Abstract
Background
A fluorochemical facility near Fayetteville, North Carolina, emitted per- and polyfluoroalkyl ether acids (PFEAs), a subgroup of per- and polyfluoroalkyl substances (PFAS), to air.
Objective
Analyze PFAS in private wells near the facility and in blood from well users to assess relationships between PFEA levels in water and serum.
Methods
In 2019, we recruited private well users into the GenX Exposure Study and collected well water and blood samples. We targeted 26 PFAS (11 PFEAs) in water and 27 PFAS (9 PFEAs) in serum using liquid chromatography-mass spectrometry. We used regression modeling to explore relationships between water and serum PFAS. For the only PFEA detected frequently in water and serum, Nafion byproduct 2, we used generalized estimating equation (GEE) models to assess well water exposure metrics and then adjusted for covariates that may influence Nafion byproduct 2 serum concentrations.
Results
We enrolled 153 participants ages 6 and older (median = 56 years) using 84 private wells. Most wells (74%) had ≥6 detectable PFEAs; median ∑PFEAs was 842 ng/L (interquartile range = 197–1760 ng/L). Low molecular weight PFEAs (PMPA, HFPO-DA [GenX], PEPA, PFO2HxA) were frequently detected in well water, had the highest median concentrations, but were not detectable in serum. Nafion byproduct 2 was detected in 73% of wells (median = 14 ng/L) and 56% of serum samples (median = 0.2 ng/mL). Cumulative dose (well concentration × duration at address) was positively associated with Nafion byproduct 2 serum levels and explained the most variability (10%). In the adjusted model, cumulative dose was associated with higher Nafion byproduct 2 serum levels while time outside the home was associated with lower levels.
IMPACT
PFAS are a large class of synthetic, fluorinated chemicals. Fluorochemical facilities are important sources of environmental PFAS contamination globally. The fluorochemical industry is producing derivatives of perfluoroalkyl acids, including per- and polyfluoroalkyl ether acids (PFEAs). PFEAs have been detected in various environmental samples but information on PFEA-exposed populations is limited. While serum biomonitoring is often used for PFAS exposure assessment, serum biomarkers were not good measures of long-term exposure to low molecular weight PFEAs in a private well community. Environmental measurements and other approaches besides serum monitoring will be needed to better characterize PFEA exposure.
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Data availability
The datasets generated and analyzed during the current study are not publicly available due to human subjects protections of these data. Data may be made available from the corresponding author on reasonable request with IRB approval.
References
US Environmental Protection Agency PFAS Master List of PFAS Substances. Accessed: 11 July 2023. Available from: https://comptox.epa.gov/dashboard/chemical-lists/PFASMASTER.
Glüge J, Scheringer M, Cousins IT, DeWitt JC, Goldenman G, Herzke D. et al. An overview of the uses of per-and polyfluoroalkyl substances (PFAS). Environ Sci: Process Impacts. 2020;22:2345–73.
United States Environmental Protection Agency Fact Sheet: 2010/2015 PFOA Stewardship Program. Available from: https://www.epa.gov/assessing-and-managing-chemicals-under-tsca/fact-sheet-20102015-pfoa-stewardship-program.
National Academies of Sciences, Engineering, Medicine: Guidance on PFAS Exposure, Testing, and Clinical Follow-Up. Available from: https://www.nationalacademies.org/news/2022/07/new-report-calls-for-expanded-pfas-testing-for-people-with-history-of-elevated-exposure-offers-advice-for-clinical-treatment.
Sunderland EM, Hu XC, Dassuncao C, Tokranov AK, Wagner CC, Allen JG. A review of the pathways of human exposure to poly-and perfluoroalkyl substances (PFASs) and present understanding of health effects. J Expo Sci Environ Epidemiol. 2019;29:131–47.
McCord J, Strynar M. Identification of per-and polyfluoroalkyl substances in the cape fear river by high resolution mass spectrometry and nontargeted screening. Environ Sci Technol. 2019;53:4717–27.
Hopkins ZR, Sun M, DeWitt JC, Knappe DR. Recently detected drinking water contaminants: genx and other per‐and polyfluoroalkyl ether acids. J‐Am Water Works Assoc. 2018;110:13–28.
Galloway JE, Moreno AV, Lindstrom AB, Strynar MJ, Newton S, May AA, et al. Evidence of air dispersion: HFPO–DA and PFOA in Ohio and West Virginia surface water and soil near a fluoropolymer production facility. Environ Sci Technol. 2020;54:7175–84.
Washington JW, Rosal CG, McCord JP, Strynar MJ, Lindstrom AB, Bergman EL, et al. Nontargeted mass-spectral detection of chloroperfluoropolyether carboxylates in New Jersey soils. Science. 2020;368:1103–7.
Gebbink, W.A., Van Asseldonk, L., Van Leeuwen, S.P.J.E.S., and technology, Presence of emerging per-and polyfluoroalkyl substances (PFASs) in river and drinking water near a fluorochemical production plant in the Netherlands. 2017. 51: p. 11057-65.
Yao J, Pan Y, Sheng N, Su Z, Guo Y, Wang J, et al. Novel perfluoroalkyl ether carboxylic acids (PFECAs) and sulfonic acids (PFESAs): occurrence and association with serum biochemical parameters in residents living near a fluorochemical plant in China. Environ Sci Technol. 2020;54:13389–98.
Pike KA, Edmiston PL, Morrison JJ, Faust JA. Correlation analysis of perfluoroalkyl substances in regional US precipitation events. Water Res. 2021;190:116685.
North Carolina Department of Environmental Quality GenX Information for Residents in Bladen, Cumberland, Robeson and Sampson Counties. Accessed: 25 Jan 2023. Available from: https://deq.nc.gov/news/key-issues/genx-investigation/genx-information-residents#DEQMaps-11849.
Pan Y, Zhang H, Cui Q, Sheng N, Yeung LW, Sun Y, et al. Worldwide distribution of novel perfluoroether carboxylic and sulfonic acids in surface water. Environ Sci Technol. 2018;52:7621–9.
Strynar M, Dagnino S, McMahen R, Liang S, Lindstrom A, Andersen E, et al. Identification of novel perfluoroalkyl ether carboxylic acids (PFECAs) and sulfonic acids (PFESAs) in natural waters using accurate mass time-of-flight mass spectrometry (TOFMS). Environ Sci Technol. 2015;49:11622–30.
Sun M, Arevalo E, Strynar M, Lindstrom A, Richardson M, Kearns B, et al. Legacy and emerging perfluoroalkyl substances are important drinking water contaminants in the Cape Fear River Watershed of North Carolina. Environ Sci Technol Lett. 2016;3:415–9.
Espartero LJL, Yamada M, Ford J, Owens G, Prow T, Juhasz A. Health-related toxicity of emerging per-and polyfluoroalkyl substances: Comparison to legacy PFOS and PFOA. Environ Res. 2022;212:113431.
Yao J, Dong Z, Jiang L, Pan Y, Zhao M, Bai X, et al. Emerging and legacy perfluoroalkyl substances in breastfed Chinese infants: renal clearance, body burden, and implications. Environ Health Perspect. 2023;131:037003.
Kotlarz N, McCord J, Collier D, Lea CS, Strynar M, Lindstrom AB, et al. Measurement of novel, drinking water-associated PFAS in blood from adults and children in Wilmington, North Carolina. Environ Health Perspect. 2020;128:077005.
Hoffman K, Webster TF, Bartell SM, Weisskopf MG, Fletcher T, Vieira VM. Private drinking water wells as a source of exposure to perfluorooctanoic acid (PFOA) in communities surrounding a fluoropolymer production facility. Environ Health Perspect. 2011;119:92–97.
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.
Seals R, Bartell SM, Steenland K. Accumulation and clearance of perfluorooctanoic acid (PFOA) in current and former residents of an exposed community. Environ Health Perspect. 2011;119:119–24.
Emmett EA, Shofer FS, Zhang H, Freeman D, Desai C, Shaw LM. Community exposure to perfluorooctanoate: relationships between serum concentrations and exposure sources. J Occup Environ Med. 2006;48:759.
Zhou J, Baumann K, Surratt JD, Turpin BJ. Legacy and emerging airborne per-and polyfluoroalkyl substances (PFAS) collected on PM 2.5 filters in close proximity to a fluoropolymer manufacturing facility. Environ Sci Process Impacts. 2022;24:2272–83.
North Carolina Department of Environmental Quality (NC DEQ) GenX Investigation: Groundwater. Accessed: 11 July 2022. Available from: https://deq.nc.gov/news/key-issues/genx-investigation/groundwater.
United States Environmental Protection Agency (US EPA) Drinking Water Health Advisory: Hexafluoropropylene Oxide (HFPO) Dimer Acid (CASRN 13252-13-6) and HFPO Dimer Acid Ammonium Salt (CASRN 62037-80-3), Also Known as “GenX Chemicals”. Available from: https://www.epa.gov/system/files/documents/2022-06/drinking-water-genx-2022.pdf.
United States Environmental Protection Agency. Per- and Polyfluoroalkyl Substances (PFAS): Proposed PFAS National Primary Drinking Water Regulation. Accessed: Oct 4, 2023. Available from: https://www.epa.gov/sdwa/and-polyfluoroalkyl-substances-pfas.
U.S. EPA, 2011 U.S. EPA, 2011 Exposure Factors Handbook 2011 Edition (Final Report). U.S. Environmental Protection Agency, Washington, DC, EPA/600/R-09/052F. Accessed: Jan 9, 2023. Available from: https://www.epa.gov/expobox/about-exposure-factors-handbook.
Pétré M-A, Genereux DP, Koropeckyj-Cox L, Knappe DR, Duboscq S, Gilmore TE, et al. Per-and polyfluoroalkyl substance (PFAS) transport from groundwater to streams near a PFAS manufacturing facility in North Carolina, USA. Environ Sci Technol. 2021;55:5848–56. https://doi.org/10.1021/acs.est.0c07978.
OECD Synthesis paper on per and polyfluorinated chemicals. Accessed: 11 July 2023. Available from: https://www.oecd.org/chemicalsafety/risk-management/synthesis-paper-on-per-and-polyfluorinated-chemicals.htm.
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.
Park SK, Peng Q, Ding N, Mukherjee B, Harlow SD. Determinants of per-and polyfluoroalkyl substances (PFAS) in midlife women: evidence of racial/ethnic and geographic differences in PFAS exposure. Environ Res. 2019;175:186–99.
Roostaei J, Colley S, Mulhern R, May AA, Gibson JM. Predicting the risk of GenX contamination in private well water using a machine-learned Bayesian network model. J Hazard Mater. 2021;411:125075.
European Chemicals Agency Exposure related observations in humans: other data for Ammonium 2,3,3,3-tetrauoro-2-(heptauoropropoxy)propanoate.
Pritchett JR, Rinsky JL, Dittman B, Christensen A, Langley R, Moore Z, et al. Notes from the field: targeted biomonitoring for GenX and other per-and polyfluoroalkyl substances following detection of drinking water contamination—North Carolina, 2018. Morbidity Mortal Wkly Rep. 2019;68:647.
C8 Science Panel. Accessed: Oct 11, 2023. Available from: http://www.c8sciencepanel.org/index.html.
Johanson G, Gyllenhammar I, Ekstrand C, Pyko A, Xu Y, Li Y, et al. Quantitative relationships of perfluoroalkyl acids in drinking water associated with serum concentrations above background in adults living near contamination hotspots in Sweden. Environ Res. 2023;219:115024.
Calafat AM, Kato K, Hubbard K, Jia T, Botelho JC, Wong L-Y. Legacy and alternative per-and polyfluoroalkyl substances in the US general population: paired serum-urine data from the 2013-4 National Health and Nutrition Examination Survey. Environ Int. 2019;131:105048.
Calafat AM, Kuklenyik Z, Reidy JA, Caudill SP, Tully JS, Needham LL. Serum concentrations of 11 polyfluoroalkyl compounds in the US population: data from the National Health and Nutrition Examination Survey (NHANES) 1999− 2000. Environ Sci Technol. 2007;41:2237–42.
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) 2003-4 and comparisons with NHANES 1999–2000. Environ Health Perspect. 2007;115:1596–602.
Chow SJ, Ojeda N, Jacangelo JG, Schwab KJ. Detection of ultrashort-chain and other per-and polyfluoroalkyl substances (PFAS) in US bottled water. Water Res. 2021;201:117292.
Neuwald IJ, Hübner D, Wiegand HL, Valkov V, Borchers U, Nödler K, et al. Ultra-short-chain PFASs in the sources of German drinking water: prevalent, overlooked, difficult to remove, and unregulated. Environ Sci Technol. 2022;56:6380–90.
Pelch KE, McKnight T, Reade A. 70 analyte PFAS test method highlights need for expanded testing of PFAS in drinking water. Sci Total Environ. 2023;876:162978.
Poothong S, Thomsen C, Padilla-Sanchez JA, Papadopoulou E, Haug LS.Distribution of novel and well-known poly-and perfluoroalkyl substances (PFASs) in human serum, plasma, and whole blood.Environ Sci Technol. 2017;51:13388–96.
Wallis D, Kotlarz N, Knappe D, Collier D, Lea CS, Reif D, et al. Estimation of the half-lives of recently detected per- and poly- fluorinated alkyl ethers in an exposed community. Environ Sci Technol. 2023;57:15348–55.
Kirkwood KI, Fleming J, Nguyen H, Reif DM, Baker ES, Belcher SM. Utilizing pine needles to temporally and spatially profile per-and polyfluoroalkyl substances (PFAS). Environ Sci Technol. 2022;56:3441–51.
Mulhern R, Bynum N, Liyanapatirana C, DeStefano NJ, Knappe DR, MacDonald Gibson J. Longitudinal assessment of point‐of‐use carbon filters for removal of per‐and polyfluoroalkyl substances from private well water. AWWA Water Sci. 2021;3:e1262.
Timeline: Tracking GenX contamination in NC. WRAL News. Posted on Aug 10, 2017. Available from: https://www.wral.com/story/timeline-tracking-the-route-of-genx-in-the-cape-fear-river/16869639/.
Nakayama SF, Yoshikane M, Onoda Y, Nishihama Y, Iwai-Shimada M, Takagi M, et al. Worldwide trends in tracing poly-and perfluoroalkyl substances (PFAS) in the environment. TrAC Trends Anal Chem. 2019;121:115410.
Hölzer J, Midasch O, Rauchfuss K, Kraft M, Reupert R, Angerer J, et al. Biomonitoring of perfluorinated compounds in children and adults exposed to perfluorooctanoate-contaminated drinking water. Environ Health Perspect. 2008;116:651–7.
Daly ER, Chan BP, Talbot EA, Nassif J, Bean C, Cavallo SJ, et al. Per-and polyfluoroalkyl substance (PFAS) exposure assessment in a community exposed to contaminated drinking water, New Hampshire, 2015. Int J Hyg Environ Health. 2018;221:569–77.
Bartell SM, Calafat AM, Lyu C, Kato K, Ryan PB, Steenland KJEHP. 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.
Guillette T, McCord J, Guillette M, Polera M, Rachels KT, Morgeson C, et al. Elevated levels of per-and polyfluoroalkyl substances in Cape Fear River Striped Bass (Morone saxatilis) are associated with biomarkers of altered immune and liver function. Environ Int. 2020;136:105358.
Acknowledgements
We thank our Fayetteville community science advisory board (T. Duncan, J. Green, V. Guidry, C Harrelson, A. Jones, J. Kimbrough, Z. Moore, J. Parsons, D. Sargent, W. Smith, T. Walters, M. Watters) for helpful discussions. We thank Stacie Reckling for creating the map in Fig. S2.
Funding
The GenX Exposure Study is supported by research funding from the National Institute of Environmental Health Sciences (1R21ES029353), Center for Human Health and the Environment (CHHE) at NC State University (P30 ES025128), the Center for Environmental and Health Effects of PFAS (P42 ES0310095), and the NC Policy Collaboratory. The research presented was not performed or funded by EPA and was not subject to EPA’s quality system requirements. The views expressed in this manuscript are those of the authors and do not necessarily represent the views or policies of the U.S. Environmental Protection Agency or the National Institutes of Health. Any mention of trade names or commercial products does not constitute EPA endorsement or recommendation for use.
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NK: Study conceptualization, sample analysis, data acquisition and interpretation, led writing of original draft and revisions. CC: Data acquisition, contributed to original draft, review of final version. DC: Data acquisition, contributed to original draft, review of final version. CSL: Data acquisition, contributed to original draft, review of final version. TG, JM, MS, ZRH: Analytical methodology, sample analysis, contributed to original draft, review of final version. MC: Data acquisition, statistical analysis, review & editing. DRUK: Methodology, data interpretation, contributed to original draft, review & editing. JAH: Study conceptualization, methodology, data interpretation, review & editing, funding acquisition.
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The GenX Exposure Study protocol and informed consent documents are approved by the Institutional Review Board of NC State University. Participants in the GenX Exposure Study gave informed consent to their information being used for research prior to participation this study.
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Kotlarz, N., Guillette, T., Critchley, C. et al. Per- and polyfluoroalkyl ether acids in well water and blood serum from private well users residing by a fluorochemical facility near Fayetteville, North Carolina. J Expo Sci Environ Epidemiol 34, 97–107 (2024). https://doi.org/10.1038/s41370-023-00626-x
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DOI: https://doi.org/10.1038/s41370-023-00626-x
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