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Design, Preparation, and Implementation of Axially Chiral Benzotetramisoles as Lewis Base Catalysts for Asymmetric Cycloadditions

Zitong Lin, Ying Yu, Rixin Liu, Weiwei Zi

2024Angewandte Chemie International Edition10 citationsDOIOpen Access PDF

Abstract

Developing novel catalysts with potent activity is of great importance in organocatalysis. In this study, we designed and prepared a new class of benzotetramisole Lewis base catalysts (AxBTM) that have both central and axial chirality. This unique feature of these catalysts results in a three-dimensional microenvironment with multi-layers of chirality. The performance of the developed catalysts was tested in a series of cycloaddition reactions. These included the AxBTM-catalyzed (2+2) cycloaddition between α-fluoro-α-aryl anhydride with imines or oxindoles, and the sequential gold/AxBTM-catalyzed (4+2) cycloaddition of enynamides with pentafluorophenyl esters. The interplay between axial and central chirality had a collaborative effect in regulating the stereochemistry in these cycloadditions, leading to high levels of stereoselectivity that would otherwise be challenging to achieve using conventional BTM catalysts. However, the (2+2) and (4+2) cycloadditions have different predilections for axial and central chirality combinations.

Topics & Concepts

Axial symmetryLewis acids and basesCatalysisBase (topology)ChemistryCombinatorial chemistryOrganic chemistryMathematicsGeometryMathematical analysisAsymmetric Synthesis and CatalysisSynthesis of β-Lactam CompoundsOrganic Chemistry Cycloaddition Reactions
Design, Preparation, and Implementation of Axially Chiral Benzotetramisoles as Lewis Base Catalysts for Asymmetric Cycloadditions | Litcius