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Coupling photocatalytic CO2 reduction and CH3OH oxidation for selective dimethoxymethane production

Author

Listed:
  • Yixuan Wang

    (Sungkyunkwan University
    Sungkyunkwan University
    Sungkyunkwan University)

  • Yang Liu

    (Sungkyunkwan University
    Sungkyunkwan University)

  • Lingling Wang

    (Sungkyunkwan University
    Sungkyunkwan University)

  • Silambarasan Perumal

    (Sungkyunkwan University
    Sungkyunkwan University
    Sungkyunkwan University)

  • Hongdan Wang

    (Sungkyunkwan University
    Sungkyunkwan University)

  • Hyun Ko

    (Sungkyunkwan University)

  • Chung-Li Dong

    (Tamkang University)

  • Panpan Zhang

    (Jiangsu University)

  • Shuaijun Wang

    (Jiangsu University)

  • Ta Thi Thuy Nga

    (Tamkang University)

  • Young Dok Kim

    (Sungkyunkwan University)

  • Yujing Ji

    (Sungkyunkwan University)

  • Shufang Zhao

    (Sungkyunkwan University)

  • Ji-Hee Kim

    (Sungkyunkwan University)

  • Dong-Yub Yee

    (Sungkyunkwan University)

  • Yosep Hwang

    (Sungkyunkwan University
    Sungkyunkwan University)

  • Jinqiang Zhang

    (The University of Adelaide)

  • Min Gyu Kim

    (Pohang University of Science and Technology)

  • Hyoyoung Lee

    (Sungkyunkwan University
    Sungkyunkwan University
    Sungkyunkwan University
    Sungkyunkwan University)

Abstract

Currently, conventional dimethoxymethane synthesis methods are environmentally unfriendly. Here, we report a photo-redox catalysis system to generate dimethoxymethane using a silver and tungsten co-modified blue titanium dioxide catalyst (Ag.W-BTO) by coupling CO2 reduction and CH3OH oxidation under mild conditions. The Ag.W-BTO structure and its electron and hole transfer are comprehensively investigated by combining advanced characterizations and theoretical studies. Strikingly, Ag.W-BTO achieve a record photocatalytic activity of 5702.49 µmol g−1 with 92.08% dimethoxymethane selectivity in 9 h of ultraviolet-visible irradiation without sacrificial agents. Systematic isotope labeling experiments, in-situ diffuse reflectance infrared Fourier-transform analysis, and theoretical calculations reveal that the Ag and W species respectively catalyze CO2 conversion to *CH2O and CH3OH oxidation to *CH3O. Subsequently, an asymmetric carbon-oxygen coupling process between these two crucial intermediates produces dimethoxymethane. This work presents a CO2 photocatalytic reduction system for multi-carbon production to meet the objectives of sustainable economic development and carbon neutrality.

Suggested Citation

  • Yixuan Wang & Yang Liu & Lingling Wang & Silambarasan Perumal & Hongdan Wang & Hyun Ko & Chung-Li Dong & Panpan Zhang & Shuaijun Wang & Ta Thi Thuy Nga & Young Dok Kim & Yujing Ji & Shufang Zhao & Ji-, 2024. "Coupling photocatalytic CO2 reduction and CH3OH oxidation for selective dimethoxymethane production," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-49927-1
    DOI: 10.1038/s41467-024-49927-1
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    References listed on IDEAS

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    1. Xiaodong Li & Yongfu Sun & Jiaqi Xu & Yanjie Shao & Ju Wu & Xiaoliang Xu & Yang Pan & Huanxin Ju & Junfa Zhu & Yi Xie, 2019. "Selective visible-light-driven photocatalytic CO2 reduction to CH4 mediated by atomically thin CuIn5S8 layers," Nature Energy, Nature, vol. 4(8), pages 690-699, August.
    2. Jie Zhou & Jie Li & Liang Kan & Lei Zhang & Qing Huang & Yong Yan & Yifa Chen & Jiang Liu & Shun-Li Li & Ya-Qian Lan, 2022. "Linking oxidative and reductive clusters to prepare crystalline porous catalysts for photocatalytic CO2 reduction with H2O," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    3. Laura Collado & Anna Reynal & Fernando Fresno & Mariam Barawi & Carlos Escudero & Virginia Perez-Dieste & Juan M. Coronado & David P. Serrano & James R. Durrant & Víctor A. Peña O’Shea, 2018. "Unravelling the effect of charge dynamics at the plasmonic metal/semiconductor interface for CO2 photoreduction," Nature Communications, Nature, vol. 9(1), pages 1-10, December.
    4. Yannan Liu & Cheng-Hao Liu & Tushar Debnath & Yong Wang & Darius Pohl & Lucas V. Besteiro & Debora Motta Meira & Shengyun Huang & Fan Yang & Bernd Rellinghaus & Mohamed Chaker & Dmytro F. Perepichka &, 2023. "Silver nanoparticle enhanced metal-organic matrix with interface-engineering for efficient photocatalytic hydrogen evolution," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
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