Crystallization behavior of iron- and boron-containing nepheline (Na2O·Al2O3·2SiO2) based model high-level nuclear waste glasses

Deshkar, Ambar; Ahmadzadeh, Mostafa; Scrimshire, Alex; Han, Edmund; Bingham, Paul A.; Guillen, Donna; McCloy, John; Goel, Ashutosh

doi:10.1111/jace.15936

Title: Crystallization behavior of iron- and boron-containing nepheline (Na₂O·Al₂O₃·2SiO₂) based model high-level nuclear waste glasses

Journal Article · 13 July 2018 · Journal of the American Ceramic Society

DOI: https://doi.org/10.1111/jace.15936 · OSTI ID:1484678

Deshkar, Ambar ^[1];

^[2]; Scrimshire, Alex ^[3]; Han, Edmund ^[1];

^[3];

^[4];

^[2];

^[1]

Rutgers Univ., Piscataway, NJ (United States). Dept. of Materials Science and Engineering
Washington State Univ., Pullman, WA (United States). School of Mechanical & Materials Engineering. Materials Science & Engineering Program
Sheffield Hallam Univ., Sheffield (United Kingdom). Materials and Engineering Research Inst.
Idaho National Lab. (INL), Idaho Falls, ID (United States). Materials Science and Engineering Dept.

This work focuses on understanding the relationship between iron redox, composition, and heat-treatment atmosphere in nepheline-based model high-level nuclear waste glasses. Glasses in the Na₂O–Al₂O₃–B₂O₃–Fe₂O₃–SiO₂ system with varying Al₂O₃/Fe₂O₃ and Na₂O/Fe₂O₃ ratios have been synthesized by melt-quench technique and studied for their crystallization behavior in different heating atmospheres—air, inert (N₂), and reducing (96%N₂–4%H₂). The compositional dependence of iron redox chemistry in glasses and the impact of heating environment and crystallization on iron coordination in glass-ceramics have been investigated by Mössbauer spectroscopy and vibrating sample magnetometry. While iron coordination in glasses and glass-ceramics changed as a function of glass chemistry, the heating atmosphere during crystallization exhibited minimal effect on iron redox. The change in heating atmosphere did not affect the phase assemblage but did affect the microstructural evolution. While glass-ceramics produced as a result of heat treatment in air and N₂ atmospheres developed a golden/brown colored iron-rich layer on their surface, those produced in a reducing atmosphere did not exhibit any such phenomenon. Furthermore, while this iron-rich layer was observed in glass-ceramics with varying Al₂O₃/Fe₂O₃ ratio, it was absent from glass-ceramics with varying Na₂O/Fe₂O₃ ratio. An explanation of these results has been provided on the basis of kinetics of diffusion of oxygen and network modifiers in the glasses under different thermodynamic conditions. Finally, the plausible implications of the formation of iron-rich layer on the surface of glass-ceramics on the chemical durability of high-level nuclear waste glasses have been discussed.

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Research Organization:: Idaho National Lab. (INL), Idaho Falls, ID (United States); Rutgers Univ., Piscataway, NJ (United States); Washington State Univ., Pullman, WA (United States)

Sponsoring Organization:: USDOE Office of Environmental Management (EM); USDOE Office of Nuclear Energy (NE), Nuclear Energy University Program (NEUP)

Grant/Contract Number:: AC07-05ID14517; EM0003207; EM0002904; NE0008597

OSTI ID:: 1484678

Report Number(s):: INL/JOU--18-45891-Rev000

Journal Information:: Journal of the American Ceramic Society, Journal Name: Journal of the American Ceramic Society Journal Issue: 3 Vol. 102; ISSN 0002-7820

Publisher:: American Ceramic SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Crystallization behavior of iron- and boron-containing nepheline (Na₂O·Al₂O₃·2SiO₂) based model high-level nuclear waste glasses