Journal
SOLID STATE IONICS
Volume 303, Issue -, Pages 58-69Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.ssi.2017.02.010
Keywords
Nanostructured materials; Solid state reactions; Diffusion; Mixed silicate and aluminate; Transmission electron microscopy; TEM
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The structural evolution of the Ce0.8Gd0.2O1.9 nanocubes supported on Al2O3 and SiO2 was investigated in oxidizing and reducing atmosphere over a temperature range up to 1100 degrees C by XRD, TEM and SEM-EDS methods. The supported Ce0.8Gd0.2O1.9 particles preserved perfect cubic shape to 900 degrees C in oxidizing atmosphere and to 750 degrees C in a hydrogen atmosphere. No evidence of crystalline aluminate or silicate formation was observed for both supports during heating in oxidizing atmosphere up to 1100 degrees C. However, for Ce0.8Gd0.2O1.9/SiO2 segregation of Gd3+ from the mixed oxide and its spreading over the silica surface was noticed at 1000 degrees C-1100 degrees C. Crystalline aluminate/silicate occurred in a hydrogen atmosphere already at 900 C. Apatite type (Ce,Gd)(4.67)(SiO4)(3)O mixed silicate was formed after reaction with SiO2 substrate, while monoclinic (Gd,Ce)(4)Al2O9 and tetragonal (Ce,Gd)AlO3 were formed on Al2O3. The (Gd,Ce)(4)Al2O9 phase became unstable at 950 degrees C and transformed into (Ce,Gd)AlO3 aluminate, which was stable up to 1100 degrees C. Various mechanisms of the solid-state reaction of mixed ceria with Al2O3 and SiO2 supports operate depending on the size of ceria nanocubes. Small particles (10-30 nm) reacted as a whole with the support forming single crystal silicate or aluminate; at the same time, for bigger particles (30-80 nm) reactions happen only near the boundary between the particle and the support. (C) 2017 Elsevier B.V. All rights reserved.
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