New tools for a legacy problem: How isotope tracers inform area of concern actions in the St. Louis River in Lake Superior.

Numerous mercury (Hg) sources can contribute to biological burdens within the Great Lakes, including atmospheric deposition (e.g., precipitation), non-point source land runoff (e.g., watershed), and legacy contamination. Due to these different environmental entry points, it is often difficult to ascertain if legacy Hg contamination contributes to contemporary fish consumption advisories within Areas of Concern (AOCs), as designated by the United States-Canada Great Lakes Water Quality Agreement. In this study, we aimed to assess the contributions of legacy Hg to sediments in nearshore wetland habitats and co-located prey items (dragonfly larvae and yellow perch) within the St. Louis River AOC using Hg stable isotopes. We observed that nearshore sediments had the same Hg source portfolio as previously examined main channel sites. Furthermore, this data confirmed that two major Hg sources were contributing to sediments within nearshore regions of the St. Louis River AOC: legacy and watershed Hg. The contribution of legacy Hg was estimated in biota and demonstrated that up to 64% of the Hg in fish tissue in the lower estuary (St. Louis Bay) was from legacy sources, but that this percentage declined substantially when examining upstream regions of the AOC. These data indicate the influence of legacy Hg to the food web varies spatially within the St. Louis River. We further found that watershed Hg sources are an important Hg contributor to the St. Louis River, which likely applies to other impacted and unimpacted tributaries across the Great Lakes region.