Comprehensive Emerging Chemical Discovery: Novel Polyfluorinated Compounds in Lake Michigan Trout
Abstract
A versatile screening algorithm capable of efficiently searching liquid chromatographic/mass spectrometric data for unknown compounds has been developed using a combination of open source and generic computing software packages. The script was used to search for select novel polyfluorinated contaminants in Great Lakes fish. However, the framework is applicable whenever full-scan, high-resolution mass spectral and chromatographic data are collected. Target compound classes are defined and a matrix of candidates is generated that includes mass spectral profiles and likely fragmentation pathways. The initial calibration was performed using a standard solution of known linear perfluoroalkyl acids. Once validated, Lake Michigan trout data files were analyzed for polyfluoroalkyl acids using the algorithm referencing 3570 possible compounds including C4-C10 perfluoro- and polyfluoroalkyl, polyfluorochloroalkyl acids and sulfonates, and potential ether forms. The results suggest the presence of 30 polyfluorinated chemical formulas which have not been previously reported in the literature. The identified candidates included mono- to hexafluoroalkyl carboxylic acids, mono- and trifluoroalkyl carboxylic acid ethers, and novel polyfluoroalkyl sulfonates. Candidate species identified in lake trout were qualified using theoretical isotopic profile matching, characteristic fragmentation patterns based on known linear perfluoroalkyl acid (PFAA) fragmentation, and retention time reproducibility among replicate extractions and injections. In addition, the relative retention times of multiple species within a compound class were compared based on theoretical octanol-water partition coefficients.
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Frequent and extensive detection of emerging or unknown PFASs in the environment highlights the risk to humans from continuous exposure to increasing amounts of such compounds.
“Frequent and extensive detection of emerging/unknown PFASs within the environment highlights the risk to humans of continuous exposure to increasing amounts of such compounds.”
From Non-Target and Suspect Screening of Per- and Polyfluoroalkyl Substances in Airborne Particulate Matter in China (2018) · cites this paper as [12]
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- Authors
- Fakouri Baygi, S., Crimmins, B. S., Hopke, P. K., & Holsen, T. M.
- Affiliations
- AEACS, LLC, Alliance, Ohio 44601, United States
- Clarkson University (US)
- Corresponding author
- Crimmins, Bernard S.
- Venue
- Environmental Science & Technology
- Publisher
- American Chemical Society (ACS)
- Published
- 2016-08-19
- Volume
- 50
- Issue
- 17
- Pages
- 9460-9468
- ISSN
- 0013-936X (ISSN-L)
- 1520-5851
- OpenAlex
- W2476960589
- Cited by
- 49
- References
- 30
- Citations by year
- 2026: 4 · 2025: 4 · 2024: 1 · 2023: 4 · 2022: 5 · 2021: 4 · 2020: 6 · 2019: 8 · 2018: 6 · 2017: 7
- FWCI
- 4.58
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Environmental Science & Technology (publishedVersion)
- PubMed (publishedVersion)
- Funders
- U.S. Environmental Protection Agency (GL-96594201-1)
- 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
- polyfluorinated compounds, Great Lakes fish, emerging contaminants, LC-MS data analysis, fragmentation pathways, octanol-water partition coefficient, perfluoroalkyl acids
- MeSH terms
- Animals, Michigan, Trout, Water Pollutants, Chemical, Reproducibility of Results, Lakes
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