Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 54, Issue 9, Pages 5676-5686Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.0c00049
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Funding
- National Sciences and Engineering Research Council (NSERC) Discovery Grant
- Environment and Climate Change Canada [GCE19P17]
- Canada Foundation for Innovation
- Ontario Research Fund
- NSERC Research Tools and Instrument Grant
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More than 1000 per- and polyfluoroalkyl substances (PFASs) have been discovered by nontarget analysis (NTA), but their prioritization for health concerns is challenging. We developed a method by incorporating size-exclusion column coelution (SECC) and NTA, to screen PFASs binding to human liver fatty acid binding protein (hL-FABP). Of 74 PFASs assessed, 20 were identified as hL-FABP ligands in which eight of them have high binding affinities. Increased PFAS binding affinities correlate with stronger responses in electrospray ionization (ESI-) and longer retention times on a C18 column. This is well explained by a mechanistic model, which revealed that both polar and hydrophobic interactions are crucial for binding affinities. Encouraged by this, we then developed an SECC method to identify hL-FABP ligands, and all eight high-affinity ligands were selectively captured from 74 PFASs. The method was further applied to an aqueous film-forming foam (AFFF) product in which 31 new hL-FABP ligands were identified. Suspect and nontargeted screening revealed these ligands as analogues of perfluorosulfonic acids and homologues of alkyl ether sulfates (C-8- and C-10/EOn, C8H17 (C2H4O)nSO(4)(-), and C10H21(C2H4O)(n)SO4). The SECC method was then applied to AFFF-contaminated surface waters. In addition to perfluorooctanesulfonic acid and perfluorohexanesulfonic acid, eight other AFFF chemicals were discovered as novel ligands, including four C-14- and C-15/EOn. This study implemented a high-throughput method to prioritize PFASs and revealed the existence of many previously unknown hL-FABP ligands.
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