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Organisationseinheit der BAM
Elastomer seals are mounted as barrier seals in lid systems of containers designed for transport and disposal of negligible heat generating radioactive waste and as auxiliary seals in spent fuel storage and transportation casks (dual purpose casks (DPC)). When the behavior of mounted seals under normal and hypothetical accident conditions of disposal and transport is to be simulated, a comprehensive knowledge of their complex mechanical properties at every state of aging is necessary. In previous works, BAM’s efforts in experimental investigations on specimen artificially aged at different temperatures and times and the implementation of the found results in finite element material models were presented. Additionally, our approaches to reproduce the aging process itself and to extrapolate the results of artificially accelerated aging to longer times were presented. Numerical simulations have shown that the behavior of the seal during mounting and one-sided pressurizing and the resulting performance values such as leakage rate strongly depend on the coefficient of friction (COF) between flange and seal. The friction coefficient, in turn, depends on the aging state of the elastomer material as several publications suggest (see below).
Dynamic COF between an exemplary ethylene propylene diene rubber (EPDM) material and a stainless steel ball were determined by using a self-designed linear oscillation tribometer. Unaged and artificially aged EPDM specimen stored for 30 days and 100 days at a temperature of 150 °C were tested. A stainless steel ball (d=10 mm) is brought in contact with the specimen’s surface und loaded by normal forces of 2.5 N, 5 N, 10 N and 20 N. During a reciprocating movement of the EPDM sheet, the horizontal force/friction force is continuously measured, and the COF can be derived.
It is well known that friction is a complex phenomenon especially in soft materials. It cannot be excluded that the measured friction force is influenced by additional force components, resulting from the ball’s grooving through the elastomer’s surface. This force depends on the penetration depth of the ball and on the resistance of the elastomer in its different states of aging. The latter results from microstructural changes i.e., chain scission and additional crosslinking that occur during aging which in turn influence the softening or hardening of the material.
A finite element (FE) ABAQUS® model was developed to reproduce the measurement process. It should help to better understand the physical mechanisms and to quantify the percentage of measured forces resulting from real friction on the one hand and forces resulting from unintended side effects that could falsify the result on the other hand. The behavior of the elastomer in its different states of aging is reproduced by a FE material model already presented in previous works of BAM.
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.
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.
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).
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.
Eine Aufgabe des Fachbereichs 3.4 Sicherheit von Lagerbehältern der Bundesanstalt für Materialforschung und -prüfung (BAM) ist es, die Sicherheit von Behältern zur Lagerung von radioaktivem Abfall mit vernachlässigbarer Wärmeentwicklung zu bewerten. Da solche Behälter vor der Entsorgung transportiert und gelagert werden, ist während dieser Zeit ein sicherer Einschluss des radioaktiven Inhalts von größter Bedeutung. Zur Abdichtung dieser Behälter sind Elastomer-O-Ringe weit verbreitet. Um für solche, wie auch für viele andere Anwendungen, eine Voraussage über die Lebensdauer dieser Komponenten treffen zu können, ist es unerlässlich zu verstehen, welchen Einfluss der durch Alterung hervorgerufene Abbau auf Dauer auf die Elastomerdichtungen hat. In einem Langzeittest wurden drei Kautschukarten (EPDM und FKM, die für die Anwendung relevant sind, und HNBR als Vergleich) über mehrere Jahre untersucht. Dabei wurden die Veränderungen der mechanischen Eigenschaften (z. B. Härte und Bruchdehnung) bei vier verschiedenen Alterungstemperaturen (75 °C, 100 °C, 125 °C und 150 °C) sowie das Dichtungsverhalten betrachtet. Um den Einfluss von Vernetzung und Kettenspaltung auf die beobachteten Alterungseffekte zu bestimmen, wurden Messungen zur kontinuierlichen und intermittierenden Druckspannungsrelaxation durchgeführt. Dadurch konnten Erkenntnisse über Kinetik und Mechanismus der Abbaureaktionen
gewonnen werden. Zur Einschätzung des Dichtungsverhaltens wurden Durckverformungsrest und Leckagerate gemessen. Die Ergebnisse zeigen, dass die O-Ringe unter statischen Bedingungen auch dann dicht halten, wenn die Werte für Druckverformungsrest, Druckspannungsrelaxation und mechanische Eigenschaften schon auf einen fortgeschrittenen Alterungsabbau hindeuten. Aus diesem Grund wurde ein modifizierter Dichtigkeitsversuch mit einer geringen und schnellen teilweisen Entlastung der Dichtung entwickelt, mit dessen Hilfe sich ein Lebensdauerkriterium bestimmen lässt, das eine Sicherheitsspanne für thermische Schrumpfung und Vibrationen beinhaltet.
Unsere Aufgabe im Fachbereich 3.4 der Bundesanstalt für Materialforschung und prüfung (BAM) ist die sicherheitstechnische Begutachtung von Transport- und Lagerbehältern für radioaktiven Abfall, die für langfristige Zwischenlagerung ausgelegt sind. Ein Arbeitsschwerpunkt ist die Bewertung der Lebensdauer von Metall- und Elastomerdichtungen in den Behältern im Hinblick auf die Anforderungen für langfristige Behältersicherheit (min. 40 Jahre in Deutschland). Um die Eigenschaftsänderungen der Elastomerdichtungen während einer beschleunigten Alterung über lange Zeiträume (bis zu fünf Jahre) untersuchen zu können, wurde ein Alterungsprogramm an ausgewählten Elastomeren (HNBR, EPDM, FKM) begonnen.
Im Gegensatz zu Normalterungsverfahren altern wir keine Normteile, sondern O-Ringe im unverpressten sowie verpressten Zustand. Diese Vorgehensweise ermöglicht die Bewertung des Einflusses der Verpressung auf die Alterung sowie die Untersuchung des Bauteilversagens mittels Leckageratenmessungen unter anwendungsnahen Bedingungen. Weitere Charakterisierungsmethoden sind Härtemessung, dynamisch-mechanische Analyse (DMA), Thermogravimetrie (TGA), Druckspannungsrelaxation, Druckverformungsrest (DVR), Dichtebestimmung und Zugversuch. Das Ziel ist, die Leckagerate mit anderen Eigenschaften bzw. Methoden zu korrelieren, um so ein aussagekräftiges und leichter zu bestimmendes Lebensdauerkriterium für elastomere O-Ringe abzuleiten.
Während der Alterung können in Abhängigkeit von Material sowie Alterungsdauer und –temperatur Inhomogenitäten aufgrund von diffusionsbegrenzter Oxidation auftreten, durch die sich unterschiedliche Eigenschaften an der Oberfläche und im Volumen der Dichtung ergeben, was zu falschen Lebensdauerabschätzungen führen kann. Mittels Mikrohärtemessung über den Querschnitt werden diese Effekte charakterisiert und bei der Extrapolation mittels Zeit-Temperatur-Verschiebung und Arrheniusgraph berücksichtigt. Bisher liegen Daten von bis zu einem Jahr bei vier verschiedenen Temperaturen (75 °C, 100 °C, 125 °C und 150 °C) gealterten Proben vor. Nach 100 Tagen bei 150 °C weisen HNBR und EPDM schon einen DVR von über 80 % auf, aber noch keinen signifikanten Anstieg der Leckagerate. Diese sinkt zunächst während der Alterung, da die Permeabilität aufgrund von Vernetzungsreaktionen sinkt. Bei HNBR ist dies aufgrund der dominanteren Vernetzungsreaktionen während der Alterung noch stärker ausgeprägt als bei EPDM.
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.
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 the investigation of elastomeric seals applied in the containers. Besides examining the low-temperature behavior 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. Furthermore, we deem it necessary to exceed the requirements given in the ageing standard DIN 53508 and take into account diffusion-limited oxidation (DLO) effects and non-Arrhenius behavior when making lifetime predictions. Therefore, we started an ageing programme with selected rubbers (HNBR, FKM and EPDM) which are oven-aged at four different temperatures (75 °C, 100 °C, 125 °C and 150 °C) in order to extrapolate the data to service temperature using different models and check which one is appropriate. Samples are examined at different times up to 5 years. In order to be able to compare between compressed and relaxed rubber, they are aged in two conditions: the undeformed O-ring state as well as compressed between plates with a compression of 25 % corresponding to the actual compression during service. Additionally, we are ageing samples in flanges that allow leakage rate measurements which is the central performance criterion. Analysis methods include hardness as a quick indicator, compression set and compression stress relaxation as measures reflecting the actual properties of a compressed seal. Additionally, we are applying classical polymer analysis methods like dynamic mechanic analysis and thermogravimetric analysis which show changes in the polymeric structure due to chain scission and crosslinking. Furthermore, we are testing the leakage rate of the O-rings in order to correlate the changes in physical properties to the actual performance of the seal.
First results of samples aged up to 100 days show a strong increase in hardness for HNBR, a moderate increase for EPDM and hardly a change for FKM. A similar result is seen in the compression set of samples aged 100 d at 100 °C in compression as HNBR has reached 60 %, EPDM 25 % and FKM 15 % compression set. However, after ageing at 150 °C, EPDM shows a worse performance with 95 % compression set compared to HNBR with only 80 %. This is probably due to DLO effects in HNBR that appear because of the fast ageing and low oxygen permeability in HNBR. This leads to a deficit of oxygen in the center of the sample which is thus protected from ageing and can retain elastic properties. The full paper shall discuss the changes in material properties observed to date and the impact on the performance of elastomeric seals.
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.