Crystallization Study of Rare Earth and Molybdenum Containing Nuclear Waste Glass Ceramics

McCloy, John S.; Riley, Brian J.; Crum, Jarrod; Marcial, José; Reiser, Joelle T.; Kruska, Karen; Peterson, Jacob A.; Neuville, Daniel R.; Patil, Deepak S.; Saleh, Muad; Barnsley, Kristian E.; Hanna, John V.

doi:10.1111/jace.16406

Title: Crystallization Study of Rare Earth and Molybdenum Containing Nuclear Waste Glass Ceramics

Journal Article · 27 February 2019 · Journal of the American Ceramic Society

DOI: https://doi.org/10.1111/jace.16406 · OSTI ID:1497078

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Washington State Univ., Pullman, WA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Washington State Univ., Pullman, WA (United States)
Institut de Physique du Globe de Paris, Paris Cedex (France)
Warwick Univ., Coventry (United Kingdom)

Here, a glass–ceramic waste form is being developed for immobilization of waste streams of alkali (A), alkaline–earth (AE), rare earth (RE), and transition metals generated by transuranic extraction for reprocessing of used nuclear fuel. Benefits over an alkali borosilicate waste form are realized by the partitioning of the fission product fraction insoluble in glass into a suite of chemically durable crystalline phases through controlled cooling, including (AE,A,RE)MoO₄ (powellite) and (RE,A,AE)₁₀Si₆O₂₆ (oxyapatite). In this study, a simplified 8–oxide system (SiO₂–Nd₂O₃–CaO–Na₂O–B₂O₃–Al₂O₃–MoO₃–ZrO₂) was melted, then soaked at various temperatures from 1450 to 1150°C, and subsequently quenched, in order to obtain snapshots into the phase distribution at these temperatures. For these samples, small angle X–ray and neutron scattering, quantitative X–ray diffraction, electron microscopy, ²³Na nuclear magnetic resonance, Nd³⁺ visible absorption, and temperature–dependent viscosity were characterized. In this composition, soak temperatures of ≲ 1250°C were necessary to nucleate calcium molybdate (~10–20 nm in diameter). Further cooling produced oxyapatite and total crystallization increased with lower soak temperatures. Both Na and Nd entered the crystalline phases with lower–temperature soak conditions. Slow cooling or long isothermal treatments at ~975°C produced significantly higher crystal fractions.

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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:: 1497078

Report Number(s):: PNNL-SA--122002

Journal Information:: Journal of the American Ceramic Society, Journal Name: Journal of the American Ceramic Society Journal Issue: 9 Vol. 102; ISSN 0002-7820

Publisher:: American Ceramic SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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