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DOE OSTI2018

Vitrification of High-Level Waste: how to Select the Best Suited Technology - 18117

Since more than 30 years now, a number of countries have selected and operated vitrification as the best industrial practice for safely and durably immobilizing the most active liquid waste. This now significant worldwide experience covers a wide range of waste compositions, from concentrated alkaline defense waste sludges with a variety of salts and chemicals (Na, Fe, Al, Cr, sulphate,... ) to relatively clear acidic HLLW from commercial, low salt, PUREX-type processes, waste that include dissolved cladding material (Al, Mg, stainless steel), waste that include high levels of noble metals and fines... The activity levels vary from 40- year old defense waste to relatively young waste from high burn-up commercial fuel. The current throughputs vary from about 5 kg/h of glass to about 90 kg/h of glass per melter. Even higher throughputs are currently being considered for Hanford facility for instance. In order to cope with the range of waste compositions, glass compositions have also evolved from low melting temperature borosilicate or phosphate glass to glass or glass ceramics with higher melting temperatures. More complex matrices are currently under study in a number of countries, to immobilize more complex waste and / or increase waste loadings. Each challenge is unique and, for each challenge, it is necessary to select the best combination of waste form and technology. For instance for very active solutions with high levels of noble metal particles that could settle, increase apparent glass viscosity, and impact electrical conductivity, one would select borosilicate glass in the mechanically-stirred hot wall induction melter with bottom pouring that has proven its efficiency in industrial conditions at La Hague. For high glass throughputs with low solids in a borosilicate melt (typically Defense waste), ceramic melters have proven their reliability and efficiency. For matrices that need higher temperatures, or with very high corrosiveness, Cold-Crucible Induction Melters are now considered, with one first industrial implementation at La Hague to produce borosilicate glass and a glass-ceramic. All these technologies have been improved over the years to increase throughput, waste loading, melting temperature, reliability... Other types of waste are now being studied worldwide, and for each, it is necessary to carefully select the adapted waste form and technology. The technologies studied will range from traditional technologies (such as hot-wall induction melter technology and liquid-fed ceramic melter technologies) to the more recent advanced technologies (such as Cold Crucible Induction Melter or Advanced Ceramic melters). In addition, the field of vitrification is extending to other types of waste; the current advances in this field will also be described. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS1983

Integrated water management system - Description and test results

Water recovery subsystems are being tested at the NASA Lyndon B. Johnson Space Center for Space Station use to process waste water generated from urine and wash water collection facilities. These subsystems are being integrated into a water management system that will incorporate wash water and urine processing through the use of hyperfiltration and vapor compression distillation subsystems. Other hardware in the water management system includes a whole body shower, a clothes washing facility, a urine collection and pretreatment unit, a recovered water post-treatment system, and a water quality monitor. This paper describes the integrated test configuration, pertinent performance data, and feasibility and design compatibility conclusions of the integrated water management system.

Elden, N. C.↗

DOE OSTI2021

Evaluation of Ammonium and Iodine Decontamination Factors for Hanford's Waste Treatment and Immobilization Plant Feed in the Effluent Treatment Facility

Savannah River National Laboratory (SRNL) reviewed the unit operations in the Effluent Treatment Facility (FTP) at the Hanford site to estimate the partitioning of iodine and ammonia when processing Waste Treatments and Immobilization Plant (WTP) feed. The evaluation consisted of literature and vendor data reviews and no experiments were performed. A list of the unit operations reviewed, along with estimated decontamination factors (DFs) for both iodine and ammonium are shown in the table below. With the exception of the Peroxide Decomposer, reasonable estimations of the decontamination factors for all operations are provided.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Reduced Neutralization Feasibility Study for H-Canyon Accelerated Basin De- Inventory (ABD) Program

An alternative approach to Spent Nuclear Fuel (SNF) and Nuclear Material Processing was developed for future H-Canyon (HCAN) and L-Area operations that involves a paradigm shift from current HCAN, Concentrate, Storage, and Transfer Facility (CSTF), and Defense Waste Processing Facility (DWPF) operations. The alternative, referred to as Accelerated Basin De-inventory (ABD), requires that all Domestic and Foreign Research Reactor SNF currently at the Savannah River Site (SRS) will be dissolved, stored, and then transferred to CSTF without recovery of Highly Enriched Uranium (HEU). Concentrated nitric acid is utilized to dissolve aluminum spent nuclear fuel (ASNF) in HCAN. The vessels and piping in HCAN are fabricated from 304L stainless steel and are ideally suited to handle the acidic waste stream. However, as the waste is transferred to the CSTF and DWPF, it will contact the carbon steel waste tanks in CSTF. In order to prevent corrosion of the carbon steel, the acidic waste is neutralized (i.e., pH adjusted over 11) by the addition of sodium hydroxide (NaOH). The NaOH is added until the final solution contains 1.2 M excess -OH. Additionally, if the waste is not neutralized to a pH greater than 11, then aluminum hydroxide (Al(OH) 3 ) would form, and solids may form in the piping as it is transferred to CSTF. This document presents an analysis of the influence of reducing the excess caustic that is added to the neutralization tanks on the corrosion protection scheme primarily for the CSTF waste tanks. The implications to HCAN and DWPF were also assessed.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Evaluation of Glass Density to Support the Estimation of Fissile Mass Loadings in Sludge Batch 10 Glasses

Per a directive from the Department of Energy Savannah River Operations Office (DOE-SR) in 2008, the fissile mass loading concentration must remain below 897 g/m 3 in each high-level waste (HLW) glass canister produced by the Defense Waste Processing Facility (DWPF). To support Sludge Batch 5 (SB5) processing, the Savannah River National Laboratory (SRNL) developed a technical basis that facilitates the evaluation of fissile mass loading of the glass product. The calculation is based on the iron (Fe) concentration in the glass as determined by measurements from the Slurry Mix Evaporator acceptability analysis as well as the glass density. In April 2022, a subsequent DOE-SR directive increased the fissile mass loading limit to 2500 g/m 3 beginning with Sludge Batch 11. Thus, the 897 g/m 3 limit still applies to Sludge Batch 10 (SB10) processing.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRS1990

Generation rates and chemical compositions of waste streams in a typical crewed space habitat

A judicious compilation of generation rates and chemical compositions of potential waste feed streams in a typical crewed space habitat was made in connection with the waste-management aspect of NASA's Physical/Chemical Closed-Loop Life Support Program. Waste composition definitions are needed for the design of waste-processing technologies involved in closing major life support functions in future long-duration human space missions. Tables of data for the constituents and chemical formulas of the following waste streams are presented and discussed: human urine, feces, hygiene (laundry and shower) water, cleansing agents, trash, humidity condensate, dried sweat, and trace contaminants. Tables of data on dust generation and pH values of the different waste streams are also presented and discussed.

Wydeven, Theodore↗

NASA NTRS1991

Waste streams in a crewed space habitat

Wydeven, T.↗

DOE OSTI2023

Technical Evaluation of Accelerated Basin De-Inventory Material Addition to Sludge Batch 11

Savannah River Nuclear Solutions has a need to discard spent nuclear fuel (SNF), currently stored in L Basin, to the Defense Waste Processing Facility (DWPF) for vitrification. The Department of Energy (DOE) has approved the Accelerated Basin De-inventory (ABD) Program for discarding SNF via transfers from H-Canyon to the Savannah River Site (SRS) Liquid Waste (LW) system. The first ABD discards will occur during the preparation of Sludge Batch (SB) 11. An initial impact evaluation of the LW flowsheet was performed by the Savannah River National Laboratory (SRNL) prior to the approval of the ABD Program. This evaluation addressed the LW downstream facilities based on the current H-Canyon flowsheet sequence for the average ABD discard. The flowsheet evaluation only included aluminum-clad SNF, specifically Materials Test Reactor (MTR) fuel and High Flux Isotope Reactor (HFIR) fuel similar to the planned SB11 discard. Following this evaluation, the flowsheet has been slightly altered to address (i) new nuclear criticality safety controls for DWPF that credit a higher amount of gadolinium as a neutron poison for all of the enriched uranium contained in a SB and (ii) potential additions of the H-Canyon neutralized fuel stream prior to the Low Temperature Aluminum Dissolution (LTAD) process in Tank 51. The early introduction of ABD material into the SB assembly process is being investigated to provide flexibility regarding transfer opportunities for H-Canyon to Tank 51 for SB11 and future sludge batches.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Washing Study with SRS Tank 26 Samples FTF-26-19-12 and -13

A recent analysis of Tank 26, one of the feed tanks for the Defense Waste Processing Facility (DWPF) Sludge Batch 10 (SB10), determined a higher than anticipated sulfur concentration in the supernatant and a significant amount of insoluble sulfur, which could negatively impact the DWPF glass waste form. Savannah River Remediation Engineering (SRR-E) requested that the Savannah River National Laboratory (SRNL) perform a washing study with Tank 26 material to determine amount of sulfur removed during washing tests. SRNL decanted supernate from a sample of Tank 26 until it was at 12 wt% insoluble solids. Subsequently, SRNL performed washing experiments from the 8 M sodium initial concentration to targeted endpoints of 4 M, 2 M and 1 M sodium concentration (assuming no sodium dissolution). Results show that over 80% of the sulfur was removed and nearly all the sulfur was in the aqueous phase at the end of washing, demonstrating effective removal of sulfur during washing. Additional washing is likely to decrease the sulfur concentration further since most of the sulfur was in the aqueous phase.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Evaluation of Thermolytic Production of Hydrogen from Glycolate and Common Tank Farm Organics in Simulated Waste

The Savannah River National Laboratory (SRNL) has performed testing to investigate the thermolytic production of hydrogen gas from organic species present in the Savannah River Site (SRS) Concentration, Storage, and Transfer Facilities (CSTF). SRNL designed an experimental apparatus to measure the time-dependent concentration of hydrogen in the headspace over a reacting mixture of simulated caustic waste media and organic compounds as well as a methodology to calculate a steady-state hydrogen generation rate (HGR) from this data. Special focus was given to glycolate, which is not currently present in CSTF waste but will be contained in the recycle stream from the Defense Waste Processing Facility (DWPF) under the upcoming alternate reductant flowsheet.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2026

Evaluation of Pu Solubility in Glass for Sludge Batch 11

Stainless-steel clad Pu from Japan’s Fast Critical Assembly (FCA) reactor is currently being dispositioned at the Savannah River Site. The electrolytic dissolver, operated by Savannah River Nuclear Solutions in H-Canyon, is being utilized to dissolve the material. The resulting solutions are transferred to the Concentration, Storage, and Transfer Facilities, operated by Savannah River Mission Completion (SRMC), for subsequent vitrification at the Defense Waste Processing Facility (DWPF). In support of the FCA mission startup, a preliminary evaluation was conducted by the Savannah River National Laboratory to assess the impact of the FCA discards on the liquid waste system.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS1993

Incineration for resource recovery in a closed ecological life support system

A functional schematic, including mass and energy balance, of a solid waste processing system for a controlled ecological life support system (CELSS) was developed using Aspen Plus, a commercial computer simulation program. The primary processor in this system is an incinerator for oxidizing organic wastes. The major products derived from the incinerator are carbon dioxide and water, which can be recycled to a crop growth chamber (CGC) for food production. The majority of soluble inorganics are extracted or leached from the inedible biomass before they reach the incinerator, so that they can be returned directly to the CGC and reused as nutrients. The heat derived from combustion of organic compounds in the incinerator was used for phase-change water purification. The waste streams treated by the incinerator system conceptualized in this work are inedible biomass from a CGC, human urine (including urinal flush water) and feces, humidity condensate, shower water, and trash. It is estimated that the theoretical minimum surface area required for the radiator to reject the unusable heat output from this system would be 0.72 sq m/person at 298 K.

Upadhye, R. S.↗

NASA NTRS1996

Earth benefits of interdisciplinary CELSS-related research by the NSCORT in Bioregenerative Life Support

Earth benefits of research from the NSCORT in Bioregenerative Life Support will include the following: development of active control mechanisms for light, CO2, and temperature to maximize photosynthesis of crop plants during important phases of crop development; automation of crop culture systems; creation of novel culture systems for optimum productivity; creation of value-added crops with superior nutritional, yield, and waste-process characteristics; environmental control of food and toxicant composition of crops; new process technologies and novel food products for safe, nutritious, palatable vegetarian diets; creation of menus for healthful vegetarian diets with psychological acceptability; enzymatic procedures to degrade recalcitrant crop residues occurring in municipal waste; control-system strategies to ensure sustainabilty of a CELSS that will enable management of diverse complex systems on Earth.

NASA Discipline Number 93-10↗

NASA NTRS2005

Designing For Human Presence in Space: An Introduction to Environmental Control and Life Support Systems (ECLSS)

Human exploration and utilization of space requires habitats to provide appropriate conditions for working and living. These conditions are provided by environmental control and life support systems (ECLSS) that ensure appropriate atmosphere composition, pressure, and temperature; manage and distribute water, process waste matter, provide fire detection and suppression; and other functions as necessary. The tables in appendix I of NASA RP 1324 "Designing for Human Presence in Space" summarize the life support functions and processes used onboard U.S. and U.S.S.R/Russian space habitats. These tables have been updated to include information on thermal control methods and to provide additional information on the ECLS systems.

Wieland, P. O.↗

NASA NTRS2005

Testing and Analysis of the First Plastic Melt Waste Compactor Prototype

A half scale Plastic Melt Waste Compactor prototype has been developed at NASA Ames Research Center. The half scale prototype unit will lead to the development of a full scale Plastic Melt Waste Compactor prototype that is representative of flight hardware that would be used on near and far term space missions. This report details the testing being done on the prototype Plastic Melt Waste Compactor by the Solid Waste Management group at NASA Ames Research Center. The tests are designed to determine the prototype's functionality, simplicity of operation, ability to contain and control noxious off-gassing, biological stability of the processed waste, and water recovery potential using a waste composite that is representative of the types of wastes produced on the International Space Station, Space Shuttle, MIR and Skylab missions.

Pace, Gregory S.↗

DOE OSTI2019

Composition-Based Density Model for High Level Waste Glasses

In this report, the Savannah River National Laboratory (SRNL) provides a first-principles model capable of predicting the density of high-level waste (HLW) glass based on the glass composition. The model relies on the additivity of the specific volume of bound glass oxides to obtain a quantitative evaluation of the approximate glass density. A database of glass densities and compositions was compiled from various sources including previous Defense Waste Processing Facility (DWPF) variability study glasses, HLW studies from other institutions, and literature references. There are a total of 1104 glass compositions in the database with densities ranging from 2.224 g/cm 3 to 3.997 g/cm 3 . The breadth of the compositional coverage space is reported as well. A predictive method was investigated in which the glass density was calculated as a function of the weighted partial molar volumes of the individual glass oxides and the molar mass of the glass. This method yielded a high correlation between the predicted density and the measured density. In addition, a linear regression of these predictions indicated that the predicted value was equal to the measured within the bounds of analytical uncertainty. The following conclusions were drawn from the results of these analyses: 1. Measured glass density is highly correlated with glass composition (R 2 ≈ 0.95). 2. The correlation between glass density and glass composition can be expressed as either: a. A weighted sum of the individual oxide glass-component densities, or b. A weighted sum of the individual oxide glass-component partial molar volumes. 3. A linear regression of the predicted density via partial molar volume method to the measured density yields a slope of 0.9975 and an intercept of -0.0007 – the uncertainty interval associated with these coefficients contain one and zero, respectively. 4. The fitted coefficients and associated uncertainty intervals of the linear regression of the predicted density via the partial molar volume method to the measured density suggest that the predicted theoretical density is, within analysis uncertainty, equal to the measured density of the glass. It is recommended that glass density measurements included with the variability study for each sludge batch be discontinued. In their place, SRNL will calculate a bounding glass density value for the frit/sludge system using the model. It is also recommended that DWPF implement the density model as part of the fissile loading determination portion of the SME acceptability process. Details for implementation are provided in this report.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Evaluation of Thermolytic Production of Hydrogen from Glycolate and Common Tank Farm Organics in Simulated Waste

The Savannah River National Laboratory (SRNL) has performed testing to investigate the thermolytic production of hydrogen gas from organic species present in the Savannah River Site (SRS) Concentration, Storage, and Transfer Facilities (CSTF). SRNL designed an experimental apparatus to measure the timedependent concentration of hydrogen in the headspace over a reacting mixture of simulated caustic waste media and organic compounds as well as a methodology to calculate a steady-state hydrogen generation rate (HGR) from this data. Special focus was given to glycolate, which is not currently present in CSTF waste but will be contained in the recycle stream from the Defense Waste Processing Facility (DWPF) under the upcoming alternate reductant flowsheet.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS2005

Design and Testing of a Lyophilizer for Water Recovery from Solid Waste

Mixed liquid/solid wastes, including feces, water processor effluents, and food waste, can be lyophilized (freeze-dried) to recover the water they contain and stabilize the solids remain. Previous research has demonstrated the potential benefits of using thermoelectric heat pumps to build a lyophilizer for processing waste in microgravity. These results were used to build a working prototype suitable for ground-based human testing. This paper describes the prototype design and presents the results of functional and performance tests. Equivalent system mass parameters are calculated, and practical issues such as sanitary waste handling in microgravity are addressed.

Litwiller, Eric↗