IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v16y2025i1d10.1038_s41467-024-54061-z.html
   My bibliography  Save this article

MoS2-confined Rh-Zn atomic pair boosts photo-driven methane carbonylation to acetic acid

Author

Listed:
  • Yanan Li

    (Xiamen University
    Chinese Academy of Sciences)

  • Huan Liu

    (Chinese Academy of Sciences)

  • Jun Mao

    (Xiamen University
    Chinese Academy of Sciences)

  • Meng Gao

    (University of Chinese Academy of Sciences)

  • Yunlong Zhang

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Qiao Zhao

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Meng Liu

    (University of Chinese Academy of Sciences
    Chinese Academy of Sciences)

  • Yao Song

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Jingting Hu

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Wangwang Zhang

    (Xiamen University)

  • Rui Huang

    (Chinese Academy of Sciences)

  • Wu Zhou

    (University of Chinese Academy of Sciences)

  • Kaifeng Wu

    (University of Chinese Academy of Sciences
    Chinese Academy of Sciences)

  • Wei Liu

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Liang Yu

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Xiaoju Cui

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Dehui Deng

    (Xiamen University
    Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

Abstract

Direct carbonylation of CH4 to CH3COOH provides a promising pathway for upgrading of natural gas to transportable liquid chemicals, in which high-efficiency CH4 activation and controllable C–C coupling are both critical but challenging. Herein, we report that highly efficient photo-driven carbonylation of CH4 with CO and O2 to CH3COOH is achieved over MoS2-confined Rh-Zn atomic-pair in conjunction with TiO2. It delivers a high CH3COOH productivity of 152.0 μmol gcat.−1 h−1 and turnover frequency of 62.0 h−1 with a superior selectivity of 96.5%, outperforming previous photocatalytic CH4 carbonylation processes. Mechanistic investigations disclose the key effect of Rh-Zn synergy in combination with photo-excited electrons from TiO2 for CH3COOH formation. The active OH species produced from O2 photoreduction on the Zn site through proton-coupled electron transfer promotes CH4 dissociation to CH3 species, which then facilely couples with adsorbed CO on the adjacent Rh site forming the key CH3CO intermediate for CH3COOH formation.

Suggested Citation

  • Yanan Li & Huan Liu & Jun Mao & Meng Gao & Yunlong Zhang & Qiao Zhao & Meng Liu & Yao Song & Jingting Hu & Wangwang Zhang & Rui Huang & Wu Zhou & Kaifeng Wu & Wei Liu & Liang Yu & Xiaoju Cui & Dehui D, 2025. "MoS2-confined Rh-Zn atomic pair boosts photo-driven methane carbonylation to acetic acid," Nature Communications, Nature, vol. 16(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-024-54061-z
    DOI: 10.1038/s41467-024-54061-z
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-54061-z
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-024-54061-z?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-024-54061-z. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    We have no bibliographic references for this item. You can help adding them by using this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.