Thermodynamics of fission products in UO2+-x

Nerikar, Pankaj V

doi:10.1088/0953-8984/21/43/435602

Title: Thermodynamics of fission products in UO2+-x

Journal Article · Thu Jan 01 00:00:00 EST 2009 · Physical Review. B, Condensed Matter and Materials Physics

DOI:https://doi.org/10.1088/0953-8984/21/43/435602· OSTI ID:962358

Nerikar, Pankaj V ^[1]

Los Alamos National Laboratory

The stabilities of selected fission products - Xe, Cs, and Sr - are investigated as a function of non-stoichiometry x in UO{sub 2{+-}x}. In particular, density functional theory (OFT) is used to calculate the incorporation and solution energies of these fission products at the anion and cation vacancy sites, at the divacancy, and at the bound Schottky defect. In order to reproduce the correct insulating state of UO{sub 2}, the DFT calculations are performed using spin polarization and with the Hubbard U tenn. In general, higher charge defects are more soluble in the fuel matrix and the solubility of fission products increases as the hyperstoichiometry increases. The solubility of fission product oxides is also explored. CS{sub 2}O is observed as a second stable phase and SrO is found to be soluble in the UO{sub 2} matrix for all stoichiometries. These observations mirror experimentally observed phenomena.

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

Sponsoring Organization:: USDOE

DOE Contract Number:: AC52-06NA25396

OSTI ID:: 962358

Report Number(s):: LA-UR-09-01586; LA-UR-09-1586; TRN: US200919%%118

Journal Information:: Physical Review. B, Condensed Matter and Materials Physics, Journal Name: Physical Review. B, Condensed Matter and Materials Physics; ISSN 1098-0121

Country of Publication:: United States

Language:: English

References (32)

The chemical effects of composition changes in irradiated oxide fuel materials II-Fission product segregation and chemical equilibria Ewart, F. T.; Taylor, R. G.; Horspool, J. M. Journal of Nuclear Materials, Vol. 61, Issue 3 https://doi.org/10.1016/0022-3115(76)90264-6	journal	September 1976
On the role of grain boundary diffusion in fission gas release Olander, D. R.; Van Uffelen, P. Journal of Nuclear Materials, Vol. 288, Issue 2-3 https://doi.org/10.1016/S0022-3115(00)00725-X	journal	February 2001
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
Solid fission product behavior in uranium-plutonium oxide fuel irradiated in a fast neutron flux O'boyle, D. R.; Brown, F. L.; Sanecki, J. E. Journal of Nuclear Materials, Vol. 29, Issue 1, p. 27-42 https://doi.org/10.1016/0022-3115(69)90124-X	journal	January 1969
Fuel research and basic aspects of fuel in-pile performance Matzke, Hj.; Blank, H. Journal of Nuclear Materials, Vol. 166, Issue 1-2 https://doi.org/10.1016/0022-3115(89)90184-0	journal	July 1989
The solubility of selected fission products in UO2 and (U, Pu)O2 Kleykamp, H. Journal of Nuclear Materials, Vol. 206, Issue 1 https://doi.org/10.1016/0022-3115(93)90236-R	journal	November 1993
Modeling Localized Defects in Ionic Materials Using Mott‐Littleton and Embedded Quantum Cluster Methodology Grimes, Robin W.; Catlow, C. Richard A. Journal of the American Ceramic Society, Vol. 73, Issue 11 https://doi.org/10.1111/j.1151-2916.1990.tb06446.x	journal	November 1990
Ab initio energetics of some fission products (Kr, I, Cs, Sr and He) in uranium dioxide Crocombette, Jean-Paul Journal of Nuclear Materials, Vol. 305, Issue 1 https://doi.org/10.1016/S0022-3115(02)00907-8	journal	September 2002
Ab initio modeling of the behavior of helium and xenon in actinide dioxide nuclear fuels Freyss, M.; Vergnet, N.; Petit, T. Journal of Nuclear Materials, Vol. 352, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2006.02.048	journal	June 2006
Molecular modelling of transmutation fuels and targets Petit, Thierry; Freyss, Michel; Garcia, Philippe Journal of Nuclear Materials, Vol. 320, Issue 1-2 https://doi.org/10.1016/S0022-3115(03)00179-X	journal	July 2003
Location of krypton atoms in uranium dioxide Petit, T.; Jomard, G.; Lemaignan, C. Journal of Nuclear Materials, Vol. 275, Issue 1 https://doi.org/10.1016/S0022-3115(99)00127-0	journal	October 1999
Correlation effects and energetics of point defects in uranium dioxide: a first principle investigation Gupta, F.; Brillant, G.; Pasturel, A. Philosophical Magazine, Vol. 87, Issue 17 https://doi.org/10.1080/14786430701235814	journal	June 2007
First-Principles Calculation of Point Defects in Uranium Dioxide Iwasawa, Misako; Chen, Ying; Kaneta, Yasunori MATERIALS TRANSACTIONS, Vol. 47, Issue 11 https://doi.org/10.2320/matertrans.47.2651	journal	January 2006
Energetics of intrinsic point defects in uranium dioxide from electronic-structure calculations Nerikar, Pankaj; Watanabe, Taku; Tulenko, James S. Journal of Nuclear Materials, Vol. 384, Issue 1 https://doi.org/10.1016/j.jnucmat.2008.10.003	journal	January 2009
Study of Ba and Zr stability in ${UO}_{2 \pm x}$ by density functional calculations Brillant, G.; Pasturel, A. Physical Review B, Vol. 77, Issue 18 https://doi.org/10.1103/PhysRevB.77.184110	journal	May 2008
Ab initio study of solution energy and diffusion of caesium in uranium dioxide Gupta, F.; Pasturel, A.; Brillant, G. Journal of Nuclear Materials, Vol. 385, Issue 2 https://doi.org/10.1016/j.jnucmat.2008.12.009	journal	March 2009
Electronic structure and Coulomb correlation energy in UO2 single crystal Baer, Y.; Schoenes, J. Solid State Communications, Vol. 33, Issue 8 https://doi.org/10.1016/0038-1098(80)91210-7	journal	February 1980
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Effect of Mott-Hubbard correlations on the electronic structure and structural stability of uranium dioxide Dudarev, S. L.; Manh, D. Nguyen; Sutton, A. P. Philosophical Magazine B, Vol. 75, Issue 5 https://doi.org/10.1080/13642819708202343	journal	May 1997
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Atomic transport properties in UO2 and mixed oxides (U, Pu)O2 Matzke, Hansjoachim Journal of the Chemical Society, Faraday Transactions 2, Vol. 83, Issue 7 https://doi.org/10.1039/f29878301121	journal	January 1987
Self-diffusion of uranium in UO2 Lidiard, A. B. Journal of Nuclear Materials, Vol. 19, Issue 1 https://doi.org/10.1016/0022-3115(66)90138-3	journal	April 1966
Ab initio investigation on oxygen defect clusters in UO2+x Geng, Hua Y.; Chen, Ying; Kaneta, Yasunori Applied Physics Letters, Vol. 93, Issue 20 https://doi.org/10.1063/1.3035846	journal	November 2008
Comparison of interatomic potentials for UO2. Part I: Static calculations Govers, K.; Lemehov, S.; Hou, M. Journal of Nuclear Materials, Vol. 366, Issue 1-2 https://doi.org/10.1016/j.jnucmat.2006.12.070	journal	June 2007
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
The General Utility Lattice Program ( GULP ) Gale, Julian D.; Rohl, Andrew L. Molecular Simulation, Vol. 29, Issue 5 https://doi.org/10.1080/0892702031000104887	journal	May 2003
Electronic structure of rare-earth nitrides using the $LSDA + U$ approach: Importance of allowing $4 f$ orbitals to break the cubic crystal symmetry Larson, P.; Lambrecht, Walter R. L.; Chantis, Athanasios Physical Review B, Vol. 75, Issue 4 https://doi.org/10.1103/PhysRevB.75.045114	journal	January 2007
$γ$ and $β$ cerium: $LDA + U$ calculations of ground-state parameters Amadon, B.; Jollet, F.; Torrent, M. Physical Review B, Vol. 77, Issue 15 https://doi.org/10.1103/PhysRevB.77.155104	journal	April 2008
Microstructural analysis of LWR spent fuels at high burnup Thomas, L. E.; Beyer, C. E.; Chariot, L. A. Journal of Nuclear Materials, Vol. 188 https://doi.org/10.1016/0022-3115(92)90457-V	journal	June 1992

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Title: Thermodynamics of fission products in UO2+-x

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