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Substituent engineering in g-C3N4/COF heterojunctions for rapid charge separation and high photo-redox activity

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Abstract

The heterojunction constructed of covalent organic frameworks (COFs) with adjustable structure and other photocatalysts has great potential in the field of photocatalysis. However, effectively enhancing the photocatalytic performance of organic heterojunctions by designing the structure of COFs has not been explored. Herein, TPB-TP-COFs fabricated from 1,3,5-tris(4-amino-phenyl)benzene (TPB) and terephthalaldehyde (TP) with different substituents (−H, −OH, −OCH3, −Br and −F groups), were applied to construct g-C3N4/COFs. The performance improvement of the heterojunction could be affected by substituents, and only −OCH3 groups can significantly improve both the photocatalytic phenol oxidation and Cr(VI) reduction. DFT calculation demonstrated that the substituents will affect the electron cloud distribution of CBM, and the location of CBM in the TPB segment is beneficial for the charge transport between TPB-TP-OCH3 and g-C3N4. The enhanced charge transfer from g-C3N4 to TPB segment and the improved light absorption of TPB-TP-OCH3 jointly optimize the photocatalytic redox capacity of g-C3N4/TPB-TP-OCH3. On the basis of this study, regulating the electronic effects of semiconductors played a vital role in improving photocatalytic performance in organic heterojunctions.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (21876154) and the Fundamental Research Funds for the Provincial Universities of Zhejiang (JRK22001). Partially support from the Robert A. Welch Foundation (B-0027) (SM) and the Researchers Supporting Program (RSP-2022/55) at King Saud University, Riyadh, Saudi Arabia (AMA) is also acknowledged.

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Author notes

  1. These authors contributed equally to this work.

Authors and Affiliations

  1. School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou, 310018, China

    Jiayun Guo & Qi Wang

  2. Department of Chemistry, College of Chemistry and Materials Engineering, Beijing Technology and Business University, Beijing, 100048, China

    Dongge Ma

  3. Institute of Industrial Catalysis, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310023, China

    Fulin Sun & Guilin Zhuang

  4. Department of Chemistry, College of Science, King Saud University, Riyadh, 11451, Saudi Arabia

    Abdullah M. Al-Enizi & Ayman Nafady

  5. Department of Chemistry, University of North Texas, Denton, TX, 76201, USA

    Shengqian Ma

Authors
  1. Jiayun Guo
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  2. Dongge Ma
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  3. Fulin Sun
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  4. Guilin Zhuang
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  5. Qi Wang
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  6. Abdullah M. Al-Enizi
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  7. Ayman Nafady
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  8. Shengqian Ma
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Corresponding authors

Correspondence to Qi Wang or Shengqian Ma.

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Conflict of interest The authors declare no conflict of interest.

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Supporting information The supporting information is available online at http://chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Guo, J., Ma, D., Sun, F. et al. Substituent engineering in g-C3N4/COF heterojunctions for rapid charge separation and high photo-redox activity. Sci. China Chem. 65, 1704–1709 (2022). https://doi.org/10.1007/s11426-022-1350-1

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  • DOI: https://doi.org/10.1007/s11426-022-1350-1

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