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Aqueous Elemental Mercury Production versus Mercury Inventories in the Lake Michigan Airshed: Deciphering the Spatial and Diel Controls of Mercury Gradients in Air and Water
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    Aqueous Elemental Mercury Production versus Mercury Inventories in the Lake Michigan Airshed: Deciphering the Spatial and Diel Controls of Mercury Gradients in Air and Water
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    • Ryan F. Lepak*
      Ryan F. Lepak
      Environmental Chemistry and Technology Program, University of Wisconsin−Madison, 660 North Park Street, Madison, Wisconsin 53706, United States
      Upper Midwest Water Science Center, USGS Mercury Research Laboratory, U.S. Geological Survey, 8505 Research Way, Middleton, Wisconsin 53562, United States
      Center for Computational Toxicology and Exposure, Great Lakes Toxicology and Ecology Division, U.S. EPA Office of Research and Development, 6201 Congdon Boulevard, Duluth, Minnesota 55804, United States
      *U.S. EPA Office of Research and Development, Center for Computational Toxicology and Exposure, Great Lakes Toxicology and Ecology Division, 6201 Congdon Blvd., Duluth, MN 55804. Email: [email protected]
    • Michael T. Tate
      Michael T. Tate
      Upper Midwest Water Science Center, USGS Mercury Research Laboratory, U.S. Geological Survey, 8505 Research Way, Middleton, Wisconsin 53562, United States
    • Jacob M. Ogorek
      Jacob M. Ogorek
      Upper Midwest Water Science Center, USGS Mercury Research Laboratory, U.S. Geological Survey, 8505 Research Way, Middleton, Wisconsin 53562, United States
    • John F. DeWild
      John F. DeWild
      Upper Midwest Water Science Center, USGS Mercury Research Laboratory, U.S. Geological Survey, 8505 Research Way, Middleton, Wisconsin 53562, United States
    • Benjamin D. Peterson
      Benjamin D. Peterson
      Environmental Chemistry and Technology Program, University of Wisconsin−Madison, 660 North Park Street, Madison, Wisconsin 53706, United States
    • James P. Hurley
      James P. Hurley
      Environmental Chemistry and Technology Program, University of Wisconsin−Madison, 660 North Park Street, Madison, Wisconsin 53706, United States
      University of Wisconsin Aquatic Sciences Center, 1975 Willow Drive, Madison, Wisconsin 53706, United States
    • David P. Krabbenhoft
      David P. Krabbenhoft
      Upper Midwest Water Science Center, USGS Mercury Research Laboratory, U.S. Geological Survey, 8505 Research Way, Middleton, Wisconsin 53562, United States
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    ACS ES&T Water

    Cite this: ACS EST Water 2021, 1, 3, 719–727
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    https://doi.org/10.1021/acsestwater.0c00187
    Published December 30, 2020
    Copyright © 2020 American Chemical Society

    Abstract

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    Atmospheric delivery of mercury (Hg) is important to the Upper Great Lakes, and understanding gaseous Hg exchange between surface water and air is critical to predicting the effects of declining mercury emissions. Speciated atmospheric Hg, dissolved gaseous Hg (DGM), and particulate and filter passing total Hg were measured on a cruise in Lake Michigan. Low mercury levels reflected pristine background conditions, especially in offshore regions. In the atmosphere, reactive and particle-associated fractions were low (1.0 ± 0.5%) compared to gaseous elemental Hg (1.34 ± 0.14 ng m–3) and were elevated in the urbanized southern basin. DGM was supersaturated, ranging from 17.5 ± 4.8 pg L–1 (330 ± 80%) in the main lake to 33.2 ± 2.4 pg L–1 (730 ± 70%) in Green Bay. Diel cycling of surface DGM showed strong Hg efflux during the day due to increased winds, and build-up at night from continued DGM production. Epilimnetic DGM is formed from photochemical reduction, while hypolimnetic DGM originates from biological Hg reduction. We found that DGM concentrations were greatest below the thermocline (30.8 ± 13.6 pg L–1), accounting for 68–92% of the total DGM in Lake Michigan, highlighting the importance of nonphotochemical reduction in deep stratified lakes.

    Copyright © 2020 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsestwater.0c00187.

    • Additional text, analytical method comparisons, vertical water chemistry profiles at point locations, satellite imagery of Lake Michigan for the cruise dates, and relevant data tables (PDF)

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    This article is cited by 8 publications.

    1. Xiaoyan Zhang, Yingying Guo, Guangliang Liu, Yanwei Liu, Jianbo Shi, Ligang Hu, Lixia Zhao, Yanbin Li, Yongguang Yin, Yong Cai, Guibin Jiang. Superoxide-Mediated Extracellular Mercury Reduction by Aerobic Marine Bacterium Alteromonas sp. KD01. Environmental Science & Technology 2023, 57 (49) , 20595-20604. https://doi.org/10.1021/acs.est.3c04777
    2. Xiaoyan Zhang, Yingying Guo, Guangliang Liu, Yanwei Liu, Maoyong Song, Jianbo Shi, Ligang Hu, Yanbin Li, Yongguang Yin, Yong Cai, Guibin Jiang. Dark Reduction of Mercury by Microalgae-Associated Aerobic Bacteria in Marine Environments. Environmental Science & Technology 2021, 55 (20) , 14258-14268. https://doi.org/10.1021/acs.est.1c03608
    3. Jacob M. Ogorek, Ryan F. Lepak, Joel C. Hoffman, John F. DeWild, Tylor J. Rosera, Michael T. Tate, James P. Hurley, David P. Krabbenhoft. Enhanced Susceptibility of Methylmercury Bioaccumulation into Seston of the Laurentian Great Lakes. Environmental Science & Technology 2021, 55 (18) , 12714-12723. https://doi.org/10.1021/acs.est.1c02319
    4. Yuwei Wang, Gideon Bartov, Thomas Wang, John R. Reinfelder, Thomas M. Johnson, Nathan Yee. Rapid Attainment of Isotopic Equilibrium after Mercury Reduction by Ferrous Iron Minerals and Isotopic Exchange between Hg(II) and Hg(0). ACS Earth and Space Chemistry 2021, 5 (6) , 1384-1394. https://doi.org/10.1021/acsearthspacechem.1c00026
    5. Jiebo Zhen, Tao Li, Hongming Cai, Xiaoling Nie, Sheng He, Mei Meng, Yan Wang, Jiubin Chen. Photoreduction and origin of dissolved and particulate mercury in cloud water: Insights from stable mercury isotopes. Journal of Hazardous Materials 2024, 474 , 134654. https://doi.org/10.1016/j.jhazmat.2024.134654
    6. Federico Floreani, Nicolò Barago, Katja Klun, Jadran Faganeli, Stefano Covelli. Dissolved gaseous mercury production and sea-air gaseous exchange in impacted coastal environments of the northern Adriatic Sea. Environmental Pollution 2023, 332 , 121926. https://doi.org/10.1016/j.envpol.2023.121926
    7. Ting Liu, Zhuo Xiong, Peng Ni, Zizhen Ma, Yan Tan, Zishun Li, Shengnan Deng, Yincui Li, Qirong Yang, Huawei Zhang. Review on adsorbents in elemental mercury removal in coal combustion flue gas, smelting flue gas and natural gas. Chemical Engineering Journal 2023, 454 , 140095. https://doi.org/10.1016/j.cej.2022.140095
    8. Federico Floreani, Alessandro Acquavita, Nicolò Barago, Katja Klun, Jadran Faganeli, Stefano Covelli. Gaseous Mercury Exchange from Water–Air Interface in Differently Impacted Freshwater Environments. International Journal of Environmental Research and Public Health 2022, 19 (13) , 8149. https://doi.org/10.3390/ijerph19138149

    ACS ES&T Water

    Cite this: ACS EST Water 2021, 1, 3, 719–727
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsestwater.0c00187
    Published December 30, 2020
    Copyright © 2020 American Chemical Society

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