Connecting tributary mercury loads to nearshore and offshore sediments in Lake Superior

Lake Superior has a vast and largely undeveloped watershed in comparison to the other Great Lakes, which makes it challenging to study mercury (Hg) sources and cycling. To examine Hg inputs to Lake Superior, we conducted an expansive binational assessment in 40 watersheds from a diverse range of landcover types. We further paired tributary Hg data to sediment source portfolios in the nearshore and offshore zones of Lake Superior through partnership with the Great Lakes Sediment Surveillance Program. We observed that total Hg loads were highest in the spring driven by the combination of elevated Hg concentrations and increased water discharge from snowmelt. In addition, total Hg concentrations in tributaries from remote, heavily forested regions, such as Pukaskwa National Park and the Minnesota Northshore, were higher than the Southshore and Thunder Bay regions. Methylmercury concentrations and loads were more spatially dependent, often corresponding to regions with more wetlands (e.g., Michigan Upper Peninsula). We estimated that the total Hg tributary load to Lake Superior in 2021 was 126 kg per year. To further examine the fate of watershed Hg sources, we examined sediments from 28 sites in Lake Superior using Hg stable isotopes. At open water sites, precipitation was the primary Hg source to sediments, but within nearshore sites Hg originated predominantly from watershed runoff. This work further defines the sources and fate of Hg within Lake Superior and highlights how Hg delivery is intrinsically tied to varying hydrologic regimes.