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Ground-state charge transfer in single-molecule junctions covalent organic frameworks for boosting photocatalytic hydrogen evolution

Author

Listed:
  • Rongchen Shen

    (South China Agricultural University
    South China Agricultural University
    Shaoguan University)

  • Can Huang

    (South China Agricultural University
    South China Agricultural University)

  • Lei Hao

    (South China Agricultural University
    South China Agricultural University)

  • Guijie Liang

    (Hubei University of Arts and Science)

  • Peng Zhang

    (Zhengzhou University)

  • Qiang Yue

    (Shaoguan University)

  • Xin Li

    (South China Agricultural University
    South China Agricultural University
    Zhengzhou University)

Abstract

Ground-state charge transfer plays a vital role in improving the photocatalytic performance of D-A type covalent organic frameworks. However, limited studies have explored the modulation of photocatalytic performance in COFs-based photocatalysts through ground-state charge transfer. Here we show the formation of extremely intense ground-state charge transfer via a unique covalent bonding approach. We transform three-dimensional stacked COF-based S-scheme heterojunctions (FOOCOF-PDIU) into co-planar single-molecule junctions (FOOCOF-PDI). This co-planar single-molecule junction structure exhibits strong ground-state charge transfer compared to the traditional randomly stacked heterojunctions and individual COFs. Ground-state charge transfer induces charge redistribution and dipole moment formation, which enhances the built-in electric field intensity in single-molecule junctions. This enhanced built-in electric field promotes exciton dissociation and charge separation, resulting in improved photocatalytic efficiency. Therefore, a stable molecule-decorated COF with broad light absorption has been successfully obtained, whose hydrogen evolution rate can reach 265 mmol g−1 h−1. This work opens an avenue for exploiting photocatalytic mechanisms in COFs based on ground-state charge transfer effects.

Suggested Citation

  • Rongchen Shen & Can Huang & Lei Hao & Guijie Liang & Peng Zhang & Qiang Yue & Xin Li, 2025. "Ground-state charge transfer in single-molecule junctions covalent organic frameworks for boosting photocatalytic hydrogen evolution," Nature Communications, Nature, vol. 16(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-57662-4
    DOI: 10.1038/s41467-025-57662-4
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    References listed on IDEAS

    as
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