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Research Article

Selective photocatalytic oxidation of methane to C1 oxygenates by regulating sizes and facets over Au/ZnO

Qiang Zhou1, Xinyu Wang1, Xiaojie Tan1, Qinhua Zhang1, Hao Yang1, Tao Xing2, Mingqing Wang2, Mingbo Wu1( ), Wenting Wu1( )
State Key Laboratory of Heavy Oil Processing, College of Chemistry and Chemical Engineering & Institute of New Energy, China University of Petroleum (East China), Qingdao 266580, China
National Engineering Research Center of Coal Gasification and Coal-Based Advanced Materials, ShanDong Energy Group CO. LTD, Jinan 250101, China
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Graphical Abstract

We propose a strategy for the selective generation of reactive oxygen species (·OOH and ·OH) by regulating the sizes and facets of Au nanoparticles loaded on ZnO in the photocatalytic CH4 oxidation. 1.0% Au/ZnO-9.6 with the medium size and Au (111) facet showed a strong ·OOH formation through mild oxygen reduction, which contributed to the production of oxygenates.

Abstract

Photocatalytic oxidation of methane to value-added chemicals is a promising process under mild conditions, nevertheless confronting great challenges in efficiently activating C–H bonds and inhibiting over-oxidation. Herein, we propose a comprehensive strategy for the selective generation of reactive oxygen species (ROS) by regulating the sizes and facets of Au nanoparticles loaded on ZnO. For photocatalytic methane oxidation at ambient temperature, a high oxygenates yield of 36.4 mmol·g−1·h−1 with a nearly 100% selectivity has been achieved over the optimized 1.0% Au/ZnO-9.6 (1% Au with (111) facet and 9.6 nm size on ZnO) photocatalyst, exceeding most reported literatures. Mechanism investigations reveal that 1.0% Au/ZnO-9.6 with the medium size and Au (111) facet guarantees the favourable formation of superoxide radicals (·OOH) through mild oxygen reduction, ultimately leading to excellent photocatalytic methane oxidation performance. This work provides some guidance for the delicate design of photocatalysts for efficient photocatalytic methane oxidation and oxygen utilization.

Keywords

photocatalysismethane oxidationradical regulationoxygen activationnanomaterial

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Nano Research
Volume 17 Issue 5,
May 2024
Pages 3810-3818
DOI: 10.1007/s12274-023-6323-5
Cite this article:
Zhou Q, Wang X, Tan X, et al. Selective photocatalytic oxidation of methane to C1 oxygenates by regulating sizes and facets over Au/ZnO. Nano Research, 2024, 17(5): 3810-3818. https://doi.org/10.1007/s12274-023-6323-5
Topics:
Photocatalysis

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Received: 24 September 2023
Revised: 27 October 2023
Accepted: 07 November 2023
Published: 13 December 2023
© Tsinghua University Press 2023
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