TY - JOUR
T1 - Kinetic lattice Monte Carlo model for oxygen vacancy diffusion in praseodymium doped ceria
T2 - Applications to materials design
AU - Dholabhai, Pratik P.
AU - Anwar, Shahriar
AU - Adams, James
AU - Crozier, Peter
AU - Sharma, Renu
N1 - Funding Information:
This paper is based on the work supported by the Department of Energy under the Grant no. DE-PS02-06ER06-17 . The authors gratefully acknowledge the Fulton High Performance Computing Initiative (HPCI) at the Arizona State University for the computational resources.
PY - 2011/4
Y1 - 2011/4
N2 - 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.
AB - 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.
KW - DFTU
KW - Ionic conductivity
KW - Kinetic lattice Monte Carlo
KW - Oxygen vacancy diffusion
KW - Pr-doped ceria
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U2 - 10.1016/j.jssc.2011.02.004
DO - 10.1016/j.jssc.2011.02.004
M3 - Article
AN - SCOPUS:79953665351
SN - 0022-4596
VL - 184
SP - 811
EP - 817
JO - Journal of Solid State Chemistry
JF - Journal of Solid State Chemistry
IS - 4
ER -