化学
苯甲醇
苯甲酸
酒
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
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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