Elevated levels of neurotoxic methylmercury in Arctic food-webs pose health risks for indigenous populations that consume large quantities of marine mammals and fish. Estuaries provide critical hunting and fishing territory for these populations, and, until recently, benthic sediment was thought to be the main methylmercury source for coastal fish. New hydroelectric developments are being proposed in many northern ecosystems, and the ecological impacts of this industry relative to accelerating climate changes are poorly characterized. Here we evaluate the competing impacts of climate-driven changes in northern ecosystems and reservoir flooding on methylmercury production and bioaccumulation through a case study of a stratified sub-Arctic estuarine fjord in Labrador, Canada. Methylmercury bioaccumulation in zooplankton is higher than in midlatitude ecosystems. Direct measurements and modeling show that currently the largest methylmercury source is production in oxic surface seawater. Water-column methylation is highest in stratified surface waters near the river mouth because of the stimulating effects of terrestrial organic matter on methylating microbes. We attribute enhanced biomagnification in plankton to a thin layer of marine snow widely observed in stratified systems that concentrates microbial methylation and multiple trophic levels of zooplankton in a vertically restricted zone. Large freshwater inputs and the extensive Arctic Ocean continental shelf mean these processes are likely widespread and will be enhanced by future increases in water-column stratification, exacerbating high biological methylmercury concentrations. Soil flooding experiments indicate that near-term changes expected from reservoir creation will increase methylmercury inputs to the estuary by 25-200%, overwhelming climate-driven changes over the next decade. mercury | plankton | estuary | biomagnification | hydroelectric reservoir

Open ocean samples of phytoplankton and zooplankton were collected from the central Pacific on board the R/V Kilo Moana in October of 2011. The cruise traveled from Hawaii to Samoa, progressing through a High Nutrient Low Chlorophyll (HNLC) zone, and an equatorial upwelling region. Phytoplankton samples were size fractioned into 0.2-5 μm, 5-20 μm, and N 20 μm samples. Methylmercury concentrations were 2.91 ± 2.58 pmol g −1 (wet weight) for the overall b200 μm size fractions, and highest around the HNLC region. Phytoplankton bioconcentration factors (logBCFs) averaged to 5.69 ± 0.98 and were higher than the values found for coastal regions. Both %MeHg ([MeHg]/[Hg]) and logBCF values indicated that the lowest size fraction had the largest fraction of the HgT as MeHg, signifying enhanced accumulation of MeHg into smaller organisms. Zooplankton vertical net tows were completed from depths of 200 m up to~10 m. Zooplankton samples were analyzed for carbon, nitrogen and sulfur in addition to Hg and MeHg at size fractionations of 0.2-0.5 mm, 0.5-1.0 mm, 1.0-2.0 mm and occasionally N 2.0 mm. Zooplankton abundance and MeHg concentrations both peaked at Stations 3 and 5 (upwelling region). The %MeHg in the organisms was highest in the N2.0 mm size class, displaying MeHg bioaccumulation for increasing zooplankton sizes. Separate day and night net tows were collected at Stations 3 and 5 in order to investigate differences due to diurnal migration of zooplankton. There were higher concentrations of MeHg for all sizes in night collections of zooplankton at Station 5, but no discrepancy for Station 3. These results represent some of the few measurements of Hg and MeHg at the base of the open ocean food chain, and are significant as they represent the instigation of bioconcentration into the base of marine food webs.

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Abstract.In an effort to understand and quantify the impact of local, regional, and far-distant atmospheric mercury sources to rainfall mercury deposition in the Pensacola, Florida watershed, a program of event-based rainfall sampling was started in late 2004. Modified Aerochem-Metrics wet/dry rainfall samplers were deployed at three sites in the region around the Crist coal-fired power plant and eventbased samples were collected continuously for three years. Samples were analyzed for total Hg and a suite of trace elements including Al, As, Ba, Bi, Cd, Ce, Co, Cr, Cs, Cu, Fe, Ga, La, Li, Mg, Mn, Na, Nb, Ni, P, Pb, Sb, Se, Si, Sn, Sr, Th, U, V, and Zn. Nutrients (ammonia and nitrate) and major anions (chloride and sulfate) were also measured on each sample. Multivariate statistical methods were used to sort these tracers into factors that represent potential source categories contributing to the rainfall chemistry. As, Hg, Sb, Se, Sn, and non sea-salt sulfate were all significantly correlated (R>0.6) with one factor which we interpret as an anthropogenic source term reflecting input from coal combustion throughout the southeastern US. Using ratios of total Hg to volatile elements, we estimate that 22-33% of the rainfall Hg results from coal combustion in the southeastern US with the majority coming from the global background.

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