Matthias Jaunich

Acoustic data of cross linked polyethylene (XLPE) and cured liquid silicone rubber (LSR) by means of ultrasonic and low frequency DMTA

Partial discharges may cause damage to electrical insulation of high voltage equipment. They initiate elastic waves in the insulating material, e.g. in the stress cone of an outdoor termination. Localisation of the origin of such elastic waves can help to predict serious damaging processes in the electrical insulation. In order to measure and evaluate the wave propagation effects in typical multilayered elastomeric structures, knowledge of the material properties is required. The propagating velocity and the attenuation of longitudinal waves are important parameters. Values for these quantities found in the literature were not appropriate. Therefore, for cross-linked polyethylene (XLPE) and cured liquid silicone rubber (LSR), the longitudinal wave velocity and the attenuation were evaluated in the temperature interval from -20°C to 50°C and in the frequency range from 200 kHz to 600 kHz using a two-sample ultrasound technique. The loss factor was determined from these measured quantities. Additionally, low frequency Dynamic Mechanical Thermal Analysis (DMTA) was applied to investigate LSR and XLPE in a temperature interval between -100 and 50°C and to check qualitatively the ultrasound data.

Understanding low temperature properties of elastomer seals

Abstract Elastomers are widely used as the main sealing materials for containers for low and intermediate level radioactive waste and as an additional component to metal seals in spent fuel and high active waste containers. The safe encapsulation of the radioactive container inventory has to be guaranteed according to regulation and appropriate guidelines for long term storage periods as well as for temperatures as low as −40°C during transport. Therefore, the understanding of failure mechanisms that lead to leakage at low temperatures is of high importance. It is known that the material properties of elastomers are strongly temperature dependent. At low temperatures, this is caused by the rubber–glass transition (abbreviated: glass transition). During continuous cooling, the material changes from a rubber-like entropy elastic to a stiff energy elastic behaviour, which allows nearly no strain or retraction. Hence, rubbers are normally used above their glass transition, but the minimum working temperature limit is not defined precisely; this can cause problems during the above noted applications. Therefore, the lower operation temperature limit of elastomer seals must be determined in dependence of the material properties. Differential scanning calorimetry (DSC) and dynamic mechanical analysis (DMA) are combined with standardised measurements to determine the compression set according to ISO 815. To reduce the test time of the standard tests, a faster technique than normally used was developed. Additionally, the breakdown temperature of the sealing function of complete O ring seals was measured in a component test set-up to compare it with the results of the other tests. The experimental set-up is capable of measuring the leakage rate at low temperatures by the pressure rise method. A fluorocarbon rubber (FKM) was selected for this investigation as it is often used for radioactive waste containers. The materials (seals and test sheets) were purchased from a commercial seal producer.

Einfluss der Härtung auf die Materialeigenschaften eines Harnstoffharzes

Kurzfassung Über die in der Technik weit verbreitete typisierte Harnstoffformmasse UF 131.5, ein Aminoplast, wird berichtet, dass sie im Zuge der thermisch aktivierten Vernetzungsreaktion wegen „Überhärtung‟ mangelhafte Eigenschaften annimmt. Zur Verifizierung dieses Effektes werden mithilfe der Ultraschall-Prozesskontrolle gezielt Proben unterschiedlicher Aushärtegrade hergestellt. Sie werden mit verschiedenen Methoden, wie der „Kochprobe‟ und der Thermoanalyse, charakterisiert und auf ihre Materialeigenschaften untersucht. Dabei zeigt sich ein deutlicher Einfluss der Härtezeit auf die Glasübergangstemperatur der Formmasse. In den mechanischen Eigenschaften ist eine Veränderung allerdings nur in der Schlagzähigkeit festzustellen, die sich mit steigender Härtezeit sogar wesentlich verbessert.

Discoloration Effects of High-Dose γ-Irradiation and Long-Term Thermal Aging of (U)HMW-PE

Two polyethylene types with ultra-high (UHMW-PE) 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 gamma source. Subsequently, thermal aging at 125°C was applied for up to one year. Degradation effects in the materials were characterized using colorimetry, UV-Vis spectroscopy, 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 from annealable color centers in the form of free radicals that are trapped in the crystalline regions of the polymer and recombine at elevated temperatures. For the antioxidant-containing HMW-PE, 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.

Investigations of Elastomeric Seals—Low-Temperature Performance and Ageing Behaviour

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 behaviour 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 behaviour.

Relation between dielectric and mechanical losses in ferroelectric poly(vinylidene fluoride — hexafluoropropylene) films

The temperature dependences of dielectric permittivity and elastic modulus of poly(vinylidene fluoride — hexafluoropropylene) (P(VDF-HFP)) are compared and explained by use of structural data obtained by differential scanning calorimetry and X-ray analysis. Special emphasis is put on the effect of uniaxial stretching which renders the polymer ferroelectric. It is shown that dielectric and mechanical relaxations at the glass transition (αa relaxation) are closely related and not significantly affected by stretching. It is further confirmed that stretching destroys the non-polar spherulitic crystalline structure and produces relatively small-sized polar crystallites. This manifests in the disappearence of the so-called αc relaxation which is associated to molecular motions within the spherulitic crystalline lamellae. However, there are discrepancies between dielectric and mechanical losses above the glass transition which point towards a still not described structural transition.

Investigation of Long-Term Behaviour of Elastomeric Seals for Transport and Storage Packages

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.

Testing and Numerical Simulation of Elastomers: From Specimen Tests to Simulation of Seal Behavior Under Assembly Conditions

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.

Testing and Numerical Simulation of Elastomeric Seals Under Consideration of Time Dependent Effects

Due to delays in the siting procedure to establish a deep geological repository for spent nuclear fuel and high level waste and in construction of the already licensed Konrad repository for low and intermediate level waste, extended periods of interim storage will become more relevant in Germany. BAM is involved in most of the cask licensing procedures and is responsible for the evaluation of cask-related long-term safety issues. Elastomeric seals are widely used as barrier seals for containers for low and intermediate level radioactive waste. In addition they are also used as auxiliary seals in spent fuel storage and transportation casks (dual purpose casks (DPC)). To address the complex requirements resulting from the described applications, BAM has initiated several test programs for investigating the behavior of elastomeric seals. These include experiments concerning the hyperelastic and viscoelastic behavior at different temperatures and strain rates, the low temperature performance down to -40°C, the influence of gamma irradiation and the aging behavior. The first part of the paper gives an overview of these tests, their relevant results and their possible impact on BAM’s work as a consultant in the framework of approval and licensing procedures. The second part presents an approach of the development of a finite element model using the finite element code ABAQUS®. The long-term goal is to simulate the complex elastomeric behavior in a complete lid closure system under specific operation and accident conditions.