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La conmutación magnética en estado sólido desencadenada por la transferencia de electrones acoplados a protones
Pauline Higel1, Françoise Villain, Michel Verdaguer
1Institut Parisien de Chimie Moléculaire, Université Pierre et Marie Curie , UMR CNRS 8232, Case 42, 4 place Jussieu, 75252 Paris Cedex 05, France.
Journal of the American Chemical Society
|April 16, 2014
Resumen
La acidez del agua en los análogos azules prusianos del hierro cobalto desencadena una transferencia de electrones reversible. Este proceso implica una reacción de transferencia de electrones acoplados a protones (PCET) facilitada por el transporte de iones a través del material.
Área de la Ciencia:
- Ciencia de los materiales Ciencia de los materiales.
- La electroquímica es electroquímica.
- Química del estado sólido.
Sus antecedentes:
- Los análogos azules prusianos (PBA) son polímeros de coordinación porosa versátiles.
- Los iones de cobalto en los PBA pueden sufrir cambios redox, cruciales para aplicaciones electroquímicas.
- Las moléculas de agua coordinadas con iones metálicos pueden influir en las propiedades y la reactividad de los materiales.
Objetivo del estudio:
- Para investigar el papel de la acidez de la molécula de agua en la activación de la transferencia de electrones en CoFe PBAs.
- Para dilucidar el mecanismo del proceso redox Co(III) Fe(II) Co(II) Fe(III.
- Explorar el potencial de los PBA para las reacciones de transferencia de electrones acoplados a protones (PCET).
Principales métodos:
- Análisis estructural del CoFe PBA.
- Estudios de la estructura electrónica.
- Mediciones electroquímicas para estudiar el comportamiento redox.
- Investigación de los mecanismos de transporte de iones dentro de los poros de PBA.
Principales resultados:
- Se descubrió que la acidez de las moléculas de agua coordinadas activa de manera reversible la transferencia de electrones Co(III) Fe(II) Co(II) Fe(III.
- El proceso fue identificado como una reacción original de PCET entre el PBA en estado sólido y los iones de hidróxido en solución.
- Se observó el transporte de largo alcance de H ((+) y Rb ((+) dentro de los canales de poro de PBA, facilitado por el agua zeolítica que actúa como cables de protones.
Conclusiones:
- La acidez de la molécula de agua es un factor clave en el control de la actividad redox en los PBA de CoFe.
- El estudio revela un nuevo mecanismo PCET de estado sólido habilitado por el transporte de iones en materiales porosos.
- Los PBA de CoFe demuestran potencial como materiales funcionales para reacciones que involucran transferencia de protones y electrones.
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