Universités Aix-Marseille I, II & III-CNRS, UMR 6264: Laboratoire Chimie Provence, Spectrométries Appliquées à la Chimie Structurale, Campus Saint-Jérôme, Case 511, 13397, Marseille Cedex 20, France.
J Am Soc Mass Spectrom. 2011 Jul;22(7):1252-9. doi: 10.1007/s13361-011-0128-6. Epub 2011 Apr 9.
Isomeric distinction of di- and tri-saccharides could be efficiently achieved by using data previously obtained while performing experiments aimed at discriminating monosaccharides using trimeric ion dissociation with data analysis by the kinetic method. This study shows that effects observed for lower homologues when one of the partners is changed in the metal/reference system (typically a transition metal divalent cation associated to amino acids) can be extrapolated to upper homologues, at least for the tested analyte series. Systems allowing galactose, glucose, and fructose distinction were used as starting conditions to resolve cellobiose, lactose, maltose, and saccharose disaccharides. When a unique dissociation reaction was observed from the trimeric clusters, a new reference was selected based on its propensity to favor the analyte or the reference release, as revealed from monosaccharide experiments, depending on the desired effect. The same approach could be implemented from data obtained for disaccharides to select efficient metal/reference systems to distinguish cellotriose, isomaltotriose, maltotriose, and panose trisaccharides. As a result, method optimization is greatly improved due to an enhanced rationalization of the search for discriminant systems. While 40 systems had to be tested for monosaccharides, by screening five transition metals and eight amino acids, the proposed approach allowed efficient metal/reference systems to be found for disaccharides after testing 18 combinations; then, only four systems had to be scrutinized to achieve trisaccharide distinction. Accurate quantitative analyses could be performed in binary mixtures using three-point calibration curves to correct for competition effects between analytes for the formation of the trimeric clusters.
通过使用在使用三聚体离子解离实验区分单糖时获得的数据,并通过动力学方法进行数据分析,能够有效地实现二糖和三糖的立体异构体区分。本研究表明,当在金属/参考体系(通常是与氨基酸结合的二价过渡金属阳离子)中改变其中一个伙伴时,观察到的低同系物的效应可以外推至高同系物,至少对于测试的分析物系列是如此。使用允许区分半乳糖、葡萄糖和果糖的系统作为起始条件来解析纤维二糖、乳糖、麦芽糖和蔗糖二糖。当从三聚体簇中观察到独特的解离反应时,根据其促进分析物或参考物释放的倾向,从单糖实验中选择新的参考物,这取决于所需的效果。可以从获得的二糖数据中采用相同的方法,选择有效的金属/参考体系来区分纤维三糖、异麦芽糖三糖、麦芽三糖和海藻三糖三糖。结果,由于对判别系统的搜索进行了增强的合理化,方法优化得到了极大的改善。虽然对于单糖必须测试 40 个系统,通过筛选五种过渡金属和八种氨基酸,但所提出的方法允许在测试 18 种组合后,为二糖找到有效的金属/参考体系;然后,只需仔细研究四个系统即可实现三糖的区分。可以使用三点校准曲线在二元混合物中进行准确的定量分析,以校正分析物在形成三聚体簇时的竞争效应。