FluoroMatch 2.0-making automated and comprehensive non-targeted PFAS annotation a reality

Area of Science:

• Environmental Chemistry
• Analytical Chemistry
• Toxicology

Background:

• Per- and polyfluoroalkyl substances (PFAS) are pervasive, persistent, and toxic, raising significant concerns about environmental contamination, human exposure, and health effects.
• The vast number of known PFAS (nearly 10,000) and the continuous discovery of new ones necessitate advanced analytical methods for comprehensive detection and characterization.
• Existing non-targeted PFAS analysis methods are often manual, time-consuming, error-prone, and lack completeness, hindering effective scope assessment and remediation efforts.

Purpose of the Study:

• To introduce FluoroMatch Flow 2.0, the first software designed for end-to-end data processing for PFAS discovery using liquid chromatography-high-resolution tandem mass spectrometry (LC-HR-MS/MS).
• To enable comprehensive detection and characterization of both known and previously uncatalogued PFAS in complex environmental and biological samples.
• To improve the accuracy and efficiency of PFAS analysis, reducing manual curation and overreporting of false positives.

Main Methods:

• Development and implementation of FluoroMatch Flow 2.0 software, integrating multiple data processing steps: feature detection, blank filtering, exact mass matching, mass defect filtering, homologous series detection, retention time analysis, class-based MS/MS screening, fragment screening, and predicted MS/MS.
• Inclusion of a confidence level criterion to assess annotation certainty by integrating diverse evidence layers.
• Application of the software to analyze aqueous film-forming foam (AFFF) samples.

Main Results:

• Discovery of over one thousand likely PFAS in AFFF samples, including previously unreported species.
• Effective filtering of 96% of features identified as likely not PFAS, significantly reducing false positives.
• A tenfold increase in the coverage of likely PFAS compared to the previous software release (FluoroMatch Flow).

Conclusions:

• FluoroMatch Flow 2.0 represents a significant advancement in PFAS analytical capabilities, offering a comprehensive and efficient solution for PFAS discovery.
• The software empowers researchers to better characterize PFAS contamination in environmental and biological systems, facilitating informed regulatory and remediation strategies.
• Enhanced PFAS identification and characterization are crucial for addressing the global challenge posed by these persistent chemicals.