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Catálisis multielectrónica asistida por ligando redox activo: un caso de complejo CoIII como catalizador de oxidación
Hao-Yi Du1, Si-Cong Chen1, Xiao-Jun Su1
1Center of Basic Molecular Science (CBMS), Department of Chemistry, Tsinghua University , Beijing 100084, China.
Journal of the American Chemical Society
|January 9, 2018
Resumen
Este estudio introduce un catalizador de metal no precioso estable, Na[(L4−) CoIII, para una oxidación molecular eficiente del agua. Los mecanismos asistidos por fosfato impulsan el ciclo catalítico para la producción de combustible solar.
Área de la Ciencia:
- Catálisis
- Fotosíntesis artificial
- La electroquímica
Sus antecedentes:
- La oxidación del agua es crucial para la captura de energía solar en la fotosíntesis natural y artificial.
- El desarrollo de catalizadores de metales no preciosos eficientes y estables para la oxidación del agua sigue siendo un desafío importante.
Objetivo del estudio:
- Para investigar la actividad de oxidación electrocatalítica en agua de Na[(L4−) CoIII] en solución acuosa a pH 7,0.
- Para aclarar el mecanismo catalítico y el papel del ligando y las características redox del metal.
Principales métodos:
- Investigación electroquímica de Na[(L4−) CoIII] en un amortiguador de fosfato de 0,1 M a un pH de 7,0.
- Cálculos de la teoría funcional de la densidad (DFT) para confirmar el ciclo catalítico propuesto.
Principales resultados:
- Na[(L4−) CoIII] demostró una catálisis homogénea estable y eficiente para la oxidación del agua con un sobrepotencial de inicio de 380 mV.
- El ciclo catalítico involucra procesos redox centrados en ligandos y metales, incluida la transferencia de electrones acoplados a protones.
- Los cálculos de DFT apoyaron el mecanismo propuesto, destacando el ataque nucleofílico de agua asistido por fosfato sobre [L2−) CoIɛO] para la formación de enlaces O-O.
Conclusiones:
- Na[(L4−) CoIII] es un catalizador prometedor para la oxidación electrocatalítica del agua.
- El estudio proporciona información mecanicista sobre los catalizadores de oxidación de agua de metales no preciosos, que implican la asistencia del fosfato en la formación de enlaces O-O.
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