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Nearly 100% selective and visible-light-driven methane conversion to formaldehyde via. single-atom Cu and Wδ+

Author

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  • Lei Luo

    (Northwest University
    Chinese Academy of Sciences)

  • Xiaoyu Han

    (The University of Manchester)

  • Keran Wang

    (Northwest University)

  • Youxun Xu

    (University College London)

  • Lunqiao Xiong

    (University College London)

  • Jiani Ma

    (Northwest University)

  • Zhengxiao Guo

    (The University of Hong Kong)

  • Junwang Tang

    (University College London)

Abstract

Direct solar-driven methane (CH4) reforming is highly desirable but challenging, particularly to achieve a value-added product with high selectivity. Here, we identify a synergistic ensemble effect of atomically dispersed copper (Cu) species and partially reduced tungsten (Wδ+), stabilised over an oxygen-vacancy-rich WO3, which enables exceptional photocatalytic CH4 conversion to formaldehyde (HCHO) under visible light, leading to nearly 100% selectivity, a very high yield of 4979.0 μmol·g−1 within 2 h, and the normalised mass activity of 8.5 × 106 μmol·g-1Cu·h−1 of HCHO at ambient temperature. In-situ EPR and XPS analyses indicate that the Cu species serve as the electron acceptor, promoting the photo-induced electron transfer from the conduction band to O2, generating reactive •OOH radicals. In parallel, the adjacent Wδ+ species act as the hole acceptor and the preferred adsorption and activation site of H2O to produce hydroxyl radicals (•OH), and thus activate CH4 to methyl radicals (•CH3). The synergy of the adjacent dual active sites boosts the overall efficiency and selectivity of the conversion process.

Suggested Citation

  • Lei Luo & Xiaoyu Han & Keran Wang & Youxun Xu & Lunqiao Xiong & Jiani Ma & Zhengxiao Guo & Junwang Tang, 2023. "Nearly 100% selective and visible-light-driven methane conversion to formaldehyde via. single-atom Cu and Wδ+," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-38334-7
    DOI: 10.1038/s41467-023-38334-7
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    References listed on IDEAS

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    1. Chengyang Feng & Shouwei Zuo & Miao Hu & Yuanfu Ren & Liwei Xia & Jun Luo & Chen Zou & Sibo Wang & Yihan Zhu & Magnus Rueping & Yu Han & Huabin Zhang, 2024. "Optimizing the reaction pathway of methane photo-oxidation over single copper sites," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Yingying Fan & Yuheng Jiang & Haiting Lin & Jianan Li & Yuanjiang Xie & Anyi Chen & Siyang Li & Dongxue Han & Li Niu & Zhiyong Tang, 2024. "Insight into selectivity of photocatalytic methane oxidation to formaldehyde on tungsten trioxide," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    3. Youxun Xu & Chao Wang & Xiyi Li & Lunqiao Xiong & Tianyu Zhang & Liquan Zhang & Qinghua Zhang & Lin Gu & Yang Lan & Junwang Tang, 2024. "Efficient methane oxidation to formaldehyde via photon–phonon cascade catalysis," Nature Sustainability, Nature, vol. 7(9), pages 1171-1181, September.

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