Per- and Polyfluoroalkyl Substances in Swedish Groundwater and

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Per- and polyfluoroalkyl substances (PFASs) in Swedish ground- and surface water – Implications for environmental quality standards and drinking water guidelines Laura Gobelius, Johanna Kim Hedlund, Wiebke Dürig, Rikard Tröger, Karl Lilja, Karin Wiberg, and Lutz Ahrens Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/acs.est.7b05718 • Publication Date (Web): 12 Mar 2018 Downloaded from http://pubs.acs.org on March 12, 2018

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Environmental Science & Technology

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Per- and polyfluoroalkyl substances (PFASs) in Swedish ground- and surface water –

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Implications for environmental quality standards and drinking water guidelines

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Laura Gobeliusa, Johanna Hedlunda, Wiebke Düriga, Rikard Trögera, Karl Liljab, Karin Wiberga, Lutz

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Ahrensa,*

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a

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7050, SE-750 07 Uppsala, Sweden

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b

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Department of Aquatic Sciences and Assessment, Swedish University of Agricultural Sciences (SLU), Box

Swedish Environmental Protection Agency (Naturvårdsverket), Valhallavägen 195, 115 53 Stockholm

*Corresponding author: Lutz Ahrens, email: [email protected]; phone: +46 (0)70-2972245

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TOC:

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ACS Paragon Plus Environment


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Abstract

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The aim of this study was to assess per- and polyfluoroalkyl substances (PFASs) in the Swedish aquatic

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environment, identify emission sources and compare measured concentrations with environmental quality

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standards (EQS) and (drinking) water guideline values. In total, 493 samples were analysed in 2015 for 26

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PFASs (∑26PFASs) in surface water, groundwater, landfill leachate, sewage treatment plant effluents and

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reference lakes, focusing on hot spots and drinking water sources. Highest ∑26PFAS concentrations were

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detected in surface- (13,000 ng L-1) and groundwater (6,400 ng L-1). The dominating fraction of PFASs in

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surface water were perfluoroalkyl carboxylates (PFCAs; 64% of ∑26PFASs), with high contributions from

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C4-C8 PFCAs (94% of ∑PFCAs), indicating high mobility of shorter chain PFCAs. In inland surface water,

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the annual average (AA)-EQS of the EU Water Framework Directive of 0.65 ng L-1 for ∑PFOS (linear and

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branched isomers) was exceeded in 46% of the samples. The drinking water guideline value of 90 ng L-1 for

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∑11PFASs recommended by the Swedish EPA was exceeded in 3% of the water samples from drinking water

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sources (n = 169). The branched isomers had a noticeable fraction in surface – and groundwater for

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perfluorooctanesulfonamide, perfluorohexane sulfonate and perfluorooctane sulfonate, highlighting the need

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to include branched isomers in future guidelines.

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Keywords: guideline values; groundwater; surface water; sewage treatment plant (STP) effluent; landfill

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leachate; source tracing; per- and polyfluoroalkyl substances; PFASs; PFOS

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Introduction

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Per- and polyfluoroalkyl substances (PFASs) are an emerging class of chemicals with unique

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physicochemical properties, such as extremely high environmental persistence and surfactant characteristics

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due to their stable carbon-fluorine bonds of the hydrophobic part of the molecule and a hydrophilic head1.

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Furthermore, they are appreciated for their stain- and water-repellent properties and have widely been used

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as surfactants, e.g. in textiles, packaging material and aqueous film forming foams (AFFFs)2. The broad

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range of applications as well as their highly persistent and bioaccumulative characteristics1 have led to a

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ubiquitous distribution in the environment3. PFASs have been detected in waters4, soils5,6, plants7, as well as

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in wildlife3 and humans8 in populated as well as in remote environments9. Main point sources for PFASs are

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fire training sites where PFAS-containing AFFFs have been used (often located at airports and military

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training grounds)10,11, discharges from manufacturing industries and sewage treatment plants (STPs)12,13, and

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landfill leachate14,15. Additionally, various diffuse sources, mainly related to the urban environment (e.g.

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surface run-off) and atmospheric deposition contribute to the environmental burden16,17. Short-chained

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PFASs with a perfluorocarbon chain length of 10% of the surface water (n = 289) samples (i.e. PFPeA,

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PFHxA, PFHpA, PFOA, PFNA, PFDA, PFBS, PFHxS, PFOS, 6:2 FTSA and FOSA) showed significant

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correlation with each other (p < 0.01), indicating a common or similar source (SI Table S15).

, maximum 57 ng L-1) in comparison to groundwater levels. The dominant PFASs in groundwater were L-

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Figure 4 Composition profiles of PFASs for different source categories for surface- and groundwater. The surface water

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categories are fire training sites (n = 142), unspecific industry (n = 45), STP effluent (n = 14), landfill/waste disposal

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sites (n = 20), skiing areas (n = 6) and urban areas (n = 8). The groundwater categories are fire training sites (n = 41),

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unspecific industry (n = 61), landfill/waste disposal sites (n = 4), skiing areas (n = 3) and urban areas (n = 16). PFCAs

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are coloured in blue and grey, PFSAs in green and PFAS precursors in orange/red.

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Linear and branched isomers. The compounds FOSA, PFHxS and PFOS were studied separately as

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∑branched or linear isomers (L-) for surface- and groundwater (Figure S5 in the SI). Isomeric composition

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has previously been used to trace emission sources15,64. The surface water samples generally showed a higher

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proportion of branched isomers than the groundwater samples, which is in contradiction to results from

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Kärrman et al. (2011)64, who concluded the opposite and suggested higher water solubility of branched

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isomers. However, the higher proportion of branched isomers in surface water was only statistically

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significant (p < 0.05; two sided student’s t-test) for FOSA and PFOS. While ∑branched-FOSA was solely

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occurring in the surface water samples (2% of the ∑FOSA), ∑branched-PFOS had the highest fraction of

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branched isomers in both, surface- (20% of the ∑PFOS) and groundwater (8% of the ∑PFOS). Kärrman et

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al., (2011) and Houde et al. (2008) found higher proportions of ∑branched-PFOS in water samples, ranging

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between 39-42% and 44-57% of the ∑PFOS concentration, respectively64,65. The ∑branched-PFHxS

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occurred with 5% and 7% of the ∑PFHxS in groundwater and surface water, respectively. As the branched

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isomers are not explicitly mentioned in the drinking water guidelines referred to earlier35,37–39,41,43, they were

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not considered in our evaluation of the drinking water safety. While the low fractions of branched isomers in

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our samples suggest a relatively low risk for drinking water, the results from Kärrman et al. (2011) and

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Houde et al. (2006) showed that branched isomers should be included in the drinking water guidelines64,65.

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For the Water Framework Directive (WFD), another 4% (n = 12) of the surface water samples exceeded the

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AA-EQS threshold value (0.65 ng L-1) compared to if only L-PFOS was considered. Ultimately, branched

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isomers should be considered in legislation and guidelines since they showed partly a high fraction in the

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aquatic environment (i.e. up to 20% for ∑branched-PFOS in surface water) and have a similar toxicity

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potential compared to the linear isomer66.

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Comparison of measured concentrations with guideline values. The sum of branched and linear

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isomers of PFOS was found at levels above the MDL (0.21 ng L-1) in 63% of the surface water samples (n =

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176 out of 289), of which 74% (n = 123) exceeded the AA-EQS of 0.65 ng L-1, while all measured

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concentrations stayed well below the MAC-EQS value of 36,000 ng L-1 of the EU WFD (Figure 5).

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However, the results should be treated with caution since the value of 0.65 ng L-1 is close to the MDLPFOS in

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this study (0.21 ng L-1). There is thus an uncertainty in whether this threshold was exceeded only at that

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particular time of sampling or over long term. Irrespectively, it might be questionable if ∑PFOS

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concentrations of >0.65 ng L-1 are threatening the ecosystems67–69. According to Loos et al. (2009), the

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median PFOS concentration in European rivers is 6.0 ng L-1, hence, many European inland surface waters

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were exceeding the AA-EQS50, while the median L-PFOS surface water concentration in this study was 0.40

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ng L-1. To the best of the author’s knowledge, there is no equally comprehensive study on PFASs in

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European inland surface waters available for comparison, however, it is not known how the concentrations

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have developed and if the data from Loos et al. (2009) is still reflecting current concentrations. Besides, the

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EU WFD only focuses on ∑PFOS, while our results show that L-PFOS constituted only a small fraction

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(14%) of the ∑26PFASs in surface water, with a similar fraction of other PFASs, namely PFHxA (17%),

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PFOA (15%) and PFHpA (14%). Thus, provided that sufficient toxicity data is available, it could be argued

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that other PFASs, including branched and linear isomers as well as PFAS precursors, need to be included in

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EU WFD and other regulations. None of the groundwater samples (n = 164) exceeded the guideline value for PFOS (45 ng L-1)

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recommended by SGI34. If assuming the same toxicity as PFOS for all 26 PFASs, 10 samples would exceed

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45 ng L-1 for ∑26PFASs. This indicates that groundwater guideline values should include more PFASs, as

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discussed for the surface water, to protect ecosystem and human health.

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For the drinking water source areas, 5 out of 169 samples (3.0%) exceeded the threshold value of 90 ng

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L-1 for ∑11PFASs (PFBA, PFPeA, PFHxA, PFHpA, PFOA, PFNA, PFDA, PFBS, PFHxS, PFOS and 6:2

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FTSA) of the Swedish National Food Agency43 (Figure S6 in the SI). The number of samples would not

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increase if ∑26PFASs were considered in the drinking water threshold value of 90 ng L-1. However, L-FOSA,

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the substance with the highest PFAS fraction (20%) and a high detection frequency (31%) is not included in

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the Swedish drinking water guideline43 and should be considered in future assessments. The few (n = 5)

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samples that exceeded the Swedish drinking water guideline value originated from groundwater, with four of

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them most probably being impacted by fire training sites, while the fifth sample was located close to an

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agricultural area where PFAS-contaminated sludge could have been applied as fertilizer, a PFAS impact that

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has been observed previously49. A spatial trend for PFASs could not be identified in the drinking water

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samples, but it is interesting to note that four counties with a low population density (< 20 people per km2)

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had composition profiles dominated by FOSA, while all other composition profiles consisted of mainly

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PFCAs and PFSAs (Figure S6 in the SI). The Swedish limit value for sensitive citizens of 900 ng L-1 was not

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exceeded in any of the samples from drinking water source areas. While the Swedish and Danish drinking

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water guideline values (i.e. 90 ng L-1 and 100 ng L-1 for ∑11PFASs and ∑12PFASs, respectively) were

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exceeded in a few cases, no drinking water sample from our study exceeds the drinking water

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recommendations from the US EPA, UK, the Netherlands and Germany. However, there are, to the best of

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the author’s knowledge, no comprehensive screening studies available for other countries, but the current

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study emphasizes the need for increased knowledge about health risks associated with intake of PFASs and

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achieving a more coherent view in protecting aquatic ecosystems and human health. Furthermore, as

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monitoring data are scarce, there are large uncertainties about spatial and temporal variation of PFASs in the

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aquatic environment. For source tracing and better understanding of limit exceedance, regular monitoring of

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PFASs in the ecosystem and in drinking water source areas is urgently needed. Sites potentially impacted by

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PFASs from firefighting training as well as landfill leachate, STP effluents and biosolid impacted

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agricultural areas are of high concern and extra efforts should be made to identify more sources that pose

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risks to the environment and human health.

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Figure 5 Concentrations of PFOS and ∑26PFASs in drinking water (n = 169), surface water (n = 289) and groundwater

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(n = 161) and comparison with applicable guideline values. Note the logarithmic scale. The drinking water thresholds

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refer to the Swedish drinking water guideline, the surface water thresholds refer to the EU WFD while the groundwater

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threshold was recommended by the Swedish SGI.

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Associated content (SI): Explanatory text about sampling and blank preparation, map of counties, hot spot

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sampling locations and composition profiles, composition profiles of PFASs in various types of water, PCA

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for groundwater samples, fraction of linear and branched isomers, drinking water composition profiles for

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respective counties, table with chemicals, purity, manufacturer, table with most important PFASs

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characteristics, sampling protocols in Swedish and English language, blank concentrations and MDLs,

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triplicates and recoveries, sample IDs and locations, individual PFAS concentration, list of samples included

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in source classification, Pearson coefficients and significance for PFASs in groundwater and surface water.

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Acknowledgements We kindly acknowledge Jelena Rakovic and Elin Andersson for assistance with the lab

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analysis, Emil Back for the compilation of the ArcGIS maps, the Swedish EPA for funding of the project

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(NV-02893-15) and all County Administration Boards for the selection of sampling sites and the conduction

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of the sampling.

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Per- and Polyfluoroalkyl Substances in Swedish Groundwater and

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