La sûreté des installations de stockage profond des déchets radioactifs repose sur l’évaluation des propriétés de confinement de la barrière géologique et des processus qui y régissent le transport des radionucléides. La thèse est menée dans le cadre de l’expérience Deep Borehole du projet Mont Terri. Elle vise à renforcer l’évaluation de l’importance relative des phénomènes de transfert convectifs et diffusifs au sein de l’Argile à Opalines (OPA) et à apporter des éclaircissements concernant l’impact des phénomènes transitoires chimique et hydraulique sur ces transferts et la génération d’anomalies de pression. Un premier volet expérimental a permis d’acquérir les paramètres de transport advectifs, diffusifs, et les forces motrices associées, nécessaires à l’estimation des flux d’eau et de solutés entre l’OPA et les aquifères adjacents. Les données de température et de pression révèlent un gradient géothermique de 8.5°C/100 m et un excès de charge d’au moins 60 m. L’inversion du profil de chlorure par méthode Bayésienne de type Monte Carlo Markov Chain valide l’évolution paléohydrogéologique du site proposé dans la littérature en considérant un transport diffusif pur à travers la formation. La contribution des phénomènes de transport osmotique a été déterminée en interprétant le profil de pression à l’aide de simulations transitoires considérant l’évolution temporelle de la chlorinité et de la pression au cours du scénario géologique et de simulations en pseudo régime permanent. Ce profil est reproduit en évaluant le flux advectif couplé incluant l’advection de Darcy, la chemo-osmose et la thermo-osmose, avec une contribution majeure de ce dernier processus. / The safety of radioactive waste disposal facilities in deep geological formation depends on the evaluation of the rock confining properties and the processes governing radionuclides transfer. The thesis is conducted in the framework of Deep Borehole experiment of the Mont Terri project. The purpose of this research is to build confidence with regard to understanding relative importance of diffusive and convective phenomena withine the Opalinus Clay (OPA) and to identify the impact of a hydraulic and chemical transient behaviour on the transfers of fluid and solutes, and anomalous pressures generation.A first experimental stage enabled to acquire the advective and diffusive transport parameters, and the associated driving forces, necessary to the evaluation of fluid and solute fluxes between the OPA and its adjacent aquifers. Temperature and pressure measurements revealed a geothermal gradient of 8.5 °C/100 m and an excess of hydraulic head of at least 60 m.The chloride profile inversion by a Bayesian method with a Monte Carlo Markov Chain algorithm validates the paleohydrological evolution proposed in the litterature, considering a pure diffusive transport through the argillaceous formation. The contribution of osmotic transport phenomena was assessed by interpreting the pressure profile, using transient simulations that takes into account the temporal evolution of chlorinity and pressure during the geological scenario, and pseudo steady-state simulations. This profile is reproduced by evaluating the coupled advective flux, including pure advection, chemo-osmosis and thermo-osmosis, with a major contribution of the latter process.

京都大学 / 0048 / 新制・課程博士 / 博士(工学) / 甲第22051号 / 工博第4632号 / 新制||工||1722(附属図書館) / 京都大学大学院工学研究科都市社会工学専攻 / (主査)教授 岸田 潔, 教授 木村 亮, 教授 小池 克明 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DFAM

Les Argiles de Boom ont été identifiées par le SCK-CEN comme un éventuel site de stockage de déchets nucléaires en couche géologique profonde : elles font l’objet d’études dans le laboratoire souterrain de Mol (Belgique). Dans ce contexte, il est important d’évaluer les conséquences du creusement de galeries sur les propriétés de ces Argiles. Ce travail de thèse cible plus particulièrement les effets d’oxydation à l’air et de biodégradation anaérobie sur la MO fossile. Les expériences d’oxydation ont combiné des suivis expérimentaux (série artificielle) et des études sur des échantillons altérés in situ (série naturelle) dans les galeries du laboratoire. Elles ont ciblé le kérogène, la MOE et MOD. La confrontation des données des deux séries révèle que nos simulations expérimentales sont représentatives des processus ayant lieu dans les galeries. Ces travaux démontrent aussi que l’oxydation induit (i) une augmentation importante de la quantité de MOD et (ii) une modification majeure de la chimie de la MOE et de la MOD caractérisée par la formation de molécules oxygénées de faible poids moléculaire. Par ailleurs, l’étude comparative des eaux issues des échantillons altérés avec celles prélevées dans les piézomètres du site démontre que ces dernières ne sont pas affectées par des processus d’oxydation et sont comparables aux eaux issues des échantillons sains. Des expériences de biodégradation menées sur des argiles saines et préalablement oxydées artificiellement n’ont montré aucune évolution significative de la MO fossile (MOE et MOD); la biodégradation anaérobie n’est donc pas un processus dominant dans le contexte des perturbations induites par les excavations / The Boom Clay was focused because it is identified by SCK-CEN as a possible radioactive waste storage in the geological disposal site and in situ experiments are performed in the underground laboratory of Mol (Belgium). In this context, it is important to assess the consequences of galleries excavation on the properties of the Boom Clay. The particular focus of this study is the effects of air oxidation and anaerobic biodegradation on the OM. The experiments dealing with the effects of air oxidation have combined studies of artificial oxidized samples (artificial series) and samples altered in the gallery of the underground laboratory (natural series). These experiments focus on the Kerogen, the EOM and the DOM. The comparison of data from artificial and natural series shows firstly that our experimental simulations are the representative of processes taking place in the galleries. These studies show that air oxidation induced (i) a significant increase in the amount of DOM and (ii) a major change in the chemistry of the EOM and DOM characterized by the formation of low molecular weight oxygenated molecules. Moreover, comparison between water extracted from altered samples and piezometers shows that the water of the site is not affected by oxidation processes. The piezometer water samples are similar to that extracted from non-altered samples. Biodegradation experiments conducted on non altered and artificially oxidized clay did not show significant changes of fossil and dissolved organic matter. It seems that anaerobic biodegradation is not a major process in the context of disturbances induced by the excavation

High-level radioactive waste (HLW) poses threat to the biosphere. Geological disposal is accepted as a safe way for HLW disposal. Waste canisters made of Sintered Silicon Carbide (SSiC) are proposed and geomechanical safety aspects relating to such SSiC canisters are investigated. First part of the thesis reviews the state-of-the-art and demands for HLW disposal. The reason for considering Silicon Carbide (SiC) as canister material is explained. Especially in terms of corrosion and lifetime, ceramics and especially SiC is superior to metals or concrete. The only concern is its brittle behavior. The second part of the thesis presents results on static and dynamic mechanical properties of SiC in general and in particular for SSiC based on literature review and own lab tests. Although strength values for SiC and especially SSiC are very high, the extreme brittle behavior has to be considered in case of impact or point-like loading. The third and most extensive part of the thesis part contains numerical simulations, which consider most critical potential loading situations during transport and installation of the canisters underground. Both, pure elastic continuum and DEM based models are used considering the following loading situations (critical scenarios): Freefall of canister during transport or installation (FF), Impact by falling rock block at disposal site (RF), Point loading due to accidental insertion of small stone below the canister (PL), Anisotropic earth pressure loading after disposal (EP). Coating to protect the canisters against damage is investigated and preliminary parameters in terms of stiffness and thickness are recommended.

The aim of this work was to study the separate effect of fission fragment damage on the structural integrity and matrix dissolution of uranium dioxide in water. Radiation damage similar to fission damage was created by irradiating bulk undoped and doped ‘SIMFUEL’ disks of UO2, undoped bulk CeO2 and thin films of UO2 and CeO2 with high energy Xe and U ions. The UO2 thin films, with thicknesses in the range of 90 – 150 nm, were deposited onto (001), (110) and (111) orientations of single crystal LSAT (Al10La3O51Sr14Ta7) and YSZ (Yttria-Stabilised Zirconia) substrates. The CeO2 thin films were deposited onto single crystal silicon (001) substrates. Part of the bulk UO2 and CeO2 samples, the thin films of UO2 on the LSAT substrates and the thin films of CeO2 were irradiated with 92 MeV 129Xe23+ ions to a fluence of 4.8 × 1015 ions/cm2 to simulate the damage produced by fission fragments in uranium dioxide nuclear fuel. Part of the bulk UO2 and CeO2 samples and the thin films of UO2 on the YSZ substrates were irradiated with 110 MeV 238U31+ ions to a fluence of 5 × 1010, 5 × 1011 and 5 × 1012 ions/cm2 to study the accumulation of the damage induced. The irradiated and unirradiated samples were studied using scanning electron microscopy (SEM), focused ion beam (FIB), atomic force microscopy (AFM), energy dispersive X-ray (EDX) spectroscopy, electron probe microanalysis (EPMA), X-ray diffraction (XRD), electron backscatter diffraction (EBSD), secondary ion mass spectrometry (SIMS) and X-ray photoelectron spectroscopy (XPS) techniques to characterise the as-produced samples and assess the effects of the ion irradiations. Dissolution experiments were conducted to assess the effect of the Xe ion irradiation on the dissolution of the thin film UO2 samples on the LSAT substrates and the bulk and thin film CeO2 samples. The solutions obtained from the leaching of the irradiated and unirradiated samples were analysed using inductively coupled plasma mass spectrometry (ICP-MS). XRD studies of the bulk UO2 samples showed that the ion irradiations resulted in an increased lattice parameter, microstrain and decreased crystallite size, as expected. The irradiated UO2 thin films on the LSAT substrates underwent significant microstructural and crystallographic rearrangements. It was shown that by irradiating thin films of UO2 with high energy, high fluence ions, it is possible to produce a structure that is similar to a thin slice through the high burn-up structure. It is expected that the ion irradiation induced chemical mixing of the UO2 films with the substrate elements (La, Sr, Al, Ta). As a result, a material similar to a doped SIMFUEL with induced radiation damage was produced.