CCNU-uOttawa Joint Research Centre, Key Laboratory of Pesticide and Chemical Biology, Ministry of Education, College of Chemistry , Central China Normal University , 152 Luoyu Road , Wuhan 430079 , China.
School of Chemistry and Chemical Engineering , Chongqing University , Chongqing 400030 , China.
J Am Chem Soc. 2019 Apr 17;141(15):6167-6172. doi: 10.1021/jacs.9b02338. Epub 2019 Apr 2.
The first asymmetric propargylic radical cyanation was realized through a dual photoredox and copper catalysis. An organic photocatalyst serves to both generate propargyl radicals and oxidize Cu(I) species to Cu(II) species. A chiral Cu complex functions as an efficient organometallic catalyst to resemble the propargyl radical and cyanide in an enantio-controlled manner. Thus, a diverse range of optically active propargyl cyanides were produced with high reaction efficiency and enantioselectivities (28 examples, 57-97% yields and 83-98% ee). Moreover, mechanistic investigations including experiments and density functional theory calculations were performed to illustrate on the reaction pathway and stereochemical results.
首例不对称炔丙基自由基氰化反应是通过双光氧化还原和铜催化实现的。一种有机光催化剂既能生成炔丙基自由基,又能将 Cu(I)物种氧化为 Cu(II)物种。手性 Cu 配合物作为一种高效的有机金属催化剂,以对映控制的方式模拟炔丙基自由基和亲核试剂氰化物。因此,以高反应效率和对映选择性(28 个实例,产率 57-97%,ee 值 83-98%)得到了多种光学活性的炔丙基氰化物。此外,还进行了包括实验和密度泛函理论计算在内的机理研究,以阐明反应途径和立体化学结果。