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Ordering and phase separation in Gd-doped ceria: a combined DFT, cluster expansion and Monte Carlo study
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory. KTH Royal Inst Technol, Dept Mat Sci & Engn, S-10044 Stockholm, Sweden..
KTH Royal Inst Technol, Dept Mat Sci & Engn, S-10044 Stockholm, Sweden.;Mat Ctr Leoben Forsch GmbH, A-8700 Leoben, Austria..
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory. KTH Royal Inst Technol, Dept Mat Sci & Engn, S-10044 Stockholm, Sweden..
2017 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 19, no 39, 26606-26620 p.Article in journal (Refereed) Published
Abstract [en]

Ordering of dopants and oxygen vacancies is studied for Gd-doped ceria (x(Gd) <= 0.25) by means of a combined density functional theory (DFT) and cluster expansion approach, where the cluster interactions derived from DFT calculations are further used in Monte Carlo simulations. The methodology is meticulously tested and the stability of the obtained solutions with respect to the volume change, applied exchange-correlation approximation and other modelling parameters is carefully analysed. We study Gd and vacancy ordering in the case of thermodynamic equilibrium and vacancy ordering for quenched Gd configurations. We find that at the thermodynamic equilibrium there exists a transition temperature (T-C) below which phase separation into C-type Gd2O3 and pure CeO2 occurs. The phase separation is observed in the whole studied concentration range and the transition temperature increases with concentration from ca. 600 (x(Gd) = 0.03) to 1000 K (x(Gd) = 0.25). Above T-C the distribution of Gd is random, oxygen vacancies tend to cluster in the coordination shells along < 1, 1/2, 0 > and < 1, 1, 1 >, and the nearest neighbour position is preferred for Gd-vacancy. In the quenched Gd case, where Gd atoms are immobilised below 1500 K, the vacancy ordering is significantly frustrated. In fact, we observe an oxygen freezing transition below temperature T-F approximate to T-C - 350 K, which is close to temperatures at which a change in the conductivity slope is observed experimentally.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY , 2017. Vol. 19, no 39, 26606-26620 p.
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-337327DOI: 10.1039/c7cp04106cISI: 000412763700014PubMedID: 28949350OAI: oai:DiVA.org:uu-337327DiVA: diva2:1170216
Funder
Swedish Research Council, VR 348-2012-6196
Available from: 2018-01-02 Created: 2018-01-02 Last updated: 2018-01-02Bibliographically approved

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Zguns, Pjotrs A.Skorodumova, Natalia V.

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