Construction of coherent interface between Cu2O and CeO2 via electrochemical reconstruction for efficient carbon dioxide reduction to methane

Developing an efficient electrocatalyst that enables the efficient electrochemical conversion from CO2 to CH4 across a wide potential range remains a formidable challenge. Herein, we introduce a precatalyst strategy that realizes the in situ electrochemical reconstruction of ultrafine Cu2O nanodomains, intricately coupled on the CeO2 surface (Cu2O/CeO2), originating from the heterointerface comprised of ultrafine CuO nanodomains on the CeO2 surface (CuO/CeO2). When served as the electrocatalyst for the electrochemical CO2 reduction reaction, Cu2O/CeO2 delivers a selectivity higher than 49 % towards CH4 over a broad potential range from −1.2 V to −1.7 V vs. RHE, maintaining negligible activity decay for 20 h. Notably, the highest selectivity for CH4 reaches an impressive 70 % at −1.5 V vs. RHE. Through the combination of comprehensive analysis including synchrotron X-ray absorption spectroscopy, spherical aberration-corrected high-angle annular dark field scanning transmission electron microscope as well as the density functional theoretical calculation, the efficient production of CH4 is attributed to the coherent interface between Cu2O and CeO2, which could converted from the original CuO and CeO2 interface, ensuring abundant active sites and enhanced intrinsic activity and selectivity towards CH4.