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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:
Journal Article: 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. doi: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. 2016. "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},
url = {https://www.osti.gov/biblio/1343721}, journal = {Journal of Nuclear Materials},
issn = {0022-3115},
number = C,
volume = 482,
place = {United States},
year = {Sat Oct 08 00:00:00 EDT 2016},
month = {Sat Oct 08 00:00:00 EDT 2016}
}

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Cited by: 45 works
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Works referenced in this record:

Thermophysical properties of U 3 Si 2 to 1773 K
journal, September 2015


Structural chemistry and magnetic behavior of binary uranium silicides
journal, April 1992


O-U (Oxygen-Uranium)
journal, July 2007


Thermodynamic assessment of the uranium–oxygen system
journal, August 2002


The chemical state of the fission products in oxide fuels
journal, April 1985


Vacancy mediated cation migration in uranium dioxide: The influence of cluster configuration
journal, November 2014


Partition of soluble fission products between the grey phase, ZrO2 and uranium dioxide
journal, July 2013


Uranium silicide pellet fabrication by powder metallurgy for accident tolerant fuel evaluation and irradiation
journal, November 2015


Fabrication and microstructural analysis of UN-U3Si2 composites for accident tolerant fuel applications
journal, August 2016


Characteristics of U 3 Si and U 3 Si 2 Powders Prepared by Centrifugal Atomization
journal, December 1997


Phase equilibria in the U-Si system from first-principles calculations
journal, October 2016


Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998


First-principles investigations on the electronic structures of U3Si2
journal, February 2016


Ab initiomolecular dynamics for liquid metals
journal, January 1993


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Crystal chemical studies of the 5f-series of elements. I. New structure types
journal, November 1948


Structure and phase stability of uranium–silicon U 3 Si at low temperatures
journal, October 1980


SGTE data for pure elements
journal, October 1991


Relations between the concentrations of imperfections in solids
journal, May 1958


The defect chemistry of sapphire (α-Al2O3)
journal, October 1998


Structural stability and fission product behaviour in U3Si
journal, November 2015


Neutron irradiation induced amorphization of uranium silicides
journal, December 1997


Microstructure of U3Si2 fuel plates submitted to a high heat flux
journal, May 2004


Irradiation behaviour of uranium silicide compounds
journal, February 2004


Structure, properties and formation of PuCrO3 and PuAlO3 of relevance to doped nuclear fuels
journal, January 2013


Effect of pores and He bubbles on the thermal transport properties of UO2 by molecular dynamics simulation
journal, January 2015


Works referencing / citing this record:

Uranium nitride-silicide advanced nuclear fuel: higher efficiency and greater safety
journal, October 2018


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