The organic complexing agents such as ethylenediaminetetraacetic acid (EDTA), nitrilotriacetic acid (NTA), and isosaccharinic acid (ISA) can enhance the radionuclides’ solubility and have the potential to induce the acceleration of radionuclides’ mobility to a far-field from the radioactive waste repository. Hence, it is essential to evaluate the effect of organic complexing agents on radionuclide solubility through experimental analysis under similar conditions to those at the radioactive waste disposal site. In this study, five radionuclides (cesium, cobalt, strontium, iodine, and uranium) and three organic complexing agents (EDTA, NTA, and ISA) were selected as model substances. To simulate environmental conditions, the groundwater was collected near the repository and applied for solubility experiments. The solubility experiments were carried out under various ranges of pHs (7, 9, 11, and 13), temperatures (10°C, 20°C, and 40°C), and concentrations of organic complexing agents (0, 10-5, 10-4, 10-3, and 10-2 M). Experimental results showed that the presence of organic complexing agents significantly increased the solubility of the radionuclides. Cobalt and strontium had high solubility enhancement factors, even at low concentrations of organic complexing agents. We also developed a support vector machine (SVM) model using some of the experimental data and validated it using the rest of the solubility data. The root mean square error (RMSE) in the training and validation sets was 0.012 and 0.016, respectively. The SVM model allowed us to estimate the solubility value under untested conditions (e.g., pH 12, temperature 30°C, ISA 5×10-4 M). Therefore, our experimental solubility data and the SVM model can be used to predict radionuclide solubility and solubility enhancement by organic complexing agents under various conditions.

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.

Radiological impact analyses were carried out for a near-surface radioactive waste repository at Gyeongju in South Korea. The RESRAD-ONSITE code was applied for the estimation of maximum exposure doses by considering various exposure pathways based on a land area of 2,500 m2 with a 0.15 m thick contamination zone. Typical influencing input parameters such as shield depth, shield materials’ density, and shield erosion rate were examined for a sensitivity analysis. Then both residential farmer and industrial worker scenarios were used for the estimation of maximum exposure doses depending on exposure duration. The radiation dose evaluation results showed that 60Co, 137Cs, and 63Ni were major contributors to the total exposure dose compared with other radionuclides. Furthermore, the total exposure dose from ingestion (plant, meat, and milk) of the contaminated plants was more significant than those assessed for inhalation, with maximum values of 5.5×10−4 mSv‧yr−1 for the plant ingestion. Thus the results of this study can be applied for determining near-surface radioactive waste repository conditions and providing quantitative analysis methods using RESRAD-ONSITE code for the safety assessment of disposing radioactive materials including decommissioning wastes to protect human health and the environment.