Isotope Exchange between Mercuric [Hg(II)] Chloride and Hg(II) Bound to Minerals and Thiolate Ligands: Implications for Enriched Isotope Tracer Studies
Abstract
Enriched mercury (Hg) stable isotopes have been widely used as tracers in field and laboratory investigations of Hg(II) biogeochemical transformations such as methylation and demethylation. Few studies, however, have considered concurrent isotope exchange reactions between newly spiked and pre-existing Hg(II) in environmental matrices, which may alter redistribution and thus transformation of the spiked and pre-existing Hg(II). Using enriched 198Hg [as mercuric Hg(II) or HgCln species], this study investigated isotope exchange between 198Hg and pre-existing Hg(II) bound to metacinnabar (β-HgS), sediments, low-molecular-weight (LMW) thiols, and dissolved organic matter (DOM). The impact of isotope exchange on methylmercury production in the presence of organic ligands was also evaluated with an iron-reducing bacterium Geobacter sulfurreducens PCA in a phosphate buffered solution (pH 7.4). We found that spiked 198Hg readily exchanged with mineral-bound ambient Hg(II) despite concurrent Hg(II) adsorption and immobilization on the solids. Rapid exchange (<3 min) was also observed between spiked 198Hg and 200Hg pre-equilibrated with LMW thiols and DOM in solution. While the exchange did not cause net changes in Hg(II) chemical speciation, it resulted in redistribution of Hg(II) isotopes bound to the ligands and thus an apparently similar methylation rate and magnitude of the spiked 198Hg and pre-existing 200Hg by PCAmore »
- Authors:
-
[1];
[1];
[1];
[1];
[2];
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
- Lanzhou Univ. (China); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1706239
- Alternate Identifier(s):
- OSTI ID: 1731074; OSTI ID: 1810929
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Geochimica et Cosmochimica Acta
- Additional Journal Information:
- Journal Volume: 292; Journal Issue: 1; Journal ID: ISSN 0016-7037
- Publisher:
- Elsevier; The Geochemical Society; The Meteoritical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 58 GEOSCIENCES; isotope exchange; thiol ligands; natural organic matter; mercury methylation; tracer studies
Citation Formats
Zhang, Lijie, Liang, Xujun, Wang, Quanying, Zhang, Yaoling, Yin, Xiangping Lisa, Pierce, Eric M., Gu, Baohua, and Lu, Xia. Isotope Exchange between Mercuric [Hg(II)] Chloride and Hg(II) Bound to Minerals and Thiolate Ligands: Implications for Enriched Isotope Tracer Studies. United States: N. p., 2020.
Web. doi:10.1016/j.gca.2020.10.013.
Zhang, Lijie, Liang, Xujun, Wang, Quanying, Zhang, Yaoling, Yin, Xiangping Lisa, Pierce, Eric M., Gu, Baohua, & Lu, Xia. Isotope Exchange between Mercuric [Hg(II)] Chloride and Hg(II) Bound to Minerals and Thiolate Ligands: Implications for Enriched Isotope Tracer Studies. United States. https://doi.org/10.1016/j.gca.2020.10.013
Zhang, Lijie, Liang, Xujun, Wang, Quanying, Zhang, Yaoling, Yin, Xiangping Lisa, Pierce, Eric M., Gu, Baohua, and Lu, Xia. Wed .
"Isotope Exchange between Mercuric [Hg(II)] Chloride and Hg(II) Bound to Minerals and Thiolate Ligands: Implications for Enriched Isotope Tracer Studies". United States. https://doi.org/10.1016/j.gca.2020.10.013. https://www.osti.gov/servlets/purl/1706239.
@article{osti_1706239,
title = {Isotope Exchange between Mercuric [Hg(II)] Chloride and Hg(II) Bound to Minerals and Thiolate Ligands: Implications for Enriched Isotope Tracer Studies},
author = {Zhang, Lijie and Liang, Xujun and Wang, Quanying and Zhang, Yaoling and Yin, Xiangping Lisa and Pierce, Eric M. and Gu, Baohua and Lu, Xia},
abstractNote = {Enriched mercury (Hg) stable isotopes have been widely used as tracers in field and laboratory investigations of Hg(II) biogeochemical transformations such as methylation and demethylation. Few studies, however, have considered concurrent isotope exchange reactions between newly spiked and pre-existing Hg(II) in environmental matrices, which may alter redistribution and thus transformation of the spiked and pre-existing Hg(II). Using enriched 198Hg [as mercuric Hg(II) or HgCln species], this study investigated isotope exchange between 198Hg and pre-existing Hg(II) bound to metacinnabar (β-HgS), sediments, low-molecular-weight (LMW) thiols, and dissolved organic matter (DOM). The impact of isotope exchange on methylmercury production in the presence of organic ligands was also evaluated with an iron-reducing bacterium Geobacter sulfurreducens PCA in a phosphate buffered solution (pH 7.4). We found that spiked 198Hg readily exchanged with mineral-bound ambient Hg(II) despite concurrent Hg(II) adsorption and immobilization on the solids. Rapid exchange (<3 min) was also observed between spiked 198Hg and 200Hg pre-equilibrated with LMW thiols and DOM in solution. While the exchange did not cause net changes in Hg(II) chemical speciation, it resulted in redistribution of Hg(II) isotopes bound to the ligands and thus an apparently similar methylation rate and magnitude of the spiked 198Hg and pre-existing 200Hg by PCA cells when 198Hg and 200Hg were added at 1:1 ratio. These observations underscore the importance of isotope exchange when an enriched Hg isotope is applied in environmental matrices, as the exchange could potentially lead to biased rate calculations of Hg(II) transformation and bioaccumulation and thus risk assessments of new Hg(II) input to the natural ecosystems.},
doi = {10.1016/j.gca.2020.10.013},
journal = {Geochimica et Cosmochimica Acta},
number = 1,
volume = 292,
place = {United States},
year = {Wed Oct 21 00:00:00 EDT 2020},
month = {Wed Oct 21 00:00:00 EDT 2020}
}
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