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首页> 外文期刊>Environmental Science & Technology >Activation of Peroxymonosulfate by Benzoquinone: A Novel Nonradical Oxidation Process
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Activation of Peroxymonosulfate by Benzoquinone: A Novel Nonradical Oxidation Process

机译：苯醌激活过氧单硫酸盐：一种新型的非自由基氧化过程。

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摘要

The reactions between peroxymonosulfate (PMS) and quinones were investigated for the first time in this work, where benzoquinone (BQ) was selected as a model quinone. It was demonstrated that BQ could efficiently activate PMS for the degradation of sulfamethoxazole (SMX; a frequently detected antibiotic in the environments), and the degradation rate increased with solution pH from 7 to 10. Interestingly, quenching studies suggested that neither hydroxyl radical (~*OH) nor sulfate radical (SO_4~(·-)) was produced therein. Instead, the generation of singlet oxygen (~1O_2) was proved by using two chemical probes (i.e., 2,2,6,6-tetramethyl-4-piperidinol and 9,10-diphenylanthracene) with the appearance of ~1O_2 indicative products detected by electron paramagnetic resonance spectrometry and liquid chromatography mass spectrometry, respectively. A catalytic mechanism was proposed involving the formation of a dioxirane intermediate between PMS and BQ and the subsequent decomposition of this intermediate into ~1O_2. Accordingly, a kinetic model was developed, and it well described the experimental observation that the pH-dependent decomposition rate of PMS was first-order with respect to BQ. These findings have important implications for the development of novel nonradical oxidation processes based on PMS, because ~1O_2 as a moderately reactive electrophile may suffer less interference from background organic matters compared with nonselective ~·OH and SO_4~(·-).
机译：在这项工作中，首次研究了过氧单硫酸盐（PMS）与醌之间的反应，其中选择了苯醌（BQ）作为模型醌。结果表明BQ可以有效地激活PMS降解磺胺甲恶唑（SMX；在环境中经常检测到的抗生素），并且降解速率随着溶液pH从7升高到10而增加。有趣的是，淬灭研究表明羟基自由基（〜产生* OH）或硫酸根（SO_4〜（·-））。取而代之的是，使用两个化学探针（即2,2,6,6-四甲基-4-哌啶醇和9,10-二苯基蒽）证明了单峰态氧（〜1O_2）的生成，并检测到了〜1O_2指示性产物分别用电子顺磁共振光谱法和液相色谱质谱法测定。提出了一种催化机理，包括在PMS和BQ之间形成二环氧乙烷中间体，然后将该中间体分解为〜1O_2。因此，建立了动力学模型，并很好地描述了实验观察结果，即PMS的pH依赖性分解速率相对于BQ为一阶。这些发现对于基于PMS的新型非自由基氧化方法的开发具有重要意义，因为与非选择性〜·OH和SO_4〜（·-）相比，〜1O_2作为中等反应性亲电试剂受背景有机物的干扰较小。

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  • 来源
    《Environmental Science & Technology》 |2015年第21期|12941-12950|共10页
  • 作者

    Yang Zhou; Jin Jiang; Yuan Gao; Jun Ma; Su-Yan Pang; Juan Li; Xue-Ting Lu; Li-Peng Yuan;

  • 作者单位

    State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China;

    State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China;

    State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China;

    State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China;

    Key Laboratory of Green Chemical Engineering and Technology of College of Heilongjiang Province, College of Chemical and Environmental Engineering, Harbin University of Science and Technology, Harbin, Heilongjiang 150040, China;

    State Key Laboratory of Urban Water Resource and Environment, School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150090, China;

    Key Laboratory of Green Chemical Engineering and Technology of College of Heilongjiang Province, College of Chemical and Environmental Engineering, Harbin University of Science and Technology, Harbin, Heilongjiang 150040, China;

    Key Laboratory of Green Chemical Engineering and Technology of College of Heilongjiang Province, College of Chemical and Environmental Engineering, Harbin University of Science and Technology, Harbin, Heilongjiang 150040, 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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