Deep geological repository (DGR) for disposal of high-level radioactive waste (HLW) is designed to rely on successive superimposed barrier systems to isolate the waste from the biosphere. This multiple barrier system comprises the natural geological barrier provided by the repository host rock and its surrounding and an engineered barrier system (EBS). The EBS represents the synthetic, engineered materials placed within the natural barrier, comprising array of components such as waste form, waste canisters, buffer materials, backfill and seals. The buffer will enclose the waste canisters from all directions and act as a barrier between canisters and host rock of the repository. It is designed to stabilise the evolving thermo-hydro-mechanical-chemical stresses in the repository over a long period (nearly 1000 years) to retard radionuclides from reaching biosphere. Bentonite clay or bentonite-sand mix have been chosen as buffer materials in EBS design in various countries pursuing deep geological repository method. The bentonite buffer is the most important barrier among the other EBS components for a geological repository. The safety of repository depends to a large extent on proper functioning of buffer over a very long period of time during which it must remain physically, chemically and mineralogically stable. The long term stability of bentonite buffer depends on varying temperature and evolution of groundwater composition of host rocks in a complex way. The groundwater in the vicinity of deep crystalline rock is often characterized by high solute concentrations and the geotechnical engineering response of bentonite buffer could be affected by the dissolved salt concentration of the inflowing ground water. Also during the initial period, radiogenic heat produced in waste canisters would radiate into buffer and the heat generated would lead to drying and some shrinkage of bentonite buffer close to canister. This could alter the dry density, moisture content and in turn the hydro-mechanical properties of bentonite buffer in DGR conditions. India has variety of bentonite deposits in North-Western states of Rajasthan and Gujarat. Previous studies on Indian bentonites suggest that bentonite from Barmer district of Rajasthan (termed as Barmer-1 bentonite) is suitable to serve as buffer material in DGR conditions. Nuclear power agencies of several countries have identified suitable bentonites for use as buffer in DGR through laboratory experiments and large scale underground testing facilities. Physico-chemical, mineralogical and engineering properties of Kunigel VI, Kyungju, GMZ, FoCa clay, MX-80, FEBEX and Avonseal bentonites have been extensively studied by Japan, South Korea, China, Belgium, Sweden, Spain, Canada. It is hence essential to examine the suitability of Barmer-1 bentonite as potential buffer in DGR and compare its physico-chemical and hydromechanical properties with bentonite buffers identified by other countries. The significant factors that impact the long-term stability of bentonite buffer in DGR include variations in moisture content, dry density and pore water chemistry. With a view to address these issues, the hydromechanical response of 70 % Barmer-1 bentonite + 30 % river sand mix (termed bentonite enhanced sand, BES specimens) under varying moisture content, dry density and pore water salt concentration conditions have been examined. The broad scope of the work includes: 1) Characterise the physico-chemical and hydro-mechanical properties of Barmer-1 bentonite from Rajasthan, India and compare its properties with bentonite buffers reported in literature. 2) Examine the influence of variations in dissolved salt concentration (of infiltrating solution), dry density and moisture content of compacted BES specimens on their hydro-mechanical response; the hydro-mechanical properties include, swell pressure, soil water characteristic curve (SWCC), unsaturated hydraulic conductivity, moisture diffusivity and unconfined compression strength. Organization of thesis: After the first introductory chapter, a detailed review of literature is performed to highlight the need for detailed characterisation of physico-chemical and hydromechanical properties of Barmer-1 bentonite for its possible application in DGR in the Indian context. Further, existing literature on hydro-mechanical response of bentonite buffer to changes in physical (degree of saturation/moisture content, dry density) and physico-chemical (solute concentration in pore water) is reviewed to define the scope and objectives of the present thesis in Chapter 2. Chapter 3 presents a detailed experimental programme of the study. Chapter 4 characterises Barmer-1 bentonite for physico-chemical (cation exchange capacity, pore water salinity, exchangeable sodium percentage) and hydro-mechanical properties, such as, swell pressure, saturated permeability, soil water characteristic curve (SWCC) and unconfined compression strength. The properties of Barmer-1 bentonite are compared with bentonite buffers reported in literature and generalized equations for determining swell pressure and saturated permeability coefficient of bentonite buffers are arrived at. Chapter 5 describes a method to determine solute concentrations in the inter-lamellar and free-solutions of compacted BES (bentonite enhanced sand) specimens. The solute concentrations in micro and macro pore solutions are used to examine the role of osmotic flow on swell pressures developed by compacted BES specimens (dry density 1.50-2.00 Mg/m3) inundated with distilled water and NaCl solutions (1000-5000 mg/L). The number of hydration layers developed by the compacted BES specimens on inundation with salt solutions in constant volume swell pressure tests is controlled by cation hydration/osmotic flow. The cation hydration of specimens compacted to dry density of 2.00 Mg/m3 is mainly driven by matric suction prevailing in the clay microtructure as the number of hydration layers developed at wetting equilibrium are independent of the total dissolved solids (TDS) of the wetting solution. Consequently, the swell pressures of specimens compacted to 2.00 Mg/m3 were insensitive to the salt concentration of the inundating solution. The cation hydration of specimens compacted to dry density of 1.50 Mg/m3 is driven by both matric suction (prevailing in the clay micro-structure) and osmotic flow as the number of hydration layers developed at wetting equilibrium is sensitive to the TDS of the wetting solution. Expectedly, the swell pressures of specimens compacted to 1.50 Mg/m3 responded to changes in salt concentration of the inundating solution. The 1.75 Mg/m3 specimens show behaviour that is intermediate to the 1.50 and 2.00 Mg/m3 series specimens. Chapter 6 examines the influence of initial degree of saturation on swell pressures developed by the compacted BES specimens (dry density range: 1.40- 2.00 Mg/m3) on wetting with distilled water from micro-structural considerations. The micro-structure of the bentonite specimens are examined in the compacted and wetted states by performing X-ray diffraction measurements. The initial degree of saturation is varied by adding requisite amount of distilled water to the oven-dried BES mix and compacting the moist mixes to the desired density. The montmorillonite fraction in the BES specimens is responsible for moisture absorption during compaction and development of swell pressure in the constant volume oedometer tests. Consequently, it was considered reasonable to calculate degree of saturation based on EMDD (effective montmorillonite dry density) values and correlate the developed swell pressure values with degree of saturation of montmorillonite voids (Sr,MF). XRD measurements with compacted and wetted specimens demonstrated that if specimens of density series developed similar number of hydration layers on wetting under constant volume condition they exhibited similar swell pressures, as was the case for specimens belonging to 1.40 and 1.50 Mg/m3 series. With specimens belonging to 1.75 and 2.00 Mg/m3 series, greater number of hydration layers were developed by specimens that were less saturated initially (smaller initial Sr,MF) and consequently such specimens developed larger swell pressures. When specimens developed similar number of hydration layers in the wetted state, the compaction dry density determined the swell pressure. Chapter 7 examines the influence of salt concentration of infiltrating solution (sodium chloride concentration ranges from 1000- 5000 mg/L) on SWCC relations, unsaturated permeability and moisture diffusivity of compacted BES specimens. Analysis of the experimental and Brooks and Corey best fit plots revealed that infiltration of sodium chloride solutions had progressively lesser influence on the micro-structure and consequently on the SWCC relations with increase in dry density of the compacted specimens. The micro-structure and SWCC relations of specimens compacted to 1.50 Mg/m3 were most affected, specimens compacted to 1.75 Mg/m3 were less affected, while specimens compacted to 2.00 Mg/m3 were unaffected by infiltration of sodium chloride solutions. Variations in dry density of compacted bentonite impacts the pore space available for moisture flow, while, salinity of wetting fluid impacts the pore structure from associated physico-chemical changes in clay structure. Experimental results showed that the unsaturated permeability coefficient is insensitive to variations in dry density and solute concentration of wetting liquid, while, the effective hydraulic diffusivity is impacted by variations in these parameters. Chapter 8 summarises the major findings of the study.

Cette thèse concerne la caractérisation expérimentale d’un sable limoneux provenant du barrage de Livet – Gavet (38) dans le cadre du projet ANR TerreDurable avec plusieurs objectifs : 1- Caractériser au travers d’essais de laboratoire le comportement hydromécanique d’un sable fin limoneux (sol A1 dans la classification GTR) en fonction de son état de saturation. Lors de cette étude, un accent particulier est porté sur la caractérisation de ce comportement dans le domaine proche de la saturation. 2- Interpréter le comportement hydrique du matériau sur chemin de drainage – imbibition en relation avec l’analyse de sa microstructure. 3- Fournir d’un point de vue général une base de données et d’analyses exhaustive permettant le développement et la calibration de modèles de comportement des sols fins proches de la saturation, en particulier en considérant des chemins de chargement hydromécanique complexes. Pour l’ensemble de cette étude, le matériau est considéré sous deux états : soit à l’état de pâte (matériau normalement consolidé) préparée à une teneur en eau proche de la limite de liquidité, soit sous forme compactée (matériau sur-consolidé) à différentes énergies de compactage et différentes teneurs en eau initiales. / This thesis concerns the experimental characterization of a silty sand from the Livet - Gavet dam (38) as part of the ANR TerreDurable project, for following objectives: 1- Through laboratory tests, characterize the hydro-mechanical behaviour of a fine silty sand (Type A1 in the GTR classification) according to its saturation state. In this study, particular emphasis is placed on the characterization of this behaviour in the near-saturated domain. 2- Interpret the water behaviour of material on the drainage - imbibition cycles, in relation to the analysis of its microstructure. 3- From a general point of view, provide a comprehensive database and analysis allowing the development and calibration of models of near-saturated fine soil's behaviour, in particular, by considering complex hydro-mechanical loading paths. For all tests in this study, the material is considered in two states: either in the state of paste (normally consolidated material) prepared at water content close to the limit of liquidity, or in compacted state (over consolidated material) at different compaction energies and different initial water contents.

Geotechnische Problem- und Fragestellungen befassen sich zunehmend mit der komplexen Interaktion unterschiedlicher physikalischer Prozesse. Ein Beispiel sind hydro-mechanische Wechselwirkungen, die in verschiedenen Anwendungsbereichen eine große Rolle spielen (Hydraulic Fracturing, Bewertung von Barriereintegrität, Böschungsanalysen, etc.). Numerische Simulationen helfen dabei, umfangreiche multiphysikalische Vorgänge abzubilden. Zur hinreichend genauen und effizienten Bearbeitung kann es jedoch sein, dass die Anwendung eines einzelnen spezialisierten Softwarepaketes nicht ausreicht und nur Softwarekopplungen Abhilfe schaffen. Die vorliegende Arbeit erweitert die geomechanische Komplexität einer hydro-mechanischen Kopplung auf visko-elasto-plastisches Materialverhalten im Salinar. Betrachtet werden langandauernde und großräumig induzierte Fluidbewegungen in den durch Volumenkonvergenz charakterisierten lösungserfüllten Abbauen in einem generischen Kali- bzw. Steinsalzbergwerk. Zur Bearbeitung der Problemstellung wird eine grundlegende Methode zur Kopplung der numerischen Codes FLAC3D und Ansys Fluent entwickelt, detailliert vorgestellt und verifiziert. Unterschiedliche Modellszenarien in Bezug auf die initiale Fluidverteilung simulieren eindrucksvoll das Strömungsverhalten im generischen Grubenmodell unter Ausbildung eines freien Fluidspiegels oder eines Überdrucks im eingeschlossenen Fluid. Die Ergebnisse werden umfassend analysiert und das Potenzial zu Effizienzsteigerung durch die Softwarekopplung aufgezeigt. / Geotechnical problems and questions are progressively dealing with complex interactions of different physical processes. An example is hydro-mechanical coupling playing an important role in various research topics and applications (e.g. hydraulic fracturing, assessment of barrier integrity and slope analysis). Numerical simulations help to model extensive multi-physical processes. However, for an accurate and efficient processing, using a single specialized numerical code may not be sufficient and solutions can be obtained only with software couplings. The presented work extends the geomechanically complexity of a hydro-mechanical coupling by visco-elasto-plastic material behaviour in salt formations considering long-lasting and large-scale induced fluid flow within solution-filled cavities in a generic potash or rock salt mine, due to volume convergence. For solving this problem, a basic method for coupling the numerical codes FLAC3D and Ansys Fluent is developed, presented, and verified in detail. Different model scenarios in respect to initial fluid saturation are simulating the fluid flow in the generic mine model, depicting either a free fluid surface or an excess pressure in the trapped fluid. The results are analysed, and the potential for the increase of efficiency through the software coupling of FLAC3D and Ansys Fluent is demonstrated.

This thesis is of the cumulative form, i.e. four peer-reviewed journal publications documenting the research are presented here (see appendices D through G). The sections leading up to the journal publications aim to provide a framework and context for the reader, in which the aforementioned journal publications should be seen: Eyes set on this goal, the thesis starts out by introducing the context of deep geological disposal of heat generating nuclear waste in argillaceous host rock formations, the particularities of argillites as host rock as well as the modelling concept including the theory of porous media. Next, a derivation and discussion of the principal partial differential equations governing the conservation of mass, energy and momentum as well as of constitutive laws is provided. A discussion and conclusion are presented in order to finalise the framing of this thesis. The research questions in this thesis have three focus points: First, the validity (and limits of validity) of the given thermo-hydro-mechanical conceptual modelling approaches and associated assumptions is explored. Second, the numerical implementations are thoroughly tested and demonstrated. Third, the system behaviour of deep geological repositories in argillaceous host rocks is investigated.:List of Figures IV List of Tables IV 1 Introduction p. 1 2 Research questions p.2 3 Disposal in argillaceous host rock p.4 3.1 Formation and properties of relevant argillites p.4 3.2 Barrier integrity p.5 3.3 Physical processes in deep geological radioactive waste disposal p.6 3.3.1 Thermal processes p.7 3.3.2 Hydraulicandaeraulicprocessesp.8 3.3.3 Mechanical processes p.8 3.3.4 Chemicalandbiologicalprocessesp.10 3.4 Process couplings p.10 3.4.1 Thermo-mechanical coupling p.10 3.4.2 Hydro-mechanical coupling p.11 3.4.3 Thermo-hydraulic coupling p.12 3.4.4 Aero-hydraulic coupling p.13 4 Modelling approach p.13 4.1 Concept of porous media p.13 4.2 Process equations p.15 4.2.1 Capillary pressure p.15 4.2.2 Component mass balance p.16 4.2.3 Solid mass balance p.19 4.2.4 Hydraulic constitutive laws p.22 4.2.5 Momentum balance p.29 4.2.6 Energy balance p.32 4.3 Numerical solution of process equations p.35 5 Summary of results p.36 6 Conclusion and outlook p.46 References p.47 Appendix A: Further peer reviewed publications p. 60 Appendix B:Technical reports p. 61 Appendix C: Conference contributions p. 62 Appendix D: Pitz et al. (2023a) p. 67 Appendix E: Pitz et al. (2023b) p. 88 Appendix F: Pitz et al. (2024a) p. 113 Appendix G: Pitz et al. (2024b) p.128