Krasavin Mikhail, Korsakov Mikhail, Dorogov Mikhail, Tuccinardi Tiziano, Dedeoglu Nurcan, Supuran Claudiu T
Institute of Chemistry, Saint Petersburg State University, 26 Universitetskii Prospect, Peterhof, 198504, Russian Federation.
The Ushinsky Yaroslavl State Pedagogical University, 108 Respublikanskaya St., Yaroslavl, 150000, Russian Federation.
Eur J Med Chem. 2015 Aug 28;101:334-47. doi: 10.1016/j.ejmech.2015.06.022. Epub 2015 Jun 25.
A series of potent inhibitors of human carbonic anhydrase (CA) isoforms I and II has been prepared via a direct, chemoselective sulfochlorination of a range of 1,3-oxazolyl benzenes and thiophenes, followed by primary sulfonamide synthesis. The latter functionality is a known zinc-binding group (ZBG) responsible for anchoring the inhibitors to the CA's zinc metal ion. The compound's periphery as well as the overall scaffold geometry was designed to enable optimal interactions with the two distinct sides of the enzyme's active site, one of which is lined with hydrophobic residues and while the other is predominantly hydrophilic. As a result, several compounds inhibiting the therapeutically important cytosolic CA I and CA II in picomolar range have been identified. These compounds are one of the most potent CA inhibitors identified to-date. Not only the remarkable (>10 000-fold), cytosolic CA I and CA II selectivity vs. the membrane-bound CA IX and CA XII isoforms, but also the pronounced CA II/I selectivity observed in some cases, allow considering this series as a set of isoform-selective chemical biology tools and promising starting points for drug candidate development.
通过对一系列1,3-恶唑基苯和噻吩进行直接的化学选择性磺酰氯化,随后合成伯磺酰胺,制备了一系列人碳酸酐酶(CA)同工型I和II的强效抑制剂。后一种官能团是已知的锌结合基团(ZBG),负责将抑制剂锚定到CA的锌金属离子上。化合物的外围以及整体支架几何结构的设计,使其能够与酶活性位点的两个不同侧面实现最佳相互作用,其中一个侧面排列着疏水残基,另一个侧面主要是亲水的。结果,已鉴定出几种在皮摩尔范围内抑制具有治疗重要性的胞质CA I和CA II的化合物。这些化合物是迄今为止鉴定出的最有效的CA抑制剂之一。不仅具有显著的(>10000倍)胞质CA I和CA II相对于膜结合CA IX和CA XII同工型的选择性,而且在某些情况下观察到明显的CA II/I选择性,这使得该系列化合物可被视为一组同工型选择性化学生物学工具以及药物候选物开发的有前景的起点。