Characterization of Glycosphingolipids and Their Diverse Lipid Forms through Two-Stage Matching of LC-MS/MS Spectra

Glycosphingolipids (GSLs) play a key role in various biological and pathological events. Thus, determination of the complete GSL compositions in human tissues is essential for comparative and functional studies of GSLs. In this work, a new strategy was developed for GSL characterization and glycolip...

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Bibliographic Details
Published in:Analytical chemistry (Washington) 2021-02, Vol.93 (6), p.3154-3162
Main Authors: Bailey, Laura S, Huang, Fanran, Gao, Tianqi, Zhao, Jinying, Basso, Kari B, Guo, Zhongwu
Format: Article
Language:English
Subjects:
Analytical chemistry
Carbohydrates
Chemistry
Chromatography, Liquid
Composition
Fragments
Glycosphingolipids
Human tissues
Humans
Lipids
Matching
Polysaccharides
Species
Tandem Mass Spectrometry
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Summary:Glycosphingolipids (GSLs) play a key role in various biological and pathological events. Thus, determination of the complete GSL compositions in human tissues is essential for comparative and functional studies of GSLs. In this work, a new strategy was developed for GSL characterization and glycolipidomics analysis based on two-stage matching of experimental and reference MS/MS spectra. In the first stage, carbohydrate fragments, which contain only glycans and thus are conserved within a GSL species, are directly matched to yield a species identification. In the second stage, glycolipid fragments from the matched GSL species, which contain both the lipid and glycans and thus shift due to lipid structural changes, are treated according to lipid rule-based matching to characterize the lipid compositions. This new strategy uses the whole spectrum for GSL characterization. Furthermore, simple databases containing only a single lipid form per GSL species can be utilized to identify multiple GSL lipid forms. It is expected that this method will help accelerate glycolipidomics analysis and disclose new and diverse lipid forms of GSLs.
ISSN:0003-2700
1520-6882
DOI:10.1021/acs.analchem.0c04542