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Eingeladener Vortrag
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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.
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.
In this work, we focus on the behaviour of elastomer seals at low temperatures with regard to potential decrease of leak-tightness or catastrophic seal failure of O-ring rubber seals. This is required as material properties of rubbers are strongly temperature dependent but their temperature application range is not always clearly defined.
Based on previous investigations which considered the physical material properties and the seal behaviour under purely static conditions we widen the focus on the sealing performance after a fast partial relief of compressed seals and additional materials.
For the investigations, different typical rubber seal materials were used as e.g. fluorocarbon (FKM), ethylene propylene diene (EPDM) and hydrogenated acrylonitrile-butadiene (HNBR) rubber.
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.
Understanding the failure mechanisms that lead to leakage of rubber seals at low temperatures is important. Rubber properties are highly temperature dependent. Changes in behaviour at low temperatures can result from the rubber-glass transition and for some rubbers by partial crystallisation. Experimental results on the low temperature behaviour of different rubber seals were discussed to help understand seal failure processes.
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.
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. The behaviour of metallic seals, which are employed in interim storage casks for used fuel and high active waste, over time is of high importance for ensuring safe enclosure. Therefore, investigations on these systems were started at BAM to get a general understanding of the relevant processes. Our investigations comprise investigations on different parameters which influence the seal performance and the main part is focussed on the time and temperature dependent behaviour.
In this contribution an overview of the performed tests and their respective results will be given. A focus will lie on a comparison between seals with large torus diameter in comparison to small diameters.
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.
For many sealing applications rubber O-rings are applied due to their special properties and easy use. In many applications as e.g. in aviation, traffic or process technology the material can be exposed to a variety of conditions during operation as e.g. low temperatures, elevated temperatures and different media. Therefore, it is important to know the material behaviour and the seal performance under those conditions. Additionally ageing of seals is an important factor which has an influence on the long term reliability.
In this contribution we would like to discuss different aspects affecting the seal performance, lifetime estimation and address open questions which should be addressed to come to a deeper understanding of these seals commonly understood as typical machine elements.
Results of running investigations at the Bundesanstalt für Materialforschung und -prüfung (BAM), Division 3.4 “Safety of Storage Containers” are presented and discussed.
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.
Low temperature performance of rubber seals - Influence of crystallite formation on seal performance
(2018)
Rubbers are widely used as sealing materials 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 rubbers possess strongly temperature dependent material properties. At low temperatures high changes in the material properties are observed which can be caused by the rubber-glass transition (abbr. glass transition) or for some rubbers also by partial crystallisation at lower temperatures. During continuous cooling the material changes during rubber-glass transition from rubber-like entropy-elastic behaviour to stiff energy-elastic behaviour. In case of (thermal-) crystallisation the formed crystallites act as additional (physical) crosslinks within the material but the molecules in the amorphous phase can still behave like a rubber. Hence, rubbers are normally used above rubber-glass transition and (thermal-) crystallization temperature but the minimum working temperature limit is heavily depending on the application conditions. Therefore, the lower operation temperature limit of rubber seals is under investigation.
In the past we have investigated material properties and sealing behaviour of rubber seals at low temperatures. As the initial work was dedicated to purely static sealing conditions we started to investigate the effect of a small partial release of rubber seals at low temperatures to study the influence of dynamic events on leak tightness. In addition, other groups report on the influence of counterpart surface and adhesion.
In this contribution we focus on the difference between purely amorphous elastomers and elastomers which become partially crystalline at low temperatures. The influence of partial crystallization on the low temperature performance of rubber seals is discussed.