Molten uranium dioxide structure and dynamics
Abstract
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.
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1174101
- Report Number(s):
- BNL-107388-2015-JA
Journal ID: ISSN 0036-8075; R&D Project: LS001
- Grant/Contract Number:
- SC00112704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Science
- Additional Journal Information:
- Journal Volume: 346; Journal Issue: 6212; Journal ID: ISSN 0036-8075
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
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., and Leibowitz, L. Molten uranium dioxide structure and dynamics. United States: N. p., 2014.
Web. doi:10.1126/science.1259709.
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. Molten uranium dioxide structure and dynamics. United States. https://doi.org/10.1126/science.1259709
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., and Leibowitz, L. Fri .
"Molten uranium dioxide structure and dynamics". United States. https://doi.org/10.1126/science.1259709. https://www.osti.gov/servlets/purl/1174101.
@article{osti_1174101,
title = {Molten uranium dioxide structure and dynamics},
author = {Skinner, L. B. and Parise, J. B. and Benmore, C. J. and Weber, J. K.R. and Williamson, M. A. and Tamalonis, A. and Hebden, A. and Wiencek, T. and Alderman, O. L.G. and Guthrie, M. and Leibowitz, L.},
abstractNote = {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.},
doi = {10.1126/science.1259709},
journal = {Science},
number = 6212,
volume = 346,
place = {United States},
year = {Fri Nov 21 00:00:00 EST 2014},
month = {Fri Nov 21 00:00:00 EST 2014}
}
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Works referenced in this record:
A new empirical potential for simulating the formation of defects and their mobility in uranium dioxide
journal, January 2003
- Morelon, N. -D.; Ghaleb, D.; Delaye, J. -M.
- Philosophical Magazine, Vol. 83, Issue 13
Aerodynamic levitation technique for containerless high temperature studies on liquid and solid samples
journal, December 1976
- Winborne, David A.; Nordine, Paul C.; Rosner, Daniel E.
- Metallurgical Transactions B, Vol. 7, Issue 4
Thermophysical properties of uranium dioxide
journal, March 2000
- Fink, J. K.
- Journal of Nuclear Materials, Vol. 279, Issue 1
New analytical scattering-factor functions for free atoms and ions
journal, May 1995
- Waasmaier, D.; Kirfel, A.
- Acta Crystallographica Section A Foundations of Crystallography, Vol. 51, Issue 3
A time resolved high energy X-ray diffraction study of cooling liquid SiO2
journal, January 2013
- Skinner, L. B.; Benmore, C. J.; Weber, J. K. R.
- Physical Chemistry Chemical Physics, Vol. 15, Issue 22
Prevented Mortality and Greenhouse Gas Emissions from Historical and Projected Nuclear Power
journal, April 2013
- Kharecha, Pushker A.; Hansen, James E.
- Environmental Science & Technology, Vol. 47, Issue 9, p. 4889-4895
Joint diffraction and modeling approach to the structure of liquid alumina
journal, January 2013
- Skinner, Lawrie B.; Barnes, Adrian C.; Salmon, Philip S.
- Physical Review B, Vol. 87, Issue 2
Oxidation of Uranium Dioxide
journal, August 1958
- Blackburn, Paul E.; Weissbart, Joseph; Gulbransen, Earl A.
- The Journal of Physical Chemistry, Vol. 62, Issue 8
Neutron Diffraction Study of the in Situ Oxidation of UO 2
journal, August 2009
- Desgranges, Lionel; Baldinozzi, Gianguido; Rousseau, Gurvan
- Inorganic Chemistry, Vol. 48, Issue 16
Melting of stoichiometric and hyperstoichiometric uranium dioxide
journal, June 2005
- Manara, D.; Ronchi, C.; Sheindlin, M.
- Journal of Nuclear Materials, Vol. 342, Issue 1-3
Neutron and x-ray diffraction studies of liquids and glasses
journal, November 2005
- Fischer, Henry E.; Barnes, Adrian C.; Salmon, Philip S.
- Reports on Progress in Physics, Vol. 69, Issue 1
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
journal, November 1997
- Su, Z.; Coppens, P.
- Acta Crystallographica Section A Foundations of Crystallography, Vol. 53, Issue 6
Corium viscosity modelling above liquidus temperature
journal, December 1997
- Sudreau, F.; Cognet, G.
- Nuclear Engineering and Design, Vol. 178, Issue 3
Potential models for ionic oxides
journal, February 1985
- Lewis, G. V.; Catlow, C. R. A.
- Journal of Physics C: Solid State Physics, Vol. 18, Issue 6
DL_POLY_2.0: A general-purpose parallel molecular dynamics simulation package
journal, June 1996
- Smith, W.; Forester, T. R.
- Journal of Molecular Graphics, Vol. 14, Issue 3, p. 136-141
Low Cation Coordination in Oxide Melts
journal, April 2014
- Skinner, L. B.; Benmore, C. J.; Weber, J. K. R.
- Physical Review Letters, Vol. 112, Issue 15
XLI. A theory of the viscosity of liquids.—Part I
journal, February 1934
- Andrade, E. N. da C.
- The London, Edinburgh, and Dublin Philosophical Magazine and Journal of Science, Vol. 17, Issue 112
Negative expansions of interatomic distances in metallic melts
journal, June 2013
- Lou, H.; Wang, X.; Cao, Q.
- Proceedings of the National Academy of Sciences, Vol. 110, Issue 25
Development of structural order during supercooling of a fragile oxide melt
journal, February 2007
- Hennet, L.; Pozdnyakova, I.; Bytchkov, A.
- The Journal of Chemical Physics, Vol. 126, Issue 7
Structural Aspects of the Electrical Resistivity of Binary Alloys
journal, October 1970
- Bhatia, A. B.; Thornton, D. E.
- Physical Review B, Vol. 2, Issue 8
Dirac–Fock calculations of X-ray scattering factors and contributions to the mean inner potential for electron scattering
journal, July 1994
- Rez, D.; Rez, P.; Grant, I.
- Acta Crystallographica Section A Foundations of Crystallography, Vol. 50, Issue 4
Pressure Dependence of UO2 Melting Measured by Double-Pulse Laser Heating
journal, January 2002
- Manara, D.; Ronchi, C.; Sheindlin, M.
- International Journal of Thermophysics, Vol. 23, Issue 5, p. 1147-1156
Molecular dynamics simulation of premelting and melting phase transitions in stoichiometric uranium dioxide
journal, September 2007
- Yakub, Eugene; Ronchi, Claudio; Staicu, Dragos
- The Journal of Chemical Physics, Vol. 127, Issue 9
Two-dimensional detector software: From real detector to idealised image or two-theta scan
journal, January 1996
- Hammersley, A. P.; Svensson, S. O.; Hanfland, M.
- High Pressure Research, Vol. 14, Issue 4-6, p. 235-248
Structure of Normal and Supercooled Liquid Aluminum Oxide
journal, May 2005
- Krishnan, Shankar; Hennet, Louis; Jahn, Sandro
- Chemistry of Materials, Vol. 17, Issue 10
Hypernetted chain calculations of molten uranium dioxide: Comparison of rigid ion potentials
journal, September 2012
- Günay, S. D.; Akdere, Ü.; Taşseven, Ç.
- Journal of Molecular Liquids, Vol. 173
Evaluation of thermal properties of UO2 and PuO2 by equilibrium molecular dynamics simulations from 300 to 2000K
journal, September 2005
- Arima, Tatsumi; Yamasaki, Sho; Inagaki, Yaohiro
- Journal of Alloys and Compounds, Vol. 400, Issue 1-2
Classical molecular dynamics simulation of UO2 to predict thermophysical properties
journal, October 2003
- Basak, C. B.; Sengupta, A. K.; Kamath, H. S.
- Journal of Alloys and Compounds, Vol. 360, Issue 1-2
Works referencing / citing this record:
High wettability of liquid caesium iodine with solid uranium dioxide
journal, September 2017
- Kurosaki, Ken; Suzuki, Masanori; Uno, Masayoshi
- Scientific Reports, Vol. 7, Issue 1
Investigation of Structure and Dynamics in Disordered Materials Using Containerless Techniques with In-Situ Quantum Beam and Thermophysical Property Measurements
journal, February 2018
- Kohara, Shinji; Ohara, Koji; Ishikawa, Takehiko
- Quantum Beam Science, Vol. 2, Issue 1
Corium lavas: structure and properties of molten UO2-ZrO2 under meltdown conditions
journal, February 2018
- Alderman, O. L. G.; Benmore, C. J.; Weber, J. K. R.
- Scientific Reports, Vol. 8, Issue 1
Polymorphic transition and nucleation pathway of barium dititanate (BaTi2O5) during crystallization from undercooled liquid
journal, May 2019
- Ge, Xuan; Hu, Qiaodan; Lu, Wenquan
- Scientific Reports, Vol. 9, Issue 1
Using laser remote heating to simulate extreme thermal heat loads on nuclear fuels
journal, January 2020
- Vidal, T.; Gallais, L.; Faucheux, J.
- EPJ Web of Conferences, Vol. 225
Superionic UO 2 : A model anharmonic crystalline material
journal, May 2019
- Zhang, Hao; Wang, Xinyi; Chremos, Alexandros
- The Journal of Chemical Physics, Vol. 150, Issue 17