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Hemin has attracted considerable interest as an efficient catalyst recently, however, its direct application is inefficient due to severe molecular aggregation. Immobilizing hemin on various supports is a feasible approach to address this issue. In this work, a CNTs-hemin catalyst was prepared by loading hemin onto multiwalled carbon nanotubes (CNTs) through ball milling. Compared with hemin, CNTs-hemin demonstrates remarkably enhanced performance in the peroxymonosulfate system, with a 650-fold improvement of apparent rate constant, reaching 97.8% degradation of sulfathiazole in 5 min. High-valent iron-oxo porphyrin cation ((Porp)+•FeIV=O) radicals are proposed as the dominant reactive species in the CNTs-hemin/peroxymonosulfate system instead of sulfate radicals (SO4•-), hydroxyl radicals (•OH), superoxide radicals (O2•-) and singlet oxygen (1O2). More in-depth mechanisms reveal that the strong electron transfer between CNTs and hemin promotes the generation of (Porp)+•FeIV=O radicals through a heterolysis pathway. This research enriches the understanding of the catalytic mechanism of supported biomimetic catalysts for PMS activation and provides a perspective on the role of support materials for catalytic activity. Copyright © 2022 Elsevier B.V. All rights reserved.

Citation

Sijing Chen, Zhen Li, Longsheng Wu, Lu Liu, Jingping Hu, Huijie Hou, Sha Liang, Jiakuan Yang. Generation of high-valent iron-oxo porphyrin cation radicals on hemin loaded carbon nanotubes for efficient degradation of sulfathiazole. Journal of hazardous materials. 2023 Feb 15;444(Pt A):130402

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PMID: 36403452

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