Reconsidering mercury sources and exposure pathways to bivalves: Insights from mercury stable isotopes.

Identifying mercury (Hg) sources and exposure pathways to bivalves, particularly in relation to sediment, is important for expanding the utility of bivalves as a monitoring organism for sediment quality. Here we use Hg isotope ratios to decipher Hg sources accumulated into bivalves by conducting field studies and in situ experiments. In the first part of this study, we characterized Hg isotope ratios in individual geochemical fractions of riverine sediment, contaminated by liquid Hg in South Korea (Hyeongsan River; HS). Asian clams (Corbicula fluminea) were then deployed at the contaminated sites to evaluate the isotopic turnover. Over the two-month period, the isotope ratios of the clams shifted toward the labile/exchangeable Hg pools (F1, F2 fractions) of the sediment. Conversely, in the control site where sediment Hg is low, we observed similar Hg isotope ratios between Asian clams and the samples of precipitation and dissolved phase of water column. In East Fork Poplar Creek, (Oak Ridge) U.S., Asian clams also displayed similar Hg isotope ratios with the dissolved phase of water column, which have undergone substantial in-stream processing or input from Hg-contaminated groundwater from the hyporheic zones and riparian tributary during high hydrologic flow seasons. Our study demonstrates that the dissolved Hg phases within the water column, whether originating via sediment diffusion or derived externally, act as the primary source and exposure pathways to bivalves. The results of our study also shed new light to the prior Hg isotope measurement in bivalves collected from estuarine, lake, and coastal systems, which showed significant isotopic deviation from bulk sediment. The fact that bivalves are sensitive to in situ and external dissolved Hg phases provides additional insight into the existing biomonitoring program, which uses bivalves as a bioindicator for sediment quality.