催化作用
部分
化学
污染物
机制(生物学)
耐火材料(行星科学)
光化学
有机化学
材料科学
冶金
哲学
认识论
作者
Cheng Chen,Yong-Yi Wang,Yajing Huang,Jian Hua,Wenshan Qu,Dehua Xia,Chun He,Virender K. Sharma,Dong Shu
标识
DOI:10.1016/j.apcatb.2022.122062
摘要
Applications of Fenton-like reactions (Fe(III)/H2O2) without catalyst have low efficiency in remediating pollutants. Herein, pollutants containing phenolic moiety (P, e.g., paracetamol (PCM)) were demonstrated to make Fe(III)/H2O2 system highly effective in degrading a wide range of contaminants. Kinetics analysis shows the self-catalytic degradation of PCM with optimum performance at pH 4.0, and Fe(III)/Fe(II) conversion was accelerated without the assistance of cocatalyst. Based on state-of-art spectroscopy measurements and theoretical calculations, the overlooked self-catalytic mechanism was revealed. In the presence of phenolic moiety, a yellow-colored high-spin P-Fe(III)-OOH complex can be formed in Fe(III)/H2O2 system, which subsequently converts to Fe(II). Afterwards, the oxidation of P gives hydroquinone that also facilitates the cycling of Fe(III)/Fe(II). The accumulated Fe(II) reacts with H2O2 to generate hydroxyl radicals, the major species responsible to oxidize pollutants, thereby achieving efficient decontaminant performance. Results provide new insights into the self-catalytic Fenton-like process for remediating a mixture of pollutants.
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