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Ligand-Enabled C–H Hydroxylation with Aqueous H<sub>2</sub>O<sub>2</sub>at Room Temperature

Zhen Li, Han Seul Park, Jennifer X. Qiao, Kap‐Sun Yeung, Jin‐Quan Yu

2022Journal of the American Chemical Society71 citationsDOIOpen Access PDF

Abstract

With the large number of Pd(II)-catalyzed C–H activation reactions of native substrates developed in the past decade, the development of catalysts to enable the use of green oxidants under safe and practical conditions has become an increasingly important challenge. Notably, the compatibility of Pd(II) catalysts with sustainable aqueous H2O2 has been a long-standing challenge in catalysis including Wacker-type oxidations. We report herein a bifunctional bidentate carboxyl-pyridone (CarboxPyridone) ligand that enables room-temperature Pd-catalyzed C–H hydroxylation of a broad range of benzoic and phenylacetic acids with an industry-compatible oxidant, aqueous hydrogen peroxide (35% H2O2). The scalability of this methodology is demonstrated by a 1000 mmol scale reaction of ibuprofen (206 g) using only a 1 mol % Pd catalyst loading. The utility of this protocol is further illustrated through derivatization of the products and synthesis of polyfluorinated natural product coumestan and pterocarpene from phenol intermediates prepared using this methodology.

Topics & Concepts

ChemistryCatalysisHydroxylationAqueous solutionBifunctionalHydrogen peroxideLigand (biochemistry)DenticityCombinatorial chemistryPhenolGreen chemistryOrganic chemistryReaction mechanismMetalBiochemistryEnzymeReceptorCatalytic C–H Functionalization MethodsOxidative Organic Chemistry ReactionsSynthesis of Indole Derivatives
Ligand-Enabled C–H Hydroxylation with Aqueous H<sub>2</sub>O<sub>2</sub>at Room Temperature | Litcius