Abstract
Methylmercury is a potent neurotoxin that accumulates in aquatic food webs. Human activities, including industry and mining, have increased inorganic mercury inputs to terrestrial and aquatic ecosystems. Methylation of this mercury generates methylmercury, and is thus a public health concern. Marine methylmercury is a particular concern in the Arctic, where indigenous peoples rely heavily on marine-based diets. In the summer, atmospheric inorganic mercury concentrations peak in the Arctic, whereas they reach a minimum in the northern mid-latitudes. Here, we use a global three-dimensional ocean–atmosphere model to examine the cause of this Arctic summertime maximum. According to our simulations, circumpolar rivers deliver large quantities of mercury to the Arctic Ocean during summer; the subsequent evasion of this riverine mercury to the atmosphere can explain the summertime peak in atmospheric mercury levels. We infer that rivers are the dominant source of mercury to the Arctic Ocean on an annual basis. Our simulations suggest that Arctic Ocean mercury concentrations could be highly sensitive to climate-induced changes in river flow, and to increases in the mobility of mercury in soils, for example as a result of permafrost thaw and forest fires.
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References
Steffen, A., Schroeder, W., Macdonald, R., Poissant, L. & Konoplev, A. Mercury in the Arctic atmosphere: An analysis of eight years of measurements of GEM at Alert (Canada) and a comparison with observations at Amderma (Russia) and Kuujjuarapik (Canada). Sci. Total Environ. 342, 185–198 (2005).
Berg, T., Aspmo, K. & Steinnes, E. Transport of Hg from Atmospheric mercury depletion events to the mainland of Norway and its possible influence on Hg deposition. Geophys. Res. Lett. 35, L09802 (2008).
Cole, A. S. & Steffen, A. Trends in long-term gaseous mercury observations in the Arctic and effects of temperature and other atmospheric conditions. Atmos. Chem. Phys. 10, 4661–4672 (2010).
Selin, N. E. et al. Chemical cycling and deposition of atmospheric mercury: Global constraints from observations. J. Geophys. Res. 112, D02308 (2007).
Steffen, A. et al. A synthesis of atmospheric mercury depletion event chemistry in the atmosphere and snow. Atmos. Chem. Phys. 8, 1445–1482 (2008).
Ariya, P. A. et al. The Arctic: A sink for mercury. Tellus B 56, 397–403 (2004).
Lindberg, S. E. et al. Dynamic oxidation of gaseous mercury in the Arctic troposphere at polar sunrise. Environ. Sci. Tech. 36, 1245–1256 (2002).
Hirdman, D. et al. Transport of mercury in the Arctic atmosphere: Evidence for a spring- time net sink and summer-time source. Geophys. Res. Lett. 36, L12814 (2009).
Kirk, J. L., St. Louis, V. L. & Sharp, M. J. Rapid reduction and reemission of mercury deposited into snowpacks during atmospheric mercury depletion events at Churchill, Manitoba, Canada. Environ. Sci. Tech. 40, 7590–7596 (2006).
Aspmo, K. et al. Mercury in the atmosphere, snow and melt water ponds in the North Atlantic Ocean during Arctic summer. Environ. Sci. Tech. 40, 4083–4089 (2006).
Sommar, J., Andersson, M. E. & Jacobi, H-W. Circumpolar measurements of speciated mercury, ozone and carbon monoxide in the boundary layer of the Arctic Ocean. Atmos. Chem. Phys. 10, 5031–5045 (2010).
Andersson, M., Sommar, J., Gårdfeldt, K. & Lindqvist, O. Enhanced concentrations of dissolved gaseous mercury in the surface waters of the Arctic Ocean. Mar. Chem. 110, 190–194 (2008).
Holmes, C. D. et al. Global atmospheric model for mercury including oxidation by bromine atoms. Atmos. Chem. Phys. 10, 12037–12057 (2010).
Soerensen, A. L. et al. An improved global model for air–sea exchange of mercury: High concentrations over the North Atlantic. Environ. Sci. Tech. 44, 8574–8580 (2010).
Bullock, O. R. Jr et al. The North American Mercury Model Intercomparison Study (NAMMIS): Study description and model-to-model comparisons. J. Geophys. Res. 113, D17310 (2008).
Task Force on Hemispheric Transport of Air Pollution. Hemispheric Transport of Air Pollution 2010 Part B: Mercury. (Economic Commission for Europe, 2010).
Steen, A. et al. Natural and anthropogenic atmospheric mercury in the European Arctic: A fractionation study. Atmos. Chem. Phys. 11, 6273–6284 (2011).
Durnford, D. & Dastoor, A. The behavior of mercury in the cryosphere:A review of what we know from observations. J. Geophys. Res. 116, D06305 (2011).
Poulain, A. J. et al. Redox transformations of mercury in an Arctic snowpack at springtime. Atmos. Environ. 38, 6763–6774 (2004).
De Boyer Montégut, C., Madec, G., Fischer, A. S., Lazar, A. & Iudicone, D. Mixed layer depth over the global ocean: An examination of profile data and a profile-based climatology. J. Geophys. Res. 109, C12003 (2004).
Toole, J. M. et al. Influences of the ocean surface mixed layer and thermohaline stratification on Arctic Sea ice in the central Canada Basin. J. Geophys. Res. 115, C10018 (2010).
Sunderland, E. M. & Mason, R. P. Human impacts on open ocean mercury concentrations. Glob. Biogeochem. Cy. 21, GB4022 (2007).
Kirk, J. L. et al. Methylated mercury species in marine waters of the Canadian high and sub Arctic. Environ. Sci. Tech. 42, 8367–8373 (2008).
Poulain, A. J. et al. Potential for mercury reduction by microbes in the high arctic. Appl. Environ. Microb. 73, 2230–2238 (2007).
Amyot, M., Gill, G. A. & Morel, F. M. M. Production and loss of dissolved gaseous mercury in coastal seawater. Environ. Sci. Tech. 31, 3606–3611 (1997).
Vörösmarty, C. J., Fekete, B. M., Meybeck, M. & Lammers, R. B. Global system of rivers: Its role in organizing continental land mass and defining land-to-ocean linkages. Glob. Biogeochem. Cy. 14, 599–621 (2000).
Dittmar, T. & Kattner, G. The biogeochemistry of the river and shelf ecosystem of the Arctic Ocean: A review. Mar. Chem. 83, 103–120 (2003).
Grigal, D. Mercury sequestration in forests and peatlands: A review. J. Environ. Qual. 32, 393–405 (2003).
Leitch, D. R. et al. The delivery of mercury to the Beaufort Sea of the Arctic Ocean by the Mackenzie River. Sci. Total Environ. 373, 178–195 (2007).
Coquery, M., Cossa, D. & Martin, J. The distribution of dissolved and particulate mercury in three Siberian estuaries and adjacent Arctic coastal waters. Wat. Air Soil Pollut. 80, 653–664 (1995).
Outridge, P., Macdonald, R., Wang, F., Stern, G. & Dastoor, A. A mass balance inventory of mercury in the Arctic Ocean. Environ. Chem. 5, 89–111 (2008).
Shiklomanov, A. I. & Lammers, R. B. Record Russian river discharge in 2007 and the limits of analysis. Environ. Res. Lett. 4, 045015 (2009).
Schuster, P. F. et al. Mercury export from the Yukon River basin and potential response to a changing climate. Environ. Sci. Tech. 45, 9262–9267 (2011).
Walling, D. & Webb, B. Estimating the discharge of contaminants to coastal waters by rivers: Some cautionary comments. Mar. Pollut. Bull. 16, 488–492 (1985).
Lantuit, H. Fifty years of coastal erosion and retrogressive thaw slump activity on Herschel Island, southern Beaufort Sea, Yukon Territory, Canada. Geomorphology 95, 84–102 (2008).
Atkinson, D. E. Observed storminess patterns and trends in the circum-Arctic coastal regime. Geo.-Mar. Lett. 25, 98–109 (2005).
Leitch, D. R. Mercury Distribution in Water and Permafrost of the Lower Mackenzie Basin, Their Contribution to the Mercury Contamination in the Beaufort Sea Marine Ecosystem, and Potential Effects of Climate Variation Master of Science thesis, Univ. Manitoba (2006).
Rachold, V. et al. in The Organic Carbon Cycle in the Arctic Ocean (eds Stein, R. & Macdonald, R.) Ch. 2, 33–55 (Springer, 2004).
Graydon, J. A., Emmerton, C. A., Lesack, L. F. W. & Kelly, E. N. Mercury in the Mackenzie River delta and estuary: Concentrations and fluxes during open-water conditions. Sci. Total Environ. 407, 2980–2988 (2009).
Rydberg, J., Klaminder, J., Rosén, P. & Bindler, R. Climate driven release of carbon and mercury from permafrost mires increases mercury loading to sub-arctic lakes. Sci. Total Environ. 408, 4778–4783 (2010).
Turetsky, M. R. et al. Wildfires threaten mercury stocks in northern soils. Geophys. Res. Lett. 33, L16403 (2006).
Reynolds, R. W., Rayner, N. A., Smith, T. M., Stokes, D. C. & Wang, W. An improved in situ and satellite SST analysis for climate. J. Clim. 15, 1609–1625 (2002).
Amos, H. A. et al. Gas-particle partitioning of atmospheric Hg(II) and its effect on global mercury deposition. Atmos. Chem. Phys. 12, 591–603 (2012).
Pöhler, D., Vogel, L., Frieß, U. & Platt, U. Observation of halogen species in the Amundsen Gulf, Arctic, by active long-path differential optical absorption spectroscopy. Proc. Natl Acad. Sci. USA 107, 6582–6587 (2010).
Prados-Roman, C. et al. Airborne DOAS limb measurements of tropospheric trace gas profiles: Case studies on the profile retrieval of O4 and BrO. Atmos. Meas. Tech. 4, 1241–1260 (2011).
Dommergue, A. et al. The fate of mercury species in a sub-arctic snowpack during snowmelt. Geophys. Res. Lett. 30, 1621 (2003).
Weiss-Penzias, P., Jaffe, D. A., McClintick, A., Prestbo, E. M. & Landis, M. S. Gaseous elemental mercury in the marine boundary layer: Evidence for rapid removal in anthropogenic pollution. Environ. Sci. Tech. 37, 3755–3763 (2003).
Sigler, J. M., Mao, H. & Talbot, R. Gaseous elemental and reactive mercury in Southern New Hampshire. Atmos. Chem. Phys. 9, 1929–1942 (2009).
Yatavelli, R. L. N. et al. Mercury, PM2.5 and gaseous co-pollutants in the Ohio River Valley region: Preliminary results from the Athens supersite. Atmos. Environ. 40, 6650–6665 (2006).
Fekete, B. M., Vörösmarty, C. J. & Grabs, W. Global, composite runoff fields based on observed river discharge and simulated water balances. (Univ. New Hampshire and Global Runoff Data Centre, 2000).
Acknowledgements
This work was financially supported by the Arctic System Science Program of the US National Science Foundation. Financial support for the Alert and Amderma data sets was provided by the Northern Contaminants Program, Environment Canada and the Arctic Monitoring and Assessment Programme. We thank A. Cole for providing the Alert data; A. Konoplev and F. Pankratov at SPA Typhoon in Obninsk, Russia for providing the Amderma data; K. A. Pfaffhuber, T. Berg and the Chemical Co-ordinating Centre of EMEP for providing the Zeppelin data; and E. Corbitt and C. Holmes for helpful conversations.
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J.A.F. designed, performed and interpreted the model simulations. D.J.J. and E.M.S. supervised the research and contributed significantly to interpretation of the results. A.L.S. and H.M.A. developed major components of the model. A.S. collected the Alert data. J.A.F. wrote the paper, and all authors edited and revised the paper.
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Fisher, J., Jacob, D., Soerensen, A. et al. Riverine source of Arctic Ocean mercury inferred from atmospheric observations. Nature Geosci 5, 499–504 (2012). https://doi.org/10.1038/ngeo1478
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DOI: https://doi.org/10.1038/ngeo1478
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