TY - JOUR A1 - Kömmling, Anja A1 - Chatzigiannakis, E. A1 - Beckmann, Jörg A1 - Wachtendorf, Volker A1 - von der Ehe, Kerstin A1 - Braun, Ulrike A1 - Jaunich, Matthias A1 - Schade, U. A1 - Wolff, Dietmar T1 - Discoloration Effects of High-Dose gamma-Irradiation and Long-Term Thermal Aging of (U) HMW-PE N2 - Two polyethylene types with ultra-high (UHMWPE) and high molecular weight (HMW-PE) used as neutron radiation shielding materials in casks for radioactive waste were irradiated with doses up to 600 kGy using a 60Co gammasource. Subsequently, thermal aging at 125∘C was applied for up to one year. Degradation effects in the materials were characterized using colorimetry, UV-Visspectroscopy, IR spectroscopy, and DSC. Both materials exhibited a yellowing upon irradiation.The discoloration of UHMW-PE disappeared again after thermal aging.Therefore, the yellowing is assumed to originate fromannealable color centers in the formof free radicals that are trapped in the crystalline regions of the polymer and recombine at elevated temperatures. For the antioxidantcontaining HMWPE, yellowing was observed after both irradiation and thermal aging. The color change was correlated mainly to decomposition products of the antioxidant in addition to trapped radicals as in UHMW-PE. Additionally, black spots appeared after thermal aging of HMW-PE. KW - Irradiation KW - UHMWPE KW - Colour center KW - Yellowness index PY - 2017 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-423992 DO - https://doi.org/10.1155/2017/1362491 SN - 1687-9422 VL - 2017 IS - Article ID 1362491 SP - 1 EP - 10 PB - Hindawi AN - OPUS4-42399 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Jaunich, Matthias A1 - Kömmling, Anja A1 - Böhning, Martin A1 - Silbernagl, Dorothee T1 - Comparison of ageing behavior of O-ring seals under hydrogen and air N2 - Elastomeric seals are essential components in the infrastructure which prevent leakage of gas and ensure proper function of technical devices and are therefore highly safety relevant. For proper function a remaining resilience and tolerance to pressure changes is required. The ageing of elastomers is an undesirable but inevitable process leading to a limited lifetime of rubber products such as seals. Independent of the application, as e.g. automotive, piping or container applications, a long lifetime or at least a timely exchange of a seal before occurrence of critical failure is desired. Hydrogen is a key element for the energy turnaround and therefore the compatibility of seals with hydrogen is essential. In addition to the effect of hydrogen uptake and release, which might also cause destructive effects such as rapid gas decompression, ageing at high temperature under hydrogen atmosphere is of interest too. Most of the existing work is addressing the performance of new materials and comprises only very limited investigations concerning long-term use and the behaviour of aged materials in contact with hydrogen. As ageing can lead to substantial changes of material properties, it must be evaluated whether these changes are beneficial or deteriorating for the component function. In this work we present and compare results of the characterization of three sealing materials (EPDM, HNBR, FKM) after ageing at high temperature under hydrogen and air. Despite the common assumption that ageing under hydrogen atmosphere should be less severe for the material in comparison to air ageing, this is not the case for every material. T2 - ASME PVP2025, Pressure Vessels & Piping Conference CY - Montreal, Quebec, Canada DA - 20.07.2025 KW - Aging KW - Seal KW - Compression set KW - Atomic force microscopy PY - 2025 SP - 1 EP - 7 AN - OPUS4-63889 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Kömmling, Anja A1 - Simbruner, Kai A1 - Grelle, Tobias A1 - Jaunich, Matthias A1 - Zencker, Uwe A1 - Wolff, Dietmar A1 - Orellana Pérez, Teresa A1 - Völzke, Holger T1 - Research at BAM for evaluating long term safety of container systems and components N2 - Safety of long term containment and storage of radioactive waste is an essential issue, which is increasingly gaining international attention. Extending interim storage beyond initial license periods is one of the major challenges worldwide. BAM has been involved in all kinds of radioactive waste container safety evaluation for storage and transportation including their long term performance from the very beginning. Today, all work related to the safe management of radioactive waste is linked by the activity field “Nuclear Waste Management” within the Focus Area “Energy” at BAM and in conjunction with a research strategy and agenda. Most recently, the working group “Long Term Safety of Container Systems and Components” was established to launch and perform research projects related to safety issues concerning the extended interim storage of radioactive waste. For example, within our project LaMEP, we investigate ageing effects of metal and elastomer seals as well as polymeric neutron shielding materials, which are container components that fulfil major safety functions. The results of the experiments help to understand the long term behaviour of these components. Likewise, our project BRUZL started at BAM in 2018 with the aim of developing a fracture mechanics approach to understand and describe a potential brittle failure mechanism of fuel cladding during long-term interim storage. BAM also contributes to the GRS project “Development of methods and models and international exchange for safety evaluation in the frame of interim storage of radioactive waste”. Additionally, BAM is involved in several international research programmes dealing with extended interim storage, such as the European Joint Programme on Radioactive Waste Management (EURAD), the Extended Storage Collaboration Program (ESCP) and IAEA Coordinated Research Projects. The present contribution provides a comprehensive overview of BAM research activities contributing to national and international gap analyses and to filling knowledge gaps regarding the safe long term management of radioactive waste. T2 - Annual Meeting on Nuclear Technology 2019 CY - Berlin, Germany DA - 07.05.2019 KW - Radioactive Waste KW - Long-term safety PY - 2019 SN - 978-3-926956-95-8 SP - 1 EP - 5 AN - OPUS4-51486 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Characterisation of degradation and determination of end-of-lifetime criterion for O-ring seals N2 - The ageing of polymers, including elastomers, is an undesirable but inevitable process leading to a limited lifetime of rubber products such as seals. Independent of the application, as e.g. in automotive, piping or container applications, a long lifetime or at least a timely exchange of a seal before occurrence of critical failure is desired. In order to investigate the degradation of material properties and to determine the lifetime of elastomers used as seals, an ageing programme was started with hydrogenated acrylonitrile butadiene rubber (HNBR), ethylene propylene diene rubber (EPDM) and fluorocarbon rubber (FKM) [1-3]. Both O-ring seals (uncompressed and compressed by 25 %) with a cord diameter of 10 mm as well as sheets with a thickness of 2 mm were aged at 75 °C, 100 °C, 125 °C and 150 °C for up to two years. The changes of material properties during ageing were characterised for each material using samples from the sheets by means of e.g. Dynamic Mechanical Analysis and tensile tests, while sealing properties such as leakage rate were determined on O-rings. The experimental results indicate that while material properties show considerable degradation effects, the static leakage rate stays constant or even decreases before failure occurs quite suddenly at advanced degradation levels. This reveals that static leakage rate has only limited sensitivity for the degradation of the seal material. Our approach to determine a suitable end of lifetime criterion, which involves a partial decompression of the seal during the leakage test, is presented and discussed. T2 - RubberCon 2017 CY - Prague, Czech Republic DA - 23.05.2017 KW - Life time prediction KW - Ageing KW - Rubber seal KW - Leakage PY - 2017 SN - 978-80-906662-0-7 SP - 65 EP - 72 AN - OPUS4-40391 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CHAP A1 - Kömmling, Anja A1 - Wolff, Dietmar A1 - Jaunich, Matthias ED - van Breugel, K. ED - Koleva, D. ED - Beek, T. T1 - Investigation of long-term behaviour of elastomeric seals for transport and storage packages N2 - Elastomers are widely used as the main sealing materials in Containers for low- and intermediate-level radioactive waste and as an additional component fo metal seals in spent-fuel and high-level waste containers. According to appropriate guidelines and regulations, safe enclosure of the radioactive container contents has to be guaranteed for lengthy storage periods of at least 40 years. Therefore, the understanding of seal ageing behaviour is of high importance and has to be considered with regard to possible dynamic events taking place during transport after storage. An accelerated ageing approach for compressed seals is presented, as well as some first results. KW - O Ring KW - Ageing KW - Rubber seal PY - 2018 SN - 978-3-319-70192-9 DO - https://doi.org/10.1007/978-3-319-70194-3_2 SP - 17 EP - 25 PB - Springer AN - OPUS4-43248 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Weber, Mike A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar A1 - Zencker, Uwe A1 - Völzke, Holger A1 - Schulze, Dietmar A1 - Probst, Ulrich T1 - Testing and Numerical Simulation of Elastomers - From Specimen Tests to Simulation of Seal Behavior under Assembly Conditions N2 - Due to delays in the siting procedure to establish a deep geological repository for spent nuclear fuel and high level radioactive waste as well as in construction of the already licensed Konrad repository for low and intermediate level radioactive waste, extended periods of interim storage become more relevant in Germany. BAM is involved in most of the cask licensing procedures and especially responsible for the evaluation of cask-related long-term safety issues. The long-term performance of elastomer seals for lid systems of transport and storage casks, whether used as auxiliary seals in spent fuel casks or as primary seals for low and intermediate level waste packages, is an important issue in this context. The polymeric structure of these seals causes a complex mechanical behavior with time-dependent sealing force reduction. The results of a comprehensive purpose-designed test program consisting of basic compression and tension tests as well as relaxation tests on unaged specimens of representative types of elastomers (fluorocarbon rubber (FKM) and ethylene propylene diene rubber (EPDM)) at different temperatures and strain rates are presented. They were used to identify the constitutive behavior and to obtain parameters for finite element material models provided by the computer code ABAQUS®. After estimating the influence of uncertainties such as Poisson’s ratio and friction coefficient by sensitivity analyses, the chosen parameters had to prove their suitability for the finite element simulation of the specimen tests themselves. Based on this preliminary work the simulation of a specific laboratory test configuration containing a typical elastomer seal with circular cross section is presented. The chosen finite element material model and the implemented parameters had to show that they are able to represent not only the specimen behavior under predominantly uniaxial load but also the more complex stress states in real components. Deviations between the measured and calculated results are pointed out and discussed. For the consideration of long-term effects in the simulation of elastomer behavior, test results of aged specimens are needed. First information about a new test program, started recently and planned to provide these data, are given. T2 - ASME 2017 Pressure Vessels & Piping Conference (PVP2017) CY - Waikoloa, Hawaii, USA DA - 16.07.2017 KW - Time dependent effects KW - Low temperature behavior KW - Elastomeric seals KW - Aging KW - Simulation KW - Testing PY - 2017 SN - 978-0-7918-5802-8 VL - 7 SP - Article UNSP V007T07A035, 1 EP - 8 AN - OPUS4-41841 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Weber, Mike A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar A1 - Zencker, Uwe A1 - Völzke, Holger A1 - Schulze, Dietmar T1 - Testing and numerical simulation of elastomeric seals under consideration of time dependent effects N2 - Due to delays in the siting procedure to establish a deep geological repository for spent nuclear fuel and high level waste and in construction of the already licensed Konrad repository for low and intermediate level waste, extended periods of interim storage will become more relevant in Germany. BAM is involved in most of the cask licensing procedures and is responsible for the evaluation of cask-related long-term safety issues. Elastomeric seals are widely used as barrier seals for containers for low and intermediate level radioactive waste. In addition they are also used as auxiliary seals in spent fuel storage and transportation casks (dual purpose casks (DPC)). To address the complex requirements resulting from the described applications, BAM has initiated several test programs for investigating the behavior of elastomeric seals. These include experiments concerning the hyperelastic and viscoelastic behavior at different temperatures and strain rates, the low temperature performance down to -40°C, the influence of gamma irradiation and the aging behavior. The first part of the paper gives an overview of these tests, their relevant results and their possible impact on BAM’s work as a consultant in the framework of approval and licensing procedures. The second part presents an approach of the development of a finite element model using the finite element code ABAQUS®. The long-term goal is to simulate the complex elastomeric behavior in a complete lid closure system under specific operation and accident conditions. T2 - ASME 2016 Pressure Vessels & Piping Conference (PVP2016) CY - Vancouver, BC, Canada DA - 17.07.2016 KW - Elastomeric seals KW - Testing KW - Low temperature behavior KW - Aging KW - Simulation KW - Time dependent effects PY - 2016 SN - 978-0-7918-5045-9 VL - 7 SP - Paper 63192, 1 EP - 10 AN - OPUS4-37046 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Zaghdoudi, M. A1 - Kömmling, Anja A1 - Böhning, Martin A1 - Jaunich, Matthias T1 - Ageing of elastomers in air and in hydrogen environment - A comparative study N2 - EPDM, HNBR and FKM materials were exposed at 150 ◦C to air under atmospheric pressure and to hydrogen at 50 bar for different ageing times. All measurements after hydrogen exposure were conducted on samples in degassed condition to assess irreversible effects resulting from that exposure and to compare them to those after ageing in air. Density, hardness, tensile properties, compression set, and hydrogen permeability of all samples were analysed. In both ageing environments, HNBR exhibited the most significant changes of material properties. However, for both EPDM and HNBR, considerably less severe ageing effects were observed under hydrogen in comparison to ageing in air. On the other hand, FKM showed about the same low level of deterioration in both ageing environments but exhibited poor resistance against damage due to rapid gas decompression in hydrogen environment that can lead to seal failure. The obtained results may serve as a guidance toward a better understanding for design and utilisation of elastomeric materials in future hydrogen infrastructure components. KW - Rapid gas decompression KW - Condensed matter physics KW - Hydrogen KW - Sustainability and the environment KW - Rubber sealing KW - Renewable energy PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-597417 DO - https://doi.org/10.1016/j.ijhydene.2024.03.053 SN - 0360-3199 SN - 1879-3487 VL - 63 SP - 207 EP - 216 PB - Elsevier CY - Oxford AN - OPUS4-59741 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Zaghdoudi, Maha A1 - Weber, Mike A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Numerical Modelling of Compression Stress Relaxation and Compression Set of Elastomer O-Ring During Aging N2 - Elastomer seals are used in many industrial applications due to their excellent mechanical properties at a wide range of temperatures. Their high versatility and recovery potential under several load conditions make them well suitable for the application in containers designed for transport, storage and/or disposal of radioactive materials. In containers for low and intermediate level radioactive waste, elastomer seals are used as barrier seals, and as auxiliary seals in storage and transportation casks (dual purpose casks) for heat generating radioactive waste, such as spent fuel and high-level waste. While a seal exchange at defined intervals is typical in many conventional applications, it is impossible or at least hard to perform when principles of minimization of radiation exposure have to be considered and prohibit an unnecessary cask handling. An extensive knowledge of the change of the elastomer’s properties during aging and the availability of reliable end-of-lifetime criteria to guarantee the permanent safe enclosure of the radioactive material is mandatory. As BAM is involved in most of the national cask licensing procedures and in the evaluation of cask-related long-term safety issues, great efforts have been already made and are still planned to scientifically support this task. Compression stress relaxation and compression set were identified as key indicators of elastomer long-term performance and quantitatively investigated in comprehensive test programs. Among other representative types of elastomers, specimens made from ethylene propylene diene rubber (EPDM) were tested before, during and after aging to capture the most important of their complex mechanical properties. In the presented study, exemplary results were used to simulate the compression stress relaxation and the compression set of elastomer O-rings during aging. Regarding the influence of temperature, the time-temperature superposition principle is applied in the relaxation analysis of elastomer O-rings. The proposed model is implemented in the commercial finite element software ABAQUS/Standard® [1] with a sequential temperature displacement coupling. Numerical results match the experimental compression stress relaxation measurements well. The prediction of compression set values after long-term aging shows a relatively good agreement with the experimental results. Nevertheless, all input parameters derived from the specimen tests, additional assumptions concerning boundary conditions and modeling strategy are discussed with regard to the identified slight discrepancies. The possibility to extend the finite element model to represent the O-ring seal’s ability to recover after a (fast) partial release is taken into account. T2 - ASME 2020 Pressure Vessels & Piping Conference (PVP2020) CY - Online meeting DA - 03.08.2020 KW - Compression Set KW - O-ring KW - Simulation KW - Sequential analysis KW - Ageing KW - stress relaxation PY - 2020 SN - 978-0-7918-8388-4 DO - https://doi.org/10.1115/PVP2020-21270 SP - PVP2020-21270 PB - ASME AN - OPUS4-51490 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - GEN A1 - Zaghdoudi, M. A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar ED - Altenbach, H. ED - Hitzler, L. ED - Johlitz, M. ED - Merkel, M. ED - Öchsner, A. T1 - Analysis of Heterogeneous Ageing of HNBR O-Rings N2 - Abstract Hydrogenated nitrile butadiene rubber (HNBR) elastomer was thermo-oxidatively aged at different temperatures up to 150 °C. Fourier transform infrared spectroscopy (FTIR), compression stress relaxation (CSR) and international rubber hardness degree (IRHD) microhardness were used to characterise the chemo-mechanical changes of HNBR O-rings during thermo-oxidative ageing. FTIR shows the development of carbonyl, methyl and ester groups but the nitrile content was not affected by ageing. The effect of sample geometry during CSR was investigated. CSR data were converted through integrated kinetic laws. The conversion has proven its sensibility to detect heterogeneous ageing. This was confirmed by the IRHD measure-ments across the section of O-rings. The influence of compression during ageing was assessed through IRHD measurements across the section of compressed and uncom-pressed aged O-rings. The DLO effect was more pronounced in compressed O-rings. By applying the model of Wise et al., theoretical IRHD and oxidation profiles were determined on the basis of IRHD experimental data of compressed O-rings. Good agreements between the experimental and the theoretical IRHD profiles in the core region were obtained. However, near the edge, the theoretical IRHD values were overestimated. KW - Ageing KW - Rubber seals KW - Stress relaxation KW - Modelling PY - 2024 SN - 978-3-031-49042-2 DO - https://doi.org/10.1007/978-3-031-49043-9 SN - 1869-8433 SP - 331 EP - 348 PB - Springer Nature CY - Cham, Switzerland AN - OPUS4-59769 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Jaunich, Matthias A1 - Weber, Mike A1 - Kömmling, Anja A1 - Zencker, Uwe A1 - Wolff, Dietmar A1 - Völzke, Holger T1 - Performance of elastomer seals in transport and storage casks N2 - Elastomer seals are widely used as barrier seals in containers for low and intermediate level radioactive waste and for spent fuel transportation casks. In addition, they are also used for spent fuel storage and transportation casks (dual purpose casks (DPC)) as auxiliary seals to allow leakage rate measurements of metal barrier seals for demonstration of their proper assembling conditions. Depending on the area of use, the rubber materials have to demonstrate proper sealing performance with regard to mechanical, thermal, and environmental conditions as well as irradiation during the entire operation period. Concerning DPC, degradation effects should be limited in a way that, for example, effects from potentially released decomposition elements may not harm e.g. metal barrier seals. Leakage rate measurements should be possible also after long interim storage periods prior to subsequent transportation. Because of the complex requirements resulting from the various applications of containers for radioactive waste and spent nuclear fuel, BAM has initiated several test programmes for investigating the behaviour of elastomer seals. In this contribution the current status is described and first results are discussed. T2 - International conference on management of spent fuel from nuclear power reactors: An integrated approach to the back end of the fuel cycle CY - Vienna, Austria DA - 15.06.2015 KW - Ageing KW - Elastomer KW - Glass-rubber transition KW - Irradiation KW - Material model PY - 2015 SP - 1 EP - 8 AN - OPUS4-33553 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Ageing and lifetime prediction of O-ring seals made of HNBR, EPDM and FKM N2 - BAM is the federal institute for materials research and testing in Germany. One of our tasks is to evaluate the safety of casks designed for transport and/or storage of radioactive waste. As elastomeric seals are used in the containers as safety-relevant parts, it is our goal to be able to evaluate the service lifetime of the seals with regard to the requirements for long-term safety (40 years and more) of the containers. For this reason, an accelerated ageing programme with selected rubbers often used for seals (HNBR, EPDM and FKM) was started. Ageing was performed at four different temperatures (75 °C, 100 °C, 125 °C and 150 °C) for up to 2 years. For assessing properties related to the sealability, O-rings were aged in compression by 25 % (corresponding to the compression during service) between plates. For comparison, uncompressed O-rings were aged as well. The aged materials were characterized with conventional polymer analysis methods such as hardness and tensile tests, but also with more seal-specific methods such as compression stress relaxation (CSR, reflecting the loss of sealing force of a compressed seal over time), and compression set (CS, representing the recovery behaviour of a seal after release from compression). CS is chosen as the property for lifetime prediction as it is both sensitive to degradation and related to the seal performance. CS data is extrapolated to 60 °C, which yields lifetimes of approximately 5 years for HNBR and 64 years for EPDM for a criterion of 85 % CS respectively, and approx. 40 years for FKM for a criterion of 65 % CS (the highest value measured so far). T2 - 12. Kautschuk Herbst Kolloquium CY - Hanover, Germany DA - 22.11.2016 KW - Rubber KW - Compression set KW - Extrapolation KW - Degradation PY - 2016 SN - 9783981407648 VL - 2016 AN - OPUS4-38483 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Zaghdoudi, Maha A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Understanding the recovery behaviour and the degradative processes of EPDM during ageing N2 - Recovery is an important measure for seal applications representing to which extent the elastomer regains its initial shape after deformation and release of an applied force. Compression set (CS) indicates the degree of recovery. Ethylene propylene diene rubber (EPDM) was aged at 75 ◦C, 100 ◦C, 125 ◦C and 150 ◦C for different ageing times up to five years and compression set measurements were performed at different times after disassembly and after additional tempering. Short- and long-term recovery up to one year after release for samples aged at 125 ◦C and 150 ◦C was also studied. To assess the curvature in the Arrhenius diagram that may occur due to non-sufficiently aged specimens, a degradation-rate based model was fitted to the CS data after tempering. For each ageing temperature, two decay fit functions were proposed, each with an activation energy and a corresponding degradative process. The influence of ageing on the leak-tightness after fast small partial release is investigated and estimated through the analysis of the shift factors from time temperature superposition (TTS) of CS measurements at different times after disassembly. Shift factors of CS measurement after 1 s and after additional tempering are in good agreement. KW - Compression set KW - Ageing KW - Recovery KW - Degradative processes KW - Leakage rate PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-573699 DO - https://doi.org/10.1016/j.polymertesting.2023.107987 SN - 0142-9418 VL - 121 SP - 107987 PB - Elsevier Ltd. AN - OPUS4-57369 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Zaghdoudi, Maha A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Oxidative ageing of elastomers: Experiment and modelling N2 - 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. KW - Compression stress relaxation KW - Compression set KW - IRHD microhardness KW - Modelling PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-545910 DO - https://doi.org/10.1007/s00161-022-01093-9 SN - 1432-0959 SP - 1 EP - 9 PB - Springer CY - Berlin AN - OPUS4-54591 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Kömmling, Anja T1 - Ageing of Elastomeric Seals for Storage Casks N2 - At BAM Federal Institute for Materials Research and Testing in Germany, it is our responsibility to audit the safety of casks designed for transport and/or storage of radioactive material. With regard to the requirements on long-term safety of the containers, it is necessary to evaluate the service lifetime of the elastomeric seals used in the containers. With ageing, the elastomers will gradually lose their elasticity and their ability for recovery, which might result in a leakage above the allowed level or in a release of radioactivity during an incident. It is important to know the rate of degradation and which property can be used as an practical and easily measurable end-of-lifetime criterion. For this reason, we devised ageing experiments on different kinds of elastomers, namely FKM, EPDM and HNBR. The former two are actually used in containers for radioactive wastes – either as auxiliary seal in casks containing high activity waste, or as main seal in casks for medium or low activity waste. The latter is an often used seal material that is tested for comparative reasons. In our ageing program, these three materials are aged at four different temperatures (75 °C, 100 °C, 125 °C and 150 °C) in order to extrapolate the data to service temperature using a suitable model. They are examined at logarithmic time intervals of several days up to 5 years. The samples are aged in their undeformed O-ring state as well as compressed between flanges with a deformation corresponding to the actual compression during service. Thus we can compare the ageing between relaxed and stressed sample. Additionally, we are ageing samples in flanges that allow leakage rate measurements. Other measurements include monitoring of the recovery force of the seal and the compression set. Furthermore, the samples are examined by thermal and dynamic-mechanical analysis for detecting changes in the glass transition temperature due to crosslinking or chain scission in the material. Besides, hardness is measured as a practical macroscopic indicator. Until now, we have analyzed samples aged up to 100 days. At the highest ageing temperature of 150 °C, the compressed EPDM has already reached a compression set of 95 %, while HNBR and FKM have reached 80 % and 30 %, respectively. Furthermore, HNBR has reached a Shore D hardness of 85, which is an immense increase after the initial value of 80 Shore A. However, when looking at the cross-section of the sample, it was obvious that only a layer of about 1 mm thickness has become so hard, while the inner part remained rubbery. This shows that there has been intense crosslinking mostly near the surface of the HNBR which forms a kind of oxygen diffusion barrier, inhibiting the thermooxidation of the inner part of sample which can retain elastic properties. In EPDM, the oxygen permeability is much greater, which leads to a more homogeneous degradation across the whole sample and thus resulted in a higher compression set. The low compression set of FKM shows the outstanding high-temperature properties of this material. T2 - Annual Meeting on Nuclear Technology 2015 CY - Berlin, Germany DA - 2015-05-05 PY - 2015 AN - OPUS4-33200 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - THES A1 - Kömmling, Anja T1 - Alterung und Lebensdauervorhersage von O-Ring-Dichtungen T1 - Aging and lifetime prediction of O-ring seals N2 - Für Anwendungen, bei denen Elastomerdichtungen ihre Dichtheit über sehr lange Zeiträume (z. B. Jahrzehnte) behalten müssen, ohne dass ein Austausch praktikabel wäre, ist es nötig, die Lebensdauer solcher Dichtungen zuverlässig bestimmen zu können. Aus diesem Grund wurden Alterungsversuche an O-Ring-Dichtungen sowie Flachproben auf Basis von hydriertem Acrylnitril-Butadien-Kautschuk (HNBR), Ethylen-Propylen-Dien-Kautschuk (EPDM) und Fluorkautschuk (FKM) über bis zu zwei Jahre bei mehreren Temperaturen durchgeführt. Zur Untersuchung der auftretenden Eigenschaftsveränderungen wurden u. a. Härtemessungen, Zugversuche, dynamisch-mechanische und thermogravimetrische Analysen durchgeführt. Zur Beurteilung des Relaxations- und Rückstellverhaltens der alternden Dichtungen wurden außerdem Druckspannungsrelaxations- und Druckverformungsrestmessungen durchgeführt. Darüber hinaus wurde die Leckagerate gemessen, um ein Versagen der Dichtung zu detektieren. Durch die Untersuchung der gealterten Proben wurden sowohl die auftretenden Eigenschaftsveränderungen charakterisiert wie auch die damit zusammenhängenden Alterungsmechanismen diskutiert. Anhand der großen Datenmenge aus Ergebnissen von verschiedenen Untersuchungsmethoden, die für mehrere Alterungszeiten und -temperaturen durchgeführt wurden, sollte zusätzlich die günstigste Vorgehensweise für Lebensdauervorhersagen ermittelt werden. Dies beinhaltete auch die Bestimmung eines Lebensdauerkriteriums, das mit dem Auftreten von Leckage und damit dem Versagen der Dichtung zusammenhängt. Hinsichtlich der Eigenschaftsänderungen und Alterungsmechanismen wurde beim HNBR eine starke Versprödung aufgrund dominanter Vernetzungsreaktionen während der Alterung festgestellt. Diese resultierten auch darin, dass die Sauerstoffpermeabilität abnahm, so dass der Sauerstofftransport ins Innere der Probe (hauptsächlich bei den dickeren O-Ringen) behindert wurde. Dies führte dazu, dass diffusionsbegrenzte Oxidationseffekte (DLO-Effekte) auftraten, d. h. dass das Probeninnere weniger stark alterte als oberflächennahe Bereiche. Während der Alterung von EPDM traten sowohl Kettenspaltungen wie auch Vernetzungsreaktionen auf, was sich vor allem in einer Verschlechterung der Zugeigenschaften und einer Abnahme der Druckkraft sowie in einem steigenden Druckverformungsrest äußerte. Bei sehr stark gealterten Proben dominierten ebenfalls Vernetzungsreaktionen, was sich auch in deutlichen DLO-Effekten äußerte. Aufgrund seiner ausgeprägten Oxidations- und Hochtemperaturbeständigkeit wies FKM vergleichsweise geringe Degradationserscheinungen auf. Nur mit Druckspannungsrelaxation und Druckverformungsrest waren nennenswerte Änderungen ersichtlich. Messungen der statischen Leckagerate ergaben, dass die O-Ringe erst bei sehr weit fortgeschrittener Degradation undicht wurden und bis zu diesem Zeitpunkt kein allmählicher Anstieg der Leckagerate beobachtet werden konnte. Aus diesem Grund wurden Leckagemessungen mit einem modifizierten Versuchsaufbau durchgeführt, bei dem die Dichtung während der Messung leicht entlastet wird. Da dieser Test eine dynamische Rückstellung der Dichtung erfordert und damit höhere Ansprüche an die Dichtung stellt, wurde am geprüften EPDM-O-Ring ein früheres Versagen beobachtet. Der entsprechende Alterungszeitpunkt wurde als Versagenszeitpunkt definiert. Dieser wurde anhand der Daten verschiedener Messmethoden mit dem Degradationszustand korreliert und entspricht beispielsweise einem Druckverformungsrest von 80 %. Auf der Grundlage dieses Kriteriums konnten Lebensdauern mittels Zeit-Temperatur-Verschiebung bestimmt werden. Im Rahmen dieser Arbeit wurden zahlreiche Erkenntnisse darüber gewonnen, worauf bei beschleunigten Alterungsversuchen und Lebensdauerprognosen von O-Ringen zu achten ist und welche Fehlerquellen vermieden werden sollten. Dies wird zusammen mit Empfehlungen für eine bestmögliche Versuchsdurchführung ausführlich diskutiert. N2 - In some applications, elastomer seals have to remain leak tight over extended time periods (up to several decades) as an exchange of the seals is not practical. Therefore, it is necessary to be able to predict the lifetime of such seals reliably. For this reason, ageing experiments with O-rings and sheets based on hydrogenated acrylonitrile butadiene rubber (HNBR), ethylene propylene diene rubber (EPDM) and fluorocarbon rubber (FKM) were performed over up to two years at different temperatures. For investigating the changes of material properties during ageing, measurements of i.a. hardness and tensile behaviour as well as dynamic-mechanical and thermogravimetric analyses were conducted. For assessing the relaxation and recovery behaviour of the ageing seals, compression stress relaxation and compression set experiments were performed. Furthermore, leakage rate was measured to detect seal failure. By examining the aged samples, both the property changes and the responsible degradation mechanisms were characterised. Additionally, the most suitable approach for lifetime predictions should be determined using the large database of results from different test methods performed at several ageing times and temperatures. This included identifying an end-of-lifetime criterion that correlates with leakage and thus seal failure. Regarding the property changes and degradation mechanisms of HNBR, a pronounced embrittlement was observed due to dominant crosslinking reactions during ageing. These also resulted in a decrease of oxygen permeability, leading to a reduction of the oxygen transport into the interior sample (mainly of the thicker O-rings). This resulted in diffusion-limited oxidation effects (DLO effects), meaning that the interior of the sample aged less strongly than regions close to the surface. During ageing of EPDM, both chain scission and crosslinking occurred, which became noticeable in deteriorated tensile properties and decreased compression force as well as an increase of compression set. For strongly aged samples, crosslinking dominated as well and also led to pronounced DLO effects. Due to its excellent heat and oxidative stability, FKM exhibited comparatively minor degradation effects. Only compression stress relaxation and compression set showed notable changes. Measurements of static leakage rate revealed that O-rings became untight only after advanced degradation and that no gradual increase of leakage rate could be observed before failure. For this reason, additional leakage measurements were performed using a modified experiment that enabled a small decompression of the seal during the measurement. As this test requires a dynamic recovery of the seal and is thus more demanding, the tested EPDM O-ring failed earlier compared to the purely static test. The corresponding ageing state was defined as the point of failure and correlated to data from other test methods, corresponding e.g. to a compression set of 80 %. Based on this criterion, the lifetimes could be determined using the time-temperature superposition approach. During this work, a number of findings regarding the best way to conduct accelerated ageing experiments and lifetime predictions of O-rings, and how to avoid possible error sources, were collected and are discussed in detail. KW - Elastomer KW - Gummi KW - Degradation KW - Leckage KW - Verpressung KW - Rubber KW - Aging KW - Lifetime prediction KW - Leakage PY - 2017 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-397374 DO - https://doi.org/10.14279/depositonce-5827 SP - 1 EP - 121 PB - Technische Universität CY - Berlin AN - OPUS4-39737 LA - deu AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Pourmand, P. A1 - Wolff, Dietmar A1 - Hedenqvist, M. T1 - Analysis of O-ring seal failure under static conditions and determination of end-of-lifetime criterion N2 - Determining a suitable and reliable end-of-lifetime criterion for O-ring seals is an important issue for long-term seal applications. Therefore, seal failure of ethylene propylene diene rubber (EPDM) and hydrogenated nitrile butadiene rubber (HNBR) O-rings aged in the compressed state at 125 °C and at 150 °C for up to 1.5 years was analyzed and investigated under static conditions, using both non-lubricated and lubricated seals. Changes of the material properties were analyzed with dynamic-mechanical analysis and permeability experiments. Indenter modulus measurements were used to investigate DLO effects. It became clear that O-rings can remain leak-tight under static conditions even when material properties have already degraded considerably, especially when adhesion effects are encountered. As a feasible and reliable end-of-lifetime criterion for O-ring seals under static conditions should include a safety margin for slight dimensional changes, a modified leakage test involving a small and rapid partial decompression of the seal was introduced that enabled determining a more realistic but still conservative end-of-lifetime criterion for an EPDM seal. KW - EPDM KW - HNBR KW - Seal failure KW - Leak-tightness KW - DLO KW - Oxygen permability KW - DMA KW - Indenter modulus PY - 2019 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-486125 DO - https://doi.org/10.3390/polym11081251 SN - 2073-4360 VL - 11 IS - 8 SP - 1251, 1 EP - 19 PB - MDPI CY - Basel, CH AN - OPUS4-48612 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Zaghdoudi, M. A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Oxidative ageing of elastomers: experiment and modelling N2 - 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. KW - Compression Set KW - Compression stress relaxation KW - Modelling KW - Ageing KW - Microhardness PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-609332 DO - https://doi.org/10.1007/s00161-022-01093-9 VL - 36 SP - 289 EP - 297 PB - Springer Nature AN - OPUS4-60933 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Zaghdoudi, Maha A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Overview of ongoing long-term ageing investigations on elastomer seals N2 - At the Bundesanstalt für Materialforschung und -prüfung (BAM) in Division 3.4 Safety of Storage Containers, one of our tasks is to evaluate the safety of containers designed for disposal of low and intermediate radioactive waste. As such containers might be transported before and stored until disposal, safe enclosure of the radioactive inventory is important for this time span. Elastomer O-rings are widely used as barrier seals in these containers. Thus, as for many other applications, an understanding of the practical effects of ageing degradation on elastomer seals during long-term exposure is mandatory for predicting the lifetime of such components. According to a long-term test programme on three kinds of rubbers (EPDM and FKM (relevant for application), HNBR (for comparison)), over several years we have studied the degradation and the change of mechanical properties (e.g. hardness, strain at break) at four different ageing temperatures (75 °C, 100 °C, 125 °C and 150 °C) as well as the change of sealing properties. Continuous and intermittent compression stress relaxation (CSR) measurements were performed in order to investigate the respective contribution of crosslinking and chain scission to the observed degradation effects. Thus, the degradation kinetics and mechanisms could be resolved more clearly. For assessing the seal performance, compression set (CS) and leakage rate measurements were conducted. The experimental results showed that the O-rings remained leak-tight under purely static conditions even when CSR, CS and mechanical properties already indicated far advanced degradation. For this reason, a modified leakage test involving a small and rapid partial decompression of the seal was developed that enabled determining an end-of-lifetime criterion for O-rings with a safety margin for thermal shrinkage and vibrations. KW - Seal KW - O-Ring KW - Ageing KW - Component tests PY - 2020 SN - 1863-7116 VL - 15 IS - 3 SP - 146 EP - 151 PB - Gupta CY - Ratingen AN - OPUS4-51161 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Influence of Ageing on Sealability of HNBR, EPDM and FKM O-rings N2 - At BAM, which is the 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 containers. Besides examining the low-temperature behaviour and irradiation effects of elastomeric seals, it is our goal to evaluate 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) up to 1 year. In order to assess sealability, O-rings are 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 are aged as well. Further methods characterising seal performance are compression stress relaxation (CSR) reflecting the loss of sealing force of a compressed seal over time, and compression set (CS) which represents the recovery behaviour of a seal after release from compression. Additionally, hardness is measured for information about the change of mechanical properties. The experimental results indicate that while hardness, CSR and CS show considerable degradation effects, the leakage rate stays constant or even decreases until shrinkage and the loss of resilience of the aged seal leads to the formation of a leakage path. This indicates that static leakage rate, which is the only available direct seal performance criterion, has only limited sensitivity for the degradation of the seal material. T2 - International Sealing Conference CY - Stuttgart, Germany DA - 12.10.2016 KW - Rubber KW - Seal KW - Degradation PY - 2016 SN - 978-3-8163-0674-9 VL - 2016 SP - 551 EP - 563 PB - VDMA AN - OPUS4-38014 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Kömmling, Anja T1 - Effects of Adapted Ageing Methodology for Elastomeric O-ring Seals N2 - At BAM Federal Institute for Materials Research and Testing in Germany, it is our responsibility to evaluate the safety of casks designed for transport and/or storage of radioactive material. This includes investigating the elastomer seals used in the containers. Our current goal is a deeper understanding of ageing processes and examination of service lifetime of compressed O-ring seals with regard to interim storage periods which might be longer than the currently licensed 40 years in Germany. For this reason, we started an ageing programme with selected rubbers (HNBR, EPDM, FKM) for investigating the change of properties during accelerated ageing over long periods of time (up to five years). In contrast to standard procedure which recommends the ageing of standard test pieces, we are ageing O-rings, both uncompressed and compressed [1]. This approach takes into account the specific geometry and stress state of compressed O-rings. Additionally, it allows leakage rate measurements as the most important property of the sealing system under conditions relevant to the application. Other investigated properties and applied methods include hardness, dynamic mechanic analysis (DMA), thermogravimetric analysis (TGA), compression stress relaxation (CSR, loss of sealing force over time), compression set (CS, increases if resilience decreases), density and tensile tests. The aim is to correlate leakage rate with common material properties in order to identify a suitable and easily measurable end-of-lifetime criterion for elastomer O-ring seals. Furthermore, the appearance of diffusion-limited oxidation (DLO) effects is investigated, as these effects can lead to heterogeneous ageing and thus distorted bulk properties, resulting in overestimated lifetimes [2]. Extrapolations are made using time-temperature shifts and Arrhenius graphs. For hardness and compression set data the extrapolation leads to different lifetimes. This is because crosslinking and chain scission reactions influence hardness in opposite directions [3], whereas both effects add up to increase compression set [4]. After 0.5 years of ageing, EPDM exhibits only slight hardness increase except at 150 °C, while CS increases substantially at all ageing temperatures. On the other hand, for HNBR, both hardness and CS increase strongly. This confirms that crosslinking is the major degradation mechanism in HNBR [5], while in EPDM both crosslinking and chain scission are apparent [6]. Consequently, hardness is not a suitable measure for extrapolation, as a slight hardness increase can be accompanied by significant chain scission, resulting in severe degradation in other properties, such as CS. NMR, TGA, DMA and density measurements can give further information about the contribution of crosslinking or chain scission in the materials at different ageing stages. The experiments are in progress and results will be presented at the conference. References [1] Kömmling A, Waste Management Symposia 2015. [2] Gillen KT, Polym. Eng. Sci. 1989:29:1. [3] Snijders EA, Polym. Degrad. Stab. 2005:89:2. [4] Andrews RD, J. Appl. Phys. 1946:17:5. [5] Bhattacharjee S, Polym. Degrad. Stab. 1991:31:1. [6] Bender H, Kautsch. Gummi Kunststoffe 2001:54. T2 - Polymer Degradation Discussion Group CY - Stockholm, Sweden DA - 2015-08-30 PY - 2015 AN - OPUS4-34094 LA - deu AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Weber, Mike A1 - Zaghdoudi, Maha A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - A numerical approach to correlate compression stress relaxation and compression set of elastomer O-rings with tightness N2 - The excellent mechanical properties of elastomer seals at a wide range of temperatures as well as their high versatility and recovery potential under several load conditions make these materials well suitable for the application in containers designed for transport and disposal of negligible heat generating radioactive waste. While a seal exchange at defined intervals is typical in many conventional applications, it is impossible or at least hard to perform when principles of minimization of radiation exposure have to be considered which prohibit an avoidable cask handling. An extensive knowledge of the change of the elastomer properties during aging and the availability of reliable end-of-lifetime criteria to guarantee the safe enclosure of the radioactive material for the required time are mandatory. As BAM is involved in most of the national cask licensing procedures and in the evaluation of cask-related long-term safety issues, great efforts have already been made and are still ongoing to scientifically support this task. Among other representative types of elastomers, specimen made from ethylene propylene diene rubber (EPDM) were tested before, during and after aging to capture the with respect to application most important of their complex mechanical properties. Exemplary results of these investigations were used to calibrate material models implemented in the commercial finite element software ABAQUS/Standard®. The finite element model already presented in previous works uses a sequential temperature displacement coupling. The calculated compression stress relaxation (CSR) and compression set (CS) values do satisfactorily match the experimental results. In many investigations performed at BAM both values (CSR and CS) were identified as key indicators of elastomer’s long-term performance. However, the possibility to correlate these equivalent indicators with performance values such as tightness and leakage rate, measurable in the mounted state, is an important goal of our future work. In the presented study the ABAQUS® feature of “pressure penetration” is introduced in the suggested finite element model for this purpose. It provides the possibility to simulate the penetration of a gas into a possible gap between flange and O-ring causing an opening of a leakage path. Three dimensional and axis-symmetric finite element models were generated to represent flat and grooved flanges of different dimensions. The sensitivity of the feature to several input parameters is investigated and the observed behavior of the O-ring is correlated with the results of performed leakage tests. T2 - ASME 2021 Pressure Vessels & Piping Conference (PVP2021) CY - Online meeting DA - 13.07.2021 KW - Elastomer KW - Tightness KW - Leakage KW - Compression set KW - Compression stress relaxation PY - 2021 SN - 978-0-7918-8535-2 DO - https://doi.org/10.1115/PVP2021-61976 SP - 1 EP - 8 PB - American Society of Mechanical Engineers (ASME) CY - New York, NY, USA AN - OPUS4-54422 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Zaghdoudi, Maha A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Scission, cross-linking, and physical relaxation during thermal degradation of elastomers N2 - Elastomers are susceptible to chemical ageing, i.e., scission and cross-linking, at high temperatures. This thermally driven ageing process affects their mechanical properties and leads to limited operating time. Continuous and intermittent stress Relaxation measurements were conducted on ethylene propylene diene rubber (EPDM) and hydrogenated nitrile butadiene rubber (HNBR) samples for different ageing times and an ageing temperature of 125 °C. The contributions of chain scission and cross-linking were analysed for both materials at different ageing states, elucidating the respective ageing mechanisms. Furthermore, compression set experiments were performed under various test conditions. Adopting the two-network model, compression set values were calculated and compared to the measured data. The additional effect of physical processes to scission and cross-linking during a long-term thermal exposure is quantified through the compression set analysis. The characteristic times relative to the degradation processes are also determined. KW - Ageing KW - Scission KW - Cross-linking KW - Compression set KW - Physical relaxation PY - 2019 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-486091 DO - https://doi.org/10.3390/polym11081280 SN - 2073-4360 VL - 11 IS - 8 SP - 1280, 1 EP - 12 PB - MDPI AN - OPUS4-48609 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Kömmling, Anja A1 - Grelle, Tobias A1 - Jaunich, Matthias A1 - Goral, Milan A1 - Wolff, Dietmar T1 - Three-dimensional thermal expansion of neat and irradiated (U)HMWPE materials at elevated temperatures N2 - The thermal expansion of polymeric parts can be an issue in many applications where the available space is limited, or exact dimensions of the part are required. For this study, a device was designed and built that allowed measuring the thermal expansion simultaneously in all three spatial directions on cubic samples with real-scale dimensions (78 mm edge length). The results are shown between 25 °C and 125 °C for two PE materials, one HMWPE and one tempered UHMWPE, for non-irradiated samples as well as cubes that have been irradiated with 100 and 400 kGy. The results measured with the new device were very similar to those measured with conventional thermo-mechanical analysis equipment and to literature data of UHMWPE. The HMWPE material shows a much larger thermal expansion coefficient in one direction compared to the other two directions during the first heating due to frozen stresses from the pressing step during material manufacturing. These stresses are mostly released by the expansion during the first heating, so that the expansion during the second heating is more uniform. The overall volumetric expansion is the same for both heating runs. By contrast, the tempered UHMWPE material shows no significant difference between first and second heating run, as the stresses from processing could already relax in the tempering step. The irradiation treatment does not affect the values significantly for the given test set-up. KW - Lupolen KW - Ultra high molecular weight polyethylene KW - GUR KW - Coefficient of thermal expansion KW - High temperature PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-563987 DO - https://doi.org/10.1016/j.polymertesting.2022.107841 SN - 0142-9418 VL - 117 SP - 1 EP - 8 PB - Elsevier Ltd. AN - OPUS4-56398 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Kömmling, Anja T1 - Research at BAM for evaluating long term safety of container systems and components N2 - Safety of long term containment and storage of radioactive waste is an essential issue, which is increasingly gaining international attention. Extending interim storage beyond initial license periods is one of the major challenges worldwide. BAM has been involved in all kinds of radioactive waste container safety evaluation for storage and transportation including their long term performance from the very beginning. Today, all work related to the safe management of radioactive waste is linked by the activity field “Nuclear Waste Management” within the Focus Area “Energy” at BAM and in conjunction with a research strategy and agenda. Most recently, the working group “Long Term Safety of Container Systems and Components” was established to launch and perform research projects related to safety issues concerning the extended interim storage of radioactive waste. For example, within our project LaMEP, we investigate ageing effects of metal and elastomer seals as well as polymeric neutron shielding materials, which are container components that fulfil major safety functions. The results of the experiments help to understand the long term behaviour of these components. Likewise, our project BRUZL started at BAM in 2018 with the aim of developing a fracture mechanics approach to understand and describe a potential brittle failure mechanism of fuel cladding during long-term interim storage. BAM also contributes to the GRS project “Development of methods and models and international exchange for safety evaluation in the frame of interim storage of radioactive waste”. Additionally, BAM is involved in several international research programmes dealing with extended interim storage, such as the European Joint Programme on Radioactive Waste Management (EURAD), the Extended Storage Collaboration Program (ESCP) and IAEA Coordinated Research Projects. The present contribution provides a comprehensive overview of BAM research activities contributing to national and international gap analyses and to filling knowledge gaps regarding the safe long term management of radioactive waste. T2 - Annual Meeting on Nuclear Technology 2019 CY - Berlin, Germany DA - 07.05.2019 KW - Radioactive Waste KW - Container Safety KW - Metal Seals KW - Elastomer Seals KW - Fuel cladding PY - 2019 AN - OPUS4-48437 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Zaghdoudi, Maha A1 - Weber, Mike A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Simulation of compression set of epdm o-rings during aging N2 - It is common practice in the application of finite element analysis to model compression set (CS) of elastomers during aging with two different material models according to the two-network theory of Tobolsky. The theory relies on the existence of two networks. The first one represents the original network after vulcanization and is sensitive to chain scission. The second network accounts for the formation of additional crosslinking during aging. Besides the use of user subroutines to describe the two-network model, an element overlay technique is also needed as the full set of both material behaviors did not exist for assignment to a single element. This element overlay technique is valuable for research and developmental purposes but makes extension to industrial usage quite challenging. Our goal is to simulate the CS of elastomers after long-term aging in a commercial finite element software with no need for extra subroutine codes or mesh superposition. Ethylene propylene diene (EPDM) O-rings were aged in a compressed state at 75 °C, 100 °C, 125 °C and 150 °C for up to 183 days. Investigations of the experimental test results were used to identify material models and their parameters to develop a finite element model to simulate CS. The model was implemented in the finite element software ABAQUS/Standard® with a sequential temperature-displacement coupling. Regarding the influence of temperature, the Arrhenius equation is adopted for the time-temperature relationship. The activation energy value that is required for the simulation is firstly determined from shifting the experimental CS results with the time-temperature superposition technique and plotting the shift factors in an Arrhenius diagram. The experiments were compared with the simulation results. Afterwards different activation energies were used in the simulation and discussed. A suitable choice of the activation energy value with regard to the reference temperature and the test temperature is presented. With the chosen activation energies, the match between numerical CS values after long-term aging and the experimental results was improved. T2 - ASME 2022 Pressure Vessels & Piping Conference CY - Las Vegas, USA DA - 17.07.2022 KW - Simulation KW - Compression set KW - EPDM KW - Aging PY - 2022 SP - 1 EP - 9 AN - OPUS4-57370 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Vega Puga, E. A1 - Wachtendorf, Volker A1 - Kömmling, Anja A1 - Brendelberger, S. A1 - Jaunich, Matthias A1 - Sattler, C. T1 - Lifetime prediction and degradation assessment of FKM and FFKM O-rings under high temperature thermo-oxidative ageing N2 - To support the development of solar reactor technologies for hydrogen production, this study investigates the thermo-oxidative degradation mechanisms of fluorinated elastomers and predicts their lifetimes at high temperatures (200–300 ◦C) consistent with the application requirements. An accelerated ageing programme is conducted with FKM and FFKM O-rings and flat samples for up to 21 days. Optical microscopy is used to analyse the exposed seals’ morphological changes, while IR microscopy is utilised to investigate the underlying chemical degradation mechanisms of both elastomers. Findings suggest that FKM’s degradation arises from dehydrofluorination of the polymer, followed by chain scission and backbone cleavage as a result of the oxidation of newly formed C=C double bonds. FFKM’s degradation is primarily associated with chain scission, but there is also indication that post-curing processes may occur during material ageing. Furthermore, hardness, equilibrium compression set (CS), continuous compression stress relaxation (CSR) and leakage rate tests are used to evaluate changes in the mechanical properties and sealing performance of the elastomers. Equilibrium CS data is extrapolated using time-temperature shifts (TTS) and used to derive an end-of-life criterion of 75 % equilibrium CS, which correlates to leakage rates higher than a predetermined threshold. Service lifetime predictions of FKM and FFKM O-rings at several temperatures are performed and a seal operating temperature of 200 ◦C is suggested, which ensures reasonable O-ring replacement intervals of more than half a year in the solar reactor for both considered materials. KW - Fluoroelastomer KW - Perfluoroelastomer KW - Thermo-oxidative ageing KW - Lifetime prediction KW - Compression set PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-630112 DO - https://doi.org/10.1016/j.polymertesting.2025.108820 SN - 1873-2348 VL - 147 SP - 1 EP - 17 PB - Elsevier BV CY - Amsterdam AN - OPUS4-63011 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Ageing of elastomeric seals for storage containers N2 - At BAM Federal Institute for Materials Research and Testing in Germany, it is our responsibility to audit the safety of casks designed for transport and/or storage of radioactive material. With regard to the requirements on long-term safety of the containers, it is necessary to evaluate the service lifetime of the elastomeric seals used in the containers. With ageing, the elastomers will gradually lose their elasticity and their ability for recovery, which might result in a leakage above the allowed level or in a release of radioactivity during an incident. It is important to know the rate of degradation and which property can be used as an practical and easily measurable end-of-lifetime criterion. For this reason, we devised ageing experiments on different kinds of elastomers, namely FKM, EPDM and HNBR. The former two are actually used in containers for radioactive wastes – either as auxiliary seal in casks containing high activity waste, or as main seal in casks for medium or low activity waste. The latter is an often used seal material that is tested for comparative reasons. In our ageing program, these three materials are aged at four different temperatures (75 °C, 100 °C, 125 °C and 150 °C) in order to extrapolate the data to service temperature using a suitable model. They are examined at logarithmic time intervals of several days up to 5 years. The samples are aged in their undeformed O-ring state as well as compressed between flanges with a deformation corresponding to the actual compression during service. Thus we can compare the ageing between relaxed and stressed sample. Additionally, we are ageing samples in flanges that allow leakage rate measurements. Other measurements include monitoring of the recovery force of the seal and the compression set. Furthermore, the samples are examined by thermal and dynamic-mechanical analysis for detecting changes in the glass transition temperature due to crosslinking or chain scission in the material. Besides, hardness is measured as a practical macroscopic indicator. Until now, we have analyzed samples aged up to 100 days. At the highest ageing temperature of 150 °C, the compressed EPDM has already reached a compression set of 95 %, while HNBR and FKM have reached 80 % and 30 %, respectively. Furthermore, HNBR has reached a Shore D hardness of 85, which is an immense increase after the initial value of 80 Shore A. However, when looking at the cross-section of the sample, it was obvious that only a layer of about 1 mm thickness has become so hard, while the inner part remained rubbery. This shows that there has been intense crosslinking mostly near the surface of the HNBR which forms a kind of oxygen diffusion barrier, inhibiting the thermooxidation of the inner part of sample which can retain elastic properties. In EPDM, the oxygen permeability is much greater, which leads to a more homogeneous degradation across the whole sample and thus resulted in a higher compression set. The low compression set of FKM shows the outstanding high-temperature properties of this material. T2 - Annual Meeting on Nuclear Technology 2015 CY - Berlin, Germany DA - 2015-05-05 KW - Elastomer KW - Rubber KW - Aging KW - Lifetime KW - Seal KW - Cask KW - Compression PY - 2015 SN - 978-3-926956-98-9 SP - 1 EP - 10(?) PB - INFORUM-Verl. u. Verwaltungsges. AN - OPUS4-33782 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Aging of elastomeric seals for storage casks N2 - Elastomeric seals are used in many containers, including casks for radioactive waste. However, like all polymers, elastomers are prone to aging, which leads to a loss of sealing force and the ability for recovery which can ultimately result in leakage. Therefore it is important to be able to define an end-of-lifetime criterion and to judge the lifetime of elastomeric seals. For this reason, we started an aging program on three kinds of rubbers (HNBR, EPDM, FKM), monitoring the change of properties at four different aging temperatures over extended periods up to five years. The measured data is used for lifetime prediction by applying a suitable model. T2 - WM2015 Conference CY - Phoenix, Arizona, USA DA - 15.03.2015 KW - Aging KW - Elastomer KW - Seal KW - Leakage KW - Compression PY - 2015 SN - 978-0-9828171-4-8 SP - 15080, 1 EP - 12 AN - OPUS4-33253 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Kömmling, Anja T1 - Ageing and lifetime prediction of O-ring seals made of HNBR, EPDM and FKM N2 - BAM is the federal institute for materials research and testing in Germany. One of our tasks is to evaluate the safety of casks designed for transport and/or storage of radioactive waste. As elastomeric seals are used in the containers as safety-relevant parts, it is our goal to be able to evaluate the service lifetime of the seals with regard to the requirements for long-term safety (40 years and more) of the containers. For this reason, an accelerated ageing programme with selected rubbers often used for seals (HNBR, EPDM and FKM) was started. Ageing was performed at four different temperatures (75 °C, 100 °C, 125 °C and 150 °C) for up to 2 years. For assessing properties related to the sealability, O-rings were aged in compression by 25 % (corresponding to the compression during service) between plates. For comparison, uncompressed O-rings were aged as well. The aged materials were characterized with conventional polymer analysis methods such as hardness and tensile tests, but also with more seal-specific methods such as compression stress relaxation (CSR, reflecting the loss of sealing force of a compressed seal over time), and compression set (CS, representing the recovery behaviour of a seal after release from compression). CS is chosen as the property for lifetime prediction as it is both sensitive to degradation and related to the seal performance. CS data is extrapolated to 60 °C, which yields lifetimes of approximately 5 years for HNBR and 64 years for EPDM for a criterion of 85 % CS respectively, and approx. 40 years for FKM for a criterion of 65 % CS (the highest value measured so far). T2 - Kautschuk Herbst Kolloquium / Fall Rubber Colloquium 2016 CY - Hanover, Germany DA - 22.11.2016 KW - Rubber KW - Compression set KW - Extrapolation KW - Leakage PY - 2016 AN - OPUS4-38480 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -