Deep disposal facility for High-Level radioactive Waste (HLW) uses a multi-barrier system to prevent the leakage of radionuclide. As a part of the engineered barrier, bentonite is primarily considered as the main buffering material. This is due to the adsorption and swelling properties of the bentonite, which are expected to effectively impede leakage of the radionuclide. In many cases, adsorption is generally regarded as occurring only within the buffer zone. However, several research has been conducted to explore the possibility of bentonite intrusion into the Excavation- Damaged Zone (EDZ) generated during excavation processes, because of the swelling properties of the bentonite. Generally, for host rock near the deep disposal facility such as granite, groundwater flows through the fracture network. Therefore, analysis of the characteristics of the fracture network is essential for predicting the behavior of radionuclide in groundwater. Accordingly, the bentonite intrusion into the fracture network is critical for safety assessment of the deep disposal facility. To analyze this, hydro-geochemical model was established utilizing COMSOL Multiphysics and PHREEQC, observing changes of the behavior of U (VI) along fracture network due to the swelling of bentonite. Modeling was conducted with progressively changing intrusion depth of the bentonite. According to the results, the behavior of U (VI) exhibited significant changes depending on the connectivity of the fractures. Based on the distribution characteristics of the fracture network, heterogeneous groundwater flow was observed. U (VI) was transported through the preferential pathway, which indicates high connectivity, due to the rapid groundwater flow. Notably, when changing the intrusion depth of bentonite, significant differences in behavior of U (VI) were observed in the 0-20 cm case. In contrast, as the intrusion depth increased, it was observed that differences became less evident. These results indicate that changes in the properties of fracture network in EDZ due to the swelling of bentonite significantly influence the behavior of U (VI).

The effect of various physicochemical processes, such as seawater intrusion, on the performance of the engineered barrier should be closely analyzed to precisely assess the safety of high-level radioactive waste repository. In order to evaluate the impact of such processes on the performance of the engineered barrier, a thermal-hydrological-chemical model was developed by using COMSOL Multiphysics and PHREEQC. The coupling of two software was achieved through the application of a sequential non-iterative approach. Model verification was executed through a comparative analysis between the outcomes derived from the developed model and those obtained in prior investigations. Two data were in a good agreement, demonstrating the model is capable of simulating aqueous speciation, adsorption, precipitation, and dissolution. Using the developed model, the geochemical evolution of bentonite buffer under a general condition was simulated as a base case. The model domain consists of 0.5 m of bentonite and 49.5 m of granite. The uraninite (UO2) was assigned at the canister-bentonite interface as the potential source of uranium. Assuming the lifetime of canister as 1,000 years, the porewater mixing without uranium leakage was simulated for 1,000 years. After then, the uranium leakage through the dissolution of uraninite was initiated and simulated for additional 1,000 years. In the base case model, where the porewater mixing between the bentonite and granite was the only considered process, the gypsum tended to dissolve throughout the bentonite, while it precipitated in the vicinity of bentonite-granite boundary. However, the precipitation and dissolution of gypsum only showed a limited effect on the performance of the bentonite. Due to the low solubility of uraninite in the reduced environment, only infinitesimal amounts of uranium dissolved and transported through the bentonite. Additional cases considering various environmental processes, such as seawater or cement porewater intrusion, will be further investigated.

The analysis of uranium migration is crucial for the accurate safety assessment of high-level radioactive waste (HLW) repository. Previous studies showed that the migration of the uranium can be affected by various physical and chemical processes, such as groundwater flow, heat transfer, sorption/ desorption and, precipitation/dissolution. Therefore, a coupled Thermal-Hydrological-Chemical (THC) model is required to accurately simulate the uranium migration near the HLW repository. In this study, COMSOL-PHREEQC coupled model was used to simulate the uranium migration. In the model, groundwater flow, heat transfer, and non-reactive solute transport were calculated by COMSOL, and geo-chemical reaction was calculated by PHREEQC. Sorption was primarily considered as geo-chemical reaction in the model, using the concept of two-site protolysis nonelctrostatic surface complexation and cation exchange (2 SP NE SC/CE). A modified operator splitting method was used to couple the results of COMSOL and PHREEQC. Three benchmarks were done to assess the accuracy of the model: 1) 1D transport and cation exchange model, 2) cesium transport in the column experiment done by Steefel et al. (2002), and 3) the batch sorption experiment done by Fernandes et al. (2012), and Bradbury and Baeyens (2009). Three benchmark results showed reliable matching with results from the previous studies. After the validation, uranium 1D transport simulation on arbitrary porewater condition was conducted. From the results, the evolution of the uranium front with sequentially saturating sites was observed. Due to the limitation of operator splitting method, time step effect was observed, which caused the uranium to sorbed at further sites then it should. For further study, 3 main tasks were proposed. First, precipitation/ dissolution will be added to the reaction part. Second, multiphase flow will be considered instead of single phase Darcy flow. Last, the effect of redox potential will be considered.

Montmorillonite plays a key role in engineered barrier systems in the high-level radioactive waste repository because of its large sorption capacity and high swelling pressure. However, the sorption capacity of montmorillonite can be largely varied dependent on the surrounding environments. This study conducted the batch simulation for U(VI) sorption on Na-montmorillonite by utilizing the cation exchange and surface complexation coupled (2SP-NE-SC/CE) model and evaluated the effects of physicochemical properties (i.e., pH, temperature, competing cations, U(VI) concentration, and carbonate species) on U(VI) sorption. The simulation demonstrated that the U(VI) sorption was affected by physicochemical properties: the pH and temperature relate to aqueous U(VI) speciation, the competing cations relate to the cation exchange process and selectivity, the U(VI) concentration relates to saturation at sorption sites. For example, the Kd (L kg−1) of Na-montmorillonite represented the largest values of 2.7×105 L kg−1 at neutral pH condition and had significantly decreased at acidic pH<3, showing non-linear and diverse U(VI) sorption at the ranged pH from 2 to 11. Additionally, the U(VI) sorption on montmorillonite significantly decreased in presence of carbonate species. The U(VI) sorption for long-term in actual porewater chemistry and temperature of high-level radioactive waste repository represented that the sorption capacity of Na-montmorillonite was affected by various external properties such as concentration of competing cation, temperature, pH, and carbonate species. These results indicate that geochemical sorption capacity of bentonite should be evaluated by considering both geological and aquifer environments in the high-level radioactive waste repository.

The design of the high-level radioactive waste (HLW) repository is made for isolating the HLW from the groundwater system by using artificial and natural barriers. Granite is usually considered to be a great natural barrier for the HLW repository in various countries including Sweden, Canada, and Korea due to its low hydraulic permeability. However, many fractures that can act as conduits for groundwater and radionuclides exist in granite. Furthermore, the decay heat generated by the HLW can induce groundwater acceleration through the fracture. Since the direction, magnitude, and lasting time of the heat-induced groundwater flow can be differed depending on the fracture geometry, the effect of fracture geometry on the groundwater flow around the repository should be carefully analyzed. In this study, groundwater models were conducted with various fracture geometries to quantify the effect of various properties of fractures (or fracture networks) on the heat-induced groundwater flow. In all models, the pressure around the repository only lasted for a short period after it peaked at 0.1 years. In contrast, the temperature lasted for 10,000 years after the disposal inducing the convective groundwater flow. Single fracture models with different orientations were conducted to evaluate the variations in groundwater velocities around the repository depending on the fracture slope. According to the results, the groundwater velocity on the fracture was the fastest when the regional groundwater flow direction and the fracture direction coincided. In double fracture models, various inclined fractures were added to the horizontal fracture. Due to the intersecting, the groundwater flow velocity showed a discontinuous change at the intersecting point. Lastly, the discrete fracture network models were conducted with different fracture densities, length distributions, and orientations. According to the modeling results, the groundwater flow was significantly accelerated when the fracture network density increased, or the average fracture length increased. However, the effect of the fracture orientation was not significant compared to the other two network properties.

Multiple sorptive sites on natural illitic clays (e.g., frayed edge [FES], type II [TS], and planar sites [PS]) play an important role to diverse 137Cs immobilization in soil and aquifer environments. This study investigated the Cs sorption capabilities of 10 natural illitic clays at ranged Cs concentrations (1 ×10−7 to 1×10−3 mol·L−1) under various competing potassium concentration (distilled water to 1×10−1 mol·L−1). Additionally, multisite cation exchange model was performed to evaluate the best-fit sorption model and optimize the sorption capacities and affinities of multiple sorptive sites for Cs. Here, the experimental Cs sorption isotherms varied among 10 illtic clays, indicating different sorption capacities of Cs on illitic clays. The best-fit sorption model exhibited that variable Cs sorption of 10 illitic clays was significantly related to the sorption capacities at the FES (1.76 × 10−5 to 1.12×10−4 eq·kg−1), TS (1.59×10−3 to 9.76×10−3 eq·kg−1), and PS (2.14×10−2 to 1.51×10−1 eq·kg−1), respectively. The FES predominantly contributed to Cs sorption at low aqueous concentrations, whereas the TS and PS sorbed Cs at high concentrations. These sorption capabilities of multiple sorptive sites were correlated to illite contents and crystallinity of illitic clays, implicating that such parameters could be key factors to predict the Cs sorption for natural illitic clays in soil and aquifer environments. Finally, 1-D transport simulations represented that the severe Cs retardation occurred at low Cs concentration, implying that the FES predominantly affected to Cs transport in actual radioactive contamination sites (i.e., where low Cs concentration prevails), compared to the TS and/or PS.