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

Journal Article · 17 July 2018 · Journal of Nuclear Materials

DOI: https://doi.org/10.1016/j.jnucmat.2018.07.031 · OSTI ID:1461644

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)

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.

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

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1461644

Journal Information:: Journal of Nuclear Materials, Vol. 509, Issue C; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 8 works

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