Chelating agents in low and intermediate radioactive wastes can form complexes with radionuclides and increase the mobility of the radionuclides. According to the Korea Radioactive Waste Agency (Acceptance criteria for low and intermediate radioactive waste, WAC-SIL-2022-1), if the amount of residual chelating agents in the waste are greater than 0.1%, the chemical names and residual amounts should be specified; if greater than 1%, the waste must be solidified and contain no more than 8%. The existing method for analyzing chelates in radioactive waste was based on UV–Visible spectrophotometry (UV-Vis), but the new method is based on liquid chromatography/mass spectrometry (LC-MS). The analysis was performed in aqueous solution before applying to real samples. Since the real sample may contain several heavy metals, it is expected that the chelates will exist as complexes. Therefore, 1.0×10-4 mol L-1 of EDTA (Ethylenediaminetetraacetic acid), DTPA (Diethylenetriaminepentaacetic acid), NTA (Nitrilotriacetic acid), and excess metals in aqueous solution were analyzed using HPLC using RP (Reverse Phase) column and HILIC (Hydrophilic interaction) column. When the RP column was used, each substance eluted without separation at the beginning of the analysis. However, when analyzed using a HILIC column, the peaks of each substance were separated. LC-MS measurements using HILIC conditions resulted in separations with better sensitivity.
As existing nuclear power plants reach the end of their lifespan, 22 nuclear power plants in korea are scheduled to be permanently shut down and decommissioned by 2050. Chelates are used as decontamination agents during nuclear power plant operation and decommissioning, and as a result, decommissioning waste contains chelates. Chelates contained in radioactive waste are complexed with radionuclides and increases their mobility. So, qualitative and quantitative analysis of chelates contained in radioactive waste is necessary. However, the spectroscopic method (UVVis), previously used for chelate analysis in Korea takes too much time for analysis and cannot analyze two or more chemically similar chelates at the same time. Due to these problems, new methods for analyzing chelate must be developed. Overseas, many cases of chelate analysis using advanced analysis equipment have been reported. CEA in France has developed a chelate analysis method for application to radioactive waste using HPLC-MS (J. Chromatogram. A, 1276, 20-25, 2013). In this method, the existing method of measuring EDTA using a complex of Fe and EDTA was improved to measuring a complex of Ni and EDTA. Based on such overseas cases, we would like to develop an analysis method for chelates in radioactive waste. For this purpose, we will verify similar overseas papers and develop pretreatment methods for mixtures of chelates (EDTA, DTPA, NTA) and metals (Fe, Ni, Cu, etc.) in various media. Finally, we will develop a separation analysis technology for multi-component chelates in nuclear decommissioning waste based on LCMS.
To effectively assess the inventory of radionuclides generated from nuclear power plants using a consistent evaluation method across diverse groups, it is imperative to analyze the similarity in radioactive distribution between these groups. Various methodologies exist for evaluating this similarity, and the application of statistical approaches allows us to establish similarity at a specific confidence level while accounting for the dataset size (degrees of freedom). Initially, if the variance characteristics of the two groups are similar, a t-test for equal variances can be employed. However, if the variance characteristics differ, methods for unequal variances should be applied. This study delineates the approach for assessing the similarity in radioactive distribution based on the analytical characteristics of the two groups. Furthermore, it delves into the results obtained through two case studies to offer insights into the assessment process.
We conducted safety assessments for the disposal of spent resin mixed waste after the removal of beta radionuclides (3H, 14C) in a landfill facility. The spent resin tank of Wolsong nuclear power plant is generated by 8:1:1 weight ratio of spent ion exchange resin, spent activated carbon and zeolite. Waste in the spent resin tank was classified as intermediate-level radioactive waste due to 14C. Other nuclides such as 60Co and 137Cs exhibit below the low-level radioactive waste criteria. The techniques for separating mixed waste and capturing 14C have been under development, with a particular focus on microwave-based methods to remove beta radionuclides (3H, 14C) from spent activated carbon and spent resin within the mixed waste. The spent resin and activated carbon within the waste mixture exhibits microwave reactivity, heated when exposed to microwaves. This technology serves as a means to remove beta isotopes within the spent resin, particularly by eliminating 14C, allowing it to meet the low-level radioactive waste criteria. Using this method, the waste mixture can meet disposal requirements through free water and 3H removal. These assessments considered the human intrusion scenarios and were carried out using the RESRAD-ONSITE code. The institutional management period after facility closure is set at 300 years, during which accidental exposures resulting from human intrusion into the disposal site are accounted for. The assessment of radiation exposure to intruders in a landfill facility included six human intrusion scenarios, such as the drilling scenario, road construction scenario, post-drilling scenario, and post-construction scenario. Among the six human intrusion scenarios considered, the most conservative assessment about annual radiation exposure was the post-drilling scenario. In this scenario, human intrusion occurs, followed by drilling and residence on the site after the institutional management period. We assumed that some of the vegetables and fruits grown in the area may originate from contaminated regions. Importantly, we confirmed that radiation doses resulting from post-institutional management period human intrusion scenarios remain below 0.1 mSv/y, thus complying with the annual dose limits for the public. This research underscores the importance of effectively managing and securing radioactive waste, with a specific focus on the safety of beta radionuclide-removed waste during long-term disposal, even in the face of potential human intrusion scenarios beyond the institutional management period.
The operation time of a disposal repository is generally more than one hundred years except for the institutional control phase. The structural integrity of a repository can be regarded as one of the most important research issues from the perspective of a long-term performance assessment, which is closely related to the public acceptance with regard to the nuclear safety. The objective of this study is to suggest the methodology for quantitative evaluation of structural integrity in a nuclear waste repository based on the adaptive artificial intelligence (AI), fractal theory, and acoustic emission (AE) monitoring. Here, adaptive AI means that the advanced AI model trained additionally based on the expert’s decision, engineering & field scale tests, numerical studies etc. in addition to the lab. test. In the process of a methodology development, AE source location, wave attenuation, the maximum AE energy and crack type classification were subsequently studied from the various lab. tests and Mazars damage model. The developed methodology for structural integrity was also applied to engineering scale concrete block (1.3 m × 1.3 m × 1.3 m) by artificial crack generation using a plate jacking method (up to 30 MPa) in KURT (KAERI Underground Research Tunnel). The concrete recipe used in engineering scale test was same as that of Gyeongju low & intermediate level waste repository. From this study, the reliability for AE crack source location, crack type classification, and damage assessment increased and all the processes for the technology development were verified from the Korea Testing Laboratory (KTL) in 2022.
The increasing accumulation of spent nuclear fuel has raised interest in High-Level Waste (HLW) repositories. For example, Sweden is under construction of the KBS-3 repository. To ensure the safety of such HLW repository, various countries have been developing assessment models. In the Republic of Korea, the Korea Atomic Energy Research Institute has been developing on the AKRS model. However, traditional safety assessment models have not considered the fracture growth in the far-field host rock as a function of time. As repository safety assessments guarantee safety for million years, sustained stress naturally leads to the progressive growth of fractures as time goes on. Therefore, it becomes essential to account for fracture growth in the surrounding host rock. To address this, our study proposes a new coupling scheme between the Fracture growth model and the radionuclide transport model. That coupling scheme consists of the Cubic Law model as a fracture growth function and the GoldSim code which is a commercial software for radionuclide transport calculations. The model that adopting such fracture growth functions showed an increase of up to 15% in the release of radionuclide compared to traditional assessment models. our observations indicated that crack growth as a function of time led to an increase in hydraulic conductivity that allowed more radionuclide transport. Notably, these findings show the significance of adopting fracture growth models as a critical element in evaluating the safety of nuclear waste repositories.
Currently, the most promising fuel candidate for use in sodium fast reactors (SFRs) is metallic fuel, which is produced by a modified casting method in which the metallic fuel material is sequentially melted in an inert atmosphere to prevent volatilization, followed by melting in a graphite crucible, and then injection casting in a quartz (SiO2) mold to produce metallic fuel slugs. In previous studies, U-Zr metallic fuel slugs have been cast using Y2O3 reaction prevent coatings. However, U-Zr alloy-based metallic fuel slugs containing highly reactive rare earth (RE) elements are highly reactive with Y2O3-coated quartz (SiO2) molds and form a significant thickness of surface reaction layer on the surface of the metallic fuel slug. Cast parts that have reacted with nuclear fuel materials become radioactive waste. To decrease amount of radioactive waste, advanced reaction prevent material was developed. Each RE (Nd, Ce, Ln, Pr) element was placed on the reaction prevent material and thermal cycling experiments were carried out. In casting experiments with U-10wt% Zr, it was reported that Y2O3 layer has a high reaction prevent performance. Therefore, the reaction layer properties for RE elements with higher reactivity than uranium elements were evaluated. To investigate the reaction layer between RE and NdYO3, the reaction composition and phase properties as a function of RE content and location were investigated using SEM, EDS, and XRD. The results showed that NdYO3 ceramics had better antireaction performance than Y2O3.
A solution combustion process for the synthesis of hollandite (BaAl2Ti6O16) powders is described. SYNROC (synthetic rock) consists of four main titanate phases: perovskite, zirconolite, hollandite and rutile. Hollandite is one of the crystalline host matrices used for the disposal of high-level radioactive wastes because it immobilizes Sr and Lns elements by forming solid solutions. The solution combustion synthesis, which is a self-sustaining oxi-reduction reaction between a nitrate and organic fuel, generates an exothermic reaction and that heat converts the precursors into their corresponding oxide products in air. The process has high energy efficiency, fast heating rates, short reaction times, and high compositional homogeneity. To confirm the combustion synthesis reaction, FT-IR analysis was conducted using glycine with a carboxyl group and an amine as fuel to observe its bonding with metal element in the nitrate. TG-DTA, X-ray diffraction analysis, SEM and EDS were performed to confirm the formed phases and morphology. Powders with an uncontrolled shape were obtained through a general oxide-route process, confirming hollandite powders with micro-sized soft agglomerates consisting of nano-sized primary particles can be prepared using these methods.
Gamma imaging devices that can accurately localize the radioactive contamination could be effectively used during nuclear decommissioning or radioactive waste management. While several hand-held devices have been proposed, their low efficiency due to small sensors have severely limited their application. To overcome this limitation, a high-speed gamma imaging system is under development which comprises two quad-type detectors and a tungsten coded aperture mask. Each quad-type detector consists of four rectangular NaI(Tl) crystals with dimensions of 146×146 mm2 and 72 square-type photomultiplier tubes (PMTs). The detectors are placed in front and back to serve as scatter and absorber, respectively, for Compton imaging. In addition, a coded aperture mask was fabricated in rank 19 modified uniformly redundant array pattern and placed in front of the scatter for coded aperture imaging. The system offers several advanced features including 1) high efficiency achieved by employing large-area NaI(Tl) crystals and 2) broad energy range of imaging by employing a hybrid imaging combining Compton and coded aperture imaging. The imaging performance of the system was evaluated through experiments in various conditions with different gamma energies and source positions. The imaging system provides clear images of the source locations for gamma energies ranging from as low as 59.5 keV (241Am) to as high as 1,330 keV (60Co). The imaging resolution was within the range of 7.5–9.4°, depending on gamma energies, when a hybrid maximum likelihood estimation maximization (MLEM) algorithm was used. The developed system showed high sensitivity, as the 137Cs source at distance, incurring dose rate lower than background level (0.03 μSv/h above background dose rate), could be imaged in approximately 2 seconds. Even under lower dose rate condition (i.e., 0.003 μSv/h above background dose rate), the system was able to image the source within 30 seconds. The system developed in the present study broadens the applicable conditions of the gamma ray imaging in terms of gamma ray energy, dose rate, and imaging speed. The performance demonstrated here suggests a new perspective on radiation imaging in the nuclear decontamination and radioactive waste management field.