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Research Article | Open Access

Controllable photooxidation of 1-phenylethanol integrated with hydrogen evolution by a polyoxometalate/ZnIn2S4/WO3 catalytic system

Jiaxin Yang1,2, Yongkang Liu2, Yun Qin2, Zhenheng Diao1 ( ), Yuanyuan Dong2 ( ), Hongjin Lv2 ( )
School of Chemical Engineering, Advanced Institute of Materials Science, Changchun University of Technology, Changchun 130012, China
MOE Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectric/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 102488, China
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Graphical Abstract

An efficient photocatalytic valorization of 1-phenylethanol coupling with hydrogen evolution was achieved by a polyoxometalate/ZnIn2S4/WO3 catalytic system, where the product distribution can be effectively controlled by the addition of [Ni4(H2O)2(PW9O34)2]10− (Ni4P2) polyoxometalate catalyst.

Abstract

The photocatalytic oxidation of 1-phenylethanol coupling with hydrogen evolution represents a promising strategy for the full utilization of the photogenerated electrons and holes to accomplish the maximum conversion of solar energy into chemical energy. To date, however, the controllable of reaction path and product distribution has yet not to be unrevealed. Herein, we report an efficient coupled catalytic system composed of ZnIn2S4/WO3 S-scheme heterojunction and Ni-containing polyoxometalate ([Ni4(H2O)2(PW9O34)2]10− (Ni4P2)), which exhibited excellent photocatalytic activities towards the oxidation valorization of 1-phenylethanol coupling with hydrogen evolution. The addition of Ni4P2 can efficiently control the product distribution. Specifically, 1-phenylethanol was preferentially converted to pinacol (86.0% selectivity) via C–C coupling over ZnIn2S4/WO3 S-scheme heterojunction accompanied by hydrogen production (202.4 μmol), whereas it would be converted to acetophenone (93.8% selectivity) by photogenerated holes with concomitant hydrogen formation (183.1 μmol) over the coupled Ni4P2/ZnIn2S4/WO3 catalytic system. Mechanism studies revealed that the hydrogen evolution cocatalyst Ni4P2, with its excellent electron storage capacity, can compete with the oxidation product acetophenone for electrons, and thus its addition can significantly inhibit the reduction of acetophenone, resulting in the inability to generate the coupling product pinacol.

Keywords

S-scheme heterojunctionZnIn2S4polyoxometalatesdehydrocouplinghydrogen evolutionphotocatalysis

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Nano Research
Volume 18 Issue 4,
April 2025
Article number: 94907303
DOI: 10.26599/NR.2025.94907303
Cite this article:
Yang J, Liu Y, Qin Y, et al. Controllable photooxidation of 1-phenylethanol integrated with hydrogen evolution by a polyoxometalate/ZnIn2S4/WO3 catalytic system. Nano Research, 2025, 18(4): 94907303. https://doi.org/10.26599/NR.2025.94907303
Topics:
Photocatalysis

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Received: 05 January 2025
Revised: 11 February 2025
Accepted: 12 February 2025
Published: 27 March 2025
© The Author(s) 2025. Published by Tsinghua University Press.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, https://creativecommons.org/licenses/by/4.0/).
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