In situ characterization of mesoporous Co/CeO2 catalysts for the high-temperature water-gas shift

Mesoporous Co/CeO2 catalysts were found to exhibit significant activity for the high-temperature water-gas shift (WGS) reaction with cobalt loadings as low as 1 wt %. The catalysts feature a uniform dispersion of cobalt within the CeO2 fluorite type lattice with no evidence of discrete cobalt phase...

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Detalhes bibliográficos
Autores: Vovchock, Dimitriy, Guild, Curtis J., Dissanayake, Shanka, Llorca Piqué, Jordi|||0000-0002-7447-9582, Stavitski, Eli, Liu, Yongyuan, Palomino, Robert M., Waluyo, Iradwikanari, Li, YuanYuan, Frenkel, Anatoly I., Rodriguez, José A., Suib, Steven L., Senanayake, S. D.
Tipo de documento: artigo
Data de publicação:2018
País:España
Recursos:Universitat Politècnica de Catalunya (UPC)
Repositório:UPCommons. Portal del coneixement obert de la UPC
Idioma:inglês
OAI Identifier:oai:upcommons.upc.edu:2117/118331
Acesso em linha:https://hdl.handle.net/2117/118331
https://dx.doi.org/10.1021/acs.jpcc.8b01271
Access Level:Acceso aberto
Palavra-chave:Catalysts
Mesoporous materials
Catalitzadors
Àrees temàtiques de la UPC::Enginyeria química
Descrição
Resumo:Mesoporous Co/CeO2 catalysts were found to exhibit significant activity for the high-temperature water-gas shift (WGS) reaction with cobalt loadings as low as 1 wt %. The catalysts feature a uniform dispersion of cobalt within the CeO2 fluorite type lattice with no evidence of discrete cobalt phase segregation. In situ XANES and ambient pressure XPS experiments were used to elucidate the active state of the catalysts as partially reduced cerium oxide doped with oxidized cobalt atoms. In situ XRD and DRIFTS experiments suggest facile cerium reduction and oxygen vacancy formation, particularly with lower cobalt loadings. In situ DRIFTS analysis also revealed the presence of surface carbonate and bidentate formate species under reaction conditions, which may be associated with additional mechanistic pathways for the WGS reaction. Deactivation behavior was observed with higher cobalt loadings. XANES data suggest the formation of small metallic cobalt clusters at temperatures above 400 °C may be responsible. Notably, this deactivation was not observed for the 1% cobalt loaded catalyst, which exhibited the highest activity per unit of cobalt.