To ensure the safety of disposal facilities for radioactive waste, it is essential to quantitatively evaluate the performance of the waste disposal facilities by using safety assessment models. This paper addresses the development of the safety assessment model for the underground silo of Wolseong Low-and Immediate-Level Waste (LILW) disposal facility in Korea. As the simulated result, the nuclides diffused from the waste were kept inside the silo without the leakage of those while the integrity of the concrete is maintained. After the degradation of concrete, radionuclides migrate in the same direction as the groundwater flow by mainly advection mechanism. The release of radionuclides has a positive linear relationship with a half-life in the range of medium half-life. Additionally, the solidified waste form delays and reduces the migration of radionuclides through the interaction between the nuclides and the solidified medium. Herein, the phenomenon of this delay was implemented with the mass transfer coefficient of the flux node at numerical modeling. The solidification effects, which are delaying and reducing the leakage of nuclides, were maintained the integrity of the nuclides. This effect was decreased by increasing the half-life and the mass transfer coefficient of radionuclides.

The permanent disposal of discharged spent nuclear fuel (SNF) and contaminated radioactive waste generated from the subsequent chemical treatments of SNF has become a serious pending issue in many countries that operate the nuclear power plants. Among the diverse engineering solutions proposed for the disposal of high-level radioactive waste (HLW), deep geological disposal (DGD) has been considered as the most proven and safe option to prevent any significant release of radionuclides into the biosphere and to predictably ensure the long-term performance of disposal system. The DGD system consists of multiple structural components; the bentonite clay-based buffer and tunnel backfills are designed to perform the primary hydrogeochemical functions of 1) inhibiting the ingress of groundwater and reactive substances that could compromise the integrity of canister and 2) retarding the migration of released radionuclides into biosphere by providing the sufficient chemisorption sites. Montmorillonite, which is a 2:1 phyllosilicate mineral belonging to smectite group, constitutes the majority of bentonite, and it mainly predominate the swelling and chemisorption capacities of the clay material. Thus, it is essentially required to thoroughly understand the chemical interactions of major radionuclides and other important substances with montmorillonite in advance to accurately evaluate the long-term retention performance of engineered barriers and to reduce the uncertainties in the safety assessment of a deep geological repository (DGR) ultimately. Thus far, sorption of dissolved species onto mineral adsorbents has been generally described and quantified using the simple sorption-desorption distribution coefficient (Kd) concept; since any specific reaction mechanisms are not considered and reflected in the Kd concept, an empirical Kd value is intrinsically dependent on the aqueous conditions under which it was measured. In this framework, substantial scientific efforts have been made to develop a robust basis for geochemically parametrizing the sorption phenomena more reliably, and the application of thermodynamic sorption modeling (TSM), which is based on the chemical principle of mass action laws, has been studied with the aim of improving overall confidence in the description of radionuclide migration under a wide range of aquatic conditions. The disposal performance demonstration R&D division of KAERI introduced a new reference Ca-bentonite clay called Bentonil-WRK (Clariant Korea) for HLW disposal research in 2021 as the domestic Ca-bentonite sources have being depleted. We successfully separated and purified Ca-montmorillonite from the Bentonil-WRK clay, and its geochemical characteristics were meticulously studied by means of XRD, BET, CEC, FT-IR analyses and controlled acid-base titration. In this work, chemical sorption behaviors of aqueous iodide and benzoate, which are a major fission product in HLW and a model ligand of complex natural organic matters present in the deep geological environment, onto the purified Camontmorillonite were assessed under ambient conditions of S/L = 5 g/L, I = 0.01 M CaCl2, pH = 4- 9, pCO2 = 10-3.4 atm, and T = 25°C. Further, their unique adsorption envelopes and corresponding thermodynamic reaction constants refined from the diffuse double layer model (DDLM)-based inverse modeling of experimental sorption data were discussed.

The safe disposal of high-level radioactive waste (HLW), including the discharged spent nuclear fuel (SNF) and contaminated by-products produced from relevant chemical treatments, has become a serious pending problem for numerous countries that operate the nuclear power plants. The deep geological disposal (DGD) has thus far been considered the most proven and viable solution for isolation of the HLW and preventing any significant release of radionuclides into the biosphere. The DGD system consists of the multiple engineered and natural barrier components. Among them, the montmorillonite-based buffer and tunnel backfills are designed to perform the two major geochemical functions: 1) preventing the ingress of groundwater and any chemicals that compromise the safety of waste canister and 2) retarding the migration of released radionuclides by providing sufficient chemisorption sites. Therefore, it is essential to investigate the sorption mechanism of radionuclides onto montmorillonite and develop a thermodynamic reaction model in advance in order to accurately predict the long-term performance of engineered barriers and to reduce the uncertainties in the safety assessment of a deep geological repository (DGR) ultimately; thus far, sorption of chemical species onto mineral adsorbents has been widely described based on the concept of sorption-desorption distribution coefficient (Kd), the value of which is intrinsically conditional, and active scientific efforts have been made to develop robust thermodynamic sorption models which offer the potential to improve confidence in demonstration of radionuclide migration under a wide range of geochemical conditions. The natural montmorillonites are generally classified into Na-type or Ca-type according to its exchangeable cation, and the Ca-montmorillonite containing clays are being considered as candidate materials for the engineered barriers of DGR in several countries; they generally have advantages of higher thermal conductivity and lower price than the Na-montmorillonite based clays, but their sorption capacities are still comparable. In this framework, we aimed to investigate the chemical interactions of Ca-montmorillonite with selenite [Se(IV)], which is a major oxyanionic species in terms of HLW disposal, and develop a reliable thermodynamic sorption model (TSM). The present work summarizes the characterization of Ca-montmorillonite separated from the newly adopted reference bentonite (Bentonil-WRK) by means of XRD, BET, FTIR, CEC measurement, and acid-base titration. Further, its sorption behaviors with aqueous selenite species under aqueous conditions of S/L = 5 g/L, I = 0.01-0.1 m CaCl2, pH = 4.5-8.5, pCO2 = 10-3.5 atm, and T = 25°C were examined, and the resulting thermodynamic data are discussed as well.

The fundamental characteristics of groundwater colloids, such as composition, concentration, size, and stability, were analyzed using granitic groundwater samples taken from the KAERI Underground Research Tunnel (KURT) site by such analytical methods as inductively coupled plasma-mass spectrometry, field emission-transmission electron microscopy, a liquid chromatography-organic carbon detector, and dynamic light scattering technique. The results show that the KURT groundwater colloids are mainly composed of clay minerals, calcite, metal (Fe) oxide, and organic matter. The size and concentration of the groundwater colloids were 10–250 nm and 33–64 μg·L−1, respectively. These values are similar to those from other studies performed in granitic groundwater. The groundwater colloids were found to be moderately stable under the groundwater conditions of the KURT site. Consequently, the groundwater colloids in the fractured granite system of the KURT site can form stable radiocolloids and increase the mobility of radionuclides if they associate with radionuclides released from a radioactive waste repository. The results provide basic data for evaluating the effects of groundwater colloids on radionuclide migration in fractured granite rock, which is necessary for the safety assessment of a high-level radioactive waste repository.

The chelating agent and cellulose generated during the operating and decommissioning of a NPP’s form organic complexing compounds. That is accelerate the migration of radionuclide and have a bad influence of LILW disposal site. In this study, the GoldSim (RT module) program was used for the effects of radionuclide migration by organic complex compounds as described above. A scenario was derived for evaluation, and a conceptual design (Concept Art) of the GoldSim model was performed. 1) Derivation of the scenario. For the scenario, we selected a groundwater flow scenario in which groundwater flows in and radionuclides flow out after a lapse of time after the operation of the LILW disposal site in Gyeongju is closed. The inflowing groundwater comes into contact with radioactive waste and the radionuclides dissolve. The dissolved nuclides move past the drum and out of the disposal vessel due to the advection phenomenon. Radionuclides spilled from the disposal vessel pass through the silo internal filler (crushed stone) and reach the engineering barrier concrete. Radionuclides from degraded concrete are scenarios that move along the flow of groundwater to the near and far. 2) Radionuclide migration concept design. The radionuclide movement section was largely designed with Inner (Inside the silo), Near and Far. (A) Inner (Inside the silo) This section is where radionuclides move from the radiation source to the engineering barrier (silo). The detailed migration path was designed to allow radioactive nuclides to flow out and move to waste drums, solidified matrix of indrum, disposal vessel fillers, disposal vessels, silo fillers (crushed stones), and engineered barriers (concrete). The LILW disposal site in Gyeongju has a total of 6 silos. Each of the 6 silos was modeled and designed in consideration of the structural information and positional impact. (B) Near & Far. In generally design, the near is form source term to engineered barrier and far is beyond the engineered barrier. In this study, the near and far designed by radionuclide in the section from the beyond the engineering barrier (silo) to the sea through the groundwater flow through the natural rock. Especially in the case of near, the design was made by applying the position of the natural rock sampling drill hole.

A deep geological disposal system, which consists of the engineered and natural barrier components, is the most proven and widely adopted concept for a permanent disposal of the high level radioactive waste (HLW) thus far. The clay-based engineered barrier is designed to not only absorb mechanical stress caused by the geological activities, but also prevent inflow of groundwater to canister and outflow of radionuclides by providing abundant sorption sites. The principal mineralogical constituent of the clay material is montmorillonite, which is a 2:1 phyllosilicate having two tetrahedral sheets of SiO2 sandwiching an octahedral sheet of Al2O3. The stacking of SiO2 and Al2O3 sheets form the layered structures, and ion-exchange and water uptake reactions occur in the interlayer space. In order to reliably assess the radionuclide retention capacity of engineered barrier under wide geochemical conditions relevant to the geological disposal environments, sorption mechanisms between montmorillonite and radionuclides should be explicitly investigated in advance. Thus far, sorption behavior of mineral adsorbents with radionuclides has been quantified by the sorption-desorption distribution coefficient (Kd), which is simply defined as the ratio of radionuclide concentration in the solid phase to that in the equilibrium solution; the Kd value is conditional, and there have been scientific efforts to develop geochemically robust bases for parameterizing the sorption phenomena more reliably. In this framework, application of thermodynamic sorption model (TSM), which is theoretically based on the concept of widely accepted equilibrium models for aquatic chemistry, offers the potential to improve confidence in demonstration of radionuclide sorption reactions on the mineral adsorbents. Specifically, it is generally regarded in the TSM that coordination of radionuclides on montmorillonite takes place at the surficial aluminol and silanol groups while their ion-exchange reactions occur in the interlayer space also. The effects of electrical charge on the surface reactions are additionally corrected in accordance with the numerous theories of electrochemical interface. The present work provides an overview of the current status of application of TSM for quantifying sorption behaviors of radionuclides on montmorillonite and experimental results for physical separation and characterization of Ca-montmorillonite from the newly adopted reference bentonite (Bentonil- WRK) by means of XRD, BET, FTIR, CEC measurement, and acid-base titration. The determined mineralogical and chemical properties of the montmorillonite obtained will be used as input parameters for further sorption studies of radionuclides with the Bentonil-WRK montmorillonite.

본 연구에서는 KURT (KAERI 지하처분연구시설)를 포함한 지하연구시설에서 핵종 및 콜로이드 이동에 대 한 연구현황을 조사하였다. 화강암과 같은 결정질 암반층에 건설된 해외 지하연구시설들을 간략하게 소개하 고 비교하였다. 특히 Grimsel Test Site (GTS)와 ¨Asp¨o Hard Rock Laboratory에서의 핵종 및 콜로이드 이동연 구에 대한 주요 국제공동연구의 연구항목 및 내용, 진행중인 연구 프로젝트, 연구계획 등에 대해 조사하였다