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Abstract Methylmercury (MeHg) production is controlled by the bioavailability of inorganic divalent mercury (Hg(II) i ) and Hg‐methylation capacity of the microbial community (conferred by the hgcAB gene cluster). However, the relative importance of these factors and their interaction in the environment remain poorly understood. Here, metagenomic sequencing and a full‐factorial MeHg formation experiment were conducted across a wetland sulfate gradient with different microbial communities and pore water chemistries. From this experiment, the relative importance of each factor on MeHg formation was isolated. Hg(II) i bioavailability correlated with the dissolved organic matter composition, while the microbial Hg‐methylation capacity correlated with the abundance of hgcA genes. MeHg formation responded synergistically to both factors. Notably, hgcA sequences were from diverse taxonomic groups, none of which contained genes for dissimilatory sulfate reduction. This work expands our understanding of the geochemical and microbial constraints on MeHg formation in situ and provides an experimental framework for further mechanistic studies. 

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. 

High levels of methylmercury accumulation in marine biota are a concern throughout the Arctic, where coastal ocean ecosystems received large riverine inputs of mercury (Hg) (40 Mg⋅y −1 ) and sediment (20 Tg⋅y −1 ) during the last decade, primarily from major Russian rivers. Hg concentrations in fish harvested from these rivers have declined since the late 20th century, but no temporal data on riverine Hg, which is often strongly associated with suspended sediments, were previously available. Here, we investigate temporal trends in Russian river particulate Hg (PHg) and total suspended solids (TSS) to better understand recent changes in the Arctic Hg cycle and its potential future trajectories. We used 1,300 measurements of Hg in TSS together with discharge observations made by Russian hydrochemistry and hydrology monitoring programs to examine changes in PHg and TSS concentrations and fluxes in eight major Russian rivers between ca. 1975 and 2010. Due to decreases in both PHg concentrations (micrograms per gram) and TSS loads, annual PHg export declined from 47 to 7 Mg⋅y −1 overall and up to 92% for individual rivers. Modeling of atmospheric Hg deposition together with published inventories on reservoir establishment and industrial Hg release point to decreased pollution and sedimentation within reservoirs as predominant drivers of declining PHg export. We estimate that Russian rivers were the primary source of Hg to the Arctic Ocean in the mid to late 20th century.