A disposal system for spent nuclear fuel mainly divides into two parts; Engineered barriers include spent nuclear fuel, canister, buffer and backfill and natural barriers mean a host rock surrounding engineered barriers. If radionuclides released from a repository, they can migrate to the ecosystem. Sorption plays an important role in retarding the migration of released radionuclides. Hence, the safety assessment for the disposal of a spent nuclear fuel should consider the migration and retardation of radionuclides in geosphere. Distribution coefficient is one of input parameters for the safety assessment. In this work, distribution coefficients for crystalline rock as a natural barrier were collected and evaluated for the purpose of safety assessment for the deep geological disposal of a spent nuclear fuel. The radionuclides considered in this work are as follows; alkali and alkaline earth metals (Cs, Sr, Ba), lanthanides (Sm), actinides (Ac, Am, Cm, Np, Pa, Pu, Th U), transition elements (Nb, Ni, Pd, Tc, Zr), and others (C, Cl, I, Rn, Se, Sn). The sorption of radionuclides is influenced by various geochemical conditions such as pH/carbonates, redox potential, ionic strength, radionuclide concentration, kinds and amounts of minerals, and microbes. For the evaluation of distribution coefficients, the data from Sweden (SKB), Finland (Posiva), Switzerland (Nagra), and Japan (JAEA) were collected, analyzed, and the recommended distribution coefficients have been suggested.

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.

With the increase of temporarily-stored spent radioactive fuels, there is an increasing necessity for the safe disposal of high-level radioactive waste (HLW). Among various methods for the disposal of HLW, a deep geological disposal system is adapted as a HLW disposal strategy in many countries. Before the construction of a repository in deep geological condition, a performance assessment, which means the use of numerical models to simulate the long-term behavior of a multi-barrier system in HLW repository, has been widely performed to ensure the isolation of radionuclides from human and related environments for more than a million years. Meanwhile, Korea Atomic Energy Research Institute (KAERI) is developing a process-based total system performance assessment framework for a geological disposal system (APro). To improve the reliability of APro, KAERI is participating in DECOVALEX-2023 Task F, which is the international joint program for the comparison of the models and methods used in deep geological performance assessment. As a final goal of Task F, the reference case for a generic repository in fractured crystalline rock is described. The three-dimensional generic repository is located in a domain of 5 km in length, 2 km in width, and 1 km in depth, and contains an engineering barrier system with 2,500 deposition holes in fractured crystalline rock. In this study, a numerical simulation of the reference case is performed with COMSOL Multiphysics as a part of Task F. The fractured crystalline rock is described with the discrete fracture matrix (DFM) model, which expresses major deterministic fractures explicitly in the domain and minor stochastic fractures implicitly with upscaled quantities. As an output of the numerical simulation, fluid flow at steady-state and radionuclide transport are evaluated for ~106 years. The result shows that fractures dominate the transport of radionuclides due to much higher hydraulic properties than rock matrix. The numerical modeling approaches used in this study are expected to provide a basis for performance assessment of nuclear waste disposal repository located in fractured crystalline rock.

The deep geological repository consisting of a multi-barrier system (engineered and natural barriers) is generally designed to isolate the high-level radioactive waste. The natural barrier is outermost portion to secure safety of the disposal. Crystalline rocks are considered for potential geological repository media to retard and inhibit the migration of radionuclides when the radionuclides leak from the canister and break through the engineered barrier. Sorption and diffusion processes play a major role in retardation of the radionuclides in deep underground environment. In order to evaluate the migration of radionuclides in the safety assessment or geochemical modelling, distribution coefficient and diffusivity of radionuclides are required as input data. In this study, we performed mineralogical and geochemical analysis for a crystalline rock (e.g., granite) to use the sorption and diffusion experiment. The fresh rock samples are obtained from a deep core samples (DB-2) drilled up to 1 km from the surface at KURT (KAERI Underground Research Tunnel) site. For the optical and microscopic examination, thin sections of the rock sample were provided. The rock samples were crushed into powder size to analyze major and trace elements of the whole-rock aliquots. The powdered specimens also used for mineral identification and measurement of specific surface area. The major constituent minerals of the granite are plagioclase, quartz, and K-feldspar and the minor minerals are phlogopite, biotite, and chlorite. According to the results of geochemical analysis, the granite specimens generally contain more than 70wt% of SiO2 and 8wt% of total alkali oxides (Na2O + K2O). The trace elements normalized to primitive mantle compositions show positive Cs, Rb, U, K, and Pb anomalies and negative Nb and Ti anomalies. The rock samples have an average density of 2.62 g·cm−3 and an average porosity of 0.222%. The crushed samples represent the specific surface area of 0.2087 m2·g−1 for the 75–150 μm fraction and 0.1616 m2·g−1 for the 150–300 μm fraction by BET method, respectively. The granite specimens will be used for the sorption and diffusion experiments to evaluate the radionuclides’ geochemical behaviors. The mineralogical and geochemical properties provided in this study can be useful in understanding the sorption and diffusion processes of significant radionuclides under the geological disposal environments.

The pH dependence of sorption distribution coefficient (Kd) of Np(IV) on MX-80 in Ca-Na-Cl type solution with the ionic strength of 0.3 M, which was similar to one of the reference groundwaters in crystalline rock, was experimentally investigated under the reducing conditions. The overall trend of Kd on MX-80 was independent of pH at 5 ≤ pH ≤ 10 but increased as pH increased at pH ≤ 5. The 2-site protolysis non-electrostatic surface complexation and cation exchange model was applied to the experimentally measured pH dependence of Kd and the optimized surface complexation constants of Np(IV) sorption on MX-80 were estimated. The values of surface complexation constants in this work agreed relatively well with those in the Na-Ca-Cl solution previously evaluated, suggesting that compared to Na+, the competition of Ca2+ with Np(IV) for surface complexation on MX-80 was not much strong in Ca-Na-Cl solution. The sorption model well predicted the pH dependence of Kd values but slightly overestimated the sorption at the low pH region.