Article

Radiation resistance of elastomeric O-rings in mixed neutron and gamma fields: Testing methodology and experimental results

AIP Publishing
Review of Scientific Instruments
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Abstract

Materials and components employed in the presence of intense neutron and gamma fields are expected to absorb high dose levels that may induce deep modifications of their physical and mechanical properties, possibly causing loss of their function. A protocol for irradiating elastomeric materials in reactor mixed neutron and gamma fields and for testing the evolution of their main mechanical and physical properties with absorbed dose has been developed. Four elastomeric compounds used for vacuum O-rings, one fluoroelastomer polymer (FPM) based and three ethylene propylene diene monomer rubber (EPDM) based, presently available on the market have been selected for the test. One EPDM is rated as radiation resistant in gamma fields, while the other elastomers are general purpose products. Particular care has been devoted to dosimetry calculations, since absorbed dose in neutron fields, unlike pure gamma fields, is strongly dependent on the material composition and, in particular, on the hydrogen content. The products have been tested up to about 2 MGy absorbed dose. The FPM based elastomer, in spite of its lower dose absorption in fast neutron fields, features the largest variations of properties, with a dramatic increase in stiffness and brittleness. Out of the three EPDM based compounds, one shows large and rapid changes in the main mechanical properties, whereas the other two feature more stable behaviors. The performance of the EPDM rated as radiation resistant in pure gamma fields does not appear significantly better than that of the standard product. The predictive capability of the accelerated irradiation tests performed as well as the applicable concepts of threshold of radiation damage is discussed in view of the use of the examined products in the selective production of exotic species facility, now under construction at the Legnaro National Laboratories of the Italian Istituto Nazionale di Fisica Nucleare. It results that a careful account of dose rate effects and oxygen penetration in the material, both during test irradiations and in operating conditions, is needed to obtain reliable predictions.

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... Elastomeric O-rings are widely used at CERN in a variety of applications, including but not limited to high radiation areas. EPDM-based elastomers are generally known to be more radiation resistant than other elastomeric materials [5], however large differences in the radiation tolerance of different commercial EPDM-based materials were observed [17]. Accordingly, it is not possible to assume that all EPDM-based materials exhibit the same resistance to radiation, and specific commercial products should be irradiated and tested. ...
... Both James Walker and Angst+Pfister EPDMs tested in this study largely exceed these end-points at the minimum investigated gamma dose of 2 MGy, suggesting that the most important degradation phenomena occur at lower doses. Figure 8 shows a comparison between three commercial EPDM O-rings including James Walker Shield-seal663®(referred to as EPDM 3 in the Graph), irradiated in the frame of a previous study performed in neutron and gamma mixed field radiation [17]. In this study, the neutron component of the dose corresponded to about 65% of the total, the rest being deposited by gamma radiation, at a very high total dose rate of approximately 0.7 MGy/h. ...
... In the graph, EPDM 3 corresponds to James Walker Shieldseal663®. Data extracted and elaborated from[17],[18]. ...
Article
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Irradiation tests are continuously needed at the European Organization for Nuclear Research (CERN), to experimentally assess the radiation tolerance of commercial non-metallic materials for use in high-radiation areas. The ’Radiation to Materials’ R2M activity organizes such tests and provides expertise in the interpretation of results, for the design and upgrade of devices absorbing critical doses during their lifetime. The various activities covered by the R2M are presented. Up to ten irradiation tests per year are organized in external 60 Co facilities, in which samples absorb up to several MGy of gamma dose at dose rates in the kGy/h range. Cables, O-rings, lubricants, glues, optical materials, and insulators are examples of possible tested materials. In parallel, selected samples are irradiated in a mixed neutron and gamma irradiation station built close to the Neutron Time-Of-Flight facility. Dedicated research studies, mainly focused on oil, greases and elastomeric O-rings, are being performed to deepen the understanding of radiation effects in these critical materials. As an example, the mechanical and structural characterization of two elastomeric EPDM-based commercial materials irradiated in gamma radiation up to 3 MGy of dose is presented.
... Four commercially available elastomeric materials were selected for irradiation and testing. Three of them are ethylene-propylene-diene monomer (EPDM)-based O-rings, while one of them is a fluoropolymer (FPM)-based one [4]. Nine lubricating greases with different chemical compositions and one lubricating oil were selected [5,6]. ...
... For this reason, the light element composition of each product was measured using CHN (carbon, hydrogen, nitrogen) analysis. The measured composition was used in the simulations to calculate the neutron and gamma dose rate for each material [4,5]. ...
... Doses were delivered with very high dose rates corresponding to about 700 kGy/h and 340 kGy/h for EPDMs and FPM, respectively. Differences are due to the different hydrogen amount, about 8% for EPDMs and about 1% for FPM in mass [4]. All the irradiation were performed in air at atmospheric pressure in containers allowing a partial recirculation of air. ...
Article
Full-text available
Lubricants and O-rings are necessarily used for the construction of many accelerator-driven facilities as spallation sources or facilities for the production of radioactive isotopes. During operation, such component will absorb high doses of mixed neutron and gamma radiation, that can degrade their mechanical and structural properties. Experimental radiation damage tests of these components are mandatory for the construction of the facility. Methodologies for irradiation in nuclear reactor mixed fields and post-irradiation examination of lubricating oils, greases and O-rings were developed and are here presented. Samples were characterized with standard mechanical and physical-chemical tests. Parametric studies on the dose rate effects have been performed on O-rings. A case studies for a specific O-ring application in a gate valve has been developed. Some of the tested samples showed a dramatic change of their properties with dose, while others remain stable. Results were collected on nine commercial greases, on one oil and on four commercial elastomeric O-rings. The most radiation resistant among the selected products are now considered for application in facilities under construction. The main mechanisms of neutron and gamma radiation damage on these polymers were investigated at the mechanical and structural level.
... In order to gather information on the resistance of polymeric Orings in such extreme conditions, in a previous work, two rubbers, namely ethylene propylene diene monomer (EPDM) rubber and a fluoroelastomer (FPM), were irradiated in reactor mixed neutron and gamma fields to investigate the effect of the adsorbed dose on their tensile properties and compression set values [11]. EPDM O-rings were then studied to assess their sealing performance both during the facility service time and the postservice storage phase [12]. ...
... Finally, elemental analyses were carried out to determine the content of the various elements, which was necessary to perform dosimetry calculations [11].The measured elemental composition of EPDM and FPM is reported in Table 1. ...
... Table 2 reports the dose rates of EPDM and FPM in the CT facility for the reactor operating at the nominal power (250 kW). Dose components and dose rates were calculated taking into account the elemental composition of materials and the irradiation conditions, as previously described in Ref. 11. Using the same methodology, dose rates for the two materials were calculated in the LS facility. ...
Article
Elastomers are widely used in radioactive environments, where ionizing radiations induce a deterioration of their properties due to degradative phenomena occurring in the polymer structure. Their radiation resistance is usually assessed using γ‐rays and relatively low dose rates, but in actual applications, they are often exposed to mixed radiation fields and higher dose rates. Ethylene propylene diene monomer (EPDM) is known for its excellent resistance to γ‐rays but absorbs a larger dose by neutron interactions than fluoroelastomer (FPM). In this work, EPDM and FPM were irradiated in mixed neutron and gamma fields, using high dose rates (from 22 to 700 kGy h−1) and total absorbed doses between 0.2 and 3.5 MGy. The effects of irradiation were assessed by swelling tests, differential scanning calorimetry analysis and dynamic mechanical thermal analysis, and tensile tests. The results show that, even if irradiations were carried out in air, degradation took place under nonoxidative conditions owing to the high dose rates employed. Under such conditions, crosslinking is the dominant radiation‐induced reaction in both elastomers. Moreover, material degradation seems to be influenced mostly by the total absorbed dose and not by the type of radiation. Contrary to what observed at the lower dose rates employed with γ‐rays, major dose rate effects are not observed. POLYM. ENG. SCI., 2019.
... The remaining 15% is represented by gamma dose, mainly due to fission prompt gammas. More details about dosimetry can be found in [5]. The TIS life cycle includes a 15-day long post-service cooling time before removal from the facility to reduce the residual activity. ...
... Neutron damage studies on polymeric materials are presently very scarce in the literature. We developed protocols for irradiation and testing of elastomeric Orings [5] and lubricating greases [7]. They aim at the selection of radiation-resistant products to be used for the SPES construction. ...
... Two main components of the neutron energy spectrum are present: a fast component and a thermal component which originates from the moderation of fast neutrons due to the materials present in the reactor core. More details can be found in [5]. Fast neutrons are particularly effective in delivering dose to polymeric materials. ...
... This allows outer containers to be reused after decontamination, following a cooldown phase. (iii) Radiation tolerance: elastomeric seals should generally be avoided, as even the most radiation tolerant ones are expected to degrade at doses in the MGy range [19,45] (see Sec. V). A full-metal container body and graphite seals are, therefore, used to ensure leak tightness. ...
Article
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A new parasitic, mixed-field, neutron-dominated irradiation station has been recently commissioned at the European Laboratory for Particle Physics (CERN). The station is installed within the neutron time-of-flight (n_TOF) facility, taking advantage of the secondary radiation produced by the neutron spallation target, with neutrons ranging from 0.025 eV to several hundreds of MeV. The new station allows radiation damage studies to be performed in irradiation conditions that are closer to the ones encountered during the operation of particle accelerators; the irradiation tests carried out in the station will be complementary to the standard tests on materials, usually performed with gamma sources. Samples will be exposed to neutron-dominated doses in the MGy range per year, with minimal impact on the n_TOF facility operation. The station has 24 irradiation positions, each hosting up to 100 cm3 of sample material. In view of its proximity to the n_TOF target, inside protective shielding, the irradiation station and its operating procedures have been carefully developed taking into account the safety of personnel and to avoid any unwanted impact on the operation of the n_TOF facility and experiments. Due to the residual radioactivity of the whole area around the n_TOF target and of the irradiated samples, access to the irradiation station is forbidden to human operators even when the n_TOF facility is not in operation. Robots are used for the remote installation and retrieval of the samples, and other optimizations of the handling procedures were developed in compliance with radiation protection regulations and the aim of minimizing doses to personnel. The sample containers were designed to be radiation tolerant, compatible with remote handling, and subject to detailed risk analysis and testing during their development. The whole life cycle of the irradiated materials, including their post-irradiation examinations and final disposal, was considered and optimized.
... • Radiation tolerance; elastomeric seals should generally be avoided, as even the most radiation tolerant ones are expected to degrade at doses in the MGy range [20,42] (see Section 5). A full-metal container body and graphite seals are therefore used to ensure leak-tightness. ...
Preprint
Full-text available
A new parasitic, mixed-field, neutron-dominated irradiation station has been recently commissioned at the European Laboratory for Particle Physics (CERN). The station is installed in the Neutron Time-Of-Flight (n\_TOF) facility, taking advantage of the secondary radiation produced by the neutron spallation target. The new station allows radiation damage studies to be performed in irradiation conditions that are closer to the ones encountered during the operation of particle accelerators; the irradiation tests carried out in the station will be complementary to the standard tests on materials, usually performed with gamma sources. Samples will be exposed to neutron doses in the MGy range per year, with minimal impact on the n TOF facility operation. The station has twenty-four irradiation positions, each hosting up to 100 cm3 of sample material. In view of its proximity to the n\_TOF target, inside protective shielding, the irradiation station and its operating procedures have been carefully developed taking into account the safety of personnel and to avoid any unwanted impact on the operation of the n\_TOF facility and experiments. Due to the residual radioactivity of the whole area around the n\_TOF target and of the irradiated samples, access to the irradiation station is forbidden to human operators even when the n\_TOF facility is not in operation. Robots are used for the remote installation and retrieval of the samples, and other optimizations of the handling procedures were developed in compliance with radiation protection regulations and the aim of minimizing doses to personnel.
... This is a special grade EPDM-based material designed to be radiation tolerant and declared by the producer as resistant up to a gamma dose of 1.6 MGy [45]. Additionally, this material was irradiated in a mixed neutron and gamma radiation field in a previous study [46], reporting moderate damage at 0.7 MGy and only severe damage at 1.5 MGy [47], which are well above the 0.12 MGy expected during Run 3. ...
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Two 6 t beam dumps, made of a graphite core encapsulated in a stainless steel vessel, are used to absorb the energy of the two Large Hadron Collider (LHC) intense proton beams during operation of the accelerator. Operational issues started to appear in 2015 during LHC Run 2 (2014–2018) as a consequence of the progressive increase of the LHC beam kinetic energy, necessitating technical interventions in the highly radioactive areas around the dumps. Nitrogen gas leaks appeared after highly energetic beam impacts and instrumentation measurements indicated an initially unforeseen movement of the dumps. A computer modelling analysis campaign was launched to understand the origin of these issues, including both Monte Carlo simulations to model the proton beam interaction as well as advanced thermo-mechanical analyses. The main findings were that the amount of instantaneous energy deposited in the dump vessel leads to a strong dynamic response of the whole dump and high accelerations (above 200 g). Based on these findings, an upgraded design, including a new support system and beam windows, was implemented to ensure the dumps' compatibility with the more intense beams foreseen during LHC Run 3 (2022–2025) of 539 MJ per beam. In this paper an integral overview of the operational behaviour of the dumps and the upgraded configurations are discussed.
... For these reasons, experimental radiation resistance tests of candidate products for use in high-power environment where neutron radiation dominates are necessary. Irradiation and testing methodologies have been developed in the last years, dedicated to the selection of elastomeric O-rings to be used in the SPES project [4,5]. The objective of this study is to examine nine commercial greases for selection for applying to use in ESS and SPES facilities [6]. ...
... In particular, mixed radiation data are necessary for the design and construction of new facilities producing intense neutron fields. We dedicated a previous study to the development of a methodology for testing elastomeric O-rings irradiated in neutron and gamma mixed fields [21]. A following study was dedicated to the experimental determination of the end-of-life conditions of a specific EPDM O-ring to be installed in a gate valve of the SPES facility. ...
Article
Full-text available
Many of the moving components in accelerator and target environments require lubrication. Lubricants in such environments are exposed to high fluxes of secondary radiation, which originates from beam interactions with the target and from beam losses. The secondary radiation is a mix of components, which can include significant fractions of neutrons. Lubricants are radiation-sensitive polymeric materials. The radiation-induced modifications of their structure reduce their service lifetime and impose additional facility maintenance, which is complicated by the environmental radioactivity. The study of the lubricants radiation resistance is therefore necessary for the construction of new generation accelerators and target systems. Nevertheless, data collected in mixed radiation fields are scarce. Nine commercial greases were irradiated at a TRIGA Mark II Research Reactor to serve for the construction of new accelerator projects like the European Spallation Source (ESS) at Lund (Sweden) and Selective Production of Exotic Species (SPES) at Legnaro, (Italy). Mixed neutron and gamma doses ranging from 0.1 MGy to 9.0 MGy were delivered to the greases. For an experimental quantification of their degradation, consistency was measured. Two of the greases remained stable, while the others became fluid. Post-irradiation examinations evidence the cleavage of the polymeric structure as the dominant radiation effect. Dose and fluence limits for the use of each product are presented. Apart from the scientific significance, the results represent an original and useful reference in selecting radiation resistant greases for accelerator and target applications. Keywords: Materials science, Aerospace engineering, Industrial engineering, Nuclear engineering, Materials chemistry, Mechanical engineering, Nuclear reactor irradiation, Polymer degradation, Neutron damage, Lubricating grease, Radiation effect, Mixed radiation field
... 10,11 A comparative study of fluoro-elastomers and EPDM-based elastomers confirmed that damage due to neutron and g radiation fields were minimal for EPDM elastomers. 12 Abdel-Aziz et al. 13 studied the influence of co-agent and fumed silica on thermal and electrical resistivity in EPDM/modified MMT nanocomposites. They also reported on thermal stability and activation energy for thermal degradation of g-irradiated specimens. ...
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In this work, blends of ethylene propylene diene monomer rubber and chlorobutyl rubber were reinforced with organo-modified layered silicate (nanoclay) to enhance their performance in radiation as well as hydrocarbons environments. The mechanical properties of the nanocomposites increased (up to 57%) and solvent transport coefficients decreased (by 30%) with increasing nanoclay content. The enhancement in properties was attributed to the dispersion of nanoclay platelets in the ethylene propylene diene monomer–chlorobutyl rubber blends and the chemical interaction between nanoclay and the polymer which were confirmed by morphological and spectroscopic analysis, respectively. The effect of nanofiller content on the mechanical properties, solvent uptake and thermal degradation of blends exposed to gamma radiation was investigated by irradiating the nanocomposites with gamma rays for cumulative doses of 0.5, 1 and 2 MGy. The ethylene propylene diene monomer–chlorobutyl rubber nanocomposites with 5 phr nanoclay had the best retention of mechanical properties and solvent sorption coefficients on exposure to radiation. Depending on the dose of cumulative radiation exposure, chain scission and/or crosslinking occurred in the nanocomposites, resulting in varying degrees of changes in properties.
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One of the key priorities in modern mechanical engineering is to ensure the safe, long-lasting operation of systems while maximizing energy efficiency and withstanding extreme and damaging conditions. This is especially relevant in environments subject to radiation, in which materials, depending on their chemical and elemental composition, exhibit specific limitations. In this review, we summarize the current state of the art in research and development regarding the performance of lubricants in radiation fields and the effectiveness of radiation-tolerant lubricated systems. We discuss the current understanding of radiation-damage mechanisms in dry-film lubricants, oils, and greases, and we summarize the experimental results of the irradiation studies performed to date. We compile and compare the established performance of various material types and chemistries in intense ionizing radiation fields. Finally, we provide an overview of future research directions, highlighting the challenges faced in irradiation studies, considerations relating to the selection of materials, new facilities and experiments aimed at advancing the field, and other issues related to the safe application and use of lubricant materials in radiation environments.
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Conference Paper
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Conference Paper
Full-text available
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In the presence of oxygen, polymeric materials may undergo diffusion-limited heterogeneous degradation with significant oxidation occurring only near the surfaces. It is important in studying polymer degradation (and in designing accelerated aging experiments) to be able to determine under what conditions heterogeneous degradation occurs, and to estimate the extent of significant oxidative penetration under those conditions. We describe here the use of several techniques for identification of oxidative degradation gradients. A rapid determination of oxidation depth is accomplished by optical examination of metallographically polished cross-sectioned samples; oxidized and nonoxidized regions are distinguished by differences in surface reflectivity. A more detailed determination of the shapes of degradation gradients is accomplished by performing a series of sensitive determinations of relative hardness changes across the surface of cross-sectioned, polished samples. Typical oxidation depths for the commercial polymers examined are on the order of fractions of millimeters over a dose-rate range of 104–106 rad/h. Significant variations among different materials are found, as would be expected given differences in oxygen consumption and permeation rates. A detailed example is given of the tensile property behavior of a Viton material over a range of dose rates where the degradation is seen to change from strongly heterogeneous at high dose rates to homogeneous as the dose rate is lowered. Degradation differences in this material are very pronounced: at high dose rates the polymer undergoes primarily crosslinking to give a hard brittle material, whereas under lower dose rates, where oxygen permeation is complete, the polymer undergoes predominantly scission to yield a soft, easily stretchable material.
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A rigorous test of theoretical treatments for diffusion-limited oxidation was completed by conducting an extensive series of radiation-initiated oxidation experiments on a commercial EPDM material. Oxidation profiles were monitored from density changes; profiles were obtained versus sample thickness, radiation dose rate and surrounding oxygen partial pressure. The resulting profile shapes and magnitudes could be quantitatively fit with a two-parameter theoretical treatment based on oxidation kinetics containing unimolecular termination reactions. The theoretical parameters derived from fitting allowed quantitative confirmation of a governing theoretical expression relating these parameters to independently measured values for the oxygen consumption and permeation rates.
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