Enantioselective Organocatalytic Diels–Alder Trapping of Photochemically Generated Hydroxy-o-Quinodimethanes

The photoenolization/Diels–Alder strategy offers straightforward access to synthetically valuable benzannulated carbocyclic products. This historical light-triggered process has never before succumbed to efforts to develop an enantioselec- tive catalytic approach. Herein, we demonstrate how asym- me...

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Detalhes bibliográficos
Autores: Dell Amico, Luca, Vega-Penaloza, Alberto, Cuadros, Sara, Melchiorre, Paolo
Formato: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2016
País:España
Recursos:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2072/350685
Acesso em linha:http://hdl.handle.net/2072/350685
https://doi.org/10.1002/anie.201509472
Access Level:acceso abierto
Palavra-chave:54
Descrição
Resumo:The photoenolization/Diels–Alder strategy offers straightforward access to synthetically valuable benzannulated carbocyclic products. This historical light-triggered process has never before succumbed to efforts to develop an enantioselec- tive catalytic approach. Herein, we demonstrate how asym- metric organocatalysis provides simple yet effective catalytic tools to intercept photochemically generated hydroxy-o-qui- nodimethanes with high stereoselectivity. We used a chiral organic catalyst, derived from natural cinchona alkaloids, to activate maleimides toward highly stereoselective Diels–Alder reactions. An unconventional mechanism of stereocontrol is operative, wherein the organocatalyst is actively involved in both the photochemical pathway, by leveraging the formation of the reactive photoenol, and the stereoselectivity-defining event.