Abstract

AbstractElevated biological concentrations of methylmercury (MeHg), a bioaccumulative neurotoxin, are observed throughout the Arctic Ocean, but major sources and degradation pathways in seawater are not well understood. We develop a mass budget for mercury species in the Arctic Ocean based on available data since 2004 and discuss implications and uncertainties. Our calculations show that high total mercury (Hg) in Arctic seawater relative to other basins reflect large freshwater inputs and sea ice cover that inhibits losses through evasion. We find that most net MeHg production (20 Mg a−1) occurs in the subsurface ocean (20–200 m). There it is converted to dimethylmercury (Me2Hg: 17 Mg a−1), which diffuses to the polar mixed layer and evades to the atmosphere (14 Mg a−1). Me2Hg has a short atmospheric lifetime and rapidly degrades back to MeHg. We postulate that most evaded Me2Hg is redeposited as MeHg and that atmospheric deposition is the largest net MeHg source (8 Mg a−1) to the biologically productive surface ocean. MeHg concentrations in Arctic Ocean seawater are elevated compared to lower latitudes. Riverine MeHg inputs account for approximately 15% of inputs to the surface ocean (2.5 Mg a−1) but greater importance in the future is likely given increasing freshwater discharges and permafrost melt. This may offset potential declines driven by increasing evasion from ice‐free surface waters. Geochemical model simulations illustrate that for the most biologically relevant regions of the ocean, regulatory actions that decrease Hg inputs have the capacity to rapidly affect aquatic Hg concentrations.

Highlights

  • Accumulation of methylmercury (MeHg) in Arctic biota is a major concern for the health of northern populations that consume large quantities of marine foods [Arctic Monitoring and Assessment Programme (AMAP), 2011a; Riget et al, 2011b]

  • Our five-box geochemical model for the Arctic Ocean includes compartments representing (1) the upper 20 m of the water column known as the polar mixed layer (PML) defined based on an observed density gradient of 0.01 kg mÀ3 [Toole et al, 2010] and consistent with previous model representations [Fisher et al, 2012; Fisher et al, 2013]; (2) the subsurface ocean that extends to the bottom on the shelf and to 200 m depth in the Central Arctic Basin and Baffin Bay [Pickard and Emery, 1990]; (3) the deep ocean below 200 m to the sea floor in the central Basin and Baffin Bay; (4) active sediment layers on the shelf (2 cm) and in the Central Basin (1 cm)

  • We have developed a five-box biogeochemical model for the Arctic Ocean to gain insight into processes and timescales driving changes in MeHg concentrations in the Arctic Ocean

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Summary

Introduction

Accumulation of methylmercury (MeHg) in Arctic biota is a major concern for the health of northern populations that consume large quantities of marine foods [Arctic Monitoring and Assessment Programme (AMAP), 2011a; Riget et al, 2011b]. We use available measurement data since 2004 to construct Arctic Ocean mass budgets for Hg and MeHg and gain insight into processes driving MeHg concentrations in Arctic Ocean seawater. MeHg is produced from divalent inorganic Hg (HgII) by bacteria in benthic sediment and in the water column [Lehnherr, 2014]. It is produced in freshwater ecosystems and wetlands and transported by rivers into the surface ocean [Nagorski et al, 2014]. We force the model with changes in sea ice since 1975 and modeled anthropogenic Hg deposition between 1850 and 2010 We use this analysis to gain insight into processes affecting MeHg concentrations in Arctic Ocean biota and timescales of response associated with. We develop hypotheses about key biogeochemical processes that can be tested in future research and discuss major uncertainties and data gaps

Model Overview
Hydrologic and Solids Budget
Mercury Reservoirs
Mercury Fluxes
Biochemical Transformations
Total Hg Budget
Methylated Hg Species Budget
Response to Global Change and Anthropogenic Emissions
Summary and Conclusion
Limitations and Uncertainties
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