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首页> 外文期刊>Environmental Science & Technology >Elucidating the Elementary Reaction Pathways and Kinetics of Hydroxyl Radical-Induced Acetone Degradation in Aqueous Phase Advanced Oxidation Processes
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Elucidating the Elementary Reaction Pathways and Kinetics of Hydroxyl Radical-Induced Acetone Degradation in Aqueous Phase Advanced Oxidation Processes

机译：阐明水相高级氧化过程中羟基自由基诱导的丙酮降解的基本反应途径和动力学

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摘要

Advanced oxidation processes (AOPs) that produce highly reactive hydroxyl radicals are promising methods to destroy aqueous organic contaminants. Hydroxyl radicals react rapidly and nonselectively with organic contaminants and degrade them into intermediates and transformation byproducts. Past studies have indicated that peroxyl radical reactions are responsible for the formation of many intermediate radicals and transformation byproducts. However, complex peroxyl radical reactions that produce identical transformation products make it difficult to experimentally study the elementary reaction pathways and kinetics. In this study, we used ab initio quantum mechanical calculations to identify the thermodynamically preferable elementary reaction pathways of hydroxyl radical-induced acetone degradation by calculating the free energies of the reaction and predicting the corresponding reaction rate constants by calculating the free energies of activation. In addition, we solved the ordinary differential equations for each species participating in the elementary reactions to predict the concentration profiles for acetone and its transformation byproducts in an aqueous phase UV/hydrogen peroxide AOP. Our ab initio quantum mechanical calculations found an insignificant contribution of Russell reaction mechanisms of peroxyl radicals, but significant involvement of HO2 center dot in the peroxyl radical reactions. The predicted concentration profiles were compared with experiments in the literature, validating our elementary reaction-based kinetic model.
机译：产生高反应性羟基自由基的高级氧化工艺（AOP）是消除水性有机污染物的有前途的方法。羟自由基与有机污染物快速且非选择性地反应，并将其降解为中间体和转化副产物。过去的研究表明，过氧自由基反应是许多中间自由基形成和转化副产物的原因。然而，产生相同转化产物的复杂的过氧自由基反应使得难以通过实验研究基本的反应途径和动力学。在这项研究中，我们使用从头算量子力学计算，通过计算反应的自由能并通过计算活化的自由能来预测相应的反应速率常数，从而确定了羟基自由基诱导的丙酮降解的热力学上优选的基本反应途径。此外，我们求解了参与基本反应的每个物种的常微分方程，以预测水相UV /过氧化氢AOP中丙酮及其转化副产物的浓度曲线。我们的从头开始的量子力学计算发现过氧自由基的Russell反应机理的贡献不大，但是HO2中心点明显参与了过氧自由基的反应。将预测的浓度曲线与文献中的实验进行比较，验证了我们基于基本反应的动力学模型。

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  • 来源
    《Environmental Science & Technology》 |2018年第14期|7763-7774|共12页
  • 作者

    Kamath Divya; Mezyk Stephen P.; Minakate Daisuke;

  • 作者单位

    Michigan Technol Univ, Dept Civil & Environm Engn, Houghton, MI 49931 USA;

    Calif State Univ Long Beach, Dept Chem & Biochem, Long Beach, CA 90840 USA;

    Michigan Technol Univ, Dept Civil & Environm Engn, Houghton, MI 49931 USA;

  • 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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