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Geology of Ore Deposits

, Volume 48, Issue 5, pp 357–368 | Cite as

Britholites as natural analogues of actinide matrices: Resistance to radiation damage

Article

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.

Keywords

Natural Analogue Radiation Stability Waste Form Annealing Duration Underground Storage 
These keywords were added by machine and not by the authors. This process is experimental and the keywords may be updated as the learning algorithm improves.

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References

  1. 1.
    O. A. Belyaev, F. P. Mitrofanov, T. B. Bayanova, et al., “The Late Archean Age of Acid Metavolcanic Rock in the Lesser Keivy, Kola Peninsula,” Dokl. Akad. Nauk 379(5), 651–654 (2001) [Dokl. Earth Sci. 379A (6), 705–708 (2001)].Google Scholar
  2. 2.
    V. V. Chuprov, “Accessory Minerals of the Kharitonovsky Alkaline Massif,” Zap. Vseross. Mineral. O-va 101(4), 430–437 (1972).Google Scholar
  3. 3.
    R. C. Ewing, “The Design and Evaluation of Nuclear-Waste Forms: Clues from Mineralogy,” Can. Mineral. 39, 697–715 (2001).Google Scholar
  4. 4.
    R. C. Ewing, W. J. Weber, and F. W. Clinard, “Radiation Effects in Nuclear Waste Forms for High-Level Radioactive Waste,” in Progress in Nuclear Energy (1995), Vol. 29, pp. 63–127.CrossRefGoogle Scholar
  5. 5.
    A. A. Glushchenko and A. F. Li, “Britholite from an Alkaline Massif in the Northern Baikal Region,” Proc. Irkutsk State Research Institute of Rare and Nonferrous Metals, No. 14, 100–107 (1966).Google Scholar
  6. 6.
    W. L. Gong, L. M. Wang, R. C. Ewing, et al., “Transmission Electron Microscopy Study of α-Decay Damage in Aeschynite and Britholite,” in Proceedings of Symposium on Scientific Basis for Nuclear Waste Management XX (MRS, Pittsburgh, 1997), Vol. 465, pp. 649–656.Google Scholar
  7. 7.
    I. I. Kupriyanova, G. A. Sidorenko, and M. A. Kudrina, “Minerals of Britholite Group,” in Geology of Rare-Element Deposits. Rare Earth Silicates (Nedra, Moscow, 1966), No. 26, pp. 23–66 [in Russian].Google Scholar
  8. 8.
    G. R. Lumpkin, “Alpha-Decay Damage and Aqueous Durability of Actinide Host Phases in Natural Systems,” J. Nucl. Mater. 289, 136–166 (2001).CrossRefGoogle Scholar
  9. 9.
    G. R. Lumpkin and B. C. Chakoumakos, “Chemistry and Radiation Effects of Thorite-Group Minerals from the Harding Pegmatite, Taos Country, New Mexico,” Am. Mineral. 73, 1405–1419 (1988).Google Scholar
  10. 10.
    J. A. C. Marples, “Vitrification of Plutonium for Disposal,” in Disposal of Weapon Plutonium (Kluwer Acad. Publ. 1996), pp. 179–195.Google Scholar
  11. 11.
    S. V. Nechaev and S. G. Krivdyuk, “Spatial Distribution of Alkaline Rocks in the Ukrainian Shield,” Geol. Zh., No. 3, 113–120 (1989).Google Scholar
  12. 12.
    Phosphate Glasses with Radioactive Waste, Ed. by A. A. Vashman and A. S. Polyakov (TSNIIAtominform, Moscow, 1997) [in Russian].Google Scholar
  13. 13.
    E. G. Proshchenko, I. D. Belyaeva, S. I. Lebedeva, and E. B. Khalezova, “Mechanism of Metamict Britholite Crystallization as a Result of Heating,” Mineral. Sb. 26(3), 306–312 (1972).Google Scholar
  14. 14.
    Radioactive Waste Forms for the Future (Elsevier, New York, 1988).Google Scholar
  15. 15.
    A. E. Ringwood, “Disposal of High-Level Nuclear Wastes: A Geological Perspective,” Mineral. Mag. 49, 159–176 (1985).Google Scholar
  16. 16.
    P. B. Rose, M. I. Ojovan, N. C. Hyatt, and W. E. Lee, “Crystallization within Simulated High Level Waste Borosilicate Glass,” in Proceedings of Symposium on Scientific Basis for Nuclear Waste Management XXVIII (MRS, Warrendale, 2004), Vol. 824, pp. 321–3260.Google Scholar
  17. 17.
    T. V. Smelova, N. V. Krylova, S. V. Yudintsev, and B. S. Nikonov, “Silicate Matrix of Actinide-Bearing Wastes,” Dokl. Akad. Nauk 374(2), 242–246 (2000) [Dokl. Earth Sci. 374 (7), 1149–1152 (2000)].Google Scholar
  18. 18.
    C. G. Sombret, “Waste Forms for Conditioning High-Level Radioactive Solutions,” in Geol. Disposal of High-Level Radioactive Wastes (Theoph. Publ, Athens, 1987).Google Scholar
  19. 19.
    S. Utsunomiya, S. Yudintsev, L. M. Wang, and R. C. Ewing, “Ion Beam and Electron Beam Irradiation of Synthetic Britholite,” J. Nucl. Mater. 322, 180–188 (2003).CrossRefGoogle Scholar
  20. 20.
    W. J. Weber, R. C. Ewing, C. A. Angell, et al., “Radiation Effects in Glasses Used for Immobilization of High-Level Waste and Plutonium Disposition,” J. Mater. Res. 12(8), 1946–1975 (1997).Google Scholar
  21. 21.
    W. J. Weber and R. C. Ewing, “Radiation Effects in Crystalline Oxide Host Phases for the Immobilization of Actinides,” in Proceedings of Symposium on Scientific Basis for Nuclear Waste Management XXVI (MRS, Warrendale, 2002), Vol. 713, pp. 443–454.Google Scholar
  22. 22.
    D. Zhao, L. Li, L. L. Davis, et al., “Gadolinium Borosilicate Glass-Bonded Gd-Silicate Apatite: A Glass-Ceramic Nuclear Waste Form for Actinides,” in Proceedings of Symposium on Scientific Basis for Nuclear Waste Management XXIV (MRS, Warrendale, 2001), Vol. 556, pp. 199–206.Google Scholar
  23. 23.
    A. Ya. Zhidkov, S. L. Mirkina, and M. N. Golubchina, “Absolute Age of Alkaline and Nepheline Syenites in the North Baikal Highland,” Dokl. Akad. Nauk SSSR 149(1), 152–155 (1963).Google Scholar

Copyright information

© Pleiades Publishing, Inc. 2006

Authors and Affiliations

  1. 1.Institute of Geology of Ore Deposits, Petrography, Mineralogy, and GeochemistryRussian Academy of SciencesMoscowRussia

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