Construction of Axially Chiral Arylpyrroles via Atroposelective Diyne Cyclization

Angew Chem Int Ed Engl. 2023 Jun 5;62(23):e202303670. doi: 10.1002/anie.202303670. Epub 2023 Apr 28.

Abstract

Axially chiral biaryls widely exist in natural products and pharmaceuticals and are used as chiral ligands and catalysts in asymmetric synthesis. Compared to the well-established axially chiral 6-membered biaryl skeletons, examples of 5-membered biaryls have been quite scarce, and mono-substituted 3-arylpyrrole atropisomers have not been reported. Here, we disclose a copper-catalyzed atroposelective diyne cyclization for the construction of a range of axially chiral arylpyrrole biaryls in good to excellent yields with generally excellent enantioselectivities via oxidation and X-H insertion of vinyl cations. Importantly, this protocol not only represents the first synthesis of mono-substituted 3-arylpyrrole atropisomers, but also constitutes the first example of atroposelective diyne cyclization and the first atropisomer construction via vinyl cations. Theoretical calculations further support the mechanism of vinyl cation-involved cyclization and elucidate the origin of enantioselectivity.

Keywords: Alkynes; Asymmetric Catalysis; Axial Chirality; Cyclizations; Heterocycles.