Atomic Cu Sites Engineering Enables Efficient CO2 Electroreduction to Methane with High CH4/C2H4 Ratio

Abstract

HighlightsThe Cu-doped graphitic carbon nitride (g-C3N4) material is synthesized by an in situ thermal polymerization strategy, through which the atomic dispersion and coordination structure of Cu on g-C3N4 are realized by regulating the doping level of Cu.High Faraday efficiency of CH4 of 49.04% and a maximum CH4/C2H4 ratio up to 35.03 are achieved for the first time on g-C3N4-supported Cu single-atom catalyst.Structure–activity relationship analysis based on experimental and theoretical studies demonstrates the well-defined Cu single atoms coordinated with N atoms in the nitrogen cavity of g-C3N4 are active sites for CO2-to-CH4.