Identification of novel non-ionic, cationic, zwitterionic, and anionic polyfluoroalkyl substances using UPLC–TOF–MSE high-resolution parent ion search
Abstract
Poly- and perfluoroalkyl substances (poly- and per-PFASs) are a large group of organic compounds that have become the target of investigation due to their widespread occurrence in the environment and biota, coupled with their known or suspected impacts on human health. Recent studies have shown that a significant portion of poly-PFASs remain unidentified. This study presents a time-of-flight mass spectrometry approach based on continuously interleaving scans at low and high collision energies (ToF-MS E) for the rapid identification and characterization of unknown PFASs. The MS E mode allowed for the simultaneous acquisition of full-spectrum accurate mass data of both parent and fragment ions in a single chromatographic run. Specific to PFASs, the hypothesis that PFASs can be selectively detected by the ToF-MS E high-resolution parent-ion search (HRPIS) of their characteristic fragments was confirmed with certified standards of 24 poly- and per-PFAS. After being validated with these certified standards, the innovative HRPIS approach was applied to a group of commercial surfactants, which led to the identification of 47 new and 43 infrequently reported PFASs, including 40 non-ionic, 30 cationic, 15 zwitterionic, and five anionic compounds. It is envisaged that the results, especially the identification of new non-ionic PFASs, may provide important insights into the historical occupational and non-occupational exposure to PFASs from the production and application of these surfactants.
Integrity signals
Registry
Cites
Statistics
Claims the paper makes
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?
Recent research has indicated the presence in the environment of numerous other PFAS comprising different molecular structures.
“Recent research has indicated the presence in the environment of numerous other PFAS comprising different molecular structures (e.g., Baduel et al., 2017; Xiao, 2017; Xiao et al., 2017).”
From PFAS concentrations in soils: Background levels versus contaminated sites (2020) · cites this paper as Xiao et al., 2017
Among recent contaminant discoveries, some are PFAA-precursors that could contribute to environmental PFAA exposure for years to come.
“Among such recent contaminant discoveries, some are PFAA-precursors (e.g.perfluorooctaneamido quaternary ammonium salt [32]) that could contribute to environmental PFAA exposure for years to come [45], some are legacy substances likely present in the environment for more than 40 years already (e.g.chlorinated perfluoroether sulfonates [42]), while others are likely new current-use alternatives (e.”
High-resolution parent ion searches using TOF-MS with continuously interleaving scans at low and high collision energies led to identification of 47 new and 43 infrequently reported PFAS, including 40 non-ionic, 30 cationic, 15 zwitterionic and 5 anionic compounds.
“which led to the identification of 47 new and 43 infrequently reported PFAS, including 40 non-ionic, 30 cationic, 15 zwitterionic and 5 anionic compounds.”
From Worldwide trends in tracing poly- and perfluoroalkyl substances (PFAS) in the environment (2019) · cites this paper as [94]
Diverse novel PFAS including anions, zwitterions, cations and neutral species were identified in AFFF samples, Fluorad surfactants, water, airborne particulate matter, fish and circulating blood.
“diverse novel PFAS including anions, zwitterions, cations and neutral species were identified in AFFF samples [92,93], Fluorad surfactants [94], water [17], airborne particulate matter [16], fish [18] and circulating blood [19].”
From Worldwide trends in tracing poly- and perfluoroalkyl substances (PFAS) in the environment (2019) · cites this paper as [94]
Cites
Global Distribution of Perfluorooctane Sulfonate in Wildlife
Giesy, J. P., & Kannan, K. (2001) · Environmental Science & Technology · doi:10.1021/es001834k · Cited by 2,750 · see citing works
Wang, Z., Cousins, I. T., Scheringer, M., & Hungerbühler, K. (2013) · Environment International · doi:10.1016/j.envint.2013.08.021 · Cited by 924 · see citing works
Persistence of Perfluoroalkyl Acid Precursors in AFFF-Impacted Groundwater and Soil
Houtz, E. F., Higgins, C. P., Field, J. A., & Sedlak, D. L. (2013) · Environmental Science & Technology · doi:10.1021/es4018877 · Cited by 849 · see citing works
McGuire, M. E., Schaefer, C., Richards, T., Backe, W. J., Field, J. A., Houtz, E., Sedlak, D. L., Guelfo, J. L., Wunsch, A., & Higgins, C. P. (2014) · Environmental Science & Technology · doi:10.1021/es5006187 · Cited by 269 · see citing works
Observation of emerging per- and polyfluoroalkyl substances (PFASs) in Greenland marine mammals
Gebbink, W. A., Bossi, R., Rigét, F. F., Rosing-Asvid, A., Sonne, C., & Dietz, R. (2016) · Chemosphere · doi:10.1016/j.chemosphere.2015.10.116 · Cited by 266 · see citing works
Production of PFOS from aerobic soil biotransformation of two perfluoroalkyl sulfonamide derivatives
Mejia Avendaño, S., & Liu, J. (2015) · Chemosphere · doi:10.1016/j.chemosphere.2014.09.059 · Cited by 225 · see citing works
Benskin, J. P., Ikonomou, M. G., Gobas, F. A. P. C., Begley, T. H., Woudneh, M. B., & Cosgrove, J. R. (2013) · Environmental Science & Technology · doi:10.1021/es304336r · Cited by 169 · see citing works
Mejia-Avendaño, S., Vo Duy, S., Sauvé, S., & Liu, J. (2016) · Environmental Science & Technology · doi:10.1021/acs.est.6b00140 · Cited by 168 · see citing works
Larsen, B. S., Stchur, P., Szostek, B., Bachmura, S. F., Rowand, R. C., Prickett, K. B., Korzeniowski, S. H., & Buck, R. C. (2006) · Journal of Chromatography A · doi:10.1016/j.chroma.2006.01.086 · Cited by 65 · see citing works
Flagged first, then by citations
Cited by
Sorted by citations
An overview of the uses of per- and polyfluoroalkyl substances (PFAS)
Glüge, J., Scheringer, M., Cousins, I. T., DeWitt, J. C., Goldenman, G., Herzke, D., Lohmann, R., Ng, C. A., Trier, X., & Wang, Z. (2020) · Environmental Science: Processes & Impacts · doi:10.1039/d0em00291g · Cited by 2,466 · see citing works
PFAS concentrations in soils: Background levels versus contaminated sites
Brusseau, M. L., Anderson, R. H., & Guo, B. (2020) · Science of The Total Environment · doi:10.1016/j.scitotenv.2020.140017 · Cited by 817 · see citing works
Worldwide trends in tracing poly- and perfluoroalkyl substances (PFAS) in the environment
Nakayama, S. F., Yoshikane, M., Onoda, Y., Nishihama, Y., Iwai-Shimada, M., Takagi, M., Kobayashi, Y., & Isobe, T. (2019) · TrAC Trends in Analytical Chemistry · doi:10.1016/j.trac.2019.02.011 · Cited by 399 · see citing works
Brase, R. A., Mullin, E. J., & Spink, D. C. (2021) · International Journal of Molecular Sciences · doi:10.3390/ijms22030995 · Cited by 374 · see citing works
Liu, Y., D'Agostino, L. A., Qu, G., Jiang, G., & Martin, J. W. (2019) · TrAC Trends in Analytical Chemistry · doi:10.1016/j.trac.2019.02.021 · Cited by 344 · see citing works
Meegoda, J. N., Kewalramani, J. A., Li, B., & Marsh, R. W. (2020) · International Journal of Environmental Research and Public Health · doi:10.3390/ijerph17218117 · Cited by 256 · see citing works
Yu, N., Guo, H., Yang, J., Jin, L., Wang, X., Shi, W., Zhang, X., Yu, H., & Wei, S. (2018) · Environmental Science & Technology · doi:10.1021/acs.est.8b02492 · Cited by 200 · see citing works
Xiao, F., Jin, B., Golovko, S. A., Golovko, M. Y., & Xing, B. (2019) · Environmental Science & Technology · doi:10.1021/acs.est.9b05379 · Cited by 197 · see citing works
Self-citationMcCord, J., & Strynar, M. (2019) · Environmental Science & Technology · doi:10.1021/acs.est.8b06017 · Cited by 183 · see citing works
Analysis of emerging per- and polyfluoroalkyl substances: Progress and current issues
Pan, Y., Wang, J., Yeung, L. W. Y., Wei, S., & Dai, J. (2020) · TrAC Trends in Analytical Chemistry · doi:10.1016/j.trac.2019.04.013 · Cited by 133 · see citing works
Mullin, L., Katz, D. R., Riddell, N., Plumb, R., Burgess, J. A., Yeung, L. W. Y., & Jogsten, I. E. (2019) · TrAC Trends in Analytical Chemistry · doi:10.1016/j.trac.2019.05.015 · Cited by 91 · see citing works
Microbial biotransformation of aqueous film-forming foam derived polyfluoroalkyl substances
Choi, Y. J., Helbling, D. E., Liu, J., Olivares, C. I., & Higgins, C. P. (2022) · Science of The Total Environment · doi:10.1016/j.scitotenv.2022.153711 · Cited by 79 · see citing works
Kotthoff, M., & Bücking, M. (2018) · Frontiers in Chemistry · doi:10.3389/fchem.2018.00103 · Cited by 73 · see citing works
- Authors
- Xiao, F., Golovko, S. A., & Golovko, M. Y.
- Affiliations
- University of North Dakota (US)
- Corresponding author
- Xiao, Feng
- Venue
- Analytica Chimica Acta
- Publisher
- Elsevier BV
- Published
- 2017-10
- Volume
- 988
- Pages
- 41-49
- ISSN
- 0003-2670 (ISSN-L)
- OpenAlex
- W2749140638
- Cited by
- 97
- References
- 9
- Citations by year
- 2026: 6 · 2025: 10 · 2024: 5 · 2023: 18 · 2022: 11 · 2021: 6 · 2020: 21 · 2019: 13 · 2018: 7
- FWCI
- 6.59
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Analytica Chimica Acta (publishedVersion)
- PubMed (publishedVersion)
- Funders
- University of North Dakota Vice President of Research & Economic Development Faculty Early Career Award (20622-4000-02545)
- NIH funded COBRE Mass Spec Core Facility (5P30GM103329-05)
- Topics
- Physical Sciences › Environmental Science › Environmental Chemistry › Per- and polyfluoroalkyl substances research
- Physical Sciences › Chemistry › Spectroscopy › Mass Spectrometry Techniques and Applications
- Life Sciences › Pharmacology, Toxicology and Pharmaceutics › Pharmaceutical Science › Fluorine in Organic Chemistry
- Keywords
- polyfluoroalkyl substances, perfluorinated compounds, time-of-flight mass spectrometry, commercial surfactants, PFAS exposure, environmental pollutants
About these checks
Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.
Statistics and arithmetic are recomputed, not judged.
Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.
What counts as a claim ›How we measure confidence ›How we check this ›
Are you an author, or do you see a problem with this page? Request a review
