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Production of Hydroxyl Radical via the Activation of Hydrogen Peroxide by Hydroxylamine

机译:通过羟胺活化过氧化氢生产羟自由基

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摘要

The production of the hydroxyl radical (HO·) is important in environmental chemistry. This study reports a new source of HO· generated solely from hydrogen peroxide (H_2O_2) activated by hydroxylamine (HA). Electron paramagnetic resonance analysis and the oxidation of a HO' probe, benzoic add, were used to confirm the production of HO·. The production of HO· increased with increasing concentrations of either HA or H_2O_2 as well as decreasing pH. The second-order rate constant for the reaction was (2.2 ± 0.2) × 10~(-4) M~(-1) s~(-1). HO· was probably produced in two steps: the activation of H_2O_2 by protonated HA and then reaction between the H_2O_2 and the intermediate protonated aminoxyl radical generated in the first step. Such a two-step oxidation can possibly be ascribed to the ionizable hydroxyl moiety in the molecular structure of HA, as is suggested by comparing the reactivity of a series of HA derivatives in HO· production. The results shed light on a previously unknown source of HO· formation, which broadens the understanding of its role in environmental processes.
机译:羟基自由基(HO·)的产生在环境化学中很重要。这项研究报告了仅由羟胺(HA)活化的过氧化氢(H_2O_2)产生的HO·的新来源。电子顺磁共振分析和HO'探针(苯甲酸)的氧化被用来确认HO·的产生。随着HA或H_2O_2浓度的增加以及pH值的降低,HO·的产量增加。反应的二级速率常数为(2.2±0.2)×10〜(-4)M〜(-1)s〜(-1)。 HO·可能是通过两个步骤产生的:通过质子化的HA活化H_2O_2,然后在第一步中生成的H_2O_2与中间质子化的氨氧基自由基反应。这种两步氧化可能归因于HA分子结构中的可电离羟基部分,如通过比较一系列HA衍生物在HO·生产中的反应性所暗示的。研究结果揭示了以前未知的HO·形成来源,从而拓宽了其在环境过程中作用的认识。

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  • 来源
    《Environmental Science & Technology》 |2015年第17期|10373-10379|共7页
  • 作者单位

    College of Biology and the Environment, Nanjing Forestry University, Nanjing 210037, China;

    College of Architecture and Environment, Sichuan University, Chengdu 610065, China;

    School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou 510275, China;

    State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin 150090, China;

    College of Biology and the Environment, Nanjing Forestry University, Nanjing 210037, China;

    College of Biology and the Environment, Nanjing Forestry University, Nanjing 210037, China;

    School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, 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);
  • 原文格式 PDF
  • 正文语种 eng
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