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La hidrogenación catalizada por protones de un complejo d(8) Ir(I) da como resultado un dihidruro trans Ir(III)

Michael Findlater¹, Wesley H Bernskoetter, Maurice Brookhart

¹Department of Chemistry, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599-3290, USA.

Journal of the American Chemical Society

|March 18, 2010

Resumen

Este estudio revela una nueva vía para la hidrogenación del iridio, formando un complejo de trans-dihidruro a través de la escisión catalizada por protones H(2), evitando los típicos intermediarios cis-dihidruro.

Área de la Ciencia:

Química organometálica Química orgánica de los metales.
La catálisis de la catálisis.
Coordinación Química de la Coordinación

Sus antecedentes:

Los complejos de iridio son cruciales en la catálisis.
Comprender los mecanismos de hidrogenación es clave para desarrollar nuevas rutas sintéticas.
El complejo (PONOP) Ir(I) CH(3) sirve como sistema modelo.

Objetivo del estudio:

Para dilucidar el mecanismo de hidrogenación para el complejo (PONOP) Ir (I) CH (III).
Para investigar la formación de especies inesperadas de trans-dihidruro.
Para explorar vías de reacción alternativas en la hidrogenación catalizada por iridio.

Principales métodos:

Síntesis a baja temperatura de los intermediarios de reacción.
Caracterización espectroscópica (por ejemplo, RMN, IR).
Estudios mecanicistas que involucran el etiquetado isotópico y el análisis cinético.

Principales resultados:

La hidrogenación de (PONOP) Ir(I) CH(3) inesperadamente da lugar a una especie de trans-dihidruro.
La reacción procede a través de una escisión de H2 catalizada por protones.
Se identificaron y confirmaron los intermediarios clave, incluido un complejo de iridio catiónico y un complejo eta(2) -H(2).

Conclusiones:

Se ha descubierto para los complejos de iridio una nueva vía catalítica que involucra la escisión catalizada por protones de H2O.
Este mecanismo evita la formación de productos intermedios cis-dihidruro, ofreciendo nuevos conocimientos sobre las reacciones de hidrogenación.
Los hallazgos proporcionan una base para el diseño de catalizadores basados en iridio más eficientes.

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