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At least 379 records · Page 21

Neutron Measurements from Boron Carbide Addition to a Plutonium Waste Form

The Department of Energy (DOE) has identified the Dilute and Dispose approach as the preferred method for the disposition of surplus plutonium materials. Dilute and Dispose requires surplus plutonium to be converted to an oxide product and then dry blended with a multi-component adulterant mixture to reduce the Safeguards and Security attractiveness level of the materials. The resulting product will be discarded in a geologic repository at the Waste Isolation Pilot Plant (WIPP).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Value of abstraction in performance assessment – When is a higher level of detail necessary?

In this study, different approaches in performance assessment (PA) of the long-term safety of a repository for radioactive waste were examined. This investigation was carried out as part of the DECOVALEX-2023 project, an international collaborative effort for research and model comparison. One specific task of the DECOVALEX-2023 project was the Salt Performance Assessment Modelling task (Salt PA), which aimed at comparing various models and methods employed in the performance assessment of deep geological repositories in salt. In the context of the Salt PA task, three distinct teams from SNL (United States), Quintessa Ltd (United Kingdom), and GRS (Germany) examined the consequences of employing different levels of abstractions when modelling the repository's geometry and implementing various features and processes, using the example of a simple hypothetical repository structure in domal salt. Each team applied their own tools: PFLOTRAN (SNL), QPAC (Quintessa) and LOPOS (GRS). These differ essentially regarding numerical concept and degree of detail in the representation of the underlying physical processes. The discussion focused on when simplifications can be appropriately applied and what consequences result from them. Furthermore, it was explored when and if a higher level of fidelity in geometry or physical processes is required.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Future Transition of WIPP from EM to Another DOE Office - 19256

The U. S. Department of Energy (DOE) Carlsbad Field Office (CBFO) has a primary mission to assist federal government entities disposition transuranic (TRU) radioactive waste. The main resource for disposition is the deep geologic repository known as the Waste Isolation Pilot Plant (WIPP). Other resources include a complete transportation system and a program that assists in the certification and shipment of TRU waste to WIPP known as the National TRU Program (NTP). All of these resources are managed by CBFO, which currently is part of the DOE Environmental Management (EM) program. EM's primary mission for DOE is to clean up the legacy remaining from many years of nuclear weapons research and production. But, CBFO estimates the need for WIPP and NTP will continue beyond the mission of EM and will assist other entities such as the National Nuclear Security Administration (NNSA), the Office of Science (OS) and the Navy. As the inventory of legacy TRU waste is reduced, the inventory of new TRU waste will continue from ongoing missions. So, over the life span of WIPP the primary customers of CBFO will shift from legacy EM sites to newly-generated TRU waste sites. And, somewhere along the way CBFO estimates that it will transition, primarily from an EM support (legacy waste) entity to a primarily a NNSA support (newly-generated waste) entity to facilitate ongoing DOE missions. This paper will address the need for that change at a programmatic level and will include some ideas for conceptual planning for such a transition. (author)

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Status of Progress Made Toward Safety Analysis and Technical Site Evaluations for DOE Managed HLW and SNF.

The Spent Fuel and Waste Science and Technology (SFWST) Campaign of the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE) is conducting research and development (R&D) on generic deep geologic disposal systems (i.e., repositories). This report describes specific activities in FY 2016 associated with the development of a Defense Waste Repository (DWR)a for the permanent disposal of a portion of the HLW and SNF derived from national defense and research and development (R&D) activities of the DOE.

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DECOVALEX-2019 (Task G Final Report)

The DECOVALEX Project is an on-going international research collaboration, established in 1992, to advance the understanding and modeling of coupled Thermal (T), Hydrological (H), Mechanical (M) and Chemical (C) processes in geological in geological systems. This document is the final report of Task G which was proposed by the Swedish Radiation Safety Authority (SSM) and coordinated by geomecon GmbH, presenting the technical definitions of the problems studied, approaches applied, achievements made and outstanding issues for future research. Task G in DECOVALEX-2019 is primarily concerned with the evolution of transmissivity throughout the lifetime of a repository for radioactive waste, and in particular of spent nuclear fuel, in sparsely fractured and competent crystalline rock masses, and the representation of these processes via numerical simulation. The numerical simulations were to be evaluated for their suitability, and to be validated. Over the course of the work presented here, not only were transmissivity changes and the best approaches to simulate those change examined, but also strategies were to be developed on how to monitor transmissivity change. Guidelines on what a control program and a monitoring system for a repository should include and be able to measure, and how this can be done in practice, was a key objective of the research project.

58 GEOSCIENCES↗

Why Cleanup Acceptance Is Running into Conflicts - Off-site Disposal Versus On Site Disposal - 19068

For years the U.S. Department of Energy (DOE) identified several sites to receive shipments of various types of wastes. However, with the backlog at the Waste Isolation Pilot Plant (WIPP), the inability to license Yucca Mountain, and the agency's desire to expedite cleanup, DOE is trying to 'dispose of' or 'store' more waste belonging to the Federal government on-site. Some states and communities that were 'promised' disposal of DoE's waste in geologic repositories and licensed landfills in arid locations, are now being told that on-site disposal is the best path forward. Competition for resources is forcing more sites to focus on near term cost savings of on-site disposal, rather than develop comprehensive life-cycle estimates representing a more realistic picture of costs associated with isolating radioactive and other hazardous materials on-site in perpetuity. The paper explores the issues and possible solutions in a case study on proposed on-site disposal of DOE waste, and concludes that DOE needs community support and community acceptance to successfully implement the agency's cleanup mission. Ongoing dialogue with the community saves both time and money but more importantly, cooperation helps ensure that effective long-term cleanup occurs. (author)

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French Innovative Processes in the Field of Thermal Treatment For Decommissioning and Legacy Waste - 18085

In order to optimize decommissioning waste management and better anticipate related issues, French nuclear waste producers CEA and AREVA, and the French Agency in charge of radioactive waste disposal (ANDRA) have decided to collectively develop technologies mastering costs, schedules and dose uptake as well as optimizing waste volumes and repository safety. In this context, several innovative projects have emerged over the past few years to develop specific thermal treatment processes. This paper focus on four new processes, presenting their goals, technical descriptions and first experimental results. (authors)

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Options assessment report: Treatment of nitrate salt waste at Los Alamos National Laboratory

This report documents the methodology used to select a method of treatment for the remediated nitrate salt (RNS) and unremediated nitrate salt (UNS) waste containers at Los Alamos National Laboratory (LANL). The method selected should treat the containerized waste in a manner that renders the waste safe and suitable for transport and final disposal in the Waste Isolation Pilot Plant (WIPP) repository, under specifications listed in the WIPP Waste Acceptance Criteria (DOE/CBFO, 2013). LANL recognized that the results must be thoroughly vetted with the New Mexico Environment Department (NMED) and the a modification to the LANL Hazardous Waste Facility Permit is a necessary step before implementation of this or any treatment option. Likewise, facility readiness and safety basis approvals must be received from the Department of Energy (DOE). This report presents LANL's preferred option, and the documentation of the process for reaching the recommended treatment option for RNS and UNS waste, and is presented for consideration by NMED and DOE.

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Options Assessment Report: Treatment of Nitrate Salt Waste at Los Alamos National Laboratory

This report documents the methodology used to select a method of treatment for the remediated nitrate salt (RNS) and unremediated nitrate salt (UNS) waste containers at Los Alamos National Laboratory (LANL). The method selected should treat the containerized waste in a manner that renders the waste safe and suitable for transport and final disposal in the Waste Isolation Pilot Plant (WIPP) repository, under specifications listed in the WIPP Waste Acceptance Criteria (DOE/CBFO, 2013). LANL recognizes that the results must be thoroughly vetted with the New Mexico Environment Department (NMED) and that a modification to the LANL Hazardous Waste Facility Permit is a necessary step before implementation of this or any treatment option. Likewise, facility readiness and safety basis approvals must be received from the Department of Energy (DOE). This report presents LANL’s preferred option, and the documentation of the process for reaching the recommended treatment option for RNS and UNS waste, and is presented for consideration by NMED and DOE.

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Electrochemical corrosion under controlled redox conditions

A method for predicting corrosion rates of a material during service conditions is provided, the method having the steps of determining a first phase composition of the material; exposing the material to service conditions chemical environment; applying an electrical potential to the exposed material to represent the solution redox; identifying ranges of the applied potential that correspond to different corrosion behaviors of the material; quantifying current and surface electrical properties during corrosion; and determining a second phase composition of the material to identify corroded phases. Also provided is a method for determining radionuclide source terms, the method having the steps of supplying a multiphase metallic waste containing the radionuclides; immersing the waste in a solution representing repository chemistry conditions; and oxidizing the immersed waste for a period of time and at particular imposed voltages representing solution redox values to establish a steady current representing corrosion rate of the waste.

Gattu, Vineeth Kumar↗

Effect of Low-Temperature Sensitization on the Corrosion Behavior of AISI Type 304L SS Weld Metal in Simulated Groundwater

The manuscript presents the investigations carried out on the effect of low-temperature sensitization (LTS) of 304L SS weld metal on its corrosion behavior in simulated groundwater, for its application as a canister material for long-term storage of nuclear vitrified high-level waste in geological repositories. AISI type 304L SS weld pad was fabricated by multipass gas tungsten arc welding process using 308L SS filler wire. The as-welded specimens were subsequently subjected to carbide nucleation and further to LTS at 500 °C for 11 days to simulate a temperature of 300 °C for 100-year life of the canister in geological repositories. Delta ferrite (δ-ferrite) content of the 304L SS weld metal substantially decreased on carbide nucleation treatment and further only a marginal decrease occurred on LTS treatment. The microstructure of the as-welded consisted of δ-ferrite as a minor phase distributed in austenite matrix. The δ-ferrite appeared fragmented in the carbide-nucleated and LTS-treated weld metal. The degree of sensitization measured by double-loop electrochemical potentokinetic reactivation method indicated an increase in carbide nucleation treatment when compared to the as-welded specimens, and further increase occurred on LTS treatment. Potentiodynamic anodic polarization investigations in simulated groundwater indicated a substantial decrease in the localized corrosion resistance of the carbide-nucleated and LTS 304L SS weld metals, when compared to the as-welded specimens. Post-experimental micrographs indicated pitting as the primary mode of attack in the as-welded, while pitting and intergranular corrosion (IGC) occurred in the carbide-nucleated weld metal. LTS-treated weld metal predominantly underwent IGC attack. The decrease in the localized corrosion resistance of the weld metal after LTS treatment was found to have a direct correlation with the degree of sensitization and the weld microstructure. The results are detailed in the manuscript.

36 MATERIALS SCIENCE↗

ORIGEN-based Nuclear Fuel Inventory Module for Fuel Cycle Assessment: Final Project Report

The goal of this project, “ORIGEN-based Nuclear Fuel Depletion Module for Fuel Cycle Assessment" is to create a physics-based reactor depletion and decay module for the Cyclus nuclear fuel cycle simulator in order to assess nuclear fuel inventories over a broad space of reactor operating conditions. The overall goal of this approach is to facilitate evaluations of nuclear fuel inventories for a broad space of scenarios, including extended used nuclear fuel storage and cascading impacts on fuel cycle options such as actinide recovery in used nuclear fuel, particularly for multiple recycle scenarios. The advantages of a physics-based approach (compared to a recipe-based approach which has been typically employed for fuel cycle simulators) is in its inherent flexibility; such an approach can more readily accommodate the broad space of potential isotopic vectors that may be encountered under advanced fuel cycle options. In order to develop this flexible reactor analysis capability, we are leveraging the Origen nuclear fuel depletion and decay module from SCALE to produce a standalone “depletion engine” which will serve as the kernel of a Cyclus-based reactor analysis module. The ORIGEN depletion module is a rigorously benchmarked and extensively validated tool for nuclear fuel analysis and thus its incorporation into the Cyclus framework can bring these capabilities to bear on the problem of evaluating long-term impacts of fuel cycle option choices on relevant metrics of interest, including materials inventories and availability (for multiple recycle scenarios), long-term waste management and repository impacts, etc. Developing this Origen-based analysis capability for Cyclus requires the refinement of the Origen analysis sequence to the point where it can reasonably be compiled as a standalone sequence outside of SCALE; i.e., wherein all of the computational aspects of Origen (including reactor cross-section library processing and interpolation, input and output processing, and depletion/decay solvers) can be self-contained into a single executable sequence. Further, to embed this capability into other software environments (such as the Cyclus fuel cycle simulator) requires that Origen’s capabilities be encapsulated into a portable, self-contained library which other codes can then call directly through function calls, thereby directly accessing the solver and data processing capabilities of Origen. Additional components relevant to this work include modernization of the reactor data libraries used by Origen for conducting nuclear fuel depletion calculations. This work has included the development of new fuel assembly lattices not previously available (such as for CANDU heavy-water reactor assemblies) as well as validation of updated lattices for light-water reactors updated to employ modern nuclear data evaluations. The CyBORG reactor analysis module as-developed under this workscope is fully capable of dynamic calculation of depleted fuel compositions from all commercial U.S. reactor assembly types as well as a number of international fuel types, including MOX, VVER, MAGNOX, and PHWR CANDU fuel assemblies. In addition, the Origen-based depletion engine allows for CyBORG to evaluate novel fuel assembly and reactor design types via creation of Origen reactor data libraries via SCALE. The establishment of this new modeling capability affords fuel cycle modelers a substantially improved ability to model dynamically-changing fuel cycle and reactor conditions, including recycled fuel compositions from fuel cycle scenarios involving material recycle into thermal-spectrum systems.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Developments in the Regulatory Framework of Nuclear Waste Management in Germany - Licensing Procedures for storage of SNF and Public Involvement - 19612

According to article 6 of the German Atomic Energy Act (AtG), storage of Spent Nuclear Fuel requires a license. The competent licensing authority in this field is the Federal Office for Safety of Nuclear Waste Management (BfE). According to the Act for selecting a repository site for heat-generating radioactive waste (HAW) (Site Selection Act - StandAG) dating from 2017, BfE has been assigned the task of developing, conducting, and evaluating public participation procedures in the process of site search and selection for a deep geological repository for radioactive waste and SNF. Article 6 AtG applies to interim storage of SNF. If the legally defined licensing conditions by article 6 (2) AtG are met, the storage license applied for has to be granted. For on-site facilities, interim storage has been limited to 40 years. The licensing procedures for interim storage of SNF are carried out in accordance with the general administrative procedural rules. In certain cases due to the Environmental Impact Assessment Act (EIA Act), an EIA has to be carried out. In these cases, a formalized licensing procedure including an involvement of the public is conducted. The Nuclear Licensing Procedure Ordinance (AtVfV) originating from 1977 and reformulated in 1995 defines formalized rules for the public participation procedure which have to be followed strictly. These include a public hearing. The risen objections are evaluated by the licensing authority and taken account of in the licensing decision. The process of repository site selection defined by the StandAG exceeds these formalized procedures significantly: The objective of this process is to achieve a broad social consensus about the site selection procedure and about a repository site that will offer the best possible safety for one million years. Therefore, the process has to be particularly transparent, and involvement of the public - including newly developed forms of public involvement - is an essential part of it. BfE as competent authority in both the fields of repository site search and selection and licensing of interim storage of SNF has recently developed new strategies of involving the public concerning interim storage of SNF. Supplementing the standard licensing procedures, BfE presently informs and involves the public about topical issues regarding the present state and recent developments in the field of interim storage of SNF. Current central topics are for example the return of HAW and MAW from reprocessing of SNF in France and UK as well as perspective longer interim storage periods on the interface with final disposal. Regarding longer interim storage, host communities of interim storage facilities are concerned that interim storage might be extended indefinitely. Additionally, there is a strong fear of transports of radioactive waste and SNF from one place to another. (authors)

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Evaluation of f -element borate chemistry

The synthesis, structure elucidation, and spectroscopic measurements of a myriad of new, f-element borates has revealed the unusual effects that this electron-rich oxoanion has on the electronic properties of lanthanides and actinides. One purpose of these studies was to provide models for actinide compounds that may exist in either vitrified nuclear waste or in repositories located within salt deposits that have significant borate content. In addition, the radiation-damage resilience of polyborate networks positions these materials as suitable candidates for probing coordination chemistry and physical properties much deeper into the actinide series than is normally possible, and compounds with actinides up to californium (Z = 98) have been successfully prepared and characterized in exquisite detail. Structural determination of these materials show that both the lanthanide and actinide series display previously unknown coordination chemistry, but, more importantly, that the two series have little overlap in terms of structure and composition, and have few parallels. In addition, some of these compounds display unique physico-chemical properties, one example of which is the selective trapping of radionuclides. The foremost discovery first identified in actinide borates is that the chemistry of californium represents an onset of unprecedented chemical behavior that compares better with high-oxidation state, early transition metal complexes than it does with earlier f-elements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Solubility of U(VI) in chloride solutions. III. The stable oxides/hydroxides in MgCl 2 systems: Pitzer activity model for the system UO 2 2+ –Na + –K + –Mg 2+ –H + –OH – –Cl – –H 2 O(l)

Here we have developed new chemical, thermodynamic and activity models for the system UO 2 2+ –Na + –K + –Mg 2+ –H + –OH – –Cl – –H 2 O(l) within the Pitzer approach. The new thermodynamic model is based on previously reported data treated within the SIT approach for NaCl and KCl systems, as well as on new experimental data determined in this work for the MgCl 2 system. The solubility of uranium(VI) was studied in 0.01–5.15 mol·kg w –1 MgCl 2 solutions at pH m = 4.1–9.7 (with pH m = –log [H + ]). Experiments were performed under Ar atmosphere at T = (22 ± 2) °C. In all investigated systems, the solubility of U(VI) is controlled by metaschoepite, UO 3 ·2H 2 O(cr). In contrast to previously investigated NaCl and KCl systems, no ternary Mg–U(VI)–OH(s) solid phases formed in alkaline MgCl 2 solutions within the timeframe of this study (≤ 200 days). A very significant increase in the solubility (up to 3 log 10 -units) is observed in acidic to near-neutral pH m conditions when increasing MgCl 2 concentration from 0.01 to 5.15 mol·kg w –1 , which reflects the strong ion interaction processes taking place in concentrated MgCl 2 brines. The solubility of UO 3 ·2H 2 O(cr) in the investigated NaCl, KCl and MgCl 2 solutions is well described with the solubility and hydrolysis constants recommended by Altmaier et al., (2017) and NEA–TDB, and a Pitzer activity model derived in the present work. The latter model considers experimental data reported in the present study and available in the literature for NaCl, KCl and MgCl 2 systems (solubility, potentiometric and spectroscopic data), in combination with well-stablished estimation methods and correlations with SIT coefficients. Finally, chemical, thermodynamic and Pitzer activity models provided in this work for the system UO 2 2+ –Na + –K + –Mg 2+ –H + –OH – –Cl – –H 2 O(l) accurately describe all evaluated datasets, and represent an adequate tool for the calculation of U(VI) solubility and aqueous speciation in a variety of geochemical conditions including concentrated brine systems of relevance in salt-based repositories for nuclear waste disposal.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Plutonium reactive transport in fractured granite: Multi-species experiments and simulations

Plutonium (Pu) in the subsurface environment can transport in different oxidation states as an aqueous solute or as colloidal particles. The transport behavior of Pu is affected by the relative abundances of these species and can be difficult to predict when they simultaneously exist. This study investigates the concurrent transport of Pu intrinsic colloids, Pu(IV) (aq) and Pu(V-VI) (aq) through a combination of controlled experiments and semi-analytical dual-porosity transport modeling. Pu transport experiments were conducted in a fractured granite at high and low flow rates to elucidate sorption processes and their scaling behavior. In the experiments, Pu(IV) (aq) was the least mobile of the Pu species, Pu(V-VI) (aq) had intermediate mobility, and the colloidal Pu, which consisted mainly of precipitated and/or hydrolyzed Pu(IV), was the most mobile. The semi-analytical modeling revealed that the sorption of each Pu species was rate-limited, as the sorption could not be described by assuming local equilibrium in the experiments. The model was able to describe the sorption of the different Pu species that occurring either on fracture surfaces, in the pores of the rock matrix, or simultaneously in both locations. While equally good fits to the data could be achieved using any of these assumptions, a fracture-dominated process was considered to be the most plausible because it provided the most reasonable estimates of sorption rate constants. Importantly, a key result of this work is that the sorption rate constant of all Pu species tends to decrease with increasing time scales, which implies that Pu will tend to be more mobile at longer time scales than observations at shorter time scales suggest. This result has important implications for predicting the environmental impacts of Pu in the safety assessments of geologic repositories for radioactive waste disposal, and we explore potential mechanistic bases for upscaling the sorption rate constants to time and distance scales that cannot be practically evaluated in experiments.

58 GEOSCIENCES↗

Evolution of texture and internal stresses within polycrystalline rock salt using in situ 3D synchrotron computed tomography and 3D X-ray diffraction

Over time rock salt caverns have been extensively used as reliable repositories for hazardous waste such as nuclear waste, oil or compressed gases. Undisturbed rock salt deposits in nature are usually impermeable and have very low porosity. However, rock salt formations under excavation stresses can develop crack networks, which increase their porosities; and in the case of a connected crack network within the media, rock salt may become permeable. Although the relationship between the permeability of rock salt and the applied stresses has been reported in the literature, a microscopic study that investigates the properties influencing this relationship, such as the evolution of texture and internal stresses, has yet to be conducted. This study employs in situ 3D synchrotron micro-computed tomography and 3D X-ray diffraction (3DXRD) on two small-scale polycrystalline rock salt specimens to investigate the evolution of the texture and internal stresses within the specimens. The 3DXRD technique measures the 3D crystal structure and lattice strains within rock salt grains. The specimens were prepared under 1D compression conditions and have shown an initial {111} preferred texture, a dominant {110}$\langle1\bar{1}0\rangle$ slip system and no fully connected crack network. The {111} preferred texture under the unconfined compression experiment became stronger, while the {111}$\langle1\bar{1}0\rangle$ slip system became more prominent. The specimens did not have a fully connected crack network until applied axial stresses reached about 30 MPa, at a point where the impermeability of the material becomes compromised due to the development of multiple major cracks.

36 MATERIALS SCIENCE↗

Physical Modeling of Coupled Thermohydraulic Behavior of Compacted MX80 Bentonite during Heating

Abstract This paper describes a tank-scale test setup and experimental methodology used to investigate coupled heat transfer and water flow processes during heating of compacted MX80 bentonite to high temperatures. Specifically, a temperature of 200°C was maintained by a cylindrical heating element at the center of a compacted bentonite layer containing an array of temperature, dielectric, and relative humidity sensors. In addition to providing an evaluation of the spatiotemporal variations in temperature, relative humidity, degree of saturation, and global volume, the coupled thermohydraulic properties of the bentonite were assessed. A wetting front was initially observed to move away from the central heater, followed by a drying process until reaching thermohydraulic equilibrium. The soil–water retention curve (SWRC) of the bentonite followed a wetting scanning path before following the primary drying path exhibiting a shift in water retention with elevated temperature. Results from the tank-scale test can be used for validation of numerical simulations of drying processes in the engineered barrier system of a high-level radioactive waste geological disposal repository and confirm that a temperature-dependent hysteretic SWRC with scanning paths is required to accurately capture the bentonite response.

Engineering↗