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Unidades de construcción secundarias de hidróxido de titanio en marcos orgánicos metálicos catalizan la evolución del
Yang Song1, Zhe Li1,2, Yuanyuan Zhu1
1Department of Chemistry , The University of Chicago , 929 E 57th Street , Chicago , Illinois 60637 , United States.
Journal of the American Chemical Society
|July 25, 2019
Resumen
Desarrollamos nuevas estructuras de metal orgánico de titanio (MOF) dopadas con iridio o rutenio para una eficiente evolución de hidrógeno fotocatalítico. Estos MOF demuestran un alto rendimiento bajo luz visible, mostrando su potencial para aplicaciones de energía renovable.
Área de la Ciencia:
- Ciencias de los materiales
- Fotocatálisis
- Energía renovable
Sus antecedentes:
- Las estructuras metálicas orgánicas (MOF) ofrecen estructuras sintonizables para aplicaciones catalíticas.
- La evolución eficiente del hidrógeno fotocatalítico (HER, por sus siglas en inglés) es crucial para la producción sostenible de energía.
- Los MOF basados en titanio son candidatos prometedores para la fotocatálisis.
Objetivo del estudio:
- Diseñar y sintetizar nuevos MOF basados en titanio dopados con complejos de iridio y rutenio.
- Investigar la actividad fotocatalítica de evolución del hidrógeno de estos nuevos MOF bajo luz visible.
- Aclarar el mecanismo de la evolución del hidrógeno fotocatalítico y los factores que influyen en la eficiencia catalítica.
Principales métodos:
- Síntesis de Ti3-BPDC-Ir y Ti3-BPDC-Ru MOF mediante el dopaje de ligandos fotosensibilizantes en un marco de Ti3-BPDC.
- Experimentos de evolución del hidrógeno fotocatalítico bajo irradiación de luz visible.
- Caracterización fotofísica y electroquímica (por ejemplo, UV-Vis, fluorescencia, voltametría cíclica).
- Cálculos de la Teoría Funcional de la Densidad (DFT) para comprender los mecanismos de reacción.
Principales resultados:
- Los MOF Ti3-BPDC-Ir y Ti3-BPDC-Ru fueron sintetizados con éxito.
- Se lograron altas cifras de rotación para la evolución del hidrógeno fotocatalítico: 6632 para Ti3-BPDC-Ir y 786 para Ti3-BPDC-Ru.
- Los estudios fotofísicos y electroquímicos revelaron un mecanismo que involucra el apagado reductivo y la transferencia de electrones a las SBU de Ti3 ((OH) 2).
- Los cálculos de DFT identificaron los principales intermedios y vías de reacción, incluida la protonación de Ti (III) -OH y la transferencia de electrones acoplados a protones.
Conclusiones:
- Los MOF de titanio diseñados exhiben una excelente actividad fotocatalítica para la evolución del hidrógeno.
- El dopaje de fotosensibilizantes de iridio y rutenio mejora significativamente el rendimiento de HER.
- El estudio proporciona información mecanicista sobre el proceso fotocatalítico, orientando el diseño futuro de MOF para aplicaciones energéticas.
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