Key Laboratory of Green Chemistry & Technology of Ministry of Education, College of Chemistry, Sichuan University, 29 Wangjiang Road, Chengdu, 610064, P. R. China.
Medical Administration Department, Sichuan Academy of Medical Sciences & Sichuan Provincial People's Hospital, Chengdu, 610072, P. R. China.
Angew Chem Int Ed Engl. 2022 Jul 25;61(30):e202202467. doi: 10.1002/anie.202202467. Epub 2022 Jun 1.
Axially chiral biaryl monophosphorus molecules, exemplified by atropisomeric 1,1'-biaryl aminophosphines, are significant motifs in numerous chiral ligands/catalysts. Developing efficient methods for preparing phosphorus compounds with these privileged motifs is an important endeavor in synthetic chemistry. Herein, we develop an effective, modular method by a chiral-phosphonium-salt-catalyzed novel cascade between phosphorus-containing nitroolefins and α,α-dicyanoolefins, leading to a great diversity of atropisomeric biaryls bearing phosphorus groups in high yields with excellent stereoselectivities. The reaction features include a Thorpe-type cycloaddition/oxidative hydroxylation/aromatization cascade pathway with a central-to-axial chirality transfer process. Insight gained from our studies is expected to advance general efforts towards the catalytic synthesis of atropisomeric biaryl phosphorus compounds, offering a platform for developing new efficient chiral ligands and catalysts.
轴手性联芳单磷分子,以手性的 1,1'-联芳基氨基膦为例,是许多手性配体/催化剂中的重要结构单元。开发具有这些优势结构单元的磷化合物的有效方法是合成化学中的一项重要任务。在此,我们通过手性磷翁盐催化的含磷硝基烯烃与α,α-二氰基烯烃之间的新型级联反应,开发了一种有效且模块化的方法,以高产率和优异的立体选择性得到了多种带有磷基团的轴手性联芳产物。该反应的特点包括 Thorpe 型环加成/氧化羟化/芳构化级联途径,具有中心到轴向手性转移过程。我们的研究获得的见解有望推动手性联芳基磷化合物的催化合成的一般努力,为开发新的高效手性配体和催化剂提供了一个平台。