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MOFs-derived porous carbon embedded Fe0 nanoparticles as peroxymonosulfate activator for efficient degradation of organic pollutants

Journal 2025 · IF 7.7 · 发表于 2025 年 1 月 8 日
作者: Jia-Qi Zhou,Huan-Yan Xu,Bo Li,Bao-Ying Wang,Yue Liu,Zhi-hao Zhao,Yan-Li Zhuang
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摘要

Achieving the harmless degradation of organic pollutants remains a challenging task for the advanced oxidation processes. Metal-organic frameworks have emerged in the field of energy and environmental catalysis. Herein, MIL-101(Fe) was employed as the precursor to prepare a porous carbon embedded Fe 0 nanoparticles (Fe 0 @C) via a pyrolytic process under N 2 protection. MIL-101(Fe) and Fe 0 @C were characterized in detail by various instrumental techniques. The control experiments indicated that Fe 0 @C exhibited much higher capacity to activate peroxymonosulfate (PMS) for the degradation of Levofloxacin (LEV) than MIL-101(Fe). Within 60 min reaction time, LEV degradation efficiency was increased from 37.0% in the MIL-101(Fe)/PMS system to 96.3% in the Fe 0 @C/PMS one. The affecting parameters of Fe 0 @C/PMS system were investigated systematically, including LEV concentration, Fe 0 @C dosage, PMS dosage, solution pH and coexisting anions. Furthermore, various representative organic pollutants could be efficiently degraded in the Fe 0 @C/PMS system. Radical quenching tests and electron paramagnetic resonance (EPR) disclosed that singlet oxygen ( 1 O 2 ), sulfate radical (SO 4 •- ) and hydroxyl radical (•OH) governed the degradation of LEV, among which 1 O 2 played the most prominent role. Meanwhile, the degradation intermediates and pathways of LEV under the radical and non-radical attacks were deduced by high-performance liquid chromatography-quadrupole-time of flight mass spectrometry (HPLC-QTOF/MS) assisted by density functional theory (DFT) calculations. The reasonably designed Fe 0 @C might facilitate electron transfer and thus promote Fe(III)/Fe(II) cycle and PMS activation. This work will provide a new idea for the development of MOFs-derived carbon-based persulfate activators.

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