Skip to main content
SpringerLink
Log in

Biomonitoring perfluorinated compounds in Catalonia, Spain: concentrations and trends in human liver and milk samples

  • AREA 6.4 • MONITORING AND FATE OF PERSISTENT CHEMICALS • RESEARCH ARTICLE
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

Background, aim and scope

Perfluorinated compounds (PFCs) are global environmental pollutants that bioaccumulate in wildlife and humans. Laboratory experiments have revealed toxic effects such as delayed development, humoral suppression, and hepatotoxicity. Although numerous human blood levels have been reported, little is known about distribution in the human body. Knowledge about PFC distribution and accumulation in the human body is crucial to understanding uptake and subsequent effects as well as to conduct risk assessments. The present study reports PFC levels in human liver and breast milk from a general population living in Catalonia, Spain. Liver and milk levels are compared to previously reported levels in blood from the same geographic area as well as to other existing reports on human liver and milk levels in other countries.

Materials and methods

Human liver (n = 12) and milk (n = 10) samples were collected in 2007 and 2008 in Catalonia, Spain. Liver samples were taken postmortem from six males and six females aged 27–79 years. Milk samples were from healthy primipara women (30–39 years old). Both liver and milk were analyzed by solid-phase extraction and ultra-performance liquid chromatography tandem mass spectrometry.

Results

Six PFCs were detected in liver, with perfluorooctanesulfonate (PFOS, 26.6 ng/g wet weight) being the chemical with the highest mean concentration. Other PFCs such as perfluorohexanesulfonate (PFHxS), perfluorooctanoic acid (PFOA), and acids with chain lengths up to C11 were also detected, with mean levels ranging between 0.50 and 1.45 ng/g wet weight. On the other hand, PFOS and PFHxS were the only PFCs detected in human milk, with mean concentrations of 0.12 and 0.04 ng/mL, respectively.

Discussion

While milk concentrations were similar to reported levels from other countries, liver samples contained more PFCs above quantification limits and higher PFOS concentrations compared to the only two other reports found in the literature. Differences between the results of the present study and those concerning previous investigations can be due to declining levels of some PFCs, which have been reported for the USA. The relationship between PFC concentrations in human liver, milk, and blood was assessed using blood concentrations previously determined in Catalonia. Those levels resulted in liver/serum ratios of 1.7:1, 1.4:1, and 2.1:1 for PFOS, perfluorodecanoic acid, and perfluoroundecanoic acid, respectively. Accumulation in liver is suggested for PFOS and the perfluorocarboxylic acids with carbon chain lengths C9, C10, and C11. For PFOA and PFHxS, fivefold and 14-fold higher concentrations, respectively, were seen in serum as compared to liver. The mean concentration of PFOS and PFHxS in milk was only 0.8% and 0.6% of the reported mean serum level, respectively.

Conclusions

The results of the present study show that several PFCs could be detected in human liver samples of subjects living in Tarragona. Concerning human milk, the mechanism by which PFCs are transferred from mother's blood to breast milk is still unclear. Considering that PFCs are strongly bound to the protein fraction in blood, the possibility of PFCs entering the milk and accumulating to levels observed in maternal plasma is limited.

Recommendations and perspectives

Interestingly, the potential accumulation difference for PFCs with different chain lengths might be of great importance for risk assessment. Continuing studies on the distribution of different PFCs in human tissue are therefore justified.

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

Similar content being viewed by others

References

  • Bernsmann T, Fürst P (2008) Determination of perfluorinated compounds in human milk. Organohalog Compd 70:718–721

    CAS  Google Scholar 

  • Butenhoff JL, Olsen GW, Pfahles-Hutchens A (2006) The applicability of biomonitoring data for perfluorooctanesulfonate to the environmental public health continuum. Environ Health Perspect 114:1776–1782

    CAS  Google Scholar 

  • Calafat AM, Kuklenyik Z, Caudill SP, Reidy JA, Needham LL (2006a) Perfluorochemicals in pooled serum samples from United States residents in 2001 and 2002. Environ Sci Technol 40:2128–2134

    Article  CAS  Google Scholar 

  • Calafat AM, Needham LL, Kuklenyik Z, Reidy JA, Tully JS, Aguilar-Villalobos M, Naeher LP (2006b) Perfluorinated chemicals in selected residents of the American continent. Chemosphere 63:490–496

    Article  CAS  Google Scholar 

  • Calafat AM, Kuklenyik Z, Reidy JA, Caudill SP, Tully JS, Needham LL (2007) Serum concentrations of 11 polyfluoroalkyl compounds in the U.S. population: data from the National Health and Nutrition Examination Survey (NHANES) 1999–2000. Environ Sci Technol 41:2237–2242

    Article  CAS  Google Scholar 

  • Cui L, Zhou QF, Liao CY, Fu JJ, Jiang GB (2009) Studies on the toxicological effects of PFOA and PFOS on rats using histological observation and chemical analysis. Arch Environ Contam Toxicol 56:338–349

    Article  CAS  Google Scholar 

  • Dauwe T, van de Vijver K, de Coen W, Eens M (2007) PFOS levels in the blood and liver of a small insectivorous songbird near a fluorochemical plant. Environ Int 33:357–361

    Article  Google Scholar 

  • EC (2002) Directive concerning the performance of analytical methods and the interpretation of results. European Commision decision of 12 August 2002. Council Directive 96/23/EC, notified under C(2002) 3044

  • Ericson I, Gomez M, Nadal M, van Bavel B, Lindström G, Domingo JL (2007) Perfluorinated chemicals in blood of residents in Catalonia (Spain) in relation to age and gender: a pilot study. Environ Int 33:616–623

    Article  Google Scholar 

  • Ericson I, Martí-Cid R, Nadal M, van Bavel B, Lindström G, Domingo JL (2008a) Human exposure to perfluorinated chemicals through the diet: intake of perfluorinated compounds in foods from the Catalan (Spain) market. J Agric Food Chem 56:1787–1794

    Article  CAS  Google Scholar 

  • Ericson I, Nadal M, van Bavel B, Lindström G, Domingo JL (2008b) Levels of perfluorochemicals in water samples from Catalonia, Spain: is drinking water a significant contribution to human exposure? Environ Sci Pollut Res 15:614–619

    Article  CAS  Google Scholar 

  • Fromme H, Midasch O, Twardella D, Angerer J, Boehmer S, Liebl B (2007a) Occurrence of perfluorinated substances in an adult German population in southern Bavaria. Int Arch Occup Environ Health 80:313–319

    Article  CAS  Google Scholar 

  • Fromme H, Schlummer M, Möller A, Gruber L, Wolz G, Ungewiss J, Böhmer S, Dekant W, Mayer R, Liebl B, Twardella D (2007b) Exposure of an adult population to perfluorinated substances using duplicate diet portions and biomonitoring data. Environ Sci Technol 41:7928–7933

    Article  CAS  Google Scholar 

  • Fromme H, Tittlemier SA, Völkel W, Wilhelm M, Twardella D (2009) Perfluorinated compounds—exposure assessment for the general population in western countries. Int J Hyg Environ Health 212:239–270

    Article  CAS  Google Scholar 

  • Fuentes S, Colomina MT, Vicens P, Domingo JL (2007) Influence of maternal restraint stress on the long-lasting effects induced by prenatal exposure to perfluorooctane sulfonate (PFOS) in mice. Toxicol Lett 171:162–170

    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 

  • Guruge KS, Manage PM, Yamanaka N, Miyazaki S, Taniyasu S, Yamashita N (2008) Species-specific concentrations of perfluoroalkyl contaminants in farm and pet animals in Japan. Chemosphere 73(1 Suppl):S210–S215

    Article  CAS  Google Scholar 

  • Harada K, Saito N, Inoue K, Yoshinaga T, Watanabe T, Sasaki S, Kamiyama S, Koizumi A (2004) The influence of time, sex and geographic factors on levels of perfluorooctane sulfonate and perfluorooctanoate in human serum over the last 25 years. J Occup Health 46:141–147

    Article  CAS  Google Scholar 

  • Harada K, Koizumi A, Saito N, Inoue K, Yoshinaga T, Date C, Fujii S, Hachiya N, Hirosawa I, Koda S, Lusaka Y, Murata K, Omae K, Shimbo S, Takenaka K, Takeshita T, Todoriki H, Wada Y, Watanabe T, Ikeda M (2007) Historical and geographical aspects of the increasing perfluorooctanoate and perfluorooctane sulfonate contamination in human serum in Japan. Chemosphere 66:293–301

    Article  CAS  Google Scholar 

  • Jensen AA, Leffers H (2008) Emerging endocrine disrupters: perfluoroalkylated substances. Int J Androl 31:161–169

    Article  CAS  Google Scholar 

  • Jin Y, Saito N, Harada KH, Inoue K, Koizumi A (2007) Historical trends in human serum levels of perfluorooctanoate and perfluorooctane sulfonate in Shenyang, China. Tohoku J Exp Med 212:63–70

    Article  CAS  Google Scholar 

  • Kannan K, Corsolini S, Falandysz J, Fillman G, Kumar KS, Loganathan BG, Mohd MA, Olivero J, van Wouwe N, Yang JH, Aldoust KM (2004) Perfluorooctanesulfonate and related fluorochemicals in human blood from several countries. Environ Sci Technol 38:4489–4495

    Article  CAS  Google Scholar 

  • Kannan K, Tao L, Sinclair E, Pastva SD, Jude DJ, Giesy JP (2005) Perfluorinated compounds in aquatic organisms at various trophic levels in a Great Lakes food chain. Arch Environ Contam Toxicol 48:559–566

    Article  CAS  Google Scholar 

  • Kärrman A, Mueller JF, van Bavel B, Harden F, Toms LM, Lindström G (2006a) Levels of 12 perfluorinated chemicals in pooled Australian serum collected 2002–2003 in relation to age, gender and region. Environ Sci Technol 40:3742–3748

    Article  CAS  Google Scholar 

  • Kärrman A, van Bavel B, Järnberg U, Hardell L, Lindström G (2006b) Perfluorinated chemicals in relation to other persistent organic pollutants in human blood. Chemosphere 64:1582–1591

    Article  CAS  Google Scholar 

  • Kärrman A, Langlois I, van Bavel B, Lindström G, Oehme M (2007a) Identification and pattern of perfluorooctane sulfonate (PFOS) isomers in human serum and plasma. Environ Int 33:782–788

    Article  CAS  Google Scholar 

  • Kärrman A, Ericson I, van Bavel B, Darnerud PO, Aune M, Glynn A, Lignell S, Lindström G (2007b) Exposure of perfluorinated chemicals through lactation: levels of matched human milk and serum and a temporal trend, 1996–2004, in Sweden. Environ Health Perspect 115:226–230

    Article  CAS  Google Scholar 

  • Kuklenyik Z, Reich JA, Tully JS, Needham LL, Calafat AM (2004) Automated solid-phase extraction and measurement of perfluorinated organic acids and amides in human serum and milk. Environ Sci Technol 38:3698–3704

    Article  CAS  Google Scholar 

  • Maestri L, Negri S, Ferrari M, Ghittori S, Fabris F, Danesino P, Imbriani M (2006) Determination of perfluorooctanoic acid and perfluorooctanesulfonate in human tissues by liquid chromatography/single quadrupole mass spectrometry. Rapid Commun Mass Spectrom 20:2728–2734

    Article  CAS  Google Scholar 

  • Midasch O, Schettgen T, Angerer J (2006) Pilot study on the perfluorooctanesulfonate and perfluorooctanoate exposure of the German general population. Int J Hyg Environ Health 209:489–496

    Article  CAS  Google Scholar 

  • Nakata A, Katsumata T, Iwasaki Y, Ito R, Saito K, Izumi S, Makino T, Kishi R, Nakazawa H (2007) Measurement of perfluorinated compounds in human milk and house dust. Organohalog Compd 69:2844–2846

    Google Scholar 

  • Nakayama K, Iwata H, Tao L, Kannan K, Imoto M, Kim EY, Tashiro K, Tanabe S (2008) Potential effects of perfluorinated compounds in common cormorants from Lake Biwa, Japan: an implication from the hepatic gene expression profiles by microarray. Environ Toxicol Chem 27:2378–2386

    Article  CAS  Google Scholar 

  • Olsen GW, Church TR, Miller JP, Burris JM, Hansen KJ, Lundberg JK, Armitage JB, Herron RM, Medhdizadehkashi Z, Nobiletti JB, O'Neill EM, Mandel JH, Zobel LR (2003a) Perfluorooctanesulfonate and other fluorochemicals in the serum of American Red Cross blood donors. Environ Health Perspect 111:1892–1901

    CAS  Google Scholar 

  • Olsen GW, Hansen KJ, Stevenson LA, Burris JM, Mandel JH (2003b) Human donor liver and serum concentrations of perfluorooctanesulfonate and other perfluorochemicals. Environ Sci Technol 37:888–891

    Article  CAS  Google Scholar 

  • Olsen GW, Mair DC, Church TR, Ellefson ME, Reagen WK, Boyd TM, Herron RM, Medhdizadehkashi Z, Nobiletti JB, Rios JA, Butenhoff JL, Zobel LR (2008) Decline in perfluorooctanesulfonate and other polyfluoroalkyl chemicals in American Red Cross adult blood donors, 2000–2006. Environ Sci Technol 42:4989–4995

    Article  CAS  Google Scholar 

  • Sáez M, de Voogt P, Parsons JR (2008) Persistence of perfluoroalkylated substances in closed bottle tests with municipal sewage sludge. Environ Sci Pollut Res 15:472–477

    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 

  • So MK, Yamashita N, Taniyasu S, Jiang Q, Giesy JP, Chen K, Lam PK (2006) Health risks in infants associated with exposure to perfluorinated compounds in human breast milk from Zhoushan, China. Environ Sci Technol 40:2924–2929

    Article  CAS  Google Scholar 

  • Strynar MJ, Lindstrom AB (2008) Perfluorinated compounds in house dust from Ohio and North Carolina, USA. Environ Sci Technol 42:3751–3756

    Article  CAS  Google Scholar 

  • Tao L, Kannan K, Aldous KM, Mauer MP, Eadon GA (2008) Biomonitoring of perfluorochemicals in plasma of New York State personnel responding to the World Trade Center disaster. Environ Sci Technol 42:3472–3478

    Article  CAS  Google Scholar 

  • Trudel D, Horowitz L, Wormuth M, Scheringer M, Cousins IT, Hungerbühler K (2008) Estimating consumer exposure to PFOS and PFOA. Risk Anal 28:251–269

    Article  Google Scholar 

  • Völkel W, Genzel-Boroviczény O, Demmelmair H, Gebauer C, Koletzko B, Twardella D, Raab U, Fromme H (2008) Perfluorooctane sulphonate (PFOS) and perfluorooctanoic acid (PFOA) in human breast milk: results of a pilot study. Int J Hyg Environ Health 211:440–446

    Article  CAS  Google Scholar 

  • Weber R (2007) 26th International Symposium on Halogenated Environmental Organic Pollutants and POPs (Dioxin 2006). Environ Sci Pollut Res 14:72–73

    Article  Google Scholar 

  • Wilhelm M, Kraft M, Rauchfuss K, Hölzer J (2008) Assessment and management of the first German case of a contamination with perfluorinated compounds (PFC) in the Region Sauerland, North Rhine-Westphalia. J Toxicol Environ Health A 71:725–733

    Article  CAS  Google Scholar 

  • Wilhelm M, Angerer J, Fromme H, Hölzer J (2009) Contribution to the evaluation of reference values for PFOA and PFOS in plasma of children and adults from Germany. Int J Hyg Environ Health 212:56–60

    Article  CAS  Google Scholar 

  • Yeung LW, So MK, Jiang G, Taniyasu S, Yamashita N, Song M, Wu Y, Li J, Giesy JP, Guruge KS, Lam PK (2006) Perfluorooctanesulfonate and related fluorochemicals in human blood samples from China. Environ Sci Technol 40:715–720

    Article  CAS  Google Scholar 

Download references

Acknowledgments

This study was financially supported by the Department of Health, Generalitat de Catalunya, Barcelona, Catalonia, Spain.

Author information

Authors and Affiliations

  1. Man-Technology-Environment Research Center (MTM), School of Science and Technology, Örebro University, 701 82, Örebro, Sweden

    Anna Kärrman, Bert van Bavel & Gunilla Lindström

  2. Laboratory of Toxicology and Environmental Health, ‘Rovira i Virgili’ University, Sant Llorenç 21, 43201, Reus, Catalonia, Spain

    José L. Domingo & Martí Nadal

  3. Health Protection Agency, Department of Health, Generalitat de Catalunya, Roc Boronat 81-95, 08005, Barcelona, Catalonia, Spain

    Xavier Llebaria & Esther Bigas

Authors
  1. Anna Kärrman
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. José L. Domingo
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Xavier Llebaria
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Martí Nadal
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Esther Bigas
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Bert van Bavel
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Gunilla Lindström
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to José L. Domingo.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Kärrman, A., Domingo, J.L., Llebaria, X. et al. Biomonitoring perfluorinated compounds in Catalonia, Spain: concentrations and trends in human liver and milk samples. Environ Sci Pollut Res 17, 750–758 (2010). https://doi.org/10.1007/s11356-009-0178-5

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-009-0178-5

Keywords

Search

Navigation