The possibility of insulation of long-lived actinides for the entire period of their potential hazard, i.e., over a virtually infinite time, is the crucial problem in safe disposal of high-level radioactive wastes (HLW). The reality of such a possibility is corroborated by the study of natural radioactive minerals that firmly retain U, Th, and REE, which are close in geochemical properties to transuranic actinides, for millions of years despite the effects of groundwater. The natural analogues of actinide HLW matrices are minerals where U, Th, and REE are contained as major elements or isomorphic admixtures. The study of these minerals is helpful for synthesis of durable artificial forms of wastes that ensure reliable insulation of HLW up to the complete decay of actinides independently of such engineering barriers of underground repositories as containers and bentonite buffers. The main requirements on confinement matrices include a high isomorphic capacity with respect to actinides and other HLW components, chemical and radiation stability, and technological feasibility of their industrial production. The natural and artificial minerals-uraninite, monazite, zirconolite, pyrochlore, britholite, garnet, and murataitecharacterized in this paper may serve as a basis for efficient matrices for immobilization of actinide wastes.
Extraction of the actinide-REE fraction and its subsequent incorporation into sparingly soluble crystalline phases (confinement matrices) is assumed in processing of spent nuclear fuel from high-level radioactive wastes (HLW). The chemical stability in the process of interaction with subsurface water governs the capability of a matrix phase to keep radionuclides from getting into the biosphere. In static experiments at 90 and 150 ° C, the chemical stability of ferrite garnets was investigated for three compositions with Th 4+ , Ce 4+ and Gd 3+ + serving as simulator components of the actinide fraction of HLW. Experiments were carried out in distilled water (pH 6.5), 0.01 M HCl solution (pH 2), and 0.01 M NaOH solution (pH 12). The behavior of ferrigarnet matrices depends on the acidity of the solution. In neutral and alkaline media, Th, Ce, and Gd are virtually not transferred into the liquid phase. Acid leaching promotes intense dissolution of garnet matrices. In this case, the leaching rate of Gd and Th from ceramics into the liquid phase is two orders of magnitude lower than the leaching rate of Ce because the Ce-doped phases contain less stable (relative to garnet) Ce-rich perovskite. Amorphization of the ferrigarnet structure due to 244 Cm isotope decay leads to an increase in the leaching rate of Cm by no more than five times. In terms of radiation and chemical stability, ferrite garnets are not inferior to zirconolites and titanate pyrochlores. The experimental results suggest that garnet matrices can reliably immobilize actinides in subsurface repositories.
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