Nguan Hock-Seng, Hsu Hsu-Chen, Li Wun-Long, Liew Chia Yen, Ni Chi-Kung
Institute of Atomic and Molecular Sciences, Academia Sinica, P.O. Box 23-166, Taipei 10617, Taiwan.
Department of Chemistry, National Taiwan Normal University, Taipei 11677, Taiwan.
J Phys Chem A. 2024 Nov 28;128(47):10213-10223. doi: 10.1021/acs.jpca.4c05929. Epub 2024 Nov 18.
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.
利用质谱对碳水化合物结构进行表征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表征这些结构至关重要。在本研究中,我们使用量子化学计算和串联质谱研究了葡萄糖、半乳糖和甘露糖的线性形式以及1-6连接二糖还原端己糖的线性形式的碰撞诱导解离(CID)。我们的结果表明,由于与C═O迁移和C-C键断裂相比,线性结构中的脱水反应具有显著高的反应势垒,因此不太可能发生。我们证明,在CID光谱中观察到的交叉环碎片的不同强度可以通过C═O迁移以及C2-C3、C3-C4和C4-C5键断裂的不同过渡态能量来解释,并且葡萄糖和半乳糖之间交叉环碎片的分支比显著不同。交叉环碎片在寡糖中的应用表明,寡糖中葡萄糖和半乳糖的立体异构体可以根据C2-C3键断裂和C3-C4键断裂产生的交叉环碎片的相对强度来区分,这是传统串联质谱无法实现的区分。