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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Ultrashort laser pulse induced nanogratings in borosilicate glass

We report on nanogratings inscribed by repetitive femtosecond laser pulses into the bulk of borosilicate glass. The irradiation produces small nanopores (10–20 nm thick) which start to self-organize in gratings as well as elongated sheets of up to 400 nm length. A quantitative description of the grating structure and its development are obtained by a combination of focused ion beam milling, scanning electron microscopy, and small angle X-ray scattering (SAXS). The SAXS partial invariant of the thin sheets is found to correlate well with the measured optical retardance. Compared to fused silica nanogratings borosilicate glass shows a much smaller retardance due to re-annealing of pores. In addition, the nanograting period strongly deviates from the well-known λ/2n prediction. We could observe periods down to 60 nm (at an inscribing wavelength of 800 nm). This has not been observed yet in other glasses.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Nanoindentation of the pristine and irradiated forms of a sodium borosilicate glass: Insights from molecular dynamics simulations

We have carried out classical molecular dynamics simulations in order to get insight into the atomistic mechanisms of the deformation during nanoindentation of the pristine and irradiated forms of a sodium borosilicate glass. In terms of the glass hardness, we have found that the primary factor affecting the decrease of hardness after irradiation is depolymerization rather than free volume, and we argue that this is a general trend applicable to other borosilicate glasses with similar compositions. We have analyzed the changes of the short- and medium-range structures under deformation and found that the creation of oxygen triclusters is an important mechanism in order to describe the deformation of highly polymerized borosilicate glasses and is essential in the understanding of the folding of large rings under stress. We have equally found that the less polymerized glasses present a higher amount of relative densification, while the analysis of bond-breaking during the nanoindentation has showed that shear flow is more likely to appear around sodium atoms. The results provided in this study can be proven to be useful in the interpretation of experimental results.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Nanoscopic structure of borosilicate glass with additives for nuclear waste vitrification

In this report we investigated the nanoscopic structure of borosilicate glasses as a host for high-level radioactive liquid waste (HLLW) in the presence of the additives Na 2 O and CaO/ZnO with and without Li 2 O. These additives have been used to lower the glass melting point, suppress the macroscopic phase separation, and increase the chemical durability of glasses. Small-angle neutron scattering was used to elucidate the effect of the additives on the nanoscopic structure along with macro- and atomic-scale observations obtained using neutron imaging and X-ray diffraction, respectively. The borosilicate glass made without Na 2 O formed a microphase-separated structure of SiO 2 - and B 2 O 3 -rich domains approximately 100 nm in size, and the material was homogeneous at length scales up to millimeters. With the addition of increasing amounts of Na 2 O, the domain spacing decreased. Introducing CaO/ZnO additives induced inhomogeneities in the glass, such as void structures several nanometers in size, although the inhomogeneity was suppressed by the coaddition of Li 2 O. These results provide insights into the performance of host glasses for HLLW vitrification. Incorporating HLLW into glasses is likely to cause changes in the nanoscopic structure of host glasses similar to those revealed here.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

The nature of the volatile technetium species formed during vitrification of borosilicate glass

Vitrification of sodium pertechnetate into borosilicate glass was performed in air at 1100 C. A glass with a composition similar to the one developed for vitrification of the low activity waste at the Hanford site was used. A red volatile species was observed above 600° C. The extended X-ray absorption fine structure results indicate the environment of the absorbing Tc atom consists of 2.9(6) O atoms at 1.73(2) A° , 2.2(4) O atoms at 2.02(2) A° , and 0.8(2) O atoms at 2.18(2) A° . The results are consistent with the presence of a mononuclear species with a structure closely related to TcO 3 (OH)(H 2 O) 2 .

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

On the effect of Al on alumino-borosilicate glass chemical durability

The chemical durability of borosilicate glass used to confine nuclear wastes is known to vary nonlinearly with their composition, making glass dissolution rate predictions difficult. Here, we focus on the effect of Al, an important oxide of these materials. The initial and residual glass dissolution rates were investigated through experiments conducted at 90 °C and pH 9. Our results show that low Al content glasses dissolve initially faster than glasses with higher Al content, but quickly achieve a lower residual rate due to the rapid formation of a more passivating gel. Nevertheless, the high Al content gel will eventually achieve passivation with a slower reorganization. The strengthening effect of Al on the Si-O bond hydrolysis will result in more stable gels, suggesting that slightly higher Al content in the gel will improve nuclear high-level waste glass durability in geological disposal conditions.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Investigating the effect of V{sub 2}O{sub 5} addition on sodium barium borosilicate glasses

V{sub 2}O{sub 5} doped sodium barium borosilicate glasses were characterized by photoluminescence spectroscopy and electron probe microanalyzer (EPMA). The glass remains homogeneous for lower concentration of V{sub 2}O{sub 5} but a phase separation is observed when V{sub 2}O{sub 5} doping is increased beyond 5 mol%. Detailed microanalysis reveals that the phase separated glass consists of a phase containing V, Ba and Si and a separate Si rich phase within the glass matrix. The luminescence study demonstrated that at low concentration the vanadium mainly interacts with the structural units of B/Si while at higher concentrations, V-O-V/ V-O{sup −} Na{sup +}/Ba{sup 2+} linkages are formed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2013

Sedimentation behavior of noble metal particles in simulated high-level waste borosilicate glasses

Solubility of noble metal elements (NME) in the melted borosilicate glass is much smaller than its normal concentration of the high level liquid waste. Thus most of NME show small particles in the melted glass and tend to sediment in the bottom region of the vitrification melter due to their higher density than that of glass. Experiments of the sedimentation of NME particles in the melted glass were carried out under static condition. Three conditions of initial NME concentration (1.1, 3.0, 6.1 wt % with an equivalent for each oxide) in the simulated glass were set and held at 1100 C. degrees up to 2880 hours. The specimen with 1.1 wt % initial NME concentration indicated zone settling, and the settling rate of the interface is constant: 2.4 mm/h. This sedimentation behavior is the type of rapid settling. Following the rapid settling, the settling rate goes gradually slower; this is the type of compressive settling. The specimens with 3.0 wt % and 6.1 wt % initial NME concentration showed compression settling from the beginning. From the settling curve of the interface, the maximum concentration of NME in sediment was estimated to be around 23- 26 wt %. Growth of NME particles was observed by holding at 1100 C. degrees for up to 2880 hours. The viscosity becomes higher as NME concentration increases and the dependence on shear rate becomes simultaneously stronger. The effect of the particle growth to viscosity appears to be not significant.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Erbium-doped borosilicate glasses containing various amounts of P{sub 2}O{sub 5} and Al{sub 2}O{sub 3}: Influence of the silica content on the structure and thermal, physical, optical and luminescence properties

Highlights: • Er{sup 3+} doped borosilicate glasses were processed with different compositions and characterizations. • An increase in the SiO{sub 2} content leads to a silicate-rich environment around the Er{sup 3+} site. • An increase in the SiO{sub 2} content decreases the Er{sup 3+} absorption cross-section at 980 nm. • Glasses with 60 mol% of SiO{sub 2} exhibit a stronger emission intensity at 1530 nm than glasses with x = 50. • Highest 1.5 μm emission intensity was achieved for the Al and P containing glass with 60 mol% of SiO{sub 2}. - Abstract: The influence of the silica content on several properties of Er-doped borosilicate glasses in the presence of various amounts of P{sub 2}O{sub 5} and Al{sub 2}O{sub 3} has been investigated. The introduction of P{sub 2}O{sub 5} and/or Al{sub 2}O{sub 3} are responsible for structural modifications in the glass network through a charge-compensation mechanism related to the formation of negatively-charged PO{sub 4} and AlO{sub 4} groups or through the formation of AlPO{sub 4}-like structural units. In this paper, we show that an increase in the SiO{sub 2} content leads to a silicate-rich environment around the Er{sup 3+} site, resulting in an increased dependence of the Er{sup 3+} ions optical and luminescence properties on the P{sub 2}O{sub 5} and/or Al{sub 2}O{sub 3} concentration. The highest emission intensity at 1.5 μm was achieved for the glass with an equal proportion of P and Al in the glass system with 60 mol% of SiO{sub 2}.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Glass transition and crystallization kinetics of a barium borosilicate glass by a non-isothermal method

The glass transition and crystallization kinetics of a glass with a molar composition 60BaO-30B{sub 2}O{sub 3}-10SiO{sub 2} were investigated by differential scanning calorimetry (DSC) under non-isothermal conditions. DSC curves exhibited an endothermic peak associated with the glass transition and two partially overlapped exothermic peaks associated with the crystallization of the glass. The dependence of the glass transition temperature (T{sub g}) and of the maximum crystallization temperature (T{sub p}) on the heating rate was used to determine the activation energy associated with the glass transition (E{sub g}), the activation energy for crystallization (E{sub c}), and the Avrami exponent (n). X-ray diffraction (XRD) revealed that barium borate (β-BaB{sub 2}O{sub 4}) was the first crystalline phase to be formed followed by the formation of barium silicate (Ba{sub 5}Si{sub 8}O{sub 21}). The variations of activation energy for crystallization and of Avrami exponent with the fraction of crystallization (χ) were also examined. When the crystallization fraction (χ) increased from 0.1 to 0.9, the value of local activation energy (E{sub c}(χ)) decreased from 554 to 458 kJ/mol for the first exothermic peak and from 1104 to 831 kJ/mol for the second exothermic peak. The value determined for the Avrami exponent was near 2 indicating a similar one-dimensional crystallization mechanism for both crystalline phases. This was confirmed by the morphological studies performed by scanning electron microscopy (SEM) on glass samples heat-treated at the first and at the second crystallization temperatures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

A comparative study of the effectiveness of empirical potentials for molecular dynamics simulations of borosilicate glasses

Despite their practical importance, atomistic modeling of B 2 O 3 containing glasses have been challenging due to the lack of reliable empirical potentials. Fortunately, a few recent developments have shown promises to simulate these glasses where the boron coordination has complex and non-linear dependence on glass composition. This work aims to provide an evaluation of the effectiveness of three recently developed potentials by a systematic study of a series (~20) of sodium borosilicate glasses with constant K (ratio of [SiO 2 ]/[B 2 O 3 ]) =2 and varying R (ratio of [Na 2 O]/[B 2 O 3 ] ranging from 0.1 to 4) values and several sodium boroaluminosilicate glasses. A comparative assessment was established on the basis of the short- and medium-range structure features, such as boron N 4 values, total correlation functions, bond angle distribution, oxygen speciation, and mechanical properties using experimental or well-established models as criteria. Furthermore, this work provides insights on the choices of empirical potentials for MD simulations of borosilicate glasses and gives directions of future potential development and refining.

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

Multiscale Investigation of the Mechanisms Controlling the Corrosion of Borosilicate Glasses in Hyper-Alkaline Media

The overarching goal of the present multiscale investigation is to unearth the kinetics and mechanisms of corrosion of borosilicate glasses in hyper-alkaline (pH = 13) environments as a function of their chemical composition. Accordingly, a series of 3- to 6-component borosilicate glasses have been designed starting from Na 2 O–B 2 O 3 –SiO 2 ternary, wherein the compositional complexity has been added in a systematic tiered approach, finally resulting in the composition of the well-known international simple glass (ISG). Tetramethylammonium hydroxide (TMAH), one of the most widely used alkaline etchant in the glass and electronics industry, has been used as the corrosion media. A series of state-of-the-art characterization techniques including magic angle spinning nuclear magnetic resonance spectroscopy, X-ray photoelectron spectroscopy, inductively coupled plasma optical emission spectroscopy, elastic recoil detection analysis, and high-resolution transmission electron microscopy have been employed to unearth the compositional dependence of glass corrosion in hyper-alkaline environments. The glass compositions underwent congruent corrosion in the forward rate regime, whereas the controlling mechanism of corrosion in the residual rate regime depends on the presence/absence of Ca in the surrounding environment and can be explained on the basis of the dissolution–reprecipitation model. The dependence of corrosion kinetics and the chemistry of alteration products (in the residual rate regime) on the glass composition have been discussed. Here, the results presented in this contribution will ultimately supplement the scientific literature attempting to understand the fundamental science governing the aqueous corrosion of silicate-based glass chemistries and add to the growing database required to develop non-empirical predictive models for designing glasses with controlled dissolution rates.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

Incorporation of Fines and Noble Metals into HLW Borosilicate Glass: Industrial Responses to a Challenging Issue - 13056

During the early stages of spent fuel reprocessing, the fuel rods are cut and dissolved to separate the solid metallic parts of the rods (cladding and end pieces) from the radioactive nitric acid solution containing uranium, plutonium, minor actinides and fission products (FP). This solution contains small, solid particles produced during the shearing process. These small particles, known as 'fines', are then separated from the liquid by centrifugation. At the La Hague plant in France, the fines solution is transferred to the vitrification facilities to be incorporated into borosilicate glass along with the highly radioactive FP solution. These fines are also composed of Zr, Mo and other noble metals (i.e. Ru, Pd, Rh, etc.) that are added before vitrification to the the FP solution that already contained noble metals. As noble metals has the potential to modify the glass properties (including viscosity, electrical conductivity, etc.) and to be affected by sedimentation inside the melter, their behavior in borosilicate glass has been studied in depth over the years by the AREVA and CEA teams which are now working together in the Joint Vitrification Laboratory (LCV). At La Hague, the R7 vitrification facility started operation in 1989 using induction-heated metallic melter technology and was quickly followed by the T7 vitrification facility in 1992. Incorporating the fines into glass has been a challenge since operation began, and has given rise to several R and D studies resulting in a number of technological enhancements to improve the mixing capability of the melters (multiple bubbling technology and mechanical stirring in the mid-90's). Nowadays, the incorporation of fines into R7T7 glass is well understood and process adaptations are deployed in the La Hague facilities to increase the operating flexibility of the melters. The paper will briefly describe the fines production mechanisms, give details of the resulting fines characteristics, explain how the metallic particles can influence the glass properties and challenge vitrification technologies and finally, give a rundown of the R and D efforts which have produced innovative solutions contributing to the operational excellence of AREVA's vitrification facilities in the La Hague reprocessing plant. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

Spherical gold nanoparticles and SiO{sub 2}/Au core/shell microparticles under intense femtosecond laser excitation: relaxation dynamics of gold nanoparticles and nanostructuring of borosilicate glass using SiO{sub 2}/Au microparticles

This paper reports surface nanostructuring of borosilicate glass covered with a water layer and the production of ∼150 nm diameter pits using SiO{sub 2}/Au core/shell microparticles under excitation with 50 fs pulses (λ = 780 nm) using the optical scheme of an inverted microscope with a 100{sup ×}, NA = 1.4 objective. We compare the thresholds for hole formation in glass with the use of SiO{sub 2}/Au and uncoated SiO{sub 2} microparticles. The threshold is 0.7 J cm{sup -2} for SiO{sub 2}/Au and 2.9 J cm{sup -2} for SiO{sub 2} microparticles, which coincides with the threshold for nanostructuring by a focused femtosecond pulse without microparticles: 3 J cm{sup -2}. Femtosecond pump – probe spectroscopy has been used to study the relaxation dynamics of laser pulse energy absorbed in a Au nanoparticle and the dynamics of energy dissipation to the ambient medium. The threshold for cavitation bubble formation in water with SiO{sub 2}/Au has been determined to be 0.06 mJ cm{sup -2}, which is a factor of 30 lower than the bubble formation threshold in the case of uncoated SiO{sub 2} microparticles. (nanostructures)

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2012

Interaction of Embedded TRISO Particles with Melt of Alkaline Borosilicate Glass (ABG) - 12008

Spent tri-isotropic (TRISO) fuel particles are a high-level waste contained within a graphite compact/pebble, which is an intermediate-level waste. In this research, the particles were extracted from their graphite matrix with a use of aqueous HNO{sub 3}/H{sub 2}SO{sub 4} solution. The intercalation process produced three types of particles with different thickness of outer layers. The damage to the outer layers of TRISO particles can cause an undesirable release of fission products from the kernel of the particle. Alkaline borosilicate glass (ABG) was used as an encapsulating matrix in order to prevent the release of fission products from kernels. The aim of the research is to investigate an interaction of embedded TRISO particles with Melt of Alkaline Borosilicate Glass (ABG), and elucidate a chemical bonding and an interface formation between them. Particular emphasis was placed on the analysis of the intermediate chemical phase at the interface SiC/ABG as a function of the material impurity and thickness of the SiC layer. The findings revealed that there is a strong wetting angle between the SiC layer and the ABG and it can completely diminish the layer. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Effects of He Ion Irradiation in Simple Borosilicate Glasses for HLW Immobilisation - 20324

High-level radioactive waste (HLW) consists of fission products and minor actinides. Borosilicate glass is the host material of choice in most countries to safely immobilize HLW, followed by eventual geological disposal. HLW glasses will experience both self-heating and self-irradiation effects due to the decay of fission products and minor actinides present therein. During the first 500 years of geological disposal, beta-gamma decay will be the main source of radiation due to short half-lives of fission products, as compared to very long-lived actinides which will be responsible for irradiation over much longer timescales. High-energy alpha particles and alpha recoil nuclei can potentially have significant impact (stored energy, volume change, accumulated dose, chemical durability) on the performance of the wasteform over longer timescales. Thus, to ensure safe and economic disposal over geological periods (10{sup 4} - 10{sup 6} years), the assessment of performance and properties in terms of radiation effects becomes indispensable. This work aims to simulate the effects of alpha decay in radioactive waste glasses. Two international glasses, namely UK 'MW' lithium-sodium borosilicate and Indian sodium-barium borosilicate, which are being used as HLW immobilization matrices by the UK and India respectively, were prepared by a melt-quench method and annealed below their glass transition temperatures. Both glasses were irradiated with 650 KeV He{sup 2+} ions with doses ranging from 10{sup 15} to 10{sup 17} ions/cm{sup 2}. Structural analysis was carried out using electron paramagnetic resonance (EPR) and Raman spectroscopies. First derivative continuous wave EPR spectra were recorded for all pristine and irradiated glass monoliths at room temperature using an X-band (frequency 9.6 GHz) EPR Bruker spectrometer. Results from EPR analyses showed the formation of irradiation induced paramagnetic centers at g ∼ 2.00 in all irradiated glasses. Raman spectra of pristine and irradiated samples were acquired, and showed notable changes in glass structure post-irradiation, with the emergence of a broad Raman band at 1560 cm{sup -1} upon irradiation with high fluences. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRS1979

Thermally stimulated conductivity studies of trapping centers in alkali-borosilicate glasses

Thermally stimulated conductivity studies have been performed on unirradiated borosilicate glasses made to contain various amounts of sodium, lithium, nickel, and iron oxides. Measurements were made between 77 and 570 K. All the samples gave one or more conductivity peaks below room temperature. Analysis of the initial-rise slope of the conductivity peaks of the various samples gave trapping-level energies ranging from 0.1 to 1.9 eV. The shape and temperature of the maximum of most of the peaks changed on each measurement cycle. A few samples exhibited a common peak that formed on annealing.

Catchings, R. M.↗