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.

RETENTION OF SULFATE IN HIGH LEVEL RADIOACTIVE WASTE GLASS.
RETENTION OF SULFATE IN HIGH LEVEL RADIOACTIVE WASTE GLASS.

Author:

Publisher:

Published: 2010

Total Pages:

ISBN-13:

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High level radioactive wastes are being vitrified at the Savannah River Site for long term disposal. Many of the wastes contain sulfate at concentrations that can be difficult to retain in borosilicate glass. This study involves efforts to optimize the composition of a glass frit for combination with the waste to improve sulfate retention while meeting other process and product performance constraints. The fabrication and characterization of several series of simulated waste glasses are described. The experiments are detailed chronologically, to provide insight into part of the engineering studies used in developing frit compositions for an operating high level waste vitrification facility. The results lead to the recommendation of a specific frit composition and a concentration limit for sulfate in the glass for the next batch of sludge to be processed at Savannah River.

Glass Optimization for Vitrification of Hanford Site Low-level Tank Waste
Glass Optimization for Vitrification of Hanford Site Low-level Tank Waste

Author:

Publisher:

Published: 2001

Total Pages:

ISBN-13:

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The radioactive defense wastes stored in 177 underground single-shell tanks (SST) and double-shell tanks (DST) at the Hanford Site will be separated into low-level and high-level fractions. One technology activity underway at PNNL is the development of glass formulations for the immobilization of the low-level tank wastes. A glass formulation strategy has been developed that describes development approaches to optimize glass compositions prior to the projected LLW vitrification facility start-up in 2005. Implementation of this strategy requires testing of glass formulations spanning a number of waste loadings, compositions, and additives over the range of expected waste compositions. The resulting glasses will then be characterized and compared to processing and performance specifications yet to be developed. This report documents the glass formulation work conducted at PNL in fiscal years 1994 and 1995 including glass formulation optimization, minor component impacts evaluation, Phase 1 and Phase 2 melter vendor glass development, liquidus temperature and crystallization kinetics determination. This report also summarizes relevant work at PNNL on high-iron glasses for Hanford tank wastes conducted through the Mixed Waste Integrated Program and work at Savannah River Technology Center to optimize glass formulations using a Plackett-Burnam experimental design.