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首页> 外文期刊>Environmental Science & Technology >Homo-Conjugation of Low Molecular Weight Organic Acids Competes with Their Complexation with Cu(Ⅱ)
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Homo-Conjugation of Low Molecular Weight Organic Acids Competes with Their Complexation with Cu(Ⅱ)

机译：低分子量有机酸与铜（Ⅱ）的络合竞争

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摘要

Dissolved organic matter (DOM) controls the bioavailability and toxicity of heavy metals in aquatic environments. The observation of decreased conditional binding constants with increasing DOM concentration is not well documented, which may result in significant uncertainties in heavy metal behavior modeling and risk assessment. We used eight low molecular weight organic acids (LMOC) with representative structures to simulate DOM molecules. The interactions between LMOC molecules resulted in the decreased Cu(II)-LMOC binding with increasing LMOC concentrations, but higher pH values than theoretical calculation after mixing LMOC solutions of different pHs. We thus proposed homoconjugation between LMOC molecules through negative charge-assisted H-bond ((−)CAHB). A mathematic model was developed to describe Cu(II)–LMOC complexation (K _(C)) and LMOC homoconjugation (K _(LHL)). The increased competition of LMOC homoconjugation over Cu(II)–LMOC complexation, as suggested by the increased ratios of K _(LHL)/K _(C), resulted in the apparently decreased Cu(II)–LMOC binding with the increased LMOC concentration. Similar concentration-dependent binding was also observed for DOM. With the identified homoconjugation between DOM molecules, some of the literature data with concentration-dependent behavior may be re-evaluated. This is the first work that quantitatively identified homoconjugation among organic molecules. Both the modeling concepts and results provide useful information in investigating the environmental roles of DOM in mediating metal bioavailability and transport.
机译：溶解有机物（DOM）控制着水环境中重金属的生物利用度和毒性。随着DOM浓度增加而观察到的条件结合常数降低的证据尚未充分记录，这可能导致重金属行为建模和风险评估存在重大不确定性。我们使用具有代表性结构的八种低分子量有机酸（LMOC）来模拟DOM分子。 LMOC分子之间的相互作用导致随着LMOC浓度的增加，Cu（II）-LMOC结合力降低，但与不同pH值的LMOC溶液混合后的理论计算相比，pH值更高。因此，我们提出了通过负电荷辅助的H键（（-）CAHB）在LMOC分子之间的均共轭。建立了描述Cu（II）–LMOC络合（ K _（C））和LMOC均共轭（ K _（LHL））的数学模型。如（i）K _（LHL）/ K _（C）的比率增加所表明的，LMOC的共轭竞争与Cu（II）–LMOC络合的竞争增加，导致Cu（II）–明显减少。 LMOC与增加的LMOC浓度结合。对于DOM也观察到类似的浓度依赖性结合。通过确定DOM分子之间的均共轭作用，可以重新评估一些具有浓度依赖性行为的文献数据。这是定量鉴定有机分子之间的共轭作用的第一项工作。建模概念和结果都为研究DOM在介导金属生物利用度和运输中的环境作用提供了有用的信息。

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  • 来源
    《Environmental Science & Technology》 |2018年第9期|5173-5181|共9页
  • 作者

    Jing Zhao; Gang Chu; Bo Pan; Yuwei Zhou; Min Wu; Yang Liu; Wenyan Duan; Di Lang; Qing Zhao; Baoshan Xing;

  • 作者单位

    Faculty of Environmental Science & Engineering, Kunming University of Science & Technology, Kunming, Yunnan 650500, China,Stockbridge School of Agriculture, University of Massachusetts, Amherst, Massachusetts 01003, United States;

    Faculty of Environmental Science & Engineering, Kunming University of Science & Technology, Kunming, Yunnan 650500, China;

    Faculty of Environmental Science & Engineering, Kunming University of Science & Technology, Kunming, Yunnan 650500, China;

    Faculty of Environmental Science & Engineering, Kunming University of Science & Technology, Kunming, Yunnan 650500, China;

    Faculty of Environmental Science & Engineering, Kunming University of Science & Technology, Kunming, Yunnan 650500, China;

    Faculty of Environmental Science & Engineering, Kunming University of Science & Technology, Kunming, Yunnan 650500, China;

    Faculty of Environmental Science & Engineering, Kunming University of Science & Technology, Kunming, Yunnan 650500, China;

    Faculty of Environmental Science & Engineering, Kunming University of Science & Technology, Kunming, Yunnan 650500, China;

    Institute of Applied Ecology, Chinese Academy of Sciences, Shenyang 110016, China;

    Stockbridge School of Agriculture, University of Massachusetts, Amherst, Massachusetts 01003, 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);
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