Fate of elemental mercury in the Arctic during atmospheric mercury depletion episodes and the load of atmospheric mercury to the Arctic.
ABSTRACT 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.
Environmental Chemistry. 01/2010; 7(6):537-547.
Article: Global concentrations of gaseous elemental mercury and reactive gaseous mercury in the marine boundary layer.[show abstract] [hide abstract]
ABSTRACT: Gaseous elemental mercury (GEM) and reactive gaseous mercury (RGM) were measured during an eight month circumnavigation to obtain knowledge of their worldwide distributions in the marine boundary layer (MBL). Background GEM concentrations were found to be 1.32 ± 0.2 ng/m(3) (summer) and 2.62 ± 0.4 ng/m(3) (spring) in the northern hemisphere and 1.27 ± 0.2 ng/m(3) (spring and summer) in the southern hemisphere. Radiation and relative humidity are shown to control diurnal cycles of RGM. During the cruise the ship passed areas of clean MBL air, air influenced by biomass burning (South Atlantic) and air with high concentrations of GEM and RGM of unknown origin (Antarctic). High GEM concentrations above the Atlantic indicate that emission from the ocean can be an important GEM source. Our data combined with data from earlier cruises provides adequate information to establish a seasonal cycle for the Atlantic. Results show a cycle similar to that found at Mace Head, Ireland but with larger amplitude. We have improved the basic knowledge of mean GEM and RGM concentrations in the MBL worldwide and shown how natural sources and reemissions can affect GEM concentrations in the MBL.Environmental Science & Technology 10/2010; 44(19):7425-30. · 4.80 Impact Factor
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ABSTRACT: Polar regions are subject to contamination by mercury (Hg) transported from lower latitudes, severely impacting human and animal health. Atmospheric Mercury Depletion Events (AMDEs) are an episodic process by which Hg is transferred from the atmospheric reservoir to arctic snowpacks. The fate of Hg deposited during these events is the subject of numerous studies, but its speciation remains unclear, especially in terms of environmentally relevant forms such as bioavailable mercury (BioHg). Here, using a bacterial mer-lux biosensor, we report the fraction of newly deposited Hg at the surface and at the bottom of the snowpack that is bioavailable. Snow samples were collected over a two-month arctic field campaign in 2008. In surface snow, BioHg is related to atmospheric Hg deposition and snow fall events were shown to contribute to higher proportions of BioHg than AMDEs. Based on our data, AMDEs represent a potential source of 20 t.y(-1) of BioHg, while wet and dry deposition pathways may provide 135-225 t.y(-1) of BioHg to Arctic surfaces.Environmental Science & Technology 02/2011; 45(6):2150-6. · 4.80 Impact Factor