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Un complejo reactivo de manganeso ((IV) -hidróxido: un intermediario que falta en la transferencia de átomos de

Jan Paulo T Zaragoza¹, Maxime A Siegler¹, David P Goldberg¹

¹Department of Chemistry , The Johns Hopkins University , 3400 North Charles Street , Baltimore , Maryland 21218 , United States.

Journal of the American Chemical Society

|March 16, 2018

Resumen

Este estudio sintetiza un raro complejo de hidróxido de manganeso, demostrando sus potentes capacidades de abstracción de átomos de hidrógeno. Esta especie de hidróxido de manganeso es un extractor de átomos de H significativamente más fuerte que los complejos de óxido de manganeso.

Área de la Ciencia:

Química inorgánica
Química bioorgánica
Catálisis

Sus antecedentes:

Las especies de hidróxido metálico de alta valencia son intermedios clave en la activación y producción de O2.
Los complejos mononucleares M ((IV) ((OH) bien caracterizados son escasos, lo que limita la comprensión mecánica.

Objetivo del estudio:

Sintetizar y caracterizar un nuevo complejo mononuclear de hidróxido de manganeso.
Investigar la reactividad y las capacidades de abstracción de átomos de H de este complejo en comparación con las especies relacionadas con el manganeso.

Principales métodos:

Síntesis y caracterización por difracción de rayos X de complejos de manganeso.
Estudios cinéticos de la abstracción del átomo H de los fenoles mediante espectroscopia UV-Vis.
Mediciones del efecto isotópico cinético (KIE).

Principales resultados:

Se sintetizó con éxito y se caracterizó estructuralmente el Mn (IV) (OH) (ttppc) utilizando un ligando de corrol estérico exigente.
Mn ((IV) ((OH) ((ttppc) exhibió una reactividad significativamente mayor (k2 ≈ 2.73 × 10 ^ 4 M ^ - 1 s ^ - 1) en la abstracción de átomos de H que Mn ((V) ((O) ((ttppc).
Las correlaciones de los fenoles sustituidos y los datos KIE confirmaron un mecanismo concertado de transferencia de átomos de H (HAT).

Conclusiones:

El complejo estérico de Mn ((IV) ((OH) es un extractor de átomos de H raro y potente.
El complejo Mn ((IV) ((OH) supera a los complejos Mn ((V) ((O) y algunos complejos Fe ((IV) ((O) de mayor valor en la abstracción de átomos de H.
Este trabajo proporciona información crucial sobre los mecanismos de escisión de enlaces OH mediados por complejos metálicos de alta valencia.

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