Per- and polyfluoroalkyl substances (PFAS) are a class of manmade organofluorine chemicals used in a variety of household and industrial applications. Exposure to PFAS has been associated with adverse health outcomes including liver damage, cancer, and elevated cholesterol, though the specific molecular mechanisms perturbed by PFAS exposure are poorly understood. Previous studies have also linked PFAS exposure with lipid dysregulation, though more comprehensive lipidomic studies that go beyond simple triglyceride and cholesterol levels are greatly needed to investigate these alterations. However, performing multiple extractions and lengthy analytical measurements to separately measure PFAS and lipids can be quite time-consuming. In this work, we leveraged a non-targeted platform coupling liquid chromatography, ion mobility spectrometry, collision induced dissociation and mass spectrometry (LC-IMS-CID-MS) separations for the simultaneous evaluations of PFAS and lipids in serum and liver from mice exposed to various PFAS. While we have previously evaluated the ability of LC-IMS-CID-MS to distinguish distinct molecular classes by their unique IMS collision cross section (CCS) and m/z values with thousands of standards, this approach has not yet been applied to different molecule types in a single analysis. Furthermore, since PFAS exposure and lipid dysregulation are important for understanding health outcomes, they are optimal for this method as they can be co-extracted, occupy similar mass ranges, and have largely different CCS values. To perform the analyses, a single, rapid extraction was followed by a LC-IMS-CID-MS analysis having a total data collection time of 50 minutes compared to 110 minutes when using separate methods for each molecule type. Importantly, the number of identifications for both PFAS and lipids were observed to be highly comparable between the new approach and traditional methods for each molecule separately. Analysis of the mouse liver was then performed and illustrated how some lipidomic changes were conserved for the multiple PFAS studied, while others were dependent on the specific PFAS applied.

Simultaneous evaluation of exposure to per- and polyfluoroalkyl substances (PFAS) and the resulting lipid dysregulation

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ACS Fall 2022

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