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

Abstract

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.

Authors:

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

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

^[1]

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

Publication Date:: 2017-10-04

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

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

OSTI Identifier:: 1416493

Alternate Identifier(s):: OSTI ID: 1549268

Report Number(s):: LLNL-JRNL-732898
Journal ID: ISSN 0022-3115; TRN: US1800939

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

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Nuclear Materials

Additional Journal Information:: Journal Volume: 496; Journal Issue: C; Journal ID: ISSN 0022-3115

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY

Citation Formats


                    Donald, Scott B., Davisson, M. Lee, Dai, Zurong, Roberts, Sarah K., and Nelson, Art J. Relative impact of H 2 O and O 2 in the oxidation of UO 2 powders from 50 to 300 °C.  United States: N. p., 2017. 
Web.  doi:10.1016/j.jnucmat.2017.10.014.

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                    Donald, Scott B., Davisson, M. Lee, Dai, Zurong, Roberts, Sarah K., & Nelson, Art J. Relative impact of H 2 O and O 2 in the oxidation of UO 2 powders from 50 to 300 °C.  United States.  https://doi.org/10.1016/j.jnucmat.2017.10.014

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                    Donald, Scott B., Davisson, M. Lee, Dai, Zurong, Roberts, Sarah K., and Nelson, Art J. Wed .  
"Relative impact of H 2 O and O 2 in the oxidation of UO 2 powders from 50 to 300 °C".  United States.  https://doi.org/10.1016/j.jnucmat.2017.10.014.  https://www.osti.gov/servlets/purl/1416493.

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@article{osti_1416493,

  title        = {Relative impact of H 2 O and O 2 in the oxidation of UO 2 powders from 50 to 300 °C},

  author       = {Donald, Scott B. and Davisson, M. Lee and Dai, Zurong and Roberts, Sarah K. and Nelson, Art J.},

  abstractNote = {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.},

  doi          = {10.1016/j.jnucmat.2017.10.014},

  journal      = {Journal of Nuclear Materials},

  number       = C,

  volume       = 496,

  place        = {United States},

  year         = {2017},

  month        = {10}

}

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Similar Records

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

Abstract

Citation Formats

A detailed study of UO2 to U3O8 oxidation phases and the associated rate-limiting steps journal, September 2006

Kinetic Study of the Oxidation of Uranium Dioxide journal, July 1957

A detailed Raman and X-ray study of UO 2+x oxides and related structure transitions journal, January 2016

First-principles calculation and experimental study of oxygen diffusion in uranium dioxide journal, January 2011

Density-functional theory investigation of oxidative corrosion of UO2 journal, May 2012

Stability of oxygen point defects in UO 2 by first-principles DFT + U calculations: Occupation matrix control and Jahn-Teller distortion journal, July 2010

A review of the oxidation of uranium dioxide at temperatures below 400°C journal, April 1998

Corrosion of UO2 and ThO2: A quantum-mechanical investigation journal, April 2008

Crystallization of U3O8 and hydrated UO3 on UO2 fuel in aerated water near 200°C journal, July 1991

The corrosion of uraninite under oxidizing conditions journal, August 1992

An XPS study on the impact of relative humidity on the aging of UO2 powders 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 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 journal, January 1980

Oxidation of spent fuel in air at 175 to 195°C journal, August 1992

Optically Active Lattice Vibrations of α‐Uranium Trioxide journal, March 1962

XPS photoemission in carbonaceous materials: A “defect” peak beside the graphitic asymmetric peak 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 journal, November 2014

Ab Initio Atomistic Thermodynamics of Water Reacting with Uranium Dioxide Surfaces journal, April 2014

Hydroxylation-induced surface stability of AnO2 (An=U, Np, Pu) from first-principles journal, February 2013

The reactions of water vapour on the surfaces of stoichiometric and reduced uranium dioxide: A high resolution XPS study journal, February 2007

Interaction of water vapor with UO2(001) journal, January 2000

Surface Interaction of PuO2, UO2+x and UO3 with Water Ice journal, July 2013

Surface reactions of uranium oxide powder, thin films and single crystals journal, March 2010

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

A detailed study of UO2 to U3O8 oxidation phases and the associated rate-limiting steps
journal, September 2006

Kinetic Study of the Oxidation of Uranium Dioxide
journal, July 1957

A detailed Raman and X-ray study of UO _2+x oxides and related structure transitions
journal, January 2016

First-principles calculation and experimental study of oxygen diffusion in uranium dioxide
journal, January 2011

Density-functional theory investigation of oxidative corrosion of UO2
journal, May 2012

Stability of oxygen point defects in ${UO}_{2}$ by first-principles $DFT + U$ calculations: Occupation matrix control and Jahn-Teller distortion
journal, July 2010

A review of the oxidation of uranium dioxide at temperatures below 400°C
journal, April 1998

Corrosion of UO2 and ThO2: A quantum-mechanical investigation
journal, April 2008

Crystallization of U3O8 and hydrated UO3 on UO2 fuel in aerated water near 200°C
journal, July 1991

The corrosion of uraninite under oxidizing conditions
journal, August 1992

An XPS study on the impact of relative humidity on the aging of UO2 powders
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
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
journal, January 1980

Oxidation of spent fuel in air at 175 to 195°C
journal, August 1992

Optically Active Lattice Vibrations of α‐Uranium Trioxide
journal, March 1962

XPS photoemission in carbonaceous materials: A “defect” peak beside the graphitic asymmetric peak
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
journal, November 2014

Ab Initio Atomistic Thermodynamics of Water Reacting with Uranium Dioxide Surfaces
journal, April 2014

Hydroxylation-induced surface stability of AnO2 (An=U, Np, Pu) from first-principles
journal, February 2013

The reactions of water vapour on the surfaces of stoichiometric and reduced uranium dioxide: A high resolution XPS study
journal, February 2007

Interaction of water vapor with UO2(001)
journal, January 2000

Surface Interaction of PuO2, UO2+x and UO3 with Water Ice
journal, July 2013

Surface reactions of uranium oxide powder, thin films and single crystals
journal, March 2010