Organic complexing agents may affect the mobility of radionuclides at low- and intermediate-level radioactive waste repositories. Especially, isosaccharinic acid (ISA) is the main cellulose degradation product under high pH conditions in cement pore water. ISA can combine with radionuclides and form stable complexes that adversely influence adsorption in the concrete phase, resulting in radionuclides to leach to the near- and far-fields of repositories. This study focuses on investigating the sorption of ISA onto engineered barriers such as concrete, thereby studying adsorption isotherms of ISA on concrete and comparing various isotherm models with the experimental data. The adsorption experiment was conducted in three background solutions, groundwater (adjusted to pH 13 using NaOH), State 1 (artificial cement pore water, pH 13.3), and State 2 (artificial cement pore water, pH 12.5), in a batch system at a temperature of 20°C. Concrete was characterized using BET, Zeta-potential analyzer, XRD, XRF, and SEM-EDS. ISA concentrations were detected using HPLC. The experimental data were best fitted to one-site Langmuir isotherm; On the other hand, either two-site isotherm or Freundlich isotherm couldn’t give reasonable fitting to the experimental data. The observed ISA sorption behavior on concrete is crucial for the disposal of radioactive waste because it can significantly lower the concentration of ISA in the pore water. Although one-site Langmuir isotherm might effectively represent the sorption behavior of ISA on concrete, the underlying mechanism is still unknown, and further investigation should be done in the near future.

Encapsulation using cement as a solidification method for disposal of radioactive waste is most commonly used in most advanced countries in the nuclear technology to date due to its advantages such as low material cost and accumulated technology. However, in case of cement solidification, since moisture or hydroxyl group in cement is decomposed by radioactivity, it may happen that gas is generated, structural stability is weakened, and leachability is increased due to low chemical durability. Therefore, the various new solidification methods are being developed to replace it. As one of these alternative technologies, for dispersible metal compounds generated through the incineration replacement process, the study on engineering element technology for powder metallurgy is under way, which overcomes the interference problem between mechanical elements and media that may occur during the process such as the homogeneous mixing process of the target powder substance and additives used in the powder metallurgy concept-based sintering process for the solidification of the final glass composite material (GCM), the process of creating a compressed molded body using a specific mold, the process of final sintering treatment. The solidification process of dispersible radioactive waste can be largely divided into pre-treatment stage, molding stage, and sintering stage, and the characteristics of the final radioactive waste solidification material can vary depending on the solidification treatment characteristics of each stage. In relation with these characteristics, the matters to be considered when designing device for each stage to solidify dispersible radioactive waste (property of super-mixing device for homogenized powder formation, structural geometry and pressure condition of molding device for production of compressed molded body, temperature and operation characteristics of sintering device for final glass composite material (GCM), etc.) are drawn out. It is expected that the solidification device design reflecting these considerations will meet all disposal conditions of radioactive waste material, such as compressive strength and leaching characteristics of solidified radioactive waste material, and create a uniformized solidification of radioactive waste material.

In this study, the process of compressing/packaging the spent filters of Kori Unit 1, which was conceptually presented in the previous study, is advanced so that disposal suitability for each step can be secure efficiently. In particular, the differences between the previous study and this study are that the disposable filters are screened using an In-Situ Object Counting System (ISOCS), and the method of collecting representative samples for development of scaling factor is specified. The process of compressing/packaging the spent filters consists of 7 stages as follows. 1) Collecting: The spent filters temporarily stored in the filter room are collected by dose and type remotely using a robot system to minimize the radiation exposure of workers according to a pre-established packaging plan. 2) Screening: The gamma activity concentration of the spent filters received by the robot system is measured by ISOCS. The spent filters below the low-level waste concentration limit and the surface dose are transferred into the compression system, while the others are returned in the filter room again. 3) Sampling: The external perforator drilling/cutting the filter was developed for sampling required for the new scaling factors. Since the sampling is collected remotely, the risk of exposure to workers can be reduced. The newly developed scaling factor will be used to verify the disposal suitability of the packages. 4) Compression: According to the pre-established plan, the spent filter collected by dose and type, is supplied to the compression system considering the dose and radionuclide inventory. Whether to additionally store the compressed filter in the drum is determined by checking the accumulated dose. 5) Immobilization: Immobilization with a safety material is necessary when inhomogeneous wastes, like spent filters, have the total radionuclide concentration with a half-life of more than 20 years is 74,000 Bq/g or more and for filling rate or non-dispersible treatment of particulates. 6) Packaging and Analysis: Waste information is labelled onto the package after the measurements of surface dose rate and surface contamination. Finally, using the drum assay system, the gamma radionuclide concentration is measured to identify at least 95% of the total radioactivity concentration of the package. 7) Temporary Storage and Delivery: The packages are moved to temporary storage in the plant prior to disposal. After establishing the plan for delivery and applying for a takeover request to KORAD, if the acceptance inspection is passed, the packages are transported to the disposal facility.

Low- and intermediate-level radioactive wastes have been disposed of in the first-phase deep underground silo disposal at Gyeongju in South Korea. These radioactive wastes contain harmful radionuclides such as Uranium-238 (238U), which can pose long-term and deleterious effects on humans and the natural environment. Ethylenediaminetetraacetic acid and isosaccharinic acid, which can be formed via cellulosic waste degradation under high alkaline conditions might considerably enhance the transport behavior of 238U with the intrusion of rainwater and groundwater. In this study, the engineered barriers (concrete and grout) and natural barriers (sedimentary rock and granite) were used to investigate the 238U transport behavior in artificial cementitious porewater of State I (pH 13.3) and State II (pH 12.5) based on groundwater or rainwater. The surface properties and geochemical compositions of barrier samples were characterized using XRD, XRF, SEM-EDX, and BET. The transport behaviors of 238U in various solution conditions were observed by sorption distribution coefficient (Kd) at a range of initial chelating agents concentration (10-5-10-2 M). The sorption behavior of 238U was retarded more in the engineered rock barriers than in the natural rock barriers. The mobility enhancement of 238U was more significant in State I than in State II. In comparison with the absence of chelating agents, negligible changes in the Kd values of 238U were observed at less than initial chelating agent concentrations of 10-4 M. However, the Kd values of 238U were significantly reduced at initial chelating agent concentrations higher than 10-3 M. Therefore, these experimental findings show that the transport behavior of 238U into the geo- and bio-sphere could be accelerated by the presence of chelating agents and the type of cement degradation states.

Engineered barriers (concrete and grout) in Low- and Intermediate-Level Waste (L/ILW) disposal facilities tend to degrade by groundwater or rainfall water over a long period of time. During the degradation process, radionuclides stored in the disposal facility might be released into the pore water, which can pass through the natural rock barriers (granite and sedimentary rock) and may reach the near-field and far-field. In this transportation, radionuclide might be sorbed onto the engineered and natural rock barriers. In addition, the organic complexing agent such as ethylenediaminetetraacetic acid (EDTA) and α-isosaccharinic acid (ISA), is also present in pore water, which may affect the sorption and mobility of radionuclide. In this study, the sorption and mobility of 90Sr under different conditions such as two pHs (7 and 13), different initial concentrations of organic complexing agents (from 10-5 M to 10-2 M), and solutions (groundwater, pore water, and rainfall water) were investigated in a batch system. The groundwater was collected at the L/ILW disposal facility located at Gyeongju in South Korea. The pore water and rainfall water were artificially made in the laboratory. The concrete, grout, granite, and sedimentary rock samples were collected from the same study sites from where the groundwater was collected. The rock samples were crushed to 53-150 micrometers and were characterized by XRD, XRF, SEM-EDS, BET, and zeta potential analyzer. 90Sr concentration was determined using liquid scintillation counting. The sorption of 90Sr was described by distribution coefficients (Kd) and sorption reduction factor (SRF). In the case of EDTA, the Kd values of 90Sr remained constant from 10-5 M to 10-3 M and tended to decrease at 10-2 M, while in case of ISA the Kd values decreased steadily as the concentration of ISA was increased from 10-5 M to 10-3 M; However, a sudden reduction in the Kd values were observed above 10-2 M. In comparison to EDTA, ISA gave a higher SRF of 90Sr. Therefore, from the above results, it can be concluded that the presence of ISA has a greater effect on the sorption and mobility of radionuclide in the solutions than EDTA, and the radionuclide may reach near- and far-field of the L/ILW disposal facility.

Radionuclides stored in a radioactive waste repository over a long period of time might be leached through the barriers such as engineered rock (cement) and natural rock (granite). Organic complexing agents such as ethylenediaminetetraacetic acid (EDTA) and isosaccharinic acid (ISA) may also influence the mobility of radionuclides. In this study, a continuous fixed-column reactor packed with engineered and natural rocks was designed to investigate the effect of organic complexing agents on cesium mobility through cement and granite under anaerobic conditions. The influent flow rate of the mixed solution (organic complexing agent and cesium) at the column bottom was 0.1 mL/min, while that of groundwater was 0.2 mL/min, which was introduced between cement and granite layers in the middle of the column. The hydraulic properties such as diffusion coefficient and retardation factor were derived by a bromide tracer test. The effects of different operating parameters, such as initial cesium concentrations, initial EDTA or ISA concentrations, and bed size, on the cesium adsorption were investigated. The Thomas, Adams-Bohart, and Yoon-Nelson models were applied to the experimental data to predict the breakthrough curves using non-linear regression. These results suggest that organic complexing agents such as EDTA and ISA significantly influence the mobility of cesium in the barriers, indicating that the presence of complexing agents enhances the migration of cesium to the geosphere.

Radionuclides can be leached into groundwater or soil over a long period of time due to unexpected situations even after being permanently disposed of in a repository. Therefore, it is necessary to investigate the mobility of radionuclides for the safety assessment of radioactive waste disposal. In this study, the effects of organic complexing agents such as ethylenediaminetetraacetic acid (EDTA) and isosaccharinic acid (ISA) on the sorption behavior of 239Pu and 99Tc over cementitious (concrete and grout) and natural rock samples (granite and sedimentary rock) were investigated in batch sorption experiments. For characterization of rock samples, XRD, XRF, FT-IR, FE-SEM, BET, and Zeta-potential analyses were performed. For the evaluation of mobility, the distribution coefficient (Kd) was selected and compared. The adsorption experiment was carried out at two pHs (7 and 13), a temperature of 20°C, and a range of organic complexing agents concentrations (10-7~10-2 M and 10- 5~10-2 M for 239Pu and 99Tc, respectively). The radionuclides concentrations in adsorption samples were analyzed using ICP-MS. The Kd values for 239Pu in all rock samples reduced significantly due to the presence of EDTA, even at low concentrations such as 10-5 M. In the case of ISA, the limiting noeffect concentration was much higher than that of EDTA. On the other hand, 99Tc showed relatively lower Kd values than 239Pu, and the sorption behavior of 99Tc was almost unaffected by the organic complexing agents for all rock samples. Therefore, it is possible to assume that the increased mobility of radionuclides, especially, 239Pu, in groundwater caused by the lowering of sorption at even low concentrations of organic complexing agents may result in the transport of radionuclides to the nearand far-field location of the repository.

Cellulose-based wastes can be degraded into short-chain organic acids at the cementitious radioactive waste repository. Isosaccharinic acid (ISA), one of the main degradation products, can form the chelate complex with metals and radionuclides, and these complexes have a potential that can accelerate to move the radionuclides to far-field from the repository. This study characterized the amount of generated ISA from typical cellulosic materials in the repository. Two different degradation experiments were conducted under alkaline conditions (saturated with Ca(OH)2 at pH 12.4): i) cellulosic material mixture under an opened condition (partially aerobic), and ii) cellulosic material under an anaerobic condition in a nitrogen-purged glove box. In the first case, three different types of cellulosic materials–paper, cotton, and wood– were mixed at the same ratio, and the experiments were carried out at three different temperatures (20°C, 40°C, and 60°C). It revealed that both the cellulose degradation rate and generated ISA concentration were high at high reaction temperatures, and various soluble degradation products such as formic acid and lactic acid were generated. The cellulose degradation in this work seems to still stay at a peeling-off process. In the second study, each type of cellulosic material was applied in its own batch experiments, and the amount of generated ISA was in the order of paper > wood > cotton. The above two experiments are supposed to be a long-term study until the generated ISA reaches an equilibrium state.

Organic complexing agents which are contained in the radioactive waste can form the complex with radionuclides and enhance the solubility of radionuclides. The mobility of radionuclides to the far-field from the repository will be increased by radionuclide-ligand complex formation. Therefore, the assessment of the radionuclides’ solubility should be performed in the presence of organic complexing agents. In this study, five radionuclides (cobalt, strontium, iodine, cesium, and uranium) and three organic complexing agents (ethylenediaminetetraacetic acid (EDTA), nitrilotriacetic acid (NTA), and isosaccharinic acid (ISA)) were selected as model radionuclides and organic complexing agents, respectively. For simulating the in-situ condition, the groundwater near the repository was collected and applied in solubility experiments and the solubility was measured in various environmental conditions such as different pHs (7, 9, 11, and 13), temperatures (10°C, 20°C, and 40°C), and a range of organic complexing agent concentrations (10-5, 10-4, 10-3, and 10-2 M). In cases of cesium and iodine, they were very soluble in all conditions, and the effect on their solubilities was not observed. However, at high pHs, cobalt and strontium showed lower solubilities than at neutral pH and the solubility enhancement by the organic complexing agents was significant. Moreover, the effects of each organic ligand showed obvious differences and were in the order of EDTA > NTA > ISA. The solubility of uranium was increased with increasing the organic ligand concentration at lower pHs, but the organic complexing agents did not cause a remarkable difference at high pHs. According to these results, the presence of complexing agents could enhance the radionuclides’ solubility and increase the potential to release the radionuclides to the far-field from the repository. Solubility experiments of other major radionuclides in the repository are in progress.

Korea Radioactive Waste Agency (KORAD), regulatory body and civic groups are calling for an infrastructure system that can more systematically and safely manage data on the results of radioactive waste sampling and nuclide analysis in accordance with radioactive waste disposal standards. To solve this problem, a study has been conducted on the analysis of the nuclide pattern of radioactive waste on the nuclide data contained in low-and intermediate-level radioactive waste. This paper will explain the optimal repackaged algorithm for reducing radioactive waste based on previous research results. The optimal repackaged algorithm for radioactive waste reduction is comprised based on nuclide pattern association indicators, classification by nuclide level of small-packaged waste, and nuclide concentration. Optimization simulation is carried out in the order of deriving nuclide concentration by small-packaged, normalizing drum minimization as a function of purpose, normalizing constraints, and optimization. Two scenarios were applied to the simulation. In Scenario 1 (generating facilities and repackaged by medium classification without optimization), it was assumed that there are 886 low-level drums and 52 very low-level drums. In Scenario 2 (generating facilities and repackaged by medium classification with optimization), 708 and 230 drums were assigned to the low-level and very low-level drums, respectively. As a result of the simulation, when repackaged in consideration of the nuclide concentration and constraints according to the generating facility cluster & middle classification by small package (Scenario 2) the low-level drum had the effect of reducing 178 drums from the baseline value of 886 drums to 708 drums. It was found that the reduced packages were moved to the very low-level drum. The system that manages the full life-cycle of radioactive waste can be operated effectively only when the function of predicting or tracking the occurrence of radioactive waste drums from the source of radioactive waste to the disposal site is secured. If the main factors affecting the concentration and pattern of nuclides are systematically managed through these systems, the system will be used as a useful tool for policy decisions that can prevent human error and drastically reduce the generation of disposable drums.