Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

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

Abstract

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.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [2];  [2];  [1]
+ Show Author Affiliations
  1. Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, United States
  2. Texas A&M University, 3380 University Drive East, College Station, Texas 77845, United States
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); PNNL Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1395607
Alternate Identifier(s):
OSTI ID: 1507573
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Published Article
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Name: Journal of Physical Chemistry. C Journal Volume: 121 Journal Issue: 40; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Citation Formats

Jiang, Weilin, Conroy, Michele A., Kruska, Karen, Overman, Nicole R., Droubay, Timothy C., Gigax, Jonathan, Shao, Lin, and Devanathan, Ram. Nanoparticle Precipitation in Irradiated and Annealed Ceria Doped with Metals for Emulation of Spent Fuels. United States: N. p., 2017. Web. doi:10.1021/acs.jpcc.7b06188.
Copy to clipboard
Jiang, Weilin, Conroy, Michele A., Kruska, Karen, Overman, Nicole R., Droubay, Timothy C., Gigax, Jonathan, Shao, Lin, & Devanathan, Ram. Nanoparticle Precipitation in Irradiated and Annealed Ceria Doped with Metals for Emulation of Spent Fuels. United States. https://doi.org/10.1021/acs.jpcc.7b06188
Copy to clipboard
Jiang, Weilin, Conroy, Michele A., Kruska, Karen, Overman, Nicole R., Droubay, Timothy C., Gigax, Jonathan, Shao, Lin, and Devanathan, Ram. Wed . "Nanoparticle Precipitation in Irradiated and Annealed Ceria Doped with Metals for Emulation of Spent Fuels". United States. https://doi.org/10.1021/acs.jpcc.7b06188.
Copy to clipboard
@article{osti_1395607,
title = {Nanoparticle Precipitation in Irradiated and Annealed Ceria Doped with Metals for Emulation of Spent Fuels},
author = {Jiang, Weilin and Conroy, Michele A. and Kruska, Karen and Overman, Nicole R. and Droubay, Timothy C. and Gigax, Jonathan and Shao, Lin and Devanathan, Ram},
abstractNote = {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.},
doi = {10.1021/acs.jpcc.7b06188},
journal = {Journal of Physical Chemistry. C},
number = 40,
volume = 121,
place = {United States},
year = {2017},
month = {9}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acs.jpcc.7b06188
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 6 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1. Figure 1.: SRIM simulation of the He concentration and atomic displacement profiles in CeO2 implanted with 90 keV He+ ions at normal incidence.
All figures and tables (16 total)
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Spent Nuclear Fuel
journal, December 2006

In Situ Study of Nanostructure and Electrical Resistance of Nanocluster Films Irradiated with Ion Beams
journal, August 2014

  • Jiang, Weilin; Sundararajan, Jennifer A.; Varga, Tamas
  • Advanced Functional Materials, Vol. 24, Issue 39
  • DOI: 10.1002/adfm.201400553

Nanostructure of metallic particles in light water reactor used nuclear fuel
journal, June 2015

Characterization of alloy particles extracted from spent nuclear fuel
journal, January 2012

Enhanced diffusion mechanisms
journal, January 1978

The chemical state of the fission products in oxide fuels
journal, April 1985

Epitaxial growth and characterization of Ce1−xZrxO2 thin films
journal, May 1999

  • Gao, Y.; Herman, G. S.; Thevuthasan, S.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 17, Issue 3
  • DOI: 10.1116/1.581671

Phase Relationships in the System Zirconia-Ceria
journal, September 1950

Room-temperature epitaxial growth of CeO2(001) thin films on Si(001) substrates by electron beam evaporation
journal, March 2001

  • Ami, T.; Ishida, Y.; Nagasawa, N.
  • Applied Physics Letters, Vol. 78, Issue 10
  • DOI: 10.1063/1.1351849

Nanostructural evolution and behavior of H and Li in ion-implanted γ-LiAlO2
journal, October 2017

Analysis of Three-dimensional Atom-probe Data by the Proximity Histogram
journal, September 2000

  • Hellman, Olof C.; Vandenbroucke, Justin A.; Rüsing, Järg
  • Microscopy and Microanalysis, Vol. 6, Issue 05
  • DOI: 10.1007/S100050010051

International Union of Crystallography. Commission on Powder Diffraction. Rietveld refinement round robin. II. Analysis of monoclinic ZrO 2
journal, October 1994

The surface chemistry of cerium oxide
journal, March 2015

Nuclear Fuel in a Reactor Accident
journal, March 2012

  • Burns, Peter C.; Ewing, Rodney C.; Navrotsky, Alexandra
  • Science, Vol. 335, Issue 6073
  • DOI: 10.1126/science.1211285

Microstructural examination of oxidized spent PWR fuel by transmission electron microscopy
journal, August 1989

SIMS quantification in Si, GaAs, and diamond - an update
journal, May 1995

Diffusion of Ag, Au and Cs implants in MAX phase Ti3SiC2
journal, July 2015

Atomistic simulation of point defects behavior in ceria
journal, December 2008

  • 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
  • DOI: 10.1016/j.nimb.2008.09.010

Fission gas transport and its interactions with irradiation-induced defects in lanthanum doped ceria
journal, February 2012

  • Yun, D.; Ye, B.; Oaks, A. J.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 272
  • DOI: 10.1016/j.nimb.2011.01.074

Growth and structure of epitaxial Ce1−xZrxO2 thin films on yttria-stabilized zirconia (111)
journal, October 2002

  • Kim, Y. J.; Thevuthasan, S.; Shutthananadan, V.
  • Journal of Electron Spectroscopy and Related Phenomena, Vol. 126, Issue 1-3
  • DOI: 10.1016/S0368-2048(02)00151-2

Microstructure and Cs Behavior of Ba-Doped Aluminosilicate Pollucite Irradiated with F + Ions
journal, July 2014

  • Jiang, Weilin; Kovarik, Libor; Zhu, Zihua
  • The Journal of Physical Chemistry C, Vol. 118, Issue 31
  • DOI: 10.1021/jp5045223

Superlattice Structure and Precipitates in O + and Zr + Ion Coimplanted SrTiO 3 : A Model Waste Form for 90 Sr
journal, July 2012

  • Jiang, W.; Van Ginhoven, R. M.; Kovarik, L.
  • The Journal of Physical Chemistry C, Vol. 116, Issue 31
  • DOI: 10.1021/jp301343b

Calculation of the threshold displacement energies in UO2 using ionic potentials
journal, May 2005

Molecular Dynamics Simulation of Fission Fragment Damage in Nuclear Fuel and Surrogate Material
journal, January 2017

Defects and Minor Phases in O + and Zr + Ion Co-implanted SrTiO 3
journal, May 2011

  • Jiang, Weilin; Bowden, Mark E.; Zhu, Zihua
  • Industrial & Engineering Chemistry Research, Vol. 51, Issue 2
  • DOI: 10.1021/ie200267n

Epsilon metal waste form for immobilization of noble metals from used nuclear fuel
journal, October 2013

Corrosion Testing of a Simulated Five-Metal Epsilon Particle in Spent Nuclear Fuel
journal, January 2002

Atomic scale modelling of hexagonal structured metallic fission product alloys
journal, April 2015

  • Middleburgh, S. C.; King, D. M.; Lumpkin, G. R.
  • Royal Society Open Science, Vol. 2, Issue 4
  • DOI: 10.1098/rsos.140292

Thermophysical properties of Mo–Ru–Rh–Pd alloys
journal, April 2003

Control of CeO2 growth by metalorganic chemical vapor deposition with a special source evaporator
journal, June 1995

The fate of the epsilon phase (Mo-Ru-Pd-Tc-Rh) in the UO2 of the Oklo natural fission reactors
journal, January 2006

Structure and bonding at the atomic scale by scanning transmission electron microscopy
journal, April 2009

    Sort by:
    [ × clear filter / sort ]

    Figures / Tables found in this record:

    Figure 1. (p. 2)figure
    Figure 2. (p. 3)figure
    Figure 3. (p. 4)figure
    Figure 4. (p. 4)figure
    Figure 5. (p. 4)figure
    Figure 6. (p. 5)figure
    Figure 7. (p. 5)figure
    Figure 8. (p. 6)figure
    Figure 9. (p. 6)figure
    Table 1. (p. 6)table
    Figure 10. (p. 7)figure
    Figure 11. (p. 7)figure
    Figure 12. (p. 8)figure
    Figure 13. (p. 9)figure
    Figure 14. (p. 9)figure
    Figure 15. (p. 10)figure
      [ × clear filter / sort ]
      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

      Similar Records in DOE PAGES and OSTI.GOV collections: