Theoretical exploration on the performance of single and dual-atom Cu catalysts on the CO 2 electroreduction process: a DFT study.

Carbon dioxide (CO 2 ) electroreduction by metal-nitrogen-doped carbon (MNC) catalysts is a promising and efficient method to mitigate global warming by converting CO 2 molecules to value-added chemicals. In this research, we systematically studied the behaviours of single and dual-atom Cu catalysts during the CO 2 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, CH 3 OH, CH 4 , C 2 H 6 O, C 2 H 4 and C 2 H 6 ) during CO 2 electroreduction on CuNC-4-pyridine and CuCuNC-4a. This research reveals the mechanisms of key product formation during CO 2 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.