Cu diatom anchored on carbon nitride nanosheet: an efficient channel for charge transfer to boost methane and carbon dioxide conversion to methanol

Efficient plasma-catalysis of CH4 and CO2 to value-added oxygenates remains challenging due to limited research on the activation and conversion mechanism of the *CO intermediate. The rational design of catalysts at the atomic level can improve mechanistic understanding. In this study, an atomically dispersed catalyst with diatomic Cu centers anchored on carbon nitride nanosheet is developed. The coordination structure of Cu diatoms with four N atoms and two C atoms provides a new channel for efficient charge transfer and separation, enhancing CH4 and CO2 conversion. Additionally, CO-DRIFT and theoretical calculations demonstrate that strong CO adsorption and the stable *CH3OH intermediate on Cu diatomic sites promote CH3OH generation. This study presents a viable strategy for designing novel diatomic catalyst for CH4 and CO2 conversion into value-added products, and expands understanding of the plasma-catalysis mechanism at the atomic level.