Bailey Laura S, Huang Fanran, Gao Tianqi, Zhao Jinying, Basso Kari B, Guo Zhongwu
Anal Chem. 2021 Feb 16;93(6):3154-3162. doi: 10.1021/acs.analchem.0c04542. Epub 2021 Feb 3.
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.
糖鞘脂（GSLs）在各种生物学和病理学事件中发挥着关键作用。因此，确定人体组织中完整的GSL组成对于GSL的比较和功能研究至关重要。在这项工作中，基于实验和参考MS/MS谱的两阶段匹配，开发了一种用于GSL表征和糖脂组学分析的新策略。在第一阶段，仅包含聚糖且因此在一个GSL物种内保守的碳水化合物片段直接进行匹配以进行物种鉴定。在第二阶段，来自匹配的GSL物种的糖脂片段，其同时包含脂质和聚糖且因此由于脂质结构变化而发生偏移，根据基于脂质规则的匹配进行处理以表征脂质组成。这种新策略使用全谱进行GSL表征。此外，每个GSL物种仅包含单一脂质形式的简单数据库可用于鉴定多种GSL脂质形式。预计该方法将有助于加速糖脂组学分析并揭示GSL新的和多样的脂质形式。
