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Covalent organic frameworks with high quantum efficiency in sacrificial photocatalytic hydrogen evolution

Author

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  • Chunzhi Li

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

  • Jiali Liu

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

  • He Li

    (Chinese Academy of Sciences)

  • Kaifeng Wu

    (Chinese Academy of Sciences)

  • Junhui Wang

    (Chinese Academy of Sciences)

  • Qihua Yang

    (Chinese Academy of Sciences)

Abstract

Organic semiconductors offer a tunable platform for photocatalysis, yet the more difficult exciton dissociation, compared to that in inorganic semiconductors, lowers their photocatalytic activities. In this work, we report that the charge carrier lifetime is dramatically prolonged by incorporating a suitable donor-acceptor (β-ketene-cyano) pair into a covalent organic framework nanosheet. These nanosheets show an apparent quantum efficiency up to 82.6% at 450 nm using platinum as co-catalyst for photocatalytic H2 evolution. Charge carrier kinetic analysis and femtosecond transient absorption spectroscopy characterizations verify that these modified covalent organic framework nanosheets have intrinsically lower exciton binding energies and longer-lived charge carriers than the corresponding nanosheets without the donor-acceptor unit. This work provides a model for gaining insight into the nature of short-lived active species in polymeric organic photocatalysts.

Suggested Citation

  • Chunzhi Li & Jiali Liu & He Li & Kaifeng Wu & Junhui Wang & Qihua Yang, 2022. "Covalent organic frameworks with high quantum efficiency in sacrificial photocatalytic hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30035-x
    DOI: 10.1038/s41467-022-30035-x
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    References listed on IDEAS

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    1. Rengui Li & Fuxiang Zhang & Donge Wang & Jingxiu Yang & Mingrun Li & Jian Zhu & Xin Zhou & Hongxian Han & Can Li, 2013. "Spatial separation of photogenerated electrons and holes among {010} and {110} crystal facets of BiVO4," Nature Communications, Nature, vol. 4(1), pages 1-7, June.
    2. Tsuyoshi Takata & Junzhe Jiang & Yoshihisa Sakata & Mamiko Nakabayashi & Naoya Shibata & Vikas Nandal & Kazuhiko Seki & Takashi Hisatomi & Kazunari Domen, 2020. "Photocatalytic water splitting with a quantum efficiency of almost unity," Nature, Nature, vol. 581(7809), pages 411-414, May.
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    Cited by:

    1. Hongnan Jia & Na Yao & Yiming Jin & Liqing Wu & Juan Zhu & Wei Luo, 2024. "Stabilizing atomic Ru species in conjugated sp2 carbon-linked covalent organic framework for acidic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. Yunyang Qian & Yulan Han & Xiyuan Zhang & Ge Yang & Guozhen Zhang & Hai-Long Jiang, 2023. "Computation-based regulation of excitonic effects in donor-acceptor covalent organic frameworks for enhanced photocatalysis," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    3. Chengxin Zhou & Jian Gao & Yunlong Deng & Ming Wang & Dan Li & Chuan Xia, 2023. "Electric double layer-mediated polarization field for optimizing photogenerated carrier dynamics and thermodynamics," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    4. Ting He & Wenlong Zhen & Yongzhi Chen & Yuanyuan Guo & Zhuoer Li & Ning Huang & Zhongping Li & Ruoyang Liu & Yuan Liu & Xu Lian & Can Xue & Tze Chien Sum & Wei Chen & Donglin Jiang, 2023. "Integrated interfacial design of covalent organic framework photocatalysts to promote hydrogen evolution from water," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    5. Yun Fan & Yu Shen & Jia Zhang & Xinglong Zhang & Zeqi Zhang & Hongfeng Li & Yong Peng & Jiena Weng & Ruijie Xie & Wenlei Zhang & Yu Han & Yawen Xiao & Suoying Zhang & Bing Zheng & Hao-Li Zhang & Sheng, 2024. "Wedging crystals to fabricate crystalline framework nanosheets via mechanochemistry," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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