Dense nanocrystalline UO 2+ x fuel pellets synthesized by high pressure spark plasma sintering
Abstract
Abstract Nanocrystalline UO 2+ x powders are prepared by high‐energy ball milling and subsequently consolidated into dense fuel pellets (>95% of theoretical density) under high pressure (750 MP a) by spark plasma sintering at low sintering temperatures (600°C‐700°C). The grain size achieved in the dense nano‐ceramic pellets varies within 60‐160 nm as controlled by sintering temperature and duration. The sintered fuel pellets are single phase UO 2+ x with hyper‐stoichiometric compositions as derived by X‐ray diffraction, and micro‐Raman measurements indicate that random oxygen interstitials and Willis clusters dominate the single phase nano‐sized oxide pellets of UO 2.03 and UO 2.11 , respectively. The thermal conductivities of the densified nano‐sized oxide fuel pellets are measured by laser flash, and the fuel stoichiometry displays a dominant effect in controlling thermal transport properties. A reduction in thermal conductivity is also observed for the dense nano‐sized pellets as compared with micron‐sized counterparts reported in the literature. The correlation among the SPS sintering parameters—microstructure control—properties is established, and the nano‐sized UO 2+ x pellets with controlled microstructure can serve as the model systems for fundamental understandings of fuel behaviors and obtaining critical experimental data for multi‐physics MARMOT model validation.
- Authors:
-
- Department of Mechanical, Aerospace, and Nuclear Engineering Rensselaer Polytechnic Institute Troy New York
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1408189
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Journal of the American Ceramic Society
- Additional Journal Information:
- Journal Name: Journal of the American Ceramic Society Journal Volume: 101 Journal Issue: 3; Journal ID: ISSN 0002-7820
- Publisher:
- Wiley-Blackwell
- Country of Publication:
- United States
- Language:
- English
Citation Formats
Yao, Tiankai, Scott, Spencer M., Xin, Guoqing, Gong, Bowen, and Lian, Jie. Dense nanocrystalline UO 2+ x fuel pellets synthesized by high pressure spark plasma sintering. United States: N. p., 2017.
Web. doi:10.1111/jace.15289.
Yao, Tiankai, Scott, Spencer M., Xin, Guoqing, Gong, Bowen, & Lian, Jie. Dense nanocrystalline UO 2+ x fuel pellets synthesized by high pressure spark plasma sintering. United States. https://doi.org/10.1111/jace.15289
Yao, Tiankai, Scott, Spencer M., Xin, Guoqing, Gong, Bowen, and Lian, Jie. Wed .
"Dense nanocrystalline UO 2+ x fuel pellets synthesized by high pressure spark plasma sintering". United States. https://doi.org/10.1111/jace.15289.
@article{osti_1408189,
title = {Dense nanocrystalline UO 2+ x fuel pellets synthesized by high pressure spark plasma sintering},
author = {Yao, Tiankai and Scott, Spencer M. and Xin, Guoqing and Gong, Bowen and Lian, Jie},
abstractNote = {Abstract Nanocrystalline UO 2+ x powders are prepared by high‐energy ball milling and subsequently consolidated into dense fuel pellets (>95% of theoretical density) under high pressure (750 MP a) by spark plasma sintering at low sintering temperatures (600°C‐700°C). The grain size achieved in the dense nano‐ceramic pellets varies within 60‐160 nm as controlled by sintering temperature and duration. The sintered fuel pellets are single phase UO 2+ x with hyper‐stoichiometric compositions as derived by X‐ray diffraction, and micro‐Raman measurements indicate that random oxygen interstitials and Willis clusters dominate the single phase nano‐sized oxide pellets of UO 2.03 and UO 2.11 , respectively. The thermal conductivities of the densified nano‐sized oxide fuel pellets are measured by laser flash, and the fuel stoichiometry displays a dominant effect in controlling thermal transport properties. A reduction in thermal conductivity is also observed for the dense nano‐sized pellets as compared with micron‐sized counterparts reported in the literature. The correlation among the SPS sintering parameters—microstructure control—properties is established, and the nano‐sized UO 2+ x pellets with controlled microstructure can serve as the model systems for fundamental understandings of fuel behaviors and obtaining critical experimental data for multi‐physics MARMOT model validation.},
doi = {10.1111/jace.15289},
journal = {Journal of the American Ceramic Society},
number = 3,
volume = 101,
place = {United States},
year = {2017},
month = {11}
}
https://doi.org/10.1111/jace.15289
Web of Science
Works referenced in this record:
Preparation of UO2, ThO2 and (Th,U)O2 pellets from photochemically-prepared nano-powders
journal, February 2016
- Pavelková, Tereza; Čuba, Václav; de Visser-Týnová, Eva
- Journal of Nuclear Materials, Vol. 469
Effect of porosity and stoichiometry on the thermal conductivity of uranium dioxide
journal, May 1974
- Hobson, I. C.; Taylor, R.; Ainscough, J. B.
- Journal of Physics D: Applied Physics, Vol. 7, Issue 7
Fabrication of Transparent Yttria by High-Pressure Spark Plasma Sintering
journal, August 2011
- Zhang, Haibin; Kim, Byung-Nam; Morita, Koji
- Journal of the American Ceramic Society, Vol. 94, Issue 10
Raman spectra of stoichiometric and hyperstoichiometric uranium dioxide
journal, September 2003
- Manara, Dario; Renker, Burkhard
- Journal of Nuclear Materials, Vol. 321, Issue 2-3
Mechanosynthesis of supersaturated solid solutions of Sn in near-equiatomic bcc FeCo
journal, September 2012
- Loureiro, J. M.; Costa, B. F. O.; Le Caër, G.
- Journal of Alloys and Compounds, Vol. 536
High-pressure spark plasma sintering (SPS) of transparent polycrystalline magnesium aluminate spinel (PMAS)
journal, December 2014
- Sokol, M.; Kalabukhov, S.; Dariel, M. P.
- Journal of the European Ceramic Society, Vol. 34, Issue 16
Multiscale modeling of thermal conductivity of high burnup structures in UO2 fuels
journal, March 2016
- Bai, Xian-Ming; Tonks, Michael R.; Zhang, Yongfeng
- Journal of Nuclear Materials, Vol. 470
Raman spectrum of U4O9: a new interpretation of damage lines in UO2: Raman spectrum of U4O9
journal, October 2011
- Desgranges, L.; Baldinozzi, G.; Simon, P.
- Journal of Raman Spectroscopy, Vol. 43, Issue 3
Thermophysical properties of uranium dioxide
journal, March 2000
- Fink, J. K.
- Journal of Nuclear Materials, Vol. 279, Issue 1
Raman spectroscopic studies of defect structures and phase transition in hyper-stoichiometric UO2+x
journal, January 2010
- He, Heming; Shoesmith, David
- Physical Chemistry Chemical Physics, Vol. 12, Issue 28
High-temperature X-ray study of uranium oxides in the UO2U3O8 region
journal, December 1955
- Grønvold, Fredrik
- Journal of Inorganic and Nuclear Chemistry, Vol. 1, Issue 6
Spark plasma sintering of transparent alumina
journal, October 2007
- Kim, Byung-Nam; Hiraga, Keijiro; Morita, Koji
- Scripta Materialia, Vol. 57, Issue 7
A conceptual model for the fuel oxidation of defective fuel
journal, June 2007
- Higgs, J. D.; Lewis, B. J.; Thompson, W. T.
- Journal of Nuclear Materials, Vol. 366, Issue 1-2
Raman spectroscopy characterization of actinide oxides (U1−yPuy)O2: Resistance to oxidation by the laser beam and examination of defects
journal, October 2010
- Jégou, C.; Caraballo, R.; Peuget, S.
- Journal of Nuclear Materials, Vol. 405, Issue 3
Optical Properties and Microstructure of Nanocrystalline Cubic Zirconia Prepared by High-Pressure Spark Plasma Sintering: Optical Properties and Microstructure of Zirconia by SPS
journal, March 2011
- Zhang, Haibin; Kim, Byung-Nam; Morita, Koji
- Journal of the American Ceramic Society, Vol. 94, Issue 9
Metallographic determination of the UO2-U409 phase diagram
journal, June 1960
- Schaner, B. E.
- Journal of Nuclear Materials, Vol. 2, Issue 2
Plasma in spark plasma sintering of ceramic particle compacts
journal, July 2014
- Marder, R.; Estournès, C.; Chevallier, G.
- Scripta Materialia, Vol. 82
Sintering of uranium oxides of composition UO2 to U3O8 in various atmospheres
journal, April 1959
- Williams, J.; Barnes, E.; Scott, R.
- Journal of Nuclear Materials, Vol. 1, Issue 1
Simulated UO2 fuel containing CsI by spark plasma sintering
journal, November 2015
- Wangle, T.; Tyrpekl, V.; Cologna, M.
- Journal of Nuclear Materials, Vol. 466
Dense Iodoapatite Ceramics Consolidated by Low-Temperature Spark Plasma Sintering
journal, September 2015
- Yao, Tiankai; Scott, Spencer; Xin, Guoqing
- Journal of the American Ceramic Society, Vol. 98, Issue 12
Thermal Conductivity of Nearly Stoichiometric Single-Crystal and Polycrystalline UO 2
journal, January 1971
- Moore, J. P.; Mcelroy, D. L.
- Journal of the American Ceramic Society, Vol. 54, Issue 1
Ordered Defects in the Oxides of Uranium
journal, August 1986
- Allen, G. C.; Tempest, P. A.
- Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 406, Issue 1831
High-pressure spark plasma sintering of MgO-doped transparent alumina
journal, January 2012
- Kim, Byung-Nam; Hiraga, Keijiro; Grasso, Salvatore
- Journal of the Ceramic Society of Japan, Vol. 120, Issue 1399
The Effect of Microstructure and Microcracking on the Thermal Conductivity of UO 2 -U 4 O 9
journal, July 1979
- Buykx, W. J.
- Journal of the American Ceramic Society, Vol. 62, Issue 7-8
Microstructural refinement in spark plasma sintering 3Y-TZP nanoceramics
journal, August 2016
- Liu, Chong; Xiang, Mingyu; Fu, Zhengyi
- Journal of the European Ceramic Society, Vol. 36, Issue 10
Kinetics of precipitation of U4O9 from hyperstoichiometric UO2+x
journal, July 2007
- Higgs, J. D.; Thompson, W. T.; Lewis, B. J.
- Journal of Nuclear Materials, Vol. 366, Issue 3
A method of determining the distribution of U4O9 in oxidised UO2
journal, December 1990
- Whillock, S.; Pearce, J. H.
- Journal of Nuclear Materials, Vol. 175, Issue 1-2
A comparative study of Spark Plasma Sintering (SPS), Hot Isostatic Pressing (HIP) and microwaves sintering techniques on p-type Bi2Te3 thermoelectric properties
journal, August 2012
- Delaizir, G.; Bernard-Granger, G.; Monnier, J.
- Materials Research Bulletin, Vol. 47, Issue 8
Refinement of the structure of β-U 4 O 9
journal, June 2004
- Cooper, R. I.; Willis, B. T. M.
- Acta Crystallographica Section A Foundations of Crystallography, Vol. 60, Issue 4
Densification of uranium dioxide fuel pellets prepared by spark plasma sintering (SPS)
journal, April 2013
- Ge, Lihao; Subhash, Ghatu; Baney, Ronald H.
- Journal of Nuclear Materials, Vol. 435, Issue 1-3
Highly Transparent Pure Alumina Fabricated by High-Pressure Spark Plasma Sintering: Rapid Communications of the American Ceramic Society
journal, April 2010
- Grasso, Salvatore; Kim, Byung-Nam; Hu, Chunfeng
- Journal of the American Ceramic Society, Vol. 93, Issue 9
Point defects in uranium dioxide: Ab initio pseudopotential approach in the generalized gradient approximation
journal, December 2005
- Freyss, Michel; Petit, Thierry; Crocombette, Jean-Paul
- Journal of Nuclear Materials, Vol. 347, Issue 1-2
The effect of grain size, porosity and yttria content on the thermal conductivity of nanocrystalline zirconia
journal, September 1998
- Raghavan, Srinivasan; Wang, Hsin; Dinwiddie, Ralph B.
- Scripta Materialia, Vol. 39, Issue 8
Investigation of the oxygen activity of oxide fuels and fuel-fission product systems by solid electrolyte techniques. Part I: Qualification and limitations of the method
journal, June 1983
- Teske, K.; Ullmann, H.; Rettig, D.
- Journal of Nuclear Materials, Vol. 116, Issue 2-3
Positions of the Oxygen Atoms in UO2.13
journal, February 1963
- Willis, B. T. M.
- Nature, Vol. 197, Issue 4869
Thermal Conductivity Measurements on UO 2+x from 300 to 1,400 K
journal, August 1996
- Amaya, Masaki; Kubo, Toshio; Korei, Yoshiaki
- Journal of Nuclear Science and Technology, Vol. 33, Issue 8
Crystallite Size Refinement of ZrB 2 by High-Energy Ball Milling
journal, December 2009
- Galán, Carlos A.; Ortiz, Angel L.; Guiberteau, Fernando
- Journal of the American Ceramic Society, Vol. 92, Issue 12
Facile low temperature solid state synthesis of iodoapatite by high-energy ball milling
journal, January 2014
- Lu, Fengyuan; Yao, Tiankai; Xu, Jinling
- RSC Adv., Vol. 4, Issue 73
Interfacial thermal resistance in nanocrystalline yttria-stabilized zirconia
journal, May 2002
- Yang, Ho-Soon; Bai, G. -R.; Thompson, L. J.
- Acta Materialia, Vol. 50, Issue 9
The high burn-up structure in nuclear fuel
journal, December 2010
- Rondinella, Vincenzo V.; Wiss, Thierry
- Materials Today, Vol. 13, Issue 12
Point defects and clustering in uranium dioxide by calculations
journal, March 2008
- Geng, Hua Y.; Chen, Ying; Kaneta, Yasunori
- Physical Review B, Vol. 77, Issue 10
Thermal barrier coating materials
journal, June 2005
- Clarke, David R.; Phillpot, Simon R.
- Materials Today, Vol. 8, Issue 6
The defect structure of hyper-stoichiometric uranium dioxide
journal, January 1978
- Willis, B. T. M.
- Acta Crystallographica Section A, Vol. 34, Issue 1