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.
Radionuclides in low- and intermediate-level radioactive wastes from the decommissioning process of nuclear power plants were generally immobilized by cementation methods. Ethylenediaminetetraacetic acid (EDTA), which is extensively used as a decontamination agent, can affect the behaviors of radionuclides immobilized in cement waste forms. In this study, the effects of EDTA contained in simulated radioactive decommissioning wastes on the leaching characteristics of immobilized Co and Cs and the microstructure evolution of cement waste form. Co leaching was accelerated by the formation of Co–EDTA complexes with high mobility and solubility. Cs leaching was hindered by the ion competition with other metal–EDTA complexes for releasing from the cement waste form. Cs leaching was also retarded by carbonated layer at edge of the cement waste form, which process is facilitated by the presence of EDTA. Finally, the effects of EDTA on the leaching characteristics of immobilized Cs and Co and the microstructure evolution of the cement waste form should be considered to ensure the safety of disposal for lowand intermediate-level radioactive wastes.
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.
Safety for the radioactive waste disposed of in the disposal facility should be secured through safety assessment in consideration of the various situations. In this study, the influence and correlation of EDTA and ISA, which are the factors that can impede the safety of the disposal facility, were analyzed using the PHREEQC computational code. Thermodynamic database (TDB) of Andra, specific ion interaction theory (SIT) model as ionic strength correction model, radionuclides (Ni, Am, Pu) were adopted to perform the calculation on the distribution of chemical species by pH. According to the results, EDTA dominated the system and the effect of ISA is relatively small for the distribution of the chemical species of divalent and trivalent cations in neutral and weak base conditions. In the case of the tetravalent cations, the effect of ISA increased compared to the previous case especially in the strong base conditions. In conclusion, EDTA has a more significant effect on the system than ISA under the environment of the domestic disposal facility. Furthermore, when EDTA and ISA are present simultaneously in the system, the effects of two materials are inversely proportional and this characteristic should be considered during the safety assessment.
Mechanism and kinetics of Rhenium complexes as a surrogate of Technetium-99 (99Tc) is worthy of study from radioactive waste safe disposal perspective. Re(IV)-EDTA was synthesized via the reduction of Re(VII) with Sn(II) in the presence of Ethylenediaminetetracetic acid (EDTA). The Re(IV)-EDTA was then degraded by H2O2 (7–30%) at pH of 3–11 in ionic strength I = 0–2 M solution. The Re- EDTA was observed to degrade more rapidly at pH of ≤ 3–4 than one of ≥ 10–11 and remained stable at pH = 7–9. At a low acidic pH, the complex degradation process was facilitated by protonation and corresponded to the exponential model (y = k. e–nt). In contrast, at an alkaline pH, the degradation was facilitated OH– complexation with Re(IV) and corresponded to a linear model (y = –mt + C). Complex degradation followed the zero-order rate kinetics for the H+ and Re-EDTA parameters, apart from a pH of 3, for which degradation was a better fit to first order kinetics. A higher Re(IV)-EDTA stability at a pH of 7–9 demonstrated that Re(IV)-EDTA (or 99Tc(IV)-EDTA) tends to be more persistent in natural environmental conditions.
Numerous low-and intermediate level radioactive wastes were generated from the decommissioning processes of nuclear power plants. Radionuclides such as Co and Cs contained in decommissioning wastes should be immobilized to prevent the release of radionuclides from the wastes due to its harmful impacts on ecosystem by high radioactivity and long half-life. Ethylenediaminetetraacetic acid (EDTA) used as decontamination agent can be contained in cement waste during decommissioning process of nuclear power plants. In addition, EDTA can be stably and strongly bound with radionuclides, resulting in the acceleration of the nuclide release from solidified cement matrix. Here, we investigated the effects of EDTA on leaching behaviors of Co and Cs immobilized in the cement specimen. The leaching tests were performed according to the ANS 16.1 “Measurement of the leachability of solidified low-level radioactive wastes by a short-term test procedure”. From the results, an increase in the EDTA content in the cement specimen led to an increase in Co leaching, whereas a decrease in Cs leaching. Leaching of Cs was dominantly controlled by diffusion from the pore space of the cement specimen to the solution. The effective diffusion coefficient and leachability index of nuclide were determined using the diffusion-release models of ANS 16.1. The results of present study can be used in the safety assessment for disposal of the radioactive waste generated by decommissioning of nuclear power plants.
In vitro culture (IVC) can be used for a variety of assisted reproductive technologies. However, IVC in dog has been low efficient compared to other mammalian. It is believed that an embryo developmental block in IVC embryos is cause of low production efficiency. There is no study of embryo developmental block in dog yet. In this study, we attempted to estimate the beneficial role of EDTA in canine parthenogenic (PA) embryos development to overcome embryo developmental block. The PA embryos were divided into EDTA treated and non-treated groups. Embryo developmental efficiency was measured by activating chemically parthenote. After EDTA induction, PA embryos were evaluated for embryonic development, ROS activity, mitochondrial integrity, ATP production and genomic activation. The EDTA treated PA embryos showed significantly higher survival rate and improved cavity formation compared to non-treated. Moreover, cytoplasmic ROS level was mitigated and mitochondrial membrane potential was found significantly higher in EDTA treated group followed by higher ATP production. Furthermore, major embryonic genomic activation specific markers/factors were also elevated in EDTA treated group. Conclusively, these results indicated that EDTA showed substantially positive effect to overcome embryo developmental block in canine.
Somatic cell nuclear transfer (SCNT) is a useful biotechnological tool for animal cloning. Until now, SCNT has been inefficient, especially in dog. It is believed that an embryo developmental block in SCNT embryos is cause of low production efficiency. However, no studies have been performed on canines for embryo developmental block. In this study, we attempted to evaluate the beneficial role of EDTA in canine parthenogenic (PA) embryos development to overcome embryo developmental block. The PA embryos were divided into 0.01 mM EDTA treated and non-treated groups. Embryo developmental efficiency was measured by activating chemically parthenote. After EDTA induction, PA embryos were evaluated for embryonic development, Reactive Oxygen Species (ROS) activity, mitochondrial integrity, ATP production and genomic activation. The EDTA treated PA embryos showed significantly higher survival rate and improved cavity formation compared to non-treated. Furthermore, cytoplasmic ROS level was mitigated and mitochondrial membrane potential was found significantly higher in EDTA treated group followed by higher ATP production. Moreover, major embryonic genomic activation specific markers/factors were also elevated in EDTA treated group. Conclusively, we elucidated that EDTA showed substantially positive effect to overcome embryo developmental block in canine.