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DOC-WMF - A Generic Model for Assessment of Waste Disposal Facilities - 19278

Numerical models and computer codes play an important role in the safety assessment of nuclear waste disposal facilities, as well as in the regulatory review of proponents' safety assessments. An important part of a safety assessment is the radiation dose calculation. This paper presents a computer code called DOC-WMF for calculating radiation dose from nuclear waste disposal facilities. DOC-WMF is a generic code that could be used for dose calculations for deep geological or near surface disposal facilities of nuclear wastes. DOC-WMF is much faster than complicated 3-D numerical models in terms of computational speed since the model uses the commercial code GoldSim as the computation engine which is based on analytical solutions for contaminant transport. As a result, it enables a user to quickly assess the dose consequences of multiple options or scenarios for a nuclear waste disposal facility. DOC-WMF was adapted from, and an improvement to, the Scoping of Options and Analyzing Risk (SOAR) model developed by the United States Nuclear Regulatory Commission (US NRC). A key improvement over the SOAR model is that DOC-WMF allows the calculation of dose contributions from other pathways such as food ingestion and air inhalation in addition to the drinking water pathway which is the sole dose contribution considered in the SOAR model. DOC-WMF also allows for: the consideration of 55 radionuclides with option to add more if required; the choice of source release method; various pathways to the biosphere; and dose calculations including an extended array of exposure pathways. In addition, DOC-WMF can simulate more complex hydrogeological settings and waste forms than SOAR does. DOC-WMF was compared against known analytical solutions for verification. It was then applied to two test cases and the results were compared. The first was a hypothetical deep geological disposal repository. The second test case was a near-surface nuclear waste disposal facility. DOC-WMF independently modeled these two test cases and achieved similar results as the more complicated numerical models did. (authors)

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A Salt Repository Concept for CSNF in 21-PWR Size Canisters

The most straightforward concept for disposal of large, heavy packages containing commercial spent nuclear fuel (CSNF) in a repository in bedded salt, would be to emplace them directly on the floor in emplacement tunnels. In-tunnel axially aligned horizontal emplacement would minimize excavated volume and avoid drilling of large-diameter emplacement boreholes. A similar concept was proposed in Germany for direct disposal of POLLUX ® canisters. The repository would be constructed at a depth of 500 to 1,000 m for isolation from the surface, and for sufficient overburden stress to ensure creep reconsolidation of repository openings. It could entail modular panels of emplacement tunnels arranged on headings oriented in cardinal directions from a central core, to accommodate the estimated 140,000 MTU total U.S. CSNF inventory. To do so, the overall area of the repository layout would be approximately 20 km 2 . Many layouts are possible, but the approach should be modular, excavation should be deferred for as long as possible to avoid maintenance, and the emplacement areas should share support facilities and shafts. Vertical shafts would be used in accordance with mining practice in sedimentary basins. Large diameter shafts would be needed for ventilation exhaust and waste transport, with smaller shafts for waste salt removal, men & materials, and ventilation intake. The spacing between disposal tunnels as estimated from thermal modeling, seeks to limit the maximum average areal thermal load in the panels to 11 W/m 2 to control long-term heat buildup in the host rock. Peak salt temperature would occur within a few years and would be dominated by each waste package locally, simplifying thermal management. There would be some flexibility to decrease the package spacing or increase the emplacement thermal power limit Backfilling emplaced waste packages immediately with mine-run crushed salt would provide shielding and expedite reconsolidation. This arrangement would isolate adjacent waste packages from one another by the intervening backfill, especially after it reconsolidates and its properties approach those of intact salt. After the repository is fully loaded and the performance confirmation program is complete, activities to permanently close the repository would be initiated. During closure operations all openings in the host salt would be backfilled, then shafts would be sealed, and boreholes plugged. Plans for the Waste Isolation Pilot Plant (WIPP) show how sealing and plugging could be done. A monitoring program could continue for 50 years or longer after repository closure. With an emplacement thermal power limit of 10 kW per waste package, nearly all the CSNF that is projected to be produced by the current fleet of reactors in the U.S. could be emplaced over a period of approximately 50 years starting in calendar 2048. No barriers to implementation in a reasonable timeframe have been identified from this generic analysis. Engineering challenges include: 1) shaft construction; 2) a very-large capacity shaft hoist; 3) overpack design; 4) a transport-emplacement-vehicle (TEV) for transporting waste packages once they are underground and emplacing them remotely; and 5) remotely operated equipment for emplacing backfill. The method of shaft construction would depend on site-specific conditions, and could involve freezing the subsurface. A shaft hoist with payload capacity of 175 MT seems technically and economically feasible based on development work in Germany, and it would be the largest hoist of its kind. The function of disposal overpacks would be to provide reliable containment during repository operations, which could be accomplished using a corrosion allowance material such as a low-carbon steel. Development effort would be needed to determine overpack thickness (e.g., 7 to 20 cm) that can resist corrosion and loading from salt creep, to rovide containment throughout the repository operational period. The transport-emplacement vehicle (TEV) would be similar to previous concepts, particularly one option proposed for a Yucca Mountain repository. It would move over a rough salt floor on independently driven and steered wheels, and carry heavy shielding in addition to a waste package. By analogy to the safety case for the WIPP in New Mexico, human intrusion is likely to be the dominant mode of radionuclide release from the repository. Treatment of human intrusion for a CSNF repository in salt could depend on promulgation of site-specific changes in the regulations. Radionuclide release and migration would be quite limited for undisturbed conditions. There may be opportunities for improved understanding of salt performance with waste heating, based on future in situ testing in an underground salt research laboratory. This report also discusses a developing area of salt rock mechanics that involves low-stress, low strain-rate creep that might cause large, heavy waste packages to slowly sink. Site-specific sampling, testing, and modeling would be used to determine if the mechanism is important enough to merit consideration in design, or inclusion in performance assessment. Part of engineering design and postclosure safety assessment for a CSNF repository in salt would be to implement a methodology to show that the probability of a criticality event in the repository, when waste packages eventually breach and are flooded, is less than the probability screening threshold for performance assessment. In the methodology, a criticality analysis would be performed for waste packages in the repository, incorporating measures that could be introduced as needed to limit reactivity, for example using fuel selection and loading rules, and crediting the absorption of thermal neutrons by natural chlorine in the environment. A similar analysis has been underway for CSNF stored in dual-purpose canisters. Ideally the strategy would be developed prior to actually loading SNF assemblies into canisters used in waste packages for disposal.

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Results of Re-evaluation of FEPs Related to Implementing the ABD Glass Program

The Savannah River Site plans to reprocess defense spent nuclear fuel currently stored in their L-Basin via the Accelerated Basin Deinventory (ABD) Program. The previous plan for the L-Basin spent nuclear fuel was to dispose of it directly in the federal repository without reprocessing. Implementing the ABD Program will result in final disposal of approximately 900 fewer canisters of defense spent nuclear fuel and the production of approximately 521 more canisters of vitrified high-level waste glass with some specific differences from the planned high-level waste glass. Because the 235U in the L-Basin spent nuclear fuel is not intended to be recovered, the fissile mass loading of the vitrified high-level glass waste form to be produced must be increased above the current value of 897 g/m 3 to a maximum of 2,500 g/m 3 . Therefore, implementing the ABD Program would produce a variant of high-level waste glass—the ABD glass—that needs to be evaluated for future repository licensing, which includes both preclosure safety and postclosure performance. This report describes the approach to and summarizes the results of an evaluation of the potential effects of implementing the ABD Program at the Savannah River Site on the technical basis for future repository licensing for a generic repository that is similar to Yucca Mountain and for one that is fully generic. This evaluation includes the effects on preclosure safety analyses and postclosure performance assessment for both repository settings. The license application for the proposed Yucca Mountain repository (DOE 2008), which is serving as a framework for this evaluation, concluded that the proposed Yucca Mountain repository would meet all applicable regulatory requirements. The evaluation documented in this report found that implementing the ABD Program is not expected to change that conclusion for a generic repository similar to Yucca Mountain or for a generic repository with respect to the preclosure safety analyses. With respect to the postclosure performance of a generic repository, no concerns were identified.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Update on Development of a U.S. Rail Transport Capability for Spent Nuclear Fuel and High-Level Waste - 20466

This paper provides an overview of the progress to date, and discussion of the path forward, related to designing, fabricating and testing prototype railcars that will comply with the safety standard S-2043. This standard was developed by the Association of American Railroads (AAR) specifically for railcars used to transport High-Level Radioactive Material (HLRM). AAR defines the term HLRM to include both spent nuclear fuel (SNF) and high-level radioactive waste (HLW). DOE is in the process of developing and testing prototype railcars that will satisfy Standard S-2043. This is a technical paper that does not take into account contractual limitations or obligations under the Standard Contract for Disposal of Spent Nuclear Fuel and/or High-Level Radioactive Waste (Standard Contract) (10 CFR Part 961). For example, under the provisions of the Standard Contract, spent nuclear fuel in multi-assembly canisters is not an acceptable waste form, absent a mutually agreed to contract amendment. To the extent discussions or recommendations in this paper conflict with the provisions of the Standard Contract, the Standard Contract governs the obligations of the parties, and this paper in no manner supersedes, overrides, or amends the Standard Contract. This paper reflects technical work which could support future decision making by the Department of Energy (DOE or Department). No inferences should be drawn from this paper regarding future actions by DOE, which are limited both by the terms of the Standard Contract and a lack of Congressional appropriations for the Department to fulfill its obligations under the Nuclear Waste Policy Act including licensing and construction of a spent nuclear fuel repository. (authors)

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WastePD, an innovative center on materials degradation

The US Department of Energy recently awarded funds to create the Center for Performance and Design of Nuclear Waste Forms and Containers (WastePD) as part of the Energy Frontier Research Center (EFRC) program. EFRCs are multi-investigator collaborations of universities, national labs and companies that “conduct fundamental research focusing on one or more “grand challenges” and use-inspired “basic research needs” identified in major strategic planning efforts by the scientific community.” The major performance parameter of nuclear waste forms is their ability to isolate the radionuclides by withstanding degradation in a repository environment over very long periods of time. So WastePD is at heart a center focused on materials degradation.

36 MATERIALS SCIENCE↗

Optimization of Deep Borehole Systems for HLW Disposal

This is the final report on a project to update and improve the conceptual design of deep boreholes for high level nuclear waste disposal. The effort was concentrated on application to intact US legacy LWR fuel assemblies, but conducted in a way in which straightforward extension to other waste forms, host rock types and countries was preserved. The reference fuel design version consists of a vertical borehole drilled into granitic bedrock, with the uppermost kilometer serving as a caprock zone containing a diverse and redundant series of plugs. There follows a one to two kilometer waste canister emplacement zone having a hole diameter of approximately 40-50 cm. Individual holes are spaced 200-300 m apart to form a repository field. The choice of verticality and the use of a graphite based mud as filler between the waste canisters and the borehole wall liner was strongly influenced by the expectation that retrievability would continue to be emphasized in US and worldwide repository regulatory criteria. An advanced version was scoped out using zinc alloy cast in place to fill void space inside a disposal canister and its encapsulated fuel assembly. This excludes water and greatly improves both crush resistance and thermal conductivity. However the simpler option of using a sand fill was found adequate and is recommended for near-term use. Thermal-hydraulic modeling of the low permeability and porosity host rock and its small (≤ 1%) saline water content showed that vertical convection induced by the waste’s decay heat should not transport nuclides from the emplacement zone up to the biosphere atop the caprock. First order economic analysis indicated that borehole repositories should be cost-competitive with shallower mined repositories. It is concluded that proceeding with plans to drill a demonstration borehole to confirm expectations, and to carry out priority experiments, such as retention and replenishment of in-hole water is in order.

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Assessing the Consequences of Postclosure Criticality in Spent Nuclear Fuel

The U.S. Department of Energy is funding research into studying the consequences of postclosure criticality on the performance of a generic repository by (1) identifying the features, events, and processes (FEPs) that need to be considered in such an analysis, (2) developing the tools needed to model the relevant FEPs in a postclosure performance assessment, and (3) conducting analyses both with and without the occurrence of a postclosure criticality and comparing the results. Here, this paper describes progress in this area of research and presents the results to date of analyzing the consequences of a postulated steady-state criticality in a hypothetical saturated shale repository. Preliminary results indicate that postclosure criticality would not affect repository performance.

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An Integrated Multiscale Experimental-Numerical Analysis on Reconsolidation of Salt-Clay Mixture for Disposal of Heat-Generating Waste (Final NEUP Technical Report)

The overall purpose of this research is to improve understanding of THMC coupling effect on the reconsolidation of granular (or crushed) salt-clay mixture used for seal systems of shafts and drifts in salt repositories. This proposed work is partially motivated by the recent work on the Waste Isolation Pilot Plant (WIPP) that shows the promising sealing capability of clay-salt mixture compared to crushed salt. In particular, primary emphasis is to develop a fully integrated multiscale experiment-numerical study to determine and explain what leads to the superior sealing ability of the clay-salt mixture. These research activities are designed to seek further understanding of (1) why clay additives may enhance the fluid trapping and (2) whether this flow barrier effect may prevail under different combinations of temperature, confining pressure, deviatoric stress and other foreseeable environmental factors. If successful, this enhanced flow trapping ability of the seal provides significant improvement to the seal and repository performance and therefore make the repository safer in the long-term. The experiment component includes microstructural investigation and macroscopic tests on a reconsolidated salt-clay mixture. In the microstructural study, the goal is to (1) characterize microscopic distributions of distinct phases (e.g., clay, salt crystal boundaries, trapped brine, and pore) to examine the connectivity of the pore network inside the salt-clay mixture with different amounts of clay additive and moisture content and (2) analyze multiscale imaging data to reconstruct the polycrystalline microstructures for numerical simulations. Meanwhile, macroscopic tests are performed to analyze how clay alters the failure/creep mechanisms in the salt-clay mixture. Microscopic and macroscopic experimental observations will both be used to calibrate and validate a multiscale model that explicitly simulates the capillary and multiphase flow in the connected pores and the deformation due to the presence of intra-crystalline brine at the pore scale via a new polyhedral discrete element–lattice Boltzmann method (DEM-LBM) coupling model. The pore-scale simulations are homogenized via an upscaling procedure that converts pore-scale information (e.g. force exerted on grain boundary, sliding, pressure-solution) to continuum measures (e.g. Cauchy stress, Darcy’s flow) at each integration point in the macroscopic multiphase TMHC model. This multiscale scheme will allow coupling be- tween high-fidelity simulations of brine-salt-clay interaction and the macroscopic TMHC model. The multiscale model helps the understanding of how the trapped brine inclusion affects the pressure-solution mechanism with the presence of clay and moisture. This work brings new insight into the sealing capacity of salt-clay mixture under elevated temperature over a long period of time - a key to evaluating the potential of salt-clay mixture usage for salt repositories.

42 ENGINEERING↗

Does the Perfect Waste Package Exist? Development of a Decisional Tool Addressing this Challenge - 17053

The definition of a safe, technically, economically and societally acceptable waste management strategy is highly dependent on the Waste Acceptance Criteria in each country and on the already available disposal routes. It is the reason why there is not a single solution but a combination of optimized solutions depending on the type of waste and on each country's considerations. In fact, when operating a nuclear plant or performing its decommissioning or legacy waste management, one has to consider a large waste diversity in term of natures, types, volumes and radioactivity spectra. All nuclear operators have to take-up the challenge of implementing solutions for conditioning its waste in packages suitable for transport short to long term interim storage and final disposal of it (or prepare for final disposal if the repository is not yet available). Operators have then to answer the following dilemma: either define a complete strategy packaging the waste for final disposal, or 'containerising' it temporarily, pending final disposal. The strategy is highly country dependent; in the first case, one has to take into account the available information and future orientations relative to acceptability of the packages in order to define a robust solution. The approach implemented in France requires a close dialogue between the Operators, the Safety Authority, the Administration and the stakeholders. Moreover it pushes forward whenever possible standardization, contributing to cost minimization. If the second approach has the advantage of leaving the options open, and reducing the initial investments, it inevitably requires future retrieval and re-packaging with potential evolutions/degradation of the initial waste form. It also induces the potential risk to produce additional secondary waste. As an additional drawback, it introduces uncertainties and unknowns related to the future waste management criteria and to the costs. The general idea is that, depending on context, a given route (i.e., treatment, conditioning, and transport), could be considered as efficient or not. Assessing a waste package is certainly highly context dependent. However it should be possible to recognize and to lead an evaluation based on a number of fixed criteria, whatever the context, to be addressed when assessing the development of a final waste package in connection to the overall management route. A waste package is always a combination of a waste container and a waste form and will have to be transported one day from the production site to the final repository or to off-site interim storage facilities. AREVA's approach consists in defining an evaluation grid based on a set of criteria which aim (i) to evaluate whether the different waste treatments, conditionings, transport and packages deserve to be considered within different national contexts, and (ii) to evaluate R and D actions to be performed for improving existing solutions or developing new ones. One of the key lessons to be drawn from AREVA's experience in developing waste packages is that the perfect waste doesn't exist even though the vitrified canister is probably the most efficient one. The performance of a package resulting from a compromise depends on context and is a strength combination between the waste container and the waste form. The approach is to evaluate a waste package development against different set of criteria and to draw optimization diagrams. In such diagram, a given waste package is assessed with respect to selected criteria such as waste form and waste container, stability, level of waste incorporation, integrity lifetime, secondary waste generation, transport, long term behavior, and economical effectiveness, etc. Addressing a waste form is a very key point. This evaluation grid and comparative approach will be presented through examples and comparison providing from AREVA feedback on waste package development related to complex waste management such as problematic waste or legacy waste. (authors)

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Use of Automation in Low Level Waste Storage and Management - 19227

The Australian Nuclear Science and Technology Organisation (ANSTO) generates Low Level Waste (LLW) and Intermediate Level Waste (ILW) from various site operations such as the operation of a research Reactor and the manufacture of Molybdenum 99. The Low Level Solid Waste (LLSW) generated is stored at ANSTO before and after conditioning. The current process flow involves the storage of LLSW waste before conditioning on racks, handled using forklifts. When the unconditioned waste is ready for conditioning, it is transferred to another facility, where volume reduction and packaging is carried out. Once conditioned, the waste is placed in further storage, pending dispatch to the proposed Australian National Radioactive Waste Management Facility (NRWMF). A new purpose built facility has been constructed, adjacent to the LLSW processing facility, for the storage and management of LLSW in both unconditioned and conditioned forms. This new facility will streamline the waste management process and significantly enhance the safety and efficiency of the process. In line with international best practises, the new facility utilises automation solutions to minimise the build footprint, and minimise the use of forklifts and other mobile plant. Most importantly, it applies the principle of ALARA (As Low as Reasonably Achievable) to minimise operator activities in areas where radioactive material is stored and eliminates double handling of the waste. The automation for unconditioned waste utilises an Automated Storage and Retrieval System (ASRS), a vertical stacker crane within high density racking, to provide easy storage and retrieval for processing and/or routine inspections. This system allows operators to control it from outside of the storage area whilst utilising integrated software that allows for the required tracking of the unconditioned waste. From the ASRS storage area, unconditioned waste will have a smooth transition to the processing facility which is located adjacent to the ASRS system. Once conditioned, the waste is catalogued and returned to a designated storage area within the new facility using an automated building gantry crane with a target delivery system to eliminate the need for operators in the main storage bay. The waste will be held here in preparation for dispatch to the future repository. The utilisation of the ASRS for the purpose of storing LLSW is an innovative use of automation that will eliminate operators from active areas, reduce dose rates received and integrate with the waste tracking software. Furthermore, the system has significant advantages with operational efficiencies increased, reduced double handling of nuclear waste and maximum use of building footprint. (authors)

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Andra's strategy and approach for operational safety of French underground facility Cigeo - 15127

According to the French Act on radioactive waste of 28 June 2006, Andra shall design a reversible repository. In response to this demand, Andra is developing the industrial project namely 'Cigeo', a reversible geological disposal facility for HLW and ILW located in Meuse/Haute-Marne. The previous safety cases of 2005, 2009 and 2012 give a sound basis to assess Cigeo's safety both for the operational and post-closure periods. Regarding operational safety, in this new stage of the project, the challenging issues for the preparation of the safety case are the following: - To adapt the various regulatory frameworks (nuclear and non-nuclear) to the underground facility - To design the underground facility and handling equipment's to reduce at first risks in the underground facility as such radioactive particles release, gas explosion, fire and co-activity and limit their consequence. - To establish waste acceptance criteria to be fulfilled by waste producers in line with operational safety and design options. The objective of the paper is to present the experience of Andra in operation safety of the underground facility of Cigeo. Operational safety for Cigeo is assessed as much as possible according to the existing French regulations and guidance for nuclear facilities. Indeed, compared to existing nuclear facilities, a geological repository is a specific case due to the existence of underground facilities with particularities such as: - ventilation management in a large scale underground facility, - fire risk management. As an input for the industrial design of Cigeo for operation, Andra defined a fire guidance and a specific reference safety guidance, based on the adaptation of the French nuclear regulatory texts for and when feasible to mines and tunnels regulatory texts and on its own experience gained through safety operational reports since 2005 and their reviews by the Safety Authority. - underground co-activity of nuclear operation with construction works. According to the common 'defense-in depth' principle for nuclear facilities, these guidelines for the industrial design of Cigeo for operation consider the successive levels of defense of: - Preventing the risk and its spreading by design and construction; - Detecting incidents and early fighting by design and operation dispositions (detection and control systems, survey procedure); - Controlling incidents and limiting of their consequences by safeguarding systems, specific procedures. At that stage, design options for Cigeo constitute an adequate response to the operational safety functions and requirements: - Two levels of containment are set up: the first one is ensured by the waste package, the second one is ensured from the surface facility to the disposal vaults by the transfer cask during the transfer of waste packages in the disposal vaults by the disposal vault itself and a nuclear ventilation with HEPA filter; - Favorable options for fire risk prevention and mitigation: transport system minimizing heat load (cable car for the transfer from the surface, electric transfer engines), twin access tunnels to ease fire-fighting and evacuation...; - Permanent complete physical separation of nuclear zone and construction zone (including ventilation systems). In practice, operation safety assessment of Cigeo, designed following the aforesaid reference safety guidelines, follows a common risk analysis (internal aggressions such as auxiliary losses, chemical and toxic risks, fall or collision, fire, human factors and external aggressions such as earthquake, air traffic, flooding) with the following steps: - Identification of the major risks and the design basis scenarios that have to be considered for dimensioning of the installations and the safety devices; - On the basis of these different situations, those who will have to be quantified are identified; one or more representative and envelop situations are chosen in order to evaluate robustness of the installation. Quantitative evaluation of these situations permits to: - identify the consequences on man, environment and installation, and in particular to gain confidence in the maintaining of the safety functions; - identify or define the technic and/or organisational dispositions classified as 'important elements for protection' (IEP); - Situations beyond dimensioning permit to verify the robustness of the installation. They permit, on one hand to identify possible complementary material or organisational dispositions; on the other hand, to define the 'hard core' i.e. structures, systems and components that permit to maintain the confinement function of radioactive substance. (authors)

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History and Status of DOE’s Standardized Canister – 19657

The U.S. Department of Energy (DOE) is responsible for managing spent nuclear fuel (SNF) that is currently in, or will in the future come into, its possession. The DOE standardized canister will be relied upon to confine radionuclides and preclude moderator in order to ensure safe, long-term management and disposition of DOE SNF. This strategy offers an avenue for avoiding the characterization costs (i.e. funds and exposure) and other technical challenges associated with the traditional approach of relying on fuel-specific properties as the basis for demonstrating compliance with the regulator. The use of the standardized canister offers the following benefits: • The standardized canister design is complete. It has been tested under a variety of drop and accident scenarios and was subsequently licensed under 10 CFR 72 as a storage system as part of the FWENC Facility. It is also part of the license submittal for Yucca Mountain. • There is high confidence that the standardized canister design can be stored within commercially available storage casks and licensed as part of a transportation-system package. • The robustness of the standardized canister simplifies accident analyses and does not rely on characterization of the contained waste. This simplifies safety analysis, provides a greater level of confidence with stake holders and reduces cost and risk. • Significant savings result from a common design for the associated packaging, closure, and loadout facilities. • Design efforts, procurement, and fabrication are simplified • Safety and surety of operations are enhanced by standardizing handling activities and associated training, procedures, equipment, and tooling. The standardized canister is the preferred package for these materials and has withstood scrutiny by the Yucca Mountain Repository License Application, the NRC’s Advisory Committee on Nuclear Waste, the Nuclear Waste Technical Review Board, an American Society of Mechanical Engineers peer review, and the Foster Wheeler Environmental Corporation storage license application. This evaluation summarizes and documents the status of the design and rationale for the DOE standardized canister and outlines the remaining needs to allow deployment. In addition, it discusses the factors that have the potential to influence storage, transportation, and disposal of DOE SNF.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Thermal Evolution near Heat-Generating Nuclear Waste Canisters Disposed in Horizontal Drillholes

We consider the disposal of spent nuclear fuel and high-level radioactive waste in horizontal holes drilled into deep, low-permeable geologic formations using directional drilling technology. Residual decay heat emanating from these waste forms leads to temperature increases within the drillhole and the surrounding host rock. The spacing of waste canisters and the configuration of the various barrier components within the horizontal drillhole can be designed such that the maximum temperatures remain below limits that are set for each element of the engineered and natural repository system. We present design calculations that examine the thermal evolution around heat-generating waste for a wide range of material properties and disposal configurations. Moreover, we evaluate alternative layouts of a monitoring system to be part of an in situ heater test that helps determine the thermal properties of the as-built repository system. A data-worth analysis is performed to ensure that sufficient information will be collected during the heater test so that subsequent model predictions of the thermal evolution around horizontal deposition holes will reliably estimate the maximum temperatures in the drillhole. The simulations demonstrate that the proposed drillhole disposal strategy can be flexibly designed to ensure dissipation of the heat generated by decaying nuclear waste. Moreover, an in situ heater test can provide the relevant data needed to develop a reliable prediction model of repository performance under as-built conditions.

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Development of an ERT‐Based Framework for Bentonite Buffers Monitoring From Laboratory Tests: 1. Characterizing Thermal–Hydrological–Mechanical Processes

Abstract Bentonite clay is widely used in engineered barrier systems for the permanent disposal of high‐level radioactive waste due to its low permeability, high swelling capacity, and thermal stability. However, the complex thermal‐hydrological‐mechanical (THM) processes induced by heating from decaying radioactive waste and hydration from surrounding rock can lead to heterogeneous changes that are difficult to measure and predict. This study develops an Electrical Resistivity Tomography (ERT)‐based framework for monitoring THM processes, progressing from sample‐scale to bench‐scale tests, to inform field‐scale applications. Sample‐scale tests analyzed small bentonite samples under controlled variations in water content, temperature, and porosity to establish fundamental resistivity relationships. Bench‐scale tests involved larger bentonite columns subjected to heating (up to 200°C) and hydration under controlled pressure, simulating repository conditions. ERT measurements, complemented by X‐ray CT imaging, temperature monitoring, and tracing sensors, revealed coupled THM processes, such as hydration‐induced compression, swelling, and thermal gradients, leading to complex resistivity patterns. The results demonstrate the potential of ERT for capturing THM‐induced resistivity changes, though challenges remain in upscaling and quantitative analysis. This study evaluates laboratory test capabilities and proposes future improvements for understanding THM‐induced resistivity responses. A conceptual framework for ERT implementation in field‐scale monitoring is presented, synthesizing findings from both scales and exploring how ERT data can inform long‐term modeling and reduce prediction uncertainties. Overall, this ERT‐based framework offers a robust method for monitoring bentonite buffers, aiding in early issue detection and supporting the safe long‐term disposal of radioactive waste in geological repositories, while highlighting the need for future development. Plain Language Summary Bentonite clay is crucial in engineered barrier systems (EBS) for containing high‐level radioactive waste due to its ability to absorb water, swell, seal and remain stable under high temperatures. When bentonite absorbs water and heats up from radioactive decay, it experiences complex changes in its physical and mechanical properties. Understanding these changes is important for ensuring the long‐term safety and effectiveness of EBS. This study used Electrical Resistivity Tomography (ERT), a non‐invasive method that measures electrical conductivity to monitor these changes during laboratory experiments. The ERT data revealed significant variations in resistivity corresponding to changes in water content, temperature, and density, providing detailed spatial and temporal insights into the behavior of bentonite. These findings enhance our ability to predict the long‐term performance of bentonite barriers, ensuring the safe containment of radioactive waste. By improving our understanding of bentonite's behavior, this research supports the development of more reliable and effective barrier systems for radioactive waste disposal, protecting the environment and public health. Key Points ERT monitoring was employed to capture resistivity changes in bentonite during controlled heating and hydration experiments, providing insights into THM processes ERT data reveal significant resistivity changes correlated with water content, temperature, and mechanical effects, enhancing the understanding of THM dynamics in bentonite This study explores the potential of the framework for application in field‐scale EBS monitoring, emphasizing the need for integrating additional geophysical methods for comprehensive subsurface imaging

Chen, Hang↗

Effect of Anoxic Iron Corrosion on WIPP Brine Geochemistry FY23 Final Report (U)

A 280-day study was completed to evaluate the effect of zero-valent iron (Fe 0 ) on the Waste Isolation Pilot Plant (WIPP) brine geochemistry under anticipated reducing conditions. Hydrogen (H 2 ) gas is expected to be present in the repository after closure due to the anoxic corrosion of a vast quantity of iron contained in the waste forms disposed at WIPP; therefore, a background argon atmosphere containing H 2 was chosen for this study. WIPP groundwater brine pH and E h will impact the mobility and fate of plutonium within the repository. Modeling and laboratory results for Castile WIPP brine indicate that equilibrium fa values relative to the standard hydrogen electrode (SHE) are 40 mV more reducing (i.e., more negative) than those for Salado WIPP brine (-480 mV vs. -440 mV, respectively) because of the higher pH of the Castile brine (pH 9 .3 for Castile vs. pH 8.8 for Salado). The E h and pH data were corrected for the effects of high ionic strength. The experimental results for both brines are consistent with thermodynamic predictions using OLI Systems' Mixed Solvent Electrolyte chemical equilibrium model. The measured and corrected pH and E h data from this study are provided in Table ES-I and Table ES-2, respectively. The experimental study, with four test conditions in triplicate, was performed in a dual glovebox with a nominally 3 vol.% H 2 in argon atmosphere (target H 2 range: 3 ± I vol.%). Simulants containing MgO only ( experimental control) and MgO+Fe 0 (WIPP base case) were prepared for both the Salado and Castile brines. MgO was included in all simulants to account for the use of bulk magnesium oxide in the WIPP repository. Fe 0 was included in some simulants to incorporate the effects of the anoxic corrosion of iron and in-situ hydrogen generation in the study. The brine compositions were developed by Sandia National Laboratory (SNL; Xiong, 2008) and have been used in previous WIPP evaluations. The test method (agitation, etc.) is partially based on ASTM D3987-12. Twelve rounds of periodic measurements of pH and E h were performed over the course of the study. Chemical analysis results for liquids and solids (ICP-MS, ICP-ES, IC Anion, TIC, SEM-EDX) are consistent with the pH, E h , and thermodynamic modeling results. This study included the following conditions that deviate from anticipated post-closure conditions following brine intrusion, but were selected to facilitate bench-scale testing to validate modeling of pH and E h for the post-closure WIP P repository: an anoxic glove box atmosphere containing ≤ 4 vol. % H 2 vs. substantially higher H 2 gas concentrations assumed in the WIPP Performance Assessment (PA); a significantly higher liquid-to-solid test ratio compared to the much lower phase ratio anticipated in the WIP P repository; agitation of the simulant bottles to maximize mass transfer; and finally the use of Fe 0 reagents having a much greater surface area than expected in the WIP P repository. Non-representative conditions were chosen for various reasons such as: to provide bounding conservative results, to provide a margin of safety for testing, or to facilitate simulant sub-sampling and analysis. In a parallel effort, aqueous electrolyte thermodynamic models were developed for the synthetic Salado and Castile brines to inform the experimental design, facilitate laboratory data interpretation, and allow extension of evaluations beyond the parameters tested. Thermodynamic modeling simulations including the MgO and Fe 0 additives that are directly relevant to the experimental measurements (e.g., pH calibration curve, ORP corrections) are included in this report. The measured fa of the simulants was close to the OLI model predictions for both brines and was largely controlled by the background H 2 partial pressure in the vapor phase as well as H 2 generated in situ in the aqueous phase by the Fe 0 corrosion. The H 2 gas-phase concentration tested and thermodynamically evaluated was much lower than is assumed in the WIPP PA; however, H 2 (g) concentrations significantly below this level are still predicted to result in very reducing conditions. In conclusion: • The experimental results are consistent with thermodynamic model predictions for fa, pH, and the effects of high ionic strength. • Evidence to date suggests that the H2 concentration in the glovebox atmosphere ultimately determined the final E h values of the simulants and resulted in highly reducing conditions. As a result, little difference was observed between the control simulants containing only MgO and the WIPP base-case simulants that contained MgO and Fe 0 . • This test methodology is recommended for future studies evaluating WIPP repository conditions. The methodology includes: (1) background H 2 in argon with agitation ( or could alternatively include in-situ-generated H 2 in sealed bottles); (2) carefully measured and corrected ORP data ( with much effort focused on allowing the probes to fully stabilize); and (3) ionic-strength-corrected pH data. Other best practices, such as simulant sparging/handling, ORP probe replacement, etc., should also be considered. • The coupling of experimental studies and thermodynamic modeling is also highly recommended because these methods inform and direct one another leading to greater confidence in and understanding of the results.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Effect of Anoxic Iron Corrosion on WIPP Brine Geochemistry FY23 Final Report (U)

A 280-day study was completed to evaluate the effect of zero-valent iron (Fe 0 ) on the Waste Isolation Pilot Plant (WIPP) brine geochemistry under anticipated reducing conditions. Hydrogen (H 2 ) gas is expected to be present in the repository after closure due to the anoxic corrosion of a vast quantity of iron contained in the waste forms disposed at WIPP; therefore, a background argon atmosphere containing H 2 was chosen for this study. WIPP groundwater brine pH and E h will impact the mobility and fate of plutonium within the repository. Modeling and laboratory results for Castile WIPP brine indicate that equilibrium E h values relative to the standard hydrogen electrode (SHE) are 40 mV more reducing (i.e., more negative) than those for Salado WIPP brine (-480 mV vs. -440 mV, respectively) because of the higher pH of the Castile brine (pH 9.3 for Castile vs. pH 8.8 for Salado). The E h and pH data were corrected for the effects of high ionic strength. The experimental results for both brines are consistent with thermodynamic predictions using OLI Systems' Mixed Solvent Electrolyte chemical equilibrium model. The measured and corrected pH and E h data from this study are provided in Table ES-1 and Table ES-2, respectively.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Radiological characterization of high Cs-137 waste items at LANL combining Cs-137 NDA results and acceptable process knowledge - 15592

Radiological characterization is an important component to disposition and disposal of radioactive waste at the Los Alamos National Laboratory. Gamma and neutron based non-destructive assay systems are available at LANL's TA-54 Area G for radiological characterization and are generally very effective in quantifying the transuranic radionuclide concentration required for a TRU or low level waste disposition determination. This is routinely performed by scaling some nuclides to direct assay results using acceptable process knowledge scaling from a directly measured key TRU nuclide, e.g., for gamma systems using a standard isotopic distribution to determine the amount of Pu-240 associated with a measured value of Pu-239. However, for two groups of LANL waste items that have high levels of Cs-137, these non-destructive assay systems were unable to make a standard TRU/LLW determination. Therefore, it was necessary to apply an extension of the typical scaling technique that keyed in on the direct Cs-137 gamma assay result to effectively characterize these waste items for TRU processing or LLW disposition. Two basic types of waste packages contained the high Cs-137 waste requiring special scaling: drums and boxes. The drums included 55-gallon, 85-gallon and 110-gallon volume sizes and the boxes included a corrugated metal box, a Standard Waste Box, and several overpack boxes containing oversized waste. All of these items contained radioactive waste generated from operations at the Chemistry and Metallurgical Research facility at LANL that included hot cell, metallographic sectioning and maintenance activities. All of the drums as well as the CMB, SWB and one oversized item in a plywood box were located above-ground at LANL's TA-54 Area G, while five of the oversized items were hot cell liners in metal boxes stored below-ground in shafts. All of the items were measured in the 2013-2014 time period at TA-54 Area G with LANL NDA systems. Most of the items were counted with LLW certified far-field gamma spectroscopy systems employing portable far-field HPGe detectors and carts and some of the items were counted on WIPP certified gamma only or gamma with neutron NDA systems. In all cases Cs-137 was quantified directly with a gamma measurement but the key TRU nuclides were not detectable. Thus, for each waste item AK/PK was studied and scaling factors to Cs-137 were established and applied to provide a comprehensive radiological characterization. A total of 49 waste items were successfully characterized as LLW based on this technique. The above ground waste items were dispositioned and disposed of at an offsite LLW repository and the below ground boxes were left in place as LLW in the TA-54 Area G shafts. This NDA with scaling application has proved effective and defensible in these high Cs-137 cases at LANL and will continue to be used as applicable and appropriate for future waste characterization at LANL. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Using Atom Dynamics to Map the Defect Structure Around an Impurity in Nano-Hematite

The geochemical cycling of actinides such as U is strongly controlled by Fe (oxyhydr)oxides. Indeed, the strong affinity of these minerals for U has factored into the design of geologic repositories for the long-term storage of nuclear waste. Many decades of work have focused on detailing the local coordination environment U associated with hematite (a-Fe2O3), a common and stable Fe(III) oxide, in order to better predict the fate and transport of U in the sub-surface. Here, for the first time, molecular dynamic simulations and atomically resolved electron microscopy of uranium atom mobility under the beam were used to map the topology of defect clusters surrounding structurally incorporated U in hematite. The ability to observe vacancies by means of metal atom hopping can be used to directly probe defects in other materials, with promising applications in geochemistry and materials science.

Ilton, Eugene S.↗