Stereoselective synthesis of 1,3-diaminotruxillic acid derivatives: an advantageous combination of C-H-ortho-palladation and on-flow [2+2]-photocycloaddition in microreactors

The stereoselective synthesis of ε-isomers of dimethyl esters of 1,3-diaminotruxillic acid in three steps is reported. The first step is the ortho-palladation of (Z)-2-aryl-4-aryliden-5(4H)-oxazolones 1 to give dinuclear complexes 2 with bridging carboxylates. The reaction occurs through regioselect...

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Bibliographic Details
Authors: Serrano, Elena, Juan, Alberto, García-Montero, Ángel, Soler, Tatiana, Jiménez-Márquez, Francisco, Cativiela, Carlos, Gómez, M. Victoria, Urriolabeitia, Esteban P.
Format: article
Status:Versión aceptada para publicación
Publication Date:2016
Country:España
Institution:Consejo Superior de Investigaciones Científicas (CSIC)
Repository:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/155773
Online Access:http://hdl.handle.net/10261/155773
Access Level:Open access
Keyword:C-H activation
Photochemistry
Palladium
Microreactors
Lactones
Description
Summary:The stereoselective synthesis of ε-isomers of dimethyl esters of 1,3-diaminotruxillic acid in three steps is reported. The first step is the ortho-palladation of (Z)-2-aryl-4-aryliden-5(4H)-oxazolones 1 to give dinuclear complexes 2 with bridging carboxylates. The reaction occurs through regioselective activation of the ortho-C-H bond of the 4-arylidene ring in carboxylic acids. The second step is the [2+2]-photocycloaddition of the C-C exocyclic bonds of the oxazolone skeleton in 2 to afford the corresponding dinuclear ortho-palladated cyclobutanes 3. This key step was performed very efficiently by using LED light sources with different wavelengths (465, 525 or 625 nm) in flow microreactors. The final step involved the depalladation of 3 by hydrogenation in methanol to afford the ε-1,3-diaminotruxillic acid derivatives as single isomers.