Single-Atom Cu anchored polymeric carbon nitride for enhanced one-step plasma-catalytic conversion of CH4 and CO2 into acetic acid

Non-thermal plasma is one of the most promising technologies for converting CH4 and CO2 into value-add chemicals under ambient pressure and room temperature. However, the challenge still lies in exploring efficient catalysts and deeply clarifying the relationship between the structure of catalyst and its catalytic performance. Herein, the Cu single-atom (Cu-N4 coordination structure) anchored in carbon nitride catalyst (CuSA-CN) is prepared by coordination pyrolysis, which not only efficiently enhances the plasma-catalytic conversion of CH4 and CO2 with high selectivity of CH3COOH, but exhibits a good stability. Characterizations and DFT calculations reveal that the combination of the excellent physical discharge properties and the charge transfer between Cu single atom and carrier is beneficial for activating of CH4 and CO2. Meanwhile, Cu single-atoms reduce the energy barriers of CH4 dissociation and C-C coupling, thereby promoting CH3COOH generation. This work provides new insights into designing single-atom catalysts for application in non-thermal plasma catalytic reactions.