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Title: CARBON DIOXIDE CAPTURE FROM FLUE GAS USING DRY REGENERABLE SORBENTS

Abstract

This report describes research conducted between April 1, 2004 and June 30, 2004 on the preparation and use of dry regenerable sorbents for removal of carbon dioxide from flue gas. Support materials and supported sorbents were prepared by spray drying. Sorbents consisting of 20 to 50% sodium carbonate on a ceramic support were prepared by spray drying in batches of approximately 300 grams. The supported sorbents exhibited greater carbon dioxide capture rates than unsupported calcined sodium bicarbonate in laboratory tests. Preliminary process design and cost estimation for a retrofit application suggested that costs of a dry regenerable sodium carbonate-based process could be lower than those of a monoethanolamine absorption system. In both cases, the greatest part of the process costs come from power plant output reductions due to parasitic consumption of steam for recovery of carbon dioxide from the capture medium.

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Research Triangle Institute (US)
Sponsoring Org.:
(US)
OSTI Identifier:
829536
DOE Contract Number:
FC26-00NT40923
Resource Type:
Technical Report
Resource Relation:
Other Information: PBD: 1 Jul 2004
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; ABSORPTION; ACID CARBONATES; CARBON DIOXIDE; CERAMICS; COST ESTIMATION; DESIGN; FLUE GAS; SODIUM CARBONATES; AIR POLLUTION CONTROL

Citation Formats

David A. Green, Brian S. Turk, Jeffrey W. Portzer, Raghubir P. Gupta, William J. McMichael, and Thomas Nelson. CARBON DIOXIDE CAPTURE FROM FLUE GAS USING DRY REGENERABLE SORBENTS. United States: N. p., 2004. Web. doi:10.2172/829536.
David A. Green, Brian S. Turk, Jeffrey W. Portzer, Raghubir P. Gupta, William J. McMichael, & Thomas Nelson. CARBON DIOXIDE CAPTURE FROM FLUE GAS USING DRY REGENERABLE SORBENTS. United States. doi:10.2172/829536.
David A. Green, Brian S. Turk, Jeffrey W. Portzer, Raghubir P. Gupta, William J. McMichael, and Thomas Nelson. 2004. "CARBON DIOXIDE CAPTURE FROM FLUE GAS USING DRY REGENERABLE SORBENTS". United States. doi:10.2172/829536. https://www.osti.gov/servlets/purl/829536.
@article{osti_829536,
title = {CARBON DIOXIDE CAPTURE FROM FLUE GAS USING DRY REGENERABLE SORBENTS},
author = {David A. Green and Brian S. Turk and Jeffrey W. Portzer and Raghubir P. Gupta and William J. McMichael and Thomas Nelson},
abstractNote = {This report describes research conducted between April 1, 2004 and June 30, 2004 on the preparation and use of dry regenerable sorbents for removal of carbon dioxide from flue gas. Support materials and supported sorbents were prepared by spray drying. Sorbents consisting of 20 to 50% sodium carbonate on a ceramic support were prepared by spray drying in batches of approximately 300 grams. The supported sorbents exhibited greater carbon dioxide capture rates than unsupported calcined sodium bicarbonate in laboratory tests. Preliminary process design and cost estimation for a retrofit application suggested that costs of a dry regenerable sodium carbonate-based process could be lower than those of a monoethanolamine absorption system. In both cases, the greatest part of the process costs come from power plant output reductions due to parasitic consumption of steam for recovery of carbon dioxide from the capture medium.},
doi = {10.2172/829536},
journal = {},
number = ,
volume = ,
place = {United States},
year = 2004,
month = 7
}

Technical Report:

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  • Electrobalance studies of calcination and carbonation of sodium bicarbonate materials were conducted at Louisiana State University. Calcination in an inert atmosphere was rapid and complete at 120 C. Carbonation was temperature dependent, and both the initial rate and the extent of reaction were found to decrease as temperature was increased between 60 and 80 C. A fluidization test apparatus was constructed at RTI and two sodium bicarbonate materials were fluidized in dry nitrogen at 22 C. The bed was completely fluidized at between 9 and 11 in. of water pressure drop. Kinetic rate expression derivations and thermodynamic calculations were conductedmore » at RTI. Based on literature data, a simple reaction rate expression, which is zero order in carbon dioxide and water, was found to provide the best fit against reciprocal temperature. Simulations based on process thermodynamics suggested that approximately 26 percent of the carbon dioxide in flue gas could be recovered using waste heat available at 240 C.« less
  • The objective of this project is to develop a simple, inexpensive process to separate CO{sub 2} as an essentially pure stream from a fossil fuel combustion system using a regenerable, sodium-based sorbent. The sorbent being used in this project is sodium carbonate which is converted to sodium bicarbonate, ''baking soda,'' through reaction with carbon dioxide and water vapor. Sodium bicarbonate is regenerated to sodium carbonate when heated, producing a nearly pure CO{sub 2} stream after condensation of water vapor. Testing conducted previously confirmed that the reaction rate and achievable CO{sub 2} capacity of sodium carbonate decreased with increasing temperature, andmore » that the global rate of reaction of sodium carbonate to sodium bicarbonate increased with an increase in both CO{sub 2} and H{sub 2}O concentrations. Energy balance calculations indicated that the rate of heat removal from the particle surface may determine the reaction rate for a particular particle system. This quarter, thermogravimetric analyses (TGA) were conducted which indicated that calcination of sodium bicarbonate at temperatures as high as 200 C did not cause a significant decrease in activity in subsequent carbonation testing. When sodium bicarbonate was subjected to a five cycle calcination/carbonation test, activity declined slightly over the first two cycles but was constant thereafter. TGA tests were also conducted with two other potential sorbents. Potassium carbonate was found to be less active than sodium carbonate, at conditions of interest in preliminary TGA tests. Sodium carbonate monohydrate showed negligible activity. Testing was also conducted in a 2-inch internal diameter quartz fluidized-bed reactor system. A five cycle test demonstrated that initial removals of 10 to 15 percent of the carbon dioxide in a simulated flue gas could be achieved. The carbonation reaction proceeded at temperatures as low as 41 C. Future work by TGA and in fixed-bed, fluidized-bed, and transport reactor systems is planned to demonstrate the feasibility of this process in large scale operations to separate carbon dioxide from flue gas.« less
  • The objective of this project is to develop a simple, inexpensive process to separate CO{sub 2} as an essentially pure stream from a fossil fuel combustion system using a regenerable, sodium-based sorbent. The sorbent being used in this project is sodium carbonate which is converted to sodium bicarbonate, or ''baking soda,'' through reaction with carbon dioxide and water vapor. Sodium bicarbonate is regenerated to sodium carbonate when heated, producing a nearly pure CO{sub 2} stream after condensation of water vapor. This quarter, five cycle thermogravimetric tests were conducted at the Louisiana State University (LSU) with sodium bicarbonate Grade 3 (SBC{number_sign}3)more » which showed that carbonation activity declined slightly over 5 cycles following severe calcination conditions of 200 C in pure CO{sub 2}. Three different sets of calcination conditions were tested. Initial carbonation activity (as measured by extent of reaction in the first 25 minutes) was greatest subsequent to calcination at 120 C in He, slightly less subsequent to calcination in 80% CO{sub 2}/20% H{sub 2}O, and lowest subsequent to calcination in pure CO{sub 2} at 200 C. Differences in the extent of reaction after 150 minutes of carbonation, subsequent to calcination under the same conditions followed the same trend but were less significant. The differences between fractional carbonation under the three calcination conditions declined with increasing cycles. A preliminary fixed bed reactor test was also conducted at LSU. Following calcination, the sorbent removed approximately 19% of the CO{sub 2} in the simulated flue gas. CO{sub 2} evolved during subsequent calcination was consistent with an extent of carbonation of approximately 49%. Following successful testing of SBC{number_sign}3 sorbent at RTI reported in the last quarter, a two cycle fluidized bed reactor test was conducted with trona as the sorbent precursor, which was calcined to sodium carbonate. In the first carbonation cycle, CO{sub 2} removal rates declined from 20% to about 8% over the course of three hours. Following calcination, a second carbonation cycle was conducted, at a lower temperature with a lower water vapor content. CO{sub 2} removal and sorbent capacity utilization declined under these conditions. Modifications were made to the reactor to permit addition of extra water for testing in the next quarter. Thermodynamic analysis of the carbonation reaction suggested the importance of other phases, intermediate between sodium carbonate and sodium bicarbonate, and the potential for misapplication of thermodynamic data from the literature. An analysis of initial rate data from TGA experiments suggested that the data may fit a model controlled by the heat transfer from the sorbent particle surface to the bulk gas.« less
  • The objective of this project is to develop a simple, inexpensive process to separate CO{sub 2} as an essentially pure stream from a fossil fuel combustion system using a regenerable, sodium-based sorbent. The sorbents being investigated in this project are primarily alkali carbonates, and particularly sodium carbonate and potassium carbonate, which are converted to bicarbonates, through reaction with carbon dioxide and water vapor. Bicarbonates are regenerated to carbonates when heated, producing a nearly pure CO{sub 2} stream after condensation of water vapor. This quarter, electrobalance tests conducted at LSU indicated that exposure of sorbent to water vapor prior to contactmore » with carbonation gas does not significantly increase the reaction rate. Calcined fine mesh trona has a greater initial carbonation rate than calcined sodium bicarbonate, but appears to be more susceptible to loss of reactivity under severe calcination conditions. The Davison attrition indices for Grade 5 sodium bicarbonate, commercial grade sodium carbonate and extra fine granular potassium carbonate were, as tested, outside of the range suitable for entrained bed reactor testing. Fluidized bed testing at RTI indicated that in the initial stages of reaction potassium carbonate removed 35% of the carbon dioxide in simulated flue gas, and is reactive at higher temperatures than sodium carbonate. Removals declined to 6% when 54% of the capacity of the sorbent was exhausted. Carbonation data from electrobalance testing was correlated using a shrinking core reaction model. The activation energy of the reaction of sodium carbonate with carbon dioxide and water vapor was determined from nonisothermal thermogravimetry.« less
  • Fossil fuels used for power generation, transportation, and by industry are the primary source of anthropogenic CO{sub 2} emissions to the atmosphere. Much of the CO{sub 2} emission reduction effort will focus on large point sources, with fossil fuel fired power plants being a prime target. The CO{sub 2} content of power plant flue gas varies from 4% to 9% (vol), depending on the type of fossil fuel used and on operating conditions. Although new power generation concepts that may result in CO{sub 2} control with minimal economic penalty are under development, these concepts are not generally applicable to themore » large number of existing power plants.« less