Linkage and sequence analysis of neutral oligosaccharides by negative-ion MALDI tandem mass spectrometry with laser-induced dissociation

Linkage and sequence analysis of neutral oligosaccharides by negative-ion MALDI tandem mass spectrometry with laser-induced dissociation
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激光诱导解离负离子 MALDI 串联质谱法对中性寡糖的连接和序列分析

DOI:
10.1016/j.aca.2019.04.067
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发表时间:
2019-09-13
影响因子:
6.2
通讯作者:
Chai,Wengang
Chai,Wengang
中科院分区:
化学1区
文献类型:
--
作者:
Huang,Chuncui;Yan,Jingyu;Chai,Wengang

文献摘要

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质谱(MS)已成为低聚糖高灵敏度结构测定的主要方法。负离子 MS 中的碎片可以提供丰富的结构信息,这些信息可用于序列测定。然而,尽管使用去质子化分子 [M−H]− 作为前体的中性寡糖负离子 MS 在电喷雾电离 (ESI) 方面非常成功,但在基质辅助激光解吸/电离 (MALDI) 方面却只取得了有限的成功。在本研究中,详细研究了负离子 MALDI 初级光谱的特征,并仔细比较了使用 [M−H]– 和 [M+Cl]– 作为前驱体的产物离子光谱。 [M−H]– 的形成是 MALDI 的主要困难,而 [M+Cl]– 被证明可用作 MALDI-MS/MS 的替代前体阴离子,以产生用于中性寡糖测序的类似碎片。然后使用 N-(1-萘基)乙二胺二盐酸盐作为基质和 Cl− 掺杂剂,以评估通过激光诱导从 [M+Cl] 中的负离子碎片获得的结构信息的程度。解离 (LID)-MS/MS,用于寡糖的连接分配以及 1 型或 2 型主链上 ABO(H) 血型和 Lewis 抗原的分型。
Mass spectrometry (MS) has become the primary method for high-sensitivity structural determination of oligosaccharides. Fragmentation in the negative-ion MS can provide a wealth of structural information and these can be used for sequence determination. However, although negative-ion MS of neutral oligosaccharide using the deprotonated molecule [M−H]−as the precursor has been very successful for electrospray ionization (ESI), it has only limited success for matrix-assisted laser desorption/ionization (MALDI). In the present study, the features of negative-ion MALDI primary spectra were investigated in detail and the product-ion spectra using [M−H]–and [M+Cl]–as the precursors were carefully compared. The formation of [M−H]–was the main difficulty for MALDI while [M+Cl]–was proved to be useful as alternative precursor anion for MALDI-MS/MS to produce similar fragmentation for sequencing of neutral oligosaccharides.N-(1-naphthyl)ethylenediamine dihydrochloride was then used as both the matrix and the Cl−dopant to evaluate the extent of structural information that can be obtained by negative-ion fragmentation from [M+Cl]–using laser-induced dissociation (LID)-MS/MS for linkage assignment of gluco-oligosaccharides and for typing of blood-group ABO(H) and Lewis antigens on either type 1 or type 2 backbone-chains.