The noncatalytic gas-solid reaction between calcined dolomite and CO2(g) has been studied in an electrobalance reactor as a function of temperature, pressure, and reactive gas composition. Multicycle tests consisting of as many as ten complete calcination-carbonation cycles were carried out to obtain information on sorbent durability. Surface area, pore volume, and pore size distribution measurements were made to supplement the reaction studies. This reaction is of interest both as a model for studying (he importance of structural property changes in gas-solid reactions, and as the basis for a possible process for the high temperature separation of CO2from gas streams.