Coordination engineering of heterogeneous high-valent Fe(IV)-oxo for safe removal of pollutants via powerful Fenton-like reactions

Yuanfang Lin, Ying Wang, Zongling Weng, Yang Zhou, Siqi Liu, Xinwen Ou, Xing Xu (), Yanpeng Cai, Jin Jiang, Bin Han () and Zhifeng Yang
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Yuanfang Lin: Guangdong University of Technology
Ying Wang: Pohang University of Science and Technology (POSTECH)
Zongling Weng: Guangdong University of Technology
Yang Zhou: Guangdong University of Technology
Siqi Liu: Dalian University of Technology
Xinwen Ou: Zhejiang University
Yanpeng Cai: Guangdong University of Technology
Jin Jiang: Guangdong University of Technology
Bin Han: Guangdong University of Technology
Zhifeng Yang: Guangdong University of Technology

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Coordination engineering of high-valent Fe(IV)-oxo (FeIV=O) is expected to break the activity-selectivity trade-off of traditional reactive oxygen species, while attempts to regulate the oxidation behaviors of heterogeneous FeIV=O remain unexplored. Here, by coordination engineering of Fe-Nx single-atom catalysts (Fe-Nx SACs), we propose a feasible approach to regulate the oxidation behaviors of heterogeneous FeIV=O. The developed Fe-N2 SACs/peroxymonosulfate (PMS) system delivers boosted performance for FeIV=O generation, and thereby can selectively remove a range of pollutants within tens of seconds. In-situ spectra and theoretical simulations suggest that low-coordination Fe-Nx SACs favor the generation of FeIV=O via PMS activation as providing more electrons to facilitate the desorption of the key *SO4H intermediate. Due to their disparate attacking sites to sulfamethoxazole (SMX) molecules, Fe-N2 SACs mediated FeIV=O (FeIVN2=O) oxidize SMX to small molecules with less toxicity, while FeIVN4=O produces series of more toxic azo compounds through N-N coupling with more complex oxidation pathways.

Date: 2024
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DOI: 10.1038/s41467-024-54225-x

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