Zanetta J P, Timmerman P, Leroy Y
Laboratoire de Chimie Biologique, CNRS UMR 111, 59655 Villeneuve d'Ascq Cedex, France.
Glycobiology. 1999 Mar;9(3):255-66. doi: 10.1093/glycob/9.3.255.
We have developed a method involving the formation of hepta-fluorobutyrate derivatives of O-methyl-glycosides liberated from glycoproteins and glycolipids following methanolysis. The stable derivatives of the most common monosaccharides of these glycoconjugates (Ara, Rha, Xyl, Fuc, Gal, Man, Glc, GlcNAc, GalNAc, Neu5Ac, KDN) can be separated and quantitatively and reproducibly determined with a high degree of sensitivity level (down to 25 pmol) in the presence of lysine as an internal standard. The GlcNAc residue bound to Asn in N-glycans is quantitatively recovered as two peaks. The latter were easily distinguished from the other GlcNAc residues of N-glycans, thus allowing a considerable improvement of the data on structure of N-glycans obtained from a single carbohydrate analysis. The most common contaminants present in buffers commonly used for the isolation of soluble or membrane-bound glycoproteins (SDS, Triton X-100, DOC, TRIS, glycine, and polyacrylamide or salts, as well as monosaccharide constituents of proteoglycans or degradation products of nucleic acids) do not interfere with these determinations. A carbohydrate analysis of glycoproteins isolated from a SDS/PAGE gel or from PDVF membranes can be performed on microgram amounts without significant interferences. Since fatty acid methyl esters and sphingosine derivatives are separated from the monosaccharide peaks, the complete composition of gangliosides can be achieved in a single step starting from less than 1 microg of the initial compound purified by preparative Silicagel TLC. Using electron impact ionization mass spectrometry, reporter ions for the different classes of O-methyl-glycosides (pentoses, deoxy-hexoses, hexoses, hexosamines, uronic acids, sialic acid, and KDN) allow the identification of these compounds in very complex mixtures. The mass of each compound can be determined in the chemical ionization mode and detection of positive or negative ions. This method presents a considerable improvement compared to those using TMS derivatives. Indeed the heptafluorobutyrate derivatives are stable, and acylation of amino groups is complete. Moreover, there is no interference with contaminants and the separation between fatty acid methyl-esters and O-methyl glycosides is achieved.
我们开发了一种方法,该方法涉及在甲醇解后从糖蛋白和糖脂中释放出的O-甲基糖苷形成七氟丁酸酯衍生物。这些糖缀合物中最常见的单糖(阿拉伯糖、鼠李糖、木糖、岩藻糖、半乳糖、甘露糖、葡萄糖、N-乙酰葡糖胺、N-乙酰半乳糖胺、N-乙酰神经氨酸、2-酮基-3-脱氧辛酸)的稳定衍生物可以在赖氨酸作为内标的情况下进行分离,并以高灵敏度水平(低至25皮摩尔)进行定量和可重复测定。与天冬酰胺结合在N-聚糖中的N-乙酰葡糖胺残基以两个峰的形式被定量回收。后者很容易与N-聚糖的其他N-乙酰葡糖胺残基区分开来,从而使得从单次碳水化合物分析中获得的N-聚糖结构数据有了显著改进。常用于分离可溶性或膜结合糖蛋白的缓冲液中存在的最常见污染物(十二烷基硫酸钠、聚山梨醇酯80、脱氧胆酸钠、三羟甲基氨基甲烷、甘氨酸以及聚丙烯酰胺或盐,以及蛋白聚糖的单糖成分或核酸降解产物)不会干扰这些测定。从十二烷基硫酸钠/聚丙烯酰胺凝胶电泳凝胶或聚偏二氟乙烯膜中分离出的糖蛋白的碳水化合物分析可以在微克量水平上进行,而不会有明显干扰。由于脂肪酸甲酯和鞘氨醇衍生物与单糖峰分离,从通过制备硅胶薄层层析纯化的不到1微克的初始化合物开始,一步即可实现神经节苷脂的完整组成分析。使用电子轰击电离质谱法,不同类别的O-甲基糖苷(戊糖、脱氧己糖、己糖、己糖胺、糖醛酸、唾液酸和2-酮基-3-脱氧辛酸)的报告离子可用于在非常复杂的混合物中鉴定这些化合物。每种化合物的质量可以在化学电离模式下通过检测正离子或负离子来确定。与使用三甲基硅烷衍生物的方法相比,该方法有了显著改进。实际上,七氟丁酸酯衍生物很稳定,氨基的酰化反应完全。此外,不受污染物干扰,并且实现了脂肪酸甲酯和O-甲基糖苷之间的分离。