Dense nanocrystalline UO 2+ x fuel pellets synthesized by high pressure spark plasma sintering

Yao, Tiankai; Scott, Spencer M.; Xin, Guoqing; Gong, Bowen; Lian, Jie

doi:10.1111/jace.15289

Title: Dense nanocrystalline UO _{2+ x} fuel pellets synthesized by high pressure spark plasma sintering

Journal Article · Wed Nov 01 00:00:00 EDT 2017 · Journal of the American Ceramic Society

DOI:https://doi.org/10.1111/jace.15289· OSTI ID:1408189

^[1];

^[1]; Xin, Guoqing ^[1]; Gong, Bowen ^[1]; Lian, Jie ^[1]

Department of Mechanical, Aerospace, and Nuclear Engineering Rensselaer Polytechnic Institute Troy New York

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.

View Accepted Manuscript (Publisher)

Cite

Export

Save

Sponsoring Organization:: USDOE

OSTI ID:: 1408189

Journal Information:: Journal of the American Ceramic Society, Journal Name: Journal of the American Ceramic Society Vol. 101 Journal Issue: 3; ISSN 0002-7820

Publisher:: Wiley-BlackwellCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 19 works

Citation information provided by
Web of Science

References (43)

Preparation of UO2, ThO2 and (Th,U)O2 pellets from photochemically-prepared nano-powders Pavelková, Tereza; Čuba, Václav; de Visser-Týnová, Eva Journal of Nuclear Materials, Vol. 469 https://doi.org/10.1016/j.jnucmat.2015.11.041	journal	February 2016
Effect of porosity and stoichiometry on the thermal conductivity of uranium dioxide Hobson, I. C.; Taylor, R.; Ainscough, J. B. Journal of Physics D: Applied Physics, Vol. 7, Issue 7 https://doi.org/10.1088/0022-3727/7/7/308	journal	May 1974
Fabrication of Transparent Yttria by High-Pressure Spark Plasma Sintering Zhang, Haibin; Kim, Byung-Nam; Morita, Koji Journal of the American Ceramic Society, Vol. 94, Issue 10 https://doi.org/10.1111/j.1551-2916.2011.04789.x	journal	August 2011
Raman spectra of stoichiometric and hyperstoichiometric uranium dioxide Manara, Dario; Renker, Burkhard Journal of Nuclear Materials, Vol. 321, Issue 2-3 https://doi.org/10.1016/S0022-3115(03)00248-4	journal	September 2003
Mechanosynthesis of supersaturated solid solutions of Sn in near-equiatomic bcc FeCo Loureiro, J. M.; Costa, B. F. O.; Le Caër, G. Journal of Alloys and Compounds, Vol. 536 https://doi.org/10.1016/j.jallcom.2011.12.036	journal	September 2012
High-pressure spark plasma sintering (SPS) of transparent polycrystalline magnesium aluminate spinel (PMAS) Sokol, M.; Kalabukhov, S.; Dariel, M. P. Journal of the European Ceramic Society, Vol. 34, Issue 16 https://doi.org/10.1016/j.jeurceramsoc.2014.07.022	journal	December 2014
Multiscale modeling of thermal conductivity of high burnup structures in UO2 fuels Bai, Xian-Ming; Tonks, Michael R.; Zhang, Yongfeng Journal of Nuclear Materials, Vol. 470 https://doi.org/10.1016/j.jnucmat.2015.12.028	journal	March 2016
Raman spectrum of U4O9: a new interpretation of damage lines in UO2: Raman spectrum of U4O9 Desgranges, L.; Baldinozzi, G.; Simon, P. Journal of Raman Spectroscopy, Vol. 43, Issue 3 https://doi.org/10.1002/jrs.3054	journal	October 2011
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
Raman spectroscopic studies of defect structures and phase transition in hyper-stoichiometric UO2+x He, Heming; Shoesmith, David Physical Chemistry Chemical Physics, Vol. 12, Issue 28 https://doi.org/10.1039/b925495a	journal	January 2010
High-temperature X-ray study of uranium oxides in the UO2U3O8 region Grønvold, Fredrik Journal of Inorganic and Nuclear Chemistry, Vol. 1, Issue 6 https://doi.org/10.1016/0022-1902(55)80046-2	journal	December 1955
Spark plasma sintering of transparent alumina Kim, Byung-Nam; Hiraga, Keijiro; Morita, Koji Scripta Materialia, Vol. 57, Issue 7 https://doi.org/10.1016/j.scriptamat.2007.06.009	journal	October 2007
A conceptual model for the fuel oxidation of defective fuel Higgs, J. D.; Lewis, B. J.; Thompson, W. T. Journal of Nuclear Materials, Vol. 366, Issue 1-2 https://doi.org/10.1016/j.jnucmat.2006.12.050	journal	June 2007
Raman spectroscopy characterization of actinide oxides (U1−yPuy)O2: Resistance to oxidation by the laser beam and examination of defects Jégou, C.; Caraballo, R.; Peuget, S. Journal of Nuclear Materials, Vol. 405, Issue 3 https://doi.org/10.1016/j.jnucmat.2010.08.005	journal	October 2010
Optical Properties and Microstructure of Nanocrystalline Cubic Zirconia Prepared by High-Pressure Spark Plasma Sintering: Optical Properties and Microstructure of Zirconia by SPS Zhang, Haibin; Kim, Byung-Nam; Morita, Koji Journal of the American Ceramic Society, Vol. 94, Issue 9 https://doi.org/10.1111/j.1551-2916.2011.04477.x	journal	March 2011
Metallographic determination of the UO2-U409 phase diagram Schaner, B. E. Journal of Nuclear Materials, Vol. 2, Issue 2 https://doi.org/10.1016/0022-3115(60)90038-6	journal	June 1960
Plasma in spark plasma sintering of ceramic particle compacts Marder, R.; Estournès, C.; Chevallier, G. Scripta Materialia, Vol. 82 https://doi.org/10.1016/j.scriptamat.2014.03.023	journal	July 2014
Sintering of uranium oxides of composition UO2 to U3O8 in various atmospheres Williams, J.; Barnes, E.; Scott, R. Journal of Nuclear Materials, Vol. 1, Issue 1 https://doi.org/10.1016/0022-3115(59)90008-X	journal	April 1959
Simulated UO2 fuel containing CsI by spark plasma sintering Wangle, T.; Tyrpekl, V.; Cologna, M. Journal of Nuclear Materials, Vol. 466 https://doi.org/10.1016/j.jnucmat.2015.07.030	journal	November 2015
Dense Iodoapatite Ceramics Consolidated by Low-Temperature Spark Plasma Sintering Yao, Tiankai; Scott, Spencer; Xin, Guoqing Journal of the American Ceramic Society, Vol. 98, Issue 12 https://doi.org/10.1111/jace.13867	journal	September 2015
Thermal Conductivity of Nearly Stoichiometric Single-Crystal and Polycrystalline UO ₂ Moore, J. P.; Mcelroy, D. L. Journal of the American Ceramic Society, Vol. 54, Issue 1 https://doi.org/10.1111/j.1151-2916.1971.tb12164.x	journal	January 1971
Ordered Defects in the Oxides of Uranium Allen, G. C.; Tempest, P. A. Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 406, Issue 1831 https://doi.org/10.1098/rspa.1986.0078	journal	August 1986
High-pressure spark plasma sintering of MgO-doped transparent alumina Kim, Byung-Nam; Hiraga, Keijiro; Grasso, Salvatore Journal of the Ceramic Society of Japan, Vol. 120, Issue 1399 https://doi.org/10.2109/jcersj2.120.116	journal	January 2012
The Effect of Microstructure and Microcracking on the Thermal Conductivity of UO ₂ -U ₄ O ₉ Buykx, W. J. Journal of the American Ceramic Society, Vol. 62, Issue 7-8 https://doi.org/10.1111/j.1151-2916.1979.tb19070.x	journal	July 1979
Microstructural refinement in spark plasma sintering 3Y-TZP nanoceramics Liu, Chong; Xiang, Mingyu; Fu, Zhengyi Journal of the European Ceramic Society, Vol. 36, Issue 10 https://doi.org/10.1016/j.jeurceramsoc.2016.03.019	journal	August 2016
Kinetics of precipitation of U4O9 from hyperstoichiometric UO2+x Higgs, J. D.; Thompson, W. T.; Lewis, B. J. Journal of Nuclear Materials, Vol. 366, Issue 3 https://doi.org/10.1016/j.jnucmat.2007.03.054	journal	July 2007
A method of determining the distribution of U4O9 in oxidised UO2 Whillock, S.; Pearce, J. H. Journal of Nuclear Materials, Vol. 175, Issue 1-2 https://doi.org/10.1016/0022-3115(90)90278-U	journal	December 1990
A comparative study of Spark Plasma Sintering (SPS), Hot Isostatic Pressing (HIP) and microwaves sintering techniques on p-type Bi2Te3 thermoelectric properties Delaizir, G.; Bernard-Granger, G.; Monnier, J. Materials Research Bulletin, Vol. 47, Issue 8 https://doi.org/10.1016/j.materresbull.2012.04.019	journal	August 2012
Refinement of the structure of β-U ₄ O ₉ Cooper, R. I.; Willis, B. T. M. Acta Crystallographica Section A Foundations of Crystallography, Vol. 60, Issue 4 https://doi.org/10.1107/S010876730401219X	journal	June 2004
Densification of uranium dioxide fuel pellets prepared by spark plasma sintering (SPS) Ge, Lihao; Subhash, Ghatu; Baney, Ronald H. Journal of Nuclear Materials, Vol. 435, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2012.12.010	journal	April 2013
Highly Transparent Pure Alumina Fabricated by High-Pressure Spark Plasma Sintering: Rapid Communications of the American Ceramic Society Grasso, Salvatore; Kim, Byung-Nam; Hu, Chunfeng Journal of the American Ceramic Society, Vol. 93, Issue 9 https://doi.org/10.1111/j.1551-2916.2010.03811.x	journal	April 2010
Point defects in uranium dioxide: Ab initio pseudopotential approach in the generalized gradient approximation Freyss, Michel; Petit, Thierry; Crocombette, Jean-Paul Journal of Nuclear Materials, Vol. 347, Issue 1-2 https://doi.org/10.1016/j.jnucmat.2005.07.003	journal	December 2005
The effect of grain size, porosity and yttria content on the thermal conductivity of nanocrystalline zirconia Raghavan, Srinivasan; Wang, Hsin; Dinwiddie, Ralph B. Scripta Materialia, Vol. 39, Issue 8 https://doi.org/10.1016/S1359-6462(98)00290-5	journal	September 1998
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 Teske, K.; Ullmann, H.; Rettig, D. Journal of Nuclear Materials, Vol. 116, Issue 2-3 https://doi.org/10.1016/0022-3115(83)90110-1	journal	June 1983
Positions of the Oxygen Atoms in UO2.13 Willis, B. T. M. Nature, Vol. 197, Issue 4869 https://doi.org/10.1038/197755a0	journal	February 1963
Thermal Conductivity Measurements on UO _2+x from 300 to 1,400 K Amaya, Masaki; Kubo, Toshio; Korei, Yoshiaki Journal of Nuclear Science and Technology, Vol. 33, Issue 8 https://doi.org/10.1080/18811248.1996.9731970	journal	August 1996
Crystallite Size Refinement of ZrB ₂ by High-Energy Ball Milling GalÃ¡n, Carlos A.; Ortiz, Angel L.; Guiberteau, Fernando Journal of the American Ceramic Society, Vol. 92, Issue 12 https://doi.org/10.1111/j.1551-2916.2009.03352.x	journal	December 2009
Facile low temperature solid state synthesis of iodoapatite by high-energy ball milling Lu, Fengyuan; Yao, Tiankai; Xu, Jinling RSC Adv., Vol. 4, Issue 73 https://doi.org/10.1039/C4RA05320F	journal	January 2014
Interfacial thermal resistance in nanocrystalline yttria-stabilized zirconia Yang, Ho-Soon; Bai, G. -R.; Thompson, L. J. Acta Materialia, Vol. 50, Issue 9 https://doi.org/10.1016/S1359-6454(02)00057-5	journal	May 2002
The high burn-up structure in nuclear fuel Rondinella, Vincenzo V.; Wiss, Thierry Materials Today, Vol. 13, Issue 12 https://doi.org/10.1016/S1369-7021(10)70221-2	journal	December 2010
Point defects and clustering in uranium dioxide by $LSDA + U$ calculations Geng, Hua Y.; Chen, Ying; Kaneta, Yasunori Physical Review B, Vol. 77, Issue 10 https://doi.org/10.1103/PhysRevB.77.104120	journal	March 2008
Thermal barrier coating materials Clarke, David R.; Phillpot, Simon R. Materials Today, Vol. 8, Issue 6 https://doi.org/10.1016/S1369-7021(05)70934-2	journal	June 2005
The defect structure of hyper-stoichiometric uranium dioxide Willis, B. T. M. Acta Crystallographica Section A, Vol. 34, Issue 1 https://doi.org/10.1107/S0567739478000157	journal	January 1978

Similar Records

Thermal Transport and Fracture Behavior of Sintered Fuel Pellets: Experimental Validation of NEAMS Tool MARMOT

Technical Report · Sat Mar 30 00:00:00 EDT 2019 · OSTI ID:1408189

Lian, Jie; Yao, Tiankai; Gong, Bowen; +4 more

Grain growth and pore coarsening in dense nano-crystalline UO_2+x fuel pellets

Journal Article · Sat Mar 25 00:00:00 EDT 2017 · Journal of the American Ceramic Society · OSTI ID:1408189

Yao, Tiankai; Mo, Kun; Yun, Di; +3 more

Spark plasma sintering (SPS) densified U₃Si₂ pellets: Microstructure control and enhanced mechanical and oxidation properties

Journal Article · Fri Jan 24 00:00:00 EST 2020 · Journal of Alloys and Compounds · OSTI ID:1408189

Gong, Bowen; Yao, Tiankai; Lei, Penghui; +3 more

Title: Dense nanocrystalline UO 2+ x fuel pellets synthesized by high pressure spark plasma sintering

Citation Formats

References (43)

Similar Records

Related Subjects

Title: Dense nanocrystalline UO _{2+ x} fuel pellets synthesized by high pressure spark plasma sintering