Investigating Methylmercury Exposure in North Atlantic Cetaceans Using Multiple Isotope Tracers

Anthropogenic emissions have substantially perturbed the global biogeochemical cycle of mercury (Hg) and high latitude ecosystems are particularly vulnerable to Hg pollution and climate change. We investigated temporal changes in methylmercury (MeHg) exposures of long-finned pilot whales (Globicephala melas, n=59) between 1985-2015 using multiple isotopes (δ202Hg, Δ199Hg, Δ200Hg, Δ201Hg, δ13C, δ15N) as tracers of the physical environment and foraging ecology. Mass-independent fraction (MIF) of Hg (Δ199Hg, Δ201Hg) is mainly driven by photochemical demethylation in seawater. Enriched δ202Hg has been shown to result from demethylation. The ranges in Δ199Hg and Δ201Hg values in whales are similar across time periods with the exception of a few years following the 2010 volcanic eruption in Iceland that may have affected light penetration in surface waters. The mean δ202Hg values of whale muscle samples are consistently 1.5 ‰ across the study period, which is 1 ‰ higher than their prey (squid, blue whiting, and greater argentine). This fractionation is consistent with in vivo demethylation as a detoxification mechanism in the whales. Individuals with the highest MeHg concentrations have the lowest δ202Hg values and we infer this may result from more limited MeHg demethylation. We find a linear relationship between Δ200Hg anomalies (-0.1 to 0.2‰) and Δ199Hg (R2=0.76) that has not previously been reported. Variability in Δ200Hg is thought to be driven by photochemical reactions in the tropopause and may provide an effective tracer for atmospheric Hg inputs to the ocean that are methylated and accumulated in aquatic biota.