The efficient conversion of electrical energy and CO2 to fuels will be important for a flexible and sustainable energy supply in the future. This will require efficient methods for CO2 recovery and efficient catalysts for CO2 reduction. To achieve these goals will require an understanding of the contributions of both the first and second coordination spheres of molecules capable of binding CO2 and transforming them to reduced products. We will describe our most recent work on developing electroactive carrier molecules for selective concentration of CO2 and the development of electrocatalysts for the reduction of CO2 to CO. A major obstacle in the development of CO2 reduction catalysts is achieving reduction beyond CO or formate. Previous work in our laboratories has involved detailed thermodynamic studies of transition metal hydride complexes and formyl complexes, and this information has been used to guide the development stoichiometric reductions of coordinated CO molecules to form formyl complexes using H2 gas as the reductant at one atm pressure and at room temperature. Further progress in the application of thermodynamic models to the development of catalysts for CO2 and CO reduction will be described.