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Oxygen diffusion in ThO2-CeO2 and ThO2-UO2 solid solutions from atomistic calculations.

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Physical Chemistry Chemical Physics : PCCP
|May 20, 2016
PubMed
Summary

Oxygen diffusivity in Thorium Dioxide-Cerium Dioxide (ThO2-CeO2) and Thorium Dioxide-Uranium Dioxide (ThO2-UO2) solid solutions was studied. Oxygen diffusion is higher in CeO2 and UO2, decreasing with Th addition.

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Area of Science:

  • Materials Science
  • Nuclear Engineering
  • Solid-State Chemistry

Background:

  • Understanding oxygen ion transport in ceramic oxides is crucial for applications like solid oxide fuel cells and nuclear fuels.
  • Thorium Dioxide (ThO2), Cerium Dioxide (CeO2), and Uranium Dioxide (UO2) are important ceramic materials with potential applications in energy technologies.
  • The influence of dopants on oxygen vacancy formation and migration significantly impacts material properties.

Purpose of the Study:

  • To investigate oxygen diffusivity across the entire phase diagram of ThO2-CeO2 and ThO2-UO2 solid solutions.
  • To elucidate the effects of composition and dopant type (tetravalent vs. trivalent) on oxygen migration barriers and vacancy binding energies.
  • To map regions of high oxygen diffusivity within the ThO2-CeO2 and ThO2-UO2 phase diagrams.

Main Methods:

  • Static pair-potential calculations were employed to model atomic interactions.
  • Molecular dynamics simulations were used to simulate oxygen ion transport.
  • Calculations covered the full concentration ranges of the ThO2-CeO2 and ThO2-UO2 phase diagrams.

Main Results:

  • Oxygen diffusivity is higher in CeO2 and UO2 compared to ThO2 due to lower migration barriers.
  • Incorporating Th into CeO2 or UO2 decreases oxygen diffusivity by increasing migration barriers.
  • Adding Ce to ThO2 reduces oxygen diffusion due to vacancy binding, despite decreased migration barriers.
  • Trivalent dopants exhibit stronger binding with oxygen vacancies than tetravalent dopants.
  • Tetravalent dopants with larger ionic radii than the host cation show negative binding energy, unlike trivalent dopants.

Conclusions:

  • The study provides a schematic of high oxygen diffusivity regions in ThO2-CeO2 and ThO2-UO2 phase diagrams.
  • Key differences in oxygen vacancy energetics between trivalent and tetravalent cations were highlighted.
  • Compositional tuning and dopant selection are critical for controlling oxygen transport properties in these oxide systems.