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Ion-beam irradiation and 244Cm-doping investigations of the radiation response of actinide-bearing crystalline waste forms

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Abstract

Candidate materials for actinide immobilization are subject to alpha-decay event doses that accumulate to values of more than 1020 alpha-decays per gram (tens displacements per atom, dpa) over the extended periods of geologic disposal. To evaluate the radiation-response of actinide-bearing materials, two experimental techniques have been used to accelerate the damage accumulation process: ion-beam irradiations and 244Cm-doping experiments. Based on modern characterization techniques, such as high-resolution transmission electron microscopy, and experimental results that involve ion-beam irradiation and chemical doping with highly active actinides, crystalline ceramics for the immobilization of actinides can be divided into three groups on the basis of their critical doses, Dc, i.e., the dose required for amorphization at 300 K: (i) low resistance to radiation damage accumulation (Dc ∼ 0.2 dpa)–murataite, Ti-perovskite, Fe-garnet; (ii) resistant (0.4 < Dc < 0.6 dpa)–Al-garnet, Ti–Zr-pyrochlore, Al-perovskite; and (iii) highly resistant (Dc > 0.8 dpa)–Zr-, Zr–Ti-, and Sn-pyrochlores. Phases with low critical temperatures (Tc below 600 K) will not become amorphous in a deep geologic repository, as long as the temperature remains between 300 and 550 K, but rather, they will remain crystalline. Only Zr-rich pyrochlore is fully resistant to radiation damage and will remain crystalline over the entire period of its disposal.

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ACKNOWLEDGMENTS

The work was performed under the support of the Russian Foundation for Basic Research (Projects #13-05-00085 and #14-05-31034).

RCE’s effort and the ion-beam irradiation experiments were supported by the U.S. Department of Energy Office of Science, Office of Basic Energy Sciences Energy Frontier Research Centers program under Award Number DE-SC0001089.

The authors thank L.A. Kochetkova, M.S. Nikolsky, B.S. Nikonov for their help in examination of the specimens and V.I. Malkovsky for temperature calculations.

The electron microscopy with in situ ion irradiation was accomplished at Argonne National Laboratory at the IVEM-Tandem Facility, a U.S. Department of Energy Facility funded by the DOE Office of Nuclear Energy, operated under Contract No. DE-AC02-06CH11357 by the University of Chicago Argonne, LLC. L.M. Wang, S. Utsunomiya, J. Lian, J. Zhang, and W. Li thank the staff and scientists at HVEM- and IVEM-Tandem Facility at Argonne National Laboratory for their help and support during the ion irradiation experiments. This facility was essential for the completion of the studies summarized in this paper.

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  1. Laboratory of Radiogeology and Radiogeoecology, Institute of Geology of Ore Deposits, Petrography, Mineralogy and Geochemistry RAS, Moscow, 119017, Russia

    Sergey V. Yudintsev & Tatiana S. Livshits

  2. Radiochemical Department, Research Institute of Atomic Reactors, Dimitrovgrad-10, Ulyanovsk reg., Moscow, Russia

    Andrey A. Lizin & Sergey V. Tomilin

  3. Laboratory of Radioecological and Radiation Problems, Frumkin Institute of Physical Chemistry and Electrochemistry RAS, 119071, Moscow, Russia

    Sergey V. Stefanovsky

  4. Department of Geological and Environmental Sciences, Stanford University, Stanford, California, 94305, USA

    Rodney C. Ewing

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  1. Sergey V. Yudintsev
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Yudintsev, S.V., Lizin, A.A., Livshits, T.S. et al. Ion-beam irradiation and 244Cm-doping investigations of the radiation response of actinide-bearing crystalline waste forms. Journal of Materials Research 30, 1516–1528 (2015). https://doi.org/10.1557/jmr.2015.23

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