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Grace Jane Armstrong

Publications and source records attributed to Grace Jane Armstrong.

5 recordsLinked to original sources

Comparing in vivo methylmercury detoxification in hunted duck: Implications for wildlife and human health

Great Salt Lake (GSL) waterfowl have elevated mercury (Hg) concentrations, and in vivo detoxification of neurotoxic and bioaccumulative methylmercury (MeHg) can occur through Hg-selenium (Se) complexation, influencing the suitability of Hg consumption advisories. Here, we present Hg chemical speciation and Hg stable isotope measurements of brain, breast muscle, liver, and kidney samples from two GSL duck species─northern shoveler ( Spatula clypeata ) and cinnamon teal (Spatula cyanoptera). Chemical and stable isotope measurements, along with high energy resolution fluorescence detected X-ray absorption near-edge structure (HERFD-XANES) spectroscopy, indicate the occurrence of in vivo MeHg demethylation in both bird species. The percentage of total Hg (THg) as MeHg (% MeHg) varied with tissue type (brain > breast muscle > kidney > liver), and differences between δ 202 THg and δ 202 MeHg were linearly correlated with % MeHg. Demethylated inorganic Hg was a mixture of Hg-dithiolate (Hg(SR) 2 ) and Hg-tetraselenolate (Hg(Sec) 4 ) in both bird species. Notably, liver THg concentrations were elevated in northern shoveler liver tissues relative to those of cinnamon teal (7.54 ± 4.69 mg/kg versus 2.19 ± 1.27 mg/kg, dry weight, respectively) and % MeHg liver values were significantly lower (40% ± 19% versus 68% ± 14%), indicating taxonomic differences in Hg detoxification and depuration. THg concentrations in waterfowl species from this study were comparable to previously reported levels, indicating that elevated Hg concentrations in northern shoveler and cinnamon teal at GSL have persisted over the past two decades. Due to in vivo demethylation, we show that THg is not an effective proxy for MeHg within duck species, carrying implications for current GSL waterfowl consumption advisories and assessments exposure risk. This study highlights important differences in MeHg detoxification between waterbird taxa and provides further insights into Hg toxicity risk to GSL waterbirds.

Utah

Seasonal stratification drives bioaccumulation of pelagic mercury sources in eutrophic lakes

Increased lake eutrophication, influenced by changing climate and land use, alters aquatic cycling and bioaccumulation of mercury (Hg). Additionally, seasonally dynamic lake circulation and plankton community composition can confound our ability to predict changes in biological Hg concentrations and sources. To assess temporal variation, we examined seasonal total Hg (THg) and methylmercury (MeHg) concentrations and stable isotope values in seston, waters, sediments, and fish from two adjacent urban eutrophic lakes in Madison, Wisconsin. In Lake Monona, surface sediment THg concentrations were elevated due to comparably higher urbanization and historical industrial inputs, whereas Lake Mendota sediments had lower concentrations corresponding with largely agricultural and suburban surrounding watershed. Surface water THg and MeHg were similar between lakes and seasonally dynamic, but water profiles exhibited elevated concentrations in the meta- and hypolimnion, highlighting water column MeHg production. Seston MeHg concentrations were often highest at shoulder seasons, possibly owing to metalimnetic MeHg delivery, but also differences in biomass and water clarity. The ∆199Hg and δ202Hg values in seston were similar between lakes, despite differing sediment THg concentrations and values, suggesting a shared bioaccumulated source of MeHg. Measurement of MeHg stable isotopes further elucidated that seston and fish predominantly bioaccumulated pelagic-sourced MeHg.

Wisconsin

Sulfate reduction drives elevated methylmercury formation in water column of eutrophic freshwater lake

Mercury (Hg) contamination of aquatic food webs is controlled in part by the formation and accumulation of toxic and bioaccumulative methylmercury (MeHg). MeHg production is mediated by metabolically diverse microorganisms carrying the hgcAB gene pair, while the demethylation reaction is mediated by several biotic and abiotic processes. However, the relative importance of these two processes on MeHg accumulation and the environmental factors that influence them are poorly characterized, especially in eutrophic environments. In this study, both Hg methylation and MeHg demethylation in a eutrophic freshwater lake were linked to ambient MeHg concentrations and hgcA abundance and expression. High methylation rate potentials indicated in situ MeHg formation was a key source of MeHg to the water column, driven by high hgcA abundance and transcription. Molybdate treatment decreased methylation rate potentials, highlighting the importance of sulfate reduction in driving MeHg formation. Sulfate-reducing bacteria accounted for over 50% of the hgcA gene transcription, despite representing less than 10% of the hgcA -carrying microbial community. An arsR -like transcriptional regulator preceded many hgcA sequences; these were transcriptionally active and linked to lower hgcA expression. Overall, this study elucidates the microbial and biogeochemical processes that influence the in situ formation of MeHg in understudied eutrophic freshwater environments.

Wisconsin

Using mercury and lead stable isotopes to assess mercury, lead, and trace metal source contributions to Great Salt Lake, Utah, USA

Great Salt Lake is a critical habitat for migratory birds that is threatened by elevated metal concentrations, including mercury (Hg) and lead (Pb), and is subject to severe hydrologic changes, such as declining lake level. When assessing metal profiles recorded in Great Salt Lake sediment, a large data gap exists regarding the sources of metals within the system, which is complicated by various source inputs to the lake and complex biogeochemistry. Here, we leverage Hg and Pb stable isotopes to track relative changes in metal source contributions to Great Salt Lake over time. Mercury and Pb concentrations increase in sediments deposited after 1920 and peak between 1965 and 1995, following closure of several local smelters and the onset of increased emission controls. The nominal associations above are confirmed via Hg stable isotopes in pre-1920 background sediments, which reflect atmospheric inputs from regional and global origin, whereas Hg and Pb stable isotopes together indicate that elevated metal concentrations in mid-late 20th century sediments reflect increased mining/smelting inputs. The observed minimal rebound towards pre-1920 Pb isotope signatures in 21st century sediments indicates that mining/smelting inputs, though reduced, remain a primary source of Pb to Great Salt Lake. In contrast, the more pronounced rebound of Hg stable isotope signatures to pre-1920 values indicate a greater contribution of atmospheric inputs of regional/global origin to current Hg inputs, though Hg concentrations are ∼10 times greater than pre-1920 background values due to global increases in atmospheric Hg concentrations or possibly slow recovery from local contamination. The importance of regional/global Hg sources to the system suggests that reductions in Hg bioaccumulation in the open water food webs of Great Salt Lake are more dependent on national and global reductions in Hg emissions and management strategies to limit methylmercury production within system. This work highlights the utility of using coupled Hg and Pb stable isotope values to assess trace metal pollution sources and pathways in aquatic systems.

Utah

Competition between dissolved organic matter and freshwater plankton control methylmercury isotope fractionation during uptake and photochemical demethylation

Isotope fractionation related to photochemical reactions and planktonic uptake at the base of the food web is a major uncertainty in the biological application of mercury (Hg) stable isotopes. In freshwater systems, it is unclear how competitive interactions among methylmercury (MeHg), dissolved organic matter (DOM), and phytoplankton govern the magnitude of mass-dependent and mass-independent fractionation. This study investigated how DOM alters rates of planktonic MeHg uptake and photodegradation and corresponding Hg isotope fractionation in the presence of freshwater phytoplankton species, Raphidocelis subcapitata . Outdoor sunlight exposure experiments utilizing R. subcapitata were performed in the presence of different DOM samples using environmentally relevant ratios of MeHg-DOM thiol groups. The extent of Δ 199 Hg in phytoplankton incubations (2.99‰ St. Louis River HPOA, 1.88‰ Lake Erie HPOA) was lower compared to paired abiotic control experiments (4.29 and 2.86‰, respectively) after ∼30 h of irradiation, resulting from cell shading or other limiting factors reducing the extent of photodemethylation. Although the Δ 199 Hg/Δ 201 Hg ratio was uniform across experiments (∼1.4), Δ 199 Hg/δ 202 Hg slopes varied dramatically (from −0.96 to 15.4) across incubations with R. subcapitata and DOM. In addition, no evidence of Hg isotope fractionation was observed within R. subcapitata cells. This study provides a refined examination of Hg isotope fractionation markers for key processes occurring in the lower food web prior to bioaccumulation, critical for accurately accounting for the photochemical processing of Hg isotopes across a wide spectrum of freshwater systems.

ACS Earth and Space Chemistry