Stability of High-Level Waste Forms

The objective of the proposed effort is to use a new approach to develop solution models of complex waste glass systems and spent fuel that are predictive with regard to composition, phase separation, and volatility. The effort will also yield thermodynamic values for waste components that are fundamentally required for corrosion models used to predict the leaching/corrosion behavior for waste glass and spent fuel material. This basic information and understanding of chemical behavior can subsequently be used directly in computational models of leaching and transport in geologic media, in designing and engineering waste forms and barrier systems, and in prediction of chemical interactions

Hanford Low-Activity Waste Vitrification: A Review

This Paper Summarizes the Vast Body of Literature (Over 200 Documents) Related to Vitrification of the Low-Activity Waste (LAW) Fraction of the Hanford Tank Wastes. Details Are Provided on the Origins of the Hanford Tank Wastes that Resulted from Nuclear Operations Conducted between 1944 and 1989 to Support Nuclear Weapons Production. Waste Treatment Processes Are Described, Including the Baseline Process to Separate the Tank Waste into LAW and High-Level Waste Fractions, and the LAW Vitrification Facility Being Started at Hanford. Significant Focus is Placed on the Glass Composition Development and the Property-Composition Relationships for Hanford LAW Glasses. Glass Disposal Plans and Criteria for Minimizing Long-Term Environmental Impacts Are Discussed Along with Research Perspectives

Sulfur Partitioning During Vitrification of INEEL Sodium Bearing Waste: Status Report

The sodium bearing tank waste (SBW) at Idaho National Engineering and Environmental Laboratory (INEEL) contains high concentrations of sulfur (roughly 5 mass% of SO3 on a nonvolatile oxide basis). The amount of sulfur that can be feed to the melter will ultimately determine the loading of SBW in glass produced by the baseline (low-temperature, joule-heated, liquid-fed, ceramic-lined) melter. The amount of sulfur which can be fed to the melter is determined by several major factors including: the tolerance of the melter for an immiscible salt layer accumulation, the solubility of sulfur in the glass melt, the fraction of sulfur removed to the off-gas, and the incorporation of sulfur into the glass up to it?s solubility limit. This report summarizes the current status of testing aimed at determining the impacts of key chemical and physical parameters on the partitioning of sulfur between the glass, a molten salt, and the off-gas

Preliminary ILAW Formulation Algorithm Description, 24590 LAW RPT-RT-04-0003, Rev. 1

The U.S. Department of Energy (DOE), Office of River Protection (ORP), has contracted with Bechtel National, Inc. (BNI) to design, construct, and commission the Hanford Tank Waste Treatment and Immobilization Plant (WTP) at the Hanford Site (DOE 2000). This plant is designed to operate for 40 years and treat roughly 50 million gallons of mixed hazardous high-level waste (HLW) stored in 177 underground tanks at the Hanford Site. The process involves separating the hight-level and low-activity waste (LAW) fractions through filtration, leaching, Cs ion exchange, and precipitation. Each fraction will be separately vitrified into borosilicate waste glass. This report documents the initial algorithm for use by Hanford WTP in batching LAW and glass-forming chemicals (GFCs) in the LAW melter feed preparation vessel (MFPV). Algorithm inputs include the chemical analyses of the pretreated LAW in the concentrate receipt vessel (CRV), the volume of the MFPV heel, and the compositions of individual GFCs. In addition to these inputs, uncertainties in the LAW composition and processing parameters are included in the algorithm

Initial Laboratory-Scale Melter Test Results for Combined Fission Product Waste

This report describes the methods and results used to vitrify a baseline glass, CSLNTM-C-2.5 in support of the AFCI (Advanced Fuel Cycle Initiative) using a Quartz Crucible Scale Melter at the Pacific Northwest National Laboratory. Document number AFCI-WAST-PMO-MI-DV-2009-000184

Glass Property Data and Models for Estimating High-Level Waste Glass Volume

This report describes recent efforts to develop glass property models that can be used to help estimate the volume of high-level waste (HLW) glass that will result from vitrification of Hanford tank waste. The compositions of acceptable and processable HLW glasses need to be optimized to minimize the waste-form volume and, hence, to save cost. A database of properties and associated compositions for simulated waste glasses was collected for developing property-composition models. This database, although not comprehensive, represents a large fraction of data on waste-glass compositions and properties that were available at the time of this report. Glass property-composition models were fit to subsets of the database for several key glass properties. These models apply to a significantly broader composition space than those previously publised. These models should be considered for interim use in calculating properties of Hanford waste glasses

Hanford Low-activity Waste Glass Composition-temperature-melt Viscosity Relationships

This study developed a model for predicting viscosity of alkali-alumino-borosilicate glass melts as functions of composition and temperature. The model is based on a total of 3935 viscosity-temperature data from 574 glasses with viscosity values ranging from 2.53 to 7260 Poise (P) in the temperature range of 900–1260°C. Several different model forms were surveyed, including those based on Arrhenius, Vogel-Fulcher-Tammann, Avramov-Milchev, and Mauro-Yue-Ellison-Gupta-Allen. For each of these models, combinations of the temperature-independent parameters were fitted to composition. It was found that generally fitting more than one temperature-independent parameter as functions of composition resulted in overfitting. The Avramov-Milchev-based model was found to best represent the Hanford low-activity waste glass melt viscosity data based on model fit and validation statistics. A 21-term partial quadratic mixture model was recommended for use. This model predicts melt viscosity with a root-mean square error of.1736 ln(P), which is similar to the error in viscosity measurements from replicate glass analyses of.1383 ln(P). Viscosity was found to be most increased by SiO2 \u3e Al2O3 \u3e ZrO2 \u3e SnO2 and most decreased by Li2O \u3e Na2O \u3e B2O3 \u3e CaO \u3e K2O \u3e MgO, at temperatures from 900 to 1260°C

Preliminary Technology Maturation Plan for Immobilization of High-Level Waste in Glass Ceramics

A technology maturation plan (TMP) was developed for immobilization of high-level waste (HLW) raffinate in a glass ceramics waste form using a cold-crucible induction melter (CCIM). The TMP was prepared by the following process: 1) define the reference process and boundaries of the technology being matured, 2) evaluate the technology elements and identify the critical technology elements (CTE), 3) identify the technology readiness level (TRL) of each of the CTE’s using the DOE G 413.3-4, 4) describe the development and demonstration activities required to advance the TRLs to 4 and 6 in order, and 5) prepare a preliminary plan to conduct the development and demonstration. Results of the technology readiness assessment identified five CTE’s and found relatively low TRL’s for each of them: • Mixing, sampling, and analysis of waste slurry and melter feed: TRL-1 • Feeding, melting, and pouring: TRL-1 • Glass ceramic formulation: TRL-1 • Canister cooling and crystallization: TRL-1 • Canister decontamination: TRL-4 Although the TRL’s are low for most of these CTE’s (TRL-1), the effort required to advance them to higher values. The activities required to advance the TRL’s are listed below: • Complete this TMP • Perform a preliminary engineering study • Characterize, estimate, and simulate waste to be treated • Laboratory scale glass ceramic testing • Melter and off-gas testing with simulants • Test the mixing, sampling, and analyses • Canister testing • Decontamination system testing • Issue a requirements document • Issue a risk management document • Complete preliminary design • Integrated pilot testing • Issue a waste compliance plan A preliminary schedule and budget were developed to complete these activities as summarized in the following table (assuming 2012 dollars). TRL Budget Year MSA FMP GCF CCC CD Overall $M 2012 1 1 1 1 4 1 0.3 2013 2 2 1 1 4 1 1.3 2014 2 3 1 1 4 1 1.8 2015 2 3 2 2 4 2 2.6 2016 2 3 2 2 4 2 4.9 2017 2 3 3 2 4 2 9.8 2018 3 3 3 3 4 3 7.9 2019 3 3 3 3 4 3 5.1 2020 3 3 3 3 4 3 14.6 2021 3 3 3 3 4 3 7.3 2022 3 3 3 3 4 3 8.8 2023 4 4 4 4 4 4 9.1 2024 5 5 5 5 5 5 6.9 2025 6 6 6 6 6 6 6.9 CCC = canister cooling and crystallization; FMP = feeding, melting, and pouring; GCF = glass ceramic formulation; MSA = mixing, sampling, and analyses. This TMP is intended to guide the development of the glass ceramics waste form and process to the point where it is ready for industrialization

Preliminary Investigation of Sulfur Loading in Hanford LAW Glass

A preliminary estimate was developed for loading limits for high-sulfur low-activity waste (LAW) feeds that will be vitrified into borosilicate glass at the Hanford Site in the waste-cleanup effort. Previous studies reported in the literature were consulted to provide a basis for the estimate. The examination of previous studies led to questions about sulfur loading in Hanford LAW glass, and scoping tests were performed to help answer these questions. These results of these tests indicated that a formulation approach developed by Vienna and colleagues shows promise for maximizing LAW loading in glass. However, there is a clear need for follow-on work. The potential for significantly lowering the amount of LAW glass produced at Hanford (after the initial phase of processing) because of higher sulfur tolerances may outweigh the cost and effort required to perform the necessary testing

Formulation Efforts for Direct Vitrification of INEEL Blend Calcine Waste Simulate: Fiscal Year 2000

This report documents the results of glass formulation efforts for Idaho National Engineering and Environmental Laboratory (INEEL) high level waste (HWL) calcine. Two waste compositions were used during testing. Testing started by using the Run 78 calcine composition and switched to simulated Blend calcine composition when it became available. The goal of the glass formulation efforts was to develop a frit composition that will accept higher waste loading that satisfies the glass processing and product acceptance constraints. 1. Melting temperature of 1125 ? 25?C 2. Viscosity between 2 and 10 Pa?s at the melting temperature 3. Liquidus temperature at least 100?C below the melting temperature 4. Normalized release of B, Li and Na each below 1 g/m2 (per ASTM C 1285-97) Glass formulation efforts tested several frit compositions with variable waste loadings of Run 78 calcine waste simulant. Frit 107 was selected as the primary candidate for processing since it met all process and performance criteria up to 45 mass% waste loading. When the simulated Blend calcine waste composition became available Frits 107 and 108 compositions were retested and again Frit 107 remained the primary candidate. However, both frits suffered a decrease in waste loading when switching from the Run 78 calcine to simulated Blend calcine waste composition. This was due to increase concentrations of both F and Al2O3 along with a decrease in CaO and Na2O in the simulate Blend calcine waste all of which have strong impacts on the glass properties that limit waste loading of this type of waste