Spatial distribution and source tracing of per- and polyfluoroalkyl substances (PFASs) in surface water in Northern Europe * Minh A. Nguyen * , Karin Wiberg, Erik Ribeli, Sarah Josefsson, Martyn Futter, Jakob Gustavsson, Lutz Ahrens Department of Aquatic Sciences and Assessment, Swedish University of Agricultural Sciences (SLU), Box 7050, SE-75007 Uppsala, Sweden article info Article history: Received 10 June 2016 Received in revised form 21 September 2016 Accepted 29 October 2016 Available online xxx Keywords: Per- and polyfluoroalkyl substances (PFASs) Source tracing Long-range atmospheric transport Surface water abstract The impact of point and diffuse sources for 26 per- and polyfluoroalkyl substances (PFASs) in northern Europe were investigated by studying Swedish rivers (n ¼ 40) and recipient seawater (Baltic Sea and Kattegat; n ¼ 18). Different composition profiles were observed in the rivers, with ten rivers having a remarkably high fraction of perfluoroalkane sulfonic acids (PFSAs; 65% of the ƩPFASs) as compared to other rivers (19%) suggesting major impact of one or several source types dominated by PFSAs. Popu- lation density and low latitude (south) were strongly correlated to the widely used per- fluorooctanesulfonic acid (PFOS), perfluorooctanoic acid (PFOA) as well as to perfluorohexanesulfonic acid (PFHxS). Significant relationships between several PFCAs and PFSAs (i.e. perfluorobutanoic acid (PFBA), perfluoroheptanoic acid (PFHpA), PFOA, perfluorobutanesulfonic acid (PFBS), and PFHxS) and dissolved organic carbon (DOC) were detected (p < 0.05), indicating chemical binding and co-transport with DOC in fresh water and seawater. Partial least squares regression analysis showed that per- fluoroalkyl carboxylic acids (PFCAs) were related to latitude according to their perfluorocarbon chain length (C 3 ,C 7 ,C 8 ,C 9 ,C 10 and C 11 ), with longer chains associated with higher latitudes. This suggests the presence of mechanisms promoting higher prevalence of longer chained PFCAs in the north, e.g. pre- cursor degradation, and/or aerosol associated stabilization of PFCAs and their precursors. © 2016 Elsevier Ltd. All rights reserved. 1. Introduction Per- and polyfluoroalkyl substances (PFASs) are synthetic chemicals of concern due to their extreme persistence and high bioaccumulative potential (Giesy et al., 2010; Martin et al., 2003). Some PFASs are potentially carcinogenic and endocrine disrupting chemicals (EDCs), and their toxicity depends on functional group and perfluorocarbon chain length (Ulhaq et al., 2013a; Ulhaq et al., 2013b). PFASs have both hydrophobic and hydrophilic properties and are used as surfactants in e.g. textiles, carpets, leather, paper products, and fire-fighting foams (Ahrens et al., 2009a; Swedish EPA, 2006). They can be emitted from point sources (e.g. fire- fighting training sites, sewage treatment plants (STPs)) (Ahrens et al., 2015; Becker et al., 2008) or derive from diffuse sources (e.g. atmospheric deposition, run-off) (Kim and Kannan, 2007; Taniyasu et al., 2013), and can undergo long-range transport to remote areas through atmosphere and water currents (Ahrens et al., 2009a; Ahrens et al., 2015; Becker et al., 2008; Davis et al., 2007; Paul et al., 2009; Prevedouros et al., 2006; Shoeib et al., 2006). As a consequence, PFASs are ubiquitously distributed in the abiotic environment, wildlife and humans (Giesy and Kannan, 2001; Yamashita et al., 2008; Yeung et al., 2008). Concerns for human health and environmental effects have led to bans or re- strictions of the use of some PFASs. For example, PFOS has been listed as a persistent organic pollutant (POP) under the Stockholm Convention since 2009 (UNEP, 2006), and PFOA and PFNA and their salts have been added to the candidate list of substances of very high concern for authorisation by the European chemicals agency (ECHA) since 2013 and 2015 (ECHA, 2013, 2015), respectively. The occurrence of PFASs has been studied in rivers and lakes in Europe (Loos et al., 2010; Munoz et al., 2015; M€ oller et al., 2010) with detected concentrations up to 1400 ng L 1 (Krka River in Slovenia) (Loos et al., 2009). PFASs in surface waters are eventually transported from land to the sea (McLachlan et al., 2007). One of the most contaminated seas globally is the semi-enclosed Baltic Sea * This paper has been recommended for acceptance by von Hippel Frank A. * Corresponding author. E-mail address: anh.minh.nguyen@slu.se (M.A. Nguyen). Contents lists available at ScienceDirect Environmental Pollution journal homepage: www.elsevier.com/locate/envpol http://dx.doi.org/10.1016/j.envpol.2016.10.089 0269-7491/© 2016 Elsevier Ltd. All rights reserved. Environmental Pollution xxx (2016) 1e9 Please cite this article in press as: Nguyen, M.A., et al., Spatial distribution and source tracing of per- and polyfluoroalkyl substances (PFASs) in surface water in Northern Europe, Environmental Pollution (2016), http://dx.doi.org/10.1016/j.envpol.2016.10.089