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.