Dual‐Interfacial Electrocatalyst Enriching Surface Bonded H for Energy‐Efficient CO2‐to‐CH3OH Conversion

Abstract Energy cost is a long‐neglected but crucial issue for electrocatalytic carbon dioxide reduction reactions (CO 2 RRs). So far, achieving efficient CO 2 RR at a low energy cost is a major unresolved challenge. Herein, energy‐efficient CO 2 ‐to‐CH 3 OH conversion by synergistically increasing the amount of favorable intermediates and depressing H 2 generation is reported. The designed precursor electrocatalyst undergoes in situ reduction, forming Cu−C 60 and ZnO−Cu dual interfaces. Cu−C 60 induces an *H‐rich surface, decreasing the hydrogenation barrier and lowering the required voltage. *H‐modified ZnO‐Cu alters the mechanism of electron transfer and improves the conversion selectivity. As a result, at an applied potential as low as −0.63 V versus a reversible hydrogen electrode, a cathodic energy efficiency of 50.5% and a faradaic efficiency of 78.3% for CH 3 OH is obtained. This work unlocks an unconventional route for improving the catalytic performance and energy efficiency of electrocatalysts, addressing the concern of energy costs for electrocatalyzed CO 2 RR.