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At least 469 records · Page 26

Cold crucible induction melter studies for making glass ceramic waste forms: A feasibility assessment

Glass ceramics are being developed to immobilize fission products, separated from used nuclear fuel by aqueous reprocessing, into a stable waste form suitable for disposal in a geological repository. This work documents the glass ceramic formulation at bench scale and for a scaled melter test performed in a pilot-scale (approximately 1/4 scale) cold crucible induction melter (CCIM). Melt viscosity, electrical conductivity, and crystallization behavior upon cooling were measured on a small set of compositions to select a formulation for melter testing. Property measurements also identified a temperature range for melter operation and cooling profiles necessary to crystallize the targeted phases in the waste form. Bench scale and melter run results successfully demonstrate the processability of the glass ceramic using the CCIM melter technology.

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Evaluate opportunities for monitoring the oxidation states of technetium in both organic and aqueous phases using Raman spectroscopy

An important isotope in the nuclear fuel cycle, 99 Tc is characterized by its long half-life of 2.1 × 10 5 years and its beta emission. It is generated through the fission of 235 U. As the burnup levels of nuclear waste continue to rise, the concentration of technetium in spent fuel increases, leading to a heightened interest in its quantification during the reprocessing of spent nuclear fuel. In HNO3 environments, technetium predominantly exists as TcO 4 − ; however, it tends to interfere with reducing agents, decreasing the separation efficiency for actinides. Therefore, accurate quantitative determination of technetium is critical to controlling its distribution and mitigating its negative effect on the reprocessing of spent fuel.

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CANDLE Burning Reactor with Plutonium Fuel Start-up Core

The CANDLE burning fast reactor concept makes it possible to utilize natural uranium or depleted uranium with high burnup of up to 40% without repossessing of spent fuel from the reactor. Once the reactor reaches equilibrium burning wave condition, it needs only natural or depleted uranium, although it needs some amount of fissile material for the startup. Studies have been performed for the startup core using enriched uranium and absorbers. It is expected that plutonium obtained by reprocessing of spent fuel from light water reactors (LWR) will be an excellent fuel for the startup core. Using this fuel for the startup core will eliminate the need to produce enriched uranium, as well as make it possible to utilize the plutonium from spent fuel effectively as a useful resource. For effective utilization of plutonium as a resource, a startup core that requires only a small amount of plutonium fuel is preferable. The purpose of this study was to clarify the CANDLE burning fast reactor concept using a minimum amount of plutonium fuel from LWR spent fuel for the startup core by analysis with a simplified reactor model. (authors)

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Radiation chemistry in the reprocessing and recycling of spent nuclear fuels

The interaction of ionizing radiation with solvent extraction solutions results in the ionization, excitation, and decay to neutral radicals of mainly diluent molecules. These produced reactive species diffuse into the bulk solution to react with solvent extraction ligands. Ligand reactions often result in deleterious effects such as loss in ligand concentration or the production of decomposition products that may also be complexing agents. This often interferes with desired separations. The common radiolysis reactions and their potential effects on solvent extraction are reviewed here.

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Handling of Ammonium Nitrate Mother-Liquid Radiochemical Production - 13089

The aim of the work is to develop a basic technology of decomposition of ammonium nitrate stock solutions produced in radiochemical enterprises engaged in the reprocessing of irradiated nuclear fuel and fabrication of fresh fuel. It was necessary to work out how to conduct a one-step thermal decomposition of ammonium nitrate, select and test the catalysts for this process and to prepare proposals for recycling condensation. Necessary accessories were added to a laboratory equipment installation decomposition of ammonium nitrate. It is tested several types of reducing agents and two types of catalyst to neutralize the nitrogen oxides. It is conducted testing of modes of the process to produce condensation, suitable for use in the conversion of a new technological scheme of production. It is studied the structure of the catalysts before and after their use in a laboratory setting. It is tested the selected catalyst in the optimal range for 48 hours of continuous operation. (authors)

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Adsorption modeling for off-gas treatment

Off-gas generated from the reprocessing of used nuclear fuel contains a mixture of several radioactive gases including {sup 129}I{sub 2}, {sup 85}Kr, HTO, and {sup 14}CO{sub 2}. Over the past few decades, various separation and recovery processes have been studied for capturing these gases. Adsorption data for gaseous mixtures of species can be difficult to determine experimentally. Therefore, procedures capable of predicting the adsorption behavior of mixtures need to be developed from the individual isotherms of each of the pure species. A particular isotherm model of interest for the pure species is the Generalized Statistical Thermodynamic Adsorption isotherm. This model contains an adjustable number of parameters and will therefore describe a wide range of adsorption isotherms for a variety of components. A code has been developed in C++ to perform the non-linear regression analysis necessary for the determination of the isotherm parameters, as well as the least number of parameters needed to describe an entire set of data. (authors)

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Product Consistency Testing of Hot Isostatically Pressed Iodine-containing Waste Forms

Silver-exchanged mordenite (AgZ) is currently under evaluation for the capture of iodine from the off-gas streams that are expected to arise during the reprocessing of used nuclear fuel. A final waste form for AgZ loaded with radioactive iodine has not yet been identified. The applicability of hot isostatic pressing (HIPing) to convert iodine-loaded, reduced silver-exchanged mordenite (I-Ag{sup 0}Z) into a suitable waste form is currently being evaluated at Oak Ridge National Laboratory (ORNL). Because production of such a waste form requires little preprocessing of the I-Ag{sup 0}Z, HIPing could prove very attractive from both safety and economic perspectives. It is desirable to produce a waste form with a distinct iodine-containing mineral phase as the major constituent. Such a mineral phase is thought to increase long-term iodine retention and overall stability. Furthermore, the transformation of the material into a known iodine-containing mineral phase would limit the additional experimental testing and modeling required to determine the long-term stability of the pressed pellet, as much of that information has already been learned for several common iodine-containing minerals. For these reasons, the current work has investigated the possibility of converting I-Ag{sup 0}Z into an iodine-containing sodalite, similar to the efforts documented by Sheppard et al. in which they transformed other silver zeolite structures into sodalite through HIPing. Building on our initial work we are now producing hot isostatically pressed waste forms using mixtures of pure sodium mordenite, AgZ, and silver iodide. The composition of these samples is well known, in contrast with the previously used commercially available, binder-containing AgZ, which has a composition that is proprietary and uncharacterized. It is expected that by controlling the initial sample composition, we might be able to control the mineral phases present in the processed waste form. Transformation of the component material into a well-characterized iodine-containing mineral phase would be desirable; however, this is not an absolute requirement for success. (authors)

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Metal–organic framework with optimally selective xenon adsorption and separation

Nuclear energy is considered among the most viable alternatives to our current fossil fuel based energy economy.1 The mass-deployment of nuclear energy as an emissions-free source requires the reprocessing of used nuclear fuel to mitigate the waste.2 One of the major concerns with reprocessing used nuclear fuel is the release of volatile radionuclides such as Xe and Kr. The most mature process for removing these radionuclides is energy- and capital-intensive cryogenic distillation. Alternatively, porous materials such as metal-organic frameworks (MOFs) have demonstrated the ability to selectively adsorb Xe and Kr at ambient conditions.3-8 High-throughput computational screening of large databases of porous materials has identified a calcium-based nanoporous MOF, SBMOF-1, as the most selective for Xe over Kr.9,10 Here, we affirm this prediction and report that SBMOF-1 exhibits by far the highest Xe adsorption capacity and a remarkable Xe/Kr selectivity under relevant nuclear reprocessing conditions. The exceptional selectivity of SBMOF-1 is attributed to its pore size tailored to Xe and its dense wall of atoms that constructs a binding site with a high affinity for Xe, as evident by single crystal X-ray diffraction and molecular simulation.

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Waste Management Approach for a Potential Future U.S. Closed Fuel Cycle - 16233

The U.S. Department of Energy, Office of Nuclear Energy has chartered an effort to develop technologies to enable safe and cost effective recycle of commercial used nuclear fuel (UNF) in the U.S. Part of this effort includes the evaluation of exiting waste management technologies for effective treatment of wastes in the context of current U.S. regulations and development of waste forms and processes with significant cost and/or performance benefits over those existing. This study summarizes the results of these ongoing efforts with a focus on the highly radioactive primary waste streams. The primary streams considered and the recommended waste forms include: - Tritium separated from either a low volume gas stream or a high volume water stream. The recommended waste form is low-water cement in high integrity containers. - Iodine-129 separated from off-gas streams in aqueous processing. There are a range of potentially suitable waste forms. As a reference case, a glass composite material (GCM) formed by the encapsulation of the silver Mordenite (AgZ) getter material in a low-temperature glass is assumed. A number of alternatives with distinct advantages are also considered including a fused silica waste form with encapsulated nano-sized AgI crystals. - Carbon-14 separated from LWR fuel treatment off-gases and immobilized as a CaCO{sub 3} in a cement waste form. - Krypton-85 separated from LWR and SFR fuel treatment off-gases and stored as a compressed gas. - An aqueous reprocessing high-level waste (HLW) raffinate waste which is immobilized by the vitrification process in one of three forms: a single phase borosilicate glass, a borosilicate based glass ceramic, or a multi-phased titanate ceramic [e.g., synthetic rock (Synroc)]. - An undissolved solids (UDS) fraction from aqueous reprocessing of LWR fuel that is either included in the borosilicate HLW glass or is immobilized in the form of a metal alloy in the case of glass ceramics or titanate ceramics. - Zirconium-based LWR fuel cladding hulls and stainless steel (SS) fuel assembly hardware that are washed and super-compacted for disposal or as an alternative Zr purification and reuse (or disposal as low-level waste, LLW) by reactive gas separations. - Electrochemical process salt HLW which is immobilized in a glass bonded Sodalite waste form known as the ceramic waste form (CWF). - Electrochemical process UDS and SS cladding hulls which are melted into an iron based alloy waste form. Mass and volume estimates for each of the recommended waste forms based on the source terms from a representative flowsheet are reported. (authors)

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Conceptual design study on very small long-life gas cooled fast reactor using metallic natural Uranium-Zr as fuel cycle input

A conceptual design study of very small 350 MWth Gas-cooled Fast Reactors with Helium coolant has been performed. In this study Modified CANDLE burn-up scheme was implemented to create small and long life fast reactors with natural Uranium as fuel cycle input. Such system can utilize natural Uranium resources efficiently without the necessity of enrichment plant or reprocessing plant. The core with metallic fuel based was subdivided into 10 regions with the same volume. The fresh Natural Uranium is initially put in region-1, after one cycle of 10 years of burn-up it is shifted to region-2 and the each region-1 is filled by fresh Natural Uranium fuel. This concept is basically applied to all axial regions. The reactor discharge burn-up is 31.8% HM. From the neutronic point of view, this design is in compliance with good performance.

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An Investigation on the Sustainability of a Sodium-cooled Breed-and-Burn Fast Reactor (B and BR)

Fast reactor can effectively handle the used nuclear fuel (UNF) by transmuting long-living transuranic (TRUs) into relatively short-living fission products. It can also be used to produce fissile from fertile nuclides as fuels for another reactor. The breed-and-burn fast reactor (B and BR) is a unique concept of fast reactor, which can breed the fissile fuels and use the bred fuels in situ. Thanks to this characteristic, the fuel utilization in a B and BR can be extremely high and even the recycled fuel of a B and BR can be used as a fuel to spawn the next generation B and BR. The UNF from the first B and BR should be reprocessed or reconditioned so that it can be reused in the second B and BR. A fuel reprocessing technology named melt refining was used in EBR-II from 1964 to 1969 and it was also applied in our previous study which showed that second B and BR can be started using the recycled UNF of first B and BR. However, about 95% of rare earths are removed during the melt refining and the associated processes are not very simple. Moreover, the actinide loss can also be significant. To enhance the proliferation-resistance and economy of the reprocessing, a super-simplified melt and treatment (SSMT) process without removing rare earth nuclides is suggested and the feasibility study to start the second B and BR using SSMT is carried out in this paper. The neutronics simulations were done using the Monte Carlo code McCARD in conjunction with ENDF/B-VII cross-section library. (authors)

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Update on Plans for Treatment of Research Reactor Used Fuels at La Hague - 19507

Over the past decades, Orano (formerly AREVA) has been transporting, unloading, storing, and reprocessing research reactor spent fuel (RRSF) in its French facilities and with its equipment. This experience has resulted in the transportation and industrial-scale reprocessing of over 23 tons of RRSF (mainly of the Al type) at Orano's facilities in France, both in the Marcoule and the La Hague plants. In order to meet its customers growing needs in terms of RRSF management, Orano is developing new RRSF reprocessing capacities for the La Hague UP2-800 facility utilizing the lessons learned from the reprocessing of the current RRSF. This new facility is called the Traitement des Combustibles Particuliers or TCP and was introduced last year. The TCP is planned to reprocess several types of RRSF, including both Al and U{sub 3}Si{sub 2} RRSF, and in the future may also be useful in the support of reprocessing LWR and fast reactor MOX fuels. The focus of the TCP is on developing shearing and dissolution processes for these fuel types that can be incorporated into, and operated along with, the existing La Hague facilities. This paper will cover each of the stages of the current reprocessing of RRSF at La Hague from its transportation to La Hague to its post-reprocessing vitrified waste production, provide an update on its status, and identifying the areas where the TCP will better facilitate the reprocessing of the RRSF. Ultimately, this paper illustrates the innovative solutions available to modify existing recycling/reprocessing facilities to address pseudo-unique used nuclear fuel (UNF) forms to improve/simplify back-end UNF management. (authors)

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Rare Earth Electrochemical Property Measurements and Phase Diagram Development in a Complex Molten Salt Mixture for Molten Salt Recycle

Pyroprocessing is a promising alternative for the reprocessing of used nuclear fuel (UNF) that uses electrochemical methods. Compared to the hydrometallurgical reprocessing method, pyroprocessing has many advantages such as reduced volume of radioactive waste, simple waste processing, ability to treat refractory material, and compatibility with fast reactor fuel recycle. The key steps of the process are the electro-refining of the spent metallic fuel in the LiCl-KCl eutectic salt, which can be integrated with an electrolytic reduction step for the reprocessing of spent oxide fuels.

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Safeguards Approaches for Very Long-Term Storage of Spent Fuel

Many States are considering interim very long-term storage (VLTS) strategies for spent fuel storage while final disposition options are developed. Under the VLTS approach, spent fuel will be stored for periods that could exceed 50 to 100 years. The long-term storage of spent fuel — and the increasing stockpile of plutonium contained in this spent fuel — exacerbate the international safeguards and verification needs for spent fuel. In particular, significant delays in any verification of the contents of spent fuel assemblies prior to disposition may cause even further delays in the final disposition (or reprocessing) of spent fuel. As a result, the resources required by the International Atomic Energy Agency (IAEA) to safeguard the increasing stockpile of spent fuel will increase. Safeguarding these interim storage facilities and subsequently, the transportation of long-term stored fuel, will place additional demands on IAEA resources if the current approach, which relies heavily upon inspectors being present at the facility, is to be continued. Current IAEA approaches to safeguarding above ground dry storage sites do not take into account the challenges associated with longer-term storage and are also very dependent on inspector presence. The IAEA is moving toward remote and unattended monitoring systems for safeguards and these systems should be utilized at VLTS facilities as much as possible. The research and development of various monitoring systems should be continued.

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Evaluation of Ruthenium Capture Methods for Tritium Pretreatment Off-Gas Streams

In the reprocessing of used nuclear fuel, radioactive elements are released into various plant off-gas streams. While much research and development has focused on the abatement of the volatile nuclides 3 H, 14 C, 85 Kr, and 129 I, the potential release of semivolatile isotopes that could also report to the off-gas streams in a reprocessing facility has been examined. Ruthenium (as 106 Ru) has been identified as one of the semivolatile nuclides requiring the greatest degree of abatement prior to discharging the plant off-gas to the environment.

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Joint Test Plan for the Evaluation of Iodine Retention for Long-Chain Organic Iodides

A number of reports have identified four volatile radionuclides that arise from the reprocessing of nuclear fuel ( 3 H, 14 C, 85 Kr, and 129 I) that require controls limiting their environmental release from reprocessing facilities in order to meet US regulatory requirements. Of these, 129 I has the longest half-life and highest potential biological impact.

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Hafnium(IV) complexation with oxalate at variable temperatures

Abstract Appropriate management of fission products in the reprocessing of spent nuclear fuel (SNF) is crucial in developing advanced reprocessing schemes. The addition of aqueous phase complexing agents can prevent the co-extraction of these fission products. A solvent extraction technique was used to study the complexation of Hf(IV) – an analog to fission product Zr(IV) – with oxalate at 15, 25, and 35°C in 1 M HClO

Chemistry↗

Development of a Regulatory Strategy for Post Operational Clean Out Activities at Sellafield Limited Nuclear Licensed Site - 20273

The Thermal Oxide Reprocessing Plant (THORP) at the Sellafield nuclear licensed site carried out its final commercial shear of spent nuclear fuel in November 2018, since when the facility has undergone rundown prior to cessation of operations. The Magnox Reprocessing Facility (MRF) is also due to cease operating, around the end of 2020. Following the cessation of spent fuel reprocessing, the facilities and supporting infrastructure will transition into Post Operational Clean Out (POCO), which will become an increasingly significant portion of Sellafield Limited's (SL) activities. POCO is defined as the set of activities undertaken directly after a nuclear facility comes to the end of its operational life, in order to place the plant in a suitable state for the subsequent decommissioning steps. The decommissioning strategy at SL is for deferred dismantling of these facilities, which will be subject to a period of Surveillance and Maintenance (S and M) following completion of POCO. This paper outlines the development and implementation of a regulatory strategy for POCO activities at the Sellafield site by the Office for Nuclear Regulation (ONR), the independent nuclear safety, transport and security regulator in the United Kingdom. The paper also describes how this regulatory strategy is applied to nuclear installations undergoing transition into POCO and subsequent decommissioning. ONR works jointly with the Environment Agency, as the environmental regulators in England, to ensure that matters relevant to them have been duly considered. In developing a regulatory strategy, ONR has taken a site-wide approach, moving away from regulation on a facility-by-facility basis, to promote consistency, as well as maximising efficiency and effectiveness. The aim of this integrated approach was to prevent complications during future decommissioning and dismantling that have been experienced previously at similar facilities in France. The strategy recognised that once reprocessing operations are concluded, the hazard present will be reduced significantly, which provides the opportunity for ONR to consider how best to deliver a proportionate approach to regulatory interventions. Once POCO has been completed and the facility has transitioned into a period of S and M, the scale and frequency of ONR's interventions will reduce, commensurate with the safety case covering the remaining hazard and activities associated with maintaining the facility prior to final decommissioning. This approach allows ONR to consider risks holistically, considering the full life cycle of the facility and by taking due account of the interdependencies between facilities across the site. The strategy also aligns with existing regulation of high hazard and risk reduction activities, which remain ONR's top priority. As SL progresses with POCO activities in THORP and across the rest of the site, ONR will review its regulatory strategy to ensure that the intended safety benefits are realised. (authors)

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