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DECOVALEX-2023: Task B Final Report

In all repository concepts for the geological disposal of radioactive waste, an engineered barrier system (EBS) is used to encapsulate the waste canister, or, to act as borehole or gallery seals. These systems are often based on bentonite clays due to their low permeability and high swelling capacity enabling the closure of engineering voids. However, in all repository concepts gases will be generated through the corrosion of metallic materials (under anoxic conditions), the radioactive decay of waste and the radiolysis of water. Thus, understanding the processes and mechanisms controlling the advective movement of gas (as a discrete phase) in clay-based materials is a key aspect when assessing the impact of gas flow in a repository safety case.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Effectiveness of an in-situ permeable reactive barrier in removing strontium-90 from groundwater - 15418

An in-situ permeable reactive barrier (PRB) is being used to remove strontium-90 from groundwater along the 100-N Area shoreline at the U.S. Department of Energy Hanford Site in southeastern Washington. The PRB was formed by emplacing apatite, a calcium phosphate mineral, in the subsurface sediments via injection of calcium-citrate and sodium-phosphate solution into the aquifer through a network of vertical wells. The relatively slow biodegradation of citrate allowed sufficient time for the injected solution to disperse in the PRB treatment zone as the free calcium and phosphate combined to form apatite. Substitution of strontium for calcium in the apatite crystal structure is thermodynamically favorable. As groundwater flows through the PRB toward the Columbia River, strontium-90 is sequestered into the apatite crystal matrix. The sequestered strontium-90 undergoes radioactive decay in place within the PRB. Groundwater monitoring wells installed between the PRB and the Columbia River are used to monitor the PRB effectiveness. The concentration of strontium-90 in the monitoring wells following apatite emplacement are compared to the pre-injection concentrations. The performance goal of the PRB is to reduce the concentration of strontium-90 in groundwater down gradient of the PRB by 90 percent, compared to the pre-injection concentrations. Groundwater samples in Fall 2013 show the percent reduction in strontium-90 concentrations ranged from 71 to 98 percent in eleven of the twelve monitoring wells. The data indicate that the PRB is effective in reducing the flux of strontium-90 toward the Columbia River and is thereby instrumental in protection of the Columbia River. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Optimization of Material Recycling During the Decommissioning Process of Nuclear Power Plants - 16123

The German Government decided in 2011 to phase out nuclear power. Therefore, in the near future there will be several nuclear power plants queued up, in parallel, for dismantling. In nuclear decommissioning there is no standardized procedure available, so that a high level of optimization potential can be assumed. We present the results of a preliminary study, in which the optimization potential of metal recycling during the dismantling process should be estimated. The project can be roughly divided into four sections: - Determination of the metal inventory of an exemplarily selected plant; - Analysis of the recycling routes of scrap metal fractions and assessment of the potential for optimization of each process step during the dismantling; - Conduction of activation calculations to uncover the potential of interim storage allowing for radioactive decay; - In collaboration with the Institute of Process Metallurgy and Metal Recycling at the RWTH Aachen, appropriate process steps and process chains of an optimized metal recycling for each of the resulting scrap metal fractions are identified. The paper and the presentation summarize the status and the results of the project implementation and will address for the optimization potentials for decommissioning projects. (authors)

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Low Power Radioisotope Conversion Technology and Performance Summary

This work presents a summary of low-power radioisotope-based power sources. This includes systems that use direct energy conversion from radioactive decay such as betavoltaics and systems that convert heat generated by the isotope decay. These types of power systems have terrestrial and space-based applications. Their main application is to provide low levels of power in remote environments where long life and reliability are the main objectives. This work looked at the potential performance of these types of systems and the range of output power they can achieve. Also considered was the amount of power that could be achieved from these different conversion technologies, while remaining under the critical limit acceptable for space flight without the need for special handling and controls. This is of interest for space missions where low power levels can be used for operating sensors or other devices, but the expense associated with the incorporation of radioactive material above this critical level would be cost prohibitive.

Colozza, Anthony J.↗

Cookoff Modeling of a WIPP waste drum (68660)

A waste drum located 2150 feet underground may have been the root cause of a radiation leak on February 14, 2014. Information provided to the WIPP Technical Assessment Team (TAT) was used to describe the approximate content of the drum, which included an organic cat litter (Swheat Scoop®, or Swheat) composed of 100% wheat products. The drum also contained various nitrate salts, oxalic acid, and a nitric acid solution that was neutralized with triethanolamine (TEA). CTH-TIGER was used with the approximate drum contents to specify the products for an exothermic reaction for the drum. If an inorganic adsorbent such as zeolite had been used in lieu of the kitty litter, the overall reaction would have been endothermic. Dilution with a zeolite adsorbent might be a useful method to remediate drums containing organic kitty litter. SIERRA THERMAL was used to calculate the pressurization and ignition of the drum. A baseline simulation of drum 68660 was performed by assuming a background heat source of 0.5-10 W of unknown origin. The 0.5 W source could be representative of heat generated by radioactive decay. The drum ignited after about 70 days. Gas generation at ignition was predicted to be 300-500 psig with a sealed drum (no vent). At ignition, the wall temperature increases modestly by about 1°C, demonstrating that heating would not be apparent prior to ignition. The ignition location was predicted to be about 0.43 meters above the bottom center portion of the drum. At ignition only 3-5 kg (out of 71.6 kg total) has been converted into gas, indicating that most of the material remained available for post-ignition reaction.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Modeling Radionuclide Releases from TRISO Particles by Simultaneous Diffusion Through and Corrosion of the Silicon Carbide Barrier Layer

TRISO nuclear fuel particles that are less than 1 mm in diameter are designed with multiple barrier layers to retain fission products both during reactor operations and for long-term geological disposal. The primary barrier is a 35 μm thick silicon carbide (SiC-a highly impermeable semi-metal) layer for which data are available on the diffusion of short-lived fission products at high temperatures (> 1000 °C). However, for a geological repository, this layer may contact brine and hence corrode even at ambient temperatures. As an initial approach to assess the effectiveness of the SiC barrier for geological repositories, ranges of fission product diffusivities and corrosion rates for SiC are modeled concurrently with the simultaneous effect of radioactive decay. Using measured corrosion rates of SiC, if the diffusivity is more than about 10 -20 m 2 /s, fission product releases may occur before the SiC barrier has corroded to the point of breach. For diffusivities less than about 10 -21 m 2 /s there may not be significant diffusional releases prior to SiC barrier removal/breach by corrosion. This work shows the importance of estimating diffusivities in SiC at geological repository temperatures, and highlights the relevance of evaluating the porosity/permeability evolution of the SiC layer in a geologic environment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Electrochemical Corrosion Studies for Modeling Metallic Waste Form Release Rates

The isotope 99 Tc is an important fission product generated from nuclear power production. Because of its long half-life (t 1/2 = 2.13 ∙ 10 5 years) and beta-radiotoxicity (β⁻ = 292 keV), it is a major concern in the long-term management of spent nuclear fuel. In the spent nuclear fuel, Tc is present as an alloy with Mo, Ru, Rh, and Pd called the epsilon-phase, the relative amount of which increases with fuel burn-up. In some separation schemes for spent nuclear fuel, Tc would be separated from the spent fuel and disposed of in a durable waste form. Technetium waste forms under consideration include metallic alloys, oxide ceramics and borosilicate glass. In the development of a metallic waste form, after separation from the spent fuel, Tc would be converted to the metal, incorporated into an alloy and the resulting waste form stored in a repository. Metallic alloys under consideration include Tc–Zr alloys, Tc–stainless steel alloys and Tc–Inconel alloys (Inconel is an alloy of Ni, Cr and iron which is resistant to corrosion). To predict the long-term behavior of the metallic Tc waste form, understanding the corrosion properties of Tc metal and Tc alloys in various chemical environments is needed, but efforts to model the behavior of Tc metallic alloys are limited. One parameter that should also be considered in predicting the long-term behavior of the Tc waste form is the ingrowth of stable Ru that occurs from the radioactive decay of 99 Tc ( 99 Tc → 99 Ru + β⁻). After a geological period of time, significant amounts of Ru will be present in the Tc and may affect its corrosion properties. Studying the effect of Ru on the corrosion behavior of Tc is also of importance. In this context, we studied the electrochemical behavior of Tc metal, Tc-Ni alloys (to model Tc-Inconel alloy) and Tc-Ru alloys in acidic media. The study of Tc-U alloys has also been performed in order to better understand the nature of Tc in metallic spent fuel. Computational modeling and simulations were performed to shed light on experimental results and explain structural and kinetics trends.

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Contaminant Migration Modeling to Support the In Situ Decommissioning of Hardened Nuclear Facilities - 20215

The decommissioning of hardened nuclear facilities provides a unique challenge in balancing current worker dose with exposure to future receptors and media. In situ decommissioning (ISD) is a cost-effective and safe option for the closure of such facilities but requires a detailed understanding of the threat that radioactive and hazardous constituents remaining in the facilities pose to groundwater and surrounding surface water. The Savannah River Site (SRS) extensively employs contaminant migration models within the decommissioning process to develop site-specific removal, grouting, and monitoring strategies in support of safe and effective final end states of nuclear facilities. This work discusses the use of contaminant migration modeling in the ISD process at SRS, including specific examples from the closure of P-Reactor and R-Reactor, Building 235-F, F-Canyon and F/H Laboratory Complex. Migration models developed during the closure of P-Reactor and R-Reactor were divided into four source areas: the reactor vessel, the process area, the disassembly basin, and the purification wing. Each source area was assigned a specific inventory and migration pathway and was then subject to varying hypothetical removal, capping, and grouting schemes. Modeling indicated that groundwater Maximum Concentration Limits (MCLs) might be exceeded if no action was taken for eleven and ten constituents of concern (COCs) at P-Reactor and R-Reactor, respectively. These exceedances could occur in as few as 200 to 500 years. Alternatively, the migration modeling demonstrated that the selected ISD actions reduced contaminant mobility which allowed for significant radioactive decay and resulted in fewer predicted exceedances of groundwater MCLs (five COCs for P-Reactor; eight COCs for R-Reactor). In response to the modeling results for P-Reactor and R-Reactor, effectiveness monitoring programs were developed to target contaminants, specific to each reactor, that may migrate to groundwater. Contaminant migration modeling also revealed that roof collapse was a large factor in the release of COCs to the environment, giving rise to roof improvements, and an inspection and vegetation control program to ensure roof stability over time. Contaminant migration modeling is also aiding in the closure planning for hardened facilities in F Area. Building 235-F housed the Actinide Billet Line, which produced Np-237 billets for irradiation in SRS reactors, and the Plutonium Fuel Form (PuFF) facility that produced Pu-238 heat sources for the space program. As a result of these missions, areas within Building 235-F contain considerable residual amounts of both Pu-238 and Np-237. Contaminant migration modeling of Building 235-F was originally performed in 2012 to identify the feasibility of ISD and the amount of radioactive material removal required to prevent the exceedance of groundwater MCLs. The original model indicated that a 60% reduction in the PuFF facility Pu-238 inventory could keep groundwater concentrations below standards, while Np-237 did not pose a threat to groundwater. However, updates to the model with an emphasis on source impact pathways revealed that, due to the orientation of the source areas relative to groundwater flow, no amount of reasonable removal of Pu-238 would keep groundwater concentrations below MCLs and that Np-237 could be a large contributor to localized MCL exceedances. With this insight, the refined 2019 model is being used to assist in the development of grouting plans specific to each facility source area, where bentonite may be utilized to slow the migration of Pu-238 and its daughter products from the PuFF facility and a reducing grout may decrease Np-237 transport by ensuring the nuclide remains in the less mobile +IV oxidation state. The beginning phases of contaminant migration modeling are underway for F-Canyon and associated facilities using lessons learned from the Reactors and Building 235-F. A contaminant migration pathway, similar to the pathway used for the reactor vessels, is being developed for the hot and warm canyons. The F-Canyon inventories are being spatially refined to identify specific and localized source zones, comparable to Building 235-F, that may impact groundwater. Contaminant migration modeling provides vital input within the ISD process, from facility investigation to post closure effectiveness monitoring, making it a valuable tool in the development of safe and effective end states for hardened nuclear facilities at SRS. (authors)

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Regulation of the First British Power Reactor to Enter into an Extended Period of 'Care and Maintenance' - 18028

All eleven of the British first-generation Magnox nuclear power plants have now ceased operating and are in various stages of decommissioning. The Magnox reactors were graphite moderated, using carbon dioxide as the primary coolant. The reactor cores are contained in steel reactor pressure vessels, except for the last two stations which have pre-stressed concrete pressure vessels. All but two of the Magnox reactor stations have been completely de-fueled. The spent fuel removed has been despatched for reprocessing at Sellafield in the north-west of England. On behalf of the UK government the Nuclear Decommissioning Authority (NDA) is responsible for cleaning up the majority of the civil nuclear legacy. The current NDA decommissioning strategy is to prepare the Magnox reactor sites for an extended period of Care and Maintenance (C and M), during which quiescent safe storage will take place (also known as safe enclosure), whereby the cores and associated structures will accrue the benefits of radioactive decay over a period of decades. This will reduce the radiation doses to workers during final dismantling and site clearance. The two Magnox rector units at the Bradwell licensed nuclear site in the south-east of England are the first scheduled to enter this quiescent safe-storage period. This is planned to commence in the second-half of 2018, and is scheduled to last for around 70 years. The Office for Nuclear Regulation (ONR) is the independent regulatory body, responsible for enforcing safety and security requirements at nuclear installations in Great Britain (GB). This paper outlines the national strategic context and how ONR's regulatory regime is applied to nuclear power plant decommissioning. It addresses some of the specific challenges posed at Bradwell during the preparatory works for entry to C and M and how ONR has addressed these. It describes how this will culminate in a regulatory decision on the acceptability of the safety and security of the Bradwell site to enter this new stage of its life cycle. Over the last few years ONR has assessed and inspected various safety aspects of decommissioning, radioactive waste management and other preparations for Bradwell's entry into C and M. Some of the operator's proposals have provided challenges to ONR, particularly where there have been changes to established approaches taken at other sites, as the licensee seeks to minimise its costs. These have included how far to remove redundant structures, systems and components prior to C and M; how to define interim and end-states for fuel cooling ponds and other contaminated areas; and how to treat and store Intermediate Level Waste (ILW), for which there is no geological disposal facility yet available. ONR has begun its final assessment of safety and security justifications supplied by the site licensee, Magnox Ltd (ML). ONR is using its legal powers conferred to it under the site licence conditions to authorise this first-of-a-kind transition into a 70 year period of safe storage. (authors)

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Thermal release of {sup 3}He from tritium aged LaNi{sub 4.25}Al{sub 0.75} hydride

The Savannah River Site Tritium Facilities (SRS-TF) utilizes LANA.75 (LaNi{sub 4.25}Al{sub 0.75})in the tritium process to store hydrogen isotopes. The vast majority of {sup 3}He born from the radioactive decay of tritium stored in LANA.75 is trapped in the hydride metal matrix. The SRS-TF has multiple LANA.75 tritium storage beds that have been retired from service with significant quantities of He-3 trapped in the metal. To support He-3 recovery, the Savannah River National Laboratory (SRNL) conducted thermogravimetric analysis coupled with mass spectrometry (TGA-MS) on a tritium aged LANA.75 sample. TGA-MS testing was performed in an argon environment. Prior to testing, the sample was isotopically exchanged with deuterium to reduce residual tritium and passivated with air to alleviate pyrophoric concerns associated with handling the material outside of an inert glovebox. Analyses indicated that gas release from this sample was bimodal, with peaks near 220 and 490 C. degrees. The first peak consisted of both {sup 3}He and residual hydrogen isotopes, the second was primarily {sup 3}He. The bulk of the gas was released by 600 Celsius degrees. (author)

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Direct Mass Measurements to Inform the Behavior of 128m $\mathrm{Sb}$ in Nucleosynthetic Environments

Nuclear isomer effects are pivotal in understanding nuclear astrophysics, particularly in the rapid neutron-capture process where the population of metastable isomers can alter the radioactive decay paths of nuclei produced during astrophysical events. The β-decaying isomer 128m Sb was identified as potentially impactful since the β-decay pathway along the A = 128 isobar funnels into this state bypassing the ground state. Here we report the first direct mass measurements of the 128 Sb isomer and ground state using the Canadian Penning Trap mass spectrometer at Argonne National Laboratory. We find mass excesses of -84564.8(25) keV and -84608.8(21) keV, respectively, resulting in an excitation energy for the isomer of 43.9(33) keV. These results provide the first key nuclear data input for understanding the role of 128m Sb in nucleosynthesis, and we show that it will influence the flow of the rapid neutron-capture process.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Alpha-Voltaic Sources Using Liquid Ga as Conversion Medium

A family of proposed miniature sources of power would exploit the direct conversion of the kinetic energy of alpha particles into electricity. In addition to having long operational lives, these sources are expected to operate with energy-conversion efficiencies from 70 to 90 percent. A power source as proposed (see figure) would be an electrolytic cell in which liquid gallium would serve as both an electrolyte and an energy-conversion medium. The cell would contain an iridium cathode and a zirconium anode. The alpha particles, each with a kinetic energy approx.5.8 MeV, would be emitted by radioactive decay of Cm-244, which has a half-life of 18 years. The Cm-244 source would be positioned so that the a particles would enter the liquid gallium, where their kinetic energy would be dissipated mostly through ionization of Ga atoms, creating Ga(+) ions and free electrons. The electrons would be collected by iridium cathode, and the Ga(+) ions would be neutralized at the zirconium cathode by electrons returning after flowing through an external circuit. Gallium is a candidate for use as the electrolyte and the energy-conversion medium because in the liquid state it is a semimetal: its electrical conductivity is greater than that of a typical semiconductor but small in comparison with the conductivities of metals. Consequently, in liquid gallium, electrons and Ga(+) can exist without immediate recombination and can be moved by electric fields. It is expected that electric fields, resulting at least partly from the difference between the work functions of the electrode metals, would move the electrons and ions to their respective electrodes. The open-circuit potential of the cell is expected to be 1.62 V - equal to the difference between the work functions of iridium and zirconium. Unlike in a solid-state energy conversion medium, the impingement of energetic a particles would not give rise to displacement damage in the liquid gallium. Hence, the cell should have a long life, limited only by the half-life of Cm-244. A cell having a volume less than 25 cu mm, containing 1 curie of Cm-244 (the curie is a unit of radioactivity equal to 3.7 10(exp 10) disintegrations per second) is expected to deliver a current between 7 and 12 mA, which, at the expected open-circuit potential, would provide a power in the approximate range of 11 to 20 mW.

Patel, Jagdish U.↗

Effects of bentonite heating on U(VI) adsorption

Engineered barrier systems designed to isolate high-level radioactive waste utilize bentonite, a montmorillonite rich material, to restrict contaminant transport due to its low hydraulic conductivity and high adsorption capacity. High temperatures (100–200 °C) near waste canisters resulting from radioactive decay may alter the clay's ability to adsorb contaminants. In this study, we examine U(VI) adsorption onto two different bentonite samples subjected to (1) 18 years of in situ heating during an underground experiment and (2) short-term (7-week), high temperature (300 °C) heating in the laboratory. Results show that U(VI) adsorption was lower for field-heated bentonite located closest to the heater, which experienced temperatures of approximately 95 °C, compared to a control sample, which experienced temperatures of approximately 20 °C, over a range of aqueous chemical conditions. On average, K d values for U(VI) adsorption were 31% lower for 95 °C heated samples. By contrast, U(VI) adsorption onto intermediate-heated bentonite (50 °C) was indistinguishable from the adsorption onto the cold-zone (20 °C) sample. U(VI) adsorption onto lab-heated bentonite was also lower than onto control bentonite over the pH range 4.5–8.0, with an average decrease in K d values of 50% after heating. Lower U(VI) adsorption to field-heated bentonite persisted after bentonite was purified to isolate the clay fraction. This allows us to rule out changes in pore-water chemistry or accessory mineral composition as causes of the lower adsorption. No evidence of montmorillonite illitization was observed in the heated samples. While some of the lower U(VI) adsorption in the lab-heated bentonite can be explained by changes in aqueous U(VI) speciation, we propose that lower U(VI) adsorption to field-heated bentonite may be primarily due to changes in the montmorillonite edge structure. The observed changes in U(VI) adsorption to bentonite after heating have implications for U(VI) diffusive transport through engineered barriers and must be considered when designing radioactive waste disposal repositories.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The DISTINCTIVE University Consortium: Theme 2: PuO{sub 2} and Fuel Residues - 18132

The safe and secure management of Pu is a matter of serious international concern, with ∼250 t of separated Pu currently stockpiled worldwide. Nearly 50% of this material is in long-term storage in the UK whilst the British government develops its options for final treatment and disposition. Options for this are: (i) reuse as a fuel in modern reactors (e.g. as MOX fuel or within a fast reactor) prior to disposal; (ii) prompt immobilisation for disposal as soon as is practicable; or, (iii) continued long term storage (prior to disposition). The focus of the work presented here is options (ii) and (iii). The R and D needs of both are now pressing: in option (iii) due to it being the current default; in option (ii) because of a comparative lack of R and D on Pu conditioning and packaging due to policy uncertainty as to whether it would be disposed of in a Geologic Disposal Facility (GDF). Addressing these needs is complicated by Pu's high radioactivity, decay heat and radiotoxicity, nuclear safeguard requirements and, for some UK Pu contaminated materials targeted for disposal, poor inventory. Thus, there is also a critical requirement for underpinning research on characterisation methods for Pu bearing materials. In response to these needs, the DISTINCTIVE Consortium (Decommissioning, Immobilisation and Storage Solutions for Nuclear Waste Inventories, a multi-disciplinary collaboration of 11 universities and 3 key industry partners from across the UK's civil nuclear sector) has been seeking to: - Understand how the structure and properties of PuO{sub 2} change with time in the presence of H{sub 2}O. - Understand the roles these processes play in gaseous product evolution from PuO{sub 2} in storage. - Understand radiation-induced amorphization and dissolution kinetics of Pu waste forms. - Develop novel, fast neutron based radiometric methods for the quantification, isotopic composition assessment and remote imaging of Pu-bearing materials. This paper describes recent progress made towards achieving these objectives. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Backfilling of Geological Disposal Facilities - Development of Optimized Backfill Material - 18146

In Belgium, low- and intermediate-level waste (B-waste) will be conditioned in concrete monoliths and high-level waste (C-waste) in so-called Super-containers (SCs). The Belgian radioactive waste management program has focused on the disposal of these waste types in two emplacement fields of a geological disposal facility (GDF). When the disposal waste packages (DWP) have been emplaced, backfilling of the galleries is supposed to be carried out in order to stabilize the galleries, to reduce voids, to guarantee a favourable chemical milieu with regard to the retention of the radionuclides, to minimize a possible gas pressure build-up, to dissipate radioactive decay heat and to enable good conditions for a potential retrieval of the DWP. The current reference solution is to mix the backfill at the surface and then to pump the mixture through pipeline distribution systems into the underground structures. The catalogue of backfill material requirements comprises common, but also different requirements due to the characteristics of the B and C waste packages and differences in the backfilling systems. It was found that two backfill material recipes have to be developed. Different requirements, such as high porosity (low strength and low gas threshold pressure) and high thermal conductivity have contrary consequences for the material. In addition, during backfill production quality variations of the raw materials that influence the backfill material properties can occur. Different lengths of the delivery pipeline may require adjustments of the material composition. In order to consider the practical experiences of backfill material production, one focus of the development programs was to identify compositional ranges that guarantee the respective material property. A combination of the individual 'conformity fields' results in optimal solutions for the standard operating conditions as well as a compositional range that guarantees compliance with the required material specifications. (authors)

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Performance Assessment of a Generic Nuclear Waste Repository in Shale - 18392

A performance assessment (PA) is an important component of a comprehensive safety analysis for a nuclear waste repository. In a PA, probabilistic simulations of the total repository system are performed, and results are evaluated against performance metrics. Uncertainty and sensitivity analyses help prioritize additional research and model development. The United States Department of Energy (DOE) has been developing a state of the art PA simulation software tool-kit, Geologic Disposal Safety Assessment (GDSA) Framework, that couples increasingly higher fidelity models of subsystem processes into total system PA simulations. Over the past several years, PAs of generic repositories in three geologic media (salt, shale, and crystalline rock) have demonstrated ongoing developments in capability. The current PA of a nuclear waste repository in a generic shale formation showcases GDSA Framework, including capabilities in domain discretization (Cubit), multi-physics simulations (PFLOTRAN), uncertainty and sensitivity analysis (Dakota), and visualization (Paraview). The generic shale reference case considers the disposal of 22,000 metric tons heavy metal of commercial spent nuclear fuel (SNF) in a generic shale formation. PA simulations account for the thermal load and radionuclide inventory of the waste form, components of the engineered barrier system including waste package and buffer, and components of the natural barrier system including the host rock shale and underlying and overlying stratigraphic units. Two repository layouts are considered, one for emplacement of waste packages containing 12 pressurized water reactor (PWR) assemblies, and one for 4-PWR waste package emplacement. Model domains are half-symmetry and contain between 7 and 22 million grid cells. Grid refinement captures the detail of individual waste packages, emplacement drifts, access drifts, and shafts. Simulations are run in a high-performance computing (HPC) environment on 512 or 2048 processes. The governing equations describing coupled heat and fluid flow and reactive transport are solved with PFLOTRAN, an open-source, massively parallel multiphase flow and reactive transport code. Additional simulated processes include waste package degradation; waste form dissolution; radioactive decay and ingrowth in aqueous, solid, and adsorbed phases; and a simple biosphere based on a pumping well. Simulations are run to 106 y; dose and radionuclide concentrations are observed within aquifers at a point approximately 5 km downgradient of the repository. Dakota is used to sample likely ranges of input parameters including waste form and waste package degradation rates and properties of engineered and natural materials to quantify uncertainty in predicted concentrations and sensitivity to input parameters. Given the assumptions of the reference case, results of 12-PWR and 4-PWR simulations are very similar. Dose at the pumping well 5-km downgradient of the repository does not exceed 10-9 Sv/y. I-129 is the largest contributor to dose. The dose due to Cl-36, the next largest contributor, is orders of magnitude smaller. At the pumping well, the concentration of I-129 5-km downgradient does not exceed 10-14 mol/L. Rank correlation coefficients indicate that the maximum concentration of I-129 within the aquifer is sensitive to shale (repository host rock) porosity and aquifer permeability. These results affirm that HPC-capable codes can be used to simulate important multi-physics couplings directly in a total system performance assessment of a geologic repository, and can be used in prioritization of future research and model development. (authors)

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The TRANSCEND University Consortium: Theme 4: Nuclear Materials - 20431

The safe and secure management of Pu is a matter of international concern, with ∼250 t of separated Pu currently stockpiled worldwide. The UK's civil inventory of nuclear materials contains significant stocks of separated Pu from the reprocessing of Magnox and AGR spent fuels. The preferred option for the 138.5 tonnes of Pu is re-use as mixed oxide (MOx) fuel, although 5% is not suitable for re-use and is recommended for direct disposal. However, it will take more than 15 years to implement re-use, requiring that the Pu be kept in interim storage in its current state for that period, i.e. as PuO{sub 2} powder within inert steel storage cans at Sellafield. The focus of the work presented here is thus plutonium storage and the direct disposal of plutonium. The Research and Development needs of both are now pressing: in the case of storage due to it being the current default; in the case of immobilization and disposal because of a comparative lack of Research and Development on Pu conditioning and packaging due to policy uncertainty as to whether it would be disposed of in a Geologic Disposal Facility (GDF). Addressing these needs is complicated by Pu's high radioactivity, decay heat and radiotoxicity, criticality, nuclear safeguard requirements and, for some UK Pu contaminated materials targeted for disposal, poor inventory. Thus, there is also a critical requirement for underpinning research on Pu bearing materials in these two contexts. In response to these needs, the TRANSCEND Consortium (Transformative Science and Engineering for Nuclear Decommissioning, a multi-disciplinary collaboration of 11 universities and 8 key industry partners from across the UK's civil nuclear sector) is seeking to provide technical underpinning to ongoing option development for the UK's civil Pu stockpile. Whilst understanding the behaviour of plutonium during its re-use as MOx is beyond the scope of the TRANSCEND Consortium work plan, the main objectives of the work are: (1) For interim storage: to understand how the surface structure and properties of pristine and radiation damaged PuO{sub 2} change with time in the absence and presence of water; and (2) For immobilization and disposal: to understand the mechanisms of incorporation of Pu into ceramic and glass-ceramic waste-forms, as well as the effect on these of self-induced radiation damage. Each objective is being addressed through separate work packages, the details of which are discussed in this paper. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Long-term stewardship - surveillance and maintenance at Hanford - 15155

In FY 2015, Hanford's Long-Term Stewardship (LTS) Program is tasked to complete the required entries into five cocooned plutonium production reactors (105-C, 105-D, 105-F, 105-H and 105-N), which sit adjacent to the Columbia River. The first reactor entered in October 2014, the cocooned plutonium production reactor, 105-F, signaled the LTS Program's entry into the Surveillance and Maintenance (S and M) era. Reactor entries at Hanford are conducted at 5-year intervals to assess the condition of the structures and evaluate potential deterioration of the reactor core, shield walls and roof. The cocooned structures are designed to protect the reactor core for up to 75 years while radioactive decay continues, ultimately making the structures safe for demolition and removal. The 105-F entry demonstrates that the LTS program at Hanford is shifting from a program focused on transitioning cleaned up land and waste sites to a program focused primarily on S and M activities. The entry process is carefully planned, choreographed and monitored to ensure safety of the workers and minimize the time the reactor structure is opened. The process includes controlled opening of the reactor, air quality monitoring, structural safety inspections, and radiological clearance. Once the structure is cleared for entry, assessments of the structural integrity and radiologic conditions are completed. Evaluation of the interior temperature and flood monitoring equipment is conducted. Facility visits by regulators and DOE personnel close out the process prior to welding the door closed until the next assessment, five years later. This paper will document execution of the entry work package, identify challenges overcome, and provide video documentation as reference material for future workers and the public. The current LTS program has responsibility for approximately 100,000 acres, over 200 waste sites and six cocooned reactors. Just over 5,600 documents have been identified, indexed and tagged for storage in the LTS document library. The program has successfully completed seven consecutive transitions since July 2011, with six more transitions planned in the next 18 months to support the U.S. Department of Energy Richland Operations Office's (DOE-RL) near-term cleanup objectives to significantly reduce the footprint of active cleanup operations for the River Corridor. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗