Emission Changes Dwarf the Influence of Feeding Habits on Temporal Trends of Per- and Polyfluoroalkyl Substances in Two Arctic Top Predators.

We monitored concentrations of per- and polyfluoroalkyl substances (PFASs) in relation to climate-associated changes in feeding habits and food availability in polar bears (Ursus maritimus) and arctic foxes (Vulpes lagopus) (192 plasma and 113 liver samples, respectively) sampled from Svalbard, Norway, during 1997-2014. PFASs concentrations became greater with increasing dietary trophic level, as bears and foxes consumed more marine as opposed to terrestrial food, and as the availability of sea ice habitat increased. Long-chained perfluoroalkyl carboxylates (PFCAs) in arctic foxes decreased with availability of reindeer carcasses. The ∼9-14% yearly decline of C perfluoroalkyl sulfonates (PFSAs) following the cease in C PFSA precursor production in 2001 indicates that the peak exposure was mainly a result of atmospheric transport of the volatile precursors. However, the stable PFSA concentrations since 2009-2010 suggest that Svalbard biota is still exposed to ocean-transported PFSAs. Long-chain ocean-transported PFCAs increased 2-4% per year and the increase in C PFCAs in polar bears tended to level off since ∼2009. Emerging short-chain PFASs showed no temporal changes. Climate-related changes in feeding habits and food availability moderately affected PFAS trends. Our results indicate that PFAS concentrations in polar bears and arctic foxes are mainly affected by emissions.