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Paper des Monats
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The German approach of storing spent nuclear fuel in dual purpose casks until final disposal is based on individually licensed storage sites concerning specific nuclear inventories and dual purpose cask types. The currently approved license period is maximum 40 years.
With nuclear policy changes including the phase-out decision of 2011 and a new approach for the HLW repository siting process set up 2013 by law also the spent fuel and HLW management strategy has to be adapted. This includes the timely development of disposal container concepts as part of the overall repository siting process and the need for longer interim storage periods until final disposal. Other aspects affect new regulations about the financing of the nuclear waste management by the industry and the public sector, the restructuring of responsible authorities in 2016/2017 and the adaption of R&D funding programs addressing also pre-disposal (or extended interim storage) issues.
BAM as a Federal Research Institute has been responsible for or in charge of container safety Evaluation for transport and storage casks for radioactive waste for several decades and started addressing potential Extended interim storage issues already several years ago. This included participation in international projects at the IAEA or in the U.S. Extended Storage Collaboration Program (ESCP) as well as long term laboratory tests with metal seals, elastomeric seals and polymers for neutron shielding purposes. Test results of BAM are published regularly and gained data provide valuable information about thermo-mechanical and radiological degradation effects as well as the long term Performance of respective cask components. Regarding the reliable extrapolation and prediction of the long term Performance of cask materials and components for time periods of up to 80 or even 100 years the continuation and extension of laboratory tests and the development of analytical and numerical simulation models and tools is essential and under way.
With the clear expectation of the need for extending spent fuel storage in Germany beyond the initial license period of maximum 40 years additional material data and knowledge about the long term performance and integrity of casks and internals like fuel rods will be required to meet major safety goals and regulatory requirements.
Based on a broad knowledge base about fuel cladding behavior, degradation mechanisms and related potential failure mechanisms, e. g. induced by reoriented Hydride precipitation, as illustrated in this paper, a specific gap analyses for the German situation regarding fuel conditions and cladding materials should identify the specific knowledge gaps to be addressed and closed in the near future. This is of specific interest as all spent fuel assemblies are going to be transferred to dry cask storage with the next decade and as a consequence of the German nuclear phase-out decision.
Within several decades, BAM as a Federal materials research institute gathered a broad range of expertise in the safety evaluation of materials, components and casks under operational and accidental thermal and mechanical conditions. This paper elucidates selected Basic considerations regarding technical and scientific knowledge about the long term aging performance and potential failure mechanisms of fuel cladding materials.
Under consideration of the national R&D funding policy which has been adapted to the extended interim storage or pre-disposal needs and the competences of BAM, its future R&D strategy is explained and some R&D objectives have already been identified. BAM will continue and expand ist engagement in the area of investigating fuel cladding material behavior in the long term and developing validated simulation and analyses tools in collaboration with national and international partners. R&D outcomes shall improve the knowledge-base to close identified knowledge gaps in the area of demonstrating fuel cladding integrity and to provide crucial information with regard to future safety assessments for the extended interim spent fuel storage.
Characterisation of degradation and determination of end-of-lifetime criterion for O-ring seals
(2017)
The ageing of polymers, including elastomers, is an undesirable but inevitable process leading to a limited lifetime of rubber products such as seals. Independent of the application, as e.g. in automotive, piping or container applications, a long lifetime or at least a timely exchange of a seal before occurrence of critical failure is desired.
In order to investigate the degradation of material properties and to determine the lifetime of elastomers used as seals, an ageing programme was started with hydrogenated acrylonitrile butadiene rubber (HNBR), ethylene propylene diene rubber (EPDM) and fluorocarbon rubber (FKM) [1-3]. Both O-ring seals (uncompressed and compressed by 25 %) with a cord diameter of 10 mm as well as sheets with a thickness of 2 mm were aged at 75 °C, 100 °C, 125 °C and 150 °C for up to two years. The changes of material properties during ageing were characterised for each material using samples from the sheets by means of e.g. Dynamic Mechanical Analysis and tensile tests, while sealing properties such as leakage rate were determined on O-rings. The experimental results indicate that while material properties show considerable degradation effects, the static leakage rate stays constant or even decreases before failure occurs quite suddenly at advanced degradation levels. This reveals that static leakage rate has only limited sensitivity for the degradation of the seal material.
Our approach to determine a suitable end of lifetime criterion, which involves a partial decompression of the seal during the leakage test, is presented and discussed.
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.
Due to delays in the siting procedure to establish a deep geological repository for spent nuclear fuel and high level radioactive waste as well as in construction of the already licensed Konrad repository for low and intermediate level radioactive waste, extended periods of interim storage become more relevant in Germany. BAM is involved in most of the cask licensing procedures and especially responsible for the evaluation of cask-related long-term safety issues.
The long-term performance of elastomer seals for lid systems of transport and storage casks, whether used as auxiliary seals in spent fuel casks or as primary seals for low and intermediate level waste packages, is an important issue in this context. The polymeric structure of these seals causes a complex mechanical behavior with time-dependent sealing force reduction.
The results of a comprehensive purpose-designed test program consisting of basic compression and tension tests as well as relaxation tests on unaged specimens of representative types of elastomers (fluorocarbon rubber (FKM) and ethylene propylene diene rubber (EPDM)) at different temperatures and strain rates are presented. They were used to identify the constitutive behavior and to obtain parameters for finite element material models provided by the computer code ABAQUS®. After estimating the influence of uncertainties such as Poisson’s ratio and friction coefficient by sensitivity analyses, the chosen parameters had to prove their suitability for the finite element simulation of the specimen tests themselves.
Based on this preliminary work the simulation of a specific laboratory test configuration containing a typical elastomer seal with circular cross section is presented. The chosen finite element material model and the implemented parameters had to show that they are able to represent not only the specimen behavior under predominantly uniaxial load but also the more complex stress states in real components. Deviations between the measured and calculated results are pointed out and discussed.
For the consideration of long-term effects in the simulation of elastomer behavior, test results of aged specimens are needed. First information about a new test program, started recently and planned to provide these data, are given.
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 the assessment of the service lifetime of elastomeric seals that are part of the container lid system 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 1.5 years. 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 relatively constant or even decreases until shrinkage combined with the loss of resilience of the aged seal leads to leakage. This demonstrates that static leakage rate, which is the only available direct seal performance criterion, has only limited sensitivity towards the degradation of the seal material. CS data is extrapolated using time-temperature shifts and Arrhenius graphs. An exemplary CS of 50 % would be reached after approx. 1.2, 17 and 29 years at 60 °C for HNBR, EPDM and FKM respectively.
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.