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首页> 外文期刊>Environmental Science & Technology >The Fenton Reaction in Water Assisted by Picolinic Acid: Accelerated Iron Cycling and Co-generation of a Selective Fe-Based Oxidant
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The Fenton Reaction in Water Assisted by Picolinic Acid: Accelerated Iron Cycling and Co-generation of a Selective Fe-Based Oxidant

机译：菲龙反应在水中辅助乌氟沙酸：加速铁循环和共同产生选择性Fe基氧化剂

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摘要

The Fenton reaction is limited by a narrow acidic pH range, the slow reduction of Fe(Ⅲ), and susceptibility of the nonselective hydroxyl radical (HO~•) to scavenging by water constituents. Here, we employed the biodegradable chelating agent picolinic acid (PICA) to address these concerns. Compared to the classical Fenton reaction at pH 3.0, PICA greatly accelerated the degradation of atrazine, sulfamethazine, and various substituted phenols at pH 5.0 in a reaction with autocatalytic characteristics. Although HO~• served as the principal oxidant, a high-spin, end-on hydroperoxo intermediate, tentatively identified as PICA-Fe~Ⅲ-OOH, also exhibited reactivity toward several test compounds. Chloride release from the oxidation of 2,4,6-trichlorophenol and the positive slope of the Hammett correlation for a series of halogenated phenols were consistent with PICA-Fe~Ⅲ-OOH reacting as a nucleophilic oxidant. Compared to HO~•, PICA-Fe~Ⅲ-OOH is less sensitive to potential scavengers in environmental water samples.Kinetic analysis reveals that PICA facilitates Fe(Ⅲ)/Fe(Ⅱ) transformation by accelerating Fe(Ⅲ) reduction by H_2O_2. Autocatalysis is ascribed to the buildup of Fe(Ⅱ) from the reduction of Fe(Ⅲ) by H_2O_2 as well as PICA oxidation products. PICA assistance in the Fenton reaction may be beneficial to wastewater treatment because it favors iron cycling, extends the pH range, and balances oxidation universality with selectivity.
机译：芬顿反应受窄酸性pH范围的限制，Fe（Ⅲ）的缓慢降低，并通过水成分清除无选择性羟基（HO〜•）的易感性。在这里，我们使用可生物降解的螯合剂吡啶酸（PICA）来解决这些问题。与pH 3.0的典型芬顿反应相比，PICA大大加速了阿特拉嗪，磺胺甲嘧啶和在与自催化特征的反应中的亚唑嗪和各种取代酚的降解。虽然HO〜•用作主要氧化剂，暂时鉴定为PICA-Fe〜Ⅲ-OOH的高旋转，结束氢过氧化氢中间体，也表现出对几种测试化合物的反应性。从2,4,6-三氯化苯酚的氧化释放的氯化物释放和Hammett与一系列卤代酚的正斜率与作为亲核氧化剂的PICA-Fe〜Ⅲ-OOH一致。与HO〜•，PICA-FE〜Ⅲ-OOH对环境水样中的潜在清除剂不太敏感.PICET分析显示，PICA通过加速通过H_2O_2减少FO（Ⅲ）的FE（Ⅲ）/ Fe（Ⅱ）转化。通过H_2O_2和PICA氧化产物的Fe（Ⅲ）的减少和PICA氧化产物归因于Fe（Ⅱ）的累积。在芬顿反应中的PICA援助可能有利于废水处理，因为它有利于铁循环，延长pH范围，并通过选择性余额融合氧化普遍性。

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  • 来源
    《Environmental Science & Technology》 |2021年第12期|8299-8308|共10页
  • 作者

    Zhichao Yang; Chao Shan; Bingcai Pan; Joseph J. Pignatello;

  • 作者单位

    State Key Laboratory of Pollution Control and Resource Reuse School of Environment Nanjing University Nanjing 210023 PR China Department of Environmental Sciences The Connecticut Agricultural Experiment Station New Haven Connecticut 06511 United States;

    State Key Laboratory of Pollution Control and Resource Reuse School of Environment Nanjing University Nanjing 210023 PR China Research Center for Environmental Nanotechnology (ReCENT) Nanjing University Nanjing 210023 PR China;

    State Key Laboratory of Pollution Control and Resource Reuse School of Environment Nanjing University Nanjing 210023 PR China Research Center for Environmental Nanotechnology (ReCENT) Nanjing University Nanjing 210023 PR China;

    Department of Environmental Sciences The Connecticut Agricultural Experiment Station New Haven Connecticut 06511 United States;

  • 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);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    picolinic acid; Fenton; PICA-Fe~Ⅲ-OOH; hydroxyl radical; iron cycling; autocatalysis;

    机译：鸟苷酸;芬顿;PICA-FE〜Ⅲ-OOH;羟基自由基;铁循环;自催化分析;

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