Glaciation is considered one of the main natural processes that can have a significant impact on the long term performance of DGRs. The northern part of the American continent has been subjected to a series of strong glaciation and deglaciation events over the past million years. Glacial cycles cause loading and unloading, temperature changes and hydraulic head changes at the ground surface. These changes can be classified as transient boundary conditions. It is widely accepted that the periodic pattern of past glacial cycles during the Late Quaternary period are resultant of the Earth’s orbital geometry changes that is expected to continue in the future. Therefore, from the safety perspective of DGRs, such probable events need to be taken into account. The objective of this thesis is to develop a numerical model to investigate the thermo-hydro-mechanical-chemical (THMC) coupled processes that have resulted from long term past and future climate changes and glaciation cycles on a proposed DGR in sedimentary rocks in southern Ontario. The first application is done on a large geological cross section that includes the entire Michigan basin by using a hydro-mechanical (HM) coupled process. The results are compared with field data of anomalous pore water pressures from deep boreholes in sedimentary rocks of southern Ontario. In this work. The modeling results seem to support the hypothesis that at least the underpressures in the Ordovician formation could be partially attributed to past glaciation. The second application is made on site conditions by using the THMC model. The results for the pore water pressure, tracer profiles, permafrost depth and effective stress profile are compared with the available field data, the results show that the solute transport in the natural limestone and shale barrier formations is controlled by diffusion, which provide evidence that the main mechanism of transport at depth is diffusion-dominant. The third application is made on site conditions to determine the effect of underground changes in DGRs due to DGR construction. The results show that future glaciation loads will induce larger increases in effective stresses on the shaft. Furthermore, it is found that hypothetical nuclide transport in a failed shaft can be controlled by diffusion and advection. The simulation results show that the solute transported in a failed shaft can reach the shallow bedrock groundwater zone. These results might imply that a failed shaft will substantially lose its effectiveness as a barrier. The fourth application is proposed to investigate the geochemical evolution of sedimentary host rock in a near field scale. In this part, a new thermo-hydro-mechanical-geochemical simulator (COMSOL-PHREEQC) is developed. It is anticipated that there will be a geochemical reaction within the host rock that results from interaction with the water enriched with the CO2 generated by nuclear waste.

Glaciation is considered one of the main natural processes that can have a significant impact on the long term performance of DGRs. The northern part of the American continent has been subjected to a series of strong glaciation and deglaciation events over the past million years. Glacial cycles cause loading and unloading, temperature changes and hydraulic head changes at the ground surface. These changes can be classified as transient boundary conditions. It is widely accepted that the periodic pattern of past glacial cycles during the Late Quaternary period are resultant of the Earth’s orbital geometry changes that is expected to continue in the future. Therefore, from the safety perspective of DGRs, such probable events need to be taken into account. The objective of this thesis is to develop a numerical model to investigate the thermo-hydro-mechanical-chemical (THMC) coupled processes that have resulted from long term past and future climate changes and glaciation cycles on a proposed DGR in sedimentary rocks in southern Ontario. The first application is done on a large geological cross section that includes the entire Michigan basin by using a hydro-mechanical (HM) coupled process. The results are compared with field data of anomalous pore water pressures from deep boreholes in sedimentary rocks of southern Ontario. In this work. The modeling results seem to support the hypothesis that at least the underpressures in the Ordovician formation could be partially attributed to past glaciation. The second application is made on site conditions by using the THMC model. The results for the pore water pressure, tracer profiles, permafrost depth and effective stress profile are compared with the available field data, the results show that the solute transport in the natural limestone and shale barrier formations is controlled by diffusion, which provide evidence that the main mechanism of transport at depth is diffusion-dominant. The third application is made on site conditions to determine the effect of underground changes in DGRs due to DGR construction. The results show that future glaciation loads will induce larger increases in effective stresses on the shaft. Furthermore, it is found that hypothetical nuclide transport in a failed shaft can be controlled by diffusion and advection. The simulation results show that the solute transported in a failed shaft can reach the shallow bedrock groundwater zone. These results might imply that a failed shaft will substantially lose its effectiveness as a barrier. The fourth application is proposed to investigate the geochemical evolution of sedimentary host rock in a near field scale. In this part, a new thermo-hydro-mechanical-geochemical simulator (COMSOL-PHREEQC) is developed. It is anticipated that there will be a geochemical reaction within the host rock that results from interaction with the water enriched with the CO2 generated by nuclear waste.

As a safe long-term management of nuclear wastes, deep geological repositories (DGRs) have been proposed or currently being constructed in several countries. The host rocks in DGRs are saturated with water after the geological disposal facilities (GDFs) are closed and sealed. Significant gas can be generated due to several processes, e.g., the metal corrosion, water radiolysis or microbial reaction of organic materials, etc. The generated gas is anticipated to span throughout the long-term disposal of waste, which may jeopardize the stability of host rocks. Correspondingly, the performance of GDF will be affected since the host rocks provide a final impediment to the radionuclide transport. As gas migration in saturated host rocks is a highly coupled hydro-mechanical (HM) process, either gas-induced micro-fracturing or macro-fracturing may contribute to the development of preferential gas pathways, which needs to be concerned to ensure the feasibility and safety of geological disposal. Current numerical studies on the gas migration behavior devoted to explaining the experimental phenomena in the gas injection tests conducted on the rock materials, in which some behaviors still cannot be well represented, i.e., gas induced fracturing, volulme dilation, anisotropic radial deformation. Therefore, to better represent the actual physical process of preferential gas flow, two modelling frameworks, i.e., macroscopic HM framework and two-scale HM framework, are proposed in the PhD study. For the macroscopic HM framework, a double porosity model is firstly developed based on the dual continuum method, in which the volumetric strains of the porous continuum (PC) and fractured continuum (FC) are work-conjugated to the respective effective stress level. The treatment in two types of porosity allows us to capture that the opening/closure of the fractures is caused by the interaction between the dilation of the PC and the dilation of the FPM, which is beneficial to describe the gas induced fracturing in an implicit way. Then, an enriched embedded fracture model (EFM) is proposed to address the mechanical behavior of fractures. A hyperbolic relation of fracture deformability is incorporated into the rock matrix, as a result the fractured rock shows a nonlinear elastic behavior, which can capture the stiffness degradation due to fracture opening. The equivalent continuum method is provided to derive the effective compliance tensor, which includes the transverse isotropic matrix and two fracture sets. Using the enriched EFM with a three-dimensional (3D) geometry is able to capture the anisotropic radial deformation during gas migration. Although the macroscopic HM framework is able to capture the major HM behaviors related to preferential gas flow, the development of gas dilatant pathways is still represented in an implicit way. Therefore, a two-scale HM framework is developed to explicitly simulate the development of preferential gas pathways. Initiating from the periodically distributed microstructures with microcracks, the asymptotic homogenization method is used to derive the macroscopic governing equations coupled with the normalized damage variable. The time-dependent damage evolution law is obtained from the microscopic mechanical energy analysis for evolving microcracks. Both time effect and size effect are incorporated in the damage model that will affect the overall HM behavior of rocks. The developed two-scale HM framework with single gas flow can qualitatively capture important behaviors, such as the discrete pathways, localized gas flow, unstabilized fracture branching. More specifically, the simulated results demonstrates that the inter-connection of fractures from gas inlet to outlet is a prerequisite for gas breakthrough, accompanied by large amounts of gas flowing out of the sample and a rapid drop in gas injection pressure. Incorporating water flow in the two-scale framework allows the model to quantitatively reproduce the experimental phenomena observed in the laboratory air injection tests, such as gas pressure evolution and mechanical deformation. More importantly, the model exlpaines that the significant differences in controlling gas breakthrough and mechanical deformation are resulting from the arbitrary nature of microstructural heterogeneities. To account for the gas-water interaction in the two-scale HM framework, a fully coupled two-phase flow and elaso-damage model is developed to simulate the laboratory and in-situ gas injection experiments. The model can quantitatively capture the experimental behaviors, e.g., gas pressure evolution and non-desaturation phenomenon. Furthermore, model results show that the highly localized fracture pathways are the major places where gas and water interacts each other, and as a result the rock is still kept fully saturated. As a whole, the obtained numerical results are synthesized and analyzed, the pros and cons of the developed models are discussed. To better improve the model performance, some recommendations are proposed for the future studies.

Clay shales are currently being assessed as possible host rock formations for the deep geological disposal of radioactive waste. However, one main concern is that the favourable long-term isolation properties of the intact rock mass could be negatively affected by the formation of an excavation damaged zone (EDZ) around the underground openings. This thesis investigated the deformation and failure process of a clay shale, namely Opalinus Clay, with particular focus on the influence of anisotropy on the short-term response of circular tunnels. To achieve this goal, a hybrid continuum-discontinuum numerical approach was used in combination with new field measurements from the Mont Terri underground research laboratory. The response of Opalinus Clay during the excavation of a full-scale emplacement (FE) test tunnel was characterized by geodetic monitoring of wall displacements, radial extensometers and longitudinal inclinometers. The deformation measurements indicated strong directionality induced by the combined effect of in situ stress field and presence of bedding planes striking parallel to the tunnel axis, with the most severe deformation occurring in the direction approximately perpendicular to the material layering. Computer simulations were conducted using a newly-extended combined finite-discrete element method (FEM/DEM), a numerical technique which allows the explicit simulation of brittle fracturing and associated seismicity. The numerical experimentation firstly focused on the laboratory-scale analysis of failure processes (e.g., acoustic activity) in brittle rocks, and on the role of strength and modulus anisotropy in the failure behaviour of Opalinus Clay in tension and compression. The fracturing behaviour of unsupported circular excavations in laminated rock masses was then analyzed under different in situ stress conditions. Lastly, the modelling methodology was applied to the aforementioned FE tunnel to obtain original insights into the possible EDZ formation process around emplacement tunnels for nuclear waste. The calibrated numerical model suggested delamination along bedding planes and subsequent extensional fracturing as key mechanisms of the damage process potentially leading to buckling and spalling phenomena. Overall, the research findings may have a potential impact on the constructability and support design of an underground repository as well as implications for its long-term safety assessment procedure.

Clay shales are currently being assessed as possible host rock formations for the deep geological disposal of radioactive waste. However, one main concern is that the favourable long-term isolation properties of the intact rock mass could be negatively affected by the formation of an excavation damaged zone (EDZ) around the underground openings. This thesis investigated the deformation and failure process of a clay shale, namely Opalinus Clay, with particular focus on the influence of anisotropy on the short-term response of circular tunnels. To achieve this goal, a hybrid continuum-discontinuum numerical approach was used in combination with new field measurements from the Mont Terri underground research laboratory. The response of Opalinus Clay during the excavation of a full-scale emplacement (FE) test tunnel was characterized by geodetic monitoring of wall displacements, radial extensometers and longitudinal inclinometers. The deformation measurements indicated strong directionality induced by the combined effect of in situ stress field and presence of bedding planes striking parallel to the tunnel axis, with the most severe deformation occurring in the direction approximately perpendicular to the material layering. Computer simulations were conducted using a newly-extended combined finite-discrete element method (FEM/DEM), a numerical technique which allows the explicit simulation of brittle fracturing and associated seismicity. The numerical experimentation firstly focused on the laboratory-scale analysis of failure processes (e.g., acoustic activity) in brittle rocks, and on the role of strength and modulus anisotropy in the failure behaviour of Opalinus Clay in tension and compression. The fracturing behaviour of unsupported circular excavations in laminated rock masses was then analyzed under different in situ stress conditions. Lastly, the modelling methodology was applied to the aforementioned FE tunnel to obtain original insights into the possible EDZ formation process around emplacement tunnels for nuclear waste. The calibrated numerical model suggested delamination along bedding planes and subsequent extensional fracturing as key mechanisms of the damage process potentially leading to buckling and spalling phenomena. Overall, the research findings may have a potential impact on the constructability and support design of an underground repository as well as implications for its long-term safety assessment procedure.

The deep geological repository concept is based on “engineered barriers systems (EBS)” that are constructed in the repository and “natural barriers” provided by the surrounding geological environment. The EBS comprises of variety of sub-systems or components, such as the waste form, canister, buffer, backfill, seals, and plugs. Geological disposal is based on the concept of multiple barriers that work together to provide containment. The buffer is made up of densely compacted bentonite or bentonite-sand mix. Bentonite has both mechanical and physico-chemical functions, to fulfill as a barrier material in DGR. The bentonite buffer should hold the containers in place and prevent collapse of the excavation. A plastic deformability of the bentonite is desired to redistribute the stresses that can result from creep in the rock, and prevent transfer of excessive stresses to the canisters. The bentonite buffer must create an impermeable zone around the containers to ensure that the radionuclide released from the vitrified waste is limited by diffusive transport rather than advective transport in groundwater. Another important property of the highly compacted bentonite is its swelling potential. Its swelling potential should be as high as possible, to guarantee the sealing of any cracks occurring in the buffer material or in the storage gallery and thus ensure good imperviousness. Besides its mechanical function, bentonite buffer must sorb escaping radionuclides and thus retard their migration to the geo-environment. The bentonite buffer must retain its mechanical and physico-chemical functions over a span of several hundred thousand years to fulfill its role as a containment barrier in DGR. The bentonite buffer should maintain its physico-chemical and hydro-mechanical integrity on exposure to groundwater. 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. Japan has identified Kunigel VI bentonite, South Korea-Kyungju bentonite, China-GMZ bentonite, Belgium-FoCa clay, Sweden-MX-80 bentonite, Spain-FEBEX bentonite and Canada-Avonseal bentonite as candidate bentonite buffer for deep geological repository program. Bentonite from Barmer (Rajasthan State) was identified as suitable buffer for use in Indian deep geological repositories. The influence of moisture and dissolved salt migration on the physico-chemical and hydro-mechanical properties of Barmer bentonite has not been examined. The study is important to understand the clay’s behaviour under deep geological repository conditions, where, the bentonite buffer would come in contact with groundwater. Infiltration of groundwater with variable chemical composition could alter the physico-chemical and hydro-mechanical properties of the clay. The objectives of the thesis are as follows: Examine the influence of permeation of distilled water (DW) and synthetic ground water (SGW) solutions under constant volume condition on suction, physico-chemical and moisture content/dry density characteristics of compacted Barmer bentonite specimens as function of permeation period (maximum permeation period– 30 days). Examine the influence of variation in dry density and gravimetric water content as consequence of DW and SGW solution permeation on swell pressure and unconfined compression strength of Barmer bentonite specimens. Compare experimental swell pressures of re-constituted bentonite specimens with swell pressures predicted by diffuse double layer models. Examine the influence of total dissolved solids (TDS) concentration of permeating solution on the unsaturated permeability of compacted Barmer bentonite specimens. Organization of thesis: After the first introductory chapter, a detailed review of literature is performed in Chapter 2 to review the physicochemical, mineralogical and hydro-mechanical properties of bentonites identified as buffer materials for deep geological repositories of various countries. Based on current understanding and need to perform similar studies with Barmer clay, the chapter develops the scope and objectives of the study. Chapter 3 presents a detailed experimental program of the study. Chapter 4 examines the influence of permeation of distilled water (DW) and synthetic groundwater (SGW) solutions (under constant volume conditions) on the total suction of compacted bentonite specimens at two locations in the clay. The influence of variation in dry density on the moisture migration-suction inter-relations of compacted bentonite specimens is also examined. The associated changes of DW and SGW solution migration under constant volume conditions on the physico-chemical properties, water content and dry density of compacted Barmer bentonite specimens are also examined. The experimental results brought out that matric suction mainly contributed (75 to 92 %) to total suction of the permeated specimens; the permeated specimens experienced reduction in matric suction with increase in gravimetric water content from increase in degree of saturation. Osmotic suction contributed to 10 to 25 % of the total suction of the permeated specimens and was observed to increase with gravimetric water content due to solubilization of salts contained in the voids of the compacted bentonite specimens. The total suction of compacted Barmer bentonite specimen was responsive to the total dissolved solids concentration of the permeating solutions as the specimen permeated with more saline solution (higher TDS value) exhibited lesser total suction. Upon permeation with DW and SGW solutions, the CEC of bentonite was unaltered, while, pH and TDS values were affected. Softening of the bentonite clay occurred from increase in water content and existence of compression zones (material used to seal 1mm gap in relative humidity probe aperture) that in turn facilitated dissipation of swelling stress leading to reduction in dry density values. Chapter 5 examines influence of reduction in dry density and increase in water content on the swell pressure and compression strength characteristics of compacted Barmer bentonite specimens upon DW and SGW solution migration as the results could provide insight into possible deviations from the design properties upon wetting of bentonite buffer by groundwater under deep geological repository conditions. The experimental swelling pressures are also compared with those predicted by Gouy-Chapman diffuse double layer theory. The dry density of 1.6 Mg/m specimens permeated with DW and SGW solutions reduced to 1.59 to 1.36 Mg/m and water contents increased to 18.9 to 27 % on permeation with distilled water and SGW solutions for 30 days. The reductions in dry density and increase in water content caused 30 to 70 % reductions in swell pressures and 31 to 74 % decrease in unconfined compression strength values. Specimens initially compacted to dry density of 1.8 Mg/m, experienced reduction in dry density ranging from 1.79 to 1.52 Mg/m and increase in water content from 18.6 to 24.2 % on permeation of DW and SGW solutions for 30 days. These reductions in dry density and increase in water caused the swell pressures to reduce from 4 to 55 % and unconfined compressive strengths to reduce by 31 to 67 %. Comparison of swell pressures gave -8 to 127 % variations between theoretical (from DDL theory) and experimental values due to errors associated with estimation of surface area and dissolved salt concentrations in pore water. Chapter 6 examines the influence of salinity of permeating solution on the unsaturated permeability of compacted Barmer bentonite specimens. The salinity of permeants was varied by permeating distilled water (DW) and synthetic ground water solutions under constant volume conditions over maximum period of 30 days. Experimental results showed that the saturated permeability coefficients (ksat) of specimens compacted to 1.6 Mg/m, responded to variations in TDS of the permeant. Comparatively, the ksat values of specimens compacted to 1.8 Mg/mwere unaffected by variation in TDS of the permeant. Permeation of DW and SGW solutions decreased the ksat values with time from cation hydration and growth of diffuse ion layers for both, 1.6 and 1.8 Mg/mseries specimens. Increase in gravimetric water content from DW and SGW permeation increased the kunsat values of 1.6 Mg/m specimens from reduction in total suction. Re-orientation of soil structure mobilized larger kunsat values for specimens permeated with SGW solutions than DW at similar total suction. Permeation of DW and SGW solutions had lesser impact on kunsat values of the 1.8 Mg/m specimens in comparison to the 1.6 Mg/m series specimens. Further at both densities, the influence of permeation was more evident at location closer to hydration surface. Chapter 7 summarizes the main findings of this study.

Sedimentary rocks are characterized with very low permeability (in the order of 10-22 m2), low diffusivity, a possible self-healing of fractures, and a good capacity to retard radionuclide transport. In recent years, sedimentary rocks are investigated by many research groups for their suitability for the disposal of radioactive waste. Development of deep geologic repositories (DGRs) for the storage of radioactive waste within these formations causes progressive modification to the state of stress, to the groundwater regime, and to the chemistry of the rock mass. Thermal effects due to the ongoing nuclear activity can cause additional disturbances to the system. All these changes in the system are coupled and time-dependent processes. These coupled processes can result in the development of an excavation damaged zone (EDZ) around excavations. More permeable than the undisturbed rock, the EDZ is likely to be a preferential pathway for water and gas flow. Consequently, the EDZ could be a potential exit pathway for the radioactive waste to biosphere. An investigation of the Hydraulic-Mechanical (HM) and Thermal-Hydraulic-Mechanical-Chemical (THMC) behaviour of sedimentary rock formations is essential for the development of DGRs within such formations. This research work consists of (1) an experimental investigation of the mechanical behaviour of the anisotropic Tournemire argillite, (2) modeling of the mechanical behaviour of the Tournemire argillite, and (3) numerical simulations of the mechanical and hydromechanical behavior of two host sedimentary rocks, the Tournemire argillite and Cobourg limestone, for deep geological repository for nuclear wastes. The experimental program includes the measurements of the physical properties of the Tournemire argillite and its mechanical response to loading during uniaxial compression tests, triaxial compression tests with different confining pressures, unconfined and confined cyclic compression tests, Brazilian tests, and creep tests. Also, acoustic emission events are recorded to detect the initiation and propagation of microcracks within the rock during the uniaxial testing. The approach for modeling the mechanical behaviour of the Tournemire argillite consists of four components: elastic properties of the argillite, a damage model, the proposed concept of mobilized strength parameters, and the classical theory of elastoplasticity. The combination of the four components results in an elastoplastic-damage model for describing the mechanical behaviour of the Tournemire argillite. The capabilities of the model are evaluated by simulating laboratory experiments. Numerical simulations consist of: (1) a numerical simulation of a mine-by-test experiment at the Tournemire site (France), and (2) numerical simulations of the mechanical and hydromechanical behaviour of the Cobourg limestone within the EDZ (Canada). The parameters influencing the initiation and evolution of EDZ over time in sedimentary rocks are discussed.

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.

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.

Sedimentary rocks are characterized with very low permeability (in the order of 10-22 m2), low diffusivity, a possible self-healing of fractures, and a good capacity to retard radionuclide transport. In recent years, sedimentary rocks are investigated by many research groups for their suitability for the disposal of radioactive waste. Development of deep geologic repositories (DGRs) for the storage of radioactive waste within these formations causes progressive modification to the state of stress, to the groundwater regime, and to the chemistry of the rock mass. Thermal effects due to the ongoing nuclear activity can cause additional disturbances to the system. All these changes in the system are coupled and time-dependent processes. These coupled processes can result in the development of an excavation damaged zone (EDZ) around excavations. More permeable than the undisturbed rock, the EDZ is likely to be a preferential pathway for water and gas flow. Consequently, the EDZ could be a potential exit pathway for the radioactive waste to biosphere. An investigation of the Hydraulic-Mechanical (HM) and Thermal-Hydraulic-Mechanical-Chemical (THMC) behaviour of sedimentary rock formations is essential for the development of DGRs within such formations. This research work consists of (1) an experimental investigation of the mechanical behaviour of the anisotropic Tournemire argillite, (2) modeling of the mechanical behaviour of the Tournemire argillite, and (3) numerical simulations of the mechanical and hydromechanical behavior of two host sedimentary rocks, the Tournemire argillite and Cobourg limestone, for deep geological repository for nuclear wastes. The experimental program includes the measurements of the physical properties of the Tournemire argillite and its mechanical response to loading during uniaxial compression tests, triaxial compression tests with different confining pressures, unconfined and confined cyclic compression tests, Brazilian tests, and creep tests. Also, acoustic emission events are recorded to detect the initiation and propagation of microcracks within the rock during the uniaxial testing. The approach for modeling the mechanical behaviour of the Tournemire argillite consists of four components: elastic properties of the argillite, a damage model, the proposed concept of mobilized strength parameters, and the classical theory of elastoplasticity. The combination of the four components results in an elastoplastic-damage model for describing the mechanical behaviour of the Tournemire argillite. The capabilities of the model are evaluated by simulating laboratory experiments. Numerical simulations consist of: (1) a numerical simulation of a mine-by-test experiment at the Tournemire site (France), and (2) numerical simulations of the mechanical and hydromechanical behaviour of the Cobourg limestone within the EDZ (Canada). The parameters influencing the initiation and evolution of EDZ over time in sedimentary rocks are discussed.