title: Temporal Shifts in Poly- and Perfluoroalkyl Substances (PFASs) in North Atlantic Pilot Whales Indicate Large Contribution of Atmospheric Precursors.
abstract: Poly- and perfluoroalkyl substances (PFASs) are persistent, bioaccumulative anthropogenic compounds associated with adverse health impacts on humans and wildlife. PFAS production changed in North America and Europe around the year 2000, but impacts on wildlife appear to vary across species and location. Unlike other mammal species, cetaceans lack the enzyme for transforming an important intermediate precursor (perfluorooctane sulfonamide: FOSA), into a prevalent compound in most wildlife (perfluorooctanesulfonate: PFOS). Thus, their tissue burden differentiates these two compounds while other mammals contain PFOS from both direct exposure and precursor degradation. Here we report temporal trends in 15 PFASs measured in muscle from juvenile male North Atlantic pilot whales (Globicephala melas) harvested between 1986 and 2013. FOSA accounted for a peak of 84% of the 15 PFASs around 2000 but declined to 34% in recent years. PFOS and long-chained PFCAs (C9-C13) increased significantly over the whole period (2.8% yr-1to 8.3% yr-1), but FOSA declined by 13% yr-1after 2006. Results from FOSA partitioning and bioaccumulation modeling forced by changes in atmospheric inputs reasonably capture magnitudes and temporal patterns in FOSA concentrations measured in pilot whales. Rapid changes in atmospheric FOSA in polar and subpolar regions around 2000 helps to explain large declines in PFOS exposure for species that metabolize FOSA, including seafood consuming human populations. This work reinforces the importance of accounting for biological exposures to PFAS precursors.
authors.affiliation: Department of Environmental Health, Harvard T.H. Chan School of Public Health, Harvard University , Boston, Massachusetts 02115, United States.|Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University , Cambridge, Massachusetts 02138, United States.
authors.forename: Clifton
authors.identifier: 0000-0001-7140-1344
authors.initials: C
authors.lastname: Dassuncao
authors.affiliation: Department of Environmental Health, Harvard T.H. Chan School of Public Health, Harvard University , Boston, Massachusetts 02115, United States.|Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University , Cambridge, Massachusetts 02138, United States.
authors.forename: Xindi C
authors.identifier: 0000-0002-4299-3931
authors.initials: XC
authors.lastname: Hu
authors.affiliation: Department of Environmental Health, Harvard T.H. Chan School of Public Health, Harvard University , Boston, Massachusetts 02115, United States.|Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University , Cambridge, Massachusetts 02138, United States.
authors.forename: Xianming
authors.identifier: 0000-0002-5301-7899
authors.initials: X
authors.lastname: Zhang
authors.affiliation: Department of Environmental Science, Aarhus University, Arctic Research Centre (ARC) , Frederiksborgvej 399, PO Box 358, DK-4000 Roskilde, Denmark.
authors.forename: Rossana
authors.initials: R
authors.lastname: Bossi
authors.affiliation: Environment Agency , PO Box 2048, FO-165 Argir, Faroe Islands.
authors.forename: Maria
authors.initials: M
authors.lastname: Dam
authors.affiliation: Museum of Natural History , Tórshavn, Faroe Islands.
authors.forename: Bjarni
authors.initials: B
authors.lastname: Mikkelsen
authors.affiliation: Department of Environmental Health, Harvard T.H. Chan School of Public Health, Harvard University , Boston, Massachusetts 02115, United States.|Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University , Cambridge, Massachusetts 02138, United States.
authors.forename: Elsie M
authors.initials: EM
authors.lastname: Sunderland
mesh_terms: D000293:Adolescent; D017738:Alkanesulfonic Acids; D000818:Animals; D004784:Environmental Monitoring; D005466:Fluorocarbons; D006801:Humans; D013449:Sulfonamides; D014874:Water Pollutants, Chemical; D050686:Whales, Pilot
chemical_list: D017738:Alkanesulfonic Acids; D005466:Fluorocarbons; D013449:Sulfonamides; D014874:Water Pollutants, Chemical