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Distal Amidoketone Synthesis Enabled by Dimethyl Benziodoxoles via Dual Copper/Photoredox Catalysis

Yuanyuan Ge, Yingbo Shao, Shuang Wu, Pan Liu, Junzhao Li, Hanzhang Qin, Yanxia Zhang, Xiao‐Song Xue, Yiyun Chen

2023ACS Catalysis20 citationsDOI

Abstract

Herein, we report distal amidoketone and nitrogen-functionalized ketone syntheses from alcohols and N–H nucleophiles enabled by hypervalent iodine dimethyl benziodoxoles, BI m . Dimethyl benziodoxoles BI m dually activate alcohols and various N–H nucleophiles by forming key BI m –O and BI m –N complexes in which the BI m –N complex is characterized by X-ray crystallography and computationally investigated. Readily available N–H nucleophile imides, sulfonamides, carbamates, triazoles, indazoles, and sulfoximines engage in photoredox/copper catalysis to synthesize distal amidoketones and nitrogen-functionalized ketones with excellent regioselectivity and chemoselectivity. This reaction scales up to grams, applies to late-stage complex molecule modification, and streamlines synthetic routes.

Topics & Concepts

NucleophileChemoselectivityChemistryRegioselectivityHypervalent moleculeCatalysisKetoneCombinatorial chemistryPhotoredox catalysisCopperOrganic chemistryIodinePhotocatalysisOxidative Organic Chemistry ReactionsSynthesis and Catalytic ReactionsCatalytic C–H Functionalization Methods