Product Models for the Vitrification of West Valley High-Level Wastes

1988 ◽  
Vol 127 ◽  
Author(s):  
I. L. Pegg ◽  
E. E. Saad ◽  
X. Feng ◽  
R. B. Adiga ◽  
W. P. Freeborn ◽  
...  

ABSTRACTProperty models have been developed for the major properties that need to be controlled in the production of borosilicate glasses for West Valley high-level nuclear waste immobilization. The chemical durability is the most important parameter for product performance, while melt viscosity is the most critical parameter in assuring the processability of the glass. Simple models for these properties are described that are based on data from numerous glasses which were prepared with compositions in the region around the West Valley reference glass. A scheme for optimization of the target glass and for predicting the acceptability of glasses resulting from natural process variations is illustrated. This involves integration of the product models with a process model that was described previously. This approach has guided the present placement of the West Valley reference glass.

1999 ◽  
Vol 5 (S2) ◽  
pp. 756-757
Author(s):  
S. X. Wang ◽  
L. M. Wang ◽  
R. C. Ewing

Zirconolite (CaZrTi207) is an important phase proposed for high level nuclear waste immobilization. Zirconolite was irradiated by 1 MeV Kr+ at various temperatures. At room temperature, zirconolite became amorphous after a dose of 7x1014 ions/cm2.1 Amorphization dose increased with temperature due to thermal annealing. The critical temperature, above which amorphization does not occur, was estimated to be 654 K. During the low temperature irradiation (<654 K), concurrent with amorphization, zirconolite transformed from a monoclinic structure to the cubic pyrochlore structure and then to the fluorite substructure. The structural change is due to the disordering between cations and between oxygen and oxygen vacancies.After an irradiation at 673 K to a dose of 3.6x1015 ions/cm, the zirconolite samples remained crystalline. The diffraction pattern consists of strong maxima from the fluorite structure and diffuse maxima surrounding the Bragg positions of the pyrochlore superlattice (FIG. 1). Diffuse scattering patterns have been reported in other phases, and were generally attributed to the shortrange- order (SRO) domains.


MRS Advances ◽  
2016 ◽  
Vol 1 (63-64) ◽  
pp. 4201-4206 ◽  
Author(s):  
Rebecca A. Robbins ◽  
Michael I. Ojovan

ABSTRACTVitreous materials are the overwhelming world-wide choice for the immobilisation of HLW resulting from nuclear fuel reprocessing due to glass tolerance for the chemical elements found in the waste as well as its inherent stability and durability. Vitrification is a mature technology and has been used for high-level nuclear waste immobilization for more than 50 years. Borosilicate glass is the formulation of choice in most applications although other formulations are also used e.g. phosphate glasses are used to immobilize high level wastes in Russia. The excellent durability of vitrified radioactive waste ensures a high degree of environment protection. Waste vitrification gives high waste volume reduction along with simple and cheap disposal facilities. Although vitrification requires a high initial investment and then operational costs, the overall cost of vitrified radioactive waste is usually lower than alternative options when account is taken of transportation and disposal expenses. Glass has proven to be also a suitable matrix for intermediate and low-level radioactive wastes and is currently used to treat legacy waste in USA, and NPP operational waste in Russia and South Korea. This report is also outlining IAEA activities aiming to support utilisation of vitreous materials for nuclear waste immobilisation.


2003 ◽  
Vol 807 ◽  
Author(s):  
Adam Duddridge ◽  
Moinul Islam ◽  
Diane Holland ◽  
Charlie R. Scales

ABSTRACTA mixed-alkali modified borosilicate base glass used in the vitrification of high-level nuclear waste (HLW) has been doped with a number of waste simulants to between 2 and 12 mol%. The simulants have been chosen to give two distinct series of glasses: one consisting of trivalent ions having the form M2O3(where M is La, Bi, Al or Fe) and the other consisting of divalent simulants of the form MO (where M is Pb, Zn or Ba). An international standard Soxhlet leach test procedure was performed on each glass to study the effect of prolonged, moderate-temperature, dynamic water corrosion. Results of these studies show that, except for BaO, as the amount of simulant is increased, the amount of Na and Li leached decreases showing them to become more chemically resistant. These corrosion tests have been correlated to ionic (D.C.) conductivity measurements, which show a decrease in the conductivity of the glass as the amount of waste simulant is increased, and 11B magic-angle spinning nuclear magnetic resonance (MAS-NMR) studies, which have shown that, as more waste-simulant is loaded into the glasses the rate of conversion of [BO4] to [BO3] units increases. All of the data from these studies reflect the different network forming abilities of the divalent and trivalent cations.


2010 ◽  
Vol 1265 ◽  
Author(s):  
Odile Majerus ◽  
Daniel Caurant ◽  
Ning Li ◽  
Jean-Baptiste Baudouin ◽  
Gabriela Manolescu ◽  
...  

AbstractThe high level nuclear waste load is likely to increase in the future containment glasses, rising new questions about their long-term chemical durability. In this study sodium borosilicate compositions with Si substituted for RE (RE = rare earth) are altered under static conditions at fixed pH (8.5). The Na and B leached fractions reached just after the rate drop increase with the RE2O3 content. Part of the RE ions remain in the altered layer which is significantly de-polymerised (IR-ATR and NMR results). Their environment is reorganized and adopts a more centrosymetrical character. The higher leached fractions are attributed to rapid hydrolysis of Si/B-O-RE bonds with respect to Si-O-Si bonds.


2008 ◽  
Vol 1124 ◽  
Author(s):  
Karl R Whittle ◽  
Mark Blackford ◽  
Gregory R Lumpkin ◽  
Katherine L Smith ◽  
Nestor J Zaluzec

AbstractGarnets, A3B2C3O12, are considered to be potential host phases for the immobilization of high-level nuclear waste as they can accommodate a number of elements of interest, including Zr, Ti and Fe. The naturally occurring garnet, kimzeyite, Ca3(Zr,Ti)2(Si,Al,Fe)3O12, can contain ˜30wt% Zr. An understanding of the radiation tolerance of these materials is crucial to their potential use in nuclear waste immobilization. In this study two synthetic analogues of kimzeyite of composition Ca3Zr2FeAlSiO12 and Ca3Hf2FeAlSiO12 were monitored in situ during irradiation with 1.0 MeV Kr ions using the intermediate voltage electron microscope-Tandem User Facility (IVEM) at Argonne National Laboratory. The structure of these materials was previously determined by neutron diffraction and 57Fe Mössbauer spectroscopy. Ca3Zr2FeAlSiO12 and Ca3Hf2FeAlSiO12 have very similar structural properties with cubic Ia3d symmetry, the only significant difference being the presence of Zr and Hf, respectively, on the 6 coordinated B sites.


2012 ◽  
Vol 1475 ◽  
Author(s):  
Diana Carolina Lago ◽  
Diana Garcés ◽  
Miguel Oscar Prado

ABSTRACTSiO2-Al2O3-Y2O3 glasses exhibit high glass transition temperatures, water corrosion resistance and good mechanical properties. These properties suggest that yttrium aluminosilicate glasses could potentially replace the borosilicate glasses usually used for immobilization of nuclear wastes. At the same time, yttrium can be used to simulate actinides.During waste immobilization, crystallization of the glassy matrix must be avoided or at least controlled, thus, the understanding of glass crystallization kinetics is essential.We found by XRD that the crystalline phases present on heat treatments are yttrium disilicate and sillimanite/mullite. By optical microscopy on polished cross-sections we could only identify highly yttrium enriched crystals which we associate with yttrium disilicate crystals.In this paper we measure the surface density of nucleation sites Ns in as obtained splat cooled pieces obtaining values of about 1.5 · 1011 nucleus · m-2. Crystal growth rate U in the temperature range 1000-1040 oC varies in the range 8-13 μm · h-1. These data are useful for designing sintering or melting thermal paths of YAS glasses in order to control their microstructure. We show the effect of glass particle size on DTA results: crystallization peaks moves towards lower temperatures for smaller particle size, which confirms that mainly surface nucleation is taking place on heating.


1988 ◽  
Vol 125 ◽  
Author(s):  
Ned E. Bibler ◽  
David G. Howitt

ABSTRACTThe study of radiation effects in complex silicate glasses has received renewed attention because of their use in special applications such as high level nuclear waste immobilization and fiber optics. Radiation changes the properties of these glasses by altering their electronic and atomic configurations. These alterations or defects may cause dilatations or microscopic phase changes along with absorption centers that limit the optical application of the glasses. Atomic displacements induced in the already disordered structure of the glasses may affect their use where heavy irradiating particles such as alpha particles, alpha recoils, fission fragments, or accelerated ions are present. Large changes (up to 1%) in density may result. In some cases the radiation damage may be severe enough to affect the durability of the glass in aqueous solutions.In this paper, we review the literature concerning radiation effects on density, durability, stored energy, microstructure and optical properties of silicate glasses. Both simple glasses and complex glasses used for immobilization of nuclear waste are considered.


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