Abstract:
Crystallization of borosilicate glasses, used now for solidification of liquid nuclear high-level wastes (HLW), is accompanied by the formation of silicates with the apatite-type structure and high contents of actinides and REE. The stability of these silicates determines the safety of immobilization of radionuclides. As a result of radioactive decay, the crystalline phases of actinides become amorphous with time and their solubility in aqueous solutions increases. One of the ways to assess the radiation stability of compounds is the study of their natural analogues that contain radioactive elements. Minerals of the britholite group are the natural analogues of synthetic rare earth silicates and actinides with the apatite-type structure. Seven britholites of different ages and with different ThO2 + UO2 contents have been studied. The stages of partial damage and complete destruction of sample structures under the effect of radioactive decay were distinguished. The radiation stability of natural britholites surpasses that of their synthetic analogues. The annealing of metamict samples recovers the primary apatite-type structure without formation of any other phases. With an increase in annealing duration from 1 to 5 h, the mineral structure is recovered at a lower (by 200°C) temperature (down to 550-600°C). The temperature conditions in underground storages and the substantially longer occurrence of HLW therein will prevent crystalline matrices with the apatite-type structure from amorphization and thus ensure the retention of their stability. © Pleiades Publishing, Inc. 2006.
