Abstract
Lipid dysregulation has been implicated in multiple sclerosis due to its involvement during and after inflammation. In this study, we have profiled fatty acids (FAs) in the mouse model of multiple sclerosis with new capabilities of assigning carbon-carbon double bond (C=C) location(s) and quantifying C=C location isomers. These new capabilities are enabled by pairing the solution phase Paternò-Büchi (PB) reaction that modifies C=C bonds in FAs, with tandem mass spectrometry (MS/MS), termed as PB-MS/MS. A series of unsaturated FAs and C=C location isomers have been identified, including FA17:1 (Δ10), FA18:1 (Δ9 and Δ11), FA18:2 (Δ9 and Δ12), and FA 20:4 (Δ5, Δ8, Δ11, Δ14). Notable differences in saturated and unsaturated FAs between normal and experimental autoimmune encephalomyelitis (EAE) mice spinal cords have been detected. Furthermore, the effects of hydralazine, a scavenger of acrolein, on profile changes of FAs in mice were studied. Increased Δ11-to-Δ9 isomer ratios for FA 18:1 were noted in the diseased samples as compared to the control. The present work provides a facile and robust analytical method for the quantitation of unsaturated FAs as well as identification of FA C=C location isomers, which will facilitate discovering prospective lipid markers in multiple sclerosis.
Highlights
Lipids are one of the most essential biomolecules that living organisms cannot survive without
The carbonyl group reacts with C=C in the unsaturated lipids to form an oxetane structure that subsequently gets ruptured by low-energy collision-induced dissociation (CID)
A rising amount of evidence has indicated a link between the disease and lipids, suggesting that lipids may be a suitable diagnostic or therapeutic target in multiple sclerosis
Summary
Lipids are one of the most essential biomolecules that living organisms cannot survive without. The lack of a fast and robust method for determining the identity of unsaturated lipids, especially with accurate information of carbon-carbon double bonds (C=C) locations, hinders the studies of the evolving area of structural. Our groups and others have demonstrated that by coupling C=C selective derivatization via the photochemical PaternòBüchi (PB) reaction with subsequent tandem mass spectrometry (MS/MS) analysis, the locations of C=C bonds in unsaturated fatty acyls can be confidently determined in a sensitive and high-throughput fashion (Ma and Xia, 2014; Ma et al, 2016a,b; Murphy et al, 2017; Ren et al, 2017; Franklin et al, 2019; Zhang et al, 2019). Due to the unique capabilities of this method, one can choose to perform direct analysis of the lipid mixtures extracted from biological samples; especially if the individual is looking for a rapid disease diagnosis (Ma et al, 2016a; Zou et al, 2019)
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