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区域发散的双环杂芳烃催化不对称去芳构化环加成反应。

Regiodivergent catalytic asymmetric dearomative cycloaddition of bicyclic heteroaromatics.

机构信息

Chongqing Key Laboratory of Natural Product Synthesis and Drug Research, Chemical Biology Research Center, School of Pharmaceutical Sciences, Chongqing University, Chongqing, China.

Chongqing Key Laboratory of Theoretical and Computational Chemistry, School of Chemistry and Chemical Engineering, Chongqing University, Chongqing, China.

出版信息

Sci Adv. 2023 Mar 29;9(13):eadg1645. doi: 10.1126/sciadv.adg1645.

Abstract

The catalytic dearomative cycloaddition of bicyclic heteroaromatics including benzofurans and indoles provides rapid access to functionalized heterocyclic molecules. Because of the inherent stereoelectronic differences, the furan or pyrrole nucleus is more prone to dearomative cycloaddition than the benzene ring. Here, we realized a geometry-based differentiation approach for achieving C6-C7 and C7-C7a regioselectivity. The rotationally restricted σ bond at C7 position respectively placed the C6-C7 and C7-C7a sites of benzofurans or indoles in an optimal spatial orientation toward the axially chiral heterodiene, thus affording two enantioenriched polycyclic compounds from a single racemic heterobiaryl atropisomers. Calculation results of density functional theory interpreted the mechanism of this parallel kinetic resolution. The bioactivity of the dearomatized products was evaluated in cancer cell lines with certain compounds exhibiting interesting biological activities.

摘要

包括苯并呋喃和吲哚在内的双环杂芳烃的催化去芳构化环加成反应为功能化杂环分子的快速构建提供了途径。由于固有立体电子差异,呋喃或吡咯核比苯环更容易发生去芳构化环加成。在这里,我们实现了一种基于几何形状的区分方法,以实现 C6-C7 和 C7-C7a 区域选择性。C7 位的旋转受限σ键分别将苯并呋喃或吲哚的 C6-C7 和 C7-C7a 位点置于与轴手性杂二烯的最佳空间取向,从而从单个外消旋杂芳基对映异构体中得到两种对映体富集的多环化合物。密度泛函理论的计算结果解释了这种平行动力学拆分的机制。对去芳构化产物的生物活性进行了评估,某些化合物在癌细胞系中表现出有趣的生物活性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d21d/10058237/cee4c2bf8367/sciadv.adg1645-f1.jpg

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