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Origin of the synchronicity in bond formation in polar Diels-Alder reactions: an ELF analysis of the reaction between cyclopentadiene and tetracyanoethylene.
MedLine Citation:
PMID:  22527420     Owner:  NLM     Status:  In-Data-Review    
Abstract/OtherAbstract:
The origin of the synchronicity in C-C bond formation in polar Diels-Alder (P-DA) reactions involving symmetrically substituted electrophilic ethylenes has been studied by an ELF analysis of the electron reorganization along the P-DA reaction of cyclopentadiene (Cp) with tetracyanoethylene (TCE) at the B3LYP/6-31G* level. The present study makes it possible to establish that the synchronicity in C-C bond formation in P-DA reactions is controlled by the symmetric distribution of the electron-density excess reached in the electrophile through the charge transfer process, which can be anticipated by an analysis of the spin electron-density at the corresponding radical anion. The ELF comparative analysis of bonding along the DA reactions of Cp with ethylene and with TCE asserts that these DA reactions, which have a symmetric electron reorganization, do not have a cyclic electron reorganization as the pericyclic mechanism states. Due to the very limited number of cases of symmetrically substituted ethylenes, we can conclude that the synchronous mechanism is an exception of DA reactions.
Authors:
Luis R Domingo; Patricia Pérez; Jose A Sáez
Publication Detail:
Type:  Journal Article    
Journal Detail:
Title:  Organic & biomolecular chemistry     Volume:  10     ISSN:  1477-0539     ISO Abbreviation:  Org. Biomol. Chem.     Publication Date:  2012 Apr 
Date Detail:
Created Date:  2012-04-24     Completed Date:  -     Revised Date:  -    
Medline Journal Info:
Nlm Unique ID:  101154995     Medline TA:  Org Biomol Chem     Country:  England    
Other Details:
Languages:  eng     Pagination:  3841-51     Citation Subset:  IM    
Affiliation:
Universidad de Valencia, Departamento de Química Orgánica, Dr. Moliner 50, E-46100 Burjassot, Valencia, Spain. domingo@utopia.uv.es.
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