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Insights into excitonic behavior in single-atom covalent organic frameworks for efficient photo-Fenton-like pollutant degradation

Author

Listed:
  • Chao Zhu

    (Zhejiang University of Technology)

  • Mingzheng Yang

    (Zhejiang University of Technology)

  • Bo Jiang

    (Zhejiang University of Technology)

  • Lun Lu

    (South China Institute of Environmental Sciences)

  • Qile Fang

    (Beijing Normal University at Zhuhai)

  • Yong Zheng

    (China Three Gorges University)

  • Shuang Song

    (Zhejiang University of Technology)

  • Baoliang Chen

    (Zhejiang University)

  • Yi Shen

    (Zhejiang University of Technology
    Zhejing University of Technology)

Abstract

The generation of radicals through photo-Fenton-like reactions demonstrates significant potential for remediating emerging organic contaminants (EOCs) in complex aqueous environments. However, the excitonic effect, induced by Coulomb interactions between photoexcited electrons and holes, reduces carrier utilization efficiency in these systems. In this study, we develop Cu single-atom-loaded covalent organic frameworks (CuSA/COFs) as models to modulate excitonic effects. Temperature-dependent photoluminescence and ultrafast transient absorption spectra reveal that incorporating acenaphthene units into the linker (CuSA/Ace-COF) significantly reduces exciton binding energy (Eb). This modification not only enhances peroxymonosulfate adsorption at Cu active sites but also facilitates rapid electron transfer and promotes selective hydroxyl radical generation. Compared to CuSA/Obq-COF (Eb = 25.6 meV), CuSA/Ace-COF (Eb = 12.2 meV) shows a 39.5-fold increase in the pseudo-first-order rate constant for sulfamethoxazole degradation (0.434 min−1). This work provides insights into modulating excitonic behavior in single-atom catalysts via linker engineering for EOCs degradation.

Suggested Citation

  • Chao Zhu & Mingzheng Yang & Bo Jiang & Lun Lu & Qile Fang & Yong Zheng & Shuang Song & Baoliang Chen & Yi Shen, 2025. "Insights into excitonic behavior in single-atom covalent organic frameworks for efficient photo-Fenton-like pollutant degradation," Nature Communications, Nature, vol. 16(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-56103-6
    DOI: 10.1038/s41467-025-56103-6
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    References listed on IDEAS

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    1. Xiao Chen & Shuaiqiang Jia & Jianxin Zhai & Jiapeng Jiao & Mengke Dong & Cheng Xue & Ting Deng & Hailian Cheng & Zhanghui Xia & Chunjun Chen & Xueqing Xing & Jianrong Zeng & Haihong Wu & Mingyuan He &, 2024. "Multivalent Cu sites synergistically adjust carbonaceous intermediates adsorption for electrocatalytic ethanol production," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    2. Haoyin Zhong & Qi Zhang & Junchen Yu & Xin Zhang & Chao Wu & Hang An & Yifan Ma & Hao Wang & Jun Zhang & Yong-Wei Zhang & Caozheng Diao & Zhi Gen Yu & Shibo Xi & Xiaopeng Wang & Junmin Xue, 2023. "Key role of eg* band broadening in nickel-based oxyhydroxides on coupled oxygen evolution mechanism," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
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