Carbon Dioxide Capture from Flue Gas Using Dry Regenerable Sorbents (2004)

Laboratory studies were conducted to investigate dry, regenerable, alkali carbonate-based sorbents for the capture of CO{sub 2} from power plant flue gas. Electrobalance, fixed-bed and fluid-bed reactors were used to examine both the CO{sub 2} capture and sorbent regeneration phases of the process. Sodium carbonate-based sorbents (calcined sodium bicarbonate and calcined trona) were the primary focus of the testing. Supported sodium carbonate and potassium carbonate sorbents were also tested. Sodium carbonate reacts with CO{sub 2} and water vapor contained in flue gas at temperatures between 60 and 80 C to form sodium bicarbonate, or an intermediate salt (Wegscheider's salt). Thermal regeneration of this sorbent produces an off-gas containing equal molar quantities of CO{sub 2} and H{sub 2}O. The low temperature range in which the carbonation reaction takes place is suited to treatment of coal-derived flue gases following wet flue gas desulfurization processes, but limits the concentration of water vapor which is an essential reactant in the carbonation reaction. Sorbent regeneration in an atmosphere of CO{sub 2} and water vapor can be carried out at a temperature of 160 C or higher. Pure CO{sub 2} suitable for use or sequestration is available after condensation of the H{sub 2}O. Flue gas contaminants such as SO{sub 2} react irreversibly with the sorbent so that upstream desulfurization will be required when sulfur-containing fossil fuels are used. Approximately 90% CO{sub 2} capture from a simulated flue gas was achieved during the early stages of fixed-bed reactor tests using a nominal carbonation temperature of 60 C. Effectively complete sorbent carbonation is possible when the fixed-bed test is carried out to completion. No decrease in sorbent activity was noted in a 15-cycle test using the above carbonation conditions coupled with regeneration in pure CO{sub 2} at 160 C. Fluidized-bed reactor tests of up to five cycles were conducted. Carbonation of sodium carbonate in these tests is initially very rapid and high degrees of removal are possible. The exothermic nature of the carbonation reaction resulted in a rise in bed temperature and subsequent decline in removal rate. Good temperature control, possibly through addition of supplemental water and evaporative cooling, appears to be the key to getting consistent carbon dioxide removal in a full-scale reactor system. The tendency of the alkali carbonate sorbents to cake on contact with liquid water complicates laboratory investigations as well as the design of larger scale systems. Also their low attrition resistance appears unsuitable for their use in dilute-phase transport reactor systems. Sodium and potassium carbonate have been incorporated in ceramic supports to obtain greater surface area and attrition resistance, using a laboratory spray dryer. The caking tendency is reduced and attrition resistance increased by supporting the sorbent. Supported sorbents with loading of up to 40 wt% sodium and potassium carbonate have been prepared and tested. These materials may improve the feasibility of large-scale CO{sub 2} capture systems based on short residence time dilute-phase transport reactor systems.