Impact of non‐framework cation mixing on the structure and crystallization behavior of model high‐level waste glasses

Balasubramanya, Nikhila; Sun, Zhenxuan; Ahmadzadeh, Mostafa; Kamali, Saeed; Neuville, Daniel R.; McCloy, John S.; Goel, Ashutosh

doi:10.1111/jace.18381

Title: Impact of non‐framework cation mixing on the structure and crystallization behavior of model high‐level waste glasses

Journal Article · 13 February 2022 · Journal of the American Ceramic Society

DOI: https://doi.org/10.1111/jace.18381 · OSTI ID:1845064

Balasubramanya, Nikhila ^[1]; Sun, Zhenxuan ^[1]; Ahmadzadeh, Mostafa ^[2]; Kamali, Saeed ^[3];

^[4];

^[2];

^[1]

Department of Materials Science and Engineering Rutgers, The State University of New Jersey Piscataway New Jersey 08854 USA
School of Mechanical and Materials Engineering and Materials Science and Engineering Program Washington State University Pullman Washington USA
Mechanical Aerospace and Biomedical Engineering Department University of Tennessee Space Institute Tullahoma Tennessee USA, Department of Physics and Astronomy Middle Tennessee State University Murfreesboro Tennessee USA
CNRS‐Géomatériaux Institut de Physique du Globe de Paris Sorbonne Paris Cité, 1 rue Jussieu Paris France

Abstract Spinel crystallization is known to be detrimental to the operation of Joule heated ceramic melters during the vitrification of iron‐rich high‐level nuclear wastes (HLW) into borosilicate glasses. The literature on this subject focuses on tackling the problem by developing empirical constraints to design compositions, which limit the fraction of spinels formed in the melter or by developing empirical models to predict the settling behavior of spinels in the melter as a function of the glass composition. While these empirical models can predict the behavior of most of the compositions, they are not failsafe as there are always some compositions, whose behavior is beyond the predictive ability of these models. This can lead to undesirable situations during the vitrification of the nuclear waste, and therefore an in‐depth investigation of the chemo‐structural descriptors controlling the crystallization behavior in these glasses is warranted. Accordingly, the present study aims to understand the impact of non‐framework cation mixing (i.e., Li ⁺ /Na ⁺ and Ca ²⁺ /Na ⁺ ) on the structure (through Raman spectroscopy and Mössbauer spectroscopy) and crystallization behavior (through XRD, SEM‐EDS, and vibrating sample magnetometry) of iron‐rich model HLW glasses in the system: (mol.%) x M _y O–(25− x ) Na ₂ O–9.12 B ₂ O ₃ –6.4 Al ₂ O ₃ –51.25 SiO ₂ –7.22 Fe ₂ O ₃ –0.38 MnO–0.08 Cr ₂ O ₃ –0.55NiO (M _y O = Li ₂ O or CaO).

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NE0008597

OSTI ID:: 1845064

Journal Information:: Journal of the American Ceramic Society, Journal Name: Journal of the American Ceramic Society Journal Issue: 6 Vol. 105; ISSN 0002-7820

Publisher:: Wiley-BlackwellCopyright Statement

Country of Publication:: United States

Language:: English

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