Low-Voltage Electrooxidation of Benzyl Alcohol to Benzoic Acid Enhanced by PtZn-ZnO<sub><i>x</i></sub> Interface

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-ZnO<sub><i>x</i></sub> catalyst featuring a PtZn intermetallic structure with abundant PtZn-ZnO<sub><i>x</i></sub> 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-CH<sub>2</sub>OH and Ph-CHO and the generation of electrophilic OH* were promoted due to the unsaturated coordination of the Zn atom in the PtZn-ZnO<sub><i>x</i></sub> interfaces. Furthermore, the potential-determining step of coupling OH* with Ph-CHO was promoted due to the low energy barrier at the PtZn-ZnO<sub><i>x</i></sub> 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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Publication Details

Journal
Journal of the American Chemical Society
Published
2025-03-12
DOI
https://doi.org/10.1021/jacs.4c17193
Citations
23
Primary Topic
Oxidative Organic Chemistry Reactions
Type
article
Field-Weighted Citation Impact
21.53
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Low-Voltage Electrooxidation of Benzyl Alcohol to Benzoic Acid Enhanced by PtZn-ZnOx Interface

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Journal of the American Chemical Society
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21.53
article

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

Renfeng Liu, Guangxu Chen, Yanyan Jia, Yun Zhao, Weiwei Zhou, Wenjing Tu, Keyou Yan, An Pei, Qiqi Wu, Wei‐Hsiang Huang, Linan Zhou, Daoru Liu, Qizhen Qin, Peng Wang
article en
23 citations

Abstract

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-ZnO<sub><i>x</i></sub> catalyst featuring a PtZn intermetallic structure with abundant PtZn-ZnO<sub><i>x</i></sub> 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-CH<sub>2</sub>OH and Ph-CHO and the generation of electrophilic OH* were promoted due to the unsaturated coordination of the Zn atom in the PtZn-ZnO<sub><i>x</i></sub> interfaces. Furthermore, the potential-determining step of coupling OH* with Ph-CHO was promoted due to the low energy barrier at the PtZn-ZnO<sub><i>x</i></sub> 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.

Journal of the American Chemical SocietyVol. 147(12)
East China University of Science and Technology (CN), National Synchrotron Radiation Research Center (TW), Advanced Materials and Devices (United States) (US), State Key Laboratory of Luminescent Materials and Devices, South China University of Technology (CN)
Openalex Percentile: Top 0%
Oxidative Organic Chemistry Reactions
21.53
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