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Química de coordinación de estanilenos desiliados con metales de transición del grupo 10 d10: complejación de
Henning Arp1, Christoph Marschner, Judith Baumgartner
1Institut für Anorganische Chemie, Technische Universität Graz, Stremayrgasse 9, 8010 Graz, Austria.
Journal of the American Chemical Society
|May 1, 2013
Resumen
Los investigadores estudiaron cómo los estanilenos desiliados se coordinan con los metales del grupo 10. La formación del producto depende del metal, con el níquel formando complejos de estanileno y el paladio/platino formando complejos de silastaneno, influenciados por factores estéricos y electrónicos.
Área de la Ciencia:
- Química organometálica Química orgánica de los metales.
- Grupo Principal Química.
- Química computacional es la química computacional.
Sus antecedentes:
- Los estanilenos desiliados son ligandos versátiles en la química organometálica.
- Comprender su comportamiento de coordinación con los metales de transición es crucial para el diseño de catalizadores.
- Los metales del grupo cerovalente 10 (Ni, Pd, Pt) ofrecen diversos entornos electrónicos y estéricos.
Objetivo del estudio:
- Investigar la química de coordinación de los estanilenos desiliados con los complejos Ni(0), Pd(0 y Pt(0).
- Para aclarar los factores que rigen la formación de estanileno frente a los complejos de silastaneno.
- Para explorar la vía mecanicista de la reorganización de ligandos sobre la coordinación del metal.
Principales métodos:
- Síntesis y caracterización de los adductos PEt3 de estanilenos desiliados.
- Reacciones de estos aductos con los precursores de metales de transición del grupo 10 zerovalentes.
- Modelado computacional (DFT) para estudiar los mecanismos de reacción y la energética.
- Análisis de los efectos estéricos y electrónicos que influyen en la distribución del producto.
Principales resultados:
- El níquel formaba preferentemente complejos metálicos de estanileno.
- El paladio y el platino produjeron predominantemente complejos inusuales de silastaneno.
- Los estudios computacionales revelaron la formación inicial del complejo metálico estanileno seguido de una reorganización.
- La isomerización es un proceso de dos pasos con pequeñas barreras, lo que indica un control termodinámico.
- Los factores estéricos y electrónicos dictan la estabilidad relativa del estanileno frente a los isómeros del silastaneno.
Conclusiones:
- El comportamiento de coordinación de los estanilenos desiliados es altamente dependiente del metal del grupo 10.
- Una sutil interacción de efectos estéricos y electrónicos gobierna la selectividad observada del producto.
- El reordenamiento del estanileno al silastaneno es un evento posterior a la coordinación impulsado por la termodinámica.
- Los disililstanilenos cíclicos favorecen los complejos de silastaneno con Pd/Pt, mientras que los acíclicos favorecen los complejos de stanileno con Ni.
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