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Allylboration of Ketones Catalyzed by BINOL Derivatives: Which Species Are Involved Depending on Substrate Reactivity?
Martel, Arnaud; Zaier, Rania; Braire, Julien; Macé, Aurélie; Vidal, Joelle; Lalli, Claudia; Carreaux, François.
Afiliación
  • Martel A; Institut des Molécules et Matériaux du Mans, IMMM UMR 6283 CNRS-Le Mans Université, Avenue Olivier Messiaen, 72085 Le Mans CEDEX 9, France.
  • Zaier R; Institut des Molécules et Matériaux du Mans, IMMM UMR 6283 CNRS-Le Mans Université, Avenue Olivier Messiaen, 72085 Le Mans CEDEX 9, France.
  • Braire J; Université de Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226, 263 Avenue du Général Leclerc, Campus de Beaulieu, F-35000 Rennes, France.
  • Macé A; Université de Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226, 263 Avenue du Général Leclerc, Campus de Beaulieu, F-35000 Rennes, France.
  • Vidal J; Université de Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226, 263 Avenue du Général Leclerc, Campus de Beaulieu, F-35000 Rennes, France.
  • Lalli C; Université de Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226, 263 Avenue du Général Leclerc, Campus de Beaulieu, F-35000 Rennes, France.
  • Carreaux F; Université de Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226, 263 Avenue du Général Leclerc, Campus de Beaulieu, F-35000 Rennes, France.
J Org Chem ; 89(18): 13224-13234, 2024 Sep 20.
Article en En | MEDLINE | ID: mdl-39258765
ABSTRACT
Allylboration reactions of ketones catalyzed by BINOL derivatives can exhibit highly variable stereochemical courses depending on the nature and reactivity of the ketone substrate. In this Article, we put into perspective the relationship between the nature of the starting material and the active species involved in the asymmetric allyboration catalyzed by BINOL derivatives. This work, aimed at comparing different plausible mechanisms by density functional theory (DFT) at the M06-2X/6-311+G(d,p) level involving different types of allylboronates in the presence of the organocatalyst, leads to the confirmation of the hitherto accepted hypothesis of a reaction promoted by the transient cyclic allyl-1,3,2-dioxaborolane derived from BINOLs in the case of unactivated or weakly activated ketones such as indanone. A hypothetical scenario involving dimeric boronate species as chiral catalysts was also investigated.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Org Chem Año: 2024 Tipo del documento: Article País de afiliación: Francia Pais de publicación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Org Chem Año: 2024 Tipo del documento: Article País de afiliación: Francia Pais de publicación: Estados Unidos