Trends in CO2 and H2O uptakes by solid K2CO3 were studied at different carbonation temperatures and flue gas compositions over 50 consecutive regeneration carbonation cycles. Differences in carbonation behavior between the initial and final cycles evidence changes in the phase composition of K2CO3 during cycling, which stabilize in accordance with the operating conditions. Rates of carbonation and hydration were observed to decrease at higher temperatures, indicating that the forward reactions are limited by adsorption, not chemical reaction. Multiple regression analysis of the uptake data yielded negative apparent activation energies for both forward reactions modeled as simple chemical reactions, thus proving the assumption invalid. A proposed Langmuir-Hinshelwood model yielded consistent apparent activation energies for the forward reactions, showing that adsorption limitations are significant in this chemisorption process. Important process design considerations, for realizing high carbonation rates and selecting promising support materials to enhance the CO2 capture capacity of K2CO3, are also discussed.