IR spectroscopic insights into the coking-resistance effect of potassium on nickel-based catalyst during dry reforming of methane

Dry reforming of methane (DRM) is an effective catalytic route for transforming CO2 and CH4 into valuable syngas and thus potentially attractive for mitigating the emission of environmental harmful gases. Therefore, it is crucial to develop rationally Ni-based catalysts highly resistant to coking an...

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Detalles Bibliográficos
Autores: Azancot Luque, Lola de las Aguas, Bobadilla Baladrón, Luis Francisco, Centeno Gallego, Miguel Ángel, Odriozola Gordón, José Antonio
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2021
País:España
Institución:Universidad de Sevilla (US)
Repositorio:idUS. Depósito de Investigación de la Universidad de Sevilla
OAI Identifier:oai:idus.us.es:11441/165312
Acceso en línea:https://hdl.handle.net/11441/165312
https://doi.org/10.1016/j.apcatb.2020.119822
Access Level:acceso abierto
Palabra clave:Coking-Resistance effect
Dry reforming
IR spectroscopy
Ni-K interaction
Descripción
Sumario:Dry reforming of methane (DRM) is an effective catalytic route for transforming CO2 and CH4 into valuable syngas and thus potentially attractive for mitigating the emission of environmental harmful gases. Therefore, it is crucial to develop rationally Ni-based catalysts highly resistant to coking and sintering. In this scenario, the addition of small amounts of potassium to nickel catalyst increases their resistance to coking during dry reforming of methane. Nonetheless, the specific role of potassium in these catalysts not have been fully understood and there are still important discrepancies between the different reported studies. This work provides a new approach on the anticoking nature of a K-promoted Ni catalyst by means of a combined IR spectroscopic study of in situ characterization by CO adsorption under static conditions and operando DRIFTS measurements under dynamic conditions of DRM reaction. The involved surface species formed during the reaction were elucidated by transient and steady-state operando DRIFTS studies. It was revealed that the existence of Ni-K interfacial sites favours the gasification of carbonaceous deposits towards reverse Boudouard reaction and reduces the sticking probability of CO2 dissociative adsorption. Moreover, the presence of strongly Mg-O-K basic sites leads to the formation of carbonate intermediates that are subsequently reduced into CO gaseous towards the associative mechanism by RWGS reaction. These results provide a fundamental understanding of the relevant anticoking effect of potassium on Ni-based catalysts.