Long-range interactions driving neighboring Fe–N4 sites in Fenton-like reactions for sustainable water decontamination
Zelin Wu,
Zhaokun Xiong,
Bingkun Huang,
Gang Yao,
Sihui Zhan () and
Bo Lai ()
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Zelin Wu: Sichuan University
Zhaokun Xiong: Sichuan University
Bingkun Huang: Sichuan University
Gang Yao: Sichuan University
Sihui Zhan: Nankai University
Bo Lai: Sichuan University
Nature Communications, 2024, vol. 15, issue 1, 1-12
Abstract:
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.
Date: 2024
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-52074-2
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DOI: 10.1038/s41467-024-52074-2
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