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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
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Hidrógenos de superficie en el electrocatalizador Fe2 Reducir CO2 a bajo sobrepotencial: Selectividad de dirección al
Karin U D Calvinho1, Abdulaziz W Alherz2, Kyra M K Yap1
1Department of Chemistry and Chemical Biology, Rutgers, The State University of New Jersey, 123 Bevier Road, Piscataway, New Jersey 08854, United States.
Journal of the American Chemical Society
|December 9, 2021
Resumen
El fosfuro de hierro (Fe2P) cataliza eficientemente la reducción de dióxido de carbono (CO2RR) a productos multicarbónicos como el etilenoglicol. Los hidritos iónicos y la selectividad del producto de control potencial aplicado ofrecen nuevos conocimientos sobre los mecanismos de la CO2RR.
Área de la Ciencia:
- La electroquímica
- Catálisis
- Ciencias de los materiales
Sus antecedentes:
- Los electrocatalizadores eficientes para la reducción de CO2 a productos multicarbónicos son cruciales, pero se enfrentan a desafíos con altos potenciales excesivos y poca selectividad.
- Se buscan catalizadores abundantes en la tierra para superar las limitaciones de los sistemas basados en metales preciosos.
Objetivo del estudio:
- Introducir el fosfuro de hierro (Fe2P) como electrocatalizador abundante en la tierra para la reducción de CO2 a productos multicarbónicos.
- Investigar el mecanismo de reacción y los factores que controlan la selectividad del producto, en particular el papel de los hidritos y el potencial aplicado.
Principales métodos:
- Experimentos de reacción electroquímica de reducción de CO2 (CO2RR).
- Los cálculos del Gran Canónico-DFT (GC-DFT).
- Análisis de las especies intermedias y de las afinidades de unión de los hidruros superficiales.
Principales resultados:
- El Fe2P demostró una eficiencia Faradaic del 53% total de CO2RR para los productos C2-C4 a 0 V frente a RHE.
- La selectividad del producto se desplazó hacia el etilenoglicol con un sesgo negativo creciente.
- GC-DFT y los experimentos revelaron formato, no CO, como el intermediario inicial, con hidritos iónicos que juegan un papel clave.
- La unión de hidrógeno se debilita con sesgo negativo, influyendo en la selectividad C2 y la velocidad de reacción de evolución de hidrógeno (HER).
Conclusiones:
- La formación de hidruro iónico y la afinidad de unión, moduladas por el potencial aplicado, dictan la distribución del producto de carbono en CO2RR.
- La comprensión de la especiación de hidrógenos proporciona información crítica sobre los mecanismos de CO2RR en los fosfuros de metales de transición.
- El Fe2P se muestra prometedor como un catalizador abundante en la tierra para la conversión selectiva de CO2.
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