Department of Chemistry, Vanderbilt Institute of Chemical Biology, Vanderbilt University, 7330 Stevenson Center, Nashville, TN 37235, USA.
Phys Chem Chem Phys. 2011 Feb 14;13(6):2196-205. doi: 10.1039/c0cp01414a. Epub 2010 Nov 29.
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 (μs 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.
本报告描述了基于离子淌度-质谱（IM-MS）提供的结构分离，对糖基位置和结构异构体进行快速特征分析。许多与糖蛋白变异相关的疾病，如果能更早地检测到，就能得到更有效的治疗，这证明了需要高通量的聚糖特征分析方法。由于糖链部分的异质性、分支和大尺寸，这使得存在大量等质量异位和结构异构体的可能性，这使得使用传统的 MS 方法难以进行特征分析。IM-MS 通过 IM 提供快速（μs 到 ms）结构分离，随后通过 MS 进行鉴定，这为糖基位置和结构异构体的特征分析提供了一种手段。为了描绘在 IM-MS 中观察到的结构变化，报告了 300 多种碳水化合物的离子-中性碰撞截面。通过使用不同的碱金属来调节通过碱金属-碳水化合物配位的分离选择性，也可以改变这种多样性。此外，还展示了在 MS 分析之前和/或之后进行 IM 前和/或后碎片化的优点，以提高碳水化合物鉴定的可信度。
