Abstract

Oxygen ion conductivity of doped ceria is observed to be two-three orders of magnitude higher than yttria stabilized zirconia, the most widely used solid electrolyte material at temperatures below 600°C. Gadolinium doped ceria (GDC) is known to be one of the most promising solid electrolyte materials for operation of solid oxide fuel cells below 600°C. To understand the atomic defect migration in GDC, we have used total energy calculations within the framework of density functional theory to follow oxygen vacancy migration in GDC. We report activation energies for various oxygen vacancy migration pathways in GDC. Oxygen vacancy formation and migration were evaluated for first, second, and third nearest neighbor positions to a Gd3+ ion. Due to the comparable ionic radii of Gd3+ and host Ce4+ ions, the first nearest neighbor site with respect to the dopant cation is found to be the most favorable oxygen vacancy formation site. The migration pathway where the vacancy migrates from a second to first nearest neighbor is found to be most favorable. The calculated activation energies for oxygen vacancy migration in GDC are compared against the reported measured and calculated values from the literature. This work will provide a foundation for the development of a kinetic lattice Monte Carlo model for vacancy diffusion in GDC, which will improve the understanding of oxygen ion conductivity in doped ceria.

Original languageEnglish (US)
Pages (from-to)7904-7910
Number of pages7
JournalPhysical Chemistry Chemical Physics
Volume12
Issue number28
DOIs
StatePublished - Jul 28 2010

Fingerprint

Cerium compounds
Gadolinium
gadolinium
Oxygen vacancies
Defects
defects
oxygen
Ions
solid electrolytes
oxygen ions
Solid electrolytes
Vacancies
activation energy
Activation energy
conductivity
Oxygen
solid oxide fuel cells
yttria-stabilized zirconia
Yttria stabilized zirconia
Solid oxide fuel cells (SOFC)

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Physics and Astronomy(all)

Cite this

A density functional study of defect migration in gadolinium doped ceria. / Dholabhai, Pratik P.; Adams, James; Crozier, Peter; Sharma, Renu.

In: Physical Chemistry Chemical Physics, Vol. 12, No. 28, 28.07.2010, p. 7904-7910.

Research output: Contribution to journalArticle

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