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[(DPEPhos)(bcp)Cu]PF6: A General and Broadly Applicable Copper-Based Photoredox Catalyst
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Activación rápida del enlace C-H por un complejo de monocopio (III) -hidróxido.

Patrick J Donoghue1, Jacqui Tehranchi, Christopher J Cramer

  • 1Department of Chemistry, Center for Metals in Biocatalysis, and Supercomputing Institute, University of Minnesota, 207 Pleasant Street SE, Minneapolis, Minnesota 55455, United States.

Journal of the American Chemical Society
|October 19, 2011
PubMed
Resumen

Los investigadores generaron un intermediario reactivo de cobre (III) -hidróxido (LCuOH) a través de la oxidación de un electrón. Este complejo Cu (III) abstrae eficazmente los átomos de hidrógeno, lo que sugiere su potencial papel en la catálisis de la oxidación.

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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 cobre son ampliamente estudiados por sus propiedades catalíticas.
  • Comprender los estados de oxidación y la reactividad del cobre es crucial para diseñar catalizadores eficientes.
  • La generación y caracterización de especies de cobre de alta valencia sigue siendo un área activa de investigación.

Objetivo del estudio:

  • Para sintetizar y caracterizar un nuevo complejo de cobre (III) -hidróxido.
  • Para investigar la reactividad de este cobre (III) intermedio en las reacciones de oxidación.
  • Para dilucidar el mecanismo de la abstracción del átomo de hidrógeno por el cobre (III) complejo.

Principales métodos:

  • Oxidación de un electrón de un complejo Cu(II) tetragonal ([Bu(4) N][LCuOH]) a baja temperatura (-80 °C).
  • Análisis espectroscópicos y teóricos para confirmar la formación e identidad del intermediario Cu(III) (LCuOH).
  • Estudios cinéticos de la reacción con dihidroantraceno, incluidas las mediciones del efecto del isótopo cinético.

Principales resultados:

  • El reactivo intermedio LCuOH fue generado con éxito e identificado como un complejo Cu (III).
  • El LCuOH reaccionó con el dihidroantraceno para producir antraceno y un complejo Cu(II) (LCu(OH(2))).
  • Los estudios cinéticos revelaron una ley de velocidad de segundo orden para la abstracción del átomo H con efectos de isótopos cinéticos significativos (k ((H) / k ((D) = 44 a -70 °C).

Conclusiones:

  • Una fracción Cu(III) -OH puede funcionar como una especie reactiva en reacciones de oxidación.
  • Los hallazgos apoyan la viabilidad del Cu (III) -OH como un intermediario clave en los procesos de oxidación catalizados por el cobre.
  • Este estudio proporciona información sobre la reactividad fundamental de las especies de cobre de alta valencia.