DFT study on the cycloreversion of thietane radical cations

The molecular mechanism of the cycloreversion (CR) of thietane radical cations has been analyzed in detail at the UB3LYP/6-31G* level of theory. Results have shown that the process takes place via a stepwise mechanism leading to alkenes and thiobenzophenone; alternatively, formal [4 + 2] cycloadduct...

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Detalles Bibliográficos
Autores: Domingo, Luis R., Pérez-Ruiz, Rauíl, Argüello, Juan Elias, Miranda, Miguel A.
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2011
País:Argentina
Institución:Consejo Nacional de Investigaciones Científicas y Técnicas
Repositorio:CONICET Digital (CONICET)
Idioma:inglés
OAI Identifier:oai:ri.conicet.gov.ar:11336/65854
Acceso en línea:http://hdl.handle.net/11336/65854
Access Level:acceso abierto
Palabra clave:Radical Cation
Ciclorevesion
Dft Calculation
Thietane
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
Descripción
Sumario:The molecular mechanism of the cycloreversion (CR) of thietane radical cations has been analyzed in detail at the UB3LYP/6-31G* level of theory. Results have shown that the process takes place via a stepwise mechanism leading to alkenes and thiobenzophenone; alternatively, formal [4 + 2] cycloadducts are obtained. Thus, the CR of radical cations 1a,b •+ is initiated by C2-C3 bond breaking, giving common intermediates INa,b. At this stage, two reaction pathways are feasible involving ion molecule complexes IMCa,b (i) or radical cations 4a,b •+ (ii). Calculations support that 1a •+ follows reaction pathway ii (leading to the formal [4 + 2] cycloadducts 5a). By contrast, 1b •+ follows pathway i, leading to trans-stilbene radical cation (2b •+) and thiobenzophenone. © 2011 American Chemical Society.