Radioactive iodine-129, a byproduct of nuclear fission in nuclear power plants, presents significant environmental and health risks due to its high solubility in water and volatility. Iodine-129, with its half-life of 1.57×1017 years, necessitates safe management and disposal. Therefore, safely capturing and managing I-129 during spent nuclear fuel reprocessing is of paramount importance. To address these challenges, various glass waste forms containing silver iodide have been developed, such as borosilicate, silver phosphate, silver vanadate, and silver tellurite glasses. These glasses effectively immobilize iodine, but the high cost of silver raises affordability concerns. This study introduces CuI·Cu2O·TeO2 glass waste forms for iodine immobilization, a novel approach. The cost-effectiveness of copper, in contrast to silver, makes it an attractive alternative. The CuI·Cu2O·TeO2 glass waste forms were synthesized with varying CuI content (x) in (1-x)(0.3Cu2O·0.7TeO2) glass matrices. Xray diffraction (XRD) confirmed amorphous structures, and X-ray fluorescence (XRF) quantified composition. X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy provided insights into structural properties. Durability assessments using a 7-day product consistency test (PCT-A) and inductively coupled plasma-mass spectrometry (ICP-MS) revealed compliance with U.S. glass regulations, making CuI·Cu2O·TeO2 glasses a promising choice for iodine immobilization in radioactive waste.

The nuclide management process for reducing the environmental burden being developed by the Korea Atomic Energy Research Institute is performed in molten salts, resulting in contaminated salt wastes containing fission products such as Cs, Sr, Ba, and rare-earth nuclides. In addition, the spent fuel of a molten salt reactor (MSR) contains a variety of fission products, and a purification process may be required for the reuse of the salt and the separation and disposal of the fission products in the spent nuclear fuel. The melt-crystallization method is a technique used for the purification and separation of chemicals or metals based on the different melting points of the different substances. In a recent study, our group developed a reactive-crystallization method using Li2CO3 precipitation agent to precipitate metal corrosion from the reactor through a chlorination reaction by HCl and Cl2, which may occur in chloride molten salt, and successfully precipitated the metal precipitate and purified and recovered LiCl salt. In this study, reactive-crystallization method has been established for removing fission products and corrosive materials. Using the reactive crystallization method, white LiCl-KCl salt that was not discolored by metal corrosion was recovered through the crystallization plates, and fission products and metal elements were shown to be suppressed to several ppm in the purified salt. Consequently, high-purity salts were recovered with high nuclide and corrosive separation efficiencies. The reactive crystallization procedure can also be applied to other salt waste systems, such as MSR nuclear fuel treatment and molten salt chemistry for the elimination of corrosive substances.

본 연구에서는 실리카 복합막 기반 고분자 전해질막을 5단 연료전지 스택에 적용하여 성능 평가를 수행하였다. 이를 통하여, 개별 구성 요소의 성능도 중요하지만, 전체적인 관점에서 공급되는 연료의 유량이 스택 성능에 중요한 역할을 하며, 특히 수소의 유량에 크게 의존한다는 사실이 확인하였다. 산소의 유량을 증가시켜도 성능의 변화는 미미한 반면, 수소 의 유량을 증가시키면 성능이 향상되는 것을 확인하였다. 그러나 수소의 유량 증가는 수소와 산소 유량 비율의 불균형을 초 래하여 장기적으로는 스택 성능과 내구성을 저하시키는 문제가 관찰되었다. 이러한 현상을 스택 구성 요소 및 개별 단위 셀 에서도 관찰할 수 있었으며, 따라서 스택 운전 시 각 구성 요소의 성능을 최적화하는 것 외에도 균일한 유량 제어를 위해 유 로 설계 및 운전 조건을 최적화하는 것이 중요하다는 것을 알 수 있었다. 마지막으로 실리카 복합막은 최대 출력 기준 25 W 이상의 성능을 나타내어 실제 연료전지 시스템에 적용하기에 충분한 성능을 갖춘 것으로 판단된다.

Many countries have used nuclear power to generate electricity. Uranium-235, which is used as fuel in nuclear power plants, produces many fission products. Among them, iodine-129 is problematic due to its long half-life (1.57×107 years) and high diffusivity in the environment. If it is released into the environment without any treatment, it could have a major impact on humans and ecosystems. Therefore, it must be treated into a stable form through capture and solidification. Iodine can be captured in the form of AgI through silver-loaded zeolite filters in off-gas treatment processes. However, AgI could be decomposed in the reducing atmosphere of groundwater, so it must be converted into a stable form. In this study, Al2O3, Bi2O3, PbO, V2O5, MoO3, or WO3 were added to the iodine solidification matrix, AgI-Ag2O-TeO2 glass. The glass precursors were mixed to the appropriate composition and placed in an alumina crucible. After heat treatment at 800°C for 1 hour, the melt was quenched in a carbon crucible. The leaching behavior and thermal properties of the glass samples were evaluated. The PCT-A test for leaching evaluation showed that the normalized releases of all elements were below 2 g/m2, which satisfied the U.S. glass wasteform leaching regulations. Diffrential scanning calorimetry (DSC) was performed to evaluate the thermal properties of all glass samples. The addition of MoO3 or WO3 to the AgI-Ag2O-TeO2 glass increased the glass transition temperature (Tg) and crystallization temperature (Tc) while maintaining the glass stability. The similar relative electro-static filed values of MoO3, and WO3 which are approxibately three times that of the glass network former TeO2, could provide sufficient force to the TeO2 interacting with the non-bridging oxygen forming Te-O-M (M=V, Mo, W) links. The high electrostatic forces of Mo and W increased the glass network cohension and prevented the crystallization of the glass.

Heat-generating nuclides such as Cs-137 and Sr-90 should be separated from spent nuclear fuel to reduce the short-term thermal load on the repository facility. In particular, Sr-90 must be separated because its decay process generates high temperatures. Recently, the Korea Atomic Energy Research Institute (KEARI) has been developing a waste burden minimization technology to reduce the environmental burden resulting from the disposal of spent nuclear fuel and maximize the utilization of the disposal facility. The technology incorporates a nuclide management process that maximizes disposal efficiency by selectively separating and accumulating key nuclides from spent nuclear fuel, such as Cs, Sr, I, TRU/RE, and Tc/Se. Sr nuclides dissolve in the chloride phase during the chlorination process of spent nuclear fuel and are recovered as carbonate or oxide through reactive distillation or reactive crystallization. Due to their chemical similarity, Ba nuclides are recovered along with Sr nuclides during this process. In this study, we prepared a ceramic waste form for group II nuclides, Ba(x)Sr(1-x)TiO3 (x=0, 0.25, 0.5, 0.75, 1), using the solid-state reaction method, taking into account the different ratios of Sr/Ba nuclides produced during the nuclide management process. Regardless of the Sr/Ba ratio, the established waste form fabrication process was able to produce a stable waste form. Physicochemical properties, including leaching and thermal properties, were evaluated to determine the stability of group II waste forms. In addition, the radiological properties of waste forms of Ba(x)Sr(1-x)TiO3 with varying Sr/Ba ratios were evaluated. These results provided fundamental data for the long-term storage and management of waste forms containing group II nuclides.

Boric acid-containing B-10 is used in a nuclear reactor as a coolant and absorbs thermal neutrons generated during nuclear fission in the primary circuit. Boron-containing coolant water waste is generated from maintenance, floor drain, decontamination, and reactor letdown flows. There are two options for aqueous solution waste of boric acid. One is recycling and discharge through filtration, ion exchange, and reverse osmosis. The other is immobilization after evaporation and crystallization processes. The dry powder of boric acid waste liquid can be immobilized by cement, polymer, etc. Before the mid-1990s, concentrated boric acid waste was solidified with a cement matrix. To overcome the disadvantage of low waste loading of cement waste form, a method of solidifying with paraffin was adopted. However, paraffin solids were insufficient to be disposed of as final waste. Paraffin is a kind of soft solidified material and has low compressive strength and poor leaching resistance. As a result, it was decided as an unsuitable form for disposal. In KOREA, paraffin waste form was adopted for boric acid waste treatment in the 1990s. A large amount of paraffin waste forms about 20,000 drums (200 l drum) were generated to treat boric acid waste and were stored in nuclear power sites without disposal. In this study, we want to obtain high-purity boric acid waste by oxidizing and decomposing solid paraffin waste form through a boric acid catalytic reaction. In this reaction, paraffin is separated in the form of various by-products, which can then be treated through a liquid waste treatment device or an exhaust gas treatment device. The proper temperature for sample decomposition during the catalytic reaction was set through TGA analysis. Compositions of by-products and residues generated at each stage of the reaction could be analyzed to determine the state during the reaction. Finally, the boric acid waste powder was perfectly separated from paraffin waste form with disposable products through this pyrolysis process.

Se-79, a fission product of uranium, is present in spent nuclear fuel. Selenium is volatilized from the spent nuclear fuel during the pretreatment of pyroprocessing, and a filter composed of calcium oxide can capture gaseous selenium in the form of CaSeO3. Because Se-79 has a long half-life (3.27E5 years) and selenite ions have high mobility in groundwater, they must be immobilized in a chemically stable form for final disposal. This study used a composition of 50 TeO2 - 10 Al2O3 - 10 B2O3 - 10 Na2O - 10 CaO - 10 ZnO (mol%). High-purity powders of TeO2, Al2O3, H3BO3, Na2CO3, CaCO3, and ZnO were used as glass precursors. The mixed powders were placed in alumina crucibles and melted in an electric furnace under an ambient atmosphere at 800°C for 1 h before being cast on a carbon mold. The obtained glasses were ground into fine powders and then mixed with CaSeO3 powders. The powders were melted in alumina crucibles at 800°C for 1 h. To simulate a seleniumcaptured calcium filter, CaSeO3 was synthesized by a precipitation method using sodium selenite (Na2SeO3) and calcium nitrate (Ca(NO3)2) solutions. The glass samples were analyzed by an X-ray diffractometer (XRD). Retention of Se in tellurite glasses was analyzed by an X-ray fluorescence spectrometer (XRF) and inductively coupled plasma (ICP). The chemical durability of tellurite glass was evaluated through the PCT method.

Uranium-235, used in nuclear power generation, produces a lot of radioactive waste. Among radioactive waste nuclides, I-129 is problematic due to its long half-life (1.57×107 y) with high mobility in the environment. It should be captured and immobilized into a geological disposal environment through a stable waste form. In this study, various additives including Al, Bi, Pb, V, Mo and W were added to silver tellurite glass to prepare a matrix for immobilizing iodine, and its thermal and leaching properties were evaluated. To prepare glass, the glass precursor mixture was placed in alumina crucibles and heated at 800°C for 1 h. Except for aluminum, there was no significant loss of constituent elements. The loading of iodine in the matrix was approximately 11-15% by weigh, excluding oxygen. The normalized releases of all the elements obtained by PCT-A were below the order of 10-1 g/m2, which satisfies US regulation (2 g/m2). Differential scanning calorimetry was performed to evaluate the thermal properties of the glass samples. The glass transition temperature (Tg) increased by adding such as V2O5, MoO3, or WO3. The similar relative electrostatic field values of V2O5, MoO3, and WO3 could provide sufficient electro static field to the TeO2 interacting with the non-bridging oxygen forming Te-O-M (M = V, Mo, W) links. The addition of MoO3 or WO3 in the silver tellurite glass system increased glass transition temperature (Tg) and crystallization temperature (Tc) while maintaining the glass stability.

To minimize the short-term thermal load on the repository facility, heat generating nuclides such as Cs-137 and Sr-90 should be separated from the spent nuclear fuel for efficiency of repository facility. In particular, Sr-90 must be separated because it generates high heat during the decay process. Recently, Korea Atomic Energy Research Institute (KEARI) is developing a waste burden minimization technology to reduce the environmental burden caused by the disposal of spent nuclear fuel and maximize the utilization of the disposal facility. The technology includes a nuclide management process that can maximize disposal efficiency by selectively separating and collecting major nuclides such as Cs, Sr, I, TRU/RE, and Tc/Se from spent nuclear fuel. Among the major nuclides, Sr nuclides dissolve in chloride phase during the chlorination process of spent nuclear fuel and recovered in the form of carbonate or oxide via reactive distillation. In this process, Ba nuclides are also recovered along with Sr nuclides due to their chemical similarity. In this study, we prepared group II nuclide ceramic waste form, Ba(x)Sr(1-x)TiO3 (x=0, 0.25, 0.5, 0.75, 1), using the solid-state reaction method by considering the various ratio of Sr/Ba nuclides generated from nuclide management process. The established waste form fabrication process was able to produce a stable waste form regardless of the ratio of Sr/Ba nuclides. To evaluate the stability of group II waste form, physicochemical properties such as leaching and thermal properties were evaluated. Also, the radiological properties of the Ba(x)Sr(1-x)TiO3 waste forms with various Sr/Ba ratios were evaluated, and the estimation of centerline temperature was carried out using the experimental thermal property data. These results provided fundamental data for long-term storage and management of group II nuclides waste form.

In this study, an aerosol process was introduced to produce CaCO3. The possibility of producing CaCO3 by the aerosol process was evaluated. The characteristics of CaCO3 prepared by the aerosol process were also evaluated. In the CaCO3 prepared in this study, as the heat treatment proceeded, the calcite phase disappeared. The portlandite phase and the lime phase were formed by the heat treatment. Even if the CO2 component is removed from the calcite phase, there is a possibility that the converted CO2 component could be adsorbed into the Ca component to form a calcite phase again. Therefore, in order to remove the calcite phase, carbon components should be removed first. The lime phase was formed when CO2 was removed from the calcite phase, while the portlandite phase was formed by the introducing of H2O to the lime phase. Therefore, the order in which each phase formed could be in the order of calcite, lime, and portlandite. The reason for the simultaneous presence of the portlandite phase and the lime phase is that the hydroxyl group (OH−) introduced by H2O was not removed completely due to low temperature and/or insufficient heating time. When the sufficient temperature (900°C) and heating time (60 min) were applied, the hydroxyl group (OH−) was removed to transform into lime phase. Since the precursor contained the hydrogen component, it could be possible that the moisture (H2O) and/or the hydroxyl group (OH−) were introduced during the heat treatment process.

Uranium-235, used for nuclear power generation, has brought radioactive waste. It could be released into the environment during reprocessing or recycling of the spent nuclear fuel. Among the radioactive waste nuclides, I-129 occurs problems due to its long half-life (1.57×107 y) with high mobility in the environment. Therefore, it should be captured and immobilized into a geological disposal system through a stable waste form. One of the methods to capture iodine in the off-gas treatment process is to use silver loaded zeolite filter. It converts radioactive iodine into AgI, one of the most stable iodine forms in the solid state. However, it is difficult to directly dispose of AgI itself in an underground repository because of its aqueous dissolution under reducing condition with Fe2+. It must be immobilized in the matrix materials to prevent release of iodine as a result of chemical reaction. Among the matrix glasses, silver tellurite glass has been proposed. In this study, additives including Al, Bi, Pb, V, Mo, and W were added into the silver tellurite glass. The thermal properties of each matrix for radioactive iodine immobilization were evaluated. The glasses were prepared by the melt-quenching method at 800°C for 1 h. Differential scanning calorimetry (DSC) was performed to evaluate the thermal properties of the glass samples. From the study, the glass transition temperature (Tg) was increased by adding additives such as V2O5, MoO3, or WO3 in the silver tellurite glass. The relative electro-static field (REF) values of V2O5, MoO3, and WO3 are about three times higher than that of the glass network former, TeO2. It could provide sufficient electro-static field (EF) to the TeO2 interacting with the non-bridging oxygen forming Te-O-M (M = V, Mo, W) links. Therefore, the addition of V2O5, MoO3, or WO3 reinforced the glass network cohesion to increase the Tg of the glass. The addition of MoO3or WO3 in the silver tellurite glass increased Tg and crystallization temperature (Tc) with remaining the glass stability.

To reduce the environmental burden caused by the disposal of spent nuclear fuel and maximize the utilization of the repository facility, waste burden minimization technology is currently being developed at the Korea Atomic Energy Research Institute (KEARI). The technology includes a nuclide management process that can maximize disposal efficiency by selectively separating and collecting major nuclides in spent nuclear fuel. In addition, for efficient storage facility utilization, the short-term decay heat generated by spent nuclear fuel must be removed from the waste stream. To minimize the short-term thermal load on the repository facility, it is necessary to separate heat generating nuclides such as Cs-137 and Sr-90 from the spent fuel. In particular, Sr-90 must be separated because it generates high heat during the decay process. KAERI has developed a technology for separating Sr nuclides from Group II nuclides separated through the nuclide management process. In this study, we prepared Sr ceramic waste form, SrTiO3, by using the solid-state reaction method for long-term storage for the decay of separated Sr nuclides and evaluated the physicochemical properties of the waste form. Also, the radiological and thermal characteristics of the Sr waste form were evaluated by predicting the composition of Sr nuclides separated through the nuclide management process, and the estimation of centerline temperature was carried out using the experimental thermal data and steady state conduction equation in a long and solid cylinder type waste form. These results provided fundamental data for long-term storage and management of Sr waste.