Department of Chemistry, Drexel University, 32 South 32nd St., Philadelphia, PA, 19104, USA.
Departmento de Química, Centro de Investigación y de Estudios Avanzados (Cinvestav), Av. Instituto Politécnico Nacional 2508, Ciudad de México, 07360, México.
Angew Chem Int Ed Engl. 2017 Apr 3;56(15):4310-4313. doi: 10.1002/anie.201612574. Epub 2017 Mar 13.
Isocyanides are exceptional building blocks, the wide deployment of which in multicomponent and metal-insertion reactions belies their limited availability. The first conjugate addition/alkylation to alkenyl isocyanides is described, which addresses this deficiency. An array of organolithiums, magnesiates, enolates, and metalated nitriles add conjugately to β- and β,β-disubstituted arylsulfonyl alkenyl isocyanides to rapidly assemble diverse isocyanide scaffolds. The intermediate metalated isocyanides are efficiently trapped with electrophiles to generate substituted isocyanides incorporating contiguous tri- and tetra-substituted centers. The substituted isocyanides are ideally functionalized for elaboration into synthetic targets as illustrated by the three-step synthesis of γ-carboline N-methyl ingenine B.
异氰化物是一种特殊的构建模块,尽管其应用广泛,但由于其有限的可用性,在多组分和金属插入反应中仍未得到广泛应用。本文首次描述了烯基异氰化物的共轭加成/烷基化反应,该方法解决了这一不足。一系列有机锂试剂、镁试剂、烯醇盐和金属化腈可以与β-和β,β-二取代芳基磺酰基烯基异氰化物进行共轭加成,从而快速构建各种异氰化物支架。通过与亲电试剂的有效捕获,中间体金属化异氰化物可以有效地生成包含连续三取代和四取代中心的取代异氰化物。取代异氰化物可以通过进一步的官能团化来制备合成目标分子,这一点在三步合成γ-咔啉 N-甲基 ingenine B 的过程中得到了很好的体现。