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

• DOI: 10.1038/s41467-024-54225-x
• Publication Date: 2024-11-19T19:29:12Z
• Authors: Yuanfang Lin; Ying Wang; Zongling Weng; Yang Zhou; Siqi Liu; Xinwen Ou; Xing Xu; Yanpeng Cai; Jin Jiang; Bin Han; Zhifeng Yang
• Keywords: Science; Q; 01 natural sciences; Article; 0104 chemical sciences

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