Suspect and Nontarget Screening Revealed Class-Specific Temporal Trends (2000-2017) of Poly- and Perfluoroalkyl Substances in St. Lawrence Beluga Whales.

The global use of >3000 per- and polyfluoroalkyl substances (PFASs) has given rise to chemical regulatory action. However, limited information exists regarding current and historical emissions for the majority of PFASs under currently implemented regulations. This study employed suspect and nontarget screening to examine the temporal trends of legacy and unregulated PFASs in liver of the endangered beluga whale () population from the St. Lawrence Estuary in Canada collected from 2000 to 2017. A suite of 54 PFASs were tentatively identified, and were grouped into nine structurally distinct classes. Single-hydrogenated perfluoro carboxylic acids (H-PFCAs), single-hydrogenated sulfonamides (H-Sulfonamides), as well as other select sulfonamides were detected for the first time in wildlife. Greater concentrations of the majority of PFASs were determined in newborns and juveniles than in adults, suggesting effective placental and lactational transfer of PFASs. Legacy per- and polyfluoroalkyl acids and perfluorooctane sulfonamide in beluga whale liver were found to significantly decrease in concentration between 2000 and 2017, while unregulated short-chain PFAS alternatives, H-PFCAs, and odd-chain FTCAs were found to increase over time. The implementation of suspect and nontarget screening revealed class-specific temporal trends of PFASs in SLE beluga whales, and supported continuous emissions of unregulated PFASs into the environment.