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Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol

Author

Listed:
  • Hailong Zhang

    (Xiamen University
    Sichuan University)

  • Peijie Han

    (Xiamen University)

  • Danfeng Wu

    (Xiamen University)

  • Congcong Du

    (Xiamen University)

  • Jiafei Zhao

    (Xiamen University)

  • Kelvin H. L. Zhang

    (Xiamen University)

  • Jingdong Lin

    (Xiamen University)

  • Shaolong Wan

    (Xiamen University)

  • Jianyu Huang

    (Yanshan University)

  • Shuai Wang

    (Xiamen University)

  • Haifeng Xiong

    (Xiamen University)

  • Yong Wang

    (Washington State University)

Abstract

The direct oxidation of methane to methanol (MTM) remains a significant challenge in heterogeneous catalysis due to the high dissociation energy of the C-H bond in methane and the high desorption energy of methanol. In this work, we demonstrate a breakthrough in selective MTM by achieving a high methanol space-time yield of 2678 mmol molCu−1 h−1 with 93% selectivity in a continuous methane-steam reaction at 400 °C. The superior performance is attributed to the confinement effect of 6-membered ring (6MR) voids in SSZ-13 zeolite, which host isolated Cu-OH single sites. Our results provide a deeper understanding of the role of Cu-zeolites in continuous methane-steam to methanol conversion and pave the way for further improvement.

Suggested Citation

  • Hailong Zhang & Peijie Han & Danfeng Wu & Congcong Du & Jiafei Zhao & Kelvin H. L. Zhang & Jingdong Lin & Shaolong Wan & Jianyu Huang & Shuai Wang & Haifeng Xiong & Yong Wang, 2023. "Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-43508-4
    DOI: 10.1038/s41467-023-43508-4
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    References listed on IDEAS

    as
    1. Raquel L. Lieberman & Amy C. Rosenzweig, 2005. "Crystal structure of a membrane-bound metalloenzyme that catalyses the biological oxidation of methane," Nature, Nature, vol. 434(7030), pages 177-182, March.
    2. Sebastian Grundner & Monica A.C. Markovits & Guanna Li & Moniek Tromp & Evgeny A. Pidko & Emiel J.M. Hensen & Andreas Jentys & Maricruz Sanchez-Sanchez & Johannes A. Lercher, 2015. "Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol," Nature Communications, Nature, vol. 6(1), pages 1-9, November.
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