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首页> 外文期刊>Environmental Science & Technology >Chlorate Formation Mechanism in the Presence of Sulfate Radical, Chloride, Bromide and Natural Organic Matter
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Chlorate Formation Mechanism in the Presence of Sulfate Radical, Chloride, Bromide and Natural Organic Matter

机译：硫酸根，氯离子，溴离子和天然有机物存在下氯酸盐的形成机理

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摘要

Halides and natural organic matter (NOM) are inevitable in aquatic environment and influence the degradation of contaminants in sulfate radical (SO_(4)~(•–))-based advanced oxidation processes. This study investigated the formation of chlorate in the coexposure of SO_(4)~(•–), chloride (Cl~(–)), bromide (Br~(–)) and/or NOM in UV/persulfate (UV/PDS) and cobalt(II)/peroxymonosulfate (Co/PMS) systems. The formation of chlorate increased with increasing Cl~(–) concentration in the UV/PDS system, however, in the Co/PMS system, it initially increased and then decreased. The chlorate formation involved the formation of hypochlorous acid/hypochlorite (HOCl/OCl~(–)) as an intermediate in both systems. The formation was primarily attributable to SO_(4)~(•–) in the UV/PDS system, whereas Co(III) played a significant role in the oxidation of Cl~(–) to HOCl/OCl~(–) and SO_(4)~(•–) was important for the oxidation of HOCl/OCl~(–) to chlorate in the Co/PMS system. The pseudo-first-order rate constants (k′ ) of the transformation from Cl~(–) to HOCl/OCl~(–) were 3.32 × 10~(–6) s~(–1) and 9.23 × 10~(–3) s~(–1) in UV/PDS and Co/PMS, respectively. Meanwhile, k′ of HOCl/OCl~(–) to chlorate in UV/PDS and Co/PMS were 2.43 × 10~(–3) s~(–1) and 2.70 × 10~(–4) s~(–1), respectively. Br~(–) completely inhibited the chlorate formation in UV/PDS, but inhibited it by 45.2% in Co/PMS. The k′ of SO_(4)~(•–) reacting with Br~(–) to form hypobromous acid/hypobromite (HOBr/OBr~(–)) was calculated to be 378 times higher than that of Cl~(–) to HOCl/OCl~(–), but the k′ of Co(III) reacting with Br~(–) to form HOBr/OBr~(–) was comparable to that of Cl~(–) to HOCl/OCl~(–). NOM also significantly inhibited the chlorate formation, due to the consumption of SO_(4)~(•–) and reactive chlorine species (RCS, such as Cl· , ClO· and HOCl/OCl~(–)). This study demonstrated the formation of chlorate in SO_(4)~(•–)-based AOPs, which should to be considered in their application in water treatment.
机译：卤化物和天然有机物（NOM）在水生环境中不可避免，并会影响基于硫酸根（SO_（4）〜（•–））的高级氧化过程中污染物的降解。本研究调查了紫外线/过硫酸盐（UV / PDS）中SO_（4）〜（•–），氯化物（Cl〜（–）），溴化物（Br〜（–））和/或NOM共同暴露下氯酸盐的形成。 ）和钴（II）/过一硫酸氢盐（Co / PMS）系统。在UV / PDS系统中，氯离子的形成随Cl〜（–）浓度的增加而增加，但是在Co / PMS系统中，氯离子的形成先增加后减少。氯酸盐的形成涉及次氯酸/次氯酸盐（HOCl / OCl〜（–））在两个系统中的形成。在UV / PDS系统中，形成主要归因于SO_（4）〜（•–），而Co（III）在将Cl〜（–）氧化为HOCl / OCl〜（–）和SO_中起重要作用。 （4）〜（•–）对于在Co / PMS系统中将HOCl / OCl〜（–）氧化为氯酸盐非常重要。从Cl〜（–）转换为HOCl / OCl〜（–）的伪一阶速率常数（ k'）为3.32×10〜（–6）s〜（–1）和9.23×在UV / PDS和Co / PMS中分别为10〜（–3）s〜（-1）。同时，UV / PDS和Co / PMS中HOCl / OCl〜（–）氯化物的 k'分别为2.43×10〜（–3）s〜（–1）和2.70×10〜（–4）s 〜（–1）分别。 Br〜（–）完全抑制了UV / PDS中氯酸盐的生成，但在Co / PMS中抑制了45.2％。计算得出SO_（4）〜（•–）与Br〜（–）反应形成次溴酸/次溴酸盐（HOBr / OBr〜（–））的 k'比Cl〜高378倍。 （–）变成HOCl / OCl〜（–），但Co（III）的 k'与Br〜（–）反应形成HOBr / OBr〜（–）与Cl〜（–）相当到HOCl / OCl〜（–）。由于消耗了SO_（4）〜（•–）和活性氯（RCS，例如Cl ·，ClO ·和HOCl / OCl〜（–），NOM也显着抑制了氯酸盐的形成。 ）。这项研究表明，在基于SO_（4）〜（•–）的AOP中会形成氯酸盐，在将其用于水处理时应予以考虑。

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  • 来源
    《Environmental Science & Technology》 |2018年第11期|6317-6325|共9页
  • 作者

    Shaodong Hou; Li Ling; Dionysios D. Dionysiou; Yuru Wang; Jiajia Huang; Kaiheng Guo; Xuchun Li; Jingyun Fang;

  • 作者单位

    Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275, China;

    Department of Civil and Environmental Engineering, the Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China;

    Environmental Engineering and Science Program, Department of Chemical and Environmental Engineering (DCEE), University of Cincinnati, Cincinnati, Ohio 45221, United States;

    Department of Environmental Science, School of Geography and Tourism, Shanxi Normal University, Xi’an 710119, China;

    Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275, China;

    Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275, China;

    School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, China;

    Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275, China;

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