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The Intrinsic Stability of Metal Ion Complexes with Nanoparticulate Fulvic Acids

机译：金属离子与富马酸纳米颗粒配合物的内在稳定性

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摘要

The electrostatic contributions to metal ion binding by fulvic acids (FAs) are characterized in light of recent theoretical developments on description of the net charge density of soft nanoparticles. Under practical electrolyte concentrations, the radius of the small, highly charged soft nanoparticulate FAs is comparable to the electrostatic screening length and their electric potential profile has a bell shape that extends into the surrounding aqueous medium. Consequently, accumulation of counterions in the extraparticulate zone can be significant. By comparison of experimentally derived Boltzmann partitioning coefficients with those computed on the basis of (i) the structural FA particle charge and (ii) the potential profile for a nanoparticulate FA entity equilibrated with indifferent electrolyte, we identify the thickness of the extraparticulate counter charge accumulation shell in 1-1 and 2-1 electrolytes. The results point to the involvement of counterion condensation phenomena and call into question the approaches for modeling electrostatic contributions to ion binding that are invoked by popular equilibrium speciation codes. Overall, the electrostatic contributions to Cd-aq(2+) and Cu-aq(2+) association with FA are weaker than those previously found for much larger humic acids (HA). The intrinsic chemical binding strength of CdFA is comparable to that of CdHA, whereas CuFA complexes are weaker than CuHA ones.
机译：根据关于软纳米颗粒净电荷密度描述的最新理论进展，表征了富叶酸（FAs）对金属离子结合的静电作用。在实际的电解质浓度下，小的高电荷软纳米颗粒FAs的半径可与静电屏蔽长度相媲美，并且它们的电势曲线呈钟形，延伸到周围的水介质中。因此，抗衡离子在颗粒外区域中的积累可能是显着的。通过将实验得出的玻尔兹曼分配系数与基于（i）结构FA粒子电荷和（ii）用无差别电解质平衡的纳米微粒FA实体的电势分布进行计算得出的比值，我们确定了微粒外反电荷积累的厚度壳中的1-1和2-1电解液。结果指出了抗衡离子缩合现象的参与，并引起人们质疑由静电平衡形成规范调用的对离子结合的静电贡献建模的方法。总体而言，静电对Cd-aq（2+）和Cu-aq（2+）与FA缔合的静电作用比以前发现的对于更大的腐殖酸（HA）弱。 CdFA的固有化学结合强度与CdHA相当，而CuFA复合物却比CuHA弱。

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  • 来源
    《Environmental Science & Technology》 |2018年第20期|11682-11690|共9页
  • 作者

    Town Raewyn M.; Duval Jerome F. L.; van Leeuwen Herman P.;

  • 作者单位

    Univ Antwerp, Dept Biol, Syst Physiol & Ecotoxicol Res SPHERE, Groenenborgerlaan 171, B-2020 Antwerp, Belgium;

    CNRS, UMR 7360, LIEC, F-54501 Nancy, France;

    Wageningen Univ & Res, Phys Chem & Soft Matter, Stippeneng 4, NL-6708 WE Wageningen, Netherlands;

  • 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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  • 正文语种 eng
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