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Title: Component effects on crystallization of RE-containing aluminoborosilicate glass

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Publication Date:
Sponsoring Org.:
OSTI Identifier:
Grant/Contract Number:
AC05-76RL01830; BK21 +
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Journal of Nuclear Materials
Additional Journal Information:
Journal Volume: 478; Journal Issue: C; Related Information: CHORUS Timestamp: 2017-10-04 15:27:13; Journal ID: ISSN 0022-3115
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Citation Formats

Mohd Fadzil, Syazwani, Hrma, Pavel, Schweiger, Michael J., and Riley, Brian J. Component effects on crystallization of RE-containing aluminoborosilicate glass. Netherlands: N. p., 2016. Web. doi:10.1016/j.jnucmat.2016.06.018.
Mohd Fadzil, Syazwani, Hrma, Pavel, Schweiger, Michael J., & Riley, Brian J. Component effects on crystallization of RE-containing aluminoborosilicate glass. Netherlands. doi:10.1016/j.jnucmat.2016.06.018.
Mohd Fadzil, Syazwani, Hrma, Pavel, Schweiger, Michael J., and Riley, Brian J. 2016. "Component effects on crystallization of RE-containing aluminoborosilicate glass". Netherlands. doi:10.1016/j.jnucmat.2016.06.018.
title = {Component effects on crystallization of RE-containing aluminoborosilicate glass},
author = {Mohd Fadzil, Syazwani and Hrma, Pavel and Schweiger, Michael J. and Riley, Brian J.},
abstractNote = {},
doi = {10.1016/j.jnucmat.2016.06.018},
journal = {Journal of Nuclear Materials},
number = C,
volume = 478,
place = {Netherlands},
year = 2016,
month = 9

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1016/j.jnucmat.2016.06.018

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  • Lanthanide-aluminoborosilicate (LABS) glass is one option for immobilizing rare earth (RE) oxide fission products generated during reprocessing of pyroprocessed fuel. This glass system can accommodate a high loading of RE oxides and has excellent chemical durability. The present study describes efforts to model equilibrium crystallinity as a function of glass composition and temperature as well as liquidus temperature (TL) as a function of glass composition. The experimental method for determining TL was ASTM C1720-11. Typically, three crystalline phases were formed in each glass: Ce-borosilicate (Ce 3BSi 2O 10), mullite (Al 10Si 2O 19), and corundum (Al 2O 3). Cerianite (CeOmore » 2) was a common minor crystalline phase and Nd-silicate (Nd 2Si 2O 7) occurred in some of the glasses. In the composition region studied, TL decreased as SiO 2 and B 2O 3 fractions increased and strongly increased with increasing fractions of RE oxides; Al 2O 3 had a moderate effect on the TL but, as expected, it strongly affected the precipitation of Alcontaining crystals.« less
  • This paper presents the structural and crystallization study of a rare-earth-rich aluminoborosilicate glass that is a simplified version of a new nuclear glass proven to be a potential candidate for the immobilization of highly concentrated radioactive wastes that will be produced in the future. In this work, we studied the impact of changing the nature of alkali (Li{sup +}, Na{sup +}, K{sup +}, Rb{sup +}, Cs{sup +}) or alkaline-earth (Mg{sup 2+}, Ca{sup 2+}, Sr{sup 2+}, Ba{sup 2+}) cations present in glass composition on glass structure (by {sup 27}Al and {sup 11}B nuclear magnetic resonance spectroscopy) and on its crystallization tendencymore » during melt cooling at 1 K/min (average cooling rate during industrial process). From these composition changes, it was established that alkali cations were preferentially involved in charge compensation of (AlO{sub 4}){sup -} and (BO{sub 4}){sup -} entities in the glassy network comparatively to alkaline-earth cations. Whatever the nature of alkali cations, glass compositions containing calcium gave way to the crystallization of an apatite silicate phase bearing calcium and rare-earth (RE) cations (Ca{sub 2}RE{sub 8}(SiO{sub 4}){sub 6}O{sub 2}, RE = Nd or La) but melt crystallization tendency during cooling strongly varied with the nature of alkaline-earth cations.« less
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  • No abstract prepared.
  • This study was undertaken to help design mathematical models for high-level waste (HLW) glass melter that simulate spinel behavior in molten glass. Spinel, (Fe,Ni,Mn) (Fe,Cr)2O4, is the primary solid phase that precipitates from HLW glasses containing Fe and Ni in sufficient concentrations. Spinel crystallization affects the anticipated cost and risk of HLW vitrification. To study melting reactions, we used simulated HLW feed, prepared with co-precipitated Fe, Ni, Cr, and Mn hydroxides. Feed samples were heated up at a temperature-increase rate (4C/min) close to that which the feed experiences in the HLW glass melter. The decomposition, melting, and dissolution of feedmore » components (such as nitrates, carbonates, and silica) and the formation of intermediate crystalline phases (spinel, sodalite [Na8(AlSiO4)6(NO2)2], and Zr-containing minerals) were characterized using evolved gas analysis, volume-expansion measurement, optical microscope, scanning electron microscope, thermogravimetric analysis, differential scanning calorimetry, and X-ray diffraction. Nitrates and quartz, the major feed components, converted to a glass-forming melt by 880C. A chromium-free spinel formed in the nitrate melt starting from 520C and Sodalite, a transient product of corundum dissolution, appeared above 600C and eventually dissolved in glass. To investigate the effects of temperature history and minor components (Ru,Ag, and Cu) on the dissolution and growth of spinel crystals, samples were heated up to temperatures above liquidus temperature (TL), then subjected to different temperature histories, and analyzed. The results show that spinel mass fraction, crystals composition, and crystal size depend on the chemical and physical makeup of the feed and temperature history.« less