Low-Voltage Electrooxidation of Benzyl Alcohol to Benzoic Acid Enhanced by PtZn-ZnOx Interface

化学 苯甲醇 苯甲酸 接口(物质) 无机化学 有机化学 分子 催化作用 吉布斯等温线
作者
Renfeng Liu,Wenjing Tu,An Pei,Wei‐Hsiang Huang,Yanyan Jia,Peng Wang,Daoru Liu,Qiqi Wu,Qizhen Qin,Weiwei Zhou,Linan Zhou,Keyou Yan,Yun Zhao,Guangxu Chen
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:147 (12): 10339-10348 被引量:26
标识
DOI:10.1021/jacs.4c17193
摘要

The electrocatalytic oxidation of benzyl alcohol to benzoic acid is a process that often requires high voltage, leading to increased energy consumption, side reactions (oxygen evolution reaction (OER)), and catalyst degradation. Herein, our study introduces a novel approach. We demonstrate that a PtZn-ZnOx catalyst featuring a PtZn intermetallic structure with abundant PtZn-ZnOx interfaces on the surface allows for the electrocatalytic oxidation of benzyl alcohol to benzoic acid with an impressive selectivity of 99.5% at a low potential of 0.725 V (vs a reversible hydrogen electrode, RHE), which is 0.6 V lower than most reported studies. This high selectivity is a testament to the efficiency of our catalyst, as it significantly reduces the occurrence of side reactions, leading to a more efficient and sustainable process. The experimental and density functional theory calculations demonstrated that the adsorption of Ph–CH2OH and Ph–CHO and the generation of electrophilic OH* were promoted due to the unsaturated coordination of the Zn atom in the PtZn-ZnOx interfaces. Furthermore, the potential-determining step of coupling OH* with Ph–CHO was promoted due to the low energy barrier at the PtZn-ZnOx interface, leading to improved catalytic activity and selectivity. This study outlines a novel approach to designing highly efficient electrocatalysts for high-efficiency alcohol valorization at low voltages.
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