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Overlooked self-catalytic mechanism in phenolic moiety-mediated Fenton-like system: Formation of Fe(III) hydroperoxide complex and co-treatment of refractory pollutants

文献类型: 外文期刊

作者: Chen, Cheng 1 ; Wang, Yongyi 1 ; Huang, Yajing 1 ; Hua, Jian 2 ; Qu, Wei 1 ; Xia, Dehua 1 ; He, Chun 1 ; Sharma, Virender K. 3 ; Shu, Dong 4 ;

作者机构: 1.Sun Yat Sen Univ, Sch Environm Sci & Engn, Guangdong Prov Key Lab Environm Pollut Control & R, Guangzhou 510275, Peoples R China

2.Guangdong Inst Ecoenvironm & Soil Sci, Guangdong Key Lab Agr Environm Pollut Integrated C, Guangzhou 510640, Peoples R China

3.Texas A&M Univ, Sch Publ Hlth, Dept Occupat & Environm Hlth, College Stn, TX 77843 USA

4.South China Normal Univ, Guangdong Univ, Sch Chem, Key Lab Technol Electrochem Energy Storage & Power, Guangzhou 510006, Peoples R China

关键词: Self-catalysis; Fe(III); Fe(II) redox cycling; Fe(III) hydroperoxide complex; Fenton-like reaction; Phenolic pollutants

期刊名称:APPLIED CATALYSIS B-ENVIRONMENTAL ( 影响因子:22.1; 五年影响因子:19.7 )

ISSN: 0926-3373

年卷期: 2023 年 321 卷

页码:

收录情况: SCI

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 selfcatalytic 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 yellowcolored 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 selfcatalytic Fenton-like process for remediating a mixture of pollutants.

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