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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 415 records · Page 23
All sourcesNASA NTRSDOE OSTI
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.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2019

WIPP Operational and Safety Lessons Learned from the 2014 Fire and Radiological Events - 19389

The Waste Isolation Pilot Plant (WIPP) experienced two accident events in 2014 within 9 days of each other (salt haul truck fire and a radiological release). The repository was designed in the 1980's for high level waste and started operations in late 1990's for defense related transuranic (TRU) waste. Several long-standing technical issues from competing requirements between an underground facility (mine), nuclear safety, and environmental requirements lead to design, operations, and safety weaknesses that were not resolved prior to the two accident events. Other design issues and actions during early recovery efforts were identified as lessons learned for the Safety Significant Confinement Ventilation System (SSCVS) and Utility Shaft (US) capital asset projects and for future planning efforts. The infrastructure at WIPP was significantly degraded at the time of the events with key safety related items that had been out of service or not maintained for years. The emergency response to the two accident events was less than adequate and caused concerns with stakeholders. There are many operational and safety lessons learned from these two events and their corrective actions that will be valuable for all future planning of deep geological repositories (DGR). (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Preliminary Long-term Safety Assessment for the Planned LLW Disposal Facility at Al-Tuwaitha, Iraq - 18142

Before 1991, Iraq had a significant nuclear program which encompassed ten nuclear sites spread out across the country. The largest nuclear site was located at the Al-Tuwaitha site near Baghdad where 18 nuclear facilities were concentrated. During the first Gulf War in 1991, all sites suffered significant damage from bombing and subsequent looting. Currently, the Ministry of Science and Technology is responsible for the ten heavily damaged nuclear sites and for the management of radioactive waste in Iraq in general. The task of decommissioning the damaged nuclear facilities and managing the resulting waste is being supported by the International Atomic Energy Agency (IAEA), the European Commission (EC), and the United States (US). In the framework of its Instrument for Nuclear Safety Cooperation (INSC), the EC has launched a cooperation project to support the planned construction of an engineered repository for short-lived low- and intermediate level waste for the safe disposal of radioactive waste resulting from the decommissioning activities, as well as for waste from the continuing use of radioisotopes in medicine and the oil and gas industry in the country. The main objectives of this project, which was awarded to a Consortium led by NUKEM Technologies Engineering Services GmbH and joined by DBE Technology GmbH of Germany and JAVYS a.s. of Slovakia, are the development of an initial conceptual level basic design and preliminary safety assessment report (PSAR) and the subsequent detailed engineering design and supporting pre-construction safety assessment report (PCSAR). The current paper focuses on the development of the PSAR. Special focus is given to the long-term calculations and difficulties associated with the limited data base in regard to site characterization as well as the expected inventory for the future repository. Because of the ongoing security concerns in Iraq, the Ministry of Science and Technology had already selected the Al-Tuwaitha Site as the best suited location for the planned surface repository at the start of the project. Although some site characterization work had already been carried out prior to the start of the project, certain data for modelling the geology and hydrology of the site are still lacking. Missing data have been compensated by conservative assumptions and the assessment of alternative scenarios. Consequently, for the development of the simplified GoldSim{sup R} computer model used to carry out the long-term calculations supporting the PSAR, existing site information was used and, as appropriate, amended or replaced by conservative assumptions. Due to the nature of the waste, data on the expected inventory are associated with large uncertainties. Although certain estimates related to the future volume of the waste exist, little to no information is available on the expected radionuclide vector and respective activities. Therefore, the long-term calculations were carried out for a generic inventory including a broad range of radionuclides that are to be expected as being important considering the kind of waste to be disposed of in the facility. Based on the results of these calculations, the maximum total capacity of the facility was estimated and converted into activity limits for individual radionuclides that will be integrated into the existing general WAC for the facility. Compliance with these WAC will then guarantee the safety of the repository in regard to potential radionuclide releases via the groundwater pathway. In parallel to the determination of activity limits for the WAC, long-term calculations were carried using different estimates for the expected total activity to determine the general suitability of the proposed technical solution of the repository for receiving the total amount of Iraqi radioactive waste principally acceptable for surface disposal. (authors)

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DOE OSTI2017

Experiments and Modeling to Support Field Test Design

Disposition of heat-generating nuclear waste (HGNW) remains a continuing technical and sociopolitical challenge. We define HGNW as the combination of both heat generating defense high level waste (DHLW) and civilian spent nuclear fuel (SNF). Numerous concepts for HGNW management have been proposed and examined internationally, including an extensive focus on geologic disposal (c.f. Brunnengräber et al., 2013). One type of proposed geologic material is salt, so chosen because of its viscoplastic deformation that causes self-repair of damage or deformation induced in the salt by waste emplacement activities (Hansen and Leigh, 2011). Salt as a repository material has been tested at several sites around the world, notably the Morsleben facility in Germany (c.f. Fahland and Heusermann, 2013; Wollrath et al., 2014; Fahland et al., 2015) and at the Waste Isolation Pilot Plant (WIPP) near Carlsbad, NM. Evaluating the technical feasibility of a HGNW repository in salt is an ongoing process involving experiments and numerical modeling of many processes at many facilities.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

DECOVALEX-2019: An international collaboration for advancing the understanding and modeling of coupled thermo-hydro-mechanical-chemical (THMC) processes in geological systems

The DECOVALEX Project is an international research collaboration for advancing the understanding and modeling of coupled thermo-hydro-mechanical-chemical (THMC) processes in geological systems. DECOVALEX stands for “DEvelopment of COupled Models and VALidation against EXperiments”. The creation of this international initiative, now running for almost 30 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, and also for a range of other sub-surface engineering activities. 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 most recent phase of the DECOVALEX Project, here referred to as DECOVALEX-2019, started in 2016 and ended in 2019. Modeling teams from 13 international partner organizations participated in the comparative evaluation of seven modeling tasks involving complex field and/or laboratory experiments. Furthermore, this Virtual Special Issue on DECOVALEX-2019 provides an in-depth overview of these collaborative research efforts and how these have advanced the state-of-the-art of understanding and modeling coupled THMC processes.

58 GEOSCIENCES↗
DOE OSTI2017

Engineering-Scale Development/Demonstration of Zirconium Recovery from Used Duel Cladding

Recognizing that the zirconium (Zr) in used nuclear fuel (UNF) cladding is the second largest mass in UNF assemblies, process development studies for the recovery and purification of Zr were initiated and have been in progress at Oak Ridge National Laboratory (ORNL) for the last several years as a major element of waste minimization for advanced nuclear fuel recycle. Together with uranium recovery and recycle, Zr recovery would divert >90% (wt.) of the UNF assemblies from emplacement in a geologic repository by converting the Zr to low-level waste or reuse/recycle.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Mineral-specific heterogeneous neptunium sorption onto geological repository rocks in oxic and anoxic conditions and various temperatures

Neptunium poses challenges for radioactive wastes management due to its long half-life and ingrowth from americium decay, as well as its high mobility in water in its oxidized forms. Np(V)-bearing aqueous solutions were contacted with polished and crushed gneiss and dolerite from the Yeniseisky site, Russia, which is under consideration as a location for an underground repository, both in oxic and anoxic conditions at 20 and 90 °C. Neptunium sorption on crushed gneiss and dolerite in oxic conditions at 20 °C was quite low, but increased substantially in anoxic conditions. Autoradiography on samples treated at 20 °C revealed that sorbed Np was associated mostly with dark colored iron-bearing minerals, and solvent extraction indicated partial reduction of Np(V) to Np(IV). Sorption of Np from aqueous solutions contacted with dolerite and gneiss at 90 °C was in all cases higher than at the lower temperature. Autoradiography of polished rock samples treated in anoxic conditions at 90 °C revealed that Fe-bearing minerals had 3–4 orders of magnitude more Np sorbed on them than the quartz and feldspar grains. X-ray photoelectron spectroscopy indicated this sorbed Np was present as NpO 2 . This study supports the concept that the geologic conditions present at the planned repository site will retard Np migration.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Engineered Barrier System R&D and International Collaborations – LANL (FY20): Spent Fuel and Waste Disposition

The United States Department of Energy’s Spent Fuel and Waste Disposition (SFWD) program is investigating the design and safety function of generic nuclear geologic repositories in a variety of geologic settings (salt, argillite, and crystalline rock). Different configurations and loadings of spent nuclear fuel and waste within disposal canisters are also being investigated, some of which have the potential to generate repository temperatures higher than previously considered (i.e., temperatures >100ºC) by foreign and domestic concepts. This report expands on engineered barrier material stability in a high temperature crystalline rock repository through high temperature hydrothermal experiments. Experiments were designed to develop engineered barrier system (EBS) concepts in a hightemperature crystalline environment in 1) bentonite-Grimsel Granodiorite interactions, 2) bentonite-cement reactions, and 3) interaction between waste canister materials and bentonite. Experiment results are applied to understanding long-term repository performance in terms of radionuclide isolation. One hydrothermal experiment was completed in the rocking autoclaves at LANL in FY-20: IEBS-6 (Grimsel Granodiorite + Wyoming bentonite + cured ordinary Portland cement + Grimsel Granodiorite synthetic groundwater, 250ºC/150 bar, 8 weeks). Several other experiments were planned but were delayed due to the COVID-19 pause in laboratory work. In addition, some characterization of the reaction products of experiments conducted in FY-20 was prevented by COVID-19. Mineral phase chemistry was not measured via electron microprobe analyses for IEBS-6. Quantitative X-ray diffraction results from IEBS-6 and HBT-1 were not completed. The missing analyses and discussion of the results will be included in next year’s report. New characterization that was completed includes scanning electron microscopy of reaction products from IEBS-6, quantitative X-ray diffraction results are presented from IEBS-1 through IBES-5, preliminary scanning electron microscope images and chemical analyses for IEBS-6, X-ray diffraction of the clay fraction from all experiments, measurement/imaging of mineral growth on the surface of steel coupons. Major observations pertaining to bentonite stability in a Grimsel Granodiorite environment include the stability of Na-montmorillonite at 250°C, the formation of trace CSH phases, and the formation of bentonite colloids on experiment cooling. The addition of a cured chip of Portland cement to the bentonite-Grimsel system results in slightly higher pH values and the formation of diverse secondary mineral phases that were not observed in the previous experiments (e.g., analcime, garronite, CSH phases). The new characterization efforts related to the interaction of stainless-steel coupons and bentonite clay focused on thickness and mineralogy of phases that formed at the steel surface. In Wyoming bentonite + Grimsel Granodiorite systems, newly formed minerals at the bentonitesteel coupon interface included alteration of the outermost steel edge to Fe,Cr-oxide phases, followed by Fe-rich phyllosilicates (Fe-saponite, chlorite) and interbedded Fe,Cr,Ni-sulfide phases (pentlandite). Hydrothermal experiments were completed to assess uranium-carbonate complexation at conditions relevant to high-temperature disposal. Autoclave solubility experiments were conducted at 150 to 250ºC with a range of carbonate and uranium concentrations. The experiment results were characterized via situ UV-Visible spectroscopy and synchrotron-based in situ XAS techniques. Results show a significant decrease in the stability of uranyl-carbonate complexes at temperatures above 100ºC along with the precipitation of uranium oxides. Further, at T > 200ºC, results show that uranyl-hydroxyl complexes control solubility of uranium instead of the previously predicted uranyl-carbonate species. These results are significant for understanding the mobility of uranium in the EBS, which will likely contain carbonate-rich fluids. International research efforts focused on three main areas: 1) participation in international conferences, 2) building collaborations with foreign repository programs, and 3) the initiation of an experimental program to complement the full-scale HotBENT test at the Grimsel test site. This experiment included Wyoming bentonite + low carbon steel + Grimsel Granodiorite synthetic groundwater and was run at the planned maximum temperature of the HotBENT test (200°C). Complete characterization of reaction products was hindered by disruptions to laboratory work but will be reported in the next FY. The experimental results obtained in FY-20 continue to document the wide-ranging effects of bulk composition and pressure-temperature conditions in the mineralogical and geochemical evolution of a high-temperature repository environment. Concepts developed will be used to inform models of long-term material stability in a generic crystalline rock-hosted repository.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2019

Development and Demonstration of Monitoring Strategies and Technologies -Modern2020 Project - 19317

The Modern2020 project aims at providing the means for developing and implementing an effective and efficient repository operational monitoring program, taking into account the requirements of specific national programs. The work allows advanced national radioactive waste disposal programs to design monitoring systems suitable for deployment when repositories start operating in the next decade and supports less developed programs and other stakeholders by illustrating how the national context can be taken into account in designing dedicated monitoring programs tailored to their national needs. The work has been established to understand what should be monitored within the frame of the wider safety cases and to provide methodology on how monitoring information can be used to support decision-making and to plan for responding to monitoring results. Several developments on innovative repository monitoring techniques (wireless data transmission, alternative power supply sources, new sensors, geophysical methods) has been done from the proof of feasibility stage to the technology development and demonstration phase. Innovative technical solutions facilitate the integration and flexibility of required monitoring components to ease the final implementation and adaptation of the monitoring system. Full-scale in-situ demonstrations of innovative monitoring techniques were done in way to evaluate the performance of the state-of-the-art, the innovative techniques and their comparison with conventional ones. Finally, we will introduce the experiences of the local public stakeholders that have been involved in the Modern2020 project by focusing on the participation in practice of the Belgian, French, Finnish and Swedish local stakeholders, This paper provides an overview of the European Commission Horizon2020 Modern2020 project's main goals and progress to date. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Glass-Bonded Monazite Waste Forms for Lanthanide and Actinide Immobilization: From Theoretical Design to Scale-Up Production and Characterization

The development of nuclear waste forms for both existing and future nuclear wastes is critical to ensuring global environmental safety. This study focuses on waste management from molten salt reactors, where fuel exists in a salt form and could be processed in real time for the removal of neutron poisons such as xenon isotopes (e.g., 135 Xe) and rare earth elements (REEs, e.g., 149 Sm). To ensure safe, stable, and long-term disposal in geological repositories, REEs must be incorporated into a durable waste form. Iron-phosphate glasses are a promising candidate due to their low melting points, high chemical durability, and their ability to incorporate high concentrations of REEs. In this study, we successfully prepared iron-phosphate glass waste forms with high Nd loadings (up to 37 mass %) in batch sizes ranging from small (23 g) to large (1600 g). The resulting materials contained up to 75 mass % NdPO 4 , contributing to their mechanical resilience and exceptional chemical durability. These findings highlight the potential of iron-phosphate glasses as high-efficiency, chemically durable waste forms and demonstrate the successful transition from theoretical design to scaled-up production.

amorphous materials↗
DOE OSTI2018

Conception and Operation of a New Treatment Center for Radioactive Waste from High Energy Accelerators - 18293

CERN has operated high-energy accelerators for more than 60 years of research in fundamental physics. The side-product of this activity is the generation of low- and intermediate-level radioactive waste, most of which is in solid form and free of surface contamination. Today, one operational year produces about 400 tons of radioactive waste which need to be disposed of towards the final repositories of the two CERN Host States, France and Switzerland. A new facility for the collection, interim storage, characterization and treatment of radioactive waste became operational at CERN in 2015. This facility was specifically conceived for an accelerator complex with a wide range of challenging waste items, which are often unique in their irradiation history as well as in their physical, chemical and radiological characteristics. The disposal rate was ramped up in 2016 with a unique treatment process tailored for metallic low-level waste. In 2017, two parallel processes were successfully tested for the elimination of radioactive cables and for the recycling of valuable metals. This paper gives an overview of the challenges in the design, commissioning and operation of the CERN radioactive waste treatment center. It outlines the methodology followed for the conception of the elimination processes, which can be of guidance for the development of similar facilities. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Reactive transport in the complex heterogeneous alluvial aquifer of Fortymile Wash, Nevada

Yucca Mountain, Nevada, had been extensively investigated as a potential deep geologic repository for storing high-level nuclear wastes. Previous field investigations of stratified alluvial aquifer downstream of the site revealed that there is a hierarchy of sedimentary facies types. There is a corresponding log conductivity and reactive surface area subpopulations within each facies at each scale of sedimentary architecture. Here in this paper, we use a Lagrangian-based transport model in order to analyze radionuclide dispersion in the saturated alluvium of Fortymile Wash, Nevada. First, we validate the Lagrangian model using high-resolution flow and reactive transport simulations. Then, we used the validated model to investigate how each scale of sedimentary architecture may affect long-term radionuclide transport at Yucca Mountain. Results show that the reactive solute dispersion developed by the Lagrangian model matches the ensemble average of numerical simulations well. The link between the alluvium spatial variability and reactive solute dispersion at different spatiotemporal scales is demonstrated using the Lagrangian model. Finally, the longitudinal dispersivity of the reactive plume can be on the order of hundreds to thousands of meters, and it may not reach its asymptotic value even after 10,000 years of travel time and 2–3 km of travel distance.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Modelling yield cap evolution in sandstone based on brittle creep experiments

The Zenifim Formation is being considered as a potential disposal formation for a deep borehole nuclear repository concept in Israel. Site selection and repository construction are intended to ensure that waste is separated from circulating groundwater, but long-term deformation of the wellbore could potentially create fluid flow pathways. To understand how time-dependent rock strength could affect wellbore stability, here we conducted creep tests under low to moderate confining pressures on retrieved core from the Zenifim formation. During creep, samples strain slowly as gradual damage accumulation progressively weakens the samples. Failure eventually occurred through the near-instantaneous formation of a shear fracture. Experimental results were used to calibrate a continuum damage poro-elastic model for sandstones. The calibrated damage-poro-elastic model successfully simulates different types of loading experiments including quasi-static and creep. The state of strain in experiments is close to yield during loading as the yield cap continuously evolves with damage accumulation. For creep tests, most damage occurs during triaxial loading. Minor damage accumulation occurs under constant load until the final stage of creep, where damage accelerates and promotes unstable fracturing.

58 GEOSCIENCES↗
DOE OSTI2024

Machine learning surrogates for surface complexation model of uranium sorption to oxides

Abstract The safety assessments of the geological storage of spent nuclear fuel require understanding the underground radionuclide mobility in case of a leakage from multi-barrier canisters. Uranium, the most common radionuclide in non-reprocessed spent nuclear fuels, is immobile in reduced form (U(IV) and highly mobile in an oxidized state (U(VI)). The latter form is considered one of the most dangerous environmental threats in the safety assessments of spent nuclear fuel repositories. The sorption of uranium to mineral surfaces surrounding the repository limits their mobility. We quantify uranium sorption using surface complexation models (SCMs). Unfortunately, numerical SCM solvers often encounter convergence problems due to the complex nature of convoluted equations and correlations between model parameters. This study explored two machine learning surrogates for the 2-pK Triple Layer Model of uranium retention by oxide surfaces if released as U(IV) in the oxidizing conditions: random forest regressor and deep neural networks. Our surrogate models, particularly DNN, accurately reproduce SCM model predictions at a fraction of the computational cost without any convergence issues. The safety assessment of spent fuel repositories, specifically the migration of leaked radioactive waste, will benefit from having ultrafast AI/ML surrogates for the computationally expensive sorption models that can be easily incorporated into larger-scale contaminant migration models. One such model is presented here.

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DOE OSTI2022

Reduced diffusion and enhanced retention of multiple radionuclides from pore structure characterization of barrier materials for enhanced repository performance

Fluid flow and chemical transport in porous media are the macroscopic consequences of pore structure, which integrates geometry (e.g., pore size and surface area, pore-size distribution) and topology (e.g., pore connectivity). Low-permeability geological media whose pores are poorly interconnected will exhibit the characteristics of anomalous diffusion and sample size-dependent effective porosity, which will strongly impact long-term net diffusion and retention of radionuclides in geological repository settings involving different host rocks and barrier materials. A suite of innovative and complementary experimental approaches is utilized to study the microscopic pore structure and macroscopic fluid flow & chemical transport for a range of host rocks and barrier materials, in addition to standard clay minerals and reference rocks. With a particular focus on quantifying the presence and magnitude of “isolated” pores for a reduced effective porosity in low-permeability geomedia, the integrated methodologies for basic properties and pore structure characterization of these geomedia include X-ray diffraction, thin section petrography, grain size distribution, water immersion porosimetry after vacuum-pulling for full saturation, mercury intrusion porosimetry, nitrogen physisorption, scanning electron microscopy, X-ray computed tomography, and (ultra-)small angle neutron (X-ray) scattering. In addition, custom-designed gas diffusion, tracer recipe involving a range of anionic and cationic chemicals with subsequent analyses by laser ablation and inductively coupled plasma-mass spectrometry, along with batch sorption, column transport, and imbibition tests were conducted for coupled effects of pore structure and chemical retention/transport. From the perspectives of pore structure in conjunction with multiple and complementary approaches to examining a range of sample sizes under different observational scales, we find that the poor pore connectivity is prevalent in low-permeability media (mudstone and crystalline rock) that is related to geological processes (e.g., compaction, diagenesis and thermal maturation). For example, the deep and organic matter-rich mudstones have a much smaller effective porosity than the total porosity (as a result of poor pore connectivity) and associated diffusion coefficient, and the effective porosity & diffusion coefficients are also dependent upon the sample sizes used in the measurement. Similarly, most of the pore space in the shallow mudstone is also controlled by pore-throat diameters in the 5-50 nm range of intergranular pore types from its fine-grained nature, but with an overall good pore connectivity. However, the nm-sized pore space (physically pore-network architecture) and strong sorption capacities (chemical retention from clay minerals) of both shallow and deep mudstones lead to the synergistic retention of cationic radionuclides and their utilities as effective host rocks and barrier materials. Our unique approaches of studying how the micro-scale pore structure affect macro-scale fluid flow, diffusion & retention, and chemical transport produce improved mechanistic understanding, and realistic quantification, of diffusion and retention of typical radionuclides in a range of generic host rocks and barrier materials (clay/shale, salt, crystalline rock, and tuff), with the overall results leading to scientifically-based understanding of enhanced isolation (from both diffusion and retention) of radionuclides and improved confidence on the long-term performance of geological repository to store high-level radioactive wastes. In addition to the training of 25 undergraduates, graduates, and postdocs of UTA, the scientists (organizations) involved in performing this work (e.g., discussion, sample sharing, and operation of SANS and SAXS instruments) include Ed Matteo, Yifeng Wang, and Kristopher Kuhlman (Sandia National Laboratories), Jens Birkholzer, Liange Zheng, Tim Kneafsey, and Sharon Borglin (Lawrence Berkeley National Laboratory), Mavrik Zavarin (Lawrence Livermore National Laboratory), Yukio Tachi and Yuta Fukatsu (Japan Atomic Energy Agency), Mieke de Craen (Euridice, Belgium), Markus Bleuel (NIST), Wei-Ren Chen, Gergely Nagy, Changwoo Do, William Heller, Larry Anovitz, and Kenneth Littrell (ORNL), as well as Jan Illvsky, Ivan Kuzmenko, Ju-Sang Park and Jon Almers (ANL). Key deliverables include a total of 13 peer-reviewed journal articles (nine published and three under review), 23 presentations at scientific conferences (AAPG, AAPG Southwest Section, AGU, Asian Clay Conference, GSA, GSA South-Central Section, IHLRWM, InterPore, International Conference on Chemistry and Migration Behavior of Actinides and Fission Products in the Geosphere, International Conference on Coupled Processes in Fractured Geological Media: Observation, Modeling and Application), and academic institutions (UTA, New Mexico State University; University of Poitiers, France; University of Helsinki, Finland; Uppsala University, Sweden; Istanbul Technical University, Turkey) and other organizations (Andra, France; Posiva Oy, Finland).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Dehalogenation reactions between halide salts and phosphate compounds

Reactions between phosphoric acid [H 3 PO 4 ] or ammonium hydrogen phosphates [i.e., NH 4 H 2 PO 4 , (NH 4 ) 2 HPO 4 ] and halide salts can be used to dehalogenate (remove halides from) salt-based waste streams, where the process of removing halides yields products that have more efficient disposal pathways for repository storage. In this context, the term efficiency is defined as higher waste loadings and simplified immobilization processes with potential for recycle of certain salt components (e.g., 37 Cl as H 37 Cl or NH 4 37 Cl). The main streams identified for these processes are nuclear wastes generated during electrochemical reprocessing of used nuclear fuel as well as used halide salts from molten salt reactor operation. The potential byproducts of these reactions are fairly consistent across the range of halide species (i.e., F, Cl, Br, I) where the most common are hydrogen halides [e.g., HCl (g) ] or ammonium halides (e.g., NH 4 Cl). However, trihalide compounds (e.g., NCl 3 ), nitrogen triiodide ammine adducts [NI 3 ·(NH 3 ) x ], and ammonium triiodide (NH 4 I 3 ) are also possible. Several of these byproducts (i.e., NCl 3 , NBr 3 , NI 3 , and NH 4 I 3 ) are shock-sensitive contact explosives so their production in these processes must be tracked and carefully controlled, which includes methods of immediate neutralization upon production such as direct transport to a caustic scrubber for dissolution. Several benefits arise from utilizing H 3 PO 4 as the phosphate additive during dehalogenation reactions for making iron phosphate waste forms including more oxidized iron (higher Fe 3+ :Fe 2+ ratios), higher chemical durabilities, and the avoidance of trihalides, but the byproducts are hydrogen halides, which are corrosive and require special handling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Unsaturated alluvium disposal modelling with improved geological realism

This report describes specific activities in the Fiscal Year (FY) 2023 associated with the Geologic Disposal Safety Assessment (GDSA) Repository Systems Analysis (RSA) work package funded by the Spent Fuel and Waste Science and Technology (SFWST) Campaign of the U.S. Department of Energy Office of Nuclear Energy (DOE-NE), Office of Spent Fuel and Waste Disposition (SFWD). The overall objective of the GDSA RSA work package is to develop generic deep geologic repository concepts and system performance assessment (PA) models in several potential host-rock environments, and to simulate and analyze these generic repository concepts and models using the GDSA Framework toolkit and other tools as needed. The specific GDSA goal addressed in this report is reference case development, simulation, and analysis for the unsaturated alluvium (UZ), one of the four potential host-rocks considered by the GDSA. Further, we aim to exercise the simulation tools and methodologies under development by GDSA for PA modelling.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Framework for The Analysis of US Permanent Geologic Disposal Options for Radioactive Waste

The U.S. study of permanent geologic disposal options of spent nuclear fuel (SNF) and high-level radioactive waste (HLW) provided a technical basis for informing policy decisions regarding strategies for the management and disposal of radioactive waste requiring geologic isolation through the evaluation of potential impacts of waste forms on the feasibility and performance of representative generic concepts for geologic disposal. The goal of the study was to help inform relevant policy questions including: Is a "one-size-fits-all" repository a good strategic option for disposal? Do different waste types and forms perform differently enough in different disposal concepts that they warrant different treatment? Do some disposal concepts perform significantly better with or without specific waste types or forms?

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗