간행물

한국방사성폐기물학회 학술논문요약집 Abstracts of Proceedings of the Korean Radioactive Wasts Society

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2023 추계학술논문요약집 (2023년 11월) 429

421.
2023.11 구독 인증기관·개인회원 무료
Molten Salt Reactor, which employs molten salt mixture as fuel, has many advantages in reactor size and operation compared to conventional nuclear reactor. In developing Molten Salt Reactor, the behavior of fission product in operation should be preliminary evaluated for the correct design of reactor and its associated system including off-gas treatment. In this study, for 100 Mw 46 KCl- 54 UCl3 based Molten Salt Reactor with operating life time of 20 year, the fission product behavior was estimated by thermodynamic modeling employing FactSage 8.2. Total inventory of all fission product were firstly calculated using OpenMC code allowing depletion during neutronic calculation. Then, among all inventory, 46 element species from Uranium to Holmium were chosen and given to the input for equilibrium module of Factsage with its mass. In phase equilibrium calculation, for the correct description of solution phase, KCl-UCl3 solution database based on modified quasichemical model in the quadruplet approximation (ANL/CFCT-21/04) was employed and the coexisting solid phase was assumed to pure state. With the assumption of no oxygen and moisture ingress into reactor system, equilibrium calculation showed that 1% of solid phase and of gas phase were newly formed and, in gas phase, major species were identified : ZrCl4 (47%), Xe (33%), UCl4 (14%), Kr (5%), Ar (1%) and others. This result reveals that off-gas treatment of system should account for the appropriate treatment of ZrCl4 and UCl4 besides treatment of noble gas such as Xe and Kr.
422.
2023.11 구독 인증기관·개인회원 무료
Heavy water (deuterium oxide, D2O) is water in which hydrogen atoms (1H, H), one of the constituent elements of water molecules, have been replaced with deuterium (2H, D), a heavier isotope. Heavy water is used in a variety of industries, including semiconductors, nuclear magnetic resonance, infrared spectroscopy, neutron deceleration, neutrino detection, metabolic rate studies, neutron capture therapy, and the production of radioactive materials such as plutonium and tritium. In particular, heavy water is used as a neutron moderator or coolant in nuclear reactors and as a fuel for nuclear fusion energy, methods for measuring heavy water are becoming increasingly important. There are methods with density, mass spectrometry, and infrared (IR) spectroscopy. In this study, Fourier transform infrared spectroscopy (FT-IR) was used, which is commonly used in IR spectroscopy because of its relatively high analytical sensitivity, low operating costs, and easy online analysis. Heavy water was identified in the range of 2,300-2,600 cm-1 wavenumber (O-D) and the range of 1,200-1,300 cm-1 wavenumber (D-O-D), which are known to be the range with strong infrared absorption. As a result, the linearity of infrared absorbance for each heavy water concentration was confirmed within the relative expansion uncertainty (k=2).
423.
2023.11 구독 인증기관·개인회원 무료
Chelating agents like ethylenediaminetetraacetic acid (EDTA), diethylenetriaminepentaacetic acid (DTPA), and nitrilotriacetic acid (NTA) find extensive application in the removal of residual substances due to their high stability constants with a wide range of metal ions. They also play a crucial role in nuclear decontamination operations aimed at eliminating metallic radionuclides such as 60Co, 90Sr, and 239Pu. However, improper disposal of chelated radioactive waste can lead to significant increases in radionuclide migration rates from disposal sites. Therefore, it is imperative to comprehend the behavior of chelating agents under varying conditions, including pH, temperature, and metal ion concentrations. In this study, we present the results of a pH-dependent composition analysis of nickel-chelate complexes using UV-Vis spectrophotometry. Nickel (Ni) serves as an ideal metal ion for investigating its interactions with chelating agents due to its solubility over a wide pH range and high stability constants with all three chelating agents mentioned earlier. Initially, UV-Vis spectra of Ni-EDTA, Ni-DTPA, and Ni-NTA complexes were recorded at various pH levels. We assigned absorption maxima and compared our findings with existing literature on each Ni-chelate complex. Furthermore, we examined mixed samples of all three complexes, varying the pH to monitor changes in composition. The results and their implications will be presented in our poster presentation.
424.
2023.11 구독 인증기관·개인회원 무료
This study explores the impact of metal doping on the surface structure of spent nuclear fuels (SNFs), particularly uranium dioxide (UO2). SNFs undergo significant microstructural changes during irradiation, affecting their physical and chemical properties. Certain elements, including actinides and lanthanides, can integrate into the UO2 lattice, leading to non-stoichiometry based on their oxidation state and environmental conditions. These modifications are closely linked to phenomena like corrosion and oxidation of UO2, making it essential to thoroughly characterize SNFs influenced by specific element doping for disposal or interim storage decisions. The research employs X-ray diffraction (XRD), scanning electron microscopy (SEM), and Raman spectroscopy to investigate the surface structure of UO2 samples doped with elements such as Nd3+, Gd3+, Zr4+, Th4+, and ε-particles (Mo, Ru, Pd). To manufacture these samples, UO2 powders are mixed and pelletized with the respective dopant oxide powders. The resulting pellet samples are sintered under specific conditions. The XRD analysis reveals that the lattice parameters of (U,Nd)O2, (U,Gd)O2, (U,Zr)O2, and (U,Th)O2 linearly vary with increasing doping levels, suggesting the formation of solid solutions. SEM images show that the grain size decreases with higher doping levels in (U,Gd)O2, (U,Nd)O2, and (U,Zr)O2, while the change is less pronounced in (U,Th)O2. Raman spectroscopy uncovers that U0.9Gd0.1O2-x and U0.9Nd0.1O2-x exhibit defect structures related to oxygen vacancies, induced by trivalent elements replacing U4+, distorting the UO2 lattice. In contrast, U0.9Zr0.1O2 shows no oxygen vacancy-related defects but features a distinct peak, likely indicating the formation of a ZrO8-type complex within the UO2 lattice. ε-Particle doped uranium dioxide shows minimal deviations in surface properties compared to pure UO2. This structural characterization of metal-doped and ε-particle-doped UO2 enhances our understanding of spent nuclear fuel behavior, with implications for the characterization of radioactive materials. This research provides valuable insights into how specific element doping affects the properties of SNFs, which is crucial for managing and disposing of these materials safely.
425.
2023.11 구독 인증기관·개인회원 무료
Owing to the rapid rise of global energy demands, the operation of nuclear power plants is still indispensable. However, following the nuclear accident at Fukushima-Daiichi in 2011, the secure sequestration of radioactive waste has become critical for ensuring safe operations. Among various forms of nuclear wastes, capturing radioactive organic iodide (ROIs, e.g., methyl iodide, ethyl iodide, and propyl iodide) as one of the important species in gas phase waste has been challenged owing to the insufficient sorbent materials. The environmental release of ROIs with high volatility can give rise to adverse effects, including the accumulation of these substances in the thyroid and the development of conditions such as hypothyroidism and thyroid cancer. Compared to an iodine molecule, ROIs exhibit low affinity for conventional sorbents such as Ag@mordenite zeolite and triethylenediamine-impregnated activated carbon (TED@AC), resulting in lower sorption rates and capacities. Furthermore, in conditions resembling practical adsorption environments with high humidity, the presence of H2O significantly impedes the adsorption process, leading to a nearly complete cessation of adsorption. To address these issues, metal-organic frameworks (MOFs) can be effective alternative sorbents owing to their high surface area and designable and tailorable pore properties. In addition, the wellfined crystalline structures of MOFs render in-depth study on the structure-properties relationship. However, there has been limited research on the adsorption of ROIs using MOFs, with the majority of adsorption processes relying on highly reversible physisorption. This type of ROIs adsorption not only exists in a precarious state that is susceptible to volatilization but also exhibits significantly reduced adsorption capabilities in humid environments. Thus, for the secure adsorption of the volatile ROIs, the development of sorbents capable of chemisorption is highly desirable. In this study, we focused on ROIs adsorption by electrophilic aromatic substitution with the electron-rich m-DOBDC4− (m-DOBDC4− = 4,6-dioxo-1,3-benzenedicarboxylate) present in Co2(m -DOBDC). The chemisorption of ROIs via electrophilic aromatic substitution not only leads to the formation of C-C bonds, ensuring stability but also triggers color changes in the crystal by interacting with open-metal sites and iodide ions. Leveraging these advantages, we developed an infrared radiation-based sensing method that demonstrates superior performance, exhibiting high adsorption capacities and rates, even under the challenging conditions of high-humidity practical environments.
426.
2023.11 구독 인증기관·개인회원 무료
Selenium (Se), a vital trace element found naturally, plays a pivotal role for human being in low concentrations. Notably, within the spectrum of essential elements, Se possesses the most restricted range between the dietary deficiency (< 40 μg day-1) and the acute toxicity (> 400 μg day-1). Therefore, it is of paramount importance to maintain bioavailable Se levels within permissible limits in our drinking water sources. Among the various Se species, inorganic variants such as selenite (SeO3 2-) and selenate (SeO4 2-) are highly water-soluble, with SeO3 2- being notably more toxic than SeO4 2-. Consequently, the primary focus lies in effectively sequestering SeO3 2- from aquatic environments. Numerous methods have been investigated for SeO3 2- adsorption, including the use of metal oxides and carbon-based materials. Especially, iron oxides have garnered extensive attention due to their water stability and environmentally friendly properties. Nevertheless, their limited surface area and insufficient adsorption sites impose constraints on their efficacy as materials for SeO3 2- removal. Recently, metal–organic frameworks (MOFs), composed of metal centers bridged by organic linkers have increasingly focused as promising adsorbents for SeO3 2- removal, offering significant advantages such as large surface areas, high porosities, and structural versatility. Furthermore, there is a growing interest in defective MOFs, where intentional defects are introduced into the MOF structure. This deliberate introduction of defects aims to enhance the adsorption capacity by increasing the number of available adsorption sites. In this context, herein, we present the Fe-BTC (BTC = 1,3,5-benzenetricarboxylic acid) synthesized via a post-synthetic metal-ion metathesis (PSMM) approach, which is one of the defect engineering methods applied to metal sites. We employ the well-established MOF, HKUST-1, known for its substantial surface area, as the pristine MOF. While the pristine MOF has a crystalline phase, during the PSMM process, Fe-BTC is transformed into an amorphous phase by allowing the introduction of numerous metal defect sites. These introduced metal defect sites serve as Lewis acidic sites, enhancing the adsorption capability for selenite. Furthermore, despite its amorphous nature, Fe-BTC exhibits a substantial surface area and porosity comparable to that of the crystalline pristine MOF. Consequently, Fe-BTC, distinguished by its numerous adsorption sites and its high porosity, demonstrates a remarkable capacity for selenite adsorption.
427.
2023.11 구독 인증기관·개인회원 무료
Chelating agents, such as EDTA, NTA, and citric acid, possess the capacity to establish complexes with radionuclides, potentially enhancing the migration of such radionuclides from the disposal sites. Hence, quantification of these chelating agents in radioactive wastes is required to ensure secure disposal protocols. The determination of chelating agents in radioactive wastes is mainly composed of two steps, e.g. extraction and detection. However, there are little information on the extraction of the chelators in various radioactive wastes. We endeavored to optimize the extraction conditions for citric acid (CA) found within concrete, a prevalent component in the context of dismantled waste materials. Given the inherent high solubility of CA in water, we applied an aliquot of deionized water to the concrete and conducted a one-hour ultrasonic leaching procedure to facilitate chelate extraction. Subsequently, following the preparation of the concrete leachate via vacuum filtration and centrifugation to yield a clarified solution, we quantified the concentration of CA within the solution using Ion Chromatography (IC). To enhance leaching efficiency, we examined the % recovery variation with respect to the pH of the leaching solution. The optimized extraction method will be applied to diverse chelating agents and radioactive waste categories.
428.
2023.11 구독 인증기관·개인회원 무료
The potentiostatic titration method is one of the effective methods for determining the total uranium assay in high-concentration uranium samples. A notable approach is the Devies-Grey titration method, which was first reported in 1964. In the U sample treatment process of this method, the reduction of U(VI) by Fe(II) is initially a non-spontaneous reaction based on the reduction potentials of the two half-reactions. However, in a high-concentration phosphoric acid medium, the reduction potential of Fe(II) is enhanced, simultaneously increasing the reduction potential of U(VI). As a result, the redox reaction becomes spontaneous due to these dual effects. On the other hand, the reaction kinetics can elucidate why nitric acid does not oxidize U(IV) during the oxidation of Fe(II) to Fe(III). Furthermore, the role of Mo(VI)/Mo(V) as a redox enhancer, employed alongside nitric acid, can be comprehended through electrochemical means. Similarly, the function of V(IV) as an electrochemical enhancer, aiding the action of the Cr(VI) titrant, becomes understandable. Grasping the various phenomena that manifest during the titration process is imperative for refining existing titration methods and pioneering new ones.
429.
2023.11 구독 인증기관·개인회원 무료
This study presents a rapid and sequential radiochemical separation method for Pu and Am isotopes in radioactive waste samples from the nuclear power plant with anion exchange resin and TRU resin. After radionuclides were leached from the radioactive waste samples with concentrated HCl and HNO3, the sample was allowed to evaporate to dryness after filtering the leaching solution with 0.45 micron filter. The Pu isotopes were separated in HNO3 medium with anion exchange resin. For leaching solution passed through anion exchange column, the Am isotopes were separated with TRU resin. The purified Pu and Am isotopes were measured by alpha spectrometer, respectively, after micro-precipitation of neodymium. The sequential radiochemical separation of Pu and Am isotopes in radioactive waste samples using anion exchange resin and TRU resin was validated with ICP-MS system.
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