Boeckler Frank M, Joerger Andreas C, Jaggi Gaurav, Rutherford Trevor J, Veprintsev Dmitry B, Fersht Alan R
Centre for Protein Engineering, Medical Research Council Centre, Hills Road, Cambridge CB2 0QH, United Kingdom.
Proc Natl Acad Sci U S A. 2008 Jul 29;105(30):10360-5. doi: 10.1073/pnas.0805326105. Epub 2008 Jul 23.
The tumor suppressor p53 is mutationally inactivated in approximately 50% of human cancers. Approximately one-third of the mutations lower the melting temperature of the protein, leading to its rapid denaturation. Small molecules that bind to those mutants and stabilize them could be effective anticancer drugs. The mutation Y220C, which occurs in approximately 75,000 new cancer cases per annum, creates a surface cavity that destabilizes the protein by 4 kcal/mol, at a site that is not functional. We have designed a series of binding molecules from an in silico analysis of the crystal structure using virtual screening and rational drug design. One of them, a carbazole derivative (PhiKan083), binds to the cavity with a dissociation constant of approximately 150 muM. It raises the melting temperature of the mutant and slows down its rate of denaturation. We have solved the crystal structure of the protein-PhiKan083 complex at 1.5-A resolution. The structure implicates key interactions between the protein and ligand and conformational changes that occur on binding, which will provide a basis for lead optimization. The Y220C mutant is an excellent "druggable" target for developing and testing novel anticancer drugs based on protein stabilization. We point out some general principles in relationships between binding constants, raising of melting temperatures, and increase of protein half-lives by stabilizing ligands.
肿瘤抑制因子p53在大约50%的人类癌症中发生突变失活。大约三分之一的突变降低了该蛋白的解链温度,导致其快速变性。与这些突变体结合并使其稳定的小分子可能是有效的抗癌药物。每年约有75000例新癌症病例中出现的Y220C突变,在一个无功能的位点产生了一个使蛋白稳定性降低4千卡/摩尔的表面腔。我们通过虚拟筛选和合理药物设计对晶体结构进行计算机分析,设计了一系列结合分子。其中之一,一种咔唑衍生物(PhiKan083),以约150μM的解离常数与该腔结合。它提高了突变体的解链温度,并减缓了其变性速率。我们已以1.5埃的分辨率解析了蛋白质-PhiKan083复合物的晶体结构。该结构揭示了蛋白质与配体之间的关键相互作用以及结合时发生的构象变化,这将为先导化合物优化提供基础。Y220C突变体是基于蛋白质稳定化开发和测试新型抗癌药物的一个极好的“可成药”靶点。我们指出了结合常数、解链温度升高以及通过稳定配体增加蛋白质半衰期之间关系的一些一般原则。