Detailed Processes of Surface Layer Formation in Borosilicate Waste Glass Dissolution

1984 ◽  
Vol 44 ◽  
Author(s):  
John F. Flintoff ◽  
Alan B. Harker
Keyword(s):  
Chemical Structure ◽  
Development Process ◽  
Waste Glass ◽  
Surface Layers ◽  
Glass Dissolution ◽  
Surface Spectroscopy ◽  
Local Saturation ◽  
Saturation Effects ◽  
Layer Development ◽  
Surface Layer Formation

AbstractThe morphology and chemical structure of surface layers formed during the aqueous leaching of the SRP-type borosilicate waste glass in simulated ground waters have been studied by SEM/EDXS, XRD, and surface spectroscopy. Comparison of layers formed in deionized, silicate, and brine waters shows the processes of both corrosion and precipitation to be highly localized. The corrosion process proceeds on the glass surface preferentially at points of stress and inhomogeneity. Crystalline and noncrystalline precipitates form in well-defined regions within the surface layers indicating the layer development process to be dominated by species migration and local saturation effects.

Surface Layer Formation on a Nuclear Waste Glass

1982 ◽  
Vol 15 ◽  
Author(s):  
Werner Lutze ◽  
GÜnter Malow ◽  
Harald Rabe ◽  
Thomas J. Headley
Keyword(s):  
Waste Glass ◽  
Layer Formation ◽  
Surface Layers ◽  
Protective Function ◽  
Leach Rate ◽  
Simulated Waste ◽  
Volcanic Glasses ◽  
The Stability ◽  
Kinetics Of ◽  
Surface Layer Formation

Surface layers are a common feature of leached surfaces of borosilicate waste glasses. Layers are also observed upon weathering of volcanic glasses[l] and of silicate minerals[2]. The question of whether these layers can protect the glass against further attack by decreasing the leach rate is stïll a subject of controversy[3]. Both in geochemical work[4] and in work on waste forms [5,6], surface layers are attributed a protective function, and the stability of leached, million years old volcanic glasses[1] may be due to the presence of palagonite, a thin (≤100 μm) alteration layer, which forms in a few years but does not seem to increase in thickness after this time. The present study investigates the effects of layer formation on leaching kinetics of a borosilicate waste glass containing 20 wt.% LWR-type simulated waste oxides.

Effect of Surface Layers on the Dissolution of Nuclear Waste Glasses

1993 ◽  
Vol 333 ◽  
Author(s):  
Shi-Ben Xing ◽  
Andrew C. Buechele ◽  
Ian L. Pegg
Keyword(s):  
Surface Layer ◽  
Nuclear Waste ◽  
Glass Composition ◽  
Reaction Rates ◽  
Surface Layers ◽  
Linear Effect ◽  
Glass Dissolution ◽  
Important Challenge ◽  
Saturation Effects ◽  
Glass Powders

ABSTRACTExplanation of the striking non-linear effect of glass composition on the aqueous dissolution represents an important challenge to existing dissolution mechanisms. Surface layers that are formed during glass dissolution may play an important role in this effect. One chemically reactive and one less-reactive nuclear waste glass (leachate concentrations differ by about a factor of 10) were reacted in deionized water. Two types of glass powders were used: Type A powders were pristine glass powders; Type B powders were the glass powders which had been reacted for 120 days to develop the surface layers. Both the solution concentrations and the surface layers were investigated. The experimental observations indicate that: (i) There is a range of glass compositions over which small differences in composition lead to large changes in both reaction rates and surface layer thickness; and (ii) The reaction rate is strongly affected by the formation of the surface layer (the layer appears to be protective) and cannot be explained in terms of saturation effects alone. The findings are contrary to the conclusion of a previous study and serve to highlight the inadequacy of existing dissolution models predicated on an overly simplistic mechanism, especially with regard to glass composition effects.

scholarly journals Chemical Durability of Glass Containing Srp Waste - Leachability Characteristics, Protective Layer Formation, and Repository System Interactions

1981 ◽  
Vol 11 ◽  
Author(s):  
George G. Wicks ◽  
Barbara M. Robnett ◽  
W. Duncan Rankin
Keyword(s):  
Protective Layer ◽  
Layer Formation ◽  
Surface Layers ◽  
Waste Products ◽  
Safety And Reliability ◽  
Experimental Findings ◽  
Nuclear Waste Forms ◽  
Leaching Models ◽  
Surface Layer Formation

Leachability is one of the most important properties of solidified nuclear waste forms because it provides information on the performance and the subsequent safety and reliability that the waste products will possess. One of the most important experimental findings in the leachability field has been the discovery and subsequent detailed characterization of protective surface layers that form on waste glass during leaching. These layers can have a beneficial effect on product performance while in storage by improving productdurability with time. As a result of surface layer formation and the effects on subsequent product leaching characteristics, new qualitative and quantitative leaching models have recently been proposed.

Mechanisms of Defense Waste Glass Dissolution

1986 ◽  
Vol 73 (2) ◽  
pp. 140-164 ◽  
Author(s):  
Aaron Barkatt ◽  
Barbara C. Gibson ◽  
Pedro B. Macedo ◽  
Charles J. Montrose ◽  
William Sousanpour ◽  
...  
Keyword(s):  
Waste Glass ◽  
Glass Dissolution

scholarly journals The initial dissolution rates of simulated UK Magnox–ThORP blend nuclear waste glass as a function of pH, temperature and waste loading

2015 ◽  
Vol 79 (6) ◽  
pp. 1529-1542 ◽  
Author(s):  
N. Cassingham ◽  
C.L. Corkhill ◽  
D.J. Backhouse ◽  
R.J. Hand ◽  
J.V. Ryan ◽  
...  
Keyword(s):  
Dissolution Kinetics ◽  
Intrinsic Rate ◽  
Waste Glass ◽  
High Level Waste ◽  
Dissolution Mechanism ◽  
Dissolution Rates ◽  
Forward Rates ◽  
Glass Dissolution ◽  
High Level ◽  
Kinetics Of

AbstractThe first comprehensive assessment of the dissolution kinetics of simulant Magnox–ThORP blended UK high-level waste glass, obtained by performing a range of single-pass flow-through experiments, is reported here. Inherent forward rates of glass dissolution were determined over a temperature range of 23 to 70°C and an alkaline pH range of 8.0 to 12.0. Linear regression techniques were applied to the TST kinetic rate law to obtain fundamental parameters necessary to model the dissolution kinetics of UK high-level waste glass (the activation energy (Ea), pH power law coefficient (η) and the intrinsic rate constant (k0)), which is of importance to the post-closure safety case for the geological disposal of vitreous products. The activation energies based on B release ranged from 55 ± 3 to 83 ± 9 kJ mol–1, indicating that Magnox–THORP blend glass dissolution has a surface-controlled mechanism, similar to that of other high-level waste simulant glass compositions such as the French SON68 and LAW in the US. Forward dissolution rates, based on Si, B and Na release, suggested that the dissolution mechanism under dilute conditions, and pH and temperature ranges of this study, was not sensitive to composition as defined by HLW-incorporation rate.

Remaining Uncertainties in Predicting Long-Term Performance of Nuclear Waste Glass From Experiments

1993 ◽  
Vol 333 ◽  
Author(s):  
B. Grambow ◽  
Kernforschungszentrum Karlsruhe
Keyword(s):  
Current Knowledge ◽  
Research Work ◽  
Waste Glass ◽  
Dissolution Mechanism ◽  
Glass Dissolution ◽  
Radionuclide Release ◽  
Long Term Performance ◽  
Term Performance ◽  
Term Maintenance

ABSTRACTThe current knowledge on the glass dissolution mechanism and the representation of glass dissolution concepts within overall repository performance assessment models are briefly summarized and uncertainties related to mechanism, radionuclide chemistry and parameters are discussed. Understanding of the major glass dissolution processes has been significantly increased in recent years. Long-term glass stability is related to the long-term maintenance of silica saturated conditions. The behavior of individual radionuclides in the presence of a dissolving glass has not been sufficiently and results do not yet allow meaningful predictions. Conservative long-term predictions of glass matrix dissolution as upper limit for radionuclide release can be made with sufficient confidence, however these estimations generally result in a situation were the barrier function of the glass is masked by the efficiency of the geologic barrier. Realistic long-term predictions may show that the borosilicate waste glass contributes to overall repository safety to a much larger extent than indicated by overconservatism. Today realistic predictions remain highly uncertain and much more research work is necessary. In particular the long-term rate under silica saturated conditions needs to be understood and the behavior of individual radionuclides in the presence of a dissolving glass deserves more systematic investigations.

Effects of Rocks and Backfill Materials on Waste Glass Leaching

1985 ◽  
Vol 50 ◽  
Author(s):  
K. Ishiguro ◽  
N. Sasaki ◽  
H. Kashihara ◽  
M. Yamamoto
Keyword(s):  
Waste Glass ◽  
Distilled Water ◽  
Leach Rate ◽  
Glass Dissolution ◽  
Crushed Granite ◽  
Backfill Materials ◽  
Long Term Experiment ◽  
Static Conditions ◽  
Glass Leaching

AbstractExtensive studies have been made on the interactions between a waste glass and repository materials under static conditions. One of the PNC reference glasses was leached in the solution prepared from water in contact with crushed granite, tuff, diabase and backfill materials such as bentonite and zeolite. The leachant solutions except for some bentonite solutions reduced the glass leach rate compared with that measured in distilled water. The extent of the reduction was a function of silicon concentration in solution. The bentonite solutions enhanced the glass dissolution rate by a factor of 2 to 3 at low bentonite/water ratios but the effect was found to be less important at high bentonite/water ratios and in the long-term experiment. Addition of granite and zeolite to the bentonite solutions decreased the leach rate below the value measured in distilled water.

scholarly journals Nanoscale Molecular Characterisation of Hair Cuticles using Integrated AFM-IR

2020 ◽  
Author(s):  
A. P. Fellows ◽  
M. T. L. Casford ◽  
P. B. Davies
Keyword(s):  
Chemical Structure ◽  
High Surface ◽  
Great Majority ◽  
Diffraction Limit ◽  
Chemical Investigation ◽  
Molecular Characterisation ◽  
Force Microscopy ◽  
Atomic Force ◽  
Surface Spectroscopy ◽  
Significant Chemical

AbstractThe nanometre-scale topography and chemical structure of hair cuticles has been investigated by vibrational spectroscopy and imaging in two spectral regions. The combination of Atomic Force Microscopy with a tuneable infrared laser (AFM-IR) circumvents the diffraction limit that has impaired traditional infrared spectroscopy, facilitating surface spectroscopy at ultra-spatial resolution. The variation in protein and lipid content of the cuticle cell surface approaching its edge, as well as the exposed layered structure of the cell at the edge itself, was investigated. Furthermore, the contribution of cystine-related products to the cuticle layers was determined. The variation of protein, lipid and cystine composition in the observed layers, as well as the measured dimensions of each, correspond closely to that of the epicuticle, A-layer, exocuticle and endocuticle layers of the cuticle cell sub-structure.Statement of SignificanceUsing AFM-IR to analyse the nanoscale cuticle features is both significant and novel in the field. Thus far, the great majority of work on the chemical investigation of the structure of hair has been limited to bulk measurements, or subject to the diffraction limit associated with traditional IR spectroscopies and microscopies. AFM-IR circumvents this diffraction limit and allows nanometre-scale, localised chemical investigation with high surface selectivity. While non-chemical investigations, e.g. those using Transmission Election Microscopy, have previously shown cuticles to have a layered substructure, AFM-IR sheds light on significant chemical variations of protein and lipid compositions within such layers, enabling their quantification.

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