The design and fabrication of suitable waste forms with high thermal and structural stability are essential for the safe management and disposal of radioactive wastes. In particular, the thermal properties and temperature distribution of waste form containing high heat-generating nuclides such as Cs and Sr can be used to evaluate its thermal stability, but also provide useful information for the design of canisters, storage systems, and repositories. In this study, a new program code-based thermal analysis framework has been developed to facilitate the characterization, design, and optimization of the waste form. Matlab was used as a software development platform because it provides powerful mathematical computation and visualization components such as the partial differential equation (PDE) toolbox for solving heat transfer problems using finite element method, the App Designer for graphical user interface (GUI), and the MATLAB Compiler for sharing MATLAB programs as standalone applications and web applications. The thermal analysis results such as temperature distribution, heat flux, maximum/ minimum temperature, and centerline/surface temperature profile are visualized with graphs and tables. To evaluate the effectiveness of the developed program, several design and optimization studies were carried out for the SrTiO3 waste form, selected as a stable form of strontium nuclide.

The nuclide management process for reducing the environmental burden being developed by the Korea Atomic Energy Research Institute is performed in molten salts, resulting in contaminated salt wastes containing fission products such as Cs, Sr, Ba, and rare-earth nuclides. In addition, the spent fuel of a molten salt reactor (MSR) contains a variety of fission products, and a purification process may be required for the reuse of the salt and the separation and disposal of the fission products in the spent nuclear fuel. The melt-crystallization method is a technique used for the purification and separation of chemicals or metals based on the different melting points of the different substances. In a recent study, our group developed a reactive-crystallization method using Li2CO3 precipitation agent to precipitate metal corrosion from the reactor through a chlorination reaction by HCl and Cl2, which may occur in chloride molten salt, and successfully precipitated the metal precipitate and purified and recovered LiCl salt. In this study, reactive-crystallization method has been established for removing fission products and corrosive materials. Using the reactive crystallization method, white LiCl-KCl salt that was not discolored by metal corrosion was recovered through the crystallization plates, and fission products and metal elements were shown to be suppressed to several ppm in the purified salt. Consequently, high-purity salts were recovered with high nuclide and corrosive separation efficiencies. The reactive crystallization procedure can also be applied to other salt waste systems, such as MSR nuclear fuel treatment and molten salt chemistry for the elimination of corrosive substances.

Heat-generating nuclides such as Cs-137 and Sr-90 should be separated from spent nuclear fuel to reduce the short-term thermal load on the repository facility. In particular, Sr-90 must be separated because its decay process generates high temperatures. Recently, the Korea Atomic Energy Research Institute (KEARI) has been developing a waste burden minimization technology to reduce the environmental burden resulting from the disposal of spent nuclear fuel and maximize the utilization of the disposal facility. The technology incorporates a nuclide management process that maximizes disposal efficiency by selectively separating and accumulating key nuclides from spent nuclear fuel, such as Cs, Sr, I, TRU/RE, and Tc/Se. Sr nuclides dissolve in the chloride phase during the chlorination process of spent nuclear fuel and are recovered as carbonate or oxide through reactive distillation or reactive crystallization. Due to their chemical similarity, Ba nuclides are recovered along with Sr nuclides during this process. In this study, we prepared a ceramic waste form for group II nuclides, Ba(x)Sr(1-x)TiO3 (x=0, 0.25, 0.5, 0.75, 1), using the solid-state reaction method, taking into account the different ratios of Sr/Ba nuclides produced during the nuclide management process. Regardless of the Sr/Ba ratio, the established waste form fabrication process was able to produce a stable waste form. Physicochemical properties, including leaching and thermal properties, were evaluated to determine the stability of group II waste forms. In addition, the radiological properties of waste forms of Ba(x)Sr(1-x)TiO3 with varying Sr/Ba ratios were evaluated. These results provided fundamental data for the long-term storage and management of waste forms containing group II nuclides.

To minimize the short-term thermal load on the repository facility, heat generating nuclides such as Cs-137 and Sr-90 should be separated from the spent nuclear fuel for efficiency of repository facility. In particular, Sr-90 must be separated because it generates high heat during the decay process. Recently, Korea Atomic Energy Research Institute (KEARI) is developing a waste burden minimization technology to reduce the environmental burden caused by the disposal of spent nuclear fuel and maximize the utilization of the disposal facility. The technology includes a nuclide management process that can maximize disposal efficiency by selectively separating and collecting major nuclides such as Cs, Sr, I, TRU/RE, and Tc/Se from spent nuclear fuel. Among the major nuclides, Sr nuclides dissolve in chloride phase during the chlorination process of spent nuclear fuel and recovered in the form of carbonate or oxide via reactive distillation. In this process, Ba nuclides are also recovered along with Sr nuclides due to their chemical similarity. In this study, we prepared group II nuclide ceramic waste form, Ba(x)Sr(1-x)TiO3 (x=0, 0.25, 0.5, 0.75, 1), using the solid-state reaction method by considering the various ratio of Sr/Ba nuclides generated from nuclide management process. The established waste form fabrication process was able to produce a stable waste form regardless of the ratio of Sr/Ba nuclides. To evaluate the stability of group II waste form, physicochemical properties such as leaching and thermal properties were evaluated. Also, the radiological properties of the Ba(x)Sr(1-x)TiO3 waste forms with various Sr/Ba ratios were evaluated, and the estimation of centerline temperature was carried out using the experimental thermal property data. These results provided fundamental data for long-term storage and management of group II nuclides waste form.

To reduce the environmental burden caused by the disposal of spent nuclear fuel and maximize the utilization of the repository facility, waste burden minimization technology is currently being developed at the Korea Atomic Energy Research Institute (KEARI). The technology includes a nuclide management process that can maximize disposal efficiency by selectively separating and collecting major nuclides in spent nuclear fuel. In addition, for efficient storage facility utilization, the short-term decay heat generated by spent nuclear fuel must be removed from the waste stream. To minimize the short-term thermal load on the repository facility, it is necessary to separate heat generating nuclides such as Cs-137 and Sr-90 from the spent fuel. In particular, Sr-90 must be separated because it generates high heat during the decay process. KAERI has developed a technology for separating Sr nuclides from Group II nuclides separated through the nuclide management process. In this study, we prepared Sr ceramic waste form, SrTiO3, by using the solid-state reaction method for long-term storage for the decay of separated Sr nuclides and evaluated the physicochemical properties of the waste form. Also, the radiological and thermal characteristics of the Sr waste form were evaluated by predicting the composition of Sr nuclides separated through the nuclide management process, and the estimation of centerline temperature was carried out using the experimental thermal data and steady state conduction equation in a long and solid cylinder type waste form. These results provided fundamental data for long-term storage and management of Sr waste.

The fabrication of waste forms with high thermal and structural stability is an essential technology for the safe management and disposal of radioactive wastes. In particular, the thermal characteristics of waste forms containing high heat-generating nuclides such as Cs and Sr can be used for the optimized design of the waste form to secure its thermal safety, and they also provide basic design data for the safe management of canisters, storage systems, and repositories. The Korea Atomic Energy Research Institute is actively developing processes and equipment for fabricating various types of high-level wastes into a stable glass or ceramic waste form. In previous research related to the thermal analysis of the waste form, a relatively simple analysis was performed by using the analytic solution of the one-dimensional steady-state heat conduction equation considering the decay heat properties of the waste. As a specific application study, the optimized diameter of the cylindrical glass waste form was proposed by evaluating the centerline temperature of the waste form. In this study, we extended previous research by introducing a more complicated model, and the main results are summarized as follows. First, an analytical solution was derived by applying the temperaturedependent thermal conductivity expressed in the general form of polynomial function to the onedimensional heat conduction problem previously studied. Second, the two-dimensional axisymmetric steady-state heat conduction problem with a more realistic cylinder model with finite length was modeled and solved by using the finite element method via Matlab’s PDE (partial differential equation) toolbox. Third, thermal analysis was performed on the SrTiO3 waste form, selected as a stable form of strontium nuclide, using the developed analytical and numerical methods. The differences in the temperature distribution and computation time were evaluated through a comparative study of both solutions. Although the problem considered in this study could easily be solved by using commercial CFD software such as ANSYS or SolidWorks, a code-based program was developed to facilitate parametric design study in conjunction with optimization algorithms. The analysis results could be used to evaluate the thermal stability of waste form and to optimize the shape and size of the waste form in consideration of the design constraints of storage systems or repositories.