Mechanisms of temperature-dependent oxygen absorption/release and appearance of intermediate phase in κ-Ce 2 Zr 2 O 8 : study based on oxygen vacancy formation energy computations.

This study clarified the mechanisms of the temperature-dependent oxygen absorption/release properties and appearance of the intermediate phase for κ-Ce 2 Zr 2 O 8 , which is known to have a high oxygen storage/release capacity (OSC). First-principle computations revealed that the vacancy formation energies depend on the number of vacancies and can be categorized into two groups: low-energy and high-energy. The intermediate phase observed experimentally was assigned to the state after all the oxygen vacancies in the low-energy group were formed. We also found that the mechanism of the improved OSC performance by Ti substitution could be explained in terms of the vacancy formation energies.