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Title: The formation of crystals in glasses containing rare earth oxides

Abstract

Korean spent nuclear fuel will reach the capacity of the available temporary storage by 2016. Pyroprocessing and direct disposal seems to be an alternative way to manage and reuse spent nuclear fuel while avoiding the wet reprocessing technology. Pyroprocessing produces several wastes streams, including metals, salts, and rare earths, which must be converted into stabilized form. A suitable form for rare earth immobilization is borosilicate glass. The borosilicate glass form exhibits excellent durability, allows a high waste loading, and is easy to process. In this work, we combined the rare earths waste of composition (in wt%) 39.2Nd{sub 2}O{sub 3}–22.7CeO{sub 2}–11.7La{sub 2}O{sub 3}–10.9PrO{sub 2}–1.3Eu{sub 2}O{sub 3}–1.3Gd{sub 2}O{sub 3}–8.1Sm{sub 2}O{sub 3}–4.8Y{sub 2}O{sub 3} with a baseline glass of composition 60.2SiO{sub 2}–16.0B{sub 2}O{sub 3}–12.6Na{sub 2}O–3.8Al{sub 2}O{sub 3}–5.7CaO–1.7ZrO{sub 2}. Crystallization in waste glasses occurs as the waste loading increases. It may produce complicate glass processing and affect the product quality. To study crystal formation, we initially made glasses containing 5%, 10% and 15% of La{sub 2}O{sub 3} and then glasses with 5%, 10% and 15% of the complete rare earth mix. Samples were heat-treated for 24 hours at temperatures 800°C to 1150°C in 50°C increments. Quenched samples were analyzed using an optical microscope, scanningmore » electron microscope with energy dispersive spectroscopy, and x-ray diffraction. Stillwellite (LaBSiO{sub 5}) and oxyapatite (Ca{sub 2}La{sub 8}Si{sub 6}O{sub 26}) were found in glasses containing La{sub 2}O{sub 3}, while oxyapatite (Ca{sub 2}La{sub 8}Si{sub 6}O{sub 26} and NaNd{sub 9}Si{sub 6}O{sub 26}) precipitated in glasses with additions of mixed rare earths. The liquidus temperature (T{sub L}) of the glasses containing 5%, 10% and 15% La{sub 2}O{sub 3} were 800°C, 959°C and 986°C, respectively; while T{sub L} was 825°C, 1059°C and 1267°C for glasses with 5%, 10% and 15% addition of mixed rare earth oxides. The component coefficients T{sub B2O3}, T{sub SiO2}, T{sub CaO}, and T{sub RE2O3} were also evaluated using a recently published study.« less

Authors:
 [1];  [2];  [3]; ; ;  [4]
  1. Pohang University of Science and Technology (POSTECH), Pohang (Korea, Republic of)
  2. Pohang University of Science and Technology (POSTECH), Pohang, South Korea and Pacific Northwest National Laboratory, Richland, Washington (United States)
  3. Pacific Northwest National Laboratory, Richland, Washington (United States)
  4. National University of Malaysia, Bandar Baru Bangi, Selangor (Malaysia)
Publication Date:
OSTI Identifier:
22266070
Resource Type:
Journal Article
Journal Name:
AIP Conference Proceedings
Additional Journal Information:
Journal Volume: 1584; Journal Issue: 1; Conference: iNuSTEC2013: International nuclear science, technology and engineering conference 2013, Kuala Lumpur (Malaysia), 30 Sep - 2 Oct 2013; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0094-243X
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; BOROSILICATE GLASS; CRYSTALLIZATION; CRYSTALS; LANTHANUM OXIDES; OPTICAL MICROSCOPES; RARE EARTHS; SCANNING ELECTRON MICROSCOPY; SPECTROSCOPY; SPENT FUELS; X-RAY DIFFRACTION

Citation Formats

Fadzil, Syazwani Mohd, Hrma, Pavel, Crum, Jarrod, Siong, Khoo Kok, Ngatiman, Mohammad Fadzlee, and Said, Riduan Mt. The formation of crystals in glasses containing rare earth oxides. United States: N. p., 2014. Web. doi:10.1063/1.4866127.
Fadzil, Syazwani Mohd, Hrma, Pavel, Crum, Jarrod, Siong, Khoo Kok, Ngatiman, Mohammad Fadzlee, & Said, Riduan Mt. The formation of crystals in glasses containing rare earth oxides. United States. https://doi.org/10.1063/1.4866127
Fadzil, Syazwani Mohd, Hrma, Pavel, Crum, Jarrod, Siong, Khoo Kok, Ngatiman, Mohammad Fadzlee, and Said, Riduan Mt. 2014. "The formation of crystals in glasses containing rare earth oxides". United States. https://doi.org/10.1063/1.4866127.
@article{osti_22266070,
title = {The formation of crystals in glasses containing rare earth oxides},
author = {Fadzil, Syazwani Mohd and Hrma, Pavel and Crum, Jarrod and Siong, Khoo Kok and Ngatiman, Mohammad Fadzlee and Said, Riduan Mt},
abstractNote = {Korean spent nuclear fuel will reach the capacity of the available temporary storage by 2016. Pyroprocessing and direct disposal seems to be an alternative way to manage and reuse spent nuclear fuel while avoiding the wet reprocessing technology. Pyroprocessing produces several wastes streams, including metals, salts, and rare earths, which must be converted into stabilized form. A suitable form for rare earth immobilization is borosilicate glass. The borosilicate glass form exhibits excellent durability, allows a high waste loading, and is easy to process. In this work, we combined the rare earths waste of composition (in wt%) 39.2Nd{sub 2}O{sub 3}–22.7CeO{sub 2}–11.7La{sub 2}O{sub 3}–10.9PrO{sub 2}–1.3Eu{sub 2}O{sub 3}–1.3Gd{sub 2}O{sub 3}–8.1Sm{sub 2}O{sub 3}–4.8Y{sub 2}O{sub 3} with a baseline glass of composition 60.2SiO{sub 2}–16.0B{sub 2}O{sub 3}–12.6Na{sub 2}O–3.8Al{sub 2}O{sub 3}–5.7CaO–1.7ZrO{sub 2}. Crystallization in waste glasses occurs as the waste loading increases. It may produce complicate glass processing and affect the product quality. To study crystal formation, we initially made glasses containing 5%, 10% and 15% of La{sub 2}O{sub 3} and then glasses with 5%, 10% and 15% of the complete rare earth mix. Samples were heat-treated for 24 hours at temperatures 800°C to 1150°C in 50°C increments. Quenched samples were analyzed using an optical microscope, scanning electron microscope with energy dispersive spectroscopy, and x-ray diffraction. Stillwellite (LaBSiO{sub 5}) and oxyapatite (Ca{sub 2}La{sub 8}Si{sub 6}O{sub 26}) were found in glasses containing La{sub 2}O{sub 3}, while oxyapatite (Ca{sub 2}La{sub 8}Si{sub 6}O{sub 26} and NaNd{sub 9}Si{sub 6}O{sub 26}) precipitated in glasses with additions of mixed rare earths. The liquidus temperature (T{sub L}) of the glasses containing 5%, 10% and 15% La{sub 2}O{sub 3} were 800°C, 959°C and 986°C, respectively; while T{sub L} was 825°C, 1059°C and 1267°C for glasses with 5%, 10% and 15% addition of mixed rare earth oxides. The component coefficients T{sub B2O3}, T{sub SiO2}, T{sub CaO}, and T{sub RE2O3} were also evaluated using a recently published study.},
doi = {10.1063/1.4866127},
url = {https://www.osti.gov/biblio/22266070}, journal = {AIP Conference Proceedings},
issn = {0094-243X},
number = 1,
volume = 1584,
place = {United States},
year = {Wed Feb 12 00:00:00 EST 2014},
month = {Wed Feb 12 00:00:00 EST 2014}
}