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Modulación de un dicobre μ-1,2-Peroxo (II) Intermedio por una fuerte interacción con iones metálicos alcalinos
Alexander Brinkmeier1, Kristian E Dalle1, Lorenzo D'Amore2
1Institute of Inorganic Chemistry, University of Göttingen, Tamannstrasse 4, D-37077 Göttingen, Germany.
Journal of the American Chemical Society
|October 18, 2021
Resumen
Los iones de metales alcalinos ligeramente ácidos de Lewis se unen fuertemente a los intermediarios reactivos de cobre y peróxido. Esta interacción altera significativamente las propiedades electrónicas y magnéticas de estas especies de catálisis de oxidación cruciales.
Área de la Ciencia:
- Química de coordinación
- Química bioorgánica
- Catalización por oxidación
Sus antecedentes:
- Las especies de metales/oxígeno son intermedios clave en la catálisis de la oxidación.
- La información estructural sobre los adductos ácidos de Lewis de estos intermediarios es limitada.
- Los ácidos de Lewis redóxido-inactivos pueden modular las propiedades del metal/oxígeno.
Objetivo del estudio:
- Investigar la interacción entre los iones de metales alcalinos y un intermediario reactivo de cis-peróxido de cobre.
- Obtener conocimientos estructurales y electrónicos sin precedentes en estos productos.
- Comprender cómo la unión de metales alcalinos afecta las propiedades de las especies de Cu2O2.
Principales métodos:
- Cristalografía de rayos X para la caracterización estructural de Cu2O2 desnudo y complejo de metales alcalinos.
- UV-vis, espectroscopia de Raman y electroquímica para estudiar la unión en solución.
- Análisis computacional para elucidar los efectos electrónicos y magnéticos.
Principales resultados:
- Se ha demostrado una fuerte unión de Li+, Na+ y K+ al intermediario cis-peroxo dicopro (II).
- Se obtienen estructuras cristalinas sin precedentes del motivo Cu2O2 desnudo y aducido con metales alcalinos.
- La fuerza de unión mostrada se correlaciona con la acidez del catión de Lewis, con una alta afinidad por el Li+.
- Reveló que los iones alcalinos modulan la transferencia de carga dentro del núcleo Cu-OO-Cu, alterando las propiedades electrónicas, magnéticas y electroquímicas.
Conclusiones:
- Los iones de metales alcalinos, a menudo considerados espectadores, interactúan significativamente con los intermediarios reactivos de metal y oxígeno e influyen en ellos.
- Esta unión afecta las características electrónicas y magnéticas fundamentales de las especies de Cu2O2.
- Los resultados son relevantes para los estudios in situ de los intermedios transitorios y para la comprensión de los procesos de oxidación (bio) química en diversos ambientes.
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