Rates and Dynamics of Mercury Isotope Exchange between Dissolved Elemental Hg(0) and Hg(II) Bound to Organic and Inorganic Ligands

Wang, Quanying; Zhang, Lijie; Liang, Xujun; Yin, Xiangping; Zhang, Yaoling; Zheng, Wang; Pierce, Eric M.; Gu, Baohua

doi:10.1021/acs.est.0c06229

Title: Rates and Dynamics of Mercury Isotope Exchange between Dissolved Elemental Hg(0) and Hg(II) Bound to Organic and Inorganic Ligands

Journal Article · Mon Nov 16 00:00:00 EST 2020 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.0c06229· OSTI ID:1714402

Wang, Quanying ^[1]; Zhang, Lijie ^[2]; Liang, Xujun ^[2]; Yin, Xiangping ^[2]; Zhang, Yaoling ^[2];

^[3];

^[2];

^[4]

Key Laboratory of Wet Ecology and Environment, Northeast Institute of Geography and Agroecology, Chinese Academy of Sciences, Changchun 130102, China;Environmental Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States
Environmental Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States
Environmental Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States;Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China
Environmental Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States;Department of Biosystems Engineering and Soil Science, University of Tennessee, Knoxville, Tennessee 37996, United States

Mercury (Hg) isotope exchange is a common process in biogeochemical transformations of Hg in the environment, but it is unclear whether and at what rates dissolved elemental Hg(0)_aq may exchange with divalent Hg(II) bound to various organic and inorganic ligands in water. Using enriched stable isotopes, in this study we investigated the rates and dynamics of isotope exchange between ²⁰²Hg(0)_aq and ²⁰¹Hg(II) bound to organic and inorganic ligands with varying chemical structures and binding affinities. Time-dependent exchange reactions were followed by isotope compositional changes using both inductively coupled plasma mass spectrometry and Zeeman cold vapor atomic absorption spectrometry. Rapid, spontaneous isotope exchange (<1 h) was observed between ²⁰²Hg(0)_aq and ²⁰¹Hg(II) bound to chloride (Cl^–), ethylenediaminetetraacetate (EDTA), and thiols, such as cysteine (CYS), glutathione (GSH), and 2,3-dimercaptopropanesulfonic acid (DMPS) at a thiol ligand-to-Hg(II) molar ratio of 1:1. Without external reductants or oxidants, the exchange resulted in transfer of two electrons and redistribution of Hg isotopes bound to the ligand but no net changes of chemical species in the system. However, an increase in the ligand-to-Hg(II) ratio decreased the exchange rates due to the formation of 2:1 or higher thiol:Hg(II) chelated complexes, but had no effects on exchange rates with ²⁰¹Hg(II) bound to EDTA or Cl^–. The exchange between ²⁰²Hg(0)_aq and ²⁰¹Hg(II) bound to dissolved organic matter (DOM) showed an initially rapid followed by a slower exchange rate, likely resulting from Hg(II) complexation with both low- and high-affinity binding functional groups on DOM (e.g., carboxylates vs bidentate thiolates). These results demonstrate that Hg(0)_aq readily exchanges with Hg(II) bound to various ligands and highlight the importance of considering exchange reactions in experimental enriched Hg isotope tracer studies or in natural abundance Hg isotope studies in environmental matrices.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1714402

Alternate ID(s):: OSTI ID: 1731063

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Vol. 54 Journal Issue: 23; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Rates and Dynamics of Mercury Isotope Exchange between Dissolved Elemental Hg(0) and Hg(II) Bound to Organic and Inorganic Ligands

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