A low- and intermediate-level radioactive waste repository contains different types of radionuclides and organic complexing agents. Their chemical interaction in the repository can result in the formation of radionuclide-ligand complexes, leading to their high transport behaviors in the engineered and natural rock barriers. Furthermore, the release of radionuclides from the repository can pose a significant risk to both human health and the environment. This study explores the impact of different experimental conditions on the transport behaviors of 99Tc, 137Cs, and 238U through three types of barrier samples: concrete, sedimentary rock, and granite. To assess the transport behavior of the samples, the geochemical characteristics were determined using X-ray diffraction (XRD), X-ray fluorescence (XRF), Fouriertransform infrared spectroscopy (FTIR), scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM-EDS), and Brunauer-Emmett-Teller (BET) analysis. The adsorption distribution coefficient (Kd) was used as an indicator of transport behavior, and it was determined in batch systems under different conditions such as solution pH (ranging from 7 to 13), temperature (ranging from 10 to 40°C), and with the presence of organic complexing agents such as ethylenediaminetetraacetic acid (EDTA), nitrilotriacetic acid (NTA), and isosaccharinic acid (ISA). A support vector machine (SVM) was used to develop a prediction model for the Kd values. It was found that, regardless of the experimental parameters, 99Tc may migrate easily due to its anionic property. Conversely, 137Cs showed low transport behaviors under all tested conditions. The transport behaviors of 238U were impacted by the order of EDTA > NTA> ISA, particularly with the concrete sample. The SVM models can also be used to predict the Kd values of the radionuclides in the event of an accidental release from the repository.

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.

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.