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Atmospheric Environment 42 (2008) 6088– 6097

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Atmospheric Environment 42 (2008) 6088– 6097 ARTICLE IN PRESS Atmospheric Environment 42 (2008) 6088– 6097 Contents lists available at ScienceDirect Atmospheric Environment journal homepage: www.elsevier.com/locate/atmosenv Local to regional emission sources affecting mercury fluxes to New York lakes$ Revital Bookman a,Ã, Charles T. Driscoll a, Daniel R. Engstrom b, Steven W. Effler c a Department of Civil and Environmental Engineering, Syracuse University, 151 Link Hall, Syracuse, NY 13244, USA b St. Croix Watershed Research Station, Science Museum of Minnesota, Marine on St. Croix, MN 55047, USA c Upstate Freshwater Institute, P.O. Box 506, Syracuse, NY 13214, USA article info abstract Article history: Lake-sediment records across the Northern Hemisphere show increases in atmospheric Received 19 December 2007 deposition of anthropogenic mercury (Hg) over the last 150 years. Most of the previous Received in revised form studies have examined remote lakes affected by the global atmospheric Hg reservoir. In 4 March 2008 this study, we present Hg flux records from lakes in an urban/suburban setting of central Accepted 7 March 2008 New York affected also by local and regional emissions. Sediment cores were collected from the Otisco and Skaneateles lakes from the Finger Lakes region, Cross Lake, a Keywords: hypereutrophic lake on the Seneca River, and Glacial Lake, a small seepage lake with a Mercury watershed that corresponds with the lake area. Sediment accumulation rates and dates 210Pb dating were established by 210Pb. The pre-anthropogenic regional atmospheric Hg flux was Atmospheric deposition À2 À1 Sediment cores estimated to be 3.0 mgm yr from Glacial Lake, which receives exclusively direct Northeastern US atmospheric deposition. Mercury fluxes peaked during 1971–2001, and were 3 to more than 30 times greater than pre-industrial deposition. Land use change and urbanization in the Otisco and Cross watersheds during the last century likely enhanced sediment loads and Hg fluxes to the lakes. Skaneateles and Glacial lakes have low sediment accumulation rates, and thus are excellent indicators for atmospheric Hg deposition. In these lakes, we found strong correlations with emission records for the Great Lakes region that markedly increased in the early 1900s, and peaked during WWII and in the early 1970s. Declines in modern Hg fluxes are generally evident in the core records. However, the decrease in sediment Hg flux at Glacial Lake was interrupted and has increased since the early 1990s probably due to the operation of new local emission sources. Assuming the global Hg reservoir tripled since the pre-industrial period, the contribution of local and regional emission sources to central New York lakes was estimated to about 80% of the total atmospheric Hg deposition. & 2008 Elsevier Ltd. All rights reserved. 1. Introduction Mercury (Hg) contamination is pervasive in aquatic $ This is contribution No. 254 of the Upstate Freshwater Institute. We ecosystems and has potential severe health consequences dedicate this paper to our colleague and principal investigator Geoffrey O. Seltzer who was a great scholar and person. He will be missed by the for wildlife and humans (United States Environmental Earth Sciences community. Protection Agency, 1997; National Academy of Sciences, Ã Corresponding author. Currently at: Leon H. Charney School for 2000). Both direct point source pollution and atmospheric Marine Sciences, University of Haifa, Haifa 31905, Israel. emissions have been historically important in delivering Tel.: +972 4 8288131. Hg to water bodies. Their relative influence is proportional E-mail addresses: [email protected] (R. Bookman), [email protected] (C.T. Driscoll), [email protected] (D.R. Engstrom), to the Hg load emitted to the atmosphere or discharged sweffl[email protected] (S.W. Effler). to water, and the proximity to the pollution sources 1352-2310/$ - see front matter & 2008 Elsevier Ltd. All rights reserved. doi:10.1016/j.atmosenv.2008.03.045 ARTICLE IN PRESS R. Bookman et al. / Atmospheric Environment 42 (2008) 6088–6097 6089 (Iverfeldt, 1991; Keeler et al., 1994). The main sources for 210Pb dated lacustrine cores. Most previous studies on Hg atmospheric Hg emissions, since the onset of the deposition in lakes have been conducted in relatively Industrial Revolution are medical waste incineration, remote locations affected by the global long distance municipal waste combustion, metal smelting, chlor-alkali transport Hg reservoir or in urban lakes affected by direct facilities, and coal combustion for electricity generation. discharges and highly developed watersheds (Swain et al., These sources contribute to contemporary Hg deposition 1992; Engstrom et al., 1994; Lorey and Driscoll, 1999; in New York state and originate from emissions from the Engstrom and Swain, 1997; Pirrone et al., 1998; Kamman state (9–25%), the contiguous United States (25–50%) and and Engstrom, 2002; Perry et al., 2005; Lamborg et al., Asia, the largest contributing continent other than North 2002a, b; Balogh et al., 1999). In this research, we studied America (11–20%; Seigneur et al., 2003). The first attempt four lakes influenced by different watershed character- to control effectively industrial emissions in the United istics, ranging from an agriculture and urban disturbed States started with the 1970 Amendments of the Clean Air watershed to a lake with almost no watershed area which Act (Driscoll et al., 2001). Over the past 35 years a variety receives Hg inputs directly from the atmosphere. of Hg emission sources have been controlled through the Clean Air Act. In addition, discussions are underway on 2. Site descriptions controls of Hg emissions from electric utilities, the largest currently unregulated source (United States Environmen- The lakes selected for this study are located in central tal Protection Agency, 2005; Driscoll et al., 2007). New York (Fig. 1). The lakes, Otisco, Skaneateles, Glacial, Anthropogenic emissions to the atmosphere occur as and Cross, are part of the Seneca River watershed that elemental Hg (Hg0), reactive gaseous Hg (RGM), and drains about 8960 km2 to the Oswego River, and subse- particulate Hg (Hg )(Mason et al., 1994). The predomi- (p) quently Lake Ontario. They exhibit a wide range of nant form of atmospheric Hg is Hg0, with an atmospheric watershed and limnological characteristics (Table 1), but lifetime of about 0.5–1 year (Schroeder and Munthe, are all hardwater alkaline systems. Land cover of the 1998). In this form, Hg is well mixed hemispherically, and watersheds has changed over the last two centuries. The can be considered a global pollutant (Fitzgerald et al., first settlers in the region established agricultural com- 1998). Oxidized Hg associated with gases or aerosols has a munities and by the 19th century most of the forestland shorter lifetime of a few days to a few weeks, and was cleared. In the last century agriculture has diminished generally impacts local to regional areas (Olmez et al., greatly, the forested area has recovered, and urban areas 1998; Ames et al., 1998). In the northeast US in 2002, the have developed further (Bloomfield, 1978). major emission sources are municipal waste combustion Skaneateles Lake and Otisco Lake are the eastern most (23%) and utility coal burners (16%) (Northeast States for of the Finger Lakes. They occupy long narrow glacial- Coordinated Air Use Management, 2005). Mercury also origin basins positioned in a north–south direction can be directly discharged to aquatic ecosystems from (Bloomfield, 1978). Both lakes are used for water supply; direct point sources, which under certain circumstances their watersheds are under land protection programs. can dominate the atmospheric inputs (e.g., Glass et al., Mercury inputs are from direct atmospheric deposition to 1990; Bloom and Effler, 1990). the surface of the lakes as well as export from their Mercury that is deposited to the lake’s watershed can be watersheds. Cross Lake is a culturally hypereutrophic lake subsequently transported to the lake. Mercury accumula- characterized by high nutrient content and productivity. tion in the lake depends on the ratio of the watershed to The lake is located on the Seneca River, which contributes lake surface area (Swain et al., 1992), and on variations in approximately 98% of its inflow. The river receives both sediment accumulation rates (Engstrom et al., 1994). The agricultural runoff and municipal wastewater discharge, processes regulating retention and release of Hg in soils and is high in suspended solids (Effler et al., 2004). Cross and wetlands can influence the Hg transport from the Lake receives atmospheric Hg inputs, but is undoubtedly watershed (Lorey and Driscoll, 1999), and cause significant also impacted by land use and wastewater discharge in inputs to a lake long after the actual deposition (Yang et al., the watershed. Glacial is a meromictic seepage lake, 2002). Once in the lake-watershed, Hg can follow several located in the Clark Reservation State Park southeast of pathways: reduction and subsequent evasion to the atmo- the city of Syracuse (Effler et al., 1981). The watershed of sphere, methylation and/or demethylation, soil phase the lake is approximately equal to the lake surface area particle scavenging and retention, and transport with and it has no outlet. Mercury inputs to the lake are almost drainage water (Watras et al., 1994). Methylation of Hg entirely derived from direct atmospheric deposition. This and subsequent transport to surface waters is a health lake is critically important
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