Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138, USA.
Science. 2021 Nov 5;374(6568):752-757. doi: 10.1126/science.abm0386. Epub 2021 Nov 4.
A strategy that facilitates the construction of a wide variety of trisubstituted stereocenters through a catalytically accessed common chiral intermediate could prove highly enabling for the field of synthetic chemistry. We report the discovery of enantioselective, catalytic 1,2-boronate rearrangements for the synthesis of α-chloro pinacol boronic esters from readily available boronic esters and dichloromethane. The chiral building blocks produced in these reactions can undergo two sequential stereospecific elaborations to generate a wide assortment of trisubstituted stereocenters. The enantioselective reaction is catalyzed by a lithium-isothiourea-boronate complex, which is proposed to promote rearrangement through a dual–lithium-induced chloride abstraction orchestrated by Lewis basic functionality on the catalyst scaffold.
一种通过催化获得的通用手性中间体来促进合成各种三取代立体中心的策略,可能会对合成化学领域具有高度的启发性。我们报告了对映选择性催化 1,2-硼酸酯重排反应的发现,该反应可从易得的硼酸酯和二氯甲烷合成α-氯频哪醇硼酸酯。这些反应中生成的手性构建块可以经历两个连续的立体特异性修饰,以生成广泛的三取代立体中心。对映选择性反应由锂异硫脲-硼酸酯配合物催化,该配合物通过催化剂骨架上的路易斯碱性官能团协调的双锂诱导的氯原子消除来促进重排。