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Inyección de electrones desde los ligandos de marco metálico orgánico fotoexcitados a las unidades de construcción
Guangxu Lan1, Yuan-Yuan Zhu1,2, Samuel S Veroneau1
1Department of Chemistry , The University of Chicago , 929 E 57th Street , Chicago , Illinois 60637 , United States.
Journal of the American Chemical Society
|March 27, 2018
Resumen
Diseñamos nuevos marcos metal-orgánicos (MOF) para una eficiente evolución del hidrógeno impulsado por la luz visible. Estos MOF utilizan unidades de construcción secundarias basadas en rutenio y ligandos de porfirina para una fotocatálisis mejorada en agua neutra.
Área de la Ciencia:
- Ciencias de los materiales
- Fotocatálisis
- Química supramolecular
Sus antecedentes:
- Las estructuras orgánicas metálicas (MOF) son materiales prometedores para la catálisis.
- El desarrollo de fotocatalizadores eficientes para la reacción de evolución del hidrógeno (HER) es crucial para la energía sostenible.
- El diseño de MOF con unidades de recolección de luz y catalíticas integradas es un área de investigación activa.
Objetivo del estudio:
- Diseñar y sintetizar nuevos MOF que incorporen unidades de construcción secundarias Ru2 (SBU) y ligandos de porfirina.
- Investigar el mecanismo de la reacción de evolución del hidrógeno impulsada por la luz visible (HER) en estos nuevos MOF.
- Establecer una nueva estrategia para la construcción de MOF multifuncionales para la fotocatálisis.
Principales métodos:
- Síntesis de Ru-TBP y Ru-TBP-Zn MOF.
- Caracterización fotofísica (por ejemplo, absorción, emisión, mediciones durante la vida útil).
- Estudios electroquímicos (por ejemplo, voltametría cíclica, espectroelectroquímica) para sondear los mecanismos de reacción.
Principales resultados:
- Diseño y síntesis exitosos de dos nuevos MOF, Ru-TBP y Ru-TBP-Zn.
- Se ha demostrado la eficacia del HER impulsado por luz visible en agua neutra.
- Identificó el apagado oxidativo de las porfirinas excitadas por Ru2 SBU como el paso inicial, facilitando la transferencia de múltiples electrones.
- Elucidado la energética de los intermedios clave en el ciclo catalítico.
Conclusiones:
- La proximidad de las SBU de Ru2 y los ligandos de porfirina en los MOF diseñados permite una HER fotocatalítica eficiente.
- El mecanismo de apagado oxidativo es clave para la alta actividad observada.
- Este trabajo presenta una estrategia viable para crear MOF sinérgicos para la fotocatálisis avanzada.
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