Someya Hidehisa, Itoh Taiki, Kato Mebae, Aoki Shin
Faculty of Pharmaceutical Sciences, Tokyo University of Science.
Faculty of Pharmaceutical Sciences, Tokyo University of Science; Imaging Frontier Center, Tokyo University of Science;
J Vis Exp. 2018 Jul 26(137):57897. doi: 10.3791/57897.
Disaccharide nucleosides, which consist of disaccharide and nucleobase moieties, have been known as a valuable group of natural products having multifarious bioactivities. Although chemical O-glycosylation is a commonly beneficial strategy to synthesize disaccharide nucleosides, the preparation of substrates such as glycosyl donors and acceptors requires tedious protecting group manipulations and a purification at each synthetic step. Meanwhile, several research groups have reported that boronic and borinic esters serve as a protecting or activating group of carbohydrate derivatives to achieve the regio- and/or stereoselective acylation, alkylation, silylation, and glycosylation. In this article, we demonstrate the procedure for the regioselective O-glycosylation of unprotected ribonucleosides utilizing boronic acid. The esterification of 2',3'-diol of ribonucleosides with boronic acid makes the temporary protection of diol, and, following O-glycosylation with a glycosyl donor in the presence of p-toluenesulfenyl chloride and silver triflate, permits the regioselective reaction of the 5'-hydroxyl group to afford the disaccharide nucleosides. This method could be applied to various nucleosides, such as guanosine, adenosine, cytidine, uridine, 5-metyluridine, and 5-fluorouridine. This article and the accompanying video represent useful (visual) information for the O-glycosylation of unprotected nucleosides and their analogs for the synthesis of not only disaccharide nucleosides, but also a variety of biologically relevant derivatives.
由二糖和核苷碱基部分组成的二糖核苷,是一类具有多种生物活性的重要天然产物。尽管化学O-糖基化是合成二糖核苷常用的有效策略,但诸如糖基供体和受体等底物的制备需要繁琐的保护基操作,并且在每个合成步骤都需要进行纯化。同时,几个研究小组报道,硼酸酯和亚硼酸酯可作为碳水化合物衍生物的保护或活化基团,以实现区域和/或立体选择性酰化、烷基化、硅烷化和糖基化。在本文中,我们展示了利用硼酸对未保护的核糖核苷进行区域选择性O-糖基化的方法。核糖核苷的2',3'-二醇与硼酸的酯化反应实现了二醇的临时保护,然后在对甲苯亚磺酰氯和三氟甲磺酸银存在下与糖基供体进行O-糖基化反应,使5'-羟基发生区域选择性反应,从而得到二糖核苷。该方法可应用于多种核苷,如鸟苷、腺苷、胞苷、尿苷、5-甲基尿苷和5-氟尿苷。本文及随附视频为未保护核苷及其类似物的O-糖基化提供了有用的(可视化)信息,不仅可用于合成二糖核苷,还可用于合成各种具有生物学意义的衍生物。