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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.
EPDM, HNBR and FKM materials were exposed at 150 ◦C to air under atmospheric pressure and to hydrogen at 50 bar for different ageing times. All measurements after hydrogen exposure were conducted on samples in degassed condition to assess irreversible effects resulting from that exposure and to compare them to those after ageing in air. Density, hardness, tensile properties, compression set, and hydrogen permeability of all samples were analysed. In both ageing environments, HNBR exhibited the most significant changes of material properties.
However, for both EPDM and HNBR, considerably less severe ageing effects were observed under hydrogen in comparison to ageing in air. On the other hand, FKM showed about the same low level of deterioration in both ageing environments but exhibited poor resistance against damage due to rapid gas decompression in hydrogen environment that can lead to seal failure. The obtained results may serve as a guidance toward a better understanding for design and utilisation of elastomeric materials in future hydrogen infrastructure components.
A state-of-the-art (SOTA) review on characterisation of spent nuclear fuel (SNF) properties in terms of source term and inventory assessment (neutron, gamma-ray emission, decay heat, radionuclide inventory, elemental content) and in terms of out-of-core fuel performance (cladding performance and fuel integrity in view of the safety criteria for SNF interim storage, transport and canister packaging) using several numerical and experimental approaches and methodologies is presented. This SOTA report is a result of the spent fuel characterisation (SFC) work package as part of the European Joint Programme on Radioactive Waste Management (EURAD), which offers an overview of the status of knowledge in the field of SNF characterisation and assessment during the pre-disposal phase. The document aims to focus on the current safety-significant gaps and related challenges, providing a direct link to the goals of the mandated actors of EURAD. The report is expected to be used by all EURAD colleagues in their national programmes as a key resource for knowledge management programmes and to contribute to demonstrating and documenting the state-of-the-art.
The prevention of brittle fracture of spent fuel claddings during long-term dry interim storage is based on experimental investigations, numerical analyses and assessment methods for predicting the mechanical behavior and determining limiting conditions. The ring compression test (RCT) is an established experimental method for characterizing cladding material. Test results for various high-burnup pressure water reactor zirconium-based fuel cladding alloys (e.g., ZIRLO®, M5®) are publicly available. To reduce the effort associated with irradiated samples in hot cells, it is helpful to perform studies on unirradiated surrogate cladding material. Based on such experimental data, load-displacement curves were numerically analyzed for selected cladding materials. In the presence of radial hydrides, a sample may suddenly fail by fracture even at small deformations. Noticeable load drops in the RCT occur associated to unstable crack propagation through the radial hydride network. The failure mechanism is quasi-cleavage in the hydrides and micro-void nucleation, growth, and coalescence in the zirconium matrix, with ductile tearing patches connecting neighboring hydrides. The failure process was simulated by cohesive zones controlled by the fracture energy and the cohesive strength. A modeling approach is presented in which the radial hydride morphology is taken into account. Based on the developed fracture mechanics approach with cohesive zone modeling, not only the deformation behavior but also the failure behavior of irradiated as well as unirradiated claddings with radial hydrides under RCT loading conditions can be adequately described.
Task 3 of Work package 8 (Spent Fuel Characterization) of the European Joint Programme on Radioactive Waste Management (EURAD) investigates the behaviour of nuclear fuel and cladding after discharge. The aim of the work is to understand and describe the be-haviour of spent nuclear fuel (SNF), irradiated cladding, fuel/cladding chemical interaction (FCCI) and ageing under conditions of extended interim storage, transportation and em-placement in a final disposal system. BAM contributes to the project as partner and leads Task 3. The presentation gives an overview of the project status, main achievements in experimental work and modelling studies, deviations from the plan, delays and challenges ahead.
The prevention of brittle fracture of spent fuel claddings during long-term dry interim storage is based on experimental investigations, numerical analyses and assessment methods for predicting the mechanical behavior and determining limiting conditions. The ring compression test (RCT) is an established experimental method for characterizing cladding material. Test results for various high-burnup pressure water reactor zirconium-based fuel cladding alloys (e.g., ZIRLO®, M5®) are publicly available. To reduce the effort associated with irradiated samples in hot cells, it is helpful to perform studies on unirradiated surrogate cladding material. Based on such experimental data, load-displacement curves were numerically analyzed for selected cladding materials. In the presence of radial hydrides, a sample may suddenly fail by fracture even at small deformations. Noticeable load drops in the RCT occur associated to unstable crack propagation through the radial hydride network. The failure mechanism is quasi-cleavage in the hydrides and micro-void nucleation, growth, and coalescence in the zirconium matrix, with ductile tearing patches connecting neighboring hydrides. The failure process was simulated by cohesive zones controlled by the fracture energy and the cohesive strength. A modeling approach is presented in which the radial hydride morphology is taken into account. Based on the developed fracture mechanics approach with cohesive zone modeling, not only the deformation behavior but also the failure behavior of irradiated as well as unirradiated claddings with radial hydrides under RCT loading conditions can be adequately described.
In this work we present results for three typical sealing materials (EPDM, HNBR, FKM) after up to 100 days ageing at high temperature under hydrogen. To allow for a better evaluation of the occurring changes the results are compared with effects of ageing in air on the material properties. Despite the common assumption that ageing under hydrogen atmosphere is expected to be less severe for the material in com-parison to air ageing, this is not seen for every material.
The storage of spent fuel and high level radioactive waste in Germany is performed in interim storage containers with double lid systems. The lids are bolted and equipped with metal seals (e.g. Helicoflex®) to ensure the safe enclosure of the inventory. The used metal seals have a layered structure consisting of three components as can be seen schematically in the cross-sectional view in Fig. 1.
In the center a helical spring is positioned that is surrounded by two C-shaped jackets and is mainly responsible for generation of the required restoring force. The inner jacket is made of stainless steel and homogenizes the restoring force of the helical spring. The outer jacket is made of silver or aluminium which both are soft metals in comparison to the contact partners (lid and container body). During bolting of the lid to the container body the seal is compressed. The generated restoring force of the helical spring causes a plastic deformation of the outer jacket and adapts to the surfaces of the lid and the container body. Hence, leakage paths are closed and the sealing function is generated.
Typical durations for existing interim storage licenses in Germany are 40 years, but it can be expected that they have to be extended to longer periods as a final repository will not be available before the end of the running licence periods. This extension of license periods requires a solid understanding of the long-term behaviour of the seals under storage conditions. To meet this challenge long-term investigations have been started at Bundesanstalt für Materialforschung und –prüfung (BAM) in 2009. These tests focus on seals assembled in test flanges which are stored at temperatures ranging from room temperature to 150 °C for accelerated ageing. The aged seals are tested repeatedly after certain ageing steps and the leakage rate as indicator for sealing performance, the remaining seal force, and the useable resilience upon decompression are determined.
In the poster an update on the performed investigations in respect to earlier publications (Grelle et al. 2019, Goral et al. 2023) will be given and the implications of the results for resilient long term safety will be presented. Additionally, a focus will be laid on the currently planned further investigations and the question “What is additionally needed for evaluation of an interim storage period extension in regard to the used metal seals?” will be addressed.
Beginning in 1976 the former iron ore mine Konrad was geologically investigated concerning its suitability as a location for a German final repository for low and intermediate level waste. After a comprehensive licensing procedure it was approved and is now being prepared and equipped for the planned start of storage in 2027. At the end of the 1980s, the requirements for waste containers for storage in this repository were defined for the first time on the basis of an incident analysis of the on-site handling procedures, beginning with the unloading of the packages after the arrival at the site up to the final positioning in the underground storage galleries. A 5-meter drop onto the rock ground of the mine was identified as the covering case for high mechanical requirements (ABK II container class). In contrast to the 9-meter drop according to the IAEA Regulations for the Safe Transport of Radioactive Material, the 5-meter drop is performed onto a hard but not essentially unyielding target. The container is typically not protected by an impact limiter. The requirements for a potential test facility are described in the regulations for the Konrad repository. The mechanical strength of the target is defined as a concrete strength equivalent to the identified properties of the rock ground of the mine.
Since 1991 BAM has consistently used precast reinforced concrete slabs as target for drop tests in the framework of licensing procedures as well as in research projects. While the original design fulfilled the requirement for the integrity of the concrete slab in most cases, it failed when drop tests onto an edge of a container were performed. A redesigned concrete slab developed in a research project and suggested as a reference target in 2009 has been successfully used in Konrad licensing procedures since then.
The paper gives a brief overview of the historical development and it describes BAM’s efforts and approaches to continuously guarantee a concrete slab of defined quality and to provide a test setup for valid drop tests from the applicants and the authorities view.
Beginning in 1976 the former iron ore mine Konrad was geologically investigated concerning its suitability as a location for a German final repository for low and intermediate level waste. After a comprehensive licensing procedure it was approved and is now being prepared and equipped for the planned start of storage in 2027. At the end of the 1980s, the requirements for waste containers for storage in this repository were defined for the first time on the basis of an incident analysis of the on-site handling procedures, beginning with the unloading of the packages after the arrival at the site up to the final positioning in the underground storage galleries. A 5-meter drop onto the rock ground of the mine was identified as the covering case for high mechanical requirements (ABK II container class). In contrast to the 9-meter drop according to the IAEA Regulations for the Safe Transport of Radioactive Material, the 5-meter drop is performed onto a hard but not essentially unyielding target. The container is typically not protected by an impact limiter. The requirements for a potential test facility are described in the regulations for the Konrad repository. The mechanical strength of the target is defined as a concrete strength equivalent to the identified properties of the rock ground of the mine.
Since 1991 BAM has consistently used precast reinforced concrete slabs as target for drop tests in the framework of licensing procedures as well as in research projects. While the original design fulfilled the requirement for the integrity of the concrete slab in most cases, it failed when drop tests onto an edge of a container were performed. A redesigned concrete slab developed in a research project and suggested as a reference target in 2009 has been successfully used in Konrad licensing procedures since then.
The paper gives a brief overview of the historical development and it describes BAM’s efforts and approaches to continuously guarantee a concrete slab of defined quality and to provide a test setup for valid drop tests from the applicants and the authorities view.
Beginning in 1976 the former iron ore mine Konrad was geologically investigated concerning its suitability as a location for a German final repository for low and intermediate level waste. After a comprehensive licensing procedure it was approved and is now being prepared and equipped for the planned start of storage in 2027. At the end of the 1980s, the requirements for waste containers for storage in this repository were defined for the first time on the basis of an incident analysis of the on-site handling procedures, beginning with the unloading of the packages after the arrival at the site up to the final positioning in the underground storage galleries. A 5-meter drop onto the rock ground of the mine was identified as the covering case for high mechanical requirements (ABK II container class). In contrast to the 9-meter drop according to the IAEA Regulations for the Safe Transport of Radioactive Material, the 5-meter drop is performed onto a hard but not essentially unyielding target. The container is typically not protected by an impact limiter. The requirements for a potential test facility are described in the regulations for the Konrad repository. The mechanical strength of the target is defined as a concrete strength equivalent to the identified properties of the rock ground of the mine.
Since 1991 BAM has consistently used precast reinforced concrete slabs as target for drop tests in the framework of licensing procedures as well as in research projects. While the original design fulfilled the requirement for the integrity of the concrete slab in most cases, it failed when drop tests onto an edge of a container were performed. A redesigned concrete slab developed in a research project and suggested as a reference target in 2009 has been successfully used in Konrad licensing procedures since then.
The paper gives a brief overview of the historical development and it describes BAM’s efforts and approaches to continuously guarantee a concrete slab of defined quality and to provide a test setup for valid drop tests from the applicants and the authorities view.
Cohesive Zone Modelling Approach on Irradiated Claddings Subjected to Long-Term Dry Interim Storage
(2023)
Long-term dry interim storage may adversely affect the mechanical properties of spent fuel rods, possibly resulting in a reduced resilience during handling or transport after storage. Pre-storage drying and the early stage of interim storage can subject the cladding to higher temperatures and higher pressure induced tensile hoop stresses than those associated with in-reactor operation and pool storage. Under these conditions, radial hydrides may precipitate in zirconium-based alloys (Zircaloy) during slow cooling, which may result in embrittlement of the cladding material and eventually a sudden failure of cladding under additional mechanical loads. Especially long, continuous radial hydride structures and low temperature can cause severe embrittlement of claddings and finally failure by fracture even at small deformations. The focus of the presented research is on the development of appropriate numerical methods for predicting the mechanical behaviour and identification of limiting conditions to prevent brittle fracture of Zircaloy claddings. An iterative inverse analysis method is used for deriving the elastic-plastic material properties in the hoop direction of a ring-shaped sample. A modelling approach based on cohesive zones is explained which can reproduce the propagation of cracks initiated at radial hydrides in the zirconium matrix. The developed methods are applied to defueled samples of cladding alloy ZIRLO®, which were subjected to a thermo-mechanical treatment to reorient existing circumferential hydrides to radial hydrides. A selected sample showing sudden load drops during a quasi-static ring compression test is analysed by means of fracture mechanics for illustrative purposes.
The European Joint Programme on Radioactive Waste Management (EURAD) is working on Spent Fuel Characterization (SFC) in its work package (WP) 8. Inspired by the EURAD activities, the International Atomic Energy Agency (IAEA) established an international Coordinated Research Project (CRP) on SFC. The EURAD WP SFC
participants are collaborating as a team on the IAEA CRP on SFC. The EURAD WP SFC project consists of four tasks. Task 3 investigates the behaviour of nuclear fuel and cladding after discharge. The aim of these activities is to understand and describe the evolution of the cladding-pellet system and its ageing under conditions of extended interim storage, transportation and emplacement in a final disposal system. At a Consultancy Meeting, BAM as contributor to Task 3 presented current results of the failure analysis of irradiated ZIRLO® claddings under conditions of the Ring Compression Test.
Elastomeric seals are essential components in the infrastructure which prevent leakage of gas and proper function of technical devices and are therefore highly safety relevant. For proper function a remaining resilience and tolerance to pressure changes is required.
The ageing of 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. automotive, piping or container applications, a long lifetime or at least a timely exchange of a seal before occurrence of critical failure is desired.
Hydrogen is a key element for the energy turnaround and therefore the compatibility of seals with hydrogen is essential. In addition to the effect of hydrogen uptake and release, which might also cause destructive effects such as rapid gas decompression, ageing at high temperature under hydrogen atmosphere is of interest too. Most of the existing work is addressing the performance of new materials and comprises only very limited investigations concerning long-term use and the behaviour of aged materials in contact with hydrogen. As ageing can lead to substantial changes of material properties, it must be evaluated whether these changes are beneficial or deteriorating for the component function.
In this work we present and compare results of the characterisation of three sealing materials (EPDM, HNBR, FKM) after ageing at high temperature under hydrogen and air. Despite the common assumption that ageing under hydrogen atmosphere should be less severe for the material in comparison to air ageing, this is not the case for every material.
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.
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.
German spent nuclear fuel and high level waste is stored in dry conditions in interim storage facilities until a final repository will be ready for operation in the future. Dual purpose casks are used for the packaging of the materials to ensure transportability at any time during long-term interim storage and fulfilling both requirements from interim storage as well as transport. Germany’s 2011 decision to phase out utilization of nuclear energy has led to a high demand for casks for decommissioning power plants as quickly as possible. Cask serial production will continue at a high level for the next few years. In the process, a system of quality assurance measures ensures that every cask reliably complies with design specification according the transport approval certificate and storage license.
When the first casks were manufactured in Germany about 40 years ago, quality assurance was oriented towards pressure vessel and general nuclear manufacturing. The system was continuously adapted to the state of the art. In particular serial production, globalization of manufacturing and deep supplier chains had to be taken into account. The system of quality assurance measures applied today for cask manufacturing shall be presented here.
The quality assurance measures can be categorized as system-related and design-related. With respect to transport regulations for example, they are independently approved and monitored by the competent authority BAM and its authorized inspection experts. The qualification of the applicant is reviewed first in the context of the design approval procedure and then periodically. The qualification of component and cask manufacturers is also checked at the start of manufacturing and then periodically. Before the start of manufacturing documents such as quality plans are pre-assessed. Manufacturing and inspection are then performed according to the pre-assessed documents. Cask manufacturing is completed by a final inspection before commissioning. Periodic inspections during operation ensure preservation of the properties specified in the approval certificate over package life time. The type and the time interval of periodic inspections depend on the use of the package. For transport after interim storage a system of specific tests and inspections is prescribed.
Long-term dry interim storage may adversely affect the mechanical properties of spent fuel rods, possibly resulting in a reduced resilience during handling or transport after storage. Since the cladding is the first barrier for the spent fuel pellets, its integrity must be demonstrated until the end of interim storage and subsequent transportation. An established method for characterizing the cladding material is the ring compression test, in which a small, cylindrical sample of the cladding tube is subjected to a compressive load. This test is a laboratory representation of a load case where the fuel rod is crushed.
Pre-storage drying and the early stage of interim storage can subject the cladding to higher temperatures and higher pressure induced tensile hoop stresses than those associated with in-reactor operation and pool storage. Under these conditions, radial hydrides may precipitate in zirconium-based alloys (Zircaloy) during slow cooling, which result in embrittlement of the cladding material and eventually a possible sudden failure of cladding integrity under additional mechanical loads. Especially long, continuous radial hydride structures and low temperature can cause severe embrittlement of claddings and finally failure by fracture even at small deformations. Therefore, the study of hydride morphology plays an important role in describing the brittle failure behaviour of the claddings.
The focus of the presented research is on the development of appropriate numerical methods for predicting the mechanical behaviour and identification of limiting conditions to prevent brittle fracture of Zircaloy claddings. Typical hydride morphologies are shown. An iterative inverse analysis method is described for deriving the elastic-plastic material properties in the hoop direction of a ring-shaped sample. A modelling approach based on cohesive zones is explained which is able to reproduce the propagation of cracks initiated at radial hydrides in the zirconium matrix. The developed methods are applied to defueled samples of cladding alloy ZIRLO®, which were subjected to a thermo-mechanical treatment to reorient existing circumferential hydrides to radial hydrides. A selected sample showing sudden load drops during a quasi-static ring compression test is analysed by means of fracture mechanics for illustrative purposes.
This project as part of the European Joint Programme on Radioactive Waste Management has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 847593.
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.
Recovery is an important measure for seal applications representing to which extent the elastomer regains its initial shape after deformation and release of an applied force. Compression set (CS) indicates the degree of recovery. Ethylene propylene diene rubber (EPDM) was aged at 75 ◦C, 100 ◦C, 125 ◦C and 150 ◦C for different ageing times up to five years and compression set measurements were performed at different times after disassembly and after additional tempering. Short- and long-term recovery up to one year after release for samples aged at 125 ◦C and 150 ◦C was also studied. To assess the curvature in the Arrhenius diagram that may occur due to non-sufficiently aged specimens, a degradation-rate based model was fitted to the CS data after tempering. For each ageing temperature, two decay fit functions were proposed, each with an activation energy and a corresponding degradative process. The influence of ageing on the leak-tightness after fast small partial release is investigated and estimated through the analysis of the shift factors from time temperature superposition (TTS) of CS measurements at different times after disassembly. Shift factors of CS measurement after 1 s and after additional tempering are in good agreement.
SFC is a work package in Eurad that investigates issues related to the properties of the spent nuclear fuel in the back-end of the nuclear fuel cycle. Decay heat, nuclide inventory, and fuel integrity (mechanical and otherwise), and not least the related uncertainties, are among the primary focal points of SFC. These have very significant importance for the safety and operational aspect of the back-end. One consequence is the operation economy of the back-end, where deeper understanding and quantification allow for significant optimization, meaning that significant parts of the costs can be reduced. In this paper, SFC is described, and examples of results are presented at about half-time of the work package, which will finish in 2024. The DisCo project started in 2017 and finished in November 2021 and was funded under the Horizon 2020 Euratom program. It investigated if the properties of modern fuel types, namely doped fuel, and MOX, cause any significant difference in the dissolution behavior of the fuel matrix compared with standard fuels. Spent nuclear fuel experiments were complemented with studies on model materials as well as the development of models describing the solid state, the dissolution process, and reactive transport in the near field. This research has improved the understanding of processes occurring at the interface between spent nuclear fuel and aqueous solution, such as redox reactions. Overall, the results show that from a long-term fuel matrix dissolution point of view, there is no significant difference between MOX fuel, Cr+Al-doped fuel, and standard fuels.
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.
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.
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 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 measurements across the section of O-rings. Oxidation profiles were determined by applying the model of Wise et al. to the IRHD experimental results.
Suitable containers for receiving high-level radioactive waste are a key elements of every repository system concerning different host rocks like rock salt, claystone and crystalline rock as being considered in Germany. The disposal container design is decisive regarding boundary conditions for the transport, emplacement techniques, and the operational and long-term safety assessment. The systematic derivation of the requirements to be placed on disposal containers forms the basis for a targeted, comprehensible and transparent development of containers that meet the requirements. The presentation summarizes the outcomes of the research project KoBrA.
Es werden Methoden zur sicherheitstechnischen Bewertung des mechanischen Verhaltens von Brennstabhüllrohren entwickelt, um sprödes Versagen in Belastungsszenarien nach längerfristiger trockener Zwischenlagerung zu verhindern. Unbestrahlte Brennstabhüllrohrsegmente aus der Zirkoniumlegierung ZIRLO® wurden hydriert und thermomechanischen Behandlungen unterzogen, um Hüllrohrmaterial durch Ausscheidung radialer Hydride zu verspröden. Die Proben mit radialen Hydriden wurden im Ring Compression Test (RCT) bei Raumtemperatur untersucht. Bereits bei kleinen Probenverformungen wurden abrupte Kraftabfälle mit instabiler Rissausbreitung durch das Netzwerk radialer Hydride beobachtet. Die Risslängen erreichten in einigen Fällen bis zu 90 % der Wanddicke. Der mikromechanische Versagensmechanismus ist Quasi-Spaltbruch in den Hydriden und Porenbildung, -wachstum und -vereinigung in der Zirkoniummatrix an den duktilen Brücken zwischen benachbarten Hydriden. Es wurde ein Finite-Elemente-Modell des Ring Compression Tests erstellt, um das Versagensverhalten zirkoniumbasierter Legierungen mit radialen Hydriden im RCT zu analysieren. Die Fließkurve für das elastisch-plastische Materialmodell des Matrixmaterials wurde durch eine inverse Finite-Elemente-Analyse ermittelt. Kohäsivzonenmodelle wurden benutzt, um die plötzlichen Kraftabfälle zu reproduzieren. Es wurde ein mikromechanisches Modell mit statistisch generierten Matrix-Hydrid-Verteilungen entwickelt, das zwischen sprödem Versagen entlang der Hydride und duktilem Versagen der Zirkoniummatrix in der Kohäsivzone unterscheidet. Für das jeweilige Materialverhalten wird ein lokales zweiparametriges Versagenskriterium auf Grundlage der Kohäsionsfestigkeit und der Separationsenergie bei einer festgelegten Form des Kohäsivgesetzes vorgeschlagen. Geeignete Kohäsivparameter lassen sich mit einer inversen Finite-Elemente-Analyse des Versagensverhaltens von hydrierten Proben im Ring Compression Test bestimmen. In den Simulationen lag der Schwerpunkt auf dem ersten Kraftabfall. Die Berechnungsergebnisse stimmen gut mit den RCT-Ergebnissen überein. Es konnte gezeigt werden, dass die Rissinitiierung und -ausbreitung stark von der speziellen Anordnung der radialen Hydride und Matrixbrücken in der Bruchzone abhängt. Die numerische Modellbildung wurde an Versuchen mit bestrahlten Proben aus der Zirkoniumlegierung M5® validiert.
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.
The thermal expansion of polymeric parts can be an issue in many applications where the available space is limited, or exact dimensions of the part are required. For this study, a device was designed and built that allowed measuring the thermal expansion simultaneously in all three spatial directions on cubic samples with real-scale dimensions (78 mm edge length). The results are shown between 25 °C and 125 °C for two PE materials, one HMWPE and one tempered UHMWPE, for non-irradiated samples as well as cubes that have been irradiated with 100 and 400 kGy. The results measured with the new device were very similar to those measured with conventional thermo-mechanical analysis equipment and to literature data of UHMWPE. The HMWPE material shows a much larger thermal expansion coefficient in one direction compared to the other two directions during the first heating due to frozen stresses from the pressing step during material manufacturing. These stresses are mostly released by the expansion during the first heating, so that the expansion during the second heating is more uniform. The overall volumetric expansion is the same for both heating runs. By contrast, the tempered UHMWPE material shows no significant difference between first and second heating run, as the stresses from processing could already relax in the tempering step. The irradiation treatment does not affect the values significantly for the given test set-up.
At BAM, which is a 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 casks. Besides examining the low-temperature behaviour and irradiation effects of elastomeric seals, it is our goal to estimate 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 five years. In order to assess sealability, O-rings were 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 were 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, material properties such as hardness, elastic modulus, glass transition temperature and viscoelastic loss factor as well as relaxation and recovery behaviour are examined in order to understand the underlying ageing mechanisms in each material. For obtaining results closely related to practical conditions, O-rings with a full-scale cord diameter of 10 mm were aged. However, this set-up can lead to heterogeneous aging caused by diffusion-limited oxidation (DLO) effects, resulting in distorted bulk properties such as compression stress relaxation and compression set. However, if DLO-affected data is excluded, extrapolations of CS data are possible using time-temperature shifts and Arrhenius graphs.
For selecting an appropriate end-of-lifetime criterion, leakage rate measurements were performed, since leakage rate is the only characteristic directly correlated to the performance of the sealing system. A significant increase in leakage rate was considered as the end of the lifetime. However, the O-rings remained leak tight under static conditions and even exhibited an improved, i.e. decreased leakage rate while other properties already indicated strong deterioration. These tests were extended by seal tests with fast partial decompression.
Overall an update will be given on the current investigations and results and the planned activities.
The European Joint Programme on Radioactive Waste Management (EURAD) is working on Spent Fuel Characterization (SFC) in its work package (WP) 8. Inspired by the EURAD activities, the International Atomic Energy Agency (IAEA) established an international Coordinated Research Project (CRP) on SFC. The EURAD WP SFC participants are collaborating as a team on the IAEA CRP on SFC. The EURAD WP SFC project consists of four tasks. Task 3 investigates the behaviour of nuclear fuel and cladding after discharge. The aim of these activities is to understand and describe the evolution of the cladding-pellet system and its ageing under conditions of extended interim storage, transportation and emplacement in a final disposal system. At the Second Research Coordination Meeting on Spent Fuel Characterization, BAM as leader of Task 3 reported on the status of the research work.
Task 3 of Work package 8 (Spent Fuel Characterization) of the European Joint Programme on Radioactive Waste Management (EURAD) investigates the behaviour of nuclear fuel and cladding after discharge. The aim of the work is to understand and describe the behaviour of spent nuclear fuel (SNF), irradiated cladding, fuel/cladding chemical interaction (FCCI) and ageing under conditions of extended interim storage, transportation and emplacement in a final disposal system. BAM contributes to the project as partner and leads Task 3. The presentation gives an overview of the project status, main achievements in experimental work and modelling studies, deviations from the plan, delays and challenges ahead.
In order to demonstrate the safety of both spent fuel and the storage system, a good understanding of the processes that might cause deterioration is required. The International Atomic Energy Agency (IAEA) continued the coordinated research on Spent Fuel Performance Assessment and Research (SPAR) into a fourth phase starting in 2015 to evaluate fuel and materials performance under wet and dry storage and to assess the impact of interim storage on associated spent fuel management activities (such as handling and transport). BAM’s understanding and experiences in the field of long-term storage of spent fuel and especially spent fuel characterization are presented to assist the preparation of the final project report.
Embrittlement of spent fuel claddings during long-term dry interim storage - Current approach at BAM
(2019)
The integrity of fuel rods and cladding tubes must be demonstrated throughout the dry interim storage of spent nuclear fuel in Germany. For at least a relevant number of casks, an extension of interim storage between 40 and 100 years is foreseeable. The drying procedure for the fuel rods in conjunction with the thermomechanical storage conditions may change the microstructure of the cladding tubes and lead to their possible embrittlement. The failure probability might increase under mechanical load by handling procedures (transport after storage) on potentially embrittled cladding tubes of fuel rods especially at low temperatures after long-term storage. Results of ring compression tests on unirradiated pre-hydrided as well as irradiated samples with radial hydrides are investigated by finite element analyses to be able to describe the failure process and to identify failure criteria.
A Memorandum of Understanding (MOU) between Argonne National Laboratory (Argonne) and the German Bundesanstalt für Materialforschung und -prüfung (BAM) was signed in October 2014. Its objectives are to promote cooperation among scientists and specialists at Argonne and BAM and establish a framework for collaboration in advanced technologies associated with the back end of the nuclear fuel cycle. Collaborative activities involving Argonne and BAM may be implemented through the promotion of joint research activities and scientific workshops and conferences; exchange of technical information; and visits by scientists, specialists, and graduate, postgraduate, and Ph.D. students. The MOU was renewed in January 2020 for another five years. Highlights of the progress and achievements are provided in identified topical areas for collaboration on ageing management guidance, storage, transportation and disposal R&D, joint conference activities, and conclude with the benefits of the MOU in fostering Argonne and BAM collaboration.
The characterization of spent fuel and radioactive waste is essential in the evaluation of the ability of these materials to meet acceptance criteria. Prior to determining a method for spent fuel characterization, it is necessary to identify the type of data required to support safety and other analyses for the storage, transportation and final disposal of spent fuel. BAM’s understanding and capabilities in the field of spent fuel characterization are presented for the scope of a coordinated research project on the topic.
A Memorandum of Understanding (MOU) between Argonne National Laboratory (Argonne) and the German Bundesanstalt für Materialforschung und -prüfung (BAM) was signed in October 2014. Its objectives are to promote cooperation among scientists and specialists at Argonne and BAM and establish a framework for collaboration in advanced technologies associated with the back end of the nuclear fuel cycle. Collaborative activities involving Argonne and BAM may be implemented through the promotion of joint research activities and scientific workshops and conferences; exchange of technical information; and visits by scientists, specialists, and graduate, postgraduate, and Ph.D. students. The MOU was renewed in January 2020 for another five years. Highlights of the progress and achievements are provided in identified topical areas for collaboration on ageing management guidance, storage, transportation and disposal R&D, joint conference activities, and conclude with the benefits of the MOU in fostering Argonne and BAM collaboration.
The general aim of this research is the development of methods for predicting mechanical behavior and identification of limiting conditions to prevent brittle failure of high-burnup (HBU) pressure water reactor (PWR) fuel cladding alloys. A finite element (FE) model of the ring compression test (RCT) was created to analyze the failure behavior of zirconium-based alloys with radial hydrides during the RCT. An elastic-plastic material model describes the zirconium alloy. The stress-strain curve needed for the elastic-plastic material model was derived by inverse finite element analyses. Cohesive zone modeling is used to reproduce sudden load drops during RCT loading. Based on the failure mechanism in non-irradiated ZIRLO® claddings, a micro-mechanical model was developed that distinguishes between brittle failure along hydrides and ductile failure of the zirconium matrix. Two different cohesive laws representing these types of failure are present in the same cohesive interface. The key differences between these constitutive laws are the cohesive strength, the stress at which damage initiates, and the cohesive energy, which is the damage energy dissipated by the cohesive zone. Statistically generated matrix-hydride distributions were mapped onto the cohesive elements and simulations with focus on the first load drop were performed. Computational results are in good agreement with the RCT results conducted on high-burnup M5® samples. It could be shown that crack initiation and propagation strongly depend on the specific configuration of hydrides and matrix material in the fracture area.
The general aim of this research is the development of methods for predicting mechanical behavior and identification of limiting conditions to prevent brittle failure of high-burnup (HBU) pressure water reactor (PWR) fuel cladding alloys. A finite element (FE) model of the ring compression test (RCT) was created to analyze the failure behavior of zirconium-based alloys with radial hydrides during the RCT. An elastic-plastic material model describes the zirconium alloy. The stress-strain curve needed for the elastic-plastic material model was derived by inverse finite element analyses. Cohesive zone modeling is used to reproduce sudden load drops during RCT loading. Based on the failure mechanism in non-irradiated ZIRLO® claddings, a micro-mechanical model was developed that distinguishes between brittle failure along hydrides and ductile failure of the zirconium matrix. Two different cohesive laws representing these types of failure are present in the same cohesive interface. The key differences between these constitutive laws are the cohesive strength, the stress at which damage initiates, and the cohesive energy, which is the damage energy dissipated by the cohesive zone. Statistically generated matrix-hydride distributions were mapped onto the cohesive elements and simulations with focus on the first load drop were performed. Computational results are in good agreement with the RCT results conducted on high-burnup M5® samples. It could be shown that crack initiation and propagation strongly depend on the specific configuration of hydrides and matrix material in the fracture area.
Since cladding acts as the first barrier for nuclear fuel, it is key to understand the degrading mechanisms leading to cladding embrittlement. Zirconium alloy based cladding samples subjected to simulated pre-storage drying conditions have shown high susceptibility to brittle failure under the occurrence of hoop stress and low temperature as expected after long-term interim storage. The stress state associated with a compressive pinch-load scenario is reproduced by the Ring Compression Test (RCT), which results in sudden failure at relatively small mechanical loads with high sensitivity to the presence of radial hydrides. As part of the BAM research project BRUZL (Fracture mechanics analysis of spent fuel claddings during long-term dry interim storage), static RCTs were conducted on non-irradiated, pre-hydrided ZIRLO® ring-shaped samples that were subjected to a radial hydride treatment. All samples failed in macroscopically brittle fashion with sudden load drops and severe crack propagation through almost the entire wall thickness. In a post-RCT examination of the fracture surfaces using scanning electron microscopy, radial hydrides could be identified as the weakest link of the structure. However, the microscopic failure mechanism is much more complex due to cracks initiating at different axial positions in depth direction of the ring, overlapping cracks, and arresting cracks. A considerable portion of the fracture surfaces appeared to have undergone plastic deformation of the zirconium matrix resulting in void growth and coalescence associated with ductile failure. The geometry of the ductile patches was measured, and the ductile surface fraction was determined. Based on these observations, a statistical model was developed that can reproduce the composition of the fracture surface as a one-dimensional projection. A micromechanically motivated cohesive zone model (CZM) was implemented in existing RCT finite element analysis (FEA) models with different constitutive laws for brittle hydrides and ductile matrix respectively. In this work, FEA results are presented for non-irradiated ZIRLO® and high-burnup M5® claddings. The impact of varying hydride-matrix combinations is discussed.
Acknowledgement:
The project was funded by the former Federal Ministry for Economic Affairs and Energy (BMWi) under contract no. 1501561.
During an extensive test programme at the Bundesanstalt für Materialforschung und prüfung, material property changes of EPDM O-rings were investigated at different ageing times and two ageing temperatures of 125∘C and 150∘C. To exclude possible diffusion-limited oxidation (DLO) effects that can distort the data, IRHD microhardness measurements were taken over the cross section of compressed O-rings. Continuous stress relaxation measurements were taken on samples free of DLO effects. The additional effect of physical processes to irreversible chemical ones during a long-term thermal exposure is quantified by the analysis of compression set measurements under various test conditions. By combining the different experimental methods, characteristic times relative to the degradation processes were determined. On the basis of experimental data, a microphysically motivated model that takes into account reversible and irreversible processes was developed. The parameter identification strategy of the material model is based on our experimental investigations on homogeneously aged elastomer O-rings. The simulated results are in good agreement with the experiments.
The excellent mechanical properties of elastomer seals at a wide range of temperatures as well as their high versatility and recovery potential under several load conditions make these materials well suitable for the application in containers designed for transport and disposal of negligible heat generating radioactive waste. While a seal exchange at defined intervals is typical in many conventional applications, it is impossible or at least hard to perform when principles of minimization of radiation exposure have to be considered which prohibit an avoidable cask handling. An extensive knowledge of the change of the elastomer properties during aging and the availability of reliable end-of-lifetime criteria to guarantee the safe enclosure of the radioactive material for the required time are mandatory. As BAM is involved in most of the national cask licensing procedures and in the evaluation of cask-related long-term safety issues, great efforts have already been made and are still ongoing to scientifically support this task.
Among other representative types of elastomers, specimen made from ethylene propylene diene rubber (EPDM) were tested before, during and after aging to capture the with respect to application most important of their complex mechanical properties.
Exemplary results of these investigations were used to calibrate material models implemented in the commercial finite element software ABAQUS/Standard®. The finite element model already presented in previous works uses a sequential temperature displacement coupling. The calculated compression stress relaxation (CSR) and compression set (CS) values do satisfactorily match the experimental results.
In many investigations performed at BAM both values (CSR and CS) were identified as key indicators of elastomer’s long-term performance.
However, the possibility to correlate these equivalent indicators with performance values such as tightness and leakage rate, measurable in the mounted state, is an important goal of our future work. In the presented study the ABAQUS® feature of “pressure penetration” is introduced in the suggested finite element model for this purpose. It provides the possibility to simulate the penetration of a gas into a possible gap between flange and O-ring causing an opening of a leakage path. Three dimensional and axis-symmetric finite element models were generated to represent flat and grooved flanges of different dimensions.
The sensitivity of the feature to several input parameters is investigated and the observed behavior of the O-ring is correlated with the results of performed leakage tests.
The excellent mechanical properties of elastomer seals at a wide range of temperatures as well as their high versatility and recovery potential under several load conditions make these materials well suitable for the application in containers designed for transport and disposal of negligible heat generating radioactive waste. While a seal exchange at defined intervals is typical in many conventional applications, it is impossible or at least hard to perform when principles of minimization of radiation exposure have to be considered which prohibit an avoidable cask handling. An extensive knowledge of the change of the elastomer properties during aging and the availability of reliable end-of-lifetime criteria to guarantee the safe enclosure of the radioactive material for the required time are mandatory. As BAM is involved in most of the national cask licensing procedures and in the evaluation of cask-related long-term safety issues, great efforts have already been made and are still ongoing to scientifically support this task.
Among other representative types of elastomers, specimen made from ethylene propylene diene rubber (EPDM) were tested before, during and after aging to capture the with respect to application most important of their complex mechanical properties.
Exemplary results of these investigations were used to calibrate material models implemented in the commercial finite element software ABAQUS/Standard®. The finite element model already presented in previous works uses a sequential temperature displacement coupling. The calculated compression stress relaxation (CSR) and compression set (CS) values do satisfactorily match the experimental results.
In many investigations performed at BAM both values (CSR and CS) were identified as key indicators of elastomer’s long-term performance.
However, the possibility to correlate these equivalent indicators with performance values such as tightness and leakage rate, measurable in the mounted state, is an important goal of our future work. In the presented study the ABAQUS® feature of “pressure penetration” is introduced in the suggested finite element model for this purpose. It provides the possibility to simulate the penetration of a gas into a possible gap between flange and O-ring causing an opening of a leakage path. Three dimensional and axis-symmetric finite element models were generated to represent flat and grooved flanges of different dimensions.
The sensitivity of the feature to several input parameters is investigated and the observed behavior of the O-ring is correlated with the results of performed leakage tests.
Aging of elastomer O-rings and PE neutron shielding materials for radioactive waste containers
(2021)
Our institution BAM in Berlin, Germany is concerned with research and testing of materials in the context of safety in chemistry and technology. Our working group is involved in the licensing procedures of casks for radioactive waste. Besides, we’re doing research on aging and lifetime prediction of elastomer O-rings and investigate degradation and thermal expansion of PE neutron shielding materials.
The BAM research project BRUZL (Fracture mechanical analysis of spent fuel claddings during long-term dry interim storage) evaluates results of quasi-static Ring Compression Tests (RCT). Due to its simple realisation, the RCT is an established method for characterising the mechanical behaviour of fuel cladding, where a small tube sample is subjected to a compressive load and the relation between load and displacement is obtained. During tests at room temperature, unirradiated ZIRLO® samples with a distinct extend of radial hydrides have shown high susceptibility to sudden, brittle failure at relatively small loads. Hydride morphology and radial hydride metrics have been an integral part of the characterisation of degradation mechanisms of cladding. A software tool for the analysation of metallographic micrographs was developed. The program allows the automated calculation of hydride lengths, detection of continuous hydride structures, their statistical evaluation and visualisation. Numerical models have been established to reproduce experimental RCT results featuring an elastic-plastic material model, which was derived from inverse finite element analyses of as-received RCT samples. A cohesive zone model (CZM) is introduced to the model to reproduce load drops in the linear regime of the load vs. displacement curve. Using a traction-separation approach for the CZM, the cohesive parameters are fitted to match numerical and experimental results yielding the fracture mechanical material properties. Combining the three key aspects hydride morphology, fracture mechanics and RCT stress-state a failure criterion can be established as a result of the BRUZL project.
The project is funded by the Federal Ministry for Economic Affairs and Energy (BMWi) under contract no. 1501561.
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.
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.
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.
Abgeleitet aus den in Teil 3 der „Systemanalyse Konrad“ [1] definierten Lastannahmen für den „untertägigen Anlagenbereich“ müssen Verpackungen, die der Abfallbehälterklasse I (ABK I) mit dem zusätzlichen Merkmal der störfallfesten (sf) Verpackung oder der ABK II zugeordnet werden, gemäß den „Endlagerungsbedingungen, Endlager Konrad“ [2], nach einem „…Fall aus 5 m Höhe auf eine unnachgiebige Unterlage…“ bestimmten Anforderungen genügen.
Eine nähere Beschreibung der Prüfeinrichtung sowie die Definition detaillierter Anforderungen an das Aufprallfundament erfolgen in der „Produktkontrolle, Endlager Konrad“ [3]: „Die Prüfeinrichtung, bestehend aus einer Hebeeinrichtung und einem Fundament ist so zu gestalten, dass der Fall des Prüfmusters in jeder beliebigen Aufprallorientierung aus 5 m Höhe, gemessen von der Unterkante des Prüfmusters zum Fundament, möglich ist. Das Fundament ist aus Beton der Mindestgüte B 35 herzustellen und muss so beschaffen und verankert sein, dass keine Zerstörung in zahlreiche kleinere Bruchstücke erfolgt und keine horizontale Verschiebung des Fundamentes oder seiner Teile auftritt. Maße und Masse des Fundaments müssen so beschaffen sein, dass der Einfluss des Baugrundes unter dem Fundament auf den Aufprallwiderstand vernachlässigbar ist.“
Im Rahmen der Bauartprüfung für Behälter zur Endlagerung radioaktiver Abfälle mit zu vernachlässigender Wärmeentwicklung im Endlager Konrad wird die Bundesanstalt für Materialforschung und -prüfung (BAM) von der Bundesgesellschaft für Endlagerung (BGE) als Sachverständige hinzugezogen und ist in der Regel auch mit der Durchführung der notwendigen Fallprüfungen auf dem Testgelände Technische Sicherheit der BAM (BAM TTS) einschließlich der Bereitstellung der benötigten Prüfeinrichtungen sowie des regelkonformen Aufprallfundamentes beauftragt. Der Prozess, beginnend von der Gewährleistung einer von allen Beteiligten als gültig bewerteten Fallprüfung bis hin zur abschließenden Bewertung und Interpretation der Versuchsergebnisse erfordert dabei u.a. eine sorgfältige Planung und Fertigung der für das Endlager Konrad repräsentativen Fundamentplatte und deren Ankopplung an einen Untergrund im Sinne der „Regulations for the Safe Transport of Radioactive Material“ [4], [5] wie er zum Beispiel auf den beiden Fallversuchsanlagen des BAM Testgelände Technische Sicherheit (BAM TTS) zur Verfügung steht.
Um diese Anforderungen zu erfüllen muss zum einen der Erhalt der Integrität der Fundamentplatte beim Fallversuch durch eine geeignete Auswahl und kraftflussgerechte Anordnung der Stabstahl-Bewehrung sowie deren Verankerung garantiert und damit eine unzulässige Energieaufnahme durch Risse sowie eine unzulässige „… Zerstörung (der Fundamentplatte) in zahlreiche kleinere Bruchstücke …“, wie in [3] gefordert, verhindert werden. Außerdem ist zu gewährleisten, dass der Beton die Anforderungen an die vorgeschriebene Mindestgüte bzw. -festigkeit zum Zeitpunkt der Fallprüfung erfüllt, die Betonfestigkeit jedoch zur Vermeidung unnötig verschärfter Prüfrandbedingungen eine zu definierende Obergrenze nicht überschreitet.
Ausgehend von dem 2009 im Rahmen der KONTEC veröffentlichten Wissensstand [6] präsentiert die BAM im vorliegenden Beitrag die wesentlichen Ergebnisse der zwischenzeitlich bei der Planung und Durchführung von zahlreichen Fallprüfungen gewonnenen Erfahrungen bzgl. Spezifikation und Fertigung der für die Fallversuche notwendigen Fundamentplatten sowie deren Anbindung an den Untergrund. Neben den immer wieder notwendigen Anstrengungen zur Gewährleistung einer im Rahmen der Definition korrekten Betondruckfestigkeit am Tag der Fallprüfung wird die Anpassung der Bewehrungsführung an verschiedene Fallpositionen diskutiert.
Zur Ergänzung des gültigen Regelwerks entsteht parallel zu diesem Dokument eine Fachnotiz, in der BGE und BAM die Vorgaben und Spezifikationen zur regelwerkskonformen Herstellung und Montage von Fundamentplatten für Fallprüfungen im Rahmen der Behälterbauartprüfungsverfahren für das Endlager Konrad zusammenfassen und veröffentlichen werden. Diese Fachnotiz soll detaillierte Vorgaben und Spezifikationen zur Planung, Beauftragung, Herstellung und abschließenden Prüfung eines solchen Fundamentes und dessen Anbindung an den Untergrund enthalten. Damit soll allen beteiligten Organisationen wie Antragstellern, Sachverständigen und BGE ein langfristig verlässlicher Leitfaden im Hinblick auf die Durchführung anforderungsgerechter Fallprüfungen unter definierten und reproduzierbaren Randbedingungen im Rahmen der Bauartprüfungsverfahren für das Endlager Konrad an die Hand gegeben werden.
Abgeleitet aus den in Teil 3 der „Systemanalyse Konrad“ definierten Lastannahmen für den „untertägigen Anlagenbereich“ müssen Verpackungen, die der Abfallbehälterklasse I (ABK I) mit dem zusätzlichen Merkmal der störfallfesten (sf) Verpackung oder der ABK II zugeordnet werden, gemäß den „Endlagerungsbedingungen, Endlager Konrad“, nach einem „…Fall aus 5 m Höhe auf eine unnachgiebige Unterlage…“ bestimmten Anforderungen genügen.
Eine nähere Beschreibung der Prüfeinrichtung sowie die Definition detaillierter Anforderungen an das Aufprallfundament erfolgen in der „Produktkontrolle, Endlager Konrad“: „Die Prüfeinrichtung, bestehend aus einer Hebeeinrichtung und einem Fundament ist so zu gestalten, dass der Fall des Prüfmusters in jeder beliebigen Aufprallorientierung aus 5 m Höhe, gemessen von der Unterkante des Prüfmusters zum Fundament, möglich ist. Das Fundament ist aus Beton der Mindestgüte B 35 herzustellen und muss so beschaffen und verankert sein, dass keine Zerstörung in zahlreiche kleinere Bruchstücke erfolgt und keine horizontale Verschiebung des Fundamentes oder seiner Teile auftritt. Maße und Masse des Fundaments müssen so beschaffen sein, dass der Einfluss des Baugrundes unter dem Fundament auf den Aufprallwiderstand vernachlässigbar ist.“
Im Rahmen der Bauartprüfung für Behälter zur Endlagerung radioaktiver Abfälle mit zu vernachlässigender Wärmeentwicklung im Endlager Konrad wird die Bundesanstalt für Materialforschung und -prüfung (BAM) von der Bundesgesellschaft für Endlagerung (BGE) als Sachverständige hinzugezogen und ist in der Regel auch mit der Durchführung der notwendigen Fallprüfungen auf dem Testgelände Technische Sicherheit der BAM (BAM TTS) einschließlich der Bereitstellung der benötigten Prüfeinrichtungen sowie des regelkonformen Aufprallfundamentes beauftragt. Der Prozess, beginnend von der Gewährleistung einer von allen Beteiligten als gültig bewerteten Fallprüfung bis hin zur abschließenden Bewertung und Interpretation der Versuchsergebnisse erfordert dabei u.a. eine sorgfältige Planung und Fertigung der für das Endlager Konrad repräsentativen Fundamentplatte und deren Ankopplung an einen Untergrund im Sinne der „Regulations for the Safe Transport of Radioactive Material“ wie er zum Beispiel auf den beiden Fallversuchsanlagen des BAM Testgelände Technische Sicherheit (BAM TTS) zur Verfügung steht.
Um diese Anforderungen zu erfüllen muss zum einen der Erhalt der Integrität der Fundamentplatte beim Fallversuch durch eine geeignete Auswahl und kraftflussgerechte Anordnung der Stabstahl-Bewehrung sowie deren Verankerung garantiert und damit eine unzulässige Energieaufnahme durch Risse sowie eine unzulässige „… Zerstörung (der Fundamentplatte) in zahlreiche kleinere Bruchstücke …“, wie in [3] gefordert, verhindert werden. Außerdem ist zu gewährleisten, dass der Beton die Anforderungen an die vorgeschriebene Mindestgüte bzw. -festigkeit zum Zeitpunkt der Fallprüfung erfüllt, die Betonfestigkeit jedoch zur Vermeidung unnötig verschärfter Prüfrandbedingungen eine zu definierende Obergrenze nicht überschreitet.
Ausgehend von dem 2009 im Rahmen der KONTEC veröffentlichten Wissensstand präsentiert die BAM im vorliegenden Beitrag die wesentlichen Ergebnisse der zwischenzeitlich bei der Planung und Durchführung von zahlreichen Fallprüfungen gewonnenen Erfahrungen bzgl. Spezifikation und Fertigung der für die Fallversuche notwendigen Fundamentplatten sowie deren Anbindung an den Untergrund. Neben den immer wieder notwendigen Anstrengungen zur Gewährleistung einer im Rahmen der Definition korrekten Betondruckfestigkeit am Tag der Fallprüfung wird die Anpassung der Bewehrungsführung an verschiedene Fallpositionen diskutiert.
Zur Ergänzung des gültigen Regelwerks entsteht parallel zu diesem Dokument eine Fachnotiz, in der BGE und BAM die Vorgaben und Spezifikationen zur regelwerkskonformen Herstellung und Montage von Fundamentplatten für Fallprüfungen im Rahmen der Behälterbauartprüfungsverfahren für das Endlager Konrad zusammenfassen und veröffentlichen werden. Diese Fachnotiz soll detaillierte Vorgaben und Spezifikationen zur Planung, Beauftragung, Herstellung und abschließenden Prüfung eines solchen Fundamentes und dessen Anbindung an den Untergrund enthalten. Damit soll allen beteiligten Organisationen wie Antragstellern, Sachverständigen und BGE ein langfristig verlässlicher Leitfaden im Hinblick auf die Durchführung anforderungsgerechter Fallprüfungen unter definierten und reproduzierbaren Randbedingungen im Rahmen der Bauartprüfungsverfahren für das Endlager Konrad an die Hand gegeben werden.