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Selective Electrochemical Hydrogenation of Phenol with Earth-abundant Ni−MoO2 Heterostructured Catalysts: Effect of Oxygen Vacancy on Product Selectivity |
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| Authors: | Peng Zhou Si-Xuan Guo Linbo Li Tadaharu Ueda Yoshinori Nishiwaki Liang Huang Zehui Zhang Jie Zhang |
| Institution: | 1. School of Chemistry, Monash University, Wellington Road, Clayton, 3800 Victoria, Australia;2. Department of Marine Resource Science, Faculty of Agriculture and Marine Science, Kochi University, Nankoku, 783-8502 Japan
Center for Advanced Marine Core Research, Kochi University, Nankoku, 783-8502 Japan;3. Teacher Training Division (Science Education Course), Faculty of Education, Kochi University, Kochi, 780-8520 Japan;4. The State Key Laboratory of Refractories and Metallurgy, Wuhan University of Science and Technology, Wuhan, 430081 China;5. Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education, South-Central Minzu University, Wuhan, 430074 P.R. China |
| Abstract: | Herein, we report highly efficient carbon supported Ni−MoO2 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 (Ov) 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 Ov density. This work opens a promising avenue to the rational design of advanced electrocatalysts for the upgrading of phenolic compounds. |
| Keywords: | Electrochemical Hydrogenation Heterostructured Catalyst Nickel Oxygen Vacancy Phenol |