Abstract
After global commercialization of short-chain perfluoroalkyl acids (PFAAs) as substitutes to conventional long-chain PFAAs by the major manufacturers, two fluorine industry parks for production of short-chain PFAAs located in the Daling River Basin of northern China have developed rapidly in the last few years. This study provides a systematic assessment of sources, emissions, transportation, and potential risks of the PFAAs in this area. The C4 perfluorobutane sulfonic acid (PFBS) and perfluorobutanoic acid (PFBA) were the predominant short-chain PFAAs in river water, with maximum concentrations of 2.90 and 1.35 μg/L, respectively. Park 1 equipped with a telomerization process was identified to be the source of linear and branched mixtures of PFBS, PFBA, and perfluorooctanoic acid (PFOA), while park 2 with an electrochemical fluorination process (ECF) was identified to be the source of linear and branched mixtures of PFBS and PFOA. Partition coefficients between water and sediment were consistent for C4-C8 perfluoroalkyl carboxylic acids (PFCAs) but directly proportional to C9-C11 PFCAs and perfluoroalkyl sulfonic acids (PFSAs). Analysis on the health risk of PFBS and PFBA suggested that they were not without risk since short chain PFAAs are known to be recalcitrant during water treatment.
Similar content being viewed by others
References
3M (2000) Phase-out plan for PFOS-based products. USEPA Docket, U.S. Environmental Protection Agency
Ahrens L, Taniyasu S, Yeung LWY, Yamashita N, Lam PKS, Ebinghaus R (2010) Distribution of polyfluoroalkyl compounds in water, suspended particulate matter and sediment from Tokyo Bay, Japan. Chemosphere 79(3):266–272
Ahrens L, Yeung LWY, Taniyasu S, Lam PKS, Yamashita N (2011) Partitioning of perfluorooctanoate (PFOA), perfluorooctane sulfonate (PFOS) and perfluorooctane sulfonamide (PFOSA) between water and sediment. Chemosphere 85(5):731–737
Armitage JM, MacLeod M, Cousins IT (2009) Comparative assessment of the global fate and transport pathways of long-chain perfluorocarboxylic acids (PFCAs) and perfluorocarboxylates (PFCs) emitted from direct sources. Environ Sci Technol 43(15):5830–5836
Bao J, Liu W, Liu L, Jin Y, Dai J, Ran X, Zhang Z, Tsuda S (2010) Perfluorinated compounds in the environment and the blood of residents living near fluorochemical plants in Fuxin, China. Environ Sci Technol 45(19):8075–8080
Betts KS (2007) Perfluoroalkyl acids: what is the evidence telling us? Environ Health Perspect 115(5):A250–A256
Buck RC, Franklin J, Berger U, Conder JM, Cousins IT, de Voogt P, Jensen AA, Kannan K, Mabury SA, van Leeuwen SPJ (2011) Perfluoroalkyl and polyfluoroalkyl substances in the environment: terminology, classification, and origins. Integr Environ Assess Manag 7(4):513–541
Calafat AM, Wong LY, Kuklenyik Z, Reidy JA, Needham LL (2007) Polyfluoroalkyl chemicals in the U.S. population: data from the National Health and Nutrition Examination Survey (NHANES) 2003-2004 and comparisons with NHANES 1999-2000. Environ Health Perspect 115(11):1596–1602
Codling G, Vogt A, Jones PD, Wang T, Wang P, Lu YL, Corcoran M, Bonina S, Li A, Sturchio NC, Rockne KJ, Ji K, Khim J-S, Naile JE, Giesy JP (2014) Historical trends of inorganic and organic fluorine in sediments of Lake Michigan. Chemosphere 114:203–209
Conder JM, Hoke RA, Wolf W, Russell MH, Buck RC (2008) Are PFCAs bioaccumulative? A critical review and comparison with regulatory criteria and persistent lipophilic compounds. Environ Sci Technol 42(4):995–1003
Davis KL, Aucoin MD, Larsen BS, Kaiser MA, Hartten AS (2007) Transport of ammonium perfluorooctanoate in environmental media near a fluoropolymer manufacturing facility. Chemosphere 67(10):2011–2019
EC (2006) Directive 2006/122/EC of the European Parliament and of the Council of 12 December 2006 amending for the 30th time Council Directive 76/769/EEC on the approximation of the laws, regulations and administrative provisions of the member states relating to restrictions on the marketing and use of certain dangerous substances and preparations (perfluorooctane sulfonates)
Eschauzier C, Raat KJ, Stuyfzand PJ, De Voogt P (2013) Perfluorinated alkylated acids in groundwater and drinking water: identification, origin and mobility. Sci Total Environ 458–460:477–485
European Commission (2010) Analysis of the risks arising from the industrial use of perfuorooctanoic acid (PFOA) and ammonium perfluorooctanoate (APFO) and from their use in consumer articles. Evaluation of the risk reduction measures for potential restrictions on the manufacture, placing on the market and use of PFOA and APFO. http://ec.europa.eu/enterprise/sectors/chemicals/files/docs_studies/final_report_pfoa_pfos_en.pdf. (July 25 2014)
Fuxin Fluorine Industry Development Zone (2012) http://www.f-china.gov.cn. (July 25 2014)
Giesy JP, Naile JE, Khim JS, Jones PD, Newsted JL (2010) Aquatic toxicology of perfluorinated chemicals. In: Whitacre DM (ed) Reviews of environmental contamination and toxicology, Vol 202. Springer, New York, pp 1–52
Glynn A, Berger U, Bignert A, Ullah S, Aune M, Lignell S, Darnerud PO (2012) Perfluorinated alkyl acids in blood serum from primiparous women in Sweden: serial sampling during pregnancy and nursing, and temporal trends 1996–2010. Environ Sci Technol 46(16):9071–9079
Higgins CP, Luthy RG (2006) Sorption of perfluorinated surfactants on sediments†. Environ Sci Technol 40(23):7251–7256
Holt R (2011) The influence of global regulatory changes and customer preferences on the development of alternatves to long chain fluorinated chemicals. DuPont for FluoroCouncil
Houde M, De Silva AO, Muir DCG, Letcher RJ (2011) Monitoring of perfluorinated compounds in aquatic biota: an updated review. Environ Sci Technol 45(19):7962–7973
POPs Action in China (2014) http://www.china-pops.org. (July 25 2014)
Kwadijk CJAF, Korytár P, Koelmans AA (2010) Distribution of perfluorinated compounds in aquatic systems in The Netherlands. Environ Sci Technol 44(10):3746–3751
Kwok KY, Taniyasu S, Yeung LWY, Murphy MB, Lam PKS, Horii Y, Kannan K, Petrick G, Sinha RK, Yamashita N (2010) Flux of perfluorinated chemicals through wet deposition in Japan, the United States, and several other countries. Environ Sci Technol 44(18):7043–7049
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(2):366–394
Lindstrom AB, Strynar MJ, Libelo EL (2011) Polyfluorinated compounds: past, present, and future. Environ Sci Technol 45(19):7954–7961
Loi EIH, Yeung LWY, Taniyasu S, Lam PKS, Kannan K, Yamashita N (2011) Trophic magnification of poly- and perfluorinated compounds in a subtropical food web. Environ Sci Technol 45(13):5506–5513
MDH (2011) 2011 Health Risk Limits for Groundwater. http://www.health.state.mn.us/divs/eh/risk/guidance/gw/table.html. (July 25 2014)
Moller 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(10):3243–3250
NICNAS (2005) POTASSIUM PERFLUOROBUTANE SULFONATE: HAZARD ASSESSMENT. http://www.nicnas.gov.au/__data/assets/pdf_file/0004/4927/Potassium_Perfluorobutane_Sulfonate_PDF.pdf. (July 25 2014)
Oliaei F, Kriens D, Weber R, Watson A (2013) PFOS and PFC releases and associated pollution from a PFC production plant in Minnesota (USA). Environ Sci Pollut R 20(4):1977–1992
Olsen GW, Chang SC, Noker PE, Gorman GS, Ehresman DJ, Lieder PH, Butenhoff JL (2009) A comparison of the pharmacokinetics of perfluorobutanesulfonate (PFBS) in rats, monkeys, and humans. Toxicology 256(1–2):65–74
Olsen GW, Lange CC, Ellefson ME, Mair DC, Church TR, Goldberg CL, Herron RM, Medhdizadekashi Z, Nobiletti JB, Rios JA, Reagen WK, Zobel LR (2012) Temporal trends of perfluoroalkyl concentrations in American Red Cross Adult Blood Donors, 2000 - 2010. Environ Sci Technol 46(11):6330–6338
Pan YY, Shi YL, Wang JM, Jin XL, Cai YQ (2011) Pilot investigation of perfluorinated compounds in river water, sediment, soil and fish in Tianjin, China. Bull Environ Contam Toxicol 87(2):152–157
Paul AG, Jones KC, Sweetman AJ (2009) A first global production, emission, and environmental inventory for perfluorooctane sulfonate. Environ Sci Technol 43(2):386–392
Prevedouros K, Cousins IT, Buck RC, Korzeniowski SH (2006) Sources, fate and transport of perfluorocarboxylates. Environ Sci Technol 40(1):32–44
Rickard RW (2009) Toxicology–perfluorocarboxylates-PFOA-PFHxA-PFBA (J. Butenhoff). http://www.epa.gov/oppt/pfoa/pubs/Toxicology-Carboxylates%20-Rickard.pdf. (July 25 2014)
Simcik MF, Dorweiler KJ (2005) Ratio of perfluorochemical concentrations as a tracer of atmospheric deposition to surface waters. Environ Sci Technol 39(22):8678–8683
Taniyasu S, Kannan K, So MK, Gulkowska A, Sinclair E, Okazawa T, Yamashita N (2005) Analysis of fluorotelomer alcohols, fluorotelorner acids, and short- and long-chain perfluorinated acids in water and biota. J Chromatogr A 1093(1–2):89–97
UNEP (2009) The conference of the parties 4 of the Stockholm Convention (COP-4) in Geneva placed perfluorooctane sulfonate and perfluorooctane sulfonyl fluoride (PFOS and PFOSF) in Annex B. http://chm.pops.int/Convention/Pressrelease/COP4Geneva9May2009/tabid/542/language/en-US/Default.aspx. (July 25 2014)
USEPA (2006) 2010/2015 PFOA Stewardship Program. http://www.epa.gov/opptintr/pfoa/pubs/stewardship/. (July 25 2014)
Wang TY, Lu YL, Chen CL, Naile JE, Khim JS, Park J, Luo W, Jiao WT, Hu WY, Giesy JP (2011) Perfluorinated compounds in estuarine and coastal areas of north Bohai Sea, China. Mar Pollut Bull 62(8):1905–1914
Wang B, Cao M, Zhu H, Chen J, Wang L, Liu G, Gu X, Lu X (2013a) Distribution of perfluorinated compounds in surface water from Hanjiang River in Wuhan, China. Chemosphere 93(3):468–473
Wang P, Wang TY, Giesy JP, Lu YL (2013b) Perfluorinated compounds in soils from Liaodong Bay with concentrated fluorine industry parks in China. Chemosphere 91(6):751–757
Wang P, Lu Y, Wang T, Fu Y, Zhu Z, Liu S, Xie S, Xiao Y, Giesy JP (2014a) Occurrence and transport of 17 perfluoroalkyl acids in 12 coastal rivers in south Bohai coastal region of China with concentrated fluoropolymer facilities. Environ Pollut 190:115–122
Wang T, Wang P, Meng J, Liu S, Lu Y, Khim JS, Giesy JP (2014b) A review of sources, multimedia distribution and health risks of perfluoroalkyl acids (PFAAs) in China. Chemosphere. doi:10.1016/j.chemosphere.2014.09.021
Wania F (2007) A global mass balance analysis of the source of perfluorocarboxylic acids in the Arctic ocean. Environ Sci Technol 41(13):4529–4535
Wilhelm M, Bergmann S, Dieter HH (2010) Occurrence of perfluorinated compounds (PFCs) in drinking water of North Rhine-Westphalia, Germany and new approach to assess drinking water contamination by shorter-chained C4-C7 PFCs. Int J Hyg Environ Health 213(3):224–232
Xie S, Lu Y, Wang T, Liu S, Jones K, Sweetman A (2013a) Estimation of PFOS emission from domestic sources in the eastern coastal region of China. Environ Int 59:336–343
Xie SW, Wang TY, Liu SJ, Jones KC, Sweetman AJ, Lu YL (2013b) Industrial source identification and emission estimation of perfluorooctane sulfonate in China. Environ Int 52:1–8
Yang S, Xu F, Wu F, Wang S, Zheng B (2014) Development of PFOS and PFOA criteria for the protection of freshwater aquatic life in China. Sci Total Environ 470–471:677–683
Zhao L, Zhu L, Yang L, Liu Z, Zhang Y (2012) Distribution and desorption of perfluorinated compounds in fractionated sediments. Chemosphere 88(11):1390–1397
Zhou Z, Liang Y, Shi Y, Xu L, Cai Y (2013) Occurrence and transport of perfluoroalkyl acids (PFAAs), including short-chain pfaas in Tangxun Lake, China. Environ Sci Technol 47(16):9249–9257
Zhou Z, Shi Y, Vestergren R, Wang T, Liang Y, Cai Y-Q (2014) Highly elevated serum concentrations of perfluoroalkyl substances in fishery employees from Tangxun Lake, China. Environ Sci Technol 48(7):3864–3874
Acknowledgement
This study was supported by the National Natural Science Foundation of China (no. 41371488 and 41171394), the Key Research Program of the Chinese Academy of Sciences (no. KZZD-EW-TZ-12), and the International Scientific Cooperation Program with Grant No. 2012DFA91150. Prof. Giesy was supported by the Canada Research Chair Program. We would like to thank the editors and reviewers for their valuable comments and suggestions.
Author information
Authors and Affiliations
Corresponding author
Additional information
Responsible editor: Leif Kronberg
Electronic supplementary material
Below is the link to the electronic supplementary material.
ESM 1
(DOCX 700 kb)
Rights and permissions
About this article
Cite this article
Wang, P., Lu, Y., Wang, T. et al. Transport of short-chain perfluoroalkyl acids from concentrated fluoropolymer facilities to the Daling River estuary, China. Environ Sci Pollut Res 22, 9626–9636 (2015). https://doi.org/10.1007/s11356-015-4090-x
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-015-4090-x