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Ferroceno binario inducido magnéticamente con hierro oxidado
Saif Ullah1, Stephanie Jensen1, Yanyao Liu2
1Department of Physics and Center for Functional Materials, Wake Forest University, Winston-Salem, North Carolina 27109, United States.
Journal of the American Chemical Society
|August 2, 2023
Resumen
El ferroceno químicamente oxidante se logró mediante el uso de un huésped de marco orgánico metálico. Esto permitió un nuevo estado de Fe ((II) de alto espín que se une y libera fácilmente O2, alterando su estructura electrónica y magnética.
Área de la Ciencia:
- Química organometálica
- Ciencias de los materiales
- Magnetoquímica
Sus antecedentes:
- La estructura y las propiedades electrónicas del ferroceno permanecen en gran medida sin cambios durante más de 70 años.
- Los intentos anteriores de oxidación química del ferroceno por unión directa al hierro no tuvieron éxito.
- No se han reportado cambios estructurales o magnéticos significativos para el ferroceno oxidado.
Objetivo del estudio:
- Para alterar fundamentalmente la estructura electrónica y magnética del ferroceno.
- Para lograr la oxidación química del ferroceno mediante la modificación de su entorno huésped.
- Para investigar la unión reversible del oxígeno al ferroceno.
Principales métodos:
- Utilizando un marco metálico-orgánico (MOF) como material huésped para el ferroceno.
- Utilizando un conjunto de técnicas espectroscópicas y analíticas que incluyen espectroscopia de Mößbauer, EXAFS, IR in situ, SQUID, TGA y EDXRF.
- Realización de modelos ab initio para complementar los datos experimentales.
Principales resultados:
- Se observó un nuevo estado de ferroceno de alto espín físicamente estirado / doblado dentro del MOF.
- Este estado de alto espín de Fe (II) acepta fácilmente el O2 del aire, lo que lleva a la oxidación a Fe (III).
- Se demostró que la unión al oxígeno es reversible mediante experimentos de oscilación de temperatura.
Conclusiones:
- La encapsulación del marco metálico-orgánico permite un control sin precedentes sobre las propiedades electrónicas y magnéticas del ferroceno.
- Se han logrado cambios reversibles en la unión al oxígeno y en el estado de oxidación del ferroceno.
- Este trabajo abre nuevas vías para manipular moléculas organometálicas para aplicaciones de detección o catalíticas.
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