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Title: Non-stoichiometry in U3Si2

Abstract

Uranium silicides, in particular U3Si2, are being explored as an advanced nuclear fuel with increased accident tolerance as well as competitive economics compared to the baseline UO2 fuel. Here we use density functional theory calculations and thermochemical analysis to assess the stability of U3Si2 with respect to non-stoichiometry reactions in both the hypo- and hyper-stoichiometric regimes. We find that the degree of non-stoichiometry in U3Si2 is much smaller than in UO2 and at most reaches a few percent at high temperature. Non-stoichiometry impacts fuel performance by determining whether the loss of uranium due to fission leads to a non-stoichiometric U3Si2±x phase or precipitation of a second U-Si phase. Lastly, we also investigate the U5Si4 phase as a candidate for the equilibrium phase diagram.

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [4]
  1. Westinghouse Electric Sweden AB, Vasteras (Sweden); Imperial College London, London (United Kingdom)
  2. Imperial College London, London (United Kingdom)
  3. Westinghouse Electric Co. LLC, Cranberry Woods, PA (United States)
  4. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1343721
Alternate Identifier(s):
OSTI ID: 1396826
Report Number(s):
LA-UR-17-20854
Journal ID: ISSN 0022-3115; TRN: US1701554
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Nuclear Materials
Additional Journal Information:
Journal Volume: 482; 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; accident tolerant fuel; density functional theory; stoichiometry; silicide

Citation Formats

Middleburgh, Simon C., Grimes, Robin W., Lahoda, Ed J., Stanek, Christopher Richard, and Andersson, David A. Non-stoichiometry in U3Si2. United States: N. p., 2016. Web. https://doi.org/10.1016/j.jnucmat.2016.10.016.
Middleburgh, Simon C., Grimes, Robin W., Lahoda, Ed J., Stanek, Christopher Richard, & Andersson, David A. Non-stoichiometry in U3Si2. United States. https://doi.org/10.1016/j.jnucmat.2016.10.016
Middleburgh, Simon C., Grimes, Robin W., Lahoda, Ed J., Stanek, Christopher Richard, and Andersson, David A. Sat . "Non-stoichiometry in U3Si2". United States. https://doi.org/10.1016/j.jnucmat.2016.10.016. https://www.osti.gov/servlets/purl/1343721.
@article{osti_1343721,
title = {Non-stoichiometry in U3Si2},
author = {Middleburgh, Simon C. and Grimes, Robin W. and Lahoda, Ed J. and Stanek, Christopher Richard and Andersson, David A.},
abstractNote = {Uranium silicides, in particular U3Si2, are being explored as an advanced nuclear fuel with increased accident tolerance as well as competitive economics compared to the baseline UO2 fuel. Here we use density functional theory calculations and thermochemical analysis to assess the stability of U3Si2 with respect to non-stoichiometry reactions in both the hypo- and hyper-stoichiometric regimes. We find that the degree of non-stoichiometry in U3Si2 is much smaller than in UO2 and at most reaches a few percent at high temperature. Non-stoichiometry impacts fuel performance by determining whether the loss of uranium due to fission leads to a non-stoichiometric U3Si2±x phase or precipitation of a second U-Si phase. Lastly, we also investigate the U5Si4 phase as a candidate for the equilibrium phase diagram.},
doi = {10.1016/j.jnucmat.2016.10.016},
journal = {Journal of Nuclear Materials},
number = C,
volume = 482,
place = {United States},
year = {2016},
month = {10}
}

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Cited by: 5 works
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    A first-principles study on the influences of metal species Al, Zr, Mo and Tc on the mechanical properties of U 3 Si 2
    journal, January 2020

    • Gao, Haigen; Liu, Yande; Hu, Jun
    • Physical Chemistry Chemical Physics, Vol. 22, Issue 4
    • DOI: 10.1039/c9cp03814k