Cited by 168Per- and polyfluoroalkyl substances researchFluoride Effects and RemovalToxic Organic Pollutants Impact

Source Attribution of Poly- and Perfluoroalkyl Substances (PFASs) in Surface Waters from Rhode Island and the New York Metropolitan Area

Open access
Zhang, Xianming, Lohmann, Rainer, Dassuncao, Clifton, Hu, Xindi C., Weber, Andrea K., Vecitis, Chad D., Sunderland, Elsie M.·2016·Environmental Science & Technology Letters

Abstract

Exposure to poly- and perfluoroalkyl substances (PFASs) has been associated with adverse health effects in humans and wildlife. Understanding pollution sources is essential for environmental regulation, but source attribution for PFASs has been confounded by limited information about industrial releases and rapid changes in chemical production. Here we use principal component analysis (PCA), hierarchical clustering, and geospatial analysis to understand source contributions to 14 PFASs measured across 37 sites in the northeastern United States in 2014. PFASs are significantly elevated in urban areas compared to rural sites except for perfluorobutanesulfonate, N -methyl perfluorooctanesulfonamidoacetic acid, perfluoroundecanate, and perfluorododecanate. The highest PFAS concentrations across sites were those of perfluorooctanate (PFOA, 56 ng L −1 ) and perfluorohexanesulfonate (PFHxS, 43 ng L −1 ), and perfluorooctanesulfonate (PFOS) levels are lower than earlier measurements of U.S. surface waters. PCA and cluster analysis indicate three main statistical groupings of PFASs. Geospatial analysis of watersheds reveals the first component/cluster originates from a mixture of contemporary point sources such as airports and textile mills. Atmospheric sources from the waste sector are consistent with the second component, and the metal smelting industry plausibly explains the third component. We find this source-attribution technique is effective for better understanding PFAS sources in urban areas.

Integrity signals

Registry

Crossref · 10.1021/acs.estlett.6b00255

Cites

31 of 31 references verified0 citation errors · 0 not checkable

Statistics

Nothing to recompute.

Claims the paper makes

0 of 20 cited sources checked · 0 supported · 0 flagged

  • Findingown data

    The highest PFHxS concentration measured was 43 ng/L, at Site 5 (Mill Cove, RI).

    “Highest concentrations of PFHxS (43 ng L−1) and PFNA (14 ng L−1) were measured at Site 5 (Mill Cove, RI).”
    Quote in the paperNot a substantial claim
  • Findingown data

    The highest PFNA concentration measured was 14 ng/L, at Site 5 (Mill Cove, RI).

    “Highest concentrations of PFHxS (43 ng L−1) and PFNA (14 ng L−1) were measured at Site 5 (Mill Cove, RI).”
    Quote in the paperNot a substantial claim
  • Findingown data

    The maximum PFOS concentration in this study is much lower than maximum levels reported in earlier studies of U.S. surface waters, which ranged from 43 to 244 ng/L.

    “This is much lower than maximum levels reported in earlier studies of US surface waters that range between 43-244 ng L−1 (Table S4) and reflects the continued decline in environmental PFOS burdens in North America following elimination of production in 2002.25,26”
    • Also stated in: § Abstract · plain
      “PFOS levels are lower than earlier measurements of U.S. surface waters.”
    Quote in the paperNot a substantial claim
  • Findingnone given

    No industrial facilities exist upstream of Sites 1 and 6.

    “No industrial facilities exist upstream of Sites 1 and 6.”
    Quote in the paperNot a substantial claim
  • Findingown data

    Geospatial analysis of the watersheds for Sites 5, 19, 20, and 31 reveals a mixture of potential sources.

    “Geospatial analysis of the watersheds for Sites 5, 19, 20 and 31 reveals a mixture of potential sources (Figure S5).”
    Quote in the paperSubstantial claim
  • May combine two claims. 14
  • Classified as probably not a substantial claim. 4
  • May combine two claims.

    Findingown data

    Site 5 (Mill Cove, RI) had the highest summed PFASs across all sites and was dominated by the first component/cluster mixture.

    “Site 5 (Mill Cove, RI) contains the highest summed PFASs across all sites and is dominated by this mixture of PFASs.”
    Quote in the paperSubstantial claim
  • May combine two claims.

    Findingown data

    The second component/cluster explains 19% of PFAS variability and includes PFUnDA, PFDoDA, MeFOSAA, and EtFOSAA.

    “The second component/cluster explains 19% of the variability in PFASs and includes two long-chain PFASs (PFUnDA and PFDoDA) and two precursors to PFOS (MeFOSAA and EtFOSAA) (Figure 2).”
    Quote in the paperSubstantial claim
  • May combine two claims.

    Findingown data

    Landfill/waste management facilities are located within 2 km of Sites 1, 3, and 6 but are not hydrologically connected to the sampling locations.

    “Landfill/waste management facilities are located within 2 km of all three sites but are not hydrologically connected to the sampling locations (Figure S5).”
    Quote in the paperSubstantial claim
  • May combine two claims.

    Findingown data

    The second component profile is most pronounced at Site 3 on the Woonasquatucket River, RI, and is also evident at Site 1 (Slack's Tributary, RI) and Site 6 (Buckeye Brook, RI).

    “This profile is most pronounced at Site 3 along the Woonasquatucket River in RI and is also evident at Site 1 (Slack’s Tributary, RI) and Site 6 (Buckeye Brook, RI).”
    Quote in the paperSubstantial claim
  • May combine two claims.

    Findingown data

    Concentrations of N-MeFOSAA, PFUnDA, and PFDoDA were not spatially variable at most sites and were only slightly elevated at Site 3.

    “Concentrations of N-MeFOSAA, PFUnDA and PFDoDA were not spatially variable at most sites and only slightly elevated at Site 3, consistent with an atmospheric input pathway.”
    Quote in the paperSubstantial claim
  • May combine two claims.

    Findingown data

    PFOA and PFNA were detectable at all sites, and more than 90% of sites had detectable PFHxS, PFOS, PFDA, and 6:2 FtS.

    “All sites had detectable PFOA and PFNA and over 90% contained detectable PFHxS, PFOS, PFDA, and 6:2 FtS (Table S2, S3, Figure S2).”
    Quote in the paperNot a substantial claim
  • May combine two claims.

    Findingown data

    The third component explains 15% of PFAS variability and includes PFPeA, PFOS, and 6:2 FTS.

    “The third component explains 15% of the variability in PFASs and includes PFPeA, PFOS, and 6:2 FTS.”
    Quote in the paperSubstantial claim
  • May combine two claims.

    Interpretationown data

    Hierarchical clustering groups Site 5 separately from those sites, suggesting some differences in source contributions.

    “However, these sites are grouped separately in the hierarchical clustering analysis (Figure 2b), suggesting some differences in source contributions.”
    Quote in the paperNot a substantial claim
  • May combine two claims.

    Premisecitation

    Both landfills and wastewater treatment plants are known atmospheric sources of fluorotelomer alcohols and FOSE.

    “Both landfills and wastewater treatment plants are known atmospheric sources of fluorotelomer alcohols and FOSE.33”
    Quote in the paperSubstantial claim0 of 1 sources checked
    • cites [33] source

      Not checked in the free run.

  • Probably not a substantial claim: may not pass S3 (load-bearing). May combine two claims.

    Study design and conductown data

    Whole method recovery was 70-120% for all but four PFASs, which ranged from 60-70%, comparable to recoveries reported by previous studies.

    “Whole method recovery tested using the positive controls was 70-120% for all but 4 PFASs that ranged from 60-70%, which is comparable to recoveries reported by previous studies.3,14,15.”
    Quote in the paperNot a substantial claim0 of 3 sources checked
    • cites [3] source

      Not checked in the free run.

    • cites [14] source

      Not checked in the free run.

    • cites [15] source

      Not checked in the free run.

  • Probably not a substantial claim: may not pass S3 (load-bearing), S4 (based). May combine two claims.

    Study design and conductnone given

    Precipitation and flow rates in rivers tend to be higher in June, potentially causing enhanced dilution and a low bias for some PFASs measured in RI rivers compared to NY/NJ.

    “Precipitation and flow rates in rivers tend to be higher in June, potentially resulting in enhanced dilution and a low bias for some PFASs measured in RI rivers compared to NY/NJ.”
    Quote in the paperNot a substantial claim
  • May combine two claims.

    Premisecitation

    PFOS was historically used as a mist/fume control agent in metal plating, in surface coatings, and as the major component in AFFFs for fighting petroleum-related fires.

    “PFOS was historically used as a mist/fume control agent in metal plating, in surface coatings and as the major component in AFFFs for fighting petroleum related fire.25,26,34”
    Quote in the paperSubstantial claim0 of 3 sources checked
    • cites [25] source

      Not checked in the free run.

    • cites [26] source

      Not checked in the free run.

    • cites [34] source

      Not checked in the free run.

  • Probably not a substantial claim: may not pass S3 (load-bearing).

    Study design and conductown data

    Variability between duplicates obtained at two sites was less than 20%.

    “Variability between duplicates obtained at two sites was <20%.”
    Quote in the paperNot a substantial claim
  • Probably not a substantial claim: may not pass S3 (load-bearing). May combine two claims.

    Study design and conductnone given

    A caveat of the FRS-based source analysis is that not all listed facilities necessarily release PFASs and the database may not include all possible sources.

    “A caveat of this analysis is that not all facilities included in the FRS database necessarily release PFASs and the database may not comprehensively include all possible sources.”
    Quote in the paperNot a substantial claim
  • May combine two claims.

    Premisecitation

    Some PFOS applications such as metal plating have been replaced by less stable fluorotelomer-based chemicals such as 6:2 FtS, which eventually degrade into PFPeA and PFHxA, with yields of 1.1% and 1.5% in activated sludge.

    “Some PFOS applications such as metal plating have been replaced by less stable fluorotelomer based chemicals such as 6:2 FtS,35 which will eventually degrade into PFPeA and PFHxA (yields of 1.1% and 1.5% in activated sludge).36”
    Quote in the paperSubstantial claim0 of 2 sources checked
    • cites [35] Persistent Organic Pollutants Review Committee of UNEP. Technical paper on the identificationand assessment of alternatives to the use of perfluorooctane sulfonicacid, its salts, perfluorooctane sulfonyl fluoride and their relatedchemicals in open applications. UNEP/POPS/POPRC.8/INF/17/Rev.1; (2012.

      Not checked in the free run.

    • cites [36] source

      Not checked in the free run.

15 of 15
  • The authors state this as an assumption.

    Branched isomers for PFOA, PFHxS, PFOS, N-MeFOSAA, and N-EtFOSAA have the same instrumental response factor as their linear isomers.

    “We quantified branched isomers for perfluorooctanate (PFOA), perfluorohexane sulfonate (PFHxS), perfluorooctane sulfonate (PFOS), N-MeFOSAA and N-EtFOSAA using calibration standards for the linear isomers, assuming the same instrumental response factor (Table S3).”
  • The authors state this as an assumption.

    The impact of a potential point source on a sampling site decays exponentially with hydrological distance from the source.

    “Within each watershed, we defined an indicator for the impact of potential point sources as a function of distance from sampling locations by assuming exponential decay in the source signature19 (i.e., impact = 1/ed, where d = hydrological distance, km).”
  • The paper relies on this without support.

    Few measurements of PFASs in U.S. surface waters are available over the past five years, and the importance of different sources is poorly understood.

    “Few measurements are available for PFASs in U.S. surface waters over the past five years and the importance of different sources is poorly understood.”
  • The paper relies on this without support.

    PFASs are used for water-resistant coating in textiles, and washing and disposal of wastewater at textile mills provides a vector for their entry to the aquatic environment.

    “PFASs are used for water resistant coating in textiles and washing and disposal of wastewater at textile mills provides a vector for their entry to the aquatic environment.”
  • The paper relies on this without support.

    N-MeFOSAA and N-EtFOSAA are intermediate degradation products from FOSE, with PFOS as the final degradation product.

    “Both N-MeFOSAA and N-EtFOSAA are intermediate degradation products from the volatile parent compound N-alkyl perfluorooctane sulfamideoethanol (FOSE) with PFOS as the final degradation product.”
5 of 5

Claims other papers make about this one

Each is checked against this paper’s own text: does it say what the citing paper says it does?

  • Zhang et al. observed high PFAS concentrations in low water flow periods and low concentrations in high water periods.

    “Zhang et al. (2016) observed high PFAS concentrations in low water flow periods, while low concentrations were observed for high water periods.”

    From Per and poly-fluoroalkyl substances (PFAS) as a contaminant of emerging concern in surface water: A transboundary review of their occurrences and toxicity effects (2021) · cites this paper as Zhang et al., 2016

    Methods > Sample collection and analysis (page not provided) says higher June river flow could have diluted some PFAS concentrations, supporting the proposed direction of the relationship. It does not report observing high concentrations during low-flow periods and low concentrations during high-flow periods; the samples were collected at different sites in June and October. (LLM, conf=0.85)

    Experimental — accuracy not yet measured
  • Characterizing regional contamination patterns due to diffuse PFAS emissions and important hydrogeological features can help identify major sources and model PFAS transport.

    “Characterizing regional contamination patterns due to diffuse PFAS emissions and important hydrogeological features can help identify major sources (Silver et al., 2023; Zhang et al., 2016) and model PFAS transport (Brusseau et al., 2019).”

    From PFAS in Iowa drinking water sources: Chemical and geospatial patterns (2025) · cites this paper as Zhang et al., 2016

  • Elevated levels of PFAAs at sites N11 and N12 might be explained by historical release of AFFF.

    “The elevated levels of PFAAs in both sites might be explained by the historical release of AFFF as observed in several studies.44,45”

Self-check

Percentages, sums and reported differences re-computed from the paper’s own numbers.

Each contradiction between two passages listed here was confirmed by an independent check.

  • Abstract misidentifies the 43 ng L−1 compound as PFOS

    Minor

    The abstract assigns the 43 ng L−1 maximum to PFOS, while the results assign it to PFHxS and give 27 ng L−1 as the maximum for PFOS.

1 of 1

Cites

Flagged first, then by citations

Research works printed but not linked: 3

  1. Helsel, D. R.Nondetects and data analysis: statistics for censored environmental data;Wiley-Interscience:Hoboken, NJ, 2005; p xv, p250.
  2. U.S. Geological Survey StreamStats
  3. Persistent Organic Pollutants Review Committee of UNEP. Technical paper on the identificationand assessment of alternatives to the use of perfluorooctane sulfonicacid, its salts, perfluorooctane sulfonyl fluoride and their relatedchemicals in open applications. UNEP/POPS/POPRC.8/INF/17/Rev.1; (2012.

Cited by

Sorted by citations

Authors
Zhang, X., Lohmann, R., Dassuncao, C., Hu, X. C., Weber, A. K., Vecitis, C. D., & Sunderland, E. M.
Affiliations
  • Harvard University (US)
  • University of Rhode Island (US)
  • Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, United States
Corresponding author
Zhang, Xianming
Venue
Environmental Science & Technology Letters
Published
2016-08-09
Volume
3
Issue
9
Pages
316-321
ISSN
2328-8930 (ISSN-L)
OpenAlex
W2487559453
Cited by
167
References
31
Citations by year
2026: 9 · 2025: 21 · 2024: 20 · 2023: 25 · 2022: 25 · 2021: 24 · 2020: 17 · 2019: 8 · 2018: 9 · 2017: 8 · 2016: 1
FWCI
5.66
Type
journal article
Language
en
Open access
Locations
  • Environmental Science & Technology Letters (publishedVersion)
  • PubMed (publishedVersion)
  • PubMed Central (acceptedVersion)
  • Digital Access to Scholarship at Harvard (DASH) (Harvard University) (submittedVersion, cc-by)
  • Journal of Media Literacy Education (submittedVersion, cc-by)
Funders
  • National Institute of Environmental Health Sciences (P30 ES000002)
  • Richard and Susan Smith Family Foundation
  • Natural Sciences and Engineering Research Council of Canada (PDF-437949-2013)
  • TomKat Foundation
  • John A. Paulson School of Engineering and Applied Science, Harvard University
Topics
  • Physical Sciences › Environmental Science › Environmental Chemistry › Per- and polyfluoroalkyl substances research
  • Physical Sciences › Environmental Science › Water Science and Technology › Fluoride Effects and Removal
  • Physical Sciences › Environmental Science › Health, Toxicology and Mutagenesis › Toxic Organic Pollutants Impact
Keywords
PFASs, source attribution, surface water contamination, perfluorooctanoic acid, PFHxS, PFOS, urban pollution, point source, textile mills, airports, smelting, atmospheric deposition, waste sector emissions, watershed analysis, Rhode Island, New York metropolitan area

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