The mobility of radionuclides in the subsurface environment is governed by a interaction of radioactivity characteristics and geochemical conditions with adsorption reactions playing a critical role. This study investigates the characteristics and mechanisms of radionuclides adsorption on site media in viewpoint of nuclear safety, particularly focusing on the potential effect of seawater infiltration in coastal site near nuclear power plant. Seawater intrusion alters the chemistry in groundwater, including parameters such as pH, redox potential, and ionic strength, thereby affecting the behavior of radionuclides. To assess the safety of site near nuclear power plant and the environmental implications of nuclide leakage, this research conducted various experiments to evaluate the behavior of radionuclides in the subsurface environment. High distribution coefficients (50-2,500 ml/g) were observed at 10 mg/L Co, with montmorillonite > hydrobiotite > illite > kaolinite. It decreased with competing cations (Ca2+) and was found to decrease significantly by 90% with a decrease in pH to 4. It is believed that the adsorption capacity of cationic radionuclides decreases significantly as the clay mineral surface becomes less negatively charged. For Cs, the distribution coefficient (180-560 ml/g) was higher for montmorillonite > hydrobiotite > illite > kaolinite. Compared to Co, it was found to be less influenced by pH and more influenced by competing cations. For Sr, the distribution coefficient (100-380 ml/g) was higher in the order of hydrobiotite > montmorillonite > illite > kaolinite. Compared to Cs, it was found to be less affected by pH and also less affected by the effect of competing cations compared to Cs. Seawater samples from Gampo and Uljin site near Nuclear Power Plant in Korea were analyzed to determine their chemical composition, which was subsequently used in adsorption experiments. Additionally, the seawater-infiltrated groundwater was synthesized in laboratory according to previous literature. The study focused on the adsorption and behavior of three key radionuclides such as cesium, strontium, and cobalt onto four low permeability media (clay minerals) such as kaolinite, illite, hydrobiotite, and montmorillonite known for their high adsorption capacity at a site of nuclear power plant. At concentrations of 5 and 10 mg/L, the adsorption coefficients followed the order of cobalt > cesium > strontium for each radionuclide. Notably, the distribution coefficient (Kd) values exhibited higher values in seawater-infiltrated groundwater environments compared to seawater with relatively high ionic strength. Cobalt exhibited a substantial adsorption coefficient, with a marked decrease in Kd values in seawater conditions due to elevated ionic strength. In contrast, cesium displayed less dependency on seawater compared to other radionuclides, suggesting distinct adsorption mechanisms, possibly involving fractured edge sites (FES) in clay. Strontium exhibited a significant reduction in adsorption in seawater compared to groundwater in all Kd sorption experiments. The adsorption data of cobalt, cesium, and strontium on clay minerals in contact with seawater and seawater-infiltrated solutions offer valuable insights for assessing radioactive contamination of groundwater beneath coastal site near nuclear power plant sites. This research provides a foundation for enhancing the safety assessment protocols of nuclear power plant sites, considering the potential effects of seawater infiltration on radionuclide behavior in the subsurface environment.

The operation of nuclear facilities involves the potential for on-site contamination of soil, primarily resulting from pipe leaks and other operational incidents. Globally, decommissioning process for commercial nuclear power plants have revealed huge-amounts of soil waste contaminated with Cs-137, Sr-90, Co-60, and H-3. For example, Connecticut Yankee in the United States produced approximately 52,800 ton of contaminated soil waste, constituting 10% of the total waste generated during its decommissioning. Environmental remediation costs associated with nuclear decommissioning in the US averaged $60 million per unit, representing a significant 10% of the whole decommissioning expenses. Consequently, this study undertook a preliminary investigation to identify important factors for establishing a site remediation strategy based on radionuclide- and site-specific media- characteristics, focusing the efficiency enhancement for the environmental remediation. The factors considered for this investigation were categorized into physical/environmental, socioeconomic, technical, and management aspects. Physical/environmental factors contained the site characteristics, contamination levels, and environmental sensitivity, while socio-economic factors included the social concerns and economic costs. Technical and management factors included subcategories such as technical considerations, policy aspects, and management factors. Especially, technical factors were further subdivided to consider the site reuse potential, secondary waste generation by site remediation, remediation efficiency, and remediation time. Additionally, our study focused the key factors that facilitate the systematic planning for the site remediation, considering the distribution coefficient (Kd) and hydrogeological characteristics associated with each radionuclide in specific site conditions. Therefore, key factors in this study focus the geochemical characteristics of site media including the particle size distribution, chemical composition, organic and inorganic constituents, and soil moisture content. Moreover, the adsorption properties of site media were examined concerning the distribution coefficient (Kd) of radionuclides and their migration characteristics. Furthermore, this study supported the development of a conceptual framework, containing the remediation strategies that incorporate the mobility of radionuclides, according to the site-specific media. This conceptual framework would necessitate the spatial analysis techniques involving the whole contamination surveys and radionuclide mobility modeling data. By integrating these key factors, the study provides the selection and simulation of optimal remediation methods, ultimately offering the estimated amounts of radioactive waste and its disposal costs. Therefore, these key factors offer foundational insights for designing the site remediation strategies according the sitespecific information such as the distribution coefficient (Kd) and hydrogeological characteristics.

The development of separation method of radioactive tritium is imperative for treating tritiumcontaminated water originating from nuclear facilities. Polymer electrolyte membrane electrolysis technology represents a promising alternative to conventional alkaline electrolysis for tritium enrichment. Nevertheless, there has been limited research conducted thus far on the composition of membrane electrode assemblies (MEAs) specifically optimized for tritium separation, as well as the methods used for their fabrication. In this study, we conducted an investigation aimed at optimizing MEAs specifically tailored for tritium separation. Our approach involved the systematic variation of MEA components, including the anode, cathode, porous transport layer, and electrode formation method. The water electrolysis efficiency and the H/D separation factor in deuterated water (1%) were evaluated with respect to both the preparation method and the composition of the MEA. To assess the long-term stability of the MEAs, changes in cell voltage, resistance, and the active electrode area were analyzed using impedance analysis and cyclic voltammetry. Furthermore, we examined H/D separation factor both before and after degradation. The results showed that MEAs with different anode/cathode configurations and electrode formation methods improved the electrolysis efficiency compared to commercial MEAs. In addition, the degree of change in the resistance value was also different depending on the electrode formation method, indicating that the electrode formation method has a significant impact on the stability of the electrolysis system. Therefore, the study showed that the efficiency and long-term stability of the water electrolzer can be improved by optimizing the MEA fabrication method.

General phases in the plan and implementation of an environmental remediation of radioactively contaminated sites are planning for remediation, site characterization, remediation criteria, remediation strategy, implementing remediation actions, and conducting post-remediation activities. Environmental remediation should commence with a planning stage. It is helpful to prepare reports which detail all the supporting activities related to these elements before significant levels of funds and efforts are committed. Site characterization is needed to provide sufficient data to make strategic decisions on the environmental remediation activities. The source characterization should include both waste characterization and facility or site characterization and should provide reliable estimates of the release rates of radioactive constituents as well as constituent distribution. During the preliminary site characterization, an engineering study should be conducted to develop remediation options which address the specific contaminant problem and are aimed to reduce radiological and chemical exposure. Options will include engineering approaches and associated technologies. A preliminary selection of options may be made based on several factors including future sites use, technical considerations, public acceptability, cost, and regulatory requirements. The implementation of remediation actions includes procurement of the selected technology, preparation of the site, development of a health and safety plan, development of operations procedures, staff selection and training, completion of site cleanup, verification, waste disposal, and release of the site for any future use. Once remediation activities have been completed and verified, the remediated site can be released for restricted or unrestricted use. Remediation of radioactively contaminated sites may require special adaptation to address sites covering very large surface areas or those which are deep and difficult to access. Quality assurance may be very important to the verification of environmental remediation activities. The selection of optimal remediation technologies to solve or mitigate the safety of an environmental contamination problem should be taken into account several factors. The several factors include performance (the ability of the technology to reduce risk to the health and safety of the public and to the environment), reliability and maintenance requirements for the technology, costs of implementing the technology, infrastructure available to support the technology, availability(the ease of accessing the technology and associated services), risk to workers and public safety, environmental impacts of the technology, ability of the technology to meet regulatory acceptance, and communication of stakeholder.

Hydrogen isotope separation involves the separation of hydrogen, deuterium, tritium, and their isotopologues. It is an essential technology for removing radioactive tritium contamination and for obtaining valuable hydrogen isotope resources. Among various hydrogen isotope separation technologies, water electrolysis technology exhibits a high separation factor. Consequently, the electrolysis of tritiated water is of paramount importance as a tritium enrichment method for treating tritium-contaminated water and for analyzing tritium in environmental samples. More recently, hydroelectrolysis technology, which utilizes proton exchange membranes (PEM) to reduce water inventory, has gained favor over traditional alkaline hydroelectrolysis. Nevertheless, it is crucial to decrease the hydrogen permeability of the PEM in order to mitigate the explosion risk associated with tritium hydrogen electrolysis devices. Additionally, efforts are needed to enhance the hydrogen isotope selectivity of the PEM and optimize the manufacturing process of the membrane-electrode assembly (MEA), thereby improving both hydrogen isotope separation performance and water electrolysis efficiency. In this presentation, we will delve into two key aspects. Firstly, we’ll explore the reduction of hydrogen permeability and the enhancement of the hydrogen isotope separation factor in PEM through the incorporation of 2D nanomaterial additives. Secondly, we’ll examine the influence of various MEAs preparation methods on electrolysis and isotope separation performances. Lastly, we will discuss the effectiveness of the developed system in separating deuterium and tritium.

Nuclear facilities present the important task related to the migration and retention of radioactive contaminants such as cesium (Cs), strontium (Sr), and cobalt (Co) for unexpected events in various environmental conditions. The distribution coefficient (Kd) is important factor for understanding these contaminants mobility, influenced by environmental variables. This study focusses the prediction of Kd values for radionuclides within solid phase groups through the application of machine-learning models trained on experimental data and open source data from Japan atomic energy agency. Three machine-learning models, such as the convolutional neural network, artificial neural network, and random forest, were trained for prediction model of the distribution coefficient (Kd). Fourteen input variables drawn from the database and experimental data, including parameters such as initial concentration, solid-phase characteristics, and solution conditions, served as the basis for model training. To enhance model performance, these variables underwent preprocessing steps involving normalization and log transformation. The performances of the models were evaluated using the coefficient of determination. These results showed that the environmental media, initial radionuclide concentration, solid phase properties, and solution conditions were significant variables for Kd prediction. These models accurately predict Kd values for different environmental conditions and can assess the environmental risk by analyzing the behavior of radionuclides in solid phase groups. The results of this study can improve safety analyses and longterm risk assessments related to waste disposal and prevent potential hazards and sources of contamination in the surrounding environment.

For decontamination and quantification of trace amount of tritium in water, an efficient separation technology capable of enriching tritium in water is required. Electrolysis is a key technology for tritium enichment as it has a high H/T and D/T separation factors. To separate tritium, it is important to develop a proton exchange membrane (PEM) electrolyzer having high hydrogen isotope separation factor as well as high electrolyzer cell efficiency. However, there has not been sufficient research on the separation factor and cell efficiency according to the composition and manufacturing method of the membrane electrode assembly (MEA) Therefore, it is necessary to study the optimal composition and manufacturing method of the MEA in PEM electrolyzer. In this study, the H/D separation factor and water electrolysis cell efficiency of PEM electrolyzer were analyzed by changing the anode and cathode materials and electrode deposition method of the MEA. After the water electrolysis experiment using deionized water, the D/H ratio in water and hydrogen gas was measured using a cavity ring down spectrometer and a mass spectrometer, respectively, and the separation factor was calculated. To calculate the cell efficiency of water electrolysis, a polarization curves were obtained by measuring the voltage changes while increasing the current density. As a result of the study, the water electrolyzer cell efficiency of the MEA fabricated with different anode/cathode configurations and electrode formation methods was higher than that of commercial MEA. On the other hand, the difference in H/D separation factor was not significant depending on the MEA fabrication methods. Therefore, using a cell with high cell efficiency when the separation factor is the same will help construct a more efficient water electrolysis system by lowering the voltage required for water electrolysis.

The physicochemical similarities of hydrogen isotopes have made their separation a challenging task. Conventional methods such as cryogenic distillation, Girdler sulfide process, chromatography, and thermal cycling absorption have low separation factors and are energy-intensive. To overcome these limitations, research has focused on kinetic quantum sieving (KQS) and chemical affinity quantum sieving (CAQS) effects for selective separation of hydrogen isotopes. Porous materials such as metal-organic frameworks (MOF), covalent organic frameworks (COF), zeolites, carbon, and organic cages have been studied for hydrogen separation. This study have the literature review for previous research on D2/H2 adsorption and analyzes the D2/H2 adsorption behaviors of hydrogen isotopes for various zeolite using BET at 77 K. The study predicts the D2/H2 adsorption selectivity based on the results obtained with BET. These hydrogen isotope adsorption fundamentals provide a foundation for future processes for tritium separation.

The mobility of radionuclides is largely determined by their radiological properties, geochemical conditions, and adsorption reactions, such as surface adsorption, chemical precipitation, and ion exchange. To evaluate the safety assessments of radionuclides in nuclear sites, it is essential to understand the behavior and mechanism of radionuclides onto soils. Since nuclear power plants are located in coastal areas, the chemical composition of groundwater can vary depending on the intrusion of seawater, altering the adsorption distribution coefficient (Kd) values of radionuclides. This study examines the impact of seawater on the Kd values of clay minerals for cesium (Cs) and strontium (Sr). The results of Cs+ adsorption experiments showed a broad range of Kd values from 36 to 1,820 mL/g at an initial concentration of 1 mg/L and a high sorption coefficient of 15-613 mL/g at an initial concentration of 10 mg/L. Montmorillonite, hydrobiotite, illite, and kaolinite were ranked in terms of their CEC values for Cs+ adsorption, with hydrobiotite having the highest adsorption at 1 mg/L. The results of Sr adsorption experiments showed a wide range of Kd values from 82 to 1,209 mL/g at an initial concentration of 1 mg/L and a lower adsorption coefficient of 6.68-344 mL/g at an initial concentration of 10 mg/L. Both Cs+ and Sr2+ demonstrated lower Kd values at higher initial concentrations. CEC of clays found to have a significant impact on Sr2+ Kd values. Ca2+ ions showed a significant impact on Sr2+ adsorption distribution coefficients, demonstrating the greater impact of seawater on Sr2+ compared to Cs+. These findings can inform future safety assessments of radionuclides in nuclear sites.

Water electrolysis is an efficient method to enrich heavy hydrogen isotopes (tritium and deuterium) in the aqueous phase. Although an alkaline water electrolyzer has been commercialized for mass production of hydrogen, such a method requires additional purification steps to remove electrolytes from the final concentrates. On the other hand, proton exchange membrane water electrolysis (PEMWE) does not require additional electrolyte treatment steps, and PEMWE is operated at higher current density compared to the alkaline water electrolysis. In this study, we investigated deuterium and tritium separation from light water by PEMWE. Separation behaviors at the anode and cathode were analyzed, and H/D and H/T separation factors were compared.

Hydrogen isotopes (H, D, T) separation technologies have received great interest for treatments of tritiated liquid waste produced in Fukushima. In addition, the separated deuterium and tritium can be utilized in various industries such as semiconductors and nuclear fusion as expensive and rare resources. However, separating hydrogen isotopes in gas and liquid forms still requires energyintensive processes. To improve efficiency and performance of hydrogen isotope separation, we are developing water electrolysis, cryosorption, distillation, isotope exchange, and hydrophobic catalyst technologies. Furthermore, an analytical method is studied to evaluate the separation of hydrogen isotopes. This presentation introduces the current status of hydrogen isotope research in this research group.

Detritiation of low-level tritiated water has become global issue after Fukushima accident. Several attempts have been made to reduce the radioactivity of Fukushima tritiated water below legal limit of nuclear plant effluents (~104 Bq·L−1). Various technologies such as water distillation, electrolysis, and catalytic exchange were tested to treat the tritiated water, however, those demand enormous expense to achieve the goal due to low process efficiency. It highlights that the performance enhancement of current technologies is necessary to improve economic feasibility. We have quantitatively evaluated the separation performance of various polymers toward low-level tritium (~105 Bq·L−1) through batch experiments. The polystyrene with grafted by 20 types of functional groups (Tris (2-aminoethyl) amine, dimethylaminomethyl, isocyanate, mercaptomethyl, aminomethyl, hydroxymethyl, triphenylphosphine, morpholine, 2-chlorotrityl amine, 4-(dimethylamino) pyridine, poly (vinyl chloride) carboxylated, poly (4-vinyl pyridine), p-toluenesulfonic acid, p-toluenesulfonyl hydrazide, piperidine, acetyl polystyrene, 2-chlorotrityl chloride, piperazine, diethylene triamine, poly (vinyl chloride)) were suspended in HTO solution (initial activity = 4.7 × 105 Bq·L−1). After the equilibration, the suspension was filtered using 3 kDa membrane filter and the activity in filtrates were quantified by LSC (HIDEX-300 SL). The results demonstrate the detritiation efficiency and separation factors of functional groups toward tritium. Carboxylic group (COOH) showed the most reactive performance as detritiation efficiency of ~4%. Compared to other functional groups, styrene sulfonyl groups including sulfonyl amide (SNH2) and sulfonyl hydrazide (SNHNH2) revealed promising performance for tritium separation as separation factor of 10.97 and 3.85, respectively. However, sulfonyl hydroxide (SOH) which is known as reactive functional group to tritium exchange showed the poor performance (detritiation efficiency: 0.68%; separation factor: 3.02). This study could suggest the promising functional groups for detritiation of low-level tritiated water which can be utilized to enhance the performance of current technologies. For example, reactive functional groups can be grafted on the surface of packing material within distillation tower resulting in the increasing detritiation efficiency.

The behaviors of various desorption agents were investigated during the desorption of cesium (Cs) from samples of clay minerals and actual soil. Results showed that polymeric cation exchange agents (polyethyleneimine (PEI)) efficiently desorbed Cs from expandable montmorillonite, whereas acidic desorption solutions containing HCl or PEI removed considerable Cs from hydrobiotite. However, most desorption agents could desorb only 54% of Cs from illite because of Cs’s specific adsorption to selective adsorption sites. Cs desorption from an actual soil sample containing Cs-selective clay mineral illite (< 200 μm) and extracted from near South Korea’s Kori Nuclear Power Plant was also investigated. Considerable adsorbed 137Cs was expected to be located at Cs-selective sites when the 137Cs loading was much lower than the sample’s cation exchange capacity. At this low 137Cs loading, the total Cs amount desorbed by repeated washing varied by desorption agent in the order HCl > PEI > NH4+, and the highest Cs desorption amount achieved using HCl was 83%. Unlike other desorption agents with only cation exchange capabilities, HCl can attack minerals and induce dissolution of metallic elements. HCl’s ability to both alter minerals and induce H+/Cs+ ion exchange is expected to promote Cs desorption from actual soil samples.