Manipulating Au−CeO 2 Interfacial Structure Toward Ultrahigh Mass Activity and Selectivity for CO 2 Reduction

Deploying the application of Au‐based catalysts directly on CO 2 reduction reactions (CO 2 RR) relies on the simultaneous improvement of mass activity (usually lower than 10 mA mg −1 Au at −0.6 V) and selectivity. To achieve this target, we herein manipulate the interface of small‐size Au (3.5 nm) and CeO 2 nanoparticles through adjusting the surface charge of Au and CeO 2 . The well‐regulated interfacial structure not only guarantees the utmost utilization of Au, but also enhances the CO 2 adsorption. Consequently, the mass activity (CO) of the optimal AuCeO 2 /C catalyst reaches 139 mA mg −1 Au with 97 % CO faradaic efficiency (FE CO ) at −0.6 V. Moreover, the strong interaction between Au and CeO 2 endows the catalyst with excellent long‐term stability. This work affords a charge‐guided approach to construct the interfacial structure for CO 2 RR and beyond.