Efficient CO2 reduction for CO production using triatomic catalyst screening: A DFT study

Abstract

The electrochemical reduction of CO2 to produce CO has garnered significant interest in recent years. Despite the significant progress made, efficient electrocatalysts for CO2 Reduction Reaction are still lacking. On the basis of the SACs, the TACs expands the multi-active sites and improves the catalytic performance. In this work, we conduct a theoretical screening of transition metal TACs on graphdiyne (TM1TM2TM3@GY, TM = Mn, Fe, Co, Ni, Cu, and Mo) and systematically investigate their catalytic activity. The results reveal that MnMoCu@GY exhibits superior catalytic performance for CO2RR-to-CO, with a low limiting potential of −0.36 eV, as evidenced by adsorption configurations and electronic structure analyses. Furthermore, MnMoCu@GY significantly inhibits the competitive hydrogen evolution reaction. We also find that the d-band center and band gap, as well as the redistribution of charge, play a critical role in determining the energy of intermediates, and consequently, the activity and selectivity of TACs in CO2RR. Our theoretical study not only further extends the TACs, but also opens a new door to boost the sustainable CO2 conversion.