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.
Authors
- Renfeng Liu
- Guangxu Chen (ORCID: https://orcid.org/0000-0002-8670-4708)
- Yanyan Jia (ORCID: https://orcid.org/0000-0002-2994-3956)
- Yun Zhao (ORCID: https://orcid.org/0000-0001-6237-5295)
- Weiwei Zhou (ORCID: https://orcid.org/0000-0003-1641-8965)
- Wenjing Tu
- Keyou Yan (ORCID: https://orcid.org/0000-0003-4380-7325)
- An Pei (ORCID: https://orcid.org/0000-0002-5000-6414)
- Qiqi Wu (ORCID: https://orcid.org/0000-0002-7034-3864)
- Wei‐Hsiang Huang (ORCID: https://orcid.org/0000-0001-9503-0373)
- Linan Zhou (ORCID: https://orcid.org/0000-0002-2989-1535)
- Daoru Liu (ORCID: https://orcid.org/0000-0002-4175-2570)
- Qizhen Qin
- Peng Wang (ORCID: https://orcid.org/0009-0004-0113-8623)
Institutions
- 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)
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