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Atroposelective Synthesis of Axially Chiral N‐Arylpyrroles by Chiral‐at‐Rhodium Catalysis

Chen‐Xi Ye, Shuming Chen, Feng Han, Xiulan Xie, Sergei I. Ivlev, K. N. Houk, Eric Meggers

2020Angewandte Chemie31 citationsDOIOpen Access PDF

Abstract

Abstract A transformation of fluxional into configurationally stable axially chiral N‐arylpyrroles was achieved with a highly atroposelective electrophilic aromatic substitution catalyzed by a chiral‐at‐metal rhodium Lewis acid. Specifically, N‐arylpyrroles were alkylated with N‐acryloyl‐1 H ‐pyrazole electrophiles in up to 93 % yield and with up to >99.5 % ee , and follow‐up conversions reveal the synthetic utility of this new method. DFT calculations elucidate the origins of the observed excellent atroposelectivity.

Topics & Concepts

RhodiumElectrophileChemistryLewis acids and basesCatalysisElectrophilic substitutionYield (engineering)AlkylationEnantioselective synthesisCombinatorial chemistryStereochemistryMedicinal chemistryOrganic chemistryMaterials scienceMetallurgyAxial and Atropisomeric Chirality SynthesisMolecular spectroscopy and chiralitySphingolipid Metabolism and Signaling
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