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At least 577 records · Page 32

Postclosure Criticality Consequence Analysis - Scoping Phase

Commercial generation of energy via nuclear power plants in the United States (U.S.) has generated thousands of metric tons of spent nuclear fuel (SNF), the disposal of which is the responsibility of the U.S. Department of Energy (DOE) (Nuclear Waste Policy Act of 1982). Any repository licensed to dispose of the SNF must meet requirements regarding the long-term performance of the repository. In evaluating the long-term performance of the repository, one of the events that may need to be considered is the SNF achieving a critical configuration. Of particular interest is the potential behavior of SNF in dual-purpose canisters (DPCs), which are currently being used to store the SNF but were not designed for permanent disposal. As part of a multiyear plan that is currently being developed for the DOE, a two-phase study has been initiated to examine the potential consequences, with respect to long-term repository performance, of criticality events that might occur during the postclosure period in a hypothetical repository containing DPCs. Phase I, a scoping phase, consists of generating an approach intended to be a starting point for the development of the modeling tools and techniques that may eventually be required either to exclude criticality from or include criticality in a performance assessment (PA) as appropriate. The Phase I approach will be used to guide the analyses and simulations done in Phase II to further the development of these modeling tools and techniques as well as the overall knowledge base. The purpose of this report is to document the approach created during Phase I. The study discussed herein focuses on the consequences of criticality in a DPC; it does not address the probability of occurrence of a criticality event. This approach examines two types of criticality events for SNF disposed of in a single type of DPC: a steady-state criticality and a transient criticality. The steady-state critical event is characterized by a relatively low constant power output over 10,000 years, while the transient critical event is characterized by a power spike that lasts on the order of seconds. Possible effects of the criticality are an increase in the radionuclide inventory; an increase in temperature; and a change in the chemistry inside the waste package, along with a change in radionuclide solubilities, fuel degradation rates, and steel corrosion rates. Additionally, for transient criticality the possibility of mechanical damage to the engineered and natural barriers also exists.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Development of Alternative Technetium Waste Forms

The UREX+1 process is under consideration for the separation of transuranic elements from spent nuclear fuel. The first steps of this process extract the fission product technicium-99 ( 99 Tc) into an organic phase containing tributylphosphate together with uranium. Treatment of this stream requires the separation of Tc from U and placement into a suitable waste storage form. A potential candidate waste form involves immobilizing the Tc as an alloy with either excess metallic zirconium or stainless steel. Although Tc-Zr alloys seem to be promising waste forms, alternative materials must be investigated. Innovative studies related to the synthesis and behavior of a different class of Tc materials will increase the scientific knowledge related to development of Tc waste forms. These studies will also provide a better understanding of the behavior of 99 Tc in repository conditions. A literature survey has selected promising alternative waste forms for further study: technetium metallic alloys, nitrides, oxides, sulfides, and pertechnetate salts. The goals of this project are to 1) synthesize and structurally characterize relevant technetium materials that may be considered as waste forms, 2) investigate material behavior in solution under different conditions of temperature, electrochemical potential, and radiation, and 3) predict the long-term behavior of these materials.

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Modeling Interfacial Glass-Water Reactions: Recent Advances and Current Limitations

Describing the reactions that occur at the glass-water interface and control the development of the altered layer constitutes one of the main scientific challenges impeding existing models from providing accurate radionuclide release estimates. Radionuclide release estimates are a critical component of the safety basis for geologic repositories. The altered layer (i.e., amorphous hydrated surface layer and crystalline reaction products) represents a complex region, both physically and chemically, sandwiched between two distinct boundaries pristine glass surface at the inner most interface and aqueous solution at the outer most interface. Computational models, spanning different length and time-scales, are currently being developed to improve our understanding of this complex and dynamic process with the goal of accurately describing the pore-scale changes that occur as the system evolves. These modeling approaches include geochemical simulations [i.e., classical reaction path simulations and glass reactivity in allowance for alteration layer (GRAAL) simulations], Monte Carlo simulations, and Molecular Dynamics methods. Finally, in this manuscript, we discuss the advances and limitations of each modeling approach placed in the context of the glass-water reaction and how collectively these approaches provide insights into the mechanisms that control the formation and evolution of altered layers.

36 MATERIALS SCIENCE↗

Reconstruction of the Room D, B, G, and Q Closure Histories at the Waste Isolation Pilot Plant

Experimental measurements of room closure in salt repositories are valuable for understanding the evolution of the underground and for validating geomechanical models. Room closure was measured during a number of experiments at the Waste Isolation Pilot Plant (WIPP) during the 1980's and 1990's. Most rooms were excavated using a multi-pass mining sequence, where each pass necessarily destroyed some of the mining sequence closure measurement points. These destroyed points were promptly reinstalled to capture the closure after the mining pass. After the room was complete, the mining sequence closure measurement stations were supplemented with remotely read closure measurement stations. Although many aspects of these experiments were thoroughly documented, the digital copies of the closure data were inadvertently destroyed, the non-trivial process of zeroing and shifting the raw closure measurements after each mining pass was not precisely described, the various closure measurements within a given room were not directly compared on the same plot, and the measurements were collected for several years longer than previously reported. Consequently, the hand-written mining sequence closure measurements for Rooms D, B, G, and Q were located in the WIPP archives, digitized, and reanalyzed for this report. The process of reconstructing the mining sequence closure histories was documented in detail and the raw data can be found in the appendices. Within the mid-section of a given room, the reconstructed closure histories were largely consistent with other mining sequence and remotely read closure histories, which builds confidence in the experiments and suggests that plane strain is an appropriate modeling assumption. The reconstructed closure histories were also reasonably consistent with previously published results, except in one notable case: the reconstructed Room Q closure histories 30 days after excavation were about 45 % less than the corresponding closures reported in Munson's 1997 capstone paper.

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Implementation and verification of a user-defined element (UEL) for coupled thermal-hydraulic-mechanical-chemical (THMC) processes in saturated geological media

Efficient and accurate modeling of the coupled thermal-hydraulic-mechanical-chemical (THMC) processes in various rock formations is indispensable for designing energy geo-structures such as underground repositories for high-level nuclear wastes. Here, this work focuses on developing and verifying an implicit finite element solver for generic coupled THMC problems in geological settings. Starting from the mass, momentum, and energy balance laws, a specialized set of governing equations and a thermoporoelastic constitutive model is derived. This system is then solved by an implicit finite element (FE) scheme. Specifically, the residuals and the Jacobians are scripted in a user-defined element (UEL) subroutine which is then combined with the general-purpose FE software Abaqus Standard to solve initial-boundary value problems. Considering the complexity of the system, the UEL development follows a stepwise manner by first solving the coupled hydraulic-mechanical (HM) and thermal-hydraulic-mechanical (THM) equations before moving on to the full THMC problem. Each implementation step consists of at least one verification test by comparing computed results with closed-form analytical solutions to ensure that the various coupling effects are correctly realized. To demonstrate the robustness of the algorithm and to validate the UEL, a three-dimensional case study is performed with reference to the in-situ heating test of ATLAS at Belgium in 1980s. A hypothetical radionuclide leakage event is then simulated by activating the chemical-concentration degree of freedom and prescribing a constant high concentration at the heater's surface. The model predicts a limited contaminated regime after six years considering both diffusion and advection effects on species transport.

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Radioactive Waste Management in a Treatability and Optimisation Perspective - 17527

In order to meet recycling criteria or to fulfil Waste Acceptance Criteria (WAC) for disposal there are many different management concepts for radioactive waste that can be applied. Which concept or set of concepts to use to optimize waste management depends on several factors, among them, the regulatory framework for recycling, the availability of a disposal facility and the acceptance criteria for disposal. The required pre-treatment and other pre-disposal activities should be carefully analyzed for each of the disposal options, as they are significant contributors to the total cost for managing the waste. Waste Acceptance Criteria are living documents that should be updated when regulatory framework changes as well as when new treatment methods and new packaging and barrier systems develop. Each waste treatment facility, has its own specific limitations and therefore its own WAC/CFA (conditions for acceptance), which depends both on the plant design and national legislation. Many waste owners, countries or licensees, have their preferred, and in some cases well established, waste routes for certain waste streams. In some countries, the full chain from waste treatment through to disposal of radioactive waste is in place, whilst other countries still are in the process of establishing their repository program. The worst case scenario for any licensee or waste owner is waste which is not possible to qualify for disposal. This can be due to poor or degraded waste containers, unspecified content in waste packages, or wastes that are not suitable for disposal in their current form. Such deficiencies result in expensive actions related to waste retrieval, new characterisation and/or costly investigations. The EDF Group has a fleet of waste treatment facilities and has, for decades, provided waste treatment services to domestic and international customers. This paper will discuss important waste owner considerations and EDF experiences related to the optimization of the waste management process. This will be from both a treatment and an end-state perspective. (authors)

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National Plan for the Disposal of Existing and Future TRU Wastes - 18616

Now that the Waste Isolation Pilot Plant (WIPP) has re-opened, after being down for three years due to an accident the DOE National TRU Program has re-developed a plan for the disposal of existing and future TRU wastes. The National TRU Waste Management Plan (NTWMP) is an integrated plan to address the needs of DOE sites across the DOE Weapons Complex that create and store TRU waste, and is centered on the capability of WIPP to receive and dispose of TRU waste. The WIPP capability is planned as a weekly shipping rate and is defined by emplacement and receipt rate capabilities since WIPP is not permitted for long-term storage. And, shipping rates may be constrained by new WIPP Waste Acceptance Criteria (WAC) and future plans for repository configurations and disposal package capabilities over the next 30 years. Since WIPP is the only disposal system available to the DOE for TRU waste disposal, DOE has a newly projected life-cycle need for WIPP to remain open and available up to 2050. It is projected that the need for WIPP will continue up to the year 2050 for the disposition of the remaining legacy TRU inventories and for the disposal of TRU waste continuing to be generated at DOE's National Laboratories. In addition, there are several other potential new waste streams in which WIPP is being considered an alternative solution for their disposition. The NTWMP has been updated to reflect the short-term and long-term plans for TRU waste disposal at WIPP. The short-term plan is used by DOE for budget projection and integration purposes to facilitate and inform budget planning, both in DOE's Environmental Management (EM) and National Nuclear Security Administration (NNSA) organizations. Most legacy TRU waste (generated in the past and stored at DOE sites today) is owned and managed by EM. And, EM submits integrated budget requests for DOE sites, including the integration of resources for TRU waste management. NNSA and DOE's Office of Science (OS) funds TRU waste management as part of their mission funding and NNSA should eventually be the primary user of the WIPP resources as EM's legacy TRU waste is cleaned-up. Prior to the unexpected shutdown of WIPP in 2014, there was a small back-log of waste certified for WIPP disposal and shipments of TRU waste to WIPP were 'just-in-time' as waste was certified. After three years of WIPP being down, DOE sites have built significant back-logs of TRU waste to be certified for WIPP. That back-log built up to over 25,000 containers of TRU waste during that three-year period (Table 1). The backlog included both Contact-Handled (CH) TRU waste and Remote-Handled (RH) TRU waste, and even though WIPP re-opened in April of 2017, it is only open for TRU waste containers that can be stacked on disposal room floors. Plans for changing RH waste disposal packages and methods are in-the-works, but are not yet mature enough for significant planning. In addition, the WIPP underground facilities are now partially contaminated with radioactive particulate, which significantly reduces the WIPP operational efficiencies as compared to 2014. With a large back-log of waste ready for WIPP disposal and limited throughput for WIPP disposal rates, the focus of the NTWMP is to prioritize the selection of TRU wastes from the various sites based on WIPP waste emplacement rates and shipping rates to WIPP. Some TRU waste sites have a significant need to be top priority for shipments to WIPP, and that must be balanced with the need for all TRU waste sites to have some shipments to deplete their back-log of TRU wastes. Storage and management of TRU waste is very costly for DOE and many of those resources could be used to optimize the overall disposition of TRU waste and save DOE significant funding. In addition, the plan will show the possible transition of TRU Waste Management from primarily being an EM function to being an NNSA function in the coming years. As legacy TRU waste inventories are removed, and as NNSA mission-related TRU waste inventories are produced, DOE will be faced with deciding where the primary responsibility for TRU waste management should reside. (author)

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Investigations into the Gas Phase Reactions of Zirconium Tetrachloride (ZrCl) from UNF Cladding

Zirconium-based cladding materials that surround used nuclear fuel (UNF) rods represent a significant fraction of the total amount of high level waste that must be disposed of in long term geological repositories. The decontamination, recovery and reuse of these materials would significantly reduce the high level waste associated with light water reactors and could provide a new source of hafnium free zirconium for the fabrication of new nuclear components. A step in a strategy to recycle zirconium from used cladding materials is the high yield chlorination of Zircaloys to produce zirconium tetrachloride (ZrCl{sub 4}). The ZrCl, is contaminated with other metal chloride species that originate from the alloying metals as well as contaminants from oxide layers on the cladding, trace fission products, fuel residues, activation byproducts, and tritium. The properties of these complex mixtures must be better understood before purification protocols can be developed that will allow zirconium chloride to be recycled further. First order thermodynamic modeling of high temperature mixtures of ZrCl, and other metal chlorides in the gas phase may not accurately predict their properties. Computational modeling studies indicate that mixed metal adducts may form under the conditions of sublimation-based purification protocols. In light of these predictions, alternate strategies may also be needed to obtain pure ZrCl, from such mixtures. (authors)

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Computational Studies of Gas Phase Reactions of Zirconium Tetrachloride (ZrCl{sub 4}) and Metal Chloride Impurities

Zirconium-based cladding materials that surround used nuclear fuel (UNF) rods represent a significant fraction of the total amount of high level waste that must be disposed of in long term geological repositories. The decontamination, recovery and reuse of these materials would significantly reduce the high level waste associated with light water reactors and could provide a new source of hafnium free zirconium for the fabrication of new nuclear components. One part in the strategy to recycle zirconium from used cladding materials involves developing a computational modeling (DFT) protocol to understand the reactions between ZrCl{sub 4} and metal chloride impurities that may occur in the gas phase during sublimation. Several of the metal chloride species present are known to form Lewis acid/base adducts in the gas phase and development of purification protocols require investigation into the properties of these ZrCl{sub 4} contaminates.

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Corrosion of 316 SS in direct contact with Zircaloy-4 in repository relevant conditions

The effects of interfacial contact between 316 stainless steel (316 SS) waste canister and spent fuel cladding material (Zircaloy-4) in case of water intrusion into a deep geological repository are investigated. Hydrothermal corrosion experiments of 316 SS and Zircaloy-4 in direct contact were performed at elevated temperatures in MilliQ water and simulated Mont Terri groundwater. Hematite, magnetite, chromite, and baddeleyite form as secondary phases. pH of the Mont Terri solution increases with corrosion duration and magnetite forms preferentially instead of hematite. Thermodynamic modeling shows that iron oxidation in 316 SS controls the pH and redox potential of the aqueous environment and is in good agreement with experimental Mont Terri results, showing that experimental Mont Terri results trend to equilibrium. All oxides except hematite are predicted to exist at thermodynamic equilibrium based on calculations, implying that experimentally formed hematite will be reduced or transformed to magnetite at equilibrium. The thermodynamically predicted chromite was observed to form only at the interface where 316 SS was in contact with Zircaloy-4 at 250°C, showing that contact with Zircaloy-4 seems to accelerate the 316 SS corrosion to thermodynamic equilibrium. Finally, Mont Terri groundwater readily trends towards thermodynamic equilibrium, leading to a pH and redox buffered system that is dominated by iron in solution coming from the accelerated corrosion of 316 SS caused by Zircaloy-4 contact.

316 stainless steel↗

From Banned to Allowed: Pathway to Sub-seabed HLW Repositories - 16279

For many countries the disposal of high-level radioactive waste (HLW) has been delayed due to a number of factors including the Not-In-My-Backyard (NIMBY) syndrome. Sub-seabed disposal has no NIMBY concerns since the disposal facilities utilize sediments underlying approximately 4000 meters of international waters. The technical feasibility of the concept was demonstrated during a 12-year joint effort of over 200 researchers from 10 different countries. Social pressures to keep the oceans off-limits to most disposal activities resulted in termination of the coordinated international effort. However, the treaty banning the concept mandated a 25-year review frequency covering the latest scientific and technical information germane to the activity. An effort is underway to supply information to the signatories of the treaty, in their native languages, so they can make a fully-informed decision -- whether or not to approve an amendment that would allow sub-seabed disposal if determined to be protective of human health and the environment and permitted in accordance with guidelines provided by the International Atomic Energy Agency (IAEA). The information highlights the environmental and safety aspects of the disposal concept within a sensible global stewardship framework. With an amended treaty to allow sub-seabed HLW repositories, the global outlook for nuclear waste disposal would be altered dramatically: the number of potential disposal facilities scattered around the world could be reduced from over sixty land-based to approximately six (three land-based, three sub-seabed). (authors)

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Coupled hydro-thermal flow and radionuclide transport driven by spatial variation of heat-generating radioactive wastes in shale formations

Deep geologic disposal of multiple nuclear waste packages with various heat sources can induce nonuniform hydro-thermal behaviors in the near-field of the repository, consequently influencing the long-term radionuclide transport in the far-field once waste form breach initiates. Here, this study looks into three cases with variation in the spatial order of six groups of heat sources (10th, 50th, 75th, 90th, 95th, and 99th percentiles of heat outputs generated from 1,981 as-loaded dual-purpose canisters in the field site) in a shale-hosted repository with respect to the uni-directional groundwater flow (from west to east): (1) cooler waste packages from west to east, (2) hotter waste packages from west to east, and (3) hottest waste packages in the middle of the repository. Our field-scale PFLOTRAN simulation represents heat-driven multiphysics coupled mechanisms, including multiphase flow, heat transfer, and chemical/radioactive transport, and also, calculates the onset of waste form breach based on temperature-dependent canister vitality. The results from this sensitivity study will quantify the short- (less than 1 × 10 3 years) and long-term (up to 1 × 10 6 years) impacts of sporadic heat pulses from waste package on the spatio-temporal perturbation in hydro-thermal flow quantities and the rate of radionuclide transport in both near- and far-field of the repository system.

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Mixed-layered bismuth--oxygen--iodine materials for capture and waste disposal of radioactive iodine

Materials and methods of synthesizing mixed-layered bismuth oxy-iodine materials, which can be synthesized in the presence of aqueous radioactive iodine species found in caustic solutions (e.g. NaOH or KOH). This technology provides a one-step process for both iodine sequestration and storage from nuclear fuel cycles. It results in materials that will be durable for repository conditions much like those found in Waste Isolation Pilot Plant (WIPP) and estimated for Yucca Mountain (YMP). By controlled reactant concentrations, optimized compositions of these mixed-layered bismuth oxy-iodine inorganic materials are produced that have both a high iodine weight percentage and a low solubility in groundwater environments.

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Recent Advances in Corrosion Science Applicable To Disposal of High-Level Nuclear Waste

High level radioactive waste is accumulating at temporary storage locations around the world and will eventually be placed in deep geological repositories. Many different types of geological formation are under consideration, but all will eventually allow water to contact the metallic waste containers considering that the period of performance required to allow sufficient decay of dangerous radionuclides is on the order of 105 – 106 years. Corrosion of the containers and waste forms in the aqueous repository environment is therefore a concern. This review describes the recent advances of the field of materials corrosion based on the work of the Center for Performance and Design of Nuclear Waste Forms and Containers (WastePD) to address the issues associated with the long-term performance assessment and the design of materials with improved performance, where performance is defined as resistance to aqueous corrosion. Glass, crystalline ceramics, and metals are discussed separately, and then the near field interactions of these different materials classes are addressed. Recommendations for future directions are provided.

Frankel, Gerald↗

Development of PFLOTRAN Transport Capability for Use in the Waste Isolation Pilot Plant Performance Assessment - 20545

Waste Isolation Pilot Plant (WIPP) performance assessment (PA) calculations estimate the probability of radionuclide release from the repository to the land surface and across the land withdrawal boundary for a regulatory period of 10,000 years after facility closure. Simulations of flow and transport in the repository and the surrounding Salado Formation are foundational to the PA. Because proposed additional waste emplacement panels would result in an asymmetric repository layout, the US Department of Energy (DOE) is preparing to transition to use of a three-dimensional (3-D) model domain for simulation of flow and transport instead of the two-dimensional (2-D) flared grid domain currently used. DOE has charged Sandia National Laboratories with developing the capability necessary to simulate processes affecting flow and transport in the WIPP in PFLOTRAN, an open-source massively parallel multi-phase flow and reactive transport code. The new flow and transport capabilities developed in PFLOTRAN incorporate WIPP-specific process models and will replace the 2-D simulators (BRAGFLO and NUTS) that are currently utilized for Salado flow and transport calculations in WIPP PA. The focus of this paper is on the development of a new Nuclear Waste Transport (NWT) mode in PFLOTRAN that has all of the capabilities necessary for Salado transport simulations, including the ability to handle complete dry-out (100% gas saturation) of arbitrary cells in the model domain, radionuclide mass conservation at step changes in porosity associated with borehole intrusion, and the ability to calculate fluxes on a flared grid. The new PFLOTRAN transport capability and a suite of verification tests were designed around a list of functional requirements for WIPP PA calculations. (authors)

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Salt Reconsolidation and Repository Engineered Barriers - 18651

Salt repositories for the permanent disposal of hazardous waste provide extraordinary advantage over other geo-media because geotechnical barriers can be constructed with confidence using crushed salt, which is a perfectly compatible material that is readily available by mining practice. Other excellent barrier materials that consist of specialty mixes of salt-based concrete, bentonite, and bitumen bolster confidence that a repository in geologic salt formations will remain impermeable forever. Practically speaking, achieving high-performance engineered barriers assumes an isolation role as important as the host formation itself. Long-term performance assessment intrinsically includes evaluating seal-system design and demonstrated operational characteristics. Consistent with global interests, specific research on salt-repository seal systems not only established significant technical bases but identified possible improvements through straightforward research and laboratory and field investigations. Engineered barriers of crushed salt with possible additives, such as clay and water, evolve to create hydrological and mechanical characteristics that approach those of the host salt formation. Demonstrating early functionality of seal systems reduces uncertainty, which is introduced when calculating or predicting when performance properties become effective in the future. (authors)

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Environmental Assessment for the Above Ground Storage Capability at the Waste Isolation Pilot Plant Draft

The Waste Isolation Pilot Plant (WIPP) is the nation’s only approved repository for the disposal of defense related/defense generated transuranic (TRU) and mixed hazardous TRU waste (henceforth called TRU waste). The mission of the WIPP Project is to realize the safe disposal of TRU waste from TRU waste generator sites in the Department of Energy waste complex. The WIPP Project was authorized by Title II, Section 213(a) of Public Law 96-164 (U. S. Congress 1979). Congress designated the WIPP facility “for the express purpose of providing a research and development facility to demonstrate the safe disposal of radioactive wastes resulting from the defense activities and programs of the United States exempted from regulation by the Nuclear Regulatory Commission (NRC).” The WIPP facility is operated by the U. S. Department of Energy (DOE). Transuranic waste that is disposed in the WIPP facility is defined by Section 2(18) the WIPP Land Withdrawal Act of 1992 (LWA) (U. S. Congress, 1992) as: “waste containing more than 100 nanocuries of alpha-emitting transuranic isotopes per gram of waste, with half-lives greater than 20 years, except for: (A) high-level radioactive waste; (B) waste that the Secretary has determined, with the concurrence of the Administrator, does not need the degree of isolation required by the disposal regulations; or (C) waste that the NRC has approved for disposal on a case-by-case basis in accordance with part 61 of title 10, Code of Federal Regulations (CFR).

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Self-accelerated corrosion of nuclear waste forms at material interfaces

The US plan for high-level nuclear waste includes the immobilization of long-lived radionuclides in glass or ceramic waste forms in stainless-steel canisters for disposal in deep geological repositories. Here we report that, under simulated repository conditions, corrosion could be significantly accelerated at the interfaces of different barrier materials, which has not been considered in the current safety and performance assessment models. Severe localized corrosion was found at the interfaces between stainless steel and a model nuclear waste glass and between stainless steel and a ceramic waste form. The accelerated corrosion can be attributed to changes of solution chemistry and local acidity/alkalinity within a confined space, which significantly alter the corrosion of both the waste-form materials and the metallic canisters. The corrosion that is accelerated by the interface interaction between dissimilar materials could profoundly impact the service life of the nuclear waste packages, which, therefore, should be carefully considered when evaluating the performance of waste forms and their packages. Moreover, compatible barriers should be selected to further optimize the performance of the geological repository system.

Guo, Xiaolei↗