Stability of Cubic Zirconia in a Granitic System Under High Pressure & Temperature

2008 ◽  
Vol 1107 ◽  
Author(s):  
Fergus G.F. Gibb ◽  
Boris E. Burakov ◽  
Kathleen J. Taylor ◽  
Yana Domracheva
Keyword(s):  
Radioactive Wastes ◽  
Waste Form ◽  
Deep Borehole ◽  
Spent Fuel ◽  
Zirconia Crystal ◽  
Cubic Zirconia ◽  
Inert Matrix ◽  
Waste Forms ◽  
Glassy Sample ◽  
Container Material

AbstractCubic zirconia is a well known, highly durable material with potential uses as an actinide host phase in ceramic waste forms and inert matrix fuels and in containers for very deep borehole disposal of some highly radioactive wastes. To investigate the behaviour of this material under the conditions of possible use, a cube of ∼ 2.5 mm edge was made from a single crystal of yttriastabilized cubic zirconia doped with 0.3 wt.% CeO2. The cube was enclosed in powdered granite within a gold capsule and a small amount of H2O added before sealing. The sealed capsule was held for 4 months in a cold-seal pressure vessel at a temperature of 780°C and a pressure 150 MPa, simulating both the conditions of a deep borehole disposal involving partial melting of the host rock and the conditions under which the actinide waste form might be encapsulated in granite prior to disposal. At the end of the experiment the quenched, largely glassy, sample was cut into thin slices and studied by optical microscopy, EMPA, SEM and cathodoluminescence methods. The results show that no corrosion of the zirconia crystal or reaction with the granite melt occurred and that no detectable diffusion of elements, including Ce, in or out of the zirconia took place on the timescale of the experiment. Consequently, it appears that cubic zirconia could perform most satisfactorily as both an actinide host waste form for encapsulation in solid granite for very deep disposal and as a container material for deep borehole disposal of highly radioactive wastes (HLW), including spent fuel.

Performance Assessment of Zircon as a Waste Form for Excess Weapons Plutonium Under Deep Borehole Burial Conditions

1995 ◽  
Vol 412 ◽  
Author(s):  
W. J. Weber ◽  
R. C. Ewing ◽  
W. Lutze
Keyword(s):  
Performance Assessment ◽  
Radiation Damage ◽  
Alpha Decay ◽  
Chemical Durability ◽  
Waste Form ◽  
Accessory Mineral ◽  
Deep Borehole ◽  
Waste Forms ◽  
Weapons Grade Plutonium ◽  
Precambrian Terranes

AbstractZircon (ZrSiO4) is proposed as a waste form for excess weapons-grade plutonium. Zircon is an extremely durable ceramic that is often found as an accessory mineral in Precambrian terranes with ages up to 4 billion years. The chemical durability of zircon in groundwater far exceeds that of other waste forms, as modeled leach rates may be as low as 10-11g/m2d. At least 10 wt% Pu can substitute for Zr in zircon. Self-radiation damage from alpha decay leads to a crystalline-to-amorphous transformation that is modeled as a function of time and temperature for deep borehole conditions. Based on the results of this assessment, zircon could meet all necessary durability and criticality criteria required for a Pu waste form. The types of data used in this analysis are generally not available for other crystalline ceramics or glasses.

Interim Waste Forms for High-Level Radioactive Wastes: Processing and Properties

1981 ◽  
Vol 6 ◽  
Author(s):  
G. Bandyopadhyay
Keyword(s):  
Sodium Silicate ◽  
Water Solubility ◽  
Mechanical Stability ◽  
Solid Material ◽  
High Water ◽  
Radioactive Wastes ◽  
Waste Form ◽  
Waste Forms ◽  
High Level ◽  
Fused Salt

ABSTRACTSeveral simulated interim waste forms have been investigated in the laboratory to study their suitability for application in handling and transportation of high-level radioactive wastes to terminal processing sites. In the fused-salt/sludge option, the neutralized supernatant liquid and the precipitated sludge are treated simultaneously to form fused-salt cakes. Silicate-based options, in which sodium silicate or sodium silicate and Ca(OH)2 act as binders for the sludge, require prior separation of the sludge and the soluble radioactive constituents from the supernatant before the waste form can be prepared. The results from tests on simulated fused-salt waste forms indicated that the process simplicity of this option is partially offset by the high water solubility and hygroscopicity of the product, which would necessitate special precautions during transportation and storage. The most promising silicate-based option is the ambienttemperature silicate sludge process, in which the sludge is mixed with sodium silicate [and sometimes with Ca(OH)2] and subsequently exposed to a contrelled-humidity environment at room temperature to form a chemical bond. Solid material containing 75 wt % synthetic calcined sludge, prepared by this process, has sufficient physical, chemical, and mechanical stability for use as an interim waste form.

Interpreting Uranyl Mineral Diffraction Patterns

1998 ◽  
Vol 4 (S2) ◽  
pp. 560-561
Author(s):  
Edgar C. Buck
Keyword(s):  
Corrosion Behavior ◽  
Nuclear Waste ◽  
Equatorial Plane ◽  
Waste Form ◽  
Spent Fuel ◽  
Secondary Phases ◽  
Form Complex ◽  
Waste Forms ◽  
Diffraction Patterns ◽  
Nuclear Waste Forms

Secondary phases that form during the corrosion of nuclear waste forms may influence both the rate of waste form dissolution and the release of radionuclides [1]. The identification of these phases is critical in developing models for the corrosion behavior of nuclear waste forms. In particular, the secondary uranyl (VI) minerals that form during waste form alteration may control uranium solubility and release of radionuclides incorporated into these phases [2].The U6+ cation in uranyl minerals is almost always present as a linear (UO2)2+ ion [3]. This uranyl (Ur) ion is coordinated by four, five, or six anions (ϕ) in the equatorial plane resulting in the formation of square (Urϕ4), pentagonal (Urϕ5), and hexagonal (Urϕ6) bipyramids, respectively [3]. These bipyramid polyhedra may polymerize to form complex infinite sheet structures. The linking of Urϕ5 is observed in a number of uranyl minerals formed during waste glass and spent fuel corrosion [2,4], such as weeksite [Na,K(UO2)2(Si205)3*4H2O] and β-uranophane [Ca[(UO2)(SiO3OH)]2*5H2O].

The Strategy of the Belgian Nuclear Research Centre in the Area of High-Level Waste Form Compatibility Research

2007 ◽  
Author(s):  
Karel Lemmens ◽  
Christelle Cachoir ◽  
Elie Valcke ◽  
Karine Ferrand ◽  
Marc Aertsens ◽  
...  
Keyword(s):  
Nuclear Research ◽  
Waste Form ◽  
Research Centre ◽  
High Level Waste ◽  
Spent Fuel ◽  
National Agency ◽  
Waste Forms ◽  
In Situ Experiments ◽  
High Level

The Belgian Nuclear Research Centre (SCK•CEN) has a long-standing expertise in research concerning the compatibility of waste forms with the final disposal environment. For high level waste, most attention goes to two waste forms that are relevant for Belgium, namely (1) vitrified waste from the reprocessing of spent fuel, and (2) spent fuel as such, referring to the direct disposal scenario. The expertise lies especially in the study of the chemical interactions between the waste forms and the disposal environment. This is done by laboratory experiments, supported by modeling. The experiments vary from traditional leach tests, to more specific tests for the determination of particular parameters, and highly realistic experiments. This results in a description of the phenomena that are expected upon disposal of the waste forms, and in quantitative data that allow a conservative long-term prediction of the in situ life time of the waste form. The predictions are validated by in situ experiments in the underground research laboratory HADES. The final objective of these studies, is to estimate the contribution of the waste form to the overall safety of the disposal system, as part of the Safety and Feasibility Case, planned by the national agency ONDRAF/NIRAS. The recent change of the Belgian disposal concept from an engineered barrier system based on the use of bentonite clay to a system based on a concrete buffer has caused a reorientation of the research programme. The expertise in the area of clay-waste interaction will however be maintained, to develop experimental methodologies in collaboration with other countries, and as a potential support to the decision making in those countries where a clay based near field is still the reference. The paper explains the current R&D approach, and highlights some recent experimental set-ups available at SCK•CEN for this purpose, with some illustrating results.

scholarly journals Development of New Waste Forms to Immobilize Iodine-129 Released from a Spent Fuel Reprocessing Plant

2010 ◽  
Vol 73 ◽  
pp. 158-170 ◽  
Author(s):  
Hiromi Tanabe ◽  
Tomofumi Sakuragi ◽  
Kenji Yamaguchi ◽  
Taemi Sato ◽  
Hitoshi Owada
Keyword(s):  
Radioactive Wastes ◽  
Behavior Modeling ◽  
Spent Fuel ◽  
Waste Forms ◽  
Reducing Conditions ◽  
Geological Repository ◽  
Spent Fuel Reprocessing ◽  
Immobilization Techniques ◽  
Reprocessing Plant ◽  
Fuel Reprocessing

I-129 is a very long-lived radionuclide that is released to an off-gas stream when spent fuels are dissolved at a reprocessing plant. An iodine filter can capture I-129 in the form of AgI. However, because AgI is unstable under the reducing conditions of a geological repository and I-129 has a very long half-life, I-129 can migrate to the biosphere. These characteristics make I-129 a key radionuclide for the safety assessment of a geological disposal of radioactive wastes generated from a reprocessing plant (TRU wastes). To improve disposal safety, several new waste forms have been developed to confine I-129 for a very long period in order to reduce the leaching of I-129 from radioactive wastes. These new waste forms have technical objectives of solidifying more than 95% of I-129 into the waste form and achieving a leaching rate of less than 10-5/y. Several iodine immobilization techniques have been examined. This paper presents experimental results concerning the treatment process, leaching behavior, modeling, and related elements of these immobilization techniques.

scholarly journals Synroc development—Past and present applications

2017 ◽  
Vol 4 ◽  
Author(s):  
Eric R. Vance ◽  
Dorji T. Chavara ◽  
Daniel J. Gregg
Keyword(s):  
Glass Ceramic ◽  
Intermediate Level ◽  
Waste Form ◽  
Spent Fuel ◽  
Process Technology ◽  
Technology Platform ◽  
Ceramic Waste ◽  
Waste Forms ◽  
Produce Glass ◽  
Waste Loading

ABSTRACTSynroc has evolved over the last 40 years from the titanate full-ceramics developed in the late 1970s to a technology platform that can be applied to produce glass, glass–ceramic, and ceramic waste forms and where there are distinct advantages in terms of waste loading and suppressing volatile losses.A first of a kind Synroc plant for immobilizing intermediate level waste arising from Mo-99 production is currently in detailed engineering at ANSTO.Since the year 2000, Synroc has evolved from the titanate full-ceramics developed in the late 1970s to a technology platform that can be applied to produce glass, glass–ceramic, and ceramic waste forms and where there are distinct advantages in terms of waste loading and suppressing volatile losses. Furthermore recent efforts have focused strongly on waste form development for plutonium-bearing wastes in the UK, for different options for the immobilization of Idaho calcines and most recently developing an engineered waste form for the intermediate level wastes arising from 99Mo production, for the Australian Nuclear Science and Technology Organisation (ANSTO). A variety of other studies are currently in progress, including engineered waste forms for spent fuel and investigating the proliferation risks for titanate-based waste forms containing highly enriched uranium or plutonium. This paper also attempts to give some perspective on Synroc waste forms and process technology development in the nuclear waste management industry.

scholarly journals Microstructure and Leaching Characteristics of a Technetium Containing Metal Waste Form

1999 ◽  
Vol 556 ◽  
Author(s):  
S. G. Johnson ◽  
D. D. Keiser ◽  
M. Noy ◽  
T. O'Holleran ◽  
S. M. Frank
Keyword(s):  
Stainless Steel ◽  
National Laboratory ◽  
Argonne National Laboratory ◽  
Fission Products ◽  
Point Of View ◽  
Waste Form ◽  
Nominal Composition ◽  
Spent Fuel ◽  
Waste Forms ◽  
Metal Waste

AbstractArgonne National Laboratory is developing an electrometallurgical treatment for spent fuel from the experimental breeder reactor II. A product of this treatment process is a metal waste form that incorporates the stainless steel cladding hulls, zirconium from the fuel and the fission products that are noble to the process, i.e., Tc, Ru, Pd, Rh, Ag. The nominal composition of this waste form is stainless steel/15 wt% zirconium/ 1–4 wt% noble metal fission products. The behavior of technetium is of particular importance from a disposal point of view for this waste form due to its long half life, 2.14E5 years, and its mobility in groundwater. To address these concerns a limited number of spiked metal waste forms were produced containing Tc. These surrogate waste forms were then studied using scanning electron microscopy (SEM) and selected leaching tests.

Host Phases for Actinide Elements in the Metallic Waste Form

2002 ◽  
Vol 757 ◽  
Author(s):  
D. E. Janney
Keyword(s):  
Stainless Steel ◽  
Electron Microscope ◽  
Electron Diffraction ◽  
Transmission Electron Microscope ◽  
Waste Form ◽  
Dissolution Behavior ◽  
Release Rates ◽  
Waste Forms ◽  
Transmission Electron ◽  
Simulated Waste

ABSTRACTArgonne National Laboratory has developed an electrometallurgical process for conditioning spent sodium-bonded metallic reactor fuel prior to disposal. A waste stream from this process consists of stainless steel cladding hulls that contain undissolved metal fission products such as Tc, Ru, Rh, Pd, and Ag; a small amount of undissolved actinides (U, Np, Pu) also remains with the hulls. These wastes will be immobilized in a waste form whose baseline composition is stainless steel alloyed with 15 wt% Zr (SS-15Zr). Scanning electron microscope (SEM) observations of simulated metal waste forms (SS-15Zr with up to 11 wt% actinides) show eutectic intergrowths of Fe-Zr-Cr-Ni intermetallic phases with steels. The actinide elements are almost entirely in the intermetallics, where they occur in concentrations ranging from 1–20 at%. Neutron- and electron-diffraction studies of the simulated waste forms show materials with structures similar to those of Fe2Zr and Fe23Zr6.Dissolution experiments on simulated waste forms show that normalized release rates of U, Np, and Pu differ from each other and from release rates of other elements in the sample, and that release rates for U exceed those for any other element (including Fe). This paper uses transmission electron microscope (TEM) observations and results from energy-dispersive X-ray spectroscopy (EDX) and selected-area electron-diffraction (SAED) to characterize relationships between structural and chemical data and understand possible reasons for the observed dissolution behavior.Transmission electron microscope observations of simulated waste form samples with compositions SS-15Zr-2Np, SS-15Zr-5U, SS-15Zr-11U-0.6Rh-0.3Tc-0.2Pd, and SS-15Zr-10Pu suggest that the major actinide-bearing phase in all of the samples has a structure similar to that of the C15 (cubic, MgCu2-type) polymorph of Fe2Zr, and that materials with this structure exhibit significant variability in chemical compositions. Material whose structure is similar to that of the C36 (dihexagonal, MgNi2-type) polymorph of Fe2Zr was also observed, and it exhibits less chemical variability than that displayed by material with the C15 structure. The TEM data also demonstrate a range of actinide concentrations in materials with the Fe23Zr6 (cubic, Mn23Th6-type) structure.Microstructures similar to those produced during experimental deformation of Fe-10 at% Zr alloys were observed in intermetallic materials in all of the simulated waste form samples. Stacking faults and associated dislocations are common in samples with U, but rarely observed in those with Np and Pu, while twins occurred in all samples. The observed differences in dissolution behavior between samples with different actinides may be related to increased defect-assisted dissolution in samples with U.

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