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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Enhanced 99 Tc retention in glass waste form using Tc(IV)-incorporated Fe minerals

Technetium (99Tc) immobilization by doping into iron oxide mineral phases may alleviate the problems with Tc volatility during vitrification of nuclear waste. Reduced Tc, Tc(IV), substitutes for Fe(III) in the crystal structure by a process of Tc reduction from Tc(VII) to Tc(IV) followed by co-precipitation of Fe oxide minerals. Two Tc-incorporated Fe minerals (Tc-goethite and Tc-magnetite/maghemite) were prepared and tested for Tc retention in glass melt samples at temperatures between 600 – 1,000 oC. After being cooled, the solid glass specimens prepared at different temperatures were analyzed for Tc oxidation state using Tc K-edge XANES. In most samples, Tc was partially oxidized from Tc(IV) to Tc(VII) as the melt temperature increased. However, Tc retention in glass melt samples prepared using Tc-incorporated Fe minerals were moderately higher than in glass prepared using KTcO4 because of limited and delayed Tc volatilization.

Um, Wooyong↗
DOE OSTI2022

Effect of zeolite type, temperature, and pH on Stage III glass alteration behavior for two nuclear waste glasses

We report long-term laboratory scale static alteration tests (up to 1500 d) were conducted on two low-activity waste glasses (LAWA44 and IDF18-A161) at S/V = 2000 m –1 . Tests were seeded with either analcime, clinoptilolite, zeolite P1, or zeolite P2 to induce Stage III glass alteration behavior. The effect of several parameters on glass Stage III behavior was studied with consideration of several variables, including temperature (22 °C – 90 °C) and pH (floating or initially set using KOH at values from 9.5 to 11.5). Temporal solution data and solids characterization at the end of the experiments are reported. Solution data demonstrated the occurrence of a sustained rate acceleration at temperatures down to 40 °C and the activation energy for these Stage III rates was determined for both glasses. Three major secondary phases were identified at the end of the experiments for both glasses: zeolite P1, zeolite P2, and/or analcime (along with minor phases: zeolites, clays, carbonates). The identification of the crystalline phases at the end of the experiment often differed from the zeolite seed phase. In addition, the use of the Avrami equation showed unimpeded zeolite growth (3-dimensional) in certain conditions, suggesting that in certain conditions the glass dissolution rate is controlled by zeolite formation kinetics whereas in other conditions the glass corrosion process impeded zeolite formation kinetics. The morphological evolution of the samples revealed the growth of the zeolites which completely fill the intergranular space in the powder bed. These results are discussed with regards to previous seeded and unseeded Stage III dissolution rate experiments performed on low- and high-activity nuclear waste glasses.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Nepheline crystallization and the residual glass composition: Understanding waste glass durability

The vast majority of High-Level Waste (HLW) originating from defense nuclear programs is sequestered and immobilized in borosilicate glass. Borosilicate glass is universally accepted for immobilizing HLW, but its efficiency has limitations based on the compositional makeup of the waste stream. The chemical durability of the glass is the most important factor in determining the longevity and usefulness of the final glass waste form. The primary detriment to this durability in glasses containing high levels of aluminum is nepheline (NaAlSiO 4 ) crystallization, as it is generally accompanied by a measurable decrease in the glass's chemical durability. This work seeks to understand nepheline crystallization, within the context of thermal history, and to elucidate the influence of compositional shifts in the residual glass (after crystallization) on the measured durability. The results presented within show a distinct deviation in leaching behavior as a function of structural makeup (calculated Q units). This understanding will provide practical information required for broadening glass compositional regions needed to more efficiently vitrify HLW.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Silane Modification of Glass and Silica Surfaces to Obtain Equally Oil-Wet Surfaces in Glass-Covered Silicon Micromodel Applications

The wettability of silicon and glass surfaces can be modified by silanization. However, similar treatments of glass and silica surfaces using the same silane do not necessarily yield the same wettability as determined by the oil-water contact angle. In this technical note, surface cleaning pretreatments were investigated to determine conditions that would yield oil-wet surfaces on glass with similar wettability to silica surfaces treated with the same silane, and both air-water and oil-water contact angles were determined. Air-water contact angles were less sensitive to differences between silanized silica and glass surfaces, often yielding similar values while the oil-water contact angles were quite different. Borosilicate glass surfaces cleaned with standard cleaning solution 1 (SC1) yield intermediate-wet surfaces when silanized with hexamethyldisilazane, while the same cleaning and silanization yields oil-wet surfaces on silica. However, cleaning glass in boiling concentrated nitric acid creates a surface that can be silanized to obtain oil-wet surfaces using HDMS. Moreover, this method is effective on glass with prior thermal treatment at an elevated temperature of 400oC. In this way, silica and glass can be silanized to obtain equally oil-wet surfaces using HMDS. It is demonstrated that pretreatment and silanization is feasible in silicon-silica/glass micromodels previously assembled by anodic bonding, and that the change in wettability has a significant observable effect on immiscisble fluid displacements in the pore network.

contact angle↗
DOE OSTI2014

Structure of Cu{sub 64.5}Zr{sub 35.5} metallic glass by reverse Monte Carlo simulations

Reverse Monte Carlo simulations (RMC) have been widely used to generate three dimensional (3D) atomistic models for glass systems. To examine the reliability of the method for metallic glass, we use RMC to predict the atomic configurations of a “known” structure from molecular dynamics (MD) simulations, and then compare the structure obtained from the RMC with the target structure from MD. We show that when the structure factors and partial pair correlation functions from the MD simulations are used as inputs for RMC simulations, the 3D atomistic structure of the glass obtained from the RMC gives the short- and medium-range order in good agreement with those from the target structure by the MD simulation. These results suggest that 3D atomistic structure model of the metallic glass alloys can be reasonably well reproduced by RMC method with a proper choice of input constraints.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Time-resolved measurement of photon emission during fast crack propagation in three-point bending fracture of silica glass and soda lime glass

Simultaneous time-resolved measurements of photon emission (PE) and fast crack propagation upon bending fracture were conducted in silica glass and soda lime glass. Observation of fracture surfaces revealed that macroscopic crack propagation behavior was similar between the silica glass and soda lime glass when fracture loads for these specimens were comparable and cracks propagated without branching. However, a large difference in the PE characteristics was found between the two glasses. In silica glass, PE (645–655 nm) was observed during the entire crack propagation process, whereas intense PE (430–490 nm and 500–600 nm) was observed during the initial stages of propagation. In contrast, only weak PE was detected in soda lime glass. These results show that there is a large difference in the atomic processes involved in fast crack propagation between these glasses, and that PE can be used to study brittle fracture on the atomic scale.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Orientational anisotropy in simulated vapor-deposited molecular glasses

Enhanced kinetic stability of vapor-deposited glasses has been established for a variety of glass organic formers. Several recent reports indicate that vapor-deposited glasses can be orientationally anisotropic. In this work, we present results of extensive molecular simulations that mimic a number of features of the experimental vapor deposition process. The simulations are performed on a generic coarse-grained model and an all-atom representation of N,N′-bis(3-methylphenyl)-N,N′-diphenylbenzidine (TPD), a small organic molecule whose vapor-deposited glasses exhibit considerable orientational anisotropy. The coarse-grained model adopted here is found to reproduce several key aspects reported in experiments. In particular, the molecular orientation of vapor-deposited glasses is observed to depend on substrate temperature during deposition. For a fixed deposition rate, the molecular orientation in the glasses changes from isotropic, at the glass transition temperature, T{sub g}, to slightly normal to the substrate at temperatures just below T{sub g}. Well below T{sub g}, molecular orientation becomes predominantly parallel to the substrate. The all-atom model is used to confirm some of the equilibrium structural features of TPD interfaces that arise above the glass transition temperature. We discuss a mechanism based on distinct orientations observed at equilibrium near the surface of the film, which get trapped within the film during the non-equilibrium process of vapor deposition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

High-precision measurements of the compressibility and the electrical resistivity of bulk g-As{sub 2}Te{sub 3} glasses at a hydrostatic pressure up to 8.5 GPa

High-precision studies of the volume and the electrical resistivity of g-As{sub 2}Te{sub 3} glasses at a high hydrostatic pressure up to 8.5 GPa at room temperature are performed. The glasses exhibit elastic behavior in compression only at a pressure up to 1 GPa, and a diffuse structural transformation and inelastic density relaxation (logarithmic in time) begin at higher pressures. When the pressure increases further, the relaxation rate passes through a sharp maximum at 2.5 GPa, which is accompanied by softening the relaxing bulk modulus, and then decreases, being noticeable up to the maximum pressure. When pressure is relieved, an unusual inflection point is observed in the baric dependence of the bulk modulus near 4 GPa. The polyamorphic transformation is only partly reversible and the residual densification after pressure release is 2%. In compression, the electrical resistivity of the g-As{sub 2}Te{sub 3} glasses decreases exponentially with increasing pressure (at a pressure up to 2 GPa); then, it decreases faster by almost three orders of magnitude in the pressure range 2–3.5 GPa. At a pressure of 5 GPa, the electrical resistivity reaches 10{sup –3} Ω cm, which is characteristic of a metallic state; this resistivity continues to decrease with increasing pressure and reaches 1.7 × 10{sup –4} Ω cm at 8.1 GPa. The reverse metal–semiconductor transition occurs at a pressure of 3 GPa when pressure is relieved. When the pressure is decreased to atmospheric pressure, the electrical resistivity of the glasses is below the initial pressure by two–three orders of magnitude. Under normal conditions, both the volume and the electrical resistivity relax to quasi-equilibrium values in several months. Comparative structural and Raman spectroscopy investigations demonstrate that the glasses subjected to high pressure have the maximum chemical order. The glasses with a higher order have a lower electrical resistivity. The polyamorphism in the As{sub 2}Te{sub 3} glasses is caused by both structural changes and chemical ordering. The g-As{sub 2}Te{sub 3} compound is the first example of glasses, where the reversible metallization under pressure has been studied under hydrostatic conditions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Degradation of Simulated HLW Glass and International Simple Glass immersed partially in water - 16474

Water degradation of glass waste forms destined for geological disposal has been studied in a variety of conditions including of bulk glass immersed completely in static or dynamic water. During the course of repository life, the canisters may be only partially immersed in the initial stages of contact with water. Under these conditions glass degradation occurs on the glass immersed in water and on the glass above water by vapor condensation. In this work degradation of International Simple Glass (ISG) and Simulated High Level Waste Glass (HSG) is examined by immersing partially in distilled water during the course of test. Under static experimental conditions at 90 deg. C, the condensation of vapor on the ISG glass surface formed Ca-rich precipitates and pits after degrading for 1 and 3 weeks respectively. Whereas HSG precipitated Ca-rich phases predominantly after 1 week and no pits were found on the surface. When compared, HSG was found to change surface chemistry faster than ISG. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2019

The Effect of Glass Chemistry on Caesium Volatility in Iron Phosphate Glass Systems - 19344

The UK currently has a stockpile of 99,000 m{sup 3} of intermediate level waste (ILW), with this figure expected to rise to 191,000 m{sup 3} by 2125. Current immobilisation options include cementation and thermal treatment, with cementation being the preferred candidate due to the simplicity of processing. However, thermal processing such as vitrification could offer significant volume reductions, up to 75 % for some waste-streams. In comparison, cementation is generally associated with a volume increase, with a typical waste package seeing a volume increase of 200 - 400 %. For vitrification to be accepted as the preferred treatment option of ILW in the UK, the issue of volatility during the vitrification process must be addressed. Volatile components of ILW such as Cs-137 and Sr-90 account for almost 50 % of the current total radioactivity produced by the UK's ILW stockpile. Therefore, the efficient retention of these elements into the glass immobilisation medium must be considered. Various approaches can be employed when trying to increase volatile retention, however this project has focussed on the influence of glass chemistry on volatility. A series of iron phosphate glasses containing 5 mol % of B{sub 2}O{sub 3}, MnO and ZnO have been produced, where additives have been substituted in place of Fe{sub 2}O{sub 3} in a standard 40Fe{sub 2}O{sub 3}-60P{sub 2}O{sub 5} system. All glass samples were characterised using Raman spectroscopy, SEM-EDX, thermal analysis, XRD and XRF. The glasses were then doped with caesium carbonate and re-melted in the system described below. A simple off-gas system has been developed and commissioned to capture and characterise volatiles released from the glass during melting. The off-gas system has been refined several times, with the most recent design comprising of a sealed stainless steel system, connected to two gas washing bottles containing 150 ml of 50 % nitric acid. Nitrogen gas is passed through the system for the duration of the experiment at a flow rate of ∼ 0.9 L/min to ensure efficient carryover of the volatiles released from the glass melt into the solutions in the gas washing bottles. The total retention of the volatiles can be measuring by analysing the contents of the gas washing bottles using ICP-MS and XRF of the final glass product. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2019

Effects of Sulfate on Rhenium Incorporation into Low-Activity Waste Glass

Technetium-99 (99Tc) is a major radionuclide of concern in the Hanford low-activity waste (LAW), which will be vitrified into borosilicate glass at the Waste Treatment and Immobilization Plant (WTP). Sulfate content in LAW has been known to be a critical factor affecting the volatile loss of 99Tc during melting of the LAW glass feed (a mix of liquid LAW and mineral/chemical additives). We investigated rhenium (a nonradioactive surrogate for 99Tc) incorporation into glass by performing crucible melting tests of two representative simulated LAW glass feeds, each prepared with varied sulfur levels. The sulfate content varied from the original content to half of the original (½S) and to zero (0S), in the range of 0 to 0.8 mass % SO3 in glass if 100% retained. The slurry feeds were dried at 105°C and heated to 400–1100°C. Deionized water leach at room temperature and at 80°C was conducted on the dried feed and heat-treated samples to analyze the chemical compositions of soluble and insoluble phases separately and to profile the partitioning of various components into different phases during the melting process. Different partitioning behavior of rhenium, sulfate, and chlorine is discussed in connection with major feed-to-glass conversion reactions. The mechanism on how sulfate affects rhenium incorporation during feed-to-glass conversion reactions, and so final retention of rhenium in glass, is proposed based on the two hypotheses that segregated sulfate-rich phase forms during feed conversion reactions and Re preferentially partitions to this sulfate-rich phase.

Jin, Tongan↗