Enhanced conversion of CO₂ into C₂H₄ on single atom Cu-anchored graphitic carbon nitride: Synergistic diatomic active...

Single atom metal-nitrogen-carbon materials have emerged as remarkably potent catalysts, demonstrating unprecedented potential for the photo-driven reduction of CO₂. Herein, a unique Cu@g-C₃N₅ catalyst obtained by cooperation of single atom Cu and nitrogen-rich g-C₃N₅ is proposed. The particular CuN diatomic active sites (DAS) in Cu@g-C₃N₅ contribute to the formation of highly stable CuOCN adsorption, a key configuration for CO₂ activation and CC coupling. The synergistic diatomic active sites interaction is found responsible for the efficient photoreduction of CO₂ to C₂H₄ which has been demonstrated in our Gibbs free energy calculation and COHP analysis. The CO₂ activation mechanism was studied, the charge density difference and DOS analysis show that the low oxidation state Cu atom significantly affects the electronic structure of g-C₃N₅ and then enhance the catalytic activity of CO₂ hydrogenation.