Artículos de revistas
Improvement in the Reduction Behavior of Novel ZrO(2)-CeO(2) Solid Solutions with a Tubular Nanostructure by Incorporation of Pd
Fecha
2010Registro en:
JOURNAL OF PHYSICAL CHEMISTRY C, v.114, n.46, p.19687-19696, 2010
1932-7447
10.1021/jp108429t
Autor
ACUNA, Leandro M.
MUNOZ, Fernando F.
CABEZAS, Marcelo D.
LAMAS, Diego G.
LEYVA, A. Gabriela
Fantini, Marcia Carvalho de Abreu
BAKER, Richard T.
FUENTES, Rodolfo O.
Institución
Resumen
In this work, 1 wt % Pd/ZrO(2)-CeO(2) mixed oxide nanotubes with 90 mol % CeO(2) were synthesized following a very simple, high-yield procedure and their properties were characterized by synchrotron radiation X-ray diffraction, X-ray absorption near-edge spectroscopy (XANES), and scanning and high-resolution transmission electron microscopy (SEM and HRTEM). In situ XANES experiments were carried out under reducing conditions to investigate the reduction behavior of these novel nanotube materials. The Pd/CeO(2)-based nanotubes exhibited the cubic phase (Fm3m space group). The nanotube walls were composed of nanoparticles with an average crystallite size of about 7 nm, and the nanotubes exhibited a large specific surface area (85 m(2).g(-1)). SEM and HRTEM studies showed that individual nanotubes were composed of a curved sheet of these nanoparticles. Elemental analysis showed that the Ce:Zr:Pd ratios appeared to be approximately constant across space, suggesting compositional homogeneity in the samples. XANES results indicated that the extent of reduction of these materials is low and that the Ce(4+) state is in the majority over the reduced Ce(3+) state. The results suggest that Pd cations-most likely Pd(2+)-form a Pd-Ce-Zr oxide solid solution and that the Pd(2+) is stabilized against reduction in this phase. However, incorporation of the Pd (1 wt %) into the crystal lattice of the nanotubes also appeared to destabilize Ce(4+) against reduction to Ce(3+) and caused a significant increase in its reducibility.