Kinetic lattice Monte Carlo model for oxygen vacancy diffusion in praseodymium doped ceria: Applications to materials design

Pratik P. Dholabhai, Shahriar Anwar, James Adams, Peter Crozier, Renu Sharma

Research output: Contribution to journalArticlepeer-review

44 Scopus citations

Abstract

Kinetic lattice Monte Carlo (KLMC) model is developed for investigating oxygen vacancy diffusion in praseodymium-doped ceria. The current approach uses a database of activation energies for oxygen vacancy migration, calculated using first-principles, for various migration pathways in praseodymium-doped ceria. Since the first-principles calculations revealed significant vacancyvacancy repulsion, we investigate the importance of that effect by conducting simulations with and without a repulsive interaction. Initially, as dopant concentrations increase, vacancy concentration and thus conductivity increases. However, at higher concentrations, vacancies interfere and repel one another, and dopants trap vacancies, creating a traffic jam that decreases conductivity, which is consistent with the experimental findings. The modeled effective activation energy for vacancy migration slightly increased with increasing dopant concentration in qualitative agreement with the experiment. The current methodology comprising a blend of first-principle calculations and KLMC model provides a very powerful fundamental tool for predicting the optimal dopant concentration in ceria related materials.

Original languageEnglish (US)
Pages (from-to)811-817
Number of pages7
JournalJournal of Solid State Chemistry
Volume184
Issue number4
DOIs
StatePublished - Apr 1 2011

Keywords

  • DFTU
  • Ionic conductivity
  • Kinetic lattice Monte Carlo
  • Oxygen vacancy diffusion
  • Pr-doped ceria

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Ceramics and Composites
  • Condensed Matter Physics
  • Physical and Theoretical Chemistry
  • Inorganic Chemistry
  • Materials Chemistry

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