Isotope ratios of methylmercury (MeHg) within organisms can be used to identify sources of MeHg that have accumulated in food webs, but these isotopic compositions are masked in organisms at lower trophic levels by the presence of inorganic mercury (iHg). To facilitate measurement of MeHg isotope ratios in organisms, we developed a method of extracting and isolating MeHg from fish and aquatic invertebrates for compound-specific isotopic analysis involving nitric acid digestion, batch anion-exchange resin separation, and pre-concentration by purge and trap. Recovery of MeHg was quantified after each step in the procedure, and the average cumulative recovery of MeHg was 93.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
November 2022
The origin of methylmercury in pelagic fish remains unclear, with many unanswered questions regarding the production and degradation of this neurotoxin in the water column. We used mercury (Hg) stable isotope ratios of marine particles and biota to elucidate the cycling of methylmercury prior to incorporation into the marine food web. The Hg isotopic composition of particles, zooplankton, and fish reveals preferential methylation of Hg within small (< 53 µm) marine particles in the upper 400 m of the North Pacific Ocean.
View Article and Find Full Text PDFSci Total Environ
December 2022
Atmospheric elemental mercury (Hg(0)) enters plant stomata, becomes oxidized, and is then transferred to annual growth rings providing an archive of air Hg(0) concentrations. To better understand the processes of Hg accumulation and translocation, the foliage of quaking aspen and Austrian pine were exposed to Hg(0), and methylmercury (MeHg) or MeHg via roots, in controlled exposures during the summer. Isotopic measurements demonstrated, in a laboratory setting, that the natural mass-dependent fractionation observed was the same as that measured in field studies, with the lighter isotopes being preferentially taken up by the leaves.
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February 2022
The geochemical cycle of mercury in Earth's surface environment (atmosphere, hydrosphere, biosphere) has been extensively studied; however, the deep geological cycling of this element is less well known. Here we document distinct mass-independent mercury isotope fractionation (expressed as ΔHg) in island arc basalts and mid-ocean ridge basalts. Both rock groups show positive ΔHg values up to 0.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
August 2021
Earth's early atmosphere witnessed multiple transient episodes of oxygenation before the Great Oxidation Event 2.4 billion years ago (Ga) [e.g.
View Article and Find Full Text PDFSci Total Environ
August 2021
Atmospheric deposition of mercury (Hg) to terrestrial and aquatic ecosystems has significant implications for human and animal exposure. Measurements of Hg isotopic composition can be utilized to trace sources of Hg, but outside of the Arctic there has been little Hg isotopic characterization of snow. To better understand deposition pathways at mid-latitudes, five time series of snowfall were collected at two sites (Dexter and Pellston, Michigan, USA) to investigate the Hg isotopic composition of snowfall, how it changes after deposition, and how it compares to rain.
View Article and Find Full Text PDFEnviron Sci Process Impacts
May 2021
The goal of this project was to assess how anthropogenic legacy mercury (Hg) retained in streambed sediment may be remobilized to stream water. To do this, we performed sequential extractions and Hg isotope analyses on streambed sediment collected along the length of East Fork Poplar Creek, a point-source contaminated stream in Oak Ridge, Tennessee, USA. Legacy Hg within streambed sediment appears to have been isotopically fractionated by equilibrium isotope effects driven by isotope exchange between co-existing Hg(0) and Hg(ii) species, potentially over-printing fractionation patterns that would have been imparted by kinetic redox reactions.
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November 2020
Mercury isotopic compositions of amphipods and snailfish from deep-sea trenches reveal information on the sources and transformations of mercury in the deep oceans. Evidence for methyl-mercury subjected to photochemical degradation in the photic zone is provided by odd-mass independent isotope values (ΔHg) in amphipods from the Kermadec Trench, which average 1.57‰ (±0.
View Article and Find Full Text PDFEnviron Sci Technol
September 2020
The atmosphere is a significant global reservoir for mercury (Hg) and its isotopic characterization is important to understand sources, distribution, and deposition of Hg to the Earth's surface. To better understand Hg isotope variability in the remote background atmosphere, we collected continuous 12-h Hg samples for 1 week from two high elevation sites, Camp Davis, Wyoming (valley), and Mount Bachelor, Oregon (mountaintop). The samples collected at Camp Davis displayed strong diel variation in δHg values of Hg, but not in ΔHg or ΔHg values.
View Article and Find Full Text PDFACS Pharmacol Transl Sci
June 2020