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Development and Characterization of Rare Earth-Rich Glassy Matrices Envisaged for the Immobilization of Concentrated Nuclear Waste Solutions

I. Bardez, D. Caurant, J. L. Dussossoy, P. Loiseau, C. Gervais, F. Ribot, D. R. Neuville, N. Baffier, C. Fillet

Nuclear Science and Engineering / Volume 153 / Number 3 / July 2006 / Pages 272-284

Technical Paper / dx.doi.org/10.13182/NSE06-A2613

New nuclear highly durable glass compositions, able to immobilize a higher concentration of high-level nuclear wastes than current borosilicate nuclear glasses, are being studied. Investigations are performed on rare earth (RE)-rich glasses, known as durable matrices. After a preliminary study on complex and simplified compositions, a basic glass composition was selected and studied (wt%): 51.0 SiO2-8.5 B2O3-12.2 Na2O-4.3 Al2O3-4.8 CaO-3.2 ZrO2-16.0 RE2O3. Chemical durability, physical properties (viscosity, transformation temperature), and crystallization tendency of glasses containing either a mixture of RE (La + Ce + Pr + Nd) or only one RE were studied and compared. The local environment of RE (for RE = Nd) in the glass and its evolution according to Nd2O3 concentration (from 1.3 to 30 wt%) was also studied by coupling characterization methods such as extended X-ray absorption fine structure spectroscopy at the neodymium LIII-edge and optical absorption spectroscopy. 11B, 27Al magic angle spinning-nuclear magnetic resonance, and Raman spectroscopy were also used to study glass structure.