An XPS study on the impact of relative humidity on the aging of UO2 powders
Abstract
High resolution x-ray photoemission spectroscopy (XPS) was used to characterize the chemical speciation of high purity uranium dioxide (UO2) powder samples following aging for periods of up to one year under controlled conditions with relative humidity ranging from 34% to 98%. A systematic shift to higher uranium oxidation states, and thus an increase in the mean uranium valence, was found to directly correlate with the dose of water received (i.e. the product of exposure time and relative humidity). Exposure duration was found to have a greater impact on sample aging than relative humidity. Lastly, the sample aged at 98% relative humidity was found to have unique structural differences for exposure time beyond 180 days when observed by scanning electron microscopy (SEM).
- Authors:
-
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1347674
- Alternate Identifier(s):
- OSTI ID: 1411827
- Report Number(s):
- LLNL-JRNL-704464
Journal ID: ISSN 0022-3115; TRN: US1700867
- Grant/Contract Number:
- AC52-07NA27344
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Nuclear Materials
- Additional Journal Information:
- Journal Volume: 487; Journal Issue: C; Journal ID: ISSN 0022-3115
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
Citation Formats
Donald, Scott B., Dai, Zurong R., Davisson, M. Lee, Jeffries, Jason R., and Nelson, Art J. An XPS study on the impact of relative humidity on the aging of UO2 powders. United States: N. p., 2017.
Web. doi:10.1016/j.jnucmat.2017.02.016.
Donald, Scott B., Dai, Zurong R., Davisson, M. Lee, Jeffries, Jason R., & Nelson, Art J. An XPS study on the impact of relative humidity on the aging of UO2 powders. United States. https://doi.org/10.1016/j.jnucmat.2017.02.016
Donald, Scott B., Dai, Zurong R., Davisson, M. Lee, Jeffries, Jason R., and Nelson, Art J. Fri .
"An XPS study on the impact of relative humidity on the aging of UO2 powders". United States. https://doi.org/10.1016/j.jnucmat.2017.02.016. https://www.osti.gov/servlets/purl/1347674.
@article{osti_1347674,
title = {An XPS study on the impact of relative humidity on the aging of UO2 powders},
author = {Donald, Scott B. and Dai, Zurong R. and Davisson, M. Lee and Jeffries, Jason R. and Nelson, Art J.},
abstractNote = {High resolution x-ray photoemission spectroscopy (XPS) was used to characterize the chemical speciation of high purity uranium dioxide (UO2) powder samples following aging for periods of up to one year under controlled conditions with relative humidity ranging from 34% to 98%. A systematic shift to higher uranium oxidation states, and thus an increase in the mean uranium valence, was found to directly correlate with the dose of water received (i.e. the product of exposure time and relative humidity). Exposure duration was found to have a greater impact on sample aging than relative humidity. Lastly, the sample aged at 98% relative humidity was found to have unique structural differences for exposure time beyond 180 days when observed by scanning electron microscopy (SEM).},
doi = {10.1016/j.jnucmat.2017.02.016},
journal = {Journal of Nuclear Materials},
number = C,
volume = 487,
place = {United States},
year = {Fri Feb 10 00:00:00 EST 2017},
month = {Fri Feb 10 00:00:00 EST 2017}
}
Web of Science
Works referenced in this record:
Inhibition of hydrogen chemisorption on uranium surfaces by traces of water vapor
journal, November 2007
- Tiferet, E.; Mintz, M. H.; Jacob, I.
- Surface Science, Vol. 601, Issue 21
A detailed study of UO2 to U3O8 oxidation phases and the associated rate-limiting steps
journal, September 2006
- Rousseau, G.; Desgranges, L.; Charlot, F.
- Journal of Nuclear Materials, Vol. 355, Issue 1-3
A review of the oxidation of uranium dioxide at temperatures below 400°C
journal, April 1998
- McEachern, R. J.; Taylor, P.
- Journal of Nuclear Materials, Vol. 254, Issue 2-3
Neutron Diffraction Study of the in Situ Oxidation of UO 2
journal, August 2009
- Desgranges, Lionel; Baldinozzi, Gianguido; Rousseau, Gurvan
- Inorganic Chemistry, Vol. 48, Issue 16
Actinide Dioxides in Water: Interactions at the Interface
journal, November 2011
- Alexandrov, Vitaly; Shvareva, Tatiana Y.; Hayun, Shmuel
- The Journal of Physical Chemistry Letters, Vol. 2, Issue 24
XPS determination of uranium oxidation states: XPS determination of uranium oxidation states
journal, October 2011
- Ilton, Eugene S.; Bagus, Paul S.
- Surface and Interface Analysis, Vol. 43, Issue 13
Surface reactions of uranium oxide powder, thin films and single crystals
journal, March 2010
- Idriss, H.
- Surface Science Reports, Vol. 65, Issue 3
XPS spectra of uranyl minerals and synthetic uranyl compounds. II: The O 1s spectrum
journal, May 2009
- Schindler, M.; Hawthorne, F. C.; Freund, M. S.
- Geochimica et Cosmochimica Acta, Vol. 73, Issue 9
The reactions of water vapour on the surfaces of stoichiometric and reduced uranium dioxide: A high resolution XPS study
journal, February 2007
- Senanayake, S. D.; Waterhouse, G. I. N.; Chan, A. S. Y.
- Catalysis Today, Vol. 120, Issue 2
Visualizing different uranium oxidation states during the surface alteration of uraninite and uranium tetrachloride
journal, June 2009
- Grossmann, Kay; Arnold, Thuro; Steudtner, Robin
- Naturwissenschaften, Vol. 96, Issue 8
Low-Temperature Oxidation of Fine UO 2 Powders: A Process of Nanosized Domain Development
journal, March 2016
- Leinders, Gregory; Pakarinen, Janne; Delville, Rémi
- Inorganic Chemistry, Vol. 55, Issue 8
First-principles study of water adsorption and dissociation on the UO2 (1 1 1), (1 1 0) and (1 0 0) surfaces
journal, November 2014
- Bo, Tao; Lan, Jian-Hui; Zhao, Yao-Lin
- Journal of Nuclear Materials, Vol. 454, Issue 1-3
First-Principles Study of Water Reaction and H 2 Formation on UO 2 (111) and (110) Single Crystal Surfaces
journal, September 2014
- Bo, Tao; Lan, Jian-Hui; Wang, Cong-Zhi
- The Journal of Physical Chemistry C, Vol. 118, Issue 38
Ab Initio Atomistic Thermodynamics of Water Reacting with Uranium Dioxide Surfaces
journal, April 2014
- Maldonado, P.; Evins, L. Z.; Oppeneer, P. M.
- The Journal of Physical Chemistry C, Vol. 118, Issue 16
Adsorption of water on UO2 (111) surface: Density functional theory calculations
journal, August 2014
- Tian, Xiao-feng; Wang, Hui; Xiao, Hong-xing
- Computational Materials Science, Vol. 91
On the role of strong electron correlations in the surface properties and chemistry of uranium dioxide
journal, January 2013
- Weck, Philippe F.; Kim, Eunja; Jové-Colón, Carlos F.
- Dalton Transactions, Vol. 42, Issue 13
Electron correlations in narrow energy bands
journal, November 1963
- Hubbard, J.
- Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, Vol. 276, Issue 1365, p. 238-257
Thermal Evolution of Hydrogen Following Water Adsorption on Defective UO 2 (100)
journal, January 2004
- Stultz, J.; Paffett, M. T.; Joyce, S. A.
- The Journal of Physical Chemistry B, Vol. 108, Issue 7
Water chemisorption on a sputter deposited uranium dioxide film — Effect of defects
journal, October 2014
- Cohen, S.; Mintz, M. H.; Zalkind, S.
- Solid State Ionics, Vol. 263
Interaction of water vapor with UO2(001)
journal, January 2000
- Hedhili, M. N.; Yakshinskiy, B. V.; Madey, T. E.
- Surface Science, Vol. 445, Issue 2-3
Oxidation and Hydration of U 3 O 8 Materials Following Controlled Exposure to Temperature and Humidity
journal, April 2015
- Tamasi, Alison L.; Boland, Kevin S.; Czerwinski, Kenneth
- Analytical Chemistry, Vol. 87, Issue 8
Surface and bulk chemistry of calcined UO2 powders
journal, May 2003
- Nelson, A. J.; Meier, T. C.; Saw, C. K.
- Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 21, Issue 3
XPS photoemission in carbonaceous materials: A “defect” peak beside the graphitic asymmetric peak
journal, January 2004
- Estrade-Szwarckopf, Henriette
- Carbon, Vol. 42, Issue 8-9
XPS spectra of uranyl minerals and synthetic uranyl compounds. I: The U 4f spectrum
journal, May 2009
- Schindler, M.; Hawthorne, F. C.; Freund, M. S.
- Geochimica et Cosmochimica Acta, Vol. 73, Issue 9
Works referencing / citing this record:
Energetics of hydration on uranium oxide and peroxide surfaces
journal, June 2019
- Guo, Xiaofeng; Wu, Di; Ushakov, Sergey V.
- Journal of Materials Research, Vol. 34, Issue 19