J Am Ceram Soc. 2020;00:1–10. wileyonlinelibrary.com/journal/jace
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1 © 2020 The American Ceramic Society
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INTRODUCTION
High-level wastes (HLWs) arising from the reprocessing of
spent nuclear fuels (SNFs) contain some fission products and
transuranium minor actinides with long half-lives, and safe
storage and disposal of these HLWs have become an urgent
global issue.
1-3
It is essential to adopt a proper conditioning
process to convert HLWs to physically stable and chemically
durable solid waste forms, suitable for further waste manage-
ment such as transportation, interim storage, and final geo-
logical disposal.
1-4
While borosilicate glass has been widely investigated as
the most popular medium for the immobilization of HLWs
from the reprocessing of civilian SNFs,
2-4
synthetic rock (ab-
breviated as synroc, which contains a group of stable titanate
mineral phases such as zirconolite, pyrochlore, brannerite,
hollandite, perovskite etc) as a representative for ceramic
waste forms has also been developed, originally for the immo-
bilization of HLWs from Purex-type reprocessing of SNFs.
5-9
Subsequently, synroc formulations based on zirconolite and
pyrochlore have been tailored for the immobilization of var-
ious actinide-rich radioactive wastes including excess weap-
ons plutonium.
10-15
The obvious advantages for synroc-type
ceramic waste forms over the conventional borosilicate
Received: 27 December 2019
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Revised: 27 February 2020
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Accepted: 12 March 2020
DOI: 10.1111/jace.17119
SPECIAL ISSUE ARTICLE
Pyrochlore glass-ceramics fabricated via both sintering and hot
isostatic pressing for minor actinide immobilization
Yingjie Zhang
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Zhaoming Zhang
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Tao Wei
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Linggen Kong
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Young J. Kim
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Daniel J. Gregg
In commemeration of Dr Eric R. Vance (1942-2019)
Australian Nuclear Science and Technology
Organisation, Kirrawee DC, NSW, Australia
Correspondence
Yingjie Zhang, Australian Nuclear Science
and Technology Organisation, Kirrawee
DC, NSW, Australia.
Email: yzx@ansto.gov.au
Abstract
Pyrochlore glass-ceramics (GCs) have been investigated with samples fabricated via
both sintering and hot isostatic pressing (HIPing) of a mixed oxide precursor. It has
been demonstrated that sintering at 1200°C in air is necessary to obtain well-crystal-
lized pyrochlore crystals in a sodium aluminoborosilicate glass through a one-step
controlled cooling. The crystallization, structure, and microstructure of Eu
2
Ti
2
O
7
py-
rochlore as the major phases in residual glass were confirmed with X-ray diffraction
(XRD), scanning electron microscopy-energy dispersive spectroscopy, transmission
electron microscopy, and Raman spectroscopy. The structures of major Eu
2
Ti
2
O
7
pyrochlore and minor [Eu
4.67
O(SiO
4
)
3
] apatite in both sintered and HIPed samples
were refined using synchrotron XRD data. While the processing atmosphere did not
appear to affect the cell parameter of the main pyrochlore phase, very small volume
expansion (~0.3%) was observed for the minor apatite phase in the HIPed sample.
In addition, static leaching of the HIPed sample confirmed that pyrochlore GCs are
chemically durable. Overall, pyrochlore GCs prepared via both sintering and HIPing
with the Eu partitioning factor of ~23 between ceramics and the residual glass are
suitable waste forms for minor actinides with processing chemicals.
KEYWORDS
europium, glass-ceramics, nuclear waste, pyrochlore, titanates