A DFT screening of transition metal single-atom catalyst anchored on Janus WSSe basal plane for highly efficient carbon dioxide reduction reaction

Electrochemical CO2 reduction reaction (CO2RR) can efficiently and selectively reduce carbon dioxide into chemical fuel. Here, we designed the novel catalysts of transition-metal atoms anchored on Janus WSSe basal plane (TM@SSe) monolayer by first-principles calculations. The results show that Zn@WSSe has the best CO2RR catalytic activity with limit potential of -0.32 V and a high selectivity for the competitive hydrogen precipitation reaction (HER). Moreover, ab initio molecular dynamics simulation (AIMD) calculation at 300 K indicated high thermodynamic stability of Zn@WSSe. The study of the rate limiting step (CO*+H++e(-) -> *CHO) of the Zn@WSSe structure illustrates that the CO2RR catalytic activity of these candidate catalysts largely depends on the better interaction between Zn atoms and surrounding W atoms, which H atom is more easily adsorbed to C atom, making the reaction process easier to achieve. The above research provides a new way to design efficient CO2RR electrocatalyst under ambient conditions.