Anthropogenic activities have been releasing mercury for centuries, and despite global efforts to control emissions, concentrations in environmental media remain high. Coastal sediments can be a long-term repository for mercury, but also a secondary source, and competing processes in marine ecosystems can lead to the conversion of mercury into the toxic and bioaccumulative species methylmercury, which threatens ecosystem and human health. We investigate the fate and transport of three mercury species in a coastal lagoon affected by historical pollution using a novel high-resolution finite element model that integrates mercury biogeochemistry, sediment dynamics and hydrodynamics. The model resolves mercury dynamics in the seawater and the seabed taking into account partitioning, transport driven by water and sediment, and photochemical and microbial transformations. We simulated three years (early 2000s, 2019, and 2020) to assess the spatio-temporal distribution of mercury species concentrations and performed a sensitivity analysis to account for uncertainties. The modeled mercury species concentrations show high temporal and spatial variability, with water concentrations in some areas of the lagoon exceeding those of the open Mediterranean Sea by two orders of magnitude, consistent with available observations from the early 2000s. The results support conclusions about the importance of different processes in shaping the environmental gradients of mercury species. Due to the past accumulation of mercury in the lagoon sediments, inorganic mercury in the water is closely related to the resuspension of contaminated sediments, which is significantly reduced by the presence of benthic vegetation. The gradients of methylmercury depend on the combination of several factors, of which sediment resuspension and mercury methylation are the most relevant. The results add insights into mercury dynamics at coastal sites characterized by a combination of past pollution (i.e. sediment enrichment) and erosive processes, and suggest possible nature-based mitigation strategies such as the preservation of the integrity of benthic vegetation and morphology.
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