Division of Biological Chemistry and Drug Discovery, College of Life Sciences, University of Dundee, Dundee, UK.
Chem Biol Drug Des. 2012 Mar;79(3):270-8. doi: 10.1111/j.1747-0285.2011.01300.x.
Disruption of glycosylphosphatidylinositol biosynthesis is genetically and chemically validated as a drug target against the protozoan parasite Trypanosoma brucei, the causative agent of African sleeping sickness. The N-acetylglucosamine-phosphatidylinositol de-N-acetylase (deNAc) is a zinc metalloenzyme responsible for the second step of glycosylphosphatidylinositol biosynthesis. We recently reported the synthesis of eight deoxy-2-C-branched monosaccharides containing carboxylic acid, hydroxamic acid, or N-hydroxyurea substituents at the C2 position that may act as zinc-binding groups. Here, we describe the synthesis of a glucocyclitol-phospholipid incorporating a hydroxamic acid moiety and report the biochemical evaluation of the monosaccharides and the glucocyclitol-phospholipid as inhibitors of the trypanosome deNAc in the cell-free system and against recombinant enzyme. Monosaccharides with carboxylic acid or hydroxamic acid substituents were found to be the inhibitors of the trypanosome deNAc with IC(50) values 0.1-1.5mM and the glucocyclitol-phospholipid was found to be a dual inhibitor of the deNAc and the α1-4-mannose transferase with an apparent IC(50)= 19±0.5μm.
糖基磷脂酰肌醇生物合成的破坏在遗传和化学上被验证为针对原生动物寄生虫布氏锥虫(引起非洲昏睡病的病原体)的药物靶点。N-乙酰葡糖胺-磷酸肌醇去-N-乙酰基酶(deNAc)是一种锌金属酶,负责糖基磷脂酰肌醇生物合成的第二步。我们最近报道了合成了八个含有羧酸、羟肟酸或 N-羟脲取代基的 2-C-去氧单糖,这些取代基可能作为锌结合基团。在这里,我们描述了一种含有羟肟酸部分的葡糖环醇磷脂的合成,并报告了这些单糖和葡糖环醇磷脂作为无细胞体系中以及针对重组酶的抑制剂对锥虫 deNAc 的生化评估。具有羧酸或羟肟酸取代基的单糖被发现是锥虫 deNAc 的抑制剂,IC(50)值为 0.1-1.5mM,而葡糖环醇磷脂被发现是 deNAc 和 α1-4-甘露糖转移酶的双重抑制剂,表观 IC(50)= 19±0.5μm。