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Mercury (Hg) concentrations and speciation were measured in nine tributaries to Lake Ontario as part of two independent field-sampling programs. Among the study tributaries, mean total Hg (THg) concentrations ranged from 0.9 to 2.6 ng/L; mean dissolved Hg (THg D ) ranged from 0.5 to 1.5 ng/L; mean particulate Hg (THg P ) ranged from 0.3 to 2.0 ng/L; and mean methylmercury (MeHg) ranged from 0.06 to 0.14 ng/L. Watershed land cover, total suspended solids (TSS), and dissolved organic carbon (DOC) were evaluated as potential controls of tributary Hg. Significant relationships between THg D and DOC were limited, whereas significant relationships between THg P and TSS were common across watersheds. Total suspended solids was strongly correlated with the percentage of agricultural land in watersheds. Particle enrichment of Hg (mass Hg/mass TSS) was highly variable, but distinctly higher in US tributaries likely due to higher TSS in Canadian tributaries associated with higher urban and agricultural land cover. MeHg was largely associated with the aqueous phase, and MeHg as a fraction of THg was positively correlated to percent open water coverage in the watershed. Wetland cover was positively correlated to THg and MeHg concentrations, while urban land cover was only related to higher THg P .

Rates of surface-air elemental mercury (Hg(0)) fluxes in the literature were synthesized for the Great Lakes Basin (GLB). For the majority of surfaces, fluxes were net positive (evasion). Digital land-cover data were combined with representative evasion rates and used to estimate annual Hg(0) evasion for the GLB (7.7 Mg/yr). This value is less than our estimate of total Hg deposition to the area (15.9 Mg/yr), suggesting the GLB is a net sink for atmospheric Hg. The greatest contributors to annual evasion for the basin are agricultural (∼55%) and forest (∼25%) land cover types, and the open water of the Great Lakes (∼15%). Areal evasion rates were similar across most land cover types (range: 7.0-21.0 μg/m(2)-yr), with higher rates associated with urban (12.6 μg/m(2)-yr) and agricultural (21.0 μg/m(2)-yr) lands. Uncertainty in these estimates could be partially remedied through a unified methodological approach to estimating Hg(0) fluxes., (Copyright © 2011 Elsevier Ltd. All rights reserved.)

Data from 104 sediment cores from the Great Lakes and "inland lakes" in the region were compiled to assess historical and recent changes in mercury (Hg) deposition. The lower Great Lakes showed sharp increases in Hg loading c. 1850-1950 from point-source water dischargers, with marked decreases during the past half century associated with effluent controls and decreases in the industrial use of Hg. In contrast, Lake Superior and inland lakes exhibited a pattern of Hg loading consistent with an atmospheric source - gradual increases followed by recent (post-1980) decreases. Variation in sedimentary Hg flux among inland lakes was primarily attributed to the ratio of watershed area:lake area, and secondarily to a lake's proximity to emission sources. A consistent region-wide decrease (∼20%) of sediment-Hg flux suggests that controls on local and regional atmospheric Hg emissions have been effective in decreasing the supply of Hg to Lake Superior and inland lakes., (Copyright © 2011 Elsevier Ltd. All rights reserved.)