Utilizing transition metal hydricity and thermochemical cycles, a method for determining optimal conditions for the selective, electrocatalytic reduction of CO2 while disfavoring the proton reduction pathway is discussed. This thermodynamic approach for selective CO2 reduction by two electrons to formate is demonstrated using controlled potential electrolysis employing several transition metal complexes in various solvents. The Faradaic efficiency of the reduction products, H2 and formate, can be tuned by varying the proton activity. This method aims to facilitate the development of electrocatalysts for selective reduction of CO2 in the presence of protons, which are often required to generate the intermediate metal hydride.

Selective reduction of CO2: A rational thermodynamic approach to disfavor proton reduction pathways

255th National Meeting (2018)

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