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Estudios mecanicistas de la reducción de O2 efectuada por complejos de hidruro bimetálico del grupo 9
Thomas S Teets1, Daniel G Nocera
1Department of Chemistry, 6-335, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139-4307, United States.
Journal of the American Chemical Society
|September 22, 2011
Resumen
Los estudios sintéticos y cinéticos revelan detalles mecánicos de la reducción de oxígeno al agua por complejos de dirhodium. Los intermediarios de peróxido e hidroperoxido son cruciales en este proceso, como lo demuestran los estudios sobre los complejos de dirhodium y diiridium.
Área de la Ciencia:
- Química Inorgánica La Química Inorgánica es la química inorgánica.
- Química organometálica Química orgánica de los metales.
- La catálisis de la catálisis.
Sus antecedentes:
- Los complejos de dirhodium son investigados por su papel en la reducción de oxígeno al agua.
- Comprender los mecanismos de estas reacciones es crucial para desarrollar sistemas catalíticos eficientes.
Objetivo del estudio:
- Para dilucidar las vías mecanicistas de la reducción de O(2) a agua mediada por complejos de dirhodium y diiridium.
- Identificar los principales intermediarios y pasos de reacción involucrados en el ciclo catalítico.
Principales métodos:
- Síntesis y caracterización de complejos de dirodio y diiridio de valencia mixta.
- Estudios de protonación para formar complejos hidruro.
- Investigaciones cinéticas de las reacciones con O(2) y HCl.
- Análisis espectroscópico y estructural de productos intermedios aislados.
Principales resultados:
- La protonación del complejo 1 de dirodio produjo el complejo 2 de hidruro de Rh (((2) ((II,II), que medió la reducción de O ((2).
- El complejo de diiridio 4 fue protonado para formar el complejo de hidruro aislable 5, que reaccionó con O(2) para formar el complejo de peróxido 6.
- El complejo 4 también formó un complejo η(2)-peróxido 7, que tras la protonación dio 6.
- Los estudios cinéticos apoyaron los mecanismos de eliminación de HCl para los sistemas de dirhodium y diiridium, con vías adicionales observadas para el dirhodium.
Conclusiones:
- Los intermediarios de peróxido e hidroperoxido juegan un papel importante en la reducción de O ((2) a agua por complejos de hidruro de dirodio.
- Las vías mecanicistas incluyen la eliminación de HCl, la inserción directa de O2 y la isomerización unimolecular.
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