Defluorinative 1,3-Dienylation of Fluoroalkyl N-Triftosylhydrazones with Homoallenols

Chemistry. 2023 Dec 1;29(67):e202302562. doi: 10.1002/chem.202302562. Epub 2023 Oct 19.

Abstract

A silver-catalyzed regioselective defluorinative 1,3-dienylation of trifluoromethyl phenyl N-triftosylhydrazones using homoallenols as 1,3-dienyl sources provides a variety of α-(di)fluoro-β-vinyl allyl ketones with excellent functional group tolerance in moderate to good yields. The reaction proceeds through a silver carbene-initiated sequential etherification and Claisen type [3,3]-sigmatropic rearrangement cascade. The synthetic utility of this protocol was demonstrated through the downstream synthetic elaboration toward diverse synthetically useful building blocks.

Keywords: 1,3-dienylation; carbene; defluorination; silver catalysis; α-fluoro-β-vinyl allyl ketones.