A Modelling and Experimental Study for Long-Term Prediction of Localised Corrosion in Carbon Steel Overpacks for High-Level Radioactive Waste.

1994 ◽  
Vol 353 ◽  
Author(s):  
A. Hoch ◽  
A. Honda ◽  
H. Ishikawa ◽  
F. Porter ◽  
S. Sharland ◽  
...  

AbstractThis paper describes a joint modelling and experimental study for investigation of pit growth in carbon steel High-Level Radioactive Waste overpacks under consideration in Japan. A mathematical model of the growth of corrosion pits in metals has been developed. This model is implemented in the computer program CAMLE, and includes representation of the chemical, electrochemical and migration processes that control pit-growth rates. Experiments to provide key input data for the model are described, in addition to experiments to measure ‘short-term’ pit growth. Predictions from the model are compared with these data. Overall, the comparisons are encouraging and the model shows good potential as a tool for assessment of the long-term corrosion behaviour of overpacks under repository conditions. Future developments of the model to improve agreement are discussed.

2003 ◽  
pp. 203-208
Author(s):  
Hideo KOMINE ◽  
Nobuhide OGATA ◽  
Akira NAKASHIMA ◽  
Hajime TAKAO ◽  
Hiroyoshi UEDA ◽  
...  

2021 ◽  
Author(s):  
Marc Wengler ◽  
Astrid Göbel ◽  
Eva-Maria Hoyer ◽  
Axel Liebscher ◽  
Sönke Reiche ◽  
...  

<p>According to the 'Act on the Organizational Restructuring in the Field of Radioactive Waste Disposal' the BGE was established in 2016. The amended 'Repository Site Selection Act' (StandAG) came into force in July 2017 and forms the base for the site selection by clearly defining the procedure. According to the StandAG the BGE implements the participative, science-based, transparent, self-questioning and learning procedure with the overarching aim to identify the site for a high-level radioactive waste (HLW) repository in a deep geological formation with best possible safety conditions for a period of one million years.</p><p>The German site selection procedure consists of three phases, of which Phase 1 is divided into two steps. Starting with a blanc map of Germany, the BGE completed Step 1 in September 2020 and identified 90 individual sub-areas that provide favorable geological conditions for the safe disposal of HLW in the legally considered host rocks; rock salt, clay and crystalline rock. Based on the results of Step 1, the on-going Step 2 will narrow down these sub-areas to siting regions for surface exploration within Phase 2 (§ 14 StandAG). Central to the siting process are representative (Phase 1), evolved (Phase 2) and comprehensive (Phase 3) preliminary safety assessments according to § 27 StandAG.</p><p>The ordinances on 'Safety Requirements' and 'Preliminary Safety Assessments' for the disposal of high-level radioactive waste from October 2020 regulate the implementation of the preliminary safety assessments within the different phases of the siting process. Section 2 of the 'Safety Requirements' ordinance provides requirements to evaluate the long-term safety of the repository system; amongst others, it states that all potential effects that may affect the long-term safety of the repository system need to be systematically identified, described and evaluated as “expected” or “divergent” evolutions. Additionally, the ordinance on 'Preliminary Safety Assessments' states in § 7, amongst others, that the geoscientific long-term prediction is a tool to identify and to evaluate geogenic processes and to infer “expected” and “divergent” evolutions from those. Hence, considering the time period of one million years for the safe disposal of the HLW and the legal requirements, it is essential to include long-term climate evolution in the German site selection process to evaluate the impact of various climate-related scenarios on the safety of the whole repository system.</p><p>To better understand and evaluate the influence of climate-related processes on the long-term safety of a HLW repository, climate-related research will be a part of the BGE research agenda. Potential research needs may address i) processes occurring on glacial – interglacial timescales (e.g. the inception of the next glaciation, formation and depth of permafrost, glacial troughs, sub-glacial channels, sea-level rise, orbital forcing) and their future evolutions, ii) effects on the host rocks and the barrier system(s) as well as iii) the uncertainties related to these effects but also to general climate models and predictions.</p>


Author(s):  
Bruno Kursten ◽  
Frank Druyts ◽  
Pierre Van Iseghem

Abstract The current worldwide trend for the final disposal of conditioned high-level, medium-level and long-lived alpha-bearing radioactive waste focuses on deep geological disposal. During the geological disposal, the isolation between the radioactive waste and the environment (biosphere) is realised by the multibarrier principle, which is based on the complementary nature of the various natural and engineered barriers. One of the main engineered barriers is the metallic container (overpack) that encloses the conditioned waste. In Belgium, the Boom Clay sediment is being studied as a potential host rock formation for the final disposal of conditioned high-level radioactive waste (HLW) and spent fuel. Since the mid 1980’s, SCK•CEN has developed an extensive research programme aimed at evaluating the suitability of a wide variety of metallic materials as candidate overpack material for the disposal of HLW. A multiple experimental approach is applied consisting of i) in situ corrosion experiments, ii) electrochemical experiments (cyclic potentiodynamic polarisation measurements and monitoring the evolution of ECORR as a function of time), and iii) immersion experiments. The in situ corrosion experiments were performed in the underground research facility, the High Activity Disposal Experimental Site, or HADES, located in the Boom clay layer at a depth of 225 metres below ground level. These experiments aimed at predicting the long-term corrosion behaviour of various candidate container materials. It was believed that this could be realised by investigating the medium-term interactions between the container materials and the host formation. These experiments resulted in a change of reasoning at the national authorities concerning the choice of over-pack material from the corrosion-allowance material carbon steel towards corrosion-resistant materials such as stainless steels. The main arguments being the severe pitting corrosion during the aerobic period and the large amount of hydrogen gas generated during the subsequent anaerobic period. The in situ corrosion experiments however, did not allow to unequivocally quantify the corrosion of the various investigated candidate overpack materials. The main shortcoming was that they did not allow to experimentally separate the aerobic and anaerobic phase. This resulted in the elaboration of a new laboratory programme. Electrochemical corrosion experiments were designed to investigate the effect of a wide variety of parameters on the localised corrosion behaviour of candidate overpack materials: temperature, SO42−, Cl−, S2O32−, oxygen content (aerobic - anaerobic),… Three characteristic potentials can be derived from the cyclic potentiodynamic polarisation (CPP) curves: i) the open circuit potential, OCP, ii) the critical potential for pit nucleation, ENP, and iii) the protection potential, EPP. Monitoring the open circuit potential as a function of time in clay slurries, representative for the underground environment, provides us with a more reliable value for the corrosion potential, ECORR, under disposal conditions. The long-term corrosion behaviour of the candidate overpack materials can be established by comparing the value of ECORR relative to ENP and EPP (determined from the CPP-curves). The immersion tests were developed to complement the in situ experiments. These experiments aimed at determining the corrosion rate and to identify the corrosion processes that can occur during the aerobic and anaerobic period of the geological disposal. Also, some experiments were elaborated to study the effect of graphite on the corrosion behaviour of the candidate overpack materials.


2021 ◽  
Vol 1 ◽  
pp. 155-156
Author(s):  
Stephan Hilpmann ◽  
Robin Steudtner ◽  
Björn Drobot ◽  
René Hübner ◽  
Frank Bok ◽  
...  

Abstract. Clay formations are potential host rocks for the long-term storage of high-level radioactive waste in a deep geological repository. Bentonites are supposed to serve as backfill material, not only for a final disposal site in clay formations but also in crystalline rock. For a long-term safety assessment, various aspects must be taken into account. Besides geological, geochemical and geophysical considerations, naturally occurring microorganisms also play a crucial part in the environment of such a repository. In the event of a worst-case scenario when water enters the disposal site, they can interact with the radionuclides and change for example the chemical speciation or the oxidation state (Lloyd et al., 2002). Desulfosporosinus spp. are an important representative of anaerobic, sulfate-reducing microorganisms, which are present in clay formations as well as in bentonites. Various studies have shown that they play a major role in the microbial communities of these surroundings (Bagnoud et al., 2016; Matschiavelli et al., 2019). A closely related microorganism to the isolated species is Desulfosporosinus hippei DSM 8344, which was originally found in permafrost soil (Vatsurina et al., 2008). This bacterium was used to investigate its interactions with uranium(VI) especially regarding the reduction to the less mobile uranium(IV). Time-dependent reduction experiments in artificial Opalinus Clay pore water (Wersin et al., 2011) (100 µM uranium(VI), pH 5.5) showed the removal of about 80 % of the uranium(VI) from the supernatants within 48 h. Corresponding UV/Vis measurements of the dissolved cell pellets exhibited an increasing proportion of uranium(IV) in the cell-bound uranium. Calculations with the inclusion of extinction coefficients led to a ratio of 39 % uranium(IV) after 1 week. Therefore, a combined sorption-reduction process is a possible interaction mechanism. Time-resolved laser-induced luminescence spectroscopy verified the presence of two uranium(VI) species in the supernatant. A comparison with reference spectra led to an assignment to a uranyl(VI) lactate and a uranyl(VI) carbonate complex. The species distribution showed a decrease of the proportion of the lactate species with time, whereas the proportion of the carbonate species remained almost constant. Uranium aggregates are formed on the cell surface during the process, as determined by transmission electron microscopy (TEM). Furthermore, uranium occurs inside and outside the cells as well as vesicles containing uranium. These findings help to close existing gaps in a comprehensive safeguard concept for a repository for high-level radioactive waste in clay rock. Moreover, this study provides new insights into the interactions of sulfate-reducing microorganisms with uranium(VI).


PLoS ONE ◽  
2022 ◽  
Vol 17 (1) ◽  
pp. e0262275
Author(s):  
Stephan Hilpmann ◽  
Miriam Bader ◽  
Robin Steudtner ◽  
Katharina Müller ◽  
Thorsten Stumpf ◽  
...  

The safe disposal of high-level radioactive waste in a deep geological repository is a huge social and technical challenge. So far, one of the less considered factors needed for a long-term risk assessment, is the impact of microorganisms occurring in the different host rocks. Even under the harsh conditions of salt formations different bacterial and archaeal species were found, e. g. Halobacterium sp. GP5 1–1, which has been isolated from a German rock salt sample. The interactions of this archaeon with uranium(VI), one of the radionuclides of major concern for the long-term storage of high-level radioactive waste, were investigated. Different spectroscopic techniques, as well as microscopy, were used to examine the occurring mechanisms on a molecular level leading to a more profound process understanding. Batch experiments with different uranium(VI) concentrations showed that the interaction is not only a simple, but a more complex combination of different processes. With the help of in situ attenuated total reflection Fourier-transform infrared spectroscopy the association of uranium(VI) onto carboxylate groups was verified. In addition, time-resolved laser-induced luminescence spectroscopy revealed the formation of phosphate and carboxylate species within the cell pellets as a function of the uranium(VI) concentration and incubation time. The association behavior differs from another very closely related halophilic archaeon, especially with regard to uranium(VI) concentrations. This clearly demonstrates the importance of studying the interactions of different, at first sight very similar, microorganisms with uranium(VI). This work provides new insights into the microbe-uranium(VI) interactions at highly saline conditions relevant to the long-term storage of radioactive waste in rock salt.


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