Unraveling the effects of Fe and Mn promoters on the tungstated zirconia catalyst: A DFT study

Periodic DFT calculations are performed to unravel the effect of the incorporation of Fe and Mn into the tung-stated zirconia catalyst, (WO3)x/ZrO2 (x = 1,3), in their electronic, geometric, and catalytic properties. Our results suggest that both Mn and Fe have a proclivity to occupy the same positi...

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Detalles Bibliográficos
Autores: Madrigal Carrillo, Karina G., Rodríguez, Juan I., Hernández Pichardo, Martha L., Jiménez Izal, Elisa
Tipo de recurso: artículo
Fecha de publicación:2022
País:España
Institución:Universidad del País Vasco
Repositorio:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/58514
Acceso en línea:http://hdl.handle.net/10810/58514
Access Level:acceso abierto
Palabra clave:DFT
tungstated zirconia
catalysis
alkane isomerization
WOx clusters
deprotonation
Descripción
Sumario:Periodic DFT calculations are performed to unravel the effect of the incorporation of Fe and Mn into the tung-stated zirconia catalyst, (WO3)x/ZrO2 (x = 1,3), in their electronic, geometric, and catalytic properties. Our results suggest that both Mn and Fe have a proclivity to occupy the same positions and thus both metals will compete for the same adsorption sites. The addition of Fe or Mn slightly destabilizes the WO3 monomer while stabilizes the (WO3)3 trimer. Hence, medium size clusters, which are the most catalytically active species, will be more sinter resistant in the presence of the promoters, leading to catalysts with longer lifetimes. The computed deprotonation energies evidence that the overall Bronstead acidity is increased upon the addition of the dopant atoms. It is proposed that the metals lead to a reduction of WZ and induce a local spin density imbalance.The function as redox initiators of these metals is confirmed.