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Complejos moleculares con enlaces de aluminio-cobre y de galio-cobre mejorados por dispersión sin soporte
Kristian L Mears1, Cary R Stennett2, Elina K Taskinen3
1Materials Chemistry Centre, Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, United Kingdom.
Journal of the American Chemical Society
|November 10, 2020
Resumen
Se sintetizaron nuevos complejos de cobre con enlaces de cobre-aluminio y cobre-gallio sin soporte. Los cálculos de la teoría funcional de la densidad revelaron que las fuerzas de dispersión de Londres contribuyen significativamente a su estabilidad.
Área de la Ciencia:
- Química de coordinación
- Química organometálica
- Química del grupo principal
Sus antecedentes:
- Los complejos de cobre (I) con ligandos β-diketiminados son precursores versátiles en la síntesis inorgánica.
- Los complejos metálicos del grupo 13 de baja valencia (por ejemplo, aluminio, galio) con ligandos β-diketiminados ofrecen una reactividad única.
- La formación de enlaces metal-metal sin soporte es un desafío significativo en la química inorgánica.
Objetivo del estudio:
- Para sintetizar nuevos complejos metálicos del grupo 13 de cobre con enlaces entre metales sin soporte.
- Caracterizar las propiedades estructurales y electrónicas de estos nuevos compuestos.
- Investigar las contribuciones de enlace que estabilizan estas interacciones únicas entre metales.
Principales métodos:
- Reacción de un complejo de cobre ((I) β-diketiminato con complejos de aluminio y galio β-diketiminato de baja valencia en tolueno.
- Aislamiento y caracterización de los complejos cobre-aluminio y cobre-gallio resultantes.
- Difracción de rayos X monocristalino para determinar las estructuras moleculares y las distancias de enlace metal-metal.
- Cálculos de la teoría funcional de la densidad (DFT) para analizar el enlace y la energética.
Principales resultados:
- Síntesis exitosa de los complejos CuAl y Dip.
- Estos complejos exhiben enlaces de cobre-aluminio y cobre-gallio sin soporte con distancias metal-metal cortas (Cu-Al = 2.3010 ((6) Å, Cu-Ga = 2.2916 ((5) Å).
- Los cálculos de DFT indican que las fuerzas de dispersión de Londres representan aproximadamente el 50% de las entalpias de asociación calculadas.
Conclusiones:
- El estudio demuestra la viabilidad de formar enlaces Cu-Al y Cu-Ga no soportados utilizando ligandos β-diketiminados.
- Las distancias cortas entre metales sugieren interacciones de enlace significativas.
- Las fuerzas de dispersión de Londres juegan un papel crucial en la estabilización de estos nuevos compuestos organometálicos.
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