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Dimeros mono-μ-oxo de iridio de alto estado de oxidación relacionados con la catálisis de la oxidación del agua

Liam S Sharninghausen¹, Shashi Bhushan Sinha¹, Dimitar Y Shopov¹

¹Department of Chemistry, Yale University , New Haven, Connecticut 06520, United States.

Journal of the American Chemical Society

|December 15, 2016

Resumen

Los investigadores desarrollaron dimeros de iridio bien definidos, ClL2Ir-O-IrL2Cl, para estudiar el catalizador de oxidación de agua de la "solución azul". Estos compuestos estructuralmente caracterizados proporcionan información sobre la catálisis basada en iridio sin enlaces metal-carbono.

Área de la Ciencia:

Química inorgánica
Ciencias de la catálisis
Ciencias de los materiales

Sus antecedentes:

El catalizador de oxidación de agua de "solución azul" de iridio altamente activo es difícil de caracterizar debido a la presencia de múltiples isómeros geométricos y pérdida de ligando.
Estudios anteriores sugieren la formación de una unidad LIr-O-IrL, pero una estructura cristalina definitiva sigue siendo difícil de alcanzar.

Objetivo del estudio:

Sintetizar y caracterizar compuestos modelo bien definidos que imiten aspectos del catalizador de la "solución azul".
Para aclarar la estructura y las propiedades de los dimeros dinucleares μ-oxo iridio ((IV,IV) sin enlaces metal-carbono.

Principales métodos:

Síntesis de dimeros de iridio ((IV,IV) mono-μ-oxo con la fórmula ClL2Ir-O-IrL2Cl.
Separación y purificación mediante cromatografía en gel de sílice.
Caracterización completa, incluida la cristalografía de rayos X.

Principales resultados:

Síntesis exitosa de tres estereoisómeros de ClL2Ir-O-IrL2Cl.
Estos compuestos modelo están caracterizados cristalográficamente, a diferencia del catalizador original.
El estudio informa de los primeros compuestos dinucleares μ-oxo Ir ((IV,IV) caracterizados estructuralmente que carecen de enlaces metal-carbono.

Conclusiones:

Los dimeros de iridio desarrollados sirven como modelos valiosos para comprender el catalizador de la "solución azul".
La caracterización estructural proporciona información crucial sobre la naturaleza de las especies de iridio-oxo en la catálisis.
Este trabajo abre nuevas vías para el diseño de catalizadores avanzados de oxidación de agua a base de iridio.

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