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De complejos de imido de hierro divalentes a pentavalentes y un nitruro de Fe (V) a través de la división de enlaces
Martin Keilwerth1, Weiqing Mao1, Sergio A V Jannuzzi2
1Department of Chemistry and Pharmacy, Inorganic Chemistry, Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU), Egerlandstraße 1, 91058 Erlangen, Germany.
Journal of the American Chemical Society
|December 30, 2022
Resumen
Los investigadores sintetizaron y caracterizaron complejos de imido de hierro utilizando un nuevo ligando, revelando diversas estructuras electrónicas y reactividades. Estos estudios proporcionan información sobre la química del hierro de valor medio a alto y las reacciones de transferencia de nitrógeno.
Área de la Ciencia:
- Química organometálica
- Química inorgánica
- Catálisis
Sus antecedentes:
- Los complejos de imido de hierro terminal son intermedios cruciales en las reacciones de transferencia de nitrógeno catalizadas por metales.
- El desarrollo de compuestos modelo versátiles es esencial para comprender su reactividad.
- El ligando quelante N-anclado tris-NHC, TIMMNMes, ofrece una nueva plataforma para sintetizar dichos complejos.
Objetivo del estudio:
- Sintetizar y comparar dos series de complejos de alquilo imido de hierro de valor medio a alto.
- Investigar las estructuras electrónicas y la reactividad de estos complejos.
- Explorar la conversión de los intermediarios de Fe ((V) imido en complejos de Fe ((V) nitrido.
Principales métodos:
- Síntesis de complejos de imido de hierro utilizando el ligando TIMMNMes y el azido de 1-adamantilo.
- Reducción química y oxidación paso a paso para acceder a complejos en los estados de oxidación II a V.
- Caracterización mediante difracción de rayos X de un solo cristal, magnetización SQUID, electroquímica, Mössbauer, IR, UV / vis, RMN, EPR y espectroscopia de absorción de rayos X.
- Los cálculos químicos cuánticos complementarios.
Principales resultados:
- Síntesis exitosa de series isostruturales de imidas de adamantilo de hierro de espín bajo [TIMMNMes) FeNAd) 0,1+,2+,3+ (2-5) en los estados de oxidación II a V.
- Observación de un intermediario inestable de Fe ((V) adamantil imido que se convierte en un complejo de nitrido de Fe ((V) aislable (6) a través de la escisión del enlace N-C.
- Síntesis de complejos de imido de etilo análogos, incluida una imida de etilo Fe ((V) estable, mediante la derivación del nitruro.
- Caracterización detallada que revela diversas estructuras electrónicas que se correlacionan con la reactividad.
Conclusiones:
- El ligando TIMMNMes facilita la síntesis de una variedad de complejos de imido y nitrido de hierro.
- Las estructuras electrónicas de los complejos de imido de hierro influyen significativamente en su reactividad.
- Este trabajo proporciona información valiosa sobre la química fundamental de los complejos de imido de hierro de alta valencia y su potencial en las reacciones de transferencia de nitrógeno.
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