Understanding the long-term geochemical evolution of engineered barrier system is crucial for conducting safety assessment in high-level radioactive waste disposal repository. One critical scenario to consider is the intrusion of seawater into the engineered barrier system, which may occur due to global sea level rise. Seawater is characterized by its high ionic strength and abundant dissolved cations, including Na, K, and Mg. When seawater infiltrates an engineered barrier, such dissolved cations displace interlayer cations within the montmorillonite and affect to precipitation/ dissolution of accessory minerals in bentonite buffer. These geochemical reactions change the porewater chemistry of bentonite buffer and influence the reactive transport of radionuclides when it leaked from the canister. In this study, the adaptive process-based total system performance assessment framework (APro), developed by the Korea Atomic Energy Research Institute, was utilized to simulate the geochemical evolution of engineered barrier system resulting from seawater intrusion. Here, the APro simulated the geochemical evolution in bentonite porewater and mineral composition by considering various geochemical reactions such as mineral precipitation/dissolution, temperature, redox processes, cation exchange, and surface complexation mechanisms. The simulation results showed that the seawater intrusion led to the dissolution of gypsum and partial precipitation of calcite, dolomite, and siderite within the engineered barrier system. Additionally, the composition of interlayer cation in montmorillonite was changed, with an increase in Na, K, and Mg and a decrease in Ca, because the concentrations of Na, K, and Mg in seawater were 2-10 times higher than those in the initial bentonite porewater. Further studies will evaluate the geochemical sorption and transport of leaked uranium-238 and iodine-129 by applying TDB-based sorption model.
In the engineered barrier system of deep geological disposal repository, complex physicochemical phenomena occur throughout the entire disposal time, consequently impacting the safety function. The bentonite buffer, a significant component of the engineered barrier system, can be geochemically altered due to the changes in host rock groundwater, temperature, and redox condition. Such changes may have direct or indirect effects on radionuclide migration in case of canister failure. Therefore, a modeling tool that accounts for coupled thermal-hydraulic-mechanical-chemical (THMC) processes is necessary for the safety assessment. To this end, the Korea Atomic Energy Research Institute (KAERI) has developed the APro, a modeling interface for conducting safety assessment of deep geological disposal repository. The APro considers coupled THMC processes that influence radionuclide migration. Here, the solute transport considering thermal and hydraulic processes are calculated using the COMSOL multi-physics, while geochemical reactions are carried out in PHREEQC. The two software are coupled using a sequential non-iterative operator splitting approach, and transport of non-water H, non-water O, and charge were additionally considered to enhance the coupling model stability. Finally, the applicability of APro to simulate long-term geochemical evolution of bentonite was demonstrated through benchmark studies to evaluate the effects of mineral precipitation/dissolution, temperature, redox, and seawater intrusion.
The reaction path of water-gneiss in 200m borehole at the Soorichi site of Yugu Myeon, Chungnam was simulated by the EQ3NR/EQ6 program. Mineral composition of borehole core and fracture-filling minerals, and chemical composition of groundwater was published by authors. In this study, chemical evolution of groundwater and formation of secondary minerals in water-gneiss system was modelled on the basis of published results. The surface water was used as a starting solution for reaction. Input parameters for modelling such as mineral assemblage and their volume percent, chemical composition of mineral phases, water/rock ratio reactive surface area, dissolution rates of mineral phases were determined by experimental measurement and model fit. EQ6 modelling of the reaction path in water-gneiss system has been carried out by a flow-centered flow through open system which can be considered as a suitable option for fracture flow of groundwater. The modelling results show that reaction time of 133 years is required to reach equilibrium state in water-gneiss system, and evolution of present groundwater will continue to pH 9.45 and higher na ion concentration. The secondary minerals formed from equeous phase are kaolinite, smectite, saponite, muscovite, mesolite, celadonite, microcline and calcite with uincreasing time. Modeling results are comparatively well fitted to pH and chemical composition of borehole groudwater, secondary minerals identified and tritium age of groundwater. The EQ6 modelling results are dependent on reliability of input parameters: water-rock ratio, effective reaction surface area and dissolution rates of mineral phases, which are difficult parameters to be measured.