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Ligand-Enabled Monoselective β-C(sp<sup>3</sup>)–H Acyloxylation of Free Carboxylic Acids Using a Practical Oxidant

Zhe Zhuang, Alastair N. Herron, Zhoulong Fan, Jin‐Quan Yu

2020Journal of the American Chemical Society101 citationsDOIOpen Access PDF

Abstract

The development of C–H activation reactions that use inexpensive and practical oxidants remains a significant challenge. Until our recent disclosure of the β-lactonization of free aliphatic acids, the use of peroxides in C–H activation reactions directed by weakly coordinating native functional groups was unreported. Herein, we report C(sp3)–H β-acetoxylation and γ-, δ-, and ε-lactonization reactions of free carboxylic acids enabled by a novel cyclopentane-based mono-N-protected β-amino acid ligand. Notably, tert-butyl hydrogen peroxide is used as the sole oxidant for these reactions. This reaction has several key advantages over other C–H activation protocols: (1) exclusive monoselectivity was observed in the presence of two α-methyl groups; (2) aliphatic carboxylic acids containing α-hydrogens are compatible with this protocol; (3) lactonization of free acids, affording γ-, δ-, or ε-lactones, has been achieved for the first time.

Topics & Concepts

ChemistryCyclopentaneHydrogen peroxideLigand (biochemistry)Carboxylic acidAmino acidMedicinal chemistryStereochemistryOrganic chemistryBiochemistryReceptorCatalytic C–H Functionalization MethodsOxidative Organic Chemistry ReactionsSynthesis and Catalytic Reactions
Ligand-Enabled Monoselective β-C(sp<sup>3</sup>)–H Acyloxylation of Free Carboxylic Acids Using a Practical Oxidant | Litcius