Characterisation and heat treatment of chloride-contaminated and humidified PuO2 samples

Sutherland-Harper, Sophie; Pearce, Carolyn; Campbell, Catherine; Carrott, Mike; Colledge, Hannah; Gregson, Colin; Hobbs, Jeff; Livens, Francis; Kaltsoyannis, Nikolas; Orr, Robin; Sarsfield, Mark; Sims, Howard; Steele, Helen; Vatter, Ian; Walton, Louise; Webb, Kevin; Taylor, Robin

doi:10.1016/j.jnucmat.2018.07.031

Title: Characterisation and heat treatment of chloride-contaminated and humidified PuO₂ samples

Abstract

To mimic the reactions that have occurred between plutonium dioxide (PuO₂) and degraded polyvinyl chloride during prolonged storage, batches of PuO₂ powders with varying specific surface area (4–38 m² g^–1) were exposed to dry hydrogen chloride gas forming a surface-sorbed exchangeable chloride species that was readily leached by dilute caustic solution. One batch was also humidified under a 95% relative humidity atmosphere. Heat treatment at temperatures between 100 and 950 °C steadily reduced the leachable chloride content at least when the initial leachable chloride surface coverage was calculated to be > 0.5 monolayer (ML). Variations between samples are attributed to differences in surface area as well as production route and period of interim storage in air or humidified atmospheres. The data are consistent with surface species and reactions proposed in the literature for HCl adsorption on to TiO₂. This indicates that it is interactions between hydrogen chloride/chloride and water/hydroxyl species on the PuO₂ surface that are key to understanding the behaviour of these materials when heated in a furnace. Furthermore, these data will inform the design of a future thermal stabilisation process for chloride-contaminated PuO₂.

Authors:

Sutherland-Harper, Sophie ^[1];

^[2]; Campbell, Catherine ^[3]; Carrott, Mike ^[3]; Colledge, Hannah ^[3]; Gregson, Colin ^[3];

^[4]; Livens, Francis ^[1];

^[1]; Orr, Robin ^[3]; Sarsfield, Mark ^[3]; Sims, Howard ^[3]; Steele, Helen ^[4]; Vatter, Ian ^[3]; Walton, Louise ^[3]; Webb, Kevin ^[3];

^[3]

Univ. of Manchester, Manchester (United Kingdom)
Univ. of Manchester, Manchester (United Kingdom); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
National Nuclear Lab., Seascale (United Kingdom)
Sellafield Ltd., Seascale (United Kingdom)

Publication Date:: Tue Jul 17 00:00:00 EDT 2018

Research Org.:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1461644

Grant/Contract Number:: AC05-76RL01830

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Nuclear Materials

Additional Journal Information:: Journal Volume: 509; Journal Issue: C; Journal ID: ISSN 0022-3115

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; Plutonium dioxide; Hydrogen chloride; Thermal treatment; Desorption; Stabilisation

Citation Formats


                    Sutherland-Harper, Sophie, Pearce, Carolyn, Campbell, Catherine, Carrott, Mike, Colledge, Hannah, Gregson, Colin, Hobbs, Jeff, Livens, Francis, Kaltsoyannis, Nikolas, Orr, Robin, Sarsfield, Mark, Sims, Howard, Steele, Helen, Vatter, Ian, Walton, Louise, Webb, Kevin, and Taylor, Robin. Characterisation and heat treatment of chloride-contaminated and humidified PuO2 samples.  United States: N. p., 2018. 
Web.  doi:10.1016/j.jnucmat.2018.07.031.

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                    Sutherland-Harper, Sophie, Pearce, Carolyn, Campbell, Catherine, Carrott, Mike, Colledge, Hannah, Gregson, Colin, Hobbs, Jeff, Livens, Francis, Kaltsoyannis, Nikolas, Orr, Robin, Sarsfield, Mark, Sims, Howard, Steele, Helen, Vatter, Ian, Walton, Louise, Webb, Kevin, & Taylor, Robin. Characterisation and heat treatment of chloride-contaminated and humidified PuO2 samples.  United States.  https://doi.org/10.1016/j.jnucmat.2018.07.031

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                    Sutherland-Harper, Sophie, Pearce, Carolyn, Campbell, Catherine, Carrott, Mike, Colledge, Hannah, Gregson, Colin, Hobbs, Jeff, Livens, Francis, Kaltsoyannis, Nikolas, Orr, Robin, Sarsfield, Mark, Sims, Howard, Steele, Helen, Vatter, Ian, Walton, Louise, Webb, Kevin, and Taylor, Robin. Tue .  
"Characterisation and heat treatment of chloride-contaminated and humidified PuO2 samples".  United States.  https://doi.org/10.1016/j.jnucmat.2018.07.031.  https://www.osti.gov/servlets/purl/1461644.

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@article{osti_1461644,

  title        = {Characterisation and heat treatment of chloride-contaminated and humidified PuO2 samples},

  author       = {Sutherland-Harper, Sophie and Pearce, Carolyn and Campbell, Catherine and Carrott, Mike and Colledge, Hannah and Gregson, Colin and Hobbs, Jeff and Livens, Francis and Kaltsoyannis, Nikolas and Orr, Robin and Sarsfield, Mark and Sims, Howard and Steele, Helen and Vatter, Ian and Walton, Louise and Webb, Kevin and Taylor, Robin},

  abstractNote = {To mimic the reactions that have occurred between plutonium dioxide (PuO2) and degraded polyvinyl chloride during prolonged storage, batches of PuO2 powders with varying specific surface area (4–38 m2 g–1) were exposed to dry hydrogen chloride gas forming a surface-sorbed exchangeable chloride species that was readily leached by dilute caustic solution. One batch was also humidified under a 95% relative humidity atmosphere. Heat treatment at temperatures between 100 and 950 °C steadily reduced the leachable chloride content at least when the initial leachable chloride surface coverage was calculated to be > 0.5 monolayer (ML). Variations between samples are attributed to differences in surface area as well as production route and period of interim storage in air or humidified atmospheres. The data are consistent with surface species and reactions proposed in the literature for HCl adsorption on to TiO2. This indicates that it is interactions between hydrogen chloride/chloride and water/hydroxyl species on the PuO2 surface that are key to understanding the behaviour of these materials when heated in a furnace. Furthermore, these data will inform the design of a future thermal stabilisation process for chloride-contaminated PuO2.},

  doi          = {10.1016/j.jnucmat.2018.07.031},

  journal      = {Journal of Nuclear Materials},

  number       = C,

  volume       = 509,

  place        = {United States},

  year         = {Tue Jul 17 00:00:00 EDT 2018},

  month        = {Tue Jul 17 00:00:00 EDT 2018}

}

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Works referencing / citing this record:

Thermal Processing of Chloride-Contaminated Plutonium Dioxide
journal, July 2019

Webb, Kevin; Taylor, Robin; Campbell, Catherine
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Title: Characterisation and heat treatment of chloride-contaminated and humidified PuO2 samples

Abstract

Citation Formats

A critical examination of the thermodynamics of water adsorption on actinide oxide surfaces journal, October 2003

Thermal desorption study of the surface interactions between water and plutonium dioxide journal, March 1973

Plutonium management policy in the United Kingdom: The need for a dual track strategy journal, February 2017

Infra-red study of hydrogen chloride adsorption on rutile surfaces journal, January 1971

Infrared Study of the Reaction of Hydrogen Chloride with the Surface of γ-Alumina and Its Effect on Surface “Acid” Sites1 journal, May 1966

Infra-red study of the surface properties of rutile. Water and surface hydroxyl species journal, January 1971

Interaction of hydrogen chloride and water with oxide surfaces journal, August 1983

Interaction of gaseous hydrogen chloride and water with oxide surfaces journal, June 1979

Adsorption and desorption of HCl on a single-crystal α-Al2O3(0001) surface journal, April 2000

Surface speciation and interactions between adsorbed chloride and water on cerium dioxide journal, June 2018

Ceria-thoria pellet manufacturing in preparation for plutonia-thoria LWR fuel production journal, October 2016

A XAS study of the local environments of cations in (U, Ce)O2 journal, January 2003

Structure and Bonding Investigation of Plutonium Peroxocarbonate Complexes Using Cerium Surrogates and Electronic Structure Modeling journal, December 2016

Fabrication of size-controlled CeO 2 microparticles by a microfluidic sol–gel process as an analog preparation of ceramic nuclear fuel particles journal, August 2013

Plutonium dioxide particle properties as a function of calcination temperature journal, March 1996

A review of plutonium oxalate decomposition reactions and effects of decomposition temperature on the surface area of the plutonium dioxide product journal, October 2015

A Convenient Way to Generate Hydrogen Chloride in the Freshman Lab journal, December 1995

Raman spectroscopy of plutonium dioxide and related materials journal, August 2012

Preparation and crystal structures of plutonium(IV) hexachloro complexes, Rb2PuCl6 and K2PuCl6 journal, February 1988

Preparation and crystal structures of plutonium(III) pentachloro complexes, K2PuCl5 and Rb2PuCl5 journal, February 1988

Study on the identification of organic and common anions in the pyrohydrolysis distillate of mixed uranium-plutonium carbide for the interference free determination of chlorine and fluorine by ion chromatography journal, January 2014

Pyrohydrolysis in Determination of Fluoride and Other Halides journal, February 1954

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Hydrogen yields from water on the surface of plutonium dioxide journal, June 2013

Oxidizing dissolution of spent MOX47 fuel subjected to water radiolysis: Solution chemistry and surface characterization by Raman spectroscopy journal, April 2010

Raman spectroscopy characterization of actinide oxides (U1−yPuy)O2: Resistance to oxidation by the laser beam and examination of defects journal, October 2010

Raman micro-spectroscopy of UOX and MOX spent nuclear fuel characterization and oxidation resistance of the high burn-up structure journal, March 2015

Raman microspectroscopic studies of unirradiated homogeneous (U0.76Pu0.24)O2+x: the effects of Pu content, non-stoichiometry, self-radiation damage and secondary phases journal, January 2017

Measurement of radiolytic yield of nitric acid in air journal, December 2005

Alterations of thorium oxalate morphology by changing elementary precipitation conditions journal, September 2017

Surface chemistry of Pu oxides journal, July 2004

Solubility and redox reactions of Pu(IV) hydrous oxide: Evidence for the formation of PuO2+x(s, hyd) journal, January 2007

Reaction of Plutonium Dioxide with Water: Formation and Properties of PuO2+x journal, January 2000

Structural investigation of self-irradiation damaged AmO2 journal, April 2014

Restauration thermique du parametre de l'uo2 faiblement irradie journal, February 1961

Annealing of self-radiation damage in 238 puO 2 journal, January 1973

Thermal recovery of self-radiation damage in uraninite and thorianite journal, November 1994

Self-radiation damage in plutonium and uranium mixed dioxide journal, August 2009

Ingrowth of lattice defects in alpha irradiated UO2 single crystals journal, May 1981

Thermal recovery of lattice defects in alpha-irradiated UO2 crystals journal, February 1983

Self-irradiation effects in americium oxides journal, January 1977

The effect of self-radiation on crystal volume journal, January 1977

Self-radiation effects on the lattice parameter of 238PuO2 journal, January 1974

Self-radiation effects on the lattice parameter of 244CmO2 journal, May 1971

Radiation Self-Damage in Plutonium Compounds journal, August 1962

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Multi-scale X-ray diffraction study of strains induced by He implantation in UO2 polycrystals journal, May 2014

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Title: Characterisation and heat treatment of chloride-contaminated and humidified PuO₂ samples

A critical examination of the thermodynamics of water adsorption on actinide oxide surfaces
journal, October 2003

Thermal desorption study of the surface interactions between water and plutonium dioxide
journal, March 1973

Plutonium management policy in the United Kingdom: The need for a dual track strategy
journal, February 2017

Infra-red study of hydrogen chloride adsorption on rutile surfaces
journal, January 1971

Infrared Study of the Reaction of Hydrogen Chloride with the Surface of γ-Alumina and Its Effect on Surface “Acid” Sites¹
journal, May 1966

Infra-red study of the surface properties of rutile. Water and surface hydroxyl species
journal, January 1971

Interaction of hydrogen chloride and water with oxide surfaces
journal, August 1983

Interaction of gaseous hydrogen chloride and water with oxide surfaces
journal, June 1979

Adsorption and desorption of HCl on a single-crystal α-Al2O3(0001) surface
journal, April 2000

Surface speciation and interactions between adsorbed chloride and water on cerium dioxide
journal, June 2018

Ceria-thoria pellet manufacturing in preparation for plutonia-thoria LWR fuel production
journal, October 2016

A XAS study of the local environments of cations in (U, Ce)O2
journal, January 2003

Structure and Bonding Investigation of Plutonium Peroxocarbonate Complexes Using Cerium Surrogates and Electronic Structure Modeling
journal, December 2016

Fabrication of size-controlled CeO ₂ microparticles by a microfluidic sol–gel process as an analog preparation of ceramic nuclear fuel particles
journal, August 2013

Plutonium dioxide particle properties as a function of calcination temperature
journal, March 1996

A review of plutonium oxalate decomposition reactions and effects of decomposition temperature on the surface area of the plutonium dioxide product
journal, October 2015

A Convenient Way to Generate Hydrogen Chloride in the Freshman Lab
journal, December 1995

Raman spectroscopy of plutonium dioxide and related materials
journal, August 2012

Preparation and crystal structures of plutonium(IV) hexachloro complexes, Rb2PuCl6 and K2PuCl6
journal, February 1988

Preparation and crystal structures of plutonium(III) pentachloro complexes, K2PuCl5 and Rb2PuCl5
journal, February 1988

Study on the identification of organic and common anions in the pyrohydrolysis distillate of mixed uranium-plutonium carbide for the interference free determination of chlorine and fluorine by ion chromatography
journal, January 2014

Pyrohydrolysis in Determination of Fluoride and Other Halides
journal, February 1954

Moisture and surface area measurements of plutonium-bearing oxides
journal, December 2009

Adsorption of water on plutonium dioxide
journal, May 1997

Hydrogen yields from water on the surface of plutonium dioxide
journal, June 2013

Oxidizing dissolution of spent MOX47 fuel subjected to water radiolysis: Solution chemistry and surface characterization by Raman spectroscopy
journal, April 2010

Raman spectroscopy characterization of actinide oxides (U1−yPuy)O2: Resistance to oxidation by the laser beam and examination of defects
journal, October 2010

Raman micro-spectroscopy of UOX and MOX spent nuclear fuel characterization and oxidation resistance of the high burn-up structure
journal, March 2015

Raman microspectroscopic studies of unirradiated homogeneous (U_0.76Pu_0.24)O_2+x: the effects of Pu content, non-stoichiometry, self-radiation damage and secondary phases
journal, January 2017

Measurement of radiolytic yield of nitric acid in air
journal, December 2005

Alterations of thorium oxalate morphology by changing elementary precipitation conditions
journal, September 2017

Surface chemistry of Pu oxides
journal, July 2004

Solubility and redox reactions of Pu(IV) hydrous oxide: Evidence for the formation of PuO2+x(s, hyd)
journal, January 2007

Reaction of Plutonium Dioxide with Water: Formation and Properties of PuO2+x
journal, January 2000

Structural investigation of self-irradiation damaged AmO2
journal, April 2014

Restauration thermique du parametre de l'uo2 faiblement irradie
journal, February 1961

Annealing of self-radiation damage in ²³⁸ puO ₂
journal, January 1973

Thermal recovery of self-radiation damage in uraninite and thorianite
journal, November 1994

Self-radiation damage in plutonium and uranium mixed dioxide
journal, August 2009

Ingrowth of lattice defects in alpha irradiated UO2 single crystals
journal, May 1981

Thermal recovery of lattice defects in alpha-irradiated UO2 crystals
journal, February 1983

Self-irradiation effects in americium oxides
journal, January 1977

The effect of self-radiation on crystal volume
journal, January 1977

Self-radiation effects on the lattice parameter of 238PuO2
journal, January 1974

Self-radiation effects on the lattice parameter of 244CmO2
journal, May 1971

Radiation Self-Damage in Plutonium Compounds
journal, August 1962

Self-radiation damage ingrowth in ²³⁸ PuO ₂
journal, January 1973

Alpha-irradiation damage in CeO ₂ , UO ₂ and PuO ₂
journal, January 1984

Multi-scale X-ray diffraction study of strains induced by He implantation in UO2 polycrystals
journal, May 2014

Thermal Processing of Chloride-Contaminated Plutonium Dioxide
journal, July 2019