Statistical Modeling and Optimization of Nuclear Waste Vitrification

Statistical Modeling and Optimization of Nuclear Waste Vitrification

Author: Todd E. Combs

Publisher:

Published: 1997-03-01

Total Pages: 175

ISBN-13: 9781423568346

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This thesis describes the development of a methodology to minimize the cost of vitrifying nuclear waste. Pacific Northwest Laboratory (PNL) regression models are used as baseline equations for modeling glass properties such as viscosity, electrical conductivity, and two types of durability. Revised PNL regression models are developed that eliminate insignificant variables from the original models. The Revised PNL regression model for electrical conductivity is shown to better predict electrical conductivity than the original PNL regression model. Neural networks are developed for viscosity and the two types of durability, PCT-B and MCC-1 B. The neural network models are shown to outperform every PNL and Revised PNL regression model in terms of predicting property values for viscosity, PCT-B, and MCC-1 B. The combined Neural Network/Revised PNL 2nd order electrical conductivity models are shown to be the best classifiers of nuclear waste glass, i.e. they have the highest probability of classifying a vitrified waste form as glass when it actually did produce glass in the laboratory. Finally, five nonlinear programs are developed with constraints containing: (1) the PNL original 1st order models, (2) the PNL original 2nd order models, (3) the Revised PNL 1st order models, (4) the Revised PNL 2nd order models, and (5) the Neural Network/Revised PNL 2nd order electrical conductivity models. The Neural Network/Revised PNL 2nd order electrical conductivity nonlinear program is shown to minimize the total expected cost of vitrifying nuclear waste glass. This nonlinear program allows DOE to minimize its risk and cost of high-level nuclear waste vitrification.


Optimization of High-level Waste Loading in a Borosilicate Glass Matrix by Using Chemical Durability Modeling Approach

Optimization of High-level Waste Loading in a Borosilicate Glass Matrix by Using Chemical Durability Modeling Approach

Author: Javeed Mohammad

Publisher:

Published: 2002

Total Pages:

ISBN-13:

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A laboratory scale study was carried out on a set of 6 borosilicate waste glasses made from simulated high-level nuclear waste. The test matrix was designed to explore the composition region suitable for the long-term geologic disposal of high-temperature-and high-waste-containing glasses. The glass compositions were selected to achieve maximum waste loading without a sacrifice in glass durability. The relationship between glass composition and chemical durability was examined. The qualitative effect of increasing B2O3 content on the overall waste glass leaching behavior has also been addressed. The glass composition matrix was designed by systematically varying the factors: %waste loading and (SiO2+Frit):B2O3 ratio, with (SiO2:Frit) ratio being held constant. In order to assess the chemical durability, the Product Consistency Test (ASTM C-1285) was performed. Under PCT protocol, crushed glass was allowed to react with ASTM type I water under static conditions. All leachate solutions were analyzed by the technique; Inductively Coupled Plasma-Atomic Emission Spectroscopy (ICP-AES). A statistical regression technique was utilized to model the normalized release of the major soluble elements, Na, Si, and B, as a function of the individual as well as interactive chemical effects (B2O3, Al2O3, Fe2O3, MnO, SiO2, SrO, Na2O, B2O3*SiO2, B2O3*Al2O3, Fe2O3*Na2O, Al2O3*Na2O, and MnO*SiO2). Geochemical modeling was performed using the computer code EQ3/6 to: (1) determine the saturation states of the possible silicate minerals, a-cristobalite and chalcedony; and (2) predict the most stable mineral phase based on the mineral thermodynamic data. Mineral/water interactions were analyzed by representing the resultant glass data on a Na-Al-Si-O-H stability diagram.


OPTIMIZATION OF HIGH-LEVEL WASTE LOADING IN A BOROSILICATE GLASS MATRIX BY USING CHEMICAL DURABILITY MODELING APPROACH.

OPTIMIZATION OF HIGH-LEVEL WASTE LOADING IN A BOROSILICATE GLASS MATRIX BY USING CHEMICAL DURABILITY MODELING APPROACH.

Author:

Publisher:

Published: 2002

Total Pages:

ISBN-13:

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A laboratory scale study was carried out on a set of 6 borosilicate waste glasses made from simulated high-level nuclear waste. The test matrix was designed to explore the composition region suitable for the long-term geologic disposal of high-temperature-and high-waste-containing glasses. The glass compositions were selected to achieve maximum waste loading without a sacrifice in glass durability. The relationship between glass composition and chemical durability was examined. The qualitative effect of increasing B2O3 content on the overall waste glass leaching behavior has also been addressed. The glass composition matrix was designed by systematically varying the factors: %waste loading and (SiO2+Frit):B2O3 ratio, with (SiO2:Frit) ratio being held constant. In order to assess the chemical durability, the Product Consistency Test (ASTM C-1285) was performed. Under PCT protocol, crushed glass was allowed to react with ASTM type I water under static conditions. All leachate solutions were analyzed by the technique; Inductively Coupled Plasma-Atomic Emission Spectroscopy (ICP-AES). A statistical regression technique was utilized to model the normalized release of the major soluble elements, Na, Si, and B, as a function of the individual as well as interactive chemical effects (B2O3, Al2O3, Fe2O3, MnO, SiO2, SrO, Na2O, B2O3*SiO2, B2O3*Al2O3, Fe2O3*Na2O, Al2O3*Na2O, and MnO*SiO2). Geochemical modeling was performed using the computer code EQ3/6 to: (1) determine the saturation states of the possible silicate minerals, a-cristobalite and chalcedony; and (2) predict the most stable mineral phase based on the mineral thermodynamic data. Mineral/water interactions were analyzed by representing the resultant glass data on a Na-Al-Si-O-H stability diagram.


Systems Approach to Nuclear Waste Glass Development

Systems Approach to Nuclear Waste Glass Development

Author:

Publisher:

Published: 1986

Total Pages:

ISBN-13:

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Development of a host solid for the immobilization of nuclear waste has focused on various vitreous wasteforms. The systems approach requires that parameters affecting product performance and processing be considered simultaneously. Application of the systems approach indicates that borosilicate glasses are, overall, the most suitable glasses for the immobilization of nuclear waste. Phosphate glasses are highly durable; but the glass melts are highly corrosive and the glasses have poor thermal stability and low solubility for many waste components. High-silica glasses have good chemical durability, thermal stability, and mechanical stability, but the associated high melting temperatures increase volatilization of hazardous species in the waste. Borosilicate glasses are chemically durable and are stable both thermally and mechanically. The borosilicate melts are generally less corrosive than commercial glasses, and the melt temperature miimizes excessive volatility of hazardous species. Optimization of borosilicate waste glass formulations has led to their acceptance as the reference nuclear wasteform in the United States, United Kingdom, Belgium, Germany, France, Sweden, Switzerland, and Japan.


Natural Glass Analogues to Alteration of Nuclear Waste Glass

Natural Glass Analogues to Alteration of Nuclear Waste Glass

Author:

Publisher:

Published: 1990

Total Pages: 36

ISBN-13:

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The purpose of this report is to review previous work on the weathering of natural glasses; and to make recommendations for further work with respect to studying the alteration of natural glasses as it relates quantifying rates of dissolution. the first task was greatly simplified by the published papers of Jercinovic and Ewing (1987) and Byers, Jercinovic, and Ewing (1987). The second task is obviously the more difficult of the two and the author makes no claim of completeness in this regard. Glasses weather in the natural environment by reacting with aqueous solutions producing a rind of secondary solid phases. It had been proposed by some workers that the thickness of this rind is a function of the age of the glass and thus could be used to estimate glass dissolution rates. However, Jercinovic and Ewing (1987) point out that in general the rind thickness does not correlate with the age of the glass owing to the differences in time of contact with the solution compared to the actual age of the sample. It should be noted that the rate of glass dissolution is also a function of the composition of both the glass and the solution, and the temperature. Quantification of the effects of these parameters (as well as time of contact with the aqueous phase and flow rates) would thus permit a prediction of the consequences of glass-fluid interactions under varying environmental conditions. Defense high- level nuclear waste (DHLW), consisting primarily of liquid and sludge, will be encapsulated by and dispersed in a borosilicate glass before permanent storage in a HLW repository. This glass containing the DHLW serves to dilute the radionuclides and to retard their dispersion into the environment. 318 refs.


Optimization of Waste Loading in High-level Glass in the Presence of Uncertainty

Optimization of Waste Loading in High-level Glass in the Presence of Uncertainty

Author:

Publisher:

Published: 1995

Total Pages: 13

ISBN-13:

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Hanford high-level liquid waste will be converted into a glass form for long-term storage. The glass must meet certain constraints on its composition and properties in order to have desired properties for processing (e.g., electrical conductivity, viscosity, and liquidus temperature) and acceptable durability for long-term storage. The Optimal Waste Loading (OWL) models, based on rigorous mathematical optimization techniques, have been developed to minimize the number of glass logs required and determine glass-former compositions that will produce a glass meeting all relevant constraints. There is considerable uncertainty in many of the models and data relevant to the formulation of high-level glass. In this paper, we discuss how we handle uncertainty in the glass property models and in the high-level waste composition to the vitrification process. Glass property constraints used in optimization are inequalities that relate glass property models obtained by regression analysis of experimental data to numerical limits on property values. Therefore, these constraints are subject to uncertainty. The sampling distributions of the regression models are used to describe the uncertainties associated with the constraints. The optimization then accounts for these uncertainties by requiring the constraints to be satisfied within specified confidence limits. The uncertainty in waste composition is handled using stochastic optimization. Given means and standard deviations of component masses in the high-level waste stream, distributions of possible values for each component are generated. A series of optimization runs is performed; the distribution of each waste component is sampled for each run. The resultant distribution of solutions is then statistically summarized. The ability of OWL models to handle these forms of uncertainty make them very useful tools in designing and evaluating high-level waste glasses formulations.


Database and Interim Glass Property Models for Hanford HLW and LAW Glasses

Database and Interim Glass Property Models for Hanford HLW and LAW Glasses

Author:

Publisher:

Published: 2002

Total Pages: 5

ISBN-13:

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This report discusses a methodology for increasing the efficiency and decreasing the cost of vitrifying nuclear waste by optimizing waste-glass formulation. This methodology involves collecting and generating a property-composition database (for glass properties that determine waste-glass processability and acceptability) and relating these properties to glass composition via property-composition models. The report explains how the property-composition models are developed, fitted to data and evaluated, validated using additional data, used for glass-formulation optimization, and continuously updated in response to changes in waste-composition estimates and processing technologies. Further, the report describes a waste-glass property-composition database compiled from literature sources and presents the results from a critical evaluation and screening of the data for applicability to Hanford waste glasses. Finally, the report provides interim property-composition models for melt viscosity, liquidus temperature (with spinel and zircon primary crystalline phases), and Product Consistency Test normalized releases of B, Na, and Li. Models were fitted to a subset of the database deemed most relevant for the anticipated Hanford waste-glass composition region.