Selective Electrochemical Hydrogenation of Phenol with Earth‐abundant Ni−MoO2 Heterostructured Catalysts: Effect of Oxygen Vacancy on Product Selectivity

Abstract Herein, we report highly efficient carbon supported Ni−MoO 2 heterostructured catalysts for the electrochemical hydrogenation (ECH) of phenol in 0.10 M aqueous sulfuric acid (pH 0.7) at 60 °C. Highest yields for cyclohexanol and cyclohexanone of 95 % and 86 % with faradaic efficiencies of ∼50 % are obtained with catalysts bearing high and low densities of oxygen vacancy (O v ) sites, respectively. In situ diffuse reflectance infrared spectroscopy and density functional theory calculations reveal that the enhanced phenol adsorption strength is responsible for the superior catalytic efficiency. Furthermore, 1‐cyclohexene‐1‐ol is an important intermediate. Its hydrogenation route and hence the final product are affected by the O v density. This work opens a promising avenue to the rational design of advanced electrocatalysts for the upgrading of phenolic compounds.