Enantioselective Cyclization of Bromoenynes: Mechanistic Understanding of Gold(I)-Catalyzed Alkoxycyclizations

The first enantioselective gold(I)-catalyzed alkoxycyclization of bromo-1,6-enynes is achieved using a modified JohnPhos ligand with a distal C2-chiral 2,5-diarylpyrrolidine. By using a chiral catalyst of the same family, the enantioselective cascade cyclization of bromo-1,5-enynes to afford polycyc...

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Detalles Bibliográficos
Autores: Cataffo, Andrea, Garcia-Padilla, Eduardo, Escofet, Imma, Fincias, Nicolas, Arnanz, Anna, Zuccarello, Giuseppe, Tian, Guilong, Cai, Luyu, Khorasani, Fereshteh, Maseras, Feliu, Echavarren, Antonio M.
Tipo de recurso: artículo
Fecha de publicación:2026
País:España
Institución: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:2072/489078
Acceso en línea:http://hdl.handle.net/2072/489078
https://doi.org/10.1039/D5SC09023G
Access Level:acceso abierto
Palabra clave:Química
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Descripción
Sumario:The first enantioselective gold(I)-catalyzed alkoxycyclization of bromo-1,6-enynes is achieved using a modified JohnPhos ligand with a distal C2-chiral 2,5-diarylpyrrolidine. By using a chiral catalyst of the same family, the enantioselective cascade cyclization of bromo-1,5-enynes to afford polycyclic scaffolds was also achieved for the first time. Performing the cyclization of bromo-1,6-enynes in absence of an alcohol as nucleophile leads to the formation of products of cycloisomerization, with lower enantiomeric excess than those of the alkoxycyclization. Control experiments and DFT calculations support the hypothesis of an in-cycle racemization process based on a 1,2-hydrogen shift, which sheds light on the mechanism of gold(I)-catalyzed alkoxycyclizations.