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Efectos de la segunda esfera de coordinación en un complejo de Ru evolucionado basado en resultados de ligandos
Nataliia Vereshchuk1,2, Roc Matheu1, Jordi Benet-Buchholz1
1Institute of Chemical Research of Catalonia (ICIQ), Barcelona Institute of Science and Technology (BIST), Avda. Països Catalans 16, 43007 Tarragona, Spain.
Journal of the American Chemical Society
|February 12, 2020
Resumen
Un nuevo complejo de rutenio demuestra una catálisis de oxidación de agua notable, logrando frecuencias de rotación récord. Este avance se atribuye a los efectos intramoleculares de los grupos fosfonatos, que mejoran la eficiencia catalítica.
Área de la Ciencia:
- Química inorgánica
- Catálisis
- Ciencias de los materiales
Sus antecedentes:
- Los complejos de rutenio se investigan para aplicaciones catalíticas.
- La catálisis por oxidación del agua es crucial para las tecnologías de conversión de energía.
- El diseño de los ligandos juega un papel clave en el rendimiento del catalizador.
Objetivo del estudio:
- Para sintetizar y caracterizar un nuevo complejo de rutenio con un ligando de ácido difosfónico.
- Investigar la actividad catalítica del complejo de rutenio en la oxidación del agua.
- Aclarar el mecanismo de oxidación del agua y el papel del diseño del ligando.
Principales métodos:
- Síntesis y caracterización de complejos de rutenio mediante técnicas espectroscópicas y electroquímicas.
- Análisis de difracción de rayos X para la determinación estructural.
- Cálculos de la teoría funcional de la densidad (DFT) para conocimientos mecanicistas.
Principales resultados:
- Se sintetizó y caracterizó un nuevo complejo de rutenio [RuII ((H3tPa-κ-N3O) ((py) 2) + (2+).
- El complejo experimenta un comportamiento dinámico y forma un complejo de fenoxo-fosfonato Ru [RuIII(tPaO-κ-N2OPOC) ((py) 2) 2- (42-) en el estado de oxidación IV.
- El complejo 42- exhibe una catálisis de oxidación de agua excepcional con frecuencias de rotación récord (TOFmax) de 16.000 s-1.
Conclusiones:
- El complejo de rutenio 42 generado in situ es un catalizador de oxidación de agua altamente eficiente.
- Los efectos de la segunda esfera de coordinación intramolecular de los grupos de fosfonato son críticos para la catálisis.
- Este estudio ofrece información sobre el diseño de catalizadores avanzados para la oxidación del agua.
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