Thermo-mechanical properties of cubic lanthanide oxides

Hussein A. Miran, Mohammednoor Altarawneh, Hantarto Widjaja, Zainab N. Jaf, M. Mahbubur Rahman, Jean Pierre Veder, Bogdan Z. Dlugogorski, Zhong Tao Jiang

Research output: Contribution to journalArticleResearchpeer-review

Abstract

This contribution investigates the effect of the addition of the Hubbard U parameter on the electronic structural and mechanical properties of cubic (C-type) lanthanide sesquioxides (Ln 2 O 3 ). Calculated Bader's charges confirm the ionic character of Ln–O bonds in the C-type Ln 2 O 3 . Estimated structural parameters (i.e., lattice constants) coincide with analogous experimental values. The calculated band gaps energies at the U eff of 5 eV for these compounds exhibit a non-metallic character and U eff of 6.5 eV reproduces the analogous experimental band gap of cerium sesquioxide Ce 2 O 3 . We have thoroughly investigated the effect of the O/Ce ratios and the effect of hafnium (Hf) and zirconium (Zr) dopants on the reduction energies of CeO x configurations. Our analysis for the reduction energy of CeO 2 , over a wide range of temperatures displays that, shuffling between the two +4 and +3 oxidation states of Ce exhibit a temperature-independent behaviour. Higher O/Ce ratios necessitate lower reduction energies. Our results on Ce–Hf–Zr–O alloys are in reasonable agreements with analogous fitted values pertinent to lowering reduction energies and shrinkage in lattice parameters when contrasted with pure CeO 2 . Structural analysis reveals that Hf and Zr atoms in the solid solution are shifted towards the nearest vacancies upon reduction. It is hoped that values provided herein to shed an atomic-base insight into the reduction/oxidation thermodynamics of increasingly deployed catalysts for environmental applications.

Original languageEnglish
Pages (from-to)37-48
Number of pages12
JournalThin Solid Films
Volume653
DOIs
Publication statusPublished - 1 May 2018
Externally publishedYes

Fingerprint

Lanthanoid Series Elements
Rare earth elements
Oxides
mechanical properties
Mechanical properties
oxides
Hafnium
hafnium
Zirconium
Lattice constants
lattice parameters
Energy gap
Cerium
Oxidation
oxidation
energy
cerium
shrinkage
structural analysis
Structural analysis

Cite this

Miran, H. A., Altarawneh, M., Widjaja, H., Jaf, Z. N., Mahbubur Rahman, M., Veder, J. P., ... Jiang, Z. T. (2018). Thermo-mechanical properties of cubic lanthanide oxides. Thin Solid Films, 653, 37-48. https://doi.org/10.1016/j.tsf.2018.01.063
Miran, Hussein A. ; Altarawneh, Mohammednoor ; Widjaja, Hantarto ; Jaf, Zainab N. ; Mahbubur Rahman, M. ; Veder, Jean Pierre ; Dlugogorski, Bogdan Z. ; Jiang, Zhong Tao. / Thermo-mechanical properties of cubic lanthanide oxides. In: Thin Solid Films. 2018 ; Vol. 653. pp. 37-48.
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abstract = "This contribution investigates the effect of the addition of the Hubbard U parameter on the electronic structural and mechanical properties of cubic (C-type) lanthanide sesquioxides (Ln 2 O 3 ). Calculated Bader's charges confirm the ionic character of Ln–O bonds in the C-type Ln 2 O 3 . Estimated structural parameters (i.e., lattice constants) coincide with analogous experimental values. The calculated band gaps energies at the U eff of 5 eV for these compounds exhibit a non-metallic character and U eff of 6.5 eV reproduces the analogous experimental band gap of cerium sesquioxide Ce 2 O 3 . We have thoroughly investigated the effect of the O/Ce ratios and the effect of hafnium (Hf) and zirconium (Zr) dopants on the reduction energies of CeO x configurations. Our analysis for the reduction energy of CeO 2 , over a wide range of temperatures displays that, shuffling between the two +4 and +3 oxidation states of Ce exhibit a temperature-independent behaviour. Higher O/Ce ratios necessitate lower reduction energies. Our results on Ce–Hf–Zr–O alloys are in reasonable agreements with analogous fitted values pertinent to lowering reduction energies and shrinkage in lattice parameters when contrasted with pure CeO 2 . Structural analysis reveals that Hf and Zr atoms in the solid solution are shifted towards the nearest vacancies upon reduction. It is hoped that values provided herein to shed an atomic-base insight into the reduction/oxidation thermodynamics of increasingly deployed catalysts for environmental applications.",
keywords = "Density functional theory, Lanthanum oxide, Mechanical stability, Reduction energy",
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Miran, HA, Altarawneh, M, Widjaja, H, Jaf, ZN, Mahbubur Rahman, M, Veder, JP, Dlugogorski, BZ & Jiang, ZT 2018, 'Thermo-mechanical properties of cubic lanthanide oxides', Thin Solid Films, vol. 653, pp. 37-48. https://doi.org/10.1016/j.tsf.2018.01.063

Thermo-mechanical properties of cubic lanthanide oxides. / Miran, Hussein A.; Altarawneh, Mohammednoor; Widjaja, Hantarto; Jaf, Zainab N.; Mahbubur Rahman, M.; Veder, Jean Pierre; Dlugogorski, Bogdan Z.; Jiang, Zhong Tao.

In: Thin Solid Films, Vol. 653, 01.05.2018, p. 37-48.

Research output: Contribution to journalArticleResearchpeer-review

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T1 - Thermo-mechanical properties of cubic lanthanide oxides

AU - Miran, Hussein A.

AU - Altarawneh, Mohammednoor

AU - Widjaja, Hantarto

AU - Jaf, Zainab N.

AU - Mahbubur Rahman, M.

AU - Veder, Jean Pierre

AU - Dlugogorski, Bogdan Z.

AU - Jiang, Zhong Tao

PY - 2018/5/1

Y1 - 2018/5/1

N2 - This contribution investigates the effect of the addition of the Hubbard U parameter on the electronic structural and mechanical properties of cubic (C-type) lanthanide sesquioxides (Ln 2 O 3 ). Calculated Bader's charges confirm the ionic character of Ln–O bonds in the C-type Ln 2 O 3 . Estimated structural parameters (i.e., lattice constants) coincide with analogous experimental values. The calculated band gaps energies at the U eff of 5 eV for these compounds exhibit a non-metallic character and U eff of 6.5 eV reproduces the analogous experimental band gap of cerium sesquioxide Ce 2 O 3 . We have thoroughly investigated the effect of the O/Ce ratios and the effect of hafnium (Hf) and zirconium (Zr) dopants on the reduction energies of CeO x configurations. Our analysis for the reduction energy of CeO 2 , over a wide range of temperatures displays that, shuffling between the two +4 and +3 oxidation states of Ce exhibit a temperature-independent behaviour. Higher O/Ce ratios necessitate lower reduction energies. Our results on Ce–Hf–Zr–O alloys are in reasonable agreements with analogous fitted values pertinent to lowering reduction energies and shrinkage in lattice parameters when contrasted with pure CeO 2 . Structural analysis reveals that Hf and Zr atoms in the solid solution are shifted towards the nearest vacancies upon reduction. It is hoped that values provided herein to shed an atomic-base insight into the reduction/oxidation thermodynamics of increasingly deployed catalysts for environmental applications.

AB - This contribution investigates the effect of the addition of the Hubbard U parameter on the electronic structural and mechanical properties of cubic (C-type) lanthanide sesquioxides (Ln 2 O 3 ). Calculated Bader's charges confirm the ionic character of Ln–O bonds in the C-type Ln 2 O 3 . Estimated structural parameters (i.e., lattice constants) coincide with analogous experimental values. The calculated band gaps energies at the U eff of 5 eV for these compounds exhibit a non-metallic character and U eff of 6.5 eV reproduces the analogous experimental band gap of cerium sesquioxide Ce 2 O 3 . We have thoroughly investigated the effect of the O/Ce ratios and the effect of hafnium (Hf) and zirconium (Zr) dopants on the reduction energies of CeO x configurations. Our analysis for the reduction energy of CeO 2 , over a wide range of temperatures displays that, shuffling between the two +4 and +3 oxidation states of Ce exhibit a temperature-independent behaviour. Higher O/Ce ratios necessitate lower reduction energies. Our results on Ce–Hf–Zr–O alloys are in reasonable agreements with analogous fitted values pertinent to lowering reduction energies and shrinkage in lattice parameters when contrasted with pure CeO 2 . Structural analysis reveals that Hf and Zr atoms in the solid solution are shifted towards the nearest vacancies upon reduction. It is hoped that values provided herein to shed an atomic-base insight into the reduction/oxidation thermodynamics of increasingly deployed catalysts for environmental applications.

KW - Density functional theory

KW - Lanthanum oxide

KW - Mechanical stability

KW - Reduction energy

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Miran HA, Altarawneh M, Widjaja H, Jaf ZN, Mahbubur Rahman M, Veder JP et al. Thermo-mechanical properties of cubic lanthanide oxides. Thin Solid Films. 2018 May 1;653:37-48. https://doi.org/10.1016/j.tsf.2018.01.063