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At least 631 records · Page 35
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

A Dose Assessment Model for Radioactive Waste Exposed by Gully Erosion at West Valley - 20513

The Western New York Nuclear Service Center (WNYNSC), located approximately 48 km south of Buffalo, New York, is the site of a former nuclear fuel reprocessing and radioactive waste disposal facility. Spent nuclear fuel was processed there from 1966 to 1972, leaving behind radioactive and chemical wastes in two disposal areas and a waste tank farm. Site operations also resulted in releases of radioactivity to site soils, groundwater, and to surface waters draining the site. The New York State Energy Research and Development Authority (NYSERDA) and the U.S. Department of Energy (DOE) are collaborating in a process of decision making for decommissioning those facilities remaining at the WNYNSC following the completion of Phase 1 decommissioning. Neptune and Company, Inc. (Neptune) was contracted to develop a probabilistic performance assessment (PPA) computer model to assist the agencies in this process. The PPA Model includes a contaminant transport component focusing on the movement of contaminants within and among environmental media including groundwater and surface water transport, contaminant translocation by plants and animals, diffusion, and erosion. The model also includes evaluation of potential exposure and health effects for a Resident Farmer exposure scenario, where the Resident Farmer represents a critical group, described as that group of individuals reasonably expected to receive the greatest exposure to residual radioactivity for any applicable set of circumstances. The West Valley Site is located in the glaciated Allegheny Plateau region of western New York State. The waste reprocessing and disposal areas were constructed on a relatively fat area of plateau dissected by drainages of Buttermilk Creek, including Erdman Brook, Franks Creek, and Quarry Creek. An important aspect of the contaminant transport component of the PPA model is consideration of erosive processes such as slumping of the stream slopes and the advance of gullies from these streams. These erosion processes remove material from the plateau, growing the size of the creek valleys and making them wider and deeper. Of particular interest for the impact of erosion is radioactive waste contained in the Nuclear Regulatory Commission (NRC)-Licensed Disposal Area (NDA), the New York State-Licensed Disposal Area (SDA), and residual radiological inventory in the underground storage tanks at the Waste Tank Farm (WTF). The PPA Model is organized around geographically-defined facilities which were constructed upon the plateau, including the NDA, SDA, and WTF. Ongoing stream erosion processes will potentially transfer radioactive waste and residual inventory from these facilities to the ground surface on adjacent hillslope areas where erosion has breached the facility. Hence, it is important to evaluate the consequences of potential exposures to a Resident Farmer on the hillslopes below a breached facility. Two interrelated aspects of the dose assessment model related to hillslope exposure are discussed: 1) representation of the physical processes related to transport of radionuclides from facilities onto the hillslopes, and from the hillslopes into adjoining creeks where contaminated material migrates downstream with surface water and sediment, and; 2) adaptation of the activities associated with the Resident Farmer scenario to assess potential exposures to contamination in the hillslope areas. This discussion will cover the conceptual basis of the hillslope exposure and transport models, and also implementation in the PPA computer model. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Frictional properties of Opalinus Clay: influence of humidity, normal stress and grain size on frictional stability

SUMMARY The Opalinus Clay (OPA) is a clay-rich formation considered as a potential host rock for radioactive waste repositories and as a caprock for carbon storage in Switzerland. Its very low permeability (10−19 to 10−21 m2) makes it a potential sealing horizon, however the presence of faults that may be activated during the lifetime of a repository project can compromise the long-term hydrological confinement, and lead to mechanical instability. Here, we have performed laboratory experiments to test the effect of relative humidity (RH), grain size (g.s.) and normal stress on rate-and-state frictional properties and stability of fault laboratory analogues corresponding to powders of OPA shaly facies. The sifted host rock powders at different grain size fractions (<63 μm and 63 < g.s. < 125 μm), at room (∼25 per cent) and 100 per cent humidity, were slid in double-direct shear configuration, under different normal stresses (5–70 MPa). We observe that peak friction, μpeak and steady-state friction, μss, depend on water vapour content and applied normal stress. Increasing relative humidity from ∼25 per cent RH (room humidity) to 100 per cent RH causes a decrease of frictional coefficient from 0.41 to 0.35. The analysis of velocity-steps in the light of rate-and-state friction framework shows that the stability parameter (a–b) is always positive (velocity-strengthening), and it increases with increasing sliding velocity and humidity. The dependence of (a–b) on slip rate is lost as normal stress increases, for each humidity condition. By monitoring the variations of the layer thickness during the velocity steps, we observe that dilation (Δh) is directly proportional to the sliding velocity, decreases with normal stress and is unaffected by humidity. Microstructural analysis shows that most of the deformation is accommodated within B-shear zones, and the increase of normal stress (σn) promotes the transition from strain localization and grain size reduction to distributed deformation on a well-developed phyllosilicate network. These results suggest that: (1) the progressive loss of velocity dependence of frictional stability parameter (a–b) at σn > 35 MPa is dictated by a transition from localized to distributed deformation and (2) water vapour content does not affect the deformation mechanisms and dilation, whereas it decreases steady-state friction (μss), and enhances fault stability.

58 GEOSCIENCES↗
DOE OSTI2015

SRNL report for the tank waste disposition integrated flowsheet: Corrosion testing

A series of cyclic potentiodynamic polarization (CPP) tests were performed in support of the Tank Waste Disposition Integrated Flowsheet (TWDIF). The focus of the testing was to assess the effectiveness of the SRNL model for predicting the amount of nitrite inhibitor needed to prevent pitting induced by increasing halide concentrations. The testing conditions were selected to simulate the dilute process stream that is proposed to be returned to tank farms from treating the off-gas from the low activity waste melter in the Waste Treatment and Immobilization Plant.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

DOE EM Sponsored Research on Long-Term Dry Storage of Aluminum Clad SNF

This PowerPoint presentation describes and discusses DOE EM and INL lead studies on addressing potential technical issues associated with long-term dry storage of aluminum clad spent nuclear fuel. This same presentation was made to the US Nuclear Waste Technical Review Board in Nov 2019.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Evaluation of Nonmetallic Components in the Hanford Waste Transfer System - 17287

Nonmetallic materials are currently being used in the United States Department of Energy's Hanford Site Tank Farm waste transfer system. These materials include the inner primary hoses in the hose-in-hose transfer lines (HIHTLs), Garlock{sup R} gaskets, ethylene propylene diene monomer (EPDM) O-rings. These materials are exposed to a number of stressors and the synergistic effects are not well understood. Florida International University (FIU) engineers have developed an experimental test loop to determine how the nonmetallic materials react to both individual and simultaneous stressors. The initial phase of testing includes exposure of coupons and components to caustic material at various temperatures for varying lengths of time. The coupons are manufactured from EPDM and Garlock{sup R} sheets and will be used to evaluate changes in material data from baseline data. Components (inner hoses, O-rings and gaskets) will also be used to determine the effects from an environment similar to its operational environment. The test loop utilizes a 25% NAOH solution as the fluid and can accommodate eighteen component assemblies, each consisting of one EPDM HIHTL, EPDM O-ring and Garlock{sup R} gasket. There are three assembly aging sets, one for each temperature (37.78 deg. C, 54.44 deg. C and 79.44 deg. C) and each set contains six assemblies; three for each of the two time periods (6 months and 1 year). Prior to aging, a sample set of the components had baseline mechanical properties tested and a sample set of the coupons had baseline material properties determined as per ASTM standards. After the aging is completed the mechanical and material properties of the aged samples will be measured and compared with the bass-line data to obtain an understanding of the synergistic effects of the two stressors. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Design, Fabrication and Start-up of Test Facilities for the LAWPS Full-Scale IX Column Test and Engineering Scale Test - 17418

The U.S. Department of Energy (DOE), Office of River Protection's (ORP) primary mission is to retrieve and treat Hanford's tank waste and close the Tank Farms to protect the Columbia River. Mixed radioactive waste is stored in 177 underground tanks at the Hanford Site as reported in DOE/ORP 2003-02, Environmental Impact Statement for Retrieval, Treatment, and Disposal of Tank Waste and Closure of the Single Shell Tanks at the Hanford Site, Richland WA, Inventory and Source Term Data Package. The 177 underground tanks are estimated to contain about 56 million gallons of waste. The Low Activity Waste Pretreatment System (LAWPS) Project provides for the early production of immobilized low activity waste (ILAW) by feeding LAW directly from Tank Farms to the Hanford Waste Treatment Plant's (WTP's) LAW Facility, bypassing the Pretreatment Facility. Prior to the transfer of feed to the WTP LAW Vitrification Facility, tank supernatant waste will be pretreated in the LAWPS to meet the WTP LAW waste acceptance criteria. The LAWPS will also facilitate the return of secondary liquid wastes from the WTP LAW Vitrification Facility to the Tank Farms. In November of 2015 DOE's Tank Operations Contractor, Washington River Protection Solutions (WRPS), awarded a contract to the AECOM Team to design, fabricate and operate two test platforms to generate performance data at two different scales and demonstrate technology maturation. The first platform models the ion exchange (IX) columns at full scale, and the second platform models the integrated flowsheet (cross flow filter (CFF) and IX) at 1/9. scale. Both test platforms underwent shakedown and start-up testing in August 2016 and moved into actual testing and NQA-1 data generation shortly thereafter. This paper covers the engineering design, procurement, construction, installation, and acceptance testing of the test platforms (which are now operational) under an aggressive fast track schedule, and initial test data as available. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Savannah River National Laboratory Collaborative Innovation Pilot Team - 17560

The Collaborative Innovation (COIN) program was established by the Savannah River National Laboratory (SRNL) in March 2016. The goal of the SRNL COIN program is to identify innovative options to significantly reduce program and project risks (improve safety, reduce schedule and cost) of high priority Department of Energy Environmental Management, National Nuclear Security Administration, and Nuclear Energy missions. The COIN Advisory Board selected as the target outcome of the first COIN effort a 50% improvement to the Savannah River Site (SRS) H-Canyon spent nuclear fuel (SNF) processing 'baseline,' or current plan, as defined in the SRS Nuclear Materials Planning Roadmap. A small team of SRNL and Savannah River Nuclear Solutions personnel with pertinent experience and expertise was co-located and largely sequestered for eight weeks to identify improvements to H-Canyon processing of SNF. Following the process defined in the SRNL COIN Charter, the COIN Pilot Team analyzed the baseline for processing SNF through H Canyon; generated alternative ideas; tested seemingly viable ideas by reaching out to other subject-matter experts; and identified options for consideration for implementation by the COIN Advisory Board. The COIN Pilot produced a number of important outcomes, including important lessons learned for subsequent COIN efforts. The two principal outcomes are these: 1. The COIN Pilot Team conducted a comprehensive examination of the individual unit operations, the integrated system, and external interfaces to produce a timeline of H-Canyon processing and sampling times that had not previously existed. The general timeline served as the baseline from which the Pilot Team identified processing improvements. In addition, the timeline has already been employed in other planning efforts. 2. The COIN Pilot Team determined that innovations to the H-Canyon Dissolving unit operation alone could increase the number of SNF bundles processed through H Canyon by the target of 50%, but with little margin for error. To ensure that the gains in throughput in the Dissolving unit operation would be maintained throughout the facility, the Pilot Team identified four additional improvements to create greater efficiency and flexibility in downstream H-Canyon unit operations. The COIN Pilot Team's innovations reduce the processing time of a single batch of SNF through H Canyon from about 70 days to about 50 days. This talk will review the COIN process and the results of the pilot of the process. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Commercial submersible mixing pump for SRS tank waste removal - 15223

The Savannah River Site Tank Farms have 45 active underground waste tanks used to store and process nuclear waste materials. There are 4 different tank types, ranging in capacity from 2839 m{sup 3} to 4921m{sup 3} (750,000 to 1,300,000 gallons). Eighteen of the tanks are older style and do not meet all current federal standards for secondary containment. The older style tanks are the initial focus of waste removal efforts for tank closure and are referred to as closure tanks. Of the original 51 underground waste tanks, six of the original 24 older style tanks have completed waste removal and are filled with grout. The insoluble waste fraction that resides within most waste tanks at SRS requires vigorous agitation to suspend the solids within the waste liquid in order to transfer this material for eventual processing into glass filled canisters at the Defense Waste Processing Facility (DWPF). SRS suspends the solid waste by use of recirculating mixing pumps. Older style tanks generally have limited riser openings which will not support larger mixing pumps, since the riser access is typically 58.4 cm (23 inches) in diameter. Agitation for these tanks has been provided by four long shafted standard slurry pumps (SLP) powered by an above tank 112 kW (150 HP) electric motor. The pump shaft is lubricated and cooled in a pressurized water column that is sealed from the surrounding waste in the tank. Closure of four waste tanks has been accomplished utilizing long shafted pump technology combined with heel removal using multiple technologies. Newer style waste tanks at SRS have larger riser openings, allowing the processing of waste solids to be accomplished with four large diameter SLPs equipped with 224 kW (300 HP) motors. These tanks are used to process the waste from closure tanks for DWPF. In addition to the SLPs, a 224 kW (300 HP) submersible mixer pump (SMP) has also been developed and deployed within older style tanks. The SMPs are product cooled and product lubricated canned motor pumps designed to fit within available risers and have significant agitation capabilities to suspend waste solids. Waste removal and closure of two tanks has been accomplished with agitation provided by 3 SMPs installed within the tanks. In 2012, a team was assembled to investigate alternative solids removal technologies to support waste removal for closing tanks. The goal of the team was to find a more cost effective approach that could be used to replace the current mixing pump technology. This team was unable to identify an alternative technology outside of mixing pumps to support waste agitation and removal from SRS waste tanks. However, the team did identify a potentially lower cost mixing pump compared to the baseline SLPs and SMPs. Rather than using the traditional procurement using an engineering specification, the team proposed to seek commercially available submersible mixer pumps (CSMP) as alternatives to SLPs and SMPs. SLPs and SMPs have a high procurement cost and the actual cost of moving pumps between tanks has shown to be significantly higher than the original estimates that justified the reuse of SMPs and SLPs. The team recommended procurement of 'off-the-shelf' industry pumps which may be available for significant savings, but at an increased risk of failure and reduced operating life in the waste tank. The goal of the CSMP program is to obtain mixing pumps that could mix from bulk waste removal through tank closure and then be abandoned in place as part of tank closure. This paper will present the development, progress and relative advantages of the CSMP. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Leak Testing with Simulated Waste of Hanford Tank Farm Valves Utilized for Double Valve Isolation - 16108

The existing Hanford Tank Farms Waste Transfer System has several models of ball valves used for double valve isolation (DVI) that have been installed for 10 or more years. The safety function of the safety-significant valves is to limit leakage of waste past the valves in order to decrease the consequences of a fine spray release due to a transfer misroute. While previous leak testing of the valves has been conducted, the testing did not address concerns in the Documented Safety Analysis concerns about the impact on valve operation and service life of the potential abrasive/erosive properties of the tank waste on the valves when cycled. Pacific Northwest National Laboratory (PNNL) conducted DVI tests at their Multi-Phase Transport Evaluation Loop Facility. Testing evaluated the leak rate of safety-significant isolation valves for DVI as a function of simulated operating cycles. PNNL developed a performance-based simulant specifically for this test program. The test environment simulated the abrasive characteristics of the Hanford Tank Farms Waste Transfer System during single-shell tank retrieval and waste feed delivery to the Hanford Tank Waste Treatment and Immobilization Plant. The testing consisted of periodically measuring leak rates and maximum operational torques on the DVI valves after prescribed numbers of valve operational cycles (open and close). The test results from the simulant cycle tests provide Washington River Protection Solutions with performance characteristics that can be used to verify compliance with the Documented Safety Analysis limits for valve seat leakage. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Canada's Underground Research Laboratory (1980-2014) - 16274

In 1980, Canada initiated a long-term, comprehensive research and development program of geologic characterization and large-scale in situ geotechnical experiments in a subsurface facility, the Underground Research Laboratory (URL). The URL was excavated specifically to evaluate the concept of permanent disposal of used CANDU{sup R} nuclear reactor fuel in a deep geological repository (DGR) constructed in Canadian Shield granite. Key phases of the URL included siting, detailed site characterization and monitoring, construction, operation, decommissioning, and closure. Much collaborative research with international organizations was undertaken at the URL and continues, even after the closure of the facility, through the ongoing Enhanced Sealing Project (ESP). The ESP monitors the engineered performance of a full-scale composite shaft seal that was emplaced during URL closure to permanently seal the main URL access shaft across a sub-horizontal hydraulically active fracture zone. Currently the ESP is jointly funded by Canadian Nuclear Laboratories (CNL) (Canada), Posiva (Finland), and Andra (France), and monitoring is planned to continue until the end of 2016. Decades of programmatic experience at the URL have shown that knowledge continuity is integral to supporting the development of a safe geological disposal facility for high level nuclear waste. This paper outlines the history of the URL and describes some technical lessons learned from its 30-plus years of construction, operation, and closure activities. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Developing a New National Programme and Implementation Plan for the Management and Disposal of Spent Fuel and Radioactive Wastes in Romania - 16391

The European 'Waste Directive' (2011/70/Euratom) required each Member State to report by August 2015 on their National Programme for management of spent fuel and radioactive wastes. In Romania, the Nuclear Agency (ANDR) was responsible for preparing the National Programme report, and this was done in a step-wise manner that involved the regulators and waste producers. The starting point for the process was an assessment of existing policy against the evolving situation in the nuclear sector in the country, most notably the decision to progress with the construction of two new CANDU reactors. The final agreed National Programme report submitted to the European Commission describes the activities currently undertaken to manage spent fuel and radioactive wastes in Romania. The report also sets out, at a high-level, the additional activities that will need to be taken in the future (and an indicative timeline), including those steps that will be required to implement a new surface repository for short-lived wastes, and a geological repository for spent fuel and long-lived wastes. Additional, on-going work is intended to lead to a revision of Government policy and the development of a more detailed implementation strategy, underpinned by a programme of R and D and robust financing plans. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

The UK's National Policy and Programme for the Management of Spent Fuel and Radioactive Waste - 16574

This paper provides a broad overview of the United Kingdom's (UK's) national policies and national programme for the management of spent fuel and radioactive waste. The aim of the paper is to ensure a clear understanding of the approach taken in the UK so that opportunities for learning lessons and joint working, where they exist, can be identified and to ensure a general understanding of the interdependencies between the various approaches taken in the UK. With a legacy that dates back to the late 1940's/early 1950's the UK have a range of complex and difficult issues to resolve that have evolved over time. What was considered to be acceptable in the past is not thought of in the same way today. We therefore need to be forward thinking, innovative and above all ready to adapt our practices and policies to address previously unknown issues and complications. Due to the wide range of types of radioactive wastes and materials to be managed in the UK we have needed to establish a set of high level principles to cover all radioactive waste types while at the same time ensure that specific approaches for specific issues are developed within that framework. In the UK we have also had to consider the issue of integration to ensure that an approach that addresses one issue does not inadvertently cause a problem elsewhere - for example: in disposing of the high volumes of very low level waste we needed an approach to ensure that other low level waste has a disposal route. Financing of decommissioning and future waste management is clearly one of the biggest challenges to be addressed. As mentioned above ensuring that the legacy left for future generation is not one of a burden - we need to ensure that measures are in place to fund and manage long lived radioactive wastes. Finally, it is clear that not all radioactive wastes are the same and therefore different approaches are needed for managing the different types of material. This requires a proportionate and prioritised approach so while the same ultimate goal is applied (i.e.: the safe and responsible management of radioactive waste) some radioactive wastes are more equal than others and need to be treated accordingly. In the UK we believe that we have a broad programme in place that allows the right balance to be struck in managing all our radioactive waste and spent fuel in a proportionate, safe and responsible manner.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Development of a U.S. Rail Transport Capability for Spent Nuclear Fuel and High-Level Waste - 16623

The U.S. Department of Energy, Office of Nuclear Energy (DOE-NE) is laying the groundwork for implementing an integrated nuclear waste management system. This includes preparing for future large-scale transport of spent nuclear fuel (SNF) and high-level radioactive waste (HLW) since transport will be a necessary component of an integrated waste management system. DOE continues to plan and develop options for the design of an integrated nuclear waste management disposition system. A significant destination-independent component of this integrated system is a rail transport capability for SNF and HLW. This paper provides an overview of the current DOE-NE effort related to designing and fabricating prototype rail cars. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Views on Long-Term Safety of Deep Borehole Disposal - 16657

The Swedish Nuclear Fuel and Waste Management Co., SKB, has since the end of the 1980s evaluated Deep Borehole Disposal (DBD), of spent nuclear fuel (SNF). This has been done in parallel with the development of a mined repository concept based on the KBS-3V method. The most recent evaluation involved a broad comparison between the KBS-3V method and DBD. The comparison highlights differences between the two methods in the whole chain of the SNF handling including premises for siting, licensing, repository construction, safety during the operational phase, post-closure safety, physical protection, nuclear safeguards, retrieval of the deposited SNF, time planning, need for development, costs and nontechnical project risks. The ambition has been to make an as objective comparison between the two methods as possible, bearing in mind that there are big differences between the two concepts in terms of technical maturity as well as in terms of both quantity and quality of available data. While the primary safety function of the KBS-3V method is long-term containment in a corrosion resistant copper canister, the safety of DBD relies on stagnant groundwater at depth. It is argued in the aforementioned study that this groundwater stagnancy may be jeopardised because of heat and gas evolution in the disposal boreholes, and that deformation of the boreholes make efficient sealing of the deposition boreholes difficult. SKB has taken the position that the DBD method is associated with too many question marks to make it interesting as an alternative method in the Swedish programme. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Development of a Conditioned System-Level Groundwater Model to Evaluate Long-Term Groundwater Impacts within a Performance Assessment - 20115

A preliminary performance assessment (PA) of single-shell tank Waste Management Area (WMA) A-AX located at the U.S. Department of Energy (DOE)'s Hanford Site in southeastern Washington is being conducted to satisfy the requirements of DOE Order 435.1 [1] as it relates to closure of the single-shell radioactive waste tanks in the WMA A-AX tank farms. A PA assesses the fate, transport, and impacts of radionuclides within a low-level radioactive waste disposal facility in its assumed closure configuration and the subsequent potential doses to humans over a 1,000-year compliance period and a 10,000-year performance evaluation period. The WMA A-AX preliminary PA evaluation is structured around the complementary use of process-level and system-level models to calculate the facility performance against established DOE Order 435.1 [1] performance objectives. Process-level models are those that represent a detailed phenomenological representation of processes of concern in the PA. Process models typically only represent one or a few of the components of the PA, such as groundwater flow and transport, and must be integrated with other modeling elements to perform PA calculations. System-level models are those that are abstracted from the process models, retaining the essential features of the process model, while allowing integration of all aspects of the PA in a single modeling framework. System-level models are often characterized by coarser numerical discretization, lower dimensionality, or other similar simplifications compared to the process-level model. Traditionally, a three-dimensional (3-D) process-level model is utilized primarily to evaluate the long-term impact on groundwater and the potential doses to individuals who consume contaminated groundwater. System-level models are also utilized to evaluate the groundwater pathway in PAs. These models typically have reduced dimensionality (1-D) and are conditioned utilizing flow fields (Darcy fluxes) and moisture content distributions that are abstracted from the process level models. The abstraction approach assures that the flow field in both models is consistent for a specific set of input parameters for flow, differing only in the discretization and dimensionality of the two models. The preliminary WMA A-AX PA incorporates a detailed representation of the geological system and hydraulic properties within the 3-D model STOMP{sup C} numerical code so that the effects of relevant features and processes on water flow and radionuclide transport in the subsurface can be evaluated. The complementary system-level model is developed utilizing the GoldSim{sup C} code to implement a simplified, 1-D equivalent model to represent the groundwater pathway. Contaminant transport through the vadose zone and unconfined aquifer for Tc-99 and I-129 were evaluated in each of the models. Adjustments to the saturated portion of the GoldSim{sup C} 1-D model were required to mimic the dispersion effect captured with the 3-D STOMP{sup C} model. Once this conditioning was conducted, highly similar results for the transport of Tc-99 and I-129 were achieved at the point of calculation, located 100 m downgradient from the WMA A-AX fenceline. These radionuclides represent elements that are regarded as primary dose drivers in the PA groundwater pathway analysis. The high degree of conformance between the two models suggests that the use of the equivalent 1-D system model is suitable for evaluating the full suite of radionuclides that will be released from the tank sources within WMA A-AX over the 1,000-year compliance period and over the 10,000-year evaluation period. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

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↗
DOE OSTI2017

Criticality effect of long-term changes in material compositions and geometry in disposal canisters

For the Swedish final repository the basic requirement concerning margin to criticality is that k{sub eff} should be less than 0.95. This criterion is always fulfilled if the disposal canister is dry. If it is assumed that a canister is filled with water it is shown that the criticality criterion is fulfilled using burnup-credit for PWR fuel and credit for burnable poison for BWR fuel. If water is assumed to leak in, long term chemical processes will change the material compositions and geometries in the canister during the one million year analysis period. The main process expected to affect significantly the chemical composition of the materials in the canister is the corrosion of cast iron and carbon steel of the insert, the corrosion of the stainless steel, Inconel or Zircaloy in the fuel element structural material, the corrosion of Zircaloy cladding and finally the corrosion of spent fuel itself. During metal corrosion, various anoxic corrosion products are formed, usually with lower density than the metal itself, causing thus a volume increase in the canister, accompanied by geometrical changes. In this paper the reactivity effects of these changes are analysed and results presented. It is shown that the largest reactivity increase is due to the decrease of the water gap between the fuel and the fuel channel, due to the formation of Magnetite. Other process that possibly will increase the reactivity is if Siderite is produced besides from Magnetite, the production of Hydrogen, corrosion of the fuel and radial movements of fuel rods. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Extending Spent Fuel Storage until Transport for Reprocessing or Disposal

Spent fuel (SF) must be stored until an end point such as reprocessing or geologic disposal is imple-mented. Selection and implementation of an end point for SF depends upon future funding, legisla-tion, licensing and other factors that cannot be predicted with certainty. Past presumptions related to the availability of an end point have often been wrong and resulted in missed opportunities for properly informing spent fuel management policies and strategies. For example, dry cask storage systems were originally conceived to free up needed space in reactor spent fuel pools and also to provide SFS of up to 20 years until reprocessing and/or deep geological disposal became available. Hundreds of dry cask storage systems are now employed throughout the world and will be relied upon well beyond the originally envisioned design life. Given present and projected rates for the use of nuclear power coupled with projections for SF repro-cessing and disposal capacities, one concludes that SF storage will be prolonged, potentially for several decades. The US Nuclear Regulatory Commission has recently considered 300 years of storage to be appropriate for the characterization and prediction of ageing effects and ageing management issues associated with extending SF storage and subsequent transport. This paper encourages addressing the uncertainty associated with the duration of SF storage by de-sign – rather than by default. It suggests ways that this uncertainty may be considered in design, li-censing, policy, and strategy decisions and proposes a framework for safely extending spent fuel storage until SF can be transported for reprocessing or disposal – regardless of how long that may be. The paper however is not intended to either encourage or facilitate needlessly extending spent fuel storage durations. Its intent is to ensure a design and safety basis with sufficient margin to accommodate the full range of potential future scenarios. Although the focus is primarily on storage of SF from commercial operation, the principles described are equally applicable to SF from research and production reactors as well as high-level radioactive waste.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗