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DOE OSTI2015

Literature Review: Assessment of DWPF Melter and Melter Off-gas System Lifetime

A glass melter for use in processing radioactive waste is a challenging environment for the materials of construction (MOC) resulting from a combination of high temperatures, chemical attack, and erosion/corrosion; therefore, highly engineered materials must be selected for this application. The focus of this report is to review the testing and evaluations used in the selection of the Defense Waste Processing Facility (DWPF), glass contact MOC specifically the Monofrax ® K-3 refractory and Inconel ® 690 alloy. The degradation or corrosion mechanisms of these materials during pilot scale testing and in-service operation were analyzed over a range of oxidizing and reducing flowsheets; however, DWPF has primarily processed a reducing flowsheet (i.e., Fe 2+ /ΣFe of 0.09 to 0.33) since the start of radioactive operations. This report also discusses the materials selection for the DWPF off-gas system and the corrosion evaluation of these materials during pilot scale testing and non-radioactive operations of DWPF Melter #1. Inspection of the off-gas components has not been performed during radioactive operations with the exception of maintenance because of plugging.

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DOE OSTI2015

Literature Review: Assessment of DWPF Melter and Melter Off-gas System Lifetime

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DOE OSTI2015

Seismic design of a nuclear waste repository against an earthquake induced rock shear load - 15346

Concepts for isolation of spent nuclear fuel have been studied by organizations in countries that employ nuclear power. These concepts typically involve a deep geological repository in bedrock, with processed radioactive waste encased in deposition canisters emplaced in underground excavations and surrounded by clay-based buffer. This multi-barrier approach is intended to provide long-term isolation of the waste package from the biosphere. According to many statistics, there is a tendency toward increasing numbers of earthquakes in the Korean peninsula each year. If an earthquake induced rock shear load occurs at a repository site, the engineered barrier system (EBS) can be sheared, resulting in a pressure increased in the buffer material. This is expected to result in damage to the canisters. Therefore, because the damage, which can be fatal to a disposal canister, can be given in case an earthquake occurs, the method protecting the canisters safely is needed. In this paper, 'an earthquake-resistance type buffer' was proposed using a method for protection from earthquake damage. To aid in achieving this objective, we have developed a technique for estimating the behavior of the EBS affected by earthquake induced rock shear using an analysis method, such as finite element method. As a first step, experimental tests are performed for understanding the behavior of the buffer material. Comparing the results of the numerical simulations to the experimental results can be used to verity the reliability of the analysis model. Then we developed the real scale analysis model of a nuclear waste repository. The main parameter having an effect on the earthquake-resistant performance was analyzed and an earthquake-resistance proof type buffer was designed. To improve the earthquake-resistance performance, we designed the buffer by putting the low- density buffer between the canister and buffer. The simulation results show that the earthquake-resistant performance was improved by about 65%. (authors)

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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).

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DOE OSTI2017

Nuclear Liquid Wastes Calcination: The High-Level French Experience - 17184

Calcination is an efficient process for volume reduction and stabilization of nuclear liquid wastes. It is often the first step of waste containment processes such as vitrification or grouting. The CEA (French Alternative Energies and Atomic Energy Commission) and AREVA have acquired a high-level experience in the field of calcination through more than forty years of R and D and industrial operation. During this period, a broad range of liquid wastes have been studied and treated. R and D work and associated engineering studies allowed defining the design and sizing of the equipment and the process control parameters to be applied for the calcination of all kinds of solutions. The calcination process has been qualified for the following effluents amongst others: - Liquid waste from UOx fuel reprocessing; - Liquid waste from UMo fuel reprocessing (high molybdenum and phosphorus contents); - Hanford HLW; - Liquid waste from D and D operation (sodium bearing waste). This paper presents several studies led by the Joint Vitrification Laboratory (L.C.V), a common research laboratory between CEA and AREVA in charge of qualifying new processes and matrices for waste containment. These studies allowed defining the calcination rules, in particular for very hard to process solutions such as effluents with high boron, molybdenum and sodium contents. The feedback from industrial operation of the calcination process with fission products and effluents from D and D operations, highly loaded with sodium, is also presented. (authors)

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DOE OSTI2018

Inorganic Ba-Sn Nanocomposite Materials for Sulfate Sequestration from Complex Aqueous Solutions

Selective sequestration of sulfate (SO42-) in the form of barite (BaSO4) from alkaline solutions of high ionic strength containing carbonate at high concentrations resembling legacy radioactive waste generated during plutonium cold war era production is problematic due to the preferential formation of BaCO3. Incorporation of sulfate into the insoluble and thermally stable BaSO4 phase can potentially benefit radioactive waste processing in reducing operational challenges and suppressing volatilization of other waste components such as technetium-99. To enhance selectivity of SO42- sequestration, a series of Ba(II)-Sn(IV) materials was prepared using simple hydrothermal synthesis from different Sn(II) and Sn(IV) precursors. Structural characterization indicated that all obtained products predominantly contained BaSn(OH)6 and Ba2SnO2(OH)4(H2O)10 crystalline phases which were disrupted upon exposure to SO42- due to formation of BaSO4. Performance of the Ba(II)-Sn(IV) materials was tested using complex alkaline solutions simulating radioactive waste containing 0.094 M SO42- and 0.5 M CO32- among other constituents. About 54 – 66% of SO42- was converted to BaSO4 when a quantity of Ba(II)-Sn(IV) material containing approximately a stoichiometric amount of Ba2+ relative to SO42- was used. In comparison, previous studies indicate negligible BaSO4 formation under similar conditions when a simple Ba2+ salt is used. This improvement is attributed to the selective replacement of the Ba(II) stannate by SO42-. Thermal stability of the sulfate-loaded product material up to 1100 °C was demonstrated. Obtained materials offer a convenient and economical option for the selective sequestration or removal of SO42- from carbonate containing solutions.

Johnson, Isaac↗

DOE OSTI2020

Development of Guidance for the Disposition of Used Oil and Oil Samples at the Columbia Generating Station - 20232

It is a fact that oil can become contaminated during plant operations. When used oil is collected, the water is decanted from the used oil. The separated used oil is typically analyzed for gamma emitting radionuclides and then sent off-site for processing (incineration) or recycling. If there is no detectable radioactivity, then some plants may release the oil for unrestricted use. Many nuclear power plants have no standard process for evaluating Tritium and Carbon-14 in oil; therefore, there may be variability in how plants are determining whether oil contains Tritium and Carbon-14, and at what concentration. Questions may arise whether there is a technically sound basis and evaluation method for used oil and if process knowledge and/or sampling may be appropriate in making that determination. Recently, there has been an increase in regulatory scrutiny regarding these practices to ensure that the utilities are evaluating oil for all plant-produced radionuclides prior to free release. Regulators have indicated that the requirement to conduct adequate surveys should include evaluating oils for Tritium and Carbon-14. (authors)

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DOE OSTI2021

Proton Nuclear Magnetic Resonance (H NMR) of Glycolate in Real Waste: Developing and Testing Analytical Methods for the Savannah River Site Liquid Waste System

In preparation for implementing the NG acid flowsheet for the SRS LWS, analytical methods for determining glycolate at low concentration are desired to support system management and safety. Previous work documented that the IC method performed well for samples with low to moderate ionic strength. That work also included a scoping effort to determine if an alternate analytical strategy using H NMR would complement and extend the capabilities of the IC method. The H NMR scoping results indicated that the method had the potential to expand glycolate analysis in LWS samples to higher ionic strength tanks/solutions. The scope of this work is to develop innovative proton NMR techniques, including demonstrating ion exchange decontamination protocols needed for application of the technique to real waste samples. Part of radioactive waste processing at SRS uses formic acid to reduce oxidized (Hg 2+ ) to more volatile elemental Hg for steam striping, collecting, and disposal. Under acidic conditions found in the Chemical Processing Cell (CPC) at the Defense Waste Processing Facility (DWPF), formic acid has a much higher hydrogen generation rate than an alternative reductant, glycolic acid. Thus, an NG acid flowsheet has been developed utilizing glycolic acid with the benefit of easing the need for headspace monitoring requirements for hydrogen and ammonia at DWPF. Low concentrations of glycolate are conservatively assumed to be in the recycle stream, which will collect in the Recycle Collection Tank (RCT). The DWPF recycle stream collected in the RCT has a distinct pathway to the LWS waste tanks that feed the 2H and 3H Evaporator. This route involves transfer of the DWPF recycle to Tank 22 in the Concentration, Storage, and Transfer Facilities (CSTF) followed by transfer to the LWS tank farm/evaporators.

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DOE OSTI2013

Overview of reductants utilized in nuclear fuel reprocessing/recycling

The most widely used reductant to partition plutonium from uranium in the Purex process was ferrous sulfamate, other alternates were proposed such as hydrazine-stabilized ferrous nitrate or uranous nitrate, platinum catalyzed hydrogen, and hydrazine, hydroxylamine salts. New candidates to replace hydrazine or hydroxylamine nitrate (HAN) are pursued worldwide. They may improve the performance of the industrial Purex process towards different operations such as de-extraction of plutonium and reduction of the amount of hydrazine which will limit the formation of hydrazoic acid. When looking at future recycling technologies using hydroxamic ligands, neither acetohydroxamic acid (AHA) nor formohydroxamic acid (FHA) seem promising because they hydrolyze to give hydroxylamine and the parent carboxylic acid. Hydroxyethylhydrazine, HOC{sub 2}H{sub 4}N{sub 2}H{sub 3} (HEH) is a promising non-salt-forming reductant of Np and Pu ions because it is selective to neptunium and plutonium ions at room temperature and at relatively low acidity, it could serve as a replacement of HAN or AHA for the development of a novel used nuclear fuel recycling process.

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DOE OSTI2017

SRR's 'Next Step' in the Lean Journey -Taking Lean to the Workforce - 17247

The Savannah River Site, a U.S. Department of Energy (DOE) facility, contracted Savannah River Remediation (SRR) to manage its liquid waste project, which is a unique, high hazard nuclear waste treatment and disposal facility consisting of 51, one million-gallon underground waste tanks, a solvent extraction processing unit, a vitrification facility for the highest radioactive waste, and a grout solidification and disposal facility for a decontaminated salt solution. Our Project mission is to treat the nuclear waste and close the associated storage and treatment facilities, of which, 8 tanks have been closed to date. At SRR, the Lean business management system has been adopted to address site inefficiencies, aging infrastructure concerns and budget constraints. The Lean philosophy took root decades ago in the manufacturing sector and started with the work of W. Edwards Deming and his contemporaries. In more recent years the process has matured in the Toyota Production System and migrated into fields as diverse as services industries, health-care, and now the DOE complex. The first step of the SRR Lean Journey was to formally identify areas of improvement and initiate Value Stream Analysis (VSAs) and Rapid Improvement Events (RIEs). SRR has achieved improvements in procedure implementation, work planning and control, project schedule compression, and engineering requirements. SRR is now phasing in the next phase of Lean through Managing for Daily Improvement (MDI), Visual Management and 5S (sort, set in order, shine, standardize, and sustain). MDI is a fundamental Lean principle in that we use our most valuable asset, our employees, to drive continuous improvement versus a smaller population through formal events. Part of MDI includes visual management where the workforce can go to a 'dashboard' to see and understand the company mission and status. 5S is a process where a work group improves performance in an area by addressing physical organization, efficiency, uniformity, standardization, and mechanisms to sustain improvements. 5S stands for: Sort, Set in Order, Shine, Standardize, and Sustain. This paper will focus on the 'Next Step' in SRR's Lean journey by address how SRR is implementing MDI and 5S to improve CONOPs, Project efficiencies, and worker engagement in day to day operations. (authors)

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DOE OSTI2017

Savannah River Remediation Liquid Waste Operations Making the Workplace Safer - Lean and Human Performance Improvement Initiatives - 17244

The Savannah River Site, a U.S. Department of Energy facility, contracted Savannah River Remediation (SRR) to manage its liquid waste project, which is a unique, high hazard nuclear waste treatment and disposal facility consisting of 51, one million gallon underground waste tanks, a solvent extraction processing unit, a vitrification facility for the highest radioactive waste, and a grout solidification and disposal facility for a decontaminated salt solution. Our Project mission is to treat the nuclear waste and close the associated storage and treatment facilities, of which, 8 of the 51 tanks have been closed to date. Over the past three years, SRR implemented a Lean Business Management System to address site inefficiencies, aging infrastructure concerns and budget constraints. The Lean philosophy started with the work of W. Edwards Deming and his contemporaries. In more recent years the process has matured in the Toyota Production System and migrated into fields as diverse as services industries, health-care, and now the DOE complex. Like safety, continuous improvement is a fundamental core business value that starts at the top. The Lean Business System, led by our executive management team, drives quality, production and waste elimination by focusing on People using a structured Process that allows the workforce to identify and fix problems in their workplace. Many inefficiencies and quality related issues start with the desire to make systems fail-safe without defining the core requirements for which that process or program was created. This leads to added complexity and latent or inherent human performance issues embedded within our processes. While Lean can't fix all problems, a combination of strong nuclear safety culture, robust conduct of operations, active human performance improvement process, and a business practice of continuously looking for improvements leads to excellence across our industry and creates a culture that is worthy of promoting. Without strong management, our systems fail because no one sponsors or encourages those attributes we covet. Leadership starts at the top with our customer defining what provides 'value' to them, and filters down through to the organization and ultimately the workforce in day to day conduct of operations. It is imperative that our customer drives these desirable ideals through recognition and contractual requirements to encourage and support those behavioral traits that are critical to our ongoing success.This paper focuses on how the Lean Business Management System supports those attributes that we value: a strong nuclear safety culture; disciplined conduct of operations; and a culture of robust human performance and continuous improvement. These attributes in our daily work environment propel a safer, more consistent, more efficient workplace. (authors)

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DOE OSTI2016

Progress Update on the Waste Treatment and Immobilization Plant Pulse- Jet Mixed Vessel Testing Program - 16286

The Waste Treatment and Immobilization Plant (WTP) is designed to use cylindrical-shaped pulse-jet mixers in the black cell vessels to mix the radioactive waste during process operations. Pulse-jet mixers operate like large turkey basters, using air pressure to suck radioactive waste up into the mixer and eject it back into the vessel at high velocity. Using pulse-jet mixers for keeping waste in process vessels adequately mixed is one of the design features that ensures that there are no mechanical parts inside the black cells that would require maintenance. The WTP Project is conducting a testing program to ensure the pulse-jet mixed vessels can address three design and nuclear safety concerns: 1) pulse jet mixer controls, 2) hydrogen gas generation, and 3) the potential for inadvertent criticality in the vessels. The currently planned pulse-jet mixed vessel testing program is divided into three major test campaigns. The first campaign consists of testing to demonstrate pulse-jet mixed vessel control system design and operating concepts. The second test campaign consisted of informational testing of select prototypic PJM vessel features in a reduced scale facility. This testing informed decision making on selection of different mixing system configurations. This test campaign was completed in March 2015. The third test campaign is planned to test the complete functionality of a pulse-jet mixed vessel at full-scale using a prototype standardized high-solids vessel design. (authors)

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DOE OSTI2016

Immobilization of Organic Radioactive and Non-Radioactive Liquid Waste in a Composite Matrix - Final CRADA Report

Treatment and safe disposal of liquid radioactive waste from the BN-350 reactor unit at the LRW Processing Facility, Kazakhstan

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DOE OSTI2013

Development of a Performance and Processing Property Acceptance Region for Cementitious Low-Level Waste Forms at Savannah River Site - 13174

The Saltstone Production and Disposal Facilities (SPF and SDF) at the Savannah River Site (SRS) have been treating decontaminated salt solution, a low-level aqueous waste stream (LLW) since facility commissioning in 1990. In 2012, the Saltstone Facilities implemented a new Performance Assessment (PA) that incorporates an alternate design for the disposal facility to ensure that the performance objectives of DOE Order 435.1 and the National Defense Authorization Act (NDAA) of Fiscal Year 2005 Section 3116 are met. The PA performs long term modeling of the waste form, disposal facility, and disposal site hydrogeology to determine the transport history of radionuclides disposed in the LLW. Saltstone has been successfully used to dispose of LLW in a grout waste form for 15 years. Numerous waste form property assumptions directly impact the fate and transport modeling performed in the PA. The extent of process variability and consequence on performance properties are critical to meeting the assumptions of the PA. The SPF has ensured performance property acceptability by way of implementing control strategies that ensure the process operates within the analyzed limits of variability, but efforts continue to improve the understanding of facility performance in relation to the PA analysis. A similar understanding of the impact of variability on processing parameters is important from the standpoint of the operability of the production facility. The fresh grout slurry properties (particularly slurry rheology and the rate of hydration and structure formation) of the waste form directly impact the pressure and flow rates that can be reliably processed. It is thus equally important to quantify the impact of variability on processing parameters to ensure that the design basis assumptions for the production facility are maintained. Savannah River Remediation (SRR) has been pursuing a process that will ultimately establish a property acceptance region (PAR) to incorporate elements important to both processability and long-term performance properties. This process involves characterization of both emplaced product samples from the disposal facility and laboratory-simulated samples to demonstrate the effectiveness of the lab simulation. With that basis confirmed, a comprehensive variability study using non-radioactive simulants will define the acceptable PAR, or 'operating window' for Saltstone production and disposal. This same process will be used in the future to evaluate new waste streams for disposal or changes to the existing process flowsheet. (authors)

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DOE OSTI2013

Processing of solid low level alpha suspected radioactive waste

Incineration of low active waste is the most efficient way to obtain high volume reduction factors. Although the initial scenario for processing low active alpha suspected waste (α- activity ≤ 400 MBq/m{sup 3}) in Belgium was supercompaction, incineration was eventually chosen for various benefits concerning volume reduction as well as the elimination of organic compounds improving the long term performance. This specific type of waste is often contaminated with for example mercury, requiring special attention in the treatment of both off-gas en waste water. In this paper it is shown that the CILVA incinerator of Belgoprocess N.V. has a high efficiency to combine both incineration and supercompaction of such types of waste. (authors)

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DOE OSTI2015

Advanced High-Level Waste Glass Research and Development Plan

The U.S. Department of Energy Office of River Protection (ORP) has implemented an integrated program to increase the loading of Hanford tank wastes in glass while meeting melter lifetime expectancies and process, regulatory, and product quality requirements. The integrated ORP program is focused on providing a technical, science-based foundation from which key decisions can be made regarding the successful operation of the Hanford Tank Waste Treatment and Immobilization Plant (WTP) facilities. The fundamental data stemming from this program will support development of advanced glass formulations, key process control models, and tactical processing strategies to ensure safe and successful operations for both the low-activity waste (LAW) and high-level waste (HLW) vitrification facilities with an appreciation toward reducing overall mission life. The purpose of this advanced HLW glass research and development plan is to identify the near-, mid-, and longer-term research and development activities required to develop and validate advanced HLW glasses and their associated models to support facility operations at WTP, including both direct feed and full pretreatment flowsheets. This plan also integrates technical support of facility operations and waste qualification activities to show the interdependence of these activities with the advanced waste glass (AWG) program to support the full WTP mission. Figure ES-1 shows these key ORP programmatic activities and their interfaces with both WTP facility operations and qualification needs. The plan is a living document that will be updated to reflect key advancements and mission strategy changes. The research outlined here is motivated by the potential for substantial economic benefits (e.g., significant increases in waste throughput and reductions in glass volumes) that will be realized when advancements in glass formulation continue and models supporting facility operations are implemented. Developing and applying advanced glass formulations will reduce the cost of Hanford tank waste management by reducing the schedule for tank waste treatment and reducing the amount of HLW glass for storage, transportation, and disposal. Additional benefits will be realized if advanced glasses are developed that demonstrate more tolerance for key components in the waste (such as Al 2 O 3 , Cr 2 O 3 , SO 3 and Na 2 O) above the currently defined WTP constraints. Tolerating these higher concentrations of key waste loading limiters may reduce the burden on (or even eliminate the need for) leaching to remove Cr and Al and washing to remove excess S and Na from the HLW fraction. Advanced glass formulations may also make direct vitrification of the HLW fraction without significant pretreatment more cost effective. Finally, the advanced glass formulation efforts seek not only to increase waste loading in glass, but also to increase glass production rate. When coupled with higher waste loading, ensuring that all of the advanced glass formulations are processable at or above the current contract processing rate leads to significant improvements in waste throughput (the amount of waste being processed per unit time),which could significantly reduce the overall WTP mission life. The integration of increased waste loading, reduced leaching/washing requirements, and improved melting rates provides a system-wide approach to improve the effectiveness of the WTP process.

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DOE OSTI2016

Experience with the Quality Control of Radioactive Waste Packages for the German Repository Konrad - 16493

The German repository Konrad for radioactive waste with negligible heat generation is designed to accept 303,000 m{sup 3} of waste packages in total. Based on the Konrad licensing conditions, any treatment and conditioning of radioactive waste should be planned and carried out in accordance with the waste acceptance requirements of the repository Konrad in order to produce waste packages suitable for disposal. The qualification of the waste treatment processes and the resulting products are achieved by interaction of different parties involved. On behalf of the Federal Office for Radiation Protection - the competent German authority for disposal of radioactive waste - TUV NORD EnSys Hannover GmbH and Co. KG acts as one of the independent expert organizations for more than twenty years in the field of qualification of waste treatment campaigns and review of waste packages documentations. The permitted amount of nuclide activity in the radioactive waste packages depends on the characteristics of the radioactive waste products. Projecting a suitable strategy for loading the waste containers contributes to determine in advance, what requirements the radioactive waste products have to fulfill as well as what properties of the waste products need to be verified and documented during conditioning or treatment process. On the basis of various examples, it is being demonstrated how appropriate advance process planning can ensure that radioactive waste packages are generated to comply with the waste acceptance requirements. In consequence, technical measures due to requalification can be avoided even in case of unpredictable difficulties. (authors)

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DOE OSTI2018

Conception and Operation of a New Treatment Center for Radioactive Waste from High Energy Accelerators - 18293

CERN has operated high-energy accelerators for more than 60 years of research in fundamental physics. The side-product of this activity is the generation of low- and intermediate-level radioactive waste, most of which is in solid form and free of surface contamination. Today, one operational year produces about 400 tons of radioactive waste which need to be disposed of towards the final repositories of the two CERN Host States, France and Switzerland. A new facility for the collection, interim storage, characterization and treatment of radioactive waste became operational at CERN in 2015. This facility was specifically conceived for an accelerator complex with a wide range of challenging waste items, which are often unique in their irradiation history as well as in their physical, chemical and radiological characteristics. The disposal rate was ramped up in 2016 with a unique treatment process tailored for metallic low-level waste. In 2017, two parallel processes were successfully tested for the elimination of radioactive cables and for the recycling of valuable metals. This paper gives an overview of the challenges in the design, commissioning and operation of the CERN radioactive waste treatment center. It outlines the methodology followed for the conception of the elimination processes, which can be of guidance for the development of similar facilities. (authors)

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