Trends in Exposure to Polyfluoroalkyl Chemicals in the U.S. Population: 1999−2008
Abstract
Since 2002, practices in manufacturing polyfluoroalkyl chemicals (PFCs) in the United States have changed. Previous results from the National Health and Nutrition Examination Survey (NHANES) documented a significant decrease in serum concentrations of some PFCs during 1999-2004. To further assess concentration trends of perfluorooctane sulfonate (PFOS), perfluorooctanoate (PFOA), perfluorohexane sulfonate (PFHxS), and perfluorononanoate (PFNA), we analyzed 7876 serum samples collected from a representative sample of the general U.S. population ≥12 years of age during NHANES 1999-2008. We detected PFOS, PFOA, PFNA, and PFHxS in more than 95% of participants. Concentrations differed by sex regardless of age and we observed some differences by race/ethnicity. Since 1999-2000, PFOS concentrations showed a significant downward trend, because of discontinuing industrial production of PFOS, but PFNA concentrations showed a significant upward trend. PFOA concentrations during 1999-2000 were significantly higher than during any other time period examined, but PFOA concentrations have remained essentially unchanged during 2003-2008. PFHxS concentrations showed a downward trend from 1999 to 2006, but concentrations increased during 2007-2008. Additional research is needed to identify the environmental sources contributing to human exposure to PFCs. Nonetheless, these NHANES data suggest that sociodemographic factors may influence exposure and also provide unique information on temporal trends of exposure.
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Levels of PFOS and PFOA in human blood samples have declined in many Western countries as a consequence of phase-out actions and regulations.
“As a consequence of phase-out actions and regulations, levels of PFOS and PFOA in human blood samples have now declined in many Western countries (Glynn et al., 2012;Kato et al., 2011;Harada et al., 2010;Yeung et al., 2013a).”
From Helsingør Statement on poly- and perfluorinated alkyl substances (PFASs) (2014) · cites this paper as Kato et al., 2011
PFCAs with longer perfluorinated chains than PFOA (8 or more perfluoroalkyl carbons) have not yet shown signs of decline in human blood samples globally.
“However, PFCAs with longer perfluorinated chains than PFOA, with 8 or more perfluoroalkyl carbons, have not yet shown signs of decline in human blood samples globally (Kato et al., 2011;Glynn et al., 2012;Yeung et al., 2013b).”
From Helsingør Statement on poly- and perfluorinated alkyl substances (PFASs) (2014) · cites this paper as Kato et al., 2011
The declines in serum PFNA, PFDA and PFUnA in Gullah African Americans are most likely a local phenomenon rather than consistent with NHANES trends among non-hispanic blacks.
“Based on the increasing temporal trends of PFNA presented by Kato et al. [103] for non-hispanic blacks, we suggest the former explanation is most likely, that this is indeed a local phenomenon.”
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“Therefore, not surprisingly, PFAS compounds, such as PFOA, PFOS and PFHxS, are detected in the blood samples of more than 95% of the general US population (Kato et al., 2011).”
BackgroundPFOS-induced hepatic steatosis, the mechanistic actions on β-oxidation and lipid transport
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“…samples are now slowly decreasing making the general population in these areas less susceptible to potential harmful exposure (e.g. Donaldson et al., 2010; Hardell et al., 2010; Hart et al., 2008; Haug et al., 2009; Kato et al., 2011; Olsen et al., 2005; Sundström et al., 2011; Zushi et al., 2010).”
BackgroundVandenberg, L. N., Colborn, T., Hayes, T. B., Heindel, J. J., Jacobs, D. R., Lee, D., Myers, J. P., Shioda, T., Soto, A. M., Saal, F. S. V., et al. (2013) · Reproductive Toxicology · doi:10.1016/j.reprotox.2013.02.002 · Cited by 208 · see citing works
Assessing Human Exposure to Organic Pollutants in the Indoor Environment
Salthammer, T., Zhang, Y., Mo, J., Koch, H. M., & Weschler, C. J. (2018) · Angewandte Chemie International Edition · doi:10.1002/anie.201711023 · Cited by 207 · see citing works
Joensen, U. N., Veyrand, B., Antignac, J., Jensen, M. B., Petersen, J. H., Marchand, P., Skakkebæk, N. E., Andersson, A., Bizec, B. L., & Jørgensen, N. (2012) · Human Reproduction · doi:10.1093/humrep/des425 · Cited by 203 · see citing works
“The temporal decrease in serum PFOS and PFOA levels is consistent with observations in other studies (Kato et al., 2011) and a beneficial effect of the voluntary phase-out of production by the major manufacturer (3M Company) in 2002, and later regulatory measures (US Environmental Protection Agency 2012).”
ResultPerfluoroalkyl substances and fish consumption
Christensen, K. L. Y., Raymond, M., Blackowicz, M. J., Liu, Y., Thompson, B. A., Anderson, H. A., & Turyk, M. E. (2017) · Environmental Research · doi:10.1016/j.envres.2016.12.032 · Cited by 202 · see citing works
Fate and redistribution of perfluoroalkyl acids through AFFF-impacted groundwater
Bräunig, J., Baduel, C., Heffernan, A., Rotander, A., Donaldson, E., & Mueller, J. F. (2017) · Science of The Total Environment · doi:10.1016/j.scitotenv.2017.04.095 · Cited by 199 · see citing works
“, 2014) and the 95th percentile for the US American general populations (Kato et al., 2011).”
BackgroundInfluentialPenetration of PFASs Across the Blood Cerebrospinal Fluid Barrier and Its Determinants in Humans
Wang, J., Pan, Y., Cui, Q., Yao, B., Wang, J., & Dai, J. (2018) · Environmental Science & Technology · doi:10.1021/acs.est.8b04550 · Cited by 192 · see citing works
Dong, G., Tung, K., Tsai, C., Liu, M.-M., Wang, D., Liu, W., Jin, Y., Hsieh, W., Lee, Y. L., & Chen, P. (2013) · Environmental Health Perspectives · doi:10.1289/ehp.1205351 · Cited by 193 · see citing works
Thyroid disruption by perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA)
Coperchini, F., Awwad, O., Rotondi, M., Santini, F., Imbriani, M., & Chiovato, L. (2016) · Journal of Endocrinological Investigation · doi:10.1007/s40618-016-0572-z · Cited by 192 · see citing works
Xiao, F., Halbach, T. R., Simcik, M. F., & Gulliver, J. S. (2012) · Water Research · doi:10.1016/j.watres.2012.03.027 · Cited by 191 · see citing works
Beesoon, S., Webster, G. M., Shoeib, M., Harner, T., Benskin, J. P., & Martin, J. W. (2011) · Environmental Health Perspectives · doi:10.1289/ehp.1003265 · Cited by 188 · see citing works
“…(Olsen et al. 2008), and the most recent data from the National Center of Health Statistics of the U.S. Centers for Disease Control and Prevention (Kato et al. 2011) indicate that serum PFOA did not decline between April 2003 and August 2007 and may be increasing [see Supplemental Material,…”
BackgroundInfluentialPersistent Environmental Pollutants and Couple Fecundity: The LIFE Study
Louis, G. M. B., Sundaram, R., Schisterman, E. F., Sweeney, A., Lynch, C. D.-J., Gore‐Langton, R. E., Maisog, J. M., Kim, S., Chen, Z., & Barr, D. B. (2012) · Environmental Health Perspectives · doi:10.1289/ehp.1205301 · Cited by 189 · see citing works
“…were measured using isotope dilution highresolution mass spec trometry for OCPs, PBBs, PBDEs, and PCBs, and isotope dilution tandem mass spectrometry for PFCs, following standard published operat ing procedures as described previously (Kato et al. 2011; Kuklenyik et al. 2005; Sjödin et al 2004).”
MethodMaternal exposure to perfluorinated chemicals and reduced fecundity: the MIREC study
Vélez, M. P., Arbuckle, T. E., & Fraser, W. D. (2015) · Human Reproduction · doi:10.1093/humrep/deu350 · Cited by 187 · see citing works
Gleason, J. A., Post, G. B., & Fagliano, J. A. (2014) · Environmental Research · doi:10.1016/j.envres.2014.10.004 · Cited by 184 · see citing works
Stein, C. R., McGovern, K. J., Pajak, A., Maglione, P. J., & Wolff, M. S. (2015) · Pediatric Research · doi:10.1038/pr.2015.213 · Cited by 186 · see citing works
“While efforts to reduce US production and use of these compounds (12,13) have led to declining serum concentrations, compounds such as perfluorononanoate (PFNA) have been increasing in both percent of the population with detectable levels and average serum concentration (14).”
BackgroundMethodKato, K., Wong, L.-Y., Chen, A., Dunbar, C. A., Webster, G. M., Lanphear, B. P., & Calafat, A. M. (2014) · Environmental Science & Technology · doi:10.1021/es501811k · Cited by 182 · see citing works
Self-citationChang, E. T., Adami, H.-O., Boffetta, P., Cole, P., Starr, T. B., & Mandel, J. S. (2014) · Critical Reviews in Toxicology · doi:10.3109/10408444.2014.905767 · Cited by 180 · see citing works
“[By comparison, contemporaneous geometric mean serum PFOS levels in the general population were approximately 30 – 35 ng/mL (Kato et al. 2011, Olsen et al. 2012).]”
BackgroundInfluentialPark, S. K., Peng, Q., Ding, N., Mukherjee, B., & Harlow, S. D. (2019) · Environmental Research · doi:10.1016/j.envres.2019.05.028 · Cited by 179 · see citing works
“We used the method with a modification described previously (Kato et al. 2011a).”
BackgroundMethodSagiv, S. K., Rifas‐Shiman, S. L., Webster, T. F., Mora, A. M., Harris, M. H., Calafat, A. M., Ye, X., Gillman, M. W., & Oken, E. (2015) · Environmental Science & Technology · doi:10.1021/acs.est.5b02489 · Cited by 178 · see citing works
Self-citationWinquist, A. G., & Steenland, K. (2014) · Environmental Health Perspectives · doi:10.1289/ehp.1307943 · Cited by 175 · see citing works
Perfluorinated Alkyl Substances
Grandjean, P., & Clapp, R. (2015) · NEW SOLUTIONS A Journal of Environmental and Occupational Health Policy · doi:10.1177/1048291115590506 · Cited by 181 · see citing works
Sun, Q., Zong, G., Valvi, D., Nielsen, F., Coull, B. A., & Grandjean, P. (2018) · Environmental Health Perspectives · doi:10.1289/ehp2619 · Cited by 175 · see citing works
“Blood concentrations of these ubiquitous environmental pollutants are declining in Americans overall, but they remain detectable in almost the entire population (Calafat et al. 2007; Kato et al. 2011; Liu et al. 2018; Olsen et al. 2017).”
BackgroundChen, Z., Yang, T., Walker, D. I., Thomas, D. C., Qiu, C., Chatzi, L., Alderete, T. L., Kim, J. S., Conti, D. V., Breton, C. V., et al. (2020) · Environment International · doi:10.1016/j.envint.2020.106091 · Cited by 176 · see citing works
“A recent study has shown ubiquitous exposures to major PFASs, such as perfluorooctanoic acid (PFOA), perfluorooctane sulfonate (PFOS), and perfluorohexane sulfonic acid (PFHxS) among the US population (Kato et al., 2011).”
BackgroundComparative pharmacokinetics of perfluorohexanesulfonate (PFHxS) in rats, mice, and monkeys
Sundström, M., Chang, S., Noker, P. E., Gorman, G. S., Hart, J. A., Ehresman, D. J., Bergman, Å., & Butenhoff, J. L. (2011) · Reproductive Toxicology · doi:10.1016/j.reprotox.2011.07.004 · Cited by 175 · see citing works
Yao, J., Pan, Y., Sheng, N., Su, Z., Guo, Y., Wang, J., & Dai, J. (2020) · Environmental Science & Technology · doi:10.1021/acs.est.0c02888 · Cited by 174 · see citing works
Zhao, Z., Xie, Z., Möller, A., Sturm, R., Tang, J., Zhang, G., & Ebinghaus, R. (2012) · Environmental Pollution · doi:10.1016/j.envpol.2012.06.004 · Cited by 173 · see citing works
“PFASs have been detected ubiquitously in air, water, sediment, wildlife and human beings all around the world as a result of their decades-long manufacture and applications (Schiavone et al., 2009; Bao et al., 2010; Genualdi et al., 2010; Kato et al., 2011; Li et al., 2011; Meyer et al., 2011).”
BackgroundChang, E. T., Adami, H., Boffetta, P., Wedner, H. J., & Mandel, J. S. (2016) · Critical Reviews in Toxicology · doi:10.3109/10408444.2015.1122573 · Cited by 174 · see citing works
Liu, G., Dhana, K., Furtado, J. D., Rood, J. C., Zong, G., Liang, L., Qi, L., Bray, G. A., de Jonge, L., Coull, B. A., et al. (2018) · PLoS Medicine · doi:10.1371/journal.pmed.1002502 · Cited by 177 · see citing works
“Although the production of PFOS and PFOA in the US has largely been phased out [31,63], the production of other PFASs, such as PFNA, may continue or even increase, especially in developing countries [64].”
BackgroundPerfluorooctanoic Acid Exposure and Pregnancy Outcome in a Highly Exposed Community
Savitz, D., Stein, C. R., Bartell, S., Elston, B., Gong, J., Shin, H.-M., & Wellenius, G. (2012) · Epidemiology · doi:10.1097/ede.0b013e31824cb93b · Cited by 163 · see citing works
Starling, A. P., Engel, S. M., Whitworth, K. W., Richardson, D. B., Stuebe, A. M., Daniels, J. L., Haug, L. S., Eggesbø, M. Å., Becher, G., Sabaredzovic, A., et al. (2013) · Environment International · doi:10.1016/j.envint.2013.10.004 · Cited by 171 · see citing works
“The median plasma concentrations of the seven PFASs in this study were comparable to reported serum levels from 2006 in Norway (Haug et al., 2009b) and somewhat lower than reported serum levels from the United States in the same year (Kato et al., 2011).”
BackgroundResultComparative pharmacokinetics of perfluorooctanesulfonate (PFOS) in rats, mice, and monkeys
Chang, S., Noker, P. E., Gorman, G. S., Gibson, S. J., Hart, J. A., Ehresman, D. J., & Butenhoff, J. L. (2011) · Reproductive Toxicology · doi:10.1016/j.reprotox.2011.07.002 · Cited by 170 · see citing works
In vitro characterization of the immunotoxic potential of several perfluorinated compounds (PFCs)
Corsini, E., Sangiovanni, E., Avogadro, A., Galbiati, V., Viviani, B., Marinovich, M., Galli, C. L., Dell’Agli, M., & Germolec, D. R. (2011) · Toxicology and Applied Pharmacology · doi:10.1016/j.taap.2011.11.004 · Cited by 169 · see citing works
Khalil, N., Chen, A., Lee, M., Czerwinski, S. A., Ebert, J. R., DeWitt, J. C., & Kannan, K. (2015) · Environmental Health Perspectives · doi:10.1289/ehp.1307909 · Cited by 170 · see citing works
“PFASs are poorly metabolized and slowly eliminated from the human body, with half-lives of 4–8 years (Kato et al. 2011), and they partition to bone tissue (Pérez et al. 2013; Bogdanska et al. 2011).”
BackgroundInfluentialThyroid-disrupting chemicals and brain development: an update
Mughal, B., Fini, J., & Demeneix, B. (2018) · Endocrine Connections · doi:10.1530/ec-18-0029 · Cited by 137 · see citing works
Sagiv, S., Rifas-Shiman, S., Fleisch, A., Webster, T., Calafat, A., Ye, X.-Y., Gillman, M., & Oken, E. (2017) · American Journal of Epidemiology · doi:10.1093/aje/kwx332 · Cited by 113 · see citing works
“As a result, plasma concentrations of these PFAS (37), and of PFOS in particular, were considerably higher in this cohort than those reported in more recent US national surveys (43, 44) but were similar to concentrations in a nationally representative survey with measurements taken during the same time period (3).”
ResultSelf-citationvon Holst, H., Nayak, P., Dembek, Z., Buehler, S., Echeverria, D., Fallacara, D., & John, L. (2021) · Heliyon · doi:10.1016/j.heliyon.2021.e08160 · Cited by 167 · see citing works
“Furthermore, cord blood used to measure PFAS levels among mothers may not be an accurate representation of PFAS during their entire pregnancy (Kato et al., 2014).”
BackgroundFraser, A. J., Webster, T. F., Watkins, D. J., Strynar, M. J., Kato, K., Calafat, A. M., Vieira, V. M., & McClean, M. D. (2013) · Environment International · doi:10.1016/j.envint.2013.08.012 · Cited by 167 · see citing works
“Low-level body burdens of some PFCs, such as perfluorooctanoate (PFOA) and perfluorooctane sulfonate (PFOS), are ubiquitous in the general human population and raise concern about the potential toxicity of these persistent organic pollutants (Kato et al., 2011; Lau et al., 2007).”
BackgroundResultInfluentialSelf-citationStarnes, H. M., Rock, K. D., Jackson, T. W., & Belcher, S. M. (2022) · Frontiers in Toxicology · doi:10.3389/ftox.2022.881584 · Cited by 166 · see citing works
“However, since efforts to limit production of these compounds were initiated, there has been a concurrent increase in production of short-chain PFAS (Kato et al., 2011; Sunderland et al., 2019).”
BackgroundDeLuca, N. M., Minucci, J. M., Mullikin, A., Slover, R., & Cohen Hubal, E. A. (2022) · Environment International · doi:10.1016/j.envint.2022.107149 · Cited by 167 · see citing works
Eriksson, U., & Kärrman, A. (2015) · Environmental Science & Technology · doi:10.1021/acs.est.5b00679 · Cited by 159 · see citing works
Per‐ and polyfluoroalkyl substances and their alternatives in paper food packaging
Glenn, G. M., Shogren, R. L., Jin, X., Orts, W. J., Hart‐Cooper, W., & Olson, L. (2021) · Comprehensive Reviews in Food Science and Food Safety · doi:10.1111/1541-4337.12726 · Cited by 163 · see citing works
Ren, X., Qin, W., Cao, L.-Y., Zhang, J., Yang, Y., Wan, B., & Guo, L. (2016) · Toxicology · doi:10.1016/j.tox.2016.08.011 · Cited by 159 · see citing works
“Thus, a downward trend for PFOS and PFOA in the general population of USA has been noted (Kato et al., 2011).”
BackgroundWatkins, D. J., Josson, J., Elston, B., Bartell, S. M., Shin, H.-M., Vieira, V. M., Savitz, D. A., Fletcher, T., & Wellenius, G. A. (2013) · Environmental Health Perspectives · doi:10.1289/ehp.1205838 · Cited by 158 · see citing works
“On the other hand, serum concentrations of PFNA have been increasing over the past 10-15 years (Kato et al. 2011).”
BackgroundInfluenza Vaccine Response in Adults Exposed to Perfluorooctanoate and Perfluorooctanesulfonate
Looker, C., Luster, M. I., Calafat, A. M., Johnson, V. J., Burleson, G. R., BURLESON, F. G., & Fletcher, T. (2013) · Toxicological Sciences · doi:10.1093/toxsci/kft269 · Cited by 158 · see citing works
Self-citationPer- and polyfluoroalkyl substances (PFAS) exposure and thyroid cancer risk
van Gerwen, M. A. G., Colicino, E., Guan, H., Dolios, G., Nadkarni, G. N., Vermeulen, R. C. H., Wolff, M. S., Arora, M., Genden, E. M., & Petrick, L. M. (2023) · EBioMedicine · doi:10.1016/j.ebiom.2023.104831 · Cited by 158 · see citing works
Mastropietro, T. F., Bruno, R., Pardo, E., & Armentano, D. (2021) · Dalton Transactions · doi:10.1039/d1dt00360g · Cited by 158 · see citing works
Unsaturated PFOS and Other PFASs in Human Serum and Drinking Water from an AFFF-Impacted Community
McDonough, C. A., Choyke, S. J., Barton, K. E., Mass, S., Starling, A. P., Adgate, J. L., & Higgins, C. P. (2021) · Environmental Science & Technology · doi:10.1021/acs.est.1c00522 · Cited by 157 · see citing works
Borg, D., Lund, B.-O., Lindquist, N.-G., & Håkansson, H. (2013) · Environment International · doi:10.1016/j.envint.2013.05.009 · Cited by 155 · see citing works
Tarapore, P., & Ouyang, B. (2021) · International Journal of Environmental Research and Public Health · doi:10.3390/ijerph18073794 · Cited by 151 · see citing works
“Support for these sex-based differences have also been observed in the NHANES database [67].”
BackgroundLiew, Z., Ritz, B. R., Ehrenstein, O. S. V., Bech, B. H., Nohr, E. A., Fei, C., Bossi, R., Henriksen, T. B., Bonefeld‐Jørgensen, E. C., & Olsen, J. (2014) · Environmental Health Perspectives · doi:10.1289/ehp.1408412 · Cited by 149 · see citing works
“PFOS and PFOA concentrations in humans were reported to be decreasing in some countries following a drop in production since 2000 (Kato et al. 2011), but exposure to other short-chain compounds such as perfluorobutane sulfonate (PFBS) and perfluorohexane sulfonate (PFHxS) and longchain…”
BackgroundInfluential
- Authors
- Kato, K., Wong, L.-Y., Jia, L. T., Kuklenyik, Z., & Calafat, A. M.
- Affiliations
- Centers for Disease Control and Prevention (US)
- Corresponding author
- Calafat, Antonia M.
- Venue
- Environmental Science & Technology
- Publisher
- American Chemical Society (ACS)
- Published
- 2011-04-06
- Volume
- 45
- Issue
- 19
- Pages
- 8037-8045
- ISSN
- 0013-936X (ISSN-L)
- 1520-5851
- OpenAlex
- W2066634548
- Cited by
- 777
- References
- 22
- Citations by year
- 2026: 36 · 2025: 46 · 2024: 68 · 2023: 55 · 2022: 50 · 2021: 54 · 2020: 63 · 2019: 38 · 2018: 60 · 2017: 50 · 2016: 50 · 2015: 52 · 2014: 55 · 2013: 45 · 2012: 39
- FWCI
- 37.44
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Environmental Science & Technology (publishedVersion)
- PubMed (publishedVersion)
- Topics
- Physical Sciences › Environmental Science › Environmental Chemistry › Per- and polyfluoroalkyl substances research
- Physical Sciences › Environmental Science › Health, Toxicology and Mutagenesis › Toxic Organic Pollutants Impact
- Life Sciences › Pharmacology, Toxicology and Pharmaceutics › Pharmaceutical Science › Fluorine in Organic Chemistry
- Keywords
- PFOS, perfluorooctanoic acid, PFHxS, perfluorononanoate, serum concentration, temporal trends, human exposure, sex differences, racial and ethnic differences, sociodemographic factors
- MeSH terms
- Adolescent, Adult, Aged, Caprylates, Child, Environmental Exposure, Female, Fluorocarbons, Health Surveys, Humans, Male, Middle Aged, Models, Biological, Nutrition Surveys, Sulfonic Acids, Time Factors, United States, Age Distribution, Young Adult
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