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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.
The special properties of high molecular weight polyethylene (HMW-PE) and ultra high molecular
weight polyethylene (UHMW-PE) result basically from their extreme chain lengths and their high
degree of crystallinity. As high-performance polymers, they are used for a variety of applications.
UHMW-PE in particular is often utilized for endoprothesis (due to its excellent slip and wear
properties) and due to its high hydrogen content as a neutron moderator in casks for storage and
transport of radioactive materials.
To prepare the material for instance for its use as a total joint replacement, it is exposed to radiation
for several reasons, such as sterilization and crosslinking, leading to partial improvement of the
mechanical properties (e.g. fracture toughness, crack propagation resistance, wear resistance) and
better chemical stability.
To be applicable for long term radiation shielding purposes for instance over a period of 40 years,
PE has to withstand any type of degradation affecting safety relevant aspects.
The scope of our investigation comprises an estimation of the radiation impact on the molecular and
supra molecular structure of two types of PE and to what extent these changes are detectable by
thermo-analytical (TA) methods, such as Differential Scanning Calorimetry (DSC), Thermo
Mechanical Analysis (TMA), Dynamic Mechanical Analysis (DMA) and Thermo Gravimetric
Analysis (TGA). Additionally FT-IR spectroscopy as well as density and gas sorption
measurements were carried out.
Due to the poor solubility of HMW-PE and UHMW-PE, some classical analytical techniques are
not applicable. But TA-methods represent a feasible approach to detect structural and
morphological features of these materials as well as changes caused by external influences, such as
thermal treatment and/or irradiation. With the combination of the applied TA-techniques it is
possible to distinguish between crosslinking and degradation.
Die Messung des dynamischen Speichermoduls mit der Dynamisch-Mechanischen-Analyse ermöglicht einen schnellen Überblick über das temperaturabhängige Verhalten von elastomeren Dichtungsmaterialien. Ein direkter Rückschluss von der so ermittelten Glasübergangstemperatur Tg auf die Versagenstemperatur einer Dichtung ist aber ohne zusätzliche Messungen bisher nicht möglich.
Mit den Ergebnissen des Druckverformungsrestes DVR und des DVRDMA ist eine ge-nauere Beschreibung der Tieftemperatureigenschaften und dadurch der Funktion von elastomeren Dichtungsmaterialien möglich. Messungen ergeben beispielsweise, dass sich das EPDM bei einer Temperatur von -40 °C laut der Dynamisch Mechanischen Analyse noch im gummielastischen Bereich befindet. Die DVRDMA-Werte zeigen eine Rückstellung um mehr als 40 % der Ausgangsdeformation in wenigen Minuten.
Mit derart detailliert bestimmten Eigenschaften lassen sich Rückschlüsse auf einsatzspezifische Anforderungen wie z. B. die Dichtwirkung in Abhängigkeit von Betriebstemperatur und mechanischer Belastungsgeschwindigkeit ziehen, so dass je nach Einsatzbedingungen für die Dichtungen eine geeignete Materialauswahl getrof-fen werden kann.
A new method for the evaluation of the low temperature properties of rubber materials is presented. The method emulates the standardized compression set measurement, which is frequently used for sealing materials, but can be performed within a considerably shorter time. The results are compared with the standard test and found to be qualitatively the same. Slight differences are discussed on the basis of the differences in the measurement procedures. Further data evaluation is done by fitting functions to describe the material behaviour.
In drop test scenarios related to assessing and licensing the storage procedure of spent fuel and high active waste, the casks under examination are generally not equipped with impact limiters. Hence, the extent of mechanical stresses in case of an assumed handling accident is largely affected by the ground properties of the reception hall floor in the specific storage facility.
Unlike conventional brittle foundation materials, damping concrete performs quite well in such applications as it features high stiffness as well as high energy absorption due to the filler pore volume. However, its damping ability is not sufficiently exploited in current finite element (FE) calculations due to a lack of advanced material models for simulating its impact response. An implementation of qualified concepts that account for plastic, strain rate dependent behavior requires additional information that has to be provided by systematic test series.
BAM recently started a research project to generate such data, subsequently to develop and to improve numerical methods for the analysis of impact limiters and damping foundation material and thus to optimize safety assessment tools for the design of transport and storage casks. A major part of this research concerns dynamic compression tests of variably shaped specimens conducted at a servo hydraulic 1MN impact testing machine as well as at a BAM facility for guided drop tests. This presentation focuses 100mm damping concrete cubes deformed vertically at constant rates under different constraint conditions. For example, a special fitting jig was constructed to subject the specimens to multi-axial loading. Thereby a deformation of 60% could be applied.
Simulation was conducted by FE code ABAQUS based on material models Concrete damaged plasticity and Crushable foam which both allow defining rate sensitive nonlinear stress-strain relations in compression beyond the classic metal plasticity approach.
Rubbers are widely used as main sealing materials for containers for low and intermediate level radioactive waste and as additional component to metal seals in spent fuel and high active waste containers. The save encapsulation of the radioactive container inventory has to be guaranteed according to legislation and appropriate guidelines for long term storage periods as well as down to temperatures of -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 rubbers are strongly temperature dependent. At low temperatures this is caused by the rubber-glass transition (abbr. glass transition). During continuous cooling the material changes from rubber-like entropy-elastic to stiff energy-elastic behaviour, that allows nearly no strain or retraction, due to the glass transition. Hence rubbers are normally used above their glass transition but the minimum working temperature limit is not defined precisely, what can cause problems during application. Therefore the lower operation temperature limit of rubber seals should be determined in dependence of the material properties.
The results of Differential Scanning Calorimetry (DSC) and Dynamic Mechanical Analysis (DMA) are combined with the results of standardized measurements as the compression set according to ISO 815. To reduce the test time of the standard tests a faster technique was developed.
Additionally, the breakdown temperature of the sealing function of complete O-ring seals is measured in a component test setup to compare it with the results of the other tests. The experimental setup 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. Some materials (seals and test sheets) were purchased from a commercial seal producer and some materials were compounded and cured at BAM in form of rubber sheets.
Ultra high molecular weight polyethylene (UHMW-PE) - due to its high hydrogen content - is used as neutron shielding material in casks for storage and transport of radioactive materials. Besides this, UHMW-PE - as a high-performance polymer - has been used for several years in medical technology due to its excellent slip and wear properties. Due to the special properties of UHMW-PE which result basically from its extreme chain lengths and its high degree of crystallinity, it is predestinated for the aforementioned applications.
In both cases, irradiation and its impact on the molecular structure of polyethylene play an important role. In the first case, irradiation exists as a by-product of inserting the radioactive material in the cask. Hence PE has to withstand any type of degradation affecting safety relevant aspects to be applicable for long term radiation shielding purposes for instance over a period of 40 years. In the second case irradiation is applied deliberately for purposes such as sterilization and crosslinking, leading to partial improvement of the mechanical properties (e.g. fracture toughness, crack propagation resistance, wear resistance) and better Chemical stability.
Specifically concerning their use in the field of medical technology, different types of UHMW-PE have been objects of numerous publications. It is generally accepted that two parallel and competitive processes, based on chain scission and reactions of Ccentered radicals and molecular fragments, occur in PE as a consequence of radiation: radical recombination accounts for crosslinking, together with some disproportionation, formation of low molecular weight fragments, and recrystallization. Furthermore, formation of oxygenated structures in the presence of traces of oxygen is an antagonist of the C-centered radicals. Radiation induced scission preferentially takes place in the amorphous phase and noncrystalline surface of the crystals. It is followed by folding of molecular fragments, crystallinity growth and increased perfection in the crystal lamellae [4, 5]. Chain scission results in shorter polymer molecules, fewer entanglements, and consequently, increased molecular mobility.
The scope of our investigation comprises an estimation of the radiation and thermal impact on the molecular and supra molecular structure of the two types of PE used for neutron shielding cask components. A further point which is worth to explore is to what extent these changes are detectable by thermo-analytical (TA) methods, such as Differential Scanning Calorimetry (DSC), Thermo Mechanical Analysis (TMA), Dynamic Mechanical Analysis (DMA) and Thermogravimetry (TG). Additionally FT-IR and solubility measurements have been performed.
In our studies we focused on the UHMW-PE material GUR 4120 which was y irradiated at RT and compared to the untreated material.
Rubbers are often used for seal applications due to their special material properties and easy use. In many applications the material is exposed to low temperatures during Operation. Therefore it is important to know the material behavior at low temperatures to determine the temperature ränge that allows a Safe Operation of the seal, e.g. in storage and transport Containers for radioactive materials.
The seal function of an elastomer is limited in temperature by the rubber-glass transition during which the material properties change from rubber-like to stiff and glass-like. For a given application this correlation is not trivial and therefore needs an in-depth investigation under consideration of the physical properties and the
application conditions.
In this work different analytical methods are used to characterize the material behavior at low temperature in the ränge of the glass-rubber-transition and are compared with the quality of Operation of a component which is here defined by the detected leakage rate.
Rubber is widely used as sealing material in various applications. In many fields the sealing function at low temperatures is necessary. Therefore the understanding of failure mechanisms is of high importance. Rubbers are normally used above their glass-rubber transition region but the minimum working temperature limit is not defined precisely. Therefore the lower operation temperature limit of rubber seals should be determined in dependence of the material properties. The results of Differential Scanning Calorimetry (DSC) and Dynamic Mechanical Analysis (DMA) are combined with the results of the standardized compression set according to ISO 815 respectively a modified test using the DMA equipment.
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.
Während des Transportes sind Behälter für hoch radioaktive Abfälle durch stoßdämpfende Bauteile vor Einwirkungen, die aus Unfallszenarien gemäß den IAEA Regularien resultieren können, weitestgehend geschützt. Nach dem Entfernen dieser Komponenten im Rahmen der Einlagerung ins Zwischenlager müssen Vorkehrungen getroffen sein, um Beanspruchungen der Behälter aus möglichen Handhabungsunfällen im Empfangsbereich zu reduzieren. Die Maßnahmen müssen vor allem darauf abzielen, die stoßdämpfenden Eigenschaften der potentiellen Aufprallflächen zu optimieren. Da Standardmaterialien für Fundamente nur ein geringes Energieabsorptionsvermögen aufweisen, wurde durch die Firma HOCHTIEF eine neuartige Betonmixtur entwickelt, bei der ein spezieller Leichtzuschlag zum Einsatz kommen. Zur Charakterisierung dieses sogenannten Dämpferbetons liegen Standardkennwerte vor sowie Messwerte aus Eindringversuchen, die zur Qualitätssicherung für jede Produktcharge durchgeführt werden. Das stoßdämpfende Potential des neuen Werkstoffs kann jedoch nur dann vollkommen ausgeschöpft werden, wenn die Energieabsorption in numerischen Simulationen der Behälterabstürze über die gesamte Belastungsdauer zuverlässig wiedergegeben wird. Für die Implementierung und Anpassung eines entsprechenden Materialmodelis in einem Finite Elemente (FE) Programm
sind Daten aus systematischen Druckversuchen mit Variation der relevanten Einflussgrößen erforderlich. An der BAM werden daher im Rahmen eines werkstoffübergreifenden Forschungsvorhabens zur Untersuchung von stoßdämpfenden Strukturen auch die Eigenschaften von Dämpferbeton experimentell untersucht und zugehörige numerische Methoden entwickelt. Der aktuelle Beitrag behandelt die Ergebnisse der ersten Projektphase, in der kubische Probekörper mit der Kantenlänge 100mm bei unterschiedlichen Lagerungsbedingungen statisch und dynamisch gestaucht wurden. In nachfolgenden Versuchen wird der Einfluß der Probengröße ermittelt sowie die Eignung der verwendeten Materialmodelle anhand realistischer Belastungssituationen validiert.
Versuchsprogramm.
Dry cask storage of spent fuel and high active waste front reprocessing is licensed and established in Germany for up to 40years so far. About 10years ago, the strategy has been shifted from centralized storage using facilities in Ahaus and Gorleben to cit-site storage facilities in Order to avoid immediate cask shipping from nuclear power plants. At present, several hundred casks are stored safeiy and without any major problem. BAM is highly involved in cask specific safety evaluations within the scope of licensing procedures as well as of quality assurance procedures during cask fabrication, loading and storage.
A major prerequisite for any cask storage license is a valid transport Type B license. Subsequently, cask transportability has to be ensured at any point during the entire storage period. So far, this requirement is met by continuous maintenance of the Type B license. Anyhow, IAEA Type B regulations do not consider permanently loaded storage casks that have the sole purpose of being finally shipped öfter decades of storage inducing ageing effects. No transport safety demonstration has to be performed on aged cask components.
Metal seals are in common use as an essential component for the leak tight closure of transport and storage casks for spent fuel and vitrified high active waste from reprocessing. They are placed between the massive monolithic cask body made of ductile cast iron or forged steel and the primary and secondary lids, which are fixed with screws around the lid circumference, in order to ensure long term safe enclosure of the radioactive cask inventory. Hereby, long term reliable pressure forces in combination with a tight surface contact are as important as well maintained seal and surface qualities and dry and clean conditions during seal assembly and operation. A few years ago BAM started systematic investigation on the long term seal behavior with re-spect to longer storage periods and seal behavior in accidental cask scenarios with dynamic de-formations of the seal groove geometry or short term drop in pressure force up to lid lifting. BAM has developed test flanges for seals with full scale cross section diameter but much small-er outer diameter to gain representative data for metal-sealed lid systems. They are placed in appropriate testing machines for relevant mechanical loading under static and dynamic condi-tions with the ability to measure the standard helium leakage rate continuously during each test phase. This paper focuses on BAM long term tests of different seal types with aluminum and silver jackets at three different temperatures of +20°C, +100°C and +150°C under static conditions over longer periods of time. Due to creeping effects, a reduction of the pressure force does ap-pear during loading and unloading depending on prior holding times. So far, test results of up to 2 years indicate a clear correlation between seal pressure forces and holding time, temperature and seal type allowing for extrapolating to much longer periods of time. The paper presents basic correlations, test and evaluation procedures as well as important provisional results and gives an outlook on further investigations.
In Germany the concept of dry interim storage of spent fuel and vitrified high active waste 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 guidelines of the German Reactor Safety Commission for dry interim storage of spent fuel. Currently part of the assessment process of the cask design for transport on public routes is to evaluate the suitability of the used materials with respect to their properties and their compatibility for possible transport periods. For transport on public routes during or after long term interim storage periods, it has to be ensured that the transport and storage casks fulfill the specifications of the transport approval or other sufficient properties which satisfy the proofs for the compliance of the safety objectives at that time. This paper describes the state-of-the-art technology in Germany and points out arising prospective challenges and which related questions have to be answered in future. Present research and knowledge concerning the long term behavior of transport and storage cask components (such as gaskets and shielding components) have to be consulted as well as experiences from interim cask storage operations. Challenges in the safety assessment are therefore i.e. the behavior 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 (aged package). Assessment methods for the material compatibility, the behavior of fuel assemblies and the aging behavior of shielding parts (e. g. influence of radiation) are further issues as well.
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.
Die mechanische Beanspruchung von Transport- und Lagerbehältern für radioaktive Stoffe gemäß den durch die IAEA vorgegebenen Prüfszenarien oder bei Unfällen, die während der Handhabung in einer kerntechnischen Anlage auftreten können, wird maßgeblich durch das Design der Stoßdämpfer und die Eigenschaften des jeweiligen Untergrundes beeinflusst. Da der Nachweis der Behälterintegrität und -dichtheit häufig an numerische Simulationen gekoppelt ist, sind für die sicherheitstechnische Auslegung der Konstruktion zuverlässige Informationen über das Energieabsorptionsvermögen der Werkstoffe und eine geeignete Umsetzung dieser Daten in FEM - Programme erforderlich. Die im Rahmen von Falluntersuchungen bei der BAM festgestellten, teilweise erheblichen Abweichungen zwischen experimentellen und berechneten Größen sind entsprechend darauf zurückzuführen, dass die zur Verfügung stehenden numerischen Verfahren das komplexe Verhalten der stoßdämpfenden Strukturen
nicht ausreichend präzise wiedergeben. Hiervon besonders betroffen sind Bauteile aus Holz und Polyurethan-Schaum (PU-Schaum), die zur Konstruktion von Behälterstoßdämpfern für die Transportkonfiguration eingesetzt werden, sowie Dämpferbeton, der in ausgewählten Bereichen im Fundament von Standort-Zwischenlagern eingebaut wird. Um die zugehörigen Materialmodelle weiter zu entwickeln und die dafür erforderliche Datenbasis zu schaffen, hat die BAM vor knapp zwei Jahren das vom BMBF geförderte Forschungsvorhaben ENREA (Entwicklung rechnerischer Analysemethoden für stoßdämpfende Strukturen beim Anprall oder Absturz von Abfallgebinden) gestartet. Wesentlicher Bestandteil ist ein systematisches Versuchsprogramm, bei dem die drei genannten Werkstoffe statisch und dynamisch hohen Druckbelastungen ausgesetzt werden. Relevante Versuchsparameter sind, neben der Dehnrate, die Temperatur und Lagerungsbedingungen sowie die Orientierung des Werkstoffes hinsichtlich der Belastungsrichtung. Dieser Beitrag präsentiert die wichtigsten Ergebnisse aus der ersten Versuchsphase, die durch weggesteuerte Versuche mit konstanten Prüfgeschwindigkeiten von 0,02 mm/s und 3000 mm/s gekennzeichnet ist. Darüber hinaus wird die Verwertung dieser Daten zur Anpassung von Materialmodellen auf der Grundlage von Nachrechnungen gezeigt, wobei die Möglichkeiten und Grenzen der verwendeten Konzepte Umrissen werden. Aufgrund des Umfangs, den die Versuche mit Holzwerkstoffen einnehmen, und des erforderlichen Aufwandes für die numerische Modellierung werden die entsprechenden Maßnahmen und Ergebnisse in einem eigenständigen Beitrag auf der KONTEC vorgestellt.
The method for the determination of compression set values with a Dynamic Mechanical Analysis (DMA) setup at low temperatures, which was presented previously, allows a much faster and readily automated procedure than the standardized compression set test according to ISO 815-2. This method is applied to a series of different elastomeric materials that are commonly used for sealing applications. The results of the compression set test are compared with results from thermal analysis to allow an in depth comparison of the material behaviour at low temperatures.
Furthermore, a comparison between two EPDM materials is presented. These materials show very similar properties determined by thermo analytical methods such as Differential Scanning Calorimetry (DSC) and Dynamic Mechanical Analysis (DMA) but differ clearly in their compression set behaviour. This comparison shows the importance and value of information of the compression set test in addition to thermal analysis to judge the behaviour of sealing materials and confirms the relevance of the new compression set test method for the investigation of low temperature properties of elastomers.
The molecular dynamics of liquid-crystalline polymethacrylates with biphenyl in the side group forming a highly ordered smectic E phase at low temperatures is investigated by dielectric spectroscopy (DS). Although no glass transition is found by DSC, DS detects a relaxation in the smectic E phase resembling to glassy dynamics. The temperature dependence of its relaxation rate is Arrhenius like at low temperatures, which changes to a VFT law at higher temperatures. Such a behavior is found to be characteristic for glassy dynamics in confining space. It is discussed, considering the structure of the polymers as nanobiphasic consisting of liquid-crystalline layers while the backbones fill the interlayer space. A comparison is made to polymethacrylates having phenyl benzoate as mesogen.