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Un catalizador molecular de hierro para la deshidrogenación y hidrogenación sin aceptor de N-heterociclos

Sumit Chakraborty¹, William W Brennessel, William D Jones

¹Department of Chemistry, University of Rochester , Rochester, New York 14627, United States.

Journal of the American Chemical Society

|June 1, 2014

Resumen

Un complejo de pinzas de hierro cataliza eficientemente la deshidrogenación y la hidrogenación del N-heterociclo. El catalizador es el catalizador.

Área de la Ciencia:

Química organometálica de las sustancias orgánicas.
La catálisis es la catálisis.
La síntesis orgánica es la síntesis orgánica.

Sus antecedentes:

Los N-heterociclos son importantes motivos estructurales en productos farmacéuticos y materiales.
Los métodos catalíticos eficientes para su transformación son muy buscados.
Los ligandos de pinza ofrecen propiedades electrónicas y estéricas únicas para el diseño de catalizadores.

Objetivo del estudio:

Desarrollar un nuevo complejo de hierro para transformaciones catalíticas de N-heterociclo.
Para investigar la actividad catalítica en las reacciones de deshidrogenación e hidrogenación.
Para aclarar el mecanismo del ciclo catalítico.

Principales métodos:

Síntesis y caracterización de un complejo de pinzas de hierro bis ((phosphino) amínico (3).
Evaluación de la actividad catalítica en la deshidrogenación y hidrogenación sin aceptor de los N-heterociclos.
Cristalografía de rayos X para determinar la estructura del complejo de hierro activo.
Espectroscopia de RMN y experimentos de captura para identificar intermediarios de reacción.

Principales resultados:

El complejo 3 cataliza eficientemente la deshidrogenación sin aceptor de los N-heterociclos en buenos rendimientos.
El complejo 3 también cataliza la hidrogenación de los N-heterociclos.
La especie catalítica activa fue sintetizada, caracterizada y su estructura confirmada.
Se propuso un intermedio trans-dihidruro (4) y se verificó su existencia.

Conclusiones:

Un bien definido complejo de pinzas de hierro es un catalizador eficaz para la deshidrogenación y hidrogenación del N-heterociclo.
El mecanismo catalítico probablemente involucra un intermediario trans-dihidruro.
Este trabajo proporciona un nuevo sistema catalítico para transformaciones orgánicas valiosas.

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