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The structural and electronic properties of nanostructured ternary oxides: Unusual concentration of and interactions
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Image of FIG. 1.
FIG. 1.

Unit cell used to study the properties of bulk . The unit cell contains 4 atoms of Ce, 4 atoms of Zr, 4 atoms of Tb, and 24 atoms of O. The positions of the metal cations were exchanged in the unit cell to reflect a random solid solution (see text). In the figure is shown a possible configuration for the ternary oxide.

Image of FIG. 2.
FIG. 2.

Lattice constants determined by x-ray diffraction at for nanoparticles of , , , and . The notation used to label the mixed-metal oxides is explained in Sec. II A.

Image of FIG. 3.
FIG. 3.

Cell parameters determined for and nanoparticles from XRD patterns (solid lines) and estimated using Vegard’s rule (Ref. 35) and the experimental lattice parameters for bulk (Ref. 4), (Ref. 34), and (Refs. 4 and 17) (dashed lines).

Image of FIG. 4.
FIG. 4.

Cell parameters for nanoparticles obtained from XRD (solid line) and Vegard’s rule (dashed line). In the top panel, the ratio is maintained constant while Zr is added. In the bottom panel, Tb is added keeping the ratio constant.

Image of FIG. 5.
FIG. 5.

Strain parameter (obtained from XRD patterns at ) for , , , and nanoparticles.

Image of FIG. 6.
FIG. 6.

Raman spectra taken at for a series of nanoparticles.

Image of FIG. 7.
FIG. 7.

Time-resolved XRD results obtained after heating a sample of nanoparticles from . Heating , and .

Image of FIG. 8.
FIG. 8.

Variation of particle size (top panel) and cell dimension (bottom panel) with temperature for nanoparticles of , (CZ11), (CT11), and (CZT111). Heating .

Image of FIG. 9.
FIG. 9.

O -edge XANES spectra taken at room temperature for and nanoparticles. The notation used to label the mixed-metal oxides is explained in Sec. II A. The top panel compares the experimental spectrum (solid trace) for nanoparticles and that obtained by adding the corresponding spectra for , (Ref. 18), and (Ref. 8) weighted by the concentration of the metals in the ternary oxide (dashed line).

Image of FIG. 10.
FIG. 10.

Ce -edge XANES spectra for and nanoparticles taken at room temperature.

Image of FIG. 11.
FIG. 11.

Room-temperature Zr -edge XANES spectra for monoclinic , , and nanoparticles.

Image of FIG. 12.
FIG. 12.

Tb -edge spectra for a reference (probably ) and nanoparticles at .


Generic image for table
Table I.

Calculated Mulliken charges (e)


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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: The structural and electronic properties of nanostructured Ce1−x−yZrxTbyO2 ternary oxides: Unusual concentration of Tb3+ and metal↔oxygen↔metal interactions