Citation:

Koelmel, J., P. Stelben, C. McDonough, D. Dukes, J. Aristizabal-Henao, S. Nason, Y. Li, S. Sternberg, E. Lin, M. Beckmann, A. Williams, J. Draper, J. Finch, J. Munk, C. Deigl, E. Rennie, J. Bowden, AND K. Godri Pollitt. FluoroMatch 2.0—making automated and comprehensive non-targeted PFAS annotation a reality. Analytical and Bioanalytical Chemistry. Springer, New York, NY, 414(3):1201-1215, (2022). https://doi.org/10.1007/s00216-021-03392-7

Impact/Purpose:

The diversity of PFAS in the environment is expected to increase as new PFAS are synthesized, used, and released into the environment and, in some cases, when existing PFAS undergo environmental and biological transformations. Therefore, to determine the potential health effects and scope of PFAS burden, it is important to empower the scientific community with tools capable of the comprehensive detection of these compounds. Non-targeted liquid chromatography-high resolution tandem mass spectrometry (LC-HRMS/MS) is one tool which can be used to detect a large portion of these chemical species in a single measurement, while also providing important information about the specific compounds present [31]. The current major bottleneck in non-targeted mass spectrometric analysis is in data-processing and interpretation. While numerous data-processing workflows have been introduced to improve the coverage and accuracy of PFAS annotations [32], use of these LC-HRMS/MS data-processing methods is tedious and prone to human error. Furthermore, it is impossible to manually survey the gigabytes of available data to comprehensively and confidently identify the PFAS covered by LC-HRMS/MS. Therefore, we introduce FluoroMatch 2.0, which is the first software to automate the non-targeted identification workflow for PFAS, aiding researchers in compound annotation.

Description:

Because of the pervasiveness, persistence, and toxicity of per- and polyfluoroalkyl substances (PFAS), there is growing concern over PFAS contamination, exposures, and health effects. The diversity of potential PFAS is astounding, with nearly 10,000 PFAS catalogued in databases to date (and growing). The ability to detect the thousands of known PFAS, and discover previously uncatalogued PFAS, is necessary to understand the scope of PFAS contamination and to identify appropriate remediation and regulatory solutions. Current non-targeted methods for PFAS analysis require manual curation and are time-consuming, prone to error, and not comprehensive. FluoroMatch Flow 2.0 is the first software to cover all steps of data processing for PFAS discovery in liquid chromatography–high-resolution tandem mass spectrometry samples. These steps include feature detection, feature blank filtering, exact mass matching to catalogued PFAS, mass defect filtering, homologous series detection, retention time pattern analysis, class-based MS/MS screening, fragment screening, and predicted MS/MS from SMILES structures. In addition, a comprehensive confidence level criterion is implemented to help users understand annotation certainty and integrate various layers of evidence to reduce overreporting. Applying the software to aqueous film forming foam analysis, we discovered over one thousand likely PFAS including previously unreported species. Furthermore, we were able to filter out 96% of features which were likely not PFAS. FluoroMatch Flow 2 increased coverage of likely PFAS by over tenfold compared to the previous release. This software will enable researchers to better characterize PFAS in the environment and in biological systems.

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