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Organisationseinheit der BAM
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.
Component and material investigations on metal seals for high level radioactive waste containers
(2018)
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.
Der Druckverformungsrest (DVR) stellt insbesondere für Dichtungsanwendungen eine wichtige Kenngröße zur Beurteilung der Eignung eines Elastomers dar. Er ermöglicht die Einschätzung des zeitabhängigen Rückstellverhaltens eines Werkstoffs nach Deformation. Neben der Prüfung bei erhöhten Temperaturen, zur Beurteilung des Alterungsverhaltens, lässt sich bei der Durchführung bei tiefen Temperaturen die limitierende Einsatztemperatur bestimmen. Die Versuchsdurchführung unterscheidet sich je nach angewandter Norm und kann einen deutlichen Einfluss auf den DVR-Wert haben. Um bei tiefen Temperaturen eine schnelle Aussage zu gestatten, ist eine im Vergleich zu genormten Methoden deutlich schneller durchzuführende, automatisierte Methode entwickelt und mit Standardmethoden verglichen worden. Durch kontinuierliche Messung des Druckverformungsrests kann die Kinetik der Materialrückstellung betrachtet und dadurch ein effizienter Materialvergleich und eine effiziente Materialauswahl ermöglicht werden. Compression set (CS) is especially for sealing applications an important parameter for material selection. It allows an assessment of the time dependent recovery after deformation.
In addition to testing at elevated temperatures which aims at the evaluation of the ageing behaviour, testing at low temperatures permits the determination of the low working temperature limit. The test procedure varies depending on the applied standard and can show a significant effect on the CS value. In order to allow a quick statement regarding low temperatures an automated procedure being significantly faster realisable in relation to the standardised methods has been developed and compared with standard procedures. Continuous measurement of the compression set allows evaluating the recovery kinetics and therefore an efficient comparison and selection of materials.
Bei der Abschätzung der Beständigkeit von Kunststoffen gegenüber niedermolekularen Flüssigkeiten ist die Kohäsionsenergiedichte CED ein wichtiger Parameter auf molekularer Ebene. Die Vernetzungsdichte ν eines polymeren Festkörpers bildet hierbei einen bedeutsamen Kennwert, der darüber hinaus neben der Löslichkeit wichtige Eigenschaften wie thermische Stabilität und Steifigkeit des Materials charakterisiert. Für die experimentelle Bestimmung von CED und ν eignet sich die Untersuchung des Quellverhaltens in unterschiedlichen Lösungsmitteln. Es werden zwei Messmethoden miteinander verglichen und die Ergebnisse unter Berücksichtigung des molekularen Aufbaus von Proben aus Polyurethan (PU) und hochmolekularem – (HMWPE) und ultrahochmolekularem Polyethylen (UHMWPE) diskutiert. Zum Verständnis des Quellverhaltens dieser Polymerproben in niedermolekularen Lösungsmitteln werden neben den Messergebnissen Literaturdaten zu Grunde gelegt.
German approach and feedback on experience of transportability of SNF packages after interim storage
(2014)
In Germany, the concept of dry interim storage of spent fuel in dual purpose metal casks is implemented, currently for periods of up to 40 years. The casks being used have an approved package design in accordance with the international transport regulations. The license for dry storage is granted on the German Atomic Energy Act with respect to the recently revised 'Guidelines for dry interim storage of irradiated fuel assemblies and heat-generating radioactive waste in casks' by the German Waste management Commission. For transport on public routes between or after long term interim storage periods, it has to be ensured that the transport and storage casks fulfil the specifications of the transport approval or other sufficient properties, which satisfy the proofs for the compliance of the safety objectives at that time. In recent years, the validation period of transport approval certificates for manufactured, loaded and stored packages were discussed among authorities and applicants. A case dependent system of 3, 5 and 10 years was established. There are consequences for the safety cases in the Package Design Safety Report, including evaluation of long term behaviour of components and specific operating procedures of the package. The present research and knowledge concerning the long term behaviour of transport and storage cask components have to be consulted as well as experiences from interim cask storage operations. Challenges in the safety assessment are e.g. the behaviour of aged metal and elastomeric gaskets under IAEA test conditions to ensure that the results of drop tests can be transferred to the compliance of the safety objectives at the time of transport after the interim storage period. Assessment methods for the material compatibility, the behaviour of fuel assemblies and the aging behaviour of shielding parts are issues as well. This paper describes the state of the art technology in Germany, explains recent experience on transport preparation after interim storage and points out arising prospective challenges.
Dual purpose casks for the transportation and storage of spent nuclear fuel and other radioactive materials require very high leak tightness of lid closure systems under accident conditions as well as in the long term to prevent activity release. For that purpose metal seals of specific types with an inner helical spring and outer metal liners are widely used and have shown their excellent performance if certain quality assurance requirements for fabrication and assembling are satisfied. Well defined surface roughness, clean and dry inert conditions are therefore essential. No seal failure in a loaded cask happened under these conditions until today. Nevertheless, the considered and licensed operation period is limited and all safety assessments have been performed and approved for this period of time which is 40 years in Germany so far. However, in the meantime longer storage periods might be necessary for the future and therefore additional material data will be required. BAM is involved in the qualification and evaluation procedures of those seals from the early beginning. Because long term tests are always time consuming BAM has early decided to perform additional tests with specific test seal configurations to gain a better understanding of the long term behaviour with regard to seal pressure force, leakage rate and useable resilience which is safety relevant mainly in case of accidental mechanical loads inside a storage facility or during a subsequent transport. Main test parameters are the material of the outer seal jacket (silver or aluminium) and the temperature. This paper presents the BAM test program including an innovative test mock-up and most recent test results. Based on these data extrapolation models to extended time periods are discussed, and also future plans to continue tests and to investigate seal behaviour for additional test parameters are explained.
Elastomers are widely used as the main sealing materials for containers for low and intermediate level radioactive waste and as an additional component to metal seals in spent fuel and high active waste containers. The safe encapsulation of the radioactive container inventory has to be guaranteed according to regulation and appropriate guidelines for long term storage periods as well as for temperatures as low as -40°C during transport. Therefore, the understanding of failure mechanisms that lead to leakage at low temperatures is of high importance. It is known that the material properties of elastomers are strongly temperature dependent. At low temperatures, this is caused by the rubber-glass transition (abbreviated: glass transition). During continuous cooling, the material changes from a rubber-like entropy elastic to a stiff energy elastic behaviour, which allows nearly no strain or retraction. Hence, rubbers are normally used above their glass transition, but the minimum working temperature limit is not defined precisely; this can cause problems during the above noted applications. Therefore, the lower operation temperature limit of elastomer seals must be determined in dependence of the material properties. Differential scanning calorimetry (DSC) and dynamic mechanical analysis (DMA) are combined with standardised measurements to determine the compression set according to ISO 815. To reduce the test time of the standard tests, a faster technique than normally used was developed. Additionally, the breakdown temperature of the sealing function of complete O ring seals was measured in a component test set-up to compare it with the results of the other tests. The experimental set-up is capable of measuring the leakage rate at low temperatures by the pressure rise method. A fluorocarbon rubber (FKM) was selected for this investigation as it is often used for radioactive waste containers. The materials (seals and test sheets) were purchased from a commercial seal producer.
The aging management system for the mechanical components of nuclear power plants (NPPs) must be established and used by the licensee in such a way that the quality of safety relevant components is guaranteed for the completely designed lifetime of the NPP. This demands an extensive plant life management with special emphases on the knowledge of the degradation in material properties. The basic safety concept in Germany observes this circumstance. Lifetime extension of the German NPPs is an aim of the current valid coalition agreement of the German government. Operational extension of interim storage facilities requires, in comparison to the aging management system for NPP, an aging management system adapted to the Special circumstances of spent fuel storage casks. Extension of interim storage periods for spent fuel casks beyond the designed lifetime requires, in comparison to the components of an NPP, an increasing knowledge of material degradation with potential impact on cask integrity, e.g. leak tightness. Dry interim storage in Germany has been approved for 40 years. After that time, according to the present strategy, a final repository should be available. However, until now, such a final facility still does not exist, and the German exploration and licensing process is heavily delayed. Currently, discussions are continuing regarding further exploration of the Gorleben salt mine. There is willingness to overcome this situation that is clearly described in the available coalition agreement of the federal government. Anyway, however, the prediction is viewed; a repository for heat generating radioactive waste in Germany will not be available in the near future and may not be available when first storage facilities and casks reach their 40 years of approved lifetime, which will occur in ~25 years starting from now. Therefore, the question must be asked:
what has to be done with the existing storage casks in the interim facilities? May these casks be fit for continued use, with an extension of the storage period? One option is to have an aging management system, which creates enough information about the technical condition of safety relevant cask properties. This is the basis for safety evaluation for extended storage periods. In the present paper, possible aging mechanisms for high level waste storage casks are discussed, as well as the influence of the time dependent changes of the component properties.
Casks for the transport and storage of heat generating radioactive waste in Germany are normally provided with screwed lid systems, which are in most cases equipped with double jacket metal seals with an inner spring wire to provide long term resistance to the seal compression force. Preservation of the high sealing quality of those seals under operational and accidental stress conditions is essentially important to the safety of those casks. Relative displacements of the lid system surfaces caused by specific impact scenarios cannot be excluded and have to be evaluated with respect to a possible increase in the leakage rate.
To get representative data for such metal sealed lid systems, BAM has developed a special conceptualised flange system placed in an appropriate testing machine for relevant mechanical loading of the metal seals under static and cyclic conditions. Furthermore, the flange system enables continuous measurement of the standard helium leakage rate during each test.
The primary aim of the investigation is to identify the correlation between variation of installation conditions (axial displacements) caused by external loads and the standard helium leakage rate. An essential parameter in this case is the useable resilience ru of a metal seal under relevant stress conditions. The useable resilience ru is the vertical difference in the cross-section between the seal's assembling status and the point where the leakage rate, by means of external load relieving, exceeds the quality criterion of 10-8 Pa m3 s-1. Load relieving can instantly occur due to modification of the seal groove dimension caused by accident impacts and deformation of the lid system. Furthermore, component specific basis data for the development of finite element calculation models should be collected. In the tests, seals are subjected to static and cyclic loads. All tests are performed at ambient temperature.
This paper presents the test configuration, different test series and results of the current experiments. Typical load-displacement-leakage rate correlations are presented and discussed.