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首页> 外文期刊>Environmental Science & Technology >Equilibrium Mercury Isotope Fractionation between Dissolved Hg(II) Species and Thiol-Bound Hg
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Equilibrium Mercury Isotope Fractionation between Dissolved Hg(II) Species and Thiol-Bound Hg

机译：溶解态Hg（II）物种与硫醇结合的Hg之间的平衡汞同位素分馏

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摘要

Stable Hg isotope ratios provide a new tool to trace environmental Hg cycling. Thiols (-SH) are the dominant Hg-binding groups in natural organic matter. Here, we report experimental and computational results on equilibrium Hg isotope fractionation between dissolved Hg(II) species and thiol-bound Hg. Hg(II) chloride and nitrate solutions were equilibrated in parallel batches with varying amounts of thiol resin resulting in different fractions of thiol-bound and free Hg. Mercury isotope ratios in both fractions were analyzed by multiple collector inductively coupled plasma mass spectrometry (MC-ICPMS). Theoretical equilibrium Hg isotope effects by mass-dependent fractionation (MDF) and nuclear volume fractionation (NVF) were calculated for 14 relevant Hg(II) species. The experimental data revealed that thiol-bound Hg was enriched in light Hg isotopes by 0.53‰ and 0.62‰(δ~(202)Hg) relative to HgCl_2 and Hg(OH)_2, respectively. The computational results were in excellent agreement with the experimental data indicating that a combination of MDF and NVF was responsible for the observed Hg isotope fractionation. Small mass-independent fractionation (MIF) effects (<0.1‰) were observed representing one of the first experimental evidences for MIF of Hg isotopes by NVF. Our results indicate that significant equilibrium Hg isotope fractionation can occur without redox transition, and that NVF must be considered in addition to MDF to explain Hg isotope variations.
机译：稳定的汞同位素比提供了一种追踪环境汞循环的新工具。硫醇（-SH）是天然有机物中主要的Hg结合基团。在这里，我们报告了溶解的Hg（II）物种和硫醇结合的Hg之间的平衡Hg同位素分级分离的实验和计算结果。用不同量的硫醇树脂平行分批平衡氯化汞和硝酸汞溶液，得到不同比例的硫醇结合和游离汞。通过多收集器电感耦合等离子体质谱法（MC-ICPMS）分析了两个馏分中的汞同位素比。针对14种相关的Hg（II）物种，通过质量依赖性分馏（MDF）和核体积分馏（NVF）得出了理论平衡的Hg同位素效应。实验数据表明，相对于HgCl_2和Hg（OH）_2，硫醇结合的Hg在轻质Hg同位素中的富集度分别为0.53‰（δ〜（202）Hg）。计算结果与实验数据非常吻合，表明MDF和NVF的结合是所观察到的汞同位素分馏的原因。观察到较小的非质量分数分离（MIF）效应（<0.1‰），这是NVF对Hg同位素MIF的最早实验证据之一。我们的结果表明，在没有氧化还原过渡的情况下，可以发生显着的平衡汞同位素分馏，并且除了MDF以外，还必须考虑NVF来解释汞同位素变化。

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  • 来源
    《Environmental Science & Technology》 |2010年第11期|P.4191-4197|共7页
  • 作者

    JAN G. WIEDERHOLD; CHRISTOPHER J. CRAMER; KELLY DANIEL; IVAN INFANTE; BERNARD BOURDON; RUBEN KRETZSCHMAR;

  • 作者单位

    Institute of Biogeochemistry and Pollutant Dynamics, Soil Chemistry, ETH Zurich, Switzerland Institute of Geochemistry and Petrology, Isotope Geochemistry, ETH Zurich, Switzerland;

    rnDepartment of Chemistry and Supercomputing Institute, University of Minnesota;

    rnDepartment of Chemistry and Supercomputing Institute, University of Minnesota;

    rnDepartment of Physical Chemistry, University of Geneva, Switzerland;

    rnInstitute of Geochemistry and Petrology, Isotope Geochemistry, ETH Zurich, Switzerland;

    rnInstitute of Biogeochemistry and Pollutant Dynamics, Soil Chemistry, ETH Zurich, Switzerland;

  • 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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