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Long-range interactions driving neighboring Fe–N4 sites in Fenton-like reactions for sustainable water decontamination

Author

Listed:
  • Zelin Wu

    (Sichuan University
    Sichuan University)

  • Zhaokun Xiong

    (Sichuan University
    Sichuan University)

  • Bingkun Huang

    (Sichuan University
    Sichuan University)

  • Gang Yao

    (Sichuan University
    Sino-German Centre for innovative Environmental Technologies (WATCH e.V.))

  • Sihui Zhan

    (Nankai University)

  • Bo Lai

    (Sichuan University
    Sichuan University)

Abstract

Actualizing efficient and sustainable environmental catalysis is essential in global water pollution control. The single-atom Fenton-like process, as a promising technique, suffers from reducing potential environmental impacts of single-atom catalysts (SACs) synthesis and modulating functionalized species beyond the first coordination shell. Herein, we devised a high-performance SAC possessing impressive Fenton-like reactivity and extended stability by constructing abundant intrinsic topological defects within carbon planes anchored with Fe−N4 sites. Coupling atomic Fe−N4 moieties and adjacent intrinsic defects provides potent synergistic interaction. Density functional theory calculations reveal that the intrinsic defects optimize the d-band electronic structure of neighboring Fe centers through long-range interactions, consequently boosting the intrinsic activity of Fe−N4 sites. Life cycle assessment and long-term steady operation at the device level indicate promising industrial-scale treatment capability for actual wastewater. This work emphasizes the feasibility of synergistic defect engineering for refining single-atom Fenton-like chemistry and inspires rational materials design toward sustainable environmental remediation.

Suggested Citation

  • Zelin Wu & Zhaokun Xiong & Bingkun Huang & Gang Yao & Sihui Zhan & Bo Lai, 2024. "Long-range interactions driving neighboring Fe–N4 sites in Fenton-like reactions for sustainable water decontamination," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-52074-2
    DOI: 10.1038/s41467-024-52074-2
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    References listed on IDEAS

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    1. Tongcai Liu & Shaoze Xiao & Nan Li & Jiabin Chen & Xuefei Zhou & Yajie Qian & Ching-Hua Huang & Yalei Zhang, 2023. "Water decontamination via nonradical process by nanoconfined Fenton-like catalysts," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Shengjie Wei & Yibing Sun & Yun-Ze Qiu & Ang Li & Ching-Yu Chiang & Hai Xiao & Jieshu Qian & Yadong Li, 2023. "Self-carbon-thermal-reduction strategy for boosting the Fenton-like activity of single Fe-N4 sites by carbon-defect engineering," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    3. Fengbo Yu & Chao Jia & Xuan Wu & Liming Sun & Zhijian Shi & Tao Teng & Litao Lin & Zhelin He & Jie Gao & Shicheng Zhang & Liang Wang & Shaobin Wang & Xiangdong Zhu, 2023. "Rapid self-heating synthesis of Fe-based nanomaterial catalyst for advanced oxidation," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
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