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PEG-stabilized coaxial stacking of two-dimensional covalent organic frameworks for enhanced photocatalytic hydrogen evolution

Author

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  • Ting Zhou

    (Fudan University)

  • Lei Wang

    (University of Science and Technology of China)

  • Xingye Huang

    (Fudan University)

  • Junjuda Unruangsri

    (Chulalongkorn University)

  • Hualei Zhang

    (Fudan University)

  • Rong Wang

    (Fudan University)

  • Qingliang Song

    (Fudan University)

  • Qingyuan Yang

    (Beijing University of Chemical Technology)

  • Weihua Li

    (Fudan University)

  • Changchun Wang

    (Fudan University)

  • Kaito Takahashi

    (Institute of Atomic and Molecular Sciences Academia Sinica)

  • Hangxun Xu

    (University of Science and Technology of China)

  • Jia Guo

    (Fudan University)

Abstract

Two-dimensional covalent organic frameworks (2D COFs) featuring periodic frameworks, extended π-conjugation and layered stacking structures, have emerged as a promising class of materials for photocatalytic hydrogen evolution. Nevertheless, the layer-by-layer assembly in 2D COFs is not stable during the photocatalytic cycling in water, causing disordered stacking and declined activity. Here, we report an innovative strategy to stabilize the ordered arrangement of layered structures in 2D COFs for hydrogen evolution. Polyethylene glycol is filled up in the mesopore channels of a β-ketoenamine-linked COF containing benzothiadiazole moiety. This unique feature suppresses the dislocation of neighbouring layers and retains the columnar π-orbital arrays to facilitate free charge transport. The hydrogen evolution rate is therefore remarkably promoted under visible irradiation compared with that of the pristine COF. This study provides a general post-functionalization strategy for 2D COFs to enhance photocatalytic performances.

Suggested Citation

  • Ting Zhou & Lei Wang & Xingye Huang & Junjuda Unruangsri & Hualei Zhang & Rong Wang & Qingliang Song & Qingyuan Yang & Weihua Li & Changchun Wang & Kaito Takahashi & Hangxun Xu & Jia Guo, 2021. "PEG-stabilized coaxial stacking of two-dimensional covalent organic frameworks for enhanced photocatalytic hydrogen evolution," Nature Communications, Nature, vol. 12(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-24179-5
    DOI: 10.1038/s41467-021-24179-5
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    Cited by:

    1. Lei Zhang & Qiu-Hong Zhu & Yue-Ru Zhou & Shuang-Long Wang & Jie Fu & Jia-Ying Liu & Guo-Hao Zhang & Lijian Ma & Guohua Tao & Guo-Hong Tao & Ling He, 2023. "Hydrogen-bonding and π-π interaction promoted solution-processable covalent organic frameworks," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Minghao Liu & Shuai Yang & Xiubei Yang & Cheng-Xing Cui & Guojuan Liu & Xuewen Li & Jun He & George Zheng Chen & Qing Xu & Gaofeng Zeng, 2023. "Post-synthetic modification of covalent organic frameworks for CO2 electroreduction," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    3. Weijun Weng & Jia Guo, 2022. "The effect of enantioselective chiral covalent organic frameworks and cysteine sacrificial donors on photocatalytic hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-11, December.

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