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PFAS Analysis with Ultrahigh Resolution 21T FT-ICR MS: Suspect and Nontargeted Screening with Unrivaled Mass Resolving Power and Accuracy

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Download Hi-Res ImageDownload to MS-PowerPointCite This:Environ. Sci. Technol. 2022, 56, 4, 2455-2465
    Contaminants in Aquatic and Terrestrial Environments

    PFAS Analysis with Ultrahigh Resolution 21T FT-ICR MS: Suspect and Nontargeted Screening with Unrivaled Mass Resolving Power and Accuracy
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    • Robert B. Young
      Robert B. Young
      Chemical Analysis & Instrumentation Laboratory, New Mexico State University, Las Cruces, New Mexico 88003, United States
      More by Robert B. Young
      Orcidhttps://orcid.org/0000-0001-7485-0604
    • Nasim E. Pica
      Nasim E. Pica
      Department of Civil and Environmental Engineering, Colorado State University, Fort Collins, Colorado 80523, United States
      Weston Solutions, Lakewood, Colorado 80401, United States
      More by Nasim E. Pica
      Orcidhttps://orcid.org/0000-0002-3745-8723
    • Hamidreza Sharifan
      Hamidreza Sharifan
      Department of Civil and Environmental Engineering, Colorado State University, Fort Collins, Colorado 80523, United States
      Department of Natural Science, Albany State University, Albany, Georgia 31705, United States
      More by Hamidreza Sharifan
      Orcidhttps://orcid.org/0000-0002-6990-0635
    • Huan Chen
      Huan Chen
      National High Magnetic Field Laboratory, Florida State University, Tallahassee, Florida 32310, United States
      More by Huan Chen
      Orcidhttps://orcid.org/0000-0002-6032-6569
    • Holly K. Roth
      Holly K. Roth
      Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523, United States
      More by Holly K. Roth
      Orcidhttps://orcid.org/0000-0003-2733-517X
    • Greg T. Blakney
      Greg T. Blakney
      National High Magnetic Field Laboratory, Florida State University, Tallahassee, Florida 32310, United States
      More by Greg T. Blakney
      Orcidhttps://orcid.org/0000-0002-4205-9866
    • Thomas Borch
      Thomas Borch
      Department of Civil and Environmental Engineering, Colorado State University, Fort Collins, Colorado 80523, United States
      Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523, United States
      Department of Soil & Crop Sciences, Colorado State University, Fort Collins, Colorado 80523, United States
      More by Thomas Borch
      Orcidhttps://orcid.org/0000-0002-4251-1613
    • Christopher P. Higgins
      Christopher P. Higgins
      Department of Civil and Environmental Engineering, Colorado School of Mines, Golden, Colorado 80401, United States
      More by Christopher P. Higgins
      Orcidhttps://orcid.org/0000-0001-6220-8673
    • John J. Kornuc
      John J. Kornuc
      NAVFAC EXWC, 1100 23rd Avenue, Port Hueneme, California 93041, United States
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    • Amy M. McKenna
      Amy M. McKenna
      National High Magnetic Field Laboratory, Florida State University, Tallahassee, Florida 32310, United States
      Department of Soil & Crop Sciences, Colorado State University, Fort Collins, Colorado 80523, United States
      More by Amy M. McKenna
      Orcidhttps://orcid.org/0000-0001-7213-521X
    • Jens Blotevogel*
      Jens Blotevogel
      Department of Civil and Environmental Engineering, Colorado State University, Fort Collins, Colorado 80523, United States
      *E-mail: [email protected]. Phone: +1-970-491-8880. Fax: +1-970-491-8224.
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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2022, 56, 4, 2455–2465
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    https://doi.org/10.1021/acs.est.1c08143
    Published January 31, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    Per- and polyfluoroalkyl substances (PFASs) are a large family of thousands of chemicals, many of which have been identified using nontargeted time-of-flight and Orbitrap mass spectrometry methods. Comprehensive characterization of complex PFAS mixtures is critical to assess their environmental transport, transformation, exposure, and uptake. Because 21 tesla (T) Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS) offers the highest available mass resolving power and sub-ppm mass errors across a wide molecular weight range, we developed a nontargeted 21 T FT-ICR MS method to screen for PFASs in an aqueous film-forming foam (AFFF) using suspect screening, a targeted formula database (C, H, Cl, F, N, O, P, S; ≤865 Da), isotopologues, and Kendrick-analogous mass difference networks (KAMDNs). False-positive PFAS identifications in a natural organic matter (NOM) sample, which served as the negative control, suggested that a minimum length of 3 should be imposed when annotating CF2-homologous series with positive mass defects. We putatively identified 163 known PFASs during suspect screening, as well as 134 novel PFASs during nontargeted screening, including a suspected polyethoxylated perfluoroalkane sulfonamide series. This study shows that 21 T FT-ICR MS analysis can provide unique insights into complex PFAS composition and expand our understanding of PFAS chemistries in impacted matrices.

    Copyright © 2022 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.1c08143.

    • PFAS database analysis; ESI– FT-ICR MS spectra and analyses; Kendrick-analogous mass difference network analyses; and statistical peak and KMD series analyses (PDF)

    • Complete lists of all putatively identified PFASs (XLSX)

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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2022, 56, 4, 2455–2465
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.est.1c08143
    Published January 31, 2022
    Copyright © 2022 American Chemical Society
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