Stereoselectivity induced by support confinement effects. Aza-pyridinoxazolines: A new family of C1-symmetric ligands for copper-catalyzed enantioselective cyclopropanation reactions
- García, J.I. 1
- Jiménez-Osés, G. 1
- López-Sánchez, B. 1
- Mayoral, J.A. 1
- Vélez, Andrea . 1
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1
Universidad de Zaragoza
info
ISSN: 1477-9226
Año de publicación: 2010
Volumen: 39
Número: 8
Páginas: 2098-2107
Tipo: Artículo
beta Ver similares en nube de resultadosOtras publicaciones en: Dalton Transactions
Resumen
Aza-pyridinoxazoline ligands, a new class of C1-symmetric ligands, are described and tested in the heterogeneous enantioselective catalysis of a cyclopropanation reaction, with the aim of improving surface confinement effects by the clay support on the reaction stereoselectivity. In the case of trans/cis diastereoselectivity, these surface effects lead to a systematic reversal of selectivity, cis-cyclopropanes being favored. Regarding the enantioselectivities, support confinement has a positive effect in the case of major cis-cyclopropane products, leading to moderate enantioselectivity values (60% ee). A theoretical (DFT) mechanistic study is carried out to explain the origin of the enantioselectivity in the homogeneous phase at a molecular level, and to get insights on the geometries of the key intermediates and transition structures. © 2010 The Royal Society of Chemistry.