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Un germilón aislable y estabilizado por bisileno y su reactividad

Yuwen Wang¹, Miriam Karni², Shenglai Yao¹

¹Metalorganics and Inorganic Materials, Department of Chemistry , Technische Universität Berlin , Straße des 17, Juni 135, Sekr. C2 , 10623 Berlin , Germany.

Journal of the American Chemical Society

|December 1, 2018

Resumen

El primer complejo de germanio cerovalente, una "germylone", fue sintetizado y caracterizado. Este nuevo compuesto exhibe una reactividad única, formando adductos de Lewis y permitiendo la química frustrada del par de Lewis para la escisión de H2.

Área de la Ciencia:

Química organometálica
Química del grupo principal
Catálisis

Sus antecedentes:

Los complejos del grupo principal zerovalentes son raros y altamente reactivos.
La estabilización de especies de germanio de baja valencia presenta desafíos sintéticos significativos.
Comprender las propiedades electrónicas de tales complejos es crucial para predecir la reactividad.

Objetivo del estudio:

Para sintetizar y caracterizar el primer complejo de germanio cerovalente estable.
Para investigar la estructura electrónica y la unión de la germilona.
Explorar la reactividad de la germilona con los ácidos de Lewis y en aplicaciones catalíticas.

Principales métodos:

Síntesis del complejo de germanio cerovalente mediante desclorado.
Caracterización estructural y espectroscópica (por ejemplo, difracción de rayos X, RMN).
Cálculos de la Teoría Funcional de la Densidad (DFT) y análisis del Orbital de Enlace Natural (NBO).
Reacciones con los ácidos de Lewis (AlBr3, 9-BBN, BPh3) y los complejos de metales de transición (Ni ((cod) 2).

Principales resultados:

Síntesis exitosa del primer complejo de germanio cerovalente estable, [SiII ((Xant) SiII] Ge0.
El análisis de NBO reveló dos pares aislados en el átomo de germanio, lo que permitió la formación de un adducto de Lewis.
Se ha demostrado una reactividad inusual, incluida la formación de boril (silil) germileno y un ciclo metálico de Ge2Ni.
Formación de un par de Lewis frustrado (FLP) con BPh3, lo que facilita la escisión heterolítica de H2 a temperatura ambiente.

Conclusiones:

El germilón sintetizado es una especie estable y rica en electrones con una reactividad única.
Este trabajo amplía el alcance de la química de grupos principales de bajo valor.
La aplicación de la germilona en la química FLP abre nuevas vías para la activación de moléculas pequeñas.

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