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Detection of Poly- and Perfluoroalkyl Substances (PFASs) in U.S. Drinking Water Linked to Industrial Sites, Military Fire Training Areas, and Wastewater Treatment Plants

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† Harvard T. H. Chan School of Public Health, Boston, Massachusetts 02215, United States
‡ Harvard John A. Paulson School of Engineering and Applied Sciences, Cambridge, Massachusetts 02138, United States
§ Environmental Working Group, Washington, D.C. 20009, United States
∥ National Exposure Research Laboratory, U.S. Environmental Protection Agency, Research Triangle Park, North Carolina 27711, United States
⊥ University of California at Berkeley, Berkeley, California 94720, United States
# Silent Spring Institute, Newton, Massachusetts 02460, United States
@ University of Rhode Island, Narragansett, Rhode Island 02882, United States
∇ Green Science Policy Institute, Berkeley, California 94705, United States
● California Department of Toxic Substances Control, 1001 I Street, Sacramento, California 95814, United States (Formerly at the Green Science Policy Institute, Berkeley, California 94705, United States)
○ Colorado School of Mines, 1500 Illinois Street, Golden, Colorado 80401, United States
*Address: 128 Pierce Hall, Harvard University, Cambridge, MA 02138. Phone: 1-617-384-8839. E-mail: [email protected]
Cite this: Environ. Sci. Technol. Lett. 2016, 3, 10, 344–350
Publication Date (Web):August 9, 2016
https://doi.org/10.1021/acs.estlett.6b00260
Copyright © 2016 American Chemical Society
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Abstract

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Drinking water contamination with poly- and perfluoroalkyl substances (PFASs) poses risks to the developmental, immune, metabolic, and endocrine health of consumers. We present a spatial analysis of 2013–2015 national drinking water PFAS concentrations from the U.S. Environmental Protection Agency’s (US EPA) third Unregulated Contaminant Monitoring Rule (UCMR3) program. The number of industrial sites that manufacture or use these compounds, the number of military fire training areas, and the number of wastewater treatment plants are all significant predictors of PFAS detection frequencies and concentrations in public water supplies. Among samples with detectable PFAS levels, each additional military site within a watershed’s eight-digit hydrologic unit is associated with a 20% increase in PFHxS, a 10% increase in both PFHpA and PFOA, and a 35% increase in PFOS. The number of civilian airports with personnel trained in the use of aqueous film-forming foams is significantly associated with the detection of PFASs above the minimal reporting level. We find drinking water supplies for 6 million U.S. residents exceed US EPA’s lifetime health advisory (70 ng/L) for PFOS and PFOA. Lower analytical reporting limits and additional sampling of smaller utilities serving <10000 individuals and private wells would greatly assist in further identifying PFAS contamination sources.

  Note

There was a text error in the Results and Discussion section in the version published ASAP August 9, 2016; the corrected version was published ASAP August 11, 2016.

Introduction

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Poly- and perfluoroalkyl substances (PFASs) make up a large group of persistent anthropogenic chemicals used in industrial processes and commercial products over the past 60 years.(1) Widespread use and extreme resistance to degradation have resulted in the ubiquitous presence of these compounds in the environment. The 2011–2012 U.S. National Health and Nutrition Examination Survey reported detectable serum PFAS concentrations in virtually all individuals (97%).(2, 3) Human PFAS exposure has been linked to cancer, elevated cholesterol, obesity, immune suppression, and endocrine disruption.(4-6) Health concerns in the early 2000s prompted manufacturers in Europe and North America to phase out production of some long-chain PFASs.(7-10) Declines in production of these compounds have been offset by increases in developing regions such as Asia.(8) Limited available data suggest widespread exposure to replacement (short-chain) PFASs may also adversely affect human health.(11, 12)
Human PFAS exposure includes dietary sources, household dust, air, and drinking water.(13, 14) Exposure from drinking water is a serious concern because of the high aqueous solubility of many PFASs.(15, 16) Relatively low PFAS concentrations can lead to elevated exposures in the general population.(17) Elevated PFAS concentrations in U.S. drinking water have been reported in numerous regions,(15, 16, 18, 19) especially near industrial sites that produce or use them.(6, 16, 20) For example, perfluorooctanoic acid (PFOA) concentrations 190-fold higher than the lifetime health advisory (70 ng/L) recommended by the U.S. Environmental Protection Agency (US EPA)(21) were measured in drinking water near a fluorochemical facility in Washington, WV, where PFOA was used in fluoropolymer production.(18)
Many civilian airports and military fire training areas have been contaminated by PFASs contained in aqueous film-forming foams (AFFFs) that are widely used during firefighting training activities. Groundwater and surface waters surrounding these sites containing PFAS concentrations that are 3–4 orders of magnitude higher than the US EPA health advisory level for drinking water have been reported.(22, 23) Wastewater treatment plants (WWTPs) are another important PFAS source because these compounds are not removed by standard treatment methods(24) and labile precursors biodegrade, increasing concentrations in effluent relative to influent.(25, 26) Land application of approximately half of the biosolids generated by WWTPs may contribute to human exposure through subsequent contamination of water, food, livestock, and wildlife.(27)
Understanding nationwide PFAS exposures from drinking water is important for identifying potentially vulnerable populations. However, previous studies have mainly focused on individual point sources of PFAS contamination and site-specific drinking water exposures.(15, 16) Here we develop a statistical framework for investigating whether increased PFAS concentrations in drinking water are associated with the number of point sources within a watershed (represented by an eight-digit hydrologic unit code, hereafter abbreviated HUC). We used publicly available drinking water concentration data for six PFASs from the US EPA’s third Unregulated Contaminant Monitoring Rule (UCMR3), including perfluorobutanesulfonic acid (PFBS), perfluorohexanesulfonic acid (PFHxS), perfluoroheptanoic acid (PFHpA), PFOA, perfluorooctanesulfonic acid (PFOS), and perfluorononanoic acid (PFNA) (Table S1).(28) We discuss the utility of the UCMR3 database for identifying sources of PFASs to U.S. drinking water supplies, locations of vulnerable populations, and priorities for future monitoring.

Methods

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Drinking Water Data

Our analysis included analytical results for six PFASs in 36149 drinking water samples from the US EPA’s UCMR3 program collected between January 2, 2013, and December 9, 2015.(28) Samples cover all 4064 public water supplies serving >10000 individuals. Data are also available for 800 public water supplies serving <10000 individuals, but this represents only a small fraction (0.5%) of the 144165 in this category. Minimum reporting levels (MRLs) for the six PFASs analyzed are listed in Table S1.
One limitation of the UCMR3 database is that national data on system intakes for public water supplies are classified,(29) making it difficult to place them within a specific hydrological network. We therefore extracted the zip codes for areas served and aggregated data within eight-digit HUCs(30) to capture the most detailed hydrologic information that exceeds the spatial resolution of PFAS data (zip code areas). We used the highest reported PFAS concentrations when multiple systems were located within a single zip code and/or when multiple zip code areas were located within the same HUC.

PFAS Point Sources

Our spatial analysis (Figure S1) included point source information for (a) 16 industrial sites listed in the US EPA’s 2010/2015 PFOA Stewardship Program (Table S2),(31) (b) 8572 WWTPs,(32) (c) 290 military fire training areas that contain 664 military fire training sites,(33) and (d) 533 civilian airports that are compliant with Title 14 Code of Federal Regulations, Part 139 for personnel trained in the use of AFFF (hereafter termed “AFFF-certified airports”).(34) PFASs produced and/or used vary across industrial sites, and not all compounds were associated with all sites. For example, a fluorochemical manufacturing facility in Decatur, AL, produced both PFOS and PFOA,(35) while only PFOA was used in the manufacturing process of another fluorochemical production facility in Parkersburg, WV.(36) We conducted a sensitivity analysis to examine the potential production misclassification bias by limiting industrial sites to include the ones that only produced or used each specific compound (Table S3). We used the Google Maps application program interface (API) to geocode coordinates based on addresses. Potentially important PFAS sources such as landfills, biosolids, and small industrial PFAS users could not be included in this analysis because comprehensive geospatial data are not available.

Spatial and Statistical Analysis

We used ArcMap 10.3.1 (ESRI) to explore statistical differences between the number of point sources in eight-digit HUCs with PFAS levels above and below the level of detection. We developed a multivariate spatial regression model for watersheds with detectable PFASs that adjusts for correlations and co-location among point sources. A natural log transformation was used to normalize the distribution of individual PFASs. PFNA and PFBS were excluded from the spatial regression analysis due to a low detection frequency (15 and 14 of 1601 watersheds, respectively). We used Moran’s I statistic to test for spatial dependence in the model residuals from an ordinary least-squares (OLS) regression and correct for spatial dependence in the final spatial regression model. Akaike Information Criterion(37) was used to compare the OLS and spatial regression models, where a lower value implies a better model fit. A series of cross-validation tests were also completed to assess the predictive capacity and stability of the final set of models. The OLS and spatial regression models were constructed using GeoDa 1.6 software,(38) and cross-validation was implemented in R version 3.1.3.

Results and Discussion

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PFASs in U.S. Drinking Water

PFASs were detected at or above the MRLs in 194 of 4864 public water supplies, serving 16.5 million residents in 33 different states, three American territories (American Samoa, Northern Mariana Islands, and Guam), and the Salt River Pima-Maricopa Indian Community. Drinking water from 13 states accounted for 75% of detections, including, by order of frequency of detection, California, New Jersey, North Carolina, Alabama, Florida, Pennsylvania, Ohio, New York, Georgia, Minnesota, Arizona, Massachusetts, and Illinois (Figure 1). Detection frequencies for PFASs across the 4864 public water supplies were 2.2% for PFOA, 2.0% for PFOS, 1.7% for PFHpA, 1.1% for PFHxS, and <0.003% for others.

Figure 1

Figure 1. Hydrologic unit codes (eight-digit HUCs) used as a proxy for watersheds with detectable PFOA and PFOS in drinking water measured in the US EPA’s UCMR3 program (2013–2015). Blank areas represent regions where no data are available.

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Many detectable PFAS concentrations in the UCMR3 database are above chronic drinking water and water quality standards for other regions (i.e., surface water European Union, PFOS, <1 ng/L; drinking water Sweden, sum of seven PFASs, <90 ng/L; groundwater State of New Jersey, PFNA, <10 ng/L; drinking water State of Vermont, sum of PFOS and PFOA, <20 ng/L).(39-42) A recent analysis developed a benchmark dose for immunotoxicity in children and suggested a drinking water limit of approximately 1 ng/L for PFOS and PFOA.(26) Data from rodents that measured sensitive end points such as mammary gland development support a similar level.(26)
Six million people were served by 66 public water supplies that have at least one sample at or above the US EPA’s 2016 health advisory for PFOS and PFOA (70 ng/L individually or combined). Concentrations ranged as high as 349 ng/L for PFOA, 1800 ng/L for PFOS, and 56 ng/L for PFNA.
The detection frequency in drinking water sourced from groundwater was more than twice that from surface water (Table S4). Long-chain PFASs(43) (PFHxS, PFOS, PFOA, and PFNA) were more frequently detected in groundwater, and short-chain compounds (PFHpA and PFBS) were detected more frequently in surface waters. This may be due to both the original mode of environmental release (as an aerosol, application to soil, and aqueous discharge) and the inverse relationship between PFAS mobility and chain length.(44) The MRLs (10–90 ng/L) in the UCMR3 database are up to 2 orders of magnitude higher than the limit of quantitation in most published studies,(45-49) and more than 10 times higher than the drinking water limit (1 ng/L) suggested by human and animal studies.(26, 50) Because PFASs are detectable in virtually all parts of the environment,(5, 7, 9, 13, 14, 20, 44, 51) we infer that the large fraction of samples below reporting limits (Table S4) is driven in part by high MRLs.

Sources Surrounding Locations with Detectable PFASs

Our analysis indicates point sources are significantly more abundant in HUCs with detectable PFASs [two-sided t test, p < 0.05 (Table 1 and Figure S2)]. This includes drinking water samples from 1601 of the 2158 total U.S. HUCs. For example, HUCs with detectable PFOA levels (8% of the total) have more industrial sites, military fire training areas, AFFF-certified airports, and WWTPs than those with concentrations below detection. These trends can be observed across all PFASs. Similarly, HUCs with point sources have higher detection frequencies for PFASs (Table S5). For example, the presence of a military fire training area within a HUC increases the frequency of detection of at least one PFAS from 10.4% to 28.2%. One caveat is that imprecise information about public water supply intakes can cause misclassification bias. Systems that draw water upstream from point sources, such as Minneapolis and St. Paul in Minnesota, may not actually be affected as indicated by the aggregated spatial analysis.
Table 1. Mean Abundance of Point Sources within Eight-Digit Hydrologic Unit Codes (HUCs) with Drinking Water PFAS Concentrations above and below the Method Reporting Limit in the UCMR3 Program
 mean abundancea within eight-digit hydrologic unit codes
compoundmajor industrial sitesbmilitary fire training areasAFFF-certified airportsWWTPsc
PFBS    
<90 ng/L (n = 1587)0.010.150.294.9
>90 ng/L (n = 14)0.210.710.5014.6
p-valued0.2060.1050.1480.069
PFHxS    
<30 ng/L (n = 1507)0.010.130.274.8
>30 ng/L (n = 94)0.060.600.638.8
p-value0.056<0.001<0.001<0.001
PFHpA    
<10 ng/L (n = 1509)0.010.130.264.7
>10 ng/L (n = 92)0.090.570.679.7
p-value0.016<0.001<0.001<0.001
PFOA    
<20 ng/L (n = 1473)0.010.130.264.6
>20 ng/L (n = 128)0.050.520.569.5
p-value0.038<0.001<0.001<0.001
PFOS    
<40 ng/L (n = 1487)0.010.130.264.7
>40 ng/L (n = 114)0.050.540.578.9
p-value0.064<0.001<0.001<0.001
PFNA    
<20 ng/L (n = 1586)0.010.150.284.9
>20 ng/L (n = 15)0.131.131.1320.1
p-value0.3660.0140.0080.007
a

The mean abundance is calculated as the mean number of point sources within HUCs with PFASs above or below the level of detection.

b

Only the major industrial sites participating in the US EPA’s 2010/2015 PFOA Stewardship Program were included.

c

Wastewater treatment plant.

d

Two-sample t-test p-values.

Results of the Spatial Regression Model

Spatial regression modeling explains 38–62% of the variance in drinking water concentrations for the four PFASs considered (Table 2). Each additional industrial site within a HUC is associated with an 81% increase in PFOA (p < 0.001), which is the strongest statistical association across compounds and point sources. Increasing PFOS concentrations are positively associated with the number of industrial sites, but this relationship is not statistically significant (p = 0.124). The small number of sites that have manufactured or used PFOS likely accounts for the lack of a statistically significant relationship.
Table 2. Spatial Regression Models for Drinking Water PFAS Concentrations as a Function of the Abundance of Point Sources
compoundmajor industrial sitesaMFTAsbAFFF-certified airportsWWTPscλdR2
PFHxS      
coefficiente24%20%–13%1%94%0.62
p-valuef0.2490.0020.0730.045<0.001 
PFHpA      
coefficient10%10%–2%0.5%72%0.40
p-value0.5690.1550.7610.436<0.001 
PFOA      
coefficient81%10%–6%2%52%0.38
p-value<0.0010.1110.3530.006<0.001 
PFOS      
coefficient46%35%–6%2%79%0.46
p-value0.124<0.0010.5120.007<0.001 
a

Only the major industrial sites participating in US EPA’s 2010/2015 PFOA Stewardship Program were included.

b

MFTA = military fire training area.

c

WWTP = wastewater treatment plant.

d

Coefficient for the spatial error term characterizing spatial influence.

e

Results have been transformed to reflect expected changes in drinking water concentrations per increase in the abundance of different sources. Positive coefficients in the results indicate increasing concentrations with an increasing abundance of point sources within the same hydrologic unit.

f

p-values for the spatial error regression model. The spatial error term is used to incorporate spatial autocorrelation structures into a linear regression model.

The number of military fire training areas within each HUC is positively associated with increasing levels of all PFOS, PFOA, PFHxS, and PFHpA, and is statistically significant for PFHxS (p = 0.045) and PFOS (p = 0.007). Each additional military fire training area within the same HUC is associated with a 20% increase in PFHxS (p = 0.002), a 10% increase in PFHpA (p = 0.155), a 10% increase in PFOA (p = 0.111), and a 35% increase in PFOS (p < 0.001). AFFFs typically contain relatively high concentrations of PFOS and PFHxS and their polyfluorinated precursors compared to the concentrations of other perfluorinated carboxylates,(23, 52-54) which is consistent with these statistical results.
We find a small but significant increase in PFOS and PFOA (2%; p < 0.01) with each additional WWTP within the same HUC. This is consistent with the greater abundance but smaller quantities of PFASs released by WWTPs.(55) Similarly, results of Valsecchi et al.(51) show PFAS releases from WWTPs are important but less significant than those from fluorochemical manufacturing facilities in Italy. The number of WWTPs may also be a proxy for other population-driven PFAS sources.
The number of AFFF-certified airports is not significantly associated with PFAS concentrations in the current data set. This may reflect misclassification bias because the certification used to identify airports indicates eligibility but not actual use of AFFF. The UCMR3 database contains limited data for smaller drinking water systems where localized reports of contamination from airports have been most abundant.(22, 56)

Current Data Limitations and Future Monitoring Efforts

The UCMR3 database has several limitations that restrict its predictive power for identifying U.S. drinking water supplies likely to contain elevated levels of PFASs. Classification of geospatial data on intakes for public water supplies limits the spatial resolution of the current data set and associated statistical models to a radius of 50 km (median radius of watersheds).(57, 58) Many of the impacted drinking water systems are groundwater systems, and contaminated groundwater plumes are often much smaller than 50 km.(23, 53, 59)
Geospatial data are lacking for many potentially important PFAS point sources such as a wide range of industries, landfills, biosolids application, and other AFFF-impacted sites where relatively smaller volumes of AFFF were released.(27, 54, 60-67) Data on PFAS releases from smaller industrial facilities (e.g., plastics, textiles, paper, and lubricants) are usually withheld as confidential business information, and little information about airborne emissions is available for characterizing the importance of atmospheric releases and potential long-range transport. For example, biosolids application resulted in one of the largest PFAS drinking water contamination events in Europe(68) but could not be included in this analysis because U.S. use data are not available on a national scale.
Sources not included in our spatial analysis are represented by the highly significant lambda (λ) coefficients (Table 2). Areas with high model residuals (greater than 1.5 standard deviation) mean that current information about sources cannot fully explain the high observed PFAS concentrations. The map of model residuals (Figure S3) can thus be used to guide high-priority sampling regions in future work.
We found a statistically greater abundance of point sources in watersheds with detectable PFASs, including AFFF-certified airports. However, multivariate spatial regression models did not show a significant association between AFFF-certified airports and concentrations of PFASs in nearby drinking water. Other studies have reported elevated PFAS concentrations in groundwater wells adjacent to AFFF-certified airports.(22) Small drinking water systems and private wells may be disproportionately affected by PFASs originating from AFFF use at civilian airports, but representative data for these small drinking water systems are not included in the UCMR3 program.(69)
Approximately 44.5 million U.S. individuals rely on private drinking water wells,(70) and 52 million individuals rely on smaller public water supplies (<10000 served). The UCMR3 program includes 0.5% testing incidence for smaller public water supplies(71) and no testing of private wells, meaning that information about drinking water PFAS exposures is therefore lacking for almost one-third of the U.S. population.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.estlett.6b00260.

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Author Information

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  • Corresponding Author
    • Xindi C. Hu - Harvard T. H. Chan School of Public Health, Boston, Massachusetts 02215, United States;  Harvard John A. Paulson School of Engineering and Applied Sciences, Cambridge, Massachusetts 02138, United States;  Email: [email protected]
  • Authors
    • David Q. Andrews - Environmental Working Group, Washington, D.C. 20009, United States
    • Andrew B. Lindstrom - National Exposure Research Laboratory, U.S. Environmental Protection Agency, Research Triangle Park, North Carolina 27711, United States
    • Thomas A. Bruton - University of California at Berkeley, Berkeley, California 94720, United States
    • Laurel A. Schaider - Silent Spring Institute, Newton, Massachusetts 02460, United States
    • Philippe Grandjean - Harvard T. H. Chan School of Public Health, Boston, Massachusetts 02215, United States
    • Rainer Lohmann - University of Rhode Island, Narragansett, Rhode Island 02882, United States
    • Courtney C. Carignan - Harvard T. H. Chan School of Public Health, Boston, Massachusetts 02215, United States
    • Arlene Blum - University of California at Berkeley, Berkeley, California 94720, United States;  Green Science Policy Institute, Berkeley, California 94705, United States
    • Simona A. Balan - California Department of Toxic Substances Control, 1001 I Street, Sacramento, California 95814, United States (Formerly at the Green Science Policy Institute, Berkeley, California 94705, United States)
    • Christopher P. Higgins - Colorado School of Mines, 1500 Illinois Street, Golden, Colorado 80401, United States
    • Elsie M. Sunderland - Harvard T. H. Chan School of Public Health, Boston, Massachusetts 02215, United States;  Harvard John A. Paulson School of Engineering and Applied Sciences, Cambridge, Massachusetts 02138, United States
  • Notes

    The authors declare no competing financial interest.

Acknowledgment

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We acknowledge financial support for research at Harvard from the Smith Family Foundation and a private donor. We thank Marcia Castro (Harvard) for her feedback on an earlier version of the manuscript and Jahred Liddie (Harvard) for his assistance with the sensitivity analysis. T.A.B. was supported by the U.S. National Institute for Environmental Health Sciences (NIEHS) Superfund Research Program (Grant P42 ES004705) and the Superfund Research Center at the University of California, Berkeley. The views expressed in this article are those of the authors and do not necessarily represent the views or policies of the U.S. Environmental Protection Agency.

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    Prenatal perfluoroalkyl substance exposure and child adiposity at 8 years of age: The HOME study
    Braun, Joseph M.; Chen, Aimin; Romano, Megan E.; Calafat, Antonia M.; Webster, Glenys M.; Yolton, Kimberly; Lanphear, Bruce P.
    Obesity (2016), 24 (1), 231-237CODEN: OBESAX; ISSN:1930-7381. (John Wiley & Sons, Inc.)
    Objective : To examine relationships between prenatal perfluoroalkyl substance (PFAS) exposure and adiposity in children born to women who lived downstream from a fluoropolymer manufg. plant. Methods : Data are from a prospective cohort in Cincinnati, Ohio (HOME Study). Perfluorooctanoic (PFOA), perfluorooctane sulfonic (PFOS), perfluorononanoic (PFNA), and perfluorohexane sulfonic (PFHxS) acids were measured in prenatal serum samples. Differences were measured in body mass index z-scores (BMI), waist circumference, and body fat at 8 years of age (n = 204) and BMI between 2-8 years of age (n = 285) according to PFAS concns. Results : Children born to women in the top two PFOA terciles had greater adiposity at 8 years than children in the 1st tercile. For example, waist circumference (cm) was higher among children in the 2nd (4.3; 95% CI: 1.7, 6.9) and 3rd tercile (2.2; 95% CI: -0.5, 4.9) compared to children in the 1st tercile. Children in the top two PFOA terciles also had greater BMI gains from 2 to 8 years compared to children in the 1st tercile (P < 0.05). PFOS, PFNA, and PFHxS were not assocd. with adiposity. Conclusions : In this cohort, higher prenatal serum PFOA concns. were assocd. with greater adiposity at 8 years and a more rapid increase in BMI between 2-8 years.
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  6. 6
    Barry, V.; Winquist, A.; Steenland, K. Perfluorooctanoic acid (PFOA) exposures and incident cancers among adults living near a chemical plant Environ. Health Perspect 2013, 121 (11–12) 1313– 1318 DOI: 10.1289/ehp.1306615
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    6
    Perfluorooctanoic acid (PFOA) exposures and incident cancers among adults living near a chemical plant
    Barry Vaughn; Winquist Andrea; Steenland Kyle
    Environmental health perspectives (2013), 121 (11-12), 1313-8 ISSN:.
    BACKGROUND: Perfluorooctanoic acid (PFOA) is a synthetic chemical ubiquitous in the serum of U.S. residents. It causes liver, testicular, and pancreatic tumors in rats. Human studies are sparse. OBJECTIVE: We examined cancer incidence in Mid-Ohio Valley residents exposed to PFOA in drinking water due to chemical plant emissions. METHODS: The cohort consisted of adult community residents who resided in contaminated water districts or worked at a local chemical plant. Most participated in a 2005-2006 baseline survey in which serum PFOA was measured. We interviewed the cohort in 2008-2011 to obtain further medical history. Retrospective yearly PFOA serum concentrations were estimated for each participant from 1952 through 2011. Self-reported cancers were validated through medical records and cancer registry review. We estimated the association between cancer and cumulative PFOA serum concentration using proportional hazards models. RESULTS: Participants (n = 32,254) reported 2,507 validated cancers (21 different cancer types). Estimated cumulative serum PFOA concentrations were positively associated with kidney and testicular cancer [hazard ratio (HR) = 1.10; 95% CI: 0.98, 1.24 and HR = 1.34; 95% CI: 1.00, 1.79, respectively, for 1-unit increases in ln-transformed serum PFOA]. Categorical analyses also indicated positive trends with increasing exposures for both cancers: for kidney cancer HRs for increasing exposure quartiles were 1.0, 1.23, 1.48, and 1.58 (linear trend test p = 0.18) and for testicular cancer, HRs were 1.0, 1.04, 1.91, 3.17 (linear trend test p = 0.04). CONCLUSIONS: PFOA exposure was associated with kidney and testicular cancer in this population. Because this is largely a survivor cohort, findings must be interpreted with caution, especially for highly fatal cancers such as pancreatic and lung cancer.
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  7. 7
    Land, M.; de Wit, C. A.; Cousins, I. T.; Herzke, D.; Johansson, J.; Martin, J. W. What is the effect of phasing out long-chain per- and polyfluoroalkyl substances on the concentrations of perfluoroalkyl acids and their precursors in the environment? A systematic review protocol Environmental Evidence 2015, 4 (1) 1– 13 DOI: 10.1186/2047-2382-4-3
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    Working Towards a Global Emission Inventory of PFASs; Environment Directorate, Organization for Economic Cooperation and Development: Paris, 2015.
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    Wang, Z.; Cousins, I. T.; Scheringer, M.; Buck, R. C.; Hungerbühler, K. Global emission inventories for C 4–C 14 perfluoroalkyl carboxylic acid (PFCA) homologues from 1951 to 2030, Part I: production and emissions from quantifiable sources Environ. Int. 2014, 70, 62– 75 DOI: 10.1016/j.envint.2014.04.013
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    Butenhoff, J. L.; Chang, S.-C.; Ehresman, D. J.; York, R. G. Evaluation of potential reproductive and developmental toxicity of potassium perfluorohexanesulfonate in Sprague Dawley rats Reprod. Toxicol. 2009, 27 (3) 331– 341 DOI: 10.1016/j.reprotox.2009.01.004
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    Evaluation of potential reproductive and developmental toxicity of potassium perfluorohexanesulfonate in Sprague Dawley rats
    Butenhoff, John L.; Chang, Shu-Ching; Ehresman, David J.; York, Raymond G.
    Reproductive Toxicology (2009), 27 (3-4), 331-341CODEN: REPTED; ISSN:0890-6238. (Elsevier B.V.)
    This study evaluated the potential reproductive and developmental toxicity of perfluorohexanesulfonate (PFHxS), a surfactant found in sera of the general population. In a modified OECD 422 guideline-based design, 15 rats per sex and treatment group (control, 0.3, 1, 3, and 10 mg/kg-d) were dosed by gavage with potassium PFHxS (K+PFHxS) or vehicle (0.5% CM-cellulose) 14 days prior to cohabitation, during cohabitation, and until the day before sacrifice (21 days of lactation or presumed gestation day 25 (if not pregnant) for females and min. of 42 days of treatment for males). Offspring were not dosed by gavage but were exposed by placental transfer in utero and potentially exposed via milk. Evaluations were made for reproductive success, clin. signs, body wt., food consumption, estrous cycling, neurobehavioral effects, gross and microscopic anatomy of selected organs, sperm, hematol., clin. pathol., and concn. of PFHxS in serum and liver. Addnl. 3 rats per sex per group were added to obtain sera and liver samples for PFHxS concn. detns. during the study. No reproductive or developmental effects were obsd. There were no treatment-related effects in dams or offspring. K+PFHxS-induced effects noted in parental males included: (1) at all doses, redns. in serum total cholesterol; (2) at 0.3, 3, and 10 mg/kg-d, decreased prothrombin time; (3) at 3 and 10 mg/kg-d, increased liver-to-body wt. and liver-to-brain wt. ratios, centrilobular hepatocellular hypertrophy, hyperplasia of thyroid follicular cells, and decreased hematocrit; (4) at 10 mg/kg-d, decreased triglycerides and increased albumin, BUN, ALP, Ca2+, and A/G ratio. Serum and liver concns. of PFHxS are reported for parents, fetuses, and pups. PFHxS was not a reproductive or developmental toxicant under study conditions.
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    Birnbaum, L. S.; Grandjean, P. Alternatives to PFASs: Perspectives on the Science Environ. Health Perspect. 2015, 123 (5) A104 DOI: 10.1289/ehp.1509944
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    Caverly Rae, J. M.; Craig, L.; Slone, T. W.; Frame, S. R.; Buxton, L. W.; Kennedy, G. L. Evaluation of chronic toxicity and carcinogenicity of ammonium 2,3,3,3-tetrafluoro-2-(heptafluoropropoxy)-propanoate in Sprague–Dawley rats Toxicology Reports 2015, 2, 939– 949 DOI: 10.1016/j.toxrep.2015.06.001
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    Vestergren, R.; Cousins, I. T. Tracking the Pathways of Human Exposure to Perfluorocarboxylates Environ. Sci. Technol. 2009, 43 (15) 5565– 5575 DOI: 10.1021/es900228k
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    Tracking the Pathways of Human Exposure to Perfluorocarboxylates
    Vestergren, Robin; Cousins, Ian T.
    Environmental Science & Technology (2009), 43 (15), 5565-5575CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    A review concerning human exposure to perfluorocarboxylates (PFCA) to provide insights into pathways of human exposure is given. Topics discussed include: concns., homolog patterns, and temporal trends in human sera; exposure ests., homolog patterns, and temporal trends in exposure media; pharmacokinetics and pharmacokinetic modeling of PFCA; concluding remarks; and supporting information (perfluorooctane sulfonate:perfluorooctanoate correlations in human serum, temporal trends of perfluorooctane sulfonate, perfluorononanoate, and perfluorodecanoic acid in human serum, PFCA and precursor compd. concns. in exposure media, explanation of derivation of a 1-compartment pharmacokinetic model, and uncertainty anal. details).
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  14. 14
    D’Hollander, W.; de Voogt, P.; De Coen, W.; Bervoets, L. Perfluorinated Substances in Human Food and Other Sources of Human Exposure. In Reviews of Environmental Contamination and Toxicology; De Voogt, P., Ed.; Springer: New York, 2010; Vol. 208, pp 179– 215.
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    Emmett, E. A.; Shofer, F. S.; Zhang, H.; Freeman, D.; Desai, C.; Shaw, L. M. Community exposure to perfluorooctanoate: relationships between serum concentrations and exposure sources J. Occup. Environ. Med. 2006, 48 (8) 759– 770 DOI: 10.1097/01.jom.0000232486.07658.74
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    Community exposure to perfluorooctanoate: Relationships between serum concentrations and exposure sources
    Emmett, Edward Anthony; Shofer, Frances Susan; Zhang, Hong; Freeman, David; Desai, Chintan; Shaw, Leslie Michael
    Journal of Occupational and Environmental Medicine (2006), 48 (8), 759-770CODEN: JOEMFM; ISSN:1076-2752. (Lippincott Williams & Wilkins)
    Objective: The objective of this study was to det. serum (perfluorooctanoate [PFOA]) in residents near a fluoropolymer prodn. facility: the contributions from air, water, and occupational exposures, personal and dietary habits, and relationships to age and gender. Methods: The authors conducted questionnaire and serum PFOA measurements in a stratified random sample and volunteers residing in locations with the same residential water supply but with higher and lower potential air PFOA exposure. Results: Serum (PFOA) greatly exceeded general population medians. Occupational exposure from prodn. processes using PFOA and residential water had additive effects; no other occupations contributed. Serum (PFOA) depended on the source of residential drinking water, and not potential air exposure. For public water users, the best-fit model included age, tap water drinks per day, servings of home-grown fruit and vegetables, and carbon filter use. Conclusions: Residential water source was the primary determinant of serum (PFOA).
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    Landsteiner, A.; Huset, C.; Williams, A.; Johnson, J. Biomonitoring for Perfluorochemicals in a Minnesota Community With Known Drinking Water Contamination Journal of Environmental Health 2014, 77 (5) 14– 19
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    Hurley, S.; Houtz, E.; Goldberg, D.; Wang, M.; Park, J.-S.; Nelson, D. O.; Reynolds, P.; Bernstein, L.; Anton-Culver, H.; Horn-Ross, P.; Petreas, M. Preliminary Associations between the Detection of Perfluoroalkyl Acids (PFAAs) in Drinking Water and Serum Concentrations in a Sample of California Women Environ. Sci. Technol. Lett. 2016, 3, 264– 269 DOI: 10.1021/acs.estlett.6b00154
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    17
    Preliminary associations between the detection of perfluoroalkyl acids (PFAAs) in drinking water and serum concentrations in a sample of California women
    Hurley, Susan; Houtz, Erika; Goldberg, Debbie; Wang, Miaomiao; Park, June-Soo; Nelson, David O.; Reynolds, Peggy; Bernstein, Leslie; Anton-Culver, Hoda; Horn-Ross, Pamela; Petreas, Myrto
    Environmental Science & Technology Letters (2016), 3 (7), 264-269CODEN: ESTLCU; ISSN:2328-8930. (American Chemical Society)
    This study compared detection of perfluoroalkyl acids (PFAAs) in public drinking water with PFAA serum concns. for 1566 California women. PFAA occurrence in drinking water from U.S. EPA's third Unregulated Contaminant Monitoring Rule (UCMR3) database was linked by residential zip code to study participants. Detectable water concns. of perfluorooctanoic acid (PFOA) ranged from 0.020 to 0.053 μg/L and of perfluorooctanesulfonic acid (PFOS) from 0.041 to 0.156 μg/L. Forty percent of detectable concns. exceeded the 2016 Health Advisory Level of 0.07 μg/L for combined PFOA and PFOS concns. Serum concns. of PFOS and PFOA significantly differed between participants with and without detectable measures of these compds. in water (Wilcoxon P ≤ 0.0007). Median serum concns. of PFOS and PFOA were 29% and 38% higher, resp., among those with detectable levels in water compared to those without detectable levels. Validation of this approach and replication of these results in other study populations are warranted.
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  18. 18
    Hoffman, K.; Webster, T. F.; Bartell, S. M.; Weisskopf, M. G.; Fletcher, T.; Vieira, V. M. 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 DOI: 10.1289/ehp.1002503
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    18
    Private drinking water wells as a source of exposure to perfluorooctanoic acid (PFOA) in communities surrounding a fluoropolymer production facility
    Hoffman, Kate; Webster, Thomas F.; Bartell, Scott M.; Weisskopf, Marc G.; Fletcher, Tony; Vieira, Veronica M.
    Environmental Health Perspectives (2011), 119 (1), 92-97CODEN: EVHPAZ; ISSN:0091-6765. (U. S. Department of Health and Human Services, Public Health Services)
    The C8 Health Project was established in 2005 to collect data on perfluorooctanoic acid (PFOA, or C8) and human health in Ohio and West Virginia communities contaminated by a fluoropolymer prodn. facility. We assessed PFOA exposure via contaminated drinking water in a subset of C8 Health Project participants who drank water from private wells. Participants provided demog. information and residential, occupational, and medical histories. Lab. analyses were conducted to det. serum-PFOA concns. PFOA data were collected from 2001 through 2005 from 62 private drinking water wells. We examd. the relationship between drinking water and PFOA levels in serum using robust regression methods. As a comparison with regression models, we used a first-order, single-compartment pharmacokinetic model to est. the serum:drinking-water concn. ratio at steady state. The median serum PFOA concn. in 108 study participants who used private wells was 75.7 μg/L, approx. 20 times greater than the levels in the U.S. general population but similar to those of local residents who drank public water. Each 1 μg/L increase in PFOA levels in drinking water was assocd. with an increase in serum concns. of 141.5 μg/L (95% confidence interval, 134.9-148.1). The serum:drinking-water concn. ratio for the steady-state pharmacokinetic model was 114. PFOA-contaminated drinking water is a significant contributor to PFOA levels in serum in the study population. Regression methods and pharmacokinetic modeling produced similar ests. of the relationship.
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    Shin, H.-M.; Vieira, V. M.; Ryan, P. B.; Detwiler, R.; Sanders, B.; Steenland, K.; Bartell, S. M. Environmental Fate and Transport Modeling for Perfluorooctanoic Acid Emitted from the Washington Works Facility in West Virginia Environ. Sci. Technol. 2011, 45 (4) 1435– 1442 DOI: 10.1021/es102769t
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    19
    Environmental Fate and Transport Modeling for Perfluorooctanoic Acid Emitted from the Washington Works Facility in West Virginia
    Shin, Hyeong-Moo; Vieira, Veronica M.; Ryan, P. Barry; Detwiler, Russell; Sanders, Brett; Steenland, Kyle; Bartell, Scott M.
    Environmental Science & Technology (2011), 45 (4), 1435-1442CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Perfluorooctanoic acid (PFOA) has been detected in environmental samples in Ohio and West Virginia near the Washington Works facility in Parkersburg, West Virginia. This work describes retrospective fate and transport modeling of PFOA concns. in local air, surface water, groundwater, and 6 municipal water systems based on estd. historic emission rates from the facility, PFOA physicochem. properties, and local geol. and meteorol. data beginning in 1951. Several environmental fate and transport modeling systems were integrated to model PFOA air dispersion, transit through the vadose zone, surface water transport, and groundwater flow and transport: AERMOD, PRZM-3, BreZo, MODFLOW, and MT3DMS. Several thousand PFOA measurements in municipal well water were collected in this region since 1998. The integrated modeling system performed better than expected, predicting water concns. within a factor of 2.1 of av. obsd. water concns. for each of the 6 municipal water districts after adjusting the org. C partition coeff. to fit the obsd. data. After model calibration, the Spearman rank correlation coeff. for predicted vs. obsd. water concns. was 0.87. These models may be useful to est. past and future public well water PFOA concns. in this region.
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    Perfluorochemical Serum Sampling in the vicinity of Decatur, Alabama, Morgan, Lawrence, and Limestone Counties; Centers for Disease Control and Prevention: Atlanta, 2013.
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    Lifetime Health Advisories and Health Effects Support Documents for Perfluorooctanoic Acid and Perfluorooctane Sulfonate; Environmental Protection Agency: Washington, DC, 2016.
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  22. 22
    Ahrens, L.; Norstrom, K.; Viktor, T.; Cousins, A. P.; Josefsson, S. Stockholm Arlanda Airport as a source of per- and polyfluoroalkyl substances to water, sediment and fish Chemosphere 2015, 129, 33– 8 DOI: 10.1016/j.chemosphere.2014.03.136
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    22
    Stockholm Arlanda Airport as a source of per- and polyfluoroalkyl substances to water, sediment and fish
    Ahrens, Lutz; Norstroem, Karin; Viktor, Tomas; Cousins, Anna Palm; Josefsson, Sarah
    Chemosphere (2015), 129 (), 33-38CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
    Fire training facilities are potential sources of per- and polyfluoroalkyl substances (PFASs) to the nearby environment due to the usage of PFAS-contg. aq. fire-fighting foams (AFFFs). The multimedia distribution of perfluoroalkyl carboxylates (PFCAs), perfluoroalkyl sulfonates (PFSAs), perfluorooctanesulfonamide (PFOSA) and 6:2 fluorotelomer sulfonate (FTSA) was investigated near a fire training facility at Stockholm Arlanda Airport in Sweden. The whole body burden of PFASs in European perch (Perca fluviatilis) was 334 ± 80 μg abs. and was distributed as follows: Gonad > liver ≈ muscle > blood > gill. The bioconcn. factor (BCF) and sediment/water partition coeff. (Kd) increased by 0.6-1.7 and 0.2-0.5 log units, resp., for each addnl. CF2 moiety for PFCAs and PFSAs. PFAS concns. in water showed no significant decreasing trend between 2009 and 2013 (p > 0.05), which indicates that Stockholm Arlanda Airport may be an important source for long-term contamination of the nearby environment with PFASs.
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  23. 23
    Moody, C. A.; Hebert, G. N.; Strauss, S. H.; Field, J. A. Occurrence and persistence of perfluorooctanesulfonate and other perfluorinated surfactants in groundwater at a fire-training area at Wurtsmith Air Force Base, Michigan, USA J. Environ. Monit. 2003, 5 (2) 341– 5 DOI: 10.1039/b212497a
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    23
    Occurrence and persistence of perfluorooctanesulfonate and other perfluorinated surfactants in groundwater at a fire-training area at Wurtsmith Air Force Base, Michigan, USA
    Moody, Cheryl A.; Hebert, Gretchen N.; Strauss, Steven H.; Field, Jennifer A.
    Journal of Environmental Monitoring (2003), 5 (2), 341-345CODEN: JEMOFW; ISSN:1464-0325. (Royal Society of Chemistry)
    Various formulations of fire-extinguishing materials, including aq. film-forming foams (AFFFs), were used as part of fire-training exercises conducted at Wurtsmith Air Force Base (WAFB) in northeastern Michigan from the 1950s until the base was decommissioned in 1993. As a result of past fire-training exercises, AFFF-laden wastewater contg. fuels, solvents, and other materials directly entered groundwater without prior treatment. Perfluorinated surfactants are key components in some AFFF formulations. In this study, groundwater was analyzed for perfluoroalkanesulfonates and perfluorocarboxylates. Perfluoroalkanesulfonates were directly detected using neg.-ion electrospray ionization mass spectrometry. Derivatized perfluorocarboxylates were detected using electron impact gas chromatog.-mass spectrometry. Groundwater from wells around fire-training area FTA-02 at WAFB contained four perfluorinated surfactants ranging in concn. from 3 to 120 μg L-1: perfluorooctanesulfonate (PFOS); perfluorohexanesulfonate; perfluorooctanoate; and perfluorohexanoate. This is the first report demonstrating that PFOS, recently shown to be toxic to organisms ranging from zooplankton to primates, is still present in groundwater in measurable quantities five or more years after its last known use.
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    Schultz, M. M.; Higgins, C. P.; Huset, C. A.; Luthy, R. G.; Barofsky, D. F.; Field, J. A. Fluorochemical mass flows in a municipal wastewater treatment facility Environ. Sci. Technol. 2006, 40 (23) 7350– 7357 DOI: 10.1021/es061025m
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    Fluorochemical Mass Flows in a Municipal Wastewater Treatment Facility
    Schultz, Melissa M.; Higgins, Christopher P.; Huset, Carin A.; Luthy, Richard G.; Barofsky, Douglas F.; Field, Jennifer A.
    Environmental Science & Technology (2006), 40 (23), 7350-7357CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Fluorochems. have widespread applications and are released into municipal wastewater treatment plants via domestic wastewater. A field study was conducted at a full-scale municipal wastewater treatment plant to det. the mass flows of selected fluorochems. Flow-proportional, 24 h samples of raw influent, primary effluent, trickling filter effluent, secondary effluent, and final effluent and grab samples of primary, thickened, activated, and anaerobically digested sludge were collected over 10 days and analyzed by liq. chromatog. electrospray-ionization tandem mass spectrometry. Significant decreases in the mass flows of perfluorohexane sulfonate and perfluorodecanoate occurred during trickling filtration and primary clarification, while activated sludge treatment decreased the mass flow of perfluorohexanoate. Mass flows of the 6:2 fluorotelomer sulfonate and perfluorooctanoate were unchanged as a result of wastewater treatment, which indicates that conventional wastewater treatment is not effective for removal of these compds. A net increase in the mass flows for perfluorooctane and perfluorodecane sulfonates occurred from trickling filtration and activated sludge treatment. Mass flows for perfluoroalkylsulfonamides and perfluorononanoate also increased during activated sludge treatment and are attributed to degrdn. of precursor mols.
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  25. 25
    Loganathan, B. G.; Sajwan, K. S.; Sinclair, E.; Senthil Kumar, K.; Kannan, K. Perfluoroalkyl sulfonates and perfluorocarboxylates in two wastewater treatment facilities in Kentucky and Georgia Water Res. 2007, 41 (20) 4611– 20 DOI: 10.1016/j.watres.2007.06.045
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    Post, G. B.; Cohn, P. D.; Cooper, K. R. Perfluorooctanoic acid (PFOA), an emerging drinking water contaminant: a critical review of recent literature Environ. Res. 2012, 116, 93– 117 DOI: 10.1016/j.envres.2012.03.007
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    Perfluorooctanoic acid (PFOA), an emerging drinking water contaminant: A critical review of recent literature
    Post, Gloria B.; Cohn, Perry D.; Cooper, Keith R.
    Environmental Research (2012), 116 (), 93-117CODEN: ENVRAL; ISSN:0013-9351. (Elsevier)
    A review. Perfluorooctanoic acid (PFOA) is an anthropogenic contaminant that differs in several ways from most other well-studied org. chems. found in drinking water. PFOA is extremely resistant to environmental degrdn. processes and thus persists indefinitely. Unlike most other persistent and bioaccumulative org. pollutants, PFOA is water-sol., does not bind well to soil or sediments, and bioaccumulates in serum rather than in fat. It has been detected in finished drinking water and drinking water sources impacted by releases from industrial facilities and waste water treatment plants, as well as in waters with no known point sources. However, the overall occurrence and population exposure from drinking water is not known. PFOA persists in humans with a half-life of several years and is found in the serum of almost all U.S. residents and in populations worldwide. Exposure sources include food, food packaging, consumer products, house dust, and drinking water. Continued exposure to even relatively low concns. in drinking water can substantially increase total human exposure, with a serum:drinking water ratio of about 100:1. For example, ongoing exposures to drinking water concns. of 10 ng/L, 40 ng/L, 100 ng/L, or 400 ng/L are expected to increase mean serum levels by about 25%, 100%, 250%, and 1000%, resp., from the general population background serum level of about 4 ng/mL. Infants are potentially a sensitive subpopulation for PFOA's developmental effects, and their exposure through breast milk from mothers who use contaminated drinking water and/or from formula prepd. with contaminated drinking water is higher than in adults exposed to the same drinking water concn. Numerous health endpoints are assocd. with human PFOA exposure in the general population, communities with contaminated drinking water, and workers. As is the case for most such epidemiol. studies, causality for these effects is not proven. Unlike most other well-studied drinking water contaminants, the human dose-response curve for several effects appears to be steepest at the lower exposure levels, including the general population range, with no apparent threshold for some endpoints. There is concordance in animals and humans for some effects, while humans and animals appear to react differently for other effects such as lipid metab. PFOA was classified as "likely to be carcinogenic in humans" by the USEPA Science Advisory Board. In animal studies, developmental effects have been identified as more sensitive endpoints for toxicity than carcinogenicity or the long-established hepatic effects. Notably, exposure to an environmentally relevant drinking water concn. caused adverse effects on mammary gland development in mice. This paper reviews current information relevant to the assessment of PFOA as an emerging drinking water contaminant. This information suggests that continued human exposure to even relatively low concns. of PFOA in drinking water results in elevated body burdens that may increase the risk of health effects.
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    Application of WWTP biosolids and resulting perfluorinated compound contamination of surface and well water in Decatur, Alabama, USA
    Lindstrom, Andrew B.; Strynar, Mark J.; Delinsky, Amy D.; Nakayama, Shoji F.; McMillan, Larry; Libelo, E. Laurence; Neill, Michael; Thomas, Lee
    Environmental Science & Technology (2011), 45 (19), 8015-8021CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Perfluorinated chems. (PFCs) such as perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) have been produced and used in a wide range of industrial and consumer products for many decades. Their resistance to degrdn. has led to their widespread distribution in the environment, but little is known about how humans become exposed. Recent studies have demonstrated that the application of PFC contaminated biosolids can have important effects on local environments, ultimately leading to demonstrable human exposures. This manuscript describes a situation in Decatur, Alabama where PFC contaminated biosolids from a local municipal wastewater treatment facility that had received waste from local fluorochem. facilities were used as a soil amendment in local agricultural fields for as many as twelve years. Ten target PFCs were measured in surface and groundwater samples. Results show that surface and well water in the vicinity of these fields had elevated PFC concns., with 22% of the samples exceeding the U.S. Environmental Protection Agency's Provisional Health Advisory level for PFOA in drinking water of 400 ng/L. Water/soil concn. ratios as high as 0.34 for perfluorohexanoic acid, 0.17 for perfluoroheptanoic acid, and 0.04 for PFOA verify decreasing mobility from soils with increasing chain length while indicating that relatively high transport from soils to surface and well water is possible.
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    Buck, R. C.; Franklin, J.; Berger, U.; Conder, J. M.; Cousins, I. T.; de Voogt, P.; Jensen, A. A.; Kannan, K.; Mabury, S. A.; van Leeuwen, S. P. J. Perfluoroalkyl and Polyfluoroalkyl Substances in the Environment: Terminology, Classification, and Origins Integr. Environ. Assess. Manage. 2011, 7 (4) 513– 541 DOI: 10.1002/ieam.258
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    Integrated Environmental Assessment and Management (2011), 7 (4), 513-541CODEN: IEAMCK; ISSN:1551-3777. (John Wiley & Sons Inc.)
    A review. The primary aim of this article is to provide an overview of perfluoroalkyl and polyfluoroalkyl substances (PFASs) detected in the environment, wildlife, and humans, and recommend clear, specific, and descriptive terminol., names, and acronyms for PFASs. The overarching objective is to unify and harmonize communication on PFASs by offering terminol. for use by the global scientific, regulatory, and industrial communities. A particular emphasis is placed on long-chain perfluoroalkyl acids, substances related to the long-chain perfluoroalkyl acids, and substances intended as alternatives to the use of the long-chain perfluoroalkyl acids or their precursors. First, we define PFASs, classify them into various families, and recommend a pragmatic set of common names and acronyms for both the families and their individual members. Terminol. related to fluorinated polymers is an important aspect of our classification. Second, we provide a brief description of the 2 main prodn. processes, electrochem. fluorination and telomerization, used for introducing perfluoroalkyl moieties into org. compds., and we specify the types of byproducts (isomers and homologues) likely to arise in these processes. Third, we show how the principal families of PFASs are interrelated as industrial, environmental, or metabolic precursors or transformation products of one another. We pay particular attention to those PFASs that have the potential to be converted, by abiotic or biotic environmental processes or by human metab., into long-chain perfluoroalkyl carboxylic or sulfonic acids, which are currently the focus of regulatory action. The Supplemental Data lists 42 families and subfamilies of PFASs and 268 selected individual compds., providing recommended names and acronyms, and structural formulas, as well as Chem. Abstrs. Service registry nos. Integr Environ Assess Manag 2011;7:513-541. © 2011 SETAC.
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    Munoz, G.; Vo Duy, S.; Budzinski, H.; Labadie, P.; Liu, J.; Sauvé, S. Quantitative analysis of poly- and perfluoroalkyl compounds in water matrices using high resolution mass spectrometry: Optimization for a laser diode thermal desorption method Anal. Chim. Acta 2015, 881, 98– 106 DOI: 10.1016/j.aca.2015.04.015
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    Quantitative analysis of poly- and perfluoroalkyl compounds in water matrices using high resolution mass spectrometry: Optimization for a laser diode thermal desorption method
    Munoz, Gabriel; Vo Duy, Sung; Budzinski, Helene; Labadie, Pierre; Liu, Jinxia; Sauve, Sebastien
    Analytica Chimica Acta (2015), 881 (), 98-106CODEN: ACACAM; ISSN:0003-2670. (Elsevier B.V.)
    An alternative anal. technique for the quantitation of 15 poly- and perfluoroalkyl substances (PFASs) in water matrixes is reported. Anal. time between each sample was reduced to <20 s, all target mols. being analyzed in a single run with the use of laser diode thermal desorption atm. pressure chem. ionization (LDTD/APCI) coupled with high resoln. accurate mass (HRMS) orbitrap mass spectrometry. LDTD optimal settings were investigated using either one-factor-at-a-time or exptl. design methodologies, while orbitrap parameters were optimized simultaneously by a Box-Behnken design. Following selection of an adequate sample concn. and purifn. procedure based on solid-phase extn. and graphite clean-up, the method was validated in an influent wastewater matrix. Environmentally significant limits of detection were reported (0.3-4 ng/L in wastewater and 0.03-0.2 ng/L in surface water) and out of the 15 target analytes, 11 showed excellent accuracies (±20% of the target values) and recovery rates (75-125%). The method was applied to a selection of environmental samples, including wastewater samples in 7 locations across Canada, as well as surface water and tap water samples from the Montreal region, providing insights into the degree of PFAS contamination in this area.
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    Grandjean, P.; Budtz-Jorgensen, E. Immunotoxicity of perfluorinated alkylates: calculation of benchmark doses based on serum concentrations in children Environ. Health 2013, 12 (1) 35 DOI: 10.1186/1476-069X-12-35
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    Immunotoxicity of perfluorinated alkylates: calculation of benchmark doses based on serum concentrations in children
    Grandjean, Philippe; Budtz-Joergensen, Esben
    Environmental Health (London, United Kingdom) (2013), 12 (), 35CODEN: EHAGAB; ISSN:1476-069X. (BioMed Central Ltd.)
    Background: Immune suppression may be a crit. effect assocd. with exposure to perfluorinated compds. (PFCs), as indicated by recent data on vaccine antibody responses in children. Therefore, this information may be crucial when deciding on exposure limits. Methods: Results obtained from follow-up of a Faroese birth cohort were used. Serum-PFC concns. were measured at age 5 years, and serum antibody concns. against tetanus and diphtheria toxoids were obtained at age 7 years. Benchmark dose results were calcd. in terms of serum concns. for 431 children with complete data using linear and logarithmic curves, and sensitivity analyses were included to explore the impact of the low-dose curve shape. Results: Under different linear assumptions regarding dose-dependence of the effects, benchmark dose levels were about 1.3 ng/mL serum for perfluorooctane sulfonic acid and 0.3 ng/mL serum for perfluorooctanoic acid at a benchmark response of 5%. These results are below av. serum concns. reported in recent population studies. Even lower results were obtained using logarithmic dose-response curves. Assumption of no effect below the lowest obsd. dose resulted in higher benchmark dose results, as did a benchmark response of 10%. Conclusions: The benchmark dose results obtained are in accordance with recent data on toxicity in exptl. models. When the results are converted to approx. exposure limits for drinking water, current limits appear to be several hundred fold too high. Current drinking water limits therefore need to be reconsidered.
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    Houtz, E. F.; Higgins, C. P.; Field, J. A.; Sedlak, D. L. Persistence of perfluoroalkyl acid precursors in AFFF-impacted groundwater and soil Environ. Sci. Technol. 2013, 47 (15) 8187– 8195 DOI: 10.1021/es4018877
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    Persistence of perfluoroalkyl acid precursors in AFFF-impacted groundwater and soil
    Houtz, Erika F.; Higgins, Christopher P.; Field, Jennifer A.; Sedlak, David L.
    Environmental Science & Technology (2013), 47 (15), 8187-8195CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Several classes of polyfluorinated chems. that are potential precursors to the perfluorinated carboxylates and sulfonates are present in aq. film-forming foams (AFFF). To assess the persistence of these AFFF-derived precursors, groundwater, soil, and aquifer solids were obtained in 2011 from an unlined firefighter training area at a U.S. Air Force Base where AFFF was regularly used between 1970 and 1990. To measure the total concn. of perfluorinated carboxylate and sulfonate precursors in archived AFFF formulations and AFFF-impacted environmental samples, a previously developed assay that uses hydroxyl radical to oxidize precursors to perfluorinated carboxylates was adapted for these media. This assay was employed along with direct measurement of 22 precursors found in AFFF and a suite of other poly- and perfluoroalkyl substances (PFASs). On a molar basis, precursors accounted for 41-100% of the total concn. of PFASs in archived AFFF formulations. In the training area, precursors measured by the oxidn. assay accounted for an av. of 23% and 28% of total PFASs (i.e., precursors and perfluorinated carboxylates and sulfonates) in groundwater and solids samples, resp. One precursor in AFFF, perfluorohexane sulfonamide amine, was obsd. on several highly contaminated soil and aquifer solids samples, but no other precursors present in AFFF formulations were detected in any samples at this field site. Suspected intermediate transformation products of precursors in AFFF that were directly measured accounted for approx. half of the total precursor concn. in samples from the training site. The fraction of PFASs consisting of perfluorinated carboxylates and sulfonates was greater in groundwater and solid samples than in any archived AFFF formulations, suggesting that much of the mass of precursors released at the site was converted to perfluorinated carboxylates and sulfonates. The precursors that have persisted at this site may generate significant amts. of addnl. perfluorinated carboxylates and sulfonates upon remediation of contaminated groundwater or aquifer solids.
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    Anderson, R. H.; Long, G. C.; Porter, R. C.; Anderson, J. K. Occurrence of select perfluoroalkyl substances at U.S. Air Force aqueous film-forming foam release sites other than fire-training areas: Field-validation of critical fate and transport properties Chemosphere 2016, 150, 678– 85 DOI: 10.1016/j.chemosphere.2016.01.014
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    Occurrence of select perfluoroalkyl substances at U.S. Air Force aqueous film-forming foam release sites other than fire-training areas: Field-validation of critical fate and transport properties
    Anderson, R. Hunter; Long, G. Cornell; Porter, Ronald C.; Anderson, Janet K.
    Chemosphere (2016), 150 (), 678-685CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
    The use of aq. film-forming foam (AFFF) to extinguish hydrocarbon-based fires is recognized as a significant source of environmental poly- and perfluoroalkyl substances (PFASs). Although the occurrence of select PFASs in soil and groundwater at former fire-training areas (FTAs) at military installations operable since 1970 has been consistently confirmed, studies reporting the occurrence of PFASs at other AFFF-impacted sites (e.g. emergency response locations, AFFF lagoons, hangar-related AFFF storage tanks and pipelines, and fire station testing and maintenance areas) are largely missing from the literature. Further, studies have mostly focused on a single site (i.e., FTAs at military installations) and, thus, lack a comparison of sites with diverse AFFF release history. Therefore, the purpose of this investigation was to evaluate select PFAS occurrence at non-FTA sites on active U. S. Air Force installations with historic AFFF use of varying magnitude. Concns. of fifteen perfluoroalkyl acids (PFAAs) and perfluorooctane sulfonamide (PFOSA), an important PFOS precursor, were measured from several hundred samples among multiple media (i.e., surface soil, subsurface soil, sediment, surface water, and groundwater) collected from forty AFFF-impacted sites across ten installations between March and Sept. 2014, representing one of the most comprehensive datasets on environmental PFAS occurrence to date. Differences in detection frequencies and obsd. concns. due to AFFF release vol. are presented along with rigorous data analyses that quant. demonstrate phase-dependent (i.e., solid-phase vs aq.-phase) differences in the chem. signature as a function of carbon chain-length and in situ PFOS (and to a slightly lesser extent PFHxS) formation, presumably due to precursor biotransformation.
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    Sinclair, E.; Kannan, K. Mass Loading and Fate of Perfluoroalkyl Surfactants in Wastewater Treatment Plants Environ. Sci. Technol. 2006, 40 (5) 1408– 1414 DOI: 10.1021/es051798v
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    Mass Loading and Fate of Perfluoroalkyl Surfactants in Wastewater Treatment Plants
    Sinclair, Ewan; Kannan, Kurunthachalam
    Environmental Science and Technology (2006), 40 (5), 1408-1414CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Wastewater treatment plants have recently been identified as a significant pathway for the introduction of perfluoroalkyl surfactants (PASs) to natural waters. We measured concns. and fate of several PASs in six wastewater treatment plants (WWTPs) in New York State. We also monitored and measured matrix effects (ionization suppression and enhancement) by postcolumn infusion and std. addns. Concns. of perfluorooctanoate (PFOA) in effluents of the 6 WWTPs were 58-1050 ng/L. Perfluorooctanesulfonate (PFOS) was also ubiquitous in effluents of these WWTPs, albeit at much lower concns. (3-68 ng/L). Two of these WWTPs used identical treatment processes, with similar hydraulic retentions, but differed only in that Plant B treated domestic and com. waste, whereas Plant A had an addnl. industrial influence. We found that this industrial influence resulted in significantly greater mass flows of all of the PASs analyzed. Primary treatment was found to have no effect on the mass flows of PASs. Secondary treatment by activated sludge in Plant A significantly increased (p <0.05) the mass flows of PFOS, PFOA, perfluorononanoate (PFNA), perfluorodecanoate (PFDA), and perfluoroundecanoate (PFUnDA). However, in Plant B, only the mass flow of PFOA was significantly increased. The obsd. increase in mass flow of several PASs may have resulted from biodegrdn. of precursor compds. such as fluorotelomer alcs., which is supported by significant correlations in the mass flow of PFOA/PFNA and PFDA/PFUnDA. The masses of PFDA and PFUnDA were significantly correlated only after the secondary treatment. In Plant A, concns. of odd-no. PFCAs were greater than those of even-no. PFCAs, and concn. decreased with increasing chain length (from C8 to C12). A different pattern was obsd. in sludge samples, in which the dominance of PFOA decreased, and PFDA and PFUnDA increased, suggesting preferential partitioning of longer-chain PFCAs to sludge.
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    Schaider, L. A.; Rudel, R. A.; Ackerman, J. M.; Dunagan, S. C.; Brody, J. G. Pharmaceuticals, perfluorosurfactants, and other organic wastewater compounds in public drinking water wells in a shallow sand and gravel aquifer Sci. Total Environ. 2014, 468–469, 384– 393 DOI: 10.1016/j.scitotenv.2013.08.067
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    Pharmaceuticals, perfluorosurfactants, and other organic wastewater compounds in public drinking water wells in a shallow sand and gravel aquifer
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    Figure 1

    Figure 1. Hydrologic unit codes (eight-digit HUCs) used as a proxy for watersheds with detectable PFOA and PFOS in drinking water measured in the US EPA’s UCMR3 program (2013–2015). Blank areas represent regions where no data are available.

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    This article references 71 other publications.

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      Perfluoroalkyl substances (PFASs) are a group of environmentally-persistent chems. that have been widely used in many industrial applications. There is human and animal evidence that PFASs may alter levels of reproductive and thyroid-related hormones. However, human studies on the potential age-related effects of PFASs on these outcomes among males and females are limited. We explored the relationship between serum PFASs and serum total testosterone (T), TSH (TSH), and free and total triiodothyronine (FT3, TT3) and thyroxine (FT4, TT4) among males and females 12 to 80 years of age from the 2011-2012 cycle of the National Health and Nutrition Examn. Survey. Assocns. were assessed using multiple linear regression models that were stratified on sex and age categories. Effect ests. from the majority of the adjusted models were not statistically significant. However, exposure to PFASs may be assocd. with increases in FT3, TT3, and FT4 among adult females, but during adolescence, PFASs may be related to increases in TSH among males and decreases in TSH among females. No significant relationships were obsd. between PFASs and T in any of the models. These findings suggest that exposure to PFASs may disrupt thyroid hormone homeostasis.
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      Context: Perfluorinated compds. (PFCs) have emerged as important food contaminants. They cause immune suppression in a rodent model at serum concns. similar to those occurring in the US population, but adverse health effects of PFC exposure are poorly understood. Objective: To det. whether PFC exposure is assocd. with antibody response to childhood vaccinations. Design, Setting, and Participants: Prospective study of a birth cohort from the National Hospital in the Faroe Islands. A total of 656 consecutive singleton births were recruited during 1997-2001, and 587 participated in follow-up through 2008. Main Outcome Measures: Serum antibody concns. against tetanus and diphtheria toxoids at ages 5 and 7 years. Results: Similar to results of prior studies in the United States, the PFCs with the highest serum concns. were perfluorooctane sulfonic acid (PFOS) and perfluorooctanoic acid (PFOA). Among PFCs in maternal pregnancy serum, PFOS showed the strongest neg. correlations with antibody concns. at age 5 years, for which a 2-fold greater concn. of exposure was assocd. with a difference of -39% (95% CI, -55% to -17%) in the diphtheria antibody concn. PFCs in the child's serum at age 5 years showed uniformly neg. assocns. with antibody levels, esp. at age 7 years, except that the tetanus antibody level following PFOS exposure was not statistically significant. In a structural equation model, a 2-fold greater concn. of major PFCs in child serum was assocd. with a difference of -49% (95% CI, -67% to -23%) in the overall antibody concn. A 2-fold increase in PFOS and PFOA concns. at age 5 years was assocd. with odds ratios between 2.38 (95% CI, 0.89 to 6.35) and 4.20 (95% CI, 1.54 to 11.44) for falling below a clin. protective level of 0.1 IU/mL for tetanus and diphtheria antibodies at age 7 years. Conclusion: Elevated exposures to PFCs were assocd. with reduced humoral immune response to routine childhood immunizations in children aged 5 and 7 years.
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      BACKGROUND: Perfluorooctanoic acid (PFOA) is a synthetic chemical ubiquitous in the serum of U.S. residents. It causes liver, testicular, and pancreatic tumors in rats. Human studies are sparse. OBJECTIVE: We examined cancer incidence in Mid-Ohio Valley residents exposed to PFOA in drinking water due to chemical plant emissions. METHODS: The cohort consisted of adult community residents who resided in contaminated water districts or worked at a local chemical plant. Most participated in a 2005-2006 baseline survey in which serum PFOA was measured. We interviewed the cohort in 2008-2011 to obtain further medical history. Retrospective yearly PFOA serum concentrations were estimated for each participant from 1952 through 2011. Self-reported cancers were validated through medical records and cancer registry review. We estimated the association between cancer and cumulative PFOA serum concentration using proportional hazards models. RESULTS: Participants (n = 32,254) reported 2,507 validated cancers (21 different cancer types). Estimated cumulative serum PFOA concentrations were positively associated with kidney and testicular cancer [hazard ratio (HR) = 1.10; 95% CI: 0.98, 1.24 and HR = 1.34; 95% CI: 1.00, 1.79, respectively, for 1-unit increases in ln-transformed serum PFOA]. Categorical analyses also indicated positive trends with increasing exposures for both cancers: for kidney cancer HRs for increasing exposure quartiles were 1.0, 1.23, 1.48, and 1.58 (linear trend test p = 0.18) and for testicular cancer, HRs were 1.0, 1.04, 1.91, 3.17 (linear trend test p = 0.04). CONCLUSIONS: PFOA exposure was associated with kidney and testicular cancer in this population. Because this is largely a survivor cohort, findings must be interpreted with caution, especially for highly fatal cancers such as pancreatic and lung cancer.
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      This study compared detection of perfluoroalkyl acids (PFAAs) in public drinking water with PFAA serum concns. for 1566 California women. PFAA occurrence in drinking water from U.S. EPA's third Unregulated Contaminant Monitoring Rule (UCMR3) database was linked by residential zip code to study participants. Detectable water concns. of perfluorooctanoic acid (PFOA) ranged from 0.020 to 0.053 μg/L and of perfluorooctanesulfonic acid (PFOS) from 0.041 to 0.156 μg/L. Forty percent of detectable concns. exceeded the 2016 Health Advisory Level of 0.07 μg/L for combined PFOA and PFOS concns. Serum concns. of PFOS and PFOA significantly differed between participants with and without detectable measures of these compds. in water (Wilcoxon P ≤ 0.0007). Median serum concns. of PFOS and PFOA were 29% and 38% higher, resp., among those with detectable levels in water compared to those without detectable levels. Validation of this approach and replication of these results in other study populations are warranted.
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      Hoffman, K.; Webster, T. F.; Bartell, S. M.; Weisskopf, M. G.; Fletcher, T.; Vieira, V. M. 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 DOI: 10.1289/ehp.1002503
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      Private drinking water wells as a source of exposure to perfluorooctanoic acid (PFOA) in communities surrounding a fluoropolymer production facility
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      Environmental Health Perspectives (2011), 119 (1), 92-97CODEN: EVHPAZ; ISSN:0091-6765. (U. S. Department of Health and Human Services, Public Health Services)
      The C8 Health Project was established in 2005 to collect data on perfluorooctanoic acid (PFOA, or C8) and human health in Ohio and West Virginia communities contaminated by a fluoropolymer prodn. facility. We assessed PFOA exposure via contaminated drinking water in a subset of C8 Health Project participants who drank water from private wells. Participants provided demog. information and residential, occupational, and medical histories. Lab. analyses were conducted to det. serum-PFOA concns. PFOA data were collected from 2001 through 2005 from 62 private drinking water wells. We examd. the relationship between drinking water and PFOA levels in serum using robust regression methods. As a comparison with regression models, we used a first-order, single-compartment pharmacokinetic model to est. the serum:drinking-water concn. ratio at steady state. The median serum PFOA concn. in 108 study participants who used private wells was 75.7 μg/L, approx. 20 times greater than the levels in the U.S. general population but similar to those of local residents who drank public water. Each 1 μg/L increase in PFOA levels in drinking water was assocd. with an increase in serum concns. of 141.5 μg/L (95% confidence interval, 134.9-148.1). The serum:drinking-water concn. ratio for the steady-state pharmacokinetic model was 114. PFOA-contaminated drinking water is a significant contributor to PFOA levels in serum in the study population. Regression methods and pharmacokinetic modeling produced similar ests. of the relationship.
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      Shin, H.-M.; Vieira, V. M.; Ryan, P. B.; Detwiler, R.; Sanders, B.; Steenland, K.; Bartell, S. M. Environmental Fate and Transport Modeling for Perfluorooctanoic Acid Emitted from the Washington Works Facility in West Virginia Environ. Sci. Technol. 2011, 45 (4) 1435– 1442 DOI: 10.1021/es102769t
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      Environmental Fate and Transport Modeling for Perfluorooctanoic Acid Emitted from the Washington Works Facility in West Virginia
      Shin, Hyeong-Moo; Vieira, Veronica M.; Ryan, P. Barry; Detwiler, Russell; Sanders, Brett; Steenland, Kyle; Bartell, Scott M.
      Environmental Science & Technology (2011), 45 (4), 1435-1442CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Perfluorooctanoic acid (PFOA) has been detected in environmental samples in Ohio and West Virginia near the Washington Works facility in Parkersburg, West Virginia. This work describes retrospective fate and transport modeling of PFOA concns. in local air, surface water, groundwater, and 6 municipal water systems based on estd. historic emission rates from the facility, PFOA physicochem. properties, and local geol. and meteorol. data beginning in 1951. Several environmental fate and transport modeling systems were integrated to model PFOA air dispersion, transit through the vadose zone, surface water transport, and groundwater flow and transport: AERMOD, PRZM-3, BreZo, MODFLOW, and MT3DMS. Several thousand PFOA measurements in municipal well water were collected in this region since 1998. The integrated modeling system performed better than expected, predicting water concns. within a factor of 2.1 of av. obsd. water concns. for each of the 6 municipal water districts after adjusting the org. C partition coeff. to fit the obsd. data. After model calibration, the Spearman rank correlation coeff. for predicted vs. obsd. water concns. was 0.87. These models may be useful to est. past and future public well water PFOA concns. in this region.
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      Lifetime Health Advisories and Health Effects Support Documents for Perfluorooctanoic Acid and Perfluorooctane Sulfonate; Environmental Protection Agency: Washington, DC, 2016.
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      Ahrens, L.; Norstrom, K.; Viktor, T.; Cousins, A. P.; Josefsson, S. Stockholm Arlanda Airport as a source of per- and polyfluoroalkyl substances to water, sediment and fish Chemosphere 2015, 129, 33– 8 DOI: 10.1016/j.chemosphere.2014.03.136
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      Stockholm Arlanda Airport as a source of per- and polyfluoroalkyl substances to water, sediment and fish
      Ahrens, Lutz; Norstroem, Karin; Viktor, Tomas; Cousins, Anna Palm; Josefsson, Sarah
      Chemosphere (2015), 129 (), 33-38CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
      Fire training facilities are potential sources of per- and polyfluoroalkyl substances (PFASs) to the nearby environment due to the usage of PFAS-contg. aq. fire-fighting foams (AFFFs). The multimedia distribution of perfluoroalkyl carboxylates (PFCAs), perfluoroalkyl sulfonates (PFSAs), perfluorooctanesulfonamide (PFOSA) and 6:2 fluorotelomer sulfonate (FTSA) was investigated near a fire training facility at Stockholm Arlanda Airport in Sweden. The whole body burden of PFASs in European perch (Perca fluviatilis) was 334 ± 80 μg abs. and was distributed as follows: Gonad > liver ≈ muscle > blood > gill. The bioconcn. factor (BCF) and sediment/water partition coeff. (Kd) increased by 0.6-1.7 and 0.2-0.5 log units, resp., for each addnl. CF2 moiety for PFCAs and PFSAs. PFAS concns. in water showed no significant decreasing trend between 2009 and 2013 (p > 0.05), which indicates that Stockholm Arlanda Airport may be an important source for long-term contamination of the nearby environment with PFASs.
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      Moody, C. A.; Hebert, G. N.; Strauss, S. H.; Field, J. A. Occurrence and persistence of perfluorooctanesulfonate and other perfluorinated surfactants in groundwater at a fire-training area at Wurtsmith Air Force Base, Michigan, USA J. Environ. Monit. 2003, 5 (2) 341– 5 DOI: 10.1039/b212497a
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      Occurrence and persistence of perfluorooctanesulfonate and other perfluorinated surfactants in groundwater at a fire-training area at Wurtsmith Air Force Base, Michigan, USA
      Moody, Cheryl A.; Hebert, Gretchen N.; Strauss, Steven H.; Field, Jennifer A.
      Journal of Environmental Monitoring (2003), 5 (2), 341-345CODEN: JEMOFW; ISSN:1464-0325. (Royal Society of Chemistry)
      Various formulations of fire-extinguishing materials, including aq. film-forming foams (AFFFs), were used as part of fire-training exercises conducted at Wurtsmith Air Force Base (WAFB) in northeastern Michigan from the 1950s until the base was decommissioned in 1993. As a result of past fire-training exercises, AFFF-laden wastewater contg. fuels, solvents, and other materials directly entered groundwater without prior treatment. Perfluorinated surfactants are key components in some AFFF formulations. In this study, groundwater was analyzed for perfluoroalkanesulfonates and perfluorocarboxylates. Perfluoroalkanesulfonates were directly detected using neg.-ion electrospray ionization mass spectrometry. Derivatized perfluorocarboxylates were detected using electron impact gas chromatog.-mass spectrometry. Groundwater from wells around fire-training area FTA-02 at WAFB contained four perfluorinated surfactants ranging in concn. from 3 to 120 μg L-1: perfluorooctanesulfonate (PFOS); perfluorohexanesulfonate; perfluorooctanoate; and perfluorohexanoate. This is the first report demonstrating that PFOS, recently shown to be toxic to organisms ranging from zooplankton to primates, is still present in groundwater in measurable quantities five or more years after its last known use.
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      Schultz, M. M.; Higgins, C. P.; Huset, C. A.; Luthy, R. G.; Barofsky, D. F.; Field, J. A. Fluorochemical mass flows in a municipal wastewater treatment facility Environ. Sci. Technol. 2006, 40 (23) 7350– 7357 DOI: 10.1021/es061025m
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      Fluorochemical Mass Flows in a Municipal Wastewater Treatment Facility
      Schultz, Melissa M.; Higgins, Christopher P.; Huset, Carin A.; Luthy, Richard G.; Barofsky, Douglas F.; Field, Jennifer A.
      Environmental Science & Technology (2006), 40 (23), 7350-7357CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Fluorochems. have widespread applications and are released into municipal wastewater treatment plants via domestic wastewater. A field study was conducted at a full-scale municipal wastewater treatment plant to det. the mass flows of selected fluorochems. Flow-proportional, 24 h samples of raw influent, primary effluent, trickling filter effluent, secondary effluent, and final effluent and grab samples of primary, thickened, activated, and anaerobically digested sludge were collected over 10 days and analyzed by liq. chromatog. electrospray-ionization tandem mass spectrometry. Significant decreases in the mass flows of perfluorohexane sulfonate and perfluorodecanoate occurred during trickling filtration and primary clarification, while activated sludge treatment decreased the mass flow of perfluorohexanoate. Mass flows of the 6:2 fluorotelomer sulfonate and perfluorooctanoate were unchanged as a result of wastewater treatment, which indicates that conventional wastewater treatment is not effective for removal of these compds. A net increase in the mass flows for perfluorooctane and perfluorodecane sulfonates occurred from trickling filtration and activated sludge treatment. Mass flows for perfluoroalkylsulfonamides and perfluorononanoate also increased during activated sludge treatment and are attributed to degrdn. of precursor mols.
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      Loganathan, B. G.; Sajwan, K. S.; Sinclair, E.; Senthil Kumar, K.; Kannan, K. Perfluoroalkyl sulfonates and perfluorocarboxylates in two wastewater treatment facilities in Kentucky and Georgia Water Res. 2007, 41 (20) 4611– 20 DOI: 10.1016/j.watres.2007.06.045
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      Post, G. B.; Cohn, P. D.; Cooper, K. R. Perfluorooctanoic acid (PFOA), an emerging drinking water contaminant: a critical review of recent literature Environ. Res. 2012, 116, 93– 117 DOI: 10.1016/j.envres.2012.03.007
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      Perfluorooctanoic acid (PFOA), an emerging drinking water contaminant: A critical review of recent literature
      Post, Gloria B.; Cohn, Perry D.; Cooper, Keith R.
      Environmental Research (2012), 116 (), 93-117CODEN: ENVRAL; ISSN:0013-9351. (Elsevier)
      A review. Perfluorooctanoic acid (PFOA) is an anthropogenic contaminant that differs in several ways from most other well-studied org. chems. found in drinking water. PFOA is extremely resistant to environmental degrdn. processes and thus persists indefinitely. Unlike most other persistent and bioaccumulative org. pollutants, PFOA is water-sol., does not bind well to soil or sediments, and bioaccumulates in serum rather than in fat. It has been detected in finished drinking water and drinking water sources impacted by releases from industrial facilities and waste water treatment plants, as well as in waters with no known point sources. However, the overall occurrence and population exposure from drinking water is not known. PFOA persists in humans with a half-life of several years and is found in the serum of almost all U.S. residents and in populations worldwide. Exposure sources include food, food packaging, consumer products, house dust, and drinking water. Continued exposure to even relatively low concns. in drinking water can substantially increase total human exposure, with a serum:drinking water ratio of about 100:1. For example, ongoing exposures to drinking water concns. of 10 ng/L, 40 ng/L, 100 ng/L, or 400 ng/L are expected to increase mean serum levels by about 25%, 100%, 250%, and 1000%, resp., from the general population background serum level of about 4 ng/mL. Infants are potentially a sensitive subpopulation for PFOA's developmental effects, and their exposure through breast milk from mothers who use contaminated drinking water and/or from formula prepd. with contaminated drinking water is higher than in adults exposed to the same drinking water concn. Numerous health endpoints are assocd. with human PFOA exposure in the general population, communities with contaminated drinking water, and workers. As is the case for most such epidemiol. studies, causality for these effects is not proven. Unlike most other well-studied drinking water contaminants, the human dose-response curve for several effects appears to be steepest at the lower exposure levels, including the general population range, with no apparent threshold for some endpoints. There is concordance in animals and humans for some effects, while humans and animals appear to react differently for other effects such as lipid metab. PFOA was classified as "likely to be carcinogenic in humans" by the USEPA Science Advisory Board. In animal studies, developmental effects have been identified as more sensitive endpoints for toxicity than carcinogenicity or the long-established hepatic effects. Notably, exposure to an environmentally relevant drinking water concn. caused adverse effects on mammary gland development in mice. This paper reviews current information relevant to the assessment of PFOA as an emerging drinking water contaminant. This information suggests that continued human exposure to even relatively low concns. of PFOA in drinking water results in elevated body burdens that may increase the risk of health effects.
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      Lindstrom, A. B.; Strynar, M. J.; Delinsky, A. D.; Nakayama, S. F.; McMillan, L.; Libelo, E. L.; Neill, M.; Thomas, L. Application of WWTP biosolids and resulting perfluorinated compound contamination of surface and well water in Decatur, Alabama, USA Environ. Sci. Technol. 2011, 45 (19) 8015– 8021 DOI: 10.1021/es1039425
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      Application of WWTP biosolids and resulting perfluorinated compound contamination of surface and well water in Decatur, Alabama, USA
      Lindstrom, Andrew B.; Strynar, Mark J.; Delinsky, Amy D.; Nakayama, Shoji F.; McMillan, Larry; Libelo, E. Laurence; Neill, Michael; Thomas, Lee
      Environmental Science & Technology (2011), 45 (19), 8015-8021CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Perfluorinated chems. (PFCs) such as perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) have been produced and used in a wide range of industrial and consumer products for many decades. Their resistance to degrdn. has led to their widespread distribution in the environment, but little is known about how humans become exposed. Recent studies have demonstrated that the application of PFC contaminated biosolids can have important effects on local environments, ultimately leading to demonstrable human exposures. This manuscript describes a situation in Decatur, Alabama where PFC contaminated biosolids from a local municipal wastewater treatment facility that had received waste from local fluorochem. facilities were used as a soil amendment in local agricultural fields for as many as twelve years. Ten target PFCs were measured in surface and groundwater samples. Results show that surface and well water in the vicinity of these fields had elevated PFC concns., with 22% of the samples exceeding the U.S. Environmental Protection Agency's Provisional Health Advisory level for PFOA in drinking water of 400 ng/L. Water/soil concn. ratios as high as 0.34 for perfluorohexanoic acid, 0.17 for perfluoroheptanoic acid, and 0.04 for PFOA verify decreasing mobility from soils with increasing chain length while indicating that relatively high transport from soils to surface and well water is possible.
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      Third Unregulated Contaminant Monitoring Rule; Environmental Protection Agency: Washington, DC (https://http://www.epa.gov/dwucmr/occurrence-data-unregulated-contaminant-monitoring-rule-3) (accessed May, 23, 2016) .
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      Per- and Polyfluoroalkyl Substances (PFASs) under TSCA; Environmental Protection Agency: Washington, DC (https://http://www.epa.gov/assessing-and-managing-chemicals-under-tsca/and-polyfluoroalkyl-substances-pfass-under-tsca).
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      Vermont Perfluorooctanoic acid (PFOA) and Perfluorooctanesulfonic acid (PFOS) Vermont Drinking Water Health Advisory (https://anrweb.vt.gov/PubDocs/DEC/PFOA/PFOA%20-%20PFOS%20Health%20Advisories/Vermont/PFOA_PFOS_HealthAdvisory_June_22_2016.pdf).
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      Buck, R. C.; Franklin, J.; Berger, U.; Conder, J. M.; Cousins, I. T.; de Voogt, P.; Jensen, A. A.; Kannan, K.; Mabury, S. A.; van Leeuwen, S. P. J. Perfluoroalkyl and Polyfluoroalkyl Substances in the Environment: Terminology, Classification, and Origins Integr. Environ. Assess. Manage. 2011, 7 (4) 513– 541 DOI: 10.1002/ieam.258
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      Perfluoroalkyl and polyfluoroalkyl substances in the environment: Terminology, classification, and origins
      Buck, Robert C.; Franklin, James; Berger, Urs; Conder, Jason M.; Cousins, Ian T.; de Voogt, Pim; Jensen, Allan Astrup; Kannan, Kurunthachalam; Mabury, Scott A.; van Leeuwen, Stefan P. J.
      Integrated Environmental Assessment and Management (2011), 7 (4), 513-541CODEN: IEAMCK; ISSN:1551-3777. (John Wiley & Sons Inc.)
      A review. The primary aim of this article is to provide an overview of perfluoroalkyl and polyfluoroalkyl substances (PFASs) detected in the environment, wildlife, and humans, and recommend clear, specific, and descriptive terminol., names, and acronyms for PFASs. The overarching objective is to unify and harmonize communication on PFASs by offering terminol. for use by the global scientific, regulatory, and industrial communities. A particular emphasis is placed on long-chain perfluoroalkyl acids, substances related to the long-chain perfluoroalkyl acids, and substances intended as alternatives to the use of the long-chain perfluoroalkyl acids or their precursors. First, we define PFASs, classify them into various families, and recommend a pragmatic set of common names and acronyms for both the families and their individual members. Terminol. related to fluorinated polymers is an important aspect of our classification. Second, we provide a brief description of the 2 main prodn. processes, electrochem. fluorination and telomerization, used for introducing perfluoroalkyl moieties into org. compds., and we specify the types of byproducts (isomers and homologues) likely to arise in these processes. Third, we show how the principal families of PFASs are interrelated as industrial, environmental, or metabolic precursors or transformation products of one another. We pay particular attention to those PFASs that have the potential to be converted, by abiotic or biotic environmental processes or by human metab., into long-chain perfluoroalkyl carboxylic or sulfonic acids, which are currently the focus of regulatory action. The Supplemental Data lists 42 families and subfamilies of PFASs and 268 selected individual compds., providing recommended names and acronyms, and structural formulas, as well as Chem. Abstrs. Service registry nos. Integr Environ Assess Manag 2011;7:513-541. © 2011 SETAC.
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      Taniyasu, S.; Kannan, K.; Wu, Q.; Kwok, K. Y.; Yeung, L. W. Y.; Lam, P. K. S.; Chittim, B.; Kida, T.; Takasuga, T.; Tsuchiya, Y.; Yamashita, N. Inter-laboratory trials for analysis of perfluorooctanesulfonate and perfluorooctanoate in water samples: Performance and recommendations Anal. Chim. Acta 2013, 770, 111– 120 DOI: 10.1016/j.aca.2013.01.056
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      Happonen, M.; Koivusalo, H.; Malve, O.; Perkola, N.; Juntunen, J.; Huttula, T. Contamination risk of raw drinking water caused by PFOA sources along a river reach in south-western Finland Sci. Total Environ. 2016, 541, 74– 82 DOI: 10.1016/j.scitotenv.2015.09.008
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      Munoz, G.; Vo Duy, S.; Budzinski, H.; Labadie, P.; Liu, J.; Sauvé, S. Quantitative analysis of poly- and perfluoroalkyl compounds in water matrices using high resolution mass spectrometry: Optimization for a laser diode thermal desorption method Anal. Chim. Acta 2015, 881, 98– 106 DOI: 10.1016/j.aca.2015.04.015
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      Quantitative analysis of poly- and perfluoroalkyl compounds in water matrices using high resolution mass spectrometry: Optimization for a laser diode thermal desorption method
      Munoz, Gabriel; Vo Duy, Sung; Budzinski, Helene; Labadie, Pierre; Liu, Jinxia; Sauve, Sebastien
      Analytica Chimica Acta (2015), 881 (), 98-106CODEN: ACACAM; ISSN:0003-2670. (Elsevier B.V.)
      An alternative anal. technique for the quantitation of 15 poly- and perfluoroalkyl substances (PFASs) in water matrixes is reported. Anal. time between each sample was reduced to <20 s, all target mols. being analyzed in a single run with the use of laser diode thermal desorption atm. pressure chem. ionization (LDTD/APCI) coupled with high resoln. accurate mass (HRMS) orbitrap mass spectrometry. LDTD optimal settings were investigated using either one-factor-at-a-time or exptl. design methodologies, while orbitrap parameters were optimized simultaneously by a Box-Behnken design. Following selection of an adequate sample concn. and purifn. procedure based on solid-phase extn. and graphite clean-up, the method was validated in an influent wastewater matrix. Environmentally significant limits of detection were reported (0.3-4 ng/L in wastewater and 0.03-0.2 ng/L in surface water) and out of the 15 target analytes, 11 showed excellent accuracies (±20% of the target values) and recovery rates (75-125%). The method was applied to a selection of environmental samples, including wastewater samples in 7 locations across Canada, as well as surface water and tap water samples from the Montreal region, providing insights into the degree of PFAS contamination in this area.
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      Grandjean, P.; Budtz-Jorgensen, E. Immunotoxicity of perfluorinated alkylates: calculation of benchmark doses based on serum concentrations in children Environ. Health 2013, 12 (1) 35 DOI: 10.1186/1476-069X-12-35
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      Immunotoxicity of perfluorinated alkylates: calculation of benchmark doses based on serum concentrations in children
      Grandjean, Philippe; Budtz-Joergensen, Esben
      Environmental Health (London, United Kingdom) (2013), 12 (), 35CODEN: EHAGAB; ISSN:1476-069X. (BioMed Central Ltd.)
      Background: Immune suppression may be a crit. effect assocd. with exposure to perfluorinated compds. (PFCs), as indicated by recent data on vaccine antibody responses in children. Therefore, this information may be crucial when deciding on exposure limits. Methods: Results obtained from follow-up of a Faroese birth cohort were used. Serum-PFC concns. were measured at age 5 years, and serum antibody concns. against tetanus and diphtheria toxoids were obtained at age 7 years. Benchmark dose results were calcd. in terms of serum concns. for 431 children with complete data using linear and logarithmic curves, and sensitivity analyses were included to explore the impact of the low-dose curve shape. Results: Under different linear assumptions regarding dose-dependence of the effects, benchmark dose levels were about 1.3 ng/mL serum for perfluorooctane sulfonic acid and 0.3 ng/mL serum for perfluorooctanoic acid at a benchmark response of 5%. These results are below av. serum concns. reported in recent population studies. Even lower results were obtained using logarithmic dose-response curves. Assumption of no effect below the lowest obsd. dose resulted in higher benchmark dose results, as did a benchmark response of 10%. Conclusions: The benchmark dose results obtained are in accordance with recent data on toxicity in exptl. models. When the results are converted to approx. exposure limits for drinking water, current limits appear to be several hundred fold too high. Current drinking water limits therefore need to be reconsidered.
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      Valsecchi, S.; Rusconi, M.; Mazzoni, M.; Viviano, G.; Pagnotta, R.; Zaghi, C.; Serrini, G.; Polesello, S. Occurrence and sources of perfluoroalkyl acids in Italian river basins Chemosphere 2015, 129, 126– 134 DOI: 10.1016/j.chemosphere.2014.07.044
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      Persistence of perfluoroalkyl acid precursors in AFFF-impacted groundwater and soil
      Houtz, Erika F.; Higgins, Christopher P.; Field, Jennifer A.; Sedlak, David L.
      Environmental Science & Technology (2013), 47 (15), 8187-8195CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Several classes of polyfluorinated chems. that are potential precursors to the perfluorinated carboxylates and sulfonates are present in aq. film-forming foams (AFFF). To assess the persistence of these AFFF-derived precursors, groundwater, soil, and aquifer solids were obtained in 2011 from an unlined firefighter training area at a U.S. Air Force Base where AFFF was regularly used between 1970 and 1990. To measure the total concn. of perfluorinated carboxylate and sulfonate precursors in archived AFFF formulations and AFFF-impacted environmental samples, a previously developed assay that uses hydroxyl radical to oxidize precursors to perfluorinated carboxylates was adapted for these media. This assay was employed along with direct measurement of 22 precursors found in AFFF and a suite of other poly- and perfluoroalkyl substances (PFASs). On a molar basis, precursors accounted for 41-100% of the total concn. of PFASs in archived AFFF formulations. In the training area, precursors measured by the oxidn. assay accounted for an av. of 23% and 28% of total PFASs (i.e., precursors and perfluorinated carboxylates and sulfonates) in groundwater and solids samples, resp. One precursor in AFFF, perfluorohexane sulfonamide amine, was obsd. on several highly contaminated soil and aquifer solids samples, but no other precursors present in AFFF formulations were detected in any samples at this field site. Suspected intermediate transformation products of precursors in AFFF that were directly measured accounted for approx. half of the total precursor concn. in samples from the training site. The fraction of PFASs consisting of perfluorinated carboxylates and sulfonates was greater in groundwater and solid samples than in any archived AFFF formulations, suggesting that much of the mass of precursors released at the site was converted to perfluorinated carboxylates and sulfonates. The precursors that have persisted at this site may generate significant amts. of addnl. perfluorinated carboxylates and sulfonates upon remediation of contaminated groundwater or aquifer solids.
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    54. 54
      Anderson, R. H.; Long, G. C.; Porter, R. C.; Anderson, J. K. Occurrence of select perfluoroalkyl substances at U.S. Air Force aqueous film-forming foam release sites other than fire-training areas: Field-validation of critical fate and transport properties Chemosphere 2016, 150, 678– 85 DOI: 10.1016/j.chemosphere.2016.01.014
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      54
      Occurrence of select perfluoroalkyl substances at U.S. Air Force aqueous film-forming foam release sites other than fire-training areas: Field-validation of critical fate and transport properties
      Anderson, R. Hunter; Long, G. Cornell; Porter, Ronald C.; Anderson, Janet K.
      Chemosphere (2016), 150 (), 678-685CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
      The use of aq. film-forming foam (AFFF) to extinguish hydrocarbon-based fires is recognized as a significant source of environmental poly- and perfluoroalkyl substances (PFASs). Although the occurrence of select PFASs in soil and groundwater at former fire-training areas (FTAs) at military installations operable since 1970 has been consistently confirmed, studies reporting the occurrence of PFASs at other AFFF-impacted sites (e.g. emergency response locations, AFFF lagoons, hangar-related AFFF storage tanks and pipelines, and fire station testing and maintenance areas) are largely missing from the literature. Further, studies have mostly focused on a single site (i.e., FTAs at military installations) and, thus, lack a comparison of sites with diverse AFFF release history. Therefore, the purpose of this investigation was to evaluate select PFAS occurrence at non-FTA sites on active U. S. Air Force installations with historic AFFF use of varying magnitude. Concns. of fifteen perfluoroalkyl acids (PFAAs) and perfluorooctane sulfonamide (PFOSA), an important PFOS precursor, were measured from several hundred samples among multiple media (i.e., surface soil, subsurface soil, sediment, surface water, and groundwater) collected from forty AFFF-impacted sites across ten installations between March and Sept. 2014, representing one of the most comprehensive datasets on environmental PFAS occurrence to date. Differences in detection frequencies and obsd. concns. due to AFFF release vol. are presented along with rigorous data analyses that quant. demonstrate phase-dependent (i.e., solid-phase vs aq.-phase) differences in the chem. signature as a function of carbon chain-length and in situ PFOS (and to a slightly lesser extent PFHxS) formation, presumably due to precursor biotransformation.
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    55. 55
      Sinclair, E.; Kannan, K. Mass Loading and Fate of Perfluoroalkyl Surfactants in Wastewater Treatment Plants Environ. Sci. Technol. 2006, 40 (5) 1408– 1414 DOI: 10.1021/es051798v
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      Mass Loading and Fate of Perfluoroalkyl Surfactants in Wastewater Treatment Plants
      Sinclair, Ewan; Kannan, Kurunthachalam
      Environmental Science and Technology (2006), 40 (5), 1408-1414CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Wastewater treatment plants have recently been identified as a significant pathway for the introduction of perfluoroalkyl surfactants (PASs) to natural waters. We measured concns. and fate of several PASs in six wastewater treatment plants (WWTPs) in New York State. We also monitored and measured matrix effects (ionization suppression and enhancement) by postcolumn infusion and std. addns. Concns. of perfluorooctanoate (PFOA) in effluents of the 6 WWTPs were 58-1050 ng/L. Perfluorooctanesulfonate (PFOS) was also ubiquitous in effluents of these WWTPs, albeit at much lower concns. (3-68 ng/L). Two of these WWTPs used identical treatment processes, with similar hydraulic retentions, but differed only in that Plant B treated domestic and com. waste, whereas Plant A had an addnl. industrial influence. We found that this industrial influence resulted in significantly greater mass flows of all of the PASs analyzed. Primary treatment was found to have no effect on the mass flows of PASs. Secondary treatment by activated sludge in Plant A significantly increased (p <0.05) the mass flows of PFOS, PFOA, perfluorononanoate (PFNA), perfluorodecanoate (PFDA), and perfluoroundecanoate (PFUnDA). However, in Plant B, only the mass flow of PFOA was significantly increased. The obsd. increase in mass flow of several PASs may have resulted from biodegrdn. of precursor compds. such as fluorotelomer alcs., which is supported by significant correlations in the mass flow of PFOA/PFNA and PFDA/PFUnDA. The masses of PFDA and PFUnDA were significantly correlated only after the secondary treatment. In Plant A, concns. of odd-no. PFCAs were greater than those of even-no. PFCAs, and concn. decreased with increasing chain length (from C8 to C12). A different pattern was obsd. in sludge samples, in which the dominance of PFOA decreased, and PFDA and PFUnDA increased, suggesting preferential partitioning of longer-chain PFCAs to sludge.
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    56. 56
      Schaider, L. A.; Rudel, R. A.; Ackerman, J. M.; Dunagan, S. C.; Brody, J. G. Pharmaceuticals, perfluorosurfactants, and other organic wastewater compounds in public drinking water wells in a shallow sand and gravel aquifer Sci. Total Environ. 2014, 468–469, 384– 393 DOI: 10.1016/j.scitotenv.2013.08.067
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      Pharmaceuticals, perfluorosurfactants, and other organic wastewater compounds in public drinking water wells in a shallow sand and gravel aquifer
      Schaider, Laurel A.; Rudel, Ruthann A.; Ackerman, Janet M.; Dunagan, Sarah C.; Brody, Julia Green
      Science of the Total Environment (2014), 468-469 (), 384-393CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)
      Approx. 40% of U. S. residents rely on groundwater as a source of drinking water. Groundwater, esp. unconfined sand and gravel aquifers, is vulnerable to contamination from septic systems and infiltration of wastewater treatment plant effluent. The authors characterized concns. of pharmaceuticals, perfluorosurfactants, and other org. wastewater compds. (OWCs) in the unconfined sand and gravel aquifer of Cape Cod, Massachusetts, USA, where septic systems are prevalent. Raw water samples from 20 public drinking water supply wells on Cape Cod were tested for 92 OWCs, as well as surrogates of wastewater impact. Fifteen of 20 wells contained at least one OWC; the two most frequently-detected chems. were sulfamethoxazole (antibiotic) and perfluorooctane sulfonate (perfluorosurfactant). Maximum concns. of sulfamethoxazole (113 ng/L) and the anticonvulsant phenytoin (66 ng/L) matched or exceeded max. reported concns. in other U. S. public drinking water sources. The sum of pharmaceutical concns. and the no. of detected chems. were both significantly correlated with nitrate, boron, and extent of unsewered residential and com. development within 500 m, indicating that wastewater surrogates can be useful for identifying wells most likely to contain OWCs. Septic systems appear to be the primary source of OWCs in Cape Cod groundwater, although wastewater treatment plants and other sources were potential contributors to several wells. Drinking water supplies in unconfined aquifers where septic systems are prevalent may be among the most vulnerable to OWCs. The presence of mixts. of OWCs in drinking water raises human health concerns; a full evaluation of potential risks is limited by a lack of health-based guidelines and toxicity assessments.
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      Pascual, P.; Stiber, N.; Sunderland, E. Draft guidance on the development, evaluation, and application of regulatory environmental models; The Council for Regulatory Environmental Modeling, Office of Science Policy, Office of Research and Development, Environmental Protection Agency: Washington, DC, 2003.
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      NRC. Models in Environmental Regulatory Decision Making; National Research Council, Committee on Models in the Regulatory Decision Process, National Academies Press: Washington, DC, 2007.
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      Houtz, E. F.; Sutton, R.; Park, J.-S.; Sedlak, M. Poly- and perfluoroalkyl substances in wastewater: Significance of unknown precursors, manufacturing shifts, and likely AFFF impacts Water Res. 2016, 95, 142– 149 DOI: 10.1016/j.watres.2016.02.055
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      Poly- and perfluoroalkyl substances in wastewater: Significance of unknown precursors, manufacturing shifts, and likely AFFF impacts
      Houtz, Erika F.; Sutton, Rebecca; Park, June-Soo; Sedlak, Margaret
      Water Research (2016), 95 (), 142-149CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)
      In late 2014, wastewater effluent samples were collected from eight treatment plants that discharge to San Francisco (SF) Bay in order to assess poly- and perfluoroalkyl substances (PFASs) currently released from municipal and industrial sources. In addn. to direct measurement of twenty specific PFAS analytes, the total concn. of perfluoroalkyl acid (PFAA) precursors was also indirectly measured by adapting a previously developed oxidn. assay. Effluent from six municipal treatment plants contained similar amts. of total PFASs, with highest median concns. of PFHxA (24 ng/L), followed by PFOA (23 ng/L), PFBA (19 ng/L), and PFOS (15 ng/L). Compared to SF Bay municipal wastewater samples collected in 2009, the short chain perfluorinated carboxylates PFBA and PFHxA rose significantly in concn. Effluent samples from two treatment plants contained much higher levels of PFASs: over two samplings, wastewater from one municipal plant contained an av. of 420 ng/L PFOS and wastewater from an airport industrial treatment plant contained 560 ng/L PFOS, 390 ng/L 6:2 FtS, 570 ng/L PFPeA, and 500 ng/L PFHxA. The elevated levels obsd. in effluent samples from these two plants are likely related to aq. film forming foam (AFFF) sources impacting their influent; PFASs attributable to both current use and discontinued AFFF formulations were obsd. Indirectly measured PFAA precursor compds. accounted for 33%-63% of the total molar concn. of PFASs across all effluent samples and the PFAA precursors indicated by the oxidn. assay were predominately short-chained. PFAS levels in SF Bay effluent samples reflect the manufg. shifts towards shorter chained PFASs while also demonstrating significant impacts from localized usage of AFFF.
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    60. 60
      Konwick, B. J.; Tomy, G. T.; Ismail, N.; Peterson, J. T.; Fauver, R. J.; Higginbotham, D.; Fisk, A. T. Concentrations and patterns of perfluoroalkyl acids in Georgia, USA surface waters near and distant to a major use source Environ. Toxicol. Chem. 2008, 27 (10) 2011– 2018 DOI: 10.1897/07-659.1
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      Clara, M.; Scheffknecht, C.; Scharf, S.; Weiss, S.; Gans, O. Emissions of perfluorinated alkylated substances (PFAS) from point sources--identification of relevant branches Water Sci. Technol. 2008, 58 (1) 59 DOI: 10.2166/wst.2008.641
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      Emissions of perfluorinated alkylated substances (PFAS) from point sources-identification of relevant branches
      Clara, M.; Scheffknecht, C.; Scharf, S.; Weiss, S.; Gans, O.
      Water Science and Technology (2008), 58 (1), 59-66CODEN: WSTED4; ISSN:0273-1223. (IWA Publishing)
      Effluents of wastewater treatment plants are relevant point sources for the emission of hazardous xenobiotic substances to the aquatic environment. One group of substances, which recently entered scientific and political discussions, is the group of the perfluorinated alkylated substances (PFAS). The most studied compds. from this group are perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS), which are the most important degrdn. products of PFAS. These two substances are known to be persistent, bioaccumulative and toxic (PBT). In the present study, eleven PFAS were investigated in effluents of municipal wastewater treatment plants (WWTP) and in industrial wastewaters. PFOS and PFOA proved to be the dominant compds. in all sampled wastewaters. Concns. of up to 340 ng/L of PFOS and up to 220 ng/L of PFOA were obsd. Besides these two compds., perfluorohexanoic acid (PFHxA) was also present in nearly all effluents and max. concns. of up to 280 ng/L were measured. Only N-ethylperfluorooctane sulfonamide (N-EtPFOSA) and its degrdn./metabolisation product perfluorooctane sulfonamide (PFOSA) were either detected below the limit of quantification or were not even detected at all. Beside the effluents of the municipal WWTPs, nine industrial wastewaters from six different industrial branches were also investigated. Significantly, the highest emissions or PFOS were obsd. from metal industry whereas paper industry showed the highest PFOA emission. Several PFAS, esp. perfluorononanoic acid (PFNA), perfluorodecanoic acid (PFDA), perfluorododecanoic acid (PFDoA) and PFOS are predominantly emitted from industrial sources, with concns. being a factor of 10 higher than those obsd. in the municipal WWTP effluents. Perfluorodecane sulfonate (PFDS), N-Et-PFOSA and PFOSA were not detected in any of the sampled industrial point sources.
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      Zhang, C.; Peng, Y.; Niu, X.; Ning, K. Determination of perfluoroalkyl substances in municipal landfill leachates from Beijing, China Asian J. Chem. 2014, 26 (13) 3833
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      Determination of perfluoroalkyl substances in municipal landfill leachates from Beijing, China
      Zhang, Chunhui; Peng, Yi; Niu, Xiameng; Ning, Ke
      Asian Journal of Chemistry (2014), 26 (13), 3833-3836CODEN: AJCHEW; ISSN:0970-7077. (Asian Journal of Chemistry)
      Perfluoroalkyl substances (PFASs) that accumulate in landfills are a potential source of PFASs via leaching into the surface or groundwater environment. In the study, 10 PFASs, including PFHxA, PFHxS, PFHpA, PFOA, PFNA, PFDA, PFUnDA, PFDoDA, PFTrDA and PFOS were detd. in untreated and treated landfill leachates at three landfill sites in Beijing, China. The results showed that PFHxA, PFHpA, PFOA and PFOS were detected in untreated leachates of three landfill sites. The PFASs in treated leachates depended on the different treatment systems. In the full scale treatment, after the biol. treatment and reverse osmosis processing, the leachate showed the lowest concns. and highest removal efficiencies of PFHxA, PFHpA, PFOA and PFOS, followed by landfill leachate after the treatment using biol. treatment, microfiltration and activated carbon. The leachate only treated by biol. treatment had the highest concns. and lowest removal efficiencies of PFASs. The ratio of PFHxA, PFHpA and PFOA concn. of leachate to Beijing tap water was 53.4, 4.5 and 132, resp. The results indicate that municipal landfill leachate is the potential source pollution of PFASs.
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      Busch, J.; Ahrens, L.; Sturm, R.; Ebinghaus, R. Polyfluoroalkyl compounds in landfill leachates Environ. Pollut. 2010, 158 (5) 1467– 1471 DOI: 10.1016/j.envpol.2009.12.031
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      Polyfluoroalkyl compounds in landfill leachates
      Busch, Jan; Ahrens, Lutz; Sturm, Renate; Ebinghaus, Ralf
      Environmental Pollution (Oxford, United Kingdom) (2010), 158 (5), 1467-1471CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)
      Polyfluoroalkyl compds. (PFCs) are widely used in industry and consumer products. These products could end up finally in landfills where their leachates are a potential source for PFCs into the aq. environment. In this study, samples of untreated and treated leachate from 22 landfill sites in Germany were analyzed for 43 PFCs. ΣPFC concns. ranged from 31 to 12,819 ng/L in untreated leachate and 4-8060 ng/L in treated leachate. The dominating compds. in untreated leachate were perfluorobutanoic acid (PFBA) (mean contribution 27%) and perfluorobutane sulfonate (PFBS) (24%). The discharge of PFCs into the aq. environment depended on the cleaning treatment systems. Membrane treatments (reverse osmosis and nanofiltrations) and activated carbon released lower concns. of PFCs into the environment than cleaning systems using wet air oxidn. or only biol. treatment. The mass flows of ΣPFCs into the aq. environment ranged between 0.08 and 956 mg/day.
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      Huset, C. A.; Barlaz, M. A.; Barofsky, D. F.; Field, J. A. Quantitative determination of fluorochemicals in municipal landfill leachates Chemosphere 2011, 82 (10) 1380– 1386 DOI: 10.1016/j.chemosphere.2010.11.072
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      Quantitative determination of fluorochemicals in municipal landfill leachates
      Huset, Carin A.; Barlaz, Morton A.; Barofsky, Douglas F.; Field, Jennifer A.
      Chemosphere (2011), 82 (10), 1380-1386CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
      In total, 24 fluoro-chems. were quantified in landfill leachate recovered from municipal refuse by solid-phase extn., dispersive-C sorbent clean-up, and liq. chromatog./tandem mass spectrometry. This method was applied to 6 landfill leachates from 4 US locations and a leachate generated by a lab. bioreactor contg. residential refuse. All 7 leachates had a common characteristic: short-chain (C4-7) carboxylates or sulfonates were greater in abundance than their resp. longer-chain homologs (≥C8). Perfluoroalkyl carboxylates were the most abundant (67 ± 4% on a nano-molar [nM] basis) fluoro-chems. detd. in leachates; concns. of individual carboxylates were as high as 2800 ng/L. Perfluoroalkyl sulfonates were the next most abundant class (22 ± 2%) on a nM basis; their abundance in each refuse-derived leachate were greater for shorter-chain homologs (C4 and C6) vs. longer-chain homologs (C8 and C10). Perfluorobutane sulfonate concns. were ≤ 2300 ng/L. Sulfonamide derivs. composed 8 ± 2.1% (nM basis) of leachate fluoro-chems.; Me (C4 and C8) and Et (C8) sulfonamide acetic acids were the most abundant. Fluoro-telomer sulfonates (6:2 and 8:2) composed 2.4 ± 1.3% (nM basis) of detected fluoro-chems. and were present in all leachates.
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    65. 65
      Blaine, A. C.; Rich, C. D.; Hundal, L. S.; Lau, C.; Mills, M. A.; Harris, K. M.; Higgins, C. P. Uptake of perfluoroalkyl acids into edible crops via land applied biosolids: Field and greenhouse studies Environ. Sci. Technol. 2013, 47 (24) 14062– 14069 DOI: 10.1021/es403094q
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      Uptake of Perfluoroalkyl Acids into Edible Crops via Land Applied Biosolids: Field and Greenhouse Studies
      Blaine, Andrea C.; Rich, Courtney D.; Hundal, Lakhwinder S.; Lau, Christopher; Mills, Marc A.; Harris, Kimberly M.; Higgins, Christopher P.
      Environmental Science & Technology (2013), 47 (24), 14062-14069CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      The presence of perfluoroalkyl acids (PFAAs) in biosolids destined for use in agriculture has raised concerns about their potential to enter the terrestrial food chain via bioaccumulation in edible plants. Uptake of PFAAs by greenhouse lettuce (Lactuca sativa) and tomato (Lycopersicon lycopersicum) grown in an industrially impacted biosolids-amended soil, a municipal biosolids-amended soil, and a control soil was measured. Bioaccumulation factors (BAFs) were calcd. for the edible portions of both lettuce and tomato. Dry wt. concns. obsd. in lettuce grown in a soil amended (biosolids:soil dry wt. ratio of 1:10) with PFAA industrially contaminated biosolids were up to 266 and 236 ng/g for perfluorobutanoic acid (PFBA) and perfluoropentanoic acid (PFPeA), resp., and reached 56 and 211 ng/g for PFBA and PFPeA in tomato, resp. BAFs for many PFAAs were well above unity, with PFBA having the highest BAF in lettuce (56.8) and PFPeA the highest in tomato (17.1). In addn., the BAFs for PFAAs in greenhouse lettuce decreased approx. 0.3 log units per CF2 group. A limited-scale field study was conducted to verify greenhouse findings. The greatest accumulation was seen for PFBA and PFPeA in both field-grown lettuce and tomato; BAFs for PFBA were highest in both crops. PFAA levels measured in lettuce and tomato grown in field soil amended with only a single application of biosolids (at an agronomic rate for nitrogen) were predominantly below the limit of quantitation (LOQ). In addn., corn (Zea mays) stover, corn grains, and soil were collected from several full-scale biosolids-amended farm fields. At these fields, all PFAAs were below the LOQ in the corn grains and only trace amts. of PFBA and PFPeA were detected in the corn stover. This study confirms that the bioaccumulation of PFAAs from biosolids-amended soils depends strongly on PFAA concns., soil properties, the type of crop, and analyte.
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    66. 66
      Sepulvado, J. G.; Blaine, A. C.; Hundal, L. S.; Higgins, C. P. Occurrence and fate of perfluorochemicals in soil following the land application of municipal biosolids Environ. Sci. Technol. 2011, 45 (19) 8106– 8112 DOI: 10.1021/es103903d
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      Occurrence and fate of perfluorochemicals in soil following the land application of municipal biosolids
      Sepulvado, Jennifer G.; Blaine, Andrea C.; Hundal, Lakhwinder S.; Higgins, Christopher P.
      Environmental Science & Technology (2011), 45 (19), 8106-8112CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      The recent implementation of soil and drinking water screening guidance values for 2 perfluorochems. (PFCs), perfluorooctanoate (PFOA) and perfluorooctane sulfonate (PFOS) by the US EPA, reflects the growing concerns regarding the presence of these persistent and bioaccumulative chems. in the natural environment. Previous work has established the potential risk to the environment from the land application of industrially contaminated biosolids, but studies focusing on environmental risk from land application of typical municipal biosolids are lacking. This study examd. the occurrence and fate of PFCs from land-applied municipal biosolids by evaluating the levels, mass balance, desorption, and transport of PFCs in soils receiving application of municipal biosolids at various loading rates. This study is the 1st to report levels of PFCs in agricultural soils amended with typical municipal biosolids. PFOS was the dominant PFC in both biosolids (80-219 ng/g) and biosolids-amended soil (2-483 ng/g). Concns. of all PFCs in soil increased linearly with increasing biosolids loading rate. These data were used to develop a model for predicting PFC soil concns. in soils amended with typical municipal biosolids using cumulative biosolids loading rates. Mass balance calcns. comparing PFCs applied vs. those recovered in the surface soil interval indicated the potential transformation of PFC precursors. Lab. desorption expts. indicated that the leaching potential of PFCs decreases with increasing chain length and that previously derived org.-C normalized partition coeffs. may not be accurate predictors of the desorption of long-chain PFCs from biosolids-amended soils. Trace levels of PFCs were also detected in soil cores from biosolids-amended soils to depths of 120 cm, suggesting potential movement of these compds. within the soil profile over time and confirming the higher transport potential for short-chain PFCs in soils amended with municipal biosolids.
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      Rich, C. D.; Blaine, A. C.; Hundal, L.; Higgins, C. P. Bioaccumulation of perfluoroalkyl acids by earthworms (Eisenia fetida) exposed to contaminated soils Environ. Sci. Technol. 2015, 49 (2) 881– 8 DOI: 10.1021/es504152d
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      Hölzer, J.; Midasch, O.; Rauchfuss, K.; Kraft, M.; Reupert, R.; Angerer, J.; Kleeschulte, P.; Marschall, N.; Wilhelm, M. Biomonitoring of Perfluorinated Compounds in Children and Adults Exposed to Perfluorooctanoate-Contaminated Drinking Water Environ. Health Perspect. 2008, 116 (5) 651– 657 DOI: 10.1289/ehp.11064
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      Report of Investigation Activities at Select Firefighting Foam Training Areas and Foam Discharge Sites in Minnesota; Minnesota Pollution Control Agency: St. Paul, MN, 2010.
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