Filtern
Erscheinungsjahr
Dokumenttyp
- Beitrag zu einem Tagungsband (77)
- Vortrag (32)
- Zeitschriftenartikel (13)
- Beitrag zu einem Sammelband (7)
- Buchkapitel (5)
- Forschungsbericht (5)
- Sonstiges (1)
Referierte Publikation
- nein (140) (entfernen)
Schlagworte
- Ageing (11)
- Seal (11)
- Elastomer (10)
- Storage (9)
- Compression set (8)
- Metal seal (8)
- Aging (7)
- Behälter (6)
- Creep (6)
- Interim storage (6)
- Rubber (6)
- Spent fuel (6)
- Dichtungen (5)
- Disposal (5)
- Elastomere (5)
- Endlager (5)
- Irradiation (5)
- O-ring (5)
- Spent Fuel (5)
- Cask (4)
- Compression (4)
- Dichtung (4)
- Glass-rubber transition (4)
- Hochradioaktive Abfälle (4)
- Long-term behavior (4)
- Metal seals (4)
- Sicherheitsanforderungen (4)
- Tieftemperaturverhalten (4)
- Alterung (3)
- Degradation (3)
- Druckverformungsrest (3)
- Dual purpose cask (3)
- Lagerung (3)
- Leakage (3)
- Lifetime (3)
- Long-term storage (3)
- Numerical analysis (3)
- O-Ring (3)
- Rubber seal (3)
- Safety (3)
- Transport (3)
- Cask accident scenario (2)
- Dehnratenabhängigkeit (2)
- Dämpferbeton (2)
- Elastomer seals (2)
- Extended storage (2)
- Gamma irradiation (2)
- Glasübergang (2)
- Leak tightness (2)
- Leakage rate (2)
- Long-term behaviour (2)
- Low temperature (2)
- Material model (2)
- Materialmodellierung (2)
- Metal Seal (2)
- Metallic seal (2)
- Partial release (2)
- Polyurethan Schaum (2)
- Radioactive Waste (2)
- Radioactive waste containers (2)
- Simulation (2)
- Stoßbelastung (2)
- Stoßdämpfende Werkstoffe (2)
- Temperaturabhängigkeit (2)
- Transport- und Lagerbehälter für radioaktive Stoffe (2)
- Versuchsprogramm (2)
- (U)HMW-PE (1)
- (U)HMWPE (1)
- Ageing Management (1)
- Ageing management (1)
- Aging mechanisms (1)
- Aircraft crash (1)
- Aluminium (1)
- Anforderungen (1)
- Axial Compression (1)
- Axial compression variation (1)
- Beständigkeit (1)
- Building of the storage facility (1)
- Cask design (1)
- Cask for storage and transport of radioactive materials (1)
- Casks (1)
- Cladding (1)
- Co-60 irradiation (1)
- Coefficient of Friction (1)
- Component tests (1)
- Container (1)
- Crosslinking (1)
- Cyclic load (1)
- Cycling Tests (1)
- DSC (1)
- Damping concrete (1)
- Degradation mechanisms (1)
- Dichtheit (1)
- Dichtsysteme (1)
- Dry storage (1)
- Dual Purpose Cask (1)
- Dual purpose casks (1)
- Dynamic mechanical analysis (1)
- EPDM (1)
- Elastomer Dichtung (1)
- Elastomers (1)
- Experiment (1)
- Extended Storage (1)
- Extended interim storage (1)
- Extended storing (1)
- Extrapolation (1)
- Federunterstützte Metalldichtungen (1)
- Fuel cladding (1)
- Gamma radiation (1)
- HMW (1)
- HMW-PE (1)
- Helium Leakage Rate (1)
- Helium leakage rate (1)
- Helium-Dichtheitsprüfung (1)
- Hydride precipitation (1)
- IR (1)
- Impact load (1)
- Infrared and far-infrared spectroscopy (1)
- Inspections (1)
- Interim storage facility (1)
- KOBAF (1)
- Kohäsionsenergie (1)
- Konrad repository (1)
- Langzeiteignung (1)
- Langzeitversuche (1)
- Larson and Miller relationship (1)
- Larson-Miller parameter (1)
- Larson-Miller-Parameter (1)
- Leakage Rate (1)
- Leckagerate (1)
- Lid-seal system (1)
- Life time prediction (1)
- Log term behavior (1)
- Long term interim storage (1)
- Long term performance (1)
- Long-term safety (1)
- Low temperature behaviour (1)
- Material degradation (1)
- Metal Seals (1)
- Metalldichtung (1)
- Modelling (1)
- Neutron Shielding Materials (1)
- Neutron radiation shielding material (1)
- Neutron shielding material (1)
- Nuclear reactor compartments of submarines (1)
- Numerical Simulation (1)
- Numerical simulation (1)
- O Ring (1)
- Operating procedures (1)
- Package (1)
- Polyehtylene (1)
- Polyethylene (1)
- Polymere (1)
- Quellungsmessung (1)
- Radioactive Materials (1)
- Radioactive material (1)
- Radioactive material storage (1)
- Radioactive material transport (1)
- Radioaktive Stoffe (1)
- Recovery (1)
- Regulation (1)
- Rubber seals (1)
- SHPB (1)
- Seal Behavior (1)
- Seal effects (1)
- Seal performance (1)
- Seal properties (1)
- Sealing material (1)
- Shielding material (1)
- Sicherheit (1)
- Silver (1)
- Spent Nuclear Fuel (1)
- Storage cask (1)
- Storage casks (1)
- Storage system components (1)
- Storing spent fuel (1)
- Strain rate sensitivity (1)
- Stress relaxation (1)
- Structure-property relationship (1)
- Struktur-Eigenschaftsbeziehung (1)
- Transport Packagings (1)
- Transport casks (1)
- Transport package design (1)
- Transportation of heavy compartments (1)
- UHMW-PE (1)
- Unknown storage duration (1)
- Venetzungsdichte (1)
- Verpackung (1)
- Very long term storage (1)
- WAXD (1)
- Wirtsgestein (1)
- hochradioaktive Abfälle (1)
- radioactive waste (1)
Organisationseinheit der BAM
- 3 Gefahrgutumschließungen; Energiespeicher (24)
- 3.4 Sicherheit von Lagerbehältern (24)
- 9 Komponentensicherheit (2)
- 3.3 Sicherheit von Transportbehältern (1)
- 5 Werkstofftechnik (1)
- 5.2 Metallische Hochtemperaturwerkstoffe (1)
- 9.5 Tribologie und Verschleißschutz (1)
- 9.6 Additive Fertigung metallischer Komponenten (1)
Eingeladener Vortrag
- nein (32)
Abstract Hydrogenated nitrile butadiene rubber (HNBR) elastomer was thermo-oxidatively aged at different temperatures up to 150 °C. Fourier transform infrared spectroscopy (FTIR), compression stress relaxation (CSR) and international rubber hardness degree (IRHD) microhardness were used to characterise the chemo-mechanical changes of HNBR O-rings during thermo-oxidative ageing. FTIR shows the development of carbonyl, methyl and ester groups but the nitrile content was not affected by ageing. The effect of sample geometry during CSR was investigated. CSR data were converted through integrated kinetic laws. The conversion has proven its sensibility to detect heterogeneous ageing. This was confirmed by the IRHD measure-ments across the section of O-rings. The influence of compression during ageing was assessed through IRHD measurements across the section of compressed and uncom-pressed aged O-rings. The DLO effect was more pronounced in compressed O-rings. By applying the model of Wise et al., theoretical IRHD and oxidation profiles were determined on the basis of IRHD experimental data of compressed O-rings. Good agreements between the experimental and the theoretical IRHD profiles in the core region were obtained. However, near the edge, the theoretical IRHD values were overestimated.
Overview of ongoing research and future prospects on polyethylene neutron shielding materials at bam
(2023)
The extension of the interim storage period of radioactive waste before disposal will cause additional challenges for the nuclear waste management in Germany, so that an extensive knowledge of the long-term performance of casks, including their components and inventories, will be required for future extended storage licenses.
Ultra-high and high molecular weight polyethylenes ((U)HMW-PE) are used for neutron shielding purposes in casks for storage and transport of spent fuel and high-level waste due to their extremely high hydrogen content. During their service life of several decades as cask components, the PE materials are exposed to neutron and gamma radiation from the radioactive inventory of the casks, mechanical assembling stresses and temperature. All these combined effects affect the material properties of such components which in turn may be crucial for some possible accident scenarios.
At the Bundesanstalt für Materialforschung und -prüfung (BAM), the effects of high temperature exposure in combination with subsequent or previous irradiation were investigated with a comprehensive aging program including thermal aging at 125 °C for different aging periods up to 5 years and irradiation with doses ranging from 50 to 600 kGy.
This contribution provides an overview of the ongoing research related to the structural changes of (U)HMW-PE induced by gamma irradiation and high temperature exposure and focuses on current research perspectives at BAM with regard to the prediction of the dynamic behavior of the material during extended interim storage in case of an accident scenario. First results of the coupled effect of temperature, radiation and mechanical loading will be presented. The effect of microstructural changes induced by gamma irradiation and high temperature on the mechanical behavior of (U)HMW-PE will be assessed.
Langzeitversuche über 10 Jahre an Federkern-Metalldichtungen mit Aluminium- bzw. Silberummantelungen
(2023)
Federunterstützte Metalldichtungen mit Aluminium(Al)- oder Silber(Ag)-Ummantelung werden u.a. in Behältern für Wärme entwickelnde radioaktive Abfälle eingesetzt, da diese Dichtungen eine sehr gute Dichtheit gewährleisten sowie Langlebigkeit und Beständigkeit gegenüber erhöhten Temperaturen und radioaktiver Strahlung aufweisen. Auch wenn die Sicherheit solcher Behälter und der verwendeten Dichtungen vielfach belegt wurde, sind sie Gegenstand andauernder Forschung, etwa im Hinblick auf eine absehbar benötigte verlängerte Zwischenlagerdauer. Aus diesem Grund werden an der Bundesanstalt für Materialforschung und -prüfung (BAM) im Fachbereich 3.4 „Sicherheit von Lagerbehältern“ seit über 20 Jahren Versuche an solchen Metalldichtungen durchgeführt. Dabei sollen zusätzliche Erkenntnisse hinsichtlich der Sicherheitsreserven der Dichtungen in unterstellten Störfallszenarien (axiale Bewegung des Deckelsystems bzw. Aufweitung der Nutgeometrie) und insbesondere detailliertere Erkenntnisse zum Langzeitverhalten gewonnen werden.
Elastomer seals are mounted as barrier seals in lid systems of containers designed for transport and disposal of negligible heat generating radioactive waste and as auxiliary seals in spent fuel storage and transportation casks (dual purpose casks (DPC)). When the behavior of mounted seals under normal and hypothetical accident conditions of disposal and transport is to be simulated, a comprehensive knowledge of their complex mechanical properties at every state of aging is necessary. In previous works, BAM’s efforts in experimental investigations on specimen artificially aged at different temperatures and times and the implementation of the found results in finite element material models were presented. Additionally, our approaches to reproduce the aging process itself and to extrapolate the results of artificially accelerated aging to longer times were presented. Numerical simulations have shown that the behavior of the seal during mounting and one-sided pressurizing and the resulting performance values such as leakage rate strongly depend on the coefficient of friction (COF) between flange and seal. The friction coefficient, in turn, depends on the aging state of the elastomer material as several publications suggest (see below).
Dynamic COF between an exemplary ethylene propylene diene rubber (EPDM) material and a stainless steel ball were determined by using a self-designed linear oscillation tribometer. Unaged and artificially aged EPDM specimen stored for 30 days and 100 days at a temperature of 150 °C were tested. A stainless steel ball (d=10 mm) is brought in contact with the specimen’s surface und loaded by normal forces of 2.5 N, 5 N, 10 N and 20 N. During a reciprocating movement of the EPDM sheet, the horizontal force/friction force is continuously measured, and the COF can be derived.
It is well known that friction is a complex phenomenon especially in soft materials. It cannot be excluded that the measured friction force is influenced by additional force components, resulting from the ball’s grooving through the elastomer’s surface. This force depends on the penetration depth of the ball and on the resistance of the elastomer in its different states of aging. The latter results from microstructural changes i.e., chain scission and additional crosslinking that occur during aging which in turn influence the softening or hardening of the material.
A finite element (FE) ABAQUS® model was developed to reproduce the measurement process. It should help to better understand the physical mechanisms and to quantify the percentage of measured forces resulting from real friction on the one hand and forces resulting from unintended side effects that could falsify the result on the other hand. The behavior of the elastomer in its different states of aging is reproduced by a FE material model already presented in previous works of BAM.
It is common practice in the application of finite element analysis to model compression set (CS) of elastomers during aging with two different material models according to the two-network theory of Tobolsky. The theory relies on the existence of two networks. The first one represents the original network after vulcanization and is sensitive to chain scission. The second network accounts for the formation of additional crosslinking during aging. Besides the use of user subroutines to describe the two-network model, an element overlay technique is also needed as the full set of both material behaviors did not exist for assignment to a single element. This element overlay technique is valuable for research and developmental purposes but makes extension to industrial usage quite challenging. Our goal is to simulate the CS of elastomers after long-term aging in a commercial finite element software with no need for extra subroutine codes or mesh superposition.
Ethylene propylene diene (EPDM) O-rings were aged in a compressed state at 75 °C, 100 °C, 125 °C and 150 °C for up to 183 days. Investigations of the experimental test results were used to identify material models and their parameters to develop a finite element model to simulate CS. The model was implemented in the finite element software ABAQUS/Standard® with a sequential temperature-displacement coupling.
Regarding the influence of temperature, the Arrhenius equation is adopted for the time-temperature relationship. The activation energy value that is required for the simulation is firstly determined from shifting the experimental CS results with the time-temperature superposition technique and plotting the shift factors in an Arrhenius diagram. The experiments were compared with the simulation results. Afterwards different activation energies were used in the simulation and discussed. A suitable choice of the activation energy value with regard to the reference temperature and the test temperature is presented. With the chosen activation energies, the match between numerical CS values after long-term aging and the experimental results was improved.
Bei der Auswahl eines Standortes für ein Endlager für hochradioaktive Abfälle (Wärme entwickelnde radioaktive Abfälle und ausgediente Brennelemente) in Deutschland werden auf Grundlage des Standortauswahlgesetzes von 2017 die drei potenziellen Wirtsgesteine Steinsalz, Tonstein und Kristallingestein in Betracht gezogen. Die Auswahl eines konkreten Endlagerstandortes steht dabei in engem Zusammenhang mit den für die jeweiligen Wirtsgesteine geeignet erscheinender Endlagersystemen. Zentraler Bestandteil dieser Endlagersysteme sind die Endlagerbehälter, deren Gestaltung und Auslegung maßgeblich die Randbedingungen für die Transport- und Einlagerungstechnik vorgibt und zudem die Nachweise zur Betriebs- und Langzeitsicherheit entscheidend prägt. Daher ist es für die Behälterentwicklung erforderlich, die an Endlagerbehälter zu stellenden Anforderungen systematisch herzuleiten. Auf dieser Grundlage können anforderungsgerechte Endlagerbehälter zielgerichtet für die jeweils zu untersuchenden Endlagerstandorte in unterschiedlichen Wirtsgesteinen entwickelt werden.
Dieser Beitrag fasst die wesentlichen Ergebnisse des von BAM und BGE TECHNOLOGY GmbH im Zeitraum 2017 bis 2020 bearbeiteten und vom Bundesministerium für Wirtschaft und Energie (BMWi) geförderten Forschungsvorhabens KoBrA zusammen, die in einem Abschlussbericht und vier zugehörigen Teilberichten umfassend dokumentiert sind.
Im hier vorliegenden Bericht wurde im Rahmen einer umfassenden Literaturrecherche der nationale und internationale Stand von Wissenschaft und Technik hinsichtlich Behälterkonzepten und Behälteranforderungen erfasst. Dabei wurde eine umfangreiche Dokumentensammlung zusammengestellt und sortiert, die als Quellenbasis für alle weiteren Arbeiten zur Verfügung steht. Die Auswertung der gesammelten Informationen resultiert in einem Überblick über internationale Behälterentwicklungen sowie einer detaillierten Übersicht über die Behälterkonzepte und die ihnen zugrundeliegenden Anforderungskataloge aus elf fortgeschrittenen Endlagerprogrammen.
Der Bericht zum Arbeitspaket 3 baut auf den Ergebnissen der internationalen Recherche (AP1) sowie der Zusammenstellung der Randbedingungen und Beanspruchungsgrößen für die Endlagerbehälter (AP2) auf. Die Anforderungen an die Behälter – regulatorische, betriebliche sowie solche aus der Standortgeologie und den Einwirkungen und Prozessen, denen die Behälter ausgesetzt sind – werden hergeleitet und systematisch dargestellt.
Die für das Endlagersystem zu betrachtenden Nutzungsphasen werden aus den regulatorischen Anforderungen hergeleitet und charakterisiert. Die Einwirkungen auf die Behälter in den drei potenziellen Wirtsgesteinen sowie die sich für die Erfüllung der Sicherheitsfunktionen des Behälters als Teil des Endlagersystems ergebenden Behälterfunktionen werden ebenfalls wirtsgesteins- und zeitphasenabhängig betrachtet. Schließlich werden aus den Einwirkungen auf die Behälter und den Anforderungen an die Behälterfunktionen auch quantifizierbare Behälterfunktionen für alle drei potenziellen Wirtsgesteine abgeleitet.
At the Bundesanstalt für Materialforschung und -prüfung (BAM) in Division 3.4 Safety of Storage Containers, one of our tasks is to evaluate the safety of containers designed for disposal of low and intermediate radioactive waste. As such containers might be transported before and stored until disposal, safe enclosure of the radioactive inventory is important for this time span. Elastomer O-rings are widely used as barrier seals in these containers. Thus, as for many other applications, an understanding of the practical effects of ageing degradation on elastomer seals during long-term exposure is mandatory for predicting the lifetime of such components. According to a long-term test programme on three kinds of rubbers (EPDM and FKM (relevant for application), HNBR (for comparison)), over several years we have studied the degradation and the change of mechanical properties (e.g. hardness, strain at break) at four different ageing temperatures (75 °C, 100 °C, 125 °C and 150 °C) as well as the change of sealing properties. Continuous and intermittent compression stress relaxation (CSR) measurements were performed in order to investigate the respective contribution of crosslinking and chain scission to the observed degradation effects. Thus, the degradation kinetics and mechanisms could be resolved more clearly. For assessing the seal performance, compression set (CS) and leakage rate measurements were conducted. The experimental results showed that the O-rings remained leak-tight under purely static conditions even when CSR, CS and mechanical properties already indicated far advanced degradation. For this reason, a modified leakage test involving a small and rapid partial decompression of the seal was developed that enabled determining an end-of-lifetime criterion for O-rings with a safety margin for thermal shrinkage and vibrations.
Eine Aufgabe des Fachbereichs 3.4 Sicherheit von Lagerbehältern der Bundesanstalt für Materialforschung und -prüfung (BAM) ist es, die Sicherheit von Behältern zur Lagerung von radioaktivem Abfall mit vernachlässigbarer Wärmeentwicklung zu bewerten. Da solche Behälter vor der Entsorgung transportiert und gelagert werden, ist während dieser Zeit ein sicherer Einschluss des radioaktiven Inhalts von größter Bedeutung. Zur Abdichtung dieser Behälter sind Elastomer-O-Ringe weit verbreitet. Um für solche, wie auch für viele andere Anwendungen, eine Voraussage über die Lebensdauer dieser Komponenten treffen zu können, ist es unerlässlich zu verstehen, welchen Einfluss der durch Alterung hervorgerufene Abbau auf Dauer auf die Elastomerdichtungen hat. In einem Langzeittest wurden drei Kautschukarten (EPDM und FKM, die für die Anwendung relevant sind, und HNBR als Vergleich) über mehrere Jahre untersucht. Dabei wurden die Veränderungen der mechanischen Eigenschaften (z. B. Härte und Bruchdehnung) bei vier verschiedenen Alterungstemperaturen (75 °C, 100 °C, 125 °C und 150 °C) sowie das Dichtungsverhalten betrachtet. Um den Einfluss von Vernetzung und Kettenspaltung auf die beobachteten Alterungseffekte zu bestimmen, wurden Messungen zur kontinuierlichen und intermittierenden Druckspannungsrelaxation durchgeführt. Dadurch konnten Erkenntnisse über Kinetik und Mechanismus der Abbaureaktionen
gewonnen werden. Zur Einschätzung des Dichtungsverhaltens wurden Durckverformungsrest und Leckagerate gemessen. Die Ergebnisse zeigen, dass die O-Ringe unter statischen Bedingungen auch dann dicht halten, wenn die Werte für Druckverformungsrest, Druckspannungsrelaxation und mechanische Eigenschaften schon auf einen fortgeschrittenen Alterungsabbau hindeuten. Aus diesem Grund wurde ein modifizierter Dichtigkeitsversuch mit einer geringen und schnellen teilweisen Entlastung der Dichtung entwickelt, mit dessen Hilfe sich ein Lebensdauerkriterium bestimmen lässt, das eine Sicherheitsspanne für thermische Schrumpfung und Vibrationen beinhaltet.
Spent nuclear fuel which is generated in the operation of nuclear reactors needs to be safely managed following its removal from the reactor core. On-site power reactor storage pools were designed on the assumption that after a short period of time spent nuclear fuel would be removed for reprocessing and disposal or further storage elsewhere. The amount of highly radioactive spent fuel that needs to be stored over longer periods of time is growing and additional storage capacity is required. One of the widely used options for additional storage capacity is the use of casks for dry storage of spent fuel. Among various existing dry storage concepts, several Member States are utilizing a concept of dual purpose casks (DPCs). This publication provides practical advice on the structure and contents of a DPC integrated safety case with reference to existing IAEA requirements relevant to the licensing and use of transport and storage casks for spent fuel.
Im Forschungsvorhaben KoBrA werden Anforderungen an Endlagerbehälter für hochradioaktive Abfälle erstmals systematisch und unter Berücksichtigung des internationalen Standes von Wissenschaft und Technik hergeleitet. Parallel werden die behälterrelevanten Randbedingungen und Beanspruchungsgrößen für Endlagerbehälter in den drei potenziellen Wirtsgesteinen Steinsalz, Tonstein und Kristallingestein ermittelt. Darauf aufbauend werden die zur Erfüllung der Anforderungen unter den gegebenen Einwirkungen und Beanspruchungen notwendigen Behälterfunktionen bestimmt und erste Konzeptideen für zukünftige Endlagerbehälter diskutiert bzw. entwickelt.
Dieser Bericht untersucht die im ersten Arbeitspaket ermittelten vorhandenen bzw. entwickelten Behälterkonzepte dahingehend, inwieweit die jeweiligen Behälterfunktionen unter den im zweiten und dritten Arbeitspaket ermittelten Randbedingungen und Einwirkungen den im dritten Arbeitspaket ermittelten Anforderungen an endlagerfähige Behälter in einem deutschen Endlager genügen. Zum anderen sollen, basierend auf den im zweiten Arbeitspaket ermittelten Randbedingungen und den im dritten Arbeitspaket hergeleiteten und zusammengestellten Anforderungen an die Endlagerbehälter, Vorschläge für mögliche generische Endlagerbehälter in den drei potenziellen Wirtsgesteinen Steinsalz, Tonstein und Kristallingestein erarbeitet werden. Die im ersten Arbeitspaket recherchierten Behälterkonzepte, deren Entwicklungslinien und zugrundeliegende Behälteranforderungen bilden hier den Ausgangspunkt für weitergehende Überlegungen hinsichtlich ihrer potenziellen Eignung für ein zukünftiges deutsches Endlager und zur Skizzierung generischer Konzepte für zukünftige Endlagerbehälter.
In this presentation, the history and actual situation of the German nuclear waste management policy of spent fuel (SF) and high-level waste (HLW) is reported. Beside the description of the restructuration of responsible authorities and organizations in Germany, the principle of dry interim storage of SF and HLW in dual purpose casks is explained. The need for extended interim storage towards disposal implicates additional challenges for the nuclear waste management strategy in Germany. (Extended)interim storage, subsequent transportation, and final disposal are closely linked. Integrated approaches concerning waste package designs and operations are supposed to be beneficial for the establishment of efficient long-term SF and HLW management strategies. Knowledge management and staff recruiting, education and training during phase out and beyond nuclear power plant operation are major issues.
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.
Safety of long term containment and storage of radioactive waste is an essential issue, which is increasingly gaining international attention. Extending interim storage beyond initial license periods is one of the major challenges worldwide.
BAM has been involved in all kinds of radioactive waste container safety evaluation for storage and transportation including their long term performance from the very beginning. Today, all work related to the safe management of radioactive waste is linked by the activity field “Nuclear Waste Management” within the Focus Area “Energy” at BAM and in conjunction with a research strategy and agenda. Most recently, the working group “Long Term Safety of Container Systems and Components” was established to launch and perform research projects related to safety issues concerning the extended interim storage of radioactive waste.
For example, within our project LaMEP, we investigate ageing effects of metal and elastomer seals as well as polymeric neutron shielding materials, which are container components that fulfil major safety functions. The results of the experiments help to understand the long term behaviour of these components. Likewise, our project BRUZL started at BAM in 2018 with the aim of developing a fracture mechanics approach to understand and describe a potential brittle failure mechanism of fuel cladding during long-term interim storage. BAM also contributes to the GRS project “Development of methods and models and international exchange for safety evaluation in the frame of interim storage of radioactive waste”. Additionally, BAM is involved in several international research programmes dealing with extended interim storage, such as the European Joint Programme on Radioactive Waste Management (EURAD), the Extended Storage Collaboration Program (ESCP) and IAEA Coordinated Research Projects.
The present contribution provides a comprehensive overview of BAM research activities contributing to national and international gap analyses and to filling knowledge gaps regarding the safe long term management of radioactive waste.
This publication summarizes the work carried out during an IAEA coordinated research project (CRP) on safe and reliabe management of spent nuclear fuel. This work contributes to the overall goal of demonstrating the performance of spent nuclear fuel and related storage systems components over long durations, and facilitates the transfer of this knowledge to Member States. The technical areas addressed by the CRP participants were related to potential degradation mechanisms in metal casks and concrete overpacks, such as stress corrosion cracking; long term integrity and performance of the fuel cladding; thermo-mechanical behaviour of the metal seals; and long term gamma and neutron shielding capability. The participants also considered past and ongoing demonstration programmes. For each technical topic addressed the main conclusions have been drawn, including information on the development of specific monitoring and inspection techniques as well as future opportunities for closing relevant data gaps. A major achievement is also the establishment of a worldwide network of experts working on current research projects to demonstrate the long term performance of spent fuel in dry storage systems.
In Germany, spent nuclear fuel and high active waste from reprocessing is stored in transport and storage containers with double lid systems that are equipped with metal seals completing the primary sealing barrier. The tasks of the Bundesanstalt für Materialforschung und -prüfung (BAM) within the interim storage licensing procedures ruled by the German Atomic Energy Act include the long-term safety evaluation of the container design regarding the permanently safe enclosure of the inventory. In order to generate a knowledge base for the safety evaluation, research regarding the long-term behavior of the critical components is performed. So far, the containers are licensed for an interim storage period of 40 years. However, due to significant delays in establishing a final repository, the required time span for interim storage is expected to increase significantly. Thus, a widespread investigation program is run to gain systematic data on the long-term behavior of the seals and to develop prediction models.
Long-term seal investigations consider the development of their restoring seal force, their useable resilience and their achievable leakage rate caused by aging at temperatures ranging from room temperature up to 150 °C. This year, the total time span of the tests reaches 10 years. Furthermore, seal segments are aged at the selected temperatures for up to 300 days. From these segments additional information on the sealing behavior, changes of the seal contact and the material behavior is gained.
This contribution deals with the current results of the long-term seal investigations at BAM. Furthermore, insights of the more in-depth component and material investigations of the metal seals with focus on the seal contact development are discussed and the ongoing work aiming for an analytical description of the thermo-mechanical aging effects on metal seals are presented.
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.
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.
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.
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.
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.
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.
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.
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.
In Germany, the concept of dry interim storage in dual purpose metal casks before disposal is being pursued for spent nuclear fuel (SNF) and high level waste (HLW) management. The main safety relevant components are the thick-walled dual purpose metal casks. These casks consist e.g. of a monolithic cask body with integrated neutron shielding components (polymers, e.g. polyethylene) and a monitored double lid barrier system equipped with metal and elastomer seals. The metal seals of this bolted closure system guarantee the required leak-tightness whereas the elastomer seals allow for leakage rate measurement of the metal seals.
This presentation provides an overview of BAM proactive R&D projects related to the long-term behavior and degradation effects of metal seals, elastomer seals and polyethylene used as neutron shielding material. Particular attention is paid to the approach and first results of the third-party-founded research project LaMEP with the aim of further closure of existing knowledge gaps of safety relevant aging effects of such cask components.
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.
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 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.
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.
In Germany spent nuclear fuel is stored and transported in casks that possess bolted lid systems equipped with double jacket metal seals of Helicoflex® type in order to enable safe enclosure of the radioactive inventory. A dry interim storage period of 40 years was planned and the casks are licensed for that time span. However, due to political reasons and delayed disposal projects this time span is expected to increase significantly. It is therefore necessary to evaluate the long-term sealing behavior of the casks exceeding 40 years of operating time. In this paper, we discuss our approach to investigate the aging behavior of such metal seals, and to predict the long-term sealing behavior.
Accelerated aging component tests with seals are performed at temperatures up to 150°C to investigate the course of seal force, useable resilience and leakage rate. Even though these tests have already shown a significant decrease in seal force and useable resilience after aging times of less than 1 year, for most seals the leakage rate stayed better than the specified value. However, observation of the leakage rate has to be continued to determine the aging effect on the seal properties. As a main influence on the seal long-term behavior the increasing permanent deformation of the outer jacket has been recognized. It is made of aluminum or silver which means that the temperatures that are relevant for the aforementioned application in casks lead to creep deformation.
For further investigation of seal behavior a comprehensive research program concerning the material characteristics and aging behavior of the individual seal components, with an emphasis on the outer jacket material, has been launched. The aim is to get a better understanding of the time and temperature dependent creep mechanisms and deformation. The examinations are separated into tests on seal segments and tests on standardized specimen.
In order to be able to study the aging process, seal segments are compressed in flanges and stored at temperatures ranging from room temperature to 150°C. After defined time intervals the segments are analyzed by using standardized tests including structure investigation and creep tests. The results are compared with the behavior of the specimen basic raw material. This is done to ensure comparability of the thin jacket material and additional sheet material used for standardized tests. Thus, the prediction of component changes after different aging times at different temperatures can be made. As a result forecasts on the long term seal behavior are intended.
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.
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.
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.
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.
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.
Unsere Aufgabe im Fachbereich 3.4 der Bundesanstalt für Materialforschung und prüfung (BAM) ist die sicherheitstechnische Begutachtung von Transport- und Lagerbehältern für radioaktiven Abfall, die für langfristige Zwischenlagerung ausgelegt sind. Ein Arbeitsschwerpunkt ist die Bewertung der Lebensdauer von Metall- und Elastomerdichtungen in den Behältern im Hinblick auf die Anforderungen für langfristige Behältersicherheit (min. 40 Jahre in Deutschland). Um die Eigenschaftsänderungen der Elastomerdichtungen während einer beschleunigten Alterung über lange Zeiträume (bis zu fünf Jahre) untersuchen zu können, wurde ein Alterungsprogramm an ausgewählten Elastomeren (HNBR, EPDM, FKM) begonnen.
Im Gegensatz zu Normalterungsverfahren altern wir keine Normteile, sondern O-Ringe im unverpressten sowie verpressten Zustand. Diese Vorgehensweise ermöglicht die Bewertung des Einflusses der Verpressung auf die Alterung sowie die Untersuchung des Bauteilversagens mittels Leckageratenmessungen unter anwendungsnahen Bedingungen. Weitere Charakterisierungsmethoden sind Härtemessung, dynamisch-mechanische Analyse (DMA), Thermogravimetrie (TGA), Druckspannungsrelaxation, Druckverformungsrest (DVR), Dichtebestimmung und Zugversuch. Das Ziel ist, die Leckagerate mit anderen Eigenschaften bzw. Methoden zu korrelieren, um so ein aussagekräftiges und leichter zu bestimmendes Lebensdauerkriterium für elastomere O-Ringe abzuleiten.
Während der Alterung können in Abhängigkeit von Material sowie Alterungsdauer und –temperatur Inhomogenitäten aufgrund von diffusionsbegrenzter Oxidation auftreten, durch die sich unterschiedliche Eigenschaften an der Oberfläche und im Volumen der Dichtung ergeben, was zu falschen Lebensdauerabschätzungen führen kann. Mittels Mikrohärtemessung über den Querschnitt werden diese Effekte charakterisiert und bei der Extrapolation mittels Zeit-Temperatur-Verschiebung und Arrheniusgraph berücksichtigt. Bisher liegen Daten von bis zu einem Jahr bei vier verschiedenen Temperaturen (75 °C, 100 °C, 125 °C und 150 °C) gealterten Proben vor. Nach 100 Tagen bei 150 °C weisen HNBR und EPDM schon einen DVR von über 80 % auf, aber noch keinen signifikanten Anstieg der Leckagerate. Diese sinkt zunächst während der Alterung, da die Permeabilität aufgrund von Vernetzungsreaktionen sinkt. Bei HNBR ist dies aufgrund der dominanteren Vernetzungsreaktionen während der Alterung noch stärker ausgeprägt als bei EPDM.
For many sealing applications rubbers are applied due to their special material properties and easy use. In many applications as 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 acitve 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 below ambient temperatures after a fast partial release. Despite the primarily static application conditions of many seals their behaviour after partial compression release is of interest with regard to potential decrease of leak-tightness.
For this investigation a special setup was designed which allows the partial release of compressed seal systems at different temperatures accompanied by leakage rate measurements.
The results for FKM seals are presented and discussed.