Molten uranium dioxide structure and dynamics

Skinner, L. B.; Parise, J. B.; Benmore, C. J.; Weber, J. K.R.; Williamson, M. A.; Tamalonis, A.; Hebden, A.; Wiencek, T.; Alderman, O. L.G.; Guthrie, M.; Leibowitz, L.

doi:10.1126/science.1259709

Title: Molten uranium dioxide structure and dynamics

Journal Article · Fri Nov 21 00:00:00 EST 2014 · Science

DOI:https://doi.org/10.1126/science.1259709· OSTI ID:1174101

Skinner, L. B. ^[1]; Parise, J. B. ^[2]; Benmore, C. J. ^[3]; Weber, J. K.R. ^[4]; Williamson, M. A. ^[3]; Tamalonis, A. ^[4]; Hebden, A. ^[3]; Wiencek, T. ^[3]; Alderman, O. L.G. ^[4]; Guthrie, M. ^[5]; Leibowitz, L. ^[3]

Argonne National Laboratory (ANL), Argonne, IL (United States); Stony Brook Univ., Stony Brook, NY (United States); Materials Development Inc., Arlington Heights, IL (United States)
Stony Brook Univ., Stony Brook, NY (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Materials Development Inc., Arlington Heights, IL (United States)
Carnegie Inst., Washington, DC (United States)

Uranium dioxide (UO₂) is the major nuclear fuel component of fission power reactors. A key concern during severe accidents is the melting and leakage of radioactive UO₂ as it corrodes through its zirconium cladding and steel containment. Yet, the very high temperatures (>3140 kelvin) and chemical reactivity of molten UO₂ have prevented structural studies. In this work, we combine laser heating, sample levitation, and synchrotron x-rays to obtain pair distribution function measurements of hot solid and molten UO₂. The hot solid shows a substantial increase in oxygen disorder around the lambda transition (2670 K) but negligible U-O coordination change. On melting, the average U-O coordination drops from 8 to 6.7 ± 0.5. Molecular dynamics models refined to this structure predict higher U-U mobility than 8-coordinated melts.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC00112704

OSTI ID:: 1174101

Report Number(s):: BNL-107388-2015-JA; R&D Project: LS001

Journal Information:: Science, Vol. 346, Issue 6212; ISSN 0036-8075

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 63 works

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References (28)

A new empirical potential for simulating the formation of defects and their mobility in uranium dioxide Morelon, N. -D.; Ghaleb, D.; Delaye, J. -M. Philosophical Magazine, Vol. 83, Issue 13 https://doi.org/10.1080/1478643031000091454	journal	January 2003
Aerodynamic levitation technique for containerless high temperature studies on liquid and solid samples Winborne, David A.; Nordine, Paul C.; Rosner, Daniel E. Metallurgical Transactions B, Vol. 7, Issue 4 https://doi.org/10.1007/BF02698607	journal	December 1976
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
New analytical scattering-factor functions for free atoms and ions Waasmaier, D.; Kirfel, A. Acta Crystallographica Section A Foundations of Crystallography, Vol. 51, Issue 3 https://doi.org/10.1107/S0108767394013292	journal	May 1995
A time resolved high energy X-ray diffraction study of cooling liquid SiO2 Skinner, L. B.; Benmore, C. J.; Weber, J. K. R. Physical Chemistry Chemical Physics, Vol. 15, Issue 22 https://doi.org/10.1039/c3cp44347g	journal	January 2013
Prevented Mortality and Greenhouse Gas Emissions from Historical and Projected Nuclear Power Kharecha, Pushker A.; Hansen, James E. Environmental Science & Technology, Vol. 47, Issue 9, p. 4889-4895 https://doi.org/10.1021/es3051197	journal	April 2013
Joint diffraction and modeling approach to the structure of liquid alumina Skinner, Lawrie B.; Barnes, Adrian C.; Salmon, Philip S. Physical Review B, Vol. 87, Issue 2 https://doi.org/10.1103/PhysRevB.87.024201	journal	January 2013
Oxidation of Uranium Dioxide Blackburn, Paul E.; Weissbart, Joseph; Gulbransen, Earl A. The Journal of Physical Chemistry, Vol. 62, Issue 8 https://doi.org/10.1021/j150566a002	journal	August 1958
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
Melting of stoichiometric and hyperstoichiometric uranium dioxide Manara, D.; Ronchi, C.; Sheindlin, M. Journal of Nuclear Materials, Vol. 342, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2005.04.002	journal	June 2005
Neutron and x-ray diffraction studies of liquids and glasses Fischer, Henry E.; Barnes, Adrian C.; Salmon, Philip S. Reports on Progress in Physics, Vol. 69, Issue 1 https://doi.org/10.1088/0034-4885/69/1/R05	journal	November 2005
Relativistic X-ray Elastic Scattering Factors for Neutral Atoms Z = 1–54 from Multiconfiguration Dirac–Fock Wavefunctions in the 0–12Å ⁻¹ sinθ /λ Range, and Six-Gaussian Analytical Expressions in the 0–6Å ⁻¹ Range Su, Z.; Coppens, P. Acta Crystallographica Section A Foundations of Crystallography, Vol. 53, Issue 6 https://doi.org/10.1107/S0108767397004558	journal	November 1997
Corium viscosity modelling above liquidus temperature Sudreau, F.; Cognet, G. Nuclear Engineering and Design, Vol. 178, Issue 3 https://doi.org/10.1016/S0029-5493(97)00137-4	journal	December 1997
Potential models for ionic oxides Lewis, G. V.; Catlow, C. R. A. Journal of Physics C: Solid State Physics, Vol. 18, Issue 6 https://doi.org/10.1088/0022-3719/18/6/010	journal	February 1985
DL_POLY_2.0: A general-purpose parallel molecular dynamics simulation package Smith, W.; Forester, T. R. Journal of Molecular Graphics, Vol. 14, Issue 3, p. 136-141 https://doi.org/10.1016/S0263-7855(96)00043-4	journal	June 1996
Low Cation Coordination in Oxide Melts Skinner, L. B.; Benmore, C. J.; Weber, J. K. R. Physical Review Letters, Vol. 112, Issue 15 https://doi.org/10.1103/PhysRevLett.112.157801	journal	April 2014
XLI. A theory of the viscosity of liquids.—Part I Andrade, E. N. da C. The London, Edinburgh, and Dublin Philosophical Magazine and Journal of Science, Vol. 17, Issue 112 https://doi.org/10.1080/14786443409462409	journal	February 1934
Negative expansions of interatomic distances in metallic melts Lou, H.; Wang, X.; Cao, Q. Proceedings of the National Academy of Sciences, Vol. 110, Issue 25 https://doi.org/10.1073/pnas.1307967110	journal	June 2013
Development of structural order during supercooling of a fragile oxide melt Hennet, L.; Pozdnyakova, I.; Bytchkov, A. The Journal of Chemical Physics, Vol. 126, Issue 7 https://doi.org/10.1063/1.2646812	journal	February 2007
Structural Aspects of the Electrical Resistivity of Binary Alloys Bhatia, A. B.; Thornton, D. E. Physical Review B, Vol. 2, Issue 8 https://doi.org/10.1103/PhysRevB.2.3004	journal	October 1970
Dirac–Fock calculations of X-ray scattering factors and contributions to the mean inner potential for electron scattering Rez, D.; Rez, P.; Grant, I. Acta Crystallographica Section A Foundations of Crystallography, Vol. 50, Issue 4 https://doi.org/10.1107/S0108767393013200	journal	July 1994
Pressure Dependence of UO₂ Melting Measured by Double-Pulse Laser Heating Manara, D.; Ronchi, C.; Sheindlin, M. International Journal of Thermophysics, Vol. 23, Issue 5, p. 1147-1156 https://doi.org/10.1023/A:1019879917797	journal	January 2002
Molecular dynamics simulation of premelting and melting phase transitions in stoichiometric uranium dioxide Yakub, Eugene; Ronchi, Claudio; Staicu, Dragos The Journal of Chemical Physics, Vol. 127, Issue 9 https://doi.org/10.1063/1.2764484	journal	September 2007
Two-dimensional detector software: From real detector to idealised image or two-theta scan Hammersley, A. P.; Svensson, S. O.; Hanfland, M. High Pressure Research, Vol. 14, Issue 4-6, p. 235-248 https://doi.org/10.1080/08957959608201408	journal	January 1996
Structure of Normal and Supercooled Liquid Aluminum Oxide Krishnan, Shankar; Hennet, Louis; Jahn, Sandro Chemistry of Materials, Vol. 17, Issue 10 https://doi.org/10.1021/cm050254p	journal	May 2005
Hypernetted chain calculations of molten uranium dioxide: Comparison of rigid ion potentials Günay, S. D.; Akdere, Ü.; Taşseven, Ç. Journal of Molecular Liquids, Vol. 173 https://doi.org/10.1016/j.molliq.2012.06.028	journal	September 2012
Evaluation of thermal properties of UO2 and PuO2 by equilibrium molecular dynamics simulations from 300 to 2000K Arima, Tatsumi; Yamasaki, Sho; Inagaki, Yaohiro Journal of Alloys and Compounds, Vol. 400, Issue 1-2 https://doi.org/10.1016/j.jallcom.2005.04.003	journal	September 2005
Classical molecular dynamics simulation of UO2 to predict thermophysical properties Basak, C. B.; Sengupta, A. K.; Kamath, H. S. Journal of Alloys and Compounds, Vol. 360, Issue 1-2 https://doi.org/10.1016/S0925-8388(03)00350-5	journal	October 2003

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High wettability of liquid caesium iodine with solid uranium dioxide Kurosaki, Ken; Suzuki, Masanori; Uno, Masayoshi Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/s41598-017-11774-0	journal	September 2017
Investigation of Structure and Dynamics in Disordered Materials Using Containerless Techniques with In-Situ Quantum Beam and Thermophysical Property Measurements Kohara, Shinji; Ohara, Koji; Ishikawa, Takehiko Quantum Beam Science, Vol. 2, Issue 1 https://doi.org/10.3390/qubs2010005	journal	February 2018
Corium lavas: structure and properties of molten UO2-ZrO2 under meltdown conditions Alderman, O. L. G.; Benmore, C. J.; Weber, J. K. R. Scientific Reports, Vol. 8, Issue 1 https://doi.org/10.1038/s41598-018-20817-z	journal	February 2018
Polymorphic transition and nucleation pathway of barium dititanate (BaTi2O5) during crystallization from undercooled liquid Ge, Xuan; Hu, Qiaodan; Lu, Wenquan Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-43357-6	journal	May 2019
Using laser remote heating to simulate extreme thermal heat loads on nuclear fuels Vidal, T.; Gallais, L.; Faucheux, J. EPJ Web of Conferences, Vol. 225 https://doi.org/10.1051/epjconf/202022508002	journal	January 2020
Superionic UO ₂ : A model anharmonic crystalline material Zhang, Hao; Wang, Xinyi; Chremos, Alexandros The Journal of Chemical Physics, Vol. 150, Issue 17 https://doi.org/10.1063/1.5091042	journal	May 2019

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