The development of advanced fuel fabrication technologies is important for developing accident-tolerant fuels and engineering fuels for safer and more effective nuclear energy systems. In this work, commercial-size uranium dioxide (UO2) fuel pellets with a theoretical density of 95% were consolidated by spark plasma sintering (SPS) at 1600°C for 5 min. Systematic investigations suggest uniform densification and stoichiometric UO2 with an ideal fluorite structure across the commercial-size fuel pellet, but with a distributed grain structure because of non-uniform distribution of temperature during sintering. This work demonstrates a great potential of using SPS for fabricating nuclear fuels at a cost-effective manner.
This is a preview of subscription content, access via your institution.
Buy single article
Instant access to the full article PDF.
Tax calculation will be finalised during checkout.
IAEA: Current trends in nuclear fuel for power reactors. (2007) Available at: https://www.iaea.org/About/Policy/GC/GC51/GC51InfDocuments/English/gc51inf-3-att5_en.pdf (accessed June 17, 2018).
IAEA: Accident tolerant fuel concepts for light water reactors. (2014) Available at: https://www.iaea.org/publications/10972/accident-tolerant-fuel-concepts-for-light-water-reactors (accessed June 17, 2018).
R.A. Wolfe and S.F. Kaufman: Mechanical properties of oxide fuels. (1967) Available at: https://www.osti.gov/servlets/purl/4511674 (accessed June 17, 2018).
I. Amato, R.L. Colombo, and A.M.P. Balzari: Hot-pressing of uranium dioxide. J. Nucl. Mater. 20, 210 (1966).
J. Williams, E. Barnes, R. Scott, and A. Hall: Sintering of uranium oxides of composition UO2 to U3O8 in various atmospheres. J. Nucl. Mater. 1, 28 (1959).
A.J. Carrea: Sintering of uranium dioxide in an atmosphere of controlled hydrogen content. J. Nucl. Mater. 8, 275 (1963).
T.R.G. Kutty, K.N. Chandrasekharan, J.P. Panakkal, and J.K. Ghosh: Fracture-toughness and fracture surface-energy of sintered uranium-dioxide fuel pellets. J. Mater. Sci. Lett. 6, 260 (1987).
V.V. Novikov, R.B. Sivov, E.N. Mikheev, and A.V. Fedotov: Fracture toughness of vver and pwr uranium-dioxide fuel pellets with different grain size. At. Energy 118, 117 (2015).
K. Yamada, K. Kurosaki, M. Uno, and S. Yamanaka: Evaluation of thermal properties of uranium dioxide by molecular dynamics. J. Alloys Compd. 307, 10 (2000).
T. Arima, S. Yamasaki, Y. Inagaki, and K. Idemitsu: Evaluation of thermal properties of UO2 and PuO2 by equilibrium molecular dynamics simulations from 300 to 2000 K. J. Alloys Compd. 400, 43 (2005).
J.H. Harding and D.G. Martin: A recommendation for the thermal-conductivity of UO2. J. Nucl. Mater. 166, 223 (1989).
T. Watanabe, S.B. Sinnott, J.S. Tulenko, R.W. Grimes, P.K. Schelling, and S.R. Phillpot: Thermal transport properties of uranium dioxide by molecular dynamics simulations. J. Nucl. Mater. 375, 388 (2008).
S. Wei, Z.H. Zhang, X.B. Shen, F.C. Wang, M.Y. Sun, R. Yang, and S.K. Lee: Simulation of temperature and stress distributions in functionally graded materials synthesized by a spark plasma sintering process. Comput. Mater. Sci. 60, 168 (2012).
L.H. Ge, G. Subhash, R.H. Baney, J.S. Tulenko, and E. McKenna: Densification of uranium dioxide fuel pellets prepared by spark plasma sintering (SPS). J. Nucl. Mater. 435, 1 (2013).
V. Tyrpekl, M. Naji, M. Holzhauser, D. Freis, D. Prieur, P. Martin, B. Cremer, M. Murray-Farthing, and M. Cologna: On the role of the electrical field in spark plasma sintering of UO2+x. Sci. Rep. 7, 46625 (2017).
T.K. Yao, S.M. Scott, G.Q. Xin, B.W. Gong, and J. Lian: Dense nanocrystalline UO2+x fuel pellets synthesized by high pressure spark plasma sintering. J. Am. Ceram. Soc. 101, 1105 (2018).
T.K. Yao, K. Mo, D. Yun, S. Nanda, A.M. Yacout, and J. Lian: Grain growth and pore coarsening in dense nano-crystalline UO2+x fuel pellets. J. Am. Ceram. Soc. 100, 2651 (2017).
M. Sopicka-lizer: Introduction to mechanochemical processing. (Woodhead Publishing, Cambridge, England, 2010), p. 1.
A. Wank and B. Wielage: High energy ball milling–a promising route for production of tailored thermal spray consumables. (Conference on Modern wear and corrosion resistant coatings obtained by thermal spraying, Warsaw, Poland, 2003).
K. Teske, H. Ullmann, and D. Rettig: 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. J. Nucl. Mater. 116, 260 (1983).
L.H. Ge, G. Subhash, R.H. Baney, and J.S. Tulenko: Influence of processing parameters on thermal conductivity of uranium dioxide pellets prepared by spark plasma sintering. J. Eur. Ceram. Soc. 34, 1791 (2014).
S. Gossé, C. Guéneau, T. Alpettaz, S. Chatain, C. Chatillon, and F. Le Guyadec: Kinetic study of the UO2/C interaction by high-temperature mass spectrometry. Nucl. Eng. Des. 238, 2866 (2008).
S. Gossé, C. Guéneau, C. Chatillon, and S. Chatain: Critical review of carbon monoxide pressure measurements in the uranium–carbon–oxygen ternary system. J. Nucl. Mater. 352, 13 (2006).
J.E. Burke and D. Turnbull: Recrystallization and grain growth. Prog. Met. Phys. 3, 220 (1952).
W.D. Kingery and B. Francois: Grain growth in porous compacts. J. Am. Ceram. Soc. 48, 546 (1965).
F.A. Nichols: Theory of grain growth in porous compacts. J. Appl. Phys. 37, 4599 (1966).
J. Diatta, G. Antou, N. Pradeilles, and A. Maître: Numerical modeling of spark plasma sintering—discussion on densification mechanism identification and generated porosity gradients. J. Eur. Ceram. Soc. 37, 4849 (2017).
P. Mondalek, L. Silva, and M. Bellet: A numerical model for powder densification by sps technique. Adv. Eng. Mater. 13, 587 (2011).
C. Wang, Z. Zhao, and L.F. Cheng: Finite element modeling of temperature distribution in spark plasma sintering. Key Eng. Mater. 434–435, 808 (2010).
P.R. Graves: Raman microprobe spectroscopy of uranium-dioxide single-crystals and ion-implanted polycrystals. Appl. Spectrosc. 44, 1665 (1990).
W.B. White: Application of infrared spectroscopy to order-disorder problems in simple ionic solids. Mater. Res. Bull. 2, 381 (1967).
M. Razdan and D.W. Shoesmith: Influence of trivalent-dopants on the structural and electrochemical properties of uranium dioxide (UO2). J. Electrochem. Soc. 161, H105 (2014).
M. Razdan and D.W. Shoesmith: The electrochemical reactivity of 6.0 wt% gd-doped UO2 in aqueous carbonate/bicarbonate solutions. J. Electrochem. Soc. 161, H225 (2014).
G.C. Allen, I.S. Butler, and N.A. Tuan: Characterization of uranium-oxides by micro-Raman spectroscopy. J. Nucl. Mater. 144, 17 (1987).
M.L. Palacios and S.H. Taylor: Characterization of uranium oxides using in situ micro-Raman spectroscopy. Appl. Spectrosc. 54, 1372 (2000).
D. Manara and B. Renker: Raman spectra of stoichiometric and hyperstoichiometric uranium dioxide. J. Nucl. Mater. 321, 233 (2003).
M. Naji, J.Y. Colle, O. Benes, M. Sierig, J. Rautio, P. Lajarge, and D. Manara: An original approach for Raman spectroscopy analysis of radioactive materials and its application to americium-containing samples. J. Raman Spectrosc. 46, 750 (2015).
M. Chollet, D. Prieur, R. Bohler, R. Belin, and D. Manara: The melting behaviour of uranium/neptunium mixed oxides. J. Chem. Thermodyn. 89, 27 (2015).
T. Livneh and E. Sterer: Effect of pressure on the resonant multiphonon Raman scattering in UO2. Phys. Rev. B 73, 085118 (2006).
L. Desgranges, G. Guimbretiere, P. Simon, C. Jegou, and R. Caraballo: A possible new mechanism for defect formation in irradiated UO2. Nucl. Instrum. Methods. B 315, 169 (2013).
L. Desgranges, G. Baldinozzi, P. Simon, G. Guimbretière, and A. Canizares: Raman spectrum of U4O9: a new interpretation of damage lines in UO2. J. Raman Spectrosc. 43, 455 (2012).
M.a.S. Razdan and David W: The electrochemical reactivity of 6.0 wt% Gd-doped UO2 in aqueous carbonate/bicarbonate solutions. J. Electrochem. Soc. 161, H225 (2014).
H. He and D. Shoesmith: Raman spectroscopic studies of defect structures and phase transition in hyper-stoichiometric UO(2+x). Phys. Chem. Chem. Phys. 12, 8108 (2010).
D. Ho Mer Lin, D. Manara, P. Lindqvist-Reis, T. Fanghänel, and K. Mayer: The use of different dispersive Raman spectrometers for the analysis of uranium compounds. Vib. Spectrosc. 73, 102 (2014).
F. Pointurier and O. Marie: Identification of the chemical forms of uranium compounds in micrometer-size particles by means of micro-Raman spectrometry and scanning electron microscope. Spectrochim. Acta Part B 65, 797 (2010).
J. Schoenes: Recent spectroscopic studies of UO2. J. Chem. Soc. Faraday Trans. 283, 1205 (1987).
This work is supported by the US Department of Energy, Office of Nuclear Energy under a Nuclear Engineer University Program (award number: DE-NE0008440) and an internal support by Westinghouse Electric Company in developing advanced technology for fuel fabrication.
About this article
Cite this article
Gong, B., Yao, T., Lu, C. et al. Consolidation of commercial-size UO2 fuel pellets using spark plasma sintering and microstructure/microchemical analysis. MRS Communications 8, 979–987 (2018). https://doi.org/10.1557/mrc.2018.121