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For many sealing applications rubber O-rings are applied due to their special properties and easy use. In many applications as e.g. in aviation, traffic or process technology the material can be exposed to a variety of conditions during operation as e.g. low temperatures, elevated temperatures and different media. Therefore, it is important to know the material behaviour and the seal performance under those conditions. Additionally ageing of seals is an important factor which has an influence on the long term reliability.
In this contribution we would like to discuss different aspects affecting the seal performance, lifetime estimation and address open questions which should be addressed to come to a deeper understanding of these seals commonly understood as typical machine elements.
Results of running investigations at the Bundesanstalt für Materialforschung und -prüfung (BAM), Division 3.4 “Safety of Storage Containers” are presented and discussed.
Compared with the original time-temperature superposition (TTS) principle, an extended non-linear time-temperature equivalent (TTE) principle is suggested in this work. Results shown us, all application of TTS and most of the TTE parameters, for example, the Orr-Sherby-Dorn, Manson-Succop, Larson-Müller, Manson-Haferd, Mendelson-Roberts-Manson parameters and the more general ‘single metamodel’ from Haque–Stewart are special cases of the new suggested principle. The merits of this new method are discussed.
In this presentation, the history and actual situation of the German nuclear waste management policy of spent fuel (SF) and high-level waste (HLW) is reported. Beside the description of the restructuration of responsible authorities and organizations in Germany, the principle of dry interim storage of SF and HLW in dual purpose casks is explained. The need for extended interim storage towards disposal implicates additional challenges for the nuclear waste management strategy in Germany. (Extended)interim storage, subsequent transportation, and final disposal are closely linked. Integrated approaches concerning waste package designs and operations are supposed to be beneficial for the establishment of efficient long-term SF and HLW management strategies. Knowledge management and staff recruiting, education and training during phase out and beyond nuclear power plant operation are major issues.
At BAM, which is a federal institute for materials research and testing in Germany, it is one of our tasks to evaluate the safety of casks designed for transport and/or storage of radioactive material. This includes assessment of elastomeric seals applied in the casks. One of the aims is to identify a suitable method for estimating the service lifetime of the seals with regard to the requirements for long-term safety (40 years and more) of the containers. Therefore, we started an accelerated ageing programme with selected rubbers often used for seals (HNBR, EPDM and FKM) which are aged at four different temperatures (75 °C, 100 °C, 125 °C and 150 °C) for up to five years. In order to assess sealability, O-rings were aged in compression by 25 % (corresponding to the compression during service) between plates as well as in flanges that allow leakage rate measurements. For comparison, uncompressed O-rings were aged as well. In order to understand the underlying ageing mechanisms in each material, material properties such as hardness, density and tensile properties were examined. Additionally, compression set (CS), which represents the recovery behaviour of a seal after release from compression, is measured. For obtaining results closely related to practical conditions, O-rings with a full-scale cord diameter of 10 mm were aged. However, this set-up can lead to heterogeneous ageing caused by diffusion-limited oxidation (DLO) effects especially for HNBR, resulting in distorted bulk properties such as compression set. However, if DLO-affected data is excluded, extrapolations of CS data are possible using time-temperature shifts.
For selecting an appropriate end-of-lifetime criterion, leakage rate measurements were performed, since leakage rate is the only characteristic directly correlated to the performance of the sealing system. A significant increase in leakage rate was considered as the end of the lifetime. However, the O-rings remained leak tight under static conditions even though material properties had already degraded strongly. For this reason, a modified, more demanding leakage test involving a fast small decompression of the seal was developed that allowed determining a more conservative end-of-lifetime criterion with a safety margin for EPDM seals. FKM, which is a very heat and oxidation resistant material, exhibited only little degradation, even though it had the smallest activation energy.
The long-term sealing behavior of metal seals, assembled in the lid system of casks for transportation and storage of radioactive materials, has been investigated. For that purpose, phenomenological models describing the time- and temperature dependent behavior have been introduced by BAM since 2016, e.g. by using the time-temperature superposition principle. Results have shown that these models describe the relaxation behavior adequately and are suitable for extrapolations. In this work, the applicability of these models is checked by analyzing the necessary scope of tests, which must be carried out to get sufficient information about the long-term behavior of metal seals based on short-term tests.
In order to demonstrate the safety of both spent fuel and the storage system, a good understanding of the processes that might cause deterioration is required. The International Atomic Energy Agency (IAEA) continued the coordinated research on Spent Fuel Performance Assessment and Research (SPAR) into a fourth phase starting in 2015 to evaluate fuel and materials performance under wet and dry storage and to assess the impact of interim storage on associated spent fuel management activities (such as handling and transport). BAM’s understanding and experiences in the field of long-term storage of spent fuel and especially spent fuel characterization are presented to assist the preparation of the final project report.
The current research project BRUZL (Fracture mechanical analysis of spent fuel claddings during long-term dry interim storage) is presented. General aim of the project is the development of methods for risk assessment and identification of boundary conditions to prevent potential sudden brittle failure of spent fuel claddings at small deformation during long-term dry interim storage and subsequent transportation. The project is funded by the Federal Ministry for Economic Affairs and Energy (BMWi) under contract no. 1501561.
The evaluation of cladding integrity is a major issue to be demonstrated in Germany for extended interim storage periods up to 100 years and subsequent transportation considering operational and accidental conditions with respect to reactor operation, cask drying and dry interim storage. The chemical reaction between the zirconium fuel cladding and the cooling water in water-cooled reactors produces hydrogen and zirconium oxide. Hydrogen diffuses into the cladding and precipitates as zirconium hydrides when the solubility limit is reached, preferably oriented in hoop direction. At high temperatures during vacuum drying procedures, the hydrides can dissolve. Over a succeeding period of slow cooling with existing hoop stress the hydrides precipitate again, but partly reoriented along the radial direction of the cladding. This change of microstructure in combination with a decreasing temperature (0.5...2 K/year) during (extended) interim storage and additional mechanical load by handling procedures or under accident conditions could lead to a potential cladding embrittlement and consequently increased failure probability. The current research project BRUZL (Fracture mechanical analysis of spent fuel claddings under long-term dry interim storage conditions) has been launched by BAM to investigate potential sudden brittle failure of spent fuel claddings at small deformation under long-term dry interim storage conditions and is presented.
The evaluation of cladding integrity is a major issue to be demonstrated in Germany for extended interim storage periods up to 100 years and subsequent transportation considering operational and accidental conditions with respect to reactor operation, cask drying and dry interim storage. The chemical reaction between the zirconium fuel cladding and the cooling water in water-cooled reactors produces hydrogen and zirconium oxide. Hydrogen diffuses into the cladding and precipitates as zirconium hydrides when the solubility limit is reached, preferably oriented in hoop direction. At high temperatures during vacuum drying procedures, the hydrides can dissolve. Over a succeeding period of slow cooling with existing hoop stress the hydrides precipitate again, but partly reoriented along the radial direction of the cladding. This change of microstructure in combination with a decreasing temperature (0.5...2 K/year) during (extended) interim storage and additional mechanical load by handling procedures or under accident conditions could lead to a potential cladding embrittlement and consequently increased failure probability. The current research project BRUZL (Fracture mechanical analysis of spent fuel claddings under long-term dry interim storage conditions) has been launched by BAM to investigate potential sudden brittle failure of spent fuel claddings at small deformation under long-term dry interim storage conditions and is presented.
Elastomeric O-ring seals are used in a wide range of applications due to their excellent elasticity. However, like all polymers, elastomers degrade under the influence of e.g. time, temperature, oxygen, radiation and mechanical stress. Especially in applications where a replacement of seals after a certain time is hard or almost impossible, it is important to know the seal lifetime. Therefore, an extensive ageing programme with elastomers made of EPDM, HNBR and other materials was started with the aim of determining suitable methods for accelerated ageing and lifetime prediction.
In order to determine the lifetime of polymeric parts, the time-temperature superposition principle is commonly used to shift property changes obtained by accelerated ageing at higher temperatures to lower temperatures. If the shift factors yield a straight line in an Arrhenius diagram, a corresponding activation energy can be determined. However, we have found that the shift factors and thus the predicted lifetime depends on the test method that yielded the shifted data. For example, the shift factor between 125 °C and 150 °C ageing temperature was roughly the same (5/5/4.5 respectively) for hardness, density and maximum of loss factor tan measured on HNBR, but different for elongation at break (8) and compression set (2.2, excluding DLO-affected data). A possible explanation might be that while the different oxidation reactions proceed with a fixed activation energy, they have differing impact on the measured properties. For example, hardness is lowered by chain scission reactions, and increases by crosslinking reactions during ageing. As usually both chain scission and crosslinking reactions occur during ageing, the measured hardness increase reflects only the net effect of both reaction types. On the other hand, compression set is influenced additively by both reaction types: chain scission leads to an increase of the remaining deformation, as broken chains lose their recovery potential, and crosslinking reactions during ageing fix the compressed geometry, which also leads to less recovery. Thus, compression set reflects the total number of changes in the network and shows degradation effects much faster, which results in lower shift factors and lower activation energy. This phenomenon was observed for EPDM as well.
In order to verify our hypotheses and to gain further insights, temperature-dependent oxygen consumption measurements are currently being performed and results will be presented at the conference. The shift factors and activation energy determined by oxygen consumption measurements are expected to be close to the values for compression set.
This publication summarizes the work carried out during an IAEA coordinated research project (CRP) on safe and reliabe management of spent nuclear fuel. This work contributes to the overall goal of demonstrating the performance of spent nuclear fuel and related storage systems components over long durations, and facilitates the transfer of this knowledge to Member States. The technical areas addressed by the CRP participants were related to potential degradation mechanisms in metal casks and concrete overpacks, such as stress corrosion cracking; long term integrity and performance of the fuel cladding; thermo-mechanical behaviour of the metal seals; and long term gamma and neutron shielding capability. The participants also considered past and ongoing demonstration programmes. For each technical topic addressed the main conclusions have been drawn, including information on the development of specific monitoring and inspection techniques as well as future opportunities for closing relevant data gaps. A major achievement is also the establishment of a worldwide network of experts working on current research projects to demonstrate the long term performance of spent fuel in dry storage systems.
Due to their high versatility and recovery potential under several load conditions, seals made from elastomers are widely used as barrier seals in containers for low and intermediate level radioactive waste and as auxiliary seals in spent fuel storage and transportation casks (dual purpose casks (DPC)). In DPC, elastomer seals allow leakage rate measurements of metal barrier seals for demonstration of their proper assembly conditions and performance.
For spent fuel and high level waste as well as for low and intermediate level waste, long time periods will be required before final disposal will be available. Therefore, the long-term behavior of elastomer seals can be an important issue when the cask’s suitability for an extended interim storage period has to be assessed.
During the licensed interim storage duration, the requested leakage rate has to be maintained under any static and dynamic load conditions. A sufficient resilience, the capability of seals to compensate a (rapid) partial release was identified as an important end-of-lifetime criterion.
In the framework of extensive aging and testing programs at BAM, specimen made from representative types of elastomer (EPDM, FKM) were aged for several years at different temperatures ranging from 23 °C to 150 °C. One aim of the experiments was to determine an end-of-lifetime criterion correlated to leakage as the point of seal failure. As the seals remained leak-tight under static conditions even after advanced material degradation, a more demanding leakage test set-up was constructed that allowed a rapid partial release of the seal. This device enables a release of the O-ring by approx. 0.2 mm from 25 % to 23 % compression in less than one second during the pressure rise measurement. If the resilience of the seal has decreased past a certain point, the seal cannot follow the decompression fast enough and a leak path can open. Using a finite element (FE) material model derived earlier from different material tests, this process was simulated with a 3D FE model, reproducing the essential characteristics of the test device.
The FE-model enables the analyzation of the occurring global mechanisms if a leak path opens. The capability of the seals to follow the lifted flange and the subsequent run of compression force depending on the current state of aging are illustrated. The findings of the simulation are correlated and discussed with respect to the pressure rise measurements.
Elastomere werden vielfach in Produkten eingesetzt, die bei verschiedenen Temperaturen verwendet werden. O-Ringe sind kostengünstige Dichtelemente, die allerdings für die Funktionsfähigkeit und Sicherheit eines Produkts entscheidend sein können. Die untere Temperatur-einsatzgrenze ist dabei relevant und aus wissenschaftlicher Sicht nicht allgemein gültig zu definieren, da diese einerseits durch die Änderungen der Materialeigenschaften im Zuge des Gummi-Glas-Übergangs definiert werden, die Temperaturlage dieses Übergangs jedoch sehr stark von den jeweiligen Einsatzbedingungen (z.B. Frequenz) abhängt. Dadurch ergeben sich große Unterschiede zwischen statischen und dynamischen Anwendungen.
Verschieden Untersuchungen sollen vorgestellt und interpretiert werden, um das Auditorium auf verschiedene Herausforderungen aufmerksam zu machen und Lösungsansätze vorzustellen.
Embrittlement of spent fuel claddings during long-term dry interim storage - Current approach at BAM
(2019)
The integrity of fuel rods and cladding tubes must be demonstrated throughout the dry interim storage of spent nuclear fuel in Germany. For at least a relevant number of casks, an extension of interim storage between 40 and 100 years is foreseeable. The drying procedure for the fuel rods in conjunction with the thermomechanical storage conditions may change the microstructure of the cladding tubes and lead to their possible embrittlement. The failure probability might increase under mechanical load by handling procedures (transport after storage) on potentially embrittled cladding tubes of fuel rods especially at low temperatures after long-term storage. Results of ring compression tests on unirradiated pre-hydrided as well as irradiated samples with radial hydrides are investigated by finite element analyses to be able to describe the failure process and to identify failure criteria.
Embrittlement of spent fuel claddings during long-term dry interim storage - Current approach at BAM
(2019)
In this presentation, the actual situation of long-term dry interim storage of spent nuclear fuel in Germany is reported. An extension of the interim storage period between 40 and 100 years for at least a relevant number of casks is foreseeable. To demonstrate the integrity of fuel rods and cladding tubes throughout the extended dry interim storage, a potential cladding embrittlement should be investigated. The current approach at BAM is a research project on experimental and numerical investigations of sudden failure of unirradiated pre-hydrided cladding tubes after hydride reorientation at small deformation under Ring Compression Test conditions. A fracture mechanics based failure analysis and suggested failure criteria for a potential brittle failure of spent fuel claddings after long-term dry interim storage under mechanical loads are discussed.
The European Joint Programme on Radioactive Waste Management (EURAD) has been launched to coordinate activities on agreed priorities of common interest between European partners. The main actions include scientific and technical activities on radioactive waste characterization and processing, interim storage of radioactive waste as well as predisposal and disposal solutions. As part of the programme, the work package on Spent Fuel Characterization and Evolution until Disposal (SFC) was proposed and accepted by the European Commission. The objectives of this work package include the development of beyond-state-of-the-art characterization techniques for spent nuclear fuel during its evolution from reactor unloading until disposal, the understanding of the spent fuel performance during prolonged storage, transport and emplacement in a deep geological repository, the understanding of the behaviour of fuel, cladding, pellet-cladding interaction and ageing effect under normal and postulated accident scenarios until disposal, and contributions to operational safety concepts for fuel handling at spent nuclear fuel packaging facilities.
The safety evaluation of cask components made of ductile cast iron includes investigations to prevent brittle fracture. Generally, ductile cast iron is endangered by brittle fracture especially at low temperatures (down to -40°C) and in combination with existing crack-like material defects. An applicable method is the assessment of fracture resistance using fracture mechanics according to the IAEA guidelines. The approach is based on the prevention of fracture initiation. For application of these principles for drop loads, account must be taken both of dynamic stresses within the component and dynamic material behavior. Basically, the dynamic stress intensity factor of postulated pre-existing crack-like defects is compared with the dynamic fracture toughness of the material. Applicable numerical and experimental methods for the safety assessment of cask components are demonstrated for the case of an artificially pre-cracked cylindrical cast iron cask which undergoes dynamic loading conditions as result of the hard impact between the cask and a concrete target. The proposed evaluation procedure is a combination of numerical and experimental steps. Exemplarily, the calculated stress intensity factor is compared with measured fracture toughness values from single edge notched bending specimens.
The safety evaluation of cask components made of ductile cast iron includes investigations to prevent brittle fracture. Generally, ductile cast iron is endangered by brittle fracture especially at low temperatures (down to -40°C) and in combination with existing crack-like material defects. An applicable method is the assessment of fracture resistance using fracture mechanics according to the IAEA guidelines. The approach is based on the prevention of fracture initiation. For application of these principles for drop loads, account must be taken both of dynamic stresses within the component and dynamic material behavior. Basically, the dynamic stress intensity factor of postulated pre-existing crack-like defects is compared with the dynamic fracture toughness of the material. Applicable numerical and experimental methods for the safety assessment of cask components are demonstrated for the case of an artificially pre-cracked cylindrical cast iron cask which undergoes dynamic loading conditions as result of the hard impact between the cask and a concrete target. The proposed evaluation procedure is a combination of numerical and experimental steps. Exemplarily, the calculated stress intensity factor is compared with measured fracture toughness values from single edge notched bending specimens.