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Broad-Scope Amination of Aryl Sulfamates Catalyzed by a Palladium Phosphine Complex

Andrea Monti, Joaquín López‐Serrano, Auxiliadora Prieto, M. Carmen Nicasio

2023ACS Catalysis13 citationsDOIOpen Access PDF

Abstract

High Resolution Image Download MS PowerPoint Slide Among phenol-derived electrophiles, aryl sulfamates are attractive substrates since they can be employed as directing groups for C–H functionalization prior to catalysis. However, their use in C–N coupling is limited only to Ni catalysis. Here, we describe a Pd-based catalyst with a broad scope for the amination of aryl sulfamates. We show that the N -methyl-2-aminobiphenyl palladacycle supported by the PCyp 2 Ar Xyl2 ligand (Cyp = cyclopentyl; Ar Xyl2 = 2,6-bis(2,6-dimethylphenyl)phenyl) efficiently catalyzes the C–N coupling of aryl sulfamates with a variety of nitrogen nucleophiles, including anilines, primary and secondary alkyl amines, heteroaryl amines, N -heterocycles, and primary amides. DFT calculations support that the oxidative addition of the aryl sulfamate is the rate-determining step. The C–N coupling takes place through a cationic pathway in the polar protic medium.

Topics & Concepts

ChemistryAminationArylNucleophileCatalysisElectrophilePalladiumOrganic chemistryPhosphineCombinatorial chemistryHomogeneous catalysisLigand (biochemistry)Medicinal chemistryAlkylBiochemistryReceptorCatalytic C–H Functionalization MethodsCatalytic Cross-Coupling ReactionsSulfur-Based Synthesis Techniques