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La conmutación redox en estado sólido del intercambio magnético y la conductividad electrónica en un compuesto de
Ie-Rang Jeon1, Lei Sun2, Bogdan Negru1
1Department of Chemistry, Northwestern University , 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States.
Journal of the American Chemical Society
|April 27, 2016
Resumen
Este estudio muestra que un ligando especial en un compuesto de cadena puede cambiar sus propiedades ópticas, magnéticas y electrónicas cuando se reduce. Esta conmutación redox reversible abre las puertas a nuevos materiales inteligentes.
Área de la Ciencia:
- Ciencias de los materiales
- Química inorgánica
- Química del estado sólido
Sus antecedentes:
- El desarrollo de materiales con propiedades intercambiables es crucial para las tecnologías avanzadas.
- Los sólidos de coordinación ofrecen marcos ajustables para explorar nuevas funcionalidades.
- Los ligandos redox activos pueden impartir un comportamiento dinámico a los materiales que contienen metales.
Objetivo del estudio:
- Para investigar la incorporación de un ligando benzoquinoide redox activo en un compuesto de cadena unidimensional.
- Para demostrar la conmutación redox simultánea en estado sólido de propiedades ópticas, magnéticas y electrónicas.
- Para explorar la reversibilidad de estas modulaciones de propiedad.
Principales métodos:
- Síntesis de un compuesto de cadena de manganeso (III) con un ligando benzoquinóide específico (4,5-bis (pyridine-2-carboxamido) -1,2-catecol).
- Reducción en estado sólido con cobaltoceno (Cp2Co) y oxidación con ferrocenio ([Cp2Fe](+)).
- Caracterización mediante espectroscopia de Raman, espectroscopia de absorción de rayos X, mediciones de susceptibilidad magnética y mediciones de conductividad.
Principales resultados:
- El compuesto sintetizado Mn (((N,O) L) ((DMSO) presenta centros de Mn ((II) conectados por ligandos parcialmente reducidos.
- La reducción centrada en los ligandos a [Mn((N,O) L) ](-) dio lugar a un cambio de color (de verde a púrpura), un aumento de 40 veces en el acoplamiento magnético y un aumento de 10.000 veces en la conductividad.
- Los cambios de propiedades observados fueron reversibles tras la reoxidación.
Conclusiones:
- Los ligandos benzoquinoides pueden facilitar las reacciones redox basadas en ligandos en sólidos de coordinación no porosos.
- Esto permite la conmutación reversible de propiedades ópticas, magnéticas y electrónicas.
- Los hallazgos ponen de relieve una vía para diseñar materiales funcionales avanzados con características intercambiables.
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