Nickel Dynamics Switches the Selectivity of CO2 Hydrogenation

The Reverse Water Gas-Shift reaction (CO2+H2mathematical equation CO+H2O) allows to balance syn-gas under industrial conditions. Nickel has been suggested as a potential catalyst but the temperature required is too high, more than 800 °C, limiting practical implementation but when lowering the tempe...

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Detalles Bibliográficos
Autores: González, José Manuel, Sabadell-Rendón, Albert, Kaźmierczak, Kamila, Euzenat, Florian, Montroussier, Nicolas, Curulla-Ferré, Daniel, López, Núria
Tipo de recurso: artículo
Fecha de publicación:2024
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2072/480027
Acceso en línea:http://hdl.handle.net/2072/480027
https://doi.org/10.1002/anie.202417392
Access Level:acceso abierto
Palabra clave:Química
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Descripción
Sumario:The Reverse Water Gas-Shift reaction (CO2+H2mathematical equation CO+H2O) allows to balance syn-gas under industrial conditions. Nickel has been suggested as a potential catalyst but the temperature required is too high, more than 800 °C, limiting practical implementation but when lowering the temperature methanation occurs. Simulations via Density Functional Theory on well-defined surfaces have systematically failed to reproduce these experimental results. But under reaction conditions, Ni surfaces are not static and DFT models coupled to microkinetics show that low temperatures (high CO coverages) drive the generation of Ni adatoms that are the active sites for methanation. At higher temperatures, the adatom population decreases, and the selectivity towards CO increases. Thus the mechanism behind the selectivity switch is driven by the dynamics induced by reaction intermediates. Our work contributes to the inclusion of dynamic aspects of materials under reaction conditions in the understanding of complex catalytic behaviour.