Effect of glass content on the phase assemblage and processing requirements of zirconolite glass-ceramics for actinide immobilisation

被引:0
作者
Abraham, Joel L. [1 ,2 ]
Dayal, Pranesh [2 ]
Farzana, Rifat [2 ]
Bahmanrokh, Ghazaleh [2 ]
Aughterson, Robert D. [2 ]
Zhang, Zhaoming [2 ]
Holmes, Rohan [2 ]
Hamilton, Jessica L. [3 ]
Sorrell, Charles C. [1 ]
Koshy, Pramod [1 ]
Gregg, Daniel J. [2 ]
机构
[1] UNSW Sydney, Sch Mat Sci & Engn, Kensington, NSW 2052, Australia
[2] Australian Nucl Sci & Technol Org ANSTO, Locked Bag 2001, Kirrawee, NSW 2232, Australia
[3] Australian Synchrotron ANSTO, Clayton, Vic 3168, Australia
关键词
Zirconolite; Glass-ceramic; Thermal processing; Synroc technology; Actinide waste immobilisation; PLUTONIUM IMMOBILIZATION; CHARGE COMPENSATION; BOROSILICATE GLASS; RADIOACTIVE-WASTE; CE; STABILITY; CERIUM; ND;
D O I
10.1016/j.jeurceramsoc.2024.116890
中图分类号
TQ174 [陶瓷工业]; TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Zirconolite is a candidate wasteform for actinides (U/Pu/Th), and glass incorporation to form glass-ceramics provides flexibility to accommodate heterogeneous wastes while simplifying processing requirements; however, the glass content required to optimise these benefits remains unestablished. This systematic study investigated the effect of glass content on zirconolite crystallisation, phase assemblage, phase composition, cerium valence states and partitioning. Cerium-bearing zirconolite glass-ceramics were fabricated by targeting zirconolite (Ca0.8Ce0.2ZrTi1.6Al0.4O7; Ce as actinide surrogate) with varying amounts (0-100 vol%) of glass addition (NaAl1.5B0.5Ca0.7Ti0.2Si2O8.6). Differential scanning calorimetry data revealed that glass addition lowered the zirconolite crystallisation temperature (1283 degrees C to 1200 degrees C). X-ray diffraction, scanning electron microscopy, and energy dispersive X-ray spectroscopy analyses showed that glass addition lowered the temperature (1320 degrees C to 1270 degrees C) required to fabricate phase-pure zirconolite glass-ceramics and minimise CeO2/ZrO2 phases, with > 90 % of cerium preferentially partitioned into zirconolite. X-ray absorption near edge spectroscopy data showed predominantly Ce4+ within zirconolite as targeted.
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页数:13
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