Iridium-Catalyzed Enantioselective Intramolecular Hydroarylation of Allenes: Formal Synthesis of (+)-Rhazinilam

We report a versatile, highly enantioselective intramolecular hydroarylation of allenyl-tethered pyrroles and indoles. The reaction, promoted by an iridium(I)/bisphosphine chiral catalyst, provides a direct access heteropolycyclic systems bearing either tertiary or quaternary carbon stereocenters an...

Descripción completa

Detalles Bibliográficos
Autores: Arribas, Andrés, Rey, Alejandro, Calvelo, Martín, Mascareñas, José L., López García, Fernando José
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2025
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/394246
Acceso en línea:http://hdl.handle.net/10261/394246
https://api.elsevier.com/content/abstract/scopus_id/105007438963
Access Level:acceso abierto
Palabra clave:Allenes
C–H activation
Enantioselective
Hydroarylation
Iridium
http://metadata.un.org/sdg/9
Build resilient infrastructure, promote inclusive and sustainable industrialization and foster innovation
Descripción
Sumario:We report a versatile, highly enantioselective intramolecular hydroarylation of allenyl-tethered pyrroles and indoles. The reaction, promoted by an iridium(I)/bisphosphine chiral catalyst, provides a direct access heteropolycyclic systems bearing either tertiary or quaternary carbon stereocenters and a synthetically appealing alkenyl pendant. The method allows a highly efficient assembly of five-, six- and even seven-membered fused indole and pyrrole products, providing enantiomeric excesses of up to 99%. DFT computational studies align nicely with the experimental results and allow to rationalize the key factors that control both regio- and stereoselectivity of the process. Finally, the synthetic potential of the method was exemplified with a very short, highly enantioselective formal synthesis of (+)-Rhazinilam.