Isolation of long-lived technetium-99 in confinement matrices |
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| Authors: | N P Laverov S V Yudintsev B I Omel’yanenko |
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| Institution: | 1.Institute of Geology of Ore Deposits, Petrography, Mineralogy, and Geochemistry,Russian Academy of Sciences,Moscow,Russia |
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| Abstract: | Amongst fission products formed in atomic reactors, 99Tc is the most hazardous for the environment because of its long half-life (213000 yr), high content in spent nuclear fuel
(SNF) (0.8–1.0 kg per ton of SNF), low sorption ability, and high mobility under aerobic conditions. The bulk of 99Tc (∼200 t) is incorporated into SNF. In the course of SNF reprocessing, this radioisotope is released as a separate fraction
or along with actinides. More than 60 t of highly concentrated 99Tc have been accumulated to date. It is evident that isolation of 99Tc from the environment is a matter of great urgency. The immobilization of technetium in a highly stable and poorly soluble
matrix is a necessary element in settling this problem. Ceramics composed of titanates with pyrochlore, perovskite, and rutile
structures are proposed as matrices able to retain technetium along with actinides. The high chemical stability of these compounds
has been corroborated by experiments. The difficulties in production of such matrices are related to the fugacity of Tc and
the necessity of converting it into Tc(IV). To overcome this obstacle, self-propagating high-temperature synthesis (SHS),
characterized by reductive conditions and a high reaction rate, is proposed. The charge for matrix synthesis consists of reducing
agents (metallic powders with a strong affinity to oxygen, e.g., Ti and Zr), oxidants (MoO3, Fe2O3, CuO), and additives (TiO2, ZrO2, Y2O3, CaO, etc.), which taken together with other elements form target phases. Instead of Tc, Mo, close in chemical properties,
is used in matrix synthesis as a simulator. Samples of Mo-bearing matrices have been synthesized with SHS; their phase compositions
and Mo distribution therein are characterized. It has been shown that up to 40 wt % Mo can be incorporated into the synthesized
matrices in the form of metal or structural admixtures in titanates. The titanate-zirconate pyrochlore-based matrices are
the most appropriate for the joint immobilization of actinides, REEs, and 99Tc. |
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