Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 56, Issue 20, Pages 14774-14787Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.2c03228
Keywords
suspect screening; advanced reduction processes (ARPs); precursors; structure-reactivity trends
Categories
Funding
- Strategic Environmental Research and Development Program (SERDP) [ER2424]
- Air Force Civil Engineering Center (AFCEC) [BAA-031]
- National Science Foundation (CHE Award) [1807739]
- NSF GRFP [DGE-1746047]
- Support for Under-Represented Groups in Engineering (SURGE) Fellowship Program (UIUC)
- Civil and Environmental Engineering Distinguished Fellowship (UIUC)
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1807739] Funding Source: National Science Foundation
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UV-sulfite has been found to effectively degrade per- and polyfluoroalkyl substances (PFASs). This study expands the analysis of a wider range of PFASs in aqueous film-forming foam (AFFF) using LC-QTOF-MS suspect screening and semiquantitative analysis. The results highlight the behavior and reactivity of the PFASs, as well as the importance of monitoring PFASs beyond conventional targeted analytical methodologies.
UV-sulfite has been shown to effectively degrade per-and polyfluoroalkyl substances (PFASs) in single-solute experiments. We recently reported treatment of 15 PFASs, including perfluoroalkyl sulfonic acids (PFSAs), perfluoroalkyl carboxylic acids (PFCAs), and fluorotelomer sulfonic acids (FTSs), detected in aqueous film-forming foam (AFFF) using high-resolution liquid chromatography quadrupole time-of-flight mass spectrometry (LC-QTOF-MS) targeted analysis. Here, we extend the analysis within those original reaction solutions to include the wider set of PFASs in AFFF for which reactivity is largely unknown by applying recently established LC-QTOF-MS suspect screening and semiquantitative analysis protocols. Sixty-eight additional PFASs were detected (15 targeted + 68 suspect screening = 83 PFASs) with semiquantitative analysis, and their behavior was binned on the basis of (1) detection in untreated AFFF, (2) PFAS photogeneration, and (3) reactivity. These 68 structures account for an additional 20% of the total fluorine content in the AFFF (targeted + suspect screening = 57% of total fluorine content). Structure-reactivity trends were also revealed. During treatment, transformations of highly reactive structures containing sulfonamide (-SO2N-) and reduced sulfur groups (e.g., -S- and -SO-) adjacent to the perfluoroalkyl [F(CF2)n-] or fluorotelomer [F(CF2)n(CH2)2-] chain are likely sources of PFCA, PFSA, and FTS generation previously reported during the early stages of reactions. The results also show the character of headgroup moieties adjacent to the F(CF2)n-/F(CF2)n(CH2)2- chain (e.g., sulfur oxidation state, sulfonamide type, and carboxylic acids) and substitution along the F(CF2)n- chain (e.g., H-, ketone, and ether) together may determine chain length-dependent reactivity trends. The results highlight the importance of monitoring PFASs outside conventional targeted analytical methodologies.
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