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

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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.

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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 of10000 Talent Project (No. W03020508).

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Authors and Affiliations

  1. 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

    Qiang Zhou, Xinyu Wang, Xiaojie Tan, Qinhua Zhang, Hao Yang, Mingbo Wu & Wenting Wu

  2. National Engineering Research Center of Coal Gasification and Coal-Based Advanced Materials, ShanDong Energy Group CO. LTD, Jinan, 250101, China

    Tao Xing & Mingqing Wang

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  1. Qiang Zhou
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  2. Xinyu Wang
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  3. Xiaojie Tan
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  4. Qinhua Zhang
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  5. Hao Yang
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  6. Tao Xing
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Correspondence to Mingbo Wu or Wenting Wu.

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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 Res. 17, 3810–3818 (2024). https://doi.org/10.1007/s12274-023-6323-5

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