Fate of Elemental Mercury in the Arctic during Atmospheric Mercury Depletion Episodes and the Load of Atmospheric Mercury to the Arctic

National Environmental Research Institute, Frederiksborgvej 399, 4000 Roskilde, Denmark.
Environmental Science and Technology (Impact Factor: 5.33). 05/2004; 38(8):2373-82. DOI: 10.1021/es030080h
Source: PubMed


Atmospheric mercury depletion episodes (AMDEs) were studied at Station Nord, Northeast Greenland, 81 degrees 36' N, 16 degrees 40' W, during the Arctic Spring. Gaseous elemental mercury (GEM) and ozone were measured starting from 1998 and 1999, respectively, until August 2002. GEM was measured with a TEKRAN 2735A automatic mercury analyzer based on preconcentration of mercury on a gold trap followed by detection using fluorescence spectroscopy. Ozone was measured by UV absorption. A scatter plot of GEM and ozone concentrations confirmed that also at Station Nord GEM and ozone are linearly correlated during AMDEs. The relationship between ozone and GEM is further investigated in this paper using basic reaction kinetics (i.e., Cl, ClO, Br, and BrO have been suggested as reactants for GEM). The analyses in this paper show that GEM in the Arctic troposphere most probably reacts with Br. On the basis of the experimental results of this paper and results from the literature, a simple parametrization for AMDE was included into the Danish Eulerian Hemispheric Model (DEHM). In the model, GEM is converted linearly to reactive gaseous mercury (RGM) over sea ice with temperature below -4 degrees C with a lifetime of 3 or 10 h. The new AMDE parametrization was used together with the general parametrization of mercury chemistry [Petersen, G.; Munthe, J.; Pleijel, K.; Bloxam, R.; Vinod Kumar, A. Atmos. Environ. 1998, 32, 829-843]. The obtained model results were compared with measurements of GEM at Station Nord. There was good agreement between the start and general features periods with AMDEs, although the model could not reproduce the fast concentration changes, and the correlation between modeled and measured values decreased from 2000 to 2001 and further in 2002. The modeled RGM concentrations over the Arctic in 2000 were found to agree well with the temporal and geographical variability of the boundary column of monthly average BrO observed by the GOME satellite. Scenario calculations were performed with and without AMDEs. For the area north of the Polar Circle, the mercury deposition increases from 89 tons/year for calculations without an AMDE to 208 tons/year with the AMDE. The 208 tons/year represent an upper limit for the mercury load to the Artic.

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    • "In the Arctic, atmospheric mercury depletion events (AMDEs) gained attention in the 1990s (Schroeder et al., 1998). These events commonly occurred during the spring in the polar coastal environments and were caused by photochemically initiated oxidation reactions that involved marine halogens (Lu et al., 2001; Lindberg et al., 2002; Skov et al., 2004) that transform GEM to RGM and PM (Faı¨n et al., 2008). The deposition of oxidised mercury results in a greater total mercury (THg) concentration in the snow and subsequently contributes to the contamination of the aquatic reservoir during snowmelt (Faı¨n et al., 2008). "
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    ABSTRACT: In this study, the concentrations of total mercury (THg) and ions deposited in the surface snow and snow pits in the eastern Antarctic along the 29th inland route of the Chinese National Antarctic Research Expedition were analysed. The THg concentrations in the surface snow ranged from 0.22 to 8.29 ng/L and elevated concentrations were detected in the inland regions of higher altitudes (3000-4000 m). The spatial distribution of the THg in the snow pits showed greater inland concentrations with mean concentrations of < 0.2-1.33 ng/L. The THg concentrations in the coastal snow pit (29-A) showed higher concentrations in the summer snow layers than in the winter snow layers. The THg records from the two inland snow pits (29-K and 29-L) spanned decades and indicated elevated THg concentrations between the late 1970s and early 1980s and during the mid-1990s. The temporal variations of THg in the Antarctic snow layers were consistent with anthropogenic emissions around the world. In addition, the Pinatubo volcanic eruption was the primary contributor to the 1992 THg peak that was observed in the inland snow pits.
    Tellus B 12/2014; 66(1). DOI:10.3402/tellusb.v66.25152 · 2.15 Impact Factor
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    • "Even after extensive regulations of anthropogenic Hg emissions over the past decades, Hg levels are increasing in Arctic seabirds and mammals (Braune et al., 2005; Riget et al., 2011; Dietz et al., 2013). Despite low emission in Arctic areas, an annual input of 90–450 metric tons of Hg from atmospheric deposition is estimated (Ariya et al., 2004; Skov et al., 2004). A large fraction is reemitted to the atmosphere, but still, a net input of Hg to Arctic ecosystems has been reported (Poissant et al., 2008). "
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    ABSTRACT: Hepatic concentrations of mercury (Hg), selenium (Se) and cadmium (Cd) were determined in black-legged kittiwakes (Rissa tridactyla) and little auks (Alle alle) from two fjords in Svalbard (Kongsfjorden; 78°57'N, 12°12'E and Liefdefjorden; 79°37'N, 13°20'E). The inflow of Arctic and Atlantic water differs between the two fjords, potentially affecting element accumulation. Trophic positions (TP) were derived from stable nitrogen isotope ratios (δ(15)N), and stable carbon isotope ratios (δ(13)C) were assessed to evaluate the terrestrial influence on element accumulation. Mercury, Cd, TP and δ(13)C varied significantly between locations and years in both species. Trophic position and feeding habits explained Hg and Cd accumulation in kittiwakes, but not in little auks. Biomagnification of Hg and Cd were found in the food webs of both the Atlantic and the Arctic fjord, and no inter-fjord differences were detected. The δ(13)C were higher in the seabirds from Kongsfjorden than in Liefdefjorden, but this did not explain variations in element accumulation. Selenium concentrations were not influenced by Hg accumulation in kittiwakes, indicating baseline levels of Se in this species. In contrast, correlations between Hg and Se and lower Se:Hg ratios in little auks from Kongsfjorden than in Liefdefjorden indicate a more pronounced influence of Se-Hg complex formation in little auks feeding in Atlantic waters. Copyright © 2014. Published by Elsevier Ltd.
    Chemosphere 11/2014; 122. DOI:10.1016/j.chemosphere.2014.10.060 · 3.34 Impact Factor
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    • "Atmospheric mercury depletion events arise from the rapid photo-oxidation of tropospheric Hg(0) catalyzed by halogen radicals in marine aerosols (Lindberg et al. 2002). Because AMDEs potentially result in the deposition of very large quantities of atmospheric Hg to polar regions, they have been the focus of intensive scientific investigation (Schroeder et al. 1998; Lindberg et al. 2002; Skov et al. 2004; Steffen et al. 2008; Berg et al. 2003; Gauchard et al. 2005). Early estimates of atmospheric Hg deposition to the Arctic ranged from 208 to 325 Mg year −1 , 20%–57% of which was attributed to AMDEs (Christensen et al. 2004; Ariya et al. 2004; Travnikov 2005). "
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    ABSTRACT: There has been increasing concern about mercury (Hg) levels in marine and freshwater organisms in the Arctic, due to the importance of traditional country foods such as fish and marine mammals to the diet of Northern Peoples. Due to its toxicity and ability to bioaccumulate and biomagnify in food webs, methylmercury (MeHg) is the form of Hg that is of greatest concern. The main sources of MeHg to Arctic aquatic ecosystems, the processes responsible for MeHg formation and degradation in the environment, MeHg bioaccumulation in Arctic biota and the human health implications for Northern Peoples are reviewed here. In Arctic marine ecosystems, Hg(II) methylation in the water column, rather than bottom sediments, is the primary source of MeHg, although a more quantitative understanding of the role of dimethylmercury (DMHg) as a MeHg source is needed. Because MeHg production in marine waters is limited by the availability of Hg(II), predicted increases in Hg(II) concentrations in oceans are likely to result in higher MeHg concentrations and increased exposure to Hg in humans and wildlife. In Arctic freshwaters, MeHg concentrations are a function of two antagonistic processes, net Hg(II) methylation in bottom sediments of ponds and lakes and MeHg photodemethylation in the water column. Hg(II) methylation is controlled by microbial activity and Hg(II) bioavailability, which in turn depend on interacting environmental factors (temperature, redox conditions, organic carbon, and sulfate) that induce nonlinear responses in MeHg production. Methylmercury bioaccumulation-biomagnification in Arctic aquatic food webs is a function of the MeHg reservoir in abiotic compartments, as well as ecological considerations such as food-chain length, growth rates, life-history characteristics, feeding behavior, and trophic interactions. Methylmercury concentrations in Arctic biota have increased significantly since the onset of the industrial age, and in some populations of fish, seabirds, and marine mammals toxicological thresholds are being exceeded. Due to the complex connection between Hg exposure and human health in Northern Peoples-arising from the dual role of country foods as both a potential Hg source and a nutritious, affordable food source with many physical and social health benefits--reductions in anthropogenic Hg emissions are seen as the only viable long-term solution.
    Environmental Reviews 01/2014; 22(3). DOI:10.1139/er-2013-0059 · 3.00 Impact Factor
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