Engineering a Cu/ZnOx Interface for High Methane Selectivity in CO2 Electrochemical Reduction

An oxidized copper species (Cu delta+) on the metallic copper surface is critical to the activity and selectivity of electrochemical reduction of CO2 gas. However, Cu delta+ species are easily reduced under working conditions of CO2 electroreduction. Herein, we propose an interface engineering strategy to stabilize Cu delta+ species; specifically, ZnOx nanoparticles are grown on a copper foil to generate a Cu/ZnOx interface. The interface stabilizes the surface Cu2+ species and delivers high methane selectivity (similar to 36%) and long-term durability (>12 h) at a potential of -1.1 V versus reversible hydrogen electrode (RHE) for CO2 reduction. By combining comprehensive characterizations with simulation experiments, we identify cupric species as active sites for CH4 formation, which is confirmed by density functional theory calculations. Our work demonstrates that interface engineering is a promising way to stabilize active sites and boost selective CO2 electroreduction.

Automated summary

The study proposes an interface engineering strategy to stabilize Cu delta+ species for electrochemical reduction of CO2 gas, achieving high methane selectivity and long-term durability. Characterizations and simulation experiments confirm cupric species as active sites for CH4 formation, demonstrating the promising potential of interface engineering in boosting selective CO2 electroreduction.