Silicate stabilisation of colloidal UO2 produced by uranium metal corrosion

Neill, Thomas S.; Morris, Katherine; Pearce, Carolyn; Abrahamsen-Mills, Liam; Kovarik, Libor; Kellet, Simon; Rigby, Bruce; Vitova, Tonya; Schacherl, Bianca; Shaw, Samuel

doi:10.1016/j.jnucmat.2019.151751

Title: Silicate stabilisation of colloidal UO₂ produced by uranium metal corrosion

Journal Article · 10 August 2019 · Journal of Nuclear Materials

DOI: https://doi.org/10.1016/j.jnucmat.2019.151751 · OSTI ID:1558707

Neill, Thomas S. ^[1]; Morris, Katherine ^[1]; Pearce, Carolyn ^[2]; Abrahamsen-Mills, Liam ^[3]; Kovarik, Libor ^[4]; Kellet, Simon ^[5]; Rigby, Bruce ^[5]; Vitova, Tonya ^[6]; Schacherl, Bianca ^[6]; Shaw, Samuel ^[1]

Univ. of Manchester (United Kingdom)
Univ. of Manchester (United Kingdom); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
National Nuclear Lab. (United Kingdom)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sellafield Ltd. (United Kingdom)
Karlsruhe Inst. of Technology (KIT) (Germany)

U(IV) mobility can be significantly enhanced by colloids in both engineered and natural environments. This is particularly relevant in decommissioning and clean-up of nuclear facilities, such as legacy fuel ponds and silos at the Sellafield site, UK, and in long-term radioactive waste geodisposal. In this study, the product of metallic uranium (U) corrosion under anaerobic, alkaline conditions was characterised, and the interaction of this product with silicate solutions was investigated. The U metal corrosion product consisted of crystalline UO₂ nanoparticles (5-10 nm) that aggregated to form clusters larger than 20 nm. Sequential ultrafiltration indicated that a small fraction of the U metal corrosion product was colloidal. When the uranium corrosion product was reacted with silicate solutions under anaerobic conditions, ultrafiltration indicated a stable colloidal uranium fraction was formed. Extended X-ray absorption fine structure (EXAFS) spectroscopy and high resolution TEM confirmed that the majority of U was still present as UO₂ after several months of exposure to silicate solutions, but an amorphous silica coating was present on the UO₂ surface. This silica coating is believed to be responsible for formation of the UO₂ colloid fraction. Atomic-resolution scanning TEM (STEM) indicated some migration of U into the silica-coating of the UO₂ particles as non-crystalline U(IV)-silicate, suggesting alteration of UO₂ at the UO₂-silica interface had occurred. This alteration at the UO₂-silica interface is a potential pathway to the formation of U-silicates (e.g. coffinite, USiO₄).

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

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1558707

Alternate ID(s):: OSTI ID: 1601823

Report Number(s):: PNNL-SA-146561; TRN: US2103686

Journal Information:: Journal of Nuclear Materials, Vol. 526, Issue C; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 6 works

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Title: Silicate stabilisation of colloidal UO2 produced by uranium metal corrosion

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Title: Silicate stabilisation of colloidal UO₂ produced by uranium metal corrosion