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首页> 外文期刊>Environmental Science & Technology >Thallium(Ⅰ) Oxidation by Permanganate and Chlorine: Kinetics and Manganese Dioxide Catalysis
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Thallium(Ⅰ) Oxidation by Permanganate and Chlorine: Kinetics and Manganese Dioxide Catalysis

机译：铊（Ⅰ）氧化高锰酸盐和氯：动力学和二氧化锰催化

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摘要

The oxidation of the toxic heavy metal thallium(Ⅰ) (Tl(Ⅰ)) is an efficient way to enhance Tl removal from water and wastewater. However, few studies have focused on the kinetics of Tl(Ⅰ) oxidation in water, especially at environmentally relevant pH values. Therefore, the kinetics and mechanisms of Tl(Ⅰ) oxidation by the common agents KMnO_4 and HOCl under environmentally relevant pH condition were explored in the present study. The results indicated that the pH-dependent oxidation of Tl(Ⅰ) by KMnO_4 exhibited second-order kinetics under alkaline conditions (pH 8-10) with the main active species being TlOH, while the reaction could be characterized by autocatalysis at pH 4-6, and Mn(Ⅲ) might also play an essential role in the MnO_2 catalysis. Furthermore, a two-electron transfer mechanism under alkaline conditions was preliminarily proposed by using linear free energy relationships and X-ray photoelectron spectroscopy (XPS) analysis. Distinctively, the reaction rate of Tl(Ⅰ) oxidation by HOCl decreased with increasing pH, and protonated chlorine might be the main active species. Moreover, the Tl(Ⅰ)-HOCl reaction could be regarded as first order with respect to Tl(Ⅰ), but the order with respect to HOCl was variable. Significant catalysis by MnO_2 could also be observed in the oxidation of Tl(Ⅰ) by HOCl, mainly due to the vacancies on MnO_2 as active sites for sorbing Tl. This study elucidates the oxidation characteristics of thallium and establishes a theoretical foundation for the oxidation processes in thallium removal.
机译：毒性重金属铊的氧化（Ⅰ）（TL（Ⅰ））是增强水和废水中的TL去除TL的有效方法。然而，很少有研究集中在水中T1（Ⅰ）氧化的动力学，特别是在环境相关的pH值。因此，在本研究中探讨了普通剂普遍代理KIMNO_4和HOCL的TL（Ⅰ）氧化的动力学和机制。结果表明，KMnO_4的T1（Ⅰ）的pH依赖性氧化在碱性条件下表现出二阶动力学，其中主要活性物质是TlOH的，而反应可以通过在pH4-的高常分分析表征6，和Mn（Ⅲ）也可能在MNO_2催化中起重要作用。此外，通过使用线性自由能量关系和X射线光电子体光谱（XPS）分析，预先提出碱性条件下的两电子转移机制。显着地，Hocl的T1（Ⅰ）氧化的反应速率随着pH的增加而降低，质子化氯可能是主要活性物质。此外，T1（Ⅰ）-HoCl反应可以被视为相对于T1（Ⅰ）的第一阶，但相对于HOCl的顺序是可变的。 MNO_2的显着催化也可以在Hocl氧化T1（Ⅰ）中，主要是由于MnO_2作为用于吸附T1的活性位点的空位。本研究阐明了铊的氧化特性，为铊去除的氧化过程建立了理论基础。

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  • 来源
    《Environmental Science & Technology》 |2020年第12期|7205-7216|共12页
  • 作者

    Yijie Zou; Haijun Cheng; Hainan Wang; Ruixing Huang; Yanghui Xu; Jin Jiang; Qiang He; Caihong Liu; Juchao Liu; Jiaming Xiong; Jinni Yao; Xiaoliu Huangfu; Jun Ma;

  • 作者单位

    Key Laboratory of Eco-environments in Three Gorges Reservoir Region Ministry of Education College of Environment and Ecology Chongqing University Chongqing 400044 China;

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

    Key Laboratory of Eco-environments in Three Gorges Reservoir Region Ministry of Education College of Environment and Ecology Chongqing University Chongqing 400044 China;

    Key Laboratory of Eco-environments in Three Gorges Reservoir Region Ministry of Education College of Environment and Ecology Chongqing University Chongqing 400044 China;

    Key Laboratory of Eco-environments in Three Gorges Reservoir Region Ministry of Education College of Environment and Ecology Chongqing University Chongqing 400044 China;

    Institute of Environmental and Ecological Engineering Guangdong University of Technology Guangzhou 510006 China;

    Key Laboratory of Eco-environments in Three Gorges Reservoir Region Ministry of Education College of Environment and Ecology Chongqing University Chongqing 400044 China;

    Key Laboratory of Eco-environments in Three Gorges Reservoir Region Ministry of Education College of Environment and Ecology Chongqing University Chongqing 400044 China;

    Key Laboratory of Eco-environments in Three Gorges Reservoir Region Ministry of Education College of Environment and Ecology Chongqing University Chongqing 400044 China;

    Key Laboratory of Eco-environments in Three Gorges Reservoir Region Ministry of Education College of Environment and Ecology Chongqing University Chongqing 400044 China;

    Key Laboratory of Eco-environments in Three Gorges Reservoir Region Ministry of Education College of Environment and Ecology Chongqing University Chongqing 400044 China;

    Key Laboratory of Eco-environments in Three Gorges Reservoir Region Ministry of Education College of Environment and Ecology Chongqing University Chongqing 400044 China;

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