Long duration activities by man in space requires a regenerable CO2 removal system. Current systems under study include those based on the oxygen/hydrogen fuel cell and an amine resin. Both approaches are based on well-known acid-base chemistry of CO2. Our efforts are directed at the development of electroactive CO2 carrier molecules that are capable of binding CO2 when in the reduced form and releasing CO2 in the oxidized form. The successful development of these carriers would provide the chemical basis for a more efficient CO2 removal system and offers other potential advantages as well. The general requirements and advantages of electroactive CO2 carrier molecules are discussed. In addition, studies on carrier molecules which demonstrate the feasibility of this approach are described.