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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Effects of surface initial condition on aqueous corrosion of glass-A study with a model nuclear waste glass

Being a nonequilibrium material, the structure of glass varies with the sample history. Thus, the initial surface condition of a glass can vary with the preparation condition and have a large impact on its reactivity. This paper shows that the aqueous corrosion behavior of international simple glass (ISG) varies depending on the initial surface state. The ISG glass samples were prepared as-polished-only and polished-then-annealed and they were immersed in aqueous solution saturated with soluble SiO 2 at 30°C (modeling a mild condition) and at 90°C (modeling a severe condition). Molecular dynamics simulations were performed to obtain coordination numbers of network formers of ISG to assist oxygen speciation calculations. The surface structures of as-prepared and corroded ISG samples were analyzed using various imaging and spectroscopic techniques. Among these analyses, only the oxygen speciation with x-ray photoelectron spectroscopy showed discernable differences between two uncorroded surfaces with different preparation histories; all other methods could not differentiate the surface preparation history before aqueous corrosion. Such minor difference in chemical structures was found to have a profound impact on corrosion behaviors in the mild condition. In the harsh condition, the surface history dependence was not as drastic as the corrosion in the mild condition. The analysis results of the corroded surfaces suggested that the thickness and structure of the alteration layer formed on ISG in aqueous corrosion can vary with the initial surface state.

nuclear, defects, corrosion↗
DOE OSTI2017

The Use of Positrons to Survey Alteration Layers on Synthetic Nuclear Waste Glasses

In order to safeguard society and the environment, understanding radioactive waste glass alteration mechanisms in interactions with solutions and near-field materials, such as Fe, is essential to nuclear waste repository performance assessments. Alteration products are formed at the surface of glasses after reaction with solution. In this study, glass altered in the presence of Fe0 in aqueous solution formed two alteration layers: one embedded with Fe closer to the surface and one without Fe found deeper in the sample. Both layers were found to be thinner than the alteration layer found in glass altered in aqueous solution only. For the first time, Doppler Broadening Positron Annihilation Spectroscopy (DB-PAS) is used to non-destructively characterize the pore structures of glass altered in the presence of Fe0. Advantages and disadvantages of DB-PAS compared to other techniques used to analyze pore structures for altered glass samples are discussed. Ultimately, DB-PAS has shown to be an excellent choice for pore structure characterization for glasses with multiple alteration layers. Monte Carlo modeling predicted positron trajectories through the layers, and helped explain DB-PAS data, which showed that the deeper alteration layer without Fe had a similar composition and pore structure to layers on glass altered in water only.

Doppler Broadening Positron Annihilation Spectrosc↗
DOE OSTI2016

Nanoscale imaging of Li and B in nuclear waste glass, a comparison of ToF-SIMS, NanoSIMS, and APT: Nanoscale imaging of Li and B in nuclear waste glass

It has been very difficult to use popular elemental imaging techniques to image Li and B distribution in glass samples with nanoscale resolution. In this study, atom probe tomography (APT), time-of-flight secondary ion mass spectrometry (ToF-SIMS), and nanoscale secondary ion mass spectrometry (NanoSIMS) were used to image the distribution of Li and B in two representative glass samples. APT can provide three-dimensional Li and B imaging with very high spatial resolution (≤ 2 nm). In addition, absolute quantification of Li and B is possible, though room remains to improve accuracy. However, the major drawbacks of APT include limited field of view (normally ≤ 100 × 100 × 500 nm 3 ) and poor sample compatibility. As a comparison, ToF-SIMS and NanoSIMS are sample-friendly with flexible field of view (up to 500 × 500 μm 2 and image stitching is feasible); however, lateral resolution is limited to only about 100 nm. Therefore, SIMS and APT can be regarded as complementary techniques for nanoscale imaging Li and B in glass and other novel materials.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
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 OSTI2016

Vitrified hillforts as anthropogenic analogues for nuclear waste glasses - project planning and initiation

Nuclear waste must be deposited in such a manner that it does not cause significant impact on the environment or human health. In some cases, the integrity of the repositories will need to sustain for tens to hundreds of thousands of years. In order to ensure such containment, nuclear waste is frequently converted into a very durable glass. It is fundamentally difficult, however, to assure the validity of such containment based on short-term tests alone. To date, some anthropogenic and natural volcanic glasses have been investigated for this purpose. However, glasses produced by ancient cultures for the purpose of joining rocks in stonewalls have not yet been utilized in spite of the fact that they might offer significant insight into the long-term durability of glasses in natural environments. Therefore, a project is being initiated with the scope of obtaining samples and characterizing their environment, as well as to investigate them using a suite of advanced materials characterization techniques. It will be analysed how the hillfort glasses may have been prepared, and to what extent they have altered under in-situ conditions. The ultimate goals are to obtain a better understanding of the alteration behaviour of nuclear waste glasses and its compositional dependence, and thus to improve and validate models for nuclear waste glass corrosion. The paper deals with project planning and initiation, and also presents some early findings on fusion of amphibolite and on the process for joining the granite stones in the hillfort walls.

ageing↗
DOE OSTI2018

Structural role of ZrO 2 and its impact on properties of boroaluminosilicate nuclear waste glasses

Addition of zirconia (ZrO 2 ) to nuclear waste glasses, even in small amount, significantly affects physical properties such as chemical durability, density, viscosity, and glass transition temperature. Hence ZrO 2 plays an important role in the development of nuclear waste glass compositions. It was found recently that addition of zirconia decreases the initial dissolution rate but increases long-term dissolution by changing the protective properties such as porosity of alteration layers. In this study, the International Simple Glass (ISG) with different amounts of ZrO 2 /SiO 2 substitution was simulated using classical molecular dynamics (MD) simulations and recently developed composition-dependent potential sets. Local structural descriptors such as bond distances, bond angle distributions, and coordination numbers were systematically studied and compared with experimental values. Zr K-edge extended X-ray absorption fine structure spectra were also calculated and compared with experiment to resolve the local coordination environment around Zr. Medium-range structural information (e.g., Qn distribution, network connectivity, and ring-size distribution) showed that ZrO 2 /SiO 2 substitution increases the overall network connectivity and the amount of smaller sized rings, which will decrease the initial dissolution rate by strengthening the glass network and limiting water diffusivity. Finally, diffusion and dynamic properties of the ions were studied and discussed to develop a better understanding of the chemical durability of these glasses.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Molecular Dynamics-based Simulations of Bulk/Interfacial Structures and Diffusion Behaviors in Nuclear Waste Glasses

This NEUP Project aimed to generate accurate atomic structural models of nuclear waste glasses by using large-scale molecular dynamics-based computer simulations and to use these models to investigate self-diffusion behaviors, interfacial structures, and hydrated gel structures formed during dissolution of these glasses. The goal was to obtain realistic and accurate short and medium range structures of these complex oxide glasses, to provide a mechanistic understanding of the dissolution behaviors, and to generate reliable information with predictive power in designing nuclear waste glasses for long-term geological storage. Looking back of the research accomplishments of this project, most of the scientific goals initially proposed have been achieved through intensive research in the three and a half year period of the project. This project has also generated a wealth of scientific data and vibrant discussions with various groups through collaborations within and outside of this project. Throughout the project one book chapter and 14 peer reviewed journal publications have been generated (including one under review) and 16 presentations (including 8 invited talks) have been made to disseminate the results of this project in national and international conference. Furthermore, this project has trained several outstanding graduate students and young researchers for future workforce in nuclear related field, especially on nuclear waste immobilization. One postdoc and four PhD students have been fully or partially supported through the project with intensive training in the field material science and engineering with expertise on glass science and nuclear waste disposal

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Ion-Exchange Interdiffusion Model with Potential Application to Long-Term Nuclear Waste Glass Performance

Ion exchange is an integral mechanism influencing the corrosion of glasses. Due to the formation of alteration layers in aqueous conditions, it is difficult to conclusively deconvolute the process of ion exchange from other processes, principally dissolution of the glass matrix. Therefore, we have developed a method to isolate alkali diffusion that involves contacting glass coupons with a solution of 6 LiCl dissolved in functionally inert dimethyl sulfoxide. Here, we employ the method at temperatures ranging from 25 to 150 °C with various glass formulations. Glass compositions include simulant nuclear waste glasses, such as SON68 and the international simple glass (ISG), glasses in which the nature of the alkali element was varied, and glasses that contained more than one alkali element. An interdiffusion model based on Fick’s second law was developed and applied to all experiments to extract diffusion coefficients. The model expands established models of interdiffusion to the case where multiple types of alkali sites are present in the glass. Activation energies for alkali ion exchange were calculated and the results are in agreement with those obtained in glass strengthening experiments but are nearly five times higher than values reported for diffusion-controlled processes in nuclear waste glass corrosion experiments. A discussion of the root causes for this apparent discrepancy is provided. The interdiffusion model derived from laboratory experiments is expected to be useful for modeling glass corrosion in a geological repository when the silicon concentration is high.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Dynamic and static corrosion of chromium-alumina refractory in simulated nuclear waste glass

Monofrax® K-3, a chromium–alumina refractory, is widely used in nuclear waste glass melters due to its high durability. However, aggressive vitrification conditions still lead to corrosion that limits melter lifespan. Here, this study investigates two key corrosion modes, subsurface and melt-line corrosion, under static and dynamic conditions, using a custom setup enabling precise control of melt velocity and temperature. Experimental results, interpreted using diffusion-limited dissolution models, show that (i) subsurface corrosion increases by approximately 10% per mm/s increase in melt velocity, while melt-line corrosion remains virtually unaffected, (ii) corrosion rate dependence on temperature is inversely proportional to melt viscosity, and (iii) glass composition affects both corrosion modes similarly, based on Cr 2 O 3 , Al 2 O 3 , and alkali contents. The experimental data also allowed the determination of diffusion coefficients of major dissolving species, which were found to be consistent between the melt-line and subsurface corrosion models, indicating their suitability for future CFD studies.

12 - MGMT OF RADIOACTIVE AND NON-RADIOACTIVE WASTE↗
DOE OSTI2024

Glass Design Using Machine Learning Property Models with Prediction Uncertainties: Nuclear Waste Glass Formulation

The United States Department of Energy is responsible for managing the legacy nuclear waste stored in underground tanks at the Hanford Site. The waste will be separately vitrified as low-activity waste and high-level waste fractions. Waste glass formulation algorithms have been traditionally developed using partial quadratic mixture property-composition models. Recently, machine learning (ML) techniques have been used to predict glass properties and discover new glass materials for nuclear waste vitrification, and these advancements can be utilized to improve waste glass composition design. In this proof-of-principle study, ML algorithms such as Gaussian process regression (GPR) were used to interpolate glass properties (e.g., viscosity, electrical conductivity, chemical durability). After selecting appropriate sets of GPR hyper-parameters for each property, an optimization program was developed to formulate glass compositions to maximize waste loading while simultaneously satisfying property within constraints. The results of the ML-based waste loadings and glass compositions were compared to those obtained using the traditional methods. Comparing to the previous glass design framework, the ML-based optimization methods offer improved glass designs and a streamlined approach to generation of optimally designed data and near real-time updates.

glass formulation, machine learning, constraints, ↗