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DOE OSTI2018

Management of Metals from Decommissioning of Nuclear Facilities - 18411

The EDF group companies within the Cyclife platform have for decades performed treatment and recycling of metals. With different approaches but all considered international Good Practice, as valuable materials are recovered for safe recycling and volumes in the repositories for radioactive waste are saved. For an efficient decommissioning project, a well-defined waste management process is one of the critical paths, not least when it comes to routes for clearance and recycling of materials. It is easy to underestimate the complexity and bottlenecks caused by shortage of logistic space. In order to mitigate these risks, activities such as strengthening categorization, quantification and adopting different routes based on the material properties should be implemented. By categorization of the of waste and materials considered/classified as contaminated or potentially contaminated it is obvious that the management of the metals is a key parameter in nuclear decommissioning. Analyses performed by the EDF companies shows that a majority of the materials, classified as contaminated, from a BWR/PWR plant are metals. Experience gives that a high percentage of these metals from decommissioning can be subject to recycling either directly upon completion of the clearance process or after certain treatment. Non-technical key parameters like the regulatory requirements on applying the waste hierarchy, the impact on repository programs as well as, not at least, the regulatory and public acceptance of recycling of materials from the nuclear industry are, together with costs essential factors when forming the routing of metals and other waste materials from a decommissioning project. Today the EDF group companies are positioned to provide a wide range of services for management of the contaminated metals from decommissioning projects, spanning from industrial management of metals which directly will be subject general clearance after verification measurements up to decontamination and melting of selected reactor internals for recycling to public domain or within the nuclear industry. In this paper the typical waste material composition for BWR and PWR plants, the different ways to treat/manage the radioactive and potentially radioactive metals including a comparison of the different approach commonly used in a technical, logistical and economical perspectives. A few success stories will be resented as well as lessons learned. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2017

'A Good Decision Is Based On Information, Not On Numbers' - A Process For National Strategic Decision Making - 17203

Waste management decision making is the process used by waste owners to determine and justify choices in across the lifecycle of a waste (from the manner of generation or retrieval to final disposition). In the UK, waste owners in the nuclear industry are obligated, by their environmental permits and authorisations, to demonstrate the application of robust and well-underpinned decision making processes for waste management. This is captured through the requirement for waste owners to demonstrate the identification and implementation of Best Available Technique (BAT). The National Waste Programme (NWP), led by LLW Repository Ltd, is a UK wide programme which leads the implementation of the UK National Strategy for the management of solid LLW from the nuclear industry [1] and which aims to deliver a self-sustaining culture for optimised management of Low Level Waste (LLW) in the UK. Recognising the requirement on waste owners, the NWP has - in conjunction with appointed contractors - led the development and publication of national strategic optioneering studies (so-called national strategic BAT studies) to support waste owners. Recognising the benefits that this approach to optioneering and strategic decision making could have for other waste producers, this paper provides an overview of the process used for the development of the suite of national strategic BAT assessments for the NWP. It details: the main phases of the process, the key features of each process phase, the benefits of the approach and key learning from its deployment in practice. Note: The legislative regime in England and Wales requires the identification and application of BAT. There is an equivalent regime in Scotland known as Best Practicable Environmental Option (BPEO) and Best Practicable Means (BPM). The requirements are comparable across the two legislative regimes and, for the purposes of simplicity, the term BAT will be utilised in this paper. The approach and outcomes of the national strategic optioneering process described are applicable across the UK. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2016

Experimental Evaluation of Dual-Opposed Jet Mixer Pump Performance for Slurry Mixing

Million-gallon double-shell tanks at Hanford are used to store transuranic, high-level, and low-level radioactive wastes. These wastes consist of a large volume of salt-laden solution covering a smaller volume of settled sludge primarily containing metal hydroxides. These wastes will be retrieved and processed into immobile waste forms suitable for permanent disposal. Retrieval is an important step in implementing these disposal scenarios. The retrieval concept evaluated is to use submerged dual-nozzle jet mixer pumps with horizontally oriented nozzles located near the tank floor that produce horizontal jets of fluid to mobilize the settled solids. The mixer pumps are oscillated through 180 about a vertical axis so the high velocity fluid jets sweep across the floor of the tank. After the solids are mobilized, the pumps will continue to operate at a reduced flow rate producing lower velocity jets sufficient to maintain the particles in a uniform suspension (concentration uniformity). Several types of waste and tank configurations exist at Hanford. The jet mixer pump systems and operating conditions required to mobilize sludge and maintain slurry uniformity will be a function of the waste type and tank configuration. The focus of this work was to conduct a 1/12-scale experiment to develop an analytical model to relate slurry uniformity to tank and mixer pump configurations, operating conditions, and sludge properties. This experimental study evaluated concentration uniformity in a 1/12-scale experiment varying the Reynolds number (Re), Froude number (Fr), and gravitational settling parameter (Gs) space. Simulant physical properties were chosen to obtain the required Re and Gs where Re and Gs were varied by adjusting the kinematic viscosity and mean particle diameter, respectively. Test conditions were achieved by scaling the jet nozzle exit velocity in a 75-in. diameter tank using a mock-up of a centrally located dual-opposed jet mixer pump located just above the tank floor. Concentration measurements at sampling locations throughout the tank were used to assess the degree of uniformity achieved during each test. Concentration data was obtained using a real time in-situ ultrasonic attenuation probe and post-test analysis of discrete batch samples. The undissolved solids concentration at these locations was analyzed to determine whether the tank contents were uniform (≤ ±10% variation about mean) or nonuniform (> ±10% variation about mean) in concentration. Concentration inhomogeneity was modeled as a function of dimensionless parameters. The parameters that best describe the maximum solids volume fraction that can be suspended were found to be 1) the Fr based on nozzle average discharge velocity and tank contents level and 2) the dimensionless particle size based on nozzle diameter. The dependence on the jet Re does not appear to be statistically significant.

correlation↗

DOE OSTI2011

Engineering Glass Passivation Layers -Model Results

The immobilization of radioactive waste into glass waste forms is a baseline process of nuclear waste management not only in the United States, but worldwide. The rate of radionuclide release from these glasses is a critical measure of the quality of the waste form. Over long-term tests and using extrapolations of ancient analogues, it has been shown that well designed glasses exhibit a dissolution rate that quickly decreases to a slow residual rate for the lifetime of the glass. The mechanistic cause of this decreased corrosion rate is a subject of debate, with one of the major theories suggesting that the decrease is caused by the formation of corrosion products in such a manner as to present a diffusion barrier on the surface of the glass. Although there is much evidence of this type of mechanism, there has been no attempt to engineer the effect to maximize the passivating qualities of the corrosion products. This study represents the first attempt to engineer the creation of passivating phases on the surface of glasses. Our approach utilizes interactions between the dissolving glass and elements from the disposal environment to create impermeable capping layers. By drawing from other corrosion studies in areas where passivation layers have been successfully engineered to protect the bulk material, we present here a report on mineral phases that are likely have a morphological tendency to encrust the surface of the glass. Our modeling has focused on using the AFCI glass system in a carbonate, sulfate, and phosphate rich environment. We evaluate the minerals predicted to form to determine the likelihood of the formation of a protective layer on the surface of the glass. We have also modeled individual ions in solutions vs. pH and the addition of aluminum and silicon. These results allow us to understand the pH and ion concentration dependence of mineral formation. We have determined that iron minerals are likely to form a complete incrustation layer and we plan to look more closely at Vivianite [Fe3(PO4)2-8(H2O)] and Siderite [FeCO3] in the next stage of the project.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2024

Viscosity Measurements of the HLW APPS Glasses

The U.S. Department of Energy is responsible for building the Hanford Waste Treatment and Immobilization Plant (WTP) at the Hanford site in Washington to remediate 56 million gallons of radioactive waste historically stored in 177 underground tanks. The Office of River Protection has requested that the Savannah River National Laboratory (SRNL) contribute in areas of recognized capabilities and expertise for glass waste form development to support successful startup of the WTP. SRNL support of this work is defined in the Task Technical and Quality Assurance Plan.1 This report provides results from viscosity measurements on a series of simulated nuclear waste glasses designed and fabricated at Pacific Northwest National Laboratory (PNNL). The glasses were designated the high-level waste – Aspen Process Performance Simulation (HLW-APPS) study glasses. The data provided in this report is to be used in the development, validation, and implementation of enhanced property/composition models for nuclear waste glasses.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2012

Lessons Learned from the Application of Bulk Characterization to Individual Containers on the Brookhaven Graphite Research Reactor Decommissioning Project at Brookhaven National Laboratory - 12056

When conducting environmental cleanup or decommissioning projects, characterization of the material to be removed is often performed when the material is in-situ. The actual demolition or excavation and removal of the material can result in individual containers that vary significantly from the original bulk characterization profile. This variance, if not detected, can result in individual containers exceeding Department of Transportation regulations or waste disposal site acceptance criteria. Bulk waste characterization processes were performed to initially characterize the Brookhaven Graphite Research Reactor (BGRR) graphite pile and this information was utilized to characterize all of the containers of graphite. When the last waste container was generated containing graphite dust from the bottom of the pile, but no solid graphite blocks, the material contents were significantly different in composition from the bulk waste characterization. This error resulted in exceedance of the disposal site waste acceptance criteria. Brookhaven Science Associates initiated an in-depth investigation to identify the root causes of this failure and to develop appropriate corrective actions. The lessons learned at BNL have applicability to other cleanup and demolition projects which characterize their wastes in bulk or in-situ and then extend that characterization to individual containers. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Expansion of the Direct Feed High-Level Waste Glass Composition in the High Al Range

Baseline glass compositions have been developed and demonstrated for successful immobilization of Hanford high-level waste (HLW) prepared through a pretreatment process. Recent enhanced waste glass formulations have shown promise to increase the waste loading of pretreated sludge compositions from a broader range of HLW feeds. This project proposes to increase the loading of minimally pretreated Hanford HLW in glass by expanding the existing database and glass property-composition models. Estimated direct-feed high level waste (DFHLW) compositions were generated by the Hanford Tank Operations Contractor and used by Pacific Northwest National Laboratory to determine target glass compositions. Gaps in existing data were identified including one high-priority gap in the high Al compositional region. This report summarizes the data collected during the characterization of the DFHLW High Al Glass Matrix. These glasses were intentionally designed with high aluminum concentrations (15 to 30 wt%) and a high likelihood of nepheline formation, which is known to negatively affect glass durability. Some glasses were expected to either fail or approach property constraints to fill data gaps in poorly understood regions of the compositional space due to lack of data. Out of the 50 glasses tested, 14 glasses formed nepheline, while the model predicted nepheline formation in 20 glasses. All quenched glasses met the product consistency test durability constraint; however, 8 glasses failed this constraint after undergoing the canister centerline cooling treatment. Additionally, 17 glasses did not meet the viscosity constraints, 4 failed the EC constraints, and 2 exceeded the allowable T2% for spinel crystal formation. All glasses satisfied the SO 3 solubility limit. The resulting dataset provides valuable information to improve model accuracy and reduce prediction uncertainty. These insights will ultimately support the development of more robust glass formulation strategies, enabling higher waste loadings, reducing operational risks, and expanding the processing envelope.

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NASA NTRS1991

Applications of CELSS technology to controlled environment agriculture

Controlled environment agriculture (CEA) is defined as the use of environmental manipulation for the commercial production of organisms, whether plants or animals. While many of the technologies necessary for aquaculture systems in North America is nevertheless doubling approximately every five years. Economic, cultural, and environmental pressures all favor CEA over field production for many non-commodity agricultural crops. Many countries around the world are already dependent on CEA for much of their fresh food. Controlled ecological life support systems (CELSS), under development at ARC, KSC, and JSC expand the concept of CEA to the extent that all human requirements for food, oxygen, and water will be provided regenerated by processing of waste streams to supply plant inputs. The CELSS will likely contain plants, humans, possibly other animals, microorganisms and physically and chemical processors. In effect, NASA will create engineered ecosystems. In the process of developing the technology for CELSS, NASA will develop information and technology which will be applied to improving the efficiency, reliability, and cost effectiveness for CEA, improving its resources recycling capabilities, and lessening its environmental impact to negligible levels.

Bates, Maynard E.↗

NASA NTRS2016

Development of Advanced ISS-WPA Catalysts for Organic Oxidation at Reduced Pressure/Temperature

The Water Processor Assembly (WPA) at International Space Station (ISS) processes a waste stream via multi-filtration beds, where inorganic and non-volatile organic contaminants are removed, and a catalytic reactor, where low molecular weight organics not removed by the adsorption process are oxidized at elevated pressure in the presence of oxygen and elevated temperature above the normal water boiling point. Operation at an elevated pressure requires a more complex system design compared to a reactor that could operate at ambient pressure. However, catalysts currently available have insufficient activity to achieve complete oxidation of the organic load at a temperature less than the water boiling point and ambient pressure. Therefore, it is highly desirable to develop a more active and efficient catalyst at ambient pressure and a moderate temperature that is less than water boiling temperature. This paper describes our efforts in developing high efficiency water processing catalysts. Different catalyst support structures and coating metals were investigated in subscale reactors and results were compared against the flight WPA catalyst. Detailed improvements achieved on alternate metal catalysts at ambient pressure and 200 F will also be presented in the paper.

Yu, Ping↗

DOE OSTI2020

Decommissioning of the V1 Nuclear Power Plant Jaslovske Bohunice - 20270

The paper focuses on introducing the approach and method applied for decommissioning of the V1 nuclear power plant (further the 'V1 NPP') located in Jaslovske Bohunice in the Slovak Republic, to the conference participants. The Paper outlines activities and steps necessary to comply with the requirements contained in the decision of the Slovak government from 1999 regarding the early shutdown of the V1 NPP. The company responsible for the V1 NPP decommissioning is Jadrova a vyradovacia spolocnost, a.s., (further JAVYS) with the State as a sole shareholder. On the basis of the V1 NPP Decommissioning Conceptual Plan, out of four assessed options, JAVYS selected the immediate decommissioning option (the 'IDO') for the V1 NPP. On the basis of multi-criteria analysis, the IDO specified the approach of immediate and continuous dismantling of equipment followed by demolition of buildings and preparation of the site for its further potential use. The IDO also included the summary of technical, environmental, legislative information as well as the determination of assumed costs for decommissioning of the V1 NPP. Prior to commencement of the V1 NPP decommissioning, within the process of termination of operation, activities connected with de-fuelling, monitoring, processing of historical waste and, not to forget, the process of obtaining the license for the V1 NPP decommissioning were executed. JAVYS decided to divide the decommissioning process into two stages. In 2011, JAVYS obtained a license for the first stage of the V1 NPP decommissioning. Within this stage, dismantling of inactive equipment, demolitions of inactive buildings, monitoring of systems and preparatory works for the upcoming stage of decommissioning were implemented. In 2015, in line with the license for the 2. stage of the V1 NPP decommissioning, the activities of decontamination and dismantling of contaminated and active equipment as well as demolitions of remaining buildings began. In this stage radioactive waste (RAW) produced during the decommissioning is to be processed. After decontamination, the material fulfilling the free release criteria is to be released into the environment, the site is to be cleared from the scope of the Atomic Act and released from the surveillance of the national regulators. Future application of certain methods and techniques for decontamination and dismantling in similar environments might bring an added value to the operators. Paper includes a description of best practices for Nuclear Power Plant VVER type reactors decommissioning. Schedule comparison is given to show how the critical path of certain projects is being managed. Application of the International Standard for Decommissioning Costing (ISDC) methodology provides a uniform method which enables comparison of cost estimates to other nuclear facilities under decommissioning. The cost estimate for the V1 NPP decommissioning has been continuously updated based on more advanced and detailed information on the decommissioning activities and projects. Monitoring of progress of the V1 NPP decommissioning is performed via four key-performance indicators. The Earned Value Management (EVM) methodology is used for evaluating time and cost aspect of decommissioning activities while waste conditioning index is calculated by comparing the actually produced waste to planned values of waste for a respective monitored period. Radiological safety index is assessed by comparison of the personnel records on the individual yearly doses received by each respective employee to the boundary value. (authors)

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DOE OSTI2015

Current limitations and challenges in nanowaste detection, characterisation and monitoring

Highlights: • First review on detection of nanomaterials in complex waste samples. • Focus on nanoparticles in solid, liquid and gaseous waste samples. • Summary of current applicable methods for nanowaste detection and characterisation. • Limitations and challenges of characterisation of nanoparticles in waste. - Abstract: Engineered nanomaterials (ENMs) are already extensively used in diverse consumer products. Along the life cycle of a nano-enabled product, ENMs can be released and subsequently accumulate in the environment. Material flow models also indicate that a variety of ENMs may accumulate in waste streams. Therefore, a new type of waste, so-called nanowaste, is generated when end-of-life ENMs and nano-enabled products are disposed of. In terms of the precautionary principle, environmental monitoring of end-of-life ENMs is crucial to allow assessment of the potential impact of nanowaste on our ecosystem. Trace analysis and quantification of nanoparticulate species is very challenging because of the variety of ENM types that are used in products and low concentrations of nanowaste expected in complex environmental media. In the framework of this paper, challenges in nanowaste characterisation and appropriate analytical techniques which can be applied to nanowaste analysis are summarised. Recent case studies focussing on the characterisation of ENMs in waste streams are discussed. Most studies aim to investigate the fate of nanowaste during incineration, particularly considering aerosol measurements; whereas, detailed studies focusing on the potential release of nanowaste during waste recycling processes are currently not available. In terms of suitable analytical methods, separation techniques coupled to spectrometry-based methods are promising tools to detect nanowaste and determine particle size distribution in liquid waste samples. Standardised leaching protocols can be applied to generate soluble fractions stemming from solid wastes, while micro- and ultrafiltration can be used to enrich nanoparticulate species. Imaging techniques combined with X-ray-based methods are powerful tools for determining particle size, morphology and screening elemental composition. However, quantification of nanowaste is currently hampered due to the problem to differentiate engineered from naturally-occurring nanoparticles. A promising approach to face these challenges in nanowaste characterisation might be the application of nanotracers with unique optical properties, elemental or isotopic fingerprints. At present, there is also a need to develop and standardise analytical protocols regarding nanowaste sampling, separation and quantification. In general, more experimental studies are needed to examine the fate and transport of ENMs in waste streams and to deduce transfer coefficients, respectively to develop reliable material flow models.

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DOE OSTI2019

Characterization and CST Batch Contact Equilibrium Testing of Aged TCCR Tank 10H Batch 1A and 2 Process Supernate Samples

The Tank Closure Cesium Removal (TCCR) system uses ion exchange columns filled with Crystalline Silicotitanate (CST) media to process radioactive waste solutions for the removal of Cs-137. TCCR currently focuses on dissolving Savannah River Site (SRS) Tank 10H waste (primarily sodium saltcake solids) within the tank followed by at-tank ion exchange column treatment. Previous equilibrium batch contact tests conducted in the SRNL Shielded Cells laboratory and associated analyses indicated that CST cesium removal performance was lower than predicted by ZAM modeling for TCCR Tank 10H Production Supernate Batch 1A. An average cesium distribution coefficient of 1,948 mL/g which corresponds to 94.1% Cs + removal was observed for Batch 1A supernate at 38 °C in January of 2019 using laboratory pretreated IONSIV™ R9120-B a CST from Lot #209900034 (predominant TCCR CST batch) at a phase ratio of 122 mL/g. This cesium loading was approximately 32% lower than model predictions, presumably due to ion exchange competition or fouling associated with alkaline earth or transition metals present in the solutions at low levels. The current testing was designed to: 1) evaluate whether supernate compositional changes during storage would result in improved cesium removal performance with CST, and 2) assist in media selection and handling protocols for future TCCR columns by evaluating several CST manufacturer batches as well as samples of one CST batch which had been pretreated using two different methods (field and laboratory methods).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2011

PILOT-SCALE TESTING OF THE SUSPENSION OF MST, CST, AND SIMULATED SLUDGE SLURRIES IN A SLUDGE TANK

The Small Column Ion Exchange (SCIX) process is being developed to remove cesium, strontium, and actinides from Savannah River Site (SRS) Liquid Waste using an existing waste tank (i.e., Tank 41H) to house the process. Following strontium, actinide, and cesium removal, the concentrated solids will be transported to a sludge tank (i.e., monosodium titanate (MST)/sludge solids to Tank 42H or Tank 51H and crystalline silicotitanate (CST) to Tank 40H) for eventual transfer to the Defense Waste Processing Facility (DWPF). Savannah River National Laboratory (SRNL) is conducting pilot-scale mixing tests to determine the pump requirements for mixing MST, CST, and simulated sludge. The purpose of this pilot scale testing is to determine the pump requirements for mixing MST and CST with sludge in a sludge tank and to determine whether segregation of particles occurs during settling. Tank 40H and Tank 51H have four Quad Volute pumps; Tank 42H has four standard pumps. The pilot-scale tank is a 1/10.85 linear scaled model of Tank 40H. The tank diameter, tank liquid level, pump nozzle diameter, pump elevation, and cooling coil diameter are all 1/10.85 of their dimensions in Tank 40H. The pump locations correspond to the current locations in Tank 40H (Risers B2, H, B6, and G). The pumps are pilot-scale Quad Volute pumps. Additional settling tests were conducted in a 30 foot tall, 4 inch inner diameter clear column to investigate segregation of MST, CST, and simulated sludge particles during settling.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Estimation of and barriers to waste heat recovery from harsh environments in industrial processes

This paper discusses the industrial potential for waste heat recovery (WHR) in harsh environments – defined as a waste heat stream having either a temperature of at least 650 °C or containing reactive constituents that complicate heat recovery. The analysis covers five industries (steel, aluminum, glass, cement, and lime), chosen based on volume of production, discharge of exhaust gases containing components that present harsh environments, possibility of recovering considerably more heat than currently recovered, and current lack of acceptable WHR options. The total potential energy savings identified in harsh environment waste heat streams from these industries is equal to 15.4% (113.6 TWh) of the process heat energy lost in U.S. manufacturing. Existing technologies and materials for these industries are evaluated and the recoverable waste heat from harsh environment gas for each industrial sector is estimated. Finally, an in-depth summary of each waste heat source shows exactly where waste heat can be recovered and what specific issues must be addressed. The most potential lies within steel blast furnaces (46 TWh/year). Other waste heat streams considered include steel electric arc furnaces (14.1 TWh/year), flat glass (3.6 TWh/year), container glass (5.7 TWh/year), glass fiber (1.1 TWh/year), specialty glass (2.2 TWh/year), aluminum melting furnaces (4.7 TWh/year), cement (17.1 TWh/year), and lime (10.5 TWh/year). Furthermore attempts to recover waste heat in harsh environments have been mostly unsuccessful, advances in research and technology could unlock an enormous potential for energy and cost savings.

42 ENGINEERING↗

DOE OSTI2023

A Prediction Method for Catchment Efficiency Loss due to Coaxial Nozzle Wear in Powder Fed Directed Energy Deposition Systems

Abstract Powder fed laser directed energy deposition systems show significant promise and their widespread adoption could greatly advance manufacturing technology; however, a significant amount of gas atomized metal powder is wasted during material deposition. As contaminated powder must be collected and disposed of as hazardous waste, this process is often criticized for its low catchment efficiency. This presents potential implementation and scaling issues, as widespread use of this technology would directly increase the amount of contaminated powder in need of safe disposal. A direct contribution to this waste issue was identified in past work as wearing exterior and interior surfaces on a replaceable nozzle component within the additive head of such a system integrated into a hybrid manufacturing machine tool. A computational fluid dynamics simulation is developed specifically for use within the manufacturing process by predicting catchment efficiency losses before a deposition operation is performed. The model is robust enough to calculate a catchment efficiency estimate within a reasonable transition time before deposition and is designed to replace visual estimation of nozzle deterioration by the machine operator. Both of two previously identified wear modes are represented in the simulation. Their effects on powder stream geometry are discussed in detail and the results are compared with in-situ measurements of powder stream geometry and concentrations. The resulting work contributes to the growing understanding of using prediction and prevention methods on catchment efficiency related part defects within these systems.

DeWitte, Lisa↗

DOE OSTI2011

Immobilization of 99-Technetium (VII) by Fe(II)-Goethite and Limited Reoxidation

During the nuclear waste vitrification process volatilized {sup 99}Tc will be trapped by melter off-gas scrubbers and then washed out into caustic solutions, and plans are currently being contemplated for the disposal of such secondary waste. Solutions containing pertechnetate [{sup 99}Tc(VII)O{sub 4}{sup -}] were mixed with precipitating goethite and dissolved Fe(II) to determine if an iron (oxy)hydroxide-based waste form can reduce Tc(VII) and isolate Tc(IV) from oxygen. The results of these experiments demonstrate that Fe(II) with goethite efficiently catalyzes the reduction of technetium in deionized water and complex solutions that mimic the chemical composition of caustic waste scrubber media. Identification of the phases, goethite + magnetite, was performed using XRD, SEM and TEM methods. Analyses of the Tc-bearing solid products by XAFS indicate that all of the Tc(VII) was reduced to Tc(IV) and that the latter is incorporated into goethite or magnetite as octahedral Tc(IV). Batch dissolution experiments, conducted under ambient oxidizing conditions for more than 180 days, demonstrated a very limited release of Tc to solution (2-7 {micro}g Tc/g solid). Incorporation of Tc(IV) into the goethite lattice thus provides significant advantages for limiting reoxidation and curtailing release of Tc disposed in nuclear waste repositories.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2011

Radioactive Demonstration of Final Mineralized Waste Forms for Hanford Waste Treatment Plant Secondary Waste (WTP-SW) by Fluidized Bed Steam Reforming (FBSR) using the Bench Scale Reformer Platform

The U.S. Department of Energy's Office of River Protection (ORP) is responsible for the retrieval, treatment, immobilization, and disposal of Hanford's tank waste. Currently there are approximately 56 million gallons of highly radioactive mixed wastes awaiting treatment. A key aspect of the River Protection Project (RPP) cleanup mission is to construct and operate the Waste Treatment and Immobilization Plant (WTP). The WTP will separate the tank waste into high-level and low-activity waste (LAW) fractions, both of which will subsequently be vitrified. The projected throughput capacity of the WTP LAW Vitrification Facility is insufficient to complete the RPP mission in the time frame required by the Hanford Federal Facility Agreement and Consent Order, also known as the Tri-Party Agreement (TPA), i.e. December 31, 2047. Therefore, Supplemental Treatment is required both to meet the TPA treatment requirements as well as to more cost effectively complete the tank waste treatment mission. In addition, the WTP LAW vitrification facility off-gas condensate known as WTP Secondary Waste (WTP-SW) will be generated and enriched in volatile components such as 137 Cs, 129 I, 99 Tc, Cl, F, and SO 4 that volatilize at the vitrification temperature of 1150°C in the absence of a continuous cold cap (that could minimize volatilization). The current waste disposal path for the WTP-SW is to process it through the Effluent Treatment Facility (ETF). Fluidized Bed Steam Reforming (FBSR) is being considered for immobilization of the ETF concentrate that would be generated by processing the WTP-SW. The focus of this current report is the WTP-SW. FBSR offers a moderate temperature (700-750°C) continuous method by which WTP-SW wastes can be processed irrespective of whether they contain organics, nitrates, sulfates/sulfides, chlorides, fluorides, volatile radionuclides or other aqueous components. The FBSR technology can process these wastes into a crystalline ceramic (mineral) waste form. The mineral waste form that is produced by co-processing waste with kaolin clay in an FBSR process has been shown to be as durable as LAW glass. Monolithing of the granular FBSR product is being investigated to prevent dispersion during transport or burial/storage, but is not necessary for performance. A Benchscale Steam Reformer (BSR) was designed and constructed at the SRNL to treat actual radioactive wastes to confirm the findings of the non-radioactive FBSR pilot scale tests and to qualify the waste form for applications at Hanford. BSR testing with WTP SW waste surrogates and associated analytical analyses and tests of granular products (GP) and monoliths began in the Fall of 2009, and then was continued from the Fall of 2010 through the Spring of 2011. Radioactive testing commenced in 2010 with a demonstration of Hanford's WTP-SW where Savannah River Site (SRS) High Level Waste (HLW) secondary waste from the Defense Waste Processing Facility (DWPF) was shimmed with a mixture of 125/129 I and 99 Tc to chemically resemble WTP-SW. Prior to these radioactive feed tests, non-radioactive simulants were also processed. Ninety six grams of radioactive granular product were made for testing and comparison to the non-radioactive pilot scale tests. The same mineral phases were found in the radioactive and non-radioactive testing.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS1994

Suitability of Gray Water for Hydroponic Crop Production Following Biological and Physical Chemical and Biological Subsystems

The water present in waste streams from a human habitat must be recycled in Controlled Ecological Life Support Systems (CELSS) to limit resupply needs and attain self-sufficiency. Plants play an important role in providing food, regenerating air, and producing purified water via transpiration. However, we have shown that the surfactants present in hygiene waste water have acute toxic effects on plant growth (Bubenheim et al. 1994; Greene et al., 1994). These phytotoxic affects can be mitigated by allowing the microbial population on the root surface to degrade the surfactant, however, a significant suppression (several days) in crop performance is experienced prior to reaching sub-toxic surfactant levels and plant recovery. An effective alternative is to stabilize the microbial population responsible for degradation of the surfactant on an aerobic bioreactor and process the waste water prior to utilization in the hydroponic solution (Wisniewski and Bubenheim, 1993). A sensitive bioassay indicates that the surfactant phytotoxicity is suppressed by more than 90% within 5 hours of introduction of the gray water to the bioreactor; processing for more than 12 hours degrades more than 99% of the phytotoxin. Vapor Compression Distillation (VCD) is a physical / chemical method for water purification which employees sequential distillation steps to separate water from solids and to volatilize contaminants. The solids from the waste water are concentrated in a brine and the pure product water (70 - 90% of the total waste water volume depending on operating conditions) retains non of the phytotoxic effects. Results of the bioassay were used to guide evaluations of the suitability of recovered gray water following biological and VCD processing for hydroponic lettuce production in controlled environments. Lettuce crops were grown for 28 days with 100% of the input water supplied with recovered water from the biological processor or VCD. When compared with the growth of plants in control hydroponic solution containing pure deionized water, no growth difference could be measured resulting from any of the recovered water treatments. Both biological treatment and VCD offer alternative technology approaches to recovering water from waste streams appropriate for input into a crop production system. A high level of crop performance (food, air, and water production) can be maintained with either processor; selection decisions can be based on other factors regarding system integration.

Bubenheim, David L.↗