1] Department of Chemistry, Imperial College London, London SW7 2AZ, UK [2] Institute of Chemical Biology, Imperial College London, London SW7 2AZ, UK.
Division of Parasitology, MRC National Institute for Medical Research, The Ridgeway, Mill Hill, London NW7 1AA, UK.
Nat Chem. 2014 Feb;6(2):112-21. doi: 10.1038/nchem.1830. Epub 2013 Dec 22.
Malaria is an infectious disease caused by parasites of the genus Plasmodium, which leads to approximately one million deaths per annum worldwide. Chemical validation of new antimalarial targets is urgently required in view of rising resistance to current drugs. One such putative target is the enzyme N-myristoyltransferase, which catalyses the attachment of the fatty acid myristate to protein substrates (N-myristoylation). Here, we report an integrated chemical biology approach to explore protein myristoylation in the major human parasite P. falciparum, combining chemical proteomic tools for identification of the myristoylated and glycosylphosphatidylinositol-anchored proteome with selective small-molecule N-myristoyltransferase inhibitors. We demonstrate that N-myristoyltransferase is an essential and chemically tractable target in malaria parasites both in vitro and in vivo, and show that selective inhibition of N-myristoylation leads to catastrophic and irreversible failure to assemble the inner membrane complex, a critical subcellular organelle in the parasite life cycle. Our studies provide the basis for the development of new antimalarials targeting N-myristoyltransferase.
疟疾是一种由疟原虫属寄生虫引起的传染病,全球每年导致约 100 万人死亡。鉴于当前药物的耐药性不断上升,迫切需要对新的抗疟靶点进行化学验证。酶 N-豆蔻酰转移酶就是这样一个假定的靶点,它催化脂肪酸豆蔻酸与蛋白质底物(N-豆蔻酰化)的连接。在这里,我们报告了一种综合的化学生物学方法,用于探索主要人体寄生虫疟原虫中的蛋白质豆蔻酰化,该方法结合了用于鉴定豆蔻酰化和糖基磷脂酰肌醇锚定蛋白质组的化学蛋白质组学工具,以及选择性的小分子 N-豆蔻酰转移酶抑制剂。我们证明了 N-豆蔻酰转移酶在体外和体内都是疟原虫中必不可少且具有化学可及性的靶点,并表明选择性抑制 N-豆蔻酰化会导致内膜复合物灾难性和不可逆转的组装失败,内膜复合物是寄生虫生命周期中的一个关键亚细胞细胞器。我们的研究为开发针对 N-豆蔻酰转移酶的新型抗疟药物提供了基础。