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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.
Overview of ongoing research and future prospects on polyethylene neutron shielding materials at bam
(2023)
The extension of the interim storage period of radioactive waste before disposal will cause additional challenges for the nuclear waste management in Germany, so that an extensive knowledge of the long-term performance of casks, including their components and inventories, will be required for future extended storage licenses.
Ultra-high and high molecular weight polyethylenes ((U)HMW-PE) are used for neutron shielding purposes in casks for storage and transport of spent fuel and high-level waste due to their extremely high hydrogen content. During their service life of several decades as cask components, the PE materials are exposed to neutron and gamma radiation from the radioactive inventory of the casks, mechanical assembling stresses and temperature. All these combined effects affect the material properties of such components which in turn may be crucial for some possible accident scenarios.
At the Bundesanstalt für Materialforschung und -prüfung (BAM), the effects of high temperature exposure in combination with subsequent or previous irradiation were investigated with a comprehensive aging program including thermal aging at 125 °C for different aging periods up to 5 years and irradiation with doses ranging from 50 to 600 kGy.
This contribution provides an overview of the ongoing research related to the structural changes of (U)HMW-PE induced by gamma irradiation and high temperature exposure and focuses on current research perspectives at BAM with regard to the prediction of the dynamic behavior of the material during extended interim storage in case of an accident scenario. First results of the coupled effect of temperature, radiation and mechanical loading will be presented. The effect of microstructural changes induced by gamma irradiation and high temperature on the mechanical behavior of (U)HMW-PE will be assessed.
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.
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.
This publication summarizes the work carried out during an IAEA coordinated research project (CRP) on safe and reliabe management of spent nuclear fuel. This work contributes to the overall goal of demonstrating the performance of spent nuclear fuel and related storage systems components over long durations, and facilitates the transfer of this knowledge to Member States. The technical areas addressed by the CRP participants were related to potential degradation mechanisms in metal casks and concrete overpacks, such as stress corrosion cracking; long term integrity and performance of the fuel cladding; thermo-mechanical behaviour of the metal seals; and long term gamma and neutron shielding capability. The participants also considered past and ongoing demonstration programmes. For each technical topic addressed the main conclusions have been drawn, including information on the development of specific monitoring and inspection techniques as well as future opportunities for closing relevant data gaps. A major achievement is also the establishment of a worldwide network of experts working on current research projects to demonstrate the long term performance of spent fuel in dry storage systems.
Spent fuel storage periods well beyond those originally foreseen are a reality. This publication offers several ideas and approaches that may be considered to address the increasingly longer storage times. The aim is to raise awareness, encourage dialogue and provide ideas on how to manage spent fuel. Key messages include the following:
- Delays in reprocessing or disposal could result in spent fuel being stored for 100 years or longer. Safe, secure and effective storage of spent fuel manages fuel degradation while preserving future fuel cycle options.
- Ageing management programmes apply engineering, operations and maintenance actions to ensure safety is maintained during storage, future handling and transport.
- Site selection and facility and equipment design can significantly reduce the risks and costs of spent fuel storage over longer periods.
- Spent fuel storage configurations can be selected to accommodate uncertain storage periods, to facilitate ageing management and to provide flexibility needed to accommodate the uncertainty of future end points, such as reprocessing or disposal.
- By considering multiple licence renewals, regulatory frameworks can be designed to ensure safe storage until an acceptable end point is achieved.
- Safety can be assured by maintaining shielding, containment, decay heat removal and criticality control. Navigating the complexity of societal beliefs and values, as well as political systems, has proven to be a greater challenge for the management of spent fuel than maintaining its safety and security or addressing the technical and economic aspects.
- Sustainable spent fuel management requires policies and strategies to provide a clear, consistent and stable direction because they drive the need for spent fuel storage as well as the available options and timing for achieving an acceptable end point. Unless States address spent fuel reprocessing and disposal on a sufficient scale to accommodate their spent fuel discharges, then storage for longer and longer periods becomes the de facto end point — which is not considered to be consistent with the responsibility to protect human health and the environment.
An effective, periodic licence renewal process can ensure effective ageing management and strong institutional control. Hence, spent fuel can be safely and securely stored for as long as it may be necessary until transport for reprocessing or disposal. However, the risks and costs of storing the growing inventory of spent fuel will continue to increase; and in the absence of an end point, it will eventually become a significant societal burden.
In this presentation, the history and actual situation of the German nuclear waste management policy of spent fuel (SF) and high-level waste (HLW) is reported. Beside the description of the restructuration of responsible authorities and organizations in Germany, the principle of dry interim storage of SF and HLW in dual purpose casks is explained. The need for extended interim storage towards disposal implicates additional challenges for the nuclear waste management strategy in Germany. (Extended)interim storage, subsequent transportation, and final disposal are closely linked. Integrated approaches concerning waste package designs and operations are supposed to be beneficial for the establishment of efficient long-term SF and HLW management strategies. Knowledge management and staff recruiting, education and training during phase out and beyond nuclear power plant operation are major issues.
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.
Bei der Auswahl eines Standortes für ein Endlager für hochradioaktive Abfälle (Wärme entwickelnde radioaktive Abfälle und ausgediente Brennelemente) in Deutschland werden auf Grundlage des Standortauswahlgesetzes von 2017 die drei potenziellen Wirtsgesteine Steinsalz, Tonstein und Kristallingestein in Betracht gezogen. Die Auswahl eines konkreten Endlagerstandortes steht dabei in engem Zusammenhang mit den für die jeweiligen Wirtsgesteine geeignet erscheinender Endlagersystemen. Zentraler Bestandteil dieser Endlagersysteme sind die Endlagerbehälter, deren Gestaltung und Auslegung maßgeblich die Randbedingungen für die Transport- und Einlagerungstechnik vorgibt und zudem die Nachweise zur Betriebs- und Langzeitsicherheit entscheidend prägt. Daher ist es für die Behälterentwicklung erforderlich, die an Endlagerbehälter zu stellenden Anforderungen systematisch herzuleiten. Auf dieser Grundlage können anforderungsgerechte Endlagerbehälter zielgerichtet für die jeweils zu untersuchenden Endlagerstandorte in unterschiedlichen Wirtsgesteinen entwickelt werden.
Dieser Beitrag fasst die wesentlichen Ergebnisse des von BAM und BGE TECHNOLOGY GmbH im Zeitraum 2017 bis 2020 bearbeiteten und vom Bundesministerium für Wirtschaft und Energie (BMWi) geförderten Forschungsvorhabens KoBrA zusammen, die in einem Abschlussbericht und vier zugehörigen Teilberichten umfassend dokumentiert sind.