Producing liquid fuels with high selectivity and low overpotential has long been a goal of electrocatalytic CO2 reduction reaction (CO2RR). Here we present a detailed study on the structural and catalytic properties of sulfur on copper for CO2RR. Cu2S was formed by enabling sulfur to deposit on the copper surface with a simple surface impregnation method. The sulfur modified samples, especially the sulfur modified oxide-derived copper (SM-OD-Cu), have significantly higher selectivity to formate than the pure and oxide-derived copper. At a potential range of -0.51∼-0.75 V vs. RHE, the selectivity of formate for SM-OD-Cu in the liquid phase was nearly 100%. Also, the partial current density of formate reached -4.26 mA/cm2 at -0.75 V vs. RHE. By using density functional theory calculation, we found that Cu2S significantly inhibits the CO pathway and hydrogen evolution reaction, and further improves the selectivity of formate.
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