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1. Large subglacial source of mercury from the southwestern margin of the Greenland Ice Sheet

   https://doi.org/10.1038/s41561-021-00753-w  

   Hawkings, Jon R.; Linhoff, Benjamin S.; Wadham, Jemma L.; Stibal, Marek; Lamborg, Carl H.; Carling, Gregory T.; Lamarche-Gagnon, Guillaume; Kohler, Tyler J.; Ward, Rachael; Hendry, Katharine R.; et al (July 2021, Nature Geoscience)

   Abstract The Greenland Ice Sheet is currently not accounted for in Arctic mercury budgets, despite large and increasing annual runoff to the ocean and the socio-economic concerns of high mercury levels in Arctic organisms. Here we present concentrations of mercury in meltwaters from three glacial catchments on the southwestern margin of the Greenland Ice Sheet and evaluate the export of mercury to downstream fjords based on samples collected during summer ablation seasons. We show that concentrations of dissolved mercury are among the highest recorded in natural waters and mercury yields from these glacial catchments (521–3,300 mmol km −2 year −1 ) are two orders of magnitude higher than from Arctic rivers (4–20 mmol km −2 year −1 ). Fluxes of dissolved mercury from the southwestern region of Greenland are estimated to be globally significant (15.4–212 kmol year −1 ), accounting for about 10% of the estimated global riverine flux, and include export of bioaccumulating methylmercury (0.31–1.97 kmol year −1 ). High dissolved mercury concentrations (~20 pM inorganic mercury and ~2 pM methylmercury) were found to persist across salinity gradients of fjords. Mean particulate mercury concentrations were among the highest recorded in the literature (~51,000 pM), and dissolved mercury concentrations in runoff exceed reported surface snow and ice values. These results suggest a geological source of mercury at the ice sheet bed. The high concentrations of mercury and its large export to the downstream fjords have important implications for Arctic ecosystems, highlighting an urgent need to better understand mercury dynamics in ice sheet runoff under global warming. 

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2. Mercury source changes and food web shifts alter contamination signatures of predatory fish from Lake Michigan

   https://doi.org/10.1073/pnas.1907484116  

   Lepak, Ryan F.; Hoffman, Joel C.; Janssen, Sarah E.; Krabbenhoft, David P.; Ogorek, Jacob M.; DeWild, John F.; Tate, Michael T.; Babiarz, Christopher L.; Yin, Runsheng; Murphy, Elizabeth W.; et al (November 2019, Proceedings of the National Academy of Sciences)

   To understand the impact reduced mercury (Hg) loading and invasive species have had on methylmercury bioaccumulation in predator fish of Lake Michigan, we reconstructed bioaccumulation trends from a fish archive (1978 to 2012). By measuring fish Hg stable isotope ratios, we related temporal changes in Hg concentrations to varying Hg sources. Additionally, dietary tracers were necessary to identify food web influences. Through combined Hg, C, and N stable isotopic analyses, we were able to differentiate between a shift in Hg sources to fish and periods when energetic transitions (from dreissenid mussels) led to the assimilation of contrasting Hg pools (2000 to present). In the late 1980s, lake trout δ 202 Hg increased (0.4‰) from regulatory reductions in regional Hg emissions. After 2000, C and N isotopes ratios revealed altered food web pathways, resulting in a benthic energetic shift and changes to Hg bioaccumulation. Continued increases in δ 202 Hg indicate fish are responding to several United States mercury emission mitigation strategies that were initiated circa 1990 and continued through the 2011 promulgation of the Mercury and Air Toxics Standards rule. Unlike archives of sediments, this fish archive tracks Hg sources susceptible to bioaccumulation in Great Lakes fisheries. Analysis reveals that trends in fish Hg concentrations can be substantially affected by shifts in trophic structure and dietary preferences initiated by invasive species in the Great Lakes. This does not diminish the benefits of declining emissions over this period, as fish Hg concentrations would have been higher without these actions. 

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3. Expanded Phylogenetic Diversity and Metabolic Flexibility of Mercury-Methylating Microorganisms

   https://doi.org/10.1128/mSystems.00299-20  

   McDaniel, Elizabeth A.; Peterson, Benjamin D.; Stevens, Sarah L.; Tran, Patricia Q.; Anantharaman, Karthik; McMahon, Katherine D. (August 2020, mSystems)

   Kent, Angela D. (Ed.)

   ABSTRACT Methylmercury is a potent bioaccumulating neurotoxin that is produced by specific microorganisms that methylate inorganic mercury. Methylmercury production in diverse anaerobic bacteria and archaea was recently linked to the hgcAB genes. However, the full phylogenetic and metabolic diversity of mercury-methylating microorganisms has not been fully unraveled due to the limited number of cultured experimentally verified methylators and the limitations of primer-based molecular methods. Here, we describe the phylogenetic diversity and metabolic flexibility of putative mercury-methylating microorganisms by hgcAB identification in publicly available isolate genomes and metagenome-assembled genomes (MAGs) as well as novel freshwater MAGs. We demonstrate that putative mercury methylators are much more phylogenetically diverse than previously known and that hgcAB distribution among genomes is most likely due to several independent horizontal gene transfer events. The microorganisms we identified possess diverse metabolic capabilities spanning carbon fixation, sulfate reduction, nitrogen fixation, and metal resistance pathways. We identified 111 putative mercury methylators in a set of previously published permafrost metatranscriptomes and demonstrated that different methylating taxa may contribute to hgcA expression at different depths. Overall, we provide a framework for illuminating the microbial basis of mercury methylation using genome-resolved metagenomics and metatranscriptomics to identify putative methylators based upon hgcAB presence and describe their putative functions in the environment. IMPORTANCE Accurately assessing the production of bioaccumulative neurotoxic methylmercury by characterizing the phylogenetic diversity, metabolic functions, and activity of methylators in the environment is crucial for understanding constraints on the mercury cycle. Much of our understanding of methylmercury production is based on cultured anaerobic microorganisms within the Deltaproteobacteria , Firmicutes , and Euryarchaeota. Advances in next-generation sequencing technologies have enabled large-scale cultivation-independent surveys of diverse and poorly characterized microorganisms from numerous ecosystems. We used genome-resolved metagenomics and metatranscriptomics to highlight the vast phylogenetic and metabolic diversity of putative mercury methylators and their depth-discrete activities in thawing permafrost. This work underscores the importance of using genome-resolved metagenomics to survey specific putative methylating populations of a given mercury-impacted ecosystem. 

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4. Bioinformatics Investigations of Universal Stress Proteins from Mercury-Methylating Desulfovibrionaceae

   https://doi.org/10.3390/microorganisms9081780  

   Isokpehi, Raphael D.; McInnis, Dominique S.; Destefano, Antoinette M.; Johnson, Gabrielle S.; Walker, Akimio D.; Hall, Yessenia A.; Mapp, Baraka W.; Johnson, Matilda O.; Simmons, Shaneka S. (August 2021, Microorganisms)

   null (Ed.)

   The presence of methylmercury in aquatic environments and marine food sources is of global concern. The chemical reaction for the addition of a methyl group to inorganic mercury occurs in diverse bacterial taxonomic groups including the Gram-negative, sulfate-reducing Desulfovibrionaceae family that inhabit extreme aquatic environments. The availability of whole-genome sequence datasets for members of the Desulfovibrionaceae presents opportunities to understand the microbial mechanisms that contribute to methylmercury production in extreme aquatic environments. We have applied bioinformatics resources and developed visual analytics resources to categorize a collection of 719 putative universal stress protein (USP) sequences predicted from 93 genomes of Desulfovibrionaceae. We have focused our bioinformatics investigations on protein sequence analytics by developing interactive visualizations to categorize Desulfovibrionaceae universal stress proteins by protein domain composition and functionally important amino acids. We identified 651 Desulfovibrionaceae universal stress protein sequences, of which 488 sequences had only one USP domain and 163 had two USP domains. The 488 single USP domain sequences were further categorized into 340 sequences with ATP-binding motif and 148 sequences without ATP-binding motif. The 163 double USP domain sequences were categorized into (1) both USP domains with ATP-binding motif (3 sequences); (2) both USP domains without ATP-binding motif (138 sequences); and (3) one USP domain with ATP-binding motif (21 sequences). We developed visual analytics resources to facilitate the investigation of these categories of datasets in the presence or absence of the mercury-methylating gene pair (hgcAB). Future research could utilize these functional categories to investigate the participation of universal stress proteins in the bacterial cellular uptake of inorganic mercury and methylmercury production, especially in anaerobic aquatic environments. 

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5. Climate-driven sulfate export in alpine watersheds may stimulate methylmercury production

   https://doi.org/10.1088/1748-9326/add8a5  

   Miller, Hannah_R; Driscoll, Charles_T; Janssen, Sarah_E; Hinckley, Eve-Lyn_S (May 2025, Environmental Research Letters)

   Abstract Climate change is increasing sulfate export and changing wetland extent in mountain regions. These changes may increase microbially mediated production of the neurotoxic substance methylmercury due to enhanced sulfate metabolism in mountain environments. Here, we assess methylmercury concentrations and formation rates across high-elevation wetlands in the Colorado Rocky Mountains. We also investigate sulfate controls on methylmercury production within subalpine peatlands by amending soils with sulfate to mimic increased stream export of sulfate from the alpine zone and measuring methylmercury formation rates for different sulfate treatments. We found that subalpine peatlands have statistically significant higher methylmercury concentrations and formation rates compared to alpine, mineral-soil wetlands. Methylmercury production in subalpine peatlands also increased significantly (p < 0.05) following sulfate additions; the highest rates occurred in sediments with intermediate extractable sulfate concentrations (~0.60–1.4 mg sulfate g-1 dry soil). Our study is the first to identify soil sulfate-related thresholds for methylmercury production and sulfate-limitation of methylmercury production in subalpine peatlands. These findings highlight important linkages between climate-driven mineral weathering and mercury cycling in mountain regions globally. 

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