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Selective light-driven methane oxidation to ethanol

Author

Listed:
  • Fei Xue

    (Chinese Academy of Sciences (CAS)
    Xiamen University)

  • Chunyang Zhang

    (Xi’an Jiaotong University)

  • Cheng Cheng

    (Xi’an Jiaotong University)

  • Xueli Yan

    (Xi’an Jiaotong University)

  • Feng Liu

    (Xi’an Jiaotong University)

  • Xiaozhi Liu

    (Chinese Academy of Sciences)

  • Biao Jiang

    (Xi’an Jiaotong University)

  • Qiuyue Zhang

    (Xiamen University)

  • Lin Sun

    (Xiamen University)

  • Huiping Peng

    (Xiamen University)

  • Wei-Hsiang Huang

    (National Synchrotron Radiation Research Center)

  • Chih-Wen Pao

    (National Synchrotron Radiation Research Center)

  • Zhiwei Hu

    (Max Planck Institute for Chemical Physics of Solids)

  • Mingshu Chen

    (Xiamen University)

  • Dong Su

    (Chinese Academy of Sciences)

  • Maochang Liu

    (Xi’an Jiaotong University)

  • Xiaoqing Huang

    (Xiamen University
    Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM))

  • Yong Xu

    (Chinese Academy of Sciences (CAS))

Abstract

Methane (CH4) photocatalytic upgrading to value-added chemicals, especially C2 products, is significant yet challenging due to sluggish energy/mass transfer and insufficient chemical driven-force in single photochemical process. Herein, we realize solar-driven CH4 oxidation to ethanol (C2H5OH) on crystalline carbon nitride (CCN) modified with Cu9S5 and Cu single atoms (Cu9S5/Cu-CCN). The integration of photothermal effect and photocatalysis overcomes CH4-to-C2H5OH conversion bottlenecks, with Cu9S5 as a hotspot to convert solar-energy to heat. In-situ characterizations demonstrate that Cu single atoms play as electron acceptor for O2 reduction to ·OOH/ · OH, while Cu9S5 acts as hole acceptor and site for CH4 adsorption, C − H activation, and C − C coupling. Theoretical calculations demonstrate that Cu9S5/Cu-CCN reduces C − C coupling energy barrier by stabilizing ·CH3 and ·CH2O. Impressively, C2H5OH productivity reaches 549.7 μmol g–1 h–1, with selectivity of 94.8% and apparent quantum efficiency of 0.9% (420 nm). This work provides a sustainable avenue for CH4 conversion to value-added chemcials.

Suggested Citation

  • Fei Xue & Chunyang Zhang & Cheng Cheng & Xueli Yan & Feng Liu & Xiaozhi Liu & Biao Jiang & Qiuyue Zhang & Lin Sun & Huiping Peng & Wei-Hsiang Huang & Chih-Wen Pao & Zhiwei Hu & Mingshu Chen & Dong Su , 2024. "Selective light-driven methane oxidation to ethanol," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-54835-5
    DOI: 10.1038/s41467-024-54835-5
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    References listed on IDEAS

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