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Complejos sándwich invertidos de diníobio con ligandos μ-η6:η6-areno: síntesis, cinética de la formación y estructura

Thomas L Gianetti¹, Grégory Nocton, Stefan G Minasian

¹Department of Chemistry, University of California, Berkeley, California 94720, USA.

Journal of the American Chemical Society

|January 25, 2013

Resumen

Nuevos complejos de niobio-areno se convierten en estructuras sándwich invertidas de diniobium. Estos complejos únicos muestran una inusual estabilidad, pero pueden ser protonados, revelando información sobre el enlace niobio-areno.

Área de la Ciencia:

Química organometálica Química orgánica de los metales.
Química del niobio
Coordinación Química de la Coordinación

Sus antecedentes:

Los complejos de niobio con ligandos de areno son de interés por sus propiedades electrónicas únicas.
Comprender el enlace y la reactividad de estos complejos es crucial para desarrollar nuevos sistemas catalíticos.
Los complejos sandwich invertidos representan un motivo estructural distinto con un comportamiento químico potencialmente nuevo.

Objetivo del estudio:

Para sintetizar y caracterizar nuevos complejos monometálicos de niobio areno.
Para investigar la conversión de estos complejos en complejos sándwich de areno invertido de diniobio.
Para dilucidar la estructura electrónica y las interacciones de enlace dentro de estos sistemas de niobio-areno.

Principales métodos:

Síntesis de complejos monometálicos de niobio areno [Nb(BDI) ((N(t) Bu) ((R-C ((6) H ((5)) ].
Estudios cinéticos utilizando (1) espectroscopia de RMN H para monitorear la conversión a complejos de diniobium.
Caracterización mediante RMN, UV-vis, estructura de absorción de rayos X cercana al borde (XANES) y cristalografía de rayos X.

Principales resultados:

Los complejos monometálicos de niobio se convierten lentamente en complejos sándwich de areno invertido de diniobium a través de un mecanismo disociativo.
Los complejos de diniobium exhiben una inusual estabilidad hacia las moléculas pequeñas.
La protonación de los ligandos BDI produce complejos monoprotonados y dicationados estables.
Los datos espectroscópicos y estructurales indican una significativa donación de electrones de Nb d-orbital a arene del sistema π sin alterar el estado de oxidación formal de Nb.

Conclusiones:

El estudio sintetizó y caracterizó con éxito nuevos complejos sándwich invertidos de niobio areno y diniobium.
Los hallazgos proporcionan evidencia de una interacción de enlace única entre los ligandos de niobio y areno.
El perfil de estabilidad y reactividad de estos complejos ofrece nuevas vías para la investigación de la química organometálica.

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