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首页> 外文期刊>Environmental Science & Technology >Formation of Halogenated Polyaromatic Compounds by Laccase Catalyzed Transformation of Halophenols
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Formation of Halogenated Polyaromatic Compounds by Laccase Catalyzed Transformation of Halophenols

机译:漆酶催化卤代酚的转化形成卤化多芳族化合物

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摘要

Laccases are a type of extracellular enzyme produced by fungi, bacteria, and plants. Laccase can catalyze one-electron oxidation of a variety of phenolic compounds using molecular oxygen as the electron acceptor. In this study, transformation of halophenols (XPs) in laccase-catalyzed oxidation processes was explored. We first examined the intrinsic reaction kinetics and found that the transformation of XPs appeared first order to the concentrations of both XPs and laccase. A numerical model was developed to describe the role of humic acid (HA) in this process. It was demonstrated that HA could reverse the oxidation of XPs by acting as the inner filtrator of XP radical intermediates formed upon reactions between the substrates and laccase. The extent of such reversion was proportional to HA concentration. MS analysis in combination with quantum chemistry computation suggested that coupling products were generated. XPs coupled to each via C-C or C-O-C pathways, generating hydroxyl polyhalogenated biphenyl ethers (OH-PCDEs) and hydroxyl polyhalogenated biphenyls, respectively. Many of these polyhalogenated products are known to be hazardous to the ecosystem and human health, but they are not synthetic chemicals. This study shed light on their genesis in the environmental media.
机译:漆酶是真菌,细菌和植物产生的一种细胞外酶。漆酶可以使用分子氧作为电子受体来催化多种酚类化合物的单电子氧化。在这项研究中,探索了漆酶催化氧化过程中卤代酚(XPs)的转化。我们首先检查了内在反应动力学,发现XPs的转化对于XPs和漆酶的浓度都是一级的。建立了一个数值模型来描述腐殖酸(HA)在此过程中的作用。结果表明,HA可以通过充当底物和漆酶之间反应形成的XP自由基中间体的内部过滤剂来逆转XPs的氧化。这种逆转的程度与HA浓度成正比。质谱分析结合量子化学计算表明产生了偶联产物。 XP通过C-C或C-O-C途径相互偶联,分别生成羟基多卤代联苯醚(OH-PCDEs)和羟基多卤代联苯。已知许多这些多卤代产品对生态系统和人类健康有害,但它们不是合成化学品。这项研究揭示了它们在环境媒介中的起源。

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  • 来源
    《Environmental Science & Technology》 |2015年第14期|8550-8557|共8页
  • 作者单位

    College of Resources and Environmental Science, Nanjing Agricultural University, Nanjing 210095, China;

    College of Resources and Environmental Science, Nanjing Agricultural University, Nanjing 210095, China;

    School of Environment, Nanjing University, Nanjing 210093, China;

    School of Environment, Nanjing University, Nanjing 210093, China;

    Department of Crop and Soil Sciences, University of Georgia, Griffin, 30223, 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
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