Regenerable Sorbents for CO.sub. 2 Capture from Moderate and High Temperature Gas Streams PDF Download
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A process for making a granular sorbent to capture carbon dioxide from gas streams comprising homogeneously mixing an alkali metal oxide, alkali metal hydroxide, alkaline earth metal oxide, alkaline earth metal hydroxide, alkali titanate, alkali zirconate, alkali silicate and combinations thereof with a binder selected from the group consisting of sodium ortho silicate, calcium sulfate dihydrate (CaSO.sub. 4.2H.sub. 2O), alkali silicates, calcium aluminate, bentonite, inorganic clays and organic clays and combinations thereof and water; drying the mixture and placing the sorbent in a container permeable to a gas stream.
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A process for making a granular sorbent to capture carbon dioxide from gas streams comprising homogeneously mixing an alkali metal oxide, alkali metal hydroxide, alkaline earth metal oxide, alkaline earth metal hydroxide, alkali titanate, alkali zirconate, alkali silicate and combinations thereof with a binder selected from the group consisting of sodium ortho silicate, calcium sulfate dihydrate (CaSO.sub. 4.2H.sub. 2O), alkali silicates, calcium aluminate, bentonite, inorganic clays and organic clays and combinations thereof and water; drying the mixture and placing the sorbent in a container permeable to a gas stream.
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The overall objective of the proposed research is to develop a low cost, high capacity CO2 sorbent and demonstrate its technical and economic viability for pre-combustion CO2 capture. The specific objectives supporting our research plan were to optimize the chemical structure and physical properties of the sorbent, scale-up its production using high throughput manufacturing equipment and bulk raw materials and then evaluate its performance, first in bench-scale experiments and then in slipstream tests using actual coal-derived synthesis gas. One of the objectives of the laboratory-scale evaluations was to demonstrate the life and durability of the sorbent for over 10,000 cycles and to assess the impact of contaminants (such as sulfur) on its performance. In the field tests, our objective was to demonstrate the operation of the sorbent using actual coal-derived synthesis gas streams generated by air-blown and oxygen-blown commercial and pilot-scale coal gasifiers (the CO2 partial pressure in these gas streams is significantly different, which directly impacts the operating conditions hence the performance of the sorbent). To support the field demonstration work, TDA collaborated with Phillips 66 and Southern Company to carry out two separate field tests using actual coal-derived synthesis gas at the Wabash River IGCC Power Plant in Terre Haute, IN and the National Carbon Capture Center (NCCC) in Wilsonville, AL. In collaboration with the University of California, Irvine (UCI), a detailed engineering and economic analysis for the new CO2 capture system was also proposed to be carried out using Aspen PlusTM simulation software, and estimate its effect on the plant efficiency.
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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.
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New low-cost CO.sub. 2 sorbents are provided that can be used in large-scale gas-solid processes. A new method is provided for making these sorbents that involves treating substrates with an amine and/or an ether so that the amine and/or ether comprise at least 50 wt. percent of the sorbent. The sorbent acts by capturing compounds contained in gaseous fluids via chemisorption and/or physisorption between the unit layers of the substrate's lattice where the polar amine liquids and solids and/or polar ether liquids and solids are located. The method eliminates the need for high surface area supports and polymeric materials for the preparation of CO.sub. 2 capture systems, and provides sorbents with absorption capabilities that are independent of the sorbents' surface areas. The sorbents can be regenerated by heating at temperatures in excess of 35.degree. C.
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Pages : 114
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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 CO2 from the flue gas. The sorbent exhibits a much higher affinity for CO2 than N2, H2O or O2, enabling effective CO2 separation from the flue gas. We also carried out a detailed process design and analysis of 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 CO2 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 CO2 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 CO2 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 CO2 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 CO2 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 CO2 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.
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A sorbent for the capture of carbon dioxide from a gas stream is provided, the sorbent containing calcium oxide (CaO) and at least one refractory dopant having a Tammann temperature greater than about 530.degree. C., wherein the refractory dopant enhances resistance to sintering, thereby conserving performance of the sorbent at temperatures of at least about 530.degree. C. Also provided are doped CaO sorbents for the capture of carbon dioxide in the presence of SO.sub. 2.
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Pages : 30
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Sodium based sorbents including sodium carbonate may be used to capture carbon dioxide from flue gas. A relatively concentrated carbon dioxide stream may be recoverable for sequestration when the sorbent is regenerated. Electrobalance tests indicated that sodium carbonate monohydrate was formed in a mixture of helium and water vapor at temperatures below 65 C. Additional compounds may also form, but this could not be confirmed. In the presence of carbon dioxide and water vapor, both the initial reaction rate of sodium carbonate with carbon dioxide and water and the sorbent capacity decreased with increasing temperature, consistent with the results from the previous quarter. Increasing the carbon dioxide concentration at constant temperature and water vapor concentration produced a measurable increase in rate, as did increasing the water vapor concentration at constant carbon dioxide concentration and temperature. Runs conducted with a flatter TGA pan resulted in a higher initial reaction rate, presumably due to improved gas-solid contact, but after a short time, there was no significant difference in the rates measured with the different pans. Analyses of kinetic data suggest that the surface of the sodium carbonate particles may be much hotter than the bulk gas due to the highly exothermic reaction with carbon dioxide and water, and that the rate of heat removal from the particle may control the reaction rate. A material and energy balance was developed for a cyclic carbonation/calcination process which captures about 26 percent of the carbon dioxide present in flue gas available at 250 C.
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A novel liquid impregnated solid sorbent was developed for CO2 removal in the temperature range of ambient to 60 °C for both fixed bed and fluidized bed reactor applications. The sorbent is regenerable at 60-80 °C. Multi-cycle tests conducted in an atmospheric bench scale reactor with simulated flue gas demonstrated that the sorbent retains its CO2 sorption capacity with CO2 removal efficiency of about 99%. A second, novel solid sorbent containing mixture of alkali earth and alkali compounds was developed for CO2 removal at 200-315 °C from high pressure gas streams (i.e., suitable for IGCC systems). The sorbent showed very high capacity for CO2 removal from gas streams containing 28% CO2 at 200 °C and 11.2 atm during lab-scale flow reactor tests as well as regenerability at 375 °C.
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This document summarizes the work performed on Cooperative Agreement DE-FE0000465,?Evaluation of Dry Sorbent Technology for Pre-Combustion CO2 Capture,? during the period of performance of January 1, 2010 through September 30, 2013. This project involves the development of a novel technology that combines a dry sorbent-based carbon capture process with the water-gas-shift reaction for separating CO2 from syngas. The project objectives were to model, develop, synthesize and screen sorbents for CO2 capture from gasified coal streams. The project was funded by the DOE National Energy Technology Laboratory with URS as the prime contractor. Illinois Clean Coal Institute and The University of Illinois Urbana-Champaign were project co-funders. The objectives of this project were to identify and evaluate sorbent materials and concepts that were suitable for capturing carbon dioxide (CO2) from warm/hot water-gas-shift (WGS) systems under conditions that minimize energy penalties and provide continuous gas flow to advanced synthesis gas combustion and processing systems. Objectives included identifying and evaluating sorbents that efficiently capture CO2 from a gas stream containing CO2, carbon monoxide (CO), and hydrogen (H2) at temperatures as high as 650 °C and pressures of 400-600 psi. After capturing the CO2, the sorbents would ideally be regenerated using steam, or other condensable purge vapors. Results from the adsorption and regeneration testing were used to determine an optimal design scheme for a sorbent enhanced water gas shift (SEWGS) process and evaluate the technical and economic viability of the dry sorbent approach for CO2 capture. Project work included computational modeling, which was performed to identify key sorbent properties for the SEWGS process. Thermodynamic modeling was used to identify optimal physical properties for sorbents and helped down-select from the universe of possible sorbent materials to seven that were deemed thermodynamically viable for the process. Molecular modeling was used to guide sorbent synthesis through first principles simulations of adsorption and regeneration. Molecular dynamics simulations also modeled the impact of gas phase impurities common in gasified coal streams (e.g., H2S) on the adsorption process. The role of inert dopants added for mechanical durability to active sorbent materials was also investigated through molecular simulations. Process simulations were conducted throughout the project to help determine the overall feasibility of the process and to help guide laboratory operating conditions. A large component of the program was the development of sorbent synthesis methods. Three different approaches were used: mechanical alloying (MA), flame spray pyrolysis (FSP), and ultrasonic spray pyrolysis (USP). Sorbents were characterized by a host of analytical techniques and screened for SEWGS performance using a thermogravimetric analyzer (TGA). A feedback loop from screening efforts to sorbent synthesis was established and used throughout the project lifetime. High temperature, high pressure reactor (HTPR) systems were constructed to test the sorbents at conditions mimicking the SEWGS process as identified through process modeling. These experiments were conducted at the laboratory scale to examine sorbents for their CO2 capacity, conversion of CO to CO2, and impacts of adsorption and regeneration conditions, and syngas composition (including impurities and H2O:CO ratio). Results from the HTPR testing showed sorbents with as high as 0.4 g{sub CO2}/g{sub sorbent} capacity with the ability to initially shift the WGS completely towards CO2/H2. A longer term experiment with a simple syngas matrix and N2/steam regeneration stream showed a USP sorbent to be stable through 50 adsorption-regeneration cycles, though the sorbent tested had a somewhat diminished initial capacity. The program culminated in a technoeconomic assessment in which two different approaches were taken; one a ...
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The operational characteristics of a hot gas desulfurization process involving regenerable sorbent injection and its subsequent collection with a ceramic filtration device were studied utilizing a bench-scale transport reactor. Hydrogen sulfide removal from simulated hot gas was evaluated as a function of both zinc oxide-based sorbent physical and chemical characteristics and various process parameters. In addition, the sorbent capture efficiency and regenerability of the ceramic filtration device were evaluated, and regeneration of sulfided sorbents via injection into an oxidizing gas was studied. For both sorbent sulfidation and spent sorbent regeneration, gas-solid reaction occurred both in the duct and within layers of partially reacted sorbent captured by the ceramic filter. Very high sulfur removal efficiencies were obtained only in highly reducing hot gas compositions at or above about 700 C, using stoichiometric ratio (defined as ZnO/H[sub 2]S ratio) values of about 1.5, and sorbent particles of about 20[micro]m or less in diameter. Under such conditions, the experimental data indicated that reaction of H[sub 2]S with zinc vapor formed by reduction of zinc oxide contributed appreciably to sulfur removal. Negligible zinc loss from the hot zone of the reactor was detected, apparently due to rapid formation of zinc sulfide product layers on zinc oxide particles. The ceramic filtration devices captured 100% of all sorbent particles and were fully regenerable over periods of several tens of injection/backpulse cleaning cycles. Spent sorbent could be fully regenerated rapidly at 850 C without problems due to exotherm generation.
