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首页> 外文期刊>Environmental Science & Technology >Chlorine Isotope Effects and Composition of Naturally Produced Organochlorines from Chloroperoxidases, Flavin-Dependent Halogenases, and in Forest Soil
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Chlorine Isotope Effects and Composition of Naturally Produced Organochlorines from Chloroperoxidases, Flavin-Dependent Halogenases, and in Forest Soil

机译：从氯过氧化物酶，黄素依赖性卤化酶以及森林土壤中自然产生的有机氯的氯同位素效应和组成

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The use of stable chlorine isotopic signatures (δ~(37)Cl) of organochlorine compounds has been suggested as a tool to determine both their origins and transformations in the environment. Here we investigated the δ~(37)Cl fractionation of two important pathways for enzymatic natural halogenation: chlorination by chloroperoxidase (CPO) and flavin-dependent halogenases (FDH). Phenolic products of CPO were highly ~(37)Cl depleted (5δ~(37)Cl = -12.6 ± 0.9‰); significantly more depleted than all known industrially produced organochlorine compounds (δ~(37)Cl = -7 to +6‰). In contrast, four FDH products did not exhibit any observable isotopic shifts (δ~(37)Cl = -0.3 ± 0.6‰). We attributed the different isotopic effect to the distinctly different chlorination mechanisms employed by the two enzymes. Furthermore, the δ~(37)Cl in bulk organochlorines extracted from boreal forest soils were only slightly depleted in ~(37)Cl relative to inorganic Cl. In contrast to previous suggestions that CPO plays a key role in production of soil organochlorines, this observation points to the additional involvement of either other chlorination pathways, or that dechlorination of naturally produced organochlorines can neutralize δ~(37)Cl shifts caused by CPO chlorination. Overall, this study demonstrates that chlorine isotopic signatures are highly useful to understand sources and cycling of organochlorines in nature. Furthermore, this study presents δ~(37)Cl values of FDH products as well of bulk organochlorines extracted from pristine forest soil for the first time.
机译：有人建议使用有机氯化合物的稳定氯同位素标记（δ〜（37）Cl）作为确定其来源和在环境中转化的工具。在这里，我们研究了酶促自然卤化的两个重要途径的δ〜（37）Cl分馏：氯过氧化物酶（CPO）和黄素依赖性卤化酶（FDH）氯化。 CPO的酚类产物中〜（37）Cl含量极低（5δ〜（37）Cl = -12.6±0.9‰）;比所有已知的工业生产的有机氯化合物（δ〜（37）Cl = -7至+ 6‰）消耗的碳明显多。相反，四种FDH产物没有表现出任何可观察到的同位素位移（δ〜（37）Cl = -0.3±0.6‰）。我们将不同的同位素效应归因于两种酶所采用的明显不同的氯化机理。此外，从北方森林土壤中提取的大量有机氯中的δ〜（37）Cl相对于无机Cl仅略微贫化了〜（37）Cl。与先前关于CPO在土壤有机氯的生产中起关键作用的建议形成鲜明对比的是，该观察结果表明，其他氯化途径也有其他参与，或者天然产生的有机氯的脱氯作用可以中和CPO氯化引起的δ〜（37）Cl转变。 。总的来说，这项研究表明氯同位素特征对于理解自然界中有机氯的来源和循环非常有用。此外，本研究首次提出了从原始森林土壤中提取的FDH产物以及大量有机氯的δ〜（37）Cl值。

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  • 来源
    《Environmental Science & Technology》 |2013年第13期|6864-6871|共8页
  • 作者

    Christoph Aeppli; David Bastviken; Per Andersson; OErjan Gustafsson;

  • 作者单位

    Department of Marine Chemistry and Geochemistry, Woods Hole Oceanographic Institution, Woods Hole, Massachusetts 02S43, United States;

    Department of Thematic Studies, Water and Environmental Studies, Linkoeping University, Sweden;

    Laboratory for Isotope Geology (LIG), Swedish Museum of Natural History, Stockholm, Sweden;

    Department of Applied Environmental Science (ITM), Stockholm University, Sweden,The Bert Bolin Centre for Climate Research, Stockholm University, Sweden;

  • 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);
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