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Título: | Surface reduction mechanism of cerium-gallium mixed oxides with enhanced redox properties |
Autor: | Vecchietti, Julia; Collins, Sebastián; Xu, Wenqia; Barrio Pliego, Laura CSIC ORCID; Stacchiola, D.; Calatayud, Mónica; Tielens, Frederik; Delgado, Juan José; Bonivardi, A. | Fecha de publicación: | 3-abr-2013 | Editor: | American Chemical Society | Citación: | Journal of Physical Chemistry C 117(17): 8822-8831 (2013) | Resumen: | The doping of CeO2 with different types of cations has been recognized as a significant factor in controlling the oxygen vacancies and improving the oxygen mobility. Thus, the catalytic properties of these materials might be determined by modifying the redox properties of ceria. A combined experimental and theoretical study of the redox properties of gallium-doped cerium dioxide is presented. Infrared spectroscopy and time-resolved X-ray diffraction were used for temperature programmed reduction (H2) and oxidation (with O2 and H2O) studies. Additionally, X-ray absorption near edge spectroscopy shows that only Ce4+ is reduced to Ce3+ in the ceria–gallia mixed oxides when annealed up to 623 K. The oxygen storage capacity (OSC) measurements show a pronounced enhancement on the reduction of ceria by gallium doping. Theoretical calculations by density functional theory (DFT) confirm the higher reducibility of gallium-doped ceria oxides and give a molecular description of the stabilization of the doped material. On the basis of infrared spectroscopic measurements, a novel mechanism is proposed for the surface reduction of Ce4+ to Ce3+ where Ga–H species are suggested to be directly involved in the process. In addition, the reoxidation by H2O was precluded in the gallium-doped ceria oxide. | Versión del editor: | https://doi.org/10.1021/jp400285b | URI: | http://hdl.handle.net/10261/187368 | DOI: | 10.1021/jp400285b | ISSN: | 1932-7447 | E-ISSN: | 1932-7455 |
Aparece en las colecciones: | (ICP) Artículos |
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