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

Electrochemical reduction of CO2 to value-added chemicals by using renewable electricity offers a promising strategy to deal with rising CO2 emission and the energy crisis. Single-site zinc-coordinated nitrogen-codoped graphene (Zn-N-G) catalyzes the electrochemical reduction of CO2 to CO. The Zn-N-G catalyst exhibits excellent intrinsic activity toward CO2 reduction, reaching a faradaic efficiency of 91% for CO production at a low overpotential of 0.39V. 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 CO2 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 CO2 to CO.