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Una estrategia de microambiente supramolecular para la catálisis de metales de transición

David M Kaphan¹, Mark D Levin², Robert G Bergman³

¹Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA. Department of Chemistry, University of California, Berkeley, Berkeley, CA 94720, USA.

Science (New York, N.Y.)

|January 20, 2016

Resumen

Un nuevo complejo supramolecular imita las enzimas para catalizar las reacciones clave de formación de enlaces en metales de alta valencia. Este sistema catalítico logra aceleraciones de velocidad significativas y permite reacciones de acoplamiento cruzado catalítico dual.

Área de la Ciencia:

Química supramolecular
Catálisis
Química organometálica

Sus antecedentes:

La eliminación reductora alquilo-alquilo es un paso crucial en muchas transformaciones catalíticas.
Los complejos de metales de transición de alta valencia son sustratos importantes pero difíciles para la eliminación reductora.
La catálisis enzimática ofrece principios para el diseño de catalizadores sintéticos eficientes.

Objetivo del estudio:

Desarrollar un complejo supramolecular autoensamblado capaz de catalizar la eliminación reductora de alquilo-alquilo.
Para imitar entornos catalíticos enzimáticos para la reactividad no biológica.
Para investigar el mecanismo y la eficiencia de este catalizador supramolecular.

Principales métodos:

Síntesis de un complejo supramolecular auto-ensamblado.
Estudios cinéticos para determinar los mecanismos de reacción y las aceleraciones de la velocidad.
Aplicación del catalizador en una reacción de acoplamiento cruzado catalítico dual.

Principales resultados:

El complejo supramolecular cataliza efectivamente la eliminación reductora de alquilo-alquilo de los complejos de oro (III) y platino (IV).
Se identificó un mecanismo cinético de tipo Michaelis-Menten.
Las velocidades de aceleración (k ((cat) /k ((uncat)) alcanzaron hasta 1,9 × 10 ((7).
El catalizador se integró con éxito en una reacción de acoplamiento cruzado catalítico dual.

Conclusiones:

Los complejos supramoleculares autoensamblados pueden servir como imitaciones eficaces de enzimas para reacciones catalíticas desafiantes.
Este enfoque permite una catálisis eficiente de la eliminación reductora de alquilo-alquilo, un paso clave para la formación de enlaces.
El catalizador supramolecular facilita los efectos cooperativos en vías de reacción complejas como el acoplamiento cruzado catalítico dual.

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