线性己糖和还原端为线性己糖的二糖的碰撞诱导解离。

IF 2.7 2区 化学 Q3 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry A Pub Date : 2024-11-18 DOI:10.1021/acs.jpca.4c05929
Hock-Seng Nguan, Hsu-Chen Hsu, Wun-Long Li, Chia Yen Liew, Chi-Kung Ni
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引用次数: 0

摘要

利用质谱法表征碳水化合物的结构是一项具有挑战性的任务。了解碳水化合物在气相中的解离机制对于通过串联质谱鉴定这些结构至关重要。在本研究中,我们利用量子化学计算和串联质谱法研究了葡萄糖、半乳糖和甘露糖线性形式的碰撞诱导解离(CID),以及 1-6 连接二糖还原端的己糖线性形式。我们的研究结果表明,与 C═O 迁移和 C-C 键裂解相比,线性结构中的脱水反应具有很高的反应障碍,因此不太可能发生。我们证明,在 CID 光谱中观察到的交叉环片段的不同强度可以用 C═O 迁移和 C2-C3、C3-C4、C4-C5 键裂解的不同过渡态能量来解释,而且葡萄糖和半乳糖的交叉环片段的支化比也明显不同。交叉环片段在低聚糖中的应用表明,可以根据 C2-C3 键裂解和 C3-C4 键裂解产生的交叉环片段的相对强度来区分低聚糖中葡萄糖和半乳糖的立体异构体,这是传统串联质谱无法实现的。
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Collision-Induced Dissociations of Linear Hexose and Disaccharides with Linear Hexose at the Reducing End.

Characterization of carbohydrate structures using mass spectrometry is a challenging task. Understanding the dissociation mechanisms of carbohydrates in the gas phase is crucial for characterizing these structures through tandem mass spectrometry. In this study, we investigated the collision-induced dissociation (CID) of glucose, galactose, and mannose in their linear forms, as well as the linear forms of hexose at the reducing end of 1-6 linked disaccharides, using quantum chemistry calculations and tandem mass spectrometry. Our results suggest that the dehydration reaction in linear structures is unlikely to occur due to the significantly high reaction barrier compared to those of C═O migration and C-C bond cleavage. We demonstrate that the different intensities of the cross-ring fragments observed in the CID spectra can be explained by the different transition state energies of C═O migration and C2-C3, C3-C4, and C4-C5 bond cleavages, and the branching ratios of the cross-ring fragments are significantly different between glucose and galactose. The application of the cross-ring fragments to oligosaccharides reveals that the stereoisomers of glucose and galactose in oligosaccharides can be differentiated based on the relative intensities of the cross-ring fragments produced by the C2-C3 bond cleavage and C3-C4 bond cleavage, a differentiation that cannot be achieved by conventional tandem mass spectrometry.

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来源期刊
The Journal of Physical Chemistry A
The Journal of Physical Chemistry A 化学-物理:原子、分子和化学物理
CiteScore
5.20
自引率
10.30%
发文量
922
审稿时长
1.3 months
期刊介绍: The Journal of Physical Chemistry A is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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