Document Detail


Unexpected synthesis of conformationally restricted analogues of gamma-amino butyric acid (GABA): mechanism elucidation by electrospray ionization mass spectrometry.
MedLine Citation:
PMID:  15624912     Owner:  NLM     Status:  MEDLINE    
Abstract/OtherAbstract:
From previous results with lower homologues, dehydroiodination of the three alkenyl-beta-enamino esters 3a-c was expected to provide six-membered N-heterocyclic products. The reactions of 3a-c with triethylamine are found to lead, however, to the unexpected stereoselective synthesis of the trisubstituted cyclopentane derivatives 4a-c, as confirmed by IR and NMR spectroscopy. Cyclopentanes 4a-c bear two chiral centers and a gamma-amino ester moiety, and are therefore conformationally restricted analogues of gamma-amino butyric acid (GABA), which is the major inhibitory neurotransmitter in the central nervous system. Use of electrospray ionization mass (ESI-MS) and tandem mass spectrometry (ESI-MS/MS) allowed the key iminium ion intermediates 5a-c(+), as well as the protonated molecules of both the reactant and final products, [3a-c + H](+) and [4a-c + H](+), to be intercepted and structurally characterized. From these findings a mechanism for this unexpected but synthetically attractive and efficient stereoselective reaction is proposed.
Authors:
Helena M C Ferraz; Fernando L C Pereira; Erika R S Gonçalo; Leonardo S Santos; Marcos N Eberlin
Publication Detail:
Type:  Journal Article; Research Support, Non-U.S. Gov't    
Journal Detail:
Title:  The Journal of organic chemistry     Volume:  70     ISSN:  0022-3263     ISO Abbreviation:  J. Org. Chem.     Publication Date:  2005 Jan 
Date Detail:
Created Date:  2004-12-30     Completed Date:  2005-02-23     Revised Date:  2006-11-15    
Medline Journal Info:
Nlm Unique ID:  2985193R     Medline TA:  J Org Chem     Country:  United States    
Other Details:
Languages:  eng     Pagination:  110-4     Citation Subset:  IM    
Affiliation:
Institute of Chemistry, University of São Paulo-USP, São Paulo SP, 05508-900, Brazil. hmferraz@iq.usp.br
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MeSH Terms
Descriptor/Qualifier:
Combinatorial Chemistry Techniques
Cyclopentanes / chemical synthesis*
Molecular Structure
Spectrometry, Mass, Electrospray Ionization / methods*
Stereoisomerism
gamma-Aminobutyric Acid / analogs & derivatives*,  chemical synthesis*,  chemistry
Chemical
Reg. No./Substance:
0/Cyclopentanes; 56-12-2/gamma-Aminobutyric Acid

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