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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 UO 2. 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 (CeO 2) as a surrogate for UO 2. Polycrystalline CeO 2 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 CeO 2 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]
  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) (SC-23); 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.
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. doi:10.1021/acs.jpcc.7b06188.
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. doi:10.1021/acs.jpcc.7b06188.
@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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1021/acs.jpcc.7b06188

Citation Metrics:
Cited by: 2 works
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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.

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