Search Results (13)

Carbon dioxide (CO₂) geosequestration is a critical technology for reducing greenhouse gas emissions, with shale caprocks, such as Opalinus Clay (OPA), serving as essential seals to prevent CO₂ leakage. This study employs computational fluid dynamics and finite element analysis to investigate the hydromechanical behavior of OPA during CO₂ injection, integrating qualitative and quantitative insights. Validated numerical models indicate that capillary forces are the most critical factor in determining the material’s reaction, with an entry capillary pressure of 2–6 MPa serving as a significant threshold for CO₂ breakthrough. The numbers show that increasing the stress loading from 5 to 30 MPa lowers permeability by 0.3–0.45% for every 5 MPa increase. Porosity, on the other hand, drops by 9.2–9.4% under the same conditions. The OPA is compacted, and axial displacements confirm numerical models with an error margin of less than 10%. Saturation analysis demonstrates that CO₂ penetration becomes stronger at higher injection pressures (8–12 MPa), although capillary barriers slow migration until critical pressures are reached. These results demonstrate how OPA’s geomechanical stability and fluid dynamics interact, indicating that it may be utilized as a caprock for CO₂ storage. The study provides valuable insights for enhancing injection techniques and assessing the safety of long-term storage. Full article

CO₂ geosequestration is an important contributor to United Nations Sustainable Development Goal 13, i.e., Climate Action, which states a global Net-Zero CO₂ emissions by 2050. A potential impact of CO₂ geosequestration in depleted oil and gas reservoirs is the variations in induced pressure across the caprocks, which can lead to significant local variations in CO₂ saturation. A detailed understanding of the relationship between the pressure gradient across the caprock and local CO₂ concentration is of utmost importance for assessing the potential of CO₂ geosequestration. Achieving this through experimental techniques is extremely difficult, and thus, we employ a coupled Computational Fluid Dynamics (CFD) and Finite Element Method (FEM) based solver to mimic sub-critical CO₂ injection in Opalinus Clay under various pressure gradients across the sample. The geomechanical and multiphase flow modelling utilising Darcy Law helps evaluate local variations in CO₂ concentration in Opalinus Clay. Well-validated numerical results indicate favourable sub-critical CO₂ geosequestration under a positive pressure gradient across Opalinus Clay. In the absence of a positive pressure gradient, a peak CO₂ concentration of 5% has been recorded, which increases substantially (above 90%) as the pressure gradient across the sample increases. Full article

During the long-term storage of radioactive waste, the continuous generation of gas in the disposal area may influence the integrity of host rock. Thus, the investigation of gas migration and breakthrough in low-permeability rock is indispensable for the stability assessment. In this work, the pore space models of four potential host rocks (Boom clay, COx argillite, Opalinus clay, and Beishan granite) were generated via the binarization of the Gaussian random field. This method provides a randomly formed pore network that does rely on an initial definition of pore shape. The constructed models were analyzed and validated by using the mathematical morphology. A numerical calculation scenario of gas breakthrough on the basis of the Young–Laplace equation was proposed and applied. Results show that the gas breakthrough pressures are 2.62–4.11 MPa in Boom clay and 3.72–4.27 MPa in COx argillite. It enhances the idea that the capillary-induced gas breakthrough is possible at pressures lower than the fracture threshold. For Opalinus clay and Beishan granite, no connected pathway exists, and the breakthrough is more likely to occur through pathway dilation or fractures. The presented method has the advantage of experimental reproducibility and brings a new idea for the investigation of fluid migration in low-permeability rocks. Full article

An in situ and a batch heating experiment were applied on the fine-grained sediments of the Opalinus Clay from Mont Terri (Switzerland) and the Boom Clay of Mol (Belgium), both being currently studied as potential host formations for deep nuclear waste disposal. The purpose was here to test the impact of a 100 °C temperature rise that is expected to be produced by nuclear waste in deep repositories. The experiment on the Opalinus Clay mimicked real conditions with 8-months operating heating devices stored in core drillings into the rock. The comparison of the major, trace, rare-earth elemental contents and of the whole-rock K-Ar data before and after heating shows only a few variations beyond analytical uncertainty. However, the necessary drillings for collecting control samples after the experiment added an unexpected uncertainty to the analyses due to the natural heterogeneity of the rock formation, even if very limited. To overcome this aspect, Boom Clay ground material was subjected to a batch experiment in sealed containers during several years. The drawback being here the fact that controls were limited with, however, similar reproducible results that also suggest limited elemental transfers from rock size into that of the <2 μm material, unless the whole rocks lost more elements than the fine fractions. The analyses generated by the two experiments point to identical conclusions: a visible degassing and dewatering of the minerals that did not induce a visible alteration/degradation of the host-rock safety characteristics after the short-term temperature increase. Full article

Transport properties of potential host rocks for nuclear waste disposal are typically determined in laboratory or in-situ experiments under geochemically controlled and constant conditions. Such a homogeneous assumption is no longer applicable on the host rock scale as can be seen from the pore water profiles of the potential host rock Opalinus Clay at Mont Terri (Switzerland). The embedding aquifers are the hydro-geological boundaries, that established gradients in the 210 m thick low permeable section through diffusive exchange over millions of years. Present-day pore water profiles were confirmed by a data-driven as well as by a conceptual scenario. Based on the modelled profiles, the influence of the geochemical gradient on uranium migration was quantified by comparing the distances after one million years with results of common homogeneous models. Considering the heterogeneous system, uranium migrated up to 24 m farther through the formation depending on the source term position within the gradient and on the partial pressure of carbon dioxide ${\mathrm{pCO}}_2$ of the system. Migration lengths were almost equal for single- and multicomponent diffusion. Differences can predominantly be attributed to changes in the sorption capacity, whereby ${\mathrm{pCO}}_2$ governs how strong uranium migration is affected by the geochemical gradient. Thus, the governing parameters for uranium migration in the Opalinus Clay can be ordered in descending priority: ${\mathrm{pCO}}_2$, geochemical gradients, mineralogical heterogeneity. Full article

Compacted bentonite is currently being considered as a suitable backfill material for sealing underground repositories for radioactive waste as part of a multi-barrier concept. Although showing favorable properties for this purpose (swelling capability, low permeability, and high adsorption capacity), the best choice of material remains unclear. The goal of this study was to examine and compare the hydration behavior of a Milos (Greek) Ca-bentonite sample (SD80) in two types of simulated ground water: (i) Opalinus clay pore water, and (ii) a diluted saline cap rock brine using a confined volume, flow-through reaction cell adapted for in situ monitoring by X-ray diffraction. Based on wet-cell X-ray diffractometry (XRD) and calculations with the software CALCMIX of the smectite d(001) reflection, it was possible to quantify the abundance of water layers (WL) in the interlayer spaces and the amount of non-interlayer water uptake during hydration using the two types of solutions. This was done by varying WL distributions to fit the CALCMIX-simulated XRD model to the observed data. Hydrating SD80 bentonite with Opalinus clay pore water resulted in the formation of a dominant mixture of 3- and 4-WLs. The preservation of ca. 10% 1-WLs and the apparent disappearance of 2-WLs in this hydrated sample are attributed to small quantities of interlayer K (ca. 8% of exchangeable cations). The SD80 bentonite of equivalent packing density that was hydrated in diluted cap rock brine also contained ca. 15% 1-WLs, associated with a slightly higher concentration of interlayer K. However, this sample showed notable suppression of WL thickness with 2- and 3-WLs dominating in the steady-state condition. This effect is to be expected for the higher salt content of the brine but the observed generation of CO₂ gas in this experiment, derived from enhanced dissolution of calcite, may have contributed to the suppression of WL thickness. Based on a comparison with all published wet-cell bentonite hydration experiments, the ratio of packing density to the total layer charge of smectite is suggested as a useful proxy for predicting the relative amounts of interlayer and non-interlayer water incorporated during hydration. Such information is important for assessing the subsequent rates of chemical transport through the bentonite barrier. Full article

Shaft seals are geotechnical barriers in nuclear waste deposits and underground mines. The Sandwich sealing system consists of alternating sealing segments (DS) of bentonite and equipotential segments (ES). MiniSandwich experiments were performed with blended Ca-bentonite (90 mm diameter and 125 mm height) to study hydration, swelling, solute transport and cation exchange during hydration with A3 Pearson water, which resembles pore water of Opalinus Clay Formation at sandy facies. Two experiments were run in parallel with DS installed either in one-layer hydrate state (1W) or in air-dry two-layer hydrate (2W) state. Breakthrough at 0.3 MPa injection pressure occurred after 20 days and the fluid inlet was closed after 543 days, where 4289 mL and 2984 mL, respectively, passed both cells. Final hydraulic permeability was 2.0–2.7 × 10⁻¹⁷ m². Cells were kept for another 142 days before dismantling. Swelling of DS resulted in slight compaction of ES. No changes in the mineralogy of the DS and ES material despite precipitated halite and sulfates occurred. Overall cation exchange capacity of the DS does not change, maintaining an overall value of 72 ± 2 cmol(+)/kg. Exchangeable Na⁺ strongly increased while exchangeable Ca²⁺ decreased. Exchangeable Mg²⁺ and K⁺ remained nearly constant. Sodium concentration in the outflow indicated two different exchange processes while the concentration of calcium and magnesium decreased potentially. Concentration of sulfate increased in the outflow, until it reached a constant value and chloride concentration decreased to a minimum before it slightly increased to a constant value. The available data set will be used to adapt numerical models for a mechanism-based description of the observed physical and geochemical processes. Full article

Shales contain magnetic minerals generally at very low concentrations. In the early stages of diagenesis, the inherited magnetic minerals are altered, while magnetic nanominerals are formed. In this study, we proposed a study of shales over a stratigraphic thickness of 1.3 km from a borehole in the Paris basin (Borehole EST 433, France), and shales from the same formation (Opalinus Clay) collected in seven boreholes in the Jura molasse basin (Swiss). Magnetic measurements at experimental temperatures <30 K allowed the formation of a proxy of magnetite nanograins named PM. We showed that some of these nanograins formed around the pyrite grains, probably under the action of temperature and organic matter. PM was then compared to the maturity values of the organic matter. We found a correlation between PM and the percentage of reflectance of vitrinite. The shales from both Paris and molassic Swiss basins showed very comparable magnetic characteristics for a given maturity level. The magnetic study therefore provided constraints on the maturity level of the shales in the oil window area. Our study showed that PM can be used as a geothermometer in shales in which CaCO₃ is lower than 60%. Full article

Bentonite is currently proposed as a potential backfill material for sealing high-level radioactive waste in underground repositories due to its low hydraulic conductivity, self-sealing ability and high adsorption capability. However, saline pore waters, high temperatures and the influence of microbes may cause mineralogical changes and affect the long-term performance of the bentonite barrier system. In this study, long-term static batch experiments were carried out at 25 °C and 90 °C for one and two years using two different industrial bentonites (SD80 from Greece, B36 from Slovakia) and two types of aqueous solutions, which simulated (a) Opalinus clay pore water with a salinity of 19 g·L⁻¹, and (b) diluted cap rock solution with a salinity of 155 g·L⁻¹. The bentonites were prepared with and without organic substrates to study the microbial community and their potential influence on bentonite mineralogy. Smectite alteration was dominated by metal ion substitutions, changes in layer charge and delamination during water–clay interaction. The degree of smectite alteration and changes in the microbial diversity depended largely on the respective bentonite and the experimental conditions. Thus, the low charged SD80 with 17% tetrahedral charge showed nearly no structural change in either of the aqueous solutions, whereas B36 as a medium charged smectite with 56% tetrahedral charge became more beidellitic with increasing temperature when reacted in the diluted cap rock solution. Based on these experiments, the alteration of the smectite is mainly attributed to the nature of the bentonite, pore water chemistry and temperature. A significant microbial influence on the here analyzed parameters was not observed within the two years of experimentation. However, as the detected genera are known to potentially influence geochemical processes, microbial-driven alteration occurring over longer time periods cannot be ruled out if organic nutrients are available at appropriate concentrations. Full article

⁷⁹Se is a critical radionuclide concerning the safety of deep geological disposal of certain radioactive wastes in clay-rich formations. To study the fate of selenium oxyanions in clayey rocks in the presence of a selenium reducing microbial community, in situ tests were performed in the Opalinus Clay at the Mont Terri Rock Laboratory (Switzerland). Furthermore, biotic and abiotic batch tests were performed to assess Se(VI) and Se(IV) reactivity in the presence of Opalinus Clay and/or stainless steel, in order to support the interpretation of the in situ tests. Geochemical modeling was applied to simulate Se(VI) reduction, Se(IV) sorption and solubility, and diffusion processes. This study shows that microbial activity is required to transform Se(VI) into more reduced and sorbing Se species in the Opalinus Clay, while in abiotic conditions, Se(VI) remains unreactive. On the other hand, Se(IV) can be reduced by microorganisms but can also sorb in the presence of clay without microorganisms. In situ microbial reduction of Se oxyanions can occur with electron donors provided by the clay itself. If microorganisms would be active in the clay surrounding a disposal facility, microbial reduction of leached Se could thus contribute to the overall retention of Se in clayey host rocks. Full article

Strong chemical gradients between clay and concrete porewater lead to diffusive transport across the interface and subsequent mineral reactions in both materials. These reactions may influence clay properties such as swelling behaviour, permeability or radionuclide retention, which are relevant for the safety of a radioactive waste repository. Different cement types lead to different interactions with Opalinus Clay (OPA), which must be understood to choose the most suitable material. The consideration of anion-depleted porosity due to electrostatic repulsion in clay modelling substantially influences overall diffusive transport and pore clogging at interfaces. The identical dual porosity model approach previously used to predict interaction between Portland cement and OPA is now applied to low-alkali cement—OPA interaction. The predictions are compared with corresponding samples from the cement-clay interaction (CI) experiment in the Mont Terri underground rock laboratory (Switzerland). Predicted decalcification of the cement at the interface (depletion of C–S–H and absence of ettringite within 1 mm from the interface), the Mg enrichment in clay and cement close to the interface (neoformation of up to 17 vol% Mg hydroxides in concrete, and up to 6 vol% in OPA within 0.6 mm at the interface), and the slightly increased S content in the cement 3–4 mm away from the interface qualitatively match the sample characterisation. Simulations of Portland cement—OPA interaction indicate a weaker chemical disturbance over a larger distance compared with low-pH cement—OPA. In the latter case, local changes in porosity are stronger and lead to predicted pore clogging. Full article

The cement–clay interaction (CI) experiment was carried out at the Mont Terri rock laboratory to complement the current knowledge on the influence that cementitious materials have on Opalinus Clay (OPA) and bentonite (MX). Drill cores including the interface of OPA, concrete (LAC = low-alkali binder, and OPC = ordinary Portland cement), and MX, which interacted for 4.9 and 10 years, were successfully retrieved after drilling, and detailed analyses were performed to evaluate potential mineralogical changes. The saturated compacted bentonites in core samples were divided into ten slices, profiling bentonite in the direction towards the interface, to evaluate the extent and spatial variation of the mineralogical alteration of bentonite. Regarding the mineral compositions of bentonite, cristobalite was dissolved within a range of 10 mm from the interface in both LAC-MX and OPC-MX, while calcite precipitated near the interface for OPC-MX. In LAC-MX and OPC-MX, secondary products containing Mg (e.g., M-S-H) also precipitated within 20 mm of the interface. These alterations of bentonite developed during the first 4.9 years, with very limited progress observed for the subsequent 5 years. Detectable changes in the mineralogical nature of montmorillonite (i.e., the formation of illite or beidellite, increase in layer charge) did not occur during the 10 years of interaction. Full article

Multi-component (MC) diffusion simulations enable a process based and more precise approach to calculate transport and sorption compared to the commonly used single-component (SC) models following Fick’s law. The MC approach takes into account the interaction of chemical species in the porewater with the diffuse double layer (DDL) adhering clay mineral surfaces. We studied the shaly, sandy and carbonate-rich facies of the Opalinus Clay. High clay contents dominate diffusion and sorption of uranium. The MC simulations show shorter diffusion lengths than the SC models due to anion exclusion from the DDL. This hampers diffusion of the predominant species $CaU{O}_2{\left(C{O}_3\right)}_3^{2-}$. On the one side, species concentrations and ionic strengths of the porewater and on the other side surface charge of the clay minerals control the composition and behaviour of the DDL. For some instances, it amplifies the diffusion of uranium. We developed a workflow to transfer computationally intensive MC simulations to SC models via calibrated effective diffusion and distribution coefficients. Simulations for one million years depict maximum uranium diffusion lengths between 10 m and 35 m. With respect to the minimum requirement of a thickness of 100 m, the Opalinus Clay seems to be a suitable host rock for nuclear waste repositories. Full article