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Reactividad controlada por el metal de un anión de radical naftílico de tipo pinza, coordinado por sigma
Christian M Frech1, Yehoshoa Ben-David, Lev Weiner
1Department of Organic Chemistry and Unit of Chemical Research Support, Weizmann Institute of Science, 76100 Rehovot, Israel.
Journal of the American Chemical Society
|June 1, 2006
Resumen
Un nuevo complejo de rodio-naftaleno fue reducido a un anión radical. Inesperadamente, este complejo reacciona con el agua para liberar gas hidrógeno, a diferencia de los aniones típicos de nafturo.
Área de la Ciencia:
- Química organometálica Química orgánica de los metales.
- Coordinación Química de la Coordinación
- Química Radical La Química Radical es una ciencia
Sus antecedentes:
- Los complejos de pinzas a base de naftaleno son valiosos en la química organometálica.
- Comprender la reactividad de los complejos de aniones radicales es crucial para desarrollar nuevos procesos catalíticos.
- El comportamiento de los aniones radicales naftídicos con los electrofilos está bien documentado.
Objetivo del estudio:
- Para sintetizar y caracterizar un nuevo complejo de pinzas a base de naftaleno.
- Para investigar la reducción y posterior reactividad de este complejo.
- Para comparar la reactividad del complejo reducido con los aniones conocidos de radicales naftídicos.
Principales métodos:
- Síntesis del complejo de pinzas basado en naftaleno [{C10H5{CH2PiPr2) }{Rh{eta1-N2}].
- Reducción utilizando metal de potasio para formar el complejo aniónico de radical naftílico coordinado sigma.
- Estudios de reoxidación utilizando el [Cp2Fe][BF4].
- Estudios de reactividad con agua en solución de THF.
Principales resultados:
- Síntesis exitosa del complejo de pinzas a base de naftaleno.
- Formación de un complejo de aniones radicales paramagnéticos, centrados en el anillo, tras la reducción con el metal potasio.
- Conservación de la integridad estructural y el estado formal de oxidación del metal durante la reducción.
- Reoxidación al complejo diamagnético inicial utilizando [Cp2Fe][BF4].
- Evolución inmediata inesperada de dihidrógeno y reoxidación al complejo inicial tras el tratamiento con agua.
- Reactividad distinta en comparación con la protonación en anillo conocida de aniones radicales naftídeos por agua.
Conclusiones:
- El complejo de pinzas reducido a base de naftaleno exhibe una reactividad única hacia el agua, que difiere significativamente de los aniones radicales simples de nafturo.
- Esta nueva reactividad ofrece nuevas vías para explorar la química de los sistemas radicales metal-ligando.
- El complejo sirve como modelo para el estudio de la transferencia de electrones y las subsiguientes transformaciones en la química organometálica.
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