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Reactividad anómala del nitrato de ceráceo en el rutenio "dimer azul" catalizado por la oxidación del agua

Jamie A Stull¹, R David Britt, Jeanne L McHale

¹Department of Chemistry, University of California-Davis, Davis, California 95616, United States.

Journal of the American Chemical Society

|November 28, 2012

Resumen

Los iones de nitrato aceleran la oxidación del agua catalizada por el rutenio "dímero azul", formando un intermedio único. El etiquetado isotópico confirmó que este intermediario implica un átomo de oxígeno coordinado Ru, no una especie peroxo.

Área de la Ciencia:

Química Inorgánica La Química Inorgánica es la química inorgánica.
La catálisis de la catálisis.
La espectroscopia es una técnica de espectroscopia.

Sus antecedentes:

Los complejos de rutenio se investigan para la catálisis de la oxidación del agua.
Comprender los intermediarios de reacción es crucial para la optimización del catalizador.

Objetivo del estudio:

Para investigar el efecto de los iones nitrato en la oxidación del agua mediada por Ce (IV) por un rutenio "dimer azul".
Para caracterizar el único intermediario de reacción formado en presencia de nitrato.

Principales métodos:

Utilizó la Resonancia Paramagnética de Electrones (EPR), la espectroscopia óptica y la espectroscopia de resonancia Raman (RR).
Se emplean materiales etiquetados isotópicamente ((18) O y (15) N) para dilucidar los mecanismos de reacción.

Principales resultados:

Las altas concentraciones de nitrato aumentaron la tasa de oxidación y condujeron a un intermedio único.
El intermedio exhibió características espectrales distintas, incluida una banda de RR sensible a los isótopos de oxígeno.
El etiquetado isotópico reveló que la banda involucra un oxígeno coordinado Ru, no un enlace peroxo.
El análisis del producto oxígeno excluyó los átomos de oxígeno derivados del nitrato, descartando ciertas vías propuestas.

Conclusiones:

Los iones nitrato alteran significativamente el mecanismo de oxidación del agua del rutenio "dimer azul".
Es probable que los complejos cerico-nitrato sean responsables de generar el intermediario observado.
Los hallazgos proporcionan nuevos conocimientos sobre la catálisis de la oxidación del agua y la formación de intermedios.

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