Theoretical exploration on the performance of single and dual-atom Cu catalysts on the CO2 electroreduction process: a DFT study

Carbon dioxide (CO2) electroreduction by metal-nitrogen-doped carbon (MNC) catalysts is a promising and efficient method to mitigate global warming by converting CO2 molecules to value-added chemicals. In this research, we systematically studied the behaviours of single and dual-atom Cu catalysts during the CO2 electroreduction process using density functional theory (DFT) calculations. Two structures, i.e., CuNC-4-pyridine and CuCuNC-4a, were found to be beneficial for C-2 chemical generation with relatively high stabilities. Subsequently, we explored the detailed pathways of key products (CO, HCOOH, CH3OH, CH4, C2H6O, C2H4 and C2H6) during CO2 electroreduction on CuNC-4-pyridine and CuCuNC-4a. This research reveals the mechanisms of key product formation during CO2 electroreduction on CuNC-4-pyridine and CuCuNC-4a, which would provide important insights to guide the design of MNC catalysts with low limiting potentials and high product selectivity.