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Title: In Situ Study of Particle Precipitation in Metal-Doped CeO 2 during Thermal Treatment and Ion Irradiation for Emulation of Irradiating Fuels

Abstract

Metallic particles formed in oxide fuels (e.g., UO2) during neutron irradiation have an adverse impact on fuel performance. A fundamental investigation of the particle precipitation is needed to predict the fuel performance and potentially improve fuel designs and operations. This study reports on the precipitation of Mo-dominant beta-phase particles in polycrystalline CeO2 (surrogate for UO2) films doped with Mo, Pd, Rh, Ru and Re (surrogate for Tc). In situ heating scanning transmission electron microscopy (STEM) data indicate that particle precipitation starts at ~1073 K with a limited particle growth to ~10 nm. While particle density increases with increasing temperature, particle size remains largely unchanged up to 1273 K. There is a dramatic change in the microstructure following vacuum annealing at 1373 K, probably due to phase transition of cerium oxide. At the high temperature, particles grow up to 75 nm or larger with distinctive facets. The particles are predominantly composed of Mo with a body-centered cubic structure (beta phase). An oxide layer was observed after storage at ambient conditions. In situ heating x-ray photoelectron spectroscopy (XPS) reveals an increasing reduction of Ce charge state from 4+ to 3+ in the doped CeO2 film from 673 K to 1273 K. Inmore » situ ion irradiation TEM with 2 MeV Al2+ ions up to a dose of ~20 displacements per atom (dpa) at nominally room temperature does not lead to precipitation of visible particles. However, irradiation with 1,7 MeV Au3+ ions to ~10 dpa at 973 K produces ~2 nm sized pure Pd particles; Au3+ irradiation at 1173 K appears to result in precipitates of ~6 nm in size.« less

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [2];  [2];  [2];  [1]
  1. Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, United States
  2. Sandia National Laboratories, P.O. Box 5800, Albuquerque, New Mexico 87185, United States
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1502051
Report Number(s):
PNNL-SA-139442
Journal ID: ISSN 1932-7447
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 123; Journal Issue: 4; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
Particle precipitation, in situ heating STEM, in situ ion irradiation TEM, in situ heating XPS, Ceria

Citation Formats

Jiang, Weilin, Conroy, Michele A., Kruska, Karen, Olszta, Matthew J., Droubay, Timothy C., Schwantes, Jon M., Taylor, Caitlin A., Price, Patrick M., Hattar, Khalid, and Devanathan, Ram. In Situ Study of Particle Precipitation in Metal-Doped CeO 2 during Thermal Treatment and Ion Irradiation for Emulation of Irradiating Fuels. United States: N. p., 2019. Web. doi:10.1021/acs.jpcc.8b11027.
Jiang, Weilin, Conroy, Michele A., Kruska, Karen, Olszta, Matthew J., Droubay, Timothy C., Schwantes, Jon M., Taylor, Caitlin A., Price, Patrick M., Hattar, Khalid, & Devanathan, Ram. In Situ Study of Particle Precipitation in Metal-Doped CeO 2 during Thermal Treatment and Ion Irradiation for Emulation of Irradiating Fuels. United States. doi:10.1021/acs.jpcc.8b11027.
Jiang, Weilin, Conroy, Michele A., Kruska, Karen, Olszta, Matthew J., Droubay, Timothy C., Schwantes, Jon M., Taylor, Caitlin A., Price, Patrick M., Hattar, Khalid, and Devanathan, Ram. Tue . "In Situ Study of Particle Precipitation in Metal-Doped CeO 2 during Thermal Treatment and Ion Irradiation for Emulation of Irradiating Fuels". United States. doi:10.1021/acs.jpcc.8b11027.
@article{osti_1502051,
title = {In Situ Study of Particle Precipitation in Metal-Doped CeO 2 during Thermal Treatment and Ion Irradiation for Emulation of Irradiating Fuels},
author = {Jiang, Weilin and Conroy, Michele A. and Kruska, Karen and Olszta, Matthew J. and Droubay, Timothy C. and Schwantes, Jon M. and Taylor, Caitlin A. and Price, Patrick M. and Hattar, Khalid and Devanathan, Ram},
abstractNote = {Metallic particles formed in oxide fuels (e.g., UO2) during neutron irradiation have an adverse impact on fuel performance. A fundamental investigation of the particle precipitation is needed to predict the fuel performance and potentially improve fuel designs and operations. This study reports on the precipitation of Mo-dominant beta-phase particles in polycrystalline CeO2 (surrogate for UO2) films doped with Mo, Pd, Rh, Ru and Re (surrogate for Tc). In situ heating scanning transmission electron microscopy (STEM) data indicate that particle precipitation starts at ~1073 K with a limited particle growth to ~10 nm. While particle density increases with increasing temperature, particle size remains largely unchanged up to 1273 K. There is a dramatic change in the microstructure following vacuum annealing at 1373 K, probably due to phase transition of cerium oxide. At the high temperature, particles grow up to 75 nm or larger with distinctive facets. The particles are predominantly composed of Mo with a body-centered cubic structure (beta phase). An oxide layer was observed after storage at ambient conditions. In situ heating x-ray photoelectron spectroscopy (XPS) reveals an increasing reduction of Ce charge state from 4+ to 3+ in the doped CeO2 film from 673 K to 1273 K. In situ ion irradiation TEM with 2 MeV Al2+ ions up to a dose of ~20 displacements per atom (dpa) at nominally room temperature does not lead to precipitation of visible particles. However, irradiation with 1,7 MeV Au3+ ions to ~10 dpa at 973 K produces ~2 nm sized pure Pd particles; Au3+ irradiation at 1173 K appears to result in precipitates of ~6 nm in size.},
doi = {10.1021/acs.jpcc.8b11027},
journal = {Journal of Physical Chemistry. C},
issn = {1932-7447},
number = 4,
volume = 123,
place = {United States},
year = {2019},
month = {1}
}