Results of experimental tests into the equilibrium and column dynamic data for the chemisorption of CO2 on two materials has identified the materials as potential candidates for the capture of CO2. The first of the materials is a K2CO3 - promoted hydrotalcite that displays good sorption capacity in 400-500 °C range. The second is a Na2O -promoted alumina that has shown good sorption capacity in 250-400 °C temperature range. The two materials both exhibited Langmuirian behavior in the low pressure region, but deviated substantially in higher pressure regions. A new analytical model that simultaneously accounts for Langmuirian chemisorption and an additional surface complexation reaction between gaseous and sorbed CO2 has been proposed to describe the measured equilibrium data for both materials. Experimental breakthrough tests showed fast kinetics and narrow mass transfer zones for CO2 adsorption. The isosteric heats of chemisorption and heats of additional complexation reaction on both materials were estimated to be low, indicating that desorption of CO2 from both materials could be achieved with relative ease. Tests have confirmed that both materials show stable sorption capacity after several sorption-desorption cycles. These characteristics make them attractive candidates for use in cyclic processes for the capture of CO2. The Na2O promoted alumina shows promise as a candidate for capture of CO2 from flue gas of a coal fired power plant, while the K2CO3 promoted hydrotalcite will be a better candidate for the Sorption Enhanced Reaction process to simultaneously produce fuel cell grade H2 and high purity CO2 at feed gas pressure.