Process Research and Development, Merck & Co., Inc., Rahway, NJ 07065, USA.
Science. 2017 Apr 28;356(6336):426-430. doi: 10.1126/science.aam7936.
The catalytic stereoselective synthesis of compounds with chiral phosphorus centers remains an unsolved problem. State-of-the-art methods rely on resolution or stoichiometric chiral auxiliaries. Phosphoramidate prodrugs are a critical component of pronucleotide (ProTide) therapies used in the treatment of viral disease and cancer. Here we describe the development of a catalytic stereoselective method for the installation of phosphorus-stereogenic phosphoramidates to nucleosides through a dynamic stereoselective process. Detailed mechanistic studies and computational modeling led to the rational design of a multifunctional catalyst that enables stereoselectivity as high as 99:1.
手性磷中心化合物的催化立体选择性合成仍然是一个未解决的问题。最先进的方法依赖于拆分或计量手性助剂。膦酰胺酯前药是用于治疗病毒病和癌症的前核苷酸(ProTide)疗法的关键组成部分。在这里,我们描述了通过动态立体选择性过程在核苷上安装磷立体磷酰胺酯的催化立体选择性方法的开发。详细的机理研究和计算模型导致了多功能催化剂的合理设计,该催化剂能够实现高达 99:1 的立体选择性。