturing CO 2 . On the basis of theoretical analysis comprised of ab initio quantum mechanical calculations and force-field molecular dynamics simulations, we show that this single-layer phase is robust and maintains its stability even at high temperatures. The chemical activity of portlandene is seen to further increase upon defect engineering of its surface using vacancy sites. Defect-containing portlandene is capable of separating CO and CO 2 from a syngas (CO/CO 2 /H 2 ) stream, yet is inert to water vapor. This selective behavior and the associated mechanisms have been elucidated by examining the electronic structure, local charge distribution, and bonding orbitals of portlandene. Additionally, unlike conventional CO 2 capturing technologies, the regeneration process of portlandene does not require high temperature heat treatment because it can release the captured CO 2 by application of a mild external electric field, making portlandene an ideal CO 2 capturing material for both pre- and postcombustion processes.

CaO-Based CO2 Sorbents Effectively Stabilized by Metal Oxides.

PubMed

Naeem, Muhammad Awais; Armutlulu, Andac; Imtiaz, Qasim; Müller, Christoph R

2017-11-17

Calcium looping (i.e., CO 2 capture by CaO) is a promising second-generation CO 2 capture technology. CaO, derived from naturally occurring limestone, offers an inexpensive solution, but due to the harsh operating conditions of the process, limestone-derived sorbents undergo a rapid capacity decay induced by the sintering of CaCO 3 . Here, we report a Pechini method to synthesize cyclically stable, CaO-based CO 2 sorbents with a high CO 2 uptake capacity. The sorbents synthesized feature compositional homogeneity in combination with a nanostructured and highly porous morphology. The presence of a single (Al 2 O 3 or Y 2 O 3 ) or bimetal oxide (Al 2 O 3 -Y 2 O 3 ) provides cyclic stability, except for MgO which undergoes a significant increase in its particle size with the cycle number. We also demonstrate a direct relationship between the CO 2 uptake and the morphology of the synthesized sorbents. After 30 cycles of calcination and carbonation, the best performing sorbent, containing an equimolar mixture of Al 2 O 3 and Y 2 O 3 , exhibits a CO 2 uptake capacity of 8.7 mmol CO 2  g -1 sorbent, which is approximately 360 % higher than that of the reference limestone. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Embedded enzymes catalyse capture

NASA Astrophysics Data System (ADS)

Kentish, Sandra

2018-05-01

Membrane technologies for carbon capture can offer economic and environmental advantages over conventional amine-based absorption, but can suffer from limited gas flux and selectivity to CO2. Now, a membrane based on enzymes embedded in hydrophilic pores is shown to exhibit combined flux and selectivity that challenges the state of the art.

Development of carbon dioxide adsorbent from rice husk char

NASA Astrophysics Data System (ADS)

Abang, S.; Janaun, J.; Anisuzzaman, S. M.; Ikhwan, F. S.

2016-06-01

This study was mainly concerned about the development of carbon dioxide (CO2) adsorbent from rice husk (RH). Several chemical treatments were used to produce activated rice husk char (RHAC) from RH. Initially the RH was refluxed with 3M of sodium hydroxide (NaOH) solution, activation followed by using 0.5M of zinc chloride (ZnCl2) solution and finally acidic treatment by using 0.1M of hydrochloric acid (HCl). Then, the RHAC was functionalized by using 3-chloropropylamine hydrochloride (3-CPA) and noted as RHN. RHN samples were characterized with scanning electron microscopy (SEM), mercury intrusion porosimetry (MIP), fourier transform infrared spectroscopy (FTIR). Based on the SEM, the RHN sample had a large pore diameter compared to RH sample after being treated. Based on MIP data, the average pore diameter between RH and RHAC samples were increased significantly from 0.928 microns to 1.017 microns. The RHN sample also had higher total porosity (%) compared to RHAC and RH (58.45%, 47.82% and 45.57% respectively). The total specific surface area of the sample was much increasing from RHO to RHAC (29.17 m2/g and 62.94 m2/g respectively) and slightly being decreasing from RHAC to RHN (58.88 m2/g). FTIR result showed the present of weak band at 1587 cm-1 which demonstrating of the amine group present on the sample. The CO2 capture result showed that the decreasing of operating temperature can increase the breakthrough time of CO2 capture. On the contrary decreasing of CO2 gas flow rate can increase the breakthrough time of CO2 capture. The highest total amount of CO2 adsorbed was 25338.57 mg of CO2/g of RHN sample by using 100 mL/min of gas flow rate at 30oC. Based on adsorption isotherm analysis, the Freundlich isotherm was the best isotherm to describe the CO2 adsorption on the sample.

Development Trends in Porous Adsorbents for Carbon Capture.

PubMed

Sreenivasulu, Bolisetty; Sreedhar, Inkollu; Suresh, Pathi; Raghavan, Kondapuram Vijaya

2015-11-03

Accumulation of greenhouse gases especially CO2 in the atmosphere leading to global warming with undesirable climate changes has been a serious global concern. Major power generation in the world is from coal based power plants. Carbon capture through pre- and post- combustion technologies with various technical options like adsorption, absorption, membrane separations, and chemical looping combustion with and without oxygen uncoupling have received considerable attention of researchers, environmentalists and the stake holders. Carbon capture from flue gases can be achieved with micro and meso porous adsorbents. This review covers carbonaceous (organic and metal organic frameworks) and noncarbonaceous (inorganic) porous adsorbents for CO2 adsorption at different process conditions and pore sizes. Focus is also given to noncarbonaceous micro and meso porous adsorbents in chemical looping combustion involving insitu CO2 capture at high temperature (>400 °C). Adsorption mechanisms, material characteristics, and synthesis methods are discussed. Attention is given to isosteric heats and characterization techniques. The options to enhance the techno-economic viability of carbon capture techniques by integrating with CO2 utilization to produce industrially important chemicals like ammonia and urea are analyzed. From the reader's perspective, for different classes of materials, each section has been summarized in the form of tables or figures to get a quick glance of the developments.

Real-time monitoring of emissions from monoethanolamine-based industrial scale carbon capture facilities.

PubMed

Zhu, Liang; Schade, Gunnar Wolfgang; Nielsen, Claus Jørgen

2013-12-17

We demonstrate the capabilities and properties of using Proton Transfer Reaction time-of-flight mass spectrometry (PTR-ToF-MS) to real-time monitor gaseous emissions from industrial scale amine-based carbon capture processes. The benchmark monoethanolamine (MEA) was used as an example of amines needing to be monitored from carbon capture facilities, and to describe how the measurements may be influenced by potentially interfering species in CO2 absorber stack discharges. On the basis of known or expected emission compositions, we investigated the PTR-ToF-MS MEA response as a function of sample flow humidity, ammonia, and CO2 abundances, and show that all can exhibit interferences, thus making accurate amine measurements difficult. This warrants a proper sample pretreatment, and we show an example using a dilution with bottled zero air of 1:20 to 1:10 to monitor stack gas concentrations at the CO2 Technology Center Mongstad (TCM), Norway. Observed emissions included many expected chemical species, dominantly ammonia and acetaldehyde, but also two new species previously not reported but emitted in significant quantities. With respect to concerns regarding amine emissions, we show that accurate amine quantifications in the presence of water vapor, ammonia, and CO2 become feasible after proper sample dilution, thus making PTR-ToF-MS a viable technique to monitor future carbon capture facility emissions, without conventional laborious sample pretreatment.

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

PubMed

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

2015-11-01

Amines have been considered as promising candidates for post-combustion CO2 capture. A mechanistic understanding for the chemical processes involved in the capture and release of CO2 is important for the rational design of amines. In this study, the structural effects of amines on the kinetic competition among three typical products (carbamates, carbamic acids and bicarbonate) from amines+CO2 were investigated, in contrast to previous thermodynamic studies to tune the reaction of amines with CO2 based on desirable reaction enthalpy and reaction stoichiometry. We used a quantum chemical method to calculate the activation energies (Ea) for the reactions of a range of substituted monoethanolamines with CO2 covering three pathways to the three products. The results indicate that the formation of carbamates is the most favorable, among the three considered products. In addition, we found that the Ea values for all pathways linearly correlate with pKa of amines, and more importantly, the kinetic competition between carbamate and bicarbonate absorption pathways varies with pKa of the amines, i.e. stronger basicity results in less difference in Ea. These results highlight the importance of the consideration of kinetic competition among different reaction pathways in amine design. Copyright © 2015. Published by Elsevier B.V.

Low-Energy Solvents For Carbon Dioxide Capture Enabled By A Combination Of Enzymes And Vacuum Regeneration

DOE Office of Scientific and Technical Information (OSTI.GOV)

Salmon, Sonja; House, Alan; Liu, Kun

An integrated bench-scale system combining the attributes of the bio-renewable enzyme carbonic anhydrase (CA) with low-enthalpy CO2 absorption solvents and vacuum regeneration was designed, built and operated for 500 hours using simulated flue gas. The objective was to develop a CO2 capture process with improved efficiency and sustainability when compared to NETL Case 10 monoethanolamine (MEA) scrubbing technology. The use of CA accelerates inter-conversion between dissolved CO2 and bicarbonate ion to enhance CO2 absorption, and the use of low enthalpy CO2 absorption solvents makes it possible to regenerate the solvent at lower temperatures relative to the reference MEA-based solvent. Themore » vacuum regeneration-based integrated bench-scale system operated successfully for an accumulated 500 hours using aqueous 23.5 wt% K2CO3-based solvent containing 2.5 g/L enzyme to deliver an average 84% CO2 capture when operated with a 20% enzyme replenishment rate per ~7 hour steady-state run period. The total inlet gas flow was 30 standard liters per minute with 15% CO2 and 85% N2. The absorber temperature was 40°C and the stripper operated under 35 kPa pressure with an approximate 77°C stripper bottom temperature. Tests with a 30°C absorber temperature delivered >90% capture. On- and off-line operational measurements provided a full process data set, with recirculating enzyme, that allowed for enzyme replenishment and absorption/desorption kinetic parameter calculations. Dissolved enzyme replenishment and conventional process controls were demonstrated as straightforward approaches to maintain system performance. Preliminary evaluation of a novel flow-through ultrasonically enhanced regeneration system was also conducted, yet resulted in CO2 release within the range of temperature-dependent release, and further work would be needed to validate the benefits of ultrasonic enhanced stripping. A full technology assessment was completed in which four techno-economic cases for enzyme-enhanced aqueous K2CO3 solvent with vacuum stripping were considered and a corresponding set of sensitivity studies were developed. The cases were evaluated using bench-scale and laboratory-based observations, AspenPlus® process simulation and modeling, AspenTech’s CCE® Parametric Software, current vendor quotations, and project partners’ know-how of unit operations. Overall, the DOE target of 90% CO2 capture could be met using the benign enzyme-enhanced aqueous K2CO3-based alternative to NETL Case 10. The model-predicted plant COE performance, scaled to 550 MWe net output, was 9% higher than NETL Case 10 for an enzyme-activated case with minimized technical risk and highest confidence in physical system performance utilizing commercially available equipment. A COE improvement of 2.8% versus NETL Case 10 was predicted when favorable features of improved enzyme longevity and additional power output from a very low pressure (VLP) turbine were combined, wherein corresponding high capital and operational costs limited the level of COE benefit. The environmental, health and safety (EH&S) profile of the system was found to be favorable and was compliant with the Federal EH&S legislation reviewed. Further work on a larger scale test unit is recommended to reduce the level of uncertainty inherent in extrapolating findings from a bench-scale unit to a full scale PCC plant, and to further investigate several identified opportunities for improvement. Production feasibility and suitability of carbonic anhydrases for scale-up testing was confirmed both through the current project and through parallel efforts.« less

Jumpstarting commercial-scale CO 2 capture and storage with ethylene production and enhanced oil recovery in the US Gulf

DOE PAGES

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

2015-04-27

CO 2 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 CO 2 capture from coal-fired power plants. Here, we propose that near-term investment could focus on implementing CO 2 capture on facilities that produce high-value chemicals/products. These facilities can absorb the expected impact of the marginal increase in the costmore » of production on the price of their product, due to the addition of CO 2 capture, more than coal-fired power plants. A financially viable demonstration of a large-scale CCUS network requires offsetting the costs of CO 2 capture by using the CO 2 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 CO 2 is captured from ethylene producers and used for enhanced oil recovery in the U.S. Gulf Coast region.« less

Light-Triggered CO2 Breathing Foam via Nonsurfactant High Internal Phase Emulsion.

PubMed

Zhang, Shiming; Wang, Dingguan; Pan, Qianhao; Gui, Qinyuan; Liao, Shenglong; Wang, Yapei

2017-10-04

Solid materials for CO 2 capture and storage have attracted enormous attention for gaseous separation, environmental protection, and climate governance. However, their preparation and recovery meet the problems of high energy and financial cost. Herein, a controllable CO 2 capture and storage process is accomplished in an emulsion-templated polymer foam, in which CO 2 is breathed-in under dark and breathed-out under light illumination. Such a process is likely to become a relay of natural CO 2 capture by plants that on the contrary breathe out CO 2 at night. Recyclable CO 2 capture at room temperature and release under light irradiation guarantee its convenient and cost-effective regeneration in industry. Furthermore, CO 2 mixed with CH 4 is successfully separated through this reversible breathing in and out system, which offers great promise for CO 2 enrichment and practical methane purification.

Membrane-based systems for carbon capture and hydrogen purification

DOE Office of Scientific and Technical Information (OSTI.GOV)

Berchtold, Kathryn A

2010-11-24

This presentation describes the activities being conducted at Los Alamos National Laboratory to develop carbon capture technologies for power systems. This work is aimed at continued development and demonstration of a membrane based pre- and post-combustion carbon capture technology and separation schemes. Our primary work entails the development and demonstration of an innovative membrane technology for pre-combustion capture of carbon dioxide that operates over a broad range of conditions relevant to the power industry while meeting the US DOE's Carbon Sequestration Program goals of 90% CO{sub 2} capture at less than a 10% increase in the cost of energy services.more » Separating and capturing carbon dioxide from mixed gas streams is a first and critical step in carbon sequestration. To be technically and economically viable, a successful separation method must be applicable to industrially relevant gas streams at realistic temperatures and pressures as well as be compatible with large gas volumes. Our project team is developing polymer membranes based on polybenzimidazole (PBI) chemistries that can purify hydrogen and capture CO{sub 2} at industrially relevant temperatures. Our primary objectives are to develop and demonstrate polymer-based membrane chemistries, structures, deployment platforms, and sealing technologies that achieve the critical combination of high selectivity, high permeability, chemical stability, and mechanical stability all at elevated temperatures (> 150 C) and packaged in a scalable, economically viable, high area density system amenable to incorporation into an advanced Integrated Gasification Combined-Cycle (IGCC) plant for pre-combustion CO{sub 2} capture. Stability requirements are focused on tolerance to the primary synthesis gas components and impurities at various locations in the IGCC process. Since the process stream compositions and conditions (temperature and pressure) vary throughout the IGCC process, the project is focused on the optimization of a technology that could be positioned upstream or downstream of one or more of the water-gas-shift reactors (WGSRs) or integrated with a WGSR.« less

Framing and bias in CO2 capture and storage communication films: Reflections from a CO2 capture and storage research group.

PubMed

Maynard, Carly M; Shackley, Simon

2017-03-01

There has been a growing trend towards incorporating short, educational films as part of research funding and project proposals. Researchers and developers in CO 2 capture and storage are using films to communicate outcomes, but such films can be influenced by experiences and values of the producers. We document the content and presentation of seven online CO 2 capture and storage films to determine how framing occurs and its influence on the tone of films. The core frame presents CO 2 capture and storage as a potential solution to an imminent crisis in climatic warming and lack of a sustainable energy supply. Three subsidiary frames represent CO 2 capture and storage as (1) the only option, (2) a partial option or (3) a scientific curiosity. The results demonstrate that an understanding of the nuanced explicit and implicit messages portrayed by films is essential both for effective framing according to one's intention and for wider public understanding of a field.

MEMBRANE PROCESS TO SEQUESTER CO2 FROM POWER PLANT FLUE GAS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tim Merkel; Karl Amo; Richard Baker

2009-03-31

The objective of this project was to assess the feasibility of using a membrane process to capture CO2 from coal-fired power plant flue gas. During this program, MTR developed a novel membrane (Polaris™) with a CO2 permeance tenfold higher than commercial CO2-selective membranes used in natural gas treatment. The Polaris™ membrane, combined with a process design that uses a portion of combustion air as a sweep stream to generate driving force for CO2 permeation, meets DOE post-combustion CO2 capture targets. Initial studies indicate a CO2 separation and liquefaction cost of $20 - $30/ton CO2 using about 15% of the plantmore » energy at 90% CO2 capture from a coal-fired power plant. Production of the Polaris™ CO2 capture membrane was scaled up with MTR’s commercial casting and coating equipment. Parametric tests of cross-flow and countercurrent/sweep modules prepared from this membrane confirm their near-ideal performance under expected flue gas operating conditions. Commercial-scale, 8-inch diameter modules also show stable performance in field tests treating raw natural gas. These findings suggest that membranes are a viable option for flue gas CO2 capture. The next step will be to conduct a field demonstration treating a realworld power plant flue gas stream. The first such MTR field test will capture 1 ton CO2/day at Arizona Public Service’s Cholla coal-fired power plant, as part of a new DOE NETL funded program.« less

A Reversed Photosynthesis-like Process for Light-Triggered CO2 Capture, Release, and Conversion.

PubMed

Wang, Dingguan; Liao, Shenglong; Zhang, Shiming; Wang, Yapei

2017-06-22

Materials for CO 2 capture have been extensively exploited for climate governance and gas separation. However, their regeneration is facing the problems of high energy cost and secondary CO 2 contamination. Herein, a reversed photosynthesis-like process is proposed, in which CO 2 is absorbed in darkness while being released under light illumination. The process is likely supplementary to natural photosynthesis of plants, in which, on the contrary, CO 2 is released during the night. Remarkably, the material used here is able to capture 9.6 wt.% CO 2 according to its active component. Repeatable CO 2 capture at room temperature and release under light irradiation ensures its convenient and cost-effective regeneration. Furthermore, CO 2 released from the system is successfully converted into a stable compound in tandem with specific catalysts. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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.

Anion-Functionalized Task-Specific Ionic Liquids: Molecular Origin of Change in Viscosity upon CO2 Capture.

PubMed

Li, Ailin; Tian, Ziqi; Yan, Tianying; Jiang, De-en; Dai, Sheng

2014-12-26

The structure and dynamics of a task-specific ionic liquid (TSIL), trihexyl(tetradecyl)phosphonium imidazolate, before and after absorbing CO(2) were studied with a molecular dynamics (MD) simulation. This particular ionic liquid is one of several newly discovered azole-based TSILs for equimolar CO(2) capture. Unlike other TSILs whose viscosity increases drastically upon reaction with CO(2), its viscosity decreases after CO(2) absorption. This unique behavior was confirmed in our MD simulation. We find that after CO(2) absorption the translational dynamics of the whole system is accelerated, accompanied by an accelerated rotational dynamics of the cations. Radial distribution function and spatial distribution function analyses show that the anions become asymmetric after reaction with CO(2), and this causes the imbalance of the interaction between the positive and negative regions of the ions. The interaction between the phosphorus atom of the cation and oxygen atoms of the carboxyl group on the anion is enhanced, while that between the phosphorus atom and the naked nitrogen atom of the anion is weakened. The ion-pair correlation functions further support that the weakened interaction leads to faster dissociation of cation-anion pairs, thereby causing an accelerated dynamics. Hence, the asymmetry of anions influences the dynamics of the system and affects the viscosity. This insight may help design better TSILs with decreased viscosity for CO(2) capture.

Structures for capturing CO.sub.2, methods of making the structures, and methods of capturing CO.sub.2

DOEpatents

Jones, Christopher W; Hicks, Jason C; Fauth, Daniel J; McMahan, Gray

2012-10-30

Briefly described, embodiments of this disclosure, among others, include carbon dioxide (CO.sub.2) sorption structures, methods of making CO.sub.2 sorption structures, and methods of using CO.sub.2 sorption structures.

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.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Basha, Omar M.; Keller, Murphy J.; Luebke, David R.

The Ionic Liquid (IL) [hmim][Tf 2N] was used as a physical solvent in an Aspen Plus simulation, employing the Peng-Robinson Equation of State (P-R EOS) with Boston-Mathias (BM) alpha function and standard mixing rules, to develop a conceptual process for CO 2 capture from a shifted warm fuel gas stream produced from Pittsburgh # 8 coal for a 400 MWe power plant. The physical properties of the IL, including density, viscosity, surface tension, vapor pressure and heat capacity were obtained from literature and modeled as a function of temperature. Also, available experimental solubility values for CO 2, H 2, Hmore » 2S, CO, and CH 4 in this IL were compiled and their binary interaction parameters (Δ ij and l ij) were optimized and correlated as functions of temperature. The Span-Wager Equation-of-State EOS was also employed to generate CO 2 solubilities in [hmim][Tf 2N] at high pressures (up to 10 MPa) and temperatures (up to 510 K). The conceptual process developed consisted of 4 adiabatic absorbers (2.4 m ID, 30 m high) arranged in parallel and packed with Plastic Pall Rings of 0.025 m for CO 2 capture; 3 flash drums arranged in series for solvent (IL) regeneration with the pressure-swing option; and a pressure-intercooling system for separating and pumping CO 2 up to 153 bar to the sequestration sites. The compositions of all process streams, CO 2 capture efficiency, and net power were calculated using Aspen Plus simulator. The results showed that, based on the composition of the inlet gas stream to the absorbers, 95.67 mol% of CO 2 was captured and sent to sequestration sites; 99.5 mol% of H 2 was separated and sent to turbines; the solvent exhibited a minimum loss of 0.31 mol%; and the net power balance of the entire system was 30.81 MW. These results indicated that [hmim][Tf 2N] IL could be used as a physical solvent for CO 2 capture from warm shifted fuel gas streams with high efficiency.« less

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

PubMed

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

2015-07-07

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

Imidazolium salt-modified porous hypercrosslinked polymers for synergistic CO2 capture and conversion.

PubMed

Wang, Jinquan; Sng, Waihong; Yi, Guangshun; Zhang, Yugen

2015-08-04

A new type of imidazolium salt-modified porous hypercrosslinked polymer (BET surface area up to 926 m(2) g(-1)) was reported. These porous materials exhibited good CO2 capture capacities (14.5 wt%) and catalytic activities for the conversion of CO2 into various cyclic carbonates under metal-free conditions. The synergistic effect of CO2 capture and conversion was observed.

Evaluation of Solid Sorbents As A Retrofit Technology for CO{sub 2} Capture from Coal-Fired Power Plants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krutka, Holly; Sjostrom, Sharon

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 kWemore » 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), 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 field sites. ADA designed and fabricated a slipstream pilot to allow an evaluation of the kinetic behavior of sorbents and provide some flexibility for the physical characteristics of the materials. The design incorporated a transport reactor for the adsorber (co-current reactor) and a fluidized-bed in the regenerator. This combination achieved the sorbent characterization goals and provided an opportunity to evaluate whether the potential cost savings associated with a relatively simple process design could overcome the sacrifices inherent in a co-current separation process. The system was installed at two field sites during the project, Luminant’s Martin Lake Steam Electric Station and Xcel Energy’s Sherburne County Generating Station (Sherco). Although the system could not maintain continuous 90% CO{sub 2} removal with the sorbents evaluated under this program, it was useful to compare the CO{sub 2} removal properties of several different sorbents on actual flue gas. One of the supported amine materials, sorbent R, was evaluated at both Martin Lake and Sherco. The 1 kWe pilot was operated in continuous mode as well as batch mode. In continuous mode, the sorbent performance could not overcome the limitations of the co-current adsorbent design. In batch mode, sorbent R was able to remove up to 90% CO{sub 2} for several cycles. Approximately 50% of the total removal occurred in the first three feet of the adsorption reactor, which was a transport reactor. During continuous testing at Sherco, CO{sub 2} removal decreased to approximately 20% at steady state. The lack of continuous removal was due primarily to the combination of a co-current adsorption system with a fluidized bed for regeneration, a combination which did not provide an adequate driving force to maintain an acceptable working CO{sub 2} capacity. In addition, because sorbent R consisted of a polymeric amine coated on a silica substrate, it was believed that the 50% amine loaded resulted in mass diffusion limitations related to the CO{sub 2} uptake rate. Three additional supported amine materials, sorbents AX, F, and BN, were selected for evaluation using the 1 kW pilot at Sherco. Sorbent AX was operated in batch mode and performed similarly to sorbent R (i.e. could achieve up to 90% removal when given adequate regeneration time). Sorbent BN was not expected to be subject to the same mass diffusion limitations as experienced with sorbent R. When sorbent BN was used in continuous mode the steady state CO{sub 2} removal was approximately double that of sorbent R, which highlighted the importance of sorbents without kinetic limitations. Many different processes and equipment designs exist that may be applicable for postcombustion CO{sub 2} capture using solids in a temperature-swing system. A thorough technology survey was completed to identify the most promising options, which were grouped and evaluated based on the four main unit operations involved with sorbent based capture: Adsorption; Heating and cooling, or heat transfer; Conveying; Desorption. The review included collecting information from a wide variety of sources, including technology databases, published papers, advertisements, web searches, and vendor interviews. Working with power producers, scoring sheets were prepared and used to compare the different technology options. Although several technologies were interesting and promising, those that were selected for the final conceptual design were commercially available and performed multiple steps simultaneously. For the adsorption step, adsorption and conveying were both accomplished in a circulating fluidized bed. A rotary kiln was selected for desorption and cooling because it can simultaneously accomplish conveying and effective heat transfer. The final technology selection was used to complete preliminary costs assessments for a conceptual 500 MW CO{sub 2} capture process. The high level cost analysis was completed to determine the key cost drivers. The conceptual sorbent-based capture options yielded significant energy penalty and cost savings versus an aqueous amine system. Specifically, the estimated levelized cost of electricity (LCOE) for final concept design without a CO{sub 2} laden/lean sorbent heat exchanger or any other integration, was over 30% lower than that of the MEA capture process. However, this cost savings was not enough to meet the DOE’s target of ≤35% increase in LCOE. In order to reach this target, the incremental LCOE due to the CO{sub 2} capture can be no higher than 2.10 ¢/kWh above the LCOE of the non-capture equivalent power plant (6.0 ¢/kWh). Although results of the 1 kWe pilot evaluations suggest that the initial full-scale concept design must be revisited to address the technical targets, the cost assessment still provides a valuable high-level estimate of the potential costs of a solids-based system. A sensitivity analysis was conducted to determine the cost drivers and the results of the sensitivity analysis will be used to direct future technology development efforts. The overall project objective was to assess the viability and accelerate development of a solid-based post-combustion CO{sub 2} capture technology that can be retrofit to the existing fleet of coal-fired power plants. This objective was successfully completed during the project along with several specific budget period goals. Based on sorbent screening and a full-scale equipment evaluation, it was determined that solid sorbents for post-combustion capture is promising and warrants continued development efforts. Specifically, the lower sensible heat could result in a significant reduction in the energy penalty versus solvent based capture systems, if the sorbents can be paired with a process and equipment that takes advantage of the beneficial sorbent properties. It was also determined that a design using a circulating fluidized bed adsorber with rotary kilns for heating during regeneration, cooling, and conveying highlighted the advantage of sorbents versus solvents. However, additional technology development and cost reductions will be required to meet the DOE’s final technology goal of 90% CO{sub 2} capture with ≤35% increase in the cost of electricity. The cost analysis identified specific targets for the capital and operating costs, which will be used as the targets for future technology development efforts.« less

CFD Simulations of a Regenerative Process for Carbon Dioxide Capture in Advanced Gasification Based Power Systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arastoopour, Hamid; Abbasian, Javad

2014-07-31

This project describes the work carried out to prepare a highly reactive and mechanically strong MgO based sorbents and to develop a Population Balance Equations (PBE) approach to describe the evolution of the particle porosity distribution that is linked with Computational Fluid Dynamics (CFD) to perform simulations of the CO2 capture and sorbent regeneration. A large number of MgO-based regenerable sorbents were prepared using low cost and abundant dolomite as the base material. Among various preparation parameters investigated the potassium/magnesium (K/Mg) ratio was identified as the key variable affecting the reactivity and CO2 capacity of the sorbent. The optimum K/Mgmore » ratio is about 0.15. The sorbent formulation HD52-P2 was identified as the “best” sorbent formulation and a large batch (one kg) of the sorbent was prepared for the detailed study. The results of parametric study indicate the optimum carbonation and regeneration temperatures are 360° and 500°C, respectively. The results also indicate that steam has a beneficial effect on the rate of carbonation and regeneration of the sorbent and that the reactivity and capacity of the sorbent decreases in the cycling process (sorbent deactivation). The results indicate that to achieve a high CO2 removal efficiency, the bed of sorbent should be operated at a temperature range of 370-410°C which also favors production of hydrogen through the WGS reaction. To describe the carbonation reaction kinetics of the MgO, the Variable Diffusivity shrinking core Model (VDM) was developed in this project, which was shown to accurately fit the experimental data. An important advantage of this model is that the changes in the sorbent conversion with time can be expressed in an explicit manner, which will significantly reduce the CFD computation time. A Computational Fluid Dynamic/Population Balance Equations (CFD/PBE) model was developed that accounts for the particle (sorbent) porosity distribution and a new version of the method of moments, called Finite size domain Complete set of trial functions Method Of Moments (FCMOM) was used to solve the population balance equations. The PBE model was implemented in a commercial CFD code, Ansys Fluent 13.0. The code was used to test the model in some simple cases and the results were verified against available analytical solution in the literature. Furthermore, the code was used to simulate CO2 capture in a packed-bed and the results were in excellent agreement with the experimental data obtained in the packed bed. The National Energy Laboratory (NETL) Carbon Capture Unit (C2U) design was used in simulate of the hydrodynamics of the cold flow gas/solid system (Clark et al.58). The results indicate that the pressure drop predicted by the model is in good agreement with the experimental data. Furthermore, the model was shown to be able to predict chugging behavior, which was observed during the experiment. The model was used as a base-case for simulations of reactive flow at elevated pressure and temperatures. The results indicate that by controlling the solid circulation rate, up to 70% CO2 removal can be achieved and that the solid hold up in the riser is one of the main factors controlling the extent of CO2 removal. The CFD/PBE simulation model indicates that by using a simulated syngas with a composition of 20% CO2, 20% H2O, 30% CO, and 30% H2, the composition (wet basis) in the reactor outlet corresponded to about 60% CO2 capture with and exit gas containing 65% H2. A preliminary base-case-design was developed for a regenerative MgO-based pre-combustion carbon capture process for a 500 MW IGCC power plant. To minimize the external energy requirement, an extensive heat integration network was developed in Aspen/HYSYS® to produce the steam required in the regenerator and heat integration. In this process, liquid CO2 produced at 50 atm can easily be pumped and sequestered or stored. The preliminary economic analyses indicate that the estimated cost of carbon v capture is in the range of $31-$44/ton, suggesting that a regenerative MgO-Based process can be a viable option for pre-combustion carbon dioxide capture in advanced gasification based power systems.« less

Cyclic carbonation calcination studies of limestone and dolomite for CO{sub 2} separation from combustion flue gases - article no. 011801

DOE Office of Scientific and Technical Information (OSTI.GOV)

Senthoorselvan, S.; Gleis, S.; Hartmut, S.

2009-01-15

Naturally occurring limestone and dolomite samples, originating from different geographical locations, were tested as potential sorbents for carbonation/calcination based CO{sub 2} capture from combustion flue gases. Samples have been studied in a thermogravimetric analyzer under simulated flue gas conditions at three calcination temperatures, viz., 750{sup o}C, 875{sup o}C, and 930{sup o}C for four carbonation calcination reaction (CCR) cycles. The dolomite sample exhibited the highest rate of carbonation than the tested limestones. At the third cycle, its CO{sub 2} capture capacity per kilogram of the sample was nearly equal to that of Gotland, the highest reacting limestone tested. At the fourthmore » cycle it surpassed Gotland, despite the fact that the CaCO{sub 3} content of the Sibbo dolomite was only 2/3 of that of the Gotland. Decay coefficients were calculated by a curve fitting exercise and its value is lowest for the Sibbo dolomite. That means, most probably its capture capacity per kilogram of the sample would remain higher well beyond the fourth cycle. There was a strong correlation between the calcination temperature, the specific surface area of the calcined samples, and the degree of carbonation. It was observed that the higher the calcination temperature, the lower the sorbent reactivity. For a given limestone/dolomite sample, sorbents CO{sub 2} capture capacity depended on the number of CCR cycles and the calcination temperature. According to the equilibrium thermodynamics, the CO{sub 2} partial pressure in the calciner should be lowered to lower the calcination temperature. This can be achieved by additional steam supply into the calciner. Steam could then be condensed in an external condenser to single out the CO{sub 2} stream from the exit gas mixture of the calciner. A calciner design based on this concept is illustrated.« less

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. Copyright © 2016 Elsevier Ltd. All rights reserved.

Rapid Design and Testing of Novel Gas/liquid Contacting Devices for Post-Combustion CO 2 Capture via 3D Printing - Phase II Final Technical Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Panaccione, Charles; Staab, Greg; Meuleman, Erik

ION has developed a mathematically driven model for a contacting device incorporating mass transfer, heat transfer, and computational fluid dynamics. This model is based upon a parametric structure for purposes of future commercialization. The most promising design from modeling was 3D printed and tested in a bench scale CO 2 capture unit and compared to commercially available structured packing tested in the same unit.

Capture-ready power plants - options, technologies and economics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bohm, M.C.

2006-06-15

A plant can be considered to be capture-ready if at some point in the future it can be retrofitted for carbon capture and sequestration and still be economical to operate. The first part of the thesis outlines the two major designs that are being considered for construction in the near-term - pulverized coal (PC) and integrated gasification/combined cycle (IGCC). It details the steps that are necessary to retrofit each of these plants for CO{sub 2} capture and sequestration and assesses the steps that can be taken to reduce the costs and output de-rating of the plant after a retrofit. The second part of the thesis evaluates the lifetime (40 year) net present value (NPV) costs of plants with differing levels of pre-investment for CO{sub 2} capture. Three scenarios are evaluated - a baseline supercritical PC plant, a baseline IGCC plant and an IGCC plant with pre-investment for capture. The results of this thesis show that a baseline PC plant is the most economical choice under low CO{sub 2} tax rates, and IGCC plants are preferable at higher tax rates. The third part of this thesis evaluates the concept of CO{sub 2} 'lock-in'. CO{sub 2} lock-in occurs when a newly built plant is so prohibitively expensive to retrofit for CO{sub 2} capture that it will never be retrofitted for capture, and offers no economic opportunity to reduce the CO{sub 2} emissions from the plant, besides shutting down or rebuilding. The results show that IGCC plants are expected to have lower lifetime CO{sub 2} emissions than a PC plant, given moderate (10-35more » $$/ton CO{sub 2}) initial tax rates. Higher 4 (above $$40) or lower (below $7) initial tax rates do not result in significant differences in lifetime CO{sub 2} emissions from these plants. Little difference is seen in the lifetime CO{sub 2} emissions between the IGCC plants with and without pre-investment for CO{sub 2} capture. 32 refs., 22 figs., 20 tabs., 1 app.« less

A process for capturing CO 2 from the atmosphere

DOE PAGES

Keith, David W.; Holmes, Geoffrey; St. Angelo, David; ...

2018-06-07

Here, we describe a process for capturing CO 2 from the atmosphere in an industrial plant. The design captures ~1 Mt-CO 2/year in a continuous process using an aqueous KOH sorbent coupled to a calcium caustic recovery loop. We describe the design rationale, summarize performance of the major unit operations, and provide a capital cost breakdown developed with an independent consulting engineering firm. We report results from a pilot plant which provides data on performance of the major unit operations. We summarize the energy and material balance computed using an Aspen process simulation. When CO 2 is delivered at 15more » MPa the design requires either 8.81 GJ of natural gas, or 5.25 GJ of gas and 366 kWhr of electricity, per ton of CO 2 captured. Depending on financial assumptions, energy costs, and the specific choice of inputs and outputs, the levelized cost per ton CO 2 captured from the atmosphere ranges from 94 to 232 $/t-CO 2.« less

A process for capturing CO 2 from the atmosphere

DOE Office of Scientific and Technical Information (OSTI.GOV)

Keith, David W.; Holmes, Geoffrey; St. Angelo, David

Here, we describe a process for capturing CO 2 from the atmosphere in an industrial plant. The design captures ~1 Mt-CO 2/year in a continuous process using an aqueous KOH sorbent coupled to a calcium caustic recovery loop. We describe the design rationale, summarize performance of the major unit operations, and provide a capital cost breakdown developed with an independent consulting engineering firm. We report results from a pilot plant which provides data on performance of the major unit operations. We summarize the energy and material balance computed using an Aspen process simulation. When CO 2 is delivered at 15more » MPa the design requires either 8.81 GJ of natural gas, or 5.25 GJ of gas and 366 kWhr of electricity, per ton of CO 2 captured. Depending on financial assumptions, energy costs, and the specific choice of inputs and outputs, the levelized cost per ton CO 2 captured from the atmosphere ranges from 94 to 232 $/t-CO 2.« less

Lake Charles CCS Project

DOE Office of Scientific and Technical Information (OSTI.GOV)

Leib, Thomas; Cole, Dan

In late September 2014 development of the Lake Charles Clean Energy (LCCE) Plant was abandoned resulting in termination of Lake Charles Carbon Capture and Sequestration (CCS) Project which was a subset the LCCE Plant. As a result, the project was only funded through Phase 2A (Design) and did not enter Phase 2B (Construction) or Phase 2C (Operations). This report was prepared relying on information prepared and provided by engineering companies which were engaged by Leucadia Energy, LLC to prepare or review Front End Engineering and Design (FEED) for the Lake Charles Clean Energy Project, which includes the Carbon Capture andmore » Sequestration (CCS) Project in Lake Charles, Louisiana. The Lake Charles Carbon Capture and Sequestration (CCS) Project was to be a large-scale industrial CCS project intended to demonstrate advanced technologies that capture and sequester carbon dioxide (CO 2) emissions from industrial sources into underground formations. The Scope of work was divided into two discrete sections; 1) Capture and Compression prepared by the Recipient Leucadia Energy, LLC, and 2) Transport and Sequestration prepared by sub-Recipient Denbury Onshore, LLC. Capture and Compression-The Lake Charles CCS Project Final Technical Report describes the systems and equipment that would be necessary to capture CO 2 generated in a large industrial gasification process and sequester the CO 2 into underground formations. The purpose of each system is defined along with a description of its equipment and operation. Criteria for selection of major equipment are provided and ancillary utilities necessary for safe and reliable operation in compliance with environmental regulations are described. Construction considerations are described including a general arrangement of the CCS process units within the overall gasification project. A cost estimate is provided, delineated by system area with cost breakdown showing equipment, piping and materials, construction labor, engineering, and other costs. The CCS Project Final Technical Report is based on a Front End Engineering and Design (FEED) study prepared by SK E&C, completed in [June] 2014. Subsequently, Fluor Enterprises completed a FEED validation study in mid-September 2014. The design analyses indicated that the FEED package was sufficient and as expected. However, Fluor considered the construction risk based on a stick-build approach to be unacceptable, but construction risk would be substantially mitigated through utilization of modular construction where site labor and schedule uncertainty is minimized. Fluor’s estimate of the overall EPC project cost utilizing the revised construction plan was comparable to SKE&C’s value after reflecting Fluor’s assessment of project scope and risk characteristic. Development was halted upon conclusion of Phase 2A FEED and the project was not constructed.Transport and Sequestration – The overall objective of the pipeline project was to construct a pipeline to transport captured CO 2 from the Lake Charles Clean Energy project to the existing Denbury Green Line and then to the Hastings Field in Southeast Texas to demonstrate effective geologic sequestration of captured CO 2 through commercial EOR operations. The overall objective of the MVA portion of the project was to demonstrate effective geologic sequestration of captured CO 2 through commercial Enhanced Oil Recovery (EOR) operations in order to evaluate costs, operational processes and technical performance. The DOE target for the project was to capture and implement a research MVA program to demonstrate the sequestration through EOR of approximately one million tons of CO 2 per year as an integral component of commercial operations.« less

Catalysis of CO₂ absorption in aqueous solution by inorganic oxoanions and their application to post combustion capture.

PubMed

Phan, Duong T; Maeder, Marcel; Burns, Robert C; Puxty, Graeme

2014-04-15

To reduce CO2 emission into the atmosphere, particularly from coal-fired power stations, post combustion capture (PCC) using amine-based solvents to chemically absorb CO2 has been extensively developed. From an infrastructure viewpoint, the faster the absorption of CO2, the smaller the absorber required. The use of catalysts for this process has been broadly studied. In this manuscript, a study of the catalytic efficiencies of inorganic oxoanions such as arsenite, arsenate, phosphite, phosphate, and borate is described. The kinetics of the accelerated CO2 absorption at 25 °C was investigated using stopped-flow spectrophotometry. The catalytic rate constants of these anions for the reaction of CO2 with H2O were determined to be 137.7(3), 30.3(7), 69(2), 32.7(9), and 13.66(7) M(-1)s(-1), respectively. A new mechanism for the catalytic reaction of oxoanions with CO2 has also been proposed. The applicability of these catalysts to PCC was further studied by simulation of the absorption process under PCC conditions using their experimental catalytic rate constants. Arsenite and phosphite were confirmed to be the best catalysts for CO2 capture. However, considering the toxicological effect of arsenic and the oxidative instability of phosphite, phosphate would be the most promising inorganic catalyst for PCC process from the series of inorganic oxoanions studied.

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...

Heteroatom-doped nanoporous carbon derived from MOF-5 for CO2 capture

NASA Astrophysics Data System (ADS)

Ma, Xiancheng; Li, Liqing; Chen, Ruofei; Wang, Chunhao; Li, Hailong; Wang, Shaobin

2018-03-01

Four nanoporous carbons (MUCT) were prepared from metal-organic framework (MOF-5) template and additional carbon source (i.e. urea) by carbonization at different temperatures (600-900 °C). The results showed that specific surface area of four samples was obtained in the range from 1030 to 2307 m2 g-1. By changing the carbonization temperature it can finely tune the pore volume of the MUCT, which having a uniform pore size of around 4.0 nm. With an increasing carbonization temperature, the micropore surface area of MUCT samples varied slightly, but mesopore surface area increased obviously, which had little influence on carbon dioxide (CO2) adsorption capacity. The as-obtained sample MUC900 exhibited the superior CO2 capture capacity of 3.7 mmol g-1 at 0 °C (1 atm). First principle calculations were conducted on carbon models with various functional groups to distinguish heterogeneity and understand carbon surface chemistry for CO2 adsorption. The interaction between CO2 and N-containing functional groups is mainly weak Lewis acid-base interaction. On the other hand, the pyrrole and amine groups show exceptional hydrogen-bonding interaction. The hydroxyls promote the interaction between carbon dioxide and functional groups through hydrogen-bonding interactions and electrostatic potentials, thereby increasing CO2 capture of MUCT.

Amine-tethered solid adsorbents coupling high adsorption capacity and regenerability for CO2 capture from ambient air.

PubMed

Choi, Sunho; Gray, McMahan L; Jones, Christopher W

2011-05-23

Silica supported poly(ethyleneimine) (PEI) materials are prepared via impregnation and demonstrated to be promising adsorbents for CO(2) capture from ultra-dilute gas streams such as ambient air. A prototypical class 1 adsorbent, containing 45 wt% PEI (PEI/silica), and two new modified PEI-based aminosilica adsorbents, derived from PEI modified with 3-aminopropyltrimethoxysilane (A-PEI/silica) or tetraethyl orthotitanate (T-PEI/silica), are prepared and characterized by using thermogravimetric analysis and FTIR spectroscopy. The modifiers are shown to enhance the thermal stability of the polymer-oxide composites, leading to higher PEI decomposition temperatures. The modified adsorbents present extremely high CO(2) adsorption capacities under conditions simulating ambient air (400 ppm CO(2) in inert gas), exceeding 2 mol(CO (2)) kg(sorbent)(-1), as well as enhanced adsorption kinetics compared to conventional class 1 sorbents. The new adsorbents show excellent stability in cyclic adsorption-desorption operations, even under dry conditions in which aminosilica adsorbents are known to lose capacity due to urea formation. Thus, the adsorbents of this type can be considered promising materials for the direct capture of CO(2) from ultra-dilute gas streams such as ambient air. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Methanol from CO2 by organo-cocatalysis: CO2 capture and hydrogenation in one process step.

PubMed

Reller, Christian; Pöge, Matthias; Lißner, Andreas; Mertens, Florian O R L

2014-12-16

Carbon dioxide chemically bound to alcohol-amines was hydrogenated to methanol under retrieval of these industrially used CO2 capturing reagents. The energetics of the process can be seen as a partial cancellation of the exothermic heat of reaction of the hydrogenation with the endothermic one of the CO2 release from the capturing reagent. The process provides a means to significantly improve the energy efficiency of CO2 to methanol conversions.

A Critical Review of the Impacts of Leaking CO 2 Gas and Brine on Groundwater Quality

DOE Office of Scientific and Technical Information (OSTI.GOV)

Qafoku, Nikolla; Zheng, Liange; Bacon, Diana H.

2015-09-30

Geological carbon sequestration (GCS) is a global carbon emission reduction strategy involving the capture of CO 2 emitted from fossil fuel burning power plants, as well as the subsequent injection of the captured CO 2 gas into deep saline aquifers or depleted oil and gas reservoirs. A critical question that arises from the proposed GCS is the potential impacts of CO 2 injection on the quality of drinking-water systems overlying CO 2 sequestration storage sites. Although storage reservoirs are evaluated and selected based on their ability to safely and securely store emplaced fluids, leakage of CO 2 from storage reservoirsmore » is a primary risk factor and potential barrier to the widespread acceptance of geologic CO 2 sequestration (OR Harvey et al. 2013; Y-S Jun et al. 2013; DOE 2007). Therefore, a systematic understanding of how CO 2 leakage would affect the geochemistry of potable aquifers, and subsequently control or affect elemental and contaminant release via sequential and/or simultaneous abiotic and biotic processes and reactions is vital.« less

Design of Stratified Functional Nanoporous Materials for CO 2 Capture and Conversion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, J. Karl; Ye, Jingyun

The objective of this project is to develop novel nanoporous materials for CO 2 capture and conversion. The motivation of this work is that capture of CO 2 from flue gas or the atmosphere coupled with catalytic hydrogenation of CO 2 into valuable chemicals and fuels can reduce the net amount of CO 2 in the atmosphere while providing liquid transportation fuels and other commodity chemicals. One approach to increasing the economic viability of carbon capture and conversion is to design a single material that can be used for both the capture and catalytic conversion of CO 2, because suchmore » a material could increase efficiency through process intensification. We have used density functional theory (DFT) methods to design catalytic moieties that can be incorporated into various metal organic framework (MOF) materials. We chose to work with MOFs because they are highly tailorable, can be functionalized, and have been shown to selectively adsorb CO 2 over N 2, which is a requirement for CO 2 capture from flue gas. Moreover, the incorporation of molecular catalytic moieties into MOF, through covalent bonding, produces a heterogeneous catalytic material having activities and selectivities close to those of homogeneous catalysts, but without the draw-backs associated with homogeneous catalysis.« less

Initial solubility & density evaluation of Non-Aqueous system of amino acid salts for CO2 capture: potassium prolinate blended with ethanol and ethylene glycol

NASA Astrophysics Data System (ADS)

Murshid, Ghulam; Garg, Sahil

2018-05-01

Amine scrubbing is the state of the art technology for CO2 capture, and solvent selection can significantly reduce the capital and energy cost of the process. Higher energy requirement for aqueous amine based CO2 removal process is still a most important downside preventive its industrial deployment. Therefore, in this study, novel non-aqueous based amino acid salt system consisting of potassium prolinate, ethanol and ethylene glycol has been studied. This work presents initial CO2 solubility study and important physical properties i.e. density of the studied solvent system. Previous work showed that non-aqueous system of potassium prolinate and ethanol has good absorption rates and requires lower energy for solvent regeneration. However, during regeneration, solvent loss issues were found due to lower boiling point of the ethanol. Therefore, ethylene glycol was added into current studied system for enhancing the overall boiling point of the system. The good initial CO2 solubility and low density of studied solvent system offers several advantages as compared to conventional amine solutions.

An early deployment strategy for carbon capture, utilisation, and storage

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carter, L.D.

2012-11-01

This report describes the current use of CO2 for EOR, and discusses potential expansion of EOR using CO2 from power plants. Analysis of potential EOR development in the USA, where most current CO2-based EOR production takes place, indicates that relatively low cost, traditional sources of CO2 for EOR (CO2 domes and CO2 from natural gas processing plants) are insufficient to exploit the full potential of EOR. To achieve that full potential will require use of CO2 from combustion and gasification systems, such as fossil fuel power plants, where capture of CO2 is more costly. The cost of current CCUS systems,more » even with the revenue stream for sale of the CO2 for EOR, is too high to result in broad deployment of the technology in the near term. In the longer term, research and development may be sufficient to reduce CO2 capture costs to a point where CCUS would be broadly deployed. This report describes a case study of conditions in the USA to explore a financial incentive to promote early deployment of CCUS, providing a range of immediate benefits to society, greater likelihood of reducing the long-term cost of CCUS, and greater likelihood of broad deployment of CCUS and CCS in the long term. Additionally, it may be possible to craft such an incentive in a manner that its cost is more than offset by taxes flowing from increased domestic oil production. An example of such an incentive is included in this report.« less

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

Phase-Change Aminopyridines as Carbon Dioxide Capture Solvents

DOE Office of Scientific and Technical Information (OSTI.GOV)

Malhotra, Deepika; Page, Jordan P.; Bowden, Mark E.

Carbon dioxide is the main atmospheric greenhouse gas released from industrial point sources. In order to mitigate adverse environmental effects of these emissions, carbon capture, storage and utilization is required. To this end, several CO2 capture technologies are being developed for application in carbon capture, which include aqueous amines and water-lean solvents. Herein we report new aminopyridine solvents with the potential for CO2 capture from coal-fired power plants. These four solvents 2-picolylamine, 3-picolylamine, 4-picolylamine and N’-(pyridin-4-ylmethyl)ethane-1,2-diamine are liquids that rapidly bind CO2 to form crystalline solids at standard room temperature and pressure. These solvents have displayed high CO2 capture capacitymore » (11 - 20 wt%) and can be regenerated at temperatures in the range of 120 - 150 C. The advantage of these primary aminopyridine solvents is that crystalline salt product can be separated, making it possible to regenerate only the CO2-rich solid ultimately resulting in reduced energy penalty.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

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

CO 2 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 CO 2 capture from coal-fired power plants. Here, we propose that near-term investment could focus on implementing CO 2 capture on facilities that produce high-value chemicals/products. These facilities can absorb the expected impact of the marginal increase in the costmore » of production on the price of their product, due to the addition of CO 2 capture, more than coal-fired power plants. A financially viable demonstration of a large-scale CCUS network requires offsetting the costs of CO 2 capture by using the CO 2 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 CO 2 is captured from ethylene producers and used for enhanced oil recovery in the U.S. Gulf Coast region.« less

Large Pilot-Scale Carbon Dioxide (CO2) Capture Project Using Aminosilicone Solvent.Final Scientific/Technical Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hancu, Dan

GE Global Research has developed, over the last 8 years, a platform of cost effective CO2 capture technologies based on a non-aqueous aminosilicone solvent (GAP-1m). As demonstrated in previous funded DOE projects (DE-FE0007502 and DEFE0013755), the GAP-1m solvent has increased CO2 working capacity, lower volatility and corrosivity than the benchmark aqueous amine technology. Performance of the GAP-1m solvent was recently demonstrated in a 0.5 MWe pilot at National Carbon Capture Center, AL with real flue gas for over 500 hours of operation using a Steam Stripper Column (SSC). The pilot-scale PSTU engineering data were used to (i) update the techno-economicmore » analysis, and EH&S assessment, (ii) perform technology gap analysis, and (iii) conduct the solvent manufacturability and scale-up study.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Benson, Steven; Envergex, Srivats; Browers, Bruce

Barr Engineering Co. was retained by the Institute for Energy Studies (IES) at University of North Dakota (UND) to conduct a technical and economic feasibility analysis of an innovative hybrid sorbent technology (CACHYS™) for carbon dioxide (CO2) capture and separation from coal combustion–derived flue gas. The project team for this effort consists of the University of North Dakota, Envergex LLC, Barr Engineering Co., and Solex Thermal Science, along with industrial support from Allete, BNI Coal, SaskPower, and the North Dakota Lignite Energy Council. An initial economic and feasibility study of the CACHYS™ concept, including definition of the process, development ofmore » process flow diagrams (PFDs), material and energy balances, equipment selection, sizing and costing, and estimation of overall capital and operating costs, is performed by Barr with information provided by UND and Envergex. The technology—Capture from Existing Coal-Fired Plants by Hybrid Sorption Using Solid Sorbents Capture (CACHYS™)—is a novel solid sorbent technology based on the following ideas: reduction of energy for sorbent regeneration, utilization of novel process chemistry, contactor conditions that minimize sorbent-CO2 heat of reaction and promote fast CO2 capture, and a low-cost method of heat management. The technology’s other key component is the use of a low-cost sorbent.« less

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...

Investigation of CO2 capture mechanisms of liquid-like nanoparticle organic hybrid materials via structural characterization.

PubMed

Park, Youngjune; Decatur, John; Lin, Kun-Yi Andrew; Park, Ah-Hyung Alissa

2011-10-28

Nanoparticle organic hybrid materials (NOHMs) have been recently developed that comprise an oligomeric or polymeric canopy tethered to surface-modified nanoparticles via ionic or covalent bonds. It has already been shown that the tunable nature of the grafted polymeric canopy allows for enhanced CO(2) capture capacity and selectivity via the enthalpic intermolecular interactions between CO(2) and the task-specific functional groups, such as amines. Interestingly, for the same amount of CO(2) loading NOHMs have also exhibited significantly different swelling behavior compared to that of the corresponding polymers, indicating a potential structural effect during CO(2) capture. If the frustrated canopy species favor spontaneous ordering due to steric and/or entropic effects, the inorganic cores of NOHMs could be organized into unusual structural arrangements. Likewise, the introduction of small gaseous molecules such as CO(2) could reduce the free energy of the frustrated canopy. This entropic effect, the result of unique structural nature, could allow NOHMs to capture CO(2) more effectively. In order to isolate the entropic effect, NOHMs were synthesized without the task-specific functional groups. The relationship between their structural conformation and the underlying mechanisms for the CO(2) absorption behavior were investigated by employing NMR and ATR FT-IR spectroscopies. The results provide fundamental information needed for evaluating and developing novel liquid-like CO(2) capture materials and give useful insights for designing and synthesizing NOHMs for more effective CO(2) capture. This journal is © the Owner Societies 2011

CO.sub.2 separation from low-temperature flue gases

DOEpatents

Dilmore, Robert; Allen, Douglas; Soong, Yee; Hedges, Sheila

2010-11-30

Two methods are provide for the separation of carbon dioxide from the flue gases. The first method utilizes a phase-separating moiety dissolved in an aqueous solution of a basic moiety to capture carbon dioxide. The second method utilizes a phase-separating moiety as a suspended solid in an aqueous solution of a basic moiety to capture carbon dioxide. The first method takes advantage of the surface-independent nature of the CO.sub.2 absorption reactions in a homogeneous aqueous system. The second method also provides permanent sequestration of the carbon dioxide. Both methods incorporate the kinetic rate enhancements of amine-based scrubbing while eliminating the need to heat the entire amine solution (80% water) in order to regenerate and release CO.sub.2. Both methods also take advantage of the low-regeneration temperatures of CO.sub.2-bearing mineral systems such as Na.sub.2CO.sub.3/NaHCO.sub.3 and K.sub.2CO.sub.3/KHCO.sub.3.

CO₂ carbonation under aqueous conditions using petroleum coke combustion fly ash.

PubMed

González, A; Moreno, N; Navia, R

2014-12-01

Fly ash from petroleum coke combustion was evaluated for CO2 capture in aqueous medium. Moreover the carbonation efficiency based on different methodologies and the kinetic parameters of the process were determined. The results show that petroleum coke fly ash achieved a CO2 capture yield of 21% at the experimental conditions of 12 g L(-1), 363°K without stirring. The carbonation efficiency by petroleum coke fly ash based on reactive calcium species was within carbonation efficiencies reported by several authors. In addition, carbonation by petroleum coke fly ash follows a pseudo-second order kinetic model. Copyright © 2014 Elsevier Ltd. All rights reserved.

Reassessing the Efficiency Penalty from Carbon Capture in Coal-Fired Power Plants.

PubMed

Supekar, Sarang D; Skerlos, Steven J

2015-10-20

This paper examines thermal efficiency penalties and greenhouse gas as well as other pollutant emissions associated with pulverized coal (PC) power plants equipped with postcombustion CO2 capture for carbon sequestration. We find that, depending on the source of heat used to meet the steam requirements in the capture unit, retrofitting a PC power plant that maintains its gross power output (compared to a PC power plant without a capture unit) can cause a drop in plant thermal efficiency of 11.3-22.9%-points. This estimate for efficiency penalty is significantly higher than literature values and corresponds to an increase of about 5.3-7.7 US¢/kWh in the levelized cost of electricity (COE) over the 8.4 US¢/kWh COE value for PC plants without CO2 capture. The results follow from the inclusion of mass and energy feedbacks in PC power plants with CO2 capture into previous analyses, as well as including potential quality considerations for safe and reliable transportation and sequestration of CO2. We conclude that PC power plants with CO2 capture are likely to remain less competitive than natural gas combined cycle (without CO2 capture) and on-shore wind power plants, both from a levelized and marginal COE point of view.

Synthesis of polybenzoxazine based nitrogen-rich porous carbons for carbon dioxide capture

NASA Astrophysics Data System (ADS)

Wan, Liu; Wang, Jianlong; Feng, Chong; Sun, Yahui; Li, Kaixi

2015-04-01

Nitrogen-rich porous carbons (NPCs) were synthesized from 1,5-dihydroxynaphthalene, urea, and formaldehyde based on benzoxazine chemistry by a soft-templating method with KOH chemical activation. They possess high surface areas of 856.8-1257.8 m2 g-1, a large pore volume of 0.15-0.65 cm3 g-1, tunable pore structure, high nitrogen content (5.21-5.32 wt%), and high char yields. The amount of the soft-templating agent F127 has multiple influences on the textural and chemical properties of the carbons, affecting the surface area and pore structure, impacting the compositions of nitrogen species and resulting in an improvement of the CO2 capture performance. At 1 bar, high CO2 uptake of 4.02 and 6.35 mmol g-1 at 25 and 0 °C was achieved for the sample NPC-2 with a molar ratio of F127 : urea = 0.010 : 1. This can be attributed to its well-developed micropore structure and abundant pyridinic nitrogen, pyrrolic nitrogen and pyridonic nitrogen functionalities. The sample NPC-2 also exhibits a remarkable selectivity for CO2/N2 separation and a fast adsorption/desorption rate and can be easily regenerated. This suggests that the polybenzoxazine-based NPCs are desirable for CO2 capture because of possessing a high micropore surface area, a large micropore volume, appropriate pore size distribution, and a large number of basic nitrogen functionalities.Nitrogen-rich porous carbons (NPCs) were synthesized from 1,5-dihydroxynaphthalene, urea, and formaldehyde based on benzoxazine chemistry by a soft-templating method with KOH chemical activation. They possess high surface areas of 856.8-1257.8 m2 g-1, a large pore volume of 0.15-0.65 cm3 g-1, tunable pore structure, high nitrogen content (5.21-5.32 wt%), and high char yields. The amount of the soft-templating agent F127 has multiple influences on the textural and chemical properties of the carbons, affecting the surface area and pore structure, impacting the compositions of nitrogen species and resulting in an improvement of the CO2 capture performance. At 1 bar, high CO2 uptake of 4.02 and 6.35 mmol g-1 at 25 and 0 °C was achieved for the sample NPC-2 with a molar ratio of F127 : urea = 0.010 : 1. This can be attributed to its well-developed micropore structure and abundant pyridinic nitrogen, pyrrolic nitrogen and pyridonic nitrogen functionalities. The sample NPC-2 also exhibits a remarkable selectivity for CO2/N2 separation and a fast adsorption/desorption rate and can be easily regenerated. This suggests that the polybenzoxazine-based NPCs are desirable for CO2 capture because of possessing a high micropore surface area, a large micropore volume, appropriate pore size distribution, and a large number of basic nitrogen functionalities. Electronic supplementary information (ESI) available: Elemental and XPS analyses and XPS peak positions and relative content of N species in the NPCs. See DOI: 10.1039/c4nr07409b

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

Carbon dioxide capture from a cement manufacturing process

DOEpatents

Blount, Gerald C [North Augusta, SC; Falta, Ronald W [Seneca, SC; Siddall, Alvin A [Aiken, SC

2011-07-12

A process of manufacturing cement clinker is provided in which a clean supply of CO.sub.2 gas may be captured. The process also involves using an open loop conversion of CaO/MgO from a calciner to capture CO.sub.2 from combustion flue gases thereby forming CaCO.sub.3/CaMg(CO.sub.3).sub.2. The CaCO.sub.3/CaMg(CO.sub.3).sub.2 is then returned to the calciner where CO.sub.2 gas is evolved. The evolved CO.sub.2 gas, along with other evolved CO.sub.2 gases from the calciner are removed from the calciner. The reactants (CaO/MgO) are feed to a high temperature calciner for control of the clinker production composition.

Near-term deployment of carbon capture and sequestration from biorefineries in the United States.

PubMed

Sanchez, Daniel L; Johnson, Nils; McCoy, Sean T; Turner, Peter A; Mach, Katharine J

2018-05-08

Capture and permanent geologic sequestration of biogenic CO 2 emissions may provide critical flexibility in ambitious climate change mitigation. However, most bioenergy with carbon capture and sequestration (BECCS) technologies are technically immature or commercially unavailable. Here, we evaluate low-cost, commercially ready CO 2 capture opportunities for existing ethanol biorefineries in the United States. The analysis combines process engineering, spatial optimization, and lifecycle assessment to consider the technical, economic, and institutional feasibility of near-term carbon capture and sequestration (CCS). Our modeling framework evaluates least cost source-sink relationships and aggregation opportunities for pipeline transport, which can cost-effectively transport small CO 2 volumes to suitable sequestration sites; 216 existing US biorefineries emit 45 Mt CO 2 annually from fermentation, of which 60% could be captured and compressed for pipeline transport for under $25/tCO 2 A sequestration credit, analogous to existing CCS tax credits, of $60/tCO 2 could incent 30 Mt of sequestration and 6,900 km of pipeline infrastructure across the United States. Similarly, a carbon abatement credit, analogous to existing tradeable CO 2 credits, of $90/tCO 2 can incent 38 Mt of abatement. Aggregation of CO 2 sources enables cost-effective long-distance pipeline transport to distant sequestration sites. Financial incentives under the low-carbon fuel standard in California and recent revisions to existing federal tax credits suggest a substantial near-term opportunity to permanently sequester biogenic CO 2 This financial opportunity could catalyze the growth of carbon capture, transport, and sequestration; improve the lifecycle impacts of conventional biofuels; support development of carbon-negative fuels; and help fulfill the mandates of low-carbon fuel policies across the United States. Copyright © 2018 the Author(s). Published by PNAS.

Near-term deployment of carbon capture and sequestration from biorefineries in the United States

PubMed Central

Johnson, Nils; McCoy, Sean T.; Turner, Peter A.; Mach, Katharine J.

2018-01-01

Capture and permanent geologic sequestration of biogenic CO2 emissions may provide critical flexibility in ambitious climate change mitigation. However, most bioenergy with carbon capture and sequestration (BECCS) technologies are technically immature or commercially unavailable. Here, we evaluate low-cost, commercially ready CO2 capture opportunities for existing ethanol biorefineries in the United States. The analysis combines process engineering, spatial optimization, and lifecycle assessment to consider the technical, economic, and institutional feasibility of near-term carbon capture and sequestration (CCS). Our modeling framework evaluates least cost source–sink relationships and aggregation opportunities for pipeline transport, which can cost-effectively transport small CO2 volumes to suitable sequestration sites; 216 existing US biorefineries emit 45 Mt CO2 annually from fermentation, of which 60% could be captured and compressed for pipeline transport for under $25/tCO2. A sequestration credit, analogous to existing CCS tax credits, of $60/tCO2 could incent 30 Mt of sequestration and 6,900 km of pipeline infrastructure across the United States. Similarly, a carbon abatement credit, analogous to existing tradeable CO2 credits, of $90/tCO2 can incent 38 Mt of abatement. Aggregation of CO2 sources enables cost-effective long-distance pipeline transport to distant sequestration sites. Financial incentives under the low-carbon fuel standard in California and recent revisions to existing federal tax credits suggest a substantial near-term opportunity to permanently sequester biogenic CO2. This financial opportunity could catalyze the growth of carbon capture, transport, and sequestration; improve the lifecycle impacts of conventional biofuels; support development of carbon-negative fuels; and help fulfill the mandates of low-carbon fuel policies across the United States. PMID:29686063

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

PubMed Central

2017-01-01

Developing efficient methods for capture and controlled release of carbon dioxide is crucial to any carbon capture and utilization technology. Herein we present an approach using an organic semiconductor electrode to electrochemically capture dissolved CO2 in aqueous electrolytes. The process relies on electrochemical reduction of a thin film of a naphthalene bisimide derivative, 2,7-bis(4-(2-(2-ethylhexyl)thiazol-4-yl)phenyl)benzo[lmn][3,8]phenanthroline-1,3,6,8(2H,7H)-tetraone (NBIT). This molecule is specifically tailored to afford one-electron reversible and one-electron quasi-reversible reduction in aqueous conditions while not dissolving or degrading. The reduced NBIT reacts with CO2 to form a stable semicarbonate salt, which can be subsequently oxidized electrochemically to release CO2. The semicarbonate structure is confirmed by in situ IR spectroelectrochemistry. This process of capturing and releasing carbon dioxide can be realized in an oxygen-free environment under ambient pressure and temperature, with uptake efficiency for CO2 capture of ∼2.3 mmol g–1. This is on par with the best solution-phase amine chemical capture technologies available today. PMID:28378994

Important roles of enthalpic and entropic contributions to CO2 capture from simulated flue gas and ambient air using mesoporous silica grafted amines.

PubMed

Alkhabbaz, Mustafa A; Bollini, Praveen; Foo, Guo Shiou; Sievers, Carsten; Jones, Christopher W

2014-09-24

The measurement of isosteric heats of adsorption of silica supported amine materials in the low pressure range (0-0.1 bar) is critical for understanding the interactions between CO2 and amine sites at low coverage and hence to the development of efficient amine adsorbents for CO2 capture from flue gas and ambient air. Heats of adsorption for an array of silica-supported amine materials are experimentally measured at low coverage using a Calvet calorimeter equipped with a customized dosing manifold. In a series of 3-aminopropyl-functionalized silica materials, higher amine densities resulted in higher isosteric heats of adsorption, clearly showing that the density/proximity of amine sites can influence the amine efficiency of adsorbents. In a series of materials with fixed amine loading but different amine types, strongly basic primary and secondary amine materials are shown to have essentially identical heats of adsorption near 90 kJ/mol. However, the adsorption uptakes vary substantially as a function of CO2 partial pressure for different primary and secondary amines, demonstrating that entropic contributions to adsorption may play a key role in adsorption at secondary amine sites, making adsorption at these sites less efficient at the low coverages that are important to the direct capture of CO2 from ambient air. Thus, while primary amines are confirmed to be the most effective amine types for CO2 capture from ambient air, this is not due to enhanced enthalpic contributions associated with primary amines over secondary amines, but may be due to unfavorable entropic factors associated with organization of the second alkyl chain on the secondary amine during CO2 adsorption. Given this hypothesis, favorable entropic factors may be the main reason primary amine based adsorbents are more effective under air capture conditions.

Method and system for capturing carbon dioxide and/or sulfur dioxide from gas stream

DOEpatents

Chang, Shih-Ger; Li, Yang; Zhao, Xinglei

2014-07-08

The present invention provides a system for capturing CO.sub.2 and/or SO.sub.2, comprising: (a) a CO.sub.2 and/or SO.sub.2 absorber comprising an amine and/or amino acid salt capable of absorbing the CO.sub.2 and/or SO.sub.2 to produce a CO.sub.2- and/or SO.sub.2-containing solution; (b) an amine regenerator to regenerate the amine and/or amino acid salt; and, when the system captures CO.sub.2, (c) an alkali metal carbonate regenerator comprising an ammonium catalyst capable catalyzing the aqueous alkali metal bicarbonate into the alkali metal carbonate and CO.sub.2 gas. The present invention also provides for a system for capturing SO.sub.2, comprising: (a) a SO.sub.2 absorber comprising aqueous alkali metal carbonate, wherein the alkali metal carbonate is capable of absorbing the SO.sub.2 to produce an alkali metal sulfite/sulfate precipitate and CO.sub.2.

In-situ capture and conversion of atmospheric CO2 into nano-CaCO3 using a novel pathway based on deep eutectic choline chloride-calcium chloride.

PubMed

Karimi, Mohammad; Jodaei, Akbar; Khajvandi, Asiyeh; Sadeghinik, Amirhosein; Jahandideh, Rahim

2018-01-15

This study presents a newfangled method and provides a new approach toward capturing-entrapping the toxic and harmful greenhouse gas CO 2 and subsequently employing it as a useful precursor for the production of value-added calcite (CaCO 3 ) nanoparticles. All the processes are done in a single system (one-pot and in-situ processing) based on deep eutectic choline chloride-calcium chloride (Calcoline) at mild temperature of 50 °C in direct contact with air. The Calcoline eutectic mixture shows the calcite production yield of 6.2 mg/ml that is reduced up to 22.6% upon recycling. The eutectic mixture provides an interesting all-in-one system acting as carbon dioxide trapper/adsorbent, solvent to solubilize CO 2 , and reagent to convert solubilized CO 2 into pure calcite nanoparticles with average particle size of 30 nm. The featured properties of the developed method including simplicity, recyclability, mobility, affordability, and sustainability make it feasible for large scale applications by which the simultaneous elimination of CO 2 from the environment and conversion of it into value added nano-products will be practicable. Copyright © 2017 Elsevier Ltd. All rights reserved.

Carbon dioxide (hydrogen sulfide) membrane separations and WGS membrane reactor modeling for fuel cells

NASA Astrophysics Data System (ADS)

Huang, Jin

Acid-gas removal is of great importance in many environmental or energy-related processes. Compared to current commercial technologies, membrane-based CO2 and H2S capture has the advantages of low energy consumption, low weight and space requirement, simplicity of installation/operation, and high process flexibility. However, the large-scale application of the membrane separation technology is limited by the relatively low transport properties. In this study, CO2 (H2S)-selective polymeric membranes with high permeability and high selectivity have been studied based on the facilitated transport mechanism. The membrane showed facilitated effect for both CO2 and H2S. A CO2 permeability of above 2000 Barrers, a CO2/H2 selectivity of greater than 40, and a CO2/N2 selectivity of greater than 200 at 100--150°C were observed. As a result of higher reaction rate and smaller diffusing compound, the H2S permeability and H2S/H2 selectivity were about three times higher than those properties for CO2. The novel CO2-selective membrane has been applied to capture CO 2 from flue gas and natural gas. In the CO2 capture experiments from a gas mixture with N2 and H2, a permeate CO 2 dry concentration of greater than 98% was obtained by using steam as the sweep gas. In CO2/CH4 separation, decent CO 2 transport properties were obtained with a feed pressure up to 500 psia. With the thin-film composite membrane structure, significant increase on the CO2 flux was achieved with the decrease of the selective layer thickness. With the continuous removal of CO2, CO2-selective water-gas-shift (WGS) membrane reactor is a promising approach to enhance CO conversion and increase the purity of H2 at process pressure under relatively low temperature. The simultaneous reaction and transport process in the countercurrent WGS membrane reactor was simulated by using a one-dimensional non-isothermal model. The modeling results show that a CO concentration of less than 10 ppm and a H2 recovery of greater than 97% are achievable from reforming syngases. In an experimental study, the reversible WGS was shifted forward by removing CO2 so that the CO concentration was significantly decreased to less than 10 ppm. The modeling results agreed well with the experimental data.

Emerging materials for lowering atmospheric carbon

DOE PAGES

Barkakaty, Balaka; Sumpter, Bobby G.; Ivanov, Ilia N.; ...

2016-12-08

CO 2 emissions from anthropogenic sources and the rate at which they increase could have deep global ramifications such as irreversible climate change and increased natural disasters. Because greater than 50% of anthropogenic CO 2 emissions come from small, distributed sectors such as homes, offices, and transportation sources, most renewable energy systems and on-site carbon capture technologies for reducing future CO 2 emissions cannot be effectively utilized. This problem might be mediated by considering novel materials and technologies for directly capturing/removing CO 2 from air. But, compared to materials for capturing CO 2 at on-site emission sources, materials for capturingmore » CO 2 directly from air must be more selective to CO 2, and should operate and be stable at near ambient conditions. Here, we briefly summarize the recent developments in materials for capturing carbon dioxide directly from air. Furthermore, we discuss the challenges in this field and offer a perspective for developing the current state-of-art and also highlight the potential of a few recent discoveries in materials science that show potential for advanced application of air capture technology.« less

Demonstration of Advanced CO 2 Capture Process Improvements for Coal-Fired Flue Gas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carroll, John

This document summarizes the activities of Cooperative Agreement DE-FE0026590, “Demonstration of Advanced CO 2 Capture Process Improvements for Coal-Fired Flue Gas” during the performance period of October 1, 2015 through May 31, 2017. This project was funded by the U.S. Department of Energy (DOE) National Energy Technology Laboratory (NETL). Southern Company Services, Inc. (SCS) was the prime contractor and co-funder of the project. Mitsubishi Heavy Industries America (MHIA) and AECOM were project team members. The overall project objective was to improve costs, energy requirements, and performance of an existing amine-based CO 2 capture process. This will occur via improvements inmore » three areas: 1. Reboiler design – The first objective of the program was to demonstrate performance of an integrated stripper/reboiler (termed Built-in Reboiler, or BIR) to reduce footprint, capital costs, and integration issues of the current technology. 2. Particulate management – The second objective was to carry out a Particulate Matter Management (PMM) test. This has the potential to reduce operating costs and capital costs due to the reduced or eliminated need for mechanical filtration. 3. Solvent – The third objective was to carry out a new solvent test plan (referred to as NSL) to demonstrate a new solvent (termed New Solvent A), which is expected to reduce regeneration steam. The bulk price is also expected to be lower than KS-1, which is the current solvent used in this process. NSL testing would include baseline testing, optimization, long term testing, solvent reclamation testing, and final inspection. These combine to form the Advanced Carbon Capture (ACC) technology. Much of this work will be applicable to generic solvent processes, especially in regards to improved reboiler design, and focused to meet or exceed the DOE’s overall carbon capture performance goals of 90% CO 2 capture rate with 95% CO 2 purity at a cost of $40/tonne of CO 2 by 2025 and at a cost of electricity (COE) 30% less than baseline CO 2 capture approaches by 2030. This project was divided into two phases. Phase 1 is the planning phase, and Phase 2 is the construction, operations, testing, and analysis phase. A down select occurred after Phase 1. Phase 1 activities were carried out during this reporting period, and therefore, Phase 1 activities are solely considered in this report. The project was not selected for Phase 2 funding.« less

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. Copyright © 2012 Elsevier Ltd. All rights reserved.

Efficient light hydrocarbon separation and CO2 capture and conversion in a stable MOF with oxalamide-decorated polar tubes.

PubMed

Li, Xiu-Yuan; Li, Yong-Zhi; Yang, Yun; Hou, Lei; Wang, Yao-Yu; Zhu, Zhonghua

2017-11-30

The first strontium-based MOF possessing polar tubular channels embedded with a high density of open Lewis acidic metal sites and basic oxalamide groups was constructed, which shows not only a high CO 2 and C 2 H 6 adsorption capability and significant selectivity for CO 2 over both CH 4 and CO, and for C 2 H 6 over CH 4 , but also size-selective chemical conversion of CO 2 with epoxides producing cyclic carbonates under ambient conditions.

Absorption of CO2 on Carbon-based Sensors: First-Principle Analysis

NASA Astrophysics Data System (ADS)

Tit, Nacir; Elezzi, Mohammed; Abdullah, Hasan; Bahlouli, Hocine; Yamani, Zain

We present first-principle investigation of the adsorption properties of CO and CO2 molecules on both graphene and carbon nano-tubes (CNTs) in presence of metal catalysis, mainly iron (Fe). The relaxations were carried out using the self-consistent-charge density-functional tight-binding (SCC-DFTB) code in neglect of heat effects. The results show the following: (1) Defected graphene is found to have high sensitivity and high selectivity towards chemisorption of CO molecules and weak physisorption with CO2 molecules. (2) In case of CNTs, the iron ``Fe'' catalyst plays an essential role in capturing CO2 molecules. The Fe ad-atoms on the surface of CNT introduce huge density of states at Fermi level, but the capture of CO2 molecules would reduce that density and consequently reduce conductivity and increase sensitivity. Concerning the selectivity, we have studied the sensitivity versus various gas molecules (such as: O2, N2, H2, H2O, and CO). Furthermore, to assess the effect of catalysis on sensitivity, we have studied the sensitivity of other metal catalysts (such as: Ni, Co, Ti, and Sc). We found that CNT-Fe is highly sensitive and selective towards detection of CO and CO2 molecules. CNT being conductive or semiconducting does not matter much on the adsorption properties.

The role of CO2 capture and utilization in mitigating climate change

NASA Astrophysics Data System (ADS)

Mac Dowell, Niall; Fennell, Paul S.; Shah, Nilay; Maitland, Geoffrey C.

2017-04-01

To offset the cost associated with CO2 capture and storage (CCS), there is growing interest in finding commercially viable end-use opportunities for the captured CO2. In this Perspective, we discuss the potential contribution of carbon capture and utilization (CCU). Owing to the scale and rate of CO2 production compared to that of utilization allowing long-term sequestration, it is highly improbable the chemical conversion of CO2 will account for more than 1% of the mitigation challenge, and even a scaled-up enhanced oil recovery (EOR)-CCS industry will likely only account for 4-8%. Therefore, whilst CO2-EOR may be an important economic incentive for some early CCS projects, CCU may prove to be a costly distraction, financially and politically, from the real task of mitigation.

Importance of Micropore-Mesopore Interfaces in Carbon Dioxide Capture by Carbon-Based Materials.

PubMed

Durá, Gema; Budarin, Vitaliy L; Castro-Osma, José A; Shuttleworth, Peter S; Quek, Sophie C Z; Clark, James H; North, Michael

2016-08-01

Mesoporous carbonaceous materials (Starbons®) derived from low-value/waste bio-resources separate CO2 from CO2 /N2 mixtures. Compared to Norit activated charcoal (AC), Starbons® have much lower microporosities (8-32 % versus 73 %) yet adsorb up to 65 % more CO2 . The presence of interconnected micropores and mesopores is responsible for the enhanced CO2 adsorption. The Starbons® also showed three-four times higher selectivity for CO2 adsorption rather than N2 adsorption compared to AC. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Practical method of CO.sub.2 sequestration

DOEpatents

Goswami, D Yogi [Gainesville, FL; Lee, Man Su [Houston, TX; Kothurkar, Nikhil K [Tampa, FL; Stefanakos, Elias K [Tampa, FL

2011-03-01

A process and device to capture of CO.sub.2 at its originating source, such as a power plant, is disclosed. Absorbent material is recharged by desorbing CO.sub.2, so that it may be sequestered or used in another application. Continual recharging results in loss of absorbent surface area, due to pore plugging and sintering of particles. Calcium oxide or calcium hydroxide was immobilized to a fibrous ceramic-based fabric substrate as a thin film and sintered, creating an absorbent material. The samples were characterized, showing continuous cyclic carbonation conversions between about 62% and 75% under mild calcination conditions at 750.degree. C. and no CO.sub.2 in N.sub.2. Under the more severe calcination condition at 850.degree. C. and 20 wt % CO.sub.2 in N.sub.2, yttria fabric was superior to alumina as a substrate for carbon dioxide capture and the reactivity of the calcium oxide absorbent immobilized to yttria was maintained at the same level in the 12 cycles.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

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 themore » energy needed for the process.« less

Novel polymer membrane process for pre-combustion CO{sub 2} capture from coal-fired syngas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Merkel, Tim

2011-09-14

This final report describes work conducted for the Department of Energy (DOE NETL) on development of a novel polymer membrane process for pre-combustion CO{sub 2} capture from coalfired syngas (award number DE-FE0001124). The work was conducted by Membrane Technology and Research, Inc. (MTR) from September 15, 2009, through December 14, 2011. Tetramer Technologies, LLC (Tetramer) was our subcontract partner on this project. The National Carbon Capture Center (NCCC) at Wilsonville, AL, provided access to syngas gasifier test facilities. The main objective of this project was to develop a cost-effective membrane process that could be used in the relatively near-term tomore » capture CO{sub 2} from shifted syngas generated by a coal-fired Integrated Gasification Combined Cycle (IGCC) power plant. In this project, novel polymeric membranes (designated as Proteus™ membranes) with separation properties superior to conventional polymeric membranes were developed. Hydrogen permeance of up to 800 gpu and H{sub 2}/CO{sub 2} selectivity of >12 was achieved using a simulated syngas mixture at 150°C and 50 psig, which exceeds the original project targets of 200 gpu for hydrogen permeance and 10 for H{sub 2}/CO{sub 2} selectivity. Lab-scale Proteus membrane modules (with a membrane area of 0.13 m{sup 2}) were also developed using scaled-up Proteus membranes and high temperature stable module components identified during this project. A mixed-gas hydrogen permeance of about 160 gpu and H{sub 2}/CO{sub 2} selectivity of >12 was achieved using a simulated syngas mixture at 150°C and 100 psig. We believe that a significant improvement in the membrane and module performance is likely with additional development work. Both Proteus membranes and lab-scale Proteus membrane modules were further evaluated using coal-derived syngas streams at the National Carbon Capture Center (NCCC). The results indicate that all module components, including the Proteus membrane, were stable under the field conditions (feed pressures: 150-175 psig and feed temperatures: 120-135°C) for over 600 hours. The field performance of both Proteus membrane stamps and Proteus membrane modules is consistent with the results obtained in the lab, suggesting that the presence of sulfur-containing compounds (up to 780 ppm hydrogen sulfide), saturated water vapor, carbon monoxide and heavy hydrocarbons in the syngas feed stream has no adverse effect on the Proteus membrane or module performance. We also performed an economic analysis for a number of membrane process designs developed in this project (using hydrogen-selective membranes, alone or in the combination with CO{sub 2}- selective membranes). The current field performance for Proteus membranes was used in the design analysis. The study showed the current best design has the potential to reduce the increase in Levelized Cost of Electricity (LCOE) caused by 90% CO{sub 2} capture to about 15% if co-sequestration of H{sub 2}S is viable. This value is still higher than the DOE target for increase in LCOE (10%); however, compared to the base-case Selexol process that gives a 30% increase in LCOE at 90% CO2 capture, the membrane-based process appears promising. We believe future improvements in membrane performance have the potential to reach the DOE target.« less

Binding CO2 from Air by a Bulky Organometallic Cation Containing Primary Amines.

PubMed

Luo, Yang-Hui; Chen, Chen; Hong, Dan-Li; He, Xiao-Tong; Wang, Jing-Wen; Ding, Ting; Wang, Bo-Jun; Sun, Bai-Wang

2018-03-21

The organometallic cation 1 (Fe(bipy-NH 2 ) 3 2+ , bipy-NH 2 = 4,4'-diamino-2,2'-bipyridine), which was constructed in situ in solution, can bind CO 2 from air effectively with a stoichiometric ratio of 1:4 (1/CO 2 ), through the formation of "H-bonded CO 2 " species: [CO 2 -OH-CO 2 ] - and [CO 2 -CO 2 -OH] - . These two species, along with the captured individual CO 2 molecules, connected 1 into a novel 3D (three-dimensional) architecture, that was crystal 1·2(OH - )·4(CO 2 ). The adsorption isotherms, recycling investigations, and the heat capacity of 1 have been investigated; the results revealed that the organometallic cation 1 can be recycled at least 10 times for the real-world CO 2 capture applications. The strategies presented here may provide new hints for the development of new alkanolamine-related absorbents or technologies for CO 2 capture and sequestration.

Dynamics of Postcombustion CO2 Capture Plants: Modeling, Validation, and Case Study

PubMed Central

2017-01-01

The capture of CO2 from power plant flue gases provides an opportunity to mitigate emissions that are harmful to the global climate. While the process of CO2 capture using an aqueous amine solution is well-known from experience in other technical sectors (e.g., acid gas removal in the gas processing industry), its operation combined with a power plant still needs investigation because in this case, the interaction with power plants that are increasingly operated dynamically poses control challenges. This article presents the dynamic modeling of CO2 capture plants followed by a detailed validation using transient measurements recorded from the pilot plant operated at the Maasvlakte power station in the Netherlands. The model predictions are in good agreement with the experimental data related to the transient changes of the main process variables such as flow rate, CO2 concentrations, temperatures, and solvent loading. The validated model was used to study the effects of fast power plant transients on the capture plant operation. A relevant result of this work is that an integrated CO2 capture plant might enable more dynamic operation of retrofitted fossil fuel power plants because the large amount of steam needed by the capture process can be diverted rapidly to and from the power plant. PMID:28413256

Method and system to reclaim functional sites on a sorbent contaminated by heat stable salts

DOEpatents

Krutka, Holly; Sjostrom, Sharon; Morris, William J.

2016-03-08

The objective of this invention is to develop a method to reclaim functional sites on a CO.sub.2 sorbent that have reacted with an acid gas (other than CO.sub.2) to form heat stable salts (HSS). HSS are a significant concern for dry sorbent based CO.sub.2 capture because over time the buildup of HSS will reduce the overall functionality of the CO.sub.2 sorbent. A chemical treatment can remove the non-CO.sub.2 acid gas and reclaim functional sites that can then be used for further CO.sub.2 adsorption.

Geological Sequestration of CO2 A Brief Overview and Potential for Application for Oklahoma

EPA Science Inventory

Geologic sequestration of CO2 is a component of C capture and storage (CCS), an emerging technology for reducing CO2 emissions to the atmosphere, and involves injection of captured CO2 into deep subsurface formations. Similar to the injection of hazardous wastes, before injection...

Final Techno-Economic Analysis of 550 MWe Supercritical PC Power Plant CO 2 Capture with Linde-BASF Advanced PCC Technology

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bostick, Devin; Stoffregen, Torsten; Rigby, Sean

This topical report presents the techno-economic evaluation of a 550 MWe supercritical pulverized coal (PC) power plant utilizing Illinois No. 6 coal as fuel, integrated with 1) a previously presented (for a subcritical PC plant) Linde-BASF post-combustion CO 2 capture (PCC) plant incorporating BASF’s OASE® blue aqueous amine-based solvent (LB1) [Ref. 6] and 2) a new Linde-BASF PCC plant incorporating the same BASF OASE® blue solvent that features an advanced stripper interstage heater design (SIH) to optimize heat recovery in the PCC process. The process simulation and modeling for this report is performed using Aspen Plus V8.8. Technical information frommore » the PCC plant is determined using BASF’s proprietary thermodynamic and process simulation models. The simulations developed and resulting cost estimates are first validated by reproducing the results of DOE/NETL Case 12 representing a 550 MWe supercritical PC-fired power plant with PCC incorporating a monoethanolamine (MEA) solvent as used in the DOE/NETL Case 12 reference [Ref. 2]. The results of the techno-economic assessment are shown comparing two specific options utilizing the BASF OASE® blue solvent technology (LB1 and SIH) to the DOE/NETL Case 12 reference. The results are shown comparing the energy demand for PCC, the incremental fuel requirement, and the net higher heating value (HHV) efficiency of the PC power plant integrated with the PCC plant. A comparison of the capital costs for each PCC plant configuration corresponding to a net 550 MWe power generation is also presented. Lastly, a cost of electricity (COE) and cost of CO 2 captured assessment is shown illustrating the substantial cost reductions achieved with the Linde-BASF PCC plant utilizing the advanced SIH configuration in combination with BASF’s OASE® blue solvent technology as compared to the DOE/NETL Case 12 reference. The key factors contributing to the reduction of COE and the cost of CO 2 captured, along with quantification of the magnitude of the reductions achieved by each of these factors, are also discussed. Additionally, a high-level techno-economic analysis of one more highly advanced Linde-BASF PCC configuration case (LB1-CREB) is also presented to demonstrate the significant impact of innovative PCC plant process design improvements on further reducing COE and cost of CO 2 captured for overall plant cost and performance comparison purposes. Overall, the net efficiency of the integrated 550 MWe supercritical PC power plant with CO 2 capture is increased from 28.4% with the DOE/NETL Case 12 reference to 30.9% with the Linde-BASF PCC plant previously presented utilizing the BASF OASE® blue solvent [Ref. 6], and is further increased to 31.4% using Linde-BASF PCC plant with BASF OASE® blue solvent and an advanced SIH configuration. The Linde-BASF PCC plant incorporating the BASF OASE® blue solvent also results in significantly lower overall capital costs, thereby reducing the COE and cost of CO 2 captured from $147.25/MWh and $56.49/MT CO 2, respectively, for the reference DOE/NETL Case 12 plant, to $128.49/MWh and $41.85/MT CO 2 for process case LB1, respectively, and $126.65/MWh and $40.66/MT CO 2 for process case SIH, respectively. With additional innovative Linde-BASF PCC process configuration improvements, the COE and cost of CO2 captured can be further reduced to $125.51/MWh and $39.90/MT CO 2 for LB1-CREB. Most notably, the Linde-BASF process options presented here have already demonstrated the potential to lower the cost of CO2 captured below the DOE target of $40/MT CO 2 at the 550 MWe scale for second generation PCC technologies.« less

Structure–property reduced order model for viscosity prediction in single-component CO 2 -binding organic liquids

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cantu, David C.; Malhotra, Deepika; Koech, Phillip K.

2016-01-01

CO2 capture from power generation with aqueous solvents remains energy intensive due to the high water content of the current technology, or the high viscosity of non-aqueous alternatives. Quantitative reduced models, connecting molecular structure to bulk properties, are key for developing structure-property relationships that enable molecular design. In this work, we describe such a model that quantitatively predicts viscosities of CO2 binding organic liquids (CO2BOLs) based solely on molecular structure and the amount of bound CO2. The functional form of the model correlates the viscosity with the CO2 loading and an electrostatic term describing the charge distribution between the CO2-bearingmore » functional group and the proton-receiving amine. Molecular simulations identify the proton shuttle between these groups within the same molecule to be the critical indicator of low viscosity. The model, developed to allow for quick screening of solvent libraries, paves the way towards the rational design of low viscosity non-aqueous solvent systems for post-combustion CO2 capture. Following these theoretical recommendations, synthetic efforts of promising candidates and viscosity measurement provide experimental validation and verification.« less

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

PubMed

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

2016-12-13

The preparation of nitrogen-doped activated carbon (NACs) has received significant attention because of their applications in CO 2 capture and sequestration (CCS) owing to abundant nitrogen atoms on their surface and controllable pore structures by carefully controlled carbonization. We report high-surface-area porous N-doped activated carbons (NAC) by using soft-template-assisted self-assembly followed by thermal decomposition and KOH activation. The activation process was carried out under different temperature conditions (600-800 °C) using polyimine as precursor. The NAC-800 was found to have a high specific surface area (1900 m 2  g -1 ), a desirable micropore size below 1 nm and, more importantly, a large micropore volume (0.98 cm 3  g -1 ). NAC-800 also exhibits a significant capacity of CO 2 capture i.e., over 6. 25 and 4.87 mmol g -1 at 273 K and 298 K respectively at 1.13 bar, which is one of among the highest values reported for porous carbons so far. Moreover, NAC also shows an excellent separation selectivity for CO 2 over N 2 .

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

PubMed Central

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

2016-01-01

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

Simultaneous high efficiency capture of CO.sub.2 and H.sub.2S from pressurized gas

DOEpatents

Gal, Eli; Krishnan, Gopala N.; Jayaweera, Indira S.

2016-10-11

Low-cost and energy-efficient CO.sub.2 and H.sub.2S capture is provided obtaining greater than 99.9% capture efficiency from pressurized gas. The acid species are captured in an ammonia solution, which is then regenerated by stripping the absorbed species. The solution can capture as much as 330 grams of CO.sub.2 and H.sub.2S per 1000 gram of water and when regenerated it produces pure pressurized acid gas containing more than 99.7% CO.sub.2 and H2S. The absorption of the acid species is accomplished in two absorbers in-series, each having multiple stages. More than 95% of the acid species are captured in the first absorber and the balance is captured in the second absorber to below 10 ppm concentration in the outlet gas. The two absorbers operate at temperatures ranging from 20-70 degrees Celsius. The two absorbers and the main stripper of the alkaline solution operate at similar pressures ranging from 5-200 bara.

Slipstream pilot-scale demonstration of a novel amine-based post-combustion technology for carbon dioxide capture from coal-fired power plant flue gas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krishnamurthy, Krish R.

Post-combustion CO 2 capture (PCC) technology offers flexibility to treat the flue gas from both existing and new coal-fired power plants and can be applied to treat all or a portion of the flue gas. Solvent-based technologies are today the leading option for PCC from commercial coal-fired power plants as they have been applied in large-scale in other applications. Linde and BASF have been working together to develop and further improve a PCC process incorporating BASF’s novel aqueous amine-based solvent technology. This technology offers significant benefits compared to other solvent-based processes as it aims to reduce the regeneration energy requirementsmore » using novel solvents that are very stable under the coal-fired power plant feed gas conditions. BASF has developed the desired solvent based on the evaluation of a large number of candidates. In addition, long-term small pilot-scale testing of the BASF solvent has been performed on a lignite-fired flue gas. In coordination with BASF, Linde has evaluated a number of options for capital cost reduction in large engineered systems for solvent-based PCC technology. This report provides a summary of the work performed and results from a project supported by the US DOE (DE-FE0007453) for the pilot-scale demonstration of a Linde-BASF PCC technology using coal-fired power plant flue gas at a 1-1.5 MWe scale in Wilsonville, AL at the National Carbon Capture Center (NCCC). Following a project kick-off meeting in November 2011 and the conclusion of pilot plant design and engineering in February 2013, mechanical completion of the pilot plant was achieved in July 2014, and final commissioning activities were completed to enable start-up of operations in January 2015. Parametric tests were performed from January to December 2015 to determine optimal test conditions and evaluate process performance over a variety of operation parameters. A long-duration 1500-hour continuous test campaign was performed from May to August 2016 at a selected process condition to evaluate process performance and solvent stability over a longer period similar to how the process would operate as a continuously running large-scale PCC plant. The pilot plant integrated a number of unique features of the Linde-BASF technology aimed at lowering overall energy consumption and capital costs. During the overall test period including startup, parametric testing and long-duration testing, the pilot plant was operated for a total of 6,764 hours out of which testing with flue gas was performed for 4,109 hours. The pilot plant testing demonstrated all of the performance targets including CO 2 capture rate exceeding 90%, CO 2 purity exceeding 99.9 mol% (dry), flue gas processing capacity up to 15,500 lbs/hr (equivalent to 1.5 MWe capacity slipstream), regeneration energy as low as 2.7 GJ/tonne CO 2, and regenerator operating pressure up to 3.4 bara. Excellent solvent stability performance data was measured and verified by Linde and BASF during both test campaigns. In addition to process data, significant operational learnings were gained from pilot tests that will contribute greatly to the commercial success of PCC. Based on a thorough techno-economic assessment (TEA) of the Linde-BASF PCC process integrated with a 550 MWe supercritical coal-fired power plant, the net efficiency of the integrated power plant with CO 2 capture is increased from 28.4% with the DOE/NETL Case 12 reference to 30.9% with the Linde-BASF PCC plant previously presented utilizing the BASF OASE® blue solvent [Ref. 4], and is further increased to 31.4% using a Linde-BASF PCC plant with BASF OASE® blue solvent and an advanced stripper interstage heater (SIH) configuration. The Linde-BASF PCC plant incorporating the BASF OASE® blue solvent also results in significantly lower overall capital costs, thereby reducing the cost of electricity (COE) and cost of CO 2 captured from $147.25/MWh and $56.49/MT CO 2, respectively, for the reference DOE/NETL Case 12 plant, to $128.49/MWh and $41.85/MT CO2 for process case LB1, respectively, and $126.65/MWh and $40.66/MT CO 2 for process case SIH, respectively. With additional innovative Linde-BASF PCC process configuration improvements, the COE and cost of CO 2 captured can be further reduced to $125.51/MWh and $39.90/MT CO 2 for a further optimized PCC process defined as LB1-CREB. Most notably, the Linde-BASF process options assessed have already demonstrated the potential to lower the cost of CO 2 captured below the DOE target of $40/MT CO 2 at the 550 MWe scale for second generation PCC technologies. Project organization, structure, goals, tasks, accomplishments, process criteria and milestones will be presented in this report along with highlights and key results from parametric and long-duration testing of the Linde-BASF PCC pilot. The parametric and long-duration testing campaigns were aimed at validating the performance of the PCC technology against targets determined from a preliminary techno-economic assessment. The stability of the solvent with extended operation in a realistic power plant setting was measured with performance verified. Additionally, general solvent classification information, process operating conditions, normalized solvent performance data, solvent stability test results, flue gas conditions data, CO 2 purity data in the gaseous product stream, steam requirements and process flow diagrams, and updated process economic data for a scaled-up 550 MWe supercritical power plant with CO 2 capture are presented and discussed in this report.« less

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.

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.

Mathematical programming (MP) model to determine optimal transportation infrastructure for geologic CO2 storage in the Illinois basin

NASA Astrophysics Data System (ADS)

Rehmer, Donald E.

Analysis of results from a mathematical programming model were examined to 1) determine the least cost options for infrastructure development of geologic storage of CO2 in the Illinois Basin, and 2) perform an analysis of a number of CO2 emission tax and oil price scenarios in order to implement development of the least-cost pipeline networks for distribution of CO2. The model, using mixed integer programming, tested the hypothesis of whether viable EOR sequestration sites can serve as nodal points or hubs to expand the CO2 delivery infrastructure to more distal locations from the emissions sources. This is in contrast to previous model results based on a point-to- point model having direct pipeline segments from each CO2 capture site to each storage sink. There is literature on the spoke and hub problem that relates to airline scheduling as well as maritime shipping. A large-scale ship assignment problem that utilized integer linear programming was run on Excel Solver and described by Mourao et al., (2001). Other literature indicates that aircraft assignment in spoke and hub routes can also be achieved using integer linear programming (Daskin and Panayotopoulos, 1989; Hane et al., 1995). The distribution concept is basically the reverse of the "tree and branch" type (Rothfarb et al., 1970) gathering systems for oil and natural gas that industry has been developing for decades. Model results indicate that the inclusion of hubs as variables in the model yields lower transportation costs for geologic carbon dioxide storage over previous models of point-to-point infrastructure geometries. Tabular results and GIS maps of the selected scenarios illustrate that EOR sites can serve as nodal points or hubs for distribution of CO2 to distal oil field locations as well as deeper saline reservoirs. Revenue amounts and capture percentages both show an improvement over solutions when the hubs are not allowed to come into the solution. Other results indicate that geologic storage of CO2 into saline aquifers does not come into solutions selected by the model until the CO 2 emissions tax approaches 50/tonne. CO2 capture and storage begins to occur when the oil price is above 24.42 a barrel based on the constraints of the model. The annual storage capacity of the basin is nearly maximized when the net price of oil is as low as 40 per barrel and the CO2 emission tax is 60/tonne. The results from every subsequent scenario that was examined by this study demonstrate that EOR utilizing anthropogenically captured CO2 will earn net revenue, and thus represents an economically viable option for CO2 storage in the Illinois Basin.

Evaluation of the impact of H2O, O2, and SO2 on postcombustion CO2 capture in metal-organic frameworks.

PubMed

Yu, Jiamei; Ma, Yuguang; Balbuena, Perla B

2012-05-29

Molecular modeling methods are used to estimate the influence of impurity species: water, O(2), and SO(2) in flue gas mixtures present in postcombustion CO(2) capture using a metal organic framework, HKUST-1, as a model sorbent material. Coordinated and uncoordinated water effects on CO(2) capture are analyzed. Increase of CO(2) adsorption is observed for both cases, which can be attributed to the enhanced binding energy between CO(2) and HKUST-1 due to the introduction of a small amount of water. Density functional theory calculations indicate that the binding energy between CO(2) and HKUST-1 with coordinated water is ~1 kcal/mol higher than that without coordinated water. It is found that the improvement of CO(2)/N(2) selectivity induced by coordinated water may mainly be attributed to the increased CO(2) adsorption on the hydrated HKUST-1. On the other hand, the enhanced selectivity induced by uncoordinated water in the flue gas mixture can be explained on the basis of the competition of adsorption sites between water and CO(2) (N(2)). At low pressures, a significant CO(2)/N(2) selectivity increase is due to the increase of CO(2) adsorption and decrease of N(2) adsorption as a consequence of competition of adsorption sites between water and N(2). However, with more water molecules adsorbed at higher pressures, the competition between water and CO(2) leads to the decrease of CO(2) adsorption capacity. Therefore, high pressure operation should be avoided in HKUST-1 sorbents for CO(2) capture. In addition, the effects of O(2) and SO(2) on CO(2) capture in HKUST-1 are investigated: The CO(2)/N(2) selectivity does not change much even with relatively high concentrations of O(2) in the flue gas (up to 8%). A slightly lower CO(2)/N(2) selectivity of a CO(2)/N(2)/H(2)O/SO(2) mixture is observed compared with that in a CO(2)/N(2)/H(2)O mixture, especially at high pressures, due to the strong SO(2) binding with HKUST-1.

Carbon capture from natural gas using multi-walled CNTs based mixed matrix membranes.

PubMed

Hussain, Abid; Farrukh, Sarah; Hussain, Arshad; Ayoub, Muhammad

2017-12-05

Most of the polymers and their blends, utilized in carbon capture membranes, are costly, but cellulose acetate (CA) being inexpensive is a lucrative choice. In this research, pure and mixed matrix membranes (MMMs) have been fabricated to capture carbon from natural gas. Polyethylene glycol (PEG) has been utilized in the fabrication of membranes to modify the chain flexibility of polymers. Multi-walled carbon nanotubes (MWCNTs) provide mechanical strength, thermal stability, an extra free path for CO 2 molecules and augment CO 2 /CH 4 selectivity. Membranes of pure CA, CA/PEG blend of different PEG concentrations (5%, 10%, 15%) and CA/PEG/MWCNTs blend of 10% PEG with different MWCNTs concentrations (5%, 10%, 15%) were prepared in acetone using solution casting techniques. Fabricated membranes were characterized using SEM, TGA and tensile testing. Permeation results revealed remarkable improvement in CO 2 /CH 4 selectivity. In single gas experiments, CO 2 /CH 4 selectivity is enhanced 8 times for pure membranes containing 10% PEG and 14 times for MMMs containing 10% MWCNTs. In mix gas experiments, the CO 2 /CH 4 selectivity is increased 13 times for 10% PEG and 18 times for MMMs with 10% MWCNTs. Fabricated MMMs have a tensile strength of 13 MPa and are more thermally stable than CA membranes.

Efficient MgO-based mesoporous CO2 trapper and its performance at high temperature.

PubMed

Han, Kun Kun; Zhou, Yu; Chun, Yuan; Zhu, Jian Hua

2012-02-15

A novel MgO-based porous adsorbent has been synthesized in a facile co-precipitation method for the first time, in order to provide a candidate for trapping CO(2) in flue gas at high temperature. The resulting composite exhibits a mesoporous structure with a wide pore size distribution, due to the even dispersion and distribution of microcrystalline MgO in the framework of alumina to form a concrete-like structure. These sorbents can capture CO(2) at high temperature (150-400°C), possessing high reactivity and stability in cyclic adsorption-desorption processes, providing competitive candidates to control CO(2) emission. Copyright © 2011 Elsevier B.V. All rights reserved.

CO2 capture from humid flue gases and humid atmosphere using a microporous coppersilicate.

PubMed

Datta, Shuvo Jit; Khumnoon, Chutharat; Lee, Zhen Hao; Moon, Won Kyung; Docao, Son; Nguyen, Thanh Huu; Hwang, In Chul; Moon, Dohyun; Oleynikov, Peter; Terasaki, Osamu; Yoon, Kyung Byung

2015-10-16

Capturing CO2 from humid flue gases and atmosphere with porous materials remains costly because prior dehydration of the gases is required. A large number of microporous materials with physical adsorption capacity have been developed as CO2-capturing materials. However, most of them suffer from CO2 sorption capacity reduction or structure decomposition that is caused by co-adsorbed H2O when exposed to humid flue gases and atmosphere. We report a highly stable microporous coppersilicate. It has H2O-specific and CO2-specific adsorption sites but does not have H2O/CO2-sharing sites. Therefore, it readily adsorbs both H2O and CO2 from the humid flue gases and atmosphere, but the adsorbing H2O does not interfere with the adsorption of CO2. It is also highly stable after adsorption of H2O and CO2 because it was synthesized hydrothermally. Copyright © 2015, American Association for the Advancement of Science.

Microporosity and CO2 Capture Properties of Amorphous Silicon Oxynitride Derived from Novel Polyalkoxysilsesquiazanes

PubMed Central

Iwase, Yoshiaki; Horie, Yoji; Honda, Sawao; Daiko, Yusuke

2018-01-01

Polyalkoxysilsesquiazanes ([ROSi(NH)1.5]n, ROSZ, R = Et, nPr, iPr, nBu, sBu, nHex, sHex, cHex, decahydronaphthyl (DHNp)) were synthesized by ammonolysis at −78 °C of alkoxytrichlorosilane (ROSiCl3), which was isolated by distillation as a reaction product of SiCl4 and ROH. The simultaneous thermogravimetric and mass spectrometry analyses of the ROSZs under helium revealed a common decomposition reaction, the cleavage of the oxygen–carbon bond of the RO group to evolve alkene as a main gaseous species formed in-situ, leading to the formation of microporous amorphous Si–O–N at 550 °C to 800 °C. The microporosity in terms of the peak of the pore size distribution curve located within the micropore size range (<2 nm) and the total micropore volume, as well as the specific surface area (SSA) of the Si–O–N, increased consistently with the molecular size estimated for the alkene formed in-situ during the pyrolysis. The CO2 capture capacity at 0 °C of the Si–O–N material increased consistently with its SSA, and an excellent CO2 capture capacity of 3.9 mmol·g−1 at 0 °C and CO2 1 atm was achieved for the Si–O–N derived from DHNpOSZ having an SSA of 750 m2·g−1. The CO2 capture properties were further discussed based on their temperature dependency, and a surface functional group of the Si–O–N formed in-situ during the polymer/ceramics thermal conversion. PMID:29534056

SO 2-Resistant Immobilized Amine Sorbents for CO 2 Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tumuluri, Uma

2014-01-01

The solid amine sorbent for CO 2 capture process has advantages of simplicity and low operating cost compared to the MEA (monoethanolamine) process. Solid amine sorbents reported so far suffered from either low CO 2 capture capacity or low stability in the flue gas environment. This project is aimed at developing a SO 2-resistant solid amine sorbent for capturing CO 2 from coal–fired power plants with SCR/FGD which emits SO 2ranging from 15 to 30 ppm and NO ranging from 5 to 10 ppm. The amine sorbent we developed in a previous project degraded rapidly with 65% decrease in themore » initial capture capacity in presence of 1% SO 2. This amine sorbent was further modified by coating with polyethyleneglycol (PEG) to increase the SO 2-resistance. Polyethylene glycol (PEG) was found to decrease the SO 2-amine interaction, resulting in the decrease in the maximum SO desorption temperature (Tmax ) of amine sorbent. The PEG-coated amine sorbent exhibited higher stability with only 40% decrease in the initial capture capacity compared to un-coated amine sorbents. The cost of the solid amine sorbent developed in this project is estimated to be less than $7.00/lb; the sorbent exhibited CO 2 capture capacity more than 2.3 mmol/g. The results of this study provided the scientific basis for further development of SO 2-resistant sorbents.« less

Device-scale CFD modeling of gas-liquid multiphase flow and amine absorption for CO 2 capture: Original Research Article: Device-scale CFD modeling of gas-liquid multiphase flow and amine absorption for CO 2 capture

DOE PAGES

Pan, Wenxiao; Galvin, Janine; Huang, Wei Ling; ...

2018-03-25

In this paper we aim to develop a validated device-scale CFD model that can predict quantitatively both hydrodynamics and CO 2 capture efficiency for an amine-based solvent absorber column with random Pall ring packing. A Eulerian porous-media approach and a two-fluid model were employed, in which the momentum and mass transfer equations were closed by literature-based empirical closure models. We proposed a hierarchical approach for calibrating the parameters in the closure models to make them accurate for the packed column. Specifically, a parameter for momentum transfer in the closure was first calibrated based on data from a single experiment. Withmore » this calibrated parameter, a parameter in the closure for mass transfer was next calibrated under a single operating condition. Last, the closure of the wetting area was calibrated for each gas velocity at three different liquid flow rates. For each calibration, cross validations were pursued using the experimental data under operating conditions different from those used for calibrations. This hierarchical approach can be generally applied to develop validated device-scale CFD models for different absorption columns.« less

Device-scale CFD modeling of gas-liquid multiphase flow and amine absorption for CO 2 capture: Original Research Article: Device-scale CFD modeling of gas-liquid multiphase flow and amine absorption for CO 2 capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pan, Wenxiao; Galvin, Janine; Huang, Wei Ling

In this paper we aim to develop a validated device-scale CFD model that can predict quantitatively both hydrodynamics and CO 2 capture efficiency for an amine-based solvent absorber column with random Pall ring packing. A Eulerian porous-media approach and a two-fluid model were employed, in which the momentum and mass transfer equations were closed by literature-based empirical closure models. We proposed a hierarchical approach for calibrating the parameters in the closure models to make them accurate for the packed column. Specifically, a parameter for momentum transfer in the closure was first calibrated based on data from a single experiment. Withmore » this calibrated parameter, a parameter in the closure for mass transfer was next calibrated under a single operating condition. Last, the closure of the wetting area was calibrated for each gas velocity at three different liquid flow rates. For each calibration, cross validations were pursued using the experimental data under operating conditions different from those used for calibrations. This hierarchical approach can be generally applied to develop validated device-scale CFD models for different absorption columns.« less

Amidine-Functionalized Poly(2-vinyl-4,4-dimethylazlactone) for Selective and Efficient CO 2 Fixing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Barkakaty, Balaka; Browning, Katie L.; Sumpter, Bobby

Development of novel polymeric materials capable of efficient CO 2 capture and separation under ambient conditions is crucial for cost-effective and practical industrial applications. Here we report the facile synthesis of a new CO 2-responsive polymer through post-polymerization modification of poly(2 vinyl-4,4-dimethylazlactone) (PVDMA). The reactive pendant azlactone groups of PVDMA are easily modified with 4-(N-methyltetrahydropyrimidine) benzyl alcohol (PBA) without any by-product formation. FTIR and TGA experiments show the new PBA functionalized polymer powder can reversibly capture CO 2 at room temperature and under atmospheric pressure. CO2 capture was selective, showing a high fixing efficiency even with a mixed gas systemmore » (20% CO 2, 80% N 2) similar to flue gas. CO 2 release occurred at room temperature and release profiles were investigated as a function of temperature. Density Functional Theory (DFT) calculations coupled with modeling and simulation reveal the presence of two CO 2 binding sites in the PBA functionalized polymer resulting in a two-step CO 2 release at room temperature. Finally, we find that the ease of material preparation, high fixing efficiency, and robust release characteristics suggest that post-polymerization modification may be a useful route to designing new materials for CO 2 capture.« less

Amidine-Functionalized Poly(2-vinyl-4,4-dimethylazlactone) for Selective and Efficient CO 2 Fixing

DOE PAGES

Barkakaty, Balaka; Browning, Katie L.; Sumpter, Bobby; ...

2016-02-12

Development of novel polymeric materials capable of efficient CO 2 capture and separation under ambient conditions is crucial for cost-effective and practical industrial applications. Here we report the facile synthesis of a new CO 2-responsive polymer through post-polymerization modification of poly(2 vinyl-4,4-dimethylazlactone) (PVDMA). The reactive pendant azlactone groups of PVDMA are easily modified with 4-(N-methyltetrahydropyrimidine) benzyl alcohol (PBA) without any by-product formation. FTIR and TGA experiments show the new PBA functionalized polymer powder can reversibly capture CO 2 at room temperature and under atmospheric pressure. CO2 capture was selective, showing a high fixing efficiency even with a mixed gas systemmore » (20% CO 2, 80% N 2) similar to flue gas. CO 2 release occurred at room temperature and release profiles were investigated as a function of temperature. Density Functional Theory (DFT) calculations coupled with modeling and simulation reveal the presence of two CO 2 binding sites in the PBA functionalized polymer resulting in a two-step CO 2 release at room temperature. Finally, we find that the ease of material preparation, high fixing efficiency, and robust release characteristics suggest that post-polymerization modification may be a useful route to designing new materials for CO 2 capture.« less

Modeling and optimal design of CO2 Direct Air Capture systems in large arrays

NASA Astrophysics Data System (ADS)

Sadri Irani, Samaneh; Luzzatto-Fegiz, Paolo

2017-11-01

As noted by the 2014 IPCC report, while the rise in atmospheric CO2 would be slowed by emissions reductions, removing atmospheric CO2 is an important part of possible paths to climate stabilization. Direct Air Capture of CO2 with chemicals (DAC) is one of several proposed carbon capture technologies. There is an ongoing debate on whether DAC is an economically viable approach to alleviate climate change. In addition, like all air capture strategies, DAC is strongly constrained by the net-carbon problem, namely the need to control CO2 emissions associated with the capture process (for example, if DAC not powered by renewables). Research to date has focused on the chemistry and economics of individual DAC devices. However, the fluid mechanics of their large-scale deployment has not been examined in the literature, to the best of our knowledge. In this presentation, we develop a model for flow through an array of DAC devices, varying their lateral extent and their separation. We build on a recent theory of canopy flows, introducing terms for CO2 entrainment into the array boundary layer, and transport into the farm. In addition, we examine the possibility of driving flow passively by wind, thereby reducing energy consumption. The optimal operational design is established considering the total cost, drag force, energy consumption and total CO2 capture.

Novel Silica Nanostructured Platforms with Engineered Surface Functionality and Spherical Morphology for Low-Cost High-Efficiency Carbon Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lai, Cheng-Yu; Radu, Daniela R.; Pizzi, Nicholas

Carbon capture is an integral part of the CO 2 mitigation efforts, and encompasses, among other measures, the demonstration of effective and inexpensive CO 2 capture technologies. The project demonstrated a novel platform—the amine-functionalized stellate mesoporous silica nanosphere (MSN)—for effective CO 2 absorption. The reported CO 2 absorption data are superior to the performance of other reported silica matrices utilized for carbon capture, featuring an amount of over 4 milimoles CO 2/g sorbent at low temperatures (in the range of 30-45 ºC), selected for simulating the temperature of actual flue gas. The reported platform is highly resilient, showing recyclability andmore » 85 % mass conservation of sorbent upon nine tested cycles. Importantly, the stellate MSNs show high CO 2 selectivity at room temperature, indicating that the presence of nitrogen in flue gas will not impair the CO 2 absorption performance. The results could lead to a simple and inexpensive new technology for CO 2 mitigation which could be implemented as measure of CO 2 mitigation in current fossil-fuel burning plants in the form of solid sorbent.« less

Hyper-crosslinked cyclodextrin porous polymer: An efficient CO 2 capturing material with tunable porosity

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meng, Bo; Li, Haiyang; East China Univ. of Science and Technology, Shanghai

We designed and synthesized the cyclodextrin (CD)-based hyper-crosslinked porous polymers (HCPPs) for selective CO 2 adsorption and storage. We also explored the effect of monomer size on micropore formation, and determined a feasible way to tailor the porosity of the materials during the hyper-crosslinking process.

Hyper-crosslinked cyclodextrin porous polymer: An efficient CO 2 capturing material with tunable porosity

DOE PAGES

Meng, Bo; Li, Haiyang; East China Univ. of Science and Technology, Shanghai; ...

2016-11-11

We designed and synthesized the cyclodextrin (CD)-based hyper-crosslinked porous polymers (HCPPs) for selective CO 2 adsorption and storage. We also explored the effect of monomer size on micropore formation, and determined a feasible way to tailor the porosity of the materials during the hyper-crosslinking process.

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.

The Inherent Tracer Fingerprint of Captured CO2

NASA Astrophysics Data System (ADS)

Flude, Stephanie; Gyore, Domokos; Stuart, Finlay; Boyce, Adrian; Haszeldine, Stuart; Chalaturnyk, Rick; Gilfillan, Stuart

2017-04-01

Inherent tracers, the isotopic and trace gas composition of captured CO2 streams, are potentially powerful tracers for use in CCS technology [1,2]. Despite this potential, the inherent tracer fingerprint in captured CO2 streams has yet to be robustly investigated and documented [3]. Here, we will present the first high quality systematic measurements of the carbon and oxygen isotopic and noble gas fingerprints measured in anthropogenic CO2 captured from combustion power stations and fertiliser plants, using amine capture, oxyfuel and gasification processes, and derived from coal, biomass and natural gas feedstocks. We will show that δ13C values are mostly controlled by the feedstock composition, as expected. The majority of the CO2 samples exhibit δ18O values similar to atmospheric O2 although captured CO2 samples from biomass and gas feedstocks at one location in the UK are significantly higher. Our measured noble gas concentrations in captured CO2 are generally as expected [2], typically being two orders of magnitude lower in concentration than in atmospheric air. Relative noble gas elemental abundances are variable and often show an opposite trend to that of a water in contact with the atmosphere. Expected enrichments in radiogenic noble gases (4He and 40Ar) for fossil fuel derived CO2 were not always observed due to dilution with atmospheric noble gases during the CO2 generation and capture process. Many noble gas isotope ratios indicate that isotopic fractionation takes place during the CO2 generation and capture processes, resulting in isotope ratios similar to fractionated air. We conclude that phase changes associated with CO2 transport and sampling may induce noble gas elemental and isotopic fractionation, due to different noble gas solubilities between high (liquid or supercritical) and low (gaseous) density CO2. Data from the Australian CO2CRC Otway test site show that δ13C of CO2 will change once injected into the storage reservoir, but that this change is small and can be quantitatively modelled in order to determine the proportion of CO2 that has dissolved into the formation waters. Furthermore, noble gas data from the Otway storage reservoir post-injection, shows evidence of noble gas stripping of formation water and contamination with Kr and Xe related to an earlier injection experiment. Importantly, He data from SaskPower's Aquistore illustrates that injected CO2 will inherit distinctive crustal radiogenic noble gas fingerprints from the subsurface once injected into an undisturbed geological storage reservoir, meaning this could be used to identify unplanned migration of the CO2 to the surface and shallow subsurface [4]. References [1] Mayer et al., (2015) IJGGC, Vol. 37, 46-60 http://dx.doi.org/10.1016/j.ijggc.2015.02.021 [2] Gilfillan et al., (2014) Energy Procedia, Vol. 63, 4123-4133 http://dx.doi.org/10.1016/j.egypro.2014.11.443 [3] Flude et al., (2016) Environ. Sci. Technol., 50 (15), pp 7939-7955 DOI: 10.1021/acs.est.6b01548 [4] Gilfillan et al., (2011) IJGGC, Vol. 5 (6) 1507-1516 http://dx.doi.org/10.1016/j.ijggc.2011.08.008

The cost of carbon capture and storage for natural gas combined cycle power plants.

PubMed

Rubin, Edward S; Zhai, Haibo

2012-03-20

This paper examines the cost of CO(2) capture and storage (CCS) for natural gas combined cycle (NGCC) power plants. Existing studies employ a broad range of assumptions and lack a consistent costing method. This study takes a more systematic approach to analyze plants with an amine-based postcombustion CCS system with 90% CO(2) capture. We employ sensitivity analyses together with a probabilistic analysis to quantify costs for plants with and without CCS under uncertainty or variability in key parameters. Results for new baseload plants indicate a likely increase in levelized cost of electricity (LCOE) of $20-32/MWh (constant 2007$) or $22-40/MWh in current dollars. A risk premium for plants with CCS increases these ranges to $23-39/MWh and $25-46/MWh, respectively. Based on current cost estimates, our analysis further shows that a policy to encourage CCS at new NGCC plants via an emission tax or carbon price requires (at 95% confidence) a price of at least $125/t CO(2) to ensure NGCC-CCS is cheaper than a plant without CCS. Higher costs are found for nonbaseload plants and CCS retrofits.

Thermal degradation of aqueous 2-aminoethylethanolamine in CO2 capture; identification of degradation products, reaction mechanisms and computational studies.

PubMed

Saeed, Idris Mohamed; Lee, Vannajan Sanghiran; Mazari, Shaukat Ali; Si Ali, B; Basirun, Wan Jeffrey; Asghar, Anam; Ghalib, Lubna; Jan, Badrul Mohamed

2017-01-01

Amine degradation is the main significant problems in amine-based post-combustion CO 2 capture, causes foaming, increase in viscosity, corrosion, fouling as well as environmental issues. Therefore it is very important to develop the most efficient solvent with high thermal and chemical stability. This study investigated thermal degradation of aqueous 30% 2-aminoethylethanolamine (AEEA) using 316 stainless steel cylinders in the presence and absence of CO 2 for 4 weeks. The degradation products were identified by gas chromatography mass spectrometry (GC/MS) and liquid chromatography-time-of-flight-mass spectrometry (LC-QTOF/MS). The results showed AEEA is stable in the absence of CO 2 , while in the presence of CO 2 AEEA showed to be very unstable and numbers of degradation products were identified. 1-(2-Hydroxyethyl)-2-imidazolidinone (HEIA) was the most abundance degradation product. A possible mechanism for the thermal degradation of AEEA has been developed to explain the formation of degradation products. In addition, the reaction energy of formation of the most abundance degradation product HEIA was calculated using quantum mechanical calculation.

Engineered yeast for enhanced CO2 mineralization†

PubMed Central

Barbero, Roberto; Carnelli, Lino; Simon, Anna; Kao, Albert; Monforte, Alessandra d’Arminio; Riccò, Moreno; Bianchi, Daniele; Belcher, Angela

2014-01-01

In this work, a biologically catalyzed CO2 mineralization process for the capture of CO2 from point sources was designed, constructed at a laboratory scale, and, using standard chemical process scale-up protocols, was modeled and evaluated at an industrial scale. A yeast display system in Saccharomyces cerevisae was used to screen several carbonic anhydrase isoforms and mineralization peptides for their impact on CO2 hydration, CaCO3 mineralization, and particle settling rate. Enhanced rates for each of these steps in the CaCO3 mineralization process were confirmed using quantitative techniques in lab-scale measurements. The effect of these enhanced rates on the CO2 capture cost in an industrial scale CO2 mineralization process using coal fly ash as the CaO source was evaluated. The model predicts a process using bCA2- yeast and fly ash is ~10% more cost effective per ton of CO2 captured than a process with no biological molecules, a savings not realized by wild-type yeast and high-temperature stable recombinant CA2 alone or in combination. The levelized cost of electricity for a power plant using this process was calculated and scenarios in which this process compares favorably to CO2 capture by MEA absorption process are presented. PMID:25289021

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chance, Ronald; Koros, William J.; McCool, Benjamin

The invention provides systems and methods for the delivery of carbon to photoautotrophs. The invention utilizes low energy regeneration of adsorbent for CO.sub.2 capture and provides for effective CO.sub.2 loading into liquids useful for photoautotroph growth and/or production of photosynthetic products, such as biofuels, via photoautotrophic culture media. The inventive system comprises a fluid/membrane/fluid contactor that provides selective transfer of molecular CO.sub.2 via a dense (non-porous) membrane from a carbonate-based CO.sub.2 snipping solution to a culture medium where the CO.sub.2 is consumed by a photoautotroph for the production of biofuels, biofuel precursors or other commercial products.

Developing a Comprehensive Risk Assessment Framework for Geological Storage CO 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Duncan, Ian

2014-08-31

The operational risks for CCS projects include: risks of capturing, compressing, transporting and injecting CO₂; risks of well blowouts; risk that CO 2 will leak into shallow aquifers and contaminate potable water; and risk that sequestered CO 2 will leak into the atmosphere. This report examines these risks by using information on the risks associated with analogue activities such as CO 2 based enhanced oil recovery (CO 2-EOR), natural gas storage and acid gas disposal. We have developed a new analysis of pipeline risk based on Bayesian statistical analysis. Bayesian theory probabilities may describe states of partial knowledge, even perhapsmore » those related to non-repeatable events. The Bayesian approach enables both utilizing existing data and at the same time having the capability to adsorb new information thus to lower uncertainty in our understanding of complex systems. Incident rates for both natural gas and CO 2 pipelines have been widely used in papers and reports on risk of CO 2 pipelines as proxies for the individual risk created by such pipelines. Published risk studies of CO 2 pipelines suggest that the individual risk associated with CO2 pipelines is between 10 -3 and 10 -4, which reflects risk levels approaching those of mountain climbing, which many would find unacceptably high. This report concludes, based on a careful analysis of natural gas pipeline failures, suggests that the individual risk of CO 2 pipelines is likely in the range of 10-6 to 10-7, a risk range considered in the acceptable to negligible range in most countries. If, as is commonly thought, pipelines represent the highest risk component of CCS outside of the capture plant, then this conclusion suggests that most (if not all) previous quantitative- risk assessments of components of CCS may be orders of magnitude to high. The potential lethality of unexpected CO 2 releases from pipelines or wells are arguably the highest risk aspects of CO 2 enhanced oil recovery (CO2-EOR), carbon capture, and storage (CCS). Assertions in the CCS literature, that CO 2 levels of 10% for ten minutes, or 20 to 30% for a few minutes are lethal to humans, are not supported by the available evidence. The results of published experiments with animals exposed to CO 2, from mice to monkeys, at both normal and depleted oxygen levels, suggest that lethal levels of CO 2 toxicity are in the range 50 to 60%. These experiments demonstrate that CO 2 does not kill by asphyxia, but rather is toxic at high concentrations. It is concluded that quantitative risk assessments of CCS have overestimated the risk of fatalities by using values of lethality a factor two to six lower than the values estimated in this paper. In many dispersion models of CO 2 releases from pipelines, no fatalities would be predicted if appropriate levels of lethality for CO 2 had been used in the analysis.« less

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.

Bench Scale Process for Low Cost CO2 Capture Using a Phase-Changing Absorbent: Topical Report EH&S Risk Assessment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Westendorf, Tiffany; Farnum, Rachel; Perry, Robert

2016-05-11

GE Global Research was contracted by the Department of Energy to design and build a bench-scale process for a novel phase-changing aminosilicone-based CO2 capture solvent (award number DEFE0013687). As part of this program, a technology EH&S assessment (Subtask 5.1) has been completed for a CO2 capture system for a 550 MW coal-fired power plant. The assessment focuses on two chemicals used in the process, the aminosilicone solvent, GAP-0, and dodecylbenzenesulfonic acid (DDBSA), the GAP-0 carbamate formed upon reaction of the GAP-0 with CO2, and two potential byproducts formed in the process, GAP-0/SOx salts and amine-terminated, urea-containing silicone (also referred tomore » as “ureas” in this report). The EH&S assessment identifies and estimates the magnitude of the potential air and water emissions and solid waste generated by the process and reviews the toxicological profiles of the chemicals associated with the process. Details regarding regulatory requirements, engineering controls, and storage and handling procedures are also provided in the following sections.« less

Rational design of a low-cost, high-performance metal–organic framework for hydrogen storage and carbon capture

DOE PAGES

Witman, Matthew; Ling, Sanliang; Gladysiak, Andrzej; ...

2016-12-16

Here, we present the in silico design of a MOF-74 analogue, hereon known as M 2(DHFUMA) [M = Mg, Fe, Co, Ni, Zn], with enhanced small-molecule adsorption properties over the original M 2(DOBDC) series. Constructed from 2,3-dihydroxyfumarate (DHFUMA), an aliphatic ligand which is smaller than the aromatic 2,5-dioxidobenzene-1,4-dicarboxylate (DOBDC), the M 2(DHFUMA) framework has a reduced channel diameter, resulting in higher volumetric density of open metal sites and significantly improved volumetric hydrogen (H 2) storage potential. Furthermore, the reduced distance between two adjacent open metal sites in the pore channel leads to a CO 2 binding mode of one moleculemore » per two adjacent metals with markedly stronger binding energetics. Through dispersion-corrected density functional theory (DFT) calculations of guest–framework interactions and classical simulation of the adsorption behavior of binary CO 2:H 2O mixtures, we theoretically predict the M 2(DHFUMA) series as an improved alternative for carbon capture over the M 2(DOBDC) series when adsorbing from wet flue gas streams. The improved CO 2 uptake and humidity tolerance in our simulations is tunable based upon metal selection and adsorption temperature which, combined with the significantly reduced ligand expense, elevates this material’s potential for CO 2 capture and H 2 storage. The dynamical and elastic stabilities of Mg 2(DHFUMA) were verified by hybrid DFT calculations, demonstrating its significant potential for experimental synthesis.« less

Rational Design of a Low-Cost, High-Performance Metal–Organic Framework for Hydrogen Storage and Carbon Capture

PubMed Central

2016-01-01

We present the in silico design of a MOF-74 analogue, hereon known as M2(DHFUMA) [M = Mg, Fe, Co, Ni, Zn], with enhanced small-molecule adsorption properties over the original M2(DOBDC) series. Constructed from 2,3-dihydroxyfumarate (DHFUMA), an aliphatic ligand which is smaller than the aromatic 2,5-dioxidobenzene-1,4-dicarboxylate (DOBDC), the M2(DHFUMA) framework has a reduced channel diameter, resulting in higher volumetric density of open metal sites and significantly improved volumetric hydrogen (H2) storage potential. Furthermore, the reduced distance between two adjacent open metal sites in the pore channel leads to a CO2 binding mode of one molecule per two adjacent metals with markedly stronger binding energetics. Through dispersion-corrected density functional theory (DFT) calculations of guest–framework interactions and classical simulation of the adsorption behavior of binary CO2:H2O mixtures, we theoretically predict the M2(DHFUMA) series as an improved alternative for carbon capture over the M2(DOBDC) series when adsorbing from wet flue gas streams. The improved CO2 uptake and humidity tolerance in our simulations is tunable based upon metal selection and adsorption temperature which, combined with the significantly reduced ligand expense, elevates this material’s potential for CO2 capture and H2 storage. The dynamical and elastic stabilities of Mg2(DHFUMA) were verified by hybrid DFT calculations, demonstrating its significant potential for experimental synthesis. PMID:28127415

Synthesis of Size-Tunable CO2-Philic Imprinted Polymeric Particles (MIPs) for Low-Pressure CO2 Capture Using Oil-in-Oil Suspension Polymerization.

PubMed

Nabavi, Seyed Ali; Vladisavljević, Goran T; Zhu, Yidi; Manović, Vasilije

2017-10-03

Highly selective molecularly imprinted poly[acrylamide-co-(ethylene glycol dimethacrylate)] polymer particles (MIPs) for CO 2 capture were synthesized by suspension polymerization via oil-in-oil emulsion. Creation of CO 2 -philic, amide-decorated cavities in the polymer matrix led to a high affinity to CO 2 . At 0.15 bar CO 2 partial pressure, the CO 2 /N 2 selectivity was 49 (corresponding to 91% purity of the gas stream after regeneration), and reached 97 at ultralow CO 2 partial pressures. The imprinted polymers showed considerably higher CO 2 uptakes compared to their nonimprinted counterparts, and the maximum equilibrium CO 2 capture capacity of 1.1 mmol g -1 was achieved at 273 K. The heat of adsorption was below 32 kJ mol -1 and the temperature of onset of intense thermal degradation was 351-376 °C. An increase in monomer-to-cross-linker molar ratio in the dispersed phase up to 1:2.5 led to a higher affinity toward CO 2 due to higher density of selective amide groups in the polymer network. MIPs are a promising option for industrial packed and fluidized bed CO 2 capture systems due to large particles with a diameter up to 1200 μm and irregular oblong shapes formed due to arrested coalescence during polymerization, occurring as a result of internal elasticity of the partially polymerized semisolid drops.

Carbon dioxide (CO2) sequestration in deep saline aquifers and formations: Chapter 3

USGS Publications Warehouse

Rosenbauer, Robert J.; Thomas, Burt

2010-01-01

Carbon dioxide (CO2) capture and sequestration in geologic media is one among many emerging strategies to reduce atmospheric emissions of anthropogenic CO2. This chapter looks at the potential of deep saline aquifers – based on their capacity and close proximity to large point sources of CO2 – as repositories for the geologic sequestration of CO2. The petrochemical characteristics which impact on the suitability of saline aquifers for CO2 sequestration and the role of coupled geochemical transport models and numerical tools in evaluating site feasibility are also examined. The full-scale commercial CO2 sequestration project at Sleipner is described together with ongoing pilot and demonstration projects.

Bottleneck Effect of N,N-Dimethylformamide in InOF-1: Increasing CO2 Capture in Porous Coordination Polymers.

PubMed

Sánchez-González, Elí; González-Zamora, Eduardo; Martínez-Otero, Diego; Jancik, Vojtech; Ibarra, Ilich A

2017-05-15

The bottleneck effect of confined N,N-dimethylformamide (DMF) molecules was observed in InOF-1 for the first time: CO 2 capture was remarkably enhanced in samples of as-synthesized InOF-1, thermally activated in such a way that a small residual amount of DMF molecules remained confined within the pores (DMF@InOF-1). Dynamic CO 2 adsorption experiments on DMF@InOF-1 exhibited a CO 2 capture of 8.06 wt % [1.5-fold higher than that of a fully activated InOF-1 (5.24%)]. DMF@InOF-1 can reversibly adsorb/desorb 8.09% CO 2 with no loss of CO 2 capacity after 10 cycles, and the desorption is accomplished by only turning the CO 2 flow off. Static CO 2 adsorption experiments (at 196 K) demonstrated a 1.4-fold CO 2 capture increase (from 5.5 mmol·g -1 , fully activated InOF-1, to 7.5 mmol·g -1 , DMF@InOF-1). Therefore, these CO 2 capture properties are the result of the presence of residual-confined DMF molecules within the InOF-1 framework and their interactions via a very strong hydrogen bond with the In 2 (μ-OH) groups, which prevent DMF leaching. The stability of this hydrogen bond is given by a perfect fit of the DMF molecule in the "dent" around the OH group that allows a nearly ideal orientation of the DMF molecule towards the OH group.

Regenerable sorbent technique for capturing CO.sub.2 using immobilized amine sorbents

DOEpatents

Pennline, Henry W; Hoffman, James S; Gray, McMahan L; Fauth, Daniel J; Resnik, Kevin P

2013-08-06

The disclosure provides a CO.sub.2 absorption method using an amine-based solid sorbent for the removal of carbon dioxide from a gas stream. The method disclosed mitigates the impact of water loading on regeneration by utilizing a conditioner following the steam regeneration process, providing for a water loading on the amine-based solid sorbent following CO.sub.2 absorption substantially equivalent to the moisture loading of the regeneration process. This assists in optimizing the CO.sub.2 removal capacity of the amine-based solid sorbent for a given absorption and regeneration reactor size. Management of the water loading in this manner allows regeneration reactor operation with significant mitigation of energy losses incurred by the necessary desorption of adsorbed water.

The catalytic effect of H2O on the hydrolysis of CO32- in hydrated clusters and its implication in the humidity driven CO2 air capture.

PubMed

Xiao, Hang; Shi, Xiaoyang; Zhang, Yayun; Liao, Xiangbiao; Hao, Feng; Lackner, Klaus S; Chen, Xi

2017-10-18

The hydration of ions in nanoscale hydrated clusters is ubiquitous and essential in many physical and chemical processes. Here we show that the hydrolysis reaction is strongly affected by relative humidity. The hydrolysis of CO 3 2- with n = 1-8 water molecules is investigated using an ab initio method. For n = 1-5 water molecules, all the reactants follow a stepwise pathway to the transition state. For n = 6-8 water molecules, all the reactants undergo a direct proton transfer to the transition state with overall lower activation free energy. The activation free energy of the reaction is dramatically reduced from 10.4 to 2.4 kcal mol -1 as the number of water molecules increases from 1 to 6. Meanwhile, the degree of hydrolysis of CO 3 2- is significantly increased compared to the bulk water solution scenario. Incomplete hydration shells facilitate the hydrolysis of CO 3 2- with few water molecules to be not only thermodynamically favorable but also kinetically favorable. We showed that the chemical kinetics is not likely to constrain the speed of CO 2 air capture driven by the humidity-swing. Instead, the pore-diffusion of ions is expected to be the time-limiting step in the humidity driven CO 2 air capture. The effect of humidity on the speed of CO 2 air capture was studied by conducting a CO 2 absorption experiment using IER with a high ratio of CO 3 2- to H 2 O molecules. Our result is able to provide valuable insights into designing efficient CO 2 air-capture sorbents.

The Methanol Economy Project

DOE Office of Scientific and Technical Information (OSTI.GOV)

Olah, George; Prakash, G. K.

2014-02-01

The Methanol Economy Project is based on the concept of replacing fossil fuels with methanol generated either from renewable resources or abundant natural (shale) gas. The full methanol cycle was investigated in this project, from production of methanol through bromination of methane, bireforming of methane to syngas, CO 2 capture using supported amines, co-electrolysis of CO 2 and water to formate and syngas, decomposition of formate to CO 2 and H 2, and use of formic acid in a direct formic acid fuel cell. Each of these projects achieved milestones and provided new insights into their respective fields.

Promoting Ethylene Selectivity from CO2 Electroreduction on CuO Supported onto CO2 Capture Materials.

PubMed

Yang, Hui-Juan; Yang, Hong; Hong, Yu-Hao; Zhang, Peng-Yang; Wang, Tao; Chen, Li-Na; Zhang, Feng-Yang; Wu, Qi-Hui; Tian, Na; Zhou, Zhi-You; Sun, Shi-Gang

2018-03-09

Cu is a unique catalyst for CO 2 electroreduction, since it can catalyze CO 2 reduction to a series of hydrocarbons, alcohols, and carboxylic acids. Nevertheless, such Cu catalysts suffer from poor selectivity. High pressure of CO 2 is considered to facilitate the activity and selectivity of CO 2 reduction. Herein, a new strategy is presented for CO 2 reduction with improved C 2 H 4 selectivity on a Cu catalyst by using CO 2 capture materials as the support at ambient pressure. N-doped carbon (N x C) was synthesized through high-temperature carbonization of melamine and l-lysine. We observed that the CO 2 uptake capacity of N x C depends on both the microporous area and the content of pyridinic N species, which can be controlled by the carbonization temperature (600-800 °C). The as-prepared CuO/N x C catalysts exhibit a considerably higher C 2 H 4 faradaic efficiency (36 %) than CuO supported on XC-72 carbon black (19 %), or unsupported CuO (20 %). Moreover, there is a good linear relationship between the C 2 H 4 faradaic efficiency and CO 2 uptake capacity of the supports for CuO. The local high CO 2 concentration near Cu catalysts, created by CO 2 capture materials, was proposed to increase the coverage of CO intermediate, which is favorable for the coupling of two CO units in the formation of C 2 H 4 . This study demonstrates that pairing Cu catalysts with CO 2 capture supports is a promising approach for designing highly effective CO 2 reduction electrocatalysts. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

The cost of getting CCS wrong: Uncertainty, infrastructure design, and stranded CO 2

DOE PAGES

Middleton, Richard Stephen; Yaw, Sean Patrick

2018-01-11

Carbon capture, and storage (CCS) infrastructure will require industry—such as fossil-fuel power, ethanol production, and oil and gas extraction—to make massive investment in infrastructure. The cost of getting these investments wrong will be substantial and will impact the success of CCS technology. Multiple factors can and will impact the success of commercial-scale CCS, including significant uncertainties regarding capture, transport, and injection-storage decisions. Uncertainties throughout the CCS supply chain include policy, technology, engineering performance, economics, and market forces. In particular, large uncertainties exist for the injection and storage of CO 2. Even taking into account upfront investment in site characterization, themore » final performance of the storage phase is largely unknown until commercial-scale injection has started. We explore and quantify the impact of getting CCS infrastructure decisions wrong based on uncertain injection rates and uncertain CO 2 storage capacities using a case study managing CO 2 emissions from the Canadian oil sands industry in Alberta. We use SimCCS, a widely used CCS infrastructure design framework, to develop multiple CCS infrastructure scenarios. Each scenario consists of a CCS infrastructure network that connects CO 2 sources (oil sands extraction and processing) with CO 2 storage reservoirs (acid gas storage reservoirs) using a dedicated CO 2 pipeline network. Each scenario is analyzed under a range of uncertain storage estimates and infrastructure performance is assessed and quantified in terms of cost to build additional infrastructure to store all CO 2. We also include the role of stranded CO 2, CO 2 that a source was expecting to but cannot capture due substandard performance in the transport and storage infrastructure. Results show that the cost of getting the original infrastructure design wrong are significant and that comprehensive planning will be required to ensure that CCS becomes a successful climate mitigation technology. Here, we show that the concept of stranded CO 2 can transform a seemingly high-performing infrastructure design into the worst case scenario.« less

The cost of getting CCS wrong: Uncertainty, infrastructure design, and stranded CO 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Middleton, Richard Stephen; Yaw, Sean Patrick

Carbon capture, and storage (CCS) infrastructure will require industry—such as fossil-fuel power, ethanol production, and oil and gas extraction—to make massive investment in infrastructure. The cost of getting these investments wrong will be substantial and will impact the success of CCS technology. Multiple factors can and will impact the success of commercial-scale CCS, including significant uncertainties regarding capture, transport, and injection-storage decisions. Uncertainties throughout the CCS supply chain include policy, technology, engineering performance, economics, and market forces. In particular, large uncertainties exist for the injection and storage of CO 2. Even taking into account upfront investment in site characterization, themore » final performance of the storage phase is largely unknown until commercial-scale injection has started. We explore and quantify the impact of getting CCS infrastructure decisions wrong based on uncertain injection rates and uncertain CO 2 storage capacities using a case study managing CO 2 emissions from the Canadian oil sands industry in Alberta. We use SimCCS, a widely used CCS infrastructure design framework, to develop multiple CCS infrastructure scenarios. Each scenario consists of a CCS infrastructure network that connects CO 2 sources (oil sands extraction and processing) with CO 2 storage reservoirs (acid gas storage reservoirs) using a dedicated CO 2 pipeline network. Each scenario is analyzed under a range of uncertain storage estimates and infrastructure performance is assessed and quantified in terms of cost to build additional infrastructure to store all CO 2. We also include the role of stranded CO 2, CO 2 that a source was expecting to but cannot capture due substandard performance in the transport and storage infrastructure. Results show that the cost of getting the original infrastructure design wrong are significant and that comprehensive planning will be required to ensure that CCS becomes a successful climate mitigation technology. Here, we show that the concept of stranded CO 2 can transform a seemingly high-performing infrastructure design into the worst case scenario.« less

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

USDA-ARS?s Scientific Manuscript database

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

Particle-scale CO2 adsorption kinetics modeling considering three reaction mechanisms

DOE Office of Scientific and Technical Information (OSTI.GOV)

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, causedmore » 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.« less

Influence of high-temperature steam on the reactivity of CaO sorbent for CO₂ capture.

PubMed

Donat, Felix; Florin, Nicholas H; Anthony, Edward J; Fennell, Paul S

2012-01-17

Calcium looping is a high-temperature CO(2) capture technology applicable to the postcombustion capture of CO(2) from power station flue gas, or integrated with fuel conversion in precombustion CO(2) capture schemes. The capture technology uses solid CaO sorbent derived from natural limestone and takes advantage of the reversible reaction between CaO and CO(2) to form CaCO(3); that is, to achieve the separation of CO(2) from flue or fuel gas, and produce a pure stream of CO(2) suitable for geological storage. An important characteristic of the sorbent, affecting the cost-efficiency of this technology, is the decay in reactivity of the sorbent over multiple CO(2) capture-and-release cycles. This work reports on the influence of high-temperature steam, which will be present in flue (about 5-10%) and fuel (∼20%) gases, on the reactivity of CaO sorbent derived from four natural limestones. A significant increase in the reactivity of these sorbents was found for 30 cycles in the presence of steam (from 1-20%). Steam influences the sorbent reactivity in two ways. Steam present during calcination promotes sintering that produces a sorbent morphology with most of the pore volume associated with larger pores of ∼50 nm in diameter, and which appears to be relatively more stable than the pore structure that evolves when no steam is present. The presence of steam during carbonation reduces the diffusion resistance during carbonation. We observed a synergistic effect, i.e., the highest reactivity was observed when steam was present for both calcination and carbonation.

Computational Modeling of the Geologic Sequestration of Carbon Dioxide

EPA Science Inventory

Geologic sequestration of CO2 is a component of C capture and storage (CCS), an emerging technology for reducing CO2 emissions to the atmosphere, and involves injection of captured CO2 into deep subsurface formations. Similar to the injection of hazardous wastes, before injection...

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

PubMed Central

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

2016-01-01

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

Near-Zero Emissions Oxy-Combustion Flue Gas Purification

DOE Office of Scientific and Technical Information (OSTI.GOV)

Minish Shah; Nich Degenstein; Monica Zanfir

2012-06-30

The objectives of this project were to carry out an experimental program to enable development and design of near zero emissions (NZE) CO{sub 2} processing unit (CPU) for oxy-combustion plants burning high and low sulfur coals and to perform commercial viability assessment. The NZE CPU was proposed to produce high purity CO{sub 2} from the oxycombustion flue gas, to achieve > 95% CO{sub 2} capture rate and to achieve near zero atmospheric emissions of criteria pollutants. Two SOx/NOx removal technologies were proposed depending on the SOx levels in the flue gas. The activated carbon process was proposed for power plantsmore » burning low sulfur coal and the sulfuric acid process was proposed for power plants burning high sulfur coal. For plants burning high sulfur coal, the sulfuric acid process would convert SOx and NOx in to commercial grade sulfuric and nitric acid by-products, thus reducing operating costs associated with SOx/NOx removal. For plants burning low sulfur coal, investment in separate FGD and SCR equipment for producing high purity CO{sub 2} would not be needed. To achieve high CO{sub 2} capture rates, a hybrid process that combines cold box and VPSA (vacuum pressure swing adsorption) was proposed. In the proposed hybrid process, up to 90% of CO{sub 2} in the cold box vent stream would be recovered by CO{sub 2} VPSA and then it would be recycled and mixed with the flue gas stream upstream of the compressor. The overall recovery from the process will be > 95%. The activated carbon process was able to achieve simultaneous SOx and NOx removal in a single step. The removal efficiencies were >99.9% for SOx and >98% for NOx, thus exceeding the performance targets of >99% and >95%, respectively. The process was also found to be suitable for power plants burning both low and high sulfur coals. Sulfuric acid process did not meet the performance expectations. Although it could achieve high SOx (>99%) and NOx (>90%) removal efficiencies, it could not produce by-product sulfuric and nitric acids that meet the commercial product specifications. The sulfuric acid will have to be disposed of by neutralization, thus lowering the value of the technology to same level as that of the activated carbon process. Therefore, it was decided to discontinue any further efforts on sulfuric acid process. Because of encouraging results on the activated carbon process, it was decided to add a new subtask on testing this process in a dual bed continuous unit. A 40 days long continuous operation test confirmed the excellent SOx/NOx removal efficiencies achieved in the batch operation. This test also indicated the need for further efforts on optimization of adsorption-regeneration cycle to maintain long term activity of activated carbon material at a higher level. The VPSA process was tested in a pilot unit. It achieved CO{sub 2} recovery of > 95% and CO{sub 2} purity of >80% (by vol.) from simulated cold box feed streams. The overall CO{sub 2} recovery from the cold box VPSA hybrid process was projected to be >99% for plants with low air ingress (2%) and >97% for plants with high air ingress (10%). Economic analysis was performed to assess value of the NZE CPU. The advantage of NZE CPU over conventional CPU is only apparent when CO{sub 2} capture and avoided costs are compared. For greenfield plants, cost of avoided CO{sub 2} and cost of captured CO{sub 2} are generally about 11-14% lower using the NZE CPU compared to using a conventional CPU. For older plants with high air intrusion, the cost of avoided CO{sub 2} and capture CO{sub 2} are about 18-24% lower using the NZE CPU. Lower capture costs for NZE CPU are due to lower capital investment in FGD/SCR and higher CO{sub 2} capture efficiency. In summary, as a result of this project, we now have developed one technology option for NZE CPU based on the activated carbon process and coldbox-VPSA hybrid process. This technology is projected to work for both low and high sulfur coal plants. The NZE CPU technology is projected to achieve near zero stack emissions, produce high purity CO{sub 2} relatively free of trace impurities and achieve ~99% CO{sub 2} capture rate while lowering the CO{sub 2} capture costs.« less

Integrating Algae with Bioenergy Carbon Capture and Storage (ABECCS) Increases Sustainability

NASA Astrophysics Data System (ADS)

Beal, Colin M.; Archibald, Ian; Huntley, Mark E.; Greene, Charles H.; Johnson, Zackary I.

2018-03-01

Bioenergy carbon capture and storage (BECCS) has been proposed to reduce atmospheric CO2 concentrations, but concerns remain about competition for arable land and freshwater. The synergistic integration of algae production, which does not require arable land or freshwater, with BECCS (called "ABECCS") can reduce CO2 emissions without competing with agriculture. This study presents a technoeconomic and life-cycle assessment for colocating a 121-ha algae facility with a 2,680-ha eucalyptus forest for BECCS. The eucalyptus biomass fuels combined heat and power (CHP) generation with subsequent amine-based carbon capture and storage (CCS). A portion of the captured CO2 is used for growing algae and the remainder is sequestered. Biomass combustion supplies CO2, heat, and electricity, thus increasing the range of sites suitable for algae cultivation. Economic, energetic, and environmental impacts are considered. The system yields as much protein as soybeans while generating 61.5 TJ of electricity and sequestering 29,600 t of CO2 per year. More energy is generated than consumed and the freshwater footprint is roughly equal to that for soybeans. Financial break-even is achieved for product value combinations that include 1) algal biomass sold for 1,400/t (fishmeal replacement) with a 68/t carbon credit and 2) algal biomass sold for 600/t (soymeal replacement) with a 278/t carbon credit. Sensitivity analysis shows significant reductions to the cost of carbon sequestration are possible. The ABECCS system represents a unique technology for negative emissions without reducing protein production or increasing water demand, and should therefore be included in the suite of technologies being considered to address global sustainability.

Carbon dioxide capture using Sodium bicarbonate/Sodium carbonate supported on nanoporous Iron(III) oxide

NASA Astrophysics Data System (ADS)

Dutcher, Bryce

Strong evidence exists suggesting that anthropogenic emissions of CO 2, primarily from the combustion of fossil fuels, have been contributing to global climate change, including warming of the atmosphere and acidification of the oceans. These, in turn, lead to other effects such as melting of ice and snow cover, rising sea levels, severe weather patterns, and extinction of life forms. With these detrimental shifts in ecosystems already being observed, it becomes imperative to mitigate anthropogenic CO2. CO2 capture is typically a costly operation, usually due to the energy required for regeneration of the capture medium. Na2CO3 is one potential capture medium with the potential to decrease this energy requirement. Extensively researched as a potential sorbent for CO2, Na2CO3 is well known for its theoretically low energy requirement, due largely to its relatively low heat of reaction compared to other capture technologies. Its primary pitfalls, however, are its extremely low reaction rate during sorption and slow regeneration of Na2CO 3. Before Na2CO3 can be used as a CO2 sorbent, then, it is critical to increase its reaction rate. In order to do so, this project studied nanoporous FeOOH as a potential supporting material for Na2CO3. Because regeneration of the sorbent is the most energy-intensive step when using Na2CO3 for CO 2 sorption, this project focused on the decomposition of NaHCO 3, which is equivalent to CO2 desorption. Using BET, FTIR, XRD, XPS, SEM, TEM, magnetic susceptibility tests, and Mossbauer spectroscopy, we show FeOOH to be thermally stable both with and without the presence of NaHCO3 at temperatures necessary for sorption and regeneration, up to about 200°C. More significantly, we observe that FeOOH not only increases the surface area of NaHCO3, but also has a catalytic effect on the decomposition of NaHCO3, reducing activation energy from 80 kJ/mol to 44 kJ/mol. This reduction in activation energy leads to a significant increase in the reaction rate by a factor of nearly 50, which could translate into a substantial decrease in the cost of using Na2 CO3 for CO2 capture.

Pilot testing of a membrane system for postcombustion CO 2 capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Merkel, Tim; Kniep, Jay; Wei, Xiaotong

2015-09-30

This final report summarizes work conducted for the U.S. Department of Energy, National Energy Technology Laboratory (DOE) to scale up an efficient post-combustion CO 2 capture membrane process to the small pilot test stage (award number DE-FE0005795). The primary goal of this research program was to design, fabricate, and operate a membrane CO 2 capture system to treat coal-derived flue gas containing 20 tonnes CO 2/day (20 TPD). Membrane Technology and Research (MTR) conducted this project in collaboration with Babcock and Wilcox (B&W), the Electric Power Research Institute (EPRI), WorleyParsons (WP), the Illinois Sustainable Technology Center (ISTC), Enerkem (EK), andmore » the National Carbon Capture Center (NCCC). In addition to the small pilot design, build and slipstream testing at NCCC, other project efforts included laboratory membrane and module development at MTR, validation field testing on a 1 TPD membrane system at NCCC, boiler modeling and testing at B&W, a techno-economic analysis (TEA) by EPRI/WP, a case study of the membrane technology applied to a ~20 MWe power plant by ISTC, and an industrial CO 2 capture test at an Enerkem waste-to-biofuel facility. The 20 TPD small pilot membrane system built in this project successfully completed over 1,000 hours of operation treating flue gas at NCCC. The Polaris™ membranes used on this system demonstrated stable performance, and when combined with over 10,000 hours of operation at NCCC on a 1 TPD system, the risk associated with uncertainty in the durability of postcombustion capture membranes has been greatly reduced. Moreover, next-generation Polaris membranes with higher performance and lower cost were validation tested on the 1 TPD system. The 20 TPD system also demonstrated successful operation of a new low-pressure-drop sweep module that will reduce parasitic energy losses at full scale by as much as 10 MWe. In modeling and pilot boiler testing, B&W confirmed the viability of CO 2 recycle to the boiler as envisioned in the MTR process design. The impact of this CO 2 recycle on boiler efficiency was quantified and incorporated into a TEA of the membrane capture process applied to a full-scale power plant. As with previous studies, the TEA showed the membrane process to be lower cost than the conventional solvent capture process even at 90% CO 2capture. A sensitivity study indicates that the membrane capture cost decreases significantly if the 90% capture requirement is relaxed. Depending on the process design, a minimum capture cost is achieved at 30-60% capture, values that would meet proposed CO 2 emission regulations for coal-fired power plants. In summary, this project has successfully advanced the MTR membrane capture process through small pilot testing (technology readiness level 6). The technology is ready for future scale-up to the 10 MWe size.« less

Field Testing of Cryogenic Carbon Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sayre, Aaron; Frankman, Dave; Baxter, Andrew

Sustainable Energy Solutions has been developing Cryogenic Carbon Capture™ (CCC) since 2008. In that time two processes have been developed, the External Cooling Loop and Compressed Flue Gas Cryogenic Carbon Capture processes (CCC ECL™ and CCC CFG™ respectively). The CCC ECL™ process has been scaled up to a 1TPD CO2 system. In this process the flue gas is cooled by an external refrigerant loop. SES has tested CCC ECL™ on real flue gas slip streams from subbituminous coal, bituminous coal, biomass, natural gas, shredded tires, and municipal waste fuels at field sites that include utility power stations, heating plants, cementmore » kilns, and pilot-scale research reactors. The CO2 concentrations from these tests ranged from 5 to 22% on a dry basis. CO2 capture ranged from 95-99+% during these tests. Several other condensable species were also captured including NO2, SO2 and PMxx at 95+%. NO was also captured at a modest rate. The CCC CFG™ process has been scaled up to a .25 ton per day system. This system has been tested on real flue gas streams including subbituminous coal, bituminous coal and natural gas at field sites that include utility power stations, heating plants, and pilot-scale research reactors. CO2 concentrations for these tests ranged from 5 to 15% on a dry basis. CO2 capture ranged from 95-99+% during these tests. Several other condensable species were also captured including NO2, SO2 and PMxx at 95+%. NO was also captured at 90+%. Hg capture was also verified and the resulting effluent from CCC CFG™ was below a 1ppt concentration. This paper will focus on discussion of the capabilities of CCC, the results of field testing and the future steps surrounding the development of this technology.« less

Throwing new light on the reduction of CO2.

PubMed

Ozin, Geoffrey A

2015-03-18

While the chemical energy in fossil fuels has enabled the rapid rise of modern civilization, their utilization and accompanying anthropogenic CO2 emissions is occurring at a rate that is outpacing nature's carbon cycle. Its effect is now considered to be irreversible and this could lead to the demise of human society. This is a complex issue without a single solution, yet from the burgeoning global research activity and development in the field of CO2 capture and utilization, there is light at the end of the tunnel. In this article a couple of recent advances are illuminated. Attention is focused on the discovery of gas-phase, light-assisted heterogeneous catalytic materials and processes for CO2 photoreduction that operate at sufficiently high rates and conversion efficiencies, and under mild conditions, to open a new pathway for an energy transition from today's "fossil fuel economy" to a new and sustainable "CO2 economy". Whichever of the competing CO2 capture and utilization approaches proves to be the best way forward for the development of a future CO2-based solar fuels economy, hopefully this can occur in a period short enough to circumvent the predicted adverse consequences of greenhouse gas climate change. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

The Concept and Experimental Investigation of CO2 and Steam Co-electrolysis for Resource Utilization in Space Exploration

NASA Technical Reports Server (NTRS)

Stoots, Carl; Mulloth, Lila M.; Luna, Bernadette; Varghese, Mini M.

2009-01-01

CO2 acquisition and utilization technologies will have a vital role in determining sustained and affordable life support and in-situ fuel production architectures for human and robotic exploration of Moon and Mars. For long-term human exploration to be practical, reliable technologies have to be implemented to capture and chemically reduce the metabolic CO2 from the cabin air to restitute oxygen consumption. Technologies that facilitate the in-situ capture and conversion of atmospheric CO2 to fuel are essential for a viable human mission to Mars and their demonstration on the moon is critical as well. This paper describes the concept and experimental investigation of a CO2 capture and reduction system that comprises an adsorption compressor and a CO2 and steam co-electrolysis unit. The process products include oxygen for life support and Syngas (CO and H2) for synthetic fuel production. Electrochemical performance in terms of CO2 conversion, oxygen production, and power consumption of a system with a capacity to process 1kg CO2 per day (1-person equivalent) will be discussed.

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 new process for the use of CaO-based sorbent in fluidized bed combustion (FBC) systems, which incorporates CO2 capture, sorbent reactivation, and SO2 retention.

Highlighting the relative effects of surface characteristics and porosity on CO2 capture by adsorbents templated from melamine-based polyaminals

NASA Astrophysics Data System (ADS)

Rehman, Adeela; Park, Soo-Jin

2018-02-01

Heteroatom doping along with well-tuned porosity are considered as significant characteristics of a porous carbon material for various potential applications. However, it is a challenging task to tune a single parameter while retaining the other variables unaffected, and this is considered a limiting factor in rational and systematic research. In the present work, in situ nitrogen-enriched microporous carbon materials were prepared by direct carbonization of conjugated porous polyaminals at two different temperatures. To evaluate the role of nitrogen doping in gas adsorption, a comparison was made with commercially available high-surface-area (2093 m2/g) microporous petroleum-pitch-based activated carbon (AC) deprived of nitrogen functionalities. It was found that the CO2 adsorption capacity of MPA-2-700, carbonized melamine based polyaminal at 700 °C, (186.1 mg/g at 273 K/1 bar with a surface area of 403 m2/g) was significantly higher than that of AC (111.0 mg/g at 273 K/1 bar). Our results present valuable insight into designing porous adsorbents with optimized surface polarity and textural characteristics as promising candidates for CO2 capture.

Stuart Cohen | NREL

Science.gov Websites

;Optimizing post-combustion CO2 capture in response to volatile electricity prices." International , S.M., H.L. Chalmers, M.E. Webber, C.W. King, and J. Gibbins. "Comparing post-combustion CO2 ., G.T. Rochelle, and M.E. Webber. "Optimal operation of flexible post- combustion CO2 capture in

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.

Integrated Solvent Design for CO 2 Capture and Viscosity Tuning

DOE PAGES

Cantu, David C.; Malhotra, Deepika; Koech, Phillip K.; ...

2017-08-18

We present novel design strategies for reduced viscosity single-component, water-lean CO 2 capture organic solvent systems. Through molecular simulation, we identify the main molecular-level descriptor that influences bulk solvent viscosity. Upon loading, a zwitterionic structure forms with a small activation energy of ca 16 kJ/mol and a small stabilization of ca 6 kJ/mol. Viscosity increases exponentially with CO 2 loading due to hydrogen-bonding between neighboring Zwitterions. We find that molecular structures that promote internal hydrogen bonding (within the same molecule) and suppress interactions with neighboring molecules have low viscosities. In addition, tuning the acid/base properties leads to a shift ofmore » the equilibrium toward a non-charged (acid) form that further reduces the viscosity. Here, based on the above structural criteria, a reduced order model is also presented that allows for the quick screening of large compound libraries and down selection of promising candidates for synthesis and testing.« less

Polyethylenimine-incorporated zeolite 13X with mesoporosity for post-combustion CO2 capture

NASA Astrophysics Data System (ADS)

Chen, Chao; Kim, Su-Sung; Cho, Won-Seung; Ahn, Wha-Seung

2015-03-01

X-type zeolite with mesoporosity (Meso-13X) was prepared by using dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride as a mesopore-generating agent, and then modified with polyethylenimine (PEI) through a physical impregnation method to form a hybrid material (Meso-13X-PEI). Meso-13X with and without PEI was characterized by X-ray powder diffraction (XRD), N2 adsorption-desorption isotherm at 77 K, scanning electron microscopy (SEM), and thermogravimetric analysis (TGA). Meso-13X-PEI exhibited higher CO2 capture capacity than PEI-modified zeolite 13X owing to its larger pore volume that accommodates more amine species inside the pore structure, and the mesoporosity also can facilitate dispersion of PEI molecules inside the pore channels. Compared to zeolite 13X, Meso-13X-PEI showed much higher CO2 capture selectivity (against N2) as well as higher CO2 capture capacity at relatively high temperature (e.g. 100 °C) and dilute CO2 concentration relevant to post-combustion conditions.

Subsurface capture of carbon dioxide

DOEpatents

Blount, Gerald; Siddal, Alvin A.; Falta, Ronald W.

2014-07-22

A process and apparatus of separating CO.sub.2 gas from industrial off-gas source in which the CO.sub.2 containing off-gas is introduced deep within an injection well. The CO.sub.2 gases are dissolved in the, liquid within the injection well while non-CO.sub.2 gases, typically being insoluble in water or brine, are returned to the surface. Once the CO.sub.2 saturated liquid is present within the injection well, the injection well may be used for long-term geologic storage of CO.sub.2 or the CO.sub.2 saturated liquid can be returned to the surface for capturing a purified CO.sub.2 gas.

Pilot-Scale Silicone Process for Low-Cost Carbon Dioxide Capture. Final Scientific/Technical Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hancu, Dan; Wood, Benjamin; Genovese, Sarah

GE Global Research has developed, over the last 8 years, a platform of cost effective CO 2 capture technologies based on a non-aqueous aminosilicone solvent (GAP-1m). As demonstrated in a previous funded DOE project (DE-FE0007502), the GAP-1m solvent has increased CO 2 working capacity, lower volatility and corrosivity than the benchmark aqueous amine technology. The current report describes the cooperative program between GE Global Research (GE GRC), and the National Carbon Capture Center (NCCC) to design, construct, and operate a pilot-scale process using GAP-1m solvent to demonstrate its performance at 0.5 MWe. (i) Performance of the GAP-1m solvent was demonstratedmore » in a 0.5 MWe pilot with real flue gas for over 900 hrs. of operation using two alternative desorption designs: a Continuous Stirred Tank Reactor (CSTR), and a Steam Stripper Column (SSC). The CSTR is a one-stage separation unit with reduced space requirements, and capital cost. The alternative is a multi-stage separation column, with improved desorption efficiency. Testing the two desorber options allowed us to identify the most cost effective, and space efficient desorber solution. (ii) CSTR Campaign: The CSTR desorber unit was designed, fabricated and integrated with the pilot solvent test unit (PSTU), replacing the PSTU Steam Stripper Column at NCCC. Solvent management and waste water special procedures were implemented to accommodate operation of the non-aqueous solvent in the PSTU. Performance of the GAP-1m solvent with the CSTR was demonstrated for over 500 hrs. while varying temperature of the desorption (230 – 265 oF), solvent circulation rate (GAP-1m : CO 2 (molar) = 1.5 – 4), and flue gas flow rates (0.2 – 0.5 MWe). Solvent carry-over in the CO 2 product was minimized by maintaining water content below 5 wt.%, and desorption pressure at 7 psig. CO 2 capture efficiency achieved was 95% at 0.25 MWe (GAP-1m : CO 2 = 4 (molar), 230 oF desorption), and 65% at 0.5 MWe (GAP-1m : CO 2 (molar) = 1.5, 248 oF). Solvent loss was dominated by thermal degradation of the rich solvent. (iii) Steam Stripper Column Campaign: Higher expected cost of the solvent vs. aqueous amines makes solvent management a top priority to maintain the low cost for the process. During the testing of the GAP-1m solvent with the CSTR, thermal degradation of the rich solvent was found to be the main mechanism in solvent loss. Small amounts of water in the working solution were found to be an effective way to enable steam stripping, thereby lowering desorption temperature, and hence reducing thermal degradation. Steam stripping also increased working capacity by 30% due to a more efficient desorption. The concept was first tested in a glass stripping column (lab scale, GE GRC), optimized in a continuous bench scale system (2 kWe, GE GRC), and demonstrated in a 0.5 MWe PSTU at NCCC. No special system modifications were required to the PSTU to accommodate the testing of the non-aqueous GAP-1 solvent with the regenerator column. SSC was found to be more robust towards solvent entrainment (H 2O < 35 wt.%). 90 – 95% CO 2 capture efficiency was achieved under stoichiometric conditions at 0.5 MWe (235 oF desorption, 2 psig and 19 wt. % H 2O). Both CO 2 capture efficiency and specific duty reached optimum conditions at 18 wt.% H 2O. Low amine degradation (< 0.05 wt.%/day) was recorded over 350 hrs. of operation. Controlled water addition to GAP-1m solvent decreased the desorption temperature, thermal degradation, and improved the CO 2 working capacity due to more efficient absorption and desorption processes. Under these conditions, the GAP-1m solvent exhibited a 25% increased working capacity, and 10% reduction in specific steam duty vs. MEA, at 10 oF lower desorption temperature. (iv) Techno-economic Analysis: The pilot-scale PSTU engineering data were used to update the capture system process models, and the techno-economic analysis was performed for a 550 MW coal fired power plant. The 1st year CO 2 removal cost for the aminosilicone-based carbon-capture process was evaluated at $48/ton CO 2 using the steam stripper column. This is a 20% reduction compared to MEA, primarily due to lower overall capital cost. CO 2 cost using the CSTR desorber is dominated by the economics of the solvent make-up. The steam stripper desorber is the preferred unit operation due to a more efficient desorption, and reduced solvent make-up rate. Further reduction in CO 2 capture cost is expected by lowering the manufacturing cost of the solvent, implementing flowsheet optimization and/or implementing the next generation aminosilicone solvent with improved stability and increased CO 2 working capacity.« less

Water impacts of CO2 emission performance standards for fossil fuel-fired power plants.

PubMed

Talati, Shuchi; Zhai, Haibo; Morgan, M Granger

2014-10-21

We employ an integrated systems modeling tool to assess the water impacts of the new source performance standards recently proposed by the U.S. Environmental Protection Agency for limiting CO2 emissions from coal- and gas-fired power plants. The implementation of amine-based carbon capture and storage (CCS) for 40% CO2 capture to meet the current proposal will increase plant water use by roughly 30% in supercritical pulverized coal-fired power plants. The specific amount of added water use varies with power plant and CCS designs. More stringent emission standards than the current proposal would require CO2 emission reductions for natural gas combined-cycle (NGCC) plants via CCS, which would also increase plant water use. When examined over a range of possible future emission standards from 1100 to 300 lb CO2/MWh gross, new baseload NGCC plants consume roughly 60-70% less water than coal-fired plants. A series of adaptation approaches to secure low-carbon energy production and improve the electric power industry's water management in the face of future policy constraints are discussed both quantitatively and qualitatively.

Microbial growth under a high-pressure CO2 environment

NASA Astrophysics Data System (ADS)

Thompson, J. R.; Hernandez, H. H.

2009-12-01

Carbon capture and storage (CCS) of CO2 has the potential to significantly reduce the emission of greenhouse gasses associated with fossil fuel combustion. The largest potential for storing captured CO2 in the United Sates is in deep geologic saline formations. Currently, little is known about the effects of CO2 storage on biologically active microbial communities found in the deep earth biosphere. Therefore, to investigate how deep earth microbial communities will be affected by the storage of CO2, we have built a high-pressure microbial growth system in which microbial samples are subjected to a supercritical CO2 (scCO2) environment. Recently we have isolated a microbial consortium that is capable of growth and extracellular matrix production in nutrient media under a supercritical CO2 headspace. This consortium was cultivated from hydrocarbon residues associated with saline formation waters and includes members of the gram-positive Bacillus genus. The cultivation of actively growing cells in an environment containing scCO2 is unexpected based on previous experimental evidence of microbial sterilization attributed to the acidic, desiccating, and solvent-like properties of scCO2. Such microbial consortia have potential for development as (i) biofilm barriers for geological carbon-dioxide sequestration, and as (ii) agents of biocatalysis in environmentally-friendly supercritical (sc) CO2 solvent systems. The discovery that microbes can remain biologically active, and grow, in these environments opens new frontiers for the use of self-regenerating biological systems in engineering applications.

Bench Scale Development and Testing of Aerogel Sorbents for CO 2 Capture Final Technical Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Begag, Redouane

The primary objective of this project was scaling up and evaluating a novel Amine Functionalized Aerogel (AFA) sorbent in a bench scale fluidized bed reactor. The project team (Aspen Aerogels, University of Akron, ADA-ES, and Longtail Consulting) has carried out numerous tests and optimization studies to demonstrate the CO 2 capture performance of the AFA sorbent in all its forms: powder, pellet, and bead. The CO 2 capture target performance of the AFA sorbent (all forms) were set at > 12 wt.% and > 6 wt.% for total and working CO 2 capacity, respectively (@ 40 °C adsorption / 100more » – 120 °C desorption). The optimized AFA powders outperformed the performance targets by more than 30%, for the total CO 2 capacity (14 - 20 wt.%), and an average of 10 % more for working CO 2 capacity (6.6 – 7.0 wt.%, and could be as high as 9.6 wt. % when desorbed at 120 °C). The University of Akron developed binder formulations, pellet production methods, and post treatment technology for increased resistance to attrition and flue gas contaminants. In pellet form the AFA total CO 2 capacity was ~ 12 wt.% (over 85% capacity retention of that of the powder), and there was less than 13% degradation in CO 2 capture capacity after 20 cycles in the presence of 40 ppm SO 2. ADA-ES assessed the performance of the AFA powder, pellet, and bead by analyzing sorption isotherms, water uptake analysis, cycling stability, jet cup attrition and crush tests. At bench scale, the hydrodynamic and heat transfer properties of the AFA sorbent pellet in fluidized bed conditions were evaluated at Particulate Solid Research, Inc. (PSRI). After the process design requirements were completed, by Longtail Consulting LLC, a techno-economic analysis was achieved using guidance from The National Energy Technology Laboratory (NETL) report. This report provides the necessary framework to estimate costs for a temperature swing post combustion CO 2 capture process using a bituminous coal fired, super-critical steam cycle power plant producing 550 MWe net generation with 90% CO 2 capture using a methylethylamine (MEA) solvent. Using the NETL report as guidance, the designed CO 2 capture system was analyzed on a cost basis to determine relative cost estimates between the benchmark MEA system and the AFA sorbent system.« less

Hierarchical calibration and validation framework of bench-scale computational fluid dynamics simulations for solvent-based carbon capture. Part 2: Chemical absorption across a wetted wall column: Original Research Article: Hierarchical calibration and validation framework of bench-scale computational fluid dynamics simulations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Chao; Xu, Zhijie; Lai, Kevin

Part 1 of this paper presents a numerical model for non-reactive physical mass transfer across a wetted wall column (WWC). In Part 2, we improved the existing computational fluid dynamics (CFD) model to simulate chemical absorption occurring in a WWC as a bench-scale study of solvent-based carbon dioxide (CO2) capture. To generate data for WWC model validation, CO2 mass transfer across a monoethanolamine (MEA) solvent was first measured on a WWC experimental apparatus. The numerical model developed in this work can account for both chemical absorption and desorption of CO2 in MEA. In addition, the overall mass transfer coefficient predictedmore » using traditional/empirical correlations is conducted and compared with CFD prediction results for both steady and wavy falling films. A Bayesian statistical calibration algorithm is adopted to calibrate the reaction rate constants in chemical absorption/desorption of CO2 across a falling film of MEA. The posterior distributions of the two transport properties, i.e., Henry's constant and gas diffusivity in the non-reacting nitrous oxide (N2O)/MEA system obtained from Part 1 of this study, serves as priors for the calibration of CO2 reaction rate constants after using the N2O/CO2 analogy method. The calibrated model can be used to predict the CO2 mass transfer in a WWC for a wider range of operating conditions.« less

Hierarchical calibration and validation framework of bench-scale computational fluid dynamics simulations for solvent-based carbon capture. Part 2: Chemical absorption across a wetted wall column: Original Research Article: Hierarchical calibration and validation framework of bench-scale computational fluid dynamics simulations

DOE PAGES

Wang, Chao; Xu, Zhijie; Lai, Kevin; ...

2017-10-24

Part 1 of this paper presents a numerical model for non-reactive physical mass transfer across a wetted wall column (WWC). In Part 2, we improved the existing computational fluid dynamics (CFD) model to simulate chemical absorption occurring in a WWC as a bench-scale study of solvent-based carbon dioxide (CO2) capture. To generate data for WWC model validation, CO2 mass transfer across a monoethanolamine (MEA) solvent was first measured on a WWC experimental apparatus. The numerical model developed in this work can account for both chemical absorption and desorption of CO2 in MEA. In addition, the overall mass transfer coefficient predictedmore » using traditional/empirical correlations is conducted and compared with CFD prediction results for both steady and wavy falling films. A Bayesian statistical calibration algorithm is adopted to calibrate the reaction rate constants in chemical absorption/desorption of CO2 across a falling film of MEA. The posterior distributions of the two transport properties, i.e., Henry's constant and gas diffusivity in the non-reacting nitrous oxide (N2O)/MEA system obtained from Part 1 of this study, serves as priors for the calibration of CO2 reaction rate constants after using the N2O/CO2 analogy method. The calibrated model can be used to predict the CO2 mass transfer in a WWC for a wider range of operating conditions.« less

CO 2 Leakage Into Shallow Aquifers: Modeling CO 2 Gas Evolution and Accumulation at Interfaces of Heterogeneity

DOE PAGES

Porter, Mark L.; Plampin, Michael; Pawar, Rajesh; ...

2014-12-31

The physicochemical processes associated with CO 2 leakage into shallow aquifer systems are complex and span multiple spatial and time scales. Continuum-scale numerical models that faithfully represent the underlying pore-scale physics are required to predict the long-term behavior and aid in risk analysis regarding regulatory and management decisions. This study focuses on benchmarking the numerical simulator, FEHM, with intermediate-scale column experiments of CO 2 gas evolution in homogeneous and heterogeneous sand configurations. Inverse modeling was conducted to calibrate model parameters and determine model sensitivity to the observed steady-state saturation profiles. It is shown that FEHM is a powerful tool thatmore » is capable of capturing the experimentally observed out ow rates and saturation profiles. Moreover, FEHM captures the transition from single- to multi-phase flow and CO 2 gas accumulation at interfaces separating sands. We also derive a simple expression, based on Darcy's law, for the pressure at which CO 2 free phase gas is observed and show that it reliably predicts the location at which single-phase flow transitions to multi-phase flow.« less

Development of a cost-effective CO2 adsorbent from petroleum coke via KOH activation

NASA Astrophysics Data System (ADS)

Jang, Eunji; Choi, Seung Wan; Hong, Seok-Min; Shin, Sangcheol; Lee, Ki Bong

2018-01-01

The capture of CO2 via adsorption is considered an effective technology for decreasing global warming issues; hence, adsorbents for CO2 capture have been actively developed. Taking into account cost-effectiveness and environmental concerns, the development of CO2 adsorbents from waste materials is attracting considerable attention. In this study, petroleum coke (PC), which is the carbon residue remaining after heavy oil upgrading, was used to produce high-value-added porous carbon for CO2 capture. Porous carbon materials were prepared by KOH activation using different weight ratios of KOH/PC (1:1, 2:1, 3:1, and 4:1) and activation temperatures (600, 700, and 800 °C). The specific surface area and total pore volume of resulting porous carbon materials increased with KOH amount, reaching up to 2433 m2/g and 1.11 cm3/g, respectively. The sample prepared under moderate conditions with a KOH/PC weight ratio of 2:1 and activation temperature of 700 °C exhibited the highest CO2 adsorption uptake of 3.68 mmol/g at 25 °C and 1 bar. Interestingly, CO2 adsorption uptake was linearly correlated with the volume of micropores less than 0.8 nm, indicating that narrow micropore volume is crucial for CO2 adsorption. The prepared porous carbon materials also exhibited good selectivity for CO2 over N2, rapid adsorption, facile regeneration, and stable adsorption-desorption cyclic performance, demonstrating potential as a candidate for CO2 capture.

Study of CO2 cyclic absorption stability of CaO-based sorbents derived from lime mud purified by sucrose method.

PubMed

Ma, AiHua; Jia, QingMing; Su, HongYing; Zhi, YunFei; Tian, Na; Wu, Jing; Shan, ShaoYun

2016-02-01

Using lime mud (LM) purified by sucrose method, derived from paper-making industry, as calcium precursor, and using mineral rejects-bauxite-tailings (BTs) from aluminum production as dopant, the CaO-based sorbents for high-temperature CO2 capture were prepared. Effects of BTs content, precalcining time, and temperature on CO2 cyclic absorption stability were illustrated. The cyclic carbonation behavior was investigated in a thermogravimetric analyzer (TGA). Phase composition and morphologies were analyzed by XRD and SEM. The results reflected that the as-synthesized CaO-based sorbent doped with 10 wt% BTs showed a superior CO2 cyclic absorption-desorption conversion during multiple cycles, with conversion being >38 % after 50 cycles. Occurrence of Ca12Al14O33 phase during precalcination was probably responsible for the excellent CO2 cyclic stability.

Comparative Study of Molecular Basket Sorbents Consisting of Polyallylamine and Polyethylenimine Functionalized SBA-15 for CO2 Capture from Flue Gas.

PubMed

Wang, Dongxiang; Wang, Xiaoxing; Song, Chunshan

2017-11-17

Polyallylamine (PAA)-based molecular basket sorbents (MBS) have been studied for CO 2 capture in comparison with polyethylenimine (PEI)-based MBS. The characterizations including N 2 physisorption, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and thermogravimetric analysis (TGA) showed that PAA (M n =15 000) is more rigid and has more steric hindrance inside SBA-15 pores than PEI owing mainly to its different polymer structure. The effects of temperature and PAA loading on the CO 2 sorption capacity of PAA-based MBS have been examined by TGA by using 100 % CO 2 gas stream and compared with PEI/SBA-15. It was found that the capacity of the PAA/SBA-15 sorbent increased with increasing temperature. The optimum capacity of 88 mg CO2  g sorb -1 was obtained at 140 °C for PAA(50)/SBA-15 whereas the optimum sorption temperature was 75 and 90 °C for PEI-I(50)/SBA-15 (PEI-I, M n =423) and PEI-II(50)/SBA-15 (PEI-II, M n =25 000), respectively. The capacity initially increased with the increase of PAA loading and then dropped at high amine contents, owing to the increased diffusion barrier. The highest CO 2 capacity of 109 mg CO2  g sorb -1 was obtained at a PAA loading of 65 wt %, whereas the PAA(50)/SBA-15 sorbent gave the best amine efficiency of 0.23 mol CO2  mol N -1 . The effect of moisture was examined in a fixed-bed flow system with simulated flue gas containing 15 % CO 2 and 4.5 % O 2 in N 2 . It was found that the presence of moisture significantly enhanced CO 2 sorption over PAA(50)/SBA-15 and greatly improved its cyclic stability and regenerability. Compared with PEI/SBA-15, PAA/SBA-15 possesses a better thermal stability and higher resistance to oxidative degradation. However, the CO 2 sorption rate over the PAA(50)/SBA-15 sorbent was much slower. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Earth 2075 (CO2) - can Ocean-Amplified Carbon Capture (oacc) Impart Atmospheric CO2-SINKING Ability to CCS Fossil Energy?

NASA Astrophysics Data System (ADS)

Fry, R.; Routh, M.; Chaudhuri, S.; Fry, S.; Ison, M.; Hughes, S.; Komor, C.; Klabunde, K.; Sethi, V.; Collins, D.; Polkinghorn, W.; Wroobel, B.; Hughes, J.; Gower, G.; Shkolnik, J.

2017-12-01

Previous attempts to capture atmospheric CO2 by algal blooming were stalled by ocean viruses, zooplankton feeding, and/or bacterial decomposition of surface blooms, re-releasing captured CO2 instead of exporting it to seafloor. CCS fossil energy coupling could bypass algal bloom limits—enabling capture of 10 GtC/yr atmospheric CO2 by selective emiliania huxleyi (EHUX) blooming in mid-latitude open oceans, far from coastal waters and polar seas. This could enable a 500 GtC drawdown, 350 ppm restoration by 2050, 280 ppm CO2 by 2075, and ocean pH 8.2. White EHUX blooms could also reflect sunlight back into outer space and seed extra ocean cloud cover, via DMS release, to raise albedo 1.8%—restoring preindustrial temperature (ΔT = 0°C) by 2030. Open oceans would avoid post-bloom anoxia, exclusively a coastal water phenomenon. The EHUX calcification reaction initially sources CO2, but net sinking prevails in follow-up equilibration reactions. Heavier-than-water EHUX sink captured CO2 to the sea floor before surface decomposition occurs. Seeding EHUX high on their nonlinear growth curve could accelerate short-cycle secondary open-ocean blooming—overwhelming mid-latitude viruses, zooplankton, and competition from other algae. Mid-latitude "ocean deserts" exhibit low viral, zooplankton, and bacterial counts. Thermocline prevents nutrient upwelling that would otherwise promote competing algae. Adding nitrogen nutrient would foster exclusive EHUX blooming. Elevated EHUX seed levels could arise from sealed, pH-buffered, floating, seed-production bioreactors infused with 10% CO2 from carbon feedstock supplied by inland CCS fossil power plants capturing 90% of emissions as liquid CO2. Deep-water SPAR platforms extract natural gas from beneath the sea floor. On-platform Haber and pH processing could convert extracted CH4 to buffered NH4+ nutrient, enabling ≥0.7 GtC/yr of bioreactor seed production and 10 GtC/yr of amplified secondary open-ocean CO2 capture—making CCS fossil energy 1400% carbon negative.

Modeling Amorphous Microporous Polymers for CO2 Capture and Separations.

PubMed

Kupgan, Grit; Abbott, Lauren J; Hart, Kyle E; Colina, Coray M

2018-06-13

This review concentrates on the advances of atomistic molecular simulations to design and evaluate amorphous microporous polymeric materials for CO 2 capture and separations. A description of atomistic molecular simulations is provided, including simulation techniques, structural generation approaches, relaxation and equilibration methodologies, and considerations needed for validation of simulated samples. The review provides general guidelines and a comprehensive update of the recent literature (since 2007) to promote the acceleration of the discovery and screening of amorphous microporous polymers for CO 2 capture and separation processes.

The Kinetics and Thermodynamics of CO2 Capture by Aqueous Ammonia Derived Using Meta-GGA Density Functional Theory and Wavefunction-Based Model Chemistry Methods

DOE Office of Scientific and Technical Information (OSTI.GOV)

Beste, Ariana; Attalla, Moetaz; Jackson, Phil

2012-01-01

A meta GGA-DFT study of CO{sub 2} activation in aqueous ammonia solutions, with an emphasis on the reaction barrier and molecularity, has been undertaken using the M06-2X functional with an augmented triple-zeta split-valence basis set (6-311++G(d,p)). Up to five base molecules were treated explicitly in order to establish the effects of solvent catalysis in the chemical capture process. Aqueous free energies of solvation were determined for optimized reactant and transition structures using SM8/M06-2X/6-311++G(d,p). The concept of the solvent pre-complex as presented by Dixon and coworkers (Nguyen, M. T.; Matus, M. H.; Jackson, V. E.; Ngan, V. T.; Rustad, J. R.;more » Dixon, D. A. J. Phys. Chem. A 2008, 112, 10386-10398) was exploited to account for the energetics of disruption of the hydrogen-bonding solvent nano-network prior to the CO{sub 2} activation step. Selected gas- and aqueous-phase thermodynamic quantities have also been derived.« less

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, Zhen-Zhen; Jiang, Deen; Zhu, Xiang

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 chemistrymore » 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.« less

Hierarchically Porous Carbon Materials for CO 2 Capture: The Role of Pore Structure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Estevez, Luis; Barpaga, Dushyant; Zheng, Jian

2018-01-17

With advances in porous carbon synthesis techniques, hierarchically porous carbon (HPC) materials are being utilized as relatively new porous carbon sorbents for CO2 capture applications. These HPC materials were used as a platform to prepare samples with differing textural properties and morphologies to elucidate structure-property relationships. It was found that high microporous content, rather than overall surface area was of primary importance for predicting good CO2 capture performance. Two HPC materials were analyzed, each with near identical high surface area (~2700 m2/g) and colossally high pore volume (~10 cm3/g), but with different microporous content and pore size distributions, which ledmore » to dramatically different CO2 capture performance. Overall, large pore volumes obtained from distinct mesopores were found to significantly impact adsorption performance. From these results, an optimized HPC material was synthesized that achieved a high CO2 capacity of ~3.7 mmol/g at 25°C and 1 bar.« less

Contribution of seagrass plants to CO2 capture in a tropical seagrass meadow under experimental disturbance

PubMed Central

Gullström, Martin; Lyimo, Liberatus D.; Dahl, Martin; Hamisi, Mariam I.; Mtolera, Matern S. P.; Björk, Mats

2017-01-01

Coastal vegetative habitats are known to be highly productive environments with a high ability to capture and store carbon. During disturbance this important function could be compromised as plant photosynthetic capacity, biomass, and/or growth are reduced. To evaluate effects of disturbance on CO2 capture in plants we performed a five-month manipulative experiment in a tropical seagrass (Thalassia hemprichii) meadow exposed to two intensity levels of shading and simulated grazing. We assessed CO2 capture potential (as net CO2 fixation) using areal productivity calculated from continuous measurements of diel photosynthetic rates, and estimates of plant morphology, biomass and productivity/respiration (P/R) ratios (from the literature). To better understand the plant capacity to coping with level of disturbance we also measured plant growth and resource allocation. We observed substantial reductions in seagrass areal productivity, biomass, and leaf area that together resulted in a negative daily carbon balance in the two shading treatments as well as in the high-intensity simulated grazing treatment. Additionally, based on the concentrations of soluble carbohydrates and starch in the rhizomes, we found that the main reserve sources for plant growth were reduced in all treatments except for the low-intensity simulated grazing treatment. If permanent, these combined adverse effects will reduce the plants’ resilience and capacity to recover after disturbance. This might in turn have long-lasting and devastating effects on important ecosystem functions, including the carbon sequestration capacity of the seagrass system. PMID:28704565

Contribution of seagrass plants to CO2 capture in a tropical seagrass meadow under experimental disturbance.

PubMed

Deyanova, Diana; Gullström, Martin; Lyimo, Liberatus D; Dahl, Martin; Hamisi, Mariam I; Mtolera, Matern S P; Björk, Mats

2017-01-01

Coastal vegetative habitats are known to be highly productive environments with a high ability to capture and store carbon. During disturbance this important function could be compromised as plant photosynthetic capacity, biomass, and/or growth are reduced. To evaluate effects of disturbance on CO2 capture in plants we performed a five-month manipulative experiment in a tropical seagrass (Thalassia hemprichii) meadow exposed to two intensity levels of shading and simulated grazing. We assessed CO2 capture potential (as net CO2 fixation) using areal productivity calculated from continuous measurements of diel photosynthetic rates, and estimates of plant morphology, biomass and productivity/respiration (P/R) ratios (from the literature). To better understand the plant capacity to coping with level of disturbance we also measured plant growth and resource allocation. We observed substantial reductions in seagrass areal productivity, biomass, and leaf area that together resulted in a negative daily carbon balance in the two shading treatments as well as in the high-intensity simulated grazing treatment. Additionally, based on the concentrations of soluble carbohydrates and starch in the rhizomes, we found that the main reserve sources for plant growth were reduced in all treatments except for the low-intensity simulated grazing treatment. If permanent, these combined adverse effects will reduce the plants' resilience and capacity to recover after disturbance. This might in turn have long-lasting and devastating effects on important ecosystem functions, including the carbon sequestration capacity of the seagrass system.

Atmospheric CO2 capture for the artificial photosynthetic system

NASA Astrophysics Data System (ADS)

Nogalska, Adrianna; Zukowska, Adrianna; Garcia-Valls, Ricard

2017-11-01

The scope of these studies is to evaluate the ambient CO2 capture abilities of the membrane contactor system in the same conditions as leaves works during photosynthesis, such as ambient temperature, pressure and low CO2 concentration, where the only driving force is the concentration gradient. The polysulfone membrane was made by phase inversion process and characterized by ESEM micrographs which were used to determine the thickness, asymmetry and pore size. Besides, the porosity of the membrane was measured from the membrane and polysulfone density correlation and hydrophobicity was analyzed by contact angle measurements. Moreover, the compatibility of the membrane and absorbent solution was evaluated, in order to exclude wetting issues. The prepared membranes were introduced in a cross flow module and used as contactor between the CO2 and the potassium hydroxide solution, as absorbing media. The influence of the membrane thickness, absorbent stirring rate and absorption time, on CO2 capture were evaluated. The results show that the efficiency of our CO2 capture system is similar to stomatal carbon dioxide assimilation rate.

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. Copyright © 2014 Elsevier Inc. All rights reserved.

Bench-Scale Silicone Process for Low-Cost CO{sub 2} Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wood, Benjamin; Genovese, Sarah; Perry, Robert

2013-12-31

A bench-scale system was designed and built to test an aminosilicone-based solvent. A model was built of the bench-scale system and this model was scaled up to model the performance of a carbon capture unit, using aminosilicones, for CO{sub 2} capture and sequestration (CCS) for a pulverized coal (PC) boiler at 550 MW. System and economic analysis for the carbon capture unit demonstrates that the aminosilicone solvent has significant advantages relative to a monoethanol amine (MEA)-based system. The CCS energy penalty for MEA is 35.9% and the energy penalty for aminosilicone solvent is 30.4% using a steam temperature of 395more » °C (743 °F). If the steam temperature is lowered to 204 °C (400 °F), the energy penalty for the aminosilicone solvent is reduced to 29%. The increase in cost of electricity (COE) over the non-capture case for MEA is ~109% and increase in COE for aminosilicone solvent is ~98 to 103% depending on the solvent cost at a steam temperature of 395 °C (743 °F). If the steam temperature is lowered to 204 °C (400 °F), the increase in COE for the aminosilicone solvent is reduced to ~95-100%.« less

New Technologies for Dealing with CO2 Emission and Carbonate Discharge Control Issues Associated with Energy Production

NASA Astrophysics Data System (ADS)

Tuwati, Abdulwahab

Carbonates and bicarbonates as two water contaminants and CO2 as an air pollutant are the byproducts of a number of fossil fuel based energy production processes. It is well known that the eco-environmental impacts of the carbon based compounds are rather negative. Discharge of co-produced waters containing carbonates and bicarbonates can lead to the significant increase of alkalinity and sodicity and eventual degradation of the quality of soils. In addition, many studies have indicated that huge CO2 emission into the atmosphere can result in disastrous climate changes in the future. Therefore, people are increasingly interested in controlling these carbon compounds. A number of technologies such as ion exchange and electrodialysis have been developed for removal of carbonates and bicarbonates from co-produced waters. However, they are too expensive to be widely used by energy producers, farmers and ranchers. Although many approaches including membrane filtration have been explored for CO2 emission control, their costs are not acceptable to fossil fuel generating companies at all. Therefore, searching cost-effective methods for control of the carbon compounds have attracted many researchers' attentions. New technologies have been developed in this research to overcome the abovementioned challenges. For example, a regenerable solid sorbent (KTi) synthesized with K2CO3 and nanoporous TiO(OH)2 can be used to capture CO2. The CO2 sorption capacity of KTi is about 36 times higher than that of conventional K2CO3. The highest CO2 sorption capacity achieved with KTi is 1.69 mmol-CO2/g-KTi. It should be noted that the theoretical sorption capacity of the KTi can be as high as 3.32 mmol-CO 2/g-KTi. Therefore, the potential and improvement in CO2 sorption capacity with the use of nanoporous TiO(OH)2 is significant. Moreover, nanostructured KTi based CO2 separation (from flue gas) does not need additional high specific-heat capacity and high vaporization-enthalpy H2O. This creates a favorable condition for considerable decrease in energy consumption of CO2 capture in coal-fired power plants. It is expected that all the technologies developed in this research could significantly benefit energy producers, although many works need to be done before they can be commercialized.

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

PubMed

Tossell, J A

2009-04-01

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

Influence of periodically changing oxidizing and reducing environment on sulfur capture under PFBC conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yrjas, P.; Hupa, M.

1997-12-31

In the literature it has been reported that sulfur capture with limestone (CaCO{sub 3}) under atmospheric fluidized bed combustion conditions reaches a maximum at about 850 C. Previously, the maximum has been attributed to the sintering of the sorbent particles which decreases the reactive surface area. Lately, also another explanation has been reported. In this case the sulfur capture decrease at higher temperatures was concluded to be due to fluctuating oxidizing/reducing conditions in the atmospheric combustor. In this paper the influence of alternating oxidizing/reducing conditions on SO{sub 2} capture at atmospheric and elevated pressure (15 bar) is reported. In themore » pressurized case, the CO{sub 2} partial pressure was kept high enough to prevent CaCO{sub 3} from calcining and therefore the CaSO{sub 4} would not form CaO but CaCO{sub 3} from calcining and therefore the CaSO{sub 4} would not form CaO but CaCO{sub 3} under reducing conditions. The experiments were done with a pressurized TGA by periodically changing the gas environment between oxidizing (O{sub 2}, SO{sub 2}, CO{sub 2} and N{sub 2}) and slightly reducing (CO, SO{sub 2}, CO{sub 2} and N{sub 2}) gas mixtures at different temperatures. The results showed that under normal pressure and slightly reducing conditions CaO formation from CaSO{sub 4} increased with temperature as expected. However, no significant amounts of CaCO{sub 3} were formed from CaSO{sub 4} at elevated pressure. It was also concluded that since the formation of CaO from CaSO{sub 4} was relatively slow it could not explain the sharp sulfur capture maximum at about 850 C. Therefore, it was assumed that the strongly reducing zones, where CaS thermodynamically is the stable compound, may play a more important role than the slightly reducing zones, concerning the sulfur capture in fluidized bed combustors.« less

Formation of Carbamate Anions by the Gas-phase Reaction of Anilide Ions with CO2

NASA Astrophysics Data System (ADS)

Liu, Chongming; Nishshanka, Upul; Attygalle, Athula B.

2016-05-01

The anilide anion ( m/z 92) generated directly from aniline, or indirectly as a fragmentation product of deprotonated acetanilide, captures CO2 readily to form the carbamate anion ( m/z 136) in the collision cell, when CO2 is used as the collision gas in a tandem-quadrupole mass spectrometer. The gas-phase affinity of the anilide ion to CO2 is significantly higher than that of the phenoxide anion ( m/z 93), which adds to CO2 only very sluggishly. Our results suggest that the efficacy of CO2 capture depends on the natural charge density on the nitrogen atom, and relative nucleophilicity of the anilide anion. Generally, conjugate bases generated from aniline derivatives with proton affinities (PA) less than 350 kcal/mol do not tend to add CO2 to form gaseous carbamate ions. For example, the anion generated from p-methoxyaniline (PA = 367 kcal/mol) reacts significantly faster than that obtained from p-nitroaniline (PA = 343 kcal/mol). Although deprotonated p-aminobenzoic acid adds very poorly because the negative charge is now located primarily on the carboxylate group, it reacts more efficiently with CO2 if the carboxyl group is esterified. Moreover, mixture of CO2 and He as the collision gas was found to afford more efficient adduct formation than CO2 alone, or as mixtures made with nitrogen or argon, because helium acts as an effective "cooling" gas and reduces the internal energy of reactant ions.

Synthesis and characterization of low viscosity carbon dioxide binding organic liquids for flue gas clean up

DOE Office of Scientific and Technical Information (OSTI.GOV)

Koech, Phillip K.; Malhotra, Deepika; Heldebrant, David J.

2015-01-01

Climate change is partly attributed to global anthropogenic carbon dioxide (CO2) emission to the atmosphere. These environmental effects can be mitigated by CO2 capture, utilization and storage. Alkanolamine solvents, such as monoethanolamine (MEA), which bind CO2 as carbamates or bicarbonate salts are used for CO2 capture in niche applications. These solvents consist of approximately 30 wt% of MEA in water, exhibiting a low, CO2-rich viscosity, fast kinetics and favorable thermodynamics. However, these solvents have low CO2 capacity and high heat capacity of water, resulting in prohibitively high costs of thermal solvent regeneration. Effective capture of the enormous amounts of CO2more » produced by coal-fired plants requires a material with high CO2 capacity and low regeneration energy requirements. To this end, several water-lean transformational solvents systems have been developed in order to reduce these energy penalties. These technologies include nano-material organic hybrids (NOHMs), task-specific, protic and conventional ionic liquids, phase change solvents. As part of an ongoing program in our group, we have developed new water lean transformational solvents known as CO2 binding organic liquids (CO2BOLs) which have the potential to be energy efficient CO2 capture solvents. These solvents, also known as switchable ionic liquids meaning, are organic solvents that can reversibly transform from non- ionic to ionic form and back. The zwitterionic state in these liquids is formed when low polarity non-ionic alkanolguanidines or alkanolamidines react with CO2 or SO2 to form ionic liquids with high polarity. These polar ionic liquids can be thermally converted to the less polar non-ionic solvent by releasing CO2.« less

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

PubMed

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

2013-05-21

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

Integration of CO2 Capture and Mineral Carbonation by Using Recyclable Ammonium Salts

PubMed Central

Wang, Xiaolong; Maroto-Valer, M Mercedes

2011-01-01

A new approach to capture and store CO2 by mineral carbonation using recyclable ammonium salts was studied. This process integrates CO2 capture with mineral carbonation by employing NH3, NH4HSO4, and NH4HCO3 in the capture, mineral dissolution, and carbonation steps, respectively. NH4HSO4 and NH3 can then be regenerated by thermal decomposition of (NH4)2SO4. The use of NH4HCO3 as the source of CO2 can avoid desorption and compression of CO2. The mass ratio of Mg/NH4HCO3/NH3 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 NH4HSO4 and NH3 in this process is 95 %. The mass balance of the process shows that about 2.63 tonnes of serpentine, 0.12 tonnes of NH4HSO4, 7.48 tonnes of NH4HCO3, and 0.04 tonnes of NH3 are required to sequester 1 tonne of CO2 as hydromagnesite. PMID:21732542

Carbon dioxide sequestration monitoring and verification via laser based detection system in the 2 mum band

NASA Astrophysics Data System (ADS)

Humphries, Seth David

Carbon Dioxide (CO2) is a known contributor to the green house gas effect. Emissions of CO2 are rising as the global demand for inexpensive energy is placated through the consumption and combustion of fossil fuels. Carbon capture and sequestration (CCS) may provide a method to prevent CO2 from being exhausted to the atmosphere. The carbon may be captured after fossil fuel combustion in a power plant and then stored in a long term facility such as a deep geologic feature. The ability to verify the integrity of carbon storage at a location is key to the success of all CCS projects. A laser-based instrument has been built and tested at Montana State University (MSU) to measure CO2 concentrations above a carbon storage location. The CO2 Detection by Differential Absorption (CODDA) Instrument uses a temperature-tunable distributed feedback (DFB) laser diode that is capable of accessing a spectral region, 2.0027 to 2.0042 mum, that contains three CO2 absorption lines and a water vapor absorption line. This instrument laser is aimed over an open-air, two-way path of about 100 m, allowing measurements of CO2 concentrations to be made directly above a carbon dioxide release test site. The performance of the instrument for carbon sequestration site monitoring is studied using a newly developed CO2 controlled release facility. The field and CO2 releases are managed by the Zero Emissions Research Technology (ZERT) group at MSU. Two test injections were carried out through vertical wells simulating seepage up well paths. Three test injections were done as CO2 escaped up through a slotted horizontal pipe simulating seepage up through geologic fault zones. The results from these 5 separate controlled release experiments over the course of three summers show that the CODDA Instrument is clearly capable of verifying the integrity of full-scale CO2 storage operations.

CO2-Binding Organic Liquids Gas Capture with Polarity-Swing-Assisted Regeneration Full Technology Feasibility Study B1 - Solvent-based Systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heldebrant, David J

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 600more » 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 demonstrated on the bench cart • No measurable solvent degradation was observed over 4 months of testing – even with 5 wt% water present« less

Carbon Capture and Sequestration from a Hydrogen Production Facility in an Oil Refinery

DOE Office of Scientific and Technical Information (OSTI.GOV)

Engels, Cheryl; Williams, Bryan, Valluri, Kiranmal; Watwe, Ramchandra

2010-06-21

The project proposed a commercial demonstration of advanced technologies that would capture and sequester CO2 emissions from an existing hydrogen production facility in an oil refinery into underground formations in combination with Enhanced Oil Recovery (EOR). The project is led by Praxair, Inc., with other project participants: BP Products North America Inc., Denbury Onshore, LLC (Denbury), and Gulf Coast Carbon Center (GCCC) at the Bureau of Economic Geology of The University of Texas at Austin. The project is located at the BP Refinery at Texas City, Texas. Praxair owns and operates a large hydrogen production facility within the refinery. Asmore » part of the project, Praxair would construct a CO2 capture and compression facility. The project aimed at demonstrating a novel vacuum pressure swing adsorption (VPSA) based technology to remove CO2 from the Steam Methane Reformers (SMR) process gas. The captured CO2 would be purified using refrigerated partial condensation separation (i.e., cold box). Denbury would purchase the CO2 from the project and inject the CO2 as part of its independent commercial EOR projects. The Gulf Coast Carbon Center at the Bureau of Economic Geology, a unit of University of Texas at Austin, would manage the research monitoring, verification and accounting (MVA) project for the sequestered CO2, in conjunction with Denbury. The sequestration and associated MVA activities would be carried out in the Hastings field at Brazoria County, TX. The project would exceed DOE?s target of capturing one million tons of CO2 per year (MTPY) by 2015. Phase 1 of the project (Project Definition) is being completed. The key objective of Phase 1 is to define the project in sufficient detail to enable an economic decision with regard to proceeding with Phase 2. This topical report summarizes the administrative, programmatic and technical accomplishments completed in Phase 1 of the project. It describes the work relative to project technical and design activities (associated with CO2 capture technologies and geologic sequestration MVA), and Environmental Information Volume. Specific accomplishments of this Phase include: 1. Finalization of the Project Management Plan 2. Development of engineering designs in sufficient detail for defining project performance and costs 3. Preparation of Environmental Information Volume 4. Completion of Hazard Identification Studies 5. Completion of control cost estimates and preparation of business plan During the Phase 1 detailed cost estimate, project costs increased substantially from the previous estimate. Furthermore, the detailed risk assessment identified integration risks associated with potentially impacting the steam methane reformer operation. While the Phase 1 work identified ways to mitigate these integration risks satisfactorily from an operational perspective, the associated costs and potential schedule impacts contributed to the decision not to proceed to Phase 2. We have concluded that the project costs and integration risks at Texas City are not commensurate with the potential benefits of the project at this time.« less

Biorefineries of carbon dioxide: From carbon capture and storage (CCS) to bioenergies production.

PubMed

Cheah, Wai Yan; Ling, Tau Chuan; Juan, Joon Ching; Lee, Duu-Jong; Chang, Jo-Shu; Show, Pau Loke

2016-09-01

Greenhouse gas emissions have several adverse environmental effects, like pollution and climate change. Currently applied carbon capture and storage (CCS) methods are not cost effective and have not been proven safe for long term sequestration. Another attractive approach is CO2 valorization, whereby CO2 can be captured in the form of biomass via photosynthesis and is subsequently converted into various form of bioenergy. This article summarizes the current carbon sequestration and utilization technologies, while emphasizing the value of bioconversion of CO2. In particular, CO2 sequestration by terrestrial plants, microalgae and other microorganisms are discussed. Prospects and challenges for CO2 conversion are addressed. The aim of this review is to provide comprehensive knowledge and updated information on the current advances in biological CO2 sequestration and valorization, which are essential if this approach is to achieve environmental sustainability and economic feasibility. Copyright © 2016 Elsevier Ltd. All rights reserved.

Enhanced Adsorption Efficiency through Materials Design for Direct Air Capture over Supported Polyethylenimine.

PubMed

Sayari, Abdelhamid; Liu, Qing; Mishra, Prashant

2016-10-06

Until recently, carbon capture and sequestration (CCS) was regarded as the most promising technology to address the alarming increase in the concentration of anthropogenic CO 2 in the atmosphere. There is now an increasing interest in carbon capture and utilization (CCU). In this context, the capture of CO 2 from air is an ideal solution to supply pure CO 2 wherever it is needed. Here, we describe innovative materials for direct air capture (DAC) with unprecedented efficiency. Polyethylenimine (PEI) was supported on PME, which is an extra-large-pore silica (pore-expanded MCM-41) with its internal surfaces fully covered by a uniform layer of readily accessible C 16 chains from cetyltrimethylammonium (CTMA + ) cations. The CTMA + layer plays a key role in enhancing the amine efficiency toward dry or humid ultradilute CO 2 (400 ppm CO 2 /N 2 ) to unprecedented levels. At the same PEI content, the amine efficiency of PEI/PME was two to four times higher than that of the corresponding calcined mesoporous silica loaded with PEI or with different combinations of C 16 chains and PEI. Under humid conditions, the amine efficiency of 40 wt % PEI/PME reached 7.31 mmolCO2 /g PEI , the highest ever reported for any supported PEI in the presence of 400 ppm CO 2 . Thus, amine accessibility, which reflects both the state of PEI dispersion and the adsorption efficiency, is intimately associated with the molecular design of the adsorbent. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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.

Efficient Purification and Release of Circulating Tumor Cells by Synergistic Effect of Biomarker and SiO2 @Gel-Microbead-Based Size Difference Amplification.

PubMed

Huang, Qinqin; Cai, Bo; Chen, Bolei; Rao, Lang; He, Zhaobo; He, Rongxiang; Guo, Feng; Zhao, Libo; Kondamareddy, Kiran Kumar; Liu, Wei; Guo, Shishang; Zhao, Xing-Zhong

2016-07-01

Microfluidics-based circulating tumor cell (CTC) isolation is achieved by using gelatin-coated silica microbeads conjugated to CTC-specific antibodies. Bead-binding selectively enlarges target cell size, providing efficient high-purity capture. CTCs captured can be further released non-invasively. This stratagem enables high-performance CTC isolation for subsequent studies. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Synthetic biology for microbial production of lipid-based biofuels.

PubMed

d'Espaux, Leo; Mendez-Perez, Daniel; Li, Rachel; Keasling, Jay D

2015-12-01

The risks of maintaining current CO2 emission trends have led to interest in producing biofuels using engineered microbes. Microbial biofuels reduce emissions because CO2 produced by fuel combustion is offset by CO2 captured by growing biomass, which is later used as feedstock for biofuel fermentation. Hydrocarbons found in petroleum fuels share striking similarity with biological lipids. Here we review synthetic metabolic pathways based on fatty acid and isoprenoid metabolism to produce alkanes and other molecules suitable as biofuels. We further discuss engineering strategies to optimize engineered biosynthetic routes, as well as the potential of synthetic biology for sustainable manufacturing. Published by Elsevier Ltd.

Amine-impregnated silica monolith with a hierarchical pore structure: enhancement of CO2 capture capacity.

PubMed

Chen, Chao; Yang, Seung-Tae; Ahn, Wha-Seung; Ryoo, Ryong

2009-06-28

A polyethylenimine-impregnated hierarchical silica monolith exhibited significantly higher CO(2) capturing capacity than other silica-supported amine sorbents, and produced a reversible and durable sorption performance.

Novel Inorganic/Polymer Composite Membranes for CO 2 Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ho, W.S. Winston; Dutta, Prabir K.; Schmit, Steve J.

The objective of this project is to develop a cost-effective design and manufacturing process for new membrane modules that capture CO 2 from flue gas in coal-fired power plants. The membrane consisted of a thin selective layer including inorganic (zeolite) embedded in a polymer structure so that it can be made in a continuous manufacturing process. The membrane was incorporated in spiral-wound modules for the field test with actual flue gas at the National Carbon Capture Center (NCCC) in Wilsonville, AL and bench scale tests with simulated flue gas at the Ohio State University (OSU). Using the modules for post-combustionmore » CO 2 capture is expected to achieve the DOE target of $40/tonne CO 2 captured (in 2007 dollar) for 2025. Membranes with the amine-containing polymer cover layer on zeolite-Y (ZY) nanoparticles deposited on the polyethersulfone (PES) substrate were successfully synthesized. The membranes showed a high CO 2 permeance of about 1100 GPU (gas permeation unit, 1 GPU = 10 -6 cm 3 (STP)/(cm 2 • s • cm Hg), 3000 GPU = 10-6 mol/(m 2 • s • Pa)) with a high CO 2/N 2 selectivity of > 200 at the typical flue gas conditions at 57°C (about 17% water vapor in feed gas) and > 1400 GPU CO 2 permeance with > 500 CO 2/N 2 selectivity at 102°C (~ 80% water vapor). The synthesis of ZY nanoparticles was successfully scaled up, and the pilot-scale membranes were also successfully fabricated using the continuous membrane machine at OSU. The transport performance of the pilot-scale membranes agreed reasonably well with the lab-scale membranes. The results from both the lab-scale and scale-up membranes were used for the techno-economic analysis. The scale-up membranes were fabricated into prototype spiral-wound membrane modules for continuous testing with simulated or real flue gas. For real flue gas testing, we worked with NCCC, in consultation with TriSep Corporation, Gradient Technology and American Electric Power (AEP). The membrane module demonstrated > 800 GPU of CO 2 permeance and > 150 CO 2/N 2 selectivity when tested with real flue gas at NCCC. The results obtained were used to update the techno-economic analysis. In addition, the EH&S assessment of the membranes for post-combustion CO 2 capture was conducted.« less

Humidity-swing mechanism for CO2 capture from ambient air.

PubMed

Yang, Hao; Singh, Manmilan; Schaefer, Jacob

2018-05-10

A humidity-swing polymeric sorbent captures CO2 from ambient air at room temperature simply by changing the humidity level. To date there has been no direct experimental evidence to characterize the chemical mechanism for this process. In this report we describe the use of solid-state NMR to study the humidity-swing CO2 absorption/desorption cycle directly. We find that at low humidity levels CO2 is absorbed as HCO3-. At high humidity levels, HCO3- is replaced by hydrated OH- and the absorbed CO2 is released.

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 extensive research. Using these mitigation technologies in combination may offer a pivotal option for reducing atmospheric carbon to pre-industrial levels with minimal human risk or inconvenience.

Pre-combustion CO2 capture by transition metal ions embedded in phthalocyanine sheets

NASA Astrophysics Data System (ADS)

Lü, Kun; Zhou, Jian; Zhou, Le; Chen, X. S.; Chan, Siew Hwa; Sun, Qiang

2012-06-01

Transition metal (TM) embedded two-dimensional phthalocyanine (Pc) sheets have been recently synthesized in experiments [M. Abel, S. Clair, O. Ourdjini, M. Mossoyan, and L. Porte, J. Am. Chem. Soc. 133, 1203 (2010)], 10.1021/ja108628r, where the transition metal ions are uniformly distributed in porous structures, providing the possibility of capturing gas molecules. Using first principles and grand canonical Monte Carlo simulations, TMPc sheets (TM = Sc, Ti, and Fe) are studied for pre-combustion CO2 capture by considering the adsorptions of H2/CO2 gas mixtures. It is found that ScPc sheet shows a good selectivity for CO2, and the excess uptake capacity of single-component CO2 on ScPc sheet at 298 K and 50 bar is found to be 2949 mg/g, larger than that of any other reported porous materials. Furthermore, electrostatic potential and natural bond orbital analyses are performed to reveal the underlying interaction mechanisms, showing that electrostatic interactions as well as the donation and back donation of electrons between the transition metal ions and the CO2 molecules play a key role in the capture.

Coal-Derived Warm Syngas Purification and CO 2 Capture-Assisted Methane Production

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dagle, Robert A.; King, David L.; Li, Xiaohong S.

2014-10-01

Gasifier-derived syngas from coal has many applications in the area of catalytic transformation to fuels and chemicals. Raw syngas must be treated to remove a number of impurities that would otherwise poison the synthesis catalysts. Inorganic impurities include alkali salts, chloride, sulfur compounds, heavy metals, ammonia, and various P, As, Sb, and Se- containing compounds. Systems comprising multiple sorbent and catalytic beds have been developed for the removal of impurities from gasified coal using a warm cleanup approach. This approach has the potential to be more economic than the currently available acid gas removal (AGR) approaches and improves upon currentlymore » available processes that do not provide the level of impurity removal that is required for catalytic synthesis application. Gasification also lends itself much more readily to the capture of CO 2, important in the regulation and control of greenhouse gas emissions. CO 2 capture material was developed and in this study was demonstrated to assist in methane production from the purified syngas. Simultaneous CO 2 sorption enhances the CO methanation reaction through relaxation of thermodynamic constraint, thus providing economic benefit rather than simply consisting of an add-on cost for carbon capture and release. Molten and pre-molten LiNaKCO 3 can promote MgO and MgO-based double salts to capture CO 2 with high cycling capacity. A stable cycling CO 2 capacity up to 13 mmol/g was demonstrated. This capture material was specifically developed in this study to operate in the same temperature range and therefore integrate effectively with warm gas cleanup and methane synthesis. By combining syngas methanation, water-gas-shift, and CO 2 sorption in a single reactor, single pass yield to methane of 99% was demonstrated at 10 bar and 330°C when using a 20 wt% Ni/MgAl 2O 4 catalyst and a molten-phase promoted MgO-based sorbent. Under model feed conditions both the sorbent and catalyst exhibited favorable stability after multiple test cycles. The cleanup for warm gas cleanup of inorganics was broken down into three major steps: chloride removal, sulfur removal, and the removal for a multitude of trace metal contaminants. Na 2CO 3 was found to optimally remove chlorides at an operating temperature of 450ºC. For sulfur removal two regenerable ZnO beds are used for bulk H 2S removal at 450ºC (<5 ppm S) and a non-regenerable ZnO bed for H 2S polishing at 300ºC (<40 ppb S). It was also found that sulfur from COS could be adsorbed (to levels below our detection limit of 40 ppb) in the presence of water that leads to no detectable slip of H 2S. Finally, a sorbent material comprising of Cu and Ni was found to be effective in removing trace metal impurities such as AsH 3 and PH 3 when operating at 300ºC. Proof-of-concept of the integrated cleanup process was demonstrated with gasifier-generated syngas produced at the Western Research Institute using Wyoming Decker Coal. When operating with a ~1 SLPM feed, multiple inorganic contaminant removal sorbents and a tar-reforming bed was able to remove the vast majority of contaminants from the raw syngas. A tar-reforming catalyst was employed due to the production of tars generated from the gasifier used in this particular study. It is envisioned that in a real application a commercial scale gasifier operating at a higher temperature would produce lesser amount of tar. Continuous operation of a poison-sensitive copper-based WGS catalyst located downstream from the cleanup steps resulted in successful demonstration.« less

Coal liquefaction by base-catalyzed hydrolysis with CO.sub.2 capture

DOEpatents

Xiao, Xin

2014-03-18

The one-step hydrolysis of diverse biomaterials including coal, cellulose materials such as lumber and forestry waste, non-food crop waste, lignin, vegetable oils, animal fats and other source materials used for biofuels under mild processing conditions which results in the formation of a liquid fuel product along with the recovery of a high purity CO.sub.2 product is provided.

Overcoming the challenges of mosquito (Diptera: Culicidae) sampling in remote localities: a comparison of CO2 attractants on mosquito communities in three tropical forest habitats.

PubMed

Steiger, D B Meyer; Ritchie, S A; Laurance, S G W

2014-01-01

Emerging infectious diseases are on the rise with future outbreaks predicted to occur in frontier regions of tropical countries. Disease surveillance in these hotspots is challenging because sampling techniques often rely on vector attractants that are either unavailable in remote localities or difficult to transport. We examined whether a novel method for producing CO2 from yeast and sugar produces similar mosquito species captures compared with a standard attractant such as dry ice. Across three different vegetation communities, we found traps baited with dry ice frequently captured more mosquitoes than yeast-baited traps; however, there was little effect on mosquito community composition. Based on our preliminary experiments, we find that this method of producing CO2 is a realistic alternative to dry ice and would be highly suitable for remote field work.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rychel, Dwight

The Permian Basin Carbon Capture, Utilization and Storage (CCUS) Training Center was one of seven regional centers formed in 2009 under the American Recovery and Reinvestment Act of 2009 and managed by the Department of Energy. Based in the Permian Basin, it is focused on the utilization of CO 2 Enhanced Oil Recovery (EOR) projects for the long term storage of CO 2 while producing a domestic oil and revenue stream. It delivers training to students, oil and gas professionals, regulators, environmental and academia through a robust web site, newsletter, tech alerts, webinars, self-paced online courses, one day workshops, andmore » two day high level forums. While course material prominently features all aspects of the capture, transportation and EOR utilization of CO 2, the audience focus is represented by its high level forums where selected graduate students with an interest in CCUS interact with Industry experts and in-house workshops for the regulatory community.« less

Solvent Effects on the Photothermal Regeneration of CO 2 in Monoethanolamine Nanofluids

DOE PAGES

Nguyen, Du; Stolaroff, Joshuah; Esser-Kahn, Aaron

2015-11-02

We present that a potential approach to reduce energy costs associated with carbon capture is to use external and renewable energy sources. The photothermal release of CO 2 from monoethanolamine mediated by nanoparticles is a unique solution to this problem. When combined with light-absorbing nanoparticles, vapor bubbles form inside the capture solution and release the CO 2 without heating the bulk solvent. The mechanism by which CO 2 is released remained unclear, and understanding this process would improve the efficiency of photothermal CO 2 release. Here we report the use of different cosolvents to improve or reduce the photothermal regenerationmore » of CO 2 captured by monoethanolamine. We found that properties that reduce the residence time of the gas bubbles (viscosity, boiling point, and convection direction) can enhance the regeneration efficiencies. The reduction of bubble residence times minimizes the reabsorption of CO 2 back into the capture solvent where bulk temperatures remain lower than the localized area surrounding the nanoparticle. These properties shed light on the mechanism of release and indicated methods for improving the efficiency of the process. We used this knowledge to develop an improved photothermal CO 2 regeneration system in a continuously flowing setup. Finally, using techniques to reduce residence time in the continuously flowing setup, such as alternative cosolvents and smaller fluid volumes, resulted in regeneration efficiency enhancements of over 200%.« less

Solvent Effects on the Photothermal Regeneration of CO 2 in Monoethanolamine Nanofluids

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nguyen, Du; Stolaroff, Joshuah; Esser-Kahn, Aaron

We present that a potential approach to reduce energy costs associated with carbon capture is to use external and renewable energy sources. The photothermal release of CO 2 from monoethanolamine mediated by nanoparticles is a unique solution to this problem. When combined with light-absorbing nanoparticles, vapor bubbles form inside the capture solution and release the CO 2 without heating the bulk solvent. The mechanism by which CO 2 is released remained unclear, and understanding this process would improve the efficiency of photothermal CO 2 release. Here we report the use of different cosolvents to improve or reduce the photothermal regenerationmore » of CO 2 captured by monoethanolamine. We found that properties that reduce the residence time of the gas bubbles (viscosity, boiling point, and convection direction) can enhance the regeneration efficiencies. The reduction of bubble residence times minimizes the reabsorption of CO 2 back into the capture solvent where bulk temperatures remain lower than the localized area surrounding the nanoparticle. These properties shed light on the mechanism of release and indicated methods for improving the efficiency of the process. We used this knowledge to develop an improved photothermal CO 2 regeneration system in a continuously flowing setup. Finally, using techniques to reduce residence time in the continuously flowing setup, such as alternative cosolvents and smaller fluid volumes, resulted in regeneration efficiency enhancements of over 200%.« less

Microwave-assisted nitric acid treatment of sepiolite and functionalization with polyethylenimine applied to CO2 capture and CO2/N2 separation

NASA Astrophysics Data System (ADS)

Vilarrasa-García, E.; Cecilia, J. A.; Bastos-Neto, M.; Cavalcante, C. L.; Azevedo, D. C. S.; Rodríguez-Castellón, E.

2017-07-01

Sepiolite was treated in HNO3 solutions with the assistance of microwave radiation. This treatment caused the progressive depletion of Mg2+, the gradual degradation of the sepiolite structure and the formation of an amorphous silica phase, which contributes to a noticeable increase of the surface area. The use of microwaves during acid treatment, after few minutes, led to materials with similar SBET to those obtained after 48 h with conventional heating methods. The influence of mineralogical impurities, crystallinity and chemical composition in the reactivity of sepiolite to this treatment was also studied. The obtained materials were impregnated with polyethylenimine and assessed for CO2 capture and CO2/N2 selectivity at different temperatures. Experimental equilibrium data were fitted to Langmuir and Sips models. The adsorption data revealed that sepiolite can be an interesting adsorbent for CO2 capture, achieving a capacity of 1.70 mmol g-1 at 338 K and 1 bar, providing a high CO2/N2 selectivity (440 mol CO2/mol N2).

Using infrastructure optimization to reduce greenhouse gas emissions from oil sands extraction and processing.

PubMed

Middleton, Richard S; Brandt, Adam R

2013-02-05

The Alberta oil sands are a significant source of oil production and greenhouse gas emissions, and their importance will grow as the region is poised for decades of growth. We present an integrated framework that simultaneously considers economic and engineering decisions for the capture, transport, and storage of oil sands CO(2) emissions. The model optimizes CO(2) management infrastructure at a variety of carbon prices for the oil sands industry. Our study reveals several key findings. We find that the oil sands industry lends itself well to development of CO(2) trunk lines due to geographic coincidence of sources and sinks. This reduces the relative importance of transport costs compared to nonintegrated transport systems. Also, the amount of managed oil sands CO(2) emissions, and therefore the CCS infrastructure, is very sensitive to the carbon price; significant capture and storage occurs only above 110$/tonne CO(2) in our simulations. Deployment of infrastructure is also sensitive to CO(2) capture decisions and technology, particularly the fraction of capturable CO(2) from oil sands upgrading and steam generation facilities. The framework will help stakeholders and policy makers understand how CCS infrastructure, including an extensive pipeline system, can be safely and cost-effectively deployed.

Sulphation of CaO-Based Sorbent Modified in CO2 Looping Cycles

NASA Astrophysics Data System (ADS)

Manovic, Vasilije; Anthony, Edward J.; Loncarevic, Davor

CaO-based looping cycles for CO2 capture at high temperatures are based on cyclical carbonation of CaO and regeneration of CaCO3. The main limitation of natural sorbents is the loss of carrying capacity with increasing numbers of reaction cycles, resulting in spent sorbent ballast. Use of spent sorbent from CO2 looping cycles for SO2 capture is a possible solution investigated in this study. Three limestones were investigated: Kelly Rock (Canada), La Blanca (Spain) and Katowice (Poland). Carbonation/calcination cycles were performed in a tube furnace with original limestones and samples thermally pretreated for different times (i.e., sintered). The spent sorbent samples were sulphated in a thermogravimetric analyzer. Changes in the resulting pore structure were then investigated using mercury porosimetry. Final conversions of both spent and pretreated sorbents after longer sulphation times were comparable or higher than those observed for the original sorbents. Maximum sulphation levels strongly depend on sorbent porosity and pore surface area. The shrinkage of sorbent particles during calcination/cycling resulted in a loss of sorbent porosity (≤48%), which corresponds to maximum sulphation levels ˜55% for spent Kelly Rock and Katowice. However, this is ˜10% higher than for the original samples. By contrast, La Blanca limestone had more pronounced particle shrinkage during pretreatment and cycling, leading to lower porosity, <35%, resulting in sulphation conversion of spent samples <30%, significantly lower than for the original sample (45%). These results showed that spent sorbent samples from CO2 looping cycles can be used as sorbents for SO2 retention if significant porosity loss does not occur during CO2 reaction cycles. For spent Kelly Rock and Katowice samples final conversions are determined by the total pore volume available for the bulky CaSO4 product.

Hierarchical calibration and validation framework of bench-scale computational fluid dynamics simulations for solvent-based carbon capture. Part 2: Chemical absorption across a wetted wall column: Original Research Article: Hierarchical calibration and validation framework of bench-scale computational fluid dynamics simulations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Chao; Xu, Zhijie; Lai, Kevin

The first part of this paper (Part 1) presents a numerical model for non-reactive physical mass transfer across a wetted wall column (WWC). In Part 2, we improved the existing computational fluid dynamics (CFD) model to simulate chemical absorption occurring in a WWC as a bench-scale study of solvent-based carbon dioxide (CO2) capture. To generate data for WWC model validation, CO2 mass transfer across a monoethanolamine (MEA) solvent was first measured on a WWC experimental apparatus. The numerical model developed in this work has the ability to account for both chemical absorption and desorption of CO2 in MEA. In addition,more » the overall mass transfer coefficient predicted using traditional/empirical correlations is conducted and compared with CFD prediction results for both steady and wavy falling films. A Bayesian statistical calibration algorithm is adopted to calibrate the reaction rate constants in chemical absorption/desorption of CO2 across a falling film of MEA. The posterior distributions of the two transport properties, i.e., Henry’s constant and gas diffusivity in the non-reacting nitrous oxide (N2O)/MEA system obtained from Part 1 of this study, serves as priors for the calibration of CO2 reaction rate constants after using the N2O/CO2 analogy method. The calibrated model can be used to predict the CO2 mass transfer in a WWC for a wider range of operating conditions.« less

Hierarchical calibration and validation framework of bench-scale computational fluid dynamics simulations for solvent-based carbon capture. Part 2: Chemical absorption across a wetted wall column: Original Research Article: Hierarchical calibration and validation framework of bench-scale computational fluid dynamics simulations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Chao; Xu, Zhijie; Lai, Kevin

Part 1 of this paper presents a numerical model for non-reactive physical mass transfer across a wetted wall column (WWC). In Part 2, we improved the existing computational fluid dynamics (CFD) model to simulate chemical absorption occurring in a WWC as a bench-scale study of solvent-based carbon dioxide (CO 2) capture. In this study, to generate data for WWC model validation, CO 2 mass transfer across a monoethanolamine (MEA) solvent was first measured on a WWC experimental apparatus. The numerical model developed in this work can account for both chemical absorption and desorption of CO 2 in MEA. In addition,more » the overall mass transfer coefficient predicted using traditional/empirical correlations is conducted and compared with CFD prediction results for both steady and wavy falling films. A Bayesian statistical calibration algorithm is adopted to calibrate the reaction rate constants in chemical absorption/desorption of CO 2 across a falling film of MEA. The posterior distributions of the two transport properties, i.e., Henry's constant and gas diffusivity in the non-reacting nitrous oxide (N 2O)/MEA system obtained from Part 1 of this study, serves as priors for the calibration of CO 2 reaction rate constants after using the N 2O/CO 2 analogy method. Finally, the calibrated model can be used to predict the CO 2 mass transfer in a WWC for a wider range of operating conditions.« less

Hierarchical calibration and validation framework of bench-scale computational fluid dynamics simulations for solvent-based carbon capture. Part 2: Chemical absorption across a wetted wall column: Original Research Article: Hierarchical calibration and validation framework of bench-scale computational fluid dynamics simulations

DOE PAGES

Wang, Chao; Xu, Zhijie; Lai, Kevin; ...

2017-10-24

Part 1 of this paper presents a numerical model for non-reactive physical mass transfer across a wetted wall column (WWC). In Part 2, we improved the existing computational fluid dynamics (CFD) model to simulate chemical absorption occurring in a WWC as a bench-scale study of solvent-based carbon dioxide (CO 2) capture. In this study, to generate data for WWC model validation, CO 2 mass transfer across a monoethanolamine (MEA) solvent was first measured on a WWC experimental apparatus. The numerical model developed in this work can account for both chemical absorption and desorption of CO 2 in MEA. In addition,more » the overall mass transfer coefficient predicted using traditional/empirical correlations is conducted and compared with CFD prediction results for both steady and wavy falling films. A Bayesian statistical calibration algorithm is adopted to calibrate the reaction rate constants in chemical absorption/desorption of CO 2 across a falling film of MEA. The posterior distributions of the two transport properties, i.e., Henry's constant and gas diffusivity in the non-reacting nitrous oxide (N 2O)/MEA system obtained from Part 1 of this study, serves as priors for the calibration of CO 2 reaction rate constants after using the N 2O/CO 2 analogy method. Finally, the calibrated model can be used to predict the CO 2 mass transfer in a WWC for a wider range of operating conditions.« less

Structure stability of HKUST-1 towards water and ethanol and their effect on its CO2 capture properties.

PubMed

Álvarez, J Raziel; Sánchez-González, Elí; Pérez, Eric; Schneider-Revueltas, Emilia; Martínez, Ana; Tejeda-Cruz, Adriana; Islas-Jácome, Alejandro; González-Zamora, Eduardo; Ibarra, Ilich A

2017-07-18

Water and ethanol stabilities of the crystal structure of the Cu-based metal-organic framework (MOF) HKUST-1 have been investigated. Vapour (water and ethanol) sorption isotherms and cyclability were measured by a dynamic strategy. The ethanol sorption capacity of HKUST-1 at 303 K remained unchanged contrasting water sorption (which decreased along with the sorption experiment time). Considering the binding energy of each sorbate with the open Cu(ii) sites, obtained by the use of diffusion coefficients, we showed the superior crystal stability of the HKUST-1 framework towards ethanol. Finally, a small quantity of ethanol (pre-adsorbed) slightly enhanced CO 2 capture without crystal structure degradation.

Screening of metal-organic frameworks for carbon dioxide capture from flue gas using a combined experimental and modeling approach.

PubMed

Yazaydin, A Ozgür; Snurr, Randall Q; Park, Tae-Hong; Koh, Kyoungmoo; Liu, Jian; Levan, M Douglas; Benin, Annabelle I; Jakubczak, Paulina; Lanuza, Mary; Galloway, Douglas B; Low, John J; Willis, Richard R

2009-12-30

A diverse collection of 14 metal-organic frameworks (MOFs) was screened for CO(2) capture from flue gas using a combined experimental and modeling approach. Adsorption measurements are reported for the screened MOFs at room temperature up to 1 bar. These data are used to validate a generalized strategy for molecular modeling of CO(2) and other small molecules in MOFs. MOFs possessing a high density of open metal sites are found to adsorb significant amounts of CO(2) even at low pressure. An excellent correlation is found between the heat of adsorption and the amount of CO(2) adsorbed below 1 bar. Molecular modeling can aid in selection of adsorbents for CO(2) capture from flue gas by screening a large number of MOFs.

Early opportunities of CO2 geological storage deployment in coal chemical industry in China

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wei, Ning; Li, Xiaochun; Liu, Shengnan

2014-11-12

Abstract: Carbon dioxide capture and geological storage (CCS) is regarded as a promising option for climate change mitigation; however, the high capture cost is the major barrier to large-scale deployment of CCS technologies. High-purity CO2 emission sources can reduce or even avoid the capture requirements and costs. Among these high-purity CO2 sources, certain coal chemical industry processes are very important, especially in China. In this paper, the basic characteristics of coal chemical industries in China is investigated and analyzed. As of 2013 there were more than 100 coal chemical plants in operation or in late planning stages. These emission sourcesmore » together emit 430 million tons CO2 per year, of which about 30% are emit high-purity and pure CO2 (CO2 concentration >80% and >99% respectively).Four typical source-sink pairs are studied by a techno-economic evaluation, including site screening and selection, source-sink matching, concept design, and experienced economic evaluation. The technical-economic evaluation shows that the levelized cost of a CO2 capture and aquifer storage project in the coal chemistry industry ranges from 14 USD/t to 17 USD/t CO2. When a 15USD/t CO2 tax and 15USD/t for CO2 sold to EOR are considered, the levelized cost of CCS project are negative, which suggests a net economic benefit from some of these CCS projects. This might provide China early opportunities to deploy and scale-up CCS projects in the near future.« less

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.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Doug Cathro

The Lake Charles CCS Project is a large-scale industrial carbon capture and sequestration (CCS) project which will demonstrate advanced technologies that capture and sequester carbon dioxide (CO{sub 2}) emissions from industrial sources into underground formations. Specifically the Lake Charles CCS Project will accelerate commercialization of large-scale CO{sub 2} storage from industrial sources by leveraging synergy between a proposed petroleum coke to chemicals plant (the LCC Gasification Project) and the largest integrated anthropogenic CO{sub 2} capture, transport, and monitored sequestration program in the U.S. Gulf Coast Region. The Lake Charles CCS Project will promote the expansion of EOR in Texas andmore » Louisiana and supply greater energy security by expanding domestic energy supplies. The capture, compression, pipeline, injection, and monitoring infrastructure will continue to sequester CO{sub 2} for many years after the completion of the term of the DOE agreement. The objectives of this project are expected to be fulfilled by working through two distinct phases. The overall objective of Phase 1 was to develop a fully definitive project basis for a competitive Renewal Application process to proceed into Phase 2 - Design, Construction and Operations. Phase 1 includes the studies attached hereto that will establish: the engineering design basis for the capture, compression and transportation of CO{sub 2} from the LCC Gasification Project, and the criteria and specifications for a monitoring, verification and accounting (MVA) plan at the Hastings oil field in Texas. The overall objective of Phase 2, provided a successful competitive down-selection, is to execute design, construction and operations of three capital projects: (1) the CO{sub 2} capture and compression equipment, (2) a Connector Pipeline from the LLC Gasification Project to the Green Pipeline owned by Denbury and an affiliate of Denbury, and (3) a comprehensive MVA system at the Hastings oil field.« less

Carbonate-based zeolitic imidazolate framework for highly selective CO2 capture.

PubMed

Basnayake, Sajani A; Su, Jie; Zou, Xiadong; Balkus, Kenneth J

2015-02-16

In this study, we report the formation of a new crystal structure, ZIF-CO3-1, which results from the reaction of Zn(2+), 2-methylimidazole, and carbonate. ZIF-CO3-1 can be synthesized solvothermally in N,N-dimethylformamide (DMF)/water (H2O) or by utilizing of CO2 gas at various temperatures in DMF/H2O or H2O. This reaction selectively consumes CO2 because CO2 is incorporated in the ZIF as carbonate. CO2 can be quantitatively released by acidifying the ZIF. Powder X-ray diffraction, single-crystal X-ray diffraction, FTIR spectroscopy, scanning electron microscopy, elemental analysis, and thermogravimetric analysis were used to characterize the ZIF structure. ZIF-CO3-1 (chemical formula C9H10N4O3Zn2), crystallizes in the orthorhombic crystal system with noncentrosymmetric space group Pba2.

In situ studies of materials for high temperature CO2 capture and storage.

PubMed

Dunstan, Matthew T; Maugeri, Serena A; Liu, Wen; Tucker, Matthew G; Taiwo, Oluwadamilola O; Gonzalez, Belen; Allan, Phoebe K; Gaultois, Michael W; Shearing, Paul R; Keen, David A; Phillips, Anthony E; Dove, Martin T; Scott, Stuart A; Dennis, John S; Grey, Clare P

2016-10-20

Carbon capture and storage (CCS) offers a possible solution to curb the CO 2 emissions from stationary sources in the coming decades, considering the delays in shifting energy generation to carbon neutral sources such as wind, solar and biomass. The most mature technology for post-combustion capture uses a liquid sorbent, amine scrubbing. However, with the existing technology, a large amount of heat is required for the regeneration of the liquid sorbent, which introduces a substantial energy penalty. The use of alternative sorbents for CO 2 capture, such as the CaO-CaCO 3 system, has been investigated extensively in recent years. However there are significant problems associated with the use of CaO based sorbents, the most challenging one being the deactivation of the sorbent material. When sorbents such as natural limestone are used, the capture capacity of the solid sorbent can fall by as much as 90 mol% after the first 20 carbonation-regeneration cycles. In this study a variety of techniques were employed to understand better the cause of this deterioration from both a structural and morphological standpoint. X-ray and neutron PDF studies were employed to understand better the local surface and interfacial structures formed upon reaction, finding that after carbonation the surface roughness is decreased for CaO. In situ synchrotron X-ray diffraction studies showed that carbonation with added steam leads to a faster and more complete conversion of CaO than under conditions without steam, as evidenced by the phases seen at different depths within the sample. Finally, in situ X-ray tomography experiments were employed to track the morphological changes in the sorbents during carbonation, observing directly the reduction in porosity and increase in tortuosity of the pore network over multiple calcination reactions.

Advanced Acid Gas Separation Technology for the Utilization of Low Rank Coals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kloosterman, Jeff

2012-12-31

Air Products has developed a potentially ground-breaking technology – Sour Pressure Swing Adsorption (PSA) – to replace the solvent-based acid gas removal (AGR) systems currently employed to separate sulfur containing species, along with CO{sub 2} and other impurities, from gasifier syngas streams. The Sour PSA technology is based on adsorption processes that utilize pressure swing or temperature swing regeneration methods. Sour PSA technology has already been shown with higher rank coals to provide a significant reduction in the cost of CO{sub 2} capture for power generation, which should translate to a reduction in cost of electricity (COE), compared to baselinemore » CO{sub 2} capture plant design. The objective of this project is to test the performance and capability of the adsorbents in handling tar and other impurities using a gaseous mixture generated from the gasification of lower rank, lignite coal. The results of this testing are used to generate a high-level pilot process design, and to prepare a techno-economic assessment evaluating the applicability of the technology to plants utilizing these coals.« less

Supersonic Post-Combustion Inertial CO 2 Extraction System Final Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Balepin, Vladimir

This report summarizes the effort carried out under NETL contract DE- FE0013122 from 1 October 2013 to 31 March 2017. As described in this document, technical challenges realized during the performance of this project resulted in completion of only the first two of three planned budget periods. Despite this outcome, substantial progress was made toward understanding and maturing the CO 2 capture technology under consideration and considerable future promise remains for applications requiring lower CO 2 capture and/or lower CO 2.

Preparation Methods of Metal Organic Frameworks and Their Capture of CO2

NASA Astrophysics Data System (ADS)

Zhang, Linjian; Liand, Fangqin; Luo, Liangfei

2018-01-01

The increasingly serious greenhouse effect makes people pay more attention to the capture and storage technology of CO2. Metal organic frameworks (MOFs) have the advantages of high specific surface area, porous structure and controllable structure, and become the research focus of CO2 emission reduction technology in recent years. In this paper, the characteristics, preparation methods and application of MOFs in the field of CO2 adsorption and separation are discussed, especially the application of flue gas environment in power plants.

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

PubMed

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

2011-09-15

CO(2) emissions, from fossil-fuel-burning power plants, the breathing, etc., influence the global worming on large scale and the man's work efficiency on small scale. The reversible capture of CO(2) is a prominent feature of CO(2) organic-inorganic hybrid adsorbent to sequester CO(2). Herein, (3-aminopropyl) trimethoxysilane (APTMS), [3-(methylamino)propyl] trimethoxysilane (MAPTMS), and [3-(diethylamino) propyl] trimethoxysilane (DEAPTMS) are immobilized on highly ordered mesoporous silicas (SBA-15) to catch CO(2) as primary, secondary, and tertiary aminosilica adsorbents. X-ray photoelectron spectroscopy was used to analyze the immobilized APTMS, MAPTMS, and DEAPTMS on the SBA-15. We report an interesting discovery that the CO(2) adsorption and desorption on the adsorbent depend on the amine type of the aminosilica adsorbent. The adsorbed CO(2) was easily desorbed from the adsorbent with the low energy consumption in the order of tertiary, secondary, and primary amino-adsorbents while the adsorption amount and the bonding-affinity increased in the reverse order. The effectiveness of amino-functionalized (1(o), 2(o), and 3(o) amines) SBA-15s as a CO(2) capturing agent was investigated in terms of adsorption capacity, adsorption-desorption kinetics, and thermodynamics. This work demonstrates apt amine types to catch CO(2) and regenerate the adsorbent, which may open new avenues to designing "CO(2) basket". Copyright © 2011. Published by Elsevier Inc.

Improved Structural Design and CO 2 Capture of Porous Hydroxy-Rich Polymeric Organic Frameworks

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kidder, Michelle K.; Earl, Lyndsey D.; de Almeida, Valmor F.

2016-04-16

Polymeric organic frameworks (POFs) are tunable and robust porous materials with potential applications for gas capture, catalysis, and separations technologies. A series of new porous POFs have been synthesized from the reaction of phloroglucinol or resorcinol derivatives with aryl aldehyde precursors. The monomers have various molecular shapes including linear, bent, trigonal, and tetrahedral geometries. Depending on the size and geometric matching of the monomers, the polymers are dominantly microporous with some mesoporous character or they are non-porous. In addition to standard spectroscopic and surface characterization, the materials were screened as adsorbents for carbon dioxide capture at low pressure (0-1 bar).more » The best performing material (POF 1D) has a CO 2 capture capacity of 9.0 wt. % (2.04 mmol g -1) at 298 K and 1 bar which is comparable to other polymeric organic frameworks. Isosteric heats of adsorption for POF 1A, POF 2A, and POF 2B were found to be dependent on the weight percent of CO 2 adsorbed: this suggests there are both chemisorptive and physisorptive components of CO 2 capture by the POFs.« less

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 and weighed against those of alternative strategies, including business as usual.

U-tube based near-surface environmental monitoring in the Shenhua carbon dioxide capture and storage (CCS) project.

PubMed

Li, Qi; Song, Ranran; Shi, Hui; Ma, Jianli; Liu, Xuehao; Li, Xiaochun

2018-04-01

The CO 2 injected into deep formations during implementation of carbon dioxide (CO 2 ) capture and storage (CCS) technology may leak and migrate into shallow aquifers or ground surfaces through a variety of pathways over a long period. The leaked CO 2 can threaten shallow environments as well as human health. Therefore, almost all monitoring programs for CCS projects around the world contain near-surface monitoring. This paper presents a U-tube based near-surface monitoring technology focusing on its first application in the Shenhua CCS demonstration project, located in the Ordos Basin, Inner Mongolia, China. First, background information on the site monitoring program of the Shenhua CCS demonstration project was provided. Then, the principle of fluid sampling and the monitoring methods were summarized for the U-tube sampler system, and the monitoring data were analyzed in detail. The U-tube based monitoring results showed that the U-tube sampler system is accurate, flexible, and representative of the subsurface fluid sampling process. The monitoring indicators for the subsurface water and soil gas at the Shenhua CCS site indicate good stratification characteristics. The concentration level of each monitoring indicator decreases with increasing depth. Finally, the significance of this near-surface environmental monitoring technology for CO 2 leakage assessments was preliminarily confirmed at the Shenhua CCS site. The application potential of the U-tube based monitoring technology was also demonstrated during the subsurface environmental monitoring of other CCS projects.

Coal-fired Power Plants with Flexible Amine-based CCS and Co-located Wind Power: Environmental, Economic and Reliability Outcomes

NASA Astrophysics Data System (ADS)

Bandyopadhyay, Rubenka

Carbon Capture and Storage (CCS) technologies provide a means to significantly reduce carbon emissions from the existing fleet of fossil-fired plants, and hence can facilitate a gradual transition from conventional to more sustainable sources of electric power. This is especially relevant for coal plants that have a CO2 emission rate that is roughly two times higher than that of natural gas plants. Of the different kinds of CCS technology available, post-combustion amine based CCS is the best developed and hence more suitable for retrofitting an existing coal plant. The high costs from operating CCS could be reduced by enabling flexible operation through amine storage or allowing partial capture of CO2 during high electricity prices. This flexibility is also found to improve the power plant's ramp capability, enabling it to offset the intermittency of renewable power sources. This thesis proposes a solution to problems associated with two promising technologies for decarbonizing the electric power system: the high costs of the energy penalty of CCS, and the intermittency and non-dispatchability of wind power. It explores the economic and technical feasibility of a hybrid system consisting of a coal plant retrofitted with a post-combustion-amine based CCS system equipped with the option to perform partial capture or amine storage, and a co-located wind farm. A techno-economic assessment of the performance of the hybrid system is carried out both from the perspective of the stakeholders (utility owners, investors, etc.) as well as that of the power system operator. (Abstract shortened by ProQuest.).

DOE Office of Scientific and Technical Information (OSTI.GOV)

Manovic, V.; Anthony, E.J.; Loncarevic, D.

CaO-based looping cycles are promising processes for CO{sub 2} Capture from both syngas and flue gas. The technology is based on cyclical carbonation of CaO and regeneration of CaCO{sub 3} in a dual fluidized-bed reactor to produce a pure CO{sub 2} stream suitable for sequestration. Use of spent sorbent from CO{sub 2} looping cycles for SO{sub 2} capture is investigated. Three limestones were investigated: Kelly Rock (Canada), La Blanca (Spain), and Katowice (Poland, Upper Silesia). Carbonation/calcination cycles were performed in a tube furnace with both the original limestones and samples thermally pretreated for different times (i.e., sintered). The spent sorbentmore » samples were sulfated in a thermogravimetric analyzer (TGA). The changes in the resulting sorbent pore structure were then investigated using mercury porosimetry. It has been shown that the sulfation rates of both thermally pretreated and spent sorbent samples are lower in comparison with those of the original samples. However, final conversions of both spent and pretreated sorbents after longer sulfation time were comparable or higher than those observed for the original sorbents under comparable conditions. Maximum sulfation levels strongly depend on sorbent porosity and pore surface area. The results showed that spent sorbent samples from CO{sub 2} looping cycles can be used as sorbents for SO{sub 2} retention in cases where significant porosity loss does not occur during CO{sub 2} reaction cycles. In the case of spent Kelly Rock and Katowice samples, sorbent particles are practically uniformly sulfated, achieving final conversions that are determined by the total pore volume available for the bulky CaSO{sub 4} product.« less

Thermodynamic and mass transfer modeling of carbon dioxide absorption into aqueous 2-amino-2-methyl-1-propanol

DOE PAGES

Sherman, Brent J.; Rochelle, Gary T.

2016-12-16

Explanations for the mass transfer behavior of 2-amino-2-methyl-1-propanol (AMP) are conflicting, despite extensive study of the amine for CO 2 capture. At equilibrium, aqueous AMP reacts with CO 2 to give bicarbonate in a 1:1 ratio. While this is the same stoichiometry as a tertiary amine, the reaction rate of AMP is 100 times faster. This work aims to explain the mass transfer behavior of AMP, specifically the stoichiometry and kinetics. An eNRTL thermodynamic model was used to regress wetted-wall column mass transfer data with two activity-based reactions: formation of carbamate and formation of bicarbonate. Data spanned 40–100 C andmore » 0.15–0.60 mol CO 2/mol alk). The fitted carbamate rate constant is three orders of magnitude greater than the bicarbonate rate constant. Rapid carbamate formation explains the kinetics, while the stoichiometry is explained by the carbamate reverting in the bulk liquid to allow CO 2 to form bicarbonate. Understanding the role of carbamate formation and diffusion in hindered amines enables optimizing solvent amine concentration by balancing viscosity and free amine concentration. Furthermore, this improves absorber design for CO 2 capture.« less

Atmospheric CO2 capture for the artificial photosynthetic system.

PubMed

Nogalska, Adrianna; Zukowska, Adrianna; Garcia-Valls, Ricard

2018-04-15

The aim of these studies is to evaluate the ambient CO 2 capture abilities of the membrane contactor system in the same conditions as leafs, such as ambient temperature, pressure and low CO 2 concentration, where the only driving force is the concentration gradient. The polysulfone membrane employed was made by a phase inversion process and characterized by ESEM micrographs which were used to determine the thickness, asymmetry and pore size. Besides, the porosity of the membrane was measured from the membrane and polysulfone density correlation and the hydrophobicity was analyzed by contact angle measurements. Moreover, the compatibility of membrane and absorbent was evaluated, in order to exclude wetting issues by meaning of swelling, dynamic contact angle and AFM analysis. The prepared membranes were introduced into a cross flow module and used as contactors between CO 2 and the absorbing media, a potassium hydroxide solution. The influence of the membrane thickness, absorbent stirring rate, solution pH and absorption time on CO 2 capture were evaluated. Absorbent solution stirring rate showed no statistically significant influence on absorption. We observed a non-linear correlation between the capture rate and the increase of absorbent solution pH as well as absorption time. The results showed that the efficiency of our CO 2 capture system is similar to stomatal carbon dioxide assimilation rate, achieving stable value of 20μmol/m 2 ·s after 1h of experiment. Copyright © 2017 Elsevier B.V. All rights reserved.

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. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Hollow fiber-supported designer ionic liquid sponges for post-combustion CO2 scrubbing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lee, JS; Hillesheim, PC; Huang, DK

A proof of concept study for a new type of carbon capture system is considered for post-combustion CO2 capture based on porous hollow fiber sorbents with ionic liquids sorbed in the cell walls of the fiber. This study proves that delicate morphological features in the open-celled porous wall can be maintained during the infusion process. Mixtures of task specific ionic liquid (i.e. [BMIM][Tf2N]) and superbase (i.e. DBU) were loaded into polyamide-imide (PAI) fibers by a so-called two-step non-solvent infusion protocol. In the protocol, methanol carries ionic liquids into the pore cell walls of hollow fibers and then hexane carries superbasemore » to create an efficient CO2 sorbent. Our ionic liquid/superbase impregnation technique overcomes a serious increase in mass transfer resistance upon reaction with CO2, thereby allowing its large scale utilization for post-combustion CO2 capture. The investigation on the effect of different pore former additives (different molecular weights of polyvinylpyrrolidone, lithium nitrate, and their mixtures) suggested that a large molecular weight of PVP (M-w; 1300k) including dope composition produces highly interconnected open cell pore structures of PAI hollow fibers. Lastly, a lumen side barrier layer was successfully formed on the bore side of neat PAI fibers by using a mixture of Neoprene (R) with crosslinking agents (TSR-633) via a post-treatment process. The lumen layer will enable heat removal from the fiber sorbents during their application in rapid thermal swing cycling processes. (C) 2012 Elsevier Ltd. All rights reserved.« less

An adsorption of carbon dioxide on activated carbon controlled by temperature swing adsorption

NASA Astrophysics Data System (ADS)

Tomas, Korinek; Karel, Frana

2017-09-01

This work deals with a method of capturing carbon dioxide (CO2) in indoor air. Temperature Swing Adsorption (TSA) on solid adsorbent was chosen for CO2 capture. Commercial activated carbon (AC) in form of extruded pellets was used as a solid adsorbent. There was constructed a simple device to testing effectiveness of CO2 capture in a fixed bed with AC. The TSA cycle was also simulated using the open-source software OpenFOAM. There was a good agreement between results obtained from numerical simulations and experimental data for adsorption process.

ECONOMIC EVALUATION OF CO2 STORAGE AND SINK ENHANCEMENT OPTIONS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bert Bock; Richard Rhudy; Howard Herzog

2003-02-01

This project developed life-cycle costs for the major technologies and practices under development for CO{sub 2} storage and sink enhancement. The technologies evaluated included options for storing captured CO{sub 2} in active oil reservoirs, depleted oil and gas reservoirs, deep aquifers, coal beds, and oceans, as well as the enhancement of carbon sequestration in forests and croplands. The capture costs for a nominal 500 MW{sub e} integrated gasification combined cycle plant from an earlier study were combined with the storage costs from this study to allow comparison among capture and storage approaches as well as sink enhancements.

Electropolymerized carbonic anhydrase immobilization for carbon dioxide capture.

PubMed

Merle, Geraldine; Fradette, Sylvie; Madore, Eric; Barralet, Jake E

2014-06-17

Biomimetic carbonation carried out with carbonic anhydrase (CA) in CO2-absorbing solutions, such as methyldiethanolamine (MDEA), is one approach that has been developed to accelerate the capture of CO2. However, there are several practical issues, such as high cost and limited enzyme stability, that need to be overcome. In this study, the capacity of CA immobilization on a porous solid support was studied to improve the instability in the tertiary amine solvent. We have shown that a 63% porosity macroporous carbon foam support makes separation and reuse facile and allows for an efficient supply and presentation of CO2 to an aqueous solvent and the enzyme catalytic center. These enzymatic supports conserved 40% of their initial activity after 42 days at 70 °C in an amine solvent, whereas the free enzyme shows no activity after 1 h in the same conditions. In this work, we have overcome the technical barrier associated with the recovery of the biocatalyst after operation, and most of all, these electropolymerized enzymatic supports have shown a remarkable increase of thermal stability in an amine-based CO2 sequestration solvent.

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.

Intercalation and retention of carbon dioxide in a smectite clay promoted by interlayer cations.

PubMed

Michels, L; Fossum, J O; Rozynek, Z; Hemmen, H; Rustenberg, K; Sobas, P A; Kalantzopoulos, G N; Knudsen, K D; Janek, M; Plivelic, T S; da Silva, G J

2015-03-05

A good material for CO2 capture should possess some specific properties: (i) a large effective surface area with good adsorption capacity, (ii) selectivity for CO2, (iii) regeneration capacity with minimum energy input, allowing reutilization of the material for CO2 adsorption, and (iv) low cost and high environmental friendliness. Smectite clays are layered nanoporous materials that may be good candidates in this context. Here we report experiments which show that gaseous CO2 intercalates into the interlayer nano-space of smectite clay (synthetic fluorohectorite) at conditions close to ambient. The rate of intercalation, as well as the retention ability of CO2 was found to be strongly dependent on the type of the interlayer cation, which in the present case is Li(+), Na(+) or Ni(2+). Interestingly, we observe that the smectite Li-fluorohectorite is able to retain CO2 up to a temperature of 35°C at ambient pressure, and that the captured CO2 can be released by heating above this temperature. Our estimates indicate that smectite clays, even with the standard cations analyzed here, can capture an amount of CO2 comparable to other materials studied in this context.

Intercalation and Retention of Carbon Dioxide in a Smectite Clay promoted by Interlayer Cations

PubMed Central

Michels, L.; Fossum, J. O.; Rozynek, Z.; Hemmen, H.; Rustenberg, K.; Sobas, P. A.; Kalantzopoulos, G. N.; Knudsen, K. D.; Janek, M.; Plivelic, T. S.; da Silva, G. J.

2015-01-01

A good material for CO2 capture should possess some specific properties: (i) a large effective surface area with good adsorption capacity, (ii) selectivity for CO2, (iii) regeneration capacity with minimum energy input, allowing reutilization of the material for CO2 adsorption, and (iv) low cost and high environmental friendliness. Smectite clays are layered nanoporous materials that may be good candidates in this context. Here we report experiments which show that gaseous CO2 intercalates into the interlayer nano-space of smectite clay (synthetic fluorohectorite) at conditions close to ambient. The rate of intercalation, as well as the retention ability of CO2 was found to be strongly dependent on the type of the interlayer cation, which in the present case is Li+, Na+ or Ni2+. Interestingly, we observe that the smectite Li-fluorohectorite is able to retain CO2 up to a temperature of 35°C at ambient pressure, and that the captured CO2 can be released by heating above this temperature. Our estimates indicate that smectite clays, even with the standard cations analyzed here, can capture an amount of CO2 comparable to other materials studied in this context. PMID:25739522

Efficacy of Mosquito Traps for Collecting Potential West Nile Mosquito Vectors in a Natural Mediterranean Wetland

PubMed Central

Roiz, David; Roussel, Marion; Muñoz, Joaquin; Ruiz, Santiago; Soriguer, Ramón; Figuerola, Jordi

2012-01-01

Surveillance, research, and control of mosquito-borne diseases such as West Nile virus require efficient methods for sampling mosquitoes. We compared the efficacy of BG-Sentinel and Centers for Disease Control and Prevention (CDC)-CO2 traps in terms of the abundances of host-seeking and blood-fed female mosquitoes and the origin of mosquito bloodmeals. Our results indicate that BG-Sentinel traps that use CO2 and attractants are as effective as CDC-CO2 traps for Culex mosquito species, Ochlerotatus caspius, and they are also highly efficient at capturing Anopheles atroparvus host-seeking and blood-fed females with or without CO2. The CDC-CO2 trap is the least efficient method for capturing blood-fed females. BG-Sentinel traps with attractants and CO2 were significantly better at capturing mosquitoes that had fed on mammals than the unbaited BG-Sentinel and CDC-CO2 traps in the cases of An. atroparvus and Cx. theileri. These results may help researchers to optimize trapping methods by obtaining greater sample sizes and saving time and money. PMID:22492149

Process for CO.sub.2 capture using zeolites from high pressure and moderate temperature gas streams

DOEpatents

Siriwardane, Ranjani V [Morgantown, WV; Stevens, Robert W [Morgantown, WV

2012-03-06

A method for separating CO.sub.2 from a gas stream comprised of CO.sub.2 and other gaseous constituents using a zeolite sorbent in a swing-adsorption process, producing a high temperature CO.sub.2 stream at a higher CO.sub.2 pressure than the input gas stream. The method utilizes CO.sub.2 desorption in a CO.sub.2 atmosphere and effectively integrates heat transfers for optimizes overall efficiency. H.sub.2O adsorption does not preclude effective operation of the sorbent. The cycle may be incorporated in an IGCC for efficient pre-combustion CO.sub.2 capture. A particular application operates on shifted syngas at a temperature exceeding 200.degree. C. and produces a dry CO.sub.2 stream at low temperature and high CO.sub.2 pressure, greatly reducing any compression energy requirements which may be subsequently required.

CO2 capture by ionic liquids - an answer to anthropogenic CO2 emissions?

PubMed

Sanglard, Pauline; Vorlet, Olivier; Marti, Roger; Naef, Olivier; Vanoli, Ennio

2013-01-01

Ionic liquids (ILs) are efficient solvents for the selective removal of CO2 from flue gas. Conventional, offthe-shelf ILs are limited in use to physisorption, which restricts their absorption capacity. After adding a chemical functionality like amines or alcohols, absorption of CO2 occurs mainly by chemisorption. This greatly enhances CO2 absorption and makes ILs suitable for potential industrial applications. By carefully choosing the anion and the cation of the IL, equimolar absorption of CO2 is possible. This paper reviews the current state of the art of CO2 capture by ILs and presents the current research in this field performed at the ChemTech Institute of the Ecole d'Ingénieurs et d'Architectes de Fribourg.

Ambient Carbon Dioxide Capture Using Boron-Rich Porous Boron Nitride: A Theoretical Study.

PubMed

Li, Lanlan; Liu, Yan; Yang, Xiaojing; Yu, Xiaofei; Fang, Yi; Li, Qiaoling; Jin, Peng; Tang, Chengchun

2017-05-10

The development of highly efficient sorbent materials for CO 2 capture under ambient conditions is of great importance for reducing the impact of CO 2 on the environment and climate change. In this account, strong CO 2 adsorption on a boron antisite (B N ) in boron-rich porous boron nitrides (p-BN) was developed and studied. The results indicated that the material achieved larger adsorption energies of 2.09 eV (201.66 kJ/mol, PBE-D). The electronic structure calculations suggested that the introduction of B N in p-BN induced defect electronic states in the energy gap region, which strongly impacted the adsorption properties of the material. The bonding between the B N defect and the CO 2 molecule was clarified, and it was found that the electron donation first occurred from CO 2 to the B N double-acceptor state then, followed by electron back-donation from B N to CO 2 accompanied by the formation of a B N -C bond. The thermodynamic properties indicated that the adsorption of CO 2 on the B N defect to form anionic CO 2 δ- species was spontaneous at temperatures below 350 K. Both the large adsorption energies and the thermodynamic properties ensured that p-BN with a B N defect could effectively capture CO 2 under ambient conditions. Finally, to evaluate the energetic stability, the defect formation energies were estimated. The formation energy of the B N defects was found to strongly depend on the chemical environment, and the selection of different reactants (B or N sources) would achieve the goal of reducing the formation energy. These findings provided a useful guidance for the design and fabrication of a porous BN sorbent for CO 2 capture.

Porous MOF with Highly Efficient Selectivity and Chemical Conversion for CO2.

PubMed

Wang, Hai-Hua; Hou, Lei; Li, Yong-Zhi; Jiang, Chen-Yu; Wang, Yao-Yu; Zhu, Zhonghua

2017-05-31

A new Co(II)-based MOF, {[Co 2 (tzpa)(OH)(H 2 O) 2 ]·DMF} n (1) (H 3 tzpa = 5-(4-(tetrazol-5-yl)phenyl)isophthalic acid), was constructed by employing a tetrazolyl-carboxyl ligand H 3 tzpa. 1 possesses 1D tubular channels that are decorated by μ 3 -OH groups, uncoordinated carboxylate O atoms, and open metal centers generated by the removal of coordinated water molecules, leading to high CO 2 adsorption capacity and significantly selective capture for CO 2 over CH 4 and CO in the temperature range of 298-333 K. Moreover, 1 shows the chemical stability in acidic and basic aqueous solutions. Grand canonical Monte Carlo simulations identified multiple CO 2 -philic sites in 1. In addition, the activated 1 as the heterogeneous Lewis and Brønsted acid bifunctional catalyst facilitates the chemical fixation of CO 2 coupling with epoxides into cyclic carbonates under ambient conditions.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kress, Joel David

The development and scale up of cost effective carbon capture processes is of paramount importance to enable the widespread deployment of these technologies to significantly reduce greenhouse gas emissions. The U.S. Department of Energy initiated the Carbon Capture Simulation Initiative (CCSI) in 2011 with the goal of developing a computational toolset that would enable industry to more effectively identify, design, scale up, operate, and optimize promising concepts. The first half of the presentation will introduce the CCSI Toolset consisting of basic data submodels, steady-state and dynamic process models, process optimization and uncertainty quantification tools, an advanced dynamic process control framework,more » and high-resolution filtered computationalfluid- dynamics (CFD) submodels. The second half of the presentation will describe a high-fidelity model of a mesoporous silica supported, polyethylenimine (PEI)-impregnated solid sorbent for CO 2 capture. The sorbent model includes a detailed treatment of transport and amine-CO 2- H 2O interactions based on quantum chemistry calculations. Using a Bayesian approach for uncertainty quantification, we calibrate the sorbent model to Thermogravimetric (TGA) data.« less

Synthetic biology for microbial production of lipid-based biofuels

DOE Office of Scientific and Technical Information (OSTI.GOV)

d’Espaux, Leo; Mendez-Perez, Daniel; Li, Rachel

The risks of maintaining current CO 2 emission trends have led to interest in producing biofuels using engineered microbes. Microbial biofuels reduce emissions because CO 2 produced by fuel combustion is offset by CO2 captured by growing biomass, which is later used as feedstock for biofuel fermentation. Hydrocarbons found in petroleum fuels share striking similarity with biological lipids. Here in this paper we review synthetic metabolic pathways based on fatty acid and isoprenoid metabolism to produce alkanes and other molecules suitable as biofuels. Lastly, we further discuss engineering strategies to optimize engineered biosynthetic routes, as well as the potential ofmore » synthetic biology for sustainable manufacturing.« less

Combined effect of fuel-design and after-treatment system on reduction of local and global emissions from CI engine.

PubMed

Thiyagarajan, S; Geo, V Edwin; Martin, Leenus Jesu; Nagalingam, B

2018-03-22

This experimental study aims to mitigate harmful emissions from a CI engine using bio-energy with carbon capture and storage (BECCS) approach. The engine used for this experimental work is a single cylinder CI engine with a rated power of 5.2 kW at a constant speed of 1500 rpm. The BECCS approach is a combination of plant-based biofuels and carbon capture and storage (CCS) system. The whole investigation was done in four phases: (1) Substituting diesel with Karanja oil methyl ester (KOME) (2) Equal volume blending of Orange oil (ORG) with KOME (3) 20% blending of n-butanol (B) with KOME-ORG blend (4) CCS system with zeolite based non-selective catalytic reduction (NSCR) and mono ethanolamine (MEA) based selective non-catalytic reduction (SNCR) system with KOME-ORG + B20 blend. The experimental results show that substitution of diesel with KOME reduces smoke emission, but increases NO and CO 2 emission. KOME-ORG blend reduces CO 2 and smoke emissions with high NO emission due to combustion improvement. In comparison with the sole combustion of KOME at full load condition, the combination of KOME-ORG + B20 as bio-fuel with zeolite based post-combustion treatment system resulted in a maximum reduction of NO, smoke and CO 2 emission by 41%, 19% and 15% respectively.

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.

Modelling atmospheric oxidation of 2-aminoethanol (MEA) emitted from post-combustion capture using WRF-Chem.

PubMed

Karl, M; Svendby, T; Walker, S-E; Velken, A S; Castell, N; Solberg, S

2015-09-15

Carbon capture and storage (CCS) is a technological solution that can reduce the amount of carbon dioxide (CO2) emissions from the use of fossil fuel in power plants and other industries. A leading method today is amine based post-combustion capture, in which 2-aminoethanol (MEA) is one of the most studied absorption solvents. In this process, amines are released to the atmosphere through evaporation and entrainment from the CO2 absorber column. Modelling is a key instrument for simulating the atmospheric dispersion and chemical transformation of MEA, and for projections of ground-level air concentrations and deposition rates. In this study, the Weather Research and Forecasting model inline coupled with chemistry, WRF-Chem, was applied to quantify the impact of using a comprehensive MEA photo-oxidation sequence compared to using a simplified MEA scheme. Main discrepancies were found for iminoethanol (roughly doubled in the detailed scheme) and 2-nitro aminoethanol, short MEA-nitramine (reduced by factor of two in the detailed scheme). The study indicates that MEA emissions from a full-scale capture plant can modify regional background levels of isocyanic acid. Predicted atmospheric concentrations of isocyanic acid were however below the limit value of 1 ppbv for ambient exposure. The dependence of the formation of hazardous compounds in the OH-initiated oxidation of MEA on ambient level of nitrogen oxides (NOx) was studied in a scenario without NOx emissions from a refinery area in the vicinity of the capture plant. Hourly MEA-nitramine peak concentrations higher than 40 pg m(-3) did only occur when NOx mixing ratios were above 2 ppbv. Therefore, the spatial variability and temporal variability of levels of OH and NOx need to be taken into account in the health risk assessment. The health risk due to direct emissions of nitrosamines and nitramines from full-scale CO2 capture should be investigated in future studies. Copyright © 2015 Elsevier B.V. All rights reserved.

Carbon Capture and Utilization in the Industrial Sector.

PubMed

Psarras, Peter C; Comello, Stephen; Bains, Praveen; Charoensawadpong, Panunya; Reichelstein, Stefan; Wilcox, Jennifer

2017-10-03

The fabrication and manufacturing processes of industrial commodities such as iron, glass, and cement are carbon-intensive, accounting for 23% of global CO 2 emissions. As a climate mitigation strategy, CO 2 capture from flue gases of industrial processes-much like that of the power sector-has not experienced wide adoption given its high associated costs. However, some industrial processes with relatively high CO 2 flue concentration may be viable candidates to cost-competitively supply CO 2 for utilization purposes (e.g., polymer manufacturing, etc.). This work develops a methodology that determines the levelized cost ($/tCO 2 ) of separating, compressing, and transporting carbon dioxide. A top-down model determines the cost of separating and compressing CO 2 across 18 industrial processes. Further, the study calculates the cost of transporting CO 2 via pipeline and tanker truck to appropriately paired sinks using a bottom-up cost model and geo-referencing approach. The results show that truck transportation is generally the low-cost alternative given the relatively small volumes (ca. 100 kt CO 2 /a). We apply our methodology to a regional case study in Pennsylvania, which shows steel and cement manufacturing paired to suitable sinks as having the lowest levelized cost of capture, compression, and transportation.

Development of environmental impact monitoring protocol for offshore carbon capture and storage (CCS): A biological perspective

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kim, Hyewon, E-mail: hyewon@ldeo.columbia.edu; Kim, Yong Hoon, E-mail: Yong.Kim@rpsgroup.com; Kang, Seong-Gil, E-mail: kangsg@kriso.re.kr

Offshore geologic storage of carbon dioxide (CO{sub 2}), known as offshore carbon capture and sequestration (CCS), has been under active investigation as a safe, effective mitigation option for reducing CO{sub 2} levels from anthropogenic fossil fuel burning and climate change. Along with increasing trends in implementation plans and related logistics on offshore CCS, thorough risk assessment (i.e. environmental impact monitoring) needs to be conducted to evaluate potential risks, such as CO{sub 2} gas leakage at injection sites. Gas leaks from offshore CCS may affect the physiology of marine organisms and disrupt certain ecosystem functions, thereby posing an environmental risk. Here,more » we synthesize current knowledge on environmental impact monitoring of offshore CCS with an emphasis on biological aspects and provide suggestions for better practice. Based on our critical review of preexisting literatures, this paper: 1) discusses key variables sensitive to or indicative of gas leakage by summarizing physico-chemical and ecological variables measured from previous monitoring cruises on offshore CCS; 2) lists ecosystem and organism responses to a similar environmental condition to CO{sub 2} leakage and associated impacts, such as ocean acidification and hypercapnia, to predict how they serve as responsive indicators of short- and long-term gas exposure, and 3) discusses the designs of the artificial gas release experiments in fields and the best model simulation to produce realistic leakage scenarios in marine ecosystems. Based on our analysis, we suggest that proper incorporation of biological aspects will provide successful and robust long-term monitoring strategies with earlier detection of gas leakage, thus reducing the risks associated with offshore CCS. - Highlights: • This paper synthesizes the current knowledge on environmental impact monitoring of offshore Carbon Capture and Sequestration (CCS). • Impacts of CO{sub 2} leakage (ocean acidification, hypercapnia) on marine organisms and ecosystems are discussed. • Insights and recommendations on EIA monitoring for CCS operations are proposed specifically in marine ecosystem perspective.« less

Lithium-functionalized germanene: A promising media for CO2 capture

NASA Astrophysics Data System (ADS)

Mehdi Aghaei, S.; Monshi, M. M.; Torres, I.; Banakermani, M.; Calizo, I.

2018-02-01

Density functional theory (DFT) is employed to investigate the interactions of CO2 gas molecules with pristine and lithium-functionalized germanene. It is discovered that although a single CO2 molecule is weakly physisorbed on pristine germanene, a significant improvement on its adsorption energy is found by utilizing Li-functionalized germanene as the adsorbent. Excitingly, the moderate adsorption energy at high CO2 coverage secures an easy release step. Moreover, the structure of Li-functionalized germanene can be fully recovered after removal of CO2 gas molecules. Our results suggest that Li-functionalized germanene show promise for CO2 sensing and capture with a storage capacity of 12.57 mol/kg.

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 commercial CO2 capture facilities at electric power-generating stations based on the use of monoethanolamine are described, as is the Rectisol process used by Dakota Gasification to separate and capture CO2 from a coal gasifier. Two technologies for storage of the captured CO2 are reviewed--sequestration in deep unmineable coalbeds with concomitant recovery of CH4 and sequestration in deep saline aquifers. Key issues for both of these techniques include estimating the potential storage capacity, the storage integrity, and the physical and chemical processes that are initiated by injecting CO2 underground. Recent studies using computer modeling as well as laboratory and field experimentation are presented here. In addition, several projects have been initiated in which CO2 is injected into a deep coal seam or saline aquifer. The current status of several such projects is discussed. Included is a commercial-scale project in which a million tons of CO2 are injected annually into an aquifer under the North Sea in Norway. The review makes the case that this can all be accomplished safely with off-the-shelf technologies. However, substantial research and development must be performed to reduce the cost, decrease the risks, and increase the safety of sequestration technologies. This review also includes discussion of possible problems related to deep injection of CO2. There are safety concerns that need to be addressed because of the possibilities of leakage to the surface and induced seismic activity. These issues are presented along with a case study of a similar incident in the past. It is clear that monitoring and verification of storage will be a crucial part of all geological sequestration practices so that such problems may be avoided. Available techniques include direct measurement of CO2 and CH4 surface soil fluxes, the use of chemical tracers, and underground 4-D seismic monitoring. Ten new hypotheses were formulated to describe what happens when CO2 is pumped into a coal seam. These hypotheses provide significant insight into the fundamental chemical, physical, and thermodynamic phenomena that occur during coal seam sequestration of CO2.

A first-principles density functional theory study of the electronic structural and thermodynamic properties of M2ZrO3 and M2CO3 (M=Na, K) and their capabilities for CO2 capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yuhua Duan

2012-01-01

Alkali metal zirconates could be used as solid sorbents for CO{sub 2} capture. The structural, electronic, and phonon properties of Na{sub 2}ZrO{sub 3}, K{sub 2}ZrO{sub 3}, Na{sub 2}CO{sub 3}, and K{sub 2}CO{sub 3} are investigated by combining the density functional theory with lattice phonon dynamics. The thermodynamics of CO{sub 2} absorption/desorption reactions of these two zirconates are analyzed. The calculated results show that their optimized structures are in a good agreement with experimental measurements. The calculated band gaps are 4.339 eV (indirect), 3.641 eV (direct), 3.935 eV (indirect), and 3.697 eV (direct) for Na{sub 2}ZrO{sub 3}, K{sub 2}ZrO{sub 3}, Na{submore » 2}CO{sub 3}, and K{sub 2}CO{sub 3}, respectively.The calculated phonon dispersions and phonon density of states for M{sub 2}ZrO{sub 3} and M{sub 2}CO{sub 3} (M = K, Na, Li) revealed that from K to Na to Li, their frequency peaks are shifted to high frequencies due to the molecular weight decreased from K to Li. From the calculated reaction heats and relationships of free energy change versus temperatures and CO{sub 2} pressures of the M{sub 2}ZrO{sub 3} (M = K, Na, Li) reacting with CO{sub 2}, we found that the performance of Na{sub 2}ZrO{sub 3} capturing CO{sub 2} is similar to that of Li{sub 2}ZrO{sub 3} and is better than that of K{sub 2}ZrO{sub 3}. Therefore, Na{sub 2}ZrO{sub 3} and Li{sub 2}ZrO{sub 3} are good candidates of high temperature CO{sub 2} sorbents and could be used for post combustion CO{sub 2} capture technologies.« less

Comparaison de la performance environnementale de la production thermique d'electricite avec et sans sequestration geologique du dioxyde de carbone

NASA Astrophysics Data System (ADS)

Bellerive, Nathalie

The research project hypothesis is that CO2 capture and sequestration technologies (CSC) leads to a significant decrease in global warming, but increases the impact of all other aspects of the study. This is because other processes used for CO2 capture and sequestration require additional quantities of raw materials and energy. Two other objectives are described in this project. The first is the modeling of an Integrated Gasification Combined Cycle power plant for which there is no known generic data. The second is to select the right hypothesis regarding electrical production technologies, CO2 capture, compression and transportation by pipeline and finally sequestration. "Life Cycle Assessment" (LCA) analyses were chosen for this research project. LCA is an exhaustive quantitative method used to evaluate potential environmental impacts associated with a product, a service or an activity from resource extraction to waste elimination. This tool is governed by ISO 14 040 through ISO 14 049 and is sustained by the Society of Environmental Toxicology and Chemistry (SETAC) and the United Nations Environment Program (UNEP). Two power plants were studied, the Integrated Gasification Combined Cycle (IGCC) power plant and the Natural Gas Combined Cycle (NGCC) power plant. In order to sequester CO2 in geological formation, it is necessary to extract CO2from emission flows. For the IGCC power plant, CO 2 was captured before the burning phase. For the NGCC power plant, the capture was done during the afterburning phase. Once the CO2 was isolated, it was compressed and directed through a transportation pipe 1 000 km in length on the ground surface and in the sea. It is hypothesized that the power plant is 300 km from the shore and the sequestration platform 700 km from France's shore, in the North Sea. The IGCC power plant modeling and data selection regarding CO2 capture and sequestration were done by using primary data from the industry and the Ecoinvent generic database (Version 1.2). This database was selected due to its European source. Finally, technical calculations and literature were used to complete the data inventory. This was validated by electrical experts in order to increase data and modeling precision. Results were similar for IGCC and NGCC power plants using Impact 2002+, an impacts analysis method. Global warming potential decreased by 67% with the implementation of CO2 capture and sequestration compared to systems without CSC. Results for all others impacts categories, demonstrated an increase from 16% to 116% in relative proportions compared to systems without CSC. The main contributor was the additional quantity of energy required to operate CO2 capture and compression facilities. This additional energy negatively affected the power plant's global efficiency because of the increase in the quantity of fossil fuel that needed to be extracted and consumed. The increase in other impacts was mainly due to additional electricity, fossil fuel (for extracting, treatment and transportation) and additional emissions generated during power plant operations. A scenario analysis was done to study the sensitivity and variability of uncertain data during the software modeling process of a power plant. Data on power plant efficiency is the most variable and sensitive during modeling, followed by the length of the transportation pipe and the leaking rate during CO2 sequestration. This result analysis is interesting because it led to the maximum efficiency scenario with capture (with a short CO 2 transportation distance and a low leaking rate) obtaining better results on all impact category indicators, compared to the minimum efficiency scenario without capture. In fact, positive results on all category indicators were possible during the system comparison between the two cases (with and without capture). (Abstract shortened by UMI.)

Role of amine structure on carbon dioxide adsorption from ultradilute gas streams such as ambient air.

PubMed

Didas, Stephanie A; Kulkarni, Ambarish R; Sholl, David S; Jones, Christopher W

2012-10-01

A fundamental study on the adsorption properties of primary, secondary, and tertiary amine materials is used to evaluate what amine type(s) are best suited for ultradilute CO(2) capture applications. A series of comparable materials comprised of primary, secondary, or tertiary amines ligated to a mesoporous silica support via a propyl linker are used to systematically assess the role of amine type. Both CO(2) and water adsorption isotherms are presented for these materials in the range relevant to CO(2) capture from ambient air and it is demonstrated that primary amines are the best candidates for CO(2) capture from air. Primary amines possess both the highest amine efficiency for CO(2) adsorption as well as enhanced water affinity compared to other amine types or the bare silica support. The results suggest that the rational design of amine adsorbents for the extraction of CO(2) from ambient air should focus on adsorbents rich in primary amines. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Carbon Dioxide Separation from Flue Gases: A Technological Review Emphasizing Reduction in Greenhouse Gas Emissions

PubMed Central

Songolzadeh, Mohammad; Soleimani, Mansooreh; Takht Ravanchi, Maryam; Songolzadeh, Reza

2014-01-01

Increasing concentrations of greenhouse gases (GHGs) such as CO2 in the atmosphere is a global warming. Human activities are a major cause of increased CO2 concentration in atmosphere, as in recent decade, two-third of greenhouse effect was caused by human activities. Carbon capture and storage (CCS) is a major strategy that can be used to reduce GHGs emission. There are three methods for CCS: pre-combustion capture, oxy-fuel process, and post-combustion capture. Among them, post-combustion capture is the most important one because it offers flexibility and it can be easily added to the operational units. Various technologies are used for CO2 capture, some of them include: absorption, adsorption, cryogenic distillation, and membrane separation. In this paper, various technologies for post-combustion are compared and the best condition for using each technology is identified. PMID:24696663

Carbon dioxide separation from flue gases: a technological review emphasizing reduction in greenhouse gas emissions.

PubMed

Songolzadeh, Mohammad; Soleimani, Mansooreh; Takht Ravanchi, Maryam; Songolzadeh, Reza

2014-01-01

Increasing concentrations of greenhouse gases (GHGs) such as CO2 in the atmosphere is a global warming. Human activities are a major cause of increased CO2 concentration in atmosphere, as in recent decade, two-third of greenhouse effect was caused by human activities. Carbon capture and storage (CCS) is a major strategy that can be used to reduce GHGs emission. There are three methods for CCS: pre-combustion capture, oxy-fuel process, and post-combustion capture. Among them, post-combustion capture is the most important one because it offers flexibility and it can be easily added to the operational units. Various technologies are used for CO2 capture, some of them include: absorption, adsorption, cryogenic distillation, and membrane separation. In this paper, various technologies for post-combustion are compared and the best condition for using each technology is identified.

High capacity immobilized amine sorbents

DOEpatents

Gray, McMahan L [Pittsburgh, PA; Champagne, Kenneth J [Fredericktown, PA; Soong, Yee [Monroeville, PA; Filburn, Thomas [Granby, CT

2007-10-30

A method is provided for making low-cost CO.sub.2 sorbents that can be used in large-scale gas-solid processes. The improved method entails treating an amine to increase the number of secondary amine groups and impregnating the amine in a porous solid support. The method increases the CO.sub.2 capture capacity and decreases the cost of utilizing an amine-enriched solid sorbent in CO.sub.2 capture systems.

Absorber modeling for NGCC carbon capture with aqueous piperazine.

PubMed

Zhang, Yue; Freeman, Brice; Hao, Pingjiao; Rochelle, Gary T

2016-10-20

A hybrid system combining amine scrubbing with membrane technology for carbon capture from natural gas combined cycle (NGCC) power plants is proposed in this paper. In this process, the CO 2 in the flue gas can be enriched from 4% to 18% by the membrane, and the amine scrubbing system will have lower capture costs. Aqueous piperazine (PZ) is chosen as the solvent. Different direct contact cooler (DCC) options, multiple absorber operating conditions, optimal intercooling designs, and different cooling options have been evaluated across a wide range of inlet CO 2 . Amine scrubbing without DCC is a superior design for NGCC carbon capture. Pump-around cooling at the bottom of the absorber can effectively manage the temperature of the hot flue gas, and still be effective for CO 2 absorption. The absorber gas inlet must be designed to avoid excessive localized temperature and solvent evaporation. When the inlet CO 2 increases from 4% to 18%, total absorber CAPEX decreases by 60%; another 10% of the total absorber CAPEX can be saved by eliminating the DCC. In-and-out intercooling works well for high CO 2 , while pump-around intercooling is more effective for low CO 2 . Dry cooling requires more packing and energy but appears to be technically and economically feasible if cooling water availability is limited.

Effects of heat exchanger tubes on hydrodynamics and CO 2 capture of a sorbent-based fluidized bed reactor

DOE PAGES

Lai, Canhai; Xu, Zhijie; Li, Tingwen; ...

2017-08-05

In virtual design and scale up of pilot-scale carbon capture systems, the coupled reactive multiphase flow problem must be solved to predict the adsorber's performance and capture efficiency under various operation conditions. This paper focuses on the detailed computational fluid dynamics (CFD) modeling of a pilot-scale fluidized bed adsorber equipped with vertical cooling tubes. Multiphase Flow with Interphase eXchanges (MFiX), an open-source multiphase flow CFD solver, is used for the simulations with custom code to simulate the chemical reactions and filtered sub-grid models to capture the effect of the unresolved details in the coarser mesh for simulations with reasonable accuracymore » and manageable computational effort. Previously developed filtered models for horizontal cylinder drag, heat transfer, and reaction kinetics have been modified to derive the 2D filtered models representing vertical cylinders in the coarse-grid CFD simulations. The effects of the heat exchanger configurations (i.e., horizontal or vertical tubes) on the adsorber's hydrodynamics and CO 2 capture performance are then examined. A one-dimensional three-region process model is briefly introduced for comparison purpose. The CFD model matches reasonably well with the process model while provides additional information about the flow field that is not available with the process model.« less

Carbon Capture: A Technology Assessment

DTIC Science & Technology

2013-10-21

gases produced at power plants burning coal or natural gas. Here, the captured CO2 is sold as a commodity to nearby industries such as food ...the food and beverage industry.19 A number of vendors currently offer commercial amine-based processes, including the Fluor Daniel Econamine FG Plus...Sleipner West Gas Field (North Sea, Norway) Natural gas separation 1996 N/A Amine (Aker) 1.0 Petronas Gas Processing Plant (Kuala Lumpur, Malaysia

Diamine-Functionalization of a Metal-Organic Framework Adsorbent for Superb Carbon Dioxide Adsorption and Desorption Properties.

PubMed

Lee, Woo Ram; Kim, Jeong Eun; Lee, Sung Jin; Kang, Minjung; Kang, Dong Won; Lee, Hwa Young; Hiremath, Vishwanath; Seo, Jeong Gil; Jin, Hailian; Moon, Dohyun; Cho, Moses; Jung, Yousung; Hong, Chang Seop

2018-05-25

For real-world postcombustion applications in the mitigation of CO 2 emissions using dry sorbents, adsorption and desorption behaviors should be controlled to design and fabricate prospective materials with optimal CO 2 performances. Herein, we prepared diamine-functionalized Mg 2 (dobpdc) (H 4 dobpdc=4,4'-dihydroxy-(1,1'-biphenyl)-3,3'-dicarboxylic acid). (1-diamine) with ethylenediamine (en), primary-secondary (N-ethylethylenediamine-een and N-isopropylethylenediamine-ipen), primary-tertiary, and secondary-secondary diamines. A slight alteration of the number of alkyl substituents on the diamines and their alkyl chain length dictates the desorption temperature (T des ) at 100 % CO 2 , desorption characteristics, and ΔT systematically to result in the tuning of the working capacity. The existence of bulky substituents on the diamines improves the framework stability upon exposure to O 2 , SO 2 , and water vapor, relevant to real flue-gas conditions. Bulky substituents are also responsible for an interesting two-step behavior observed for the ipen case, as revealed by DFT calculations. Among the diamine-appended metal-organic frameworks, 1-een, which has the required adsorption and desorption properties, is a promising material for sorbent-based CO 2 capture processes. Hence, CO 2 performance and framework durability can be tailored by the judicial selection of the diamine structure, which enables property design at will and facilitates the development of desirable CO 2 -capture materials. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

UOP; Honeywell Resins & Chemicals; Honeywell Process Solutions

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 wasmore » 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 conductivity sensors is suitable for process control of algae cultivation in an open pond systems. This project concluded that the Hopewell wastewater is very suitable for algal cultivation but the potential for significant CO2 sequestration from the plant stack gas emissions was minimal due to the high endogenous CO2 generation in the wastewater from the organic wastewater content. Algae cultivation was found to be promising, however, for nitrogen remediation in the Hopewell wastewater.« less

Environmental potential of the use of CO2 from alcoholic fermentation processes. The CO2-AFP strategy.

PubMed

Alonso-Moreno, Carlos; García-Yuste, Santiago

2016-10-15

A novel Carbon Dioxide Utilization (CDU) approach from a relatively minor CO2 emission source, i.e., alcoholic fermentation processes (AFP), is presented. The CO2 produced as a by-product from the AFP is estimated by examining the EtOH consumed per year reported by the World Health Organization in 2014. It is proposed that the extremely pure CO2 from the AFP is captured in NaOH solutions to produce one of the Top 10 commodities in the chemical industry, Na2CO3, as a good example of an atomic economy process. The novel CDU strategy could yield over 30.6Mt of Na2CO3 in oversaturated aqueous solution on using ca. 12.7Mt of captured CO2 and this process would consume less energy than the synthetic methodology (Solvay ammonia soda process) and would not produce low-value by-products. The quantity of Na2CO3 obtained by this strategy could represent ca. 50% of the world Na2CO3 production in one year. In terms of the green economy, the viability of the strategy is discussed according to the recommendations of the CO2Chem network, and an estimation of the CO2negative emission achieved suggests a capture of around 280.0Mt of CO2 from now to 2020 or ca. 1.9Gt from now to 2050. Finally, the results obtained for this new CDU proposal are discussed by considering different scenarios; the CO2 production in a typical winemaking corporation, the CO2 released in the most relevant wine-producing countries, and the use of CO2 from AFP as an alternative for the top Na2CO3-producing countries. Copyright © 2016 Elsevier B.V. All rights reserved.

Synthesis of sintering-resistant sorbents for CO2 capture.

PubMed

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

2010-04-15

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

Application of halloysite nanotubes for carbon dioxide capture

NASA Astrophysics Data System (ADS)

Kim, Jinsoo; Rubino, Ilaria; Lee, Joo-Youp; Choi, Hyo-Jick

2016-04-01

Halloysite is a naturally occurring clay, with physical structure represented by halloysite nanotubes (HNTs). We investigated the potential applicability of HNTs for carbon dioxide (CO2) capture, using two amine-functionalized HNTs: (3-aminopropyl) triethoxysilane (APTES)-grafted HNTs and polyethylenimine (PEI)-impregnated HNTs. APTES-HNTs and PEI-HNTs resulted in 5.6 and 30 wt. % (in sorbent) in functionalization onto HNTs, respectively. Capture efficiency was higher in APTES-HNTs at lower temperatures, while it was maximum in PEI-HNTs at 70°C-75 °C. At 75 °C, adsorption/desorption tests showed that 95% of the two reactions occurred within 30 min, and exhibited 0.15 and 0.21 millimole of CO2 adsorption capacity per millimole of amine group for APTES-HNTs and PEI-HNTs, respectively. During 10 cycles of CO2 adsorption/desorption, there was no significant decrease in sorbent weight and adsorption capacity in both HNTs. These results show that inherent structural features of HNTs can be easily tailored for the development of operational condition-specific CO2 capture system.

Asphalt-derived high surface area activated porous carbons for carbon dioxide capture.

PubMed

Jalilov, Almaz S; Ruan, Gedeng; Hwang, Chih-Chau; Schipper, Desmond E; Tour, Josiah J; Li, Yilun; Fei, Huilong; Samuel, Errol L G; Tour, James M

2015-01-21

Research activity toward the development of new sorbents for carbon dioxide (CO2) capture have been increasing quickly. Despite the variety of existing materials with high surface areas and high CO2 uptake performances, the cost of the materials remains a dominant factor in slowing their industrial applications. Here we report preparation and CO2 uptake performance of microporous carbon materials synthesized from asphalt, a very inexpensive carbon source. Carbonization of asphalt with potassium hydroxide (KOH) at high temperatures (>600 °C) yields porous carbon materials (A-PC) with high surface areas of up to 2780 m(2) g(-1) and high CO2 uptake performance of 21 mmol g(-1) or 93 wt % at 30 bar and 25 °C. Furthermore, nitrogen doping and reduction with hydrogen yields active N-doped materials (A-NPC and A-rNPC) containing up to 9.3% nitrogen, making them nucleophilic porous carbons with further increase in the Brunauer-Emmett-Teller (BET) surface areas up to 2860 m(2) g(-1) for A-NPC and CO2 uptake to 26 mmol g(-1) or 114 wt % at 30 bar and 25 °C for A-rNPC. This is the highest reported CO2 uptake among the family of the activated porous carbonaceous materials. Thus, the porous carbon materials from asphalt have excellent properties for reversibly capturing CO2 at the well-head during the extraction of natural gas, a naturally occurring high pressure source of CO2. Through a pressure swing sorption process, when the asphalt-derived material is returned to 1 bar, the CO2 is released, thereby rendering a reversible capture medium that is highly efficient yet very inexpensive.

Potentiel des méthodes de séparation et stockage du CO2 dans la lutte contre l'effet de serreThe role of CO2 capture and sequestration in mitigation of climate change

NASA Astrophysics Data System (ADS)

Jean-Baptiste, Philippe; Ducroux, René

2003-06-01

Increasing atmospheric level of greenhouse gases are causing global warming and putting at risk the global climate system. The main anthropogenic greenhouse gas is CO 2. Technical solutions exist to reduce CO 2 emission and stabilise atmospheric CO 2 concentration, including energy saving and energy efficiency, switch to lower carbon content fuels like natural gas and to energy sources that operate with zero CO 2 emissions such as renewable or nuclear energy, enhance the natural sinks for CO 2 (forests, soils, etc.), and last but not least, sequester CO 2 from fossil fuels combustion. The purpose of this paper is to provide an overview of the technology and cost for capture and storage of CO 2. Some of the factors that will influence application, including environmental impact, cost and efficiency, are also discussed. Capturing CO 2 and storing it in underground geological reservoirs appears as the best environmentally acceptable option. It can be done with existing technology; however, substantial R&D is needed to improve available technology and to lower the cost. Applicable to large CO 2 emitting industrial facilities such as power plants, cement factories, steel industry, etc., which amount to more than 30% of the global anthropogenic CO 2 emission, it represents a valuable tool in the battle against global warming. To cite this article: P. Jean-Baptiste, R. Ducroux, C. R. Geoscience 335 (2003).

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.

Enhancements in mass transfer for carbon capture solvents part I: Homogeneous catalyst

DOE PAGES

Widger, Leland R.; Sarma, Moushumi; Bryant, Jonathan J.; ...

2017-06-15

The novel small molecule carbonic anhydrase (CA) mimic [Co III(Salphen-COO -)Cl]HNEt 3 ( 1), was synthesized as an additive for increasing CO 2 absorption rates in amine-based post-combustion carbon capture processes (CCS), and its efficacy was verified. 1 was designed for use in a kinetically slow but thermally stable blended solvent, containing the primary amines 1-amino-2-propanol (A2P) and 2-amino-2-methyl-1-propanol (AMP). Together, the A2P/AMP solvent and 1 reduce the overall energy penalty associated with CO 2 capture from coal-derived flue gas, relative to the baseline solvent MEA. 1 is also effective at increasing absorption kinetics of kinetically fast solvents, such asmore » MEA, which can reduce capital costs by requiring a smaller absorber tower. The transition from catalyst testing under idealized laboratory conditions, to process relevant lab- and bench-scale testing adds many additional variables that are not well understood and rarely discussed. As a result, the stepwise testing of both 1 and the novel A2P/AMP solvent blend is described through a transition process that identifies many of these process and evaluation challenges not often addressed when designing a chemical or catalytic additive for industrial CCS systems, where consideration of solvent chemistry is typically the primary goal.« less

Enhancements in mass transfer for carbon capture solvents part II: Micron-sized solid particles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mannel, David S.; Qi, Guojie; Widger, Leland R.

2017-06-01

The novel small molecule carbonic anhydrase (CA) mimic [CoIII(Salphen-COO-)Cl]HNEt3 (1), was synthesized as an additive for increasing CO2 absorption rates in amine-based post-combustion carbon capture processes (CCS), and its efficacy was verified. 1 was designed for use in a kinetically slow but thermally stable blended solvent, containing the primary amines 1-amino-2-propanol (A2P) and 2-amino-2-methyl-1-propanol (AMP). Together, the A2P/AMP solvent and 1 reduce the overall energy penalty associated with CO2 capture from coal-derived flue gas, relative to the baseline solvent MEA. 1 is also effective at increasing absorption kinetics of kinetically fast solvents, such as MEA, which can reduce capital costsmore » by requiring a smaller absorber tower. The transition from catalyst testing under idealized laboratory conditions, to process relevant lab- and bench-scale testing adds many additional variables that are not well understood and rarely discussed. The stepwise testing of both 1 and the novel A2P/AMP solvent blend is described through a transition process that identifies many of these process and evaluation challenges not often addressed when designing a chemical or catalytic additive for industrial CCS systems, where consideration of solvent chemistry is typically the primary goal.« less

The fabrication of porous N-doped carbon from widely available urea formaldehyde resin for carbon dioxide adsorption.

PubMed

Liu, Zhen; Du, Zhenyu; Song, Hao; Wang, Chuangye; Subhan, Fazle; Xing, Wei; Yan, Zifeng

2014-02-15

N-doped carbon material constitutes abundant of micropores and basic nitrogen species that have potential implementation for CO2 capture. In this paper, porous carbon material with high nitrogen content was simply fabricated by carbonizing low cost and widely available urea formaldehyde resin, and then followed by KOH activation. CO2 capture experiment showed high adsorption capacity of 3.21 mmol g(-1) at 25 °C under 1 atm for UFCA-2-600. XRD, SEM, XPS and FT-IR analysis confirmed that a graphitic-like structure was retained even after high temperature carbonization and strong base activation. Textural property analysis revealed that narrow micropores, especially below 0.8 nm, were effective for CO2 adsorption by physical adsorption mechanism. Chemical evolved investigation revealed that graphitic-like embedded basic nitrogen groups are generated from bridged and terminal amines of urea formaldehyde resin from thermal carbonization and KOH activation treatment, which is responsible for the enrichment of CO2 capacity by chemical adsorption mechanism. The relationship between CO2 adsorption capacity and pore size or basic N species was also studied, which turned out that both of them played crucial role by physical and chemical adsorption mechanism, respectively. Copyright © 2013 Elsevier Inc. All rights reserved.

Particulate Formation from a Copper Oxide-Based Oxygen Carrier in Chemical Looping Combustion for CO2 Capture

EPA Science Inventory

Attrition behavior and particle loss of a copper oxide-based oxygen carrier from a methane chemical looping combustion (CLC) process was investigated in a fluidized bed reactor. The aerodynamic diameters of most elutriated particulates, after passing through a horizontal settling...

Scoping Alternatives for Negative Emission Technologies. FRACCC - Possible Routes to Biomass-Derived Carbon Injection in Shallow Aquifers?

NASA Astrophysics Data System (ADS)

Correa Silva, R.; Larter, S.

2016-12-01

Atmospheric CO2 capture into biomass is one of the capture options for negative emission technologies, although proposed sequestration systems such as the permanent burial of total fresh biomass, algal lipids or soil amendment with biochar are yet to be successfully demonstrated as effective at scale. In the context of carbon sequestration, shallow geological reservoirs have not been exhaustively explored, even though they pose, away from groundwater protection zones, potentially low implementation cost, and geographically abundant potential carbon storage reservoirs. Typical carbon storage vectors considered, such as CO2 and biochar, are not suitable for shallow aquifer disposal, due either to cap rock containment requirements, or shallow aquifer CO2 densities, or issues related to formation damage from solid particles. Thus, a cost-effective technology, aimed at converting biomass into a large-scale carbon vector fit-for-disposal in shallow formations could be significant, linking promising carbon capture and containment strategies. In this work, we discuss the development of unconventional carbon vectors for subsurface storage in the form of Functionalized, Refractory and Aqueous Compatible Carbon Compounds (FRACCC), as a potential alternative negative emission technology (Larter et al., 2010). The concept is based on CO2 capture into microbial and algal biomass, followed by the modification of biomass constituents through facile chemical reactions aimed at rendering the biomass efficiently into a stable, biologically refractory but water soluble form, similar in some regards, to dissolved organic matter in the oceans, then sequestering the material in geological settings. As the injected material is not buoyant, containment specifications are more modest than for CO2 injection and potentially, more reservoirs could be accessible! This work analyses the technological, economic and societal implications of such potential FRACCC technologies, and make an assessment of whether such routes are likely to be technically, economically and politically viable.

NRG CO 2NCEPT - Confirmation Of Novel Cost-effective Emerging Post-combustion Technology

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stevenson, Matthew; Armpriester, Anthony

Under DOE's solicitation DE-FOA-0001190, NRG and Inventys conceptualized a Large-Scale pilot (>10MWe) post-combustion CO 2 capture project using Inventys' VeloxoThermTM carbon capture technology. The technology is comprised of an intensified thermal swing adsorption (TSA) process that uses a patented architecture of structured adsorbent and a novel process design and embodiment to capture CO 2 from industrial flue gas streams. The result of this work concluded that the retrofit of this technology is economically and technically viable, but that the sorbent material selected for the program would need improving to meet the techno-economic performance requirements of the solicitation.

The thiocyanate anion is a primary driver of carbon dioxide capture by ionic liquids

NASA Astrophysics Data System (ADS)

Chaban, Vitaly

2015-01-01

Carbon dioxide, CO2, capture by room-temperature ionic liquids (RTILs) is a vivid research area featuring both accomplishments and frustrations. This work employs the PM7-MD method to simulate adsorption of CO2 by 1,3-dimethylimidazolium thiocyanate at 300 K. The obtained result evidences that the thiocyanate anion plays a key role in gas capture, whereas the impact of the 1,3-dimethylimidazolium cation is mediocre. Decomposition of the computed wave function on the individual molecular orbitals confirms that CO2-SCN binding extends beyond just expected electrostatic interactions in the ion-molecular system and involves partial sharing of valence orbitals.

Improving ecophysiological simulation models to predict the impact of elevated atmospheric CO2 concentration on crop productivity

PubMed Central

Yin, Xinyou

2013-01-01

Background Process-based ecophysiological crop models are pivotal in assessing responses of crop productivity and designing strategies of adaptation to climate change. Most existing crop models generally over-estimate the effect of elevated atmospheric [CO2], despite decades of experimental research on crop growth response to [CO2]. Analysis A review of the literature indicates that the quantitative relationships for a number of traits, once expressed as a function of internal plant nitrogen status, are altered little by the elevated [CO2]. A model incorporating these nitrogen-based functional relationships and mechanisms simulated photosynthetic acclimation to elevated [CO2], thereby reducing the chance of over-estimating crop response to [CO2]. Robust crop models to have small parameterization requirements and yet generate phenotypic plasticity under changing environmental conditions need to capture the carbon–nitrogen interactions during crop growth. Conclusions The performance of the improved models depends little on the type of the experimental facilities used to obtain data for parameterization, and allows accurate projections of the impact of elevated [CO2] and other climatic variables on crop productivity. PMID:23388883

Process modeling of an advanced NH₃ abatement and recycling technology in the ammonia-based CO₂ capture process.

PubMed

Li, Kangkang; Yu, Hai; Tade, Moses; Feron, Paul; Yu, Jingwen; Wang, Shujuan

2014-06-17

An advanced NH3 abatement and recycling process that makes great use of the waste heat in flue gas was proposed to solve the problems of ammonia slip, NH3 makeup, and flue gas cooling in the ammonia-based CO2 capture process. The rigorous rate-based model, RateFrac in Aspen Plus, was thermodynamically and kinetically validated by experimental data from open literature and CSIRO pilot trials at Munmorah Power Station, Australia, respectively. After a thorough sensitivity analysis and process improvement, the NH3 recycling efficiency reached as high as 99.87%, and the NH3 exhaust concentration was only 15.4 ppmv. Most importantly, the energy consumption of the NH3 abatement and recycling system was only 59.34 kJ/kg CO2 of electricity. The evaluation of mass balance and temperature steady shows that this NH3 recovery process was technically effective and feasible. This process therefore is a promising prospect toward industrial application.

Response surface method for modeling the removal of carbon dioxide from a simulated gas using water absorption enhanced with a liquid-film-forming device.

PubMed

Nguyen, Diem-Mai Kim; Imai, Tsuyoshi; Dang, Thanh-Loc Thi; Kanno, Ariyo; Higuchi, Takaya; Yamamoto, Koichi; Sekine, Masahiko

2018-03-01

This paper presents the results from using a physical absorption process to absorb gaseous CO 2 mixed with N 2 using water by producing tiny bubbles via a liquid-film-forming device (LFFD) that improves the solubility of CO 2 in water. The influence of various parameters-pressure, initial CO 2 concentration, gas-to-liquid ratios, and temperature-on the CO 2 removal efficiency and its absorption rate in water were investigated and estimated thoroughly by statistical polynomial models obtained by the utilization of the response surface method (RSM) with a central composite design (CCD). Based on the analysis, a high efficiency of CO 2 capture can be reached in conditions such as low pressure, high CO 2 concentration at the inlet, low gas/liquid ratio, and low temperature. For instance, the highest removal efficiency in the RSM-CCD experimental matrix of nearly 80% occurred for run number 20, which was conducted at 0.30MPa, CO 2 concentration of 35%, gas/liquid ratio of 0.71, and temperature of 15°C. Furthermore, the coefficients of determination, R 2 , were 0.996 for the removal rate and 0.982 for the absorption rate, implying that the predicted values computed by the constructed models correlate strongly and fit well with the experimental values. The results obtained provide essential information for implementing this method properly and effectively and contribute a promising approach to the problem of CO 2 capture in air pollution treatment. Copyright © 2017. Published by Elsevier B.V.

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

PubMed

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

2015-09-15

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

Geophysical monitoring technology for CO2 sequestration

NASA Astrophysics Data System (ADS)

Ma, Jin-Feng; Li, Lin; Wang, Hao-Fan; Tan, Ming-You; Cui, Shi-Ling; Zhang, Yun-Yin; Qu, Zhi-Peng; Jia, Ling-Yun; Zhang, Shu-Hai

2016-06-01

Geophysical techniques play key roles in the measuring, monitoring, and verifying the safety of CO2 sequestration and in identifying the efficiency of CO2-enhanced oil recovery. Although geophysical monitoring techniques for CO2 sequestration have grown out of conventional oil and gas geophysical exploration techniques, it takes a long time to conduct geophysical monitoring, and there are many barriers and challenges. In this paper, with the initial objective of performing CO2 sequestration, we studied the geophysical tasks associated with evaluating geological storage sites and monitoring CO2 sequestration. Based on our review of the scope of geophysical monitoring techniques and our experience in domestic and international carbon capture and sequestration projects, we analyzed the inherent difficulties and our experiences in geophysical monitoring techniques, especially, with respect to 4D seismic acquisition, processing, and interpretation.

Liquid Hydrocarbon Production from CO2 : Recent Development in Metal-Based Electrocatalysis.

PubMed

Daiyan, Rahman; Lu, Xunyu; Ng, Yun Hau; Amal, Rose

2017-11-23

Rising levels of CO 2 accumulation in the atmosphere have attracted considerable interest in technologies capable of CO 2 capture, storage and conversion. The electrochemical reduction of CO 2 into high-value liquid organic products could be of vital importance to mitigate this issue. The conversion of CO 2 into liquid fuels by using photovoltaic cells, which can readily be integrated in the current infrastructure, will help realize the creation of a sustainable cycle of carbon-based fuel that will promote zero net CO 2 emissions. Despite promising findings, significant challenges still persist that must be circumvented to make the technology profitable for large-scale utilization. With such possibilities, this Minireview presents the current high-performing catalysts for the electrochemical reduction of CO 2 to liquid hydrocarbons, address the limitations and unify the current understanding of the different reaction mechanisms. The Minireview also explores current research directions to improve process efficiencies and production rate and discusses the scope of using photo-assisted electrochemical reduction systems to find stable, highly efficient catalysts that can harvest solar energy directly to convert CO 2 into liquid hydrocarbons. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Process for CO.sub.2 capture using a regenerable magnesium hydroxide sorbent

DOEpatents

Siriwardane, Ranjani V; Stevens, Jr., Robert W

2013-06-25

A process for CO.sub.2 separation using a regenerable Mg(OH).sub.2 sorbent. The process absorbs CO.sub.2 through the formation of MgCO.sub.3 and releases water product H.sub.2O. The MgCO.sub.3 is partially regenerated through direct contact with steam, which acts to heat the magnesium carbonate to a higher temperature, provide heat duty required to decompose the magnesium carbonate to yield MgO and CO.sub.2, provide an H.sub.2O environment over the magnesium carbonate thereby shifting the equilibrium and increasing the potential for CO.sub.2 desorption, and supply H.sub.2O for rehydroxylation of a portion of the MgO. The mixture is polished in the absence of CO.sub.2 using water product H.sub.2O produced during the CO.sub.2 absorption to maintain sorbent capture capacity. The sorbent now comprised substantially of Mg(OH).sub.2 is then available for further CO.sub.2 absorption duty in a cyclic process.

A portable molecular-sieve-based CO2 sampling system for radiocarbon measurements

NASA Astrophysics Data System (ADS)

Palonen, V.

2015-12-01

We have developed a field-capable sampling system for the collection of CO2 samples for radiocarbon-concentration measurements. Most target systems in environmental research are limited in volume and CO2 concentration, making conventional flask sampling hard or impossible for radiocarbon studies. The present system captures the CO2 selectively to cartridges containing 13X molecular sieve material. The sampling does not introduce significant under-pressures or significant losses of moisture to the target system, making it suitable for most environmental targets. The system also incorporates a significantly larger sieve container for the removal of CO2 from chambers prior to the CO2 build-up phase and sampling. In addition, both the CO2 and H2O content of the sample gas are measured continuously. This enables in situ estimation of the amount of collected CO2 and the determination of CO2 flux to a chamber. The portable sampling system is described in detail and tests for the reliability of the method are presented.

A portable molecular-sieve-based CO2 sampling system for radiocarbon measurements.

PubMed

Palonen, V

2015-12-01

We have developed a field-capable sampling system for the collection of CO2 samples for radiocarbon-concentration measurements. Most target systems in environmental research are limited in volume and CO2 concentration, making conventional flask sampling hard or impossible for radiocarbon studies. The present system captures the CO2 selectively to cartridges containing 13X molecular sieve material. The sampling does not introduce significant under-pressures or significant losses of moisture to the target system, making it suitable for most environmental targets. The system also incorporates a significantly larger sieve container for the removal of CO2 from chambers prior to the CO2 build-up phase and sampling. In addition, both the CO2 and H2O content of the sample gas are measured continuously. This enables in situ estimation of the amount of collected CO2 and the determination of CO2 flux to a chamber. The portable sampling system is described in detail and tests for the reliability of the method are presented.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zheng, Feng; Heldebrant, David J.; Mathias, Paul M.

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

Doping of alkali, alkaline-earth, and transition metals in covalent-organic frameworks for enhancing CO2 capture by first-principles calculations and molecular simulations.

PubMed

Lan, Jianhui; Cao, Dapeng; Wang, Wenchuan; Smit, Berend

2010-07-27

We use the multiscale simulation approach, which combines the first-principles calculations and grand canonical Monte Carlo simulations, to comprehensively study the doping of a series of alkali (Li, Na, and K), alkaline-earth (Be, Mg, and Ca), and transition (Sc and Ti) metals in nanoporous covalent organic frameworks (COFs), and the effects of the doped metals on CO2 capture. The results indicate that, among all the metals studied, Li, Sc, and Ti can bind with COFs stably, while Be, Mg, and Ca cannot, because the binding of Be, Mg, and Ca with COFs is very weak. Furthermore, Li, Sc, and Ti can improve the uptakes of CO2 in COFs significantly. However, the binding energy of a CO2 molecule with Sc and Ti exceeds the lower limit of chemisorptions and, thus, suffers from the difficulty of desorption. By the comparative studies above, it is found that Li is the best surface modifier of COFs for CO2 capture among all the metals studied. Therefore, we further investigate the uptakes of CO2 in the Li-doped COFs. Our simulation results show that at 298 K and 1 bar, the excess CO2 uptakes of the Li-doped COF-102 and COF-105 reach 409 and 344 mg/g, which are about eight and four times those in the nondoped ones, respectively. As the pressure increases to 40 bar, the CO2 uptakes of the Li-doped COF-102 and COF-105 reach 1349 and 2266 mg/g at 298 K, respectively, which are among the reported highest scores to date. In summary, doping of metals in porous COFs provides an efficient approach for enhancing CO2 capture.

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

Ionic liquid-impregnated activated carbon for biohydrogen purification in an adsorption unit

NASA Astrophysics Data System (ADS)

Yusuf, N. Y.; Masdar, M. S.; Isahak, W. N. R. W.; Nordin, D.; Husaini, T.; Majlan, E. H.; Rejab, S. A. M.; Chew, C. L.

2017-06-01

Biological methods for hydrogen production (biohydrogen) are known as energy intensive and can be operated at ambient temperature and pressure; however, consecutive productions such as purification and separation processes still remain challenging in the industry. Various techniques are used to purify and separate hydrogen. These techniques include the use of sorbents/solvents, membranes and cryogenic distillation. In this study, carbon dioxide (CO2) was purified and separated from biohydrogen to produce high purity hydrogen gas. CO2 capture was studied using the activated carbon (AC) modified with the ionic liquid (IL) choline chloride as adsorbent. The physical and chemical properties of the adsorbents were characterized through XRD, FTIR, SEM-EDX, TGA, and BET analyses. The effects of IL loading, flow rate, temperature, and gas mixture were also investigated based on the absorption and desorption of CO2. The CO2 level in the biohydrogen composition was analyzed using a CO2 gas analyzer. The SEM image indicated that the IL homogeneously covered the AC surface. High IL dispersion inlet enhanced the capability of the adsorbent to capture CO2 gas. The thermal stability and presence of the functionalized group of ILs on AC were analyzed by TGA and FTIR techniques, respectively. CO2 adsorption experiments were conducted using a 1 L adsorber unit. Hence, adsorption technologies exhibit potential for biohydrogen purification and mainly affected by adsorbent ability and operating parameters. This research presents an improved biohydrogen technique based on adsorption technology with novel adsorbents. Two different types of commercial CO2 adsorbents were used in the experiment. Results show that the IL/AC exhibited properties suitable for CO2 adsorption. The IL/AC sample presented a high CO2 uptake of 30 wt. % IL when treated at 30 °C for 6 h under a flow rate of 1 L/min. The presence of IL increased the selectivity of CO2 removal during the adsorption process. This IL/AC can be regenerated for several times without any significant loss in the performance.

MgO-based adsorbents for CO2 adsorption: Influence of structural and textural properties on the CO2 adsorption performance.

PubMed

Elvira, Gutiérrez-Bonilla; Francisco, Granados-Correa; Víctor, Sánchez-Mendieta; Alberto, Morales-Luckie Raúl

2017-07-01

A series of MgO-based adsorbents were prepared through solution-combustion synthesis and ball-milling process. The prepared MgO-based powders were characterized using X-ray diffraction, scanning electron microscopy, N 2 physisorption measurements, and employed as potential adsorbents for CO 2 adsorption. The influence of structural and textural properties of these adsorbents over the CO 2 adsorption behaviour was also investigated. The results showed that MgO-based products prepared by solution-combustion and ball-milling processes, were highly porous, fluffy, nanocrystalline structures in nature, which are unique physico-chemical properties that significantly contribute to enhance their CO 2 adsorption. It was found that the MgO synthesized by solution combustion process, using a molar ratio of urea to magnesium nitrate (2:1), and treated by ball-milling during 2.5hr (MgO-BM2.5h), exhibited the maximum CO 2 adsorption capacity of 1.611mmol/g at 25°C and 1atm, mainly via chemisorption. The CO 2 adsorption behaviour on the MgO-based adsorbents was correlated to their improved specific surface area, total pore volume, pore size distribution and crystallinity. The reusability of synthesized MgO-BM2.5h was confirmed by five consecutive CO 2 adsorption-desorption times, without any significant loss of performance, that supports the potential of MgO-based adsorbent. The results confirmed that the special features of MgO prepared by solution-combustion and treated by ball-milling during 2.5hr are favorable to be used as effective MgO-based adsorbent in post-combustion CO 2 capture technologies. Copyright © 2016. Published by Elsevier B.V.

Molecular simulation study of the competitive adsorption of H2O and CO2 in zeolite 13X.

PubMed

Joos, Lennart; Swisher, Joseph A; Smit, Berend

2013-12-23

The presence of H2O in postcombustion gas streams is an important technical issue for deploying CO2-selective adsorbents. Because of its permanent dipole, H2O can interact strongly with materials where the selectivity for CO2 is a consequence of its quadrupole interacting with charges in the material. We performed molecular simulations to model the adsorption of pure H2O and CO2 as well as H2O/CO2 mixtures in 13X, a popular zeolite for CO2 capture processes that is commercially available. The simulations show that H2O reduces the capacity of these materials for adsorbing CO2 by an order of magnitude and that at the partial pressures of H2O relevant for postcombustion capture, 13X will be essentially saturated with H2O .

Carbon Capture and Storage (CCS): Risk assessment focused on marine bacteria.

PubMed

Borrero-Santiago, A R; DelValls, T A; Riba, I

2016-09-01

Carbon capture and storage (CCS) is one of the options to mitigate the negative effects of the climate change. However, this strategy may have associated some risks such as CO2 leakages due to an escape from the reservoir. In this context, marine bacteria have been underestimated. In order to figure out the gaps and the lack of knowledge, this work summarizes different studies related to the potential effects on the marine bacteria associated with an acidification caused by a CO2 leak from CSS. An improved integrated model for risk assessment is suggested as a tool based on the rapid responses of bacterial community. Moreover, this contribution proposes a strategy for laboratory protocols using Pseudomona stanieri (CECT7202) as a case of study and analyzes the response of the strain under different CO2 conditions. Results showed significant differences (p≤0.05) under six diluted enriched medium and differences about the days in the exponential growth phase. Dilution 1:10 (Marine Broth 2216 with seawater) was selected as an appropriate growth medium for CO2 toxicity test in batch cultures. This work provide an essential and a complete tool to understand and develop a management strategy to improve future works related to possible effects produced by potential CO2 leaks. Copyright © 2016 Elsevier Inc. All rights reserved.

Hybrid Encapsulated Ionic Liquids for Post-Combustion Carbon Dioxide (CO 2) Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brennecke, Joan; Degnan, Thomas; McCready, Mark

Ionic liquids (ILs) and Phase Change Ionic Liquids (PCILs) are excellent materials for selective removal of carbon dioxide from dilute post-combustion streams. However, they are typically characterized as having high viscosities, which impairs their effectiveness due to mass transfer limitations, caused by the high viscosities. In this project, we are examining the benefits of encapsulating ILs and PCILs in thin polymeric shells to produce particles of approximately 100 to 600 μm in diameter that can be used in a fluidized bed absorber. The particles are produced by microencapsulation of the ILs and PCILs in CO 2-permeable polymer shells. Here wemore » report on the synthesis of the IL and PCIL materials, measurements of thermophysical properties including CO 2 capacity and reprotonation equilibrium and kinetics, encapsulation of the ILs and PCILs, mechanical and thermodynamic testing of the encapsulated materials, development of a rate based model of the absorber, and the design of a laboratory scale unit to test the encapsulated particles for CO 2 capture ability and efficiency. We show that the IL/PCIL materials can be successfully encapsulated, that they retain CO 2 uptake capacity, and that the uptake rates are increased relative to a stagnant sample of IL liquid or PCIL powder.« less

Energy-efficient stirred-tank photobioreactors for simultaneous carbon capture and municipal wastewater treatment.

PubMed

Mohammed, K; Ahammad, S Z; Sallis, P J; Mota, C R

2014-01-01

Algal based wastewater treatment (WWT) technologies are attracting renewed attention because they couple energy-efficient sustainable treatment with carbon capture, and reduce the carbon footprint of the process. A low-cost energy-efficient mixed microalgal culture-based pilot WWT system, coupled with carbon dioxide (CO2) sequestration, was investigated. The 21 L stirred-tank photobioreactors (STPBR) used light-emitting diodes as the light source, resulting in substantially reduced operational costs. The STPBR were operated at average optimal light intensity of 582.7 μmol.s(-1).m(-2), treating synthetic municipal wastewater containing approximately 250, 90 and 10 mg.L(-1) of soluble chemical oxygen demand (SCOD), ammonium (NH4-N), and phosphate, respectively. The STPBR were maintained for 64 days without oxygen supplementation, but had a supply of CO2 (25 mL.min(-1), 25% v/v in N2). Relatively high SCOD removal efficiency (>70%) was achieved in all STPBR. Low operational cost was achieved by eliminating the need for mechanical aeration, with microalgal photosynthesis providing all oxygenation. The STPBR achieved an energy saving of up to 95%, compared to the conventional AS system. This study demonstrates that microalgal photobioreactors can provide effective WWT and carbon capture, simultaneously, in a system with potential for scaling-up to municipal WWT plants.

Barriers and Prospects of Carbon Sequestration in India.

PubMed

Gupta, Anjali; Nema, Arvind K

2014-04-01

Carbon sequestration is considered a leading technology for reducing carbon dioxide (CO2) emissions from fossil-fuel based electricity generating power plants and could permit the continued use of coal and gas whilst meeting greenhouse gas targets. India will become the world's third largest emitter of CO2 by 2015. Considering the dependence of health of the Indian global economy, there is an imperative need to develop a global approach which could address the capturing and securely storing carbon dioxide emitted from an array of energy. Therefore technology such as carbon sequestration will deliver significant CO2 reductions in a timely fashion. Considerable energy is required for the capture, compression, transport and storage steps. With the availability of potential technical storage methods for carbon sequestration like forest, mineral and geological storage options with India, it would facilitate achieving stabilization goal in the near future. This paper examines the potential carbon sequestration options available in India and evaluates them with respect to their strengths, weakness, threats and future prospects.

Intro to Carbon Sequestration

ScienceCinema

None

2017-12-09

NETL's Carbon Sequestration Program is helping to develop technologies to capture, purify, and store carbon dioxide (CO2) in order to reduce greenhouse gas emissions without adversely influencing energy use or hindering economic growth. Carbon sequestration technologies capture and store CO2 that would otherwise reside in the atmosphere for long periods of time.

Flue-gas and direct-air capture of CO2 by porous metal–organic materials

PubMed Central

2017-01-01

Sequestration of CO2, either from gas mixtures or directly from air (direct air capture), is a technological goal important to large-scale industrial processes such as gas purification and the mitigation of carbon emissions. Previously, we investigated five porous materials, three porous metal–organic materials (MOMs), a benchmark inorganic material, Zeolite 13X and a chemisorbent, TEPA-SBA-15, for their ability to adsorb CO2 directly from air and from simulated flue-gas. In this contribution, a further 10 physisorbent materials that exhibit strong interactions with CO2 have been evaluated by temperature-programmed desorption for their potential utility in carbon capture applications: four hybrid ultramicroporous materials, SIFSIX-3-Cu, DICRO-3-Ni-i, SIFSIX-2-Cu-i and MOOFOUR-1-Ni; five microporous MOMs, DMOF-1, ZIF-8, MIL-101, UiO-66 and UiO-66-NH2; an ultramicroporous MOM, Ni-4-PyC. The performance of these MOMs was found to be negatively impacted by moisture. Overall, we demonstrate that the incorporation of strong electrostatics from inorganic moieties combined with ultramicropores offers improved CO2 capture performance from even moist gas mixtures but not enough to compete with chemisorbents. This article is part of the themed issue ‘Coordination polymers and metal–organic frameworks: materials by design’. PMID:27895255

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.

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

PubMed

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

2017-03-22

Direct use of atmospheric CO 2 as a C 1 source to synthesize high-value chemicals through environmentally benign processes is of great interest, yet challenging. Porous heterogeneous catalysts that are capable of simultaneously capturing and converting CO 2 are promising candidates for such applications. Herein, a family of organic ionic polymers with nanoporous structure, large surface area, strong affinity for CO 2 , and very high density of catalytic active sites (halide ions) was synthesized through the free-radical polymerization of vinylfunctionalized quaternary phosphonium salts. The resultant porous ionic polymers (PIPs) exhibit excellent activities in the cycloaddition of epoxides with atmospheric CO 2 , outperforming the corresponding soluble phosphonium salt analogues and ranking among the highest of known metal-free catalytic systems. The high CO 2 uptake capacity of the PIPs facilitates the enrichment of CO 2 molecules around the catalytic centers, thereby benefiting its conversion. We have demonstrated for the first time that atmospheric CO 2 can be directly converted to cyclic carbonates at room temperature using a heterogeneous catalytic system under metal-solvent free conditions. Moreover, the catalysts proved to be robust and fully recyclable, demonstrating promising potential for practical utilization for the chemical fixation of CO 2 . Our work thereby paves a way to the advance of PIPs as a new type of platform for capture and conversion of CO 2 . © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Complexes in the Photocatalytic Reaction of CO2 and H2O: Theoretical Studies

PubMed Central

Luo, Dongmei; Zhang, Ning; Hong, Sanguo; Wu, Huanwen; Liu, Zhihua

2010-01-01

Complexes (H2O/CO2, e–(H2O/CO2) and h+–(H2O/CO2)) in the reaction system of CO2 photoreduction with H2O were researched by B3LYP and MP2 methods along with natural bond orbital (NBO) analysis. Geometries of these complexes were optimized and frequencies analysis performed. H2O/CO2 captured photo-induced electron and hole produced e–(H2O/CO2) and h+–(H2O/CO2), respectively. The results revealed that CO2 and H2O molecules could be activated by the photo-induced electrons and holes, and each of these complexes possessed two isomers. Due to the effect of photo-induced electrons, the bond length of C=O and H-O were lengthened, while H-O bonds were shortened, influenced by holes. The infrared (IR) adsorption frequencies of these complexes were different from that of CO2 and H2O, which might be attributed to the synergistic effect and which could not be captured experimentally. PMID:21152274

Technological advances in CO2 conversion electro-biorefinery: A step toward commercialization.

PubMed

ElMekawy, Ahmed; Hegab, Hanaa M; Mohanakrishna, Gunda; Elbaz, Ashraf F; Bulut, Metin; Pant, Deepak

2016-09-01

The global atmospheric warming due to increased emissions of carbon dioxide (CO2) has attracted great attention in the last two decades. Although different CO2 capture and storage platforms have been proposed, the utilization of captured CO2 from industrial plants is progressively prevalent strategy due to concerns about the safety of terrestrial and aquatic CO2 storage. Two utilization forms were proposed, direct utilization of CO2 and conversion of CO2 to chemicals and energy products. The latter strategy includes the bioelectrochemical techniques in which electricity can be used as an energy source for the microbial catalytic production of fuels and other organic products from CO2. This approach is a potential technique in which CO2 emissions are not only reduced, but it also produce more value-added products. This review article highlights the different methodologies for the bioelectrochemical utilization of CO2, with distinctive focus on the potential opportunities for the commercialization of these techniques. Copyright © 2016 Elsevier Ltd. All rights reserved.

Interpretaion of synthetic seismic time-lapse monitoring data for Korea CCS project based on the acoustic-elastic coupled inversion

NASA Astrophysics Data System (ADS)

Oh, J.; Min, D.; Kim, W.; Huh, C.; Kang, S.

2012-12-01

Recently, the CCS (Carbon Capture and Storage) is one of the promising methods to reduce the CO2 emission. To evaluate the success of the CCS project, various geophysical monitoring techniques have been applied. Among them, the time-lapse seismic monitoring is one of the effective methods to investigate the migration of CO2 plume. To monitor the injected CO2 plume accurately, it is needed to interpret seismic monitoring data using not only the imaging technique but also the full waveform inversion, because subsurface material properties can be estimated through the inversion. However, previous works for interpreting seismic monitoring data are mainly based on the imaging technique. In this study, we perform the frequency-domain full waveform inversion for synthetic data obtained by the acoustic-elastic coupled modeling for the geological model made after Ulleung Basin, which is one of the CO2 storage prospects in Korea. We suppose the injection layer is located in fault-related anticlines in the Dolgorae Deformed Belt and, for more realistic situation, we contaminate the synthetic monitoring data with random noise and outliers. We perform the time-lapse full waveform inversion in two scenarios. One scenario is that the injected CO2 plume migrates within the injection layer and is stably captured. The other scenario is that the injected CO2 plume leaks through the weak part of the cap rock. Using the inverted P- and S-wave velocities and Poisson's ratio, we were able to detect the migration of the injected CO2 plume. Acknowledgment This work was financially supported by the Brain Korea 21 project of Energy Systems Engineering, the "Development of Technology for CO2 Marine Geological Storage" program funded by the Ministry of Land, Transport and Maritime Affairs (MLTM) of Korea and the Korea CCS R&D Center (KCRC) grant funded by the Korea government (Ministry of Education, Science and Technology) (No. 2012-0008926).

Thermodynamic screening of metal-substituted MOFs for carbon capture.

PubMed

Koh, Hyun Seung; Rana, Malay Kumar; Hwang, Jinhyung; Siegel, Donald J

2013-04-07

Metal-organic frameworks (MOFs) have emerged as promising materials for carbon capture applications due to their high CO2 capacities and tunable properties. Amongst the many possible MOFs, metal-substituted compounds based on M-DOBDC and M-HKUST-1 have demonstrated amongst the highest CO2 capacities at the low pressures typical of flue gasses. Here we explore the possibility for additional performance tuning of these compounds by computationally screening 36 metal-substituted variants (M = Be, Mg, Ca, Sr, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, W, Sn, and Pb) with respect to their CO2 adsorption enthalpy, ΔH(T=300K). Supercell calculations based on van der Waals density functional theory (vdW-DF) yield enthalpies in good agreement with experimental measurements, out-performing semi-empirical (DFT-D2) and conventional (LDA & GGA) functionals. Our screening identifies 13 compounds having ΔH values within the targeted thermodynamic window -40 ≤ ΔH ≤ -75 kJ mol(-1): 8 are based on M-DODBC (M = Mg, Ca, Sr, Sc, Ti, V, Mo, and W), and 5 on M-HKUST-1 (M = Be, Mg, Ca, Sr and Sc). Variations in the electronic structure and the geometry of the structural building unit are examined and used to rationalize trends in CO2 affinity. In particular, the partial charge on the coordinatively unsaturated metal sites is found to correlate with ΔH, suggesting that this property may be used as a simple performance descriptor. The ability to rapidly distinguish promising MOFs from those that are "thermodynamic dead-ends" will be helpful in guiding synthesis efforts towards promising compounds.

Selective gas capture via kinetic trapping

DOE PAGES

Kundu, Joyjit; Pascal, Tod; Prendergast, David; ...

2016-07-13

Conventional approaches to the capture of CO 2 by metal-organic frameworks focus on equilibrium conditions, and frameworks that contain little CO 2 in equilibrium are often rejected as carbon-capture materials. Here we use a statistical mechanical model, parameterized by quantum mechanical data, to suggest that metal-organic frameworks can be used to separate CO 2 from a typical flue gas mixture when used under nonequilibrium conditions. The origin of this selectivity is an emergent gas-separation mechanism that results from the acquisition by different gas types of different mobilities within a crowded framework. The resulting distribution of gas types within the frameworkmore » is in general spatially and dynamically heterogeneous. Our results suggest that relaxing the requirement of equilibrium can substantially increase the parameter space of conditions and materials for which selective gas capture can be effected.« less

Pilot project at Hazira, India, for capture of carbon dioxide and its biofixation using microalgae.

PubMed

Yadav, Anant; Choudhary, Piyush; Atri, Neelam; Teir, Sebastian; Mutnuri, Srikanth

2016-11-01

The objective of the present study was to set up a small-scale pilot reactor at ONGC Hazira, Surat, for capturing CO 2 from vent gas. The studies were carried out for CO 2 capture by either using microalgae Chlorella sp. or a consortium of microalgae (Scenedesmus quadricauda, Chlorella vulgaris and Chlorococcum humicola). The biomass harvested was used for anaerobic digestion to produce biogas. The carbonation column was able to decrease the average 34 vol.% of CO 2 in vent gas to 15 vol.% of CO 2 in the outlet gas of the carbonation column. The yield of Chlorella sp. was found to be 18 g/m 2 /day. The methane yield was 386 l CH 4 /kg VS fed of Chlorella sp. whereas 228 l CH 4 /kg VS fed of the consortium of algae.

Thermodynamic and kinetic studies on CO2 capture with Poly[VBTMA][Arg

NASA Astrophysics Data System (ADS)

Raja Shahrom, Maisara Shahrom; Wilfred, Cecilia Devi; Chong, Fai Kait

2018-05-01

This paper discusses the technologies for capturing CO2 from the natural gas using poly[VBTMA][Arg], a type of poly(ionic liquids) with an amino acid as the anion. The results revealed that the CO2 uptake increased from 3.23 mmol/g to 7.91 mmol/g at 1-10 bar, 298 K due to both chemical absorption and physical adsorption increments. Four adsorption isotherm models were applied to study the interaction between adsorbate and adsorbent to study the physical adsorption i.e. Freundlich, Langmuir, Dubinin Raduschkevich and Temkin isotherms at 298 K, 313 K and 333 K. Promising results were obtained that suggested the Freundlich model and the pseudo-first order model are well fitted with the kinetic data at 298 K with a 0.9943 R2 value. This study has provided empirical evidence to the current body of knowledge pertaining to CO2 capture technologies.

A Diaminopropane-Appended Metal–Organic Framework Enabling Efficient CO 2 Capture from Coal Flue Gas via a Mixed Adsorption Mechanism

DOE Office of Scientific and Technical Information (OSTI.GOV)

Milner, Phillip J.; Siegelman, Rebecca L.; Forse, Alexander C.

A new diamine-functionalized metal–organic framework comprised of 2,2-dimethyl-1,3-diaminopropane (dmpn) appended to the Mg 2+ sites lining the channels of Mg 2(dobpdc) (dobpdc4– = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) is characterized for the removal of CO 2 from the flue gas emissions of coal-fired power plants. Unique to members of this promising class of adsorbents, dmpn–Mg2(dobpdc) displays facile step-shaped adsorption of CO 2 from coal flue gas at 40 °C and near complete CO 2 desorption upon heating to 100 °C, enabling a high CO 2 working capacity (2.42 mmol/g, 9.1 wt %) with a modest 60 °C temperature swing. Evaluation of the thermodynamic parametersmore » of adsorption for dmpn–Mg 2(dobpdc) suggests that the narrow temperature swing of its CO 2 adsorption steps is due to the high magnitude of its differential enthalpy of adsorption (Δhads = -73 ± 1 kJ/mol), with a larger than expected entropic penalty for CO 2 adsorption (Δsads = -204 ± 4 J/mol·K) positioning the step in the optimal range for carbon capture from coal flue gas. In addition, thermogravimetric analysis and breakthrough experiments indicate that, in contrast to many adsorbents, dmpn–Mg 2(dobpdc) captures CO 2 effectively in the presence of water and can be subjected to 1000 humid adsorption/desorption cycles with minimal degradation. Solid-state 13C NMR spectra and single-crystal X-ray diffraction structures of the Zn analogue reveal that this material adsorbs CO 2 via formation of both ammonium carbamates and carbamic acid pairs, the latter of which are crystallographically verified for the first time in a porous material. Taken together, these properties render dmpn–Mg 2(dobpdc) one of the most promising adsorbents for carbon capture applications.« less

A Diaminopropane-Appended Metal-Organic Framework Enabling Efficient CO2 Capture from Coal Flue Gas via a Mixed Adsorption Mechanism.

PubMed

Milner, Phillip J; Siegelman, Rebecca L; Forse, Alexander C; Gonzalez, Miguel I; Runčevski, Tomče; Martell, Jeffrey D; Reimer, Jeffrey A; Long, Jeffrey R

2017-09-27

A new diamine-functionalized metal-organic framework comprised of 2,2-dimethyl-1,3-diaminopropane (dmpn) appended to the Mg 2+ sites lining the channels of Mg 2 (dobpdc) (dobpdc 4- = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) is characterized for the removal of CO 2 from the flue gas emissions of coal-fired power plants. Unique to members of this promising class of adsorbents, dmpn-Mg 2 (dobpdc) displays facile step-shaped adsorption of CO 2 from coal flue gas at 40 °C and near complete CO 2 desorption upon heating to 100 °C, enabling a high CO 2 working capacity (2.42 mmol/g, 9.1 wt %) with a modest 60 °C temperature swing. Evaluation of the thermodynamic parameters of adsorption for dmpn-Mg 2 (dobpdc) suggests that the narrow temperature swing of its CO 2 adsorption steps is due to the high magnitude of its differential enthalpy of adsorption (Δh ads = -73 ± 1 kJ/mol), with a larger than expected entropic penalty for CO 2 adsorption (Δs ads = -204 ± 4 J/mol·K) positioning the step in the optimal range for carbon capture from coal flue gas. In addition, thermogravimetric analysis and breakthrough experiments indicate that, in contrast to many adsorbents, dmpn-Mg 2 (dobpdc) captures CO 2 effectively in the presence of water and can be subjected to 1000 humid adsorption/desorption cycles with minimal degradation. Solid-state 13 C NMR spectra and single-crystal X-ray diffraction structures of the Zn analogue reveal that this material adsorbs CO 2 via formation of both ammonium carbamates and carbamic acid pairs, the latter of which are crystallographically verified for the first time in a porous material. Taken together, these properties render dmpn-Mg 2 (dobpdc) one of the most promising adsorbents for carbon capture applications.

Convenient and large-scale synthesis of nitrogen-rich hierarchical porous carbon spheres for supercapacitors and CO2 capture

NASA Astrophysics Data System (ADS)

Chang, Binbin; Zhang, Shouren; Yin, Hang; Yang, Baocheng

2017-08-01

Herein, considering the great potential of nitrogen-doped hierarchical porous carbons in energy storage and CO2 capture, we designed a convenient and easily large-scale production strategy for preparing nitrogen-doped hierarchical porous carbon sphere (NHPCS) materials. In this synthesis route, spherical resorcinol-formaldehyde (RF) resins were selected as carbon precursor, and then the ZnCl2-impregnated RF resin spheres were carbonized in a NH3 atmosphere at a temperature range of 600-800 °C. During the one-step heat-treatment process, nitrogen atom could be efficiently incorporated into the carbon skeleton, and the interconnected and hierarchical pore structure with different micro/mesopore proportion could be generated and tuned by adjusting the activating agent ZnCl2 dosage and carbonization temperature. The resultant nitrogen-doped hierarchical porous carbon sphere materials exhibited a satisfactory charge storage capacity, and the optimal sample of NHPCS-2-8 with a high mesopore proportion obtained at 800 °C with a ZnCl2/RF mass ratio of 2:1 presented a specific capacitance of 273.8 F g-1 at a current density of 0.5 A g-1. More importantly, the assembled NHPCS-2-8-based symmetric capacitor displayed a high energy density of 17.2 Wh kg-1 at a power density of 178.9 W kg-1 within a voltage window of 0 ∼ 1.8 V in 0.5 M Na2SO4 aqueous electrolyte. In addition, the CO2 capture application of these NHPCS materials was also explored, and the optimal sample of NHPCS-0-8 with a large micropore proportion prepared at 800 °C exhibited an exceptional CO2 uptake capacity at ambient pressures of up to 4.23 mmol g-1 at 0 °C.

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. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Direct electrolytic dissolution of silicate minerals for air CO2 mitigation and carbon-negative H2 production

PubMed Central

Rau, Greg H.; Carroll, Susan A.; Bourcier, William L.; Singleton, Michael J.; Smith, Megan M.; Aines, Roger D.

2013-01-01

We experimentally demonstrate the direct coupling of silicate mineral dissolution with saline water electrolysis and H2 production to effect significant air CO2 absorption, chemical conversion, and storage in solution. In particular, we observed as much as a 105-fold increase in OH− concentration (pH increase of up to 5.3 units) relative to experimental controls following the electrolysis of 0.25 M Na2SO4 solutions when the anode was encased in powdered silicate mineral, either wollastonite or an ultramafic mineral. After electrolysis, full equilibration of the alkalized solution with air led to a significant pH reduction and as much as a 45-fold increase in dissolved inorganic carbon concentration. This demonstrated significant spontaneous air CO2 capture, chemical conversion, and storage as a bicarbonate, predominantly as NaHCO3. The excess OH− initially formed in these experiments apparently resulted via neutralization of the anolyte acid, H2SO4, by reaction with the base mineral silicate at the anode, producing mineral sulfate and silica. This allowed the NaOH, normally generated at the cathode, to go unneutralized and to accumulate in the bulk electrolyte, ultimately reacting with atmospheric CO2 to form dissolved bicarbonate. Using nongrid or nonpeak renewable electricity, optimized systems at large scale might allow relatively high-capacity, energy-efficient (<300 kJ/mol of CO2 captured), and inexpensive (<$100 per tonne of CO2 mitigated) removal of excess air CO2 with production of carbon-negative H2. Furthermore, when added to the ocean, the produced hydroxide and/or (bi)carbonate could be useful in reducing sea-to-air CO2 emissions and in neutralizing or offsetting the effects of ongoing ocean acidification. PMID:23729814

40 CFR 98.422 - GHGs to report.

Code of Federal Regulations, 2010 CFR

2010-07-01

... GREENHOUSE GAS REPORTING Suppliers of Carbon Dioxide § 98.422 GHGs to report. (a) Mass of CO2 captured from each production process unit. (b) Mass of CO2 extracted from each CO2 production wells. (c) Mass of CO2 imported. (d) Mass of CO2 exported. ...

Combined Pressure, Temperature Contrast and Surface-Enhanced Separation of Carbon Dioxide for Post-Combustion Carbon Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Zhen; Wong, Michael; Gupta, Mayank

The Rice University research team developed a hybrid carbon dioxide (CO 2) absorption process combining absorber and stripper columns using a high surface area ceramic foam gas-liquid contactor for enhanced mass transfer and utilizing waste heat for regeneration. This integrated absorber/desorber arrangement will reduce space requirements, an important factor for retrofitting existing coal-fired power plants with CO 2 capture technology. Described in this report, we performed an initial analysis to estimate the technical and economic feasibility of the process. A one-dimensional (1D) CO 2 absorption column was fabricated to measure the hydrodynamic and mass transfer characteristics of the ceramic foam.more » A bench-scale prototype was constructed to implement the complete CO 2 separation process and tested to study various aspects of fluid flow in the process. A model was developed to simulate the two-dimensional (2D) fluid flow and optimize the CO 2 capture process. Test results were used to develop a final technoeconomic analysis and identify the most appropriate absorbent as well as optimum operating conditions to minimize capital and operating costs. Finally, a technoeconomic study was performed to assess the feasibility of integrating the process into a 600 megawatt electric (MWe) coal-fired power plant. With process optimization, $82/MWh of COE can be achieved using our integrated absorber/desorber CO 2 capture technology, which is very close to DOE's target that no more than a 35% increase in COE with CCS. An environmental, health, and safety (EH&S) assessment of the capture process indicated no significant concern in terms of EH&S effects or legislative compliance.« less

Robust Immobilized Amine CO 2 Sorbent Pellets Utilizing a Poly(Chloroprene) Polymer Binder and Fly Ash Additive

DOE PAGES

Wilfong, Walter Christopher; Kail, Brian W.; Howard, Bret H.; ...

2016-08-04

Pelletization of ca. 50 wt % amine/silica carbon dioxide sorbents was achieved with the novel combination of fly ash (FA) as a strength additive and hydrophobic poly(chloroprene) (PC) as a binder. The PC content and overall synthesis procedure of these materials were optimized to produce pellets, labeled as FA/E100-S_(20/80)_12.2, with the highest ball-mill attrition resistance (<0.5 wt % by fines, 24 h) and maximum CO 2 capture capacity of 1.78 mmol CO 2 g -1. The strength of the pellets was attributed to hydrogen-bonding of the relatively homogeneous PC network with the interlocked FA and BIAS particles (DRIFTS, SEM-EDS). Themore » low degradation of 3–4 % in the pellet's CO 2 capture capacity under both dry TGA (7.5 h) and practical fixed-bed (6.5 h dry; 4.5 h humid,≈5 vol % H 2O) CO 2 adsorption–desorption conditions highlights the pellet's excellent cyclic stability. These robust pellet characteristics make PC/FA/sorbent materials promising for commercial scale, point-source CO 2 capture.« less

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.

Preparation and characterization of novel carbon dioxide adsorbents based on polyethylenimine-modified Halloysite nanotubes.

PubMed

Cai, Haohao; Bao, Feng; Gao, Jie; Chen, Tao; Wang, Si; Ma, Rui

2015-01-01

New nano-sized carbon dioxide (CO2) adsorbents based on Halloysite nanotubes impregnated with polyethylenimine (PEI) were designed and synthesized, which were excellent adsorbents for the capture of CO2 at room temperature and had relatively high CO2 adsorption capacity. The prepared adsorbents were characterized by various techniques such as Fourier transform infrared spectrometry, gel permeation chromatography, dynamic light scattering, thermogravimetry, thermogravimetry-Fourier transform-infrared spectrometry, scanning electron microscopy and transmission electron microscopy. The adsorption characteristics and capacity were studied at room temperature, the highest CO2 adsorption capacity of 156.6 mg/g-PEI was obtained and the optimal adsorption capacity can reach a maximum value of 54.8 mg/g-adsorbent. The experiment indicated that this kind of adsorbent has a high stability at 80°C and PEI-impregnated adsorbents showed good reversibility and stability during cyclic adsorption-regeneration tests.

A simulation study on the abatement of CO2 emissions by de-absorption with monoethanolamine.

PubMed

Greer, T; Bedelbayev, A; Igreja, J M; Gomes, J F; Lie, B

2010-01-01

Because of the adverse effect of CO2 from fossil fuel combustion on the earth's ecosystems, the most cost-effective method for CO2 capture is an important area of research. The predominant process for CO2 capture currently employed by industry is chemical absorption in amine solutions. A dynamic model for the de-absorption process was developed with monoethanolamine (MEA) solution. Henry's law was used for modelling the vapour phase equilibrium of the CO2, and fugacity ratios calculated by the Peng-Robinson equation of state (EOS) were used for H2O, MEA, N2 and O2. Chemical reactions between CO2 and MEA were included in the model along with the enhancement factor for chemical absorption. Liquid and vapour energy balances were developed to calculate the liquid and vapour temperature, respectively.

Bifunctional application of sodium cobaltate as a catalyst and captor through CO oxidation and subsequent CO 2 chemisorption processes

DOE PAGES

Vera, Elizabeth; Alcántar-Vázquez, Brenda; Duan, Yuhua; ...

2015-12-21

The potential bifunctional mechanism of sodium cobaltate (NaCoO 2) in the catalysis of CO oxidation and subsequent CO 2 chemisorption was systematically analysed. Different catalytic and gravimetric experiments were performed dynamically and isothermally at multiple temperatures. Initially, the CO oxidation process was evaluated using a catalytic reactor connected to a gas chromatograph. Once the production of CO 2 was confirmed, its chemisorption capacity with NaCoO 2 was studied gravimetrically. Catalytic and gravimetric analysis products were studied by XRD, FTIR and SEM to elucidate the double reaction mechanism. Sodium cobaltate exhibited interesting catalytic properties over a wide temperature range, although themore » NaCoO 2 crystalline structure and chemical composition changed during the CO 2 capture process. Furthermore, all the experiments were theoretically supported by first-principles density functional theory thermodynamic calculations. Finally, the calculated thermodynamic properties of the CO oxidation and CO 2 capture reactions with NaCoO 2 under different oxidation conditions were in good agreement with the experimental measurements.« less

77 FR 58533 - Notice of Availability of the Draft Environmental Impact Statement for the W.A. Parish Post...

Federal Register 2010, 2011, 2012, 2013, 2014

2012-09-21

....A. Parish Post-Combustion CO 2 Capture and Sequestration Project, Southeastern TX AGENCY: U.S... availability of the Draft Environmental Impact Statement for the W.A. Parish Post-Combustion Carbon Dioxide.... Parish Post-Combustion CO 2 Capture and Sequestration Project (Parish PCCS Project). NRG's proposed...

Textural content in 3T MR: an image-based marker for Alzheimer's disease

NASA Astrophysics Data System (ADS)

Bharath Kumar, S. V.; Mullick, Rakesh; Patil, Uday

2005-04-01

In this paper, we propose a study, which investigates the first-order and second-order distributions of T2 images from a magnetic resonance (MR) scan for an age-matched data set of 24 Alzheimer's disease and 17 normal patients. The study is motivated by the desire to analyze the brain iron uptake in the hippocampus of Alzheimer's patients, which is captured by low T2 values. Since, excess iron deposition occurs locally in certain regions of the brain, we are motivated to investigate the spatial distribution of T2, which is captured by higher-order statistics. Based on the first-order and second-order distributions (involving gray level co-occurrence matrix) of T2, we show that the second-order statistics provide features with sensitivity >90% (at 80% specificity), which in turn capture the textural content in T2 data. Hence, we argue that different texture characteristics of T2 in the hippocampus for Alzheimer's and normal patients could be used as an early indicator of Alzheimer's disease.

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

PubMed

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

2018-05-23

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

The Chemical Route to a Carbon Dioxide Neutral World.

PubMed

Martens, Johan A; Bogaerts, Annemie; De Kimpe, Norbert; Jacobs, Pierre A; Marin, Guy B; Rabaey, Korneel; Saeys, Mark; Verhelst, Sebastian

2017-03-22

Excessive CO 2 emissions in the atmosphere from anthropogenic activity can be divided into point sources and diffuse sources. The capture of CO 2 from flue gases of large industrial installations and its conversion into fuels and chemicals with fast catalytic processes seems technically possible. Some emerging technologies are already being demonstrated on an industrial scale. Others are still being tested on a laboratory or pilot scale. These emerging chemical technologies can be implemented in a time window ranging from 5 to 20 years. The massive amounts of energy needed for capturing processes and the conversion of CO 2 should come from low-carbon energy sources, such as tidal, geothermal, and nuclear energy, but also, mainly, from the sun. Synthetic methane gas that can be formed from CO 2 and hydrogen gas is an attractive renewable energy carrier with an existing distribution system. Methanol offers advantages as a liquid fuel and is also a building block for the chemical industry. CO 2 emissions from diffuse sources is a difficult problem to solve, particularly for CO 2 emissions from road, water, and air transport, but steady progress in the development of technology for capturing CO 2 from air is being made. It is impossible to ban carbon from the entire energy supply of mankind with the current technological knowledge, but a transition to a mixed carbon-hydrogen economy can reduce net CO 2 emissions and ultimately lead to a CO 2 -neutral world. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Geologic Carbon Sequestration: Mitigating Climate Change by Injecting CO2 Underground (LBNL Summer Lecture Series)

ScienceCinema

Oldenburg, Curtis M. [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Earth Sciences Division

2018-05-07

Summer Lecture Series 2009: Climate change provides strong motivation to reduce CO2 emissions from the burning of fossil fuels. Carbon dioxide capture and storage involves the capture, compression, and transport of CO2 to geologically favorable areas, where its injected into porous rock more than one kilometer underground for permanent storage. Oldenburg, who heads Berkeley Labs Geologic Carbon Sequestration Program, will focus on the challenges, opportunities, and research needs of this innovative technology.

A catalytic role of surface silanol groups in CO2 capture on the amine-anchored silica support.

PubMed

Cho, Moses; Park, Joonho; Yavuz, Cafer T; Jung, Yousung

2018-05-03

A new mechanism of CO2 capture on the amine-functionalized silica support is demonstrated using density functional theory calculations, in which the silica surface not only acts as a support to anchor amines, but also can actively participate in the CO2 capture process through a facile proton transfer reaction with the amine groups. The surface-mediated proton transfer mechanism in forming a carbamate-ammonium product has lower kinetic barrier (8.1 kcal mol-1) than the generally accepted intermolecular mechanism (12.7 kcal mol-1) under dry conditions, and comparable to that of the water-assisted intermolecular mechanism (6.0 kcal mol-1) under humid conditions. These findings suggest that the CO2 adsorption on the amine-anchored silica surface would mostly occur via the rate-determining proton transfer step that is catalyzed by the surface silanol groups.

Tilted pillar array fabrication by the combination of proton beam writing and soft lithography for microfluidic cell capture Part 2: Image sequence analysis based evaluation and biological application.

PubMed

Járvás, Gábor; Varga, Tamás; Szigeti, Márton; Hajba, László; Fürjes, Péter; Rajta, István; Guttman, András

2018-02-01

As a continuation of our previously published work, this paper presents a detailed evaluation of a microfabricated cell capture device utilizing a doubly tilted micropillar array. The device was fabricated using a novel hybrid technology based on the combination of proton beam writing and conventional lithography techniques. Tilted pillars offer unique flow characteristics and support enhanced fluidic interaction for improved immunoaffinity based cell capture. The performance of the microdevice was evaluated by an image sequence analysis based in-house developed single-cell tracking system. Individual cell tracking allowed in-depth analysis of the cell-chip surface interaction mechanism from hydrodynamic point of view. Simulation results were validated by using the hybrid device and the optimized surface functionalization procedure. Finally, the cell capture capability of this new generation microdevice was demonstrated by efficiently arresting cells from a HT29 cell-line suspension. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Flying MOFs: polyamine-containing fluidized MOF/SiO 2 hybrid materials for CO 2 capture from post-combustion flue gas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Luz, Ignacio; Soukri, Mustapha; Lail, Marty

Solid-state synthesis ensures a high loading and well dispersed growth of a large collection of metal–organic framework (MOF) nanostructures within a series of commercially available mesoporous silica allowing to render MOFs into fluidized solid sorbents for CO 2 capture from post-combustion flue gas in a fluidized-bed reactor.

Flying MOFs: polyamine-containing fluidized MOF/SiO 2 hybrid materials for CO 2 capture from post-combustion flue gas

DOE PAGES

Luz, Ignacio; Soukri, Mustapha; Lail, Marty

2018-01-01

Solid-state synthesis ensures a high loading and well dispersed growth of a large collection of metal–organic framework (MOF) nanostructures within a series of commercially available mesoporous silica allowing to render MOFs into fluidized solid sorbents for CO 2 capture from post-combustion flue gas in a fluidized-bed reactor.

Evaluating the efficacy of amino acids as CO2 capturing agents: a first principles investigation.

PubMed

Hussain, M Althaf; Soujanya, Yarasi; Sastry, G Narahari

2011-10-01

Comprehension of the basic concepts for the design of systems for CO2 adsorption is imperative for increasing interest in technology for CO2 capture from the effluents. The efficacy of 20 naturally occurring amino acids (AAs) is demonstrated as the most potent CO2 capturing agents in the process of chemical absorption and physisorption through a systematic computational study using highly parametrized M05-2X/6-311+G(d,p) method. The ability of AAs to bind CO2 both in the noncovalent and covalent fashion and presence of multiple adsorption sites with varying magnitude of binding strengths in all 20 AAs makes them as most promising materials in the process of physisorption. The binding energies (BEs) estimating the strength of noncovalent interaction of AAs and CO2 are calculated and results are interpreted in terms of the nature and strength of the various types of cooperative interactions which are present. The study underlines the possibility to engineer the porous solid materials with extended networks by judiciously employing AA chains as linkers which can substantially augment their efficacy. Results show that a significant increase in the CO2···AA affinity is achieved in the case of AAs with polar neutral side chains. Furthermore, the study proposes AAs as effective alternatives to alkanolamines in chemical dissolution of CO2.

Early atmospheric detection of carbon dioxide from carbon capture and storage sites.

PubMed

Pak, Nasrin Mostafavi; Rempillo, Ofelia; Norman, Ann-Lise; Layzell, David B

2016-08-01

The early atmospheric detection of carbon dioxide (CO2) leaks from carbon capture and storage (CCS) sites is important both to inform remediation efforts and to build and maintain public support for CCS in mitigating greenhouse gas emissions. A gas analysis system was developed to assess the origin of plumes of air enriched in CO2, as to whether CO2 is from a CCS site or from the oxidation of carbon compounds. The system measured CO2 and O2 concentrations for different plume samples relative to background air and calculated the gas differential concentration ratio (GDCR = -ΔO2/ΔCO2). The experimental results were in good agreement with theoretical calculations that placed GDCR values for a CO2 leak at 0.21, compared with GDCR values of 1-1.8 for the combustion of carbon compounds. Although some combustion plume samples deviated in GDCR from theoretical, the very low GDCR values associated with plumes from CO2 leaks provided confidence that this technology holds promise in providing a tool for the early detection of CO2 leaks from CCS sites. This work contributes to the development of a cost-effective technology for the early detection of leaks from sites where CO2 has been injected into the subsurface to enhance oil recovery or to permanently store the gas as a strategy for mitigating climate change. Such technology will be important in building public confidence regarding the safety and security of carbon capture and storage sites.

Feasibility study of algae-based Carbon Dioxide capture

EPA Science Inventory

SUMMARY: 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 undertak...

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lu, D.Y.; Hughes, R.W.; Anthony, E.J.

Sintering during calcination/carbonation may introduce substantial economic penalties for a CO{sub 2} looping cycle using limestone/dolomite-derived sorbents. Cyclic carbonation and calcination reactions were investigated for CO{sub 2} capture under fluidized bed combustion (FBC) conditions. The cyclic carbonation characteristics of CaCO{sub 3}-derived sorbents were compared at various calcination temperatures (700-925{sup o} C) and different gas stream compositions: pure -2 and a realistic calciner environment where high concentrations of CO{sub 2}>80-90% are expected. The conditions during carbonation were 700 {sup o}C and 15% CO{sub 2} in N{sub 2} and 0.18% or 0.50% SO{sub 2} in selected tests. Up to 20 calcination/carbonation cyclesmore » were conducted using a thermogravimetric analyzer (TGA) apparatus. Three Canadian limestones were tested: Kelly Rock, Havelock, and Cadomin, using a prescreened particle size range of 400-650 {mu} m. Calcined Kelly Rock and Cadomin samples were hydrated by steam and examined. Sorbent reactivity was reduced whenever SO{sub 2} was introduced to either the calcining or carbonation streams. The multicyclic capture capacity of CaO for CO{sub 2} was substantially reduced at high concentrations of CO{sub 2} during the sorbent regeneration process and carbonation conversion of the Kelly Rock sample obtained after 20 cycles was only 10.5%. Hydrated sorbents performed better for CO{sub 2} capture but showed deterioration following calcination in high CO{sub 2} gas streams indicating that high CO{sub 2} and SO{sub 2} levels in the gas stream lead to lower CaO conversion because of enhanced sintering and irreversible formation of CaSO{sub 4}.« less

β-Na2TeO4: Phase Transition from an Orthorhombic to a Monoclinic Form. Reversible CO2 Capture.

PubMed

Galven, Cyrille; Pagnier, Thierry; Rosman, Noël; Le Berre, Françoise; Crosnier-Lopez, Marie-Pierre

2018-06-18

The present work concerns the tellurate Na 2 TeO 4 which has a 1D structure and could then present a CO 2 capture ability. It has been synthesized in a powder form via a solid-state reaction and structurally characterized by thermal X-ray diffraction experiments, Raman spectroscopy, and differential scanning calorimetry. The room temperature structure corresponds to the β-Na 2 TeO 4 orthorhombic form, and we show that it undergoes a reversible structural transition near 420 °C toward a monoclinic system. Ab initio computations were also performed on the room temperature structure, the Raman vibration modes calculated, and a normal mode attribution proposed. In agreement with our expectations, this sodium oxide is able to trap CO 2 by a two-step mechanism: Na + /H + exchange and carbonation of the released sodium as NaHCO 3 . This capture is reversible since CO 2 can be released upon heating by recombination of the mother phase.

Modeling Effects of Annealing on Coal Char Reactivity to O 2 and CO 2 , Based on Preparation Conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Holland, Troy; Bhat, Sham; Marcy, Peter

Oxy-fired coal combustion is a promising potential carbon capture technology. Predictive computational fluid dynamics (CFD) simulations are valuable tools in evaluating and deploying oxyfuel and other carbon capture technologies, either as retrofit technologies or for new construction. However, accurate predictive combustor simulations require physically realistic submodels with low computational requirements. A recent sensitivity analysis of a detailed char conversion model (Char Conversion Kinetics (CCK)) found thermal annealing to be an extremely sensitive submodel. In the present work, further analysis of the previous annealing model revealed significant disagreement with numerous datasets from experiments performed after that annealing model was developed. Themore » annealing model was accordingly extended to reflect experimentally observed reactivity loss, because of the thermal annealing of a variety of coals under diverse char preparation conditions. The model extension was informed by a Bayesian calibration analysis. In addition, since oxyfuel conditions include extraordinarily high levels of CO 2, the development of a first-ever CO 2 reactivity loss model due to annealing is presented.« less

Modeling Effects of Annealing on Coal Char Reactivity to O 2 and CO 2 , Based on Preparation Conditions

DOE PAGES

Holland, Troy; Bhat, Sham; Marcy, Peter; ...

2017-08-25

Oxy-fired coal combustion is a promising potential carbon capture technology. Predictive computational fluid dynamics (CFD) simulations are valuable tools in evaluating and deploying oxyfuel and other carbon capture technologies, either as retrofit technologies or for new construction. However, accurate predictive combustor simulations require physically realistic submodels with low computational requirements. A recent sensitivity analysis of a detailed char conversion model (Char Conversion Kinetics (CCK)) found thermal annealing to be an extremely sensitive submodel. In the present work, further analysis of the previous annealing model revealed significant disagreement with numerous datasets from experiments performed after that annealing model was developed. Themore » annealing model was accordingly extended to reflect experimentally observed reactivity loss, because of the thermal annealing of a variety of coals under diverse char preparation conditions. The model extension was informed by a Bayesian calibration analysis. In addition, since oxyfuel conditions include extraordinarily high levels of CO 2, the development of a first-ever CO 2 reactivity loss model due to annealing is presented.« less

Biomimetic CO2 capture using a highly thermostable bacterial α-carbonic anhydrase immobilized on a polyurethane foam.

PubMed

Migliardini, Fortunato; De Luca, Viviana; Carginale, Vincenzo; Rossi, Mosè; Corbo, Pasquale; Supuran, Claudiu T; Capasso, Clemente

2014-02-01

The biomimetic approach represents an interesting strategy for carbon dioxide (CO2) capture, offering advantages over other methods, due to its specificity for CO2 and its eco-compatibility, as it allows concentration of CO2 from other gases, and its conversion to water soluble ions. This approach uses microorganisms capable of fixing CO2 through metabolic pathways or via the use of an enzyme, such as carbonic anhydrase (CA, EC 4.2.1.1). Recently, our group cloned and purified a novel bacterial α-CA, named SspCA, from the thermophilic bacteria, Sulfurihydrogenibium yellowstonense YO3AOP1 living in hot springs at temperatures of up to 110 °C. This enzyme showed an exceptional thermal stability, retaining its high catalytic activity for the CO2 hydration reaction even after being heated at 70 °C for several hours. In the present paper, the SspCA was immobilized within a polyurethane (PU) foam. The immobilized enzyme was found to be catalytically active and showed a long-term stability. A bioreactor containing the "PU-immobilized enzyme" (PU-SspCA) as shredded foam was used for experimental tests aimed to verify the CO2 capture capability in conditions close to those of a power plant application. In this bioreactor, a gas phase, containing CO2, was put into contact with a liquid phase under conditions, where CO2 contained in the gas phase was absorbed and efficiently converted into bicarbonate by the extremo-α-CA.

Viability of Carbon Capture and Sequestration Retrofits for Existing Coal-Fired Power Plants under an Emission Trading Scheme.

PubMed

Talati, Shuchi; Zhai, Haibo; Morgan, M Granger

2016-12-06

Using data on the coal-fired electric generating units (EGUs) in Texas we assess the economic feasibility of retrofitting existing units with carbon capture and sequestration (CCS) in order to comply with the Clean Power Plan's rate-based emission standards under an emission trading scheme. CCS with 90% capture is shown to be more economically attractive for a range of existing units than purchasing emission rate credits (ERCs) from a trading market at an average credit price above $28 per MWh under the final state standard and $35 per MWh under the final national standard. The breakeven ERC trading prices would decrease significantly if the captured CO 2 were sold for use in enhanced oil recovery, making CCS retrofits viable at lower trading prices. The combination of ERC trading and CO 2 use can greatly reinforce economic incentives and market demands for CCS and hence accelerate large-scale deployment, even under scenarios with high retrofit costs. Comparing the levelized costs of electricity generation between CCS retrofits and new renewable plants under the ERC trading scheme, retrofitting coal-fired EGUs with CCS may be significantly cheaper than new solar plants under some market conditions.

How Do Deep Saline Aquifer Microbial Communities Respond to Supercritical CO2 Injection?

NASA Astrophysics Data System (ADS)

Mu, A.; Billman-Jacobe, H.; Boreham, C.; Schacht, U.; Moreau, J. W.

2011-12-01

Carbon Capture and Storage (CCS) is currently seen as a viable strategy for mitigating anthropogenic carbon dioxide pollution. The Cooperative Research Centre for Greenhouse Gas Technologies (CO2CRC) is currently conducting a field experiment in the Otway Basin (Australia) studying residual gas saturation in the water-saturated reservoir of the Paaratte Formation. As part of this study, a suite of pre-CO2 injection water samples were collected from approximately 1400 meters depth (60°C, 13.8 MPa) via an in situ sampling system. The in situ sampling system isolates aquifer water from sources of contamination while maintaining the formation pressure. Whole community DNA was extracted from these samples to investigate the prokaryotic biodiversity of the saline Paaratte aquifer (EC = 1509.6 uS/cm). Bioinformatic analysis of preliminary 16S ribosomal gene data revealed Thermincola, Acinetobacter, Sphingobium, and Dechloromonas amongst the closest related genera to environmental clone sequences obtained from a subset of pre-CO2 injection groundwater samples. Epifluorescent microscopy with 4',6-diamidino-2-phenylindole (DAPI) highlighted an abundance of filamentous cells ranging from 5 to 45 μM. Efforts are currently directed towards utilising a high throughput sequencing approach to capture an exhaustive profile of the microbial diversity of the Paaratte aquifer CO2 injection site, and to understand better the response of in situ microbial populations to the injection of large volumes (e.g. many kilotonnes) of supercritical CO2 (sc-CO2). Sequencing results will be used to direct cultivation efforts towards enrichment of a CO2-tolerant microorganism. Understanding the microbial response to sc-CO2 is an integral aspect of carbon dioxide storage, for which very little information exists in the literature. This study aims to elucidate molecular mechanisms, through genomic and cultivation-based methods, for CO2 tolerance with the prospect of engineering biofilms to enhance trapping of CO2 in saline aquifers.

About how to capture and exploit the CO2 surplus that nature, per se, is not capable of fixing.

PubMed

Godoy, Manuel S; Mongili, Beatrice; Fino, Debora; Prieto, M Auxiliadora

2017-09-01

Human activity has been altering many ecological cycles for decades, disturbing the natural mechanisms which are responsible for re-establishing the normal environmental balances. Probably, the most disrupted of these cycles is the cycle of carbon. In this context, many technologies have been developed for an efficient CO 2 removal from the atmosphere. Once captured, it could be stored in large geological formations and other reservoirs like oceans. This strategy could present some environmental and economic problems. Alternately, CO 2 can be transformed into carbonates or different added-value products, such as biofuels and bioplastics, recycling CO 2 from fossil fuel. Currently different methods are being studied in this field. We classified them into biological, inorganic and hybrid systems for CO 2 transformation. To be environmentally compatible, they should be powered by renewable energy sources. Although hybrid systems are still incipient technologies, they have made great advances in the recent years. In this scenario, biotechnology is the spearhead of ambitious strategies to capture CO 2 and reduce global warming. © 2017 The Authors. Microbial Biotechnology published by John Wiley & Sons Ltd and Society for Applied Microbiology.

Understanding of Electrochemical Mechanisms for CO2 Capture and Conversion into Hydrocarbon Fuels in Transition-Metal Carbides (MXenes).

PubMed

Li, Neng; Chen, Xingzhu; Ong, Wee-Jun; MacFarlane, Douglas R; Zhao, Xiujian; Cheetham, Anthony K; Sun, Chenghua

2017-11-28

Two-dimensional (2D) transition-metal (groups IV, V, VI) carbides (MXenes) with formulas M 3 C 2 have been investigated as CO 2 conversion catalysts with well-resolved density functional theory calculations. While MXenes from the group IV to VI series have demonstrated an active behavior for the capture of CO 2 , the Cr 3 C 2 and Mo 3 C 2 MXenes exhibit the most promising CO 2 to CH 4 selective conversion capabilities. Our results predicted the formation of OCHO • and HOCO • radical species in the early hydrogenation steps through spontaneous reactions. This provides atomic level insights into the computer-aided screening for high-performance catalysts and the understanding of electrochemical mechanisms for CO 2 reduction to energy-rich hydrocarbon fuels, which is of fundamental significance to elucidate the elementary steps for CO 2 fixation.

Techno-economic analysis of sorption-enhanced steam methane reforming in a fixed bed reactor network integrated with fuel cell

NASA Astrophysics Data System (ADS)

Diglio, Giuseppe; Hanak, Dawid P.; Bareschino, Piero; Mancusi, Erasmo; Pepe, Francesco; Montagnaro, Fabio; Manovic, Vasilije

2017-10-01

Sorption-enhanced steam methane reforming (SE-SMR) is a promising alternative for H2 production with inherent CO2 capture. This study evaluates the techno-economic performance of SE-SMR in a network of fixed beds and its integration with a solid oxide fuel cell (SE-SMR-SOFC) for power generation. The analysis revealed that both proposed systems are characterised by better economic performance than the reference systems. In particular, for SE-SMR the levelised cost of hydrogen is 1.6 €ṡkg-1 and the cost of CO2 avoided is 29.9 €ṡtCO2-1 (2.4 €ṡkg-1 and 50 €ṡtCO2-1, respectively, for SMR with CO2 capture) while for SE-SMR-SOFC the levelised cost of electricity is 0.078 €ṡkWh-1 and the cost of CO2 avoided is 36.9 €ṡtCO2-1 (0.080 €ṡkWh-1 and 80 €ṡtCO2-1, respectively, for natural gas-fired power plant with carbon capture). The sensitivity analysis showed that the specific cost of fuel and the capital cost of fuel cell mainly affect the economic performance of SE-SMR and SE-SMR-SOFC, respectively. The daily revenue of the SE-SMR-SOFC system is higher than that of the natural gas-fired power plant if the difference between the carbon tax and the CO2 transport and storage cost is > 6 €ṡtCO2-1.

Hydrogen sulfide capture by limestone and dolomite at elevated pressure. 1: Sorbent performance

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yrjas, K.P.; Zevenhoven, C.A.P.; Hupa, M.M.

1996-01-01

Sulfur emission control in fossil fuel gasification plants implies the removal of H{sub 2}S from the product gas either inside the furnace or in the gas clean-up system. In a fluidized-bed gasifier, in-bed sulfur capture can be accomplished by adding a calcium-based sorbent such as limestone or dolomite to the bend and removing the sulfur from the system with the bottom ash in the form of CaS. This work describes the H{sub 2}S uptake by a set of physically and chemically different limestones and dolomites under pressurized conditions, typically for those in a pressurized fluidized-bed gasifier (2 MPa, 950 C).more » The tests were done with a pressurized thermobalance at two p{sub CO{sub 2}} levels. Thus, the sulfidation of both calcined and uncalcined sorbents could be analyzed. The effect of p{sub H{sub 2}S} was also investigated for uncalcined limestones and half-calcined dolomites. The results are presented as conversion of CaCO{sub 3} or CaO to CaS vs time plots. The results are also compared with the sulfur capture performance of the same sorbents under pressurized combustion conditions.« less

Insights into the mechanism of the capture of CO2 by K2CO3 sorbent: a DFT study.

PubMed

Liu, Hongyan; Qin, Qiaoyun; Zhang, Riguang; Ling, Lixia; Wang, Baojun

2017-09-13

The adsorption and reactions of CO 2 and H 2 O on both monoclinic and hexagonal crystal K 2 CO 3 were investigated using the density functional theory (DFT) approach. The calculated adsorption energies showed that adsorption of H 2 O molecules was clearly substantially stronger on the K 2 CO 3 surface than the adsorption of CO 2 , except on the (001)-1 surface of hexagonal K 2 CO 3 , where CO 2 is competitively adsorbed with H 2 O. Carbonation reactions easily occur on pure K 2 CO 3 and involve two parallel paths: one is where adsorbed H 2 O reacts with molecular CO 2 in gas to form the bicarbonate, while the other is where H 2 O dissociates into OH and H before bicarbonate formation, and then OH reacts with gaseous CO 2 to form a bicarbonate. Our results indicate that adding a support or promoter or using a special technique to expose more (001)-1 surfaces in hexagonal K 2 CO 3 may improve the conversion of CO 2 to the bicarbonate, which provides a theoretical direction for the experimental preparation of the K 2 CO 3 sorbent to capture CO 2 .

Kinetic analysis of an anion exchange absorbent for CO2 capture from ambient air.

PubMed

Shi, Xiaoyang; Li, Qibin; Wang, Tao; Lackner, Klaus S

2017-01-01

This study reports a preparation method of a new moisture swing sorbent for CO2 capture from air. The new sorbent components include ion exchange resin (IER) and polyvinyl chloride (PVC) as a binder. The IER can absorb CO2 when surrounding is dry and release CO2 when surrounding is wet. The manuscript presents the studies of membrane structure, kinetic model of absorption process, performance of desorption process and the diffusivity of water molecules in the CO2 absorbent. It has been proved that the kinetic performance of CO2 absorption/desorption can be improved by using thin binder and hot water treatment. The fast kinetics of P-100-90C absorbent is due to the thin PVC binder, and high diffusion rate of H2O molecules in the sample. The impressive is this new CO2 absorbent has the fastest CO2 absorption rate among all absorbents which have been reported by other up-to-date literatures.

Kinetic analysis of an anion exchange absorbent for CO2 capture from ambient air

PubMed Central

Shi, Xiaoyang; Li, Qibin; Lackner, Klaus S.

2017-01-01

This study reports a preparation method of a new moisture swing sorbent for CO2 capture from air. The new sorbent components include ion exchange resin (IER) and polyvinyl chloride (PVC) as a binder. The IER can absorb CO2 when surrounding is dry and release CO2 when surrounding is wet. The manuscript presents the studies of membrane structure, kinetic model of absorption process, performance of desorption process and the diffusivity of water molecules in the CO2 absorbent. It has been proved that the kinetic performance of CO2 absorption/desorption can be improved by using thin binder and hot water treatment. The fast kinetics of P-100-90C absorbent is due to the thin PVC binder, and high diffusion rate of H2O molecules in the sample. The impressive is this new CO2 absorbent has the fastest CO2 absorption rate among all absorbents which have been reported by other up-to-date literatures. PMID:28640914

Stability of a Benzyl Amine Based CO2 Capture Adsorbent in View of Regeneration Strategies

PubMed Central

2017-01-01

In this work, the chemical and thermal stability of a primary amine-functionalized ion-exchange resin (Lewatit VP OC 1065) is studied in view of the potential options of regenerating this sorbent in a CO2 removal application. The adsorbent was treated continuously in the presence of air, different O2/CO2/N2 mixtures, concentrated CO2, and steam, and then the remaining CO2 adsorption capacity was measured. Elemental analysis, BET/BJH analysis, Fourier transform infrared spectroscopy, and thermogravimetric analysis were applied to characterize adsorbent properties. This material was found to be thermally and hydrothermally stable at high temperatures. However, significant oxidative degradation occurred already at moderate temperatures (above 70 °C). Temperatures above 120 °C lead to degradation in concentrated dry CO2. Adding moisture to the concentrated CO2 stream improves the CO2-induced stability. Adsorbent regeneration with nitrogen stripping is studied with various parameters, focusing on minimizing the moles of purge gas required per mole of CO2 desorbed. PMID:28405055

Relationship between mosquito (Diptera: Culicidae) landing rates on a human subject and numbers captured using CO2-baited light traps

USDA-ARS?s Scientific Manuscript database

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...

Designing and Demonstrating a Master Student Project to Explore Carbon Dioxide Capture Technology

ERIC Educational Resources Information Center

Asherman, Florine; Cabot, Gilles; Crua, Cyril; Estel, Lionel; Gagnepain, Charlotte; Lecerf, Thibault; Ledoux, Alain; Leveneur, Sebastien; Lucereau, Marie; Maucorps, Sarah; Ragot, Melanie; Syrykh, Julie; Vige, Manon

2016-01-01

The rise in carbon dioxide (CO[subscript 2]) concentration in the Earth's atmosphere, and the associated strengthening of the greenhouse effect, requires the development of low carbon technologies. New carbon capture processes are being developed to remove CO[subscript 2] that would otherwise be emitted from industrial processes and fossil fuel…

Membrane contactors for CO2 capture processes - critical review

NASA Astrophysics Data System (ADS)

Nogalska, Adrianna; Trojanowska, Anna; Garcia-Valls, Ricard

2017-07-01

The use of membrane contactor in industrial processes is wide, and lately it started to be used in CO2 capture process mainly for gas purification or to reduce the emission. Use of the membrane contactor provides high contact surface area so the size of the absorber unit significantly decreases, which is an important factor for commercialization. The research has been caried out regarding the use of novel materials for the membrane production and absorbent solution improvements. The present review reveals the progress in membrane contactor systems for CO2 capture processes concerning solution for ceramic membrane wetting, comparison study of different polymers used for fabrication and methods of enzyme immobilization for biocomposite membrane. Also information about variety of absorbent solutions is described.

Novel Solvent System for Post Combustion CO{sub 2} Capture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brown, Alfred; Brown, Nathan

2013-09-30

The purpose of this project was to evaluate the performance of ION’s lead solvent and determine if ION’s solvent candidate could potentially meet DOE’s target of achieving 90% CO{sub 2} Capture from a 550 MWe Pulverized Coal Plant without resulting in an increase in COE greater than 35%. In this project, ION’s lead solvent demonstrated a 65% reduction in regeneration energy and a simultaneous 35% reduction in liquid to gas ratio (L/G) in comparison to aqMEA at 90% CO{sub 2} capture using actual flue gas at 0.2 MWe. Results have clearly demonstrated that the ION technology is in line withmore » DOE performance expectations and has the potential to meet DOE’s performance targets in larger scale testing environments.« less

Physical Activation of Oil Palm Empty Fruit Bunch via CO2 Activation Gas for CO2 Adsorption

NASA Astrophysics Data System (ADS)

Joseph, C. G.; Quek, K. S.; Daud, W. M. A. W.; Moh, P. Y.

2017-06-01

In this study, different parameters for the preparation of activated carbon were investigated for their yield and CO2 capture capabilities. The activated carbon was prepared from Oil Palm Empty Fruit Bunch (OPEFB) via a 2-step physical activation process. The OPEFB was pyrolyzed under inert conditions at 500 °C and activated via CO2. A 2-factorial design was employed and the effects of activation temperature, activation dwell time and gas flow rate on yield and CO2 capture capabilities were compared and studied. The yield obtained ranged from between 20 - 26, whereby the temperature was determined to be the most significant factor in influencing CO2 uptake. The CO2 capture capacity was determined using Temperature Programmed Desorption (TPD) technique. The CO2 uptake of EFB activated carbon achieved was between 1.85 - 2.09 mmol/g. TPD analysis has shown that the surface of AC were of basic nature. AC was found to be able to withhold the CO2 up to 663°C before maximum desorption occurs. The surface area and pore size of OPEFB obtained from BET analysis is 2.17 m2 g-1 and 0.01 cm3 g-1. After activation, both surface area and pore size increased with a maximum observed surface area and pore size of 548.07 m2 g-1 and 0.26 cm3 g-1. Surface morphology, functional groups, pore size and surface area were analyzed using SEM, FT-IR, TPD and BET.

A portable molecular-sieve-based CO{sub 2} sampling system for radiocarbon measurements

DOE Office of Scientific and Technical Information (OSTI.GOV)

Palonen, V., E-mail: vesa.palonen@helsinki.fi

We have developed a field-capable sampling system for the collection of CO{sub 2} samples for radiocarbon-concentration measurements. Most target systems in environmental research are limited in volume and CO{sub 2} concentration, making conventional flask sampling hard or impossible for radiocarbon studies. The present system captures the CO{sub 2} selectively to cartridges containing 13X molecular sieve material. The sampling does not introduce significant under-pressures or significant losses of moisture to the target system, making it suitable for most environmental targets. The system also incorporates a significantly larger sieve container for the removal of CO{sub 2} from chambers prior to the CO{submore » 2} build-up phase and sampling. In addition, both the CO{sub 2} and H{sub 2}O content of the sample gas are measured continuously. This enables in situ estimation of the amount of collected CO{sub 2} and the determination of CO{sub 2} flux to a chamber. The portable sampling system is described in detail and tests for the reliability of the method are presented.« less

Negative emissions—Part 2: Costs, potentials and side effects

NASA Astrophysics Data System (ADS)

Fuss, Sabine; Lamb, William F.; Callaghan, Max W.; Hilaire, Jérôme; Creutzig, Felix; Amann, Thorben; Beringer, Tim; de Oliveira Garcia, Wagner; Hartmann, Jens; Khanna, Tarun; Luderer, Gunnar; Nemet, Gregory F.; Rogelj, Joeri; Smith, Pete; Vicente, José Luis Vicente; Wilcox, Jennifer; del Mar Zamora Dominguez, Maria; Minx, Jan C.

2018-06-01

The most recent IPCC assessment has shown an important role for negative emissions technologies (NETs) in limiting global warming to 2 °C cost-effectively. However, a bottom-up, systematic, reproducible, and transparent literature assessment of the different options to remove CO2 from the atmosphere is currently missing. In part 1 of this three-part review on NETs, we assemble a comprehensive set of the relevant literature so far published, focusing on seven technologies: bioenergy with carbon capture and storage (BECCS), afforestation and reforestation, direct air carbon capture and storage (DACCS), enhanced weathering, ocean fertilisation, biochar, and soil carbon sequestration. In this part, part 2 of the review, we present estimates of costs, potentials, and side-effects for these technologies, and qualify them with the authors’ assessment. Part 3 reviews the innovation and scaling challenges that must be addressed to realise NETs deployment as a viable climate mitigation strategy. Based on a systematic review of the literature, our best estimates for sustainable global NET potentials in 2050 are 0.5–3.6 GtCO2 yr‑1 for afforestation and reforestation, 0.5–5 GtCO2 yr‑1 for BECCS, 0.5–2 GtCO2 yr‑1 for biochar, 2–4 GtCO2 yr‑1 for enhanced weathering, 0.5–5 GtCO2 yr‑1 for DACCS, and up to 5 GtCO2 yr‑1 for soil carbon sequestration. Costs vary widely across the technologies, as do their permanency and cumulative potentials beyond 2050. It is unlikely that a single NET will be able to sustainably meet the rates of carbon uptake described in integrated assessment pathways consistent with 1.5 °C of global warming.

Molecular modeling studies of interfacial reactions in wet supercritical CO2.

NASA Astrophysics Data System (ADS)

Glezakou, V.; McGrail, B. P.; Windisch, C. F.; Schaef, H. T.; Martin, P.

2011-12-01

In the recent years, Carbon Capture and Sequestration (CCS) technologies have gained considerable momentum in a globally organized effort to mitigate greenhouse emissions and adverse climate change. Co-sequestration refers to the capture and geologic sequestration of carbon dioxide and minor contaminants (sulfur compounds, NOx, Hg, etc.) in subsurface formations. Cosequestration offers the potential to make carbon management more economically acceptable to industry relative to sequestration of pure CO2. This may be achieved through significant savings in plant (and retrofit) capital cost, operating cost, and energy savings as well by eliminating the need for one or more individual pollutant capture systems (such as SO2 scrubbers). The latter point is important because co-sequestration may result in a net positive impact to the environment through avoided loss of power generation capacity from parasitic loads and reduced fuel needs. This paper will discuss our research on modeling, imaging and characterization of cosequestration processes and reactivity at a fundamental level. Our work examines the interactions of CO2-rich fluids with metal and mineral surfaces, and how these are affected by the presence of other gas components (e.g. SO2, H2O or NOx) commonly present in the CO2 streams. We have found that reactivity is also affected by the composition of the surface or, less obviously, by the surface exposed, for example, (104) vs (100 )of carbonate minerals. We combine experimental techniques such as XRD and Raman spectroscopy, which can detect and follow reactive processes, with ab initio modeling methods based on density functional theory, to establish a reliable correspondence between theory and experiment with predictive capability. Analysis of our molecular dynamics simulations, reveals structural information and vibrational density of states that can directly compare with XRD measurements and vibrational spectroscopy. While reactivity in CO2-containing aqueous environments has been widely studied, the reverse, i.e. reactivity in water-bearing condensed media, is not true. Our simulations show that mechanistic details in these environments can be drastically different, and they are very important in elucidating molecular transformations relevant to CCS or carbon conversion.