Nations using borosilicate glass as an immobilization material for radioactive waste have reinforced the importance of scientific collaboration to obtain a consensus on the mechanisms controlling the long-term dissolution rate of glass. This goal is deemed to be crucial for the development of reliable performance assessment models for geological disposal. The collaborating laboratories all conduct fundamental and/or applied research using modern materials science techniques. This paper briefly reviews the radioactive waste vitrification programs of the six participant nations and summarizes the current state of glass corrosion science, emphasizing the common scientific needs and justifications for on-going initiatives
Chemical durability is not a single material property that can be uniquely measured. Instead, it is the response to a host of coupled material and environmental processes whose rates are estimated by a combination of theory, experiment and modeling. High‐level nuclear waste (HLW) glass is perhaps the most studied of any material yet there remain significant technical gaps regarding their chemical durability. The phenomena affecting the long‐term performance of HLW glasses in their disposal environment include surface reactions, transport properties to and from the reacting glass surface, and ion exchange between the solid glass and the surrounding solution and alteration products. The rates of these processes are strongly influenced and are coupled through the solution chemistry, which is in turn influenced by the reacting glass and also by reaction with the near‐field materials and precipitation of alteration products. Therefore, those processes must be understood sufficiently well to estimate or bound the performance of HLW glass in its disposal environment over geologic time scales. This article summarizes the current state of understanding of surface reactions, transport properties and ion exchange along with the near‐field materials and alteration products influences on solution chemistry and glass reaction rates. Also summarized are the remaining technical gaps along with recommended approaches to fill those technical gaps.
International simple glass (ISG) is a six-component alumino-borosilicate glass developed as a reference benchmark glass for six nations collaborating study on high-level nuclear waste glass dissolution/corrosion mechanism. In this study, aqueous dissolution tests were performed for the ISG using microchannel flow-through (MCFT) method to evaluate the initial dissolution rate of glass matrix, r 0 , precisely and systematically as a function of solution pH and temperature. The test results indicated that the r 0 shows a "V-shaped" pH dependence with a bottom at around pH4 at each temperature. Compared with Japanese reference glass of P0798, for which the r 0 showed a "U-shaped" pH dependence with a bottom at around pH6 in our previous study, the ISG shows the higher dissolution rate at basic pH, and lower dissolution rate at neutral to acidic pH. The results also indicated that the r 0 increases with temperature according to an Arrhenius law, and the apparent activation energy evaluated from Arrhenius relation is 62-77 [kJ/mol] at any pH from 3 to 10, which suggests the initial dissolution of ISG proceeds controlled by a surface-reaction mechanism in this pH range.
Thermophysical properties of rare-earth-stabilized zirconia and zirconate pyrochlores, A 2 Zr 2 O 7 (A = La, Nd, Sm, Gd, Dy, Y), were evaluated by X-ray diffractometry, Raman spectroscopy, and the ultrasound pulse-echo method. Crystallographic analyses elucidated that had the pyrochlore structure, whereas Dy 2 Zr 2 O 7 and Y 2 Zr 2 O 7 had the defect fluorite structure. For lanthanide pyrochlores, the thermal expansion became smaller with increasing ionic radius of A and increasing crystal binding energy. The elastic moduli and Debye temperature evaluated using longitudinal and transverse sound velocities also depend on the ionic radius and binding energy, and hence these values related to mechanical properties increase with the ionic radius of A. On the other hand, Poisson's ratio was almost comparable among these pyrochlores. In addition, thermophysical properties of actinide pyrochlore are discussed in this study.
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