The role of dissolved organic carbon in the chemistry and bioavailability of mercury in remote Adirondack lakes

A number of recent studies have documented elevated concentrations of mercury (Hg) in fish caught in remote lakes and a pattern of increased concentrations of Hg in fish tissue with decreasing water column pH. Because of the potential linkage between fish Hg and surface water acidification, factors regulating water column concentrations and bioavailability of Hg were investigated in Adirondack lakes through a field study and application of the Mercury Cycling Model (MCM). Concentrations of total Hg and total MeHg were highly variable, with concentrations of total MeHg about 10% of total Hg in lakes which did not show anoxic conditions. In lakes exhibiting anoxic conditions in the hypolimnion during summer stratification, concentrations of total MeHg were elevated. Concentrations of total Hg and total MeHg increased with decreasing pH in remote Adirondack lakes. However, more importantly, concentrations of total Hg and total MeHg increased with increasing concentrations of dissolved organic carbon (DOC) and percent near-shore wetlands in the drainage basin. Mercury concentrations in muscle tissue of yellow perch from Adirondack lakes were elevated above the U.S. FDA action level (1 μg/g Hg) in 7% of the fish sampled or in one or more individual fish from 9 of the 16 lakes sampled. Fish Hg concentrations generally increased with increasing fish length, weight and age. Patterns of increasing Hg concentration with age likely reflect shifts in prey of yellow perch and the bioconcentration of Hg along the food chain. For age 3 to 5 perch, concentrations of Hg increased with increasing concentrations of DOC and percent near-shore wetlands in the drainage basin. However, for a lake with very high DOC concentrations, fish concentrations of Hg declined. Calculations with the MCM also show that concentrations of Hg species increase with increasing DOC due to complexation reactions. Increases in DOC result in increasing concentrations of Hg in biota but decreases in the bioconcentration factor of Hg in fish tissue. This research suggests that DOC is important in the transport of Hg to lake systems. High concentrations of DOC may complex MeHg, diminishing its bioavailability. At high concentrations of monomeric Al, the complexation of MeHg with DOC apparently decreases, enhancing the bioavailability of MeHg.