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Los estados excitados altamente oxidantes de los complejos Re y Tc

Andrew S Del Negro¹, Carl J Seliskar, William R Heineman

¹Pacific Northwest National Laboratory, Richland, WA 99352, USA.

Journal of the American Chemical Society

|December 21, 2006

Resumen

Los complejos de tecnecio y renio [Tc(dmpe) 3 2+ y [Re(dmpe) 3 2+ exhiben luminiscencia y poseen potenciales de estado excitado excepcionalmente altos como oxidantes, alcanzables con luz visible.

Área de la Ciencia:

Química Inorgánica La Química Inorgánica es la química inorgánica.
La fotoquímica es la fotoquímica.
Coordinación Química de la Coordinación

Sus antecedentes:

La transferencia de carga de ligando a metal (LMCT) estados excitados de los complejos de metales de transición pueden exhibir propiedades fotofísicas únicas.
El bis-1,2-(dimetilfosfino) etano (dmpe) es un ligando de fosfina quelato utilizado en la química de la coordinación.

Objetivo del estudio:

Para investigar las propiedades fotofísicas y los potenciales de estado excitado de [Tc(dmpe) 3) 2+ y su análogo de renio.
Para determinar si estos complejos pueden funcionar como potentes oxidantes de estado excitado.

Principales métodos:

Espectroscopia de fotoluminiscencia para evaluar las propiedades de emisión.
Análisis de Rehm-Weller utilizando hidrocarburos aromáticos como apagadores de transferencia de electrones para determinar potenciales de estado excitado.
Mediciones electroquímicas para caracterizar los potenciales redox.

Principales resultados:

Tanto [Tc(dmpe) 3 2+ como [Re(dmpe) 3 2+ muestran luminiscencia en solución a temperatura ambiente.
Estos complejos poseen excepcionalmente altos potenciales de estado excitado (ESP) como oxidantes, entre los más altos para complejos de coordinación de metales de transición simples.
Las ESP son accesibles a través de la excitación de luz visible (lambdamax = 526 nm para Re, 585 nm para Tc).
La determinación experimental de E1/2 ((Re2+*/Re+) a través del análisis de Rehm-Weller (2.58 V) concuerda bien con los valores calculados.
Ambos complejos son apagados por los iones cloruro y funcionan como oxidantes de estado excitado en solución acuosa.

Conclusiones:

[Tc(dmpe) 3 2+ y su análogo Re son complejos de coordinación altamente luminiscentes con un notable poder oxidante en estado excitado.
Estos hallazgos resaltan el potencial de tales complejos en la catálisis fotorredóxica y otras aplicaciones que requieren fuertes oxidantes fotoactivados.

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