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Factores que controlan la reducción catalítica de dos versus cuatro electrones del dioxígeno por complejos de cobre

Shunichi Fukuzumi¹, Laleh Tahsini, Yong-Min Lee

¹Department of Bioinspired Science, Ewha Womans University, Seoul 120-750, Korea. fukuzumi@chem.eng.osaka-u.ac.jp

Journal of the American Chemical Society

|April 3, 2012

Resumen

Un complejo de cobre binuclear cataliza eficientemente la reducción de dos electrones del oxígeno utilizando el decametilferroceno como reductor. Este proceso implica pasos de protonación y transferencia de electrones, que en última instancia producen peróxido de hidrógeno y regeneran el catalizador.

Área de la Ciencia:

Coordinación Química de la Coordinación
La catálisis de la catálisis.
Química bioorgánica Química bioorgánica.

Sus antecedentes:

La reducción de oxígeno es crucial en los sistemas biológicos y la catálisis.
Los derivados del ferroceno son eficaces reductores de un solo electrón.
Los complejos binucleares de cobre pueden imitar los sitios activos de las enzimas.

Objetivo del estudio:

Investigar el mecanismo catalítico de un complejo binuclear Cu (II) para la reducción de oxígeno.
Para aclarar el papel del ácido trifluoroacético en el ciclo catalítico.
Para identificar intermediarios y vías de reacción.

Principales métodos:

Análisis espectroscópico (UV-Vis) a bajas temperaturas.
Estudios cinéticos de las reacciones de transferencia de electrones.
Caracterización electroquímica de complejos de cobre.

Principales resultados:

El complejo binuclear Cu{II}, [Cu{II}{2}{LO}{OH}}{2+), cataliza la reducción de dos electrones de O{2) por el decametilferroceno (Fc*) en presencia del ácido trifluoroacético (HOTF).
La protonización del complejo por HOTF facilita la reducción por Fc*, procediendo a través de un mecanismo de transferencia de electrones en dos pasos.
En estudios a bajas temperaturas se identificaron peroxo ([Cu ((II) ((2) ((LO)) ((OO)))) e hidroperoxo ([Cu ((II) ((2) ((LO)) ((OOH)))) intermedios.
El ciclo catalítico produce H(2) O(2) y regenera el catalizador activo, [Cu(II) ((2) ((LO) ((OTF) ] ((2+).
El análisis cinético reveló dos vías de reacción distintas que implican la transferencia de electrones a un intermediario de dicopro de valencia mixta (II).

Conclusiones:

El complejo de cobre binuclear cataliza efectivamente la reducción de O(2) a H(2) O(2) utilizando Fc* como reductor.
El ácido trifluoroacético juega un papel clave en la activación del catalizador y la facilitación de la reacción.
El estudio proporciona información sobre el mecanismo de reducción de oxígeno por complejos de cobre, relevante para la química bioinorgánica y la catálisis.

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