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Eingeladener Vortrag
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Due to delays in the siting procedure to establish a deep geological repository for spent nuclear fuel and high level radioactive waste as well as in construction of the already licensed Konrad repository for low and intermediate level radioactive waste, extended periods of interim storage become more relevant in Germany. BAM is involved in most of the cask licensing procedures and especially responsible for the evaluation of cask-related long-term safety issues.
The long-term performance of elastomer seals for lid systems of transport and storage casks, whether used as auxiliary seals in spent fuel casks or as primary seals for low and intermediate level waste packages, is an important issue in this context. The polymeric structure of these seals causes a complex mechanical behavior with time-dependent sealing force reduction.
The results of a comprehensive purpose-designed test program consisting of basic compression and tension tests as well as relaxation tests on unaged specimens of representative types of elastomers (fluorocarbon rubber (FKM) and ethylene propylene diene rubber (EPDM)) at different temperatures and strain rates are presented. They were used to identify the constitutive behavior and to obtain parameters for finite element material models provided by the computer code ABAQUS®. After estimating the influence of uncertainties such as Poisson’s ratio and friction coefficient by sensitivity analyses, the chosen parameters had to prove their suitability for the finite element simulation of the specimen tests themselves.
Based on this preliminary work the simulation of a specific laboratory test configuration containing a typical elastomer seal with circular cross section is presented. The chosen finite element material model and the implemented parameters had to show that they are able to represent not only the specimen behavior under predominantly uniaxial load but also the more complex stress states in real components. Deviations between the measured and calculated results are pointed out and discussed.
For the consideration of long-term effects in the simulation of elastomer behavior, test results of aged specimens are needed. First information about a new test program, started recently and planned to provide these data, are given.
Due to delays in the site-selection procedure to establish a deep geological repository for spent nuclear fuel and high level waste and in construction of the already licensed Konrad-repository for low and intermediate level waste without heat generation, extended periods of interim storage become more relevant in Germany. BAM is involved in most of the cask licensing procedures and especially responsible for the evaluation of cask-related long-term safety issues.
The long-term performance of elastomer seals for lid Systems of transport and storage casks whether used as auxiliary seals in spent fuel caslcs or as primary seals for low and intermediate level waste packages is an important issue in this context (Jaunich, 2013; Jaunich, 2014; Kömmling, 2015). The polymeric structure of these seals causes a complex mechanical behaviour with time-dependent elasticity reduction and loss of elastic recovery.
The paper presents first results of a comprehensive test Programme consisting of several static and dynamic mechanical short- and long-term tests which have been carried out at BAM on specimens made of representative types of elastomers, fluorocarbon rubber (FKM) and ethylene propylene diene rubber (EPDM). The investigation of the test results used to identify material models and their Parameters as well as the development of two finite element models for the numerical Simulation of tension and compression tests using the finite element code ABAQUS® are described. The calculation results are presented in comparison to the test results. The influence of important material and test parameters was investigated and discussed in sensitivity analyses.
Testing and numerical simulation of elastomeric seals under consideration of time dependent effects
(2016)
Due to delays in the siting procedure to establish a deep geological repository for spent nuclear fuel and high level waste and in construction of the already licensed Konrad repository for low and intermediate level waste, extended periods of interim storage will become more relevant in Germany. BAM is involved in most of the cask licensing procedures and is responsible for the evaluation of cask-related long-term safety issues. Elastomeric seals are widely used as barrier seals for containers for low and intermediate level radioactive waste. In addition they are also used as auxiliary seals in spent fuel storage and transportation casks (dual purpose casks (DPC)).
To address the complex requirements resulting from the described applications, BAM has initiated several test programs for investigating the behavior of elastomeric seals. These include experiments concerning the hyperelastic and viscoelastic behavior at different temperatures and strain rates, the low temperature performance down to -40°C, the influence of gamma irradiation and the aging behavior.
The first part of the paper gives an overview of these tests, their relevant results and their possible impact on BAM’s work as a consultant in the framework of approval and licensing procedures.
The second part presents an approach of the development of a finite element model using the finite element code ABAQUS®. The long-term goal is to simulate the complex elastomeric behavior in a complete lid closure system under specific operation and accident conditions.
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.
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.
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.
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.
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.
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.
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.
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.
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.
THz and Mid IR Fourier transform spectroscopy on polyethylene irradiated with Gamma- Co60 radiation
(2014)
THz and mid IR spectroscopy of high molecular PE (HMW) and ultra high molecular PE (UHMW) reveals modifications of the molecular structure induced by γ-Co60 radiation. UHMW-PE and HMW-PE can be distinguished. The integral absorption in the B1u THz-region can quantitatively describe the amorphization of crystallinity. The formation of trans vinylene unsaturations and the decay of vinyl can be followed by mid IR spectroscopy
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.
For many sealing applications rubbers are applied due to their special material properties and easy use. In many applications, e.g. in aviation, traffic or process technology the material can be exposed to low temperatures during Operation. Therefore it is important to know the material behaviour at those low temperatures to determine the temperature range that allows a safe Operation of the seal. As rubbers are 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, a comprehensive elastomer investigation program is run at BAM. This program comprises investigations of elastomer overall performance, durability, influence of gamma irradiation and low temperature behaviour.
In this paper we focus on the behaviour of elastomer seals at low temperatures with regard to potential decrease of leak-tightness as material properties of rubbers are strongly temperature dependent. But additionally to the investigation presented in the past which considered the material properties of new materials and the seal behaviour under purely static conditions [1, 2] we now focus on irradiated materials and on the sealing performance after a fast partial release of the compressed seal.
For the investigations different materials were used, e.g. fluorocarbon (FKM) and ethylenepropylene-diene (EPDM) rubber. To determine the effect of gamma irradiation some samples were irradiated and studied by several thermo-analytical methods and compression set. For the investigation of the seal performance under non static conditions we decided to design a new measurement setup which allows for a small flange deflection and simultaneous leakage rate measurement at low temperatures.
Fourier-Spektroskopische Untersuchungen von hochmolekularem Polyethylen (HMW-PE) und ultrahochmolekularem Polyethylen (UHMW-PE) im Mittleren - und Fernen Infrarotbereich können Veränderungen der molekularen Strukturen nachweisen, die durch Co60 γ-Strahlung und Rekristallisationsprozesse initiiert werden. UHMW-PE und HMW-PE sind im gewählten IR-Bereich unterscheidbar. Die integrale Absorption der B1u – Gitterschwingungen im Fernen Infrarotbereich (THz-Bereich) ermöglichen die quantitative Beschreibung des Kristallinitätsgrades und dessen Abbau. Die Bildung ungesättigter Vinylengruppen und der Abbau ungesättigter Methylengruppen können im Mittleren Infrarotbereich nachgewiesen werden.
Mechanical drop test scenarios for Type B (U) packages according to the IAEA regulations have to be carried out onto the so-called “unyielding target” (usually with cask impact limiters) and onto the puncture bar respectively. They are predefined and do not require any further investigation of scenarios that really could happen on transportation routes. Cask accident scenarios in the framework of approval procedures for interim storage sites are derived from a detailed analysis of the handling procedures necessary from arrival of cask at the site to its storing position.
In that case, casks are usually handled without impact limiters. Dependent on possible drop heights, drop positions and floor properties, conservative cask accident scenarios are derived for further safety proofs.
According to the mechanical assessment concept of the considered approval procedure numerical calculations have to be provided by the applicant to demonstrate mechanical cask safety. Stresses and strains in the cask body as well as in the lid System have to be identified and assessed. Using the example of a 3-mvertical-drop of a transport and storage cask for spent fuel elements onto the floor construction made of damping concrete covered by screed, BAM developed a finite element model. The finite element code ABAQUS/Explicit™ was used. Results of experimental investigations are not available. Therefore parameter studies are necessary to identify the sensitivity of the finite element model to significant Parameters and to verify the finite element models according to the requirements of the Guidelines for the Numerical Safety Analyses for the Approval of Transport and Storage Casks for Radioactive Materials (BAM GGR-008).
The paper describes the modeling of the material behavior and attachment of bottom side cask components. Questions concerning the modeling of a crack length limiting reinforcement in the screed layer are discussed. The influence of the mesh density of the screed layer and its strength is considered as well. Finally, the developed finite element model can be used for a numerical safety assessment. It can help to understand the complex mechanisms of the interaction between the cask components and floor construction.
According to the relevant guidelines and regulations, the safe enclosure of radioactive Container contents has to be guaranteed for long storage periods as well as down to temperatures of -40 °C during transportation. As rubbers are widely used as the 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, a comprehensive eiastomer investigation Programme is in place at BAM. This Programme comprises investigations of overall eiastomer performance, durability, influence of gamma irradiation and low temperature behaviour.
In this paper we focus on the behaviour of eiastomer seals at low temperatures with regard to the potential increase in leakage as material properties of rubbers are strongly temperature-dependent. During continuous cooling, the material behaviour of elastomers changes in the rubber-glass transition temperature ränge from rubberlike entropy-elasticity to stiff energy-elasticity, allowing for almost no strain or retraction. Hence rubbers are normally used above their rubber-glass transition but the minimum limit at which they work has not been defined precisely. For the investigations, fluorocarbon (FKM) and ethylene-propylene-diene (EPDM) rubbers were selected, as they are often used in radioactive waste Containers. The elastomers were studied using several thermoanalytical methods and compression set. The results were compared with component tests to determine the temperature at which the sealing function of O-rings made of eiastomer breaks down. In addition to these results, under static conditions we designed a new measurement set-up which allows for a small deflection of the flange and simultaneous leakage rate measurement at low temperatures.
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.
High and ultra-high molecular weight polyethylenes are high performance materials, which are predestined for a wide range of applications due to characteristics like high density, low weight, good dimensional stability, high chemical resistance, and high hydrogen content. These polymers are used in two demanding areas: as implant material in medical technology (only ultra-high molecular weight polyethylenes) and as a component for neutron shielding purposes in casks for storage and transport of radioactive waste. In the medical field (joint replacements) as well as during neutron radiation shielding application, high and ultra-high molecular weight polyethylenes are exposed to gamma irradiation: in the first case requested as sterilization process and for surface-crosslinking and in the second case existing as a side effect of inserting the radioactive material in the cask.
Given that polyethylene as shielding material 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, the durability of the material is of special interest. High molecular weight polyethylene (HMW-PE; LUPOLEN 5261Z; Lyondell Basell) and ultra-high molecular weight polyethylene (UHMW-PE; GUR 4120; Ticona) were subjected to gamma radiation and afterwards thermally treated. The gamma doses used are in the range of 50 to 600 kGy and irradiation takes place at RT using a Co-60 source. The planned thermal treatment will take place at a temperature of 125 °C for periods of minimum 30 days and maximum of five years. With the applied conventional analytical techniques it is possible to detect structural changes of both types of polyethylene induced by gamma irradiation and certainly of thermal treatment. Through gamma irradiation melting temperature, crystallinity, and density, respectively increased. Furthermore both polyethylenes get oxidized and cross-linked. With regard to the special application as neutron radiation shielding material in casks for storage and transport of radioactive materials, the impact of irradiation lead to changes of material properties. A consolidated view indicates that the detected changes of the irradiated (U)HMW-PE are not safety relevant for long-term neutron radiation shielding purposes over a period of 40 years in Germany.
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.
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.
In many fields the function of seal materials is required at low temperatures. Therefore the understanding of failure mechanisms at low temperatures is of high importance. In some applications elastomeric seals are used in environments with increased irradiation backgrounds, as e.g. in containers for radioactive waste. This paper reports on the influence of gamma irradiation on the low temperature properties of different fluorocarbon rubber (FKM) materials.
The samples were irradiated with gamma doses of up to 600 kGy and the induced changes of material properties were tested by methods sensitive to the rubber-glass transition, like DSC and DMA. Additionally, compression set measurements were performed to give information about recovery behaviour at low temperatures.
Elastomer seals are widely used as barrier seals in containers for low and intermediate level radioactive waste and for spent fuel transportation casks. In addition, they are also used for spent fuel storage and transportation casks (dual purpose casks (DPC)) as auxiliary seals to allow leakage rate measurements of metal barrier seals for demonstration of their proper assembling conditions. Depending on the area of use, the rubber materials have to demonstrate proper sealing performance with regard to mechanical, thermal, and environmental conditions as well as irradiation during the entire operation period. Concerning DPC, degradation effects should be limited in a way that, for example, effects from potentially released decomposition elements may not harm e.g. metal barrier seals. Leakage rate measurements should be possible also after long interim storage periods prior to subsequent transportation.
Because of the complex requirements resulting from the various applications of containers for radioactive waste and spent nuclear fuel, BAM has initiated several test programmes for investigating the behaviour of elastomer seals. In this contribution the current status is described and first results are discussed.
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).
Rubber is widely used as sealing material in various applications. In many fields the function of seal materials at low temperatures is necessary. 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 behaviour 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. In the past we investigated the material properties and sealing behaviour of elastomeric seals at low temperatures. Additionally we started to study the effect of a small partial release of elastomer seals at low temperatures. To study the influence of dynamic events on seal performance and to enhance the understanding of occurring seal failure, a setup for a fast partial seal release was designed. In this contribution we focus on the correlation of material properties and component behaviour under different application conditions. It is desired to widen the understanding of the process of seal failure at low temperature.
In technical applications, static seals are sometimes also subjected to dynamic loadings. Therefore, the leakage behaviour under dynamic conditions has to be evaluated as well. For this purpose, FKM elastomer seals have been tested by using newly designed equipment that allows for rapid partial release of the seal and simultaneous leakage rate measurement at a wide range of test temperatures. Furthermore, material characterisation was done by using Dynamic Mechanical Analysis, Differential Scanning Calorimetry and Compression Set. It was shown that, under static conditions, the leakage rate increased significantly during cooling at temperatures around 18 K lower than the glass transition range. On reheating, the seal’s functionality was restored in the high temperature region of the glass rubber transition. In the subsequent dynamic release tests, that comprised a reduction of the seal compression within 1 s from 25 % to 23 %, increased leakage rates were observed in the high temperature region of the glass transition range. It was shown that the temperature that is critical for increased leakage is significantly lower under static conditions compared to dynamic conditions. The obtained leakage rates for static tests and dynamic release tests at different temperatures were analysed with reference to results of the material characterisation.
Both chain scission and crosslinking reactions occur during ageing of EPDM rubber. However, with many conventional polymer analysis methods such as hardness and DMA, it is hardly possible to obtain information about the contribution of each reaction type to the measured data. For example, hardness and Tg both increase during ageing of EPDM, indicating crosslinking during ageing, but it is not clear whether this is partly counterbalanced by chain scission reactions which would lower hardness and Tg. An indication that chain scission reactions probably counteract the hardness or Tg increase by crosslinking is given by Compression Set (CS) measurements. CS exhibits a higher change than hardness or Tg, as CS increases additively through both chain scission and crosslinking reactions. In order to elucidate the share of chain scission reactions in the total degradation, a method testing relaxation and recovery behaviour using DMA equipment was applied. The method revealed the strong influence of chain scissions, leading to more pronounced relaxation and higher residual strain after compression.
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.
The Bundesanstalt für Materialforschung und –prüfung (BAM) is a federal institute for materials research and testing in Germany and has been involved in the qualification and safety evaluation procedures of metal seals from the early beginning of the interim storage licensing procedures for radioactive materials, stored in dual purpose casks. Regarding this subject, BAM investigates the long-term behavior of metal seals under the influence of temperature using experimental data and analytical approaches. The development of numerical models is in progress as well. Systematic experimental investigations performed by BAM indicate a continuous decrease of the remaining seal force and the usable resilience considering the leak tightness. Hence, there is a fundamental interest of describing time and temperature dependency to gain predictable values for the long-term behavior and to achieve reliable results with help of short-term tests.
The paper gives an overview about the sealing principle, test program and test results of metal seals of the type HELICOFLEX® HN200. The aging effect, respectively the long-term behavior in dependency of time and temperature, are introduced for two different outer liner materials, aluminum and silver.
Discoloration Effects of High-Dose gamma-Irradiation and Long-Term Thermal Aging of (U) HMW-PE
(2017)
Two polyethylene types with ultra-high (UHMWPE) and high molecular weight (HMW-PE) used as neutron radiation shielding materials in casks for radioactive waste were irradiated with doses up to 600 kGy using a 60Co gammasource. Subsequently, thermal aging at 125∘C was applied for up to one year. Degradation effects in the materials were characterized using colorimetry, UV-Visspectroscopy, IR spectroscopy, and DSC. Both materials exhibited a yellowing upon irradiation.The discoloration of UHMW-PE disappeared again after thermal aging.Therefore, the yellowing is assumed to originate fromannealable color centers in the formof free radicals that are trapped in the crystalline regions of the polymer and recombine at elevated temperatures. For the antioxidantcontaining HMWPE, yellowing was observed after both irradiation and thermal aging. The color change was correlated mainly to decomposition products of the antioxidant in addition to trapped radicals as in UHMW-PE. Additionally, black spots appeared after thermal aging of HMW-PE.
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.
Einfluss der Alterung auf dichtungsrelevante Eigenschaften von FKM-, VMQ- und EPDM-Elastomeren
(2017)
Da Elastomere in vielfältigen Dichtungsanwendungen eingesetzt werden und dabei teilweise großen Einfluss auf die Funktionsfähigkeit und Sicherheit haben, ist der Einfluss der Alterung auf dichtungsrelevante Eigenschaften relevant. Eine strukturierte Untersuchung des Einflusses von verschiedenen Mischungsrezepturen auf die Bauteileigenschaften, das Alterungsverhalten und die Funktion wird vorgestellt.
For many sealing applications low temperature performance is required. The overall understanding of the relevant influences on low temperature performance of rubber seals are summarized and the currently running investigations described.
The correlation of the physical material properties with seal performance is studied. This includes as well purely static sealing applications as the performance during/after fast partial relief of seals at low temperatures.
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.
Elastomer seals are widely used as barrier seals in containers for low and intermediate level radioactive waste. In addition, they are also used in waste fuel storage and transportation casks as auxiliary seals. Depending on the area of use, the rubber materials have to demonstrate proper sealing performance with respect to mechanical, thermal and environmental conditions as well as irradiation during the entire operation period. A fundamental understanding of the structure property relationship and their changes during aging can help to evaluate the long-term sealing performance.
In the present study, specific materials are investigated to study the structure-property and seal performance-correlation. Fluoro-elastomer (FKM), silicone rubber (VMQ) and ethylene propylene diene rubber (EPDM) were chosen as base rubbers. Comparable mechanical properties for these seals, especially in terms of a comparable compression behavior were achieved by careful control of base rubber formulation, i.e., by opting for the right filler and its concentration, amount of crosslinking chemicals, and with the assistance of process oils. Moreover, with the same rubber, similar mechanical properties were achieved by varying the filler concentration and crosslinking degree, which shall enable to correlate the particular influence on the structure property dependency of the seals in detail. The materials are investigated under pristine and aged conditions to evaluate the influence of aging, e.g. on the stress relaxation or recovery behavior. These values appear to be suitable parameters to judge the expected sealing performance.
Due to the electrically conducting nature of some fillers used to reinforce rubbers (such as carbon blacks, carbon nanotubes (CNTs), Graphene, etc.) it is possible to obtain current information about mechanical and visco-elastic properties by monitoring the electrical conductivity or resistivity. A simple relation that relates electrical resistance with mechanical stress was derived and the stress values were theoretically predicted from the electrical resistance values, which showed good correlation with experimental results.
In Germany, for the transport and storage of spent nuclear fuel, casks with double closure lid systems are used, which are equipped with Helicoflex® metal seals. The original interim storage period for these casks was planned to be 40 years. However, recent political developments indicate that a storage time of more than 80 years might be necessary. Therefore, the current storage licenses have to be renewed in due course, which requires extended knowledge of the long-term behaviour of all cask components.
At the Bundesanstalt für Materialforschung und -prüfung (BAM), metal seals have been investigated after ageing at temperatures between room temperature and 150 °C for up to 7 years. At regular intervals the seals have been tested for leakage rate as well as for their mechanical behaviour. From these tests pronounced influence of ageing could be shown which results in the decrease of the seal force and the useable resilience. The main reason attributed to these performance changes is the increasing permanent deformation of the outer layer of the seal due to creep. So far, an explicit analytical description of the long-term behaviour that could be used for predictions exceeding the tested ageing times and temperatures was not suitable.
In addition to the component tests that were already conducted, a comprehensive investigation programme has been started to describe the mechanical behaviour of the individual seal components.
The individual seal components are tested regarding different material characteristics including creep, deformation and microstructural properties. The comparability of the material characterization is ensured by comparing the basic raw material of the specimen with the actual component material.
Furthermore, detailed investigations of the time and temperature dependent deformation behaviour are realized by ageing seal segments at multiple temperatures for different periods of time and employing standardized tests.
By analysing the acquired data in combination with the ongoing long-term component tests a dataset for analytical prediction of the long-term behaviour of the seals is intended for an extended period of time under a certain temperature regime.
The German nuclear waste management strategy consists of dry interim storage of spent fuel inside dual purpose casks and its subsequent direct final disposal in a deep geological repository. Interim storage is limited to 40 years so far, but will have to be extended until repository site selection and operation is concluded, potentially up to 100 years. In this context, research on the long term performance of safety relevant cask components and fuel rod integrity during such extended periods of time is of outmost importance. The barrier function of the fuel cladding depends on its integrity under operational and accidental conditions along with storage and subsequent transportation and is mainly affected over time by altering of the cladding microstructure and by thermo-mechanical conditions during reactor operation and subsequent wet and dry storage.
This paper focuses on failure mechanisms regarding cladding embrittlement caused by physical phenomena concerning hydrogen dissolution and precipitation of hydrides in the zirconium matrix. Within this context, potential cladding integrity issues under extended interim storage conditions followed by transportation are emphasized.
Delayed hydride cracking (DHC) is a well-known time-dependent temperature-activated phenomenon failure mechanism of the fuel cladding during reactor operation. The phenomenon consists of hydrogen diffusion and hydride precipitation at the tip of an initial crack and the propagation of the crack to an approximate distance equal to the length of the hydride. This failure mechanism is temperature-activated phenomenon and enhances along with thermal cycling of the fuel cladding, e. g. during reactor shutdowns. DHC shows limited relevance under quasi static storage conditions with continuously lowering temperatures. However, the literature points that DHC may occur when the temperature during storage decreases to a certain level after some decades and in combination with stress concentrations in the cladding material.
When spent fuel is transferred to dry storage by vacuum drying, the cladding temperature raises up to peak temperatures of ~370°C. Under these conditions, hydrides dissolute into the zirconium matrix up to the solubility limit defined by the peak temperature and this amount of hydrogen can precipitate in a radial re-oriented fashion due to the temperature decrease during storage. Cladding materials with radially precipitated hydrides show significant embrittlement. Radially oriented hydrides are perpendicularly oriented to hoop stresses representing the most critical configuration. Brittle failure of the cladding then occurs by crack propagation through radially oriented hydrides and finally through the zirconium matrix. The susceptibility to radial hydride precipitation depends on cladding material type and microstructure, hydrogen content, pre-drying hydride distribution, irradiation conditions, and temperature and stress histories during drying and storage operations.
This paper addresses major considerations concerning spent fuel cladding embrittlement due to hydride precipitation with regard to the boundary conditions of dry spent fuel storage in Germany. Analytical, numerical, and experimental approaches are to be discussed by BAM in order to identify the specific needs for future R&D work in that area with the purpose to provide the necessary data base for proper safety demonstration and evaluation along with future extended storage licensing procedures.
Transport and storage of radioactive materials are performed in countries with policy of either closed or open nuclear fuel cycle. The related technologies have been established by accumulation of experiences and researches including demonstrative tests using full scale or scale models and analyses. Those are essential before commercialization, but are often costly and time consuming. Such demonstrative works should not be repeated meaninglessly, but can be shared through this kind of book and used by readers and the future generations to advance the technology effectively. This book systematically provides findings from lots of valuable researches on safety of transport and storage of radioactive materials under normal and accident conditions that have an impact on basis of safe regulations, designs, and operations.
Experimental and numerical studies of shock absorbing materials for containers for radioactive waste
(2012)
Aufgrund ihrer einfachen und zuverlässigen Anwendung werden Elastomere für viele Dichtungsaufgaben eingesetzt. In vielen Anwendungsbereichen, wie z.B. Verkehr, Luftfahrt und Verfahrenstechnik, können während des Einsatzes tiefe Temperaturen auftreten, bei denen die Funktionsfähigkeit der Dichtung erhalten bleiben muss. Daher ist die Untersuchung des Verhaltens von Elastomerdichtungen bei tiefen Temperaturen wichtig, um ihren Temperatureinsatzbereich nach unten abzugrenzen und dadurch einen verlässlichen Betrieb zu sichern. Ziel dieser Arbeit ist es, den sicheren Einschluss von gefährlichen Gütern unter verschiedenen Umgebungsbedingungen und über lange Zeiten zu ermöglichen bzw. die Materialauswahl entsprechend zu steuern.
To achieve the required tightness levels of Containers for low and intermediate level radioactive wastes rubbers are widely applied as main sealing materials. The save encapsulation of the radioactive Container contents has to be guaranteed according to legislation and appropriate guidelines for long storage periods as well as down to temperatures of-40 °C during transportation.
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 influenced by temperature. 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. Therefore, rubbers are normally used above their glass transition but the minimum working temperature limit is not defrned precisely, what can cause problems during application. The temperature ränge where full functionality is possible is strongly dependent on the application conditions and the material.
For this investigation mainly ethylene propylene diene (EPDM) and fluorocarbon rubbers (FKM) were selected as they are often used for radioactive waste Containers.
Differential Scanning Calorimetry (DSC) and Dynamic Mechanical Analysis (DMA) are typically used for the determination of the temperature ränge of the glass transition process. The standardized compression set measurement according to ISO 815 is common for investigation of rubber sealing materials as the test simulates the seal behaviour after release. To reduce the test time of the Standard tests a faster technique giving the same information 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 model was developed that allows calculating the minimum working temperature limit of a seal by combining the results of the applied methods.
Langzeituntersuchungen an Metalldichtungen mit innen liegendem Federkern und doppelter Ummantelung
(2013)
In Deutschland werden in Transport- und Lagerbehältern (TLB) wärmeentwickelnde radioaktive Abfälle gegenwärtig über einen Zeitraum von bis zu 40 Jahren zwischengelagert. Aufgrund der Situation der noch nicht abgeschlossenen Endlagersuche werden hier möglicherweise Verlängerungen in Betracht zu ziehen sein. Im Deckeldichtsystem der TLB werden in der Regel Metalldichtungen vom Typ Helicoflex® eines französischen Herstellers verwendet, die aus einem innen liegenden Spiralfederkern und zwei Ummantelungen bestehen. Die Ermittlung der Fliess- und Relaxationseigenschaften der Dichtungskomponenten über den vorgesehenen langen Betriebseitraum sind vor dem Hintergrund des Erhalte eines geforderten hohen Dichtniveaus ein wichtiger Untersuchungsgegenstand.
Rubbers are widely used as sealing material in various applications. In many fieldsthefunction of seal materials at lowtemperatures is required. Therefore the understanding of faiiure mechanisms that lead to leakage at low temperatures is of high importance. 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 results of standardized measurements as the compression set according to ISO 815. To reduce the test time of the Standard tests a faster and more efficient technique was developed and applied. In addition the breakdown temperature of the sealing function of O-ring seals at lowtemperatures is measured in a component test Setup in dependence of the material and the degree of compression.
In Germany dual purpose casks for spent nuclear fuel (SF) or high level radioactive waste (HLW) are used for safe transportation and interim storage. Key safety issues in both fields are the safe enclosure of the radioactive material, the safe removal of decay heat, securing nuclear criticality safety, limitation of radiation exposure to acceptable levels and keeping it as low as reasonable achievable (ALARA principle).
Whereas these safety requirements during transportation are ensured by the Type-B(U)-design testing and approval procedure on basis of internationally agreed IAEA (International Atomic Energy Agency) requirements storage licenses are issued on national and site specific safety analyses.
This paper presents experiences from recent interim storage safety evaluation and licensing procedures in Germany on basis of a Type-B(U) certified cask designs concerning specific differences from Operation and accident conditions inside the storage facility. The focus is laid on the interaction of cask and building structures with regard to shielding, heat removal and accident analyses including aircraft crash. Basic safety is assured by thick-walled metal casks with monitored double lid Systems. They also reduce radiation to levels where workers can safely operate and maintain the casks inside the storage facility. The storage building e. g. provides additional shielding and protection against extemal hazards depending on the building construction. In addition, the storage building helps to reduce radiation levels at the boundary of the storage site well below regulatory limits given by the German Radiation Protection Ordinance (StrSchV).
Existing spent nuclear fuel (SF) and high active waste (HAW) management policies and practices worldwide are the result of past presumptions that sufficient reprocessing and/or disposal capacity would be available in the near term. Consequently, in the past many countries have developed specific solutions for different periods of time due to their individual national nuclear policies.
In Germany the concept of dry interim storage in dual purpose metal casks before disposal is being pursued for SF and HAW management and transport and storage licenses have been issued accordingly. The current operation licenses for existing storage facilities have been granted for a storage period of up to 40 years. This concept has demonstrated its suitability for over 20 years so far. Relevant safety requirements haven been assessed for the short-term as well as for the long-term for site-specific operational and accidental storage conditions. But in the meantime significant delays in the national repository siting procedure occured which will make extended storage periods necessary in the future.
This paper describes the current situation in Germany with regard to dry cask storage and focuses on current perspectives considering regulatory, technical, and scientific aspects for storage license renewal. Since there is one case of a storage license limitation to only 20 years due to administrative reasons, first experience is currently gathered in case of an expiring storage license. Subsequent license options have been pursued intensively including the extension of the initial storage license as well as shipping all casks to another storage facility considering an extended storage period at that storage facility as well. All safety relevant aspects have to be reviewed on basis of the current state-of-the-art which might be different from the initial safety demonstrations. That includes new safety assessment standards as well as improved knowledge base. Major issues are e.g. improved accident scenario analyses, assessment methods, and consideration of aging effects from previous operation periods. Inspection programs with respect, e.g. to bolts and seals to verify leak-tightness and lid screw pre-stress have been initiated to demonstrate proper cask conditions for extended storage as well as transportation to another storage facility.
Existing spent nuclear fuel (SF) and high active waste (HAW) management policies and practices worldwide are the result of past presumptions that sufficient reprocessing and/or disposal capacity would be available in the near term. Consequently, in the past many countries have developed specific solutions for different periods of time due to their individual national nuclear policies.
In Germany the concept of dry interim storage in dual purpose metal casks before disposal is being pursued for SF and HAW management and transport and storage licenses have been issued accordingly. The current operation licenses for existing storage facilities have been granted for a storage period of up to 40 years. This concept has demonstrated its suitability for over 20 years so far. Relevant safety requirements have been assessed for the short-term as well as for the long-term for site-specific operational and accidental storage conditions. But in the meantime significant delays in the national repository siting procedure occurred which will make extended storage periods necessary in the future.
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. According to appropriate guidelines and regulations safe enclosure of the radioactive container contents has to be guaranteed for long storage periods as well as down to temperatures of -40 °C for transportation. Therefore the understanding of seal behavior is of high importance.
In this paper we focus on the behavior of elastomer seals at low temperatures with regard to poten-tial decrease of leak-tightness. In addition, changes in material properties due to aging effects over long periods of time and their influence on the seal performance is investigated.
It is known that material properties of rubbers are strongly temperature dependent. At low tempera-tures this is caused by the rubber-glass transition (abbr. glass transition). During continuous cool-ing, the material changes from rubber-like entropy-elastic to stiff energy-elastic behavior, that al-lows 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.
Aging of elastomer seals is important, as possible dynamic loads may have to be considered during the whole interim storage period (so far approved in Germany for up to 40 years) and for transporta-tion after storage.
For the investigations, fluorocarbon (FKM) and ethylene-propylene-diene (EPDM) rubbers were selected as they are often used in radioactive waste containers. Some materials were purchased from a commercial seal producer and some materials were compounded and cured at BAM. The elastom-ers where studied by several thermo-analytical methods and compression set to characterize the material behavior at low temperatures. Additionally component tests were performed to determine the breakdown temperature of the sealing function of complete elastomer O-rings.
Für Elastomenwerkstoffe im Allgemeinen und im Bereich der Dichtungstechnik im Besonderen ist der Druckverformungsrest eine wichtige Kenngröße zur Beurteilung der Eignung eines Werkstoffs bzw. der Funktion eines Bauteils. Er ermöglicht eine Einschätzung des zeitabhängigen Rückstellverhaltens eines Werkstoffs nach Deformation. Dieses ist für Dichtungen von besonderer Bedeutung, da der Test deren Einbauzustand nachstellt.
Oft wird er, bei der Prüfung unter erhöhten Temperaturen, zur Beurteilung des Alterungsverhaltens verwendet und kann anhand eines definierten Versagenskriteriums zur Lebensdauerabschätzung eingesetzt werden. Bei tiefen Temperaturen dient er dazu, die limitierende Einsatztemperatur zu bestimmen. Dabei spielt eine Alterung im eigentlichen Sinne nur eine untergeordnete Rolle, wohl aber physikalische Effekte wie Tieftemperaturkristallisation und Glasübergang. Diese Effekte sind weit weniger durch lange Lagerzeiten beeinflusst als die eigentliche Alterung.
Die Versuchsdurchführung unterscheidet sich je nach angewandter Norm und kann einen deutlichen Einfluss auf den Druckverformungsrest haben. Alle standardisierten Methoden sind aufgrund der langen Lagerzeiten relativ langwierig und erfordern das regelmäßige Eingreifen durch den Prüfer. Zusätzlich sehen einige Methoden nur die Bestimmung eines einzelnen Wertes nach einer definierten Zeit vor.
Um die Messungen zu beschleunigen wurde eine Methode entwickelt, die automatisch die erforderlichen Messungen bei mehreren Temperaturen durchführt.
Dazu wird ein Prüfgerät der Dynamisch Mechanischen Analyse verwendet, das kontinuierlich die Deformation während eines frei programmierbaren Temperaturzyklus misst, wodurch eine sehr große Datenmenge verfügbar ist.
Ein Vergleich der neuen Methode mit den Ergebnissen des nach ISO 815 genormten Messprinzips ergibt eine gute Übereinstimmung. Ergebnisse der neuen Methode werden vorgestellt und die Vorzüge der kontinuierlichen Datenerfassung, z.B. für die Materialauswahl, diskutiert.
Die vorgestellten Ergebnisse beziehen sich zum großen Teil auf die in beschriebenen Untersuchungen und Ergebnisse.
Component and material investigations on metal seals for high level radioactive waste containers
(2018)
In Germany casks for interim storage of spent nuclear fuel and high level radioactive waste are equipped with Helicoflex® metal seals as main sealing barrier of the double lid system. The long-term behaviour of those seals is investigated at Bundesanstalt für Materialforschung und –prüfung (BAM) in order to evaluate the safety function of the containment at different temperatures over storage periods of 40 years or more in case extended interim storage becomes necessary.
Long-term investigations have been done for ageing times of up to 8.5 years at temperatures ranging from room temperature to 150 °C. It was found that the seal force and useable resilience decrease over time, which is mainly caused by creep deformation of the aluminium (or silver) outer jacket of the seals. This effect becomes stronger with increasing temperature.
The ageing processes of the seal material and the overall seal behaviour is under investigation in order to derive analytical descriptions for the long-term seal performance. Thus, standardized tests on the basic seal materials, with focus on aluminium, and additional investigations on the seals as a component are conducted. The current investigations include compression and tension creep measurements as well as tensile testing. Furthermore, ageing of seal segments provides information on the development of the contact area width, jacket thickness and microstructural changes in dependence of time and temperature. The obtained data are used for the development of material models and an analytical approach to describe and predict the time and temperature dependent sealing behaviour in the long-term.
In Germany spent nuclear fuel and high level radioactive waste is stored in interim storage containers with double lid systems. Those lids are equipped with metal seals (e.g. Helicoflex®) that ensure the safe enclosure of the inventory. The used metal seals consist of three components as can be seen in the cross-sectional view in Figure 1. The innermost part is a helical spring that is surrounded by an inner jacket made of stainless steel. The outer jacket that is made of a softer material which in case of assembly in the aforementioned storage containers is silver or aluminum (i.e. Al 99.5). During application the seal is compressed and due to the restoring force of the helical spring, the outer jacket is plastically deformed and adapts to the sealing surface. Hence, leakage paths are closed and the sealing function is generated. In Germany the above-mentioned containers are licensed for up to 40 years of interim storage, which in case extended storage becomes necessary before a final repository is available will have to be extended to even longer periods. Therefore, the evaluation of the long-term behavior of the seals is necessary, taking into account storage conditions, decay heat and possible mechanical loads as well.
At Bundesanstalt für Materialforschung und –prüfung (BAM) long-term investigations are being conducted in which seals are assembled in test flanges and aged at temperatures ranging from room temperature to 150°C for accelerated aging. The aged seals are tested semi-annually (after the first 6 months in which the seals are tested more frequently) regarding the sealing performance, the remaining seal force, and the useable resilience upon decompression. Results of these investigations have been published over the past years (e.g. Grelle, Wolff, Probst, Jaunich, & Völzke, 2017; Völzke, Wolff, Probst, Nagelschmidt, & Schulz, 2014). It was found that the seal force and the useable resilience decrease with time and temperature, which is in agreement with the result of other studies (Sassoulas et al., 2006; Wataru et al., 2016) as well. Geometry change of the outer jacket has been identified as the main reason for this seal behavior. At the prevailing operating temperatures and stresses the aluminum is subjected to creep deformation leading to a thinning of the outer jacket. Since the seal groove depth remains unchanged the helical spring expands, which in turn leads to a decrease of the generated spring and seal force.
Although the main reason for the change of seal parameters over time and temperature is known, a detailed characterization of the seal behavior and a reliable prediction of the parameter development for aging times that exceed the experimental time frame have not been possible, yet.
For deeper understanding of the aging processes, an Investigation program, which is covered in this contribution, is conducted at Bundesanstalt für Materialforschung und –prüfung (BAM) that focusses on the behavior of the aluminum jacket and its influence on the long-term sealing performance. The program investigates properties of material samples as well as the behavior of the seal as a component.
Original sheet material of the same aluminum that is used for manufacturing of the seals is investigated in compression creep tests. For this, a DMA (dynamic mechanical analysis) machine is employed (here used for static tests) that allows for a measurement of the specimens deformation under forces of up to 500 N. The advantage of this method is that the original material can be tested in the same shape as used for the seals which is 0.5 mm thick sheet material. For investigation of tensile creep standard specimens are used, that were machined from surrogate material of the same composition and annealing condition.
Furthermore, aluminum seals that are cut into smaller segments are assembled in flanges and placed in heating chambers at temperatures ranging from 23°C to 150°C. After different periods of time from 3 days to 300 days the segments are taken out of the flanges and are investigated, thus giving information on different states of aging. Measurements of the development of the seal contact width and the aluminum jacket thickness are done with an optical microscope. Further investigations on the segments will include metallography and hardness measurements.
From the detailed material and component behavior including the results of the long-term seal force and useable resilience investigations a better understanding of the overall seal behavior can be gained. The aim is to contribute to the development of material models and analytical approaches for the prediction of the sealing behavior in dependence of time and temperature.
The Bundesanstalt für Materialforschung und –Prüfung (BAM) runs an investigation program on the long-term behavior of multi-component metal seals. Such seals are used in a wide area of applications including transport and storage casks for spent nuclear fuel and high level radioactive waste.
The seal function is mainly based on the compression of the inner helical spring, which generates the necessary seal force to keep the sealing surfaces in close contact. This in turn leads to a plastic deformation of the outer jacket of the seal, comprised of highly ductile aluminum or silver that adapts to the sealing surfaces of cask body and bolted lid, thus providing high Level leak tightness. In Germany, those casks are licensed for Interim storage periods of up to 40 years or more if extended Interim storage would become necessary before a final repository is available. Thus, the sealing performance has to be evaluated, including factors like elevated temperature due to decay heat or mechanical loads due to transport under normal as well as accident conditions. Long-term investigations at BAM have been running over the last nine years to identify and evaluate the seal performance by measuring the remaining seal force, the useable resilience and the leakage rate after various time intervals at temperatures ranging from room temperature up
to 150 °C. It was found that the seal force and useable resilience decrease with time and temperature, caused by creep deformation of the outer jacket. In order to obtain an analytical description for the seal behavior and to achieve more information on the material behavior under application conditions a comprehensive investigation program with Focus on aluminum as outer jacket material was launched. The program includes material investigations such as compression and tension creep tests with representative basic materials. An additional test setup allows for the continuous measurement of the remaining seal force at temperatures of up to 150 °C. Furthermore, seal segments are compressed and stored in heating chambers, thus producing segments at different stages of the aging process. The segments are investigated regarding the development of the contact area width, jacket thickness and microstructural changes. This data will be used to develop material models and an analytical description of the time and temperature dependent long-term sealing behavior. This paper explains the current status of gained test results and modelling approaches and closes with an outlook to the future Project plans.
For the long-term storage of spent nuclear fuel and other high-Level radioactive waste, dual purpose casks for the transportation and storage are widely used. Usually, these casks consist of a thick-walled monolithic cask body and a bolted double barrier lid System equipped with metal seals (consisting of an inner helical spring and two outer metal layers with a total cross-section diameter between 5 and 10 mm) to ensure the long-term safe confinement of the radioactive inventory.
Based on analytical and experimental studies, such metallic Systems have been qualified of storage periods of up to four decades so far as long as proper manufacturing and assembling conditions are met. More than 20 years of Operation experience with a permanently increasing number of casks has shown full compliance with the expectations.
In the meantime many countries have to face a significant delay of establishing a high-level radioactive waste repository what leads to Need for extending interim storage periods for probably 60, 80 or 100 years.
For that reason the long-term performance of metal seals for such time periods is of specific internst to demonstrate their sufficient safety function and specific investigations have already been launched, e.g. by BAM, to gain more experimental data and to develop validated models to extrapolate the seal performance to longer periods of time and or requested temperature levels.
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.
The investigation of the long-term performance of sealing systems employed in containers for radioactive waste and spent nuclear fuel is one research focus area for division 3.4 “Safety of Storage Containers” at the Bundesanstalt für Materialforschung und -prüfung (BAM). Our investigations comprise investigations on metallic and elastomeric seals and covers experimental investigations to get a database on the component/material behaviour, work on analytical descriptions and numerical analysis. Our aim is to understand the long-term behaviour of the sealing systems for evaluation of their performance during possible extended interim storage and subsequent transportation.
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.
The German approach of storing spent nuclear fuel in dual purpose casks until final disposal is based on individually licensed storage sites concerning specific nuclear inventories and dual purpose cask types. The currently approved license period is maximum 40 years.
With nuclear policy changes including the phase-out decision of 2011 and a new approach for the HLW repository siting process set up 2013 by law also the spent fuel and HLW management strategy has to be adapted. This includes the timely development of disposal container concepts as part of the overall repository siting process and the need for longer interim storage periods until final disposal. Other aspects affect new regulations about the financing of the nuclear waste management by the industry and the public sector, the restructuring of responsible authorities in 2016/2017 and the adaption of R&D funding programs addressing also pre-disposal (or extended interim storage) issues.
BAM as a Federal Research Institute has been responsible for or in charge of container safety Evaluation for transport and storage casks for radioactive waste for several decades and started addressing potential Extended interim storage issues already several years ago. This included participation in international projects at the IAEA or in the U.S. Extended Storage Collaboration Program (ESCP) as well as long term laboratory tests with metal seals, elastomeric seals and polymers for neutron shielding purposes. Test results of BAM are published regularly and gained data provide valuable information about thermo-mechanical and radiological degradation effects as well as the long term Performance of respective cask components. Regarding the reliable extrapolation and prediction of the long term Performance of cask materials and components for time periods of up to 80 or even 100 years the continuation and extension of laboratory tests and the development of analytical and numerical simulation models and tools is essential and under way.
With the clear expectation of the need for extending spent fuel storage in Germany beyond the initial license period of maximum 40 years additional material data and knowledge about the long term performance and integrity of casks and internals like fuel rods will be required to meet major safety goals and regulatory requirements.
Based on a broad knowledge base about fuel cladding behavior, degradation mechanisms and related potential failure mechanisms, e. g. induced by reoriented Hydride precipitation, as illustrated in this paper, a specific gap analyses for the German situation regarding fuel conditions and cladding materials should identify the specific knowledge gaps to be addressed and closed in the near future. This is of specific interest as all spent fuel assemblies are going to be transferred to dry cask storage with the next decade and as a consequence of the German nuclear phase-out decision.
Within several decades, BAM as a Federal materials research institute gathered a broad range of expertise in the safety evaluation of materials, components and casks under operational and accidental thermal and mechanical conditions. This paper elucidates selected Basic considerations regarding technical and scientific knowledge about the long term aging performance and potential failure mechanisms of fuel cladding materials.
Under consideration of the national R&D funding policy which has been adapted to the extended interim storage or pre-disposal needs and the competences of BAM, its future R&D strategy is explained and some R&D objectives have already been identified. BAM will continue and expand ist engagement in the area of investigating fuel cladding material behavior in the long term and developing validated simulation and analyses tools in collaboration with national and international partners. R&D outcomes shall improve the knowledge-base to close identified knowledge gaps in the area of demonstrating fuel cladding integrity and to provide crucial information with regard to future safety assessments for the extended interim spent fuel storage.
Characterisation of degradation and determination of end-of-lifetime criterion for O-ring seals
(2017)
The ageing of polymers, including elastomers, is an undesirable but inevitable process leading to a limited lifetime of rubber products such as seals. Independent of the application, as e.g. in automotive, piping or container applications, a long lifetime or at least a timely exchange of a seal before occurrence of critical failure is desired.
In order to investigate the degradation of material properties and to determine the lifetime of elastomers used as seals, an ageing programme was started with hydrogenated acrylonitrile butadiene rubber (HNBR), ethylene propylene diene rubber (EPDM) and fluorocarbon rubber (FKM) [1-3]. Both O-ring seals (uncompressed and compressed by 25 %) with a cord diameter of 10 mm as well as sheets with a thickness of 2 mm were aged at 75 °C, 100 °C, 125 °C and 150 °C for up to two years. The changes of material properties during ageing were characterised for each material using samples from the sheets by means of e.g. Dynamic Mechanical Analysis and tensile tests, while sealing properties such as leakage rate were determined on O-rings. The experimental results indicate that while material properties show considerable degradation effects, the static leakage rate stays constant or even decreases before failure occurs quite suddenly at advanced degradation levels. This reveals that static leakage rate has only limited sensitivity for the degradation of the seal material.
Our approach to determine a suitable end of lifetime criterion, which involves a partial decompression of the seal during the leakage test, is presented and discussed.
This paper describes and discusses the major challenges of spent fuel management in Germany after the phase-out of nuclear electricity generation was decided in 2011 and a new repository siting procedure was implemented in 2013. Consequences from those decisions which were legally founded by amendments of the German Atomic Energy Act (AtG) result in the need to transfer all remaining spent fuel from limited reactor operation (last reactor shutdown until the end of 2022) into casks for subsequent dry interim storage on-site. Storage licenses are generally issued site-specific considering specific dual purpose casks (DPC) and their inventories and they are generally limited to 40 years so far. But the need for extending the interim storage period in the future has become obvious. Even though, this may not be an issue to be solved already today questions about additional safety demonstrations will arise as soon as licenses need to be extended. Certainly, these questions will ask for reliable data about the long term performance and safety of structures, systems, and components, e. g. the long term performance of cask components and materials like bolted closure systems including metal seals, or fuel rod behaviour concerning cladding materials under stress and temperature conditions. In case of dual purpose casks for storage and transportation this includes aspects on how to demonstrate transportability during or after several decades of interim storage. Long term investigations often require plenty of time and therefore need to be initiated timely.
This paper describes and discusses the major challenges of spent fuel management in Germany after the phase-out of nuclear electricity generation was decided in 2011 and a new repository siting procedure was implemented in 2013. Consequences from those decisions which were legally founded by amendments of the German Atomic Energy Act (AtG) result in the need to transfer all remaining spent fuel from limited reactor operation (last reactor shutdown until the end of 2022) into casks for subsequent dry interim storage on-site. Storage licenses are generally issued site-specific considering specific dual purpose casks (DPC) and their inventories and they are generally limited to 40 years so far. But the need for extending the interim storage period in the future has become obvious. Even though, this may not be an issue to be solved already today questions about additional safety demonstrations will arise as soon as licenses need to be extended. Certainly, these questions will ask for reliable data about the long term performance and safety of structures, systems, and components, e. g. the long term performance of cask components and materials like bolted closure systems including metal seals, or fuel rod behaviour concerning cladding materials under stress and temperature conditions. In case of dual purpose casks for storage and transportation this includes aspects on how to demonstrate transportability during or after several decades of interim storage. Long term investigations often require plenty of time and therefore need to be initiated timely.
The safe and secure long term storage of spent nuclear fuel until its final disposal in a deep geological repository is a corner stone of the German nuclear waste management strategy. So far interim storage licenses are limited to 40 years concerning the initial concept of having a repository available until 2035. But in the meantime the exploration of the designated Gorleben salt dome was finally stopped and a reset of the complete site selection process was concluded by the German Federal parliament and subsequently fixed by law. A 33-member “Commission on the storage of highly radioactive materials” was established in 2014, to elaborate a consent based siting process and to develop criteria for the safe disposal of heat generating waste. The disposal commission agreed and published its final report in 2016.
As a major consequence, the necessary timeframe for establishing the final repository is going to be exceeded significantly and with that, an extension of the current dry interim storage in dual purpose casks becomes necessary. This paper explains the major actions to be taken in Germany to address all relevant issues for a future extension of storage licenses beyond the initial timeframe of 40 years.
Elastomer seals are widely used as barrier seals in containers for low and intermediate level radioactive waste and in some countries for spent fuel transportation casks. Depending on the area of use, the rubber materials have to demonstrate proper sealing performance with regard to mechanical, thermal and environmental conditions as well as irradiation during the entire operation period.
In Germany the low and intermediate level radioactive waste is planned to be disposed in the Konrad repository in standardized containers. Many of these containers use an elastomer seal between lid and container body. Depending on the radiactive inventory and a possible containment of the waste in inner barrels and/or concrete structures, such containers may require a specific leak tightness. In such cases, specified leakage rates are shall not be exceeded by the the seals to keep potential activity releases from the inventories well below defined limits.
Generally, all waste containers have to fulfill the waste acceptance criteria for the Konrad repository as defined by the reports BfS SE-IB-29/08 and SE-IB-30/08. From these criteria several requirements for seal performance are derived. The seals have to:
- ensure full functionality until final container disposal,
- maintain its function in case of a thermal or mechanical accident,
- ensure encapsulation also at -20 °C.
This combination of requirements is challenging especially as a seal exchange, which is typical for many other applications, is hardly possible and thus a sound understanding of how to perform safety evaluation of containers is required. Therefore BAM has initiated investigations on elastomer seal behaviour. This work focuses on low temperature behaviour and sealing performance concerning static conditions as well as partial loss of compression and ageing of elastomer seals. Concerning ageing, property changes caused by long-term thermooxidative conditions as well as gamma irradiation are investigated.
This contribution presents an overview and explanation of the aims of the ongoing research and gives an update of the most relevant results.
In Germany, the concept of dry interim storage in dual purpose metal casks before disposal is being pursued for spent nuclear fuel (SF) and high active waste (HAW) management. However, since there is no repository available today, the initially planned and established dry interim storage license duration of up to 40 years will be too short and its extension will become necessary. For such a storage license extension it is required to assess the long-term performance of SF and all safety related storage system components in order to confirm the viability of extended storage.
The main safety relevant components are the thick-walled dual purpose metal casks. These casks consist of a monolithic cask body with integrated neutron shielding components (polymers, e.g. polyethylene) and a monitored double lid barrier system with metal and elastomeric seals. The metal seals of this bolted closure system guarantee the required leak-tightness whereas the elastomeric seals allow for leakage rate measurement of the metal seals.
This paper presents an update on running long-term tests on metal seals at different temperatures under static conditions over longer periods of time. In addition, first results of our approach to understand the aging behavior of different elastomeric seals and neutron radiation shielding material polyethylene are discussed.
Ziel unserer Arbeit ist es, den sicheren Einschluss von gefährlichen Gütern in entsprechenden Verpackungen (z.B. Behälter für radioaktive Stoffe) unter verschiedenen Umgebungsbedingungen und über lange Zeiten sicher zu stellen bzw. die Materialauswahl entsprechend zu steuern. Aufgrund ihrer einfachen und zuverlässigen Anwendung werden Elastomere für viele Dichtungsaufgaben eingesetzt. In vielen Anwendungsbereichen wie z.B. Verkehr, Luftfahrt und Verfahrenstechnik können während des Einsatzes tiefe Temperaturen auftreten, bei denen die Funktionsfähigkeit der Dichtung erhalten bleiben muss. Daher ist die Untersuchung des Verhaltens von Elastomerdichtungen bei tiefen Temperaturen wichtig, um ihren Temperatureinsatzbereich nach unten abzugrenzen und dadurch einen verlässlichen Betrieb zu sichern. Dazu wurden umfangreiche Untersuchungen durchgeführt, auf deren Ergebnisse hier kurz eingegangen werden soll.
Bei allen Anwendungen ist die Frage nach der Lebenszeit einer Dichtung entscheidend für z.B. Austauschintervalle oder Wartung. Besondere Bedeutung hat die Lebensdauer allerdings bei Anwendungen, in denen ein Austausch der Dichtung nicht möglich ist. Hier kann die Dichtung über die Lebensdauer des Gesamtsystems entscheiden. Daher ist eine verlässliche Abschätzung der Lebensdauer für diese Anwendungen relevant. Dazu ist eine umfangreiche Datenbasis erforderlich. Entsprechende Arbeiten, die gerade begonnenen worden sind, sollen ergänzend vorgestellt werden. Erste konkrete Ergebnisse werden im Vortrag vorgestellt.
It is important to evaluate the effect of thermal ageing on the sealing performance of metal gaskets under high temperature for long-term usage. Therefore, in order to gain representative data for this kind of metal-sealed lid System, BAM is currently performing laboratory tests of different gasket types with aluminum and silver jackets at three different temperatures under static conditions up to four years so far, using test flanges for gaskets with full scale cross section diameter but much smaller outer diameter. On the other hand, in order to investigate the applicability of the numerical methodology to evaluate the long-term behavior of the metal gaskets, such as a correlation between seal pressure force and holding time, CRIEPI is developing a modeling method including material tests (tensile and creep tests) at high temperature. In this paper, the applicability of the finite element method (ABAQUS) to predict the recovery displacement and residual seal pressure force of the gasket complex was verified by comparing the calculated values with BAM’s laboratory test results under the joint research agreement between BAM and CRIEPI.
Elastomers are widely used as main sealing materials in Containers for low and intermediate level radioactive waste and as additional component to metal seals in spent fuel and high active waste Containers. They are applied due to their special material properties and easy use [1]. For this application several challenging prerequisites must be met for the essential reliable Operation of the seal.
Elastomers are widely used as main sealing materials for Containers for low and intermediate Ievel radioactive waste and as additional component to metal seals in spent fuel and high active waste Containers. According to appropriate guidelines and regulations safe enclosure of the radioactive Container contents has to be guaranteed for long storage periods as well as down to temperatures of -40 °C for transportation. Therefore the understanding of seal behaviour in general is of high importance and ageing of elastomeric seals has to be considered with regard to possible dynamic events taking possibly place during transport after storage.
Metal seals are widely used for extreme applications, e.g. in dual-purpose casks for dry interim storage of spent nuclear fuel in Germany. Due to the fact that interim storage must be safe at least for the approved period of 40 years there is a major interest to investigate the long-term behaviour and ageing mechanisms of metal seals. Experimental analyses indicate a time and temperature dependency of seal characteristics. This dependency was researched with a time- and temperature parameterization based up on Larson-Miller. The paper describes the derivation of the material parameter C from test results and the applicability of the Larson-Miller-Relationship for those metal seals in principle. Overall a constant material parameter C was not. Nevertheless, an approach comparable to the Larson-Miller-Parameter was developed.
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.