18 research outputs found
Geochemical and Microbiological Controls on Mercury Methylation in Natural Waters
No full textMercury (Hg) is a global pollutant toxic to humans and wildlife. Monomethylmercury (MMHg) is a bioavailable compound that bioaccumulates and biomagnifies in food webs. Humans are primarily exposed to MMHg from seafood consumption (Sunderland 2007), and high quantities of the neurotoxin lead to reduced neurocognitive functioning in adults and the children of exposed mothers (Cohen et al. 2005, Yokoo et al. 2003). Negative effects from MMHg accumulation on the health of humans and wildlife requires a more complete understanding of the chemistry and microbiology driving Hg methylation in both marine and freshwater systems. This work focuses on water column distribution, speciation, and methylation of Hg. The aims of this dissertation are three-fold: (1) characterize the speciation and distribution of Hg in the western Arctic Ocean; (2) examine seasonal variations in Hg speciation, methylation, and demethylation, and the microbial communities of Hg methylators in Crystal Lake, Ohio; and (3) quantify Hg methylation rates and characterize methylating microbial communities in waters on the continental shelf of the northwest Atlantic Ocean. While Hg methylation has been studied for decades, this work is built upon recent improvements in Hg detection limits, and newly discovered genes responsible for Hg methylation. In conjunction with U.S. Arctic GEOTRACES (GN01), the western Arctic Ocean was sampled in the summer of 2015. Although Hg concentrations in the Canada and Eurasian Basins were low relative to the Atlantic and Pacific Oceans, higher MMHg concentrations were observed in Arctic seawater that recently interacted with continental margins. We estimate that the Arctic Ocean receives 4-71 kmol Hg yr−1 from the Bering Strait, which is likely to interact with sediments of the shallow continental shelves before entering into the Arctic Ocean. This is potentially important, because while the estimated atmospheric input to the Arctic Ocean is ~400 kmol Hg yr−1, inflowing Hg from the Bering Strait may still be an important source of Hg that can be methylated on the Chukchi Shelf. Mercury methylation potentials were measured in a stratified freshwater system, Crystal Lake, in Dayton, Ohio (objective #2). Mercury methylation occurred in both oxic and anoxic portions of the water column, but methylation potentials were greatest at the oxic/anoxic boundary layer. Mercury methylating genes were found throughout the water column and had the greatest copy number in the hypolimnion. Similarly, previous marine work showed that sediments and the microbial communities therein are large sources of MMHg to near shore marine systems (Fitzgerald et al. 2007), which led to methylation and demethylation studies along the northwest Atlantic shelf (objective #3). Greater abundance of Hg methylating microbes were observed in water overlying sediment as opposed to shallower waters, but methylation potentials did not significantly differ. Together, these results suggested that (1) Archaea may be responsible for Hg methylation in oxic waters; and (2) redox transition zones in the water column and the sediment-water interface are important sources of bioavailable MMHg. These studies improve our understanding of Hg cycling in natural waters and suggest possible conditions and organisms that stimulate Hg methylation
The spatial and temporal variability of Mn speciation in the coastal Northwest Atlantic Ocean
No full textAuthor Posting. © American Geophysical Union, 2020. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Journal of Geophysical Research-Oceans 125(1),(2020): e2019JC015167, doi:10.1029/2019JC015167.Manganese (Mn) is distributed widely throughout the global ocean, where it cycles between three oxidation states that each play important biogeochemical roles. The speciation of Mn in seawater was previously operationally defined on filtration, with soluble Mn presumed to be Mn(II) and solid‐phase Mn as Mn(III/IV) oxides. Recent findings of abundant soluble Mn(III) complexes (Mn(III)‐L) highlights the need to reexamine the redox cycling of Mn, as these complexes can donate or accept electrons. To better understand the complex cycling of Mn in coastal waters, the distribution of Mn species at four Northwest Atlantic sites with different characteristics was examined. Diurnal influences on Mn speciation were investigated within a productive site. At all sites, Mn(III)‐L complexes dominated, particularly in surface waters, and Mn oxides were low in abundance in surface waters but high in bottom waters. Despite intrasite similarities, Mn speciation was highly variable between our stations, emphasizing the diverse processes that impact Mn redox. Diel Mn measurements revealed that the cycling of Mn is also highly variable over time, even on time scales as short as hours. We observed a change of over 100 nM total Mn over 17 hrs and find that speciation changed drastically. These changes could include contributions from biological, light‐mediated, and/or abiotic mechanisms but more likely point to the importance of lateral mixing at coastal sites. This exploration demonstrates the spatial and temporal variability of the Mn redox cycle and indicates that single timepoint vertical profiling is not sufficient when describing the geochemistry of dynamic coastal systems.This work was funded by grants from the Chemical Oceanography program of the National Science Foundation (OCE‐1355720 to CMH and CHL). Véronique Oldham thanks Woods Hole Oceanographic Institution for the receipt of the WHOI Postdoctoral Scholarship. Thanks also to Kevin Sutherland, Jen Karolweski, Gabriella Farfan, Kalina Grabb, Kaitlin Bowman, Alison Agather, and Lindsey Starr for the shipboard sampling assistance, as well as the captain and crew of the R/V Endeavor who made the sampling for this research possible. All data presented in the manuscript are available through the Biological and Chemical Oceanography Data Management Office (BCO‐DMO) under Project 756930 at the following link (https://www.bco‐dmo.org/project/756930).2020-06-2
Distribution of mercury species across a zonal section of the eastern tropical South Pacific Ocean (U.S. GEOTRACES GP16)
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Distribution of mercury species in the Western Arctic Ocean (U.S. GEOTRACES GN01)
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External Sources Inhibit Benthic Phosphorus Fluxes in the Lower Great Miami River, Southwest Ohio
No full textDistribution of mercury‐cycling genes in the Arctic and equatorial Pacific Oceans and their relationship to mercury speciation
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