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

Abstract

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.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [2];  [2]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [3];  [5]; ORCiD logo [5]
  1. Washington State Univ., Pullman, WA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  3. Washington State Univ., Pullman, WA (United States)
  4. Institut de Physique du Globe de Paris, Paris Cedex (France)
  5. Warwick Univ., Coventry (United Kingdom)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Washington State Univ., Pullman, WA (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1497078
Alternate Identifier(s):
OSTI ID: 1499073; OSTI ID: 1558457; OSTI ID: 1571521
Report Number(s):
PNNL-SA-122002
Journal ID: ISSN 0002-7820
Grant/Contract Number:  
AC05-76RL01830; NE0008431
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Ceramic Society
Additional Journal Information:
Journal Volume: 102; Journal Issue: 9; Journal ID: ISSN 0002-7820
Publisher:
American Ceramic Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; glass‐ceramics; nuclear magnetic resonance; nuclear waste; rare earths; X‐ray methods

Citation Formats

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., and Hanna, John V. Crystallization Study of Rare Earth and Molybdenum Containing Nuclear Waste Glass Ceramics. United States: N. p., 2019. Web. doi:10.1111/jace.16406.
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. Crystallization Study of Rare Earth and Molybdenum Containing Nuclear Waste Glass Ceramics. United States. doi:10.1111/jace.16406.
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., and Hanna, John V. Wed . "Crystallization Study of Rare Earth and Molybdenum Containing Nuclear Waste Glass Ceramics". United States. doi:10.1111/jace.16406. https://www.osti.gov/servlets/purl/1497078.
@article{osti_1497078,
title = {Crystallization Study of Rare Earth and Molybdenum Containing Nuclear Waste Glass Ceramics},
author = {McCloy, John S. and Riley, Brian J. and Crum, Jarrod and Marcial, José and Reiser, Joelle T. and Kruska, Karen and Peterson, Jacob A. and Neuville, Daniel R. and Patil, Deepak S. and Saleh, Muad and Barnsley, Kristian E. and Hanna, John V.},
abstractNote = {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.},
doi = {10.1111/jace.16406},
journal = {Journal of the American Ceramic Society},
number = 9,
volume = 102,
place = {United States},
year = {2019},
month = {2}
}

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