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Kinetics of Methylmercury Production Revisited
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    Kinetics of Methylmercury Production Revisited
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    Environmental Sciences Division, Oak Ridge National Laboratory, P.O. Box 2008, MS 6038, Oak Ridge, Tennessee 37831-6038, United States
    *E-mail: [email protected]. Tel: 865-574-6398. Fax: 865-576-8646.
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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2018, 52, 4, 2063–2070
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    https://doi.org/10.1021/acs.est.7b05152
    Published January 27, 2018
    Copyright © 2018 American Chemical Society

    Abstract

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    Laboratory measurements of the biologically mediated methylation of mercury (Hg) to the neurotoxin monomethylmercury (MMHg) often exhibit kinetics that are inconsistent with first-order kinetic models. Using time-resolved measurements of filter passing Hg and MMHg during methylation/demethylation assays, a multisite kinetic sorption model, and reanalyses of previous assays, we show that competing kinetic sorption reactions can lead to time-varying availability and apparent non-first-order kinetics in Hg methylation and MMHg demethylation. The new model employing a multisite kinetic sorption model for Hg and MMHg can describe the range of behaviors for time-resolved methylation/demethylation data reported in the literature including those that exhibit non-first-order kinetics. Additionally, we show that neglecting competing sorption processes can confound analyses of methylation/demethylation assays, resulting in rate constant estimates that are systematically biased low. Simulations of MMHg production and transport in a hypothetical periphyton biofilm bed illustrate the implications of our new model and demonstrate that methylmercury production may be significantly different than projected by single-rate first-order models.

    Copyright © 2018 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.7b05152.

    • All data generated or analyzed during this study are included in the Supporting Information file. MATLAB files used in this study and the Mathematica files used to generate Figure 6 are available from the authors upon request. The Supporting Information includes details on the field-scale transport model, five additional figures and five tables (PDF)

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    This article is cited by 20 publications.

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    2. Mareike Gutensohn, Jeffra K. Schaefer, Elena Yunda, Ulf Skyllberg, Erik Björn. The Combined Effect of Hg(II) Speciation, Thiol Metabolism, and Cell Physiology on Methylmercury Formation by Geobacter sulfurreducens. Environmental Science & Technology 2023, 57 (18) , 7185-7195. https://doi.org/10.1021/acs.est.3c00226
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    9. Stefanie Helmrich, Dimitri Vlassopoulos, Charles N. Alpers, Peggy A. O’Day. Critical review of mercury methylation and methylmercury demethylation rate constants in aquatic sediments for biogeochemical modeling. Critical Reviews in Environmental Science and Technology 2022, 52 (24) , 4353-4378. https://doi.org/10.1080/10643389.2021.2013073
    10. Grace E. Schwartz, Katherine A. Muller, Saubhagya S. Rathore, Regina L. Wilpiszeski, Alyssa A. Carrell, Melissa A. Cregger, Dwayne A. Elias, Mircea Podar, Scott L. Painter, Scott C. Brooks. Incorporating concentration-dependent sediment microbial activity into methylmercury production kinetics modeling. Environmental Science: Processes & Impacts 2022, 24 (9) , 1392-1405. https://doi.org/10.1039/D1EM00287B
    11. Saubhagya S. Rathore, Grace E. Schwartz, Scott C. Brooks, Scott L. Painter. Joint estimation of biogeochemical model parameters from multiple experiments: A bayesian approach applied to mercury methylation. Environmental Modelling & Software 2022, 155 , 105453. https://doi.org/10.1016/j.envsoft.2022.105453
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    15. Maxime Leclerc, Makayla C. Harrison, Veronika Storck, Dolors Planas, Marc Amyot, David A. Walsh, . Microbial Diversity and Mercury Methylation Activity in Periphytic Biofilms at a Run-of-River Hydroelectric Dam and Constructed Wetlands. mSphere 2021, 6 (2) https://doi.org/10.1128/mSphere.00021-21
    16. Alyssa A. Carrell, Grace E. Schwartz, Melissa A. Cregger, Caitlin M. Gionfriddo, Dwayne A. Elias, Regina L. Wilpiszeski, Dawn M. Klingeman, Ann M. Wymore, Katherine A. Muller, Scott C. Brooks. Nutrient Exposure Alters Microbial Composition, Structure, and Mercury Methylating Activity in Periphyton in a Contaminated Watershed. Frontiers in Microbiology 2021, 12 https://doi.org/10.3389/fmicb.2021.647861
    17. Van Liem-Nguyen, Ulf Skyllberg, Erik Björn. Methylmercury formation in boreal wetlands in relation to chemical speciation of mercury(II) and concentration of low molecular mass thiols. Science of The Total Environment 2021, 755 , 142666. https://doi.org/10.1016/j.scitotenv.2020.142666
    18. Ke Pan, Jingli Liu, Yanping Li, Dandan Duan, Guogan Peng, Ping Li, Pei Lei, Huan Zhong, Martin Tsz-Ki Tsui. Effects and Mechanisms of Organic Matter Regulating the Methylmercury Dynamics in Mangrove Sediments. SSRN Electronic Journal 2021, 82 https://doi.org/10.2139/ssrn.3997666
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    20. Grace E. Schwartz, Todd A. Olsen, Katherine A. Muller, Scott C. Brooks. Ecosystem Controls on Methylmercury Production by Periphyton Biofilms in a Contaminated Stream: Implications for Predictive Modeling. Environmental Toxicology and Chemistry 2019, 38 (11) , 2426-2435. https://doi.org/10.1002/etc.4551

    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2018, 52, 4, 2063–2070
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.est.7b05152
    Published January 27, 2018
    Copyright © 2018 American Chemical Society

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