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La tensión molecular acelera la transferencia de electrones para mejorar la reducción de oxígeno

Charles B Musgrave1, Jianjun Su2, Pei Xiong3

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La tensión local en los catalizadores de hierro-nitrógeno-carbono (Fe-N-C) mejora significativamente la cinética de la reacción de reducción de oxígeno (ORR). Esta cepa molecular mejora el rendimiento del catalizador para aplicaciones de energía renovable.

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Área de la Ciencia:

  • Ciencias de los materiales
  • La electroquímica
  • Química computacional

Sus antecedentes:

  • Los materiales de hierro-nitrógeno-carbono (Fe-N-C) son alternativas prometedoras a los catalizadores de platino para la reacción de reducción de oxígeno (ORR).
  • La cinética ORR lenta en los materiales Fe-N-C conduce a altos sobrepotenciales, lo que limita su eficiencia en los dispositivos de conversión de energía.

Objetivo del estudio:

  • Investigar el efecto de la tensión molecular local en el rendimiento ORR de los catalizadores Fe-N-C.
  • Elucidar el mecanismo por el cual la tensión influye en la cinética de la ORR utilizando la ftalacianina de hierro (FePc) como sistema modelo.

Principales métodos:

  • Cálculos de la teoría funcional de la densidad (DFT) para predecir el mecanismo ORR y las barreras energéticas.
  • Síntesis experimental y caracterización electroquímica de catalizadores de FePc tensados en nanotubos de carbono de pared única.
  • Integración del catalizador optimizado en una batería de zinc-aire para la evaluación del rendimiento.

Principales resultados:

  • Los cálculos de DFT revelaron que la tensión molecular acelera la desorción reductora de *OH al disminuir la barrera de energía en aproximadamente 60 meV.
  • Experimentalmente, el FePc tensado logró un potencial de media onda (E1/2) de 0.952 V y una pendiente Tafel de 35.7 mV dec-1, competitivo con los catalizadores Fe-N-C de última generación.
  • Se observó un desplazamiento de 70 mV en E1 / 2 y pendientes de Tafel distintas para configuraciones de FePc planas versus curvas, alineadas con las predicciones teóricas.

Conclusiones:

  • La tensión molecular es una estrategia eficaz para mejorar la actividad ORR de los materiales Fe-N-C.
  • Los resultados proporcionan una vía para diseñar catalizadores de alto rendimiento para aplicaciones de energía renovable mediante el control de la estructura del catalizador.
  • El catalizador de FePc tensado demostró un excelente rendimiento en una batería de zinc-aire, logrando una densidad de potencia máxima de 350,6 mW cm-2.