Wang Jinhui, Wang Shengchun, Wei Zhihong, Wang Pengjie, Cao Yanwei, Huang Yang, He Lin, Lei Aiwen
State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics (LICP), Chinese Academy of Sciences, Lanzhou 730000, China.
Institute for Advanced Studies (IAS), College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, China.
Science. 2024 Nov 15;386(6723):776-782. doi: 10.1126/science.adl0149. Epub 2024 Nov 14.
Unsymmetrical ureas are commonly found in pharmaceuticals and bioactive compounds. However, devising strategies to introduce two distinct amines selectively in the construction of unsymmetrical ureas remains a challenge. In this work, we use a synchronous recognition strategy that takes advantage of radical and nucleophilic activation to discriminate between secondary and primary amines. Specifically, a copper catalyst preferentially oxidizes secondary amines to radical species, whereas a cobalt catalyst carbonylates primary amines to produce cobalt amides. Coupling these fragments by cooperative catalysis produces unsymmetrical ureas with high selectivity, as showcased by the modification of 41 biologically active compounds and six drugs.
不对称脲常见于药物和生物活性化合物中。然而,在构建不对称脲的过程中设计选择性引入两种不同胺的策略仍然是一项挑战。在这项工作中,我们使用了一种同步识别策略,该策略利用自由基和亲核活化来区分仲胺和伯胺。具体而言,铜催化剂优先将仲胺氧化为自由基物种,而钴催化剂使伯胺羰基化以生成钴酰胺。通过协同催化将这些片段偶联可产生具有高选择性的不对称脲,41种生物活性化合物和6种药物的修饰展示了这一点。