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RoboCount{sup TM} 2020 - A Robotic Non-Destructive Waste Assay System - 19331

A robotic system for non-destructive assay of radioactive waste - RoboCount{sup TM} 2020ab - has been designed, manufactured, and a prototype delivered to a customer. RoboCount{sup TM} 2020 is based on an industrial 6-axis articulating robot platform, combined with a dedicated waste package platform and a high-resolution HPGe gamma spectrometer. The system enables measurement of waste packages including drums (100-l, 200-l, 400-l), crates (up to 1200 x 800 x 800 mm), 1 m{sup 3} flexible intermediate bulk containers (FIBC), and others. Assay type can be freely defined, ranging from currently accepted protocols such as segmented gamma scan (SGS) or integral gamma scan (IGS) to new protocols developed for specific non-cylindrical waste packages, e.g., measurement of FIBCs from all four sides and the top. As a result of the robotic hardware flexibility, reconfiguration of the system for a new task is a matter of software changes only. In addition, while primarily geared towards waste characterization, the system can be configured for free release (clearance) by installing a second detector and field-of-view shielding. The prototype is currently in operation at a NPP site in Europe where it is used for D and D waste characterization in crates and FIBCs. Additional features beyond the basic functionality have been implemented such as an automatic lead collimator change based on measured HPGe detector dead time and an automatic liquid nitrogen refill, performed by the robot via a docking station at predefined time intervals. (Use of electrically cooled HPGe detectors is also possible). (authors)

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Design, Construction, and Commissioning of the RH LLW Disposal Facility at INL - 19445

The newly-commissioned Remote-Handled Low-Level Waste (RH LLW) Disposal Facility at Idaho National Laboratory (INL) provides permanent disposal capability critical for continuing INL nuclear research and Naval Reactors missions at the Idaho site. The facility mission need [critical decision (CD)- 0] was approved in 2009. Alternative selection (CD-1) was finalized in 2011. The project performance baseline (CD-2/3) was approved and design was initiated in 2014 and construction began in 2015. Construction was completed and transitioned to Materials and Fuels Complex (MFC) Operations in 2017. The facility successfully achieved readiness with authorization to begin operations (CD-4) in 2018. The $77 M line-item capital-acquisition project was completed six months ahead of the congressional commitment date and significantly under budget. This paper presents highlights of the RH LLW Disposal Facility project delivery and a summary of facility features and critical characteristics. Highlights include: - As a hazard category II nuclear facility, the project complied with United States Department of Energy (DOE) requirements for incorporation of nuclear safety into facility design and construction as identified in DOE-STD-1189 as well as 10 CFR 835 Subpart K requirements for incorporation of ALARA principles in facility design. - From an environmental compliance perspective, the facility was subject to National Environmental Policy Act requirements resulting in a Finding of No Significant Impact as determined by an Environmental Assessment. An operating disposal authorization statement from the Low-Level Waste Disposal Facility Federal Review Group (LFRG) authorizing waste disposal operations in accordance with DOE Order 435.1 was obtained. - The project was delivered using a design-build delivery method with a firm-fixed price with incentive fee contracting mechanism. The project was executed as a line-item capital-acquisition project, in full compliance with DOE Order 413.3B under INL's certified Earned Value Management System (EVMS) program. - The facility supports twenty years of waste disposal operations with five disposal vault configurations in four vault arrays supporting six different cask/canister system configurations. Three of the six cask/canister systems currently exist and three will be developed to support future operations. There are a total of 446 waste disposal vaults that will accommodate disposal of a total of 939 stainless steel radioactive waste canisters. The facility is designed to accommodate canisters with contact radiation dose rates as high as 600 Sievert/hour (60,000 Rem/hour). - The facility underwent a rigorous readiness review process in accordance with DOE Order 425.1D. Readiness activities included rigorous facility testing and shakedown activities, a management-self assessment, a contractor operational readiness review, and a DOE operational readiness review. Readiness was demonstrated for an existing cask/canister system (the MFC HFEF-5 cask). Separate readiness activities will be conducted for each cask/canister system as they are brought online for facility operations. INL's successful delivery of the project has provided waste disposal capability to ensure long-term viability of planned and current facilities and missions associated with both INL and the Naval Reactors Facility. Successful execution of the project has proven to be strategically important to future capital investments in capabilities necessary to advance INL's mission. (authors)

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Impact of dilution-induced precipitates on the filtration of Hanford liquid tank wastes

To facilitate its vitrification, a portion of the radioactive wastes currently stored at the Hanford Site will be staged and treated using tank-side operations to render their chemistry compliant with the requirements of Hanford’s low-activity waste vitrification facility. Initial sampling of staged feeds indicates that process-water dilution, used to reduce waste feed sodium content to levels acceptable for vitrification (5–6 M Na), may cause precipitation of fine, difficult to settle solids that could affect downstream tank-side filtration and ion-exchange. However, dilution-induced precipitation has not been demonstrated under controlled, rigorous laboratory conditions. This paper presents a set of qualitative and quantitative assessments of dilution-induced precipitation using a nonradioactive, Hanford Tank AP-105 simulated waste. Further, these studies found that dilution of AP-farm waste simulants induced precipitation of up to 150 ppm solids, regardless of whether dilution was done with process water (which contains, among other analytes, naturally occurring Ca and Mg) or deionized water. Naturally occurring process-water analytes appeared to accelerate the rate (and possibly extent) of precipitation. Filtration of diluted waste simulants also found that the precipitated solids challenged prototypic tank-side filter operations; however, the impact to filtration performance was readily managed through waste staging settle/decant operations.

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Corrosion Behavior of Fe-7Cr-1Mo-12Zr Metal Waste Form Alloy in Simulated Repository Environment

Metal waste forms (MWF) are solid metallic waste categorized as high-level radioactive waste generated during pyro-reprocessing of spent metallic fuels and geologically disposed off. This waste form generated requires an excellent corrosion resistance in a geological repository environment. In the present work, Fe-7Cr-1Mo-12Zr MWF alloy was developed by casting in an arc melting furnace. The x-ray diffraction analysis revealed the formation of stable phases of α-Fe solid solution and the intermetallic phases of Fe{sub 2}Zr and Fe{sub 23}Zr{sub 6}. The corrosion behavior of Fe-7Cr-1Mo-12Zr alloy was investigated using electrochemical techniques in aggressive (highly acidic with Cl{sup −}) and nominal repository pH environment. Cyclic potentiodynamic polarization studies indicated the shift in corrosion potential toward cathodic potential in highly acidic solution with Cl{sup −}. The corrosion mechanism of pitting is associated with acidified pH medium with more Cl{sup −}, whereas uniform corrosion or transpassive dissolution is resultant of mild acidity or mild alkaline medium. The passive region is wider in pH 5 and 8 when compared to pH 1 and 3. Electrochemical impedance spectroscopic (EIS) analysis revealed the lowering of passive film stability in the highly acidic medium in the presence of Cl{sup −}. The role of passive oxide layers on the corrosion resistance of the Fe-7Cr-1Mo-12Zr MWF alloy is discussed.

36 MATERIALS SCIENCE↗

Panel Session 76: US DOE Problematic Waste Streams and Policy Impacts

This panel provided an overview of DOE problematic waste streams including status and path forward. Potential policy implications that exist now and/or in the future were discussed. Topics included, greater-than-Class C low level waste, depleted uranium, and sodium waste. The panel also discussed potential treatment options for these wastes. As part of the introduction, Renee Echols welcomed the audience and went over a quick overview of what would be discussed on the panel. Theresa Kliczewski provided an overview of why this panel is relevant to US Department of Energy's Office of Environmental Management: there are problematic waste streams that still exist across the DOE cleanup complex. Theresa noted that the DOE EM Headquarters Office of Waste and Materials Management (EM-4.2), for which she is employed with, continues to work with the DOE cleanup sites on a path forward for these problematic waste streams. Presentations proposed include: 1 - Overview of Greater-Than-Class C Low-Level Radioactive Waste Disposal Path Forward (Theresa Kliczewski, US DOE EM (USA)); 2 - Status of Draft Supplemental Environmental Impact Statement for Disposition of Depleted Uranium Oxide Conversion Product Generated from DoE's Inventory of Depleted Uranium Hexafluoride (Jaffet Ferrer-Torres, US DOE (USA)); 3 - Problematic Waste Streams on the Oak Ridge Reservation (John Wrapp, UCOR (USA)); 4 - K Basin Sludge Removal (Ryan Covert, CH2M Hill PRC (USA)); 5 - Providing Technology Solutions for Treatment of Challenging Waste Streams (Tammy Monday, Perma-Fix Environmental Services (USA)); 6 - Treatment of Problematic Reactive Metal Waste Using the GeoMelt{sup R} In-Container Vitrification (ICV{sup TM}) Process (Ron Mitchell, Veolia Nuclear Solutions (USA))

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An Assessment of the Materials of Construction for the Transfer Lines and Unit Operations Equipment Associated with the Recycle Diversion Process

The Defense Waste Processing Facility (DWPF) processes and vitrifies radioactive waste that it receives from the Concentration, Storage, and Transfer Facility (CSTF) and Salt Waste Processing Facility (SWPF). As a result of the evaporation of water during both the melter feed preparation and the melter feed vitrification steps in DWPF, a recycle waste stream is generated, neutralized, and sent back to the CSTF. The recycle waste is a dilute water stream originating from the collection of condensate liquids containing some minor sludge and frit solids and other waste components primarily resulting from entrainment into the condensate during foam-over events. The recycle stream volume is significant and is expected to approach 3 million gallons per year once the SWPF reaches full operation. Diverting the bulk of the recycle waste stream from the CSTF is essential for the eventual closure of the waste tanks, and hence the completion of the SRS liquid waste mission.

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Measurements of Hydrogen Generation Rates using a Sealed Reactor System - 19428

Sealed reactor tests were performed to measure the hydrogen generation rate (HGR) from stored radioactive waste at the Savannah River Site. HGR may be very low, on the order of 7.5 x 10{sup -13} (m{sup 3}/h)/L [that is, cubic meters of H{sub 2} generated per hour per liter of radioactive liquid waste, or 10{sup -10} (ft{sup 3}/h)/gal]. Because the estimated HGR limit of detection for an open, continuous flow, system is approximately 7.5 x 10{sup -10} (m{sup 3}/h)/L [or 10{sup -7} (ft{sup 3}/h)/gal], a more sensitive method was needed. By accumulating generated gasses in a sealed system without a continuous purge gas, the resulting concentrations can increase the sensitivity of measurement, which is based on time of heating. In 2017, Savannah River Remediation declared a Potential Inadequacy in the Safety Analysis related to the potential thermal decomposition of organics that generate hydrogen in each of three Liquid Waste facilities: Concentration, Storage and Transfer Facility, Saltstone Production Facility, and the Defense Waste Processing Facility. The research for this study concerns low activity waste of Tank 50, which feeds the Saltstone Production Facility. This study evaluated the impact of organics including formate on the generation of H{sub 2}. Samples of SRS Tank 50 waste, which is a nominal 5 molar sodium salt solution, were sealed in stainless steel reactors and held at varying temperatures, e.g., 50 deg. C, 75 deg. C, 100 deg. C, and 120 deg. C, to determine if organic compounds are decomposing into H2. The experiments included trace solids used to stabilize waste in grout, e.g., grout-premix and Blast Furnace Slag, to determine if any solid phase reactions are present, which would accelerate or inhibit the generation of H{sub 2} at these temperatures. This paper describes the sealed reactors designed and constructed at Savannah River National Laboratory and the radioactive tests that were performed to measure HGR in both oxic and anoxic atmospheres. The shakedown tests showed the sealed reactors to be leak tight and hydrogen concentrations from calibrated standards could be accurately measured. Previous simulant tests helped to perfect the test methods and better design the radioactive tests. The radioactive results showed that the rate of hydrogen generated from Tank 50 waste, over a range of temperatures from 30 deg. C up to 120 deg. C, is bounded by an empirical relation (Hu Equation) that can be used to approximate HGRs in Tank 50 radioactive waste. (authors)

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Stakeholder-Engaged Structured Decision Making for the Los Alamos Legacy Cleanup Mission - 20501

The Los Alamos National Laboratory (LANL) environmental legacy cleanup program requires decisions to be made for environmental remediation, decommissioning and disposal or management of radioactive waste. This legacy cleanup program was established to address groundwater contamination, material disposal areas (MDAs) that have been used to dispose of radioactive and other waste material, and 'aggregate areas' that might produce radioactive or other chemical waste as a result of remediation activities. The LANL site is regulated for environmental concerns under the Resource Conservation and Recovery Act (RCRA). However, some parts of LANL, such as material disposal area G (MDA G), have disposed of radioactive waste under DOE Order 435.1, and are subject to other regulations. For example, decommissioning the remote-handled TRU material stored in 33 shafts at MDA G falls under EPA's 40 CFR 191. Collectively, the regulations are all aimed in the same direction of finding the best solution, either through constructs such as 'as low as reasonably achievable' (ALARA), considering balancing factors as opposed to only cost and human health risk, and, under EPA regulations such as RCRA and NEPA, evaluating impact from all chemicals and both human health and ecological endpoints. Despite the basic goals and objectives of the regulations or their guidance, the main challenge is in their implementation. Arguably perhaps, but really in principle, all of these (and similar) regulations are asking for a decision analysis to be performed. Implementation challenges encountered have included lack of understanding of decision analysis in the industry, lack of effective stakeholder engagement in the decision analysis process, and lack of appreciation of the need to separate value judgments from science, the latter leading to developing conservative, or protective, science-based models. Conservative models lead to poor solutions, lack of effective stakeholder engagement leads to long drawn out protracted approaches to finding a solution (which also might never be found with this approach), and lack of understanding of decision analysis and Bayesian statistics causes poor models to be built, which creates unfortunate situations of 'garbage in, garbage out' becoming the basis for decision making. Stakeholder-engaged structured decision making (SDM) is an approach to solving problems that relies on the theory of decision science to involve stakeholders in the decision-making process. This approach incorporates stakeholder values using a scientifically rigorous methodology that separates value judgments from science in a way that helps avoid the pitfalls of biased, protective, or conservative modeling. This approach has its foundation in Keeney's 1992 treatise on value-focused thinking [1]. Keeney advocated a paradigm shift in decision making based on the idea that the standard way of thinking about decisions is backwards. The standard approach of focusing first on identifying alternatives rather than on articulating values results in a reactive approach with the emphasis on mechanics and fixed choices instead of the core values that have meaning to stakeholders. This paradigm shift effectively engages all stakeholders in the decision-making process while using a values focused thinking approach that can lead to the identification of decision opportunities and the creation of better alternatives. The intent is to be proactive and generate solutions that are related directly to values and objectives as identified by stakeholders. There are, perhaps, two overarching reasons why SDM can be used to benefit LANL's environmental legacy cleanup. Some of LANL's remaining waste management and environmental management problems are challenging and complex (for example, the Cr and RDX plumes, and MDAs) and while the traditional approach has, arguably, worked well for relatively simple risk-based problems, it cannot, or should not, be applied to more complex problems if the most effective and efficient solutions are desired. The second reason is cost. This has perhaps become more critical since publication of the Government Accountability Office (GAO) reports that DoE's environmental liability is considered a high-risk concern for the nation [2]. The focus of SDM is on structuring solutions to decision risk problems by first addressing stakeholder and decision maker values and subsequently developing decision objectives and ways to measure those objectives, preference weighting across objectives, identifying decision alternatives that best achieve those values, and characterizing uncertainty in predictions of the measures. Because a complete decision model is created using SDM, it can be evaluated to find the main elements of the model that drive, or predict, the best solution. This approach creates complete decision models that are transparent, traceable, reproducible and technically defensible. The science behind SDM, or decision analysis, is well founded, yet it is not unusual to see ad hoc approaches to decision making implemented under various environmental regulations that are pertinent to the LANL site, including NEPA, RCRA and DOE Order 435.1. Such ad hoc approaches are often not transparent or traceable, and lack reproducibility and technical defensibility. The LANL legacy cleanup program has embarked on using SDM to address the complex problems that remain. Stakeholder meetings have been held, and a prototype version of the stakeholder value system has been developed. Further meetings are expected in the future to address specific project needs. This is a long-term endeavor considering the complex environmental problems faced by DOE EM in Los Alamos (EM-LA), and careful planning, consideration of stakeholder value systems, and engagement with stakeholders throughout the SDM process is expected to lead to a successful endpoint. (authors)

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Approaches to multi-scale analyses of mechanically and thermally-driven migration of fluid inclusions in salt rocks

Fluid inclusions are found within mineral crystals or along grain boundaries in many sedimentary rocks, notably in evaporite formations, and can migrate along a thermal or hydro-mechanical gradient. Shale and salt rocks have been considered potential host rocks for radioactive waste disposal, due to their low permeability. Previously stagnant inclusions may become mobilised by a perturbation of the in situ state by a geotechnical installation or the emplacement of heat-generating waste. Here, the migration of fluid inclusions can thus have important impacts on the long-term performance of a geologic repository for high-level radioactive waste disposal. As a part of the international research project DECOVALEX-2019, two aspects of fluid inclusion migration in rock salt are currently investigated under different boundary conditions: a) altered hydro-mechanical conditions as a consequence of tunnel excavation or borehole drilling and b) coupled thermo-hydro-mechanical-chemical conditions during the heating period of the post-closure phase of a repository.

58 GEOSCIENCES↗

Reduced-order modeling of near-field THMC coupled processes for nuclear waste repositories in shale

Performance assessment (PA) of geologic radioactive waste repositories requires three-dimensional simulation of highly nonlinear, thermo-hydro-mechanical-chemical (THMC), multiphase flow and transport processes across many kilometers and over tens to hundreds of thousands of years. Integrating the effects of a near-field geomechanical process (i.e. buffer swelling) into coupled THC simulations through reduced-order modeling, rather than through fully coupled geomechanics, can reduce the dimensionality of the problem and improve computational efficiency. In this study, PFLOTRAN simulations model a single waste package in a shale host rock repository, where re-saturation of a bentonite buffer causes the buffer to swell and exert stress on a highly fractured disturbed rock zone (DRZ). Three types of stress-dependent permeability functions (exponential, modified cubic, and Two-part Hooke’s law models) are implemented to describe mechanical characteristics of the system. Overall, our modeling study suggests that compressing fractures reduces DRZ permeability, which could influence the rate of radionuclide transport and exchange with corrosive species in host rock groundwater that could accelerate waste package degradation. Less permeable shale host rock delays buffer swelling, consequently retarding DRZ permeability reduction as well as chemical transport within the barrier system.

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Panel Session 120: Roundtable: Waste Management - Energy Facilities Contractor Operating Group (EFCOG WM)

This Roundtable focused on the WM EFCOG working group as they met to discuss a variety of issues of importance to US DOE waste management operations. The purpose of the WM EFCOG is to seek out and promote the best management and operating practices, cost effective technologies and disposal options for all waste streams generated at US DOE facilities whether destined for US DOE or commercial facilities. Each site representative provided a radioactive waste management lessons learned briefing. Panelists with presentations: Savannah River Site (SRS) Solid Waste Program Update (Kerri Crawford); Idaho Clean-up Project Status (Frederick Hughes); West Valley Demonstration Project Update - EFCOG Waste Management Working Group (John Rendall); Key Project Challenges and Successes (Kalli Shupe); EFCOG WMWG Challenging Waste Subgroup Update (Tammy Monday); CH TRU Difficult Waste Stream Processing Challenges (Daniel Pancake); Argonne Building 350 Clean-up Success Using Effective Work Control (Daniel Dilday); Problematic Waste Streams on the Oak Ridge Reservation (John Wrapp)

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Conceptual Design of the Belgian Geological Disposal Facility for Category B and C Wastes - 19341

For more than 40 years, ONDRAF/NIRAS (the federal agency responsible for managing radioactive waste and enriched fissile materials in Belgium) has been studying the concept of a geological disposal facility (GDF), within poorly indurated clays, as an option for the long-term management of both category B waste (low-level and intermediate-level long-lived waste - LILW-LL) and category C waste (high-level waste - HLW and spent fuel). The proposed Belgian reference option for disposal of such waste is a GDF within poorly indurated clays, located at a depth of between 200 m and 600 m. Within the framework of the first Safety and Feasibility Case (SFC-1) undertaken by ONDRAF/NIRAS, the former GDF layout, which dates back from 2003 has been updated. The first part of the paper describes the main drivers behind the evolution of the former 2003 GDF design towards the current reference SFC-1 design. It also details how these drivers, related to operational and constructional constraints, have affected the GDF layout, such as the disposal gallery length, the crossing shapes of the GDF galleries and the layout of access and waste shafts. The second part of the paper focuses on the engineering and construction challenges generated by GDF development within poorly indurated clays. This includes discussion of the impact of the specific mechanical characteristics such poorly indurated clays have on the construction methods used for the shafts, the rock support (concrete lining), the drift connections, the crossings and the global GDF design. These construction methods have been selected based on research conducted at the underground research laboratory HADES in Mol (Belgium). Finally, the main axes for further development of the GDF design within the SFC-1 framework is presented. (authors)

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Implementation of a Dose-based Compliance System for WCS - 19178

Waste Control Specialists LLC (WCS) operates a low-level radioactive waste (LLRW) disposal facility in Andrews, Texas. The site includes a compact waste facility (CWF) that began receiving waste in 2012, a federal waste facility (FWF) that started receiving waste in 2013, as well as a Resource Conservation and Recovery Act (RCRA) landfill and a byproduct facility. The current site license uses a complex system of concentration-based investigation levels and action levels (ILs and ALs) coupled with analytical decision levels (ADLs) that, when exceeded, require specific steps to be taken. These concentration-based ILs and ALs are media specific (i.e. air, soil, water), radionuclide specific, location specific, and disposal facility specific. This results in thousands of individual ILs, ALs, and ADLs that need to be managed and evaluated routinely in order to demonstrate compliance. Further, under the current system, each exceedance of an IL and AL can trigger comparisons to numerous additional isotopic ILs per sample, which is cumbersome, error prone, and costly. This paper describes implementation of a dose-based compliance system that has been developed to replace the existing system. The dose-based compliance system is implemented in RACER{sup C}, a cloud-based software developed by Risk Assessment Corporation (RAC). This system maintains all the analytical results related to the sampling and analysis conducted as part of the Radiological Environmental Monitoring Program (REMP) together with the geo-spatial data allowing instantaneous trending and analysis of the data. Further, the system contains the information needed to compare the analytical results to the new media-specific screening levels that have been developed, and the parameters and routines to compute doses using prescribed exposure scenarios and dose coefficients for compliance evaluation. Once measurement data are entered into RACER, the routines for continuous screening of air, soil, groundwater, and dosimeter data are triggered, and any sample result failing the screening step or exceeding the dose IL/AL is identified and flagged automatically for further review or action, as appropriate. Because RACER is cloud-based, the data, screening, and dose calculations can be accessed remotely at any time, providing a timely and efficient method for identifying any possible releases from the site to the environment as well as determining the potential dose consequences associated with a release. Furthermore, the system is accessible by the regulator providing transparency and ensuring they remain fully informed in an efficient manner. (authors)

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Panel Session 57: Nuclear Power Plant Waste Management - LLW Processor Issues

This panel resulted in senior utility managers discussing issues with commercial LLW processors. LLW processors updated utilities/NPPs on new or different services or technologies being offered to assist in their radioactive waste management goals, changes to their facility license, revisions to their acceptance guidelines, and emerging compliance issues. Presentations proposed include: 1 - EnergySolutions Waste Processing Overview (Joe Heckman, EnergySolutions (USA)); 2 - Perma-Fix: A Nuclear Services and Waste Management Company (John Kelly, Perma-Fix Environmental Services (USA)); 3 - UniTech - 'Expanding to Reduce Costs' LLW Processor Update (Gregg Johnstone, UniTech Services Group, Inc. (USA)); 4 - Low - Level Radioactive Materials Processing (Michael Miller, Veolia Nuclear Solutions (USA))

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Site Characterization and Adaptation - Lessons Learned from the Port Granby LLRW Project in Canada - 19255

The Port Hope Area Initiative (PHAI) is a community-based solution for the long-term management of historic low level radioactive waste (LLRW) resulting from 60 years of uranium and radium processing operations in the Town of Port Hope, Ontario. The Eldorado refinery, on the shores of Lake Ontario, began refining radium-226 from pitchblende ore, later transitioning to the refining of uranium ore. Process residues were deposited at the Welcome Waste Management Facility in the Town of Port Hope until the mid-1950's switching to the Port Granby Waste Management Facility (PGWMF), which continued to accept waste until the late 1980's. The Port Granby Project is part of the broader PHAI being completed by Canadian Nuclear Laboratories (CNL). The scope of remediation activities at Port Granby includes: 1) constructing a new, secure long-term waste management facility (LTWMF) and supporting infrastructure, and 2) excavating and relocating LLRW and marginally contaminated soil from the Port Granby Waste Management Facility (PGWMF) to the newly constructed LTWMF. Remediation design required extensive site investigations of waste buried in unmarked and unlined trenches across the PGWMF area. Investigations included reviews of historical records, interviews with past staff of Eldorado and Atomic Energy Canada Limited (the entity managing the PHAI cleanup prior to CNL), radiological surveys, and the advancement of boreholes across the site to facilitate the physical sampling of soil and groundwater contaminants indicative of the presence of LLRW. This paper describes the challenges associated with characterizing and quantifying waste prior to remediation and lessons-learned to adjust procedural adaptations during the characterization phase of a project to better anticipate the unanticipated nature and growth of the contamination profile that often occurs during remediation. Despite substantial pre-remediation investigative efforts, current PGWMF remediation activities have resulted in growth of both the areal and vertical extent of contamination. The contamination profile was shown to be dramatically influenced by leaching of contaminants deeper into native soils. In addition, remedial excavation discovered specific waste types such as unidentified compressed gas cylinders outside of the location indicated by historical records, as well as a quantity of unknown liquids and unmarked drums. These discoveries have resulted in higher waste quantity estimates and have required a partial redesign of the LTWMF mound (a higher final elevation and steeper slopes) to accommodate the increased waste volume. In addition, the means and methods necessary to execute the remedial construction had to be modified to account for the new conceptual model developed from the new contamination data. Despite extensive historical review and site characterization to define the nature and extent of LLRW buried at the PGWMF, actual conditions encountered during remediation efforts necessitated taking an adaptive approach to both the design of the LTWMF and the means and methods used for excavation and transport of waste. (authors)

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Panel Session 56: Nuclear Power Plant Waste Management - US LLW Disposal Issues

This panel focused on specific disposal site issues with the disposal site operators. Representatives from each of the operating commercial disposal sites presented an update of their facility, license, and waste acceptance criteria (WAC) followed by a panel discussion in response to audience questions. WM attendees that ship their radioactive waste to one or more of these commercial disposal sites attended this panel session. Presentations proposed include: 1 - US Nuclear Power Plant Waste Management - US LLW Disposal Issues (Joe Weismann, US Ecology (USA)); 2 - Waste Control Specialists Update 2019 (Dan Burns, Waste Control Specialists LLC (USA)); 3 - Barnwell LLRW Disposal Facility (Mark Lewis, EnergySolutions (USA), Benjamin Smith, Chem Nuclear Systems (USA)); 4 - EnergySolutions Clive Treatment and Disposal Facility Update (Bret Rogers, EnergySolutions (USA))

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Colloidal Behavior of Plutonium Oxide in Concentrated Electrolyte Solutions

The Hanford Site in Washington State manages legacy high-level radioactive waste streams that display major chemistry and engineering challenges, including the high salt levels and pH values that correspond to conditions under which many classical concepts describing chemical reactivity cannot be applied. One particular challenge that needs to be tackled at Hanford is that Pu concentrations, [Pu], in the soluble phases of the tank wastes are higher than expected based on the solubility of crystalline PuO2, which is widely accepted to be caused by the formation of PuO2 colloid, consisting of nano- to submicron-sized particles (PuO2 NPs). Fundamental research underpinning the behavior of PuO2 NPs under conditions not only relevant to the Hanford tank waste but at high ionic strength in general is needed to reliably predict the chemical reactivity of PuO2 NPs and develop engineering solutions to safely and efficiently process high-level radioactive waste into forms suitable for long-term storage. In this work, we study the behavior of PuO2 NPs (particle size ~100 nm) under high ionic strength conditions by reacting it with highly concentrated (up to 5 M) salt solutions. We explore different electrolyte compositions to elucidate the impact of different anions (NO3-, Cl-, ClO4-, SO42-, C2O42-, CO32-) on the stability of PuO2 NP in the acidic and alkaline pH regime. PuO2 NP aggregation and precipitation as function electrolyte concentration is tracked by a combination of liquid scintillation counting, dynamic light scattering for determination of particle size distributions, and zeta potentials as a proxy for particle charge. At acidic pH, electrolytes containing non-coordinating anions, such as NaNO3, NaCl, and NaClO4 mostly stabilize PuO2 NPs over a large electrolyte concentration range, showing only subtle differences in their reactivity. Other electrolyte anions show a more pronounced effect on the PuO2 NP stability: SO42-, binds directly to the particles’ surface, reverses the particle charge, and precipitates the PuO2 NPs efficiently even at intermediate sulfate concentrations (>0.1 M). In contrast, C2O42- is found to lead to high [Pu] in solution, in the milli-molar range, even at mildly acidic pH (~4). Thermodynamic modeling of the dissolved Pu concentrations using PHREEQC is unable to predict the observed [Pu] in the acidic pH regime, supporting the influence of colloids in maintaining elevated [Pu]. It is noteworthy that the current thermodynamic databases do not include constants for colloidal Pu phases and cannot accurately predict many of the high ionic strength solutions relevant to this work. The mechanisms and models responsible for these observations will need further investigation in the future. At high pH values (~12), PuO2 NPs exhibits classical sol-gel chemistry, meaning that upon destabilization of the colloidal sol, for example by addition of concentrated NaOH, highly porous and viscid PuO2 coagulates are formed that consist of a three-dimensional network likely held together by physical interactions. The PuO2 NP coagulate shows no significant reversibility of the aggregation when contacted with concentrated brines; however, PuO2 NPs can be efficiently resuspended in solution by addition of diluted electrolytes, alkaline solutions containing high amounts of carbonate, or simple addition of water. Especially carbonate is shown to stabilize PuO2 NPs in solution at high pH, characterized by stable colloidal suspensions that are resistant against sedimentation during centrifugation. Thermodynamic modeling of the carbonate system was able to predict an increasing dissolved Pu concentration with increasing carbonate concentration. However, the model was profoundly sensitive to the fixed redox potential and does not include any thermodynamic constants for colloidal Pu species.

Neumann, Julia↗