Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

Computational estimates of daily aggregate exposure to PFOA/PFOS from 2011 to 2017 using a basic intake model

Abstract

Background

Human exposure to per- and polyfluoroalkyl substances has been modeled to estimate serum concentrations. Given that the production and use of these compounds have decreased in recent years, especially PFOA and PFOS, and that additional concentration data have become available from the US and other industrialized countries over the past decade, aggregate median intakes of these two compounds were estimated using more recent data.

Methods

Summary statistics from secondary sources were collected, averaged, and mapped for indoor and outdoor air, water, dust, and soil for PFOA and PFOS to estimate exposures for adults and children. European dietary intake estimates were used to estimate daily intake from food.

Results

In accordance with decreased concentrations in media, daily intake estimates among adults, i.e., 40 ng/day PFOA and 40 ng/day PFOS, are substantially lower than those reported previously, as are children’s estimates of 14 ng/day PFOA and 17 ng/day PFOS. Using a first-order pharmacokinetic model, these results compare favorably to the National Health and Nutrition Examination Survey serum concentration measurements.

Conclusion

Concomitant blood concentrations support this enhanced estimation approach that captures the decline of PFOA/PFOS serum concentration over a decade.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Generalized demonstrated approach to assessing exposure in this paper.
Fig. 2: PFOA and PFOS exposure route boxplots for adults and children.
Fig. 3: The 2013-2014 NHANES serum concentration and model estimate for PFOA and PFOS in adults.
Fig. 4: A sensitivity analysis of steady-state and dynamical models for PFOA and PFOS in Adults with variation in volume of distribution (Vd), and the corresponding impact on the serum concentration (ng/mL).

Similar content being viewed by others

References

  1. Agency for Toxic Substances Disease Registry. Toxicological profile for perfluoroalkyls. Draft for public comment. Updated June 2018. Atlanta, Georgia: US Department of Health and Human Services, Public Health Service. http://www.atsdr.cdc.gov/toxprofiles/tp200.pdf (2018). Accessed 31 Aug 2020.

  2. US Environmental Protection Agency. Perfluoroalkyl sulfonates; Significant New Use Rule. 40 CFR 721 ed. Federal Register; 2002. 72854–67.

  3. US Environmental Protection Agency. PFAS action plan: program update February 2020, Research Triangle Park, North Carolina: Office of Air Quality Planning & Standards. Updated February 27, 2020. https://www.epa.gov/pfas/pfas-action-plan-program-update-february-2020 (2020). Accessed 31 Aug 2020.

  4. Egeghy PP, Lorber M. An assessment of the exposure of Americans to perfluorooctane sulfonate: a comparison of estimated intake with values inferred from NHANES data. J Exposure Sci Environ Epidemiol. 2011;21:150–68.

    Article  CAS  Google Scholar 

  5. Lorber M, Egeghy PP. Simple intake and pharmacokinetic modeling to characterize exposure of Americans to perfluoroctanoic acid, PFOA. Environ Sci Technol. 2011;45:8006–14.

    Article  CAS  Google Scholar 

  6. Vallero D. Translating diverse environmental data into reliable information: how to coordinate evidence from different sources. Amsterdam, The Netherlands;Academic Press; 2017.

  7. Vestergren R, Cousins IT. Tracking the pathways of human exposure to perfluorocarboxylates. Environ Sci Technol. 2009;43:5565–75.

    Article  CAS  Google Scholar 

  8. Domingo JL. Health risks of dietary exposure to perfluorinated compounds. Environ Int. 2012;40:187–95.

    Article  CAS  Google Scholar 

  9. Haug LS, Huber S, Becher G, Thomsen C. Characterisation of human exposure pathways to perfluorinated compounds—comparing exposure estimates with biomarkers of exposure. Environ Int. 2011;37:687–93.

    Article  CAS  Google Scholar 

  10. Hornung RW, Reed LD. Estimation of average concentration in the presence of nondetectable values. Appl Occup Environ Hyg. 1990;5:46–51.

    Article  CAS  Google Scholar 

  11. Pleil JD, Sobus JR, Stiegel MA, Hu D, Oliver KD, Olenick C, et al. Estimating common parameters of lognormally distributed environmental and biomonitoring data: Harmonizing disparate statistics from publications. J Toxicol Environ health Part B. 2014;17:341–68.

    Article  CAS  Google Scholar 

  12. Hozo SP, Djulbegovic B, Hozo I. Estimating the mean and variance from the median, range, and the size of a sample. BMC Med Res Methodol. 2005;5:13.

    Article  Google Scholar 

  13. Ramirez A, Cox C. Improving on the range rule of thumb. Rose-Hulman Undergrad Math J. 2012;13:1.

    Google Scholar 

  14. Strom DJ, Stansbury PS. Determining parameters of lognormal distributions from minimal information. AIHAJ. 2000;61:877–80.

    Article  CAS  Google Scholar 

  15. Ott WR. A physical explanation of the lognormality of pollutant concentrations. J Air Waste Manag Assoc. 1990;40:1378–83.

    Article  CAS  Google Scholar 

  16. Lorber M. Exposure of Americans to polybrominated diphenyl ethers. J Exposure Sci Environ Epidemiol. 2008;18:2–19.

    Article  CAS  Google Scholar 

  17. US Environmental Protection Agency. Exposure factors handbook. Washington, DC: Office of Research and Development; 1997;20460:2–6..

  18. US Environmental Protection Agency. Child-specific exposure factors handbook (final report). Washington, DC: National Center for Environmental Assessment, Office of Research and Development (EPA/600/R-08/135); 2008.

  19. Pang Y, MacIntosh DL, Camann DE, Ryan PB. Analysis of aggregate exposure to chlorpyrifos in the NHEXAS-Maryland investigation. Environ Health Perspect. 2002;110:235–40.

    Article  CAS  Google Scholar 

  20. Hubal EAC, Egeghy PP, Leovic KW, Akland GG. Measuring potential dermal transfer of a pesticide to children in a child care center. Environ Health Perspect. 2006;114:264–9.

    Article  Google Scholar 

  21. Fasano W, Kennedy G, Szostek B, Farrar D, Ward R, Haroun L, et al. Penetration of ammonium perfluorooctanoate through rat and human skin in vitro. Drug Chem Toxicol. 2005;28:79–90.

    Article  CAS  Google Scholar 

  22. US Environmental Protection Agency. Exposure factors handbook – soil and dust ingestion. ExpoBox. https://www.epa.gov/expobox/exposure-factors-handbook-chapter-5 (2017).

  23. Knutsen HK, Alexander J, Barregård L, Bignami M, Brüschweiler B, Ceccatelli S, et al. Risk to human health related to the presence of perfluorooctane sulfonic acid and perfluorooctanoic acid in food. EFSA J. 2018;16:e05194.

    Google Scholar 

  24. Vestergren R, Orata F, Berger U, Cousins IT. Bioaccumulation of perfluoroalkyl acids in dairy cows in a naturally contaminated environment. Environ Sci Pollut Res. 2013;20:7959–69.

    Article  CAS  Google Scholar 

  25. Thompson J, Lorber M, Toms L-ML, Kato K, Calafat AM, Mueller JF. Use of simple pharmacokinetic modeling to characterize exposure of Australians to perfluorooctanoic acid and perfluorooctane sulfonic acid. Environ Int. 2010;36:390–7.

    Article  CAS  Google Scholar 

  26. Bartell SM, Calafat AM, Lyu C, Kato K, Ryan PB, Steenland K. Rate of decline in serum PFOA concentrations after granular activated carbon filtration at two public water systems in Ohio and West Virginia. Environ Health Perspect. 2010;118:222–8.

    Article  CAS  Google Scholar 

  27. Olsen GW, Burris JM, Ehresman DJ, Froehlich JW, Seacat AM, Butenhoff JL, et al. Half-life of serum elimination of perfluorooctanesulfonate, perfluorohexanesulfonate, and perfluorooctanoate in retired fluorochemical production workers. Environ Health Perspect. 2007;115:1298–305.

    Article  CAS  Google Scholar 

  28. Calafat AM, Wong L-Y, Kuklenyik Z, Reidy JA, Needham LL. Polyfluoroalkyl chemicals in the US population: data from the National Health and Nutrition Examination Survey (NHANES) 2003–2004 and comparisons with NHANES 1999–2000. Environ Health Perspect. 2007;115:1596–602.

    Article  CAS  Google Scholar 

  29. Xiao F, Simcik MF, Halbach TR, Gulliver JS. Perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA) in soils and groundwater of a US metropolitan area: migration and implications for human exposure. Water Res. 2015;72:64–74.

    Article  CAS  Google Scholar 

  30. Rankin K, Mabury SA, Jenkins TM, Washington JW. A North American and global survey of perfluoroalkyl substances in surface soils: distribution patterns and mode of occurrence. Chemosphere. 2016;161:333–41.

    Article  CAS  Google Scholar 

  31. Tittlemier SA, Pepper K, Seymour C, Moisey J, Bronson R, Cao X-L, et al. Dietary exposure of Canadians to perfluorinated carboxylates and perfluorooctane sulfonate via consumption of meat, fish, fast foods, and food items prepared in their packaging. J Agric Food Chem. 2007;55:3203–10.

    Article  CAS  Google Scholar 

  32. Fromme H, Tittlemier SA, Völkel W, Wilhelm M, Twardella D. Perfluorinated compounds–exposure assessment for the general population in western countries. Int J Hyg Environ Health. 2009;212:239–70.

    Article  CAS  Google Scholar 

  33. Endres CJ. nhanesA: NHANES data retrieval. 2021 https://cran.r-project.org/web/packages/nhanesA/vignettes/Introducing_nhanesA.html2021. Accessed 31 Mar 2021.

  34. R Core Team. R: a language and environment for statistical computing. Computing RFfS, editor. R Core Team: Vienna, Austria; 2019.

  35. Shoeib M, Harner T, Webster MG, Lee SC. Indoor sources of poly-and perfluorinated compounds (PFCS) in Vancouver, Canada: implications for human exposure. Environ Sci Technol. 2011;45:7999–8005.

    Article  CAS  Google Scholar 

  36. Eriksson U, Kärrman A. World-wide indoor exposure to polyfluoroalkyl phosphate esters (PAPs) and other PFASs in household dust. Environ Sci Technol. 2015;49:14503–11.

    Article  CAS  Google Scholar 

  37. Fraser AJ, Webster TF, Watkins DJ, Strynar MJ, Kato K, Calafat AM, et al. Polyfluorinated compounds in dust from homes, offices, and vehicles as predictors of concentrations in office workers’ serum. Environ Int. 2013;60:128–36.

    Article  CAS  Google Scholar 

  38. Goosey E, Harrad S. Perfluoroalkyl compounds in dust from Asian, Australian, European, and North American homes and UK cars, classrooms, and offices. Environ Int. 2011;37:86–92.

    Article  CAS  Google Scholar 

  39. Karásková P, Venier M, Melymuk L, Bečanová J, Vojta Š, Prokeš R, et al. Perfluorinated alkyl substances (PFASs) in household dust in Central Europe and North America. Environ Int. 2016;94:315–24.

    Article  Google Scholar 

  40. Knobeloch L, Imm P, Anderson H. Perfluoroalkyl chemicals in vacuum cleaner dust from 39 Wisconsin homes. Chemosphere. 2012;88:779–83.

    Article  CAS  Google Scholar 

  41. Lankova D, Svarcova A, Kalachova K, Lacina O, Pulkrabova J, Hajslova J. Multi-analyte method for the analysis of various organohalogen compounds in house dust. Analytica Chim Acta. 2015;854:61–9.

    Article  CAS  Google Scholar 

  42. Xu Z, Fiedler S, Pfister G, Henkelmann B, Mosch C, Völkel W, et al. Human exposure to fluorotelomer alcohols, perfluorooctane sulfonate and perfluorooctanoate via house dust in Bavaria, Germany. Sci Total Environ. 2013;443:485–90.

    Article  CAS  Google Scholar 

  43. Winkens K, Koponen J, Schuster J, Shoeib M, Vestergren R, Berger U, et al. Perfluoroalkyl acids and their precursors in indoor air sampled in children’s bedrooms. Environ Pollut. 2017;222:423–32.

    Article  CAS  Google Scholar 

  44. Llorca M, Farré M, Picó Y, Müller J, Knepper TP, Barceló D. Analysis of perfluoroalkyl substances in waters from Germany and Spain. Sci Total Environ. 2012;431:139–50.

    Article  CAS  Google Scholar 

  45. Schwanz TG, Llorca M, Farré M, Barceló D. Perfluoroalkyl substances assessment in drinking waters from Brazil, France and Spain. Sci Total Environ. 2016;539:143–52.

    Article  CAS  Google Scholar 

  46. Shafique U, Schulze S, Slawik C, Böhme A, Paschke A, Schüürmann G. Perfluoroalkyl acids in aqueous samples from Germany and Kenya. Environ Sci Pollut Res. 2017;24:11031–43.

    Article  CAS  Google Scholar 

  47. Ullah S, Alsberg T, Berger U. Simultaneous determination of perfluoroalkyl phosphonates, carboxylates, and sulfonates in drinking water. J Chromatogr A. 2011;1218:6388–95.

    Article  CAS  Google Scholar 

  48. Strynar MJ, Lindstrom AB. Perfluorinated compounds in house dust from Ohio and North Carolina, USA. Environ Sci Technol. 2008;42:3751–6.

    Article  CAS  Google Scholar 

  49. Hu XC, Andrews DQ, Lindstrom AB, Bruton TA, Schaider LA, Grandjean P, et al. Detection of poly-and perfluoroalkyl substances (PFASs) in US drinking water linked to industrial sites, military fire training areas, and wastewater treatment plants. Environ Sci Technol Lett. 2016;3:344–50.

    Article  CAS  Google Scholar 

  50. Nguyen VK, Kahana A, Heidt J, Polemi K, Kvasnicka J, Jolliet O, et al. A comprehensive analysis of racial disparities in chemical biomarker concentrations in United States women, 1999–2014. Environ Int. 2020;137:105496.

    Article  CAS  Google Scholar 

  51. Hu XC, Tokranov AK, Liddie J, Zhang X, Grandjean P, Hart JE, et al. Tap water contributions to plasma concentrations of poly-and perfluoroalkyl substances (PFAS) in a nationwide prospective cohort of US women. Environ Health Perspect. 2019;127:067006.

    Article  Google Scholar 

  52. Dionisio KL, Frame AM, Goldsmith M-R, Wambaugh JF, Liddell A, Cathey T, et al. Exploring consumer exposure pathways and patterns of use for chemicals in the environment. Toxicol Rep. 2015;2:228–37.

    Article  CAS  Google Scholar 

  53. US Environmental Protection Agency. Overview of PFAS actions under TSCA: Office of Air Quality Planning & Standards. Updated August 10, 2020. https://www.epa.gov/assessing-and-managing-chemicals-under-tsca/risk-management-and-polyfluoroalkyl-substances-pfas (2020). Accessed 28 Sept 2020.

  54. European Environment Agency. Emerging chemical risks in Europe—‘PFAS’. https://www.eea.europa.eu/themes/human/chemicals/emerging-chemical-risks-in-europe (2020). Accessed 28 Sept 2020.

  55. European Comission. Directive of the European Parliament and of the Council on the quality of water intended for human consumption. 2017. https://eur-lex.europa.eu/resource.html?uri=cellar:8c5065b2-074f-11e8-b8f5-01aa75ed71a1.0016.02/DOC_1&format=PDF. Accessed 6 Oct 2020.

  56. Balk FG, Pütz KW, Ribbenstedt A, Gomis MI, Filipovic M, Cousins IT. Children’s exposure to perfluoroalkyl acids–a modelling approach. Environ Sci Process Impacts. 2019;21:1875–86.

    Article  CAS  Google Scholar 

  57. Barton KE, Starling AP, Higgins CP, McDonough CA, Calafat AM, Adgate JL. Sociodemographic and behavioral determinants of serum concentrations of per-and polyfluoroalkyl substances in a community highly exposed to aqueous film-forming foam contaminants in drinking water. Int J Hyg Environ Health. 2020;223:256–66.

    Article  CAS  Google Scholar 

  58. Agency for Toxic Substances and Disease Registry. Toxicological profile for perfluoroalkyls. Draft for public comment. Atlanta, GA: Department of Health and Human Services, Public Health Service, United States Department of Health and Human Services. https://www.atsdr.cdc.gov/substances/toxsubstance.asp?toxid=237 (2015).

  59. Agency for Toxic Substances and Disease Registry. Toxicological Profile for Perfluoroalkyls. 2021. https://www.atsdr.cdc.gov/toxprofiles/tp200.pdf. Accessed 5 Aug 2021.

  60. Liu X. Characterise sources for exposure assessment of chemicals in indoor environment. London, England: SAGE Publications Sage UK; 2018.

  61. Gebbink WA, Berger U, Cousins IT. Estimating human exposure to PFOS isomers and PFCA homologues: the relative importance of direct and indirect (precursor) exposure. Environ Int. 2015;74:160–9.

    Article  CAS  Google Scholar 

  62. Vestergren R, Cousins IT, Trudel D, Wormuth M, Scheringer M. Estimating the contribution of precursor compounds in consumer exposure to PFOS and PFOA. Chemosphere. 2008;73:1617–24.

    Article  CAS  Google Scholar 

  63. Xiao F, Hanson RA, Golovko SA, Golovko MY, Arnold WA. PFOA and PFOS are generated from zwitterionic and cationic precursor compounds during water disinfection with chlorine or ozone. Environ Sci Technol Lett. 2018;5:382–8.

    Article  CAS  Google Scholar 

  64. Butenhoff J, Kennedy G Jr, Hinderliter P, Lieder P, Jung R, Hansen K, et al. Pharmacokinetics of perfluorooctanoate in cynomolgus monkeys. Toxicological Sci. 2004;82:394–406.

    Article  CAS  Google Scholar 

  65. Andersen ME, Clewell HJ III, Tan Y-M, Butenhoff JL, Olsen GW. Pharmacokinetic modeling of saturable, renal resorption of perfluoroalkylacids in monkeys—probing the determinants of long plasma half-lives. Toxicology. 2006;227:156–64.

    Article  CAS  Google Scholar 

  66. Harada K, Saito N, Sasaki K, Inoue K, Koizumi A. Perfluorooctane sulfonate contamination of drinking water in the Tama River, Japan: estimated effects on resident serum levels. Bull Environ Contamination Toxicol. 2003;71:0031–6.

    Article  CAS  Google Scholar 

  67. Trudel D, Horowitz L, Wormuth M, Scheringer M, Cousins IT, Hungerbühler K. Estimating consumer exposure to PFOS and PFOA. Risk Anal. 2008;28:251–69.

    Article  Google Scholar 

  68. Gomis MI, Vestergren R, MacLeod M, Mueller JF, Cousins IT. Historical human exposure to perfluoroalkyl acids in the United States and Australia reconstructed from biomonitoring data using population-based pharmacokinetic modelling. Environ Int. 2017;108:92–102.

    Article  CAS  Google Scholar 

  69. US Environmental Protection Agency. Basic information on PFAS. Research Triangle Park, North Carolina: Office of Air Quality Planning & Standards. Updated December 6, 2018. https://www.epa.gov/pfas/basic-information-pfas (2018).

Download references

Acknowledgements

Paul Schlosser, Rocky Goldsmith, Rogelio Tornero-Velez, and Andrew Gillespie of EPA’s Office of Research and Development provided vital reviews and advice, especially on enhancements of the PK model and sensitivity analysis. This work built upon PFAS data curation work led by Valerie Zartarian. This research was supported by the National Student Service Contract Number 68HERH20D0003. The research was also supported by student service contractor Hunter Fisher and Pathways intern Ashley Mullikin. The curation, analysis, and presentation in this study adhered to an approved quality assurance project plan, which was developed with advice from EPA’s James Noel.

Author information

Authors and Affiliations

Authors

Contributions

AE, with input from his co-authors, drafted and revised the manuscript. He led the analysis, including coding in R and developing repositories in GitHub. He applied statistical methods and updated and revised the pharmacokinetic model. PPE provided input files from his previous work in PFOA and PFOS model development. He also provided expertise to AE and DAV in the data analysis, especially on the application of statistical methods and algorithm-based modeling of route-specific exposure and intake, and model parameterization. RS conducted the initial PFAS literature screening, data curation, quality assurance of literature review, data analysis, and reporting. EACH provided oversight and advice of the model development, curation, and application of the PFAS screening results and reports, which represented a substantial source of secondary data included in the input files, initial outline, and extensive review and edits to the manuscript. As EPA’s student service contract mentor, DAV assisted AE in analyzing data, interpreting statistical results, conducting literature reviews, and providing scientific expertise on PFAS. DAV also ensured that all work met the requirements of the quality assurance project plan.

Corresponding author

Correspondence to Daniel A. Vallero.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

East, A., Egeghy, P.P., Hubal, E.A.C. et al. Computational estimates of daily aggregate exposure to PFOA/PFOS from 2011 to 2017 using a basic intake model. J Expo Sci Environ Epidemiol 33, 56–68 (2023). https://doi.org/10.1038/s41370-021-00374-w

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41370-021-00374-w

Keyword

Search

Quick links