Stereodivergent Carbamate Synthesis by Selective In Situ Trapping of Organic Carbonate Intermediates

Trans-carbamate structures can be prepared in a diastereoselective approach by a judicious one-pot combination of in situ prepared organic carbonates and suitable amine reagents under appropriate reaction conditions. This unprecedented approach allows for stereo-divergence from a single oxirane subs...

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Detalles Bibliográficos
Autores: Guo, Wusheng, Laserna, Victor, Martin, Eddy, Escudero-Adán, Eduardo C., Kleij, Arjan W.
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2016
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:2072/356074
Acceso en línea:http://hdl.handle.net/2072/356074
https://doi.org/10.1002/chem.201504510
Access Level:acceso abierto
Palabra clave:54
Descripción
Sumario:Trans-carbamate structures can be prepared in a diastereoselective approach by a judicious one-pot combination of in situ prepared organic carbonates and suitable amine reagents under appropriate reaction conditions. This unprecedented approach allows for stereo-divergence from a single oxirane substrate with easy access to both cis and trans carbamate isomers with high stereo- selectivity (dr > 19:1). Key to control the diastereo-selective nature of the conversions leading to the trans carbamates is the in situ formation of trans-configured oligo/polycarbonates through Al- catalysis providing the targeted products after aminolysis. The present results demonstrate the valorization of a renewable carbon-based reagent (CO2) into new valuable scaffolds and an unusual stereo- control exerted through carbonate intermediates. A series of control experiments support the proposed mechanistic rationale towards the trans-carbamate products which is based on the trapping of an in situ formed trans-configured oligo/polycarbonate.