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[{Cyclen}{4}Ru{4}{pz}{4}}{9}+): un cuadrado de Creutz-Taube en el centro
Victor C Lau1, Louise A Berben, Jeffrey R Long
1Department of Chemistry, University of California, Berkeley, California 94720-1460, USA.
Journal of the American Chemical Society
|August 1, 2002
Resumen
Los investigadores ensamblaron un complejo cuadrado de valencia mixta utilizando cicleno (1,4,7,10-tetraazaciclododecano) y ligandos de pirazina. Este complejo exhibe una deslocalización significativa de electrones, que excede a la del ion Creutz-Taube, como lo confirman los estudios electroquímicos.
Área de la Ciencia:
- Coordinación Química de la Coordinación
- Química supramolecular de las moléculas.
- La electroquímica es electroquímica.
Sus antecedentes:
- Los complejos metálicos de valencia mixta son cruciales para comprender los procesos de transferencia de electrones.
- El ligando cicleno (1,4,7,10-tetraazaciclododecano) es eficaz en la estabilización de ensamblajes metálicos multinucleares discretos.
- Los complejos de rutenio con puentes de pirazina han sido ampliamente estudiados por sus propiedades electrónicas.
Objetivo del estudio:
- Para sintetizar y caracterizar un nuevo complejo cuadrado de valencia mixta de rutenio.
- Para investigar la comunicación electrónica y la deslocalización de electrones dentro del complejo.
- Para comparar la deslocalización de electrones en este complejo con los sistemas de referencia existentes como el ion de Creutz-Taube.
Principales métodos:
- Ensamblaje del complejo cuadrado de valencia mixta utilizando ligandos de cicleno y pirazina.
- Determinación de la estructura cristalina para dilucidar la geometría molecular y el entorno de coordinación.
- Voltametría cíclica para sondear el comportamiento redox y determinar las constantes de comproporción.
Principales resultados:
- Se sintetizó y caracterizó estructuralmente con éxito un complejo cuadrado regular, [(cicleno) 4Ru4(pz) 4 9 +.
- El análisis electroquímico reveló ondas redox distintas correspondientes a los estados de valencia mixta.
- La constante de comproporción (Kc = 108.9) indicó una extensa deslocalización de electrones, mayor que en el ion de Creutz-Taube.
Conclusiones:
- El complejo cuadrado basado en ciclenos demuestra una significativa comunicación electrónica entre los centros de rutenio.
- La deslocalización de electrones observada es altamente dependiente del estado de oxidación del complejo.
- Este estudio proporciona información sobre los principios de diseño para complejos metálicos multinucleares con propiedades electrónicas sintonizables.
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