XPS Investigation on Changes in UO2 Speciation following Exposure to Humidity

Donald, Scott B.; Davisson, M. Lee; Nelson, Art J.

doi:10.1557/adv.2016.286

Title: XPS Investigation on Changes in UO₂ Speciation following Exposure to Humidity

Journal Article · Wed Apr 27 00:00:00 EDT 2016 · MRS Advances

DOI:https://doi.org/10.1557/adv.2016.286· OSTI ID:1247285

Donald, Scott B. ^[1]; Davisson, M. Lee ^[1]; Nelson, Art J. ^[1]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

High purity UO₂powder samples were subjected to accelerated aging under controlled conditions with relative humidity ranging from 34% to 98%. Characterization of the chemical speciation of the products was accomplished using X-ray photoelectron spectroscopy (XPS). A shift to higher uranium oxidation states was found to be directly correlated to increased relative humidity exposure. In addition, the relative abundance of O^2-, OH^-, and H₂O was found to vary with exposure time. Therefore, it is expected that uranium oxide materials exposed to high relative humidity conditions during processing and storage would display a similar increase in average uranium valence.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1247285

Report Number(s):: LLNL-CONF-685861; applab; PII: S2059852116002863

Journal Information:: MRS Advances, Vol. 1, Issue 44; Conference: Presented at: 2016 MRS Spring Meeting & Exhibit, Phoenix, AZ, United States, Mar 28 - Apr 01, 2016; ISSN 2059-8521

Publisher:: Materials Research Society (MRS)Copyright Statement

Country of Publication:: United States

Language:: English

References (14)

XPS spectra of uranyl minerals and synthetic uranyl compounds. II: The O 1s spectrum Schindler, M.; Hawthorne, F. C.; Freund, M. S. Geochimica et Cosmochimica Acta, Vol. 73, Issue 9 https://doi.org/10.1016/j.gca.2008.10.041	journal	May 2009
Adsorption of water on UO2 (111) surface: Density functional theory calculations Tian, Xiao-feng; Wang, Hui; Xiao, Hong-xing Computational Materials Science, Vol. 91 https://doi.org/10.1016/j.commatsci.2014.05.009	journal	August 2014
On the role of strong electron correlations in the surface properties and chemistry of uranium dioxide Weck, Philippe F.; Kim, Eunja; Jové-Colón, Carlos F. Dalton Transactions, Vol. 42, Issue 13 https://doi.org/10.1039/c3dt32536a	journal	January 2013
Actinide Dioxides in Water: Interactions at the Interface Alexandrov, Vitaly; Shvareva, Tatiana Y.; Hayun, Shmuel The Journal of Physical Chemistry Letters, Vol. 2, Issue 24 https://doi.org/10.1021/jz201458x	journal	November 2011
Neutron Diffraction Study of the in Situ Oxidation of UO ₂ Desgranges, Lionel; Baldinozzi, Gianguido; Rousseau, Gurvan Inorganic Chemistry, Vol. 48, Issue 16 https://doi.org/10.1021/ic9000889	journal	August 2009
A detailed study of UO2 to U3O8 oxidation phases and the associated rate-limiting steps Rousseau, G.; Desgranges, L.; Charlot, F. Journal of Nuclear Materials, Vol. 355, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2006.03.015	journal	September 2006
First-principles study of water adsorption and dissociation on the UO2 (1 1 1), (1 1 0) and (1 0 0) surfaces Bo, Tao; Lan, Jian-Hui; Zhao, Yao-Lin Journal of Nuclear Materials, Vol. 454, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.09.001	journal	November 2014
A review of the oxidation of uranium dioxide at temperatures below 400°C McEachern, R. J.; Taylor, P. Journal of Nuclear Materials, Vol. 254, Issue 2-3 https://doi.org/10.1016/S0022-3115(97)00343-7	journal	April 1998
Ab Initio Atomistic Thermodynamics of Water Reacting with Uranium Dioxide Surfaces Maldonado, P.; Evins, L. Z.; Oppeneer, P. M. The Journal of Physical Chemistry C, Vol. 118, Issue 16 https://doi.org/10.1021/jp501715m	journal	April 2014
Surface reactions of uranium oxide powder, thin films and single crystals Idriss, H. Surface Science Reports, Vol. 65, Issue 3 https://doi.org/10.1016/j.surfrep.2010.01.001	journal	March 2010
The reactions of water vapour on the surfaces of stoichiometric and reduced uranium dioxide: A high resolution XPS study Senanayake, S. D.; Waterhouse, G. I. N.; Chan, A. S. Y. Catalysis Today, Vol. 120, Issue 2 https://doi.org/10.1016/j.cattod.2006.07.040	journal	February 2007
XPS determination of uranium oxidation states: XPS determination of uranium oxidation states Ilton, Eugene S.; Bagus, Paul S. Surface and Interface Analysis, Vol. 43, Issue 13 https://doi.org/10.1002/sia.3836	journal	October 2011
Theoretical Studies of Hydrogen and Water Adsorption on Actinide Oxide Surfaces Hay, P. Jeffrey MRS Proceedings, Vol. 893 https://doi.org/10.1557/PROC-0893-JJ08-04	journal	January 2005
Measurement of the Auger parameter and Wagner plot for uranium compounds Holliday, Kiel S.; Siekhaus, Wigbert; Nelson, Art J. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 31, Issue 3 https://doi.org/10.1116/1.4793477	journal	May 2013

Similar Records

An XPS study on the impact of relative humidity on the aging of UO₂ powders

Journal Article · Fri Feb 10 00:00:00 EST 2017 · Journal of Nuclear Materials · OSTI ID:1247285

Donald, Scott B.; Dai, Zurong R.; Davisson, M. Lee; +2 more

Hydration of α-UO₃ following storage under controlled conditions of temperature and relative humidity

Journal Article · Mon Jul 20 00:00:00 EDT 2020 · Dalton Transactions · OSTI ID:1247285

Wilkerson, Marianne P.; Hernandez, Sarah C.; Mullen, W. Tyler; +7 more

Submicrometer spectromicroscopy of UO₂ aged under high humidity conditions

Journal Article · Mon May 16 00:00:00 EDT 2022 · Journal of Vacuum Science and Technology A · OSTI ID:1247285

Ditter, Alex S.; Pacold, Joseph I.; Dai, Zurong; +5 more

Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
actinide
x-ray photoelectron spectroscopy (XPS)
surface chemistry

Title: XPS Investigation on Changes in UO2 Speciation following Exposure to Humidity

Citation Formats

References (14)

Similar Records

Related Subjects

Title: XPS Investigation on Changes in UO₂ Speciation following Exposure to Humidity