A North American and global survey of perfluoroalkyl substances in surface soils: Distribution patterns and mode of occurrence

Abstract

The distribution of 32 per/polyfluoroalkyl substances (PFASs) in surface soils was determined at 62 locations representing all continents (North America n = 33, Europe n = 10, Asia n = 6, Africa n = 5, Australia n = 4, South America n = 3 and Antarctica n = 1) using ultra performance liquid chromatography tandem mass spectrometry (UPLC-MS/MS) systems. Quantifiable levels of perfluoroalkyl carboxylates (PFCAs: PFHxA-PFTeDA) were observed in all samples with total concentrations ranging from 29 to 14,300 pg/g (dry weight), while perfluoroalkane sulfonates (PFSAs: PFHxS, PFOS and PFDS) were detected in all samples but one, ranging from <LOQ-3270 pg/g, confirming the global distribution of PFASs in terrestrial settings. The geometric mean PFCA and PFSA concentrations were observed to be higher in the northern hemisphere (930 and 170 pg/g) compared to the southern hemisphere (190 and 33 pg/g). Perfluorooctanoate (PFOA) and perfluorooctanesulfonate (PFOS) were the most commonly detected analytes at concentrations up to 2670 and 3100 pg/g, respectively. The sum of PFCA homologues of PFOA commonly were roughly twice the concentration of PFOA. The PFCA and PFSA congener profiles were similar amongst most locations, with a few principal-component statistical anomalies suggesting impact from nearby urban and point sources. The ratio of even to odd PFCAs was consistent with the atmospheric oxidation of fluorotelomer-based precursors previously observed in laboratory and environmental studies. Given the soils were collected from locations absent of direct human activity, these results suggest that the atmospheric long-range transport (LRT) of neutral PFASs followed by oxidation and deposition are a significant source of PFCAs and PFSAs to soils.