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Estructuras y reactividad de los complejos de Zr(IV) clorobenzeno

Fan Wu¹, Aswini K Dash, Richard F Jordan

¹Department of Chemistry, The University of Chicago, 5735 South Ellis Avenue, Chicago, IL 60637, USA.

Journal of the American Chemical Society

|November 26, 2004

Resumen

Este estudio detalla la síntesis y la reactividad de los complejos de zirconio. Los complejos estéricamente impedidos exhiben una activación térmica única de C-H, a diferencia de las contrapartes menos concurridas que son fotoquímicamente reactivas.

Área de la Ciencia:

Química organometálica Química orgánica de los metales.
Complejos de zirconio Complejos de zirconio
Coordinación Química de la Coordinación

Sus antecedentes:

Los complejos de circonoceno son catalizadores versátiles y intermedios sintéticos.
Comprender los efectos de los ligandos en la reactividad es crucial para el diseño del catalizador.
Los complejos de clorobenzeno presentan vías de reactividad únicas.

Objetivo del estudio:

Para sintetizar y caracterizar nuevos complejos de clorobenzeno de circonio.
Investigar la reactividad térmica y fotoquímica de estos complejos.
Para dilucidar la influencia del bulto estérico en las vías de reacción.

Principales métodos:

Síntesis de complejos de zirconio con diferentes ligandos de ciclopentadienilo.
Caracterización mediante técnicas espectroscópicas (NMR, cristalografía de rayos X).
Investigación de la reactividad en condiciones térmicas y fotoquímicas en el clorobenzeno.

Principales resultados:

Síntesis de los complejos de clorobenzeno [(C5R5) 2ZrR'(ClC6D5)][B(C6F5) 4].
Los complejos 1 y 2b,c mostraron conversión fotoquímica a dimeros de cloro-zirconio puenteados.
El complejo 2d, con ligandos Cp* estéricamente exigentes, se sometió a una fácil activación térmica orto-C-H.
Producto de activación de ortho-C-H reorganizado a través de la eliminación de beta-Cl y la inserción de benceno.

Conclusiones:

La inhibición estérica en los ligandos Cp* promueve la activación térmica orto-C-H en los complejos de clorobenzeno de zirconio.
Las vías fotoquímicas dominan para complejos menos obstaculizados.
Los hallazgos ofrecen información sobre los mecanismos de activación de C-H y los efectos de ligando en la química organometálica.

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