Christensen Helle, Christiansen Mira Steinicke, Petersen Jette, Jensen Henrik Helligsø
Department of Chemistry, University of Aarhus, Langelandsgade 140, DK-8000, Aarhus C, Denmark.
Org Biomol Chem. 2008 Sep 21;6(18):3276-83. doi: 10.1039/b807064d. Epub 2008 Jul 28.
A direct, mild and efficient protocol for the preparation of beta-glycosides of N-acetyl glucosamine (GlcNAc) and N-acetyl galactosamine (GalNAc) has been developed using peracetylated beta-GlcNAc and beta-GalNAc as donors. All rare Earth metal triflate promoters screened were found to promote glycosylation with Sc(OTf)(3) being superior in terms of reaction rate. Simple alcohol glycosylation was found to proceed smoothly in refluxing dichloromethane, whereas higher temperatures under microwave conditions were needed to attain acceptable yields with less reactive, carbohydrate based glycosyl acceptors. The protocol developed was applied to provide the first example of direct chemical formation of a disaccharide using both GlcNAc as a glycosyl donor and acceptor. The alpha-acetate donor was found to be significantly less reactive than the corresponding beta-anomer necessitating higher reaction temperatures under which glycoside anomerisation was found to occur. It was established, that the anomerisation only took place in the presence of both Sc(OTf)(3) and acetic acid.
以全乙酰化的β - N - 乙酰葡糖胺(GlcNAc)和β - N - 乙酰半乳糖胺(GalNAc)作为供体,已开发出一种直接、温和且高效的制备N - 乙酰葡糖胺(GlcNAc)和N - 乙酰半乳糖胺(GalNAc)的β - 糖苷的方法。筛选出的所有稀土金属三氟甲磺酸盐促进剂均能促进糖基化反应,其中Sc(OTf)₃在反应速率方面表现更优。发现简单的醇糖基化反应在回流的二氯甲烷中能顺利进行,而对于反应活性较低的基于碳水化合物的糖基受体,在微波条件下需要更高的温度才能获得可接受的产率。所开发的方法被用于提供第一个使用GlcNAc作为糖基供体和受体直接化学合成二糖的实例。发现α - 乙酸酯供体的反应活性明显低于相应的β - 端基异构体,这需要更高的反应温度,在此温度下发现会发生糖苷端基异构化。已确定,端基异构化仅在Sc(OTf)₃和乙酸同时存在的情况下发生。