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DOE OSTI2016

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)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2017

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

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

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↗

DOE OSTI2016

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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DOE OSTI2024

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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DOE OSTI2015

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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DOE OSTI2021

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↗

DOE OSTI2020

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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DOE OSTI2018

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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DOE OSTI2017

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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DOE OSTI2020

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↗

DOE OSTI2015

Uniaxial Creep as a Control on Mercury Intrusion Capillary Pressure in Consolidating Rock Salt

The nature of geologic disposal of nuclear waste in salt formations requires validated and verified two-phase flow models of transport of brine and gas through intact, damaged, and consolidating crushed salt. Such models exist in other realms of subsurface engineering for other lithologic classes (oil and gas, carbon sequestration etc. for clastics and carbonates) but have never been experimentally validated and parameterized for salt repository scenarios or performance assessment. Models for waste release scenarios in salt back-fill require phenomenological expressions for capillary pressure and relative permeability that are expected to change with degree of consolidation, and require experimental measurement to parameterize and validate. This report describes a preliminary assessment of the influence of consolidation (i.e. volume strain or porosity) on capillary entry pressure in two phase systems using mercury injection capillary pressure (MICP). This is to both determine the potential usefulness of the mercury intrusion porosimetry method, but also to enable a better experimental design for these tests. Salt consolidation experiments are performed using novel titanium oedometers, or uniaxial compression cells often used in soil mechanics, using sieved run-of-mine salt from the Waste Isolation Pilot Plant (WIPP) as starting material. Twelve tests are performed with various starting amounts of brine pore saturation, with axial stresses up to 6.2 MPa (~900 psi) and temperatures to 90°C. This corresponds to UFD Work Package 15SN08180211 milestone “FY:15 Transport Properties of Run-of-Mine Salt Backfill – Unconsolidated to Consolidated”. Samples exposed to uniaxial compression undergo time-dependent consolidation, or creep, to various degrees. Creep volume strain-time relations obey simple log-time behavior through the range of porosities (~50 to 2% as measured); creep strain rate increases with temperature and applied stress as expected. Mercury porosimetry is used to determine characteristic capillary pressure curves from a series of consolidation tests and show characteristic saturation-capillary pressure curves that follow the common van Genuchten (1978, 1980) formulation at low stresses. Higher capillary pressure data are suspect due to the large potential for sample damage, including fluid inclusion decrepitation and pore collapse. Data are supportive of use of the Leverett “J” function (Leverett, 1941) to use for scaling characteristic curves at different degrees of consolidation, but better permeability determinations are needed to support this hypothesis. Recommendations for further and refined testing are made with the goal of developing a self- consistent set of constitutive laws for granular salt consolidation and multiphase (brine-air) flow.

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DOE OSTI2024

RANGERS: Modeling Report on Integrity and Performance Assessment of Engineered Barrier Systems in a Salt Repository for HLW/SNF

The Engineered Barrier System (EBS) plays an important role in ensuring the long-term safety and containment of high-level waste (HLW) and spent nuclear fuel (SNF) in deep geological repositories in salt formation. As part of a multi-barrier system, the EBS works alongside the natural barrier, which is the salt formation itself and the technical barrier comprising the disposal casks. The primary function of the EBS is to maintain containment during a defined period until the backfill used in the repository made of crushed salt, develops its sealing capacity through compaction. Over the time, the backfill eventually compacts to a state of low porosity and permeability, acting as a long-term seal. However, until this process is complete, the EBS must retain its structural and functional integrity. Regulatory guidelines in Germany currently require the EBS to remain effective for up to next ice age, that is expected in 50,000 years. The significant hydro-geological and topographic changes expected during an ice age could make it impossible to accurately predict the hydro-chemical conditions within the repository system at that time. In response to these challenges, BGE TECHNOLOGY GmbH (BGE TEC) and Sandia National Laboratories (SNL) have jointly developed a comprehensive methodology for the design and safety assessment of engineered barrier systems within the scope of the RANGERS project. This methodology is tailored for repositories in salt formations. The developed methodology provides a structured approach for designing and assessing the performance of the EBS in salt-based repositories. It begins with defining a sealing concept based on the geological characteristics of the selected site and the overall repository design. The entire repository system, comprising the geological site, repository infrastructure, and EBS, is then subjected to a Features, Events, and Processes (FEP) analysis, focusing solely on those FEPs that affect the EBS. The derived FEPs help identify the loads and stresses acting on the EBS, which serve as the foundation for conducting an integrity assessment. This analysis helps predict the EBS’s evolution and performance over the regulatory time frame, feeding into integrated performance assessment simulations.

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DOE OSTI2021

International collaboration in disposal research: comparative modeling of coupled processes in the DECOVALEX project

Abstract. This presentation gives an overview of an international research collaboration for advancing the understanding and modeling of coupled thermo-hydro-mechanical-chemical (THMC) processes in geological systems. The creation of the international DECOVALEX project, now running for more than 25 years, was motivated by the recognition that prediction of these coupled effects is an essential part of the performance and safety assessment of geologic disposal systems for radioactive waste and spent nuclear fuel. DECOVALEX emphasizes joint analysis and comparative modeling of state-of-the-art field and laboratory experiments, across a range of host rock options and repository designs. Participating research teams are from radioactive waste management organizations, national research institutes, regulatory agencies, universities, and consulting groups, providing a wide range of perspectives and solutions to these complex problems. The presentation provides examples of the research contributions made collectively in past DECOVALEX tasks and also touches on the unique modeling challenges tackled in the ongoing project phase, referred to as DECOVALEX-2023. The current phase comprises 17 partner organizations, about 50 modeling teams, and 7 modeling tasks, which cover a broad portfolio from fundamental studies on gas migration to full-scale in situ heater experiments in different host rocks to performance assessment studies. Together, these examples illustrate that the insight and scientific knowledge gained within the DECOVALEX project would not have been possible if one group had studied these complex THMC modeling challenges alone rather than within a truly collaborative setting.

Birkholzer, Jens T.↗

DOE OSTI2018

Assessment of the potential for criticality in the far field of a used nuclear fuel repository

This study aims to assess the likelihood for criticality in the far field of a repository for direct disposal of commercial light water reactor used nuclear fuel. Two models are used in combination: (1) a neutronics model to estimate the minimum critical masses of spherical, water-saturated depositions of fissile material; (2) a transport model to simulate the dissolution of waste packages arranged in an array and the subsequent transport of fissile solutes through fractured bedrock to a single accumulation location. The neutronics model shows that heavy metals from different types of used fuel present the same minimum critical mass behavior in the parameter space of initial enrichment and burnup, dictated largely by the fissile content. However, the magnitude of the minimum critical mass varies significantly within that parameter space, and secondary effects like the presence of absorbing nuclides play a minor role. Here, the transport model employs various subsurface transport scenarios, and for each scenario the mass of each isotope and the overall fissile content of the accumulation is reported from the time of canister failure up to one hundred million years at various distances from the repository edge. Taking the results of the two models in concert, it is shown that even if the accumulation of a critical mass is possible under conservative conditions, these conditions are unlikely to be present in the vicinity of a carefully engineered repository. Based on the results of each model, recommendations for risk mitigation in terms of waste characteristics and repository design are given.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

Analysis of the Effects of Postclosure Criticality on Repository Performance

The United States Department of Energy’s (DOE) Office of Nuclear Energy’s Disposal Research & Development Campaign seeks to better understand the technical basis, risks, and uncertainty associated with the safe and secure disposition of spent nuclear fuel (SNF) and high-level radioactive waste (HLW). Commercial nuclear power generation in the United States has resulted in thousands of metric tons of SNF, the disposal of which is the responsibility of DOE (Nuclear Waste Policy Act of 1982, as amended). Any repository licensed to dispose of SNF will be subject to requirements regarding the long-term performance of that repository. Evaluating the long-term performance of the repository may consider the consequences of the SNF achieving a critical configuration during the postclosure period. Of particular interest is the potential for this to occur in dual-purpose canisters (DPCs), which are currently licensed and being used to store and transport SNF but were not designed for permanent geologic disposal. DOE has been considering disposing of SNF in DPCs to avoid the costs and worker dose associated with repackaging the SNF currently stored in DPCs into repository-specific canisters. This report examines the consequences of postclosure criticality to provide technical support to DOE in developing a disposal plan.

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DOE OSTI2017

Purification of Zirconium Tetrachloride (ZrCl{sub 4}) from UNF Cladding - A Progress Report

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 and/or recovery and reuse of these materials would significantly reduce the amount of high level waste associated with light water nuclear energy 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 direct, high yield chlorination reaction that produces zirconium tetrachloride (ZrCl{sub 4}). The ZrCl{sub 4} so obtained is contaminated with other metal chloride species (FeCl{sub 3}, NbCl{sub 5}, NbOCl{sub 3}, SnCl{sub 4}, CsCl, SbCl{sub 5}, etc.) that originate from the alloying metals present initially as well as contaminants from oxide layers on the cladding, trace fission products, fuel residues, activation byproducts, and tritium. The suggested strategy to remove the metal chloride impurities is based on sublimation at atmospheric pressure combined with chemical treatments influencing volatility of the impurities.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2018

Reporting the Radionuclide Inventory of the DWPF Product

In the Defense Waste Processing Facility (DWPF) at the Savannah River Site (SRS), the radionuclides contained in the liquid high-level waste currently stored at SRS are being converted into a durable borosilicate glass. This glass in its sealed stainless-steel canister, the DWPF product, eventually must be sent to a federal repository for final disposal. In order to ensure that the DWPF product is suitable for acceptance by the U. S. Department of Energy’s (DOE) Civilian Radioactive Waste Management System (CRWMS)*, the DOE Office of Environmental Management (DOE-EM) established the Waste Acceptance Product Specifications for Vitrified High-Level Waste Forms (WAPS). DOE-EM is tentatively performing surrogate CRWMS waste acceptance functions, as the office was eliminated in 2009, for review and concurrence of technical baseline documents and waste form non conformances. The specifications are divided into five sections, dealing with the waste form (borosilicate glass) itself, the canister, the canistered waste form, quality assurance, and documentation and other administrative requirements. The DWPF is required to document its compliance with the specifications in the Waste Form Compliance Plan (WCP), the Waste Form Qualification Report (WQR), the Production Records, and the Storage and Shipping Records. The WCP provides general information about the DWPF process and product, and a general description of the methods and programs by which the DWPF will demonstrate compliance with each specification in the WAPS. The WCP was vital to DWPF startup with respect to operations planning and also assurance to DOE that the canistered waste forms would be acceptable for disposal at any future High-Level Waste (HLW) geologic repository. The WQR is a compilation of the results of the testing and analysis programs identified in the WCP. The WQR details the method of compliance with each specification, and the testing performed to demonstrate the effectiveness of each method. The WQR is published in separate volumes which each correspond to one or more of the specifications. The WQR also contains a description of the DWPF’s Glass Product Control Program. Each volume contains Part and Item designators which indicate the corresponding item(s) in the WCP. The Production Records, and the Storage and Shipping Records document that each DWPF product has been produced and stored in compliance with the WAPS. This document, Volume 4 of the WQR, responds to WAPS Specifications 1.2.2, 1.6, and 3.14 which require that the DWPF report the radionuclide inventory of each canistered waste form, and of each waste type. This volume describes the systems the DWPF uses to determine and report the radionuclide inventory of the glass product, and provides evidence that these systems allow the DWPF to satisfy the WAPS specification. This volume of the WQR has been prepared to establish that methods are available to determine and report the radionuclide inventory, and that the DWPF is ready to collect the facility-specific data necessary to provide definitive estimates of the errors associated with the use of these methods.

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