Spatiotemporal variations, sources and health risk assessment of perfluoroalkyl substances in a temperate bay adjacent to metropolis, North China

Fourteen perfluoroalkyl substances (PFASs) in fishery organism, surface seawater, river water, rainwater, and wastewater samples collected from Jiaozhou Bay (JZB) in China and its surrounding area were determined to understand their contamination status, sources, health risk, and causes of spatiotemporal variations in the aquatic environment of a temperate bay adjacent to a metropolis. The total concentration of PFASs in 14 species of fishery organisms ranged from 1.77 ng/g to 31.09 ng/g wet weight, and perfluorooctane sulfonate (PFOS) was the dominant PFAS. ∑PFASs concentration in surface seawater ranged from 5.54 ng/L to 48.27 ng/L over four seasons, and dry season (winter and spring) had higher levels than wet season (summer and autumn). Perfluorooctanoic acid (PFOA) was the predominant individual PFAS in seawater, indicating that notorious C8 homologs remained the major PFASs in this region. The seasonal variation in seawater concentrations of three major PFASs, namely, PFOA, perfluoroheptanoic acid, and perfluorononanoic acid, was similar to that of ∑PFASs. However, the seasonal variation of PFOS concentration was different from that of ∑PFASs, with the lowest in winter and the highest in spring. In general, seasonal variations of terrigenous input and water exchange capacity were the main reasons for the spatiotemporal variation of PFASs in the aquatic environment of JZB. Moreover, bioselective enrichment for individual PFAS affected the partition of PFASs in different environment medium. Wet precipitation, sewage discharge, and surface runoff were the main sources of PFASs in this area. Nevertheless, the contribution of different sources to individual PFAS indicated a clear difference, and wastewater and river water were not consistently the most important source for every PFAS. Preliminary risk assessment revealed that the consumption of seafood, especially fish, from JZB might pose a certain extent of health risk to local consumers based on their estimated daily intake of PFASs.