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The report addresses the experimental characterisation, thermo-mechanical modelling and performance of unirradiated and irradiated samples of spent nuclear fuel rod segments and cladding. Hydrogen is relocated in nuclear fuel claddings by diffusion along temperature, stress, and concentration gradients, and towards a liner if existent. The precipitation of hydrides during cool-down at the beginning of the storage is influenced by mechanical stress. A strong accumulation of hydrides and a disadvantageous hydride alignment in relation to the stress state can affect the mechanical properties and compromise the fuel cladding integrity. Neutron radiography is used to determine spatially resolved hydrogen and hydride distributions in claddings. A liner in duplex claddings attracts hydrogen, which will then no longer be available to form detrimental hydrides in the bulk part of the cladding. Individual three-point bending and gravitational impact tests on filled pressurised spent nuclear fuel rod segments were conducted in hot-cell facilities. The material behaviour under three-point bending in the presence of hydrides and at different temperatures was systematically investigated in quasi-static laboratory tests on unirradiated rod segments with and without surrogate pellets until rupture. Ring compression tests were carried out on irradiated and unirradiated samples at different temperatures and both with and without radial hydrides. With radial hydrides, brittle failure is possible even at low deformation and simultaneously low temperature. Crack initiation will occur on the radial hydride with the highest fracture mechanics load, which depends on the hydride size in the regions with the highest hoop stresses. Due to the high hydrogen content used in creep tests conducted, precipitation hardening of the hydrides in the zirconium alloy significantly reduces the creep rate, as it strengthens the material and inhibits the dislocation sliding. The use of finite element analyses on mechanical tests to determine the cladding properties using a numerical optimisation method based on a large number of automatically generated sensitivity calculations is demonstrated. The brittle fracture of cladding samples with radial hydrides in the ring compression test can be described with a cohesive zone model if the cohesive parameters are selected appropriately and the hydride morphology is specified. Progress was made in the verification, validation and enhancement of spent fuel performance codes by the compilation of a representative validation database (related to rod internal pressure, fission gas release, rod void volume, and in-clad hydrogen distribution), the enhancement of CIEMAT’s FRAPCON-xt code for rod internal pressure prediction at high burnup, the enhancement of CIEMAT’s in-clad hydrogen performance subroutine HYDCLAD with more phenomenological modelling, the extension of INL’s BISON code with a cladding creep law for dry storage, and a benchmark with FRAPCON-xt and BISON simulating in-reactor and dry storage scenarios.
During an extensive test programme at the Bundesanstalt für Materialforschung und prüfung, material property changes of EPDM O-rings were investigated at different ageing times and two ageing temperatures of 125 ◦ C and 150 ◦ C. To exclude possible diffusion-limited oxidation (DLO) effects that can distort the data, IRHD microhardness measurements were taken over the cross section of compressed O-rings. Continuous stress relaxation measurements were taken on samples free of DLO effects. The additional effect of physical processes to irreversible chemical ones during a long-term thermal exposure is quantified by the analysis of compression set measurements under various test conditions. By combining the different experimental methods, characteristic times relative to the degradation processes were determined. On the basis of experimental data, a microphysically motivated model that takes into account reversible and irreversible processes was developed. The parameter identification strategy of the material model is based on our experimental investigations on homogeneously aged elastomer O-rings. The simulated results are in good agreement with the experiments.
Long-term dry interim storage may adversely affect the mechanical properties of spent fuel rods, possibly resulting in a reduced resilience during handling or transport after storage. The cladding is the first barrier for the spent fuel pellets. An established method for characterising the cladding material is the ring compression test (RCT), in which a small, cylindrical sample of the cladding tube is subjected to a compressive load. Radial hydrides may precipitate in zirconium-based alloys (Zircaloy) under pre-storage drying and during slow cooling, which result in embrittlement of the cladding material and eventually a possible sudden failure of cladding integrity under additional mechanical loads. The focus of the presented research is on the development of appropriate nu-merical methods for predicting the mechanical behaviour and identification of limiting conditions to prevent brittle fracture of Zircaloy claddings. A modelling approach based on cohesive zones is ex-plained which is able to reproduce the propagation of cracks initiated at radial hydrides in the zir-conium matrix. The developed methods are applied to defueled samples of cladding alloy ZIRLO®, which were subjected to a thermo-mechanical treatment to reorient existing circumferential hy-drides to radial hydrides. A selected sample showing sudden load drops during a quasi-static ring compression test is analysed by means of fracture mechanics for illustrative purposes. Based on the developed fracture mechanics approach, not only the deformation behaviour but also the fail-ure behaviour of irradiated as well as unirradiated Zircaloy claddings with radial hydrides under RCT loading conditions can be adequately described.
Long-term dry interim storage may adversely affect the mechanical properties of spent fuel rods, possibly resulting in a reduced resilience during handling or transport after storage. The cladding is the first barrier for the spent fuel pellets. An established method for characterising the cladding material is the ring compression test (RCT), in which a small, cylindrical sample of the cladding tube is subjected to a compressive load. Radial hydrides may precipitate in zirconium-based alloys (Zircaloy) under pre-storage drying and during slow cooling, which result in embrittlement of the cladding material and eventually a possible sudden failure of cladding integrity under additional mechanical loads. The focus of the presented research is on the development of appropriate nu-merical methods for predicting the mechanical behaviour and identification of limiting conditions to prevent brittle fracture of Zircaloy claddings. A modelling approach based on cohesive zones is ex-plained which is able to reproduce the propagation of cracks initiated at radial hydrides in the zir-conium matrix. The developed methods are applied to defueled samples of cladding alloy ZIRLO®, which were subjected to a thermo-mechanical treatment to reorient existing circumferential hy-drides to radial hydrides. A selected sample showing sudden load drops during a quasi-static ring compression test is analysed by means of fracture mechanics for illustrative purposes. Based on the developed fracture mechanics approach, not only the deformation behaviour but also the fail-ure behaviour of irradiated as well as unirradiated Zircaloy claddings with radial hydrides under RCT loading conditions can be adequately described.
The European Joint Programme on Radioactive Waste Management (EURAD) is working on Spent Fuel Characterization (SFC) in its work package (WP) 8. Inspired by the EURAD activities, the International Atomic Energy Agency (IAEA) established an international Coordinated Research Project (CRP) on SFC. The EURAD WP SFC participants are collaborating as a team on the IAEA CRP on SFC. The EURAD WP SFC project consists of four tasks. Task 3 investigates the behaviour of nuclear fuel and cladding after discharge. The aim of these activities is to understand and describe the evolution of the cladding-pellet system and its ageing under conditions of extended interim storage, transportation and emplacement in a final disposal system. At the Third Research Coordination Meeting on Spent Fuel Characterization, BAM as contributor to Task 3 reported on the activities and status of its research work.
The investigation of the long-term performance of sealing systems employed in containers for radioactive waste and spent nuclear fuel is one research focus area for division 3.4 “Safety of Storage Containers” at the Bundesanstalt für Materialforschung und -prüfung. Metallic seals are in use in interim storage casks for used fuel and high active waste. Their change in performance over time is of high importance for maintaining safe enclosure. Therefore, investigations on these systems were started at BAM to get a general understanding of the relevant processes. Our investigations comprise investigations on different parameters which influence the seal performance and the main part is focussed on the time and temperature dependent behaviour.
In this contribution an update on the performed tests and their respective results will be given in respect to the overview presented in 2020.
The understanding of the long-term behaviour of the sealing systems and the performance evaluation during interim storage and subsequent transportation are our goals.
Brittle Failure Limits of Spent Fuel Claddings Subjected to Long-Term Dry Interim Storage Conditions
(2024)
The mechanical properties of spent fuel claddings can be adversely affected under the conditions of long-term dry interim storage, so that the failure limits may be reached in case of mechanical loads during handling or transport after storage. Pre-storage drying and the early stage of interim storage can expose the cladding to higher temperatures and higher tensile hoop stresses than those associated with in-reactor operation and pool storage. During slow cooling of a cladding tube under internal pressure, radial hydrides may precipitate in zirconium-based cladding alloys. This can lead to embrittlement of the material and sudden failure of the cladding integrity under mechanical stress. In order to prevent brittle failure, numerical methods are being developed to predict the mechanical behaviour and identify limiting conditions. Experimental investigations, numerical analyses and evaluation methods are discussed.
An established experimental method for characterising cladding materials is the Ring Compression Test (RCT). Some test results on irradiated cladding tubes after operation in pressure water reactors are publicly available. However, it is helpful to carry out studies on unirradiated surrogate claddings with similar material properties to reduce the effort associated with irradiated samples in hot cells and to perform material tests with a wider range of parameters. On the basis of such experimental data, load-displacement curves have been numerically analysed for a selection of cladding materials.
Radial hydrides can cause a sample to break suddenly due to fracture even at low deformation. Noticeable load drops in the RCT are caused by unstable crack propagation through the radial hydride network. The failure mechanism is quasi-cleavage in the hydrides and micro-void nucleation, growth, and coalescence in the zirconium matrix, with ductile tearing patches connecting adjacent hydrides. The cohesive zone approach was used to simulate the failure process taking into account the radial hydride morphology.
The developed method can adequately describe both the deformation and failure behaviour of irradiated as well as unirradiated claddings of zirconium-based alloys with radial hydrides under RCT conditions. Limiting conditions can be expressed in terms of fracture energy and cohesive strength.
Brittle Failure Limits of Spent Fuel Claddings Subjected to Long-Term Dry Interim Storage Conditions
(2024)
The mechanical properties of spent fuel claddings can be adversely affected under the conditions of long-term dry interim storage, so that the failure limits may be reached in case of mechanical loads during handling or transport after storage. Pre-storage drying and the early stage of interim storage can expose the cladding to higher temperatures and higher tensile hoop stresses than those associated with in-reactor operation and pool storage. During slow cooling of a cladding tube under internal pressure, radial hydrides may precipitate in zirconium-based cladding alloys. This can lead to embrittlement of the material and sudden failure of the cladding integrity under mechanical stress. In order to prevent brittle failure, numerical methods are being developed to predict the mechanical behaviour and identify limiting conditions. Experimental investigations, numerical analyses and evaluation methods are discussed.
An established experimental method for characterising cladding materials is the Ring Compression Test (RCT). Some test results on irradiated cladding tubes after operation in pressure water reactors are publicly available. However, it is helpful to carry out studies on unirradiated surrogate claddings with similar material properties to reduce the effort associated with irradiated samples in hot cells and to perform material tests with a wider range of parameters. On the basis of such experimental data, load-displacement curves have been numerically analysed for a selection of cladding materials.
Radial hydrides can cause a sample to break suddenly due to fracture even at low deformation. Noticeable load drops in the RCT are caused by unstable crack propagation through the radial hydride network. The failure mechanism is quasi-cleavage in the hydrides and micro-void nucleation, growth, and coalescence in the zirconium matrix, with ductile tearing patches connecting adjacent hydrides. The cohesive zone approach was used to simulate the failure process taking into account the radial hydride morphology.
The developed method can adequately describe both the deformation and failure behaviour of irradiated as well as unirradiated claddings of zirconium-based alloys with radial hydrides under RCT conditions. Limiting conditions can be expressed in terms of fracture energy and cohesive strength.
In der Wissenschaft und Technik gibt es verschiedene Gründe, um auf Basis geeigneter Modelle in die Zukunft schauen zu wollen, beispielsweise um zu bewerten, ob ein Bauteil auch noch deutlich länger verwendet werden kann als eigentlich einmal vorgesehen. Eine Methode dieses zu tun, basiert auf dem Zeit-Temperatur-Äquivalenz-Prinzip, welches besagt, dass ein Zustand oder eine Materialeigenschaft gleichwertig bei verschiedenen Zeit-Temperatur-Kombinationen auftritt oder erreicht werden kann. Höhere Temperaturen verkürzen in der Regel die Dauer und umgekehrt. In den letzten Jahrzehnten hat sich ein umfangreiches Methodenspektrum für unterschiedliche Werkstoffe und Anwendungsgebiete entwickelt, sodass die Identifikation einer geeigneten Methode für einen konkreten Anwendungsfall oder neue Materialien eine Herausforderung darstellt. These: „Fortschrittlich wäre, existierende Methoden zusammenzuführen, methodenspezifische Vorteile zu kombinieren, um mit geringerem Aufwand ein geeignetes Prognosemodell zu entwickeln.“
Für metallische Werkstoffe und Polymere verläuft die Entwicklung von Prognosemodellen mit Zeit-Temperatur-Korrelation seit ca. 1940 parallel und unabhängig voneinander. In diesem Zusammenhang bekannte Methoden sind das Zeit-Temperatur-Superpositionsprinzip und Zeit-Temperatur-Parameter, wie der LARSON-MILLER-Parameter. Die jeweiligen methodischen Ansätze sind in der Regel anwendungs- und materialspezifisch und nur einzelnen Fachartikeln zu entnehmen. Eine zusammenführende thematische Übersicht und Untersuchung existierender Methoden wurden bislang nicht publiziert. Diese Forschungsarbeit verfolgt dahingehend einen neuartigen methodischen Ansatz und zeigt untersuchte Gemeinsamkeiten und Unterschiede als auch Analogien für das Zeit-Temperatur-Superpositionsprinzip und Zeit-Temperatur-Parameter anhand bestimmter Merkmale auf. Dafür wurden verschiedene analytische und grafische Ansätze verwendet. Ferner wird eine zusammenführende Untersuchung anhand eines rheologischen Materialmodells sowie anhand eines praktischen Anwendungsbeispiels gezeigt. Hergeleitet wurde u. a., dass das Prinzip der Zeit-Temperatur-Superposition für sogenanntes thermorheologisch einfaches und komplexes Verhalten konkreten Zeit-Temperatur-Parametern zugeordnet werden können. Und dadurch Verschiebefunktionen nicht nur in Abhängigkeit der Temperatur, sondern auch abhängig vom Zustand untersucht und definiert werden können. Ferner ermöglicht eine Skalierung der Zeit-Temperatur-Parameter auf eine Referenztemperatur physikalisch anschaulichere Auswertungen analog zum Zeit-Temperatur-Superpositionsprinzip. Untersuchungen zeigen, dass sich für einen konkreten Anwendungsfall die geeignetste Zeit-Temperatur-Äquivalenz-Methode aus einer gegenseitigen Abhängigkeit bzw. Kompatibilität einzelner Elemente, wie zugrunde gelegte Daten, Koordinatenachsenskalierung, ermittelte Zeit-Temperatur-Äquivalenz, Masterfunktionsansatz und der geforderten Interpolationsgüte herleitet.
Der gewählte Forschungsansatz und die erzielten Ergebnisse bieten eine Plattform für die weitere Entwicklung von Prognosemodellen auf Basis des Zeit-Temperatur-Äquivalenz-Prinzips, insbesondere im Hinblick auf eine Zusammenführung und Kombination existierender Methoden.
In 2007 the license for the German Konrad repository for low and intermediate level radioactive waste was finally confirmed. Since then, the site is improved, prepared and equipped for the currently planned start of waste package emplacement in 2029. Bundesanstalt fuer Materialforschung und -pruefung is regularly contracted by the Bundesgesellschaft für Endlagerung as the responsible authority for waste product control, waste container design testing, and waste package acceptance. In this context BAM is mainly responsible for design testing of various container types including the evaluation of quality assurance measures for container manufacturing.
In addition to general requirements concerning container design, the casks have to withstand specific mechanical load scenarios. Drop tests from different heights under consideration of the most damaging drop orientation and a stacking test are two examples for necessary safety demonstrations.
If the containers are made from concrete the reinforcement has the function to absorb tensile forces the concrete is not able to withstand by its own. Because of manufacturing imperfections of cylindrical concrete containers manufactured already decades ago, the reinforcement cages are not always exactly, asymmetrically positioned when they were poured. This inspired BAM to perform various ABAQUS® finite-element (FE) simulations by using the example of a simplified cylindrical container design with generic dimensions. On the basis of the calculated tensile and compressive stress distributions suggestions are derived on how a cylindrical concrete container with an imperfectly placed reinforcement cage has to be oriented for a drop or stacking test to ensure the most damaging test scenario.