Characterization of glycosphingolipid epimers by radical-directed dissociation mass spectrometry

The Analyst
Huong T Pham, Ryan R Julian

Abstract

Glycosphingolipids (GSLs) are important metabolic regulators that control critical cellular functions and are found in all cell membranes. GSL epimers which only differ in the orientation of a single OH group are indicators for different lysosomal storage diseases. In this study, we investigate structural discrimination of GSL isomers using radical-directed dissociation (RDD). Radical fragmentation of different GSL species can be enabled by either noncovalent or covalent modification strategies. The results reveal that RDD can quantitatively distinguish lyso-GSL epimers without the requirement of prior separation by liquid chromatography. In addition, it is demonstrated that covalent labeling with boronic acid enables chemical separation of the two glycolipids isomers due to differential reactiviy of the respective sugar moiteties, offering another avenue for both molecular identification and radical characterization.

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Citations

Jan 21, 2017·International Journal of Molecular Sciences·Roza WojcikRichard D Smith
Feb 6, 2020·Rapid Communications in Mass Spectrometry : RCM·Venkateswara R NarreddulaStephen J Blanksby
Sep 23, 2020·European Journal of Mass Spectrometry·Edgar White Buenger, Gavin E Reid
Feb 24, 2021·Nature Communications·Carla KirschbaumKevin Pagel
Sep 28, 2020·Analytica Chimica Acta·Rodell C Barrientos, Qibin Zhang
Aug 24, 2017·Journal of the American Society for Mass Spectrometry·Rodell C BarrientosQibin Zhang
Jun 19, 2021·Analytical and Bioanalytical Chemistry·Sven Heiles
Dec 19, 2019·Chemical Reviews·Jennifer S BrodbeltInês Santos
Jul 13, 2019·Analytical Chemistry·Venkateswara R NarreddulaStephen J Blanksby

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