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

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 s...

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Veröffentlicht in:Nature communications 2024-09, Vol.15 (1), p.7775-12, Article 7775
Hauptverfasser: Wu, Zelin, Xiong, Zhaokun, Huang, Bingkun, Yao, Gang, Zhan, Sihui, Lai, Bo
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Sprache:eng
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Zusammenfassung: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−N 4 sites. Coupling atomic Fe−N 4 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−N 4 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. Non-metallic functionalized species in single-atom catalysts potentially contribute to catalytic performance. Herein, the authors report a long range interaction induced by intrinsic carbon defects to enhance the Fenton-like reactivity and stability of adjacent single-atom sites.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-024-52074-2