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Eingeladener Vortrag
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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.
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.
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.
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.
Due to their simple and reliable application, elastomers are used for many tasks. Many fields of application like transport, aviation and process technology, entail low temperatures where proper functionality of the employed seals has to be ensured. Therefore, understanding the low temperature behavior of elastomeric seals is important for safe seal operation to restrict the temperature application range.
For all areas of application, the question of seal lifetime is also important for replacement or maintenance intervals. The lifetime is especially important in applications that allow no seal replacement. Since the seal can determine the lifetime of storage in such cases, reliable lifetime estimation is necessary for these applications, and requires an extensive knowledge of the specific aging behavior.