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Title: Effects of irradiation temperature on the response of CeO2, ThO2, and UO2 to highly ionizing radiation

Abstract

Microcrystalline CeO2, ThO2, and UO2 were irradiated with 198 MeV132Xe ions to the same fluence at temperatures ranging from 25°C to 700°C then characterized by synchrotron X-ray diffraction and X-ray absorption spectroscopy. All samples retain crystallinity and their nominal fluorite-type phase at a fluence of 1.5x1013 ions/cm2. Both CeO2 and ThO2 display defect-induced unit cell expansion after irradiation at room temperature (~0.15% and ~0.10%, respectively), yet as irradiation temperature increases, the maximum swelling produced decreases to ~0.02%. Alternatively, UO2 shows an initial contraction in unit cell parameter (approximately -0.05%), for room temperature irradiation most likely related to irradiation-enhanced annealing or irradiation-induced oxidation. At higher temperatures (above 200°C), UO2 begins to swell, surpassing its unit cell parameter prior to irradiation (~0.05%), an effect which could be attributed to minor reduction in uranium oxidation state in vacuum. However, while CeO2 irradiated at room temperature undergoes partial reduction, both UO2 and ThO2 exhibit no measurable change in cation oxidation state as evidenced by X-ray absorption spectroscopy. All samples display a decrease in irradiation-induced heterogeneous microstrain as a function of increasing irradiation temperature.

Authors:
 [1];  [1];  [2];  [1];  [1];  [3];  [4];  [5];  [1]
+ Show Author Affiliations
  1. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Nuclear Engineering
  2. Stanford Univ., CA (United States). Dept. of Geological Sciences; Harvard Univ., Cambridge, MA (United States)
  3. Inst. of Nuclear Physics, Almaty (Kazakhstan); L.N. Gumilyov Eurasian National Univ., Nur-Sultan (Kazakhstan); Ural Federal Univ., Yekaterinburg (Russia)
  4. Stanford Univ., CA (United States). Dept. of Geological Sciences
  5. Centre National de la Recherche Scientifique (CNRS), Caen (France). Centre de Recherche sur les Ions, les Matériaux et la Photonique (CIMAP), Grand Accelerateur National d'Ions Lourds (GANIL)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA); George Washington Univ., Washington, DC (United States); Univ. of Tennessee, Knoxville, TN (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Programs (DP)
OSTI Identifier:
1559294
Alternate Identifier(s):
OSTI ID: 1562592
Grant/Contract Number:  
NA0003858
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Nuclear Materials
Additional Journal Information:
Journal Volume: 525; Journal Issue: C; Journal ID: ISSN 0022-3115
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; CeO2, ThO2, UO2, ion irradiation, high temperature, x-ray diffraction , x-ray absorption spectroscopy

Citation Formats

Cureton, William F., Palomares, Raul I., Tracy, Cameron L., O'Quinn, Eric C., Walters, Jeffrey, Zdorovets, Maxim, Ewing, Rodney C., Toulemonde, Marcel, and Lang, Maik. Effects of irradiation temperature on the response of CeO2, ThO2, and UO2 to highly ionizing radiation. United States: N. p., 2019. Web. doi:10.1016/j.jnucmat.2019.07.029.
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Cureton, William F., Palomares, Raul I., Tracy, Cameron L., O'Quinn, Eric C., Walters, Jeffrey, Zdorovets, Maxim, Ewing, Rodney C., Toulemonde, Marcel, & Lang, Maik. Effects of irradiation temperature on the response of CeO2, ThO2, and UO2 to highly ionizing radiation. United States. https://doi.org/10.1016/j.jnucmat.2019.07.029
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Cureton, William F., Palomares, Raul I., Tracy, Cameron L., O'Quinn, Eric C., Walters, Jeffrey, Zdorovets, Maxim, Ewing, Rodney C., Toulemonde, Marcel, and Lang, Maik. Fri . "Effects of irradiation temperature on the response of CeO2, ThO2, and UO2 to highly ionizing radiation". United States. https://doi.org/10.1016/j.jnucmat.2019.07.029. https://www.osti.gov/servlets/purl/1559294.
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@article{osti_1559294,
title = {Effects of irradiation temperature on the response of CeO2, ThO2, and UO2 to highly ionizing radiation},
author = {Cureton, William F. and Palomares, Raul I. and Tracy, Cameron L. and O'Quinn, Eric C. and Walters, Jeffrey and Zdorovets, Maxim and Ewing, Rodney C. and Toulemonde, Marcel and Lang, Maik},
abstractNote = {Microcrystalline CeO2, ThO2, and UO2 were irradiated with 198 MeV132Xe ions to the same fluence at temperatures ranging from 25°C to 700°C then characterized by synchrotron X-ray diffraction and X-ray absorption spectroscopy. All samples retain crystallinity and their nominal fluorite-type phase at a fluence of 1.5x1013 ions/cm2. Both CeO2 and ThO2 display defect-induced unit cell expansion after irradiation at room temperature (~0.15% and ~0.10%, respectively), yet as irradiation temperature increases, the maximum swelling produced decreases to ~0.02%. Alternatively, UO2 shows an initial contraction in unit cell parameter (approximately -0.05%), for room temperature irradiation most likely related to irradiation-enhanced annealing or irradiation-induced oxidation. At higher temperatures (above 200°C), UO2 begins to swell, surpassing its unit cell parameter prior to irradiation (~0.05%), an effect which could be attributed to minor reduction in uranium oxidation state in vacuum. However, while CeO2 irradiated at room temperature undergoes partial reduction, both UO2 and ThO2 exhibit no measurable change in cation oxidation state as evidenced by X-ray absorption spectroscopy. All samples display a decrease in irradiation-induced heterogeneous microstrain as a function of increasing irradiation temperature.},
doi = {10.1016/j.jnucmat.2019.07.029},
journal = {Journal of Nuclear Materials},
number = C,
volume = 525,
place = {United States},
year = {Fri Nov 01 00:00:00 EDT 2019},
month = {Fri Nov 01 00:00:00 EDT 2019}
}
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