Diffusion in undoped and Cr-doped amorphous UO2

Owen, Megan W.; Cooper, Michael William Donald; Rushton, Michael J.D.; Claisse, Antoine; Lee, William E.; Middleburgh, Simon C.

doi:10.1016/j.jnucmat.2023.154270

Title: Diffusion in undoped and Cr-doped amorphous UO₂

Journal Article · Fri Jan 13 00:00:00 EST 2023 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2023.154270· OSTI ID:1922030

^[1];

^[2]; Rushton, Michael J.D. ^[1]; Claisse, Antoine ^[3]; Lee, William E. ^[1];

^[1]

Bangor University (United Kingdom)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Westinghouse Electric (Sweden)

UO₂ fuel pellets are often doped with chromium oxide to obtain favourable properties such as higher density, improved thermal stability, large grain sizes, improved pellet-clad interaction margins, and increased fission gas retention during transients. Chromium has a low solubility limit in UO₂, with past experimental work reporting solubility limits ranging between 0.004 to 0.06 wt.% Cr. Due to its low solubility, segregation of Cr ions to the grain boundary may occur. Further, the complexity of these boundaries may be high as observed in other ceramics resulting in disordered or amorphous regions along the boundary, affecting a range of material and operational properties of the fuel pellet. To assess these disordered regions, in this work we study amorphous undoped and Cr doped UO₂ systems (containing 10–50 at.% Cr³⁺) that have been modelled using classical molecular dynamics methods incorporating Cr³⁺ into the well-used CRG potential library. Diffusion coefficients, pre-exponential factors, and activation energies for diffusion were computed for oxygen ions, assessing the impact of structure and extrinsic species on migration. Oxygen diffusion was observed to be much faster in the undoped amorphous system compared to its crystalline counterpart. Oxygen diffusion in doped systems decreased with increasing Cr concentration, highlighting the importance of additives to retain fission products and other migratory species.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1922030

Report Number(s):: LA-UR-22-30021; TRN: US2312260

Journal Information:: Journal of Nuclear Materials, Vol. 576; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (47)

Effect of Dopants on Zirconia Stabilization-An X-ray Absorption Study: I, Trivalent Dopants Li, Ping; Chen, I-Wei; Penner-Hahn, James E. Journal of the American Ceramic Society, Vol. 77, Issue 1 https://doi.org/10.1111/j.1151-2916.1994.tb06964.x	journal	January 1994
Effect of grain-boundaries on uranium and oxygen diffusion in polycrystalline UO2 Sabioni, A. C. S.; Ferraz, W. B.; Millot, F. Journal of Nuclear Materials, Vol. 278, Issue 2-3 https://doi.org/10.1016/S0022-3115(99)00250-0	journal	April 2000
The elastic constants and distance dependence of the magnetic interactions of Cr2O3 Alberts, H. L.; Boeyens, J. C. A. Journal of Magnetism and Magnetic Materials, Vol. 2, Issue 4 https://doi.org/10.1016/0304-8853(76)90044-5	journal	July 1976
The chemical state of the fission products in oxide fuels Kleykamp, H. Journal of Nuclear Materials, Vol. 131, Issue 2-3, p. 221-246 https://doi.org/10.1016/0022-3115(85)90460-X	journal	April 1985
Thermophysical and anion diffusion properties of (U _x ,Th _{1− x} )O ₂ Cooper, Michael W. D.; Murphy, Samuel T.; Fossati, Paul C. M. Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 470, Issue 2171 https://doi.org/10.1098/rspa.2014.0427	journal	November 2014
Die thermische Ausdehnung der isotypen Mischreihen-Endglieder Cr2O3 und ?-Al3O2, ermittelt mit einer neuen, lichtstarken Seemann?Bohlin-Kammer Kudielka, Heinz Monatshefte f�r Chemie, Vol. 103, Issue 1 https://doi.org/10.1007/BF00912929	journal	January 1972
Atomsk: A tool for manipulating and converting atomic data files Hirel, Pierre Computer Physics Communications, Vol. 197 https://doi.org/10.1016/j.cpc.2015.07.012	journal	December 2015
A many-body potential approach to modelling the thermomechanical properties of actinide oxides Cooper, M. W. D.; Rushton, M. J. D.; Grimes, R. W. Journal of Physics: Condensed Matter, Vol. 26, Issue 10 https://doi.org/10.1088/0953-8984/26/10/105401	journal	February 2014
Structure and properties of amorphous uranium dioxide Middleburgh, Simon C.; Lee, William E.; Rushton, Michael J. D. Acta Materialia, Vol. 202 https://doi.org/10.1016/j.actamat.2020.10.069	journal	January 2021
A charge-optimized many-body potential for the U–UO ₂ –O ₂ system Li, Yangzhong; Liang, Tao; Sinnott, Susan B. Journal of Physics: Condensed Matter, Vol. 25, Issue 50 https://doi.org/10.1088/0953-8984/25/50/505401	journal	November 2013
Vacancy mediated cation migration in uranium dioxide: The influence of cluster configuration Cooper, M. W. D.; Middleburgh, S. C.; Grimes, R. W. Solid State Ionics, Vol. 266 https://doi.org/10.1016/j.ssi.2014.08.010	journal	November 2014
Chromium Doped UO2-Based Ceramics: Synthesis and Characterization of Model Materials for Modern Nuclear Fuels Kegler, Philip; Klinkenberg, Martina; Bukaemskiy, Andrey Materials, Vol. 14, Issue 20 https://doi.org/10.3390/ma14206160	journal	October 2021
On the solubility of chromium sesquioxide in uranium dioxide fuel Leenaers, A.; de Tollenaere, L.; Delafoy, Ch Journal of Nuclear Materials, Vol. 317, Issue 1 https://doi.org/10.1016/S0022-3115(02)01693-8	journal	April 2003
First study of uranium self-diffusion in UO2 by SIMS Sabioni, A. C. S.; Ferraz, W. B.; Millot, F. Journal of Nuclear Materials, Vol. 257, Issue 2 https://doi.org/10.1016/S0022-3115(98)00482-6	journal	November 1998
Formation of (Cr,Al)UO4 from doped UO2 and its influence on partition of soluble fission products Cooper, M. W. D.; Gregg, D. J.; Zhang, Y. Journal of Nuclear Materials, Vol. 443, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.07.038	journal	November 2013
Neutron Diffraction Study of the in Situ Oxidation of UO ₂ Desgranges, Lionel; Baldinozzi, Gianguido; Rousseau, Gurvan Inorganic Chemistry, Vol. 48, Issue 16 https://doi.org/10.1021/ic9000889	journal	August 2009
Thermoelastic properties of chromium oxide Cr2O3 (eskolaite) at high pressures and temperatures Dymshits, Anna M.; Dorogokupets, Peter I.; Sharygin, Igor S. Physics and Chemistry of Minerals, Vol. 43, Issue 6 https://doi.org/10.1007/s00269-016-0808-7	journal	March 2016
Influence of trivalent doping on point and Frenkel defect formation in bulk chromium (III) oxide Carey, John J.; Nolan, Michael Solid State Ionics, Vol. 307 https://doi.org/10.1016/j.ssi.2017.04.016	journal	September 2017
Diffusion in doped and undoped amorphous zirconia Owen, Megan W.; Rushton, Michael J. D.; Evitts, Lee J. Journal of Nuclear Materials, Vol. 555 https://doi.org/10.1016/j.jnucmat.2021.153108	journal	November 2021
Post-irradiation examination of high burnup Mg doped UO2 in comparison with undoped UO2, Mg–Nb doped UO2 and Ti doped UO2 Fujino, Takeo; Shiratori, Tetsuo; Sato, Nobuaki Journal of Nuclear Materials, Vol. 297, Issue 2 https://doi.org/10.1016/S0022-3115(01)00609-2	journal	August 2001
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
The calculation of defect parameters in UO ₂ Jackson, R. A.; Murray, A. D.; Harding, J. H. Philosophical Magazine A, Vol. 53, Issue 1 https://doi.org/10.1080/01418618608242805	journal	January 1986
GULP: A computer program for the symmetry-adapted simulation of solids Gale, Julian D. Journal of the Chemical Society, Faraday Transactions, Vol. 93, Issue 4 https://doi.org/10.1039/a606455h	journal	January 1997
Crystallographic and magnetic studies of mesoporous eskolaite, Hill, Adrian H.; Harrison, Andrew; Dickinson, Calum Microporous and Mesoporous Materials, Vol. 130, Issue 1-3 https://doi.org/10.1016/j.micromeso.2009.11.021	journal	May 2010
Oxygen chemical diffusion coefficient in hyperstoichiometric uranium dioxide Taskinen, A.; Kuliberg, H. Journal of Nuclear Materials, Vol. 83, Issue 2 https://doi.org/10.1016/0022-3115(79)90620-2	journal	September 1979
Grain Boundaries in Uranium Dioxide: Scanning Electron Microscopy Experiments and Atomistic Simulations: Grain Boundaries in Uranium Dioxide Nerikar, Pankaj V.; Rudman, Karin; Desai, Tapan G. Journal of the American Ceramic Society, Vol. 94, Issue 6 https://doi.org/10.1111/j.1551-2916.2010.04295.x	journal	January 2011
Experimental and simulation study of grain boundaries in UO2 Bourasseau, Emeric; Mouret, Alexandre; Fantou, Paul Journal of Nuclear Materials, Vol. 517 https://doi.org/10.1016/j.jnucmat.2019.02.033	journal	April 2019
Visualization and analysis of atomistic simulation data with OVITO–the Open Visualization Tool Stukowski, Alexander Modelling and Simulation in Materials Science and Engineering, Vol. 18, Issue 1 https://doi.org/10.1088/0965-0393/18/1/015012	journal	December 2009
Solution of trivalent cations into uranium dioxide Middleburgh, S. C.; Parfitt, D. C.; Grimes, R. W. Journal of Nuclear Materials, Vol. 420, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2011.10.006	journal	January 2012
Segregation of xenon to dislocations and grain boundaries in uranium dioxide Nerikar, P. V.; Parfitt, D. C.; Casillas Trujillo, L. A. Physical Review B, Vol. 84, Issue 17 https://doi.org/10.1103/PhysRevB.84.174105	journal	November 2011
Multiscale simulation of xenon diffusion and grain boundary segregation in UO2 Andersson, David A.; Tonks, Michael R.; Casillas, Luis Journal of Nuclear Materials, Vol. 462 https://doi.org/10.1016/j.jnucmat.2015.03.019	journal	July 2015
Oxygen diffusion in yttria stabilised zirconia—experimental results and molecular dynamics calculations Kilo, Martin; Argirusis, Christos; Borchardt, Günter Phys. Chem. Chem. Phys., Vol. 5, Issue 11 https://doi.org/10.1039/B300151M	journal	January 2003
Physics-based modelling of fission gas swelling and release in UO2 applied to integral fuel rod analysis Pastore, Giovanni; Luzzi, Lelio; Di Marcello, Valentino Nuclear Engineering and Design, Vol. 256 https://doi.org/10.1016/j.nucengdes.2012.12.002	journal	March 2013
A Simplex Method for Function Minimization Nelder, J. A.; Mead, R. The Computer Journal, Vol. 7, Issue 4 https://doi.org/10.1093/comjnl/7.4.308	journal	January 1965
Oxygen diffusion in UO2, ThO2 and PuO2. A review Murch, G. E.; Catlow, C. Richard A. Journal of the Chemical Society, Faraday Transactions 2, Vol. 83, Issue 7 https://doi.org/10.1039/f29878301157	journal	January 1987
Advanced Doped UO ₂ Pellets in LWR Applications Arborelius, Jakob; Backman, Karin; Hallstadius, Lars Journal of Nuclear Science and Technology, Vol. 43, Issue 9 https://doi.org/10.1080/18811248.2006.9711184	journal	September 2006
Effects of Gadolinium Doping on Electrical Properties of U02 Grain Boundaries Kubo, Toshio; Ishimoto, Shinji; Ama, Takao KOY Journal of Nuclear Science and Technology, Vol. 30, Issue 7 https://doi.org/10.1080/18811248.1993.9734532	journal	July 1993
Defect segregation facilitates oxygen transport at fluorite UO ₂ grain boundaries Symington, A. R.; Molinari, M.; Brincat, N. A. Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2152 https://doi.org/10.1098/rsta.2019.0026	journal	July 2019
The van Hove distribution function for Brownian hard spheres: Dynamical test particle theory and computer simulations for bulk dynamics Hopkins, Paul; Fortini, Andrea; Archer, Andrew J. The Journal of Chemical Physics, Vol. 133, Issue 22 https://doi.org/10.1063/1.3511719	journal	December 2010
The effect of additives on the irradiation behaviour of UO2 Killeen, J. C. Journal of Nuclear Materials, Vol. 58, Issue 1 https://doi.org/10.1016/0022-3115(75)90164-6	journal	October 1975
The role of charge and ionic radius on fission product segregation to a model UO ₂ grain boundary Hong, Minki; Uberuaga, Blas P.; Phillpot, Simon R. Journal of Applied Physics, Vol. 113, Issue 13 https://doi.org/10.1063/1.4798347	journal	April 2013
Doping UO2 with niobia — Beneficial or not? Assmann, H.; Dörr, W.; Gradel, G. Journal of Nuclear Materials, Vol. 98, Issue 1-2 https://doi.org/10.1016/0022-3115(81)90401-3	journal	May 1981
Grain boundary complexions Cantwell, Patrick R.; Tang, Ming; Dillon, Shen J. Acta Materialia, Vol. 62 https://doi.org/10.1016/j.actamat.2013.07.037	journal	January 2014
The crystallization of amorphous UO2 Matzke, H. J.; Nitzki, V.; Ronchi, C. Thin Solid Films, Vol. 22, Issue 1 https://doi.org/10.1016/0040-6090(74)90281-8	journal	May 1974
EXAFS and the structure of glass Greaves, G. N. Journal of Non-Crystalline Solids, Vol. 71, Issue 1-3 https://doi.org/10.1016/0022-3093(85)90289-3	journal	May 1985
The defect structure of hyper-stoichiometric uranium dioxide Willis, B. T. M. Acta Crystallographica Section A, Vol. 34, Issue 1 https://doi.org/10.1107/S0567739478000157	journal	January 1978
Atomistic investigation of the structure and transport properties of tilt grain boundaries of UO2 Williams, Nicholas R.; Molinari, Marco; Parker, Stephen C. Journal of Nuclear Materials, Vol. 458 https://doi.org/10.1016/j.jnucmat.2014.11.120	journal	March 2015

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