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Modeling of Ce2, Ce2O3 ,and CeO2-x in the LDA+U formalism
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering.
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2007 (English)In: Physical Review B Condensed Matter, ISSN 0163-1829, E-ISSN 1095-3795, Vol. 75, no 3, 035109- p.Article in journal (Refereed) Published
Abstract [sv]

The electronic structure and thermodynamic properties of CeO2 and Ce2O3 have been studied from first principles by the all-electron projector-augmented-wave (PAW) method, as implemented in the ab initio total-energy and molecular-dynamics program VASP (Vienna ab initio simulation package). The local density approximation (LDA)+U formalism has been used to account for the strong on-site Coulomb repulsion among the localized Ce 4f electrons. We discuss how the properties of CeO2 and Ce2O3 are affected by the choice of U as well as the choice of exchange-correlation potential, i.e., the local density approximation or the generalized gradient approximation. Further, reduction of CeO2, leading to formation of Ce2O3 and CeO2-x, and its dependence on U and exchange-correlation potential have been studied in detail. Our results show that by choosing an appropriate U it is possible to consistently describe structural, thermodynamic, and electronic properties of CeO2, Ce2O3, and CeO2-x, which enables modeling of redox processes involving ceria-based materials.

Place, publisher, year, edition, pages
2007. Vol. 75, no 3, 035109- p.
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
URN: urn:nbn:se:kth:diva-6888DOI: 10.1103/PhysRevB.75.035109ISI: 000243895400042Scopus ID: 2-s2.0-33846442083OAI: oai:DiVA.org:kth-6888DiVA: diva2:11728
Note
QC 20100622Available from: 2007-03-14 Created: 2007-03-14 Last updated: 2017-12-14Bibliographically approved
In thesis
1. From the Electronic Structure of Point Defects to Functional Properties of Metals and Ceramics
Open this publication in new window or tab >>From the Electronic Structure of Point Defects to Functional Properties of Metals and Ceramics
2007 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

Point defects are an inherent part of crystalline materials and they influence important physical and chemical properties, such as diffusion, hardness, catalytic activity and phase stability. Increased understanding of point defects enables us to tailor the defect-related properties to the application at hand. Modeling and simulation have a prominent role in acquiring this knowledge. In this thesis thermodynamic and kinetic properties of point defects in metals and ceramics are studied using first-principles calculations based on density functional theory. Phenomenological models are used to translate the atomic level properties, obtained from the first-principles calculations, into functional materials properties. The next paragraph presents the particular problems under study.

The formation and migration of vacancies and simple vacancy clusters in copper are investigated by calculating the energies associated with these processes. The structure, stability and electronic properties of the low-oxygen oxides of titanium, TiOx with 1/3 < x < 3/2, are studied and the importance of structural vacancies is demonstrated. We develop an integrated first-principles and Calphad approach to calculate phase diagrams in the titanium-carbon-nitrogen system, with particular focus on vacancy-induced ordering of the substoichiometric

carbonitride phase, TiCxNy (x+y < 1). The possibility of forming higher oxides of plutonium than plutonium dioxide is explored by calculating the enthalpies for nonstoichiometric defect-containing compounds and the analysis shows that such oxidation is only produced by strong oxidants. For ceria (CeO2) doped with trivalent ions from the lanthanide series we probe the connection between the choice of a dopant and the improvement of ionic conductivity by studying the oxygen-vacancy formation and migration properties. The significance of minimizing the dopant-vacancy interactions is highlighted. We investigate the redox thermodynamics of CeO2-MO2 solid solutions with M being Ti, Zr, Hf, Th, Si, Ge, Sn or Pb and show that reduction is facilitated by small solutes.

The results in this thesis are relevant for the performance of solid electrolytes, which are an integral part of solid oxide fuel cells, oxygen storage materials in automotive three-way catalysts, nuclear waste materials and cutting tool materials.

Place, publisher, year, edition, pages
Stockholm: Materialvetenskap, 2007
Keyword
first principles, ab initio, density functional theory, Calphad, point defects, diffusion, solid electrolytes, oxygen storage materials
National Category
Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:kth:diva-4309 (URN)978-91-7178-590-9 (ISBN)
Public defence
2007-03-30, F2, Lindstedtsvägen 26, Stockholm, 10:00
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Note
QC 20100622Available from: 2007-03-14 Created: 2007-03-14 Last updated: 2012-03-22Bibliographically approved

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