Relative impact of H 2 O and O 2 in the oxidation of UO 2 powders from 50 to 300 °C

Donald, Scott B.; Davisson, M. Lee; Dai, Zurong; Roberts, Sarah K.; Nelson, Art J.

doi:10.1016/j.jnucmat.2017.10.014

Title: Relative impact of H ₂ O and O ₂ in the oxidation of UO ₂ powders from 50 to 300 °C

Journal Article · 04 October 2017 · Journal of Nuclear Materials

DOI: https://doi.org/10.1016/j.jnucmat.2017.10.014 · OSTI ID:1416493

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

^[1]; Roberts, Sarah K. ^[1];

^[1]

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

Here, we studied the reaction of water and molecular oxygen with stoichiometric uranium dioxide (i.e. UO₂) powder at elevated temperature by high-resolution x-ray photoelectron spectroscopy (XPS), infrared (IR) spectroscopy, powder x-ray diffraction (XRD), and scanning electron microscopy (SEM). We observed and quatified oxidation resulting from the dissociative chemisorption of the adsorbing molecules and subsequent incorporation into the oxide lattice. Molecular oxygen was found to be a stronger oxidation agent than water at elevated temperatures but not at ambient.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

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

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation

Grant/Contract Number:: AC52-07NA27344; LL15-U_Surface_Oxidation-NDD3B

OSTI ID:: 1416493

Alternate ID(s):: OSTI ID: 1549268

Report Number(s):: LLNL-JRNL-732898; TRN: US1800939

Journal Information:: Journal of Nuclear Materials, Vol. 496, Issue C; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 7 works

Citation information provided by
Web of Science

References (30)

Specific outcomes of the research on the spent fuel long-term evolution in interim dry storage and deep geological disposal Ferry, C.; Poinssot, C.; Cappelaere, C. Journal of Nuclear Materials, Vol. 352, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2006.02.061	journal	June 2006
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
Kinetic Study of the Oxidation of Uranium Dioxide Aronson, S.; Roof, R. B.; Belle, J. The Journal of Chemical Physics, Vol. 27, Issue 1 https://doi.org/10.1063/1.1743653	journal	July 1957
A detailed Raman and X-ray study of UO _2+x oxides and related structure transitions Elorrieta, J. M.; Bonales, L. J.; Rodríguez-Villagra, N. Physical Chemistry Chemical Physics, Vol. 18, Issue 40 https://doi.org/10.1039/C6CP03800J	journal	January 2016
First-principles calculation and experimental study of oxygen diffusion in uranium dioxide Dorado, Boris; Garcia, Philippe; Carlot, Gaëlle Physical Review B, Vol. 83, Issue 3 https://doi.org/10.1103/PhysRevB.83.035126	journal	January 2011
Density-functional theory investigation of oxidative corrosion of UO2 Chaka, Anne M.; Oxford, Gloria A. E.; Stubbs, Joanne E. Computational and Theoretical Chemistry, Vol. 987 https://doi.org/10.1016/j.comptc.2011.11.028	journal	May 2012
Stability of oxygen point defects in UO 2 by first-principles DFT + U calculations: Occupation matrix control and Jahn-Teller distortion Dorado, Boris; Jomard, Gérald; Freyss, Michel Physical Review B, Vol. 82, Issue 3 https://doi.org/10.1103/PhysRevB.82.035114	journal	July 2010
Biogenic nanoparticulate UO2: Synthesis, characterization, and factors affecting surface reactivity Singer, David M.; Farges, François; Brown, Gordon E. Geochimica et Cosmochimica Acta, Vol. 73, Issue 12 https://doi.org/10.1016/j.gca.2009.03.031	journal	June 2009
Corrosion of UO2 and ThO2: A quantum-mechanical investigation Skomurski, F. N.; Shuller, L. C.; Ewing, R. C. Journal of Nuclear Materials, Vol. 375, Issue 3 https://doi.org/10.1016/j.jnucmat.2007.12.007	journal	April 2008
Crystallization of U3O8 and hydrated UO3 on UO2 fuel in aerated water near 200°C Taylor, Peter; Wood, Donald D.; Owen, Derrek G. Journal of Nuclear Materials, Vol. 183, Issue 1-2 https://doi.org/10.1016/0022-3115(91)90477-O	journal	July 1991
The corrosion of uraninite under oxidizing conditions Finch, Robert J.; Ewing, Rodney C. Journal of Nuclear Materials, Vol. 190 https://doi.org/10.1016/0022-3115(92)90083-W	journal	August 1992
An XPS study on the impact of relative humidity on the aging of UO2 powders Donald, Scott B.; Dai, Zurong R.; Davisson, M. Lee Journal of Nuclear Materials, Vol. 487 https://doi.org/10.1016/j.jnucmat.2017.02.016	journal	April 2017
Oxidation of UO2 fuel pellets in air at 503 and 543 K studied using X-ray photoelectron spectroscopy and X-ray diffraction Tempest, P. A.; Tucker, P. M.; Tyler, J. W. Journal of Nuclear Materials, Vol. 151, Issue 3 https://doi.org/10.1016/0022-3115(88)90019-0	journal	February 1988
An X-ray diffraction study of the formation of β-UO2.33 on UO2 pellet surfaces in air at 229 to 275°C Taylor, Peter; Burgess, Elizabeth A.; Owen, Derrek G. Journal of Nuclear Materials, Vol. 88, Issue 1 https://doi.org/10.1016/0022-3115(80)90395-5	journal	January 1980
Oxidation of spent fuel in air at 175 to 195°C Einziger, R. E.; Thomas, L. E.; Buchanan, H. C. Journal of Nuclear Materials, Vol. 190 https://doi.org/10.1016/0022-3115(92)90075-V	journal	August 1992
Infrared spectroscopy of the uranium/oxygen system Allen, G. C.; Crofts, J. A.; Griffiths, A. J. Journal of Nuclear Materials, Vol. 62, Issue 2-3 https://doi.org/10.1016/0022-3115(76)90024-6	journal	November 1976
Optically Active Lattice Vibrations of α‐Uranium Trioxide Tsuboi, Masamichi; Terada, Minoru; Shimanouchi, Takehiko The Journal of Chemical Physics, Vol. 36, Issue 5 https://doi.org/10.1063/1.1732732	journal	March 1962
Uranium-oxygen lattice vibrations of triuranium octoxide Ohwada, Ken; Soga, Takeshi Spectrochimica Acta Part A: Molecular Spectroscopy, Vol. 29, Issue 5 https://doi.org/10.1016/0584-8539(73)80055-8	journal	May 1973
The electronic structure of actinide dioxides Goodman, G. L. Journal of Alloys and Compounds, Vol. 181, Issue 1-2 https://doi.org/10.1016/0925-8388(92)90295-K	journal	April 1992
Oxidation of uranium dioxide at 298 K studied by using x-ray photoelectron spectroscopy Allen, G. C.; Tucker, P. M.; Tyler, J. W. The Journal of Physical Chemistry, Vol. 86, Issue 2 https://doi.org/10.1021/j100391a018	journal	January 1982
A study of synthetic and natural uranium oxides by X-ray photoelectron spectroscopy Teterin, Yu. A.; Kulakov, V. M.; Baev, A. S. Physics and Chemistry of Minerals, Vol. 7, Issue 4 https://doi.org/10.1007/BF00307259	journal	September 1981
XPS photoemission in carbonaceous materials: A “defect” peak beside the graphitic asymmetric peak Estrade-Szwarckopf, Henriette Carbon, Vol. 42, Issue 8-9 https://doi.org/10.1016/j.carbon.2004.03.005	journal	January 2004
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
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
Hydroxylation-induced surface stability of AnO2 (An=U, Np, Pu) from first-principles Rák, Zs.; Ewing, R. C.; Becker, U. Surface Science, Vol. 608 https://doi.org/10.1016/j.susc.2012.10.002	journal	February 2013
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
Interaction of water vapor with UO2(001) Hedhili, M. N.; Yakshinskiy, B. V.; Madey, T. E. Surface Science, Vol. 445, Issue 2-3 https://doi.org/10.1016/S0039-6028(99)01117-6	journal	January 2000
Quasiepitaxial growth of a monoclinic phase on UO 2 single crystals upon leaching in H 2 O Nowicki, L.; Turos, A.; Choffel, C. Physical Review B, Vol. 56, Issue 2 https://doi.org/10.1103/PhysRevB.56.534	journal	July 1997
Surface Interaction of PuO2, UO2+x and UO3 with Water Ice Gouder, T.; Shick, A. B.; Huber, F. Topics in Catalysis, Vol. 56, Issue 12 https://doi.org/10.1007/s11244-013-0077-3	journal	July 2013
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

Similar Records

Submicrometer spectromicroscopy of UO₂ aged under high humidity conditions

Journal Article · 2022 · Journal of Vacuum Science and Technology A · OSTI ID:1871781

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

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

Journal Article · 2017 · Journal of Nuclear Materials · OSTI ID:1347674

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

Synthesis and characterization of nanometric powders of UO{sub 2+x}, (Th,U)O{sub 2+x} and (La,U)O{sub 2+x}

Journal Article · 2009 · Journal of Solid State Chemistry · OSTI ID:21372319

Rousseau, G; Fattahi, M; Grambow, B; +5 more

Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY

Title: Relative impact of H 2 O and O 2 in the oxidation of UO 2 powders from 50 to 300 °C

Citation Formats

References (30)

Similar Records

Related Subjects

Title: Relative impact of H ₂ O and O ₂ in the oxidation of UO ₂ powders from 50 to 300 °C