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Title: Crystallization behavior of iron- and boron-containing nepheline (Na 2O·Al 2O 3·2SiO 2) based model high-level nuclear waste glasses

Abstract

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 Na 2O–Al 2O 3–B 2O 3–Fe 2O 3–SiO 2 system with varying Al 2O 3/Fe 2O 3 and Na 2O/Fe 2O 3 ratios have been synthesized by melt-quench technique and studied for their crystallization behavior in different heating atmospheres—air, inert (N 2), and reducing (96%N 2–4%H 2). 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 N 2 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 Al 2O 3/Fe 2O 3 ratio, it wasmore » absent from glass-ceramics with varying Na 2O/Fe 2O 3 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.« less

Authors:
 [1]; ORCiD logo [2];  [3];  [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [2]; ORCiD logo [1]
  1. Rutgers Univ., Piscataway, NJ (United States). Dept. of Materials Science and Engineering
  2. Washington State Univ., Pullman, WA (United States). School of Mechanical & Materials Engineering. Materials Science & Engineering Program
  3. Sheffield Hallam Univ., Sheffield (United Kingdom). Materials and Engineering Research Inst.
  4. Idaho National Lab. (INL), Idaho Falls, ID (United States). Materials Science and Engineering Dept.
Publication Date:
Research Org.:
Idaho National Lab. (INL), Idaho Falls, ID (United States); Rutgers Univ., Piscataway, NJ (United States); Washington State Univ., Pullman, WA (United States)
Sponsoring Org.:
USDOE Office of Environmental Management (EM); USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1484678
Alternate Identifier(s):
OSTI ID: 1462595
Report Number(s):
INL/JOU-18-45891-Rev000
Journal ID: ISSN 0002-7820
Grant/Contract Number:  
AC07-05ID14517; EM0003207; EM0002904; NE0008597
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Ceramic Society
Additional Journal Information:
Journal Volume: 102; Journal Issue: 3; Journal ID: ISSN 0002-7820
Publisher:
American Ceramic Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Deshkar, Ambar, Ahmadzadeh, Mostafa, Scrimshire, Alex, Han, Edmund, Bingham, Paul A., Guillen, Donna, McCloy, John, and Goel, Ashutosh. Crystallization behavior of iron- and boron-containing nepheline (Na2O·Al2O3·2SiO2) based model high-level nuclear waste glasses. United States: N. p., 2018. Web. doi:10.1111/jace.15936.
Deshkar, Ambar, Ahmadzadeh, Mostafa, Scrimshire, Alex, Han, Edmund, Bingham, Paul A., Guillen, Donna, McCloy, John, & Goel, Ashutosh. Crystallization behavior of iron- and boron-containing nepheline (Na2O·Al2O3·2SiO2) based model high-level nuclear waste glasses. United States. doi:10.1111/jace.15936.
Deshkar, Ambar, Ahmadzadeh, Mostafa, Scrimshire, Alex, Han, Edmund, Bingham, Paul A., Guillen, Donna, McCloy, John, and Goel, Ashutosh. Fri . "Crystallization behavior of iron- and boron-containing nepheline (Na2O·Al2O3·2SiO2) based model high-level nuclear waste glasses". United States. doi:10.1111/jace.15936.
@article{osti_1484678,
title = {Crystallization behavior of iron- and boron-containing nepheline (Na2O·Al2O3·2SiO2) based model high-level nuclear waste glasses},
author = {Deshkar, Ambar and Ahmadzadeh, Mostafa and Scrimshire, Alex and Han, Edmund and Bingham, Paul A. and Guillen, Donna and McCloy, John and Goel, Ashutosh},
abstractNote = {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.},
doi = {10.1111/jace.15936},
journal = {Journal of the American Ceramic Society},
number = 3,
volume = 102,
place = {United States},
year = {2018},
month = {7}
}

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Works referenced in this record:

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976