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Tuning Oxide Properties by Oxygen Vacancy Control During Growth and Annealing
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Oxygen vacancy formation and migration in Ce(x)Th(1-x)O2 solid solution.

H Y Xiao1, W J Weber

  • 1Department of Materials Science & Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States.

The Journal of Physical Chemistry. B
|May 6, 2011
PubMed
Summary
This summary is machine-generated.

Introducing cerium dioxide (CeO2) into thorium dioxide (ThO2) significantly lowers oxygen vacancy formation and migration energies. This suggests CeO2 enhances oxygen mobility in ThO2-based materials.

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Computational Materials Science

Background:

  • Thorium dioxide (ThO2) and cerium dioxide (CeO2) are important ceramic materials.
  • Understanding oxygen vacancy behavior is crucial for applications like solid oxide fuel cells and catalysis.
  • The electronic and magnetic properties of mixed oxides are influenced by composition.

Purpose of the Study:

  • To investigate the effect of CeO2 addition on oxygen vacancy formation and migration in ThO2.
  • To explore the electronic and magnetic properties of Ce(x)Th(1-x)O(2) solid solutions.
  • To determine the optimal CeO2 content for enhanced oxygen mobility and tunable magnetic properties.

Main Methods:

  • Employed the local-density approximation with the Hubbard U correction (LDA+U) method for electronic structure calculations.
  • Calculated oxygen vacancy formation energies across various CeO2 concentrations.
  • Calculated oxygen vacancy migration energies to assess mobility.
  • Investigated magnetic ordering (antiferromagnetic vs. ferromagnetic) as a function of CeO2 content.

Main Results:

  • Addition of CeO2 significantly decreases oxygen vacancy formation and migration energies in ThO2.
  • The lowest formation energy (3.7 eV) was observed for 50% CeO2 content.
  • The lowest migration energy (0.2 eV) occurred at 75% CeO2 content, indicating enhanced oxygen mobility.
  • Reduced Ce(x)Th(1-x)O(2) exhibits antiferromagnetic ordering for <35% CeO2 and ferromagnetic ordering for >35% CeO2.

Conclusions:

  • Introducing CeO2 into ThO2 promotes the formation of mobile oxygen vacancies.
  • The composition of Ce(x)Th(1-x)O(2) can be tailored to control oxygen vacancy mobility.
  • Varying the CeO2 content allows for tuning the magnetic properties of the material, transitioning from antiferromagnetic to ferromagnetic states.