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Photochemical Wolff Rearrangement Initiated Generation and Subsequent α-Chlorination of C1 Ammonium Enolates

David Weinzierl, Magdalena Piringer, Paul Zebrowski, Lotte Stockhammer, Mario Waser

2023Organic Letters27 citationsDOIOpen Access PDF

Abstract

High Resolution Image Download MS PowerPoint Slide The enantioselective synthesis of α-chlorinated carboxylic acid esters with er up to 99:1 and yields up to 82% was achieved via a one-pot multistep protocol starting from α-diazoketones. This process proceeds via a photochemical Wolff rearrangement, trapping of the generated ketene with a chiral Lewis base catalyst, subsequent enantioselective α-chlorination, and a final nucleophilic displacement of the bound catalyst. The obtained products were successfully utilized for stereospecific nucleophilic displacement reactions with N - and S -nucleophiles.

Topics & Concepts

ChemistryWolff rearrangementNucleophileKeteneEnantioselective synthesisLewis acids and basesCatalysisStereospecificityMedicinal chemistryPhotochemistryOrganic chemistryCombinatorial chemistryCyclopropane Reaction MechanismsCatalytic C–H Functionalization MethodsOxidative Organic Chemistry Reactions
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