A mercury transport and fate model (LM2-Mercury) for mass budget assessment of mercury cycling in Lake Michigan

LM2-Mercury, a mercury mass balance model, was developed to simulate and evaluate the transport, fate, and biogeochemical transformations of mercury in Lake Michigan. The model simulates total suspended and resuspendable solids (TSRS), dissolved organic carbon (DOC), and total, elemental, divalent, and methylmercury as state variables. Simplified processes among the mercury state variables including net methylation, net reduction of divalent mercury, and reductive demethylation are incorporated in the model. Volatilization of elemental mercury as a kinetic (phase transfer) process and partitioning of total, divalent, and methylmercury as a set of instantaneous equilibrium processes were also simulated. The model was calibrated to data collected in 1994 and 1995 and corroborated by comparing model output generated from a long-term model hindcast to total mercury measured in high quality sediment profiles. Model hindcast predictions of total mercury in the water column were within estimates of total mercury calculated from observed lake trout bioaccumulation factors. Using the model, a mass budget assessment of mercury cycling in the lake was conducted. Atmospheric deposition, including wet and dry (particle) deposition and absorption of gaseous divalent mercury, was the dominant source of total mercury to the lake, followed by sediment resuspension, and then tributary loads. The major loss mechanism of total mercury from the water was associated with the settling of solids, followed by net volatilization. Methylmercury loading associated with wet deposition was the dominant source to the lake, followed by tributary loadings, and in situ net methylation.