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

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

doi:10.1021/acs.jpcc.8b11027

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

Journal Article · Tue Jan 08 04:00:00 EST 2019 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.8b11027· OSTI ID:1502051

^[1]; Conroy, Michele A. ^[1]; Kruska, Karen ^[1]; Olszta, Matthew J. ^[1]; Droubay, Timothy C. ^[1]; Schwantes, Jon M. ^[1]; Taylor, Caitlin A. ^[2]; Price, Patrick M. ^[2]; Hattar, Khalid ^[2]; Devanathan, Ram ^[1]

Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, United States
Sandia National Laboratories, P.O. Box 5800, Albuquerque, New Mexico 87185, United States

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.

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)

DOE Contract Number:: AC04-94AL85000; AC05-76RL01830; NA0003525

OSTI ID:: 1502051

Report Number(s):: PNNL-SA--139442

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 4 Vol. 123; ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

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Cited By (2)

A new non-diffusional gas bubble production route in used nuclear fuel: implications for fission gas release, cladding corrosion, and next generation fuel design Schwantes, Jon M.; Bair, Jacob L.; Buck, Edgar C. Physical Chemistry Chemical Physics, Vol. 22, Issue 11 https://doi.org/10.1039/c9cp05363h	journal	January 2020
Changing the rules of the game: used fuel studies outside of a remote handling facility Schwantes, Jon M.; Conroy, Michele; Lach, Timothy G. Journal of Radioanalytical and Nuclear Chemistry, Vol. 322, Issue 3 https://doi.org/10.1007/s10967-019-06921-y	journal	November 2019

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Related Subjects

Particle precipitation
in situ heating STEM
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in situ heating XPS
Ceria