Structural resolution of carbohydrate positional and structural isomers based on gas-phase ion mobility-mass spectrometry

Structural resolution of carbohydrate positional and structural isomers based on gas-phase ion mobility-mass spectrometry
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DOI:
10.1039/c0cp01414a
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发表时间:
2011-01-01
影响因子:
3.3
通讯作者:
McLean, John A.
McLean, John A.
中科院分区:
化学2区
文献类型:
--
作者:
Fenn, Larissa S.;McLean, John A.

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本报告描述了基于离子迁移-质谱(IM-MS)提供的结构分离的快速表征位置和结构碳水化合物异构体。许多与糖蛋白变异相关的疾病可以通过早期检测更有效地治疗,这证实了对糖蛋白表征的高通量方法的需求。由于碳水化合物的非均质性、分支性和大尺寸的碳水化合物,这就产生了许多等压位置和结构异构体的可能性,这些异构体很难用传统的质谱方法进行表征。IM- ms提供了快速(毫秒到毫秒)的IM结构分离和随后的ms鉴定,这为表征碳水化合物的位置和结构异构体提供了一种手段。为了描绘在IM-MS中观察到的结构变化,报道了300多种碳水化合物的离子中性碰撞截面。这种多样性也可以通过使用不同的碱金属通过碱金属-碳水化合物配位调整分离选择性的效用来改变。此外,在质谱分析之前结合im前和/或im后片段的优势被证明可以提高碳水化合物鉴定的可信度。
This report describes the rapid characterization of positional and structural carbohydrate isomers based on structural separations provided by ion mobility-mass spectrometry (IM-MS). Many of the diseases associated with glycoprotein variation can be more effectively treated with earlier detection substantiating the need for high-throughput methodologies for glycan characterization. This remains particularly difficult due to heterogeneity, branching, and large size of carbohydrate moieties which creates the potential for numerous isobaric positional and structural isomers that are difficult to characterize using conventional MS methods. IM-MS provides rapid (mu s to ms) structural separations by IM and subsequent identification by MS which presents a means for characterization of positional and structural carbohydrate isomers. To chart the structural variation observed in IM-MS, the ion-neutral collision cross sections for over 300 carbohydrates are reported. This diversity can also be varied through the utility of using different alkali metals to tune separation selectivity via alkali metal-carbohydrate coordination. Furthermore, the advantages of combining either pre- and/or post-IM fragmentation prior to MS analysis is demonstrated for enhanced confidence in carbohydrate identification.