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 (CO2RRs). So far, achieving efficient CO2RR at a low energy cost is a major unresolved challenge. Herein, energy‐efficient CO2‐to‐CH3OH conversion by synergistically increasing the amount of favorable intermediates and depressing H2 generation is reported. The designed precursor electrocatalyst undergoes in situ reduction, forming Cu−C60 and ZnO−Cu dual interfaces. Cu−C60 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 CH3OH 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 CO2RR.

Experimental and DFT Study of Electrochemical Promotion of Cu/ZnO Catalysts for the Reverse Water Gas Shift Reaction

“…This provides an opportunity for EPOC studies over catalysts with multiple phases for the RWGS reaction. ZnO is a commonly used support for Cu in methanol synthesis via CO 2 hydrogenation. , It was reported that ZnO played an important role in preventing sintering of Cu and removing catalyst poisons in Cu/ZnO . The Cu/ZnO interfaces were also confirmed to be crucial in facilitating the CO 2 conversion process, where the initial step should primarily be the H 2 -free CO 2 dissociation .…”