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Nano Research 2024, 17(5): 3810-3818 https://doi.org/10.1007/s12274-023-6323-5
Research Article | Issue | Published: 13 December 2023

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

Show Author's Information 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
Keywords:
nanomaterial, photocatalysis, oxygen activation, methane oxidation, radical regulation
Topics:
Photocatalysis
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
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Abstract Full text Electronic supplementary material About this article

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.


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Electronic supplementary material
About this article

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

Show Author's information 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

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: nanomaterial, photocatalysis, oxygen activation, methane oxidation, radical regulation

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Publication history
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Acknowledgements

Publication history

Received: 24 September 2023
Revised: 27 October 2023
Accepted: 07 November 2023
Published: 13 December 2023
Issue date: May 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Key Research and Development Program of China (No. 2019YFA0708700), the National Natural Science Foundation of China (Nos. 22322815, 22179146, 51672309, 51172285, and 51372277), the Major Scientific and Technological Innovation Project of Shandong Province (No. 2020CXGC010402), the Fundamental Research Funds for Central Universities (No. 18CX07009A), YanKuang Group Co., Ltd. (No. YKZB2020-167), the Young Taishan Scholar Program of Shandong Province (No. tsqn20182027), Taishan Scholar Project (No. ts201712020), and the Technological Leading Scholar of 10000 Talent Project (No. W03020508).

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