A DFT Study of CO(2) Hydrogenation on Faujasite‐Supported Ir(4) Clusters: on the Role of Water for Selectivity Control

Reaction mechanisms for the catalytic hydrogenation of CO(2) by faujasite‐supported Ir(4) clusters were studied by periodic DFT calculations. The reaction can proceed through two alternative paths. The thermodynamically favoured path results in the reduction of CO(2) to CO, whereas the other, kineti...

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Detalles Bibliográficos
Autores principales: Szyja, Bartłomiej M., Smykowski, Daniel, Szczygieł, Jerzy, Hensen, Emiel J. M., Pidko, Evgeny A.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2016
Materias:
Full Papers
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5094556/
https://www.ncbi.nlm.nih.gov/pubmed/27840663
http://dx.doi.org/10.1002/cctc.201600644
Descripción
Sumario:Reaction mechanisms for the catalytic hydrogenation of CO(2) by faujasite‐supported Ir(4) clusters were studied by periodic DFT calculations. The reaction can proceed through two alternative paths. The thermodynamically favoured path results in the reduction of CO(2) to CO, whereas the other, kinetically preferred channel involves CO(2) hydrogenation to formic acid under water‐free conditions. Both paths are promoted by catalytic amounts of water confined inside the zeolite micropores with a stronger promotion effect for the reduction path. Co‐adsorbed water facilitates the cooperation between the zeolite Brønsted acid sites and Ir(4) cluster by opening low‐energy reaction channels for CO(2) conversion.

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