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首页> 外文期刊>Environmental Science & Technology >Is Sulfate Radical Really Generated from Peroxydisulfate Activated by Iron(Ⅱ) for Environmental Decontamination?
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Is Sulfate Radical Really Generated from Peroxydisulfate Activated by Iron(Ⅱ) for Environmental Decontamination?

机译：铁（Ⅱ）活化过氧二硫酸盐是否真的产生硫酸根，用于环境净化？

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摘要

It is well documented that the traditional Fenton reagent (i.e., the combination of Fe(II) and H2O2) produces hydroxyl radical ((OH)-O-center dot) under acidic conditions, while at near-neutral pH the reactive intermediate converts to ferryl ion (Fe(IV)) that can oxidize sulfoxides to produce corresponding sulfones, markedly differing from their (OH)-O-center dot-induced products. However, it remains unclear whether Fe(IV) is generated in the Fe(II) activated peroxydisulfate (PDS) process, where sulfate radical (SO4 center dot-) is long recognized as the dominant intermediate in literature. Here we demonstrated that SO4 center dot- oxidized methyl phenyl sulfoxide (PMSO, a model sulfoxide) to produce biphenyl compounds rather than methyl phenyl sulfone (PMSO2). Interestingly, the formation of PMSO2 was observed when PMSO was treated by the Fe(II)/PDS system over a wide pH range, and the yields of PMSO2 were quantified to be similar to 100% at acidic pH 3-5. The identification of Fe(IV) in the Fe(II)/PDS system could also reasonably explain the literature results on alcohol scavenging effect and ESR spectra analysis. Further, a Fe(IV)-based kinetic model was shown to accurately simulate the experimental data. This work urges re-evaluation of the Fe(II)/PDS system for environmental decontamination, given that Fe(W) would have different reactivity toward environmental contaminants compared with SO4 center dot- and/or (OH)-O-center dot.
机译：有充分的文献证明，传统的Fenton试剂（即Fe（II）和H2O2的组合）在酸性条件下会产生羟基自由基（（OH）-O-中心点），而在接近中性的pH下，反应性中间体会转化为可以氧化亚砜产生相应的砜的亚铁离子（Fe（IV）），与它们的（OH）-O-中心点诱导产物明显不同。但是，目前尚不清楚是否在Fe（II）活化的过氧二硫酸盐（PDS）工艺中生成了Fe（IV），在该工艺中，硫酸根（SO4中心点-）长期以来被认为是文献中的主要中间体。在这里，我们证明了SO4中心点氧化了甲基苯基亚砜（PMSO，一种模型亚砜），而不是甲基苯基砜（PMSO2）产生了联苯化合物。有趣的是，当用Fe（II）/ PDS系统在较宽的pH范围内处理PMSO时，观察到PMSO2的形成，并且在酸性pH 3-5下，PMSO2的产率被定量为接近100％。 Fe（II）/ PDS系统中Fe（IV）的鉴定也可以合理地解释有关酒精清除作用和ESR光谱分析的文献结果。此外，显示了基于Fe（IV）的动力学模型可以准确地模拟实验数据。鉴于Fe（W）与SO4中心点和/或（OH）-O中心点相比，对环境污染物的反应性不同，因此该工作敦促对用于环境净化的Fe（II）/ PDS系统进行重新评估。

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  • 来源
    《Environmental Science & Technology》 |2018年第19期|11276-11284|共9页
  • 作者

    Wang Zhen; Jiang Jin; Pang Suyan; Zhou Yang; Guan Chaoting; Gao Yuan; Li Juan; Yang Yi; Qu Wei; Jiang Chengchun;

  • 作者单位

    Sch Environm, Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Heilongjiang, Peoples R China;

    Sch Environm, Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Heilongjiang, Peoples R China;

    Jilin Jianzhu Univ, Sch Municipal & Environm Engn, Changchun 130118, Jilin, Peoples R China;

    Sch Environm, Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Heilongjiang, Peoples R China;

    Sch Environm, Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Heilongjiang, Peoples R China;

    Sch Environm, Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Heilongjiang, Peoples R China;

    Sch Environm, Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Heilongjiang, Peoples R China;

    Sch Environm, Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Heilongjiang, Peoples R China;

    Sch Environm, Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Heilongjiang, Peoples R China;

    Shenzhen Polytech, Sch Civil & Environm Engn, Shenzhen 518055, Peoples R China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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