Density functional theory calculations of self- and Xe diffusion in U3Si2

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Dangosydd eitem ddigidol (DOI)

  • Simon Middleburgh
  • David Andersson
    Los Alamos National Laboratory
  • Chris Stanek
    Los Alamos National Laboratory
  • Antoine Claisse
    Westinghouse Electric Sweden AB
  • Ben Beeler
    Idaho National Laboratory
  • X-Y Liu
    Los Alamos National Laboratory
Uranium silicide, U3Si2, has been proposed as an advanced nuclear fuel to be used in light water reactors (LWRs). Development of this alternative to the predominant current fuel, UO2, is motivated by enhanced accident tolerance as a result of higher thermal conductivity as well as improved fuel cycle economics through increased uranium density. In order to accurately model the fuel performance of U3Si2, the diffusion rate of point defects, which is related to self-diffusion, and of fission gas atoms must be determined. DFT calculations are used to predict the U and Si point defect concentrations, the corresponding self-diffusivities, the preferred Xe trap site and the Xe diffusivity. Effects of irradiation are not considered. A low defect formation energy and a high entropy for Si interstitials give rise to Si-rich non-stoichiometry at elevated temperatures. Both U and Si self-diffusion and Xe diffusion are anisotropic as a consequence of the tetragonal crystal structure of U3Si2. Si diffusion occurs by interstitial mechanisms in both the a-b plane and along the c axis, while the U c axis diffusion rate is controlled by a vacancy mechanism. Interstitial diffusion of U is very fast in the a-b plane of the U3Si2 crystal structure. Xe atoms prefer to occupy U vacancy trap sites. The highest Xe diffusion rate occurs by a vacancy mechanism in both the a-b plane and along the c axis. The diffusion rate is similar in the a-b plane and along the c axis. U and Si self-diffusion and Xe diffusion are all faster in U3Si2 than intrinsic U and Xe diffusion in conventional UO2 nuclear fuel.
Iaith wreiddiolSaesneg
Tudalennau (o-i)312-325
Nifer y tudalennau14
CyfnodolynJournal of Nuclear Materials
Cyfrol515
Dyddiad ar-lein cynnar21 Rhag 2018
Dynodwyr Gwrthrych Digidol (DOIs)
StatwsCyhoeddwyd - Maw 2019

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