Performance and properties evolution of near-term accident tolerant fuel: Cr-doped UO2

Terricabras, Adrien Jose Emile; Drewry, Sean Michael; Campbell, Keri; Judge, Elizabeth J.; Byler, Darrin David; Teti, Emily S.; van Veelen, Arjen; Widgeon Paisner, Scarlett; White, Joshua Taylor

doi:10.1016/j.jnucmat.2024.155022

Performance and properties evolution of near-term accident tolerant fuel: Cr-doped UO₂

Journal Article · Sun Mar 17 00:00:00 EDT 2024 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2024.155022· OSTI ID:2329260

^[1]; ^[2]; ^[1]; Judge, Elizabeth J. ^[1]; Byler, Darrin David ^[1]; ^[1]; ^[1]; ^[1]; White, Joshua Taylor ^[1]

Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Univ. of Tennessee, Knoxville, TN (United States)

Chromium-doped UO₂ fuel has received significant interest due to the ability for chromium to produce pellets with large average grain size (>30 μm), which has shown to increase fission gas retention during operation. Sintering of chromium-doped UO₂ pellets was pursued with oxygen potential and sintering atmosphere controlled to tailor the final microstructure of the material. Chromium additions in this study ranged from 750 to 7800 ppm. Cr concentrations were studied pre and post sintering using Inductively Coupled Plasma Optical Emission Spectroscopy (ICP-OES). Effects of chromium content on lattice parameter and microstructure were examined with X-ray diffraction (XRD) and scanning electron microscopy (SEM). Contraction of the UO₂ lattice parameter was observed, as well as enlargement of grain size with increasing chromium content up to 4900 ppm Cr₂O₃. In addition, SEM indicated Cr incorporation within the matrix and the formation of chromium oxide precipitates throughout the microstructure at high Cr concentrations. Evaluation of thermophysical properties of Cr-doped UO₂ pellets were conducted up to 1200 °C to illustrate their evolution with increased dopant concentration and microstructural changes. The results show that grain size is maximized at 52 μm with Cr₂O₃ concentration equal to 4900 ppm; however, grain size decreases at higher Cr₂O₃ concentrations. No significant changes were observed in specific heat capacity, linear thermal expansion, and coefficient of thermal expansion compared to undoped UO₂. The thermal conductivity also decreased through the incorporation of Cr₂O₃ dopants above 750 ppm and is shown to be ~15 % lower than reported UO₂ values.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 2329260

Alternate ID(s):: OSTI ID: 2325508

Report Number(s):: LA-UR--23-34124

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Vol. 594; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (35)

Thermodynamics of gas phase chromium species: The chromium oxides, the chromium oxyhydroxides, and volatility calculations in waste incineration processes Ebbinghaus, Bartley B. Combustion and Flame, Vol. 93, Issue 1-2 https://doi.org/10.1016/0010-2180(93)90087-J	journal	April 1993
Grain growth in pure and titania-doped uranium dioxide Amato, I.; Colombo, R. L.; Balzari, A. Petruccioli Journal of Nuclear Materials, Vol. 18, Issue 3 https://doi.org/10.1016/0022-3115(66)90166-8	journal	March 1966
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
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
The thermal expansion of solid UO2 and (U, Pu) mixed oxides — a review and recommendations Martin, D. G. Journal of Nuclear Materials, Vol. 152, Issue 2-3 https://doi.org/10.1016/0022-3115(88)90315-7	journal	May 1988
Effects of Nb2O5 addition on grain growth and densification in UO2 pellets under reducing and/or oxidizing atmospheres No authors listed Journal of Nuclear Materials, Vol. 209, Issue 3 https://doi.org/10.1016/0022-3115(94)90264-X	journal	May 1994
Factors governing microstructure development of Cr2O3-doped UO2 during sintering Bourgeois, L.; Dehaudt, Ph.; Lemaignan, C. Journal of Nuclear Materials, Vol. 297, Issue 3 https://doi.org/10.1016/S0022-3115(01)00626-2	journal	September 2001
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
Solubility of magnesium in uranium dioxide Fujino, Takeo; Nakama, Shohei; Sato, Nobuaki Journal of Nuclear Materials, Vol. 246, Issue 2-3 https://doi.org/10.1016/S0022-3115(97)00143-8	journal	August 1997
Effect of additives (Cr2O3, Al2O3, SiO2, MgO) on diffusional release of from UO2 fuels Kashibe, S.; Une, K. Journal of Nuclear Materials, Vol. 254, Issue 2-3 https://doi.org/10.1016/S0022-3115(97)00356-5	journal	April 1998
Rim structure formation and high burnup fuel behavior of large-grained UO2 fuels Une, K.; Hirai, M.; Nogita, K. Journal of Nuclear Materials, Vol. 278, Issue 1 https://doi.org/10.1016/S0022-3115(99)00214-7	journal	February 2000
Thermophysical properties of uranium dioxide Fink, J. K. Journal of Nuclear Materials, Vol. 279, Issue 1 https://doi.org/10.1016/S0022-3115(99)00273-1	journal	March 2000
Measurement and interpretation of the thermo-physical properties of UO 2 at high temperatures: The viral effect of oxygen defects Pavlov, T. R.; Wenman, M. R.; Vlahovic, L. Acta Materialia, Vol. 139 https://doi.org/10.1016/j.actamat.2017.07.060	journal	October 2017
The role of dopant charge state on defect chemistry and grain growth of doped UO2 Cooper, M. W. D.; Stanek, C. R.; Andersson, D. A. Acta Materialia, Vol. 150 https://doi.org/10.1016/j.actamat.2018.02.020	journal	May 2018
High temperature chromium volatilization from Cr2O3 powder and Cr2O3-doped UO2 pellets in reducing atmospheres Peres, V.; Favergeon, L.; Andrieu, M. Journal of Nuclear Materials, Vol. 423, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2012.01.001	journal	April 2012
Chromia doped UO2 fuel: Investigation of the lattice parameter Cardinaels, T.; Govers, K.; Vos, B. Journal of Nuclear Materials, Vol. 424, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2012.02.025	journal	May 2012
Effect of step wise variation of oxygen potential during the isothermal sintering on the grain growth behavior in Cr2O3 doped UO2 pellets Yang, Jae Ho; Kim, Keon Sik; Nam, Ik Hui Journal of Nuclear Materials, Vol. 429, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2012.05.034	journal	October 2012
Thermodynamics of chromium in UO2 fuel: A solubility model Riglet-Martial, Ch.; Martin, Ph.; Testemale, D. Journal of Nuclear Materials, Vol. 447, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.12.021	journal	April 2014
Local atomic structure of chromium bearing precipitates in chromia doped uranium dioxide investigated by combined micro-beam X-ray diffraction and absorption spectroscopy Kuri, G.; Mieszczynski, C.; Martin, M. Journal of Nuclear Materials, Vol. 449, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.03.017	journal	June 2014
Forward for special JNM issue on accident tolerant fuels for LWRs Carmack, Jon; Goldner, Frank Journal of Nuclear Materials, Vol. 448, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.03.030	journal	May 2014
Accurate lattice parameter measurements of stoichiometric uranium dioxide Leinders, Gregory; Cardinaels, Thomas; Binnemans, Koen Journal of Nuclear Materials, Vol. 459 https://doi.org/10.1016/j.jnucmat.2015.01.029	journal	April 2015
TiO2 doped UO2 fuels sintered by spark plasma sintering Yao, Tiankai; Scott, Spencer M.; Xin, Guoqing Journal of Nuclear Materials, Vol. 469 https://doi.org/10.1016/j.jnucmat.2015.11.025	journal	February 2016
Grand potential sintering simulations of doped UO2 accident-tolerant fuel concepts Greenquist, Ian; Tonks, Michael; Cooper, Michael Journal of Nuclear Materials, Vol. 532 https://doi.org/10.1016/j.jnucmat.2020.152052	journal	April 2020
Raman spectroscopy coupled to principal component analysis for studying UO2 nuclear fuels with different grain sizes due to the chromia addition Milena-Pérez, A.; Bonales, L. J.; Rodríguez-Villagra, N. Journal of Nuclear Materials, Vol. 543 https://doi.org/10.1016/j.jnucmat.2020.152581	journal	January 2021
A new heat capacity law for UO2, PuO2 and (U,Pu)O2 derived from molecular dynamics simulations and useable in fuel performance codes Bathellier, Didier; Lainet, Marc; Freyss, Michel Journal of Nuclear Materials, Vol. 549 https://doi.org/10.1016/j.jnucmat.2021.152877	journal	June 2021
An evaluation of tri-valent oxide (Cr2O3) as a grain enlarging dopant for UO2 nuclear fuels fabricated under reducing environment Silva, Chinthaka M.; Hunt, Rodney D.; Holliday, Kiel S. Journal of Nuclear Materials, Vol. 553 https://doi.org/10.1016/j.jnucmat.2021.153053	journal	September 2021
Correlations for the specific heat capacity of (UxPu1−x)1−yGdyO2−z derived from molecular dynamics Galvin, Conor O. T.; Machida, Masahiko; Nakamura, Hiroki Journal of Nuclear Materials, Vol. 572 https://doi.org/10.1016/j.jnucmat.2022.154028	journal	December 2022
Modeling of Cr2O3-doped UO2 as a near-term accident tolerant fuel for LWRs using the BISON code Che, Yifeng; Pastore, Giovanni; Hales, Jason Nuclear Engineering and Design, Vol. 337 https://doi.org/10.1016/j.nucengdes.2018.07.015	journal	October 2018
Sensitivity of UO2 fuel performance to microstructural evolutions driven by dilute additives Cheniour, Amani; Sweet, Ryan T.; Nelson, Andrew T. Nuclear Engineering and Design, Vol. 410 https://doi.org/10.1016/j.nucengdes.2023.112383	journal	August 2023
The Vapor Pressure and Heat of Sublimation of Chromium Dickson, D. S.; Myers, J. R.; Saxer, R. K. The Journal of Physical Chemistry, Vol. 69, Issue 11 https://doi.org/10.1021/j100895a508	journal	November 1965
Deconvoluting Cr states in Cr-doped UO2 nuclear fuels via bulk and single crystal spectroscopic studies Murphy, Gabriel L.; Gericke, Robert; Gilson, Sara Nature Communications, Vol. 14, Issue 1 https://doi.org/10.1038/s41467-023-38109-0	journal	April 2023
Cr2+ solid solution in UO2 evidenced by advanced spectroscopy Smith, Hannah; Townsend, Luke T.; Mohun, Ritesh Communications Chemistry, Vol. 5, Issue 1 https://doi.org/10.1038/s42004-022-00784-3	journal	December 2022
Temperature and Finite Pulse‐Time Effects in the Flash Method for Measuring Thermal Diffusivity Cape, J. A.; Lehman, G. W. Journal of Applied Physics, Vol. 34, Issue 7 https://doi.org/10.1063/1.1729711	journal	July 1963
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
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

Similar Records

2022 Accomplishments Report Template

Technical Report · Tue Sep 20 00:00:00 EDT 2022 · OSTI ID:1889923

Report on the effect of dopants on FLASH sintering of enhanced UO₂

Technical Report · Fri Jun 28 00:00:00 EDT 2019 · OSTI ID:1711331

Statistical fracture behavior of doped UO₂ using a ball-on-ring equibiaxial flexure test method

Journal Article · Mon Feb 24 19:00:00 EST 2025 · Journal of Nuclear Materials · OSTI ID:2523685

Related Subjects

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
ATF
Chromium
Large grain UO2
Microstructure
Thermophysical properties

Performance and properties evolution of near-term accident tolerant fuel: Cr-doped UO2

Citation Formats

References (35)

Similar Records

Related Subjects

Performance and properties evolution of near-term accident tolerant fuel: Cr-doped UO₂