Aquatic Ecosystem Exposure Associated with Atmospheric Mercury Deposition: Importance of Watershed and Water Body Hot Spots and Hot Moments

Atmospheric deposition of divalent mercury (Hg(II)) is the often the primary driving force for mercury contamination in fish tissue, resulting in mercury exposure to wildlife and humans. In lake systems associated with small watersheds, direct deposition to the water surface is typically the dominant mercury loading source; however, in lake systems with large watersheds and river systems, these inputs may be relatively small compared to loadings from the watershed via erosion and surface runoff. Within each system, transformation of the deposited mercury into the environmentally relevant form, methylmercury (MeHg), proceeds at different rates largely regulated by physical characteristics such as watershed land use types and water body hydraulic residence times, as water body chemistry, such as pH and trophic status Therefore, to fully represent mercury exposure in aquatic ecosystems, we must couple watershed models with water body models and explore where, why, and when hot spots and hot moments of transformation and transport occur. Here we link the simulated atmospheric mercury deposition results from the Community Multi-Scale Air Quality (CMAQ) model, a spatially distributed grid-based watershed mercury (Hg) model (GBMM), and the Water Quality Analysis Simulation Program (WASP). We use this multi-media modeling framework to simulate mercury species cycling over time for the different river reaches and watersheds within the Cape Fear River Basin, North Carolina. Through these simulations we investigate the importance of specific watershed and surface water system characteristics in simulating MeHg exposure concentrations. Because GBMM is a spatially-distributed model we are able to investigate the importance of such factors (i.e., watershed area, land-use types, and land-use percentages) in transporting and transforming deposited mercury. We present how particular land-use types and land-use change influence total loading and total mercury concentrations, how different hydrological transport and transformation characteristics impact MeHg exposure, and how these relate spatially ("hot spots") and temporally ("hot moments").