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DOE OSTI2019

AP-105 Melter Offgas Condensate and EMF Evaporator Concentrate Raman and LIBS Qualitative Evaluation for the use of In-Line Monitoring (Rev. 0)

The Pacific Northwest National Laboratory (PNNL) was tasked to perform Raman spectroscopy and laser induced breakdown spectroscopy (LIBS) testing on the melter off-gas condensate generated during low-activity waste process testing of a sample from Hanford Site tank AP-105 and/or evaporate from evaporation of the condensate. This was a proof-of-principle demonstration that Raman spectroscopy and LIBS have the potential to be used as analytical tools for in-line process analysis of key aqueous phase analytes in radioactive process streams associated with the Hanford Waste Treatment and Immobilization Plant. The work completed under this project complements work completed for WRPS with the development of in-line monitoring systems to characterize and quantify constituents of tank waste following Cs removal and filtration. The WRPS work is currently limited to Raman sensors and utilizes chemometric models for quantification of several anionic species in the sample system. It should be noted that while this approach can be applied to off-gas condensate streams, new chemometric models are needed to accurately quantify analytes under off-gas condensate conditions. The work completed under this project makes timely use of available samples and equipment at PNNL. The project utilized the opportunity to collect off-gas samples from planned AP-105 processing work and included the direct condensate and the evaporate from the DFLAW Radioactive Waste Test Platform. Samples were characterized by instruments already in place at PNNL including a Raman spectrometer optimized for in-line monitoring of flowing and stationary samples as well as a LIBS instrument, which was optimized for static liquid droplet analysis. The ultimate objective was to determine if these techniques could be used to qualitatively characterize analytes present within the off-gas samples. The testing confirmed the use of the Raman as an in-line monitoring system was able to qualitatively observe NO 3 - , NO 2 - , aluminum (as aluminate, Al(OH) 4 - ), SO 4 2- , CrO 4 2- , CO 3 2- , and PO 4 3- in the AP-105 melter feed evaporator condensate samples. The testing also confirmed LIBS as a potential useful technique for in-line monitoring, able to qualitatively detect Na, N, Al, and tentatively Cr and Cl in a simulant stock evaporate solution.

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DOE OSTI2013

The analysis of metal melting application in the management of metallic radioactive materials arising from decommissioning of nuclear installations

Basic characterization of the waste management process during decommissioning of nuclear installations is described in the presented paper. A brief description is given of conditional and unconditional release of materials into the environment. The paper deals also with metal melting as prospective decontamination technique which can significantly reduce metallic radioactive waste. The material and radioactivity flow in the decommissioning process should be followed using the integrated material flow tool that is implemented into the standardized analytical decommissioning parameters calculation code OMEGA. Applying the integrated material flow tool, it is possible to monitor radiological and physical properties of individual material items listed in the nuclear installation input database, from dismantling up to their release into the environment or disposal in repository. Using the OMEGA code and two model databases, several scenarios related to metal melting are evaluated. The impact of applying different input decommissioning parameters on the metal distribution is the main result discussed in the paper. (authors)

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DOE OSTI2019

Permanganate Oxidation of Defense Waste Processing Facility (DWPF) Recycle Collection Tank (RCT) Simulants Larger Scale Protocol Runs - Chemical Process Cell (CPC) Nominal and Foamover Conditions

Testing to develop a process to oxidize glycolate and other organic species in non-radioactive waste simulants was requested by Savannah River Remediation (SRR). A Task Technical and Quality Assurance Plan (TTQAP) was written to describe the testing requested by SRR in the development of a process to oxidize glycolate and other organic species that are responsible for hydrogen generation from thermolysis. Scoping studies have been completed as requested by a Technical Assistance Request (TAR) to evaluate the feasibility of using sodium permanganate and Fenton's Reagent (iron catalyzed hydrogen peroxide) for destroying glycolate. The results from these scoping studies were summarized in a report. Six phases of tests with simulants have been planned in developing an oxidation flowsheet for the Recycle Collection Tank (RCT), as shown in Table 1. The first three phases have been completed. The first phase comprised of scoping tests of permanganate and Fenton's reagent. The second phase was a matrix of 23 tests completed to inform a down-select decision by SRR and to complete testing needed to understand the influence of various factors in defining the optimum processing conditions for oxidation of organics. From the results of this testing, oxidation by permanganate was chosen over Fenton's reagent with hydrogen peroxide. The third phase of testing was to demonstrate nominal operation of the permanganate oxidation process under protocols similar to those used in the Defense Waste Processing Facility (DWPF).

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DOE OSTI2016

Port Hope Area Initiative - Community Based Concepts Become Reality - 16538

The Port Hope Area Initiative (PHAI) involves the cleanup of historic low-level radioactive waste (LLRW) resulting from radium and uranium processing by the former Crown Corporation, Eldorado Nuclear Limited, and its predecessor companies, during the period between 1932 and 1988. The PHAI, which is based on a legal agreement between the Government of Canada and the adjacent municipalities of Port Hope and Clarington in Ontario, Canada, comprises two separate community-initiated projects for the long-term management of the historic LLRW located in each of these municipalities. The Port Hope Project involves the cleanup of approximately 1.2 million cubic metres of historic LLRW from various sites within the urban area of Port Hope, the construction and operation of an engineered aboveground mound where the waste will be safely contained, and the long-term maintenance and monitoring of the new waste management facility. The waste is currently located in 13 large-scale sites and an estimated 375 small-scale sites within the community. In contrast, the Port Granby Project involves the relocation of approximately 450,000 cubic metres of historic LLRW from the existing waste site on the north shore of Lake Ontario in rural Clarington, to a new engineered aboveground mound to be built 700 metres north of the shoreline. The work also involves the restoration of the existing site and long-term maintenance and monitoring the new facility. The PHAI entered Phase 2 (construction) of a three-phase program in early 2012, when $1.28 billion (Canadian) in federal funding was announced by the Minister of Natural Resources Canada. The funding, together with regulatory approval from the Canadian Nuclear Safety Commission (CNSC), which granted 10-year waste management licences to both projects, have permitted the PHAI to move forward with construction and remediation. Waste water treatment plants based on best-available technologies have been constructed for each project to remove a wide range of contaminants from groundwater, surface water and leachate collected during construction and operation of the aboveground mounds. Each treatment process has been designed to ensure the quality of treated water being discharged into Lake Ontario meets or exceeds stringent regulatory requirements, resulting in the enhanced protection of the Great Lakes Basin ecosystem. In 2015, the contract to build the Port Granby long-term waste management facility and remediate the existing waste site was awarded, and the long-awaited facility development will soon begin. The use of a dedicated internal waste transportation route along, which the LLRW will be trucked from the existing site to the new facility, is a key component of the design to minimize the impact on the local, rural community. In Port Hope, the removal of contaminated soil within the site for the new long-term management facility commenced in the fall of 2015. Over the next several years, multiple contracts will be awarded for construction and operation of the new waste management facility and remediation of the large and small-scale sites. In short, the Port Hope and Port Granby community-based concepts have matured into tangible projects with appropriate regulatory approvals and federal funding in place. Ongoing communications with the two communities have resulted in a well-informed public that understands the work to be done and is eager to see their projects take shape and become reality. As Canada's largest environmental remediation and restoration undertaking, the PHAI has never been closer to fulfilling its vision - working with the local communities to fulfil Canada's commitment for the cleanup of historic waste in Port Hope and Port Granby to leave an honourable legacy for future generations. (authors)

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DOE OSTI2016

Laboratory-scale integrated ARP filter test

The Savannah River Site (SRS) is currently treating radioactive liquid waste with the Actinide Removal Process (ARP) and the Modular Caustic Side Solvent Extraction Unit (MCU). Recently, the low filter flux through the ARP of approximately 5 gallons per minute has limited the rate at which radioactive liquid waste can be treated. Salt Batch 6 had a lower processing rate and required frequent filter cleaning. There is a desire to understand the causes of the low filter flux and to increase ARP/MCU throughput. This task attempted to simulate the entire ARP process, including multiple batches (5), washing, chemical cleaning, and blending the feed with heels and recycle streams. The objective of the tests was to determine whether one of these processes is causing excessive fouling of the crossflow or secondary filter. The authors conducted the tests with feed solutions containing 6.6 M sodium Salt Batch 6 simulant supernate with no MST.

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DOE OSTI2012

Operation of Bubblers in the Savannah River Site Defense Waste Processing Facility Melter - 12166

Savannah River Remediation (SRR) LLC acquired the liquid waste contract at the Savannah River Site (SRS) in the summer of 2009. In order to achieve the main goal of the contract, closing of High Level Waste (HLW) tanks, it was necessary to process more waste throughout the SRS liquid waste facilities. The Defense Waste Processing Facility (DWPF) would need to increase its production rate of radioactive waste glass filled canisters as a part of the plan to achieve this commitment. To attain the increased production rate, four bubblers were installed in the DWPF Melter in September 2010 to agitate the DWPF Melter glass pool. The four bubblers were designed to be installed in existing nozzles on the top-head of the DWPF Melter. The design and fabrication of the four (4) bubblers was accomplished through SRR critical subcontractor EnergySolutions LLC. In addition to the existing bubbler design, a new design concept has been approved and is in the process of fabrication. The new design will allow for the lower end (inside melter) of the bubbler to be replaced while the upper end (outside melter) of the bubbler is reused to minimize cost and waste at the DWPF. The bubblers have been operating in the DWPF Melter for approximately 1 year. The originally installed bubbler set was replaced in January 2011. The bubblers were visually examined once removed from the melter and showed minimal signs of wear. Material testing of the Inconel 690 is being performed to determine if the bubblers operational life can be extended. The use of the bubblers has changed the dynamics within the melter glass pool. This is shown through indications that the bubblers have increased the glass pool circulation. Overall, performance of the bubblers has been encouraging and the DWPF Melter has seen a significant improvement in its ability to process waste since the bubbler installation. The installation of the bubblers accomplished the goal of increasing the glass production capability of DWPF Melter. Currently the DWPF Melter is producing glass at a rate of 91 to 93 kg of glass/hour (200 to 205 lbs of glass/hour). As a result of this increased glass production rate the DWPF has been able to produce the most canisters since radioactive operations began in 1996. These accomplishments can be directly attributed to the bubblers ability to increase mixing/convection within the glass melt pool thereby improving the heat transfer from melt pool to the cold cap. Further, this has helped SRR take a significant step forward toward closing the HLW tanks at the aggressive pace set forth in the most recent liquid waste contract at the SRS. As a path forward, the DWPF is continuing work with SRNL to complete the final metallurgical examination of the bubbler samples to help determine methods to increase the design life of the bubblers beyond the current 6-month restriction. Also, the DWPF is continuing work with EnergySolutions on a new bubbler design concept to minimize cost and waste at the DWPF. The new design will allow for the lower end (inside melter) of the bubbler to be replaced while the upper end (outside melter) of the bubbler is reused. This new design is currently in the final design approval phase and EnergySolutions will be selecting a fabricator to begin the work to build bubbler sets 5 and 6 using the new design. (authors)

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DOE OSTI2016

Cementitious Grouts for ILW Encapsulation - Hydration and Continuity of Supply within the UK - 16184

In the UK the preferred route to disposal for the majority of intermediate level nuclear waste (ILW) streams is encapsulation within a cementitious matrix, accounting for 83% of waste conditioned to date (NDA, 2013). The method is well-defined and produces a waste package that is both chemically and physically stable, providing a multi-layered barrier to the release of the waste species contained within. Due to the process of treatment, facilitated via remote operation, it is necessary for the grouting matrices to meet strict performance limits in terms of their flow, setting time and avoidance of the formation of bleed water or segregation. To this end, the limits on composition of the anhydrous materials (a mixture of ordinary Portland cement [OPC] and blast furnace slag [BFS]) are tight to ensure conformity. Whilst these limits on composition are well understood, their impact upon grout hydration, and hence performance, is poorly defined. This study investigates the effects of modifying the physical and chemical composition of both the OPC and the BFS components of the matrix in order to identify the sensitivity or otherwise of the system to ensure that a continuity of supply is maintained. A number of techniques, scanning electron microscopy - image analysis (SEM-IA), chemical shrinkage (measured via dilatometry), isothermal conduction calorimetry (ICC), thermogravimetric analysis (TGA) and X-ray diffraction (XRD), have been applied to assess the rate and degree of hydration (DoH) of a range of grouts prepared with OPC and BFS with a range of chemical and physical compositions. This has been coupled with subsequent engineering performance testing, with additional analysis to understand the impact of a fire scenario within a storage or disposal facility, to provide an indication towards the resilience of the waste packages to a potential catastrophic event. (authors)

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DOE OSTI2014

Transient thermal analysis for radioactive liquid mixing operations in a large-scaled tank

A transient heat balance model was developed to assess the impact of a Submersible Mixer Pump (SMP) on radioactive liquid temperature during the process of waste mixing and removal for the high-level radioactive materials stored in Savannah River Site (SRS) tanks. The model results will be mainly used to determine the SMP design impacts on the waste tank temperature during operations and to develop a specification for a new SMP design to replace existing longshaft mixer pumps used during waste removal. The present model was benchmarked against the test data obtained by the tank measurement to examine the quantitative thermal response of the tank and to establish the reference conditions of the operating variables under no SMP operation. The results showed that the model predictions agreed with the test data of the waste temperatures within about 10%.

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DOE OSTI2016

Mercury Phase II Study - Mercury Behavior across the High-Level Waste Evaporator System

The Mercury Program team’s effort continues to develop more fundamental information concerning mercury behavior across the liquid waste facilities and unit operations. Previously, the team examined the mercury chemistry across salt processing, including the Actinide Removal Process/Modular Caustic Side Solvent Extraction Unit (ARP/MCU), and the Defense Waste Processing Facility (DWPF) flowsheets. This report documents the data and understanding of mercury across the high level waste 2H and 3H evaporator systems.

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DOE OSTI2024

Tank Closure Cesium Removal Ion Exchange Column CST Characterization: SRNL-STI-2024-00072 (Rev.0) pdf

Savannah River Mission Completion (SRMC) recently suspended operation of the Tank Closure Cesium Removal (TCCR) system which utilized an ion exchange (IX) process to remove radioactive cesium from waste supernate. During the demonstration phase, a total of three batches of Tank 10H dissolved salt waste were processed through the original TCCR columns. Subsequently, dissolved salt waste from Tank 9H was processed through TCCR in a phase referred to as TCCR 1A with four new IX columns. All eight columns have now been moved to Interim Safe Storage (ISS). For each batch processed through the TCCR IX columns, SRNL performed a number of analyses on surface and variable depth samples as well as batch equilibrium contact tests (BECT) to determine equilibrium loadings of Cs on the crystalline silicotitanate (CST) IX media. The BECTs were performed by lowering “teabags” containing ~0.1 g of CST each into the tank for a period of at least 10 days. The teabags were then retrieved and sent to SRNL for digestion and analysis.

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DOE OSTI2015

The completion of the construction and commissioning of the liquid radwaste treatment plant at ChNPP - 15685

Since a beginning of ChNPP operation, and after a tragedy in 1986, a few thousands m{sup 3} of LRW have been collected in a storage tanks. In 2004 ChNPP started the new project on creation of LRW treatment plant (LRWTP) financed from EBRD fund. But it was stopped in 2008 because of financial and contract problems. In 2010, FSUE RADON jointly with Ukrainian partners has won a tender on completion of LRWTP, in particular I and C system. The purpose of LRTP is to process liquid rad-wastes from SSE 'Chernobyl NPP' site and those liquids stored in the LRWS and SLRWS tanks as well as the would-be wastes after ChNPP Power Units 1, 2 and 3 decommissioning. The LRTP design lifetime - 20 years. (authors)

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DOE OSTI2014

Radioactive Demonstration Of Mineralized Waste Forms Made From Hanford Low Activity Waste (Tank SX-105 And AN-103) By Fluidized Bed Steam Reformation

One of the immobilization technologies under consideration as a Supplemental Treatment for Hanford’s Low Activity Waste (LAW) is Fluidized Bed Steam Reforming (FBSR). The FBSR technology forms a mineral waste form at moderate processing temperatures thus retaining and atomically bonding the halides, sulfates, and technetium in the mineral phases (nepheline, sodalite, nosean, carnegieite). Additions of kaolin clay are used instead of glass formers and the minerals formed by the FBSR technology offers (1) atomic bonding of the radionuclides and constituents of concern (COC) comparable to glass, (2) short and long term durability comparable to glass, (3) disposal volumes comparable to glass, and (4) higher Na2O and SO{sub 4} waste loadings than glass. The higher FBSR Na{sub 2}O and SO{sub 4} waste loadings contribute to the low disposal volumes but also provide for more rapid processing of the LAW. Recent FBSR processing and testing of Hanford radioactive LAW (Tank SX-105 and AN-103) waste is reported and compared to previous radioactive and non-radioactive LAW processing and testing.

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DOE OSTI2017

Impact of Glycolate Anion on Aqueous Corrosion in DWPF and Downstream Facilities

Glycolic acid is being evaluated as an alternate reductant in the preparation of high level waste for the Defense Waste Processing Facility (DWPF) at the Savannah River Site (SRS). During processing, the glycolic acid may not be completely consumed with small quantities of the glycolate anion being carried forward to other high level waste (HLW) facilities. The SRS liquid waste contractor requested an assessment of the impact of the glycolate anion on the corrosion of the materials of construction (MoC) throughout the waste processing system since this impact had not been previously evaluated. A literature review revealed that corrosion data were not available for the MoCs in glycolic-bearing solutions applicable to SRS systems. Data on the material compatibility with only glycolic acid or its derivative products were identified; however, data were limited for solutions containing glycolic acid or the glycolate anion. For the proprietary coating systems applied to the DWPF concrete, glycolic acid was deemed compatible since the coatings were resistant to more aggressive chemistries than glycolic acid. Additionally similar coating resins showed acceptable resistance to glycolic acid.

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DOE OSTI2013

Benchmarking Of Improved DPAC Transient Deflagration Analysis Code

The transient deflagration code DPAC (Deflagration Pressure Analysis Code) has been upgraded for use in modeling hydrogen deflagration transients. The upgraded code is benchmarked using data from vented hydrogen deflagration tests conducted at the HYDRO-SC Test Facility at the University of Pisa. DPAC originally was written to calculate peak deflagration pressures for deflagrations in radioactive waste storage tanks and process facilities at the Savannah River Site. Upgrades include the addition of a laminar flame speed correlation for hydrogen deflagrations and a mechanistic model for turbulent flame propagation, incorporation of inertial effects during venting, and inclusion of the effect of water vapor condensation on vessel walls. In addition, DPAC has been coupled with CEA, a NASA combustion chemistry code. The deflagration tests are modeled as end-to-end deflagrations. The improved DPAC code successfully predicts both the peak pressures during the deflagration tests and the times at which the pressure peaks.

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DOE OSTI2017

Impact of Glycolate Anion on Aqueous Corrosion in DWPF and Downstream Facilities

Glycolic acid is being evaluated as an alternate reductant in the preparation of high level waste for the Defense Waste Processing Facility (DWPF) at the Savannah River Site (SRS). During processing, the glycolic acid may not be completely consumed with small quantities of the glycolate anion being carried forward to other high level waste (HLW) facilities. The SRS liquid waste contractor requested an assessment of the impact of the glycolate anion on the corrosion of the materials of construction (MoC) throughout the waste processing system since this impact had not been previously evaluated. A literature review revealed that corrosion data were not available for the MoCs in glycolic-bearing solutions applicable to SRS systems. Data on the material compatibility with only glycolic acid or its derivative products were identified; however, data were limited for solutions containing glycolic acid or the glycolate anion. For the proprietary coating systems applied to the DWPF concrete, glycolic acid was deemed compatible since the coatings were resistant to more aggressive chemistries than glycolic acid. Additionally, similar coating resins showed acceptable resistance to glycolic acid.

36 MATERIALS SCIENCE↗

DOE OSTI2011

Conjugates of Actinide Chelator-Magnetic Nanoparticles for Used Fuel Separation Technology

The actinide separation method using magnetic nanoparticles (MNPs) functionalized with actinide specific chelators utilizes the separation capability of ligand and the ease of magnetic separation. This separation method eliminated the need of large quantity organic solutions used in the liquid-liquid extraction process. The MNPs could also be recycled for repeated separation, thus this separation method greatly reduces the generation of secondary waste compared to traditional liquid extraction technology. The high diffusivity of MNPs and the large surface area also facilitate high efficiency of actinide sorption by the ligands. This method could help in solving the nuclear waste remediation problem.

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DOE OSTI2015

Operating experience in the treatment and storage of LLW in Turkey - 15010

Treatment and storage of low-level radioactive wastes (LLW) are being carried out in Radioactive Waste Management Unit (RWMU) at Cekmece Nuclear Research and Training Center (CNRTC) in Istanbul. The wastes are generated from nuclear research and nuclear applications mainly in medicine, biology, ng to these specifications, LLW are classified as exempt waste, very low level waste (VLLW) etc. Decay storage is applied at a designated area for short lived radionuclide. Long lived spent radioactive sources are immobilized in retrievable packages. Generally liquid radioactive wastes are decontaminated by filtration or chemical precipitation. The radioactive sludge or filtration media from liquid waste processing is solidified using cementation. Solid waste is compacted into drums for size reduction. TENORM wastes and contaminated metal wastes are handled for decontamination and size reduction. Then these types of waste are placed in 20 ton bulk containers for long term storage. (authors)

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DOE OSTI2019

Maintenance Plan for the Performance Assessments and Composite Analyses for the Area 3 and Area 5 Radioactive Waste Management Sites at the Nevada National Security Site (Rev.3)

U.S. Department of Energy (DOE) Order 435.1, Radioactive Waste Management, requires that performance assessments (PAs) and composite analyses (CAs) for low-level radioactive waste (LLW) disposal facilities be maintained by the responsible field office. This plan describes the activities performed to maintain the PA and the CA for the Area 3 and Area 5 Radioactive Waste Management Sites (RWMSs) at the Nevada National Security Site (NNSS). The plan is based on DOE Order 435.1 Radioactive Waste Management (DOE 2007), DOE Manual 435.1-1, Radioactive Waste Management Manual (DOE 2011), and DOE Standard DOE-STD-5002-2017, Disposal Authorization Statement and Tank Closure Documentation (DOE 2017). The facility’s Disposal Authorization Statement (DAS) specifies conditions for the continuing operation of a LLW facility. The DAS is issued based on a review of the facility's PA, CA, the maintenance plan, preliminary closure plan, and preliminary monitoring plan. The DAS specifies the limits and conditions on construction, design, operations, and closure of the low-level waste facility based on these reviews. The Maintenance Plan uses an Unreviewed Disposal Question (UDQ)/Unreviewed Composite Analysis Question (UCAQ) change control process to identify, evaluate, and control planned or discovered changes affecting the PA, CA, DAS, or other documents composing the Radioactive Waste Management Basis (RWMB). The UDQ/UCAQ process uses the PA and CA GoldSim models to calculate updated results, assess the significance of changes, and to assess the need to revise the PA, CA, or DAS. In addition to the change control process, the Maintenance Plan requires an annual review of all changes and an annual assessment of the need to revise RWMB documents, plans, and programs. The cumulative effect of all changes is assessed annually by preparing a revised PA and CA baseline model that is used to update PA and CA results. The updated results are used to assess compliance with the PA performance objectives and the CA dose constraint, and to assess the need to revise the PAs, CAs, and other documents, plans, and programs supporting the RWMB. An Annual Summary Report documenting the results and conclusions of the annual review is prepared and submitted to DOE.

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