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Molecular Fates of Organometallic Mercury in Human Brain

  • Ashley K. James
    Ashley K. James
    Toxicology Centre, University of Saskatchewan, 44 Campus Drive, Saskatoon, Saskatchewan S7N 5B3, Canada
    Department of Geological Sciences, University of Saskatchewan, 114 Science Place, Saskatoon, Saskatchewan S7N 5E2, Canada
  • Natalia V. Dolgova
    Natalia V. Dolgova
    Department of Geological Sciences, University of Saskatchewan, 114 Science Place, Saskatoon, Saskatchewan S7N 5E2, Canada
  • Susan Nehzati
    Susan Nehzati
    Department of Geological Sciences, University of Saskatchewan, 114 Science Place, Saskatoon, Saskatchewan S7N 5E2, Canada
  • Malgorzata Korbas
    Malgorzata Korbas
    Canadian Light Source, 44 Innovation Blvd., Saskatoon, Saskatchewan S7N 2V3, Canada
  • Julien J. H. Cotelesage
    Julien J. H. Cotelesage
    Department of Geological Sciences, University of Saskatchewan, 114 Science Place, Saskatoon, Saskatchewan S7N 5E2, Canada
  • Dimosthenis Sokaras
    Dimosthenis Sokaras
    Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Stanford University, Menlo Park, California 94025, United States
  • Thomas Kroll
    Thomas Kroll
    Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Stanford University, Menlo Park, California 94025, United States
    More by Thomas Kroll
  • John L. O’Donoghue
    John L. O’Donoghue
    Department of Environmental Medicine, School of Medicine and Dentistry, University of Rochester, Rochester, New York 14642, United States
  • Gene E. Watson
    Gene E. Watson
    Department of Environmental Medicine, School of Medicine and Dentistry, University of Rochester, Rochester, New York 14642, United States
    Eastman Institute for Oral Health, School of Medicine and Dentistry, University of Rochester, Rochester, New York 14642, United States
  • Gary J. Myers
    Gary J. Myers
    Department of Environmental Medicine, School of Medicine and Dentistry, University of Rochester, Rochester, New York 14642, United States
    Departments of Neurology and Pediatrics, School of Medicine and Dentistry, University of Rochester, Rochester, New York 14642, United States
  • Ingrid J. Pickering*
    Ingrid J. Pickering
    Department of Geological Sciences, University of Saskatchewan, 114 Science Place, Saskatoon, Saskatchewan S7N 5E2, Canada
    Toxicology Centre, University of Saskatchewan, 44 Campus Drive, Saskatoon, Saskatchewan S7N 5B3, Canada
    Department of Chemistry, University of Saskatchewan, Saskatoon, Saskatchewan S7N 5C9, Canada
    *Email: [email protected]
  • , and 
  • Graham N. George*
    Graham N. George
    Department of Geological Sciences, University of Saskatchewan, 114 Science Place, Saskatoon, Saskatchewan S7N 5E2, Canada
    Toxicology Centre, University of Saskatchewan, 44 Campus Drive, Saskatoon, Saskatchewan S7N 5B3, Canada
    Department of Chemistry, University of Saskatchewan, Saskatoon, Saskatchewan S7N 5C9, Canada
    *Email: [email protected]
Cite this: ACS Chem. Neurosci. 2022, 13, 12, 1756–1768
Publication Date (Web):May 11, 2022
https://doi.org/10.1021/acschemneuro.2c00166
Copyright © 2022 American Chemical Society

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    Abstract

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    Mercury is ubiquitous in the environment, with rising levels due to pollution and climate change being a current global concern. Many mercury compounds are notorious for their toxicity, with the potential of organometallic mercury compounds for devastating effects on the structures and functions of the central nervous system being of particular concern. Chronic exposure of human populations to low levels of methylmercury compounds occurs through consumption of fish and other seafood, although the health consequences, if any, from this exposure remain controversial. We have used high energy resolution fluorescence detected X-ray absorption spectroscopy to determine the speciation of mercury and selenium in human brain tissue. We show that the molecular fate of mercury differs dramatically between individuals who suffered acute organometallic mercury exposure (poisoning) and individuals with chronic low-level exposure from a diet rich in marine fish. For long-term low-level methylmercury exposure from fish consumption, mercury speciation in brain tissue shows methylmercury coordinated to an aliphatic thiolate, resembling the coordination environment observed in marine fish. In marked contrast, for short-term high-level exposure, we observe the presence of biologically less available mercuric selenide deposits, confirmed by X-ray fluorescence imaging, as well as mercury(II)-bis-thiolate complexes, which may be signatures of severe poisoning in humans. These differences between low-level and high-level exposures challenge the relevance of studies involving acute exposure as a proxy for low-level chronic exposure.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acschemneuro.2c00166.

    • Procedures for preparation of standard compounds used in linear combination fitting for both mercury and selenium (PDF)

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    Cited By

    This article is cited by 2 publications.

    1. Marina Patriarca, Nicola Barlow, Alan Cross, Sarah Hill, Anna Robson, Julian Tyson. Atomic spectrometry update: review of advances in the analysis of clinical and biological materials, foods and beverages. Journal of Analytical Atomic Spectrometry 2023, 38 (3) , 496-577. https://doi.org/10.1039/D3JA90008H
    2. Miantai Ye, Yunhui Xiang, Jiankang Gong, Xiaoyu Wang, Zhiqiang Mao, Zhihong Liu. Monitoring Hg2+ and MeHg+ poisoning in living body with an activatable near-infrared II fluorescence probe. Journal of Hazardous Materials 2023, 445 , 130612. https://doi.org/10.1016/j.jhazmat.2022.130612

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