葡萄糖苷酶抑制剂作用机理的分子动力学模拟和自由能计算(英文)

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含有锍离子的葡萄糖苷酶抑制剂如kotalanol(SK)和它除去磺酸基团后的衍生物(DSK),是潜在的毒副作用较小的治疗Ⅱ型糖尿病的候选药物.α-葡萄糖苷酶抑制活性实验显示,DSK活性比SK略高,而将二者环上的S原子替换成NH后(分别称为DSN和SN),DSN的活性要比SN高1500倍左右.本文用分子动力学模拟,结合自由能计算和自由能分解的方法对上述四个抑制剂的作用机理进行了研究.研究结果表明活性的巨大差异是由NH基团取代效应和磺酸基团立体效应共同作用的结果,由于N―C键长比S―C键长短,NH基团取代导致烷基链的翻转,同时,磺酸基团限制了链的翻转,因此改变了抑制剂的结合模式.计算结果与实验基本一致.本文的研究结果有助于进一步理解含锍离子的葡萄糖苷酶抑制剂的结合机理,并为设计更有潜力的葡萄糖苷酶抑制剂提供了有价值的信息. Sulfonium ion-containing glucosidase inhibitors such as kotalanol (SK) and its derivatives after sulfonic acid group removal (DSK) are potential drug candidates for the treatment of type 2 diabetes with less toxic side effects.α-Glucosidase The activity of DSK showed that the activity of DSK was slightly higher than that of SK, and after replacing the S atom on both rings with NH (respectively referred to as DSN and SN), the activity of DSN was about 1500 times higher than that of SN.In this paper, Simulation, combined with the calculation of free energy and free energy decomposition method for the above four inhibitors mechanism of action was studied.The results show that the great difference in activity is the result of the combination of the NH group substitution effect and the three-dimensional effect of sulfonic acid groups , As the N-C bond length is longer than the S-C bond length, the substitution of NH group leads to the reversal of the alkyl chain, meanwhile, the sulfonic acid group restricts the turnover of the chain, thus changing the binding mode of the inhibitor. The results of this study will help to further understand the binding mechanism of glucosidase inhibitor containing sulfonium ions and provide valuable information for designing more potential glucosidase inhibitors.
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