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 JF - Polymer Testing 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 - JOUR A1 - Zaghdoudi, Maha A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Oxidative ageing of elastomers: Experiment and modelling JF - Continuum mechanics and thermodynamics 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 - JOUR A1 - Zaghdoudi, Maha A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Wolff, Dietmar T1 - Erroneous or Arrhenius: A Degradation Rate-Based Model for EPDM during Homogeneous Ageing JF - Polymers N2 - To improve the predictive capability of long-term stress relaxation of elastomers during thermo-oxidative ageing, a method to separate reversible and irreversible processes was adopted. The separation is performed through the analysis of compression set after tempering. On the Basis of this separation, a numerical model for long-term stress relaxation during homogeneous ageing is proposed. The model consists of an additive contribution of physical and chemical relaxation. Computer simulations of compression stress relaxation were performed for long ageing times and the results were validated with the Arrhenius treatment, the kinetic study and the time-temperature superposition technique based on experimental data. For chemical relaxation, two decay functions are introduced each with an activation energy and a degradative process. The first process with the lower activation energy dominates at lower ageing times, while the second one with the higher activation energy at longer ageing times. A degradation-rate based model for the evolution of each process and ist contribution to the total system during homogeneous ageing is proposed. The main advantage of the model is the possibility to quickly validate the interpolation at lower temperatures within the range of slower chemical processes without forcing a straight-line extrapolation. KW - Kinetic study KW - Arrhenius KW - TTS KW - Modeling KW - Chemical processes KW - Stress relaxation PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-512931 DO - https://doi.org/10.3390/polym12092152 SN - 2073-4360 VL - 12 IS - 9 SP - 1 EP - 21 AN - OPUS4-51293 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Kömmling, Anja A1 - Jaunich, Matthias A1 - Goral, Milan A1 - Wolff, Dietmar T1 - Insights for lifetime predictions of O-ring seals from five-year long-term aging tests JF - Polymer Degradation and Stability N2 - O-rings made of HNBR, EPDM and FKM were aged in the compressed and uncompressed state at 150 °C, 125 °C, 100 °C, 75 °C, 60 °C and 23 °C for aging times of up to five years. Hardness was measured and increased with aging time and temperature for HNBR and EPDM, but it remained practically constant for FKM. Indenter modulus measurements were performed on the lateral O-ring surface (that was free of DLO effects) to assess an influence of the compression during aging, but none was detected. The equilibrium compression set (CS) exhibited faster and stronger degradation than hardness and was used for lifetime predictions using the time-temperature superposition (TTS) principle. With an end-of-lifetime criterion of 70 % CS, lifetimes of 4.5 years, 50 years and 526 years at 75 °C were estimated for HNBR, EPDM and FKM, respectively. The activation energies derived from an Arrhenius plot of the shift factors from the TTS were 85 kJ/mol, 99 kJ/mol and 78 kJ/mol for HNBR, EPDM and FKM, respectively, revealing that a higher activation energy does not necessarily mean that the material has a higher lifetime at lower temperatures. Furthermore, the measured lifetime of EPDM O-rings at 100 °C (5 years) was compared to that predicted on the basis of the lifetime at 150 °C as well as 125 °C using the corresponding shift factors. The error of the prediction was only ± 4 %. However, this precise prediction could only be achieved using the five-year long-term aging data. When using only data from aging times up to 0.5 years and 2 years, the lifetime of EPDM O-rings at 100 °C was underestimated by 31 % and 22 %, respectively. KW - HNBR KW - EPDM KW - FKM KW - DLO KW - Hardness KW - Compression set KW - Rubber KW - Elastomer KW - Degradation PY - 2020 DO - https://doi.org/10.1016/j.polymdegradstab.2020.109278 VL - 179 SP - 109278 PB - Elsevier Ltd. AN - OPUS4-51060 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 JF - Rubber, fibres, plastics international - RFP 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 - 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 JF - Polymers 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 - 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 JF - Polymers 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 - Kömmling, Anja A1 - von der Ehe, Kerstin A1 - Wolff, Dietmar A1 - Jaunich, Matthias T1 - Effect of high-dose gamma irradiation on (U)HMWPE neutron shielding materials JF - Radiation Physics and Chemistry N2 - High and ultra-high molecular weight polyethylenes were gamma-irradiated with doses up to 600 kGy. The changes in the material properties were analysed using DSC, DMA, IR spectroscopy, as well as measurements of density and insoluble content. The irradiation led to an increase of the degree of crystallinity because of chain scissions during irradiation, leading to shorter and thus more mobile chains. Both the plateau value of the shear modulus G′ and the insoluble content increased with Irradiation dose, indicating the formation of additional crosslinks. Furthermore, IR spectroscopy revealed irradiation induced oxidation and the formation of double bonds, indicating that some of the hydrogen atoms responsible for the neutron shielding capability have been released. KW - Ultra high molecular weight KW - Polyethylene KW - Gamma irradiation KW - Crosslinking KW - Oxidation PY - 2018 DO - https://doi.org/10.1016/j.radphyschem.2017.02.014 SN - 0969-806X VL - 142 SP - 29 EP - 33 PB - Elsevier AN - OPUS4-42941 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 JF - Polymer Testing 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 - Grelle, Tobias A1 - Wolff, Dietmar A1 - Probst, Ulrich A1 - Jaunich, Matthias A1 - Völzke, Holger T1 - Component and material investigations on metal seals for high level radioactive waste containers JF - Nuclear future N2 - Long-term investigations performed at BAM look to extend the state of knowledge on safety-related components of interim storage containers. Metal seals act as the primary sealing barrier in the bolted double lid closure system of the containers. The behaviour of metal seals has been investigated for ageing times up to 8.5 years and for various temperatures. The main cause for reduction in useable resilience overtime was due to creep deformation of the outer jacket of the seal. KW - Metal seal KW - Radioactive waste containers KW - Creep KW - Long-term behaviour PY - 2018 SN - 1745-2058 SP - 32 EP - 34 PB - Nuclear Institute CY - London AN - OPUS4-48206 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -