Skip to main content

Advertisement

SpringerLink
Log in

Neutral poly- and perfluoroalkyl substances in air and seawater of the North Sea

  • Nordic Research on Perfluoroalkyl and Polyfluoroalkyl Substances (PFASs)
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

Concentrations of neutral poly- and perfluoroalkyl substances (PFASs), such as fluorotelomer alcohols (FTOHs), perfluoroalkane sulfonamides (FASAs), perfluoroalkane sufonamidoethanols (FASEs), and fluorotelomer acrylates (FTACs), have been simultaneously determined in surface seawater and the atmosphere of the North Sea. Seawater and air samples were taken aboard the German research vessel Heincke on the cruise 303 from 15 to 24 May 2009. The concentrations of FTOHs, FASAs, FASEs, and FTACs in the dissolved phase were 2.6–74, <0.1–19, <0.1–63, and <1.0–9.0 pg L−1, respectively. The highest concentrations were determined in the estuary of the Weser and Elbe rivers and a decreasing concentration profile appeared with increasing distance from the coast toward the central part of the North Sea. Gaseous FTOHs, FASAs, FASEs, and FTACs were in the range of 36–126, 3.1–26, 3.7–19, and 0.8–5.6 pg m−3, which were consistent with the concentrations determined in 2007 in the North Sea, and approximately five times lower than those reported for an urban area of Northern Germany. These results suggested continuous continental emissions of neutral PFASs followed by transport toward the marine environment. Air–seawater gas exchanges of neutral PFASs were estimated using fugacity ratios and the two-film resistance model based upon paired air–seawater concentrations and estimated Henry's law constant values. Volatilization dominated for all neutral PFASs in the North Sea. The air–seawater gas exchange fluxes were in the range of 2.5 × 103–3.6 × 105 pg m−2 for FTOHs, 1.8 × 102–1.0 × 105 pg m−2 for FASAs, 1.1 × 102–3.0 × 105 pg m−2 for FASEs and 6.3 × 102–2.0 × 104 pg m−2 for FTACs, respectively. These results suggest that the air–seawater gas exchange is an important process that intervenes in the transport and fate for neutral PFASs in the marine environment.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5

Similar content being viewed by others

References

  • Ahrens L, Felizeter S, Ebinghaus R (2009) Spatial distribution of polyfluoroalkyl compounds in seawater of the German Bight. Chemosphere 76:179–184

    Article  CAS  Google Scholar 

  • Ahrens L, Shoeib M, Harner T, Lee SC, Guo R, Reiner EJ (2011) Wastewater treatment plant and landfills as sources of polyfluoroalkyl compounds to the atmosphere. Environ Sci Technol 45:8098–8105

    Article  CAS  Google Scholar 

  • Andersen MPS, Nielsen OJ, Hurley MD, Ball JC, Wallington TJ, Ellis DA, Martin JW, Mabury SA (2005) Atmospheric chemistry of 4:2 fluorotelomer alcohol (n-C4F9CH2CH2OH): products and mechanism of Cl atom initiated oxidation in the presence of NOx. J Phys Chem A 109:1849–1856

    Article  CAS  Google Scholar 

  • Armitage J, Cousins IT, Buck RC, Prevedouros K, Russell MH, MacLeod M, Korzeniowski S (2006) Modeling globalscale fate and transport of perfluorooctanoate emitted from direct sources. Environ Sci Technol 40:6969–6975

    Article  CAS  Google Scholar 

  • Armitage J, MacLeod M, Cousins I (2009) Modeling the global fate of perfluorooctanoic acid (PFOA) and perfluorooctanoate (PFO) emitted from direct sources using a multispecies mass balance model. Enivon Sci Technol 43:1134–1140

    Article  CAS  Google Scholar 

  • Benskin JP, Ikonomou MG, Gobas FAPC, Begley TH, Woudneh MB, Cosgrove JR (2013) Biodegradation of N-ethyl perfluorooctane sulfonamido ethanol (EtFOSE) and EtFOSE-based phosphate diester (SAmPAP Diester) in marine sediments. Environ Sci Technol 47:1381–1389

    CAS  Google Scholar 

  • Bidleman TF, McConnell LL (1995) A review of field experiments to determine air–water gas exchange of persistent organic pollutants. Sci Total Environ 159:101–117

    Article  CAS  Google Scholar 

  • Bruhn R, Lakaschus S, McLachlan MS (2003) Air/sea gas exchange of PCBs in the southern Baltic Sea. Atmos Environ 37:3445–3454

    Article  CAS  Google Scholar 

  • Butt CM, Young CJ, Mabury SA, Hurley MD, Wallington TJ (2009) Atmospheric chemistry of 4:2 fluorotelomer acrylate [C4F9CH2CH2OC(O)CH=CH2]: kinetics, mechanisms, and products of chlorine-atom- and OH-radical-initiated oxidation. J Phys Chem A 113:3155–3161

    Article  CAS  Google Scholar 

  • Cousins I, Kong D, VestergrenA R (2011) Reconciling measurement and modelling studies of the sources and fate of perfluorinated carboxylates. Environ Chem 8:339–354

    CAS  Google Scholar 

  • Del Vento S, Halsall C, Gioia R, Jones K, Dachs J (2012) Volatile per- and polyfluoroalkyl compounds in the remote atmosphere of the western Antarctic Peninsula: an indirect source of perfluoroalkyl acids to Antarctic waters? Atmos Pollut Res 3:450–455

    Article  Google Scholar 

  • D'Eon JC, Hurley MD, Wallington TJ, Mabury SA (2006) Atmospheric chemistry of N-methyl perfluorobutane sulfonamidoethanol, C4F9SO2N(CH3)CH2CH2OH: kinetics and mechanism of reaction with OH. Environ Sci Technol 40:1862–1868

    Article  Google Scholar 

  • Dietz R, Bossi R, Riget FF, Sonne C, Born EW (2008) Increasing perfluoroalkyl contaminants in east Greenland polar bears (Ursus maritimus): a new toxic threat to the Arctic bears. Environ Sci Technol 42:2701–2707

    Article  CAS  Google Scholar 

  • Dreyer A, Ebinghaus R (2009) Polyfluorinated compounds in ambient air from ship- and land-based measurements in northern Germany. Atmos Environ 43:1527–1535

    Article  CAS  Google Scholar 

  • Dreyer A, Temme C, Sturm R, Ebinghaus R (2008) Optimized method avoiding solvent-induced response enhancement in the analysis of volatile and semi-volatile polyfluorinated alkylated compounds using gas chromatography–mass spectrometry. J Chromatogr A 1178:199–205

    Article  CAS  Google Scholar 

  • Dreyer A, Matthias V, Temme C, Ebinghaus R (2009a) Annual time series of air concentrations of polyfluorinated compounds. Environ Sci Technol 43:4029–4036

    Article  CAS  Google Scholar 

  • Dreyer A, Weinberg I, Temme C, Ebinghaus R (2009b) Polyfluorinated compounds in the atmosphere of the Atlantic and Southern oceans: evidence for a global distribution. Environ Sci Technol 43:6507–6514

    Article  CAS  Google Scholar 

  • Ellis DA, Martin JW, De Silva AO, Mabury SA, Hurley MD, Sulbaek Andersen MP, Wallington TJ (2004) Degradation of fluorotelomer alcohols: a likely atmospheric source of perfluorinated carboxylic acids. Environ Sci Technol 38:3316–3321

    Article  CAS  Google Scholar 

  • Giesy JP, Kannan K (2001) Global distribution of perfluorooctane sulfonate in wildlife. Environ Sci Technol 35:1339–1342

    Article  CAS  Google Scholar 

  • Hornbuckle KC, Jeremiason JD, Sweet CW, Eisenreich SJ (1994) Seasonal variations in air–water exchange of polychlorinated biphenyls in Lake Superior. Environ Sci Technol 28:1491–1501

    Article  CAS  Google Scholar 

  • Jahnke A, Ahrens L, Ebinghaus R, Temme C (2007) Urban versus remote air concentrations of fluorotelomer alcohols and other polyfluorinated alkyl substances in Germany. Environ Sci Technol 41:745–752

    Article  CAS  Google Scholar 

  • Kissa E (ed) (2001) Fluorinated surfactants and repellents, 97. Marcel Dekker, New York

    Google Scholar 

  • Lau C, Anitole K, Hodes C, Lai D, Pfahles-Hutchens A, Seed J (2007) Perfluoroalkyl acids: a review of monitoring and toxicological findings. Toxicol Sci 99:366–394

    Article  CAS  Google Scholar 

  • Li J, Del Vento S, Schuster J, Zhang G, Chakraborty P, Kobara Y, Jones KC (2011) Perfluorinated compounds in the Asian atmosphere. Environ Sci Technol 45:7241–7248

    Article  CAS  Google Scholar 

  • Liss PS, Slater PG (1974) Flux of gases across air–sea interface. Nature 247:181–184

    Article  CAS  Google Scholar 

  • Lohmann R, Gioia R, Jones KC, Nizzetto L, Temme C, Xie Z, Schulz-Bull D, Hand I, Morgan E, Jantunen L (2009) Organochlorine pesticides and PAHs in the surface water and atmosphere of the North Atlantic and Arctic Ocean. Environ Sci Technol 43:5633–5639

    Article  CAS  Google Scholar 

  • Mahmoud MAM, Karrman A, Oono S, Harada KH, Koizumi A (2009) Polyfluorinated telomers in precipitation and surface water in an urban area of Japan. Chemosphere 74:467–472

    Article  CAS  Google Scholar 

  • Martin JW, Ellis DA, Mabury SA, Hurley MD, Wallington TJ (2006) Atmospheric chemistry of perfluoroalkanesulfonamides: kinetic and product studies of the OH radical and Cl atom initiated oxidation of N-ethyl perfluorobutanesulfonamide. Environ Sci Technol 40:864–872

    Article  CAS  Google Scholar 

  • Möller A, Ahrens L, Surm R, Westerveld J, van der Wielen F, Ebinghaus R, de Voogt P (2010) Distribution and sources of polyfluoroalkyl substances (PFAS) in the River Rhine watershed. Environ Pollut 158:3243–3250

    Article  Google Scholar 

  • Oono S, Matsubara E, Harada KH, Takagi S, Hamada S, Asakawa A, Inoue K, Watanabe I, Koizumi A (2008) Survey of airborne polyfluorinated telomers in Keihan area, Japan. Bull Environ Contam Toxicol 80:102–106

    Article  CAS  Google Scholar 

  • Paul AG, Jones KC, Sweetman AJ (2008) A first global production, emission, and environmental inventory for perfluorooctane sulfonate. Environ Sci Technol 43:386–392

    Article  Google Scholar 

  • Piekarz AM, Primbs T, Field JA, Barofsky DF, Simonich S (2007) Semivolatile fluorinated organic compounds in Asian and western US air masses. Environ Sci Technol 41:8248–8255

    Article  CAS  Google Scholar 

  • Plumlee MH, McNeill K, Reinhard M (2009) Indirect photolysis of perfluorochemicals: hydroxyl radical-initiated oxidation of N-ethyl perfluorooctane sulfonamido acetate (N-EtFOSAA) and other perfluoroalkanesulfonamides. Environ Sci Technol 43:3662–3668

    Article  CAS  Google Scholar 

  • Prevedouros K, Cousins IT, Buck RC, Korzeniowski SH (2006) Sources, fate and transport of perfluorocarboxylates. Environ Sci Technol 40:32–44

    Article  CAS  Google Scholar 

  • Rhoads KR, Janssen EML, Luthy RG, Criddle CS (2008) Aerobic biotransformation and fate of N-ethyl perfluorooctane sulfonamidoethanol (N-EtFOSE) in activated sludge. Environ Sci Technol 42:2873–2878

    Article  CAS  Google Scholar 

  • Ritter SK (2010) Fluorochemicals go short. Chem Eng News 88:12–17

    Google Scholar 

  • Schultz MM, Barofsky DF, Field JA (2003) Fluorinated alkyl surfactants. Environ Eng Sci 20:487–501

    Article  CAS  Google Scholar 

  • Schwarzenbach RP, Gschwend PM, Imboden DM (2003) Environmental organic chemistry. Wiley, Hoboken

    Google Scholar 

  • Shoeib M, Harner T, Vlahos P (2006) Perfluorinated chemicals in the Arctic atmosphere. Environ Sci Technol 40:7577–7583

    Article  CAS  Google Scholar 

  • Stock NL, Furdui VI, Muir DCG, Mabury SA (2007) Perfluoroalkyl contaminants in the Canadian Arctic: evidence of atmospheric transport and local contamination. Environ Sci Technol 41:3529–3536

    Article  CAS  Google Scholar 

  • Sun H, Zhang X, Wang L, Zhang T, Li F, He N, Alder AC (2012) Perfluoroalkyl compounds in municipal WWTPs in Tianjin, China—concentrations, distribution and mass flow. Environ Sci Pollut Res 19:1405–1415

    Article  CAS  Google Scholar 

  • Wang N, Szostek B, Folsom PW, Sulecki LM, Capka V, Buck RC, Berti WR, Gannon JT (2005a) Aerobic biotransformation of 14 C-labeled 8–2 telomer B alcohol by activated sludge from a domestic sewage treatment plant. Environ Sci Technol 39:531–538

    Article  CAS  Google Scholar 

  • Wang N, Bogdan Szostek B, Buck RC, Folsom PW, Sulecki LM, Capka V, Berti WR, Gannon JT (2005b) Fluorotelomer alcohol biodegradation: direct evidence that perfluorinated carbon chains breakdown. Environ Sci Technol 39:7516–7528

    Article  CAS  Google Scholar 

  • Wang T, Khim JS, Chen C, Naile JE, Lu Y, Kannan K, Park J, Luo W, Jiao W, Hu W, Giesy JP (2012) Perfluorinated compounds in surface waters from Northern China: comparison to level of industrialization. Environ Int 42:37–46

    Article  CAS  Google Scholar 

  • Weinberg I, Dreyer A, Ebinghaus R (2010) Landfills as sources of polyfluorinated compounds, polybrominated diphenyl ethers and musk fragrances to ambient air. Atmos Environ 45:935–941

    Article  Google Scholar 

  • Weinberg I, Dreyer A, Ebinghaus R (2011) Waste water treatment plants as sources of polyfluorinated compounds, polybrominated diphenyl ethers and musk fragrances to ambient air. Environ Pollut 159:125–132

    Article  CAS  Google Scholar 

  • Xie Z, Ebinghaus R, Temme C, Caba A, Ruck W (2005) Atmospheric concentrations and air-sea exchanges of phthalates in the North Sea (German Bight). Atmos Environ 39:3209–3219

    Article  CAS  Google Scholar 

  • Xie Z, Lakaschus S, Ebinghaus R, Caba A, Ruck W (2006) Atmospheric concentrations and air-sea exchanges of nonylphenol, tertiary octylphenol and nonylphenol monoethoxylate in the North Sea. Environ Pollut 489(142):170–180

    Article  Google Scholar 

  • Xie Z, Moller A, Ahrens L, Sturm R, Ebinghaus R (2011) Brominated flame retardants in seawater and atmosphere of the Atlantic and the Southern Ocean. Environ Sci Technol 45:1820–1826

    Article  CAS  Google Scholar 

  • Zhao Z, Xie Z, Moller A, Sturm R, Tang J, Zhang G, Ebinghaus R (2012) Distribution and long-range transport of polyfluoroalkyl substances in the Arctic, Atlantic Ocean and Antarctic coast. Environ Pollut 170:71–77

    Article  CAS  Google Scholar 

  • Zhao L, Folsom PW, Wolstenholme BW, Sun H, Wang N, Buck RC (2013) 6:2 Fluorotelomer alcohol biotransformation in an aerobic river sediment system. Chemosphere 90:203–209

    Article  CAS  Google Scholar 

Download references

Acknowledgments

We acknowledge Alfred-Wegener-Institute for Polar and Marine Research (AWI), Bremerhaven, Germany, for the possibility of taking part in the expedition cruise. We are grateful to the captain and the crew of R/V Heincke. Armando Caba (HZG) is kindly acknowledged for organizing and assisting on the cruise.

Author information

Authors and Affiliations

  1. Centre for Materials and Coastal Research, Institute of Coastal Research, Department for Environmental Chemistry, Helmholtz-Zentrum Geesthacht, Geesthacht, Germany

    Zhiyong Xie, Zhen Zhao, Axel Möller, Hendrik Wolschke, Renate Sturm & Ralf Ebinghaus

  2. Key Laboratory of Coastal Zone Environmental Processes, Yantai Institute of Coastal Zone Research, CAS, Yantai, 264003, People’s Republic of China

    Zhen Zhao

  3. Department of Aquatic Sciences and Assessment, Swedish University of Agricultural Sciences, SE-750 07, Uppsala, Sweden

    Lutz Ahrens

Authors
  1. Zhiyong Xie
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Zhen Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Axel Möller
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Hendrik Wolschke
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Lutz Ahrens
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Renate Sturm
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Ralf Ebinghaus
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Zhiyong Xie.

Additional information

Responsible editor: Constantini Samara

Rights and permissions

Reprints and permissions

About this article

Cite this article

Xie, Z., Zhao, Z., Möller, A. et al. Neutral poly- and perfluoroalkyl substances in air and seawater of the North Sea. Environ Sci Pollut Res 20, 7988–8000 (2013). https://doi.org/10.1007/s11356-013-1757-z

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-013-1757-z

Keywords

Search

Navigation