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Activation of Peroxymonosulfate by FeVO3-x for the Degradation of Carbamazepine: Vanadium Mediated Electron Shuttle and Oxygen Vacancy Modulated Interface Chemistry

CHINESE CHEMICAL LETTERS(2024)

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Abstract
Fast Fe(III)/Fe(II) circulation in heterogeneous peroxymonosulfate (PMS) activation remains as a bottle-neck issue that restricts the development of PMS based advanced oxidation processes. Herein, we pro-posed a facile ammonia reduction strategy and synthesized a novel FeVO3-x catalysts to activate PMS for the degradation of a typical pharmaceutical, carbamazepine (CBZ). Rapid CBZ removal could be achieved within 10 min, which outperforms most of the other iron or vanadium-based catalysts. Electron para-magnetic resonance analysis and chemical probe experiments revealed SO4 center dot -, center dot OH, O2 center dot - and high valent iron (Fe(IV)) were all generated in this system, but SO4 center dot - and Fe(IV) primarily contributed to the degrada-tion of CBZ. Besides, X-ray photoelectron spectroscopy and X-ray adsorption spectroscopy indicated that both the generated low-valent V provides and oxygen vacancy acted as superior electron donors and ac-celerated internal electron transfer via the unsaturated V -O -Fe bond. Finally, the proposed system also exhibited satisfactory performance in practical applications. This work provides a promising platform in heterogeneous PMS activation. (c) 2023 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
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Key words
Peroxymonosulfate,Fe(III)/Fe(II) cycle,Electron shuttles,Oxygen vacancy,Bimetallic catalysts
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