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

Andersson, D. A.; Liu, X. -Y.; Beeler, B.; Middleburgh, S. C.; Claisse, A.; Stanek, C. R.

doi:10.1016/j.jnucmat.2018.12.021

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

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Abstract

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 atomsmore »« less

Authors:

Andersson, D. A. ^[1]; Liu, X. -Y. ^[1]; Beeler, B. ^[2]; Middleburgh, S. C. ^[3]; Claisse, A. ^[4]; Stanek, C. R. ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Idaho National Lab. (INL), Idaho Falls, ID (United States)
Bangor Univ. (United Kingdom)
Westinghouse Electric Sweden, Vasteras (Sweden)

Publication Date:: Fri Dec 21 00:00:00 EST 2018

Research Org.:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE Office of Nuclear Energy (NE)

OSTI Identifier:: 1489979

Alternate Identifier(s):: OSTI ID: 1507802

Report Number(s):: LA-UR-18-28448
Journal ID: ISSN 0022-3115

Grant/Contract Number:: 89233218CNA000001

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Nuclear Materials

Additional Journal Information:: Journal Volume: 515; Journal Issue: C; Journal ID: ISSN 0022-3115

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

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                    Andersson, D. A., Liu, X. -Y., Beeler, B., Middleburgh, S. C., Claisse, A., and Stanek, C. R. Density functional theory calculations of self- and Xe diffusion in U3Si2.  United States: N. p., 2018. 
Web.  doi:10.1016/j.jnucmat.2018.12.021.

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                    Andersson, D. A., Liu, X. -Y., Beeler, B., Middleburgh, S. C., Claisse, A., & Stanek, C. R. Density functional theory calculations of self- and Xe diffusion in U3Si2.  United States.  https://doi.org/10.1016/j.jnucmat.2018.12.021

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                    Andersson, D. A., Liu, X. -Y., Beeler, B., Middleburgh, S. C., Claisse, A., and Stanek, C. R. Fri .  
"Density functional theory calculations of self- and Xe diffusion in U3Si2".  United States.  https://doi.org/10.1016/j.jnucmat.2018.12.021.  https://www.osti.gov/servlets/purl/1489979.

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@article{osti_1489979,

  title        = {Density functional theory calculations of self- and Xe diffusion in U3Si2},

  author       = {Andersson, D. A. and Liu, X. -Y. and Beeler, B. and Middleburgh, S. C. and Claisse, A. and Stanek, C. R.},

  abstractNote = {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.},

  doi          = {10.1016/j.jnucmat.2018.12.021},

  journal      = {Journal of Nuclear Materials},

  number       = C,

  volume       = 515,

  place        = {United States},

  year         = {Fri Dec 21 00:00:00 EST 2018},

  month        = {Fri Dec 21 00:00:00 EST 2018}

}

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

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