Litcius/Paper detail

Enantio‐ and Regioselective Construction of 1,4‐Diamines via Cascade Hydroamination of Methylene Cyclopropanes

Jian Zhou, Qingjing Yang, Chi‐Sing Lee, Jun Wang

2022Angewandte Chemie International Edition45 citationsDOI

Abstract

Abstract Despite the widespread existence of chiral 1,4‐diamines in bioactive molecules and their applications in asymmetric catalysis, the catalytic and asymmetric synthesis of such structures from readily accessible substrates remains a long‐standing challenge. Here, we report a Cu‐catalyzed asymmetric cascade hydroamination protocol to construct a wide range of chiral 1,4‐diamine derivatives in high yields with excellent enatioselectivities (up to 95 % yield and up to >99 % ee). The use of two hydroxylamine esters containing different functionalized amino groups allowed us to increase the complexity of the final 1,4‐diamine structures. The desired products could be easily transformed into chiral 1,4‐diamines and chiral NH 2 ‐Terfenadine. Mechanistic study demonstrates that this reaction proceeds through hydroamination ring‐opening and cascade hydroamination sequence.

Topics & Concepts

HydroaminationRegioselectivityChemistryDiamineCombinatorial chemistryEnantioselective synthesisHydroxylamineCascade reactionCatalysisYield (engineering)StereochemistryOrganic chemistryMaterials scienceMetallurgyCyclopropane Reaction MechanismsCatalytic C–H Functionalization MethodsSynthesis and Catalytic Reactions