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Temporal and spatial trends of 15 per- and polyfluoroalkyl substances (PFAS) were determined in white-tailed sea eagle (WTSE) eggs ( Haliaeetus albicilla ) from two inland and two coastal regions of Sweden between 1969 and 2021. PFAS concentrations generally increased from ∼1969 to ∼1990s-2010 (depending on target and site) and thereafter plateaued or declined, with perfluorooctane sulfonamide (FOSA) and perfluorooctane sulfonate (PFOS) declining faster than most perfluoroalkyl carboxylic acids (PFCAs). The net result was a shift in the PFAS profile from PFOS-dominant in 1969-2010 to an increased prevalence of PFCAs over the last decade. Further, during the entire period higher PFAS concentrations were generally observed in coastal populations, possibly due to differences in diet and/or proximity to more densely populated areas. Fluorine mass balance determination in pooled samples from three of the regions (2019-2021) indicated that target PFAS accounted for the vast majority ( i.e. 81-100%) of extractable organic fluorine (EOF). Nevertheless, high resolution mass-spectrometry-based suspect screening identified 55 suspects (31 at a confidence level [CL] of 1-3 and 24 at a CL of 4-5), of which 43 were substances not included in the targeted analysis. Semi-quantification of CL ≤ 2 suspects increased the identified EOF to >90% in coastal samples. In addition to showing the impact of PFAS regulation and phase-out initiatives, this study demonstrates that most extractable organofluorine in WTSE eggs is made up of known (legacy) PFAS, albeit with low levels of novel substances.

Twenty per- and polyfluoroalkyl substances (PFAS) were determined in human milk from residents of three Chinese cities (Shanghai, Jiaxing, and Shaoxing; [n = 10 individuals per city]), sampled between 2010 and 2016. These data were compared to a combination of new and previously reported PFAS concentrations in human milk from Stockholm, Sweden, collected in 2016 (n = 10 individuals). Across the three Chinese cities, perfluorooctanoate (PFOA; sum isomers), 9-chlorohexadecafluoro-3-oxanone-1-sulfonic acid (9Cl-PF3ONS; also known as 6:2 Cl-PFESA or by its trade name "F53-B"), and perfluorooctane sulfonate (PFOS; sum isomers) occurred at the highest concentrations among all PFAS (up to 411, 976, and 321 pg mL -1 , respectively), while in Stockholm, PFOA and PFOS were dominant (up to 89 and 72 pg mL -1 , respectively). 3H-Perfluoro-3-[(3-methoxy-propoxy)propanoic acid] (ADONA) was intermittently detected but at concentrations below the method quantification limit (i.e. <10 pg mL -1 ) in Chinese samples, and was non-detectable in Swedish milk. The extremely high concentrations of F53-B in Chinese milk suggest that human exposure assessments focused only on legacy substances may severely underestimate overall PFAS exposure in breastfeeding infants.