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Perfluoroalkyl compounds in municipal WWTPs in Tianjin, China—concentrations, distribution and mass flow

  • Urbanization in China and its Environmental Impact
  • Published:
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Abstract

Backgrounds

Perfluorinated compounds (PFCs) have drawn much attention due to their environmental persistence, ubiquitous existence, and bioaccumulation potential. Wastewater treatment plants (WWTPs) are fundamental utilities in cities, playing an important role in preventing water pollution by lowering pollution load in waste waters. However, some of the emerging organic pollutants, like PFCs cannot be efficiently removed by traditional biological technologies in WWTPs, and some even increase in effluents compared to influents due to the incomplete degradation of precursors. Hence, WWTPs are considered to be a main point source in cities for PFCs that enter the aquatic environment. However, the mass flow of PFCs from WWTPs has seldom been analyzed for a whole city. Hence, in the present study, 11 PFCs including series of perfluoroalkyl carboxylic acids (PFCAs, C4–C12) and two perfluoroalkyl sulfonates (PFASs, C6 and C8) were measured in WWTP influents and effluents and sludge samples from six municipal WWTPs in Tianjin, China. Generation and dissipation of the target PFCs during wastewater treatment process and their mass flow in effluents were discussed.

Results

All the target PFCs were detected in the six WWTPs, and the total PFC concentration in different WWTPs was highly influenced by the population density and commercial activities of the corresponding catchments. Perfluorooctanoic acid (PFOA) was the predominant PFC in water phase, with concentrations ranging from 20 to 170 ng/L in influents and from 30 to 145 ng/L in effluents. Concentrations of perfluoroalkyl sulfonates decreased substantially in the effluent compared to the influent, which could be attributed to the sorption onto sludge, whereas concentrations of PFOA and some other PFCAs increased in the effluent in some WWTPs due to their weaker sorption onto solids and the incomplete degradation of precursors. Perfluorooctane sulfonic acid (PFOS) was the predominant PFC in sludge samples followed by PFOA, and their concentrations ranged from 42 to 169 g/kg and from 12 to 68 g/kg, respectively. Sludge-wastewater distribution coefficients (log K d) ranged from 0.62 to 3.87 L/kg, increasing with carbon chain length of the homologues. The mass flow of some PFCs in the effluent was calculated, and the total mass flow from all the six municipal WWTPs in Tianjin was 26, 47, and 3.5 kg/year for perfluorohexanoic acid, PFOA, and PFOS, respectively.

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References

  • Becker AM, Gerstmann S, Frank H (2008) Perfluorooctane surfactants in waste waters, the major source of river pollution. Chemosphere 72:115–121

    Article  CAS  Google Scholar 

  • Bossi R, Strand J, Sortkjær O, Larsen MM (2008) Perfluoroalkyl compounds in Danish wastewater treatment plants and aquatic environments. Environ Int 34:443–450

    Article  CAS  Google Scholar 

  • Boulanger B, Vargo JD, Schnoor JL, Hornbuckle K (2005) Evaluation of perfluorooctane surfactants in a wastewater treatment system and in a commercial surface protection product. Environ Sci Technol 39:5524–5530

    Article  CAS  Google Scholar 

  • Clara M, Scheffknecht C, Scharf S, Weiss S, Gans O (2008) Emissions of perfluorinated alkylated substances (PFAS) from point sources—identification of relevant branches. Water Sci Technol 58:59–66

    Article  CAS  Google Scholar 

  • D’Eon JC, Mabury SA (2007) Production of perfluorinated carboxylic acids (PFCAs) from the biotransformation of polyfluoroalkyl phosphate surfactants (PAPS): exploring routes of human contamination. Environ Sci Technol 41:4799–4805

    Article  Google Scholar 

  • Dinglasan MJA, Ye Y, Edwards EA, Mabury SA (2004) Fluorotelomer alcohol biodegradation yields polyfluorinated acids. Environ Sci Technol 38:2857–2864

    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 

  • Furdui VI, Crozier PW, Reiner EJ, Maburi SA (2008) Optimized trace level analysis of perfluorinated acids in the Great Lakes Watershed. Chemosphere 73:S24–S30

    Article  CAS  Google Scholar 

  • Guo R, Zhou Q, Cai Y, Jiang G (2008) Determination of perfluorooctanesulfonate and perfluorooctanoic acid in sewage sludge samples using liquid chromatography/quadrupole time-of-flight mass spectrometry. Talanta 75:1394–1399

    Article  CAS  Google Scholar 

  • Hekster FM, Laane RWPM, de Voogt P (2003) Environmental and toxicity effects of perfluoroalkylated substances. Rev Environ Contam Toxicol 179:99–121

    Article  CAS  Google Scholar 

  • Higgins CP, Field JA, Criddle CS, Luthy RG (2005) Evidence of perfluorochemicals in sediments and sludge. Environ Sci Technol 39:3946–3956

    Article  CAS  Google Scholar 

  • Higgins CP, Luthy RG (2006) Sorption of perfluorinated surfactants on sediments. Environ Sci Technol 40:7251–7256

    Article  CAS  Google Scholar 

  • Houde M, Martin JW, Letcher RJ, Solomon KR, Muir DCG (2006) Biological monitoring of polyfluoroalkyl compounds: a review. Environ Sci Technol 40:3463–3473

    Article  CAS  Google Scholar 

  • Huset CA, Chiaia AC, Barofsky DF, Jonkers N, Kohler HPE, Ort C, Giger W, Field JA (2008) Occurrence and mass flows of fluorochemicals in the Glatt Valley Watershed, Switzerland. Environ Sci Technol 42:6369–6377

    Article  CAS  Google Scholar 

  • Key BD, Howell RD, Criddle CS (1997) Fluorinated organics in the biosphere. Environ Sci Technol 31:2445–2454

    Article  CAS  Google Scholar 

  • Kissa E (2001) Fluorinated surfactants and repellents, 2nd edn. 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 

  • Lee H, D’Eon J, Mabury SA (2010) Biodegradation of polyfluoroalkyl phosphates as a source of perfluorinated acids to the environment. Environ Sci Technol 44:3305–3310

    Article  CAS  Google Scholar 

  • Li F, Zhang C, Qu Y, Chen J, Chen L, Liu Y, Zhou Q (2010) Quantitative characterization of short- and long-chain perfluorinated acids in solid matrices in Shanghai, China. Sci Total Environ 408:617–623

    Article  CAS  Google Scholar 

  • Li F, Sun H, Hao Z, He N, Zhao L, Zhang T, Sun T (2011a) Perfluorinated compounds in Haihe River and Dagu Drainage Canal in Tianjin, China. Chemosphere 84:265–271

    Article  CAS  Google Scholar 

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

    CAS  Google Scholar 

  • Loganathan BG, Sajwan KS, Sinclair E, Senthil KK, Kannan K (2007) Perfluoroalkyl sulfonates and perfluorocarboxylates in two wastewater treatment facilities in Kentucky and Georgia. Water Res 41:4611–4620

    Article  CAS  Google Scholar 

  • 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 45:5506–5513

    Article  CAS  Google Scholar 

  • Martin JW, Mabury SA, Solomon KR (2003) Bioconcentration and tissue distribution of perfluorinated acids in rainbow trout (Oncorhynchus mykiss). Environ Toxicol Chem 22:196–204

    CAS  Google Scholar 

  • Miyake Y, Yamashita N, So MK, Rostkowski P, Taniyasu S, Lam PKS, Kannan K (2007) Trace analysis of total fluorine in human blood using combustion ion chromatography for fluorine: A mass balance approach for the determination of known and unknown organofluorine compounds. J Chromatogr A 1154:214–221

    Article  CAS  Google Scholar 

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

    Article  Google Scholar 

  • Murakami M, Shinohara H, Takada H (2009) Evaluation of wastewater and street runoff as sources of perfluorinated surfactants (PFSs). Chemosphere 74:487–493

    Article  CAS  Google Scholar 

  • Paul AG, Jones KC, Sweetman AJ (2009) A first global production, emission, and environmental inventory for perfluorooctane sulfonate. Environ Sci Technol 43:386–392

    Article  CAS  Google Scholar 

  • Powley CR, George SW, Ryan TW, Buck RC (2005) Matrix effect free analytical methods for determination of perfluorinated carboxylic acids in environmental matrixes. Anal Chem 77:6353–6358

    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 

  • Schultz MM, Barofsky DF, Field JA (2006a) Quantitative determination of fluorinated alkyl substances by large-volume-injection liquid chromatography tandem mass spectrometry—characterization of municipal wastewaters. Environ Sci Technol 40:289–295

    Article  CAS  Google Scholar 

  • Schultz MM, Higgins CP, Huset CA, Duthy RG, Barofsky DF, Field JA (2006b) Fluorochemical mass flows in a municipal wastewater treatment facility. Environ Sci Technol 40:7350–7357

    Article  CAS  Google Scholar 

  • Shivakoti BR, Tanak S, Fuji S, Kunacheva C, Boontanon SK, Musirat C, Seneviratne ST, Tanaka H (2010) Occurrences and behavior of perfluorinated compounds (PFCs) in several wastewater treatment plants (WWTPs) in Japan and Thailand. J Environ Monitor 12:1255–1264

    Article  CAS  Google Scholar 

  • Sinclair E, Kannan K (2006) Mass loading and fate of perfluoroalkyl surfactants in wastewater treatment plants. Environ Sci Technol 40:1408–1414

    Article  CAS  Google Scholar 

  • Skutlarek D, Exner M, Farber H (2006) Perfluorinated surfactants in surface and drinking waters. Environ Sci Pollut Res 13:299–307

    Article  CAS  Google Scholar 

  • Sun H, Gerecke AC, Giger W, Alfredo AC (2010) Long-chain perfluorinated chemicals in digested sewage sludges in Switzerland. Environ Pollut 159:654–662

    Article  Google Scholar 

  • Sun H, Li F, Zhang T, Zhang X, He N, Song Q, Zhao L, Sun L, Sun T (2011) Perfluorinated compounds in surface waters and WWTPs in Shenyang, China: mass flows and source analysis. Water Res 45:4483–4490

    Article  CAS  Google Scholar 

  • Taniyasu S, Kannan K, So MK, Gulkowska A, Sinclair E, Okazawa T, Yamashita N (2005) A method for the analysis of fluorotelomer alcohols, fluorotelomer acids, and short- and long-chain perfluorinated acids in water and biota. J Chromatogr A 1093:89–97

    Article  CAS  Google Scholar 

  • UBW (2009) http://www.um.baden-wuerttemberg.de/servlet/is/63509

  • US EPA (2010) Long-chain perfluorinated chemicals (PFCs)—action plan summary. http://www.epa.gov/opptintr/existingchemicals/pubs/actionplans/pfcs.html

  • Wang N, Szostek B, Folsom PW, Sulecki LM, Capka V, Buck RC, Berti WR, Gannon JT (2005) 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, Szostek B, Buck RC, Folsom PW, Sulecki LM, Gannon JT (2009a) 8-2 fluorotelomer alcohol aerobic soil biodegradation: pathways, metabolites, and metabolite yields. Chemosphere 75:1089–1096

    Article  CAS  Google Scholar 

  • Wang T, Wang Y, Liao C, Cai Y, Jiang G (2009b) Perspectives on the inclusion of perfluorooctane sulfonate into the Stockholm Convention on persistent organic pollutants. Environ Sci Technol 43:5171–5175

    Article  CAS  Google Scholar 

  • You C, Jia CX, Pan G (2010) Effect of salinity and sediment characteristics on the sorption and desorption of perfluorooctane sulfonate at sediment–water interface. Environ Pollut 158:1343–1347

    Article  CAS  Google Scholar 

  • Yu J, Hu J, Tanaka S, Fujii S (2009) Perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA) in sewage treatment plants. Water Res 43:2399–2408

    Article  CAS  Google Scholar 

  • Zhang T, Wu Q, Sun H, Zhang X, Yun HS, Kannan K (2010) Perfluorinated compounds in whole blood samples from infants, children, and adults in China. Environ Sci Technol 44:4341–4347

    Article  CAS  Google Scholar 

  • Zhou Q, Deng S, Zhang Q, Fan Q, Huang J, Yu G (2010) Sorption of perfluorooctane sulfonate and perfluorooctanoate on activated sludge. Chemosphere 81:453–458

    Article  CAS  Google Scholar 

Download references

Acknowledgments

This paper was supported by the Ministry of Science and Technology (no. 2009DFA92390) and the Natural Science Foundation of China (no. 20877043). We are grateful to the WWTP authorities in Tianjin for permitting us to conduct sampling in WWTPs.

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Authors and Affiliations

  1. MOE Key Laboratory of Pollution Processes and Environmental Criteria, College of Environmental Science and Engineering, Nankai University, Tianjin, 300071, China

    Hongwen Sun, Lei Wang, Tao Zhang, Fasong Li & Na He

  2. Tianjin Fire Research Institute of Ministry of Public Security, Tianjin, 300381, China

    Xianzhong Zhang

  3. Swiss Federal Institute of Environmental Science and Technology (EAWAG), 8600, Dübendorf, Switzerland

    Alfredo C. Alder

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  1. Hongwen Sun
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  2. Xianzhong Zhang
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  3. Lei Wang
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  4. Tao Zhang
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  6. Na He
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  7. Alfredo C. Alder
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Correspondence to Hongwen Sun.

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Responsible editor: Ake Bergman

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Sun, H., Zhang, X., Wang, L. et al. Perfluoroalkyl compounds in municipal WWTPs in Tianjin, China—concentrations, distribution and mass flow. Environ Sci Pollut Res 19, 1405–1415 (2012). https://doi.org/10.1007/s11356-011-0727-6

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