Ce1−xPrxO2−δ (x = 0, 0.1, 0.5, 0.9) mesoarchitectures built from nanoparticles with crystalline framework have been synthesized by the self-assembly method assisted by surfactants and hydrothermal treatment. Cetyltrimethylammonium bromide (CTAB) was used as template, urea as hydrolyzing agent and tetraethylammonium hydroxide (TEAOH) as pH mediator to obtain pH 9. The inorganic precursors have been co-assembled with surfactant template to produce mesoarchitectures which have uniform pore size distribution, crystalline channel walls, high thermal stability, and high catalytic activity in the oxidation reaction of methane. The resulting powders, calcined at 550 °C, were characterized by X-ray diffraction (XRD), Raman spectroscopy, N2 adsorption/desorption isotherms (BET), thermogravimetric analysis (TG-DTG), scanning and transmission electron microscopy (SEM, TEM, and HRTEM), and X-ray photoelectron spectroscopy (XPS). The as-synthesized mesoporous nanoparticles are single-phase fluorite Ce1−xPrxO2−δ solid solution without additional Ce- or Pr-based oxides, or secondary phases with different lattice symmetry or stoichiometry. A clear morphology of dispersed nanoparticles, with uniform grain size between 5 and 7 nm, and mean pore size around 5 nm, have been observed. The specific surface area of the as-synthesized mesoporous samples after calcination at 550 °C remains in the range 60–150 m2 g−1. All the spectroscopic methods clearly confirm the homogeneous incorporation of Pr into the CeO2 lattice of the nanocrystallites, to form a single-phase solid solution with fluorite structure, modifying the absorption spectra of the nanocrystallites. All the samples showed high catalytic activity in the oxidation reactions of methane.
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This article was carried out within the research program Surface Chemistry and Catalysis of the ‘‘Ilie Murgulescu’’ Institute of Physical Chemistry, financed by the Romanian Academy. Support of the EU (ERDF) and Romanian Government that allowed for acquisition of the research infrastructure under POS-CCE O 2.2.1 project INFRANANOCHEM-Nr. 19/01.03.2009, is gratefully acknowledged.
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