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Control de la reactividad de fotoisomerización a través de sustituciones de grupo funcional único en complejos de
Gilbert K Kosgei1, Douglas J Breen1, Robert W Lamb2
1Department of Chemistry and Chemical Biology , 1 University of New Mexico , Albuquerque , New Mexico 87131 , United States.
Journal of the American Chemical Society
|July 27, 2018
Resumen
Los complejos de rutenio con nuevos ligandos de fosfina muestran una reactividad de fotoisomerización variada. Esto se debe a las diferencias en la donación de densidad de electrones y las propiedades del estado excitado, que afectan a sus aplicaciones potenciales.
Área de la Ciencia:
- Química organometálica
- La fotoquímica
- Ciencias de los materiales
Sus antecedentes:
- Los complejos de rutenio son vitales en la catálisis y la fotofísica.
- Los ligandos de trifenilfosfina son comunes en la química de la coordinación.
- Las fracciones de sulfóxido pueden ajustar las propiedades electrónicas.
Objetivo del estudio:
- Sintetizar y caracterizar nuevos complejos de rutenio con ligandos de trifenilfosfina funcionalizados con sulfóxido.
- Investigar el impacto de los para-sustitutos en las propiedades electrónicas de los ligandos.
- Para correlacionar las características estructurales y electrónicas con la reactividad de fotoisomerización.
Principales métodos:
- Cristalografía de rayos X para la determinación estructural.
- Espectroscopia de emisión para analizar las propiedades fotofísicas.
- Espectroscopia de bomba y sonda de femtosegundos para estudiar la dinámica del estado excitado.
- Cálculos de la teoría funcional de la densidad (DFT) para el análisis de la estructura electrónica.
Principales resultados:
- Se sintetizó una serie de complejos de rutenio con diferentes para-sustitutos (H, OCH3, CF3) en el ligando de la fosfina.
- Se observaron variaciones significativas en la reactividad de fotoisomerización en todas las series.
- Los cálculos de DFT revelaron diferencias en la donación de densidad de electrones del ligando de fosfina al rutenio.
- Se encontró que las propiedades del estado excitado son sensibles a las modificaciones del ligando.
Conclusiones:
- La reactividad de fotoisomerización de estos complejos de rutenio está fuertemente influenciada por las propiedades electrónicas de los ligandos de trifenilfosfina adheridos al sulfóxido.
- El diseño de ligandos, específicamente el para-sustituto, ofrece una herramienta poderosa para controlar el comportamiento del estado excitado y la reactividad en los complejos de rutenio.
- Estos hallazgos proporcionan información sobre el desarrollo de nuevos materiales y catalizadores fotorresponsivos.
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