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Title: A calcium oxide sorbent process for bulk separation of carbon dioxide. Quarterly progress report No. 18, October 1993--December 1993

Abstract

This research project is investigating the technical feasibility of a high-temperature, high-pressure (HTHP) process for the bulk separation of CO{sub 2} from coal-derived gas. Phase I research, in which an electrobalance reactor was used to establish the technical feasibility of the regenerable sorbent process, was completed in March 1992 and results have been fully described in earlier quarterly reports. In Phase I, the calcination and carbonation characteristics of three calcium sorbents were studied as a function of calcination and carbonation temperature and pressure, mol fraction CO{sub 2} in the carbonation gas, and carbonation background gas composition. Desirable reaction conditions required for high reactivity and good sorbent durability were determined. Multicycle tests consisting of as many as ten complete calcination and carbonation cycles were completed. Indirect evidence which suggested that the water-gas shift reaction occurred simultaneously with CO{sub 2} removal was found. Occurrence of the simultaneous reactions created the possibility of a direct one-step process for the manufacture of hydrogen from coal-gas while at the same time separating a concentrated stream of CO{sub 2}. The concentrated CO{sub 2} stream could be quite significant if, in the future, environmental regulations restrict atmospheric CO{sub 2}, emissions.

Authors:
Publication Date:
Research Org.:
Louisiana State Univ., Baton Rouge, LA (United States). Dept. of Chemical Engineering
Sponsoring Org.:
USDOE, Washington, DC (United States)
OSTI Identifier:
10157238
Report Number(s):
DOE/MC/26366-3758
ON: DE94013215; BR: AA8575000
DOE Contract Number:
AC21-89MC26366
Resource Type:
Technical Report
Resource Relation:
Other Information: PBD: Jan 1994
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 01 COAL, LIGNITE, AND PEAT; 08 HYDROGEN; CARBON DIOXIDE; MATERIALS RECOVERY; ABSORPTION; CALCIUM OXIDES; SORPTIVE PROPERTIES; SEPARATION PROCESSES; COAL GASIFICATION; COAL GAS; WATER GAS PROCESSES; SHIFT PROCESSES; CARBON MONOXIDE; OXIDATION; HYDROGEN PRODUCTION; PROGRESS REPORT; CALCINATION; REGENERATION; TEMPERATURE DEPENDENCE; PRESSURE DEPENDENCE; FEASIBILITY STUDIES; EXPERIMENTAL DATA; 540120; 010404; 080107; CHEMICALS MONITORING AND TRANSPORT; GASIFICATION

Citation Formats

Harrison, D.P. A calcium oxide sorbent process for bulk separation of carbon dioxide. Quarterly progress report No. 18, October 1993--December 1993. United States: N. p., 1994. Web. doi:10.2172/10157238.
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Harrison, D.P. A calcium oxide sorbent process for bulk separation of carbon dioxide. Quarterly progress report No. 18, October 1993--December 1993. United States. doi:10.2172/10157238.
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Harrison, D.P. Sat . "A calcium oxide sorbent process for bulk separation of carbon dioxide. Quarterly progress report No. 18, October 1993--December 1993". United States. doi:10.2172/10157238. https://www.osti.gov/servlets/purl/10157238.
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@article{osti_10157238,
title = {A calcium oxide sorbent process for bulk separation of carbon dioxide. Quarterly progress report No. 18, October 1993--December 1993},
author = {Harrison, D.P.},
abstractNote = {This research project is investigating the technical feasibility of a high-temperature, high-pressure (HTHP) process for the bulk separation of CO{sub 2} from coal-derived gas. Phase I research, in which an electrobalance reactor was used to establish the technical feasibility of the regenerable sorbent process, was completed in March 1992 and results have been fully described in earlier quarterly reports. In Phase I, the calcination and carbonation characteristics of three calcium sorbents were studied as a function of calcination and carbonation temperature and pressure, mol fraction CO{sub 2} in the carbonation gas, and carbonation background gas composition. Desirable reaction conditions required for high reactivity and good sorbent durability were determined. Multicycle tests consisting of as many as ten complete calcination and carbonation cycles were completed. Indirect evidence which suggested that the water-gas shift reaction occurred simultaneously with CO{sub 2} removal was found. Occurrence of the simultaneous reactions created the possibility of a direct one-step process for the manufacture of hydrogen from coal-gas while at the same time separating a concentrated stream of CO{sub 2}. The concentrated CO{sub 2} stream could be quite significant if, in the future, environmental regulations restrict atmospheric CO{sub 2}, emissions.},
doi = {10.2172/10157238},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Sat Jan 01 00:00:00 EST 1994},
month = {Sat Jan 01 00:00:00 EST 1994}
}
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Technical Report:
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DOI:  10.2172/10157238
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  • The original contract f or two years was awarded in September 1989 as a result of solicitation number DE-RA21-89MC26040 entitled ``Novel Concepts for Bulk Separation of Gases in Coal Gasification Systems.`` Two no-cost extensions without a change in the statement of work extended the performance period by six months to March 1992. At that time a two-year contract extension with an enlarged scope of work and additional funding was approved so that the research is now scheduled to end in March 1994. Phase I research, in which an electrobalance reactor was used to establish the technical feasibility of the regenerablemore » sorbent process, was completed in March 1992 and results have been fully described in earlier quarterly reports. In Phase I, the calcination and carbonation characteristics of three calcium sorbents were studied as a function of calcination and carbonation temperature and pressure, mol fraction CO{sub 2} in the carbonation gas, and carbonation background gas composition. Desirable reaction conditions required for high reactivity and good sorbent durability were determined. Multicycle tests consisting of as many as ten complete calcination and carbonation cycles were completed. Indirect evidence which suggested that the water-gas shift reaction occurred simultaneously with CO{sub 2} removal was found. Occurrence of the simultaneous reactions created the possibility of a direct one-step process for the manufacture of hydrogen from coal-gas while at the same time separating a concentrated stream of CO{sub 2} The concentrated CO{sub 2} stream could be quite significant if, in the future, environmental regulations restrict atmospheric CO{sub 2} emissions.« less

  • ; ;
    The expected commercialization of coal gasification technology in the US and world-wide will create a need for advanced gas purification and separation processes capable of operating at higher temperatures and in more hostile environments than is common today. For example, a high-temperature, high-pressure process capable of separating CO{sub 2} from coal-derived gas may find application in purifying synthesis gas for H{sub 2}, NH{sub 3}, or CH{sub 3}OH production. High temperature CO{sub 2} removal has the potential for significantly improving the operating efficiency of integrated gasification-molten carbonate fuel cells for electric power generation. This study proved the technical feasibility of amore » CO{sub 2}-separation process based upon the regenerable noncatalytic gas-solid reaction between CaO and CO{sub 2} to form CACO{sub 3}. Such a process operating at 650{degree}C and 15 atm with 15% CO{sub 2} in the coal gas has the potential for removing in excess of 99% of the CO{sub 2} fed. Selection of a sorbent precursor which, upon calcination, produces high-porosity CaO is important for achieving rapid and complete reaction. The addition of magnesium to the sorbent appears to improve the multicycle durability at a cost of reduced CO{sub 2} capacity per unit mass of sorbent. Reaction conditions, principally calcination and carbonation temperatures, are important factors in multicycle durability. Reaction pressure and CO{sub 2} concentration are important in so far as the initial rapid reaction rate is concerned, but are relatively unimportant in terms of sorbent capacity and durability. Indirect evidence for the simultaneous occurrence of the shift reaction and CO{sub 2}-removal reaction creates the possibility of a direct one-step process for the production of hydrogen from coal-derived gas.« less

  • Phase I research, in which an electrobalance reactor was used to establish the technical feasibility of the regenerable sorbent process, was completed in March 1992 and results have been fully described in earlier quarterly reports. In Phase I, the calcination and carbonation characteristics of three calcium sorbents were studied as a function of calcination and carbonation temperature and pressure, mol fraction CO{sub 2} in the carbonation gas, and carbonation background gas composition. Desirable reaction conditions required for high reactivity and good sorbent durability were determined. Multicycle tests consisting of as many as ten complete calcination and carbonation cycles were completed.more » Indirect evidence which suggested that the water-gas shift reaction occurred simultaneously with CO{sub 2} removal was found. Occurrence of the simultaneous reactions created the possibility of a direct one-step process for the manufacture of hydrogen from coal-gas while at the same time separating a concentrated stream of CO{sub 2}. The concentrated CO{sub 2} stream could be quite significant if, in the future, environmental regulations restrict atmospheric CO{sub 2} emissions.« less

  • This research project is investigating the technical feasibility of a high-temperature, high pressure (HTHP) process for the bulk separation Of CO{sub 2} from coal-derived gas. Phase I research, in which an electrobalance reactor was used to establish the technical feasibility of the regenerable sorbent process, was completed in March 1992 and results have been fully described in earlier quarterly reports. In Phase 1, the calcination and carbonation characteristics of three calcium sorbents were studied as a function of calcination and carbonation temperature and pressure, mol fraction CO{sub 2} in the carbonation gas, and carbonation background gas composition. Desirable reaction conditionsmore » required for high reactivity and good sorbent durability were determined. Multicycle tests consisting of as many as ten complete calcination and carbonation cycles were completed. Indirect evidence which suggested that the water-gas shift reaction occurred simultaneously with CO{sub 2} removal was found. Occurrence of the simultaneous reactions created the possibility of a direct one-step process for the manufacture of hydrogen from coal-gas while at the same time separating a concentrated stream of CO{sub 2}The concentrated CO{sub 2} Stream could be quite significant if, in the future, environmental regulations restrict atmospheric CO{sub 2} emissions.« less

  • Phase II research involves a scale-up from microgram to gram quantities of sorbent and a switch from the electrobalance reactor to a fixed-bed reactor with capability for feed and product gas analysis. Parameters being studied in Phase II are essentially the same as in Phase I. The reactor response is being studied as a function of calcination and carbonation temperature and pressure, composition of the calcination and carbonation feed gas, and space velocity during the carbonation cycle. Multicycle tests are also being conducted to extend the information on sorbent durability. During the current quarter, reactor modifications to permit easier additionmore » and removal of sorbent to and from the reactor were accomplished. It is now possible to remove sorbent after a run in discrete axial sections which will permit characterization of the sorbent as a function of axial position. Tracer response tests in which the chromatograph response to step function injections of hydrogen to flowing nitrogen under non-reactive conditions were carried out to evaluate the lag time between feeding reactive gases to the reactor and their appearance in the product gas sample. Fourteen additional calcination/carbonation reaction tests were completed this quarter, and the effects of carbonation background gas composition, sorbent particle size, calcination temperature, calcination gas flow rate, and calcination gas composition were studied. In addition, the first multicycle test involving complete calcination/carbonation cycles was carried out.« less