Nanoparticle Precipitation in Irradiated and Annealed Ceria Doped with Metals for Emulation of Spent Fuels

Jiang, Weilin; Conroy, Michele A.; Kruska, Karen; Overman, Nicole R.; Droubay, Timothy C.; Gigax, Jonathan; Shao, Lin; Devanathan, Ram

doi:10.1021/acs.jpcc.7b06188

Title: Nanoparticle Precipitation in Irradiated and Annealed Ceria Doped with Metals for Emulation of Spent Fuels

Journal Article · Wed Sep 20 00:00:00 EDT 2017 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.7b06188· OSTI ID:1395607

^[1]; Conroy, Michele A. ^[1]; Kruska, Karen ^[1]; Overman, Nicole R. ^[1]; Droubay, Timothy C. ^[1]; Gigax, Jonathan ^[2]; Shao, Lin ^[2]; Devanathan, Ram ^[1]

Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, United States
Texas A&M University, 3380 University Drive East, College Station, Texas 77845, United States

Epsilon-phase alloy precipitates have been observed with varied compositions and sizes in spent nuclear fuels, such as UO₂. The presence of the inclusions, along with other oxide precipitates, gas bubbles, and irradiation-induced structural defects, can significantly degrade the physical properties of the fuel. To predict fuel performance, a fundamental study of the precipitation processes is needed. This study uses ceria (CeO₂) as a surrogate for UO₂. Polycrystalline CeO₂ films doped with Mo, Ru, Rh, Pd, and Re (surrogate for Tc) were grown at 823 K using pulsed laser deposition, irradiated at 673 K with He⁺ ions, and subsequently annealed at higher temperatures. A number of methods, including transmission electron microscopy and atom probe tomography, were applied to characterize the samples. The results indicate that there is a uniform distribution of the doped metals in the as-grown CeO₂ film. Pd particles of ~3 nm in size appear near the dislocation edges after He⁺ ion irradiation to ~13 dpa. Thermal annealing at 1073 K in air leads to formation of precipitates of Mo and Pd near the grain boundaries. Further annealing at 1373 K produces 70 nm sized precipitates consisting of nanograins at cavities.

View Journal Article

Cite

Export

Save

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER); PNNL Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1395607

Alternate ID(s):: OSTI ID: 1507573

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Vol. 121 Journal Issue: 40; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 6 works

Citation information provided by
Web of Science

References (32)

Spent Nuclear Fuel Bruno, J.; Ewing, R. C. Elements, Vol. 2, Issue 6 https://doi.org/10.2113/gselements.2.6.343	journal	December 2006
In Situ Study of Nanostructure and Electrical Resistance of Nanocluster Films Irradiated with Ion Beams Jiang, Weilin; Sundararajan, Jennifer A.; Varga, Tamas Advanced Functional Materials, Vol. 24, Issue 39 https://doi.org/10.1002/adfm.201400553	journal	August 2014
Nanostructure of metallic particles in light water reactor used nuclear fuel Buck, Edgar C.; Mausolf, Edward J.; McNamara, Bruce K. Journal of Nuclear Materials, Vol. 461 https://doi.org/10.1016/j.jnucmat.2015.03.001	journal	June 2015
Characterization of alloy particles extracted from spent nuclear fuel Cui, D.; Rondinella, V. V.; Fortner, J. A. Journal of Nuclear Materials, Vol. 420, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2011.10.015	journal	January 2012
Enhanced diffusion mechanisms Bourgoin, J. C.; Corbett, J. W. Radiation Effects, Vol. 36, Issue 3-4 https://doi.org/10.1080/00337577808240846	journal	January 1978
The chemical state of the fission products in oxide fuels Kleykamp, H. Journal of Nuclear Materials, Vol. 131, Issue 2-3, p. 221-246 https://doi.org/10.1016/0022-3115(85)90460-X	journal	April 1985
Epitaxial growth and characterization of Ce1−xZrxO2 thin films Gao, Y.; Herman, G. S.; Thevuthasan, S. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 17, Issue 3 https://doi.org/10.1116/1.581671	journal	May 1999
Composition and structure of fission product precipitates in irradiated oxide fuels: Correlation with phase studies in the Mo-Ru-Rh-Pd and BaO-UO2-ZrO2-MoO2 Systems Kleykamp, H.; Paschoal, J. O.; Pejsa, R. Journal of Nuclear Materials, Vol. 130 https://doi.org/10.1016/0022-3115(85)90329-0	journal	February 1985
Phase Relationships in the System Zirconia-Ceria Duwez, Pol; Odell, Francis Journal of the American Ceramic Society, Vol. 33, Issue 9 https://doi.org/10.1111/j.1151-2916.1950.tb12798.x	journal	September 1950
Room-temperature epitaxial growth of CeO2(001) thin films on Si(001) substrates by electron beam evaporation Ami, T.; Ishida, Y.; Nagasawa, N. Applied Physics Letters, Vol. 78, Issue 10 https://doi.org/10.1063/1.1351849	journal	March 2001
Nanostructural evolution and behavior of H and Li in ion-implanted γ-LiAlO2 Jiang, Weilin; Zhang, Jiandong; Edwards, Danny J. Journal of Nuclear Materials, Vol. 494 https://doi.org/10.1016/j.jnucmat.2017.07.048	journal	October 2017
International Union of Crystallography. Commission on Powder Diffraction. Rietveld refinement round robin. II. Analysis of monoclinic ZrO ₂ Hill, R. J.; Cranswick, L. M. D. Journal of Applied Crystallography, Vol. 27, Issue 5 https://doi.org/10.1107/S0021889894000646	journal	October 1994
The surface chemistry of cerium oxide Mullins, David R. Surface Science Reports, Vol. 70, Issue 1 https://doi.org/10.1016/j.surfrep.2014.12.001	journal	March 2015
Nuclear Fuel in a Reactor Accident Burns, Peter C.; Ewing, Rodney C.; Navrotsky, Alexandra Science, Vol. 335, Issue 6073 https://doi.org/10.1126/science.1211285	journal	March 2012
Microstructural examination of oxidized spent PWR fuel by transmission electron microscopy Thomas, L. E.; Einziger, R. E.; Woodley, R. E. Journal of Nuclear Materials, Vol. 166, Issue 3 https://doi.org/10.1016/0022-3115(89)90221-3	journal	August 1989
SIMS quantification in Si, GaAs, and diamond - an update Wilson, R. G. International Journal of Mass Spectrometry and Ion Processes, Vol. 143 https://doi.org/10.1016/0168-1176(94)04136-U	journal	May 1995
Diffusion of Ag, Au and Cs implants in MAX phase Ti3SiC2 Jiang, Weilin; Henager, Charles H.; Varga, Tamas Journal of Nuclear Materials, Vol. 462 https://doi.org/10.1016/j.jnucmat.2015.04.002	journal	July 2015
Atomistic simulation of point defects behavior in ceria Guglielmetti, Aurore; Chartier, Alain; Brutzel, Laurent van Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 266, Issue 24 https://doi.org/10.1016/j.nimb.2008.09.010	journal	December 2008
Fission gas transport and its interactions with irradiation-induced defects in lanthanum doped ceria Yun, D.; Ye, B.; Oaks, A. J. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 272 https://doi.org/10.1016/j.nimb.2011.01.074	journal	February 2012
Growth and structure of epitaxial Ce1−xZrxO2 thin films on yttria-stabilized zirconia (111) Kim, Y. J.; Thevuthasan, S.; Shutthananadan, V. Journal of Electron Spectroscopy and Related Phenomena, Vol. 126, Issue 1-3 https://doi.org/10.1016/S0368-2048(02)00151-2	journal	October 2002
Microstructure and Cs Behavior of Ba-Doped Aluminosilicate Pollucite Irradiated with F ⁺ Ions Jiang, Weilin; Kovarik, Libor; Zhu, Zihua The Journal of Physical Chemistry C, Vol. 118, Issue 31 https://doi.org/10.1021/jp5045223	journal	July 2014
Superlattice Structure and Precipitates in O ⁺ and Zr ⁺ Ion Coimplanted SrTiO ₃ : A Model Waste Form for ⁹⁰ Sr Jiang, W.; Van Ginhoven, R. M.; Kovarik, L. The Journal of Physical Chemistry C, Vol. 116, Issue 31 https://doi.org/10.1021/jp301343b	journal	July 2012
Calculation of the threshold displacement energies in UO2 using ionic potentials Meis, C.; Chartier, A. Journal of Nuclear Materials, Vol. 341, Issue 1 https://doi.org/10.1016/j.jnucmat.2005.01.001	journal	May 2005
Molecular Dynamics Simulation of Fission Fragment Damage in Nuclear Fuel and Surrogate Material Devanathan, Ram MRS Advances, Vol. 2, Issue 21-22 https://doi.org/10.1557/adv.2017.9	journal	January 2017
Defects and Minor Phases in O ⁺ and Zr ⁺ Ion Co-implanted SrTiO ₃ Jiang, Weilin; Bowden, Mark E.; Zhu, Zihua Industrial & Engineering Chemistry Research, Vol. 51, Issue 2 https://doi.org/10.1021/ie200267n	journal	May 2011
Epsilon metal waste form for immobilization of noble metals from used nuclear fuel Crum, Jarrod V.; Strachan, Denis; Rohatgi, Aashish Journal of Nuclear Materials, Vol. 441, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.05.043	journal	October 2013
Corrosion Testing of a Simulated Five-Metal Epsilon Particle in Spent Nuclear Fuel Wronkiewicz, D. J.; Watkins, C. S.; Baughman, A. C. MRS Proceedings, Vol. 713 https://doi.org/10.1557/PROC-713-JJ14.4	journal	January 2002
Atomic scale modelling of hexagonal structured metallic fission product alloys Middleburgh, S. C.; King, D. M.; Lumpkin, G. R. Royal Society Open Science, Vol. 2, Issue 4 https://doi.org/10.1098/rsos.140292	journal	April 2015
Thermophysical properties of Mo–Ru–Rh–Pd alloys Yamanaka, Shinsuke; Kurosaki, Ken Journal of Alloys and Compounds, Vol. 353, Issue 1-2 https://doi.org/10.1016/S0925-8388(02)01211-2	journal	April 2003
Control of CeO2 growth by metalorganic chemical vapor deposition with a special source evaporator Liang, S.; Chern, C. S.; Shi, Z. Q. Journal of Crystal Growth, Vol. 151, Issue 3-4 https://doi.org/10.1016/0022-0248(95)00061-5	journal	June 1995
The fate of the epsilon phase (Mo-Ru-Pd-Tc-Rh) in the UO2 of the Oklo natural fission reactors Utsunomiya, Satoshi; Ewing, Rodney C. Radiochimica Acta, Vol. 94, Issue 9-11 https://doi.org/10.1524/ract.2006.94.9-11.749	journal	January 2006
Structure and bonding at the atomic scale by scanning transmission electron microscopy Muller, David A. Nature Materials, Vol. 8, Issue 4 https://doi.org/10.1038/nmat2380	journal	April 2009