Zinc‐Coordinated Nitrogen‐Codoped Graphene as an Efficient Catalyst for Selective Electrochemical Reduction of CO2 to CO

Abstract Electrochemical reduction of CO 2 to value‐added chemicals by using renewable electricity offers a promising strategy to deal with rising CO 2 emission and the energy crisis. Single‐site zinc‐coordinated nitrogen‐codoped graphene (Zn–N–G) catalyzes the electrochemical reduction of CO 2 to CO. The Zn–N–G catalyst exhibits excellent intrinsic activity toward CO 2 reduction, reaching a faradaic efficiency of 91 % for CO production at a low overpotential of 0.39 V. X‐ray absorption fine structure and X‐ray photoelectron spectroscopy both confirm the presence of isolated Zn–N x moieties, which act as the key active sites for CO formation. DFT calculations reveal the origin of enhanced activity for CO 2 reduction on Zn–N–G catalysts. This work provide further understanding of the active centers on transition metal–nitrogen–carbon (M–N–C) catalysts for electrochemical reduction of CO 2 to CO.