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Solidification of glass-ceramics of simulated fission products RE3+, Sr2+, Ba2+ in chlorine-containing waste molten salt
Affiliation:1. Institute of Solid State Chemistry UB RAS, 620041, 91, Pervomayskaya St., Yekaterinburg, Russia;2. Institute of Natural Science and Mathematics, Ural Federal University, 620000, 51 Lenin Av., Yekaterinburg, Russia;3. Laboratory of Hydrogen Energy, Ural Federal University, 620002, 19 Mira St., Yekaterinburg, Russia;1. Chemistry Department, Faculty of Science, King Abdulaziz University, P.O. Box 80203, Jeddah, 21589, Saudi Arabia;2. Nanomaterials and Nanotechnology Department, Advanced Materials Institute, Central Metallurgical R&D Institute (CMRDI), P.O. Box 87 Helwan, 11421, Cairo, Egypt;1. School of Materials and Metallurgy, University of Science and Technology Liaoning, Anshan, 114051, China;2. School of Metallurgical Engineering, Liaoning Institute of Science and Technology, Benxi, 117004, China;3. Haicheng Far East Mining Co. Ltd, Anshan, 114200, China;1. Jerzy Haber Institute of Catalysis and Surface Chemistry, Polish Academy of Sciences, Niezapominajek 8, PL–30239, Krakow, Poland;2. Department of Inorganic Chemistry, Faculty of Natural Sciences, Comenius University in Bratislava, Ilkovicova 6, Mlynska Dolina, 842 15, Bratislava, Slovakia;3. Institute of Applied Electrodynamics and Telecommunications, Faculty of Physics, Vilnius University, Sauletekio al. 9/3, 10222, Vilnius, Lithuania;4. AGH University of Science and Technology, Faculty of Material Science and Ceramics, Mickiewicza 30, Krakow, Poland;5. Department of Experimental Physics, Faculty of Mathematics, Physics, and Informatics, Comenius University Bratislava, 842 48, Bratislava, Slovakia;1. Key Lab. for New Type of Functional Materials in Hebei Province, School of Materials Science and Engineering, State Key Laboratory of Reliability and Intelligence of Electrical Equipment, Tianjin Key Laboratory of Materials Laminating Fabrication and Interface Control Technology, Hebei University of Technology, 300132, Tianjin, China;2. AECC Sichuan Gas Turbine Establishment, Sichuan Province, Chengdu, 610500, China
Abstract:Embedding nuclear waste in glass-ceramic and immobilizing nuclides in ceramic lattice is an effective way for the disposal of high-level radioactive waste. In this paper, a method of solidification of simulated various nuclides was proposed, i.e., RE3+(RE = La, Sm, Nd, Dy), Sr2+ and Ba2+ precipitated from waste molten salt in the form of REPO4, SrCO3 and BaCO3 were solidified in glass-ceramics. To avoid the decomposition of SrCO3 and BaCO3 at high temperature, SrCO3/BaCO3 containing Cl? salt was further sintered with NH4H2PO4 to form Sr5(PO4)3Cl/Ba5(PO4)3Cl ceramics. It was found that the prepared REPO4 belonged to monoclinic or tetragonal crystal system, while Sr5(PO4)3Cl and Ba5(PO4)3Cl belonged to hexagonal crystal system. REPO4, Sr5(PO4)3Cl and Ba5(PO4)3Cl ceramics were co-solidified in iron phosphate glass. BET results showed that the ceramics had a dense structure without any pore inside. XRD, TEM and HRTEM results showed all ceramics had high crystallinity, and nuclides could enter the lattice structure of ceramics through isomorphic replacement, which made the nuclides stable in the crystal structure. The effects of embedding rate on the volume density, Vickers hardness and wettability of glass-ceramics were explored. It was found that the density of the glass-ceramics gradually increased with the increase of ceramic embedding rate, however, the Vickers hardness firstly increased and then decreased. When the embedding rate reached 20 wt%, the Vickers hardness of the glass-ceramics could reach 583.90 GPa. The water contact angles of glass-ceramics with an embedding rate 0–40 wt% were measured to be 70.45°–84.05°, indicating glass-ceramics having a good water leaching resistance. Furthermore, the normalized leaching rate NRi of La3+, Sm3+, Nd3+, Dy3+, Sr2+, Ba2+, Cl? on the 28th day were estimated to be 7.53 × 10?7, 5.02 × 10?7, 5.12 × 10?7, 4.04 × 10?7, 1.22 × 10?3, 1.59 × 10?4, 1.07 × 10?4 g?m?2?d?1, which indicating that all elements remained good leaching resistance.
Keywords:Spent electrolyte  Precipitate  Iron phosphate glass  Glass-ceramics  Normalized leaching rate
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